Techniques for improving material fidelity and contrast consistency in secondary electron mode helium ion microscope (HIM) imaging

NASA Astrophysics Data System (ADS)

Thompson, William; Stern, Lewis; Ferranti, Dave; Huynh, Chuong; Scipioni, Larry; Notte, John; Sanford, Colin

2010-06-01

Recent helium ion microscope (HIM) imaging studies have shown the strong sensitivity of HIM induced secondary electron (SE) yields [1] to the sample physical and chemical properties and to its surface topography. This SE yield sensitivity is due to the low recoil energy of the HIM initiated electrons and their resulting short mean free path. Additionally, a material's SE escape probability is modulated by changes in the material's work function and surface potential. Due to the escape electrons' roughly 2eV mean energy and their nanometer range mean free path, HIM SE mode image contrast has significant material and surface sensitivity. The latest generation of HIM has a 0.35 nanometer resolution specification and is equipped with a plasma cleaning process to mitigate the effects of hydrocarbon contamination. However, for surfaces that may have native oxide chemistries influencing the secondary electron yield, a new process of low energy, shallow angle argon sputtering, was evaluated. The intent of this work was to study the effect of removing pre-existing native oxides and any in-situ deposited surface contaminants. We will introduce the sputter yield predictions of two established computer models and the sputter yield and sample modification forecasts of the molecular dynamics program, Kalypso. We will review the experimental technique applied to copper samples and show the copper grain contrast improvement that resulted when argon cleaned samples were imaged in HIM SE mode.

Observation of oscillatory relaxation in the Sn-terminated surface of epitaxial rock-salt SnSe { 111 } topological crystalline insulator

NASA Astrophysics Data System (ADS)

Jin, Wencan; Dadap, Jerry; Osgood, Richard; Vishwanath, Suresh; Lien, Huai-Hsun; Chaney, Alexander; Xing, Huili; Liu, Jianpeng; Kong, Lingyuan; Ma, Junzhang; Qian, Tian; Ding, Hong; Sadowski, Jerzy; Dai, Zhongwei; Pohl, Karsten; Lou, Rui; Wang, Shancai; Liu, Xinyu; Furdyna, Jacek

Topological crystalline insulators have been recently observed in rock-salt SnSe { 111 } thin films. Previous studies have suggested that the Se-terminated surface of this thin film with hydrogen passivation is a preferred configuration. In this work, synchrotron-based angle-resolved photoemission spectroscopy, along with density functional theory calculations, are used to demonstrate conclusively that a rock-salt SnSe { 111 } thin film has a stable Sn-terminated surface. These observations are supported by low energy electron diffraction (LEED) intensity-voltage measurements and dynamical LEED calculations, which further show that the Sn-terminated SnSe { 111 } thin film has undergone an oscillatory surface structural relaxation. In sharp contrast to the Se-terminated counterpart, the Dirac surface state in the Sn-terminated SnSe { 111 } thin film yields a high Fermi velocity, 0 . 50 ×106 m/s, which may lead to high-speed electronic device applications. DOE No. DE-FG 02-04-ER-46157.

Band structure and spin texture of Bi2Se3 3 d ferromagnetic metal interface

NASA Astrophysics Data System (ADS)

Zhang, Jia; Velev, Julian P.; Dang, Xiaoqian; Tsymbal, Evgeny Y.

2016-07-01

The spin-helical surface states in a three-dimensional topological insulator (TI), such as Bi2Se3 , are predicted to have superior efficiency in converting charge current into spin polarization. This property is said to be responsible for the giant spin-orbit torques observed in ferromagnetic metal/TI structures. In this work, using first-principles and model tight-binding calculations, we investigate the interface between the topological insulator Bi2Se3 and 3 d -transition ferromagnetic metals Ni and Co. We find that the difference in the work functions of the topological insulator and the ferromagnetic metals shift the topological surface states down about 0.5 eV below the Fermi energy where the hybridization of these surface states with the metal bands destroys their helical spin structure. The band alignment of Bi2Se3 and Ni (Co) places the Fermi energy far in the conduction band of bulk Bi2Se3 , where the spin of the carriers is aligned with the magnetization in the metal. Our results indicate that the topological surface states are unlikely to be responsible for the huge spin-orbit torque effect observed experimentally in these systems.

Effect of core quantum-dot size on power-conversion-efficiency for silicon solar-cells implementing energy-down-shift using CdSe/ZnS core/shell quantum dots.

PubMed

Baek, Seung-Wook; Shim, Jae-Hyoung; Seung, Hyun-Min; Lee, Gon-Sub; Hong, Jin-Pyo; Lee, Kwang-Sup; Park, Jea-Gun

2014-11-07

Silicon solar cells mainly absorb visible light, although the sun emits ultraviolet (UV), visible, and infrared light. Because the surface reflectance of a textured surface with SiNX film on a silicon solar cell in the UV wavelength region (250-450 nm) is higher than ∼27%, silicon solar-cells cannot effectively convert UV light into photo-voltaic power. We implemented the concept of energy-down-shift using CdSe/ZnS core/shell quantum-dots (QDs) on p-type silicon solar-cells to absorb more UV light. CdSe/ZnS core/shell QDs demonstrated clear evidence of energy-down-shift, which absorbed UV light and emitted green-light photoluminescence signals at a wavelength of 542 nm. The implementation of 0.2 wt% (8.8 nm QDs layer) green-light emitting CdSe/ZnS core/shell QDs reduced the surface reflectance of the textured surface with SiNX film on a silicon solar-cell from 27% to 15% and enhanced the external quantum efficiency (EQE) of silicon solar-cells to around 30% in the UV wavelength region, thereby enhancing the power conversion efficiency (PCE) for p-type silicon solar-cells by 5.5%.

Low-Temperature Growth of Two-Dimensional Layered Chalcogenide Crystals on Liquid.

PubMed

Zhou, Yubing; Deng, Bing; Zhou, Yu; Ren, Xibiao; Yin, Jianbo; Jin, Chuanhong; Liu, Zhongfan; Peng, Hailin

2016-03-09

The growth of high-quality two-dimensional (2D) layered chalcogenide crystals is highly important for practical applications in future electronics, optoelectronics, and photonics. Current route for the synthesis of 2D chalcogenide crystals by vapor deposition method mainly involves an energy intensive high-temperature growth process on solid substrates, often suffering from inhomogeneous nucleation density and grain size distribution. Here, we first demonstrate a facile vapor-phase synthesis of large-area high-quality 2D layered chalcogenide crystals on liquid metal surface with relatively low surface energy at a growth temperature as low as ∼100 °C. Uniform and large-domain-sized 2D crystals of GaSe and GaxIn1-xSe were grown on liquid metal surface even supported on a polyimide film. As-grown 2D GaSe crystals have been fabricated to flexible photodetectors, showing high photoresponse and excellent flexibility. Our strategy of energy-sustainable low-temperature growth on liquid metal surface may open a route to the synthesis of high-quality 2D crystals of Ga-, In-, Bi-, Hg-, Pb-, or Sn-based chalcogenides and halides.

Smectic C liquid crystal growth through surface orientation by ZnxCd1-xSe thin films

NASA Astrophysics Data System (ADS)

Katranchev, B.; Petrov, M.; Bineva, I.; Levi, Z.; Mineva, M.

2012-12-01

A smectic C liquid crystal (LC) texture, consisting of distinct local single crystals (DLSCs) was grown using predefined orientation of ternary nanocrystalline thin films of ZnxCd1-xSe. The surface morphology and orientation features of the ZnxCd1-xSe films were investigated by AFM measurements and micro-texture polarization analysis. The ZnxCd1-xSe surface causes a substantial enlargement of the smectic C DLSCs and induction of a surface bistable state. The specific character of the morphology of this coating leads to the decrease of the corresponding anchoring energy. Two new chiral states, not typical for this LC were indicated. The physical mechanism providing these new effects is presented.

Introducing sampling entropy in repository based adaptive umbrella sampling

NASA Astrophysics Data System (ADS)

Zheng, Han; Zhang, Yingkai

2009-12-01

Determining free energy surfaces along chosen reaction coordinates is a common and important task in simulating complex systems. Due to the complexity of energy landscapes and the existence of high barriers, one widely pursued objective to develop efficient simulation methods is to achieve uniform sampling among thermodynamic states of interest. In this work, we have demonstrated sampling entropy (SE) as an excellent indicator for uniform sampling as well as for the convergence of free energy simulations. By introducing SE and the concentration theorem into the biasing-potential-updating scheme, we have further improved the adaptivity, robustness, and applicability of our recently developed repository based adaptive umbrella sampling (RBAUS) approach [H. Zheng and Y. Zhang, J. Chem. Phys. 128, 204106 (2008)]. Besides simulations of one dimensional free energy profiles for various systems, the generality and efficiency of this new RBAUS-SE approach have been further demonstrated by determining two dimensional free energy surfaces for the alanine dipeptide in gas phase as well as in water.

Quasiparticle energy bands and Fermi surfaces of monolayer NbSe2

NASA Astrophysics Data System (ADS)

Kim, Sejoong; Son, Young-Woo

2017-10-01

A quasiparticle band structure of a single layer 2 H -NbSe2 is reported by using first-principles G W calculation. We show that a self-energy correction increases the width of a partially occupied band and alters its Fermi surface shape when comparing those using conventional mean-field calculation methods. Owing to a broken inversion symmetry in the trigonal prismatic single layer structure, the spin-orbit interaction is included and its impact on the Fermi surface and quasiparticle energy bands are discussed. We also calculate the doping dependent static susceptibilities from the band structures obtained by the mean-field calculation as well as G W calculation with and without spin-orbit interactions. A complete tight-binding model is constructed within the three-band third nearest neighbor hoppings and is shown to reproduce our G W quasiparticle energy bands and Fermi surface very well. Considering variations of the Fermi surface shapes depending on self-energy corrections and spin-orbit interactions, we discuss the formations of charge density wave (CDW) with different dielectric environments and their implications on recent controversial experimental results on CDW transition temperatures.

Growth and microtopographic study of CuInSe{sub 2} single crystals

DOE Office of Scientific and Technical Information (OSTI.GOV)

Chauhan, Sanjaysinh M.; Chaki, Sunil, E-mail: sunilchaki@yahoo.co.in; Deshpande, M. P.

2016-05-23

The CuInSe{sub 2} single crystals were grown by chemical vapour transport (CVT) technique using iodine as transporting agent. The elemental composition of the as-grown CuInSe{sub 2} single crystals was determined by energy dispersive analysis of X-ray (EDAX). The unit cell crystal structure and lattice parameters were determined by X-ray diffraction (XRD) technique. The surface microtopographic study of the as-grown CuInSe{sub 2} single crystals surfaces were done to study the defects, growth mechanism, etc. of the CVT grown crystals.

ENERGY CONVERSION FOR THE TRANSITION FROM Al TO γ-Al2O3 NANOPARTICLES

NASA Astrophysics Data System (ADS)

Wang, Shulin; Li, Shengjuan; Xu, Bo; Jian, Dunliang; Zhu, Yufang

2013-07-01

We have successfully converted large volume Al particles into γ-Al2O3 nanostructures by vibration milling at room temperature and successive treatment. We show that there exist special relationships among stacking fault energy (SFE), strain energy (SRE), and surface energy (SE) of the materials, including interdependence, intercompetition, and interconversion during the phase transition. SFE and SRE perform the same changing tendency, while SE just does the opposite. However, it is not the particle size but the energy state that determines the reactivity of the materials. And it is the SE that can directly determine the physical chemical reaction and the conversion into the end product rather than SFE and SRE. When SE goes up, the material reactivity and the product yield will be enhanced; and when SE goes down, the reaction and the product yield will decay. However, the state of SE depends closely on the change tendency of the SFE and SRE. That is, when SFE and SRE goes up, SE will goes down; if SFE and SRE goes down, SE will goes up. It seems that energy conservation law may be followed in a sense in the particle system if the external input keeps constant. The work may be significant for energy conversion in nano-scale and mechanosynthesis of oxide nanoparticles.

Intrinsic Josephson junction behaviour of the low Tc superconductor (LaSe) 1.14(NbSe 2)

NASA Astrophysics Data System (ADS)

Kačmarčík, J.; Szabó, P.; Samuely, P.; Rodrigo, J. G.; Suderow, H.; Vieira, S.; Lafond, A.; Meerschaut, A.

2008-04-01

Interlayer magnetotransport measurements on the highly anisotropic (LaSe)1.14(NbSe2) superconductor with Tc ∼ 1.2 K have indicated that this layered compound represents a model system of intrinsic Josephson junctions [P. Szabó et al., Phys. Rev. Lett. 86 (2001) 5990]. Scanning tunneling microscopy at room temperature and tunneling spectroscopy measurements at very low temperatures are presented in this work. STM imaging has revealed the presence of two types of surfaces which can be attributed to the appearance of LaSe or NbSe2 layers on the surface. The use of STM tip made of superconducting lead enabled a precise measurement of the temperature dependence of the superconducting energy gap Δ(T) on the NbSe2 layer. Δ(T) obtained from the surface sensitive STS data support the scenario obtained from our previous interlayer - ergo bulk sensitive magnetotransport measurements.

Ab initio calculation of pentacene-PbSe hybrid interface for photovoltaic applications.

PubMed

Roy, P; Nguyen, Thao P

2016-07-21

We perform density functional theory (DFT) quantum chemical calculations for the pentacene-PbSe hybrid interface at both molecular and crystal levels. At the interface, the parallel orientation of pentacene on the PbSe surface is found to be the most favorable, analogous to a pentacene-gold interface. The molecule-surface distance and the value of charge transfer from one pentacene molecule to the PbSe surface are estimated at around 4.15 Å and 0.12 e(-) respectively. We found that, standard-LDA/GGA-PBE/hybrid/meta-GGA xc-functionals incorrectly determine the band gaps of both pentacene and PbSe and leads to a failed prediction of the energy alignment in this system. So, we use a relativistic G0W0 functional and accurately model the electronic properties of pentacene and PbSe in both bulk material and near the interface. An energy shift of 0.23 eV, due to the difference in work function at the interface was supplemented after a detailed analysis of the electrostatic potential. The highest occupied molecular orbital level of pentacene is 0.01 eV above PbSe while the lowest unoccupied molecular orbital of pentacene lies 1.70 eV above PbSe, allowing both electrons and holes to transfer along the donor-acceptor junction. Our results provide additional insights into the electronic structure properties of the pentacene-PbSe heterojunction and establish it as a promising and efficient candidate for photovoltaic applications.

Surface roughness estimation of MBE grown CdTe/GaAs(211)B by ex-situ spectroscopic ellipsometry

DOE Office of Scientific and Technical Information (OSTI.GOV)

Karakaya, Merve, E-mail: mervegunnar@iyte.edu.tr; Bilgilisoy, Elif; Arı, Ozan

Spectroscopic ellipsometry (SE) ranging from 1.24 eV to 5.05 eV is used to obtain the film thickness and optical properties of high index (211) CdTe films. A three-layer optical model (oxide/CdTe/GaAs) was chosen for the ex-situ ellipsometric data analysis. Surface roughness cannot be determined by the optical model if oxide is included. We show that roughness can be accurately estimated, without any optical model, by utilizing the correlation between SE data (namely the imaginary part of the dielectric function, or phase angle, ψ) and atomic force microscopy (AFM) roughness. and ψ values at 3.31 eV, which corresponds to E{sub 1}more » critical transition energy of CdTe band structure, are chosen for the correlation since E{sub 1} gives higher resolution than the other critical transition energies. On the other hand, due to the anisotropic characteristic of (211) oriented CdTe surfaces, SE data ( and ψ) shows varieties for different azimuthal angle measurements. For this reason, in order to estimate the surface roughness by considering these correlations, it is shown that SE measurements need to be taken at the same surface azimuthal angle. Estimating surface roughness in this manner is an accurate way to eliminate cumbersome surface roughness measurement by AFM.« less

Selenidation of epitaxial silicene on ZrB2

NASA Astrophysics Data System (ADS)

Wiggers, F. B.; Yamada-Takamura, Y.; Kovalgin, A. Y.; de Jong, M. P.

2018-01-01

The deposition of elemental Se on epitaxial silicene on ZrB2 thin films was investigated with synchrotron-based core-level photoelectron spectroscopy and low-energy electron diffraction. The deposition of Se at room temperature caused the appearance of Si 2p peaks with chemical shifts of n × 0.51 ± 0.04 eV (n = 1-4), suggesting the formation of SiSe2. This shows that capping the silicene monolayer, without affecting its structural and electronic properties, is not possible with Se. The annealing treatments that followed caused the desorption of Se and Si, resulting in the etching of the Si atoms formerly part of the silicene layer, and the formation of bare ZrB2(0001) surface area. In addition, a ZrB2(0001)-(√7 × 3)R40.9° surface reconstruction was observed, attributed to a Se-termination of the surface of the transition metal diboride thin film.

Surface atomic structure characterization of SnSe and black phosphorus using selected area uLEED-IV via LEEM

NASA Astrophysics Data System (ADS)

Dai, Zhongwei; Grady, Maxwell; Yu, Jiexiang; Zang, Jiadong; Pohl, Karsten; Jin, Wencan; Kim, Young Duck; Hone, James; Dadap, Jerry; Osgood, Richard; Sadowski, Jerzy; Vishwanath, Suresh; Xing, Huili

Selected area diffraction intensity-voltage (μLEED-IV) analysis via low energy electron microscopy (LEEM) has the combined functionality of atomic surface structure determination and μm area selectivity, making it ideal for structural investigations of 2-D materials. SnSe thin films have been predicted and observed to be topological crystalline insulators. Previous studies suggested that SnSe has a preferred Se-terminated surface configuration. Using μLEED-IV, we determined that SnSe has, on the contrary, a stable Sn termination. This surface is stabilized through an oscillatory interlayer relaxation, which agrees with previous DFT predictions. Black phosphorus (BP) has an intrinsic layer-dependent bandgap ranging from 0.3 eV to 2 eV. Previous STM and DFT studies suggested BP surfaces have a buckling of 0.02 Å to 0.06 Å. We experimentally determined that the surface buckling of BP to be near 0.2 Å. We further propose, using DFT calculations, that this large surface buckling is induced by the presence of surface defects. The influence of this surface buckling on the electronic structures of BP is under investigation.

Controlled growth of ZnO/Zn₁-xPbxSe core-shell nanowires and their interfacial electronic energy alignment.

PubMed

Chen, Z H; Yeung, S Y; Li, H; Qian, J C; Zhang, W J; Li, Y Y; Bello, I

2012-05-21

ZnO/Zn(1-x)Pb(x)Se core-shell nanowires (NWs) have been synthesized by a solution based surface ion transfer method at various temperatures. The energy dispersive spectroscopic (EDS) mapping of single NWs suggests that the Zn, Pb and Se atoms are uniformly distributed in their shell layers. The ternary Zn(1-x)Pb(x)Se layers with tunable bandgaps extend the band-edge of optical absorption from 450 nm to 700 nm contrasting with the binary ZnSe layers. The ultraviolet photoelectron spectroscopic (UPS) analysis reveals a transition from the type I to type II band alignment when the x fraction decreases from 0.66 to the value of 0.36 in the nanoshell layers. This quantitative investigation of electronic energy levels at ZnO and Zn(1-x)Pb(x)Se interfaces indicates that the proper type II band alignment is well suited for photovoltaic energy conversion. The photovoltaic cells comprising a ZnO/Zn(1-x)Pb(x)Se nano-heterojunction with the optimized Pb content are expected to be more efficient than the devices sensitized by binary ZnSe or PbSe.

Energy deposition by heavy ions: Additivity of kinetic and potential energy contributions in hillock formation on CaF2

PubMed Central

Wang, Y. Y.; Grygiel, C.; Dufour, C.; Sun, J. R.; Wang, Z. G.; Zhao, Y. T.; Xiao, G. Q.; Cheng, R.; Zhou, X. M.; Ren, J. R.; Liu, S. D.; Lei, Y.; Sun, Y. B.; Ritter, R.; Gruber, E.; Cassimi, A.; Monnet, I.; Bouffard, S.; Aumayr, F.; Toulemonde, M.

2014-01-01

Modification of surface and bulk properties of solids by irradiation with ion beams is a widely used technique with many applications in material science. In this study, we show that nano-hillocks on CaF2 crystal surfaces can be formed by individual impact of medium energy (3 and 5 MeV) highly charged ions (Xe22+ to Xe30+) as well as swift (kinetic energies between 12 and 58 MeV) heavy xenon ions. For very slow highly charged ions the appearance of hillocks is known to be linked to a threshold in potential energy (Ep) while for swift heavy ions a minimum electronic energy loss per unit length (Se) is necessary. With our results we bridge the gap between these two extreme cases and demonstrate, that with increasing energy deposition via Se the Ep-threshold for hillock production can be lowered substantially. Surprisingly, both mechanisms of energy deposition in the target surface seem to contribute in an additive way, which can be visualized in a phase diagram. We show that the inelastic thermal spike model, originally developed to describe such material modifications for swift heavy ions, can be extended to the case where both kinetic and potential energies are deposited into the surface. PMID:25034006

Energy deposition by heavy ions: additivity of kinetic and potential energy contributions in hillock formation on CaF2.

PubMed

Wang, Y Y; Grygiel, C; Dufour, C; Sun, J R; Wang, Z G; Zhao, Y T; Xiao, G Q; Cheng, R; Zhou, X M; Ren, J R; Liu, S D; Lei, Y; Sun, Y B; Ritter, R; Gruber, E; Cassimi, A; Monnet, I; Bouffard, S; Aumayr, F; Toulemonde, M

2014-07-18

Modification of surface and bulk properties of solids by irradiation with ion beams is a widely used technique with many applications in material science. In this study, we show that nano-hillocks on CaF2 crystal surfaces can be formed by individual impact of medium energy (3 and 5 MeV) highly charged ions (Xe(22+) to Xe(30+)) as well as swift (kinetic energies between 12 and 58 MeV) heavy xenon ions. For very slow highly charged ions the appearance of hillocks is known to be linked to a threshold in potential energy (Ep) while for swift heavy ions a minimum electronic energy loss per unit length (Se) is necessary. With our results we bridge the gap between these two extreme cases and demonstrate, that with increasing energy deposition via Se the Ep-threshold for hillock production can be lowered substantially. Surprisingly, both mechanisms of energy deposition in the target surface seem to contribute in an additive way, which can be visualized in a phase diagram. We show that the inelastic thermal spike model, originally developed to describe such material modifications for swift heavy ions, can be extended to the case where both kinetic and potential energies are deposited into the surface.

Two-photon photoemission study of competing Auger and surface-mediated relaxation of hot electrons in CdSe quantum dot solids.

PubMed

Sippel, Philipp; Albrecht, Wiebke; Mitoraj, Dariusz; Eichberger, Rainer; Hannappel, Thomas; Vanmaekelbergh, Daniel

2013-04-10

Solids composed of colloidal quantum dots hold promise for third generation highly efficient thin-film photovoltaic cells. The presence of well-separated conduction electron states opens the possibility for an energy-selective collection of hot and equilibrated carriers, pushing the efficiency above the one-band gap limit. However, in order to reach this goal the decay of hot carriers within a band must be better understood and prevented, eventually. Here, we present a two-photon photoemission study of the 1Pe→1Se intraband relaxation dynamics in a CdSe quantum dot solid that mimics the active layer in a photovoltaic cell. We observe fast hot electron relaxation from the 1Pe to the 1Se state on a femtosecond-scale by Auger-type energy donation to the hole. However, if the oleic acid capping is exchanged for hexanedithiol capping, fast deep hole trapping competes efficiently with this relaxation pathway, blocking the Auger-type electron-hole energy exchange. A slower decay becomes then visible; we provide evidence that this is a multistep process involving the surface.

Electronic structures of of PuX (X=S, Se, Te)

NASA Astrophysics Data System (ADS)

Maehira, Takahiro; Sakai, Eijiro; Tatetsu, Yasutomi

2013-08-01

We have calculated the energy band structures and the Fermi surfaces of PuS, PuSe, and PuTe by using a self-consistent relativistic linear augmented-plane-wave method with the exchange and correlation potential in the local density approximation. In general, the energy bands near the Fermi level are mainly caused by the hybridization between the Pu 5 f and the monochalcogenide p electrons. The obtained main Fermi surfaces consisted of two hole sheets and one electron sheet, which were constructed from the band having both the Pu 5 f state and the monochalcogenide p state.

Growth and optical properties of Dy doped and undoped n-type InSe single crystal

NASA Astrophysics Data System (ADS)

Gürbulak, B.

1999-02-01

Undoped n-InSe and Dy doped n-InSe (n-InSe : Dy) single crystals were grown by a method which is similar to direct freezing method. Ingots had no cracks and voids on the surface. There were no processes to polish and clean treatment at cleavage faces of these samples because of the natural mirror-like cleavage faces. The absorption measurements were carried out in n-InSe and n-InSe : Dy samples in the temperature range 10-320 K. The first exciton energies for n=1 were calculated as 1.331, 1.248 eV in n-InSe and were 1.326, 1.244 eV in n-InSe : Dy at 10 and 300 K, respectively. The second exciton energies for n=2 in n-InSe were calculated as 1.346, 1.336 eV and in n-InSe : Dy were 1.340, 1.332 eV at 10 and 80 K, respectively. Binding energies of n-InSe and n-InSe : Dy were calculated as 19.47 and 18.87 meV, respectively. The direct bands gap for n-InSe are 1.350, 1.267 eV and for n-InSe : Dy are 1.344, 1.263 eV at 10, 300 K, respectively.

Ubiquitous strong electron–phonon coupling at the interface of FeSe/SrTiO3

PubMed Central

Zhang, Chaofan; Liu, Zhongkai; Chen, Zhuoyu; Xie, Yanwu; He, Ruihua; Tang, Shujie; He, Junfeng; Li, Wei; Jia, Tao; Rebec, Slavko N.; Ma, Eric Yue; Yan, Hao; Hashimoto, Makoto; Lu, Donghui; Mo, Sung-Kwan; Hikita, Yasuyuki; Moore, Robert G.; Hwang, Harold Y.; Lee, Dunghai; Shen, Zhixun

2017-01-01

The observation of replica bands in single-unit-cell FeSe on SrTiO3 (STO)(001) by angle-resolved photoemission spectroscopy (ARPES) has led to the conjecture that the coupling between FeSe electrons and the STO phonons are responsible for the enhancement of Tc over other FeSe-based superconductors. However the recent observation of a similar superconducting gap in single-unit-cell FeSe/STO(110) raised the question of whether a similar mechanism applies. Here we report the ARPES study of the electronic structure of FeSe/STO(110). Similar to the results in FeSe/STO(001), clear replica bands are observed. We also present a comparative study of STO(001) and STO(110) bare surfaces, and observe similar replica bands separated by approximately the same energy, indicating this coupling is a generic feature of the STO surfaces and interfaces. Our findings suggest that the large superconducting gaps observed in FeSe films grown on different STO surface terminations are likely enhanced by a common mechanism. PMID:28186084

Ubiquitous strong electron–phonon coupling at the interface of FeSe/SrTiO 3

DOE PAGES

Zhang, Chaofan; Liu, Zhongkai; Chen, Zhuoyu; ...

2017-02-10

The observation of replica bands in single-unit-cell FeSe on SrTiO 3 (STO)(001) by angle-resolved photoemission spectroscopy (ARPES) has led to the conjecture that the coupling between FeSe electrons and the STO phonons are responsible for the enhancement of T c over other FeSe-based superconductors. However the recent observation of a similar superconducting gap in single-unit-cell FeSe/STO(110) raised the question of whether a similar mechanism applies. Here we report the ARPES study of the electronic structure of FeSe/STO(110). Similar to the results in FeSe/STO(001), clear replica bands are observed. We also present a comparative study of STO(001) and STO(110) bare surfaces,more » and observe similar replica bands separated by approximately the same energy, indicating this coupling is a generic feature of the STO surfaces and interfaces. Lastly, our findings suggest that the large superconducting gaps observed in FeSe films grown on different STO surface terminations are likely enhanced by a common mechanism.« less

Symmetry analysis of strain, electric and magnetic fields in the Bi2Se3-class of topological insulators

NASA Astrophysics Data System (ADS)

Rosdahl Brems, Mathias; Paaske, Jens; Lunde, Anders Mathias; Willatzen, Morten

2018-05-01

Based on group theoretical arguments we derive the most general Hamiltonian for the Bi2Se3-class of materials including terms to third order in the wave vector, first order in electric and magnetic fields, first order in strain and first order in both strain and wave vector. We determine analytically the effects of strain on the electronic structure of Bi2Se3. For the most experimentally relevant surface termination we analytically derive the surface state (SS) spectrum, revealing an anisotropic Dirac cone with elliptical constant energy contours giving rise to a direction-dependent group velocity. The spin-momentum locking of strained Bi2Se3 is shown to be modified. Hence, strain control can be used to manipulate the spin degree of freedom via the spin–orbit coupling. We show that for a thin film of Bi2Se3 the SS band gap induced by coupling between the opposite surfaces changes opposite to the bulk band gap under strain. Tuning the SS band gap by strain, gives new possibilities for the experimental investigation of the thickness dependent gap and optimization of optical properties relevant for, e.g., photodetector and energy harvesting applications. We finally derive analytical expressions for the effective mass tensor of the Bi2Se3 class of materials as a function of strain and electric field.

Unimolecular rearrangement of the simplest compound models with a selenium-oxygen, selenium-sulphur and selenium-selenium bond: SeXH and HSeXH (X = O,S,Se)

NASA Astrophysics Data System (ADS)

Viana, Rommel B.

2017-04-01

The aim of this study was to characterise the simplest compound models with a selenium-oxygen, selenium-sulphur and selenium-selenium bond as the SeXH and HSeXH isomers (X = O,S,Se). One of the main aspects of this investigation was to provide a description on the isomerisation pathways involving 2[H,Se,X] and 1[2H,Se,X] potential energy surfaces calculated at the CCSD(T)/CBS//MP2/cc-pVTZ level. The energy difference was 13 kcal mol-1 between hydroxyselenide (SeOH) and oxoselenium (HSeO), while a gap of 3 kcal mol-1 was predicted between thiol-selenide (SeSH) and selenol-sulphide (HSeS). The SeOH→HSeO unimolecular rearrangement showed a barrier energy of 44.6 kcal mol-1, decreasing almost two times in sulphur and selenium analogous reactions. In addition, hydroxyselenide (HSeOH), thioselenenic acid (HSeSH) and diselane (HSeSeH) were the global minimum configurations in the ground state, while the energy differences among the other isomers were close to 30 kcal mol-1. The HSeXH→H2SeX and HSeXH→SeXH2 isomerisations showed barrier energies ranging from 40 to 65 kcal mol-1, while these reverse routes presented heights that were three times smaller. The kinetic rate constant of each 1,2-H shift reaction was performed here as well as an analysis of the selenium-chalcogen bonds using natural bond orbital and bond order index methodologies.

Distinct effects of Cr bulk doping and surface deposition on the chemical environment and electronic structure of the topological insulator Bi2Se3

NASA Astrophysics Data System (ADS)

Yilmaz, Turgut; Hines, William; Sun, Fu-Chang; Pletikosić, Ivo; Budnick, Joseph; Valla, Tonica; Sinkovic, Boris

2017-06-01

In this report, it is shown that Cr doped into the bulk and Cr deposited on the surface of Bi2Se3 films produced by molecular beam epitaxy (MBE) have strikingly different effects on both the electronic structure and chemical environment. Angle resolved photoemission spectroscopy (ARPES) shows that Cr doped into the bulk opens a surface state energy gap which can be seen at room temperature; much higher than the measured ferromagnetic transition temperature of ≈10 K. On the other hand, similar ARPES measurements show that the surface states remain gapless down to 15 K for films with Cr surface deposition. In addition, core-level photoemission spectroscopy of the Bi 5d, Se 3d, and Cr 3p core levels show distinct differences in the chemical environment for the two methods of Cr introduction. Surface deposition of Cr results in the formation of shoulders on the lower binding energy side for the Bi 5d peaks and two distinct Cr 3p peaks indicative of two Cr sites. These striking differences suggests an interesting possibility that better control of doping at only near surface region may offer a path to quantum anomalous Hall states at higher temperatures than reported in the literature.

New quaternary thallium indium germanium selenide TlInGe2Se6: Crystal and electronic structure

NASA Astrophysics Data System (ADS)

Khyzhun, O. Y.; Parasyuk, O. V.; Tsisar, O. V.; Piskach, L. V.; Myronchuk, G. L.; Levytskyy, V. O.; Babizhetskyy, V. S.

2017-10-01

Crystal structure of a novel quaternary thallium indium germanium selenide TlInGe2Se6 was investigated by means of powder X-ray diffraction method. It was determined that the compound crystallizes in the trigonal space group R3 with the unit cell parameters a = 10.1798(2) Å, c = 9.2872(3) Å. The relationship with similar structures was discussed. The as-synthesized TlInGe2Se6 ingot was tested with X-ray photoelectron spectroscopy (XPS) and X-ray emission spectroscopy (XES). In particular, the XPS valence-band and core-level spectra were recorded for initial and Ar+ ion-bombarded surfaces of the sample under consideration. The XPS data allow for statement that the TlInGe2Se6 surface is rigid with respect to Ar+ ion-bombardment. Particularly, Ar+ ion-bombardment (3.0 keV, 5 min duration, ion current density fixed at 14 μA/cm2) did not cause substantial modifications of stoichiometry in topmost surface layers. Furthermore, comparison on a common energy scale of the XES Se Kβ2 and Ge Kβ2 bands and the XPS valence-band spectrum reveals that the principal contributions of the Se 4p and Ge 4p states occur in the upper and central portions of the valence band of TlInGe2Se6, respectively, with also their substantial contributions in other portions of the band. The bandgap energy of TlInGe2Se6 at the level of αg=103 cm-1 is equal to 2.38 eV at room temperature.

Aeolian contamination of Se and Ag in the North Pacific from Asian fossil fuel combustion.

PubMed

Ranville, Mara A; Cutter, Gregory A; Buck, Clifton S; Landing, William M; Cutter, Lynda S; Resing, Joseph A; Flegal, A Russell

2010-03-01

Energy production from fossil fuels, and in particular the burning of coal in China, creates atmospheric contamination that is transported across the remote North Pacific with prevailing westerly winds. In recent years this pollution from within Asia has increased dramatically, as a consequence of vigorous economic growth and corresponding energy consumption. During the fourth Intergovernmental Oceanographic Commission baseline contaminant survey in the western Pacific Ocean from May to June, 2002, surface waters and aerosol samples were measured to investigate whether atmospheric deposition of trace elements to the surface North Pacific was altering trace element biogeochemical cycling. Results show a presumably anthropogenic enrichment of Ag and of Se, which is a known tracer of coal combustion, in the North Pacific atmosphere and surface waters. Additionally, a strong correlation was seen between dissolved Ag and Se concentrations in surface waters. This suggests that Ag should now also be considered a geochemical tracer for coal combustion, and provides further evidence that Ag exhibits a disturbed biogeochemical cycle as the result of atmospheric deposition to the North Pacific.

Application of quantum dots CdZnSeS / ZnS luminescence, enhanced by plasmons of silver rough surface for detection of albumin in blood facies of infected person

NASA Astrophysics Data System (ADS)

Konstantinova, E.; Zyubin, A.; Moiseeva, E.; Matveeva, K.; Slezhkin, V.; Samusev, I.; Bryukhanov, V.

2017-12-01

The study of the luminescence of CdZnSeS / ZnS quantum dots (QDs) absorbed on the rough surface of a silver film, including the energy transfer between human serum albumin molecules, isolated from the blood plasma of healthy and infected with sepsis patients, was performed by spectral-kinetic methods.

Designed Long-Lived Emission from CdSe Quantum Dots through Reversible Electronic Energy Transfer with a Surface-Bound Chromophore.

PubMed

La Rosa, Marcello; Denisov, Sergey A; Jonusauskas, Gediminas; McClenaghan, Nathan D; Credi, Alberto

2018-03-12

The size-tunable emission of luminescent quantum dots (QDs) makes them highly interesting for applications that range from bioimaging to optoelectronics. For the same applications, engineering their luminescence lifetime, in particular, making it longer, would be as important; however, no rational approach to reach this goal is available to date. We describe a strategy to prolong the emission lifetime of QDs through electronic energy shuttling to the triplet excited state of a surface-bound molecular chromophore. To implement this idea, we made CdSe QDs of different sizes and carried out self-assembly with a pyrene derivative. We observed that the conjugates exhibit delayed luminescence, with emission decays that are prolonged by more than 3 orders of magnitude (lifetimes up to 330 μs) compared to the parent CdSe QDs. The mechanism invokes unprecedented reversible quantum dot to organic chromophore electronic energy transfer. © 2018 The Authors. Published by Wiley-VCH Verlag GmbH & Co. KGaA.

Electron Phonon Coupling versus Photoelectron Energy Loss at the Origin of Replica Bands in Photoemission of FeSe on SrTiO3

NASA Astrophysics Data System (ADS)

Li, Fengmiao; Sawatzky, George A.

2018-06-01

The recent observation of replica bands in single-layer FeSe /SrTiO3 by angle-resolved photoemission spectroscopy (ARPES) has triggered intense discussions concerning the potential influence of the FeSe electrons coupling with substrate phonons on the superconducting transition temperature. Here we provide strong evidence that the replica bands observed in the single-layer FeSe /SrTiO3 system and several other cases are largely due to the energy loss processes of the escaping photoelectron, resulted from the well-known strong coupling of external propagating electrons to Fuchs-Kliewer surface phonons in ionic materials in general. The photoelectron energy loss in ARPES on single-layer FeSe /SrTiO3 is calculated using the demonstrated successful semiclassical dielectric theory in describing low energy electron energy loss spectroscopy of ionic insulators. Our result shows that the observed replica bands are mostly a result of extrinsic photoelectron energy loss and not a result of the electron phonon interaction of the Fe d electrons with the substrate phonons. The strong enhancement of the superconducting transition temperature in these monolayers remains an open question.

Quasiparticle interference, quasiparticle interactions, and the origin of the charge density wave in 2H-NbSe2.

PubMed

Arguello, C J; Rosenthal, E P; Andrade, E F; Jin, W; Yeh, P C; Zaki, N; Jia, S; Cava, R J; Fernandes, R M; Millis, A J; Valla, T; Osgood, R M; Pasupathy, A N

2015-01-23

We show that a small number of intentionally introduced defects can be used as a spectroscopic tool to amplify quasiparticle interference in 2H-NbSe2 that we measure by scanning tunneling spectroscopic imaging. We show, from the momentum and energy dependence of the quasiparticle interference, that Fermi surface nesting is inconsequential to charge density wave formation in 2H-NbSe2. We demonstrate that, by combining quasiparticle interference data with additional knowledge of the quasiparticle band structure from angle resolved photoemission measurements, one can extract the wave vector and energy dependence of the important electronic scattering processes thereby obtaining direct information both about the fermiology and the interactions. In 2H-NbSe2, we use this combination to confirm that the important near-Fermi-surface electronic physics is dominated by the coupling of the quasiparticles to soft mode phonons at a wave vector different from the charge density wave ordering wave vector.

Surface Modification of Cu(In,Ga)Se2 Grains

NASA Astrophysics Data System (ADS)

Alruqobah, Essam H.

Nearly all of the world’s energy demand today is being met by the use of non-renewable energy sources. With the worldwide energy demand projected to increase in the coming years, it is vital to find alternative and renewable energy sources. Among the available renewable energy sources, solar energy is the most promising in meeting the worldwide energy demand. Recently, thin film solar cells have garnered attention due to their thinner architecture and relatively high optical absorption coefficients, as opposed to the conventional crytslline silicon solar cells. One of the most promising thin-film solar cell absorber materials is Cu(In,Ga)Se2 (CIGSe), achieving power conversion efficiencies approaching those of crystalline Si. The highest efficiency CIGSe devices were made via costly vacuum-based co-evaporation process. CIGSe devices made from solution-processed methods have also garnered attention due to their lower costs, and their efficiencies have increased considerably in recent years. In this thesis, CIGSe absorber layers are fabricated via the solution-processed from nanoparticle-based sulfide CIGS. The most important step in fabrication of a CIGSe solar cell absorber layer is the selenization step, which is the thermal sintering of a CIGSe precursor layer in the presence of selenium vapor to achieve large, dense selenide grains that are required for adequate PV performance. It is determined that maintaining adequate selenium vapor pressure on the substrate during the selenization and subsequent cooldown is crucial in producing high efficiency solar cell devices. Furthermore, exposing the CIGSe grains to a Se-deficient atmosphere causes Se to evaporate from the grains, and subsequently modifying the CIGSe grain surface. The modified grain surface adversely impacts the PV performance of the final solar cell device by forming defects due to the decrease in selenium concentration. These defects are manifested in increased current shunting, and decrease the overall efficiency of the device.

Layer structured bismuth selenides Bi2Se3 and Bi3Se4 for high energy and flexible all-solid-state micro-supercapacitors.

PubMed

Hao, Chunxue; Wang, Lidan; Wen, Fusheng; Xiang, Jianyong; Li, Lei; Hu, Wentao; Liu, Zhongyuan

2018-01-19

In this work, bismuth selenides (Bi 2 Se 3 and Bi 3 Se 4 ), both of which have a layered rhombohedral crystal structure, have been found to be useful as electrode materials for supercapacitor applications. In a liquid electrolyte system (6M KOH), Bi 2 Se 3 nanoplates exhibit much better performance as an electrode material than Bi 3 Se 4 nanoparticles do, delivering a higher specific capacitance (272.9 F g -1 ) than that of Bi 3 Se 4 (193.6 F g -1 ) at 5 mV s -1 . This result may be attributed to the fact that Bi 2 Se 3 nanoplates possess more active electrochemical surfaces for the reversible surface redox reactions owing to their planar quintuple stacked layers (septuple layers for Bi 3 Se 4 ). To meet the demands of electronic skin, we used a novel flexible annular interdigital structure electrode to support the all-solid-state micro-supercapacitors (AMSCs). The Bi 2 Se 3 AMSC device delivers a much better supercapacitor performance, exhibits a large stack capacitance of 89.5 F cm -3 at 20 mV s -1 (Bi 3 Se 4 : 79.1 F cm -3 ), a high energy density of 17.9 mWh cm -3 and a high power density of 18.9 W cm -3 . The bismuth selenides also exhibit good cycle stability, with 95.5% retention after 1000 c for Bi 2 Se 3 (Bi 3 Se 4 :90.3%). Clearly, Bi 2 Se 3 nanoplates can be promising electrode materials for flexible annular interdigital AMSCs.

Layer Structured Bismuth Selenides of Bi₂Se₃ and Bi₃Se₄ for High Energy and Flexible All-Solid-State Micro-Supercapacitors.

PubMed

Hao, Chunxue; Wang, Lidan; Wen, Fusheng; Xiang, Jianyong; Li, Lei; Hu, Wentao; Liu, Zhongyuan

2017-12-20

Bismuth selenides (Bi2Se3 and Bi3Se4), both of which have the layered rhombohedral crystal structure, and found to be useful as electrode materials for supercapacitor application in this work. Bi2Se3 nanoplates as electrode material exhibit much better performance than that of Bi3Se4 nanoparticles in liquid electrolyte system (6 M KOH), which delivers a higher specific capacitance (272.9 F/g) than that of Bi3Se4 (193.6 F/g) at 5 mV/s. This result would may be attributed to that Bi2Se3 nanoplates possess more active electrochemical surfaces for the reversible surface redox reactions owing to its planar quintuple stacked layers (septuple layers for Bi3Se4). For the demand of electronic skin, we used a novel flexible annular interdigital structure electrode applying for all-solid-state micro-supercapacitors (AMSCs). Bi2Se3 AMSCs device delivers a much more excellent supercapacitor performance, exhibits a large stack capacitance 89.5 F/cm3 (Bi3Se4: 79.1 F/cm3) at 20 mV/s, a high energy density 17.9 mWh/cm3 and high power density 18.9 W/cm3. The bismuth selenides also exhibit good cycle stability, retention 95.5% (90.3%) after 1000 c for Bi2Se3 (Bi3Se4). Obviously, Bi2Se3 nanoplates can be promising electrode materials for flexible annular interdigital all-solid-sate supercapacitor. © 2017 IOP Publishing Ltd.

Layer structured bismuth selenides Bi2Se3 and Bi3Se4 for high energy and flexible all-solid-state micro-supercapacitors

NASA Astrophysics Data System (ADS)

Hao, Chunxue; Wang, Lidan; Wen, Fusheng; Xiang, Jianyong; Li, Lei; Hu, Wentao; Liu, Zhongyuan

2018-02-01

In this work, bismuth selenides (Bi2Se3 and Bi3Se4), both of which have a layered rhombohedral crystal structure, have been found to be useful as electrode materials for supercapacitor applications. In a liquid electrolyte system (6M KOH), Bi2Se3 nanoplates exhibit much better performance as an electrode material than Bi3Se4 nanoparticles do, delivering a higher specific capacitance (272.9 F g-1) than that of Bi3Se4 (193.6 F g-1) at 5 mV s-1. This result may be attributed to the fact that Bi2Se3 nanoplates possess more active electrochemical surfaces for the reversible surface redox reactions owing to their planar quintuple stacked layers (septuple layers for Bi3Se4). To meet the demands of electronic skin, we used a novel flexible annular interdigital structure electrode to support the all-solid-state micro-supercapacitors (AMSCs). The Bi2Se3 AMSC device delivers a much better supercapacitor performance, exhibits a large stack capacitance of 89.5 F cm-3 at 20 mV s-1 (Bi3Se4: 79.1 F cm-3), a high energy density of 17.9 mWh cm-3 and a high power density of 18.9 W cm-3. The bismuth selenides also exhibit good cycle stability, with 95.5% retention after 1000 c for Bi2Se3 (Bi3Se4:90.3%). Clearly, Bi2Se3 nanoplates can be promising electrode materials for flexible annular interdigital AMSCs.

Impact of Antibody Bioconjugation on Emission and Energy Band Profile of CdSeTe/ZnS Quantum Dots

NASA Astrophysics Data System (ADS)

Torchynska, T. V.; Gomez, J. A. Jaramillo; Polupan, G.; Macotela, L. G. Vega

2018-03-01

The variation of the photoluminescence (PL) and Raman scattering spectra of CdSeTe/ZnS quantum dots (QDs) on conjugation to an antibody has been investigated. Two types of CdSeTe/ZnS QD with different emission wavelength (705 nm and 800 nm) were studied comparatively before and after conjugation to anti-pseudorabies virus antibody (AB). Nonconjugated QDs were characterized by Gaussian-type PL bands. PL shifts to higher energy and asymmetric shape of PL bands was detected in PL spectra of bioconjugated QDs. The surface-enhanced Raman scattering effect was exhibited by the bioconjugated CdSeTe/ZnS QDs, indicating that the excitation light used in the Raman study generated electric dipoles in the AB molecules. The optical bandgap of the CdSeTe core was calculated numerically as a function of its radius based on an effective mass approximation model. The energy band diagrams for non- and bioconjugated CdSeTe/ZnS QDs were obtained, revealing a type II quantum well in the CdSeTe core. The calculations show that AB dipoles, excited in the bioconjugated QDs, stimulate a change in the energy band diagram of the QDs that alters the PL spectrum. These results could be useful for improving the sensitivity of QD biosensors.

An ab initio investigation of Bi2Se3 topological insulator deposited on amorphous SiO2.

PubMed

de Oliveira, I S S; Scopel, W L; Miwa, R H

2017-02-01

We use first-principles simulations to investigate the topological properties of Bi 2 Se 3 thin films deposited on amorphous SiO 2 , Bi 2 Se 3 /a-SiO 2 , which is a promising substrate for topological insulator (TI) based device applications. The Bi 2 Se 3 films are bonded to a-SiO 2 mediated by van der Waals interactions. Upon interaction with the substrate, the Bi 2 Se 3 topological surface and interface states remain present, however the degeneracy between the Dirac-like cones is broken. The energy separation between the two Dirac-like cones increases with the number of Bi 2 Se 3 quintuple layers (QLs) deposited on the substrate. Such a degeneracy breaking is caused by (i) charge transfer from the TI to the substrate and charge redistribution along the Bi 2 Se 3 QLs, and (ii) by deformation of the QL in contact with the a-SiO 2 substrate. We also investigate the role played by oxygen vacancies ([Formula: see text]) on the a-SiO 2 , which increases the energy splitting between the two Dirac-like cones. Finally, by mapping the electronic structure of Bi 2 Se 3 /a-SiO 2 , we found that the a-SiO 2 surface states, even upon the presence of [Formula: see text], play a minor role on gating the electronic transport properties of Bi 2 Se 3 .

Distinct effects of Cr bulk doping and surface deposition on the chemical environment and electronic structure of the topological insulator Bi 2 Se 3

DOE Office of Scientific and Technical Information (OSTI.GOV)

Yilmaz, Turgut; Hines, William; Sun, Fu-Chang

In this report, it is shown that Cr doped into the bulk and Cr deposited on the surface of Bi2Se3 films produced by molecular beam epitaxy (MBE) have strikingly different effects on both the electronic structure and chemical environment. Angle resolved photoemission spectroscopy (ARPES) shows that Cr doped into the bulk opens a surface state energy gap which can be seen at room temperature; much higher than the measured ferromagnetic transition temperature of ≈ 10 K. On the other hand, similar ARPES measurements show that the surface states remain gapless down to 15 K for films with Cr surface deposition.more » In addition, core-level photoemission spectroscopy of the Bi 5d, Se 3d, and Cr 3p core levels show distinct differences in the chemical environment for the two methods of Cr introduction. Surface deposition of Cr results in the formation of shoulders on the lower binding energy side for the Bi 5d peaks and two distinct Cr 3p peaks indicative of two Cr sites. These striking differences suggests an interesting possibility that better control of doping at only near surface region may offer a path to quantum anomalous Hall states at higher temperatures than reported in the literature.« less

Distinct effects of Cr bulk doping and surface deposition on the chemical environment and electronic structure of the topological insulator Bi 2 Se 3

DOE PAGES

Yilmaz, Turgut; Hines, William; Sun, Fu-Chang; ...

2017-02-21

In this report, it is shown that Cr doped into the bulk and Cr deposited on the surface of Bi2Se3 films produced by molecular beam epitaxy (MBE) have strikingly different effects on both the electronic structure and chemical environment. Angle resolved photoemission spectroscopy (ARPES) shows that Cr doped into the bulk opens a surface state energy gap which can be seen at room temperature; much higher than the measured ferromagnetic transition temperature of ≈ 10 K. On the other hand, similar ARPES measurements show that the surface states remain gapless down to 15 K for films with Cr surface deposition.more » In addition, core-level photoemission spectroscopy of the Bi 5d, Se 3d, and Cr 3p core levels show distinct differences in the chemical environment for the two methods of Cr introduction. Surface deposition of Cr results in the formation of shoulders on the lower binding energy side for the Bi 5d peaks and two distinct Cr 3p peaks indicative of two Cr sites. These striking differences suggests an interesting possibility that better control of doping at only near surface region may offer a path to quantum anomalous Hall states at higher temperatures than reported in the literature.« less

Amplified all-optical polarization phase modulator assisted by a local surface plasmon in Au-hybrid CdSe quantum dots.

PubMed

Kyhm, Kwangseuk; Je, Koo-Chul; Taylor, Robert A

2012-08-27

We propose an amplified all-optical polarization phase modulator assisted by a local surface plasmon in Au-hybrid CdSe quantum dots. When the local surface plasmon of a spherical Au quantum dot is in resonance with the exciton energy level of a CdSe quantum dot, a significant enhancement of the linear and nonlinear refractive index is found in both the real and imaginary terms via the interaction with the dipole field of the local surface plasmon. Given a gating pulse intensity, an elliptical polarization induced by the phase retardation is described in terms of elliptical and rotational angles. In the case that a larger excitation than the bleaching intensity is applied, the signal light can be amplified due to the presence of gain in the CdSe quantum dot. This enables a longer propagation of the signal light relative to the metal loss, resulting in more feasible polarization modulation.

Large Area Atomically Flat Surfaces via Exfoliation of Bulk Bi 2Se 3 Single Crystals

DOE Office of Scientific and Technical Information (OSTI.GOV)

Melamed, Celeste L.; Ortiz, Brenden R.; Gorai, Prashun

In this paper, we present an exfoliation method that produces cm 2-area atomically flat surfaces from bulk layered single crystals, with broad applications such as for the formation of lateral heterostructures and for use as substrates for van der Waals epitaxy. Single crystals of Bi 2Se 3 were grown using the Bridgman method and examined with X-ray reciprocal space maps, Auger spectroscopy, low-energy electron diffraction, and X-ray photoelectron spectroscopy. An indium-bonding exfoliation technique was developed that produces multiple ~100 um thick atomically flat, macroscopic (>1 cm 2) slabs from each Bi 2Se 3 source crystal. Two-dimensional X-ray diffraction and reciprocalmore » space maps confirm the high crystalline quality of the exfoliated surfaces. Atomic force microscopy reveals that the exfoliated surfaces have an average root-mean-square (RMS) roughness of ~0.04 nm across 400 μm 2 scans and an average terrace width of 70 um between step edges. First-principles calculations reveal exfoliation energies of Bi 2Se 3 and a number of other layered compounds, which demonstrate relevance of our method across the field of 2D materials. While many potential applications exist, excellent lattice matching with the III-V alloy space suggests immediate potential for the use of these exfoliated layered materials as epitaxial substrates for photovoltaic development.« less

Large Area Atomically Flat Surfaces via Exfoliation of Bulk Bi 2Se 3 Single Crystals

DOE PAGES

Melamed, Celeste L.; Ortiz, Brenden R.; Gorai, Prashun; ...

2017-09-12

In this paper, we present an exfoliation method that produces cm 2-area atomically flat surfaces from bulk layered single crystals, with broad applications such as for the formation of lateral heterostructures and for use as substrates for van der Waals epitaxy. Single crystals of Bi 2Se 3 were grown using the Bridgman method and examined with X-ray reciprocal space maps, Auger spectroscopy, low-energy electron diffraction, and X-ray photoelectron spectroscopy. An indium-bonding exfoliation technique was developed that produces multiple ~100 um thick atomically flat, macroscopic (>1 cm 2) slabs from each Bi 2Se 3 source crystal. Two-dimensional X-ray diffraction and reciprocalmore » space maps confirm the high crystalline quality of the exfoliated surfaces. Atomic force microscopy reveals that the exfoliated surfaces have an average root-mean-square (RMS) roughness of ~0.04 nm across 400 μm 2 scans and an average terrace width of 70 um between step edges. First-principles calculations reveal exfoliation energies of Bi 2Se 3 and a number of other layered compounds, which demonstrate relevance of our method across the field of 2D materials. While many potential applications exist, excellent lattice matching with the III-V alloy space suggests immediate potential for the use of these exfoliated layered materials as epitaxial substrates for photovoltaic development.« less

Growth of Bi2Se3 topological insulator thin film on Ge(1 1 1) substrate

NASA Astrophysics Data System (ADS)

Kim, Seungyeon; Lee, Sangsoo; Woo, Jeongseok; Lee, Geunseop

2018-02-01

Atomically smooth, single crystalline Bi2Se3 thin films were grown on a Ge(1 1 1) substrate using molecular beam epitaxy. Crystallinities of both the surface and the bulk as well as the stoichiometry of the grown film were characterized by using low-energy electron diffraction, scanning tunneling microscopy, X-ray diffraction, and photoelectron spectroscopies. Hexagonal atomic structures, quintuple layer steps observed in STM images confirmed that the Bi2Se3 film with a (0 0 0 1) surface was grown. Diffraction peak positions as well as the chemical composition determined from the core-level photoelectron spectra coincide well with those expected for the Bi2Se3 crystal. The surface state with a Dirac cone was observed in the valence photoelectron spectra, which also support that a high-quality Bi2Se3 film was grown on the Ge(1 1 1) substrate. The interface between Ge(1 1 1) and Bi2Se3(0 0 0 1) is expected to be abrupt due to the small lattice between them.

Quantum chemistry of the minimal CdSe clusters

NASA Astrophysics Data System (ADS)

Yang, Ping; Tretiak, Sergei; Masunov, Artëm E.; Ivanov, Sergei

2008-08-01

Colloidal quantum dots are semiconductor nanocrystals (NCs) which have stimulated a great deal of research and have attracted technical interest in recent years due to their chemical stability and the tunability of photophysical properties. While internal structure of large quantum dots is similar to bulk, their surface structure and passivating role of capping ligands (surfactants) are not fully understood to date. We apply ab initio wavefunction methods, density functional theory, and semiempirical approaches to study the passivation effects of substituted phosphine and amine ligands on the minimal cluster Cd2Se2, which is also used to benchmark different computational methods versus high level ab initio techniques. Full geometry optimization of Cd2Se2 at different theory levels and ligand coverage is used to understand the affinities of various ligands and the impact of ligands on cluster structure. Most possible bonding patterns between ligands and surface Cd/Se atoms are considered, including a ligand coordinated to Se atoms. The degree of passivation of Cd and Se atoms (one or two ligands attached to one atom) is also studied. The results suggest that B3LYP/LANL2DZ level of theory is appropriate for the system modeling, whereas frequently used semiempirical methods (such as AM1 and PM3) produce unphysical results. The use of hydrogen atom for modeling of the cluster passivating ligands is found to yield unphysical results as well. Hence, the surface termination of II-VI semiconductor NCs with hydrogen atoms often used in computational models should probably be avoided. Basis set superposition error, zero-point energy, and thermal corrections, as well as solvent effects simulated with polarized continuum model are found to produce minor variations on the ligand binding energies. The effects of Cd-Se complex structure on both the electronic band gap (highest occupied molecular orbital-lowest unoccupied molecular orbital energy difference) and ligand binding energies are systematically examined. The role played by positive charges on ligand binding is also explored. The calculated binding energies for various ligands L are found to decrease in the order OPMe3>OPH3>NH2Me>=NH3>=NMe3>PMe3>PH3 for neutral clusters and OPMe3>OPH3>PMe3>=NMe3>=NH2Me>=NH3>PH3 and OPMe3>OPH3>NH2Me>=NMe3>=PMe3>=NH3>PH3 for single and double ligations of positively charged Cd2Se22+ cluster, respectively.

Electronic properties of one-dimensional nanostructures of the Bi2Se3 topological insulator

NASA Astrophysics Data System (ADS)

Virk, Naunidh; Autès, Gabriel; Yazyev, Oleg V.

2018-04-01

We theoretically study the electronic structure and spin properties of one-dimensional nanostructures of the prototypical bulk topological insulator Bi2Se3 . Realistic models of experimentally observed Bi2Se3 nanowires and nanoribbons are considered using the tight-binding method. At low energies, the band structures are composed of a series of evenly spaced degenerate subbands resulting from circumferential confinement of the topological surface states. The direct band gaps due to the nontrivial π Berry phase show a clear dependence on the circumference. The spin-momentum locking of the topological surface states results in a pronounced 2 π spin rotation around the circumference with the degree of spin polarization dependent on the momentum along the nanostructure. Overall, the band structures and spin textures are more complicated for nanoribbons, which expose two distinct facets. The effects of reduced dimensionality are rationalized with the help of a simple model that considers circumferential quantization of the topological surface states. Furthermore, the surface spin density induced by an electric current along the nanostructure shows a pronounced oscillatory dependence on the charge-carrier energy, which can be exploited in spintronics applications.

Chemically prepared La2Se3 nanocubes thin film for supercapacitor application.

PubMed

Patil, S J; Lokhande, V C; Chodankar, N R; Lokhande, C D

2016-05-01

Lanthanum selenide (La2Se3) nanocubes thin film is prepared via successive ionic layer adsorption and reaction (SILAR) method and utilized for energy storage application. The prepared La2Se3 thin film is characterized by X-ray diffraction, field emission scanning electron microscopy and contact angle measurement techniques for structural, surface morphological and wettability studies, respectively. Energy dispersive X-ray microanalysis (EDAX) is performed in order to obtain the elemental composition of the thin film. The La2Se3 film electrode shows a maximum specific capacitance of 363 F g(-1) in a 0.8 M LiClO4/PC electrolyte at a scan rate of 5 mV s(-1) within 1.3 V/SCE potential range. The specific capacitive retention of 83 % of La2Se3 film electrode is obtained over 1000 cyclic voltammetry cycles. The predominant performance, such as high energy (80 Wh kg(-1)) and power density (2.5 kW kg(-1)), indicates that La2Se3 film electrode facilitates fast ion diffusion during redox processes. Copyright © 2016 Elsevier Inc. All rights reserved.

Slow-muon study of quaternary solar-cell materials: Single layers and p -n junctions

NASA Astrophysics Data System (ADS)

Alberto, H. V.; Vilão, R. C.; Vieira, R. B. L.; Gil, J. M.; Weidinger, A.; Sousa, M. G.; Teixeira, J. P.; da Cunha, A. F.; Leitão, J. P.; Salomé, P. M. P.; Fernandes, P. A.; Törndahl, T.; Prokscha, T.; Suter, A.; Salman, Z.

2018-02-01

Thin films and p -n junctions for solar cells based on the absorber materials Cu (In ,G a ) Se2 and Cu2ZnSnS4 were investigated as a function of depth using implanted low energy muons. The most significant result is a clear decrease of the formation probability of the Mu+ state at the heterojunction interface as well as at the surface of the Cu (In ,G a ) Se2 film. This reduction is attributed to a reduced bonding reaction of the muon in the absorber defect layer at its surface. In addition, the activation energies for the conversion from a muon in an atomiclike configuration to a anion-bound position are determined from temperature-dependence measurements. It is concluded that the muon probe provides a measurement of the effective surface defect layer width, both at the heterojunctions and at the films. The CIGS surface defect layer is crucial for solar-cell electrical performance and additional information can be used for further optimizations of the surface.

Fermi level pinning characterisation on ammonium fluoride-treated surfaces of silicon by energy-filtered doping contrast in the scanning electron microscope

PubMed Central

Chee, Augustus K. W.

2016-01-01

Two-dimensional dopant profiling using the secondary electron (SE) signal in the scanning electron microscope (SEM) is a technique gaining impulse for its ability to enable rapid and contactless low-cost diagnostics for integrated device manufacturing. The basis is doping contrast from electrical p-n junctions, which can be influenced by wet-chemical processing methods typically adopted in ULSI technology. This paper describes the results of doping contrast studies by energy-filtering in the SEM from silicon p-n junction specimens that were etched in ammonium fluoride solution. Experimental SE micro-spectroscopy and numerical simulations indicate that Fermi level pinning occurred on the surface of the treated-specimen, and that the doping contrast can be explained in terms of the ionisation energy integral for SEs, which is a function of the dopant concentration, and surface band-bending effects that prevail in the mechanism for doping contrast as patch fields from the specimen are suppressed. PMID:27576347

Surface conduction of topological Dirac electrons in bulk insulating Bi2Se3

NASA Astrophysics Data System (ADS)

Fuhrer, Michael

2013-03-01

The three dimensional strong topological insulator (STI) is a new phase of electronic matter which is distinct from ordinary insulators in that it supports on its surface a conducting two-dimensional surface state whose existence is guaranteed by topology. I will discuss experiments on the STI material Bi2Se3, which has a bulk bandgap of 300 meV, much greater than room temperature, and a single topological surface state with a massless Dirac dispersion. Field effect transistors consisting of thin (3-20 nm) Bi2Se3 are fabricated from mechanically exfoliated from single crystals, and electrochemical and/or chemical gating methods are used to move the Fermi energy into the bulk bandgap, revealing the ambipolar gapless nature of transport in the Bi2Se3 surface states. The minimum conductivity of the topological surface state is understood within the self-consistent theory of Dirac electrons in the presence of charged impurities. The intrinsic finite-temperature resistivity of the topological surface state due to electron-acoustic phonon scattering is measured to be ~60 times larger than that of graphene largely due to the smaller Fermi and sound velocities in Bi2Se3, which will have implications for topological electronic devices operating at room temperature. As samples are made thinner, coherent coupling of the top and bottom topological surfaces is observed through the magnitude of the weak anti-localization correction to the conductivity, and, in the thinnest Bi2Se3 samples (~ 3 nm), in thermally-activated conductivity reflecting the opening of a bandgap.

Effect of deposition temperature on the structural and optical properties of CdSe QDs thin films deposited by CBD method

DOE Office of Scientific and Technical Information (OSTI.GOV)

Laatar, F., E-mail: fakher8laatar@gmail.com; Harizi, A.; Smida, A.

2016-06-15

Highlights: • Synthesis of CdSe QDs with L-Cysteine capping agent for applications in nanodevices. • The films of CdSe QDs present uniform and good dispersive particles at the surface. • Effect of bath temperature on the structural and optical properties of CdSe QDs thin films. • Investigation of the optical constants and dispersion parameters of CdSe QDs thin films. - Abstract: Cadmium selenide quantum dots (CdSe QDs) thin films were deposited onto glass substrates by a chemical bath deposition (CBD) method at different temperatures from an aqueous solution containing L-Cysteine (L-Cys) as capping agent. The evolution of the surface morphologymore » and elemental composition of the CdSe films were studied by AFM, SEM, and EDX analyses. Structural and optical properties of CdSe thin films were investigated by XRD, UV–vis and PL spectroscopy. The dispersion behavior of the refractive index is described using the single oscillator Wemple-DiDomenico (W-D) model, and the physical dispersion parameters are calculated as a function of deposition temperature. The dispersive optical parameters such as average oscillator energy (E{sub o}), dispersion energy (E{sub d}), and static refractive index (n{sub o}) were found to vary with the deposition temperature. Besides, the electrical free carrier susceptibility (χ{sub e}) and the carrier concentration of the effective mass ratio (N/m*) were evaluated according to the Spitzer-Fan model.« less

Secondary electron emission influenced by oxidation on the aluminum surface: the roles of the chemisorbed oxygen and the oxide layer

NASA Astrophysics Data System (ADS)

Li, Jiangtao; Hoekstra, Bart; Wang, Zhen-Bin; Qiu, Jie; Pu, Yi-Kang

2018-04-01

A relationship between the apparent secondary electron yield ({γ }{{se}}) and the oxygen coverage/oxide layer thickness on an aluminum cathode is obtained in an experiment under a controlled environment. The apparent secondary electron yield ({γ }{{se}}) is deduced from the breakdown voltage between two parallel plate electrodes in a 360 mTorr argon environment using a simple Townsend breakdown model with the assumption that the variation of the apparent secondary electron yield is dominated by the variation of the argon ion induced processes. The oxygen coverage/oxide layer thickness on the aluminum cathode is measured by a semi in situ x-ray photoemission spectroscopy equipment which is directly attached to the discharge chamber. It is found that three phases exist: (1) in the monomonolayer regime, as the oxygen coverage increases from 0 to 0.3, {γ }{{se}} decreases by nearly 40 % , (2) as the oxygen coverage increases from 0.3 to 1, {γ }{{se}} keeps nearly constant, (3) as the oxide layer thickness increases from about 0.3 nm to about 1.1 nm, {γ }{{se}} increases by 150 % . We propose that, in the submonolayer regime, the chemisorbed oxygen on the aluminum surface causes the decrease of {γ }{{se}} by creating a local potential barrier, which reduces the Auger neutralization rate and the energy gained by the Auger electrons. In the multilayer regime, as the oxide layer grows in thickness, there are three proposed mechanisms which cause the increase of {γ }{{se}}: (1) the work function decreases; (2) resonance neutralization and Auger de-excitation may exist. This is served as another channel for secondary electron production; (3) the kinetic energy of Auger electrons is increased on average, leading to a higher probability for electrons to overcome the surface potential barrier.

Passivation effect of Cl, F and H atoms on CuIn0.75Ga0.25Se2 (1 1 2) surface

NASA Astrophysics Data System (ADS)

Qi, Rong-fei; Wang, Zhao-hui; Tang, Fu-ling; Agbonkina, Itohan C.; Xue, Hong-tao; Si, Feng-juan; Ma, Sheng-ling; Wang, Xiao-ka

2018-06-01

Using the first-principles calculations within the density functional-theory (DFT) framework, we theoretically investigated the surface reconstruction, surface states near the Fermi level and their passivation on CuIn0.75Ga0.25Se2 (1 1 2) (CIGS) surface by chlorine, fluorine and hydrogen. Surface reconstruction appears on CIG-terminated CIGS (1 1 2) surface and it is a self-passivation. For the locations of Cl, F and H atoms adsorbing on Se-terminated CIGS (1 1 2) surface, four high symmetry adsorption sites: top sites, bridge sites, hexagonal close-packed (hcp) sites and faced centered cubic (fcc) sites were studied respectively. With the coverage of 0.5 monolayer (ML), Cl, F and H adatoms energetically occupy the top sites on the CIGS (112) surface. The corresponding adsorption energies were -2.20 eV, -3.29 eV, -2.60 eV, respectively. The bond length and electronic properties were analyzed. We found that the surface state density near the Fermi level was markedly diminished for 0.5 ML Cl, F and H adsorption on Se-terminated CIGS (1 1 2) surface at top sites. It was also found that H can more efficiently passivate the surface state density than Cl and F atoms, and the effect of adsorption of Cl atoms is better than that of F.

ZnO/ZnSxSe1-x core/shell nanowire arrays as photoelectrodes with efficient visible light absorption

NASA Astrophysics Data System (ADS)

Wang, Zhenxing; Zhan, Xueying; Wang, Yajun; Safdar, Muhammad; Niu, Mutong; Zhang, Jinping; Huang, Ying; He, Jun

2012-08-01

ZnO/ZnSxSe1-x core/shell nanowires have been synthesized on n+-type silicon substrate via a two-step chemical vapor deposition method. Transmission electron microscopy reveals that ZnSxSe1-x can be deposited on the entire surface of ZnO nanowire, forming coaxial heterojunction along ZnO nanowire with very smooth shell surface and high shell thickness uniformity. The photoelectrode after deposition of the ternary alloy shell significantly improves visible light absorption efficiency. Electrochemical impedance spectroscopy results explicitly indicate that the introduction of ZnSxSe1-x shell to ZnO nanowires effectively improves the photogenerated charge separation process. Our finding opens up an efficient means for achieving high efficient energy conversion devices.

Gigantic Surface Lifetime of an Intrinsic Topological Insulator

DOE PAGES

Neupane, Madhab; Xu, Su-Yang; Ishida, Yukiaki; ...

2015-09-09

We report that the interaction between light and novel two-dimensional electronic states holds promise to realize new fundamental physics and optical devices. Here, we use pump-probe photoemission spectroscopy to study the optically excited Dirac surface states in the bulk-insulating topological insulator Bi 2Te 2Se and reveal optical properties that are in sharp contrast to those of bulk-metallic topological insulators. We observe a gigantic optical lifetime exceeding 4 μs (1 μs=10 more » $${-}$$6 s) for the surface states in Bi 2Te 2Se, whereas the lifetime in most topological insulators, such as Bi2Se3, has been limited to a few picoseconds (1 ps=10 $${-}$$12 s). Moreover, we discover a surface photovoltage, a shift of the chemical potential of the Dirac surface states, as large as 100 mV. Lastly, our results demonstrate a rare platform to study charge excitation and relaxation in energy and momentum space in a two-dimensional system.« less

CdSe/beta-Pb0.33V2O5 heterostructures: Nanoscale semiconductor interfaces with tunable energetic configurations for solar energy conversion and storage

NASA Astrophysics Data System (ADS)

Milleville, Christopher C.

This dissertation focuses on the formation and characterization of semiconductor heterostructures, consisting of light-harvesting cadmium selenide quantum dots (CdSe QDs) and single crystalline lead vanadium oxide nanowires (β-Pb0.33V2O5 NWs), for the purpose of excited-state charge transfer and photocatalytic production of solar fuels. We reported two distinct routes for assembling CdSe/β-Pb0.33V2O5 heterostructures: linker-assisted assembly (LAA) mediated by a bifunctional ligand and successive ionic layer adsorption and reaction (SILAR). In the former case, the thiol end of a molecular linker, cysteine (Cys) is found to bind to the QD surface, whereas a protonated amine moiety interacts electrostatically with the negatively charged NW surface. In the alternative SILAR route, the surface coverage of CdSe on the β-Pb0.33V2O5 NWs is tuned by varying the number of successive precipitation cycles. Hard X-ray photoelectron spectroscopy (HAXPES) measurements revealed that the mid-gap states of β-Pb0.33V2O5 NWs are closely overlapped in energy with the valence band edges of CdSe QDs, suggesting that hole transfer from the valence band of CdSe into the mid-gap states is possible. Preliminary evidence of hole transfer was obtained through photoluminescence quenching experiments. Steady-state and time-resolved photoluminescence measurements on Cys-CdSe dispersions, mixed dispersions of Cys-CdSe QDs and β-Pb0.33V¬2O5 NWs, and mixed dispersions of Cys-CdS QDs and V2O5 revealed a greater extent of quenching of the emission of Cys-CdSe QDs by β Pb0.33V¬2O5 relative to V2O5. V2O5, devoid of mid-gap states, is unable to accept holes from CdSe and therefore should not quench emission to the same extent as β-Pb0.33V¬2O5. The additional quenching was dynamic, consistent with a mechanism involving the transfer of photogenerated holes from CdSe QDs to the mid-gap states of β Pb0.33V2O5. Transient absorption spectroscopy (TA) was used to probe the dynamics of interfacial charge transfer of CdSe/β-Pb0.33V¬2O5 and CdSe/V2O5 heterostructures. TA measurements indicate that, for both types of heterostructures, photoexcitation of CdSe QDs was followed by a transfer of electrons to the conduction band of β-Pb0.33V¬2O5 and holes to the mid-gap states of β-Pb0.33V¬2O5. Ultrafast transient absoprtion measurements revealed that holes actually transferred before electrons, on time scales of ca. 2 ps. In contrast, for analogous heterostructures consisting of CdSe QDs interfaced with V2O5, only electron transfer was observed. In addition, electron transfer was readily achieved for SILAR-prepared heterostructures; however, for LAA-prepared heterostructures, electron transfer was observed only upon excitation at energies substantially greater than the bandgap absorption threshold of CdSe. Transient absorbance decay traces revealed longer excited-state lifetimes (1-3 μs) for CdSe/β Pb0.33V2O5 heterostructures relative to bare β-Pb0.33V2O5 NWs (0.2 to 0.6 μs); the difference was attributed to surface passivation of intrinsic surface defects in β-Pb0.33V2O5 upon interfacing with CdSe. In an effort to improve the energetic offset in QD/β-Pb0.33V2O5 heterostructures, cadmium sulfide (CdS) QDs were used in place of CdSe QDs. X-ray photoelectron spectroscopy (XPS) valence band spectra of CdS/β-Pb0.33V2O5 and CdSe/β-Pb0.33V2O5 revealed a greater binding energy onset for CdS compared to CdSe. Binding energy onsets of 1.33 (± 0.03) and 0.92 (± 0.02) eV were determined for Cys-CdS/β Pb0.33V2O5 and Cys-CdSe/β Pb0.33V2O5, respectively; suggesting a 0.41 (±0.04) eV decrease in the free energy (ΔG) needed for hole transfer from the valence band edge of the QDs to the mid-gap states. Linear sweep voltammetry was employed to measure the photocatalytic activity of CdSe/β Pb0.33V2O5 heterostructures in electrolytes containing ascorbic acid as a sacrificial proton donor. Preliminary photoelectrochemical measurements on CdSe/β-Pb0.33V2O5 electrodes revealed reductive photocurrents at applied potentials ca. 450 mV positive of the dark proton reduction onset. Importantly, no reductive photocurrents were measured on bare β-Pb0.33V2O5 electrodes. These results are consistent with a mechanism in which photoinduced hole transfer from CdSe QDs to the mid-gap states of β Pb0.33V2O5 NWs facilitates the reduction of protons, as the charge-separated state allows proton reduction to compete with exciton recombination. This avenue of research is ongoing.

Comparison of calculation and experiment implicates significant electrostatic contributions to the binding stability of barnase and barstar.

PubMed

Dong, Feng; Vijayakumar, M; Zhou, Huan-Xiang

2003-07-01

The contributions of electrostatic interactions to the binding stability of barnase and barstar were studied by the Poisson-Boltzmann model with three different protocols: a), the dielectric boundary specified as the van der Waals (vdW) surface of the protein along with a protein dielectric constant (epsilon (p)) of 4; b), the dielectric boundary specified as the molecular (i.e., solvent-exclusion (SE)) surface along with epsilon (p) = 4; and c), "SE + epsilon (p) = 20." The "vdW + epsilon (p) = 4" and "SE + epsilon (p) = 20" protocols predicted an overall electrostatic stabilization whereas the "SE + epsilon (p) = 4" protocol predicted an overall electrostatic destabilization. The "vdW + epsilon (p) = 4" protocol was most consistent with experiment. It quantitatively reproduced the observed effects of 17 mutations neutralizing charged residues lining the binding interface and the measured coupling energies of six charge pairs across the interface and reasonably rationalized the experimental ionic strength and pH dependences of the binding constant. In contrast, the "SE + epsilon (p) = 4" protocol predicted significantly larger coupling energies of charge pairs whereas the "SE + epsilon (p) = 20" protocol did not predict any pH dependence. This study calls for further scrutiny of the different Poisson-Boltzmann protocols and demonstrates potential danger in drawing conclusions on electrostatic contributions based on a particular calculation protocol.

Thermodynamic properties of model CdTe/CdSe mixtures

DOE PAGES

van Swol, Frank; Zhou, Xiaowang W.; Challa, Sivakumar R.; ...

2015-02-20

We report on the thermodynamic properties of binary compound mixtures of model groups II–VI semiconductors. We use the recently introduced Stillinger–Weber Hamiltonian to model binary mixtures of CdTe and CdSe. We use molecular dynamics simulations to calculate the volume and enthalpy of mixing as a function of mole fraction. The lattice parameter of the mixture closely follows Vegard's law: a linear relation. This implies that the excess volume is a cubic function of mole fraction. A connection is made with hard sphere models of mixed fcc and zincblende structures. We found that the potential energy exhibits a positive deviation frommore » ideal soluton behaviour; the excess enthalpy is nearly independent of temperatures studied (300 and 533 K) and is well described by a simple cubic function of the mole fraction. Using a regular solution approach (combining non-ideal behaviour for the enthalpy with ideal solution behaviour for the entropy of mixing), we arrive at the Gibbs free energy of the mixture. The Gibbs free energy results indicate that the CdTe and CdSe mixtures exhibit phase separation. The upper consolute temperature is found to be 335 K. Finally, we provide the surface energy as a function of composition. Moreover, it roughly follows ideal solution theory, but with a negative deviation (negative excess surface energy). This indicates that alloying increases the stability, even for nano-particles.« less

Controllable synthesis of metal selenide heterostructures mediated by Ag2Se nanocrystals acting as catalysts

NASA Astrophysics Data System (ADS)

Zhou, Jiangcong; Huang, Feng; Xu, Ju; Wang, Yuansheng

2013-09-01

Ag2Se nanocrystals were demonstrated to be novel semiconductor mediators, or in other word catalysts, for the growth of semiconductor heterostructures in solution. This is a result of the unique feature of Ag2Se as a fast ion conductor, allowing foreign cations to dissolve and then to heterogrow the second phase. Using Ag2Se nanocrystals as catalysts, dimeric metal selenide heterostructures such as Ag2Se-CdSe and Ag2Se-ZnSe, and even multi-segment heterostructures such as Ag2Se-CdSe-ZnSe and Ag2Se-ZnSe-CdSe, were successfully synthesized. Several interesting features were found in the Ag2Se based heterogrowth. At the initial stage of heterogrowth, a layer of the second phase forms on the surface of an Ag2Se nanosphere, with a curved junction interface between the two phases. With further growth of the second phase, the Ag2Se nanosphere tends to flatten the junction surface by modifying its shape from sphere to hemisphere in order to minimize the conjunct area and thus the interfacial energy. Notably, the crystallographic relationship of the two phases in the heterostructure varies with the lattice parameters of the second phase, in order to reduce the lattice mismatch at the interface. Furthermore, a small lattice mismatch at the interface results in a straight rod-like second phase, while a large lattice mismatch would induce a tortuous product. The reported results may provide a new route for developing novel selenide semiconductor heterostructures which are potentially applicable in optoelectronic, biomedical, photovoltaic and catalytic fields.Ag2Se nanocrystals were demonstrated to be novel semiconductor mediators, or in other word catalysts, for the growth of semiconductor heterostructures in solution. This is a result of the unique feature of Ag2Se as a fast ion conductor, allowing foreign cations to dissolve and then to heterogrow the second phase. Using Ag2Se nanocrystals as catalysts, dimeric metal selenide heterostructures such as Ag2Se-CdSe and Ag2Se-ZnSe, and even multi-segment heterostructures such as Ag2Se-CdSe-ZnSe and Ag2Se-ZnSe-CdSe, were successfully synthesized. Several interesting features were found in the Ag2Se based heterogrowth. At the initial stage of heterogrowth, a layer of the second phase forms on the surface of an Ag2Se nanosphere, with a curved junction interface between the two phases. With further growth of the second phase, the Ag2Se nanosphere tends to flatten the junction surface by modifying its shape from sphere to hemisphere in order to minimize the conjunct area and thus the interfacial energy. Notably, the crystallographic relationship of the two phases in the heterostructure varies with the lattice parameters of the second phase, in order to reduce the lattice mismatch at the interface. Furthermore, a small lattice mismatch at the interface results in a straight rod-like second phase, while a large lattice mismatch would induce a tortuous product. The reported results may provide a new route for developing novel selenide semiconductor heterostructures which are potentially applicable in optoelectronic, biomedical, photovoltaic and catalytic fields. Electronic supplementary information (ESI) available: Fig. S1-S8 and Table S1. See DOI: 10.1039/c3nr03601d

Dynamic surface electronic reconstruction as symmetry-protected topological orders in topological insulator Bi2Se3

NASA Astrophysics Data System (ADS)

Shu, G. J.; Liou, S. C.; Karna, S. K.; Sankar, R.; Hayashi, M.; Chou, F. C.

2018-04-01

The layered narrow-band-gap semiconductor Bi2Se3 is composed of heavy elements with strong spin-orbital coupling, which has been identified both as a good candidate for a thermoelectric material with high thermoelectric figure of merit (Z T ) and as a topological insulator of the Z2 type with a gapless surface band in a Dirac-cone shape. The existence of a conjugated π -bond system on the surface of each Bi2Se3 quintuple layer is proposed based on an extended valence bond model with valence electrons distributed in the hybridized orbitals. Supporting experimental evidence of a two-dimensional (2D) conjugated π -bond system on each quintuple layer of Bi2Se3 is provided using electron energy-loss spectroscopy and electron density mapping through inverse Fourier transform of x-ray diffraction data. Quantum chemistry calculations support the π -bond existence between partially filled 4 pz orbitals of Se via side-to-side orbital overlap positively. The conjugated π -bond system on the surface of each quintuple Bi2Se3 layer is proposed to be similar to that found in graphite (graphene) and responsible for the unique 2D conduction mechanism. The van der Waals (vdW) attractive force between quintuple layers is interpreted to be coming from the antiferroelectrically ordered effective electric dipoles, which are constructed with π -bond trimer pairs on Se layers across the vdW gap of minimized Coulomb repulsion.

Probing Dirac fermion dynamics in topological insulator Bi2Se3 films with a scanning tunneling microscope.

PubMed

Song, Can-Li; Wang, Lili; He, Ke; Ji, Shuai-Hua; Chen, Xi; Ma, Xu-Cun; Xue, Qi-Kun

2015-05-01

Scanning tunneling microscopy and spectroscopy have been used to investigate the femtosecond dynamics of Dirac fermions in the topological insulator Bi2Se3 ultrathin films. At the two-dimensional limit, bulk electrons become quantized and the quantization can be controlled by the film thickness at a single quintuple layer level. By studying the spatial decay of standing waves (quasiparticle interference patterns) off steps, we measure directly the energy and film thickness dependence of the phase relaxation length lϕ and inelastic scattering lifetime τ of topological surface-state electrons. We find that τ exhibits a remarkable (E - EF)(-2) energy dependence and increases with film thickness. We show that the features revealed are typical for electron-electron scattering between surface and bulk states.

Investigations of the electronic and magnetic properties of newly (001) surface LiCrS and LiCrSe half-Heusler compounds

NASA Astrophysics Data System (ADS)

Hussain, Moaid K.

2018-04-01

We analyzed the electronic and magnetic properties of newly (001) surface LiCrS and LiCrSe half-Heusler compounds with the C1b structure, based on calculations of the first principles. We examine the influences of (001) surface and correlation interactions on the structural properties and electricity and magnetism of the bulk and surface (001) LiCrS and LiCrSe half-Heusler compounds with two ideal terminations named Cr-S and li-li and Cr-Se and li-term terminated (001) surfaces, respectively. We noticed that the half-metallicity assured in the bulk is kept at the Cr-S and Cr-Se terminations, with a total spin polarization equal to 100%, with a wide range in the energy gap, and the magnetic moments calculated for both terminations were found to be equal to 29 µB/f.u., which have a great scientifics in varied application. For the li-li and li-term terminations, we noticed that the half-metallicity is destroy with a total spin polarization equal to 84 and 67%, respectively, with a magnetic moment of 25.5 µB/f.u. The calculated magnetic moment of all terminations was found of all the subsurface is close to that of the bulk system and this makes these compounds of maximum benefit in the pilot applications of spintronic systems.

Effect of Sn Content in a CuSnZn Metal Precursor on Formation of MoSe2 Film during Selenization in Se+SnSe Vapor

PubMed Central

Yao, Liyong; Ao, Jianping; Jeng, Ming-Jer; Bi, Jinlian; Gao, Shoushuai; Sun, Guozhong; He, Qing; Zhou, Zhiqiang; Sun, Yun; Chang, Liann-Be

2016-01-01

The preparation of Cu2ZnSnSe4 (CZTSe) thin films by the selenization of an electrodeposited copper–tin–zinc (CuSnZn) precursor with various Sn contents in low-pressure Se+SnSex vapor was studied. Scanning electron microscope (SEM) and energy dispersive spectroscopy (EDS) measurements revealed that the Sn content of the precursor that is used in selenization in a low-pressure Se+SnSex vapor atmosphere only slightly affects the elemental composition of the formed CZTSe films. However, the Sn content of the precursor significantly affects the grain size and surface morphology of CZTSe films. A metal precursor with a very Sn-poor composition produces CZTSe films with large grains and a rough surface, while a metal precursor with a very Sn-rich composition procures CZTSe films with small grains and a compact surface. X-ray diffraction (XRD) and SEM revealed that the metal precursor with a Sn-rich composition can grow a thicker MoSe2 thin film at CZTSe/Mo interface than one with a Sn-poor composition, possibly because excess Sn in the precursor may catalyze the formation of MoSe2 thin film. A CZTSe solar cell with an efficiency of 7.94%was realized by using an electrodeposited metal precursor with a Sn/Cu ratio of 0.5 in selenization in a low-pressure Se+SnSex vapor. PMID:28773366

Origin of n-type conductivity in two-dimensional InSe: In atoms from surface adsorption and van der Waals gap

NASA Astrophysics Data System (ADS)

Wang, Hui; Shi, Jun-jie; Huang, Pu; Ding, Yi-min; Wu, Meng; Cen, Yu-lang; Yu, Tongjun

2018-04-01

Recently, two-dimensional (2D) InSe nanosheet becomes a promising material for electronic and optoelectronic nano-devices due to its excellent electron transport, wide bandgap tunability and good metal contact. The inevitable native point defects are essential in determining its characteristics and device performance. Here we investigate the defect formation energy and thermodynamic transition levels for the most important native defects and clarify the physical origin of n-type conductivity in unintentionally doped 2D InSe by using the powerful first-principles calculations. We find that both surface In adatom and Se vacancy are the key defects, and the In adatom, donated 0.65 electrons to the host, causes the n-type conductivity in monolayer InSe under In-rich conditions. For bilayer or few-layer InSe, the In interstitial within the van der Waals gap, transferred 0.68 electrons to InSe, is found to be the most stable donor defect, which dominates the n-type character. Our results are significant for understanding the defect nature of 2D InSe and improving the related nano-device performance.

Magnesium effects on CdSe self-assembled quantum dot formation on Zn xCd yMg 1-x-ySe layers

NASA Astrophysics Data System (ADS)

Noemi Perez-Paz, M.; Lu, Hong; Shen, Aidong; Jean Mary, F.; Akins, Daniel; Tamargo, Maria C.

2006-09-01

Optical and morphological studies are used to investigate the effects of chemical composition and, in particular, the magnesium content of the Zn xCd yMg 1-x-ySe barrier layers on the size, density and uniformity of CdSe self-assembled quantum dots (QDs). A reduction of the uncapped QD size, as well as a blue shift of the capped QD photoluminescence peak position by increasing Mg concentration in the Zn xCd yMg 1-x-ySe barrier has been demonstrated by changing the Mg cell temperature during growth. In addition, a more uniform and more densely packed QD layer has been observed with an increase of the MgSe fraction in the Zn xCd yMg 1-x-ySe barrier layer using three-dimensional topographic atomic force microscopy images of the surface of uncapped QDs. Results point to Mg as a chemical factor that induces QD formation, either by increasing the density of atomic steps or/and by changing the energy of the Zn xCd yMg 1-x-ySe surface.

Superconducting topological surface states in the noncentrosymmetric bulk superconductor PbTaSe2.

PubMed

Guan, Syu-You; Chen, Peng-Jen; Chu, Ming-Wen; Sankar, Raman; Chou, Fangcheng; Jeng, Horng-Tay; Chang, Chia-Seng; Chuang, Tien-Ming

2016-11-01

The search for topological superconductors (TSCs) is one of the most urgent contemporary problems in condensed matter systems. TSCs are characterized by a full superconducting gap in the bulk and topologically protected gapless surface (or edge) states. Within each vortex core of TSCs, there exists the zero-energy Majorana bound states, which are predicted to exhibit non-Abelian statistics and to form the basis of the fault-tolerant quantum computation. To date, no stoichiometric bulk material exhibits the required topological surface states (TSSs) at the Fermi level ( E F ) combined with fully gapped bulk superconductivity. We report atomic-scale visualization of the TSSs of the noncentrosymmetric fully gapped superconductor PbTaSe 2 . Using quasi-particle scattering interference imaging, we find two TSSs with a Dirac point at E ≅ 1.0 eV, of which the inner TSS and the partial outer TSS cross E F , on the Pb-terminated surface of this fully gapped superconductor. This discovery reveals PbTaSe 2 as a promising candidate for TSC.

Comparison of Calculation and Experiment Implicates Significant Electrostatic Contributions to the Binding Stability of Barnase and Barstar

PubMed Central

Dong, Feng; Vijayakumar, M.; Zhou, Huan-Xiang

2003-01-01

The contributions of electrostatic interactions to the binding stability of barnase and barstar were studied by the Poisson-Boltzmann model with three different protocols: a), the dielectric boundary specified as the van der Waals (vdW) surface of the protein along with a protein dielectric constant (ɛp) of 4; b), the dielectric boundary specified as the molecular (i.e., solvent-exclusion (SE)) surface along with ɛp = 4; and c), “SE + ɛp = 20.” The “vdW + ɛp = 4” and “SE + ɛp = 20” protocols predicted an overall electrostatic stabilization whereas the “SE + ɛp = 4” protocol predicted an overall electrostatic destabilization. The “vdW + ɛp = 4” protocol was most consistent with experiment. It quantitatively reproduced the observed effects of 17 mutations neutralizing charged residues lining the binding interface and the measured coupling energies of six charge pairs across the interface and reasonably rationalized the experimental ionic strength and pH dependences of the binding constant. In contrast, the “SE + ɛp = 4” protocol predicted significantly larger coupling energies of charge pairs whereas the “SE + ɛp = 20” protocol did not predict any pH dependence. This study calls for further scrutiny of the different Poisson-Boltzmann protocols and demonstrates potential danger in drawing conclusions on electrostatic contributions based on a particular calculation protocol. PMID:12829463

Direct synthesis of all-inorganic heterostructured CdSe/CdS QDs in aqueous solution for improved photocatalytic hydrogen generation

DOE Office of Scientific and Technical Information (OSTI.GOV)

Li, Zhi-Jun; Fan, Xiang-Bing; Li, Xu-Bing

2017-01-01

Here we present a facile aqueous approach to synthesize heterostructured CdSe/CdS QDs with all-inorganic chalcogenide S2- ligands under mild conditions. High-resolution transmission electron microscopy (HRTEM), X-ray diffraction (XRD), Raman spectroscopy, X-ray photoelectron spectroscopy (XPS), and steady-state emission spectroscopy demonstrate that the heterostructured CdSe/CdS QDs with sulfur-rich surface composition are formed by heterogeneous nucleation of Cd2+ and S2- precursors on the CdSe QDs. After adsorption of small Ni(OH)(2) clusters over the surface in situ, the CdSe/CdS-Ni(OH)(2) photocatalyst enables H-2 production efficiently with an internal quantum yield of 52% under visible light irradiation at 455 nm, up to an 8-fold increase ofmore » activity to that of spherical CdSe QDs-Ni(OH)(2) under the same conditions. Femtosecond transient absorption spectroscopy, X-ray transient absorption (XTA) spectroscopy, steady-state and time-resolved emission spectroscopy show that the quasi-type-II band alignment in the CdSe/CdS heterostructure is responsible for the efficiency enhancement of light harvesting and surface/interfacial charge separation in solar energy conversion. The unprecedented results exemplify an easily accessible pattern of aqueous synthesis of all-inorganic heterostructured QDs for advanced photosynthetic H-2 evolution.« less

Structure-Dependent Optical Properties of Self-Organized Bi2Se3 Nanostructures: From Nanocrystals to Nanoflakes.

PubMed

Yang, Shang-Dong; Yang, Liao; Zheng, Yu-Xiang; Zhou, Wen-Jie; Gao, Meng-Yu; Wang, Song-You; Zhang, Rong-Jun; Chen, Liang-Yao

2017-08-30

Bismuth selenide (Bi 2 Se 3 ), with a wide bulk band gap and single massless Dirac cone at the surface, is a promising three-dimensional topological insulator. Bi 2 Se 3 possesses gapless surface states and an insulator-like bulk band gap as a new type of quantum matter. Different Bi 2 Se 3 nanostructures were prepared using electron beam evaporation with high production efficiency. Structural investigations by energy-dispersive X-ray analysis, scanning electron microscopy, and X-ray diffraction revealed the sample stoichiometries and the structural transition mechanism from nanocrystals to nanoflakes. The optical properties systematically probed and analyzed by spectroscopic ellipsometry showed strong dependence on the nanostructures and were also predicted to have structure-modifiable technological prospects. The optical parameters, plasma frequencies, scattering rates of the free electrons, and optical band gaps were related to the topological properties of the Bi 2 Se 3 nanostructures via light-matter interactions, offering new opportunities and approaches for studies on topological insulators and spintronics. The high-quality Bi 2 Se 3 nanostructures provide advantages in exploring novel physics and exploiting prospective applications.

Quaternary schematics for property engineering of CdSe thin films

NASA Astrophysics Data System (ADS)

Chavan, G. T.; Pawar, S. T.; Prakshale, V. M.; Sikora, A.; Pawar, S. M.; Chaure, N. B.; Kamble, S. S.; Maldar, N. N.; Deshmukh, L. P.

2017-12-01

The synthesis of quaternary Cd1-xZnxSySe1-y (0 ≤ x = y ≤ 0.35) thin films was done through indigenously developed chemical solution growth process. As-obtained thin films were subjected to the physical, chemical, structural and optical characterizations. The nearly hydrophobic nature of the as-deposited films except binary CdSe was observed through the wettability studies. The colorimetric studies supported a change in physical color attributes. The elemental analysis done confirmed the formation of Cd(Zn, S)Se and the chemical states of constituent elements as Cd2+, Zn2+, S2- and Se2-. Structural assessment suggested the formation of the polycrystalline quaternary phase of the hexagonal wurtzite structure. The Raman spectroscopy was also employed for the confirmation studies on Cd1-xZnxSySe1-y thin films. Morphological observations indicated microstructural transformation from an aggregated bunch of nano-sized globular grains into a rhomboid network of petal/flakes like crystallites. The atomic force micrographs (AFM) revealed the enhancement in the hillock structures. From advanced AFM characterizations, we observed that the CdSe thin film has leptokurtic (Sku = 3.23) surface, whereas, quaternary Cd(Zn, S)Se films have platykurtic (Sku < 3) surface. The orientation of the surface morphology was observed through the angular spectrum studies. The optical absorption studies revealed direct allowed transition for the films with a continuous modulation of the energy bandgap from 1.8 eV to 2.31 eV.

Atomically thick bismuth selenide freestanding single layers achieving enhanced thermoelectric energy harvesting.

PubMed

Sun, Yongfu; Cheng, Hao; Gao, Shan; Liu, Qinghua; Sun, Zhihu; Xiao, Chong; Wu, Changzheng; Wei, Shiqiang; Xie, Yi

2012-12-19

Thermoelectric materials can realize significant energy savings by generating electricity from untapped waste heat. However, the coupling of the thermoelectric parameters unfortunately limits their efficiency and practical applications. Here, a single-layer-based (SLB) composite fabricated from atomically thick single layers was proposed to optimize the thermoelectric parameters fully. Freestanding five-atom-thick Bi(2)Se(3) single layers were first synthesized via a scalable interaction/exfoliation strategy. As revealed by X-ray absorption fine structure spectroscopy and first-principles calculations, surface distortion gives them excellent structural stability and a much increased density of states, resulting in a 2-fold higher electrical conductivity relative to the bulk material. Also, the surface disorder and numerous interfaces in the Bi(2)Se(3) SLB composite allow for effective phonon scattering and decreased thermal conductivity, while the 2D electron gas and energy filtering effect increase the Seebeck coefficient, resulting in an 8-fold higher figure of merit (ZT) relative to the bulk material. This work develops a facile strategy for synthesizing atomically thick single layers and demonstrates their superior ability to optimize the thermoelectric energy harvesting.

Magnetic behavior of Fe(Se,Te) systems: First-principles calculations

NASA Astrophysics Data System (ADS)

Shi, Hongliang; Huang, Zhong-Bing; Tse, John S.; Lin, Hai-Qing

2011-08-01

The magnetic behaviors in Fe(Se,Te) systems have been investigated systematically using density functional calculations. At the experimental lattice parameters, the ground state is found to be in the double stripe magnetic phase for FeTe but in the single stripe magnetic phase for FeSe and FeSe0.5Te0.5, and there is no preference in the different easy axes of magnetization. Substitution of Se by Te enlarges the size of the Fermi surface in FeSe0.5Te0.5, resulting in a stronger nesting effect and thus enhancing the superconductivity. It is found that the double stripe order in FeTe1-xSex changes to the single stripe order when x > 0.18. Spiral calculations on FeSe0.5Te0.5 show that the lowest energy is at the commensurate point Q→= (0.5,0.5), accompanied by additional local minima at two incommensurate points near Q→= (0.5,0.5). This observation is consistent with the experimentally observed positions of low energy magnetic excitations. Geometry optimization calculations show that the tetragonal cell relaxes to orthorhombic and monoclinic cells for FeSe and FeTe, respectively, but remains unchanged for FeSe0.5Te0.5.

Tetradymites as thermoelectrics and topological insulators

NASA Astrophysics Data System (ADS)

Heremans, Joseph P.; Cava, Robert J.; Samarth, Nitin

2017-10-01

Tetradymites are M2X3 compounds — in which M is a group V metal, usually Bi or Sb, and X is a group VI anion, Te, Se or S — that crystallize in a rhombohedral structure. Bi2Se3, Bi2Te3 and Sb2Te3 are archetypical tetradymites. Other mixtures of M and X elements produce common variants, such as Bi2Te2Se. Because tetradymites are based on heavy p-block elements, strong spin-orbit coupling greatly influences their electronic properties, both on the surface and in the bulk. Their surface electronic states are a cornerstone of frontier work on topological insulators. The bulk energy bands are characterized by small energy gaps, high group velocities, small effective masses and band inversion near the centre of the Brillouin zone. These properties are favourable for high-efficiency thermoelectric materials but make it difficult to obtain an electrically insulating bulk, which is a requirement of topological insulators. This Review outlines recent progress made in bulk and thin-film tetradymite materials for the optimization of their properties both as thermoelectrics and as topological insulators.

Controllable synthesis of metal selenide heterostructures mediated by Ag2Se nanocrystals acting as catalysts.

PubMed

Zhou, Jiangcong; Huang, Feng; Xu, Ju; Wang, Yuansheng

2013-10-21

Ag2Se nanocrystals were demonstrated to be novel semiconductor mediators, or in other word catalysts, for the growth of semiconductor heterostructures in solution. This is a result of the unique feature of Ag2Se as a fast ion conductor, allowing foreign cations to dissolve and then to heterogrow the second phase. Using Ag2Se nanocrystals as catalysts, dimeric metal selenide heterostructures such as Ag2Se-CdSe and Ag2Se-ZnSe, and even multi-segment heterostructures such as Ag2Se-CdSe-ZnSe and Ag2Se-ZnSe-CdSe, were successfully synthesized. Several interesting features were found in the Ag2Se based heterogrowth. At the initial stage of heterogrowth, a layer of the second phase forms on the surface of an Ag2Se nanosphere, with a curved junction interface between the two phases. With further growth of the second phase, the Ag2Se nanosphere tends to flatten the junction surface by modifying its shape from sphere to hemisphere in order to minimize the conjunct area and thus the interfacial energy. Notably, the crystallographic relationship of the two phases in the heterostructure varies with the lattice parameters of the second phase, in order to reduce the lattice mismatch at the interface. Furthermore, a small lattice mismatch at the interface results in a straight rod-like second phase, while a large lattice mismatch would induce a tortuous product. The reported results may provide a new route for developing novel selenide semiconductor heterostructures which are potentially applicable in optoelectronic, biomedical, photovoltaic and catalytic fields.

Nematic superconductivity in CuxBi2Se3 : Surface Andreev bound states

NASA Astrophysics Data System (ADS)

Hao, Lei; Ting, C. S.

2017-10-01

We study theoretically the topological surface states (TSSs) and the possible surface Andreev bound states (SABSs) of CuxBi2Se3 , which is known to be a topological insulator at x =0 . The superconductivity (SC) pairing of this compound is assumed to have broken spin-rotation symmetry, similar to that of the A-phase of 3He as suggested by recent nuclear-magnetic resonance experiments. For both spheroidal and corrugated cylindrical Fermi surfaces with the hexagonal warping terms, we show that the bulk SC gap is rather anisotropic; the minimum of the gap is negligibly small as compared to the maximum of the gap. This would make the fully gapped pairing effectively nodal. For a clean system, our results indicate the bulk of this compound to be a topological superconductor with the SABSs appearing inside the bulk SC gap. The zero-energy SABSs, which are Majorana fermions, together with the TSSs not gapped by the pairing, produce a zero-energy peak in the surface density of states (SDOS). The SABSs are expected to be stable against short-range nonmagnetic impurities, and the local SDOS is calculated around a nonmagnetic impurity. The relevance of our results to experiments is discussed.

Electronic and Optical Properties of Core/Shell Pb16X16/Cd52X52 (X =S, Se, Te) Quantum Dots

NASA Astrophysics Data System (ADS)

Tamukong, Patrick; Mayo, Michael; Kilina, Svetlana

2015-03-01

The electronic and optoelectronic properties of semiconductor quantum dots (QDs) are mediated by surface defects due to the presence of dangling bonds producing trap states within the HOMO-LUMO energy gap, and contributing to fluorescence quenching. Surface capping ligands are generally used to alleviate this problem and increase the quantum yields of QDs. An alternative way is to synthesize core-shell QD structures; i.e., a QD core with a shell of another semiconductor material. We have investigated the effects of Cd52X52 shells on the photoexcited dynamics of Pb16X16 (X =S, Se, Te) QDs. The thin (~ 0.50 nm) shells were found to result largely in type I core/shell structures and a blue shift of the absorption spectra. Our studies revealed fairly strong core-shell hybridization in the electronic states close to the conduction band (CB) edge for Pb16S16andPb16Se16 cores, whereas for the Pb16Te16 core, such CB states were largely shell-like in nature. Nonadiabatic DFT-based dynamics, coupled with the surface hopping method, was used to study the effects of the core and shell compositions on energy relaxation rates in these systems.

Scanning tunneling spectroscopic (STS) studies of magnetically doped MBE-grown topological insulators (TIs)

NASA Astrophysics Data System (ADS)

Chu, Hao; Teague, Marcus; Chen, Chien-Chang; Woodward, Nicholas; Yeh, Nai-Chang; Kou, Xufeng; He, Liang; Lang, Murong; Wang, Kang; Caltech Collaboration; UCLA Collaboration

2013-03-01

We conduct STS studies on MBE-grown heterostructures of non-magnetic TI (Bi2Se3) with a range of thicknesses (d = 1, 3, 5, 7 quintuple layers, QL) on top of 7-QL magnetically doped TI (Cr-doped Bi2Se3) . For d = 1 and 3-QL, a spatially homogeneous magnetism-induced surface gap (as large as about 150 meV for d = 1-QL) is observed at 77 K, whereas gapless Dirac spectra are found for d = 5 and 7-QL, suggesting that the effective magnetic length for Cr-doped Bi2Se3 is approximately 4 ~ 5-QL. These findings are further corroborated by ARPES and bulk electrical transport measurements. The magnetism-induced surface gap differs from those found in pure Bi2Se3 and (Bi0.5Sb0.5)2 Te3 films of thicknesses smaller than 6-QL, because the latter are due to overlaps of wave functions between the surface and interface layers, which lead to Rashba-like spin-orbit splitting and spin-preserving quasiparticle interference wave-vectors. In contrast, STS studies of TIs with magnetism-induced surface gap do not yield any quasiparticle interferences for energies within the bulk Bi2Se3 gap. Finally, comparative STS studies of pure and magnetically doped TIs in high magnetic fields will be discussed. This work was supported by DARPA.

Orbital selectivity causing anisotropy and particle-hole asymmetry in the charge density wave gap of 2 H -TaS2

NASA Astrophysics Data System (ADS)

Zhao, J.; Wijayaratne, K.; Butler, A.; Yang, J.; Malliakas, C. D.; Chung, D. Y.; Louca, D.; Kanatzidis, M. G.; van Wezel, J.; Chatterjee, U.

2017-09-01

We report an in-depth angle-resolved photoemission spectroscopy study on 2 H -TaS2 , a canonical incommensurate charge density wave (CDW) system. This study demonstrates that just as in related incommensurate CDW systems, 2 H -TaSe2 and 2 H -NbSe2 , the energy gap (ΔCDW) of 2 H -TaS2 is localized along the K -centered Fermi surface barrels and is particle-hole asymmetric. The persistence of ΔCDW even at temperatures higher than the CDW transition temperature TCDW in 2 H -TaS2 , reflects the similar pseudogap behavior observed previously in 2 H -TaSe2 and 2 H -NbSe2 . However, in sharp contrast to 2 H -NbSe2 , where ΔCDW is nonzero only in the vicinity of a few "hot spots" on the inner K -centered Fermi surface barrels, ΔCDW in 2 H -TaS2 is nonzero along the entirety of both K -centered Fermi surface barrels. Based on a tight-binding model, we attribute this dichotomy in the momentum dependence and the Fermi surface specificity of ΔCDW between otherwise similar CDW compounds to the different orbital orientations of their electronic states that participate in the CDW pairing. Our results suggest that the orbital selectivity plays a critical role in the description of incommensurate CDW materials.

Photoelectrochemical processes in polymer-tethered CdSe nanocrystals.

PubMed

Shallcross, R Clayton; D'Ambruoso, Gemma D; Pyun, Jeffrey; Armstrong, Neal R

2010-03-03

We demonstrate the electrochemical capture of CdSe semiconductor nanocrystals (NCs), with thiophene-terminated carboxylic acid capping ligands, at the surfaces of electrodeposited poly(thiophene) films (i) poly((diethyl)propylenedixoythiophene), P(Et)(2)ProDOT; (ii) poly(propylenedioxythiophene), PProDOT; and (iii) poly(ethylenedioxythiophene), PEDOT, coupled with the exploration of their photoelectrochemical properties. Host polymer films were created using a kinetically controlled electrodeposition protocol on activated indium-tin oxide electrodes (ITO), producing conformal films that facilitate high rates of electron transfer. ProDOT-terminated, ligand-capped CdSe-NCs were captured at the outer surface of the host polymer films using a unique pulse-potential step electrodeposition protocol, providing for nearly close-packed monolayers of the NCs at the host polymer/solution interface. These polymer-confined CdSe NCs were used as sensitizers in the photoelectrochemical reduction of methyl viologen (MV(+2)). High internal quantum efficiencies (IQEs) are estimated for photoelectrochemical sensitized MV(+2) reduction using CdSe NCs ranging from 3.1 to 7.0 nm diameters. Cathodic photocurrent at high MV(+2) concentrations are limited by the rate of hole-capture by the host polymer from photoexcited NCs. The rate of this hole-capture process is determined by (a) the onset potential for reductive dedoping of the host polymer film; (b) the concentration ratio of neutral to oxidized forms of the host polymer ([P(n)]/[P(ox)]); and (c) the NC diameter, which controls its valence band energy, E(VB). These relationships are consistent with control of photoinduced electron transfer by Marcus-like excess free energy relationships. Our electrochemical assembly methods provide an enabling route to the capture of functional NCs in conducting polymer hosts in both photoelectrochemical and photovoltaic energy conversion systems.

Effect of organic materials used in the synthesis on the emission from CdSe quantum dots

NASA Astrophysics Data System (ADS)

Lee, Jae-Won; Yang, Ho-Soon; Hong, K. S.; Kim, S. M.

2013-12-01

Quantum-dot nanocrystals have particular optical properties due to the quantum confinement effect and the surface effect. This study focuses on the effect of surface conditions on the emission from quantum dots. The quantum dots prepared with 1-hexadecylamine (HDA) in the synthesis show strong emission while the quantum dots prepared without HDA show weak emission, as well as emission from surface energy traps. The comparison of the X-ray patterns of these two sets of quantum dots reveals that HDA forms a layer on the surface of quantum dot during the synthesis. This surface passivation with a layer of HDA reduces surface energy traps, therefore the emission from surface trap levels is suppressed in the quantum dots synthesized with HDA.

Electronic structure and optical properties of defect chalcopyrite HgGa2Se4

NASA Astrophysics Data System (ADS)

Gabrelian, B. V.; Lavrentyev, A. A.; Vu, Tuan V.; Parasyuk, O. V.; Khyzhun, O. Y.

2018-01-01

We report on studies from an experimental and theoretical viewpoint of the electronic structure of mercury digallium selenide, HgGa2Se4, a very promising optoelectronic material. In particular, the method of X-ray photoelectron spectroscopy (XPS) was used to evaluate binding energies of the constituent element core electrons and the shape of the valence band for pristine and Ar+-ion bombarded surfaces of HgGa2Se4 single crystal. First principles band-structure calculations were performed in the present work using the augmented plane wave + local orbitals (APW+lo). These calculations indicate that the Se 4p states are the main contributors at the top and in the upper portion of the valence band with slightly smaller contributions of the Ga 4p states in the upper portion of the band as well. Further, the central portion of the valence band is determined mainly by contributions of the Ga 4s states, and the Hg 5d states are the principal contributors to the bottom of the valence band. These theoretical data are in fair agreement when matching on a common energy scale of the X-ray emission bands giving information on the energy distribution of the Se 4p and Ga 4p states and the XPS valence-band spectrum of the HgGa2Se4 crystal. The principal optical constants are elucidated from the DFT calculations.

Quaternary Chalcogenide-Based Misfit Nanotubes LnS(Se)-TaS(Se)2 (Ln = La, Ce, Nd, and Ho): Synthesis and Atomic Structural Studies.

PubMed

Lajaunie, Luc; Radovsky, Gal; Tenne, Reshef; Arenal, Raul

2018-01-16

We have synthesized quaternary chalcogenide-based misfit nanotubes LnS(Se)-TaS 2 (Se) (Ln = La, Ce, Nd, and Ho). None of the compounds described here were reported in the literature as a bulk compound. The characterization of these nanotubes, at the atomic level, has been developed via different transmission electron microscopy techniques, including high-resolution scanning transmission electron microscopy, electron diffraction, and electron energy-loss spectroscopy. In particular, quantification at sub-nanometer scale was achieved by acquiring high-quality electron energy-loss spectra at high energy (∼between 1000 and 2500 eV). Remarkably, the sulfur was found to reside primarily in the distorted rocksalt LnS lattice, while the Se is associated with the hexagonal TaSe 2 site. Consequently, these quaternary misfit layered compounds in the form of nanostructures possess a double superstructure of La/Ta and S/Se with the same periodicity. In addition, the interlayer spacing between the layers and the interatomic distances within the layer vary systematically in the nanotubes, showing clear reduction when going from the lightest (La atom) to the heaviest (Ho) atom. Amorphous layers, of different nature, were observed at the surface of the nanotubes. For La-based NTs, the thin external amorphous layer (inferior to 10 nm) can be ascribed to a Se deficiency. Contrarily, for Ho-based NTs, the thick amorphous layer (between 10 and 20 nm) is clearly ascribed to oxidation. All of these findings helped us to understand the atomic structure of these new compounds and nanotubes thereof.

Magnetothermoelectric properties of Bi2Se3

NASA Astrophysics Data System (ADS)

Fauqué, Benoît; Butch, Nicholas P.; Syers, Paul; Paglione, Johnpierre; Wiedmann, Steffen; Collaudin, Aurélie; Grena, Benjamin; Zeitler, Uli; Behnia, Kamran

2013-01-01

We present a study of entropy transport in Bi2Se3 at low temperatures and high magnetic fields. In the zero-temperature limit, the magnitude of the Seebeck coefficient quantitatively tracks the Fermi temperature of the three-dimensional Fermi surface at the Γ point as the carrier concentration changes by two orders of magnitude (1017 to 1019 cm-3). In high magnetic fields, the Nernst response displays giant quantum oscillations indicating that this feature is not exclusive to compensated semimetals. A comprehensive analysis of the Landau level spectrum firmly establishes a large g factor in this material and a substantial decrease of the Fermi energy with increasing magnetic field across the quantum limit. Thus, the presence of bulk carriers significantly affects the spectrum of the intensively debated surface states in Bi2Se3 and related materials.

Kinetics studies of the reactions of main fourth-period monocations (Ga+, Ge+, As+, and Se+) with methyl fluoride.

PubMed

Barrientos, Carmen; Rayón, Víctor Manuel; Largo, Antonio; Sordo, José Ángel; Redondo, Pilar

2013-08-22

Thermodynamics and kinetics theoretical studies on the gas-phase reactions of fluoromethane with main fourth-period monocations (Ga(+), Ge(+), As(+), and Se(+)) have been carried out. Density functional theory (in particular mPW1K functional) was employed in the description of the potential energy surfaces, and refinement of the energies were done at the CCSD(T) level. The reaction rate constants were estimated using variational/conventional microcanonical transition state theory. From a thermodynamic viewpoint, the fluorine abstraction product is predicted for Ga(+) and Ge(+), whereas for As(+) and Se(+) the elimination product, MCH2(+) (M = As, Se) + HF, is the preferred one. Nevertheless, the most favorable channel for the reactions of CH3F with Ga(+) and Se(+) cations present a net activation barrier. In the case of Ga(+), the reaction proceeds via an addition channel forming the adduct complex, CH3FGa(+), whereas for Se(+) no reaction is found, in agreement with the experiments. The predicted reaction rate constants are in reasonable good agreement with the experimental values available. Apart from the harpoon-like mechanism, our results suggest that an oxidative addition mechanism seems to play a relevant role.

Study on the growth mechanism and optical properties of sputtered lead selenide thin films

NASA Astrophysics Data System (ADS)

Sun, Xigui; Gao, Kewei; Pang, Xiaolu; Yang, Huisheng; Volinsky, Alex A.

2015-11-01

Lead selenide thin films with different microstructure were deposited on Si (1 0 0) substrates using magnetron sputtering at 50 °C, 150 °C and 250 °C, respectively. The crystal structure of the sputtered PbSe thin films varies from amorphous crystalline to columnar grain, and then to double-layer (nano-crystalline layer and columnar grain layer) structure as the deposition temperature increases, which is due to the dominating growth mode of the thin films changes from Frank-van der Merwe (or layer-by-layer) growth mode at 50 °C to Volmer-Weber (or 3D island) growth mode at 150 °C, and then to Stranski-Krastanow (or 3D island-on-wetting-layer) growth mode at 250 °C. The growth mechanism of the sputtered PbSe thin films is mainly dominated by the surface and strain energy contributions. Moreover, the strain energy contribution is more prominent when the deposition temperature is less than 180 °C, while, the surface energy contribution is more prominent when the deposition temperature is higher than 180 °C. The absorption spectra of the sputtered PbSe thin films are in 3.1-5 μm range. Besides, the sputtered PbSe thin film prepared at 250 °C has two different optical band gaps due to its unique double-layer structure. According to the theoretical calculation results, the variation of the band gap with the deposition temperature is determined by the shift of the valence band maximum with the lattice constant.

Converting topological insulators into topological metals within the tetradymite family

NASA Astrophysics Data System (ADS)

Chen, K.-W.; Aryal, N.; Dai, J.; Graf, D.; Zhang, S.; Das, S.; Le Fèvre, P.; Bertran, F.; Yukawa, R.; Horiba, K.; Kumigashira, H.; Frantzeskakis, E.; Fortuna, F.; Balicas, L.; Santander-Syro, A. F.; Manousakis, E.; Baumbach, R. E.

2018-04-01

We report the electronic band structures and concomitant Fermi surfaces for a family of exfoliable tetradymite compounds with the formula T2C h2P n , obtained as a modification to the well-known topological insulator binaries Bi2(Se,Te ) 3 by replacing one chalcogen (C h ) with a pnictogen (P n ) and Bi with the tetravalent transition metals T = Ti, Zr, or Hf. This imbalances the electron count and results in layered metals characterized by relatively high carrier mobilities and bulk two-dimensional Fermi surfaces whose topography is well-described by first-principles calculations. Intriguingly, slab electronic structure calculations predict Dirac-like surface states. In contrast to Bi2Se3 , where the surface Dirac bands are at the Γ point, for (Zr,Hf ) 2Te2 (P,As) there are Dirac cones of strong topological character around both the Γ ¯ and M ¯ points, which are above and below the Fermi energy, respectively. For Ti2Te2P , the surface state is predicted to exist only around the M ¯ point. In agreement with these predictions, the surface states that are located below the Fermi energy are observed by angle-resolved photoemission spectroscopy measurements, revealing that they coexist with the bulk metallic state. Thus this family of materials provides a foundation upon which to develop novel phenomena that exploit both the bulk and surface states (e.g., topological superconductivity).

Surfactant mediated synthesis of bismuth selenide thin films for photoelectrochemical solar cell applications.

PubMed

Desai, Neha D; Khot, Kishorkumar V; Ghanwat, Vishvanath B; Kharade, Suvarta D; Bhosale, Popatrao N

2018-03-15

In the present report, nanostructured bismuth selenide (Bi 2 Se 3 ) thin films have been successfully deposited by using arrested precipitation technique (APT) at room temperature. The effect of three different surfactants on the optostructural, morphological, compositional and photoelectrochemical properties of Bi 2 Se 3 thin films were investigated. Optical absorption data indicates direct and allowed transition with a band gap energy varied from 1.4 eV to 1.8 eV. The X-ray diffraction pattern (XRD) revealed that Bi 2 Se 3 thin films are crystalline in nature and confirmed rhombohedral crystal structure. SEM micrographs shows morphological transition from interconnected mesh to nanospheres like and finally granular morphology. Surface topography of Bi 2 Se 3 thin films was determined by AFM. Compositional analysis of all samples was carried out by energy dispersive X-ray spectroscopy (EDS). Finally, all Bi 2 Se 3 thin films shows good PEC performance with highest photoconversion efficiency 1.47%. In order to study the stability of Bi 2 Se 3 thin films four cycles are repeated after gap of one week each. Further PEC performance of all Bi 2 Se 3 thin films are also supported by electrochemical impedance (EIS) measurement study. Copyright © 2017 Elsevier Inc. All rights reserved.

Multi-Layer SnSe Nanoflake Field-Effect Transistors with Low-Resistance Au Ohmic Contacts

NASA Astrophysics Data System (ADS)

Cho, Sang-Hyeok; Cho, Kwanghee; Park, No-Won; Park, Soonyong; Koh, Jung-Hyuk; Lee, Sang-Kwon

2017-05-01

We report p-type tin monoselenide (SnSe) single crystals, grown in double-sealed quartz ampoules using a modified Bridgman technique at 920 °C. X-ray powder diffraction (XRD) and energy dispersive X-ray spectroscopy (EDX) measurements clearly confirm that the grown SnSe consists of single-crystal SnSe. Electrical transport of multi-layer SnSe nanoflakes, which were prepared by exfoliation from bulk single crystals, was conducted using back-gated field-effect transistor (FET) structures with Au and Ti contacts on SiO2/Si substrates, revealing that multi-layer SnSe nanoflakes exhibit p-type semiconductor characteristics owing to the Sn vacancies on the surfaces of SnSe nanoflakes. In addition, a strong carrier screening effect was observed in 70-90-nm-thick SnSe nanoflake FETs. Furthermore, the effect of the metal contacts to multi-layer SnSe nanoflake-based FETs is also discussed with two different metals, such as Ti/Au and Au contacts.

Orbital selectivity causing anisotropy and particle-hole asymmetry in the charge density wave gap of 2 H - TaS 2

DOE Office of Scientific and Technical Information (OSTI.GOV)

Zhao, J.; Wijayaratne, K.; Butler, A.

We report an in-depth angle-resolved photoemission spectroscopy study on 2H-TaS2, a canonical incommensurate charge density wave (CDW) system. This study demonstrates that just as in related incommensurate CDW systems, 2H-TaSe2 and 2H-NbSe2, the energy gap (triangle(CDW)) of 2H-TaS2 is localized along the K-centered Fermi surface barrels and is particle-hole asymmetric. The persistence of triangle(CDW) even at temperatures higher than the CDW transition temperature T-CDW in 2H-TaS2, reflects the similar pseudogap behavior observed previously in 2H-TaSe2 and 2H-NbSe2. However, in sharp contrast to 2H-NbSe2, where triangle(CDW) is nonzero only in the vicinity of a few "hot spots" on the innerK-centered Fermimore » surface barrels, triangle(CDW) in 2H-TaS2 is nonzero along the entirety of both K-centered Fermi surface barrels. Based on a tight-binding model, we attribute this dichotomy in the momentum dependence and the Fermi surface specificity of triangle(CDW) between otherwise similar CDW compounds to the different orbital orientations of their electronic states that participate in the CDW pairing. Our results suggest that the orbital selectivity plays a critical role in the description of incommensurate CDW materials.« less

Synthesis and Spectroscopy of Silver-Doped PbSe Quantum Dots

DOE PAGES

Kroupa, Daniel M.; Hughes, Barbara K.; Miller, Elisa M.; ...

2017-06-25

Electronic impurity doping of bulk semiconductors is an essential component of semiconductor science and technology. Yet there are only a handful of studies demonstrating control of electronic impurities in semiconductor nanocrystals. Here, we studied electronic impurity doping of colloidal PbSe quantum dots (QDs) using a postsynthetic cation exchange reaction in which Pb is exchanged for Ag. We found that varying the concentration of dopants exposed to the as-synthesized PbSe QDs controls the extent of exchange. The electronic impurity doped QDs exhibit the fundamental spectroscopic signatures associated with injecting a free charge carrier into a QD under equilibrium conditions, including amore » bleach of the first exciton transition and the appearance of a quantum-confined, low-energy intraband absorption feature. Photoelectron spectroscopy confirms that Ag acts as a p-type dopant for PbSe QDs and infrared spectroscopy is consistent with k • p calculations of the size-dependent intraband transition energy. We find that to bleach the first exciton transition by an average of 1 carrier per QD requires that approximately 10% of the Pb be replaced by Ag. Here, we hypothesize that the majority of incorporated Ag remains at the QD surface and does not interact with the core electronic states of the QD. Instead, the excess Ag at the surface promotes the incorporation of <1% Ag into the QD core where it causes p-type doping behavior.« less

Saddle-like topological surface states on the T T'X family of compounds (T , T' = Transition metal, X =Si , Ge)

NASA Astrophysics Data System (ADS)

Singh, Bahadur; Zhou, Xiaoting; Lin, Hsin; Bansil, Arun

2018-02-01

Topological nodal-line semimetals are exotic conductors that host symmetry-protected conducting nodal lines in their bulk electronic spectrum and nontrivial drumhead states on the surface. Based on first-principles calculations and an effective model analysis, we identify the presence of topological nodal-line semimetal states in the low crystalline symmetric T T'X family of compounds (T ,T' = transition metal, X = Si or Ge) in the absence of spin-orbit coupling (SOC). Taking ZrPtGe as an exemplar system, we show that owing to small lattice symmetry this material harbors a single nodal line on the ky=0 plane with large energy dispersion and unique drumhead surface state with a saddlelike energy dispersion. When the SOC is included, the nodal line gaps out and the system transitions to a strong topological insulator state with Z2=(1 ;000 ) . The topological surface state evolves from the drumhead surface state via the sharing of its saddlelike energy dispersion within the bulk energy gap. These features differ remarkably from those of the currently known topological surface states in topological insulators such as Bi2Se3 with Dirac-cone-like energy dispersions.

Quantum Hall Ferroelectrics and Nematics in Multivalley Systems

NASA Astrophysics Data System (ADS)

Sodemann, Inti; Zhu, Zheng; Fu, Liang

2017-10-01

We study broken symmetry states at integer Landau-level fillings in multivalley quantum Hall systems whose low-energy dispersions are anisotropic. When the Fermi surface of individual pockets lacks twofold rotational symmetry, like in bismuth (111) [Feldman et al. , Observation of a Nematic Quantum Hall Liquid on the Surface of Bismuth, Science 354, 316 (2016), 10.1126/science.aag1715] and in Sn1 -xPbxSe (001) [Dziawa et al., Topological Crystalline Insulator States in Pb1 -xSnxSe , Nat. Mater. 11, 1023 (2012), 10.1038/nmat3449] surfaces, interactions tend to drive the formation of quantum Hall ferroelectric states. We demonstrate that the dipole moment in these states has an intimate relation to the Fermi surface geometry of the parent metal. In quantum Hall nematic states, like those arising in AlAs quantum wells, we demonstrate the existence of unusually robust Skyrmion quasiparticles.

Opto-electronic characterizations of oriented nano-structure CdSe film/Si (0 0 1) heterostructure

NASA Astrophysics Data System (ADS)

Al-Kotb, M. S.; Al-Waheidi, Jumana Z.; Kotkata, M. F.

2014-05-01

Nano-crystalline CdSe thin films were fabricated by evaporating CdSe nano-powders on glass and p-Si (0 0 1) substrates. X-ray diffraction analysis indicated the hexagonal structure for the growing film along the (0 0 2) plane. The results revealed that the thermally evaporated thin film has a comparatively smoother surface with grain size ˜21 nm. Analysis of the absorption coefficient dependence on the photon energy predicts two direct band-gap values of 2.11 ± 0.02 and 1.71 ± 0.03 eV. On the basis of the Wemple-diDomenico single oscillator model, the values of single oscillator energy (Eu) and oscillator dispersion energy (Ed) found to be 2.71 ± 0.09 and 12.94 ± 0.35 eV, respectively. The photoluminescence measurements show levels at the following values: 1.824, 1.786, 1.682, and 1.617 eV confirming the native defects existence in the gap of CdSe films because of stoichiometric deviation. The forward I-V characteristics of Ni/CdSe/p-Si (0 0 1) structure have been primarily analyzed within the framework of a standard thermionic emission theory over the temperature range of 160-360 K. The characteristic parameters of the Ni/CdSe/p-Si(0 0 1) structure such as barrier height (φb), ideality factor (n), and series resistance (Rs) have been calculated using a method developed by Cheung-Cheung.

Thickness-dependent transition of the valence band shape from parabolic to Mexican-hat-like in the MBE grown InSe ultrathin films

NASA Astrophysics Data System (ADS)

Kibirev, I. A.; Matetskiy, A. V.; Zotov, A. V.; Saranin, A. A.

2018-05-01

Using molecular beam epitaxy, InSe films of thicknesses from one to six quadruple layers were grown on Si(111). The surface morphology and structure of the InSe films were monitored using reflection high-energy electron diffraction and scanning tunneling microscopy observations. Angle resolved photoemission experiments revealed that the bulk-like parabolic shape of the valence band of InSe/Si(111) changes for the so-called "Mexican hat" shape when the thickness of the InSe film reduces to one and two quadruple layers. The observed effect is in a qualitative agreement with the reported calculation results on the free-standing InSe films. However, in the InSe/Si(111) system, the features used to characterize the Mexican hat dispersion appear to be more pronounced, which makes the one- and two-quadruple InSe layers on Si(111) promising candidates as thermoelectric materials.

STS studies of the surface of Bi2Se3

NASA Astrophysics Data System (ADS)

Romanowich, Megan; Lee, Mal-Soon; Mahanti, S. D.; Tessmer, Stuart; Chung, Duck Young; Song, Jung-Hwan; Kanatzidis, Mercouri

2012-02-01

We apply scanning tunneling spectroscopy to characterize the surface of the topological insulator Bi2Se3. Spectroscopy reveals that the minimum in the local density of states (LDOS) does not actually vanish in the region where Dirac cone states exist. We demonstrate with density functional theory calculations that this can be understood in terms of an asymmetric addition to the LDOS associated with a contribution from the bulk valence band that overlaps in energy with the Dirac point. We will discuss the origin of the fluctuations in the LDOS seen in the experiment near 0.2 eV above the Dirac point, which are associated with tunneling into the lowest conduction band states.

Elucidating the role of surface passivating ligand structural parameters in hole wave function delocalization in semiconductor cluster molecules.

PubMed

Teunis, Meghan B; Nagaraju, Mulpuri; Dutta, Poulami; Pu, Jingzhi; Muhoberac, Barry B; Sardar, Rajesh; Agarwal, Mangilal

2017-09-28

This article describes the mechanisms underlying electronic interactions between surface passivating ligands and (CdSe) 34 semiconductor cluster molecules (SCMs) that facilitate band-gap engineering through the delocalization of hole wave functions without altering their inorganic core. We show here both experimentally and through density functional theory calculations that the expansion of the hole wave function beyond the SCM boundary into the ligand monolayer depends not only on the pre-binding energetic alignment of interfacial orbitals between the SCM and surface passivating ligands but is also strongly influenced by definable ligand structural parameters such as the extent of their π-conjugation [π-delocalization energy; pyrene (Py), anthracene (Anth), naphthalene (Naph), and phenyl (Ph)], binding mode [dithiocarbamate (DTC, -NH-CS 2 - ), carboxylate (-COO - ), and amine (-NH 2 )], and binding head group [-SH, -SeH, and -TeH]. We observe an unprecedentedly large ∼650 meV red-shift in the lowest energy optical absorption band of (CdSe) 34 SCMs upon passivating their surface with Py-DTC ligands and the trend is found to be Ph- < Naph- < Anth- < Py-DTC. This shift is reversible upon removal of Py-DTC by triethylphosphine gold(i) chloride treatment at room temperature. Furthermore, we performed temperature-dependent (80-300 K) photoluminescence lifetime measurements, which show longer lifetime at lower temperature, suggesting a strong influence of hole wave function delocalization rather than carrier trapping and/or phonon-mediated relaxation. Taken together, knowledge of how ligands electronically interact with the SCM surface is crucial to semiconductor nanomaterial research in general because it allows the tuning of electronic properties of nanomaterials for better charge separation and enhanced charge transfer, which in turn will increase optoelectronic device and photocatalytic efficiencies.

Synthesis of ZnSe and ZnSe:Cu quantum dots by a room temperature photochemical (UV-assisted) approach using Na2 SeO3 as Se source and investigating optical properties.

PubMed

Khafajeh, R; Molaei, M; Karimipour, M

2017-06-01

In this study, ZnSe and ZnSe:Cu quantum dots (QDs) were synthesized using Na 2 SeO 3 as the Se source by a rapid and room temperature photochemical (UV-assisted) approach. Thioglycolic acid (TGA) was employed as the capping agent and UV illumination activated the chemical reactions. Synthesized QDs were successfully characterized using X-ray diffraction (XRD), transmission electron microscopy (TEM), photoluminescence (PL) and UV-visible (UV-vis) spectroscopy, Fourier transform-infrared (FT-IR), and energy dispersive X-ray spectroscopy (EDX). XRD analysis demonstrated the cubic zinc blend phase QDs. TEM images indicated that round-shaped particles were formed, most of which had a diameter of about 4 nm. The band gap of the ZnSe QDs was higher than that for ZnSe in bulk. PL spectra indicated an emission with three peaks related to the excitonic, surface trap states and deep level (DL) states. The band gap and QD emission were tunable only by UV illumination time during synthesis. ZnSe:Cu showed green emission due to transition of electrons from the Conduction band (CB) or surface trap states to the 2 T 2 acceptor levels of Cu 2 + . The emission was increased by increasing the Cu 2 + ion concentration, such that the optimal value of PL intensity was obtained for the nominal mole ratio of Cu:Zn 1.5%. Copyright © 2016 John Wiley & Sons, Ltd.

Persistent Charge-Density-Wave Order in Single-Layer TaSe2.

PubMed

Ryu, Hyejin; Chen, Yi; Kim, Heejung; Tsai, Hsin-Zon; Tang, Shujie; Jiang, Juan; Liou, Franklin; Kahn, Salman; Jia, Caihong; Omrani, Arash A; Shim, Ji Hoon; Hussain, Zahid; Shen, Zhi-Xun; Kim, Kyoo; Min, Byung Il; Hwang, Choongyu; Crommie, Michael F; Mo, Sung-Kwan

2018-02-14

We present the electronic characterization of single-layer 1H-TaSe 2 grown by molecular beam epitaxy using a combined angle-resolved photoemission spectroscopy, scanning tunneling microscopy/spectroscopy, and density functional theory calculations. We demonstrate that 3 × 3 charge-density-wave (CDW) order persists despite distinct changes in the low energy electronic structure highlighted by the reduction in the number of bands crossing the Fermi energy and the corresponding modification of Fermi surface topology. Enhanced spin-orbit coupling and lattice distortion in the single-layer play a crucial role in the formation of CDW order. Our findings provide a deeper understanding of the nature of CDW order in the two-dimensional limit.

Influence of Te and Se doping on ZnO films growth by SILAR method

NASA Astrophysics Data System (ADS)

Güney, Harun; Duman, Ćaǧlar

2016-04-01

The AIP Successive ionic layer adsorption and reaction (SILAR) is an economic and simple method to growth thin films. In this study, SILAR method is used to growth Selenium (Se) and Tellurium (Te) doped zinc oxide (ZnO) thin films with different doping rates. For characterization of the films X-ray diffraction (XRD), absorbance and scanning electron microscopy (SEM) are used. XRD results are showed well-defined strongly (002) oriented crystal structure for all samples. Also, absorbance measurements show, Te and Se concentration are proportional and inversely proportional with band gap energy, respectively. SEM measurements show that the surface morphology and thickness of the material varied with Se and/or Te and varying concentrations.

Influence of Te and Se doping on ZnO films growth by SILAR method

DOE Office of Scientific and Technical Information (OSTI.GOV)

Güney, Harun, E-mail: harunguney25@hotmail.com; Duman, Çağlar, E-mail: caglarduman@erzurum.edu.tr

2016-04-18

The AIP Successive ionic layer adsorption and reaction (SILAR) is an economic and simple method to growth thin films. In this study, SILAR method is used to growth Selenium (Se) and Tellurium (Te) doped zinc oxide (ZnO) thin films with different doping rates. For characterization of the films X-ray diffraction (XRD), absorbance and scanning electron microscopy (SEM) are used. XRD results are showed well-defined strongly (002) oriented crystal structure for all samples. Also, absorbance measurements show, Te and Se concentration are proportional and inversely proportional with band gap energy, respectively. SEM measurements show that the surface morphology and thickness ofmore » the material varied with Se and/or Te and varying concentrations.« less

Penetration Depth Study of Superconducting Gap Structure of 2H-NbSe2

NASA Astrophysics Data System (ADS)

Fletcher, J. D.; Carrington, A.; Diener, P.; Rodière, P.; Brison, J. P.; Prozorov, R.; Olheiser, T.; Giannetta, R. W.

2007-02-01

We report measurements of the temperature dependence of both in-plane and out-of-plane penetration depths (λa and λc, respectively) in 2H-NbSe2. Measurements were made with a radio-frequency tunnel diode oscillator circuit at temperatures down to 100 mK. Analysis of the anisotropic superfluid density shows that a reduced energy gap is located on one or more of the quasi-two-dimensional Nb Fermi surface sheets rather than on the Se sheet, in contrast with some previous reports. This result suggests that the gap structure is not simply related to the weak electron-phonon coupling on the Se sheet and is therefore important for microscopic models of anisotropic superconductivity in this compound.

Thickness dependent structural, optical and electrical properties of Se85In12Bi3 nanochalcogenide thin films

NASA Astrophysics Data System (ADS)

Tripathi, Ravi P.; Zulfequar, M.; Khan, Shamshad A.

2018-04-01

Our aim is to study the thickness dependent effects on structure, electrical and optical properties of Se85In12Bi3 nanochalcogenide thin films. Bulk alloy of Se85In12Bi3 was synthesized by melt-quenching technique. The amorphous as well as glassy nature of Se85In12Bi3 chalcogenide was confirmed by non-isothermal Differential Scanning Calorimetry (DSC) measurements. The nanochalcogenide thin films of thickness 30, 60 and 90 nm were prepared on glass/Si wafer substrate using Physical Vapour Condensation Technique (PVCT). From XRD studies it was found that thin films have amorphous texture. The surface morphology and particle size of films were studied by Field Emission Scanning Electron Microscope (FESEM). From optical studies, different optical parameters were estimated for Se85In12Bi3 thin films at different thickness. It was found that the absorption coefficient (α) and extinction coefficient (k) increases with photon energy and decreases with film thickness. The optical absorption process followed the rule of indirect transitions and optical band gap were found to be increase with film thickness. The value of Urbach energy (Et) and steepness parameter (σ) were also calculated for different film thickness. For electrical studies, dc-conductivity measurement was done at different temperature and activation energy (ΔEc) were determined and found to be increase with film thickness.

Integrated MoSe2 with n+p-Si photocathodes for solar water splitting with high efficiency and stability

NASA Astrophysics Data System (ADS)

Huang, Guanping; Mao, Jie; Fan, Ronglei; Yin, Zhihao; Wu, Xi; Jie, Jiansheng; Kang, Zhenhui; Shen, Mingrong

2018-01-01

Many earth-abundant transition metal dichalcogenides (TMDs) have been employed as catalysts for H2 evolution reaction (HER); however, their impactful integration onto photocathodes for photoelectrochemical (PEC) HER is less developed. In this study, we directly sputtered a MoSe2 catalyst onto an n+p-Si photocathode for efficient and stable PEC-HER. An onset potential of 0.4 V vs. RHE, a saturated photocurrent of 29.3 mA/cm2, a fill factor of 0.32, and an energy conversion efficiency of 3.8% were obtained under 100 mA/cm2 Xe lamp illumination. Such superior PEC properties were ascribed to the nearly vertically standing two dimensional MoSe2 rough surface layer and the sharp interface between Si and MoSe2 with small charge transfer resistance. The balance between the reflectivity of the electrode surface and the absorptivity of MoSe2 was also discussed. In addition, the MoSe2 layer can protect the n+p-Si photocathode with a 120 h stability due to its initial growth on Si with high flatness and compactness. This study provides a path to the effective and scalable growth of TMDs onto the Si photocathode aiming for high efficiency and stability.

Electrochemical synthesis of nanostructured Se-doped SnS: Effect of Se-dopant on surface characterizations

NASA Astrophysics Data System (ADS)

Kafashan, Hosein; Azizieh, Mahdi; Balak, Zohre

2017-07-01

SnS1-xSex nanostructures with different Se-dopant concentrations were deposited on fluorine doped tin oxide (FTO) substrate through cathodic electrodeposition technique. The pH, temperature, applied potential (E), and deposition time remained were 2.1, 60 °C, -1 V, and 30 min, respectively. SnS1-xSex nanostructures were characterized using X-ray diffraction (XRD), field emission scanning electron microcopy (FESEM), energy dispersive X-ray spectroscopy (EDX), room temperature photoluminescence (PL), and UV-vis spectroscopy. The XRD patterns revealed that the SnS1-xSex nanostructures were polycrystalline with orthorhombic structure. FESEM showed various kinds of morphologies in SnS1-xSex nanostructures due to Se-doping. PL and UV-vis spectroscopy were used to evaluate the optical properties of SnS1-xSex thin films. The PL spectra of SnS1-xSex nanostructures displayed four emission peaks, those are a blue, a green, an orange, and a red emission. UV-vis spectra showed that the optical band gap energy (Eg) of SnS1-xSex nanostructures varied between 1.22-1.65 eV, due to Se-doping.

Ab initio study of the adsorption, diffusion, and intercalation of alkali metal atoms on the (0001) surface of the topological insulator Bi{sub 2}Se{sub 3}

DOE Office of Scientific and Technical Information (OSTI.GOV)

Ryabishchenkova, A. G., E-mail: ryaange@gmail.com; Otrokov, M. M.; Kuznetsov, V. M.

2015-09-15

Ab initio study of the adsorption, diffusion, and intercalation of alkali metal adatoms on the (0001) step surface of the topological insulator Bi{sub 2}Se{sub 3} has been performed for the case of low coverage. The calculations of the activation energies of diffusion of adatoms on the surface and in van der Waals gaps near steps, as well as the estimate of diffusion lengths, have shown that efficient intercalation through steps is possible only for Li and Na. Data obtained for K, Rb, and Cs atoms indicate that their thermal desorption at high temperatures can occur before intercalation. The results havemore » been discussed in the context of existing experimental data.« less

Effect of copper concentration in the electrolyte on the surface morphology and the microstructure of CuInSe2 films

NASA Astrophysics Data System (ADS)

Hung, Pin-Kun; Kuo, Ting-Wei; Huang, Kuo-Chan; Wang, Na-Fu; Hsieh, Po-Tsung; Houng, Mau-Phon

2012-07-01

The surface morphology and the microstructure of CuInSe2 precursor films have been investigated by co-electrodeposition with different [Cu2+] concentrations from 2 mM to 4 mM. The characteristic of the precursor films was examined using field-emission scanning electron microscopy (FE-SEM), energy dispersive X-ray spectroscopy (EDS), glancing incidence angle X-ray diffraction (GIXRD) and micro-Raman spectrometer, respectively. The surface morphology of the precursor films become more smoother and compact with choice of appropriate [Cu2+] concentration (3-3.5 mM) in the electrolyte. The relation between surface morphology and [Cu2+] concentration is also considered in terms of electrodeposition nucleation mechanisms using the mathematical models of Scharifker and Hills. It is suggested that the higher [Cu2+] concentrations can provide more numbers of nucleation sites on the surface of the electrode. Results simulated from the Rietveld refinement method suggest that decreasing dCusbnd Se is related to charge transfer from interstitial copper atoms and can affect the film microstructure. Micro-Raman spectrum also shows that the excess Cu atoms in the precursor films does not contribute significantly to large amounts of secondary phases but rather exists in the crystallite structure as other defect types.

Synthesis and characterization of ZnO/ZnSe NWs/PbS QDs solar cell

NASA Astrophysics Data System (ADS)

Kamruzzaman, M.; Zapien, J. A.

2017-04-01

The capture of solar energy has gained the attention for the next generation solar cell. ZnO/ZnSe NW arrays were synthesized on an FTO glass substrate using a simple and facile hydrothermal and ion-exchange approaches. The lead sulfide (PbS) QDs was infiltrated into ZnO/ZnSe NWs via SILAR method for making inorganic quantum dot sensitized ZnO/ZnSe/PbS QDs solar cell. The surface morphology, structural, optical, and J-V characteristics have been investigated. The ZnO/ZnSe NW is a core-shell like structure, and the absorption edge shifted from the UV region (ZnO NWs) to the near infrared region for ZnO/ZnSe NWs/PbS QDs. For PbS QDs-sensitized solar cell, the obtained value of η = 1.1%, J sc = 20.60 mA/cm2, V oc = 155 mV, and FF = 34.7%, respectively. The photovoltaic performance of the device in this study is still inferior. However, it is the first report regarding to ZnO/ZnZe NWs/PbS QDs solar cell. The achieving high absorption and large short circuit current density may interest in further improvement of the device performance by suppressing surface defects, optimizing the quality of ZnO/ZnSe NWs and PbS QDs.

Manipulating Nonlinear Emission and Cooperative Effect of CdSe/ZnS Quantum Dots by Coupling to a Silver Nanorod Complex Cavity

PubMed Central

Nan, Fan; Cheng, Zi-Qiang; Wang, Ya-Lan; Zhang, Qing; Zhou, Li; Yang, Zhong-Jian; Zhong, Yu-Ting; Liang, Shan; Xiong, Qihua; Wang, Qu-Quan

2014-01-01

Colloidal semiconductor quantum dots have three-dimensional confined excitons with large optical oscillator strength and gain. The surface plasmons of metallic nanostructures offer an efficient tool to enhance exciton-exciton coupling and excitation energy transfer at appropriate geometric arrangement. Here, we report plasmon-mediated cooperative emissions of approximately one monolayer of ensemble CdSe/ZnS quantum dots coupled with silver nanorod complex cavities at room temperature. Power-dependent spectral shifting, narrowing, modulation, and amplification are demonstrated by adjusting longitudinal surface plasmon resonance of silver nanorods, reflectivity and phase shift of silver nanostructured film, and mode spacing of the complex cavity. The underlying physical mechanism of the nonlinear excitation energy transfer and nonlinear emissions are further investigated and discussed by using time-resolved photoluminescence and finite-difference time-domain numerical simulations. Our results suggest effective strategies to design active plasmonic complex cavities for cooperative emission nanodevices based on semiconductor quantum dots. PMID:24787617

Highly Enhanced Fluorescence of CdSeTe Quantum Dots Coated with Polyanilines via In-Situ Polymerization and Cell Imaging Application.

PubMed

Xue, Jingjing; Chen, Xinyi; Liu, Shanglin; Zheng, Fenfen; He, Li; Li, Lingling; Zhu, Jun-Jie

2015-09-02

The polyaniline (PAN)-coated CdSeTe quantum dots (QDs) were prepared by in situ polymerization of aniline on the surface of CdSeTe QDs. The PAN-coated CdSeTe QDs has a tremendously enhanced fluorescence (∼40 times) and improved biocompatibility compared to the uncoated CdSeTe QDs. The fluorescence intensity of the PAN-coated CdSeTe QDs can be adjusted by controlling the construction parameters of the PAN shell. The kinetics of the in situ controllable polymerization process was studied by varying the temperature, and the apparent activation energy of polymerization was estimated. With the same method, a series of the PAN derivatives were also tested to coat the CdSeTe QDs in this study. All the QDs showed a significant enhancement of the fluorescence intensity and better biocompatibility. The significantly enhanced fluorescence can provide highly amplified signal for luminescence-based cell imaging.

2D layered transport properties from topological insulator Bi2Se3 single crystals and micro flakes

PubMed Central

Chiatti, Olivio; Riha, Christian; Lawrenz, Dominic; Busch, Marco; Dusari, Srujana; Sánchez-Barriga, Jaime; Mogilatenko, Anna; Yashina, Lada V.; Valencia, Sergio; Ünal, Akin A.; Rader, Oliver; Fischer, Saskia F.

2016-01-01

Low-field magnetotransport measurements of topological insulators such as Bi2Se3 are important for revealing the nature of topological surface states by quantum corrections to the conductivity, such as weak-antilocalization. Recently, a rich variety of high-field magnetotransport properties in the regime of high electron densities (∼1019 cm−3) were reported, which can be related to additional two-dimensional layered conductivity, hampering the identification of the topological surface states. Here, we report that quantum corrections to the electronic conduction are dominated by the surface states for a semiconducting case, which can be analyzed by the Hikami-Larkin-Nagaoka model for two coupled surfaces in the case of strong spin-orbit interaction. However, in the metallic-like case this analysis fails and additional two-dimensional contributions need to be accounted for. Shubnikov-de Haas oscillations and quantized Hall resistance prove as strong indications for the two-dimensional layered metallic behavior. Temperature-dependent magnetotransport properties of high-quality Bi2Se3 single crystalline exfoliated macro and micro flakes are combined with high resolution transmission electron microscopy and energy-dispersive x-ray spectroscopy, confirming the structure and stoichiometry. Angle-resolved photoemission spectroscopy proves a single-Dirac-cone surface state and a well-defined bulk band gap in topological insulating state. Spatially resolved core-level photoelectron microscopy demonstrates the surface stability. PMID:27270569

Rational Construction of Hollow Core-Branch CoSe2 Nanoarrays for High-Performance Asymmetric Supercapacitor and Efficient Oxygen Evolution.

PubMed

Chen, Tian; Li, Songzhan; Wen, Jian; Gui, Pengbin; Guo, Yaxiong; Guan, Cao; Liu, Jinping; Fang, Guojia

2018-02-01

Metal selenides have great potential for electrochemical energy storage, but are relatively scarce investigated. Herein, a novel hollow core-branch CoSe 2 nanoarray on carbon cloth is designed by a facile selenization reaction of predesigned CoO nanocones. And the electrochemical reaction mechanism of CoSe 2 in supercapacitor is studied in detail for the first time. Compared with CoO, the hollow core-branch CoSe 2 has both larger specific surface area and higher electrical conductivity. When tested as a supercapacitor positive electrode, the CoSe 2 delivers a high specific capacitance of 759.5 F g -1 at 1 mA cm -2 , which is much larger than that of CoO nanocones (319.5 F g -1 ). In addition, the CoSe 2 electrode exhibits excellent cycling stability in that a capacitance retention of 94.5% can be maintained after 5000 charge-discharge cycles at 5 mA cm -2 . An asymmetric supercapacitor using the CoSe 2 as cathode and an N-doped carbon nanowall as anode is further assembled, which show a high energy density of 32.2 Wh kg -1 at a power density of 1914.7 W kg -1 , and maintains 24.9 Wh kg -1 when power density increased to 7354.8 W kg -1 . Moreover, the CoSe 2 electrode also exhibits better oxygen evolution reaction activity than that of CoO. © 2017 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

In-Situ Probing Plasmonic Energy Transfer in Cu(In, Ga)Se2 Solar Cells by Ultrabroadband Femtosecond Pump-Probe Spectroscopy.

PubMed

Chen, Shih-Chen; Wu, Kaung-Hsiung; Li, Jia-Xing; Yabushita, Atsushi; Tang, Shih-Han; Luo, Chih Wei; Juang, Jenh-Yih; Kuo, Hao-Chung; Chueh, Yu-Lun

2015-12-18

In this work, we demonstrated a viable experimental scheme for in-situ probing the effects of Au nanoparticles (NPs) incorporation on plasmonic energy transfer in Cu(In, Ga)Se2 (CIGS) solar cells by elaborately analyzing the lifetimes and zero moment for hot carrier relaxation with ultrabroadband femtosecond pump-probe spectroscopy. The signals of enhanced photobleach (PB) and waned photoinduced absorption (PIA) attributable to surface plasmon resonance (SPR) of Au NPs were in-situ probed in transient differential absorption spectra. The results suggested that substantial carriers can be excited from ground state to lower excitation energy levels, which can reach thermalization much faster with the existence of SPR. Thus, direct electron transfer (DET) could be implemented to enhance the photocurrent of CIGS solar cells. Furthermore, based on the extracted hot carrier lifetimes, it was confirmed that the improved electrical transport might have been resulted primarily from the reduction in the surface recombination of photoinduced carriers through enhanced local electromagnetic field (LEMF). Finally, theoretical calculation for resonant energy transfer (RET)-induced enhancement in the probability of exciting electron-hole pairs was conducted and the results agreed well with the enhanced PB peak of transient differential absorption in plasmonic CIGS film. These results indicate that plasmonic energy transfer is a viable approach to boost high-efficiency CIGS solar cells.

Dual-energy computed tomography of the head: a phantom study assessing axial dose distribution, eye lens dose, and image noise level

NASA Astrophysics Data System (ADS)

Matsubara, Kosuke; Kawashima, Hiroki; Hamaguchi, Takashi; Takata, Tadanori; Kobayashi, Masanao; Ichikawa, Katsuhiro; Koshida, Kichiro

2016-03-01

The aim of this study was to propose a calibration method for small dosimeters to measure absorbed doses during dual- source dual-energy computed tomography (DECT) and to compare the axial dose distribution, eye lens dose, and image noise level between DE and standard, single-energy (SE) head CT angiography. Three DE (100/Sn140 kVp 80/Sn140 kVp, and 140/80 kVp) and one SE (120 kVp) acquisitions were performed using a second-generation dual-source CT device and a female head phantom, with an equivalent volumetric CT dose index. The axial absorbed dose distribution at the orbital level and the absorbed doses for the eye lens were measured using radiophotoluminescent glass dosimeters. CT attenuation numbers were obtained in the DE composite images and the SE images of the phantom at the orbital level. The doses absorbed at the orbital level and in the eye lens were lower and standard deviations for the CT attenuation numbers were slightly higher in the DE acquisitions than those in the SE acquisition. The anterior surface dose was especially higher in the SE acquisition than that in the DE acquisitions. Thus, DE head CT angiography can be performed with a radiation dose lower than that required for a standard SE head CT angiography, with a slight increase in the image noise level. The 100/Sn140 kVp acquisition revealed the most balanced axial dose distribution. In addition, our proposed method was effective for calibrating small dosimeters to measure absorbed doses in DECT.

Spatial variations of the local density of states modified by CDWs in 1 T- TaS2- xSex

NASA Astrophysics Data System (ADS)

Hasegawa, T.; Yamaguchi, W.; Kim, J.-J.; Wei, W.; Nantoh, M.; Ikuta, H.; Kitazawa, K.; Manivannan, A.; Fujishima, A.; Uchinokura, K.

1994-07-01

Spatial variations of the local density of states (LDOS) near the Fermi level have been observed on the layered dichalcogenides 1 T- TaS2- xSex ( x = 0, 0.2, 2) for the first time. The tunneling spectra on the cleaved surfaces were measured by atomic-site tunneling (AST) spectroscopy technique at room temperature. In 1T-TaS 2, the LDOS was substantially different among the three inequivalent Ta atomic sites induced by the CDW formation. However, the surface electronic structure became homogeneous, as the Se content was increased. By substituting Se for S, the minimum position of the LDOS was systematically shifted to a higher energy side above the Fermi level.

Electronic structure and optical properties of noncentrosymmetric LiGaGe2Se6, a promising nonlinear optical material

NASA Astrophysics Data System (ADS)

Lavrentyev, A. A.; Gabrelian, B. V.; Vu, V. T.; Ananchenko, L. N.; Isaenko, L. I.; Yelisseyev, A.; Krinitsin, P. G.; Khyzhun, O. Y.

2016-11-01

X-ray photoelectron core-level and valence-band spectra are measured for pristine and Ar+ ion-bombarded surfaces of LiGaGe2Se6 single crystal grown by Bridgman-Stockbarger technique. Further, electronic structure of LiGaGe2Se6 is elucidated from both theoretical and experimental viewpoints. Density functional theory (DFT) calculations are made using the augmented plane wave +local orbitals (APW+lo) method to study total and partial densities of states in the LiGaGe2Se6 compound. The present calculations indicate that the principal contributors to the valence band are the Se 4p states: they contribute mainly at the top and in the central portion of the valence band of LiGaGe2Se6, with also their significant contributions in its lower portion. The Ge 4s and Ge 4p states are among other significant contributors to the valence band of LiGaGe2Se6, contributing mainly at the bottom and in the central portion, respectively. In addition, the calculations indicate that the bottom of the conduction band is composed mainly from the unoccupied Ge s and Se p states. The present DFT calculations are supported experimentally by comparison on a common energy scale of the X-ray emission bands representing the energy distribution of the 4p states associated with Ga, Ge and Se and the XPS valence-band spectrum of the LiGaGe2Se6 single crystal. The main optical characteristics of the LiGaGe2Se6 compound are elucidated by the first-principles calculations.

Defect specific luminescence dead layers in CdS and CdSe

DOE Office of Scientific and Technical Information (OSTI.GOV)

Rosenberg, R. A.

CdS and CdSe are often used in optoelectronic devices whose effectiveness is may be dictated by defects in the near surface region. Luminescence is one of the main tools for studying such defects. The energy dependence of the x-ray excited optical luminescence (XEOL) spectra of these materials enables the extraction of the depth dependence of the defect distribution. Normal and time-gated XEOL spectra were obtained from these materials in the energy range 600 to 1500 eV. Here, we find that the results can best be understood in terms of a luminescence dead layer whose width depends on the position ofmore » the defect level in the band gap.« less

Defect specific luminescence dead layers in CdS and CdSe

DOE PAGES

Rosenberg, R. A.

2017-04-28

CdS and CdSe are often used in optoelectronic devices whose effectiveness is may be dictated by defects in the near surface region. Luminescence is one of the main tools for studying such defects. The energy dependence of the x-ray excited optical luminescence (XEOL) spectra of these materials enables the extraction of the depth dependence of the defect distribution. Normal and time-gated XEOL spectra were obtained from these materials in the energy range 600 to 1500 eV. Here, we find that the results can best be understood in terms of a luminescence dead layer whose width depends on the position ofmore » the defect level in the band gap.« less

Effects of quantum confinement and shape on band gap of core/shell quantum dots and nanowires

NASA Astrophysics Data System (ADS)

Gao, Faming

2011-05-01

A quantum confinement model for nanocrystals developed is extended to study for the optical gap shifts in core/shell quantum dots and nanowires. The chemical bond properties and gap shifts in the InP/ZnS, CdSe/CdS, CdSe/ZnS, and CdTe/ZnS core/shell quantum dots are calculated in detail. The calculated band gaps are in excellent agreement with experimental values. The effects of structural taping and twinning on quantum confinement of InP and Si nanowires are elucidated. It is found theoretically that a competition between the positive Kubo energy-gap shift and the negative surface energy shift plays the crucial role in the optical gaps of these nanosystems.

Simulation of Electron Scattering in Complex Nanostructures: Lithography, Metrology, and Characterization.

NASA Astrophysics Data System (ADS)

Johnson, Sylvester, IV

A CAE (Computer Aided Engineering) tool called SEEL (Simulation of Electron Energy Loss) is described in detail. SEEL simulates in any material the energy loss and trajectories of electrons in the complex, multilayered nanostructures typical of ULSI, at beam energies from 1 to 50 keV. Structures and materials are defined in the input file rather than in the source code of the program, for which flowcharts are included in addition to an explanation of the algorithms implemented. Satisfactory comparisons of simulated with experimental results are made of both secondary electron (SE) and backscattered electron (BSE) linescans across an array of MOS gate structures capped by rough oxide. Many other comparisons are made. The effects of varying line edge slopes on SE linescan peak shape are simulated and analyzed. A data library containing the simulated variation of the FWHM, peak height, and peak location with slope for different materials, line heights or trench depths, widths, beam energies, and nominal diameters could be used to find the edge location relative to the peak for improvement of the accuracy of linewidth measurement algorithms. An investigation indicates that the use of such a library would be complicated by the effect of surface roughness on the SE signal at the edge of a feature. SEEL can be used as the first module in a series of programs that simulate energy deposition in resist structures and correct the exposure of a circuit pattern. Pixel by pixel convolution for prediction of the proximity effect is time-consuming. Another method of proximity effect prediction based on the reciprocity of the RED is described. Such programs could be used to reduce the number of iterations in the lab required to optimize resist structures and exposure parameters. For both smooth and rough interfaces between a bottom layer of PMMA in a multilayer resist structure and a W film, the simulated exposure contrast declines from that with an oxide film beneath the structure. A comparison of Auger peak to background ratios resulting from simulation of smooth and rough surfaces indicates that roughening of an Al surface on a small scale could result in a smaller ratio.

Sonocatalytic degradation of methylene blue by a novel graphene quantum dots anchored CdSe nanocatalyst.

PubMed

Sajjadi, Saeed; Khataee, Alireza; Kamali, Mehdi

2017-11-01

Cadmium selenide/graphene quantum dots (CdSe/GQDs) nanocatalyst with small band gap energy and a large specific surface area was produced via a facile three-step sonochemical-hydrothermal process. The features of the as-prepared CdSe, GQDs and CdSe/GQDs samples were characterized by photoluminescence spectroscopy (PL), scanning electron microscopy (SEM), energy dispersive X-ray (EDX), X-ray diffraction (XRD), Fourier transformed infrared (FT-IR), diffuse-reflectance spectrophotometer (DRS), and Brunauer-Emmett-Teller (BET) analysis. The sonocatalytic activity of the synthesized CdSe/GQDs was effectively accelerated compared with that of pure CdSe nanoparticles in degradation of methylene blue (MB). The influence of the CdSe/GQDs dosage (0.25-1.25g/L), initial MB concentration (20-30mg/L), initial solution pH (3-12), and ultrasonic output power (200-600W/L) were examined on the sonocatalytic treatment of MB aqueous solutions. The degradation efficiency (DE%) of 99% attained at 1g/L of CdSe/GQDs, 20mg/L of MB, pH of 9, and an output power of 200W/L at 90min of ultrasonic irradiation. Furthermore, DE% increased with addition of K 2 S 2 O 8 and H 2 O 2 as the enhancers via producing more free radicals. However, addition of sulfate, carbonate, and chloride as radical sweeper decreased DE%. Furthermore, well-reusability of the CdSe/GQDs sonocatalyst was demonstrated for 5 successive runs and some of the sonocatalytic generated intermediates were indicated by GC-MS analysis. Copyright © 2017 Elsevier B.V. All rights reserved.

Optimizing non-radiative energy transfer in hybrid colloidal-nanocrystal/silicon structures by controlled nanopillar architectures for future photovoltaic cells

NASA Astrophysics Data System (ADS)

Seitz, O.; Caillard, L.; Nguyen, H. M.; Chiles, C.; Chabal, Y. J.; Malko, A. V.

2012-01-01

To optimize colloidal nanocrystals/Si hybrid structures, nanopillars are prepared and organized via microparticle patterning and Si etching. A monolayer of CdSe nanocrystals is then grafted on the passivated oxide-free nanopillar surfaces, functionalized with carboxy-alkyl chain linkers. This process results to a negligible number of non-radiative surface state defects with a tightly controlled separation between the nanocrystals and Si. Steady-state and time-resolved photoluminescence measurements confirm the close-packing nanocrystal arrangement and the dominance of non-radiative energy transfer from nanocrystals to Si. We suggest that radially doped p-n junction devices based on energy transfer offer a viable approach for thin film photovoltaic devices.

Spray-painted binder-free SnSe electrodes for high-performance energy-storage devices.

PubMed

Wang, Xianfu; Liu, Bin; Xiang, Qingyi; Wang, Qiufan; Hou, Xiaojuan; Chen, Di; Shen, Guozhen

2014-01-01

SnSe nanocrystal electrodes on three-dimensional (3D) carbon fabric and Au-coated polyethylene terephthalate (PET) wafer have been prepared by a simple spray-painting process and were further investigated as binder-free active-electrodes for Lithium-ion batteries (LIBs) and flexible stacked all-solid-state supercapacitors. The as-painted SnSe nanocrystals/carbon fabric electrodes exhibit an outstanding capacity of 676 mAh g(-1) after 80 cycles at a current density of 200 mA g(-1) and a considerable high-rate capability in lithium storage because of the excellent ion transport from the electrolyte to the active materials and the efficient charge transport between current collector and electrode materials. The binder-free electrodes also provide a larger electrochemical active surface compared with electrodes containing binders, which leads to the enhanced capacities of energy-storage devices. A flexible stacked all-solid-state supercapacitor based on the SnSe nanocrystals on Au-coated PET wafers shows high capacitance reversibility with little performance degradation at different current densities after 2200 charge-discharge cycles and even when bent. This allows for many potential applications in facile, cost-effective, spray-paintable, and flexible energy-storage devices. The results indicate that the fabrication of binder-free electrodes by a spray painting process is an interesting direction for the preparation of high-performance energy-storage devices. Copyright © 2014 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Photophysical Properties of II-VI Semiconductor Nanocrystals

NASA Astrophysics Data System (ADS)

Gong, Ke

As it is well known, semiconductor nanocrystals (also called quantum dots, QDs) are being actively pursued for use in many different types of luminescent optical materials. These materials include the active media for luminescence downconversion in artificial lighting, lasers, luminescent solar concentrators and many other applications. Chapter 1 gives general introduction of QDs, which describe the basic physical properties and optical properties. Based on the experimental spectroscopic study, a semiquantitative method-effective mass model is employed to give theoretical prediction and guide. The following chapters will talks about several topics respectively. A predictive understanding of the radiative lifetimes is therefore a starting point for the understanding of the use of QDs for these applications. Absorption intensities and radiative lifetimes are fundamental properties of any luminescent material. Meantime, achievement of high efficiency with high working temperature and heterostructure fabrication with manipulation of lattice strain are not easy and need systematic investigation. To make accurate connections between extinction coefficients and radiative recombination rates, chapter 2 will consider three closely related aspects of the size dependent spectroscopy of II-VI QDs. First, it will consider the existing literature on cadmium selenide (CdSe) QD absorption spectra and extinction coefficients. From these results and fine structure considerations Boltzmann weighted radiative lifetimes are calculated. These lifetimes are compared to values measured on very high quality CdSe and CdSe coated with zinc selenide (ZnSe) shells. Second, analogous literature data are analyzed for cadmium telluride (CdTe) nanocrystals and compared to lifetimes measured for very high quality QDs. Furthermore, studies of the absorption and excitation spectra and measured radiative lifetimes for CdTe/CdSe Type-II core/shell QDs are reported. These results are also analyzed in terms of a Boltzmann population of exciton sublevels and calculated electron and hole wave functions. Much of the absorption data and fine structure calculations are already in the literature. These results are combined with new measurements of radiative lifetimes and electron-hole overlap calculations to produce an integrated picture of the II-VI QD spectroscopic fundamentals. Finally, we adopt recent synthetic advances to make very monodisperse zincblende CdSe/CdS quantum dots having near-unity photoluminescence quantum yields (PLQYs). Due the absence of nonradiative decay pathways, accurate values of the radiative lifetimes can be obtained from time resolved PL measurements. Radiative lifetimes can also be obtained from the Einstein relations, using the static absorption spectra and the relative thermal populations in the angular momentum sublevels. One of the inputs into these calculations is the shell thickness, and it is useful to be able to determine shell thickness from spectroscopic measurements. We use an empirically corrected effective mass model to produce a "map" of exciton wavelength as a function of core size and shell thickness. These calculations use an elastic continuum model and the known lattice and elastic constants to include the effect of lattice strain on the band gap energy. Radiative lifetimes calculated both experimentally and theoretically are checked and the size dependence is compared to previous studied Type-I, II and single component particles. However, it is not enough to just understanding these basic photophysics of absorption and emission. The emission intensities (related to QYs) also change with changes of the temperature. The temperature dependent PLs of II-VI QDs is extensively studied, but most of this work is at low temperatures. Temperatures well above ambient are of interest to lighting applications and in this regime both the reversible and irreversible loss of quantum yield (thermal quenching) are serious impediments to the implementation of QDs in commercial devices. Chapter 3 will elucidate the mechanism of static thermal quenching, in which the reduction of QYs does not affect the PL decay kinetics, on CdSe, CdTe and CdSe/ZnSe QDs as a function of particle sizes/shapes, surface composition and surface ligands. Through systematic experiments, this part of the dissertation discusses several possible mechanisms (e.g. structural, activated excited state, and electronic charging) and examines which the dominant cause for loss of QY at high temperature is. The more practical step is to develop the synthetic method of highly luminescent and stable core/shell QDs with minimum thermal quenching, which greatly enhance the energy efficiency of light emitting and photovoltaic devices. As the nonradiative Auger processed are induced by surface charging described in chapter 3, static and time-resolved fluorescence and high and low power transient absorption results on CdSe/CdS and CdSe/ZnSe core/shell particles are presented in chapter 4. Two CdS shell thicknesses were examined and all of the particles had either octadecylamine (ODA) and tributylphosphine (TBP) or just ODA ligands. The results can be understood in terms of a mechanism in which there is a thermal equilibrium between electrons being in the valence band or in chalcogenide localized surface states. Thermal promotion of a valence band electron to a surface state leaves the particle core positively charged. Photon absorption when the particle is in this state results in a positive trion, which undergoes a fast Auger recombination, making the particle nonluminescent. A lack of TBP ligands results in more empty surface orbitals and therefore shifts the equilibrium toward surface trapped electrons and hence trion formation. Low- and high-power transient absorption measurements give the trion and biexciton lifetimes and the ratio of the trion to biexciton Auger lifetimes are examined and compared to the degeneracies of Auger pathways. We also study the shell thickness and composition dependence of Auger times, which is compared to the scaling factors of effective volume and electron-hole overlap considerations. Core/shell QDs often exhibit much higher luminescence quantum yields (QYs), more stability, and are depicted as having a nearly spherical core and a shell of very nearly uniform thickness, which results in a very simple picture of surface passivation. The uniformity of the shell is crucial in obtaining QDs with well passivated surfaces. However, transmission electron microscope (TEM) images disprove the ideal situation. Defects and thickness inhomogeneity in shell materials are treated qualitatively as an analog to film thickness inhomogeneity in epitaxially grown thin films. More quantitatively, the extent to which the shell thickness of core/shell particles is constant can be determined by time-resolved PL studies that measure the dynamics of hole tunneling to acceptors that are adsorbed on the shell surface due that tunneling rates varies strongly with core-acceptor separation. Careful analysis of the hole transfer kinetics reveals the extent of shell thickness inhomogeneity, however, it may be complicated by the distribution of numbers of adsorbed acceptors. All the considerations can be incorporated into a model we establish in Chapter 5for the distribution of measured hole tunneling rates. From this analysis the distribution of shell thicknesses can be extracted from the luminescence kinetic results. This approach is therefore a sensitive measure of the distribution of tunneling distances. Thus, any defects or structural irregularities that allow the hole acceptors to adsorb closer to the particle core increases the hole tunneling rate and can be detected and quantified. A quantitative treatment of the lattice strain energy in determining the shell morphology of CdSe/CdS core/shell nanoparticles is presented in chapter 5. We use the inhomogeneity in hole tunneling rates through the shell to adsorbed hole acceptors to quantify the extent of shell thickness inhomogeneity. The results can be understood in terms of a model based on elastic continuum calculations, which indicate that the lattice strain energy depends on both core size and shell thickness. This model assumes thermodynamic equilibrium, i.e., that the shell morphology corresponds to a minimum total (lattice strain plus surface) energy. Comparison with the experimental results indicates that CdSe/CdS nanoparticles undergo an abrupt transition from smooth to rough shells when the total lattice strain energy exceeds about 27eV or the strain energy density exceeds 0.59 eV/nm2. The predictions of this model are not followed for CdSe/CdS nanoparticles when the shell is deposited at very low temperature and therefore equilibrium is not established. The effects of lattice strain on the spectroscopy and photoluminescence quantum yields of zincblende CdSe/CdS core/shell quantum dots are examined. The quantum yields are measured as a function of core size and shell thickness. High quantum yields are achieved as long as the lattice strain energy density is below ~0.85 eV/nm2, which is considerably greater than the limiting value of 0.59 eV/nm2 for thermodynamicstability of a smooth, defect free shell, as previously reported in chapter 5. Thus, core/shell quantum dots having strain energy densities between 0.59 and 0.85 eV/nm2 can have very high PL QYs, but are metastable with respect to surface defect formation. Such metastable core/shell QDs can be produced by shell deposition at comparatively low temperatures (< 140 °C). Annealing of these particles causes partial loss of core pressure, and a red shift of the spectrum.

Phase equilibria in the quasi-ternary system Ag{sub 2}Se–Ga{sub 2}Se{sub 3}–In{sub 2}Se{sub 3} and physical properties of (Ga{sub 0.6}In{sub 0.4}){sub 2}Se{sub 3}, (Ga{sub 0.594}In{sub 0.396}Er{sub 0.01}){sub 2}Se{sub 3} single crystals

DOE Office of Scientific and Technical Information (OSTI.GOV)

Ivashchenko, I.A., E-mail: inna.ivashchenko@mail.ru; Danyliuk, I.V.; Olekseyuk, I.D.

2014-02-15

The quasi-ternary system Ag{sub 2}Se–Ga{sub 2}Se{sub 3}–In{sub 2}Se{sub 3} was investigated by differential thermal, X-ray phase, X-ray structure, microstructure analysis and microhardness measurements. Five quasi-binary phase diagrams, six polythermal sections, isothermal section at 820 K and the liquidus surface projection were constructed. The character and temperature of the invariant processes were determined. The specific resistance of the single crystals (Ga{sub 0.6}In{sub 0.4}){sub 2}Se{sub 3}, (Ga{sub 0.594}In{sub 0.396}Er{sub 0.01}){sub 2}Se{sub 3} was measured, 7.5×10{sup 5} and 3.15×10{sup 5} Ω m, respectively, optical absorption spectra in the 600–1050 nm range were recorded at room temperature, and the band gap energy was estimatedmore » which is 1.95±0. 01 eV for both samples. - Graphical abstract: The article reports for the first time the investigated liquidus surface projection of the Ag{sub 2}Se–Ga{sub 2}Se{sub 3}–In{sub 2}Se{sub 3} system and isothermal section at 820 K of the system. Five phase diagrams, six polythermal sections, isothermal section at 820 K and the liquidus surface projection were built at the first time. The existence of the large region of the solid solutions based on AgIn{sub 5}Se{sub 8}, Ga{sub 2}Se{sub 3} and AgGa{sub 1−x}In{sub x}Se{sub 2} was investigated. The existence of two ternary phases was established in the Ga{sub 2}Se{sub 3}–In{sub 2}Se{sub 3} system. Two single crystals (Ga{sub 0.6}In{sub 0.4}){sub 2}Se{sub 3}, (Ga{sub 0.594}In{sub 0.396}Er{sub 0.01}){sub 2}Se{sub 3} were grown and some of optical properties of them were studied at first time. Display Omitted - Highlights: • Liquidus surface projection was built for Ag{sub 2}Se–Ga{sub 2}Se{sub 3}–In{sub 2}Se{sub 3} system. • Solid solution ranges of AgIn{sub 5}Se{sub 8}, Ga{sub 2}Se{sub 3} and AgGa{sub 1−x}In{sub x}Se{sub 2} were investigated. • Two single crystals (Ga{sub 0.6}In{sub 0.4}){sub 2}Se{sub 3}, (Ga{sub 0.594}In{sub 0.396}Er{sub 0.01}){sub 2}Se{sub 3} were grown. • Some optical properties of these single crystals were studied.« less

Electronic structures of Plutonium compounds with the NaCl-type monochalcogenides structure

NASA Astrophysics Data System (ADS)

Maehira, Takahiro; Tatetsu, Yasutomi

2012-12-01

We calculate the energy band structure and the Fermi surface of PuS, PuSe and PuTe by using a self-consistent relativistic linear augmented-plane-wave method with the exchange and correlation potential in a local density approximation. It is found in common that the energy bands in the vicinity of the Fermi level are mainly due to the hybridization between Pu 5/ and monochalcogenide p electrons. The obtained main Fermi surfaces are composed of two hole sheets and one electron sheet, all of which are constructed from the band having the Pu 5/ state and the monochalcogenide p state.

Stable topological insulators achieved using high energy electron beams

PubMed Central

Zhao, Lukas; Konczykowski, Marcin; Deng, Haiming; Korzhovska, Inna; Begliarbekov, Milan; Chen, Zhiyi; Papalazarou, Evangelos; Marsi, Marino; Perfetti, Luca; Hruban, Andrzej; Wołoś, Agnieszka; Krusin-Elbaum, Lia

2016-01-01

Topological insulators are potentially transformative quantum solids with metallic surface states which have Dirac band structure and are immune to disorder. Ubiquitous charged bulk defects, however, pull the Fermi energy into the bulk bands, denying access to surface charge transport. Here we demonstrate that irradiation with swift (∼2.5 MeV energy) electron beams allows to compensate these defects, bring the Fermi level back into the bulk gap and reach the charge neutrality point (CNP). Controlling the beam fluence, we tune bulk conductivity from p- (hole-like) to n-type (electron-like), crossing the Dirac point and back, while preserving the Dirac energy dispersion. The CNP conductance has a two-dimensional character on the order of ten conductance quanta and reveals, both in Bi2Te3 and Bi2Se3, the presence of only two quantum channels corresponding to two topological surfaces. The intrinsic quantum transport of the topological states is accessible disregarding the bulk size. PMID:26961901

Double heterojunction nanowire photocatalysts for hydrogen generation.

PubMed

Tongying, P; Vietmeyer, F; Aleksiuk, D; Ferraudi, G J; Krylova, G; Kuno, M

2014-04-21

Charge separation and charge transfer across interfaces are key aspects in the design of efficient photocatalysts for solar energy conversion. In this study, we investigate the hydrogen generating capabilities and underlying photophysics of nanostructured photocatalysts based on CdSe nanowires (NWs). Systems studied include CdSe, CdSe/CdS core/shell nanowires and their Pt nanoparticle-decorated counterparts. Femtosecond transient differential absorption measurements reveal how semiconductor/semiconductor and metal/semiconductor heterojunctions affect the charge separation and hydrogen generation efficiencies of these hybrid photocatalysts. In turn, we unravel the role of surface passivation, charge separation at semiconductor interfaces and charge transfer to metal co-catalysts in determining photocatalytic H2 generation efficiencies. This allows us to rationalize why Pt nanoparticle decorated CdSe/CdS NWs, a double heterojunction system, performs best with H2 generation rates of ∼434.29 ± 27.40 μmol h(-1) g(-1) under UV/Visible irradiation. In particular, we conclude that the CdS shell of this double heterojunction system serves two purposes. The first is to passivate CdSe NW surface defects, leading to long-lived charges at the CdSe/CdS interface capable of carrying out reduction chemistries. Upon photoexcitation, we also find that CdS selectively injects charges into Pt NPs, enabling simultaneous reduction chemistries at the Pt NP/solvent interface. Pt nanoparticle decorated CdSe/CdS NWs thus enable reduction chemistries at not one, but rather two interfaces, taking advantage of each junction's optimal catalytic activities.

Structural and optoelectronic properties of ZnGaO thin film by pulsed laser deposition

NASA Astrophysics Data System (ADS)

Han, Xiaowei; Wang, Li; Li, Shufeng; Gao, Dongwen; Pan, Yong

2018-01-01

ZnO has attracted much attention because of its high-energy gap and exciton binding energy at room temperature. Compared to ZnO thin films, ZnGaO thin films are more resistive to oxidation and have smaller deformation of lattice. In this study, the high purity ZnSe and Ga2O3 powders were weighted at a molar ratio of 18:1. Se was oxidized to Se2O3 and separated from the mixture powders by using conventional solid state reaction method in air, and the ZnGaO ceramic target was prepared. We fabricated the ZnGaO films on silica glass by pulsed laser deposition (PLD) method under different oxygen pressure at room temperature. The as-grown films were tested by X-ray diffraction and atomic force microscope (AFM) to diagnose the crystal structure and surface morphology. Moreover, we obtained the optical transmittance of ZnGaO film and found that the electrical conductivity capacity varied with the increase of oxygen pressure.

Photo- and thermally induced property change in Ag diffusion into Ag/As2Se3 thin films

NASA Astrophysics Data System (ADS)

Aparimita, Adyasha; Sripan, C.; Ganesan, R.; Naik, Ramakanta

2018-03-01

In the present report, we have prepared As2Se3 and bilayer Ag/As2Se3 chalcogenide thin films prepared by thermal evaporation process. The top Ag layer is being diffused into the bottom As2Se3 layer by 532 nm laser irradiation and thermal annealing process. The photo and thermal energy drives the Ag+ ions into the As2Se3 matrix that enhances the formation of As-Se-Ag solid solution which shows the changes of optical properties such as transmission, absorption power, refractive index, and optical band gap. The transmission power drastically decreased for the thermal-induced film than the laser induced one; and the reverse effect is seen for the absorption coefficient. The non-linear refractive index is found to be increased due to the Ag diffusion into As2Se3 film. The indirect allowed optical band gap is being reduced by a significant amount of 0.17 eV (thermal diffusion) and 0.03 eV (photo diffusion) from the Ag/As2Se3 film. The Ag diffusion creates chemical disorderness in the film observed from the two parameters which measures the degree of disorder such as Urbach energy and Tauc parameter. The structural change is not noticed in the studied film as seen from the X-ray diffraction pattern. Scanning electron microscopy and atomic force microscopy investigations showed that the surface morphology was influenced by the diffusion phenomena. The change in optical constants in such type of film can be used in optical waveguides and optical devices.

Direct comparison of current-induced spin polarization in topological insulator Bi2Se3 and InAs Rashba states

DOE PAGES

Li, C. H.; van ‘t Erve, O. M. J.; Rajput, S.; ...

2016-11-17

Three-dimensional topological insulators (TIs) exhibit time-reversal symmetry protected, linearly dispersing Dirac surface states with spin–momentum locking. Band bending at the TI surface may also lead to coexisting trivial two-dimensional electron gas (2DEG) states with parabolic energy dispersion. A bias current is expected to generate spin polarization in both systems, although with different magnitude and sign. Here we compare spin potentiometric measurements of bias current-generated spin polarization in Bi2Se3(111) where Dirac surface states coexist with trivial 2DEG states, and in InAs(001) where only trivial 2DEG states are present. We observe spin polarization arising from spin–momentum locking in both cases, with oppositemore » signs of the measured spin voltage. We present a model based on spin dependent electrochemical potentials to directly derive the sign expected for the Dirac surface states, and show that the dominant contribution to the current-generated spin polarization in the TI is from the Dirac surface states.« less

Electronic transport in bismuth selenide in the topological insulator regime

NASA Astrophysics Data System (ADS)

Kim, Dohun

The 3D topological insulators (TIs) have an insulating bulk but spin-momentum coupled metallic surface states stemming from band inversion due to strong spin-orbit interaction, whose existence is guaranteed by the topology of the band structure of the insulator. While the STI surface state has been studied spectroscopically by e.g. photoemission and scanned probes, transport experiments have failed to demonstrate clear signature of the STI due to high level of bulk conduction. In this thesis, I present experimental results on the transport properties of TI material Bi2Se3 in the absence of bulk conduction (TI regime), achieved by applying novel p-type doping methods. Field effect transistors consisting of thin (thickness: 5-17 nm) Bi2Se3 are fabricated by mechanical exfoliation of single crystals, and a combination of conventional dielectric (300 nm thick SiO2) and electrochemical or chemical gating methods are used to move the Fermi energy through the surface Dirac point inside bulk band gap, revealing the ambipolar gapless nature of transport in the Bi2Se3 surface states. The minimum conductivity of the topological surface state is understood within the self-consistent theory of Dirac electrons in the presence of charged impurities. The intrinsic finite-temperature resistivity of the topological surface state due to electron-acoustic phonon scattering is measured to be 60 times larger than that of graphene largely due to the smaller Fermi and sound velocities in Bi2Se 3, which will have implications for topological electronic devices operating at room temperature. Along with semi-classical Boltzmann transport, I also discuss 2D weak anti-localization (WAL) behavior of the topological surface states. By investigating gate-tuned WAL behavior in thin (5-17 nm) TI films, I show that WAL in the TI regime is extraordinarily sensitive to the hybridization induced quantum mechanical tunneling between top and bottom topological surfaces, and interplay of phase coherence time and inter-surface tunneling time results in a crossover from two decoupled (top and bottom) symplectic 2D metal surfaces to a coherently coupled single channel. Furthermore, a complete suppression of WAL is observed in the 5 nm thick Bi2Se 3 film which was found to occur when the hybridization gap becomes comparable to the disorder strength.

Spectroscopic and Structural Studies of a Surface Active Porphyrin in Solution and in Langmuir-Blodgett Films.

PubMed

Ponce, Concepcion P; Araghi, Hessamaddin Younesi; Joshi, Neeraj K; Steer, Ronald P; Paige, Matthew F

2015-12-22

Controlling aggregation of the dual sensitizer-emitter (S-E) zinc tetraphenylporphyrin (ZnTPP) is an important consideration in solid state noncoherent photon upconversion (NCPU) applications. The Langmuir-Blodgett (LB) technique is a facile means of preparing ordered assemblies in thin films to study distance-dependent energy transfer processes in S-E systems and was used in this report to control the aggregation of a functionalized ZnTPP on solid substrates. This was achieved by synthetic addition of a short polar tail to one of the pendant phenyl rings in ZnTPP in order to make it surface active. The surface active ZnTPP derivative formed rigid films at the air-water interface and exhibited mean molecular areas consistent with approximately vertically oriented molecules under appropriate film compression. A red shift in the UV-vis spectra as well as unquenched fluorescence emission of the LB films indicated formation of well-ordered aggregates. However, NCPU, present in the solution phase, was not observed in the LB films, suggesting that NCPU from ZnTPP as a dual S-E required not just a controlled aggregation but a specific orientation of the molecules with respect to each other.

Back surface studies of Cu(In,Ga)Se2 thin film solar cells

NASA Astrophysics Data System (ADS)

Simchi, Hamed

Cu(In,Ga)Se2 thin film solar cells have attracted a lot of interest because they have shown the highest achieved efficiency (21%) among thin film photovoltaic materials, long-term stability, and straightforward optical bandgap engineering by changing relative amounts of present elements in the alloy. Still, there are several opportunities to further improve the performance of the Cu(In,Ga)Se2 devices. The interfaces between layers significantly affect the device performance, and knowledge of their chemical and electronic structures is essential in identifying performance limiting factors. The main goal of this research is to understand the characteristics of the Cu(In,Ga)Se2-back contact interface in order to design ohmic back contacts for Cu(In,Ga)Se2-based solar cells with a range of band gaps and device configurations. The focus is on developing either an opaque or transparent ohmic back contact via surface modification or introduction of buffer layers in the back surface. In this project, candidate back contact materials have been identified based on modeling of band alignments and surface chemical properties of the absorber layer and back contact. For the first time, MoO3 and WO 3 transparent back contacts were successfully developed for Cu(In,Ga)Se 2 solar cells. The structural, optical, and surface properties of MoO 3 and WO3 were optimized by controlling the oxygen partial pressure during reactive sputtering and post-deposition annealing. Valence band edge energies were also obtained by analysis of the XPS spectra and used to characterize the interface band offsets. As a result, it became possible to illuminate of the device from the back, resulting in a recently developed "backwall superstrate" device structure that outperforms conventional substrate Cu(In,Ga)Se2 devices in the absorber thickness range 0.1-0.5 microm. Further enhancements were achieved by introducing moderate amounts of Ag into the Cu(In,Ga)Se2 lattice during the co-evaporation method resulting in a 9.7% cell (with 0.3 microm thickness) which has the highest efficiency reported for ultrathin CIGS solar cells to date. In addition, sulfized back contacts including ITO-S and MoS 2 are compared. Interface properties of different contact layers with (Ag,Cu)(In,Ga)Se2 absorber layers with various Ga/(Ga+In) and Ag/(Ag+Cu) ratios are discussed based on the XPS analysis and thermodynamics of reactions.

Theoretical aspects of graphene-like group IV semiconductors

NASA Astrophysics Data System (ADS)

Houssa, M.; van den Broek, B.; Scalise, E.; Ealet, B.; Pourtois, G.; Chiappe, D.; Cinquanta, E.; Grazianetti, C.; Fanciulli, M.; Molle, A.; Afanas'ev, V. V.; Stesmans, A.

2014-02-01

Silicene and germanene are the silicon and germanium counterparts of graphene, respectively. Recent experimental works have reported the growth of silicene on (1 1 1)Ag surfaces with different atomic configurations, depending on the growth temperature and surface coverage. We first theoretically study the structural and electronic properties of silicene on (1 1 1)Ag surfaces, focusing on the (4 × 4)silicene/Ag structure. Due to symmetry breaking in the silicene layer (nonequivalent number of top and bottom Si atoms), the corrugated silicene layer, with the Ag substrate removed, is predicted to be semiconducting, with a computed energy bandgap of about 0.3 eV. However, the hybridization between the Si 3p orbitals and the Ag 5s orbital in the silicene/(1 1 1)Ag slab model leads to an overall metallic system, with a distribution of local electronic density of states, which is related to the slightly disordered structure of the silicene layer on the (1 1 1)Ag surface. We next study the interaction of silicene and germanene with different hexagonal non-metallic substrates, namely ZnS and ZnSe. On reconstructed (0 0 0 1)ZnS or ZnSe surfaces, which should be more energetically stable for very thin layers, silicene and germanene are found to be semiconducting. Remarkably, the nature and magnitude of their energy bandgap can be controlled by an out-of-plane electric field, an important finding for the potential use of these materials in nanoelectronic devices.

Selenium speciation and partitioning within Burkholderia cepacia biofilms formed on α-Al 2O 3 surfaces

NASA Astrophysics Data System (ADS)

Templeton, Alexis S.; Trainor, Thomas P.; Spormann, Alfred M.; Brown, Gordon E.

2003-10-01

The distribution and speciation of Se within aerobic Burkholderia cepacia biofilms formed on α-Al 2O 3 (1-102) surfaces have been examined using grazing-angle X-ray spectroscopic techniques. We present quantitative information on the partitioning of 10 -6 M to 10 -3 M selenate and selenite between the biofilms and underlying alumina surfaces derived from long-period X-ray standing wave (XSW) data. Changes in the Se partitioning behavior over time are correlated with microbially induced reduction of Se(VI) and Se(IV) to Se(0), as observed from X-ray absorption near edge structure (XANES) spectroscopy. Selenite preferentially binds to the alumina surfaces, particularly at low [Se], and is increasingly partitioned into the biofilms at higher [Se]. When B. cepacia is metabolically active, B. cepacia rapidly reduces a fraction of the SeO 32- to red elemental Se(0). In contrast, selenate is preferentially partitioned into the B. cepacia biofilms at all [Se] tested due to a lower affinity for binding to the alumina surface. Rapid reduction of SeO 42- by B. cepacia to Se(IV) and Se(0) subsequently results in a vertical segregation of Se species at the B. cepacia/α-Al 2O 3 interface. Elemental Se(0) accumulates within the biofilm with Se(VI), whereas Se(IV) intermediates preferentially sorb to the alumina surface. B. cepacia/α-Al 2O 3 samples incubated with SeO 42- and SeO 32- when the bacteria were metabolically active result in a significant reduction in the mobility of Se vs. X-ray treated biofilms. Remobilization experiments show that a large fraction of the insoluble Se(0) produced within the biofilm is retained during exchange with Se-free solutions. In addition, Se(IV) intermediates generated during Se(VI) reduction are preferentially bound to the alumina surface and do not fully desorb. In contrast, Se(VI) is rapidly and extensively remobilized.

Surface states in the photoionization of high-quality CdSe core/shell nanocrystals.

PubMed

Li, Shu; Steigerwald, Michael L; Brus, Louis E

2009-05-26

We use electric force microscopy (EFM) to study single nanocrystal photoionization in two classes of high-quality nanocrystals whose exciton luminescence quantum yields approach unity in solution. The CdSe/CdS/ZnS core/shell nanocrystals do not photoionize, while the CdSe/CdS nanocrystals do show substantial photoionization. This verifies the theoretical prediction that the ZnS shell confines the excited electron within the nanocrystal. Despite the high luminescence quantum yield, photoionization varies substantially among the CdSe/CdS nanocrystals. We have studied the nanocrystal photoionization with both UV (396 nm) and green (532 nm) light, and we have found that the magnitude of the charge due to photoionization per absorbed photon is greater for UV excitation than for green excitation. A fraction of the photoionization occurs directly via a "hot electron" process, using trap states that are either on the particle surface, within the ligand sphere, or within the silicon oxide layer. This must occur without relaxation to the thermalized, lowest-energy, emitting exciton. We discuss the occurrence of hot carrier processes that are common to photoionization, luminescence blinking, and the fast transient optical absorption that is associated with multiple exciton generation MEG studies.

Rare earth substitution on structural and optical behaviour of CdSe thin films

NASA Astrophysics Data System (ADS)

Singh, Sarika; Shrivastava, A. K.; Tapdiya, Swati

2018-05-01

A series of Sm2+,Gd2+ doped with Cadmium selenide CdSe (x =0.01) has been prepared by using Chemical bath deposition technique. Structural, Optical and Morphological studies were performed using X-ray diffraction (XRD), UV-Visible spectrometer, Raman Studies and Scanning Electron Microscopy (SEM). XRD patterns confirm the samples with Sm,Gd ions, some diffraction peaks appeared which belongs to the cubic phase structure. The values of lattice parameter (a) decreased and particle size decrease on doping. Morphology of the grown films reveals that surface are homogeneous and uniformly spread on the substrates. The elemental analysis of CdSe doped Sm and Gd (1%) different composition was analyzed by Energy Dispersive X-Rays (EDX). The optical values of some important parameters of the studied films were calculated by UVstudy are determined from transmission spectra at wavelength 200 to 900nm. Optical band gap Eg was calculated by tauc relation. Energy band gap of CdSe doped with Sm and Gd varies at 1.8eV and 1.9eV respectively. Bandgap In Raman analysis, a prominent peak shows that confirmation of nano crystalline phase. And intensity of peaks was decreasing after doping.

Topological Insulators in Ternary Compounds with a Honeycomb Lattice

NASA Astrophysics Data System (ADS)

Zhang, Hai-Jun; Chadov, Stanislav; Muchler, Lukas; Yan, Binghai; Qi, Xiao-Liang; Kübler, Jürgen; Zhang, Shou-Cheng; Felser, Claudia

2011-03-01

One of the most exciting subjects in solid state physics is a single layer of graphite which exhibits a variety of unconventional novel properties. The key feature of its electronic structure are linear dispersive bands which cross in a single point at the Fermi energy. This is so-called Dirac cone. The ternary compounds, such as LiAuSe and KHgSb with a honeycomb structure of their Au-Se and Hg-Sb layers feature band inversion very similar to HgTe which is a strong precondition for existence of the topological surface states. These materials exhibit the surface states formed by only a single Dirac cone at the G point together with the small direct band gap opened by a strong spin-orbit coupling (SOC) in the bulk. These materials are centro-symmetric, therefore, it is possible to determine the parity of their wave functions, and hence, their topological character. The work was supported by the supercomputing center at Stanford Institute Materials and Energy Science. The financial support of the DFG/ASPIMATT project (unit 1.2-A) is gratefully acknowledged.

Directional charge transfer mediated by mid-gap states: A transient absorption spectroscopy study of CdSe quantum dot/β-Pb 0.33V 2O 5 heterostructures

DOE PAGES

Milleville, Christopher C.; Pelcher, Kate E.; Sfeir, Matthew Y.; ...

2016-02-15

For solar energy conversion, not only must a semiconductor absorb incident solar radiation efficiently but also its photoexcited electron—hole pairs must further be separated and transported across interfaces. Charge transfer across interfaces requires consideration of both thermodynamic driving forces as well as the competing kinetics of multiple possible transfer, cooling, and recombination pathways. In this work, we demonstrate a novel strategy for extracting holes from photoexcited CdSe quantum dots (QDs) based on interfacing with β-Pb 0.33V 2O 5 nanowires that have strategically positioned midgap states derived from the intercalating Pb 2+ ions. Unlike midgap states derived from defects or dopants,more » the states utilized here are derived from the intrinsic crystal structure and are thus homogeneously distributed across the material. CdSe/β-Pb 0.33V 2O 5 heterostructures were assembled using two distinct methods: successive ionic layer adsorption and reaction (SILAR) and linker-assisted assembly (LAA). Transient absorption spectroscopy measurements indicate that, for both types of heterostructures, photoexcitation of CdSe QDs was followed by the transfer of electrons to the conduction band of β-Pb 0.33V 2O 5 nanowires and holes to the midgap states of β-Pb 0.33V 2O 5 nanowires. Holes were transferred on time scales less than 1 ps, whereas electrons were transferred more slowly on time scales of ~2 ps. In contrast, for analogous heterostructures consisting of CdSe QDs interfaced with V 2O 5 nanowires (wherein midgap states are absent), only electron transfer was observed. Interestingly, electron transfer was readily achieved for CdSe QDs interfaced with V 2O 5 nanowires by the SILAR method; however, for interfaces incorporating molecular linkers, electron transfer was observed only upon excitation at energies substantially greater than the bandgap absorption threshold of CdSe. Furthermore, transient absorbance decay traces reveal longer excited-state lifetimes (1–3 μs) for CdSe/β-Pb 0.33V 2O 5 heterostructures relative to bare β-Pb 0.33V 2O 5 nanowires (0.2 to 0.6 μs); the difference is attributed to surface passivation of intrinsic surface defects in β-Pb 0.33V 2O 5 upon interfacing with CdSe.« less

DOE Office of Scientific and Technical Information (OSTI.GOV)

Kroupa, Daniel M.; Hughes, Barbara K.; Miller, Elisa M.

Electronic impurity doping of bulk semiconductors is an essential component of semiconductor science and technology. Yet there are only a handful of studies demonstrating control of electronic impurities in semiconductor nanocrystals. Here, we studied electronic impurity doping of colloidal PbSe quantum dots (QDs) using a postsynthetic cation exchange reaction in which Pb is exchanged for Ag. We found that varying the concentration of dopants exposed to the as-synthesized PbSe QDs controls the extent of exchange. The electronic impurity doped QDs exhibit the fundamental spectroscopic signatures associated with injecting a free charge carrier into a QD under equilibrium conditions, including amore » bleach of the first exciton transition and the appearance of a quantum-confined, low-energy intraband absorption feature. Photoelectron spectroscopy confirms that Ag acts as a p-type dopant for PbSe QDs and infrared spectroscopy is consistent with k • p calculations of the size-dependent intraband transition energy. We find that to bleach the first exciton transition by an average of 1 carrier per QD requires that approximately 10% of the Pb be replaced by Ag. Here, we hypothesize that the majority of incorporated Ag remains at the QD surface and does not interact with the core electronic states of the QD. Instead, the excess Ag at the surface promotes the incorporation of <1% Ag into the QD core where it causes p-type doping behavior.« less

Large Exciton Energy Shifts by Reversible Surface Exchange in 2D II-VI Nanocrystals.

PubMed

Zhou, Yang; Wang, Fudong; Buhro, William E

2015-12-09

Reaction of n-octylamine-passivated {CdSe[n-octylamine](0.53±0.06)} quantum belts with anhydrous metal carboxylates M(oleate)2 (M = Cd, Zn) results in a rapid exchange of the L-type amine passivation for Z-type M(oleate)2 passivation. The cadmium-carboxylate derivative is determined to have the composition {CdSe[Cd(oleate)2](0.19±0.02)}. The morphologies and crystal structures of the quantum belts are largely unaffected by the exchange processes. Addition of n-octylamine or oleylamine to the M(oleate)2-passivated quantum belts removes M(oleate)2 and restores the L-type amine passivation. Analogous, reversible surface exchanges are also demonstrated for CdS quantum platelets. The absorption and emission spectra of the quantum belts and platelets are reversibly shifted to lower energy by M(oleate)2 passivation vs amine passivation. The largest shift of 140 meV is observed for the Cd(oleate)2-passivated CdSe quantum belts. These shifts are attributed entirely to changes in the strain states in the Zn(oleate)2-passivated nanocrystals, whereas changes in strain states and confinement dimensions contribute roughly equally to the shifts in the Cd(oleate)2-passivated nanocrystals. Addition of Cd(oleate)2, which electronically couples to the nanocrystal lattices, increases the effective thickness of the belts and platelets by approximately a half of a monolayer, thus increasing the confinement dimension.

Band alignment measurements at heterojunction interfaces in layered thin film solar cells & thermoelectrics

NASA Astrophysics Data System (ADS)

Fang, Fang

2011-12-01

Public awareness of the increasing energy crisis and the related serious environmental concerns has led to a significantly growing demand for alternative clean and renewable energy resources. Thin film are widely applied in multiple renewable energy devices owing to the reduced amount of raw materials and increase flexibility of choosing from low-cost candidates, which translates directly into reduced capital cost. This is a key driving force to make renewable technology competitive in the energy market. This thesis is focused on the measurement of energy level alignments at interfaces of thin film structures for renewable energy applications. There are two primary foci: II -VI semiconductor ZnSe/ZnTe thin film solar cells and Bi2Te3/Sb2Te3 thin film structures for thermoelectric applications. In both cases, the electronic structure and energy band alignment at interfaces usually controls the carrier transport behavior and determines the quality of the device. High-resolution photoemission spectroscopy (lab-based XPS & synchrotron-based UPS) was used to investigate the chemical and electronic properties of epitaxial Bi2Te3 and Sb2Te3 thin films, in order to validate the anticipated band alignment at interfaces in Bi 2Te3/Sb2Te3 superlattices as one favoring electron-transmission. A simple, thorough two-step treatment of a chemical etching in dilute hydrochloric acid solution and a subsequent annealing at ˜150°C under ultra-high vacuum environment is established to remove the surface oxides completely. It is an essential step to ensure the measurements on electronic states are acquired on stoichimetric, oxide-free clean surface of Bi 2Te3 and Sb2Te3 films. The direct measurement of valence band offsets (VBO) at a real Sb 2Te3/Bi2Te3 interface is designed based on the Kraut model; a special stacking film structure is prepared intentionally: sufficiently thin Sb2Te3 film on top of Bi2Te 3 that photoelectrons from both of them are collected simultaneously. From a combination of core levels and valence band ultraviolet photoemission spectra of the bulk materials as well as the heterojunction (Sb2Te 3/Bi2Te3), the VBO at p-type Sb2Te 3 and n-type Bi2Te3 is determined as 0.04 +/- 0.10 eV. Such a small energy offset is within the same magnitude of the thermal energy of kT, at room temperature. The motivation for the II-VI ZnTe-based thin film solar cell derives from the need to identify and overcome performance-limiting properties related to the processing of film deposition using close space sublimation (CSS). Chemical and electronic properties of the CSS grown ZnTe/ZnSe films were studied in x-ray diffraction, scanning electron microscopy and photoemission spectroscopy. Specifically, Se oxide was observed on the ZnSe surface, the removal of this oxide generated apparent offsets in the valence band and hence the alignment at the heterojunction energy diagram. Processing steps to mitigate oxidation yielded the best cells. Film structure was studied on the dependence of growth time; physical film damage is found during the initial stages when depositing ZnTe on a grown ZnSe film. Preliminary studies of films grown by evaporation and their characterizations are presented at last. In this thesis, a better understanding of the electronic structure at interfaces is built in two different thin film devices, and the resulting band energy diagram of the corresponding devices offered effective feedback in materials and device.The problem of energy equilibrium in the human body has received a great deal.

Evolving optical second-harmonic anisotropy at the cleaved Bi2Se3 surface

NASA Astrophysics Data System (ADS)

An, Yong; Green, Avery; Diebold, Alain

Bismuth selenide (Bi2Se3) is a centrosymmetric topological insulator with conducting surface states. The surface states have been studied by various electrical and optical techniques in air, but ambience effects and surface aging have not been adequately addressed. Optical second-harmonic generation (SHG) is a suitable probe for the Bi2Se3 surface because SHG arises from symmetry breaking at the surface and thus should detect surface states preferentially over bulk states. However, a strong time dependence of SHG is often observed, hampering the detection and investigation of the surface states. Here we find a new phenomenon in which the major and minor intensity lobes of a measured rotational-anisotropy SHG pattern from a cleaved Bi2Se3 (111) surface can significantly change with time and eventually switch their amplitudes. This switching provides a means for tracking the progress of surface oxidation inside a quintuple layer of Bi2Se3. We also perform pump-probe SHG experiments, comparatively on freshly cleaved and oxidized Bi2Se3 surfaces, to study charge dynamics at the oxide/Bi2Se3 interface and to detect spin polarization of photoexcited surface states in the Bi2Se3 topological insulator. This work was supported by the SRC NRI Institute for Nanoelectronics Discovery and Exploration (INDEX).

The effect of defect emissions on enhancement photocatalytic performance of ZnSe QDs and ZnSe/rGO nanocomposites

NASA Astrophysics Data System (ADS)

Yousefi, Ramin; Azimi, H. R.; Mahmoudian, M. R.; Basirun, Wan Jeffrey

2018-03-01

A systematic study about the origin of defects emission of ZnSe structure was conducted by photoluminescence (PL) spectrometer at room temperature. It was observed that different intermediate energy levels in band-gap space of ZnSe structure were generated by different defects such as Se-, Zn-vacancies, Se-, Zn-interstitials, and surface states. Effects of these defects on the photocatalytic performance of ZnSe quantum dots (QDs) and ZnSe/graphene nanocomposites were investigated. The pristine ZnSe QDs and ZnSe/graphene nanocomposites were synthesized by a co-precipitation method. The PL spectra of the samples showed four emissions from four regions of the visible spectrum such as violet, green, orange, and red emissions. The violet emission was associated with the near-band-edge (NBE) of the ZnSe nanostructures, while, the other emissions were related to different defects of ZnSe structures. Annealing the samples in the H2 atmosphere caused to increase orange emission intensity and indicated that origin of orange emission was a donor-acceptor pair (DAPs) related to singly positively charged Se-vacancies (VSe) to singly negatively charged zinc vacancy (VZn-). Photocatalytic study of the samples to remove the methylene blue (MB) dye showed that the photocatalytic performance of the samples improved by graphene as an additive and increasing the orange emission intensity.

Performance evaluation of multi-material electronic cleansing for ultra-low-dose dual-energy CT colonography

NASA Astrophysics Data System (ADS)

Tachibana, Rie; Kohlhase, Naja; Näppi, Janne J.; Hironaka, Toru; Ota, Junko; Ishida, Takayuki; Regge, Daniele; Yoshida, Hiroyuki

2016-03-01

Accurate electronic cleansing (EC) for CT colonography (CTC) enables the visualization of the entire colonic surface without residual materials. In this study, we evaluated the accuracy of a novel multi-material electronic cleansing (MUMA-EC) scheme for non-cathartic ultra-low-dose dual-energy CTC (DE-CTC). The MUMA-EC performs a wateriodine material decomposition of the DE-CTC images and calculates virtual monochromatic images at multiple energies, after which a random forest classifier is used to label the images into the regions of lumen air, soft tissue, fecal tagging, and two types of partial-volume boundaries based on image-based features. After the labeling, materials other than soft tissue are subtracted from the CTC images. For pilot evaluation, 384 volumes of interest (VOIs), which represented sources of subtraction artifacts observed in current EC schemes, were sampled from 32 ultra-low-dose DE-CTC scans. The voxels in the VOIs were labeled manually to serve as a reference standard. The metric for EC accuracy was the mean overlap ratio between the labels of the reference standard and the labels generated by the MUMA-EC, a dualenergy EC (DE-EC), and a single-energy EC (SE-EC) scheme. Statistically significant differences were observed between the performance of the MUMA/DE-EC and the SE-EC methods (p<0.001). Visual assessment confirmed that the MUMA-EC generated less subtraction artifacts than did DE-EC and SE-EC. Our MUMA-EC scheme yielded superior performance over conventional SE-EC scheme in identifying and minimizing subtraction artifacts on noncathartic ultra-low-dose DE-CTC images.

Oxidation and mobilization of selenium by nitrate in irrigation drainage

USGS Publications Warehouse

Wright, W.G.

1999-01-01

Selenium (Se) can be oxidized by nitrate (NO3-) from irrigation on Cretaceous marine shale in western Colorado. Dissolved Se concentrations are positively correlated with dissolved NO3- concentrations in surface water and ground water samples from irrigated areas. Redox conditions dominate in the mobilization of Se in marine shale hydrogeologic settings; dissolved Se concentrations increase with increasing platinum-electrode potentials. Theoretical calculations for the oxidation of Se by NO3- and oxygen show favorable Gibbs free energies for the oxidation of Se by NO3-, indicating NO3- can act as an electron acceptor for the oxidation of Se. Laboratory batch experiments were performed by adding Mancos Shale samples to zero- dissolved-oxygen water containing 0, 5, 50, and 100 mg/L NO3- as N (mg N/L). Samples were incubated in airtight bottles at 25??C for 188 d; samples collected from the batch experiment bottles show increased Se concentrations over time with increased NO3- concentrations. Pseudo first-order rate constants for NO3- oxidation of Se ranged from 0.0007 to 0.0048/d for 0 to 100 mg N/L NO3- concentrations, respectively. Management of N fertilizer applications in Cretaceous shale settings might help to control the oxidation and mobilization of Se and other trace constituents into the environment.

Double heterojunction nanowire photocatalysts for hydrogen generation

NASA Astrophysics Data System (ADS)

Tongying, P.; Vietmeyer, F.; Aleksiuk, D.; Ferraudi, G. J.; Krylova, G.; Kuno, M.

2014-03-01

Charge separation and charge transfer across interfaces are key aspects in the design of efficient photocatalysts for solar energy conversion. In this study, we investigate the hydrogen generating capabilities and underlying photophysics of nanostructured photocatalysts based on CdSe nanowires (NWs). Systems studied include CdSe, CdSe/CdS core/shell nanowires and their Pt nanoparticle-decorated counterparts. Femtosecond transient differential absorption measurements reveal how semiconductor/semiconductor and metal/semiconductor heterojunctions affect the charge separation and hydrogen generation efficiencies of these hybrid photocatalysts. In turn, we unravel the role of surface passivation, charge separation at semiconductor interfaces and charge transfer to metal co-catalysts in determining photocatalytic H2 generation efficiencies. This allows us to rationalize why Pt nanoparticle decorated CdSe/CdS NWs, a double heterojunction system, performs best with H2 generation rates of ~434.29 +/- 27.40 μmol h-1 g-1 under UV/Visible irradiation. In particular, we conclude that the CdS shell of this double heterojunction system serves two purposes. The first is to passivate CdSe NW surface defects, leading to long-lived charges at the CdSe/CdS interface capable of carrying out reduction chemistries. Upon photoexcitation, we also find that CdS selectively injects charges into Pt NPs, enabling simultaneous reduction chemistries at the Pt NP/solvent interface. Pt nanoparticle decorated CdSe/CdS NWs thus enable reduction chemistries at not one, but rather two interfaces, taking advantage of each junction's optimal catalytic activities.Charge separation and charge transfer across interfaces are key aspects in the design of efficient photocatalysts for solar energy conversion. In this study, we investigate the hydrogen generating capabilities and underlying photophysics of nanostructured photocatalysts based on CdSe nanowires (NWs). Systems studied include CdSe, CdSe/CdS core/shell nanowires and their Pt nanoparticle-decorated counterparts. Femtosecond transient differential absorption measurements reveal how semiconductor/semiconductor and metal/semiconductor heterojunctions affect the charge separation and hydrogen generation efficiencies of these hybrid photocatalysts. In turn, we unravel the role of surface passivation, charge separation at semiconductor interfaces and charge transfer to metal co-catalysts in determining photocatalytic H2 generation efficiencies. This allows us to rationalize why Pt nanoparticle decorated CdSe/CdS NWs, a double heterojunction system, performs best with H2 generation rates of ~434.29 +/- 27.40 μmol h-1 g-1 under UV/Visible irradiation. In particular, we conclude that the CdS shell of this double heterojunction system serves two purposes. The first is to passivate CdSe NW surface defects, leading to long-lived charges at the CdSe/CdS interface capable of carrying out reduction chemistries. Upon photoexcitation, we also find that CdS selectively injects charges into Pt NPs, enabling simultaneous reduction chemistries at the Pt NP/solvent interface. Pt nanoparticle decorated CdSe/CdS NWs thus enable reduction chemistries at not one, but rather two interfaces, taking advantage of each junction's optimal catalytic activities. Electronic supplementary information (ESI) available: Details of NW syntheses, processing and characterization. Additional TEM images of CdS, CdSe and CdSe/CdS core/shell NWs. NW concentration and cross section estimates. Details of the Pt NP decoration. Additional TEM images of Pt NP decorated CdS, CdSe and CdSe/CdS core/shell NWs. Size distribution of Pt NPs for CdSe/Pt NP and CdSe/CdS/Pt NP NWs. Xe arc lamp spectrum. Details of H2 generation experiments. Estimated photon absorption rate. Details of TDA measurements. TDA spectra and kinetics of CdS and CdS/Pt NP NWs. Plot illustrating CdSe NW band edge bleach kinetics. Comparison of CdSe band edge bleach kinetics in CdSe/CdS core/shell NWs when excited at λexc = 387 nm and λexc = 560 nm. Comparison of CdSe band edge bleach kinetics in CdSe/Pt NP NWs when excited at λexc = 387 nm and λexc = 560 nm. Bar graph showing H2 generation efficiencies of CdS and CdS/Pt NP NWs. Bleach kinetics of CdSe/CdS/Pt NP NWs at λexc = 387 nm and λexc = 560 nm. Comparison of CdS band edge bleach kinetics in CdS/Pt NP, and CdSe/CdS core/shell NWs when excited at λexc = 387 nm. See DOI: 10.1039/c4nr00298a

Tuning band alignment by CdS layers using a SILAR method to enhance TiO2/CdS/CdSe quantum-dot solar-cell performance.

PubMed

Zhang, Bingkai; Zheng, Jiaxin; Li, Xiaoning; Fang, Yanyan; Wang, Lin-Wang; Lin, Yuan; Pan, Feng

2016-04-28

We report tuning band alignment by optimized CdS layers using a SILAR method to achieve the recorded best performance with about 6% PCE in TiO2/CdS/CdSe QDSSCs. Combining experimental and theoretical studies, we find that a better lattices match between CdS and TiO2 assists the growth of CdSe, and the combined effect of charge transfer and surface dipole moment at the TiO2/CdS/CdSe interface shifts the energy levels of TiO2 upward and increases Voc of the solar cells. More importantly, the band gap of CdS buffer layers is sensitive to the distortion induced by lattice mismatch and numbers of CdS layers. For example, the barrier for charge transfer disappears when there are more than 4 layers of CdS, facilitating the charge injection from CdSe to TiO2.

Orbitally-driven giant phonon anharmonicity in SnSe

DOE PAGES

Li, Chen W.; Hong, Jiawang; May, Andrew F.; ...

2015-10-19

We understand that elementary excitations and their couplings in condensed matter systems is critical to develop better energy-conversion devices. In thermoelectric materials, the heat-to-electricity conversion efficiency is directly improved by suppressing the propagation of phonon quasiparticles responsible for macroscopic thermal transport. The material with the current record for thermoelectric conversion efficiency, SnSe, achieves an ultra-low thermal conductivity, but the mechanism enabling this strong phonon scattering remains largely unknown. Using inelastic neutron scattering measurements and first-principles simulations, we mapped the four-dimensional phonon dispersion surfaces of SnSe, and revealed the origin of ionic-potential anharmonicity responsible for the unique properties of SnSe. Wemore » show that the giant phonon scattering arises from an unstable electronic structure, with orbital interactions leading to a ferroelectric-like lattice instability. Our results provide a microscopic picture connecting electronic structure and phonon anharmonicity in SnSe, and offers precious insights on how electron-phonon and phononphonon interactions may lead to the realization of ultra-low thermal conductivity.« less

Orbitally driven giant phonon anharmonicity in SnSe

DOE Office of Scientific and Technical Information (OSTI.GOV)

Li, C. W.; Hong, J.; May, A. F.

Understanding elementary excitations and their couplings in condensed matter systems is critical for developing better energy-conversion devices. In thermoelectric materials, the heat-to-electricity conversion efficiency is directly improved by suppressing the propagation of phonon quasiparticles responsible for macroscopic thermal transport. The current record material for thermoelectric conversion efficiency, SnSe, has an ultralow thermal conductivity, but the mechanism behind the strong phonon scattering remains largely unknown. From inelastic neutron scattering measurements and first-principles simulations, we mapped the four-dimensional phonon dispersion surfaces of SnSe, and found the origin of the ionic-potential anharmonicity responsible for the unique properties of SnSe. We show that themore » giant phonon scattering arises from an unstable electronic structure, with orbital interactions leading to a ferroelectric-like lattice instability. The present results provide a microscopic picture connecting electronic structure and phonon anharmonicity in SnSe, and offers new insights on how electron–phonon and phonon–phonon interactions may lead to the realization of ultralow thermal conductivity.« less

Discovery of orbital-selective Cooper pairing in FeSe

DOE PAGES

Sprau, P. O.; Kostin, A.; Kreisel, A.; ...

2017-07-07

The superconductor iron selenide (FeSe) is of intense interest owing to its unusual nonmagnetic nematic state and potential for high-temperature superconductivity. But its Cooper pairing mechanism has not been determined. Here, we used Bogoliubov quasiparticle interference imaging to determine the Fermi surface geometry of the electronic bands surrounding the Γ = (0,0) and X = (π/a Fe, 0) points of FeSe and to measure the corresponding superconducting energy gaps. We show that both gaps are extremely anisotropic but nodeless and that they exhibit gap maxima oriented orthogonally in momentum space. Moreover, by implementing a novel technique, we demonstrate that thesemore » gaps have opposite sign with respect to each other. This complex gap configuration reveals the existence of orbital-selective Cooper pairing that, in FeSe, is based preferentially on electrons from the d yz orbitals of the iron atoms.« less

Discovery of orbital-selective Cooper pairing in FeSe

DOE Office of Scientific and Technical Information (OSTI.GOV)

Sprau, P. O.; Kostin, A.; Kreisel, A.

The superconductor iron selenide (FeSe) is of intense interest owing to its unusual nonmagnetic nematic state and potential for high-temperature superconductivity. But its Cooper pairing mechanism has not been determined. Here, we used Bogoliubov quasiparticle interference imaging to determine the Fermi surface geometry of the electronic bands surrounding the Γ = (0,0) and X = (π/a Fe, 0) points of FeSe and to measure the corresponding superconducting energy gaps. We show that both gaps are extremely anisotropic but nodeless and that they exhibit gap maxima oriented orthogonally in momentum space. Moreover, by implementing a novel technique, we demonstrate that thesemore » gaps have opposite sign with respect to each other. This complex gap configuration reveals the existence of orbital-selective Cooper pairing that, in FeSe, is based preferentially on electrons from the d yz orbitals of the iron atoms.« less

Surface Passivation of CdSe Quantum Dots in All Inorganic Amorphous Solid by Forming Cd1-xZnxSe Shell.

PubMed

Xia, Mengling; Liu, Chao; Zhao, Zhiyong; Wang, Jing; Lin, Changgui; Xu, Yinsheng; Heo, Jong; Dai, Shixun; Han, Jianjun; Zhao, Xiujian

2017-02-07

CdSe quantum dots (QDs) doped glasses have been widely investigated for optical filters, LED color converter and other optical emitters. Unlike CdSe QDs in solution, it is difficult to passivate the surface defects of CdSe QDs in glass matrix, which strongly suppress its intrinsic emission. In this study, surface passivation of CdSe quantum dots (QDs) by Cd 1-x Zn x Se shell in silicate glass was reported. An increase in the Se/Cd ratio can lead to the partial passivation of the surface states and appearance of the intrinsic emission of CdSe QDs. Optimizing the heat-treatment condition promotes the incorporation of Zn into CdSe QDs and results in the quenching of the defect emission. Formation of CdSe/Cd 1-x Zn x Se core/graded shell QDs is evidenced by the experimental results of TEM and Raman spectroscopy. Realization of the surface passivation and intrinsic emission of II-VI QDs may facilitate the wide applications of QDs doped all inorganic amorphous materials.

Magnetic excitations in iron chalcogenide superconductors.

PubMed

Kotegawa, Hisashi; Fujita, Masaki

2012-10-01

Nuclear magnetic resonance and neutron scattering experiments in iron chalcogenide superconductors are reviewed to make a survey of the magnetic excitations in FeSe, FeSe 1- x Te x and alkali-metal-doped A x Fe 2- y Se 2 ( A = K, Rb, Cs, etc). In FeSe, the intimate relationship between the spin fluctuations and superconductivity can be seen universally for the variations in the off-stoichiometry, the Co-substitution and applied pressure. The isovalent compound FeTe has a magnetic ordering with different wave vector from that of other Fe-based magnetic materials. The transition temperature T c of FeSe increases with Te substitution in FeSe 1- x Te x with small x , and decreases in the vicinity of the end member FeTe. The spin fluctuations are drastically modified by the Te substitution. In the vicinity of the end member FeTe, the low-energy part of the spin fluctuation is dominated by the wave vector of the ordered phase of FeTe; however, the reduction of T c shows that it does not support superconductivity. The presence of same wave vector as that of other Fe-based superconductors in FeSe 1- x Te x and the observation of the resonance mode demonstrate that FeSe 1- x Te x belongs to the same group as most of other Fe-based superconductors in the entire range of x , where superconductivity is mediated by the spin fluctuations whose wave vector is the same as the nesting vector between the hole pockets and the electron pockets. On the other hand, the spin fluctuations differ for alkali-metal-doped A x Fe 2- y Se 2 and FeSe or other Fe-based superconductors in their wave vector and strength in the low-energy part, most likely because of the different Fermi surfaces. The resonance mode with different wave vector suggests that A x Fe 2- y Se 2 has an exceptional superconducting symmetry among Fe-based superconductors.

Electronic structure and optical properties of noncentrosymmetric LiGaSe2: Experimental measurements and DFT band structure calculations

NASA Astrophysics Data System (ADS)

Lavrentyev, A. A.; Gabrelian, B. V.; Vu, V. T.; Ananchenko, L. N.; Isaenko, L. I.; Yelisseyev, A. P.; Khyzhun, O. Y.

2017-04-01

We report on measurements of X-ray photoelectron (XP) spectra for pristine and Ar+ ion-irradiated surfaces of LiGaSe2 single crystal grown by Bridgman-Stockbarger method. Electronic structure of the LiGaSe2 compound is studied from a theoretical and experimental viewpoint. In particular, total and partial densities of states of LiGaSe2 are investigated by density functional theory (DFT) calculations employing the augmented plane wave + local orbitals (APW + lo) method and they are verified by data of X-ray spectroscopy measurements. The DFT calculations indicate that the main contributors to the valence band of LiGaSe2 are the Se 4p states, which contribute mainly at the top and in the upper portion of the valence band, with also essential contributions of these states in the lower portion of the band. Other substantial contributions to the valence band of LiGaSe2 emerge from the Ga 4s and Ga 4p states contributing mainly at the lower ant upper portions of the valence band, respectively. With respect to the conduction band, the calculations indicate that its bottom is composed mainly from contributions of the unoccupied Ga s and Se p states. The present calculations are confirmed experimentally when comparing the XP valence-band spectrum of the LiGaS2 single crystal on a common energy scale with the X-ray emission bands representing the energy distribution of the Ga 4p and Se 4p states. Measurements of the fundamental absorption edges at room temperature reveal that bandgap value, Eg, of LiGaSe2 is equal to 3.47 eV and the Eg value increases up to 3.66 eV when decreasing temperature to 80 K. The main optical characteristics of the LiGaSe2 compound are clarified by the DFT calculations.

A transferable force field for CdS-CdSe-PbS-PbSe solid systems

NASA Astrophysics Data System (ADS)

Fan, Zhaochuan; Koster, Rik S.; Wang, Shuaiwei; Fang, Changming; Yalcin, Anil O.; Tichelaar, Frans D.; Zandbergen, Henny W.; van Huis, Marijn A.; Vlugt, Thijs J. H.

2014-12-01

A transferable force field for the PbSe-CdSe solid system using the partially charged rigid ion model has been successfully developed and was used to study the cation exchange in PbSe-CdSe heteronanocrystals [A. O. Yalcin et al., "Atomic resolution monitoring of cation exchange in CdSe-PbSe heteronanocrystals during epitaxial solid-solid-vapor growth," Nano Lett. 14, 3661-3667 (2014)]. In this work, we extend this force field by including another two important binary semiconductors, PbS and CdS, and provide detailed information on the validation of this force field. The parameterization combines Bader charge analysis, empirical fitting, and ab initio energy surface fitting. When compared with experimental data and density functional theory calculations, it is shown that a wide range of physical properties of bulk PbS, PbSe, CdS, CdSe, and their mixed phases can be accurately reproduced using this force field. The choice of functional forms and parameterization strategy is demonstrated to be rational and effective. This transferable force field can be used in various studies on II-VI and IV-VI semiconductor materials consisting of CdS, CdSe, PbS, and PbSe. Here, we demonstrate the applicability of the force field model by molecular dynamics simulations whereby transformations are initiated by cation exchange.

Nuclear structure properties and stellar weak rates for 76Se: Unblocking of the Gamow Teller strength

NASA Astrophysics Data System (ADS)

Nabi, Jameel-Un; Ishfaq, Mavra; Böyükata, Mahmut; Riaz, Muhammad

2017-10-01

At finite temperatures (≥ 107K), 76Se is abundant in the core of massive stars and electron capture on 76Se has a consequential role to play in the dynamics of core-collapse. The present work may be classified into two main categories. In the first phase we study the nuclear structure properties of 76Se using the interacting boson model-1 (IBM-1). The IBM-1 investigations include the energy levels, B (E 2) values and the prediction of the geometry. We performed the extended consistent-Q formalism (ECQF) calculation and later the triaxial formalism calculation (constructed by adding the cubic term to the ECQF). The geometry of 76Se can be envisioned within the formalism of the potential energy surface based on the classical limit of IBM-1 model. In the second phase, we reconfirm the unblocking of the Gamow-Teller (GT) strength in 76Se (a test case for nuclei having N > 40 and Z < 40). Using the deformed pn-QRPA model we calculate GT transitions, stellar electron capture cross section (within the limit of low momentum transfer) and stellar weak rates for 76Se. The distinguishing feature of our calculation is a state-by-state evaluation of stellar weak rates in a fully microscopic fashion. Results are compared with experimental data and previous calculations. The calculated GT distribution fulfills the Ikeda sum rule. Rates for β-delayed neutrons and emission probabilities are also calculated. Our study suggests that at high stellar temperatures and low densities, the β+-decay on 76Se should not be neglected and needs to be taken into consideration along with electron capture rates for simulation of presupernova evolution of massive stars.

Topological surface Fermi arcs in the magnetic Weyl semimetal Co3Sn2S2

NASA Astrophysics Data System (ADS)

Xu, Qiunan; Liu, Enke; Shi, Wujun; Muechler, Lukas; Gayles, Jacob; Felser, Claudia; Sun, Yan

2018-06-01

Very recently, the half-metallic compound Co3Sn2S2 was proposed to be a magnetic Weyl semimetal (WSM) with Weyl points only 60 meV above the Fermi level EF. Owing to the low charge carrier density and large Berry curvature induced, Co3Sn2S2 possesses both a large anomalous Hall conductivity and a large anomalous Hall angle, which provide strong evidence for the existence of Weyl points in Co3Sn2S2 . In this work, we theoretically study the surface topological feature of Co3Sn2S2 and its counterpart Co3Sn2Se2 . By cleaving the sample at the weak Sn-S/Se bonds, one can achieve two different surfaces terminated with Sn and S/Se atoms, respectively. The resulting Fermi-arc-related states can range from the energy of the Weyl points to EF-0.1 eV in the Sn-terminated surface. Therefore, it should be possible to observe the Fermi arcs in angle-resolved photoemission spectroscopy (ARPES) measurements. Furthermore, in order to simulate quasiparticle interference in scanning tunneling microscopy (STM) measurements, we also calculate the joint density of states for both terminals. This work should be helpful for a comprehensive understanding of the topological properties of these two magnetic WSMs and further ARPES and STM measurements.

Aqueous based synthesis of N-acetyl-L-cysteine capped ZnSe nanocrystals with intense blue emission

NASA Astrophysics Data System (ADS)

Soheyli, Ehsan; Sahraei, Reza; Nabiyouni, Gholamreza

2016-10-01

In this work a very simple reflux route for preparation of ZnSe nanocrystals with minor modification and faster preparation over conventional ones is introduced. X-ray diffraction analysis indicated that the ZnSe nanocrystals have a cubic structure. The complete disappearance of the S-H band in FT-IR spectrum of N-acetyl-L-cysteine capped ZnSe nanocrystals was an indication over formation of Zn-thiol covalent bonds at the surface of the nanocrystals which results in passivation of small nanocrystals. The strong size-quantization regime was responsible of significant blue shift in absorption/emission spectra. Using the well-known calculations, band gap and Urbach energy of the ZnSe nanocrystals were measured and their average size was estimated optically to be around 4.6 nm along with the TEM image. A dark blue emission with higher relative intensity of excitonic to trap emissions (compared to conventional method), very narrow excitonic emission peak of about 16 nm and remarkable stability was obtained from the ZnSe nanocrystals.

Interface-Driven Structural Distortions and Composition Segregation in Two-Dimensional Heterostructures

DOE PAGES

Ditto, Jeffrey; Merrill, Devin R.; Mitchson, Gavin; ...

2017-09-06

The discovery of emergent phenomena in 2D materials has sparked substantial research efforts in the materials community. A significant experimental challenge for this field is exerting atomistic control over the structure and composition of the constituent 2D layers and understanding how the interactions between layers drive both structure and properties. While no segregation for single bilayers was observed, segregation of Pb to the surface of three bilayer thick PbSe–SnSe alloy layers was discovered within [(Pb xSn 1–xSe) 1+δ] n(TiSe 2) 1 heterostructures using electron microscopy. This segregation is thermodynamically favored to occur when Pb xSn 1–xSe layers are interdigitated withmore » TiSe 2 monolayers. DFT calculations indicate that the observed segregation depends on what is adjacent to the Pb xSn 1–xSe layers. As a result, the interplay between interface- and volume-free energies controls both the structure and composition of the constituent layers, which can be tuned using layer thickness.« less

Luminescence study of ZnSe/PVA (polyvinyl alcohol) composite film

DOE Office of Scientific and Technical Information (OSTI.GOV)

Lahariya, Vikas

The ZnSe nanocrystals have been prepared into poly vinyl alcohol(PVA) polymer matrix on glass using ZnCl2 and Na2SeSO3 as zinc and selenium source respectively. Poly vinyl Alcohol (PVA) used as polymer matrix cum capping agent due to their high viscosity and water solubility. It is transparent for visible region and prevents Se- ions to photo oxidation. The ZnSe/PVA composite film was deposited on glass substrate. The film was characterized by X Ray Diffraction (XRD) and UV-Visible absorption Spectroscopy and Photoluminescence. The X Ray Diffraction (XRD) study confirms the nanometer size (10 nm) particle formation within PVA matrix with cubic zinc blendmore » crystal structure. The UV-Visible Absorption spectrum of ZnSe/PVA composite film shown blue shift in absorption edge indicating increased band gap due to quantum confinement. The calculated energy band gap from the absorption edge using Tauc relation is 3.4 eV. From the Photoluminescence study a broad peak at 435 nm has been observed in violet blue region due to recombination of surface states.« less

Interface-Driven Structural Distortions and Composition Segregation in Two-Dimensional Heterostructures

DOE Office of Scientific and Technical Information (OSTI.GOV)

Ditto, Jeffrey; Merrill, Devin R.; Mitchson, Gavin

The discovery of emergent phenomena in 2D materials has sparked substantial research efforts in the materials community. A significant experimental challenge for this field is exerting atomistic control over the structure and composition of the constituent 2D layers and understanding how the interactions between layers drive both structure and properties. While no segregation for single bilayers was observed, segregation of Pb to the surface of three bilayer thick PbSe–SnSe alloy layers was discovered within [(Pb xSn 1–xSe) 1+δ] n(TiSe 2) 1 heterostructures using electron microscopy. This segregation is thermodynamically favored to occur when Pb xSn 1–xSe layers are interdigitated withmore » TiSe 2 monolayers. DFT calculations indicate that the observed segregation depends on what is adjacent to the Pb xSn 1–xSe layers. As a result, the interplay between interface- and volume-free energies controls both the structure and composition of the constituent layers, which can be tuned using layer thickness.« less

Study of optical properties of vacuum evaporated carbon nanotube containing Se80Te16Cu4 thin films

NASA Astrophysics Data System (ADS)

Upadhyay, A. N.; Tiwari, R. S.; Singh, Kedar

2016-08-01

Thin films of Se80Te16Cu4 glassy alloy and 3 wt.% of carbon nanotubes (CNTs) containing Se80Te16Cu4 glassy composite were deposited on clean glass substrate by thermal evaporation technique. The scanning electron microscope and energy dispersive x-ray analysis were performed to investigate the surface morphology and elemental composition of as synthesised samples. The reflectance and transmittance spectra of as-deposited thin films were recorded (200-1100 nm) by using UV/VIS/NIR spectrophotometer. The optical band gap and optical constants such as absorption coefficient (α), refractive index (n) and extinction coefficient (k) of Se80Te16Cu4 and 3 wt.% CNTs-Se80Te16Cu4 glassy composite thin films were calculated. It is observed that optical properties alter due to CNTs incorporation in Se80Te16Cu4 glassy alloy. Effect on optical properties due to CNTs incorporation can be explained in terms of concentration of unsaturated bonds/defects in the localised states.

Robust, functional nanocrystal solids by infilling with atomic layer deposition.

PubMed

Liu, Yao; Gibbs, Markelle; Perkins, Craig L; Tolentino, Jason; Zarghami, Mohammad H; Bustamante, Jorge; Law, Matt

2011-12-14

Thin films of colloidal semiconductor nanocrystals (NCs) are inherently metatstable materials prone to oxidative and photothermal degradation driven by their large surface-to-volume ratios and high surface energies. (1) The fabrication of practical electronic devices based on NC solids hinges on preventing oxidation, surface diffusion, ripening, sintering, and other unwanted physicochemical changes that can plague these materials. Here we use low-temperature atomic layer deposition (ALD) to infill conductive PbSe NC solids with metal oxides to produce inorganic nanocomposites in which the NCs are locked in place and protected against oxidative and photothermal damage. Infilling NC field-effect transistors and solar cells with amorphous alumina yields devices that operate with enhanced and stable performance for at least months in air. Furthermore, ALD infilling with ZnO lowers the height of the inter-NC tunnel barrier for electron transport, yielding PbSe NC films with electron mobilities of 1 cm2 V(-1) s(-1). Our ALD technique is a versatile means to fabricate robust NC solids for optoelectronic devices.

Surface properties of neutron-rich exotic nuclei within relativistic mean field formalisms

NASA Astrophysics Data System (ADS)

Bhuyan, M.; Carlson, B. V.; Patra, S. K.; Zhou, Shan-Gui

2018-02-01

In this theoretical study, we establish a correlation between the neutron skin thickness and the nuclear symmetry energy for the even-even isotopes of Fe, Ni, Zn, Ge, Se, and Kr within the framework of the axially deformed self-consistent relativistic mean field for the nonlinear NL 3* and density-dependent DD-ME1 interactions. The coherent density functional method is used to formulate the symmetry energy, the neutron pressure, and the curvature of finite nuclei as a function of the nuclear radius. We have performed broad studies for the mass dependence on the symmetry energy in terms of the neutron-proton asymmetry for mass 70 ≤A ≤96 . From this analysis, we found a notable signature of a shell closure at N =50 in the isotopic chains of Fe, Ni, Zn, Ge, Se, and Kr nuclei. The present study reveals a interrelationship between the characteristics of infinite nuclear matter and the neutron skin thickness of finite nuclei.

Fermiology and Superconductivity of Topological Surface States in PdTe2

NASA Astrophysics Data System (ADS)

Clark, O. J.; Neat, M. J.; Okawa, K.; Bawden, L.; Marković, I.; Mazzola, F.; Feng, J.; Sunko, V.; Riley, J. M.; Meevasana, W.; Fujii, J.; Vobornik, I.; Kim, T. K.; Hoesch, M.; Sasagawa, T.; Wahl, P.; Bahramy, M. S.; King, P. D. C.

2018-04-01

We study the low-energy surface electronic structure of the transition-metal dichalcogenide superconductor PdTe2 by spin- and angle-resolved photoemission, scanning tunneling microscopy, and density-functional theory-based supercell calculations. Comparing PdTe2 with its sister compound PtSe2 , we demonstrate how enhanced interlayer hopping in the Te-based material drives a band inversion within the antibonding p -orbital manifold well above the Fermi level. We show how this mediates spin-polarized topological surface states which form rich multivalley Fermi surfaces with complex spin textures. Scanning tunneling spectroscopy reveals type-II superconductivity at the surface, and moreover shows no evidence for an unconventional component of its superconducting order parameter, despite the presence of topological surface states.

Colloidal Nanocrystals with Near-infrared Optical Properties: Synthesis, Characterization, and Applications

NASA Astrophysics Data System (ADS)

Panthani, Matthew George

2011-07-01

Colloidal nanocrystals with optical properties in the near-infrared (NIR) are of interest for many applications such as photovoltaic (PV) energy conversion, bioimaging, and therapeutics. For PVs and other electronic devices, challenges in using colloidal nanomaterials often deal with the surfaces. Because of the high surface-to-volume ratio of small nanocrystals, surfaces and interfaces play an enhanced role in the properties of nanocrystal films and devices. Organic ligand-capped CuInSe2 (CIS) and Cu(InXGa 1-X)Se2 (CIGS) nanocrystals were synthesized and used as the absorber layer in prototype solar cells. By fabricating devices from spray-coated CuInSe nanocrystals under ambient conditions, solar-to-electric power conversion efficiencies as high as 3.1% were achieved. Many treatments of the nanocrystal films were explored. Although some treatments increased the conductivity of the nanocrystal films, the best devices were from untreated CIS films. By modifying the reaction chemistry, quantum-confined CuInSe XS2-X (CISS) nanocrystals were produced. The potential of the CISS nanocrystals for targeted bioimaging was demonstrated via oral delivery to mice and imaging of nanocrystal fluorescence. The size-dependent photoluminescence of Si nanocrystals was measured. Si nanocrystals supported on graphene were characterized by conventional transmission electron microscopy and spherical aberration (Cs)-corrected scanning transmission electron microscopy (STEM). Enhanced imaging contrast and resolution was achieved by using Cs-corrected STEM with a graphene support. In addition, clear imaging of defects and the organic-inorganic interface was enabled by utilizing this technique.

Achieving 14.4% Alcohol-Based Solution-Processed Cu(In,Ga)(S,Se)2 Thin Film Solar Cell through Interface Engineering.

PubMed

Park, Gi Soon; Chu, Van Ben; Kim, Byoung Woo; Kim, Dong-Wook; Oh, Hyung-Suk; Hwang, Yun Jeong; Min, Byoung Koun

2018-03-28

An optimization of band alignment at the p-n junction interface is realized on alcohol-based solution-processed Cu(In,Ga)(S,Se) 2 (CIGS) thin film solar cells, achieving a power-conversion-efficiency (PCE) of 14.4%. To obtain a CIGS thin film suitable for interface engineering, we designed a novel "3-step chalcogenization process" for Cu 2- x Se-derived grain growth and a double band gap grading structure. Considering S-rich surface of the CIGS thin film, an alternative ternary (Cd,Zn)S buffer layer is adopted to build favorable "spike" type conduction band alignment instead of "cliff" type. Suppression of interface recombination is elucidated by comparing recombination activation energies using a dark J- V- T analysis.

Operational tools and applications of EO satellite data to retrieve surface fluxes in semi-arid countries

NASA Astrophysics Data System (ADS)

Tanguy, Maliko

The objective of the thesis is to develop and evaluate useful tools and applications of Earth Observation (EO) satellite data to estimate surface fluxes in semi-arid countries. In a first part (Chapter 4), we assess the performance of a new parameterisation scheme of ground heat flux (G) to be used in remote sensing (RS) evapotranspiration (ET) estimation methods. The G-parameterisation optimized with AMMA flux data performs well and improves the sensible heat flux (H) and ET retrieved by means of the triangle method (Jiang & Islam, 2001). In a second part (Chapter 5), the triangle method is compared with ET estimated by means of a land surface model (JULES). An attempt is made to calibrate JULES using the triangle method through Monte Carlo simulations, but the two methods supply rather different results, indicating that further intercomparison tasks should be carried out to assess the performance of RS-based algorithms and land surface models in estimating the components of the land surface energy balance. Chapter 6 presents a set of operational examples for retrieving surface fluxes using RS data. The first example is the study of temporal evolution of ET-maps in Western Africa under monsoonal influence. In a second example, we apply the new scheme proposed in Chapter 4 to retrieve and analyse the long term evolution (2000-2009) of the surface energy balance components, G, H and ET at several sites of the Segura Basin (S-E Spain) using MODIS-Terra data (land surface temperature and NDVI). Temporal and spatial distribution of evapotranspiration reveals different controls on ET. (Chapter 6). In the last example, MODIS-Aqua Sea Surface Temperature (SST) is used to validate a mathematical model to retrieve surface fluxes in a Mediterranean coastal lagoon (Mar Menor, S-E Spain). El objetivo de esta tesis es de desarrollar y evaluar herramientas y aplicaciones de la teledetección para estimar flujos de superficie en zonas semiáridas. En una primera parte (Capítulo 4), se evalúa la fiabilidad de una nueva parametrización para estimar el flujo de calor en el suelo (G) con el fin de ser utilizado en métodos de estimación de la evapotranspiración (ET) usando datos de teledetección. La parametrización de G se optimiza usando datos de flujo de energía obtenido durante las campañas del proyecto AMMA, y muestra buenos resultados y una mejora de las estimaciones del flujo de calor sensible (H) y de ET cuando se utiliza conjuntamente con el método del triángulo (Jiang & Islam, 2001). En una segunda parte (Capítulo 5), el método del triángulo se compara con valores de ET estimado por un modelo de superficie terrestre (JULES). Se intenta calibrar JULES usando el método del triángulo mediante simulaciones de Monte Carlo, pero los dos métodos muestran resultados muy diferentes, indicando que se necesita tareas de comparación profundizadas para poder evaluar la eficacia de estos modelos (de superficie terrestre y basados en la teledetección) para estimar los flujos de energía a la superficie. El capítulo 6 presenta un conjunto de ejemplos de aplicaciones operacionales para estimar los flujos de superficie usando datos de teledetección. El primer ejemplo consiste en el estudio de la evolución temporal de mapas de ET en África occidental bajo la influencia del monzón africano. En el segundo ejemplo, se aplica la nueva parametrización de G descrita en el capítulo 4 para calcular y analizar la evolución a largo plazo (2000-2009) de los componentes del balance de energía a la superficie, G, H y ET, en diferentes puntos de la cuenca del río Segura (Sureste español) utilizando datos del sensor MODIS-Terra (temperatura superficial y NDVI). La distribución temporal y espacial de ET revela diferentes controles sobre ET. En el último ejemplo, datos de temperatura superficial del mar del sensor MODIS-Aqua se utilizaron para validar un modelo matemático para calcular los flujos superficiales de una laguna costera del Mediterráneo (Mar Menor en el Sureste español).

Ohmic Contact Fabrication Using a Focused-ion Beam Technique and Electrical Characterization for Layer Semiconductor Nanostructures.

PubMed

Chen, Ruei-San; Tang, Chih-Che; Shen, Wei-Chu; Huang, Ying-Sheng

2015-12-05

Layer semiconductors with easily processed two-dimensional (2D) structures exhibit indirect-to-direct bandgap transitions and superior transistor performance, which suggest a new direction for the development of next-generation ultrathin and flexible photonic and electronic devices. Enhanced luminescence quantum efficiency has been widely observed in these atomically thin 2D crystals. However, dimension effects beyond quantum confinement thicknesses or even at the micrometer scale are not expected and have rarely been observed. In this study, molybdenum diselenide (MoSe2) layer crystals with a thickness range of 6-2,700 nm were fabricated as two- or four-terminal devices. Ohmic contact formation was successfully achieved by the focused-ion beam (FIB) deposition method using platinum (Pt) as a contact metal. Layer crystals with various thicknesses were prepared through simple mechanical exfoliation by using dicing tape. Current-voltage curve measurements were performed to determine the conductivity value of the layer nanocrystals. In addition, high-resolution transmission electron microscopy, selected-area electron diffractometry, and energy-dispersive X-ray spectroscopy were used to characterize the interface of the metal-semiconductor contact of the FIB-fabricated MoSe2 devices. After applying the approaches, the substantial thickness-dependent electrical conductivity in a wide thickness range for the MoSe2-layer semiconductor was observed. The conductivity increased by over two orders of magnitude from 4.6 to 1,500 Ω(-) (1) cm(-) (1), with a decrease in the thickness from 2,700 to 6 nm. In addition, the temperature-dependent conductivity indicated that the thin MoSe2 multilayers exhibited considerably weak semiconducting behavior with activation energies of 3.5-8.5 meV, which are considerably smaller than those (36-38 meV) of the bulk. Probable surface-dominant transport properties and the presence of a high surface electron concentration in MoSe2 are proposed. Similar results can be obtained for other layer semiconductor materials such as MoS2 and WS2.

Ohmic Contact Fabrication Using a Focused-ion Beam Technique and Electrical Characterization for Layer Semiconductor Nanostructures

PubMed Central

Chen, Ruei-San; Tang, Chih-Che; Shen, Wei-Chu; Huang, Ying-Sheng

2015-01-01

Layer semiconductors with easily processed two-dimensional (2D) structures exhibit indirect-to-direct bandgap transitions and superior transistor performance, which suggest a new direction for the development of next-generation ultrathin and flexible photonic and electronic devices. Enhanced luminescence quantum efficiency has been widely observed in these atomically thin 2D crystals. However, dimension effects beyond quantum confinement thicknesses or even at the micrometer scale are not expected and have rarely been observed. In this study, molybdenum diselenide (MoSe2) layer crystals with a thickness range of 6-2,700 nm were fabricated as two- or four-terminal devices. Ohmic contact formation was successfully achieved by the focused-ion beam (FIB) deposition method using platinum (Pt) as a contact metal. Layer crystals with various thicknesses were prepared through simple mechanical exfoliation by using dicing tape. Current-voltage curve measurements were performed to determine the conductivity value of the layer nanocrystals. In addition, high-resolution transmission electron microscopy, selected-area electron diffractometry, and energy-dispersive X-ray spectroscopy were used to characterize the interface of the metal–semiconductor contact of the FIB-fabricated MoSe2 devices. After applying the approaches, the substantial thickness-dependent electrical conductivity in a wide thickness range for the MoSe2-layer semiconductor was observed. The conductivity increased by over two orders of magnitude from 4.6 to 1,500 Ω−1 cm−1, with a decrease in the thickness from 2,700 to 6 nm. In addition, the temperature-dependent conductivity indicated that the thin MoSe2 multilayers exhibited considerably weak semiconducting behavior with activation energies of 3.5-8.5 meV, which are considerably smaller than those (36-38 meV) of the bulk. Probable surface-dominant transport properties and the presence of a high surface electron concentration in MoSe2 are proposed. Similar results can be obtained for other layer semiconductor materials such as MoS2 and WS2. PMID:26710105

Probing Selenium-Ion Distributions and Changes in Redox-State at Biofilm/Mineral Interfaces by Coupling Long-period X-ray Standing Wave and XANES Measurements

NASA Astrophysics Data System (ADS)

Templeton, A. S.; Trainor, T. P.; Spormann, A. M.; Brown, G. E.

2002-12-01

Metal sorption and precipitation reactions at biological as well as mineral surfaces are important controls on metal speciation and bioavailability in natural environments. When highly hydrated biofilms form on mineral surfaces, numerous competitive and synergistic effects are predicted to occur. Experimentally, it is challenging to determine where the sorbed metal ions are localized, the relative affinity of the biological vs. mineral surface sites, or to monitor biomineralization reactions or changes in metal speciation that may also occur. A large part of the difficulty is due to the low concentrations of sorbed ions, the small length-scale of the biofilm-mineral interface, and the complex interplay between microbially-catalayzed redox transformations vs. sorption and/or transport processes. Long-period x-ray standing wave (XSW) techniques are well-suited to determining the vertical distribution of metal(oid) species within biofilms overlying mineral surfaces. We will discuss experiments where Se fluorescence yield profiles are used to compare the affinity of Burkholderia cepacia biofilms for binding Se(IV) and Se(VI) species relative to underlying alpha-Al2O3 substrates over three orders of magnitude in [Se]. In addition, we will discuss how coupling the XSW experiments to grazing-incidence, spatially-resolved Se K-edge XANES spectroscopy can be used to differentiate between the oxidation state of the Se complexes localized within the biofilm vs. the mineral surface. This approach is used to monitor changes in the relative distributions of Se(VI), Se(IV) and Se(0) species as a function of time and proximity to the mineral surface. The long-period XSW data show that selenite preferentially binds to the oxide surfaces, particularly at low [Se]. When B. cepacia is metabolically active, B. cepacia rapidly reduces a fraction of the Se(IV) to the red elemental Se form. In contrast, selenate is preferentially partitioned into the B. cepacia biofilms at all [Se] tested due to a lower affinity for binding to the mineral surface. XANES spectra show that rapid reduction of selenate by B. cepacia to Se(IV) and Se(0) species subsequently results in a vertical segregation of Se species at the B. cepacia/alpha-Al2O3 interface. Elemental Se accumulates within the biofilm with the Se(VI), whereas selenite intermediates preferentially sorb to the underlying oxide surface.

{112} Polar surfaces of copper(indium,gallium)selenide: Properties and effects on crystal growth

NASA Astrophysics Data System (ADS)

Liao, Dongxiang

Cu(In,Ga)Se2 (GIGS) are promising materials for thin film photovoltaic applications. This work studies the epitaxial growth of CIGS single crystal films on GaAs substrates of various orientations and characterizes the properties of the thin films. A surprising finding is the strong tendency of film surfaces to facet to {112} planes. The work attempted to establish the connections between the film morphology, the surface energies, the surface chemical compositions, and the reconstruction of polar surfaces. Using angle-resolved photoelectron emission spectroscopy, I found that there is a severe Cu depletion at the first 1-2 layer of the free surface of CuInSe2 and the surface is semiconducting. The results strongly support the model of a reconstructed non-stoichiometric polar surface and exclude the previously believed existence of a bulk second phase on the CIS surface. Unique features of the film morphology suggest that the properties and structure of the polar surfaces have great effects on the growth of the crystals, and probably on the incorporation of the large amount of point defects. Measured chemical composition profiles indicate that the Cu depletion observed on free CIGS surface remains at the CIGS/CdS heterojunction interface and Cd is incorporated into the surface of CIGS. It is proposed that this non-stoichiometric composition leads to charge imbalance at the interface and causes the type-inversion of the CIGS surface, which are favorable for the device performance.

Impact of stacking order on the microstructural properties of Cu2ZnGeSe4 thin film absorber layer

NASA Astrophysics Data System (ADS)

Mary, G. Swapna; Chandra, G. Hema; Sunil, M. Anantha; Subbaiah, Y. P. Venkata; Gupta, Mukul; Rao, R. Prasada

2018-05-01

Six possible multiple stacks of Cu-ZnSe-Ge with selenium incorporation at a precursor stage were prepared using electron beam evaporation followed by vacuum selenization at 475 °C for 30 min to investigate the role of stacking order on the growth and properties of Cu2ZnGeSe4 films. The X-ray diffraction measurements affirm the existence of various binary and ternary phases (ZnSe, Cu2Se, GeSe2 and Cu2GeSe3) for all the precursor stacks. These phases are completely diminished after selenization at 475 °C except a minor co-existence of ZnSe (111) phase along with dominant Cu2ZnGeSe4 (112) phase for stack A: (Cu/Se/ZnSe/Se/Ge/Se) × 4. The Raman measurements for selenized multiple stack A, revealed two major A3, A1 modes at 206 cm-1 and 176 cm-1 and one minor E5 mode at 270 cm-1 corresponding to CZGSe phase. The surface morphology and the elemental distribution across the thickness found to vary significantly with the change of stacking order. The selenized multiple stacks A films shows densely packed flake and capsule shaped grains. The selenized stack A found to have a direct energy band gap of 1.60 eV, showing p-type conductivity with a Hall mobility of 22 cm2 (Vs)-1.

Clean Energy Solutions Center and SE4All: Partnering to Support Country Actions

DOE Office of Scientific and Technical Information (OSTI.GOV)

2016-05-01

Since 2012, the Clean Energy Solutions Center (Solutions Center) and Sustainable Energy for All (SE4All) have partnered to deliver information, knowledge and expert assistance to policymakers and practitioners in countries actively working to achieve SE4All objectives. Through SE4All efforts, national governments are implementing integrated country actions to strategically transform their energy markets. This fact sheet details the Solutions Center and SE4All partnership and available areas of technical assistance.

Determining suitability of Large Aperture Scintillometer for validating remote sensing based evapotranspiration maps

NASA Astrophysics Data System (ADS)

Paul, G.; Gowda, P. H.; Howell, T. A.; Basu, S.; Colaizzi, P. D.; Marek, T.

2013-12-01

Scintillation method is a relatively new technique for measuring the sensible heat and water fluxes over land surfaces. Path integrating capabilities of scintillometer over heterogeneous landscapes make it a potential tool for comparing the energy fluxes derived from remote sensing based energy balance algorithms. For this reason, scintillometer-derived evapotranspiration (ET) fluxes are being used to evaluate remote sensing based energy balance algorithms for their ability to estimate ET fluxes. However, LAS' (Large Aperture Scintillometer) ability to derive ET fluxes is not thoroughly tested. The objective of this study was to evaluate LAS- and Surface Energy Balance System (SEBS)-derived fluxes against lysimetric data to determine LAS' suitability for validating remote sensing based evapotranspiration (ET) maps. The study was conducted during the Bushland Evapotranspiration and Agricultural Remote sensing EXperiment - 2008 (BEAREX-08) at the USDA-ARS Conservation and Production Research Laboratory (CPRL), Bushland, Texas. SEBS was coded in a GIS environment to retrieve ET fluxes from the high resolution imageries acquired using airborne multispectral sensors. The CPRL has four large weighing lysimeters (3 m long x 3 m wide x 2.4 m deep), each located in the middle of approximately 5 ha fields, arranged in a block pattern. The two lysimeter fields located on the east (NE and SE) were managed under irrigated conditions, and the other two lysimeters on the west (NW and SW) were under dryland management. Each lysimeter field was equipped with an automated weather station that provided measurements for net radiation (Rn), Ts, soil heat flux (Go), Ta, relative humidity, and wind speed. During BEAREX08, the NE and SE fields were planted to cotton on May 21, and the NW and SW dryland lysimeters fields were planted to cotton on June 5. One LAS each was deployed across two large dryland lysimeter fields (NW and SW) and two large irrigated lysimeter fields (NE and SE). The structural parameter of refractive index of air was measured at 1-min interval and averaged at 15-min, and synchronized with weather station. The source area (footprint) of the surface energy fluxes were computed using a footprint model. ET fluxes were derived using LAS-estimated H as a residual from the energy balance equation. Comparison of SEBS- and LAS-derived ET fluxes were made against lysimetric data and performance of each method was discussed to determine the suitability of LAS for evaluating accuracy of remote sensing based ET maps.

Carrier multiplication in semiconductor nanocrystals: theoretical screening of candidate materials based on band-structure effects.

PubMed

Luo, Jun-Wei; Franceschetti, Alberto; Zunger, Alex

2008-10-01

Direct carrier multiplication (DCM) occurs when a highly excited electron-hole pair decays by transferring its excess energy to the electrons rather than to the lattice, possibly exciting additional electron-hole pairs. Atomistic electronic structure calculations have shown that DCM can be induced by electron-hole Coulomb interactions, in an impact-ionization-like process whose rate is proportional to the density of biexciton states rho XX. Here we introduce a DCM "figure of merit" R2(E) which is proportional to the ratio between the biexciton density of states rhoXX and the single-exciton density of states rhoX, restricted to single-exciton and biexciton states that are coupled by Coulomb interactions. Using R2(E), we consider GaAs, InAs, InP, GaSb, InSb, CdSe, Ge, Si, and PbSe nanocrystals of different sizes. Although DCM can be affected by both quantum-confinement effects (reflecting the underly electronic structure of the confined dot-interior states) and surface effects, here we are interested to isolate the former. To this end the nanocrystal energy levels are obtained from the corresponding bulk band structure via the truncated crystal approximation. We find that PbSe, Si, GaAs, CdSe, and InP nanocrystals have larger DCM figure of merit than the other nanocrystals. Our calculations suggest that high DCM efficiency requires high degeneracy of the corresponding bulk band-edge states. Interestingly, by considering band structure effects we find that as the dot size increases the DCM critical energy E0 (the energy at which R2(E) becomes >or=1) is reduced, suggesting improved DCM. However, whether the normalized E0/epsilong increases or decreases as the dot size increases depends on dot material.

Semiconductor electrolyte photovoltaic energy converter

NASA Technical Reports Server (NTRS)

Anderson, W. W.; Anderson, L. B.

1975-01-01

Feasibility and practicality of a solar cell consisting of a semiconductor surface in contact with an electrolyte are evaluated. Basic components and processes are detailed for photovoltaic energy conversion at the surface of an n-type semiconductor in contact with an electrolyte which is oxidizing to conduction band electrons. Characteristics of single crystal CdS, GaAs, CdSe, CdTe and thin film CdS in contact with aqueous and methanol based electrolytes are studied and open circuit voltages are measured from Mott-Schottky plots and open circuit photo voltages. Quantum efficiencies for short circuit photo currents of a CdS crystal and a 20 micrometer film are shown together with electrical and photovoltaic properties. Highest photon irradiances are observed with the GaAs cell.

Growth and characterization of PbSe and Pb{sub 1{minus}x}Sn{sub x}Se layers on Si (100)

DOE Office of Scientific and Technical Information (OSTI.GOV)

Sachar, H.K.; Chao, I.; Fang, X.M.

1998-12-31

Crack-free layers of PbSe were grown on Si (100) by a combination of liquid phase epitaxy (LPE) and molecular beam epitaxy (MBE) techniques. The PbSe layer was grown by LPE on Si(100) using a MBE-grown PbSe/BaF{sub 2}/CaF{sub 2} buffer layer structure. Pb{sub 1{minus}x}Sn{sub x}Se layers with tin contents in the liquid growth solution equal to 3%, 5%, 6%, 7%, and 10%, respectively, were also grown by LPE on Si(100) substrates using similar buffer layer structures. The LPE-grown PbSe and Pb{sub 1{minus}x}Sn{sub x}Se layers were characterized by optical Nomarski microscopy, X-ray diffraction (XRD), Fourier transform infrared spectroscopy (FTIR), and scanning electronmore » microscopy (SEM). Optical Nomarski characterization of the layers revealed their excellent surface morphologies and good growth solution wipe-offs. FTIR transmission experiments showed that the absorption edge of the Pb{sub 1{minus}x}Sn{sub x}Se layers shifted to lower energies with increasing tin contents. The PbSe epilayers were also lifted-off from the Si substrate by dissolving the MBE-grown BaF{sub 2} buffer layer. SEM micrographs of the cleaved edges revealed that the lifted-off layers formed structures suitable for laser fabrication.« less

Effect of selenization time on the structural and morphological properties of Cu(In,Ga)Se2 thin films absorber layers using two step growth process

NASA Astrophysics Data System (ADS)

Korir, Peter C.; Dejene, Francis B.

2018-04-01

In this work two step growth process was used to prepare Cu(In, Ga)Se2 thin film for solar cell applications. The first step involves deposition of Cu-In-Ga precursor films followed by the selenization process under vacuum using elemental selenium vapor to form Cu(In,Ga)Se2 film. The growth process was done at a fixed temperature of 515 °C for 45, 60 and 90 min to control film thickness and gallium incorporation into the absorber layer film. The X-ray diffraction (XRD) pattern confirms single-phase Cu(In,Ga)Se2 film for all the three samples and no secondary phases were observed. A shift in the diffraction peaks to higher 2θ (2 theta) values is observed for the thin films compared to that of pure CuInSe2. The surface morphology of the resulting film grown for 60 min was characterized by the presence of uniform large grain size particles, which are typical for device quality material. Photoluminescence spectra show the shifting of emission peaks to higher energies for longer duration of selenization attributed to the incorporation of more gallium into the CuInSe2 crystal structure. Electron probe microanalysis (EPMA) revealed a uniform distribution of the elements through the surface of the film. The elemental ratio of Cu/(In + Ga) and Se/Cu + In + Ga strongly depends on the selenization time. The Cu/In + Ga ratio for the 60 min film is 0.88 which is in the range of the values (0.75-0.98) for best solar cell device performances.

Investigation of Positron Sticking to the Surfaces of Topological Insulators

NASA Astrophysics Data System (ADS)

Shastry, K.; Joglekar, P. V.; Olenga, A. Y.; Fazleev, N. G.; Weiss, A. H.; Barniellini, B.

2013-03-01

We describe experiments aimed at probing the sticking of positrons to the surfaces of topological insulators. In these experiments, a magnetically beam will be used to deposit positrons at the surface of Bi2Te2Se. The energy spectra and intensities of electrons emitted as a result of Positron Annihilation induced Auger electron Spectroscopy (PAES) provides a distinct element specific signal which can be used to determine if positrons can be trapped efficiently into a surface localized bound state. The experiments are aimed at determining the practicality of using positron annihilation to selectively probe the critically important top most layer of topological insulator system. Welch Y1100, NSF DMR 0907679

Observation of Majorana fermions in the vortex on topological insulator-superconductor heterostructure Bi2Te3/NbSe2

NASA Astrophysics Data System (ADS)

Jia, Jinfeng

Majorana fermion (MF) zero modes have been predicted in a wide variety of condensed matter systems and proposed as a potential building block for fault-tolerant quantum computer. Signatures of the MFs have been reported in the form of zero-energy conductance peak in various systems. As predicted, MFs appear as zero-energy vortex core modes with distinctive spatial profile in proximity-induced superconducting surface states of topological insulators. Furthermore, MFs can induce spin selective Andreev reflection (SSAR), a unique signature of MFs. We report the observation of all the three features for the MFs inside vortices in Bi2Te3/NbSe2 hetero-structure, in which proximity-induced superconducting gap on topological surface states was previously established. Especially, by using spin-polarized scanning tunneling microscopy/spectroscopy (STM/STS), we observed the spin dependent tunneling effect, and fully supported by theoretical analyses, which is a direct evidence for the SSAR from MFs. More importantly, all evidences are self-consistent. Our work provides definitive evidences of MFs and will stimulate the MFs research on their novel physical properties, hence a step towards their non-Abelian statistics and application in quantum computing.

Quasiparticle dynamics in reshaped helical Dirac cone of topological insulators

PubMed Central

Miao, Lin; Wang, Z. F.; Ming, Wenmei; Yao, Meng-Yu; Wang, Meixiao; Yang, Fang; Song, Y. R.; Zhu, Fengfeng; Fedorov, Alexei V.; Sun, Z.; Gao, C. L.; Liu, Canhua; Xue, Qi-Kun; Liu, Chao-Xing; Liu, Feng; Qian, Dong; Jia, Jin-Feng

2013-01-01

Topological insulators and graphene present two unique classes of materials, which are characterized by spin-polarized (helical) and nonpolarized Dirac cone band structures, respectively. The importance of many-body interactions that renormalize the linear bands near Dirac point in graphene has been well recognized and attracted much recent attention. However, renormalization of the helical Dirac point has not been observed in topological insulators. Here, we report the experimental observation of the renormalized quasiparticle spectrum with a skewed Dirac cone in a single Bi bilayer grown on Bi2Te3 substrate from angle-resolved photoemission spectroscopy. First-principles band calculations indicate that the quasiparticle spectra are likely associated with the hybridization between the extrinsic substrate-induced Dirac states of Bi bilayer and the intrinsic surface Dirac states of Bi2Te3 film at close energy proximity. Without such hybridization, only single-particle Dirac spectra are observed in a single Bi bilayer grown on Bi2Se3, where the extrinsic Dirac states Bi bilayer and the intrinsic Dirac states of Bi2Se3 are well separated in energy. The possible origins of many-body interactions are discussed. Our findings provide a means to manipulate topological surface states. PMID:23382185

Quasiparticle dynamics in reshaped helical Dirac cone of topological insulators.

PubMed

Miao, Lin; Wang, Z F; Ming, Wenmei; Yao, Meng-Yu; Wang, Meixiao; Yang, Fang; Song, Y R; Zhu, Fengfeng; Fedorov, Alexei V; Sun, Z; Gao, C L; Liu, Canhua; Xue, Qi-Kun; Liu, Chao-Xing; Liu, Feng; Qian, Dong; Jia, Jin-Feng

2013-02-19

Topological insulators and graphene present two unique classes of materials, which are characterized by spin-polarized (helical) and nonpolarized Dirac cone band structures, respectively. The importance of many-body interactions that renormalize the linear bands near Dirac point in graphene has been well recognized and attracted much recent attention. However, renormalization of the helical Dirac point has not been observed in topological insulators. Here, we report the experimental observation of the renormalized quasiparticle spectrum with a skewed Dirac cone in a single Bi bilayer grown on Bi(2)Te(3) substrate from angle-resolved photoemission spectroscopy. First-principles band calculations indicate that the quasiparticle spectra are likely associated with the hybridization between the extrinsic substrate-induced Dirac states of Bi bilayer and the intrinsic surface Dirac states of Bi(2)Te(3) film at close energy proximity. Without such hybridization, only single-particle Dirac spectra are observed in a single Bi bilayer grown on Bi(2)Se(3), where the extrinsic Dirac states Bi bilayer and the intrinsic Dirac states of Bi(2)Se(3) are well separated in energy. The possible origins of many-body interactions are discussed. Our findings provide a means to manipulate topological surface states.

A methodology for investigating new nonprecious metal catalysts for PEM fuel cells.

PubMed

Susac, D; Sode, A; Zhu, L; Wong, P C; Teo, M; Bizzotto, D; Mitchell, K A R; Parsons, R R; Campbell, S A

2006-06-08

This paper reports an approach to investigate metal-chalcogen materials as catalysts for the oxygen reduction reaction (ORR) in proton exchange membrane (PEM) fuel cells. The methodology is illustrated with reference to Co-Se thin films prepared by magnetron sputtering onto a glassy-carbon substrate. Scanning Auger microscopy (SAM), X-ray photoelectron spectroscopy (XPS), energy-dispersive X-ray spectroscopy (EDX), and X-ray diffraction (XRD) have been used, in parallel with electrochemical activity and stability measurements, to assess how the electrochemical performance relates to chemical composition. It is shown that Co-Se thin films with varying Se are active for oxygen reduction, although the open circuit potential (OCP) is lower than for Pt. A kinetically controlled process is observed in the potential range 0.5-0.7 V (vs reversible hydrogen electrode) for the thin-film catalysts studied. An initial exposure of the thin-film samples to an acid environment served as a pretreatment, which modified surface composition prior to activity measurements with the rotating disk electrode (RDE) method. Based on the SAM characterization before and after electrochemical tests, all surfaces demonstrating activity are dominated by chalcogen. XRD shows that the thin films have nanocrystalline character that is based on a Co(1-x)Se phase. Parallel studies on Co-Se powder supported on XC72R carbon show comparable OCP, Tafel region, and structural phase as for the thin-film model catalysts. A comparison for ORR activity has also been made between this Co-Se powder and a commercial Pt catalyst.

The formation of organic (propolis films)/inorganic (layered crystals) interfaces for optoelectronic applications

NASA Astrophysics Data System (ADS)

Drapak, S. I.; Bakhtinov, A. P.; Gavrylyuk, S. V.; Kovalyuk, Z. D.; Lytvyn, O. S.

2008-10-01

Propolis (honeybee glue) organic films were prepared from an alcoholic solution on the surfaces of inorganic layered semiconductors (indium, gallium and bismuth selenides). Atomic force microscopy (AFM) and X-ray diffraction (XRD) are used to characterize structural properties of an organic/inorganic interfaces. It is shown that nanodimensional linear defects and nanodimensional cavities of various shapes are formed on the van der Waals (VDW) surfaces of layered crystals as a result of chemical interaction between the components of propolis (flavonoids, aminoacids and phenolic acids) and the VDW surfaces as well as deformation interaction between the VDW surfaces and propolis films during their polymerization. The nanocavities are formed as a result of the rupture of strong covalent bonds in the upper layers of layered crystals and have the shape of hexagons or triangles in the (0001) plane. The shape, lateral size and distribution of nanodimensional defects on the VDW surfaces depends on the type of crystals, the magnitude and distribution of surface stresses. We have obtained self-organized nanofold structures of propolis/InSe interface. It is established that such heterostructures have photosensitivity in the infrared range hν<1.2 eV (the values of energy gap are 1.2 eV for InSe and 3.07 eV for propolis films at room temperature).

The Advent of Indium Selenide: Synthesis, Electronic Properties, Ambient Stability and Applications

PubMed Central

Boukhvalov, Danil W.; Gürbulak, Bekir; Duman, Songül; Wang, Lin; Caputi, Lorenzo S.; Chiarello, Gennaro; Cupolillo, Anna

2017-01-01

Among the various two-dimensional semiconductors, indium selenide has recently triggered the interest of scientific community, due to its band gap matching the visible region of the electromagnetic spectrum, with subsequent potential applications in optoelectronics and especially in photodetection. In this feature article, we discuss the main issues in the synthesis, the ambient stability and the application capabilities of this novel class of two-dimensional semiconductors, by evidencing open challenges and pitfalls. In particular, we evidence how the growth of single crystals with reduced amount of Se vacancies is crucial in the road map for the exploitation of indium selenide in technology through ambient-stable nanodevices with outstanding values of both mobility of charge carriers and ON/OFF ratio. The surface chemical reactivity of the InSe surface, as well as applications in the fields of broadband photodetection, flexible electronics and solar energy conversion are also discussed. PMID:29113090

Structural, morphological and optical properties of pulsed laser deposited ZnSe/ZnSeO3 thin films

NASA Astrophysics Data System (ADS)

Hassan, Syed Ali; Bashir, Shazia; Zehra, Khushboo; Salman Ahmed, Qazi

2018-04-01

The effect of varying laser pulses on structural, morphological and optical behavior of Pulsed Laser Deposited (PLD) ZnSe/ZnSeO3 thin films has been investigated. The films were grown by employing Excimer laser (100 mJ, 248 nm, 18 ns, 30 Hz) at various number of laser pulses i.e. 3000, 4000, 5000 and 6000 with elevated substrate temperature of 300 °C. One film was grown at Room Temperature (RT) by employing 3000 number of laser pulses. In order to investigate the structural analysis of deposited films, XRD analysis was performed. It was observed that the room temperature is not favorable for the growth of crystalline film. However, elevated substrate temperature to 300°C, two phases with preferred orientation of ZnSeO3 (2 1 2) and ZnSe (3 3 1) were identified. AFM and SEM analysis were performed to explore the surface morphology of grown films. Morphological analysis also confirmed the non-uniform film growth at room temperature. At elevated substrate temperature (300 °C), the growth of dendritic rods and cubical crystalline structures are observed for lower number of laser pulses i.e. 3000 and 4000 respectively. With increased number of pulses i.e. 5000 and 6000, the films surface morphology becomes smooth which is confirmed by measurement of surface RMS roughness. Number of grains, skewness, kurtosis and other parameters have been evaluated by statistical analysis. In order to investigate the thickness, and optical properties of deposited films, ellipsometery and UV–Vis spectroscopy techniques were employed. The estimated band gap energy is 2.67 eV for the film grown at RT, whereas band gap values varies from 2.80 eV to 3.01 eV for the films grown at 300 °C with increasing number of laser pulses.

Comments on "The Sensitivity Study of Radiative-Convective Equilibrium in the Tropics with a Convective Resolving Model"

NASA Technical Reports Server (NTRS)

Tao, W.-K.; Shie, C.-L.; Simpson, J.

2000-01-01

In general, there are two broad scientific objectives when using cloud resolving models (CRMs or cloud ensemble models-CEMs) to study tropical convection. The first one is to use them as a physics resolving models to understand the dynamic and microphysical processes associated with the tropical water and energy cycles and their role in the climate system. The second approach is to use the CRMs to improve the representation of moist processes and their interaction with radiation in large-scale models. In order to improve the credibility of the CRMs and achieve the above goals, CRMs using identical initial conditions and large-scale influences need to produce very similar results. Two CRMs produced different statistical equilibrium (SE) states even though both used the same initial thermodynamic and wind conditions. Sensitivity tests to identify the major physical processes that determine the SE states for the different CRM simulations were performed. Their results indicated that atmospheric horizontal wind is treated quite differently in these two CRMs. The model that had stronger surface winds and consequently larger latent and sensible heat fluxes from the ocean produced a warmer and more humid modeled thermodynamic SE state. In addition, the domain mean thermodynamic state is more unstable for those experiments that produced a warmer and more humid SE state. Their simulated wet (warm and humid) SE states are thermally more stable in the lower troposphere (from the surface to 4-5 km in altitude). The large-scale horizontal advective effects on temperature and water vapor mixing ratio are needed when using CRMs to perform long-term integrations to study convective feedback under specified large-scale environments. In addition, it is suggested that the dry and cold SE state simulated was caused by enhanced precipitation but not enough surface evaporation. We find some problems with the interpretation of these three phenomena.

Shell effect on the electron and hole reorganization energy of core-shell II-VI nanoclusters

NASA Astrophysics Data System (ADS)

Cui, Xianhui; Wang, Xinqin; Yang, Fang; Cui, Yingqi; Yang, Mingli

2017-09-01

Density functional theory calculations were performed to study the effect of shell encapsulation on the geometrical and electronic properties of pure and hybrid core-shell CdSe nanoclusters. The CdSe cores are distorted by the shells, and the shells exhibit distinct surface activity from the cores, which leads to remarkable changes in their electron transition behaviors. Although the electron and hole reorganization energies, which are related to the formation and recombination of electron-hole pairs, vary in a complicated way, their itemized contributions, potentials of electron extraction, ionization and affinity, and hole extraction (HEP), are dependent on the cluster size, shell composition and/or solvent. Our calculations suggest that the behaviors of charge carriers, free electrons and holes, in the semiconductor core-shell nanoclusters can be modulated by selecting appropriate cluster size and controlling the chemical composition of the shells.

Probing Bioluminescence Resonance Energy Transfer in Quantum Rod-Luciferase Nanoconjugates.

PubMed

Alam, Rabeka; Karam, Liliana M; Doane, Tennyson L; Coopersmith, Kaitlin; Fontaine, Danielle M; Branchini, Bruce R; Maye, Mathew M

2016-02-23

We describe the necessary design criteria to create highly efficient energy transfer conjugates containing luciferase enzymes derived from Photinus pyralis (Ppy) and semiconductor quantum rods (QRs) with rod-in-rod (r/r) microstructure. By fine-tuning the synthetic conditions, CdSe/CdS r/r-QRs were prepared with two different emission colors and three different aspect ratios (l/w) each. These were hybridized with blue, green, and red emitting Ppy, leading to a number of new BRET nanoconjugates. Measurements of the emission BRET ratio (BR) indicate that the resulting energy transfer is highly dependent on QR energy accepting properties, which include absorption, quantum yield, and optical anisotropy, as well as its morphological and topological properties, such as aspect ratio and defect concentration. The highest BR was found using r/r-QRs with lower l/w that were conjugated with red Ppy, which may be activating one of the anisotropic CdSe core energy levels. The role QR surface defects play on Ppy binding, and energy transfer was studied by growth of gold nanoparticles at the defects, which indicated that each QR set has different sites. The Ppy binding at those sites is suggested by the observed BRET red-shift as a function of Ppy-to-QR loading (L), where the lowest L results in highest efficiency and furthest shift.

Thermal desorption of metals from tungsten single crystal surfaces

NASA Technical Reports Server (NTRS)

Bauer, E.; Bonczek, F.; Poppa, H.; Todd, G.

1975-01-01

After a short review of experimental methods used to determine desorption energies and frequencies the assumptions underlying the theoretical analysis of experimental data are discussed. Recent experimental results on the flash desorption of Cu, Ag, and Au from clean, well characterized W (110) and (100) surfaces are presented and analyzed in detail with respect to the coverage dependence. The results obtained clearly reveal the limitations of previous analytical methods and of the experimental technique per se (such as structure and phase changes below and in the temperature region in which desorption occurs).

Optically detecting the edge-state of a three-dimensional topological insulator under ambient conditions by ultrafast infrared photoluminescence spectroscopy

PubMed Central

Maezawa, Shun-ya; Watanabe, Hiroshi; Takeda, Masahiro; Kuroda, Kenta; Someya, Takashi; Matsuda, Iwao; Suemoto, Tohru

2015-01-01

Ultrafast infrared photoluminescence spectroscopy was applied to a three-dimensional topological insulator TlBiSe2 under ambient conditions. The dynamics of the luminescence exhibited bulk-insulating and gapless characteristics bounded by the bulk band gap energy. The existence of the topologically protected surface state and the picosecond-order relaxation time of the surface carriers, which was distinguishable from the bulk response, were observed. Our results provide a practical method applicable to topological insulators under ambient conditions for device applications. PMID:26552784

Spatial Imaging, Speciation, and Quantification of Selenium in theHyperaccumulator Plants Astragalus bisulcatus and Stanleya pinnata

DOE Office of Scientific and Technical Information (OSTI.GOV)

Freeman, J.L.; Zhang, L.H.; Marcus, M.A.

2006-09-01

Astragalus bisulcatus and Stanleya pinnata hyperaccumulate selenium (Se) up to 1% of plant dry weight. In the field, Se was mostly present in the young leaves and reproductive tissues of both hyperaccumulators. Microfocused scanning x-ray fluorescence mapping revealed that Se was hyperaccumulated in trichomes in young leaves of A. bisulcatus. None of 10 other elements tested were accumulated in trichomes. Micro x-ray absorption spectroscopy and liquid chromatography-mass spectrometry showed that Se in trichomes was present in the organic forms methylselenocysteine (MeSeCys; 53%) and {gamma}-glutamyl-MeSeCys (47%). In the young leaf itself, there was 30% inorganic Se (selenate and selenite) in additionmore » to 70% MeSeCys. In young S. pinnata leaves, Se was highly concentrated near the leaf edge and surface in globular structures that were shown by energy-dispersive x-ray microanalysis to be mainly in epidermal cells. Liquid chromatography-mass spectrometry revealed both MeSeCys (88%) and selenocystathionine (12%) inside leaf edges. In contrast, both the Se accumulator Brassica juncea and the nonaccumulator Arabidopsis thaliana accumulated Se in their leaf vascular tissues and mesophyll cells. Se in hyperaccumulators appears to be mobile in both the xylem and phloem because Se-treated S. pinnata was found to be highly toxic to phloem-feeding aphids, and MeSeCys was present in the vascular tissues of a S. pinnata young leaf petiole as well as in guttation fluid. The compartmentation of organic selenocompounds in specific storage areas in the plant periphery appears to be a unique property of Se hyperaccumulators. The high concentration of Se in the plant periphery may contribute to Se tolerance and may also serve as an elemental plant defense mechanism.« less

Surface and Bulk Effects of K in Highly Efficient Cu1-xKxInSe2 Solar Cells

DOE Office of Scientific and Technical Information (OSTI.GOV)

Muzzillo, Christopher; Mansfield, Lorelle M; Ramanathan, Kannan

To advance knowledge of the beneficial effects of K in Cu(In,Ga)(Se,S)2 (CIGS) photovoltaic (PV) absorbers, recent Cu-K-In-Se phase growth studies have been extended to PV performance. First, the effect of distributing K throughout bulk Cu1-xKxInSe2 absorbers at low K/(K+Cu) compositions (0 = x = 0.30) was studied. Efficiency, open-circuit voltage (VOC), and fill factor (FF) were greatly enhanced for x ~ 0.07, resulting in an officially-measured 15.0%-efficient solar cell, matching the world record CuInSe2 efficiency. The improvements were a result of reduced interface and bulk recombination, relative to CuInSe2 (x ~ 0). However, higher x compositions had reduced efficiency, short-circuitmore » current density (JSC), and FF due to greatly increased interface recombination, relative to the x ~ 0 baseline. Next, the effect of confining K at the absorber/buffer interface at high K/(K+Cu) compositions (0.30 = x = 0.92) was researched. Previous work showed that these surface layer growth conditions produced CuInSe2 with a large phase fraction of KInSe2. After optimization (75 nm surface layer with x ~ 0.41), these KInSe2 surface samples exhibited increased efficiency (officially 14.9%), VOC, and FF as a result of decreased interface recombination. The KInSe2 surfaces had features similar to previous reports for KF post-deposition treatments (PDTs) used in world record CIGS solar cells - taken as indirect evidence that KInSe2 can form during these PDTs. Both the bulk and surface growth processes greatly reduced interface recombination. However, the KInSe2 surface had higher K levels near the surface, greater lifetimes, and increased inversion near the buffer interface, relative to the champion bulk Cu1-xKxInSe2 absorber. These characteristics demonstrate that K may benefit PV performance by different mechanisms at the surface and in the absorber bulk.« less

Influences of CdSe NCs on the photovoltaic parameters of BHJ organic solar cells

NASA Astrophysics Data System (ADS)

Ongul, Fatih; Yuksel, Sureyya Aydin; Allahverdi, Cagdas; Bozar, Sinem; Kazici, Mehmet; Gunes, Serap

2018-04-01

In this study, the high quality CdSe nanocrystals (NCs) capped with stearic acid were synthesized in a solvent and then purified four times by using the precipitation and redissolution process. The average size of the synthesized CdSe NCs was determined 3.0 nm via transmission electron microscopy (TEM) measurement and their corresponding optical band edge energy was also calculated as 2.1 eV using ultraviolet-visible (UV-Vis) absorption spectroscopy. The bulk heterojunction (BHJ) hybrid solar cells based on a ternary system including P3HT, PCBM and CdSe NCs at different weight concentrations (0 wt%, 0.1 wt%, 0.5 wt%, 1 wt% and 2 wt%) were fabricated by spin-casting process. The effect of the concentration of CdSe NCs on the photovoltaic parameters of these BHJ organic solar cells was investigated. The surface morphology of the photoactive layer modified by the incorporation of CdSe NCs into P3HT:PCBM matrix was observed with scanning electron microscopy (SEM). It was shown that when the concentration of CdSe NCs increases above 0.1 wt% in this ternary system, the photovoltaic performance of the devices significantly decreases. The power conversion efficiency of the organic photovoltaic (OPV) device was enhanced 20% by incorporating CdSe NCs with 0.1 wt% with respect to those without CdSe NCs.

Influences of CdSe NCs on the photovoltaic parameters of BHJ organic solar cells.

PubMed

Ongul, Fatih; Yuksel, Sureyya Aydin; Allahverdi, Cagdas; Bozar, Sinem; Kazici, Mehmet; Gunes, Serap

2018-04-05

In this study, the high quality CdSe nanocrystals (NCs) capped with stearic acid were synthesized in a solvent and then purified four times by using the precipitation and redissolution process. The average size of the synthesized CdSe NCs was determined ~3.0nm via transmission electron microscopy (TEM) measurement and their corresponding optical band edge energy was also calculated as ~2.1eV using ultraviolet-visible (UV-Vis) absorption spectroscopy. The bulk heterojunction (BHJ) hybrid solar cells based on a ternary system including P3HT, PCBM and CdSe NCs at different weight concentrations (0wt%, 0.1wt%, 0.5wt%, 1wt% and 2wt%) were fabricated by spin-casting process. The effect of the concentration of CdSe NCs on the photovoltaic parameters of these BHJ organic solar cells was investigated. The surface morphology of the photoactive layer modified by the incorporation of CdSe NCs into P3HT:PCBM matrix was observed with scanning electron microscopy (SEM). It was shown that when the concentration of CdSe NCs increases above 0.1wt% in this ternary system, the photovoltaic performance of the devices significantly decreases. The power conversion efficiency of the organic photovoltaic (OPV) device was enhanced ~20% by incorporating CdSe NCs with 0.1wt% with respect to those without CdSe NCs. Copyright © 2017 Elsevier B.V. All rights reserved.

Transient and modulated charge separation at CuInSe2/C60 and CuInSe2/ZnPc hybrid interfaces

NASA Astrophysics Data System (ADS)

von Morzé, Natascha; Dittrich, Thomas; Calvet, Wolfram; Lauermann, Iver; Rusu, Marin

2017-02-01

Spectral dependent charge transfer and exciton dissociation have been investigated at hybrid interfaces between inorganic polycrystalline CuInSe2 (untreated and Na-conditioned) thin films and organic C60 as well as zinc phthalocyanine (ZnPc) layers by transient and modulated surface photovoltage measurements. The stoichiometry and electronic properties of the bare CuInSe2 surface were characterized by photoelectron spectroscopy which revealed a Cu-poor phase with n-type features. After the deposition of the C60 layer, a strong band bending at the CuInSe2 surface was observed. Evidence for dissociation of excitons followed by charge separation was found at the CuInSe2/ZnPc interface. The Cu-poor layer at the CuInSe2 surface was found to be crucial for transient and modulated charge separation at CuInSe2/organic hybrid interfaces.

High spin state driven magnetism and thermoelectricity in Mn doped topological insulator Bi2Se3

NASA Astrophysics Data System (ADS)

Maurya, V. K.; Dong, C. L.; Chen, C. L.; Asokan, K.; Patnaik, S.

2018-06-01

We report on the synthesis, and structural - magnetic characterizations of Mn doped Bi2Se3 towards achieving a magnetically doped topological insulator. High quality single crystals of MnxBi2-xSe3 (x = 0, 0.03, 0.05, 0.1) are grown and analysed by X-ray diffraction (XRD), Low Energy Electron Diffraction (LEED), Scanning electron microscopy (SEM), and X-ray absorption near-edge structure spectroscopy (XANES). Magnetic properties of these samples under ZFC-FC protocol and isothermal magnetization confirm ferromagnetic correlation above x = 0.03 value. XANES measurements confirm that the dopant Mn is in Mn2+ state. This is further reconfirmed to be in high spin state by fitting magnetic data with Brillouin function for J = 5/2. Both Hall and Seebeck measurements indicate a sign change of charge carriers above x = 0.03 value of Mn doping. We propose Mn doped Bi2Se3 to be a potential candidate for electromagnetic and thermoelectric device applications involving topological surface states.

The Key Ingredients of the Electronic Structure of FeSe

NASA Astrophysics Data System (ADS)

Coldea, Amalia I.; Watson, Matthew D.

2018-03-01

FeSe is a fascinating superconducting material at the frontier of research in condensed matter physics. Here, we provide an overview of the current understanding of the electronic structure of FeSe, focusing in particular on its low-energy electronic structure as determined from angle-resolved photoemission spectroscopy, quantum oscillations, and magnetotransport measurements of single-crystal samples. We discuss the unique place of FeSe among iron-based superconductors, as it is a multiband system exhibiting strong orbitally dependent electronic correlations and unusually small Fermi surfaces and is prone to different electronic instabilities. We pay particular attention to the evolution of the electronic structure that accompanies the tetragonal-orthorhombic structural distortion of the lattice around 90 K, which stabilizes a unique nematic electronic state. Finally, we discuss how the multiband multiorbital nematic electronic structure impacts our understanding of the superconductivity, and show that the tunability of the nematic state with chemical and physical pressure helps to disentangle the role of different competing interactions relevant for enhancing superconductivity.

Effects of hydrogen on the structural and optical properties of MoSe2 grown by hot filament chemical vapor deposition

NASA Astrophysics Data System (ADS)

Wang, B. B.; Zhu, M. K.; Levchenko, I.; Zheng, K.; Gao, B.; Xu, S.; Ostrikov, K.

2017-10-01

The role of reactive environment and hydrogen specifically in growth and structure of molybdenum selenide (MoSe2) nanomaterials is presently debated, and it is not clear whether hydrogen can promote the growth of MoSe2 sheets and alter their electronic properties. To find efficient, convenient methods for controlling the nucleation, growth and resultant properties of MoSe2 nanomaterials, MoSe2 nanoflakes were synthesized on silicon substrates by hot filament chemical vapor deposition using molybdenum trioxide and selenium powders in pure hydrogen, nitrogen gases and hydrogen-nitrogen mixtures. The structures and composition of synthesized MoSe2 nanoflakes were studied using the advanced characterization instruments including field emission scanning electron microscopy, micro-Raman spectroscopy, X-ray photoelectron spectroscopy, transmission electron microscopy and energy dispersive X-ray spectrometry. The analysis of the growth process indicates that hydrogen can improve the formation of MoSe2 nanoflakes and significantly alter their properties due to the high reduction capacity of hydrogen and the creation of more nucleation centers of MoSe2 nanoflakes on the silicon surface. The study of photoluminescent (PL) properties reveals that the MoSe2 nanoflakes can generate a strong PL band at about 631 nm, differently from the plain MoSe2 nanoflakes. The major difference in the PL properties may be related to the edges of MoSe2 nanoflakes. These results can be used to control the growth and structure of MoSe2-based nanomaterials and contribute to the development of advanced MoSe2-based optoelectronic devices.

Effect of sucrose ester concentration on the interfacial characteristics and physical properties of sodium caseinate-stabilized oil-in-water emulsions.

PubMed

Zhao, Qiangzhong; Liu, Daolin; Long, Zhao; Yang, Bao; Fang, Min; Kuang, Wanmei; Zhao, Mouming

2014-05-15

The effect of sucrose ester (SE) concentration on interfacial tension and surface dilatational modulus of SE and sodium caseinate (NaCas)-SE solutions were investigated. The critical micelle concentration (CMC) of SE was presumed to be 0.05% by measuring interfacial tension of SE solution. The interfacial tension of NaCas-SE solution decreased with increased SE concentration. A sharp increase in surface dilatational modulus of NaCas solution was observed when 0.01% SE was added and a decline was occurred at higher SE level. The influence of SE concentration on droplet size and confocal micrograph, surface protein concentration, ζ-potential and rheological properties of oil-in-water (O/W) emulsions prepared with 1% NaCas was also examined. The results showed that addition of SE reduced droplet size and surface protein concentration of the O/W emulsions. The ζ-potential of the O/W emulsions increased initially and decreased afterward with increased SE concentration. All the O/W emulsions exhibited a shear-thinning behaviour and the data were well-fitted into the Herschel-Bulkley model. Copyright © 2013 Elsevier Ltd. All rights reserved.

Chelating ligands for nanocrystals' surface functionalization.

PubMed

Querner, Claudia; Reiss, Peter; Bleuse, Joël; Pron, Adam

2004-09-22

A new family of ligands for the surface functionalization of CdSe nanocrystals is proposed, namely alkyl or aryl derivatives of carbodithioic acids (R-C(S)SH). The main advantages of these new ligands are as follows: they nearly quantitatively exchange the initial surface ligands (TOPO) in very mild conditions; they significantly improve the resistance of nanocrystals against photooxidation because of their ability of strong chelate-type binding to metal atoms; their relatively simple preparation via Grignard intermediates facilitates the development of new bifunctional ligands containing, in addition to the anchoring carbodithioate group, a second function, which enables the grafting of molecules or macromolecules of interest on the nanocrystal surface. To give an example of this approach, we report, for the first time, the grafting of an electroactive oligomer from the polyaniline family-aniline tetramer-on CdSe nanocrystals after their functionalization with 4-formyldithiobenzoic acid. The grafting proceeds via a condensation reaction between the aldehyde group of the ligand and the terminal primary amine group of the tetramer. The resulting organic/inorganic hybrid exhibits complete extinction of the fluorescence of its constituents, indicating efficient charge or energy transfer between the organic and the inorganic semiconductors.

Selenium-assisted controlled growth of graphene-Bi2Se3 nanoplates hybrid Dirac materials by chemical vapor deposition

NASA Astrophysics Data System (ADS)

Sun, Zhencui; Man, Baoyuan; Yang, Cheng; Liu, Mei; Jiang, Shouzhen; Zhang, Chao; Zhang, Jiaxin; Liu, Fuyan; Xu, Yuanyuan

2016-03-01

Se seed layers were used to synthesize the high-quality graphene-Bi2Se3 nanoplates hybrid Dirac materials via chemical vapor deposition (CVD) method. The morphology, crystallization and structural properties of the hybrid Dirac materials were characterized by SEM, EDS, Raman, XRD, AFM and HRTEM. The measurement results verify that the Se seed layer on the graphene surface can effectively saturate the surface dangling bonds of the graphene, which not only impel the uniform Bi2Se3 nanoplates growing along the horizontal direction but also can supply enough Se atoms to fill the Se vacancies. We also demonstrate the Se seed layer can effectively avoid the interaction of Bi2Se3 and the graphene. Further experiments testify the different Se seed layer on the graphene surface can be used to control the density of the Bi2Se3 nanoplates.

Substrate driven photochemistry of CdSe quantum dot films: charge injection and irreversible transformations on oxide surfaces.

PubMed

Tvrdy, Kevin; Kamat, Prashant V

2009-04-23

The photochemical behavior of CdSe quantum dots anchored to different surfaces was probed through their deposition on glass, SiO2, and TiO2 films. Following visible light irradiation under ambient conditions, CdSe quantum dots deposited on semiconducting TiO2 surface degraded, where no such degradation was observed when deposited on inert SiO2 surface or glass. Fluorescence decay and transient absorption experiments confirmed that charge injection from excited CdSe into TiO2 occurs with an apparent rate constant of 5.62 x 10(8) s(-1) and is the primary event responsible for photodegradation. In the presence of air, injected electrons are scavenged by surface adsorbed oxygen leaving behind reactive holes which induce anodic corrosion of CdSe quantum dots. In a vacuum environment, minimal CdSe degradation was observed as electron scavenging by oxygen is replaced with charge recombination between injected electrons and holes in CdSe nanocrystals. Spectroscopic measurements presented in this study highlight the role of both substrate and medium in dictating the photochemistry of CdSe quantum dots.

A microscopic study investigating the structure of SnSe surfaces

NASA Astrophysics Data System (ADS)

Kim, Sang-ui; Duong, Anh-Tuan; Cho, Sunglae; Rhim, S. H.; Kim, Jungdae

2016-09-01

SnSe has been widely studied due to its many potential applications that take advantage of its excellent thermoelectric, photovoltaic, and optoelectronic properties. However, experimental investigations into the microscopic structure of SnSe remain largely unexplored. Herein, for the first time, the atomic and electronic structures of SnSe surfaces are studied by a home-built low temperature scanning tunneling microscope (STM) and density functional theory (DFT) calculations. The cleaved surface of SnSe is comprised of covalently bonded Se and Sn atoms in zigzag patterns. However, rectangular periodicity was observed in the atomic images of SnSe surfaces for filled and empty state probing. Detailed atomic structures are analyzed by DFT calculations, indicating that the bright extrusions of both filled and empty state images are mostly located at the positions of Sn atoms.

Single-Nanoflake Photo-Electrochemistry Reveals Champion and Spectator Flakes in Exfoliated MoSe 2 Films

DOE PAGES

Todt, Michael A.; Isenberg, Allan E.; Nanayakkara, Sanjini U.; ...

2018-03-06

Semiconducting transition-metal dichalcogenide (TMD) nanoflake thin films are promising large-area electrodes for photo-electrochemical solar energy conversion applications. However, their energy conversion efficiencies are typically much lower than those of bulk electrodes. It is unclear to what extent this efficiency gap stems from differences among nanoflakes (e.g., area, thickness, and surface structural features). It is also unclear whether individual exfoliated nanoflakes can achieve energy conversion efficiencies similar to those of bulk crystals. Here, we use a single-nanoflake photo-electrochemical approach to show that there are both highly active and completely inactive nanoflakes within a film. For the exfoliated MoSe 2 samples studiedmore » herein, 7% of nanoflakes are highly active champions, whose photocurrent efficiency exceeds that of the bulk crystal. However, 66% of nanoflakes are inactive spectators, which are mostly responsible for the overall lower photocurrent efficiency compared to the bulk crystal. The photocurrent collection efficiency increases with nanoflake area and decreases more at perimeter edges than at interior step edges. These observations, which are hidden in ensemble-level measurements, reveal the underlying performance issues of exfoliated TMD electrodes for photo-electrochemical energy conversion applications.« less

Robust, functional nanocrystal solids by infilling with atomic layer deposition

DOE Office of Scientific and Technical Information (OSTI.GOV)

Liu, Yao; Gibbs, Markelle; Perkins, Craig L.

2011-12-14

Thin films of colloidal semiconductor nanocrystals (NCs) are inherently metatstable materials prone to oxidative and photothermal degradation driven by their large surface-to-volume ratios and high surface energies. The fabrication of practical electronic devices based on NC solids hinges on preventing oxidation, surface diffusion, ripening, sintering, and other unwanted physicochemical changes that can plague these materials. Here we use low-temperature atomic layer deposition (ALD) to infill conductive PbSe NC solids with metal oxides to produce inorganic nanocomposites in which the NCs are locked in place and protected against oxidative and photothermal damage. Infilling NC field-effect transistors and solar cells with amorphousmore » alumina yields devices that operate with enhanced and stable performance for at least months in air. Furthermore, ALD infilling with ZnO lowers the height of the inter-NC tunnel barrier for electron transport, yielding PbSe NC films with electron mobilities of 1 cm² V -1 s -1. Our ALD technique is a versatile means to fabricate robust NC solids for optoelectronic devices.« less

Comparison of Three Operative Models for Estimating the Surface Water Deficit using ASTER Reflective and Thermal Data

PubMed Central

García, Mónica; Villagarcía, Luis; Contreras, Sergio; Domingo, Francisco; Puigdefábregas, Juan

2007-01-01

Three operative models with minimum input data requirements for estimating the partition of available surface energy into sensible and latent heat flux using ASTER data have been evaluated in a semiarid area in SE Spain. The non-evaporative fraction (NEF) is proposed as an indicator of the surface water deficit. The best results were achieved with NEF estimated using the “Simplified relationship” for unstable conditions (NEFSeguin) and with the S-SEBI (Simplified Surface Energy Balance Index) model corrected for atmospheric conditions (NEFS-SEBIt,) which both produced equivalent results. However, results with a third model, NEFCarlson, that estimates the exchange coefficient for sensible heat transfer from NDVI, were unrealistic for sites with scarce vegetation cover. These results are very promising for an operative monitoring of the surface water deficit, as validation with field data shows reasonable errors, within those reported in the literature (RMSE were 0.18 and 0.11 for the NEF, and 29.12 Wm-2 and 25.97 Wm-2 for sensible heat flux, with the Seguin and S-SEBIt models, respectively).

Direct Magnetic Relief Recording Using As40S60: Mn-Se Nanocomposite Multilayer Structures.

PubMed

Stronski, A; Achimova, E; Paiuk, O; Meshalkin, A; Prisacar, A; Triduh, G; Oleksenko, P; Lytvyn, P

2017-12-01

Processes of holographic recording of surface relief structures using As 2 S 3 :Mn-Se multilayer nanostructures as registering media were studied in this paper. Optical properties of As 2 S 3 :Mn, Se layers, and As 2 S 3 :Mn-Se multilayer nanostructures were investigated. Values of optical bandgaps were obtained from Tauc dependencies. Surface relief diffraction gratings were recorded. Direct one-stage formation of surface relief using multilayer nanostructures is considered. For the first time, possibility of direct formation of magnetic relief simultaneous with surface relief formation under optical recording using As 2 S 3 :Mn-Se multilayer nanostructures is shown.

Evolution of opto-electronic properties during film formation of complex semiconductors

NASA Astrophysics Data System (ADS)

Heinemann, M. D.; Mainz, R.; Österle, F.; Rodriguez-Alvarez, H.; Greiner, D.; Kaufmann, C. A.; Unold, T.

2017-04-01

Optical and electrical properties of complex semiconducting alloys like Cu(In,Ga)Se2 (CIGS) are strongly influenced by the reaction pathways occurring during their deposition process. This makes it desirable to observe and control these properties in real-time during the deposition. Here we show for the first time the evolution of the band gap and the sub-band-gap defect absorption of CIGS thin film as well as surface roughness during a three-stage co-evaporation process by means of an optical analysis technique, based on white light reflectometry (WLR). By simultaneously recording structural information with in-situ energy dispersive X-ray diffraction and X-ray fluorescence we can directly correlate the evolution of opto-electronic material parameters with the structural properties of the film during growth. We find that the surface roughness and the sub-gap light absorption can be correlated with the phase evolution during the transformation from (In,Ga)2Se3 to Cu(In,Ga)Se2 by the incorporation of Cu into the film. Sub-bandgap light absorption is found to be influenced by the Cu-saturated growth phase and is lowered close to the points of stoichiometry, allowing for an advanced process design.

Synthesis and characterization of manganese diselenide nanoparticles (MnSeNPs): Determination of capsaicin by using MnSeNP-modified glassy carbon electrode.

PubMed

Sukanya, Ramaraj; Sakthivel, Mani; Chen, Shen-Ming; Chen, Tse-Wei; Al-Hemaid, Fahad M A; Ajmal Ali, M; Elshikh, Mohamed Soliman

2018-06-02

A new type of manganese diselenide nanoparticles (MnSeNPs) was synthesized by using a hydrothermal method. Their surface morphology, crystallinity and elemental distribution were characterized by using transmission electron microscopy, X-ray diffraction, energy dispersive X-ray spectroscopy, and X-ray photoelectron spectroscopy which scrutinize the formation of the NPs. The NPs were coated on a glassy carbon electrode (GCE), and electrochemical impedance spectroscopy, cyclic voltammetry and differential pulse voltammetry were applied to study the electroanalytical properties towards the oxidation of the food additive capsaicin. The modified GCE displays lower charge transfer resistance (R ct  = 29.52 Ω), a larger active surface area (0.089 cm 2 /g, and more efficient electrochemical oxidation of capsaicin compared to a MnS 2 /GCE and a bare GCE. The oxidation peak potential is 0.43 V (vs. Ag/AgCl) which is lower than that of previously reported GCEs. The sensor has a detection limit as low as 0.05 μM and an electrochemical sensitivity of 2.41 μA μM -1  cm -2 . The method was applied to the determination of capsaicin in pepper samples. Graphical abstract Electrochemical determination of capsaicin in pepper extract by using MnSeNPs modified electrode.

Investigation of argon ion sputtering on the secondary electron emission from gold samples

NASA Astrophysics Data System (ADS)

Yang, Jing; Cui, Wanzhao; Li, Yun; Xie, Guibai; Zhang, Na; Wang, Rui; Hu, Tiancun; Zhang, Hongtai

2016-09-01

Secondary electron (SE) yield, δ, is a very sensitive surface property. The values of δ often are not consistent for even identical materials. The influence of surface changes on the SE yield was investigated experimentally in this article. Argon ion sputtering was used to remove the contamination from the surface. Surface composition was monitored by X-ray photoelectron spectroscopy (XPS) and surface topography was scanned by scanning electron microscope (SEM) and atomic force microscope (AFM) before and after every sputtering. It was found that argon sputtering can remove contamination and roughen the surface. An ;equivalent work function; is presented in this thesis to establish the relationship between SE yield and surface properties. Argon ion sputtering of 1.5keV leads to a significant increase of so called ;work function; (from 3.7 eV to 6.0 eV), and a decrease of SE yield (from 2.01 to 1.54). These results provided a new insight into the influence of surface changes on the SE emission.

Synthesis characterisation series of newly fabricated type II CdSe CdSe/CdTe nanocrystals and their optical properties

NASA Astrophysics Data System (ADS)

Ahmed, A. S.; Christopher, W.

2018-03-01

Nanocrystalline semiconductors exhibit different properties due to two basic factors. They possess high surface to volume ratio and the actual size of particle can determine the electronic and physical properties of the material. The small size results in an observable quantum confinement effect, defined by the increasing bandgap accompanied by the quantization of the energy levels to discrete values. In present work we have synthesized the series of cadmium selenide/cadmium telluride (CdSe/CdTe) core/shell and CdSe/CdTe/CdS core/shell/shell to investigate the biexciton energy through transient absorption measurements. These structures are type II nanocrystals are with a hole in the shell and the electron confined to the core. We specifically investigate the effect of nanoparticle shape on the electronic structure and ultrafast electronic dynamics in the band-edge exciton states of CdSe quantum dots, nanorods, and nanoplatelets. Particle size was chosen to enable straightforward comparisons of the effects of particle shape on the spectra and dynamics without retuning the laser source. In our results the Uv-vis showed only a mild redshift in the first excitonic an elongated tail with increasing shell thickness. High resolution Transmission Electron Microscopy (HRTEM) shows the slight agglomeration of the nanocrystals but still the size distribution was calculate able. Spherical small crystals ranging from 5.9 nm to 10 nm are observed. CdTe/CdSe structures were quasi spherical with a rough diameter 6 nm with some little agglomerated structure. . The spherical nanocrystals could be peanut shaped oriented along the c axis or the spherical only, which could explain the two peak emission. p-XRD results indicate the predominant wurtzite structure throughout.

RBS-channeling study of radiation damage in Ar{sup +} implanted CuInSe{sub 2} crystals

DOE Office of Scientific and Technical Information (OSTI.GOV)

Yakushev, Michael V., E-mail: michael.yakushev@strath.ac.uk; Ural Federal University, Ekaterinburg 620002; Institute of Solid State Chemistry of the Urals Branch of RAS, Ekaterinburg 620990

2016-09-15

Chalcopyrite solar cells are reported to have a high tolerance to irradiation by high energy electrons or ions, but the origin of this is not well understood. This work studies the evolution of damage in Ar{sup +}-bombarded CuInSe{sub 2} single crystal using Rutherford backscattering/channeling analysis. Ar{sup +} ions of 30 keV were implanted with doses in the range from 10{sup 12} to 3 × 10{sup 16} cm{sup −2} at room temperature. Implantation was found to create two layers of damage: (1) on the surface, caused by preferential sputtering of Se and Cu atoms; (2) at the layer of implanted Ar, possibly consisting of stackingmore » faults and dislocation loops. The damage in the second layer was estimated to be less than 2% of the theoretical prediction suggesting efficient healing of primary implantation defects.« less

Effects of strain on the electronic structure, superconductivity, and nematicity in FeSe studied by angle-resolved photoemission spectroscopy

NASA Astrophysics Data System (ADS)

Phan, G. N.; Nakayama, K.; Sugawara, K.; Sato, T.; Urata, T.; Tanabe, Y.; Tanigaki, K.; Nabeshima, F.; Imai, Y.; Maeda, A.; Takahashi, T.

2017-06-01

One of central issues in iron-based superconductors is the role of structural change to the superconducting transition temperature (Tc). It was found in FeSe that the lattice strain leads to a drastic increase in Tc, accompanied by suppression of nematic order. By angle-resolved photoemission spectroscopy on tensile- or compressive-strained and strain-free FeSe, we experimentally show that the in-plane strain causes a marked change in the energy overlap (Δ Eh -e ) between the hole and electron pockets in the normal state. The change in Δ Eh -e modifies the Fermi-surface volume, leading to a change in Tc. Furthermore, the strength of nematicity is also found to be characterized by Δ Eh -e . These results suggest that the key to understanding the phase diagram is the fermiology and interactions linked to the semimetallic band overlap.

Solid-state reactions to synthesize nanostructured lead selenide semiconductor powders by high-energy milling

DOE Office of Scientific and Technical Information (OSTI.GOV)

Rojas-Chavez, H., E-mail: uu_gg_oo@yahoo.com.mx; Reyes-Carmona, F.; Jaramillo-Vigueras, D.

2011-10-15

Highlights: {yields} PbSe synthesized from PbO instead of Pb powder do not require an inert atmosphere. {yields} During high-energy milling oxygen has to be chemically reduced from the lead oxide. {yields} Solid-state and solid-gas chemical reactions promote both solid and gaseous products. -- Abstract: Both solid-solid and gas-solid reactions have been traced during high-energy milling of Se and PbO powders under vial (P, T) conditions in order to synthesize the PbSe phase. Chemical and thermodynamic arguments are postulated to discern the high-energy milling mechanism to transform PbO-Se micropowders onto PbSe-nanocrystals. A set of reactions were evaluated at around room temperature.more » Therefore an experimental campaign was designed to test the nature of reactions in the PbO-Se system during high-energy milling.« less

Controllable Surface Reorganization Engineering on Cobalt Phosphide Nanowire Arrays for Efficient Alkaline Hydrogen Evolution Reaction.

PubMed

Xu, Kun; Cheng, Han; Lv, Haifeng; Wang, Jingyu; Liu, Linqi; Liu, Si; Wu, Xiaojun; Chu, Wangsheng; Wu, Changzheng; Xie, Yi

2018-01-01

Developing highly efficient hydrogen evolution reaction (HER) catalysts in alkaline media is considered significant and valuable for water splitting. Herein, it is demonstrated that surface reorganization engineering by oxygen plasma engraving on electocatalysts successfully realizes a dramatically enhanced alkaline HER activity. Taking CoP nanowire arrays grown on carbon cloth (denoted as CoP NWs/CC) as an example, the oxygen plasma engraving can trigger moderate CoO x species formation on the surface of the CoP NWs/CC, which is visually verified by the X-ray absorption fine structure, high-resolution transmission electron microscopy, and energy-dispersive spectrometer (EDS) mapping. Benefiting from the moderate CoO x species formed on the surface, which can promote the water dissociation in alkaline HER, the surface reorganization of the CoP NWs/CC realizes almost fourfold enhanced alkaline HER activity and a 180 mV decreased overpotential at 100 mA cm -2 , compared with the pristine ones. More interestingly, this surface reorganization strategy by oxygen plasma engraving can also be effective to other electrocatalysts such as free-standing CoP, Co 4 N, O-CoSe 2 , and C-CoSe 2 nanowires, which verifies the universality of the strategy. This work thus opens up new avenues for designing alkaline HER electrocatalysts based on oxygen plasma engraving. © 2017 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Ab initio calculation of transport properties between PbSe quantum dots facets with iodide ligands

NASA Astrophysics Data System (ADS)

Wang, B.; Patterson, R.; Chen, W.; Zhang, Z.; Yang, J.; Huang, S.; Shrestha, S.; Conibeer, G.

2018-01-01

The transport properties between Lead Selenide (PbSe) quantum dots decorated with iodide ligands has been studied using density functional theory (DFT). Quantum conductance at each selected energy levels has been calculated along with total density of states and projected density of states. The DFT calculation is carried on using a grid-based planar augmented wave (GPAW) code incorporated with the linear combination of atomic orbital (LCAO) mode and Perdew Burke Ernzerhof (PBE) exchange-correlation functional. Three iodide ligand attached low index facets including (001), (011), (111) are investigated in this work. P-orbital of iodide ligand majorly contributes to density of state (DOS) at near top valence band resulting a significant quantum conductance, whereas DOS of Pb p-orbital shows minor influence. Various values of quantum conductance observed along different planes are possibly reasoned from a combined effect electrical field over topmost surface and total distance between adjacent facets. Ligands attached to (001) and (011) planes possess similar bond length whereas it is significantly shortened in (111) plane, whereas transport between (011) has an overall low value due to newly formed electric field. On the other hand, (111) plane with a net surface dipole perpendicular to surface layers leading to stronger electron coupling suggests an apparent increase of transport probability. Apart from previously mentioned, the maximum transport energy levels located several eVs (1 2 eVs) from the edge of valence band top.

A study on micro-structural and optical parameters of InxSe1-x thin film

NASA Astrophysics Data System (ADS)

Patel, P. B.; Desai, H. N.; Dhimmar, J. M.; Modi, B. P.

2018-04-01

Thin film of Indium Selenide (InSe) has been deposited by thermal evaporation technique onto pre cleaned glass substrate under high vacuum condition. The micro-structural and optical properties of InxSe1-x (x = 0.6, 1-x = 0.4) thin film have been characterized by X-ray diffractrometer (XRD) and UV-Visible spectrophotometer. The XRD spectra showed that InSe thin film has single phase hexagonal structure with preferred orientation along (1 1 0) direction. The micro-structural parameters (crystallite size, lattice strain, dislocation density, domain population) for InSe thin film have been calculated using XRD spectra. The optical parameters (absorption, transmittance, reflectance, energy band gap, Urbach energy) of InSe thin film have been evaluated from absorption spectra. The direct energy band gap and Urbach energy of InSe thin film is found to be 1.90 eV and 235 meV respectively.

A Reexamination of the Emergy Input to a System from the ...

EPA Pesticide Factsheets

The wind energy absorbed in the global boundary layer (GBL, 900 mb surface) is the basis for calculating the wind emergy input for any system on the Earth’s surface. Estimates of the wind emergy input to a system depend on the amount of wind energy dissipated, which can have a range of magnitudes for a given velocity depending on surface drag and atmospheric stability at the location and time period under study. In this study, we develop a method to consider this complexity in estimating the emergy input to a system from the wind. A new calculation of the transformity of the wind energy dissipated in the GBL (900 mb surface) based on general models of atmospheric circulation in the planetary boundary layer (PBL, 100 mb surface) is presented and expressed on the 12.0E+24 seJ y-1 geobiosphere baseline to complete the information needed to calculate the emergy input from the wind to the GBL of any system. The average transformity of wind energy dissipated in the GBL (below 900 mb) was 1241±650 sej J-1. The analysis showed that the transformity of the wind varies over the course of a year such that summer processes may require a different wind transformity than processes occurring with a winter or annual time boundary. This is a paper in the proceedings of Emergy Synthesis 9, thus it will be available online for those interested in this subject. The paper describes a new and more accurate way to estimate the wind energy input to any system. It also has a new cal

Why surface chemistry matters for QD–QD resonance energy transfer

DOE Office of Scientific and Technical Information (OSTI.GOV)

Hoffman, Jacob B.; Alam, Rabeka; Kamat, Prashant V.

Resonance energy transfer (RET) has been shown to occur in films of semiconductor quantum dots (QDs) with variation in QD composition and size. When coupled with charge carrier transfer, RET could provide a complementary strategy for light harvesting in QD based solid state photovoltaic devices. Due to a direct dependence on the optical properties of the donor and acceptor, QD surface chemistry plays a drastic role in determining the efficiency of RET. Here, the impact of QD surface chemistry on RET in QD films was investigated using a pair of different sized CdSe QDs spin-cast onto a glass substrate. Themore » effects of QD surface passivation on RET were studied by removing surface ligands through QD washing and adding an insulating ZnS shell. In addition, QD films were subjected to solid state ligand exchanges with thiolated ligands in order to mimic a layer-by-layer deposition method commonly used in the construction of QD photovoltaics. These solid state ligand exchanges exhibit drastic quenching of RET in the films. As a result, these experiments highlight the importance of understanding surface chemistry when designing photovoltaics that utilize RET.« less

Why surface chemistry matters for QD–QD resonance energy transfer

DOE PAGES

Hoffman, Jacob B.; Alam, Rabeka; Kamat, Prashant V.

2017-01-12

Resonance energy transfer (RET) has been shown to occur in films of semiconductor quantum dots (QDs) with variation in QD composition and size. When coupled with charge carrier transfer, RET could provide a complementary strategy for light harvesting in QD based solid state photovoltaic devices. Due to a direct dependence on the optical properties of the donor and acceptor, QD surface chemistry plays a drastic role in determining the efficiency of RET. Here, the impact of QD surface chemistry on RET in QD films was investigated using a pair of different sized CdSe QDs spin-cast onto a glass substrate. Themore » effects of QD surface passivation on RET were studied by removing surface ligands through QD washing and adding an insulating ZnS shell. In addition, QD films were subjected to solid state ligand exchanges with thiolated ligands in order to mimic a layer-by-layer deposition method commonly used in the construction of QD photovoltaics. These solid state ligand exchanges exhibit drastic quenching of RET in the films. As a result, these experiments highlight the importance of understanding surface chemistry when designing photovoltaics that utilize RET.« less

Structural and electrochemical analysis of chemically synthesized microcubic architectured lead selenide thin films

NASA Astrophysics Data System (ADS)

Bhat, T. S.; Shinde, A. V.; Devan, R. S.; Teli, A. M.; Ma, Y. R.; Kim, J. H.; Patil, P. S.

2018-01-01

The present work deals with the synthesis of lead selenide (PbSe) thin films by simple and cost-effective chemical bath deposition method with variation in deposition time. The structural, morphological, and electrochemical properties of as-deposited thin films were examined using characterization techniques such as X-ray diffraction spectroscopy (XRD), field-emission scanning electron microscopy (FE-SEM), X-ray photoelectron spectroscopy (XPS), cyclic voltammetry (CV), galvanostatic charge-discharge and electrochemical impedance spectroscopy. XRD reveals formation of rock salt phase cubic structured PbSe. FE-SEM images show the formation of microcubic structured morphology. The existence of the PbSe is confirmed from the XPS analysis. On the other hand, CV curves show four reaction peaks corresponding to oxidation [PbSe and Pb(OH)2] and reduction (PbO2 and Pb(OH)2) at the surface of PbSe thin films. The PbSe:2 sample deposited for 80 min. shows maximum specific capacitance of 454 ± 5 F g- 1 obtained at 0.25 mA cm- 2 current density. The maximum energy density of 69 Wh kg- 1 was showed by PbSe:2 electrode with a power density of 1077 W kg- 1. Furthermore, electrochemical impedance studies of PbSe:2 thin film show 80 ± 3% cycling stability even after 500 CV cycles. Such results show the importance of microcubic structured PbSe thin film as an anode in supercapacitor devices.

Spatial and thickness dependence of coupling interaction of surface states and influence on transport and optical properties of few-layer Bi2Se3

NASA Astrophysics Data System (ADS)

Li, Zhongjun; Chen, Shi; Sun, Jiuyu; Li, Xingxing; Qiu, Huaili; Yang, Jinlong

2018-02-01

Coupling interaction between the bottom and top surface electronic states and the influence on transport and optical properties of Bi2Se3 thin films with 1-8 quintuple layers (QLs) have been investigated by first principles calculations. Obvious spatial and thickness dependences of coupling interaction are found by analyzing hybridization of two surface states. In the thin film with a certain thickness, from the outer to inner atomic layers, the coupling interaction exhibits an increasing trend. On the other hand, as thickness increases, the coupling interaction shows a disproportionate decrease trend. Moreover, the system with 3 QLs exhibits stronger interaction than that with 2 QLs. The presence of coupling interaction would suppress destructive interference of surface states and enhance resistance in various degrees. In view of the inversely proportional relation to transport channel width, the resistance of thin films should show disproportionate thickness dependence. This prediction is qualitatively consistent with the transport measurements at low temperature. Furthermore, the optical properties also exhibit obvious thickness dependence. Especially as the thickness increases, the coupling interaction results in red and blue shifts of the multiple-peak structures in low and high energy regions of imaginary dielectric function, respectively. The red shift trend is in agreement with the recent experimental observation and the blue shift is firstly predicted by the present calculation. The present results give a concrete understanding of transport and optical properties in devices based on Bi2Se3 thin films with few QLs.

Effect of ZnSe/GaAs interface treatment in ZnSe quality control for optoelectronic device applications

DOE PAGES

Park, Kwangwook; Beaton, Daniel; Steirer, Kenneth X.; ...

2017-01-27

Here, we investigate the role of interface initiation conditions on the growth of ZnSe/GaAs heterovalent heterostructures. ZnSe epilayers were grown on a GaAs surface with various degrees of As-termination and the application of either a Zn or Se pre-treatment. Structural analysis revealed that Zn pre-treatment of an As-rich GaAs surface suppresses Ga 2Se 3 formation at the interface and promotes the growth of high crystal quality ZnSe. This is confirmed with low-temperature photoluminescence. However, moderation of Ga-Se bonding through a Se pre-treatment of an As-rich GaAs surface can prevent excessive intermixing at the interface and promote excitonic emission in themore » underlying GaAs layer. These results provide guidance on how best to prepare heterovalent interfaces for various applications.« less

Generalized stacking fault energies, cleavage energies, ionicity and brittleness of Cu(Al/Ga/In)Se2 and CuGa(S/Se/Te)2

NASA Astrophysics Data System (ADS)

Xue, H. T.; Tang, F. L.; Gruhn, T.; Lu, W. J.; Wan, F. C.; Rui, Z. Y.; Feng, Y. D.

2014-04-01

We calculate the generalized stacking fault (GSF) energies and cleavage energies γcl of the chalcopyrite compounds CuAlSe2, CuGaSe2, CuInSe2, CuGaS2 and CuGaTe2 using first principles. From the GSF energies, we obtain the unstable stacking fault energies γus and intrinsic stacking fault energies γisf. By analyzing γus and γisf, we find that the \\langle \\bar{{1}}\\,1\\,0\\rangle (1 1 2) direction is the easiest slip direction for these five compounds. Also, for CuInSe2, it is most possible to undergo a dislocation-nucleation-induced plastic deformation along the \\langle \\bar{{1}}\\,1\\,0\\rangle (1 1 2) slip direction. We show that the (1 1 2) plane is the preferable plane for fracture in the five compounds by comparing γcl of the (0 0 1) and (1 1 2) planes. It is also found that both γus and γcl decrease as the cationic or anionic radius increases in these chalcopyrites, i.e. along the sequences CuAlSe2 → CuGaSe2 → CuInSe2 and CuGaS2 → CuGaSe2 → CuGaTe2. Based on the values of the ratio γcl/γus, we discuss the brittle-ductile properties of these compounds. All of the compounds can be considered as brittle materials. In addition, a strong relationship between γcl/γus and the total proportion of ionic bonding in these compounds is found.

Semiconductor Nanowires and Nanotubes for Energy Conversion

NASA Astrophysics Data System (ADS)

Fardy, Melissa Anne

In recent years semiconductor nanowires and nanotubes have garnered increased attention for their unique properties. With their nanoscale dimensions comes high surface area and quantum confinement, promising enhancements in a wide range of applications. 1-dimensional nanostructures are especially attractive for energy conversion applications where photons, phonons, and electrons come into play. Since the bohr exciton radius and phonon and electron mean free paths are on the same length scales as nanowire diameters, optical, thermal, and electrical properties can be tuned by simple nanowire size adjustments. In addition, the high surface area inherent to nanowires and nanotubes lends them towards efficient charge separation and superior catalytic performance. In thermoelectric power generation, the nanoscale wire diameter can effectively scatter phonons, promoting reductions in thermal conductivity and enhancements in the thermoelectric figure of merit. To that end, single-crystalline arrays of PbS, PbSe, and PbTe nanowires have been synthesized by a chemical vapor transport approach. The electrical and thermal transport properties of the nanowires were characterized to investigate their potential as thermoelectric materials. Compared to bulk, the lead chalcogenide nanowires exhibit reduced thermal conductivity below 100 K by up to 3 orders of magnitude, suggesting that they may be promising thermoelectric materials. Smaller diameters and increased surface roughness are expected to give additional enhancements. The solution-phase synthesis of PbSe nanowires via oriented attachment of nanoparticles enables facile surface engineering and diameter control. Branched PbSe nanowires synthesized by this approach showed near degenerately doped charge carrier concentrations. Compared to the bulk, the PbSe nanowires exhibited a similar Seebeck coefficient and a significant reduction in thermal conductivity in the temperature range 20 K to 300 K. Thermal annealing of the PbSe nanowires allowed their thermoelectric properties to be controllably tuned by increasing their carrier concentration or hole mobility. After optimal annealing, single PbSe nanowires exhibited a thermoelectric figure of merit (ZT) of 0.12 at 300 K. In addition, using a field-effect gated device, the Seebeck coefficient of single PbSe nanowires could be tuned from 64 to 193 muV˙K-1. This direct electrical field control of the electrical conductivity and Seebeck coefficient suggests a powerful strategy for optimizing ZT in thermoelectric devices and these results represent the first demonstration of field-effect modulation of the thermoelectric figure of merit in a single semiconductor nanowire. This novel strategy for thermoelectric property modulation could prove especially important in optimizing the thermoelectric properties of semiconductors where reproducible doping is difficult to achieve. Recent theoretical work has shown large enhancements in ZT for single-crystal nanowires containing nanoscale interfaces along their lengths. M2O3(ZnO) n ( M = In, Ga, Fe) superlattice nanowires were synthesized via a novel solid-state diffusion approach to investigate this possible enhancement. Using atomic resolution Z-contrast STEM imaging a detailed structural analysis was performed on In2-xGaxO3(ZnO) n nanowires, leading to the discovery that octahedral inclusions within the superlattice structure are likely generated through a defect-assisted process. Single-nanowire thermal and electrical measurements on In2-x GaxO3(ZnO)n reveal a simultaneous improvement in all contributing factors to the thermoelectric figure of merit, giving an order of magnitude enhancement over similar bulk materials at room temperature. This is the first report of enhancement of all three thermoelectric parameters (Seebeck coefficient, electrical conductivity, and thermal resistivity) for a nanowire system. Photoelectrochemical water splitting is another exciting renewable energy application that can benefit from the high surface area of nanomaterials. Recently, (Ga1-xZnx)(N1-xOx) has gained widespread attention as a high efficiency material for visible-light-driven H2 and O2 generation. To improve the crystallinity of the material and reduce charge recombination (Ga1-xZnx)(N 1-xOx) nanotubes were synthesized by epitaxial coating of GaN onto ZnO nanowires. The nanotubes were single-crystalline, solid solutions of GaN and ZnO with ZnO compositions up to 10% and bandgaps as low as 2.6 eV. Incorporation of In into these nanotubes pushed the absorption even further into the visible. After decoration with Rh2-yCryO3 nanoparticle cocatalysts, (Ga1-xZnx)(N1-xOx) nanotubes spontaneously generated H2 in aqueous solutions under illumination. The photoanodic properties of these nanotubes are still under investigation. The significant reductions in thermal conductivity achieved using lead chalcogenide and In2-xGaxO3(ZnO) n nanowires highlight their use in thermoelectric power generation. The promise of 1-dimensional materials for energy conversion is further evident in the superior crystalline quality and high surface areas of the (Ga 1-xZnx)(N1-xOx) nanotubes. As research continues along these direction we move ever closer toward implementation of nanowires and nanotubes for clean, renewable, and more efficient energy use.

Ligand-surface interactions and surface oxidation of colloidal PbSe quantum dots revealed by thin-film positron annihilation methods

NASA Astrophysics Data System (ADS)

Shi, Wenqin; Eijt, Stephan W. H.; Suchand Sandeep, C. S.; Siebbeles, Laurens D. A.; Houtepen, Arjan J.; Kinge, Sachin; Brück, Ekkes; Barbiellini, Bernardo; Bansil, Arun

2016-02-01

Positron Two Dimensional Angular Correlation of Annihilation Radiation (2D-ACAR) measurements reveal modifications of the electronic structure and composition at the surfaces of PbSe quantum dots (QDs), deposited as thin films, produced by various ligands containing either oxygen or nitrogen atoms. In particular, the 2D-ACAR measurements on thin films of colloidal PbSe QDs capped with oleic acid ligands yield an increased intensity in the electron momentum density (EMD) at high momenta compared to PbSe quantum dots capped with oleylamine. Moreover, the EMD of PbSe QDs is strongly affected by the small ethylenediamine ligands, since these molecules lead to small distances between QDs and favor neck formation between near neighbor QDs, inducing electronic coupling between neighboring QDs. The high sensitivity to the presence of oxygen atoms at the surface can be also exploited to monitor the surface oxidation of PbSe QDs upon exposure to air. Our study clearly demonstrates that positron annihilation spectroscopy applied to thin films can probe surface transformations of colloidal semiconductor QDs embedded in functional layers.

Secondary-electron emission by 0.5-MeV/u H, He, and Li ions specularly reflected from a SnTe(001) surface: Possibility of the surface track potential reducing the secondary-electron yield at a semiconductor surface

NASA Astrophysics Data System (ADS)

Kimura, Kenji; Usui, Satoshi; Nakajima, Kaoru

2000-12-01

We have measured secondary-electron (SE) yield γ induced by 0.5 MeV/u H, He, and Li ions specularly reflected from a SnTe(001) surface. The position-dependent SE production rate is derived from the observed γ. The SE production rate normalized by the observed mean square charge of the reflected ions is almost independent of the atomic number of the projectile ion. This indicates that the surface track potential induced by the projectile ion is negligibly small to affect the SE emission at semiconductor surfaces probably due to rapid relaxation processes.

The influence of salivary contamination on shear bond strength of dentin adhesive systems.

PubMed

Park, Jeong-won; Lee, Kyung Chae

2004-01-01

This study evaluated the influence of salivary contamination during dentin bonding procedures on shear bond strength and investigated the effect of contaminant-removing treatments on the recovery of bond strength for two dentin bonding agents. One hundred and ten human molars were embedded in cylindrical molds with self-curing acrylic resin. The occlusal dentin surface was exposed by wet grinding with #800 silicon carbide abrasive paper. The teeth were divided into five groups for One-step (OS) (BISCO, Inc) and six groups for Clearfil SE Bond (SE) (Kuraray Co, Ltd, Osaka, Japan). For One-step, the grinding surface was treated with 32% phosphoric acid; BAC (BISCO Inc) and divided into five groups: OS control group (uncontaminated), OS I (salivary contamination, blot dried), OS II (salivary contamination, completely dried), OS III (salivary contamination, wash and blot dried) and OS IV (salivary contamination, re-etching for 10 seconds, wash and blot dried). For SE bond, the following surface treatments were done: SE control group (primer applied to the fresh dentin surface), SE I (after salivary contamination, primer applied), SE II (primer, salivary contamination, dried), SE III (primer, salivary contamination, wash and dried), SE IV (after procedure of SE II, re-application of primer) and SE V (after procedure of SE III, re-application of primer). Each bonding agent was applied and light cured for 10 seconds. Clearfil AP-X (Kuraray Co, Ltd) composite was packed into the Ultradent mount jig mold and light cured for 40 seconds. The bonded specimens were stored for 24 hours in a 37 degrees C waterbath. The shear bond strengths were measured using an Instron testing machine (Model 4202, Instron Corp). The data for each group were subjected to one-way ANOVA followed by the Newman-Keuls test to make comparisons among the groups. The results were as follows: In the One-step groups, the OS II group showed statistically significant lower shear bond strength than the OS control, I, III and IV (p<0.05). In the Clearfil SE Bond groups, the SE II and SE III groups had decreased shear bond strength compared with the control and SE I, SE IV and SE V groups (p<0.05). In conclusion, when using One-step total etch adhesive and when the etched surface is contaminated by saliva, blotting the surface and applying the primer can recover the bond strength. Complete drying of the salivary contaminated surface should be avoided. In the Clearfil SE Bond groups, the re-priming treatment (SE IV and SE V) resulted in the recovery of shear bond strength in the specimens contaminated after priming.

High-Resolution AES Mapping and TEM Study of Cu(In,Ga)Se2 Thin Film Growth: Preprint

DOE Office of Scientific and Technical Information (OSTI.GOV)

Perkins, C. L.; Yan, Y.; Jones, K.

2001-10-01

Presented at 2001 NCPV Program Review Meeting: TEM and high-resolution AES mapping data on CIGS samples. The chalcopyrite Cu(In,Ga)Se{sub 2} (CIGS) shows promise as an absorber layer in thin polycrystalline solar cells, however, details of the PVD growth of this complicated material remain in a developing stage. Previous workers have postulated the existence of a thin film of liquid Cu{sub x}Se on the growing CIGS film, and that this layer acts as a reservoir of copper as well as a layer in which rapid mass transport is possible. In this paper we present transmission electron microscopy (TEM) and high resolutionmore » Auger electron spectroscopy (AES) mapping data taken on samples that had their growth interrupted at a stage when Cu{sub x}Se was expected to be present. The AES maps show CIGS grains which are highly enriched in copper relative to the rest of the CIGS film, and that these same areas contain almost no indium, results consistent with the presence of CuxSe. Small-area diffraction analysis and energy dispersive spectroscopy (EDS) performed on these same samples independently confirm the presence of Cu{sub x}Se at the surface of growing CIGS films.« less

Enhanced electrical transport and thermoelectric properties in Ni doped Cu3SbSe4

NASA Astrophysics Data System (ADS)

Kumar, Aparabal; Dhama, P.; Das, Anish; Sarkar, Kalyan Jyoti; Banerji, P.

2018-05-01

In this study, we report the enhanced thermoelectric performance of Cu3SbSe4 by Ni doping at Cu site. Cu3-xNixSbSe4 (x = 0, 0.01, 0.03, 0.05) were prepared by melt growth, ball milling followed by spark plasma sintering. Structural characterization, phase analysis and surface morphology were carried out using X-ray diffraction, field emission scanning electron microscopy and energy dispersive X-ray spectroscopy. Electrical and thermal properties of all the samples were investigated in the temperature range 300 - 650 K. Decrease in electrical resistivity with Ni doping due to increase in carrier concentration with enhanced Seebeck coefficient via increase in density of state near the Fermi level gives a remarkably high power factor. At the same time, thermal conductivity was found to decrease due to increased carrier-phonon scattering and acoustic phonon scattering. Consequently, a remarkable enhancement in the thermoelectric figure of merit (ZT˜ 0.65) of Cu3-xNixSbSe4 was achieved for x = 0.01 sample. Thus, Ni doping is an effective approach to improve the efficiency of Cu3SbSe4.

Influence of Ge addition on the optical properties of As40Se50Ge10 thin film probed by spectroscopy techniques

NASA Astrophysics Data System (ADS)

Naik, Ramakanta; Pradhan, Jagnaseni; Sripan, Chinnaiyah; Ganesan, R.

2018-05-01

The thin films of As40Se60 and As40Se50Ge10 were prepared on glass substrates by thermal evaporation method with thickness 1000 nm. The prepared films were amorphous in nature which was confirmed through X-ray diffraction. The chemical composition and the surface picture were obtained from energy dispersive X-ray analysis and Scanning Electron Microscopy analysis. The transmission data of the two films were collected in the wavelength range 400-1000 nm. The transmission percentage is found to be decreased whereas the absorption coefficient is increased with the Ge addition. The addition of Ge into As40Se60 is found to increase the refractive index and the extinction coefficient of As40Se50Ge10 thin film. The decrease in optical band gap is explained on the basis of increase in density of states and disorderness due to Ge addition. The optical absorption in the film is due to allowed indirect transition, and the homopolar bond density is increased with Ge addition. The Raman shift observed in the two films clearly supports the optical changes due to Ge addition.

Electronic structure of germanium selenide investigated using ultra-violet photo-electron spectroscopy

NASA Astrophysics Data System (ADS)

Mishra, P.; Lohani, H.; Kundu, A. K.; Patel, R.; Solanki, G. K.; Menon, Krishnakumar S. R.; Sekhar, B. R.

2015-07-01

The valence band electronic structure of GeSe single crystals has been investigated using angle resolved photoemission spectroscopy (ARPES) and x-ray photoelectron spectroscopy. The experimentally observed bands from ARPES, match qualitatively with our LDA-based band structure calculations along the Γ-Z, Γ-Y and Γ-T symmetry directions. The valence band maximum occurs nearly midway along the Γ-Z direction, at a binding energy of -0.5 eV, substantiating the indirect band gap of GeSe. Non-dispersive features associated with surface states and indirect transitions have been observed. The difference in hybridization of Se and Ge 4p orbitals leads to the variation of dispersion along the three symmetry directions. The predominance of the Se 4pz orbitals, evidenced from theoretical calculations, may be the cause for highly dispersive bands along the Γ-T direction. Detailed electronic structure analysis reveals the significance of the cation-anion 4p orbitals hybridization in the valence band dispersion of IV-VI semiconductors. This is the first comprehensive report of the electronic structure of a GeSe single crystal using ARPES in conjugation with theoretical band structure analysis.

STM study on the surface structures and defects of SnSe

NASA Astrophysics Data System (ADS)

Kim, Jungdae; Duvjir, Ganbat; Ly, Trinh Thi; Min, Taewon; Kim, Taehoon; Kim, Sang Hwa; Duong, Anh-Tuan; Rhim, S. H.; Cho, Sunglae; Lee, Jaekwang

Tin selenide (SnSe) is a IV-VI semiconductor with a band gap of 1.0 eV, and also one of layered chalcogenide materials (LCMs) where each layer is coupled by weak van der Waals interactions. SnSe has been widely studied due to its many potential applications that take advantage of its excellent thermoelectric, photovoltaic, and optoelectronic properties. However, experimental investigations into the microscopic structure of SnSe remain largely unexplored. The atomic and electronic structures of SnSe surfaces are studied by a home-built low temperature scanning tunneling microscope (STM). The cleaved surface of SnSe is comprised of covalently bonded Se and Sn atoms in zigzag patterns. However, rectangular periodicity was observed in the atomic images of SnSe surfaces for filled and empty state probing. Detailed atomic structures are analyzed by density functional theory (DFT) calculations, indicating that the bright extrusions of both filled and empty state images are mostly located at the positions of Sn atoms. We also report the origin of p-type behavior in SnSe by investigating three dominant intrinsic defects (Sn, Se, and Se-Sn-Se vacancies) using STM and DFT calculations. This work was supported by the National Research Foundation of Korea (NRF-2015R1D1A1A01057271, NRF-2009-0093818, and NRF-2014R1A4A1071686).

Aqueous solution epitaxy of CdS layers on CuInSe 2

NASA Astrophysics Data System (ADS)

Furlong, M. J.; Froment, M.; Bernard, M. C.; Cortès, R.; Tiwari, A. N.; Krejci, M.; Zogg, H.; Lincot, D.

1998-09-01

Epitaxial CdS thin films have been deposited from an aqueous ammonia solution containing cadmium ions and thiourea as precursors on single crystalline CuInSe 2 films prepared by MBE on Si(1 1 1) and GaAs(1 0 0) substrates. The structure and quality of the films were investigated by RHEED, glancing angle XRD and HRTEM in cross-section. The films are cubic on (1 0 0) substrates, and mixed cubic and hexagonal on (1 1 1) substrates due to the presence of stacking faults parallel to the substrate. The growth is under surface kinetic control with an activation energy of 85 kJ mol -1. Epitaxy improves with increasing temperature and an epitaxial transition temperature at approx. 60°C is demonstrated in the selected experimental conditions. The epitaxy is very sensitive to the preparation of the surface. Beneficial effects of in situ or ex situ chemical etching are found. Similarities between aqueous solution and vapor-phase chemical depositions are pointed out.

Optical and structural properties of indium doped bismuth selenide thin films

NASA Astrophysics Data System (ADS)

Pavagadhi, Himanshu; Vyas, S. M.; Patel, Piyush; Patel, Vimal; Patel, Jaydev; Jani, M. P.

2015-08-01

In: Bi2Se3 crystals were grown by Bridgman method at a growth velocity of 0.5cm/h with temperature gradient of 650 C/cm in our laboratory. The thin films of In:Bi2se3 were grown on amorphous substrate (glass) at a room temperature under a pressure of 10-4Pa by thermal evaporation technique. Thin film were deposited at various thicknesses and optical absorption spectrum of such thin films, obtain in wave no. range 300 to 2600 cm-1. The optical energy gap calculated from this data were found to be inverse function of square of thickness, particularly for thickness about 1800 Å or less. This dependence is explained in terms of quantum size effect. For thicker films, the bandgap is found to be independent of film thickness. For the surface stud of the as grown thin film by using AFM, which shows continuous film with some step height and surface roughness found in terms of few nm and particle size varies with respect to thickness.

Probing and controlling terahertz-driven structural dynamics with surface sensitivity

DOE PAGES

Bowlan, Pamela Renee; Bowlan, J.; Trugman, S. A.; ...

2017-03-17

Intense, single-cycle terahertz (THz) pulses are powerful tools to understand and control material properties through low-energy resonances, such as phonons. Combining this with optical second harmonic generation (SHG) makes it possible to observe the resulting ultrafast structural changes with surface sensitivity. This makes SHG an ideal method to probe phonon dynamics in topological insulators (TI), materials with unique surface transport properties. Here, we resonantly excite a phonon mode in the TI Bi 2Se 3with THz pulses and use SHG to separate the resulting symmetry changes at the surface from the bulk. Furthermore, we coherently control the lattice vibrations with amore » pair of THz pulses. Lastly, our work demonstrates a versatile, table-top tool to probe and control phonon dynamics in a range of systems, particularly at surfaces and interfaces.« less

SRS in the single molecule limit (Conference Presentation)

NASA Astrophysics Data System (ADS)

Potma, Eric O.; Crampton, Kevin T.; Fast, Alexander; Apkarian, Vartkess A.

2017-02-01

We present combined surface-enhanced stimulated Raman scattering (SE-SRS) and surface-enhanced coherent anti-Stokes Raman scattering (SE-CARS) measurements on individual plasmonic antennas dressed with bipyridyl-ethylene molecules. By carefully optimizing the conditions for performing SE-SRS experiments, we have obtained stable and reproducible molecular surface-enhanced SRS spectra from single nano-antennas. Using surface-enhanced Raman scattering (SERS) and transmission electron microscopy of the same antennas, we confirm that the observed SE-SRS signals originate from only one or a few molecules. We highlight the physics of surface enhancement in the context of coherent Raman scattering and derive sensitivity parameters under the relevant conditions. The implications of single molecule SRS measurements are discussed.

Sorption and reduction of selenite on chlorite surfaces in the presence of Fe(II) ions.

PubMed

Baik, Min Hoon; Lee, Seung Yeop; Jeong, Jongtae

2013-12-01

The sorption and reduction of selenite on chlorite surfaces in the presence of Fe(II) ions were investigated as a function of pH, Se(IV) concentration, and Fe(II) concentration under an anoxic condition. The sorption of Se(IV) onto chlorite surfaces followed the Langmuir isotherm regardless of the presence of Fe(II) ions in the solution. The Se(IV) sorption was observed to be very low at all pH values when the solution was Fe(II)-free or the concentration of Fe(II) ions was as low as 0.5 mg/L. However, the Se(IV) sorption was enhanced at a pH > 6.5 when the Fe(II) concentration was higher than 5 mg/L because of the increased sorption of Fe(II) onto the chlorite surfaces. XANES (X-ray absorption near edge structure) spectra of the Se K-edge showed that most of the sorbed Se(IV) was reduced to Se(0) by Fe(II) sorbed onto the chlorite surfaces, especially at pH > 9. The combined results of field-emission scanning electron microscopy (FE-SEM) and X-ray diffraction (XRD) also showed that elemental selenium and goethite were formed and precipitated on the chlorite surfaces during the sorption of selenite. Consequently it can be concluded that Se(IV) can be reduced to Se(0) in the presence of Fe(II) ions by the surface catalytic oxidation of Fe(II) into Fe(III) and the formation of goethite at neutral and particularly alkaline conditions. Thus the mobility of selenite in groundwater is expected to be reduced by the presence of a relatively higher concentration of Fe(II) in subsurface environments. Copyright © 2013 Elsevier Ltd. All rights reserved.

Hydrothermal assisted growth of CdSe nanoparticles and study on its dielectric properties

NASA Astrophysics Data System (ADS)

Jamble, Shweta N.; Ghoderao, Karuna P.; Kale, Rohidas B.

2017-11-01

In this work, we have synthesized cadmium selenide (CdSe) nanoparticles by using cadmium chloride (CdCl2) as cadmium ion and sodium selenosulfate (Na2SeSO3) as selenium ion sources through a simple, convenient and cost-effective hydrothermal route at 180 °C temperature for 24 h. Aqueous ammonia was employed as a complex reagent to adjust the pH of the solution. Structural analysis of the obtained product was carried out by using x-ray diffractometer, which revealed that the final product has a cubic structure of CdSe with average crystallite size 13.15 nm. The cauliflower-like CdSe nanostructures were confirmed from the scanning electron microscopy and high-resolution transmission electron microscopy. EDS analysis indicates that the obtained product has a good elemental stoichiometric ratio. The electron diffraction pattern reveals the polycrystalline nature of CdSe. From UV-visible absorption spectral analysis, the optical energy bandgap of CdSe nanoparticles was found to be 1.90 eV. XPS spectra presented Cd 3d3/2, Cd 3d5/2 and Se 3d3/2 peaks at 411.04, 404.29 and 53.52 eV respectively. The CdSe nanoparticles exhibit photoluminescence with two distinct emission bands at 632 nm and 720 nm. FTIR study was used towards the understanding of the formation mechanism and bonding on the surface of the resulting nanoparticles. The dielectric properties of a pelletized sample of CdSe nanoparticles were carried out at room temperature.

DOE Office of Scientific and Technical Information (OSTI.GOV)

Matetskiy, A. V., E-mail: mateckij@iacp.dvo.ru; Kibirev, I. A.; Saranin, A. A.

The formation, structure and electronic properties of SnSe{sub 2}–Bi{sub 2}Se{sub 3} van der Waals heterostructures were studied. Both heterostructures, SnSe{sub 2} on Bi{sub 2}Se{sub 3} and Bi{sub 2}Se{sub 3} on SnSe{sub 2}, were grown epitaxially with high crystallinity and sharp interfaces. Their electron band structures are of trivial and topological insulators, respectively. The Dirac surface states of Bi{sub 2}Se{sub 3} survive under the SnSe{sub 2} overlayer. One triple layer of SnSe{sub 2} was found to be an efficient spacer for separating a Bi{sub 2}Se{sub 3} topological-insulator slab into two and creating the corresponding topological surface states.

Emergent Momentum-Space Skyrmion Texture on the Surface of Topological Insulators

NASA Astrophysics Data System (ADS)

Mohanta, Narayan; Kampf, Arno P.; Kopp, Thilo

The quantum anomalous Hall effect has been theoretically predicted and experimentally verified in magnetic topological insulators. In addition, the surface states of these materials exhibit a hedgehog-like ``spin'' texture in momentum space. Here, we apply the previously formulated low-energy model for Bi2Se3, a parent compound for magnetic topological insulators, to a slab geometry in which an exchange field acts only within one of the surface layers. In this sample set up, the hedgehog transforms into a skyrmion texture beyond a critical exchange field. This critical field marks a transition between two topologically distinct phases. The topological phase transition takes place without energy gap closing at the Fermi level and leaves the transverse Hall conductance unchanged and quantized to e2 / 2 h . The momentum-space skyrmion texture persists in a finite field range. It may find its realization in hybrid heterostructures with an interface between a three-dimensional topological insulator and a ferromagnetic insulator. The work was supported by the Deutsche Forschungsgemeinschaft through TRR 80.

Growth and quantum transport properties of vertical Bi2Se3 nanoplate films on Si substrates.

PubMed

Li, Mingze; Wang, Zhenhua; Yang, Liang; Pan, Desheng; Li, Da; Gao, Xuan P A; Zhang, Zhidong

2018-08-03

Controlling the growth direction (planar versus vertical) and surface-to-bulk ratio can lead to lots of unique properties for two-dimensional layered materials. We report a simple method to fabricate continuous films of vertical Bi 2 Se 3 nanoplates on Si substrate and investigate the quantum transport properties of such films. In contrast to (001) oriented planar Bi 2 Se 3 nanoplate film, vertical Bi 2 Se 3 nanoplate films are enclosed by (015) facets, which possess high surface-to-bulk ratio that can enhance the quantum transport property of topological surface states. And by controlling the compactness of vertical Bi 2 Se 3 nanoplates, we realized an effective tuning of the weak antilocalization effect from topological surface states in Bi 2 Se 3 films. Our work paves a way for exploring the unique transport properties of this unconventional structure topological insulator film.

Studies of Nano-structured Se77Sb23- x Ge x Thin Films Prepared by Physical Vapor Condensation Technique

NASA Astrophysics Data System (ADS)

Alvi, M. A.

2017-02-01

Bulk Se77Sb23- x Ge x material with x = 4 and 12 was prepared by employing a melt quench technique. Its amorphous as well as glassy nature was confirmed by x-ray diffraction analysis and nonisothermal differential scanning calorimetry measurements. The physical vapor condensation technique was applied to prepare nanostructured thin films of Se77Sb23- x Ge x material. The surface morphology of the films was examined using field-emission scanning electron microscopy, revealing average particle size between 20 nm and 50 nm. Systematic investigation of optical absorption data indicated that the optical transition was indirect in nature. The dark conductivity (dc conductivity) of nano-structured Se77Sb23- x Ge x thin films was also investigated at temperatures from 313 K to 463 K, revealing that it tended to increase with increasing temperature. Analyses of our experimental data also indicate that the conduction is due to thermally supported tunneling of charge carriers in confined states close to the band edges. The calculated values of activation energy agree well with the optical bandgap.

DOE Office of Scientific and Technical Information (OSTI.GOV)

Gao, Bing; Shen, Chao; Zhang, Mengya

Green synthesis of CdSe quantum dots for application in the quantum-dots-sensitized solar cells (QDSCs) is investigated in this work. The CdSe QDs were prepared with glycerol as the solvent, with sharp emission peak, full width at half maximum around 30 nm, and absorption peak from 475 nm to 510 nm. The reaction is environmental friendly and energy saving. What's more, the green synthesized CdSe QDs are coherence to the maximum remittance region of the solar spectrum and suitable as sensitizers to assemble onto TiO{sub 2} electrodes for cell devices application. What's more, the dynamic procedure of the carriers' excitation, transportation, and recombination inmore » the QDSCs are discussed. Because the recombination of the electrons from the conduction band of TiO{sub 2}'s to the electrolyte affects the efficiency of the solar cells greatly, 3-Mercaptopropionic acid capped water-dispersible QDs were used to cover the surface of TiO{sub 2}. The resulting green synthesized CdSe QDSCs with Cu{sub 2}S as the electrode show a photovoltaic performance with a conversion efficiency of 3.39%.« less

Surface State-Dominated Photoconduction and THz Generation in Topological Bi2Te2Se Nanowires

PubMed Central

2017-01-01

Topological insulators constitute a fascinating class of quantum materials with nontrivial, gapless states on the surface and insulating bulk states. By revealing the optoelectronic dynamics in the whole range from femto- to microseconds, we demonstrate that the long surface lifetime of Bi2Te2Se nanowires allows us to access the surface states by a pulsed photoconduction scheme and that there is a prevailing bolometric response of the surface states. The interplay of the surface and bulk states dynamics on the different time scales gives rise to a surprising physical property of Bi2Te2Se nanowires: their pulsed photoconductance changes polarity as a function of laser power. Moreover, we show that single Bi2Te2Se nanowires can be used as THz generators for on-chip high-frequency circuits at room temperature. Our results open the avenue for single Bi2Te2Se nanowires as active modules in optoelectronic high-frequency and THz circuits. PMID:28081604

Optical properties of ultrathin CIGS films studied by spectroscopic ellipsometry assisted by chemical engineering

NASA Astrophysics Data System (ADS)

Loubat, Anaïs; Eypert, Céline; Mollica, Fabien; Bouttemy, Muriel; Naghavi, Negar; Lincot, Daniel; Etcheberry, Arnaud

2017-11-01

CIGS (Cu(In1-x,Gax)Se2) based devices are very efficient for photovoltaic conversion. A non-destructive optical study of CIGS is an important challenge as for evaluation of the material quality, and for device modeling. Spectroscopic Ellipsometry (SE) is well adapted for a quantitative characterization only if the handicaps of the roughness limitation, the oxidized surface, or the compositional gradient are minimized. For this SE study, ungraded and thin CIGS samples are prepared with GGI (x) ratio (=[Ga]/([Ga] + [In])) ranging from 0.15 to 0.60. Thanks to chemical engineering based on acidic bromine solution etching and/or HCl de-oxidation, the SE experiments are performed on flattened surfaces, and also, on as grown de-oxidized samples. Using assumptions based on XPS, AFM and SEM complementary characterizations, we give proof of oxide free flattening surfaces and chemical homogeneity in depth. Using these observations, the SE data are modeled on the basis of a three layer model using an Adachi/Tauc-Lorentz formula for the CIGS dispersion. The optical gap values are determined in good agreement with the x ratio measured by the other characterization techniques. SE is able to well estimate the thickness and roughness variations on each sample. Furthermore, the CIGS optical constant extracted on such reference flat surfaces are then applied to the as grown-de-oxidized surfaces, enabling to describe the SE data obtained on rougher surfaces. A complete consistency of the proposed model is shown as well as the capability of SE to be sensitive to the chemistry of the surface.

Prediction of weak and strong topological insulators in layered semiconductors.

NASA Astrophysics Data System (ADS)

Felser, Claudia

2013-03-01

We investigate a new class of ternary materials such as LiAuSe and KHgSb with a honeycomb structure in Au-Se and Hg-Sb layers. We demonstrate the band inversion in these materials similar to HgTe, which is a strong precondition for existence of the topological surface states. In contrast with graphene, these materials exhibit strong spin-orbit coupling and a small direct band gap at the point. Since these materials are centrosymmetric, it is straightforward to determine the parity of their wave functions, and hence their topological character. Surprisingly, the compound with strong spin-orbit coupling (KHgSb) is trivial, whereas LiAuSe is found to be a topological insulator. However KHgSb is a weak topological insulators in case of an odd number of layers in the primitive unit cell. Here, the single-layered KHgSb shows a large bulk energy gap of 0.24 eV. Its side surface hosts metallic surface states, forming two anisotropic Dirac cones. Although the stacking of even-layered structures leads to trivial insulators, the structures can host a quantum spin Hall layer with a large bulk gap, if an additional single layer exists as a stacking fault in the crystal. The reported honeycomb compounds can serve as prototypes to aid in the finding of new weak topological insulators in layered small-gap semiconductors. In collaboration with Binghai Yan, Lukas Müchler, Hai-Jun Zhang, Shou-Cheng Zhang and Jürgen Kübler.

Hybrid optical materials of plasmon-coupled CdSe/ZnS coreshells for photonic applications

PubMed Central

Seo, Jaetae; Fudala, Rafal; Kim, Wan-Joong; Rich, Ryan; Tabibi, Bagher; Cho, Hyoyeong; Gryczynski, Zygmunt; Gryczynski, Ignacy; Yu, William

2013-01-01

A hybrid optical nanostructure of plasmon-coupled SQDs was developed for photonic applications. The coupling distances between the mono-layers of Au nanoparticles with a surface concentration of ~9.18 × 10−4 nm−2 and CdSe/ZnS SQDs with that of ~3.7 × 10−3 nm−2 were controlled by PMMA plasma etching. Time-resolved spectroscopy of plasmon-coupled SQDs revealed a strong shortening of the longest lifetime and ~9-fold PL enhancement. Polarization-resolved PL spectroscopy displayed linear polarization and depolarization at near- and far-field plasmon-coupling, respectively. The physical origin of PL enhancement could be attributable to both the large local field enhancement and the fast resonant energy transfer. PMID:23457661

When exercise does not pay: Counterproductive effects of impending exercise on energy intake among restrained eaters.

PubMed

Sim, Aaron Y; Lee, Li Ling; Cheon, Bobby K

2018-04-01

Evidence suggests people may overestimate the effectiveness of future positive behaviour, leading to counterproductive behaviours in the present. Applied to weight-management, we hypothesize that inaccurate expectations about impending exercise may impede weight management by promoting overconsumption prior to exercise. This study aimed to determine how expectations about impending exercise and its potential ability to expend energy may influence i) energy intake before exercise and ii) overall energy balance (energy intake minus energy expended via exercise). Using a randomised, counterbalanced design, 21 inactive, overweight males, following a baseline session, completed two experimental trials: i) ad-libitum snack meal (potato-crisps) followed by an exercise session (SE) and ii) ad-libitum snack meal only (SO). There was no main effect of condition (SE vs. SO) on ad-libitum snack intake (p = .917). However, after accounting for dietary restraint (covariate), a difference in snack intake between SE and SO was revealed (p = .050). Specifically, participants who scored higher in dietary restraint consumed more in the SE (vs. SO) session (162 ± 359 kcal more) compared with participants who scored lower in dietary restraint (89 ± 135 kcal less). Among restrained eaters, the relative (net) energy consumed after accounting for energy expended from exercise in SE was not different from the energy consumed in the SO condition, suggesting that energy expended via exercise in SE does not appear to negate extra energy consumed in this condition compared with SO. Of interest, desire to eat and prospective food consumption ratings at the start of the trial were greater (p ≤ .029) in SE compared with SO. Findings suggest that restrained-eaters are at risk of adopting compensatory eating behaviour that may impede negative energy balance typically resulting from exercise (i.e. expending insufficient energy to negate compensatory energy intake). Copyright © 2017 Elsevier Ltd. All rights reserved.

Iowa Developed Energy Activity Sampler (IDEAS), Grades 7-12: Industrial Arts.

ERIC Educational Resources Information Center

Simonis, Doris G.

Described is the Industrial Arts component of the Iowa Developed Energy Activity Sampler (IDEAS), a multidisciplinary energy education program designed for infusion into the curriculum of grades 7-12. Also included in the program are activity sets for Home Economics (SE 034 678), Language Arts (SE 034 680), Mathematics (SE 034 681), Science (SE…

Fabrication of CIGS Films by Electrodeposition Method for Photovoltaic Cells

NASA Astrophysics Data System (ADS)

Lee, Hyunju; Yoon, Hyukjoo; Ji, Changwook; Lee, Dongyun; Lee, Jae-Ho; Yun, Jae-Ho; Kim, Yangdo

2012-12-01

Cu(InGa)Se2 (CIGS) thin films were fabricated by electrochemical deposition in a single bath containing Cu, In, Ga, and Se ions. The electrolyte was prepared by dissolving CuCl2, InCl3, GaCl3, H2SeO3, and LiCl in deionized water. The potentiostatic deposition process was achieved by applying a voltage ranging from -0.5 V to -0.8 V versus Ag/AgCl. The effects of different chemical bath concentrations on the film composition and morphology were investigated. Stoichiometric CIGS film composition could be achieved by controlling the chemical compositions of the bath and the voltage. Gelatin was added to the solution to improve the surface and microstructures of the CIGS film. The as-deposited films were annealed at 500°C in Ar atmosphere for crystallization. The structural, morphological, and compositional properties of the CIGS thin films before and after annealing were examined by x-ray diffraction, scanning electron microscopy, and energy-dispersive spectroscopy. This study showed that the composition of the CIGS films is dependent on the bath concentration, whereas the applied potential had relatively less effect on the CIGS film composition. In addition, the use of gelatin helped in the fabrication of crack-free CIGS thin films with greatly improved surface morphology.

Theory versus experiment for a family of single-layer compounds with a similar atomic arrangement: (Tl,X )/Si(111 )√{3 }×√{3 }(X =Pb,Sn,Bi,Sb,Te,Se)

NASA Astrophysics Data System (ADS)

Matetskiy, A. V.; Kibirev, I. A.; Mihalyuk, A. N.; Eremeev, S. V.; Gruznev, D. V.; Bondarenko, L. V.; Tupchaya, A. Y.; Zotov, A. V.; Saranin, A. A.

2017-08-01

Two-dimensional compounds made of one monolayer of Tl and one-third monolayer of Pb, Bi, Te, or Se (but not of Sn or Sb) on Si(111) have been found to have a similar atomic arrangement which can be visualized as a √{3 }×√{3 } -periodic honeycomb network of chained Tl trimers with atoms of the second adsorbate occupying the centers of the honeycomb units. Structural and electronic properties of the compounds have been examined in detail theoretically using density functional theory (DFT) calculations and experimentally using low-energy electron diffraction (LEED), scanning tunneling microscopy (STM), and angle-resolved photoelectron spectroscopy (ARPES) observations. It has been found that though structural parameters of the compounds are very similar for all species, the only common feature of their band structure is a considerable spin-splitting of the surface-state bands, while other basic electronic properties vary greatly with a change of species. The Tl-Pb compound is strongly metallic with two metallic surface-state bands; the Tl-Bi compound is also metallic but with a single metallic band; the Tl-Te and Tl-Se compounds appear to be insulators.

Superconducting proximity effect in a topological insulator using Fe(Te, Se)

NASA Astrophysics Data System (ADS)

Zhao, He; Rachmilowitz, Bryan; Ren, Zheng; Han, Ruobin; Schneeloch, J.; Zhong, Ruidan; Gu, Genda; Wang, Ziqiang; Zeljkovic, Ilija

2018-06-01

Interest in the superconducting proximity effect has recently been reignited by theoretical predictions that it could be used to achieve topological superconductivity. Low-Tc superconductors have predominantly been used in this effort, but small energy scales of ˜1 meV have hindered the characterization of the emergent electronic phase, limiting it to extremely low temperatures. In this work, we use molecular beam epitaxy to grow topological insulator B i2T e3 in a range of thicknesses on top of a high-Tc superconductor Fe(Te,Se). Using scanning tunneling microscopy and spectroscopy, we detect Δind as high as ˜3.5 meV, which is the largest reported gap induced by proximity to an s -wave superconductor to date. We find that Δind decays with B i2T e3 thickness, but remains finite even after the topological surface states have been formed. Finally, by imaging the scattering and interference of surface state electrons, we provide a microscopic visualization of the fully gapped B i2T e3 surface state due to Cooper pairing. Our results establish Fe-based high-Tc superconductors as a promising new platform for realizing high-Tc topological superconductivity.

Experimental indication for band gap widening of chalcopyrite solar cell absorbers after potassium fluoride treatment

NASA Astrophysics Data System (ADS)

Pistor, P.; Greiner, D.; Kaufmann, C. A.; Brunken, S.; Gorgoi, M.; Steigert, A.; Calvet, W.; Lauermann, I.; Klenk, R.; Unold, T.; Lux-Steiner, M.-C.

2014-08-01

The implementation of potassium fluoride treatments as a doping and surface modification procedure in chalcopyrite absorber preparation has recently gained much interest since it led to new record efficiencies for this kind of solar cells. In the present work, Cu(In,Ga)Se2 absorbers have been evaporated on alkali containing Mo/soda-lime glass substrates. We report on compositional and electronic changes of the Cu(In,Ga)Se2 absorber surface as a result of a post deposition treatment with KF (KF PDT). In particular, by comparing standard X-ray photoelectron spectroscopy and synchrotron-based hard X-ray photoelectron spectroscopy (HAXPES), we are able to confirm a strong Cu depletion in the absorbers after the KF PDT which is limited to the very near surface region. As a result of the Cu depletion, we find a change of the valence band structure and a shift of the valence band onset by approximately 0.4 eV to lower binding energies which is tentatively explained by a band gap widening as expected for Cu deficient compounds. The KF PDT increased the open circuit voltage by 60-70 mV compared to the untreated absorbers, while the fill factor deteriorated.

Nickel: The time-reversal symmetry conserving partner of iron on a chalcogenide topological insulator

NASA Astrophysics Data System (ADS)

Vondráček, M.; Cornils, L.; Minár, J.; Warmuth, J.; Michiardi, M.; Piamonteze, C.; Barreto, L.; Miwa, J. A.; Bianchi, M.; Hofmann, Ph.; Zhou, L.; Kamlapure, A.; Khajetoorians, A. A.; Wiesendanger, R.; Mi, J.-L.; Iversen, B.-B.; Mankovsky, S.; Borek, St.; Ebert, H.; Schüler, M.; Wehling, T.; Wiebe, J.; Honolka, J.

2016-10-01

We report on the quenching of single Ni adatom moments on Te-terminated Bi2Te2Se and Bi2Te3 topological insulator surfaces. The effect is noted as a missing x-ray magnetic circular dichroism for resonant L3 ,2 transitions into partially filled Ni 3 d states of theory-derived occupancy nd=9.2 . On the basis of a comparative study of Ni and Fe using scanning tunneling microscopy and ab initio calculations, we are able to relate the element specific moment formation to a local Stoner criterion. Our theory shows that while Fe adatoms form large spin moments of ms=2.54 μB with out-of-plane anisotropy due to a sufficiently large density of states at the Fermi energy, Ni remains well below an effective Stoner threshold for local moment formation. With the Fermi level remaining in the bulk band gap after adatom deposition, nonmagnetic Ni and preferentially out-of-plane oriented magnetic Fe with similar structural properties on Bi2Te2Se surfaces constitute a perfect platform to study the off-on effects of time-reversal symmetry breaking on topological surface states.

Investigating the Effect of Nanoscale Changes on the Chemistry and Energetics of Nanocrystals with a Novel Photoemission Spectroscopy Methodology

NASA Astrophysics Data System (ADS)

Liao, Michael W.

This dissertation explores the effect of nanometer-scale changes in structure on the energetics of photocatalytic and photovoltaic materials. Of particular interest are semiconductor nanocrystals (NCs), which have interesting chemical properties that lead to novel structures and applications. Chief among these properties are quantum confinement and the high surface area-to-volume ratio, which allow for chemical tuning of the energetics and structure of NCs. This tunable energetic landscape has led to increasing application of NCs in various areas of research, including solar energy conversion, light-emitting diode technologies, and photocatalysis. However, spectroscopic methods to determine the energetics of NCs have not been well developed, due to chemical complexities of relevant NCs such as polydispersity, capping ligand effects, core-shell structures, and other chemical modifications. In this work, we demonstrate and expand the utility of photoelectron spectroscopy (PES) to probe the energetics of NCs by considering the physical processes that lead to background and secondary photoemission to enhance photoemission from the sample of interest. A new methodology for the interpretation of UP spectra was devised in order to emphasize the minute changes to the UP spectra line shape that arise from nanoscopic changes to the NCs. We applied various established subtractions that correct for photon source satellites, secondary photoelectrons, and substrate photoemission. We then investigated the effect of ligand surface coverage on the surface chemistry and density of states at the top of valence band (VB). We systematically removed ligands by increasing numbers of purification steps for two diameters of NCs and found that doing so increased photoemission density at the top of the VB, which is due to undercoordinated surface atoms. Deeper VB structure was also altered, possibly due to reorganization of the atoms in the NC. Using the new UPS interpretation methodology, we examined the evolution of the valence band energy (EVB) of CdSe NCs as it was modified from spherical NC to rod to Au-NP tipped nanorod (NR). We also employed potential-modulated attenuated total reflectance spectroscopy (PM-ATR) to probe the conduction band energy (ECB) of the series. The EVB decreased with each modification, which is predicted with a band-bending model. This trend was also observed in the ECB, as revealed by spectroelectrochemistry, along with the appearance of new metal-semiconductor states in the band gap. UPS was finally used to investigate the even more complex Pt-NP tipped CdSe CdS core shell NR heterostructure. The addition of the CdS shell decreases the EVB relative to CdSe, as expected from common cation II-VI compounds. The Pt-NC increases the EVB, which, like the Au-CdSe NR, is predicted by employing a band-bending model. XPS revealed that PtSx-like chemical states were formed near the CdS-Pt interface. These experiments, along with the improved UP spectra interpretation methodology, demonstrate the wealth of information regarding surface chemistry and energetics that can be obtained with PES which can be applied to not only NCs, but also to metal oxide or molecular thin films.

Dipole strength in 80Se below the neutron-separation energy for the nuclear transmutation of 79Se

NASA Astrophysics Data System (ADS)

Makinaga, Ayano; Massarczyk, Ralph; Beard, Mary; Schwengner, Ronald; Otsu, Hideaki; Müller, Stefan; Röder, Marko; Schmidt, Konrad; Wagner, Andreas

2017-09-01

The γ-ray strength function (γSF) in 80Se is an important parameter to estimate the neutron-capture cross section of 79Se which is one of the long-lived fission products (LLFPs). Until now, the γSF method was applied for 80Se only above the neutron-separation energy (Sn) and the evaluated 79Se(n,γ) cross section has an instability caused by the GSF below Sn. We studied the dipole-strength distribution of 80Se in a photon-scattering experiment using bremsstrahlung produced by an electron beam of an energy of 11.5 MeV at the linear accelerator ELBE at HZDR. The present photoabsorption cross section of 80Se was combined with results of (γ,n) experiments and are compared with predictions usinmg the TALYS code. We also estimated the 79Se(n,γ) cross sections and compare them with TALYS predictionms and earlier work by other groups.

Bifunctional bamboo-like CoSe2 arrays for high-performance asymmetric supercapacitor and electrocatalytic oxygen evolution.

PubMed

Chen, Tian; Li, Songzhan; Gui, Pengbin; Wen, Jian; Fu, Xuemei; Fang, Guojia

2018-05-18

Bifunctional bamboo-like CoSe 2 arrays are synthesized by thermal annealing of Co(CO 3 ) 0.5 OH grown on carbon cloth in Se atmosphere. The CoSe 2 arrays obtained have excellent electrical conductivity, larger electrochemical active surface areas, and can directly serve as a binder-free electrode for supercapacitors and the oxygen evolution reaction (OER). When tested as a supercapacitor electrode, the CoSe 2 delivers a higher specific capacitance (544.6 F g -1 at current density of 1 mA cm -2 ) compared with CoO (308.2 F g -1 ) or Co 3 O 4 (201.4 F g -1 ). In addition, the CoSe 2 electrode possesses excellent cycling stability. An asymmetric supercapacitor (ASC) is also assembled based on bamboo-like CoSe 2 as a positive electrode and active carbon as a negative electrode in a 3.0 M KOH aqueous electrolyte. Owing to the unique stucture and good electrochemical performance of bamboo-like CoSe 2 , the as-assembled ACS can achieve a maximum operating voltage window of 1.7 V, a high energy density of 20.2 Wh kg -1 at a power density of 144.1 W kg -1 , and an outstanding cyclic stability. As the catalyst for the OER, the CoSe 2 exhibits a lower potential of 1.55 V (versus RHE) at current density of 10 mA cm -2 , a smaller Tafel slope of 62.5 mV dec -1 and an also outstanding stability.

Bifunctional bamboo-like CoSe2 arrays for high-performance asymmetric supercapacitor and electrocatalytic oxygen evolution

NASA Astrophysics Data System (ADS)

Chen, Tian; Li, Songzhan; Gui, Pengbin; Wen, Jian; Fu, Xuemei; Fang, Guojia

2018-05-01

Bifunctional bamboo-like CoSe2 arrays are synthesized by thermal annealing of Co(CO3)0.5OH grown on carbon cloth in Se atmosphere. The CoSe2 arrays obtained have excellent electrical conductivity, larger electrochemical active surface areas, and can directly serve as a binder-free electrode for supercapacitors and the oxygen evolution reaction (OER). When tested as a supercapacitor electrode, the CoSe2 delivers a higher specific capacitance (544.6 F g‑1 at current density of 1 mA cm‑2) compared with CoO (308.2 F g‑1) or Co3O4 (201.4 F g‑1). In addition, the CoSe2 electrode possesses excellent cycling stability. An asymmetric supercapacitor (ASC) is also assembled based on bamboo-like CoSe2 as a positive electrode and active carbon as a negative electrode in a 3.0 M KOH aqueous electrolyte. Owing to the unique stucture and good electrochemical performance of bamboo-like CoSe2, the as-assembled ACS can achieve a maximum operating voltage window of 1.7 V, a high energy density of 20.2 Wh kg‑1 at a power density of 144.1 W kg‑1, and an outstanding cyclic stability. As the catalyst for the OER, the CoSe2 exhibits a lower potential of 1.55 V (versus RHE) at current density of 10 mA cm‑2, a smaller Tafel slope of 62.5 mV dec‑1 and an also outstanding stability.

Surface and bulk effects of K in Cu 1-xK xIn 1-yGa ySe 2 solar cells

DOE PAGES

Muzzillo, Christopher P.; Anderson, Timothy J.

2017-12-29

Two strategies for enhancing photovoltaic (PV) performance in chalcopyrite solar cells were investigated: Cu 1-xK xIn 1-yGa ySe 2 absorbers with low K content (K/(K+Cu), or x ~ 0.07) distributed throughout the bulk, and CuIn 1-yGa ySe 2 absorbers with KIn 1-yGa ySe 2 grown on their surfaces. Distributing K throughout the bulk absorbers improved power conversion efficiency, open-circuit voltage (VOC) and fill factor (FF) for Ga/(Ga+In) of 0, 0.3 and 0.5. Surface KIn 1-yGa ySe 2 and bulk x ~ 0.07 Cu 1-xK xIn 1-yGa ySe 2 films with Ga/(Ga+In), or y of 0.3 and 0.5 also had improvedmore » efficiency, VOC, and FF, relative to CuIn 1-yGa ySe 2 baselines. On the other hand, y ~ 1 absorbers did not benefit from K introduction. Similar to Cu 1-xK xInSe 2, the formation of Cu 1-xK xGaSe 2 alloys was favored at low temperatures and high Na supply by the substrate, relative to the formation of mixed-phase CuGaSe 2 + KGaSe 2. KIn 1-yGa ySe 2 alloys were grown for the first time, as evidenced by X-ray diffraction and ultraviolet/visible spectroscopy. For all Ga/(Ga+In) compositions, the surface KIn 1-yGa ySe 2 absorbers had superior PV performance in buffered and buffer-free devices. However, the bulk x ~ 0.07 absorbers only outperformed the baselines in buffered devices. The data demonstrate that KIn 1-yGa ySe 2 passivates the surface of CuIn 1-yGa ySe 2 to increase efficiency, VOC, and FF, while bulk Cu 1-xK xIn 1-yGa ySe 2 absorbers with x ~ 0.07 enhance efficiency, VOC, and FF by some other mechanism.« less

Surface and bulk effects of K in Cu 1-xK xIn 1-yGa ySe 2 solar cells

DOE Office of Scientific and Technical Information (OSTI.GOV)

Muzzillo, Christopher P.; Anderson, Timothy J.

Two strategies for enhancing photovoltaic (PV) performance in chalcopyrite solar cells were investigated: Cu 1-xK xIn 1-yGa ySe 2 absorbers with low K content (K/(K+Cu), or x ~ 0.07) distributed throughout the bulk, and CuIn 1-yGa ySe 2 absorbers with KIn 1-yGa ySe 2 grown on their surfaces. Distributing K throughout the bulk absorbers improved power conversion efficiency, open-circuit voltage (VOC) and fill factor (FF) for Ga/(Ga+In) of 0, 0.3 and 0.5. Surface KIn 1-yGa ySe 2 and bulk x ~ 0.07 Cu 1-xK xIn 1-yGa ySe 2 films with Ga/(Ga+In), or y of 0.3 and 0.5 also had improvedmore » efficiency, VOC, and FF, relative to CuIn 1-yGa ySe 2 baselines. On the other hand, y ~ 1 absorbers did not benefit from K introduction. Similar to Cu 1-xK xInSe 2, the formation of Cu 1-xK xGaSe 2 alloys was favored at low temperatures and high Na supply by the substrate, relative to the formation of mixed-phase CuGaSe 2 + KGaSe 2. KIn 1-yGa ySe 2 alloys were grown for the first time, as evidenced by X-ray diffraction and ultraviolet/visible spectroscopy. For all Ga/(Ga+In) compositions, the surface KIn 1-yGa ySe 2 absorbers had superior PV performance in buffered and buffer-free devices. However, the bulk x ~ 0.07 absorbers only outperformed the baselines in buffered devices. The data demonstrate that KIn 1-yGa ySe 2 passivates the surface of CuIn 1-yGa ySe 2 to increase efficiency, VOC, and FF, while bulk Cu 1-xK xIn 1-yGa ySe 2 absorbers with x ~ 0.07 enhance efficiency, VOC, and FF by some other mechanism.« less

Avalanche multiplication and impact ionization in amorphous selenium photoconductive target

NASA Astrophysics Data System (ADS)

Park, Wug-Dong; Tanioka, Kenkichi

2014-03-01

The avalanche multiplication factor and the hole ionization coefficient in the amorphous selenium (a-Se) high-gain avalanche rushing amorphous photoconductor (HARP) target depend on the electric field. The phenomenon of avalanche multiplication and impact ionization in the 0.4-µm-thick a-Se HARP target is investigated. The hot carrier energy in the 0.4-µm-thick a-Se HARP target increases linearly as the target voltage increases. The energy relaxation length of hot carriers in the a-Se photoconductor of the 0.4-µm-thick HARP target saturates as the electric field increases. The average energy Eav of a hot carrier and the energy relaxation length λE in the a-Se photoconductor of the 0.4-µm-thick HARP target at 1 × 108 V/m were 0.25 eV and 2.5 nm, respectively. In addition, the hole ionization coefficient β and the avalanche multiplication factor M are derived as a function of the electric field, the average energy of a hot carrier, and the impact ionization energy. The experimental hole ionization coefficient β and the avalanche multiplication factor M in the 0.4-µm-thick a-Se HARP target agree with the theoretical results.

A DFT investigation of a bulky biomimetic model catalyzing the 5'-outer ring deiodination of thyroxine.

PubMed

Fortino, Mariagrazia; Marino, Tiziana; Russo, Nino; Sicilia, Emilia

2016-12-01

This paper illustrates the outcomes of a density functional theory investigation aimed at unraveling mechanistic aspects of the 5'-outer ring deiodination process of thyroxine (T4) assisted by the sterically protected organoselenol compound BpqSeH. BpqSeH, which was previously synthesized and tested for its deiodinase activity, is able to afford the active hormone 3,5,3'-tetraiodothyronine (T3) by selective outer-ring deiodination of T4, and to protect the SeH moiety inside the nano-sized molecular cavity from further reactivity, allowing its isolation and characterization. Calculations were also performed including an imidazole ring that, mimicking a His residue in the active site of the original enzyme, plays an crucial role in deprotonating the selenol moiety. Both the suggested enol/keto tautomerization and the previously proven formation of an intermediate whose main characteristic is the presence of a Se⋯I⋯C halogen bond, were examined along the pathway leading to 5'-outer ring deiodination. The calculated potential energy surface showed that neither the pathway encompassing enol/keto tautomerism nor the formation of a halogen bond paving the way to C-I bond breaking and chalcogen-I bond forming is viable. The exergonic formation of the final selenenyl iodide product confirms the stabilization effect of the molecular cavity. Graphical Abstract Computed free energy profile describing the 5'-outer deiodination of thyroxine assisted by the steric hindered organoselenol BpqSH compound. The molecular electrostatic potential map reoported for the INT1 intermediate shows the non-covalent Se-I interaction, due to the attraction between charges of opposite sign, that weakens the C-I bond and prepares the formation of the new Se-I bond.

Engineering p-n junctions and bandgap tuning of InSe nanolayers by controlled oxidation

NASA Astrophysics Data System (ADS)

Balakrishnan, Nilanthy; Kudrynskyi, Zakhar R.; Smith, Emily F.; Fay, Michael W.; Makarovsky, Oleg; Kovalyuk, Zakhar D.; Eaves, Laurence; Beton, Peter H.; Patanè, Amalia

2017-06-01

Exploitation of two-dimensional (2D) van der Waals (vdW) crystals can be hindered by the deterioration of the crystal surface over time due to oxidation. On the other hand, the existence of a stable oxide at room temperature can offer prospects for several applications. Here we report on the chemical reactivity of γ-InSe, a recent addition to the family of 2D vdW crystals. We demonstrate that, unlike other 2D materials, InSe nanolayers can be chemically stable under ambient conditions. However, both thermal- and photo-annealing in air induces the oxidation of the InSe surface, which converts a few surface layers of InSe into In2O3, thus forming an InSe/In2O3 heterostructure with distinct and interesting electronic properties. The oxidation can be activated in selected areas of the flake by laser writing or prevented by capping the InSe surface with an exfoliated flake of hexagonal boron nitride. We exploit the controlled oxidation of p-InSe to fabricate p-InSe/n-In2O3 junction diodes with room temperature electroluminescence and spectral response from the near-infrared to the visible and near-ultraviolet ranges. These findings reveal the limits and potential of thermal- and photo-oxidation of InSe in future technologies.

Enhanced Visible-Light Photocatalytic H2 Evolution in Cu2O/Cu2Se Multilayer Heterostructure Nanowires Having {111} Facets and Physical Mechanism.

PubMed

Liu, Bin; Ning, Lichao; Zhang, Congjie; Zheng, Hairong; Liu, Shengzhong Frank; Yang, Heqing

2018-06-21

It is rather challenging to develop photocatalysts based on narrow-band-gap semiconductors for water splitting under solar irradiation. Herein, we synthesized the Cu 2 O/Cu 2 Se multilayer heterostructure nanowires exposing {111} crystal facets by a hydrothermal reaction of Se with Cu and KBH 4 in ethanol amine aqueous solution and subsequent annealing in air. The photocatalytic H 2 production activity of Cu 2 O/Cu 2 Se multilayer heterostructure nanowires is dramatically improved, with an increase on the texture coefficient of Cu 2 O(111) and Cu 2 Se(111) planes, and thus the exposed {111} facets may be the active surfaces for photocatalytic H 2 production. On the basis of the polar structure of Cu 2 O {111} and Cu 2 Se {111} surfaces, we presented a model of charge separation between the Cu-Cu 2 Se(111) and O-Cu 2 O(1̅ 1̅ 1̅) polar surfaces. An internal electric field is created between Cu-Cu 2 Se(111) and O-Cu 2 O(1̅ 1̅ 1̅) polar surfaces, because of spontaneous polarization. As a result, this internal electric field drives the photocreated charge separation. The oxidation and reduction reactions selectively occur at the negative O-Cu 2 O(1̅ 1̅ 1̅) and the positive Cu-Cu 2 Se(111) surfaces. The polar surface-engineering may be a general strategy for enhancing the photocatalytic H 2 -production activity of semiconductor photocatalysts. The charge separation mechanism not only can deepen the understanding of photocatalytic H 2 production mechanism but also provides a novel insight into the design of advanced photocatalysts, other photoelectric devices, and solar cells.

Phosphine-free synthesis of high-quality reverse type-I ZnSe/CdSe core with CdS/CdxZn1 - xS/ZnS multishell nanocrystals and their application for detection of human hepatitis B surface antigen

NASA Astrophysics Data System (ADS)

Shen, Huaibin; Yuan, Hang; Niu, Jin Zhong; Xu, Shasha; Zhou, Changhua; Ma, Lan; Li, Lin Song

2011-09-01

Highly photoluminescent (PL) reverse type-I ZnSe/CdSe nanocrystals (NCs) and ZnSe/CdSe/CdS/CdxZn1 - xS/ZnS core/multishell NCs were successfully synthesized by a phosphine-free method. By this low-cost, 'green' synthesis route, more than 10 g of high-quality ZnSe/CdSe/CdS/CdxZn1 - xS/ZnS NCs were synthesized in a large scale synthesis. After the overgrowth of a CdS/CdxZn1 - xS/ZnS multishell on ZnSe/CdSe cores, the PL quantum yields (QYs) increased from 28% to 75% along with the stability improvement. An amphiphilic oligomer was used as a surface coating agent to conduct a phase transfer experiment, core/multishell NCs were dissolved in water by such surface modification and the QYs were still kept above 70%. The as-prepared water dispersible ZnSe/CdSe/CdS/CdxZn1 - xS/ZnS core/multishell NCs not only have high fluorescence QYs but also are extremely stable in various physiological conditions. Furthermore, a biosensor system (lateral flow immunoassay system, LFIA) for the detection of human hepatitis B surface antigen (HBsAg) was developed by using this water-soluble core/multishell NCs as a fluorescent label and a nitrocellulose filter membrane for lateral flow. The result showed that such ZnSe/CdSe/CdS/CdxZn1 - xS/ZnS core/multishell NCs were excellent fluorescent labels to detect HBsAg. The sensitivity of HBsAg detection could reach as high as 0.05 ng ml - 1.

Luminescent Quantum Dot Bioconjugates in Fluorescence Resonance Energy Transfer (FRET) Assays

NASA Astrophysics Data System (ADS)

Clapp, Aaron; Medintz, Igor; Goldman, Ellen; Anderson, George; Mauro, J. Matthew; Mattoussi, Hedi

2003-03-01

Colloidal semiconductor quantum dots (QDs) such as those made of CdSe-ZnS core-shell nanocrystals offer a promising alternative to organic dyes in a variety of biological tagging applications. They exhibit high resistance to chemical and photo-degradations, are highly luminescent, and show unique size-specific optical and spectroscopic properties. We have previously demonstrated a useful method for attaching proteins to CdSe-ZnS QDs using dihydrolipoic acid (DHLA) surface capping groups and electrostatic self-assembly in aqueous environments. We have used this conjugation strategy to build solution-based QD-conjugate sensors based on fluorescence resonance energy transfer (FRET) between QD donors and dye-labeled protein acceptors. Specific binding between the QD-ligand donor and dye-labeled receptor was achieved. In another example, the dye receptor was grafted directly onto the protein, then immobilized onto the QD surface via an electrostatic self-assembly process. The QD-complexes were optically excited in a region where absorption of the dye is negligible compared to that of the nanocrystals. We observed a continuous decrease of the QD emission accompanied by a steady and pronounced increase of the acceptor emission as the ratio of dye to QD was increased. The results of these experiments suggest efficient resonance energy transfer between the QD donor and the dye acceptor upon ligand-receptor binding. We will present these data and discuss other aspects such as donor-acceptor separation distance, degree of overlap between absorption of the acceptor and emission of the QD, and reverse FRET (upon ligand-receptor release) in a reversible assay.

High throughput secondary electron imaging of organic residues on a graphene surface

NASA Astrophysics Data System (ADS)

Zhou, Yangbo; O'Connell, Robert; Maguire, Pierce; Zhang, Hongzhou

2014-11-01

Surface organic residues inhibit the extraordinary electronic properties of graphene, hindering the development of graphene electronics. However, fundamental understanding of the residue morphology is still absent due to a lack of high-throughput and high-resolution surface characterization methods. Here, we demonstrate that secondary electron (SE) imaging in the scanning electron microscope (SEM) and helium ion microscope (HIM) can provide sub-nanometer information of a graphene surface and reveal the morphology of surface contaminants. Nanoscale polymethyl methacrylate (PMMA) residues are visible in the SE imaging, but their contrast, i.e. the apparent lateral dimension, varies with the imaging conditions. We have demonstrated a quantitative approach to readily obtain the physical size of the surface features regardless of the contrast variation. The fidelity of SE imaging is ultimately determined by the probe size of the primary beam. HIM is thus evaluated to be a superior SE imaging technique in terms of surface sensitivity and image fidelity. A highly efficient method to reveal the residues on a graphene surface has therefore been established.

Detection of Cu2Zn5SnSe8 and Cu2Zn6SnSe9 phases in co-evaporated Cu2ZnSnSe4 thin-films

NASA Astrophysics Data System (ADS)

Schwarz, Torsten; Marques, Miguel A. L.; Botti, Silvana; Mousel, Marina; Redinger, Alex; Siebentritt, Susanne; Cojocaru-Mirédin, Oana; Raabe, Dierk; Choi, Pyuck-Pa

2015-10-01

Cu2ZnSnSe4 thin-films for photovoltaic applications are investigated using combined atom probe tomography and ab initio density functional theory. The atom probe studies reveal nano-sized grains of Cu2Zn5SnSe8 and Cu2Zn6SnSe9 composition, which cannot be assigned to any known phase reported in the literature. Both phases are considered to be metastable, as density functional theory calculations yield positive energy differences with respect to the decomposition into Cu2ZnSnSe4 and ZnSe. Among the conceivable crystal structures for both phases, a distorted zinc-blende structure shows the lowest energy, which is a few tens of meV below the energy of a wurtzite structure. A band gap of 1.1 eV is calculated for both the Cu2Zn5SnSe8 and Cu2Zn6SnSe9 phases. Possible effects of these phases on solar cell performance are discussed.

Positron surface state as a spectroscopic probe for characterizing surfaces of topological insulator materials

NASA Astrophysics Data System (ADS)

Callewaert, Vincent; Shastry, K.; Saniz, Rolando; Makkonen, Ilja; Barbiellini, Bernardo; Assaf, Badih A.; Heiman, Donald; Moodera, Jagadeesh S.; Partoens, Bart; Bansil, Arun; Weiss, A. H.

2016-09-01

Topological insulators are attracting considerable interest due to their potential for technological applications and as platforms for exploring wide-ranging fundamental science questions. In order to exploit, fine-tune, control, and manipulate the topological surface states, spectroscopic tools which can effectively probe their properties are of key importance. Here, we demonstrate that positrons provide a sensitive probe for topological states and that the associated annihilation spectrum provides a technique for characterizing these states. Firm experimental evidence for the existence of a positron surface state near Bi2Te2Se with a binding energy of Eb=2.7 ±0.2 eV is presented and is confirmed by first-principles calculations. Additionally, the simulations predict a significant signal originating from annihilation with the topological surface states and show the feasibility to detect their spin texture through the use of spin-polarized positron beams.

Nanocrystal Size-Dependent Efficiency of Quantum Dot Sensitized Solar Cells in the Strongly Coupled CdSe Nanocrystals/TiO2 System.

PubMed

Yun, Hyeong Jin; Paik, Taejong; Diroll, Benjamin; Edley, Michael E; Baxter, Jason B; Murray, Christopher B

2016-06-15

Light absorption and electron injection are important criteria determining solar energy conversion efficiency. In this research, monodisperse CdSe quantum dots (QDs) are synthesized with five different diameters, and the size-dependent solar energy conversion efficiency of CdSe quantum dot sensitized solar cell (QDSSCs) is investigated by employing the atomic inorganic ligand, S(2-). Absorbance measurements and transmission electron microscopy show that the diameters of the uniform CdSe QDs are 2.5, 3.2, 4.2, 6.4, and 7.8 nm. Larger CdSe QDs generate a larger amount of charge under the irradiation of long wavelength photons, as verified by the absorbance results and the measurements of the external quantum efficiencies. However, the smaller QDs exhibit faster electron injection kinetics from CdSe QDs to TiO2 because of the high energy level of CBCdSe, as verified by time-resolved photoluminescence and internal quantum efficiency results. Importantly, the S(2-) ligand significantly enhances the electronic coupling between the CdSe QDs and TiO2, yielding an enhancement of the charge transfer rate at the interfacial region. As a result, the S(2-) ligand helps improve the new size-dependent solar energy conversion efficiency, showing best performance with 4.2-nm CdSe QDs, whereas conventional ligand, mercaptopropionic acid, does not show any differences in efficiency according to the size of the CdSe QDs. The findings reported herein suggest that the atomic inorganic ligand reinforces the influence of quantum confinement on the solar energy conversion efficiency of QDSSCs.

Exciton-Delocalizing Ligands Can Speed Up Energy Migration in Nanocrystal Solids.

PubMed

Azzaro, Michael S; Dodin, Amro; Zhang, Diana Y; Willard, Adam P; Roberts, Sean T

2018-05-09

Researchers have long sought to use surface ligands to enhance energy migration in nanocrystal solids by decreasing the physical separation between nanocrystals and strengthening their electronic coupling. Exciton-delocalizing ligands, which possess frontier molecular orbitals that strongly mix with nanocrystal band-edge states, are well-suited for this role because they can facilitate carrier-wave function extension beyond the nanocrystal core, reducing barriers for energy transfer. This report details the use of the exciton-delocalizing ligand phenyldithiocarbamate (PDTC) to tune the transport rate and diffusion length of excitons in CdSe nanocrystal solids. A film composed of oleate-terminated CdSe nanocrystals is subjected to a solid-state ligand exchange to replace oleate with PDTC. Exciton migration in the films is subsequently investigated by femtosecond transient absorption. Our experiments indicate that the treatment of nanocrystal films with PDTC leads to rapid (∼400 fs) downhill energy migration (∼80 meV), while no such migration occurs in oleate-capped films. Kinetic Monte Carlo simulations allow us to extract both rates and length scales for exciton diffusion in PDTC-treated films. These simulations reproduce dynamics observed in transient absorption measurements over a range of temperatures and confirm excitons hop via a Miller-Abrahams mechanism. Importantly, our experiments and simulations show PDTC treatment increases the exciton hopping rate to 200 fs, an improvement of 5 orders of magnitude relative to oleate-capped films. This exciton hopping rate stands as one of the fastest determined for CdSe solids. The facile, room-temperature processing and improved transport properties offered by the solid-state exchange of exciton-delocalizing ligands show they offer promise for the construction of strongly coupled nanocrystal arrays.

Surface Morphology of Undoped and Doped ZnSe Films

NASA Technical Reports Server (NTRS)

George, T.; Hayes, M.; Chen, H.; Chattopadhyay, K.; Thomas E.; Morgan, S.; Burger, A.

1998-01-01

Rare-earth doped ions in polar II-VI semiconductors have recently played an important role in the optical properties of materials and devices. In this study, undoped ZnSe and erbium doped ZnSe films were grown by radio frequency (RF) magnetron sputtering method. Atomic Force Microscopy (AFM) was used together with optical microscopy and UV-Vis spectroscopy to characterize the films. Doped samples were found to have higher surface roughness and quite different surface morphology compared to that of undoped samples. The grown films generally show a relatively smooth and uniform surface indicating that they are of overall good quality. The impact of plasma etching on ZnSe:Er film examined under AFM is also discussed.

SE-FIT

NASA Technical Reports Server (NTRS)

Chen, Yongkang; Weislogel, Mark; Schaeffer, Ben; Semerjian, Ben; Yang, Lihong; Zimmerli, Gregory

2012-01-01

The mathematical theory of capillary surfaces has developed steadily over the centuries, but it was not until the last few decades that new technologies have put a more urgent demand on a substantially more qualitative and quantitative understanding of phenomena relating to capillarity in general. So far, the new theory development successfully predicts the behavior of capillary surfaces for special cases. However, an efficient quantitative mathematical prediction of capillary phenomena related to the shape and stability of geometrically complex equilibrium capillary surfaces remains a significant challenge. As one of many numerical tools, the open-source Surface Evolver (SE) algorithm has played an important role over the last two decades. The current effort was undertaken to provide a front-end to enhance the accessibility of SE for the purposes of design and analysis. Like SE, the new code is open-source and will remain under development for the foreseeable future. The ultimate goal of the current Surface Evolver Fluid Interface Tool (SEFIT) development is to build a fully integrated front-end with a set of graphical user interface (GUI) elements. Such a front-end enables the access to functionalities that are developed along with the GUIs to deal with pre-processing, convergence computation operation, and post-processing. In other words, SE-FIT is not just a GUI front-end, but an integrated environment that can perform sophisticated computational tasks, e.g. importing industry standard file formats and employing parameter sweep functions, which are both lacking in SE, and require minimal interaction by the user. These functions are created using a mixture of Visual Basic and the SE script language. These form the foundation for a high-performance front-end that substantially simplifies use without sacrificing the proven capabilities of SE. The real power of SE-FIT lies in its automated pre-processing, pre-defined geometries, convergence computation operation, computational diagnostic tools, and crash-handling capabilities to sustain extensive computations. SE-FIT performance is enabled by its so-called file-layer mechanism. During the early stages of SE-FIT development, it became necessary to modify the original SE code to enable capabilities required for an enhanced and synchronized communication. To this end, a file-layer was created that serves as a command buffer to ensure a continuous and sequential execution of commands sent from the front-end to SE. It also establishes a proper means for handling crashes. The file layer logs input commands and SE output; it also supports user interruption requests, back and forward operation (i.e. undo and redo), and others. It especially enables the batch mode computation of a series of equilibrium surfaces and the searching of critical parameter values in studying the stability of capillary surfaces. In this way, the modified SE significantly extends the capabilities of the original SE.

Influence of the State of the Tungsten Tip on STM Topographic Images of SnSe Surfaces

NASA Astrophysics Data System (ADS)

Ly, Trinh Thi; Kim, Jungdae

2018-03-01

Tin selenide (SnSe) has recently attracted significant attention because of its excellent thermoelectric properties with a figure of merit (ZT) of 2.6. Previous scanning tunneling microscopy (STM) studies of SnSe surfaces showed that only Sn atoms are resolved in topographic images due to the dominant contribution of the Sn 5 p z states in tunneling. However, when the state of the tungsten (W) tip changes from a typical four-lobe d state such as d xy or {d_{{x^2} - {y^2}}} to a two-lobe {d_{{z^2}}} state, the atomic features observed on the SnSe surface in STM topography can be dramatically altered. In this report, we present the results of a systematic study on the influence of the W tip's states on the STM images of SnSe surfaces. Sn atoms are observed with much stronger corrugation amplitude and smaller apparent radius when the tip is in a {d_{{z^2}}} state. In addition, the atomic features of the Se atoms become visible because of the sharply focused shape of the W {d_{{z^2}}} state. We expect our results to provide important information for establishing a better understanding of the microscopic nature of SnSe surfaces.

Superconductivity and ferromagnetism in topological insulators

NASA Astrophysics Data System (ADS)

Zhang, Duming

Topological insulators, a new state of matter discovered recently, have attracted great interest due to their novel properties. They are insulating inside the bulk, but conducting at the surface or edges. This peculiar behavior is characterized by an insulating bulk energy gap and gapless surface or edge states, which originate from strong spin-orbit coupling and time-reversal symmetry. The spin and momentum locked surface states not only provide a model system to study fundamental physics, but can also lead to applications in spintronics and dissipationless electronics. While topological insulators are interesting by themselves, more exotic behaviors are predicted when an energy gap is induced at the surface. This dissertation explores two types of surface state gap in topological insulators, a superconducting gap induced by proximity effect and a magnetic gap induced by chemical doping. The first three chapters provide introductory theory and experimental details of my research. Chapter 1 provides a brief introduction to the theoretical background of topological insulators. Chapter 2 is dedicated to material synthesis principles and techniques. I will focus on two major synthesis methods: molecular beam epitaxy for the growth of Bi2Se3 thin films and chemical vapor deposition for the growth of Bi2Se3 nanoribbons and nanowires. Material characterization is discussed in Chapter 3. I will describe structural, morphological, magnetic, electrical, and electronic characterization techniques used to study topological insulators. Chapter 4 discusses the experiments on proximity-induced superconductivity in topological insulator (Bi2Se3) nanoribbons. This work is motivated by the search for the elusive Majorana fermions, which act as their own antiparticles. They were proposed by Ettore Majorara in 1937, but have remained undiscovered. Recently, Majorana's concept has been revived in condensed matter physics: a condensed matter analog of Majorana fermions is predicted to exist when topological insulators are interfaced with superconductors. The observation of Majorana fermions would not only be fundamentally important, but would also lead to applications in fault-tolerant topological quantum computation. By interfacing topological insulator nanoribbons with superconducting electrodes, we observe distinct signatures of proximity-induced superconductivity, which is found to be present in devices with channel lengths that are much longer than the normal transport characteristic lengths. This might suggest preferential coupling of the proximity effect to a ballistic surface channel of the topological insulator. In addition, when the electrodes are in the superconducting state, we observe periodic magnetoresistance oscillations which suggest the formation of vortices in the proximity-induced region of the nanoribbons. Our results demonstrate that proximity-induced superconductivity and vortices can be realized in our nanoribbon geometry, which accomplishes a first important step towards the search for Majorana fermions in condensed matter. In Chapter 5, I will discuss experiments on a magnetically-doped topological insulator (Mn-doped Bi2Se3) to induce a surface state gap. The metallic Dirac cone surface states of a topological insulator are expected to be protected against small perturbations by time-reversal symmetry. However, these surface states can be dramatically modified and a finite energy gap can be opened at the Dirac point by breaking the time-reversal symmetry via magnetic doping. The interplay between magnetism and topological surface states is predicted to yield novel phenomena of fundamental interest such as a topological magneto-electric effect, a quantized anomalous Hall effect, and the induction of magnetic monopoles. Our systematic measurements reveal a close correlation between the onset of ferromagnetism and quantum corrections to diffusive transport, which crosses over from the symplectic (weak anti-localization) to the unitary (weak localization) class. A comprehensive interpretation of data obtained from electrical transport, angle-resolved photoemission spectroscopy, superconducting quantum interference device magnetometry, and scanning tunneling microscopy indicates that the ferromagnetism responsible for modifications in the surface states occurs in nanoscale regions on the surface where magnetic atoms segregate during sample growth. This suggests that some aspects of the observed magnetoconductance may indeed originate from surface transport despite the non-ideal nature of the samples. These observations are consistent with the prediction of a time-reversal symmetry breaking gap, which is further supported by angle-resolved photoemission spectroscopy measurements.

Tuning Topological Surface States by Charge Transfer

NASA Astrophysics Data System (ADS)

Chen, Zhiyi

Three-dimensional (3D) topological insulators (TIs), Bi2Se 3, Bi2Te3, Sb2Te3, are a class of materials that has non-trivial bulk band structure and metallic surface states. Access to charge transport through Dirac surface states in TIs can be challenging due to their intermixing with bulk states or non-topological two-dimensional electron gas quantum well states caused by bending of electronic bands near the surface. The band bending arises via charge transfer from surface adatoms or interfaces and, therefore, the choice of layers abutting topological surfaces is critical. Surfaces of these 3D TIs have also been proposed to host new quantum phases at the interfaces with other types of materials, provided that the topological properties of interfacial regions remain unperturbed. This thesis presents a systematic experimental study of both bulk conducting and surface charge transfer problems. We started with optimizing growth condition of Bi2Se3 on various substrates, to achieve best quality of Bi2Se3 single layers we can get. We then move on to growth of Bi2Se3/ZnxCd1-xSe bilayers. Here we improved lattice mismatch between Bi2Se 3 and ZnxCd1-xSe layers by tuning lattice parameter of ZnxCd1-xSe. After that, we achieved molecular beam epitaxial growth of Bi2Se3/ZnxCd1-x Se superlattices that hold only one topological surface channel per TI layer. The topological nature of conducting channels is supported by pi-Berry phase evident from observed Shubnikov de Haas quantum oscillations and by the associated two-dimensional weak antilocalization quantum interference correction to magnetoresistance. Both density functional theory calculations and transport measurements suggest that a single topological Dirac cone per TI layer can be realized by asymmetric interfaces: Se-terminated Znx Cd1-xSe interface with the TI remains 'electronically intact', while charge transfer occurs at the Zn-terminated interface. Our findings indicate that topological transport could be controlled by adjusting charge transfer from non-topological spacers in hybrid structures. The first chapter contains a brief introduction to TIs. It describes basic concepts and notations used later in the bulk of the thesis. These include the topological surface states of a TI, crystal structure of 3D TIs, the origin of defects and their effects on transport study. The second chapter presents experimental techniques employed for growth and for structural, and electrical characterization of the 3D TIs thin films and superlattices. First, every component of our custom-designed molecular beam epitaxy system will be described in detail, and then the important in situ surface morphology monitoring tool - RHEED will also be mentioned, as well as high resolution X-ray diffraction (XRD). In the second part, a standard procedure for device fabrication will be presented. The last part will focus on the electron transport measurement setup and various techniques for characterization. In the third chapter we present explorations of different substrates for growth of Bi2Se3 thin films, describe growth of Bi2Se3 thin films on sapphire, GaAs(111), InP(001) and InP(111), then optimize growth conditions accordingly. The quality of films are investigated to study the effects of substrates on quality of the films. The fourth chapter is a growth study of superlattice of a TI with a traditional II-VI semiconductor, Bi2Se3/ZnxCd1-x Se. we explore II-VI semiconductor family and study the optimal material to grow on top of Bi2Se3. Then we focus on the growth of Bi2Se3/ZnxCd1-xSe superlattice and structural study. The fifth chapter studies charge transfer at the interface between Bi 2Se3 layer and ZnxCd1-xSe layer. We start by looking at the result of charge transport study of our superlattice. Then we will present the result of our density functional theory (DFT) calculation, which showed completely different charge transfer between Bi2Se 3 sits on top of ZnxCd1-xSe and ZnxCd 1-xSe on top of Bi2Se3. This will provide a perfect explanation of our experimental results. Then we designed experiment using transport measurement to test and confirm out explanation. The sixth chapter gives a short summary of this thesis work and a proposal for future work.

Surface state-dominated photoconduction and THz-generation in topological Bi2Te2Se-nanowires

NASA Astrophysics Data System (ADS)

Seifert, Paul; Vaklinova, Kristina; Kern, Klaus; Burghard, Marko; Holleitner, Alexander

Topological insulators constitute a fascinating class of quantum materials with non-trivial, gapless states on the surface and trivial, insulating bulk states. In revealing the optoelectronic dynamics in the whole range from femto- to microseconds, we demonstrate that the long surface lifetime of Bi2Te2Se-nanowires allows to access the surface states by a pulsed photoconduction scheme and that there is a prevailing bolometric response of the surface states. The interplay of the surface state dynamics on the different timescales gives rise to a surprising physical property of Bi2Te2Se-nanowires: their pulsed photoconductance changes polarity as a function of laser power. Moreover, we show that single Bi2Te2Se-nanowires can be used as THz-generators for on-chip high-frequency circuits at room temperature. Our results open the avenue for single Bi2Te2Se-nanowires as active modules in optoelectronic high-frequency and THz-circuits. We acknowledge financial support by the ERC Grant NanoReal (n306754).

Electron and hole relaxation pathways in semiconductor quantum dots

DOE Office of Scientific and Technical Information (OSTI.GOV)

Klimov, V.I.; McBranch, D.W.; Leatherdale, C.A.

1999-11-01

Femtosecond (fs) broad-band transient absorption (TA) is used to study the intraband relaxation and depopulation dynamics of electron and hole quantized states in CdSe nanocrystals (NC{close_quote}s) with a range of surface properties. Instead of the drastic reduction in the energy relaxation rate expected due to a {open_quotes}phonon bottleneck,{close_quotes} we observe a fast subpicosecond 1P-to-1S electron relaxation, with the rate exceeding that due to phonon emission in bulk semiconductors. The energy relaxation is enhanced with reducing the NC{close_quote}s radius, and does not show any dependence on the NC surface properties (quality of the surface passivation). These data indicate that electron energymore » relaxation occurs by neither multiphonon emission nor by coupling to surface defects, but is likely meditated by Auger-type electron-hole energy transfer. We use fs infrared TA to probe electron and hole intraband transitions, which allows us to distinguish between electron and hole relaxation pathways leading to the depopulation of NC quantized states. In contrast to the electron relaxation, which is controlled by NC surface passivation, the depopulation of hole quantized states is extremely fast (sub-ps-to-ps time scales) in all types of samples, independent of NC surface treatment (including NC{close_quote}s overcoated with a ZnS layer). Our results indicate that ultrafast hole dynamics are not due to trapping at localized surface defects such as a vacancy, but rather arise from relaxation into intrinsic NC states or intrinsically unpassivated interface states. {copyright} {ital 1999} {ital The American Physical Society}« less

Some physical investigations on ZnS 1- xSe x films obtained by selenization of ZnS sprayed films using the Boubaker polynomials expansion scheme

NASA Astrophysics Data System (ADS)

Fridjine, S.; Touihri, S.; Boubaker, K.; Amlouk, M.

2010-01-01

ZnS 1- xSe x thin films have been grown by selenization process, applied to ZnS sprayed thin films deposited on Pyrex glass substrates at 550 °C. The crystal structure and surface morphology were investigated by the XRD technique and by the atomic force microscopy. This structural study shows that selenium-free ( x=0) ZnS thin films, prepared at substrate temperature TS=450 °C, were well crystallized in cubic structure and oriented preferentially along (1 1 1) direction. The thermal and mechanical properties were also investigated using a photothermal protocol along with Vickers hardness measurements. On the other hand, the analyze of the transmittance T( λ) and the reflectance R( λ), optical measurements of these films depicts a decrease in the band gap energy value Eg with an increase in Se content ( x). Indeed, Eg values vary from 3.6 to 3.1 eV.

Work function of bulk-insulating topological insulator Bi{sub 2–x}Sb{sub x}Te{sub 3–y}Se{sub y}

DOE Office of Scientific and Technical Information (OSTI.GOV)

Takane, Daichi; Souma, Seigo; Center for Spintronics Research Network, Tohoku University, Sendai 980-8577

Recent discovery of bulk insulating topological insulator (TI) Bi{sub 2–x}Sb{sub x}Te{sub 3–y}Se{sub y} paved a pathway toward practical device application of TIs. For realizing TI-based devices, it is necessary to contact TIs with a metal. Since the band-bending at the interface dominates the character of devices, knowledge of TIs' work function is of essential importance. We have determined the compositional dependence of the work function in Bi{sub 2–x}Sb{sub x}Te{sub 3–y}Se{sub y} by high-resolution photoemission spectroscopy. The obtained work-function values (4.95–5.20 eV) track the energy shift of the surface chemical potential seen by angle-resolved photoemission spectroscopy. The present result serves as amore » useful guide for developing TI-based electronic devices.« less

Role of ZnO photoanode nanostructures and sensitizer deposition approaches on the photovoltaic properties of CdS/CdSe and CdS1-xSex quantum dot-sensitized solar cells

NASA Astrophysics Data System (ADS)

Şişman, İlkay; Tekir, Oktay; Karaca, Hüseyin

2017-02-01

Hierarchical bundle-like ZnO nanorod arrays (BNRs) were synthesized by a one-pot hydrothermal method based on two consecutive temperature steps for cascade CdS/CdSe and ternary CdS1-xSex alloy quantum dot-sensitized solar cells (QDSSCs) as photoanode. The CdS/CdSe and CdS1-xSex QDs were deposited on the surface of the ZnO BNRs by conventional and modified successive ionic-layer adsorption and reaction (SILAR) methods, respectively. Using the ZnO BNRs/CdS/CdSe photoanode, the power conversion efficiency reaches 2.08%, which is 1.8 times higher than that of pristine ZnO nanorods/CdS/CdSe photoanode, while by applying ZnO BNRs/CdS1-xSex, the power conversion efficiency improves 2.52%. The remarkably improved photovoltaic performance is mainly derived from the bundle-like nanorod arrays structure, which increases the QDs loading amount and the scattering effect for light absorption, and the appropriate conduction band energy, sufficient Se amount and well coverage of the ternary CdS1-xSex QDs result in enhanced photogenerated electron injection, high light absorption and reduced recombination, respectively. As a result, ZnO BNRs/CdS1-xSex combination can significantly improve performance of QDSSCs.

AgGaSe2 thin films grown by chemical close-spaced vapor transport for photovoltaic applications: structural, compositional and optical properties.

PubMed

Merschjann, C; Mews, M; Mete, T; Karkatzinou, A; Rusu, M; Korzun, B V; Schorr, S; Schubert-Bischoff, P; Seeger, S; Schedel-Niedrig, Th; Lux-Steiner, M-Ch

2012-05-02

Thin films of chalcopyrite AgGaSe(2) have been successfully grown on glass and glass/molybdenum substrates using the technique of chemical close-spaced vapor transport. The high crystallinity of the samples is confirmed by grazing-incidence x-ray diffraction, scanning and transmission electron microscopy, and optical transmission/reflection spectroscopy. Here, two of the three expected direct optical bandgaps are found at 1.77(2) and 1.88(6) eV at 300 K. The lowest bandgap energy at 4 K is estimated to be 1.82(3) eV. Photoluminescence spectroscopy has further revealed the nature of the point defects within the AgGaSe(2), showing evidence for the existence of very shallow acceptor levels of 5(1) and 10(1) meV, and thus suggesting the AgGaSe(2) phase itself to exhibit a p-type conductivity. At the same time, electrical characterization by Hall, Seebeck and four-point-probe measurements indicate properties of a compensated semiconductor. The electrical properties of the investigated thin films are mainly influenced by the presence of Ag(2)Se and Ga(2)O(3) nanometer-scaled surface layers, as well as by Ag(2)Se inclusions in the bulk and Ag clusters at the layers' rear side. © 2012 IOP Publishing Ltd

Density functional theory (DFT) study of the gas-phase decomposition of the Cd[((i)Pr)2PSSe] 2 single-source precursor for the CVD of binary and ternary cadmium chalcogenides.

PubMed

Opoku, Francis; Asare-Donkor, Noah Kyame; Adimado, Anthony A

2014-11-01

The chemistry of group II-VI semiconductors has spurred considerable interest in decomposition reaction mechanisms and has been exploited for various technological applications. In this work, computational chemistry was employed to investigate the possible gas-phase decomposition pathways of the mixed Cd[((i)Pr)2PSSe]2 single-source precursor for the chemical vapour deposition of cadmium chalcogenides as thin films. The geometries of the species involved were optimised by employing density functional theory at the MO6/LACVP* level. The results indicate that the steps that lead to CdS formation on the singlet potential energy surface are favoured kinetically over those that lead to CdSe and ternary CdSe(x)S(1-x) formation. On the doublet PES, the steps that lead to CdSe formation are favoured kinetically over those that lead to CdS and CdSe(x)S(1-x) formation. However, thermodynamically, the steps that lead to ternary CdSe(x)S(1-x) formation are more favourable than those that lead to CdSe and CdS formation on both the singlet and the doublet PESs. Density functional theory calculations revealed that the first steps exhibit huge activation barriers, meaning that the thermodynamically favourable process takes a very long time to initiate.

Analysis of cutting force signals by wavelet packet transform for surface roughness monitoring in CNC turning

NASA Astrophysics Data System (ADS)

García Plaza, E.; Núñez López, P. J.

2018-01-01

On-line monitoring of surface finish in machining processes has proven to be a substantial advancement over traditional post-process quality control techniques by reducing inspection times and costs and by avoiding the manufacture of defective products. This study applied techniques for processing cutting force signals based on the wavelet packet transform (WPT) method for the monitoring of surface finish in computer numerical control (CNC) turning operations. The behaviour of 40 mother wavelets was analysed using three techniques: global packet analysis (G-WPT), and the application of two packet reduction criteria: maximum energy (E-WPT) and maximum entropy (SE-WPT). The optimum signal decomposition level (Lj) was determined to eliminate noise and to obtain information correlated to surface finish. The results obtained with the G-WPT method provided an in-depth analysis of cutting force signals, and frequency ranges and signal characteristics were correlated to surface finish with excellent results in the accuracy and reliability of the predictive models. The radial and tangential cutting force components at low frequency provided most of the information for the monitoring of surface finish. The E-WPT and SE-WPT packet reduction criteria substantially reduced signal processing time, but at the expense of discarding packets with relevant information, which impoverished the results. The G-WPT method was observed to be an ideal procedure for processing cutting force signals applied to the real-time monitoring of surface finish, and was estimated to be highly accurate and reliable at a low analytical-computational cost.

Roughness, surface energy, and superficial damages of CAD/CAM materials after surface treatment.

PubMed

Strasser, Thomas; Preis, Verena; Behr, Michael; Rosentritt, Martin

2018-02-05

The aim of this study was to examine the effects of surface pre-treatment on CAD/CAM materials including ceramics, zirconia, resin-infiltrated ceramic, and resin-based composite. Specimens were made of ten CAD/CAM materials (Celtra Duo, Degudent, D; Vita Suprinity, Vita, D; E.max CAD, Ivoclar-Vivadent, FL; E.max ZirCAD, Ivoclar-Vivadent, FL; Vita Enamic, Vita, D; Cerasmart, GC, B; LAVA Ultimate, 3M, D; SHOFU Block HC, SHOFU, US; Grandio Blocs, VOCO, D; BRILLIANT Crios, Coltene, CH) and pretreated to represent clinical procedures (Hf 20 s/5%; phosphoric acid 20 s/37%; Monobond etch and prime (Ivoclar-Vivadent, FL); water-cooled diamond bur (80 μm; 4 μm); Al 2 O 3 -blasting (50 μm/1 bar, 50 μm/2 bar, 120 μm/1 bar, 120 μm/2 bar); untreated; manufacturer's instructions). SEM-analysis (Phenom, FEI, NL) of the surfaces was performed (magnifications ≤ 10,000×). Roughness values R a , R z (KJ 3D, Keyence, J), and surface energy SE (OCA15 plus, SCA20, DataPhysics, D) were determined (statistics: non-parametric Mann-Whitney U test/Kruskal-Wallis test for independent specimen, α = 0.05). Kruskal-Wallis revealed significant (p < 0.001) differences for all materials with different surface treatments. Roughness ranged from R a  = 0.05 μm (VS; D4)/R z  = 0.41 μm (VS; D4) to R a  = 1.82 μm (EMA; SB120/2)/R z  = 12.05 μm (CS; SB 120/2), SE from 22.7 mN/m (VE; M) to 52.8 mN/m (CD; M). SEM analysis showed material-dependent damages after pre-treatment. Different CAD/CAM materials require individual pre-treatment for optimized and protective surface activation. Cementation is a key factor for clinical success. Given the variety of available CAD/CAM materials, specific procedures are needed.

Micelle-templated composite quantum dots for super-resolution imaging.

PubMed

Xu, Jianquan; Fan, Qirui; Mahajan, Kalpesh D; Ruan, Gang; Herrington, Andrew; Tehrani, Kayvan F; Kner, Peter; Winter, Jessica O

2014-05-16

Quantum dots (QDs) have tremendous potential for biomedical imaging, including super-resolution techniques that permit imaging below the diffraction limit. However, most QDs are produced via organic methods, and hence require surface treatment to render them water-soluble for biological applications. Previously, we reported a micelle-templating method that yields nanocomposites containing multiple core/shell ZnS-CdSe QDs within the same nanocarrier, increasing overall particle brightness and virtually eliminating QD blinking. Here, this technique is extended to the encapsulation of Mn-doped ZnSe QDs (Mn-ZnSe QDs), which have potential applications in super-resolution imaging as a result of the introduction of Mn(2+) dopant energy levels. The size, shape and fluorescence characteristics of these doped QD-micelles were compared to those of micelles created using core/shell ZnS-CdSe QDs (ZnS-CdSe QD-micelles). Additionally, the stability of both types of particles to photo-oxidation was investigated. Compared to commercial QDs, micelle-templated QDs demonstrated superior fluorescence intensity, higher signal-to-noise ratios, and greater stability against photo-oxidization,while reducing blinking. Additionally, the fluorescence of doped QD-micelles could be modulated from a bright 'on' state to a dark 'off' state, with a modulation depth of up to 76%, suggesting the potential of doped QD-micelles for applications in super-resolution imaging.

An overview of distributed microgrid state estimation and control for smart grids.

PubMed

Rana, Md Masud; Li, Li

2015-02-12

Given the significant concerns regarding carbon emission from the fossil fuels, global warming and energy crisis, the renewable distributed energy resources (DERs) are going to be integrated in the smart grid. This grid can spread the intelligence of the energy distribution and control system from the central unit to the long-distance remote areas, thus enabling accurate state estimation (SE) and wide-area real-time monitoring of these intermittent energy sources. In contrast to the traditional methods of SE, this paper proposes a novel accuracy dependent Kalman filter (KF) based microgrid SE for the smart grid that uses typical communication systems. Then this article proposes a discrete-time linear quadratic regulation to control the state deviations of the microgrid incorporating multiple DERs. Therefore, integrating these two approaches with application to the smart grid forms a novel contributions in green energy and control research communities. Finally, the simulation results show that the proposed KF based microgrid SE and control algorithm provides an accurate SE and control compared with the existing method.

Energy Scaling of Nanosecond Gain-Switched Cr2+:ZnSe Lasers

DTIC Science & Technology

2011-01-01

outcoupler or absorption from the lightly-doped active ions. Additionally, the edges of the crystals are cut at the Brewster angle , which raises...experiments we used Brewster cut Cr:ZnSe gain elements with a chromium concentration of 8x1018 cm-3. Under Cr:Tm:Ho:YAG pumping, the first Cr:ZnSe laser...the energy scaling of nanosecond gain-switched Cr:ZnSe lasers is optimization of the gain medium. In this study we used Brewster cut Cr:ZnSe gain

Andreev Reflection Spectroscopy of Nb-doped Bi2Se3 Topological Insulator

NASA Astrophysics Data System (ADS)

Kurter, C.; Finck, A. D. K.; Qiu, Y.; Huemiller, E.; Weis, A.; Atkinson, J.; Medvedeva, J.; Hor, Y. S.; van Harlingen, D. J.

2015-03-01

Doped topological insulators are speculated to realize p-wave superconductivity with unusual low energy quasiparticles, such as surface Andreev bound states. We present point contact spectroscopy of thin exfoliated flakes of Nb-doped Bi2Se3 where superconductivity persists up to ~ 1 K, compared to 3.2 K in bulk crystals. The critical magnetic field is strongly anisotropic, consistent with quasi-2D behavior. Andreev reflection measurements of devices with low resistance contacts result in prominent BTK-like behavior with an enhanced conductance plateau at low bias. For high resistance contacts, we observe a split zero bias conductance anomaly and additional features at the superconducting gap. Our results suggest that this material is a promising platform for studying topological superconductivity. We acknowledge support from Microsoft Project Q.

Ultrafast dynamics of colloidal semiconductor nanocrystals relevant to solar fuels production

NASA Astrophysics Data System (ADS)

Cogan, Nicole M. B.; Liu, Cunming; Qiu, Fen; Burke, Rebeckah; Krauss, Todd D.

2017-05-01

Artificial conversion of sunlight to chemical fuels has attracted attention for several decades as a potential source of clean, renewable energy. We recently found that CdSe quantum dots (QDs) and simple aqueous Ni2+ salts in the presence of a sacrificial electron donor form a highly efficient, active, and robust system for photochemical reduction of protons to molecular hydrogen. Ultrafast transient absorption spectroscopy studies of electron transfer (ET) processes from the QDs to the Ni catalysts reveal extremely fast ET, and provide a fundamental explanation for the exceptional photocatalytic H2 activity. Additionally, by studying H2 production of the Ni catalyst with CdSe/CdS nanoparticles of various structures, it was determined that surface charge density plays an important role in charge transfer and ultimately H2 production activity.

Ab initio nonadiabatic molecular dynamics of the ultrafast electron injection from a PbSe quantum dot into the TiO2 surface.

PubMed

Long, Run; Prezhdo, Oleg V

2011-11-30

Following recent experiments [Science 2010, 328, 1543; PNAS 2011, 108, 965], we report an ab initio nonadiabatic molecular dynamics (NAMD) simulation of the ultrafast photoinduced electron transfer (ET) from a PbSe quantum dot (QD) into the rutile TiO(2) (110) surface. The system forms the basis for QD-sensitized semiconductor solar cells and demonstrates that ultrafast interfacial ET is instrumental for achieving high efficiencies in solar-to-electrical energy conversion. The simulation supports the observation that the ET successfully competes with energy losses due to electron-phonon relaxation. The ET proceeds by the adiabatic mechanism because of strong donor-acceptor coupling. High frequency polar vibrations of both QD and TiO(2) promote the ET, since these modes can rapidly influence the donor-acceptor state energies and coupling. Low frequency vibrations generate a distribution of initial conditions for ET, which shows a broad variety of scenarios at the single-molecule level. Compared to the molecule-TiO(2) interfaces, the QD-TiO(2) system exhibits pronounced differences that arise due to the larger size and higher rigidity of QDs relative to molecules. Both donor and acceptor states are more delocalized in the QD system, and the ET is promoted by optical phonons, which have relatively low frequencies in the QD materials composed of heavy elements. In contrast, in molecular systems, optical phonons are not thermally accessible under ambient conditions. Meanwhile, TiO(2) acceptor states resemble surface impurities due to the local influence of molecular chromophores. At the same time, the photoinduced ET at both QD-TiO(2) and molecule-TiO(2) interfaces is ultrafast and occurs by the adiabatic mechanism, as a result of strong donor-acceptor coupling. The reported state-of-the-art simulation generates a detailed time-domain atomistic description of the interfacial ET process that is fundamental to a wide variety of applications.

Understanding the features in the ultrafast transient absorption spectra of CdSe quantum dots

NASA Astrophysics Data System (ADS)

Zhang, Cheng; Do, Thanh Nhut; Ong, Xuanwei; Chan, Yinthai; Tan, Howe-Siang

2016-12-01

We describe a model to explain the features of the ultrafast transient absorption (TA) spectra of CdSe core type quantum dots (QDs). The measured TA spectrum consists of contributions by the ground state bleach (GSB), stimulated emission (SE) and excited state absorption (ESA) processes associated with the three lowest energy transition of the QDs. We model the shapes of the GSB, SE and ESA spectral components after fits to the linear absorption. The spectral positions of the ESA components take into account the biexcitonic binding energy. In order to obtain the correct weightage of the GSB, SE and ESA components to the TA spectrum, we enumerate the set of coherence transfer pathways associated with these processes. From our fits of the experimental TA spectra of 65 Å diameter QDs, biexcitonic binding energies for the three lowest energy transitions are obtained.

Excited-state relaxation in PbSe quantum dots

NASA Astrophysics Data System (ADS)

An, Joonhee M.; Califano, Marco; Franceschetti, Alberto; Zunger, Alex

2008-04-01

In solids the phonon-assisted, nonradiative decay from high-energy electronic excited states to low-energy electronic excited states is picosecond fast. It was hoped that electron and hole relaxation could be slowed down in quantum dots, due to the unavailability of phonons energy matched to the large energy-level spacings ("phonon-bottleneck"). However, excited-state relaxation was observed to be rather fast (⩽1ps) in InP, CdSe, and ZnO dots, and explained by an efficient Auger mechanism, whereby the excess energy of electrons is nonradiatively transferred to holes, which can then rapidly decay by phonon emission, by virtue of the densely spaced valence-band levels. The recent emergence of PbSe as a novel quantum-dot material has rekindled the hope for a slow down of excited-state relaxation because hole relaxation was deemed to be ineffective on account of the widely spaced hole levels. The assumption of sparse hole energy levels in PbSe was based on an effective-mass argument based on the light effective mass of the hole. Surprisingly, fast intraband relaxation times of 1-7ps were observed in PbSe quantum dots and have been considered contradictory with the Auger cooling mechanism because of the assumed sparsity of the hole energy levels. Our pseudopotential calculations, however, do not support the scenario of sparse hole levels in PbSe: Because of the existence of three valence-band maxima in the bulk PbSe band structure, hole energy levels are densely spaced, in contradiction with simple effective-mass models. The remaining question is whether the Auger decay channel is sufficiently fast to account for the fast intraband relaxation. Using the atomistic pseudopotential wave functions of Pb2046Se2117 and Pb260Se249 quantum dots, we explicitly calculated the electron-hole Coulomb integrals and the P →S electron Auger relaxation rate. We find that the Auger mechanism can explain the experimentally observed P →S intraband decay time scale without the need to invoke any exotic relaxation mechanisms.

Tuning the emission of aqueous Cu:ZnSe quantum dots to yellow light window

NASA Astrophysics Data System (ADS)

Wang, Chunlei; Hu, Zhiyang; Xu, Shuhong; Wang, Yanbin; Zhao, Zengxia; Wang, Zhuyuan; Cui, Yiping

2015-07-01

Synthesis of internally doped Cu:ZnSe QDs in an aqueous solution still suffers from narrow tunable emissions from the blue to green light window. In this work, we extended the emission window of aqueous Cu:ZnSe QDs to the yellow light window. Our results show that high solution pH, multiple injections of Zn precursors, and nucleation doping strategy are three key factors for preparing yellow emitted Cu:ZnSe QDs. All these factors can depress the reactivity of CuSe nuclei and Zn monomers, promoting ZnSe growth outside CuSe nuclei rather than form ZnSe nuclei separately. With increased ZnSe QD size, the conduction band and nearby trap state energy levels shift to higher energy sites, causing Cu:ZnSe QDs to have a much longer emission.

First-principles study of defect formation in a photovoltaic semiconductor Cu2ZnGeSe4

NASA Astrophysics Data System (ADS)

Nishihara, Hironori; Maeda, Tsuyoshi; Wada, Takahiro

2018-02-01

The formation energies of neutral Cu, Zn, Ge, and Se vacancies in kesterite-type Cu2ZnGeSe4 were evaluated by first-principles pseudopotential calculations using plane-wave basis functions. The calculations were performed at typical points in Cu-(Zn1/2Ge1/2)-Se and Cu3Se2-ZnSe-GeSe2 pseudoternary phase diagrams for Cu2ZnGeSe4. The results were compared with those for Cu2ZnSnSe4, Cu2ZnGeS4, and Cu2ZnSnS4 calculated using the same version of the CASTEP program code. The results indicate that Cu vacancies are easily formed in Cu2ZnGeSe4 under the Cu-poor condition as in the above compounds and CuInSe2, suggesting that Cu2ZnGeSe4 is also a preferable p-type absorber material for thin-film solar cells. The formation energies of possible antisite defects, such as CuZn and CuGe, and of possible complex defects, such as CuZn+ZnCu, were also calculated and compared within the above materials. The antisite defect of CuZn, which has the smallest formation energy within the possible defects, is concluded to be the most hardly formed in Cu2ZnGeSe4 among the compounds.

Formation and reconstruction of Se nanoislands at the surface of thin epitaxial ZnSe layers grown on GaAs substrates

DOE Office of Scientific and Technical Information (OSTI.GOV)

Kozlovskiy, V. I.; Krivobok, V. S., E-mail: krivobok@lebedev.ru; Kuznetsov, P. I.

2016-05-15

Strained epitaxial ZnSe layers are grown on GaAs substrates by the method of vapor-phase epitaxy from metal-organic compounds. It is found that Se nanoislands with a density of 10{sup 8} to 10{sup 9} cm{sup –2} are formed at the surface of such layers. It is established that an increase in the size of Se islands and a decrease in their density take place after completion of growth. Annealing in a H{sub 2} atmosphere at a temperature higher than 260°C leads to the disappearance of Se islands and to a decrease in the surface roughness. It is shown that annealing doesmore » not lead to deterioration of the structural perfection of the epitaxial ZnSe films; rather, annealing gives rise to a decrease in the intensity of impurity–defect luminescence and to an increase in the intensity of intrinsic radiation near the bottom of the exciton band.« less

Rapid surface accumulation of NMDA receptors increases glutamatergic excitation during status epilepticus.

PubMed

Naylor, David E; Liu, Hantao; Niquet, Jerome; Wasterlain, Claude G

2013-06-01

After 1h of lithium-pilocarpine status epilepticus (SE), immunocytochemical labeling of NMDA receptor NR1 subunits reveals relocation of subunits from the interior to the cell surface of dentate gyrus granule cells and CA3 pyramidal cells. Simultaneously, an increase in NMDA-miniature excitatory postsynaptic currents (mEPSC) as well as an increase in NMDA receptor-mediated tonic currents is observed in hippocampal slices after SE. Mean-variance analysis of NMDA-mEPSCs estimates that the number of functional postsynaptic NMDA receptors per synapse increases 38% during SE, and antagonism by ifenprodil suggests that an increase in the surface representation of NR2B-containing NMDA receptors is responsible for the augmentation of both the phasic and tonic excitatory currents with SE. These results provide a potential mechanism for an enhancement of glutamatergic excitation that maintains SE and may contribute to excitotoxic injury during SE. Therapies that directly antagonize NMDA receptors may be a useful therapeutic strategy during refractory SE. Copyright © 2013 Elsevier Inc. All rights reserved.

Rapid surface accumulation of NMDA receptors increases glutamatergic excitation during status epilepticus

PubMed Central

Naylor, David E.; Liu, Hantao; Niquet, Jerome; Wasterlain, Claude G.

2017-01-01

After 1 h of lithium-pilocarpine status epilepticus (SE), immunocytochemical labeling of NMDA receptor NR1 subunits reveals relocation of subunits from the interior to the cell surface of dentate gyrus granule cells and CA3 pyramidal cells. Simultaneously, an increase in NMDA-miniature excitatory postsynaptic currents (mEPSC) as well as an increase in NMDA receptor-mediated tonic currents is observed in hippocampal slices after SE. Mean-variance analysis of NMDA-mEPSCs estimates that the number of functional postsynaptic NMDA receptors per synapse increases 38% during SE, and antagonism by ifenprodil suggests that an increase in the surface representation of NR2B-containing NMDA receptors is responsible for the augmentation of both the phasic and tonic excitatory currents with SE. These results provide a potential mechanism for an enhancement of glutamatergic excitation that maintains SE and may contribute to excitotoxic injury during SE. Therapies that directly antagonize NMDA receptors may be a useful therapeutic strategy during refractory SE. PMID:23313318

Effect of adding Te to layered GaSe crystals to increase the van der Waals bonding force

NASA Astrophysics Data System (ADS)

Tanabe, Tadao; Zhao, Shu; Sato, Yohei; Oyama, Yutaka

2017-10-01

The interplanar binding strength of layered GaSe1-xTex crystals was directly measured using a tensile testing machine. The GaSe1-xTex crystals were grown by a low temperature liquid phase solution method under a controlled Se vapor pressure. The stoichiometry-controlled GaSe1-xTex crystal has the ɛ-polytype structure of GaSe, where the Te atoms are substituted for some of the Se atoms in the GaSe crystal. The effect of adding Te on the bonding strength between the GaSe layers was determined from direct measurements of the van der Waals bonding energy. The bonding energy was increased from 0.023 × 106 N/m2 for GaSe to 0.16 × 106 N/m2 for GaSe1-xTex (x = 0.106).

Dark and photo conductivity analysis of Cu doped CdSe-PVA nanocomposites synthesized by chemical route

DOE Office of Scientific and Technical Information (OSTI.GOV)

Rani, Amita; Kurchania, Rajnish; Tripathi, S. K., E-mail: surya@pu.ac.in

2016-05-06

Present communication deals with the study of electrical conductivity measurements of Cu doped CdSe-PVA nanocomposite via chemical method. In electrical measurements, the dark conductivity (σ{sub d}) and the photoconductivity (σ{sub ph}) of CdSe prepared thin films have been studied in the temperature range of 308–343 K. The effect of temperature and the intensity on conductivity has been analyzed for CdSe and CdSe:Cu nanocomposite films. The conductivity of all the samples increases with increasing temperature indicating the semiconducting behavior of the samples. The value of photo activation energy is less than the dark activation energy due to the shift in energy levelsmore » under illumination.« less

Graphene oxide based CdSe photocatalysts: Synthesis, characterization and comparative photocatalytic efficiency of rhodamine B and industrial dye

DOE Office of Scientific and Technical Information (OSTI.GOV)

Ghosh, Trisha; Lee, Jeong-Ho; Meng, Ze-Da

Highlights: ► CdSe–graphene is synthesized by hydrothermal method. ► Three molar solutions of CdSe were used making three different composites. ► RhB and Texbrite MST-L were used as sample dye solutions. ► Texbrite MST-L is photo degraded in visible light. ► UV-spectroscopic analysis was done to measure degradation. - Abstract: CdSe–graphene composites were prepared using simple “hydrothermal method” where the graphene surface was modified using different molar solutions of cadmium selenide (CdSe) in aqueous media. The characterization of CdSe–graphene composites were studied by X-ray diffraction (XRD), energy dispersive X-ray (EDX), scanning electron microscope (SEM), and with transmission electron microscope (TEM).more » The catalytic activities of CdSe-composites were evaluated by degradation of rhodamine B (RhB) and commercial industrial dye “Texbrite MST-L (TXT-MST)” with fixed concentration. The degradation was observed by the decrease in the absorbance peak studied by UV spectrophotometer. The decrease in the dye concentration indicated catalytic degradation effect by CdSe–graphene composites.« less

Influence of Doping and Nanostructuration on n-Type Bi2(Te0.8Se0.2)3 Alloys Synthesized by Arc Melting

NASA Astrophysics Data System (ADS)

Gharsallah, Mouna; Serrano-Sanchez, Federico; Nemes, Norbert M.; Martinez, Jose Luis; Alonso, Jose Antonio

2017-01-01

In competitive thermoelectric devices for energy conversion and generation, high-efficiency materials of both n-type and p-type are required. For this, Bi2Te3-based alloys have the best thermoelectric properties in room temperature applications. Partial replacement of tellurium by selenium is expected to introduce new donor states in the band gap, which would alter electrical conductivity and thermopower. We report on the preparation of n-type Bi2(Te1-xSex)3 solid solutions by a straightforward arc-melting technique, yielding nanostructured polycrystalline pellets. X-ray and neutron powder diffraction was used to assess Se inclusion, also indicating that the interactions between quintuple layers constituting this material are weakened upon Se doping, while the covalency of intralayer bonds is augmented. Moreover, scanning electron microscopy shows large surfaces perpendicular to the c crystallographic axis assembled as stacked sheets. Grain boundaries related to this 2D nanostructuration affect the thermal conductivity reducing it below 0.8 Wm-1K-1 at room temperature. Furthermore, Se doping increases the absolute Seebeck coefficient up to -140 μV K-1 at 400 K, which is also beneficial for improved thermoelectric efficiency.

Characterizing the electronic ground states of single-layer NbSe2 via STM/STS

NASA Astrophysics Data System (ADS)

Chen, Yi; Ugeda, Miguel; Bradley, Aaron; Zhang, Yi; Onishi, Seita; Ruan, Wei; Ojeda-Aristizabal, Claudia; Ryu, Hyejin; Edmonds, Mark; Tsai, Hsin-Zon; Riss, Alexander; Mo, Sung-Kwan; Lee, Dunghai; Zettl, Alex; Hussain, Zahid; Shen, Zhi-Xun; Crommie, Michael

Layered transition metal dichalcogenides (TMDs) are ideal systems for exploring collective electronic phases such as charge density wave (CDW) order and superconductivity. In bulk NbSe2 the CDW sets in at TCDW = 33K and superconductivity sets in at Tc = 7.2K. Below Tc these electronic states coexist but their microscopic formation mechanisms remain controversial. Here we present an electronic characterization study of a single 2D layer of NbSe2 by means of low temperature scanning tunneling microscopy/spectroscopy (STM/STS), angle-resolved photoemission spectroscopy (ARPES), and electrical transport measurements. We demonstrate that the CDW order remains intact in 2D and exhibits a robust 3 x 3 superlattice. Superconductivity also still occurs but its onset is depressed to 1.6K. Our STS measurements at 5K reveal a CDW gap of Δ = 4 meV at the Fermi energy, which is accessible via STS due to the removal of bands crossing the Fermi surface in the 2D limit. Our observations are consistent with the predicted simplified (compared to bulk) electronic structure of single-layer NbSe2, thus providing new insight into CDW formation and superconductivity in this model strongly-correlated system.

The interactions between CdSe quantum dots and yeast Saccharomyces cerevisiae: adhesion of quantum dots to the cell surface and the protection effect of ZnS shell.

PubMed

Mei, Jie; Yang, Li-Yun; Lai, Lu; Xu, Zi-Qiang; Wang, Can; Zhao, Jie; Jin, Jian-Cheng; Jiang, Feng-Lei; Liu, Yi

2014-10-01

The interactions between quantum dots (QDs) and biological systems have attracted increasing attention due to concerns on possible toxicity of the nanoscale materials. The biological effects of CdSe QDs and CdSe/ZnS QDs with nearly identical hydrodynamic size on Saccharomyces cerevisiae were investigated via microcalorimetric, spectroscopic and microscopic methods, demonstrating a toxic order CdSe>CdSe/ZnS QDs. CdSe QDs damaged yeast cell wall and reduced the mitochondrial membrane potential. Noteworthy, adhesion of QDs to the yeast cell surface renders this work a good example of interaction site at cell surface, and the epitaxial coating of ZnS could greatly reduce the toxicity of Cd-containing QDs. These results will contribute to the safety evaluation of quantum dots, and provide valuable information for design of nanomaterials. Copyright © 2014 Elsevier Ltd. All rights reserved.

Shell Thickness Dependence of Interparticle Energy Transfer in Core-Shell ZnSe/ZnSe Quantum Dots Doping with Europium

NASA Astrophysics Data System (ADS)

Liu, Ni; Li, Shuxin; Wang, Caifeng; Li, Jie

2018-04-01

Low-toxic core-shell ZnSe:Eu/ZnS quantum dots (QDs) were prepared through two steps in water solution: nucleation doping and epitaxial shell grown. The structural and morphological characteristics of ZnSe/ZnS:Eu QDs with different shell thickness were explored by transmission electron microscopy (TEM) and X-ray diffraction (XRD) results. The characteristic photoluminescence (PL) intensity of Eu ions was enhanced whereas that of band-edge luminescence and defect-related luminescence of ZnSe QDs was decreased with increasing shell thickness. The transformation of PL intensity revealed an efficient energy transfer process between ZnSe and Eu. The PL intensity ratio of Eu ions ( I 613) to ZnSe QDs ( I B ) under different shell thickness was systemically analyzed by PL spectra and time-resolved PL spectra. The obtained results were in agreement with the theory analysis results by the kinetic theory of energy transfer, revealing that energy was transmitted in the form of dipole-electric dipole interaction. This particular method of adjusting luminous via changing the shell thickness can provide valuable insights towards the fundamental understanding and application of QDs in the field of optoelectronics.

Myocardial signal density levels and beam-hardening artifact attenuation using dual-energy computed tomography.

PubMed

Rodriguez-Granillo, Gaston A; Carrascosa, Patricia; Cipriano, Silvina; de Zan, Macarena; Deviggiano, Alejandro; Capunay, Carlos; Cury, Ricardo C

2015-01-01

The assessment of myocardial perfusion using single-energy (SE) imaging is influenced by beam-hardening artifacts (BHA). We sought to explore the ability of dual-energy (DE) imaging to attenuate the presence of BHA. Myocardial signal density (SD) was evaluated in 2240 myocardial segments (112 for each energy level) and in 320 American Heart Association segments among the SE group. Compared to DE reconstructions at the best energy level, SE acquisitions showed no significant differences overall regarding myocardial SD or signal-to-noise ratio. The segments most commonly affected by BHA showed significantly lower myocardial SD at the lowest energy levels, progressively normalizing at higher energy levels. Copyright © 2015 Elsevier Inc. All rights reserved.

Disorder Effects in Charge Transport and Spin Response of Topological Insulators

NASA Astrophysics Data System (ADS)

Zhao, Lukas Zhonghua

Topological insulators are a class of solids in which the non-trivial inverted bulk band structure gives rise to metallic surface states that are robust against impurity backscattering. First principle calculations predicted Bi2Te3, Sb2Te3 and Bi2Se3 to be three-dimensional (3D) topological insulators with a single Dirac cone on the surface. The topological surface states were subsequently observed by angle-resolved photoemission (ARPES) and scanning tunneling microscopy (STM). The investigations of charge transport through topological surfaces of 3D topological insulators, however, have faced a major challenge due to large charge carrier densities in the bulk donated by randomly distributed defects such as vacancies and antisites. This bulk disorder intermixes surface and bulk conduction channels, thereby complicating access to the low-energy (Dirac point) charge transport or magnetic response and resulting in the relatively low measured carrier mobilities. Moreover, charge inhomogeneity arising from bulk disorder can result in pronounced nanoscale spatial fluctuations of energy on the surface, leading to the formation of surface `puddles' of different carrier types. Great efforts have been made to combat the undesirable effects of disorder in 3D topological insulators and to reduce bulk carriers through chemical doping, nanostructure fabrication, and electric gating. In this work we have developed a new way to reduce bulk carrier densities using high-energy electron irradiation, thereby allowing us access to the topological surface quantum channels. We also found that disorder in 3D topological insulators can be beneficial. It can play an important part in enabling detection of unusual magnetic response from Dirac fermions and in uncovering new excitations, namely surface superconductivity in Dirac `puddles'. In Chapter 3 we show how by using differential magnetometry we could probe spin rotation in the 3D topological material family (Bi2Se 3, Bi2Te3 and Sb2Te3), and describe our detection of paramagnetic singularity in the magnetic susceptibility at low magnetic fields that persists up to room temperature, and which we have demonstrated to arise from the surfaces of the samples. The singularity is universal to the entire family, largely independent of the bulk carrier density, and consistent with the existence of electronic states near the spin-degenerate Dirac point of the 2D helical metal. The exceptional thermal stability of the signal points to an intrinsic surface cooling process, probably of thermoelectric organ, and establishes a sustainable platform for the singular field-tunable Dirac spin response. In Chapter 4 we describe our discovery of surface superconductivity in a hole-conducting topological insulator Sb2Te3 with transition to zero resistance induced through a minor tuning of growth chemistry that depletes bulk conduction channels. The depletion shifts Fermi energy towards the Dirac point as witnessed by over two orders of magnitude reduced bulk hole density and by the largest carrier mobility (~ 25,000 cm 2 V-1 s-1) found in any topological material. Direct evidence from transport, the unprecedentedly large diamagnetic screening, and the presence of up to ~ 25 meV gaps in differential conductance detected by scanning tunneling spectroscopy (STM) reveal the superconducting condensate to emerge first in surface puddles at unexpectedly high temperature, near 50 K. Percolative Josephson paths mediated by diffusing quasiparticles establish global phase coherence around 9 K. Rich structure of this state lends itself to manipulation and tuning via growth conditions and the topological material's parameters such as Fermi velocity and mean free path. In Chapter 5 we describe a new approach we have developed to reaching stable charge neutrality in 3D topological materials. The technique uses swift (~ 2.5 MeV energy) electron beams to compensate charged bulk defects and bring the Fermi level back into the bulk gap. By controlling the beam fluence we could tune bulk conductivity from p- (hole-like) to n-type (electron-like), crossing the Dirac point and back, while preserving the robust topological signatures of surface channels. We establish that at charge neutrality conductance has a two-dimensional (2D) character with a minimum value on the order of ten conductance quanta G=e 2 /h. From quantum interference contribution to 2D conductance we demonstrate in two systems, Bi2Te3 and Bi2Se 3, that at charge neutrality only two quantum channels corresponding to two topological surfaces are present. The charge neutrality point achieved using electron irradiation with long penetration range shows a route to intrinsic quantum transport of the topological states unconstrained by the bulk size.

Helium ion microscopy and energy selective scanning electron microscopy - two advanced microscopy techniques with complementary applications

NASA Astrophysics Data System (ADS)

Rodenburg, C.; Jepson, M. A. E.; Boden, Stuart A.; Bagnall, Darren M.

2014-06-01

Both scanning electron microscopes (SEM) and helium ion microscopes (HeIM) are based on the same principle of a charged particle beam scanning across the surface and generating secondary electrons (SEs) to form images. However, there is a pronounced difference in the energy spectra of the emitted secondary electrons emitted as result of electron or helium ion impact. We have previously presented evidence that this also translates to differences in the information depth through the analysis of dopant contrast in doped silicon structures in both SEM and HeIM. Here, it is now shown how secondary electron emission spectra (SES) and their relation to depth of origin of SE can be experimentally exploited through the use of energy filtering (EF) in low voltage SEM (LV-SEM) to access bulk information from surfaces covered by damage or contamination layers. From the current understanding of the SES in HeIM it is not expected that EF will be as effective in HeIM but an alternative that can be used for some materials to access bulk information is presented.

Enhanced Adsorption of Selenium Ions from Aqueous Solution Using Iron Oxide Impregnated Carbon Nanotubes

PubMed Central

Bakather, Omer Y.; Khraisheh, Majeda; Nasser, Mustafa S.

2017-01-01

The aim of this research was to investigate the potential of raw and iron oxide impregnated carbon nanotubes (CNTs) as adsorbents for the removal of selenium (Se) ions from wastewater. The original and modified CNTs with different loadings of Fe2O3 nanoparticles were characterized using high resolution transmission electron microscopy (HRTEM), scanning electron microscopy (SEM), X-ray diffractometer (XRD), Brunauer, Emmett, and Teller (BET) surface area analyzer, thermogravimetric analysis (TGA), zeta potential, and energy dispersive X-ray spectroscopy (EDS). The adsorption parameters of the selenium ions from water using raw CNTs and iron oxide impregnated carbon nanotubes (CNT-Fe2O3) were optimized. Total removal of 1 ppm Se ions from water was achieved when 25 mg of CNTs impregnated with 20 wt.% of iron oxide nanoparticles is used. Freundlich and Langmuir isotherm models were used to study the nature of the adsorption process. Pseudo-first and pseudo-second-order models were employed to study the kinetics of selenium ions adsorption onto the surface of iron oxide impregnated CNTs. Maximum adsorption capacity of the Fe2O3 impregnated CNTs, predicted by Langmuir isotherm model, was found to be 111 mg/g. This new finding might revolutionize the adsorption treatment process and application by introducing a new type of nanoadsorbent that has super adsorption capacity towards Se ions. PMID:28555093

Effects of nanoparticle shape on the morphology and properties of porous CdSe assemblies (aerogels).

PubMed

Yu, Hongtao; Brock, Stephanie L

2008-08-01

We demonstrate the effect of differently shaped CdSe nanoscale building blocks (dots, rods, branched nanoparticles, and hyperbranched nanoparticles) on the morphologies, surface characteristics, and optical properties of resultant porous CdSe nanostructured aerogels. Monolithic CdSe aerogels were produced by controlled oxidative removal of surface thiolate ligands from differently shaped CdSe nanoparticles to yield a wet gel, followed by CO(2) supercritical drying. The X-ray diffraction data show that the resultant CdSe aerogels maintain the crystalline phase of the building blocks without significant grain growth. However, the transmission electron microscopy images indicate that the morphology of CdSe aerogels changes from a colloid-type morphology to a polymer-type morphology when the building block changes from dot to rod or the branched nanoparticle. The morphology of the CdSe aerogel assembled from hyperbranched nanoparticles appears to be intermediate between the colloid-type and the polymer-type. Nitrogen physisorption measurements suggest that the surface areas and porosity are a direct function of the shape of the primary building blocks, with aerogels formed from rods or branched particles exhibiting the greatest surface areas (>200 m(2)/g) and those prepared from hyperbranched nanoparticles exhibiting the least (<100 m(2)/g). Band gap measurements and photoluminescence studies show that the as-prepared CdSe aerogels retain to a large extent the intrinsic quantum confinement of the differently shaped building blocks, despite being connected into a 3D network.

The relationship between structural and optical properties of Se-Ge-As glasses

NASA Astrophysics Data System (ADS)

Ghayebloo, M.; Rezvani, M.; Tavoosi, M.

2018-05-01

In this study, the structural and optical characterization of bulk Se-Ge-As glasses has been investigated. In this regards, six different Se60Ge40-xAsx (0 ≤ x ≤ 25) glasses were prepared by conventional melt quenching technique in quartz ampoule. The produced samples were characterized using X-ray diffraction (XRD), Raman spectroscopy, differential thermal analysis (DTA), ultraviolet-visible (UV-Vis) and Fourier transform infrared (FTIR) spectroscopy. The fundamental absorption edge for all the glasses was analyzed in terms of the theory proposed by Davis and Mott. According to achieved results, fully amorphous phase can easily form in different Se-Ge-As systems. The thermal and optical characteristic of Se60Ge40-xAsx glasses shows anomalous behavior at 5 mol% of As for the glass transition temperature, transmittance, absorption edge, optical energy gap and Urbach energy. The highest glass transition temperature, transmittance, optical energy gap and Urbach energy properties were achieved in Se60Ge35As5 glass as a result of the highest connectivity of cations and anions in glass network.

One-dimensional carrier confinement in “Giant” CdS/CdSe excitonic nanoshells

DOE PAGES

Razgoniaeva, Natalia; Moroz, Pavel; Yang, Mingrui; ...

2017-05-23

Here, the emerging generation of quantum dot optoelectronic devices offers an appealing prospect of a size-tunable band gap. The confinement-enabled control over electronic properties, however, requires nanoparticles to be sufficiently small, which leads to a large area of interparticle boundaries in a film. Such interfaces lead to a high density of surface traps which ultimately increase the electrical resistance of a solid. To address this issue, we have developed an inverse energy-gradient core/shell architecture supporting the quantum confinement in nanoparticles larger than the exciton Bohr radius. The assembly of such nanostructures exhibits a relatively low surface-to-volume ratio, which was manifestedmore » in this work through the enhanced conductance of solution-processed films. The reported core/shell geometry was realized by growing a narrow gap semiconductor layer (CdSe) on the surface of a wide-gap core material (CdS) promoting the localization of excitons in the shell domain, as was confirmed by ultrafast transient absorption and emission lifetime measurements. The band gap emission of fabricated nanoshells, ranging from 15 to 30 nm in diameter, has revealed a characteristic size-dependent behavior tunable via the shell thickness with associated quantum yields in the 4.4–16.0% range.« less

Experimental indication for band gap widening of chalcopyrite solar cell absorbers after potassium fluoride treatment

DOE Office of Scientific and Technical Information (OSTI.GOV)

Pistor, P., E-mail: paul.pistor@physik.uni-halle.de; Greiner, D.; Kaufmann, C. A.

2014-08-11

The implementation of potassium fluoride treatments as a doping and surface modification procedure in chalcopyrite absorber preparation has recently gained much interest since it led to new record efficiencies for this kind of solar cells. In the present work, Cu(In,Ga)Se{sub 2} absorbers have been evaporated on alkali containing Mo/soda-lime glass substrates. We report on compositional and electronic changes of the Cu(In,Ga)Se{sub 2} absorber surface as a result of a post deposition treatment with KF (KF PDT). In particular, by comparing standard X-ray photoelectron spectroscopy and synchrotron-based hard X-ray photoelectron spectroscopy (HAXPES), we are able to confirm a strong Cu depletionmore » in the absorbers after the KF PDT which is limited to the very near surface region. As a result of the Cu depletion, we find a change of the valence band structure and a shift of the valence band onset by approximately 0.4 eV to lower binding energies which is tentatively explained by a band gap widening as expected for Cu deficient compounds. The KF PDT increased the open circuit voltage by 60–70 mV compared to the untreated absorbers, while the fill factor deteriorated.« less

One-dimensional carrier confinement in “Giant” CdS/CdSe excitonic nanoshells

DOE Office of Scientific and Technical Information (OSTI.GOV)

Razgoniaeva, Natalia; Moroz, Pavel; Yang, Mingrui

Here, the emerging generation of quantum dot optoelectronic devices offers an appealing prospect of a size-tunable band gap. The confinement-enabled control over electronic properties, however, requires nanoparticles to be sufficiently small, which leads to a large area of interparticle boundaries in a film. Such interfaces lead to a high density of surface traps which ultimately increase the electrical resistance of a solid. To address this issue, we have developed an inverse energy-gradient core/shell architecture supporting the quantum confinement in nanoparticles larger than the exciton Bohr radius. The assembly of such nanostructures exhibits a relatively low surface-to-volume ratio, which was manifestedmore » in this work through the enhanced conductance of solution-processed films. The reported core/shell geometry was realized by growing a narrow gap semiconductor layer (CdSe) on the surface of a wide-gap core material (CdS) promoting the localization of excitons in the shell domain, as was confirmed by ultrafast transient absorption and emission lifetime measurements. The band gap emission of fabricated nanoshells, ranging from 15 to 30 nm in diameter, has revealed a characteristic size-dependent behavior tunable via the shell thickness with associated quantum yields in the 4.4–16.0% range.« less

Ordered CdSe nanoparticles within self-assembled block copolymer domains on surfaces.

PubMed

Zou, Shan; Hong, Rui; Emrick, Todd; Walker, Gilbert C

2007-02-13

Hierarchical, high-density, ordered patterns were fabricated on Si substrates by self-assembly of CdSe nanoparticles within approximately 20-nm-thick diblock copolymer films in a controlled manner. Surface-modified CdSe nanoparticles formed well-defined structures within microphase-separated polystyrene-b-poly(2-vinylpyridine) (PS-b-P2VP) domains. Trioctylphosphine oxide (TOPO)-coated CdSe nanoparticles were incorporated into PS domains and polyethylene glycol-coated CdSe nanoparticles were located primarily in the P2VP domains. Nearly close-packed CdSe nanoparticles were clearly identified within the highly ordered patterns on Si substrates by scanning electron microscopy (SEM). Contact angle measurements together with SEM results indicate that TOPO-CdSe nanoparticles were partially placed at the air/copolymer interface.

New organoselenium compounds with intramolecular Se⋯O/ Se⋯H interactions: NMR and theoretical studies

NASA Astrophysics Data System (ADS)

Fragoso, Erick; Azpiroz, Ramón; Sharma, Pankaj; Espinosa-Pérez, Georgina; Lara-Ochoa, Francisco; Toscano, Alfredo; Gutierrez, Rene; Portillo, Oscar

2018-03-01

New 1,3-bis(phenylselanylmethyl)benzene (1, 2 and 4) and butyl phenylselane derivatives (3 and 5) are synthesized and full heteronuclear NMR characterization of these compounds are reported. Interestingly, NMR spectrum of compounds 2-5 show coupling of 1H and 13C signals of groups involved in intramolecular nonbonding interactions with 77Se. The coupling constants JH-Se and JC-Se are in the range 13.6-21.6 Hz and 28-49 Hz, respectively. For compounds 4 and 5, JH-Se coupling constants of formyl proton are smaller than their respective acetal sbnd CH protons for compounds 2 and 3. However, this trend is opposite for JC-Se coupling constants, indicating that in formyl group containing compounds 4 and 5, Se⋯O interactions are present while in compounds 2 and 3 with acetal fragments, Se⋯H interactions also could be present because of steric constraints. To confirm these interactions, quantum chemical analyses were performed for 2, 4 and 5. The minimal energy conformation for these compounds present Se⋯O/Se⋯H interactions and are at lower energy in comparison to different conformers which do not show any interaction. For compounds 4 and 5, minimal energy conformation present Se⋯O interactions and for compound 2, Se⋯H is the favored conformation. These results are in accordance with the NMR data for these compounds. X-ray crystal structure of compound 1,3-bis(phenylselanylmethyl)benzene (1) was also determined during this work. In order to understand the effect of the Se⋯O/Se⋯H interactions and the position of phenylselanylmethyl groups, quantum chemical analyses were also carried out for 1,4-bis(phenylselanylmethyl)benzene derivatives (6 and 7). Interestingly, minimal energy conformers of 1,3-bis(phenylselanylmethyl)benzene derivatives 2 and 4 are more stable than their corresponding conformers of 1,4-bis-(phenylselanylmethyl)benzene derivatives 6 and 7.1,3-bis[{(2-(diethoxymethyl)phenyl)selanyl}methyl]benzene (2) with an energy barrier of 16.22 kcal/mol is more stable than corresponding 1,4-bis [{(2-(diethoxymethyl)phenyl)selanyl}methyl]benzene (7), while molecule 4 is 1.79 kcal/mol more stable than its corresponding 2'-[{1,4-phenylenebis(methylene)}bis(selanediyl)]dibenzaldehyde (6).

An Overview of Distributed Microgrid State Estimation and Control for Smart Grids

PubMed Central

Rana, Md Masud; Li, Li

2015-01-01

Given the significant concerns regarding carbon emission from the fossil fuels, global warming and energy crisis, the renewable distributed energy resources (DERs) are going to be integrated in the smart grid. This grid can spread the intelligence of the energy distribution and control system from the central unit to the long-distance remote areas, thus enabling accurate state estimation (SE) and wide-area real-time monitoring of these intermittent energy sources. In contrast to the traditional methods of SE, this paper proposes a novel accuracy dependent Kalman filter (KF) based microgrid SE for the smart grid that uses typical communication systems. Then this article proposes a discrete-time linear quadratic regulation to control the state deviations of the microgrid incorporating multiple DERs. Therefore, integrating these two approaches with application to the smart grid forms a novel contributions in green energy and control research communities. Finally, the simulation results show that the proposed KF based microgrid SE and control algorithm provides an accurate SE and control compared with the existing method. PMID:25686316

Solar Cells from Plastics? Mission Possible at the PHaSE Energy Research Center, UMass Amherst (A "Life at the Frontiers of Energy Research" contest entry from the 2011 Energy Frontier Research Centers (EFRCs) Summit and Forum)

ScienceCinema

Russell, Thomas P; Lahti, Paul M. (PHaSE - Polymer-Based Materials for Harvesting Solar Energy); PHaSE Staff

2017-12-09

'Solar Cells from Plastics? Mission Possible at the PHaSE Energy Research Center, UMass Amherst' was submitted by the Polymer-Based Materials for Harvesting Solar Energy (PHaSE) EFRC to the 'Life at the Frontiers of Energy Research' video contest at the 2011 Science for Our Nation's Energy Future: Energy Frontier Research Centers (EFRCs) Summit and Forum. Twenty-six EFRCs created short videos to highlight their mission and their work. PHaSE, an EFRC co-directed by Thomas P. Russell and Paul M. Lahti at the University of Massachusetts, Amherst, is a partnership of scientists from six institutions: UMass (lead), Oak Ridge National Laboratory, Pennyslvania State University, Rensselaer Polytechnic Institute, and the University of Pittsburgh. The Office of Basic Energy Sciences in the U.S. Department of Energy's Office of Science established the 46 Energy Frontier Research Centers (EFRCs) in 2009. These collaboratively-organized centers conduct fundamental research focused on 'grand challenges' and use-inspired 'basic research needs' recently identified in major strategic planning efforts by the scientific community. The overall purpose is to accelerate scientific progress toward meeting the nation's critical energy challenges.

Solar Cells from Plastics? Mission Possible at the PHaSE Energy Research Center, UMass Amherst (A "Life at the Frontiers of Energy Research" contest entry from the 2011 Energy Frontier Research Centers (EFRCs) Summit and Forum)

DOE Office of Scientific and Technical Information (OSTI.GOV)

Pentzer, Emily

"Solar Cells from Plastics? Mission Possible at the PHaSE Energy Research Center, UMass Amherst" was submitted by the Polymer-Based Materials for Harvesting Solar Energy (PHaSE) EFRC to the "Life at the Frontiers of Energy Research" video contest at the 2011 Science for Our Nation's Energy Future: Energy Frontier Research Centers (EFRCs) Summit and Forum. Twenty-six EFRCs created short videos to highlight their mission and their work. PHaSE, an EFRC co-directed by Thomas P. Russell and Paul M. Lahti at the University of Massachusetts, Amherst, is a partnership of scientists from six institutions: UMass (lead), Oak Ridge National Laboratory, Pennsylvania Statemore » University, Rensselaer Polytechnic Institute, and the University of Pittsburgh. The Office of Basic Energy Sciences in the U.S. Department of Energy's Office of Science established the 46 Energy Frontier Research Centers (EFRCs) in 2009. These collaboratively-organized centers conduct fundamental research focused on 'grand challenges' and use-inspired 'basic research needs' recently identified in major strategic planning efforts by the scientific community. The overall purpose is to accelerate scientific progress toward meeting the nation's critical energy challenges.« less

One-pot synthesis of hollow NiSe-CoSe nanoparticles with improved performance for hybrid supercapacitors

NASA Astrophysics Data System (ADS)

Chen, Haichao; Fan, Meiqiang; Li, Chao; Tian, Guanglei; Lv, Chunju; Chen, Da; Shu, Kangying; Jiang, Jianjun

2016-10-01

Hollow NiSe-CoSe samples have been synthesized for the first time via a one-pot solvothermal approach. The strategy is robust enough to synthesize NiSe-CoSe nanoparticles with different NiSe to CoSe ratios but with a similar hollow structure. Co ions in the NiSe-CoSe nanoparticles play decisive role for formation of the hollow structure; otherwise, the nanoparticles become solid for the NiSe sample. When used as the positive electroactive materials for energy storage, the NiSe-CoSe samples show excellent electrochemical activity in alkaline electrolyte. Using the synergistic effect between NiSe and CoSe, the electrochemical performance of NiSe-CoSe can be tuned by varying the NiSe to CoSe ratios. The NiSe-CoSe sample with a NiSe to CoSe ratio of 4:2 shows the best electrochemical performance in terms of superior specific capacity, improved rate capability and excellent cycling stability. In addition, the electrochemical performance of NiSe-CoSe sample with a NiSe to CoSe ratio of 4:2 is also evaluated via assembling hybrid supercapacitors with RGO, and the hybrid supercapacitor delivers both high power and energy densities (41.8 Wh kg-1 at 750 W kg-1 and 20.3 Wh kg-1 at 30 kW kg-1).

Electron Irradiation Effects on Nanocrystal Quantum Dots Used in Bio-Sensing Applications

NASA Technical Reports Server (NTRS)

Leon, R.; Nadeau, J.; Evans, K.; Paskova, T.; Monemar, B.

2004-01-01

Effects of electron irradiation on some of the optical properties in organic CdSe nanocrystals coated in trioctylphosphine oxide (TOPO) and biologically compatible CdSe nanocrystals coated in mercaptoacetic acid, as CdSe as CdSe nanocrystals conjugated with the protein are investigated using the technique of cathodoluminescence. Effects of varying the beam energy and temperatures were examined and faster degradation at cryogenic temperatures and higher beam energies was found under some conditions.

Selenium mobilization during a flood experiment in a contaminated wetland: Stewart Lake Waterfowl Management Area, Utah

USGS Publications Warehouse

Naftz, D.L.; Yahnke, J.; Miller, J.; Noyes, S.

2005-01-01

Constructed and natural wetlands can accumulate elevated levels of Se; however, few data are available on cost-effective methods for remobilization and removal of Se from these areas. A field experiment was conducted to assess the effectiveness of flooding on the removal of Se from dry surface sediments. The 83-m2 flood-experiment plot contained 10 monitoring wells, a water-quality minimonitor (continuous measurement of pH, specific conductance, water temperature, and dissolved O2), a down-hole Br electrode, and 2 pressure transducers. Flooding was initiated on August 27, 2002, and a Br tracer was added to water delivered through a pipeline to the flood plot during the first 1.2 h. Standing water depth in the flood plot was maintained at 0.3 m through September 1, 2002. The Br tracer data indicate a dual porosity system that includes fracture (mud cracks) and matrix flow components. Mean vertical water velocities for the matrix flow component were estimated to range from 0.002 to 0.012 m/h. Dissolved (less than 0.45 ??m) Se increased from pre-flood concentrations of less than 10 ??g/L to greater than 800 ??g/L during flooding in samples from deep (2.0 m below land surface) ground water. Selenium concentrations exceeded 5500 ??g/L in samples from shallow (0.8 m below land surface) ground water. Ratios of Se to Br in water samples indicate that Se moved conservatively during the experiment and was derived from leaching of near-surface sediments. Cumulative Se flux to the deep ground water during the experiment ranged from 9.0 to 170 mg/m2. Pre- and post-flood surface soil sampling indicated a mean Se flux of 720 mg/m2 through the top 15 cm of soil. Ground-water samples collected 8 months after termination of the flood experiment contained Se concentrations of less than 20 ??g/L. The minimonitor data indicate a rapid return to chemically reducing conditions in the deep ground water, limiting the mobility of the Se dissolved in the water pulse introduced during the flood experiment. Ratios of Se to Br in deep ground-water samples collected 8 months after the experiment confirmed the removal of Se from the aqueous phase. Based on the median Se flux rate estimated during the experiment of 0.65 mg/h/m2 (n = 52), 7 flooding cycles would be required to meet the 4 ??g/g remediation goal in surface soils from the SLWMA wetland.

Influence of Selenization Time on Microstructural, Optical, and Electrical Properties of Cu2ZnGeSe4 Films

NASA Astrophysics Data System (ADS)

Swapna Mary, G.; Hema Chandra, G.; Anantha Sunil, M.; Gupta, Mukul

2018-01-01

We have studied the effects of selenization time on the microstructural, optical, and electrical properties of stacked (Cu/Se/ZnSe/Se/Ge/Se) × 4 layers to demonstrate growth of Cu2ZnGeSe4 (CZGSe) thin films. Electron beam evaporation was used to deposit CZGSe films on glass substrates for selenization in high vacuum at 450°C for different times (15 min, 30 min, 45 min, and 60 min). The incomplete reaction of the precursor layers necessitates selenization at higher temperature for different durations to achieve desirable microstructural and optoelectronic properties. Energy-dispersive spectroscopic measurements revealed that the stacked layers selenized at 450°C for 30 min were nearly stoichiometric with atomic ratios of Cu/(Zn + Ge) = 0.88, Zn/Ge = 1.11, and Se/(Cu + Zn + Ge) = 1.03. X-ray diffraction analysis revealed that the stacks selenized at 450°C for 30 min crystallized in tetragonal stannite structure. Selenization-time-dependent Raman measurements of the selenized stacks are systematically presented to understand the growth of CZGSe. The elemental distribution through depth as a function of selenization time was investigated using secondary-ion mass spectroscopy. The ionic valency of the constituent elements in CZGSe films selenized at 450°C for 30 min was examined using high-resolution x-ray photoelectron spectroscopy. Significant changes were observed in the surface morphology of the stacked layers with increase in selenization time. The effects of defects on the electrical properties and of binary phases on the optical properties are discussed.

The Potential for Launching a Postgraduate Course on Sustainable Energy in Saudi Arabia

ERIC Educational Resources Information Center

Taleb, Hanan M.

2014-01-01

The pressures of a growing global population, compounded by environmental degradation, escalating energy use and the depletion of natural energy resources, have led to sustainable energy (SE) holding a prominent position on the international agenda. In spite of the widespread recognition of the important role of SE education in securing a…

Distribution of soil selenium in China is potentially controlled by deposition and volatilization?

PubMed Central

Sun, Guo-Xin; Meharg, Andrew A.; Li, Gang; Chen, Zheng; Yang, Lei; Chen, Song-Can; Zhu, Yong-Guan

2016-01-01

Elucidating the environmental drivers of selenium (Se) spatial distribution in soils at a continental scale is essential to better understand it’s biogeochemical cycling to improve Se transfer into diets. Through modelling Se biogeochemistry in China we found that deposition and volatilization are key factors controlling distribution in surface soil, rather than bedrock-derived Se (<0.1 mg/kg). Wet deposition associated with the East Asian summer monsoon, and dry deposition associated with the East Asian winter monsoon, are responsible for dominant Se inputs into northwest and southeast China, respectively. In Central China the rate of soil Se volatilization is similar to that of Se deposition, suggesting that Se volatilization offsets it’s deposition, resulting in negligible net Se input in soil. Selenium in surface soil at Central China is roughly equal to low petrogenic Se, which is the main reason for the presence of the Se poor belt. We suggest that both deposition and volatilization of Se could play a key role in Se balance in other terrestrial environments worldwide. PMID:26883576

Energy, angular and spatial distributions of primary electrons inside photoconducting materials for digital mammography: Monte Carlo simulation studies.

PubMed

Sakellaris, T; Spyrou, G; Tzanakos, G; Panayiotakis, G

2007-11-07

Materials such as a-Se, a-As(2)Se(3), GaSe, GaAs, Ge, CdTe, CdZnTe, Cd(0.8)Zn(0.2)Te, ZnTe, PbO, TlBr, PbI(2) and HgI(2) are potential candidates as photoconductors in direct detectors for digital mammography. The x-ray induced primary electrons inside a photoconductor's bulk comprise the initial signal that propagates and forms the final signal (image) on the detector's electrodes. An already developed model for a-Se has been properly extended to simulate the primary electron production in the materials mentioned. Primary electron characteristics, such as their energy, angular and spatial distributions that strongly influence the characteristics of the final image, were studied for both monoenergetic and polyenergetic x-ray spectra in the mammographic energy range. The characteristic feature in the electron energy distributions for PbI(2) and HgI(2) is the atomic deexcitation peaks, whereas for the rest of the materials their shape can also be influenced by the electrons produced from primary photons. The electrons have a small tendency to be forward ejected whereas they prefer to be ejected perpendicular (theta = pi/2) to the incident beam's axis and at two lobes around phi = 0 and phi = pi. At practical mammographic energies (15-40 keV) a-Se, a-As(2)Se(3) and Ge have the minimum azimuthal uniformity whereas CdZnTe, Cd(0.8)Zn(0.2)Te and CdTe the maximum one. The spatial distributions for a-Se, a-As(2)Se(3), GaSe, GaAs, Ge, PbO and TlBr are almost independent of the polyenergetic spectrum, while those for CdTe, CdZnTe, Cd(0.8)Zn(0.2)Te, ZnTe, PbI(2) and HgI(2) have a spectrum dependence. In the practical mammographic energy range and at this primitive stage of primary electron production, a-Se has the best inherent spatial resolution as compared to the rest of the photoconductors. PbO has the minimum bulk space in which electrons can be produced whereas CdTe has the maximum one.

Materials Design of the Codoping for the Fabrication of Low-Resistivity p-Type ZnSe and GaN by ab-initio Electronic Structure Calculation

NASA Astrophysics Data System (ADS)

Katayama-Yoshida, H.; Yamamoto, T.

1997-08-01

We propose an effective doping method, the codoping (doping with n- and p-type dopants at the same time) method, for the fabrication of low-resistivity p-type ZnSe and GaN with wide-band-gap based upon ab-initio electronic band structure calculations. p-type doping eminently leads to an increase in the electrostatic energy, called the Madelung energy, which shifts the Se 4p levels for p-type doped ZnSe and the N 2p levels for p-type doped GaN materials towards higher energy regions. This leads to a destabilization of ionic charge distributions in p-type ZnSe and p-type GaN crystals, resulting in the self-compensation of anion intrinsic defects. For ZnSe crystals, we propose the codoping of n-type In donors at Zn sites and p-type N acceptors at Se sites based on the calculation. In addition, we propose the codoping of n-type Si-donors at Ga sites (n-type O donors at N sites) and p-type Be- or Mg acceptors at Ga sites. The codoping decreases the Madelung energy and leads to an increase in the net acceptor carrier density.

Spectroscopic investigation of the chemical and electronic properties of chalcogenide materials for thin-film optoelectronic devices

NASA Astrophysics Data System (ADS)

Horsley, Kimberly Anne

Chalcogen-based materials are at the forefront of technologies for sustainable energy production. This progress has come only from decades of research, and further investigation is needed to continue improvement of these materials. For this dissertation, a number of chalcogenide systems were studied, which have applications in optoelectronic devices, such as LEDs and Photovoltaics. The systems studied include Cu(In,Ga)Se2 (CIGSe) and CuInSe 2 (CISe) thin-film absorbers, CdTe-based photovoltaic structures, and CdTe-ZnO nanocomposite materials. For each project, a sample set was prepared through collaboration with outside institutions, and a suite of spectroscopy techniques was employed to answer specific questions about the system. These techniques enabled the investigation of the chemical and electronic structure of the materials, both at the surface and towards the bulk. CdS/Cu(In,Ga)Se2 thin-films produced from the roll-to-roll, ambient pressure, Nanosolar industrial line were studied. While record-breaking efficiency cells are usually prepared in high-vacuum (HV) or ultra-high vacuum (UHV) environments, these samples demonstrate competitive mass-production efficiency without the high-cost deposition environment. We found relatively low levels of C contaminants, limited Na and Se oxidation, and a S-Se intermixing at the CdS/CIGSe interface. The surface band gap compared closely to previously investigated CIGSe thin-films deposited under vacuum, illustrating that roll-to-roll processing is a promising and less-expensive alternative for solar cell production. An alternative deposition process for CuInSe2 was also studied, in collaboration with the University of Luxembourg. CuInSe2 absorbers were prepared with varying Cu content and surface treatments to investigate the potential to produce an absorber with a Cu-rich bulk and Cu-poor surface. This is desired to combine the bulk characteristics of reduced defects and larger grains in Cu-rich films, while maintaining a wide surface band gap, as seen in Cu-poor films. A novel absorber was prepared Cu-rich with a final In-Se treatment to produce a Cu-poor surface, and compared directly to Cu-poor and Cu-rich produced samples. Despite reduced Cu at the surface, the novel absorber was found to have a surface band gap similar to that of traditional, Cu-poor grown absorbers. Furthermore, estimation of the near-surface bulk band gap suggests a narrowing of the band gap away from the surface, similar to highly efficient, Cu-poor grown absorbers. Long-term degradation is another concern facing solar cells, as heat and moistures stress can result in reduced efficiencies over time. The interface of the back contact material and absorber layer in (Au/Cu)/CdTe/CdS thin-film structures from the University of Toledo were investigated after a variety of accelerated stress treatments with the aim of further understanding the chemical and/or electronic degradation of this interface. Sulfur migration to the back contact was observed, along with the formation of Au-S and Cu-S bonds. A correlation between heat stress under illumination and the formation of Cu-Cl bonds was also found. Nanocomposite materials hold promise as a next-generation photovoltaic material and for use in LED devices, due in part to the unique ability to tune the absorption edge of the film by adjusting the semiconductor particle size, and the prospective for long-range charge-carrier (exciton) transport through the wide band gap matrix material. Thin films of CdTe were sputter deposited onto ZnO substrates at the University of Arizona and studied before and after a short, high temperature annealing to further understand the effects of annealing on the CdTe/ZnO interface. A clumping of the CdTe layer and the formation of Cd- and Te-oxides was observed using surface microscopy and photoelectron spectroscopy techniques. These findings help to evaluate post-deposition annealing as a treatment to adjust the final crystallinity and optoelectronic properties of these films. Through publication and/or discussion with collaborators, each project presented in this dissertation contributed to the understanding of the chemical and electronic properties of the material surface, near-surface bulk, and/or interfaces formed. The information gained on these unique chalcogenide materials will assist in designing more efficient and successful optoelectronic devices for the next generation of solar cells and LEDs.

Surfactant-Free Aqueous Synthesis of Pure Single-Crystalline SnSe Nanosheet Clusters as Anode for High Energy- and Power-Density Sodium-Ion Batteries.

PubMed

Yuan, Shuang; Zhu, Yun-Hai; Li, Wang; Wang, Sai; Xu, Dan; Li, Lin; Zhang, Yu; Zhang, Xin-Bo

2017-01-01

SnSe with 3D hierarchical nanostructure composed of interconnected single-crystal SnSe nanosheets is synthesized via a fast and effective strategy. Unexpectedly, when used as the anode material for Na-ion batteries (NIBs), the SnSe exhibits a high capacity (738 mA h g -1 ), superior rate capability (40 A g -1 ), and high energy density in a full cell. These results provide the possibility of SnSe use as NIBs anodes. © 2016 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Hot-electron-mediated surface chemistry: toward electronic control of catalytic activity.

PubMed

Park, Jeong Young; Kim, Sun Mi; Lee, Hyosun; Nedrygailov, Ievgen I

2015-08-18

Energy dissipation at surfaces and interfaces is mediated by excitation of elementary processes, including phonons and electronic excitation, once external energy is deposited to the surface during exothermic chemical processes. Nonadiabatic electronic excitation in exothermic catalytic reactions results in the flow of energetic electrons with an energy of 1-3 eV when chemical energy is converted to electron flow on a short (femtosecond) time scale before atomic vibration adiabatically dissipates the energy (in picoseconds). These energetic electrons that are not in thermal equilibrium with the metal atoms are called "hot electrons". The detection of hot electron flow under atomic or molecular processes and understanding its role in chemical reactions have been major topics in surface chemistry. Recent studies have demonstrated electronic excitation produced during atomic or molecular processes on surfaces, and the influence of hot electrons on atomic and molecular processes. We outline research efforts aimed at identification of the intrinsic relation between the flow of hot electrons and catalytic reactions. We show various strategies for detection and use of hot electrons generated by the energy dissipation processes in surface chemical reactions and photon absorption. A Schottky barrier localized at the metal-oxide interface of either catalytic nanodiodes or hybrid nanocatalysts allows hot electrons to irreversibly transport through the interface. We show that the chemicurrent, composed of hot electrons excited by the surface reaction of CO oxidation or hydrogen oxidation, correlates well with the turnover rate measured separately by gas chromatography. Furthermore, we show that hot electron flows generated on a gold thin film by photon absorption (or internal photoemission) can be amplified by localized surface plasmon resonance. The influence of hot charge carriers on the chemistry at the metal-oxide interface are discussed for the cases of Au, Ag, and Pt nanoparticles on oxide supports and Pt-CdSe-Pt nanodumbbells. We show that the accumulation or depletion of hot electrons on metal nanoparticles, in turn, can also influence catalytic reactions. Mechanisms suggested for hot-electron-induced chemical reactions on a photoexcited plasmonic metal are discussed. We propose that the manipulation of the flow of hot electrons by changing the electrical characteristics of metal-oxide and metal-semiconductor interfaces can give rise to the intriguing capability of tuning the catalytic activity of hybrid nanocatalysts.

The influence of sequence of precursor films on CZTSe thin films prepared by ion-beam sputtering deposition

NASA Astrophysics Data System (ADS)

Zhao, Jun; Liang, Guangxing; Zeng, Yang; Fan, Ping; Hu, Juguang; Luo, Jingting; Zhang, Dongping

2017-02-01

The CuZnSn (CZT) precursor thin films are grown by ion-beam sputtering Cu, Zn, Sn targets with different orders and then sputtering Se target to fabricate Cu2ZnSnSe4 (CZTSe) absorber thin films on molybdenum substrates. They are annealed in the same vacuum chamber at 400 °C. The characterization methods of CZTSe thin films include X-ray diffraction (XRD), energy dispersive spectroscopy (EDS), scanning electron microscopy (SEM), and X-ray photoelectron spectra (XPS) in order to study the crystallographic properties, composition, surface morphology, electrical properties and so on. The results display that the CZTSe thin films got the strongest diffraction peak intensity and were with good crystalline quality and its morphology appeared smooth and compact with a sequence of Cu/Zn/Sn/Se, which reveals that the expected states for CZTSe are Cu1+, Zn2+, Sn4+, Se2+. With the good crystalline quality and close to ideal stoichiometric ratio the resistivity of the CZTSe film with the sequence of Cu/Zn/Sn/Se is lower, whose optical band gap is about 1.50 eV. Project supported by the National Natural Science Foundation of China (No. 61404086), the Basical Research Program of Shenzhen (Nos. JCYJ20150324140036866, JCYJ20150324141711581), and the Natural Science Foundation of SZU (No. 2014017).

Skin denervation does not alter cortical potentials to surface concentric electrode stimulation: A comparison with laser evoked potentials and contact heat evoked potentials.

PubMed

La Cesa, S; Di Stefano, G; Leone, C; Pepe, A; Galosi, E; Alu, F; Fasolino, A; Cruccu, G; Valeriani, M; Truini, A

2018-01-01

In the neurophysiological assessment of patients with neuropathic pain, laser evoked potentials (LEPs), contact heat evoked potentials (CHEPs) and the evoked potentials by the intraepidermal electrical stimulation via concentric needle electrode are widely agreed as nociceptive specific responses; conversely, the nociceptive specificity of evoked potentials by surface concentric electrode (SE-PREPs) is still debated. In this neurophysiological study we aimed at verifying the nociceptive specificity of SE-PREPs. We recorded LEPs, CHEPs and SE-PREPs in eleven healthy participants, before and after epidermal denervation produced by prolonged capsaicin application. We also used skin biopsy to verify the capsaicin-induced nociceptive nerve fibre loss in the epidermis. We found that whereas LEPs and CHEPs were suppressed after capsaicin-induced epidermal denervation, the surface concentric electrode stimulation of the same denervated skin area yielded unchanged SE-PREPs. The suppression of LEPs and CHEPs after nociceptive nerve fibre loss in the epidermis indicates that these techniques are selectively mediated by nociceptive system. Conversely, the lack of SE-PREP changes suggests that SE-PREPs do not provide selective information on nociceptive system function. Capsaicin-induced epidermal denervation abolishes laser evoked potentials (LEPs) and contact heat evoked potentials (CHEPs), but leaves unaffected pain-related evoked potentials by surface concentric electrode (SE-PREPs). These findings suggest that unlike LEPs and CHEPs, SE-PREPs are not selectively mediated by nociceptive system. © 2017 European Pain Federation - EFIC®.

Synthesis, Surface Studies, Composition and Structural Characterization of CdSe, Core/Shell, and Biologically Active Nanocrystals

PubMed Central

Rosenthal, Sandra J.; McBride, James; Pennycook, Stephen J.; Feldman, Leonard C.

2011-01-01

Nanostructures, with their very large surface to volume ratio and their non-planar geometry, present an important challenge to surface scientists. New issues arise as to surface characterization, quantification and interface formation. This review summarizes the current state of the art in the synthesis, composition, surface and interface control of CdSe nanocrystal systems, one of the most studied and useful nanostructures. PMID:21479151

Pressure-induced increase of exciton-LO-phonon coupling in a ZnCdSe/ZnSe quantum well

NASA Astrophysics Data System (ADS)

Guo, Z. Z.; Liang, X. X.; Ban, S. L.

2003-07-01

The possibility of pressure-induced increase of exciton-LO-phonon coupling in ZnCdSe/ZnSe quantum wells is studied. The ground state binding energies of the heavy hole excitons are calculated using a variational method with consideration of the electron-phonon interaction and the pressure dependence of the parameters. The results show that for quantum wells with intermediate well width, the exciton binding energy and the LO-phonon energy may coincide in the course of pressure increasing, resulting in the increase of exciton-LO-phonon coupling. It is also found that among the pressure-dependent parameters, the influence of the lattice constant is the most important one. The changes of both the effective masses and the dielectric constants have obvious effects on the exciton binding energy, but their influences are counterbalanced.

A stable lithiated silicon-chalcogen battery via synergetic chemical coupling between silicon and selenium.

PubMed

Eom, KwangSup; Lee, Jung Tae; Oschatz, Martin; Wu, Feixiang; Kaskel, Stefan; Yushin, Gleb; Fuller, Thomas F

2017-01-05

Li-ion batteries dominate portable energy storage due to their exceptional power and energy characteristics. Yet, various consumer devices and electric vehicles demand higher specific energy and power with longer cycle life. Here we report a full-cell battery that contains a lithiated Si/graphene anode paired with a selenium disulfide (SeS 2 ) cathode with high capacity and long-term stability. Selenium, which dissolves from the SeS 2 cathode, was found to become a component of the anode solid electrolyte interphase (SEI), leading to a significant increase of the SEI conductivity and stability. Moreover, the replacement of lithium metal anode impedes unwanted side reactions between the dissolved intermediate products from the SeS 2 cathode and lithium metal and eliminates lithium dendrite formation. As a result, the capacity retention of the lithiated silicon/graphene-SeS 2 full cell is 81% after 1,500 cycles at 268 mA g SeS2 -1 . The achieved cathode capacity is 403 mAh g SeS2 -1 (1,209 mAh cm SeS2 -3 ).

Status of photoelectrochemical production of hydrogen and electrical energy

NASA Technical Reports Server (NTRS)

Byvik, C. E.; Walker, G. H.

1976-01-01

The efficiency for conversion of electromagnetic energy to chemical and electrical energy utilizing semiconductor single crystals as photoanodes in electrochemical cells was investigated. Efficiencies as high as 20 percent were achieved for the conversion of 330 nm radiation to chemical energy in the form of hydrogen by the photoelectrolysis of water in a SrTiO3 based cell. The SrTiO3 photoanodes were shown to be stable in 9.5 M NaOH solutions for periods up to 48 hours. Efficiencies of 9 percent were measured for the conversion of broadband visible radiation to hydrogen using n-type GaAs crystals as photoanodes. Crystals of GaAs coated with 500 nm of gold, silver, or tin for surface passivation show no significant change in efficiency. By suppressing the production of hydrogen in a CdSe-based photogalvanic cell, an efficiency of 9 percent was obtained in conversion of 633 nm light to electrical energy. A CdS-based photogalvanic cell produced a conversion efficiency of 5 percent for 500 nm radiation.

Understanding the electronic structure of CdSe quantum dot-fullerene (C{sub 60}) hybrid nanostructure for photovoltaic applications

DOE Office of Scientific and Technical Information (OSTI.GOV)

Sarkar, Sunandan; Rajbanshi, Biplab; Sarkar, Pranab, E-mail: pranab.sarkar@visva-bharati.ac.in

2014-09-21

By using the density-functional tight binding method, we studied the electronic structure of CdSe quantum dot(QD)-buckminsterfullerene (C{sub 60}) hybrid systems as a function of both the size of the QD and concentration of the fullerene molecule. Our calculation reveals that the lowest unoccupied molecular orbital energy level of the hybrid CdSeQD-C{sub 60} systems lies on the fullerene moiety, whereas the highest occupied molecular orbital (HOMO) energy level lies either on the QD or the fullerene depending on size of the CdSe QD. We explored the possibility of engineering the energy level alignment by varying the size of the CdSe QD.more » With increase in size of the QD, the HOMO level is shifted upward and crosses the HOMO level of the C{sub 60}-thiol molecule resulting transition from the type-I to type-II band energy alignment. The density of states and charge density plot support these types of band gap engineering of the CdSe-C{sub 60} hybrid systems. This type II band alignment indicates the possibility of application of this nanohybrid for photovoltaic purpose.« less

Dual Signal Amplification Using Gold Nanoparticles-Enhanced Zinc Selenide Nanoflakes and P19 Protein for Ultrasensitive Photoelectrochemical Biosensing of MicroRNA in Cell.

PubMed

Tu, Wenwen; Cao, Huijuan; Zhang, Long; Bao, Jianchun; Liu, Xuhui; Dai, Zhihui

2016-11-01

Using Au nanoparticles (NPs)-decorated, water-soluble, ZnSe-COOH nanoflakes (NFs), an ultrasensitive photoelectrochemical (PEC) biosensing strategy based on the dual signal amplification was proposed. As a result of the localized surface plasmon resonance (SPR) of Au NPs, the ultraviolet-visible absorption spectrum of Au NPs overlapped with emission spectrum of ZnSe-COOH NFs, which generated efficient resonant energy transfer (RET) between ZnSe-COOH NFs and Au NPs. The RET improved photoelectric conversion efficiency of ZnSe-COOH NFs and significantly amplified PEC signal. Taking advantage of the specificity and high affinity of p19 protein for 21-23 bp double-stranded RNA, p19 protein was introduced. P19 protein could generate remarkable steric hindrance, which blocked interfacial electron transfer and impeded the access of the ascorbic acid to electrode surface for scavenging holes. This led to the dramatic decrease of photocurrent intensity and the amplification of PEC signal change versus concentration change of target. Using microRNA (miRNA)-122a as a model analyte, an ultrasensitive signal-off PEC biosensor for miRNA detection was developed under 405 nm irradiation at -0.30 V. Owing to RET and remarkable steric hindrance of p19 protein as dual signal amplification, the proposed strategy exhibited a wide linear range from 350 fM to 5 nM, with a low detection limit of 153 fM. It has been successfully applied to analyze the level of miRNA-122a in HeLa cell, which would have promising prospects for early diagnosis of tumor.

Dimensionality of nanoscale TiO 2 determines the mechanism of photoinduced electron injection from a CdSe nanoparticle

DOE PAGES

Tafen, De Nyago; Long, Run; Prezhdo, Oleg V.

2014-03-10

Assumptions about electron transfer (ET) mechanisms guide design of catalytic, photovoltaic, and electronic systems. We demonstrate that the mechanism of ET from a CdSe quantum dot (QD) into nanoscale TiO 2 depends on TiO 2 dimensionality. The injection into a TiO 2 QD is adiabatic due to strong donor–acceptor coupling, arising from unsaturated chemical bonds on the QD surface, and low density of acceptor states. In contrast, the injection into a TiO 2 nanobelt (NB) is nonadiabatic, because the state density is high, the donor–acceptor coupling is weak, and multiple phonons accommodate changes in the electronic energy. The CdSe adsorbantmore » breaks symmetry of delocalized TiO 2 NB states, relaxing coupling selection rules, and generating more ET channels. Both mechanisms can give efficient ultrafast injection. Furthermore, the dependence on system properties is very different for the two mechanisms, demonstrating that the fundamental principles leading to efficient charge separation depend strongly on the type of nanoscale material.« less

Dimensionality of nanoscale TiO 2 determines the mechanism of photoinduced electron injection from a CdSe nanoparticle

DOE Office of Scientific and Technical Information (OSTI.GOV)

Tafen, De Nyago; Long, Run; Prezhdo, Oleg V.

Assumptions about electron transfer (ET) mechanisms guide design of catalytic, photovoltaic, and electronic systems. We demonstrate that the mechanism of ET from a CdSe quantum dot (QD) into nanoscale TiO 2 depends on TiO 2 dimensionality. The injection into a TiO 2 QD is adiabatic due to strong donor–acceptor coupling, arising from unsaturated chemical bonds on the QD surface, and low density of acceptor states. In contrast, the injection into a TiO 2 nanobelt (NB) is nonadiabatic, because the state density is high, the donor–acceptor coupling is weak, and multiple phonons accommodate changes in the electronic energy. The CdSe adsorbantmore » breaks symmetry of delocalized TiO 2 NB states, relaxing coupling selection rules, and generating more ET channels. Both mechanisms can give efficient ultrafast injection. Furthermore, the dependence on system properties is very different for the two mechanisms, demonstrating that the fundamental principles leading to efficient charge separation depend strongly on the type of nanoscale material.« less

Quasiparticle interference, quasiparticle interactions, and the origin of the charge density wave in 2 H – NbSe 2

DOE PAGES

Arguello, C. J.; Rosenthal, E. P.; Andrade, E. F.; ...

2015-01-21

We show that a small number of intentionally introduced defects can be used as a spectroscopic tool to amplify quasiparticle interference in 2H-NbSe₂ that we measure by scanning tunneling spectroscopic imaging. We show, from the momentum and energy dependence of the quasiparticle interference, that Fermi surface nesting is inconsequential to charge density wave formation in 2H-NbSe₂. We demonstrate that, by combining quasiparticle interference data with additional knowledge of the quasiparticle band structure from angle resolved photoemission measurements, one can extract the wave vector and energy dependence of the important electronic scattering processes thereby obtaining direct information both about the fermiologymore » and the interactions. In 2H-NbSe₂, we use this combination to confirm that the important near-Fermi-surface electronic physics is dominated by the coupling of the quasiparticles to soft mode phonons at a wave vector different from the charge density wave ordering wave vector.« less

Nonlinear optical effects in a three-nanolayer metal sandwich assembly

NASA Astrophysics Data System (ADS)

Khmelinskii, Igor; Makarov, Vladimir I.

2018-04-01

We report spectral properties and frequency summing that induce superemission (SE) in sandwich structures built of Co nanolayers. We found that separate Co films with a layer thickness of 8.1, 9.2, and 11.3 nm have discrete absorption spectra, originating in transverse quantum confinement in such thin metal films. The surface plasmon resonance in this system should appear at energies over 50 000 cm-1, with its longer-wavelength tail easily observable. All of the nanolayers studied also presented discrete emission spectra, with the emission bands strongly overlapping due to large bandwidths (1500-2300 cm-1). The emission decay is described by a single-exponential function with the lifetime of 103±5 ns. Similarly, the sandwich assembly with three Co nanolayers separated by two BN nanolayers also has discrete lines in its absorption spectrum. The spectrum of the assembly is a superposition of the respective spectra of the individual Co layers. We report that the assembly can sum the pumping radiation photons, producing photons with a higher energy. This excitation summing/exciton joining effect, discovered in sandwich film systems, is reported for the first time. Exiting the two outside Co nanolayers at specific frequencies, the Co nanolayer in the middle produces the sum frequency. We identified this emission as SE, with a bandwidth of only 179±5 cm-1. This superemission band appeared with the rise time of 36±3 ns and disappeared with 73±5 ns decay time, with the estimated SE quantum yield of 0.063. We analyzed the energy transfer by the exchange mechanism in detail, although a contribution of the electric dipole-dipole mechanism could not be excluded.

Nanophotonics with Surface Enhanced Coherent Raman Microscopy

NASA Astrophysics Data System (ADS)

Fast, Alexander

Nonlinear nanophotonics is a rapidly developing field of research that aims at detecting and disentangling weak congested optical signatures on the nanoscale. Sub-wavelength field confinement of the local electromagnetic fields and the resulting field enhancement is achieved by utilizing plasmonic near-field antennas. This allows for probing nanoscopic volumes, a property unattainable by conventional far-field microscopy techniques. Combination of plasmonics and nonlinear optical microscopy provides a path to visualizing a small chemical and spatial subset of target molecules within an ensemble. This is achieved while maintaining rapid signal acquisition, which is necessary for capturing biological processes in living systems. Herein, a novel technique, wide-field surface enhanced coherent anti-Stokes Raman scattering (wfSE-CARS) is presented. This technique allows for isolating weak vibrational signals in nanoscopic proximity to the surface by using chemical sensitivity of coherent Raman microspectroscopy (CRM) and field confinement from surface plasmons supported on a thin gold film. Uniform field enhancement over a large field of view, achieved with surface plasmon polaritons (SPP) in wfSE-CARSS, allows for biomolecular imaging demonstrated on extended structures like phospholipid droplets and live cells. Surface selectivity and chemical contrast are achieved at 70 fJ/mum2 incident energy densities, which is over five orders of magnitude lower than used in conventional point scanning CRM. Next, a novel surface sensing imaging technique, local field induced metal emission (LFIME), is introduced. Presence of a sample material at the surface influences the local fields of a thin flat gold film, such that nonlinear fluorescence signal of the metal can be detected in the far-field. Nanoscale nonmetallic, nonfluorescent objects can be imaged with high signal-to-background ratio and diffraction limited lateral resolution using LFIME. Additionally, structure of the extended samples' surfaces can be visualized with a nanoscale axial resolution providing topographic information. Finally, a platform for coherently interrogating single molecules is presented. Single-molecule limit SE-CARS on non-resonant molecules is achieved by means of 3D local field confinement in the nanojunctions between two spherical gold nanoparticles. Localized plasmon resonance of the dimer nanostructure confines the probe volume down to 1 nm3 and provides the local field enhancement necessary to reach single-molecule detection limit. Nonlinear excitation of Raman vibrations in SE-CARS microspectroscopy allows for higher image acquisition rates than in conventionally used single-molecule surface enhanced Raman spectroscopy (SERS). Therefore, data throughput is significantly improved while preserving spectral information despite the presence of the metal. Data simultaneously acquired from hundreds of nanoantennas allows to establish the peak enhancement factor from the observed count rates and define the maximum allowed local-field that preserves the integrity of the antenna. These results are paramount for the future design of time resolved single-molecule studies with multiple pulsed laser excitations, required for single-molecule coherence manipulation and quantum computing.

Record surface state mobility and quantum Hall effect in topological insulator thin films via interface engineering

DOE PAGES

Koirala, Nikesh; Han, Myung -Geun; Brahlek, Matthew; ...

2015-11-19

Material defects remain as the main bottleneck to the progress of topological insulators (TIs). In particular, efforts to achieve thin TI samples with dominant surface transport have always led to increased defects and degraded mobilities, thus making it difficult to probe the quantum regime of the topological surface states. Here, by utilizing a novel buffer layer scheme composed of an In 2Se 3/(Bi 0.5In 0.5) 2Se 3 heterostructure, we introduce a quantum generation of Bi 2Se 3 films with an order of magnitude enhanced mobilities than before. Furthermore, this scheme has led to the first observation of the quantum Hallmore » effect in Bi 2Se 3.« less

Influence of light intensity on surface free energy and dentin bond strength of core build-up resins.

PubMed

Shimizu, Y; Tsujimoto, A; Furuichi, T; Suzuki, T; Tsubota, K; Miyazaki, M; Platt, J A

2015-01-01

We examined the influence of light intensity on surface free energy characteristics and dentin bond strength of dual-cure direct core build-up resin systems. Two commercially available dual-cure direct core build-up resin systems, Clearfil DC Core Automix with Clearfil Bond SE One and UniFil Core EM with Self-Etching Bond, were studied. Bovine mandibular incisors were mounted in acrylic resin and the facial dentin surfaces were wet ground on 600-grit silicon carbide paper. Adhesives were applied to dentin surfaces and cured with light intensities of 0 (no irradiation), 200, 400, and 600 mW/cm(2). The surface free energy of the adhesives (five samples per group) was determined by measuring the contact angles of three test liquids placed on the cured adhesives. To determine the strength of the dentin bond, the core build-up resin pastes were condensed into the mold on the adhesive-treated dentin surfaces according to the methods described for the surface free energy measurement. The resin pastes were cured with the same light intensities as those used for the adhesives. Ten specimens per group were stored in water maintained at 37°C for 24 hours, after which they were shear tested at a crosshead speed of 1.0 mm/minute in a universal testing machine. Two-way analysis of variance (ANOVA) and a Tukey-Kramer test were performed, with the significance level set at 0.05. The surface free energies of the adhesive-treated dentin surfaces decreased with an increase in the light intensity of the curing unit. Two-way ANOVA revealed that the type of core build-up system and the light intensity significantly influence the bond strength, although there was no significant interaction between the two factors. The highest bond strengths were achieved when the resin pastes were cured with the strongest light intensity for all the core build-up systems. When polymerized with a light intensity of 200 mW/cm(2) or less, significantly lower bond strengths were observed. CONClUSIONS: The data suggest that the dentin bond strength of core build-up systems are still affected by the light intensity of the curing unit, which is based on the surface free energy of the adhesives. On the basis of the results and limitations of the test conditions used in this study, it appears that a light intensity of >400 mW/cm(2) may be required for achieving the optimal dentin bond strength.

Synchronized energy and electron transfer processes in covalently linked CdSe-squaraine dye-TiO2 light harvesting assembly.

PubMed

Choi, Hyunbong; Santra, Pralay K; Kamat, Prashant V

2012-06-26

Manipulation of energy and electron transfer processes in a light harvesting assembly is an important criterion to mimic natural photosynthesis. We have now succeeded in sequentially assembling CdSe quantum dot (QD) and squaraine dye (SQSH) on TiO(2) film and couple energy and electron transfer processes to generate photocurrent in a hybrid solar cell. When attached separately, both CdSe QDs and SQSH inject electrons into TiO(2) under visible-near-IR irradiation. However, CdSe QD if linked to TiO(2) with SQSH linker participates in an energy transfer process. The hybrid solar cells prepared with squaraine dye as a linker between CdSe QD and TiO(2) exhibited power conversion efficiency of 3.65% and good stability during illumination with global AM 1.5 solar condition. Transient absorption spectroscopy measurements provided further insight into the energy transfer between excited CdSe QD and SQSH (rate constant of 6.7 × 10(10) s(-1)) and interfacial electron transfer between excited SQSH and TiO(2) (rate constant of 1.2 × 10(11) s(-1)). The synergy of covalently linked semiconductor quantum dots and near-IR absorbing squaraine dye provides new opportunities to harvest photons from selective regions of the solar spectrum in an efficient manner.

Topological phase transition and unexpected mass acquisition of Dirac fermion in TlBi(S1-xSex)2

NASA Astrophysics Data System (ADS)

Niu, Chengwang; Dai, Ying; Zhu, Yingtao; Lu, Jibao; Ma, Yandong; Huang, Baibiao

2012-10-01

Based on first-principles calculations and effective Hamiltonian analysis, we predict a topological phase transition from normal to topological insulators and the opening of a gap without breaking the time-reversal symmetry in TlBi(S1-xSex)2. The transition can be driven by modulating the Se concentration, and the rescaled spin-orbit coupling and lattice parameters are the key ingredients for the transition. For topological surface states, the Dirac cone evolves differently as the explicit breaking of inversion symmetry and the energy band can be opened under asymmetry surface. Our results present theoretical evidence for experimental observations [Xu et al., Science 332, 560 (2011); Sato et al., Nat. Phys. 7, 840 (2011)].

Time-resolved photoluminescence study of CdSe/CdMnS/CdS core/multi-shell nanoplatelets

DOE Office of Scientific and Technical Information (OSTI.GOV)

Murphy, J. R.; Department of Physics, State University of New York, University at Buffalo, Buffalo, New York 14260; Delikanli, S.

2016-06-13

We used photoluminescence spectroscopy to resolve two emission features in CdSe/CdMnS/CdS and CdSe/CdS core/multi-shell nanoplatelet heterostructures. The photoluminescence from the magnetic sample has a positive circular polarization with a maximum centered at the position of the lower energy feature. The higher energy feature has a corresponding signature in the absorption spectrum; this is not the case for the low-energy feature. We have also studied the temporal evolution of these features using a pulsed-excitation/time-resolved photoluminescence technique to investigate their corresponding recombination channels. A model was used to analyze the temporal dynamics of the photoluminescence which yielded two distinct timescales associated withmore » these recombination channels. The above results indicate that the low-energy feature is associated with recombination of electrons with holes localized at the core/shell interfaces; the high-energy feature, on the other hand, is excitonic in nature with the holes confined within the CdSe cores.« less

Fermi surfaces of the pyrite-type cubic AuSb2 compared with split Fermi surfaces of the ullmannite-type cubic chiral NiSbS and PdBiSe

NASA Astrophysics Data System (ADS)

Nishimura, K.; Kakihana, M.; Nakamura, A.; Aoki, D.; Harima, H.; Hedo, M.; Nakama, T.; Ōnuki, Y.

2018-05-01

We grew high-quality single crystals of AuSb2 with the pyrite (FeS2)-type cubic structure by the Bridgman method and studied the Fermi surface properties by the de Haas-van Alphen (dHvA) experiment and the full potential LAPW band calculation. The Fermi surfaces of AuSb2 are found to be similar to those of NiSbS and PdBiSe with the ullmannite (NiSbS)-type cubic chiral structure because the crystal structures are similar each other and the number of valence electrons is the same between two different compounds. Note that each Fermi surface splits into two Fermi surfaces in NiSbS and PdBiSe, reflecting the non-centrosymmetric crystal structure.

Constrained Hartree-Fock Theory and Study of Deformed Structures of Closed Shell Nuclei

NASA Astrophysics Data System (ADS)

Praharaj, Choudhury

2016-03-01

We have studied some N or Z = 50 nuclei in a microscopic model with effective interaction in a reasonably large shell model space. Excitation of particles across 50 shell closure leads to well-deformed excited prolate configurations. The potential energy surfaces of nuclei are studied using Hartree-Fock theory with quadrupole constraint to explore the various deformed configurations of N = 50 nuclei 82Ge , 84Se and 86Kr . Energy spectra are calculated from various intrinsic states using Peierls-Yoccoz angular momentum projection technique. Results of spectra and electromagnetic moments and transitions will be presented for N = 50 nuclei and for Z = 50 114Sn nucleus. Supported by Grant No SB/S2/HEP-06/2013 of DST.

Phonon spectrum of single-crystalline FeSe probed by high-resolution electron energy-loss spectroscopy

NASA Astrophysics Data System (ADS)

Zakeri, Khalil; Engelhardt, Tobias; Le Tacon, Matthieu; Wolf, Thomas

2018-06-01

Utilizing high-resolution electron energy-loss spectroscopy (HREELS) we measure the phonon frequencies of β-FeSe(001), cleaved under ultra-high vacuum conditions. At the zone center (Γ bar-point) three prominent loss features are observed at loss energies of about ≃ 20.5 and 25.6 and 40 meV. Based on the scattering selection rules we assign the observed loss features to the A1g, B1g, and A2u phonon modes of β-FeSe(001). The experimentally measured phonon frequencies do not agree with the results of density functional based calculations in which a nonmagnetic, a checkerboard or a strip antiferromagnetic order is assumed for β-FeSe(001). Our measurements suggest that, similar to the other Fe-based materials, magnetism has a profound impact on the lattice dynamics of β-FeSe(001).

Molecular beam epitaxy of large-area SnSe2 with monolayer thickness fluctuation

NASA Astrophysics Data System (ADS)

Park, Young Woon; Jerng, Sahng-Kyoon; Jeon, Jae Ho; Roy, Sanjib Baran; Akbar, Kamran; Kim, Jeong; Sim, Yumin; Seong, Maeng-Je; Kim, Jung Hwa; Lee, Zonghoon; Kim, Minju; Yi, Yeonjin; Kim, Jinwoo; Noh, Do Young; Chun, Seung-Hyun

2017-03-01

The interest in layered materials is largely based on the expectation that they will be beneficial for a variety of applications, from low-power-consuming, wearable electronics to energy harvesting. However, the properties of layered materials are highly dependent on thickness, and the difficulty of controlling thickness over a large area has been a bottleneck for commercial applications. Here, we report layer-by-layer growth of SnSe2, a layered semiconducting material, via van der Waals epitaxy. The films were fabricated on insulating mica substrates with substrate temperatures in the range of 210 °C-370 °C. The surface consists of a mixture of N and (N ± 1) layers, showing that the thickness of the film can be defined with monolayer accuracy (±0.6 nm). High-resolution transmission electron microscopy reveals a polycrystalline film with a grain size of ˜100 nm and clear Moiré patterns from overlapped grains with similar thickness. We also report field effect mobility values of 3.7 cm2 V-1 s-1 and 6.7 cm2 V-1 s-1 for 11 and 22 nm thick SnSe2, respectively. SnSe2 films with customizable thickness can provide valuable platforms for industry and academic researchers to fully exploit the potential of layered materials.

Atomistic simulations of activated processes in nanoparticles synthesis

NASA Astrophysics Data System (ADS)

Giberti, Federico; Galli, Giulia

Core-shell and Janus nanopartices are promising building blocks for new, highly efficient solar cells. One of the most common synthetic pathways to produce such nanostructures is the use of cation exchange reactions. Although widely used, these procedures are not completely understood. We employed classical Molecular Dynamics and Monte Carlo simulations to understand these transformation at the molecular level; in particular we investigated the conversion from CdSe (sphalerite) to PbSe (rocksalt) NPs with 2-3 nm diameter. In order to recover the equilibrium free energy surfaces we used state of the art enhanced sampling techniques, including Metadynamics. The formation of hybrid core-shell structures resulted to be an activated process, where the limiting step is the transition of a sphalerite to a rocksalt PbSe nucleus. We found that the barrier height and the stability of the two phases depend on the size of the PbSe nucleus, suggesting that the process could proceed via a two step mechanism, where a small sphalerite nucleus is formed first, and it then transforms to a rocksalt nucleus. Our results give insight into possible manipulation processes at the molecular scale, which could be used to stabilize metastable NPs and tune their physical and chemical properties. This work was supported by the DOE Grant No. DE-FG02-06ER46262.

Few-Layer MoSe2 Possessing High Catalytic Activity towards Iodide/Tri-iodide Redox Shuttles

PubMed Central

Lee, Lawrence Tien Lin; He, Jian; Wang, Baohua; Ma, Yaping; Wong, King Young; Li, Quan; Xiao, Xudong; Chen, Tao

2014-01-01

Due to the two-dimensional confinement of electrons, single- and few-layer MoSe2 nanostructures exhibit unusual optical and electrical properties and have found wide applications in catalytic hydrogen evolution reaction, field effect transistor, electrochemical intercalation, and so on. Here we present a new application in dye-sensitized solar cell as catalyst for the reduction of I3− to I− at the counter electrode. The few-layer MoSe2 is fabricated by surface selenization of Mo-coated soda-lime glass. Our results show that the few-layer MoSe2 displays high catalytic efficiency for the regeneration of I− species, which in turn yields a photovoltaic energy conversion efficiency of 9.00%, while the identical photoanode coupling with “champion” electrode based on Pt nanoparticles on FTO glass generates efficiency only 8.68%. Thus, a Pt- and FTO-free counter electrode outperforming the best conventional combination is obtained. In this electrode, Mo film is found to significantly decrease the sheet resistance of the counter electrode, contributing to the excellent device performance. Since all of the elements in the electrode are of high abundance ratios, this type of electrode is promising for the fabrication of large area devices at low materials cost. PMID:24525919

Selenium stable isotope ratios in California agricultural drainage water management systems

USGS Publications Warehouse

Herbel, M.J.; Johnson, T.M.; Tanji, K.K.; Gao, S.; Bullen, T.D.

2002-01-01

Selenium stable isotope ratios are known to shift in predictable ways during various microbial, chemical, and biological processes, and can be used to better understand Se cycling in contaminated environments. In this study we used Se stable isotopes to discern the mechanisms controlling the transformation of oxidized, aqueous forms of Se to reduced, insoluble forms in sediments of Se-affected environments. We measured 80Se/76Se in surface waters, shallow ground waters, evaporites, digested plants and sediments, and sequential extracts from several sites where agricultural drainage water is processed in the San Joaquin Valley of California. Selenium isotope analyses of samples obtained from the Tulare Lake Drainage District flow-through wetland reveal small isotopic contrasts (mean difference 0.7%o) between surface water and reduced Se species in the underlying sediments. Selenium in aquatic macrophytes was very similar isotopically to the NaOH and Na2SO3 sediment extracts designed to recover soluble organic Se and Se(O), respectively. For the integrated on-farm drainage management sites, evaporite salts were slightly (approximately 0.6%o) enriched in the heavier isotope relative to the inferred parent waters, whereas surface soils were slightly (approximately 1.4%o) depleted. Bacterial or chemical reduction of Se(VI) or Se(IV) may be occurring at these sites, but the small isotopic contrasts suggest that other, less isotopically fractionating mechanisms are responsible for accumulation of reduced forms in the sediments. These findings provide evidence that Se assimilation by plants and algae followed by deposition and mineralization is the dominant transformation pathway responsible for accumulation of reduced forms of Se in the wetland sediments.

Comparison of carrier multiplication yields in PbS and PbSe nanocrystals: the role of competing energy-loss processes.

PubMed

Stewart, John T; Padilha, Lazaro A; Qazilbash, M Mumtaz; Pietryga, Jeffrey M; Midgett, Aaron G; Luther, Joseph M; Beard, Matthew C; Nozik, Arthur J; Klimov, Victor I

2012-02-08

Infrared band gap semiconductor nanocrystals are promising materials for exploring generation III photovoltaic concepts that rely on carrier multiplication or multiple exciton generation, the process in which a single high-energy photon generates more than one electron-hole pair. In this work, we present measurements of carrier multiplication yields and biexciton lifetimes for a large selection of PbS nanocrystals and compare these results to the well-studied PbSe nanocrystals. The similar bulk properties of PbS and PbSe make this an important comparison for discerning the pertinent properties that determine efficient carrier multiplication. We observe that PbS and PbSe have very similar biexciton lifetimes as a function of confinement energy. Together with the similar bulk properties, this suggests that the rates of multiexciton generation, which is the inverse of Auger recombination, are also similar. The carrier multiplication yields in PbS nanocrystals, however, are strikingly lower than those observed for PbSe nanocrystals. We suggest that this implies the rate of competing processes, such as phonon emission, is higher in PbS nanocrystals than in PbSe nanocrystals. Indeed, our estimations for phonon emission mediated by the polar Fröhlich-type interaction indicate that the corresponding energy-loss rate is approximately twice as large in PbS than in PbSe. © 2011 American Chemical Society

Optical Characterization of Bulk ZnSeTe Solid Solutions

NASA Technical Reports Server (NTRS)

Su, Ching-Hua; Feth, S.; Zhu, Shen; Lehoczky, S. L.; Wang, Ling Jun

2000-01-01

Optical characterization was performed on wafers sliced from crystals of ZnSe, ZnTe, and ZnSe(1-x)Te(x)(0 less than x less than 0.4) grown by physical vapor transport. Energy band gaps at room temperature were determined from optical transmission measurements on 11 wafers. A best fit curve to the band gap versus composition x data gives a bowing parameter of 1.45. This number lies between the value of 1.23 determined previously on ZnSeTe bulk crystals and the value of 1.621 reported on ZnSeTe epilayers. Low-temperature photoluminescence (PL) spectra were measured on six samples. The spectra of ZnSe and ZnTe were dominated by near band edge emissions and no deep donor-acceptor pairs were observed. The PL spectrum exhibited a broad emission for each of the ZnSe(1-x)Te(x) samples, 0.09 less than x less than 0.39. For x=0.09, this emission energy is about 0.2 eV lower than the band gap energy measured at low temperature. As x increases the energy discrepancy gradually decreases and reduces to almost zero at x=0.4. The single broad PL emission spectra and the spectra measured as a function of temperature were interpreted as being associated with the exciton bound to Te clusters because of the high Te content in these samples.

Shallow to deep transformation of Se donors in GaSb under hydrostatic pressure

DOE Office of Scientific and Technical Information (OSTI.GOV)

Navarro-Contreras, H.; de Anda-Salazar, F.; Olvera-Hernandez, J.

1999-03-01

We have observed that highly doped GaSb:Se, which is opaque to far IR radiation, becomes transparent at hydrostatic pressures above 9.8{plus_minus}2&hthinsp;kbar. We discuss how this behavior may be explained by the transformation of Se shallow donors into Se-DX (where DX is the unknown donor or X donor) centers in GaSb. Under this assumption the position of the Se-DX energy level at zero pressure is calculated to lie 80{plus_minus}30 meV above the conduction band at atmospheric pressure. The onset of transparency allowed us to observe several multiphonon absorbance features. We assign six of them to two-phonon absorptions. From the measured pressuremore » dependence of the TO phonon, the Gr{umlt u}neisen parameter for this compound is calculated to be {gamma}{sub TO}=1.23{plus_minus}0.18. No persistent photoconductivity is observed for these Se-DX centers, a fact that may be explained by the expectation that the optical energy necessary to transform them back into the shallow form is larger than the band-gap energy of GaSb at all pressures examined, although it may be also an indication that the Se shallow donors change to deep donors associated with the L{sub 1} minima of ionization energy larger than 90 meV. {copyright} {ital 1999} {ital The American Physical Society}« less

Effects of magnetic dopants in (Li0.8M0.2OH )FeSe (M =Fe , Mn, Co): Density functional theory study using a band unfolding technique

NASA Astrophysics Data System (ADS)

Chen, M. X.; Chen, Wei; Zhang, Zhenyu; Weinert, M.

2017-12-01

The effects of Fe dopants on the electronic bands structure of (Li0.8Fe0.2OH )FeSe are investigated by a band unfolding (k -projection) technique and first-principles supercell calculations. Doping 20% Fe into the LiOH layers causes electron donation to the FeSe layers, significantly changing the profile of bands around the Fermi level. Because of the weak bonding between the LiOH and FeSe layers the magnetic configuration of the dopants has only minor effects on the band structure. The electronic bands for the surface FeSe layer of (Li0.8Fe0.2OH )FeSe show noticeable differences compared to those of the inner layers, both in the location of the Fermi level and in details of the bands near the high symmetry points, resulting from different effective doping levels and the broken symmetry at the surface. The band structure for the surface FeSe layer with checkerboard antiferromagnetic order is reasonably consistent with angle-resolved photoemission results. The 3 d transition metals Mn and Co have similar doping effects on the band structure of (LiOH)FeSe.

Nanostructured Mo-based electrode materials for electrochemical energy storage.

PubMed

Hu, Xianluo; Zhang, Wei; Liu, Xiaoxiao; Mei, Yueni; Huang, Yunhui

2015-04-21

The development of advanced energy storage devices is at the forefront of research geared towards a sustainable future. Nanostructured materials are advantageous in offering huge surface to volume ratios, favorable transport features, and attractive physicochemical properties. They have been extensively explored in various fields of energy storage and conversion. This review is focused largely on the recent progress in nanostructured Mo-based electrode materials including molybdenum oxides (MoO(x), 2 ≤ x ≤ 3), dichalconides (MoX2, X = S, Se), and oxysalts for rechargeable lithium/sodium-ion batteries, Mg batteries, and supercapacitors. Mo-based compounds including MoO2, MoO3, MoO(3-y) (0 < y < 1), MMo(x)O(y) (M = Fe, Co, Ni, Ca, Mn, Zn, Mg, or Cd; x = 1, y = 4; x = 3, y = 8), MoS2, MoSe2, (MoO2)2P2O7, LiMoO2, Li2MoO3, etc. possess multiple valence states and exhibit rich chemistry. They are very attractive candidates for efficient electrochemical energy storage systems because of their unique physicochemical properties, such as conductivity, mechanical and thermal stability, and cyclability. In this review, we aim to provide a systematic summary of the synthesis, modification, and electrochemical performance of nanostructured Mo-based compounds, as well as their energy storage applications in lithium/sodium-ion batteries, Mg batteries, and pseudocapacitors. The relationship between nanoarchitectures and electrochemical performances as well as the related charge-storage mechanism is discussed. Moreover, remarks on the challenges and perspectives of Mo-containing compounds for further development in electrochemical energy storage applications are proposed. This review sheds light on the sustainable development of advanced rechargeable batteries and supercapacitors with nanostructured Mo-based electrode materials.

Extracellular polymeric substances govern the surface charge of biogenic elemental selenium nanoparticles.

PubMed

Jain, Rohan; Jordan, Norbert; Weiss, Stephan; Foerstendorf, Harald; Heim, Karsten; Kacker, Rohit; Hübner, René; Kramer, Herman; van Hullebusch, Eric D; Farges, François; Lens, Piet N L

2015-02-03

The origin of the organic layer covering colloidal biogenic elemental selenium nanoparticles (BioSeNPs) is not known, particularly in the case when they are synthesized by complex microbial communities. This study investigated the presence of extracellular polymeric substances (EPS) on BioSeNPs. The role of EPS in capping the extracellularly available BioSeNPs was also examined. Fourier transform infrared (FT-IR) spectroscopy and colorimetric measurements confirmed the presence of functional groups characteristic of proteins and carbohydrates on the BioSeNPs, suggesting the presence of EPS. Chemical synthesis of elemental selenium nanoparticles in the presence of EPS, extracted from selenite fed anaerobic granular sludge, yielded stable colloidal spherical selenium nanoparticles. Furthermore, extracted EPS, BioSeNPs, and chemically synthesized EPS-capped selenium nanoparticles had similar surface properties, as shown by ζ-potential versus pH profiles and isoelectric point measurements. This study shows that the EPS of anaerobic granular sludge form the organic layer present on the BioSeNPs synthesized by these granules. The EPS also govern the surface charge of these BioSeNPs, thereby contributing to their colloidal properties, hence affecting their fate in the environment and the efficiency of bioremediation technologies.

Surface decoration by Spirulina polysaccharide enhances the cellular uptake and anticancer efficacy of selenium nanoparticles.

PubMed

Yang, Fang; Tang, Quanming; Zhong, Xueyun; Bai, Yan; Chen, Tianfeng; Zhang, Yibo; Li, Yinghua; Zheng, Wenjie

2012-01-01

A simple and solution-phase method for functionalization of selenium nanoparticles (SeNPs) with Spirulina polysaccharides (SPS) has been developed in the present study. The cellular uptake and anticancer activity of SPS-SeNPs were also evaluated. Monodisperse and homogeneous spherical SPS-SeNPs with diameters ranging from 20 nm to 50 nm were achieved under optimized conditions, which were stable in the solution phase for at least 3 months. SPS surface decoration significantly enhanced the cellular uptake and cytotoxicity of SeNPs toward several human cancer cell lines. A375 human melanoma cells were found extremely susceptible to SPS-SeNPs with half maximal (50%) inhibitory concentration value of 7.94 μM. Investigation of the underlying mechanisms revealed that SPS-SeNPs inhibited cancer cell growth through induction of apoptosis, as evidenced by an increase in sub-G(1) cell population, deoxyribonucleic acid fragmentation, chromatin condensation, and phosphatidylserine translocation. Results suggest that the strategy to use SPS as a surface decorator could be an effective way to enhance the cellular uptake and anticancer efficacy of nanomaterials. SPS-SeNPs may be a potential candidate for further evaluation as a chemopreventive and chemotherapeutic agent against human cancers.

Temperature induced CuInSe2 nanocrystal formation in the Cu2Se-In3Se2 multilayer thin films

NASA Astrophysics Data System (ADS)

Mohan, A.; Rajesh, S.

2017-04-01

The paper deals with the impact of annealing on Cu2Se-In3Se2 multilayer structure and discusses the quantum confinements. Thermal evaporation technique was used to prepare multilayer films over the glass substrates. The films were annealed at different temperatures (150 °C-350 °C) under vacuum atmosphere. The XRD pattern reveals that the films exhibit (112) peaks with CuInSe2 Chalcopyrite structure and upon annealing crystallinity improved. The grain size comes around 13-19 nm. The optical band gap value was found to be 2.21 to 2.09 eV and band gap splitting was observed for higher annealing temperatures. The increase in the band gap is related to quantum confinement effect. SEM image shows nano crystals spread over the entire surface for higher annealing temperatures. Optical absorption and PL spectra shows the blue shift during annealing. The HR-TEM shows the particle size in the nano range and which confirms the CuInSe2 nanocrystal formation. AFM image shows the rough surface with homogenous grains for the as deposited films and smooth surface for annealed films.

Surface decoration by Spirulina polysaccharide enhances the cellular uptake and anticancer efficacy of selenium nanoparticles

PubMed Central

Yang, Fang; Tang, Quanming; Zhong, Xueyun; Bai, Yan; Chen, Tianfeng; Zhang, Yibo; Li, Yinghua; Zheng, Wenjie

2012-01-01

A simple and solution-phase method for functionalization of selenium nanoparticles (SeNPs) with Spirulina polysaccharides (SPS) has been developed in the present study. The cellular uptake and anticancer activity of SPS-SeNPs were also evaluated. Monodisperse and homogeneous spherical SPS-SeNPs with diameters ranging from 20 nm to 50 nm were achieved under optimized conditions, which were stable in the solution phase for at least 3 months. SPS surface decoration significantly enhanced the cellular uptake and cytotoxicity of SeNPs toward several human cancer cell lines. A375 human melanoma cells were found extremely susceptible to SPS-SeNPs with half maximal (50%) inhibitory concentration value of 7.94 μM. Investigation of the underlying mechanisms revealed that SPS-SeNPs inhibited cancer cell growth through induction of apoptosis, as evidenced by an increase in sub-G1 cell population, deoxyribonucleic acid fragmentation, chromatin condensation, and phosphatidylserine translocation. Results suggest that the strategy to use SPS as a surface decorator could be an effective way to enhance the cellular uptake and anticancer efficacy of nanomaterials. SPS-SeNPs may be a potential candidate for further evaluation as a chemopreventive and chemotherapeutic agent against human cancers. PMID:22359460

Indium selenide monolayer: strain-enhanced optoelectronic response and dielectric environment-tunable 2D exciton features

NASA Astrophysics Data System (ADS)

Ben Amara, Imen; Hichri, Aida; Jaziri, Sihem

2017-12-01

Electronic and optical performances of the β-InSe monolayer (ML) are considerably boosted by tuning the corresponding band energies through lattice in-plane compressive strain engineering. First principles calculations show an indirect-direct gap transition with a large bandgap size. The crossover is due to different responses of the near-gap state energies with respect to strain. This is explained by the variation of In-Se bond length, the bond nature of near-band-edge electronic orbital and of the momentum angular contribution versus in-plane compressive strain. The effective masses of charge carriers are also found to be highly modulated and significantly light at the indirect-direct-gap transition. The tuned optical response of the resulting direct-gap ML β-InSe is evaluated versus applied energy to infer the allowed optical transitions, dielectric constants, semiconductor-metal behavior and refractive index. The environmental dielectric engineering of exciton behavior of the resulting direct-gap ML β-InSe is handled within the effective mass Wannier-Mott model and is expected to be important. Our results highlight the increase of binding energy and red-shifted exciton energy with decreasing screening substrates, resulting in a stable exciton at room temperature. The intensity and energy of the ground-state exciton emission are expected to be strongly influenced under substrate screening effect. According to our findings, the direct-gap ML β-InSe assures tremendous 2D optoelectronic and nanoelectronic merits that could overcome several limitations of unstrained ML β-InSe.

A layered Dirac system candidate: Fermi surface and anomalous Berry phase in ZrSiSe

NASA Astrophysics Data System (ADS)

Chiu, Yu-Che; Chen, Kuan-Wen; Graf, David; Zhou, Qiong; Martin, Thomas J.; Chan, Julia Y.; Johannes, Michelle; Baumbach, Ryan E.; Balicas, Luis

ZrSiSe was recently claimed to correspond to a novel type of nodal Dirac system. We synthesized single crystals through a combination of solid state reaction and chemical vapor transport. The as-grown single crystals display residual resistivities on the order of 100 nOhmcm at 2K yielding a resistivity ratio surpassing 200. Magnetoresistance (MR) measurements reveal a non-saturating increase in the resistivity by a factor of 500000% under fields up to 35 Tesla. De Haas van Alphen measurements under high magneticfields reveal a Fermi surface that is more complex than previously reported, although its geometry generally agrees with band structure calculations that indicate Dirac-like dispersion in the bulk around the Fermi energy. The charge carrier effective masses extracted from Lifshitz-Kosevich (LK) fits to the amplitude of quantum oscillations were found to range between 0.08me to 0.5me where me is the free electron mass. Fittings of the oscillatory signal to the LK formalism further reveal the existence of cyclotron orbits displaying non-trivial Berry phases approaching pi, which is consistent with the expectations from band structure calculations. funded by DOE, NSF, NHMFL.

Two-step growth of two-dimensional WSe 2/MoSe 2 heterostructures

DOE PAGES

Gong, Yongji; Lei, Sidong; Lou, Jun; ...

2015-08-03

Two dimensional (2D) materials have attracted great attention due to their unique properties and atomic thickness. Although various 2D materials have been successfully synthesized with different optical and electrical properties, a strategy for fabricating 2D heterostructures must be developed in order to construct more complicated devices for practical applications. Here we demonstrate for the first time a two-step chemical vapor deposition (CVD) method for growing transition-metal dichalcogenide (TMD) heterostructures, where MoSe 2 was synthesized first and followed by an epitaxial growth of WSe 2 on the edge and on the top surface of MoSe 2. Compared to previously reported one-stepmore » growth methods, this two-step growth has the capability of spatial and size control of each 2D component, leading to much larger (up to 169 μm) heterostructure size, and cross-contamination can be effectively minimized. Furthermore, this two-step growth produces well-defined 2H and 3R stacking in the WSe 2/MoSe 2 bilayer regions and much sharper in-plane interfaces than the previously reported MoSe 2/WSe 2 heterojunctions obtained from one-step growth methods. The resultant heterostructures with WSe 2/MoSe 2 bilayer and the exposed MoSe 2 monolayer display rectification characteristics of a p-n junction, as revealed by optoelectronic tests, and an internal quantum efficiency of 91% when functioning as a photodetector. As a result, a photovoltaic effect without any external gates was observed, showing incident photon to converted electron (IPCE) efficiencies of approximately 0.12%, providing application potential in electronics and energy harvesting.« less

Antibacterial effect of the laser-generated Se nanocoatings on Staphylococcus aureus and Pseudomonas aeruginosa biofilms

NASA Astrophysics Data System (ADS)

Ionin, A. A.; Ivanova, A. K.; Khmel'nitskii, R. A.; Klevkov, Yu V.; Kudryashov, S. I.; Levchenko, A. O.; Nastulyavichus, A. A.; Rudenko, A. A.; Saraeva, I. N.; Smirnov, N. A.; Zayarny, D. A.; Gonchukov, S. A.; Tolordava, E. R.

2018-01-01

The antibacterial properties of selenium nanoparticles (Se NPs) were successfully demonstrated in vitro for Staphylococcus aureus and Pseudomonas aeruginosa biofilms. The possible mechanisms of antibacterial impact included the emergence of reactive oxygen species, induced by free radicals on the NP surface and accompanied by subsequent oxidative stress, as well as mechanical decomposition of the mitochondrial membrane. Se nanocoatings were deposited on bare and silver-coated silica glass substrates via inkjet printing with concentrated nanoinks, prepared by infrared laser-ablative processing of a solid Se target in a 50%-isopropyl solution. The resulted porous nanofilms with high-percentage surface coverage, consisting of spherical Se NPs and Se nanorods, were characterized by means of standard microscopy techniques (optical, scanning electron, transmission), UV-vis-IR and EDX spectroscopy.

Low kV versus dual-energy virtual monoenergetic CT imaging for proven liver lesions: what are the advantages and trade-offs in conspicuity and image quality? A pilot study.

PubMed

Hanson, G Jay; Michalak, Gregory J; Childs, Robert; McCollough, Brian; Kurup, Anil N; Hough, David M; Frye, Judson M; Fidler, Jeff L; Venkatesh, Sudhakar K; Leng, Shuai; Yu, Lifeng; Halaweish, Ahmed F; Harmsen, W Scott; McCollough, Cynthia H; Fletcher, J G

2018-06-01

Single-energy low tube potential (SE-LTP) and dual-energy virtual monoenergetic (DE-VM) CT images both increase the conspicuity of hepatic lesions by increasing iodine signal. Our purpose was to compare the conspicuity of proven liver lesions, artifacts, and radiologist preferences in dose-matched SE-LTP and DE-VM images. Thirty-one patients with 72 proven liver lesions (21 benign, 51 malignant) underwent full-dose contrast-enhanced dual-energy CT (DECT). Half-dose images were obtained using single tube reconstruction of the dual-source SE-LTP projection data (80 or 100 kV), and by inserting noise into dual-energy projection data, with DE-VM images reconstructed from 40 to 70 keV. Three blinded gastrointestinal radiologists evaluated half-dose SE-LTP and DE-VM images, ranking and grading liver lesion conspicuity and diagnostic confidence (4-point scale) on a per-lesion basis. Image quality (noise, artifacts, sharpness) was evaluated, and overall image preference was ranked on per-patient basis. Lesion-to-liver contrast-to-noise ratio (CNR) was compared between techniques. Mean lesion size was 1.5 ± 1.2 cm. Across the readers, the mean conspicuity ratings for 40, 45, and 50 keV half-dose DE-VM images were superior compared to other half-dose image sets (p < 0.0001). Per-lesion diagnostic confidence was similar between half-dose SE-LTP compared to half-dose DE-VM images (p ≥ 0.05; 1.19 vs. 1.24-1.32). However, SE-LTP images had less noise and artifacts and were sharper compared to DE-VM images less than 70 keV (p < 0.05). On a per-patient basis, radiologists preferred SE-LTP images the most and preferred 40-50 keV the least (p < 0.0001). Lesion CNR was also higher in SE-LTP images than DE-VM images (p < 0.01). For the same applied dose level, liver lesions were more conspicuous using DE-VM compared to SE-LTP; however, SE-LTP images were preferred more than any single DE-VM energy level, likely due to lower noise and artifacts.

Thiolated graphene - a new platform for anchoring CdSe quantum dots for hybrid heterostructures

NASA Astrophysics Data System (ADS)

Debgupta, Joyashish; Pillai, Vijayamohanan K.

2013-04-01

Effective organization of small CdSe quantum dots on graphene sheets has been achieved by a simple solution exchange with thiol terminated graphene prepared by diazonium salt chemistry. This generic methodology of CdSe QD attachment to any graphene surface has remarkable implications in designing hybrid heterostructures.Effective organization of small CdSe quantum dots on graphene sheets has been achieved by a simple solution exchange with thiol terminated graphene prepared by diazonium salt chemistry. This generic methodology of CdSe QD attachment to any graphene surface has remarkable implications in designing hybrid heterostructures. Electronic supplementary information (ESI) available. See DOI: 10.1039/c3nr00363a

Combining ligand-induced quantum-confined stark effect with type II heterojunction bilayer structure in CdTe and CdSe nanocrystal-based solar cells.

PubMed

Yaacobi-Gross, Nir; Garphunkin, Natalia; Solomeshch, Olga; Vaneski, Aleksandar; Susha, Andrei S; Rogach, Andrey L; Tessler, Nir

2012-04-24

We show that it is possible to combine several charge generation strategies in a single device structure, the performance of which benefits from all methods used. Exploiting the inherent type II heterojunction between layered structures of CdSe and CdTe colloidal quantum dots, we systematically study different ways of combining such nanocrystals of different size and surface chemistry and with different linking agents in a bilayer solar cell configuration. We demonstrate the beneficial use of two distinctly different sizes of NCs not only to improve the solar spectrum matching but also to reduce exciton binding energy, allowing their efficient dissociation at the interface. We further make use of the ligand-induced quantum-confined Stark effect in order to enhance charge generation and, hence, overall efficiency of nanocrystal-based solar cells.

Micro/nano hierarchical structured titanium treated by NH4OH/H2O2 for enhancing cell response

PubMed Central

Yuan, Xin; Kang, Yi; Zuo, Jun; Xie, Youneng; Ma, Li; Ren, Xuelei; Bian, Zeyu; Zhou, Kechao; Wang, Xiyang; Yu, Zhiming

2018-01-01

In this paper, two kinds of titanium surfaces with novel micro/nano hierarchical structures, namely Etched (E) surface and Sandblast and etched (SE) surface, were successfully fabricated by NH4OH and H2O2 mixture. And their cellular responses of MG63 were investigated compared with Sandblast and acid-etching (SLA) surface. Scanning electron microscope (SEM), Surface profiler, X-ray photoelectron spectroscopy (XPS), and Contact angle instrument were employed to assess the surface morphologies, roughness, chemistry and wettability respectively. Hierarchical structures with micro holes of 10–30 μm in diameter and nano pits of tens of nanometers in diameter formed on both E and SE surfaces. The size of micro holes is very close to osteoblast cell, which makes them wonderful beds for osteoblast. Moreover, these two kinds of surfaces possess similar roughness and superior hydrophilicity to SLA. Reactive oxygen species were detected on E and SE surface, and thus considerable antimicrobial performance and well fixation can be speculated on them. The cell experiments also demonstrated a boost in cell attachment, and that proliferation and osteogenic differentiation were achieved on them, especially on SE surface. The results indicate that the treatment of pure titanium with H2O2/NH4OH is an effective technique to improve the initial stability of implants and enhance the osseointegration, which may be a promising surface treatment to titanium implant. PMID:29723214

Frequency power analyses of seismic sources on firn

NASA Astrophysics Data System (ADS)

Sanz, Christopher; Diez, Anja; Coen, Hofstede; Kristoffersen, Yngve; Mayer, Christoph; Lambrecht, Astrid; Miller, Heinz; Eisen, Olaf

2013-04-01

A great obstacle for seismic surveys on firn-covered ice masses is the ability of firn to strongly attenuate seismic energy and divert downward ray paths away from the vertical because of the velocity gradient. The standard way to overcome these limitations is the drilling of shotholes about 10-30 m deep. However, drilling of shotholes is a time and energy consuming task. Another possibility is to use vibroseismic sources at the surface and increase the signal-to-noise ratio by repeated stacking. However, compared to explosive charges, vibroseismic signals are bandlimited per se. As a third variant, we investigate the usage of ordered patterns of surface charges consisting of detonation cord. Previous applications of detonation cord only explored their general comparison to bulk explosives when deployed in a linear fashion, i.e. a single line. Our approach extends these results to other geometries, like fan- or comb-shaped patterns. These have two advantages: first, over the pattern area a locally plane wave is generated, limiting the spherical and velocity-gradient induced spreading of energy during propagation; second, the ratio between seismic wave speed of the firn and the detonation cord of typically about 1:5 causes the wave to propagate in an angle downward. When using large offsets like a snow streamer, it is possible to direct the refected energy towards the streamer, depending on offset range and reflector depth. We compare the different source types for several surveys conducted in Antarctica in terms of frequency spectra. Our results show that ordered patterns of detonation cord serve as suitable seismic surface charges, avoiding the need to drill shotholes. Moreover, an example of a short profile with patterned surface charges is presented. The technique can be of advantage for surveys in remote areas, which can only be accessed by aircrafts.

Enhanced conversion efficiency in Si solar cells employing photoluminescent down-shifting CdSe/CdS core/shell quantum dots.

PubMed

Lopez-Delgado, R; Zhou, Y; Zazueta-Raynaud, A; Zhao, H; Pelayo, J E; Vomiero, A; Álvarez-Ramos, M E; Rosei, F; Ayon, A

2017-10-26

Silicon solar cells have captured a large portion of the total market of photovoltaic devices mostly due to their relatively high efficiency. However, Silicon exhibits limitations in ultraviolet absorption because high-energy photons are absorbed at the surface of the solar cell, in the heavily doped region, and the photo-generated electron-hole pairs need to diffuse into the junction region, resulting in significant carrier recombination. One of the alternatives to improve the absorption range involves the use of down-shifting nano-structures able to interact with the aforementioned high energy photons. Here, as a proof of concept, we use downshifting CdSe/CdS quantum dots to improve the performance of a silicon solar cell. The incorporation of these nanostructures triggered improvements in the short circuit current density (J sc , from 32.5 to 37.0 mA/cm 2 ). This improvement led to a ∼13% increase in the power conversion efficiency (PCE), from 12.0 to 13.5%. Our results demonstrate that the application of down-shifting materials is a viable strategy to improve the efficiency of Silicon solar cells with mass-compatible techniques that could serve to promote their widespread utilization.

Laser microprocessing technologies for automotive, flexible electronics, and solar energy sectors

NASA Astrophysics Data System (ADS)

Nikumb, Suwas; Bathe, Ravi; Knopf, George K.

2014-10-01

Laser microprocessing technologies offer an important tool to fulfill the needs of many industrial sectors. In particular, there is growing interest in applications of these processes in the manufacturing areas such as automotive parts fabrication, printable electronics and solar energy panels. The technology is primarily driven by our understanding of the fundamental laser-material interaction, process control strategies and the advancement of significant fabrication experience over the past few years. The wide-ranging operating parameters available with respect to power, pulse width variation, beam quality, higher repetition rates as well as precise control of the energy deposition through programmable pulse shaping technologies, enables pre-defined material removal, selective scribing of individual layer within a stacked multi-layer thin film structure, texturing of material surfaces as well as precise introduction of heat into the material to monitor its characteristic properties are a few examples. In this research, results in the area of laser surface texturing of metals for added hydrodynamic lubricity to reduce friction, processing of ink-jet printed graphene oxide for flexible printed electronic circuit fabrication and scribing of multi-layer thin films for the development of photovoltaic CuInGaSe2 (CIGS) interconnects for solar panel devices will be discussed.

Industrial perspectives on earth abundant, multinary thin film photovoltaics

NASA Astrophysics Data System (ADS)

Haight, Richard; Gershon, Talia; Gunawan, Oki; Antunez, Priscilla; Bishop, Douglas; Seog Lee, Yun; Gokmen, Tayfun; Sardashti, Kasra; Chagarov, Evgueni; Kummel, Andrew

2017-03-01

The most efficient earth abundant, non-toxic thin film multelemental PV devices are fabricated from Cu, Zn, Sn, S and Se, with the chemical formula of Cu2ZnSn(S x Se1-x )4 (CZTS,Se). This material has enjoyed relatively rapid increases in efficiency from its inception to its present-day power conversion efficiency of 12.6%. But further increases in efficiency have been hampered by the inability to substantially increase Voc, the open circuit voltage. In this review article we will discuss the fundamentals of this important kesterite material including methods of film growth, post growth processing and device fabrication. Detailed studies of the properties of CZTS,Se including chemical, structural and electronic as well as full device electrical characterization have been performed in an effort to coax out the critical issues that limit performance. These experimental studies, enhanced by density functional theory calculations have pointed to fundamental bulk point defects, such as Cu-Zn antisites, and clusters of defects, as the primary culprits in limiting Voc increases. Improvements in device performance through grain boundary passivation and interface modifications are described. Exfoliation of functioning solar cells to expose the back surface along with engineering of new back contacts designed to impose electrostatic fields that drive electron-hole separation and increase Voc are discussed. A parallel route to increasing device performance by alloying Ag with CZTS,Se in order to inhibit Cu-Zn antisite defect formation has shown significant improvement in material properties. Finally, applications of high S (and hence higher Voc) CZTS,Se based devices to energy harvesting for ‘Internet-of-Things’ devices is discussed.

BariumCopperChFluorine (Ch = Sulfur, Selenium, Tellurium) p-type transparent conductors

NASA Astrophysics Data System (ADS)

Zakutayev, Andriy

BaCuChF (Ch = S, Se, Te) materials are chalcogen-based transparent conductors with wide optical band gaps (2.9 -- 3.5 eV) and a high concentration of free holes (1018 -- 1020 cm-3 ) caused by the presence of copper vacancies. Chalcogen vacancies compensate copper vacancies in these materials, setting the Fermi level close to the valence band maximum. BaCuChF thin film solid solutions prepared by pulsed laser deposition (PLD) have tunable properties, such as lattice constants, conductivity and optical band gaps. BaCuSF and BaCuSeF materials also feature room-temperature stable 3D excitons with spin-orbit-split levels. BaCuTeF has forbidden lowest-energy optical transitions which extends its transparency range. BaCuChF surfaces oxidize when exposed to air, but can be protected using Ch capping layers. Polycrystalline BaCuSeF thin films have a 4.85 eV work function, a 0.11 eV hole injection barrier into ZnPc, and 0.00 eV valence band offset with ZnTe. BaCuSeF should have s similar band offset and similar interfacial properties with CdTe and Cu(InGa)Se2, and BaCuSF should have no valence band offset with Cu2ZnSnS4, according to the transitivity rule. Therefore, BaCuSeF is suitable for applications as a p-layer in organic light-emitting diodes, p-i-n double-heterojunction and tandem chalcogenide solar cells.

Bulk Fermi surface and electronic properties of Cu0.07Bi2Se3

NASA Astrophysics Data System (ADS)

Martin, C.; Craciun, V.; Miller, K. H.; Uzakbaiuly, B.; Buvaev, S.; Berger, H.; Hebard, A. F.; Tanner, D. B.

2013-05-01

The electronic properties of Cu0.07Bi2Se3 have been investigated using Shubnikov-de Haas and optical reflectance measurements. Quantum oscillations reveal a bulk, three-dimensional Fermi surface with anisotropy kFc/kFab≈ 2 and a modest increase in free-carrier concentration and in scattering rate with respect to the undoped Bi2Se3, also confirmed by reflectivity data. The effective mass is almost identical to that of Bi2Se3. Optical conductivity reveals a strong enhancement of the bound impurity bands with Cu addition, suggesting that a significant number of Cu atoms enter the interstitial sites between Bi and Se layers or may even substitute for Bi. This conclusion is also supported by x-ray diffraction measurements, where a significant increase of microstrain was found in Cu0.07Bi2Se3, compared to Bi2Se3.

Energy band-gap calculations of short-period (ZnTe)m(ZnSe)n and (ZnS)m(ZnSe)n strained-layer superlattices

NASA Astrophysics Data System (ADS)

Wu, Yi-hong; Fujita, Shizuo; Fujita, Shigeo

1990-01-01

We report on the calculations of energy band gaps based on the semiempirical tight-binding model for short-period (ZnTe)m(ZnSe)n and (ZnS)m(ZnSe)n strained-layer superlattices (SLSs). During the calculation, much attention has been paid to the modeling of strain effect. It is found that (ZnTe)m(ZnSe)n superlattices grown on InAs, InP, and GaAs substrates show very different electronic properties from each other, which is consistent with experimental results now available. Assuming that the emission observed for (ZnTe)m(ZnSe)n SLS originates from intrinsic luminescence, we obtain an unstrained valence-band offset of 1.136±0.1 eV for this superlattice. On the other hand, the band gap of (ZnS)m(ZnSe)n superlattice grown coherently on GaP is found to exhibit a much stronger structure dependence than that grown coherently on GaAs. The difference of energy gap between superlattice with equal monolayers (m=n) and the corresponding alloy with equal chalcogenide composition is also discussed.

A stable lithiated silicon–chalcogen battery via synergetic chemical coupling between silicon and selenium

PubMed Central

Eom, KwangSup; Lee, Jung Tae; Oschatz, Martin; Wu, Feixiang; Kaskel, Stefan; Yushin, Gleb; Fuller, Thomas F.

2017-01-01

Li-ion batteries dominate portable energy storage due to their exceptional power and energy characteristics. Yet, various consumer devices and electric vehicles demand higher specific energy and power with longer cycle life. Here we report a full-cell battery that contains a lithiated Si/graphene anode paired with a selenium disulfide (SeS2) cathode with high capacity and long-term stability. Selenium, which dissolves from the SeS2 cathode, was found to become a component of the anode solid electrolyte interphase (SEI), leading to a significant increase of the SEI conductivity and stability. Moreover, the replacement of lithium metal anode impedes unwanted side reactions between the dissolved intermediate products from the SeS2 cathode and lithium metal and eliminates lithium dendrite formation. As a result, the capacity retention of the lithiated silicon/graphene—SeS2 full cell is 81% after 1,500 cycles at 268 mA gSeS2−1. The achieved cathode capacity is 403 mAh gSeS2−1 (1,209 mAh cmSeS2−3). PMID:28054543

Density-functional theory computer simulations of CZTS0.25Se0.75 alloy phase diagrams

NASA Astrophysics Data System (ADS)

Chagarov, E.; Sardashti, K.; Haight, R.; Mitzi, D. B.; Kummel, A. C.

2016-08-01

Density-functional theory simulations of CZTS, CZTSe, and CZTS0.25Se0.75 photovoltaic compounds have been performed to investigate the stability of the CZTS0.25Se0.75 alloy vs. decomposition into CZTS, CZTSe, and other secondary compounds. The Gibbs energy for vibrational contributions was estimated by calculating phonon spectra and thermodynamic properties at finite temperatures. It was demonstrated that the CZTS0.25Se0.75 alloy is stabilized not by enthalpy of formation but primarily by the mixing contributions to the Gibbs energy. The Gibbs energy gains/losses for several decomposition reactions were calculated as a function of temperature with/without intermixing and vibration contributions to the Gibbs energy. A set of phase diagrams was built in the multidimensional space of chemical potentials at 300 K and 900 K temperatures to demonstrate alloy stability and boundary compounds at various chemical conditions. It demonstrated for CZTS0.25Se0.75 that the chemical potentials for stability differ between typical processing temperature (˜900 K) and operating temperature (300 K). This implies that as cooling progresses, the flux/concentration of S should be increased in MBE growth to maintain the CZTS0.25Se0.75 in a thermodynamically stable state to minimize phase decomposition.

Confined lattice dynamics of single and quadruple SnSe bilayers in [(SnSe) 1.04 ] m [MoSe 2 ] n ferecrystals

DOE PAGES

Klobes, Benedikt; Hu, Michael Y.; Beekman, Matt; ...

2015-11-30

The Sn specific densities of phonon states in the SnSe subunits of [(SnSe) 1.04] m[MoSe 2] n ferecrystals with (m,n) = (1,1), (4,1) and in bulk SnSe were derived from nuclear inelastic scattering by the 119Sn M ssbauer resonance. When using different measurement configurations, phonons with polarization parallel and perpendicular to the ferecrystal plane were specifically probed. Vibrational properties and phonon spectral weight are found to strongly depend on the phonon polarization and layer count m. Moreover, a highly peculiar feature of these ferecrystal densities of phonon states is the emergence of rather sharp high energy vibrational modes polarized perpendicularmore » to the ferecrystal plane, which contrasts with usual findings in thin layered structures and nanostructured materials in general, and a depletion of modes with a gap appearing between acoustic and high energy modes. The spectral weight of these phonons depends on the overall SnSe content, m, but cannot be unambiguously attributed to SnSe MoSe 2 interfaces. Considering the low energy part of lattice dynamics, ferecrystals exhibit rather low average phonon group velocities as compared to the speed of sound in the long wavelength limit. For the (1,1) ferecrystal, this effect is most pronounced for vibrations polarized in the ferecrystal plane. Therefore, an experimental microscopic origin for the vibrational and bonding anisotropy in subunits of ferecrystals is provided.« less

Tuning the structural and electronic properties of heterogeneous chalcogenide nanostructures

NASA Astrophysics Data System (ADS)

Giberti, Federico; Voros, Marton; Galli, Giulia

Heterogeneous nanostructures, such as quantum dots (QDs) embedded in solid matrices, are promising platforms for solar energy conversion. Unfortunately, there is scarce information on the structure of the interface between the dots and their embedding matrix, thus hampering the design of functional materials with desired optoelectronic properties. Here, we developed a hierarchical computational strategy to obtain realistic models of semiconductor QDs embedded in matrices using enhanced sampling classical molecular dynamics simulations and predicted their electronic structure using first-principles electronic structure methods. We investigated PbSe/CdSe systems which are promising materials for solar cell applications and found a favorable quasi-type-II band alignments both for PbSe QDs in CdSe matrices and for CdSe embedded in PbSe. However, in the former case, we found the presence of detrimental intra-gap states, while in the latter no defect states are present. Hence we predict that embedding CdSe in PbSe leads to a more efficient platform for solar energy conversion. In addition, we showed that the structure of CdSe QD and in turn its band gap might be tuned by applying pressure to the PbSe matrix, providing a way to engineer the properties of new functional materials. Work by F. Giberti was supported by MICCoM funded by the U.S. Department of Energy (DOE), DOE/BES 5J-30161-0010A; work by M. Voros was supported by the U.S. DOE, under Award DE-AC02-06CH11357.

Growth and characterization of epitaxial silver indium diselenide

NASA Astrophysics Data System (ADS)

Pena Martin, Pamela

Photovoltaics (solar cells) are a key player in the renewable energy frontier, and will become increasingly important as their cost per watt continues to drop, especially if fossil fuel costs increase. One particularly promising photovoltaic technology is based on chalcopyrite-structure semiconductors. Within the chalcopyrite compounds the highest efficiency thin film solar cell absorber material to date is Cu(In,Ga)Se2 (CIGS). While current efficiency records are over 21% for single-junction cells, there is still room for improvement. Replacing some of the Cu with Ag has been shown to be beneficial in CIGS devices. However, the Ag- containing chalcopyrites are still relatively unknown in terms of their growth mechanism, energetics, and surface atomic and electronic properties. These are best inferred through study of epitaxial films, yet they have little mention in literature and have not been the subject of a detailed study. This work describes the growth of epitaxial AgInSe2 (AIS) on GaAs substrates, studying the morphology, structure, and surface properties to understand how growth takes place. It also seeks to experimentally determine the surface electronic and atomic structure at the atomic scale to gain insight into the part of the material that forms the heterojunction that collects photon energy in the device. Finally, this work seeks to compare and contrast these findings with what is known about CIGS to determine where similarities and, more importantly, the differences may lie. This study has found that single phase tetragonal AIS can be epitaxially grown on GaAs, as illustrated by x-ray diffraction (XRD), transmission electron microscope (TEM), and surface morphology data. Like CIGS, the close packed polar (112) planes have the lowest energy. The morphology points to a difference in step dynamics, leading to less faceted, straight edged island shapes compared to CIGS. Epitaxial temperature as a function of growth direction shows a different trend in AIS than in CIGS. Interdiffusion of the group III elements across the substrate interface was found to result in an epitaxial intermixed layer between the film and substrate in some cases, which may help mediate the lattice mismatch. At the atomic scale, scanning tunneling microscopy (STM) was used to observe details of the surface morphology, which indicated growth of the (112)A orientation of AIS by a screw dislocation mechanism (other surfaces were not examined by STM but are expected to show similar results). The surface atomic structure was directly imaged for the first time, revealing an arrangement similar to that expected from a bulk terminated surface. The electronic structure shows a gap in surface electronic states with a width comparable to bulk AIS, n-type conduction, and a tail of states near the valence band edge that decay well into the gap. The conduction and valence bands show fluctuations as a function of position on the surface, with greater magnitude in the valence band. The fluctuations in both bands are less than those observed on the surface of CIS by STM. It seems to indicate a reduction in band tails, both in magnitude and spacial extent, in AIS compared to CIS, likely tied to a reduction in point defect concentration at the surface.

Enhanced photoluminescence of corrugated Al2O3 film assisted by colloidal CdSe quantum dots.

PubMed

Bai, Zhongchen; Hao, Licai; Zhang, Zhengping; Huang, Zhaoling; Qin, Shuijie

2017-05-19

We present the enhanced photoluminescence (PL) of a corrugated Al 2 O 3 film enabled by colloidal CdSe quantum dots. The colloidal CdSe quantum dots are fabricated directly on a corrugated Al 2 O 3 substrate using an electrochemical deposition (ECD) method in a microfluidic system. The photoluminescence is excited by using a 150 nm diameter ultraviolet laser spot of a scanning near-field optical microscope. Owing to the electron transfer from the conduction band of the CdSe quantum dots to that of Al 2 O 3 , the enhanced photoluminescence effect is observed, which results from the increase in the recombination rate of electrons and holes on the Al 2 O 3 surface and the reduction in the fluorescence of the CdSe quantum dots. A periodically-fluctuating fluorescent spectrum was exhibited because of the periodical wire-like corrugated Al 2 O 3 surface serving as an optical grating. The spectral topographic map around the fluorescence peak from the Al 2 O 3 areas covered with CdSe quantum dots was unique and attributed to the uniform deposition of CdSe QDs on the corrugated Al 2 O 3 surface. We believe that the microfluidic ECD system and the surface enhanced fluorescence method described in this paper have potential applications in forming uniform optoelectronic films of colloidal quantum dots with controllable QD spacing and in boosting the fluorescent efficiency of weak PL devices.

The RiSE climbing robot: body and leg design

NASA Astrophysics Data System (ADS)

Saunders, A.; Goldman, D. I.; Full, R. J.; Buehler, M.

2006-05-01

The RiSE robot is a biologically inspired, six legged climbing robot, designed for general mobility in scansorial (vertical walls, horizontal ledges, ground level) environments. It exhibits ground reaction forces that are similar to animal climbers and does not rely on suction, magnets or other surface-dependent specializations to achieve adhesion and shear force. We describe RiSE's body and leg design as well as its electromechanical, communications and computational infrastructure. We review design iterations that enable RiSE to climb 90° carpeted, cork covered and (a growing range of) stucco surfaces in the quasi-static regime.

Regimes of association of arsenic and selenium during pulverized coal combustion

DOE Office of Scientific and Technical Information (OSTI.GOV)

Wayne S. Seames; Jost O.L. Wendt

2007-07-01

A suite of six coals, of widely differing As, Se, Ca, Fe, and sulfur contents, was burned under self-sustaining conditions in a 17 kW downflow laboratory combustor. Size segregated ash-laden aerosol samples were isokinetically withdrawn and collected on a Berner low pressure impactor. Correlations between trace element concentration (As or Se) and that of major elements (as functions of particle size) were then used to infer chemical associations between trace metals and Ca and/or Fe, and how these depended on sulfur. These baseline data led to formation of the following hypotheses, namely: (1) dominant As and Se partitioning mechanisms dependmore » on the availability of Ca and/or Fe active sites for surface reaction; (2) increasing combustion temperature increases the availability of active cation sites, and increases partitioning of As and Se to fly ash by surface reaction; (3) sulfur competes with these surface reactions, decreasing As and Se partitioning to fly ash surfaces. These hypotheses were tested by manipulating the As, Se, Ca, Fe, and S contents for various coals by doping. Temperature was adjusted in order to achieve comparisons of different coals and different coal constituents at similar thermal conditions, through O{sub 2} and CO{sub 2} addition, as required. These results confirmed the hypotheses above, and allowed an association regime map to be constructed. This map shows that both As and Se associate with Fe and Ca, provided active sites are available. Se reacts preferentially with Fe over Ca when both are available while As reactions with both Fe and Ca are comparable. Sulfur can prevent association of both As and Se, by preferentially reacting with active sites, especially those on Fe. When sufficient sites are not available, the release of vapor-phase As and Se species is promoted. 23 refs., 4 figs., 4 tabs.« less

ZnSe Window Layers for GaAs and GaInP2 Solar Cells

NASA Technical Reports Server (NTRS)

Olsen, Larry C.

1997-01-01

This report concerns studies of the use of n-type ZnSe as a window layer for n/p GaAs and GaInP2 solar cells. Emphasis was placed in this phase of the project on characterizing the interface between n-type ZnSe films grown on epi-GaAs films grown onto single crystal GaAs. Epi-GaAs and heteroepitaxial ZnSe films were grown by MOCVD with a Spire 50OXT Reactor. After growing epitaxial GaAs films on single crystal GaAs wafers, well-oriented crystalline ZnSe films were grown by MOCVD. ZnSe films were grown with substrate temperatures ranging from 250 C to 450 C. Photoluminescence studies carried out by researchers at NASA Lewis determined that the surface recombination velocity at a GaAs surface was significantly reduced after the deposition of a heteroepitaxial layer of ZnSe. The optimum temperature for ZnSe deposition appears to be on the order of 350 C.

Electron transport in Bi2Se3 ultra thin films

NASA Astrophysics Data System (ADS)

Bauer, Sebastian; Bernhart, Alexander M.; Bobisch, Christian A.

2018-02-01

We studied the electronic transport properties of a 4 QL thin Bi2Se3 film in the hybridized phase on Si(111) by scanning tunneling potentiometry. When a transverse voltage is applied, the film exhibits a homogeneous electric field on the nm scale. In addition, thermovoltage signals with lateral nm variations are found which result from sample heating by the transverse current. The thermovoltage signals are directly correlated to morphological structures on the surface, i.e. step edges, and indicate a lateral variation of the local density of states at the Bi2Se3 surface. No discernible voltage drops appear at the surface so that the whole film serves as a current carrying medium and scattering at surface defects is less important.

Study of Surface States at the Semiconductor/electrolyte Interface of Liquid-Junction Solar Cells.

NASA Astrophysics Data System (ADS)

Siripala, Withana P.

The existence of surface states at the semiconductor electrolyte interface of photoelectrochemical (PEC) cells plays a major role in determining the performance of the device in regard to the potential distribution and transport mechanisms of photogenerated carriers at the interface. We have investigated the n-TiO(,2)/electrolyte interface using three experimental techniques: relaxation spectrum analysis, photocurrent spectroscopy, and electrolyte electroreflectance (EER) spectroscopy. The effect of Fermi level pinning at the CdIn(,2)SE(,4)/aqueous-polysulfide interface was also studied using EER. Three distinct surface states were observed at the n-TiO(,2)/aqueous-electrolyte interface. The dominant state, which tails from the conduction band edge, is primarily responsible for the surface recombination of photocarriers at the interface. The second surface state, observed at 0.8 eV below the conduction band of TiO(,2), originates in the dark charge transfer intermediates (TiO(,2)-H). It is proposed that the sub-bandgap (SBG) photocurrent-potential behavior is a result of the mechanism of dynamic formation and annihilation of these surface states. The third surface state was at 1.3 eV below the conduction band of TiO(,2), and the SBG EER measurements show this state is "intrinsic" to the surface. These states were detected with SBG EER and impedance measurements in the presence of electrolytes that can adsorb on the surface of TiO(,2). Surface concentration of these states was evaluated with impedance measurements. EER measurements on a CdIn(,2)Se(,4)/polysulfide system have shown that the EER spectrum is sensitive to the surface preparation of the sample. The EER signal was quenched as the surface was driven to strong depletion, owing to Fermi level pinning at the interface in the presence of a high density of surface states. The full analysis of this effect enables us to measure the change in the flatband potential, as a function of the electrode potential, and also the energy distribution of these states.

Structural and electronic properties of CdSe/ZnS and ZnS/CdSe core/shell nanowires via first principles study

NASA Astrophysics Data System (ADS)

Rehman, Shafiq Ur; Li, H. M.; Ding, Z. J.

2018-05-01

First principles calculations have been performed to predict the structural stability and electronic structures of hydrogen passivated wurtzite CdSe/ZnS and ZnS/CdSe core/shell nanowires (CSNWs) in the [0001] direction. The calculated binding energy shows that ZnS/CdSe CSNWs are more stable than CdSe/ZnS CSNWs and the stability of ZnS/CdSe CSNWs increases with increasing the thickness of ZnS shell. The modulated electronic band gap demonstrates an increase when the size of both CSNWs is reduced, as a result of the quantum confinement effect. The core-to-shell chemical composition of atoms shows that a strong composition effect also exists in these CSNWs, which in turn affects their electronic properties. Our simulated results show that the photoemission spectra of the CSNWs can be significantly improved by tuning the energy gap of CSNWs.

Electronic structure of ruthenium-doped iron chalcogenides

NASA Astrophysics Data System (ADS)

Winiarski, M. J.; Samsel-Czekała, M.; Ciechan, A.

2014-12-01

The structural and electronic properties of hypothetical RuxFe1-xSe and RuxFe1-xTe systems have been investigated from first principles within the density functional theory (DFT). Reasonable values of lattice parameters and chalcogen atomic positions in the tetragonal unit cell of iron chalcogenides have been obtained with the use of norm-conserving pseudopotentials. The well known discrepancies between experimental data and DFT-calculated results for structural parameters of iron chalcogenides are related to the semicore atomic states which were frozen in the used here approach. Such an approach yields valid results of the electronic structures of the investigated compounds. The Ru-based chalcogenides exhibit the same topology of the Fermi surface (FS) as that of FeSe, differing only in subtle FS nesting features. Our calculations predict that the ground states of RuSe and RuTe are nonmagnetic, whereas those of the solid solutions RuxFe1-xSe and RuxFe1-xTe become the single- and double-stripe antiferromagnetic, respectively. However, the calculated stabilization energy values are comparable for each system. The phase transitions between these magnetic arrangements may be induced by slight changes of the chalcogen atom positions and the lattice parameters a in the unit cell of iron selenides and tellurides. Since the superconductivity in iron chalcogenides is believed to be mediated by the spin fluctuations in single-stripe magnetic phase, the RuxFe1-xSe and RuxFe1-xTe systems are good candidates for new superconducting iron-based materials.

Atomic and electronic structures of single-layer FeSe on SrTiO 3(001): The role of oxygen deficiency

DOE PAGES

Bang, Junhyeok; Li, Zhi; Sun, Y. Y.; ...

2013-06-06

Using first-principles calculation, we propose an interface structure for single triple-layer FeSe on the SrTiO 3(001) surface, a high-T c superconductor found recently. The key component of this structure is the oxygen deficiency on the top layer of the SrTiO 3 substrate, as a result of Se etching used in preparing the high-T c samples. The O vacancies strongly bind the FeSe triple layer to the substrate giving rise to a (2×1) reconstruction, as observed by scanning tunneling microscopy. The enhanced binding correlates to the significant increase of T c observed in experiment. The O vacancies also serve as themore » source of electron doping, which modifies the Fermi surface of the first FeSe layer by filling the hole pocket near the center of the surface Brillouin zone, as suggested from angle-resolved photoemission spectroscopy measurement.« less

Exciton Energy Transfer from Halide Terminated Nanocrystals to Graphene in Solar Photovoltaics

NASA Astrophysics Data System (ADS)

Ajayi, Obafunso; Abramson, Justin; Anderson, Nicholas; Owen, Jonathan; Zhao, Yue; Kim, Phillip; Gesuele, Felice; Wong, Chee Wei

2011-03-01

Graphene, a zero-gap semiconductor, has been identified as an ideal electrode for nanocrystal solar cell photovoltaic applications due to its high carrier mobility. Further advances in efficient current extraction are required towards this end. We investigate the resonant energy transfer dynamics between photoexcited nanocrystals and graphene, where the energy transfer rate is characterized by the fluorescent quenching of the quantum dots in the presence of graphene. Energy transfer has been shown to have a d -4 dependence on the nanocrystal distance from the graphene surface, with a correction due to blinking statistics. We investigate this relationship with single and few layer graphene. We study halide-terminated CdSe quantum dots; where the absence of the insulating outershell improves the electronic coupling of the donor-acceptor system leads to improved electron transfer. We observe quenching of the halide terminated nanocrystals on graphene, with the quenching factor ρ defined as IQ /IG (the relative intensities on quartz and graphene).

Coupled Effect of Ferrous Ion and Oxygen on the Electron Selectivity of Zerovalent Iron for Selenate Sequestration.

PubMed

Qin, Hejie; Li, Jinxiang; Yang, Hongyi; Pan, Bingcai; Zhang, Weiming; Guan, Xiaohong

2017-05-02

Although the electron selectivity (ES) of zerovalent iron (ZVI) for target contaminant and its utilization ratio (UR) decide the removal capacity of ZVI, little effort has been made to improve them. Taking selenate [Se(VI)] as a target contaminant, this study investigated the coupled influence of aeration gas and Fe(II) on the ES and UR of ZVI. Oxygen was necessary for effective removal of Se(VI) by ZVI without Fe(II) addition. Due to the application of 1.0 mM Fe(II), the ES of ZVI was increased from 3.2-3.6% to 6.2-6.8% and the UR of ZVI was improved by 5.0-19.4% under aerobic conditions, which resulted in a 100-180% increase in the Se(VI) removal capacity by ZVI. Se(VI) reduction by Fe 0 was a heterogeneous redox reaction, and the enrichment of Se(VI) on ZVI surface was the first step of electron transfer from Fe 0 core to Se(VI). Oxygen promoted the generation of iron (hydr)oxides, which facilitated the enrichment of Se(VI) on the ZVI particle surface. Therefore, the high oxygen fraction (25-50%) in the purging gas resulted in only a slight decrease in the ES of ZVI. Fe(II) addition resulted in a pH drop and promoted the generation of lepidocrocite and magnetite, which benefited Se(VI) adsorption and the following electron transfer from underlying Fe 0 to surface-located Se(VI).

Electric field induced optical gain of a hydrogenic impurity in a Cd{sub 0.8}Zn{sub 0.2}Se/ZnSe parabolic quantum dot

DOE Office of Scientific and Technical Information (OSTI.GOV)

Jasmine, P. Christina Lily; Peter, A. John, E-mail: a.john.peter@gmail.com

The dependence of electric field on the electronic and optical properties is investigated in a Cd{sub 0.8}Zn{sub 0.2}Se/ZnSe quantum dot. The hydrogenic binding energy, in the presence of electric field, is calculated with the spatial confinement effect. The electric field dependent optical gain with the photon energy is found using compact density matrix method. The results show that the electric field has a great influence on the optical properties of II-VI semiconductor quantum dot.

Electrochemiluminescence energy transfer-promoted ultrasensitive immunoassay using near-infrared-emitting CdSeTe/CdS/ZnS quantum dots and gold nanorods

PubMed Central

Li, Lingling; Chen, Ying; Lu, Qian; Ji, Jing; Shen, Yuanyuan; Xu, Mi; Fei, Rong; Yang, Guohai; Zhang, Kui; Zhang, Jian-Rong; Zhu, Jun-Jie

2013-01-01

The marriage of energy transfer with electrochemiluminescence has produced a new technology named electrochemiluminescence energy transfer (ECL-ET), which can realize effective and sensitive detection of biomolecules. To obtain optimal ECL-ET efficiency, perfect energy overlapped donor/acceptor pair is of great importance. Herein, we present a sensitive ECL-ET based immunosensor for the detection of tumor markers, using energy tunable CdSeTe/CdS/ZnS double shell quantum dots (QDs) and gold nanorods (GNRs) as the donor and acceptor, respectively. Firstly a facile microwave-assisted strategy for the synthesis of green- to near-infrared-emitting CdSeTe/CdS/ZnS QDs with time- and component-tunable photoluminescence was proposed. And, on the basis of the adjustable optical properties of both CdSeTe/CdS/ZnS QDs and GNRs, excellent overlap between donor emission and acceptor absorption can be obtained to ensure effective ECL-ET quenching, thus improving the sensing sensitivity. This method represents a novel approach for versatile detection of biomolecules at low concentrations. PMID:23524874

Charge Versus Energy Transfer in Atomically Thin Graphene-Transition Metal Dichalcogenide van der Waals Heterostructures

NASA Astrophysics Data System (ADS)

Froehlicher, Guillaume; Lorchat, Etienne; Berciaud, Stéphane

2018-01-01

Made from stacks of two-dimensional materials, van der Waals heterostructures exhibit unique light-matter interactions and are promising for novel optoelectronic devices. The performance of such devices is governed by near-field coupling through, e.g., interlayer charge and/or energy transfer. New concepts and experimental methodologies are needed to properly describe two-dimensional heterointerfaces. Here, we report an original study of interlayer charge and energy transfer in atomically thin metal-semiconductor [i.e., graphene-transition metal dichalcogenide (TMD, here molybdenum diselenide, MoSe2 )] heterostructures using a combination of microphotoluminescence and Raman scattering spectroscopies. The photoluminescence intensity in graphene /MoSe2 is quenched by more than 2 orders of magnitude and rises linearly with the incident photon flux, demonstrating a drastically shortened (about 1 ps) room-temperature MoSe2 exciton lifetime. Key complementary insights are provided from a comprehensive analysis of the graphene and MoSe2 Raman modes, which reveals net photoinduced electron transfer from MoSe2 to graphene and hole accumulation in MoSe2 . Remarkably, the steady-state Fermi energy of graphene saturates at 290 ±15 meV above the Dirac point. This reproducible behavior is observed both in ambient air and in vacuum and is discussed in terms of intrinsic factors (i.e., band offsets) and environmental effects. In this saturation regime, balanced photoinduced flows of electrons and holes may transfer to graphene, a mechanism that effectively leads to energy transfer. Using a broad range of incident photon fluxes and diverse environmental conditions, we find that the presence of net photoinduced charge transfer has no measurable impact on the near-unity photoluminescence quenching efficiency in graphene /MoSe2 . This absence of correlation strongly suggests that energy transfer to graphene (either in the form of electron exchange or dipole-dipole interaction) is the dominant interlayer coupling mechanism between atomically thin TMDs and graphene.

Variation of serum selenium concentrations in German sheep flocks and implications for herd health management consultancy.

PubMed

Humann-Ziehank, Esther; Tegtmeyer, Philip C; Seelig, Bjoern; Roehrig, Petra; Ganter, Martin

2013-11-19

This study was performed to demonstrate the widespread distribution and severity of selenium (Se) deficiency in sheep flocks and to evaluate the impact of influencing factors. In 150 flocks, ten serum samples of adult ewes were analysed for Se concentration. The farmers were interviewed concerning flock size, provision of mineral supplement, predominant form of husbandry (stationary fenced pasture/transhumance), predominant form of water provision (tap water/well/surface water) and predominant soil (sandy, silty/loamy, clay) in the area. The location of the flock was recorded as well as the production stage/season at the time of sampling. Intra-group variation and the validity to analyse pooled samples were tested. Pools of five samples correlated well with the mean of individually analysed samples. The intra-group range of serum Se concentration varied enormously (mean 45.4 ± 18.8 μg Se/l). About 60% of the flocks showed mean serum Se concentrations below 80 μg/l, 37.4% were below 60 μg Se/l, representing a Se deficient stage. Using mineral supplement in general was no key factor for Se status. Stationary flocks on fenced pasture had constantly higher mean serum Se concentrations during breeding (outdoors, August-November), lambing (mainly indoors, December-March) and lactation (outdoors, April-July), whereas flocks practising transhumance had significantly lower Se status, except during lambing. There was no significant correlation between the soil type and the Se status, but flocks in Southern Germany tend to show a lower Se status compared to Central and Northern Germany. Increasing flock size was associated with lower mean serum Se concentrations. In stationary flocks only, the use of surface water was accompanied by significantly lower Se status. Se deficiency is widespread in German sheep flocks. More than one third of the flocks showed Se deficiency, indicating the need to optimise the nutritional management. Factors raising suspicion of Se deficiency are large flocks, transhumance during lactation and the breeding season as well as surface water provision in stationary flocks.

Photon-induced selenium migration in TiSe 2

DOE Office of Scientific and Technical Information (OSTI.GOV)

Lioi, David B.; Gosztola, David J.; Wiederrecht, Gary P.

2017-02-20

TiSe 2 is a member of the transition metal dichalcogenide family of layered van der Waals materials which exhibits some distinct electronic and optical properties. Here, we perform Raman spectroscopy and microscopy studies on single crystal TiSe 2 to investigate thermal and photon-induced defects associated with diffusion of selenium to the surface. Additional phonon peaks near 250 cm -1 are observed in the laser- irradiated regions that are consistent with formation of amorphous and nanocrys- talline selenium on the surface. Temperature dependent studies of the threshold temperature and laser intensity necessary to initiate selenium migration to the surface show anmore » activation barrier for the process of 1.55 eV. The impact of these results on the properties of strongly correlated electron states in TiSe 2 are discussed« less

Development and Application of Explicitly Correlated Wave Function Based Methods for the Investigation of Optical Properties of Semiconductor Nanomaterials

NASA Astrophysics Data System (ADS)

Elward, Jennifer Mary

Semiconductor nanoparticles, or quantum dots (QDs), are well known to have very unique optical and electronic properties. These properties can be controlled and tailored as a function of several influential factors, including but not limited to the particle size and shape, effect of composition and heterojunction as well as the effect of ligand on the particle surface. This customizable nature leads to extensive experimental and theoretical research on the capabilities of these quantum dots for many application purposes. However, in order to be able to understand and thus further the development of these materials, one must first understand the fundamental interaction within these nanoparticles. In this thesis, I have developed a theoretical method which is called electron-hole explicitly correlated Hartee-Fock (eh-XCHF). It is a variational method for solving the electron-hole Schrodinger equation and has been used in this work to study electron-hole interaction in semiconductor quantum dots. The method was benchmarked with respect to a parabolic quantum dot system, and ground state energy and electron-hole recombination probability were computed. Both of these properties were found to be in good agreement with expected results. Upon successful benchmarking, I have applied the eh-XCHF method to study optical properties of several quantum dot systems including the effect of dot size on exciton binding energy and recombination probability in a CdSe quantum dot, the effect of shape on a CdSe quantum dot, the effect of heterojunction on a CdSe/ZnS quantum dot and the effect of quantum dot-biomolecule interaction within a CdSe-firefly Luciferase protein conjugate system. As metrics for assessing the effect of these influencers on the electron-hole interaction, the exciton binding energy, electron-hole recombination probability and the average electron-hole separation distance have been computed. These excitonic properties have been found to be strongly infuenced by the changing composition of the particle. It has also been found through this work that the explicitly correlated method performs very well when computing these properties as it provides a feasible computational route to compare to both experimental and other theoretical results.

Superthermal Electron Energy Interchange in the Ionosphere-Plasmasphere System

NASA Technical Reports Server (NTRS)

Khazanov, G. V.; Glocer, A.; Liemohn, M. W.; Himwich, E. W.

2013-01-01

A self-consistent approach to superthermal electron (SE) transport along closed field lines in the inner magnetosphere is used to examine the concept of plasmaspheric transparency, magnetospheric trapping, and SE energy deposition to the thermal electrons. The dayside SE population is generated both by photoionization of the thermosphere and by secondary electron production from impact ionization when the photoelectrons collide with upper atmospheric neutral particles. It is shown that a self-consistent approach to this problem produces significant changes, in comparison with other approaches, in the SE energy exchange between the plasmasphere and the two magnetically conjugate ionospheres. In particular, plasmaspheric transparency can vary by a factor of two depending on the thermal plasma content along the field line and the illumination conditions of the two conjugate ionospheres. This variation in plasmaspheric transparency as a function of thermal plasma and ionospheric conditions increases with L-shell, as the field line gets longer and the equatorial pitch angle extent of the fly-through zone gets smaller. The inference drawn from these results is that such a self-consistent approach to SE transport and energy deposition should be included to ensure robustness in ionosphere-magnetosphere modeling networks.

Investigation of scanning tunneling spectra on iron-based superconductor FeSe 0.5Te 0.5(in Chinese)

DOE PAGES

Du, Z. -Y.; Fang, D. -L.; Wang, Z. -Y.; ...

2015-05-05

FeSe 0.5Te 0.5 single crystals with superconducting critical temperature of 13.5 K are investigated by scanning tunneling microscopy/spectroscopy (STM/STS) measureflents in detail. STM image on the top surface shows an atomically resolved square lattice consisted by white and dark spots with a constant of about 3.73± 0.03 Å which is consistent with the lattice constant 3.78 Å. The Se and Te atoms with a height difference of about 0.35 Å are successfully identified since the sizes of the two kinds of atoms are different. The tunneling spectra show very large zero-bias conductance value and asymmetric coherent peaks in the superconductingmore » state. According to the positions of coherence peaks, we determine the superconducting gap 2Δ = 5.5 meV, and the reduced gap 2Δ/kBTc = 4.9 is larger than the value predicted by the weak-coupling BCS theory. The zero-bias conductance at 1.7 K only have a decrease of about 40% compared with the normal state conductance, which may originate from some scattering and broadening mechanism in the material. This broadening effect will also make the superconducting gap determined by the distance between the coherence peaks larger than the exact gap value. The asymmetric structure of the tunneling spectra near the superconducting gap is induced by the hump on the background. This hump appears at temperature more than twice the superconducting critical temperature. This kind of hump has also been observed in other iron pnictides and needs further investigation. A possible bosonic mode outside the coherence peak with a mode energy Ω of about 5.5 meV is observed in some tunneling spectra, and the ratio between the mode energy and superconducting transition temperature Ω/kBTc ≈ 4.7 is roughly consistent with the universal ratio 4.3 in iron-based superconductors. The high-energy background of the spectra beyond the superconducting gaps shows a V-shape feature. The slopes of the differential conductance spectra at high energy are very different in the areas of Te-atom cluster and Se-atom cluster, and the difference extends to the energy of more than 300 meV. The differential conductance mapping has very little information about the quasi-particle interference of the superconducting state, which may result from the other strong scattering mechanism in the sample.« less

Investigation of scanning tunneling spectra on iron-based superconductor FeSe 0.5Te 0.5 (in Chinese)

DOE Office of Scientific and Technical Information (OSTI.GOV)

Du, Z. -Y.; Fang, D. -L.; Wang, Z. -Y.

FeSe 0.5Te 0.5 single crystals with superconducting critical temperature of 13.5 K are investigated by scanning tunneling microscopy/spectroscopy (STM/STS) measureflents in detail. STM image on the top surface shows an atomically resolved square lattice consisted by white and dark spots with a constant of about 3.73± 0.03 Å which is consistent with the lattice constant 3.78 Å. The Se and Te atoms with a height difference of about 0.35 Å are successfully identified since the sizes of the two kinds of atoms are different. The tunneling spectra show very large zero-bias conductance value and asymmetric coherent peaks in the superconductingmore » state. According to the positions of coherence peaks, we determine the superconducting gap 2Δ = 5.5 meV, and the reduced gap 2Δ/kBTc = 4.9 is larger than the value predicted by the weak-coupling BCS theory. The zero-bias conductance at 1.7 K only have a decrease of about 40% compared with the normal state conductance, which may originate from some scattering and broadening mechanism in the material. This broadening effect will also make the superconducting gap determined by the distance between the coherence peaks larger than the exact gap value. The asymmetric structure of the tunneling spectra near the superconducting gap is induced by the hump on the background. This hump appears at temperature more than twice the superconducting critical temperature. This kind of hump has also been observed in other iron pnictides and needs further investigation. A possible bosonic mode outside the coherence peak with a mode energy Ω of about 5.5 meV is observed in some tunneling spectra, and the ratio between the mode energy and superconducting transition temperature Ω/kBTc ≈ 4.7 is roughly consistent with the universal ratio 4.3 in iron-based superconductors. The high-energy background of the spectra beyond the superconducting gaps shows a V-shape feature. The slopes of the differential conductance spectra at high energy are very different in the areas of Te-atom cluster and Se-atom cluster, and the difference extends to the energy of more than 300 meV. The differential conductance mapping has very little information about the quasi-particle interference of the superconducting state, which may result from the other strong scattering mechanism in the sample.« less

A DFT study on surface-enhanced Raman spectroscopy of aromatic dithiol derivatives adsorbed on gold nanojunctions

NASA Astrophysics Data System (ADS)

You, Tingting; Lang, Xiufeng; Huang, Anping; Yin, Penggang

2018-01-01

A computational study on aromatic dithiol derivatives (HS-Ar-X-Ar-SH, X = O, S, Se, NH, CH2, Ndbnd N, CHdbnd CH, Ctbnd C) interacting with gold cluster(s) was presented to investigate the chemical enhancement mechanism related to surface-enhanced Raman spectroscopy (SERS) for molecular junctions. Density functional theory (DFT) were performed on derivatives molecules as well as their single-end-linked (SEL) or double-end-linked (DEL) complexes for geometric, spectra, electronic and excitation properties, leading to discussions on dominant factor during SERS process. The resulted enhancement factors of SEL and DEL complexes exhibited specific dependency on linking atom or functional group between two phenyls, which was in accordance with the variation of polarizabilities and molecule-cluster transition energy.

Attenuation of the cortisol response to stress in female rainbow trout chronically exposed to dietary selenomethionine.

PubMed

Wiseman, Steve; Thomas, Jith K; McPhee, Landon; Hursky, Olesya; Raine, Jason C; Pietrock, Michael; Giesy, John P; Hecker, Markus; Janz, David M

2011-10-01

Selenomethionine (Se-Met) is the major dietary form of selenium (Se). While Se is a required nutrient, it can also influence the physiological stress response because it stimulates greater concentrations of cortisol in blood plasma of exposed fish. However, little is known about the effects of exposure to Se on the ability to cope with a secondary stressor. In the current study, female rainbow trout were exposed to an environmentally relevant dietary concentration (8.47 mg Se/kg dry mass (dm)) of Se-Met for 126 d, after which time fish were subjected to a 3-min handling stressor and sampled at 2h and 24h post-stressor exposure. Concentrations of cortisol, cortisone, glucose, and lactate in blood plasma and concentrations of glycogen and triglycerides in liver and muscle were determined. Abundances of transcripts of proteins involved in corticosteroidogenesis were determined using quantitative RT-PCR. Concentrations of cortisol were significantly greater in blood plasma of trout exposed to Se-Met, relative to control trout sampled prior to the handling stressor. A typical response of cortisol to the handling stressor was observed in the control trout. However, trout exposed to Se-Met were unable to mount a cortisol response to the handling stressor. Concentrations of cortisone, the inactive metabolite of cortisol, were significantly greater following the handling stressor in trout exposed to Se-Met. In trout exposed to Se-Met, transcript abundance of melanocortin 2 receptor (mc2r) and peripheral benzodiazepine receptor (pbr) were greater, which is consistent with the conclusion that synthesis of cortisol was greater. However, abundances of transcripts of cytochrome P450 side-chain cleavage (p450scc) and cytochrome P450 11B1 (cyp11b1) were not significantly different between controls and Se-Met exposed trout. Exposure to Se-Met affected accumulation and tissue partitioning of glycogen and triglycerides in liver and muscle as concentrations of these energy reserves were greater in muscle, but not liver. Concentrations of glycogen and triglycerides in muscle, but not in liver, were lesser following the handling stressor suggesting that the muscle energy reserves are an important source of energy required for recovery from the handling stressor. The results of the study demonstrate that chronic exposure to dietary Se-Met elicits a stress response, but prevents a cortisol response to a secondary handling stressor, most likely due to cortisol inactivation. Moreover, exposure to Se-Met has effects on concentrations of energy reserves that are important for providing the energy necessary to cope with a secondary stressor. Copyright © 2011 Elsevier B.V. All rights reserved.

Visible light to electrical energy conversion using photoelectrochemical cells

NASA Technical Reports Server (NTRS)

Wrighton, Mark S. (Inventor); Ellis, Arthur B. (Inventor); Kaiser, Steven W. (Inventor)

1983-01-01

Sustained conversion of low energy visible or near i.r. light (>1.25 eV) to electrical energy has been obtained using wet photoelectrochemical cells where there are no net chemical changes in the system. Stabilization of n-type semi-conductor anodes of CdS, CdSe, CdTe, GaP, GaAs and InP to photoanodic dissolution is achieved by employing selected alkaline solutions of Na.sub.2 S, Na.sub.2 S/S, Na.sub.2 Se, Na.sub.2 Se/Se, Na.sub.2 Te and Na.sub.2 Te/Te as the electrolyte. The oxidation of (poly) sulfide, (poly)selenide or (poly)telluride species occurs at the irradiated anode, and reduction of polysulfide, polyselenide or polytelluride species occurs at the dark Pt cathode of the photoelectrochemical cell. Optical to electrical energy conversion efficiencies approaching 15% at selected frequencies have been observed in some cells. The wavelength for the onset of photocurrent corresponds to the band gap of the particular anode material used in the cell.

Magneto-optical spectrum and the effective excitonic Zeeman splitting energies of Mn and Co-doped CdSe nanowires

DOE Office of Scientific and Technical Information (OSTI.GOV)

Xiong, Wen, E-mail: wenxiong@cqu.edu.cn; Chen, Wensuo

2013-12-21

The electronic structure of Mn and Co-doped CdSe nanowires are calculated based on the six-band k·p effective-mass theory. Through the calculation, it is found that the splitting energies of the degenerate hole states in Mn-doped CdSe nanowires are larger than that in Co-doped CdSe nanowires when the concentration of these two kinds of magnetic ions is the same. In order to analysis the magneto-optical spectrum of Mn and Co-doped CdSe nanowires, the four lowest electron states and the four highest hole states are sorted when the magnetic field is applied, and the 10 lowest optical transitions between the conduction subbandsmore » and the valence subbands at the Γ point in Mn and Co-doped CdSe nanowires are shown in the paper, it is found that the order of the optical transitions at the Γ point almost do not change although two different kinds of magnetic ions are doped in CdSe nanowires. Finally, the effective excitonic Zeeman splitting energies at the Γ point are found to increase almost linearly with the increase of the concentration of the magnetic ions and the magnetic field; meanwhile, the giant positive effective excitonic g factors in Mn and Co-doped CdSe nanowires are predicted based on our theoretical calculation.« less

A fluorescence resonance energy transfer-derived structure of a quantum dot-protein bioconjugate nanoassembly

PubMed Central

Medintz, I. L.; Konnert, J. H.; Clapp, A. R.; Stanish, I.; Twigg, M. E.; Mattoussi, H.; Mauro, J. M.; Deschamps, J. R.

2004-01-01

The first generation of luminescent semiconductor quantum dot (QD)-based hybrid inorganic biomaterials and sensors is now being developed. It is crucial to understand how bioreceptors, especially proteins, interact with these inorganic nanomaterials. As a model system for study, we use Rhodamine red-labeled engineered variants of Escherichia coli maltose-binding protein (MBP) coordinated to the surface of 555-nm emitting CdSe-ZnS core–shell QDs. Fluorescence resonance energy transfer studies were performed to determine the distance from each of six unique MBP-Rhodamine red dye-acceptor locations to the center of the energy-donating QD. In a strategy analogous to a nanoscale global positioning system determination, we use the intraassembly distances determined from the fluorescence resonance energy transfer measurements, the MBP crystallographic coordinates, and a least-squares approach to determine the orientation of the MBP relative to the QD surface. Results indicate that MBP has a preferred orientation on the QD surface. The refined model is in agreement with other evidence, which indicates coordination of the protein to the QD occurs by means of its C-terminal pentahistidine tail, and the size of the QD estimated from the model is in good agreement with physical measurements of QD size. The approach detailed here may be useful in determining the orientation of proteins in other hybrid protein–nanoparticle materials. To our knowledge, this is the first structural model of a hybrid luminescent QD-protein receptor assembly elucidated by using spectroscopic measurements in conjunction with crystallographic and other data. PMID:15210939

Agrobacterium-assisted selenium nanoparticles: molecular aspect of antifungal activity

NASA Astrophysics Data System (ADS)

Kumar, Anil; Bera, Smritilekha; Singh, Man; Mondal, Dhananjoy

2018-03-01

Selenium nanoparticles (SeNPs) were synthesized through the bioreduction of sodium selenite (Na2SeO3) using gram-negative agrobacterium (AGBT) species. Subsequently, their physicochemical properties (pH, viscosity and surface tension) and medicinal activities as anti-dermatophyte against soil keratinophilic fungi at the molecular level were assessed. UV-visible and FTIR spectroscopic data of the biologically synthesized SeNPs were then recorded for confirming the presence of native biological materials adhered to nanoparticles, which are inherently required to enhance the stability and solubility through inhibition of the nanoparticle’s natural aggregation and agglomeration. The λ max value between 290-300 nm in the absorption spectra of the biogenic materials in different concentrations of the Na2SeO3 corroborated the presence of SeNPs in the solution. The interaction of SeNPs in solution state was further studied through the determination of pH, viscosity and surface tension values of agrobacterium-derived SeNPs in different solvents. The pH value of SeNPs dispersed in water is reported as above 7.0 and the average viscosity, and surface tensions of the SeNPs are appeared as near to the water. The particle size distribution was further determined by DLS and the highest % of particle size of the synthesized SeNPs is found in between 200-300 nm. The anti-dermatophyte activity and molecular interaction with fungi DNA molecules were assessed providing the highest anti-dermatophyte activity at 0.1 M concentration and it is observed that the quantities and qualities of fungi DNA were affected by SeNPs. Considering all the outcomes of the studies together, our findings suggest that agrobacterium-mediated synthesis of SeNPs is dependent on bacterial metabolisms but not on the concentration of Na2SeO3 and are promising selenium-derived species with potential application in the prevention of fungal infection through denaturation of fungi DNA.

Number distribution of emitted electrons by MeV H+ impact on carbon

NASA Astrophysics Data System (ADS)

Ogawa, H.; Koyanagi, Y.; Hongo, N.; Ishii, K.; Kaneko, T.

2017-09-01

The statistical distributions of the number of the forward- and backward-emitted secondary electrons (SE's) from a thin carbon foil have been measured in coincidence with foil-transmitted H+ ions of 0.5-3.0 MeV in every 0.5 MeV step. The measured SE energy spectra were fitted by assuming a Pólya distribution for the simultaneous n-SE emission probabilities. For our previous data with a couple of the carbon foils with different thicknesses, a similar analysis has been carried out. As a result, it was found that the measured spectra could be reproduced as well as by an analysis without placing any restriction on the emission probabilities both for the forward and backward SE emission. The obtained b-parameter of the Pólya distribution, which is a measure of the deviation from a Poisson distribution due to the cascade multiplication by high energy internal SE's, increases monotonically with the incident energy of proton beams. On the other hand, a clear foil-thickness dependence is not observed for the b-parameter. A theoretical model which could reproduced the magnitude of the b-parameter for the SE energy spectra obtained with thick Au, Cu and Al targets is found to overestimates our values for thin carbon foils significantly. Another model calculation is found to reproduce our b-values very well.

Density-functional theory computer simulations of CZTS{sub 0.25}Se{sub 0.75} alloy phase diagrams

DOE Office of Scientific and Technical Information (OSTI.GOV)

Chagarov, E.; Sardashti, K.; Kummel, A. C.

2016-08-14

Density-functional theory simulations of CZTS, CZTSe, and CZTS{sub 0.25}Se{sub 0.75} photovoltaic compounds have been performed to investigate the stability of the CZTS{sub 0.25}Se{sub 0.75} alloy vs. decomposition into CZTS, CZTSe, and other secondary compounds. The Gibbs energy for vibrational contributions was estimated by calculating phonon spectra and thermodynamic properties at finite temperatures. It was demonstrated that the CZTS{sub 0.25}Se{sub 0.75} alloy is stabilized not by enthalpy of formation but primarily by the mixing contributions to the Gibbs energy. The Gibbs energy gains/losses for several decomposition reactions were calculated as a function of temperature with/without intermixing and vibration contributions to themore » Gibbs energy. A set of phase diagrams was built in the multidimensional space of chemical potentials at 300 K and 900 K temperatures to demonstrate alloy stability and boundary compounds at various chemical conditions. It demonstrated for CZTS{sub 0.25}Se{sub 0.75} that the chemical potentials for stability differ between typical processing temperature (∼900 K) and operating temperature (300 K). This implies that as cooling progresses, the flux/concentration of S should be increased in MBE growth to maintain the CZTS{sub 0.25}Se{sub 0.75} in a thermodynamically stable state to minimize phase decomposition.« less

Optical Characterization of Bulk ZnSeTe Solid Solutions

NASA Technical Reports Server (NTRS)

Su, Ching-Hua; Feth, S.; Zhu, Shen; Lehoczky, S. L.; Wang, Ling Jun

2000-01-01

Optical characterization was performed on wafers sliced from crystals of ZnSe, ZnTe and ZnSe (sub 1-x) Te (sub x) (0 less than x less than 0.4) grown by physical vapor transport technique. The energy band gaps at room temperature were determined from optical transmission measurements on 11 wafers. The best fit to the band gap vs. composition, x, data gives a bowing parameter of 1.336 which is between the value of 1.23 determined previously on ZnSeTe bulk crystals by reflectivity and the value of 1.621 reported on epilayers by photoconductivity. Low-temperature photoluminescence (PL) spectra were measured on 6 samples. The spectra of ZnSe and ZnTe were dominated by near band edge emissions and no deep donor-acceptor pairs were observed. The PL spectrum exhibited a broad emission for each of the ZnSe (sub 1-x) Te (sub x) samples, 0.09 less than x less than 0.39. For x = 0.09, this emission energy is about 0.2eV lower than the band gap energy measured at low temperature. As x increases the energy discrepancy gradually decreases and reduces to almost zero at x = 0.4. The single broad PL emission spectra and the spectra measured as a function of temperature were interpreted to be associated with the exciton bound to Te clusters because of the high Te content in these samples.

Effect of van der Waals interactions on the structural and binding properties of GaSe

DOE Office of Scientific and Technical Information (OSTI.GOV)

Sarkisov, Sergey Y., E-mail: sarkisov@mail.tsu.ru; Kosobutsky, Alexey V., E-mail: kosobutsky@kemsu.ru; Kemerovo State University, Krasnaya 6, 650043 Kemerovo

The influence of van der Waals interactions on the lattice parameters, band structure, elastic moduli and binding energy of layered GaSe compound has been studied using projector-augmented wave method within density functional theory. We employed the conventional local/semilocal exchange-correlation functionals and recently developed van der Waals functionals which are able to describe dispersion forces. It is found that application of van der Waals density functionals allows to substantially increase the accuracy of calculations of the lattice constants a and c and interlayer distance in GaSe at ambient conditions and under hydrostatic pressure. The pressure dependences of the a-parameter, Ga–Ga, Ga–Semore » bond lengths and Ga–Ga–Se bond angle are characterized by a relatively low curvature, while c(p) has a distinct downward bowing due to nonlinear shrinking of the interlayer spacing. From the calculated binding energy curves we deduce the interlayer binding energy of GaSe, which is found to be in the range 0.172–0.197 eV/layer (14.2–16.2 meV/Å{sup 2}). - Highlights: • Effects of van der Waals interactions are analyzed using advanced density functionals. • Calculations with vdW-corrected functionals closely agree with experiment. • Interlayer binding energy of GaSe is estimated to be 14.2–16.2 meV/Å{sup 2}.« less

Optimal packing size of non-ligated CdSe nanoclusters for microstructure synthesis

DOE Office of Scientific and Technical Information (OSTI.GOV)

Tefera, Anteneh G.; Mochena, Mogus D.; Johnson, Elijah

2014-09-14

Structural and electrostatic properties of nanoclusters of CdSe of diameter 1–2 nm are studied with first principle calculations to determine the optimal size for synthesizing microstructures. Based on robustness of the core structure, i.e., the retention of tetrahedral geometry, hexagonal ring structure, and overall wu{sup ¨}rtzite structure to surface relaxations, we conclude that nanoclusters of ~2 nm diameter are the best candidates to form a dense microstructure with minimal interstitial space. Se-terminated surfaces retain a zigzag structure as Se atoms are pulled out and Cd atoms are pulled in due to relaxation, therefore, are best suited for inter-nanocluster formations.

Understanding catalyst behavior during in situ heating through simultaneous secondary and transmitted electron imaging

DOE PAGES

Howe, Jane Y.; Allard, Jr., Lawrence Frederick; Demers, Hendrix; ...

2014-11-14

In situ heating study via a simultaneous secondary electron (SE) and transmitted electron (TE) microscopy is extremely insightful because information from the surface (SE) and bulk (TE) can be readily obtained. The leached Au/Fe 2O 3 catalyst has voids on the surface of Fe 2O 3. Upon heating to 500 °C, voids shrank and disappeared, while internal Au species diffused to the surface to form new nanoparticles. Heating in vacuum reduced Fe 2O 3 to Fe 3O 4. Heating at 700 °C caused coalescence and growth of Au particles and formation of faceted Fe 3O 4 surfaces. We achieved 1.1more » nm resolution in SE imaging during in situ heating.« less

SPECTROSCOPIC INVESTIGATION OF (NH4)2S TREATED GaSeTe FOR RADIATION DETECTOR APPLICATIONS

DOE Office of Scientific and Technical Information (OSTI.GOV)

Nelson, A; Laurence, T; Conway, A

2009-08-04

The surface of the layered III-VI chalcogenide semiconductor GaSeTe was treated with (NH{sub 4}){sub 2}S at 60 C to modify the surface chemistry and determine the effect on transport properties. Room temperature photoluminescence (PL) measurements were used to assess the effect of the (NH{sub 4}){sub 2}S treatment on surface defect states. Evaluation of the subsequent surface chemistry was performed with high-resolution core-level photoemission measurements. Metal overlayers were deposited on the (NH{sub 4}){sub 2}S treated surfaces and the I-V characteristics were measured. The measurements were correlated to understand the effect of (NH{sub 4}){sub 2}S modification of the interfacial electronic structure withmore » the goal of optimizing the metal/GaSeTe interface for radiation detector devices.« less

Possibilities of new materials surface sensibility express determination based on ZnSe-CdS system by pH isoelectric state measurements of the surface state

NASA Astrophysics Data System (ADS)

Kirovskaya, I. A.; Mironova, E. V.; Ushakov, O. V.; Nor, P. E.; Yureva, A. V.; Matyash, Yu I.

2018-01-01

A method for determining the hydrogen index of the surfaces isoelectric state (pHiso) at various gases pressures -possible components of the surrounding and technological media has been developed. With its use, changes in pH of binary and more complex semiconductors-components of the new system-ZnSe-CdS under the influence of nitrogen dioxide-have been found. The limiting sensitivity of surfaces - minimum PNO2, causing a change in pH has been estimated. The most active components of ZnSe-CdS system, recommended as materials for measuring cells of NO2, have been revealed. The relationship between the changing patterns with the composition of surface (acid-base) and bulk (in particular, theoretical calculated crystal density) properties has been established, allowing to find the most effective materials for sensor technology and for semiconductor analysis.

Spin accumulation in disordered topological insulator ultrathin films

NASA Astrophysics Data System (ADS)

Siu, Zhuo Bin; Ho, Cong Son; Tan, Seng Ghee; Jalil, Mansoor B. A.

2017-08-01

Topological insulator (TI) ultrathin films differ from the more commonly studied semi-infinite bulk TIs in that the former possess both top and bottom surfaces where the surface states localized at different surfaces can couple to one another across the finite thickness of the film. In the presence of an in-plane magnetization, the TI thin films display two distinct phases depending on which of the inter-surface coupling or the magnetization is stronger. In this work, we consider a Bi2Se3 TI thin film system with an in-plane magnetization and numerically calculate the resulting spin accumulation on both surfaces of the film due to an in-plane electric field to linear order. We describe a numerical scheme for performing the Kubo formula calculation in which we include impurity scattering and vertex corrections. We find that the sums of the spin accumulation over the two surfaces in the in-plane direction perpendicular to the magnetization and in the out of plane direction are antisymmetric in Fermi energy around the charge neutrality point and are non-vanishing only when the symmetry between the top and bottom TI surfaces is broken. The impurity scattering, in general, diminishes the magnitude of the spin accumulation.

Direct evidence of superconductivity and determination of the superfluid density in buried ultrathin FeSe grown on SrTiO3

NASA Astrophysics Data System (ADS)

Biswas, P. K.; Salman, Z.; Song, Q.; Peng, R.; Zhang, J.; Shu, L.; Feng, D. L.; Prokscha, T.; Morenzoni, E.

2018-05-01

Bulk FeSe is superconducting with a critical temperature Tc≅8 K and SrTiO3 is insulating in nature, yet high-temperature superconductivity has been reported at the interface between a single-layer FeSe and SrTiO3. Angle-resolved photoemission spectroscopy and scanning tunneling microscopy measurements observe a gap opening at the Fermi surface below ≈60 K. Elucidating the microscopic properties and understanding the pairing mechanism of single-layer FeSe is of utmost importance as it is a basic building block of iron-based superconductors. Here, we use the low-energy muon spin rotation/relaxation technique to detect and quantify the supercarrier density and determine the gap symmetry in FeSe grown on SrTiO3 (100). Measurements in applied field show a temperature-dependent broadening of the field distribution below ˜60 K, reflecting the superconducting transition and formation of a vortex state. Zero-field measurements rule out the presence of magnetism of static or fluctuating origin. From the inhomogeneous field distribution, we determine an effective sheet supercarrier density ns2 D≃6 ×1014cm-2 at T →0 K, which is a factor of 4 larger than expected from ARPES measurements of the excess electron count per Fe of 1 monolayer FeSe. The temperature dependence of the superfluid density ns(T ) can be well described down to ˜10 K by simple s -wave BCS, indicating a rather clean superconducting phase with a gap of 10.2(1.1) meV. The result is a clear indication of the gradual formation of a two-dimensional vortex lattice existing over the entire large FeSe/STO interface and provides unambiguous evidence for robust superconductivity below 60 K in ultrathin FeSe.

A new signal amplification strategy of photoelectrochemical immunoassay for highly sensitive interleukin-6 detection based on TiO2/CdS/CdSe dual co-sensitized structure.

PubMed

Fan, Gao-Chao; Ren, Xiao-Lin; Zhu, Cheng; Zhang, Jian-Rong; Zhu, Jun-Jie

2014-09-15

Dual co-sensitized structure of TiO2/CdS/CdSe was designed to develop a novel photoelectrochemical immunoassay for highly sensitive detection of human interleukin-6 (IL-6). To construct a sensing electrode, TiO2/CdS hybrid was prepared by successive adsorption and reaction of Cd(2+) and S(2-) ions on the surface of TiO2 and then was employed as matrix for immobilization of anti-IL-6 antibody, whereas CdSe QDs linked to IL-6 were used for signal amplification via the specific antibody-antigen immunoreaction between anti-IL-6 and IL-6-CdSe bioconjugate. Greatly enhanced sensitivity for IL-6 detection was derived from the new co-sensitization signal amplification strategy. First, the TiO2/CdS/CdSe co-sensitized structure extended the absorption range to long wavelength of white light, which adequately utilized the light energy. Second, the TiO2/CdS/CdSe co-sensitized structure possessed stepwise band-edge levels favoring ultrafast transfer of photogenerated electrons and significantly prompted the photoelectrochemical performance. Besides, the introduction of CdSe effectively prevented the recombination of photogenerated electrons in the conduction band of CdS, further causing an enhanced photocurrent. Accordingly, upon the co-sensitization strategy, a novel immunoassay based on the competitive binding of anti-IL-6 antibody with IL-6 antigen and IL-6-CdSe bioconjugate was developed, and it exhibited a wide linear range from 1.0 pg/mL to 100 ng/mL with a low detection limit of 0.38 pg/mL for IL-6 detection. The proposed co-sensitization strategy presented high sensitivity, reproducibility, specificity and stability, and also opened up a new promising platform for detection of other biomarkers. Copyright © 2014 Elsevier B.V. All rights reserved.

Lead and selenite adsorption at water–goethite interfaces from first principles

DOE Office of Scientific and Technical Information (OSTI.GOV)

Leung, Kevin; Criscenti, Louise J.

Here, the complexation of toxic and/or radioactive ions on to mineral surfaces is an important topic in geochemistry. We apply periodic-boundary-conditions density functional theory (DFT) molecular dynamics simulations to examine the coordination of Pb(II),more » $${\\rm SeO}_3^{2-}$$ , and their contact ion pairs to goethite (1 0 1) and (2 1 0) surfaces. The multitude of Pb(II) adsorption sites and possibility of Pb(II)-induced FeOH deprotonation make this a complex problem. At surface sites where Pb(II) is coordinated to three FeO and/or FeOH groups, and with judicious choices of FeOH surface group protonation states, the predicted Fe–Pb distances are in good agreement with EXAFS measurements. Trajectories where Pb(II) is in part coordinated to only two surface Fe–O groups exhibit larger fluctuations in Pb–O distances. Pb(II)/$${\\rm SeO}_3^{2-}$$ contact ion pairs are at least metastable on goethite (2 1 0) surfaces if the $${\\rm SeO}_3^{2-}$$ has a monodentate Se–O–Fe bond. Our DFT-based molecular dynamics calculations are a prerequisite for calculations of finite temperature equilibrium binding constants of Pb(II) and Pb(II)/$${\\rm SeO}_3^{2-}$$ ion pairs to goethite adsorption sites.« less

Lead and selenite adsorption at water–goethite interfaces from first principles

DOE PAGES

Leung, Kevin; Criscenti, Louise J.

2017-08-04

Here, the complexation of toxic and/or radioactive ions on to mineral surfaces is an important topic in geochemistry. We apply periodic-boundary-conditions density functional theory (DFT) molecular dynamics simulations to examine the coordination of Pb(II),more » $${\\rm SeO}_3^{2-}$$ , and their contact ion pairs to goethite (1 0 1) and (2 1 0) surfaces. The multitude of Pb(II) adsorption sites and possibility of Pb(II)-induced FeOH deprotonation make this a complex problem. At surface sites where Pb(II) is coordinated to three FeO and/or FeOH groups, and with judicious choices of FeOH surface group protonation states, the predicted Fe–Pb distances are in good agreement with EXAFS measurements. Trajectories where Pb(II) is in part coordinated to only two surface Fe–O groups exhibit larger fluctuations in Pb–O distances. Pb(II)/$${\\rm SeO}_3^{2-}$$ contact ion pairs are at least metastable on goethite (2 1 0) surfaces if the $${\\rm SeO}_3^{2-}$$ has a monodentate Se–O–Fe bond. Our DFT-based molecular dynamics calculations are a prerequisite for calculations of finite temperature equilibrium binding constants of Pb(II) and Pb(II)/$${\\rm SeO}_3^{2-}$$ ion pairs to goethite adsorption sites.« less

Effect of annealing on the optical properties of amorphous Se79Te10Sb4Bi7 thin films

NASA Astrophysics Data System (ADS)

Nyakotyo, H.; Sathiaraj, T. S.; Muchuweni, E.

2017-07-01

Thin films of Se79Te10Sb4Bi7, were prepared by Electron beam deposition technique. The structure of the as-prepared and annealed films has been studied by X-ray diffraction and the surface morphology by the scanning electron microscope (SEM). These studies show that there is a gradual change in structure and the formation of some polycrystalline structures in the amorphous phases is observed when the Se79Te10Sb4Bi7 film is annealed in the temperature range of 333-393 K. The optical transmission of these films has been studied as a function of photon wavelength in the range 300-2500 nm. It has been found that the optical band gap Egopt decreased with increasing annealing temperature in the range 333-393 K. The Urbach energy (Eu), optical conductivity (σopt), imaginary (εi), and real (εr) parts of the complex dielectric constant (ε) and lattice dielectric constant (εL) were also determined. The changes noticed in optical parameters with increasing annealing temperature were explained on the basis of structural relaxation as well as change in defect states and density of localized states due to amorphous-crystalline transformation.

Analysis of the electrodeposition and surface chemistry of CdTe, CdSe, and CdS thin films through substrate-overlayer surface-enhanced Raman spectroscopy.

PubMed

Gu, Junsi; Fahrenkrug, Eli; Maldonado, Stephen

2014-09-02

The substrate-overlayer approach has been used to acquire surface enhanced Raman spectra (SERS) during and after electrochemical atomic layer deposition (ECALD) of CdSe, CdTe, and CdS thin films. The collected data suggest that SERS measurements performed with off-resonance (i.e. far from the surface plasmonic wavelength of the underlying SERS substrate) laser excitation do not introduce perturbations to the ECALD processes. Spectra acquired in this way afford rapid insight on the quality of the semiconductor film during the course of an ECALD process. For example, SERS data are used to highlight ECALD conditions that yield crystalline CdSe and CdS films. In contrast, SERS measurements with short wavelength laser excitation show evidence of photoelectrochemical effects that were not germane to the intended ECALD process. Using the semiconductor films prepared by ECALD, the substrate-overlayer SERS approach also affords analysis of semiconductor surface adsorbates. Specifically, Raman spectra of benzenethiol adsorbed onto CdSe, CdTe, and CdS films are detailed. Spectral shifts in the vibronic features of adsorbate bonding suggest subtle differences in substrate-adsorbate interactions, highlighting the sensitivity of this methodology.

[Effects of different surface conditioning agents on the bond strength of resin-opaque porcelain composite].

PubMed

Liu, Wenjia; Fu, Jing; Liao, Shuang; Su, Naichuan; Wang, Hang; Liao, Yunmao

2014-04-01

The objective of this research is to evaluate the effects of different silane coupling agents on the bond strength between Ceramco3 opaque porcelain and indirect composite resin. Five groups of Co-Cr metal alloy substrates were fabricated according to manufacturer's instruction. The surface of metal alloy with a layer of dental opaque porcelain was heated by fire. After the surface of opaque porcelain was etched, five different surface treatments, i.e. RelyX Ceramic Primer (RCP), Porcelain Bond Activator and SE Bond Primer (mixed with a proportion of 1:1) (PBA), Shofu Porcelain Primer (SPP), SE bond primer (SEP), and no primer treatment (as a control group), were used to combine P60 and opaque porcelain along with resin cement. Shear bond strength of specimens was tested in a universal testing machine. The failure modes of specimens in all groups were observed and classified into four types. Selected specimens were subjected to scanning electron microscope and energy disperse spectroscopy to reveal the relief of the fracture surface and to confirm the failure mode of different types. The experimental results showed that the values of the tested items in all the tested groups were higher than that in the control group. Group PBA exhibited the highest value [(37.52 +/- 2.14) MPa] and this suggested a fact that all of the specimens in group PBA revealed combined failures (failure occurred in metal-porcelain combined surface and within opaque porcelain). Group SPP and RCP showed higher values than SEP (P < 0.05) and most specimens of SPP and RCP performed combined failures (failure occurred in bond surface and within opaque porcelain or composite resin) while all the specimens in group SEP and control group revealed adhesive failures. Conclusions could be drawn that silane coupling agents could reinforce the bond strength of dental composite resin to metal-opaque porcelain substrate. The bond strength between dental composite resin and dental opaque porcelain could meet the clinical requirements.

Thermodynamics of Manganese Oxides at Bulk and Nanoscale: Phase Formation, Transformation, Oxidation-Reduction, and Hydration

NASA Astrophysics Data System (ADS)

Birkner, Nancy R.

Natural manganese oxides are generally formed in surficial environments that are near ambient temperature and water-rich, and may be exposed to wet-dry cycles and a variety of adsorbate species that influence dramatically their level of hydration. Manganese oxide minerals are often poorly crystalline, nanophase, and hydrous. In the near-surface environment they are involved in processes that are important to life, such as water column oxygen cycling, biomineralization, and transport of minerals/nutrients through soils and water. These processes, often involving transformations among manganese oxide polymorphs, are governed by a complex interplay between thermodynamics and kinetics. Manganese oxides are also used in technology as catalysts, and for other applications. The major goal of this dissertation is to examine the energetics of bulk and nanophase manganese oxide phases as a function of particle size, composition, and surface hydration. Careful synthesis and characterization of manganese oxide phases with different surface areas provided samples for the study of enthalpies of formation by high temperature oxide melt solution calorimetry and of the energetics of water adsorption on their surfaces. These data provide a quantitative picture of phase stability and how it changes at the nanoscale. The surface energy of the hydrous surface of Mn3O4 is 0.96 +/- 0.08 J/m2, of Mn2O3 is 1.29 +/- 0.10 J/m2, and of MnO2 is 1.64 +/- 0.10 J/m2. The surface energy of the anhydrous surface of Mn3O4 is 1.62 +/- 0.08 J/m 2, of Mn2O3 is 1.77 +/- 0.10 J/m 2, and of MnO2 is 2.05 +/- 0.10 J/m2. Supporting preliminary findings (Navrotsky et al., 2010), the spinel phase (Mn3O4) has a lower surface energy (more stabilizing) than bixbyite, while the latter has a smaller surface energy than pyrolusite. These differences significantly change the positions in oxygen fugacity---temperature space of the redox couples Mn3O4-Mn2O 3 and Mn2O3-MnO2 favoring the lower surface enthalpy phase (the spinel Mn3O4) for smaller particle size and in the presence of surface hydration. Chemisorption of water onto anhydrous nanophase Mn2O 3 surfaces promotes rapidly reversible redox phase changes at room temperature as confirmed by calorimetry, X-ray diffraction, and titration for manganese average oxidation state. Water adsorption microcalorimetry (in situ) at room temperature measured the strongly exothermic integral enthalpy of water adsorption (-103.5 kJ/mol) and monitored the energetics of the redox phase transformation. Hydration-driven redox transformation of anhydrous nanophase Mn(III) 2O3, (high surface enthalpy of anhydrous surfaces 1.77 +/- 0.10 J/m2) to Mn(II,III)3O4 (lower surface enthalpy 0.96 +/- 0.08 J/m2) occurred during the first few doses of water vapor. Surface reduction of nanoparticle bixbyite (Mn 2O3) to hausmannite (Mn3O4) occurs under conditions where no such reactions are seen or expected on grounds of bulk thermodynamics in coarse-grained materials. Layered structure manganese oxides contain alkali or alkaline earth cations and water, are generally fine-grained, and have considerable thermodynamic stability. The surface enthalpies (SE) of layered and tunnel structure complex manganese oxides are significantly lower than those of the binary manganese oxide phases. The SE for hydrous surfaces and overall manganese average oxidation state (AOS) (value in parentheses) are: cryptomelane 0.77 +/- 0.10 J/m 2 (3.78), sodium birnessite 0.69 +/- 0.13 J/m2 (3.56), potassium birnessite 0.55 +/- 0.11 J/m2 (3.52), and calcium birnessite 0.41 +/- 0.11 J/m2 (3.50). Surface enthalpies of hydrous surfaces of the calcium manganese oxide nanosheets are: deltaCa 0.39MnO2.3nH2O 0.75 +/- 0.10 J/m2 (3.89) and deltaCa0.43MnO2.3nH2O 0.57 +/- 0.12 J/m2 (3.68). The surface enthalpy of the complex manganese oxides appears to decrease with decreasing manganese average oxidation state, that is, with greater mixed valence manganese (Mn 3+/4+). Low surface energy suggests loose binding of H2O on the internal and external surfaces and may be critical to catalysis in both natural and technological settings.

Electronic effects of Se and Pb dopants in TlBr

NASA Astrophysics Data System (ADS)

Smith, Holland M.; Phillips, David J.; Sharp, Ian D.; Beeman, Jeffrey W.; Chrzan, Daryl C.; Haegel, Nancy M.; Haller, Eugene E.; Ciampi, Guido; Kim, Hadong; Shah, Kanai S.

2012-05-01

Deep levels in Se- and Pb-doped bulk TlBr detectors were characterized with photo-induced conductivity transient spectroscopy (PICTS) and cathodoluminescence (CL). Se-doped TlBr revealed two traps with energies of 0.35 and 0.45 eV in PICTS spectra. The Pb-doped material revealed three levels with energies of 0.11, 0.45, and 0.75 eV. CL measurements in both materials correlate with optical transitions involving some of the identified levels. The ambipolar carrier lifetimes of Se-doped and Pb-doped TlBr were measured with microwave reflectivity transients and found to be significantly lower than the lifetime of undoped TlBr.

Room temperature chemical synthesis of lead selenide thin films with preferred orientation

NASA Astrophysics Data System (ADS)

Kale, R. B.; Sartale, S. D.; Ganesan, V.; Lokhande, C. D.; Lin, Yi-Feng; Lu, Shih-Yuan

2006-11-01

Room temperature chemical synthesis of PbSe thin films was carried out from aqueous ammoniacal solution using Pb(CH3COO)2 as Pb2+ and Na2SeSO3 as Se2- ion sources. The films were characterized by a various techniques including, X-ray diffraction (XRD), energy dispersive X-ray analysis (EDAX), scanning electron microscopy (SEM), transmission electron microscopy (TEM), high resolution transmission electron microscopy (HR-TEM), selected area electron diffraction (SAED), Fast Fourier transform (FFT) and UV-vis-NIR techniques. The study revealed that the PbSe thin film consists of preferentially oriented nanocubes with energy band gap of 0.5 eV.

The first principles study of elastic and thermodynamic properties of ZnSe

NASA Astrophysics Data System (ADS)

Khatta, Swati; Kaur, Veerpal; Tripathi, S. K.; Prakash, Satya

2018-05-01

The elastic and thermodynamic properties of ZnSe are investigated using thermo_pw package implemented in Quantum espresso code within the framework of density functional theory. The pseudopotential method within the local density approximation is used for the exchange-correlation potential. The physical parameters of ZnSe bulk modulus and shear modulus, anisotropy factor, Young's modulus, Poisson's ratio, Pugh's ratio and Frantsevich's ratio are calculated. The sound velocity and Debye temperature are obtained from elastic constant calculations. The Helmholtz free energy and internal energy of ZnSe are also calculated. The results are compared with available theoretical calculations and experimental data.

The effect of amorphous selenium detector thickness on dual-energy digital breast imaging

PubMed Central

Hu, Yue-Houng; Zhao, Wei

2014-01-01

Purpose: Contrast enhanced (CE) imaging techniques for both planar digital mammography (DM) and three-dimensional (3D) digital breast tomosynthesis (DBT) applications requires x-ray photon energies higher than the k-edge of iodine (33.2 keV). As a result, x-ray tube potentials much higher (>40 kVp) than those typical for screening mammography must be utilized. Amorphous selenium (a-Se) based direct conversion flat-panel imagers (FPI) have been widely used in DM and DBT imaging systems. The a-Se layer is typically 200 μm thick with quantum detective efficiency (QDE) >87% for x-ray energies below 26 keV. However, QDE decreases substantially above this energy. To improve the object detectability of either CE-DM or CE-DBT, it may be advantageous to increase the thickness (dSe) of the a-Se layer. Increasing the dSe will improve the detective quantum efficiency (DQE) at the higher energies used in CE imaging. However, because most DBT systems are designed with partially isocentric geometries, where the gantry moves about a stationary detector, the oblique entry of x-rays will introduce additional blur to the system. The present investigation quantifies the effect of a-Se thickness on imaging performance for both CE-DM and CE-DBT, discussing the effects of improving photon absorption and blurring from oblique entry of x-rays. Methods: In this paper, a cascaded linear system model (CLSM) was used to investigate the effect of dSe on the imaging performance (i.e., MTF, NPS, and DQE) of FPI in CE-DM and CE-DBT. The results from the model are used to calculate the ideal observer signal-to-noise ratio, d′, which is used as a figure-of-merit to determine the total effect of increasing dSe for CE-DM and CE-DBT. Results: The results of the CLSM show that increasing dSe causes a substantial increase in QDE at the high energies used in CE-DM. However, at the oblique projection angles used in DBT, the increased length of penetration through a-Se introduces additional image blur. The reduced MTF and DQE at high spatial frequencies lead to reduced two-dimensional d′. These losses in projection image resolution may subsequently result in a decrease in the 3D d′, but the degree of which is largely dependent on the DBT reconstruction algorithm. For a filtered backprojection (FBP) algorithm with spectral apodization and slice-thickness filters, which dominate the blur for reconstructed images at oblique angles, the effect of oblique entry of x-rays on 3D d′ is minimal. Thus, increasing dSe results in an improvement in d′ for both CE-DM and CE-DBT with typical FBP reconstruction parameters. Conclusions: Increased dSe improves CE breast imaging performance by increasing QDE of detectors at higher energies, e.g., 49 kVp. Although there is additional blur in the oblique angled projections of a DBT scan, the overall 3D d′ for DBT is not degraded because the dominant source blur at these angles results from the reconstruction filters of the employed FBP algorithm. PMID:25370637

The effect of amorphous selenium detector thickness on dual-energy digital breast imaging.

PubMed

Hu, Yue-Houng; Zhao, Wei

2014-11-01

Contrast enhanced (CE) imaging techniques for both planar digital mammography (DM) and three-dimensional (3D) digital breast tomosynthesis (DBT) applications requires x-ray photon energies higher than the k-edge of iodine (33.2 keV). As a result, x-ray tube potentials much higher (>40 kVp) than those typical for screening mammography must be utilized. Amorphous selenium (a-Se) based direct conversion flat-panel imagers (FPI) have been widely used in DM and DBT imaging systems. The a-Se layer is typically 200 μm thick with quantum detective efficiency (QDE) >87% for x-ray energies below 26 keV. However, QDE decreases substantially above this energy. To improve the object detectability of either CE-DM or CE-DBT, it may be advantageous to increase the thickness (dSe) of the a-Se layer. Increasing the dSe will improve the detective quantum efficiency (DQE) at the higher energies used in CE imaging. However, because most DBT systems are designed with partially isocentric geometries, where the gantry moves about a stationary detector, the oblique entry of x-rays will introduce additional blur to the system. The present investigation quantifies the effect of a-Se thickness on imaging performance for both CE-DM and CE-DBT, discussing the effects of improving photon absorption and blurring from oblique entry of x-rays. In this paper, a cascaded linear system model (CLSM) was used to investigate the effect of dSe on the imaging performance (i.e., MTF, NPS, and DQE) of FPI in CE-DM and CE-DBT. The results from the model are used to calculate the ideal observer signal-to-noise ratio, d', which is used as a figure-of-merit to determine the total effect of increasing dSe for CE-DM and CE-DBT. The results of the CLSM show that increasing dSe causes a substantial increase in QDE at the high energies used in CE-DM. However, at the oblique projection angles used in DBT, the increased length of penetration through a-Se introduces additional image blur. The reduced MTF and DQE at high spatial frequencies lead to reduced two-dimensional d'. These losses in projection image resolution may subsequently result in a decrease in the 3D d', but the degree of which is largely dependent on the DBT reconstruction algorithm. For a filtered backprojection (FBP) algorithm with spectral apodization and slice-thickness filters, which dominate the blur for reconstructed images at oblique angles, the effect of oblique entry of x-rays on 3D d' is minimal. Thus, increasing dSe results in an improvement in d' for both CE-DM and CE-DBT with typical FBP reconstruction parameters. Increased dSe improves CE breast imaging performance by increasing QDE of detectors at higher energies, e.g., 49 kVp. Although there is additional blur in the oblique angled projections of a DBT scan, the overall 3D d' for DBT is not degraded because the dominant source blur at these angles results from the reconstruction filters of the employed FBP algorithm.

Discovery of highly spin-polarized conducting surface states in the strong spin-orbit coupling semiconductor Sb2Se3

NASA Astrophysics Data System (ADS)

Das, Shekhar; Sirohi, Anshu; Kumar Gupta, Gaurav; Kamboj, Suman; Vasdev, Aastha; Gayen, Sirshendu; Guptasarma, Prasenjit; Das, Tanmoy; Sheet, Goutam

2018-06-01

Majority of the A2B3 -type chalcogenide systems with strong spin-orbit coupling (SOC), such as Bi2Se3,Bi2Te3 , and Sb2Te3 , etc., are topological insulators. One important exception is Sb2Se3 where a topological nontrivial phase was argued to be possible under ambient conditions, but such a phase could be detected to exist only under pressure. In this paper, we show that Sb2Se3 like Bi2Se3 displays a generation of highly spin-polarized current under mesoscopic superconducting point contacts as measured by point-contact Andreev reflection spectroscopy. In addition, we observe a large negative and anisotropic magnetoresistance of the mesoscopic metallic point contacts formed on Sb2Se3 . Our band-structure calculations confirm the trivial nature of Sb2Se3 crystals and reveal two trivial surface states one of which shows large spin splitting due to Rashba-type SOC. The observed high spin polarization and related phenomena in Sb2Se3 can be attributed to this spin splitting.

Selenium in irrigated agricultural areas of the western United States

USGS Publications Warehouse

Nolan, B.T.; Clark, M.L.

1997-01-01

A logistic regression model was developed to predict the likelihood that Se exceeds the USEPA chronic criterion for aquatic life (5 ??g/L) in irrigated agricultural areas of the western USA. Preliminary analysis of explanatory variables used in the model indicated that surface-water Se concentration increased with increasing dissolved solids (DS) concentration and with the presence of Upper Cretaceous, mainly marine sediment. The presence or absence of Cretaceous sediment was the major variable affecting Se concentration in surface-water samples from the National Irrigation Water Quality Program. Median Se concentration was 14 ??g/L in samples from areas underlain by Cretaceous sediments and < 1 ??g/L in samples from areas underlain by non-Cretaceous sediments. Wilcoxon rank sum tests indicated that elevated Se concentrations in samples from areas with Cretaceous sediments, irrigated areas, and from closed lakes and ponds were statistically significant. Spearman correlations indicated that Se was positively correlated with a binary geology variable (0.64) and DS (0.45). Logistic regression models indicated that the concentration of Se in surface water was almost certain to exceed the Environmental Protection Agency aquatic-life chronic criterion of 5 ??g/L when DS was greater than 3000 mg/L in areas with Cretaceous sediments. The 'best' logistic regression model correctly predicted Se exceedances and nonexceedances 84.4% of the time, and model sensitivity was 80.7%. A regional map of Cretaceous sediment showed the location of potential problem areas. The map and logistic regression model are tools that can be used to determine the potential for Se contamination of irrigated agricultural areas in the western USA.

Development of nitric oxide catalytic coatings by conjugating 3,3-disulfodipropionic acid and 3,3-diselenodipropionic acid for improving hemocompatibility.

PubMed

Yang, Ying; Li, Yalong; Li, Xiangyang; Qi, Pengkai; Tu, Qiufen; Yang, Zhilu; Huang, Nan

2015-12-02

Nitric oxide (NO), discovered as an endothelium-derived relaxing factor, has been found to have multiple intracellular effects in vascular diseases including vasorelaxation regulation, endothelial regeneration, inhibition of leukocyte chemotaxis, and platelet activation. In the work described here, the authors have developed a NO-catalytic bioactive coating for improving hemocompatibility. The authors first prepared a dopamine and hexamethylendiamine (PDAM/HD) amine-rich adherent copolymer coating to introduce amine groups onto 316L stainless steel, followed by covalently conjugating 3,3-disulfodipropionic acid (S-S) and 3,3-diselenodipropionic acid (Se-Se), which mimic glutathione peroxidase-like catalytic production of NO. S-S and Se-Se were immobilized on the PDAM/HD surface via carbodiimide coupling chemistry. X-ray photoelectron spectroscopy analysis revealed clear S2p and Se3d signals, confirming the immobilization of S-S and Se-Se on the PDAM/HD surface. The NO release behavior of different samples was investigated. In detail, two species of thionitrites (RSNO), S-nitrosoglutathione (GSNO, endogenous NO donors) and S-nitrosoacetylpenicillamine (SNAP) were chosen as NO donors to investigate the NO catalytic properties of S-S and Se-Se modified PDAM/HD surfaces. Not only Se-Se@PDAM/HD but also S-S@PDAM/HD coatings showed the ability to continuously catalyze RSNO to generate NO in the presence of proper thiol reducing agent. For the Se-Se@PDAM/HD coating, the NO release amount and rate were greater than S-S@PDAM/HD in both GSNO and SNAP conditions. The results showed that organosulfide species possesses NO catalytic ability as well as organoselenium species. The authors demonstrated that both S-S@PDAM/HD and Se-Se@PDAM/HD coatings exhibited outstanding inhibition effect on platelet adhesion, aggregation and activation via the cyclic guanylate monophosphate signal pathway. Thus these results suggested that NO catalytic coatings based on organoselenium and organosulfide species immobilization can help to improve hemocompatibility. NO-catalytic strategies possess huge potential applications in blood-contacting devices.

Enhanced photoelectrochemical aptasensing platform based on exciton energy transfer between CdSeTe alloyed quantum dots and SiO2@Au nanocomposites.

PubMed

Fan, Gao-Chao; Zhu, Hua; Shen, Qingming; Han, Li; Zhao, Ming; Zhang, Jian-Rong; Zhu, Jun-Jie

2015-04-25

High-efficient exciton energy transfer between CdSeTe alloyed quantum dots and SiO2@Au nanocomposites was applied to develop an enhanced photoelectrochemical aptasensing platform with ultrahigh sensitivity, good selectivity, reproducibility and stability.

A Review of SnSe: Growth and Thermoelectric Properties

NASA Astrophysics Data System (ADS)

Nguyen, Van Quang; Kim, Jungdae; Cho, Sunglae

2018-04-01

SnSe is a 2D semiconductor with an indirect energy gap of 0.86 - 1 eV; it is widely used in solar cell, optoelectronics, and electronic device applications. Recently, SnSe has been considered as a robust candidate for energy conversion applications due to its high thermoelectric performance ( ZT = 2.6 in p-type and 2.2 in n-type), which is assigned mainly to its anhamornic bonding leading to an ultralow thermal conductivity. In this review, we first discuss the crystalline and electronic structures of SnSe and the source of its p-type characteristic. Then, some typical single crystal and polycrystal growth techniques, as well as an epitaxial thin film growth technique, are outlined. The reported thermoelectric properties of SnSe grown by using each technique are also reviewed. Finally, we will describe some remaining issues concerning the use of SnSe for thermoelectric applications.

Adsorption of Selenium and Strontium on Goethite: EXAFS Study and Surface Complexation Modeling of the Ternary Systems.

PubMed

Nie, Zhe; Finck, Nicolas; Heberling, Frank; Pruessmann, Tim; Liu, Chunli; Lützenkirchen, Johannes

2017-04-04

Knowledge of the geochemical behavior of selenium and strontium is critical for the safe disposal of radioactive wastes. Goethite, as one of the most thermodynamically stable and commonly occurring natural iron oxy-hydroxides, promisingly retains these elements. This work comprehensively studies the adsorption of Se(IV) and Sr(II) on goethite. Starting from electrokinetic measurements, the binary and ternary adsorption systems are investigated and systematically compared via batch experiments, EXAFS analysis, and CD-MUSIC modeling. Se(IV) forms bidentate inner-sphere surface complexes, while Sr(II) is assumed to form outer-sphere complexes at low and intermediate pH and inner-sphere complexes at high pH. Instead of a direct interaction between Se(IV) and Sr(II), our results indicate an electrostatically driven mutual enhancement of adsorption. Adsorption of Sr(II) is promoted by an average factor of 5 within the typical groundwater pH range from 6 to 8 for the concentration range studied here. However, the interaction between Se(IV) and Sr(II) at the surface is two-sided, Se(IV) promotes Sr(II) outer-sphere adsorption, but competes for inner-sphere adsorption sites at high pH. The complexity of surfaces is highlighted by the inability of adsorption models to predict isoelectric points without additional constraints.

Fermi-level tuning of the Dirac surface state in (Bi1-x Sb x )2Se3 thin films

NASA Astrophysics Data System (ADS)

Satake, Yosuke; Shiogai, Junichi; Takane, Daichi; Yamada, Keiko; Fujiwara, Kohei; Souma, Seigo; Sato, Takafumi; Takahashi, Takashi; Tsukazaki, Atsushi

2018-02-01

We report on the electronic states and the transport properties of three-dimensional topological insulator (Bi1-x Sb x )2Se3 ternary alloy thin films grown on an isostructural Bi2Se3 buffer layer on InP substrates. By angle-resolved photoemission spectroscopy, we clearly detected Dirac surface states with a large bulk band gap of 0.2-0.3 eV in the (Bi1-x Sb x )2Se3 film with x  =  0.70. In addition, we observed by Hall effect measurements that the dominant charge carrier converts from electron (n-type) to hole (p-type) at around x  =  0.7, indicating that the Fermi level can be controlled across the Dirac point. Indeed, the carrier transport was shown to be governed by Dirac surface state in 0.63  ⩽  x  ⩽  0.75. These features suggest that Fermi-level tunable (Bi1-x Sb x )2Se3-based heterostructures provide a platform for extracting exotic topological phenomena.

Transport Properties of ZnSe- ITO Hetero Junction

NASA Astrophysics Data System (ADS)

Ichibakase, Tsuyoshi

In this report, ITO(Indium Tin Oxide) was used on the glass substrates as the transparent electrode, and ZnSe layer was prepared by the vacuum deposition on this ITO. Then, the electrical characteristics of this sample were investigated by mans of the electric current transport analysis. The sample that ZnSe was prepared as 3.4 μm in case of ITO-ZnSe sample, has high density level at the junction surface. The ITO-ZnSe junction has two type of diffusion current. However, the ITO-ZnSe sample that ZnSe layer was prepared as 0.1 μm can be assumed as the ohmic contact, and ITO-ZnSe(0.1μm) -CdTe sample shows the avalanche breakdown, and it is considered that the avalanche breakdown occurs in CdTe layer. It is difficult to occur the avalanche breakdown, if ZnSe-CdTe junction has high-density level and CdTe layer has high-density defect. Hence, the ZnSe-CdTe sample that CdTe layer was prepared on ITO-ZnSe(0.1μm) substrate has not high-density level at the junction surface, and the CdTe layer with little lattice imperfection can be prepared. It found that ITO-ZnSe(0.1μm) substrate is available for the II-VI compounds semiconductor device through above analysis result.

Hydrological and geochemical investigations of selenium behavior at Kesterson Reservoir. Progress report, October 1, 1994--September 30, 1996

DOE Office of Scientific and Technical Information (OSTI.GOV)

Zawislanski, P.; Tokunaga, T.; Benson, S.M.

1997-10-01

This report describes research relevant to selenium (Se) speciation, fractionation, physical redistribution, reduction and oxidation, and spatial distribution as related to Kesterson Reservoir. The work was carried out by scientists and engineers from the Earth Sciences Division of the Lawrence Berkeley Laboratory over a two year period from October 1994 to September 1996. Much of the focus of this research was on long-term, Reservoir-wide changes in Se concentrations and distribution; estimation and prediction of the physical extent ephemeral pools; and the quantification and prediction of Se levels in ephemeral pools waters and underlying sediments. Chapter 2 contains descriptions of fieldmore » monitoring of soil processes. In Section 2.1, elevated Se concentrations observed in groundwater in the northern part of Pond 9 are investigated. The past removal of the original surface soil in the northern Pond 9 area resulted in the enhancement of Se transport into the shallow groundwater in this area. Removal of the most organic-rich surface soil horizon left the remaining profile with a lower capacity to generate and sustain reducing conditions needed to immobilize Se. Furthermore, removal of the lower permeability surface soil left the remaining profile more hydraulically conductive since sands are encountered at fairly shallow depths. These conditions result in Se remaining oxidized down to the 2.00 m depth throughout the year.« less

Effect of Indium nano-sandwiching on the structural and optical performance of ZnSe films

NASA Astrophysics Data System (ADS)

Al Garni, S. E.; Qasrawi, A. F.

In the current study, we attempted to explore the effects of the Indium nanosandwiching on the mechanical and optical properties of the physically evaporated ZnSe thin films by means of X-ray diffractions and ultraviolet spectrophotometry techniques. While the thickness of each layer of ZnSe was fixed at 1.0 μm, the thickness of the nanosandwiched Indium thin films was varied in the range of 25-100 nm. It was observed that the as grown ZnSe films exhibits cubic and hexagonal nature of crystallization as those of the ZnSe powders before the film deposition. The cubic phases weighs ∼70% of the structure. The analysis of this phases revealed that there is a systematic variation process presented by the decreasing of; the lattice constant, compressing strain, stress, stacking faults and dislocation intensity and increasing grain size resulted from increasing the Indium layer thickness in the range of 50-100 nm. In addition, the nanosandwiching of Indium between two layers of ZnSe is observed to enhance the absorbability of the ZnSe. Particularly, at incident photon energy of 2.38 eV the absorbability of the ZnSe films which are sandwiched with 100 nm Indium is increased by 13.8 times. Moreover, increasing the thickness of the Indium layer shrinks the optical energy band gap. These systematic variations in mechanical and optical properties are assigned to the better recrystallization process that is associated with Indium insertion which in turn allows total internal energy redistribution in the ZnSe films through the enlargement of grains.

Thermal kinetics and short range order parameters of Se80X20 (X = Te, Sb) binary glasses

NASA Astrophysics Data System (ADS)

Moharram, A. H.; Abu El-Oyoun, M.; Abdel-Baset, A. M.

2014-06-01

Bulk Se80Te20 and Se80Sb20 glasses were prepared using the melt-quench technique. Differential scanning calorimetry (DSC) curves measured at different heating rates (5 K/min≤ α≤50 K/min) and X-ray diffraction (XRD) are used to characterize the as-quenched specimens. Based on the obtained results, the activation energy of glass transition and the activation energy of crystallization ( E g, E c) of the Se80Te20 glass are (137.5, 105.1 kJ/mol) higher than the corresponding values of the Se80Sb20 glass (106.8, 71.2 kJ/mol). An integer n value ( n=2) of the Se80Te20 glass indicates that only one crystallization mechanism is occurring while a non-integer exponent ( n=1.79) in the Se80Sb20 glass means that two mechanisms are working simultaneously during the amorphous-crystalline transformations. The total structure factor, S( K), indicates the presence of the short-range order (SRO) and the absence of the medium-range order (MRO) inside the as-quenched alloys. In an opposite way to the activation energies, the values of the first peak position and the total coordination number ( r 1, η 1), obtained from a Gaussian fit of the radial distribution function, of the Se80Te20 glass are (2.42 nm, 1.99 atom) lower than the corresponding values (2.55 nm, 2.36 atom) of the Se80Sb20 specimens.

Improving polymer/nanocrystal hybrid solar cell performance via tuning ligand orientation at CdSe quantum dot surface.

PubMed

Fu, Weifei; Wang, Ling; Zhang, Yanfang; Ma, Ruisong; Zuo, Lijian; Mai, Jiangquan; Lau, Tsz-Ki; Du, Shixuan; Lu, Xinhui; Shi, Minmin; Li, Hanying; Chen, Hongzheng

2014-11-12

Achieving superior solar cell performance based on the colloidal nanocrystals remains challenging due to their complex surface composition. Much attention has been devoted to the development of effective surface modification strategies to enhance electronic coupling between the nanocrystals to promote charge carrier transport. Herein, we aim to attach benzenedithiol ligands onto the surface of CdSe nanocrystals in the "face-on" geometry to minimize the nanocrystal-nanocrystal or polymer-nanocrystal distance. Furthermore, the "electroactive" π-orbitals of the benzenedithiol are expected to further enhance the electronic coupling, which facilitates charge carrier dissociation and transport. The electron mobility of CdSe QD films was improved 20 times by tuning the ligand orientation, and high performance poly[2,6-(4,4-bis(2-ethylhexyl)-4H-cyclopenta[2,1-b;3,4-b']-dithiophene)-alt-4,7-(2,1,3-benzothiadiazole)] (PCPDTBT):CdSe nanocrystal hybrid solar cells were also achieved, showing a highest power conversion efficiency of 4.18%. This research could open up a new pathway to improve further the performance of colloidal nanocrystal based solar cells.

Optical Metrology for CIGS Solar Cell Manufacturing and its Cost Implications

NASA Astrophysics Data System (ADS)

Sunkoju, Sravan Kumar

Solar energy is a promising source of renewable energy which can meet the demand for clean energy in near future with advances in research in the field of photovoltaics and cost reduction by commercialization. Availability of a non-contact, in-line, real time robust process control strategies can greatly aid in reducing the gap between cell and module efficiencies, thereby leading to cost-effective large-scale manufacturing of high efficiency CIGS solar cells. In order to achieve proper process monitoring and control for the deposition of the functional layers of CuIn1-xGaxSe 2 (CIGS) based thin film solar cell, optical techniques such as spectroscopic reflectometry and polarimetry are advantageous because they can be set up in an unobtrusive manner in the manufacturing line, and collect data in-line and in-situ. The use of these techniques requires accurate optical models that correctly represent the properties of the layers being deposited. In this study, Spectroscopic ellipsometry (SE) has been applied for the characterization of each individual stage of CIGS layers deposited using the 3-stage co-evaporation process along with the other functional layers. Dielectric functions have been determined for the energy range from 0.7 eV to 5.1 eV. Critical-point line-shape analysis was used in this study to determine the critical point energies of the CIGS based layers. To control the compositional and thickness uniformity of all the functional layers during the fabrication of CIGS solar cells over large areas, multilayer photovoltaics (PV) stack optical models were developed with the help of extracted dielectric functions. In this study, mapping capability of RC2 spectroscopic ellipsometer was used to map all the functional layer thicknesses of a CIGS solar cell in order to probe the spatial non-uniformities that can affect the performance of a cell. The optical functions for each of the stages of CIGS 3-stage deposition process along with buffer layer and transparent conducting oxide (TCO) bi-layer, thus derived were used in a fiber optic-based spectroscopic reflectometry optical monitoring system installed in the pilot line at the PVMC's Halfmoon facility. Results obtained from this study show that the use of regular fiber optics, instead of polarization-maintaining fiber optics, is sufficient for the purpose of process monitoring. Also, the technique does not need to be used "in-situ", but the measurements can be taken in-line, and are applicable to a variety of deposition techniques used for different functional layers deposited on rigid or flexible substrates. In addition, effect of Cu concentration on the CIGS optical properties has been studied. Mixed CIGS/Cu2-xSe phase was observed at the surface at the end of the second stage of 3-stage deposition process, under Cu-rich conditions. A significant change in optical behavior of CIGS due to Cu2-xSe at the surface was observed under Cu-rich conditions, which can be used as end-point detection method to move from 2nd stage to 3rd stage in the deposition process. Developed optical functions were applied to in-line reflectance measurements not only to identify the Cu2-xSe phase at the surface but also to measure the thickness of the mixed CIGS/Cu2-xSe layer. This spectroscopic reflectometry based in-line process control technique can be used for end-point detection as well as to control thickness during the preparation of large area CIGS films. These results can assist in the development of optical process-control tools for the manufacturing of high quality CIGS based photovoltaic cells, increasing the uptime and yield of the production line. Finally, to understand the cost implications, low cost potential of two different deposition technologies has been studied on both rigid and flexible substrates with the help of cost analysis. Cost advantages of employing a contactless optics based process control technique have been investigated in order to achieve a low cost of < 0.5 $/W for CIGS module production. Based on cost analysis, one of the best strategies for achieving the low cost targets would be increasing manufacturing throughput, using roll-to-roll thin-film module manufacturing, with co-evaporation and chemical bath deposition processes for absorber and buffer layer respectively, while applying a low-cost process control technique such as spectroscopic reflectometry to improve module efficiencies and maintain high yield.

Topological phase diagram and saddle point singularity in a tunable topological crystalline insulator

DOE PAGES

Neupane, Madhab; Xu, Su-Yang; Sankar, R.; ...

2015-08-20

Here we report the evolution of the surface electronic structure and surface material properties of a topological crystalline insulator (TCI), Pb 1more » $${-}$$xSnxSe, as a function of various material parameters including composition x, temperature T , and crystal structure. Our spectroscopic data demonstrate the electronic ground-state condition for the saddle point singularity, the tunability of surface chemical potential, and the surface states’ response to circularly polarized light. Our results show that each material parameter can tune the system between the trivial and topological phase in a distinct way, unlike that seen in Bi 2Se 3 and related compounds, leading to a rich topological phase diagram. Our systematic studies of the TCI Pb 1$${-}$$xSnxSe are a valuable materials guide to realize new topological phenomena.« less

A comparison of fate and toxicity of selenite, biogenically, and chemically synthesized selenium nanoparticles to zebrafish (Danio rerio) embryogenesis.

PubMed

Mal, Joyabrata; Veneman, Wouter J; Nancharaiah, Y V; van Hullebusch, Eric D; Peijnenburg, Willie J G M; Vijver, Martina G; Lens, Piet N L

2017-02-01

Microbial reduction of selenium (Se) oxyanions to elemental Se is a promising technology for bioremediation and treatment of Se wastewaters. But a fraction of biogenic nano-Selenium (nano-Se b ) formed in bioreactors remains suspended in the treated waters, thus entering the aquatic environment. The present study investigated the toxicity of nano-Se b formed by anaerobic granular sludge biofilms on zebrafish embryos in comparison with selenite and chemogenic nano-Se (nano-Se c ). The nano-Se b formed by granular sludge biofilms showed a LC 50 value of 1.77 mg/L, which was 3.2-fold less toxic to zebrafish embryos than selenite (LC 50  =   0.55 mg/L) and 10-fold less toxic than bovine serum albumin stabilized nano-Se c (LC 50  =   0.16 mg/L). Smaller (nano-Se cs ; particle diameter range: 25-80 nm) and larger (nano-Se cl ; particle diameter range: 50-250 nm) sized chemically synthesized nano-Se c particles showed comparable toxicity on zebrafish embryos. The lower toxicity of nano-Se b in comparison with nano-Se c was analyzed in terms of the stabilizing organic layer. The results confirmed that the organic layer extracted from the nano-Se b consisted of components of the extracellular polymeric substances (EPS) matrix, which govern the physiochemical stability and surface properties like ζ-potential of nano-Se b . Based on the data, it is contented that the presence of humic acid like substances of EPS on the surface of nano-Se b plays a major role in lowering the bioavailability (uptake) and toxicity of nano-Se b by decreasing the interactions between nanoparticles and embryos.

Evidence of superconductivity-induced phonon spectra renormalization in alkali-doped iron selenides

DOE Office of Scientific and Technical Information (OSTI.GOV)

Opačić, M.; Lazarević, N.; Šćepanović, M.

2015-11-16

Polarized Raman scattering spectra of superconducting K xFe 2-ySe 2 and nonsuperconducting K 0.8Fe 1.8Co 0.2Se 2 single crystals were measured in a temperature range from 10 K up to 300 K. Two Raman active modes from the I4/mmm phase and seven from the I4/m phase are observed in frequency range from 150 to 325 cm -1 in both compounds, suggesting that K 0.8Fe 1.8Co 0.2Se 2 single crystal also has two-phase nature. Temperature dependence of Raman mode energy is analyzed in terms of lattice thermal expansion and phonon-phonon interaction. Temperature dependence of Raman mode linewidth is considered as temperature-inducedmore » anharmonic effects. It is shown that change of Raman mode energy with temperature is dominantly driven by thermal expansion of the crystal lattice. Abrupt change of the A 1g mode energy near T C was observed in K xFe 2-ySe 2 , whereas it is absent in K 0.8Fe 1.8Co 0.2Se 2. Phonon energy hardening at low temperatures in the superconducting sample is a consequence of superconductivity-induced redistribution of the electronic states below critical temperature.« less

Selenium and selenium-sulfur cathode materials for high-energy rechargeable magnesium batteries

NASA Astrophysics Data System (ADS)

Zhao-Karger, Zhirong; Lin, Xiu-Mei; Bonatto Minella, Christian; Wang, Di; Diemant, Thomas; Behm, R. Jürgen; Fichtner, Maximilian

2016-08-01

Magnesium (Mg) is an attractive metallic anode material for next-generation batteries owing to its inherent dendrite-free electrodeposition, high capacity and low cost. Here we report a new class of Mg batteries based on both elemental selenium (Se) and selenium-sulfur solid solution (SeS2) cathode materials. Elemental Se confined into a mesoporous carbon was used as a cathode material. Coupling the Se cathode with a metallic Mg anode in a non-nucleophilic electrolyte, the Se cathode delivered a high initial volumetric discharge capacity of 1689 mA h cm-3 and a reversible capacity of 480 mA h cm-3 was retained after 50 cycles at a high current density of 2 C. The mechanistic insights into the electrochemical conversion in Mg-Se batteries were investigated by microscopic and spectroscopic methods. The structural transformation of cyclic Se8 into chainlike Sen upon battery cycling was revealed by ex-situ Raman spectroscopy. In addition, the promising battery performance with a SeS2 cathode envisages the perspective of a series of SeSn cathode materials combining the benefits of both selenium and sulfur for high energy Mg batteries.

Design of a Hole Trapping Ligand

DOE PAGES

La Croix, Andrew D.; O’Hara, Andrew; Reid, Kemar R.; ...

2017-01-18

A new ligand that covalently attaches to the surface of colloidal CdSe/ CdS nanorods and can simultaneously chelate a molecular metal center is described. The dithiocarbamate$-$bipyridine ligand system facilitates hole transfer through energetic overlap at the inorganic$-$organic interface and conjugation through the organic ligand to a chelated metal center. Density functional theory calculations show that the coordination of the free ligand to a CdS surface causes the formation of two hybridized molecular states that lie in the band gap of CdS. The further chelation of Fe(II) to the bipyridine moiety causes the presence of seven midgap states. Hole transfer frommore » the CdS valence band to the midgap states is dipole allowed and occurs at a faster rate than what is experimentally known for the CdSe/CdS band-edge radiative recombination. In the case of the ligand bound with iron, a two-step process emerges that places the hole on the iron, again at rates much faster than band gap recombination. The system was experimentally assembled and characterized via UV$-$vis absorbance spectroscopy, fluorescence spectroscopy, time-resolved photoluminescence spectroscopy, and energy dispersive X-ray spectroscopy. Lastly, theoretically predicted red shifts in absorbance were observed experimentally, as well as the expected quench in photoluminescence and lifetimes in time-resolved photoluminescence« less

Design of a Hole Trapping Ligand

DOE Office of Scientific and Technical Information (OSTI.GOV)

La Croix, Andrew D.; O’Hara, Andrew; Reid, Kemar R.

A new ligand that covalently attaches to the surface of colloidal CdSe/ CdS nanorods and can simultaneously chelate a molecular metal center is described. The dithiocarbamate$-$bipyridine ligand system facilitates hole transfer through energetic overlap at the inorganic$-$organic interface and conjugation through the organic ligand to a chelated metal center. Density functional theory calculations show that the coordination of the free ligand to a CdS surface causes the formation of two hybridized molecular states that lie in the band gap of CdS. The further chelation of Fe(II) to the bipyridine moiety causes the presence of seven midgap states. Hole transfer frommore » the CdS valence band to the midgap states is dipole allowed and occurs at a faster rate than what is experimentally known for the CdSe/CdS band-edge radiative recombination. In the case of the ligand bound with iron, a two-step process emerges that places the hole on the iron, again at rates much faster than band gap recombination. The system was experimentally assembled and characterized via UV$-$vis absorbance spectroscopy, fluorescence spectroscopy, time-resolved photoluminescence spectroscopy, and energy dispersive X-ray spectroscopy. Lastly, theoretically predicted red shifts in absorbance were observed experimentally, as well as the expected quench in photoluminescence and lifetimes in time-resolved photoluminescence« less

Topological phases of topological-insulator thin films

NASA Astrophysics Data System (ADS)

Asmar, Mahmoud M.; Sheehy, Daniel E.; Vekhter, Ilya

2018-02-01

We study the properties of a thin film of topological insulator material. We treat the coupling between helical states at opposite surfaces of the film in the properly-adapted tunneling approximation, and show that the tunneling matrix element oscillates as a function of both the film thickness and the momentum in the plane of the film for Bi2Se3 and Bi2Te3 . As a result, while the magnitude of the matrix element at the center of the surface Brillouin zone gives the gap in the energy spectrum, the sign of the matrix element uniquely determines the topological properties of the film, as demonstrated by explicitly computing the pseudospin textures and the Chern number. We find a sequence of transitions between topological and nontopological phases, separated by semimetallic states, as the film thickness varies. In the topological phase, the edge states of the film always exist but only carry a spin current if the edge potentials break particle-hole symmetry. The edge states decay very slowly away from the boundary in Bi2Se3 , making Bi2Te3 , where this scale is shorter, a more promising candidate for the observation of these states. Our results hold for free-standing films as well as heterostructures with large-gap insulators.

AN UPDATED {sup 6}Li(p, {alpha}){sup 3}He REACTION RATE AT ASTROPHYSICAL ENERGIES WITH THE TROJAN HORSE METHOD

DOE Office of Scientific and Technical Information (OSTI.GOV)

Lamia, L.; Spitaleri, C.; Sergi, M. L.

2013-05-01

The lithium problem influencing primordial and stellar nucleosynthesis is one of the most interesting unsolved issues in astrophysics. {sup 6}Li is the most fragile of lithium's stable isotopes and is largely destroyed in most stars during the pre-main-sequence (PMS) phase. For these stars, the convective envelope easily reaches, at least at its bottom, the relatively low {sup 6}Li ignition temperature. Thus, gaining an understanding of {sup 6}Li depletion also gives hints about the extent of convective regions. For this reason, charged-particle-induced reactions in lithium have been the subject of several studies. Low-energy extrapolations of these studies provide information about bothmore » the zero-energy astrophysical S(E) factor and the electron screening potential, U{sub e} . Thanks to recent direct measurements, new estimates of the {sup 6}Li(p, {alpha}){sup 3}He bare-nucleus S(E) factor and the corresponding U{sub e} value have been obtained by applying the Trojan Horse method to the {sup 2}H({sup 6}Li, {alpha} {sup 3}He)n reaction in quasi-free kinematics. The calculated reaction rate covers the temperature window 0.01 to 2T{sub 9} and its impact on the surface lithium depletion in PMS models with different masses and metallicities has been evaluated in detail by adopting an updated version of the FRANEC evolutionary code.« less

Toward Determining ATPase Mechanism in ABC Transporters: Development of the Reaction Path–Force Matching QM/MM Method

PubMed Central

Zhou, Y.; Ojeda-May, P.; Nagaraju, M.; Pu, J.

2016-01-01

Adenosine triphosphate (ATP)-binding cassette (ABC) transporters are ubiquitous ATP-dependent membrane proteins involved in translocations of a wide variety of substrates across cellular membranes. To understand the chemomechanical coupling mechanism as well as functional asymmetry in these systems, a quantitative description of how ABC transporters hydrolyze ATP is needed. Complementary to experimental approaches, computer simulations based on combined quantum mechanical and molecular mechanical (QM/MM) potentials have provided new insights into the catalytic mechanism in ABC transporters. Quantitatively reliable determination of the free energy requirement for enzymatic ATP hydrolysis, however, requires substantial statistical sampling on QM/MM potential. A case study shows that brute force sampling of ab initio QM/MM (AI/MM) potential energy surfaces is computationally impractical for enzyme simulations of ABC transporters. On the other hand, existing semiempirical QM/MM (SE/MM) methods, although affordable for free energy sampling, are unreliable for studying ATP hydrolysis. To close this gap, a multiscale QM/MM approach named reaction path–force matching (RP–FM) has been developed. In RP–FM, specific reaction parameters for a selected SE method are optimized against AI reference data along reaction paths by employing the force matching technique. The feasibility of the method is demonstrated for a proton transfer reaction in the gas phase and in solution. The RP–FM method may offer a general tool for simulating complex enzyme systems such as ABC transporters. PMID:27498639

A density functional study of silicon fullerene endohedral X@Si20F20 and exohedral X-Si20F20 (X=O2-, S2-, Se2-) complexes

NASA Astrophysics Data System (ADS)

Behzadi, Hadi; Esrafili, Mehdi D.; Manzetti, Sergio; Roonasi, Payman

2014-02-01

This study reports the structure and electronic properties of three stable endohedral X@Si20F20 and exohedral X-Si20F20 (X=O2-, S2-, Se2-) complexes. The study revealed that the endohedral complexes with S2- and Se2- result as energy minimum structures, with the guest anion located in the cage center. In the case of endohedral O2--complexes, the pattern is quite different whereas the O2- complexes dramatically deviated from the architecture of S2- and Se2-, by having O2- located toward one of silicon atoms in the cage. With respect to the exohedral form, the energy minimized structure is obtained by positioning the anion between two silicon atoms and forming two Si-X bonds. For both cases, the strength of the interactions is calculated to increase accordingly to the pattern: Se2-@Si20F20 (Se2--Si20F20)

Optical damage observed in the LHMEL II output coupler

NASA Astrophysics Data System (ADS)

Eric, John J.; Bagford, John O.; Devlin, Christie L. H.; Hull, Robert J.; Seibert, Daniel B.

2008-01-01

During the annual NIST calibration testing done at the LHMEL facility in FY06 on its high energy Carbon-Dioxide lasers, the LHMEL II device suffered severe damage to the internal surface of its ZnSe output coupler optics. The damage occurred during a high power, short duration run and it was believed to have been the result of a significant amount of surface contaminants interacting with the LHMEL cavity beam. Initial theories as to the source of the contamination led to the inspection of the vacuum grease that seals the piping that supplies the source gases to the laser cavity. Other contamination sources were considered, and analysis was conducted in an effort to identify the material found at the damage sites on the optic, but the tests were mainly inconclusive. Some procedure changes were initiated to identify possible contamination before high energy laser operation in an attempt to mitigate and possibly prevent the continued occurrence of damage to the output coupler window. This paper is to illustrate the type and extent of the damage encountered, highlight some of the theories as to the contamination source, and serve as a notice as to the severity and consequences of damage that is possible even due to small amounts of foreign material in a high energy laser environment.

Bandgap Engineering of Cu(In 1-xGax)Se 2 Absorber Layers Fabricated using CuInSe 2 and CuGaSe 2 Targets for One-Step Sputtering Process

DOE PAGES

Park, Jae -Cheol; Lee, Jeon -Ryang; Al-Jassim, Mowafak; ...

2016-10-17

Here we have demonstrated that the bandgap of Cu(In 1-xGa x)Se 2(CIGS) absorber layers was readily controlled by using a one-step sputtering process. CIGS thin-film sample libraries with different Ga/(In + Ga) ratios were synthesized on soda-lime glass at 550 °C using a combinatorial magnetron sputtering system employing CuInSe 2(CIS) and CuGaSe 2(CGS) targets. Energy-dispersive X-ray fluorescence spectrometry (EDS-XRF) confirmed that the CIGS films had different Ga/(In + Ga) ratios, which were varied by the sample configuration on the substrate and ranged from 0.2 to 0.9. X-ray diffraction and Raman spectroscopy revealed that the CIGS films had a pure chalcopyritemore » phase without any secondary phase such as Cu-Se or ordered vacancy compound (OVC), respectively. Furthermore, we found that the optical bandgap energies of the CIGS films determined by transmittance measurements ranged from 1.07 eV to 1.53 eV as the Ga/(In + Ga) ratio increased from 0.2 to 0.9, demonstrating that the one-step sputtering process using CIS and CGS targets is another simple route to control the bandgap energy of the CIGS absorber layer.« less

The ZnSe(110) puzzle - Comparison with GaAs(110)

NASA Technical Reports Server (NTRS)

Duke, C. B.; Paton, A.; Kahn, A.; Tu, D.-W.

1984-01-01

The surface structure of monocrystalline ZnSe(110) and of 4-5-nm-thick ZnSe(110) layers epitaxially grown on GaAs(110) is investigated by means of elastic LEED and AES; the results are analyzed using the computer programs and R-factor methods of Duke et al. (1981 and 1983), presented in graphs and tables, and compared to those for GaAs(110). Significant differences are attributed to bond-length-conserving outward rotation of Se and inward rotation of Zn in the top layer, with an angle of 4 deg between the actual plane of the cation-anion chain and the truncated bulk surface. The R intensities measured for ZnSe(110) and GaAs(110) are given as Rx = 0.22 and RI = 0.21 and Rx = 0.24 and RI = 0.16, respectively.

First-principles study on alkali-metal effect of Li, Na, and K in CuInSe2 and CuGaSe2

NASA Astrophysics Data System (ADS)

Maeda, Tsuyoshi; Kawabata, Atsuhito; Wada, Takahiro

2015-08-01

The substitution energies and migration energies of the alkali metal atoms of Li, Na, and K in CuInSe2 (CIS) and CuGaSe2 (CGS) were investigated by first-principles calculations. The substitution energies of Li, Na, and K atoms in CIS and CGS were calculated for two different cationic atom positions of Cu and In/Ga in the chalcopyrite unit cell. In CIS and CGS, the substitution energies of NaCu are much lower than those of NaIn and NaGa. The substitution energies of the LiCu atoms in CIS and CGS are lower than those of NaCu, while the substitution energies of KCu atoms in CIS and CGS are much higher than those of NaCu. Therefore, it is difficult to form KCu in CIS and CGS. The migration energies of Li, Na, and K atoms in CIS and CGS are obtained by a combination of the linear and quadratic synchronous transit (LST/QST) methods and the nudged elastic band (NEB) method. The theoretical migration energies of a Na atom at the Cu site to the nearest Cu vacancy (NaCu → VCu) in CIS and CGS are much lower than those of (CuCu → VCu) in CIS and CGS. The mechanism underlying the alkali metal effect of Li, Na, and K in the CIGS film during the post-deposition treatment of LiF, NaF, and KF is discussed on the basis of the calculated substitution and migration energies.

NMR evidence for static local nematicity and its cooperative interplay with low-energy magnetic fluctuations in FeSe under pressure

DOE PAGES

Wiecki, P.; Nandi, M.; Bohmer, Anna; ...

2017-11-13

Here, we present 77Se -NMR measurements on single-crystalline FeSe under pressures up to 2 GPa. Based on the observation of the splitting and broadening of the NMR spectrum due to structural twin domains, we discovered that static, local nematic ordering exists well above the bulk nematic ordering temperature, T s. The static, local nematic order and the low-energy stripe-type antiferromagnetic spin fluctuations, as revealed by NMR spin-lattice relaxation rate measurements, are both insensitive to pressure application. Our NMR results provide clear evidence for the microscopic cooperation between magnetism and local nematicity in FeSe.

NMR evidence for static local nematicity and its cooperative interplay with low-energy magnetic fluctuations in FeSe under pressure

DOE Office of Scientific and Technical Information (OSTI.GOV)

Wiecki, P.; Nandi, M.; Bohmer, Anna

Here, we present 77Se -NMR measurements on single-crystalline FeSe under pressures up to 2 GPa. Based on the observation of the splitting and broadening of the NMR spectrum due to structural twin domains, we discovered that static, local nematic ordering exists well above the bulk nematic ordering temperature, T s. The static, local nematic order and the low-energy stripe-type antiferromagnetic spin fluctuations, as revealed by NMR spin-lattice relaxation rate measurements, are both insensitive to pressure application. Our NMR results provide clear evidence for the microscopic cooperation between magnetism and local nematicity in FeSe.

Ultrafast carrier dynamics in band edge and broad deep defect emission ZnSe nanowires

NASA Astrophysics Data System (ADS)

Othonos, Andreas; Lioudakis, Emmanouil; Philipose, U.; Ruda, Harry E.

2007-12-01

Ultrafast carrier dynamics of ZnSe nanowires grown under different growth conditions have been studied. Transient absorption measurements reveal the dependence of the competing effects of state filling and photoinduced absorption on the probed energy states. The relaxation of the photogenerated carriers occupying defect states in the stoichiometric and Se-rich samples are single exponentials with time constants of 3-4ps. State filling is the main contribution for probe energies below 1.85eV in the Zn-rich grown sample. This ultrafast carrier dynamics study provides an important insight into the role that intrinsic point defects play in the observed photoluminescence from ZnSe nanowires.

NIR-Emitting Alloyed CdTeSe QDs and Organic Dye Assemblies: A Nontoxic, Stable, and Efficient FRET System.

PubMed

Ramírez-Herrera, Doris E; Rodríguez-Velázquez, Eustolia; Alatorre-Meda, Manuel; Paraguay-Delgado, Francisco; Tirado-Guízar, Antonio; Taboada, Pablo; Pina-Luis, Georgina

2018-04-11

In the present work, we synthesize Near Infrared (NIR)-emitting alloyed mercaptopropionic acid (MPA)-capped CdTeSe quantum dots (QDs) in a single-step one-hour process, without the use of an inert atmosphere or any pyrophoric ligands. The quantum dots are water soluble, non-toxic, and highly photostable and have high quantum yields (QYs) up to 84%. The alloyed MPA-capped CdTeSe QDs exhibit a red-shifted emission, whose color can be tuned between visible and NIR regions (608-750 nm) by controlling the Te:Se molar ratio in the precursor mixtures and/or changing the time reaction. The MPA-capped QDs were characterized by UV-visible absorption spectroscopy, fluorescence spectroscopy, transmission electron microscopy (TEM), energy dispersive X-ray spectroscopy (EDS), and zeta potential measurements. Photostability studies were performed by irradiating the QDs with a high-power xenon lamp. The ternary MPA-CdTeSe QDs showed greater photostability than the corresponding binary MPA-CdTe QDs. We report the Förster resonance energy transfer (FRET) from the MPA-capped CdTeSe QDs as energy donors and Cyanine5 NHS-ester (Cy5) dye as an energy acceptor with efficiency ( E ) up to 95%. The distance between the QDs and dye ( r ), the Förster distance ( R ₀), and the binding constant ( K ) are reported. Additionally, cytocompatibility and cell internalization experiments conducted on human cancer cells (HeLa) cells revealed that alloyed MPA-capped CdTeSe QDs are more cytocompatible than MPA-capped CdTe QDs and are capable of ordering homogeneously all over the cytoplasm, which allows their use as potential safe, green donors for biological FRET applications.

NIR-Emitting Alloyed CdTeSe QDs and Organic Dye Assemblies: A Nontoxic, Stable, and Efficient FRET System

PubMed Central

Ramírez-Herrera, Doris E.; Rodríguez-Velázquez, Eustolia; Alatorre-Meda, Manuel; Paraguay-Delgado, Francisco; Tirado-Guízar, Antonio; Taboada, Pablo; Pina-Luis, Georgina

2018-01-01

In the present work, we synthesize Near Infrared (NIR)-emitting alloyed mercaptopropionic acid (MPA)-capped CdTeSe quantum dots (QDs) in a single-step one-hour process, without the use of an inert atmosphere or any pyrophoric ligands. The quantum dots are water soluble, non-toxic, and highly photostable and have high quantum yields (QYs) up to 84%. The alloyed MPA-capped CdTeSe QDs exhibit a red-shifted emission, whose color can be tuned between visible and NIR regions (608–750 nm) by controlling the Te:Se molar ratio in the precursor mixtures and/or changing the time reaction. The MPA-capped QDs were characterized by UV-visible absorption spectroscopy, fluorescence spectroscopy, transmission electron microscopy (TEM), energy dispersive X-ray spectroscopy (EDS), and zeta potential measurements. Photostability studies were performed by irradiating the QDs with a high-power xenon lamp. The ternary MPA-CdTeSe QDs showed greater photostability than the corresponding binary MPA-CdTe QDs. We report the Förster resonance energy transfer (FRET) from the MPA-capped CdTeSe QDs as energy donors and Cyanine5 NHS-ester (Cy5) dye as an energy acceptor with efficiency (E) up to 95%. The distance between the QDs and dye (r), the Förster distance (R0), and the binding constant (K) are reported. Additionally, cytocompatibility and cell internalization experiments conducted on human cancer cells (HeLa) cells revealed that alloyed MPA-capped CdTeSe QDs are more cytocompatible than MPA-capped CdTe QDs and are capable of ordering homogeneously all over the cytoplasm, which allows their use as potential safe, green donors for biological FRET applications. PMID:29641435

Hot electron dynamics at semiconductor surfaces: Implications for quantum dot photovoltaics

NASA Astrophysics Data System (ADS)

Tisdale, William A., III

Finding a viable supply of clean, renewable energy is one of the most daunting challenges facing the world today. Solar cells have had limited impact in meeting this challenge because of their high cost and low power conversion efficiencies. Semiconductor nanocrystals, or quantum dots, are promising materials for use in novel solar cells because they can be processed with potentially inexpensive solution-based techniques and because they are predicted to have novel optoelectronic properties that could enable the realization of ultra-efficient solar power converters. However, there is a lack of fundamental understanding regarding the behavior of highly-excited, or "hot," charge carriers near quantum-dot and semiconductor interfaces, which is of paramount importance to the rational design of high-efficiency devices. The elucidation of these ultrafast hot electron dynamics is the central aim of this Dissertation. I present a theoretical framework for treating the electronic interactions between quantum dots and bulk semiconductor surfaces and propose a novel experimental technique, time-resolved surface second harmonic generation (TR-SHG), for probing these interactions. I then describe a series of experimental investigations into hot electron dynamics in specific quantum-dot/semiconductor systems. A two-photon photoelectron spectroscopy (2PPE) study of the technologically-relevant ZnO(1010) surface reveals ultrafast (sub-30fs) cooling of hot electrons in the bulk conduction band, which is due to strong electron-phonon coupling in this highly polar material. The presence of a continuum of defect states near the conduction band edge results in Fermi-level pinning and upward (n-type) band-bending at the (1010) surface and provides an alternate route for electronic relaxation. In monolayer films of colloidal PbSe quantum dots, chemical treatment with either hydrazine or 1,2-ethanedithiol results in strong and tunable electronic coupling between neighboring quantum dots. A TR-SHG study of these electronically-coupled quantum-dot films reveals temperature-activated cooling of hot charge carriers and coherent excitation of a previously-unidentified surface optical phonon. Finally, I report the first experimental observation of ultrafast electron transfer from the higher excited states of a colloidal quantum dot (PbSe) to delocalized conduction band states of a widely-used electron acceptor (TiO2). The electric field resulting from ultrafast (<50fs) separation of charge carriers across the PbSe/TiO2(110) interface excites coherent vibration of the TiO2 surface atoms, whose collective motions can be followed in real time.

Wide-range ideal 2D Rashba electron gas with large spin splitting in Bi2Se3/MoTe2 heterostructure

NASA Astrophysics Data System (ADS)

Wang, Te-Hsien; Jeng, Horng-Tay

2017-02-01

An application-expected ideal two-dimensional Rashba electron gas, i.e., nearly all the conduction electrons occupy the Rashba bands, is crucial for semiconductor spintronic applications. We demonstrate that such an ideal two-dimensional Rashba electron gas with a large Rashba splitting can be realized in a topological insulator Bi2Se3 ultrathin film grown on a transition metal dichalcogenides MoTe2 substrate through first-principle calculations. Our results show the Rashba bands exclusively over a very large energy interval of about 0.6 eV around the Fermi level within the MoTe2 semiconducting gap. Such a wide-range ideal two-dimensional Rashba electron gas with a large spin splitting, which is desirable for real devices utilizing the Rashba effect, has never been found before. Due to the strong spin-orbit coupling, the strength of the Rashba splitting is comparable with that of the heavy-metal surfaces such as Au and Bi surfaces, giving rise to a spin precession length as small as 10 nm. The maximum in-plane spin polarization of the inner (outer) Rashba band near the Γ point is about 70% (60%). The room-temperature coherence length is at least several times longer than the spin precession length, providing good coherency through the spin processing devices. The wide energy window for ideal Rashba bands, small spin precession length, as well as long spin coherence length in this two-dimensional topological insulator/transition metal dichalcogenides heterostructure pave the way for realizing an ultrathin nano-scale spintronic device such as the Datta-Das spin transistor at room-temperature.

Direct evidence of void passivation in Cu(InGa)(SSe){sub 2} absorber layers

DOE Office of Scientific and Technical Information (OSTI.GOV)

Lee, Dongho; Kim, Young-Su; Mo, Chan B.

We have investigated the charge collection condition around voids in copper indium gallium sulfur selenide (CIGSSe) solar cells fabricated by sputter and a sequential process of selenization/sulfurization. In this study, we found direct evidence of void passivation by using the junction electron beam induced current method, transmission electron microscopy, and energy dispersive X-ray spectroscopy. The high sulfur concentration at the void surface plays an important role in the performance enhancement of the device. The recombination around voids is effectively suppressed by field-assisted void passivation. Hence, the generated carriers are easily collected by the electrodes. Therefore, when the S/(S + Se)more » ratio at the void surface is over 8% at room temperature, the device performance degradation caused by the recombination at the voids is negligible at the CIGSSe layer.« less

Room Temperature Intrinsic Ferromagnetism in Epitaxial Manganese Selenide Films in the Monolayer Limit

NASA Astrophysics Data System (ADS)

O'Hara, Dante J.; Zhu, Tiancong; Trout, Amanda H.; Ahmed, Adam S.; Luo, Yunqiu Kelly; Lee, Choong Hee; Brenner, Mark R.; Rajan, Siddharth; Gupta, Jay A.; McComb, David W.; Kawakami, Roland K.

2018-05-01

Monolayer van der Waals (vdW) magnets provide an exciting opportunity for exploring two-dimensional (2D) magnetism for scientific and technological advances, but the intrinsic ferromagnetism has only been observed at low temperatures. Here, we report the observation of room temperature ferromagnetism in manganese selenide (MnSe$_x$) films grown by molecular beam epitaxy (MBE). Magnetic and structural characterization provides strong evidence that in the monolayer limit, the ferromagnetism originates from a vdW manganese diselenide (MnSe$_2$) monolayer, while for thicker films it could originate from a combination of vdW MnSe$_2$ and/or interfacial magnetism of $\\alpha$-MnSe(111). Magnetization measurements of monolayer MnSe$_x$ films on GaSe and SnSe$_2$ epilayers show ferromagnetic ordering with large saturation magnetization of ~ 4 Bohr magnetons per Mn, which is consistent with density functional theory calculations predicting ferromagnetism in monolayer 1T-MnSe$_2$. Growing MnSe$_x$ films on GaSe up to high thickness (~ 40 nm) produces $\\alpha$-MnSe(111), and an enhanced magnetic moment (~ 2x) compared to the monolayer MnSe$_x$ samples. Detailed structural characterization by scanning transmission electron microscopy (STEM), scanning tunneling microscopy (STM), and reflection high energy electron diffraction (RHEED) reveal an abrupt and clean interface between GaSe(0001) and $\\alpha$-MnSe(111). In particular, the structure measured by STEM is consistent with the presence of a MnSe$_2$ monolayer at the interface. These results hold promise for potential applications in energy efficient information storage and processing.

Synthesis and spectroscopic properties of silica-dye-semiconductor nanocrystal hybrid particles.

PubMed

Ren, Ting; Erker, Wolfgang; Basché, Thomas; Schärtl, Wolfgang

2010-12-07

We prepared silica-dye-nanocrystal hybrid particles and studied the energy transfer from semiconductor nanocrystals (= donor) to organic dye molecules (= acceptor). Multishell CdSe/CdS/ZnS semiconductor nanocrystals were adsorbed onto monodisperse Stöber silica particles with an outer silica shell of thickness 2-23 nm containing organic dye molecules (Texas Red). The thickness of this dye layer has a strong effect on the energy transfer efficiency, which is explained by the increase in the number of dye molecules homogeneously distributed within the silica shell, in combination with an enhanced surface adsorption of nanocrystals with increasing dye amount. Our conclusions were underlined by comparison of the experimental results with numerically calculated FRET efficiencies and by control experiments confirming attractive interaction between the nanocrystals and Texas Red freely dissolved in solution.

Widespread spin polarization effects in photoemission from topological insulators

DOE Office of Scientific and Technical Information (OSTI.GOV)

Jozwiak, C.; Chen, Y. L.; Fedorov, A. V.

2011-06-22

High-resolution spin- and angle-resolved photoemission spectroscopy (spin-ARPES) was performed on the three-dimensional topological insulator Bi{sub 2}Se{sub 3} using a recently developed high-efficiency spectrometer. The topological surface state's helical spin structure is observed, in agreement with theoretical prediction. Spin textures of both chiralities, at energies above and below the Dirac point, are observed, and the spin structure is found to persist at room temperature. The measurements reveal additional unexpected spin polarization effects, which also originate from the spin-orbit interaction, but are well differentiated from topological physics by contrasting momentum and photon energy and polarization dependencies. These observations demonstrate significant deviations ofmore » photoelectron and quasiparticle spin polarizations. Our findings illustrate the inherent complexity of spin-resolved ARPES and demonstrate key considerations for interpreting experimental results.« less

Structural and optical properties of nanostructured CdSe thin films prepared by electrochemical deposition

NASA Astrophysics Data System (ADS)

Bai, Rekha; Chaudhary, Sujeet; Pandya, Dinesh K.

2018-05-01

Cadmium selenide (CdSe) nanostructured thin films have been grown on fluorine doped tin oxide (FTO) coated glass substrates by potentiostatic electrochemical deposition (ECD) technique for use in solar energy conversion devices. The effect of bath temperature on the structural, morphological and optical properties of prepared CdSe films has been explored. X-ray diffraction (XRD) and Raman spectroscopy clearly show that the CdSe films are polycrystalline and exhibit phase transformation from wurtzite to zincblende structure with increase in bath temperature. Optical spectra reveal that the nanostructured CdSe films have high absorbance in visible region and the films show a red shift in direct optical energy band gap from 1.90 to 1.65 eV with increase in bath temperature due to change in phase and bandgap tuning related to quantum confinement effect.

Common electronic origin of superconductivity in (Li,Fe)OHFeSe bulk superconductor and single-layer FeSe/SrTiO3 films.

PubMed

Zhao, Lin; Liang, Aiji; Yuan, Dongna; Hu, Yong; Liu, Defa; Huang, Jianwei; He, Shaolong; Shen, Bing; Xu, Yu; Liu, Xu; Yu, Li; Liu, Guodong; Zhou, Huaxue; Huang, Yulong; Dong, Xiaoli; Zhou, Fang; Liu, Kai; Lu, Zhongyi; Zhao, Zhongxian; Chen, Chuangtian; Xu, Zuyan; Zhou, X J

2016-02-08

The mechanism of high-temperature superconductivity in the iron-based superconductors remains an outstanding issue in condensed matter physics. The electronic structure plays an essential role in dictating superconductivity. Recent revelation of distinct electronic structure and high-temperature superconductivity in the single-layer FeSe/SrTiO3 films provides key information on the role of Fermi surface topology and interface in inducing or enhancing superconductivity. Here we report high-resolution angle-resolved photoemission measurements on the electronic structure and superconducting gap of an FeSe-based superconductor, (Li0.84Fe0.16)OHFe0.98Se, with a Tc at 41 K. We find that this single-phase bulk superconductor shows remarkably similar electronic behaviours to that of the superconducting single-layer FeSe/SrTiO3 films in terms of Fermi surface topology, band structure and the gap symmetry. These observations provide new insights in understanding high-temperature superconductivity in the single-layer FeSe/SrTiO3 films and the mechanism of superconductivity in the bulk iron-based superconductors.

Quantum Hall effect in dual gated BiSbTeSe2 topological insulator

NASA Astrophysics Data System (ADS)

Chong, Su Kong; Han, Kyu Bum; Nagaoka, Akira; Harmer, Jared; Tsuchikawa, Ryuichi; Sparks, Taylor D.; Deshpande, Vikram V.

The discovery of topological insulators (TIs) has expanded the family of Dirac materials and enables the probing of exotic matter such as Majorana fermions and magnetic monopoles. Different from conventional 2D electron gas, 3D TIs exhibit a gapped insulating bulk and gapless topological surface states as a result of the strong spin-orbit coupling. BiSbTeSe2 is also known to be a 3D TI with a large intrinsic bulk gap of about 0.3 eV and a single Dirac cone surface state. The highly bulk insulating BiSbTeSe2 permits surface dominated conduction, which is an ideal system for the study of quantum Hall effect (QHE). Due to the spin-momentum locking, the Dirac fermions at the topological surface states have a degeneracy of one. In the QH regime, the Hall conductance is quantized to (n + 1 / 2) e2 / h , where n is an integer and the factor of half is related to Berry curvature. In this work, we study the QHE 3D TI using a dual gated BiSbTeSe2 device. By tuning the chemical potentials on top and bottom surfaces, integer QHE with Landau filling factors, ν = 0, +/-1, and +/-2 are observed.

Hybrid crystals of cuprates and iron-based superconductors

NASA Astrophysics Data System (ADS)

Xia, Dai; Cong-Cong, Le; Xian-Xin, Wu; Jiang-Ping, Hu

2016-07-01

We propose two possible new compounds, Ba2CuO2Fe2As2 and K2CuO2Fe2Se2, which hybridize the building blocks of two high temperature superconductors, cuprates and iron-based superconductors. These compounds consist of square CuO2 layers and antifluorite-type Fe2 X 2 (X = As, Se) layers separated by Ba/K. The calculations of binding energies and phonon spectra indicate that they are dynamically stable, which ensures that they may be experimentally synthesized. The Fermi surfaces and electronic structures of the two compounds inherit the characteristics of both cuprates and iron-based superconductors. These compounds can be superconductors with intriguing physical properties to help to determine the pairing mechanisms of high T c superconductivity. Project supported by the National Basic Research Program of China (Grant No. 2015CB921300), the National Natural Science Foundation of China (Grant Nos. 1190020 and 11334012), and the Strategic Priority Research Program of Chinese Academy of Sciences (Grant No. XDB07000000).

Electron beam crystallization of Te 1-xSe x films

NASA Astrophysics Data System (ADS)

Vermaak, J. S.; Raubenheimer, D.

1987-11-01

In situ transmission electron microscopy has been used to study the effect of high energy electrons on the amorphous-to-crystalline phase transformation, the isothermal growth rates, as well as the structure and orientation of the recrystallized Te 0.7Se 0.3 thin films. It is shown that the beam effect is not a pure thermal effect. It is proposed that the electron beam initiates nucleation and promotes growth by the interaction of the high energy electrons with the van der Waals type bonds between the short composite Te-Se chains.

Single-energy intensity modulated proton therapy

NASA Astrophysics Data System (ADS)

Farace, Paolo; Righetto, Roberto; Cianchetti, Marco

2015-09-01

In this note, an intensity modulated proton therapy (IMPT) technique, based on the use of high single-energy (SE-IMPT) pencil beams, is described. The method uses only the highest system energy (226 MeV) and only lateral penumbra to produce dose gradient, as in photon therapy. In the study, after a preliminary analysis of the width of proton pencil beam penumbras at different depths, SE-IMPT was compared with conventional IMPT in a phantom containing titanium inserts and in a patient, affected by a spinal chordoma with fixation rods. It was shown that SE-IMPT has the potential to produce a sharp dose gradient and that it is not affected by the uncertainties produced by metal implants crossed by the proton beams. Moreover, in the chordoma patient, target coverage and organ at risk sparing of the SE-IMPT plan resulted comparable to that of the less reliable conventional IMPT technique. Robustness analysis confirmed that SE-IMPT was not affected by range errors, which can drastically affect the IMPT plan. When accepting a low-dose spread as in modern photon techniques, SE-IMPT could be an option for the treatment of lesions (e.g. cervical bone tumours) where steep dose gradient could improve curability, and where range uncertainty, due for example to the presence of metal implants, hampers conventional IMPT.