Interface Physics in Complex Oxide Heterostructures
NASA Astrophysics Data System (ADS)
Zubko, Pavlo; Gariglio, Stefano; Gabay, Marc; Ghosez, Philippe; Triscone, Jean-Marc
2011-03-01
Complex transition metal oxides span a wide range of crystalline structures and play host to an incredible variety of physical phenomena. High dielectric permittivities, piezo-, pyro-, and ferroelectricity are just a few of the functionalities offered by this class of materials, while the potential for applications of the more exotic properties like high temperature superconductivity and colossal magnetoresistance is still waiting to be fully exploited. With recent advances in deposition techniques, the structural quality of oxide heterostructures now rivals that of the best conventional semiconductors, taking oxide electronics to a new level. Such heterostructures have enabled the fabrication of artificial multifunctional materials. At the same time they have exposed a wealth of phenomena at the boundaries where compounds with different structural instabilities and electronic properties meet, giving unprecedented access to new physics emerging at oxide interfaces. Here we highlight some of these exciting new interface phenomena.
Electrically coupling complex oxides to semiconductors: A route to novel material functionalities
Ngai, J. H.; Ahmadi-Majlan, K.; Moghadam, J.; ...
2017-01-12
Complex oxides and semiconductors exhibit distinct yet complementary properties owing to their respective ionic and covalent natures. By electrically coupling complex oxides to traditional semiconductors within epitaxial heterostructures, enhanced or novel functionalities beyond those of the constituent materials can potentially be realized. Essential to electrically coupling complex oxides to semiconductors is control of the physical structure of the epitaxially grown oxide, as well as the electronic structure of the interface. In this paper, we discuss how composition of the perovskite A- and B-site cations can be manipulated to control the physical and electronic structure of semiconductor—complex oxide heterostructures. Two prototypicalmore » heterostructures, Ba 1-xSr xTiO 3/Ge and SrZr xTi 1-xO 3/Ge, will be discussed. In the case of Ba 1-xSr xTiO 3/Ge, we discuss how strain can be engineered through A-site composition to enable the re-orientable ferroelectric polarization of the former to be coupled to carriers in the semiconductor. In the case of SrZr xTi 1-xO 3/Ge we discuss how B-site composition can be exploited to control the band offset at the interface. Finally, analogous to heterojunctions between compound semiconducting materials, control of band offsets, i.e., band-gap engineering, provides a pathway to electrically couple complex oxides to semiconductors to realize a host of functionalities.« less
Electrically coupling complex oxides to semiconductors: A route to novel material functionalities
DOE Office of Scientific and Technical Information (OSTI.GOV)
Ngai, J. H.; Ahmadi-Majlan, K.; Moghadam, J.
Complex oxides and semiconductors exhibit distinct yet complementary properties owing to their respective ionic and covalent natures. By electrically coupling complex oxides to traditional semiconductors within epitaxial heterostructures, enhanced or novel functionalities beyond those of the constituent materials can potentially be realized. Essential to electrically coupling complex oxides to semiconductors is control of the physical structure of the epitaxially grown oxide, as well as the electronic structure of the interface. In this paper, we discuss how composition of the perovskite A- and B-site cations can be manipulated to control the physical and electronic structure of semiconductor—complex oxide heterostructures. Two prototypicalmore » heterostructures, Ba 1-xSr xTiO 3/Ge and SrZr xTi 1-xO 3/Ge, will be discussed. In the case of Ba 1-xSr xTiO 3/Ge, we discuss how strain can be engineered through A-site composition to enable the re-orientable ferroelectric polarization of the former to be coupled to carriers in the semiconductor. In the case of SrZr xTi 1-xO 3/Ge we discuss how B-site composition can be exploited to control the band offset at the interface. Finally, analogous to heterojunctions between compound semiconducting materials, control of band offsets, i.e., band-gap engineering, provides a pathway to electrically couple complex oxides to semiconductors to realize a host of functionalities.« less
Instrumentation for Epitaxial Growth of Complex Oxides
2015-12-17
synthesis of complex oxide heterostructures. A RF oxygen plasma source was acquired to increase the oxidizing ability of the growth environment, an...improvement that will prove critical in stabilizing materials with high oxidization states. The plasma source and accompanying electronics were purchased...2014 14-Aug-2015 Approved for Public Release; Distribution Unlimited Final Report: Instrumentation for Epitaxial Growth of Complex Oxides The views
Atomic-scale visualization of oxide thin-film surfaces.
Iwaya, Katsuya; Ohsawa, Takeo; Shimizu, Ryota; Okada, Yoshinori; Hitosugi, Taro
2018-01-01
The interfaces of complex oxide heterostructures exhibit intriguing phenomena not observed in their constituent materials. The oxide thin-film growth of such heterostructures has been successfully controlled with unit-cell precision; however, atomic-scale understandings of oxide thin-film surfaces and interfaces have remained insufficient. We examined, with atomic precision, the surface and electronic structures of oxide thin films and their growth processes using low-temperature scanning tunneling microscopy. Our results reveal that oxide thin-film surface structures are complicated in contrast to the general perception and that atomically ordered surfaces can be achieved with careful attention to the surface preparation. Such atomically ordered oxide thin-film surfaces offer great opportunities not only for investigating the microscopic origins of interfacial phenomena but also for exploring new surface phenomena and for studying the electronic states of complex oxides that are inaccessible using bulk samples.
NASA Astrophysics Data System (ADS)
Wang, Aaron; Chien, TeYu
2018-03-01
Complex oxide heterostructure interfaces have shown novel physical phenomena which do not exist in bulk materials. These heterostructures can be used in the potential applications in the next generation devices and served as the playgrounds for the fundamental physics research. The direct measurements of the interfaces with excellent spatial resolution and physical property information is rather difficult to achieve with the existing tools. Recently developed cross-sectional scanning tunneling microscopy and spectroscopy (XSTM/S) for complex oxide interfaces have proven to be capable of providing local electronic density of states (LDOS) information at the interface with spatial resolution down to nanometer scale. In this perspective, we will briefly introduce the basic idea and some recent achievements in using XSTM/S to study complex oxide interfaces. We will also discuss the future of this technique and the field of the interfacial physics.
Structural “ δ Doping” to Control Local Magnetization in Isovalent Oxide Heterostructures
DOE Office of Scientific and Technical Information (OSTI.GOV)
Moon, E. J.; He, Q.; Ghosh, S.
Modulation and δ-doping strategies, in which atomically thin layers of charged dopants are precisely deposited within a heterostructure, have played enabling roles in the discovery of new physical behavior in electronic materials. Here in this paper, we demonstrate a purely structural “δ-doping” strategy in complex oxide heterostructures, in which atomically thin manganite layers are inserted into an isovalent manganite host, thereby modifying the local rotations of corner-connected MnO 6 octahedra. Combining scanning transmission electron microscopy, polarized neutron reflectometry, and density functional theory, we reveal how local magnetic exchange interactions are enhanced within the spatially confined regions of suppressed octahedral rotations.more » Finally, the combined experimental and theoretical results illustrate the potential to utilize noncharge-based approaches to “doping” in order to enhance or suppress functional properties within spatially confined regions of oxide heterostructures.« less
Structural “ δ Doping” to Control Local Magnetization in Isovalent Oxide Heterostructures
Moon, E. J.; He, Q.; Ghosh, S.; ...
2017-11-08
Modulation and δ-doping strategies, in which atomically thin layers of charged dopants are precisely deposited within a heterostructure, have played enabling roles in the discovery of new physical behavior in electronic materials. Here in this paper, we demonstrate a purely structural “δ-doping” strategy in complex oxide heterostructures, in which atomically thin manganite layers are inserted into an isovalent manganite host, thereby modifying the local rotations of corner-connected MnO 6 octahedra. Combining scanning transmission electron microscopy, polarized neutron reflectometry, and density functional theory, we reveal how local magnetic exchange interactions are enhanced within the spatially confined regions of suppressed octahedral rotations.more » Finally, the combined experimental and theoretical results illustrate the potential to utilize noncharge-based approaches to “doping” in order to enhance or suppress functional properties within spatially confined regions of oxide heterostructures.« less
Interfacial Magnetism in Complex Oxide Heterostructures Probed by Neutrons and X-rays
Liu, Yaohua; Ke, Xianglin
2015-09-02
Magnetic complex-oxide heterostructures are of keen interest because a wealth of phenomena at the interface of dissimilar materials can give rise to fundamentally new physics and potentially valuable functionalities. Altered magnetization, novel magnetic coupling and emergent interfacial magnetism at the epitaxial layered-oxide interfaces have all been intensively investigated, which shapes our understanding on how to utilize those materials, particularly for spintronics. Neutron and x-ray based techniques have played a decisive role in characterizing interfacial magnetic structures and clarifying the underlying physics in this rapidly developing field. Here we review some recent experimental results, with an emphasis on those studied viamore » polarized neutron reflectometery and polarized x-ray absorption spectroscopy. We conclude with some perspectives.« less
Interfacial magnetism in complex oxide heterostructures probed by neutrons and x-rays.
Liu, Yaohua; Ke, Xianglin
2015-09-23
Magnetic complex-oxide heterostructures are of keen interest because a wealth of phenomena at the interface of dissimilar materials can give rise to fundamentally new physics and potentially valuable functionalities. Altered magnetization, novel magnetic coupling and emergent interfacial magnetism at the epitaxial layered-oxide interfaces are under intensive investigation, which shapes our understanding on how to utilize those materials, particularly for spintronics. Neutron and x-ray based techniques have played a decisive role in characterizing interfacial magnetic structures and clarifying the underlying physics in this rapidly developing field. Here we review some recent experimental results, with an emphasis on those studied via polarized neutron reflectometery and polarized x-ray absorption spectroscopy. We conclude with some perspectives.
Thermoelectric Properties of Complex Oxide Heterostructures
NASA Astrophysics Data System (ADS)
Cain, Tyler Andrew
Thermoelectrics are a promising energy conversion technology for power generation and cooling systems. The thermal and electrical properties of the materials at the heart of thermoelectric devices dictate conversion efficiency and technological viability. Studying the fundamental properties of potentially new thermoelectric materials is of great importance for improving device performance and understanding the electronic structure of materials systems. In this dissertation, investigations on the thermoelectric properties of a prototypical complex oxide, SrTiO3, are discussed. Hybrid molecular beam epitaxy (MBE) is used to synthesize La-doped SrTiO3 thin films, which exhibit high electron mobilities and large Seebeck coefficients resulting in large thermoelectric power factors at low temperatures. Large interfacial electron densities have been observed in SrTiO3/RTiO 3 (R=Gd,Sm) heterostructures. The thermoelectric properties of such heterostructures are investigated, including the use of a modulation doping approach to control interfacial electron densities. Low-temperature Seebeck coefficients of extreme electron-density SrTiO3 quantum wells are shown to provide insight into their electronic structure.
DOE Office of Scientific and Technical Information (OSTI.GOV)
Chopra, Nitin, E-mail: nchopra@eng.ua.edu; Department of Biological Sciences, The University of Alabama, Tuscaloosa, AL 35487; Shi, Wenwu
2014-10-15
Nanoscale heterostructures composed of standing copper oxide nanowires decorated with Au nanoparticles and shells of titania and indium tin oxide were fabricated. The fabrication process involved surfactant-free and wet-chemical nucleation of gold nanoparticles on copper oxide nanowires followed by a line-of-sight sputtering of titania or indium tin oxide. The heterostructures were characterized using high resolution electron microscopy, diffraction, and energy dispersive spectroscopy. The interfaces, morphologies, crystallinity, phases, and chemical compositions were analyzed. The process of direct nucleation of gold nanoparticles on copper oxide nanoparticles resulted in low energy interface with aligned lattice for both the components. Coatings of polycrystalline titaniamore » or amorphous indium tin oxide were deposited on standing copper oxide nanowire–gold nanoparticle heterostructures. Self-shadowing effect due to standing nanowire heterostructures was observed for line-of-sight sputter deposition of titania or indium tin oxide coatings. Finally, the heterostructures were studied using Raman spectroscopy and ultraviolet–visible spectroscopy, including band gap energy analysis. Tailing in the band gap energy at longer wavelengths (or lower energies) was observed for the nanowire heterostructures. - Highlights: • Heterostructures comprised of CuO nanowires coated with Au nanoparticles. • Au nanoparticles exhibited nearly flat and low energy interface with nanowire. • Heterostructures were further sputter-coated with oxide shell of TiO{sub 2} or ITO. • The process resulted in coating of polycrystalline TiO{sub 2} and amorphous ITO shell.« less
Non-Fermi liquids in oxide heterostructures
NASA Astrophysics Data System (ADS)
Stemmer, Susanne; Allen, S. James
2018-06-01
Understanding the anomalous transport properties of strongly correlated materials is one of the most formidable challenges in condensed matter physics. For example, one encounters metal-insulator transitions, deviations from Landau Fermi liquid behavior, longitudinal and Hall scattering rate separation, a pseudogap phase, and bad metal behavior. These properties have been studied extensively in bulk materials, such as the unconventional superconductors and heavy fermion systems. Oxide heterostructures have recently emerged as new platforms to probe, control, and understand strong correlation phenomena. This article focuses on unconventional transport phenomena in oxide thin film systems. We use specific systems as examples, namely charge carriers in SrTiO3 layers and interfaces with SrTiO3, and strained rare earth nickelate thin films. While doped SrTiO3 layers appear to be a well behaved, though complex, electron gas or Fermi liquid, the rare earth nickelates are a highly correlated electron system that may be classified as a non-Fermi liquid. We discuss insights into the underlying physics that can be gained from studying the emergence of non-Fermi liquid behavior as a function of the heterostructure parameters. We also discuss the role of lattice symmetry and disorder in phenomena such as metal-insulator transitions in strongly correlated heterostructures.
NASA Astrophysics Data System (ADS)
Sanchez-Santolino, Gabriel; Tornos, Javier; Leon, Carlos; Varela, María; Pennycook, Stephen J.; Santamaría, Jacobo
2014-03-01
Interfaces in complex oxide heterostructures are responsible for exciting new physics, which is directly related to the chemical, structural and electronic properties at the atomic scale. Here, we study artificial multiferroic heterostructures combining ferromagnetic La0.7Sr0.3MnO3 with ferroelectric BaTiO3 by atomic resolution aberration-corrected scanning transmission electron microscopy (STEM) and electron energy-loss spectroscopy. Measurements of the atomic positions in the STEM images permit calculating relative displacements and hence, local polarization. Polarization gradients can be observed in annular bright field images which seem to be correlated to strain gradients associated with the large lattice mismatch between barriers and electrodes. Spectroscopic measurements suggest the presence of O vacancies through the ferroelectric layers. Understanding the effect of the charge carriers associated with the oxygen vacancies may be the key to control the dynamics of domain walls in these heterostructures. Acknowledgements ORNL: U.S. DOE-BES, Materials Sciences and Engineering Division. UCM: ERC Starting Investigator Award, Spanish MICINN MAT2011-27470-C02 and Consolider Ingenio 2010 - CSD2009-00013 (Imagine), CAM S2009/MAT-1756 (Phama).
2014-01-08
more energy efficient, lightweight, compact, and less noisy. Studies on ME heterostructures are mostly based on complex oxide piezoelectric ceramic or...except for a recent demonstration of a spin spray deposited ZnO films [17, 18]. ZnO is a typical piezoelectric material , which makes it a good...erties which makes it applicable in a wide variety of electron, optoelectronic, spintronics and nanodevices [17, 18]. The piezoelectric properties of
Ultrathin Limit of Exchange Bias Coupling at Oxide Multiferroic/Ferromagnetic Interfaces
2013-07-12
perfect, lattice-matched hetero- structures of complex perovskite oxides using state-of-the-art thin fi lm growth techniques has generated new physical...investigated for several BFO/LSMO heterostructures by X-ray absorption spectroscopy (XAS) measurements at 17 K of the Fe- L 2,3 edge at the Advanced Light
NASA Astrophysics Data System (ADS)
Cui, B.; Song, C.; Li, F.; Zhong, X. Y.; Wang, Z. C.; Werner, P.; Gu, Y. D.; Wu, H. Q.; Saleem, M. S.; Parkin, S. S. P.; Pan, F.
2017-10-01
Manipulation of oxygen vacancies (VO ) in single oxide layers by varying the electric field can result in significant modulation of the ground state. However, in many oxide multilayers with strong application potentials, e.g., ferroelectric tunnel junctions and solid-oxide fuel cells, understanding VO behavior in various layers under an applied electric field remains a challenge, owing to complex VO transport between different layers. By sweeping the external voltage, a reversible manipulation of VO and a corresponding fixed magnetic phase transition sequence in cobaltite/manganite (SrCoO3 -x/La0.45Sr0.55MnO3 -y ) heterostructures are reported. The magnetic phase transition sequence confirms that the priority of electric-field-induced VO formation or annihilation in the complex bilayer system is mainly determined by the VO formation energies and Gibbs free-energy differences, which is supported by theoretical analysis. We not only realize a reversible manipulation of the magnetic phase transition in an oxide bilayer but also provide insight into the electric-field control of VO engineering in heterostructures.
NASA Astrophysics Data System (ADS)
Wrobel, F.; Mark, A. F.; Christiani, G.; Sigle, W.; Habermeier, H.-U.; van Aken, P. A.; Logvenov, G.; Keimer, B.; Benckiser, E.
2017-01-01
Variations in growth conditions associated with different deposition techniques can greatly affect the phase stability and defect structure of complex oxide heterostructures. We synthesized superlattices of the paramagnetic metal LaNiO3 and the large band gap insulator LaAlO3 by atomic layer-by-layer molecular beam epitaxy (MBE) and pulsed laser deposition (PLD) and compared their crystallinity and microstructure as revealed by high-resolution transmission electron microscopy images and resistivity. The MBE samples show a higher density of stacking faults but smoother interfaces and generally higher electrical conductivity. Our study identifies the opportunities and challenges of MBE and PLD growth and serves as a general guide for the choice of the deposition technique for perovskite oxides.
Polarization-coupled tunable resistive behavior in oxide ferroelectric heterostructures
DOE Office of Scientific and Technical Information (OSTI.GOV)
Gruverman, Alexei; Tsymbal, Evgeny Y.; Eom, Chang-Beom
2017-05-03
This research focuses on investigation of the physical mechanism of the electrically and mechanically tunable resistive behavior in oxide ferroelectric heterostructures with engineered interfaces realized via a strong coupling of ferroelectric polarization with tunneling electroresistance and metal-insulator (M-I) transitions. This report describes observation of electrically conductive domain walls in semiconducting ferroelectrics, voltage-free control of resistive switching and demonstration of a new mechanism of electrical control of 2D electron gas (2DEG) at oxide interfaces. The research goals are achieved by creating strong synergy between cutting-edge fabrication of epitaxial single-crystalline complex oxides, nanoscale electrical characterization by scanning probe microscopy and theoretical modelingmore » of the observed phenomena. The concept of the ferroelectric devices with electrically and mechanically tunable nonvolatile resistance represents a new paradigm shift in realization of the next-generation of non-volatile memory devices and low-power logic switches.« less
Quantifying the electronic reconstruction in LaTiO3/LaNiO3/(LaAlO3)3 heterostructures using RIXS
NASA Astrophysics Data System (ADS)
Fabbris, Gilberto; Disa, Ankit S.; Ismail-Beigi, Sohab; Walker, Frederick J.; Ahn, Charles H.; Pelliciari, Jonathan; Huang, Yaobo; Schmitt, Thorsten; Xu, Lei; Hozoi, Liviu; van den Brink, Jeroen; Dean, Mark
A novel approach for manipulating the 3d state in transition metal oxide heterostructures has emerged with the growth of trilayer nickelate LaTiO3/LaNiO3/(LaAlO3)3 (LTNAO). This heterostructure induces a striking reconstruction of the LaNiO3 electronic structure, which is due to a combination of charge transfer from Ti's 3d state and octahedral elongation along the c axis. We use resonant inelastic x-ray scattering (RIXS) experiments at Ni L2,3 and O K edges to spectroscopically resolve the LTNAO electronic structure. Surprisingly, our results show that the octahedral elongation generates minor changes in crystal fields at Ni's 3d state compared to bulk LaNiO3. Instead, heterostructuring creates an anisotropic reconstruction of the Ni 3d - O 2p hybridization. The x2-y2 orbital is significantly more hybridized with O p, leading to a 3z2-r2/x2-y2 hole ratio of ~0.55 and large orbital polarization as measured by x-ray absorption spectroscopy. This work establishes RIXS as an ultra-sensitive probe of complex oxide heterostructures. Work at BNL was supported by the US Department of Energy under Award No DEAC02-98CH10886 and under Early Career Award No 20878.
NASA Astrophysics Data System (ADS)
Jana, S. K.; Rao, V. P.; Banerjee, S.
2013-02-01
In this paper we have shown enhanced supercapacitive property of electrochemically reduced graphene oxide (ERGO) and manganese dioxide (MnO2) based heterostructure over single MnO2 thin film grown by electrochemical deposition on indium tin oxide (ITO). ERGO improves the electrical conduction leading to decrease of the internal resistance of the heterostructure.
NASA Astrophysics Data System (ADS)
Shao, Liangzhi; Nie, Shibin; Shao, Xiankun; Zhang, LinLin; Li, Benxia
2018-03-01
One-dimensional metal-oxide/carbon-fiber (MO/CF) heterostructures were prepared by a facile two-step method using the natural cotton as a carbon source the low-cost commercial metal salts as precursors. The metal oxide nanostructures were first grown on the cotton fibers by a solution chemical deposition, and the metal-oxide/cotton heterostructures were then calcined and carbonized in nitrogen atmosphere. Three typical MO/CF heterostructures of TiO2/CF, ZnO/CF, and Fe2O3/CF were prepared and characterized. The loading amount of the metal oxide nanostructures on carbon fibers can be tuned by controlling the concentration of metal salt in the chemical deposition process. Finally, the performance of the as-obtained MO/CF heterostructures for organic dye removal from water was tested by the photocatalytic degradation under a simulated sunlight, and their properties of high-temperature CO2 adsorption were predicted by the temperature programmed desorption. The present study would provide a desirable strategy for the synthesis of MO/CF heterostructures for various applications.
NASA Astrophysics Data System (ADS)
Entani, S.; Kiguchi, M.; Saiki, K.; Koma, A.
2003-01-01
Epitaxial growth of CoO films was studied using reflection high-energy electron diffraction (RHEED), electron energy loss spectroscopy (EELS), ultraviolet photoelectron spectroscopy (UPS) and Auger electron spectroscopy (AES). The RHEED results indicated that an epitaxial CoO film grew on semiconductor and metal substrates (CoO (0 0 1)∥GaAs (0 0 1), Cu (0 0 1), Ag (0 0 1) and [1 0 0]CoO∥[1 0 0] substrates) by constructing a complex heterostructure with two alkali halide buffer layers. The AES, EELS and UPS results showed that the grown CoO film had almost the same electronic structure as bulk CoO. We could show that use of alkali halide buffer layers was a good way to grow metal oxide films on semiconductor and metal substrates in an O 2 atmosphere. The alkali halide layers not only works as glue to connect very dissimilar materials but also prevents oxidation of metal and semiconductor substrates.
Dynamic defect correlations dominate activated electronic transport in SrTiO3
Snijders, Paul C.; Şen, Cengiz; McConnell, Michael P.; Ma, Ying-Zhong; May, Andrew F.; Herklotz, Andreas; Wong, Anthony T.; Ward, T. Zac
2016-01-01
Strontium titanate (SrTiO3, STO) is a critically important material for the study of emergent electronic phases in complex oxides, as well as for the development of applications based on their heterostructures. Despite the large body of knowledge on STO, there are still many uncertainties regarding the role of defects in the properties of STO, including their influence on ferroelectricity in bulk STO and ferromagnetism in STO-based heterostructures. We present a detailed analysis of the decay of persistent photoconductivity in STO single crystals with defect concentrations that are relatively low but significantly affect their electronic properties. The results show that photo-activated electron transport cannot be described by a superposition of the properties due to independent point defects as current models suggest but is, instead, governed by defect complexes that interact through dynamic correlations. These results emphasize the importance of defect correlations for activated electronic transport properties of semiconducting and insulating perovskite oxides. PMID:27443503
Dynamic defect correlations dominate activated electronic transport in SrTiO 3
Snijders, Paul C.; Sen, Cengiz; McConnell, Michael P.; ...
2016-07-22
Strontium titanate (SrTiO 3, STO) is a critically important material for the study of emergent electronic phases in complex oxides, as well as for the development of applications based on their heterostructures. Despite the large body of knowledge on STO, there are still many uncertainties regarding the role of defects in the properties of STO, including their influence on ferroelectricity in bulk STO and ferromagnetism in STO-based heterostructures. In this paper, we present a detailed analysis of the decay of persistent photoconductivity in STO single crystals with defect concentrations that are relatively low but significantly affect their electronic properties. Themore » results show that photo-activated electron transport cannot be described by a superposition of the properties due to independent point defects as current models suggest but is, instead, governed by defect complexes that interact through dynamic correlations. In conclusion, these results emphasize the importance of defect correlations for activated electronic transport properties of semiconducting and insulating perovskite oxides.« less
NASA Astrophysics Data System (ADS)
Yang, Chi-Yuan; Yadav, Ajay K.; Ramesh, Ramamoorthy; Wen, Yu-Chieh; Hsu, Chia-Hao; Wu, Maw-Kuen; Chia, Chih-Ta; Lin, Kung-Hsuan
Strontium titanate (SrTiO3, STO) and strontium ruthenate (SrRuO3, SRO) are complex oxide with perovskite structure. Their property, such as thermoelectricity and superconductivity, has been widely investigated for scientific and industrial purposes. Recently, complex oxide heterostructures can be grown by pulsed laser deposition. It opens many possibilities f or new properties of materials. With ultrafast pump-probe spectroscopy, we demonstrated that metal-like SRO thin film can be served as a phonon transducer to generate hypersound with frequency of several tens to several hundreads of GHz. This technique can be utilized to study not only the elastic properties of perovskite thin films but also the interfaces. In this study, we used this technique to study the temperature dependence of structural phases in STO. During the crossing over the soft-mode transition in STO around 110 K, the shortening of phonon lifetime were also observed.
DOE Office of Scientific and Technical Information (OSTI.GOV)
Chopra, Nitin, E-mail: nchopra@eng.ua.edu; McWhinney, Hylton G.; Shi Wenwu
2011-06-15
Heterostructures composed of carbon nanotube (CNT) coated with Ni/NiO core/shell nanoparticles (denoted as CNC heterostructures) were synthesized in a wet-chemistry and single-step synthesis route involving direct nucleation of nanoparticles on CNT surface. Two different aspects of CNC heterostructures were studied here. First, it was observed that the nanoparticle coatings were more uniform on the as-produced and non-purified CNTs compared to purified (or acid treated) CNTs. These heterostructures were characterized using electron microscopy, Raman spectroscopy, and energy dispersive spectroscopy. Second, thermal stability of CNC heterostructures was studied by annealing them in N{sub 2}-rich (O{sub 2}-lean) environment between 125 and 750 deg.more » C for 1 h. A detailed X-ray photoelectron spectroscopy and Raman spectroscopy analysis was performed to evaluate the effects of annealing temperatures on chemical composition, phases, and stability of the heterostructures. It was observed that the CNTs present in the heterostructures completely decomposed and core Ni nanoparticle oxidized significantly between 600 and 750 deg. C. - Research Highlights: {yields} Heterostructures composed of CNTs coated with Ni/NiO core/shell nanoparticles. {yields} Poor nanoparticle coverage on purified CNT surface compared to non-purified CNTs. {yields} CNTs in heterostructures decompose between 600 and 750 deg. C in N{sub 2}-rich atmosphere. {yields} Metallic species in heterostructures were oxidized at higher temperatures.« less
Oxide Interfaces: emergent structure and dynamics
DOE Office of Scientific and Technical Information (OSTI.GOV)
Clarke, Roy
This Final Report describes the scientific accomplishments that have been achieved with support from grant DE-FG02-06ER46273 during the period 6/1/2012– 5/31/2016. The overall goals of this program were focused on the behavior of epitaxial oxide heterostructures at atomic length scales (Ångstroms), and correspondingly short time-scales (fs -ns). The results contributed fundamentally to one of the currently most active frontiers in condensed matter physics research, namely to better understand the intricate relationship between charge, lattice, orbital and spin degrees of freedom that are exhibited by complex oxide heterostructures. The findings also contributed towards an important technological goal which was to achievemore » a better basic understanding of structural and electronic correlations so that the unusual properties of complex oxides can be exploited for energy-critical applications. Specific research directions included: probing the microscopic behavior of epitaxial interfaces and buried layers; novel materials structures that emerge from ionic and electronic reconfiguration at epitaxial interfaces; ultrahigh-resolution mapping of the atomic structure of heterointerfaces using synchrotron-based x-ray surface scattering, including direct methods of phase retrieval; using ultrafast lasers to study the effects of transient strain on coherent manipulation of multi-ferroic order parameters; and investigating structural ordering and relaxation processes in real-time.« less
Band Alignment and Charge Transfer in Complex Oxide Interfaces
NASA Astrophysics Data System (ADS)
Zhong, Zhicheng; Hansmann, Philipp
2017-01-01
The synthesis of transition metal heterostructures is currently one of the most vivid fields in the design of novel functional materials. In this paper, we propose a simple scheme to predict band alignment and charge transfer in complex oxide interfaces. For semiconductor heterostructures, band-alignment rules like the well-known Anderson or Schottky-Mott rule are based on comparison of the work function or electron affinity of the bulk components. This scheme breaks down for oxides because of the invalidity of a single work-function approximation as recently shown in [Phys. Rev. B 93, 235116 (2016), 10.1103/PhysRevB.93.235116; Adv. Funct. Mater. 26, 5471 (2016), 10.1002/adfm.201600243]. Here, we propose a new scheme that is built on a continuity condition of valence states originating in the compounds' shared network of oxygen. It allows for the prediction of sign and relative amplitude of the intrinsic charge transfer, taking as input only information about the bulk properties of the components. We support our claims by numerical density functional theory simulations as well as (where available) experimental evidence. Specific applications include (i) controlled doping of SrTiO3 layers with the use of 4 d and 5 d transition metal oxides and (ii) the control of magnetic ordering in manganites through tuned charge transfer.
Enhancing the electron mobility of SrTiO3 with strain
NASA Astrophysics Data System (ADS)
Jalan, Bharat; Allen, S. James; Beltz, Glenn E.; Moetakef, Pouya; Stemmer, Susanne
2011-03-01
We demonstrate, using high-mobility SrTiO3 thin films grown by molecular beam epitaxy, that stress has a pronounced influence on the electron mobility in this prototype complex oxide. Moderate strains result in more than 300% increases in the electron mobilities with values exceeding 120 000 cm2/V s and no apparent saturation in the mobility gains. The results point to a range of opportunities to tailor high-mobility oxide heterostructure properties and open up ways to explore oxide physics.
Electronic and structural reconstruction in titanate heterostructures from first principles
NASA Astrophysics Data System (ADS)
Mulder, Andrew T.; Fennie, Craig J.
2014-03-01
Recent advances in transition metal oxide heterostructures have opened new routes to create materials with novel functionalities and properties. One direction has been to combine a Mott insulating perovskite with an electronic d1 configuration, such as LaTiO3, with a band insulating d0 perovskite, such as SrTiO3. An exciting recent development is the demonstration of interfacial conductivity in GdTiO3/SrTiO3 heterostructures that display a complex structural motif of octahedral rotations and ferromagnetic properties similar to bulk GdTiO3. In this talk we present our first principles investigation of the interplay of structural, electronic, magnetic, and orbital degrees of freedom for a wide range of d1/d0 titanate heterostructures. We find evidence for both rotation driven ferroelectricity and a symmetry breaking electronic reconstruction with a concomitant structural distortion at the interface. We argue that these materials represent an ideal platform to realize novel functionalities such as the electric field control of electronic and magnetic properties.
Highly insulating ferromagnetic cobaltite heterostructures
Choi, Woo Seok; Kang, Kyeong Tae; Jeen, Hyoungjeen; ...
2017-04-02
Ferromagnetic insulators are rather rare but possess great technological potential in, for example, spintronics. Individual control of ferromagnetic properties and electronic transport provides a useful design concept of multifunctional oxide heterostructures. We studied the close correlation among the magnetism, atomic structure, and electronic structure of oxide heterostructures composed of the ferromagnetic perovskite LaCoO 3 and the antiferromagnetic brownmillerite SrCoO 2.5 epitaxial thin film layers. By reversing the stacking sequence of the two layers, we could individually modify the electric resistance and saturation magnetic moment. Lastly, the ferromagnetic insulating behavior in the heterostructures was understood in terms of the electronic reconstructionmore » at the oxide surface/interfaces and crystalline quality of the constituent layers.« less
Highly insulating ferromagnetic cobaltite heterostructures
DOE Office of Scientific and Technical Information (OSTI.GOV)
Choi, Woo Seok; Kang, Kyeong Tae; Jeen, Hyoungjeen
Ferromagnetic insulators are rather rare but possess great technological potential in, for example, spintronics. Individual control of ferromagnetic properties and electronic transport provides a useful design concept of multifunctional oxide heterostructures. We studied the close correlation among the magnetism, atomic structure, and electronic structure of oxide heterostructures composed of the ferromagnetic perovskite LaCoO 3 and the antiferromagnetic brownmillerite SrCoO 2.5 epitaxial thin film layers. By reversing the stacking sequence of the two layers, we could individually modify the electric resistance and saturation magnetic moment. Lastly, the ferromagnetic insulating behavior in the heterostructures was understood in terms of the electronic reconstructionmore » at the oxide surface/interfaces and crystalline quality of the constituent layers.« less
Shi, Wenwu; Chopra, Nitin
2012-10-24
Fabrication of oxide nanowire heterostructures with controlled morphology, interface, and phase purity is critical for high-efficiency and low-cost photocatalysis. Here, we have studied the formation of copper oxide-cobalt nanowire heterostructures by sputtering and subsequent air annealing to result in cobalt oxide (Co(3)O(4))-coated CuO nanowires. This approach allowed fabrication of standing nanowire heterostructures with tunable compositions and morphologies. The vertically standing CuO nanowires were synthesized in a thermal growth method. The shell growth kinetics of Co and Co(3)O(4) on CuO nanowires, morphological evolution of the shell, and nanowire self-shadowing effects were found to be strongly dependent on sputtering duration, air-annealing conditions, and alignment of CuO nanowires. Finite element method (FEM) analysis indicated that alignment and stiffness of CuO-Co nanowire heterostructures greatly influenced the nanomechanical aspects such as von Mises equivalent stress distribution and bending of nanowire heterostructures during the Co deposition process. This fundamental knowledge was critical for the morphological control of Co and Co(3)O(4) on CuO nanowires with desired interfaces and a uniform coating. Band gap energies and phenol photodegradation capability of CuO-Co(3)O(4) nanowire heterostructures were studied as a function of Co(3)O(4) morphology. Multiple absorption edges and band gap tailings were observed for these heterostructures, indicating photoactivity from visible to UV range. A polycrystalline Co(3)O(4) shell on CuO nanowires showed the best photodegradation performance (efficiency ~50-90%) in a low-powered UV or visible light illumination with a sacrificial agent (H(2)O(2)). An anomalously high efficiency (~67.5%) observed under visible light without sacrificial agent for CuO nanowires coated with thin (∼5.6 nm) Co(3)O(4) shell and nanoparticles was especially interesting. Such photoactive heterostructures demonstrate unique sacrificial agent-free, robust, and efficient photocatalysts promising for organic decontamination and environmental remediation.
Surface- and interface-engineered heterostructures for solar hydrogen generation
NASA Astrophysics Data System (ADS)
Chen, Xiangyan; Li, Yanrui; Shen, Shaohua
2018-04-01
Photoelectrochemical (PEC) water splitting based on semiconductor photoelectrodes provides a promising platform for reducing environmental pollution and solving the energy crisis by developing clean, sustainable and environmentally friendly hydrogen energy. In this context, metal oxides with their advantages including low cost, good chemical stability and environmental friendliness, have attracted extensive attention among the investigated candidates. However, the large bandgap, poor charge transfer ability and high charge recombination rate limit the PEC performance of metal oxides as photoelectrodes. To solve this limitation, many approaches toward enhanced PEC water splitting performance, which focus on surface and interface engineering, have been presented. In this topical review, we concentrate on the heterostructure design of some typical metal oxides with narrow bandgaps (e.g. Fe2O3, WO3, BiVO4 and Cu2O) as photoelectrodes. An overview of the surface- and interface-engineered heterostructures, including semiconductor heterojunctions, surface protection, surface passivation and cocatalyst decoration, will be given to introduce the recent advances in metal oxide heterostructures for PEC water splitting. This article aims to provide fundamental references and principles for designing metal oxide heterostructures with high activity and stability as photoelectrodes for PEC solar hydrogen generation.
Interfacial Symmetry Control of Emergent Ferromagnetism
NASA Astrophysics Data System (ADS)
Grutter, Alexander; Borchers, Julie; Kirby, Brian; He, Chunyong; Arenholz, Elke; Vailionis, Arturas; Flint, Charles; Suzuki, Yuri
Atomically precise complex oxide heterostructures provide model systems for the discovery of new emergent phenomena since their magnetism, structure and electronic properties are strongly coupled. Octahedral tilts and rotations have been shown to alter the magnetic properties of complex oxide heterostructures, but typically induce small, gradual magnetic changes. Here, we demonstrate sharp switching between ferromagnetic and antiferromagnetic order at the emergent ferromagnetic interfaces of CaRuO3/CaMnO3 superlattices. Through synchrotron X-ray diffraction and neutron reflectometry, we show that octahedral distortions in superlattices with an odd number of CaMnO3 unit cells in each layer are symmetry mismatched across the interface. In this case, the rotation symmetry switches across the interface, reducing orbital overlap, suppressing charge transfer from Ru to Mn, and disrupting the interfacial double exchange. This disruption switches half of the interfaces from ferromagnetic to antiferromagnetic and lowers the saturation magnetic of the superlattice from 1.0 to 0.5 μB/interfacial Mn. By targeting a purely interfacial emergent magnetic system, we achieve drastic alterations to the magnetic ground state with extremely small changes in layer thickness.
Tunable inversion symmetry in heterostructures of layered oxides
NASA Astrophysics Data System (ADS)
Rondinelli, James
Traditional approaches to create and control functional electronic materials have focused on new phases in previously unknown bulk minerals. More recently, interlayer physics has spawned interest in known materials in unexplored atomic scale geometries, especially in complex transition metal oxides (TMO), where heterostructures can be created on demand. In this talk, I show that although epitaxial strain routinely induces (enhances) electric polarizations, biaxial strain can also induce an unanticipated polar-to-nonpolar (P-NP) structural transition in (001) thin films of naturally layered An + 1Bn O3n+1 (n = 1 - ∞) oxides. Density functional theory calculations and a complete phenomenological model for Ca3Ti2O7 are used to show that the origin of the P-NP transition originates from the interplay of trilinear-related lattice mode interactions active in the layered oxides, and those interactions are directly strain tunable. Moreover these layered oxides exhibit a quasi-two dimensional phonon mode-an acoustic branch with quadratic dispersion, enabling unusual membrane effects such as tunable negative thermal expansion. I conclude by emphasizing that broken inversion symmetric structures offer a plentiful playground for realizing new functionalities in thin films, including new multiferroics from polar metals.
Atomically Precise Interfaces from Non-stoichiometric Deposition
NASA Astrophysics Data System (ADS)
Nie, Yuefeng; Zhu, Ye; Lee, Che-Hui; Kourkoutis, Lena; Mundy, Julia; Junquera, Javier; Ghosez, Philippe; Baek, David; Sung, Suk Hyun; Xi, Xiaoxing; Shen, Kyle; Muller, David; Schlom, Darrell
2015-03-01
Complex oxide heterostructures display some of the most chemically abrupt, atomically precise interfaces, which is advantageous when constructing new interface phases with emergent properties by juxtaposing incompatible ground states. One might assume that atomically precise interfaces result from stoichiometric growth. Here we show that the most precise control is, however, obtained by using deliberate and specific non-stoichiometric growth conditions. For the precise growth of Srn+1TinO3n+1 Ruddlesden-Popper (RP) phases, stoichiometric deposition leads to the loss of the first RP rock-salt double layer, but growing with a strontium-rich surface layer restores the bulk stoichiometry and ordering of the subsurface RP structure. Our results dramatically expand the materials that can be prepared in epitaxial heterostructures with precise interface control--from just the n = 1 end members (perovskites) to the entire RP homologous series--enabling the exploration of novel quantum phenomena at a richer variety of oxide interfaces.
Atomically precise interfaces from non-stoichiometric deposition
NASA Astrophysics Data System (ADS)
Nie, Y. F.; Zhu, Y.; Lee, C.-H.; Kourkoutis, L. F.; Mundy, J. A.; Junquera, J.; Ghosez, Ph.; Baek, D. J.; Sung, S.; Xi, X. X.; Shen, K. M.; Muller, D. A.; Schlom, D. G.
2014-08-01
Complex oxide heterostructures display some of the most chemically abrupt, atomically precise interfaces, which is advantageous when constructing new interface phases with emergent properties by juxtaposing incompatible ground states. One might assume that atomically precise interfaces result from stoichiometric growth. Here we show that the most precise control is, however, obtained by using deliberate and specific non-stoichiometric growth conditions. For the precise growth of Srn+1TinOn+1 Ruddlesden-Popper (RP) phases, stoichiometric deposition leads to the loss of the first RP rock-salt double layer, but growing with a strontium-rich surface layer restores the bulk stoichiometry and ordering of the subsurface RP structure. Our results dramatically expand the materials that can be prepared in epitaxial heterostructures with precise interface control—from just the n=∞ end members (perovskites) to the entire RP homologous series—enabling the exploration of novel quantum phenomena at a richer variety of oxide interfaces.
One-pot growth of two-dimensional lateral heterostructures via sequential edge-epitaxy
NASA Astrophysics Data System (ADS)
Sahoo, Prasana K.; Memaran, Shahriar; Xin, Yan; Balicas, Luis; Gutiérrez, Humberto R.
2018-01-01
Two-dimensional heterojunctions of transition-metal dichalcogenides have great potential for application in low-power, high-performance and flexible electro-optical devices, such as tunnelling transistors, light-emitting diodes, photodetectors and photovoltaic cells. Although complex heterostructures have been fabricated via the van der Waals stacking of different two-dimensional materials, the in situ fabrication of high-quality lateral heterostructures with multiple junctions remains a challenge. Transition-metal-dichalcogenide lateral heterostructures have been synthesized via single-step, two-step or multi-step growth processes. However, these methods lack the flexibility to control, in situ, the growth of individual domains. In situ synthesis of multi-junction lateral heterostructures does not require multiple exchanges of sources or reactors, a limitation in previous approaches as it exposes the edges to ambient contamination, compromises the homogeneity of domain size in periodic structures, and results in long processing times. Here we report a one-pot synthetic approach, using a single heterogeneous solid source, for the continuous fabrication of lateral multi-junction heterostructures consisting of monolayers of transition-metal dichalcogenides. The sequential formation of heterojunctions is achieved solely by changing the composition of the reactive gas environment in the presence of water vapour. This enables selective control of the water-induced oxidation and volatilization of each transition-metal precursor, as well as its nucleation on the substrate, leading to sequential edge-epitaxy of distinct transition-metal dichalcogenides. Photoluminescence maps confirm the sequential spatial modulation of the bandgap, and atomic-resolution images reveal defect-free lateral connectivity between the different transition-metal-dichalcogenide domains within a single crystal structure. Electrical transport measurements revealed diode-like responses across the junctions. Our new approach offers greater flexibility and control than previous methods for continuous growth of transition-metal-dichalcogenide-based multi-junction lateral heterostructures. These findings could be extended to other families of two-dimensional materials, and establish a foundation for the development of complex and atomically thin in-plane superlattices, devices and integrated circuits.
DOE Office of Scientific and Technical Information (OSTI.GOV)
Szyszka, A., E-mail: szyszka@ihp-microelectronics.com, E-mail: adam.szyszka@pwr.wroc.pl; Faculty of Microsystem Electronics and Photonics, Wroclaw University of Technology, Janiszewskiego 11/17, 50-372 Wroclaw; Lupina, L.
2014-08-28
Based on a novel double step oxide buffer heterostructure approach for GaN integration on Si, we present an optimized Metal-Semiconductor-Metal (MSM)-based Ultraviolet (UV) GaN photodetector system with integrated short-period (oxide/Si) Distributed Bragg Reflector (DBR) and leakage suppressing Metal-Oxide-Semiconductor (MOS) electrode contacts. In terms of structural properties, it is demonstrated by in-situ reflection high energy electron diffraction and transmission electron microscopy-energy dispersive x-ray studies that the DBR heterostructure layers grow with high thickness homogeneity and sharp interface structures sufficient for UV applications; only minor Si diffusion into the Y{sub 2}O{sub 3} films is detected under the applied thermal growth budget. Asmore » revealed by comparative high resolution x-ray diffraction studies on GaN/oxide buffer/Si systems with and without DBR systems, the final GaN layer structure quality is not significantly influenced by the growth of the integrated DBR heterostructure. In terms of optoelectronic properties, it is demonstrated that—with respect to the basic GaN/oxide/Si system without DBR—the insertion of (a) the DBR heterostructures and (b) dark current suppressing MOS contacts enhances the photoresponsivity below the GaN band-gap related UV cut-off energy by almost up to two orders of magnitude. Given the in-situ oxide passivation capability of grown GaN surfaces and the one order of magnitude lower number of superlattice layers in case of higher refractive index contrast (oxide/Si) systems with respect to classical III-N DBR superlattices, virtual GaN substrates on Si via functional oxide buffer systems are thus a promising robust approach for future GaN-based UV detector technologies.« less
Generalized Ellipsometry on Complex Nanostructures and Low-Symmetry Materials
NASA Astrophysics Data System (ADS)
Mock, Alyssa Lynn
In this thesis, complex anisotropic materials are investigated and characterized by generalized ellipsometry. In recent years, anisotropic materials have gained considerable interest for novel applications in electronic and optoelectronic devices, mostly due to unique properties that originate from reduced crystal symmetry. Examples include white solid-state lighting devices which have become ubiquitous just recently, and the emergence of high-power, high-voltage electronic transistors and switches in all-electric vehicles. The incorporation of single crystalline material with low crystal symmetry into novel device structures requires reconsideration of existing optical characterization approaches. Here, the generalized ellipsometry concept is extended to include applications for materials with monoclinic and triclinic symmetries. A model eigendielectric displacement vector approach is developed, described and utilized to characterize monoclinic materials. Materials are investigated in spectral regions spanning from the far-infrared to the vacuum ultraviolet. Examples are demonstrated for phonon mode determination in cadmium tungstate and yttrium silicate and for band-to-band transitions in gallia (beta-Ga2O3) single crystals. Furthermore, the anisotropic optical properties of an emerging class of spatially coherent heterostructure materials with nanostructure dimensions are investigated. The so-called anisotropic effective medium approximation for slanted columnar thin films is extended to the concept of slanted columnar heterostructure thin films as well as core-shell heterostructure thin films. Examples include the determination of band-to-band transitions, phonon modes and oxidation properties of cobalt-oxide core shell structures and gas-liquid-solid distribution during controlled adsorption of organic solvents in silicon slanted columnar thin films.
DOE Office of Scientific and Technical Information (OSTI.GOV)
Thompson, J.; Nichols, J.; Connell, J. G.
2014-09-08
We have synthesized and investigated the heterointerfaces of KTaO{sub 3} (KTO) and GdScO{sub 3} (GSO), which are both polar complex-oxides along the pseudo-cubic [001] direction. Since their layers have the same, conflicting net charges at interfaces, i.e., KO(−1)/ScO{sub 2}(−1) or TaO{sub 2}(+1)/GdO(+1), forming the heterointerface of KTO/GSO should be forbidden due to strong Coulomb repulsion, the so-called polarity conflict. However, we have discovered that atomic reconstruction occurs at the heterointerfaces between KTO thin-films and GSO substrates, which effectively alleviates the polarity conflict without destroying the hetero-epitaxy. Our result demonstrates one of the important ways to create artificial heterostructures from polarmore » complex-oxides.« less
Charge transfer in rectifying oxide heterostructures and oxide access elements in ReRAM
DOE Office of Scientific and Technical Information (OSTI.GOV)
Stefanovich, G. B.; Pergament, A. L.; Boriskov, P. P.
2016-05-15
The main aspects of the synthesis and experimental research of oxide diode heterostructures are discussed with respect to their use as selector diodes, i.e., access elements in oxide resistive memory. It is shown that charge transfer in these materials differs significantly from the conduction mechanism in p–n junctions based on conventional semiconductors (Si, Ge, A{sup III}–B{sup V}), and the model should take into account the electronic properties of oxides, primarily the low carrier drift mobility. It is found that an increase in the forward current requires an oxide with a small band gap (<1.3 eV) in the heterostructure composition. Heterostructuresmore » with Zn, In–Zn (IZO), Ti, Ni, and Cu oxides are studied; it is found that the CuO–IZO heterojunction has the highest forward current density (10{sup 4} A/cm{sup 2}).« less
Baek, David J.; Lu, Di; Hikita, Yasuyuki; ...
2016-12-22
Incorporating oxides with radically different physical and chemical properties into heterostructures offers tantalizing possibilities to derive new functions and structures. Recently, we have fabricated freestanding 2D oxide membranes using the water-soluble perovskite Sr 3Al 2O 6 as a sacrificial buffer layer. Here, with atomic-resolution spectroscopic imaging, we observe that direct growth of oxide thin films on Sr 3Al 2O 6 can cause complete phase transformation of the buffer layer, rendering it water-insoluble. More importantly, we demonstrate that an ultrathin SrTiO 3 layer can be employed as an effective barrier to preserve Sr 3Al 2O 6 during subsequent growth, thus allowingmore » its integration in a wider range of oxide heterostructures.« less
Magnetocaloric effect in epitaxial La0.56Sr0.44MnO3 alloy and digital heterostructures
NASA Astrophysics Data System (ADS)
Belyea, Dustin D.; Santos, Tiffany S.; Miller, Casey W.
2012-04-01
This work investigates the magnetocaloric effect of two epitaxial manganite heterostructures, one being a single layer La0.56Sr0.44MnO3 alloy with randomly distributed La and Sr cations, the other a digitally synthesized superlattice of LaMnO3 and SrMnO3 fabricated to be compositionally identical to the alloy. The magnetic entropy change and relative cooling power were larger for the alloy than the superlattice, though both are suppressed relative to bulk materials. These results indicate that disorder of the A-site cation species in the perovskite structure may play a crucial role in defining the magnetocaloric effect in complex oxide materials.
NASA Technical Reports Server (NTRS)
Sieg, R. M.; Alterovitz, S. A.; Croke, E. T.; Harrell, M. J.; Tanner, M.; Wang, K. L.; Mena, R. A.; Young, P. G.
1993-01-01
Spectroscopic ellipsometry (SE) characterization of several complex Si (sub X)Ge (sub 1-x)/Si heterostructures prepared for device fabrication, including structures for heterojunction bipolar transistors (HBT), p-type and n-type heterostructure modulation doped field effect transistors, has been performed. We have shown that SE can simultaneously determine all active layer thicknesses, Si (sub X)Ge (sub 1-x) compositions, and the oxide overlayer thickness, with only a general knowledge of the structure topology needed a priori. The characterization of HBT material included the SE analysis of a Si (sub X)Ge (sub 1-x) layer deeply buried (600 nanometers) under the silicon emitter and cap layers. In the SE analysis of n-type heterostructures, we examined for the first time a silicon layer under tensile strain. We found that an excellent fit can be obtained using optical constants of unstrained silicon to represent the strained silicon conduction layer. We also used SE to measure lateral sample homogeneity, providing quantitative identification of the inhomogeneous layer. Surface overlayers resulting from prior sample processing were also detected and measured quantitatively. These results should allow SE to be used extensively as a non-destructive means of characterizing Si (sub X)Ge (sub 1-x)/Si heterostructures prior to device fabrication and testing.
On-stack two-dimensional conversion of MoS2 into MoO3
NASA Astrophysics Data System (ADS)
Yeoung Ko, Taeg; Jeong, Areum; Kim, Wontaek; Lee, Jinhwan; Kim, Youngchan; Lee, Jung Eun; Ryu, Gyeong Hee; Park, Kwanghee; Kim, Dogyeong; Lee, Zonghoon; Lee, Min Hyung; Lee, Changgu; Ryu, Sunmin
2017-03-01
Chemical transformation of existing two-dimensional (2D) materials can be crucial in further expanding the 2D crystal palette required to realize various functional heterostructures. In this work, we demonstrate a 2D ‘on-stack’ chemical conversion of single-layer crystalline MoS2 into MoO3 with a precise layer control that enables truly 2D MoO3 and MoO3/MoS2 heterostructures. To minimize perturbation of the 2D morphology, a nonthermal oxidation using O2 plasma was employed. The early stage of the reaction was characterized by a defect-induced Raman peak, drastic quenching of photoluminescence (PL) signals and sub-nm protrusions in atomic force microscopy images. As the reaction proceeded from the uppermost layer to the buried layers, PL and optical second harmonic generation signals showed characteristic modulations revealing a layer-by-layer conversion. The plasma-generated 2D oxides, confirmed as MoO3 by x-ray photoelectron spectroscopy, were found to be amorphous but extremely flat with a surface roughness of 0.18 nm, comparable to that of 1L MoS2. The rate of oxidation quantified by Raman spectroscopy decreased very rapidly for buried sulfide layers due to protection by the surface 2D oxides, exhibiting a pseudo-self-limiting behavior. As exemplified in this work, various on-stack chemical transformations can be applied to other 2D materials in forming otherwise unobtainable materials and complex heterostructures, thus expanding the palette of 2D material building blocks.
Liu, Yuan; Sheng, Jiming; Wu, Hao; He, Qiyuan; Cheng, Hung-Chieh; Shakir, Muhammad Imran; Huang, Yu; Duan, Xiangfeng
2016-06-01
Scalable fabrication of vertical-tunneling transistors is presented based on heterostructures formed between graphene, highly doped silicon, and its native oxide. Benefiting from the large density of states of highly doped silicon, the tunneling transistors can deliver a current density over 20 A cm(-2) . This study demonstrates that the interfacial native oxide plays a crucial role in governing the carrier transport in graphene-silicon heterostructures. © 2016 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.
Formation and characterization of Ta2O5/TaOx films formed by O ion implantation
NASA Astrophysics Data System (ADS)
Ruffell, S.; Kurunczi, P.; England, J.; Erokhin, Y.; Hautala, J.; Elliman, R. G.
2013-07-01
Ta2O5/TaOx (oxide/suboxide) heterostructures are fabricated by high fluence O ion-implantation into deposited Ta films. The resultant films are characterized by depth profiling X-ray photoelectron spectroscopy (XPS), cross-sectional transmission electron microscopy (XTEM), four-point probe, and current-voltage and capacitance-voltage measurements. The measurements show that Ta2O5/TaOx oxide/suboxide heterostructures can be fabricated with the relative thicknesses of the layers controlled by implantation energy and fluence. Electrical measurements show that this approach has promise for high volume manufacturing of resistive switching memory devices based on oxide/suboxide heterostructures.
Symmetry Mismatched Heterostructures: New Routes to Bandwidth Control in Oxides
2015-08-11
SECURITY CLASSIFICATION OF: This project aims to discover novel physical phenomena in correlated ABO3 oxide heterostructures by using interfacial...to properties at oxide interfaces, and provides insight into the length scale associated with interfacial 1. REPORT DATE (DD-MM-YYYY) 4. TITLE AND...in oxides The views, opinions and/or findings contained in this report are those of the author(s) and should not contrued as an official Department
Krausmann, Jan; Sanctis, Shawn; Engstler, Jörg; Luysberg, Martina; Bruns, Michael; Schneider, Jörg J
2018-06-20
The influence of the composition within multilayered heterostructure oxide semiconductors has a critical impact on the performance of thin-film transistor (TFT) devices. The heterostructures, comprising alternating polycrystalline indium oxide and zinc oxide layers, are fabricated by a facile atomic layer deposition (ALD) process, enabling the tuning of its electrical properties by precisely controlling the thickness of the individual layers. This subsequently results in enhanced TFT performance for the optimized stacked architecture after mild thermal annealing at temperatures as low as 200 °C. Superior transistor characteristics, resulting in an average field-effect mobility (μ sat. ) of 9.3 cm 2 V -1 s -1 ( W/ L = 500), an on/off ratio ( I on / I off ) of 5.3 × 10 9 , and a subthreshold swing of 162 mV dec -1 , combined with excellent long-term and bias stress stability are thus demonstrated. Moreover, the inherent semiconducting mechanism in such multilayered heterostructures can be conveniently tuned by controlling the thickness of the individual layers. Herein, devices comprising a higher In 2 O 3 /ZnO ratio, based on individual layer thicknesses, are predominantly governed by percolation conduction with temperature-independent charge carrier mobility. Careful adjustment of the individual oxide layer thicknesses in devices composed of stacked layers plays a vital role in the reduction of trap states, both interfacial and bulk, which consequently deteriorates the overall device performance. The findings enable an improved understanding of the correlation between TFT performance and the respective thin-film composition in ALD-based heterostructure oxides.
Wu, Wei; Zhang, Shaofeng; Ren, Feng; Xiao, Xiangheng; Zhou, Juan; Jiang, Changzhong
2011-11-01
Iron oxide/SnO(2) magnetic semiconductor core-shell heterostructures with high purity were synthesized by a low-cost, surfactant-free and environmentally friendly hydrothermal strategy via a seed-mediated method. The morphology and structure of the hybrid nanostructures were characterized by means of high-resolution transmission electron microscopy and X-ray diffraction. The morphology evolution investigations reveal that the Kirkendall effect directs the diffusion and causes the formation of iron oxide/SnO(2) quasi-hollow particles. Significantly, the as-obtained iron oxides/SnO(2) core-shell heterostructures exhibited enhanced visible light or UV photocatalytic abilities, remarkably superior to as-used α-Fe(2)O(3) seeds and commercial SnO(2) products, mainly owing to the effective electron hole separation at the iron oxides/SnO(2) interfaces.
NASA Astrophysics Data System (ADS)
Jia, S.; Sun, H. D.; Du, J. H.; Zhang, Z. K.; Zhang, D. D.; Ma, L. P.; Chen, J. S.; Ma, D. G.; Cheng, H. M.; Ren, W. C.
2016-05-01
The relatively high sheet resistance, low work function and poor compatibility with hole injection layers (HILs) seriously limit the applications of graphene as transparent conductive electrodes (TCEs) for organic light emitting diodes (OLEDs). Here, a graphene oxide/graphene (GO/G) vertical heterostructure is developed as TCEs for high-performance OLEDs, by directly oxidizing the top layer of three-layer graphene films with ozone treatment. Such GO/G heterostructure electrodes show greatly improved optical transmittance, a large work function, high stability, and good compatibility with HIL materials (MoO3 in this work). Moreover, the conductivity of the heterostructure is not sacrificed compared to the pristine three-layer graphene electrodes, but is significantly higher than that of pristine two-layer graphene films. In addition to high flexibility, OLEDs with different emission colors based on the GO/G heterostructure TCEs show much better performance than those based on indium tin oxide (ITO) anodes. Green OLEDs with GO/G heterostructure electrodes have the maximum current efficiency and power efficiency, as high as 82.0 cd A-1 and 98.2 lm W-1, respectively, which are 36.7% (14.8%) and 59.2% (15.0%) higher than those with pristine graphene (ITO) anodes. These findings open up the possibility of using graphene for next generation high-performance flexible and wearable optoelectronics with high stability.The relatively high sheet resistance, low work function and poor compatibility with hole injection layers (HILs) seriously limit the applications of graphene as transparent conductive electrodes (TCEs) for organic light emitting diodes (OLEDs). Here, a graphene oxide/graphene (GO/G) vertical heterostructure is developed as TCEs for high-performance OLEDs, by directly oxidizing the top layer of three-layer graphene films with ozone treatment. Such GO/G heterostructure electrodes show greatly improved optical transmittance, a large work function, high stability, and good compatibility with HIL materials (MoO3 in this work). Moreover, the conductivity of the heterostructure is not sacrificed compared to the pristine three-layer graphene electrodes, but is significantly higher than that of pristine two-layer graphene films. In addition to high flexibility, OLEDs with different emission colors based on the GO/G heterostructure TCEs show much better performance than those based on indium tin oxide (ITO) anodes. Green OLEDs with GO/G heterostructure electrodes have the maximum current efficiency and power efficiency, as high as 82.0 cd A-1 and 98.2 lm W-1, respectively, which are 36.7% (14.8%) and 59.2% (15.0%) higher than those with pristine graphene (ITO) anodes. These findings open up the possibility of using graphene for next generation high-performance flexible and wearable optoelectronics with high stability. Electronic supplementary information (ESI) available: XPS spectra, Raman spectra, sheet resistance and transmittance of graphene films with different numbers of layers and different ozone treatment times, doping effect of MoO3 on graphene and GO/G electrodes, performance of green OLEDs with different graphene anodes, a movie showing the flexibility of device. See DOI: 10.1039/c6nr01649a
A high density two-dimensional electron gas in an oxide heterostructure on Si (001)
NASA Astrophysics Data System (ADS)
Jin, E. N.; Kornblum, L.; Kumah, D. P.; Zou, K.; Broadbridge, C. C.; Ngai, J. H.; Ahn, C. H.; Walker, F. J.
2014-11-01
We present the growth and characterization of layered heterostructures comprised of LaTiO3 and SrTiO3 epitaxially grown on Si (001). Magnetotransport measurements show that the sheet carrier densities of the heterostructures scale with the number of LaTiO3/SrTiO3 interfaces, consistent with the presence of an interfacial 2-dimensional electron gas (2DEG) at each interface. Sheet carrier densities of 8.9 × 1014 cm-2 per interface are observed. Integration of such high density oxide 2DEGs on silicon provides a bridge between the exceptional properties and functionalities of oxide 2DEGs and microelectronic technologies.
Optically Tunable Resistive-Switching Memory in Multiferroic Heterostructures
NASA Astrophysics Data System (ADS)
Zheng, Ming; Ni, Hao; Xu, Xiaoke; Qi, Yaping; Li, Xiaomin; Gao, Ju
2018-04-01
Electronic phase separation has been used to realize exotic functionalities in complex oxides with external stimuli, such as magnetic field, electric field, current, light, strain, etc. Using the Nd0.7Sr0.3MnO3/0.7 Pb (Mg1 /3Nb2 /3)O3-0 .3 PbTiO3 multiferroic heterostructure as a model system, we investigate the electric field and light cocontrol of phase separation in resistive switching. The electric-field-induced nonvolatile electroresistance response is achieved at room temperature using reversible ferroelastic domain switching, which can be robustly modified on illumination of light. Moreover, the electrically controlled ferroelastic strain can effectively enhance the visible-light-induced photoresistance effect. These findings demonstrate that the electric-field- and light-induced effects strongly correlate with each other and are essentially driven by electronic phase separation. Our work opens a gate to design electrically tunable multifunctional storage devices based on multiferroic heterostructures by adding light as an extra control parameter.
NASA Astrophysics Data System (ADS)
Wu, Wei; Zhang, Shaofeng; Ren, Feng; Xiao, Xiangheng; Zhou, Juan; Jiang, Changzhong
2011-11-01
Iron oxide/SnO2 magnetic semiconductor core-shell heterostructures with high purity were synthesized by a low-cost, surfactant-free and environmentally friendly hydrothermal strategy via a seed-mediated method. The morphology and structure of the hybrid nanostructures were characterized by means of high-resolution transmission electron microscopy and X-ray diffraction. The morphology evolution investigations reveal that the Kirkendall effect directs the diffusion and causes the formation of iron oxide/SnO2 quasi-hollow particles. Significantly, the as-obtained iron oxides/SnO2 core-shell heterostructures exhibited enhanced visible light or UV photocatalytic abilities, remarkably superior to as-used α-Fe2O3 seeds and commercial SnO2 products, mainly owing to the effective electron hole separation at the iron oxides/SnO2 interfaces.Iron oxide/SnO2 magnetic semiconductor core-shell heterostructures with high purity were synthesized by a low-cost, surfactant-free and environmentally friendly hydrothermal strategy via a seed-mediated method. The morphology and structure of the hybrid nanostructures were characterized by means of high-resolution transmission electron microscopy and X-ray diffraction. The morphology evolution investigations reveal that the Kirkendall effect directs the diffusion and causes the formation of iron oxide/SnO2 quasi-hollow particles. Significantly, the as-obtained iron oxides/SnO2 core-shell heterostructures exhibited enhanced visible light or UV photocatalytic abilities, remarkably superior to as-used α-Fe2O3 seeds and commercial SnO2 products, mainly owing to the effective electron hole separation at the iron oxides/SnO2 interfaces. Electronic supplementary information (ESI) available: TEM and HRTEM images of hematite seeds and iron oxide/SnO2 (12 h and 36 h). See DOI: 10.1039/c1nr10728c
Insight into spin transport in oxide heterostructures from interface-resolved magnetic mapping
Bruno, F. Y.; Grisolia, M. N.; Visani, C.; ...
2015-02-17
At interfaces between complex oxides, electronic, orbital and magnetic reconstructions may produce states of matter absent from the materials involved, offering novel possibilities for electronic and spintronic devices. Here we show that magnetic reconstruction has a strong influence on the interfacial spin selectivity, a key parameter controlling spin transport in magnetic tunnel junctions. In epitaxial heterostructures combining layers of antiferromagnetic LaFeO 3 (LFO) and ferromagnetic La 0.7Sr 0.3MnO 3 (LSMO), we find that a net magnetic moment is induced in the first few unit planes of LFO near the interface with LSMO. Using X-ray photoemission electron microscopy, we show thatmore » the ferromagnetic domain structure of the manganite electrodes is imprinted into the antiferromagnetic tunnel barrier, endowing it with spin selectivity. Finally, we find that the spin arrangement resulting from coexisting ferromagnetic and antiferromagnetic interactions strongly influences the tunnel magnetoresistance of LSMO/LFO/LSMO junctions through competing spin-polarization and spin-filtering effects.« less
NASA Technical Reports Server (NTRS)
Zou, Yingyin Kevin (Inventor); Jiang, Hua (Inventor); Li, Kewen Kevin (Inventor); Guo, Xiaomei (Inventor)
2012-01-01
A heterostructure of multiferroics or magnetoelectrics (ME) was disclosed. The film has both ferromagnetic and ferroelectric properties, as well as magneto-optic (MO) and electro-optic (EO) properties. Oxide buffer layers were employed to allow grown a cracking-free heterostructure a solution coating method.
Prajapat, C L; Singh, Surendra; Paul, Amitesh; Bhattacharya, D; Singh, M R; Mattauch, S; Ravikumar, G; Basu, S
2016-05-21
Coupling between superconducting and ferromagnetic states in hybrid oxide heterostructures is presently a topic of intense research. Such a coupling is due to the leakage of the Cooper pairs into the ferromagnet. However, tunneling of the Cooper pairs though an insulator was never considered plausible. Using depth sensitive polarized neutron reflectivity we demonstrate the coupling between superconductor and magnetic layers in epitaxial La2/3Ca1/3MnO3 (LCMO)/SrTiO3/YBa2Cu3O7-δ (YBCO) hybrid heterostructures, with SrTiO3 as an intervening oxide insulator layer between the ferromagnet and the superconductor. Measurements above and below the superconducting transition temperature (TSC) of YBCO demonstrate a large modulation of magnetization in the ferromagnetic layer below the TSC of YBCO in these heterostructures. This work highlights a unique tunneling phenomenon between the epitaxial layers of an oxide superconductor (YBCO) and a magnetic layer (LCMO) through an insulating layer. Our work would inspire further investigations on the fundamental aspect of a long range order of the triplet spin-pairing in hybrid structures.
Interface-engineered oxygen octahedral coupling in manganite heterostructures
NASA Astrophysics Data System (ADS)
Huijben, M.; Koster, G.; Liao, Z. L.; Rijnders, G.
2017-12-01
Control of the oxygen octahedral coupling (OOC) provides a large degree of freedom to manipulate physical phenomena in complex oxide heterostructures. Recently, local tuning of the tilt angle has been found to control the magnetic anisotropy in ultrathin films of manganites and ruthenates, while symmetry control can manipulate the metal insulator transition in nickelate thin films. The required connectivity of the octahedra across the heterostructure interface enforces a geometric constraint to the 3-dimensional octahedral network in epitaxial films. Such geometric constraint will either change the tilt angle to retain the connectivity of the corner shared oxygen octahedral network or guide the formation of a specific symmetry throughout the epitaxial film. Here, we will discuss the control of OOC in manganite heterostructures by interface-engineering. OOC driven magnetic and transport anisotropies have been realized in LSMO/NGO heterostructures. Competition between the interfacial OOC and the strain further away from the interface leads to a thickness driven sharp transition of the anisotropic properties. Furthermore, octahedral relaxation leading to a change of p-d hybridization driven by interfacial OOC appears to be the strongest factor in thickness related variations of magnetic and transport properties in epitaxial LSMO films on NGO substrates. The results unequivocally link the atomic structure near the interfaces to the macroscopic properties. The strong correlation between a controllable oxygen network and the functionalities will have significant impact on both fundamental research and technological application of correlated perovskite heterostructures. By controlling the interfacial OOC, it is possible to pattern in 3 dimensions the magnetization to achieve non-collinear magnetization in both in-plane and out of plane directions, thus making the heterostructures promising for application in orthogonal spin transfer devices, spin oscillators, and low field sensors.
Herklotz, A.; Dörr, Kathrin; Ward, T. Z.; ...
2015-04-03
In this paper, to have precise atomic layer control over interfaces, we examine the growth of complex oxides through the sequential deposition from binary targets by pulsed laser deposition. In situ reflection high-energy electron diffraction (RHEED) is used to control the growth and achieve films with excellent structural quality. The growth from binary oxide targets is fundamentally different from single target growth modes and shows more similarities to shuttered growth by molecular beam epitaxy. The RHEED intensity oscillations of non-stoichiometric growth are consistent with a model of island growth and accumulation of excess material on the surface that can bemore » utilized to determine the correct stoichiometry for growth. Correct monolayer doses can be determined through an envelope frequency in the RHEED intensity oscillations. In order to demonstrate the ability of this growth technique to create complex heterostructures, the artificial n = 2 and 3 Sr n +1Ti n O 3 n +1 Ruddlesden-Popper phases are grown with good long-range order. Finally, this method enables the precise unit-cell level control over the structure of perovskite-type oxides, and thus the growth of complex materials with improved structural quality and electronic functionality.« less
Herklotz, Andreas; Dorr, Kathrin; Ward, Thomas Zac; ...
2015-04-03
To have precise atomic layer control over interfaces, we examine the growth of complex oxides through the sequential deposition from binary targets by pulsed laser deposition. In situ reflection high-energy electron diffraction (RHEED) is used to control the growth and achieve films with excellent structural quality. The growth from binary oxide targets is fundamentally different from single target growth modes and shows more similarities to shuttered growth by molecular beam epitaxy. The RHEED intensity oscillations of non-stoichiometric growth are consistent with a model of island growth and accumulation of excess material on the surface that can be utilized to determinemore » the correct stoichiometry for growth. Correct monolayer doses can be determined through an envelope frequency in the RHEED intensity oscillations. In order to demonstrate the ability of this growth technique to create complex heterostructures, the artificial n = 2 and 3 Sr n+1Ti nO 3 n+1 Ruddlesden-Popper phases are grown with good long-range order. Furthermore, this method enables the precise unit-cell level control over the structure of perovskite-type oxides, and thus the growth of complex materials with improved structural quality and electronic functionality.« less
Perspective: Oxide molecular-beam epitaxy rocks!
DOE Office of Scientific and Technical Information (OSTI.GOV)
Schlom, Darrell G., E-mail: schlom@cornell.edu
2015-06-01
Molecular-beam epitaxy (MBE) is the “gold standard” synthesis technique for preparing semiconductor heterostructures with high purity, high mobility, and exquisite control of layer thickness at the atomic-layer level. Its use for the growth of multicomponent oxides got off to a rocky start 30 yr ago, but in the ensuing decades, it has become the definitive method for the preparation of oxide heterostructures too, particularly when it is desired to explore their intrinsic properties. Examples illustrating the unparalleled achievements of oxide MBE are given; these motivate its expanding use for exploring the potentially revolutionary states of matter possessed by oxide systems.
Zinc-oxide-based nanostructured materials for heterostructure solar cells
DOE Office of Scientific and Technical Information (OSTI.GOV)
Bobkov, A. A.; Maximov, A. I.; Moshnikov, V. A., E-mail: vamoshnikov@mail.ru
Results obtained in the deposition of nanostructured zinc-oxide layers by hydrothermal synthesis as the basic method are presented. The possibility of controlling the structure and morphology of the layers is demonstrated. The important role of the procedure employed to form the nucleating layer is noted. The faceted hexagonal nanoprisms obtained are promising for the fabrication of solar cells based on oxide heterostructures, and aluminum-doped zinc-oxide layers with petal morphology, for the deposition of an antireflection layer. The results are compatible and promising for application in flexible electronics.
Towards precise defect control in layered oxide structures by using oxide molecular beam epitaxy
Baiutti, Federico; Christiani, Georg
2014-01-01
Summary In this paper we present the atomic-layer-by-layer oxide molecular beam epitaxy (ALL-oxide MBE) which has been recently installed in the Max-Planck Institute for Solid State Research and we report on its present status, providing some examples that demonstrate its successful application in the synthesis of different layered oxides, with particular reference to superconducting La2CuO4 and insulator-to-metal La2− xSrxNiO4. We briefly review the ALL-oxide MBE technique and its unique capabilities in the deposition of atomically smooth single-crystal thin films of various complex oxides, artificial compounds and heterostructures, introducing our goal of pursuing a deep investigation of such systems with particular emphasis on structural defects, with the aim of tailoring their functional properties by precise defects control. PMID:24995148
Reactive metal-oxide interfaces: A microscopic view
NASA Astrophysics Data System (ADS)
Picone, A.; Riva, M.; Brambilla, A.; Calloni, A.; Bussetti, G.; Finazzi, M.; Ciccacci, F.; Duò, L.
2016-03-01
Metal-oxide interfaces play a fundamental role in determining the functional properties of artificial layered heterostructures, which are at the root of present and future technological applications. Magnetic exchange and magnetoelectric coupling, spin filtering, metal passivation, catalytic activity of oxide-supported nano-particles are just few examples of physical and chemical processes arising at metal-oxide hybrid systems, readily exploited in working devices. These phenomena are strictly correlated with the chemical and structural characteristics of the metal-oxide interfacial region, making a thorough understanding of the atomistic mechanisms responsible of its formation a prerequisite in order to tailor the device properties. The steep compositional gradient established upon formation of metal-oxide heterostructures drives strong chemical interactions at the interface, making the metal-oxide boundary region a complex system to treat, both from an experimental and a theoretical point of view. However, once properly mastered, interfacial chemical interactions offer a further degree of freedom for tuning the material properties. The goal of the present review is to provide a summary of the latest achievements in the understanding of metal/oxide and oxide/metal layered systems characterized by reactive interfaces. The influence of the interface composition on the structural, electronic and magnetic properties will be highlighted. Particular emphasis will be devoted to the discussion of ultra-thin epitaxial oxides stabilized on highly oxidizable metals, which have been rarely exploited as oxide supports as compared to the much more widespread noble and quasi noble metallic substrates. In this frame, an extensive discussion is devoted to the microscopic characterization of interfaces between epitaxial metal oxides and the Fe(001) substrate, regarded from the one hand as a prototypical ferromagnetic material and from the other hand as a highly oxidizable metal.
Hsu, Chih-Hung; Chen, Lung-Chien; Lin, Yi-Feng
2013-01-01
This study reports the optoelectronic characteristics of ZnO/GaP buffer/CuO-Cu2O complex (COC) inverse heterostructure for solar cell applications. The GaP and COC layers were used as buffer and absorber in the cell structure, respectively. An energy gap widening effect and CuO whiskers were observed as the copper (Cu) layer was exerted under heat treatment for oxidation at 500 °C for 10 min, and arose from the center of the Cu2O rods. For preparation of the 30 nm-thick GaP buffer by sputtering from GaP target, as the nitrogen gas flow rate increased from 0 to 2 sccm, the transmittance edge of the spectra demonstrated a blueshift form 2.24 to 3.25 eV. Therefore, the layer can be either GaP, GaNP, or GaN by changing the flow rate of nitrogen gas. PMID:28788341
DOE Office of Scientific and Technical Information (OSTI.GOV)
Feng, Zhenxing; Yacoby, Yuzhak; Gadre, Milind
2014-01-01
Heterostructured materials have shown unusual physiochemical properties at the interfaces such as two dimensional electron gas systems, high-temperature superconductivity, and enhanced catalysis. Here we report the first atomic-scale evidence of the microscopic structure of a perovskite/Ruddlesden-Popper heterostructure (having La1-xSrxCoO3- /(La1-ySry)2CoO4 ), and anomalous strontium segregation at the interface and in the Ruddlesden-Popper structure using direct X-ray methods combined with ab initio calculations. The remarkably enhanced activity of such heterostructured surfaces relative to bulk perovskite and Ruddlesden-Popper oxides previously shown for oxygen electrocatalysis at elevated temperatures can be attributed to reduced thermodynamic penalty of oxygen vacancies in the oxide structure associatedmore » with Sr segregation observed in the heterostructure. Our findings provide insights for the design of highly active catalysts for energy conversion and storage applications.« less
NASA Astrophysics Data System (ADS)
Chen, Fayun; Zhang, Laijun; Wang, Xuewen; Zhang, Rongbin
2017-11-01
Noble-metal-free semiconductor materials are widely used for photocatalytic hydrogen generation because of their low cost. ZnO-based heterostructures with synergistic effects exhibit an effective photocatalytic activity. In this work, NiO@Ni-ZnO/reduced graphene oxide (rGO)/CdS heterostructures are synthesized by a multi-step method. rGO nanosheets and CdS nanoparticles were introduced into the heterostructures via a redox reaction and light-assisted growth, respectively. A novel Ni-induced electrochemical growth method was developed to prepare ZnO rods from Zn powder. NiO@Ni-ZnO/rGO/CdS heterostructures with a wide visible-light absorption range exhibited highly photocatalytic hydrogen generation rates under UV-vis and visible light irradiation. The enhanced photocatalytic activity is attributed to the Ni nanoparticles that act as cocatalysts for capturing photoexcited electrons and the improved synergistic effect between ZnO and CdS due to the rGO nanosheets acting as photoexcited carrier transport channels.
Conducting LaAlO3/SrTiO3 heterointerfaces on atomically-flat substrates prepared by deionized-water
Connell, J. G.; Nichols, J.; Gruenewald, J. H.; Kim, D.-W.; Seo, S. S. A.
2016-01-01
We have investigated how the recently-developed water-leaching method for atomically-flat SrTiO3 (STO) substrates affects the transport properties of LaAlO3 (LAO) and STO heterointerfaces. Using pulsed laser deposition at identical growth conditions, we have synthesized epitaxial LAO thin-films on two different STO substrates, which are prepared by water-leaching and buffered hydrofluoric acid (BHF) etching methods. The structural, transport, and optical properties of LAO/STO heterostructures grown on water-leached substrates show the same high-quality as the samples grown on BHF-etched substrates. These results indicate that the water-leaching method can be used to grow complex oxide heterostructures with atomically well-defined heterointerfaces without safety concerns. PMID:27033248
NASA Astrophysics Data System (ADS)
Bjørlig, Anders V.; von Soosten, Merlin; Erlandsen, Ricci; Dahm, Rasmus Tindal; Zhang, Yu; Gan, Yulin; Chen, Yunzhong; Pryds, Nini; Jespersen, Thomas S.
2018-04-01
A simple approach is presented for designing complex oxide mesoscopic electronic devices based on the conducting interfaces of room temperature grown LaAlO3/SrTiO3 heterostructures. The technique is based entirely on methods known from conventional semiconductor processing technology, and we demonstrate a lateral resolution of ˜100 nm. We study the low temperature transport properties of nanoscale wires and demonstrate the feasibility of the technique for defining in-plane gates allowing local control of the electrostatic environment in mesoscopic devices.
Thermal oxidation of Si/SiGe heterostructures for use in quantum dot qubits
NASA Astrophysics Data System (ADS)
Neyens, Samuel F.; Foote, Ryan H.; Knapp, T. J.; McJunkin, Thomas; Savage, D. E.; Lagally, M. G.; Coppersmith, S. N.; Eriksson, M. A.
Here we demonstrate dry thermal oxidation of a Si/SiGe heterostructure at 700°C and use a Hall bar device to measure the mobility after oxidation to be 43,000 cm2V-1s-1 at a carrier density of 4.1 ×1011 cm-2. Surprisingly, we find no significant reduction in mobility compared with an Al2O3 device made with atomic layer deposition on the same heterostructure, indicating thermal oxidation can be used to process Si/SiGe quantum dot devices. This result provides a path for investigating improvements to the gate oxide in Si/SiGe qubit devices, whose performance is believed to be limited by charge noise in the oxide layer. This work was supported in part by ARO (W911NF-12-0607) and NSF (DMR-1206915 and PHY-1104660). Development and maintenance of the growth facilities used for fabricating samples is supported by DOE (DE-FG02-03ER46028). This research utilized NSF-supported shared facilities at the University of Wisconsin-Madison.
Optimising the visibility of graphene and graphene oxide on gold with multilayer heterostructures
NASA Astrophysics Data System (ADS)
Velický, Matěj; Hendren, William R.; Donnelly, Gavin E.; Katzen, Joel M.; Bowman, Robert M.; Huang, Fumin
2018-07-01
Metals have been increasingly used as substrates in devices based on two-dimensional (2D) materials. However, the high reflectivity of bulk metals results in low optical contrast (<3%) and therefore poor visibility of transparent mono- and few-layer 2D materials on these surfaces. Here we demonstrate that by engineering the complex reflectivity of a purpose-designed multilayer heterostructure composed of thin Au films (2–8 nm) on SiO2/Si substrate, the optical contrast of graphene and graphene oxide (GO) can be significantly enhanced in comparison to bulk Au, up to about 3 and 5 times, respectively. In particular, we achieved ∼17% optical contrast for monolayer GO, which is even 2 times higher than that on bare SiO2/Si substrate. The experimental results are in good agreement with theoretical simulations. This concept is demonstrated for Au, but the methodology is applicable to other metals and can be adopted to design a variety of high-contrast metallic substrates. This will facilitate research and applications of 2D materials in areas such as plasmonics, photonics, catalysis and sensors.
Nano suboxide layer generated in Ta{sub 2}O{sub 5} by Ar{sup +} ion irradiation
DOE Office of Scientific and Technical Information (OSTI.GOV)
Song, W. D., E-mail: song-wendong@dsi.a-star.edu.sg, E-mail: ying-ji-feng@dsi.a-star.edu.sg; Ying, J. F., E-mail: song-wendong@dsi.a-star.edu.sg, E-mail: ying-ji-feng@dsi.a-star.edu.sg; He, W.
2015-01-19
Ta{sub 2}O{sub 5}/TaO{sub x} heterostructure has become a leading oxide layer in memory cells and/or a bidirectional selector for resistive random access memory (RRAM). Although atomic layer deposition (ALD) was found to be uniquely suitable for depositing uniform and conformal films on complex topographies, it is hard to use ALD to grow suboxide TaO{sub x} layer. In this study, tantalum oxide films with a composition of Ta{sub 2}O{sub 5} were grown by ALD. Using Ar{sup +} ion irradiation, the suboxide was formed in the top layer of Ta{sub 2}O{sub 5} films by observing the Ta core level shift toward lowermore » binding energy with angle-resolved X-ray photoelectron spectroscopy. By controlling the energy and irradiation time of an Ar{sup +} ion beam, Ta{sub 2}O{sub 5}/TaO{sub x} heterostructure can be reliably produced on ALD films, which provides a way to fabricate the critical switching layers of RRAM.« less
Optimising the visibility of graphene and graphene oxide on gold with multilayer heterostructures.
Velický, Matěj; Hendren, William R; Donnelly, Gavin E; Katzen, Joel M; Bowman, Robert M; Huang, Fumin
2018-07-06
Metals have been increasingly used as substrates in devices based on two-dimensional (2D) materials. However, the high reflectivity of bulk metals results in low optical contrast (<3%) and therefore poor visibility of transparent mono- and few-layer 2D materials on these surfaces. Here we demonstrate that by engineering the complex reflectivity of a purpose-designed multilayer heterostructure composed of thin Au films (2-8 nm) on SiO 2 /Si substrate, the optical contrast of graphene and graphene oxide (GO) can be significantly enhanced in comparison to bulk Au, up to about 3 and 5 times, respectively. In particular, we achieved ∼17% optical contrast for monolayer GO, which is even 2 times higher than that on bare SiO 2 /Si substrate. The experimental results are in good agreement with theoretical simulations. This concept is demonstrated for Au, but the methodology is applicable to other metals and can be adopted to design a variety of high-contrast metallic substrates. This will facilitate research and applications of 2D materials in areas such as plasmonics, photonics, catalysis and sensors.
NASA Astrophysics Data System (ADS)
Subramanyam, Guru; Cole, M. W.; Sun, Nian X.; Kalkur, Thottam S.; Sbrockey, Nick M.; Tompa, Gary S.; Guo, Xiaomei; Chen, Chonglin; Alpay, S. P.; Rossetti, G. A.; Dayal, Kaushik; Chen, Long-Qing; Schlom, Darrell G.
2013-11-01
There has been significant progress on the fundamental science and technological applications of complex oxides and multiferroics. Among complex oxide thin films, barium strontium titanate (BST) has become the material of choice for room-temperature-based voltage-tunable dielectric thin films, due to its large dielectric tunability and low microwave loss at room temperature. BST thin film varactor technology based reconfigurable radio frequency (RF)/microwave components have been demonstrated with the potential to lower the size, weight, and power needs of a future generation of communication and radar systems. Low-power multiferroic devices have also been recently demonstrated. Strong magneto-electric coupling has also been demonstrated in different multiferroic heterostructures, which show giant voltage control of the ferromagnetic resonance frequency of more than two octaves. This manuscript reviews recent advances in the processing, and application development for the complex oxides and multiferroics, with the focus on voltage tunable RF/microwave components. The over-arching goal of this review is to provide a synopsis of the current state-of the-art of complex oxide and multiferroic thin film materials and devices, identify technical issues and technical challenges that need to be overcome for successful insertion of the technology for both military and commercial applications, and provide mitigation strategies to address these technical challenges.
NASA Astrophysics Data System (ADS)
Fadley, Charles
2015-03-01
It is clear that interfaces in complex oxide heterostructures often represent emergent materials that possess surprising properties not associated with the parent oxides, such as two-dimensional electron gases (2DEGs), superconductivity, and magnetism. A detailed knowledge of the composition, atomic structure, and electronic structure through such interfaces is thus critical. Photomission (PES) and angle-resolved photoemission (ARPES) represent techniques of choice for such studies, but have certain limitations in being too surface sensitive and in not being able to focus specifically on buried interfaces or heterostructure layers. In this talk, I will discuss combining two newer elements of PES/ARPES to deal with this challenge: - the use of soft x-rays in the ca. few hundred-to-2000 eV regime, or even into the true hard x-ray regime, to probe more deeply into the structure, and - tailoring of the x-ray intensity profile into a strong standing wave (SW) through reflection from a multilayer heterostructure to provide much enhanced depth resolution. The relative advantages of soft/hard x-ray PES and ARPES and their complementarity to conventional VUV ARPES in the ca. 5-150 eV regime will be considered. As illustrative examples, by combining SW-PES and SW-ARPES, it has been possible to measure for the first time the detailed concentration profiles and momentum-resolved electronic structure at the SrTiO3/La0.67Sr0.33MnO3 interface and to directly measure the depth profile of the 2DEG at SrTiO3/GdTiO3 interfaces. Future directions for such measurements will also be discussed. Supported by US DOE Contract No. DE-AC02-05CH11231, ARO-MURI Grant W911-NF-09-1-0398, and the PALM-APTCOM Project (France).
Pure electronic metal-insulator transition at the interface of complex oxides
Meyers, D.; Liu, Jian; Freeland, J. W.; ...
2016-06-21
We observed complex materials in electronic phases and transitions between them often involve coupling between many degrees of freedom whose entanglement convolutes understanding of the instigating mechanism. Metal-insulator transitions are one such problem where coupling to the structural, orbital, charge, and magnetic order parameters frequently obscures the underlying physics. We demonstrate a way to unravel this conundrum by heterostructuring a prototypical multi-ordered complex oxide NdNiO3 in ultra thin geometry, which preserves the metal-to-insulator transition and bulk-like magnetic order parameter, but entirely suppresses the symmetry lowering and long-range charge order parameter. Furthermore, these findings illustrate the utility of heterointerfaces as amore » powerful method for removing competing order parameters to gain greater insight into the nature of the transition, here revealing that the magnetic order generates the transition independently, leading to an exceptionally rare purely electronic metal-insulator transition with no symmetry change.« less
Fabrication of Coaxial Si1−xGex Heterostructure Nanowires by O2 Flow-Induced Bifurcate Reactions
2010-01-01
We report on bifurcate reactions on the surface of well-aligned Si1−xGex nanowires that enable fabrication of two different coaxial heterostructure nanowires. The Si1−xGex nanowires were grown in a chemical vapor transport process using SiCl4 gas and Ge powder as a source. After the growth of nanowires, SiCl4 flow was terminated while O2 gas flow was introduced under vacuum. On the surface of nanowires was deposited Ge by the vapor from the Ge powder or oxidized into SiO2 by the O2 gas. The transition from deposition to oxidation occurred abruptly at 2 torr of O2 pressure without any intermediate region and enables selectively fabricated Ge/Si1−xGex or SiO2/Si1−xGex coaxial heterostructure nanowires. The rate of deposition and oxidation was dominated by interfacial reaction and diffusion of oxygen through the oxide layer, respectively. PMID:21076699
Fabrication of Coaxial Si1- x Ge x Heterostructure Nanowires by O2 Flow-Induced Bifurcate Reactions
NASA Astrophysics Data System (ADS)
Kim, Ilsoo; Lee, Ki-Young; Kim, Ungkil; Park, Yong-Hee; Park, Tae-Eon; Choi, Heon-Jin
2010-10-01
We report on bifurcate reactions on the surface of well-aligned Si1- x Ge x nanowires that enable fabrication of two different coaxial heterostructure nanowires. The Si1- x Ge x nanowires were grown in a chemical vapor transport process using SiCl4 gas and Ge powder as a source. After the growth of nanowires, SiCl4 flow was terminated while O2 gas flow was introduced under vacuum. On the surface of nanowires was deposited Ge by the vapor from the Ge powder or oxidized into SiO2 by the O2 gas. The transition from deposition to oxidation occurred abruptly at 2 torr of O2 pressure without any intermediate region and enables selectively fabricated Ge/Si1- x Ge x or SiO2/Si1- x Ge x coaxial heterostructure nanowires. The rate of deposition and oxidation was dominated by interfacial reaction and diffusion of oxygen through the oxide layer, respectively.
Kim, Ilsoo; Lee, Ki-Young; Kim, Ungkil; Park, Yong-Hee; Park, Tae-Eon; Choi, Heon-Jin
2010-06-17
We report on bifurcate reactions on the surface of well-aligned Si(1-x)Ge(x) nanowires that enable fabrication of two different coaxial heterostructure nanowires. The Si(1-x)Ge(x) nanowires were grown in a chemical vapor transport process using SiCl(4) gas and Ge powder as a source. After the growth of nanowires, SiCl(4) flow was terminated while O(2) gas flow was introduced under vacuum. On the surface of nanowires was deposited Ge by the vapor from the Ge powder or oxidized into SiO(2) by the O(2) gas. The transition from deposition to oxidation occurred abruptly at 2 torr of O(2) pressure without any intermediate region and enables selectively fabricated Ge/Si(1-x)Ge(x) or SiO(2)/Si(1-x)Ge(x) coaxial heterostructure nanowires. The rate of deposition and oxidation was dominated by interfacial reaction and diffusion of oxygen through the oxide layer, respectively.
NASA Astrophysics Data System (ADS)
Min, Jie; Wang, Kangyan; Liu, Jun; Yao, Yang; Wang, Wenjun; Yang, Linyu; Zhang, Ruizhi; Lei, Ming
2017-09-01
Uniform nano/micro-spherical MoO2/Mo2CTx (T = O) heterostructures have been synthesized through a heterocatalytic reaction with subsequent facile calcinations. Given the high activity of HxMoO3/C precursors, this strategy opens a low-temperature route to realize the fabrication of nanocrystalline MoO2/Mo2CTx heterostructures, leading to achieve rapidly activated conversion reaction and extrinsic pseudocapacitive behaviour. Rather than carbon, highly conductive Mo2CTx decreases the charge transfer resistance in MoO2 and maintains its structural stability upon lithiation/delithiation, ensuring the heterostructures with excellent cyclability (e.g., up to 833 mA h g-1 at 100 mA g-1 for 160 cycles with 95% capacity retention) and high rate capability (e.g., 665 mA h g-1 at 1 A g-1). Additionally, owing to the carbon-free characteristic, the secondary nano/microstructure feature and the suppressed surface oxidation trait, MoO2/Mo2CTx heterostructures, therefore, can deliver an improved initial Coulombic efficiency (e.g., up to 78% at 100 mA g-1). The present oxycarbide transformation and hybridization strategies are facile but effective, and they are very promising to be applied to converting other oxides-carbon composites into oxides/carbides heterostructures towards achieving higher electrochemical performance.
Antiferroelectric Materials, Applications and Recent Progress on Multiferroic Heterostructures
NASA Astrophysics Data System (ADS)
Zhou, Ziyao; Yang, Qu; Liu, Ming; Zhang, Zhiguo; Zhang, Xinyang; Sun, Dazhi; Nan, Tianxiang; Sun, Nianxiang; Chen, Xing
2015-04-01
Antiferroelectric (AFE) materials with adjacent dipoles oriented in antiparallel directions have a double polarization hysteresis loops. An electric field (E-field)-induced AFE-ferroelectric (FE) phase transition takes place in such materials, leading to a large lattice strain and energy change. The high dielectric constant and the distinct phase transition in AFE materials provide great opportunities for the realization of energy storage devices like super-capacitors and energy conversion devices such as AFE MEMS applications. Lots of work has been done in this field since 60-70 s. Recently, the strain tuning of the spin, charge and orbital orderings and their interactions in complex oxides and multiferroic heterostructures have received great attention. In these systems, a single control parameter of lattice strain is used to control lattice-spin, lattice-phonon, and lattice-charge interactions and tailor properties or create a transition between distinct magnetic/electronic phases. Due to the large strain/stress arising from the phase transition, AFE materials are great candidates for integrating with ferromagnetic (FM) materials to realize in situ manipulation of magnetism and lattice-ordered parameters by voltage. In this paper, we introduce the AFE material and it's applications shortly and then review the recent progress in AFEs based on multiferroic heterostructures. These new multiferroic materials could pave a new way towards next generation light, compact, fast and energy efficient voltage tunable RF/microwave, spintronic and memory devices promising approaches to in situ manipulation of lattice-coupled order parameters is to grow epitaxial oxide films on FE/ferroelastic substrates.
Enhancement of SOFC Cathode Electrochemical Performance Using Multi-Phase Interfaces
DOE Office of Scientific and Technical Information (OSTI.GOV)
Morgan, Dane
2015-09-30
This work explored the use of oxide heterostructures for enhancing the catalytic and degradation properties of solid oxide fuel cell (SOFC) cathode electrodes. We focused on heterostructures of Ruddlesden-Popper and perovskite phases. Building on previous work showing enhancement of the Ruddlesden-Popper (La,Sr) 2CoO 4 / perovskite (La,Sr)CoO 3 heterostructure compared to pure (La,Sr)CoO 3 we explored the application of related heterostructures of Ruddlesden-Popper phases on perovskite (La,Sr)(Co,Fe)O 3. Our approaches included thin-film electrodes, physical and electrochemical characterization, elementary reaction kinetics modeling, and ab initio simulations. We demonstrated that Sr segregation to surfaces is likely playing a critical role in themore » performance of (La,Sr)CoO 3 and (La,Sr)(Co,Fe)O 3 and that modification of this Sr segregation may be the mechanism by which Ruddlesden-Popper coatings enhance performances. We determined that (La,Sr)(Co,Fe)O 3 could be enhanced in thin films by about 10× by forming a heterostructure simultaneously with (La,Sr) 2CoO 4 and (La,Sr)CoO 3. We hope that future work will develop this heterostructure for use as a bulk porous electrode.« less
DOE Office of Scientific and Technical Information (OSTI.GOV)
Veal, Boyd W.; Kim, Seong Keun; Zapol, Peter
2016-06-10
Oxygen vacancies in proximity to surfaces and heterointerfaces in oxide thin film heterostructures have major effects on properties, resulting, for example, in emergent conduction behaviour, large changes in metal-insulator transition temperatures or enhanced catalytic activity. Here we report the discovery of a means of reversibly controlling the oxygen vacancy concentration and distribution in oxide heterostructures consisting of electronically conducting In2O3 films grown on ionically conducting Y2O3-stabilized ZrO2 substrates. Oxygen ion redistribution across the heterointerface is induced using an applied electric field oriented in the plane of the interface, resulting in controlled oxygen vacancy (and hence electron) doping of the filmmore » and possible orders-of-magnitude enhancement of the film's electrical conduction. The reversible modified behaviour is dependent on interface properties and is attained without cation doping or changes in the gas environment.« less
Veal, Boyd W.; Kim, Seong Keun; Zapol, Peter; ...
2016-06-10
Oxygen vacancies in proximity to surfaces and heterointerfaces in oxide thin film heterostructures have major effects on properties, resulting, for example, in emergent conduction behavior, large changes in metal-insulator transition temperatures, or enhanced catalytic activity. Here in this paper, we report the discovery of a means of reversibly controlling the oxygen vacancy concentration and distribution in oxide heterostructures consisting of electronically conducting In 2O 3 films grown on ionically conducting Y 2O 3-stabilized ZrO 2 substrates. Oxygen ion redistribution across the heterointerface is induced using an applied electric field oriented in the plane of the interface, resulting in controlled oxygenmore » vacancy (and hence electron) doping of the film and possible orders-of-magnitude enhancement of the film's electrical conduction. The reversible modified behavior is dependent on interface properties and is attained without cation doping or changes in the gas environment.« less
NASA Astrophysics Data System (ADS)
Tronganh, Nguyen; Gao, Yang; Jiang, Wei; Tao, Haihua; Wang, Shanshan; Zhao, Bing; Jiang, Yong; Chen, Zhiwen; Jiao, Zheng
2018-05-01
Constructing heterostructure can endow composites with many novel physical and electrochemical properties due to the built-in specific charge transfer dynamics. However, controllable fabrication route to heterostructures is still a great challenge up to now. In this work, a SiO2-assisted hydrothermal method is developed to fabricate heterostructured nickel sulfides/reduced graphene oxide (NiSx/rGO) composite. The SiO2 particles hydrolyzed from tetraethyl orthosilicate could assist the surface controllable co-growth of 3D nanoflowers and 0D nanoparticles of Ni3S2/NiS decorated on reduced graphene oxide, and the possible co-growth mechanism is discussed in detail. In this composite, the heterostructured nanocomposite with different morphologies, chemical compositions and crystal structures, along with varied electronic states and band structure, can promote the interface charge transfer kinetics and lead to excellent lithium storage performances. Electrochemical measurements reveal that the NiSx/rGO composite presents 1187.0 mA h g-1 at 100 mA g-1 and achieves a highly stable capacity of 561.2 mA h g-1 even when the current density is up to 5 A g-1.
Wu, Wei; Zhang, Shaofeng; Xiao, Xiangheng; Zhou, Juan; Ren, Feng; Sun, Lingling; Jiang, Changzhong
2012-07-25
Mesoporous spindlelike iron oxide/ZnO core-shell heterostructures are successfully fabricated by a low-cost, surfactant-free, and environmentally friendly seed-mediate strategy with the help of postannealing treatment. The material composition and stoichiometry, as well as these magnetic and optical properties, have been examined and verified by means of high-resolution transmission electron microscopy and X-ray diffraction, the thickness of ZnO layer can be simply tailored by the concentration of zinc precursor. Considering that both α-Fe2O3 and ZnO are good photocatalytic materials, we have investigated the photodegradation performances of the core-shell heterostructures using organic dyes Rhodamin B (RhB). It is interesting to find that the as-obtained iron oxides/ZnO core-shell heterostructures exhibited enhanced visible light or UV photocatalytic abilities, remarkably superior to the as-used α-Fe2O3 seeds and commercial TiO2 products (P25), mainly owing to the synergistic effect between the narrow and wide bandgap semiconductors and effective electron-hole separation at the interfaces of iron oxides/ZnO.
Fabrication and characterization of complex oxide RENiO3/LaAlO3 superlattices
NASA Astrophysics Data System (ADS)
Kareev, M.; Freeland, J. W.; Liu, J.; Kirby, B.; Keimer, B.; Chakhalian, J.
2008-03-01
Nowadays there has been growing interest to synthesis of atomically thin complex oxide superlattices which can result in novel electronic and magnetic properties at the interface. Here we report on digital synthesis of single unit cell nickel based heterostructures of RENiO3/LaAlO3 (RE = La, Nd and Pr) superlattices on SrTiO3 and LaAlO3 by laser MBE. RHEED analysis, grazing angle XRD and AFM imaging have confirmed the high quality of the epitaxially grown superlattices. The magnetic and electronic properties of the superlattices have been elucidated by polarized X-ray spectroscopies, which show a non-trivial evolution of magnetism and charge of the LNO layer with increasing LNO layer thickness. The work has been supported by U.S. DOD-ARO under Contract No. 0402-17291.
DOE Office of Scientific and Technical Information (OSTI.GOV)
Spurgeon, Steven R.; Chambers, Scott A.
Scanning transmission electron microscopy (STEM) has become one of the fundamental tools to characterize oxide interfaces and superlattices. Atomic-scale structure, chemistry, and composition mapping can now be conducted on a wide variety of materials systems thanks to the development of aberration-correctors and advanced detectors. STEM imaging and diffraction, coupled with electron energy loss (EELS) and energy-dispersive X-ray (EDS) spectroscopies, offer unparalleled, high-resolution analysis of structure-property relationships. In this chapter we highlight investigations into key phenomena, including interfacial conductivity in oxide superlattices, charge screening effects in magnetoelectric heterostructures, the design of high-quality iron oxide interfaces, and the complex physics governing atomic-scalemore » chemical mapping. These studies illustrate how unique insights from STEM characterization can be integrated with other techniques and first-principles calculations to develop better models for the behavior of functional oxides.« less
A dewetting route to grow heterostructured nanoparticles based on thin film heterojunctions.
Li, Junjie; Yin, Deqiang; Li, Qiang; Chen, Chunlin; Huang, Sumei; Wang, Zhongchang
2015-12-21
Heterostructured nanoparticles have received considerable attention for their various applications due to their unique and tunable functionalities with respect to their individual bulk constituents. However, the current wet chemical synthesis of multicomponent heterostructured nanoparticles is rather complicated. Here, we report a simple and quick method to fabricate Co-Au dumbbell arrays by dewetting Co/Au heterojunctions on a Si substrate and demonstrate that the Co-Au dumbbells vary in size from 2 to 28 nm. We further show by chemical mapping that Co bells are covered by a pseudomorphic Au wetting layer of ∼4 Å, preventing the bells from oxidation. By controlling the thickness of metal heterojunctions and the annealing time, the morphology of the Co-Au nanoparticle is found to be transformed from the dumbbell to the core shell. This facile route is demonstrated to be useful for fabricating other metal-metal and metal-oxide heterostructures and hence holds technological promise for functional applications.
Li, Lihua; Yu, Lili; Lin, Zhaoyong; Yang, Guowei
2016-04-06
The reduced TiO2-graphene oxide heterostructure as an alternative broad spectrum-driven efficient water splitting photocatalyst has become a really interesting topic, however, its syntheses has many flaws, e.g., tedious experimental steps, time-consuming, small scale production, and requirement of various additives, for example, hydrazine hydrate is widely used as reductant to the reduction of graphene oxide, which is high toxicity and easy to cause the second pollution. For these issues, herein, we reported the synthesis of the reduced TiO2-graphene oxide heterostructure by a facile chemical reduction agent-free one-step laser ablation in liquid (LAL) method, which achieves extended optical response range from ultraviolet to visible and composites TiO(2-x) (reduced TiO2) nanoparticle and graphene oxide for promoting charge conducting. 30.64% Ti(3+) content in the reduced TiO2 nanoparticles induces the electronic reconstruction of TiO2, which results in 0.87 eV decrease of the band gap for the visible light absorption. TiO(2-x)-graphene oxide heterostructure achieved drastically increased photocatalytic H2 production rate, up to 23 times with respect to the blank experiment. Furthermore, a maximum H2 production rate was measured to be 16 mmol/h/g using Pt as a cocatalyst under the simulated sunlight irradiation (AM 1.5G, 135 mW/cm(2)), the quantum efficiencies were measured to be 5.15% for wavelength λ = 365 ± 10 nm and 1.84% for λ = 405 ± 10 nm, and overall solar energy conversion efficiency was measured to be 14.3%. These findings provided new insights into the broad applicability of this methodology for accessing fascinate photocatalysts.
DOE Office of Scientific and Technical Information (OSTI.GOV)
Subramanyam, Guru, E-mail: gsubramanyam1@udayton.edu; Cole, M. W., E-mail: melanie.w.cole.civ@mail.mil; Sun, Nian X.
2013-11-21
There has been significant progress on the fundamental science and technological applications of complex oxides and multiferroics. Among complex oxide thin films, barium strontium titanate (BST) has become the material of choice for room-temperature-based voltage-tunable dielectric thin films, due to its large dielectric tunability and low microwave loss at room temperature. BST thin film varactor technology based reconfigurable radio frequency (RF)/microwave components have been demonstrated with the potential to lower the size, weight, and power needs of a future generation of communication and radar systems. Low-power multiferroic devices have also been recently demonstrated. Strong magneto-electric coupling has also been demonstratedmore » in different multiferroic heterostructures, which show giant voltage control of the ferromagnetic resonance frequency of more than two octaves. This manuscript reviews recent advances in the processing, and application development for the complex oxides and multiferroics, with the focus on voltage tunable RF/microwave components. The over-arching goal of this review is to provide a synopsis of the current state-of the-art of complex oxide and multiferroic thin film materials and devices, identify technical issues and technical challenges that need to be overcome for successful insertion of the technology for both military and commercial applications, and provide mitigation strategies to address these technical challenges.« less
2015-09-23
with a metal oxide ( TiO2 ). Our novel direct synthesis of graphene/ TiO2 heterostructure is achieved by C60 deposition on transition Ti metal surface...of TiO2 and C 2p orbitals in the conduction band of graphene enabled by Coulomb interactions at the interface. In addition, this heterostructure...provides a platform for realization of bottom gated graphene field effect devices with graphene and TiO2 playing the roles of channel and gate dielectric
Chen, Binbin; Chen, Pingfan; Xu, Haoran; Jin, Feng; Guo, Zhuang; Lan, Da; Wan, Siyuan; Gao, Guanyin; Chen, Feng; Wu, Wenbin
2016-12-21
Controlling functionalities in oxide heterostructures remains challenging for the rather complex interfacial interactions. Here, by modifying the interface properties with chemical doping, we achieve a nontrivial control over the ferromagnetism in ultrathin La 0.67 Ca 0.33 MnO 3 (LCMO) layer sandwiched between CaRu 1-x Ti x O 3 [CRTO(x)] epilayers. The Ti doping suppresses the interfacial electron transfer from CRTO(x) to LCMO side; as a result, a steadily decreased Curie temperature with increasing x, from 262 K at x = 0 to 186 K at x = 0.8, is observed for the structures with LCMO fixed at 3.2 nm. Moreover, for more insulating CRTO(x ≥ 0.5), the electron confinement induces an interfacial Mn-e g (x 2 -y 2 ) orbital order in LCMO which further attenuates the ferromagnetism. Also, in order to characterize the heterointerfaces, for the first time the doping- and thickness-dependent metal-insulator transitions in CRTO(x) films are examined. Our results demonstrate that the LCMO/CRTO(x) heterostructure could be a model system for investigating the interfacial multiple interactions in correlated oxides.
Pinhole mediated electrical transport across LaTiO3/SrTiO3 and LaAlO3/SrTiO3 oxide hetero-structures
NASA Astrophysics Data System (ADS)
Kumar, Pramod; Dogra, Anjana; Toutam, Vijaykumar
2013-11-01
Metal-insulator-metal configuration of LaTiO3/SrTiO3 and LaAlO3/SrTiO3 hetero-structures between two dimensional electron gas formed at the interface and different area top electrodes is employed for Conductive Atomic force microscopy (CAFM) imaging, Current-Voltage (I-V), and Capacitance-Voltage (C-V) spectroscopy. Electrode area dependent I-V characteristics are observed for these oxide hetero-structures. With small area electrodes, rectifying I-V characteristics are observed, compared to, both tunneling and leakage current characteristics for large area electrodes. CAFM mapping confirmed the presence of pinholes on both surfaces. Resultant I-V characteristics have a contribution from both tunneling and leakage due to pinholes.
Samal, Alaka; Das, D P; Nanda, K K; Mishra, B K; Das, J; Dash, A
2016-02-18
A visible light driven, direct Z-scheme reduced graphene oxide-Ag3PO4 (RGO-Ag3 PO4 ) heterostructure was synthesized by means of a simple one-pot photoreduction route by varying the amount of RGO under visible light illumination. The reduction of graphene oxide (GO) and growth of Ag3PO4 took place simultaneously. The effect of the amount of RGO on the textural properties and photocatalytic activity of the heterostructure was investigated under visible light illumination. Furthermore, total organic carbon (TOC) analysis confirmed 97.1 % mineralization of organic dyes over RGO-Ag3PO4 in just five minutes under visible-light illumination. The use of different quenchers in the photomineralization suggested the presence of hydroxyl radicals ((.)OH), superoxide radicals ((.)O2 (-)), and holes (h(+)), which play a significant role in the mineralization of organic dyes. In addition to that, clean hydrogen fuel generation was also observed with excellent reusability. The 4 RGO-Ag3PO4 heterostructure has a high H2 evolution rate of 3690 μmol h(-1) g(-1), which is 6.15 times higher than that of RGO. © 2016 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.
Tunable intraparticle frameworks for creating complex heterostructured nanoparticle libraries
NASA Astrophysics Data System (ADS)
Fenton, Julie L.; Steimle, Benjamin C.; Schaak, Raymond E.
2018-05-01
Complex heterostructured nanoparticles with precisely defined materials and interfaces are important for many applications. However, rationally incorporating such features into nanoparticles with rigorous morphology control remains a synthetic bottleneck. We define a modular divergent synthesis strategy that progressively transforms simple nanoparticle synthons into increasingly sophisticated products. We introduce a series of tunable interfaces into zero-, one-, and two-dimensional copper sulfide nanoparticles using cation exchange reactions. Subsequent manipulation of these intraparticle frameworks yielded a library of 47 distinct heterostructured metal sulfide derivatives, including particles that contain asymmetric, patchy, porous, and sculpted nanoarchitectures. This generalizable mix-and-match strategy provides predictable retrosynthetic pathways to complex nanoparticle features that are otherwise inaccessible.
Tunable one-dimensional electron gas carrier densities at nanostructured oxide interfaces
Zhang, Lipeng; Xu, Haixuan; Kent, Paul R. C.; ...
2016-05-06
The emergence of two-dimensional metallic states at the LaAlO 3/SrTiO 3 (LAO/STO) heterostructure interface is known to occur at a critical thickness of four LAO over layers. This insulator-to-metal transition can be explained through the polar catastrophe mechanism arising from the divergence of the electrostatic potential at the LAO surface. Here, we demonstrate that nanostructuring can be effective in reducing or eliminating this critical thickness. Employing a modified polar catastrophe" model, we demonstrate that the nanowire heterostructure electrostatic potential diverges more rapidly as a function of layer thickness than in a regular heterostructure. Our first principles calculations indicate that formore » nanowire heterostructure geometries a one-dimensional electron gas (1DEG) can be induced, consistent with recent experimental observations of 1D conductivity in LAO/STO steps. Similar to LAO/STO 2DEGs, we predict that the 1D charge density will decay laterally within a few unit cells away from the nanowire; thus providing a mechanism for tuning the carrier behavior between 1D and 2D conductivity. Furthermore, our work provides insight into the creation and manipulation of charge density at an oxide heterostructure interface and therefore may be beneficial for future nanoelectronic devices and for the engineering of novel quantum phases.« less
Hidden Interface Driven Exchange Coupling in Oxide Heterostructures
Chen, Aiping; Wang, Qiang; Fitzsimmons, Michael R.; ...
2017-05-02
In a variety of emergent phenomena have been enabled by interface engineering in complex oxides. The existence of an intrinsic interfacial layer has often been found at oxide heterointerfaces. But, the role of such an interlayerin controlling functionalities is not fully explored. Here, we report the control of the exchange bias (EB) in single-phase manganite thin films with nominallyuniform chemical composition across the interfaces. The sign of EB depends on the magnitude of the cooling field. A pinned layer, confirmed by polarized neutron reflectometry, provides the source of unidirectional anisotropy. The origin of the exchange bias coupling is discussed inmore » terms of magnetic interactions between the interfacial ferromagnetically reduced layer and the bulk ferromagnetic region. The sign of EB is related to the frustration of antiferromagnetic coupling between the ferromagnetic region and the pinned layer. These results shed new light on using oxide interfaces to design functional spintronic devices.« less
Spatially resolved ultrafast magnetic dynamics initiated at a complex oxide heterointerface
Forst, M.; Wilkins, S. B.; Caviglia, A. D.; ...
2015-07-06
Static strain in complex oxide heterostructures 1,2 has been extensively used to engineer electronic and magnetic properties at equilibrium 3. In the same spirit, deformations of the crystal lattice with light may be used to achieve functional control across heterointerfaces dynamically 4. Here, by exciting large-amplitude infrared-active vibrations in a LaAlO 3 substrate we induce magnetic order melting in a NdNiO 3 film across a heterointerface. Femtosecond resonant soft X-ray diffraction is used to determine the spatiotemporal evolution of the magnetic disordering. We observe a magnetic melt front that propagates from the substrate interface into the film, at a speedmore » that suggests electronically driven motion. Lastly, light control and ultrafast phase front propagation at heterointerfaces may lead to new opportunities in optomagnetism, for example by driving domain wall motion to transport information across suitably designed devices.« less
Achieving tunable doping of MoSe2 based devices using GO@MoSe2 heterostructure
NASA Astrophysics Data System (ADS)
Maji, Tuhin Kumar; Tiwary, Krishna Kanhaiya; Karmakar, Debjani
2017-05-01
Doping nature of MoSe2, one of the promising Graphene analogous device material, can be tuned by controlling the concentration of functional groups in Graphene oxide (GO)@MoSe2 heterostructure. In this study, by first-principles simulation, we have observed that GO can be used as a carrier injection layer for MoSe2, where n or p type carriers are introduced within MoSe2 layer depending on the type and concentration of functional moieties in it. Both n and p-type Schottky barrier height modulations are investigated for different modeled configurations of the heterostructure. This combinatorial heterostructure can be a promising material for future electronic device application.
Tian, Chengcheng; Zhu, Xiang; Abney, Carter W.; ...
2017-04-12
An ultrastable Au nanocatalyst based on a heterostructured perovskite support with high surface area and uniform LaFeO3 nanocoatings was successfully synthesized and tested for CO oxidation. Strikingly, small Au nanoparticles (4-6 nm) are obtained after calcination in air at 700 °C and under reaction conditions. The designed Au catalyst not only possessed extreme sintering resistance but also showed high catalytic activity and stability because of the strong interfacial interaction between Au and the heterostructured perovskite support.
An Emergent Spin-Filter at the interface between Ferromagnetic and Insulating Layered Oxides
NASA Astrophysics Data System (ADS)
Liu, Yaohua
2014-03-01
Complex oxide heterostructures are of keen interest because modified bonding at the interfaces can give rise to fundamentally new phenomena and valuable functionalities. Particularly, an induced magnetization is widely observed at epitaxial interfaces between layered transition-metal oxides; however, much less effort has been spent on investigating how it affects the charge transport properties. To this end, we have studied magnetic tunneling junctions consisting of ferromagnetic manganite La0.7Ca0.3MnO3 (LCMO) and insulating cuprate PrBa2Cu3O7 (PBCO). Contrary to the typically observed steady increase of the tunnel magnetoresistance with decreasing temperature, this system exhibits an anomalous decrease at low temperatures. Polarized neutron reflectometry (PNR) and x-ray magnetic circular dichroism (XMCD) studies on LCMO/PBCO/LCMO trilayers show that the saturation magnetization of the LCMO contacts increase as the temperature decreases. In other words, degradation of the ferromagnetic contacts is ruled out as a cause. Interestingly, there exists induced net Cu moments, which indicates that the spin degeneracy of the conduction band of the PBCO barrier is lifted and thus the barrier becomes spin selective. Our calculations, within the Wentzel-Kramers-Brillouin approximation, show that the complex temperature dependence can arise from a competition between the high positive spin polarization of the manganite electrodes and a negative spin-filter effect from the interfacial Cu magnetization. This work illustrates that the interface-induced magnetization in layered oxide heterostructures can have non-trivial effects on the macroscopic transport properties. Work performed in collaboration with FA Cuellar, Z Sefrioui, C Leon, J Santamaria (Universidad Complutense de Madrid), JW Freeland, SGE te Velthuis (ANL) and MR Fitzsimmons (LANL). Work at Argonne National Laboratory was supported by the U.S. Department of Energy, Office of Basic Energy Sciences under contract no. DE-AC02-06CH11357.
Solar photochemical and thermochemical splitting of water.
Rao, C N R; Lingampalli, S R; Dey, Sunita; Roy, Anand
2016-02-28
Artificial photosynthesis to carry out both the oxidation and the reduction of water has emerged to be an exciting area of research. It has been possible to photochemically generate oxygen by using a scheme similar to the Z-scheme, by using suitable catalysts in place of water-oxidation catalyst in the Z-scheme in natural photosynthesis. The best oxidation catalysts are found to be Co and Mn oxides with the e(1) g configuration. The more important aspects investigated pertain to the visible-light-induced generation of hydrogen by using semiconductor heterostructures of the type ZnO/Pt/Cd1-xZnxS and dye-sensitized semiconductors. In the case of heterostructures, good yields of H2 have been obtained. Modifications of the heterostructures, wherein Pt is replaced by NiO, and the oxide is substituted with different anions are discussed. MoS2 and MoSe2 in the 1T form yield high quantities of H2 when sensitized by Eosin Y. Two-step thermochemical splitting of H2O using metal oxide redox pairs provides a strategy to produce H2 and CO. Performance of the Ln0.5A0.5MnO3 (Ln = rare earth ion, A = Ca, Sr) family of perovskites is found to be promising in this context. The best results to date are found with Y0.5Sr0.5MnO3. © 2016 The Author(s).
Origin of fieldlike spin-orbit torques in heavy metal/ferromagnet/oxide thin film heterostructures
NASA Astrophysics Data System (ADS)
Ou, Yongxi; Pai, Chi-Feng; Shi, Shengjie; Ralph, D. C.; Buhrman, R. A.
2016-10-01
We report measurements of the thickness and temperature (T ) dependencies of current-induced spin-orbit torques, especially the fieldlike (FL) component, in various heavy metal (HM)/normal metal (NM) spacer/ferromagnet (FM)/oxide (MgO and Hf Ox/MgO ) heterostructures. The FL torque in these samples originates from spin current generated by the spin Hall effect in the HM. For a FM layer sufficiently thin that a substantial portion of this spin current can reach the FM/oxide interface, T-dependent spin scattering there can yield a strong FL torque that is, in some cases, opposite in sign to that exerted at the NM/FM interface.
Xu, Tao; Dick, Kimberly A; Plissard, Sébastien; Nguyen, Thanh Hai; Makoudi, Younes; Berthe, Maxime; Nys, Jean-Philippe; Wallart, Xavier; Grandidier, Bruno; Caroff, Philippe
2012-03-09
III-V antimonide nanowires are among the most interesting semiconductors for transport physics, nanoelectronics and long-wavelength optoelectronic devices due to their optimal material properties. In order to investigate their complex crystal structure evolution, faceting and composition, we report a combined scanning electron microscopy (SEM), transmission electron microscopy (TEM), and scanning tunneling microscopy (STM) study of gold-nucleated ternary InAs/InAs(1-x)Sb(x) nanowire heterostructures grown by molecular beam epitaxy. SEM showed the general morphology and faceting, TEM revealed the internal crystal structure and ternary compositions, while STM was successfully applied to characterize the oxide-free nanowire sidewalls, in terms of nanofaceting morphology, atomic structure and surface composition. The complementary use of these techniques allows for correlation of the morphological and structural properties of the nanowires with the amount of Sb incorporated during growth. The addition of even a minute amount of Sb to InAs changes the crystal structure from perfect wurtzite to perfect zinc blende, via intermediate stacking fault and pseudo-periodic twinning regimes. Moreover, the addition of Sb during the axial growth of InAs/InAs(1-x)Sb(x) heterostructure nanowires causes a significant conformal lateral overgrowth on both segments, leading to the spontaneous formation of a core-shell structure, with an Sb-rich shell.
Thermal and Electrical Transport in Oxide Heterostructures
NASA Astrophysics Data System (ADS)
Ravichandran, Jayakanth
This dissertation presents a study of thermal and electrical transport phenomena in heterostructures of transition metal oxides, with specific interest in understanding and tailoring thermoelectricity in these systems. Thermoelectric energy conversion is a promising method for waste heat recovery and the efficiency of such an engine is directly related to a material dependent figure of merit, Z, given as S2sigma/kappa, where S is thermopower and sigma and kappa are electrical and thermal conductivity respectively. Achieving large figure of merit has been hampered by the coupling between these three thermoelectric coefficients, and the primary aim of this study is to understand the nature of thermoelectricity in complex oxides and identify mechanisms which can allow tuning of one or more thermoelectric coefficients in a favorable manner. Unlike the heavily studied conventional thermoelectric semiconductors, transition metals based complex oxides show conduction band characteristics dominated by d-bands, with much larger effective masses and varying degrees of electron correlations. These systems provide for exotic thermoelectric effects which are typically not explained by conventional theories and hence provide an ideal platform for exploring the limits of thermoelectricity. Meanwhile, oxides are composed of earth abundant elements and have excellent high temperature stability, thus providing compelling technological possibilities for thermoelectrics based power generation. In this dissertation, we address specific aspects of thermoelectricity in model complex oxide systems such as perovskite titanates and layered cobaltates to understand thermal and thermoelectric behavior and explore the tunability of thermoelectricity in these systems. The demonstration of band engineering as a viable method to tune physical properties of materials is explored. The model system used for this case is strontium titanate, where two dopants such as La on the Sr-site and oxygen vacancies are employed to achieve band engineering. This method was used to obtain tunable transparent conducting properties and thermoelectric properties for heavily doped strontium titanate. The second aspect investigated is the use of strongly correlated materials for thermoelectricity. The cobaltates, specifically layered cobaltates, show large thermopower even at very large carrier densities. The coupling of thermopower and electrical conductivity is shown to be weaker for a strongly correlated material such as cobaltate, which opens up possibilities of complete decoupling of all three thermoelectric coefficients. Finally, the thermal properties of complex oxides, specifically in perovskite titanates, is addressed in detail. Thermal conductivity is demonstrated to be a sensitive probe for defects in a system, where processing conditions play a significant role in modulating the crystallinity of the material. The perovskite titanate superlattice system of strontium titanate and calcium titanate is used beat alloy limit. It also shows interesting period thickness dependent thermal properties. The possible origin of this effect is briefly discussed and future directions for this research is also elaborated in detail.
Superconductivity in interacting interfaces of cuprate-based heterostructures
NASA Astrophysics Data System (ADS)
Di Castro, Daniele; Balestrino, Giuseppe
2018-07-01
Low dimensional superconducting systems have been the subject of numerous studies in the recent past, with the aim of achieving a higher and higher critical temperature (T c ). The recent improvement in film deposition techniques has allowed the realization of artificial heterostructures, with atomically flat surfaces and interfaces, where novel properties appear that are not present in the single constituent. For instance, quasi-2D superconductivity was found at the interface between different oxides. In this review we analyze, in particular, the quasi-2D superconductivity occurring at the interface between two non-superconducting oxides, mostly cuprates. Throughout a comparison of the superconducting properties of different oxide heterostructures and superlattices, we propose a phenomenological explanation of the behavior of the T c as a function of the number of conducting CuO2 planes. This is achieved by introducing two different interactions between the superconducting 2D sheets. This interpretation is finally extended also to standard high T c cuprates, contributing to the solution of the long-standing question of the dependence of T c on the number of CuO2 planes in these systems.
n-VO2/p-GaN based nitride-oxide heterostructure with various thickness of VO2 layer grown by MBE
NASA Astrophysics Data System (ADS)
Wang, Minhuan; Bian, Jiming; Sun, Hongjun; Liu, Weifeng; Zhang, Yuzhi; Luo, Yingmin
2016-12-01
High quality VO2 films with precisely controlled thickness were grown on p-GaN/sapphire substrates by oxide molecular beam epitaxy (O-MBE). Results indicated that a distinct reversible semiconductor-to-metal (SMT) phase transition was observed for all the samples in the temperature dependent electrical resistance measurement, and the influence of VO2 layer thickness on the SMT properties of the as-grown n-VO2/p-GaN based nitride-oxide heterostructure was investigated. Meanwhile, the clear rectifying transport characteristics originated from the n-VO2/p-GaN interface were demonstrated before and after SMT of the VO2 over layer, which were attributed to the p-n junction behavior and Schottky contact character, respectively. Moreover, the X-ray photoelectron spectroscopy (XPS) analyses confirmed the valence state of vanadium (V) in VO2 films was principally composed of V4+ with trace amount of V5+. The design and modulation of the n-VO2/p-GaN based heterostructure devices will benefit significantly from these achievements.
Gas Sensing Properties of p-Co₃O₄/n-TiO₂ Nanotube Heterostructures.
Alev, Onur; Kılıç, Alp; Çakırlar, Çiğdem; Büyükköse, Serkan; Öztürk, Zafer Ziya
2018-03-23
In this paper, we fabricated p-Co₃O₄/n-TiO₂ heterostructures and investigated their gas sensing properties. The structural and morphological characterization were performed by scanning electron microscopy (SEM), X-ray diffraction (XRD), and X-ray photoelectron spectroscopy analysis (XPS). The electrical properties of the heterostructure were studied within the temperature range from 293 K to 423 K. Changes in electrical properties and sensing behavior against reducing and oxidizing gases were attributed to the formation of p-n heterojunctions at the Co₃O₄ and TiO₂ interface. In comparison with sensing performed with pristine TiO₂ nanotubes (NTs), a significant improvement in H₂ sensing at 200 °C was observed, while the sensing response against NO₂ decreased for the heterostructures. Additionally, a response against toluene gas, in contrast to pristine TiO₂ NTs, appeared in the Co₃O₄/TiO₂ heterostructure samples.
Graphitic carbon nitride based nanocomposites: a review
NASA Astrophysics Data System (ADS)
Zhao, Zaiwang; Sun, Yanjuan; Dong, Fan
2014-11-01
Graphitic carbon nitride (g-C3N4), as an intriguing earth-abundant visible light photocatalyst, possesses a unique two-dimensional structure, excellent chemical stability and tunable electronic structure. Pure g-C3N4 suffers from rapid recombination of photo-generated electron-hole pairs resulting in low photocatalytic activity. Because of the unique electronic structure, the g-C3N4 could act as an eminent candidate for coupling with various functional materials to enhance the performance. According to the discrepancies in the photocatalytic mechanism and process, six primary systems of g-C3N4-based nanocomposites can be classified and summarized: namely, the g-C3N4 based metal-free heterojunction, the g-C3N4/single metal oxide (metal sulfide) heterojunction, g-C3N4/composite oxide, the g-C3N4/halide heterojunction, g-C3N4/noble metal heterostructures, and the g-C3N4 based complex system. Apart from the depiction of the fabrication methods, heterojunction structure and multifunctional application of the g-C3N4-based nanocomposites, we emphasize and elaborate on the underlying mechanisms in the photocatalytic activity enhancement of g-C3N4-based nanocomposites. The unique functions of the p-n junction (semiconductor/semiconductor heterostructures), the Schottky junction (metal/semiconductor heterostructures), the surface plasmon resonance (SPR) effect, photosensitization, superconductivity, etc. are utilized in the photocatalytic processes. Furthermore, the enhanced performance of g-C3N4-based nanocomposites has been widely employed in environmental and energetic applications such as photocatalytic degradation of pollutants, photocatalytic hydrogen generation, carbon dioxide reduction, disinfection, and supercapacitors. This critical review ends with a summary and some perspectives on the challenges and new directions in exploring g-C3N4-based advanced nanomaterials.
Novel engineered compound semiconductor heterostructures for advanced electronics applications
NASA Astrophysics Data System (ADS)
Stillman, Gregory E.; Holonyak, Nick, Jr.; Coleman, James J.
1992-06-01
To provide the technology base that will enable SDIO capitalization on the performance advantages offered through novel engineered multiple-lavered compound semiconductor structures, this project has focussed on three specific areas: (1) carbon doping of AlGaAs/GaAs and InP/InGaAs materials for reliable high frequency heterojunction bipolar transistors; (2) impurity induced layer disordering and the environmental degradation of AlxGal-xAs-GaAs quantum-well heterostructures and the native oxide stabilization of AlxGal-xAs-GaAs quantum well heterostructure lasers; and (3) non-planar and strained-layer quantum well heterostructure lasers and laser arrays. The accomplishments in this three year research are reported in fifty-six publications and the abstracts included in this report.
Physics of SrTiO3-based heterostructures and nanostructures: a review.
Pai, Yun-Yi; Tylan-Tyler, Anthony; Irvin, Patrick; Levy, Jeremy
2018-02-09
This review provides a summary of the rich physics expressed within SrTiO 3 -based heterostructures and nanostructures. The intended audience is researchers who are working in the field of oxides, but also those with different backgrounds (e.g., semiconductor nanostructures). After reviewing the relevant properties of SrTiO 3 itself, we will then discuss the basics of SrTiO 3 -based heterostructures, how they can be grown, and how devices are typically fabricated. Next, we will cover the physics of these heterostructures, including their phase diagram and coupling between the various degrees of freedom. Finally, we will review the rich landscape of quantum transport phenomena, as well as the devices that elicit them.
Exposing high-energy surfaces by rapid-anneal solid phase epitaxy
Wang, Y.; Song, Y.; Peng, R.; ...
2017-08-08
The functional design of nanoscale transition metal oxide heterostructures depends critically on the growth of atomically flat epitaxial thin films. Much of the time, improved functionality is expected for heterostructures and surfaces with orientations that do not have the lowest surface free energy. For example, crystal faces with a high surface free energy, such as rutile (001) planes, frequently exhibit higher catalytic activities but are correspondingly harder to synthesize due to energy-lowering faceting transitions. We propose a broadly applicable rapid-anneal solid phase epitaxial synthesis approach for the creation of atomically flat, high surface free energy oxide heterostructures. We also demonstratemore » its efficacy via the synthesis of atomically flat, epitaxial RuO 2(001) films with a superior oxygen evolution activity, quantified by their lower onset potential and higher current density, relative to that of more common RuO 2(110) films.« less
Sun, Mingjuan; Hu, Jiayue; Zhai, Chunyang; Zhu, Mingshan; Pan, Jianguo
2017-04-19
In this paper, CuI, as a typical hole-transport channel, was used to construct a high-performance visible-light-driven CuI/BiOI heterostructure for photoelectrocatalytic applications. The heterostructure combines the broad visible absorption of BiOI and high hole mobility of CuI. Compared to pure BiOI, the CuI/BiOI heterostructure exhibited distinctly enhanced photoelectrocatalytic performance for the oxidation of methanol and organic pollutants under visible-light irradiation. The photogenerated electron-hole pairs of the excited BiOI can be separated efficiently through CuI, in which the CuI acts as a superior hole-transport channel to improve photoelectrocatalytic oxidization of methanol and organic pollutants. The outstanding photoelectrocatalytic activity shows that the p-type CuI works as a promising hole-transport channel to improve the photocatalytic performance of traditional semiconductors.
Growth and Transport Studies of LaTiO3 / KTaO3 Heterostructures
NASA Astrophysics Data System (ADS)
Zou, K.; Walker, F. J.; Ahn, C. H.
2014-03-01
Perovskite oxide heterostructures provide a rich platform for exploring emergent electronic properties, such as 2D electron gases (2DEGs) at interfaces. In this talk, we present results on the growth of LaTiO3 / KTaO3 heterostructures by molecular beam epitaxy and subsequent measurements of transport properties. Although both oxide materials are insulating in the bulk, metallic conduction is observed from T = 2 - 300 K. We achieve a room temperature carrier mobility of ~ 25 cm2 /Vs at a carrier density of ~ 1014 /cm2. By comparison, 2DEGs in LaTiO3 / SrTiO3 and LaAlO3 / SrTiO3 have lower carrier mobility, but the same carrier density. We attribute some of the increase in mobility to the smaller band effective mass of the Ta 4d electrons compared to the Ti 3d electrons.
NASA Astrophysics Data System (ADS)
Šály, V.; Perný, M.; Janíček, F.; Huran, J.; Mikolášek, M.; Packa, J.
2017-04-01
Progressive smart photovoltaic technologies including heterostructures a-SiC/c-Si with ITO antireflection film are one of the prospective replacements of conventional photovoltaic silicon technology. Our paper is focused on the investigation of heterostructures a-SiC/c-Si provided with a layer of ITO (indium oxide/tin oxide 90/10 wt.%) which acts as a passivating and antireflection coating. Prepared photovoltaic cell structure was investigated at various temperatures and the influence of temperature on its operation was searched. The investigation of the dynamic properties of heterojunction PV cells was carried out using impedance spectroscopy. The equivalent AC circuit which approximates the measured impedance data was proposed. Assessment of the influence of the temperature on the operation of prepared heterostructure was carried out by analysis of the temperature dependence of AC equivalent circuit elements.
Fan, Jinchang; Qi, Kun; Zhang, Lei; Zhang, Haiyan; Yu, Shansheng; Cui, Xiaoqiang
2017-05-31
Tailoring the interfacial structure of Pt-based catalysts has emerged as an effective strategy to improve catalytic activity. However, little attention has been focused on investigating the relationship between the interfacial facets and their catalytic activity. Here, we design and implement Pd-Pt interfaces with controlled heterostructure features by epitaxially growing Pt nanoparticles on Pd nanosheets. On the basis of both density functional theory calculation and experimental results, we demonstrate that charge transfer from Pd to Pt is highly dependent on the interfacial facets of Pd substrates. Therefore, the Pd-Pt heterostructure with Pd(100)-Pt interface exhibits excellent activity and long-term stability for hydrogen evolution and methanol/ethanol oxidation reactions in alkaline medium, much better than that with Pd (111)-Pt interface or commercial Pt/C. Interfacial crystal facet-dependent electronic structural modulation sheds a light on the design and investigation of new heterostructures for high-activity catalysts.
Heterostructured nanohybrid of zinc oxide-montmorillonite clay.
Hur, Su Gil; Kim, Tae Woo; Hwang, Seong-Ju; Hwang, Sung-Ho; Yang, Jae Hun; Choy, Jin-Ho
2006-02-02
We have synthesized heterostructured zinc oxide-aluminosilicate nanohybrids through a hydrothermal reaction between the colloidal suspension of exfoliated montmorillonite nanosheets and the sol solution of zinc acetate. According to X-ray diffraction, N2 adsorption-desorption isotherm, and field emission-scanning electron microscopic analyses, it was found that the intercalation of zinc oxide nanoparticles expands the basal spacing of the host montmorillonite clay, and the crystallites of the nanohybrids are assembled to form a house-of-cards structure. From UV-vis spectroscopic investigation, it becomes certain that calcined nanohybrid contains two kinds of the zinc oxide species in the interlayer space of host lattice and in mesopores formed by the house-of-cards type stacking of the crystallites. Zn K-edge X-ray absorption near-edge structure/extended X-ray absorption fine structure analyses clearly demonstrate that guest species in the nanohybrids exist as nanocrystalline zinc oxides with wurzite-type structure.
Physics of Ultrathin Films and Heterostructures of Rare-Earth Nickelates
Middey, Srimanta; Chakhalian, J.; Mahadevan, P.; ...
2016-04-06
The electronic structure of transition metal oxides featuring correlated electrons can be rationalized within the Zaanen-Sawatzky-Allen framework. Following a brief description of the present paradigms of electronic behavior, we focus on the physics of rare-earth nickelates as an archetype of complexity emerging within the charge transfer regime. The intriguing prospect of realizing the physics of high- Tc cuprates through heterostructuring resulted in a massive endeavor to epitaxially stabilize these materials in ultrathin form. A plethora of new phenomena unfolded in such artificial structures due to the effect of epitaxial strain, quantum confinement, and interfacial charge transfer. Here we review themore » present status of artificial rare-earth nickelates in an effort to uncover the interconnection between the electronic and magnetic behavior and the underlying crystal structure. Here, we conclude by discussing future directions to disentangle the puzzle regarding the origin of the metal-insulator transition, the role of oxygen holes, and the true nature of the antiferromagnetic spin configuration in the ultrathin limit.« less
Shi, Jinwei; Lin, Meng-Hsien; Chen, I-Tung; Mohammadi Estakhri, Nasim; Zhang, Xin-Quan; Wang, Yanrong; Chen, Hung-Ying; Chen, Chun-An; Shih, Chih-Kang; Alù, Andrea; Li, Xiaoqin; Lee, Yi-Hsien; Gwo, Shangjr
2017-06-26
Atomically thin lateral heterostructures based on transition metal dichalcogenides have recently been demonstrated. In monolayer transition metal dichalcogenides, exciton energy transfer is typically limited to a short range (~1 μm), and additional losses may be incurred at the interfacial regions of a lateral heterostructure. To overcome these challenges, here we experimentally implement a planar metal-oxide-semiconductor structure by placing a WS 2 /MoS 2 monolayer heterostructure on top of an Al 2 O 3 -capped Ag single-crystalline plate. We find that the exciton energy transfer range can be extended to tens of microns in the hybrid structure mediated by an exciton-surface plasmon polariton-exciton conversion mechanism, allowing cascaded exciton energy transfer from one transition metal dichalcogenides region supporting high-energy exciton resonance to a different transition metal dichalcogenides region in the lateral heterostructure with low-energy exciton resonance. The realized planar hybrid structure combines two-dimensional light-emitting materials with planar plasmonic waveguides and offers great potential for developing integrated photonic and plasmonic devices.Exciton energy transfer in monolayer transition metal dichalcogenides is limited to short distances. Here, Shi et al. fabricate a planar metal-oxide-semiconductor structure and show that exciton energy transfer can be extended to tens of microns, mediated by an exciton-surface-plasmon-polariton-exciton conversion mechanism.
NASA Astrophysics Data System (ADS)
Hao, Guanhua; Noviasky, Nicholas; Cao, Shi; Sabirianov, Ildar; Yin, Yuewei; Ilie, Carolina C.; Kirianov, Eugene; Sharma, Nishtha; Sokolov, Andrei; Marshall, Andrew; Xu, Xiaoshan; Dowben, Peter A.
2018-04-01
The effect of intermediate interfacial oxidation on the in-plane magnetization of multilayer stack Pt/Co/Gd2O3, on a p-type silicon substrate, has been investigated by magneto-optical Kerr effect (MOKE) measurements, the anomalous Hall effect, and magnetoresistance measurements. While voltage controlled perpendicular magnetic anisotropy of a metal/oxide heterostructure is known, this heterostructure displays an inverse relationship between voltage and coercivity. The anomalous Hall effect demonstrates a significant change in hysteresis, with the applied bias sign. There is a higher perpendicular magnetic anisotropy with positive bias exposure.
Wang, Shijian; Liu, Shuaishuai; Li, Xuemei; Li, Cong; Zang, Rui; Man, Zengming; Wu, Yuhan; Li, Pengxin; Wang, Guoxiu
2018-03-12
Tin disulfide, as a promising high-capacity anode material for sodium-ion batteries, exhibits high theoretical capacity but poor practical electrochemical properties due to its low electrical conductivity. Constructing heterostructures has been considered to be an effective approach to enhance charge transfer and ion-diffusion kinetics. In this work, composites of SnS 2 /Sb 2 S 3 heterostructures with reduced graphene oxide nanosheets were synthesized by a facile one-pot hydrothermal method. When applied as anode material in sodium-ion batteries, the composite showed a high reversible capacity of 642 mA h g -1 at a current density of 0.2 A g -1 and good cyclic stability without capacity loss in 100 cycles. In particular, SnS 2 /Sb 2 S 3 heterostructures exhibited outstanding rate performance with capacities of 593 and 567 mA h g -1 at high current densities of 2 and 4 A g -1 , respectively, which could be ascribed to the dramatically improved Na + diffusion kinetics and electrical conductivity. © 2018 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.
Colloquium : Emergent properties in plane view: Strong correlations at oxide interfaces
DOE Office of Scientific and Technical Information (OSTI.GOV)
Chakhalian, Jak; Freeland, John W.; Millis, Andrew J.
2014-10-01
Finding new collective electronic states in materials is one of the fundamental goals of condensed matter physics. Atomic-scale superlattices formed from transition metal oxides are a particularly appealing hunting ground for new physics. In bulk form, transition metal oxides exhibit a remarkable range of magnetic, superconducting, and multiferroic phases that are of great scientific interest and are potentially capable of providing innovative energy, security, electronics, and medical technology platforms. In superlattices new states may emerge at the interfaces where dissimilar materials meet. This Colloquium illustrates the essential features that make transition metal oxide-based heterostructures an appealing discovery platform for emergentmore » properties with a few selected examples, showing how charge redistributes, magnetism and orbital polarization arises, and ferroelectric order emerges from heterostructures comprised of oxide components with nominally contradictory behavior with the aim providing insight into the creation and control of novel behavior at oxide interfaces by suitable mechanical, electrical, or optical boundary conditions and excitations.« less
DOE Office of Scientific and Technical Information (OSTI.GOV)
Chen, Yan; Fong, Dillon D.; Herbert, F. William
Transition metal oxide hetero-structures are interesting due to the distinctly different properties that can arise from their interfaces, such as superconductivity, high catalytic activity and magnetism. Oxygen point defects can play an important role at these interfaces in inducing potentially novel properties. The design of oxide hetero-structures in which the oxygen defects are manipulated to attain specific functionalities requires the ability to resolve the state and concentration of local oxygen defects across buried interfaces. In this work, we utilized a novel combination of hard x-ray photoelectron spectroscopy (HAXPES) and high resolution xray diffraction (HRXRD) to probe the local oxygen defectmore » distribution across the buried interfaces of oxide heterolayers. This approach provides a non-destructive way to qualitatively probe locally the oxygen defects in transition metal oxide hetero-structures. We studied two trilayer structures as model systems - the La 0.8Sr 0.2CoO 3-δ/(La 0.5Sr 0.5) 2CoO 4/La 0.8Sr 0.2CoO 3-δ (LSC 113/LSC 214) and the La 0.8Sr 0.2CoO 3-δ/La 2NiO 4+δ/La 0.8Sr 0.2CoO 3-δ (LSC 113/LNO 214) on SrTiO 3(001) single crystal substrates. We found that the oxygen defect chemistry of these transition metal oxides was strongly impacted by the presence of interfaces and the properties of the adjacent phases. Under reducing conditions, the LSC 113 in the LSC 113/LNO 214 tri-layer had less oxygen vacancies than the LSC 113 in the LSC 113/LSC 214 tri-layer and the LSC 113 single phase film. On the other hand, LSC 214 and LNO 214 were more reduced in the two tri-layer structures when in contact with the LSC 113 layer compared to their single phase counterparts. Furthermore, the results point out a potential way to modify the local oxygen defect states at oxide hetero-interfaces.« less
Chen, Yan; Fong, Dillon D.; Herbert, F. William; ...
2018-04-17
Transition metal oxide hetero-structures are interesting due to the distinctly different properties that can arise from their interfaces, such as superconductivity, high catalytic activity and magnetism. Oxygen point defects can play an important role at these interfaces in inducing potentially novel properties. The design of oxide hetero-structures in which the oxygen defects are manipulated to attain specific functionalities requires the ability to resolve the state and concentration of local oxygen defects across buried interfaces. In this work, we utilized a novel combination of hard x-ray photoelectron spectroscopy (HAXPES) and high resolution xray diffraction (HRXRD) to probe the local oxygen defectmore » distribution across the buried interfaces of oxide heterolayers. This approach provides a non-destructive way to qualitatively probe locally the oxygen defects in transition metal oxide hetero-structures. We studied two trilayer structures as model systems - the La 0.8Sr 0.2CoO 3-δ/(La 0.5Sr 0.5) 2CoO 4/La 0.8Sr 0.2CoO 3-δ (LSC 113/LSC 214) and the La 0.8Sr 0.2CoO 3-δ/La 2NiO 4+δ/La 0.8Sr 0.2CoO 3-δ (LSC 113/LNO 214) on SrTiO 3(001) single crystal substrates. We found that the oxygen defect chemistry of these transition metal oxides was strongly impacted by the presence of interfaces and the properties of the adjacent phases. Under reducing conditions, the LSC 113 in the LSC 113/LNO 214 tri-layer had less oxygen vacancies than the LSC 113 in the LSC 113/LSC 214 tri-layer and the LSC 113 single phase film. On the other hand, LSC 214 and LNO 214 were more reduced in the two tri-layer structures when in contact with the LSC 113 layer compared to their single phase counterparts. Furthermore, the results point out a potential way to modify the local oxygen defect states at oxide hetero-interfaces.« less
NASA Astrophysics Data System (ADS)
Zhan, Wenwen; He, Yue; Guo, Jiangbin; Chen, Luning; Kong, Xiangjian; Zhao, Haixia; Kuang, Qin; Xie, Zhaoxiong; Zheng, Lansun
2016-07-01
It is becoming a challenge to achieve simpler characterization and wider application of flexible metal organic frameworks (MOFs) exhibiting the gate-opening or breathing behavior. Herein, we designed an intelligent MOF-based system where the gate-opening or breathing behavior of MOFs can be facially visualized in solution. Two types of metal oxide@MOF core-shell heterostructures, ZnO@ZIF-7 and ZnO@ZIF-71, were prepared using ZnO nanorods as self-sacrificial templates. The structural flexibility of both the MOFs can be easily judged from the distinct molecular-size-related formation modes and photoelectrochemical performances between the two ZnO@ZIF heterostructures. Moreover, the rotational dynamics of the flexible parts of ZIF-7 were studied by analyzing the intrinsic physical properties, such as dielectric constants, of the structure. The present work reminds us to pay particular attention to the influences of the structural flexibility of MOFs on the structure and properties of MOF-involved heterostructures in future studies.It is becoming a challenge to achieve simpler characterization and wider application of flexible metal organic frameworks (MOFs) exhibiting the gate-opening or breathing behavior. Herein, we designed an intelligent MOF-based system where the gate-opening or breathing behavior of MOFs can be facially visualized in solution. Two types of metal oxide@MOF core-shell heterostructures, ZnO@ZIF-7 and ZnO@ZIF-71, were prepared using ZnO nanorods as self-sacrificial templates. The structural flexibility of both the MOFs can be easily judged from the distinct molecular-size-related formation modes and photoelectrochemical performances between the two ZnO@ZIF heterostructures. Moreover, the rotational dynamics of the flexible parts of ZIF-7 were studied by analyzing the intrinsic physical properties, such as dielectric constants, of the structure. The present work reminds us to pay particular attention to the influences of the structural flexibility of MOFs on the structure and properties of MOF-involved heterostructures in future studies. Electronic supplementary information (ESI) available: Experimental details, XRD patterns and SEM images of products in other reactions, concentration-dependent photocurrent responses, and supplementary data of dielectric measurements. See DOI: 10.1039/c6nr02257j
Oxygen Diode Formed in Nickelate Heterostructures by Chemical Potential Mismatch
Guo, Erjia; Liu, Yaohua; Sohn, Changhee; ...
2018-03-07
Deliberate control of oxygen vacancy formation and migration in perovskite oxide thin films is important for developing novel electronic and iontronic devices. Here in this paper, it is found that the concentration of oxygen vacancies (V O) formed in LaNiO 3 (LNO) during pulsed laser deposition is strongly affected by the chemical potential mismatch between the LNO film and its proximal layers. Increasing the V O concentration in LNO significantly modifies the degree of orbital polarization and drives the metal–insulator transition. Changes in the nickel oxidization state and carrier concentration in the films are confirmed by soft X-ray absorption spectroscopymore » and optical spectroscopy. The ability to unidirectional-control the oxygen flow across the heterointerface, e.g., a so-called “oxygen diode”, by exploiting chemical potential mismatch at interfaces provides a new avenue to tune the physical and electrochemical properties of complex oxides.« less
Oxygen Diode Formed in Nickelate Heterostructures by Chemical Potential Mismatch
DOE Office of Scientific and Technical Information (OSTI.GOV)
Guo, Erjia; Liu, Yaohua; Sohn, Changhee
Deliberate control of oxygen vacancy formation and migration in perovskite oxide thin films is important for developing novel electronic and iontronic devices. Here in this paper, it is found that the concentration of oxygen vacancies (V O) formed in LaNiO 3 (LNO) during pulsed laser deposition is strongly affected by the chemical potential mismatch between the LNO film and its proximal layers. Increasing the V O concentration in LNO significantly modifies the degree of orbital polarization and drives the metal–insulator transition. Changes in the nickel oxidization state and carrier concentration in the films are confirmed by soft X-ray absorption spectroscopymore » and optical spectroscopy. The ability to unidirectional-control the oxygen flow across the heterointerface, e.g., a so-called “oxygen diode”, by exploiting chemical potential mismatch at interfaces provides a new avenue to tune the physical and electrochemical properties of complex oxides.« less
Li, Yuan; Chopra, Nitin
2015-05-21
Patterned growth of multilayer graphene shell encapsulated gold nanoparticles (GNPs) and their covalent linking with inorganic quantum dots are demonstrated. GNPs were grown using a xylene chemical vapor deposition process, where the surface oxidized gold nanoparticles catalyze the multilayer graphene shell growth in a single step process. The graphene shell encapsulating gold nanoparticles could be further functionalized with carboxylic groups, which were covalently linked to amine-terminated quantum dots resulting in GNP-quantum dot heterostructures. The compositions, morphologies, crystallinity, and surface functionalization of GNPs and their heterostructures with quantum dots were evaluated using microscopic, spectroscopic, and analytical methods. Furthermore, optical properties of the derived architectures were studied using both experimental methods and simulations. Finally, GNP-quantum dot heterostructures were studied for photocatalytic degradation of phenol.
Complexes of dipolar excitons in layered quasi-two-dimensional nanostructures
NASA Astrophysics Data System (ADS)
Bondarev, Igor V.; Vladimirova, Maria R.
2018-04-01
We discuss neutral and charged complexes (biexcitons and trions) formed by indirect excitons in layered quasi-two-dimensional semiconductor heterostructures. Indirect excitons—long-lived neutral Coulomb-bound pairs of electrons and holes of different layers—have been known for semiconductor coupled quantum wells and have recently been reported for van der Waals heterostructures such as double bilayer graphene and transition-metal dichalcogenides. Using the configuration space approach, we derive the analytical expressions for the trion and biexciton binding energies as a function of interlayer distance. The method captures essential kinematics of complex formation to reveal significant binding energies, up to a few tens of meV for typical interlayer distances ˜3 -5 Å , with the trion binding energy always being greater than that of the biexciton. Our results can contribute to the understanding of more complex many-body phenomena such as exciton Bose-Einstein condensation and Wigner-like electron-hole crystallization in layered semiconductor heterostructures.
Tilka, J. A.; Park, J.; Ahn, Y.; ...
2016-07-06
Here, the highly coherent and tightly focused x-ray beams produced by hard x-ray light sources enable the nanoscale characterization of the structure of electronic materials but are accompanied by significant challenges in the interpretation of diffraction and scattering patterns. X-ray nanobeams exhibit optical coherence combined with a large angular divergence introduced by the x-ray focusing optics. The scattering of nanofocused x-ray beams from intricate semiconductor heterostructures produces a complex distribution of scattered intensity. We report here an extension of coherent xray optical simulations of convergent x-ray beam diffraction patterns to arbitrary x-ray incident angles to allow the nanobeam diffraction patternsmore » of complex heterostructures to be simulated faithfully. These methods are used to extract the misorientation of lattice planes and the strain of individual layers from synchrotron x-ray nanobeam diffraction patterns of Si/SiGe heterostructures relevant to applications in quantum electronic devices. The systematic interpretation of nanobeam diffraction patterns from semiconductor heterostructures presents a new opportunity in characterizing and ultimately designing electronic materials.« less
DOE Office of Scientific and Technical Information (OSTI.GOV)
Paskiewicz, Deborah M.; Sichel-Tissot, Rebecca; Karapetrova, Evguenia
The field of oxide electronics has benefited from the wide spectrum of functionalities available to the ABO 3 perovskites, and researchers are now employing defect engineering in single crystalline heterostructures to tailor properties. However, bulk oxide single crystals are not conducive to many types of applications, particularly those requiring mechanical flexibility. Here, we demonstrate the realization of an all-oxide, single-crystalline nanomembrane heterostructure. With a surface-to-volume ratio of 2 × 10 7 , the nanomembranes are fully flexible and can be readily transferred to other materials for handling purposes or for new materials integration schemes. Using in situ synchrotron X-ray scattering,more » we find that the nanomembranes can bond to other host substrates near room temperature and demonstrate coupling between surface reactivity and electromechanical properties in ferroelectric nanomembrane systems. Finally, the synthesis technique described here represents a significant advancement in materials integration and provides a new platform for the development of flexible oxide electronics.« less
Emerging magnetism and anomalous Hall effect in iridate–manganite heterostructures
Nichols, John; Gao, Xiang; Lee, Shinbuhm; Meyer, Tricia L.; Freeland, John W.; Lauter, Valeria; Yi, Di; Liu, Jian; Haskel, Daniel; Petrie, Jonathan R.; Guo, Er-Jia; Herklotz, Andreas; Lee, Dongkyu; Ward, Thomas Z.; Eres, Gyula; Fitzsimmons, Michael R.; Lee, Ho Nyung
2016-01-01
Strong Coulomb repulsion and spin–orbit coupling are known to give rise to exotic physical phenomena in transition metal oxides. Initial attempts to investigate systems, where both of these fundamental interactions are comparably strong, such as 3d and 5d complex oxide superlattices, have revealed properties that only slightly differ from the bulk ones of the constituent materials. Here we observe that the interfacial coupling between the 3d antiferromagnetic insulator SrMnO3 and the 5d paramagnetic metal SrIrO3 is enormously strong, yielding an anomalous Hall response as the result of charge transfer driven interfacial ferromagnetism. These findings show that low dimensional spin–orbit entangled 3d–5d interfaces provide an avenue to uncover technologically relevant physical phenomena unattainable in bulk materials. PMID:27596572
Graphene analogue in (111)-oriented BaBiO3 bilayer heterostructures for topological electronics.
Kim, Rokyeon; Yu, Jaejun; Jin, Hosub
2018-01-11
Topological electronics is a new field that uses topological charges as current-carrying degrees of freedom. For topological electronics applications, systems should host topologically distinct phases to control the topological domain boundary through which the topological charges can flow. Due to their multiple Dirac cones and the π-Berry phase of each Dirac cone, graphene-like electronic structures constitute an ideal platform for topological electronics; graphene can provide various topological phases when incorporated with large spin-orbit coupling and mass-gap tunability via symmetry-breaking. Here, we propose that a (111)-oriented BaBiO 3 bilayer (BBL) sandwiched between large-gap perovskite oxides is a promising candidate for topological electronics by realizing a gap-tunable, and consequently a topology-tunable, graphene analogue. Depending on how neighboring perovskite spacers are chosen, the inversion symmetry of the BBL heterostructure can be either conserved or broken, leading to the quantum spin Hall (QSH) and quantum valley Hall (QVH) phases, respectively. BBL sandwiched by ferroelectric compounds enables switching of the QSH and QVH phases and generates the topological domain boundary. Given the abundant order parameters of the sandwiching oxides, the BBL can serve as versatile topological building blocks in oxide heterostructures.
Multiple Supersonic Phase Fronts Launched at a Complex-Oxide Heterointerface
DOE Office of Scientific and Technical Information (OSTI.GOV)
Först, M.; Beyerlein, K. R.; Mankowsky, R.
Selective optical excitation of a substrate lattice can drive phase changes across heterointerfaces. This phenomenon is a nonequilibrium analogue of static strain control in heterostructures and may lead to new applications in optically controlled phase change devices. Here, we make use of time-resolved nonresonant and resonant x-ray diffraction to clarify the underlying physics and to separate different microscopic degrees of freedom in space and time. We also measure the dynamics of the lattice and that of the charge disproportionation in NdNiO 3 , when an insulator-metal transition is driven by coherent lattice distortions in the LaAlO 3 substrate. We findmore » that charge redistribution propagates at supersonic speeds from the interface into the NdNiO 3 film, followed by a sonic lattice wave. Our results establish a hierarchy of events for ultrafast control at complex-oxide heterointerfaces, when combined with measurements of magnetic disordering and of the metal-insulator transition.« less
Multiple Supersonic Phase Fronts Launched at a Complex-Oxide Heterointerface
Först, M.; Beyerlein, K. R.; Mankowsky, R.; ...
2017-01-09
Selective optical excitation of a substrate lattice can drive phase changes across heterointerfaces. This phenomenon is a nonequilibrium analogue of static strain control in heterostructures and may lead to new applications in optically controlled phase change devices. Here, we make use of time-resolved nonresonant and resonant x-ray diffraction to clarify the underlying physics and to separate different microscopic degrees of freedom in space and time. We also measure the dynamics of the lattice and that of the charge disproportionation in NdNiO 3 , when an insulator-metal transition is driven by coherent lattice distortions in the LaAlO 3 substrate. We findmore » that charge redistribution propagates at supersonic speeds from the interface into the NdNiO 3 film, followed by a sonic lattice wave. Our results establish a hierarchy of events for ultrafast control at complex-oxide heterointerfaces, when combined with measurements of magnetic disordering and of the metal-insulator transition.« less
Li, An-Ping; Park, Jewook; Lee, Jaekwang; ...
2014-01-01
Two-dimensional (2D) interfaces between crystalline materials have been shown to generate unusual interfacial electronic states in complex oxides1-4. Recently, a onedimensional (1D) polar-on-nonpolar interface has been realized in hexagonal boron nitride (hBN) and graphene heterostructures 5-10, where a coherent 1D boundary is expected to possess peculiar electronic states dictated by edge states of graphene and the polarity of hBN 11-13. Here we present a combined scanning tunneling microscopy (STM) and firstprinciples theory study of the graphene-hBN boundary to provide a rare glimpse into the spatial and energetic distributions of the 1D boundary states in real-space. The interfaces studied here aremore » crystallographically coherent with sharp transitions from graphene zigzag edges to B (or N) terminated hBN atomic layers on a Cu foil substrate5. The revealed boundary states are about 0.6 eV below or above the Fermi energy depending on the termination of the hBN at the boundary, and are extended along but localized at the boundary with a lateral thickness of 2-3nm. These results suggest that unconventional physical effects similar to those observed at 2D interfaces can also exist in lower dimensions, opening a route for tuning of electronic properties at interfaces in 2D heterostructures.« less
NASA Astrophysics Data System (ADS)
Wagner, Markus R.; Reparaz, Juan Sebastian; Callsen, Gordon; Nippert, Felix; Kure, Thomas; Hoffmann, Axel; Hugues, Maxime; Teysseire, Monique; Damilano, Benjamin; Chauveau, Jean-Michel
2017-03-01
We address the electronic, phononic, and thermal properties of oxide based superlattices and multi quantum well heterostructures. In the first part, we review the present understanding of phonon coupling and phonon propagation in superlattices and elucidate current research aspects of phonon coherence in these structure. Subsequently, we focus on the experimental study of MBE grown ZnO/ZnMgO multi quantum well heterostructures with varying Mg content, barrier thickness, quantum well thickness, and number of periods. In particular, we discuss how the controlled variation of these parameters affect the phonon dispersion relation and phonon propagation and their impact on the thermal properties.
Wei, Wei; Qin, Zhixin; Fan, Shunfei; Li, Zhiwei; Shi, Kai; Zhu, Qinsheng; Zhang, Guoyi
2012-10-10
A sample of the β-Ga2O3/wurtzite GaN heterostructure has been grown by dry thermal oxidation of GaN on a sapphire substrate. X-ray diffraction measurements show that the β-Ga2O3 layer was formed epitaxially on GaN. The valence band offset of the β-Ga2O3/wurtzite GaN heterostructure is measured by X-ray photoelectron spectroscopy. It is demonstrated that the valence band of the β-Ga2O3/GaN structure is 1.40 ± 0.08 eV.
2012-01-01
A sample of the β-Ga2O3/wurtzite GaN heterostructure has been grown by dry thermal oxidation of GaN on a sapphire substrate. X-ray diffraction measurements show that the β-Ga2O3 layer was formed epitaxially on GaN. The valence band offset of the β-Ga2O3/wurtzite GaN heterostructure is measured by X-ray photoelectron spectroscopy. It is demonstrated that the valence band of the β-Ga2O3/GaN structure is 1.40 ± 0.08 eV. PMID:23046910
Single-Crystalline SrRuO 3 Nanomembranes: A Platform for Flexible Oxide Electronics
Paskiewicz, Deborah M.; Sichel-Tissot, Rebecca; Karapetrova, Evguenia; ...
2016-12-11
The field of oxide electronics has benefited from the wide spectrum of functionalities available to the ABO 3 perovskites, and researchers are now employing defect engineering in single crystalline heterostructures to tailor properties. However, bulk oxide single crystals are not conducive to many types of applications, particularly those requiring mechanical flexibility. Here, we demonstrate the realization of an all-oxide, single-crystalline nanomembrane heterostructure. With a surface-to-volume ratio of 2 × 10 7 , the nanomembranes are fully flexible and can be readily transferred to other materials for handling purposes or for new materials integration schemes. Using in situ synchrotron X-ray scattering,more » we find that the nanomembranes can bond to other host substrates near room temperature and demonstrate coupling between surface reactivity and electromechanical properties in ferroelectric nanomembrane systems. Finally, the synthesis technique described here represents a significant advancement in materials integration and provides a new platform for the development of flexible oxide electronics.« less
Zhang, Kexiong; Sumiya, Masatomo; Liao, Meiyong; Koide, Yasuo; Sang, Liwen
2016-01-01
The concept of p-channel InGaN/GaN heterostructure field effect transistor (FET) using a two-dimensional hole gas (2DHG) induced by polarization effect is demonstrated. The existence of 2DHG near the lower interface of InGaN/GaN heterostructure is verified by theoretical simulation and capacitance-voltage profiling. The metal-oxide-semiconductor FET (MOSFET) with Al2O3 gate dielectric shows a drain-source current density of 0.51 mA/mm at the gate voltage of −2 V and drain bias of −15 V, an ON/OFF ratio of two orders of magnitude and effective hole mobility of 10 cm2/Vs at room temperature. The normal operation of MOSFET without freeze-out at 8 K further proves that the p-channel behavior is originated from the polarization-induced 2DHG. PMID:27021054
Novel p-n heterojunction copper phosphide/cuprous oxide photocathode for solar hydrogen production.
Chen, Ying-Chu; Chen, Zhong-Bo; Hsu, Yu-Kuei
2018-08-01
A Copper phosphide (Cu 3 P) micro-rod (MR) array, with coverage by an n-Cu 2 O thin layer by electrodeposition as a photocathode, has been directly fabricated on copper foil via simple electro-oxidation and phosphidation for photoelectrochemical (PEC) hydrogen production. The morphology, structure, and composition of the Cu 3 P/Cu 2 O heterostructure are systematically analyzed using a scanning electron microscope (SEM), X-ray diffraction and X-ray photoelectron spectra. The PEC measurements corroborate that the p-Cu 3 P/n-Cu 2 O heterostructural photocathode illustrates efficient charge separation and low charge transfer resistance to achieve the highest photocurrent of 430 μA cm -2 that is greater than other transition metal phosphide materials. In addition, a detailed energy diagram of the p-Cu 3 P/n-Cu 2 O heterostructure was investigated using Mott-Schottky analysis. Our study paves the way to explore phosphide-based materials in a new class for solar energy applications. Copyright © 2018 Elsevier Inc. All rights reserved.
Li, Binzhi; Chopdekar, Rajesh V.; N'Diaye, Alpha T.; ...
2016-10-10
The impact of interfacial electronic reconstruction on the magnetic characteristics of La0.7Sr0.3CoO3 (LSCO)/La0.7Sr0.3MnO3 (LSMO) superlattices was investigated as a function of layer thickness using a combination of soft x-ray magnetic spectroscopy and bulk magnetometry. We found that the magnetic properties of the LSCO layers are impacted by two competing electronic interactions occurring at the LSCO/substrate and LSMO/LSCO interfaces. For thin LSCO layers (< 5 nm), the heterostructures exist in a highly coupled state where the chemically distinct layers behave as a single magnetic compound with magnetically active Co2+ ions. As the LSCO thickness increases, a high coercivity LSCO layer developsmore » which biases a low coercivity layer, which is composed not only of the LSMO layer, but also an interfacial LSCO layer. These results suggest a new route to tune the magnetic properties of transition metal oxide heterostructures through careful control of the interface structure.« less
NASA Astrophysics Data System (ADS)
Zhu, Shuai-Ru; Wu, Meng-Ke; Zhao, Wen-Na; Yi, Fei-Yan; Tao, Kai; Han, Lei
2017-11-01
The pyrolysis of metal-organic frameworks has emerged as a promising route to synthesize metal oxides with diverse phase compositions, morphologies, sizes and surface areas. The BiOBr/Bi24O31Br10/TiO2 (BBT) heterostructures have been achieved for the first time by calcining BiOBr/MIL-125(Ti) composite at 500 °C in air. The BBT-2 composite exhibited the highest photocatalytic performance for degradation of RhB under visible light irradiation. The enhanced photocatalytic activity is attributed to narrower band-gaps and synergistic effect originating from the well-aligned straddling band-structures between BiOBr, Bi24O31Br10 and TiO2, also result in an faster interfacial charge transfer during the photocatalytic reaction. This work could be conductive to the design of heterostructured photocatalysts contained metal oxide by pyrolytic conversion of metal-organic frameworks for significantly improved photocatalytic performance.
Strain-induced magnetization control in an oxide multiferroic heterostructure
NASA Astrophysics Data System (ADS)
Motti, Federico; Vinai, Giovanni; Petrov, Aleksandr; Davidson, Bruce A.; Gobaut, Benoit; Filippetti, Alessio; Rossi, Giorgio; Panaccione, Giancarlo; Torelli, Piero
2018-03-01
Controlling magnetism by using electric fields is a goal of research towards novel spintronic devices and future nanoelectronics. For this reason, multiferroic heterostructures attract much interest. Here we provide experimental evidence, and supporting density functional theory analysis, of a transition in L a0.65S r0.35Mn O3 thin film to a stable ferromagnetic phase, that is induced by the structural and strain properties of the ferroelectric BaTi O3 (BTO) substrate, which can be modified by applying external electric fields. X-ray magnetic circular dichroism measurements on Mn L edges with a synchrotron radiation show, in fact, two magnetic transitions as a function of temperature that correspond to structural changes of the BTO substrate. We also show that ferromagnetism, absent in the pristine condition at room temperature, can be established by electrically switching the BTO ferroelectric domains in the out-of-plane direction. The present results confirm that electrically induced strain can be exploited to control magnetism in multiferroic oxide heterostructures.
Synthesis and Characterization of Ferromagnetic/Antiferromagnetic Perovskite Oxide Superlattices
NASA Astrophysics Data System (ADS)
Jia, Yue
Perovskite oxides span a diverse range of functional properties such as ferromagnetism, superconductivity, and ferroelectricity, which makes them promising candidate materials for applications such as sensors, energy conversion and data storage devices. With recent advances in thin film deposition techniques, the precise manipulation of atomic layers on the unit cell level make it possible to synthesize epitaxial thin film heterostructures consisting of layers with different properties. The structural compatibility of perovskite oxides allows them to be epitaxially grown in complex heterostructures such as superlattices with a large density of interfaces where the interplay between spin, charge, orbital, and lattice degrees of freedom gives rise to new behaviors. The ferromagnetic (FM)/antiferromagnetic (AF) interface is particularly interesting due to exchange coupling which is not only of interest for fundamental research but also is of great significance for industrial applications. Unlike metallic systems that have been studied for decades with wide ranges of applications in devices such as hard disk drives, thin films of complex metal oxides is a relatively new field. Perovskite oxides show much more diverse functional properties than metals and open new pathways for tailoring propertiestowards specific device applications. Epitaxial La0.7Sr0.3MnO3 (LSMO)/La 0.7Sr0.3FeO3 (LSFO) superlattices serve as model systems to explore the magnetic structure and exchange coupling at perovskite oxide interfaces. Earlier work suggested that (001)-oriented LSMO/LSFO superlattices with compensated AF spins at the interface display spin-flop coupling characterized by perpendicular alignment between the AF spin axes and the FM moments at a sublayer thickness of 6 unit cells (u.c.). Changing the crystallographic orientation of the interface from (001) to (111) introduces changes to factors such as the charge density of each stacking layer, the magnetic iiistructure of the AF layer at the interface, the symmetry of the lattice, and the orbital degeneracy. Therefore, different properties and exchange coupling mechanisms are expected. (111)-oriented LSMO/LSFO superlattices with sublayer thicknesses ranging from 3 to 60 u.c. were synthesized and characterized. Detailed analysis of their structural, electronic, and magnetic properties were performed using synchrotron radiation based resonant x-ray reflectivity, soft x-ray magnetic spectroscopy, and photoemission electron microscopy to explore the effect of sublayer thickness on the magnetic structure and exchange coupling at (111)-oriented perovskite oxide interfaces. Interfacial effects and ultrathin superlattice sublayers can stabilize orientations of the LSFO AF spin axis which differ from that of LSFO films and LSMO/LSFO bilayers. In the ultrathin limit (3 to 6 u.c.), it was found that the AF properties of the LSFO sublayers are preserved with an out-of-plane canting of the AF spin axis, while the FM properties of the LSMO sublayers are significantly depressed. For thicker LSFO layers (> 9 u.c.), the out-of-plane canting of the AF spin axis is only present in superlattices with thick LSMO sublayers. As a result, exchange coupling in the form of spin-flop coupling exists only in superlattices which display both robust ferromagnetism and out-of-plane canting of the AF spin axis. A portion of the AF moments can be reoriented by a moderate external magnetic field through spin-flop coupling with the FM LSMO sublayers that have low magnetocrystalline anisotropy in the (111) plane. The AF order in the spin-flop coupled superlattices was studied using angle-dependent x-ray magnetic linear dichroism. The AF order can be categorized into two types: majority of the AF moments cant out-of-the-plane of the film along the or directions depending on the LSFO layer thickness, while a minority portion lies within the (111) plane in different AF domains. The energy difference between domains with their spin axes along the in-plane or out-of-plane directions is small, and the magnetic order of AF thin films is far ivmore complex than in bulk LSFO. The complex AF structure in these (111)-oriented LSMO/LSFO superlattices illustrates that complex metal oxide heterostructures can serve as fertile ground for discovery of new magnetic phases, which have potential applications in next generation information technology devices.
Branch-point energies and the band-structure lineup at Schottky contacts and heterostrucures
NASA Astrophysics Data System (ADS)
Mönch, Winfried
2011-06-01
Empirical branch-point energies of Si, the group-III nitrides AlN, GaN, and InN, and the group-II and group-III oxides MgO, ZnO, Al2O3 and In2O3 are determined from experimental valance-band offsets of their heterostructures. For Si, GaN, and MgO, these values agree with the branch-point energies obtained from the barrier heights of their Schottky contacts. The empirical branch-point energies of Si and the group-III nitrides are in very good agreement with results of previously published calculations using quite different approaches such as the empirical tight-binding approximation and modern electronic-structure theory. In contrast, the empirical branch-point energies of the group-II and group-III oxides do not confirm the respective theoretical results. As at Schottky contacts, the band-structure lineup at heterostructures is also made up of a zero-charge-transfer term and an intrinsic electric-dipole contribution. Hence, valence-band offsets are not equal to the difference of the branch-point energies of the two semiconductors forming the heterostructure. The electric-dipole term may be described by the electronegativity difference of the two solids in contact. A detailed analysis of experimental Si Schottky barrier heights and heterostructure valence-band offsets explains and proves these conclusions.
Oh, Pilgun; Oh, Seung -Min; Li, Wangda; ...
2016-05-30
The Ni-rich layered oxides with a Ni content of >0.5 are drawing much attention recently to increase the energy density of lithium-ion batteries. However, the Ni-rich layered oxides suffer from aggressive reaction of the cathode surface with the organic electrolyte at the higher operating voltages, resulting in consequent impedance rise and capacity fade. To overcome this difficulty, we present here a heterostructure composed of a Ni-rich LiNi 0.7Co 0.15Mn 0.15O 2 core and a Li-rich Li 1.2-xNi 0.2Mn 0.6O 2 shell, incorporating the advantageous features of the structural stability of the core and chemical stability of the shell. With amore » unique chemical treatment for the activation of the Li 2MnO 3 phase of the shell, a high capacity is realized with the Li-rich shell material. Aberration-corrected scanning transmission electron microscopy (STEM) provides direct evidence for the formation of surface Li-rich shell layer. Finally, the heterostructure exhibits a high capacity retention of 98% and a discharge- voltage retention of 97% during 100 cycles with a discharge capacity of 190 mA h g -1 (at 2.0–4.5 V under C/3 rate, 1C = 200 mA g -1).« less
Zhong, Xiaoliang; Rungger, Ivan; Zapol, Peter; ...
2016-02-15
Reversible resistive switching between high-resistance and low-resistance states in metal-oxide-metal heterostructures makes them very interesting for applications in random access memories. While recent experimental work has shown that inserting a metallic "oxygen scavenger layer'' between the positive electrode and oxide improves device performance, the fundamental understanding of how the scavenger layer modifies the heterostructure properties is lacking. We use density functional theory to calculate thermodynamic properties and conductance of TiN/HfO 2/TiN heterostructures with and without a Ta scavenger layer. First, we show that Ta insertion lowers the formation energy of low-resistance states. Second, while the Ta scavenger layer reduces themore » Schottky barrier height in the high-resistance state by modifying the interface charge at the oxide-electrode interface, the heterostructure maintains a high resistance ratio between high-and low-resistance states. Lastly, we show that the low-bias conductance of device on-states becomes much less sensitive to the spatial distribution of oxygen removed from the HfO 2 in the presence of the Ta layer. By providing a fundamental understanding of the observed improvements with scavenger layers, we open a path to engineer interfaces with oxygen scavenger layers to control and enhance device performance. In turn, this may enable the realization of a non-volatile low-power memory technology with concomitant reduction in energy consumption by consumer electronics and offering significant benefits to society.« less
Greco, Giuseppe; Fiorenza, Patrick; Giannazzo, Filippo; Alberti, Alessandra; Roccaforte, Fabrizio
2014-01-17
In this paper, the structural and electrical modifications induced, in the nanoscale, by a rapid thermal oxidation process on AlGaN/GaN heterostructures, are investigated. A local rapid oxidation (900 ° C in O2, 10 min) localized under the anode region of an AlGaN/GaN diode enabled a reduction of the leakage current with respect to a standard Schottky contact. The insulating properties of the near-surface oxidized layer were probed by a nanoscale electrical characterization using scanning probe microscopy techniques. The structural characterization indicated the formation of a thin uniform oxide layer on the surface, with preferential oxidation paths along V-shaped defects penetrating through the AlGaN/GaN interface. The oxidation process resulted in an expansion of the lattice parameters due to the incorporation of oxygen atoms, accompanied by an increase of the crystal mosaicity. As a consequence, a decrease of the sheet carrier density of the two-dimensional electron gas and a positive shift of the threshold voltage are observed. The results provide useful insights for a possible future integration of rapid oxidation processes during GaN device fabrication.
Via Method for Lithography Free Contact and Preservation of 2D Materials.
Telford, Evan J; Benyamini, Avishai; Rhodes, Daniel; Wang, Da; Jung, Younghun; Zangiabadi, Amirali; Watanabe, Kenji; Taniguchi, Takashi; Jia, Shuang; Barmak, Katayun; Pasupathy, Abhay N; Dean, Cory R; Hone, James
2018-02-14
Atomically thin 2D materials span the common components of electronic circuits as metals, semiconductors, and insulators, and can manifest correlated phases such as superconductivity, charge density waves, and magnetism. An ongoing challenge in the field is to incorporate these 2D materials into multilayer heterostructures with robust electrical contacts while preventing disorder and degradation. In particular, preserving and studying air-sensitive 2D materials has presented a significant challenge since they readily oxidize under atmospheric conditions. We report a new technique for contacting 2D materials, in which metal via contacts are integrated into flakes of insulating hexagonal boron nitride, and then placed onto the desired conducting 2D layer, avoiding direct lithographic patterning onto the 2D conductor. The metal contacts are planar with the bottom surface of the boron nitride and form robust contacts to multiple 2D materials. These structures protect air-sensitive 2D materials for months with no degradation in performance. This via contact technique will provide the capability to produce "atomic printed circuit boards" that can form the basis of more complex multilayer heterostructures.
Dong, Yongqi; Xu, Haoran; Luo, Zhenlin; ...
2017-05-16
The effect of gate voltage polarity on the behavior of NdNiO 3 epitaxial thin films during ionic liquid gating is studied using in situ synchrotron X-ray techniques. We show that while negative biases have no discernible effect on the structure or composition of the films, large positive gate voltages result in the injection of a large concentration of oxygen vacancies (similar to 3%) and pronounced lattice expansion (0.17%) in addition to a 1000-fold increase in sheet resistance at room temperature. Despite the creation of large defect densities, the heterostructures exhibit a largely reversible switching behavior when sufficient time is providedmore » for the vacancies to migrate in and out of the thin film surface. The results confirm that electrostatic gating takes place at negative gate voltages for p-type complex oxides while positive voltages favor the electrochemical reduction of Ni 3+. Switching between positive and negative gate voltages therefore involves a combination of electronic and ionic doping processes that may be utilized in future electrochemical transistors.« less
NASA Astrophysics Data System (ADS)
Zheng, Ming; Xu, Xiao-Ke; Ni, Hao; Qi, Ya-Ping; Li, Xiao-Min; Gao, Ju
2018-03-01
The phase separation, i.e., the competition between coexisting multi-phases, can be adjusted by external stimuli, such as magnetic field, electric field, current, light, and strain. Here, a multiferroic heterostructure composed of a charge-ordered Nd0.5Sr0.5MnO3 thin film and a ferroelectric Pb(Mg1/3Nb2/3)O3-PbTiO3 single crystal is fabricated to investigate the lattice strain and magnetic field co-control of phase separation in resistive switching. The stable and nonvolatile resistance tuning is realized at room temperature using the electric-field-induced reversible ferroelastic strain effect, which can be enhanced by 84% under the magnetic field. Moreover, the magnetoresistance can be effectively tuned by the electrically driven ferroelastic strain. These findings reveal that the ferroelastic strain and the magnetic field strongly correlate with each other and are mediated by phase separation. Our work provides an approach to design strain-engineered multifunctional memory devices based on complex oxides by introducing an extra magnetic field stimulus.
General Considerations of the Electrostatic Boundary Conditions in Oxide Heterostructures
DOE Office of Scientific and Technical Information (OSTI.GOV)
Higuchi, Takuya
2011-08-19
When the size of materials is comparable to the characteristic length scale of their physical properties, novel functionalities can emerge. For semiconductors, this is exemplified by the 'superlattice' concept of Esaki and Tsu, where the width of the repeated stacking of different semiconductors is comparable to the 'size' of the electrons, resulting in novel confined states now routinely used in opto-electronics. For metals, a good example is magnetic/non-magnetic multilayer films that are thinner than the spin-scattering length, from which giant magnetoresistance (GMR) emerged, used in the read heads of hard disk drives. For transition metal oxides, a similar research programmore » is currently underway, broadly motivated by the vast array of physical properties that they host. This long-standing notion has been recently invigorated by the development of atomic-scale growth and probe techniques, which enables the study of complex oxide heterostructures approaching the precision idealized in Fig. 1(a). Taking the subset of oxides derived from the perovskite crystal structure, the close lattice match across many transition metal oxides presents the opportunity, in principle, to develop a 'universal' heteroepitaxial materials system. Hand-in-hand with the continual improvements in materials control, an increasingly relevant challenge is to understand the consequences of the electrostatic boundary conditions which arise in these structures. The essence of this issue can be seen in Fig. 1(b), where the charge sequence of the sublayer 'stacks' for various representative perovskites is shown in the ionic limit, in the (001) direction. To truly 'universally' incorporate different properties using different materials components, be it magnetism, ferroelectricity, superconductivity, etc., it is necessary to access and join different charge sequences, labelled here in analogy to the designations 'group IV, III-V, II-VI' for semiconductors. As we will review, interfaces between different families creates a host of electrostatic issues. They can be somewhat avoided if, as in many semiconductor heterostructures, only one family is used, with small perturbations (such as n-type or p-type doping) around them. However, for most transition metal oxides, this is greatly restrictive. For example, LaMnO{sub 3} and SrMnO{sub 3} are both insulators in part due to strong electron correlations, and only in their solid solution does 'colossal magnetoresistance' emerge in bulk. Similarly, the metallic superlattice shown in Fig. 1(c) can be considered a nanoscale deconstruction of (La,Sr)TiO{sub 3} to the insulating parent compounds. Therefore the aspiration to arbitrarily mix and match perovskite components requires a basic understanding of, and ultimately control over, these issues. In this context, here we present basic electrostatic features that arise in oxide heterostructures which vary the ionic charge stacking sequence. In close relation to the analysis of the stability of polar surfaces and semiconductor heterointerfaces, the variation of the dipole moment across a heterointerface plays a key role in determining its stability. Different self-consistent assignments of the unit cell are presented, allowing the polar discontinuity picture to be recast in terms of an equivalent local charge neutrality picture. The latter is helpful in providing a common framework with which to discuss electronic reconstructions, local-bonding considerations, crystalline defects, and lattice polarization on an equal footing, all of which are the subject of extensive current investigation.« less
NASA Astrophysics Data System (ADS)
Dai, Wen-Wu; Zhao, Zong-Yan
2017-06-01
Heterostructure constructing is a feasible and powerful strategy to enhance the performance of photocatalysts, because they can be tailored to have desirable photo-electronics properties and couple distinct advantageous of components. As a novel layered photocatalyst, the main drawback of BiOI is the low edge position of the conduction band. To address this problem, it is meaningful to find materials that possess suitable band gap, proper band edge position, and high mobility of carrier to combine with BiOI to form hetertrostructure. In this study, graphene-based materials (including: graphene, graphene oxide, and g-C3N4) were chosen as candidates to achieve this purpose. The charge transfer, interface interaction, and band offsets are focused on and analyzed in detail by DFT calculations. Results indicated that graphene-based materials and BiOI were in contact and formed van der Waals heterostructures. The valence and conduction band edge positions of graphene oxide, g-C3N4 and BiOI changed with the Fermi level and formed the standard type-II heterojunction. In addition, the overall analysis of charge density difference, Mulliken population, and band offsets indicated that the internal electric field is facilitate for the separation of photo-generated electron-hole pairs, which means these heterostructures can enhance the photocatalytic efficiency of BiOI. Thus, BiOI combines with 2D materials to construct heterostructure not only make use of the unique high electron mobility, but also can adjust the position of energy bands and promote the separation of photo-generated carriers, which provide useful hints for the applications in photocatalysis.
Orbital Engineering in Symmetry-Breaking Polar Heterostructures
NASA Astrophysics Data System (ADS)
Disa, Ankit S.; Kumah, Divine P.; Malashevich, Andrei; Chen, Hanghui; Arena, Dario A.; Specht, Eliot D.; Ismail-Beigi, Sohrab; Walker, F. J.; Ahn, Charles H.
2015-01-01
We experimentally demonstrate a novel approach to substantially modify orbital occupations and symmetries in electronically correlated oxides. In contrast to methods using strain or confinement, this orbital tuning is achieved by exploiting charge transfer and inversion symmetry breaking using atomically layered heterostructures. We illustrate the technique in the LaTiO3-LaNiO3-LaAlO3 system; a combination of x-ray absorption spectroscopy and ab initio theory reveals electron transfer and concomitant polar fields, resulting in a ˜50 % change in the occupation of Ni d orbitals. This change is sufficiently large to remove the orbital degeneracy of bulk LaNiO3 and creates an electronic configuration approaching a single-band Fermi surface. Furthermore, we theoretically show that such three-component heterostructuring is robust and tunable by choice of insulator in the heterostructure, providing a general method for engineering orbital configurations and designing novel electronic systems.
NASA Astrophysics Data System (ADS)
Li, Delong; Gong, Youning; Wang, Miaosheng; Pan, Chunxu
2017-04-01
A kind of sandwich-like NiCo2O4/rGO/NiO heterostructure composite has been successfully anchored on nickel foam substrate via a three-step hydrothermal method with successive annealing treatment. The smart combination of NiCo2O4, reduced graphene oxide (rGO), and NiO nanostructure in the sandwich-like nano architecture shows a promising synergistic effect for supercapacitors with greatly enhanced electrochemical performance. For serving as supercapacitor electrode, the NiCo2O4/rGO/NiO heterostructure materials exhibit remarkable specific capacitance of 2644 mF cm-2 at current density of 1 mA cm-2, and excellent capacitance retentions of 97.5% after 3000 cycles. It is expected that the present heterostructure will be a promising electrode material for high-performance supercapacitors.
Rare-earth nickelates RNiO3: thin films and heterostructures
NASA Astrophysics Data System (ADS)
Catalano, S.; Gibert, M.; Fowlie, J.; Íñiguez, J.; Triscone, J.-M.; Kreisel, J.
2018-04-01
This review stands in the larger framework of functional materials by focussing on heterostructures of rare-earth nickelates, described by the chemical formula RNiO3 where R is a trivalent rare-earth R = La, Pr, Nd, Sm, …, Lu. Nickelates are characterized by a rich phase diagram of structural and physical properties and serve as a benchmark for the physics of phase transitions in correlated oxides where electron–lattice coupling plays a key role. Much of the recent interest in nickelates concerns heterostructures, that is single layers of thin film, multilayers or superlattices, with the general objective of modulating their physical properties through strain control, confinement or interface effects. We will discuss the extensive studies on nickelate heterostructures as well as outline different approaches to tuning and controlling their physical properties and, finally, review application concepts for future devices.
Rare-earth nickelates RNiO3: thin films and heterostructures.
Catalano, S; Gibert, M; Fowlie, J; Íñiguez, J; Triscone, J-M; Kreisel, J
2018-04-01
This review stands in the larger framework of functional materials by focussing on heterostructures of rare-earth nickelates, described by the chemical formula RNiO 3 where R is a trivalent rare-earth R = La, Pr, Nd, Sm, …, Lu. Nickelates are characterized by a rich phase diagram of structural and physical properties and serve as a benchmark for the physics of phase transitions in correlated oxides where electron-lattice coupling plays a key role. Much of the recent interest in nickelates concerns heterostructures, that is single layers of thin film, multilayers or superlattices, with the general objective of modulating their physical properties through strain control, confinement or interface effects. We will discuss the extensive studies on nickelate heterostructures as well as outline different approaches to tuning and controlling their physical properties and, finally, review application concepts for future devices.
Frisenda, Riccardo; Navarro-Moratalla, Efrén; Gant, Patricia; Pérez De Lara, David; Jarillo-Herrero, Pablo; Gorbachev, Roman V; Castellanos-Gomez, Andres
2018-01-02
Designer heterostructures can now be assembled layer-by-layer with unmatched precision thanks to the recently developed deterministic placement methods to transfer two-dimensional (2D) materials. This possibility constitutes the birth of a very active research field on the so-called van der Waals heterostructures. Moreover, these deterministic placement methods also open the door to fabricate complex devices, which would be otherwise very difficult to achieve by conventional bottom-up nanofabrication approaches, and to fabricate fully-encapsulated devices with exquisite electronic properties. The integration of 2D materials with existing technologies such as photonic and superconducting waveguides and fiber optics is another exciting possibility. Here, we review the state-of-the-art of the deterministic placement methods, describing and comparing the different alternative methods available in the literature, and we illustrate their potential to fabricate van der Waals heterostructures, to integrate 2D materials into complex devices and to fabricate artificial bilayer structures where the layers present a user-defined rotational twisting angle.
NASA Astrophysics Data System (ADS)
Supee, A.; Ichimura, M.
2017-12-01
Heterostructures which consist of ZnO and FeS x O y were deposited via electrochemical deposition (ECD) for application to solar cells. Galvanostatic ECD was used in FeS x O y deposition with a solution containing 100 mM Na2S2O3 and 30 mM FeSO4. To alter the film properties, L(+)-tartaric acid (C4H6O6) and lactic acid [CH3CH(OH)COOH] were introduced as the complexing agents into the FeS x O y deposition solution. Larger film thickness and smaller oxygen content were obtained for the films deposited with the complexing agents. ZnO was deposited on FeS x O y by two-step pulse ECD from a solution containing Zn(NO3)2. For the ZnO/FeS x O y heterostructures fabricated with/without complexing agents, rectifying properties were confirmed in the current density-voltage ( J- V) characteristics. However, photovoltaic properties were not improved with addition of both complexing agents.
Polarity-driven oxygen vacancy formation in ultrathin LaNiO 3 films on SrTiO 3
Tung, I-Cheng; Luo, Guangfu; Lee, June Hyuk; ...
2017-10-18
Oxide heterostructures offer a pathway to control emergent phases in complex oxides, but their creation often leads to boundaries that have a polar discontinuity. In order to fabricate atomic-scale arrangements of dissimilar materials, we need a clear understanding of the pathways by which materials resolve polarity issues. By examining the real-time lattice structure in-situ during growth for the case of polar LaNiO 3 synthesized on non-polar SrTiO 3 (001), we demonstrate how films in ultra-thin limit form as LaNiO 2.5 and then evolve into LaNiO 3 as the thickness increases. Theory explains how the polar energetics drives the formation ofmore » oxygen vacancies and the stability of these phases with thickness and structure.« less
Emerging magnetism and anomalous Hall effect in iridate–manganite heterostructures
Nichols, John; Gao, Xiang; Lee, Shinbuhm; ...
2016-09-06
We know strong Coulomb repulsion and spin–orbit coupling to give rise to exotic physical phenomena in transition metal oxides. Initial attempts to investigate systems, where both of these fundamental interactions are comparably strong, such as 3d and 5d complex oxide superlattices, have revealed properties that only slightly differ from the bulk ones of the constituent materials. Furthermore, we observe that the interfacial coupling between the 3d antiferromagnetic insulator SrMnO 3 and the 5d paramagnetic metal SrIrO 3 is enormously strong, yielding an anomalous Hall response as the result of charge transfer driven interfacial ferromagnetism. Our findings show that low dimensionalmore » spin–orbit entangled 3d–5d interfaces provide an avenue to uncover technologically relevant physical phenomena unattainable in bulk materials.« less
Disentangled Cooperative Orderings in Artificial Rare-Earth Nickelates.
Middey, S; Meyers, D; Kareev, M; Cao, Yanwei; Liu, X; Shafer, P; Freeland, J W; Kim, J-W; Ryan, P J; Chakhalian, J
2018-04-13
Coupled transitions between distinct ordered phases are important aspects behind the rich phase complexity of correlated oxides that hinder our understanding of the underlying phenomena. For this reason, fundamental control over complex transitions has become a leading motivation of the designer approach to materials. We have devised a series of new superlattices by combining a Mott insulator and a correlated metal to form ultrashort period superlattices, which allow one to disentangle the simultaneous orderings in RENiO_{3}. Tailoring an incommensurate heterostructure period relative to the bulk charge ordering pattern suppresses the charge order transition while preserving metal-insulator and antiferromagnetic transitions. Such selective decoupling of the entangled phases resolves the long-standing puzzle about the driving force behind the metal-insulator transition and points to the site-selective Mott transition as the operative mechanism. This designer approach emphasizes the potential of heterointerfaces for selective control of simultaneous transitions in complex materials with entwined broken symmetries.
Disentangled Cooperative Orderings in Artificial Rare-Earth Nickelates
NASA Astrophysics Data System (ADS)
Middey, S.; Meyers, D.; Kareev, M.; Cao, Yanwei; Liu, X.; Shafer, P.; Freeland, J. W.; Kim, J.-W.; Ryan, P. J.; Chakhalian, J.
2018-04-01
Coupled transitions between distinct ordered phases are important aspects behind the rich phase complexity of correlated oxides that hinder our understanding of the underlying phenomena. For this reason, fundamental control over complex transitions has become a leading motivation of the designer approach to materials. We have devised a series of new superlattices by combining a Mott insulator and a correlated metal to form ultrashort period superlattices, which allow one to disentangle the simultaneous orderings in RENiO3 . Tailoring an incommensurate heterostructure period relative to the bulk charge ordering pattern suppresses the charge order transition while preserving metal-insulator and antiferromagnetic transitions. Such selective decoupling of the entangled phases resolves the long-standing puzzle about the driving force behind the metal-insulator transition and points to the site-selective Mott transition as the operative mechanism. This designer approach emphasizes the potential of heterointerfaces for selective control of simultaneous transitions in complex materials with entwined broken symmetries.
Band gap and mobility of epitaxial perovskite BaSn1 -xHfxO3 thin films
NASA Astrophysics Data System (ADS)
Shin, Juyeon; Lim, Jinyoung; Ha, Taewoo; Kim, Young Mo; Park, Chulkwon; Yu, Jaejun; Kim, Jae Hoon; Char, Kookrin
2018-02-01
A wide band-gap perovskite oxide BaSn O3 is attracting much attention due to its high electron mobility and oxygen stability. On the other hand, BaHf O3 was recently reported to be an effective high-k gate oxide. Here, we investigate the band gap and mobility of solid solutions of BaS n1 -xH fxO3 (x =0 -1 ) (BSHO) as a basis to build advanced perovskite oxide heterostructures. All the films were epitaxially grown on MgO substrates using pulsed laser deposition. Density functional theory calculations confirmed that Hf substitution does not create midgap states while increasing the band gap. From x-ray diffraction and optical transmittance measurements, the lattice constants and the band-gap values are significantly modified by Hf substitution. We also measured the transport properties of n -type La-doped BSHO films [(Ba ,La ) (Sn ,Hf ) O3 ] , investigating the feasibility of modulation doping in the BaSn O3/BSHO heterostructures. The Hall measurement data revealed that, as the Hf content increases, the activation rate of the La dopant decreases and the scattering rate of the electrons sharply increases. These properties of BSHO films may be useful for applications in various heterostructures based on the BaSn O3 system.
NASA Astrophysics Data System (ADS)
Han, M. J.; Marianetti, C. A.; Millis, A. J.
2010-10-01
The application of modern layer-by-layer growth techniques to transition-metal oxide materials raises the possibility of creating new classes of materials with rationally designed correlated electron properties. An important step toward this goal is the demonstration that electronic structure can be controlled by atomic composition. In compounds with partially occupied transition-metal d shells, one important aspect of the electronic structure is the relative occupancy of different d orbitals. Previous work has established that strain and quantum confinement can be used to influence orbital occupancy. In this paper we demonstrate a different modality for orbital control in transition-metal oxide heterostructures, using density-functional band calculations supplemented by a tight-binding analysis to show that the choice of nontransition-metal counterion X in transition-metal oxide heterostructures composed of alternating LaNiO3 and LaXO3 units strongly affects orbital occupancy, changing the magnitude and in some cases the sign of the orbital polarization.
Strongly enhanced Rashba splittings in an oxide heterostructure: A tantalate monolayer on BaHfO 3
Kim, Minsung; Ihm, Jisoon; Chung, Suk Bum
2016-09-22
In the two-dimensional electron gas emerging at the transition metal oxide surface and interface, various exotic electronic ordering and topological phases can become experimentally more accessible with the stronger Rashba spin-orbit interaction. Here, we present a promising route to realize significant Rashba-type band splitting using a thin film heterostructure. Based on first-principles methods and analytic model analyses, a tantalate monolayer on BaHfO 3 is shown to host two-dimensional bands originating from Ta t 2g states with strong Rashba spin splittings, nearly 10% of the bandwidth, at both the band minima and saddle points. An important factor in this enhanced splittingmore » is the significant t 2g–e g interband coupling, which can generically arise when the inversion symmetry is maximally broken due to the strong confinement of the 2DEG on a transition metal oxide surface. Here, our results could be useful in realizing topological superconductivity at oxide surfaces.« less
DOE Office of Scientific and Technical Information (OSTI.GOV)
Lu, Di; Baek, David J.; Hong, Seung Sae
2016-08-22
The ability to create and manipulate materials in two-dimensional (2D) form has repeatedly had transformative impact on science and technology. In parallel with the exfoliation and stacking of intrinsically layered crystals, atomic-scale thin film growth of complex materials has enabled the creation of artificial 2D heterostructures with novel functionality and emergent phenomena, as seen in perovskite heterostructures. However, separation of these layers from the growth substrate has proven challenging, limiting the manipulation capabilities of these heterostructures with respect to exfoliated materials. Here we present a general method to create freestanding perovskite membranes. The key is the epitaxial growth of water-solublemore » Sr 3Al 2O 6 on perovskite substrates, followed by in situ growth of films and heterostructures. Millimetre-size single-crystalline membranes are produced by etching the Sr 3Al 2O 6 layer in water, providing the opportunity to transfer them to arbitrary substrates and integrate them with heterostructures of semiconductors and layered compounds.« less
Han, Jinkyu; McBean, Coray; Wang, Lei; ...
2015-01-30
In this report, we synthesize and characterize the structural and optical properties of novel heterostructures composed of (i) semiconducting nanocrystalline CdSe quantum dot (QDs) coupled with (ii) both one and zero-dimensional (1D and 0D) motifs of self-activated luminescence CaWO₄ metal oxides. Specifically, ~4 nm CdSe QDs have been anchored onto (i) high-aspect ratio 1D nanowires, measuring ~230 nm in diameter and ~3 μm in length, as well as onto (ii) crystalline 0D nanoparticles (possessing an average diameter of ~ 80 nm) of CaWO₄ through the mediation of 3-mercaptopropionic acid (MPA) as a connecting linker. Composite formation was confirmed by complementarymore » electron microscopy and spectroscopy (i.e. IR and Raman) data. In terms of luminescent properties, our results show that our 1D and 0D heterostructures evince photoluminescence (PL) quenching and shortened PL lifetimes of CaWO₄ as compared with unbound CaWO₄. We propose that a photo-induced electron transfer process occurs from CaWO₄ to CdSe QDs, a scenario which has been confirmed by NEXAFS measurements and which highlights a decrease in the number of unoccupied orbitals in the conduction bands of CdSe QDs. By contrast, the PL signature and lifetimes of MPA-capped CdSe QDs within these heterostructures do not exhibit noticeable changes as compared with unbound MPA-capped CdSe QDs. The striking difference in optical behavior between CaWO₄ nanostructures and CdSe QDs within our heterostructures can be correlated with the relative positions of their conduction and valence energy band levels. In addition, the PL quenching behaviors for CaWO₄ within the heterostructure configuration were examined by systematically varying (i) the quantities and coverage densities of CdSe QDs as well as (ii) the intrinsic morphology (and by extension, the inherent crystallite size) of CaWO₄ itself.« less
Electronic Interfacial Effects in Epitaxial Heterostructures based on LaMnO3.
NASA Astrophysics Data System (ADS)
Christen, Hans M.; Varela, M.; Lee, H. N.; Kim, D. H.; Chisholm, M. F.; Cantoni, C.; Petit, L.; Schulthess, T. C.; Lowndes, D. H.
2006-03-01
Studies of chemically abrupt interfaces provide an ideal platform to study the effects of discontinuities and asymmetries of the electronic configuration on the transport and magnetic properties of complex oxides. In addition, the behavior of complex materials near interfaces plays the most crucial role not only in devices and nanostructures but also in complex structures in the form of composites and superlattices, including artificial multiferroics. Interfaces in the ABO3 perovskite system are particularly attractive because structurally similar oxides with fundamentally different physical properties can be integrated epitaxially. To explore the electronic effects at interfaces and to probe the physical properties that result from local electronic changes, we have synthesized structures containing LaMnO3 and insulating perovskites using pulsed laser deposition. The local electron energy loss spectroscopy (EELS) capability of a scanning transmission electron microscope (STEM) is used to probe the electronic configuration in the LaMnO3 films as a function of the distance from the interfaces. The results are compared to macroscopic measurements and theoretical predictions. Research sponsored by the U.S. Department of Energy under contract DE-AC05-00OR22725 with the Oak Ridge National Laboratory, managed by UT-Battelle, LLC.
Trilayer TMDC Heterostructures for MOSFETs and Nanobiosensors
NASA Astrophysics Data System (ADS)
Datta, Kanak; Shadman, Abir; Rahman, Ehsanur; Khosru, Quazi D. M.
2017-02-01
Two dimensional materials such as transition metal dichalcogenides (TMDC) and their bi-layer/tri-layer heterostructures have become the focus of intense research and investigation in recent years due to their promising applications in electronics and optoelectronics. In this work, we have explored device level performance of trilayer TMDC heterostructure (MoS2/MX2/MoS2; M = Mo or, W and X = S or, Se) metal oxide semiconductor field effect transistors (MOSFETs) in the quantum ballistic regime. Our simulation shows that device `on' current can be improved by inserting a WS2 monolayer between two MoS2 monolayers. Application of biaxial tensile strain reveals a reduction in drain current which can be attributed to the lowering of carrier effective mass with increased tensile strain. In addition, it is found that gate underlap geometry improves electrostatic device performance by improving sub-threshold swing. However, increase in channel resistance reduces drain current. Besides exploring the prospect of these materials in device performance, novel trilayer TMDC heterostructure double gate field effect transistors (FETs) are proposed for sensing Nano biomolecules as well as for pH sensing. Bottom gate operation ensures these FETs operating beyond Nernst limit of 59 mV/pH. Simulation results found in this work reveal that scaling of bottom gate oxide results in better sensitivity while top oxide scaling exhibits an opposite trend. It is also found that, for identical operating conditions, proposed TMDC FET pH sensors show super-Nernst sensitivity indicating these materials as potential candidates in implementing such sensor. Besides pH sensing, all these materials show high sensitivity in the sub-threshold region as a channel material in nanobiosensor while MoS2/WS2/MoS2 FET shows the least sensitivity among them.
NASA Astrophysics Data System (ADS)
Liao, P. H.; Peng, K. P.; Lin, H. C.; George, T.; Li, P. W.
2018-05-01
We report channel and strain engineering of self-organized, gate-stacking heterostructures comprising Ge-nanosphere gate/SiO2/SiGe-channels. An exquisitely-controlled dynamic balance between the concentrations of oxygen, Si, and Ge interstitials was effectively exploited to simultaneously create these heterostructures in a single oxidation step. Process-controlled tunability of the channel length (5–95 nm diameters for the Ge-nanospheres), gate oxide thickness (2.5–4.8 nm), as well as crystal orientation, chemical composition and strain engineering of the SiGe-channel was achieved. Single-crystalline (100) Si1‑x Ge x shells with Ge content as high as x = 0.85 and with a compressive strain of 3%, as well as (110) Si1‑x Ge x shells with Ge content of x = 0.35 and corresponding compressive strain of 1.5% were achieved. For each crystal orientation, our high Ge-content, highly-stressed SiGe shells feature a high degree of crystallinity and thus, provide a core ‘building block’ required for the fabrication of Ge-based MOS devices.
Liao, P H; Peng, K P; Lin, H C; George, T; Li, P W
2018-05-18
We report channel and strain engineering of self-organized, gate-stacking heterostructures comprising Ge-nanosphere gate/SiO 2 /SiGe-channels. An exquisitely-controlled dynamic balance between the concentrations of oxygen, Si, and Ge interstitials was effectively exploited to simultaneously create these heterostructures in a single oxidation step. Process-controlled tunability of the channel length (5-95 nm diameters for the Ge-nanospheres), gate oxide thickness (2.5-4.8 nm), as well as crystal orientation, chemical composition and strain engineering of the SiGe-channel was achieved. Single-crystalline (100) Si 1-x Ge x shells with Ge content as high as x = 0.85 and with a compressive strain of 3%, as well as (110) Si 1-x Ge x shells with Ge content of x = 0.35 and corresponding compressive strain of 1.5% were achieved. For each crystal orientation, our high Ge-content, highly-stressed SiGe shells feature a high degree of crystallinity and thus, provide a core 'building block' required for the fabrication of Ge-based MOS devices.
Optically-Induced Persistent Magnetization in Oxygen Deficient Strontium Titanate
NASA Astrophysics Data System (ADS)
Crooker, Scott
2015-03-01
Interest in electronics and spintronics based on complex oxide materials has exploded in recent years, fueled by the ability to grow atomically-precise heterostructures of various oxides 1. A foundational material in this burgeoning field is strontium titanate, a (nominally) non-magnetic wide-bandgap semiconductor. Owing to its ubiquity in oxide materials science, studies of SrTiO3's interesting dielectric, lattice, and optical properties represent mature research areas. However, renewed interest in SrTiO3 was recently sparked by observations of unexpected spin and magnetization phenomena at interfaces between SrTiO3 and other nonmagnetic oxides 1. The formation and distribution of oxygen vacancies (VO) in SrTiO3 are widely thought to play an essential but as-yet-incompletely understood role in these emergent phenomena. Here we demonstrate a surprising new aspect to the phenomenology of magnetism in SrTiO3 by reporting the observation of an optically-induced and persistent magnetization in slightly oxygen-deficient SrTiO3-δ bulk crystals, using magnetic circular dichroism spectroscopy and optically-coupled SQUID studies 2. This magnetization appears below 18K, persists for hours below 10K, and is tunable via the polarization and wavelength of sub-bandgap (400-500 nm) light. As such, magnetic patterns can be ``written'' into SrTiO3-δ, and subsequently read out, using light alone. This magnetism occurs only in crystals containing VO, and is consistent with a metastable spin polarization of VO-related defect complexes. These data reveal a detailed interplay between magnetism, lattice defects, and light in an archetypal complex oxide material, which may yield new insights into the recent exciting spin physics observed at oxide interfaces.
Probing 1D superlattices at the LaAlO3 / SrTiO3 interface
NASA Astrophysics Data System (ADS)
Briggeman, M.; Huang, M.; Tylan-Tyler, A.; Irvin, P.; Levy, J.; Lee, J.-W.; Lee, H.; Eom, C.-B.
Complex oxides and other quantum systems exhibit behavior that is currently too complex to be understood using analytic or computational methods. One approach is to use a configurable quantum system whose Hamiltonian can be mapped onto the system of interest. This approach, known as quantum simulation, requires a rich physical system whose quanta and interactions can be controlled precisely, at the level of single electrons and other degrees of freedom. Here we describe steps toward developing a quantum simulation platform, using the complex oxide heterostructure LaAlO3 / SrTiO3 , by creating quantum systems with features comparable to the mean spacing between electrons. This interface has strong, sign changing, gate-tunable electron-electron interactions that can strongly influence the quantum ground state. We explore the magnetotransport properties of 1D superlattices, where periodic modulation produces reproducible dispersive features not seen in control structures. The results of these experiments can be compared with effective 1D model Hamiltonians to bridge experiment and theory and enable quantum simulation of more complex systems. We gratefully acknowledge financial support from AFOSR (FA9550-12-1- 0057 (JL) and FA9550-12-1-0342 (CBE)), ONR N00014-15-1-2847 (JL), and NSF DMR-1234096 (CBE).
Resistive and Capacitive Memory Effects in Oxide Insulator/ Oxide Conductor Hetero-Structures
NASA Astrophysics Data System (ADS)
Meyer, Rene; Miao, Maosheng; Wu, Jian; Chevallier, Christophe
2013-03-01
We report resistive and capacitive memory effects observed in oxide insulator/ oxide conductor hetero-structures. Electronic transport properties of Pt/ZrO2/PCMO/Pt structures with ZrO2 thicknesses ranging from 20A to 40A are studied before and after applying short voltage pulses of positive and negative polarity for set and reset operation. As processed devices display a non-linear IV characteristic which we attribute to trap assisted tunneling through the ZrO2 tunnel oxide. Current scaling with electrode area and tunnel oxide thickness confirms uniform conduction. The set/reset operation cause an up/down shift of the IV characteristic indicating that the conduction mechanism of both states is still dominated by tunneling. A change in the resistance is associated with a capacitance change of the device. An exponential relation between program voltages and set times is found. A model based on electric field mediated non-linear transport of oxygen ions across the ZrO2/PCMO interface is proposed. The change in the tunnel current is explained by ionic charge transfer between tunnel oxide and conductive metal oxide changing both tunnel barrier height and PCMO conductivity. DFT techniques are employed to explain the conductivity change in the PCMO interfacial layer observed through capacitance measurements.
NASA Astrophysics Data System (ADS)
Dong, Zhizhong; Huo, Di; Kear, Bernard H.; Tse, Stephen D.
2015-12-01
Heterostructures of tungsten-oxide nanowires decorated with zinc/tin-oxide nanostructures are synthesized via a combined flame and solution synthesis approach. Vertically well-aligned tungsten-oxide nanowires are grown on a tungsten substrate by a flame synthesis method. Here, tetragonal WO2.9 nanowires (diameters of 20-50 nm, lengths >10 μm, and coverage density of 109-1010 cm-2) are produced by the vapor-solid mechanism at 1720 K. Various kinds of Zn/Sn-oxide nanostructures are grown or deposited on the WO2.9 nanowires by adjusting the Sn2+ : Zn2+ molar ratio in an aqueous ethylenediamine solution at 65 °C. With WO2.9 nanowires serving as the base structures, sequential growth or deposition on them of hexagonal ZnO nanoplates, Zn2SnO4 nanocubes, and SnO2 nanoparticles are attained for Sn2+ : Zn2+ ratios of 0 : 1, 1 : 10, and 10 : 1, respectively, along with different saturation conditions. High-resolution transmission electron microscopy of the interfaces at the nanoheterojunctions shows abrupt interfaces for ZnO/WO2.9 and Zn2SnO4/WO2.9, despite lattice mismatches of >20%.
2011-07-06
biaxial compressive strain is known to split the light- and heavy-hole bands, reducing the interband scattering and causing the light hole band to move up...and heterostructure design are presented. In Section V, we use temperature- dependent measurements and pulsed I-V measurements to analyze the results...minimal in our devices. The temperature dependence of hole mobility was stud- ied for both the surface and buried channel devices, as plot- ted in Fig
Thomas Edwin Beechem; McDonald, Anthony E.; Ohta, Taisuke; ...
2015-10-26
Oxidation of exfoliated gallium selenide (GaSe) is investigated through Raman, photoluminescence, Auger, and X-ray photoelectron spectroscopies. Photoluminescence and Raman intensity reductions associated with spectral features of GaSe are shown to coincide with the emergence of signatures emanating from the by-products of the oxidation reaction, namely, Ga 2Se 3 and amorphous Se. Furthermore, photoinduced oxidation is initiated over a portion of a flake highlighting the potential for laser based patterning of two-dimensional heterostructures via selective oxidation.
Time-spliced X-ray diffraction imaging of magnetism dynamics in a NdNiO3 thin film
NASA Astrophysics Data System (ADS)
Beyerlein, Kenneth R.
2018-03-01
Diffraction imaging of nonequilibrium dynamics at atomic resolution is becoming possible with X-ray free-electron lasers. However, there are unresolved problems with applying this method to objects that are confined in only one dimension. Here I show that reliable one-dimensional coherent diffraction imaging is possible by splicing together images recovered from different time delays in an optical pump X-ray probe experiment. The time and space evolution of antiferromagnetic order in a vibrationally excited complex oxide heterostructure is recovered from time-resolved measurements of a resonant soft X-ray diffraction peak. Midinfrared excitation of the substrate is shown to lead to a demagnetization front that propagates at a velocity exceeding the speed of sound, a critical observation for the understanding of driven phase transitions in complex condensed matter.
Time-spliced X-ray diffraction imaging of magnetism dynamics in a NdNiO3 thin film.
Beyerlein, Kenneth R
2018-02-27
Diffraction imaging of nonequilibrium dynamics at atomic resolution is becoming possible with X-ray free-electron lasers. However, there are unresolved problems with applying this method to objects that are confined in only one dimension. Here I show that reliable one-dimensional coherent diffraction imaging is possible by splicing together images recovered from different time delays in an optical pump X-ray probe experiment. The time and space evolution of antiferromagnetic order in a vibrationally excited complex oxide heterostructure is recovered from time-resolved measurements of a resonant soft X-ray diffraction peak. Midinfrared excitation of the substrate is shown to lead to a demagnetization front that propagates at a velocity exceeding the speed of sound, a critical observation for the understanding of driven phase transitions in complex condensed matter.
NASA Astrophysics Data System (ADS)
Mori, Ryo; Marshall, Patrick; Isaac, Brandon; Denlinger, Jonathan; Stemmer, Susanne; Lanzara, Alessandra
The confined electron system in the quantum well of the transition metal oxide, SrTiO3, embedded in the rare earth titanate, SmTiO3, shows unique properties, such as high carrier density, fermi liquid to non-fermi liquid transition, and pseudo-gap, which can be controlled by changing the shape of the quantum well. We will present a distinct difference in the electronic structures between the different quantum well structures obtained by angle-resolved photoemission spectroscopy (ARPES) measurements, suggesting the possibility to control the orbital character and the electron correlation near the interface as well as carrier density. The work was supported by the Quantum Materials Program at LBNL, funded by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, Materials Sciences and Engineering Division, under Contract No. DE-AC02-05CH11231.
Nanoscale control of oxide interface conduction in graphene-complex-oxide heterostructures
NASA Astrophysics Data System (ADS)
Huang, Mengchen; Ryu, Sangwoo; Ghahari, Fereshte; Jnawali, Giriraj; Ravichandran, Jayakanth; Irvin, Patrick; Kim, Philip; Eom, Chang-Beom; Levy, Jeremy
2014-03-01
Graphene is a promising material for high-speed optoelectronic devices such as THz modulators and detectors. Recently, broadband THz emission and detection can be achieved with nanostructures at the LaAlO3/SrTiO3 interface [2]. We have mechanically exfoliated single layer and multilayer graphene on top of 3.4 unit cell LaAlO3/SrTiO3 and successfully sketched nanowires in the 2DEG underneath graphene using conductive AFM lithgraphy [3]. Raman and AFM investigations confirm that the graphene quality and surface morphology remain unaltered by the writing process. These first experimental demonstrations of integrating graphene and LaAlO3/SrTiO3 are promising for future DC-THz photonic applications. We gratefully acknowledge support for this work from ONR (N00014-13-1-0806), NSF(DMR-1124131, DMR-1104191), and AFOSR (FA9550-12-1-0342).
He, Qing Lin; Lai, Ying Hoi; Lu, Yao; Law, Kam Tuen; Sou, Iam Keong
2013-01-01
We present a study of the surface reactivity of a Pd/Bi2Te3 thin film heterostructure. The topological surface states from Bi2Te3, being delocalized and robust owing to their topological natures, were found to act as an effective electron bath that significantly enhances the surface reactivity of palladium in the presence of two oxidizing agents, oxygen and tellurium respectively, which is consistent with a theoretical calculation. The surface reactivity of the adsorbed tellurium on this heterostructure is also intensified possibly benefitted from the effective transfer of the bath electrons. A partially inserted iron ferromagnetic layer at the interface of this heterostructure was found to play two competing roles arising from the higher-lying d-band center of the Pd/Fe bilayer and the interaction between the ferromagnetism and the surface spin texture of Bi2Te3 on the surface reactivity and their characteristics also demonstrate that the electron bath effect is long-lasting against accumulated thickness of adsorbates. PMID:23970163
Transfer matrix approach to electron transport in monolayer MoS2/MoO x heterostructures
NASA Astrophysics Data System (ADS)
Li, Gen
2018-05-01
Oxygen plasma treatment can introduce oxidation into monolayer MoS2 to transfer MoS2 into MoO x , causing the formation of MoS2/MoO x heterostructures. We find the MoS2/MoO x heterostructures have the similar geometry compared with GaAs/Ga1‑x Al x As semiconductor superlattice. Thus, We employ the established transfer matrix method to analyse the electron transport in the MoS2/MoO x heterostructures with double-well and step-well geometries. We also considere the coupling between transverse and longitudinal kinetic energy because the electron effective mass changes spatially in the MoS2/MoO x heterostructures. We find the resonant peaks show red shift with the increasing of transverse momentum, which is similar to the previous work studying the transverse-momentum-dependent transmission in GaAs/Ga1‑x Al x As double-barrier structure. We find electric field can enhance the magnitude of peaks and intensify the coupling between longitudinal and transverse momentums. Moreover, higher bias is applied to optimize resonant tunnelling condition to show negative differential effect can be observed in the MoS2/MoO x system.
Cu2O-directed in situ growth of Au nanoparticles inside HKUST-1 nanocages.
Liu, Yongxin; Liu, Ting; Tian, Long; Zhang, Linlin; Yao, Lili; Tan, Taixing; Xu, Jin; Han, Xiaohui; Liu, Dan; Wang, Cheng
2016-12-07
Controllable integration of metal nanoparticles (MNPs) and metal-organic frameworks (MOFs) is attracting considerable attention as the obtained composite materials always show synergistic effects in applications of catalysis, delivery, as well as sensing. Herein, a Cu 2 O-directed in situ growth strategy was developed to integrate Au nanoparticles and HKUST-1. In this strategy, Cu 2 O@HKUST-1 core-shell heterostructures, HKUST-1 nanocages, Cu 2 O@Au@HKUST-1 sandwich core-shell heterostructures and Au@HKUST-1 balls-in-cage heterostructures were successfully synthesized. Cu 2 O@HKUST-1 core-shell heterostructures were synthesized by soaking Cu 2 O nanocrystals in benzene-1,3,5-tricarboxylic acid solution. The well-defined Cu 2 O@HKUST-1 core-shell heterostructures were demonstrated to be dominated by the ratio of Cu 2+ cations to btc 3- ligands in solution during the period of HKUST-1 formation. Cu 2 O@Au@HKUST-1 sandwich core-shell or Au@HKUST-1 balls-in-cage heterostructures were obtained by impregnating HAuCl 4 into Cu 2 O@HKUST-1 core-shell heterostructures. Due to the porosity of HKUST-1 and reducibility of Cu 2 O, HAuCl 4 could pass through the HKUST-1 shell and be reduced by the Cu 2 O core in situ forming Au nanoparticles. Finally, CO oxidation reaction at high temperatures was carried out to assess the catalytic functionality of the obtained composite heterostructures. This strategy can circumvent some drawbacks of the existing approaches for integrating MNPs and MOFs, such as nonselective deposition of MNPs at the outer surface of the MOF matrices, extreme treatment conditions and additional surface modifications.
Lu, Di; Baek, David J.; Hong, Seung Sae; ...
2016-09-12
Here, the ability to create and manipulate materials in two-dimensional (2D) form has repeatedly had transformative impact on science and technology. In parallel with the exfoliation and stacking of intrinsically layered crystals 1, 2, 3, 4, 5, atomic-scale thin film growth of complex materials has enabled the creation of artificial 2D heterostructures with novel functionality 6, 7, 8, 9 and emergent phenomena, as seen in perovskite heterostructures 10, 11, 12. However, separation of these layers from the growth substrate has proved challenging, limiting the manipulation capabilities of these heterostructures with respect to exfoliated materials. Here we present a general methodmore » to create freestanding perovskite membranes. The key is the epitaxial growth of water-soluble Sr 3Al 2O 6 on perovskite substrates, followed by in situ growth of films and heterostructures. Millimetre-size single-crystalline membranes are produced by etching the Sr 3Al 2O 6 layer in water, providing the opportunity to transfer them to arbitrary substrates and integrate them with heterostructures of semiconductors and layered compounds 13, 14.« less
Growth and interface engineering in thin-film Ba0.6Sr0.4TiO3 /SrMoO3 heterostructures
NASA Astrophysics Data System (ADS)
Radetinac, Aldin; Ziegler, Jürgen; Vafaee, Mehran; Alff, Lambert; Komissinskiy, Philipp
2017-04-01
Epitaxial heterostructures of ferroelectric Ba0.6Sr0.4TiO3 and highly conducting SrMoO3 were grown by pulsed laser deposition on SrTiO3 (0 0 1) substrates. Surface oxidation of the SrMoO3 film is suppressed using a thin cap interlayer of Ba0.6Sr0.4TiO3-δ grown in reduced atmosphere. As shown by X-ray photoelectron spectroscopy, the Mo4+ valence state of the SrMoO3 films is stable upon annealing of the sample in oxygen up to 600 °C. The described oxygen interface engineering enables utilization of the highly conducting material SrMoO3 in multilayer oxide ferroelectric varactors.
Transition-Metal Oxide (111) Bilayers
Okamoto, Satoshi; Xiao, Di
2018-04-15
Correlated electron systems on a honeycomb lattice have emerged as a fertile playground to explore exotic electronic phenomena. Theoretical and experimental work has appeared to realize novel behavior, including quantum Hall effects and valleytronics, mainly focusing on van der Waals compounds, such as graphene, chalcogenides, and halides. Here in this paper, we review our theoretical study on perovskite transition-metal oxides (TMOs) as an alternative system to realize such exotic phenomena. We demonstrate that novel quantum Hall effects and related phenomena associated with the honeycomb structure could be artificially designed by such TMOs by growing their heterostructures along the [111] crystallographicmore » axis. One of the important predictions is that such TMO heterostructures could support two-dimensional topological insulating states. The strong correlation effects inherent to TM d electrons further enrich the behavior.« less
Transition-Metal Oxide (111) Bilayers
NASA Astrophysics Data System (ADS)
Okamoto, Satoshi; Xiao, Di
2018-04-01
Correlated electron systems on a honeycomb lattice have emerged as a fertile playground to explore exotic electronic phenomena. Theoretical and experimental work has appeared to realize novel behavior, including quantum Hall effects and valleytronics, mainly focusing on van der Waals compounds, such as graphene, chalcogenides, and halides. In this article, we review our theoretical study on perovskite transition-metal oxides (TMOs) as an alternative system to realize such exotic phenomena. We demonstrate that novel quantum Hall effects and related phenomena associated with the honeycomb structure could be artificially designed by such TMOs by growing their heterostructures along the [111] crystallographic axis. One of the important predictions is that such TMO heterostructures could support two-dimensional topological insulating states. The strong correlation effects inherent to TM d electrons further enrich the behavior.
Room temperature synthesis and enhanced photocatalytic property of CeO2/ZnO heterostructures
NASA Astrophysics Data System (ADS)
Wang, Chao; Fan, Huiqing; Ren, Xiaohu; Fang, Jiawen
2018-02-01
To achieve better photocatalytic performance, we proposed a facile solid-state reaction method to produce CeO2/ZnO heterostructures. Ceria and zinc oxide were synthesized simultaneously by thoroughly grinding the mixture of zinc acetate dihydrate, cerium nitrate hexahydrate and sodium hydroxide. The morphology of the as-prepared heterostructures varies dramatically as different amount of ceria was introduced in the composition. The photocatalytic performance of CeO2/ZnO heterojunctions was 4.6 times higher than that of pure ZnO. The enhanced photocatalytic activity could be ascribed to that more electrons and holes could transport to the surface of catalysts and react with the pollution due to the extended light-responsive range, accelerated migration, increased specific surface area and suppressed recombination of photogenerated carriers.
Strain Effects in Epitaxial VO2 Thin Films on Columnar Buffer-Layer TiO2/Al2O3 Virtual Substrates.
Breckenfeld, Eric; Kim, Heungsoo; Burgess, Katherine; Charipar, Nicholas; Cheng, Shu-Fan; Stroud, Rhonda; Piqué, Alberto
2017-01-18
Epitaxial VO 2 /TiO 2 thin film heterostructures were grown on (100) (m-cut) Al 2 O 3 substrates via pulsed laser deposition. We have demonstrated the ability to reduce the semiconductor-metal transition (SMT) temperature of VO 2 to ∼44 °C while retaining a 4 order of magnitude SMT using the TiO 2 buffer layer. A combination of electrical transport and X-ray diffraction reciprocal space mapping studies help examine the specific strain states of VO 2 /TiO 2 /Al 2 O 3 heterostructures as a function of TiO 2 film growth temperatures. Atomic force microscopy and transmission electron microscopy analyses show that the columnar microstructure present in TiO 2 buffer films is responsible for the partially strained VO 2 film behavior and subsequently favorable transport characteristics with a lower SMT temperature. Such findings are of crucial importance for both the technological implementation of the VO 2 system, where reduction of its SMT temperature is widely sought, as well as the broader complex oxide community, where greater understanding of the evolution of microstructure, strain, and functional properties is a high priority.
Pelcher, Kate E.; Milleville, Christopher C.; Wangoh, Linda; ...
2016-12-06
Here, semiconductor heterostructures for solar energy conversion interface light-harvesting semiconductor nanoparticles with wide-band-gap semiconductors that serve as charge acceptors. In such heterostructures, the kinetics of charge separation depend on the thermodynamic driving force, which is dictated by energetic offsets across the interface. A recently developed promising platform interfaces semiconductor quantum dots (QDs) with ternary vanadium oxides that have characteristic midgap states situated between the valence and conduction bands. In this work, we have prepared CdS/β-Pb 0.33V 2O 5 heterostructures by both linker-assisted assembly and surface precipitation and contrasted these materials with CdSe/β-Pb 0.33V 2O 5 heterostructures prepared by the samemore » methods. Increased valence-band (VB) edge onsets in X-ray photoelectron spectra for CdS/β-Pb 0.33V 2O 5 heterostructures relative to CdSe/β-Pb 0.33V 2O 5 heterostructures suggest a positive shift in the VB edge potential and, therefore, an increased driving force for the photoinduced transfer of holes to the midgap state of β-Pb 0.33V 2O 5. This approach facilitates a ca. 0.40 eV decrease in the thermodynamic barrier for hole injection from the VB edge of QDs suggesting an important design parameter. Transient absorption spectroscopy experiments provide direct evidence of hole transfer from photoexcited CdS QDs to the midgap states of β-Pb 0.33V 2O 5 NWs, along with electron transfer into the conduction band of the β-Pb 0.33V 2O 5 NWs. Hole transfer is substantially faster and occurs at <1-ps time scales, whereas completion of electron transfer requires 5—30 ps depending on the nature of the interface. The differentiated time scales of electron and hole transfer, which are furthermore tunable as a function of the mode of attachment of QDs to NWs, provide a vital design tool for designing architectures for solar energy conversion. More generally, the approach developed here suggests that interfacing semiconductor QDs with transition-metal oxide NWs exhibiting intercalative midgap states yields a versatile platform wherein the thermodynamics and kinetics of charge transfer can be systematically modulated to improve the efficiency of charge separation across interfaces.« less
DOE Office of Scientific and Technical Information (OSTI.GOV)
Pelcher, Kate E.; Milleville, Christopher C.; Wangoh, Linda
Here, semiconductor heterostructures for solar energy conversion interface light-harvesting semiconductor nanoparticles with wide-band-gap semiconductors that serve as charge acceptors. In such heterostructures, the kinetics of charge separation depend on the thermodynamic driving force, which is dictated by energetic offsets across the interface. A recently developed promising platform interfaces semiconductor quantum dots (QDs) with ternary vanadium oxides that have characteristic midgap states situated between the valence and conduction bands. In this work, we have prepared CdS/β-Pb 0.33V 2O 5 heterostructures by both linker-assisted assembly and surface precipitation and contrasted these materials with CdSe/β-Pb 0.33V 2O 5 heterostructures prepared by the samemore » methods. Increased valence-band (VB) edge onsets in X-ray photoelectron spectra for CdS/β-Pb 0.33V 2O 5 heterostructures relative to CdSe/β-Pb 0.33V 2O 5 heterostructures suggest a positive shift in the VB edge potential and, therefore, an increased driving force for the photoinduced transfer of holes to the midgap state of β-Pb 0.33V 2O 5. This approach facilitates a ca. 0.40 eV decrease in the thermodynamic barrier for hole injection from the VB edge of QDs suggesting an important design parameter. Transient absorption spectroscopy experiments provide direct evidence of hole transfer from photoexcited CdS QDs to the midgap states of β-Pb 0.33V 2O 5 NWs, along with electron transfer into the conduction band of the β-Pb 0.33V 2O 5 NWs. Hole transfer is substantially faster and occurs at <1-ps time scales, whereas completion of electron transfer requires 5—30 ps depending on the nature of the interface. The differentiated time scales of electron and hole transfer, which are furthermore tunable as a function of the mode of attachment of QDs to NWs, provide a vital design tool for designing architectures for solar energy conversion. More generally, the approach developed here suggests that interfacing semiconductor QDs with transition-metal oxide NWs exhibiting intercalative midgap states yields a versatile platform wherein the thermodynamics and kinetics of charge transfer can be systematically modulated to improve the efficiency of charge separation across interfaces.« less
Spin State Control using Oxide Interfaces in LaCoO3-based Heterostructures
NASA Astrophysics Data System (ADS)
Lee, Sangjae; Disa, Ankit; Walker, Frederick; Ahn, Charles
The flexibility of the spin degree of freedom of the Co 3d orbitals in LaCoO3 suggests that they can be changed through careful design of oxide heterostructures. Interfacial coupling and dimensional confinement can be used to control the magnetic exchange, crystal fields, and Hund's coupling, through orbital and charge reconstructions. These parameters control the balance between multiple spin configurations, thereby modifying the magnetic ordering of LaCoO3. We study (LaCoO3)m /(LaTiO3)2 heterostructures grown by molecular beam epitaxy, which allow interfacial charge transfer from Ti to Co, in addition to structural and dimensional constraints. The electronic polarization at the interface and consequent structural distortions suppress the ferromagnetism in the LaCoO3 layers. This effect extends well beyond the interface, with ferromagnetic order absent up to LaCoO3 layer thickness of m =10. We compare the properties of the LaCoO3/LaTiO3heterostructureswithLaCoO3/SrTiO3, to untangle how charge transfer and structural modifications control the spin and magnetic configuration in cobaltates.
NASA Astrophysics Data System (ADS)
Niu, Xiaoyou; Yan, Weijing; Zhao, Hongli; Yang, Jingkai
2018-05-01
Limited by the narrowed photoresponse range and unsatisfactory recombination of photoinduced electron-hole pairs, the photocatalytic efficiency of TiO2 is still far below what is expected. Here, we initially doped TiO2 nanotubes (TNTS) by transition metal ion Nb, then it is coupled with reduced graphene oxide (rGO) to construct a heterostructure photocatalyst. The defect state presented in TiO2 leading to the formation of localized midgap states (MS) in the bandgap, which regulating the band structure of TiO2 and extending the optical absorption to visible light region. The internal charge transport and transfer behavior analyzed by electrochemical impedance spectroscopy (EIS) reveal that the coupling of rGO with TNTS results in the formation of electron transport channel in the heterostructure, which makes a great contribution to the photoinduced charge separation. As expected, the Nb-TNTS/rGO exhibits a stable and remarkably enhanced photocatalytic activity in the visible-light irradiation degradation of methylene blue (MB), up to ∼5 times with respect to TNTS, which is attributed to the effective inhibition of charge recombination, the reduction of bandgap and higher redox potential, as well as the great adsorptivity.
NASA Astrophysics Data System (ADS)
Frabboni, S.; Grillo, V.; Gazzadi, G. C.; Balboni, R.; Trotta, R.; Polimeni, A.; Capizzi, M.; Martelli, F.; Rubini, S.; Guzzinati, G.; Glas, F.
2012-09-01
Hydrogen incorporation in diluted nitride semiconductors dramatically modifies the electronic and structural properties of the crystal through the creation of nitrogen-hydrogen complexes. We report a convergent beam electron-diffraction characterization of diluted nitride semiconductor-heterostructures patterned at a sub-micron scale and selectively exposed to hydrogen. We present a method to determine separately perpendicular mismatch and static disorder in pristine and hydrogenated heterostructures. The roles of chemical composition and strain on static disorder have been separately assessed.
NASA Astrophysics Data System (ADS)
Lei, Qingyu; Golalikhani, Maryam; Davidson, Bruce A.; Liu, Guozhen; Schlom, Darrell G.; Qiao, Qiao; Zhu, Yimei; Chandrasena, Ravini U.; Yang, Weibing; Gray, Alexander X.; Arenholz, Elke; Farrar, Andrew K.; Tenne, Dmitri A.; Hu, Minhui; Guo, Jiandong; Singh, Rakesh K.; Xi, Xiaoxing
2017-12-01
Advancements in nanoscale engineering of oxide interfaces and heterostructures have led to discoveries of emergent phenomena and new artificial materials. Combining the strengths of reactive molecular-beam epitaxy and pulsed-laser deposition, we show here, with examples of Sr1+xTi1-xO3+δ, Ruddlesden-Popper phase Lan+1NinO3n+1 (n = 4), and LaAl1+yO3(1+0.5y)/SrTiO3 interfaces, that atomic layer-by-layer laser molecular-beam epitaxy significantly advances the state of the art in constructing oxide materials with atomic layer precision and control over stoichiometry. With atomic layer-by-layer laser molecular-beam epitaxy we have produced conducting LaAlO3/SrTiO3 interfaces at high oxygen pressures that show no evidence of oxygen vacancies, a capability not accessible by existing techniques. The carrier density of the interfacial two-dimensional electron gas thus obtained agrees quantitatively with the electronic reconstruction mechanism.
Band offset engineering of 2DEG oxide systems on Si
NASA Astrophysics Data System (ADS)
Jin, Eric; Kornblum, Lior; Kumah, Divine; Zou, Ke; Broadbridge, Christine; Ngai, Joseph; Ahn, Charles; Walker, Fred
2015-03-01
The discovery of 2-dimensional electron gases (2DEGs) at perovskite oxide interfaces has sparked much interest in recent years due to their large carrier densities when compared with semiconductor heterostructures. For device applications, these oxide systems are plagued by low room temperature electrical mobilities. We present an approach to combine the high carrier density of 2DEG oxides with a higher mobility medium in order to realize the combined benefits of higher mobility and carrier density. We grow epitaxial films of the interfacial oxide system LaTiO3/SrTiO3 (LTO/STO) on silicon by molecular beam epitaxy. Magnetotransport measurements show that the sheet carrier densities of the heterostructures scale with the number of LTO/STO interfaces, consistent with the presence of a 2DEG at each interface. Sheet carrier densities of 8.9 x 1014 cm-2 per interface are measured. Band offsets between the STO and Si are obtained, showing that the conduction band edge of the STO is close in energy to that of silicon, but in a direction that hinders carrier transfer to the silicon substrate. Through modification of the STO/Si interface, we suggest an approach to raise the band offset in order to move the 2DEG from the oxide into the silicon.
Disentangled Cooperative Orderings in Artificial Rare-Earth Nickelates
Middey, S.; Meyers, D.; Kareev, M.; ...
2018-04-09
Coupled transitions between distinct ordered phases are important aspects behind the rich phase complexity of correlated oxides that hinder our understanding of the underlying phenomena. For this reason, fundamental control over complex transitions has become a leading motivation of the designer approach to materials. We have devised a series of new superlattices by combining a Mott insulator and a correlated metal to form ultrashort period superlattices, which allow one to disentangle the simultaneous orderings in RENiO 3. Tailoring an incommensurate heterostructure period relative to the bulk charge ordering pattern suppresses the charge order transition while preserving metal-insulator and antiferromagnetic transitions.more » Such selective decoupling of the entangled phases resolves the long-standing puzzle about the driving force behind the metal-insulator transition and points to the site-selective Mott transition as the operative mechanism. In conclusion, this designer approach emphasizes the potential of heterointerfaces for selective control of simultaneous transitions in complex materials with entwined broken symmetries.« less
Disentangled Cooperative Orderings in Artificial Rare-Earth Nickelates
DOE Office of Scientific and Technical Information (OSTI.GOV)
Middey, S.; Meyers, D.; Kareev, M.
Coupled transitions between distinct ordered phases are important aspects behind the rich phase complexity of correlated oxides that hinder our understanding of the underlying phenomena. For this reason, fundamental control over complex transitions has become a leading motivation of the designer approach to materials. We have devised a series of new superlattices by combining a Mott insulator and a correlated metal to form ultrashort period superlattices, which allow one to disentangle the simultaneous orderings in RENiO 3. Tailoring an incommensurate heterostructure period relative to the bulk charge ordering pattern suppresses the charge order transition while preserving metal-insulator and antiferromagnetic transitions.more » Such selective decoupling of the entangled phases resolves the long-standing puzzle about the driving force behind the metal-insulator transition and points to the site-selective Mott transition as the operative mechanism. In conclusion, this designer approach emphasizes the potential of heterointerfaces for selective control of simultaneous transitions in complex materials with entwined broken symmetries.« less
DOE Office of Scientific and Technical Information (OSTI.GOV)
Meyers, D.; Liu, Jian; Freeland, J. W.
We observed complex materials in electronic phases and transitions between them often involve coupling between many degrees of freedom whose entanglement convolutes understanding of the instigating mechanism. Metal-insulator transitions are one such problem where coupling to the structural, orbital, charge, and magnetic order parameters frequently obscures the underlying physics. We demonstrate a way to unravel this conundrum by heterostructuring a prototypical multi-ordered complex oxide NdNiO3 in ultra thin geometry, which preserves the metal-to-insulator transition and bulk-like magnetic order parameter, but entirely suppresses the symmetry lowering and long-range charge order parameter. Furthermore, these findings illustrate the utility of heterointerfaces as amore » powerful method for removing competing order parameters to gain greater insight into the nature of the transition, here revealing that the magnetic order generates the transition independently, leading to an exceptionally rare purely electronic metal-insulator transition with no symmetry change.« less
IZO deposited by PLD on flexible substrate for organic heterostructures
NASA Astrophysics Data System (ADS)
Socol, M.; Preda, N.; Stanculescu, A.; Breazu, C.; Florica, C.; Rasoga, O.; Stanculescu, F.; Socol, G.
2017-05-01
In:ZnO (IZO) thin films were deposited on flexible plastic substrates by pulsed laser deposition (PLD) method. The obtained layers present adequate optical and electrical properties competitive with those based on indium tin oxide (ITO). The figure of merit (9 × 10-3 Ω-1) calculated for IZO layers demonstrates that high quality coatings can be prepared by this deposition technique. A thermal annealing (150 °C for 1 h) or an oxygen plasma etching (6 mbar for 10 min.) were applied to the IZO layers to evaluate the influence of these treatments on the properties of the transparent coatings. Using vacuum evaporation, organic heterostructures based on cooper phthalocyanine (CuPc) and 3,4,9,10-perylenetetracarboxylic dianhydride (PTCDA) were deposited on the untreated and treated IZO layers. The optical and electrical properties of the heterostructures were investigated by UV-Vis, FTIR and current-voltage ( I- V) measurements. For the heterostructure fabricated on IZO treated in oxygen plasma, an improvement in the current value with at least one order of magnitude was evidenced in the I- V characteristics recorded in dark conditions. Also, an increase in the current value for the heterostructure deposited on untreated IZO layer can be achieved by adding an organic layer such as tris-8-hydroxyquinoline aluminium (Alq3).
Impact of MoO3 interlayer on the energy level alignment of pentacene-C60 heterostructure.
Zou, Ye; Mao, Hongying; Meng, Qing; Zhu, Daoben
2016-02-28
Using in situ ultraviolet photoelectron spectroscopy, the electronic structure evolutions at the interface between pentacene and fullerene (C60), a classical organic donor-acceptor heterostructure in organic electronic devices, on indium-tin oxide (ITO) and MoO3 modified ITO substrates have been investigated. The insertion of a thin layer MoO3 has a significant impact on the interfacial energy level alignment of pentacene-C60 heterostructure. For the deposition of C60 on pentacene, the energy difference between the highest occupied molecular orbital of donor and the lowest unoccupied molecular orbital of acceptor (HOMO(D)-LUMO(A)) offset of C60/pentacene heterostructure increased from 0.86 eV to 1.54 eV after the insertion of a thin layer MoO3 on ITO. In the inverted heterostructrure where pentacene was deposited on C60, the HOMO(D)-LUMO(A) offset of pentacene/C60 heterostructure increased from 1.32 to 2.20 eV after MoO3 modification on ITO. The significant difference of HOMO(D)-LUMO(A) offset shows the feasibility to optimize organic electronic device performance through interfacial engineering approaches, such as the insertion of a thin layer high work function MoO3 films.
NASA Astrophysics Data System (ADS)
Wang, Qingpeng; Ao, Jin-Ping; Wang, Pangpang; Jiang, Ying; Li, Liuan; Kawaharada, Kazuya; Liu, Yang
2015-04-01
GaN metal-oxide-semiconductor field-effect transistors (MOSFETs) on AlGaN/GaN heterostructure with a recess gate were fabricated and characterized. The device showed good pinch-off characteristics and a maximum field-effect mobility of 145.2 cm2·V-1·s-1. The effects of etching gas of Cl2 and SiCl4 were investigated in the gate recess process. SiCl4-etched devices showed higher channel mobility and lower threshold voltage. Atomic force microscope measurement was done to investigate the etching profile with different etching protection mask. Compared with photoresist, SiO2-masked sample showed lower surface roughness and better profile with stepper sidewall and weaker trenching effect resulting in higher channel mobility in the MOSFET.
NASA Astrophysics Data System (ADS)
Fiorenza, Patrick; Greco, Giuseppe; Schilirò, Emanuela; Iucolano, Ferdinando; Lo Nigro, Raffaella; Roccaforte, Fabrizio
2018-05-01
This letter presents time-dependent gate-capacitance transient measurements (C–t) to determine the oxide trapped charges (N ot) in Al2O3 films deposited on recessed AlGaN/GaN heterostructures. The C–t transients acquired at different temperatures under strong accumulation allowed to accurately monitor the gradual electron trapping, while hindering the re-emission by fast traps that may affect conventional C–V hysteresis measurements. Using this method, an increase of N ot from 2 to 6 × 1012 cm‑2 was estimated between 25 and 150 °C. The electron trapping is ruled by an Arrhenius dependence with an activation energy of 0.12 eV which was associated to points defects present in the Al2O3 films.
Mubeen, Syed; Singh, Nirala; Lee, Joun; Stucky, Galen D; Moskovits, Martin; McFarland, Eric W
2013-05-08
Efficient and cost-effective conversion of solar energy to useful chemicals and fuels could lead to a significant reduction in fossil hydrocarbon use. Artificial systems that use solar energy to produce chemicals have been reported for more than a century. However the most efficient devices demonstrated, based on traditionally fabricated compound semiconductors, have extremely short working lifetimes due to photocorrosion by the electrolyte. Here we report a stable, scalable design and molecular level fabrication strategy to create photoelectrochemically active heterostructure (PAH) units consisting of an efficient semiconductor light absorber in contact with oxidation and reduction electrocatalysts and otherwise protected by alumina. The functional heterostructures are fabricated by layer-by-layer, template-directed, electrochemical synthesis in porous anodic aluminum oxide membranes to produce high density arrays of electronically autonomous, nanostructured, corrosion resistant, photoactive units (~10(9)-10(10) PAHs per cm(2)). Each PAH unit is isolated from its neighbor by the transparent electrically insulating oxide cellular enclosure that makes the overall assembly fault tolerant. When illuminated with visible light, the free floating devices have been demonstrated to produce hydrogen at a stable rate for over 24 h in corrosive hydroiodic acid electrolyte with light as the only input. The quantum efficiency (averaged over the solar spectrum) for absorbed photons-to-hydrogen conversion was 7.4% and solar-to-hydrogen energy efficiency of incident light was 0.9%. The fabrication approach is scalable for commercial manufacturing and readily adaptable to a variety of earth abundant semiconductors which might otherwise be unstable as photoelectrocatalysts.
Identifying suitable substrates for high-quality graphene-based heterostructures
NASA Astrophysics Data System (ADS)
Banszerus, L.; Janssen, H.; Otto, M.; Epping, A.; Taniguchi, T.; Watanabe, K.; Beschoten, B.; Neumaier, D.; Stampfer, C.
2017-06-01
We report on a scanning confocal Raman spectroscopy study investigating the strain-uniformity and the overall strain and doping of high-quality chemical vapour deposited (CVD) graphene-based heterostuctures on a large number of different substrate materials, including hexagonal boron nitride (hBN), transition metal dichalcogenides, silicon, different oxides and nitrides, as well as polymers. By applying a hBN-assisted, contamination free, dry transfer process for CVD graphene, high-quality heterostructures with low doping densities and low strain variations are assembled. The Raman spectra of these pristine heterostructures are sensitive to substrate-induced doping and strain variations and are thus used to probe the suitability of the substrate material for potential high-quality graphene devices. We find that the flatness of the substrate material is a key figure for gaining, or preserving high-quality graphene.
Two dimensional graphene nanogenerator by coulomb dragging: Moving van der Waals heterostructure
DOE Office of Scientific and Technical Information (OSTI.GOV)
Zhong, Huikai; Li, Xiaoqiang; Wu, Zhiqian
2015-06-15
Harvesting energy from environment is the current focus of scientific community. Here, we demonstrate a graphene nanogenerator, which is based on moving van der Waals heterostructure formed between graphene and two dimensional (2D) graphene oxide (GO). This nanogenerator can convert mechanical energy into electricity with a voltage output of around 10 mV. Systematic experiments reveal the generated electricity originates from the coulomb interaction induced momentum transfer between 2D GO and holes in graphene. 2D boron nitride was also demonstrated to be effective in the framework of moving van der Waals heterostructure nanogenerator. This investigation of nanogenerator based on the interaction betweenmore » 2D macromolecule materials will be important to understand the origin of the flow-induced potential in nanomaterials and may have great potential in practical applications.« less
Hoffman, Jason D.; Kirby, Brian J.; Kwon, Jihwan; ...
2016-11-22
Interfaces between correlated complex oxides are promising avenues to realize new forms of magnetism that arise as a result of charge transfer, proximity effects, and locally broken symmetries. We report on the discovery of a noncollinear magnetic structure in superlattices of the ferromagnetic metallic oxide La 2/3Sr 1/3MnO 3 (LSMO) and the correlated metal LaNiO 3 (LNO). The exchange interaction between LSMO layers is mediated by the intervening LNO, such that the angle between the magnetization of neighboring LSMO layers varies in an oscillatory manner with the thickness of the LNO layer. The magnetic field, temperature, and spacer thickness dependencemore » of the noncollinear structure are inconsistent with the bilinear and biquadratic interactions that are used to model the magnetic structure in conventional metallic multilayers. A model that couples the LSMO layers to a helical spin state within the LNO fits the observed behavior. We propose that the spin-helix results from the interaction between a spatially varying spin susceptibility within the LNO and interfacial charge transfer that creates localized Ni 2+ states. In conclusion, our work suggests a new approach to engineering noncollinear spin textures in metallic oxide heterostructures.« less
NASA Astrophysics Data System (ADS)
Hou, Minmin; Jain, Sambhav R.; So, Hongyun; Heuser, Thomas A.; Xu, Xiaoqing; Suria, Ateeq J.; Senesky, Debbie G.
2017-11-01
In this paper, the electron mobility and sheet density of the two-dimensional electron gas (2DEG) in both air and argon environments at 600 °C were measured intermittently over a 5 h duration using unpassivated and Al2O3-passivated AlGaN/GaN (with 3 nm GaN cap) van der Pauw test structures. The unpassivated AlGaN/GaN heterostructures annealed in air showed the smallest decrease (˜8%) in 2DEG electron mobility while Al2O3-passivated samples annealed in argon displayed the largest drop (˜70%) based on the Hall measurements. Photoluminescence and atomic force microscopy showed that minimal strain relaxation and surface roughness changes have occurred in the unpassivated samples annealed in air, while those with Al2O3 passivation annealed in argon showed significant microstructural degradations. This suggests that cracks developed in the samples annealed in air were healed by oxidation reactions. To further confirm this, Auger electron spectroscopy was conducted on the unpassivated samples after the anneal in air and results showed that extra surface oxides have been generated, which could act as a dislocation pinning layer to suppress the strain relaxation in AlGaN. On the other hand, similar 2DEG sheet densities were observed in passivated and unpassivated AlGaN/GaN samples at the end of the 5-h anneal in air or argon due to the combined impact of strain relaxation and changes in the ionized electronic states. The results support the use of unpassivated GaN-capped AlGaN/GaN heterostructures as the material platform for high-temperature electronics and sensors used in oxidizing environmental conditions.
DOE Office of Scientific and Technical Information (OSTI.GOV)
Pal, Shreyasi, E-mail: Shreyasi.tua@gamil.com; Maiti, Soumen; Chattopadhyay, Kalyan Kumar, E-mail: kalyan-chattopadhyay@yahoo.com
2016-05-06
Rational construction of heterostructure is a key pathway to pursue highly active photocatalysts that also offers prospects to explore the relationship between structural aspect and photocatalytic efficiency. Here, we adopted a two-step wet chemical protocol for decoration of ZnO nanowires with SnO{sub 2} nanoclusters. ZnO nanowires were prepared by one pot ambient conditioned synthesis from commercial zinc powder. In sequence, synthesized ZnO nanowires were engineered with varying quantity SnO{sub 2} nanoclusters via low temperature hydrothermal method. Environmental remediation through catalytic activity of the samples was inspected taking two dyes having different ionic character (Methyl Orange and Rhodamine B) under UVmore » irradiation where the optimized hybrid displayed better performance than mono component oxides. Enhancement in catalytic performance could be enlightened by the heterostructure formation at the ZnO/SnO{sub 2} interface which in turns prolonged photogenerated carrier separation and extend the photo response range. Furthermore, the photocatalysis performance by heterostructure could be recycled for several times without noticeable decrease in their catalytic activity.« less
Zhang, Jing; Zhong, Zhicheng; Guan, Xiangxiang; Shen, Xi; Zhang, Jine; Han, Furong; Zhang, Hui; Zhang, Hongrui; Yan, Xi; Zhang, Qinghua; Gu, Lin; Hu, Fengxia; Yu, Richeng; Shen, Baogen; Sun, Jirong
2018-05-15
Grouping different transition metal oxides together by interface engineering is an important route toward emergent phenomenon. While most of the previous works focused on the interface effects in perovskite/perovskite heterostructures, here we reported on a symmetry mismatch-driven spin reorientation toward perpendicular magnetic anisotropy in perovskite/brownmillerite heterostructures, which is scarcely seen in tensile perovskite/perovskite heterostructures. We show that alternately stacking perovskite La 2/3 Sr 1/3 MnO 3 and brownmillerite LaCoO 2.5 causes a strong interface reconstruction due to symmetry discontinuity at interface: neighboring MnO 6 octahedra and CoO 4 tetrahedra at the perovskite/brownmillerite interface cooperatively relax in a manner that is unavailable for perovskite/perovskite interface, leading to distinct orbital reconstructions and thus the perpendicular magnetic anisotropy. Moreover, the perpendicular magnetic anisotropy is robust, with an anisotropy constant two orders of magnitude greater than the in-plane anisotropy of the perovskite/perovskite interface. The present work demonstrates the great potential of symmetry engineering in designing artificial materials on demand.
Liang, Yuan-Chang; Lung, Tsai-Wen; Wang, Chein-Chung
2016-12-01
Well-crystallized Sn 2 S 3 semiconductor thin films with a highly (111)-crystallographic orientation were grown using RF sputtering. The surface morphology of the Sn 2 S 3 thin films exhibited a sheet-like feature. The Sn 2 S 3 crystallites with a sheet-like surface had a sharp periphery with a thickness in a nanoscale size, and the crystallite size ranged from approximately 150 to 300 nm. Postannealing the as-synthesized Sn 2 S 3 thin films further in ambient air at 400 °C engendered roughened and oxidized surfaces on the Sn 2 S 3 thin films. Transmission electron microscopy analysis revealed that the surfaces of the Sn 2 S 3 thin films transformed into a SnO 2 phase, and well-layered Sn 2 S 3 -SnO 2 heterostructure thin films were thus formed. The Sn 2 S 3 -SnO 2 heterostructure thin film exhibited a visible photoassisted room-temperature gas-sensing behavior toward low concentrations of NO 2 gases (0.2-2.5 ppm). By contrast, the pure Sn 2 S 3 thin film exhibited an unapparent room-temperature NO 2 gas-sensing behavior under illumination. The suitable band alignment at the interface of the Sn 2 S 3 -SnO 2 heterostructure thin film and rough surface features might explain the visible photoassisted room-temperature NO 2 gas-sensing responses of the heterostructure thin film on exposure to NO 2 gas at low concentrations in this work.
NASA Astrophysics Data System (ADS)
Mirzadeh Vaghefi, P.; Baghizadeh, A.; Willinger, M.; Lourenço, A. A. C. S.; Amaral, V. S.
2017-12-01
Oxide multiferroic thin films and heterostructures offer a wide range of properties originated from intrinsic coupling between lattice strain and nanoscale magnetic/electronic ordering. La0.9Ba0.1MnO3 (LBM) thin-films and LBM/BaTiO3/LBM (LBMBT) heterostructures were grown on single crystalline [100] silicon and [0001] Al2O3 using RF magnetron sputtering to study the effect of crystallinity and induced lattice mismatch in the film on magnetic properties of deposited films and heterostructures. The thicknesses of the films on Al2O3 and Si are 70 and 145 nm, respectively, and for heterostructures are 40/30/40 nm on both substrates. The microstructure of the films, state of strain and growth orientations was studied by XRD and microscopy techniques. Interplay of microstructure, strain and magnetic properties is further investigated. It is known that the crystal structure of substrates and imposed tensile strain affect the physical properties; i.e. magnetic behavior of the film. The thin layer grown on Al2O3 substrate shows out-of-plane compressive strain, while Si substrate induces tensile strain on the deposited film. The magnetic transition temperatures (Tc) of the LBM film on the Si and Al2O3 substrates are found to be 195 K and 203 K, respectively, slightly higher than the bulk form, 185 K. The LBMBT heterostructure on Si substrate shows drastic decrease in magnetization due to produced defects created by diffusion of Ti ions into magnetic layer. Meanwhile, the Tc in LBMBTs increases in respect to other studied single layers and heterostructure, because of higher tensile strain induced at the interfaces.
Flynn, G; Stokes, K; Ryan, K M
2018-05-31
Herein, we report the formation of silicon, germanium and more complex Si-SixGe1-x and Si-Ge axial 1D heterostructures, at low temperatures in solution. These nanorods/nanowires are grown using phenylated compounds of silicon and germanium as reagents, with precursor decomposition achieved at substantially reduced temperatures (200 °C for single crystal nanostructures and 300 °C for heterostructures), through the addition of a reducing agent. This low energy route for the production of these functional nanostructures as a wet chemical in high yield is attractive to meet the processing needs for next generation photovoltaics, batteries and electronics.
Quasi 2D Ultrahigh Carrier Density in a Complex Oxide Broken Gap Heterojunction
DOE Office of Scientific and Technical Information (OSTI.GOV)
Xu, Peng; Droubay, Timothy C.; Jeong, Jong S.
2016-01-21
Two-dimensional (2D) ultra-high carrier densities at complex oxide interfaces are of considerable current research interest for novel plasmonic and high charge-gain devices. However, the highest 2D electron density obtained in oxide heterostructures is thus far limited to 3×1014 cm-2 (½ electron/unit cell/interface) at GdTiO3/SrTiO3 interfaces, and is typically an order of magnitude lower at LaAlO3/SrTiO3 interfaces. Here we show that carrier densities much higher than 3×1014 cm-2 can be achieved via band engineering. Transport measurements for 3 nm SrTiO3/t u.c. NdTiO3/3 nm SrTiO3/LSAT (001) show that charge transfer significantly in excess of the value expected from the polar discontinuity modelmore » occurs for higher t values. The carrier density remains unchanged, and equivalent to ½ electron/unit cell/interface for t < 6 unit cells. However, above a critical NdTiO3 thickness of 6 u.c., electrons from the valence band of NdTiO3 spill over into the SrTiO3 conduction band as a natural consequence of the band alignment. An atomistic model consistent with first-principle calculations and experimental results is proposed for the charge transfer mechanisms. These results may provide an exceptional route to the realization of the room-temperature oxide electronics.« less
NASA Astrophysics Data System (ADS)
Craciun, Valentin; Sánchez, Florencio
2016-09-01
The present issue contains a collection of representative papers presented in the Symposium L, "Towards Oxide-Based Electronics: growth and applications of oxide thin films and heterostructures", organized during the E-MRS Fall Meeting, 15-18 September 2015 in Warsaw, Poland. The Symposium L was organised and sponsored by the COST Action MP1308 "Towards oxide-based electronics" (TO-BE), a four-year EU project that started in June 2014. Over 100 participants from different countries all over the world presented new results on oxide thin films epitaxial growth, on emergent functionalities at oxide interfaces, and on applications of oxides in the fields on nanoelectronics, energy, sensing and actuation.
NASA Astrophysics Data System (ADS)
Wang, Liyang; Tian, Guohui; Chen, Yajie; Xiao, Yuting; Fu, Honggang
2016-04-01
In this study, a ZnO/ZnSe nanonail array was prepared via a two-step sequential hydrothermal synthetic route. In this synthetic process, the ZnO nanorod array was first grown on a fluorine-doped tin oxide (FTO) substrate using a seed-mediated growth approach via the hydrothermal process. Then, the ZnO nanonail array was obtained via in situ growth of ZnSe nano caps onto the ZnO nanorod array via a hydrothermal process in the presence of a Se source. The surface morphology and amount of ZnSe grown on the surface of the ZnO nanorods can be regulated by varying the reaction time and reactant concentration. Compared with pure ZnO nanorods, this unique nanonail array heterostructure exhibits enhanced visible light absorption. The transient photocurrent condition, in combination with steady-state and time-resolved photoluminescence spectroscopy, reveals that the ZnO/ZnSe nanonail array electrode has the highest charge separation rate, highest electron injection efficiency, and highest chemical stability. The photocurrent density of the ZnO/ZnSe nanonail array heterostructure reaches 1.01 mA cm-2 at an applied potential of 0.1 V (vs. Ag/AgCl), which is much higher than that of the ZnO/ZnSe nanorod array (0.71 mA cm-2), the pristine ZnO nanorod array (0.39 mA cm-2), and the ZnSe electrode (0.21 mA cm-2), indicating its significant visible light driven activities for photoelectrochemical water oxidation. This unique morphology of nail-capped nanorods might be important for providing better insight into the correlation between heterostructure and photoelectrochemical activity.In this study, a ZnO/ZnSe nanonail array was prepared via a two-step sequential hydrothermal synthetic route. In this synthetic process, the ZnO nanorod array was first grown on a fluorine-doped tin oxide (FTO) substrate using a seed-mediated growth approach via the hydrothermal process. Then, the ZnO nanonail array was obtained via in situ growth of ZnSe nano caps onto the ZnO nanorod array via a hydrothermal process in the presence of a Se source. The surface morphology and amount of ZnSe grown on the surface of the ZnO nanorods can be regulated by varying the reaction time and reactant concentration. Compared with pure ZnO nanorods, this unique nanonail array heterostructure exhibits enhanced visible light absorption. The transient photocurrent condition, in combination with steady-state and time-resolved photoluminescence spectroscopy, reveals that the ZnO/ZnSe nanonail array electrode has the highest charge separation rate, highest electron injection efficiency, and highest chemical stability. The photocurrent density of the ZnO/ZnSe nanonail array heterostructure reaches 1.01 mA cm-2 at an applied potential of 0.1 V (vs. Ag/AgCl), which is much higher than that of the ZnO/ZnSe nanorod array (0.71 mA cm-2), the pristine ZnO nanorod array (0.39 mA cm-2), and the ZnSe electrode (0.21 mA cm-2), indicating its significant visible light driven activities for photoelectrochemical water oxidation. This unique morphology of nail-capped nanorods might be important for providing better insight into the correlation between heterostructure and photoelectrochemical activity. Electronic supplementary information (ESI) available: SEM, EDS, XPS and photocurrent test. See DOI: 10.1039/c6nr01969b
Lin, S S; Chen, B G; Xiong, W; Yang, Y; He, H P; Luo, J
2012-09-10
Graphene is an atomic thin two-dimensional semimetal whereas ZnO is a direct wide band gap semiconductor with a strong light-emitting ability. In this paper, we report on photoluminescence (PL) of ZnO-nanowires (NWs)-core/Graphene-shell heterostructures, which shows a negative thermal quenching (NTQ) behavior both for the near band-edge and deep level emission. The abnormal PL behavior was understood through the charging and discharging processes between ZnO NWs and graphene. The NTQ properties are most possibly induced by the unique rapidly increasing density of states of graphene as a function of Fermi level, which promises a higher quantum tunneling probability between graphene and ZnO at a raised temperature.
Ab initio Design of Noncentrosymmetric Metals: Crystal Engineering in Oxide Heterostructures
2015-07-29
electronic, magnetic, and optical properties of these materials are reported. Where available the experimental studies of these systems through...RevModPhys.86.1189 James M. Rondinelli, Emmanouil Kioupakis. Predicting and Designing Optical Properties of Inorganic Materials , Annual Review of Materials ...Advances in oxide materials : Preparation, properties , performance, at University of California, Santa Barbara California, USA (August 28, 2014
Epitaxial Growth of Intermetallic MnPt Films on Oxides and Large Exchange Bias
Liu, Zhiqi; Biegalski, Michael D; Hsu, Mr. S. L.; ...
2015-11-05
We achieved a high-quality epitaxial growth of intermetallic MnPt films on oxides, with potential for multiferroic heterostructure applications. Also, antisite-stabilized spin-flipping induces ferromagnetism in MnPt films, although it is robustly antiferromagnetic in bulk. Moreover, highly ordered antiferromagnetic MnPt films exhibit superiorly large exchange coupling with a ferromagnetic layer.
NASA Astrophysics Data System (ADS)
Cui, Xingkai; Tian, Lin; Xian, Xiaozhai; Tang, Hua; Yang, Xiaofei
2018-02-01
Solar-driven water splitting over semiconductor-based photocatalysts provides direct conversion of solar energy to chemical energy, in which electron-hole separation and charge transport are critical for enhancing the photocatalytic activity of semiconducting materials. Moreover, the search for active photocatalysts that efficiently oxidize water remains a challenging task. Here, we demonstrate that a series of Ag3PO4/Ag/graphene/graphitic carbon nitride (g-C3N4) heterostructured materials can drive photocatalytic water oxidation efficiently under LED illumination. The water oxidation behavior of as-prepared composite photocatalysts in relation to the added amount of g-C3N4 and the roles of electron mediators was investigated in detail. Based on the illuminated Z-scheme photocatalytic mechanism, the photogenerated electrons and holes can be separated effectively and the electron-hole recombination of bulk material is suppressed. The reduced metallic Ag nanoparticles were found to function as the center for the accumulation of electrons from Ag3PO4 and holes from g-C3N4. By exploiting the proper addition of g-C3N4 into the composite, photocatalytic oxygen evolution performance over the heterostructured materials could be suitably tuned, which resulted in highly efficient water oxidation.
NASA Astrophysics Data System (ADS)
Seifarth, O.; Dietrich, B.; Zaumseil, P.; Giussani, A.; Storck, P.; Schroeder, T.
2010-10-01
Strained and relaxed single crystalline Si on insulator systems is an important materials science approach for future Si-based nanoelectronics. Layer transfer techniques are the dominating global integration approach over the whole wafer system but are difficult to scale down for local integration purposes limited to the area of the future device. In this respect, the heteroepitaxy approach by two simple subsequent epitaxial deposition steps of the oxide and the Si thin film is a promising way. We introduce tailored (Pr2O3)1-x(Y2O3)x oxide heterostructures on Si(111) as flexible heteroepitaxy concept for the integration of either strained or fully relaxed single crystalline Si thin films. Two different buffer concepts are explored by a combined experimental and theoretical study. First, the growth of fully relaxed single crystalline Si films is achieved by the growth of mixed PrYO3 insulators on Si(111) whose lattice constant is matched to Si. Second, isomorphic oxide-on-oxide epitaxy is exploited to grow strained Si films on lattice mismatched Y2O3/Pr2O3/Si(111) support systems. A thickness dependent multilayer model, based on Matthew's approach for strain relaxation by misfit dislocations, is presented to describe the experimental data.
Fabrication and Gas-Sensing Properties of Ni-Silicide/Si Nanowires.
Hsu, Hsun-Feng; Chen, Chun-An; Liu, Shang-Wu; Tang, Chun-Kai
2017-12-01
Ni-silicide/Si nanowires were fabricated by atomic force microscope nano-oxidation on silicon-on-insulator substrates, selective wet etching, and reactive deposition epitaxy. Ni-silicide nanocrystal-modified Si nanowire and Ni-silicide/Si heterostructure multi-stacked nanowire were formed by low- and high-coverage depositions of Ni, respectively. The Ni-silicide/Si Schottky junction and Ni-silicide region were attributed high- and low-resistance parts of nanowire, respectively, causing the resistance of the Ni-silicide nanocrystal-modified Si nanowire and the Ni-silicide/Si heterostructure multi-stacked nanowire to be a little higher and much lower than that of Si nanowire. An O 2 sensing device was formed from a nanowire that was mounted on Pt electrodes. When the nanowires exposed to O 2 , the increase in current in the Ni-silicide/Si heterostructure multi-stacked nanowire was much larger than that in the other nanowires. The Ni-silicide nanocrystal-modified Si nanowire device had the highest sensitivity. The phenomenon can be explained by the formation of a Schottky junction at the Ni-silicide/Si interface in these two types of Ni-Silicide/Si nanowire and the formation of a hole channel at the silicon nanowire/native oxide interface after exposing the nanowires to O 2 .
Catalytic growth of vertically aligned SnS/SnS2 p-n heterojunctions
NASA Astrophysics Data System (ADS)
Degrauw, Aaron; Armstrong, Rebekka; Rahman, Ajara A.; Ogle, Jonathan; Whittaker-Brooks, Luisa
2017-09-01
Nanowire arrays of SnS/SnS2 p-n heterojunctions are grown on transparent indium tin oxide (ITO) coated-glass and Si/SiO2 substrates via chemical vapor transport (CVT). The nanowire arrays are comprised of individual SnS/SnS2 heterostructures that are highly oriented with their lengths and morphologies controlled by the CVT conditions (i.e. reaction temperature, flow rate, and reaction time). The growth and optoelectronic characterization of these well-defined SnS/SnS2 p-n heterostructures pave the way for the fabrication of highly efficient solar cell devices.
Control of Interfacial Phenomena in Artificial Oxide Heterostructures
2015-09-01
heterostructures using the field effect to control superconductivity, magnetism, and metal‐insulator transitions. We also identify the existence of double TiO2 ...double TiO2 layers play a crucial role in determining the superconducting states of monolayer FeSe/SrTiO3. 15. SUBJECT TERMS Thin films, conductor...development of oxide‐based electronic devices. We also identify the existence of double TiO2 layers at the surface of SrTiO3 in the recently
NASA Astrophysics Data System (ADS)
Gabor, Nathaniel M.
2017-05-01
Van de Waals (vdW) heterostructures - which consist of precisely assembled atomically thin electronic materials - exhibit unusual quantum behavior. These quantum materials-by-design are of fundamental interest in basic scientific research and hold tremendous potential in advanced technological applications. Problematically, the fundamental optoelectronic response in these heterostructures is difficult to access using the standard techniques within the traditions of materials science and condensed matter physics. In the standard approach, characterization is based on the measurement of a small amount of one-dimensional data, which is used to gain a precise picture of the material properties of the sample. However, these techniques are fundamentally lacking in describing the complex interdependency of experimental degrees of freedom in vdW heterostructures. In this talk, I will present our recent experiments that utilize a highly data-intensive approach to gain deep understanding of the infrared photoresponse in vdW heterostructure photodetectors. These measurements, which combine state-of-the-art data analytics and measurement design with fundamentally new device structures and experimental parameters, give a clear picture of electron-hole pair interactions at ultrafast time scales.
Tunable two-dimensional interfacial coupling in molecular heterostructures
Xu, Beibei; Chakraborty, Himanshu; Yadav, Vivek K.; ...
2017-08-22
Two-dimensional van der Waals heterostructures are of considerable interest for the next generation nanoelectronics because of their unique interlayer coupling and optoelectronic properties. Here, we report a modified Langmuir–Blodgett method to organize twodimensional molecular charge transfer crystals into arbitrarily and vertically stacked heterostructures, consisting of bis(ethylenedithio)tetrathiafulvalene (BEDT–TTF)/C 60 and poly (3-dodecylthiophene-2,5-diyl) (P3DDT)/C 60 nanosheets. A strong and anisotropic interfacial coupling between the charge transfer pairs is demonstrated. The van der Waals heterostructures exhibit pressure dependent sensitivity with a high piezoresistance coefficient of -4.4 × 10 -6 Pa -1, and conductance and capacitance tunable by external stimuli (ferroelectric field and magneticmore » field). Density functional theory calculations confirm charge transfer between the n-orbitals of the S atoms in BEDT–TTF of the BEDT–TTF/C 60 layer and the π* orbitals of C atoms in C 60 of the P3DDT/C 60 layer contribute to the inter-complex CT. Thus, the two-dimensional molecular van der Waals heterostructures with tunable optical–electronic–magnetic coupling properties are promising for flexible electronic applications.« less
In situ catalytic growth of large-area multilayered graphene/MoS2 heterostructures.
Fu, Wei; Du, Fei-Hu; Su, Juan; Li, Xin-Hao; Wei, Xiao; Ye, Tian-Nan; Wang, Kai-Xue; Chen, Jie-Sheng
2014-04-14
Stacking various two-dimensional atomic crystals on top of each other is a feasible approach to create unique multilayered heterostructures with desired properties. Herein for the first time, we present a controlled preparation of large-area graphene/MoS2 heterostructures via a simple heating procedure on Mo-oleate complex coated sodium sulfate under N2 atmosphere. Through a direct in situ catalytic reaction, graphene layer has been uniformly grown on the MoS2 film formed by the reaction of Mo species with Species, which is from the carbothermal reduction of sodium sulfate. Due to the excellent graphene "painting" on MoS2 atomic layers, the significantly shortened lithium ion diffusion distance and the markedly enhanced electronic conductivity, these multilayered graphene/MoS2 heterostructures exhibit high specific capacity, unprecedented rate performance and outstanding cycling stability, especially at a high current density, when used as an anode material for lithium batteries. This work provides a simple but efficient route for the controlled fabrication of large-area multilayered graphene/metal sulfide heterostructures with promising applications in battery manufacture, electronics or catalysis.
In situ catalytic growth of large-area multilayered graphene/MoS2 heterostructures
Fu, Wei; Du, Fei-Hu; Su, Juan; Li, Xin-Hao; Wei, Xiao; Ye, Tian-Nan; Wang, Kai-Xue; Chen, Jie-Sheng
2014-01-01
Stacking various two-dimensional atomic crystals on top of each other is a feasible approach to create unique multilayered heterostructures with desired properties. Herein for the first time, we present a controlled preparation of large-area graphene/MoS2 heterostructures via a simple heating procedure on Mo-oleate complex coated sodium sulfate under N2 atmosphere. Through a direct in situ catalytic reaction, graphene layer has been uniformly grown on the MoS2 film formed by the reaction of Mo species with S pecies, which is from the carbothermal reduction of sodium sulfate. Due to the excellent graphene “painting” on MoS2 atomic layers, the significantly shortened lithium ion diffusion distance and the markedly enhanced electronic conductivity, these multilayered graphene/MoS2 heterostructures exhibit high specific capacity, unprecedented rate performance and outstanding cycling stability, especially at a high current density, when used as an anode material for lithium batteries. This work provides a simple but efficient route for the controlled fabrication of large-area multilayered graphene/metal sulfide heterostructures with promising applications in battery manufacture, electronics or catalysis. PMID:24728289
In situ catalytic growth of large-area multilayered graphene/MoS2 heterostructures
NASA Astrophysics Data System (ADS)
Fu, Wei; Du, Fei-Hu; Su, Juan; Li, Xin-Hao; Wei, Xiao; Ye, Tian-Nan; Wang, Kai-Xue; Chen, Jie-Sheng
2014-04-01
Stacking various two-dimensional atomic crystals on top of each other is a feasible approach to create unique multilayered heterostructures with desired properties. Herein for the first time, we present a controlled preparation of large-area graphene/MoS2 heterostructures via a simple heating procedure on Mo-oleate complex coated sodium sulfate under N2 atmosphere. Through a direct in situ catalytic reaction, graphene layer has been uniformly grown on the MoS2 film formed by the reaction of Mo species with S pecies, which is from the carbothermal reduction of sodium sulfate. Due to the excellent graphene ``painting'' on MoS2 atomic layers, the significantly shortened lithium ion diffusion distance and the markedly enhanced electronic conductivity, these multilayered graphene/MoS2 heterostructures exhibit high specific capacity, unprecedented rate performance and outstanding cycling stability, especially at a high current density, when used as an anode material for lithium batteries. This work provides a simple but efficient route for the controlled fabrication of large-area multilayered graphene/metal sulfide heterostructures with promising applications in battery manufacture, electronics or catalysis.
NASA Astrophysics Data System (ADS)
George, Chandramohan; Genovese, Alessandro; Qiao, Fen; Korobchevskaya, Kseniya; Comin, Alberto; Falqui, Andrea; Marras, Sergio; Roig, Anna; Zhang, Yang; Krahne, Roman; Manna, Liberato
2011-11-01
We report here a simple synthetic route to Au-FexOy heterostructures in which spinel ferrite (FexOy) grows as a nanorod on a spherical gold (Au) seed. The large red shift in the plasmon resonance in the heterostructures could be explained by a dielectric effect (although we could not entirely exclude a contribution due to electron transfer from Au to defect states at the Au-FexOy interface), while the magnetic properties of the Au-FexOy heterostructures were basically the same as those of the corresponding nanocrystals after Au leaching. In films of Au-FexOy heterostructures the electrical conductivity appeared to be mediated by the Au domains.We report here a simple synthetic route to Au-FexOy heterostructures in which spinel ferrite (FexOy) grows as a nanorod on a spherical gold (Au) seed. The large red shift in the plasmon resonance in the heterostructures could be explained by a dielectric effect (although we could not entirely exclude a contribution due to electron transfer from Au to defect states at the Au-FexOy interface), while the magnetic properties of the Au-FexOy heterostructures were basically the same as those of the corresponding nanocrystals after Au leaching. In films of Au-FexOy heterostructures the electrical conductivity appeared to be mediated by the Au domains. Electronic supplementary information (ESI) available: TEM/HRTEM images of (i) aliquots at the earliest stages of the growth of Au-FexOy HSs; (ii) Au-FexOy HSs synthesized at low DDAB concentrations; (iii) spherical iron oxide nanocrystals synthesized under the same conditions as the HSs, but in the absence of Au seeds; (iv) Au-FexOy urchin like nanostructures, also after attempts to leach out Au; (v) Au-FexOy HSs after treatment with hydrazine; (vi) FexOy HSs after Au leaching from Au-FexOy HSs; additional optical absorption spectra; additional I-V curves, also from films made of Au-FexOy dumbbells; and additional SEM images; vii) X-ray diffraction (XRD) pattern of a sample of Au-FexOy HSs. See DOI: 10.1039/c1nr10768b
High Performance Amplifier Element Realization via MoS2/GaTe Heterostructures.
Yan, Xiao; Zhang, David Wei; Liu, Chunsen; Bao, Wenzhong; Wang, Shuiyuan; Ding, Shijin; Zheng, Gengfeng; Zhou, Peng
2018-04-01
2D layered materials (2DLMs), together with their heterostructures, have been attracting tremendous research interest in recent years because of their unique physical and electrical properties. A variety of circuit elements have been made using mechanically exfoliated 2DLMs recently, including hard drives, detectors, sensors, and complementary metal oxide semiconductor field-effect transistors. However, 2DLM-based amplifier circuit elements are rarely studied. Here, the integration of 2DLMs with 3D bulk materials to fabricate vertical junction transistors with current amplification based on a MoS 2 /GaTe heterostructure is reported. Vertical junction transistors exhibit the typical current amplification characteristics of conventional bulk bipolar junction transistors while having good current transmission coefficients (α ∼ 0.95) and current gain coefficient (β ∼ 7) at room temperature. The devices provide new attractive prospects in the investigation of 2DLM-based integrated circuits based on amplifier circuits.
NASA Astrophysics Data System (ADS)
Hu, Chaohao; Zhuang, Jing; Zhong, Liansheng; Zhong, Yan; Wang, Dianhui; Zhou, Huaiying
2017-12-01
Heterostructured AgBr/Bi2Sn2O7 photocatalysts were synthesized successfully via the ultrasonic-assisted chemical precipitation method. XRD, FT-IR, FE-SEM, TEM, XPS, UV-vis-DRS and PL spectroscopy were used to characterize the phase structure, morphology, chemical composition, oxidation state, and optical properties of AgBr/Bi2Sn2O7 heterojunction. The photocatalytic activity of as-prepared catalysts was evaluated by the degradation of RhB under visible light irradiation. The obtained AgBr/Bi2Sn2O7 composite with the 1:1 molar ratio exhibited significantly enhanced photocatalytic performance. Further first-principles calculations indicated that the hybridization interaction between Ag and O atoms at AgBr/Bi2Sn2O7 interface is expected to be beneficial for enhancing the charge transfer and improving the photocatalytic activity of heterostructured composites.
A comparative study of heterostructured CuO/CuWO4 nanowires and thin films
NASA Astrophysics Data System (ADS)
Polyakov, Boris; Kuzmin, Alexei; Vlassov, Sergei; Butanovs, Edgars; Zideluns, Janis; Butikova, Jelena; Kalendarev, Robert; Zubkins, Martins
2017-12-01
A comparative study of heterostructured CuO/CuWO4 core/shell nanowires and double-layer thin films was performed through X-ray diffraction, confocal micro-Raman spectroscopy and electron (SEM and TEM) microscopies. The heterostructures were produced using a two-step process, starting from a deposition of amorphous WO3 layer on top of CuO nanowires and thin films by reactive DC magnetron sputtering and followed by annealing at 650 °C in air. The second step induced a solid-state reaction between CuO and WO3 oxides through a thermal diffusion process, revealed by SEM-EDX analysis. Morphology evolution of core/shell nanowires and double-layer thin films upon heating was studied by electron (SEM and TEM) microscopies. A formation of CuWO4 phase was confirmed by X-ray diffraction and confocal micro-Raman spectroscopy.
Band offsets in ITO/Ga2O3 heterostructures
NASA Astrophysics Data System (ADS)
Carey, Patrick H.; Ren, F.; Hays, David C.; Gila, B. P.; Pearton, S. J.; Jang, Soohwan; Kuramata, Akito
2017-11-01
The valence band offsets in rf-sputtered Indium Tin Oxide (ITO)/single crystal β-Ga2O3 (ITO/Ga2O3) heterostructures were measured with X-Ray Photoelectron Spectroscopy using the Kraut method. The bandgaps of the component materials in the heterostructure were determined by Reflection Electron Energy Loss Spectroscopy as 4.6 eV for Ga2O3 and 3.5 eV for ITO. The valence band offset was determined to be -0.78 ± 0.30 eV, while the conduction band offset was determined to be -0.32 ± 0.13 eV. The ITO/Ga2O3 system has a nested gap (type I) alignment. The use of a thin layer of ITO between a metal and the Ga2O3 is an attractive approach for reducing contact resistance on Ga2O3-based power electronic devices and solar-blind photodetectors.
Pressure sensing element based on the BN-graphene-BN heterostructure
NASA Astrophysics Data System (ADS)
Li, Mengwei; Wu, Chenggen; Zhao, Shiliang; Deng, Tao; Wang, Junqiang; Liu, Zewen; Wang, Li; Wang, Gao
2018-04-01
In this letter, we report a pressure sensing element based on the graphene-boron nitride (BN) heterostructure. The heterostructure consists of monolayer graphene sandwiched between two layers of vertically stacked dielectric BN nanofilms. The BN layers were used to protect the graphene layer from oxidation and pollution. Pressure tests were performed to investigate the characteristics of the BN-graphene-BN pressure sensing element. A sensitivity of 24.85 μV/V/mmHg is achieved in the pressure range of 130-180 kPa. After exposing the BN-graphene-BN pressure sensing element to the ambient environment for 7 days, the relative resistance change in the pressure sensing element is only 3.1%, while that of the reference open-faced graphene device without the BN protection layers is 15.7%. Thus, this strategy is promising for fabricating practical graphene pressure sensors with improved performance and stability.
NASA Astrophysics Data System (ADS)
Ahmadi-Majlan, Kamyar; Chen, Tongjie; Lim, Zheng Hui; Conlin, Patrick; Hensley, Ricky; Chrysler, Matthew; Su, Dong; Chen, Hanghui; Kumah, Divine P.; Ngai, Joseph H.
2018-05-01
We present electrical and structural characterization of epitaxial LaTiO3/SrTiO3 heterostructures integrated directly on Si(100). By reducing the thicknesses of the heterostructures, an enhancement in carrier-carrier scattering is observed in the Fermi liquid behavior, followed by a metal to insulator transition in the electrical transport. The insulating behavior is described by activated transport, and its onset occurs near an occupation of 1 electron per Ti site within the SrTiO3, providing evidence for a Mott driven transition. We also discuss the role that structure and gradients in strain could play in enhancing the carrier density. The manipulation of Mott metal-insulator behavior in oxides grown directly on Si opens the pathway to harnessing strongly correlated phenomena in device technologies.
Ahmadi-Majlan, Kamyar; Chen, Tongjie; Lim, Zheng Hui; ...
2018-05-07
Here, we present electrical and structural characterization of epitaxial LaTiO 3/SrTiO 3 heterostructures integrated directly on Si(100). By reducing the thicknesses of the heterostructures, an enhancement in carrier-carrier scattering is observed in the Fermi liquid behavior, followed by a metal to insulator transition in the electrical transport. The insulating behavior is described by activated transport, and its onset occurs near 1 electron per Ti occupation within the SrTiO 3 well, providing evidence for a Mott driven transition. We also discuss the role that structure and gradients in strain could play in enhancing the carrier density. The manipulation of Mott metal-insulatormore » behavior in oxides grown directly on Si opens the pathway to harnessing strongly correlated phenomena in device technologies.« less
DOE Office of Scientific and Technical Information (OSTI.GOV)
Ahmadi-Majlan, Kamyar; Chen, Tongjie; Lim, Zheng Hui
Here, we present electrical and structural characterization of epitaxial LaTiO 3/SrTiO 3 heterostructures integrated directly on Si(100). By reducing the thicknesses of the heterostructures, an enhancement in carrier-carrier scattering is observed in the Fermi liquid behavior, followed by a metal to insulator transition in the electrical transport. The insulating behavior is described by activated transport, and its onset occurs near 1 electron per Ti occupation within the SrTiO 3 well, providing evidence for a Mott driven transition. We also discuss the role that structure and gradients in strain could play in enhancing the carrier density. The manipulation of Mott metal-insulatormore » behavior in oxides grown directly on Si opens the pathway to harnessing strongly correlated phenomena in device technologies.« less
High Performance Amplifier Element Realization via MoS2/GaTe Heterostructures
Yan, Xiao; Zhang, David Wei; Liu, Chunsen; Bao, Wenzhong; Wang, Shuiyuan; Ding, Shijin; Zheng, Gengfeng
2018-01-01
Abstract 2D layered materials (2DLMs), together with their heterostructures, have been attracting tremendous research interest in recent years because of their unique physical and electrical properties. A variety of circuit elements have been made using mechanically exfoliated 2DLMs recently, including hard drives, detectors, sensors, and complementary metal oxide semiconductor field‐effect transistors. However, 2DLM‐based amplifier circuit elements are rarely studied. Here, the integration of 2DLMs with 3D bulk materials to fabricate vertical junction transistors with current amplification based on a MoS2/GaTe heterostructure is reported. Vertical junction transistors exhibit the typical current amplification characteristics of conventional bulk bipolar junction transistors while having good current transmission coefficients (α ∼ 0.95) and current gain coefficient (β ∼ 7) at room temperature. The devices provide new attractive prospects in the investigation of 2DLM‐based integrated circuits based on amplifier circuits. PMID:29721428
NASA Astrophysics Data System (ADS)
Zhang, Jing; Yan, Xi; Han, Furong; Zhang, Jine; Liu, Dan; Shen, Baogen; Sun, Jirong
2018-05-01
The interface engineering of the complex oxides with strongly coupled degrees of freedom opens a wide space for the exploration of novel effects. La0.67Sr0.33MnO3 is one of the most typical complex oxides used for atomic level material engineering. Herein we reported an in-plane reversal of the magnetic anisotropy in (110)-oriented LaCoO3/La0.67Sr0.33MnO3 (LCO/LSMO) bilayers grown on (110)-oriented LaAlO3 substrates. Fixing the LSMO layer thickness to 8 nm and varying the LCO layer from 0 to 8 nm, totally six bilayers were fabricated. Without the LCO layer, the LSMO film exhibits an easy axis along the [1-10] direction. However, when the thickness of the LCO layer exceeds 1 nm, a signature of spin-reorientation appears; the easy axis turns from the [1-10] to the [001] direction below 225 K. This tendency is continuously enhanced by increasing the LCO. We reveal that lattice strains are different along these two directions. The magnetic anisotropy is not only controlled by lattice strain but also by structural distortion at interface. This work shows the great potential of the interface engineering with differently structured oxides for the exploration of novel functional materials.
Giant switchable Rashba effect in oxide heterostructures
Zhong, Zhicheng; Si, Liang; Zhang, Qinfang; ...
2015-03-01
One of the most fundamental phenomena and a reminder of the electron’s relativistic nature is the Rashba spin splitting for broken inversion symmetry. Usually this splitting is a tiny relativistic correction. Interfacing ferroelectric BaTiO₃ and a 5d (or 4d) transition metal oxide with a large spin-orbit coupling, Ba(Os,Ir,Ru)O₃, we show that giant Rashba spin splittings are indeed possible and even controllable by an external electric field. Based on density functional theory and a microscopic tight binding understanding, we conclude that the electric field is amplified and stored as a ferroelectric Ti-O distortion which, through the network of oxygen octahedra, inducesmore » a large (Os,Ir,Ru)-O distortion. The BaTiO₃/Ba(Os,Ru,Ir)O₃ heterostructure is hence the ideal test station for switching and studying the Rashba effect and allows applications at room temperature.« less
Multilayer heterostructures and their manufacture
Hammond, Scott R; Reese, Matthew; Rupert, Benjamin; Miedaner, Alexander; Curtis, Clavin; Olson, Dana; Ginley, David S
2015-11-04
A method of synthesizing multilayer heterostructures including an inorganic oxide layer residing on a solid substrate is described. Exemplary embodiments include producing an inorganic oxide layer on a solid substrate by a liquid coating process under relatively mild conditions. The relatively mild conditions include temperatures below 225.degree. C. and pressures above 9.4 mb. In an exemplary embodiment, a solution of diethyl aluminum ethoxide in anhydrous diglyme is applied to a flexible solid substrate by slot-die coating at ambient atmospheric pressure, and the diglyme removed by evaporation. An AlO.sub.x layer is formed by subjecting material remaining on the solid substrate to a relatively mild oven temperature of approximately 150.degree. C. The resulting AlO.sub.x layer exhibits relatively high light transmittance and relatively low vapor transmission rates for water. An exemplary embodiment of a flexible solid substrate is polyethylene napthalate (PEN). The PEN is not substantially adversely affected by exposure to 150.degree. C
NASA Astrophysics Data System (ADS)
Shi, Liang; Han, Qian; Cao, Lixin; Zhao, Fenghuan; Xia, Chenghui; Dong, Bohua; Xi, Yaoning
2016-12-01
Heterojunctions have been often employed to improve the photocatalytic behavior of titania-based materials. Herein, we propose a novel strategy to fabricate PdO/TiO2 heterostructured nanorods, as PdO was proved to be an efficient co-catalyst in photocatalytic reactions. Primarily, ammonia complex-assisted ion-exchange method was used to store Pd(II) ions in protonated titanate nanotubes, as which cannot be replaced by metallic cations via traditional route. Then, PdO/TiO2 heterojunctions formed through calcination in air, as nanotubes dehydrated and shrank into nanorods. X-ray diffraction, Raman spectra, and X-ray photoelectron spectroscopy were used to demonstrate the formation of PdO component, and transmission electron microscopy was employed to prove the successful connection between TiO2 nanorods and PdO nanoparticles. Moreover, inductive coupled plasma proved excellent compositional gradient of Pd(II) in the PdO/TiO2 heterostructured nanorods. In the present work, the photocatalytic activities of PdO/TiO2 heterostructured nanorods were investigated by decoloring several dyes under UV illumination. Our research revealed appropriate PdO loading (1.0 wt%) enhanced photocatalytic performance compared with bare TiO2 nanorods, where PdO/TiO2 heterojunctions were responsible for the prohibitive photogenerated carries recombination.
DOE Office of Scientific and Technical Information (OSTI.GOV)
Nayyar, Iffat H.; Chamberlin, Sara E.; Kaspar, Tiffany C.
2017-01-01
The electronic and optical properties of a-(Fe1xVx)2O3 at low (x = 0.04) and high (x = 0.5) doping levels are investigated using a combination of periodic and embedded cluster approaches, and time dependent density functional theory. At low V concentrations the onset of the optical absorption is B0.5 eV (i.e., nearly 1.6 eV lower than that in pure a-Fe2O3) and corresponds to the electron transitions from V 3d to Fe 3d* orbitals. At high V concentrations, optical absorption energies and intensities are sensitive to specific arrangements of Fe and V atoms and their spin configuration that determine Fe–V hybridization. Themore » onset of the lowest inter-vanadium absorption band in the case of Fe2O3/V2O3 hetero-structures is as low as B0.3 eV and the corresponding peak is at B0.7 eV. In contrast, in the case of solid solutions this peak has lower intensity and is shifted to higher energy (B1.2 eV). Analysis of the orbital character of electronic excitation suggests that Fe2O3/V2O3 hetero-structures absorb light much more effectively than random alloys, thus promoting efficient photo-induced carrier generation. These predictions can be tested in a-(Fe1xVx)2O3 thin films synthesized with well-controlled spatial distribution of Fe and V species.« less
Electron trapping in the photo-induced conductivity decay in GaAs/SnO2 heterostructure
NASA Astrophysics Data System (ADS)
de Freitas Bueno, Cristina; de Andrade Scalvi, Luis Vicente
2018-06-01
The decay of photo-induced conductivity is measured for GaAs/SnO2 heterostructure, after illumination with appropriate wavelength. The top oxide layer is deposited by sol-gel-dip-coating and doped with Eu3+, and the GaAs bottom layer is deposited by resistive evaporation. It shows quite unusual behavior since the decay rate gets slower as the temperature is raised. The trapping by intrabandgap defects in the SnO2 top layer is expected, but a GaAs/SnO2 interface arrest becomes also evident, mainly for temperatures below 100 K. Concerning the SnO2 layer, trapping by different defects is possible, due to the observed distinct capture time range. Besides Eu3+ centers and oxygen vacancies, this sort of heterostructure also leads to Eu3+ agglomerate areas in the SnO2 top layer surface, which may contribute for electron scattering. The electrical behavior reported here aims to contribute for the understanding of the electrical transport mechanisms which, combined with emission from Eu3+ ions from the top layer of the heterostructure, opens new possibilities for optoelectronic devices because samples in the form of films are desirable for circuit integration. The modeling of the photo-induced decay data yields the capture barrier in the range 620-660 meV, and contributes for the defect rules on the electrical properties of this heterostructure.
Chen, Guohui; Ji, Shaozheng; Li, Haidong; Kang, Xueliang; Chang, Sujie; Wang, Yana; Yu, Guangwei; Lu, Jianren; Claverie, Jerome; Sang, Yuanhua; Liu, Hong
2015-11-11
A SnO2 gas sensor was prepared by a two-step oxidation process whereby a Sn(II) precursor was partially oxidized by a hydrothermal process and the resulting Sn3O4 nanoplates were thermally oxidized to yield SnO2 nanoplates. The SnO2 sensor was selective and responsive toward ethanol at a temperature as low as 43 °C. This low sensing temperature stems from the rapid charge transport within SnO2 and from the presence of high-energy (001) facets available for oxygen chemisorption. SnO2/TiO2 nanobelt heterostructures were fabricated by a similar two-step process in which TiO2 nanobelts acted as support for the epitaxial growth of intermediate Sn3O4. At temperatures ranging from 43 to 276 °C, the response of these branched nanobelts is more than double the response of SnO2 for ethanol detection. Our observations demonstrate the potential of low-cost SnO2-based sensors with controlled morphology and reactive facets for detecting gases around room temperature.
NASA Astrophysics Data System (ADS)
Cui, Jizhai; Liang, Cheng-Yen; Paisley, Elizabeth A.; Sepulveda, Abdon; Ihlefeld, Jon F.; Carman, Gregory P.; Lynch, Christopher S.
2015-08-01
Experimental results demonstrate the ability of a surface electrode pattern to produce sufficient in-plane strain in a PbZr0.52Ti0.48O3 (PZT) thin film clamped by a Si substrate to control magnetism in a 1000 nm diameter Ni ring. The electrode pattern and the Ni ring/PZT thin film heterostructure were designed using a finite element based micromagnetics code. The magnetoelectric heterostructures were fabricated on the PZT film using e-beam lithography and characterized using magnetic force microscopy. Application of voltage to the electrodes moved one of the "onion" state domain walls. This method enables the development of complex architectures incorporating strain-mediated multiferroic devices.
Enhanced photoemission from glancing angle deposited SiOx-TiO2 axial heterostructure nanowire arrays
NASA Astrophysics Data System (ADS)
Dhar, J. C.; Mondal, A.; Singh, N. K.; Chattopadhyay, K. K.
2013-05-01
The glancing angle deposition technique has been employed to synthesize SiOx-TiO2 heterostructure nanowire (NW) arrays on indium tin oxide (ITO) coated glass substrate. A field emission gun scanning electron microscopic image shows that the average diameter of the NWs is ˜50 nm. Transmission electron microscopy images show the formation of heterostructure NWs, which consist of ˜180 nm SiOx and ˜210 nm long TiO2. The selected-area electron diffraction shows the amorphous nature of the synthesized NWs, which was also confirmed by X-ray diffraction method. The main band absorption edges at 3.5 eV were found for both the SiOx-TiO2 and TiO2 NW arrays on ITO coated glass plate from optical absorption measurement. Ti3+ defect related sub-band gap transition at 2.5 eV was observed for TiO2 NWs, whereas heterostructure NWs revealed the SiOx optical band gap related transition at ˜2.2 eV. Two fold improved photon absorption as well as five times photoluminescence emission enhancement were observed for the SiOx-TiO2 multilayer NWs compared to TiO2 NWs.
GaN MOSFET with Boron Trichloride-Based Dry Recess Process
NASA Astrophysics Data System (ADS)
Jiang, Y.; Wang, Q. P.; Tamai, K.; Miyashita, T.; Motoyama, S.; Wang, D. J.; Ao, J. P.; Ohno, Y.
2013-06-01
The dry recessed-gate GaN metal-oxide-semiconductor field-effect transistors (MOSFETs) on AlGaN/GaN heterostructure using boron trichloride (BCl3) as etching gas were fabricated and characterized. Etching with different etching power was conducted. Devices with silicon tetrachloride (SiCl4) etching gas were also prepared for comparison. Field-effect mobility and interface state density were extracted from current-voltage (I-V) characteristics. GaN MOSFETs on AlGaN/GaN heterostructure with BCl3 based dry recess achieved a high maximum electron mobility of 141.5 cm2V-1s-1 and a low interface state density.
Vertical epitaxial wire-on-wire growth of Ge/Si on Si(100) substrate.
Shimizu, Tomohiro; Zhang, Zhang; Shingubara, Shoso; Senz, Stephan; Gösele, Ulrich
2009-04-01
Vertically aligned epitaxial Ge/Si heterostructure nanowire arrays on Si(100) substrates were prepared by a two-step chemical vapor deposition method in anodic aluminum oxide templates. n-Butylgermane vapor was employed as new safer precursor for Ge nanowire growth instead of germane. First a Si nanowire was grown by the vapor liquid solid growth mechanism using Au as catalyst and silane. The second step was the growth of Ge nanowires on top of the Si nanowires. The method presented will allow preparing epitaxially grown vertical heterostructure nanowires consisting of multiple materials on an arbitrary substrate avoiding undesired lateral growth.
Recent Progress in Photocatalysis Mediated by Colloidal II-VI Nanocrystals
Wilker, Molly B; Schnitzenbaumer, Kyle J; Dukovic, Gordana
2012-01-01
The use of photoexcited electrons and holes in semiconductor nanocrystals as reduction and oxidation reagents is an intriguing way of harvesting photon energy to drive chemical reactions. This review focuses on recent research efforts to understand and control the photocatalytic processes mediated by colloidal II-VI nanocrystalline materials, such as cadmium and zinc chalcogenides. First, we highlight how nanocrystal properties govern the rates and efficiencies of charge-transfer processes relevant to photocatalysis. We then describe the use of nanocrystal catalyst heterostructures for fuel-forming reactions, most commonly H2 generation. Finally, we review the use of nanocrystal photocatalysis as a synthetic tool for metal–semiconductor nano-heterostructures. PMID:24115781
Probing the Interlayer Exciton Physics in a MoS2/MoSe2/MoS2 van der Waals Heterostructure.
Baranowski, M; Surrente, A; Klopotowski, L; Urban, J M; Zhang, N; Maude, D K; Wiwatowski, K; Mackowski, S; Kung, Y C; Dumcenco, D; Kis, A; Plochocka, P
2017-10-11
Stacking atomic monolayers of semiconducting transition metal dichalcogenides (TMDs) has emerged as an effective way to engineer their properties. In principle, the staggered band alignment of TMD heterostructures should result in the formation of interlayer excitons with long lifetimes and robust valley polarization. However, these features have been observed simultaneously only in MoSe 2 /WSe 2 heterostructures. Here we report on the observation of long-lived interlayer exciton emission in a MoS 2 /MoSe 2 /MoS 2 trilayer van der Waals heterostructure. The interlayer nature of the observed transition is confirmed by photoluminescence spectroscopy, as well as by analyzing the temporal, excitation power, and temperature dependence of the interlayer emission peak. The observed complex photoluminescence dynamics suggests the presence of quasi-degenerate momentum-direct and momentum-indirect bandgaps. We show that circularly polarized optical pumping results in long-lived valley polarization of interlayer exciton. Intriguingly, the interlayer exciton photoluminescence has helicity opposite to the excitation. Our results show that through a careful choice of the TMDs forming the van der Waals heterostructure it is possible to control the circular polarization of the interlayer exciton emission.
DOE Office of Scientific and Technical Information (OSTI.GOV)
Cui, Jizhai; Liang, Cheng-Yen; Sepulveda, Abdon
Experimental results demonstrate the ability of a surface electrode pattern to produce sufficient in-plane strain in a PbZr{sub 0.52}Ti{sub 0.48}O{sub 3} (PZT) thin film clamped by a Si substrate to control magnetism in a 1000 nm diameter Ni ring. The electrode pattern and the Ni ring/PZT thin film heterostructure were designed using a finite element based micromagnetics code. The magnetoelectric heterostructures were fabricated on the PZT film using e-beam lithography and characterized using magnetic force microscopy. Application of voltage to the electrodes moved one of the “onion” state domain walls. This method enables the development of complex architectures incorporating strain-mediated multiferroicmore » devices.« less
DOE Office of Scientific and Technical Information (OSTI.GOV)
Schrottke, L., E-mail: lutz@pdi-berlin.de; Lü, X.; Grahn, H. T.
We present a self-consistent model for carrier transport in periodic semiconductor heterostructures completely formulated in the Fourier domain. In addition to the Hamiltonian for the layer system, all expressions for the scattering rates, the applied electric field, and the carrier distribution are treated in reciprocal space. In particular, for slowly converging cases of the self-consistent solution of the Schrödinger and Poisson equations, numerous transformations between real and reciprocal space during the iterations can be avoided by using the presented method, which results in a significant reduction of computation time. Therefore, it is a promising tool for the simulation and efficientmore » design of complex heterostructures such as terahertz quantum-cascade lasers.« less
NASA Astrophysics Data System (ADS)
Shin, Dong-Myeong; Kim, Kyujungg; Hong, Suck Won; Oh, Jin-Woo; Kim, Hyung Kook; Hwang, Yoon-Hwae
2016-09-01
Recently, the portable and wearable electronic devices, operated in the power range of microwatt to miliwatt, become available thank to the nanotechnology development and become an essential element for a comfortable life. Our recent research interest mainly focuses on the fabrication of piezoelectric nanogenerators based on smart nanomaterials such as zinc oxide novel nanostructure, M13 bacteriophage. In this talk, we present a simple strategy for fabricating the freestanding ZnO nanorods/graphene/ZnO nanorods double sided heterostructures. The characterization of the double sided heterostructures by using SEM, and Raman scattering spectroscopy reveals the key process and working mechanism of a formation of the heterostructure. The mechanism is discussed in detail in term of the decomposed seed layer and the vacancy defect of graphene. The approach consists of a facile one-step fabrication process and could achieve ZnO coverage with a higher number density than that of the epitaxial single heterostructure. The resulting improvement in the number density of nanorods has a direct beneficial effect on the double side heterostructured nanogenerator performance. The total output voltage and current density are improved up to 2 times compared to those of a single heterostructure due to the coupling of the piezoelectric effects from both upward and downward grown nanorods. The facile one-step fabrication process suggests that double sided heterostructures would improve the performance of electrical and optoelectrical device, such as touch pad, pressure sensor, biosensor and dye-sensitized solar cells. Further, ioinspired nanogenerators based on vertically aligned phage nanopillars are inceptively demonstrated. Vertically aligned phage nanopillars enable not only a high piezoelectric response but also a tuneable piezoelectricity. Piezoelectricity is also modulated by tuning of the protein's dipoles in each phage. The sufficient electrical power from phage nanopillars thus holds promise for the development of self-powered implantable and wearable electronics.
Sol–gel synthesis and enhanced photocatalytic activity of doped bismuth tungsten oxide composite
DOE Office of Scientific and Technical Information (OSTI.GOV)
Xu, Xuetang; Ge, Yuanxing; School of Chemistry and Chemical Engineering, Guangxi University, Nanning 530004
2016-01-15
Highlights: • Co dopant results in the phase change from Bi{sub 2}WO{sub 6} to Bi{sub 2}WO{sub 6}/Bi{sub 14}W{sub 2}O{sub 27} heterostructure. • Enhanced photocatalytic activity of Bi{sub 2}WO{sub 6}/Bi{sub 14}W{sub 2}O{sub 27} heterostructure. • Synergistic effects coming from the interactions between Bi{sub 14}W{sub 2}O{sub 27} and Bi{sub 2}WO{sub 6} - Abstract: Pristine Bi{sub 2}WO{sub 6} and Bi{sub 2}WO{sub 6}/Bi{sub 14}W{sub 2}O{sub 27} photocatalysts were synthesized by sol–gel method using Co(II) cation as dopant. The influence of Co dopant to the formation of Bi{sub 2}WO{sub 6}/Bi{sub 14}W{sub 2}O{sub 27} heterostructure composite was discussed. The photocatalytic activities of as-prepared samples were evaluatedmore » sufficiently by using rhodamine B as target organic pollutants under visible light. The as-prepared Bi{sub 2}WO{sub 6}/Bi{sub 14}W{sub 2}O{sub 27} heterostructure achieved enhanced optical absorption in the visible-light region, and exhibited much higher photocatalytic activities than that of pristine Bi{sub 2}WO{sub 6}. The optimum Bi/Co molar ratio and calcining temperature were also explored. The enhanced activities were attributed to the formation of heterostructure in suppressing the recombination of photo-generated carriers. The Co dopant species would participate to reduce the charge carrier recombination by acting as trapping sites for photogenerated charges. A possible photocatalytic mechanism over Bi{sub 2}WO{sub 6}/Bi{sub 14}W{sub 2}O{sub 27} heterostructure was proposed.« less
DOE Office of Scientific and Technical Information (OSTI.GOV)
Hoffman, Jason D.; Kirby, Brian J.; Kwon, Jihwan
Interfaces between correlated complex oxides are promising avenues to realize new forms of magnetism that arise as a result of charge transfer, proximity effects, and locally broken symmetries. We report on the discovery of a noncollinear magnetic structure in superlattices of the ferromagnetic metallic oxide La 2/3Sr 1/3MnO 3 (LSMO) and the correlated metal LaNiO 3 (LNO). The exchange interaction between LSMO layers is mediated by the intervening LNO, such that the angle between the magnetization of neighboring LSMO layers varies in an oscillatory manner with the thickness of the LNO layer. The magnetic field, temperature, and spacer thickness dependencemore » of the noncollinear structure are inconsistent with the bilinear and biquadratic interactions that are used to model the magnetic structure in conventional metallic multilayers. A model that couples the LSMO layers to a helical spin state within the LNO fits the observed behavior. We propose that the spin-helix results from the interaction between a spatially varying spin susceptibility within the LNO and interfacial charge transfer that creates localized Ni 2+ states. In conclusion, our work suggests a new approach to engineering noncollinear spin textures in metallic oxide heterostructures.« less
Water-based and biocompatible 2D crystal inks for all-inkjet-printed heterostructures
NASA Astrophysics Data System (ADS)
McManus, Daryl; Vranic, Sandra; Withers, Freddie; Sanchez-Romaguera, Veronica; Macucci, Massimo; Yang, Huafeng; Sorrentino, Roberto; Parvez, Khaled; Son, Seok-Kyun; Iannaccone, Giuseppe; Kostarelos, Kostas; Fiori, Gianluca; Casiraghi, Cinzia
2017-05-01
Exploiting the properties of two-dimensional crystals requires a mass production method able to produce heterostructures of arbitrary complexity on any substrate. Solution processing of graphene allows simple and low-cost techniques such as inkjet printing to be used for device fabrication. However, the available printable formulations are still far from ideal as they are either based on toxic solvents, have low concentration, or require time-consuming and expensive processing. In addition, none is suitable for thin-film heterostructure fabrication due to the re-mixing of different two-dimensional crystals leading to uncontrolled interfaces and poor device performance. Here, we show a general approach to achieve inkjet-printable, water-based, two-dimensional crystal formulations, which also provide optimal film formation for multi-stack fabrication. We show examples of all-inkjet-printed heterostructures, such as large-area arrays of photosensors on plastic and paper and programmable logic memory devices. Finally, in vitro dose-escalation cytotoxicity assays confirm the biocompatibility of the inks, extending their possible use to biomedical applications.
Yang, Chen; Zhao, Zong-Yan
2017-11-08
In the field of photocatalysis, constructing hetero-structures is an efficient strategy to improve quantum efficiency. However, a lattice mismatch often induces unfavorable interfacial states that can act as recombination centers for photo-generated electron-hole pairs. If the hetero-structure's components have the same crystal structure, this disadvantage can be easily avoided. Conversely, in the process of loading a noble metal co-catalyst onto the TiO 2 surface, a transition layer of noble metal oxides is often formed between the TiO 2 layer and the noble metal layer. In this article, interfacial properties of hetero-structures composed of a noble metal dioxide and TiO 2 with a rutile crystal structure have been systematically investigated using first-principles calculations. In particular, the Schottky barrier height, band bending, and energy band alignments are studied to provide evidence for practical applications. In all cases, no interfacial states exist in the forbidden band of TiO 2 , and the interfacial formation energy is very small. A strong internal electric field generated by interfacial electron transfer leads to an efficient separation of photo-generated carriers and band bending. Because of the differences in the atomic properties of the components, RuO 2 /TiO 2 and OsO 2 /TiO 2 hetero-structures demonstrate band dividing, while RhO 2 /TiO 2 and IrO 2 /TiO 2 hetero-structures have a pseudo-gap near the Fermi energy level. Furthermore, NMO 2 /TiO 2 hetero-structures show upward band bending. Conversely, RuO 2 /TiO 2 and OsO 2 /TiO 2 hetero-structures present a relatively strong infrared light absorption, while RhO 2 /TiO 2 and IrO 2 /TiO 2 hetero-structures show an obvious absorption edge in the visible light region. Overall, considering all aspects of their properties, RuO 2 /TiO 2 and OsO 2 /TiO 2 hetero-structures are more suitable than others for improving the photocatalytic performance of TiO 2 . These findings will provide useful information for understanding the role and effects of a noble metal dioxide as a transition layer between a noble metal co-catalyst and a TiO 2 photocatalyst.
Balanced electron-hole transport in spin-orbit semimetal SrIrO3 heterostructures
NASA Astrophysics Data System (ADS)
Manca, Nicola; Groenendijk, Dirk J.; Pallecchi, Ilaria; Autieri, Carmine; Tang, Lucas M. K.; Telesio, Francesca; Mattoni, Giordano; McCollam, Alix; Picozzi, Silvia; Caviglia, Andrea D.
2018-02-01
Relating the band structure of correlated semimetals to their transport properties is a complex and often open issue. The partial occupation of numerous electron and hole bands can result in properties that are seemingly in contrast with one another, complicating the extraction of the transport coefficients of different bands. The 5 d oxide SrIrO3 hosts parabolic bands of heavy holes and light electrons in gapped Dirac cones due to the interplay between electron-electron interactions and spin-orbit coupling. We present a multifold approach relying on different experimental techniques and theoretical calculations to disentangle its complex electronic properties. By combining magnetotransport and thermoelectric measurements in a field-effect geometry with first-principles calculations, we quantitatively determine the transport coefficients of different conduction channels. Despite their different dispersion relationships, electrons and holes are found to have strikingly similar transport coefficients, yielding a holelike response under field-effect and thermoelectric measurements and a linear electronlike Hall effect up to 33 T.
Electrical breakdown and nanogap formation of indium oxide core/shell heterostructure nanowires.
Jung, Minkyung; Song, Woon; Sung Lee, Joon; Kim, Nam; Kim, Jinhee; Park, Jeunghee; Lee, Hyoyoung; Hirakawa, Kazuhiko
2008-12-10
We report the electrical breakdown behavior and subsequent nanogap formation of In(2)O(3)/InO(x) core/shell heterostructure nanowires with substrate-supported and suspended structures. The radial heterostructure nanowires, composed of crystalline In(2)O(3) cores and amorphous In-rich shells, are grown by chemical vapor deposition. As the nanowires broke down, they exhibited two distinct current drops in the current-voltage characteristics. The tips of the broken nanowires were found to have a cone or a volcano shape depending on the width of the nanowire. The shape, the size, and the position of the nanogap depend strongly on the device structure and the nanowire dimensions. The substrate-supported and the suspended devices exhibit distinct breakdown behavior which can be explained by the diffusive thermal transport model. The breakdown temperature of the nanowire is estimated to be about 450 K, close to the melting temperature of indium. We demonstrated the usefulness of this technique by successful fabrication of working pentacene field-effect transistors.
Exfoliation and van der Waals heterostructure assembly of intercalated ferromagnet Cr1/3TaS2
NASA Astrophysics Data System (ADS)
Yamasaki, Yuji; Moriya, Rai; Arai, Miho; Masubuchi, Satoru; Pyon, Sunseng; Tamegai, Tsuyoshi; Ueno, Keiji; Machida, Tomoki
2017-12-01
Ferromagnetic van der Waals (vdW) materials are in demand for spintronic devices with all-two-dimensional-materials heterostructures. Here, we demonstrate mechanical exfoliation of magnetic-atom-intercalated transition metal dichalcogenide Cr1/3TaS2 from its bulk crystal; previously such intercalated materials were thought difficult to exfoliate. Magnetotransport in exfoliated tens-of-nanometres-thick flakes revealed ferromagnetic ordering below its Curie temperature T C ~ 110 K as well as strong in-plane magnetic anisotropy; these are identical to its bulk properties. Further, van der Waals heterostructure assembly of Cr1/3TaS2 with another intercalated ferromagnet Fe1/4TaS2 is demonstrated using a dry-transfer method. The fabricated heterojunction composed of Cr1/3TaS2 and Fe1/4TaS2 with a native Ta2O5 oxide tunnel barrier in between exhibits tunnel magnetoresistance (TMR), revealing possible spin injection and detection with these exfoliatable ferromagnetic materials through the vdW junction.
NASA Astrophysics Data System (ADS)
Shi, Jinwei; Lin, Meng-Hsien; Chen, Yi-Tong; Estakhri, Nasim Mohammadi; Tseng, Guo-Wei; Wang, Yanrong; Chen, Hung-Ying; Chen, Chun-An; Shih, Chih-Kang; Alã¹, Andrea; Li, Xiaoqin; Lee, Yi-Hsien; Gwo, Shangjr
Recently, two-dimensional (2D) semiconductor heterostructures, i.e., atomically thin lateral heterostructures (LHSs) based on transition metal dichalcogenides (TMDs) have been demonstrated. In an optically excited LHS, exciton transport is typically limited to a rather short spatial range ( 1 micron). Furthermore, additional losses may occur at the lateral interfacial regions. Here, to overcome these challenges, we experimentally implement a planar metal-oxide-semiconductor (MOS) structure by placing a monolayer of WS2/MoS2 LHS on top of an Al2O3 capped Ag single-crystalline plate. We found that the exciton transport range can be extended to tens of microns. The process of long-range exciton transport in the MOS structure is confirmed to be mediated by an exciton-surface plasmon polariton-exciton conversion mechanism, which allows a cascaded energy transfer process. Thus, the planar MOS structure provides a platform seamlessly combining 2D light-emitting materials with plasmonic planar waveguides, offering great potential for developing integrated photonic/plasmonic functionalities.
Kim, Janghyuk; Mastro, Michael A; Tadjer, Marko J; Kim, Jihyun
2017-06-28
β-gallium oxide (β-Ga 2 O 3 ) and hexagonal boron nitride (h-BN) heterostructure-based quasi-two-dimensional metal-insulator-semiconductor field-effect transistors (MISFETs) were demonstrated by integrating mechanical exfoliation of (quasi)-two-dimensional materials with a dry transfer process, wherein nanothin flakes of β-Ga 2 O 3 and h-BN were utilized as the channel and gate dielectric, respectively, of the MISFET. The h-BN dielectric, which has an extraordinarily flat and clean surface, provides a minimal density of charged impurities on the interface between β-Ga 2 O 3 and h-BN, resulting in superior device performances (maximum transconductance, on/off ratio, subthreshold swing, and threshold voltage) compared to those of the conventional back-gated configurations. Also, double-gating of the fabricated device was demonstrated by biasing both top and bottom gates, achieving the modulation of the threshold voltage. This heterostructured wide-band-gap nanodevice shows a new route toward stable and high-power nanoelectronic devices.
Chiu, Chung-Hua; Huang, Chun-Wei; Chen, Jui-Yuan; Huang, Yu-Ting; Hu, Jung-Chih; Chen, Lien-Tai; Hsin, Cheng-Lun; Wu, Wen-Wei
2013-06-07
Copper silicide has been studied in the applications of electronic devices and catalysts. In this study, Cu3Si/Si nanowire heterostructures were fabricated through solid state reaction in an in situ transmission electron microscope (TEM). The dynamic diffusion of the copper atoms in the growth process and the formation mechanism are characterized. We found that two dimensional stacking faults (SF) may retard the growth of Cu3Si. Due to the evidence of the block of edge-nucleation (heterogeneous) by the surface oxide, center-nucleation (homogeneous) is suggested to dominate the silicidation. Furthermore, the electrical transport properties of various silicon channel length with Cu3Si/Si heterostructure interfaces and metallic Cu3Si NWs have been investigated. The observations not only provided an alternative pathway to explore the formation mechanisms and interface properties of Cu3Si/Si, but also suggested the potential application of Cu3Si at nanoscale for future processing in nanotechnology.
Carrad, D J; Burke, A M; Reece, P J; Lyttleton, R W; Waddington, D E J; Rai, A; Reuter, D; Wieck, A D; Micolich, A P
2013-08-14
We have studied the efficacy of (NH4)2Sx surface passivation on the (311)A GaAs surface. We report XPS studies of simultaneously-grown (311)A and (100) heterostructures showing that the (NH4)2Sx solution removes surface oxide and sulfidizes both surfaces. Passivation is often characterized using photoluminescence measurements; we show that while (NH4)2Sx treatment gives a 40-60 × increase in photoluminescence intensity for the (100) surface, an increase of only 2-3 × is obtained for the (311)A surface. A corresponding lack of reproducible improvement in the gate hysteresis of (311)A heterostructure transistor devices made with the passivation treatment performed immediately prior to gate deposition is also found. We discuss possible reasons why sulfur passivation is ineffective for (311)A GaAs, and propose alternative strategies for passivation of this surface.
Facile fabrication of nanofluidic diode membranes using anodic aluminium oxide.
Wu, Songmei; Wildhaber, Fabien; Vazquez-Mena, Oscar; Bertsch, Arnaud; Brugger, Juergen; Renaud, Philippe
2012-09-21
Active control of ion transport plays important roles in chemical and biological analytical processes. Nanofluidic systems hold the promise for such control through electrostatic interaction between ions and channel surfaces. Most existing experiments rely on planar geometry where the nanochannels are generally very long and shallow with large aspect ratios. Based on this configuration the concepts of nanofluidic gating and rectification have been successfully demonstrated. However, device minimization and throughput scaling remain significant challenges. We report here an innovative and facile realization of hetero-structured Al(2)O(3)/SiO(2) (Si) nanopore array membranes by using pattern transfer of self-organized nanopore structures of anodic aluminum oxide (AAO). Thanks to the opposite surface charge states of Al(2)O(3) (positive) and SiO(2) (negative), the membrane exhibits clear rectification of ion current in electrolyte solutions with very low aspect ratios compared to previous approaches. Our hetero-structured nanopore arrays provide a valuable platform for high throughput applications such as molecular separation, chemical processors and energy conversion.
Emergent ultrafast phenomena in correlated oxides and heterostructures
NASA Astrophysics Data System (ADS)
Gandolfi, M.; Celardo, G. L.; Borgonovi, F.; Ferrini, G.; Avella, A.; Banfi, F.; Giannetti, C.
2017-03-01
The possibility of investigating the dynamics of solids on timescales faster than the thermalization of the internal degrees of freedom has disclosed novel non-equilibrium phenomena that have no counterpart at equilibrium. Transition metal oxides (TMOs) provide an interesting playground in which the correlations among the charges in the metal d-orbitals give rise to a wealth of intriguing electronic and thermodynamic properties involving the spin, charge, lattice and orbital orders. Furthermore, the physical properties of TMOs can be engineered at the atomic level, thus providing the platform to investigate the transport phenomena on timescales of the order of the intrinsic decoherence time of the charge excitations. Here, we review and discuss three paradigmatic examples of transient emerging properties that are expected to open new fields of research: (i) the creation of non-thermal magnetic states in spin-orbit Mott insulators; (ii) the possible exploitation of quantum paths for the transport and collection of charge excitations in heterostructures; (iii) the transient wave-like behavior of the temperature field in strongly anisotropic TMOs.
Controllable positive exchange bias via redox-driven oxygen migration
Gilbert, Dustin A.; Olamit, Justin; Dumas, Randy K.; ...
2016-03-21
We report that ionic transport in metal/oxide heterostructures offers a highly effective means to tailor material properties via modification of the interfacial characteristics. However, direct observation of ionic motion under buried interfaces and demonstration of its correlation with physical properties has been challenging. Using the strong oxygen affinity of gadolinium, we design a model system of Gd xFe 1-x/NiCoO bilayer films, where the oxygen migration is observed and manifested in a controlled positive exchange bias over a relatively small cooling field range. The exchange bias characteristics are shown to be the result of an interfacial layer of elemental nickel andmore » cobalt, a few nanometres in thickness, whose moments are larger than expected from uncompensated NiCoO moments. This interface layer is attributed to a redox-driven oxygen migration from NiCoO to the gadolinium, during growth or soon after. Ultimately, these results demonstrate an effective path to tailoring the interfacial characteristics and interlayer exchange coupling in metal/oxide heterostructures.« less
Visualizing Redox Dynamics of a Single Ag/AgCl Heterogeneous Nanocatalyst at Atomic Resolution
DOE Office of Scientific and Technical Information (OSTI.GOV)
Wu, Yimin A.; Li, Liang; Li, Zheng
Operando characterization of gas solid reactions at the atomic scale is of great importance for determining the mechanism of catalysis. This is especially true in the study of heterostructures because of structural correlation between the different parts. However, such experiments are challenging and have rarely been accomplished. In this work, atomic scale redox dynamics of Ag/AgCl heterostructures have been studied using in situ environmental transmission electron microscopy (ETEM) in combination with density function theory (DFT) calculations. The reduction of Ag/AgCl to Ag is likely a result of the formation of Cl vacancies while Ag+ ions accept electrons. The oxidation processmore » of Ag/AgCl has been observed: rather than direct replacement of Cl by O, the Ag/AgCl nanocatalyst was first reduced to Ag, and then Ag was oxidized to different phases of silver oxide under different O-2 partial pressures. Ag2O formed at low O-2 partial pressure, whereas AgO formed at atmospheric pressure. By combining in situ ETEM observation and DFT calculations, this structural evolution is characterized in a distinct nanoscale environment.« less
Heterogeneity in magnetic complex oxides
NASA Astrophysics Data System (ADS)
Arenholz, Elke
Heterogeneity of quantum materials on the nanoscale can result from the spontaneous formation of regions with distinct atomic, electronic and/or magnetic order, and indicates coexistence of competing quantum phases. In complex oxides, the subtle interplay of lattice, charge, orbital, and spin degrees of freedom gives rise to especially rich phase diagrams. For example, coexisting conducting and insulating phases can occur near metal-insulator transitions, colossal magnetoresistance can emerge where ferromagnetic and antiferromagnetic domains compete, and charge-ordered and superconducting regions are present simultaneously in materials exhibiting high-temperature superconductivity. Additionally, externally applied fields (electric, magnetic, or strain) or other external excitations (light or heat) can tip the energy balance towards one phase, or support heterogeneity and phase coexistence and provide the means to perturb and tailor quantum heterogeneity at the nanoscale. Engineering nanomaterials, with structural, electronic and magnetic characteristics beyond what is found in bulk materials, is possible today through the technique of thin film epitaxy, effectively a method of `spray painting' atoms on single crystalline substrates to create precisely customized layered structures with atomic arrangements defined by the underlying substrate. Charge transfer and spin polarization across interfaces as well as imprinting nanoscale heterogeneity between adjacent layers lead to intriguing and important new phenomena testing our understanding of basic physics and creating new functionalities. Moreover, the abrupt change of orientation of an order parameter between nanoscale domains can lead to unique phases that are localized at domain walls, including conducting domain walls in insulating ferroelectrics, and ferromagnetic domain walls in antiferromagnets. Here we present our recent results on tailoring the electronic anisotropy of multiferroic heterostructures by imprinting the BiFeO3 domain pattern in an adjacent La0.7Sr0.3MnO3 layer, understanding the metal-insulator transition in strained VO2 thin films and identifying a three-dimensional quasi-long-range electronic supermodulation in YBa2Cu3O7-x/La0.7Ca0.3MnO3 heterostructures. The Advanced Light Source is supported by the Director, Office of Science, Office of Basic Energy Sciences, of the U.S. Department of Energy under Contract No. DE-AC02-05CH11231.
Strain-induced phenomenon in complex oxide thin films
NASA Astrophysics Data System (ADS)
Haislmaier, Ryan
Complex oxide materials wield an immense spectrum of functional properties such as ferroelectricity, ferromagnetism, magnetoelectricity, optoelectricity, optomechanical, magnetoresistance, superconductivity, etc. The rich coupling between charge, spin, strain, and orbital degrees of freedom makes this material class extremely desirable and relevant for next generation electronic devices and technologies which are trending towards nanoscale dimensions. Development of complex oxide thin film materials is essential for realizing their integration into nanoscale electronic devices, where theoretically predicted multifunctional capabilities of oxides could add tremendous value. Employing thin film growth strategies such as epitaxial strain and heterostructure interface engineering can greatly enhance and even unlock novel material properties in complex oxides, which will be the main focus of this work. However, physically incorporating oxide materials into devices remains a challenge. While advancements in molecular beam epitaxy (MBE) of thin film oxide materials has led to the ability to grow oxide materials with atomic layer precision, there are still major limitations such as controlling stoichiometric compositions during growth as well as creating abrupt interfaces in multi-component layered oxide structures. The work done in this thesis addresses ways to overcome these limitations in order to harness intrinsic material phenomena. The development of adsorption-controlled stoichiometric growth windows of CaTiO3 and SrTiO3 thin film materials grown by hybrid MBE where Ti is supplied using metal-organic titanium tetraisopropoxide material is thoroughly outlined. These growth windows enable superior epitaxial strain-induced ferroelectric and dielectric properties to be accessed as demonstrated by chemical, structural, electrical, and optical characterization techniques. For tensile strained CaTiO3 and compressive strained SrTiO 3 films, the critical effects of nonstoichiometry on ferroelectric properties are investigated, where enhanced ferroelectric responses are only found for stoichiometric films grown inside of the growth windows, whereas outside of the optimal growth window conditions, ferroelectric properties are greatly deteriorated and eventually disappear for highly nonstoichiometric film compositions. Utilizing these stoichiometric growth windows, high temperature polar phase transitions are discovered for compressively strained CaTiO3 films with transition temperatures in excess of 700 K, rendering this material as a strong candidate for high temperature electronic applications. Beyond the synthesis of single phase materials using hybrid MBE, a methodology is presented for constructing layered (SrTiO3)n/(CaTiO 3)n superlattice structures, where precise control over the unit cell layering thickness (n) is demonstrated using in-situ reflection high energy electron diffraction. The effects of interface roughness and layering periodicity (n) on the strain-induced ferroelectric properties for a series of n=1-10 (SrTiO3)n/(CaTiO3) n superlattice films are investigated. It is found that the stabilization of a ferroelectric phase is independent of n, but is however strongly dominated by the degree of interface roughness which is quantified by measuring the highest nth order X-ray diffraction peak splitting of each superlattice film. A counter-intuitive realization is made whereby a critical amount of interface roughness is required in order to enable the formation of the predicted strain-stabilized ferroelectric phase, whereas sharp interfaces actually suppress this ferroelectric phase from manifesting. It is shown how high-quality complex oxide superlattices can be constructed using hybrid MBE technique, allowing the ability to control layered materials at the atomic scale. Furthermore, a detailed growth methodology is provided for constructing a layered n=4 SrO(SrTiO3)n Ruddlesden-Popper (RP) phase by hybrid MBE, where the ability to deposit single monolayers of SrO and TiO2 is utilized to build the RP film structure over a time period of 5 hours. This is the first time that a thin film RP phase has been grown using hybrid MBE, where an a stable control over the fluxes is demonstrated during relatively long time periods of growth, which advantageously facilitates the synthesis of high-quality RP materials with excellent structural and chemical homogeneity. Additionally, this work demonstrates some major advancements in optical second harmonic generation (SHG) characterization techniques of ferroelectric thin film materials. The SHG characterization techniques developed here proved to be the 'bread-and-butter' for most of the work performed in this thesis, providing a powerful tool for identifying the existence of strain-induced ferroelectric phases, including their temperature dependence and polar symmetry. The work presented in this dissertation will hopefully provide a preliminary road map for future hybrid MBE growers, scientists and researchers, to develop and investigate epitaxial strain and heterostructure layering induced phenomena in other complex oxide systems.
Tuning Magnetic Order in Transition Metal Oxide Thin Films
NASA Astrophysics Data System (ADS)
Grutter, Alexander John
In recent decades, one of the most active and promising areas of condensed matter research has been that of complex oxides. With the advent of new growth techniques such as pulsed laser deposition and molecular beam epitaxy, a wealth of new magnetic and electronic ground states have emerged in complex oxide heterostructures. The wide variety of ground states in complex oxides is well known and generally attributed to the unprecedented variety of valence, structure, and bonding available in these systems. The tunability of this already diverse playground of states and interactions is greatly multiplied in thin films and heterostructures by the addition of parameters such as substrate induced strain and interfacial electronic reconstruction. Thus, recent studies have shown emergent properties such as the stabilization of ferromagnetism in a paramagnetic system, conductivity at the interface of two insulators, and even exchange bias at the interface between a paramagnet and a ferromagnet. Despite these steps forward, there remains remarkable disagreement on the mechanisms by which these emergent phenomena are stabilized. The contributions of strain, stoichiometry, defects, intermixing, and electronic reconstruction are often very difficult to isolate in thin films and superlattices. This thesis will present model systems for isolating the effects of strain and interfacial electronic interactions on the magnetic state of complex oxides from alternative contributions. We will focus first on SrRuO3, an ideal system in which to isolate substrate induced strain effects. We explore the effects of structural distortions in the simplest case of growth on (100) oriented substrates. We find that parameters including saturated magnetic moment and Curie temperature are all highly tunable through substrate induced lattice distortions. We also report the stabilization of a nonmagnetic spin-zero configuration of Ru4+ in tetragonally distorted films under tensile strain. Through growth on (110) and (111) oriented substrates we explore the effects of different distortion symmetries on SrRuO3 and demonstrate the first reported strain induced transition to a high-spin state of Ru 4+. Finally, we examine the effects of strain on SrRuO3 thin films and demonstrate a completely reversible universal out-of-plane magnetic easy axis on films grown on different substrate orientations. Having demonstrated the ability to tune nearly every magnetic parameter of SrRuO 3 through strain, we turn to magnetic properties at interfaces. We study the emergent interfacial ferromagnetism in superlattices of the paramagnetic metal CaRuO3 and the antiferromagnetic insulator CaMnO3 and demonstrate that the interfacial ferromagnetic layer in this system is confined to a single unit cell of CaMnO3 at the interface. We discuss the remarkable oscillatory dependence of the saturated magnetic moment on the thickness of the CaMnO3 layers and explore mechanisms by which this oscillation may be stabilized. We find long range coherence of the antiferromagnetism of the CaMnO3 layers across intervening layers of paramagnetic CaRuO3. Finally, we utilize the system of LaNiO3/CaMnO3 to separate the effects of intermixing and interfacial electronic reconstruction and conclusively demonstrate intrinsic interfacial ferromagnetism at the interface between a paramagnetic metal and an antiferromagnetic insulator. We find that the emergent ferromagnetism is stabilized through interfacial double exchange and that the leakage of conduction electrons from the paramagnetic metal to the antiferromagnetic insulator is critical to establishing the ferromagnetic ground state.
Wang, Shuangbao; Bai, Yuhang; Xie, Lin; Li, Chen; Key, Julian D; Wu, Di; Wang, Peng; Pan, Xiaoqing
2018-01-10
Interfacial fine structures of bare LaAlO 3 /SrTiO 3 (LAO/STO) heterostructures are compared with those of LAO/STO heterostructures capped with upward-polarized Pb(Zr 0.1 ,Ti 0.9 )O 3 (PZT up ) or downward-polarized Pb(Zr 0.5 ,Ti 0.5 )O 3 (PZT down ) overlayers by aberration-corrected scanning transmission electron microscopy experiments. By combining the acquired electron energy-loss spectroscopy mapping, we are able to directly observe electron transfer from Ti 4+ to Ti 3+ and ionic displacements at the interface of bare LAO/STO and PZT down /LAO/STO heterostructure unit cell by unit cell. No evidence of Ti 3+ is observed at the interface of the PZT up /LAO/STO samples. Furthermore, the confinement of the two-dimensional electron gas (2DEG) at the interface is determined by atomic-column spatial resolution. Compared with the bare LAO/STO interface, the 2DEG density at the LAO/STO interface is enhanced or depressed by the PZT down or PZT up overlayer, respectively. Our microscopy studies shed light on the mechanism of ferroelectric modulation of interfacial transport at polar/nonpolar oxide heterointerfaces, which may facilitate applications of these materials as nonvolatile memory.
Limbach, F.; Gotschke, T.; Stoica, T.; ...
2011-01-01
InGaN/GaN nanowire (NW) heterostructures grown by plasma assisted molecular beam epitaxy were studied in comparison to their GaN and InGaN counterparts. The InGaN/GaN heterostructure NWs are composed of a GaN NW, a thin InGaN shell, and a multifaceted InGaN cap wrapping the top part of the GaN NW. High-resolution transmission electron microscopy (HRTEM) images taken from different parts of a InGaN/GaN NW show a wurtzite structure of the GaN core and the epitaxial InGaN shell around it, while additional crystallographic domains are observed whithin the InGaN cap region. Large changes in the lattice parameter along the wire, from pure GaNmore » to higher In concentration demonstrate the successful growth of a complex InGaN/GaN NW heterostructure. Photoluminescence (PL) spectra of these heterostructure NW ensembles show rather broad and intense emission peak at 2.1 eV. However, μ-PL spectra measured on single NWs reveal a reduced broadening of the visible luminescence. The analysis of the longitudinal optical phonon Raman peak position and its shape reveal a variation in the In content between 20% and 30%, in agreement with the values estimated by PL and HRTEM investigations. The reported studies are important for understanding of the growth and properties of NW heterostructures suitable for applications in optoelectronics and photovoltaics.« less
NASA Astrophysics Data System (ADS)
Limbach, F.; Gotschke, T.; Stoica, T.; Calarco, R.; Sutter, E.; Ciston, J.; Cusco, R.; Artus, L.; Kremling, S.; Höfling, S.; Worschech, L.; Grützmacher, D.
2011-01-01
InGaN/GaN nanowire (NW) heterostructures grown by plasma assisted molecular beam epitaxy were studied in comparison to their GaN and InGaN counterparts. The InGaN/GaN heterostructure NWs are composed of a GaN NW, a thin InGaN shell, and a multifaceted InGaN cap wrapping the top part of the GaN NW. High-resolution transmission electron microscopy (HRTEM) images taken from different parts of a InGaN/GaN NW show a wurtzite structure of the GaN core and the epitaxial InGaN shell around it, while additional crystallographic domains are observed whithin the InGaN cap region. Large changes in the lattice parameter along the wire, from pure GaN to higher In concentration demonstrate the successful growth of a complex InGaN/GaN NW heterostructure. Photoluminescence (PL) spectra of these heterostructure NW ensembles show rather broad and intense emission peak at 2.1 eV. However, μ-PL spectra measured on single NWs reveal a reduced broadening of the visible luminescence. The analysis of the longitudinal optical phonon Raman peak position and its shape reveal a variation in the In content between 20% and 30%, in agreement with the values estimated by PL and HRTEM investigations. The reported studies are important for understanding of the growth and properties of NW heterostructures suitable for applications in optoelectronics and photovoltaics.
NASA Astrophysics Data System (ADS)
Chiu, Ya-Ping; Huang, Bo-Chao; Shih, Min-Chuan; Huang, Po-Cheng; Chen, Chun-Wei
2015-09-01
Interfacial science has received much attention recently based on the development of state-of-the-art analytical tools that can create and manipulate the charge, spin, orbital, and lattice degrees of freedom at interfaces. Motivated by the importance of nanoscale interfacial science that governs device operation, we present a technique to probe the electronic characteristics of heterointerfaces with atomic resolution. In this work, the interfacial characteristics of heteroepitaxial structures are investigated and the fundamental mechanisms that pertain in these systems are elucidated through cross-sectional scanning tunneling microscopy (XSTM). The XSTM technique is employed here to directly observe epitaxial interfacial structures and probe local electronic properties with atomic-level capability. Scanning tunneling microscopy and spectroscopy experiments with atomic precision provide insight into the origin and spatial distribution of electronic properties across heterointerfaces. The first part of this report provides a brief description of the cleavage technique and spectroscopy analysis in XSTM measurements. The second part addresses interfacial electronic structures of several model heterostructures in current condensed matter research using XSTM. Topics to be discussed include high-κ‘s/III-V’s semiconductors, polymer heterojunctions, and complex oxide heterostructures, which are all material systems whose investigation using this technique is expected to benefit the research community. Finally, practical aspects and perspectives of using XSTM in interface science are presented.
Single InAs/GaSb nanowire low-power CMOS inverter.
Dey, Anil W; Svensson, Johannes; Borg, B Mattias; Ek, Martin; Wernersson, Lars-Erik
2012-11-14
III-V semiconductors have so far predominately been employed for n-type transistors in high-frequency applications. This development is based on the advantageous transport properties and the large variety of heterostructure combinations in the family of III-V semiconductors. In contrast, reports on p-type devices with high hole mobility suitable for complementary metal-oxide-semiconductor (CMOS) circuits for low-power operation are scarce. In addition, the difficulty to integrate both n- and p-type devices on the same substrate without the use of complex buffer layers has hampered the development of III-V based digital logic. Here, inverters fabricated from single n-InAs/p-GaSb heterostructure nanowires are demonstrated in a simple processing scheme. Using undoped segments and aggressively scaled high-κ dielectric, enhancement mode operation suitable for digital logic is obtained for both types of transistors. State-of-the-art on- and off-state characteristics are obtained and the individual long-channel n- and p-type transistors exhibit minimum subthreshold swings of SS = 98 mV/dec and SS = 400 mV/dec, respectively, at V(ds) = 0.5 V. Inverter characteristics display a full signal swing and maximum gain of 10.5 with a small device-to-device variability. Complete inversion is measured at low frequencies although large parasitic capacitances deform the waveform at higher frequencies.
NASA Astrophysics Data System (ADS)
Kondo, A.; Yin, G.; Srinivasan, N.; Atarashi, D.; Sakai, E.; Miyauchi, M.
2015-07-01
Metal oxide and quantum dot (QD) heterostructures have attracted considerable recent attention as materials for developing efficient solar cells, photocatalysts, and display devices, thus nanoscale imaging of trapped electrons in these heterostructures provides important insight for developing efficient devices. In the present study, Kelvin probe force microscopy (KPFM) of CdS quantum dot (QD)-grafted Cs4W11O362- nanosheets was performed before and after visible-light irradiation. After visible-light excitation of the CdS QDs, the Cs4W11O362- nanosheet surface exhibited a decreased work function in the vicinity of the junction with CdS QDs, even though the Cs4W11O362- nanosheet did not absorb visible light. X-ray photoelectron spectroscopy revealed that W5+ species were formed in the nanosheet after visible-light irradiation. These results demonstrated that excited electrons in the CdS QDs were injected and trapped in the Cs4W11O362- nanosheet to form color centers. Further, the CdS QDs and Cs4W11O362- nanosheet composite films exhibited efficient remote photochromic coloration, which was attributed to the quantum nanostructure of the film. Notably, the responsive wavelength of the material is tunable by adjusting the size of QDs, and the decoloration rate is highly efficient, as the required length for trapped electrons to diffuse into the nanosheet surface is very short owing to its nanoscale thickness. The unique properties of this photochromic device make it suitable for display or memory applications. In addition, the methodology described in the present study for nanoscale imaging is expected to aid in the understanding of electron transport and trapping processes in metal oxide and metal chalcogenide heterostructure, which are crucial phenomena in QD-based solar cells and/or photocatalytic water-splitting systems.Metal oxide and quantum dot (QD) heterostructures have attracted considerable recent attention as materials for developing efficient solar cells, photocatalysts, and display devices, thus nanoscale imaging of trapped electrons in these heterostructures provides important insight for developing efficient devices. In the present study, Kelvin probe force microscopy (KPFM) of CdS quantum dot (QD)-grafted Cs4W11O362- nanosheets was performed before and after visible-light irradiation. After visible-light excitation of the CdS QDs, the Cs4W11O362- nanosheet surface exhibited a decreased work function in the vicinity of the junction with CdS QDs, even though the Cs4W11O362- nanosheet did not absorb visible light. X-ray photoelectron spectroscopy revealed that W5+ species were formed in the nanosheet after visible-light irradiation. These results demonstrated that excited electrons in the CdS QDs were injected and trapped in the Cs4W11O362- nanosheet to form color centers. Further, the CdS QDs and Cs4W11O362- nanosheet composite films exhibited efficient remote photochromic coloration, which was attributed to the quantum nanostructure of the film. Notably, the responsive wavelength of the material is tunable by adjusting the size of QDs, and the decoloration rate is highly efficient, as the required length for trapped electrons to diffuse into the nanosheet surface is very short owing to its nanoscale thickness. The unique properties of this photochromic device make it suitable for display or memory applications. In addition, the methodology described in the present study for nanoscale imaging is expected to aid in the understanding of electron transport and trapping processes in metal oxide and metal chalcogenide heterostructure, which are crucial phenomena in QD-based solar cells and/or photocatalytic water-splitting systems. Electronic supplementary information (ESI) available. See DOI: 10.1039/c5nr02405f
Multifunctional epitaxial systems on silicon substrates
DOE Office of Scientific and Technical Information (OSTI.GOV)
Singamaneni, Srinivasa Rao, E-mail: ssingam@ncsu.edu; Materials Science Division, Army Research Office, Research Triangle Park, North Carolina 27709; Department of Physics, The University of Texas at El Paso, El Paso, Texas 79968
2016-09-15
Multifunctional heterostructures can exhibit a wide range of functional properties, including colossal magneto-resistance, magnetocaloric, and multiferroic behavior, and can display interesting physical phenomena including spin and charge ordering and strong spin-orbit coupling. However, putting this functionality to work remains a challenge. To date, most of the work reported in the literature has dealt with heterostructures deposited onto closely lattice matched insulating substrates such as DyScO{sub 3}, SrTiO{sub 3} (STO), or STO buffered Si(100) using concepts of lattice matching epitaxy (LME). However, strain in heterostructures grown by LME is typically not fully relaxed and the layers contain detrimental defects such asmore » threading dislocations that can significantly degrade the physical properties of the films and adversely affect the device characteristics. In addition, most of the substrates are incompatible with existing CMOS-based technology, where Si (100) substrates dominate. This review discusses recent advances in the integration of multifunctional oxide and non-oxide materials onto silicon substrates. An alternative thin film growth approach, called “domain matching epitaxy,” is presented which identifies approaches for minimizing lattice strain and unwanted defects in large misfit systems (7%–25% and higher). This approach broadly allows for the integration of multifunctional materials onto silicon substrates, such that sensing, computation, and response functions can be combined to produce next generation “smart” devices. In general, pulsed laser deposition has been used to epitaxially grow these materials, although the concepts developed here can be extended to other deposition techniques, as well. It will be shown that TiN and yttria-stabilized zirconia template layers provide promising platforms for the integration of new functionality into silicon-based computer chips. This review paper reports on a number of thin-film heterostructure systems that span a variety of ferroelectric, multiferroic, magnetic, photocatalytic, and smart materials. Their properties have been extensively investigated and their functionality found to be comparable to films grown on single-crystal oxide substrates previously reported by researchers in this field. In addition, this review explores the utility of using laser processing to introduce stable defects in a controlled way and induce magnetism and engineer the optical and electrical properties of nonmagnetic oxides such as BaTiO{sub 3}, VO{sub 2}, NiO, and TiO{sub 2} as an alternative for incorporating additional magnetic and conducting layers into the structure. These significant materials advancements herald a flurry of exciting new advances in CMOS-compatible multifunctional devices.« less
Nanoscale Strontium Titanate Sheets and Crystals
NASA Astrophysics Data System (ADS)
Tilka, Jack Andrew
The physical properties of materials are dominated by their structure and composition. Insight into the structure of complex oxide materials has the potential to improve our understanding and eventually control of their physical properties. This PhD thesis reports the development of characterization and fabrication techniques relevant to improving the scientific understanding of complex oxide materials. The work presented here has two components. I report a way to use ideas that were originally developed in semiconductor processing to control the elastic strain state and crystallization process of the model complex oxide SrTiO3. An additional component is an important series of advances in the analysis of diffraction patterns acquired with focused x-ray nanobeams. The fabrication and characterization of nanoscale SrTiO3 has been experimentally shown to allow the introduction of elastic strain into SrTiO3. The creation of thin SrTiO3 crystals from (001)-oriented SrTiO3 bulk single crystals using focused ion beam milling techniques yields sheets with submicron thickness and arbitrary orientation within the (001) plane. Synchrotron x-ray nanodiffraction experiments show that the SrTiO 3 sheets have rocking curves with angular widths less than 0.02°. These widths are less than a factor of two larger than bulk SrTiO3, which shows that the sheets are suitable substrates for epitaxial thin film growth. A precisely selected elastic strain can be introduced into the SrTiO 3 sheets using a silicon nitride stressor layer. Synchrotron x-ray nanodiffraction studies show that the strain introduced in the SrTiO3 sheets is on the order of 10-4, matching the predictions of an elastic model. This approach to elastic strain sharing in complex oxides allows the strain to be selected within a wide and continuous range of values, an effect not achievable in heteroepitaxy on rigid substrates. An additional fabrication technique is also evaluated here based on the crystallization of SrTiO3 from initially amorphous thin films. This process is known as solid-phase epitaxy in two-dimensional samples but is just beginning to be explored in more complex geometries. I report experiments in both homoepitaxy and heteroepitaxy including measurements of crystal growth rates and the crystallographic orientations of crystals formed in this way. The lateral growth rates are consistent with previously measured vertical growth. This result indicated that previous work on vertical solid-phase epitaxy could be extended into lateral solid-phase epitaxy, which has the power to be applied to complicated non-planar geometries. The highly coherent and tightly focused x-ray beams produced by hard x-ray light sources enable the nanoscale structural characterization of materials but are accompanied by significant challenges in the interpretation of diffraction and scattering patterns. I report here a series of methods that expand the range of physical problems that can be accurately captured by coherent x-ray optical simulations. My approach has been to expand simulations methods to include arbitrary x-ray incident angles and arbitrary epitaxial heterostructures. I first applied these methods to extract the misorientation of lattice planes and the strain of individual layers of Si/SiGe heterostructures relevant to applications in quantum electronics. Further applications reported in this thesis are in probing defects created in the processing of SrTiO3 and in measuring the change in lattice parameter introduced into strained SrTiO3 sheets. The systematic interpretation of nanobeam diffraction patterns aids in the fabrication of SrTiO3 nanostructures.
Valence-state reflectometry of complex oxide heterointerfaces
Hamann-Borrero, Jorge E.; Macke, Sebastian; Choi, Woo Seok; ...
2016-09-16
Emergent phenomena in transition-metal-oxide heterostructures such as interface superconductivity and magnetism have been attributed to electronic reconstruction, which, however, is difficult to detect and characterise. Here we overcome the associated difficulties to simultaneously address the electronic degrees of freedom and distinguish interface from bulk effects by implementing a novel approach to resonant X-ray reflectivity (RXR). Our RXR study of the chemical and valance profiles along the polar (001) direction of a LaCoO 3 film on NdGaO 3 reveals a pronounced valence-state reconstruction from Co 3+ in the bulk to Co 2+ at the surface, with an areal density close tomore » 0.5 Co 2+ ions per unit cell. An identical film capped with polar (001) LaAlO 3 maintains the Co 3+ valence over its entire thickness. As a result, we interpret this as evidence for electronic reconstruction in the uncapped film, involving the transfer of 0.5e – per unit cell to the subsurface CoO 2 layer at its LaO-terminated polar surface.« less
Electric polarization control of magnetoresistance in complex oxide heterojunctions
NASA Astrophysics Data System (ADS)
Swartz, Adrian G.; Inoue, Hisashi; Hwang, Harold Y.
2016-10-01
Lorentzian magnetoresistance (L-MR) has been widely observed in three-terminal ferromagnet-nonmagnet (FM-NM) tunnel junctions. One possible explanation for this behavior is ensemble dephasing (Hanle effect) of a spin accumulation, potentially offering a powerful approach for characterizing the spin lifetime of emerging spintronics materials. However, discrepancies between the extracted spin parameters with known materials properties has cast doubt on this interpretation for most implementations. Here, we have developed a method to control band alignments in perovskite oxide heterostructures through the use of epitaxial interface dipoles, providing a highly effective method for manipulating the Schottky barrier height and contact resistance. Using these atomically engineered heterojunctions, we are able to tune key parameters relevant to various spin accumulation models, providing an experimental platform which can test their applicability. We find that the observed L-MR is inconsistent with an interpretation of spin accumulation in either the NM material or in interface states. Rather, we consider a mechanism analogous to Coulomb blockade in quantum dots, where spin-dependent tunneling through an ensemble of interfacial defect states is controlled by local and external magnetic fields.
Layer-by-layer growth by pulsed laser deposition in the unit-cell limit.
NASA Astrophysics Data System (ADS)
Kareev, M.; Prosandeev, S.; Liu, J.; Ryan, P.; Freeland, J. W.; Chakhalian, J.
2009-03-01
Unlike conventional growth of complex oxide heterostructures, the ultimate unit cell limit imposes strict constrains for a multitude of parameters critical to layer-by-layer growth. Here we report on detailed analysis of far-from-equilibrium growth by interrupted pulsed laser deposition with application to RENiO3/LaAlO3 superlattices grown on a diverse set of substrates SrTiO3, NdGaO3, LSAT and LaAlO3. A combination of in-situ high-pressure RHEED and AFM along with extensive data obtained from synchrotron based XRD and resonant XAS allows us critically assess the meaning of RHEED intensity oscillation and the effect of a polar/non-polar interface on the heteroepitaxial growth. The role of defects formed during the initial stages of growth is also addressed.
Interdiffusion-driven synthesis of tetragonal chromium (III) oxide on BaTi O3
NASA Astrophysics Data System (ADS)
Asa, M.; Vinai, G.; Hart, J. L.; Autieri, C.; Rinaldi, C.; Torelli, P.; Panaccione, G.; Taheri, M. L.; Picozzi, S.; Cantoni, M.
2018-03-01
Interfaces play a crucial role in the study of novel phenomena emerging at heterostructures comprising metals and functional oxides. For this reason, attention should be paid to the interface chemistry, which can favor the interdiffusion of atomic species and, under certain conditions, lead to the formation of radically different compounds with respect to the original constituents. In this work, we consider Cr/BaTi O3 heterostructures grown on SrTi O3 (100) substrates. Chromium thin films (1-2 nm thickness) are deposited by molecular beam epitaxy on the BaTi O3 layer, and subsequently annealed in vacuum at temperatures ranging from 473 to 773 K. A disordered metallic layer is detected for annealing temperatures up to 573 K, whereas, at higher temperatures, we observe a progressive oxidation of chromium, which we relate to the thermally activated migration of oxygen from the substrate. The chromium oxidation state is +3 and the film shows a defective rocksalt structure, which grows lattice matched on the underlying BaTi O3 layer. One out of every three atoms of chromium is missing, producing an uncommon tetragonal phase with C r2O3 stoichiometry. Despite the structural difference with respect to the ordinary corundum α-C r2O3 phase, we demonstrate both experimentally and theoretically that the electronic properties of the two phases are, to a large extent, equivalent.
NASA Astrophysics Data System (ADS)
Xiao, Jian-Hua; Huang, Wei-Qing; Hu, Yong-sheng; Zeng, Fan; Huang, Qin-Yi; Zhou, Bing-Xin; Pan, Anlian; Li, Kai; Huang, Gui-Fang
2018-02-01
High photocatalytic activity and photostability are the pursuit of the goal for designing promising photocatalysts. Herein, using ZnO to encapsulate ZnS nanoparticles is proposed as an effective strategy to enhance photocatalytic activity and anti-photocorrosion. The ZnS/ZnO core/shell heterostructures are obtained via an annealing treatment of ZnS nanoparticles produced by a facile wet chemical approach. Due to its small size, the nascent cubic sphalerite ZnS (s-ZnS) converts into a hexagonal wurtzite ZnS (w-ZnS)/ZnO core/shell structure after annealing treatment. In situ oxidation leads to increasing ZnO, simultaneously decreasing the w-ZnS content in the resultant w-ZnS/ZnO with thermal annealing time. The w-ZnS/ZnO core/shell heterostructures show high photocatalytic activity, demonstrated by the photodegradation rate of methylene blue being up to ten-fold and seven-fold higher than that of s-ZnS under UV and visible light irradiation, respectively, and the high capability of degrading rhodamine B. The enhanced photocatalytic activity may be attributed to the large specific surface and improved charge carrier separation at the core/shell interface. Moreover, it displays high photostability owing to the protection of the ZnO shell, greatly inhibiting the photocorrosion of ZnS. This facile in situ oxidation is effective and easily scalable, providing opportunities for developing novel core/shell structure photocatalysts with high activity and photostability.
Li, Chia-Hsun; Hsu, Chan-Wei; Lu, Shih-Yuan
2018-07-01
TiO 2 nanocrystals decorated core-shell CdS-CdO nanorod arrays, TiO 2 @CdO/CdS NR, were fabricated as high efficiency anodes for photoelctrochemical hydrogen generation. The novel sandwich heterostructure was constructed from first growth of CdS nanorod arrays on a fluorine doped tin oxide (FTO) substrate with a hydrothermal process, followed by in situ generation of CdO thin films of single digit nanometers from the CdS nanorod surfaces through thermal oxidation, and final decoration of TiO 2 nanocrystals of 10-20 nm via a successive ionic layer absorption and reaction process. The core-shell CdS-CdO heterostructure possesses a Z-scheme band structure to enhance interfacial charge transfer, facilitating effective charge separation to suppress electron-hole recombination within CdS for much improved current density generation. The final decoration of TiO 2 nanocrystals passivates surface defects and trap states of CdO, further suppressing surface charge recombination for even higher photovoltaic conversion efficiencies. The photoelectrochemical performances of the plain CdS nanorod array were significantly improved with the formation of the sandwich heterostructure, achieving a photo current density of 3.2 mA/cm 2 at 1.23 V (vs. RHE), a 141% improvement over the plain CdS nanorod array and a 32% improvement over the CdO/CdS nanorod array. Copyright © 2018 Elsevier Inc. All rights reserved.
Process dependency on threshold voltage of GaN MOSFET on AlGaN/GaN heterostructure
NASA Astrophysics Data System (ADS)
Wang, Qingpeng; Jiang, Ying; Miyashita, Takahiro; Motoyama, Shin-ichi; Li, Liuan; Wang, Dejun; Ohno, Yasuo; Ao, Jin-Ping
2014-09-01
GaN metal-oxide-semiconductor field-effect transistors (MOSFETs) with recessed gate on AlGaN/GaN heterostructure are reported in which the drain and source ohmic contacts were fabricated on the AlGaN/GaN heterostructure and the electron channel was formed on the GaN buffer layer by removing the AlGaN barrier layer. Negative threshold voltages were commonly observed in all devices. To investigate the reasons of the negative threshold voltages, different oxide thickness, etching gas and bias power of inductively-coupled plasma (ICP) system were utilized in the fabrication process of the GaN MOSFETs. It is found that positive charges of around 1 × 1012 q/cm2 exist near the interface at the just threshold condition in both silane- and tetraethylorthosilicate (TEOS)-based devices. It is also found that the threshold voltages do not obviously change with the different etching gas (SiCl4, BCl3 and two-step etching of SiCl4/Cl2) at the same ICP bias power level (20-25 W) and will become deeper when higher bias power is used in the dry recess process which may be related to the much serious ion bombardment damage. Furthermore, X-ray photoelectron spectroscopy (XPS) experiments were done to investigate the surface conditions. It is found that N 1s peaks become lower with higher bias power of the dry etching process. Also, silicon contamination was found and could be removed by HNO3/HF solution. It indicates that the nitrogen vacancies are mainly responsible for the negative threshold voltages rather than the silicon contamination. It demonstrates that optimization of the ICP recess conditions and improvement of the surface condition are still necessary to realize enhancement-mode GaN MOSFETs on AlGaN/GaN heterostructure.
NASA Astrophysics Data System (ADS)
Kim, Gunwoo
Magnetoelectric random access memory (MERAM) has emerged as a promising new class of non-volatile solid-state memory device. It offers nondestructive reading along with low power consumption during the write operation. A common implementation of MERAM involves use of multiferroic tunneling junctions (MFTJs), which besides offering non-volatility are both electrically and magnetically tunable. Fundamentally, a MFTJ consists of a heterostructure of an ultrathin multiferroic or ferroelectric material as the active tunneling barrier sandwiched between ferromagnetic electrodes. Thereby, the MFTJ exhibits both tunnel electroresistance (TER) and tunnel magnetoresistance (TMR) effects with application of an electric and magnetic field, respectively. In this thesis work, we have developed two-dimensional (2D) thin-film multiferroic heterostructure METJ prototypes consisting of ultrathin ferroelectric BaTiO3 (BTO) layer and a conducting ferromagnetic La0.67Sr 0.33MnO3 (LSMO) electrode. The heteroepitaxial films are grown using the pulsed laser deposition (PLD) technique. This oxide heterostructure offers the opportunity to study the nano-scale details of the tunnel electroresistance (TER) effect using scanning probe microscopy techniques. We performed the measurements using the MFP-3D (Asylum Research) scanning probe microscope. The ultrathin BTO films (1.2-2.0 nm) grown on LSMO electrodes display both ferro- and piezo-electric properties and exhibit large tunnel resistance effect. We have explored the growth and properties of one-dimensional (1D) heterostructures, referred to as multiferoric nanowire (NW) heterostructures. The ferromagnetic/ferroelectric composite heterostructures are grown as sheath layers using PLD on lattice-matched template NWs, e.g. MgO, that are deposited by chemical vapor deposition utilizing the vapor-liquid-solid (VLS) mechanism. The one-dimensional geometry can substantially overcome the clamping effect of the substrate present in two-dimensional structures because of the reduced volume of the template. This leads to minimum constraint of displacements at the interface and thereby significantly enhances the magnetoelectric (ME) effect. We characterized the nanostructures using scanning electron microscopy (SEM) and transmission electron microscopy (TEM). The results of our studies utilizing multiferroic 2-D thin films and 1-D NW architectures clearly demonstrate the potential of these heterostructures for future device applications, such as in MERAM, data storage, magneto-electric field sensors, etc.
Facile fabrication of nanofluidic diode membranes using anodic aluminium oxide
NASA Astrophysics Data System (ADS)
Wu, Songmei; Wildhaber, Fabien; Vazquez-Mena, Oscar; Bertsch, Arnaud; Brugger, Juergen; Renaud, Philippe
2012-08-01
Active control of ion transport plays important roles in chemical and biological analytical processes. Nanofluidic systems hold the promise for such control through electrostatic interaction between ions and channel surfaces. Most existing experiments rely on planar geometry where the nanochannels are generally very long and shallow with large aspect ratios. Based on this configuration the concepts of nanofluidic gating and rectification have been successfully demonstrated. However, device minimization and throughput scaling remain significant challenges. We report here an innovative and facile realization of hetero-structured Al2O3/SiO2 (Si) nanopore array membranes by using pattern transfer of self-organized nanopore structures of anodic aluminum oxide (AAO). Thanks to the opposite surface charge states of Al2O3 (positive) and SiO2 (negative), the membrane exhibits clear rectification of ion current in electrolyte solutions with very low aspect ratios compared to previous approaches. Our hetero-structured nanopore arrays provide a valuable platform for high throughput applications such as molecular separation, chemical processors and energy conversion.Active control of ion transport plays important roles in chemical and biological analytical processes. Nanofluidic systems hold the promise for such control through electrostatic interaction between ions and channel surfaces. Most existing experiments rely on planar geometry where the nanochannels are generally very long and shallow with large aspect ratios. Based on this configuration the concepts of nanofluidic gating and rectification have been successfully demonstrated. However, device minimization and throughput scaling remain significant challenges. We report here an innovative and facile realization of hetero-structured Al2O3/SiO2 (Si) nanopore array membranes by using pattern transfer of self-organized nanopore structures of anodic aluminum oxide (AAO). Thanks to the opposite surface charge states of Al2O3 (positive) and SiO2 (negative), the membrane exhibits clear rectification of ion current in electrolyte solutions with very low aspect ratios compared to previous approaches. Our hetero-structured nanopore arrays provide a valuable platform for high throughput applications such as molecular separation, chemical processors and energy conversion. Electronic supplementary information (ESI) available: Pattern transfer of local AAO mask into Si layers of different thickness; characterization of the Ag/AgCl electrodes and the cell constant; control experiments of mono-charged nanopore membranes; and simulation of ionic transport in nanofluidic diodes. See DOI: 10.1039/c2nr31243c
NASA Astrophysics Data System (ADS)
Nohavica, D.; Têminová, J.; Berková, D.; Zagrádková, M.; Kortan, I.; Zelinka, I.; Walachová, I.; Malina, V.
1988-11-01
A modified single-phase liquid phase epitaxy method was developed on the basis of a novel variant of the growth boat. The method was used to grow GaInAsP/InP double heterostructures for lasers emitting at 1.3 and 1.55 μm. The main properties of wide-contact diodes (radiation power and threshold current density) were adopted as the characteristics of the quality of heterostructures characterized by different configurations of active and guiding layers. The quality of the structure was confirmed by the fabrication of laser diodes of the following types: stripe with oxide insulation, clad-ridge waveguide, and double-channel planar buried.
NASA Astrophysics Data System (ADS)
Borisov, Vladislav; Schuetz, Philipp; Pfaff, Florian; Scheiderer, Philipp; Dudy, Lenart; Zapf, Michael; Gabel, Judith; Christensen, Dennis Valbjorn; Chen, Yunzhong; Pryds, Nini; Strocov, Vladimir; Rogalev, Victor; Schlueter, Christoph; Lee, Tien-Lin; Jeschke, Harald O.; Valenti, Roser; Sing, Michael; Claessen, Ralph
Oxygen vacancies in oxide heterostructures create a plethora of electronic phenomena not observed in the stoichiometric systems. In this talk we will discuss the presence of a new type of in-gap states at the spinel/perovskite γ-Al2O3/SrTiO3 interface, as observed in soft x-ray resonant photoemission spectroscopy. Based on ab initio calculations and crystal-field analysis of different atomic environments, we identify the origin of this behavior and we argue on the possible origin of the extraordinarily high electron mobility measured in this heterostructure. This work was financially supported by the Deutsche Forschungsgemeinschaft SFB/TR 49 and SFB 1170.
Ultrafast Study of Dynamic Exchange Coupling in Ferromagnet/Oxide/Semiconductor Heterostructures
NASA Astrophysics Data System (ADS)
Ou, Yu-Sheng
Spintronics is the area of research that aims at utilizing the quantum mechanical spin degree of freedom of electrons in solid-state materials for information processing and data storage application. Since the discovery of the giant magnetoresistance, the field of spintronics has attracted lots of attention for its numerous potential advantages over contemporary electronics, such as less power consumption, high integration density and non-volatility. The realization of a spin battery, defined by the ability to create spin current without associated charge current, has been a long-standing goal in the field of spintronics. The demonstration of pure spin current in ferromagnet/nonmagnetic material hybrid structures by ferromagnetic resonance spin pumping has defined a thrilling direction for this field. As such, this dissertation targets at exploring the spin and magnetization dynamics in ferromagnet/oxide/semiconductor heterostructures (Fe/MgO/GaAs) using time-resolved optical pump-probe spectroscopy with the long-range goal of understanding the fundamentals of FMR-driven spin pumping. Fe/GaAs heterostructures are complex systems that contain multiple spin species, including paramagnetic spins (GaAs electrons), nuclear spins (Ga and As nuclei) and ferromagnetic spins (Fe). Optical pump-probe studies on their interplay have revealed a number of novel phenomena that has not been explored before. As such they will be the major focus of this dissertation. First, I will discuss the effect of interfacial exchange coupling on the GaAs free-carrier spin relaxation. Temperature- and field-dependent spin-resolved pump-probe studies reveal a strong correlation of the electron spin relaxation with carrier freeze-out, in quantitative agreement with a theoretical interpretation that at low temperatures the free-carrier spin lifetime is dominated by inhomogeneity in the local hyperfine field due to carrier localization. Second, we investigate the impact of tunnel barrier thickness on GaAs electron spin dynamics in Fe/MgO/GaAs heterostructures. Comparison of the Larmor frequency between samples with thick and thin MgO barriers reveals a four-fold variation in exchange coupling strength, and investigation of the spin lifetimes argues that inhomogeneity in the local hyperfine field dominates free-carrier spin relaxation across the entire range of barrier thickness. These results provide additional evidence to support the theory of hyperfine-dominated spin relaxation in GaAs. Third, we investigated the origin and dynamics of an emergent spin population by pump power and magnetic field dependent spin-resolved pump-probe studies. Power dependent study confirms its origin to be filling of electronic states in GaAs, and further field dependent studies reveal the impact of contact hyperfine coupling on the dynamics of electron spins occupying distinct electronic states. Beyond above works, we also pursue optical detection of dynamic spin pumping in Fe/MgO/GaAs heterostructures in parallel. I will discuss the development and progress that we have made toward this goal. This project can be simply divided into two phases. In the first phase, we focused on microwave excitation and optical detection of spin pumping. In the second phase, we focused on all-optical excitation and detection of spin pumping. A number of measurement strategies have been developed and executed in both stages to hunt for a spin pumping signal. I will discuss the preliminary data based upon them.
Development of Energy-Efficient Single-Electron Transistors with Oxide Nanoelectronics
2011-05-01
Eom, and J. Levy, "“ Water - cycle ” mechanism for writing and erasing nanostructures at the LaAlO3/SrTiO3 interface," Appl. Phys. Lett. 97, 173110 (2010...process as a “ water cycle ” because it permits multiple writing and erasing without physical modification of the oxide heterostructure. Figure 8...test of the “ water cycle ” mechanism outlined above replaces atmospheric conditions with gas environments that lack H2O. Figure 9(a-c) shows the
Tunable magnetism in the LaAlO3/SrTiO3 heterostructure: Insights from first-principles calculations
NASA Astrophysics Data System (ADS)
Xue, Yuanbin; Zhao, Jinzhu; Shan, Yueyue; Xu, Hu
2018-04-01
By performing first-principles calculations, we explored the origin and controlling methods of magnetism in ideal and oxygen deficient (001) LaAlO3/SrTiO3 (LAO/STO) heterostructures. It was found that the ferromagnetic ordering is the ground state and that the interfacial Ti 3d electrons introduced by the LaO-termination, polar catastrophe and oxygen vacancies can all contribute to the magnetism. With respect to the ways of tuning the magnetic properties, our results show that LaO-terminated films generally carry much stronger magnetic moments than their AlO2-terminated counterparts and that the magnitude of magnetic moments can also be effectively controlled by the LAO film thickness. In addition, oxygen vacancy leads to substantial electronic reconstruction of the interfacial Ti 3d orbitals, which enhances the magnetization and makes the magnetism emerge in thinner polar LAO films. This work offers useful information to facilitate one's understanding of the magnetism and to provide clues to engineer the magnetic behaviors in related oxide heterostructures.
Chen, Yu-Ze; Wang, Sheng-Wen; Su, Teng-Yu; Lee, Shao-Hsin; Chen, Chia-Wei; Yang, Chen-Hua; Wang, Kuangye; Kuo, Hao-Chung; Chueh, Yu-Lun
2018-05-01
Phase-engineered type-II metal-selenide heterostructures are demonstrated by directly selenizing indium-tin oxide to form multimetal selenides in a single step. The utilization of a plasma system to assist the selenization facilitates a low-temperature process, which results in large-area films with high uniformity. Compared to single-metal-selenide-based photodetectors, the multimetal-selenide photodetectors exhibit obviously improved performance, which can be attributed to the Schottky contact at the interface for tuning the carrier transport, as well as the type-II heterostructure that is beneficial for the separation of the electron-hole pairs. The multimetal-selenide photodetectors exhibit a response to light over a broad spectrum from UV to visible light with a high responsivity of 0.8 A W -1 and an on/off current ratio of up to 10 2 . Interestingly, all-transparent photodetectors are successfully produced in this work. Moreover, the possibility of fabricating devices on flexible substrates is also demonstrated with sustainable performance, high strain tolerance, and high durability during bending tests. © 2018 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.
NASA Astrophysics Data System (ADS)
Belenchuk, A.; Shapoval, O.; Roddatis, V.; Bruchmann-Bamberg, V.; Samwer, K.; Moshnyaga, V.
2016-12-01
We report on the interface engineering in correlated manganite heterostructures by octahedral decoupling using embedded stacks of atomic layers that form the Ruddlesden-Popper structure. A room temperature magnetic decoupling was achieved through deposition of a (SrO)2-TiO2-(SrO)2 sequence of atomic layers at the interface between La0.7Sr0.3MnO3 and La0.7Sr0.3Mn0.9Ru0.1O3 films. Moreover, the narrowing of the interfacial dead layer in ultrathin La0.7Sr0.3MnO3 films was demonstrated by insertion of a single (SrO)2 rock-salt layer at the interface with the SrTiO3(100) substrate. The obtained results are discussed based on the symmetry breaking and disconnection of the MnO6 octahedra network at the interface that may lead to the improved performance of all-oxide magnetic tunnel junctions. We suggest that octahedral decoupling realized by formation of Ruddlesden-Popper interfaces is an effective structural mechanism to control functionalities of correlated perovskite heterostructures.
He, Xuexia; Chow, WaiLeong; Liu, Fucai; Tay, BengKang; Liu, Zheng
2017-01-01
2D transition metal dichalcogenides are promising channel materials for the next-generation electronic device. Here, vertically 2D heterostructures, so called van der Waals solids, are constructed using inorganic molybdenum sulfide (MoS 2 ) few layers and organic crystal - 5,6,11,12-tetraphenylnaphthacene (rubrene). In this work, ambipolar field-effect transistors are successfully achieved based on MoS 2 and rubrene crystals with the well balanced electron and hole mobilities of 1.27 and 0.36 cm 2 V -1 s -1 , respectively. The ambipolar behavior is explained based on the band alignment of MoS 2 and rubrene. Furthermore, being a building block, the MoS 2 /rubrene ambipolar transistors are used to fabricate CMOS (complementary metal oxide semiconductor) inverters that show good performance with a gain of 2.3 at a switching threshold voltage of -26 V. This work paves a way to the novel organic/inorganic ultrathin heterostructure based flexible electronics and optoelectronic devices. © 2016 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.
Ferromagnet / superconductor oxide superlattices
NASA Astrophysics Data System (ADS)
Santamaria, Jacobo
2006-03-01
The growth of heterostructures combining oxide materials is a new strategy to design novel artificial multifunctional materials with interesting behaviors ruled by the interface. With the (re)discovery of colossal magnetoresistance (CMR) materials, there has been renewed interest in heterostructures involving oxide superconductors and CMR ferromagnets where ferromagnetism (F) and superconductivity (S) compete within nanometric distances from the interface. In F/S/F structures involving oxides, interfaces are especially complex and various factors like interface disorder and roughness, epitaxial strain, polarity mismatch etc., are responsible for depressed magnetic and superconducting properties at the interface over nanometer length scales. In this talk I will focus in F/S/F structures made of YBa2Cu3O7 (YBCO) and La0.7Ca0.3MnO3 (LCMO). The high degree of spin polarization of the LCMO conduction band, together with the d-wave superconductivity of the YBCO make this F/S system an adequate candidate for the search of novel spin dependent effects in transport. We show that superconductivity at the interface is depressed by various factors like charge transfer, spin injection or ferromagnetic superconducting proximity effect. I will present experiments to examine the characteristic distances of the various mechanisms of superconductivity depression. In particular, I will discuss that the critical temperature of the superconductor depends on the relative orientation of the magnetization of the F layers, giving rise to a new giant magnetoresistance effect which might be of interest for spintronic applications. Work done in collaboration with V. Peña^1, Z. Sefrioui^1, J. Garcia-Barriocanal^1, C. Visani^1, D. Arias^1, C. Leon^1 , N. Nemes^2, M. Garcia Hernandez^2, S. G. E. te Velthuis^3, A. Hoffmann^3, M. Varela^4, S. J. Pennycook^4. Work supported by MCYT MAT 2005-06024, CAM GR- MAT-0771/2004, UCM PR3/04-12399 Work at Argonne supported by the Department of Energy, Basic Energy Sciences, contract No.W-31-109-ENG-38. ^1GFMC, Departamento de F'isica Aplicada III, Universidad Complutense de Madrid, 28040 Madrid, Spain ^2Instituto de Ciencia de Materiales de Madrid (ICMM-CSIC). 28049 Cantoblanco. Madrid. ^3Materials Science Division, Argonne National Laboratory, Argonne, Illinois 60439, USA ^4Condensed Matter Sciences Division, Oak Ridge National Laboratory, Oak Ridge, Tennessee 37831-6031, USA
Zhu, Gangbing; Yi, Yinhui; Han, Zhixiang; Wang, Kun; Wu, Xiangyang
2014-10-03
Being awfully harmful to the environment and human health, the qualitative and quantitative determinations of polycyclic aromatic amines (PAAs) are of great significance. In this paper, a novel core-shell heterostructure of multiwalled carbon nanotubes (MWCNTs) as the core and graphene oxide nanoribbons (GONRs) as the shell (MWCNTs@GONRs) was produced from longitudinal partially unzipping of MWCNTs side walls using a simple wet chemical strategy and applied for electrochemical determination of three kinds of PAAs (1-aminopyrene (1-AP), 1-aminonaphthalene and 3,3'-diaminobiphenyl). Scanning electron microscopy, transmission electron microscopy, Fourier transform infrared spectroscopy, Raman spectroscopy, thermogravimetric analysis and electrochemical methods were used to characterize the as-prepared MWCNTs@GONRs. Due to the synergistic effects from MWCNTs and GONRs, the oxidation currents of PAAs at the MWCNTs@GONRs modified glassy carbon (GC) electrode are much higher than that at the MWCNTs/GC, graphene/GC and bare GC electrodes. 1-AP was used as the representative analyte to demonstrate the sensing performance of the MWCNTs@GONRs/GC electrode, and the proposed modified electrode has a linear response range of 8.0-500.0 nM with a detection limit of 1.5 nM towards 1-AP. Copyright © 2014 Elsevier B.V. All rights reserved.
NASA Astrophysics Data System (ADS)
Sivakumar, Chockalingam
Efficient electrical spin injection from half-metal (HM) electrodes into semiconducting (SC) channel material is a desirable aspect in spintronics, but a challenging one. Half-metals based on the Heusler alloy family are promising candidates as spin sources due to their compatibility with compound SCs, and very high Curie temperatures. Numerous efforts were made in the past two decades to grow atomically abrupt interfaces between HM_Heusler and SC heterostructures. However, diffusion of magnetic impurities into the semiconductor, defects and disorder near the interface, and formation of reacted phases were great challenges. A number of theoretical efforts were undertaken to understand the role of such material defects in destroying the half-metallicity and also to propose promising half-metal/SC heterostructures based on first principles. This dissertation summarizes the investigations undertaken to decode the complexity of, and to understand the various physical properties of, a number of real-world Heusler/SC heterostructure samples, based on the ab initio density functional theory (DFT) approach. In addition, it summarizes various results from the first principles-based search for promising half-metal/SC heterostructures. First, I present results from DFT-based predictive models of actual Co 2MnSi (CMS)/GaAs heterostructures grown in (001) texture. I investigate the physical, chemical, electronic, and magnetic properties to understand the complexity of these structures and to pinpoint the origin of interfacial effects, when present. Based on the investigations of such models, I discuss the utility of those actual samples in spintronic applications. Next, I summarise the results from an ab initio DFT-based survey of 6 half-Heusler half-metal/GaAs heterostructure models in (110) texture, since compound semiconductors such as GaAs have very long spin lifetime in (110) layering. I show 3 half-Heusler alloys (CoVAs, NiMnAs, and RhFeGe), that when interfaced with GaAs(110), fully preserve the half-metallicity at the interface. Finally, I show the advantages of inserting half-Heusler SCs, particularly CoTiAs and CoTiSb, as spacers in between CMS/GaAs systems in (110) layering. Based on DFT calculations, I show that CoTiAs is a promising spacer that could enhance the perpendicular magnetic anisotropy in CMS, while preserving the important half-metallic character at the heterojunctions between CMS/CoTiAs/GaAs(110). This spacer could also serve to prevent in-diffusion of magnetic impurities into the channel material.
Photoelectrochemical enhancement of ZnO/BiVO4/ZnFe2O4/rare earth oxide hetero-nanostructures
NASA Astrophysics Data System (ADS)
She, Xuefeng; Zhang, Zhuo; Baek, Minki; Yong, Kijung
2018-01-01
Over the decades, researchers have made great efforts to turn the world into a cleaner place through efficient recycling of industrial waste and developing of green energy. Here we demonstrate a prototype heterostructure photoelectrochemical (PEC) cell fabricated using recycled industrial waste. ZnFe2O4 (ZFO) nanorod (NR) clusters were synthesized on the BiVO4@ZnO hetero-nanostructures using recycled rare earth oxide (REO) slags as Fe source. The NR-based PEC cell exhibited a significantly enhanced photon to hydrogen conversion efficiency over the entire UV and visible spectrum. Further study demonstrates that the photo-carrier separation and migration processes can be facilitated by the cascade band alignment of the heterostructure and the clustered nanostructure network. In addition, the life-time of the photo-carriers can be enhanced by the REO passivation layer, leading to a further increased PEC performance. Our results present a novel approach for high efficiency PEC cells, and offer great promises to the efficient recycling of industrial waste for clean renewable energy applications.
Oxide-mediated recovery of field-effect mobility in plasma-treated MoS2
Jadwiszczak, Jakub; O’Callaghan, Colin; Zhou, Yangbo; Fox, Daniel S.; Weitz, Eamonn; Keane, Darragh; Cullen, Conor P.; O’Reilly, Ian; Downing, Clive; Shmeliov, Aleksey; Maguire, Pierce; Gough, John J.; McGuinness, Cormac; Ferreira, Mauro S.; Bradley, A. Louise; Boland, John J.; Duesberg, Georg S.; Nicolosi, Valeria; Zhang, Hongzhou
2018-01-01
Precise tunability of electronic properties of two-dimensional (2D) nanomaterials is a key goal of current research in this field of materials science. Chemical modification of layered transition metal dichalcogenides leads to the creation of heterostructures of low-dimensional variants of these materials. In particular, the effect of oxygen-containing plasma treatment on molybdenum disulfide (MoS2) has long been thought to be detrimental to the electrical performance of the material. We show that the mobility and conductivity of MoS2 can be precisely controlled and improved by systematic exposure to oxygen/argon plasma and characterize the material using advanced spectroscopy and microscopy. Through complementary theoretical modeling, which confirms conductivity enhancement, we infer the role of a transient 2D substoichiometric phase of molybdenum trioxide (2D-MoOx) in modulating the electronic behavior of the material. Deduction of the beneficial role of MoOx will serve to open the field to new approaches with regard to the tunability of 2D semiconductors by their low-dimensional oxides in nano-modified heterostructures. PMID:29511736
Topological properties and functionalities in oxide thin films and interfaces
NASA Astrophysics Data System (ADS)
Uchida, Masaki; Kawasaki, Masashi
2018-04-01
As symbolized by the Nobel Prize in Physics 2016, ‘topology’ has been recognized as an essential standpoint to understand and control the physics of condensed matter. This concept may be spreading even into application areas such as novel electronics. In this trend, there has been reported a number of studies for oxide films and heterostructures with topologically non-trivial electronic or magnetic states. In this review, we overview the trends of new topological properties and functionalities in oxide materials by sorting out a number of examples. The technological advances in oxide film growth achieved over the last few decades are now opening the door for harnessing novel topological properties.
Pathway to oxide photovoltaics via band-structure engineering of SnO
Peng, Haowei; Bikowski, Andre; Zakutayev, Andriy; ...
2016-10-04
All-oxide photovoltaics could open rapidly scalable manufacturing routes, if only oxide materials with suitable electronic and optical properties were developed. SnO has exceptional doping and transport properties among oxides, but suffers from a strongly indirect band gap. Here, we address this shortcoming by band-structure engineering through isovalent but heterostructural alloying with divalent cations (Mg, Ca, Sr, and Zn). Furthermore, using first-principles calculations, we show that suitable band gaps and optical properties close to that of direct semiconductors are achievable, while the comparatively small effective masses are preserved in the alloys. Initial thin film synthesis and characterization support the feasibility ofmore » the approach.« less
Integration of functional oxides and semiconductors
NASA Astrophysics Data System (ADS)
Demkov, Alex
2012-10-01
The astounding progress of recent years in the area of oxide deposition has made possible the creation of oxide heterostructures with atomically abrupt interfaces. The ability to control the length scale, strain, and orbital order in these materials structures offers a uniquely rich toolbox for condensed matter physicists. Because the oxide layers are very thin, the physics is often controlled by the interface. The electronic properties of oxide interfaces are governed by a subtle interplay of many competing interactions such as strain, polar catastrophe, electron correlation, and Jahn-Teller coupling, as well as by defects and phase stability. It is not clear which, if any, of these newly discovered systems will find applications in future high-tech devices. However, they undoubtedly hold tremendous promise, particularly when integrated with conventional semiconductors such as Si. In this talk I will review our recent results in theoretical modeling and experimental realization of several epitaxial oxide heterostructures. I will set the stage with a brief discussion of extrinsic magnetoelectric coupling at the interface of a perovskite ferroelectric and conventional ferromagnet. I will then describe our recent successful attempt to integrate anatase, a photo-catalytic polymorph of TiO2, with Si (001) using molecular beam epitaxy. In conclusion, I will talk about strain stabilized ferromagnetism in correlated LaCoO3 (LCO) and monolithic integration of LCO and silicon for possible applications in spintronics. The integration is achieved via the single crystal SrTiO3 (STO) buffer epitaxially grown on Si. Superconducting quantum interference device magnetization measurements show that, unlike the bulk material, the ground state of the strained LaCoO3 on silicon is ferromagnetic with a TC of 85 K.
NASA Astrophysics Data System (ADS)
Winkler, Christian; Harivyasi, Shashank S.; Zojer, Egbert
2018-07-01
Van der Waals heterostructures based on the heteroassembly of 2D materials represent a recently developed class of materials with promising properties especially for optoelectronic applications. The alignment of electronic energy bands between consecutive layers of these heterostructures crucially determines their functionality. In the present paper, relying on dispersion-corrected density-functional theory calculations, we present electrostatic design as a promising tool for manipulating this band alignment. The latter is achieved by inserting a layer of aligned polar molecules between consecutive transition-metal dichalcogenide (TMD) sheets. As a consequence, collective electrostatic effects induce a shift of as much as 0.3 eV in the band edges of successive TMD layers. Building on that, the proposed approach can be used to design electronically more complex systems, like quantum cascades or quantum wells, or to change the type of band lineup between type II and type I.
Ohmic contact formation between metal and AlGaN/GaN heterostructure via graphene insertion
NASA Astrophysics Data System (ADS)
Sung Park, Pil; Reddy, Kongara M.; Nath, Digbijoy N.; Yang, Zhichao; Padture, Nitin P.; Rajan, Siddharth
2013-04-01
A simple method for the creation of Ohmic contact to 2D electron gas in AlGaN/GaN high electron-mobility transistors using Cr/graphene layer is demonstrated. A weak temperature dependence of this Ohmic contact observed in the range 77 to 300 K precludes thermionic emission or trap-assisted hopping as possible carrier-transport mechanisms. It is suggested that the Cr/graphene combination acts akin to a doped n-type semiconductor in contact with AlGaN/GaN heterostructure, and promotes carrier transport along percolating Al-lean paths through the AlGaN layer. This use of graphene offers a simple method for making Ohmic contacts to AlGaN/GaN heterostructures, circumventing complex additional processing steps involving high temperatures. These results could have important implications for the fabrication and manufacturing of AlGaN/GaN-based microelectronic and optoelectronic devices/sensors of the future.
Ha, Enna; Liu, Wei; Wang, Luyang; Man, Ho-Wing; Hu, Liangsheng; Tsang, Shik Chi Edman; Chan, Chris Tsz-Leung; Kwok, Wai-Ming; Lee, Lawrence Yoon Suk; Wong, Kwok-Yin
2017-01-03
Hydrogen generation from water using noble metal-free photocatalysts presents a promising platform for renewable and sustainable energy. Copper-based chalcogenides of earth-abundant elements, especially Cu 2 ZnSnS 4 (CZTS), have recently arisen as a low-cost and environment-friendly material for photovoltaics and photocatalysis. Herein, we report a new heterostructure consisting of CZTS nanoparticles anchored onto a MoS 2 -reduced graphene oxide (rGO) hybrid. Using a facile two-step method, CZTS nanoparticles were in situ grown on the surface of MoS 2 -rGO hybrid, which generated high density of nanoscale interfacial contact between CZTS and MoS 2 -rGO hybrid. The photoexcited electrons of CZTS can be readily transported to MoS 2 through rGO backbone, reducing the electron-hole pair recombination. In photocatalytic hydrogen generation under visible light irradiation, the presence of MoS 2 -rGO hybrids enhanced the hydrogen production rate of CZTS by 320%, which can be attributed to the synergetic effect of increased charge separation by rGO and more catalytically active sites from MoS 2 . Furthermore, this CZTS/MoS 2 -rGO heterostructure showed much higher photocatalytic activity than both Au and Pt nanoparticle-decorated CZTS (Au/CZTS and Pt/CZTS) photocatalysts, indicating the MoS 2 -rGO hybrid is a better co-catalyst for photocatalytic hydrogen generation than the precious metal. The CZTS/MoS 2 -rGO system also demonstrated stable photocatalytic activity for a continuous 20 h reaction.
NASA Astrophysics Data System (ADS)
Ha, Enna; Liu, Wei; Wang, Luyang; Man, Ho-Wing; Hu, Liangsheng; Tsang, Shik Chi Edman; Chan, Chris Tsz-Leung; Kwok, Wai-Ming; Lee, Lawrence Yoon Suk; Wong, Kwok-Yin
2017-01-01
Hydrogen generation from water using noble metal-free photocatalysts presents a promising platform for renewable and sustainable energy. Copper-based chalcogenides of earth-abundant elements, especially Cu2ZnSnS4 (CZTS), have recently arisen as a low-cost and environment-friendly material for photovoltaics and photocatalysis. Herein, we report a new heterostructure consisting of CZTS nanoparticles anchored onto a MoS2-reduced graphene oxide (rGO) hybrid. Using a facile two-step method, CZTS nanoparticles were in situ grown on the surface of MoS2-rGO hybrid, which generated high density of nanoscale interfacial contact between CZTS and MoS2-rGO hybrid. The photoexcited electrons of CZTS can be readily transported to MoS2 through rGO backbone, reducing the electron-hole pair recombination. In photocatalytic hydrogen generation under visible light irradiation, the presence of MoS2-rGO hybrids enhanced the hydrogen production rate of CZTS by 320%, which can be attributed to the synergetic effect of increased charge separation by rGO and more catalytically active sites from MoS2. Furthermore, this CZTS/MoS2-rGO heterostructure showed much higher photocatalytic activity than both Au and Pt nanoparticle-decorated CZTS (Au/CZTS and Pt/CZTS) photocatalysts, indicating the MoS2-rGO hybrid is a better co-catalyst for photocatalytic hydrogen generation than the precious metal. The CZTS/MoS2-rGO system also demonstrated stable photocatalytic activity for a continuous 20 h reaction.
Ha, Enna; Liu, Wei; Wang, Luyang; Man, Ho-Wing; Hu, Liangsheng; Tsang, Shik Chi Edman; Chan, Chris Tsz-Leung; Kwok, Wai-Ming; Lee, Lawrence Yoon Suk; Wong, Kwok-Yin
2017-01-01
Hydrogen generation from water using noble metal-free photocatalysts presents a promising platform for renewable and sustainable energy. Copper-based chalcogenides of earth-abundant elements, especially Cu2ZnSnS4 (CZTS), have recently arisen as a low-cost and environment-friendly material for photovoltaics and photocatalysis. Herein, we report a new heterostructure consisting of CZTS nanoparticles anchored onto a MoS2-reduced graphene oxide (rGO) hybrid. Using a facile two-step method, CZTS nanoparticles were in situ grown on the surface of MoS2-rGO hybrid, which generated high density of nanoscale interfacial contact between CZTS and MoS2-rGO hybrid. The photoexcited electrons of CZTS can be readily transported to MoS2 through rGO backbone, reducing the electron-hole pair recombination. In photocatalytic hydrogen generation under visible light irradiation, the presence of MoS2-rGO hybrids enhanced the hydrogen production rate of CZTS by 320%, which can be attributed to the synergetic effect of increased charge separation by rGO and more catalytically active sites from MoS2. Furthermore, this CZTS/MoS2-rGO heterostructure showed much higher photocatalytic activity than both Au and Pt nanoparticle-decorated CZTS (Au/CZTS and Pt/CZTS) photocatalysts, indicating the MoS2-rGO hybrid is a better co-catalyst for photocatalytic hydrogen generation than the precious metal. The CZTS/MoS2-rGO system also demonstrated stable photocatalytic activity for a continuous 20 h reaction. PMID:28045066
Orbital engineering of nickelates in three-component heterostructures
NASA Astrophysics Data System (ADS)
Disa, Ankit; Kumah, Divine; Malashevich, Andrei; Chen, Hanghui; Ismail-Beigi, Sohrab; Walker, Fred; Ahn, Charles; Specht, Eliot; Arena, Dario
2015-03-01
The orbital configuration of complex oxides dictates the emergence of a wide range of properties, including metal-insulator transitions, interfacial magnetism, and high-temperature superconductivity. In this work, we experimentally demonstrate a novel method for achieving large and tunable orbital polarizations in nickelates. The technique is based on leveraging three-component, atomically layered superlattices to yield a combination of inversion symmetry breaking, charge transfer, and polar distortions. In the system we studied, composed of LaTiO3/LaNiO3/LaAlO3, we use synchrotron x-ray diffraction and spectroscopy to characterize these properties and show that they lead to fully broken orbital degeneracy in the nickelate layer consistent with a single-band Fermi surface. Furthermore, we show that this system is widely tunable and enables quasi-continuous orbital control unachievable by conventional strain and confinement-based approaches. This technique provides an experimentally realizable route for accessing and studying novel orbitally dependent quantum phenomena.
Micrometer-Scale Ballistic Transport of Electron Pairs in LaAlO_{3}/SrTiO_{3} Nanowires.
Tomczyk, Michelle; Cheng, Guanglei; Lee, Hyungwoo; Lu, Shicheng; Annadi, Anil; Veazey, Joshua P; Huang, Mengchen; Irvin, Patrick; Ryu, Sangwoo; Eom, Chang-Beom; Levy, Jeremy
2016-08-26
High-mobility complex-oxide heterostructures and nanostructures offer new opportunities for extending the paradigm of quantum transport beyond the realm of traditional III-V or carbon-based materials. Recent quantum transport investigations with LaAlO_{3}/SrTiO_{3}-based quantum dots reveal the existence of a strongly correlated phase in which electrons form spin-singlet pairs without becoming superconducting. Here, we report evidence for the micrometer-scale ballistic transport of electron pairs in quasi-1D LaAlO_{3}/SrTiO_{3} nanowire cavities. In the paired phase, Fabry-Perot-like quantum interference is observed, in sync with conductance oscillations observed in the superconducting regime (at a zero magnetic field). Above a critical magnetic field B_{p}, the electron pairs unbind and the conductance oscillations shift with the magnetic field. These experimental observations extend the regime of ballistic electronic transport to strongly correlated phases.
H2 gas sensing properties of a ZnO/CuO and ZnO/CuO/Cu2O Heterostructures
NASA Astrophysics Data System (ADS)
Ababii, N.; Postica, V.; Hoppe, M.; Adelung, R.; Lupan, O.; Railean, S.; Pauporté, T.; Viana, B.
2017-03-01
The most important parameters of gas sensors are sensitivity and especially high selectivity to specific chemical species. To improve these parameters we developed sensor structures based on layered semiconducting oxides, namely CuO/Cu2O, CuO:Zn/Cu2O:Zn, NiO/ZnO. In this work, the ZnO/CuxO (where x = 1, 2) bi-layer heterostructure were grown via a simple synthesis from chemical solution (SCS) at relatively low temperatures (< 95 °C), representing a combination of layered n-type and p-type semiconducting oxides which are widely used as sensing material for gas sensors. The main advantages of the developed device structures are given by simplicity of the synthesis and technological cost-efficiency. Structural investigations showed high crystallinity of synthesized layers confirming the presence of zinc oxide nanostructures on the surface of the copper oxide film deposited on glass substrate. Structural changes in morphology of grown nanostructures induced by post-grown thermal annealing were observed by scanning electron microscopy (SEM) investigations, and were studied in detail. The influence of thermal annealing type on the optical properties was also investigated. As an example of practical applications, the ZnO/CuxO bi-layer heterojunctions and ZnO/CuO/Cu2O three-layered structures were integrated into sensor structures and were tested to different types of reducing gases at different operating temperatures (OPT), showing promising results for fabrication of selective gas sensors.
Zhang, Wen; Fan, Guozheng; Yi, Huan; Jia, Gan; Li, Zhaosheng; Yuan, Chunwei; Bai, Yunfei; Fu, Degang
2018-05-01
Hydrogen peroxide (H 2 O 2 ) is a major messenger molecule in cellular signal transduction. Direct detection of H 2 O 2 in complex environments provides the capability to illuminate its various biological functions. With this in mind, a novel electrochemical approach is here proposed by integrating a series of CoO nanostructures on CuO backbone at electrode interfaces. High-resolution transmission electron microscopy (HRTEM), X-ray diffraction, and X-ray photoelectron spectroscopy demonstrate successful formation of core-shell CuO-CoO hetero-nanostructures. Theoretical calculations further confirm energy-favorable adsorption of H 2 O 2 on surface sites of CuO-CoO heterostructures. Contributing to the efficient electron transfer path and enhanced capture of H 2 O 2 in the unique leaf-like CuO-CoO hierarchical 3D interface, an optimal biosensor-based CuO-CoO-2.5 h electrode exhibits an ultrahigh sensitivity (6349 µA m m -1 cm -2 ), excellent selectivity, and a wide detection range for H 2 O 2 , and is capable of monitoring endogenous H 2 O 2 derived from human lung carcinoma cells A549. The synergistic effects for enhanced H 2 O 2 adsorption in integrated CuO-CoO nanostructures and performance of the sensor suggest a potential for exploring pathological and physiological roles of reactive oxygen species like H 2 O 2 in biological systems. © 2018 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.
Selective tuning of high-Q silicon photonic crystal nanocavities via laser-assisted local oxidation.
Chen, Charlton J; Zheng, Jiangjun; Gu, Tingyi; McMillan, James F; Yu, Mingbin; Lo, Guo-Qiang; Kwong, Dim-Lee; Wong, Chee Wei
2011-06-20
We examine the cavity resonance tuning of high-Q silicon photonic crystal heterostructures by localized laser-assisted thermal oxidation using a 532 nm continuous wave laser focused to a 2.5 μm radius spot-size. The total shift is consistent with the parabolic rate law. A tuning range of up to 8.7 nm is achieved with ∼ 30 mW laser powers. Over this tuning range, the cavity Qs decreases from 3.2×10(5) to 1.2×10(5). Numerical simulations model the temperature distributions in the silicon photonic crystal membrane and the cavity resonance shift from oxidation.
Kale, Sayali B; Kalubarme, Ramchandra S; Mahadadalkar, Manjiri A; Jadhav, Harsharaj S; Bhirud, Ashwini P; Ambekar, Jalinder D; Park, Chan-Jin; Kale, Bharat B
2015-12-21
Hierarchical 3D ZnIn2S4/graphene (ZnIn2S4/Gr) nano-heterostructures were successfully synthesized using an in-situ hydrothermal method. The dual functionality of these nano-heterostructures i.e. for solar hydrogen production and lithium ion batteries has been demonstrated for the first time. The ZnIn2S4/Gr nano-heterostructures were optimized by varying the concentrations of graphene for utmost hydrogen production. An inspection of the structure shows the existence of layered hexagonal ZnIn2S4 wrapped in graphene. The reduction of graphene oxide (GO) to graphene was confirmed by Raman and XPS analyses. The morphological analysis demonstrated that ultrathin ZnIn2S4 nanopetals are dispersed on graphene sheets. The optical study reveals the extended absorption edge to the visible region due to the presence of graphene and hence is used as a photocatalyst to transform H2S into eco-friendly hydrogen using solar light. The ZnIn2S4/Gr nano-heterostructure that is comprised of graphene and ZnIn2S4 in a weight ratio of 1 : 99 exhibits enhanced photocatalytically stable hydrogen production i.e. ∼6365 μmole h(-1) under visible light irradiation using just 0.2 g of nano-heterostructure, which is much higher as compared to bare hierarchical 3D ZnIn2S4. The heightened photocatalytic activity is attributed to the enhanced charge carrier separation due to graphene which acts as an excellent electron collector and transporter. Furthermore, the usage of nano-heterostructures and pristine ZnIn2S4 as anodes in lithium ion batteries confers the charge capacities of 590 and 320 mA h g(-1) after 220 cycles as compared to their initial reversible capacities of 645 and 523 mA h g(-1), respectively. These nano-heterostructures show high reversible capacity, excellent cycling stability, and high-rate capability indicating their potential as promising anode materials for LIBs. The excellent performance is due to the nanostructuring of ZnIn2S4 and the presence of a graphene layer, which works as a channel for the supply of electrons during the charge-discharge process. More significantly, their dual functionality in energy generation and storage is quite unique and commendable.
NASA Astrophysics Data System (ADS)
Tian, Qingyong; Wu, Wei; Yang, Shuanglei; Liu, Jun; Yao, Weijing; Ren, Feng; Jiang, Changzhong
2017-03-01
Flower-like MoS2 nanoparticles (NPs) consist of ultra-thin MoS2 nanosheets are synthesized via a facile one-pot hydrothermal method. The MoS2/ZnO p-n heterostructure is formed by coating n-type ZnO on the surface of flower-like MoS2 NPs through the seed-mediate route and post-annealing treatment. The effects for the dye removal and photocatalytic performances after ZnO coating are systematically investigated. The results demonstrated that the coating of ZnO nanoparticles has a positive promotion to the photodegrading properties while negative effect on the adsorption capacity of the MoS2/ZnO heterostructures. The related mechanisms on the relationship of adsorption capacity and photocatalysis are discussed in detail.
NASA Astrophysics Data System (ADS)
Driad, R.; Sah, R. E.; Schmidt, R.; Kirste, L.
2012-01-01
We present structural, stress, and electrical properties of plasma assisted e-beam evaporated hafnium dioxide (HfO2) layers on n-type InP substrates. These layers have subsequently been used for surface passivation of InGaAs/InP heterostructure bipolar transistors either alone or in combination with plasma enhanced chemical vapor deposited SiO2 layers. The use of stacked HfO2/SiO2 results in better interface quality with InGaAs/InP heterostructures, as illustrated by smaller leakage current and improved breakdown voltage. These improvements can be attributed to the reduced defect density and charge trapping at the dielectric-semiconductor interface. The deposition at room temperature makes these films suitable for sensitive devices.
Modulation-Doped SrTiO3/SrTi1-xZrxO3 Heterostructures
NASA Astrophysics Data System (ADS)
Kajdos, Adam Paul
Two-dimensional electron gases (2DEGs) in SrTiO3 have attracted considerable attention for exhibiting a variety of interesting physical phenomena, such as superconductivity and magnetism. So far, most of the literature has focused on interfaces between nonpolar SrTiO3 and polar perovskite oxides (e.g. LaAlO3 or rare-earth titanates), where high carrier density 2DEGs (˜3 x 1014 cm-2) are generated by polar discontinuity. Modulation doping is an alternative approach to generating a 2DEG that has been explored extensively in III-V semiconductors but has not heretofore been explored in complex oxides. This approach involves interfacing an undoped semiconductor with a doped semiconductor whose conduction band edge lies at a higher energy, which results in electrons diffusing into the undoped semiconductor transport channel, where scattering from ionized dopants is minimized. Realizing a high-mobility modulation-doped structure with a SrTiO3 transport channel therefore requires both the optimization of the transport channel by minimizing native defects as well as the development of a perovskite oxide which has a suitable band offset with SrTiO3 and can be electron-doped. The growth of high electron mobility SrTiO3 as a suitable transport channel material was previously demonstrated using the hybrid molecular beam epitaxy (MBE) approach, where Sr is delivered via a solid source and Ti is delivered using a metal-organic precursor, titanium (IV) tetra-isopropoxide (TTIP). Expanding on this, in-situ reflection high-energy electron diffraction (RHEED) is used to track the surface and resulting film cation stoichiometry of homoepitaxial SrTiO3 (001) thin films grown by hybrid MBE. It is shown that films with lattice parameters identical to bulk single-crystal substrates within the detection limit of high-resolution X-ray diffraction (XRD) measurements exhibit an evolution in surface reconstruction with increasing TTIP beam-equivalent pressure. The change in the observed surface reconstruction from (1x1) to (2x1) to c(4x4) is correlated with a change from mixed SrO/TiO2 to pure TiO2 surface termination. It is argued that optimal cation stoichiometry is achieved for growth conditions within the XRD-defined growth window that result in a c(4x4) surface lattice. The development of a doped perovskite oxide semiconductor with a suitable conduction band offset is then discussed as the next necessary step towards realizing modulation-doped heterostructures. The SrTixZr1-x O3 solid solution is investigated for this purpose, with a focus on optimizing cation stoichiometry to allow for controlled doping. In particular, the hybrid MBE growth of SrTixZr1-xO3 thin films is explored using a metal-organic precursor for Zr, zirconium tert-butoxide (ZTB). The successful generation of 2DEGs by modulation doping of SrTiO3 is then demonstrated in SrTiO3/La:SrTi0.95Zr0.05O 3 heterostructures, and the electronic structure is studied by Shubnikov-de Haas analysis using multiple-subband models.
Tailored Assembly of 2D Heterostructures beyond Graphene
2017-05-11
liquid crystal and catalyst application. Another important approach we have explored during this project is the solution phase assembly of two...graphene oxide, and its potential functionalities in liquid crystal and catalyst application. Another important approach we have explored during...exfoliation, liquid phase exfoliation, and chemical vapor deposition, and opened up new opportunities to graphene based platform for novel
The controlled growth of perovskite thin films: Opportunities, challenges, and synthesis
DOE Office of Scientific and Technical Information (OSTI.GOV)
Schlom, D.G.; Theis, C.D.; Hawley, M.E.
1997-10-01
The broad spectrum of electronic and optical properties exhibited by perovskites offers tremendous opportunities for microelectronic devices, especially when a combination of properties in a single device is desired. Molecular beam epitaxy (MBE) has achieved unparalleled control in the integration of semiconductors at the monolayer-level; its use for the integration of perovskites with similar nanoscale customization appears promising. Composition control and oxidation are often significant challenges to the growth of perovskites by MBE, but we show that these can be met through the use of purified ozone as an oxidant and real-time atomic absorption composition control. The opportunities, challenges, andmore » synthesis of oxide heterostructures by reactive MBE are described, with examples taken from the growth of oxide superconductors and oxide ferroelectrics.« less
Pöpsel, Christian; Becker, Jonathan; Jeon, Nari; Döblinger, Markus; Stettner, Thomas; Gottschalk, Yeanitza Trujillo; Loitsch, Bernhard; Matich, Sonja; Altzschner, Marcus; Holleitner, Alexander W; Finley, Jonathan J; Lauhon, Lincoln J; Koblmüller, Gregor
2018-06-13
Core-shell semiconductor nanowires (NW) with internal quantum heterostructures are amongst the most complex nanostructured materials to be explored for assessing the ultimate capabilities of diverse ultrahigh-resolution imaging techniques. To probe the structure and composition of these materials in their native environment with minimal damage and sample preparation calls for high-resolution electron or ion microscopy methods, which have not yet been tested on such classes of ultrasmall quantum nanostructures. Here, we demonstrate that scanning helium ion microscopy (SHeIM) provides a powerful and straightforward method to map quantum heterostructures embedded in complex III-V semiconductor NWs with unique material contrast at ∼1 nm resolution. By probing the cross sections of GaAs-Al(Ga)As core-shell NWs with coaxial GaAs quantum wells as well as short-period GaAs/AlAs superlattice (SL) structures in the shell, the Al-rich and Ga-rich layers are accurately discriminated by their image contrast in excellent agreement with correlated, yet destructive, scanning transmission electron microscopy and atom probe tomography analysis. Most interestingly, quantitative He-ion dose-dependent SHeIM analysis of the ternary AlGaAs shell layers and of compositionally nonuniform GaAs/AlAs SLs reveals distinct alloy composition fluctuations in the form of Al-rich clusters with size distributions between ∼1-10 nm. In the GaAs/AlAs SLs the alloy clustering vanishes with increasing SL-period (>5 nm-GaAs/4 nm-AlAs), providing insights into critical size dimensions for atomic intermixing effects in short-period SLs within a NW geometry. The straightforward SHeIM technique therefore provides unique benefits in imaging the tiniest nanoscale features in topography, structure and composition of a multitude of diverse complex semiconductor nanostructures.
Zhan, Wen-wen; Kuang, Qin; Zhou, Jian-zhang; Kong, Xiang-jian; Xie, Zhao-xiong; Zheng, Lan-sun
2013-02-06
Metal-organic frameworks (MOFs) and related material classes are attracting considerable attention for their applications in gas storage/separation as well as catalysis. In contrast, research concerning potential uses in electronic devices (such as sensors) is in its infancy, which might be due to a great challenge in the fabrication of MOFs and semiconductor composites with well-designed structures. In this paper, we proposed a simple self-template strategy to fabricate metal oxide semiconductor@MOF core-shell heterostructures, and successfully obtained freestanding ZnO@ZIF-8 nanorods as well as vertically standing arrays (including nanorod arrays and nanotube arrays). In this synthetic process, ZnO nanorods not only act as the template but also provide Zn(2+) ions for the formation of ZIF-8. In addition, we have demonstrated that solvent composition and reaction temperature are two crucial factors for successfully fabricating well-defined ZnO@ZIF-8 heterostructures. As we expect, the as-prepared ZnO@ZIF-8 nanorod arrays display distinct photoelectrochemical response to hole scavengers with different molecule sizes (e.g., H(2)O(2) and ascorbic acid) owing to the limitation of the aperture of the ZIF-8 shell. Excitingly, such ZnO@ZIF-8 nanorod arrays were successfully applied to the detection of H(2)O(2) in the presence of serous buffer solution. Therefore, it is reasonable to believe that the semiconductor@MOFs heterostructure potentially has promising applications in many electronic devices including sensors.
Jeon, Sanghun; Song, Ihun; Lee, Sungsik; Ryu, Byungki; Ahn, Seung-Eon; Lee, Eunha; Kim, Young; Nathan, Arokia; Robertson, John; Chung, U-In
2014-11-05
A technique for invisible image capture using a photosensor array based on transparent conducting oxide semiconductor thin-film transistors and transparent interconnection technologies is presented. A transparent conducting layer is employed for the sensor electrodes as well as interconnection in the array, providing about 80% transmittance at visible-light wavelengths. The phototransistor is a Hf-In-Zn-O/In-Zn-O heterostructure yielding a high quantum-efficiency in the visible range. © 2014 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.
Acauan, Luiz; Dias, Anna C; Pereira, Marcelo B; Horowitz, Flavio; Bergmann, Carlos P
2016-06-29
The chemical inertness of carbon nanotubes (CNT) requires some degree of "defect engineering" for controlled deposition of metal oxides through atomic layer deposition (ALD). The type, quantity, and distribution of such defects rules the deposition rate and defines the growth behavior. In this work, we employed ALD to grow titanium oxide (TiO2) on vertically aligned carbon nanotubes (VACNT). The effects of nitrogen doping and oxygen plasma pretreatment of the CNT on the morphology and total amount of TiO2 were systematically studied using transmission electron microscopy, Raman spectroscopy, and thermogravimetric analysis. The induced chemical changes for each functionalization route were identified by X-ray photoelectron and Raman spectroscopies. The TiO2 mass fraction deposited with the same number of cycles for the pristine CNT, nitrogen-doped CNT, and plasma-treated CNT were 8, 47, and 80%, respectively. We demonstrate that TiO2 nucleation is dependent mainly on surface incorporation of heteroatoms and their distribution rather than structural defects that govern the growth behavior. Therefore, selecting the best way to functionalize CNT will allow us to tailor TiO2 distribution and hence fabricate complex heterostructures.
NASA Astrophysics Data System (ADS)
Ryu, S.; Zhou, H.; Paudel, T. R.; Irwin, J.; Podkaminer, J. P.; Bark, C. W.; Lee, D.; Kim, T. H.; Fong, D. D.; Rzchowski, M. S.; Tsymbal, E. Y.; Eom, C. B.
2017-10-01
Microscopic understanding of the surface-controlled conductivity of the two dimensional electron gas at complex oxide interfaces is crucial for developing functional interfaces. We observe conductivity and structural modification using in-situ synchrotron surface x-ray diffraction as the surface of a model LaAlO3/SrTiO3 (001) heterostructure is changed by polar adsorbates. We find that polar adsorbate-induced interfacial metallicity reduces polar distortions in the LaAlO3 layer. First-principles density functional theory calculations show that surface dipoles introduced by polar adsorbates lead to additional charge transfer and the reduction of polar displacements in the LaAlO3 layer, consistent with the experimental observations. Our study supports that internal structural deformations controlling functionalities can be driven without the application of direct electrical or thermal bias and offers a route to tuning interfacial properties. These results also highlight the important role of in-situ x-ray scattering with atomic resolution in capturing and exploring structural distortions and charge density changes caused by external perturbations such as chemical adsorption, redox reaction, and generation and/or annihilation of surface defects.
Magnetism and electronic structure at the interface of a metal CaRuO3 and Mott insulator CaMnO3.
NASA Astrophysics Data System (ADS)
Boris, Alexander; Freeland, John; Kavich, Jerald; Lee, Ho Nyung; Yordanov, Petar; Khaliullin, Giniyat; Keimer, Bernhard; Chakhalian, Jak
2007-03-01
Recent advances in fabrication of ultra-thin complex oxide heterostructures have opened new opportunities to investigate possible novel quantum states at the correlated interfaces. With this aim we fabricated ultra-thin superlattices of CaMnO3(CMO)/CaRuO3(CRO) with the thickness of CRO layers from 1 to 12 unit cells by laser MBE. Electronic properties of CRO/CMO were investigated by soft x-ray spectroscopies at the L-edges of Mn and Ru. SQUID and optical reflectivity revealed a ferromagnetic thickness-independent transition at Tc 100K and CRO thickness-dependent negative magnetoresistance. This behavior is in marked contrast to the individual layers. At the interface we found a clear sign of net magnetic moment on Mn, which saturates only at magnetic field of 5T. Unlike CMO, similar measurements at the Ru L3-edge showed no detectable magnetism in the field up to 5T. Comparison with Ru references confirmed Ru(IV) oxidation state. These findings are in the sharp contrast with previously suggested models involving Ru(IV-V) valency exchange and thus reveal intricate nature of the interface between a metal and Mott insulator.
DOE Office of Scientific and Technical Information (OSTI.GOV)
Ryu, S.; Zhou, H.; Paudel, T. R.
Microscopic understanding of the surface-controlled conductivity of the two dimensional electron gas at complex oxide interfaces is crucial for developing functional interfaces. We observe conductivity and structural modification using in-situ synchrotron surface x-ray diffraction as the surface of a model LaAlO3/SrTiO3 (001) heterostructure is changed by polar adsorbates. We find that polar adsorbate-induced interfacial metallicity reduces polar distortions in the LaAlO3 layer. First-principles density functional theory calculations show that surface dipoles introduced by polar adsorbates lead to additional charge transfer and the reduction of polar displacements in the LaAlO3 layer, consistent with the experimental observations. Our study supports that internalmore » structural deformations controlling functionalities can be driven without the application of direct electrical or thermal bias and offers a route to tuning interfacial properties. These results also highlight the important role of in-situ x-ray scattering with atomic resolution in capturing and exploring structural distortions and charge density changes caused by external perturbations such as chemical adsorption, redox reaction, and generation and/or annihilation of surface defects.« less
NASA Astrophysics Data System (ADS)
Chen, Jian; Xu, Xiaochan; Li, Tao; Pandiselvi, Kannusamy; Wang, Jingyu
2016-11-01
Efficient metal-free visible photocatalysts with high stability are highly desired for sufficient utilization of solar energy. In this work, the popular carbon nitride (CN) photocatalyst is rationally modified by acid exfoliation of molecular grafted CN, achieving improved visible-light utilization and charge carriers mobility. Moreover, the modification process tuned the surface electrical property of CN, which enabled it to be readily coupled with the oppositely charged graphene oxide during the following photo-assisted electrostatic assembly. Detailed characterizations indicate the formation of well-contacted 2D/2D heterostructure with strong interfacial interaction between the modified CN nanosheets (CNX-NSs) and reduced graphene oxide (RGO). The optimized hybrid (with a RGO ratio of 20%) exhibits the best photocatalytic performance toward MB degradation, which is almost 12.5 and 7.0 times of CN under full spectrum and visible-light irradiation, respectively. In addition, the hybrid exhibits high stability after five successive cycles with no obvious change in efficiency. Unlike pure CNX-NSs, the dye decomposition mostly depends on the H2O2 generation by a two-electron process due to the electron reservoir property of RGO. Thus the enhancement in photocatalytic activity could be ascribed to the improved light utilization and increased charge transfer ability across the interface of CNX-NSs/RGO heterostructure.
NASA Astrophysics Data System (ADS)
Zhou, Jun; Yang, Ming; Feng, Yuan Ping; Rusydi, Andrivo
2017-11-01
Perovskite oxide interfaces have attracted tremendous research interest for their fundamental physics and promising all-oxide electronic applications. Here, based on first-principles calculations, we propose a surface La interstitial promoted interface insulator-metal transition in LaAl O3 /SrTi O3 (110). Compared with surface oxygen vacancies, which play a determining role on the insulator-metal transition of LaAl O3 /SrTi O3 (001) interfaces, we find that surface La interstitials can be more experimentally realistic and accessible for manipulation and more stable in an ambient atmospheric environment. Interestingly, these surface La interstitials also induce significant spin-splitting states with a Ti dy z/dx z character at a conducting LaAl O3 /SrTi O3 (110) interface. On the other hand, for insulating LaAl O3 /SrTi O3 (110) (<4 unit cells LaAl O3 thickness), a distortion between La (Al) and O atoms is found at the LaAl O3 side, partially compensating the polarization divergence. Our results reveal the origin of the metal-insulator transition in LaAl O3 /SrTi O3 (110) heterostructures, and also shed light on the manipulation of the superior properties of LaAl O3 /SrTi O3 (110) for different possibilities in electronic and magnetic applications.
Tuning the physical properties in strontium iridate heterostructures
NASA Astrophysics Data System (ADS)
Nichols, John; Meyer, Tricia; Lee, Ho Nyung
2015-03-01
Strontium iridate (Srn+1IrnO3n+1) has received lots of attention recently for its potential to reveal novel physical phenomena due to strong spin-orbital coupling with an interaction energy comparable to that of the on-site Coulomb interaction and crystal field splitting. The coexistence of fundamental interactions has created an exotic Jeff = 1/2 antiferromagnetic insulating ground state in Sr2IrO4. In particular, it is known that this system can be driven into a metallic state with the simultaneous increase in dimensionality (n) and strain. We have investigated the effects of electron confinement by interfacing strontium iridates with other perovskite oxides. We have synthesized thin film heterostructures, SrIrO3/AMO3 (A = Sr, La; B = Ti, Mn, Rh), layer-by-layer with pulsed laser deposition equipped with reflection high-energy electron diffraction. Based on investigations with x-ray diffraction, dc transport, SQUID magnetometry, and various spectroscopic measurements, we will present that the physical properties of the heterostructures are strongly dependent on spatial confinement and epitaxial strain. *This work was supported by the U. S. Department of Energy, Office of Science, Basic Energy Sciences, Materials Science and Engineering Division.
NASA Astrophysics Data System (ADS)
Nazirfakhr, Maryam; Shahhoseini, Ali
2018-03-01
By applying non-equilibrium Green's functions (NEGF) in combination with tight-binding (TB) model, we investigate and compare the electronic transport properties of H-terminated zigzag graphene nanoribbon (H/ZGNR) and O-terminated ZGNR/H-terminated ZGNR (O/ZGNR-H/ZGNR) heterostructure under finite bias. Moreover, the effect of width and symmetry on the electronic transport properties of both models is also considered. The results reveal that asymmetric H/ZGNRs have linear I-V characteristics in whole bias range, but symmetric H-ZGNRs show negative differential resistance (NDR) behavior which is inversely proportional to the width of the H/ZGNR. It is also shown that the I-V characteristic of O/ZGNR-H/ZGNR heterostructure shows a rectification effect, whether the geometrical structure is symmetric or asymmetric. The fewer the number of zigzag chains, the bigger the rectification ratio. It should be mentioned that, the rectification ratios of symmetric heterostructures are much bigger than asymmetric one. Transmission spectrum, density of states (DOS), molecular projected self-consistent Hamiltonian (MPSH) and molecular eigenstates are analyzed subsequently to understand the electronic transport properties of these ZGNR devices. Our findings could be used in developing nanoscale rectifiers and NDR devices.
Rouhi, Jalal; Mamat, Mohamad Hafiz; Ooi, C. H. Raymond; Mahmud, Shahrom; Mahmood, Mohamad Rusop
2015-01-01
High-density and well-aligned ZnO–ZnS core–shell nanocone arrays were synthesized on fluorine-doped tin oxide glass substrate using a facile and cost-effective two-step approach. In this synthetic process, the ZnO nanocones act as the template and provide Zn2+ ions for the ZnS shell formation. The photoluminescence spectrum indicates remarkably enhanced luminescence intensity and a small redshift in the UV region, which can be associated with the strain caused by the lattice mismatch between ZnO and ZnS. The obtained diffuse reflectance spectra show that the nanocone-based heterostructure reduces the light reflection in a broad spectral range and is much more effective than the bare ZnO nanocone and nanorod structures. Dye-sensitized solar cells based on the heterostructure ZnO–ZnS nanocones are assembled, and high conversion efficiency (η) of approximately 4.07% is obtained. The η improvement can be attributed primarily to the morphology effect of ZnO nanocones on light-trapping and effectively passivating the interface surface recombination sites of ZnO nanocones by coating with a ZnS shell layer. PMID:25875377
Tailoring Electronic Properties in Semiconducting Perovskite Materials through Octahedral Control
NASA Astrophysics Data System (ADS)
Choquette, Amber K.
Perovskite oxides, which take the chemical formula ABO 3, are a very versatile and interesting materials family, exhibiting properties that include ferroelectricity, ferromagnetism, mixed ionic/electronic conductivity, metal-insulator behavior and multiferroicity. Key to these functionalities is the network of BO6 corner-connected octahedra, which are known to distort and rotate, directly altering electronic and ferroic properties. By controlling the BO6 octahedral distortions and rotations through cationic substitutions, the use of strain engineering, or through the formation of superlattice structures, the functional properties of perovskites can be tuned. Motivating the use of structure-driven design in oxide heterostructures is the prediction of hybrid improper ferroelectricity in A'BO3/ABO3 superlattices. Two key design rules to realizing hybrid improper ferroelectricity are the growth of high quality superlattice structures with odd periodicities of the A / A' layers, and the control of the octahedral rotation pattern. My work explores the rotational response in perovskite oxides to strain and interface effects in thin films of RFeO3 ( R = La, Eu). I demonstrate a synchrotron x-ray diffraction technique to identify the rotation pattern that is present in the films. I then establish substrate imprinting as a key tool for controlling the rotation patterns in heterostructures, providing a means to realize the necessary structural variants of the predicted hybrid improper ferroelectricity in superlattices. In addition, by pairing measured diffraction data with a structure factor calculation, I demonstrate how one can extract both A-site and oxygen atomic positions in single crystal perovskite oxide films. Finally, I show results from (LaFeO 3)n/(EuFeO3)n superlattices (n = 1-5), synthesized to test the motivating predictions of hybrid improper ferroelectricity in oxide superlattices.
Yin, Ruiyang; Liu, Mingyang; Tang, Rui; Yin, Longwei
2017-09-02
In this work, we demonstrate a facile successive ionic layer adsorption and reaction process accompanied by hydrothermal method to synthesize CdS nanoparticle-modified α-Fe 2 O 3 /TiO 2 nanorod array for efficient photoelectrochemical (PEC) water oxidation. By integrating CdS/α-Fe 2 O 3 /TiO 2 ternary system, light absorption ability of the photoanode can be effectively improved with an obviously broadened optical-response to visible light region, greatly facilitates the separation of photogenerated carriers, giving rise to the enhancement of PEC water oxidation performance. Importantly, for the designed abnormal type-II heterostructure between Fe 2 O 3 /TiO 2 , the conduction band position of Fe 2 O 3 is higher than that of TiO 2 , the photogenerated electrons from Fe 2 O 3 will rapidly recombine with the photogenerated holes from TiO 2 , thus leads to an efficient separation of photogenerated electrons from Fe 2 O 3 /holes from TiO 2 at the Fe 2 O 3 /TiO 2 interface, greatly improving the separation efficiency of photogenerated holes within Fe 2 O 3 and enhances the photogenerated electron injection efficiency in TiO 2 . Working as the photoanodes of PEC water oxidation, CdS/α-Fe 2 O 3 /TiO 2 heterostucture electrode exhibits improved photocurrent density of 0.62 mA cm - 2 at 1.23 V vs. reversible hydrogen electrode (RHE) in alkaline electrolyte, with an obviously negatively shifted onset potential of 80 mV. This work provides promising methods to enhance the PEC water oxidation performance of the TiO 2 -based heterostructure photoanodes.
Towards Rational Design of Functional Fluoride and Oxyfluoride Materials from First Principles
NASA Astrophysics Data System (ADS)
Charles, Nenian
Complex transition metal compounds (TMCs) research has produced functional materials with a range of properties, including ferroelectricity, colossal magnetoresistance, nonlinear optical activity and high-temperature superconductivity. Conventional routes to tune properties in transition metal oxides, for example, have relied primarily on cation chemical substitution and interfacial effects in thin film heterostructures. In heteroanionic TMCs, exhibiting two chemically distinct anions coordinating the same or different cations, engineering of the anion sub-lattice for property control is a promising alternative approach. The presence of multiple anions provides additional design variables, such as anion order, that are absent in homoanionic counterparts. The more complex structural and chemical phase space of heteroanionic materials provides a unique opportunity to realize enhanced or unanticipated electronic, optical, and magnetic responses. Although there is growing interest in heteroanionic materials, and synthetic and characterization advances are occurring for these materials, the crystal-chemistry principles for realizing structural and property control are only slowing emerging. This dissertation employs anion engineering to investigate phenomena in transition metal fluorides and oxyfluorides compounds using first principles density functional theory calculations. Oxyfluorides are particularly intriguing owing their tendency to stabilize highly ordered anion sublattices as well as the potential to combine the advantageous properties of transition metal oxides and fluorides. This work 1) addresses the challenges of studying fluorides and oxyfluorides using first principles calculations; 2) evaluates the feasibility of using external stimuli, such as epitaxial strain and hydrostatic pressure, to control properties of fluorides and oxyfluorides; and 3) formulates a computational workflow based on multiple levels of theory and computation to elucidate structure-property relationships and anion-order descriptors. The insights gained in this work advance the understanding of oxide-fluoride anion engineered materials and we anticipate that it will motivate novel experimental efforts and materials by design in the future.
Magnetism in Complex Oxide Heterostructures Determined with Neutron Scattering
NASA Astrophysics Data System (ADS)
Te Velthuis, Suzanne G. E.
2009-03-01
With the creation of high quality superlattices consisting of complex oxide materials novel materials exhibiting a wide range of interesting phenomena are emerging. Due to the diverse physical properties of complex oxides, (e.g., ferromagnetism, antiferromagnetism, superconductivity), some of which can be varied by doping, the versatility in their applications is large. The physical properties in these new materials, often is tied to the behavior at the interfaces between the different components of the superlattice, and therefore requires detailed knowledge of the relationship between the chemical and electronic composition. Polarized neutron reflectometry (PNR) provides access to the depth-dependent magnitude and orientation of the magnetization and can therefore link the magnetic to the electronic and chemical properties, especially close to these interfaces. Several examples of our work will be presented, including that on La0.7Ca0.3MnO3/ YBa2Cu3O7-δ/ La0.7Ca0.3MnO3 trilayers which exhibit the inverse superconducting spin switch behavior, and where suppression of the magnetization close to the interface, as well as a varying anisotropy axis have been determined [1]. Another example is work on digitally layered analogs of La1-xSrxMnO3, where PNR reveals an asymmetric distribution of the magnetization across the two components (antiferromagnetic) LaMnO3and SrMnO3, which has been linked to structural properties at the interfaces [2]. [4pt] [1] V. Peña, Z. Sefrioui, D. Arias, C. Leon, J. Santamaria, J. L. Martinez, S. G. E. te Velthuis, A. Hoffmann, Phys. Rev. Lett. 94 (2005) 057002. [0pt] [2] S. J. May, A. B. Shah, S. G. E. te Velthuis, M. R. Fitzsimmons, J. M. Zuo, X. Zhai, J. N. Eckstein, S. D. Bader, and A. Bhattacharya, Phys. Rev. B 77 (2008) 174409.
Local switching of two-dimensional superconductivity using the ferroelectric field effect
NASA Astrophysics Data System (ADS)
Takahashi, K. S.; Gabay, M.; Jaccard, D.; Shibuya, K.; Ohnishi, T.; Lippmaa, M.; Triscone, J.-M.
2006-05-01
Correlated oxides display a variety of extraordinary physical properties including high-temperature superconductivity and colossal magnetoresistance. In these materials, strong electronic correlations often lead to competing ground states that are sensitive to many parameters-in particular the doping level-so that complex phase diagrams are observed. A flexible way to explore the role of doping is to tune the electron or hole concentration with electric fields, as is done in standard semiconductor field effect transistors. Here we demonstrate a model oxide system based on high-quality heterostructures in which the ferroelectric field effect approach can be studied. We use a single-crystal film of the perovskite superconductor Nb-doped SrTiO3 as the superconducting channel and ferroelectric Pb(Zr,Ti)O3 as the gate oxide. Atomic force microscopy is used to locally reverse the ferroelectric polarization, thus inducing large resistivity and carrier modulations, resulting in a clear shift in the superconducting critical temperature. Field-induced switching from the normal state to the (zero resistance) superconducting state was achieved at a well-defined temperature. This unique system could lead to a field of research in which devices are realized by locally defining in the same material superconducting and normal regions with `perfect' interfaces, the interface being purely electronic. Using this approach, one could potentially design one-dimensional superconducting wires, superconducting rings and junctions, superconducting quantum interference devices (SQUIDs) or arrays of pinning centres.
NASA Astrophysics Data System (ADS)
Molaei, Roya
The novel functionalities of Vanadium dioxide (VO2), such as, several orders of magnitude transition in resistivity and IR transmittance, provide the exciting opportunity for the development of next generation memory, sensor, and field-effect based devices. A critical issue in the development of practical devices based on metal oxides is the integration of high quality epitaxial oxide thin films with the existing silicon technology which is based on silicon (100) substrates. However, silicon is not suitable for epitaxial growth of oxides owing to its tendency to readily form an amorphous oxide layer or silicide at the film-substrate interface. The oxide films deposited directly on silicon exhibit poor crystallinity and are not suitable for device applications. To overcome this challenge, appropriate substrate templates must be developed for the growth of oxide thin films on silicon substrates. The primary objective of this dissertation was to develop an integration methodology of VO2 with Si (100) substrates so they could be used in "smart" sensor type of devices along with other multifunctional devices on the same silicon chip. This was achieved by using a NiO/c- YSZ template layer deposited in situ. It will be shown that if the deposition conditions are controlled properly. This approach was used to integrate VO 2 thin films with Si (100) substrates using pulsed laser deposition (PLD) technique. The deposition methodology of integrating VO2 thin films on silicon using various other template layers will also be discussed. Detailed epitaxial relationship of NiO/c-YSZ/Si(100) heterostructures as a template to growth of VO2 as well as were studied. We also were able to create a p-n junction within a single NiO epilayer through subsequent nanosecond laser annealing, as well as established a structure-property correlation in NiO/c-YSZ/Si(100) thin film epitaxial heterostructures with especial emphasis on the stoichiometry and crystallographic characteristics. NiO/c-YSZ/Si(100) heterostructures were used as template to grow fully relaxed VO2 thin films. The detailed x-ray diffraction, transmission electron microscopy (TEM), electrical characterization results for the deposited films will be presented. In the framework on domain matching epitaxy, epitaxial growth of VO2 (tetragonal crystal structure at growth temperature) on NiO has been explained. Our detailed phi-scan X-ray diffraction measurements corroborate our understanding of the epitaxial growth and in-plane atomic arrangements at the interface. It was observed that the transition characteristics (sharpness, over which electrical property changes are completed, amplitude, transition temperature, and hysteresis) are a strong function of microstructure, strain, and stoichiometry. We have shown that by the choosing the right template layer, strain in the VO2 thin films can be fully relaxed and near-bulk VO2 transition temperatures can be achieved. Finally, I will present my research work on modification of semiconductor-to-metal transition characteristics and effect on room temperature magnetic properties of VO2 thin films upon laser annealing. While the microstructure (epitaxy, crystalline quality etc.) and phase were preserved, we envisage these changes to occur as a result of introduction of oxygen vacancies upon laser treatment.
Carrier Localization in Confined Vanadate Superlattices
NASA Astrophysics Data System (ADS)
Eaton, Craig; Zhang, Lei; Engel-Herbert, Roman
2015-03-01
Perovskite oxide heterostructures have attracted attention due to the wealth of phenomena emerging at the interface, as well as the presence of strong electron correlations with potential applications as active electronic material for logic application utilizing the metal-to-insulator transition. Successful monolithic integration of perovskite oxides with Si makes them an ideal material choice. Here we present the growth of cubic SrTiO3/SrVO3/SrTiO3 heterostructures on (La0.3Sr0.7) (Al0.65Ta0.35) O3 substrates and orthorhombically distorted CaTiO3/CaVO3/CaTiO3 heterostructures on (LaSrAlTa4) O3 substrates by hybrid molecular beam epitaxy, where alkaline earth metals were supplied using conventional effusion cells and the transition metals from the metal-organic precursor titanium-isopropoxide and vanadium oxi-tri-isopropoxide. Here, the interfaces are non-polar and carrier confinement in the correlated vanadate metals (d1 configuration, 1 electron per unit cell) is achieved using insulating titanates as barrier material. Growth challenges associated with optimizing conditions for cation and oxygen stoichiometry are discussed. Confined structures down to 2 ML have been studied to demonstrate the potential for tuning incipient 2D Mott transition from 3D correlated metal. Room temperature hall measurements revealed carrier concentration in SrVO3 films are 2 × 1022 cm-3 in thick films and decreases to 8 × 1020 cm-3 at 3 ML confinement, revealing the onset of strong carrier localization. Direct comparison between SrVO3 and CaVO3 structures are presented to elucidate the role of dimensional confinement and structural distortion.
Alcaire, Maria; Sanchez-Valencia, Juan R; Aparicio, Francisco J; Saghi, Zineb; Gonzalez-Gonzalez, Juan C; Barranco, Angel; Zian, Youssef Oulad; Gonzalez-Elipe, Agustin R; Midgley, Paul; Espinos, Juan P; Groening, Pierangelo; Borras, Ana
2011-11-01
Hierarchical (branched) and hybrid metal-NPs/organic supported NWs are fabricated through controlled plasma processing of metalloporphyrin, metallophthalocyanine and perylene nanowires. The procedure is also applied for the development of a general template route for the synthesis of supported metal and metal oxide nanowires.
Nikam, Pratibha R; Baviskar, Prashant K; Majumder, Sutripto; Sali, Jaydeep V; Sankapal, Babasaheb R
2018-08-15
Controlled growth of different sizes of cadmium selenide (CdSe) nanoparticles over well aligned ZnO nanorods have been performed using successive ionic layer adsorption and reaction (SILAR) technique at room temperature (27 °C) in order to form nano heterostructure solar cells. Deposition of compact layer of zinc oxide (ZnO) by SILAR technique on fluorine doped tin oxide (FTO) coated glass substrate followed by growth of vertically aligned ZnO nanorods array using chemical bath deposition (CBD) at low temperature (<100 °C). Different characterization techniques viz. X-ray diffractometer, UV-Vis spectrophotometer, field emission scanning electron microscopy, transmission electron microscopy and X-ray photoelectron spectroscopy have been used to know the structural, optical, morphological and compositional properties of synthesized nano heterostructure. The photovoltaic performance of the cells with variation in SILAR cycles for CdSe and with use of different electrolytes have been recorded as J-V characteristics and the maximum conversion efficiency of 0.63% have been attained with ferro/ferri cyanide electrolyte for 12 cycles CdSe coating over 1-D ZnO nanorods. Copyright © 2018 Elsevier Inc. All rights reserved.
NASA Astrophysics Data System (ADS)
Lee, Ching-Sung; Hsu, Wei-Chou; Huang, Yi-Ping; Liu, Han-Yin; Yang, Wen-Luh; Yang, Shen-Tin
2018-06-01
Comparative study on a novel Al2O3-dielectric graded-barrier (GB) AlxGa1‑xN/AlN/GaN/Si (x = 0.22 ∼ 0.3) metal-oxide-semiconductor heterostructure field-effect transistor (MOS-HFET) formed by using the ultrasonic spray pyrolysis deposition (USPD) technique has been made with respect to a conventional-barrier (CB) Al0.26Ga0.74N/AlN/GaN/Si MOS-HFET and the reference Schottky-gate HFET devices. The GB AlxGa1‑xN was devised to improve the interfacial quality and enhance the Schottky barrier height at the same time. A cost-effective ultrasonic spray pyrolysis deposition (USPD) method was used to form the high-k Al2O3 gate dielectric and surface passivation on the AlGaN barrier of the present MOS-HFETs. Comprehensive device performances, including maximum extrinsic transconductance (g m,max), maximum drain-source current density (I DS,max), gate-voltage swing (GVS) linearity, breakdown voltages, subthreshold swing (SS), on/off current ratio (I on /I off ), high frequencies, and power performance are investigated.
Sistani, Masiar; Staudinger, Philipp; Greil, Johannes; Holzbauer, Martin; Detz, Hermann; Bertagnolli, Emmerich; Lugstein, Alois
2017-08-09
Conductance quantization at room temperature is a key requirement for the utilizing of ballistic transport for, e.g., high-performance, low-power dissipating transistors operating at the upper limit of "on"-state conductance or multivalued logic gates. So far, studying conductance quantization has been restricted to high-mobility materials at ultralow temperatures and requires sophisticated nanostructure formation techniques and precise lithography for contact formation. Utilizing a thermally induced exchange reaction between single-crystalline Ge nanowires and Al pads, we achieved monolithic Al-Ge-Al NW heterostructures with ultrasmall Ge segments contacted by self-aligned quasi one-dimensional crystalline Al leads. By integration in electrostatically modulated back-gated field-effect transistors, we demonstrate the first experimental observation of room temperature quantum ballistic transport in Ge, favorable for integration in complementary metal-oxide-semiconductor platform technology.
NASA Astrophysics Data System (ADS)
Ferragut, R.; Dupaquier, A.; Brivio, S.; Bertacco, R.; Egger, W.
2011-09-01
Defects in an ultrathin Au/La2/3Sr1/3MnO3/SrTiO3 (Au/LSMO/STO) heterostructure displaying electroresistive behavior were studied using variable energy positron annihilation spectroscopy. Vacancy-like defects were found to be the dominant positron traps in the LSMO and STO thin perovskite oxides with a number density >1017 cm-3 and 2 × 1017 cm-3 in the STO substrate. High defect density was revealed by strong positron trapping at the Au/LSMO interface. Oxygen deficiency in LSMO would be the main source of these traps. Besides, a low density of sub-nano voids of ˜6 Å was found in the substrate and in the thin LSMO/STO films.
Fabrication and characterization of AlN metal-insulator-semiconductor grown Si substrate
NASA Astrophysics Data System (ADS)
Mahyuddin, A.; Azrina, A.; Mohd Yusoff, M. Z.; Hassan, Z.
2017-11-01
An experimental investigation was conducted to explore the effect of inserting a single AlGaN interlayer between AlN epilayer and GaN/AlN heterostructures on Si (111) grown by molecular beam epitaxy (MBE). It is confirmed from the scanning electron microscopy (SEM) that the AlGaN interlayer has a remarkable effect on reducing the tensile stress and dislocation density in AlN top layer. Capacitance-voltage (C-V) measurements were conducted to study the electrical properties of AlN/GaN heterostructures. While deriving the findings through the calculation it is suggested that the AlGaN interlayer can significantly reduce the value of effective oxide charge density and total effective number of charges per unit area which are 1.37 × 10-6C/cm2 and 8.55 × 1012cm-2, respectively.
On stoichiometry and intermixing at the spinel/perovskite interface in CoFe2O4/BaTiO3 thin films.
Tileli, Vasiliki; Duchamp, Martial; Axelsson, Anna-Karin; Valant, Matjaz; Dunin-Borkowski, Rafal E; Alford, Neil McN
2015-01-07
The performance of complex oxide heterostructures depends primarily on the interfacial coupling of the two component structures. This interface character inherently varies with the synthesis method and conditions used since even small composition variations can alter the electronic, ferroelectric, or magnetic functional properties of the system. The focus of this article is placed on the interface character of a pulsed laser deposited CoFe2O4/BaTiO3 thin film. Using a range of state-of-the-art transmission electron microscopy methodologies, the roles of substrate morphology, interface stoichiometry, and cation intermixing are determined on the atomic level. The results reveal a surprisingly uneven BaTiO3 substrate surface formed after the film deposition and Fe atom incorporation in the top few monolayers inside the unit cell of the BaTiO3 crystal. Towards the CoFe2O4 side, a disordered region extending several nanometers from the interface was revealed and both Ba and Ti from the substrate were found to diffuse into the spinel layer. The analysis also shows that within this somehow incompatible composite interface, a different phase is formed corresponding to the compound Ba2Fe3Ti5O15, which belongs to the ilmenite crystal structure of FeTiO3 type. The results suggest a chemical activity between these two oxides, which could lead to the synthesis of complex engineered interfaces.
Madaan, Nitesh; Bao, Jie; Nandasiri, Manjula I.; ...
2015-08-31
The experimental atom probe tomography results from two different specimen orientations (top-down and side-ways) of a high oxygen ion conducting Samaria-doped-ceria/Scandia-stabilized-zirconia multilayer thin film solid oxide fuel cell electrolyte was correlated with level-set method based field evaporation simulations for the same specimen orientations. This experiment-theory correlation explains the dynamic specimen shape evolution and ion trajectory aberrations that can induce density artifacts in final reconstruction leading to inaccurate estimation of interfacial intermixing. This study highlights the need and importance of correlating experimental results with field evaporation simulations when using atom probe tomography for studying oxide heterostructure interfaces.
Xiao, Gang; Xu, Shengnan; Li, Peifeng; Su, Haijia
2018-08-03
Heterostructured photocatalysts based on g-C 3 N 4 and TiO 2 represent a promising kind of photocatalyst in environmental fields, but the synthesis methods are always complex and not green. In the present paper, a facile and green one-step calcination procedure at lower temperature (450 °C) with the assistance of water is developed to synthesize a visible-light-active TiO 2 @g-C 3 N 4 heterostructured photocatalyst, which shows higher visible-light-driven activity (k = 0.014 min -1 ) than pure g-C 3 N 4 (k = 0.0036 min -1 ) and TiO 2 (k = 0.0067 min -1 ) for methyl orange degradation. Excellent performance (over 90% conversion) was also observed for the removal of rhodamine B, phenol, and Cr(VI) under visible light. The heterostructured photocatalyst showed favorable reusability, preserving 86% of its activity after five successive cycles. A mechanism study demonstrates that the enhanced photocatalytic activity results from the efficient separation of the photo-generated charge carriers through the intimate interface between the two semiconductors based on their appropriate band structures and light-induced mechanism. The heterostructured photocatalyst will certainly find wide applications in the treatment of various toxic pollutants in wastewater using abundant solar energy. Furthermore, this facile and green procedure and the proposed synergistic mechanism will provide guidelines in designing other g-C 3 N 4 based organic-inorganic composite photocatalysts for various applications.
Challenges and opportunities of ZnO-related single crystalline heterostructures
DOE Office of Scientific and Technical Information (OSTI.GOV)
Kozuka, Y.; Tsukazaki, A.; PRESTO, Japan Science and Technology Agency
2014-03-15
Recent technological advancement in ZnO heterostructures has expanded the possibility of device functionalities to various kinds of applications. In order to extract novel device functionalities in the heterostructures, one needs to fabricate high quality films and interfaces with minimal impurities, defects, and disorder. With employing molecular-beam epitaxy and single crystal ZnO substrates, the density of residual impurities and defects can be drastically reduced and the optical and electrical properties have been dramatically improved for the ZnO films and heterostructures with Mg{sub x}Zn{sub 1-x}O. Here, we overview such recent technological advancement from various aspects of application. Towards optoelectronic devices such asmore » a light emitter and a photodetector in an ultraviolet region, the development of p-type ZnO and the fabrication of excellent Schottky contact, respectively, have been subjected to intensive studies for years. For the former, the fine tuning of the growth conditions to make Mg{sub x}Zn{sub 1-x}O as intrinsic as possible has opened the possibilities of making p-type Mg{sub x}Zn{sub 1-x}O through NH{sub 3} doping method. For the latter, conducting and transparent polymer films spin-coated on Mg{sub x}Zn{sub 1-x}O was shown to give almost ideal Schottky junctions. The wavelength-selective detection can be realized with varying the Mg content. From the viewpoint of electronic devices, two-dimensional electrons confined at the Mg{sub x}Zn{sub 1-x}O/ZnO interfaces are promising candidate for quantum devices because of high electron mobility and strong electron-electron correlation effect. These wonderful features and tremendous opportunities in ZnO-based heterostructures make this system unique and promising in oxide electronics and will lead to new quantum functionalities in optoelectronic devices and electronic applications with lower energy consumption and high performance.« less
DOE Office of Scientific and Technical Information (OSTI.GOV)
Bolkhovityanov, Yu. B., E-mail: bolkhov@isp.nsc.ru; Gutakovskii, A. K.; Deryabin, A. S.
2016-11-15
The Ge/Ge{sub x}Si{sub 1–x}/Si(001) (x = 0.2–0.6) heterostructures grown by the molecular epitaxy method are analyzed using high-resolution electron microscopy with atomic resolution. The thickness of the Ge{sub x}Si{sub 1–x} buffer layer is 7–35 nm. It is shown that such heterostructures relax in two stages: an ordered network of edge dislocations is formed during their growth (500°C) at the Ge/GeSi interface and then, contrary to the generally accepted opinion concerning their immobility, some of the edge dislocations move through the buffer GeSi layer to the GeSi/Si(001) interface during annealing at higher temperatures and x > 0.3. It is found thatmore » plastic relaxation of the GeSi buffer layer occurs due to motion of dislocation complexes of the edge type, consisting of a pair of complementary 60° dislocations with the ends of (111) extra planes located approximately at a distance from 2 to 12 interplanar spacings. It is shown that the penetration of dislocation complexes into the GeSi buffer layer and further to the GeSi/Si interface is intensified with increasing annealing temperature (600–800°C) and the fraction of Ge in the buffer layer.« less
Crystal S. Lewis; Wong, Stanislaus S.; Liu, Haiqing; ...
2016-01-04
We report on the synthesis and structural characterization of novel semiconducting heterostructures composed of cadmium selenide (CdSe) quantum dots (QDs) attached onto the surfaces of novel high-surface area, porous rare-earth-ion doped alkaline earth titanate micron-scale spherical motifs, i.e. both Eu-doped and Pr-doped CaTiO 3, composed of constituent, component nanoparticles. These unique metal oxide perovskite building blocks were created by a multi-pronged synthetic strategy involving molten salt and hydrothermal protocols. Subsequently, optical characterization of these heterostructures indicated a clear behavioral dependence of charge transfer in these systems upon a number of parameters such as the nature of the dopant, the reactionmore » temperature, and particle size. Specifically, 2.7 nm diameter ligand-functionalized CdSe QDs were anchored onto sub-micron sized CaTiO 3-based spherical assemblies, prepared by molten salt protocols. We found that both the Pr- and Eu-doped CaTiO 3 displayed pronounced PL emissions, with maximum intensities observed using optimized lanthanide concentrations of 0.2 mol% and 6 mol%, respectively. Analogous experiments were performed on Eu-doped BaTiO 3 and SrTiO 3 motifs, but CaTiO 3 still performed as the most effective host material amongst the three perovskite systems tested. Furthermore, the ligand-capped CdSe QD-doped CaTiO 3 heterostructures exhibited effective charge transfer between the two individual constituent nanoscale components, an assertion corroborated by the corresponding quenching of their measured PL signals.« less
DOE Office of Scientific and Technical Information (OSTI.GOV)
Liu, Xingbo
2016-11-14
New unique hetero-structured cathode has been developed in this project. La 2NiO 4+δ (LNO) as a surface catalyst with interstitial oxygen defects was introduced onto the state-of-the-art (La 0.6Sr 0.4) 0.95Co 0.2Fe 0.8O 3-δ (LSCF) cathode to enhance the surface-limited ORR kinetics on SOFC cathode. Furthermore, the hetero-structured cathode surface maintains high activity under electrode polarization with much less negative effects from surface cation segregation of Sr, which is known to cause degradation issues for conventional LSCF and LSC cathodes, thus improving the cathode long-term stability. The interface chemistry distribution and oxygen transport properties have been studied to prove themore » enhancement of power out and stability of LNO-infiltrated LSCF cathode. The further investigation demonstrates that CeO 2 & La 2-xNiO 4+δ (x=0-0.2) co-infiltration is a simple and cost-effective method to improve both performance and stability of LSCF cathode by limiting nano-particles growth/delamination and further improve the surface stability. For the first time, a physical model is proposed to illustrate how unique interstitial species on hetero-structured cathode surface work to regulate the exchange rate of the incorporation reaction. Meanwhile, fundamental investigation of the surface oxygen exchange and bulk oxygen transport properties under over-potential conditions across cathode materials have been carried out in this project, which were discussed and compared to the Nernst equation that is generally applied to treat any oxide electrodes under equilibrium.« less
Artificial Oxide Heterostructures with Tunable Band Gap
2016-12-20
PIs: Xiaoxing Xi 1, and Jon Spanier2 1. Department of Physics , Temple University, Philadelphia, PA 19122, USA 2. Department of Materials Science...been summarized in the following. Our thin-film experimental group under the leadership of Prof. Xiaoxing Xi at physics department of Temple...theoretical group of Xifan Wu at physics department of Temple University. The first- principles calculations were performed by using density functional theory
Oscillatory bistability of real-space transfer in semiconductor heterostructures
NASA Astrophysics Data System (ADS)
Do˙ttling, R.; Scho˙ll, E.
1992-01-01
Charge transport parallel to the layers of a modulation-doped GaAs/AlxGa1-xAs heterostructure is studied theoretically. The heating of electrons by the applied electric field leads to real-space transfer of electrons from the GaAs into the adjacent AlxGa1-xAs layer. For sufficiently large dc bias, spontaneous periodic 100-GHz current oscillations, and bistability and hysteretic switching transitions between oscillatory and stationary states are predicted. We present a detailed investigation of complex bifurcation scenarios as a function of the bias voltage U0 and the load resistance RL. For large RL subcritical Hopf bifurcations and global bifurcations of limit cycles are displayed.
Electronic properties and morphology of copper oxide/n-type silicon heterostructures
NASA Astrophysics Data System (ADS)
Lindberg, P. F.; Gorantla, S. M.; Gunnæs, A. E.; Svensson, B. G.; Monakhov, E. V.
2017-08-01
Silicon-based tandem heterojunction solar cells utilizing cuprous oxide (Cu2O) as the top absorber layer show promise for high-efficiency conversion and low production cost. In the present study, single phase Cu2O films have been realized on n-type Si substrates by reactive magnetron sputtering at 400 °C. The obtained Cu2O/Si heterostructures have subsequently been heat treated at temperatures in the 400-700 °C range in Ar flow and extensively characterized by x-ray diffraction (XRD) measurements, transmission electron microscopy (TEM) imaging and electrical techniques. The Cu2O/Si heterojunction exhibits a current rectification of ~5 orders of magnitude between forward and reverse bias voltages. High resolution cross-sectional TEM-images show the presence of a ~2 nm thick interfacial SiO2 layer between Cu2O and the Si substrate. Heat treatments below 550 °C result in gradual improvement of crystallinity, indicated by XRD. At and above 550 °C, partial phase transition to cupric oxide (CuO) occurs followed by a complete transition at 700 °C. No increase or decrease of the SiO2 layer is observed after the heat treatment at 550 °C. Finally, a thin Cu-silicide layer (Cu3Si) emerges below the SiO2 layer upon annealing at 550 °C. This silicide layer influences the lateral current and voltage distributions, as evidenced by an increasing effective area of the heterojunction diodes.
Controlled Synthesis and Utilization of Metal and Oxide Hybrid Nanoparticles
NASA Astrophysics Data System (ADS)
Crane, Cameron
This dissertation reports the development of synthetic methods concerning rationally-designed, hybrid, and multifunctional nanomaterials. These methods are based on a wet chemical, solution phase approach that utilizes the knowledge of synthetic organic and inorganic chemistry to generate building blocks in solution for the growth of nanocrystals and hybrid nanostructures. This work builds on the prior knowledge of shape-controlled synthesis of noble metal nanocrystals and expands into the challenging realm of the more reactive first row transition metals. Specifically, a microemulsion sol-gel method was developed to synthesize Au-SiO2 dimers as precursors for the synthesis of segmented heterostructures of noble metals that can be used for catalysis. This microemulsion sol-gel method was modified to synthesize an aqueous suspension of oxidation-resistant Cu-SiO2 core-shell nanoparticles that can be used for sensing and catalysis. A thermal decomposition approach was developed, wherein zero-valence metal precursor complexes in the presence of seed nanoparticles produced metal-metal oxide core-shell structures with well-controlled shell thickness. This method was demonstrated on AuCu 3-Fe3O4, AuCu3-NiO, and AuCu3 -MnO core-shell systems. Switching the core from AuCu3 alloy to pure Cu, this method could extend to Cu-Fe3O4 and Cu-MnO systems. Further etching the Cu core in these core-shell structures led to the formation of the hollow metal oxides which provides a versatile route to hollow nanostructures of metal oxides. This work develops the synthetic library of tools for the production of hybrid nanostructures with multiple functionalities.
High temperature interface superconductivity
Gozar, A.; Bozovic, I.
2016-01-20
High-T c superconductivity at interfaces has a history of more than a couple of decades. In this review we focus our attention on copper-oxide based heterostructures and multi-layers. We first discuss the technique, atomic layer-by-layer molecular beam epitaxy (ALL-MBE) engineering, that enabled High-T c Interface Superconductivity (HT-IS), and the challenges associated with the realization of high quality interfaces. Then we turn our attention to the experiments which shed light on the structure and properties of interfacial layers, allowing comparison to those of single-phase films and bulk crystals. Both ‘passive’ hetero-structures as well as surface-induced effects by external gating are discussed.more » Here, we conclude by comparing HT-IS in cuprates and in other classes of materials, especially Fe-based superconductors, and by examining the grand challenges currently laying ahead for the field.« less
Designing a Spin-one Mott Insulator: Complete Charge Transfer in Nickelate-Titanate Heterostructures
NASA Astrophysics Data System (ADS)
Chen, Hanghui; Marianetti, Chris; Millis, Andrew
2013-03-01
Ab initio calculations are performed to show that complete charge transfer may occur from the TiO2 to the NiO2 layers in (LaTiO3)1/(LaNiO3)1 superlattices. Although the two component materials are an S = 1 / 2 Mott insulator and a weakly correlated paramagnetic metal, strong correlation effects on Ni d states can render the superlattice an unusual S = 1 charge transfer insulator, with the Ti- d band empty, the Ni in the d8 state and the oxygen bands filled. The charge transfer gap is set by the Ti/Ni d level splitting. Magnetic, photoemission and x-ray scattering experiments are suggested to test the theory. The results show that heterostructuring can lead to very high levels of electron doping of oxides. This research was supported by the Army Research Office under ARO-Ph 56032 and DOE-ER-046169.
III-V heterostructure tunnel field-effect transistor.
Convertino, C; Zota, C B; Schmid, H; Ionescu, A M; Moselund, K E
2018-07-04
The tunnel field-effect transistor (TFET) is regarded as one of the most promising solid-state switches to overcome the power dissipation challenge in ultra-low power integrated circuits. TFETs take advantage of quantum mechanical tunneling hence exploit a different current control mechanism compared to standard MOSFETs. In this review, we describe state-of-the-art development of TFET both in terms of performances and of materials integration and we identify the main remaining technological challenges such as heterojunction defects and oxide/channel interface traps causing trap-assisted-tunneling (TAT). Mesa-structures, planar as well as vertical geometries are examined. Conductance slope analysis on InAs/GaSb nanowire tunnel diodes are reported, these two-terminal measurements can be relevant to investigate the tunneling behavior. A special focus is dedicated to III-V heterostructure TFET, as different groups have recently shown encouraging results achieving the predicted sub-thermionic low-voltage operation.
Emerging Robust Heterostructure of MoS2-rGO for High-Performance Supercapacitors.
Saraf, Mohit; Natarajan, Kaushik; Mobin, Shaikh M
2018-05-16
The intermittent nature of renewable energy resources has led to a continuous mismatch between energy demand and supply. A possible solution to overcome this persistent problem is to design appropriate energy-storage materials. Supercapacitors based on different nanoelectrode materials have emerged as one of the promising storage devices. In this work, we investigate the supercapacitor properties of a molybdenum disulfide-reduced graphene oxide (rGO) heterostructure-based binder-free electrode, which delivered a high specific capacitance (387.6 F g -1 at 1.2 A g -1 ) and impressive cycling stability (virtually no loss up to 1000 cycles). In addition, the possible role of rGO in the composite toward synergistically enhanced supercapacitance has been highlighted. Moreover, an attempt has been made to correlate the electrochemical impedance spectroscopy studies with the voltammetric analyses. The performance exceeds that of the reported state-of-the-art structures.
III–V heterostructure tunnel field-effect transistor
NASA Astrophysics Data System (ADS)
Convertino, C.; Zota, C. B.; Schmid, H.; Ionescu, A. M.; Moselund, K. E.
2018-07-01
The tunnel field-effect transistor (TFET) is regarded as one of the most promising solid-state switches to overcome the power dissipation challenge in ultra-low power integrated circuits. TFETs take advantage of quantum mechanical tunneling hence exploit a different current control mechanism compared to standard MOSFETs. In this review, we describe state-of-the-art development of TFET both in terms of performances and of materials integration and we identify the main remaining technological challenges such as heterojunction defects and oxide/channel interface traps causing trap-assisted-tunneling (TAT). Mesa-structures, planar as well as vertical geometries are examined. Conductance slope analysis on InAs/GaSb nanowire tunnel diodes are reported, these two-terminal measurements can be relevant to investigate the tunneling behavior. A special focus is dedicated to III–V heterostructure TFET, as different groups have recently shown encouraging results achieving the predicted sub-thermionic low-voltage operation.
Growth of heterostructures on InAs for high mobility device applications
NASA Astrophysics Data System (ADS)
Contreras-Guerrero, R.; Wang, S.; Edirisooriya, M.; Priyantha, W.; Rojas-Ramirez, J. S.; Bhuwalka, K.; Doornbos, G.; Holland, M.; Oxland, R.; Vellianitis, G.; Van Dal, M.; Duriez, B.; Passlack, M.; Diaz, C. H.; Droopad, R.
2013-09-01
The growth of heterostructures lattice matched to InAs(100) substrates for high mobility electronic devices has been investigated. The oxide removal process and homoepitaxial nucleation depends on the deposition parameters to avoid the formation of surface defects that can propagate through the structure during growth which can result in degraded device performance. The growth parameters for InAs homoepitaxy were found to be within an extremely narrow range when using As4 with a slight increase using As2. High structural quality lattice matched AlAsxSb1-x buffer layer was grown on InAs(100) substrates using a digital growth technique with the AlAs mole fraction adjusted by varying the incident As flux. Using the AlAsxSb1-x buffer layer, the transport properties of thin InAs channel layers were determined on conducting native substrates.
NASA Astrophysics Data System (ADS)
Wu, Kongping; Liao, Meiyong; Sang, Liwen; Liu, Jiangwei; Imura, Masataka; Ye, Haitao; Koide, Yasuo
2018-04-01
Tailoring the electronic states of the dielectric oxide/diamond interface is critical to the development of next generation semiconductor devices like high-power high-frequency field-effect transistors. In this work, we investigate the electronic states of the TiO2/diamond 2 × 1-(100) interface by using first principles total energy calculations. Based on the calculation of the chemical potentials for the TiO2/diamond interface, it is observed that the hetero-interfaces with the C-OTi configuration or with two O vacancies are the most energetically favorable structures under the O-rich condition and under Ti-rich condition, respectively. The band structure and density of states of both TiO2/diamond and TiO2/H-diamond hetero-structures are calculated. It is revealed that there are considerable interface states at the interface of the anatase TiO2/diamond hetero-structure. By introducing H on the diamond surface, the interface states are significantly suppressed. A type-II alignment band structure is disclosed at the interface of the TiO2/diamond hetero-structure. The valence band offset increases from 0.6 to 1.7 eV when H is introduced at the TiO2/diamond interface.
NASA Astrophysics Data System (ADS)
Pan, Dan-Feng; Bi, Gui-Feng; Chen, Guang-Yi; Zhang, Hao; Liu, Jun-Ming; Wang, Guang-Hou; Wan, Jian-Guo
2016-03-01
Recently, ferroelectric perovskite oxides have drawn much attention due to potential applications in the field of solar energy conversion. However, the power conversion efficiency of ferroelectric photovoltaic effect currently reported is far below the expectable value. One of the crucial problems lies in the two back-to-back Schottky barriers, which are formed at the ferroelectric-electrode interfaces and blocking most of photo-generated carriers to reach the outside circuit. Herein, we develop a new approach to enhance the ferroelectric photovoltaic effect by introducing the polarization-dependent interfacial coupling effect. Through inserting a semiconductor ZnO layer with spontaneous polarization into the ferroelectric ITO/PZT/Au film, a p-n junction with strong polarization-dependent interfacial coupling effect is formed. The power conversion efficiency of the heterostructure is improved by nearly two orders of magnitude and the polarization modulation ratio is increased about four times. It is demonstrated that the polarization-dependent interfacial coupling effect can give rise to a great change in band structure of the heterostructure, not only producing an aligned internal electric field but also tuning both depletion layer width and potential barrier height at PZT-ZnO interface. This work provides an efficient way in developing highly efficient ferroelectric-based solar cells and novel optoelectronic memory devices.
Pan, Dan-Feng; Bi, Gui-Feng; Chen, Guang-Yi; Zhang, Hao; Liu, Jun-Ming; Wang, Guang-Hou; Wan, Jian-Guo
2016-03-08
Recently, ferroelectric perovskite oxides have drawn much attention due to potential applications in the field of solar energy conversion. However, the power conversion efficiency of ferroelectric photovoltaic effect currently reported is far below the expectable value. One of the crucial problems lies in the two back-to-back Schottky barriers, which are formed at the ferroelectric-electrode interfaces and blocking most of photo-generated carriers to reach the outside circuit. Herein, we develop a new approach to enhance the ferroelectric photovoltaic effect by introducing the polarization-dependent interfacial coupling effect. Through inserting a semiconductor ZnO layer with spontaneous polarization into the ferroelectric ITO/PZT/Au film, a p-n junction with strong polarization-dependent interfacial coupling effect is formed. The power conversion efficiency of the heterostructure is improved by nearly two orders of magnitude and the polarization modulation ratio is increased about four times. It is demonstrated that the polarization-dependent interfacial coupling effect can give rise to a great change in band structure of the heterostructure, not only producing an aligned internal electric field but also tuning both depletion layer width and potential barrier height at PZT-ZnO interface. This work provides an efficient way in developing highly efficient ferroelectric-based solar cells and novel optoelectronic memory devices.
Pan, Dan-Feng; Bi, Gui-Feng; Chen, Guang-Yi; Zhang, Hao; Liu, Jun-Ming; Wang, Guang-Hou; Wan, Jian-Guo
2016-01-01
Recently, ferroelectric perovskite oxides have drawn much attention due to potential applications in the field of solar energy conversion. However, the power conversion efficiency of ferroelectric photovoltaic effect currently reported is far below the expectable value. One of the crucial problems lies in the two back-to-back Schottky barriers, which are formed at the ferroelectric-electrode interfaces and blocking most of photo-generated carriers to reach the outside circuit. Herein, we develop a new approach to enhance the ferroelectric photovoltaic effect by introducing the polarization-dependent interfacial coupling effect. Through inserting a semiconductor ZnO layer with spontaneous polarization into the ferroelectric ITO/PZT/Au film, a p-n junction with strong polarization-dependent interfacial coupling effect is formed. The power conversion efficiency of the heterostructure is improved by nearly two orders of magnitude and the polarization modulation ratio is increased about four times. It is demonstrated that the polarization-dependent interfacial coupling effect can give rise to a great change in band structure of the heterostructure, not only producing an aligned internal electric field but also tuning both depletion layer width and potential barrier height at PZT-ZnO interface. This work provides an efficient way in developing highly efficient ferroelectric-based solar cells and novel optoelectronic memory devices. PMID:26954833
NASA Astrophysics Data System (ADS)
Gurram, M.; Omar, S.; van Wees, B. J.
2018-07-01
The current research in graphene spintronics strives for achieving a long spin lifetime, and efficient spin injection and detection in graphene. In this article, we review how hexagonal boron nitride (hBN) has evolved as a crucial substrate, as an encapsulation layer, and as a tunnel barrier for manipulation and control of spin lifetimes and spin injection/detection polarizations in graphene spin valve devices. First, we give an overview of the challenges due to conventional SiO2/Si substrate for spin transport in graphene followed by the progress made in hBN based graphene heterostructures. Then we discuss in detail the shortcomings and developments in using conventional oxide tunnel barriers for spin injection into graphene followed by introducing the recent advancements in using the crystalline single/bi/tri-layer hBN tunnel barriers for an improved spin injection and detection which also can facilitate two-terminal spin valve and Hanle measurements at room temperature, and are of technological importance. A special case of bias induced spin polarization of contacts with exfoliated and chemical vapour deposition (CVD) grown hBN tunnel barriers is also discussed. Further, we give our perspectives on utilizing graphene-hBN heterostructures for future developments in graphene spintronics.
Electrical properties of thermoelectric cobalt Ca3Co4O9 epitaxial heterostructures
NASA Astrophysics Data System (ADS)
Guo, Haizhong; Wang, Shufang; Wang, Le; Jin, Kui-juan; Chen, Shanshan; Fu, Guangsheng; Ge, Chen; Lu, Huibin; Wang, Can; He, Meng; Yang, Guozhen
2013-03-01
Heterostructures fabricated from layered cobalt oxides offer substantial advantages for thermoelectric applications. C-axis-oriented Ca3Co4O9 (CCO) thin films on SrTiO3 substrates and Ca3Co4O9/SrTi0.993Nb0.007O3 p-n heterojunctions were fabricated by pulsed laser deposition. The measurements of in-plane resistivity, thermopower, and magnetic properties performed on the Ca3Co4O9 thin films were found to be comparable to ab-plane those of the single crystals due to good orientation of the films. The temperature dependence of the electrical transport properties of Ca3Co4O9/SrTi0.993Nb0.007O3 p-n heterojunction was also investigated. The junction shows two distinctive transport mechanisms at different temperature regimes under forward bias: tunneling across the Schottky barrier in the temperature range of 100-380 K, and tunneling mechanism at low bias and thermal emission mechanism at high bias between 10 and 100 K. However, for the case of low reverse bias, the trap assisted tunneling process should be considered for the leakage current. Negative magnetoresistance effect is observed at low temperatures, related to the electron spin-dependent scattering and the interface resistance of the heterostructures.
Bano, Amreen; Gaur, N K
2018-01-15
A variety of theoretical and experimental works have reported several potential applications of MoS 2 monolayer based heterostructures (HSs) such as light emitting diodes, photodetectors and field effect transistors etc. In the present work, we have theoretically performed as a model case study, MoS 2 monolayer deposited over insulating SrTiO 3 (001) to study the band alignment at TiO 2 termination. The interfacial characteristics are found to be highly dependent on the interface termination. With an insulating oxide material, a significant band gap (0.85eV) is found in MoS 2 /TiO 2 interface heterostructure (HS). A unique electronic band profile with an indirect band gap (0.67eV) is observed in MoS 2 monolayer when confined in a cubic environment of SrTiO 3 (STO). Adsorption analysis showed the chemisorption of MoS 2 on the surface of STO substrate with TiO 2 termination which is justified by the charge density calculations that shows the existence of covalent bonding at the interface. The fabrication of HS of such materials paves the path for developing the unprecedented 2D materials with exciting properties such as semiconducting devices, thermoelectric and optoelectronic applications.
NASA Astrophysics Data System (ADS)
Chen, Yi; Tse, Wai Hei; Chen, Longyan; Zhang, Jin
2015-03-01
Heteronanostructured zinc oxide nanorod (ZnO NR) array are vertically grown on polydimethylsiloxane (PDMS) through a hydrothermal method followed by an in situ deposition of silver nanoparticles (Ag NPs) through a photoreduction process. The Ag-ZnO heterostructured nanorods on PDMS are measured with an average diameter of 160 nm and an average length of 2 μm. ZnO NRs measured by high-resolution transmission electron microscope (HRTEM) shows highly crystalline with a lattice fringe of 0.255 nm, which corresponds to the (0002) planes in ZnO crystal lattice. The average diameter of the Ag NPs in situ deposited on the ZnO NRs is estimated at 22 ± 2 nm. As compared to the bare ZnO NRs, the heterostructured Ag-ZnO nanorod array shows enhanced ultraviolet (UV) absorption at 440 nm, and significant emission in the visible region (λem = 542 nm). In addition, the antimicrobial efficiency of Ag-ZnO heterostructured nanorod array shows obvious improvement as compared to bare ZnO nanorod array. The cytotoxicity of ZnO nanorod array with and without Ag NPs was studied by using 3 T3 mouse fibroblast cell line. No significant toxic effect is imposed on the cells.
Chen, Yi; Tse, Wai Hei; Chen, Longyan; Zhang, Jin
2015-01-01
Heteronanostructured zinc oxide nanorod (ZnO NR) array are vertically grown on polydimethylsiloxane (PDMS) through a hydrothermal method followed by an in situ deposition of silver nanoparticles (Ag NPs) through a photoreduction process. The Ag-ZnO heterostructured nanorods on PDMS are measured with an average diameter of 160 nm and an average length of 2 μm. ZnO NRs measured by high-resolution transmission electron microscope (HRTEM) shows highly crystalline with a lattice fringe of 0.255 nm, which corresponds to the (0002) planes in ZnO crystal lattice. The average diameter of the Ag NPs in situ deposited on the ZnO NRs is estimated at 22 ± 2 nm. As compared to the bare ZnO NRs, the heterostructured Ag-ZnO nanorod array shows enhanced ultraviolet (UV) absorption at 440 nm, and significant emission in the visible region (λem = 542 nm). In addition, the antimicrobial efficiency of Ag-ZnO heterostructured nanorod array shows obvious improvement as compared to bare ZnO nanorod array. The cytotoxicity of ZnO nanorod array with and without Ag NPs was studied by using 3 T3 mouse fibroblast cell line. No significant toxic effect is imposed on the cells.
Co3O4-x-Carbon@Fe2-yCoyO3 Heterostructural Hollow Polyhedrons for the Oxygen Evolution Reaction.
Xu, Wangwang; Xie, Weiwei; Wang, Ying
2017-08-30
Hollow heterostructured nanomaterials have received tremendous interest in new-generation electrocatalyst applications. However, the design and fabrication of such materials remain a significant challenge. In this work, we present Co 3 O 4-x -carbon@Fe 2-y Co y O 3 heterostructural hollow polyhedrons that have been fabricated by facile thermal treatment followed by solution-phase growth for application as efficient oxygen evolution reaction (OER) electrocatalysts. Starting from a single ZIF-67 hollow polyhedron, a novel complex structured composite material constructed from Co 3 O 4-x nanocrystallite-embedded carbon matrix embedded with Fe 2-y Co y O 3 nanowires was successfully prepared. The Co 3 O 4-x nanocrystallite with oxygen vacancies provides both heterogeneous nucleation sites and growth platform for Fe 2-y Co y O 3 nanowires. The resultant heterostructure combines the advantages of Fe 2-y Co y O 3 nanowires with the large surface area and surface defects of Co 3 O 4-x nanocrystallite, resulting in improved electrocatalytic activity and electrical conductivity. As a result, such novel heterostructured OER electrocatalysts exhibit much lower onset potential (1.52 V) and higher current density (70 mA/cm 2 at 1.7 V) than Co 3 O 4-x -carbon hollow polyhedrons (onset 1.55 V, 35 mA/cm 2 at 1.7 V) and pure Co 3 O 4 hollow polyhedrons (onset 1.62 V, 5 mA/cm 2 at 1.7 V). Furthermore, the design and synthesis of metal-organic framework (MOF)-derived nanomaterials in this work offer new opportunities for developing novel and efficient electrocatalysts in electrochemical devices.
DOE Office of Scientific and Technical Information (OSTI.GOV)
Thompson, J.; Nichols, John A.; Lee, Shinbuhm
Metal electrodes are a universal element of all electronic devices. Conducting SrRuO 3 (SRO) epitaxial thin films have been extensively used as electrodes in complex-oxide heterostructures due to good lattice mismatches with perovskite substrates. However, when compared to SRO single crystals, SRO thin films have shown reduced conductivity and Curie temperatures (T C), which can lead to higher Joule heating and energy loss in the devices. In this paper, we report that high-quality SRO thin films can be synthesized by controlling the plume dynamics and growth rate of pulsed laser epitaxy (PLE) with real-time optical spectroscopic monitoring. The SRO thinmore » films grown under the kinetically controlled conditions, down to ca. 16 nm in thickness, exhibit both enhanced conductivity and T C as compared to bulk values, due to their improved stoichiometry and a strain-mediated increase of the bandwidth of Ru 4d electrons. Finally, this result provides a direction for enhancing the physical properties of PLE-grown thin films and paves a way to improved device applications.« less
In vivo degeneration and the fate of inorganic nanoparticles.
Feliu, Neus; Docter, Dominic; Heine, Markus; Del Pino, Pablo; Ashraf, Sumaira; Kolosnjaj-Tabi, Jelena; Macchiarini, Paolo; Nielsen, Peter; Alloyeau, Damien; Gazeau, Florence; Stauber, Roland H; Parak, Wolfgang J
2016-05-03
What happens to inorganic nanoparticles (NPs), such as plasmonic gold or silver, superparamagnetic iron oxide, or fluorescent quantum dot NPs after they have been administrated to a living being? This review discusses the integrity, biodistribution, and fate of NPs after in vivo administration. The hybrid nature of the NPs is described, conceptually divided into the inorganic core, the engineered surface coating comprising of the ligand shell and optionally also bio-conjugates, and the corona of adsorbed biological molecules. Empirical evidence shows that all of these three compounds may degrade individually in vivo and can drastically modify the life cycle and biodistribution of the whole heterostructure. Thus, the NPs may be decomposed into different parts, whose biodistribution and fate would need to be analyzed individually. Multiple labeling and quantification strategies for such a purpose will be discussed. All reviewed data indicate that NPs in vivo should no longer be considered as homogeneous entities, but should be seen as inorganic/organic/biological nano-hybrids with complex and intricately linked distribution and degradation pathways.
DOE Office of Scientific and Technical Information (OSTI.GOV)
Middey, Srimanta; Chakhalian, J.; Mahadevan, P.
The electronic structure of transition metal oxides featuring correlated electrons can be rationalized within the Zaanen-Sawatzky-Allen framework. Following a brief description of the present paradigms of electronic behavior, we focus on the physics of rare-earth nickelates as an archetype of complexity emerging within the charge transfer regime. The intriguing prospect of realizing the physics of high- Tc cuprates through heterostructuring resulted in a massive endeavor to epitaxially stabilize these materials in ultrathin form. A plethora of new phenomena unfolded in such artificial structures due to the effect of epitaxial strain, quantum confinement, and interfacial charge transfer. Here we review themore » present status of artificial rare-earth nickelates in an effort to uncover the interconnection between the electronic and magnetic behavior and the underlying crystal structure. Here, we conclude by discussing future directions to disentangle the puzzle regarding the origin of the metal-insulator transition, the role of oxygen holes, and the true nature of the antiferromagnetic spin configuration in the ultrathin limit.« less
Sketched oxide single-electron transistor
NASA Astrophysics Data System (ADS)
Cheng, Guanglei; Siles, Pablo F.; Bi, Feng; Cen, Cheng; Bogorin, Daniela F.; Bark, Chung Wung; Folkman, Chad M.; Park, Jae-Wan; Eom, Chang-Beom; Medeiros-Ribeiro, Gilberto; Levy, Jeremy
2011-06-01
Devices that confine and process single electrons represent an important scaling limit of electronics. Such devices have been realized in a variety of materials and exhibit remarkable electronic, optical and spintronic properties. Here, we use an atomic force microscope tip to reversibly `sketch' single-electron transistors by controlling a metal-insulator transition at the interface of two oxides. In these devices, single electrons tunnel resonantly between source and drain electrodes through a conducting oxide island with a diameter of ~1.5 nm. We demonstrate control over the number of electrons on the island using bottom- and side-gate electrodes, and observe hysteresis in electron occupation that is attributed to ferroelectricity within the oxide heterostructure. These single-electron devices may find use as ultradense non-volatile memories, nanoscale hybrid piezoelectric and charge sensors, as well as building blocks in quantum information processing and simulation platforms.
Marquardt, Oliver; Krause, Thilo; Kaganer, Vladimir; Martín-Sánchez, Javier; Hanke, Michael; Brandt, Oliver
2017-05-26
We present a systematic theoretical study of the influence of elastic strain relaxation on the built-in electrostatic potentials and the electronic properties of axial [Formula: see text] nanowire (NW) heterostructures. Our simulations reveal that for a sufficiently large ratio between the thickness of the [Formula: see text] disk and the diameter of the NW, the elastic relaxation leads to a significant reduction of the built-in electrostatic potential in comparison to a planar system of similar layer thickness and In content. In this case, the ground state transition energies approach constant values with increasing thickness of the disk and only depend on the In content, a behavior usually associated to that of a quantum well free of built-in electrostatic potentials. We show that the structures under consideration are by no means field-free, and the built-in potentials continue to play an important role even for ultrathin NWs. In particular, strain and the resulting polarization potentials induce complex confinement features of electrons and holes, which depend on the In content, shape, and dimensions of the heterostructure.
NASA Astrophysics Data System (ADS)
Anderson, T. J.; Zhou, H.; Xie, L.; Podkaminer, J. P.; Patzner, J. J.; Ryu, S.; Pan, X. Q.; Eom, C. B.
2017-09-01
The precise control of interfacial atomic arrangement in ABO3 perovskite heterostructures is paramount, particularly in cases where the subsequent electronic properties of the material exhibit geometrical preferences along polar crystallographic directions that feature inevitably complex surface reconstructions. Here, we present the B-site interfacial structure in polar (111) and non-polar (001) SrIrO3/SrTiO3 interfaces. The heterostructures were examined using scanning transmission electron microscopy and synchrotron-based coherent Bragg rod analysis. Our results reveal the preference of B-site intermixing across the (111) interface due to the polarity-compensated SrTiO3 substrate surface prior to growth. By comparison, the intermixing at the non-polar (001) interface is negligible. This finding suggests that the intermixing may be necessary to mitigate epitaxy along heavily reconstructed and non-stoichiometric (111) perovskite surfaces. Furthermore, this preferential B-site configuration could allow the geometric design of the interfacial perovskite structure and chemistry to selectively engineer the correlated electronic states of the B-site d-orbital.
3D Localized Trions in Monolayer WSe2 in a Charge Tunable van der Waals Heterostructure.
Chakraborty, Chitraleema; Qiu, Liangyu; Konthasinghe, Kumarasiri; Mukherjee, Arunabh; Dhara, Sajal; Vamivakas, Nick
2018-05-09
Monolayer transition metal dichalcogenides (TMDCs) have recently emerged as a host material for localized optically active quantum emitters that generate single photons. (1-5) Here, we investigate fully localized excitons and trions from such TMDC quantum emitters embedded in a van der Waals heterostructure. We use direct electrostatic doping through the vertical heterostructure device assembly to generate quantum confined trions. Distinct spectral jumps as a function of applied voltage bias, and excitation power-dependent charging, demonstrate the observation of the two different excitonic complexes. We also observe a reduction of the intervalley electron-hole exchange interaction in the confined trion due to the addition of an extra electron, which is manifested by a decrease in its fine structure splitting. We further confirm this decrease of exchange interaction for the case of the charged states by a comparative study of the circular polarization resolved photoluminescence from individual excitonic states. The valley polarization selection rules inherited by the localized trions will provide a pathway toward realizing a localized spin-valley-photon interface.
NASA Astrophysics Data System (ADS)
Liu, Jiatong; Sun, Cuifeng; Fu, Ming; Long, Jie; He, Dawei; Wang, Yongsheng
2018-02-01
The development of porous materials exhibiting photon regulation abilities for improved photoelectrochemical catalysis performance is always one of the important goals of solar energy harvesting. In this study, methods to improve the photocatalytic activity of TiO2 inverse opals were discussed. TiO2 inverse opals were prepared by atomic layer deposition (ALD) using colloidal crystal templates. In addition, TiO2 inverse opal heterostructures were fabricated using colloidal heterocrystals by repeated vertical deposition using different colloidal spheres. The hydrothermal method and ALD were used to prepare ZnO- or Fe2O3-modified TiO2 inverse opals on the internal surfaces of the TiO2 porous structures. Although the photonic reflection band was not significantly varied by oxide modification, the presence of Fe2O3 in the TiO2 inverse opals enhanced their visible absorption. The conformally modified oxides on the TiO2 inverse opals could also form energy barriers and avoid the recombination of electrons and holes. The fabrication of the TiO2 photonic crystal heterostructures and modification with ZnO or Fe2O3 can enhance the photocatalytic activity of TiO2 inverse opals.
Engineering magnetism at functional oxides interfaces: manganites and beyond
NASA Astrophysics Data System (ADS)
Yi, Di; Lu, Nianpeng; Chen, Xuegang; Shen, Shengchun; Yu, Pu
2017-11-01
The family of transition metal oxides (TMOs) is a large class of magnetic materials that has been intensively studied due to the rich physics involved as well as the promising potential applications in next generation electronic devices. In TMOs, the spin, charge, orbital and lattice are strongly coupled, and significant advances have been achieved to engineer the magnetism by different routes that manipulate these degrees of freedom. The family of manganites is a model system of strongly correlated magnetic TMOs. In this review, using manganites thin films and the heterostructures in conjunction with other TMOs as model systems, we review the recent progress of engineering magnetism in TMOs. We first discuss the role of the lattice that includes the epitaxial strain and the interface structural coupling. Then we look into the role of charge, focusing on the interface charge modulation. Having demonstrated the static effects, we continue to review the research on dynamical control of magnetism by electric field. Next, we review recent advances in heterostructures comprised of high T c cuprate superconductors and manganites. Following that, we discuss the emergent magnetic phenomena at interfaces between 3d TMOs and 5d TMOs with strong spin-orbit coupling. Finally, we provide our outlook for prospective future directions.
Fabrication and Characterization of N-Type Zinc Oxide/P-Type Boron Doped Diamond Heterojunction
NASA Astrophysics Data System (ADS)
Marton, Marián; Mikolášek, Miroslav; Bruncko, Jaroslav; Novotný, Ivan; Ižák, Tibor; Vojs, Marian; Kozak, Halyna; Varga, Marián; Artemenko, Anna; Kromka, Alexander
2015-09-01
Diamond and ZnO are very promising wide-bandgap materials for electronic, photovoltaic and sensor applications because of their excellent electrical, optical, physical and electrochemical properties and biocompatibility. In this contribution we show that the combination of these two materials opens up the potential for fabrication of bipolar heterojunctions. Semiconducting boron doped diamond (BDD) thin films were grown on Si and UV grade silica glass substrates by HFCVD method with various boron concentration in the gas mixture. Doped zinc oxide (ZnO:Al, ZnO:Ge) thin layers were deposited by diode sputtering and pulsed lased deposition as the second semiconducting layer on the diamond films. The amount of dopants within the films was varied to obtain optimal semiconducting properties to form a bipolar p-n junction. Finally, different ZnO/BDD heterostructures were prepared and analyzed. Raman spectroscopy, SEM, Hall constant and I-V measurements were used to investigate the quality, structural and electrical properties of deposited heterostructures, respectively. I-V measurements of ZnO/BDD diodes show a rectifying ratio of 55 at ±4 V. We found that only very low dopant concentrations for both semiconducting materials enabled us to fabricate a functional p-n junction. Obtained results are promising for fabrication of optically transparent ZnO/BDD bipolar heterojunction.
DOE Office of Scientific and Technical Information (OSTI.GOV)
Oh, Pilgun; Oh, Seung -Min; Li, Wangda
The Ni-rich layered oxides with a Ni content of >0.5 are drawing much attention recently to increase the energy density of lithium-ion batteries. However, the Ni-rich layered oxides suffer from aggressive reaction of the cathode surface with the organic electrolyte at the higher operating voltages, resulting in consequent impedance rise and capacity fade. To overcome this difficulty, we present here a heterostructure composed of a Ni-rich LiNi 0.7Co 0.15Mn 0.15O 2 core and a Li-rich Li 1.2-xNi 0.2Mn 0.6O 2 shell, incorporating the advantageous features of the structural stability of the core and chemical stability of the shell. With amore » unique chemical treatment for the activation of the Li 2MnO 3 phase of the shell, a high capacity is realized with the Li-rich shell material. Aberration-corrected scanning transmission electron microscopy (STEM) provides direct evidence for the formation of surface Li-rich shell layer. Finally, the heterostructure exhibits a high capacity retention of 98% and a discharge- voltage retention of 97% during 100 cycles with a discharge capacity of 190 mA h g -1 (at 2.0–4.5 V under C/3 rate, 1C = 200 mA g -1).« less
Probing the bulk ionic conductivity by thin film hetero-epitaxial engineering
NASA Astrophysics Data System (ADS)
Pergolesi, Daniele; Roddatis, Vladimir; Fabbri, Emiliana; Schneider, Christof W.; Lippert, Thomas; Traversa, Enrico; Kilner, John A.
2015-02-01
Highly textured thin films with small grain boundary regions can be used as model systems to directly measure the bulk conductivity of oxygen ion conducting oxides. Ionic conducting thin films and epitaxial heterostructures are also widely used to probe the effect of strain on the oxygen ion migration in oxide materials. For the purpose of these investigations a good lattice matching between the film and the substrate is required to promote the ordered film growth. Moreover, the substrate should be a good electrical insulator at high temperature to allow a reliable electrical characterization of the deposited film. Here we report the fabrication of an epitaxial heterostructure made with a double buffer layer of BaZrO3 and SrTiO3 grown on MgO substrates that fulfills both requirements. Based on such template platform, highly ordered (001) epitaxially oriented thin films of 15% Sm-doped CeO2 and 8 mol% Y2O3 stabilized ZrO2 are grown. Bulk conductivities as well as activation energies are measured for both materials, confirming the success of the approach. The reported insulating template platform promises potential application also for the electrical characterization of other novel electrolyte materials that still need a thorough understanding of their ionic conductivity.
NASA Astrophysics Data System (ADS)
Ni, Qing-Qing; Zhu, Yao-Feng; Yu, Lu-Jun; Fu, Ya-Qin
2015-04-01
Multiple-phase nanocomposites filled with carbon nanotubes (CNTs) have been developed for their significant potential in microwave attenuation. The introduction of other phases onto the CNTs to achieve CNT-based heterostructures has been proposed to obtain absorbing materials with enhanced microwave absorption properties and broadband frequency due to their different loss mechanisms. The existence of polyaniline (PANI) as a coating with controllable electrical conductivity can lead to well-matched impedance. In this work, a one-dimensional CNT@BaTiO3@PANI heterostructure composite was fabricated. The fabrication processes involved coating of an acid-modified CNT with BaTiO3 (CNT@BaTiO3) through a sol-gel technique followed by combustion and the formation of CNT@BaTiO3@PANI nanohybrids by in situ polymerization of an aniline monomer in the presence of CNT@BaTiO3, using ammonium persulfate as an oxidant and HCl as a dopant. The as-synthesized CNT@BaTiO3@PANI composites with heterostructures were confirmed by various morphological and structural characterization techniques, as well as conductivity and microwave absorption properties. The measured electromagnetic parameters showed that the CNT@BaTiO3@PANI composites exhibited excellent microwave absorption properties. The minimum reflection loss of the CNT@BaTiO3@PANI composites with 20 wt % loadings in paraffin wax reached -28.9 dB (approximately 99.87% absorption) at 10.7 GHz with a thickness of 3 mm, and a frequency bandwidth less than -20 dB was achieved from 10 to 15 GHz. This work demonstrated that the CNT@BaTiO3@PANI heterostructure composite can be potentially useful in electromagnetic stealth materials, sensors, and electronic devices.
NASA Astrophysics Data System (ADS)
Cai, Li; Jiang, Hui; Wang, Luxi
2017-10-01
Ag3PO4 photocatalysts modified with BiPO4 and polypyrrole (PPy) were successfully synthesized via a combination of co-precipitation hydrothermal technique and oxidative polymerization method. Their morphologies, structures and optical and electronic properties were characterized by means of scanning electron microscopy (SEM), energy-dispersive X-ray spectroscopy (EDS), transmission electron microscope (TEM), Brunauer-Emmett-Teller (BET) surface areas, X-ray diffraction (XRD), fourier transform infrared spectra (FT-IR), X-ray photo-electron spectroscopy (XPS), UV-vis diffuse reflection spectra (UV-vis DRS), photocurrent technique and electrochemical impedance spectra (EIS). The typical triphenylmethane dye (malachite green) was chosen as a target organic contaminants to estimate the photocatalytic activities and photo-stabilities of Ag3PO4-BiPO4-PPy heterostructures under visible light irradiation. The results indicated that the existence of BiPO4 and PPy not only showed great influences on the photocatalytic activity, but also significantly enhanced photo-stability of Ag3PO4 in repeated and long-term applications. The degradation conversion of Ag3PO4-BiPO4-PPy heterostructures (ABP-3) was 1.58 times of that of pure Ag3PO4. The photo-corrosion phenomenon of Ag3PO4 was effectively avoided. The photocatalytic activity of up to 87% in the Ag3PO4-BiPO4-PPy heterostructures (ABP-3) can be remained after five repeated cycles, while only about 33% of the degradation efficiency can be reserved in pure Ag3PO4. The possible mechanism of enhanced photo-stability and photocatalytic activity of Ag3PO4-BiPO4-PPy heterostructures was also discussed in this work.
Ni, Qing-Qing; Zhu, Yao-Feng; Yu, Lu-Jun; Fu, Ya-Qin
2015-01-01
Multiple-phase nanocomposites filled with carbon nanotubes (CNTs) have been developed for their significant potential in microwave attenuation. The introduction of other phases onto the CNTs to achieve CNT-based heterostructures has been proposed to obtain absorbing materials with enhanced microwave absorption properties and broadband frequency due to their different loss mechanisms. The existence of polyaniline (PANI) as a coating with controllable electrical conductivity can lead to well-matched impedance. In this work, a one-dimensional CNT@BaTiO3@PANI heterostructure composite was fabricated. The fabrication processes involved coating of an acid-modified CNT with BaTiO3 (CNT@BaTiO3) through a sol-gel technique followed by combustion and the formation of CNT@BaTiO3@PANI nanohybrids by in situ polymerization of an aniline monomer in the presence of CNT@BaTiO3, using ammonium persulfate as an oxidant and HCl as a dopant. The as-synthesized CNT@BaTiO3@PANI composites with heterostructures were confirmed by various morphological and structural characterization techniques, as well as conductivity and microwave absorption properties. The measured electromagnetic parameters showed that the CNT@BaTiO3@PANI composites exhibited excellent microwave absorption properties. The minimum reflection loss of the CNT@BaTiO3@PANI composites with 20 wt % loadings in paraffin wax reached -28.9 dB (approximately 99.87% absorption) at 10.7 GHz with a thickness of 3 mm, and a frequency bandwidth less than -20 dB was achieved from 10 to 15 GHz. This work demonstrated that the CNT@BaTiO3@PANI heterostructure composite can be potentially useful in electromagnetic stealth materials, sensors, and electronic devices.
NASA Astrophysics Data System (ADS)
Singh, Kirandeep; Kaur, Davinder
2017-02-01
The manipulation of magnetic states and materials' spin degree-of-freedom via a control of an electric (E-) field has been recently pursued to develop magnetoelectric (ME) coupling-driven electronic data storage devices with high read/write endurance, fast dynamic response, and low energy dissipation. One major hurdle for this approach is to develop reliable materials which should be compatible with prevailing silicon (Si)-based complementary metal-oxide-semiconductor (CMOS) technology, simultaneously allowing small voltage for the tuning of magnetization switching. In this regard, multiferroic heterostructures where ferromagnetic (FM) and ferroelectric (FE) layers are alternatively grown on conventional Si substrates are promising as the piezoelectric control of magnetization switching is anticipated to be possible by an E-field. In this work, we study the ferromagnetic shape memory alloys based PbZr0.52Ti0.48O3/Ni50Mn35In15 (PZT/Ni-Mn-In) multiferroic heterostructures, and investigate their potential for CMOS compatible non-volatile magnetic data storage applications. We demonstrate the voltage-impulse controlled nonvolatile, reversible, and bistable magnetization switching at room temperature in Si-integrated PZT/Ni-Mn-In thin film multiferroic heterostructures. We also thoroughly unveil the various intriguing features in these materials, such as E-field tuned ME coupling and magnetocaloric effect, shape memory induced ferroelectric modulation, improved fatigue endurance as well as Refrigeration Capacity (RC). This comprehensive study suggests that these novel materials have a great potential for the development of unconventional nanoscale memory and refrigeration devices with self-cooling effect and enhanced refrigeration efficiency, thus providing a new venue for their applications.
NASA Astrophysics Data System (ADS)
Turkulets, Yury; Shalish, Ilan
2018-01-01
Modern bandgap engineered electronic devices are typically made of multi-semiconductor multi-layer heterostructures that pose a major challenge to silicon-era characterization methods. As a result, contemporary bandgap engineering relies mostly on simulated band structures that are hardly ever verified experimentally. Here, we present a method that experimentally evaluates bandgap, band offsets, and electric fields, in complex multi-semiconductor layered structures, and it does so simultaneously in all the layers. The method uses a modest optical photocurrent spectroscopy setup at ambient conditions. The results are analyzed using a simple model for electro-absorption. As an example, we apply the method to a typical GaN high electron mobility transistor structure. Measurements under various external electric fields allow us to experimentally construct band diagrams, not only at equilibrium but also under any other working conditions of the device. The electric fields are then used to obtain the charge carrier density and mobility in the quantum well as a function of the gate voltage over the entire range of operating conditions of the device. The principles exemplified here may serve as guidelines for the development of methods for simultaneous characterization of all the layers in complex, multi-semiconductor structures.
NASA Astrophysics Data System (ADS)
Jo, Jung-Ho; Kim, Min-Seok; Han, Chang-Yeol; Jang, Eun-Pyo; Do, Young Rag; Yang, Heesun
2018-01-01
Fluorescent efficiency of various visible quantum dots (QDs) has been incessantly improved to meet industrially high standard mainly through the advance in core/shell heterostructural design, however, their stability against degradable environments appears still lacking. The most viable strategy to cope with this issue was to exploit chemically inert oxide phases to passivate QD surface in the form of either individual overcoating or matrix embedding. Herein, we report a simple but effective means to passivate QD surface by complexing its organic ligands with a metal alkoxide of titanium isopropoxide (Ti(i-PrO)4). For this, highly efficient red-emitting InP QDs with a multi-shell structure of ZnSeS intermediate plus ZnS outer shell are first synthesized and then the surface of resulting InP/ZnSeS/ZnS QDs is in-situ decorated with Ti(i-PrO)4. The presence of Tisbnd O species from Ti(i-PrO)4 on QD surface is verified by x-ray photoelectron and Fourier transform infrared spectroscopic analyses. Two comparative dispersions of pristine versus Ti(i-PrO)4-complexed QDs are exposed for certain periods of time to UV photon and heat and their temporal changes in photoluminescence are monitored, resulting in a huge improvement in QD stability from the latter ones through Ti(i-PrO)4-mediated better surface passivation.
Veal, B. W.; Eastman, J. A.
2017-03-01
Thin film In 2O 3/YSZ heterostructures exhibit significant increases in electrical conductance with time when small in-plane electric fields are applied. Contact resistances between the current electrodes and film, and between current electrodes and substrate are responsible for the behavior. With an in-plane electric field, different field profiles are established in the two materials, with the result that oxygen ions can be driven across the heterointerface, altering the doping of the n-type In 2O 3. Furthermore, a low frequency inductive feature observed in AC impedance spectroscopy measurements under DC bias conditions was found to be due to frequency-dependent changes inmore » the contact resistance.« less
Yao, Xin; Guo, Guilue; Ma, Xing; Zhao, Yang; Ang, Chung Yen; Luo, Zhong; Nguyen, Kim Truc; Li, Pei-Zhou; Yan, Qingyu; Zhao, Yanli
2015-12-02
Three-dimensional (3D) graphene aerogel (GA) has emerged as an outstanding support for metal oxides to enhance the overall energy-storage performance of the resulting hybrid materials. In the current stage of the studies, metals/metal oxides inside GA are in uncrafted geometries. Introducing structure-controlled metal oxides into GA may further push electrochemical properties of metal oxide-GA hybrids. Using rutile SnO2 as an example, we demonstrated here a facile hydrothermal strategy combined with a preconditioning technique named vacuum-assisted impregnation for in situ construction of controlled anisotropic SnO2 heterostructures inside GA. The obtained hybrid material was fully characterized in detail, and its formation mechanism was investigated by monitoring the phase-transformation process. Rational integration of the two advanced structures, anisotropic SnO2 and 3D GA, synergistically led to enhanced lithium-storage properties (1176 mAh/g for the first cycle and 872 mAh/g for the 50th cycle at 100 mA/g) as compared with its two counterparts, namely, rough nanoparticles@3D GA and anisotropic SnO2@2D graphene sheets (618 and 751 mAh/g for the 50th cycle at 100 mA/g, respectively). It was also well-demonstrated that this hybrid material was capable of delivering high specific capacity at rapid charge/discharge cycles (1044 mAh/g at 100 mA/g, 847 mAh/g at 200 mA/g, 698 mAh/g at 500 mA/g, and 584 mAh/g at 1000 mA/g). The in situ integration strategy along with vacuum-assisted impregnation technique presented here shows great potential as a versatile tool for accessing a variety of sophisticated smart structures in the form of anisotropic metals/metal oxides within 3D GA toward useful applications.
Ultra-thin solid oxide fuel cells: Materials and devices
NASA Astrophysics Data System (ADS)
Kerman, Kian
Solid oxide fuel cells are electrochemical energy conversion devices utilizing solid electrolytes transporting O2- that typically operate in the 800 -- 1000 °C temperature range due to the large activation barrier for ionic transport. Reducing electrolyte thickness or increasing ionic conductivity can enable lower temperature operation for both stationary and portable applications. This thesis is focused on the fabrication of free standing ultrathin (<100 nm) oxide membranes of prototypical O 2- conducting electrolytes, namely Y2O3-doped ZrO2 and Gd2O3-doped CeO2. Fabrication of such membranes requires an understanding of thin plate mechanics coupled with controllable thin film deposition processes. Integration of free standing membranes into proof-of-concept fuel cell devices necessitates ideal electrode assemblies as well as creative processing schemes to experimentally test devices in a high temperature dual environment chamber. We present a simple elastic model to determine stable buckling configurations for free standing oxide membranes. This guides the experimental methodology for Y 2O3-doped ZrO2 film processing, which enables tunable internal stress in the films. Using these criteria, we fabricate robust Y2O3-doped ZrO2 membranes on Si and composite polymeric substrates by semiconductor and micro-machining processes, respectively. Fuel cell devices integrating these membranes with metallic electrodes are demonstrated to operate in the 300 -- 500 °C range, exhibiting record performance at such temperatures. A model combining physical transport of electronic carriers in an insulating film and electrochemical aspects of transport is developed to determine the limits of performance enhancement expected via electrolyte thickness reduction. Free standing oxide heterostructures, i.e. electrolyte membrane and oxide electrodes, are demonstrated. Lastly, using Y2O3-doped ZrO2 and Gd2O 3-doped CeO2, novel electrolyte fabrication schemes are explored to develop oxide alloys and nanoscale compositionally graded membranes that are thermomechanically robust and provide added interfacial functionality. The work in this thesis advances experimental state-of-the-art with respect to solid oxide fuel cell operation temperature, provides fundamental boundaries expected for ultrathin electrolytes, develops the ability to integrate highly dissimilar material (such as oxide-polymer) heterostructures, and introduces nanoscale compositionally graded electrolyte membranes that can lead to monolithic materials having multiple functionalities.
Ligand-induced dependence of charge transfer in nanotube–quantum dot heterostructures
Wang, Lei; Han, Jinkyu; Sundahl, Bryan; ...
2016-07-01
As a model system to probe ligand-dependent charge transfer in complex composite heterostructures, we fabricated double-walled carbon nanotube (DWNT) – CdSe quantum dot (QD) composites. Whereas the average diameter of the QDs probed was kept fixed at ~4.1 nm and the nanotubes analyzed were similarly oxidatively processed, by contrast, the ligands used to mediate the covalent attachment between the QDs and DWNTs were systematically varied to include p-phenylenediamine (PPD), 2-aminoethanethiol (AET), and 4-aminothiophenol (ATP). Herein, we have put forth a unique compilation of complementary data from experiment and theory, including results from transmission electron microscopy (TEM), near-edge X-ray absorption finemore » structure (NEXAFS) spectroscopy, Raman spectroscopy, electrical transport measurements, and theoretical modeling studies, in order to fundamentally assess the nature of the charge transfer between CdSe QDs and DWNTs, as a function of the structure of various, intervening bridging ligand molecules. Specifically, we correlated evidence of charge transfer as manifested by changes and shifts associated with NEXAFS intensities, Raman peak positions, and threshold voltages both before and after CdSe QD deposition onto the underlying DWNT surface. Importantly, for the first time ever in these types of nanoscale composite systems, we have sought to use theoretical modeling to justify and account for our experimental results. Finally, our overall data suggest that (i) QD coverage density on the DWNTs varies, based upon the different ligand pendant groups used and that (ii) the presence of a π-conjugated carbon framework within the ligands themselves and the electron affinity of the pendant groups collectively play important roles in the resulting charge transfer from QDs to the underlying CNTs.« less
DOE-EPSCoR Final Report Period: September 1, 2008- August 31, 2016
DOE Office of Scientific and Technical Information (OSTI.GOV)
Katiyar, Ram; Gomez, M.; Morell, G.
In this project, multifunctional nanostructured spintronic and magnetoelectric materials were investigated by experimental and computational efforts for applications in energy efficient electronic systems that integrate functionalities and thus have the potential to enable a new generation of faster responding devices and increased integration densities. The team systematically investigated transition metal (TM)-doped ZnO nanostructures, silicide nanorods, magnetoelectric oxides, and ferroelectric/ferromagnetic heterostructures. In what follows, we report the progress made by researchers during the above period in developing and understanding of 1) Spintronics nanostructures; 2) Resistive switching phenomenon in oxides for memory devices; 3) Magnetoelectric multiferroics; 4) Novel high-k gate oxides formore » logic devices; 5) Two dimensional (2D) materials; and 6) Theoretical studies in the above fields.« less
Coaxial metal-oxide-semiconductor (MOS) Au/Ga2O3/GaN nanowires.
Hsieh, Chin-Hua; Chang, Mu-Tung; Chien, Yu-Jen; Chou, Li-Jen; Chen, Lih-Juann; Chen, Chii-Dong
2008-10-01
Coaxial metal-oxide-semiconductor (MOS) Au-Ga2O3-GaN heterostructure nanowires were successfully fabricated by an in situ two-step process. The Au-Ga2O3 core-shell nanowires were first synthesized by the reaction of Ga powder, a mediated Au thin layer, and a SiO2 substrate at 800 degrees C. Subsequently, these core-shell nanowires were nitridized in ambient ammonia to form a GaN coating layer at 600 degrees C. The GaN shell is a single crystal, an atomic flat interface between the oxide and semiconductor that ensures that the high quality of the MOS device is achieved. These novel 1D nitride-based MOS nanowires may have promise as building blocks to the future nitride-based vertical nanodevices.
Nanowires, nanostructures and devices fabricated therefrom
Majumdar, Arun; Shakouri, Ali; Sands, Timothy D.; Yang, Peidong; Mao, Samuel S.; Russo, Richard E.; Feick, Henning; Weber, Eicke R.; Kind, Hannes; Huang, Michael; Yan, Haoquan; Wu, Yiying; Fan, Rong
2005-04-19
One-dimensional nanostructures having uniform diameters of less than approximately 200 nm. These inventive nanostructures, which we refer to as "nanowires", include single-crystalline homostructures as well as heterostructures of at least two single-crystalline materials having different chemical compositions. Because single-crystalline materials are used to form the heterostructure, the resultant heterostructure will be single-crystalline as well. The nanowire heterostructures are generally based on a semiconducting wire wherein the doping and composition are controlled in either the longitudinal or radial directions, or in both directions, to yield a wire that comprises different materials. Examples of resulting nanowire heterostructures include a longitudinal heterostructure nanowire (LOHN) and a coaxial heterostructure nanowire (COHN).
Zhu, Yinlong; Zhou, Wei; Ran, Ran; Chen, Yubo; Shao, Zongping; Liu, Meilin
2016-01-13
Solid oxide fuel cells (SOFCs) have potential to be the cleanest and most efficient electrochemical energy conversion devices with excellent fuel flexibility. To make SOFC systems more durable and economically competitive, however, the operation temperature must be significantly reduced, which depends sensitively on the development of highly active electrocatalysts for oxygen reduction reaction (ORR) at low temperatures. Here we report a novel silver nanoparticle-decorated perovskite oxide, prepared via a facile exsolution process from a Sr0.95Ag0.05Nb0.1Co0.9O3-δ (SANC) perovskite precursor, as a highly active and robust ORR electrocatalyst for low-temperature SOFCs. The exsolved Sr0.95Ag0.05Nb0.1Co0.9O3-δ (denoted as e-SANC) electrode is very active for ORR, achieving a very low area specific resistance (∼0.214 Ω cm(2) at 500 °C). An anode-supported cell with the new heterostructured cathode demonstrates very high peak power density (1116 mW cm(-2) at 500 °C) and stable operation for 140 h at a current density of 625 mA cm(-2). The superior ORR activity and stability are attributed to the fast oxygen surface exchange kinetics and the firm adhesion of the Ag nanoparticles to the Sr0.95Nb0.1Co0.9O3-δ (SNC0.95) support. Moreover, the e-SANC cathode displays improved tolerance to CO2. These unique features make the new heterostructured material a highly promising cathode for low-temperature SOFCs.
Qian, Min; Pan, Yiming; Liu, Fengyuan; Wang, Miao; Shen, Haoliang; He, Daowei; Wang, Baigeng; Shi, Yi; Miao, Feng; Wang, Xinran
2014-05-28
Memristive devices based on vertical heterostructures of graphene and TiOx show a significant power reduction that is up to ∼10(3) times smaller than that of conventional structures. This power reduction arises as a result of a tunneling barrier at the interface. The barrier is tunable, opening up the possibility of engineering several key memory characteristics. © 2014 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.
Sketched Oxide Single-Electron Transistor
NASA Astrophysics Data System (ADS)
Cheng, Guanglei
2012-02-01
Devices that confine and process single electrons represent an important scaling limit of electronics. Such devices have been realized in a variety of materials and exhibit remarkable electronic, optical and spintronic properties. Here, we use an atomic force microscope tip to reversibly ``sketch'' single-electron transistors by controlling a metal-insulator transition at the interface of two oxides.ootnotetextCheng et al., Nature Nanotechnology 6, 343 (2011). In these devices, single electrons tunnel resonantly between source and drain electrodes through a conducting oxide island with a diameter of ˜1.5 nm. We demonstrate control over the number of electrons on the island using bottom- and side-gate electrodes, and observe hysteresis in electron occupation that is attributed to ferroelectricity within the oxide heterostructure. These single-electron devices may find use as ultradense non-volatile memories, nanoscale hybrid piezoelectric and charge sensors, as well as building blocks in quantum information processing and simulation platforms.
Methods of fabricating nanostructures and nanowires and devices fabricated therefrom
Majumdar, Arun [Orinda, CA; Shakouri, Ali [Santa Cruz, CA; Sands, Timothy D [Moraga, CA; Yang, Peidong [Berkeley, CA; Mao, Samuel S [Berkeley, CA; Russo, Richard E [Walnut Creek, CA; Feick, Henning [Kensington, CA; Weber, Eicke R [Oakland, CA; Kind, Hannes [Schaffhausen, CH; Huang, Michael [Los Angeles, CA; Yan, Haoquan [Albany, CA; Wu, Yiying [Albany, CA; Fan, Rong [El Cerrito, CA
2009-08-04
One-dimensional nanostructures having uniform diameters of less than approximately 200 nm. These inventive nanostructures, which we refer to as "nanowires", include single-crystalline homostructures as well as heterostructures of at least two single-crystalline materials having different chemical compositions. Because single-crystalline materials are used to form the heterostructure, the resultant heterostructure will be single-crystalline as well. The nanowire heterostructures are generally based on a semiconducting wire wherein the doping and composition are controlled in either the longitudinal or radial directions, or in both directions, to yield a wire that comprises different materials. Examples of resulting nanowire heterostructures include a longitudinal heterostructure nanowire (LOHN) and a coaxial heterostructure nanowire (COHN).
Methods Of Fabricating Nanosturctures And Nanowires And Devices Fabricated Therefrom
Majumdar, Arun; Shakouri, Ali; Sands, Timothy D.; Yang, Peidong; Mao, Samuel S.; Russo, Richard E.; Feick, Henning; Weber, Eicke R.; Kind, Hannes; Huang, Michael; Yan, Haoquan; Wu, Yiying; Fan, Rong
2006-02-07
One-dimensional nanostructures having uniform diameters of less than approximately 200 nm. These inventive nanostructures, which we refer to as "nanowires", include single-crystalline homostructures as well as heterostructures of at least two single-crystalline materials having different chemical compositions. Because single-crystalline materials are used to form the heterostructure, the resultant heterostructure will be single-crystalline as well. The nanowire heterostructures are generally based on a semiconducting wire wherein the doping and composition are controlled in either the longitudinal or radial directions, or in both directions, to yield a wire that comprises different materials. Examples of resulting nanowire heterostructures include a longitudinal heterostructure nanowire (LOHN) and a coaxial heterostructure nanowire (COHN).
Methods of fabricating nanostructures and nanowires and devices fabricated therefrom
Majumdar, Arun; Shakouri, Ali; Sands, Timothy D.; Yang, Peidong; Mao, Samuel S.; Russo, Richard E.; Feick, Henning; Weber, Eicke R.; Kind, Hannes; Huang, Michael; Yan, Haoquan; Wu, Yiying; Fan, Rong
2010-11-16
One-dimensional nanostructures having uniform diameters of less than approximately 200 nm. These inventive nanostructures, which we refer to as "nanowires", include single-crystalline homostructures as well as heterostructures of at least two single-crystalline materials having different chemical compositions. Because single-crystalline materials are used to form the heterostructure, the resultant heterostructure will be single-crystalline as well. The nanowire heterostructures are generally based on a semiconducting wire wherein the doping and composition are controlled in either the longitudinal or radial directions, or in both directions, to yield a wire that comprises different materials. Examples of resulting nanowire heterostructures include a longitudinal heterostructure nanowire (LOHN) and a coaxial heterostructure nanowire (COHN).
Methods of fabricating nanostructures and nanowires and devices fabricated therefrom
Majumdar, Arun; Shakouri, Ali; Sands, Timothy D.; Yang, Peidong; Mao, Samuel S.; Russo, Richard E.; Feick, Henning; Weber, Eicke R.; Kind, Hannes; Huang, Michael; Yan, Haoquan; Wu, Yiying; Fan, Rong
2018-01-30
One-dimensional nanostructures having uniform diameters of less than approximately 200 nm. These inventive nanostructures, which we refer to as "nanowires", include single-crystalline homostructures as well as heterostructures of at least two single-crystalline materials having different chemical compositions. Because single-crystalline materials are used to form the heterostructure, the resultant heterostructure will be single-crystalline as well. The nanowire heterostructures are generally based on a semiconducting wire wherein the doping and composition are controlled in either the longitudinal or radial directions, or in both directions, to yield a wire that comprises different materials. Examples of resulting nanowire heterostructures include a longitudinal heterostructure nanowire (LOHN) and a coaxial heterostructure nanowire (COHN).
Vempati, Sesha; Uyar, Tamer
2014-10-21
2D crystals such as graphene and its oxide counterpart have sought good research attention for their application as well as fundamental interest. Especially graphene oxide (GO) is quite interesting because of its versatility and diverse application potential. However the mechanism of fluorescence from GO is under severe discussion. To explain the emission in general two interpretations were suggested, viz localization of sp(2) clusters and involvement of oxygeneous functional groups. Despite this disagreement, it should be acknowledged that the heterogeneous atomic structure, synthesis dependent and uncontrollable implantation of oxygen functional groups on the basal plane make such explanations more difficult. Nevertheless, a suitable explanation enhances the applicability of the material which also enables the design of novel materials. At this juncture we believe that given the complexity in understanding the emission mechanism it would be very useful to review the literature. In this perspective we juxtapose various results related to fluorescence and influencing factors so that a conclusive interpretation may be unveiled. Apparently, the existing interpretations have largely ignored the factors such as self-rolling, byproduct formation etc. Vis-a-vis previous reviews did not discuss the interfacial charge transfer across heterostructures and the implication on the optical properties of GO or reduced graphene oxide (rGO). Such analysis would be very insightful to determine the energetic location of sub band gap states. Moreover, ionic and π-π type interactions are also considered for their influence on emission properties. Apart from these, quantum dots, covalent modifications and nonlinear optical properties of GO and rGO were discussed for completeness. Finally we made concluding remarks with outlook.
Impurity-induced disorder in III-nitride materials and devices
Wierer, Jr., Jonathan J; Allerman, Andrew A
2014-11-25
A method for impurity-induced disordering in III-nitride materials comprises growing a III-nitride heterostructure at a growth temperature and doping the heterostructure layers with a dopant during or after the growth of the heterostructure and post-growth annealing of the heterostructure. The post-growth annealing temperature can be sufficiently high to induce disorder of the heterostructure layer interfaces.
NASA Astrophysics Data System (ADS)
Sydor, O. M.
2016-09-01
The investigations of photoelectric characteristics and photoresponce spectral dependences were carried out for intrinsic oxide-InSe heterostructures (HSs) and their changes induced by bremsstrahlung γ-quanta with an energy of 1-34 MeV at fluences of 1012-1015 cm-2. The thermal oxidation of the p-InSe:Cd substrates was carried out at a temperature of 420 °С. For three selected groups of samples the duration of the process was 15 min, 60 min, and 96 h. At a short-term oxidation (15 and 60 min) a layer of In2O3 appears. The only difference between the samples of these two groups is a higher photosensitivity in the range of energy 1.25-2.8 eV of the HSs obtained after the 60 min oxidation. At the long-term oxidation the photoresponce spectra η(hν) of the obtained HSs are characterized with a sharp short-wavelength decrease at hν≅2.0 eV. It is established that the intrinsic oxide films act as transparent barrier electrodes in the corresponding HSs and are low-sensitive to γ-irradiation in the all range of fluences. The shape of the photoresponce spectra for all the gamma irradiated HSs remains practically the same. However, it was found: (i) some decrease of photosensitivity at the long-wavelength edge, (ii) decreasing the width of η(hν) at half-height, (iii) the appearance of the exciton peak, (iv) the improvement of a slope of the low-energy edge of the photoresponce spectra with increasing irradiation dose whereas at the maximum fluence this parameter decreases, and (v) the slight extension of the spectral sensitivity to the short-wavelength range for the structures obtained after oxidation for 96 h. The photoelectric parameters of the intrinsic oxide-p-InSe HSs, open circuit voltage Voc, short-circuit current Jsc, current SIλmax and voltage SVλmax sensitivities become only improved after irradiation with the fluences 1012-1013 cm-2. At the maximum fluence a small decreasing of the values of Voc and Jsc was detected except for the structures obtained after oxidation for 15 min. An increase of the SIλmax and SVλmax sensitivities in comparison with the initial value were found for all the HSs even at the maximum fluence except for the structures obtained by a long-term oxidation.
Van der Waals epitaxy of functional MoO{sub 2} film on mica for flexible electronics
DOE Office of Scientific and Technical Information (OSTI.GOV)
Ma, Chun-Hao; Department of Materials Science and Engineering, National Chiao Tung University, Hsinchu 30010, Taiwan; Lin, Jheng-Cyuan
Flexible electronics have a great potential to impact consumer electronics and with that our daily life. Currently, no direct growth of epitaxial functional oxides on commercially available flexible substrates is possible. In this study, in order to address this challenge, muscovite, a common layered oxide, is used as a flexible substrate that is chemically similar to typical functional oxides. We fabricated epitaxial MoO{sub 2} films on muscovite via pulsed laser deposition technique. A combination of X-ray diffraction and transmission electron microscopy confirms van der Waals epitaxy of the heterostructures. The electrical transport properties of MoO{sub 2} films are similar tomore » those of the bulk. Flexible or free-standing MoO{sub 2} thin film can be obtained and serve as a template to integrate additional functional oxide layers. Our study demonstrates a remarkable concept to create flexible electronics based on functional oxides.« less
Studies on the InAlN/InGaN/InAlN/InGaN double channel heterostructures with low sheet resistance
NASA Astrophysics Data System (ADS)
Zhang, Yachao; Wang, Zhizhe; Xu, Shengrui; Chen, Dazheng; Bao, Weimin; Zhang, Jinfeng; Zhang, Jincheng; Hao, Yue
2017-11-01
High quality InAlN/InGaN/InAlN/InGaN double channel heterostructures were proposed and grown by metal organic chemical vapor deposition. Benefiting from the adoption of the pulsed growth method and Two-Step AlN interlayer, the material quality and interface characteristics of the double channel heterostructures are satisfactory. The results of the temperature-dependent Hall effect measurement indicated that the transport properties of the double channel heterostructures were superior to those of the traditional single channel heterostructures in the whole test temperature range. Meanwhile, the sheet resistance of the double channel heterostructures reached 218.5 Ω/□ at 300 K, which is the record of InGaN-based heterostructures. The good transport properties of the InGaN double channel heterostructures are beneficial to improve the performance of the microwave power devices based on nitride semiconductors.
Shiue, Ren-Jye; Gao, Yuanda; Wang, Yifei; Peng, Cheng; Robertson, Alexander D; Efetov, Dmitri K; Assefa, Solomon; Koppens, Frank H L; Hone, James; Englund, Dirk
2015-11-11
Graphene and other two-dimensional (2D) materials have emerged as promising materials for broadband and ultrafast photodetection and optical modulation. These optoelectronic capabilities can augment complementary metal-oxide-semiconductor (CMOS) devices for high-speed and low-power optical interconnects. Here, we demonstrate an on-chip ultrafast photodetector based on a two-dimensional heterostructure consisting of high-quality graphene encapsulated in hexagonal boron nitride. Coupled to the optical mode of a silicon waveguide, this 2D heterostructure-based photodetector exhibits a maximum responsivity of 0.36 A/W and high-speed operation with a 3 dB cutoff at 42 GHz. From photocurrent measurements as a function of the top-gate and source-drain voltages, we conclude that the photoresponse is consistent with hot electron mediated effects. At moderate peak powers above 50 mW, we observe a saturating photocurrent consistent with the mechanisms of electron-phonon supercollision cooling. This nonlinear photoresponse enables optical on-chip autocorrelation measurements with picosecond-scale timing resolution and exceptionally low peak powers.
DOE Office of Scientific and Technical Information (OSTI.GOV)
Li, Binzhi; Chopdekar, Rajesh V.; N'Diaye, Alpha T.
The impact of interfacial electronic reconstruction on the magnetic characteristics of La0.7Sr0.3CoO3 (LSCO)/La0.7Sr0.3MnO3 (LSMO) superlattices was investigated as a function of layer thickness using a combination of soft x-ray magnetic spectroscopy and bulk magnetometry. We found that the magnetic properties of the LSCO layers are impacted by two competing electronic interactions occurring at the LSCO/substrate and LSMO/LSCO interfaces. For thin LSCO layers (< 5 nm), the heterostructures exist in a highly coupled state where the chemically distinct layers behave as a single magnetic compound with magnetically active Co2+ ions. As the LSCO thickness increases, a high coercivity LSCO layer developsmore » which biases a low coercivity layer, which is composed not only of the LSMO layer, but also an interfacial LSCO layer. These results suggest a new route to tune the magnetic properties of transition metal oxide heterostructures through careful control of the interface structure.« less
NASA Astrophysics Data System (ADS)
Uchida, Takayuki; Jinno, Riena; Takemoto, Shu; Kaneko, Kentaro; Fujita, Shizuo
2018-04-01
The band alignment at an α-Ga2O3/α-(Al x Ga1‑ x )2O3 heterointerface, with different Al compositions (x), grown on a c-plane sapphire substrate was evaluated by X-ray photoelectron spectroscopy. The experimental results show that the heterointerface has the type-I band discontinuity with the valence band offsets of 0.090, 0.12, and 0.14 eV, and the conduction band offsets of 0.34, 0.79, and 1.87 eV, for x values of 0.1, 0.4, and 0.8, respectively. The small band offset for the valence band is attributed to the fact that the valence band of oxides is constituted by the localized O 2p level, which is dominated by the nature of oxygen atoms. The type-I band discontinuity is desirable for a variety of heterostructure devices.
Dynamic observation on the growth behaviors in manganese silicide/silicon nanowire heterostructures.
Hsieh, Yu-Hsun; Chiu, Chung-Hua; Huang, Chun-Wei; Chen, Jui-Yuan; Lin, Wan-Jhen; Wu, Wen-Wei
2015-02-07
Metal silicide nanowires (NWs) are very interesting materials with diverse physical properties. Among the silicides, manganese silicide nanostructures have attracted wide attention due to their several potential applications, including in microelectronics, optoelectronics, spintronics and thermoelectric devices. In this work, we exhibited the formation of pure manganese silicide and manganese silicide/silicon nanowire heterostructures through solid state reaction with line contacts between manganese pads and silicon NWs. Dynamical process and phase characterization were investigated by in situ transmission electron microscopy (in situ TEM) and spherical aberration corrected scanning transmission electron microscopy (Cs-corrected STEM), respectively. The growth dynamics of the manganese silicide phase under thermal effects were systematically studied. Additionally, Al2O3, serving as the surface oxide, altered the growth behavior of the MnSi nanowire, enhancing the silicide/Si epitaxial growth and effecting the diffusion process in the silicon nanowire as well. In addition to fundamental science, this significant study has great potential in advancing future processing techniques in nanotechnology and related applications.
NASA Astrophysics Data System (ADS)
Marquardt, Oliver; Krause, Thilo; Kaganer, Vladimir; Martín-Sánchez, Javier; Hanke, Michael; Brandt, Oliver
2017-05-01
We present a systematic theoretical study of the influence of elastic strain relaxation on the built-in electrostatic potentials and the electronic properties of axial {{In}}x{{Ga}}1-x{{N}}/{GaN} nanowire (NW) heterostructures. Our simulations reveal that for a sufficiently large ratio between the thickness of the {{In}}x{{Ga}}1-x{{N}} disk and the diameter of the NW, the elastic relaxation leads to a significant reduction of the built-in electrostatic potential in comparison to a planar system of similar layer thickness and In content. In this case, the ground state transition energies approach constant values with increasing thickness of the disk and only depend on the In content, a behavior usually associated to that of a quantum well free of built-in electrostatic potentials. We show that the structures under consideration are by no means field-free, and the built-in potentials continue to play an important role even for ultrathin NWs. In particular, strain and the resulting polarization potentials induce complex confinement features of electrons and holes, which depend on the In content, shape, and dimensions of the heterostructure.
Carey, Tian; Cacovich, Stefania; Divitini, Giorgio; Ren, Jiesheng; Mansouri, Aida; Kim, Jong M; Wang, Chaoxia; Ducati, Caterina; Sordan, Roman; Torrisi, Felice
2017-10-31
Fully printed wearable electronics based on two-dimensional (2D) material heterojunction structures also known as heterostructures, such as field-effect transistors, require robust and reproducible printed multi-layer stacks consisting of active channel, dielectric and conductive contact layers. Solution processing of graphite and other layered materials provides low-cost inks enabling printed electronic devices, for example by inkjet printing. However, the limited quality of the 2D-material inks, the complexity of the layered arrangement, and the lack of a dielectric 2D-material ink able to operate at room temperature, under strain and after several washing cycles has impeded the fabrication of electronic devices on textile with fully printed 2D heterostructures. Here we demonstrate fully inkjet-printed 2D-material active heterostructures with graphene and hexagonal-boron nitride (h-BN) inks, and use them to fabricate all inkjet-printed flexible and washable field-effect transistors on textile, reaching a field-effect mobility of ~91 cm 2 V -1 s -1 , at low voltage (<5 V). This enables fully inkjet-printed electronic circuits, such as reprogrammable volatile memory cells, complementary inverters and OR logic gates.
ERIC Educational Resources Information Center
Afanasiev, Sergey A.; Afanasiev, Mikhail S.; Zhukov, Alexander O.; Egorov, Vladimir K.; Egorov, Evgeniy V.
2016-01-01
The background of the study is that the planar film heterostructures are nowadays the most common objects nanophotonic and nanoelectronic technologies. The authors noted that, among such objects found so-called quantum wells, which are formed by a complex series of nanoscale layers are deposited with differing elemental composition, and simple…
Phase Separation from Electron Confinement at Oxide Interfaces
NASA Astrophysics Data System (ADS)
Scopigno, N.; Bucheli, D.; Caprara, S.; Biscaras, J.; Bergeal, N.; Lesueur, J.; Grilli, M.
2016-01-01
Oxide heterostructures are of great interest for both fundamental and applicative reasons. In particular, the two-dimensional electron gas at the LaAlO3/SrTiO3 or LaTiO3/SrTiO3 interfaces displays many different properties and functionalities. However, there are clear experimental indications that the interface electronic state is strongly inhomogeneous and therefore it is crucial to investigate possible intrinsic mechanisms underlying this inhomogeneity. Here, the electrostatic potential confining the electron gas at the interface is calculated self-consistently, finding that such confinement may induce phase separation, to avoid a thermodynamically unstable state with a negative compressibility. This provides a robust mechanism for the inhomogeneous character of these interfaces.
Jiang, Xiaocheng; Tian, Bozhi; Xiang, Jie; Qian, Fang; Zheng, Gengfeng; Wang, Hongtao; Mai, Liqiang; Lieber, Charles M.
2011-01-01
Branched nanostructures represent unique, 3D building blocks for the “bottom-up” paradigm of nanoscale science and technology. Here, we report a rational, multistep approach toward the general synthesis of 3D branched nanowire (NW) heterostructures. Single-crystalline semiconductor, including groups IV, III–V, and II–VI, and metal branches have been selectively grown on core or core/shell NW backbones, with the composition, morphology, and doping of core (core/shell) NWs and branch NWs well controlled during synthesis. Measurements made on the different composition branched NW structures demonstrate encoding of functional p-type/n-type diodes and light-emitting diodes (LEDs) as well as field effect transistors with device function localized at the branch/backbone NW junctions. In addition, multibranch/backbone NW structures were synthesized and used to demonstrate capability to create addressable nanoscale LED arrays, logic circuits, and biological sensors. Our work demonstrates a previously undescribed level of structural and functional complexity in NW materials, and more generally, highlights the potential of bottom-up synthesis to yield increasingly complex functional systems in the future. PMID:21730174
France-Lanord, Arthur; Soukiassian, Patrick; Glattli, Christian; Wimmer, Erich
2016-03-14
In an effort to extend the reach of current ab initio calculations to simulations requiring millions of configurations for complex systems such as heterostructures, we have parameterized the third-generation Charge Optimized Many-Body (COMB3) potential using solely ab initio total energies, forces, and stress tensors as input. The quality and the predictive power of the new forcefield are assessed by computing properties including the cohesive energy and density of SiO2 polymorphs, surface energies of alpha-quartz, and phonon densities of states of crystalline and amorphous phases of SiO2. Comparison with data from experiments, ab initio calculations, and molecular dynamics simulations using published forcefields including BKS (van Beest, Kramer, and van Santen), ReaxFF, and COMB2 demonstrates an overall improvement of the new parameterization. The computed temperature dependence of the thermal conductivity of crystalline alpha-quartz and the Kapitza resistance of the interface between crystalline Si(001) and amorphous silica is in excellent agreement with experiment, setting the stage for simulations of complex nanoscale heterostructures.
Qi, Zhengqing John; Hong, Sung Ju; Rodríguez-Manzo, Julio A; Kybert, Nicholas J; Gudibande, Rajatesh; Drndić, Marija; Park, Yung Woo; Johnson, A T Charlie
2015-03-25
CVD graphene devices on stacked CVD hexagonal boron nitride (hBN) are demonstrated using a novel low-contamination transfer method, and their electrical performance is systematically compared to devices on SiO(2). An order of magnitude improvement in mobility, sheet resistivity, current density, and sustained power is reported when the oxide substrate is covered with five-layer CVD hBN. © 2014 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.
Naturally formed ultrathin V2O5 heteroepitaxial layer on VO2/sapphire(001) film
NASA Astrophysics Data System (ADS)
Littlejohn, Aaron J.; Yang, Yunbo; Lu, Zonghuan; Shin, Eunsung; Pan, KuanChang; Subramanyam, Guru; Vasilyev, Vladimir; Leedy, Kevin; Quach, Tony; Lu, Toh-Ming; Wang, Gwo-Ching
2017-10-01
Vanadium dioxide (VO2) and vanadium pentoxide (V2O5) thin films change their properties in response to external stimuli such as photons, temperature, electric field and magnetic field and have applications in electronics, optical devices, and sensors. Due to the multiple valence states of V and non-stoichiometry in thin films, it is challenging to grow epitaxial, single-phase V-oxide on a substrate, or a heterostructure of two epitaxial V-oxides. We report the formation of a heterostructure consisting of a few nm thick ultrathin V2O5 epitaxial layer on pulsed laser deposited tens of nm thick epitaxial VO2 thin films grown on single crystal Al2O3(001) substrates without post annealing of the VO2 film. The simultaneous observation of the ultrathin epitaxial V2O5 layer and VO2 epitaxial film is only possible by our unique reflection high energy electron diffraction pole figure analysis. The out-of-plane and in-plane epitaxial relationships are V2O5[100]||VO2[010]||Al2O3[001] and V2O5[03 2 bar ]||VO2[100]||Al2O3[1 1 bar 0], respectively. The existence of the V2O5 layer on the surface of the VO2 film is also supported by X-ray photoelectron spectroscopy and Raman spectroscopy.
Effective theory of exotic superconductivity in LaAlO3/SrTiO3 interfaces
NASA Astrophysics Data System (ADS)
Esmailzadeh, Haniyeh; Moghaddam, Ali G.
2018-05-01
Motivated by experimental and theoretical works about superconductivity at the oxide interfaces, we provide a simple model for possible unconventional pairings inside the exotic two-dimensional electron gas formed in heterostructures of SrTiO3 and LaAlO3. At the low energy limit, the electron gas at the interfaces is usually modeled with an effective three band model considering of 3d t2g orbitals which are slightly coupled by atomic spin-orbit couplings (SOC). Considering direct superconducting pairing in two higher delocalized bands and by exploiting a perturbative scheme based on canonical transformation, we derive the effective pairing amplitudes with possibly exotic nature inside the localized dxy band as well as various inter-band pairing components. In particular we show that equal-spin triplet pairings are possible between the band dxy and any of other dxz and dyz bands. In addition weaker effective pairings take place inside the localized band itself and between delocalized dxz and dyz bands with singlet and opposite-spin triplet characters. These unconventional effective pairings are indeed mediated by SOC-induced higher order virtual transitions between the bands and particularly into the localized band. Our model suggest that unconventional effective superconductivity is possible at oxide interfaces, simply, due to the special band structure and important role of atomic SOC and perhaps other magnetic effects present at these heterostructures.
Stability and band offsets between c-plane ZnO semiconductor and LaAlO3 gate dielectric
NASA Astrophysics Data System (ADS)
Wang, Jianli; Chen, Xinfeng; Wu, Shuyin; Tang, Gang; Zhang, Junting; Stampfl, C.
2018-03-01
Wurtzite-perovskite heterostructures composed of a high dielectric constant oxide and a wide bandgap semiconductor envision promising applications in field-effect transistors. In the present paper, the structural and electronic properties of LaAlO3/ZnO heterojunctions are investigated by first-principles calculations. We study the initial adsorption of La, Al, and oxygen atoms on ZnO (0001) and (000 1 ¯ ) surfaces and find that La atoms may occupy interstitial sites during the growth of stoichiometric ZnO (0001). The band gap of the stoichiometric ZnO (0001) surface is smaller than that of the stoichiometric ZnO (000 1 ¯ ) surface. The surface formation energy indicates that La or Al atoms may substitute Zn atoms at the nonstoichiometric ZnO (0001) surface. The atomic charges, electronic density of states, and band offsets are analyzed for the optimized LaAlO3/ZnO heterojunctions. There is a band gap for the LaAlO3/ZnO (000 1 ¯ ) heterostructures, and the largest variation in charge occurs at the surface or interface. Our results suggest that the Al-terminated LaAlO3/ZnO (000 1 ¯ ) interfaces are suitable for the design of metal oxide semiconductor devices because the valence and conduction band offsets are both larger than 1 eV and the interface does not produce any in-gap states.
Atomic layer MoS2-graphene van der Waals heterostructure nanomechanical resonators.
Ye, Fan; Lee, Jaesung; Feng, Philip X-L
2017-11-30
Heterostructures play significant roles in modern semiconductor devices and micro/nanosystems in a plethora of applications in electronics, optoelectronics, and transducers. While state-of-the-art heterostructures often involve stacks of crystalline epi-layers each down to a few nanometers thick, the intriguing limit would be hetero-atomic-layer structures. Here we report the first experimental demonstration of freestanding van der Waals heterostructures and their functional nanomechanical devices. By stacking single-layer (1L) MoS 2 on top of suspended single-, bi-, tri- and four-layer (1L to 4L) graphene sheets, we realize an array of MoS 2 -graphene heterostructures with varying thickness and size. These heterostructures all exhibit robust nanomechanical resonances in the very high frequency (VHF) band (up to ∼100 MHz). We observe that fundamental-mode resonance frequencies of the heterostructure devices fall between the values of graphene and MoS 2 devices. Quality (Q) factors of heterostructure resonators are lower than those of graphene but comparable to those of MoS 2 devices, suggesting interface damping related to interlayer interactions in the van der Waals heterostructures. This study validates suspended atomic layer heterostructures as an effective device platform and provides opportunities for exploiting mechanically coupled effects and interlayer interactions in such devices.
Electronic properties of ZnPSe3-MoS2 Van der Waals heterostructure
NASA Astrophysics Data System (ADS)
Sharma, Munish; Kumar, Ashok; Ahluwalia, P. K.
2018-04-01
We present a comparative study of electronic properties of ZnPSe3-MoS2 heterostructure using GGA-PBE functional and DFT-D2 method within the framework of density functional theory (DFT). Electronic band structure for the considered heterostructure shows a direct band gap semiconducting character. A decrease in band gap is observed with the heterostructuring as compared to their constituent pristine monolayers. The alignment of valance band maxima and conduction band minima on different layers in heterostructure indicate the physical separation of charge carriers. A work function of 5.31 eV has been calculated for ZnPSe3-MoS2 heterostructure. These results provide a physical basis for the potential applications of these ZnPSe3-MoS2 heterostructure in optoelectronic devices.
Two-dimensional GaSe/MoSe 2 misfit bilayer heterojunctions by van der Waals epitaxy
DOE Office of Scientific and Technical Information (OSTI.GOV)
Li, Xufan; Lin, Ming-Wei; Lin, Junhao
Two-dimensional (2D) heterostructures hold the promise for future atomically-thin electronics and optoelectronics due to their diverse functionalities. While heterostructures consisting of different transition metal dichacolgenide monolayers with well-matched lattices and novel physical properties have been successfully fabricated via van der Waals (vdW) or edge epitaxy, constructing heterostructures from monolayers of layered semiconductors with large lattice misfits still remains challenging. Here, we report the growth of monolayer GaSe/MoSe 2 heterostructures with large lattice misfit by two-step chemical vapor deposition (CVD). Both vertically stacked and lateral heterostructures are demonstrated. The vertically stacked GaSe/MoSe 2 heterostructures exhibit vdW epitaxy with well-aligned lattice orientationmore » between the two layers, forming an incommensurate vdW heterostructure. However, the lateral heterostructures exhibit no lateral epitaxial alignment at the interface between GaSe and MoSe 2 crystalline domains. Instead of a direct lateral connection at the boundary region where the same lattice orientation is observed between GaSe and MoSe 2 monolayer domains in lateral GaSe/MoSe 2 heterostructures, GaSe monolayers are found to overgrow MoSe 2 during CVD, forming a stripe of vertically stacked vdW heterostructure at the crystal interface. Such vertically-stacked vdW GaSe/MoSe 2 heterostructures are shown to form p-n junctions with effective transport and separation of photo-generated charge carriers between layers, resulting in a gate-tunable photovoltaic response. In conclusion, these GaSe/MoSe 2 vdW heterostructures should have applications as gate-tunable field-effect transistors, photodetectors, and solar cells.« less
Two-dimensional GaSe/MoSe 2 misfit bilayer heterojunctions by van der Waals epitaxy
Li, Xufan; Lin, Ming-Wei; Lin, Junhao; ...
2016-04-01
Two-dimensional (2D) heterostructures hold the promise for future atomically-thin electronics and optoelectronics due to their diverse functionalities. While heterostructures consisting of different transition metal dichacolgenide monolayers with well-matched lattices and novel physical properties have been successfully fabricated via van der Waals (vdW) or edge epitaxy, constructing heterostructures from monolayers of layered semiconductors with large lattice misfits still remains challenging. Here, we report the growth of monolayer GaSe/MoSe 2 heterostructures with large lattice misfit by two-step chemical vapor deposition (CVD). Both vertically stacked and lateral heterostructures are demonstrated. The vertically stacked GaSe/MoSe 2 heterostructures exhibit vdW epitaxy with well-aligned lattice orientationmore » between the two layers, forming an incommensurate vdW heterostructure. However, the lateral heterostructures exhibit no lateral epitaxial alignment at the interface between GaSe and MoSe 2 crystalline domains. Instead of a direct lateral connection at the boundary region where the same lattice orientation is observed between GaSe and MoSe 2 monolayer domains in lateral GaSe/MoSe 2 heterostructures, GaSe monolayers are found to overgrow MoSe 2 during CVD, forming a stripe of vertically stacked vdW heterostructure at the crystal interface. Such vertically-stacked vdW GaSe/MoSe 2 heterostructures are shown to form p-n junctions with effective transport and separation of photo-generated charge carriers between layers, resulting in a gate-tunable photovoltaic response. In conclusion, these GaSe/MoSe 2 vdW heterostructures should have applications as gate-tunable field-effect transistors, photodetectors, and solar cells.« less
DOE Office of Scientific and Technical Information (OSTI.GOV)
Morrison, C., E-mail: c.morrison.2@warwick.ac.uk; Casteleiro, C.; Leadley, D. R.
The complex quantum transport of a strained Ge quantum well (QW) modulation doped heterostructure with two types of mobile carriers has been observed. The two dimensional hole gas (2DHG) in the Ge QW exhibits an exceptionally high mobility of 780 000 cm{sup 2}/Vs at temperatures below 10 K. Through analysis of Shubnikov de-Haas oscillations in the magnetoresistance of this 2DHG below 2 K, the hole effective mass is found to be 0.065 m{sub 0}. Anomalous conductance peaks are observed at higher fields which deviate from standard Shubnikov de-Haas and quantum Hall effect behaviour due to conduction via multiple carrier types. Despite this complex behaviour,more » analysis using a transport model with two conductive channels explains this behaviour and allows key physical parameters such as the carrier effective mass, transport, and quantum lifetimes and conductivity of the electrically active layers to be extracted. This finding is important for electronic device applications, since inclusion of highly doped interlayers which are electrically active, for enhancement of, for example, room temperature carrier mobility, does not prevent analysis of quantum transport in a QW.« less
Tin monochalcogenide heterostructures as mechanically rigid infrared band gap semiconductors
NASA Astrophysics Data System (ADS)
Özçelik, V. Ongun; Fathi, Mohammad; Azadani, Javad G.; Low, Tony
2018-05-01
Based on first-principles density functional calculations, we show that SnS and SnSe layers can form mechanically rigid heterostructures with the constituent puckered or buckled monolayers. Due to the strong interlayer coupling, the electronic wave functions of the conduction and valence band edges are delocalized across the heterostructure. The resultant band gaps of the heterostructures reside in the infrared region. With strain engineering, the heterostructure band gap undergoes a transition from indirect to direct in the puckered phase. Our results show that there is a direct correlation between the electronic wave function and the mechanical rigidity of the layered heterostructure.
Two-dimensional GaSe/MoSe2 misfit bilayer heterojunctions by van der Waals epitaxy.
Li, Xufan; Lin, Ming-Wei; Lin, Junhao; Huang, Bing; Puretzky, Alexander A; Ma, Cheng; Wang, Kai; Zhou, Wu; Pantelides, Sokrates T; Chi, Miaofang; Kravchenko, Ivan; Fowlkes, Jason; Rouleau, Christopher M; Geohegan, David B; Xiao, Kai
2016-04-01
Two-dimensional (2D) heterostructures hold the promise for future atomically thin electronics and optoelectronics because of their diverse functionalities. Although heterostructures consisting of different 2D materials with well-matched lattices and novel physical properties have been successfully fabricated via van der Waals (vdW) epitaxy, constructing heterostructures from layered semiconductors with large lattice misfits remains challenging. We report the growth of 2D GaSe/MoSe2 heterostructures with a large lattice misfit using two-step chemical vapor deposition (CVD). Both vertically stacked and lateral heterostructures are demonstrated. The vertically stacked GaSe/MoSe2 heterostructures exhibit vdW epitaxy with well-aligned lattice orientation between the two layers, forming a periodic superlattice. However, the lateral heterostructures exhibit no lateral epitaxial alignment at the interface between GaSe and MoSe2 crystalline domains. Instead of a direct lateral connection at the boundary region where the same lattice orientation is observed between GaSe and MoSe2 monolayer domains in lateral GaSe/MoSe2 heterostructures, GaSe monolayers are found to overgrow MoSe2 during CVD, forming a stripe of vertically stacked vdW heterostructures at the crystal interface. Such vertically stacked vdW GaSe/MoSe2 heterostructures are shown to form p-n junctions with effective transport and separation of photogenerated charge carriers between layers, resulting in a gate-tunable photovoltaic response. These GaSe/MoSe2 vdW heterostructures should have applications as gate-tunable field-effect transistors, photodetectors, and solar cells.
Two-dimensional GaSe/MoSe2 misfit bilayer heterojunctions by van der Waals epitaxy
Li, Xufan; Lin, Ming-Wei; Lin, Junhao; Huang, Bing; Puretzky, Alexander A.; Ma, Cheng; Wang, Kai; Zhou, Wu; Pantelides, Sokrates T.; Chi, Miaofang; Kravchenko, Ivan; Fowlkes, Jason; Rouleau, Christopher M.; Geohegan, David B.; Xiao, Kai
2016-01-01
Two-dimensional (2D) heterostructures hold the promise for future atomically thin electronics and optoelectronics because of their diverse functionalities. Although heterostructures consisting of different 2D materials with well-matched lattices and novel physical properties have been successfully fabricated via van der Waals (vdW) epitaxy, constructing heterostructures from layered semiconductors with large lattice misfits remains challenging. We report the growth of 2D GaSe/MoSe2 heterostructures with a large lattice misfit using two-step chemical vapor deposition (CVD). Both vertically stacked and lateral heterostructures are demonstrated. The vertically stacked GaSe/MoSe2 heterostructures exhibit vdW epitaxy with well-aligned lattice orientation between the two layers, forming a periodic superlattice. However, the lateral heterostructures exhibit no lateral epitaxial alignment at the interface between GaSe and MoSe2 crystalline domains. Instead of a direct lateral connection at the boundary region where the same lattice orientation is observed between GaSe and MoSe2 monolayer domains in lateral GaSe/MoSe2 heterostructures, GaSe monolayers are found to overgrow MoSe2 during CVD, forming a stripe of vertically stacked vdW heterostructures at the crystal interface. Such vertically stacked vdW GaSe/MoSe2 heterostructures are shown to form p-n junctions with effective transport and separation of photogenerated charge carriers between layers, resulting in a gate-tunable photovoltaic response. These GaSe/MoSe2 vdW heterostructures should have applications as gate-tunable field-effect transistors, photodetectors, and solar cells. PMID:27152356
Determination of interfacial states in solid heterostructures using a variable-energy positron beam
Asoka kumar, Palakkal P. V.; Lynn, Kelvin G.
1993-01-01
A method and means is provided for characterizing interfacial electron states in solid heterostructures using a variable energy positron beam to probe the solid heterostructure. The method includes the steps of directing a positron beam having a selected energy level at a point on the solid heterostructure so that the positron beam penetrates into the solid heterostructure and causes positrons to collide with the electrons at an interface of the solid heterostructure. The number and energy of gamma rays emitted from the solid heterostructure as a result of the annihilation of positrons with electrons at the interface are detected. The data is quantified as a function of the Doppler broadening of the photopeak about the 511 keV line created by the annihilation of the positrons and electrons at the interface, preferably, as an S-parameter function; and a normalized S-parameter function of the data is obtained. The function of data obtained is compared with a corresponding function of the Doppler broadening of the annihilation photopeak about 511 keV for a positron beam having a second energy level directed at the same material making up a portion of the solid heterostructure. The comparison of these functions facilitates characterization of the interfacial states of electrons in the solid heterostructure at points corresponding to the penetration of positrons having the particular energy levels into the interface of the solid heterostructure. Accordingly, the invention provides a variable-energy non-destructive probe of solid heterostructures, such as SiO.sub.2 /Si, MOS or other semiconductor devices.
Determination of interfacial states in solid heterostructures using a variable-energy positron beam
Asokakumar, P.P.V.; Lynn, K.G.
1993-04-06
A method and means is provided for characterizing interfacial electron states in solid heterostructures using a variable energy positron beam to probe the solid heterostructure. The method includes the steps of directing a positron beam having a selected energy level at a point on the solid heterostructure so that the positron beam penetrates into the solid heterostructure and causes positrons to collide with the electrons at an interface of the solid heterostructure. The number and energy of gamma rays emitted from the solid heterostructure as a result of the annihilation of positrons with electrons at the interface are detected. The data is quantified as a function of the Doppler broadening of the photopeak about the 511 keV line created by the annihilation of the positrons and electrons at the interface, preferably, as an S-parameter function; and a normalized S-parameter function of the data is obtained. The function of data obtained is compared with a corresponding function of the Doppler broadening of the annihilation photopeak about 511 keV for a positron beam having a second energy level directed at the same material making up a portion of the solid heterostructure. The comparison of these functions facilitates characterization of the interfacial states of electrons in the solid heterostructure at points corresponding to the penetration of positrons having the particular energy levels into the interface of the solid heterostructure. Accordingly, the invention provides a variable-energy non-destructive probe of solid heterostructures, such as SiO[sub 2]/Si, MOS or other semiconductor devices.
Epitaxial strain-mediated spin-state transitions: can we switch off magnetism?
NASA Astrophysics Data System (ADS)
Rondinelli, James; Spaldin, Nicola
2008-03-01
We use first-principles density functional theory calculations to explore spin-state transitions in epitaxially strained LaCoO3. While high-spin to low-spin state transitions in minerals are common in geophysics, where pressures can reach over 200 GPa, we explore whether heteroepitaxial strain can achieve similar transitions with moderate strain in thin films. LaCoO3 is known to undergo a low-spin (S=0, t2g^6eg^0) to intermediate-spin (S=1, t2g^5eg^1) or high-spin (S=2, t2g^4eg^2) state transition with increasing temperature, and thus makes it a promising candidate material for strain-mediated spin transitions. Here we discuss the physics of the low-spin transition and changes in the electronic structure of LaCoO3, most notably, the metal-insulator transition that accompanies the spin-state transitions with epitaxial strain. As thin film growth techniques continue to reach atomic-level precision, we suggest this is another approach for controlling magnetism in complex oxide heterostructures.
Materials and processing science: Limits for microelectronics
NASA Astrophysics Data System (ADS)
Rosenberg, R.
1988-09-01
The theme of this talk will be to illustrate examples of technologies that will drive materials and processing sciences to the limit and to describe some of the research being pursued to understand materials interactions which are pervasive to projected structure fabrication. It is to be expected that the future will see a progression to nanostructures where scaling laws will be tested and quantum transport will become more in evidence, to low temperature operation for tighter control and improved performance, to complex vertical profiles where 3D stacking and superlattices will produce denser packing and device flexibility, to faster communication links with optoelectronics, and to compatible packaging technologies. New low temperature processing techniques, such as epitaxy of silicon, PECVD of dielectrics, low temperature high pressure oxidation, silicon-germanium heterostructures, etc., must be combined with shallow metallurgies, new lithographic technologies, maskless patterning, rapid thermal processing (RTP) to produce needed profile control, reduce process incompatibilities and develop new device geometries. Materials interactions are of special consequence for chip substrates and illustrations of work in metal-ceramic and metal-polymer adhesion will be offered.
DOE Office of Scientific and Technical Information (OSTI.GOV)
Bi, Feng; Huang, Mengchen; Irvin, Patrick
2015-08-24
Complex-oxide heterostructures exhibit rich physical behavior such as emergent conductivity, superconductivity, and magnetism that are intriguing for scientific reasons as well as for potential technological applications. It was recently discovered that in-plane magnetism at the LaAlO{sub 3}/SrTiO{sub 3} (LAO/STO) interface can be electronically controlled at room temperature. Here, we employ magnetic force microscopy to investigate electronically controlled ferromagnetism at the LAO/STO interface with LAO thickness t varied from 4 unit cell (u.c.) to 40 u.c. Magnetic signatures are observed only within a thickness window 8 u.c. ≤ t ≤ 25 u.c. Within this window, the device capacitance corresponds well to the expected geometric value, while for thicknessesmore » outside this window, the capacitance is strongly suppressed. The ability to modulate electronic and magnetic properties of LAO/STO devices depends on the ability to control carrier density, which is in turn constrained by intrinsic tunneling mechanisms.« less
NASA Astrophysics Data System (ADS)
Lazarenko, A. A.; Berezovskaya, T. N.; Denisov, D. V.; Sobolev, M. S.; Pirogov, E. V.; Nikitina, E. V.
2017-11-01
This article discusses the process of preparation of a silicon surface for subsequent growth of dilute nitride alloys by molecular-beam epitaxy. The method of preparation of Si (100) and Si (111) substrates was developed. This method provides reproducible high-quality silicon surface for molecular-beam epitaxy of Si-GaP heterostructures. As a result, it managed to reduce the eviction oxide temperature below 800 °C, which is an important parameter for the MBE technology.
NASA Astrophysics Data System (ADS)
Fu, Yanhui; Liang, Wei; Guo, Jinqiu; Tang, Hua; Liu, Shuaishuai
2018-02-01
A novel MoS2 quantum dots (QDs) decorated g-C3N4/Ag heterostructured photocatalyst has been synthesized via a two-step method including in situ microemulsion-assisted reduction and wetness impregnation method. The obtained heterostructure photocatalyst was characterized by X-ray diffraction (XRD), transmission electron microscopy (TEM), X-ray photoelectron spectroscopy (XPS), UV-vis diffuse reflectance spectroscopy (DRS) and photoluminescence spectrosxopy (PL). The photocatalytic activity was evaluated by the degradation of methyl orange (MO) under visible-light irradiation. The MoS2 QDs decorated hybrid photocatalysts exhibited significantly enhanced photocatalytic performance. The concentration of Ag and MoS2 QDs showing the optimal photocatalytic performance was determined to be 10% and 0.3% respectively, which exceeded the photocatalytic performance of pure g-C3N4 by more than 4.7 times. Recycling experiments confirmed that the hybrid catalysts had superior cycle performance and stability. The enhanced photocatalytic activity of MoS2 QDs decorated g-C3N4/Ag hybrid photocatalysts can be mainly ascribed to enhanced visible-light absorption, the efficient separation of photogenerated charge carriers and the stronger oxidation and reduction ability through a Z-scheme system composed of g-C3N4, Ag and MoS2 QDs, in which Ag nanoparticles act as the charge separation center. The evidence of the Z-scheme photocatalytic mechanism of the composite photocatalysts was obtained from the active species trapping experiments.
NASA Astrophysics Data System (ADS)
Shah, M. A. H.; Khan, M. K. R.; Tanveer Karim, A. M. M.; Rahman, M. M.; Kamruzzaman, M.
2018-01-01
Heterojunction diodes of n-ZnO/ p-Si (100) and n-ZnO:Al/ p-Si (100) were fabricated by spray pyrolysis technique. X-ray diffraction (XRD), energy dispersive x-ray spectroscopy (EDX), and field emission scanning electron microscopy (FESEM) were used to characterize the as-prepared samples. The XRD pattern indicates the hexagonal wurzite structure of zinc oxide (ZnO) and Al-doped ZnO (AZO) thin films grown on Si (100) substrate. The compositional analysis by EDX indicates the presence of Al in the AZO structure. The FESEM image indicates the smooth and compact surface of the heterostructures. The current-voltage characteristics of the heterojunction confirm the rectifying diode behavior at different temperatures and illumination intensities. For low forward bias voltage, the ideality factors were determined to be 1.24 and 1.38 for un-doped and Al-doped heterostructures at room temperature (RT), respectively, which indicates the good diode characteristics. The capacitance-voltage response of the heterojunctions was studied for different oscillation frequencies. From the 1/ C 2- V plot, the junction built-in potentials were found 0.30 V and 0.40 V for un-doped and Al-doped junctions at RT, respectively. The differences in built-in potential for different heterojunctions indicate the different interface state densities of the junctions. From the RT photoluminescence (PL) spectrum of the n-ZnO/ p-Si (100) heterostructure, an intense main peak at near band edge (NBE) 378 nm (3.28 eV) and weak deep-level emissions (DLE) centered at 436 nm (2.84 eV) and 412 nm (3.00 eV) were observed. The NBE emission is attributed to the radiative recombination of the free and bound excitons and the DLE results from the radiative recombination through deep level defects.
Design of lateral heterostructure from arsenene and antimonene
NASA Astrophysics Data System (ADS)
Sun, Qilong; Dai, Ying; Ma, Yandong; Yin, Na; Wei, Wei; Yu, Lin; Huang, Baibiao
2016-09-01
Lateral heterostructures fabricated by two-dimensional building blocks have opened up exciting realms in material science and device physics. Identifying suitable materials for creating such heterostructures is urgently needed for the next-generation devices. Here, we demonstrate a novel type of seamless lateral heterostructures with excellent stabilities formed within pristine arsenene and antimonene. We find that these heterostructures could possess direct and reduced energy gaps without any modulations. Moreover, the highly coveted type-II alignment and the high carrier mobility are also identified, marking the enhanced quantum efficiency. The tensile strain can result in efficient bandgap engineering. Besides, the proposed critical condition for favored direct energy gaps would have a guiding significance on the subsequent works. Generally, our predictions not only introduce new vitality into lateral heterostructures, enriching available candidate materials in this field, but also highlight the potential of these lateral heterostructures as appealing materials for future devices.
Novel Magnetic Phenomena in Oxide Thin Films, Interfaces and Heterostructures
NASA Astrophysics Data System (ADS)
Venkatesan, Thirumalai
2015-03-01
Oxide films, heterostructures and interfaces present wonderful opportunities for exploring novel magnetic phenomena. The idea of cationic vacancy induced ferromagnetism was demonstrated by observing ferromagnetism in TaxTi1-xO2(x = 2 - 6%). Using XAS, XPS and XMCD, the magnetism was mainly located at the Ti sites and was shown to arise from Ti vacancies as opposed to Ti3+. The substrate-film interface was crucial for observing the ferromagnetism, as the required concentration of Ti vacancies could only be maintained close to the interface. With electron transport we were able to see with increasing thickness the emerging role of Kondo scattering (mediated by Ti3+) and at larger thickness impurity scattering. The polar LaAlO3/non-polar SrTiO3 interface exhibits a mixture of magnetic phases most likely arising from cationic defects and selective electron occupancy in Ti t2g levels. Using XMCD ferromagnetism was seen at these interfaces even at room temperature. Unlike LaAlO3, polar LaMnO3 is an insulator exhibiting orbital order that has a smaller band gap than SrTiO3. It is a traditional antiferromagnetic material, but when grown on SrTiO3, LaMnO3 exhibits ferromagnetism for film thicknesses exceeding 5 unit cells. This is discussed in terms of electronic reconstruction with polar charge transfer to the LaMnO3 side of the interface and also to the surface of the over layer. Novel magnetic coupling effects are seen in perovskite ferromagnets separated by a polar oxide layer such as LaAlO3 or NdGaO3, whereas non-polar oxides do not show the same effect. The coupling between the ferromagnetic layers oscillates in sign between FM and AFM, depending on the barrier thickness. Such coupling is totally unexpected in the absence of any itinerary electrons, with insulating barriers that are too thick for tunneling. The novel magnetic coupling is shown to be mediated by spin-orbit coupling and also magnetic excitation of defect levels in the polar oxide planes.
Van der Waals Epitaxy of Functional Oxide Heterostructures
NASA Astrophysics Data System (ADS)
Chu, Ying-Hao
In the diligent pursuit of low-power consumption, multifunctional, and environmentally friendly electronics, more sophisticated requirements on functional materials are on demand. Recently, the discovery of 2D layered materials has created a revolution to this field. Pioneered by graphene, these new 2D materials exhibit abundant unusual physical phenomena that is undiscovered in bulk forms. These materials are characterized with their layer form and almost pure 2D electronic behavior. The confinement of charge and heat transport at such ultrathin planes offers possibilities to overcome the bottleneck of present device development in thickness limitation, and thus push the technologies into next generation. Van der Waals epitaxy, an epitaxial growth method to combine 2D and 3D materials, is one of current reliable manufacturing processes to fabricate 2D materials by growing these 2D materials epitaxially on 3D materials. Then, transferring the 2D materials to the substrates for practical applications. In the mean time, van der Waals epitaxy has also been used to create free-standing 3D materials by growing 3D materials on 2D materials and then removing them from 2D materials since the interfacial boding between 2D and 3D materials should be weak van der Waals bonds. In this study, we intend to take the same concept, but to integrate a family of functional materials in order to open new avenue to flexible electronics. Due to the interplay of lattice, charge, orbital, and spin degrees of freedom, correlated electrons in oxides generate a rich spectrum of competing phases and physical properties. Recently, lots of studies have suggested that oxide heterostructures provide a powerful route to create and manipulate the degrees of freedom and offer new possibilities for next generation devices, thus create a new playground for researchers to investigate novel physics and the emergence of fascinating states of condensed matter. In this talk, we use a 2D layered material as the substrate. And we take several oxides as examples to demonstrate a pathway to integrate 3D functional oxides on 2D layered materials.
Transparent conducting oxides: A δ-doped superlattice approach
Cooper, Valentino R.; Seo, Sung S. Ambrose; Lee, Suyoun; Kim, Jun Sung; Choi, Woo Seok; Okamoto, Satoshi; Lee, Ho Nyung
2014-01-01
Metallic states appearing at interfaces between dissimilar insulating oxides exhibit intriguing phenomena such as superconductivity and magnetism. Despite tremendous progress in understanding their origins, very little is known about how to control the conduction pathways and the distribution of charge carriers. Using optical spectroscopic measurements and density-functional theory (DFT) simulations, we examine the effect of SrTiO3 (STO) spacer layer thickness on the optical transparency and carrier distribution in La δ-doped STO superlattices. We experimentally observe that these metallic superlattices remain highly transparent to visible light; a direct consequence of the appropriately large gap between the O 2p and Ti 3d states. In superlattices with relatively thin STO layers, we predict that three-dimensional conduction would occur due to appreciable overlap of quantum mechanical wavefunctions between neighboring δ-doped layers. These results highlight the potential for using oxide heterostructures in optoelectronic devices by providing a unique route for creating novel transparent conducting oxides. PMID:25109668
Schottky barrier at graphene/metal oxide interfaces: insight from first-principles calculations
NASA Astrophysics Data System (ADS)
Cheng, Kai; Han, Nannan; Su, Yan; Zhang, Junfeng; Zhao, Jijun
2017-02-01
Anode materials play an important role in determining the performance of lithium ion batteries. In experiment, graphene (GR)/metal oxide (MO) composites possess excellent electrochemical properties and are promising anode materials. Here we perform density functional theory calculations to explore the interfacial interaction between GR and MO. Our result reveals generally weak physical interactions between GR and several MOs (including Cu2O, NiO). The Schottky barrier height (SBH) in these metal/semiconductor heterostructures are computed using the macroscopically averaged electrostatic potential method, and the role of interfacial dipole is discussed. The calculated SBHs below 1 eV suggest low contact resistance; thus these GR/MO composites are favorable anode materials for better lithium ion batteries.
Schottky barrier at graphene/metal oxide interfaces: insight from first-principles calculations.
Cheng, Kai; Han, Nannan; Su, Yan; Zhang, Junfeng; Zhao, Jijun
2017-02-06
Anode materials play an important role in determining the performance of lithium ion batteries. In experiment, graphene (GR)/metal oxide (MO) composites possess excellent electrochemical properties and are promising anode materials. Here we perform density functional theory calculations to explore the interfacial interaction between GR and MO. Our result reveals generally weak physical interactions between GR and several MOs (including Cu2O, NiO). The Schottky barrier height (SBH) in these metal/semiconductor heterostructures are computed using the macroscopically averaged electrostatic potential method, and the role of interfacial dipole is discussed. The calculated SBHs below 1 eV suggest low contact resistance; thus these GR/MO composites are favorable anode materials for better lithium ion batteries.
NASA Astrophysics Data System (ADS)
Wu, Liangpeng; Yang, Xu; Huang, Yanqin; Li, Xinjun
2017-06-01
Titanium oxide nanotubes were prepared by hydrothermal treatment of TiO2 powder in NaOH aqueous solution and subsequently calcined. Titanium oxide nanotubes were further decorated by TiO2 nanoparticles through in situ hydrolysis of titanium isopropoxide containing alcohol and ammonia in an aqueous medium to form the composite catalyst (TNP/TiO2NTs). The morphology and structure of TNP/TiO2NTs were characterized by scanning and transmission electron microscopy, X-ray diffraction, UV-Vis, and Raman spectra. The separation efficiency of photo-excited carriers was investigated by photoluminescence technique and photoelectrochemical behavior. The photocatalytic activity was evaluated by the photocatalytic degradation of methyl orange. Due to the synergy effect caused by the interaction of titanium oxide nanotubes and TiO2 nanoparticles, the TNP/TiO2NTs composite shows efficient photogenerated carriers' separation and the increased light absorption. The photocatalytic activity was enhanced.
Magneto-ionic control of interfacial magnetism
NASA Astrophysics Data System (ADS)
Bauer, Uwe; Yao, Lide; Tan, Aik Jun; Agrawal, Parnika; Emori, Satoru; Tuller, Harry L.; van Dijken, Sebastiaan; Beach, Geoffrey S. D.
2015-02-01
In metal/oxide heterostructures, rich chemical, electronic, magnetic and mechanical properties can emerge from interfacial chemistry and structure. The possibility to dynamically control interface characteristics with an electric field paves the way towards voltage control of these properties in solid-state devices. Here, we show that electrical switching of the interfacial oxidation state allows for voltage control of magnetic properties to an extent never before achieved through conventional magneto-electric coupling mechanisms. We directly observe in situ voltage-driven O2- migration in a Co/metal-oxide bilayer, which we use to toggle the interfacial magnetic anisotropy energy by >0.75 erg cm-2 at just 2 V. We exploit the thermally activated nature of ion migration to markedly increase the switching efficiency and to demonstrate reversible patterning of magnetic properties through local activation of ionic migration. These results suggest a path towards voltage-programmable materials based on solid-state switching of interface oxygen chemistry.
Zhao, Lina; Lu, Zengxing; Zhang, Fengyuan; Tian, Guo; Song, Xiao; Li, Zhongwen; Huang, Kangrong; Zhang, Zhang; Qin, Minghui; SujuanWu; Lu, Xubing; Zeng, Min; Gao, Xingsen; Dai, Jiyan; Liu, Jun-Ming
2015-01-01
Ultrahigh density well-registered oxide nanocapacitors are very essential for large scale integrated microelectronic devices. We report the fabrication of well-ordered multiferroic BiFeO3 nanocapacitor arrays by a combination of pulsed laser deposition (PLD) method and anodic aluminum oxide (AAO) template method. The capacitor cells consist of BiFeO3/SrRuO3 (BFO/SRO) heterostructural nanodots on conductive Nb-doped SrTiO3 (Nb-STO) substrates with a lateral size of ~60 nm. These capacitors also show reversible polarization domain structures, and well-established piezoresponse hysteresis loops. Moreover, apparent current-rectification and resistive switching behaviors were identified in these nanocapacitor cells using conductive-AFM technique, which are attributed to the polarization modulated p-n junctions. These make it possible to utilize these nanocapacitors in high-density (>100 Gbit/inch2) nonvolatile memories and other oxide nanoelectronic devices. PMID:25853937
Photonic slab heterostructures based on opals
NASA Astrophysics Data System (ADS)
Palacios-Lidon, Elisa; Galisteo-Lopez, Juan F.; Juarez, Beatriz H.; Lopez, Cefe
2004-09-01
In this paper the fabrication of photonic slab heterostructures based on artificial opals is presented. The innovated method combines high-quality thin-films growing of opals and silica infiltration by Chemical Vapor Deposition through a multi-step process. By varying structure parameters, such as lattice constant, sample thickness or refractive index, different heterostructures have been obtained. The optical study of these systems, carried out by reflectance and transmittance measurements, shows that the prepared samples are of high quality further confirmed by Scanning Electron Microscopy micrographs. The proposed novel method for sample preparation allows a high control of the involved structure parameters, giving the possibility of tunning their photonic behavior. Special attention in the optical response of these materials has been addressed to the study of planar defects embedded in opals, due to their importance in different photonic fields and future technological applications. Reflectance and transmission measurements show a sharp resonance due to localized states associated with the presence of planar defects. A detailed study of the defect mode position and its dependance on defect thickness and on the surrounding photonic crystal is presented as well as evidence showing the scalability of the problem. Finally, it is also concluded that the proposed method is cheap and versatile allowing the preparation of opal-based complex structures.
Behura, Sanjay; Nguyen, Phong; Debbarma, Rousan; Che, Songwei; Seacrist, Michael R; Berry, Vikas
2017-05-23
Hexagonal boron nitride (h-BN) is an ideal platform for interfacing with two-dimensional (2D) nanomaterials to reduce carrier scattering for high-quality 2D electronics. However, scalable, transfer-free growth of hexagonal boron nitride (h-BN) remains a challenge. Currently, h-BN-based 2D heterostructures require exfoliation or chemical transfer of h-BN grown on metals resulting in small areas or significant interfacial impurities. Here, we demonstrate a surface-chemistry-influenced transfer-free growth of large-area, uniform, and smooth h-BN directly on silicon (Si)-based substrates, including Si, silicon nitride (Si 3 N 4 ), and silicon dioxide (SiO 2 ), via low-pressure chemical vapor deposition. The growth rates increase with substrate electronegativity, Si < Si 3 N 4 < SiO 2 , consistent with the adsorption rates calculated for the precursor molecules via atomistic molecular dynamics simulations. Under graphene with high grain density, this h-BN film acts as a polymer-free, planar-dielectric interface increasing carrier mobility by 3.5-fold attributed to reduced surface roughness and charged impurities. This single-step, chemical interaction guided, metal-free growth mechanism of h-BN for graphene heterostructures establishes a potential pathway for the design of complex and integrated 2D-heterostructured circuitry.
Lin, Yung-Chen; Kim, Dongheun; Li, Zhen; ...
2016-12-14
Here we report on strain-induced structural defect formation in core Si nanowire of Si/Ge core/shell nanowire heterostructure and influences of the structural defects on the electrochemical performances in lithium-ion battery anodes based on Si/Ge core/shell nanowire heterostructures. The induced structural defects consisting of stacking faults and dislocations in the core Si nanowire were observed for the first time. The generation of stacking faults in Si/Ge core/shell nanowire heterostructure is observed to prefer settling in either only Ge shell region or in both Ge shell and Si core regions and is associated with the increase of the shell volume fraction. Themore » relax of misfit strain in [112] oriented core/shell nanowire heterostructure leads to subsequent gliding of Shockley partial dislocations, preferentially forming the twins. The observation of cross-over defect formation is of great importance for the understanding of heteroepitaxy in radial heterostructures at nanoscale and building the three dimensional heterostructures for the various applications. In addition, the effect of the defect formation on nanomaterial’s functionality is investigated by electrochemical performance test. The Si/Ge core/shell nanowire heterostructures enhance the gravimetric capacity of lithium ion battery anodes under fast charging/discharging rates compared to Si nanowires. However, the induced structural defects hamper lithiation of the Si/Ge core/shell nanowire heterostructure.« less
DOE Office of Scientific and Technical Information (OSTI.GOV)
Lin, Yung-Chen; Kim, Dongheun; Li, Zhen
Here we report on strain-induced structural defect formation in core Si nanowire of Si/Ge core/shell nanowire heterostructure and influences of the structural defects on the electrochemical performances in lithium-ion battery anodes based on Si/Ge core/shell nanowire heterostructures. The induced structural defects consisting of stacking faults and dislocations in the core Si nanowire were observed for the first time. The generation of stacking faults in Si/Ge core/shell nanowire heterostructure is observed to prefer settling in either only Ge shell region or in both Ge shell and Si core regions and is associated with the increase of the shell volume fraction. Themore » relax of misfit strain in [112] oriented core/shell nanowire heterostructure leads to subsequent gliding of Shockley partial dislocations, preferentially forming the twins. The observation of cross-over defect formation is of great importance for the understanding of heteroepitaxy in radial heterostructures at nanoscale and building the three dimensional heterostructures for the various applications. In addition, the effect of the defect formation on nanomaterial’s functionality is investigated by electrochemical performance test. The Si/Ge core/shell nanowire heterostructures enhance the gravimetric capacity of lithium ion battery anodes under fast charging/discharging rates compared to Si nanowires. However, the induced structural defects hamper lithiation of the Si/Ge core/shell nanowire heterostructure.« less
Luo, Dong; Fang, Shaohua; Yang, Li; Hirano, Shin-Ichi
2017-12-22
Although Li-rich layered oxides (LLOs) have the highest capacity of any cathodes used, the rate capability of LLOs falls short of meeting the requirements of electric vehicles and smart grids. Herein, a layered-spinel microsphere/reduced graphene oxide heterostructured cathode (LS@rGO) is prepared in situ. This cathode is composed of a spinel phase, two layered structures, and a small amount of reduced graphene oxide (1.08 wt % of carbon). The assembly delivers a considerable charge capacity (145 mA h g -1 ) at an ultrahigh charge- discharge rate of 60 C (12 A g -1 ). The rate capability of LS@rGO is influenced by the introduced spinel phase and rGO. X-ray absorption and X-ray photoelectron spectroscopy data indicate that Cr ions move from octahedral lattice sites to tetrahedral lattice sites, and that Mn ions do not participate in the oxidation reaction during the initial charge process. © 2017 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.
NASA Astrophysics Data System (ADS)
Hu, Xue-Rong; Zheng, Ji-Ming; Ren, Zhao-Yu
2018-04-01
Based on first-principles calculations within the framework of density functional theory, we study the electronic properties of phosphorene/graphene heterostructures. Band gaps with different sizes are observed in the heterostructure, and charges transfer from graphene to phosphorene, causing the Fermi level of the heterostructure to shift downward with respect to the Dirac point of graphene. Significantly, strong coupling between two layers is discovered in the band spectrum even though it has a van der Waals heterostructure. A tight-binding Hamiltonian model is used to reveal that the resonance of the Bloch states between the phosphorene and graphene layers in certain K points combines with the symmetry matching between band states, which explains the reason for the strong coupling in such heterostructures. This work may enhance the understanding of interlayer interaction and composition mechanisms in van der Waals heterostructures consisting of two-dimensional layered nanomaterials, and may indicate potential reference information for nanoelectronic and optoelectronic applications.
Enhanced photoresponse characteristics of transistors using CVD-grown MoS2/WS2 heterostructures
NASA Astrophysics Data System (ADS)
Shan, Junjie; Li, Jinhua; Chu, Xueying; Xu, Mingze; Jin, Fangjun; Fang, Xuan; Wei, Zhipeng; Wang, Xiaohua
2018-06-01
Semiconductor heterostructures based on transition metal dichalcogenides provide a broad platform to research two-dimensional nanomaterials and design atomically thin devices for fundamental and applied interests. The MoS2/WS2 heterostructure was prepared on SiO2/Si substrate by chemical vapor deposition (CVD) in our research. And the optical properties of the heterostructure was characterized by Raman and photoluminescence (PL) spectroscopy. The similar 2 orders of magnitude decrease of PL intensity in MoS2/WS2 heterostructures was tested, which is attribute to the electrical and optical modulation effects are connected with the interfacial charge transfer between MoS2 and WS2 films. Using MoS2/WS2 heterostructure as channel material of the phototransistor, we demonstrated over 50 folds enhanced photoresponsivity of multilayer MoS2 field-effect transistor. The results indicate that the MoS2/WS2 films can be a promising heterostructure material to enhance the photoresponse characteristics of MoS2-based phototransistors.
Organic heterostructures deposited by MAPLE on AZO substrate
NASA Astrophysics Data System (ADS)
Socol, M.; Preda, N.; Stanculescu, A.; Breazu, C.; Florica, C.; Stanculescu, F.; Iftimie, S.; Girtan, M.; Popescu-Pelin, G.; Socol, G.
2017-09-01
Organic heterostructures based on poly(3-hexylthiophene) (P3HT) and fullerene (C60) as blends or multilayer were deposited on Al:ZnO (AZO) by Matrix-Assisted Pulsed Laser Evaporation (MAPLE) technique. The AZO layers were obtained by Pulsed Laser Deposition (PLD) on glass substrate, the high quality of the films being reflected by the calculated figure of merit. The organic heterostructures were investigated from morphological, optical and electrical point of view by atomic force microscopy (AFM), UV-vis spectroscopy, photoluminescence (PL) and current-voltage (I-V) measurements, respectively. The increase of the C60 content in the blend heterostructure has as result a high roughness. Compared with the multilayer heterostructure, those based on blends present an improvement in the electrical properties. Under illumination, the highest current value was recorded for the heterostructure based on the blend with the higher C60 amount. The obtained results showed that MAPLE is a useful technique for the deposition of the organic heterostructures on AZO as transparent conductor electrode.
NASA Astrophysics Data System (ADS)
Gao, Yuanda
Graphene has emerged as an appealing material for a variety of optoelectronic applications due to its unique electrical and optical characteristics. In this thesis, I will present recent advances in integrating graphene and graphene-boron nitride (BN) heterostructures with confined optical architectures, e.g. planar photonic crystal (PPC) nanocavities and silicon channel waveguides, to make this otherwise weakly absorbing material optically opaque. Based on these integrations, I will further demonstrate the resulting chip-integrated optoelectronic devices for optical interconnects. After transferring a layer of graphene onto PPC nanocavities, spectral selectivity at the resonance frequency and orders-of-magnitude enhancement of optical coupling with graphene have been observed in infrared spectrum. By applying electrostatic potential to graphene, electro-optic modulation of the cavity reflection is possible with contrast in excess of 10 dB. And furthermore, a novel and complex modulator device structure based on the cavity-coupled and BN-encapsulated dual-layer graphene capacitor is demonstrated to operate at a speed of 1.2 GHz. On the other hand, an enhanced broad-spectrum light-graphene interaction coupled with silicon channel waveguides is also demonstrated with ?0.1 dB/?m transmission attenuation due to graphene absorption. A waveguide-integrated graphene photodetector is fabricated and shown 0.1 A/W photoresponsivity and 20 GHz operation speed. An improved version of a similar photodetector using graphene-BN heterostructure exhibits 0.36 A/W photoresponsivity and 42 GHz response speed. The integration of graphene and graphene-BN heterostructures with nanophotonic architectures promises a new generation of compact, energy-efficient, high-speed optoelectronic device concepts for on-chip optical communications that are not yet feasible or very difficult to realize using traditional bulk semiconductors.
Light-matter interaction in transition metal dichalcogenides and their heterostructures
NASA Astrophysics Data System (ADS)
Wurstbauer, Ursula; Miller, Bastian; Parzinger, Eric; Holleitner, Alexander W.
2017-05-01
The investigation of two-dimensional (2D) van der Waals materials is a vibrant, fast-moving and still growing interdisciplinary area of research. These materials are truly 2D crystals with strong covalent in-plane bonds and weak van der Waals interaction between the layers, and have a variety of different electronic, optical and mechanical properties. Transition metal dichalcogenides are a very prominent class of 2D materials, particularly the semiconducting subclass. Their properties include bandgaps in the near-infrared to the visible range, decent charge carrier mobility together with high (photo-) catalytic and mechanical stability, and exotic many-body phenomena. These characteristics make the materials highly attractive for both fundamental research as well as innovative device applications. Furthermore, the materials exhibit a strong light-matter interaction, providing a high sunlight absorbance of up to 15% in the monolayer limit, strong scattering cross section in Raman experiments, and access to excitonic phenomena in van der Waals heterostructures. This review focuses on the light-matter interaction in MoS2, WS2, MoSe2 and WSe2, which is dictated by the materials’ complex dielectric functions, and on the multiplicity of studying the first-order phonon modes by Raman spectroscopy to gain access to several material properties such as doping, strain, defects and temperature. 2D materials provide an interesting platform for stacking them into van der Waals heterostructures without the limitation of lattice mismatch, resulting in novel devices for applications but also to enable the study of exotic many-body interaction phenomena such as interlayer excitons. Future perspectives of semiconducting transition metal dichalcogenides and their heterostructures for applications in optoelectronic devices will be examined, and routes to study emergent fundamental problems and many-body quantum phenomena under excitations with photons will be discussed.
Zhang, Dongzhi; Fan, Xin; Yang, Aijun; Zong, Xiaoqi
2018-08-01
In this paper, we fabricated a high-performance ethanol sensor using layer-by-layer self-assembled urchin-like alpha-iron oxide (α-Fe 2 O 3 ) hollow microspheres/molybdenum disulphide (MoS 2 ) nanosheets heterostructure as sensitive materials. The nanostructural, morphological, and compositional properties of the as-prepared α-Fe 2 O 3 /MoS 2 heterostructure were characterized by X-ray diffraction (XRD), energy dispersive spectrometer (EDS), scanning electron microscopy (SEM), transmission electron microscope (TEM) and X-ray photoelectron spectroscopy (XPS), which confirmed its successful preparation and rationality. The α-Fe 2 O 3 /MoS 2 nanocomposite sensor shows good selectivity, excellent reproducibility, fast response/recovery time and low detection limit towards ethanol gas at room temperature, which is superior to the single component of α-Fe 2 O 3 hollow microspheres and MoS 2 nanosheets. Furthermore, the response of the α-Fe 2 O 3 /MoS 2 nanocomposite sensor as a function of ethanol gas concentration was also demonstrated. The enhanced ethanol sensing properties of the α-Fe 2 O 3 /MoS 2 nanocomposite sensor were ascribed to the synergistic effect and heterojunction between the urchin-Like α-Fe 2 O 3 hollow microspheres and MoS 2 nanosheets. This work verifies that the hierarchical α-Fe 2 O 3 /MoS 2 nanoheterostructure is a potential candidate for fabricating room-temperature ethanol gas sensor. Copyright © 2018 Elsevier Inc. All rights reserved.
Positrons as interface-sensitive probes of polar semiconductor heterostructures
NASA Astrophysics Data System (ADS)
Makkonen, I.; Snicker, A.; Puska, M. J.; Mäki, J.-M.; Tuomisto, F.
2010-07-01
Group-III nitrides in their wurtzite crystal structure are characterized by large spontaneous polarization and significant piezoelectric contributions in heterostructures formed of these materials. Polarization discontinuities in polar heterostructures grown along the (0001) direction result in huge built-in electric fields on the order of megavolt per centimeter. We choose the III-nitride heterostructures as archetypal representatives of polar heterostructures formed of semiconducting or insulating materials and study the behavior of positrons in these structures using first-principles electronic-structure theory supported by positron annihilation experiments for bulk systems. The strong electric fields drive positrons close to interfaces, which is clearly seen in the predicted momentum distributions of annihilating electron-positron pairs as changes relative to the constituent bulk materials. Implications of the effect to positron defect studies of polar heterostructures are addressed.
Hlaing, Htay; Kim, Chang-Hyun; Carta, Fabio; Nam, Chang-Yong; Barton, Rob A; Petrone, Nicholas; Hone, James; Kymissis, Ioannis
2015-01-14
The vertical integration of graphene with inorganic semiconductors, oxide semiconductors, and newly emerging layered materials has recently been demonstrated as a promising route toward novel electronic and optoelectronic devices. Here, we report organic thin film transistors based on vertical heterojunctions of graphene and organic semiconductors. In these thin heterostructure devices, current modulation is accomplished by tuning of the injection barriers at the semiconductor/graphene interface with the application of a gate voltage. N-channel devices fabricated with a thin layer of C60 show a room temperature on/off ratio >10(4) and current density of up to 44 mAcm(-2). Because of the ultrashort channel intrinsic to the vertical structure, the device is fully operational at a driving voltage of 200 mV. A complementary p-channel device is also investigated, and a logic inverter based on two complementary transistors is demonstrated. The vertical integration of graphene with organic semiconductors via simple, scalable, and low-temperature fabrication processes opens up new opportunities to realize flexible, transparent organic electronic, and optoelectronic devices.
Electrical transport measurements of thin film samples under high hydrostatic pressure
NASA Astrophysics Data System (ADS)
Zabaleta, J.; Parks, S. C.; Baum, B.; Teker, A.; Syassen, K.; Mannhart, J.
2017-03-01
We present a method to perform electrical measurements of epitaxial films and heterostructures a few nanometers thick under high hydrostatic pressures in a diamond anvil cell (DAC). Hydrostatic pressure offers the possibility to tune the rich landscape of properties shown by epitaxial heterostructures, systems in which the combination of different materials, performed with atomic precision, can give rise to properties not present in their individual constituents. Measuring electrical conductivity under hydrostatic pressure in these systems requires a robust method that can address all the challenges: the preparation of the sample with side length and thickness that fits in the DAC setup, a contacting method compatible with liquid media, a gasket insulation that resists high forces, as well as an accurate procedure to place the sample in the pressure chamber. We prove the robustness of the method described by measuring the resistance of a two dimensional electron system buried at the interface between two insulating oxides under hydrostatic conditions up to ˜5 GPa. The setup remains intact until ˜10 GPa, where large pressure gradients affect the two dimensional conductivity.
Electrical transport measurements of thin film samples under high hydrostatic pressure.
Zabaleta, J; Parks, S C; Baum, B; Teker, A; Syassen, K; Mannhart, J
2017-03-01
We present a method to perform electrical measurements of epitaxial films and heterostructures a few nanometers thick under high hydrostatic pressures in a diamond anvil cell (DAC). Hydrostatic pressure offers the possibility to tune the rich landscape of properties shown by epitaxial heterostructures, systems in which the combination of different materials, performed with atomic precision, can give rise to properties not present in their individual constituents. Measuring electrical conductivity under hydrostatic pressure in these systems requires a robust method that can address all the challenges: the preparation of the sample with side length and thickness that fits in the DAC setup, a contacting method compatible with liquid media, a gasket insulation that resists high forces, as well as an accurate procedure to place the sample in the pressure chamber. We prove the robustness of the method described by measuring the resistance of a two dimensional electron system buried at the interface between two insulating oxides under hydrostatic conditions up to ∼5 GPa. The setup remains intact until ∼10 GPa, where large pressure gradients affect the two dimensional conductivity.
NASA Astrophysics Data System (ADS)
Shariati, M.; Ghafouri, V.
2014-05-01
Indium Oxide quasi one-dimensional (1D) nanostructures known as nanowires and nanorods synthesis using the thermal evaporation method, has been articulated. To nucleate growth sites, substrate seeding promoted 1D nanostructures growth. The catalyst-mediated growth mechanism showed more favorable morphologies and physical properties in under vacuum conditions associated with bottom-up technique. Scanning electron microscopy (SEM) results showed that the Zn-doped 1D nanostructures had spherical caps. The X-ray diffraction (XRD) pattern and energy-dispersive X-ray (EDX) spectrum indicated that these caps intensively associated with ZnO. Therefore, it was reasonable that the vapor-liquid-solid mechanism (VLS) was responsible for the growth of the In2O3-ZnO heterostructure nanowires. This technique enhances optical and electrical properties in nanostructures. The photoluminescence (PL) analysis in Zn-doped In2O3 nanowires and nanorods shows that the intensity of the visible and UV-region emissions overwhelmingly increases and resistance measurement professes the improvement of linear conductance in VLS growth mechanism.
Hu, Tao; Hong, Jisang
2015-10-28
Phosphorene is receiving great research interests because of its peculiar physical properties. Nonetheless, the phosphorus has a trouble of degradation due to oxidation. Hereby, we propose that the electrical and optical anisotropic properties can be preserved by encapsulating into hexagonal boron nitride (h-BN). We found that the h-BN contributed to enhancing the band gap of the phosphorene layer. Comparing the band gap of the pristine phosphorene layer, the band gap of the phosphorene/BN(1ML) system was enhanced by 0.15 eV. It was further enhanced by 0.31 eV in the BN(1ML)/phosphorene/BN(1ML) trilayer structure. However, the band gap was not further enhanced when we increased the thickness of the h-BN layers even up to 4 MLs. Interestingly, the anisotropic effective mass and optical property were still preserved in BN/phosphorene/BN heterostructures. Overall, we predict that the capping of phosphorene by the h-BN layers can be an excellent solution to protect the intrinsic properties of the phosphorene.
Review of - SiC wide-bandgap heterostructure properties as an alternate semiconductor material
NASA Astrophysics Data System (ADS)
Rajput Priti, J.; Patankar, Udayan S.; Koel, Ants; Nitnaware, V. N.
2018-05-01
Silicon substance (is also known as Quartz) is an abundant in nature and the electrical properties it exhibits, plays a vital role in developing its usage in the field of semiconductor. More than decades we can say that Silicon has shown desirable signs but at the later parts it has shown some research potential for development of alternative material as semiconductor devices. This need has come to light as we started scaling down in size of the Silicon material and up in speed. This semiconductor material started exhibiting several fundamental physical limits that include the minimum gate oxide thickness and the maximum saturation velocity of carriers which determines the operation frequency. Though the alternative semiconductors provide some answers (such as III-V's for high speed devices) for a path to skirt these problems, there also may be some ways to extend the life of silicon itself. Two paths are used as for alternative semiconductors i.e alternative gate dielectrics and silicon-based heterostructures. The SiC material has some strength properties under different conditions and find out the defects available in the material.
Integration of Multi-Functional Oxide Thin Film Heterostructures with III-V Semiconductors
NASA Astrophysics Data System (ADS)
Rahman, Md. Shafiqur
Integration of multi-functional oxide thin films with semiconductors has attracted considerable attention in recent years due to their potential applications in sensing and logic functionalities that can be incorporated in future system-on-a-chip devices. III-V semiconductor, for example, GaAs, have higher saturated electron velocity and mobility allowing transistors based on GaAs to operate at a much higher frequency with less noise compared to Si. In addition, because of its direct bandgap a number of efficient optical devices are possible and by oxide integrating with other III-V semiconductors the wavelengths can be made tunable through hetero-engineering of the bandgap. This study, based on the use of SrTiO3 (STO) films grown on GaAs (001) substrates by molecular beam epitaxy (MBE) as an intermediate buffer layer for the hetero-epitaxial growth of ferromagnetic La0.7Sr 0.3MnO3 (LSMO) and room temperature multiferroic BiFeO 3 (BFO) thin films and superlattice structures using pulsed laser deposition (PLD). The properties of the multilayer thin films in terms of growth modes, lattice spacing/strain, interface structures and texture were characterized by the in-situ reflection high energy electron diffraction (RHEED). The crystalline quality and chemical composition of the complex oxide heterostructures were investigated by a combination of X-ray diffraction (XRD) and X-ray photoelectron absorption spectroscopy (XPS). Surface morphology, piezo-response with domain structure, and ferroelectric switching observations were carried out on the thin film samples using a scanning probe microscope operated as a piezoresponse force microscopy (PFM) in the contact mode. The magnetization measurements with field cooling exhibit a surprising increment in magnetic moment with enhanced magnetic hysteresis squareness. This is the effect of exchange interaction between the antiferromagnetic BFO and the ferromagnetic LSMO at the interface. The integration of BFO materials with LSMO on GaAs substrate also facilitated the demonstration of resistive random access memory (ReRAM) devices which can be faster with lower energy consumption compared to present commercial technologies. Ferroelectric switching observations using piezoresponse force microscopy show polarization switching demonstrating its potential for read-write operation in NVM devices. The ferroelectric and electrical characterization exhibit strong resistive switching with low SET/RESET voltages. Furthermore, a prototypical epitaxial field effect transistor based on multiferroic BFO as the gate dielectric and ferromagnetic LSMO as the conducting channel was also demonstrated. The device exhibits a modulation in channel conductance with high ON/OFF ratio. The measured nanostructure and physical-compositional results from the multilayer are correlated with their corresponding dielectric, piezoelectric, and ferroelectric properties. These results provide an understanding of the heteroepitaxial growth of ferroelectric (FE)-antiferromagnetic (AFM) BFO on ferromagnetic LSMO as a simple thin film or superlattice structure, integrated on STO buffered GaAs (001) with full control over the interface structure at the atomic-scale. This work also represents the first step toward the realization of magnetoelectronic devices integrated with GaAs (001).
Shape Evolution of Highly Lattice-Mismatched InN/InGaN Nanowire Heterostructures
NASA Astrophysics Data System (ADS)
Yan, Lifan; Hazari, Arnab; Bhattacharya, Pallab; Millunchick, Joanna M.
2018-02-01
We have investigated the structure and shape of GaN-based nanowires grown on (001) Si substrates for optoelectronic device applications. The nanowire heterostructures contained InN disks and In0.4Ga0.6N barrier layers in the active region. The resulting nanowire array comprised two differently shaped nanowires: shorter pencil-like nanowires and longer bead-like nanowires. The two different nanowire shapes evolve due to a variation in the In incorporation rate, which was faster for the bead-like nanowires. Both types of nanowires exhibited evidence of significant migration of both Ga and In during growth. Ga tended to diffuse away and down along the sidewalls, resulting in a Ga-rich shell for all nanowires. Despite the complex structure and great variability in the In composition, the optical properties of the nanowire arrays were very good, with strong luminescence peaking at ˜ 1.63 μm.
DOE Office of Scientific and Technical Information (OSTI.GOV)
Lü, X.; Schrottke, L.; Grahn, H. T.
We present scattering rates for electrons at longitudinal optical phonons within a model completely formulated in the Fourier domain. The total intersubband scattering rates are obtained by averaging over the intrasubband electron distributions. The rates consist of the Fourier components of the electron wave functions and a contribution depending only on the intersubband energies and the intrasubband carrier distributions. The energy-dependent part can be reproduced by a rational function, which allows for the separation of the scattering rates into a dipole-like contribution, an overlap-like contribution, and a contribution which can be neglected for low and intermediate carrier densities of themore » initial subband. For a balance between accuracy and computation time, the number of Fourier components can be adjusted. This approach facilitates an efficient design of complex heterostructures with realistic, temperature- and carrier density-dependent rates.« less
The role of collective motion in the ultrafast charge transfer in van der Waals heterostructures
Wang, Han; Bang, Junhyeok; Sun, Yiyang; ...
2016-05-10
Here, the success of van der Waals (vdW) heterostructures, made of graphene, metal dichalcogenides, and other layered materials, hinges on the understanding of charge transfer across the interface as the foundation for new device concepts and applications. In contrast to conventional heterostructures, where a strong interfacial coupling is essential to charge transfer, recent experimental findings indicate that vdW heterostructues can exhibit ultra-fast charge transfer despite the weak binding of the heterostructure. Using time-dependent density functional theory molecular dynamics, we identify a strong dynamic coupling between the vdW layers associated with charge transfer. This dynamic coupling results in rapid nonlinear coherentmore » charge oscillations which constitute a purely electronic phenomenon and are shown to be a general feature of vdW heterostructures provided they have a critical minimum dipole coupling. Application to MoS2/WS2 heterostructure yields good agreement with experiment, indicating near complete charge transfer within a timescale of 100 fs.The success of van der Waals heterostructures made of graphene, metal dichalcogenides and other layered materials, hinges on the understanding of charge transfer across the interface as the foundation for new device concepts and applications. In contrast to conventional heterostructures, where a strong interfacial coupling is essential to charge transfer, recent experimental findings indicate that van der Waals heterostructues can exhibit ultrafast charge transfer despite the weak binding of these heterostructures. Here we find, using time-dependent density functional theory molecular dynamics, that the collective motion of excitons at the interface leads to plasma oscillations associated with optical excitation. By constructing a simple model of the van der Waals heterostructure, we show that there exists an unexpected criticality of the oscillations, yielding rapid charge transfer across the interface. Application to the MoS2/WS2 heterostructure yields good agreement with experiments, indicating near complete charge transfer within a timescale of 100 fs.« less
The role of collective motion in the ultrafast charge transfer in van der Waals heterostructures
DOE Office of Scientific and Technical Information (OSTI.GOV)
Wang, Han; Bang, Junhyeok; Sun, Yiyang
Here, the success of van der Waals (vdW) heterostructures, made of graphene, metal dichalcogenides, and other layered materials, hinges on the understanding of charge transfer across the interface as the foundation for new device concepts and applications. In contrast to conventional heterostructures, where a strong interfacial coupling is essential to charge transfer, recent experimental findings indicate that vdW heterostructues can exhibit ultra-fast charge transfer despite the weak binding of the heterostructure. Using time-dependent density functional theory molecular dynamics, we identify a strong dynamic coupling between the vdW layers associated with charge transfer. This dynamic coupling results in rapid nonlinear coherentmore » charge oscillations which constitute a purely electronic phenomenon and are shown to be a general feature of vdW heterostructures provided they have a critical minimum dipole coupling. Application to MoS2/WS2 heterostructure yields good agreement with experiment, indicating near complete charge transfer within a timescale of 100 fs.The success of van der Waals heterostructures made of graphene, metal dichalcogenides and other layered materials, hinges on the understanding of charge transfer across the interface as the foundation for new device concepts and applications. In contrast to conventional heterostructures, where a strong interfacial coupling is essential to charge transfer, recent experimental findings indicate that van der Waals heterostructues can exhibit ultrafast charge transfer despite the weak binding of these heterostructures. Here we find, using time-dependent density functional theory molecular dynamics, that the collective motion of excitons at the interface leads to plasma oscillations associated with optical excitation. By constructing a simple model of the van der Waals heterostructure, we show that there exists an unexpected criticality of the oscillations, yielding rapid charge transfer across the interface. Application to the MoS2/WS2 heterostructure yields good agreement with experiments, indicating near complete charge transfer within a timescale of 100 fs.« less
DOE Office of Scientific and Technical Information (OSTI.GOV)
Egorov, A. Yu., E-mail: anton@beam.ioffe.ru; Karachinsky, L. Ya.; Novikov, I. I.
It is demonstrated that metamorphic GaAs/InAlGaAs/InGaAs heterostructures with InAs/InGaAs quantum wells, which emit light in the 1250–1400 nm spectral range, can be fabricated by molecular-beam epitaxy. The structural and optical properties of the heterostructures are studied by X-ray diffraction analysis, transmission electron microscopy, and the photoluminescence method. Comparative analysis of the integrated photoluminescence intensity of the heterostructures and a reference sample confirm the high efficiency of radiative recombination in the heterostructures. It is confirmed by transmission electron microscopy that dislocations do not penetrate into the active region of the metamorphic heterostructures, where the radiative recombination of carriers occurs.
Lin, Yung-Chen; Bilgin, Ismail; Ahmed, Towfiq; ...
2016-09-21
Heterostructuring provides novel opportunities for exploring emergent phenomena and applications by developing designed properties beyond those of homogeneous materials. Advances in nanoscience enable the preparation of heterostructures formed incommensurate materials. Two-dimensional (2D) materials, such as graphene and transition metal dichalcogenides, are of particular interest due to their distinct physical characteristics. There have been recent changes in new research areas related to 2D/2D heterostructures. But, other heterostructures such as 2D/three-dimensional (3D) materials have not been thoroughly studied yet although the growth of 3D materials on 2D materials creating 2D/3D heterostructures with exceptional carrier transport properties has been reported. Here also wemore » report a novel heterostructure composed of Ge and monolayer MoS 2, prepared by chemical vapor deposition. A single crystalline Ge (110) thin film was grown on monolayer MoS 2. The electrical characteristics of Ge and MoS 2 in the Ge/MoS 2 heterostructure were remarkably different from those of isolated Ge and MoS 2. The field-effect conductivity type of the monolayer MoS 2 is converted from n-type to p-type by growth of the Ge thin film on top of it. Undoped Ge on MoS 2 is highly conducting. The observations can be explained by charge transfer in the heterostructure as opposed to chemical doping via the incorporation of impurities, based on our first-principles calculations.« less
Analysis of the auger recombination rate in P+N-n-N-N HgCdTe detectors for HOT applications
NASA Astrophysics Data System (ADS)
Schuster, J.; Tennant, W. E.; Bellotti, E.; Wijewarnasuriya, P. S.
2016-05-01
Infrared (IR) photon detectors must be cryogenically cooled to provide the highest possible performance, usually to temperatures at or below ~ 150K. Such low operating temperatures (Top) impose very stringent requirements on cryogenic coolers. As such, there is a constant push in the industry to engineer new detector architectures that operate at higher temperatures, so called higher operating temperature (HOT) detectors. The ultimate goal for HOT detectors is room temperature operation. While this is not currently possibly for photon detectors, significant increases in Top are nonetheless beneficial in terms of reduced size, weight, power and cost (SWAP-C). The most common HgCdTe IR detector architecture is the P+n heterostructure photodiode (where a capital letter indicates a wide band gap relative to the active layer or "AL"). A variant of this architecture, the P+N-n-N-N heterostructure photodiode, should have a near identical photo-response to the P+n heterostructure, but with significantly lower dark diffusion current. The P+N-n-N-N heterostructure utilizes a very low doped AL, surrounded on both sides by wide-gap layers. The low doping in the AL, allows the AL to be fully depleted, which drastically reduces the Auger recombination rate in that layer. Minimizing the Auger recombination rate reduces the intrinsic dark diffusion current, thereby increasing Top. Note when we use the term "recombination rate" for photodiodes, we are actually referring to the net generation and recombination of minority carriers (and corresponding dark currents) by the Auger process. For these benefits to be realized, these devices must be intrinsically limited and well passivated. The focus of this proceeding is on studying the fundamental physics of the intrinsic dark currents in ideal P+N-n-N-N heterostructures, namely Auger recombination. Due to the complexity of these devices, specifically the presence of multiple heterojunctions, numerical device modeling techniques must be utilized to predict and understand the device operation, as analytical models do not exist for heterojunction devices.
NASA Astrophysics Data System (ADS)
Li, Jiayu; Lin, Li; Huang, Guang-Yao; Kang, N.; Zhang, Jincan; Peng, Hailin; Liu, Zhongfan; Xu, H. Q.
2018-02-01
Graphene/hexagonal boron nitride (G/h-BN) heterostructures offer an excellent platform for developing nanoelectronic devices and for exploring correlated states in graphene under modulation by a periodic superlattice potential. Here, we report on transport measurements of nearly 0 ° -twisted G/h-BN heterostructures. The heterostructures investigated are prepared by dry transfer and thermally annealing processes and are in the low mobility regime (approximately 3000 cm2 V-1 s-1 at 1.9 K). The replica Dirac spectra and Hofstadter butterfly spectra are observed on the hole transport side, but not on the electron transport side, of the heterostructures. We associate the observed electron-hole asymmetry with the presence of a large difference between the opened gaps in the conduction and valence bands and a strong enhancement in the interband contribution to the conductivity on the electron transport side in the low-mobility G/h-BN heterostructures. We also show that the gaps opened at the central Dirac point and the hole-branch secondary Dirac point are large, suggesting the presence of strong graphene-substrate interaction and electron-electron interaction in our G/h-BN heterostructures. Our results provide additional helpful insight into the transport mechanism in G/h-BN heterostructures.
Photon-induced thermoelectric voltages in complex oxide superlattices
NASA Astrophysics Data System (ADS)
Habermeier, Hanns-Ulrich; Heinze, Stefan
2014-03-01
Heterostructures composed of transition metal oxides with strong electron correlation offer a unique opportunity to design new artificial materials whose electrical, magnetic and optical properties can be manipulated by tailoring the occupation of the 3d-orbitals of the transition metal in the compound. This possibility is an implication of symmetry constraints at interfaces resulting in a delicate interplay of spin-, charge-, orbital and lattice interactions of electrons. In turn, the material properties are sensitive to external perturbations such as strain, electrical and magnetic fields and photon flux as well. In this contribution we use photon flux exposure to explore the consequences of superlattice formation of YBa2Cu3O7-δ/La 2/3Ca1/3MnO3 on the entropy transport, especially on the Seebeck coefficient. In addition to the investigation of the fundamental aspects of entropy transport in oxide superlattices, the driving force for this work is the development of optical sensing devices. The method applied is based on the off-diagonal thermoelectric effect (ODTE) appearing in films deposited on substrates with a vicinal cut. This well-known principle serves as a technique to investigate the anisotropic transport properties and the components of the Seebeck tensor in these superlattices. It could be shown that the normalized ODTE signals scale linearly with the number of interfaces in the structures. We observed an enhancement of the ODTE signals by a factor of four due to superlattice formation. The results are discussed with respect to cross-plane coherent backscattering of phonon waves at the superlattice interfaces and the thermal boundary resistance at the YBa2Cu3O7-δ/La2/3Ca1/3MnO3 interfaces.
Graphene/blue-phosphorus heterostructure as potential anode materials for sodium-ion batteries
NASA Astrophysics Data System (ADS)
Fan, Kaimin; Tang, Ting; Wu, Shiyun; Zhang, Zhiyuan
2018-01-01
The first-principles calculations based on density functional theory (DFT) have been implemented to investigate the graphene/blue-phosphorus (G/BP) heterostructure as potential anode material for SIBs. The adsorption and diffusion behaviors of sodium (Na) in G/BP heterostructure and the effect of external electric field on Na adsorption have been investigated. The results indicate that G/BP heterostructure with Na adsorption is metallic due to Na incorporation, which is of benefit for electronic conductivity as anode material. The results show that the design of G/BP heterostructure is an efficient scheme to enhance the Na adsorption in G/BP without affecting the high mobility of Na in the G/BP heterostructure surface. The present work demonstrates that the external electric field can effectively modulate the adsorption of Na, and the adsorption behavior of Na is more sensitive to the external electric field when E > 0.10 V Å-1 in G/BP heterostructure. The Mulliken population analysis and DOS calculations have been performed to explore the charge transfer and the interaction between Na and G/BP.
Yu, Yifei; Hu, Shi; Su, Liqin; ...
2014-12-03
Semiconductor heterostructurs provide a powerful platform for the engineering of excitons. Here we report on the excitonic properties of two-dimensional (2D) heterostructures that consist of monolayer MoS2 and WS2 stacked epitaxially or non-epitaxially in the vertical direction. We find similarly efficient interlayer relaxation and transition of excitons in both the epitaxial and non-epitaxial heterostructures. This is manifested by a two orders of magnitude decrease in the photoluminescence and an extra absorption peak at low energy region of both heterostructures. The MoS2/WS2 heterostructures show weak interlayer coupling and essentially act as an atomic-scale heterojunction with the intrinsic band structures of themore » two monolayers largely preserved. They are particularly promising for the applications that request efficient dissociation of excitons and strong light absorption, including photovoltaics, solar fuels, photodetectors, and optical modulators. Our results also indicate that 2D heterostructures promise to provide capabilities to engineer excitons from the atomic level without concerns of interfacial imperfection.« less
Lee, Gooyong; Ibrahim, Shaliza; Kittappa, Shanmuga; Park, Heekyung; Park, Chang Min
2018-06-01
Novel heterostructured β-Bi 2 O 3 /Bi 2 O 2 CO 3 nanoplates (hBN) were synthesized to observe the sonocatalytic degradation of bisphenol A (BPA) (widely used as a model pollutant) under ultrasonic (US) irradiation. Prior to obtaining the hBN, the Bi 2 O 2 CO 3 micropowder precursor was prepared under hydrothermal conditions and then converted to hBN by increasing the calcination temperature to 300 °C. The synthesized hBN samples were characterized by field emission scanning electron microscope with energy dispersive X-ray analysis (FESEM/EDX), transmission electron microscopy (TEM), X-ray diffraction (XRD), ultraviolet-visible spectrophotometer diffuse reflection spectroscopy (UV-vis DRS), and X-ray photoelectron spectroscopy (XPS). The hBN/US system exhibited greater sonocatalytic activity for the degradation of BPA than the US treatment with the single element bismuth oxide, β-Bi 2 O 3 prepared by annealing the Bi 2 O 2 CO 3 precursor at 400 °C for 1 h. The US frequency and US power intensity in the hBN/US system were the key operating parameters, which were responsible for the complete degradation of BPA during 6 h of reactions. The degradation efficiency of BPA under the US irradiation was positively correlated with the dose of hBN. Our findings indicate that heterostructured hBN can be used as an efficient sonocatalyst for the catalytic degradation of BPA in water and wastewater treatment. Copyright © 2018 Elsevier B.V. All rights reserved.
NASA Astrophysics Data System (ADS)
Mostovyi, Andrii I.; Solovan, Mykhailo M.; Brus, Viktor V.; Pullerits, Toǧnu; Maryanchuk, Pavlo D.
2018-01-01
MoOx/n-CdTe photosensitive heterostructures were prepared by the deposition of molybdenum oxide thin films onto three different n-type CdTe substrates (ρ1=0.4 Ωṡcm, ρ2=10 Ωṡcm, ρ3=40 Ωṡcm) by DC reactive magnetron sputtering. The height of the potential barrier and series resistance of the MoOx/CdTe heterojunctions were investigated. The dominating current transport mechanisms through the heterojunctions were determined at forward and reverse biases.
NASA Astrophysics Data System (ADS)
Phillips, Patrick J.; Rui, Xue; Georgescu, Alexandru B.; Disa, Ankit S.; Longo, Paolo; Okunishi, Eiji; Walker, Fred; Ahn, Charles H.; Ismail-Beigi, Sohrab; Klie, Robert F.
2017-05-01
Epitaxial strain, layer confinement, and inversion symmetry breaking have emerged as powerful new approaches to control the electronic and atomic-scale structural properties of complex metal oxides. Trivalent rare-earth (RE) nickelate R E NiO3 heterostructures have been shown to be exemplars since the orbital occupancy, degeneracy, and, consequently, electronic/magnetic properties can be altered as a function of epitaxial strain, layer thickness, and superlattice structure. One recent example is the tricomponent LaTiO3-LaNiO3-LaAlO3 superlattice which exhibits charge transfer and orbital polarization as the result of its interfacial dipole electric field. A crucial step towards control of these parameters for future electronic and magnetic device applications is to develop an understanding of both the magnitude and range of the octahedral network's response towards interfacial strain and electric fields. An approach that provides atomic-scale resolution and sensitivity towards the local octahedral distortions and orbital occupancy is therefore required. Here, we employ atomic-resolution imaging coupled with electron spectroscopies and first-principles theory to examine the role of interfacial charge transfer and symmetry breaking in a tricomponent nickelate superlattice system. We find that nearly complete charge transfer occurs between the LaTiO3 and LaNiO3 layers, resulting in a mixed Ni2 +/Ni3 + valence state. We further demonstrate that this charge transfer is highly localized with a range of about 1 unit cell within the LaNiO3 layers. We also show how Wannier-function-based electron counting provides a simple physical picture of the electron distribution that connects directly with formal valence charges. The results presented here provide important feedback to synthesis efforts aimed at stabilizing new electronic phases that are not accessible by conventional bulk or epitaxial film approaches.
NASA Astrophysics Data System (ADS)
Qiao, Jia-Bin; Gong, Yue; Zuo, Wei-Jie; Wei, Yi-Cong; Ma, Dong-Lin; Yang, Hong; Yang, Ning; Qiao, Kai-Yao; Shi, Jin-An; Gu, Lin; He, Lin
2017-05-01
Assembling different two-dimensional (2D) crystals, covering a very broad range of properties, into van der Waals (vdW) heterostructures enables unprecedented possibilities for combining the best of different ingredients in one objective material. So far, metallic, semiconducting, and insulating 2D crystals have been used successfully in making functional vdW heterostructures with properties by design. Here, we expand 2D superconducting crystals as a building block of vdW hererostructures. One-step growth of large-scale high-quality vdW heterostructures of graphene and 2D superconducting α -M o2C by using chemical vapor deposition is reported. The superconductivity and its 2D nature of the heterostructures are characterized by our scanning tunneling microscopy measurements. This adds 2D superconductivity, the most attractive property of condensed matter physics, to vdW heterostructures.
Xie, Ying Peng; Yang, Yongqiang; Wang, Guosheng; Liu, Gang
2017-10-01
The solid-state Z-scheme trinary/binary heterostructures show the advantage of utilizing the high-energy photogenerated charge carriers in photocatalysis. However, the key factors controlling such Z-scheme in the binary heterostructures are still unclear. In this paper, we showed that oxygen vacancies could act as an interface electron transfer mediator to promote the direct Z-scheme charge transfer process in binary semiconductor heterostructures of CdS/ZnS. Increasing the concentration of surface oxygen vacancies of ZnO crystal can greatly enhance photocatalytic hydrogen generation of CdS/ZnO heterostructure. This was attributed to the strengthened direct Z-scheme charge transfer process in CdS/ZnO, as evidenced by steady-state/time-resolved photoluminescence spectroscopy and selective photodeposition of metal particles on the heterostructure. Copyright © 2017 Elsevier Inc. All rights reserved.
Myoung, Nojoon; Park, Hee Chul; Lee, Seung Joo
2016-01-01
Controlling tunneling properties through graphene vertical heterostructures provides advantages in achieving large conductance modulation which has been known as limitation in lateral graphene device structures. Despite of intensive research on graphene vertical heterosturctures for recent years, the potential of spintronics based on graphene vertical heterostructures remains relatively unexplored. Here, we present an analytical device model for graphene-based spintronics by using ferromagnetic graphene in vertical heterostructures. We consider a normal or ferroelectric insulator as a tunneling layer. The device concept yields a way of controlling spin transport through the vertical heterostructures, resulting in gate-tunable spin-switching phenomena. Also, we revealed that a ‘giant’ resistance emerges through a ferroelectric insulating layer owing to the anti-parallel configuration of ferromagnetic graphene layers by means of electric fields via gate and bias voltages. Our findings discover the prospect of manipulating the spin transport properties in vertical heterostructures without use of magnetic fields. PMID:27126101
Wang, Pengtang; Zhang, Xu; Zhang, Jin; Wan, Sheng; Guo, Shaojun; Lu, Gang; Yao, Jianlin; Huang, Xiaoqing
2017-01-01
Comprising abundant interfaces, multicomponent heterostructures can integrate distinct building blocks into single entities and yield exceptional functionalities enabled by the synergistic components. Here we report an efficient approach to construct one-dimensional metal/sulfide heterostructures by directly sulfuring highly composition-segregated platinum-nickel nanowires. The heterostructures possess a high density of interfaces between platinum-nickel and nickel sulfide components, which cooperate synergistically towards alkaline hydrogen evolution reaction. The platinum-nickel/nickel sulfide heterostructures can deliver a current density of 37.2 mA cm−2 at an overpotential of 70 mV, which is 9.7 times higher than that of commercial Pt/C. The heterostructures also offer enhanced stability revealed by long-term chronopotentiometry measurements. The present work highlights a potentially powerful interface-engineering strategy for designing multicomponent heterostructures with advanced performance in hydrogen evolution reaction and beyond. PMID:28239145
Electronic transport and photovoltaic properties in Bi2Sr2Co2Oyepitaxial heterostructures
NASA Astrophysics Data System (ADS)
Guo, Hai-Zhong; Gu, Lin; Yang, Zhen-Zhong; Wang, Shu-Fang; Fu, Guang-Sheng; Wang, Le; Jin, Kui-Juan; Lu, Hui-Bin; Wang, Can; Ge, Chen; He, Meng; Yang, Guo-Zhen
2013-08-01
Epitaxial heterostructures constructed from the thermoelectric cobalt Bi2Sr2Co2Oy thin films and SrTiO3 as well as SrTi0.993Nb0.007O3 substrates were fabricated by pulsed-laser deposition. The scanning transmission electron microscopy results confirm that the heterostructures are epitaxial, with sharp and coherent interfaces. The temperature-dependent electrical transport properties and the Hall effects were systematically investigated. The Bi2Sr2Co2Oy/SrTi0.993Nb0.007O3 p-n heterostructure exhibits good rectifying current-voltage characteristics over a wide temperature range. A strong photovoltaic effect was observed in the Bi2Sr2Co2Oy/SrTi0.993Nb0.007O3 heterostructure, with the temperature-dependent photovoltage being systematically investigated. The present work shows a great potential of this new heterostructures as photoelectric devices.
Wu, Kaifeng; Song, Nianhui; Liu, Zheng; Zhu, Haiming; Rodríguez-Córdoba, William; Lian, Tianquan
2013-08-15
Recent studies of group II-VI colloidal semiconductor heterostuctures, such as CdSe/CdS core/shell quantum dots (QDs) or dot-in-rod nanorods, show that type II and quasi-type II band alignment can facilitate electron transfer and slow down charge recombination in QD-molecular electron acceptor complexes. To explore the general applicability of this wave function engineering approach for controlling charge transfer properties, we investigate exciton relaxation and dissociation dynamics in InP (a group III-V semiconductor) and InP/CdS core/shell (a heterostructure beween group III-V and II-VI semiconductors) QDs by transient absorption spectroscopy. We show that InP/CdS QDs exhibit a quasi-type II band alignment with the 1S electron delocalized throughout the core and shell and the 1S hole confined in the InP core. In InP-methylviologen (MV(2+)) complexes, excitons in the QD can be dissociated by ultrafast electron transfer to MV(2+) from the 1S electron level (with an average time constant of 11.4 ps) as well as 1P and higher electron levels (with a time constant of 0.39 ps), which is followed by charge recombination to regenerate the complex in its ground state (with an average time constant of 47.1 ns). In comparison, InP/CdS-MV(2+) complexes show similar ultrafast charge separation and 5-fold slower charge recombination rates, consistent with the quasi-type II band alignment in these heterostructures. This result demonstrates that wave function engineering in nanoheterostructures of group III-V and II-VI semiconductors provides a promising approach for optimizing their light harvesting and charge separation for solar energy conversion applications.
NASA Astrophysics Data System (ADS)
Santana, Juan A.; Krogel, Jaron T.; Kent, Paul R.; Reboredo, Fernando
Materials based on transition metal oxides (TMO's) are among the most challenging systems for computational characterization. Reliable and practical computations are possible by directly solving the many-body problem for TMO's with quantum Monte Carlo (QMC) methods. These methods are very computationally intensive, but recent developments in algorithms and computational infrastructures have enabled their application to real materials. We will show our efforts on the application of the diffusion quantum Monte Carlo (DMC) method to study the formation of defects in binary and ternary TMO and heterostructures of TMO. We will also outline current limitations in hardware and algorithms. This work is supported by the Materials Sciences & Engineering Division of the Office of Basic Energy Sciences, U.S. Department of Energy (DOE).
Charge carrier transfer in tungsten disulfide—black phosphorus heterostructures
NASA Astrophysics Data System (ADS)
Zhao, Siqi; He, Dawei; Wang, Yongsheng; Zhang, Xinwu; He, Jiaqi
2017-11-01
Photocarrier dynamics in tungsten disulfide—black phosphorus (BP) heterostructures were studied by time-resolved differential reflection measurements. The heterostructures were fabricated by stacking together monolayer WS2 and BP flakes that are both fabricated by mechanical exfoliation. Efficient and ultrafast transfer of photocarriers from WS2 to BP flakes was observed. This confirms the type-I band alignment of WS2/BP heterostructures that was predicted by theory. Accompanied with the photocarrier interlayer transfer process from WS2 to BP flakes, the change of the absorption of WS2 persists for several nanoseconds. These results promote the consciousness about the carrier dynamics of interlayer transfer process in van der Waals heterostructures and its application in optoelectronic devices.
Impurity-induced states in superconducting heterostructures
NASA Astrophysics Data System (ADS)
Liu, Dong E.; Rossi, Enrico; Lutchyn, Roman M.
2018-04-01
Heterostructures allow the realization of electronic states that are difficult to obtain in isolated uniform systems. Exemplary is the case of quasi-one-dimensional heterostructures formed by a superconductor and a semiconductor with spin-orbit coupling in which Majorana zero-energy modes can be realized. We study the effect of a single impurity on the energy spectrum of superconducting heterostructures. We find that the coupling between the superconductor and the semiconductor can strongly affect the impurity-induced states and may induce additional subgap bound states that are not present in isolated uniform superconductors. For the case of quasi-one-dimensional superconductor/semiconductor heterostructures we obtain the conditions for which the low-energy impurity-induced bound states appear.