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Sample records for cdse colloidal quantum

  1. Colloidal CdSe Quantum Rings.

    PubMed

    Fedin, Igor; Talapin, Dmitri V

    2016-08-10

    Semiconductor quantum rings are of great fundamental interest because their non-trivial topology creates novel physical properties. At the same time, toroidal topology is difficult to achieve for colloidal nanocrystals and epitaxially grown semiconductor nanostructures. In this work, we introduce the synthesis of luminescent colloidal CdSe nanorings and nanostructures with double and triple toroidal topology. The nanorings form during controlled etching and rearrangement of two-dimensional nanoplatelets. We discuss a possible mechanism of the transformation of nanoplatelets into nanorings and potential utility of colloidal nanorings for magneto-optical (e.g., Aharonov-Bohm effect) and other applications.

  2. Selenium Redox Reactivity on Colloidal CdSe Quantum Dot Surfaces

    PubMed Central

    2016-01-01

    Understanding the structural and compositional origins of midgap states in semiconductor nanocrystals is a longstanding challenge in nanoscience. Here, we report a broad variety of reagents useful for photochemical reduction of colloidal CdSe quantum dots, and we establish that these reactions proceed via a dark surface prereduction step prior to photoexcitation. Mechanistic studies relying on the specific properties of various reductants lead to the proposal that this surface prereduction occurs at oxidized surface selenium sites. These results demonstrate the use of small-molecule inorganic chemistries to control the physical properties of colloidal QDs and provide microscopic insights into the identities and reactivities of their localized surface species. PMID:27518320

  3. Selenium Redox Reactivity on Colloidal CdSe Quantum Dot Surfaces.

    PubMed

    Tsui, Emily Y; Hartstein, Kimberly H; Gamelin, Daniel R

    2016-09-01

    Understanding the structural and compositional origins of midgap states in semiconductor nanocrystals is a longstanding challenge in nanoscience. Here, we report a broad variety of reagents useful for photochemical reduction of colloidal CdSe quantum dots, and we establish that these reactions proceed via a dark surface prereduction step prior to photoexcitation. Mechanistic studies relying on the specific properties of various reductants lead to the proposal that this surface prereduction occurs at oxidized surface selenium sites. These results demonstrate the use of small-molecule inorganic chemistries to control the physical properties of colloidal QDs and provide microscopic insights into the identities and reactivities of their localized surface species. PMID:27518320

  4. Photon echo studies of biexcitons and coherences in colloidal CdSe quantum dots

    NASA Astrophysics Data System (ADS)

    Colonna, Anne E.; Yang, Xiujuan; Scholes, Gregory D.

    2005-04-01

    The cover picture shows the size-dependent photoluminescence from CdSe colloidal quantum dots that were investigated in the work [1]. Ultrafast photon echo experiments were undertaken in conjunction with simulations based on a realistic many-body theory, shown in the picture, to ascertain the significance of many-body contributions to the third-order nonlinear response.The first author Anne E. Colonna undertook this research during a summer internship in the Department of Chemistry, University of Toronto. She is currently pursuing graduate studies at École Polytechnique, Saclay, in the Laboratoire d'Optique et Biosciences.The author Gregory D. Scholes is an Assistant Professor in the Department of Chemistry, University of Toronto. His research interests include synthesis and shape control of quantum dots, as well as the application of ultrafast laser spectroscopy to investigate the electronic structure of inorganic and organic semiconductors.

  5. Measuring photoluminescence spectra of self-assembly array nanowire of colloidal CdSe quantum dots using scanning near-field optics microscopy

    NASA Astrophysics Data System (ADS)

    Bai, Zhongchen; Hao, Licai; Zhang, Zhengping; Qin, Shuijie

    2016-05-01

    A novel periodic array CdSe nanowire is prepared on a substrate of the porous titanium dioxide by using a self-assembly method of the colloidal CdSe quantum dots (QDs). The experimental results show that the colloidal CdSe QDs have renewedly assembled on its space scale and direction in process of losing background solvent and form the periodic array nanowire. The main peak wavelength of Photoluminescence (PL) spectra, which is measured by using a 100-nm aperture laser beam spot on a scanning near-field optics microscopy, has shifted 60 nm with compared to the colloidal CdSe QDs. Furthermore, we have measured smaller ordered nanometer structure in thin QDs area as well, a 343-nm periodic nanowire in thick QDs area and the colloidal QDs in edge of well-ordered nanowire.

  6. A mirage study of CdSe colloidal quantum dot films, Urbach tail, and surface states.

    PubMed

    Guyot-Sionnest, Philippe; Lhuillier, Emmanuel; Liu, Heng

    2012-10-21

    Thermal deflection spectroscopy allows to measure very small absorption and uncovers absorption tails extending well below the bulk bandgap energy for CdSe quantum dots films after ligand exchange by sulfide. In this monodispersed system, the redshift, the broadening, and the absorption tails cannot be solely attributed to electronic coupling between the dots. Instead, mixing of hole states from the quantum dot and surface is proposed to dominate the changes of the interband spectra at the absorption edge. PMID:23083181

  7. A mirage study of CdSe colloidal quantum dot films, Urbach tail, and surface states

    NASA Astrophysics Data System (ADS)

    Guyot-Sionnest, Philippe; Lhuillier, Emmanuel; Liu, Heng

    2012-10-01

    Thermal deflection spectroscopy allows to measure very small absorption and uncovers absorption tails extending well below the bulk bandgap energy for CdSe quantum dots films after ligand exchange by sulfide. In this monodispersed system, the redshift, the broadening, and the absorption tails cannot be solely attributed to electronic coupling between the dots. Instead, mixing of hole states from the quantum dot and surface is proposed to dominate the changes of the interband spectra at the absorption edge.

  8. Dipolar structures in colloidal dispersions of PbSe and CdSe quantum dots.

    PubMed

    Klokkenburg, Mark; Houtepen, Arjan J; Koole, Rolf; de Folter, Julius W J; Erné, Ben H; van Faassen, Ernst; Vanmaekelbergh, Daniël

    2007-09-01

    We show by cryogenic transmission electron microscopy that PbSe and CdSe nanocrystals of various shapes in a liquid colloidal dispersion self-assemble into equilibrium structures that have a pronounced dipolar character, to an extent that depends on particle concentration and size. Analyzing the cluster-size distributions with a one-dimensional (1D) aggregation model yields a dipolar pair attraction of 8-10 kBT at room temperature. This accounts for the long-range alignment of the crystal planes of individual nanocrystals in self-assembled superstructures and for anisotropic nanostructures grown via oriented attachment. PMID:17713960

  9. Direct Observation of sp-d Exchange Interactions in Colloidal Mn2+- and Co2+-Doped CdSe Quantum Dots

    SciTech Connect

    Archer, Paul I.; Santangelo, Steven A.; Gamelin, Daniel R.

    2007-03-23

    The defining attribute of a diluted magnetic semiconductor (DMS) is the existence of dopant-carrier magnetic exchange interactions. In this letter, we report the first direct observation of such exchange interactions in colloidal doped CdSe nanocrystals. Doped CdSe quantum dots were synthesized by thermal decomposition of (Me4N)2[Cd4(SePh)10] in the presence of TMCl2 (TM2+ ) Mn2+ or Co2+) in hexadecylamine and were characterized by several analytical and spectroscopic techniques. Using magnetic circular dichroism spectroscopy, successful doping and the existence of giant excitonic Zeeman splittings in both Mn2+- and Co2+-doped wurtzite CdSe quantum dots are demonstrated unambiguously.

  10. Two-photon absorption in CdSe colloidal quantum dots compared to organic molecules.

    PubMed

    Makarov, Nikolay S; Lau, Pick Chung; Olson, Christopher; Velizhanin, Kirill A; Solntsev, Kyril M; Kieu, Khanh; Kilina, Svetlana; Tretiak, Sergei; Norwood, Robert A; Peyghambarian, Nasser; Perry, Joseph W

    2014-12-23

    We discuss fundamental differences in electronic structure as reflected in one- and two-photon absorption spectra of semiconductor quantum dots and organic molecules by performing systematic experimental and theoretical studies of the size-dependent spectra of colloidal quantum dots. Quantum-chemical and effective-mass calculations are used to model the one- and two-photon absorption spectra and compare them with the experimental results. Currently, quantum-chemical calculations are limited to only small-sized quantum dots (nanoclusters) but allow one to study various environmental effects on the optical spectra such as solvation and various surface functionalizations. The effective-mass calculations, on the other hand, are applicable to the larger-sized quantum dots and can, in general, explain the observed trends but are insensitive to solvent and ligand effects. Careful comparison of the experimental and theoretical results allows for quantifying the range of applicability of theoretical methods used in this work. Our study shows that the small clusters can be in principle described in a manner similar to that used for organic molecules. In addition, there are several important factors (quality of passivation, nature of the ligands, and intraband/interband transitions) affecting optical properties of the nanoclusters. The larger-size quantum dots, on the other hand, behave similarly to bulk semiconductors, and can be well described in terms of the effective-mass models. PMID:25427158

  11. Nonlinear optical switching and optical limiting in colloidal CdSe quantum dots investigated by nanosecond Z-scan measurement

    NASA Astrophysics Data System (ADS)

    Valligatla, Sreeramulu; Haldar, Krishna Kanta; Patra, Amitava; Desai, Narayana Rao

    2016-10-01

    The semiconductor nanocrystals are found to be promising class of third order nonlinear optical materials because of quantum confinement effects. Here, we highlight the nonlinear optical switching and optical limiting of cadmium selenide (CdSe) quantum dots (QDs) using nanosecond Z-scan measurement. The intensity dependent nonlinear absorption and nonlinear refraction of CdSe QDs were investigated by applying the Z-scan technique with 532 nm, nanosecond laser pulses. At lower intensities, the nonlinear process is dominated by saturable absorption (SA) and it is changed to reverse saturable absorption (RSA) at higher intensities. The SA behaviour is attributed to the ground state bleaching and the RSA is ascribed to free carrier absorption (FCA) of CdSe QDs. The nonlinear optical switching behaviour and reverse saturable absorption makes CdSe QDs are good candidate for all-optical device and optical limiting applications.

  12. Enhancement of emission efficiency of colloidal CdSe quantum dots on silicon substrate via an ultra-thin layer of aluminum oxide.

    PubMed

    Patty, K; Sadeghi, S M; Nejat, A; Mao, C-B

    2014-04-18

    We demonstrate that an ultra-thin layer of aluminum oxide can significantly enhance the emission efficiency of colloidal quantum dots on a Si substrate. For an ensemble of single quantum dots, our results show that this super brightening process can increase the fluorescence of CdSe quantum dots, forming well-resolved spectra, while in the absence of this layer the emission remains mostly at the noise level. We demonstrate that this process can be further enhanced with irradiation of the quantum dots, suggesting a significant photo-induced fluorescence enhancement via considerable suppression of non-radiative decay channels of the quantum dots. We study the impact of the Al oxide thickness on Si and interdot interactions, and discuss the results in terms of photo-induced catalytic properties of the Al oxide and the effects of such an oxide on the Coulomb blockade responsible for suppression of photo-ionization of the quantum dots.

  13. Elimination of deep surface traps in charged colloidal PbS and CdSe quantum dots

    NASA Astrophysics Data System (ADS)

    Voznyy, Oleksandr; Thon, Susanna; Ip, Alex; Sargent, Edward

    2013-03-01

    Colloidal quantum dots (CQDs) offer a promising path towards high efficiency, scalable, solution and room processed photovoltaics and electronics. Their promise is curtailed today by difficulty of doping, inefficient transport, nonradiative recombination, and blinking, all generally attributed to electronic trap formation. Using first-principles simulations on off-stoichiometric colloidal quantum dots, we show that preparing a CQD free of traps is possible. However, self-compensating defects can form deep electronic trap states in response to charging or doping even in the most idealized CQDs. Surface traps arise from atomic dimers whose energy levels reside within the bandgap. The same states can also form upon photoexcitation, providing an atomistic mechanism for blinking. We show that avoiding the trap formation upon doping is possible by incorporation of select cations on the surface which shift the dimer energy levels above the quantum-confined bandedge.

  14. Spontaneous emission enhancement of colloidal CdSe nanoplatelets

    NASA Astrophysics Data System (ADS)

    Yang, Zhili; Pelton, Matthew; Waks, Edo

    Colloidal CdS /CdSe/CdS nanoplatelets synthesized recently are high efficient nano-emitters and gain media for nanoscale lasers and other nonlinear optical devices. They are characterized as quantum well structure due to energy gap difference between core CdSe and shell CdS, of which the luminescent wavelength could be tuned precisely by their thickness of growth. However, the influence of environment on the material's optical properties and further enhancement of the emission to implement nanoscale systems remains to be investigated. Here we demonstrate spontaneous emission rate enhancement of these CdSe nanoplatelets coupled to a photonic crystal cavity. We show clearly the photoluminescent spectrum modification of the nanoplatelets emission and an averaged Purcell enhancement factor of 3.1 is achieved when they are coupled to carefully-designed nanobeam photonic crystal cavities compared to the ones on unpatterned surface in our experiment of lifetime measurement. Also the phenomenon of cavity quality factor increasing is observed when increasing intensity of pumping, which attributes to saturable absorption of the nanoplatelets. Our success in enhancement of emission from these nanoplatelets here paves the road to realize actual nanoscale integrated systems such as ultra-low threshold micro-cavity lasers.

  15. Amphoteric CdSe nanocrystalline quantum dots.

    PubMed

    Islam, Mohammad A

    2008-06-25

    The nanocrystal quantum dot (NQD) charge states strongly influence their electrical transport properties in photovoltaic and electroluminescent devices, optical gains in NQD lasers, and the stability of the dots in thin films. We report a unique electrostatic nature of CdSe NQDs, studied by electrophoretic methods. When we submerged a pair of metal electrodes, in a parallel plate capacitor configuration, into a dilute solution of CdSe NQDs in hexane, and applied a DC voltage across the pair, thin films of CdSe NQDs were deposited on both the positive and the negative electrodes. Extensive characterizations including scanning electron microscopy (SEM), atomic force microscopy (AFM), Fourier transform infrared (FTIR) and Raman studies revealed that the films on both the positive and the negative electrodes were identical in every respect, clearly indicating that: (1) a fraction (<1%) of the CdSe NQDs in free form in hexane solution are charged and, more importantly, (2) there are equal numbers of positive and negative CdSe NQDs in the hexane solution. Experiments also show that the number of deposited dots is at least an order of magnitude higher than the number of initially charged dots, indicating regeneration. We used simple thermodynamics to explain such amphoteric nature and the charging/regeneration of the CdSe NQDs.

  16. Persistent Inter-Excitonic Quantum Coherence in CdSe Quantum Dots

    PubMed Central

    Caram, Justin R.; Zheng, Haibin; Dahlberg, Peter D.; Rolczynski, Brian S.; Griffin, Graham B.; Fidler, Andrew F.; Dolzhnikov, Dmitriy S.; Talapin, Dmitri V.; Engel, Gregory S.

    2014-01-01

    The creation and manipulation of quantum superpositions is a fundamental goal for the development of materials with novel optoelectronic properties. In this letter, we report persistent (~80 fs lifetime) quantum coherence between the 1S and 1P excitonic states in zinc-blende colloidal CdSe quantum dots at room temperature, measured using Two-Dimensional Electronic Spectroscopy. We demonstrate that this quantum coherence manifests as an intradot phenomenon, the frequency of which depends on the size of the dot excited within the ensemble of QDs. We model the lifetime of the coherence and demonstrate that correlated interexcitonic fluctuations preserve relative phase between excitonic states. These observations suggest an avenue for engineering long-lived interexcitonic quantum coherence in colloidal quantum dots. PMID:24719679

  17. Fluorescence relaxation dynamics of CdSe and CdSe/CdS core/shell quantum dots

    SciTech Connect

    Kaur, Gurvir; Kaur, Harmandeep; Tripathi, S. K.

    2014-04-24

    Time-resolved fluorescence spectra for colloidal CdSe and CdSe/CdS core/shell quantum dots have been investigated to know their electron relaxation dynamics at the maximum steady state fluorescence intensity. CdSe core and CdSe/CdS type I core-shell materials with different shell (CdS) thicknesses have been synthesized using mercaptoacetic acid as a capping agent. Steady state absorption and emission studies confirmed successful synthesis of CdSe and CdSe/CdS core-shell quantum dots. The fluorescence shows a tri-exponential decay with lifetimes 57.39, 7.82 and 0.96 ns for CdSe quantum dots. The lifetime of each recombination decreased with growth of CdS shell over the CdSe core, with maximum contribution to fluorescence by the fastest transition.

  18. Temporary Charge Carrier Separation Dominates the Photoluminescence Decay Dynamics of Colloidal CdSe Nanoplatelets.

    PubMed

    Rabouw, Freddy T; van der Bok, Johanna C; Spinicelli, Piernicola; Mahler, Benoît; Nasilowski, Michel; Pedetti, Silvia; Dubertret, Benoît; Vanmaekelbergh, Daniël

    2016-03-01

    Luminescent colloidal CdSe nanoplatelets with atomically defined thicknesses have recently been developed, and their potential for various applications has been shown. To understand their special properties, experiments have until now focused on the relatively short time scales of at most a few nanoseconds. Here, we measure the photoluminescence decay dynamics of colloidal nanoplatelets on time scales up to tens of microseconds. The excited state dynamics are found to be dominated by the slow (∼μs) dynamics of temporary exciton storage in a charge-separated state, previously overlooked. We study the processes of charge carrier separation and exciton recovery in pure CdSe nanoplatelets as well as in core-crown and core-shell CdSe/CdS nanoplatelets with high ensemble quantum yields of 50%, and discuss the implications. Our work highlights the importance of reversible charge carrier trapping and experiments over a wide range of time scales for the understanding of colloidal nanoemitters in general and nanoplatelets in particular. PMID:26863992

  19. Photoluminescence of patterned CdSe quantum dot for anti-counterfeiting label on paper

    NASA Astrophysics Data System (ADS)

    Isnaeni, Yulianto, Nursidik; Suliyanti, Maria Margaretha

    2016-03-01

    We successfully developed a method utilizing colloidal CdSe nanocrystalline quantum dot for anti-counterfeiting label on a piece of glossy paper. We deposited numbers and lines patterns of toluene soluble CdSe quantum dot using rubber stamper on a glossy paper. The width of line pattern was about 1-2 mm with 1-2 mm separation between lines. It required less than one minute for deposited CdSe quantum dot on glossy paper to dry and become invisible by naked eyes. However, patterned quantum dot become visible using long-pass filter glasses upon excitation of UV lamp or blue laser. We characterized photoluminescence of line patterns of quantum dot, and we found that emission boundaries of line patterns were clearly observed. The error of line size and shape were mainly due to defect of the original stamper. The emission peak wavelength of CdSe quantum dot was 629 nm. The emission spectrum of deposited quantum dot has full width at half maximum (FWHM) of 30-40 nm. The spectra similarity between deposited quantum dot and the original quantum dot in solution proved that our stamping method can be simply applied on glossy paper without changing basic optical property of the quantum dot. Further development of this technique is potential for anti-counterfeiting label on very important documents or objects.

  20. Synthesis and Optical Properties of Colloidal CdS/CdSe/CdS Quantum Wells

    NASA Astrophysics Data System (ADS)

    Hai, Le Ba; Nghia, Nguyen Xuan; Nga, Pham Thu; Chinh, Vu Duc; Linh, Pham Thuy; Trang, Nguyen Thi Thu

    Colloidal CdS/CdSe/CdS quantum wells were synthesized from TOPSe and cadmium oleate in octadecene, a non-coordinating solvent. Absorption, emission, and Raman scattering spectra of colloidal CdS/CdSe/CdS quantum wells with different thickness of CdSe well were investigated. The effect of thickness of CdSe well on the optical and vibrational properties of colloidal CdS/CdSe/CdS quantum wells was discussed. The expri-mental results provide further evidence for the existence of quantum dot-quantum well structures in CdS/CdSe/CdS type materials.

  1. Detection of CdSe quantum dot photoluminescence for security label on paper

    NASA Astrophysics Data System (ADS)

    Isnaeni, Sugiarto, Iyon Titok; Bilqis, Ratu; Suseno, Jatmiko Endro

    2016-02-01

    CdSe quantum dot has great potential in various applications especially for emitting devices. One example potential application of CdSe quantum dot is security label for anti-counterfeiting. In this work, we present a practical approach of security label on paper using one and two colors of colloidal CdSe quantum dot, which is used as stamping ink on various types of paper. Under ambient condition, quantum dot is almost invisible. The quantum dot security label can be revealed by detecting emission of quantum dot using photoluminescence and cnc machine. The recorded quantum dot emission intensity is then analyzed using home-made program to reveal quantum dot pattern stamp having the word 'RAHASIA'. We found that security label using quantum dot works well on several types of paper. The quantum dot patterns can survive several days and further treatment is required to protect the quantum dot. Oxidation of quantum dot that occurred during this experiment reduced the emission intensity of quantum dot patterns.

  2. Slow electron cooling in colloidal quantum dots.

    PubMed

    Pandey, Anshu; Guyot-Sionnest, Philippe

    2008-11-01

    Hot electrons in semiconductors lose their energy very quickly (within picoseconds) to lattice vibrations. Slowing this energy loss could prove useful for more efficient photovoltaic or infrared devices. With their well-separated electronic states, quantum dots should display slow relaxation, but other mechanisms have made it difficult to observe. We report slow intraband relaxation (>1 nanosecond) in colloidal quantum dots. The small cadmium selenide (CdSe) dots, with an intraband energy separation of approximately 0.25 electron volts, are capped by an epitaxial zinc selenide (ZnSe) shell. The shell is terminated by a CdSe passivating layer to remove electron traps and is covered by ligands of low infrared absorbance (alkane thiols) at the intraband energy. We found that relaxation is markedly slowed with increasing ZnSe shell thickness.

  3. Origins of low energy-transfer efficiency between patterned GaN quantum well and CdSe quantum dots

    SciTech Connect

    Xu, Xingsheng

    2015-03-02

    For hybrid light emitting devices (LEDs) consisting of GaN quantum wells and colloidal quantum dots, it is necessary to explore the physical mechanisms causing decreases in the quantum efficiencies and the energy transfer efficiency between a GaN quantum well and CdSe quantum dots. This study investigated the electro-luminescence for a hybrid LED consisting of colloidal quantum dots and a GaN quantum well patterned with photonic crystals. It was found that both the quantum efficiency of colloidal quantum dots on a GaN quantum well and the energy transfer efficiency between the patterned GaN quantum well and the colloidal quantum dots decreased with increases in the driving voltage or the driving time. Under high driving voltages, the decreases in the quantum efficiency of the colloidal quantum dots and the energy transfer efficiency can be attributed to Auger recombination, while those decreases under long driving time are due to photo-bleaching and Auger recombination.

  4. Study of the Spectral Properties of Nanocomposites with CdSe Quantum Dots in a Wide Range of Low Temperatures

    NASA Astrophysics Data System (ADS)

    Magaryan, K. A.; Eremchev, I. Y.; Karimullin, K. R.; Knyazev, M. V.; Mikhailov, M. A.; Vasilieva, I. A.; Klimusheva, G. V.

    2015-09-01

    Luminescence spectra of the colloidal solution of CdSe quantum dots (in toluene) were studied in a wide range of low temperatures. Samples were synthesized in the liquid crystal matrix of cadmium octanoate (CdC8). A comparative analysis of the obtained data with previous results was performed.

  5. Colloidal Double Quantum Dots

    PubMed Central

    2016-01-01

    Conspectus Pairs of coupled quantum dots with controlled coupling between the two potential wells serve as an extremely rich system, exhibiting a plethora of optical phenomena that do not exist in each of the isolated constituent dots. Over the past decade, coupled quantum systems have been under extensive study in the context of epitaxially grown quantum dots (QDs), but only a handful of examples have been reported with colloidal QDs. This is mostly due to the difficulties in controllably growing nanoparticles that encapsulate within them two dots separated by an energetic barrier via colloidal synthesis methods. Recent advances in colloidal synthesis methods have enabled the first clear demonstrations of colloidal double quantum dots and allowed for the first exploratory studies into their optical properties. Nevertheless, colloidal double QDs can offer an extended level of structural manipulation that allows not only for a broader range of materials to be used as compared with epitaxially grown counterparts but also for more complex control over the coupling mechanisms and coupling strength between two spatially separated quantum dots. The photophysics of these nanostructures is governed by the balance between two coupling mechanisms. The first is via dipole–dipole interactions between the two constituent components, leading to energy transfer between them. The second is associated with overlap of excited carrier wave functions, leading to charge transfer and multicarrier interactions between the two components. The magnitude of the coupling between the two subcomponents is determined by the detailed potential landscape within the nanocrystals (NCs). One of the hallmarks of double QDs is the observation of dual-color emission from a single nanoparticle, which allows for detailed spectroscopy of their properties down to the single particle level. Furthermore, rational design of the two coupled subsystems enables one to tune the emission statistics from single

  6. Quantum chemistry of the minimal CdSe clusters.

    PubMed

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

    2008-08-21

    Colloidal quantum dots are semiconductor nanocrystals (NCs) which have stimulated a great deal of research and have attracted technical interest in recent years due to their chemical stability and the tunability of photophysical properties. While internal structure of large quantum dots is similar to bulk, their surface structure and passivating role of capping ligands (surfactants) are not fully understood to date. We apply ab initio wavefunction methods, density functional theory, and semiempirical approaches to study the passivation effects of substituted phosphine and amine ligands on the minimal cluster Cd(2)Se(2), which is also used to benchmark different computational methods versus high level ab initio techniques. Full geometry optimization of Cd(2)Se(2) at different theory levels and ligand coverage is used to understand the affinities of various ligands and the impact of ligands on cluster structure. Most possible bonding patterns between ligands and surface CdSe atoms are considered, including a ligand coordinated to Se atoms. The degree of passivation of Cd and Se atoms (one or two ligands attached to one atom) is also studied. The results suggest that B3LYP/LANL2DZ level of theory is appropriate for the system modeling, whereas frequently used semiempirical methods (such as AM1 and PM3) produce unphysical results. The use of hydrogen atom for modeling of the cluster passivating ligands is found to yield unphysical results as well. Hence, the surface termination of II-VI semiconductor NCs with hydrogen atoms often used in computational models should probably be avoided. Basis set superposition error, zero-point energy, and thermal corrections, as well as solvent effects simulated with polarized continuum model are found to produce minor variations on the ligand binding energies. The effects of Cd-Se complex structure on both the electronic band gap (highest occupied molecular orbital-lowest unoccupied molecular orbital energy difference) and ligand

  7. Anisotropy in CdSe quantum rods

    SciTech Connect

    Li, Liang-shi

    2003-09-01

    The size-dependent optical and electronic properties of semiconductor nanocrystals have drawn much attention in the past decade, and have been very well understood for spherical ones. The advent of the synthetic methods to make rod-like CdSe nanocrystals with wurtzite structure has offered us a new opportunity to study their properties as functions of their shape. This dissertation includes three main parts: synthesis of CdSe nanorods with tightly controlled widths and lengths, their optical and dielectric properties, and their large-scale assembly, all of which are either directly or indirectly caused by the uniaxial crystallographic structure of wurtzite CdSe. The hexagonal wurtzite structure is believed to be the primary reason for the growth of CdSe nanorods. It represents itself in the kinetic stabilization of the rod-like particles over the spherical ones in the presence of phosphonic acids. By varying the composition of the surfactant mixture used for synthesis we have achieved tight control of the widths and lengths of the nanorods. The synthesis of monodisperse CdSe nanorods enables us to systematically study their size-dependent properties. For example, room temperature single particle fluorescence spectroscopy has shown that nanorods emit linearly polarized photoluminescence. Theoretical calculations have shown that it is due to the crossing between the two highest occupied electronic levels with increasing aspect ratio. We also measured the permanent electric dipole moment of the nanorods with transient electric birefringence technique. Experimental results on nanorods with different sizes show that the dipole moment is linear to the particle volume, indicating that it originates from the non-centrosymmetric hexagonal lattice. The elongation of the nanocrystals also results in the anisotropic inter-particle interaction. One of the consequences is the formation of liquid crystalline phases when the nanorods are dispersed in solvent to a high enough

  8. Femtosecond cooling of hot electrons in CdSe quantum-well platelets.

    PubMed

    Sippel, Philipp; Albrecht, Wiebke; van der Bok, Johanna C; Van Dijk-Moes, Relinde J A; Hannappel, Thomas; Eichberger, Rainer; Vanmaekelbergh, Daniel

    2015-04-01

    Semiconductor quantum wells are ubiquitous in high-performance optoelectronic devices such as solar cells and lasers. Understanding and controlling of the (hot) carrier dynamics is essential to optimize their performance. Here, we study hot electron cooling in colloidal CdSe quantum-well nanoplatelets using ultrafast two-photon photoemission spectroscopy at low excitation intensities, resulting typically in 1-5 hot electrons per platelet. We observe initial electron cooling in the femtosecond time domain that slows down with decreasing electron energy and is finished within 2 ps. The cooling is considerably faster at cryogenic temperatures than at room temperature, and at least for the systems that we studied, independent of the thickness of the platelets (here 3-5 CdSe units) and the presence of a CdS shell. The cooling rates that we observe are orders of magnitude faster than reported for similar CdSe platelets under strong excitation. Our results are understood by a classic cooling mechanism with emission of longitudinal optical phonons without a significant influence of the surface. PMID:25764379

  9. Synthesis of CdSe quantum dots for quantum dot sensitized solar cell

    SciTech Connect

    Singh, Neetu Kapoor, Avinashi; Kumar, Vinod; Mehra, R. M.

    2014-04-24

    CdSe Quantum Dots (QDs) of size 0.85 nm were synthesized using chemical route. ZnO based Quantum Dot Sensitized Solar Cell (QDSSC) was fabricated using CdSe QDs as sensitizer. The Pre-synthesized QDs were found to be successfully adsorbed on front ZnO electrode and had potential to replace organic dyes in Dye Sensitized Solar Cells (DSSCs). The efficiency of QDSSC was obtained to be 2.06 % at AM 1.5.

  10. Experimental Observation of Quantum Confinement in the Conduction Band of CdSe Quantum Dots

    SciTech Connect

    Lee, J I; Meulenberg, R W; Hanif, K M; Mattoussi, H; Klepeis, J E; Terminello, L J; van Buuren, T

    2006-12-15

    Recent theoretical descriptions as to the magnitude of effect that quantum confinement has on he conduction band (CB) of CdSe quantum dots (QD) have been conflicting. In this manuscript, we experimentally identify quantum confinement effects in the CB of CdSe QDs for the first time. Using X-ray absorption spectroscopy, we have unambiguously witnessed the CB minimum shift to higher energy with decreasing particle size and have been able to compare these results to recent theories. Our experiments have been able to identify which theories correctly describe the CB states in CdSe QDs. In particular, our experiments suggest that multiple theories describe the shifts in the CB of CdSe QDs and are not mutually exclusive.

  11. CdTe and CdSe Quantum Dots Cytotoxicity: A Comparative Study on Microorganisms

    PubMed Central

    Gomes, Suzete A.O.; Vieira, Cecilia Stahl; Almeida, Diogo B.; Santos-Mallet, Jacenir R.; Menna-Barreto, Rubem F. S.; Cesar, Carlos L.; Feder, Denise

    2011-01-01

    Quantum dots (QDs) are colloidal semiconductor nanocrystals of a few nanometers in diameter, being their size and shape controlled during the synthesis. They are synthesized from atoms of group II–VI or III–V of the periodic table, such as cadmium telluride (CdTe) or cadmium selenium (CdSe) forming nanoparticles with fluorescent characteristics superior to current fluorophores. The excellent optical characteristics of quantum dots make them applied widely in the field of life sciences. Cellular uptake of QDs, location and translocation as well as any biological consequence, such as cytotoxicity, stimulated a lot of scientific research in this area. Several studies pointed to the cytotoxic effect against micoorganisms. In this mini-review, we overviewed the synthesis and optical properties of QDs, and its advantages and bioapplications in the studies about microorganisms such as protozoa, bacteria, fungi and virus. PMID:22247686

  12. CdSe quantum dot internalization by Bacillus subtilis and Escherichia coli

    NASA Technical Reports Server (NTRS)

    Kloepfer, Jeremiah A.; Mielke, Randall E.; Nadeau, Jay L.

    2004-01-01

    Biological labeling has been demonstrated with CdSe quantum dots in a variety of animal cells, but bacteria are harder to label because of their cell walls. We discuss the challenges of using minimally coated, bare CdSe quantum dots as luminescent internal labels for bacteria.

  13. Influence of Surfactants and Charges on CdSe Quantum Dots

    SciTech Connect

    Yang, Ping; Tretiak, Sergei; Ivanov, Sergei

    2011-07-11

    The chemistry between CdSe quantum dots and common surface capping ligands is invested using density functional theory. We will discuss the electronic structures and optical properties of CdSe QDs controlled by the size of particle, self-organization, capping ligands, and positive charges. Charges on quantum dots have profound effects on their structures, binding energies, and optical properties.

  14. A Safer, Easier, Faster Synthesis for CdSe Quantum Dot Nanocrystals

    ERIC Educational Resources Information Center

    Boatman, Elizabeth M.; Lisensky, George C.; Nordell, Karen J.

    2005-01-01

    The synthesis for CdSe quantum dot nanocrystals that vary in color and are a visually engaging way to demonstrate quantum effects in chemistry is presented. CdSe nanocrystals are synthesized from CdO and elemental Se using a kinetic growth method where particle size depends on reaction time.

  15. Two-Photon Photochemistry of CdSe Quantum Dots.

    PubMed

    Zeng, Youhong; Kelley, David F

    2015-10-27

    The two-photon photochemistry of CdSe quantum dots (QDs) has been systematically studied. We find that upon intense irradiation CdSe quantum dots that absorb two or more visible photons undergo photodarkening. The quantum yield for this process is on the order of 6% in chloroform and much smaller in nonpolar solvents, such as octane. An analysis of the energetics indicates that, following two-photon excitation, the biexciton undergoes an Auger process producing a hot hole. This hot hole is ejected to a surface-bound TOP ligand, forming a QD(-)/TOP(+) contact ion pair that separates in chloroform, but not in octane. The charged and deligated QD is dark, resulting in the overall photodarkening. This photodarkening reaction may or may not be reversible, depending on what other chemical components are in the irradiated solution. The quantum dot concentration dependence and PL decay kinetics indicate that charge recombination occurs rapidly, followed by ligand reattachment and reorganization on a longer (tens of minutes) time scale. The relation of this mechanism to one-photon photochemistry is also discussed.

  16. A Closer Look into the Traditional Purification Process of CdSe Semiconductor Quantum Dots.

    PubMed

    Shakeri, Behtash; Meulenberg, Robert W

    2015-12-15

    This paper describes how the postprocessing procedure for wurtzite CdSe quantum dots (QDs) 4.8 and 6.7 nm in diameter is affected by both the choice of nonsolvent and the number of processing steps. Using a host of analytical techniques (ultraviolet-visible, photoluminescence, nuclear magnetic, X-ray photoelectron, and infrared spectroscopy, as well as thermogravimetric analysis), we find that control over the ligand type and surface density can be achieved simply by the number of washing steps used during the postprocessing procedure. Using multiple washing steps we can achieve colloidally stable solutions of QDs with organic mass fractions as low as 13% by mass. For CdSe QDs passivated with trioctylphosphine oxide (TOPO) and stearic acid (SA), essentially no TOPO is bound to the particle surface after three or four washing steps, with a plateau in the amount of SA being removed. The results can be explained using the L- and X-type ligand classification system for QDs, with L-type ligands (TOPO) removed in the early processing steps but the removal of X-type (SA) ligand stalling at a large number of washing steps due to charging of the QDs. Importantly, very little change is observed in the photoluminescence (PL) properties, suggesting that the choice of nonsolvent during postprocessing will allow the production of QD materials with very low organic content by mass but with good PL quantum yields. PMID:26625188

  17. Optical enhancement of photoluminescence with colloidal quantum dots

    NASA Astrophysics Data System (ADS)

    Abraham, Gabrielle; French, David A.; Bajwa, Pooja; Heyes, Colin D.; Herzog, Joseph B.

    2015-08-01

    This work investigates colloidal, semiconductor Cadmium Selenide (CdSe) QDs with optical spectroscopy measurements. A custom-built microscope has been used for photoluminescence spectroscopy and has collected images, videos, and spectra of samples to study the effects of substrates, sample density, uniformity, and QD aging with time. This set up will be used to detect single to a few molecules, shown by fluorescent intermittency, or QD blinking. Differences in the spectrum will be noted as related to the age of samples, the density of the quantum dots, and the concentration of samples. Further experiments include the potential plasmonic enhancement of QD photoluminescence by gold nanoparticles or nanostructures.

  18. Thermal Recovery of Colloidal Quantum Dot Ensembles Following Photoinduced Dimming.

    PubMed

    Jensen, Russell A; Coropceanu, Igor; Chen, Yue; Bawendi, Moungi G

    2015-08-01

    Colloidal CdSe quantum dot (QD) core ensembles were photodimmed and allowed to recover in the dark using ambient thermal energy at a range of temperatures. Nonlinear thermal recovery is well described by a stretched exponential function, and further analysis yields an underlying probability distribution of rate constants. Casting the rate constants as a collection of first-order activated processes provides an activation barrier probability distribution with significant density at room-temperature thermal energy that peaks at 200 meV before decaying to zero. This treatment for the recovery transition intuitively describes the distributed kinetics observed and complements commonly proposed blinking mechanisms.

  19. Direct Patterning of CdSe Quantum Dots into Sub-100 nm Structures

    SciTech Connect

    Hampton, Meredith J.; Templeton, Joseph L.; DeSimone, Joseph M.

    2010-03-02

    Ordered, two-dimensional cadmium selenide (CdSe) arrays have been fabricated on indium-doped tin oxide (ITO) electrodes using the pattern replication in nonwetting templates (PRINT) process. CdSe quantum dots (QDs) with an average diameter of 2.7 nm and a pyridine surface ligand were used for patterning. The PRINT technique utilizes a perfluoropolyether (PFPE) elastomeric mold that is tolerant of most organic solvents, thus allowing solutions of CdSe QDs in 4-picoline to be used for patterning without significant deformation of the mold. Nanometer-scale diffraction gratings have been successfully replicated with CdSe QDs.

  20. Thiolated graphene--a new platform for anchoring CdSe quantum dots for hybrid heterostructures.

    PubMed

    Debgupta, Joyashish; Pillai, Vijayamohanan K

    2013-05-01

    Effective organization of small CdSe quantum dots on graphene sheets has been achieved by a simple solution exchange with thiol terminated graphene prepared by diazonium salt chemistry. This generic methodology of CdSe QD attachment to any graphene surface has remarkable implications in designing hybrid heterostructures.

  1. Fluorescence quenching of CdSe quantum dots on graphene

    SciTech Connect

    Guo, Xi Tao; Hua Ni, Zhen Yan Nan, Hai; Hui Wang, Wen; Yan Liao, Chun; Zhang, Yan; Wei Zhao, Wei

    2013-11-11

    We studied systematically the fluorescence quenching of CdSe quantum dots (QDs) on graphene and its multilayers, as well as graphene oxide (GO) and reduced graphene oxide (rGO). Raman intensity of QDs was used as a quantitatively measurement of its concentration in order to achieve a reliable quenching factor (QF). It was found that the QF of graphene (∼13.1) and its multilayers is much larger than rGO (∼4.4), while GO (∼1.5) has the lowest quenching efficiency, which suggests that the graphitic structure is an important factor for quenching the fluorescence of QDs. It was also revealed that the QF of graphene is not strongly dependent on its thicknesses.

  2. Ligand Induced Circular Dichroism and Circularly Polarized Luminescence in CdSe Quantum Dots

    PubMed Central

    Tohgha, Urice; Deol, Kirandeep K.; Porter, Ashlin G.; Bartko, Samuel G.; Choi, Jung Kyu; Leonard, Brian M.; Varga, Krisztina; Kubelka, Jan; Muller, Gilles; Balaz, Milan

    2014-01-01

    Chiral thiol capping ligands L- and D-cysteines induced modular chiroptical properties in achiral cadmium selenide quantum dots (CdSe QDs). Cys-CdSe prepared from achiral oleic acid capped CdSe by post-synthetic ligand exchange displayed size-dependent electronic circular dichroism (CD) and circularly polarized luminescence (CPL). Opposite CPL signals were measured for the CdSe QDs capped with D- and L-cysteine. The CD profile and CD anisotropy varied with size of CdSe nanocrystals with largest anisotropy observed for CdSe nanoparticles of 4.4 nm. Magic angle spinning solid state NMR (MAS ssNMR) experiments suggested bidentate interaction between cysteine and the surface of CdSe. Density functional theory (DFT) calculations verified that attachment of L- and D-cysteine to the surface of model (CdSe)13 nanoclusters induces measurable opposite CD signals for the exitonic band of the nanocluster. The chirality was induced by the hybridization of highest occupied CdSe molecular orbitals with those of the chiral ligand. PMID:24200288

  3. Ligand induced circular dichroism and circularly polarized luminescence in CdSe quantum dots.

    PubMed

    Tohgha, Urice; Deol, Kirandeep K; Porter, Ashlin G; Bartko, Samuel G; Choi, Jung Kyu; Leonard, Brian M; Varga, Krisztina; Kubelka, Jan; Muller, Gilles; Balaz, Milan

    2013-12-23

    Chiral thiol capping ligands L- and D-cysteines induced modular chiroptical properties in achiral cadmium selenide quantum dots (CdSe QDs). Cys-CdSe prepared from achiral oleic acid capped CdSe by postsynthetic ligand exchange displayed size-dependent electronic circular dichroism (CD) and circularly polarized luminescence (CPL). Opposite CPL signals were measured for the CdSe QDs capped with D- and L-cysteine. The CD profile and CD anisotropy varied with size of CdSe nanocrystals with largest anisotropy observed for CdSe nanoparticles of 4.4 nm. Magic angle spinning solid state NMR (MAS ssNMR) experiments suggested bidentate interaction between cysteine and the surface of CdSe. Time Dependent Density Functional Theory (TDDFT) calculations verified that attachment of L- and D-cysteine to the surface of model (CdSe)13 nanoclusters induces measurable opposite CD signals for the exitonic band of the nanocluster. The origin of the induced chirality is consistent with the hybridization of highest occupied CdSe molecular orbitals with those of the chiral ligand.

  4. CdSe quantum dot formation: alternative paths to relaxation of a strained CdSe layer and influence of the capping conditions.

    PubMed

    Robin, I C; Aichele, T; Bougerol, C; André, R; Tatarenko, S; Bellet-Amalric, E; Van Daele, B; Van Tendeloo, G

    2007-07-01

    CdSe/ZnSe quantum dot formation is investigated by studying different steps of the growth. To precisely control the critical thickness of CdSe grown on a ZnSe buffer layer, the CdSe self-regulated growth rate in atomic layer epitaxy growth mode is determined by reflection high-energy electron diffraction (RHEED) measurements for a temperature range between 180 and 280 °C. Then, the two-dimensional-three-dimensional (2D-3D) transition of a strained CdSe layer on (001)-ZnSe induced by the use of amorphous selenium is studied. The formation of CdSe islands is found when 3 monolayers (ML) of CdSe are deposited. When only 2.5 ML of CdSe are deposited, another relaxation mechanism is observed, leading to the appearance of strong undulations on the surface. We also studied the evolution of the surface morphology when 2.7 ML are deposited, to study the boundary between those two phenomena. The influence of capping on quantum dot morphology is investigated. It is found that cadmium is redistributed within the layer during capping. Our results show that the cadmium distribution after capping depends on the capping temperature and on the strain of the CdSe layer. Cadmium incorporation after capping is also studied. It is found that the amount of incorporated cadmium depends on the strain of the CdSe layer before capping.

  5. Improved luminescence from CdSe quantum dots with a strain-compensated shell

    NASA Astrophysics Data System (ADS)

    Lu, Y.; Zhang, Y. Q.; Cao, X. A.

    2013-01-01

    Colloidal CdSe quantum dots (QDs) with a strain-compensated ZnS/ZnCdS bilayer shell were synthesized and characterized. The core/shell/shell structure enjoys the benefits of excellent exciton confinement by the ZnS intermediate shell and strain compensation by the ZnCdS outer shell. The resulting CdSe/ZnS/ZnCdS QDs exhibited a 40% higher photoluminescence quantum yield and a more controllable wavelength compared to conventional CdSe/ZnCdS/ZnS core/shell/shell QDs with an intermediate lattice adaptor. CdSe/ZnS/ZnCdS QD light-emitting diodes (LEDs) had a luminance of 556 cd/m2 at 20 mA/cm2, 28% higher than that of CdSe/ZnCdS/ZnS QD-LEDs. The former also had better spectral purity at high injection currents and are thus better suited for full-color displays.

  6. Sulforaphane Protects the Liver against CdSe Quantum Dot-Induced Cytotoxicity

    PubMed Central

    Wang, Wei; He, Yan; Yu, Guodong; Li, Baolong; Sexton, Darren W.; Wileman, Thomas; Roberts, Alexandra A.; Hamilton, Chris J.; Liu, Ruoxi; Chao, Yimin; Shan, Yujuan; Bao, Yongping

    2015-01-01

    The potential cytotoxicity of cadmium selenide (CdSe) quantum dots (QDs) presents a barrier to their use in biomedical imaging or as diagnostic and therapeutic agents. Sulforaphane (SFN) is a chemoprotective compound derived from cruciferous vegetables which can up-regulate antioxidant enzymes and induce apoptosis and autophagy. This study reports the effects of SFN on CdSe QD-induced cytotoxicity in immortalised human hepatocytes and in the livers of mice. CdSe QDs induced dose-dependent cell death in hepatocytes with an IC50 = 20.4 μM. Pre-treatment with SFN (5 μM) increased cell viability in response to CdSe QDs (20 μM) from 49.5 to 89.3%. SFN induced a pro-oxidant effect characterized by depletion of intracellular reduced glutathione during short term exposure (3–6 h), followed by up-regulation of antioxidant enzymes and glutathione levels at 24 h. SFN also caused Nrf2 translocation into the nucleus, up-regulation of antioxidant enzymes and autophagy. siRNA knockdown of Nrf2 suggests that the Nrf2 pathway plays a role in the protection against CdSe QD-induced cell death. Wortmannin inhibition of SFN-induced autophagy significantly suppressed the protective effect of SFN on CdSe QD-induced cell death. Moreover, the role of autophagy in SFN protection against CdSe QD-induced cell death was confirmed using mouse embryonic fibroblasts lacking ATG5. CdSe QDs caused significant liver damage in mice, and this was decreased by SFN treatment. In conclusion, SFN attenuated the cytotoxicity of CdSe QDs in both human hepatocytes and in the mouse liver, and this protection was associated with the induction of Nrf2 pathway and autophagy. PMID:26402917

  7. Tuning luminescence and reducing reabsorption of CdSe quantum disks for luminescent solar concentrators

    NASA Astrophysics Data System (ADS)

    Lin, Huichuan; Xie, Peng; Liu, Yong; Zhou, Xiang; Li, Baojun

    2015-08-01

    Cadmium selenide (CdSe) quantum disks (QDs) have been synthesized for application in luminescent solar concentrators (LSCs). Luminescence tuning and reabsorption reduction of the QDs were achieved by controlling their size using a hot injection method. The overlap of the absorption and photoluminescence spectra of the as-prepared CdSe QDs was negligible. The as-prepared CdSe QDs were incorporated into polymethylmethacrylate without aggregation and luminescence quenching. The obtained highly transparent composites with non-affecting light-emitting properties were used as LSCs. The placement of a CdSe QDs doped LSC prototype (10 × 1 × 0.1 cm) on a Si-cell resulted in a 201% increase in the electrical power output of the Si-cell compared with that of the bare Si-cell.

  8. Enchanced methods of hydrophilized CdSe quantum dots synthesis

    NASA Astrophysics Data System (ADS)

    Potapkin, D. V.; Zharkova, I. S.; Goryacheva, I. Y.

    2015-03-01

    Quantum dots are bright and stable fluorescence signal sources, but for most of applications they need an additional hydrophilization step. Unfortunately, most of existing approaches lead to QD's fluorescence quenching, so there is a need for additional enhancing of hydrophilized QD's brightness like UV irradiation, which can be used both on water insoluble QD's with oleic acid ligands (in toluene) and on hydrophilized QD's covered with UV-stable polymer (in aqueous solution). For synthesis of bright water-soluble fluorescent labels CdSe/CdS/ZnS colloidal quantum dots were covered with PAMAM dendrimer and irradiated with UV lamp in quartz cuvettes for 3 hours at the room temperature and then compared with control sample.

  9. In-situ material state monitoring using embedded CdSe quantum dots

    NASA Astrophysics Data System (ADS)

    Brubaker, Cole D.; Frecker, Talitha M.; Njoroge, Ian; Shane, Dylan O.; Smudde, Christine M.; Rosenthal, Sandra J.; Jennings, G. Kane; Adams, Douglas E.

    2016-04-01

    The development of new, smart materials capable of intrinsically detecting and communicating the occurrence of external loads and resultant damage present in a material will be crucial in the advancement of future structural health monitoring (SHM) and nondestructive evaluation (NDE) technologies. Traditionally, many SHM and NDE approaches have relied on the use of physical sensors to monitor a structure for damage, but are often hindered by their requirements for power consumption and large-scale data collection. In this work, we seek to evaluate the effectiveness of ultrasmall, white-light emitting Cadmium Selenide quantum dots (CdSe QDs) as an alternative to providing in-situ material state monitoring capabilities, while also aiming to reduce reliance on data collection and power consumption to effectively monitor a material and structure for damage. To achieve this goal, CdSe QDs are embedded in an optically clear epoxy composite matrix and exposed to external mechanical loadings. Initial results show a corresponding relationship between the shifts in observed emission spectra and external load for samples containing CdSe QDs. The effectiveness of CdSe QDs as a surface strain gauge on aluminum and fiberglass are also investigated in this paper. By monitoring changes in the emission spectra for materials containing CdSe QDs before, during and after the application of external loads, the effectiveness of CdSe QDs for communicating the occurrence of external loads acting on a material and detecting changes in material state is evaluated.

  10. Pulsed laser deposition of Mn doped CdSe quantum dots for improved solar cell performance

    SciTech Connect

    Dai, Qilin; Wang, Wenyong E-mail: jtang2@uwyo.edu; Tang, Jinke E-mail: jtang2@uwyo.edu; Sabio, Erwin M.

    2014-05-05

    In this work, we demonstrate (1) a facile method to prepare Mn doped CdSe quantum dots (QDs) on Zn{sub 2}SnO{sub 4} photoanodes by pulsed laser deposition and (2) improved device performance of quantum dot sensitized solar cells of the Mn doped QDs (CdSe:Mn) compared to the undoped QDs (CdSe). The band diagram of photoanode Zn{sub 2}SnO{sub 4} and sensitizer CdSe:Mn QD is proposed based on the incident-photon-to-electron conversion efficiency (IPCE) data. Mn-modified band structure leads to absorption at longer wavelengths than the undoped CdSe QDs, which is due to the exchange splitting of the CdSe:Mn conduction band by the Mn dopant. Three-fold increase in the IPCE efficiency has also been observed for the Mn doped samples.

  11. Blue and green electroluminescence from CdSe nanocrystal quantum-dot-quantum-wells

    SciTech Connect

    Lu, Y. F.; Cao, X. A.

    2014-11-17

    CdS/CdSe/ZnS quantum dot quantum well (QDQW) nanocrystals were synthesized using the successive ion layer adsorption and reaction technique, and their optical properties were tuned by bandgap and strain engineering. 3-monolayer (ML) CdSe QWs emitted blue photoluminescence at 467 nm with a spectral full-width-at-half-maximum of ∼30 nm. With a 3 ML ZnS cladding layer, which also acts as a passivating and strain-compensating layer, the QDQWs acquired a ∼35% quantum yield of the QW emission. Blue and green electroluminescence (EL) was obtained from QDQW light-emitting devices with 3–4.5 ML CdSe QWs. It was found that as the peak blueshifted, the overall EL was increasingly dominated by defect state emission due to poor hole injection into the QDQWs. The weak EL was also attributed to strong field-induced charge separation resulting from the unique QDQW geometry, weakening the oscillator strength of optical transitions.

  12. Surface-enhanced Raman scattering by colloidal CdSe nanocrystal submonolayers fabricated by the Langmuir-Blodgett technique.

    PubMed

    Milekhin, Alexander G; Sveshnikova, Larisa L; Duda, Tatyana A; Rodyakina, Ekaterina E; Dzhagan, Volodymyr M; Gordan, Ovidiu D; Veber, Sergey L; Himcinschi, Cameliu; Latyshev, Alexander V; Zahn, Dietrich R T

    2015-01-01

    We present the results of an investigation of surface-enhanced Raman scattering (SERS) by optical phonons in colloidal CdSe nanocrystals (NCs) homogeneously deposited on both arrays of Au nanoclusters and Au dimers using the Langmuir-Blodgett technique. The coverage of the deposited NCs was less than one monolayer, as determined by transmission and scanning electron microscopy. SERS by optical phonons in CdSe nanocrystals showed a significant enhancement that depends resonantly on the Au nanocluster and dimer size, and thus on the localized surface plasmon resonance (LSPR) energy. The deposition of CdSe nanocrystals on the Au dimer nanocluster arrays enabled us to study the polarization dependence of SERS. The maximal SERS signal was observed for light polarization parallel to the dimer axis. The polarization ratio of the SERS signal parallel and perpendicular to the dimer axis was 20. The SERS signal intensity was also investigated as a function of the distance between nanoclusters in a dimer. Here the maximal SERS enhancement was observed for the minimal distance studied (about 10 nm), confirming the formation of SERS "hot spots". PMID:26734529

  13. Surface-enhanced Raman scattering by colloidal CdSe nanocrystal submonolayers fabricated by the Langmuir–Blodgett technique

    PubMed Central

    Sveshnikova, Larisa L; Duda, Tatyana A; Rodyakina, Ekaterina E; Dzhagan, Volodymyr M; Gordan, Ovidiu D; Veber, Sergey L; Himcinschi, Cameliu; Latyshev, Alexander V; Zahn, Dietrich R T

    2015-01-01

    Summary We present the results of an investigation of surface-enhanced Raman scattering (SERS) by optical phonons in colloidal CdSe nanocrystals (NCs) homogeneously deposited on both arrays of Au nanoclusters and Au dimers using the Langmuir–Blodgett technique. The coverage of the deposited NCs was less than one monolayer, as determined by transmission and scanning electron microscopy. SERS by optical phonons in CdSe nanocrystals showed a significant enhancement that depends resonantly on the Au nanocluster and dimer size, and thus on the localized surface plasmon resonance (LSPR) energy. The deposition of CdSe nanocrystals on the Au dimer nanocluster arrays enabled us to study the polarization dependence of SERS. The maximal SERS signal was observed for light polarization parallel to the dimer axis. The polarization ratio of the SERS signal parallel and perpendicular to the dimer axis was 20. The SERS signal intensity was also investigated as a function of the distance between nanoclusters in a dimer. Here the maximal SERS enhancement was observed for the minimal distance studied (about 10 nm), confirming the formation of SERS “hot spots”. PMID:26734529

  14. An oleic acid-capped CdSe quantum-dot sensitized solar cell

    SciTech Connect

    Chen Jing; Song, J. L.; Deng, W. Q.; Sun, X. W.; Jiang, C. Y.; Lei, W.; Huang, J. H.; Liu, R. S.

    2009-04-13

    In this letter, we report an oleic acid (OA)-capped CdSe quantum-dot sensitized solar cell (QDSSC) with an improved performance. The TiO{sub 2}/OA-CdSe photoanode in a two-electrode device exhibited a photon-to-current conversion efficiency of 17.5% at 400 nm. At AM1.5G irradiation with 100 mW/cm{sup 2} light intensity, the QDSSCs based on OA-capped CdSe showed a power conversion efficiency of about 1%. The function of OA was to increase QD loading, extend the absorption range and possibly suppress the surface recombination.

  15. CdSe quantum dot internalization by Bacillus subtilis and Escherichia coli

    NASA Astrophysics Data System (ADS)

    Kloepfer, Jeremiah A.; Mielke, Randall E.; Nadeau, Jay L.

    2004-06-01

    Biological labeling has been demonstrated with CdSe quantum dots in a variety of animal cells, but bacteria are harder to label because of their cell walls. We discuss the challenges of using minimally coated, bare CdSe quantum dots as luminescent internal labels for bacteria. These quantum dots were solubilized with mercaptoacetic acid and conjugated to adenine. Significant evidence for the internal staining of Bacillus subtilis (Gram positive) and Escherichia coli (Gram negative) using these structures is presented via steady-state emission, epifluorescence microscopy, transmission electron microscopy, and energy dispersive spectroscopy. In particular, the E. coli adenine auxotroph, and not the wild type, took up adenine coated quantum dots, and this only occurred in adenine deficient growth media. Labeling strength was enhanced by performing the incubation under room light. This process was examined with steady-state emission spectra and time-resolved luminescence profiles obtained from time-correlated-single-photon counting.

  16. The Optical Properties of CdSe Quantum Dots by Using Spray-Atomization Method

    NASA Astrophysics Data System (ADS)

    Rosmani, C. H.; Abdullah, S.; Rusop, M.

    2013-06-01

    Cadmium Selenide (CdSe) quantum dots (QDs) is inorganic material by using spray-atomization method which is the novelty to find out the optical properties for the CdSe QDs. The Selenium (Se) precursor and Cadmium (Cd) precursor were prepared first. Se precursor by using sodium sulfite aqueous was mixed with selenium (Se) powder. For Cd precursor was used cadmium chloride (CdCI) as the Cd precursor. From previous research, CdSe QDs was obtained by using capping agent such as tri-n-octylphosphine oxide (TOPO) and trioctylphosphine (TOP). These capping agent are hazardous to environment and human. By using spray-atomization method it is more safe and economically. The photoluminescence (PL) was used to investigate the optical properties and to investigate the energy band gap from PL result. The field emission scanning electron microscopy (FESEM) was used to know the surface morphology of CdSe QDs. By PL result, the energy band gap was calculate and the comparison was investigate between the size of particle and the energy band gap. This important in this paper is to investigate the optical properties of CdSe QDs by using sprays-atomization method and to relate with the particle size.

  17. Observation of an Excitonic Quantum Coherence in CdSe Nanocrystals.

    PubMed

    Dong, Shuo; Trivedi, Dhara; Chakrabortty, Sabyasachi; Kobayashi, Takayoshi; Chan, Yinthai; Prezhdo, Oleg V; Loh, Zhi-Heng

    2015-10-14

    Recent observations of excitonic coherences within photosynthetic complexes suggest that quantum coherences could enhance biological light harvesting efficiencies. Here, we employ optical pump-probe spectroscopy with few-femtosecond pulses to observe an excitonic quantum coherence in CdSe nanocrystals, a prototypical artificial light harvesting system. This coherence, which encodes the high-speed migration of charge over nanometer length scales, is also found to markedly alter the displacement amplitudes of phonons, signaling dynamics in the non-Born-Oppenheimer regime.

  18. Enhanced photorefractive performance in CdSe quantum-dot-dispersed poly(styrene-co-acrylonitrile) polymers

    SciTech Connect

    Li Xiangping; Embden, Joel van; Chon, James W. M.; Gu Min; Evans, Richard A.

    2010-06-21

    This paper reports on the enhanced photorefractive behavior of a CdSe quantum-dot-dispersed less expensive polymer of poly(styrene-co-acrylonitrile). The capability of CdSe quantum dots used as photosensitizers and the associated photorefractive performance are characterized through a photocurrent experiment and a two-beam coupling experiment, respectively. An enhanced two-beam coupling gain coefficient of 12.2 cm{sup -1} at 46 V/mum was observed owning to the reduced potential barrier. The photorefractive performance per CdSe quantum dot is three orders of magnitude higher than that in the sample sensitized by trinitrofluorenone in poly(styrene-co-acrylonitrile), and almost ten times higher than that in the CdSe quantum-dot-sensitized poly(N-vinylcarbazole) polymers.

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

    PubMed

    Tvrdy, Kevin; Kamat, Prashant V

    2009-04-23

    The photochemical behavior of CdSe quantum dots anchored to different surfaces was probed through their deposition on glass, SiO2, and TiO2 films. Following visible light irradiation under ambient conditions, CdSe quantum dots deposited on semiconducting TiO2 surface degraded, where no such degradation was observed when deposited on inert SiO2 surface or glass. Fluorescence decay and transient absorption experiments confirmed that charge injection from excited CdSe into TiO2 occurs with an apparent rate constant of 5.62 x 10(8) s(-1) and is the primary event responsible for photodegradation. In the presence of air, injected electrons are scavenged by surface adsorbed oxygen leaving behind reactive holes which induce anodic corrosion of CdSe quantum dots. In a vacuum environment, minimal CdSe degradation was observed as electron scavenging by oxygen is replaced with charge recombination between injected electrons and holes in CdSe nanocrystals. Spectroscopic measurements presented in this study highlight the role of both substrate and medium in dictating the photochemistry of CdSe quantum dots. PMID:19152253

  20. Investigation of size dependent structural and optical properties of thin films of CdSe quantum dots

    SciTech Connect

    Sharma, Madhulika; Sharma, A.B.; Mishra, N.; Pandey, R.K.

    2011-03-15

    Research highlights: {yields} CdSe q-dots have been synthesized using simple chemical synthesis route. {yields} Thin film of CdSe quantum dots exhibited self-organized growth. {yields} Size dependent blue shift observed in the absorption edge of CdSe nanocrystallites. {yields} PL emission band corresponds to band edge luminescence and defect luminescence. {yields} Organized growth led to enhancement in luminescence yield of smaller size Q-dots. -- Abstract: Cadmium selenide (CdSe) quantum dots were grown on indium tin oxide substrate using wet chemical technique for possible application as light emitting devices. The structural, morphological and luminescence properties of the as deposited thin films of CdSe Q-dot have been investigated, using X-ray diffraction, transmission electron microscopy, atomic force microscopy and optical and luminescence spectroscopy. The quantum dots have been shown to deposit in an organized array on ITO/glass substrate. The as grown Q-dots exhibited size dependent blue shift in the absorption edge. The effect of quantum confinement also manifested as a blue shift of photoluminescence emission. It is shown that the nanocrystalline CdSe exhibits intense photoluminescence as compared to the large grained polycrystalline CdSe films.

  1. Quantum confinement effect of CdSe induced by nanoscale solvothermal reaction

    NASA Astrophysics Data System (ADS)

    Lee, Jin-Wook; Im, Jeong-Hyuk; Park, Nam-Gyu

    2012-09-01

    We report a novel method, nanoscale solvothermal reaction (NSR), to induce the quantum confinement effect of CdSe on nanostructured TiO2 by solvothermal route. The time-dependent growth of CdSe is observed in solution at room temperature, which is found to be accomplished instantly by heat-treatment in the presence of solvent at 1 atm. However, no crystal growth occurs upon heat-treatment in the absence of solvent. The nanoscale solvothermal growth of CdSe quantum dot is realized on the nanocrystalline oxide surface, where Cd(NO3)2.4H2O and Na2SeSO3 solutions are sequentially spun on nanostructured TiO2, followed by heat-treatment at temperatures ranging from 100 °C to 250 °C. Size of CdSe increases from 4.4 nm to 5.3 nm, 8.7 nm and 14.8 nm, which results in decrease in optical band gap from 2.19 eV to, 1.95 eV, 1.74 eV and 1.75 eV with increasing the NSR temperature from 100 °C to 150 °C, 200 °C and 250 °C, respectively, which is indicative of the quantum confinement effect. Thermodynamic studies reveal that increase in the size of CdSe is related to increase in enthalpy, for instance, from 3.77 J mg-1 for 100 °C to 8.66 J mg-1 for 200 °C. Quantum confinement effect is further confirmed from the CdSe-sensitized solar cell, where onset wavelength in external quantum efficiency spectra is progressively shifted from 600 nm to 800 nm as the NSR temperature increases, which leads to a significant improvement of power conversion efficiency by a factor of more than four. A high photocurrent density of 13.7 mA cm-2 is obtained based on CdSe quantum dot grown by NSR at 200 °C.

  2. Direct growth of CdSe semiconductor quantum dots in glass matrix by femtosecond laser beam

    NASA Astrophysics Data System (ADS)

    Bell, G.; Filin, A. I.; Romanov, D. A.; Levis, R. J.

    2016-02-01

    Controllable, spatially inhomogeneous distributions of CdSe nanocrystals smaller than the exciton Bohr radius are grown in a glass matrix under combined action of sample heating (below the transformation temperature) and focused high-repetition femtosecond (fs) laser beam. Selective quantum dot precipitation is evidenced by position-dependent absorption and Raman spectra. The particle size is estimated as r = 2.1 ± 0.3 nm by comparing the measured absorption and Raman spectra with those obtained from the samples grown in glass by traditional heat-treatment procedure. Direct growth of CdSe quantum dots in glass is enabled by nonlinear excitation using a focused fs duration laser beam (as differentiated from other methods), and this opens an avenue for adjustable selective growth patterns.

  3. Photostability of CdSe quantum dots functionalized with aromatic dithiocarbamate ligands.

    PubMed

    Tan, Yizheng; Jin, Song; Hamers, Robert J

    2013-12-26

    Organic ligands are widely used to enhance the ability of CdSe quantum dots (QDs) to resist photodegradation processes such as photo-oxidation. Because long alkyl chains may adversely affect the performance of QD devices that require fast and efficient charge transfer, shorter aromatic ligands are of increasing interest. In this work, we characterize the formation of phenyl dithiocarbamate (DTC) adducts on CdSe surfaces and the relative effectiveness of different para-substituted phenyl dithiocarbamates to enhance the aqueous photostability of CdSe QDs on TiO2. Optical absorption and photoluminescence measurements show that phenyl DTC ligands can be highly effective at reducing QD photocorrosion in water, and that ligands bearing electron-donating substituents are the most effective. A comparison of the QD photostability resulting from use of ligands bearing DTC versus thiol surface-binding groups shows that the DTC group provides greater QD photostability. Density functional calculations with natural bond order analysis show that the effectiveness of substituted phenyl DTC results from the ability of these ligands to remove positive charge away from the CdSe and to delocalize positive charge on the ligand. PMID:24256318

  4. Influence of Surfactants and Charges on CdSe Quantum Dots

    SciTech Connect

    Yang, Ping; Tretiak, Sergei; Ivanov, Sergei

    2011-01-01

    Surface effects significantly influence the functionality of semiconductor nanocrystals. High quality nanocrystals can be achieved with good control of surface passivation by various hydrophobic ligands. In this work, the chemistry between CdSe quantum dots and common surface capping ligands is investigated using density functional theory (DFT). We discuss the electronic structures and optical properties of small CdSe clusters controlled by their size of particle, self-organization, capping ligands, and positive charges. The chosen model ligands reproduce good structural and energetic description of the interactions between the ligands and quantum dots. In order to capture the chemical nature and energetics of the interactions between the capping ligands and CdSe quantum dots, we found that PMe3 is needed to adequately model trioctylphosphine (TOP), NH3 is sufficient for amines, while OPH2Me could be used to model trioctylphosphine oxide. The relative binding interaction strength between ligands was found to decrease in order Cd–O > Cd–N > Cd–P with average binding energy per ligand being -25 kcal/mol for OPH₂Me, -20 kcal/mol for NH₃ and -10 kcal/mol for PMe₃. Charges on studied stoichiometric clusters were found to have a significant effect on their structures, binding energies, and optical properties.

  5. CdTe and CdSe quantum dots: synthesis, characterizations and applications in agriculture

    NASA Astrophysics Data System (ADS)

    Dieu Thuy Ung, Thi; Tran, Thi Kim Chi; Nga Pham, Thu; Nghia Nguyen, Duc; Khang Dinh, Duy; Liem Nguyen, Quang

    2012-12-01

    This paper highlights the results of the whole work including the synthesis of highly luminescent quantum dots (QDs), characterizations and testing applications of them in different kinds of sensors. Concretely, it presents: (i) the successful synthesis of colloidal CdTe and CdSe QDs, their core/shell structures with single- and/or double-shell made by CdS, ZnS or ZnSe/ZnS; (ii) morphology, structural and optical characterizations of the synthesized QDs; and (iii) testing examples of QDs as the fluorescence labels for agricultural-bio-medical objects (for tracing residual pesticide in agricultural products, residual clenbuterol in meat/milk and for detection of H5N1 avian influenza virus in breeding farms). Overall, the results show that the synthesized QDs have very good crystallinity, spherical shape and strongly emit at the desired wavelengths between ˜500 and 700 nm with the luminescence quantum yield (LQY) of 30-85%. These synthesized QDs were used in fabrication of the three testing fluorescence QD-based sensors for the detection of residual pesticides, clenbuterol and H5N1 avian influenza virus. The specific detection of parathion methyl (PM) pesticide at a content as low as 0.05 ppm has been realized with the biosensors made from CdTe/CdS and CdSe/ZnSe/ZnS QDs and the acetylcholinesterase (AChE) enzymes. Fluorescence resonance energy transfer (FRET)-based nanosensors using CdTe/CdS QDs conjugated with 2-amino-8-naphthol-6-sulfonic acid were fabricated that enable detection of diazotized clenbuterol at a content as low as 10 pg ml-1. For detection of H5N1 avian influenza virus, fluorescence biosensors using CdTe/CdS QDs bound on the surface of chromatophores extracted and purified from bacteria Rhodospirillum rubrum were prepared and characterized. The specific detection of H5N1 avian influenza virus in the range of 3-50 ng μl-1 with a detection limit of 3 ng μL-1 has been performed based on the antibody-antigen recognition.

  6. Templating growth of gold nanostructures with a CdSe quantum dot array.

    PubMed

    Paul, Neelima; Metwalli, Ezzeldin; Yao, Yuan; Schwartzkopf, Matthias; Yu, Shun; Roth, Stephan V; Müller-Buschbaum, Peter; Paul, Amitesh

    2015-06-01

    In optoelectronic devices based on quantum dot arrays, thin nanolayers of gold are preferred as stable metal contacts and for connecting recombination centers. The optimal morphology requirements are uniform arrays with precisely controlled positions and sizes over a large area with long range ordering since this strongly affects device performance. To understand the development of gold layer nanomorphology, the detailed mechanism of structure formation are probed with time-resolved grazing incidence small-angle X-ray scattering (GISAXS) during gold sputter deposition. Gold is sputtered on a CdSe quantum dot array with a characteristic quantum dot spacing of ≈7 nm. In the initial stages of gold nanostructure growth, a preferential deposition of gold on top of quantum dots occurs. Thus, the quantum dots act as nucleation sites for gold growth. In later stages, the gold nanoparticles surrounding the quantum dots undergo a coarsening to form a complete layer comprised of gold-dot clusters. Next, growth proceeds dominantly via vertical growth of gold on these gold-dot clusters to form an gold capping layer. In this capping layer, a shift of the cluster boundaries due to ripening is found. Thus, a templating of gold on a CdSe quantum dot array is feasible at low gold coverage.

  7. Green synthesis of highly efficient CdSe quantum dots for quantum-dots-sensitized solar cells

    NASA Astrophysics Data System (ADS)

    Gao, Bing; Shen, Chao; Zhang, Bo; Zhang, Mengya; Yuan, Shuanglong; Yang, Yunxia; Chen, Guorong

    2014-05-01

    Green synthesis of CdSe quantum dots for application in the quantum-dots-sensitized solar cells (QDSCs) is investigated in this work. The CdSe QDs were prepared with glycerol as the solvent, with sharp emission peak, full width at half maximum around 30 nm, and absorption peak from 475 nm to 510 nm. The reaction is environmental friendly and energy saving. What's more, the green synthesized CdSe QDs are coherence to the maximum remittance region of the solar spectrum and suitable as sensitizers to assemble onto TiO2 electrodes for cell devices application. What's more, the dynamic procedure of the carriers' excitation, transportation, and recombination in the QDSCs are discussed. Because the recombination of the electrons from the conduction band of TiO2's to the electrolyte affects the efficiency of the solar cells greatly, 3-Mercaptopropionic acid capped water-dispersible QDs were used to cover the surface of TiO2. The resulting green synthesized CdSe QDSCs with Cu2S as the electrode show a photovoltaic performance with a conversion efficiency of 3.39%.

  8. Green synthesis of highly efficient CdSe quantum dots for quantum-dots-sensitized solar cells

    SciTech Connect

    Gao, Bing; Shen, Chao; Zhang, Mengya; Yuan, Shuanglong; Yang, Yunxia E-mail: grchen@ecust.edu.cn; Chen, Guorong E-mail: grchen@ecust.edu.cn; Zhang, Bo

    2014-05-21

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

  9. Optical properties of water soluble CdSe quantum dots modified by a novel biopolymer based on sodium alginate.

    PubMed

    Bardajee, Ghasem Rezanejade; Hooshyar, Zari

    2013-10-01

    Water soluble CdSe quantum dots (QDs) were modified using a novel biopolymer based on the graft copolymerization of poly (acrylic acid) as a monomer onto sodium alginate as a backbone at room temperature. The obtained CdSe QDs were characterized by Fourier transform infrared spectrometer, thermo-gravimetry analysis, transmission electron microscopy, and dynamic light scattering. Optical properties of the prepared CdSe QDs were investigated by absorption and fluorescence spectra. It was found that the resultant QDs incredibly exhibited high fluorescence intensity and quantum yields. Lastly, the influence of the aging time on the fluorescence intensity of the modified CdSe QDs was studied by their fluorescence spectra. Due to the optical behavior of this modified QDs; it could be of potential interest in biological systems.

  10. Photophysical properties of CdSe quantum dot self-assemblies with zinc phthalocyanines and azaphthalocyanines.

    PubMed

    Suchánek, Jan; Lang, Kamil; Novakova, Veronika; Zimcik, Petr; Zelinger, Zdeněk; Kubát, Pavel

    2013-05-01

    The formation of self-assemblies between CdSe quantum dots (QDs) and Zn phthalocyanines (Pc) and azaphthalocyanines (AzaPc) bearing alkylsulfanyl substituents and the photophysical properties of these assemblies were studied using both steady-state and time-resolved luminescence/absorption spectroscopy. The formation of the self-assemblies was accompanied by a blue shift of the Q band of the dyes and by a quenching of the CdSe QDs luminescence. The largest spectral shift of the Q-band was approximately 7 nm and was observed for pentan-3-ylsulfanyl-functionalised phthalocyanine (). Assuming a 1 : 1 stoichiometry, the calculated binding constant was 4 × 10(4) M(-1). Pc substituted with the bulky tert-butylsulfanyl groups (1) exhibited a smaller shift of the Q band. The quenching of the CdSe QDs luminescence by 1 was more effective than that observed for 3. The results indicated that the luminescence quenching may be due to a photoinduced charge transfer between 1 or 3 and the CdSe QDs. In contrast, the AzaPc (2) with the same substituents as 1 had little effect on the QDs luminescence. For all cases, we found an inefficient resonance energy transfer between the attached dyes and the CdSe QD. The formation of the self-assemblies had negligible effects on the photogeneration of the singlet oxygen, O2((1)Δg), that was fully controlled only by the absorption of the light by the macrocycles.

  11. Multicolored silica coated CdSe core/shell quantum dots

    NASA Astrophysics Data System (ADS)

    Goftman, Valentina V.; Markin, Alexey V.; De Saeger, Sarah; Goryacheva, Irina Y.

    2016-04-01

    Silanization is a convenient route to provide water-solubility to the quantum dots (QDs) with different structure. Green, orange and red emitting CdSe-based QDs were synthesized by varying of number and material of wider-band gap shells and fluorescent properties of QDs were characterized before and after silanization. It was shown that structure of the QD influences on the quantum yield of the silanized QDs: the better CdSe core is protected with wider-band gap semiconductor shells, the more fluorescence properties remain after silica coated QD possess. Hence silica coated QDs have a great perspectives for the multiplex analysis.

  12. CdSe Quantum-Dot-Sensitized Solar Cell with ~100% Internal Quantum Efficiency

    SciTech Connect

    Fuke, Nobuhiro; Hoch, Laura B.; Koposov, Alexey Y.; Manner, Virginia W.; Werder, Donald J.; Fukui, Atsushi; Koide, Naoki; Katayama, Hiroyuki; Sykora, Milan

    2010-10-20

    We have constructed and studied photoelectrochemical solar cells (PECs) consisting of a photoanode prepared by direct deposition of independently synthesized CdSe nanocrystal quantum dots (NQDs) onto a nanocrystalline TiO2 film (NQD/TiO2), aqueous Na2S or Li2S electrolyte, and a Pt counter electrode. We show that light harvesting efficiency (LHE) of the NQD/TiO2 photoanode is significantly enhanced when the NQD surface passivation is changed from tri-n-octylphosphine oxide (TOPO) to 4-butylamine (BA). In the PEC the use of NQDs with a shorter passivating ligand, BA, leads to a significant enhancement in both the electron injection efficiency at the NQD/TiO2 interface and charge collection efficiency at the NQD/electrolyte interface, with the latter attributed mostly to a more efficient diffusion of the electrolyte through the pores of the photoanode. We show that by utilizing BA-capped NQDs and aqueous Li2S as an electrolyte, it is possible to achieve ~100% internal quantum efficiency of photon-to-electron conversion, matching the performance of dye-sensitized solar cells.

  13. Thermodynamic Equilibrium-Driven Formation of Single-Sized Nanocrystals: Reaction Media Tuning CdSe Magic-Sized versus Regular Quantum Dots

    SciTech Connect

    Yu, Kui; Hu, Michael Z.; Wang, Ruibing; Le Piolet, Mickael; Frotey, Marion; Zaman, Md. Badruz; Wu, Xiaohua; Leek, Donald M.; Tao, Ye; Wilkinson, Diana; Li, Chunsheng

    2010-01-01

    A concept for the fundamental science of nanoparticle synthesis, thermodynamic equilibrium-driven formation of colloidal single-sized nanoparticle ensembles, is proposed and demonstrated in this manuscript, which addresses the controlled formation of CdSe magic-sized and regular quantum dots (MSQDs and RQDs). During formation, the former are magic-sized nuclei without further growth in size, while the latter experience nucleation and growth. Both MSQDs and RQDs exhibit bandgap emission, while the former have homogeneous spectra broadening only and the latter both homogeneous and inhomogeneous spectra broadening. The former are single-sized and the latter have size distribution. With continuous and homogeneous nucleation, the thermodynamically driven formation of MSQDs was realized via our one-pot noninjection approach, which features highly synthetic reproducibility and large-scale capability. With the proper tuning of the synthetic parameters, such as the nature of the reaction medium, that affect the thermodynamic equilibria, various CdSe MSQDs and RQDs were synthesized discriminately under otherwise identical synthetic formulation and reaction conditions; the reaction media were noncoordinating 1-octadecene, coordinating trioctylphosphine, and mixtures of the two. The nature of Cd precursors, affected also by the reaction media, plays a major role in the formation of MSQDs versus RQDs. The present investigation on the thermodynamically driven formation of CdSe single-sized nanoparticles via tuning of the reaction medium, mainly, brings novel insights into the formation mechanism and into the surface ligands of the resulting colloidal nanocrystals. More importantly, the present study provides novel experimental design and approaches to single-sized nanoparticles desired for various applications.

  14. Electroluminescence of colloidal quasi-two-dimensional semiconducting CdSe nanostructures in a hybrid light-emitting diode

    SciTech Connect

    Selyukov, A. S. Vitukhnovskii, A. G.; Lebedev, V. S.; Vashchenko, A. A.; Vasiliev, R. B.; Sokolikova, M. S.

    2015-04-15

    We report on the results of studying quasi-two-dimensional nanostructures synthesized here in the form of semiconducting CdSe nanoplatelets with a characteristic longitudinal size of 20–70 nm and a thick-ness of a few atomic layers. Their morphology is studied using TEM and AFM and X-ray diffraction analysis; the crystal structure and sizes are determined. At room and cryogenic temperatures, the spectra and kinetics of the photoluminescence of such structures (quantum wells) are investigated. A hybrid light-emitting diode operating on the basis of CdSe nanoplatelets as a plane active element (emitter) is developed using the organic materials TAZ and TPD to form electron and hole transport layers, respectively. The spectral and current-voltage characteristics of the constructed device with a radiation wavelength λ = 515 nm are obtained. The device triggering voltage is 5.5 V (visible glow). The use of quasi-two-dimensional structures of this type is promising for hybrid light-emitting diodes with pure color and low operating voltages.

  15. Green route synthesis of high quality CdSe quantum dots for applications in light emitting devices

    SciTech Connect

    Bera, Susnata; Singh, Shashi B.; Ray, S.K.

    2012-05-15

    Investigation was made on light emitting diodes fabricated using CdSe quantum dots. CdSe quantum dots were synthesized chemically using olive oil as the capping agent, instead of toxic phosphine. Room temperature photoluminescence investigation showed sharp 1st excitonic emission peak at 568 nm. Bi-layer organic/inorganic (P3HT/CdSe) hybrid light emitting devices were fabricated by solution process. The electroluminescence study showed low turn on voltage ({approx}2.2 V) .The EL peak intensity was found to increase by increasing the operating current. - Graphical abstract: Light emitting diode was fabricated using CdSe quantum dots using olive oil as the capping agent, instead of toxic phosphine. Bi-layer organic/inorganic (P3HT/CdSe) hybrid light emitting device shows strong electroluminescence in the range 630-661 nm. Highlights: Black-Right-Pointing-Pointer CdSe Quantum dots were synthesized using olive oil as the capping agent. Black-Right-Pointing-Pointer Light emitting device was fabricated using CdSe QDs/P3HT polymer heterojunction. Black-Right-Pointing-Pointer The I-V characteristics study showed low turn on voltage at {approx}2.2 V. Black-Right-Pointing-Pointer The EL peak intensity increases with increasing the operating current.

  16. Interaction of the CdSe quantum dots with plant cell walls.

    PubMed

    Djikanović, Daniela; Kalauzi, Aleksandar; Jeremić, Milorad; Xu, Jianmin; Mićić, Miodrag; Whyte, Jeffrey D; Leblanc, Roger M; Radotić, Ksenija

    2012-03-01

    There is an increasing application of quantum dots (QDs) in plant science, as markers for the cells or their cell walls (CWs). In a plant cell the CW is a first target place for external agents. We studied interaction of CdSe QDs with CWs isolated from a conifer -Picea omorika (Panč) Purkynĕ branch. Binding of CdSe QDs was followed by using fluorescence microscopy, fluorescence and FT-IR spectroscopy. The aim of the study was to see whether the QDs induce structural changes in the CW, as well as to find out which kind of interactions between QDs and CWs occur and to which particular constituent polymers QDs preferably bind. The isolated CW is an appropriate object for study of the interactions with nanoparticles. The results show that in the CW, CdSe predominantly binds to cellulose, via OH groups and to lignin, via the conjugated CC/C-C chains. The differences in interaction of wet and dry CWs with QDs/chloroform were also studied. In the reaction of the dry CW sample with QDs/chloroform, hydrophobic interactions are dominant. When water was added after QDs/chloroform, hydrophilic interactions enable a partial reconstruction of the CC chains. The results have an implication on the use of the QDs in plant bio-imaging.

  17. Spin Selective Charge Transport through Cysteine Capped CdSe Quantum Dots.

    PubMed

    Bloom, Brian P; Kiran, Vankayala; Varade, Vaibhav; Naaman, Ron; Waldeck, David H

    2016-07-13

    This work demonstrates that chiral imprinted CdSe quantum dots (QDs) can act as spin selective filters for charge transport. The spin filtering properties of chiral nanoparticles were investigated by magnetic conductive-probe atomic force microscopy (mCP-AFM) measurements and magnetoresistance measurements. The mCP-AFM measurements show that the chirality of the quantum dots and the magnetic orientation of the tip affect the current-voltage curves. Similarly, magnetoresistance measurements demonstrate that the electrical transport through films of chiral quantum dots correlates with the chiroptical properties of the QD. The spin filtering properties of chiral quantum dots may prove useful in future applications, for example, photovoltaics, spintronics, and other spin-driven devices. PMID:27336320

  18. Reversed oxygen sensing using colloidal quantum wells towards highly emissive photoresponsive varnishes

    PubMed Central

    Lorenzon, Monica; Christodoulou, Sotirios; Vaccaro, Gianfranco; Pedrini, Jacopo; Meinardi, Francesco; Moreels, Iwan; Brovelli, Sergio

    2015-01-01

    Colloidal quantum wells combine the advantages of size-tunable electronic properties with vast reactive surfaces that could allow one to realize highly emissive luminescent-sensing varnishes capable of detecting chemical agents through their reversible emission response, with great potential impact on life sciences, environmental monitoring, defence and aerospace engineering. Here we combine spectroelectrochemical measurements and spectroscopic studies in a controlled atmosphere to demonstrate the ‘reversed oxygen-sensing’ capability of CdSe colloidal quantum wells, that is, the exposure to oxygen reversibly increases their luminescence efficiency. Spectroelectrochemical experiments allow us to directly relate the sensing response to the occupancy of surface states. Magneto-optical measurements demonstrate that, under vacuum, heterostructured CdSe/CdS colloidal quantum wells stabilize in their negative trion state. The high starting emission efficiency provides a possible means to enhance the oxygen sensitivity by partially de-passivating the particle surfaces, thereby enhancing the density of unsaturated sites with a minimal cost in term of luminescence losses. PMID:25910499

  19. A novel strategy towards designing a CdSe quantum dot-metallohydrogel composite material.

    PubMed

    Chatterjee, Sayantan; Maitra, Uday

    2016-08-11

    We have described here an efficient method to disperse hydrophobic CdSe quantum dots (QDs) in an aqueous phase using cetyltrimethylammonium bromide (CTAB) micelles without any surface ligand exchange. The water soluble QDs were then embedded in 3D self assembled fibrillar networks (SAFINs) of a hydrogel showing homogeneous dispersibility as evidenced from optical and electron microscopic techniques. The photophysical studies of the hydrogel-QD composite are reported for the first time. These composite materials may have potential applications in biology, optoelectronics, sensors, non-linear optics and materials science.

  20. Electrooptical properties of hybrid liquid crystalline systems containing CdSe quantum dots

    NASA Astrophysics Data System (ADS)

    Dradrach, K.; Bartkiewicz, S.; Miniewicz, A.

    2014-12-01

    In this paper, we present electrooptical properties of hybrid liquid crystalline systems, which contained CdSe quantum dots (QDs). We have shown by experiments of degenerated two-wave mixing and transverse conductivity measurements that liquid crystal cells filled with nematic and doped with semiconductor nanoparticles exhibit photorefractive effect associated with photoconductivity appearing in the system. We also present the mathematical model, which explains the relationship between the photoconductivity of the layer on which the QDs reside and the generation of holographic gratings. Our research may help to develop better understanding of processes observed in such systems and create more efficient materials for holographic data storage.

  1. Electrooptical properties of hybrid liquid crystalline systems containing CdSe quantum dots

    SciTech Connect

    Dradrach, K. Bartkiewicz, S.; Miniewicz, A.

    2014-12-08

    In this paper, we present electrooptical properties of hybrid liquid crystalline systems, which contained CdSe quantum dots (QDs). We have shown by experiments of degenerated two-wave mixing and transverse conductivity measurements that liquid crystal cells filled with nematic and doped with semiconductor nanoparticles exhibit photorefractive effect associated with photoconductivity appearing in the system. We also present the mathematical model, which explains the relationship between the photoconductivity of the layer on which the QDs reside and the generation of holographic gratings. Our research may help to develop better understanding of processes observed in such systems and create more efficient materials for holographic data storage.

  2. CdSe quantum dot-fullerene hybrid nanocomposite for solar energy conversion: electron transfer and photoelectrochemistry.

    PubMed

    Bang, Jin Ho; Kamat, Prashant V

    2011-12-27

    The development of organic/inorganic hybrid nanocomposite systems that enable efficient solar energy conversion has been important for applications in solar cell research. Nanostructured carbon-based systems, in particular C(60), offer attractive strategies to collect and transport electrons generated in a light harvesting assembly. We have assembled CdSe-C(60) nanocomposites by chemically linking CdSe quantum dots (QDs) with thiol-functionalized C(60). The photoinduced charge separation and collection of electrons in CdSe QD-C(60) nanocomposites have been evaluated using transient absorption spectroscopy and photoelectrochemical measurements. The rate constant for electron transfer between excited CdSe QD and C(60) increased with the decreasing size of the CdSe QD (7.9 × 10(9) s(-1) (4.5 nm), 1.7 × 10(10) s(-1) (3.2 nm), and 9.0 × 10(10) s(-1) (2.6 nm)). Slower hole transfer and faster charge recombination and transport events were found to dominate over the forward electron injection process, thus limiting the deliverance of maximum power in CdSe QD-C(60)-based solar cells. The photoinduced charge separation between CdSe QDs and C(60) opens up new design strategies for developing light harvesting assemblies.

  3. Effect of reaction media on the growth and photoluminescence of colloidal CdSe nanocrystals.

    PubMed

    Yu, Kui; Singh, Shanti; Patrito, Natasha; Chu, Virginia

    2004-12-01

    Using cadium oxide (CdO) as the Cd precursor and tri-n-octylphosphine selenide (TOPSe) as the Se source, TOP-capped and TOP/tri-n-octylphosphine oxide (TOPO)-capped CdSe nanocrystals were synthesized without the use of an acid. The synthetic approach involved the addition of a TOPSe/TOP solution into a CdO/TOP solution with or without TOPO at one temperature and subsequent growth at a lower temperature. The temporal evolution of the optical properties, namely, absorption and luminescence, of the growing nanocrystals was monitored in detail. A comprehensive examination on the control of the photoluminescence (PL) properties was performed by systematically varying the TOP/TOPO weight ratio of the reaction media. Surprisingly, a rational choice of 100% TOP or 80% TOP was found to produce "quality" nanocrystals when monitored under the present experimental conditions and growth-time scale. The term "quality" is mainly based on the sharp features and rich substructure exhibited in the absorption spectra of the growing nanocrystals, as well as the sharp features in the emission spectra with narrow full width at half-maximum (fwhm). There are two distinguishable stages of growth: an early stage (<5 min) and a later stage. TOP plays a major role in the control of a slow growth rate in the early stage, while TOPO controls slow growth in the later stage. The optical sensitivity of the growing nanocrystals when dispersed in nonpolar or polar solvents was studied, including two size-dependent parameters, namely, the solvent sensitivity (PL intensity) and nonresonant Stokes shift (NRSS). The insights gained from the present study enable a synthetic approach in which high-quality CdSe nanocrystals are achieved with high synthetic reproducibility.

  4. Efficient intranuclear gene delivery by CdSe aqueous quantum dots electrostatically-coated with polyethyleneimine

    NASA Astrophysics Data System (ADS)

    Au, Giang H. T.; Y Shih, Wan; Shih, Wei-Heng

    2015-01-01

    Quantum dots (QDs) are semiconducting nanoparticles with photoluminescence properties that do not photobleach. Due to these advantages, using QDs for non-viral gene delivery has the additional benefit of being able to track the delivery of the genes in real time as it happens. We investigate the efficacy of mercaptopropionic acid (MPA)-capped CdSe aqueous quantum dots (AQDs) electrostatically complexed with branched polyethyleneimine (PEI) both as a non-viral gene delivery vector and as a fluorescent probe for tracking the delivery of genes into nuclei. The MPA-capped CdSe AQDs that were completely synthesized in water were the model AQDs. A nominal MPA:Cd:Se = 4:3:1 was chosen for optimal photoluminescence and zeta potential. The gene delivery study was carried out in vitro using a human colon cancer cell line, HT29 (ATCC). The model gene was a plasmid DNA (pDNA) that can express red fluorescent protein (RFP). Positively charged branched PEI was employed to provide a proton buffer to the AQDs to allow for endosomal escape. It is shown that by using a PEI-AQD complex with a PEI/AQD molar ratio of 300 and a nominal pDNA/PEI-AQD ratio of 6, we can achieve 75 ± 2.6% RFP expression efficiency with cell vitality remaining at 78 ± 4% of the control.

  5. Comparison of three empirical force fields for phonon calculations in CdSe quantum dots.

    PubMed

    Kelley, Anne Myers

    2016-06-01

    Three empirical interatomic force fields are parametrized using structural, elastic, and phonon dispersion data for bulk CdSe and their predictions are then compared for the structures and phonons of CdSe quantum dots having average diameters of ˜2.8 and ˜5.2 nm (˜410 and ˜2630 atoms, respectively). The three force fields include one that contains only two-body interactions (Lennard-Jones plus Coulomb), a Tersoff-type force field that contains both two-body and three-body interactions but no Coulombic terms, and a Stillinger-Weber type force field that contains Coulombic interactions plus two-body and three-body terms. While all three force fields predict nearly identical peak frequencies for the strongly Raman-active "longitudinal optical" phonon in the quantum dots, the predictions for the width of the Raman peak, the peak frequency and width of the infrared absorption peak, and the degree of disorder in the structure are very different. The three force fields also give very different predictions for the variation in phonon frequency with radial position (core versus surface). The Stillinger-Weber plus Coulomb type force field gives the best overall agreement with available experimental data.

  6. Hybrid passivated colloidal quantum dot solids

    NASA Astrophysics Data System (ADS)

    Ip, Alexander H.; Thon, Susanna M.; Hoogland, Sjoerd; Voznyy, Oleksandr; Zhitomirsky, David; Debnath, Ratan; Levina, Larissa; Rollny, Lisa R.; Carey, Graham H.; Fischer, Armin; Kemp, Kyle W.; Kramer, Illan J.; Ning, Zhijun; Labelle, André J.; Chou, Kang Wei; Amassian, Aram; Sargent, Edward H.

    2012-09-01

    Colloidal quantum dot (CQD) films allow large-area solution processing and bandgap tuning through the quantum size effect. However, the high ratio of surface area to volume makes CQD films prone to high trap state densities if surfaces are imperfectly passivated, promoting recombination of charge carriers that is detrimental to device performance. Recent advances have replaced the long insulating ligands that enable colloidal stability following synthesis with shorter organic linkers or halide anions, leading to improved passivation and higher packing densities. Although this substitution has been performed using solid-state ligand exchange, a solution-based approach is preferable because it enables increased control over the balance of charges on the surface of the quantum dot, which is essential for eliminating midgap trap states. Furthermore, the solution-based approach leverages recent progress in metal:chalcogen chemistry in the liquid phase. Here, we quantify the density of midgap trap states in CQD solids and show that the performance of CQD-based photovoltaics is now limited by electron-hole recombination due to these states. Next, using density functional theory and optoelectronic device modelling, we show that to improve this performance it is essential to bind a suitable ligand to each potential trap site on the surface of the quantum dot. We then develop a robust hybrid passivation scheme that involves introducing halide anions during the end stages of the synthesis process, which can passivate trap sites that are inaccessible to much larger organic ligands. An organic crosslinking strategy is then used to form the film. Finally, we use our hybrid passivated CQD solid to fabricate a solar cell with a certified efficiency of 7.0%, which is a record for a CQD photovoltaic device.

  7. Hybrid passivated colloidal quantum dot solids.

    PubMed

    Ip, Alexander H; Thon, Susanna M; Hoogland, Sjoerd; Voznyy, Oleksandr; Zhitomirsky, David; Debnath, Ratan; Levina, Larissa; Rollny, Lisa R; Carey, Graham H; Fischer, Armin; Kemp, Kyle W; Kramer, Illan J; Ning, Zhijun; Labelle, André J; Chou, Kang Wei; Amassian, Aram; Sargent, Edward H

    2012-09-01

    Colloidal quantum dot (CQD) films allow large-area solution processing and bandgap tuning through the quantum size effect. However, the high ratio of surface area to volume makes CQD films prone to high trap state densities if surfaces are imperfectly passivated, promoting recombination of charge carriers that is detrimental to device performance. Recent advances have replaced the long insulating ligands that enable colloidal stability following synthesis with shorter organic linkers or halide anions, leading to improved passivation and higher packing densities. Although this substitution has been performed using solid-state ligand exchange, a solution-based approach is preferable because it enables increased control over the balance of charges on the surface of the quantum dot, which is essential for eliminating midgap trap states. Furthermore, the solution-based approach leverages recent progress in metal:chalcogen chemistry in the liquid phase. Here, we quantify the density of midgap trap states in CQD solids and show that the performance of CQD-based photovoltaics is now limited by electron-hole recombination due to these states. Next, using density functional theory and optoelectronic device modelling, we show that to improve this performance it is essential to bind a suitable ligand to each potential trap site on the surface of the quantum dot. We then develop a robust hybrid passivation scheme that involves introducing halide anions during the end stages of the synthesis process, which can passivate trap sites that are inaccessible to much larger organic ligands. An organic crosslinking strategy is then used to form the film. Finally, we use our hybrid passivated CQD solid to fabricate a solar cell with a certified efficiency of 7.0%, which is a record for a CQD photovoltaic device.

  8. Quantum-confined emission and fluorescence blinking of individual exciton complexes in CdSe nanowires.

    PubMed

    Franz, Dennis; Reich, Aina; Strelow, Christian; Wang, Zhe; Kornowski, Andreas; Kipp, Tobias; Mews, Alf

    2014-11-12

    One-dimensional semiconductor nanostructures combine electron mobility in length direction with the possibility of tailoring the physical properties by confinement effects in radial direction. Here we show that thin CdSe quantum nanowires exhibit low-temperature fluorescence spectra with a specific universal structure of several sharp lines. The structure strongly resembles the pattern of bulk spectra but show a diameter-dependent shift due to confinement effects. Also the fluorescence shows a pronounced complex blinking behavior with very different blinking dynamics of different emission lines in one and the same spectrum. Time- and space-resolved optical spectroscopy are combined with high-resolution transmission electron microscopy of the very same quantum nanowires to establish a detailed structure-property relationship. Extensive numerical simulations strongly suggest that excitonic complexes involving donor and acceptor sites are the origin of the feature-rich spectra.

  9. Selective recognition of dysprosium(III) ions by enhanced chemiluminescence CdSe quantum dots.

    PubMed

    Hosseini, Morteza; Ganjali, Mohammad R; Vaezi, Zahra; Faridbod, Farnoush; Arabsorkhi, Batool; Sheikhha, Mohammad H

    2014-01-01

    The intensity of emitted light from CdSe quantum dots (QDs)-H2O2 is described as a novel chemiluminescence (CL) reaction for determination of dysprosium. This reaction is based on the catalytic effect of Dy(3+) ions, causing a significant increase in the light emission, as a result of the reaction of quantum dots (QDs) with hydrogen peroxide. In the optimum conditions, this method was satisfactorily described by linear calibration curve in the range of 8.3×10(-7)-5.0×10(-6)M, the detection limit of 6.0×10(-8)M, and the relative standard deviation for five determinations of 2.5×10(-6)M Dy(3+) 3.2%. The main experimental advantage of the proposed method is its selective to Dy(3+) ions compared with common coexisting cations, therefore, it was successfully applied for the determination of dysprosium ions in water samples.

  10. Charge-extraction strategies for colloidal quantum dot photovoltaics.

    PubMed

    Lan, Xinzheng; Masala, Silvia; Sargent, Edward H

    2014-03-01

    The solar-power conversion efficiencies of colloidal quantum dot solar cells have advanced from sub-1% reported in 2005 to a record value of 8.5% in 2013. Much focus has deservedly been placed on densifying, passivating and crosslinking the colloidal quantum dot solid. Here we review progress in improving charge extraction, achieved by engineering the composition and structure of the electrode materials that contact the colloidal quantum dot film. New classes of structured electrodes have been developed and integrated to form bulk heterojunction devices that enhance photocharge extraction. Control over band offsets, doping and interfacial trap state densities have been essential for achieving improved electrical communication with colloidal quantum dot solids. Quantum junction devices that not only tune the optical absorption spectrum, but also provide inherently matched bands across the interface between p- and n-materials, have proven that charge separation can occur efficiently across an all-quantum-tuned rectifying junction.

  11. Photocurrent enhancement of SiNW-FETs by integrating protein-shelled CdSe quantum dots.

    PubMed

    Moh, Sang Hyun; Kulkarni, Atul; San, Boi Hoa; Lee, Jeong Hun; Kim, Doyoun; Park, Kwang Su; Lee, Min Ho; Kim, Taesung; Kim, Kyeong Kyu

    2016-01-28

    We proposed a new strategy to increase the photoresponsivity of silicon NW field-effect transistors (FETs) by integrating CdSe quantum dots (QDs) using protein shells (PSs). CdSe QDs were synthesized using ClpP, a bacterial protease, as protein shells to control the size and stability of QD and to facilitate the mounting of QDs on SiNWs. The photocurrent of SiNW-FETs in response to light at a wavelength of 480 nm was enhanced by a factor of 6.5 after integrating CdSe QDs because of the coupling of the optical properties of SiNWs and QDs. As a result, the photoresponsivity to 480 nm light reached up to 3.1 × 10(6), the highest value compared to other SiNW-based devices in the visible light range. PMID:26755346

  12. Comparative behavior of CdS and CdSe quantum dots in poly(3-hexylthiophene) based nanocomposites

    SciTech Connect

    Sonar, Prashant . E-mail: sonar@mat.ethz.ch; Sreenivasan, K.P.; Madddanimath, Trupti; Vijayamohanan, K. . E-mail: viji@ems.ncl.res.in

    2006-01-05

    CdS and CdSe nanoparticles have been prepared using conducting poly(3-hexylthiophene) (P3HT) matrix with an objective to understand the effect of nanoparticles on the polymer matrix using electrochemical and spectroscopic techniques. The spectroscopic results reveal that the electronic structure of polymer is strongly influenced by the characteristics of embedded semiconducting nanoparticles. SEM and TEM images show the ordered morphology of the CdS and CdSe nanoparticles in presence of the polymer matrix. Cyclic voltammetry performed both in the presence and absence of light enables us to understand the redox changes in P3HT due to CdS and CdSe quantum dots such as the generation of free radical in the excited state and their electrochemical band gaps.

  13. Nanoparticle Concentration Effects on Kinetic Stability of CdSe Quantum Dots in Waters

    NASA Astrophysics Data System (ADS)

    Wan, J.; Kim, Y.; Tokunaga, T. K.

    2009-12-01

    Many recent laboratory studies on nanoparticle (NP) behavior used highly concentrated particle suspensions (up to several mM concentrations), largely to overcome instrument detection limits. In potentially engineered-NP impacted aquatic systems NP-concentrations can vary many orders of magnitude lower depending on the pathways of their release. We investigated NP concentration effects on kinetic stability of CdSe quantum dots (QDs), that have CdSe core diameter of 4.4 ±0.2 nm (by TEM), and the mercaptoundecanoic acid (MUA) coatings. The term stability is used to describe resistance to NP aggregation/coagulation and precipitation. We measured stability ratios of varied NP suspension concentrations, 10 to 0.1 mM (atom-based concentrations), under stability-favorable pH condition, and ionic strength (IS) from 1.0 mM to 2.0 M NaCl. In addition to determining short-term stability (10 seconds to 60 minute), we also measured long-term stability, up to 2 months (in order to observe precipitation). The results were compared with DLVO predictions using calculated Hamaker constants for MUA-coated CdSe QDs). Our data indicate that at the high concentrations (≥ 1.4 mM), CdSe QDs are extremely stable under low IS and favorable pH conditions, staying monodispersed for beyond the long experiment duration. Surprisingly, decreasing NP concentrations to < 1.4 mM resulted in rapid coagulation (< 10 seconds) of the primary NPs under the same low IS and stability-favorable pH. Interestingly, after this initial rapid coagulation the aggregates were relatively stable in suspensions, with larger aggregate sizes in more diluted solutions, suspended in water for beyond the long experiment duration. Measured electrokinetic properties of NP suspensions at different concentrations are presented, and mechanisms are discussed. The phenomena observed in this study may be extended to some of other types of charge-stabilized engineered NPs, and their impacts on transport and bioavailability can

  14. Passivation of CdSe Quantum Dots by Graphene and MoS2 Monolayer Encapsulation

    NASA Astrophysics Data System (ADS)

    Zhang, Datong; Wang, Dennis Zi-Ren; Creswell, Richard C.; Lu, Chenguang; Herman, Irving P.

    The encapsulation of a monolayer of CdSe quantum dots (QDs) by one-to-three layer graphene and MoS2 sheets protects the QDs from oxidation. Photoluminescence (PL) from the QD cores shows a much slower decrease in core diameter over time due to slower oxidation in regions where the QDs are covered by van der Waals (vdW) layers than in those where they are not, for chips stored both in the dark and in the presence of light. PL mapping shows that the CdSe QDs under the central part of the vdW sheet age slower than those near its edges, because oxidation of the covered QDs is limited by transport of oxygen from the edges of the vdW sheets and not transport across the vdW layers. This encapsulation effect is also tested with other environments. Preliminary results show that vdW materials could be promising candidates for nano-coating materials for devices operating in extreme environments.

  15. Modulated fluorescence of colloidal quantum dots embedded in a porous alumina membrane.

    PubMed

    Xu, Hao; Li, Li; Manneberg, Otto; Russom, Aman; Gylfason, Kristinn B; Brismar, Hjalmar; Fu, Ying

    2013-11-14

    The fluorescence spectrum of CdSe core-CdS/ZnS shell colloidal quantum dots (QDs) embedded in porous alumina membrane was studied. Small peaks, superimposed on the principal QD fluorescence spectrum, were observed. Finite-difference time-domain simulation indicates that the QD point radiation emitting from within the membrane is strongly modulated by the photonic band structure introduced by the membrane pores, leading to the observed fine spectral features. Moreover, the principal QD fluorescence peak red-shifted when the optical excitation power was increased, which is attributed to QD material heating due to emitted phonons when the photoexcited electron and hole relax nonradiatively from high-energy states to the ground exciton state before fluorescence.

  16. Photocurrent enhancement of SiNW-FETs by integrating protein-shelled CdSe quantum dots

    NASA Astrophysics Data System (ADS)

    Moh, Sang Hyun; Kulkarni, Atul; San, Boi Hoa; Lee, Jeong Hun; Kim, Doyoun; Park, Kwang Su; Lee, Min Ho; Kim, Taesung; Kim, Kyeong Kyu

    2016-01-01

    We proposed a new strategy to increase the photoresponsivity of silicon NW field-effect transistors (FETs) by integrating CdSe quantum dots (QDs) using protein shells (PSs). CdSe QDs were synthesized using ClpP, a bacterial protease, as protein shells to control the size and stability of QD and to facilitate the mounting of QDs on SiNWs. The photocurrent of SiNW-FETs in response to light at a wavelength of 480 nm was enhanced by a factor of 6.5 after integrating CdSe QDs because of the coupling of the optical properties of SiNWs and QDs. As a result, the photoresponsivity to 480 nm light reached up to 3.1 × 106, the highest value compared to other SiNW-based devices in the visible light range.We proposed a new strategy to increase the photoresponsivity of silicon NW field-effect transistors (FETs) by integrating CdSe quantum dots (QDs) using protein shells (PSs). CdSe QDs were synthesized using ClpP, a bacterial protease, as protein shells to control the size and stability of QD and to facilitate the mounting of QDs on SiNWs. The photocurrent of SiNW-FETs in response to light at a wavelength of 480 nm was enhanced by a factor of 6.5 after integrating CdSe QDs because of the coupling of the optical properties of SiNWs and QDs. As a result, the photoresponsivity to 480 nm light reached up to 3.1 × 106, the highest value compared to other SiNW-based devices in the visible light range. Electronic supplementary information (ESI) available: Materials and methods. See DOI: 10.1039/c5nr07901b

  17. Building devices from colloidal quantum dots.

    PubMed

    Kagan, Cherie R; Lifshitz, Efrat; Sargent, Edward H; Talapin, Dmitri V

    2016-08-26

    The continued growth of mobile and interactive computing requires devices manufactured with low-cost processes, compatible with large-area and flexible form factors, and with additional functionality. We review recent advances in the design of electronic and optoelectronic devices that use colloidal semiconductor quantum dots (QDs). The properties of materials assembled of QDs may be tailored not only by the atomic composition but also by the size, shape, and surface functionalization of the individual QDs and by the communication among these QDs. The chemical and physical properties of QD surfaces and the interfaces in QD devices are of particular importance, and these enable the solution-based fabrication of low-cost, large-area, flexible, and functional devices. We discuss challenges that must be addressed in the move to solution-processed functional optoelectronic nanomaterials. PMID:27563099

  18. Electronic structure of cobalt doped CdSe quantum dots using soft X-ray spectroscopy

    SciTech Connect

    Joshua T. Wright; Su, Dong; van Buuren, Tony; Meulenberg, Robert W.

    2014-08-21

    The electronic structure and magnetic properties of cobalt doped CdSe quantum dots (QDs) are studied using electron microscopy, soft X-ray spectroscopy, and magnetometry. Magnetometry measurements suggest these QDs are superparamagnetic, contrary to a spin-glass state observed in the bulk analogue. Moreover, the electron microscopy shows well formed QDs, but with cobalt existing as doped into the QD and as unreacted species not contained in the QD. X-ray absorption measurements at the Co L3-edge suggest that changes in spectra features as a function of particle size can be described considering combination of a cobalt ion in a tetrahedral crystal field and an octahedrally coordinated (impurity) phase. With decreasing particle sizes, the impurity phase increases, suggesting that small QDs can be difficult to dope.

  19. Silver nanowires-based signal amplification for CdSe quantum dots electrochemiluminescence immunoassay.

    PubMed

    Huang, Tingyu; Meng, Qingmin; Jie, Guifen

    2015-04-15

    A novel silver-cysteine hybrid nanowires (SCNWs) with many reactive carboxyl and amine groups were prepared, which enable them to be used as idea signal amplifying labels in bioassays. A large number of CdSe quantum dots (QDs) were loaded on the SCNWs to develop amplified SCNWs-QDs electrochemiluminescence (ECL) signal probe. The PAMAM dendrimer-SCNWs nanohybrids covered on the electrode constructed an effective antibody immobilization matrix and made the immobilized biomolecules hold high stability and bioactivity. Based on the specific sandwich immunoreaction strategy, the detection antibody (Ab2)-SCNWs-QDs ECL signal probe was applied to the sensitive signal-on ECL immunoassay of human IgG. The SCNWs-QDs ECL not only opens promising new ECL emitting species, but also promotes the development of novel ECL signal-transition platforms for biosensing devices.

  20. Photoconductivity of composites based on CdSe quantum dots and low-band-gap polymers

    NASA Astrophysics Data System (ADS)

    Dayneko, Sergey; Linkov, Pavel; Martynov, Igor; Tameev, Alexey; Tedoradze, Marine; Samokhvalov, Pavel; Nabiev, Igor; Chistyakov, Alexander

    2016-05-01

    Photoconductivity of thin layers prepared by spin coating of blends of CdSe quantum dots (QDs) and a low-band-gap polymer PCDTBT or PTB7 has been studied. It has been found that photocurrent in the composites containing QDs of 10-nm in size is significantly higher than in those of containing 5-nm QDs. Analysis of the results showed that the photoresponse of the thin layers is mainly determined by the relative positions of the frontier energy levels of the materials used, organic semiconductors and QDs. Therefore, the ability to tune the relative positions of these levels by varying the QD size is of special importance, thus allowing the optimization of photodetectors and photovoltaic cells.

  1. Radiative rate modification in CdSe quantum dot-coated microcavity

    SciTech Connect

    Veluthandath, Aneesh V.; Bisht, Prem B.

    2015-12-21

    Whispering gallery modes (WGMs) of the microparticles with spherical or cylindrical symmetry have exceptionally high quality factors and small mode volume. Quantum dots (QDs) are zero dimensional systems with variable band gap as well as luminescent properties with applications in photonics. In this paper, the WGMs have been observed in the luminescence spectra of CdSe QD-coated single silica microspheres. Theoretical estimations of variation of resonance frequency, electric field, and Q-values have been done for a multilayer coating of QDs on silica microspheres. Observed WGMs have been identified for their mode number and polarization using Mie theory. Broadening of modes due to material absorption has been observed. Splitting of WGMs has also been observed due to coherent coupling of counter propagating waves in the microcavity due to the presence of QDs. At room temperature, the time-resolved study indicates the modification of the radiative rate due to coupling of WGMs of the microcavity-QD hybrid system.

  2. Optical and Phonon Characterization of Ternary CdSe x S1- x Alloy Quantum Dots

    NASA Astrophysics Data System (ADS)

    Thi, L. A.; Cong, N. D.; Dang, N. T.; Nghia, N. X.; Quang, V. X.

    2016-05-01

    Ternary CdSe x S1- x alloy quantum dots (QDs) were synthesized using a wet chemical method. Their morphology, particle size, structural, optical, and vibrational properties were investigated using transmission electron microscopy, x-ray diffraction, UV-Vis, fluorescence and Raman spectroscopy, respectively. The optical and vibrational properties of the QDs can be controlled by adjusting the Se/S molar ratio. The absorption and emission peaks shift to a longer wavelength range when increasing the Se content. The presence of two CdSe-like and CdS-like longitudinal optical phonon modes was observed. The dependencies of the optical and phonon modes on the Se content are discussed in detail.

  3. Inclusion of CdSe quantum dots on the P-doped emitter of Si solar cells.

    PubMed

    Choi, Jaeho; Parida, Bhaskar; Ji, Hyung Yong; Park, Seungil; Kim, Keunjoo

    2012-07-01

    We investigated Cadium Selenide quantum dots embedded in the Si solar cell in order to improve the efficiency of conventional Si solar cell. CdSe quantum dots with 3 to approximately 4 nm size were printed on the phospho-silicate glass layer grown over the emitter surface of p-n junction Si solar cells during the phosphorous diffusion process. Ohmic contact was formed by the contribution of nanoparticles at the Si emitter in spite of the existance of phospho-silicate glass layer. The enhanced light absorption due to the quantum dots was ranged from 500 to 600 nm where the CdSe nanodots have the corresponding emission wavelength of 560 nm. The efficiency of reference solar cell with the glass layer was measured to be 1.0% and it was increased to 12.72% for the reference sample without the glass layer. Furthermore, the efficiency of CdSe quantum dot sample was measured to be 13.6%. This indicates that the quantum dots play the roles of both the formation of tunneling channel and the enhancement of the light conversion efficiency in the visible spectral range.

  4. Colloidal quantum dot light-emitting devices

    PubMed Central

    Wood, Vanessa; Bulović, Vladimir

    2010-01-01

    Colloidal quantum dot light-emitting devices (QD-LEDs) have generated considerable interest for applications such as thin film displays with improved color saturation and white lighting with a high color rendering index (CRI). We review the key advantages of using quantum dots (QDs) in display and lighting applications, including their color purity, solution processability, and stability. After highlighting the main developments in QD-LED technology in the past 15 years, we describe the three mechanisms for exciting QDs - optical excitation, Förster energy transfer, and direct charge injection - that have been leveraged to create QD-LEDs. We outline the challenges facing QD-LED development, such as QD charging and QD luminescence quenching in QD thin films. We describe how optical downconversion schemes have enabled researchers to overcome these challenges and develop commercial lighting products that incorporate QDs to achieve desirable color temperature and a high CRI while maintaining efficiencies comparable to inorganic white LEDs (>65 lumens per Watt). We conclude by discussing some current directions in QD research that focus on achieving higher efficiency and air-stable QD-LEDs using electrical excitation of the luminescent QDs. PMID:22110863

  5. Small bright charged colloidal quantum dots.

    PubMed

    Qin, Wei; Liu, Heng; Guyot-Sionnest, Philippe

    2014-01-28

    Using electrochemical charge injection, the fluorescence lifetimes of negatively charged core/shell CdTe/CdSe QDs are measured as a function of core size and shell thickness. It is found that the ensemble negative trion lifetimes reach a maximum (∼4.5 ns) for an intermediate shell thickness. This leads to the smallest particles (∼4.5 nm) with the brightest trion to date. Single dot measurements show that the negative charge suppresses blinking and that the trion can be as bright as the exciton at room temperature. In contrast, the biexciton lifetimes remain short and exhibit only a monotonous increase with shell thickness, showing no correlation with the negative trion decays. The suppression of the Auger process in small negatively charged CdTe/CdSe quantum dots is unprecedented and a significant departure from prior results with ultrathick CdSe/CdS core/shell or dot-in-rod structures. The proposed reason for the optimum shell thickness is that the electron-hole overlap is restricted to the CdTe core while the electron is tuned to have zero kinetic energy in the core for that optimum shell thickness. The different trend of the biexciton lifetime is not explained but tentatively attributed to shorter-lived positive trions at smaller sizes. These results improve our understanding of multiexciton recombination in colloidal quantum dots and may lead to the design of bright charged QDs for more efficient light-emitting devices.

  6. Colloidal quantum dot materials for infrared optoelectronics

    NASA Astrophysics Data System (ADS)

    Arinze, Ebuka S.; Nyirjesy, Gabrielle; Cheng, Yan; Palmquist, Nathan; Thon, Susanna M.

    2015-09-01

    Colloidal quantum dots (CQDs) are an attractive material for optoelectronic applications because they combine flexible, low-cost solution-phase synthesis and processing with the potential for novel functionality arising from their nanostructure. Specifically, the bandgap of films composed of arrays of CQDs can be tuned via the quantum confinement effect for tailored spectral utilization. PbS-based CQDs can be tuned throughout the near and mid-infrared wavelengths and are a promising materials system for photovoltaic devices that harvest non-visible solar radiation. The performance of CQD solar cells is currently limited by an absorption-extraction compromise, whereby photon absorption lengths in the near infrared spectral regime exceed minority carrier diffusion lengths in the bulk films. Several light trapping strategies for overcoming this compromise and increasing the efficiency of infrared energy harvesting will be reviewed. A thin-film interference technique for creating multi-colored and transparent solar cells will be presented, and a discussion of designing plasmonic nanomaterials based on earth-abundant materials for integration into CQD solar cells is developed. The results indicate that it should be possible to achieve high absorption and color-tunability in a scalable nanomaterials system.

  7. Synthesis and characterization of CdSe quantum dots dispersed in PVA matrix by chemical route

    NASA Astrophysics Data System (ADS)

    Khan, Zubair M. S. H.; Ganaie, Mohsin; Khan, Shamshad A.; Husain, M.; Zulfequar, M.

    2016-05-01

    CdSe quantum dots using polyvinyl alcohol as a capping agent have been synthesized via a simple heat induced thermolysis technique. The structural analysis of CdSe/PVA thin film was studied by X-ray diffraction, which confirms crystalline nature of the prepared film. The surface morphology and particle size of the prepared sample was studied by Scanning Electron Microscopy (SEM) and Transmission Electron Microscopy (TEM). The SEM studies of CdSe/PVA thin film shows the average size of particles in the form of clusters of several quantum dots in the range of 10-20 nm. The morphology of CdSe/PVA thin film was further examined by TEM. The TEM image shows the fringes of tiny dots with average sizes of 4-7 nm. The optical properties of CdSe/PVA thin film were studied by UV-VIS absorption spectroscopy. The CdSe/PVA quantum dots follow the role of direct transition and the optical band gap is found to be 4.03 eV. From dc conductivity measurement, the observed value of activation energy was found to be 0.71 eV.

  8. Mn2+-Doped CdSe/CdS Core/Multishell Colloidal Quantum Wells Enabling Tunable Carrier-Dopant Exchange Interactions

    NASA Astrophysics Data System (ADS)

    Delikanli, Savas; Scrace, Thomas; Murphy, Joseph; Barman, Biblop; Tsai, Yutsung; Zhang, Peiyao; Hernandez-Martinez, Pedro Ludwig; Christodoulides, Joseph; Cartwright, Alexander N.; Petrou, Athos; Demir, Hilmi Volkan

    We report the manifestations of carrier-dopant exchange interactions in colloidal Mn2+-doped CdSe/CdS core/multishell quantum wells. In our solution-processed quantum well heterostructures, Mn2+ was incorporated by growing a Cd0.985Mn0:015S monolayer shell on undoped CdSe nanoplatelets using the colloidal atomic layer deposition technique. The carrier-magnetic ion exchange interaction effects are tunable through wave function engineering. This is realized by controlling the spatial overlap between the carrier wave functions with the manganese ions through adjusting the location, composition, and number of the CdSe, Cd1-xMnxS, and CdS layers. Our colloidal quantum wells, which exhibit magneto-optical properties analogous to those of epitaxially grown quantum wells, offer new opportunities for solution-processed spin-based semiconductor devices. H.V.D. acknowledges support from EU-FP7 Nanophotonics4Energy NoE, TUBITAK, NRF-CRP-6-2010-02 and A*STAR of Singapore. Work at the University at Buffalo was supported by NSF DMR 1305770.

  9. Computational insights into CdSe quantum dots' interactions with acetate ligands.

    PubMed

    Tamukong, Patrick K; Peiris, Wadumesthrige D N; Kilina, Svetlana

    2016-07-27

    Using density functional theory (DFT) and time-dependent DFT (TDDFT), we investigate the effects of carboxylate groups on the electronic and optical properties of CdSe quantum dots (QDs). We specifically focus on the mechanisms of the binding of the acetate anion to the QD surface with and without excess of Cd(2+) cations. Our calculations show that the most stable ligated conformations are those where an acetate is attached to extra Cd(2+) ion forming a [Cd(2+)(CH3COO(-))] at the QD's surface, while also accompanied by an acetate attached nearby at the surface balancing the overall neutral charge of the system. In contrast, formation of a neutral metal-acetate complex [Cd(2+)(CH3COO(-))2] at the QD surface is found to be the least energetically preferable. A strength of the QD-ligand interaction depends on the solvent, the facet of the QD to which the ligands are attached, and the binding mode - with the bridging mode found to be the most stable conformation for both acetate and cadmium acetate ligands. The cadmium acetate ligands introduce electron trap states at the edge of the conduction band - unoccupied orbitals predominately localized on Cd(2+) ion - that are extremely sensitive to the ligand position and the solvent polarity. Polar solvents like acetonitrile delocalize the electronic density over the entire system and, thus, eliminate trap states. As a result, mixed passivation of the CdSe QDs by pairs of cadmium acetate and acetate ligands provides optimal optical properties with minimal contributions of the ligand-related trap states and optically bright lowest energy transitions. PMID:27406268

  10. Controlled synthesis and optical properties of tunable CdSe quantum dots and effect of pH

    SciTech Connect

    Ratnesh, R. K.; Mehata, Mohan Singh

    2015-09-15

    Cadmium selenide (CdSe) quantum dots (Q-dots) were prepared by using non-coordinating solvent octadecene instead of coordinating agent trioctylphosphine oxide (TOPO). Reaction processes were carried out at various temperatures of 240°, 260°, 280° and 300° C under nitrogen atmosphere. The prepared CdSe Q-dots which are highly stable show uniform size distribution and tunable optical absorption and photoluminescence (PL). The growth temperature significantly influenced the particle size; spectral behavior, energy band gap and PL intensity and the full width at half maxima (FWHM). Three different methods were employed to determine the particle size and the average particle size of the CdSe Q-dots is 3.2 - 4.3 nm, grown at different temperatures. In addition, stable and mono-dispersed water soluble CdSe Q-dots were prepared by the ligand exchange technique. Thus, the water soluble Q-dots, which are sensitive to the basic pH may be important for biological applications.

  11. Size-Dependent Exciton Formation Dynamics in Colloidal Silicon Quantum Dots.

    PubMed

    Bergren, Matthew R; Palomaki, Peter K B; Neale, Nathan R; Furtak, Thomas E; Beard, Matthew C

    2016-02-23

    We report size-dependent exciton formation dynamics within colloidal silicon quantum dots (Si QDs) using time-resolved terahertz (THz) spectroscopy measurements. THz photoconductivity measurements are used to distinguish the initially created hot carriers from excitons that form at later times. At early pump/probe delays, the exciton formation dynamics are revealed by the temporal evolution of the THz transmission. We find an increase in the exciton formation time, from ∼500 to ∼900 fs, as the Si QD diameter is reduced from 7.3 to 3.4 nm and all sizes exhibit slower hot-carrier relaxation times compared to bulk Si. In addition, we determine the THz absorption cross section at early delay times is proportional to the carrier mobility while at later delays is proportional to the exciton polarizability, αX. We extract a size-dependent αX and find an ∼r(4) dependence, consistent with previous reports for quantum-confined excitons in CdSe, InAs, and PbSe QDs. The observed slowing in exciton formation time for smaller Si QDs is attributed to decreased electron-phonon coupling due to increased quantum confinement. These results experimentally verify the modification of hot-carrier relaxation rates by quantum confinement in Si QDs, which likely plays a significant role in the high carrier multiplication efficiency observed in these nanomaterials. PMID:26811876

  12. Enhanced lateral photovoltaic effect observed in CdSe quantum dots embedded structure of Zn/CdSe/Si.

    PubMed

    Lan, Tian; Liu, Shuai; Wang, Hui

    2011-01-01

    The quantum dots (QDs) system has been intensively studied for decades owing to its huge potential for applications. In this Letter, we report a lateral photovoltaic effect (LPE) with a large sensitivity observed in CdSe QDs embedded structure of Zn/CdSe/Si. This result not only enriches applications of the QDs system but also opens a new window to study the carrier dynamics of the QDs system.

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

    PubMed

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

    2016-06-15

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

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

    PubMed

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

    2016-06-15

    Light absorption and electron injection are important criteria determining solar energy conversion efficiency. In this research, monodisperse CdSe quantum dots (QDs) are synthesized with five different diameters, and the size-dependent solar energy conversion efficiency of CdSe quantum dot sensitized solar cell (QDSSCs) is investigated by employing the atomic inorganic ligand, S(2-). Absorbance measurements and transmission electron microscopy show that the diameters of the uniform CdSe QDs are 2.5, 3.2, 4.2, 6.4, and 7.8 nm. Larger CdSe QDs generate a larger amount of charge under the irradiation of long wavelength photons, as verified by the absorbance results and the measurements of the external quantum efficiencies. However, the smaller QDs exhibit faster electron injection kinetics from CdSe QDs to TiO2 because of the high energy level of CBCdSe, as verified by time-resolved photoluminescence and internal quantum efficiency results. Importantly, the S(2-) ligand significantly enhances the electronic coupling between the CdSe QDs and TiO2, yielding an enhancement of the charge transfer rate at the interfacial region. As a result, the S(2-) ligand helps improve the new size-dependent solar energy conversion efficiency, showing best performance with 4.2-nm CdSe QDs, whereas conventional ligand, mercaptopropionic acid, does not show any differences in efficiency according to the size of the CdSe QDs. The findings reported herein suggest that the atomic inorganic ligand reinforces the influence of quantum confinement on the solar energy conversion efficiency of QDSSCs. PMID:27224958

  15. Colloidal quantum dot photodetectors (Presentation Recording)

    NASA Astrophysics Data System (ADS)

    Adinolfi, Valerio; Sargent, Edward H.

    2015-08-01

    Colloidal quantum dots (CQDs) are emerging solution processed materials combining low cost, easy deposition on large and flexible substrates, and bandgap tunability. The latter feature, which allows spectral tuning of the absorption profile of the semiconductor, makes these materials particularly attractive for light detection applications. Lead sulfide (PbS) CQDs, in particular, have shown astonishing performance as a light sensitive material operating at visible and infrared (IR) wavelengths. Early studies of PbS CQDs used as a photosensitive resistor (photoconductor) showed an impressive responsivity - exceeding 1000 A/W - and a detectivity (D*) higher then 10^13 Jones. This impressive D* was preserved in the successive development of the first PbS CQD photodiode, showing the possibility to realize fast - f_3db > 1Mhz - and sensitive IR detectors. Currently, the field is moving toward the development of hybrid devices and phototransitors. PbS CQDs have been combined in field effect transistors (FETs) with graphene and MoS2 channels, showing ultra-high gain (exceeding 10^8 electrons/photons) and high D*. Recently a photo-junction FET (photo-JFET) has been reported that breaks the inherent dark current/gain/bandwidth compromise affecting photoconductive light detectors. With this presentation we offer a broad overview on CQD photodetection highlighting the past achievements, the benefits, the challenges and the prospects for the future research on this field.

  16. Advancing colloidal quantum dot photovoltaic technology

    NASA Astrophysics Data System (ADS)

    Cheng, Yan; Arinze, Ebuka S.; Palmquist, Nathan; Thon, Susanna M.

    2016-06-01

    Colloidal quantum dots (CQDs) are attractive materials for solar cells due to their low cost, ease of fabrication and spectral tunability. Progress in CQD photovoltaic technology over the past decade has resulted in power conversion efficiencies approaching 10%. In this review, we give an overview of this progress, and discuss limiting mechanisms and paths for future improvement in CQD solar cell technology.We briefly summarize nanoparticle synthesis and film processing methods and evaluate the optoelectronic properties of CQD films, including the crucial role that surface ligands play in materials performance. We give an overview of device architecture engineering in CQD solar cells. The compromise between carrier extraction and photon absorption in CQD photovoltaics is analyzed along with different strategies for overcoming this trade-off. We then focus on recent advances in absorption enhancement through innovative device design and the use of nanophotonics. Several light-trapping schemes, which have resulted in large increases in cell photocurrent, are described in detail. In particular, integrating plasmonic elements into CQD devices has emerged as a promising approach to enhance photon absorption through both near-field coupling and far-field scattering effects. We also discuss strategies for overcoming the single junction efficiency limits in CQD solar cells, including tandem architectures, multiple exciton generation and hybrid materials schemes. Finally, we offer a perspective on future directions for the field and the most promising paths for achieving higher device efficiencies.

  17. Optical and Surface Characterization Studies of CdSe Quantum Dots Undergoing Photooxidation

    NASA Astrophysics Data System (ADS)

    Powell, Lauren C. J.

    Realization of the potential of Quantum Dots (QDs) for biological, energy-efficient lighting and energy harvesting applications requires that their long-term photostability be improved, especially with regards to protection from photooxidation. The overarching objective of this project was the determination of the chemical and physical mechanisms of photooxidation of CdSe QDs. Pittsburgh-based Crystalplex, Inc. provided CdSe QDs with different organic ligands for this research. Three integrated in situ and ex situ characterization techniques were used to observe changes in optical behavior, QD morphology, and surface chemistry during photooxidation conditions. Single-molecule fluorescence microscopy experiments were used to observe real-time changes in the photoluminescence (PL) behavior of single QDs with oleic and lauric acid ligands. The QDs are exposed to 1 atm of pure O2, dry Ar, Ar bubbled through DI water, or air in an environmental chamber and excited with a 488 nm light. Changes in PL intensities were analyzed with respect to the periods of exposure to controlled atmospheres and light. Samples illuminated continuously exhibited strong photoenhancement effects, while those kept in the dark showed atmospheric-dependent PL loss. Microstructural and chemical identification was performed with aberration-corrected transmission electron microscopy (TEM). Ex situ exposures of QD samples to air, dry O2, and dry Ar revealed changes in surface oxide growth with respect to exposure length, illumination, and column vacuum pressure. Samples exposed to air and light exhibited the most extensive photooxidation. Quantum dots with oleic acid ligands were treated with UV/ozone plasma, and extensive degradation of QDs was observed. X-ray photoemission spectroscopy (XPS) measurements at CMU were used to identify the chemical and bonding states of the surface species before and after photooxidation. Analysis of the acquired spectra showed that exposure to below-bandgap light

  18. Thiolated DAB dendrimers and CdSe quantum dots nanocomposites for Cd(II) or Pb(II) sensing.

    PubMed

    Algarra, M; Campos, B B; Alonso, B; Miranda, M S; Martínez, A M; Casado, C M; Esteves da Silva, J C G

    2012-01-15

    Four different generation of thiol-DAB dendrimers were synthesized, S-DAB-G(x) (x=1, 2, 3 and 5), and coupled with CdSe quantum dots, to obtain fluorescent nanocomposites as metal ions sensing. Cd(II) and Pb(II) showed the higher enhancement and quenching effects respectively towards the fluorescence of S-DAB-G(5)-CdSe nanocomposite. The fluorescence enhancement provoked by Cd(II) can be linearized using a Henderson-Hasselbalch type equation and the quenching provoked by Pb(II) can be linearized by a Stern-Volmer equation. The sensor responds to Cd(II) ion in the 0.05-0.7μM concentration range and to Pb(II) ion in the 0.01-0.15mM concentration range with a LOD of 0.06mM. The sensor has selectivity limitations but its dendrimer configuration has analytical advantages.

  19. CdSe quantum dots-poly(3-hexylthiophene) nanocomposite sensors for selective chloroform vapor detection at room temperature

    NASA Astrophysics Data System (ADS)

    Mondal, S. P.; Bera, S.; Narender, G.; Ray, S. K.

    2012-10-01

    Olive oil capped CdSe quantum dots (QDs) of average size ˜6 nm have been grown by a green chemical route synthesis for the fabrication of nanocomposite organic vapor sensing devices. A highly selective, room temperature chloroform vapor sensor has been fabricated using capped CdSe QDs and conducting polymer [poly(3-hexylthiophene)] nanocomposites. The nanocomposite sensor has been tested with the choloroform vapor of concentration varying from 100-1200 ppm at room temperature using different bias voltages. The recovery time of the sensor has been found to be improved on illumination with a monochromatic light of 600 nm, due to the photo-induced enhancement of charge transfer in nanocomposites.

  20. Increased carrier mobility and lifetime in CdSe quantum dot thin films through surface trap passivation and doping.

    PubMed

    Straus, Daniel B; Goodwin, E D; Gaulding, E Ashley; Muramoto, Shin; Murray, Christopher B; Kagan, Cherie R

    2015-11-19

    Passivating surface defects and controlling the carrier concentration and mobility in quantum dot (QD) thin films is prerequisite to designing electronic and optoelectronic devices. We investigate the effect of introducing indium in CdSe QD thin films on the dark mobility and the photogenerated carrier mobility and lifetime using field-effect transistor (FET) and time-resolved microwave conductivity (TRMC) measurements. We evaporate indium films ranging from 1 to 11 nm in thickness on top of approximately 40 nm thick thiocyanate-capped CdSe QD thin films and anneal the QD films at 300 °C to densify and drive diffusion of indium through the films. As the amount of indium increases, the FET and TRMC mobilities and the TRMC lifetime increase. The increase in mobility and lifetime is consistent with increased indium passivating midgap and band-tail trap states and doping the films, shifting the Fermi energy closer to and into the conduction band. PMID:26536065

  1. Spectroscopic properties of colloidal indium phosphide quantum wires

    SciTech Connect

    Wang, Lin-Wang; Wang, Fudong; Yu, Heng; Li, Jingbo; Hang, Qingling; Zemlyanov, Dmitry; Gibbons, Patrick C.; Wang, Lin-Wang; Janes, David B.; Buhro, William E.

    2008-07-11

    Colloidal InP quantum wires are grown by the solution-liquid-solid (SLS) method, and passivated with the traditional quantum dots surfactants 1-hexadecylamine and tri-n-octylphosphine oxide. The size dependence of the band gaps in the wires are determined from the absorption spectra, and compared to other experimental results for InP quantum dots and wires, and to the predictions of theory. The photoluminescence behavior of the wires is also investigated. Efforts to enhance photoluminescence efficiencies through photochemical etching in the presence of HF result only in photochemical thinning or photo-oxidation, without a significant influence on quantum-wire photoluminescence. However, photo-oxidation produces residual dot and rod domains within the wires, which are luminescent. The results establish that the quantum-wire band gaps are weakly influenced by the nature of the surface passivation, and that colloidal quantum wires have intrinsically low photoluminescence efficiencies.

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

    PubMed

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

    2012-08-27

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

  3. Enhancement in the photorefractive performance of organic composites photosensitized with functionalized CdSe quantum dots

    NASA Astrophysics Data System (ADS)

    Liang, Yichen; Wang, Wei; Moon, Jong-Sik; Winiarz, Jeffrey G.

    2016-08-01

    Enhancement in the photorefractive (PR) performance of organic composites photosensitized by CdSe quantum dots (QCdSe) passivated with the charge-transport ligands, sulfonated triphenyldiamine (STPD), is reported. This enhancement is primarily attributed to the ability of the passivating ligand, STPD, to facilitate the charge-transfer process between the QCdSe and the triphenyldiamine (TPD) charge-transport matrix. The PR composites exhibited a maximum photocharge-generation efficiency of 0.9% and two-beam coupling gain coefficient of 110 cm-1. These figures of merit represent a significant improvement over similar composites photosensitized with more conventional trioctylphosphine oxide-passivated QCdSe (TQCdSe). Moreover, composites photosensitized with SQCdSe had a faster response time of τ = 128 ms at an electric field of 60 V/μm compared with τ = 982 ms for those containing TQCdSe. Because of the molecular similarity between the STPD passivating groups and the TPD-based charge-transport matrix, concentrations of up to 1.4 wt% of SQCdSe are achieved in PR composites without any detectable phase separation, a considerable improvement over the 0.7 wt% for TQCdSe.

  4. Directed energy transfer in films of CdSe quantum dots: beyond the point dipole approximation.

    PubMed

    Zheng, Kaibo; Žídek, Karel; Abdellah, Mohamed; Zhu, Nan; Chábera, Pavel; Lenngren, Nils; Chi, Qijin; Pullerits, Tõnu

    2014-04-30

    Understanding of Förster resonance energy transfer (FRET) in thin films composed of quantum dots (QDs) is of fundamental and technological significance in optimal design of QD based optoelectronic devices. The separation between QDs in the densely packed films is usually smaller than the size of QDs, so that the simple point-dipole approximation, widely used in the conventional approach, can no longer offer quantitative description of the FRET dynamics in such systems. Here, we report the investigations of the FRET dynamics in densely packed films composed of multisized CdSe QDs using ultrafast transient absorption spectroscopy and theoretical modeling. Pairwise interdot transfer time was determined in the range of 1.5 to 2 ns by spectral analyses which enable separation of the FRET contribution from intrinsic exciton decay. A rational model is suggested by taking into account the distribution of the electronic transition densities in the dots and using the film morphology revealed by AFM images. The FRET dynamics predicted by the model are in good quantitative agreement with experimental observations without adjustable parameters. Finally, we use our theoretical model to calculate dynamics of directed energy transfer in ordered multilayer QD films, which we also observe experimentally. The Monte Carlo simulations reveal that three ideal QD monolayers can provide exciton funneling efficiency above 80% from the most distant layer. Thereby, utilization of directed energy transfer can significantly improve light harvesting efficiency of QD devices.

  5. Probing Interfacial Electronic States in CdSe Quantum Dots using Second Harmonic Generation Spectroscopy

    DOE PAGES

    Doughty, Benjamin L.; Ma, Yingzhong; Shaw, Robert W

    2015-01-07

    Understanding and rationally controlling the properties of nanomaterial surfaces is a rapidly expanding field of research due to the dramatic role they play on the optical and electronic properties vital to light harvesting, emitting and detection technologies. This information is essential to the continued development of synthetic approaches designed to tailor interfaces for optimal nanomaterial based device performance. In this work, closely spaced electronic excited states in model CdSe quantum dots (QDs) are resolved using second harmonic generation (SHG) spectroscopy, and the corresponding contributions from surface species to these states are assessed. Two distinct spectral features are observed in themore » SHG spectra, which are not readily identified in linear absorption and photoluminescence excitation spectra. These features include a weak band at 395 6 nm, which coincides with transitions to the 2S1/2 1Se state, and a much more pronounced band at 423 4 nm arising from electronic transitions to the 1P3/2 1Pe state. Chemical modification of the QD surfaces through oxidation resulted in disappearance of the SHG band corresponding to the 1P3/2 1Pe state, indicating prominent surface contributions. Signatures of deep trap states localized on the surfaces of the QDs are also observed. We further find that the SHG signal intensities depend strongly on the electronic states being probed and their relative surface contributions, thereby offering additional insight into the surface specificity of SHG signals from QDs.« less

  6. Probing Interfacial Electronic States in CdSe Quantum Dots using Second Harmonic Generation Spectroscopy

    SciTech Connect

    Doughty, Benjamin L.; Ma, Yingzhong; Shaw, Robert W

    2015-01-07

    Understanding and rationally controlling the properties of nanomaterial surfaces is a rapidly expanding field of research due to the dramatic role they play on the optical and electronic properties vital to light harvesting, emitting and detection technologies. This information is essential to the continued development of synthetic approaches designed to tailor interfaces for optimal nanomaterial based device performance. In this work, closely spaced electronic excited states in model CdSe quantum dots (QDs) are resolved using second harmonic generation (SHG) spectroscopy, and the corresponding contributions from surface species to these states are assessed. Two distinct spectral features are observed in the SHG spectra, which are not readily identified in linear absorption and photoluminescence excitation spectra. These features include a weak band at 395 6 nm, which coincides with transitions to the 2S1/2 1Se state, and a much more pronounced band at 423 4 nm arising from electronic transitions to the 1P3/2 1Pe state. Chemical modification of the QD surfaces through oxidation resulted in disappearance of the SHG band corresponding to the 1P3/2 1Pe state, indicating prominent surface contributions. Signatures of deep trap states localized on the surfaces of the QDs are also observed. We further find that the SHG signal intensities depend strongly on the electronic states being probed and their relative surface contributions, thereby offering additional insight into the surface specificity of SHG signals from QDs.

  7. SU-E-T-526: On the Linearity, Stability and Beam Energy Dependence of CdSe Quantum Dots as Scintillating Probes

    SciTech Connect

    Delage, M-E; Lecavalier, M-E; Lariviere, D; Allen, C; Beaulieu, L

    2014-06-01

    Purpose: Structure and energy transfer mechanisms confer colloidal quantum dots (cQDs) interesting properties, among them their potential as scintillators. CdSe multi-shell cQDs in powder were investigated under photons irradiation. The purpose of this work is to characterize signal to dose linearity, stability with time and to quantify the dependence of their light output with beam energy. Methods: The cQDs are placed at the extremity of a non-scintillating plastic collecting fiber, with the other extremity connected to an Apogee U2000C CCD camera. The CCD camera collects the fluorescence light from irradiated cQDs from which the delivered dose is extracted. This signal is corrected for Cerenkov contamination at MV energies using the chromatic technique. The detector was irradiated with two devices: Xstrahl 200 orthovoltage unit for 120, 180 and 220 kVp and a Varian Clinac iX for 6 and 23 MV. Results: Linear output response with varying dose is observed for all beam energies with R2 factors > 0,999. Reproducibility measurements were performed at 120 kVp: the same set-up was irradiated at different time intervals (one week and three months). The results showed only a small relative decrease of light output of 3,2 % after a combine deposited dose of approximately 95 Gy. CdSe nanocrystals response has been studied as a function of beam energy. The output increases with decreasing energy from 120 kVp to 6 MV and increase again for 23 MV. This behavior could be explained in part by the cQDs high-Z composition. Conclusion: The fluorescence light output of CdSe cQDs was found to be linear as a function of dose. The results suggest stability of the scintillation output of cQDs over time. The specific composition of cQDs is the main cause of the observed energy dependence. We will further look into particle beam dependence of the cQDs. Bourse d'excellence aux etudes graduees du CRC (Centre de Recherche sur le Cancer, Universite Laval) Bourse d'excellence aux etudes

  8. Tandem structured quantum dot/rod sensitized solar cell based on solvothermal synthesized CdSe quantum dots and rods

    NASA Astrophysics Data System (ADS)

    Golobostanfard, Mohammad Reza; Abdizadeh, Hossein

    2014-06-01

    The quantum dots (QD) and quantum rods (QR) of different sizes, shapes, and crystalline phases are synthesized by modified solvothermal method spontaneously employed stirring system and controlled internal applied pressure. The tandem structure of QDs and QRs as well as tetrapods is formed on hierarchical porous titania photoanode by means of electrophoretic deposition. A tremendous enhancement in efficiency of the cell is obtained in samples synthesized at 220 °C for 24 h due to the formation of tandem structure, utilization of Cu2S/CNT composite cathode, co-sensitization of CdS and CdSe, and beneficial role of QRs in electron lifetime. Smaller size QDs with higher band gaps penetrate deeper through the macro-channels of the hierarchical porous structure, while the QRs and tetrapods with lower band gaps are placed on upper layers. Although the charge injection is improved in smaller QDs, the electron lifetime in QRs is longer mainly due to the higher absorption cross section, proper charge separation, introduction of quasi-one dimensional route for charge transport through QRs, and higher surface area available for regeneration with electrolyte. The cell shows the efficiency of 1.05% with JSC of 4.48 mA cm-2, VOC of 0.45 V, and fill factor of 0.52.

  9. Aqueous-phase linker-assisted attachment of cysteinate(2-)-capped cdse quantum dots to TiO2 for quantum dot-sensitized solar cells.

    PubMed

    Coughlin, Kathleen M; Nevins, Jeremy S; Watson, David F

    2013-09-11

    We have synthesized water-dispersible cysteinate(2-)-capped CdSe nanocrystals and attached them to TiO2 using one-step linker-assisted assembly. Room-temperature syntheses yielded CdSe magic-sized clusters (MSCs) exhibiting a narrow and intense first excitonic absorption band centered at 422 nm. Syntheses at 80 °C yielded regular CdSe quantum dots (RQDs) with broader and red-shifted first excitonic absorption bands. Cysteinate(2-)-capped CdSe MSCs and RQDs adsorbed to bare nanocrystalline TiO2 films from aqueous dispersions. CdSe-functionalized TiO2 films were incorporated into working electrodes of quantum dot-sensitized solar cells (QDSSCs). Short-circuit photocurrent action spectra of QDSSCs corresponded closely to absorptance spectra of CdSe-functionalized TiO2 films. Power-conversion efficiencies were (0.43±0.04)% for MSC-functionalized TiO2 and (0.83±0.11)% for RQD-functionalized TiO2. Absorbed photon-to-current efficiencies under white-light illumination were approximately 0.3 for both MSC- and RQD-based QDSSCs, despite the significant differences in the electronic properties of MSCs and RQDs. Cysteinate(2-) is an attractive capping group and ligand, as it engenders water-dispersibility of CdSe nanocrystals with a range of photophysical properties, enables facile all-aqueous linker-assisted attachment of nanocrystals to TiO2, and promotes efficient interfacial charge transfer.

  10. Understanding the electronic structure of CdSe quantum dot-fullerene (C60) hybrid nanostructure for photovoltaic applications

    NASA Astrophysics Data System (ADS)

    Sarkar, Sunandan; Rajbanshi, Biplab; Sarkar, Pranab

    2014-09-01

    By using the density-functional tight binding method, we studied the electronic structure of CdSe quantum dot(QD)-buckminsterfullerene (C60) hybrid systems as a function of both the size of the QD and concentration of the fullerene molecule. Our calculation reveals that the lowest unoccupied molecular orbital energy level of the hybrid CdSeQD-C60 systems lies on the fullerene moiety, whereas the highest occupied molecular orbital (HOMO) energy level lies either on the QD or the fullerene depending on size of the CdSe QD. We explored the possibility of engineering the energy level alignment by varying the size of the CdSe QD. With increase in size of the QD, the HOMO level is shifted upward and crosses the HOMO level of the C60-thiol molecule resulting transition from the type-I to type-II band energy alignment. The density of states and charge density plot support these types of band gap engineering of the CdSe-C60 hybrid systems. This type II band alignment indicates the possibility of application of this nanohybrid for photovoltaic purpose.

  11. A dry method to synthesize dendritic Ag2Se nanostructures utilizing CdSe quantum dots and Ag thin films.

    PubMed

    Hu, Lian; Zhang, Bingpo; Xu, Tianning; Li, Ruifeng; Wu, Huizhen

    2015-01-01

    Dendritic Ag2Se nanostructures are synthesized in a dry environment by UV irradiating the hybrids composed of CdSe quantum dots (QDs) and silver (Ag). UV irradiation on CdSe QDs induces a photooxidation effect on the QD surface and leads to the formation of SeO2 components. Then SeO2 reacts with the Ag atoms in either Ag film or QD layer to produce the Ag2Se. The growth mechanism of Ag2Se dendrites on solid Ag films is explored and explained by a diffusion limited aggregation model in which the QD layer provides enough freedom for Ag2Se motion. Since the oxidation of the CdSe QDs is the critical step for the Ag2Se dendrites formation this dry chemical interaction between QDs and Ag film can be applied in the study of the QD surface chemical properties. With this dry synthesis method, the Ag2Se dendrites can also be facilely formed at the designed area on Ag substrates. PMID:25483981

  12. A dry method to synthesize dendritic Ag2Se nanostructures utilizing CdSe quantum dots and Ag thin films

    NASA Astrophysics Data System (ADS)

    Hu, Lian; Zhang, Bingpo; Xu, Tianning; Li, Ruifeng; Wu, Huizhen

    2015-01-01

    Dendritic Ag2Se nanostructures are synthesized in a dry environment by UV irradiating the hybrids composed of CdSe quantum dots (QDs) and silver (Ag). UV irradiation on CdSe QDs induces a photooxidation effect on the QD surface and leads to the formation of SeO2 components. Then SeO2 reacts with the Ag atoms in either Ag film or QD layer to produce the Ag2Se. The growth mechanism of Ag2Se dendrites on solid Ag films is explored and explained by a diffusion limited aggregation model in which the QD layer provides enough freedom for Ag2Se motion. Since the oxidation of the CdSe QDs is the critical step for the Ag2Se dendrites formation this dry chemical interaction between QDs and Ag film can be applied in the study of the QD surface chemical properties. With this dry synthesis method, the Ag2Se dendrites can also be facilely formed at the designed area on Ag substrates.

  13. Photonic Enhancement of Colloidal Quantum Dot Photovoltaics

    NASA Astrophysics Data System (ADS)

    Labelle, Andre Jean-Romeo Richard

    Colloidal quantum dots, nanocrystal semiconductors that can be cross-linked and assembled into absorbing thin films, are an attractive material for third-generation photovoltaic applications due to low-cost fabrication and bandgap tunability. As a result of their limited charge transport, these solution-processed thin films suffer from a mismatch in absorption length and charge extraction length. Concepts based on the interdigitation of n- and p-doped layers, approaches that reduce the distance photogenerated carriers must travel before extraction, offer promise on overcoming this limitation. In this thesis, I explore and develop techniques to address the absorption-extraction compromise in CQD materials by implementing nano- and micro-structuring techniques to enhance light absorption in the active film. First, I focus on the development of nanomaterials for light guiding/scattering enhancement in CQD films. For this, I develop a nanostructured gold reflector that, when suitably designed, guides light and traps it within the active film. I show that this yields enhanced broadband absorption with more than 4-fold improvement at the most improved wavelength, which translated into a 34% improvement in photocurrent in a working solar cell. I also show that periodic nanostructures employed for absorption enhancement can lead to improvements in solar cell performance. Limitations in device architecture and film formation, however, prevented significant performance advances for these nano-scale approaches. Regardless, these early results pointed me to a new and more impactful strategy. I focus in on realizing micron-scale structured electrodes to enhance absorption, which I show to be considerably more useful in view of the need to extract charge carriers with high efficiency. I discover that conformal film formation atop these structured electrodes is an absolute prerequisite to enhancing performance. These devices, which I term micro-pyramid CQD cells, provide a 24

  14. Photoluminescence and structural properties of CdSe quantum dot-gelatin composite films

    NASA Astrophysics Data System (ADS)

    Borkovska, L.; Korsunska, N.; Stara, T.; Gudymenko, O.; Kladko, V.; Stroyuk, O.; Raevskaya, A.; Kryshtab, T.

    2014-11-01

    Optical and structural properties of composite films of CdSe quantum dots (QDs) embedded in gelatin matrix have been investigated by photoluminescence (PL), optical absorption and X-ray diffraction (XRD) methods. The optical absorption of the composite in the visible spectral range is found to be determined mainly by light absorption in the QDs. The decrease of the film transparency and the shift of the absorption edge to lower energies observed upon thermal annealing of the films at 140-160 °C are ascribed to the formation of chromophore groups in gelatin matrix. XRD patterns of the composite revealed helix to coil transition in gelatin matrix under thermal annealing of the composite at 100-160 °C. It is found that PL spectra of the composite are dominated by exciton and defect-related emission of the QDs and also contain weak emission of gelatin matrix. It is found that thermal annealing of the composite at 100-160 °C changes PL intensity and produces the shift of the PL bands to lower energies. As the annealed composite was kept in air for several months, the shift of exciton-related PL band position restored partially and the PL intensity increased. It is proposed that the increase of the PL intensity upon the thermal annealing of composite at 140 °C can be used for enhancement of the QD-related PL. Changes that occurred in the PL spectra of composite are ascribed to structural and chemical transformations in gelatin matrix and at the QD/gelatin interface.

  15. A differential dielectric spectroscopy setup to measure the electric dipole moment and net charge of colloidal quantum dots

    SciTech Connect

    Kortschot, R. J.; Bakelaar, I. A.; Erné, B. H.; Kuipers, B. W. M.

    2014-03-15

    A sensitive dielectric spectroscopy setup is built to measure the response of nanoparticles dispersed in a liquid to an alternating electric field over a frequency range from 10{sup −2} to 10{sup 7} Hz. The measured complex permittivity spectrum records both the rotational dynamics due to a permanent electric dipole moment and the translational dynamics due to net charges. The setup consists of a half-transparent capacitor connected in a bridge circuit, which is balanced on pure solvent only, using a software-controlled compensating voltage. In this way, the measured signal is dominated by the contributions of the nanoparticles rather than by the solvent. We demonstrate the performance of the setup with measurements on a dispersion of colloidal CdSe quantum dots in the apolar liquid decalin.

  16. Plasmon-phonon coupling in charged n-type CdSe quantum dots: A THz time-domain spectroscopic study.

    PubMed

    Mandal, Pankaj K; Chikan, Viktor

    2007-08-01

    This work aims to experimentally determine the polarizability of confined electron in CdSe quantum dots (QD). The dielectric response of uncharged and charged CdSe quantum dots (3.2 and 6.3 nm) has been measured using terahertz time-domain spectroscopy in the frequency range of 2.0-7.0 THz. A strong coupling between the surface plasmon and surface phonons appears upon charging the QDs. The absolute polarizability of an electron in 3.2 and 6.3 nm charged QDs are experimentally determined to be 0.5 +/- 0.1 x 10(3) A3 and 14.6 +/- 0.3 x 10(3) A3, respectively, and the values agree reasonably well with theory and the previous experiment. The observed plasmon-phonon coupling is expected to play an important role in electron relaxation in absence of a hole in CdSe QDs.

  17. Colloidal quantum dot solids for solution-processed solar cells

    NASA Astrophysics Data System (ADS)

    Yuan, Mingjian; Liu, Mengxia; Sargent, Edward H.

    2016-03-01

    Solution-processed photovoltaic technologies represent a promising way to reduce the cost and increase the efficiency of solar energy harvesting. Among these, colloidal semiconductor quantum dot photovoltaics have the advantage of a spectrally tuneable infrared bandgap, which enables use in multi-junction cells, as well as the benefit of generating and harvesting multiple charge carrier pairs per absorbed photon. Here we review recent progress in colloidal quantum dot photovoltaics, focusing on three fronts. First, we examine strategies to manage the abundant surfaces of quantum dots, strategies that have led to progress in the removal of electronic trap states. Second, we consider new device architectures that have improved device performance to certified efficiencies of 10.6%. Third, we focus on progress in solution-phase chemical processing, such as spray-coating and centrifugal casting, which has led to the demonstration of manufacturing-ready process technologies.

  18. Nanoscale and Single-Dot Patterning of Colloidal Quantum Dots.

    PubMed

    Xie, Weiqiang; Gomes, Raquel; Aubert, Tangi; Bisschop, Suzanne; Zhu, Yunpeng; Hens, Zeger; Brainis, Edouard; Van Thourhout, Dries

    2015-11-11

    Using an optimized lift-off process we develop a technique for both nanoscale and single-dot patterning of colloidal quantum dot films, demonstrating feature sizes down to ~30 nm for uniform films and a yield of 40% for single-dot positioning, which is in good agreement with a newly developed theoretical model. While first of all presenting a unique tool for studying physics of single quantum dots, the process also provides a pathway toward practical quantum dot-based optoelectronic devices.

  19. Study of optical nonlinearity of CdSe and CdSe@ZnO core-shell quantum dots in nanosecond regime

    NASA Astrophysics Data System (ADS)

    Deepika; Dhar, Rakesh; Mohan, Devendra

    2015-12-01

    Thioglycolic acid capped cadmium selenide (CdSe) and CdSe@ZnO core-shell quantum dots have been synthesized in aqueous phase. The sample was characterized by UV-vis spectrophotometer, TEM and Z-scan technique. The nonlinear optical parameters viz. nonlinear absorption coefficient (β), nonlinear refractive index (n2) and third-order nonlinear susceptibilities (χ3) of quantum dots have been estimated using second harmonic of Nd:YAG laser. The study predicts that CdSe@ZnO quantum dots exhibits strong nonlinearity as compared to core CdSe quantum dots. The nonlinearity in quantum dots is attributed to the presence of resonant excitation and free optical processes. The presence of RSA in these nanoparticles makes them a potential material for the development of optical limiter.

  20. Metal colloids and semiconductor quantum dots: Linear and nonlinear optical properties

    NASA Astrophysics Data System (ADS)

    Henderson, D. O.; My, R.; Tung, Y.; Ueda, A.; Zhu, J.; Collins, W. E.; Hall, Christopher

    1995-08-01

    One aspect of this project involves a collaborative effort with the Solid State Division of ORNL. The thrust behind this research is to develop ion implantion for synthesizing novel materials (quantum dots wires and wells, and metal colloids) for applications in all optical switching devices, up conversion, and the synthesis of novel refractory materials. In general the host material is typically a glass such as optical grade silica. The ions of interest are Au, Ag, Cd, Se, In, P, Sb, Ga and As. An emphasis is placed on host guest interactions between the matrix and the implanted ion and how the matrix effects and implantation parameters can be used to obtain designer level optical devices tailored for specific applications. The specific materials of interest are: CdSe, CdTe, InAs, GaAs, InP, GaP, InSb, GaSb and InGaAs. A second aspect of this research program involves using porous glass (25-200 A) for fabricating materials of finite size. In this part of the program, we are particularly interested in characterizing the thermodynamic and optical properties of these non-composite materials. We also address how phase diagram of the confined material is altered by the interfacial properties between the confined material and the pore wall.

  1. Metal colloids and semiconductor quantum dots: Linear and nonlinear optical properties

    NASA Technical Reports Server (NTRS)

    Henderson, D. O.; My, R.; Tung, Y.; Ueda, A.; Zhu, J.; Collins, W. E.; Hall, Christopher

    1995-01-01

    One aspect of this project involves a collaborative effort with the Solid State Division of ORNL. The thrust behind this research is to develop ion implantion for synthesizing novel materials (quantum dots wires and wells, and metal colloids) for applications in all optical switching devices, up conversion, and the synthesis of novel refractory materials. In general the host material is typically a glass such as optical grade silica. The ions of interest are Au, Ag, Cd, Se, In, P, Sb, Ga and As. An emphasis is placed on host guest interactions between the matrix and the implanted ion and how the matrix effects and implantation parameters can be used to obtain designer level optical devices tailored for specific applications. The specific materials of interest are: CdSe, CdTe, InAs, GaAs, InP, GaP, InSb, GaSb and InGaAs. A second aspect of this research program involves using porous glass (25-200 A) for fabricating materials of finite size. In this part of the program, we are particularly interested in characterizing the thermodynamic and optical properties of these non-composite materials. We also address how phase diagram of the confined material is altered by the interfacial properties between the confined material and the pore wall.

  2. Microsecond-sustained lasing from colloidal quantum dot solids

    PubMed Central

    Adachi, Michael M.; Fan, Fengjia; Sellan, Daniel P.; Hoogland, Sjoerd; Voznyy, Oleksandr; Houtepen, Arjan J.; Parrish, Kevin D.; Kanjanaboos, Pongsakorn; Malen, Jonathan A.; Sargent, Edward H.

    2015-01-01

    Colloidal quantum dots have grown in interest as materials for light amplification and lasing in view of their bright photoluminescence, convenient solution processing and size-controlled spectral tunability. To date, lasing in colloidal quantum dot solids has been limited to the nanosecond temporal regime, curtailing their application in systems that require more sustained emission. Here we find that the chief cause of nanosecond-only operation has been thermal runaway: the combination of rapid heat injection from the pump source, poor heat removal and a highly temperature-dependent threshold. We show microsecond-sustained lasing, achieved by placing ultra-compact colloidal quantum dot films on a thermally conductive substrate, the combination of which minimizes heat accumulation. Specifically, we employ inorganic-halide-capped quantum dots that exhibit high modal gain (1,200 cm−1) and an ultralow amplified spontaneous emission threshold (average peak power of ∼50 kW cm−2) and rely on an optical structure that dissipates heat while offering minimal modal loss. PMID:26493282

  3. Microsecond-sustained lasing from colloidal quantum dot solids.

    PubMed

    Adachi, Michael M; Fan, Fengjia; Sellan, Daniel P; Hoogland, Sjoerd; Voznyy, Oleksandr; Houtepen, Arjan J; Parrish, Kevin D; Kanjanaboos, Pongsakorn; Malen, Jonathan A; Sargent, Edward H

    2015-01-01

    Colloidal quantum dots have grown in interest as materials for light amplification and lasing in view of their bright photoluminescence, convenient solution processing and size-controlled spectral tunability. To date, lasing in colloidal quantum dot solids has been limited to the nanosecond temporal regime, curtailing their application in systems that require more sustained emission. Here we find that the chief cause of nanosecond-only operation has been thermal runaway: the combination of rapid heat injection from the pump source, poor heat removal and a highly temperature-dependent threshold. We show microsecond-sustained lasing, achieved by placing ultra-compact colloidal quantum dot films on a thermally conductive substrate, the combination of which minimizes heat accumulation. Specifically, we employ inorganic-halide-capped quantum dots that exhibit high modal gain (1,200 cm(-1)) and an ultralow amplified spontaneous emission threshold (average peak power of ∼50 kW cm(-2)) and rely on an optical structure that dissipates heat while offering minimal modal loss. PMID:26493282

  4. Momentum Transfer Studies and Studies of Linear and Nonlinear Optical Properties of Metal Colloids and Semiconductor Quantum Dots

    NASA Technical Reports Server (NTRS)

    Collins, W. E.; Burger, A.; Dyer, K.; George, M.; Henderson, D.; Morgan, S.; Mu, R.; Shi, D.; Conner, D; Thompson, E.; Collins, L.; Curry, L.; Mattox, S.; Williams, G.

    1996-01-01

    Phase 1 of this work involved design work on a momentum transfer device. The progress on design and testing will be presented. Phase 2 involved the systematic study of the MPD thruster for dual uses. Though it was designed as a thruster for space vehicles, the characteristics of the plasma make it an excellent candidate for industrial applications. This project sought to characterize the system for use in materials processing and characterization. The surface modification on ZnCdTe, CdTe, and ZnTe will be presented. Phase 3 involved metal colloids and semiconductor quantum dots. One aspect of this project involves a collaborative effort with the Solid State Division of ORNL. The thrust behind this research is to develop ion implantation for synthesizing novel materials (quantum dots wires and wells, and metal colloids) for applications in all optical switching devices, up conversion, and the synthesis of novel refractory materials. The ions of interest are Au, Ag, Cd, Se, In, P, Sb, Ga, and As. The specific materials of interest are: CdSe, CdTe, InAs, GaAs, InP, GaP, InSb, GaSb, and InGaAs. A second aspect of this research program involves using porous glass (25-200 A) for fabricating materials of finite size. The results of some of this work will also be reported.

  5. Fast, sensitive and spectrally tuneable colloidal-quantum-dot photodetectors

    NASA Astrophysics Data System (ADS)

    Clifford, Jason P.; Konstantatos, Gerasimos; Johnston, Keith W.; Hoogland, Sjoerd; Levina, Larissa; Sargent, Edward H.

    2009-01-01

    Solution-processed semiconductors are compatible with a range of substrates, which enables their direct integration with organic circuits, microfluidics, optical circuitry and commercial microelectronics. Ultrasensitive photodetectors based on solution-process colloidal quantum dots operating in both the visible and infrared have been demonstrated, but these devices have poor response times (on the scale of seconds) to changes in illumination, and rapid-response devices based on a photodiode architecture suffer from low sensitivity. Here, we show that the temporal response of these devices is determined by two components-electron drift, which is a fast process, and electron diffusion, which is a slow process. By building devices that exclude the diffusion component, we are able to demonstrate a >1,000-fold improvement in the sensitivity-bandwidth product of tuneable colloidal-quantum-dot photodiodes operating in the visible and infrared.

  6. Effects of morphology, diameter and periodic distance of the Ag nanoparticle periodic arrays on the enhancement of the plasmonic field absorption in the CdSe quantum dots

    NASA Astrophysics Data System (ADS)

    Kohnehpoushi, Saman; Eskandari, Mehdi; Ahmadi, Vahid; Yousefirad, Mansooreh; Nabavi, Elham

    2016-09-01

    In this work, the numerical calculations of plasmonic field absorption of Ag nanoparticles (Ag NPs) periodic arrays in the CdSe quantum dot (QD) film are investigated by the three-dimensional finite difference time domain (FDTD). Diameter (D), periodic distance (P), and morphology effects of Ag NPs are investigated on the improvement of the plasmonic field absorption in CdSe QD film. Results show that plasmonic field absorption in CdSe QD film is enhanced with reduction of D of Ag NPs until 5 nm and reduces thereafter. It is observed that with raising D of Ag NPs, optimum plasmonic field absorption in CdSe QD film is shifted toward the higher P. Moreover, with varying morphology of Ag NPs from spherical to cylindrical, cubic, ringing and pyramid, the plasmonic field absorption is considerably enhanced in CdSe QD film and position of quadrupole plasmon mode (QPPM) is shifted toward further wavelength. For cylindrical Ag NPs, the QPPM intensity increased with raising height (H) until 15 nm and reduces thereafter.

  7. Fabrication of fluorescence-based biosensors from functionalized CdSe and CdTe quantum dots for pesticide detection

    NASA Astrophysics Data System (ADS)

    Tran, Thi Kim Chi; Chinh Vu, Duc; Dieu Thuy Ung, Thi; Yen Nguyen, Hai; Hai Nguyen, Ngoc; Cao Dao, Tran; Nga Pham, Thu; Liem Nguyen, Quang

    2012-09-01

    This paper presents the results on the fabrication of highly sensitive fluorescence biosensors for pesticide detection. The biosensors are actually constructed from the complex of quantum dots (QDs), acetylcholinesterase (AChE) and acetylthiocholine (ATCh). The biosensor activity is based on the change of luminescence from CdSe and CdTe QDs with pH, while the pH is changed with the hydrolysis rate of ATCh catalyzed by the enzyme AChE, whose activity is specifically inhibited by pesticides. Two kinds of QDs were used to fabricate our biosensors: (i) CdSe QDs synthesized in high-boiling non-polar organic solvent and then functionalized by shelling with two monolayers (2-ML) of ZnSe and eight monolayers (8-ML) of ZnS and finally capped with 3-mercaptopropionic acid (MPA) to become water soluble; and (ii) CdTe QDs synthesized in aqueous phase then shelled with CdS. For normal checks the fabricated biosensors could detect parathion methyl (PM) pesticide at very low contents of ppm with the threshold as low as 0.05 ppm. The dynamic range from 0.05 ppm to 1 ppm for the pesticide detection could be expandable by increasing the AChE amount in the biosensor.

  8. Linear and nonlinear optical properties of functionalized CdSe quantum dots prepared by plasma sputtering and wet chemistry.

    PubMed

    Humbert, Christophe; Dahi, Abdellatif; Dalstein, Laetitia; Busson, Bertrand; Lismont, Marjorie; Colson, Pierre; Dreesen, Laurent

    2015-05-01

    We develop an innovative manufacturing process, based on radio-frequency magnetron sputtering (RFMS), to prepare neat CdSe quantum dots (QDs) on glass and silicon substrates and further chemically functionalize them. In order to validate the fabrication protocol, their optical properties are compared with those of QDs obtained from commercial solutions and deposited by wet chemistry on the substrates. Firstly, AFM measurements attest that nano-objects with a mean diameter around 13 nm are located on the substrate after RFMS treatment. Secondly, the UV-Vis absorption study of this deposited layer shows a specific optical absorption band, located at 550 nm, which is related to a discrete energy level of QDs. Thirdly, by using two-color sum-frequency generation (2C-SFG) nonlinear optical spectroscopy, we show experimentally the functionalization efficiency of the RFMS CdSe QDs layer with thiol derived molecules, which is not possible on the QDs layer prepared by wet chemistry due to the surfactant molecules from the native solution. Finally, 2C-SFG spectroscopy, performed at different visible wavelengths, highlights modifications of the vibration mode shape whatever the QDs deposition method, which is correlated to the discrete energy level of the QDs.

  9. Tunable optical properties of colloidal quantum dots in electrolytic environments.

    PubMed

    Ramadurai, D; Kohanpour, B; Alexson, D; Shi, P; Sethuraman, A; Li, Y; Saini, V; Dutta, M; Stroscio, M A

    2004-12-01

    The absorption spectra of colloidal cadmium sulfide quantum dots in electrolytic solutions are found to manifest a shift in the absorption threshold as the concentration of the electrolyte is varied. These results are consistent with a shift in the absorption threshold that would be caused by electrolytic screening of the field caused by the intrinsic spontaneous polarisation of these würtzite structured quantum dots. These electrolyte-dependent absorption properties provide a potential means of gaining insights on the variable extracellular and intracellular electrolytic concentrations that are present in biological systems.

  10. Hybrid light emitting diodes based on solution processed polymers, colloidal quantum dots, and colloidal metal nanoparticles

    NASA Astrophysics Data System (ADS)

    Ma, Xin

    This dissertation focuses on solution-processed light-emitting devices based on polymer, polymer/PbS quantum dot, and polymer/silver nanoparticle hybrid materials. Solution based materials and organic/inorganic hybrid light emitting diodes attracted significant interest recently due to many of their advantages over conventional light emitting diodes (LEDs) including low fabrication cost, flexible, high substrate compatibility, as well as tunable emission wavelength of the quantum dot materials. However, the application of these novel solution processed materials based devices is still limited due to their low performances. Material properties and fabrication parameters need to be carefully examined and understood for further device improvement. This thesis first investigates the impact of solvent property and evaporation rate on the polymer molecular chain morphology and packaging in device structures. Solvent is a key component to make the active material solution for spin coating fabrication process. Their impacts are observed and examined on both polymer blend system and mono-polymer device. Secondly, PbS colloidal quantum dot are introduced to form hybrid device with polymer and to migrate the device emission into near-IR range. As we show, the dithiol molecules used to cross-link quantum dots determine the optical and electrical property of the resulting thin films. By choosing a proper ligand for quantum dot ligand exchange, a high performance polymer/quantum dot hybrid LED is fabricated. In the end, the interaction of polymer exciton with surface plasmon mode in colloidal silver nanoparticles and the use of this effect to enhance solution processed LEDs' performances are investigated.

  11. High performance of Mn-doped CdSe quantum dot sensitized solar cells based on the vertical ZnO nanorod arrays

    NASA Astrophysics Data System (ADS)

    Hou, Juan; Zhao, Haifeng; Huang, Fei; Jing, Qun; Cao, Haibin; Wu, Qiang; Peng, Shanglong; Cao, Guozhong

    2016-09-01

    Doping transition metal ions Mn2+ to semiconductor quantum dots (QDs) are extremely interesting for the development of photovoltaic devices. Quantum dot sensitized solar cells (QDSCs) are able to show promising power conversion efficiencies (PCE) by employing Mn2+ doped QDs. Herein we achieve effective CdS/Mnsbnd CdSe/ZnS QDs co-sensitized vertical ZnO nanorod arrays film that provides an appreciable enhancement in photovoltaic performance. The measured PCE of the solar cells with Mn2+ doped CdSe QDs is 4.14%, which is higher than the efficiency of 2.91% for the solar cells without Mn2+ or a ∼42% increase. The improvement in PCE is ascribed to a higher open-circuit voltage (Voc = 0.74 V) and a superior short-circuit current density (Jsc = 12.6 mA cm-2) with the introduction of Mn2+ into CdSe QDs. The enhancement seen with Mn2+ doped CdSe QDs are investigated and explained by the fact that the enhanced light absorption and reduced charge recombination by the formation of Mnsbnd CdSe passivation layer covering the QDs.

  12. Ultrafast Photoinduced Interfacial Proton Coupled Electron Transfer from CdSe Quantum Dots to 4,4'-Bipyridine.

    PubMed

    Chen, Jinquan; Wu, Kaifeng; Rudshteyn, Benjamin; Jia, Yanyan; Ding, Wendu; Xie, Zhao-Xiong; Batista, Victor S; Lian, Tianquan

    2016-01-27

    Pyridine and derivatives have been reported as efficient and selective catalysts for the electrochemical and photoelectrochemical reduction of CO2 to methanol. Although the catalytic mechanism remains a subject of considerable recent debate, most proposed models involve interfacial proton coupled electron transfer (PCET) to electrode-bound catalysts. We report a combined experimental and theoretical study of the photoreduction of 4,4'-bipyridium (bPYD) using CdSe quantum dots (QDs) as a model system for interfacial PCET. We observed ultrafast photoinduced PCET from CdSe QDs to form doubly protonated [bPYDH2](+•) radical cations at low pH (4-6). Through studies of the dependence of PCET rate on isotopic substitution, pH and bPYD concentration, the radical formation mechanism was identified to be a sequential interfacial electron and proton transfer (ET/PT) process with a rate-limiting pH independent electron transfer rate constant, kint, of 1.05 ± 0.13 × 10(10) s(-1) between a QD and an adsorbed singly protonated [bPYDH](+). Theoretical studies of the adsorption of [bPYDH](+) and methylviologen on QD surfaces revealed important effects of hydrogen bonding with the capping ligand (3-mercaptopropionic acid) on binding geometry and interfacial PCET. In the presence of sacrificial electron donors, this system was shown to be capable of generating [bPYDH2](+•) radical cations under continuous illumination at 405 nm with a steady-state photoreduction quantum yield of 1.1 ± 0.1% at pH 4. The mechanism of bPYD photoreduction reported in this work may provide useful insights into the catalytic roles of pyridine and pyridine derivatives in the electrochemical and photoelectrochemical reduction of CO2. PMID:26713752

  13. Photoinduced electron donor/acceptor processes in colloidal II-VI semiconductor quantum dots and nitroxide free radicals

    NASA Astrophysics Data System (ADS)

    Dutta, Poulami

    Electron transfer (ET) processes are one of the most researched topics for applications ranging from energy conversion to catalysis. An exciting variation is utilizing colloidal semiconductor nanostructures to explore such processes. Semiconductor quantum dots (QDs) are emerging as a novel class of light harvesting, emitting and charge-separation materials for applications such as solar energy conversion. Detailed knowledge of the quantitative dissociation of the photogenerated excitons and the interfacial charge- (electron/hole) transfer is essential for optimization of the overall efficiency of many such applications. Organic free radicals are the attractive counterparts for studying ET to/from QDs because these undergo single-electron transfer steps in reversible fashion. Nitroxides are an exciting class of stable organic free radicals, which have recently been demonstrated to be efficient as redox mediators in dye-sensitized solar cells, making them even more interesting for the aforementioned studies. This dissertation investigates the interaction between nitroxide free radicals TEMPO (2,2,6,6-tetramethylpiperidine-1-oxyl), 4-amino-TEMPO (4-amino- 2,2,6,6-tetramethylpiperidine-1-oxyl) and II-VI semiconductor (CdSe and CdTe) QDs. The nature of interaction in these hybrids has been examined through ground-state UV-Vis absorbance, steady state and time-resolved photoluminescence (PL) spectroscopy, transient absorbance, upconversion photoluminescence spectroscopy and electron paramagnetic resonance (EPR). The detailed analysis of the PL quenching indicates that the intrinsic charge transfer is ultrafast however, the overall quenching is still limited by the lower binding capacities and slower diffusion related kinetics. Careful analysis of the time resolved PL decay kinetics reveal that the decay rate constants are distributed and that the trap states are involved in the overall quenching process. The ultrafast hole transfer from CdSe QDs to 4-Amino TEMPO observed

  14. Parametric interactions in presence of different size colloids in semiconductor quantum plasmas

    SciTech Connect

    Vanshpal, R. Sharma, Uttam; Dubey, Swati

    2015-07-31

    Present work is an attempt to investigate the effect of different size colloids on parametric interaction in semiconductor quantum plasma. Inclusion of quantum effect is being done in this analysis through quantum correction term in classical hydrodynamic model of homogeneous semiconductor plasma. The effect is associated with purely quantum origin using quantum Bohm potential and quantum statistics. Colloidal size and quantum correction term modify the parametric dispersion characteristics of ion implanted semiconductor plasma medium. It is found that quantum effect on colloids is inversely proportional to their size. Moreover critical size of implanted colloids for the effective quantum correction is determined which is found to be equal to the lattice spacing of the crystal.

  15. Hot spot assisted blinking suppression of CdSe quantum dots

    NASA Astrophysics Data System (ADS)

    Lu, Liu; Tong, Xuan; Zhang, Xu; Ren, Naifei; Jiang, Bo; Lu, Haifei

    2016-05-01

    This work compares the blinking of CdSe QDs on glass, single silver nanowire, and double aligned nanowires. The corresponding on-time fractions of these three cases are 50%, 70% and 85% respectively, which indicates that aligned double nanowires shows more efficient suppression than that of single nanowire. This phenomenon is attributed to the higher concentration of hot electron from hot spot between nanowires. Occupation of the non-radiative recombination centers by hot electrons from silver nanowires can be explained for the suppressed blinking behavior. The result has provided a novel pathway of suppressing the blinking behavior of QDs through plasmonic hot spot.

  16. High Efficiency Colloidal Quantum Dot Phosphors

    SciTech Connect

    Kahen, Keith

    2013-12-31

    The project showed that non-Cd containing, InP-based nanocrystals (semiconductor materials with dimensions of ~6 nm) have high potential for enabling next-generation, nanocrystal-based, on chip phosphors for solid state lighting. Typical nanocrystals fall short of the requirements for on chip phosphors due to their loss of quantum efficiency under the operating conditions of LEDs, such as, high temperature (up to 150 °C) and high optical flux (up to 200 W/cm2). The InP-based nanocrystals invented during this project maintain high quantum efficiency (>80%) in polymer-based films under these operating conditions for emission wavelengths ranging from ~530 to 620 nm. These nanocrystals also show other desirable attributes, such as, lack of blinking (a common problem with nanocrystals which limits their performance) and no increase in the emission spectral width from room to 150 °C (emitters with narrower spectral widths enable higher efficiency LEDs). Prior to these nanocrystals, no nanocrystal system (regardless of nanocrystal type) showed this collection of properties; in fact, other nanocrystal systems are typically limited to showing only one desirable trait (such as high temperature stability) but being deficient in other properties (such as high flux stability). The project showed that one can reproducibly obtain these properties by generating a novel compositional structure inside of the nanomaterials; in addition, the project formulated an initial theoretical framework linking the compositional structure to the list of high performance optical properties. Over the course of the project, the synthetic methodology for producing the novel composition was evolved to enable the synthesis of these nanomaterials at a cost approximately equal to that required for forming typical conventional nanocrystals. Given the above results, the last major remaining step prior to scale up of the nanomaterials is to limit the oxidation of these materials during the tens of

  17. Efficient CdSe quantum dot-sensitized solar cells prepared by an improved successive ionic layer adsorption and reaction process.

    PubMed

    Lee, Hyojoong; Wang, Mingkui; Chen, Peter; Gamelin, Daniel R; Zakeeruddin, Shaik M; Grätzel, Michael; Nazeeruddin, Md K

    2009-12-01

    In pursuit of efficient quantum dot (QD)-sensitized solar cells based on mesoporous TiO(2) photoanodes, a new procedure for preparing selenide (Se(2-)) was developed and used for depositing CdSe QDs in situ over TiO(2) mesopores by the successive ionic layer adsorption and reaction (SILAR) process in ethanol. The sizes and density of CdSe QDs over TiO(2) were controlled by the number of SILAR cycles applied. After some optimization of these QD-sensitized TiO(2) films in regenerative photoelectrochemical cells using a cobalt redox couple [Co(o-phen)(3)(2+/3+)], including addition of a final layer of CdTe, over 4% overall efficiencies were achieved at 100 W/m(2) with about 50% IPCE at its maximum. Light-harvesting properties and transient voltage decay/impedance measurements confirmed that CdTe-terminated CdSe QD cells gave better charge-collection efficiencies and kinetic parameters than corresponding CdSe QD cells. In a preliminary study, a CdSe(Te) QD-sensitized TiO(2) film was combined with an organic hole conductor, spiro-OMeTAD, and shown to exhibit a promising efficiency of 1.6% at 100 W/m(2) in inorganic/organic hybrid all-solid-state cells.

  18. Hybrid systems of AlInP microdisks and colloidal CdSe nanocrystals showing whispering-gallery modes at room temperature

    SciTech Connect

    Strelow, Christian; Weising, Simon; Bonatz, Dennis; Mews, Alf; Kipp, Tobias; Penttinen, Jussi-Pekka; Hakkarainen, Teemu V.; Schramm, Andreas

    2014-09-01

    We report on the realization of hybrid systems composed of passive optical microdisk resonators prepared from epitaxial layer systems and nanocrystal quantum emitters synthesized by colloidal chemistry. The AlInP disk material allows for the operation in the visible range, as probed by CdSe-based nanocrystals. Photoluminescence spectra at room temperature reveal sets of whispering-gallery modes consistent with finite-difference time-domain simulations. In the experiments, a special sample geometry renders it possible to detect resonant optical modes perpendicular to the disk plane.

  19. Chirality Inversion of CdSe and CdS Quantum Dots without Changing the Stereochemistry of the Capping Ligand.

    PubMed

    Choi, Jung Kyu; Haynie, Benjamin E; Tohgha, Urice; Pap, Levente; Elliott, K Wade; Leonard, Brian M; Dzyuba, Sergei V; Varga, Krisztina; Kubelka, Jan; Balaz, Milan

    2016-03-22

    L-cysteine derivatives induce and modulate the optical activity of achiral cadmium selenide (CdSe) and cadmium sulfide (CdS) quantum dots (QDs). Remarkably, N-acetyl-L-cysteine-CdSe and L-homocysteine-CdSe as well as N-acetyl-L-cysteine-CdS and L-cysteine-CdS showed "mirror-image" circular dichroism (CD) spectra regardless of the diameter of the QDs. This is an example of the inversion of the CD signal of QDs by alteration of the ligand's structure, rather than inversion of the ligand's absolute configuration. Non-empirical quantum chemical simulations of the CD spectra were able to reproduce the experimentally observed sign patterns and demonstrate that the inversion of chirality originated from different binding arrangements of N-acetyl-L-cysteine and L-homocysteine-CdSe to the QD surface. These efforts may allow the prediction of the ligand-induced chiroptical activity of QDs by calculating the specific binding modes of the chiral capping ligands. Combined with the large pool of available chiral ligands, our work opens a robust approach to the rational design of chiral semiconducting nanomaterials.

  20. Colloidal quantum dot solar cells on curved and flexible substrates

    SciTech Connect

    Kramer, Illan J.; Moreno-Bautista, Gabriel; Minor, James C.; Kopilovic, Damir; Sargent, Edward H.

    2014-10-20

    Colloidal quantum dots (CQDs) are semiconductor nanocrystals synthesized with, processed in, and deposited from the solution phase, potentially enabling low-cost, facile manufacture of solar cells. Unfortunately, CQD solar cell reports, until now, have only explored batch-processing methods—such as spin-coating—that offer limited capacity for scaling. Spray-coating could offer a means of producing uniform colloidal quantum dot films that yield high-quality devices. Here, we explore the versatility of the spray-coating method by producing CQD solar cells in a variety of previously unexplored substrate arrangements. The potential transferability of the spray-coating method to a roll-to-roll manufacturing process was tested by spray-coating the CQD active layer onto six substrates mounted on a rapidly rotating drum, yielding devices with an average power conversion efficiency of 6.7%. We further tested the manufacturability of the process by endeavoring to spray onto flexible substrates, only to find that spraying while the substrate was flexed was crucial to achieving champion performance of 7.2% without compromise to open-circuit voltage. Having deposited onto a substrate with one axis of curvature, we then built our CQD solar cells onto a spherical lens substrate having two axes of curvature resulting in a 5% efficient device. These results show that CQDs deposited using our spraying method can be integrated to large-area manufacturing processes and can be used to make solar cells on unconventional shapes.

  1. Red shift in the photoluminescence of colloidal carbon quantum dots induced by photon reabsorption

    SciTech Connect

    Zhang, Wenxia; Dai, Dejian; Chen, Xifang; Guo, Xiaoxiao; Fan, Jiyang

    2014-03-03

    We synthesize the colloidal carbon/graphene quantum dots 1–9 nm in diameter and study their photoluminescence properties. Surprisingly, the luminescence properties of a fixed collection of colloidal carbon quantum dots can be systematically changed as the concentration varies. A model based on photon reabsorption is proposed which explains well the experiment. Infrared spectral study indicates that the surfaces of the carbon quantum dots are substantially terminated by oxygen atoms, which causes their ultra-high hydrophilicity. Our result clarifies the mystery of distinct emission colors in carbon quantum dots and indicates that photon reabsorption can strongly affect the luminescence properties of colloidal nanocrystals.

  2. Vectorial electron transfer for improved hydrogen evolution by mercaptopropionic-acid-regulated CdSe quantum-dots-TiO2 -Ni(OH)2 assembly.

    PubMed

    Yu, Shan; Li, Zhi-Jun; Fan, Xiang-Bing; Li, Jia-Xin; Zhan, Fei; Li, Xu-Bing; Tao, Ye; Tung, Chen-Ho; Wu, Li-Zhu

    2015-02-01

    A visible-light-induced hydrogen evolution system based on a CdSe quantum dots (QDs)-TiO2 -Ni(OH)2 ternary assembly has been constructed under an ambient environment, and a bifunctional molecular linker, mercaptopropionic acid, is used to facilitate the interaction between CdSe QDs and TiO2 . This hydrogen evolution system works effectively in a basic aqueous solution (pH 11.0) to achieve a hydrogen evolution rate of 10.1 mmol g(-1)  h(-1) for the assembly and a turnover frequency of 5140 h(-1) with respect to CdSe QDs (10 h); the latter is comparable with the highest value reported for QD systems in an acidic environment. X-ray photoelectron spectroscopy, X-ray absorption spectroscopy, and control experiments demonstrate that Ni(OH)2 is an efficient hydrogen evolution catalyst. In addition, inductively coupled plasma optical emission spectroscopy and the emission decay of the assembly combined with the hydrogen evolution experiments show that TiO2 functions mainly as the electron mediator; the vectorial electron transfer from CdSe QDs to TiO2 and then from TiO2 to Ni(OH)2 enhances the efficiency for hydrogen evolution. The assembly comprises light antenna CdSe QDs, electron mediator TiO2 , and catalytic Ni(OH)2 , which mimics the strategy of photosynthesis exploited in nature and takes us a step further towards artificial photosynthesis.

  3. Coexpression of CdSe and CdSe/CdS quantum dots in live cells using molecular hyperspectral imaging technology.

    PubMed

    Li, Qingli; Peng, Hui; Wang, Jing; Wang, Yiting; Guo, Fangmin

    2015-11-01

    A direct spatial and spectral observation of CdSe and CdSe/CdS quantum dots (QDs) as probes in live cells is performed by using a custom molecular hyperspectral imaging (MHI) system. Water-soluble CdSe and CdSe/CdS QDs are synthesized in aqueous solution under the assistance of high-intensity ultrasonic irradiation and incubated with colon cancer cells for bioimaging. Unlike the traditional fluorescence microscopy methods, MHI technology can identify QD probes according to their spectral signatures and generate coexpression and stain titer maps by a clustering method. The experimental results show that the MHI method has potential to unmix biomarkers by their spectral information, which opens up a pathway of optical multiplexing with many different QD probes. PMID:26588112

  4. Coexpression of CdSe and CdSe/CdS quantum dots in live cells using molecular hyperspectral imaging technology

    NASA Astrophysics Data System (ADS)

    Li, Qingli; Peng, Hui; Wang, Jing; Wang, Yiting; Guo, Fangmin

    2015-11-01

    A direct spatial and spectral observation of CdSe and CdSe/CdS quantum dots (QDs) as probes in live cells is performed by using a custom molecular hyperspectral imaging (MHI) system. Water-soluble CdSe and CdSe/CdS QDs are synthesized in aqueous solution under the assistance of high-intensity ultrasonic irradiation and incubated with colon cancer cells for bioimaging. Unlike the traditional fluorescence microscopy methods, MHI technology can identify QD probes according to their spectral signatures and generate coexpression and stain titer maps by a clustering method. The experimental results show that the MHI method has potential to unmix biomarkers by their spectral information, which opens up a pathway of optical multiplexing with many different QD probes.

  5. Size and Temperature Dependence of Electron Transfer between CdSe Quantum Dots and a TiO 2 Nanobelt

    DOE PAGES

    Tafen, De Nyago; Prezhdo, Oleg V.

    2015-02-24

    Understanding charge transfer reactions between quantum dots (QD) and metal oxides is fundamental for improving photocatalytic, photovoltaic and electronic devices. The complexity of these processes makes it difficult to find an optimum QD size with rapid charge injection and low recombination. We combine time-domain density functional theory with nonadiabatic molecular dynamics to investigate the size and temperature dependence of the experimentally studied electron transfer and charge recombination at CdSe QD-TiO2 nanobelt (NB) interfaces. The electron injection rate shows strong dependence on the QD size, increasing for small QDs. The rate exhibits Arrhenius temperature dependence, with the activation energy of themore » order of millielectronvolts. The charge recombination process occurs due to coupling of the electronic subsystem to vibrational modes of the TiO2 NB. Inelastic electron-phonon scattering happens on a picosecond time scale, with strong dependence on the QD size. Our simulations demonstrate that the electron-hole recombination rate decreases significantly as the QD size increases, in excellent agreement with experiments. The temperature dependence of the charge recombination rates can be successfully modeled within the framework of the Marcus theory through optimization of the electronic coupling and the reorganization energy. Our simulations indicate that by varying the QD size, one can modulate the photoinduced charge separation and charge recombination, fundamental aspects of the design principles for high efficiency devices.« less

  6. Lifetime and Polarization of the Radiative Decay of Excitons, Biexcitons, and Trions in CdSe Nanocrystal Quantum Dots

    SciTech Connect

    Califano, M.; Franceschetti, A.; Zunger, A.

    2007-01-01

    Using the pseudopotential configuration-interaction method, we calculate the intrinsic lifetime and polarization of the radiative decay of single excitons (X), positive and negative trions (X{sup +} and X{sup -}), and biexcitons (XX) in CdSe nanocrystal quantum dots. We investigate the effects of the inclusion of increasingly more complex many-body treatments, starting from the single-particle approach and culminating with the configuration-interaction scheme. Our configuration-interaction results for the size dependence of the single-exciton radiative lifetime at room temperature are in excellent agreement with recent experimental data. We also find the following. (i) Whereas the polarization of the bright exciton emission is always perpendicular to the hexagonal c axis, the polarization of the dark exciton switches from perpendicular to parallel to the hexagonal c axis in large dots, in agreement with experiment. (ii) The ratio of the radiative lifetimes of mono- and biexcitons (X):(XX) is {approx}1:1 in large dots (R=19.2 {angstrom}). This ratio increases with decreasing nanocrystal size, approaching 2 in small dots (R=10.3 {angstrom}). (iii) The calculated ratio (X{sup +}):(X{sup -}) between positive and negative trion lifetimes is close to 2 for all dot sizes considered.

  7. Electron relaxation in the CdSe quantum dot--ZnO composite: prospects for photovoltaic applications.

    PubMed

    Zídek, Karel; Abdellah, Mohamed; Zheng, Kaibo; Pullerits, Tõnu

    2014-11-28

    Quantum dot (QD)-metal oxide composite forms a "heart" of the QD-sensitized solar cells. It maintains light absorption and electron-hole separation in the system and has been therefore extensively studied. The interest is largely driven by a vision of harvesting the hot carrier energy before it is lost via relaxation. Despite of importance of the process, very little is known about the carrier relaxation in the QD-metal oxide composites. In order to fill this gap of knowledge we carry out a systematic study of initial electron dynamics in different CdSe QD systems. Our data reveal that QD attachment to ZnO induces a speeding-up of transient absorption onset. Detailed analysis of the onset proves that the changes are caused by an additional relaxation channel dependent on the identity of the QD-ZnO linker molecule. The faster relaxation represents an important factor for hot carrier energy harvesting, whose efficiency can be influenced by almost 50%.

  8. Quantitative assessment of Tn antigen in breast tissue micro-arrays using CdSe aqueous quantum dots.

    PubMed

    Au, Giang H T; Mejias, Linette; Swami, Vanlila K; Brooks, Ari D; Shih, Wan Y; Shih, Wei-Heng

    2014-03-01

    In this study, we examined the use of CdSe aqueous quantum dots (AQDs) each conjugated to three streptavidin as a fluorescent label to image Tn antigen expression in various breast tissues via a sandwich staining procedure where the primary monoclonal anti-Tn antibody was bound to the Tn antigen on the tissue, a biotin-labeled secondary antibody was bound to the primary anti-Tn antibody, and finally the streptavidin-conjugated AQDs were bound to the biotin on the secondary antibody. We evaluated the AQD staining of Tn antigen on tissue microarrays consisting of 395 cores from 115 cases including three tumor cores and one normal-tissue core from each breast cancer case and three tumor cores from each benign case. The results indicated AQD-Tn staining was positive in more than 90% of the cells in the cancer cores but not the cells in the normal-tissue cores and the benign tumor cores. As a result, AQD-Tn staining exhibited 95% sensitivity and 90% specificity in differentiating breast cancer against normal breast tissues and benign breast conditions. These results were better than the 90% sensitivity and 80% specificity exhibited by the corresponding horse radish peroxidase (HRP) staining using the same antibodies on the same tissues and those of previous studies that used different fluorescent labels to image Tn antigen. In addition to sensitivity and specificity, the current AQD-Tn staining with a definitive threshold was quantitative. PMID:24411673

  9. Conditions for Directional Charge Transfer in CdSe Quantum Dots Functionalized by Ru(II) Polypyridine Complexes.

    PubMed

    Kilina, Svetlana; Cui, Peng; Fischer, Sean A; Tretiak, Sergei

    2014-10-16

    Thermodynamic conditions governing the charge transfer direction in CdSe quantum dots (QD) functionalized by either Ru(II)-trisbipyridine or black dye are studied using density functional theory (DFT) and time-dependent DFT (TDDFT). Compared to the energy offsets of the isolated QD and the dye, QD-dye interactions strongly stabilize dye orbitals with respect to the QD states, while the surface chemistry of the QD has a minor effect on the energy offsets. In all considered QD/dye composites, the dyes always introduce unoccupied states close to the edge of the conduction band and control the electron transfer. Negatively charged ligands and less polar solvents significantly destabilize the dye's occupied orbitals shifting them toward the very edge of the valence band, thus, providing favorite conditions for the hole transfer. Overall, variations in the dye's ligands and solvent polarity can progressively adjust the electronic structure of QD/dye composites to modify conditions for the directed charge transfer. PMID:26278611

  10. Dead zones in colloidal quantum dot photovoltaics: evidence and implications.

    PubMed

    Barkhouse, D Aaron R; Kramer, Illan J; Wang, Xihua; Sargent, Edward H

    2010-09-13

    In order to fabricate photovoltaic (PV) cells incorporating light-trapping electrodes, flexible foil substrates, or more than one junction, illumination through the top-contact (i.e.: non-substrate) side of a photovoltaic device is desirable. We investigate the relative collection efficiency for illumination through the top vs. bottom of PbS colloidal quantum dot (CQD) PV devices. The external quantum efficiency spectra of FTO/TiO₂/PbS CQD/ITO PV devices with various PbS layer thicknesses were measured for illumination through either the top (ITO) or bottom (FTO) contacts. By comparing the relative shapes and intensities of these spectra with those calculated from an estimation of the carrier generation profile and the internal quantum efficiency as a function of distance from the TiO₂ interface in the devices, a substantial dead zone, where carrier extraction is dramatically reduced, is identified near the ITO top contact. The implications for device design, and possible means of avoiding the formation of such a dead zone, are discussed.

  11. Colloidal quantum dots for low-cost MWIR imaging

    NASA Astrophysics Data System (ADS)

    Ciani, Anthony J.; Pimpinella, Richard E.; Grein, Christoph H.; Guyot-Sionnest, Philippe

    2016-05-01

    Monodisperse suspensions of HgTe colloidal quantum dots (CQD) are readily synthesized with infrared energy gaps between 3 and 12 microns. Infrared photodetection using dried films of these CQDs has been demonstrated up to a wavelength of 12 microns, and HgTe CQD single-elemnet devices with 3.6 micron cutoff have bee nreported nad show ogod absorption <(10^4 cm^-1), response time and detectivity (2*10^10 Jones) at at emperature of 175 K; with the potential fo uncooled imaging. The synthesis of CQDs and fabrication of detector devices employ bench-top chemistry techniques, leading to the potential for rapid, wafer-scale manufacture of MWIR imaging devices with low production costs and overhead. The photoconductive, photovoltaic and optical properties of HgTe CQD films will be discussed relative to infrared imaging, along with recent achievements in integrating CQD films with readout integrated circuits to produce CQD-based MWIR focal plane arrays.

  12. Exciton Dynamics in InSb Colloidal Quantum Dots.

    PubMed

    Sills, Andrew; Harrison, Paul; Califano, Marco

    2016-01-01

    Extraordinarily fast biexciton decay times and unexpectedly large optical gaps are two striking features observed in InSb colloidal quantum dots that have remained so far unexplained. The former, should its origin be identified as an Auger recombination process, would have important implications regarding carrier multiplication efficiency, suggesting these nanostructures as potentially ideal active materials in photovoltaic devices. The latter could offer new insights into the factors that influence the electronic structure and consequently the optical properties of systems with reduced dimensionality and provide additional means to fine-tune them. Using the state-of-the-art atomistic semiempirical pseudopotential method we unveil the surprising origins of these features and show that a comprehensive explanation for these properties requires delving deep into the atomistic detail of these nanostructures and is, therefore, outside the reach of less sophisticated, albeit more popular, theoretical approaches. PMID:26650516

  13. Colloidal graphene quantum dots with well-defined structures.

    PubMed

    Yan, Xin; Li, Binsong; Li, Liang-shi

    2013-10-15

    When the size of a semiconductor crystal is reduced to the nanometer scale, the crystal boundary significantly modifies electron distribution, making properties such as bandgap and energy relaxation dynamics size dependent. This phenomenon, known as quantum confinement, has been demonstrated in many semiconductor materials, leading to practical applications in areas such as bioimaging, photovoltaics, and light-emitting diodes. Graphene, a unique type of semiconductor, is a two-dimensional crystal with a zero bandgap and a zero effective mass of charge carriers. Consequently, we expect new phenomena from nanometer-sized graphene, or graphene quantum dots (QDs), because the energy of charge carriers in graphene follows size-scaling laws that differ from those in other semiconductors. From a chemistry point of view, graphene is made of carbon, an element for which researchers have developed a whole branch of chemistry. Thus, it is possible to synthesize graphene QDs through stepwise, well-controlled organic chemistry, achieving structures with an atomic precision that has not been possible for any other semiconductor materials. Recently, we developed a new solubilizing strategy that led to synthesis of stable colloidal graphene QDs with more than 100 conjugated carbon atoms, allowing us to study their properties in a new size regime. In this Account, we review our recent progress working with the colloidal graphene QDs, including their synthesis and stabilization, tuning of their properties, and new phenomena in energy relaxation dynamics. In particular, we have observed extraordinarily slow "electron cooling"--the relaxation of electrons from high excited states to lower ones. With further investigation, these high-energy electrons could potentially be harvested in solar energy applications, for example, creating more efficient photovoltaic cells. We discuss additional emerging opportunities with these new materials and current challenges, hoping to draw the interest

  14. Study of optical and structural properties of CdSe quantum dot embedded in PVA polymer matrix

    NASA Astrophysics Data System (ADS)

    Tyagi, Chetna; Sharma, Ambika

    2015-08-01

    To enhance the properties and applicability of devices it is essential to incorporate semiconductor nanoparticles into polymer matrix. This introduces a new branch of science which includes device fabrications such as gas sensors, nonlinear optics, catalysis etc. Herein, we have synthesized CdSe/PVA nanocomposite (NC) material using wet chemical synthesis technique. The XRD studies revealed the formation of crystalline structure of CdSe nanoparticles (NP's) and PVA NC's with an average size of 100 nm and 5 nm respectively. Energy band gap is determined using UV-VIS Spectroscopy. A red shift in the absorption edge of CdSe/PVA NC is observed with respect to CdSe Np's, The photoluminescence spectra also show red shift for CdSe/PVA NC as compared to CdSe NP's Thus the use of CdSe/PVA for solar cell application would be more preferable than CdSe NP's.

  15. A CdSe thin film: a versatile buffer layer for improving the performance of TiO2 nanorod array:PbS quantum dot solar cells

    NASA Astrophysics Data System (ADS)

    Tan, Furui; Wang, Zhijie; Qu, Shengchun; Cao, Dawei; Liu, Kong; Jiang, Qiwei; Yang, Ying; Pang, Shan; Zhang, Weifeng; Lei, Yong; Wang, Zhanguo

    2016-05-01

    To fully utilize the multiple exciton generation effects in quantum dots and improve the overall efficiency of the corresponding photovoltaic devices, nanostructuralizing the electron conducting layer turns out to be a feasible strategy. Herein, PbS quantum dot solar cells were fabricated on the basis of morphologically optimized TiO2 nanorod arrays. By inserting a thin layer of CdSe quantum dots into the interface of TiO2 and PbS, a dramatic enhancement in the power conversion efficiency from 4.2% to 5.2% was realized and the resulting efficiency is one of the highest values for quantum dot solar cells based on nanostructuralized buffer layers. The constructed double heterojunction with a cascade type-II energy level alignment is beneficial for promoting photogenerated charge separation and reducing charge recombination, thereby responsible for the performance improvement, as revealed by steady-state analyses as well as ultra-fast photoluminescence and photovoltage decays. Thus this paper provides a good buffer layer to the community of quantum dot solar cells.To fully utilize the multiple exciton generation effects in quantum dots and improve the overall efficiency of the corresponding photovoltaic devices, nanostructuralizing the electron conducting layer turns out to be a feasible strategy. Herein, PbS quantum dot solar cells were fabricated on the basis of morphologically optimized TiO2 nanorod arrays. By inserting a thin layer of CdSe quantum dots into the interface of TiO2 and PbS, a dramatic enhancement in the power conversion efficiency from 4.2% to 5.2% was realized and the resulting efficiency is one of the highest values for quantum dot solar cells based on nanostructuralized buffer layers. The constructed double heterojunction with a cascade type-II energy level alignment is beneficial for promoting photogenerated charge separation and reducing charge recombination, thereby responsible for the performance improvement, as revealed by steady

  16. Anodic Electrogenerated Chemiluminescence of Ru(bpy)3(2+) with CdSe Quantum Dots as Coreactant and Its Application in Quantitative Detection of DNA.

    PubMed

    Dong, Yong-Ping; Gao, Ting-Ting; Zhou, Ying; Jiang, Li-Ping; Zhu, Jun-Jie

    2015-01-01

    In the present paper, we report that CdSe quantum dots (QDs) can act as the coreactant of Ru(bpy)3(2+) electrogenerated chemiluminescence (ECL) in neutral condition. Strong anodic ECL signal was observed at ~1.10 V at CdSe QDs modified glassy carbon electrode (CdSe/GCE), which might be mainly attributed to the apparent electrocatalytic effect of QDs on the oxidation of Ru(bpy)3(2+). Ru(bpy)3(2+) can be intercalated into the loop of hairpin DNA through the electrostatic interaction to fabricate a probe. When the probe was bound to the CdSe QDs modified on the GCE, the intense ECL signal was obtained. The more Ru(bpy)3(2+) can be intercalated when DNA loop has larger diameter and the stronger ECL signal can be observed. The loop of hairpin DNA can be opened in the presence of target DNA to release the immobilized Ru(bpy)3(2+), which can result in the decrease of ECL signal. The decreased ECL signal varied linearly with the concentration of target DNA, which showed the ECL biosensor can be used in the sensitive detection of DNA. The proposed ECL biosensor showed an excellent performance with high specificity, wide linear range and low detection limit. PMID:26472243

  17. Current matching using CdSe quantum dots to enhance the power conversion efficiency of InGaP/GaAs/Ge tandem solar cells.

    PubMed

    Lee, Ya-Ju; Yao, Yung-Chi; Tsai, Meng-Tsan; Liu, An-Fan; Yang, Min-De; Lai, Jiun-Tsuen

    2013-11-01

    A III-V multi-junction tandem solar cell is the most efficient photovoltaic structure that offers an extremely high power conversion efficiency. Current mismatching between each subcell of the device, however, is a significant challenge that causes the experimental value of the power conversion efficiency to deviate from the theoretical value. In this work, we explore a promising strategy using CdSe quantum dots (QDs) to enhance the photocurrent of the limited subcell to match with those of the other subcells and to enhance the power conversion efficiency of InGaP/GaAs/Ge tandem solar cells. The underlying mechanism of the enhancement can be attributed to the QD's unique capacity for photon conversion that tailors the incident spectrum of solar light; the enhanced efficiency of the device is therefore strongly dependent on the QD's dimensions. As a result, by appropriately selecting and spreading 7 mg/mL of CdSe QDs with diameters of 4.2 nm upon the InGaP/GaAs/Ge solar cell, the power conversion efficiency shows an enhancement of 10.39% compared to the cell's counterpart without integrating CdSe QDs.

  18. Current matching using CdSe quantum dots to enhance the power conversion efficiency of InGaP/GaAs/Ge tandem solar cells.

    PubMed

    Lee, Ya-Ju; Yao, Yung-Chi; Tsai, Meng-Tsan; Liu, An-Fan; Yang, Min-De; Lai, Jiun-Tsuen

    2013-11-01

    A III-V multi-junction tandem solar cell is the most efficient photovoltaic structure that offers an extremely high power conversion efficiency. Current mismatching between each subcell of the device, however, is a significant challenge that causes the experimental value of the power conversion efficiency to deviate from the theoretical value. In this work, we explore a promising strategy using CdSe quantum dots (QDs) to enhance the photocurrent of the limited subcell to match with those of the other subcells and to enhance the power conversion efficiency of InGaP/GaAs/Ge tandem solar cells. The underlying mechanism of the enhancement can be attributed to the QD's unique capacity for photon conversion that tailors the incident spectrum of solar light; the enhanced efficiency of the device is therefore strongly dependent on the QD's dimensions. As a result, by appropriately selecting and spreading 7 mg/mL of CdSe QDs with diameters of 4.2 nm upon the InGaP/GaAs/Ge solar cell, the power conversion efficiency shows an enhancement of 10.39% compared to the cell's counterpart without integrating CdSe QDs. PMID:24514936

  19. Anodic Electrogenerated Chemiluminescence of Ru(bpy)32+ with CdSe Quantum Dots as Coreactant and Its Application in Quantitative Detection of DNA

    PubMed Central

    Dong, Yong-Ping; Gao, Ting-Ting; Zhou, Ying; Jiang, Li-Ping; Zhu, Jun-Jie

    2015-01-01

    In the present paper, we report that CdSe quantum dots (QDs) can act as the coreactant of Ru(bpy)32+ electrogenerated chemiluminescence (ECL) in neutral condition. Strong anodic ECL signal was observed at ~1.10 V at CdSe QDs modified glassy carbon electrode (CdSe/GCE), which might be mainly attributed to the apparent electrocatalytic effect of QDs on the oxidation of Ru(bpy)32+. Ru(bpy)32+ can be intercalated into the loop of hairpin DNA through the electrostatic interaction to fabricate a probe. When the probe was bound to the CdSe QDs modified on the GCE, the intense ECL signal was obtained. The more Ru(bpy)32+ can be intercalated when DNA loop has larger diameter and the stronger ECL signal can be observed. The loop of hairpin DNA can be opened in the presence of target DNA to release the immobilized Ru(bpy)32+, which can result in the decrease of ECL signal. The decreased ECL signal varied linearly with the concentration of target DNA, which showed the ECL biosensor can be used in the sensitive detection of DNA. The proposed ECL biosensor showed an excellent performance with high specificity, wide linear range and low detection limit. PMID:26472243

  20. Understanding the electronic structure of CdSe quantum dot-fullerene (C{sub 60}) hybrid nanostructure for photovoltaic applications

    SciTech Connect

    Sarkar, Sunandan; Rajbanshi, Biplab; Sarkar, Pranab

    2014-09-21

    By using the density-functional tight binding method, we studied the electronic structure of CdSe quantum dot(QD)-buckminsterfullerene (C{sub 60}) hybrid systems as a function of both the size of the QD and concentration of the fullerene molecule. Our calculation reveals that the lowest unoccupied molecular orbital energy level of the hybrid CdSeQD-C{sub 60} systems lies on the fullerene moiety, whereas the highest occupied molecular orbital (HOMO) energy level lies either on the QD or the fullerene depending on size of the CdSe QD. We explored the possibility of engineering the energy level alignment by varying the size of the CdSe QD. With increase in size of the QD, the HOMO level is shifted upward and crosses the HOMO level of the C{sub 60}-thiol molecule resulting transition from the type-I to type-II band energy alignment. The density of states and charge density plot support these types of band gap engineering of the CdSe-C{sub 60} hybrid systems. This type II band alignment indicates the possibility of application of this nanohybrid for photovoltaic purpose.

  1. Nondestructive chemical functionalization of MWNTs by poly(2-dimethylaminoethyl methacrylate) and their conjugation with CdSe quantum dots: Synthesis, properties, and cytotoxicity studies

    NASA Astrophysics Data System (ADS)

    Islam, Md. Rafiqul; Bach, Long Giang; Vo, Thanh-Sang; Tran, Thi-Nga; Lim, Kwon Taek

    2013-12-01

    Multi-walled carbon nanotubes (MWNTs) were functionalized with poly(2-dimethylaminoethyl methacrylate) (PDMAEMA) in a nondestructive manner by UV-driven surface-initiated reversible addition fragmentation chain transfer (RAFT) polymerization. The RAFT agent having benzophenone groups was initially synthesized, and anchored to MWNTs through UV-triggered photoreaction. The subsequent RAFT polymerization of DMAEMA from the surface of MWNTs afforded PDMAEMA grafted MWNTs (MWNTs-g-PDMAEMA). The successful grafting of PDMAEMA on MWNTs via chemical linkage was confirmed by FT-IR, 1H NMR, XPS, EDX, TGA, TEM, and SEM analyses. A reversible dispersion phenomenon was observed in an aqueous solution of MWNTs-g-PDMAEMA as induced either by temperature or pH. The CdSe quantum dots (CdSe QDs) were attached to quaternized MWNTs-g-PDMAEMA to produce MWNTs-g-PDMAEMA-MeI/CdSe nanohybrids via electrostatic self-assembly. The formation of the nanohybrids was elucidated by EDS, TEM, and XRD. The cell viability assessment of the nanohybrids suggested their biocompatible character. The photoluminescence spectra of the nanohybrids indicated that the CdSe QDs significantly preserved its optical property after conjugation with MWNTs-g-PDMAEMA.

  2. CdSe magic-sized quantum dots incorporated in biomembrane models at the air-water interface composed of components of tumorigenic and non-tumorigenic cells.

    PubMed

    Goto, Thiago E; Lopes, Carla C; Nader, Helena B; Silva, Anielle C A; Dantas, Noelio O; Siqueira, José R; Caseli, Luciano

    2016-07-01

    Cadmium selenide (CdSe) magic-sized quantum dots (MSQDs) are semiconductor nanocrystals with stable luminescence that are feasible for biomedical applications, especially for in vivo and in vitro imaging of tumor cells. In this work, we investigated the specific interaction of CdSe MSQDs with tumorigenic and non-tumorigenic cells using Langmuir monolayers and Langmuir-Blodgett (LB) films of lipids as membrane models for diagnosis of cancerous cells. Surface pressure-area isotherms and polarization modulation reflection-absorption spectroscopy (PM-IRRAS) showed an intrinsic interaction between the quantum dots, inserted in the aqueous subphase, and Langmuir monolayers constituted either of selected lipids or of tumorigenic and non-tumorigenic cell extracts. The films were transferred to solid supports to obtain microscopic images, providing information on their morphology. Similarity between films with different compositions representing cell membranes, with or without the quantum dots, was evaluated by atomic force microscopy (AFM) and confocal microscopy. This study demonstrates that the affinity of quantum dots for models representing cancer cells permits the use of these systems as devices for cancer diagnosis. PMID:27107554

  3. CdSe magic-sized quantum dots incorporated in biomembrane models at the air-water interface composed of components of tumorigenic and non-tumorigenic cells.

    PubMed

    Goto, Thiago E; Lopes, Carla C; Nader, Helena B; Silva, Anielle C A; Dantas, Noelio O; Siqueira, José R; Caseli, Luciano

    2016-07-01

    Cadmium selenide (CdSe) magic-sized quantum dots (MSQDs) are semiconductor nanocrystals with stable luminescence that are feasible for biomedical applications, especially for in vivo and in vitro imaging of tumor cells. In this work, we investigated the specific interaction of CdSe MSQDs with tumorigenic and non-tumorigenic cells using Langmuir monolayers and Langmuir-Blodgett (LB) films of lipids as membrane models for diagnosis of cancerous cells. Surface pressure-area isotherms and polarization modulation reflection-absorption spectroscopy (PM-IRRAS) showed an intrinsic interaction between the quantum dots, inserted in the aqueous subphase, and Langmuir monolayers constituted either of selected lipids or of tumorigenic and non-tumorigenic cell extracts. The films were transferred to solid supports to obtain microscopic images, providing information on their morphology. Similarity between films with different compositions representing cell membranes, with or without the quantum dots, was evaluated by atomic force microscopy (AFM) and confocal microscopy. This study demonstrates that the affinity of quantum dots for models representing cancer cells permits the use of these systems as devices for cancer diagnosis.

  4. Hybrid passivated colloidal quantum dot solids for photovoltaics

    NASA Astrophysics Data System (ADS)

    Thon, Susanna M.; Ip, Alexander H.; Hoogland, Sjoerd; Voznyy, Oleksandr; Zhitomirsky, David; Debnath, Ratan; Levina, Larissa; Rollny, Lisa R.; Carey, Graham H.; Fischer, Armin; Kemp, Kyle W.; Kramer, Illan J.; Ning, Zhijun; Labelle, André J.; Chou, Kang Wei; Amassian, Aram; Sargent, Edward H.

    2013-03-01

    Colloidal quantum dot (CQD) films are an attractive photovoltaic material due to their large-area-compatible solution processing and bandgap tuning through the quantum size effect. However, the large internal surface areas make CQD films prone to high trap state densities, leading to recombination of charge carriers. We quantify the density of midgap trap states in PbS CQD solids and show that the current photovoltaic performance is limited by these states. We develop a robust hybrid passivation scheme that involves introducing halide anions during the end stages of the synthesis process, which can passivate trap sites that are inaccessible to much larger standard organic ligands, and combine this with an organic crosslinking strategy to form the film. We use our hybrid passivated CQD solid to fabricate a solar cell with a certified efficiency of 7.0%, which is a record for a CQD photovoltaic device. This work is supported by an award (KUS-11-009-21) from KAUST, by the Ontario Research Fund Research Excellence Program and by the Natural Sciences and Engineering Research Council of Canada.

  5. Surface ligands increase photoexcitation relaxation rates in CdSe quantum dots.

    PubMed

    Kilina, Svetlana; Velizhanin, Kirill A; Ivanov, Sergei; Prezhdo, Oleg V; Tretiak, Sergei

    2012-07-24

    Understanding the pathways of hot exciton relaxation in photoexcited semiconductor nanocrystals, also called quantum dots (QDs), is of paramount importance in multiple energy, electronics and biological applications. An important nonradiative relaxation channel originates from the nonadiabatic (NA) coupling of electronic degrees of freedom to nuclear vibrations, which in QDs depend on the confinement effects and complicated surface chemistry. To elucidate the role of surface ligands in relaxation processes of nanocrystals, we study the dynamics of the NA exciton relaxation in Cd(33)Se(33) semiconductor quantum dots passivated by either trimethylphosphine oxide or methylamine ligands using explicit time-dependent modeling. The large extent of hybridization between electronic states of quantum dot and ligand molecules is found to strongly facilitate exciton relaxation. Our computational results for the ligand contributions to the exciton relaxation and electronic energy-loss in small clusters are further extrapolated to larger quantum dots. PMID:22742432

  6. Fast current blinking in individual PbS and CdSe quantum dots.

    PubMed

    Maturova, Klara; Nanayakkara, Sanjini U; Luther, Joseph M; van de Lagemaat, Jao

    2013-06-12

    Fast current intermittency of the tunneling current through single semiconductor quantum dots was observed through time-resolved intermittent contact conductive atomic force microscopy in the dark and under illumination at room temperature. The current through a single dot switches on and off at time scales ranging from microseconds to seconds with power-law distributions for both the on and off times. On states are attributed to the resonant tunneling of charges from the electrically conductive AFM tip to the quantum dot, followed by transfer to the substrate, whereas off states are attributed to a Coulomb blockade effect in the quantum dots that shifts the energy levels out of resonance conditions due to the presence of the trapped charge, while at the same bias. The observation of current intermittency due to Coulomb blockade effects has important implications for the understanding of carrier transport through arrays of quantum dots.

  7. Green biosynthesis of biocompatible CdSe quantum dots in living Escherichia coli cells

    NASA Astrophysics Data System (ADS)

    Yan, Zhengyu; Qian, Jing; Gu, Yueqing; Su, Yilong; Ai, Xiaoxia; Wu, Shengmei

    2014-03-01

    A green and efficient biosynthesis method to prepare fluorescence-tunable biocompatible cadmium selenide quantum dots using Escherichia coli cells as biological matrix was proposed. Decisive factors in biosynthesis of cadmium selenide quantum dots in a designed route in Escherichia coli cells were elaborately investigated, including the influence of the biological matrix growth stage, the working concentration of inorganic reactants, and the co-incubation duration of inorganic metals to biomatrix. Ultraviolet-visible, photoluminescence, and inverted fluorescence microscope analysis confirmed the unique optical properties of the biosynthesized cadmium selenide quantum dots. The size distribution of the nanocrystals extracted from cells and the location of nanocrystals foci in vivo were also detected seriously by transmission electron microscopy. A surface protein capping layer outside the nanocrystals was confirmed by Fourier transform infrared spectroscopy measurements, which were supposed to contribute to reducing cytotoxicity and maintain a high viability of cells when incubating with quantum dots at concentrations as high as 2 μM. Cell morphology observation indicated an effective labeling of living cells by the biosynthesized quantum dots after a 48 h co-incubation. The present work demonstrated an economical and environmentally friendly approach to fabricating highly fluorescent quantum dots which were expected to be an excellent fluorescent dye for broad bio-imaging and labeling.

  8. Enhanced performance of branched TiO{sub 2} nanorod based Mn-doped CdS and Mn-doped CdSe quantum dot-sensitized solar cell

    SciTech Connect

    Kim, Soo-Kyoung; Gopi, Chandu V. V. M.; Lee, Jae-Cheol; Kim, Hee-Je

    2015-04-28

    TiO{sub 2} branched nanostructures could be efficient as photoanodes for quantum dot-sensitized solar cells (QDSCs) due to their large surface area for QD deposition. In this study, Mn-doped CdS/Mn-doped CdSe deposited branched TiO{sub 2} nanorods were fabricated to enhance the photovoltaic performance of QDSCs. Mn doping in CdS and CdSe retards the recombination losses of electrons, while branched TiO{sub 2} nanorods facilitate effective electron transport and compensate for the low surface area of the nanorod structure. As a result, the charge-transfer resistance (R{sub CT}), electron lifetime (τ{sub e}), and the amount of QD deposition were significantly improved with branched TiO{sub 2} nanorod based Mn-doped CdS/Mn-doped CdSe quantum dot-sensitized solar cell.

  9. Efficient Spray-Coated Colloidal Quantum Dot Solar Cells

    NASA Astrophysics Data System (ADS)

    Moreno-Bautista, Gabriel

    Colloidal quantum dots (CQDs) offer the promise of low-cost, high-performance solar cells due to their ability to be synthesized and deposited from solution, which makes it possible for this material to be adapted to production-scale manufacturing protocols such as roll-to-roll (R2R) processing. Here we describe the design and implementation of a spray-coating process for the fabrication of CQD solar cells. We find that spray-coated films are morphologically superior to films that were fabricated using the conventional spin-coating method. Spray coating is found to be effective at removing an electronic trap caused by an organic impurity, enhancing the diffusion length of the CQD film and leading to an average power conversion efficiency (PCE) of 6.5%, which is higher than the average PCE of spin-coated cells (5.2%). We also show that the spray process can be adapted to R2R methodologies and can be used to fabricate efficient solar cells with unconventional form factors, such as surfaces with multiple dimensions of curvature.

  10. The molecular recognition of β-cyclodextrin modified CdSe quantum dots with tyrosine enantiomers: Theoretical calculation and experimental study

    NASA Astrophysics Data System (ADS)

    Cao, Yujuan; Wu, Shuangshuang; Liang, Yaozhen; Yu, Ying

    2013-01-01

    In the present work, the molecular recognition of mono-(6-mercapto)-β-cyclodextrin modified CdSe quantum dots (β-CD/CdSe QDs) with tyrosine enantiomers were investigated with theoretical calculation and fluorescence spectroscopy. The inclusion processes and the most probable structures of the inclusion complexes were simulated using PM3 energy scanning and optimization method. The trends of stability of the two inclusion complexes deduced from their calculated stabilization energies were studied. Moreover, the fluorescence spectra of β-CD/CdSe QDs in the presence of tyrosine enantiomers as well as the effect of ionic strength on the complexation of β-CD/CdSe QDs-tyrosine were discussed. The experimental results indicated that the β-CD/CdSe QDs have better enantioselectivity to L-tyrosine than that to D-tyrosine, and good linearity between the fluorescence intensity of β-CD/CdSe QDs and L-tyrosine over the concentration range from 0.10 × 10-4 mol/L to 4.00 × 10-4 mol/L with relative coefficient of 0.9909 was obtained. The experimental data agrees well with that obtained from theoretical calculation, indicating that β-cyclodextrin modified CdSe quantum dots contained good inclusion capability and fluorescence property, it has good potential application in the field of biological diagnosis, analysis, etc.

  11. Molecularly imprinted optosensing material based on hydrophobic CdSe quantum dots via a reverse microemulsion for specific recognition of ractopamine.

    PubMed

    Liu, Huilin; Fang, Guozhen; Wang, Shuo

    2014-05-15

    A novel molecularly imprinted polymer (MIP) based on hydrophobic CdSe quantum dots (QDs) was synthesized using a one-pot room-temperature reverse microemulsion polymerization, and this polymer was applied as a molecular recognition element to construct a ractopamine (RAC) optosensor. Here, hydrophobic CdSe QDs were first introduced to the hydrophilic analyte-imprinted polymer for highly selective and sensitive detection of RAC via the change in fluorescence intensity, because of the high-quality hydrophobic QDs with high quantum yield, sharp photoluminescence spectra and chemical and fluorescent stability. Under optimal conditions, the relative fluorescence intensity of MIP based on hydrophobic QDs decreased linearly with the increasing concentration of RAC in the range of 1.21 × 10(-9) -3.03 × 10(-6)mol L(-1) with a detection limit of 7.57 × 10(-10)mol L(-1), and the precision for five replicate detections of 1.51 × 10(-8)mol L(-1) RAC was 2.09% (relative standard deviation). The proposed method was successfully applied for the determination of trace RAC in pork samples, with good recoveries ranging from 82.79% to 97.23%. PMID:24370883

  12. Extracellular bio-production and characterization of small monodispersed CdSe quantum dot nanocrystallites

    NASA Astrophysics Data System (ADS)

    Suresh, Anil K.

    2014-09-01

    Engineered nanoparticles of diverse forms are being profoundly used for various applications and demand ecologically benign synthesis processes. Conventional chemical methods employed for the syntheses of nanoparticles are environmentally unfriendly and energy intensive. Biologically inspired biofabrication approaches that utilize naturally existing microorganisms or plant extracts or biomaterials might overcome these issues. The present investigation for the first time shows the synthesis of small and monodispersed cadmium selenide nanoparticles utilizing the plant pathogenic fungus, Helminthosporum solani upon incubating with an aqueous solution of CdCl2 and SeCl4 under ambient conditions. Multiple physical characterizations involving ultraviolet-visible and photoluminescence spectroscopy, transmission electron microscopy, selected area electron diffraction and X-ray photoelectron spectroscopy confirmed the production, purity, optical and surface characteristics, crystalline nature, size and shape distributions, and elemental composition of the nanoparticles. Pluralities of the particles are monodisperse spheres with a mean diameter of 5.5 ± 2 nm, are hydrophilic, highly stable with a broad photoluminescence and 1% quantum yield. This approach provides an alternative facile route for the biofabrication of quantum dot that is reliable, environmentally friendly, and lends itself directly for the creation of fluorescent biological labels.

  13. Fluorescence modulation in single CdSe quantum dots by moderate applied electric fields

    NASA Astrophysics Data System (ADS)

    LeBlanc, Sharonda J.; McClanahan, Mason R.; Moyer, Tully; Jones, Marcus; Moyer, Patrick J.

    2014-01-01

    Single molecule time-resolved fluorescence spectroscopy of CdSe/ZnS core-shell quantum dots (QDs) under the influence of moderate applied electric fields reveals distributed emission from states which are neither fully on nor off and pronounced changes in the excited state decay. The data suggest that a 54 kV/cm applied electric field causes small perturbations to the QD surface charge distribution, effectively increasing the surface trapping probability and resulting in the appearance of gray states. We present simultaneous blinking and fluorescence decay results for two sets of QDs, with and without an applied electric field. Further kinetic modeling analysis suggests that a single trapped charged cannot be responsible for a blinking off event.

  14. Delayed Exciton Emission and Its Relation to Blinking in CdSe Quantum Dots.

    PubMed

    Rabouw, Freddy T; Kamp, Marko; van Dijk-Moes, Relinde J A; Gamelin, Daniel R; Koenderink, A Femius; Meijerink, Andries; Vanmaekelbergh, Daniël

    2015-11-11

    The efficiency and stability of emission from semiconductor nanocrystal quantum dots (QDs) is negatively affected by "blinking" on the single-nanocrystal level, that is, random alternation of bright and dark periods. The time scales of these fluctuations can be as long as many seconds, orders of magnitude longer than typical lifetimes of exciton states in QDs. In this work, we investigate photoluminescence from QDs delayed over microseconds to milliseconds. Our results prove the existence of long-lived charge-separated states in QDs. We study the properties of delayed emission as a direct way to learn about charge carrier separation and recovery of the exciton state. A new microscopic model is developed to connect delayed emission to exciton recombination and blinking from which we conclude that bright periods in blinking are in fact not characterized by uninterrupted optical cycling as often assumed.

  15. Study of optical and structural properties of CdSe quantum dot embedded in PVA polymer matrix

    SciTech Connect

    Tyagi, Chetna Sharma, Ambika

    2015-08-28

    To enhance the properties and applicability of devices it is essential to incorporate semiconductor nanoparticles into polymer matrix. This introduces a new branch of science which includes device fabrications such as gas sensors, nonlinear optics, catalysis etc. Herein, we have synthesized CdSe/PVA nanocomposite (NC) material using wet chemical synthesis technique. The XRD studies revealed the formation of crystalline structure of CdSe nanoparticles (NP’s) and PVA NC’s with an average size of 100 nm and 5 nm respectively. Energy band gap is determined using UV-VIS Spectroscopy. A red shift in the absorption edge of CdSe/PVA NC is observed with respect to CdSe Np’s, The photoluminescence spectra also show red shift for CdSe/PVA NC as compared to CdSe NP’s Thus the use of CdSe/PVA for solar cell application would be more preferable than CdSe NP’s.

  16. Photo- and electroluminescence from semiconductor colloidal quantum dots in organic matrices: QD-OLED

    SciTech Connect

    Vitukhnovskii, A. G. Vaschenko, A. A.; Bychkovskii, D. N.; Dirin, D. N.; Tananaev, P. N.; Vakshtein, M. S.; Korzhonov, D. A.

    2013-12-15

    The results are reported of an experimental study of samples of organic light-emitting diodes (OLEDs) with luminescent layers fabricated on the basis of two types of CdSe/CdS/ZnS semiconductor quantum dots (QDs) with average CdSe core diameters of 3.2 and 4.1 nm and the same overall diameters of 6.5 nm. The dependences of the LED efficiency on the applied voltage are determined. Assumptions are made about ways of optimizing the design of high-efficiency LEDs.

  17. Near-unity quantum yields from chloride treated CdTe colloidal quantum dots.

    PubMed

    Page, Robert C; Espinobarro-Velazquez, Daniel; Leontiadou, Marina A; Smith, Charles; Lewis, Edward A; Haigh, Sarah J; Li, Chen; Radtke, Hanna; Pengpad, Atip; Bondino, Federica; Magnano, Elena; Pis, Igor; Flavell, Wendy R; O'Brien, Paul; Binks, David J

    2015-04-01

    Colloidal quantum dots (CQDs) are promising materials for novel light sources and solar energy conversion. However, trap states associated with the CQD surface can produce non-radiative charge recombination that significantly reduces device performance. Here a facile post-synthetic treatment of CdTe CQDs is demonstrated that uses chloride ions to achieve near-complete suppression of surface trapping, resulting in an increase of photoluminescence (PL) quantum yield (QY) from ca. 5% to up to 97.2 ± 2.5%. The effect of the treatment is characterised by absorption and PL spectroscopy, PL decay, scanning transmission electron microscopy, X-ray diffraction and X-ray photoelectron spectroscopy. This process also dramatically improves the air-stability of the CQDs: before treatment the PL is largely quenched after 1 hour of air-exposure, whilst the treated samples showed a PL QY of nearly 50% after more than 12 hours.

  18. XANES: observation of quantum confinement in the conduction band of colloidal PbS quantum dots

    NASA Astrophysics Data System (ADS)

    Demchenko, I. N.; Chernyshova, M.; He, X.; Minikayev, R.; Syryanyy, Y.; Derkachova, A.; Derkachov, G.; Stolte, W. C.; Piskorska-Hommel, E.; Reszka, A.; Liang, H.

    2013-04-01

    The presented investigations aimed at development of inexpensive method for synthesized materials suitable for utilization of solar energy. This important issue was addressed by focusing, mainly, on electronic local structure studies with supporting x-ray diffraction (XRD) and transmission electron microscopy (TEM) analysis of colloidal galena nano-particles (NPs) and quantum dots (QDs) synthesized using wet chemistry under microwave irradiation. Performed x-ray absorption near edge structure (XANES) analysis revealed an evidence of quantum confinement for the sample with QDs, where the bottom of the conduction band was shifted to higher energy. The QDs were found to be passivated with oxides at the surface. Existence of sulfate/sulfite and thiosulfate species in pure PbS and QDs, respectively, was identified.

  19. Role of ZnS shell on stability, cytotoxicity, and photocytotoxicity of water-soluble CdSe semiconductor quantum dots surface modified with glutathione

    NASA Astrophysics Data System (ADS)

    Ibrahim, Salwa Ali; Ahmed, Wafaa; Youssef, Tareq

    2014-09-01

    Biomedical applications of quantum dots (QDs) have become a subject of a considerable concern in the past few decades. The present study examines the stability and cytotoxicity of two QDs systems in cell culture medium in the presence and absence of a thin layer of ZnS shell. The two systems were built from core, CdSe QDs, surface modified with glutathione (GSH), named CdSe˜GSH and CdSe/ZnS˜GSH. Our results demonstrated that 0.7 nm layer of ZnS shell played a significant role in the stability of CdSe/ZnS~GSH QDs in supplemented cell culture medium (RPMI). Also, a significant improvement in the physicochemical properties of the core CdSe QDs was shown by maintaining their spectroscopic characteristics in RPMI medium due to the wide band gap of ZnS shell. Both systems showed insignificant reduction in cell viability of HFB-4 or MCF-7 cell lines in the dark which was attributed to the effective GSH coating. Following photoirradiation with low laser power (irradiance 10 mW cm-2), CdSe~GSH QDs showed a significant decrease in cell viability after 60 min irradiation which may result from detachment of GSH molecules. Under the same irradiation condition, CdSe/ZnS~GSH QDs showed insignificant decrease in cell viability or after 2 h incubation from laser irradiation which was attributed to the strong binding between ZnS and GSH coatings. It can be concluded that the stability of CdSe core QDs was significantly improved in cell culture medium by encapsulation with a thin layer of ZnS shell whereas their cytotoxicity and photo-cytotoxicity are highly dependent on surface modification.

  20. Comparison of Toxicity of CdSe: ZnS Quantum Dots on Male Reproductive System in Different Stages of Development in Mice

    PubMed Central

    Amiri, Gholamreza; Valipoor, Akram; Parivar, Kazem; Modaresi, Mehrdad; Noori, Ali; Gharamaleki, Hamideh; Taheri, Jafar; Kazemi, Ali

    2016-01-01

    Background Quantum dots (QDs) are new types of fluorescent materials for biological labeling. QDs toxicity study is an essential requirement for future clinical applications. Therefore, this study aimed to evaluate cytotoxic effects of CdSe: ZnS QDs on male reproductive system. Materials and Methods In this experimental study, the different concentrations of CdSe: ZnS QDs (10, 20 and 40 mg/kg) were injected to 32 male mice (adult group) and 24 pregnant mice (embryo group) on day 8 of gestation. The histological changes of testis and epididymis were studied by a light microscopy, and the number of seminiferous tubules between two groups was compared. One-way analysis of variance (one-way Anova) using the Statistical Package for the Social Sciences (SPSS, SPSS Inc., USA) version 16 were performed for statistical analysis. Results In adult group, histological studies of testis tissues showed a high toxicity of CdSe: ZnS in 40 mg/kg dose followed by a decrease in lamina propria; destruction in interstitial tissue; deformation of seminiferous tubules; and a reduction in number of spermatogonia, spermatocytes, and spermatids. However, there was an interesting result in fetal testis development, meaning there was no significant effect on morphology and structure of the seminiferous tubules and number of sperm stem cells. Also histological study of epididymis tissues in both groups (adult and embryo groups) showed no significant effect on morphology and structure of tubule and epithelial cells, but there was a considerable reduction in number of spermatozoa in the lumen of the epididymal duct in 40 mg/kg dose of adult group. Conclusion The toxicity of QDs on testicular tissue of the mice embryo and adult are different before and after puberty. Due to lack of research in this field, this study can be an introduction to evaluate the toxicity of QDs on male reproduction system in different stages of development. PMID:26985339

  1. Interband optical transition energy and oscillator strength in a lead based CdSe quantum dot quantum well heterostructure

    SciTech Connect

    Saravanamoorthy, S. N.; Peter, A. John

    2015-06-24

    Binding energies of the exciton and the interband optical transition energies are studied in a CdSe/Pb{sub 1-x}Cd{sub x}Se/CdSe spherical quantum dot-quantum well nanostructure taking into account the geometrical confinement effect. The core and shell are taken as the same material. The initial and final states of energy and the overlap integrals of electron and hole wave functions are determined by the oscillator strength. The oscillator strength and the radiative transition life time with the dot radius are investigated for various Cd alloy content in the core and shell materials.

  2. Self assembly and optical properties of CdSe nanoplatelet superlattice

    NASA Astrophysics Data System (ADS)

    Gao, Yunan; Tisdale, William; Tisdale Lab MIT Team

    Colloidal CdSe nanoplatelets (NPs) are 1-D confined materials with atomic uniform thickness, and only have homogeneous broadening in energy level distributions and very narrow emission spectrum. Additionally, NPs have a giant oscillator strength that leads to a faster emission rate compared to quantum dots and rods. Due to these properties, NPs have shown promising potential applications in light-emitting diodes, colloidal lasers, and harvesting multiple exciton generation in photovoltaic cells.Self-assembly of superlattice has been studied broadly for many nano-particles, but not yet for CdSe NPs. We will show for the first time a selective control of CdSe NP superlattice self-assembly, i.e., self-assembled into columnar or lamellar superlattice. Moreover, we will present that the assembly morphology of superlattice has direct effects on their optical properties, like polarization, absorption efficiency and emission rate, etc., and also on their Forster energy transfer properties. The self-assembly is based on liquid interfacial self-assembly and transfer technique. The structure and propertied of the superlattice are characterized by transmission electron microscopy, and time-, polarization- and space-resolved photo-luminescent micro-spectroscopy.

  3. Quantum dots laser desorption/ionization MS: multifunctional CdSe quantum dots as the matrix, concentrating probes and acceleration for microwave enzymatic digestion for peptide analysis and high resolution detection of proteins in a linear MALDI-TOF MS.

    PubMed

    Shrivas, Kamlesh; Kailasa, Suresh Kumar; Wu, Hui-Fen

    2009-05-01

    We report the first use of functionalized cadmium selinide quantum dots (CdSe QDs) with 11-mercaptoundecanoic acid (MUA) as the matrix for the selective ionization of proteins with high resolution and rapid analysis of amino acids and peptides by using quantum dots laser desorption/ionization mass spectrometry (QDLDI-MS). The mercaptocarboxylic groups of CdSe QDs have been known to be an effective affinity probe to interact with the biomolecules at low abundance level. Using these QDs as the matrix, sensitivity of the method was greatly enhanced and the LOQ of peptides was found to be 100 pM with RSD <10%. The QDLDI-MS is capable for the selective ionization of insulin, lysozyme and myoglobin with high resolution, which is not observed with sinapic acid (SA) as the matrix. The QDLDI-MS technique offers many advantages for the analysis of amino acids, peptides and proteins with regard to simplicity, rapidity, sensitivity and the mass spectra were generated in the presence of signal suppressors such as urea and Trition X-100. In addition, the CdSe QDs have been successfully applied as preconcentrating probes for the analysis of digested peptides in lysozyme from chicken egg white by microwave-assisted enzymatic digestion. This indicates that the QDs are able to absorb radiation from microwave and their ability to trap peptides from microwave-digested lysozyme. These results demonstrate that the CdSe QDs are promising candidates for the selective ionization of the analytes with an accurate platform to the rapid screening of biomolecules. PMID:19391181

  4. Single-step fabrication of quantum funnels via centrifugal colloidal casting of nanoparticle films

    PubMed Central

    Kim, Jin Young; Adinolfi, Valerio; Sutherland, Brandon R.; Voznyy, Oleksandr; Kwon, S. Joon; Kim, Tae Wu; Kim, Jeongho; Ihee, Hyotcherl; Kemp, Kyle; Adachi, Michael; Yuan, Mingjian; Kramer, Illan; Zhitomirsky, David; Hoogland, Sjoerd; Sargent, Edward H.

    2015-01-01

    Centrifugal casting of composites and ceramics has been widely employed to improve the mechanical and thermal properties of functional materials. This powerful method has yet to be deployed in the context of nanoparticles—yet size–effect tuning of quantum dots is among their most distinctive and application-relevant features. Here we report the first gradient nanoparticle films to be constructed in a single step. By creating a stable colloid of nanoparticles that are capped with electronic-conduction-compatible ligands we were able to leverage centrifugal casting for thin-films devices. This new method, termed centrifugal colloidal casting, is demonstrated to form films in a bandgap-ordered manner with efficient carrier funnelling towards the lowest energy layer. We constructed the first quantum-gradient photodiode to be formed in a single deposition step and, as a result of the gradient-enhanced electric field, experimentally measured the highest normalized detectivity of any colloidal quantum dot photodetector. PMID:26165185

  5. Single-step fabrication of quantum funnels via centrifugal colloidal casting of nanoparticle films.

    PubMed

    Kim, Jin Young; Adinolfi, Valerio; Sutherland, Brandon R; Voznyy, Oleksandr; Kwon, S Joon; Kim, Tae Wu; Kim, Jeongho; Ihee, Hyotcherl; Kemp, Kyle; Adachi, Michael; Yuan, Mingjian; Kramer, Illan; Zhitomirsky, David; Hoogland, Sjoerd; Sargent, Edward H

    2015-07-13

    Centrifugal casting of composites and ceramics has been widely employed to improve the mechanical and thermal properties of functional materials. This powerful method has yet to be deployed in the context of nanoparticles--yet size-effect tuning of quantum dots is among their most distinctive and application-relevant features. Here we report the first gradient nanoparticle films to be constructed in a single step. By creating a stable colloid of nanoparticles that are capped with electronic-conduction-compatible ligands we were able to leverage centrifugal casting for thin-films devices. This new method, termed centrifugal colloidal casting, is demonstrated to form films in a bandgap-ordered manner with efficient carrier funnelling towards the lowest energy layer. We constructed the first quantum-gradient photodiode to be formed in a single deposition step and, as a result of the gradient-enhanced electric field, experimentally measured the highest normalized detectivity of any colloidal quantum dot photodetector.

  6. The influence of capping thioalkyl acid on the growth and photoluminescence efficiency of CdTe and CdSe quantum dots.

    PubMed

    Aldeek, Fadi; Balan, Lavinia; Lambert, Jacques; Schneider, Raphaël

    2008-11-26

    The influence of thioalkyl acid ligand was evaluated during aqueous synthesis at 100 °C and under hydrothermal conditions (150 °C) of CdTe and CdSe quantum dots (QDs). Experiments performed with 3-mercaptopropionic acid (MPA), 6-mercaptohexanoic acid (MHA) and 11-mercaptoundecanoic acid (MUA) demonstrated that the use of MHA and MUA allowed for the preparation of very small nanoparticles (0.6-2.5 nm) in carrying out the reaction under atmospheric pressure or in an autoclave and that the photophysical properties of QDs were dependent on the ligand and on the synthesis conditions. The influence of various experimental conditions, including the Te-to-Cd ratio, temperature, and precursor concentration, on the growth rate of CdTe or CdSe QDs has been systematically investigated. The fluorescence intensities of CdTe QDs capped with MPA, MHA, or MUA versus pH were also found to be related to the surface coverage of the nanoparticles. PMID:21836270

  7. Differences in soil mobility and degradability between water-dispersible CdSe and CdSe/ZnS quantum dots.

    PubMed

    Navarro, Divina A; Banerjee, Sarbajit; Watson, David F; Aga, Diana S

    2011-08-01

    The relative leaching potential and degradation of water-dispersible CdSe and CdSe/ZnS quantum dots (QDs) were evaluated using small-scale soil columns. The potential of QDs to release toxic Cd(2+) and/or Se(2-)/SeO(3)(2-) ions upon degradation is of environmental concern and warrants investigation. Both classes of QDs exhibited limited soil mobility in CaCl(2), with more than 70% of the total Cd and Se species from QDs retained in the top soil after passing 10 column volumes of solution through the soil column. However, mobilization of Cd- and Se-species was observed when EDTA was used as the leaching solution. Approximately 98% of the total Cd(2+) loaded leached out from the Cd(2+)-spiked soil, while only 30% and 60% leached out from the CdSe and CdSe/ZnS QD-spiked soils, respectively. Soil column profiles and analysis of leachates suggest that intact QDs leached through the soil. Longer incubation (15 days) in soil prior to leaching indicated some degradation and/or surface modification of both QDs. These results suggest that chelating agents in the environment can enhance the soil mobility of intact and degraded QDs. It is apparent that QDs in soil, including the polymer-coated CdSe/ZnS QDs that are generally assumed to possess a higher degree of environmental stability, can undergo chemical transformations, which subsequently dictate their overall mobility.

  8. Colloidal CdSe nanocrystals from tri-n-octylphosphine: Part II: control of growth rate for high quality and large-scale production by tuning Cd-to-Se stoichiometry.

    PubMed

    Yu, Kui; Zaman, Badruz; Ripmeester, John A

    2005-04-01

    Colloidal CdSe nanocrystals were synthesized in reaction media consisting of tri-n-octylphosphine (TOP) without addition of other species; the single-step approach used cadmium oxide (CdO) and TOPSe as Cd and Se sources, respectively. The temporal evolution of the optical properties of the growing TOP-capped CdSe nanocrystals was monitored for a couple of hours, showing that there are two distinguishable stages of growth: an early stage (less than 5 minutes) and a later stage; the growth kinetics of the two stages is a function of the Cd-to-Se precursor molar ratios. A rational choice of 2-6Cd-to-1Se molar ratio was found, based on the temporal evolution of the photoluminescent (PL) efficiency (studied as PL intensity and sensitivity to the media of dispersion, and non-resonant Stokes shifts). For a 2Cd-to-1Se synthesis, the growth in size was slow in the early stages and became fast in the later stages; this fast-later-stage feature could be suppressed by going to a synthesis with a 4-6Cd-to-1Se mole ratio: the nanocrystals between 0.5-60 min growth time exhibit very much similar optical properties, with less than 19 nm redshift of bandgap absorption and emission occurring. Thus, the synthetic route developed here, with a rational 4-6Cd-to-1Se molar ratio, enables us to produce high-quality CdSe nanocrystals on a large-scale with a high degree of synthetic reproducibility. The insights gained facilitate a deeper understanding of the concept of what constitutes high-quality nano-crystals: high PL efficiency resulting from a low growth rate, which can be thoroughly and readily investigated by the red-shift rate of the band-gap peak positions; in addition, the insights gained help us to define a proper synthetic approach for large-scale production with high-quality product.

  9. Photoluminenscence blinking dynamics of colloidal quantum dots in the presence of controlled external electron traps.

    PubMed

    Xu, Zhihua; Cotlet, Mircea

    2012-01-23

    The effect of the external charge trap on the photoluminescence blinking dynamics of individual colloidal quantum dots is investigated with a series of colloidal quantum dot-bridge-fullerene dimers with varying bridge lengths, where the fullerene moiety acts as a well-defined, well-positioned external charge trap. It is found that charge transfer followed by charge recombination is an important mechanism in determining the blinking behavior of quantum dots when the external trap is properly coupled with the excited state of the quantum dot, leading to a quasi-continuous distribution of 'on' states and an early fall-off from a power-law distribution for both 'on' and 'off' times associated with quantum dot photoluminescence blinking.

  10. Photoluminescence Blinking Dynamics of Colloidal Quantum Dots in the Presence of Controlled External Electron Traps

    SciTech Connect

    Cotlet, M.; Xu, Z.

    2012-01-23

    The effect of the external charge trap on the photoluminescence blinking dynamics of individual colloidal quantum dots is investigated with a series of colloidal quantum dot-bridge-fullerene dimers with varying bridge lengths, where the fullerene moiety acts as a well-defined, well-positioned external charge trap. It is found that charge transfer followed by charge recombination is an important mechanism in determining the blinking behavior of quantum dots when the external trap is properly coupled with the excited state of the quantum dot, leading to a quasi-continuous distribution of 'on' states and an early fall-off from a power-law distribution for both 'on' and 'off' times associated with quantum dot photoluminescence blinking.

  11. Quantum efficiency of colloidal suspensions containing quantum dot/silica hybrid particles

    NASA Astrophysics Data System (ADS)

    Jeon, Hyungjoon; Yoon, Cheolsang; Lee, Sooho; Lee, Doh C.; Shin, Kyusoon; Lee, Kangtaek

    2016-10-01

    We have investigated the fluorescence properties of colloidal suspensions conntaining quantum dot (QD)/silica hybrid particles. First, we synthesized QD/silica hybrid particles with silica-QD-silica (SQS) core-shell-shell geometry, and monitored the quantum efficiencies of their suspensions at various particle concentrations. We found that the quantum efficiency (QE) of SQS particles in deionized (DI) water was much lower than that of the QDs even at low particle concentration, mainly due to the light scattering of emitted photons at the silica/water interface, followed by reabsorption by QDs. As the concentration of SQS particles was increased, both light scattering and reabsorption by QDs became more important, which further reduced the QE. Refractive index-matched solvent, however, reduced light scattering, yielding greater QE than DI water. Next, we induced aggregation of SQS particles, and found that QE increased as particles aggregated in DI water because of reduced light scattering and reabsorption, whereas it remained almost constant in the refractive index-matched solvent. Finally, we studied aggregation of highly concentrated silica particle suspensions containing a low concentration of SQS particles, and found that QE increased with aggregation because light scattering and reabsorption were reduced.

  12. Quantum efficiency of colloidal suspensions containing quantum dot/silica hybrid particles.

    PubMed

    Jeon, Hyungjoon; Yoon, Cheolsang; Lee, Sooho; Lee, Doh C; Shin, Kyusoon; Lee, Kangtaek

    2016-10-28

    We have investigated the fluorescence properties of colloidal suspensions conntaining quantum dot (QD)/silica hybrid particles. First, we synthesized QD/silica hybrid particles with silica-QD-silica (SQS) core-shell-shell geometry, and monitored the quantum efficiencies of their suspensions at various particle concentrations. We found that the quantum efficiency (QE) of SQS particles in deionized (DI) water was much lower than that of the QDs even at low particle concentration, mainly due to the light scattering of emitted photons at the silica/water interface, followed by reabsorption by QDs. As the concentration of SQS particles was increased, both light scattering and reabsorption by QDs became more important, which further reduced the QE. Refractive index-matched solvent, however, reduced light scattering, yielding greater QE than DI water. Next, we induced aggregation of SQS particles, and found that QE increased as particles aggregated in DI water because of reduced light scattering and reabsorption, whereas it remained almost constant in the refractive index-matched solvent. Finally, we studied aggregation of highly concentrated silica particle suspensions containing a low concentration of SQS particles, and found that QE increased with aggregation because light scattering and reabsorption were reduced. PMID:27658534

  13. Quantum funneling in blended multi-band gap core/shell colloidal quantum dot solar cells

    SciTech Connect

    Neo, Darren C. J.; Assender, Hazel E.; Watt, Andrew A. R.; Stranks, Samuel D.; Eperon, Giles E.; Snaith, Henry J.

    2015-09-07

    Multi-band gap heterojunction solar cells fabricated from a blend of 1.2 eV and 1.4 eV PbS colloidal quantum dots (CQDs) show poor device performance due to non-radiative recombination. To overcome this, a CdS shell is epitaxially formed around the PbS core using cation exchange. From steady state and transient photoluminescence measurements, we understand the nature of charge transfer between these quantum dots. Photoluminescence decay lifetimes are much longer in the PbS/CdS core/shell blend compared to PbS only, explained by a reduction in non-radiative recombination resulting from CdS surface passivation. PbS/CdS heterojunction devices sustain a higher open-circuit voltage and lower reverse saturation current as compared to PbS-only devices, implying lower recombination rates. Further device performance enhancement is attained by modifying the composition profile of the CQD species in the absorbing layer resulting in a three dimensional quantum cascade structure.

  14. Quantum efficiency of colloidal suspensions containing quantum dot/silica hybrid particles.

    PubMed

    Jeon, Hyungjoon; Yoon, Cheolsang; Lee, Sooho; Lee, Doh C; Shin, Kyusoon; Lee, Kangtaek

    2016-10-28

    We have investigated the fluorescence properties of colloidal suspensions conntaining quantum dot (QD)/silica hybrid particles. First, we synthesized QD/silica hybrid particles with silica-QD-silica (SQS) core-shell-shell geometry, and monitored the quantum efficiencies of their suspensions at various particle concentrations. We found that the quantum efficiency (QE) of SQS particles in deionized (DI) water was much lower than that of the QDs even at low particle concentration, mainly due to the light scattering of emitted photons at the silica/water interface, followed by reabsorption by QDs. As the concentration of SQS particles was increased, both light scattering and reabsorption by QDs became more important, which further reduced the QE. Refractive index-matched solvent, however, reduced light scattering, yielding greater QE than DI water. Next, we induced aggregation of SQS particles, and found that QE increased as particles aggregated in DI water because of reduced light scattering and reabsorption, whereas it remained almost constant in the refractive index-matched solvent. Finally, we studied aggregation of highly concentrated silica particle suspensions containing a low concentration of SQS particles, and found that QE increased with aggregation because light scattering and reabsorption were reduced.

  15. Synthesis of a CdSe-graphene hybrid composed of CdSe quantum dot arrays directly grown on CVD-graphene and its ultrafast carrier dynamics

    NASA Astrophysics Data System (ADS)

    Kim, Yong-Tae; Shin, Hee-Won; Ko, Young-Seon; Ahn, Tae Kyu; Kwon, Young-Uk

    2013-01-01

    We report the original fabrication and performance of a photocurrent device that uses directly grown CdSe quantum dots (QDs) on a graphene basal plane. The direct junction between the QDs and graphene and the high quality of the graphene grown by chemical vapor deposition enables highly efficient electron transfer from the QDs to the graphene. Therefore, the hybrids show large photocurrent effects with a fast response time and shortened photoluminescence (PL) lifetime. The PL lifetime quenching can be explained as being due to the efficient electron transfer as evidenced by femtosecond transient absorption spectroscopy. These hybrids are expected to find applications in flexible electronics and optoelectronic devices.We report the original fabrication and performance of a photocurrent device that uses directly grown CdSe quantum dots (QDs) on a graphene basal plane. The direct junction between the QDs and graphene and the high quality of the graphene grown by chemical vapor deposition enables highly efficient electron transfer from the QDs to the graphene. Therefore, the hybrids show large photocurrent effects with a fast response time and shortened photoluminescence (PL) lifetime. The PL lifetime quenching can be explained as being due to the efficient electron transfer as evidenced by femtosecond transient absorption spectroscopy. These hybrids are expected to find applications in flexible electronics and optoelectronic devices. Electronic supplementary information (ESI) available: TEM data of MSTF, AFM data of T-QD-G samples, PL decay fitting results to the multiexponential decay equation, photoconductivity data of T-QD-2LG with two different illumination wavelengths, photocurrent efficiencies of QD-G hybrids prepared in various ways, photoconductivity and photoresponse data of T-QD-2LG and T-QD-3LG, and the bending stress on a PET film. See DOI: 10.1039/c2nr33294a

  16. The Dynamic Organic/Inorganic Interface of Colloidal PbS Quantum Dots.

    PubMed

    Grisorio, Roberto; Debellis, Doriana; Suranna, Gian Paolo; Gigli, Giuseppe; Giansante, Carlo

    2016-06-01

    Colloidal quantum dots are composed of nanometer-sized crystallites of inorganic semiconductor materials bearing organic molecules at their surface. The organic/inorganic interface markedly affects forms and functions of the quantum dots, therefore its description and control are important for effective application. Herein we demonstrate that archetypal colloidal PbS quantum dots adapt their interface to the surroundings, thus existing in solution phase as equilibrium mixtures with their (metal-)organic ligand and inorganic core components. The interfacial equilibria are dictated by solvent polarity and concentration, show striking size dependence (leading to more stable ligand/core adducts for larger quantum dots), and selectively involve nanocrystal facets. This notion of ligand/core dynamic equilibrium may open novel synthetic paths and refined nanocrystal surface-chemistry strategies.

  17. The Dynamic Organic/Inorganic Interface of Colloidal PbS Quantum Dots.

    PubMed

    Grisorio, Roberto; Debellis, Doriana; Suranna, Gian Paolo; Gigli, Giuseppe; Giansante, Carlo

    2016-06-01

    Colloidal quantum dots are composed of nanometer-sized crystallites of inorganic semiconductor materials bearing organic molecules at their surface. The organic/inorganic interface markedly affects forms and functions of the quantum dots, therefore its description and control are important for effective application. Herein we demonstrate that archetypal colloidal PbS quantum dots adapt their interface to the surroundings, thus existing in solution phase as equilibrium mixtures with their (metal-)organic ligand and inorganic core components. The interfacial equilibria are dictated by solvent polarity and concentration, show striking size dependence (leading to more stable ligand/core adducts for larger quantum dots), and selectively involve nanocrystal facets. This notion of ligand/core dynamic equilibrium may open novel synthetic paths and refined nanocrystal surface-chemistry strategies. PMID:27038221

  18. CdSe quantum dot-functionalized TiO2 nanohybrids as a visible light induced photoelectrochemical platform for the detection of proprotein convertase subtilisin/kexin type 6.

    PubMed

    Pang, Xuehui; Pan, Jihong; Wang, Lin; Ren, Wei; Gao, Picheng; Wei, Qin; Du, Bin

    2015-09-15

    Proprotein convertase subtilisin/kexin type 6 (PCSK6) plays a major role in promoting the progression of rheumatoid arthritis to a higher aggressive status. A novel highly sensitive photoelectrochemical platform was developed for the detection of PCSK6 by using CdSe quantum dots (QDs)-functionalized TiO2 nanoparticles (NPs) nanohybrids (TiO2@CdSe) as the photo-to-electron conversion medium. TiO2@CdSe showed excellent visible-light absorbency, and much higher photoelectrochemical activity than both CdSe QDs and TiO2 NPs. The 5' and 3' primers of PCSK6 ssDNA acted as capture probes to realize the detection of PCSK6 ssDNA by the specific recognition. The capture probes can be fixed by poly-l-lysine (PLL) through positively strong electrostatic attraction and the carboxyl group of TiO2@CdSe nanohybrids. PLL was electropolymerized on ITO electrode by cyclic voltammetry (CV). Simultaneously, the amino group of PLL can interact with the carboxyl group of TiO2@CdSe nanohybrids to enhance the stability of the photoelectrochemical signal. The fabricated aptsensor exhibited excellent performance towards PCSK6 with a wide linear range (0.5 pg/mL to 80.0 ng/mL) and a detection limit of 0.1 fg/mL. This work opens up a new detection platform for PCSK6 with good sensitivity, reproducibility and stability. PMID:25889349

  19. Background limited mid-infrared photodetection with photovoltaic HgTe colloidal quantum dots

    NASA Astrophysics Data System (ADS)

    Guyot-Sionnest, Philippe; Roberts, John Andris

    2015-12-01

    The photovoltaic response of thin films of HgTe colloidal quantum dots in the 3-5 μm range is observed. With no applied bias, internal quantum efficiency exceeding 40%, specific detectivity above 1010 Jones and microseconds response times are obtained at 140 K. The cooled devices detect the ambient thermal radiation. A detector with 5.25 μm cut-off achieves Background Limited Infrared Photodetection at 90 K.

  20. Background limited mid-infrared photodetection with photovoltaic HgTe colloidal quantum dots

    SciTech Connect

    Guyot-Sionnest, Philippe Roberts, John Andris

    2015-12-21

    The photovoltaic response of thin films of HgTe colloidal quantum dots in the 3–5 μm range is observed. With no applied bias, internal quantum efficiency exceeding 40%, specific detectivity above 10{sup 10} Jones and microseconds response times are obtained at 140 K. The cooled devices detect the ambient thermal radiation. A detector with 5.25 μm cut-off achieves Background Limited Infrared Photodetection at 90 K.

  1. Investigations into photo-excited state dynamics in colloidal quantum dots

    NASA Astrophysics Data System (ADS)

    Singh, Gaurav

    Colloidal Quantum dots (QDs) have garnered considerable scientific and technological interest as a promising material for next generation solar cells, photo-detectors, lasers, bright light-emitting diodes (LEDs), and reliable biomarkers. However, for practical realization of these applications, it is crucial to understand the complex photo-physics of QDs that are very sensitive to surface chemistry and chemical surroundings. Depending on the excitation density, QDs can support single or multiple excitations. The first part of this talk addresses evolution of QD excited state dynamics in the regime of low excitation intensity. We use temperature-resolved time-resolved fluorescence spectroscopy to study exciton dynamics from picoseconds to microseconds and use kinetic modeling based on classical electron transfer to show the effect of surface trap states on dynamics of ground-state exciton manifold in core-shell CdSe/CdS QDs. We show that the thickness of CdS shell plays an important role in interaction of CdSe core exciton states with nanocrystal environment, and find that a thicker shell can minimize the mixing of QD exciton states with surface trap states. I will then present an investigation into the dynamics of multiply-excited states in QDs. One of the key challenges in QD spectroscopy is to reliably distinguish multi- from single-excited states that have similar lifetime components and spectroscopic signatures. I will describe the development of a novel multi-pulse fluorescence technique to selectively probe multi-excited states in ensemble QD samples and determine the nature of the multi-excited state contributing to the total fluorescence even in the limit of low fluorescent yields. We find that in our sample of CdSe/CdS core/shell QDs the multi-excited emission is dominated by emissive trion states rather than biexcitons. Next, I will discuss the application of this technique to probe exciton-plasmon coupling in layered hybrid films of QD/gold nanoparticles

  2. Air-stable operation of transparent, colloidal quantum dot based LEDs with a unipolar device architecture.

    PubMed

    Wood, Vanessa; Panzer, Matthew J; Caruge, Jean-Michel; Halpert, Jonathan E; Bawendi, Moungi G; Bulović, Vladimir

    2010-01-01

    We report a novel unipolar light-emitting device architecture that operates using direct-current, field-driven electroluminescence of colloidally synthesized quantum dots (QDs). This device architecture, which is based only on transparent ceramics and QDs, enables emission from different color QDs and, for the first time, constant QD electroluminescence during extended operation in air, unpackaged.

  3. Red, green, and blue lasing enabled by single-exciton gain in colloidal quantum dot films

    DOEpatents

    Nurmikko, Arto V.; Dang, Cuong

    2016-06-21

    The methods and materials described herein contemplate the use films of colloidal quantum dots as a gain medium in a vertical-cavity surface-emitting laser. The present disclosure demonstrates a laser with single-exciton gain in the red, green, and blue wavelengths. Leveraging this nanocomposite gain, the results realize a significant step toward full-color single-material lasers.

  4. Chemical control of the photoluminescence of CdSe quantum dot-organic complexes with a series of para-substituted aniline ligands.

    PubMed

    Knowles, Kathryn E; Tice, Daniel B; McArthur, Eric A; Solomon, Gemma C; Weiss, Emily A

    2010-01-27

    Replacement of the native (as-synthesized) ligands of colloidal CdSe QDs with varying concentrations of a series of para-substituted anilines (R-An), where R ranges from strongly electron-withdrawing to strongly electron-donating, decreases the PL of the QDs. The molar ratio of R-An to QD ([R-An]:[QD]) at which the PL decreases by 50% shifts by 4 orders of magnitude over the series R-An. The model employed to describe the data combines a Freundlich binding isotherm (which reflects the dependence of the binding affinity of the amine headgroups of R-An on the substituent R) with a function that describes the response of the PL to R-An ligands once they are bound at their equilibrium surface coverage. The latter function includes as a parameter the rate constant, k(nr), for nonradiative decay of the exciton at a site to which an R-An ligand is coordinated. The value of this parameter reveals that the predominant mechanism of QD-ligand interaction is passivation of Cd(2+) surface sites through sigma-donation for R-An ligands with R = H, Br, OCF(3), and reductive quenching through photoinduced hole transfer for R = MeO, (Me)(2)N.

  5. Colloidal transition-metal-doped ZnO quantum dots.

    PubMed

    Radovanovic, Pavle V; Norberg, Nick S; McNally, Kathryn E; Gamelin, Daniel R

    2002-12-25

    Methods for introducing new magnetic, optical, electronic, photophysical, or photochemical properties to semiconductor nanocrystals are attracting intense applications-oriented interest. In this communication, we report the preparation and electronic absorption spectroscopy of colloidal ZnO DMS-QDs. Our synthetic procedure involves modification of literature methods known to yield highly crystalline and relatively monodisperse nanocrystals of pure ZnO to allow introduction of transition-metal dopants. We use ligand-field electronic absorption spectroscopy as a dopant-specific optical probe to monitor dopant incorporation during nanocrystal growth and to verify internal substitutional doping in Co2+:ZnO and Ni2+:ZnO DMS-QDs. To the best of our knowledge, these are the first free-standing oxide DMS-QDs reported. The synthesis of colloidal oxide DMS-QDs introduces a new category of magnetic semiconductor materials available for detailed physical study and application in nanotechnology.

  6. Colloidal CdSe nanocrystals from tri-n-octylphosphine with various Cd sources: Control of a slow growth for high-quality and large-scale production

    NASA Astrophysics Data System (ADS)

    Yu, Kui; Zaman, Badruz; Taal, Remon; Ripmeester, John A.

    2005-09-01

    A slow growth in size at the early stages of reaction, together with a period of zero growth in size and size distribution is observed via monitoring the temporal evolution of the optical properties of the growing CdSe nanocrystals from reaction media consisting of tri-n-octylphosphine (TOP). The synthetic approach is as simple as a swift injection of a TOPSe/TOP solution into a Cd-source/TOP solution at 300 °C with subsequent growth at 250 °C. The various Cd sources investigated are cadmium acetate (Cd(Ac)2), cadmium oxide (CdO)/tetradecylphosphonic acid (TDPA), CdO, and CdO/oleylamine (OLA). With these various Cd sources studied, CdO with a 4Cd-to-1Se stoichiometry demonstrates its suitability for high-quality and large-scale production, due to a slow growth in size (less than 17 nm redshift of bandgap absorption and emission) and size distribution, as well as fairly constant photoluminescent properties of the growing nanocrystals during the 0.5-60 min growth time.

  7. Preparative size-exclusion chromatography for purification and characterization of colloidal quantum dots bound by chromophore-labeled polymers and low-molecular-weight chromophores.

    PubMed

    Wang, Mingfeng; Bardajee, Ghasem Rezanejade; Kumar, Sandeep; Nitz, Mark; Scholes, Gregory D; Winnik, Mitchell A

    2009-06-19

    We explore the use of preparative size-exclusion chromatography (SEC) and high-performance liquid chromatography (HPLC) to purify quantum dots (QDs) after surface modification. In one example, in which Bio-Beads (S-X1) were used as the packing material for the preparative SEC column, CdSe QDs treated with a functional coumarin dye could be separated from the excess free dye by using tetrahydrofuran (THF) as the mobile phase. This column was unable to separate polymer-coated QDs from free polymer (M approximately 8000) because of the relatively low cutoff mass of the column. Here a preparative HPLC column packed with TOYOPEARL gel allowed the effective separation of polymer-bound QDs from the excess free polymer by using N-methyl-2-pyrrolidinone (NMP) as the mobile phase. When other solvents such as absolute ethanol, acetonitrile, THF, and THF-triethylamine mixtures were used as the eluent, QDs stuck to the column. While NMP was an effective medium to remove excess free polymer from the QDs, it was difficult to transfer the purified QDs to more volatile solvents and maintain colloidal stability.

  8. Novel magnetic Fe3O4@CdSe composite quantum dot-based electrochemiluminescence detection of thrombin by a multiple DNA cycle amplification strategy.

    PubMed

    Jie, Guifen; Yuan, Jinxin

    2012-03-20

    A novel small magnetic electrochemiluminescent Fe(3)O(4)@CdSe composite quantum dot (QD) was facilely prepared and successfully applied to sensitive electrochemiluminescence (ECL) detection of thrombin by a multiple DNA cycle amplification strategy for the first time. The as-prepared composite QDs feature intense ECL, excellent magnetism, strong fluorescence, and favorable biocompatibility, which offers promising advantages for ECL biosensing. ECL of the composite QDs was efficiently quenched by gold nanoparticles (NPs). Taking advantages of the unique and attractive ECL and magnetic characteristics of the composite QDs, a novel DNA-amplified detection method based on ECL quenching was thus developed for a sensitive assay of thrombin. More importantly, the DNA devices by cleavage reaction were cycled multiple rounds, which greatly amplified the ECL signal and much improve the detection sensitivity. This flexible biosensing system exhibits not only high sensitivity and specificity but also excellent performance in real human serum assay. The present work opens a promising approach to develop magnetic quantum dot-based amplified ECL bioassays, which has wider potential application with more favorable analytical performances than other ECL reagent-based systems. Moreover, the composite QDs are suitable for long-term fluorescent cellular imaging, which also highlights the promising directions for further development of QD-based in vitro and in vivo imaging materials.

  9. Performance Enhancement of 3-Mercaptopropionic Acid-Capped CdSe Quantum-Dot Sensitized Solar Cells Incorporating Single-Walled Carbon Nanotubes.

    PubMed

    Yang, Jonghee; Park, Taehee; Lee, Jongtaek; Lee, Junyoung; Shin, Hokyeong; Yi, Whikun

    2016-03-01

    We fabricated a series of linker-assisted quantum-dot-sensitized solar cells based on the ex situ self-assembly of CdSe quantum dots (QDs) onto TiO2 electrode using sulfide/polysulfide (S(2-)/Sn(2-)) as an electrolyte and Au cathode. Our cell were combined with single-walled carbon nanotubes (SWNTs) by two techniques; One was mixing SWNTs with TiO2 electrode and the other was spraying SWNTs onto Au electrode. Absorption spectra were used to confirm the adsorption of QDs onto TiO2 electrode. Cell performance was measured on samples containing and not-containing SWNTs. Samples mixing SWNTs with TiO2 showed higher cell efficiency, on the while sample spraying SWNTs onto Au electrode showed lower efficiency compared with pristine sample (not-containing SWNTs). Electrochemical impedance spectroscopy analysis suggested that SWNTs can act as either barriers or excellent carrier transfers according their position and mixing method.

  10. Study of optically trapped living Trypanosoma cruzi/Trypanosoma rangeli - Rhodnius prolixus interactions by real time confocal images using CdSe quantum dots

    NASA Astrophysics Data System (ADS)

    de Thomaz, A. A.; Almeida, D. B.; Faustino, W. M.; Jacob, G. J.; Fontes, A.; Barbosa, L. C.; Cesar, C. L.; Stahl, C. V.; Santos-Mallet, J. R.; Gomes, S. A. O.; Feder, D.

    2008-08-01

    One of the fundamental goals in biology is to understand the interplay between biomolecules of different cells. This happen, for example, in the first moments of the infection of a vector by a parasite that results in the adherence to the cell walls. To observe this kind of event we used an integrated Optical Tweezers and Confocal Microscopy tool. This tool allow us to use the Optical Tweezers to trigger the adhesion of the Trypanosoma cruzi and Trypanosoma rangeli parasite to the intestine wall cells and salivary gland of the Rhodnius prolixus vector and to, subsequently observe the sequence of events by confocal fluorescence microscopy under optical forces stresses. We kept the microorganism and vector cells alive using CdSe quantum dot staining. Besides the fact that Quantum Dots are bright vital fluorescent markers, the absence of photobleaching allow us to follow the events in time for an extended period. By zooming to the region of interested we have been able to acquire confocal images at the 2 to 3 frames per second rate.

  11. Use of Surface Photovoltage Spectroscopy to Measure Built-in Voltage, Space Charge Layer Width, and Effective Band Gap in CdSe Quantum Dot Films.

    PubMed

    Zhao, Jing; Nail, Benjamin A; Holmes, Michael A; Osterloh, Frank E

    2016-09-01

    Surface photovoltage spectroscopy (SPS) was used to study the photochemistry of mercaptoethanol-ligated CdSe quantum dot (2.0-4.2 nm diameter) films on indium doped tin oxide (ITO) in the absence of an external bias or electrolyte. The n-type films generate negative voltages under super band gap illumination (0.1-0.5 mW cm(-2)) by majority carrier injection into the ITO substrate. The photovoltage onset energies track the optical band gaps of the samples and are assigned as effective band gaps of the films. The photovoltage values (-125 to -750 mV) vary with quantum dot sizes and are modulated by the built-in potential of the CdSe-ITO Schottky type contacts. Deviations from the ideal Schottky model are attributed to Fermi level pinning in states approximately 1.1 V negative of the ITO conduction band edge. Positive photovoltage signals of +80 to +125 mV in films of >4.0 nm nanocrystals and in thin (70 nm) nanocrystal films are attributed to electron-hole (polaron) pairs that are polarized by a space charge layer at the CdSe-ITO boundary. The space charge layer is 70-150 nm wide, based on thickness-dependent photovoltage measurements. The ability of SPS to directly measure built-in voltages, space charge layer thickness, sub-band gap states, and effective band gaps in drop-cast quantum dot films aids the understanding of photochemical charge transport in quantum dot solar cells. PMID:27505130

  12. Use of Surface Photovoltage Spectroscopy to Measure Built-in Voltage, Space Charge Layer Width, and Effective Band Gap in CdSe Quantum Dot Films.

    PubMed

    Zhao, Jing; Nail, Benjamin A; Holmes, Michael A; Osterloh, Frank E

    2016-09-01

    Surface photovoltage spectroscopy (SPS) was used to study the photochemistry of mercaptoethanol-ligated CdSe quantum dot (2.0-4.2 nm diameter) films on indium doped tin oxide (ITO) in the absence of an external bias or electrolyte. The n-type films generate negative voltages under super band gap illumination (0.1-0.5 mW cm(-2)) by majority carrier injection into the ITO substrate. The photovoltage onset energies track the optical band gaps of the samples and are assigned as effective band gaps of the films. The photovoltage values (-125 to -750 mV) vary with quantum dot sizes and are modulated by the built-in potential of the CdSe-ITO Schottky type contacts. Deviations from the ideal Schottky model are attributed to Fermi level pinning in states approximately 1.1 V negative of the ITO conduction band edge. Positive photovoltage signals of +80 to +125 mV in films of >4.0 nm nanocrystals and in thin (70 nm) nanocrystal films are attributed to electron-hole (polaron) pairs that are polarized by a space charge layer at the CdSe-ITO boundary. The space charge layer is 70-150 nm wide, based on thickness-dependent photovoltage measurements. The ability of SPS to directly measure built-in voltages, space charge layer thickness, sub-band gap states, and effective band gaps in drop-cast quantum dot films aids the understanding of photochemical charge transport in quantum dot solar cells.

  13. Determination of the rod-wire transition length in colloidal indium phosphide quantum rods.

    PubMed

    Wang, Fudong; Buhro, William E

    2007-11-21

    Colloidal InP quantum rods (QRs) having controlled diameters and lengths are grown by the solution-liquid-solid method, from Bi nanoparticles in the presence of hexadecylamine and other conventional quantum dot surfactants. These quantum rods show band-edge photoluminescence after HF photochemical etching. Photoluminescence efficiency is further enhanced after the Bi tips are selectively removed from the QRs by oleic acid etching. The QRs are anisotropically 3D confined, the nature of which is compared to the corresponding isotropic 3D confinement in quantum dots and 2D confinement in quantum wires. The 3D-2D rod-wire transition length is experimentally determined to be 25 nm, which is about 2 times the bulk InP exciton Bohr radius (of approximately 11 nm).

  14. Photoluminescence quantum yield of PbS nanocrystals in colloidal suspensions

    SciTech Connect

    Greben, M.; Fucikova, A.; Valenta, J.

    2015-04-14

    The absolute photoluminescence (PL) quantum yield (QY) of oleic acid-capped colloidal PbS quantum dots (QDs) in toluene is thoroughly investigated as function of QD size, concentration, excitation photon energy, and conditions of storage. We observed anomalous decrease of QY with decreasing concentration for highly diluted suspensions. The ligand desorption and QD-oxidation are demonstrated to be responsible for this phenomenon. Excess of oleic acid in suspensions makes the QY values concentration-independent over the entire reabsorption-free range. The PL emission is shown to be dominated by surface-related recombinations with some contribution from QD-core transitions. We demonstrate that QD colloidal suspension stability improves with increasing the concentration and size of PbS QDs.

  15. Detection of viral infections using colloidal quantum dots

    NASA Astrophysics Data System (ADS)

    Bentzen, Elizabeth L.; House, Frances S.; Utley, Thomas J.; Crowe, James E., Jr.; Wright, David W.

    2006-02-01

    Fluorescence is a tool widely employed in biological assays. Fluorescent semiconducting nanocrystals, quantum dots (QDs), are beginning to find their way into the tool box of many biologist, chemist and biochemist. These quantum dots are an attractive alternative to the traditional organic dyes due to their broad excitation spectra, narrow emission spectra and photostability. Quantum dots were used to detect and monitor the progession of viral glycoproteins, F (fusion) and G (attachment), from Respiratory Syncytial Virus (RSV) in HEp-2 cells. Additionally, oligo-Qdot RNA probes have been developed for identification and detection of mRNA of the N(nucleocapsid) protein for RSV. The use of quantum dot-FISH probes provides another confirmatory route to diagnostics as well as a new class of probes for monitoring the flux and fate of viral RNA RSV is the most common cause of lower respiratory tract infection in children worldwide and the most common cause of hospitalization of infants in the US. Antiviral therapy is available for treatment of RSV but is only effective if given within the first 48 hours of infection. Existing test methods require a virus level of at least 1000-fold of the amount needed for infection of most children and require several days to weeks to obtain results. The use of quantum dots may provide an early, rapid method for detection and provide insight into the trafficking of viral proteins during the course of infection.

  16. Double-Sided Junctions Enable High-Performance Colloidal-Quantum-Dot Photovoltaics.

    PubMed

    Liu, Mengxia; de Arquer, F Pelayo García; Li, Yiying; Lan, Xinzheng; Kim, Gi-Hwan; Voznyy, Oleksandr; Jagadamma, Lethy Krishnan; Abbas, Abdullah Saud; Hoogland, Sjoerd; Lu, Zhenghong; Kim, Jin Young; Amassian, Aram; Sargent, Edward H

    2016-06-01

    The latest advances in colloidal-quantum-dot material processing are combined with a double-sided junction architecture, which is done by efficiently incorporating indium ions in the ZnO eletrode. This platform allows the collection of all photogenerated carriers even at the maximum power point. The increased depletion width in the device facilitates full carrier collection, leading to a record 10.8% power conversion efficiency.

  17. Water-dispersable colloidal quantum dots for the detection of ionizing radiation.

    PubMed

    Lecavalier, Marie-Eve; Goulet, Mathieu; Allen, Claudine Nì; Beaulieu, Luc; Larivière, Dominic

    2013-12-25

    Fluorescent CdSe-CdS-Cd0.5Zn0.5S-ZnS core-shell colloidal quantum dots (cQDs) dispersed in aqueous and organic solvents have been prepared and used as scintillators for detecting ionizing radiation. Results demonstrate a linear relationship between emitted luminescence and dose-activity. These results suggest that cQDs alone could be used as liquid scintillators for specific environmental and medical applications.

  18. Colloidal Quantum Dot Photovoltaics Enhanced by Perovskite Shelling.

    PubMed

    Yang, Zhenyu; Janmohamed, Alyf; Lan, Xinzheng; García de Arquer, F Pelayo; Voznyy, Oleksandr; Yassitepe, Emre; Kim, Gi-Hwan; Ning, Zhijun; Gong, Xiwen; Comin, Riccardo; Sargent, Edward H

    2015-11-11

    Solution-processed quantum dots are a promising material for large-scale, low-cost solar cell applications. New device architectures and improved passivation have been instrumental in increasing the performance of quantum dot photovoltaic devices. Here we report photovoltaic devices based on inks of quantum dot on which we grow thin perovskite shells in solid-state films. Passivation using the perovskite was achieved using a facile solution ligand exchange followed by postannealing. The resulting hybrid nanostructure created a more intrinsic CQD film, which, when incorporated into a photovoltaic device with graded bandstructure, achieved a record solar cell performance for single-step-deposited CQD films, exhibiting an AM1.5 solar power conversion efficiency of 8.95%.

  19. Optimization schemes for efficient multiple exciton generation and extraction in colloidal quantum dots

    NASA Astrophysics Data System (ADS)

    Damtie, Fikeraddis A.; Karki, Khadga J.; Pullerits, Tõnu; Wacker, Andreas

    2016-08-01

    Multiple exciton generation (MEG) is a process in which more than one electron hole pair is generated per absorbed photon. It allows us to increase the efficiency of solar energy harvesting. Experimental studies have shown the multiple exciton generation yield of 1.2 in isolated colloidal quantum dots. However real photoelectric devices require the extraction of electron hole pairs to electric contacts. We provide a systematic study of the corresponding quantum coherent processes including extraction and injection and show that a proper design of extraction and injection rates enhances the yield significantly up to values around 1.6.

  20. A Highly Efficient Hybrid GaAs Solar Cell Based on Colloidal-Quantum-Dot-Sensitization

    PubMed Central

    Han, Hau-Vei; Lin, Chien-Chung; Tsai, Yu-Lin; Chen, Hsin-Chu; Chen, Kuo-Ju; Yeh, Yun-Ling; Lin, Wen-Yi; Kuo, Hao-Chung; Yu, Peichen

    2014-01-01

    This paper presents a hybrid design, featuring a traditional GaAs-based solar cell combined with various colloidal quantum dots. This hybrid design effectively boosts photon harvesting at long wavelengths while enhancing the collection of photogenerated carriers in the ultraviolet region. The merits of using highly efficient semiconductor solar cells and colloidal quantum dots were seamlessly combined to increase overall power conversion efficiency. Several photovoltaic parameters, including short-circuit current density, open circuit voltage, and external quantum efficiency, were measured and analyzed to investigate the performance of this hybrid device. Offering antireflective features at long wavelengths and luminescent downshifting for high-energy photons, the quantum dots effectively enhanced overall power conversion efficiency by as high as 24.65% compared with traditional GaAs-based devices. The evolution of weighted reflectance as a function of the dilution factor of QDs was investigated. Further analysis of the quantum efficiency response showed that the luminescent downshifting effect can be as much as 6.6% of the entire enhancement of photogenerated current. PMID:25034623

  1. Near-field light design with colloidal quantum dots for photonics and plasmonics.

    PubMed

    Kress, Stephan J P; Richner, Patrizia; Jayanti, Sriharsha V; Galliker, Patrick; Kim, David K; Poulikakos, Dimos; Norris, David J

    2014-10-01

    Colloidal quantum-dots are bright, tunable emitters that are ideal for studying near-field quantum-optical interactions. However, their colloidal nature has hindered their facile and precise placement at desired near-field positions, particularly on the structured substrates prevalent in plasmonics. Here, we use high-resolution electro-hydrodynamic printing (<100 nm feature size) to deposit countable numbers of quantum dots on both flat and structured substrates with a few nanometer precision. We also demonstrate that the autofocusing capability of the printing method enables placement of quantum dots preferentially at plasmonic hot spots. We exploit this control and design diffraction-limited photonic and plasmonic sources with arbitrary wavelength, shape, and intensity. We show that simple far-field illumination can excite these near-field sources and generate fundamental plasmonic wave-patterns (plane and spherical waves). The ability to tailor subdiffraction sources of plasmons with quantum dots provides a complementary technique to traditional scattering approaches, offering new capabilities for nanophotonics.

  2. Efficient, stable infrared photovoltaics based on solution-cast colloidal quantum dots.

    PubMed

    Koleilat, Ghada I; Levina, Larissa; Shukla, Harnik; Myrskog, Stefan H; Hinds, Sean; Pattantyus-Abraham, Andras G; Sargent, Edward H

    2008-05-01

    Half of the sun's power lies in the infrared. As a result, the optimal bandgaps for solar cells in both the single-junction and even the tandem architectures lie beyond 850 nm. However, progress in low-cost, large-area, physically flexible solar cells has instead been made in organic and polymer materials possessing absorption onsets in the visible. Recent advances have been achieved in solution-cast infrared photovoltaics through the use of colloidal quantum dots. Here we report stable solution-processed photovoltaic devices having 3.6% power conversion efficiency in the infrared. The use of a strongly bound bidentate linker, benzenedithiol, ensures device stability over weeks. The devices reach external quantum efficiencies of 46% in the infrared and 70% across the visible. We investigate in detail the physical mechanisms underlying the operation of this class of device. In contrast with drift-dominated behavior in recent reports of PbS quantum dot photovoltaics, we find that diffusion of electrons and holes over hundreds of nanometers through our PbSe colloidal quantum dot solid is chiefly responsible for the high external quantum efficiencies obtained in this new class of devices. PMID:19206479

  3. Integrating an electrically active colloidal quantum dot photodiode with a graphene phototransistor

    PubMed Central

    Nikitskiy, Ivan; Goossens, Stijn; Kufer, Dominik; Lasanta, Tania; Navickaite, Gabriele; Koppens, Frank H. L.; Konstantatos, Gerasimos

    2016-01-01

    The realization of low-cost photodetectors with high sensitivity, high quantum efficiency, high gain and fast photoresponse in the visible and short-wave infrared remains one of the challenges in optoelectronics. Two classes of photodetectors that have been developed are photodiodes and phototransistors, each of them with specific drawbacks. Here we merge both types into a hybrid photodetector device by integrating a colloidal quantum dot photodiode atop a graphene phototransistor. Our hybrid detector overcomes the limitations of a phototransistor in terms of speed, quantum efficiency and linear dynamic range. We report quantum efficiencies in excess of 70%, gain of 105 and linear dynamic range of 110 dB and 3 dB bandwidth of 1.5 kHz. This constitutes a demonstration of an optoelectronically active device integrated directly atop graphene and paves the way towards a generation of flexible highly performing hybrid two-dimensional (2D)/0D optoelectronics. PMID:27311710

  4. Size-dependent absolute quantum yields for size-separated colloidally-stable silicon nanocrystals.

    PubMed

    Mastronardi, Melanie L; Maier-Flaig, Florian; Faulkner, Daniel; Henderson, Eric J; Kübel, Christian; Lemmer, Uli; Ozin, Geoffrey A

    2012-01-11

    Size-selective precipitation was used to successfully separate colloidally stable allylbenzene-capped silicon nanocrystals into several visible emitting monodisperse fractions traversing the quantum size effect range of 1-5 nm. This enabled the measurement of the absolute quantum yield and lifetime of photoluminescence of allylbenzene-capped silicon nanocrystals as a function of size. The absolute quantum yield and lifetime are found to monotonically decrease with decreasing nanocrystal size, which implies that nonradiative vibrational and surface defect effects overwhelm spatial confinement effects that favor radiative relaxation. Visible emission absolute quantum yields as high as 43% speak well for the development of "green" silicon nanocrystal color-tunable light emitting diodes that can potentially match the performance of their toxic heavy metal chalcogenide counterparts.

  5. Integrating an electrically active colloidal quantum dot photodiode with a graphene phototransistor

    NASA Astrophysics Data System (ADS)

    Nikitskiy, Ivan; Goossens, Stijn; Kufer, Dominik; Lasanta, Tania; Navickaite, Gabriele; Koppens, Frank H. L.; Konstantatos, Gerasimos

    2016-06-01

    The realization of low-cost photodetectors with high sensitivity, high quantum efficiency, high gain and fast photoresponse in the visible and short-wave infrared remains one of the challenges in optoelectronics. Two classes of photodetectors that have been developed are photodiodes and phototransistors, each of them with specific drawbacks. Here we merge both types into a hybrid photodetector device by integrating a colloidal quantum dot photodiode atop a graphene phototransistor. Our hybrid detector overcomes the limitations of a phototransistor in terms of speed, quantum efficiency and linear dynamic range. We report quantum efficiencies in excess of 70%, gain of 105 and linear dynamic range of 110 dB and 3 dB bandwidth of 1.5 kHz. This constitutes a demonstration of an optoelectronically active device integrated directly atop graphene and paves the way towards a generation of flexible highly performing hybrid two-dimensional (2D)/0D optoelectronics.

  6. Size and Temperature Dependence of Electron Transfer between CdSe Quantum Dots and a TiO 2 Nanobelt

    SciTech Connect

    Tafen, De Nyago; Prezhdo, Oleg V.

    2015-02-24

    Understanding charge transfer reactions between quantum dots (QD) and metal oxides is fundamental for improving photocatalytic, photovoltaic and electronic devices. The complexity of these processes makes it difficult to find an optimum QD size with rapid charge injection and low recombination. We combine time-domain density functional theory with nonadiabatic molecular dynamics to investigate the size and temperature dependence of the experimentally studied electron transfer and charge recombination at CdSe QD-TiO2 nanobelt (NB) interfaces. The electron injection rate shows strong dependence on the QD size, increasing for small QDs. The rate exhibits Arrhenius temperature dependence, with the activation energy of the order of millielectronvolts. The charge recombination process occurs due to coupling of the electronic subsystem to vibrational modes of the TiO2 NB. Inelastic electron-phonon scattering happens on a picosecond time scale, with strong dependence on the QD size. Our simulations demonstrate that the electron-hole recombination rate decreases significantly as the QD size increases, in excellent agreement with experiments. The temperature dependence of the charge recombination rates can be successfully modeled within the framework of the Marcus theory through optimization of the electronic coupling and the reorganization energy. Our simulations indicate that by varying the QD size, one can modulate the photoinduced charge separation and charge recombination, fundamental aspects of the design principles for high efficiency devices.

  7. Comparison of magneto-optical properties of various excitonic complexes in CdTe and CdSe self-assembled quantum dots

    NASA Astrophysics Data System (ADS)

    Kobak, J.; Smoleński, T.; Goryca, M.; Rousset, J.-G.; Pacuski, W.; Bogucki, A.; Oreszczuk, K.; Kossacki, P.; Nawrocki, M.; Golnik, A.; Płachta, J.; Wojnar, P.; Kruse, C.; Hommel, D.; Potemski, M.; Kazimierczuk, T.

    2016-07-01

    We present a comparative study of two self-assembled quantum dot (QD) systems based on II-VI compounds: CdTe/ZnTe and CdSe/ZnSe. Using magneto-optical techniques we investigated a large population of individual QDs. The systematic photoluminescence studies of emission lines related to the recombination of neutral exciton X, biexciton XX, and singly charged excitons (X+, X-) allowed us to determine average parameters describing CdTe QDs (CdSe QDs): X-XX transition energy difference 12 meV (24 meV); fine-structure splitting δ1=0.14 meV (δ1=0.47 meV); g-factor g  =  2.12 (g  =  1.71) diamagnetic shift γ=2.5 μeV T-2 (γ =1.3 μeV T-2). We find also statistically significant correlations between various parameters describing internal structure of excitonic complexes.

  8. Rapid and One-Pot Synthesis of Self-Assembled CdSe Quantum Dots Functionalized with β-Cyclodextrin: Reduced Cytotoxicity and Band Gap Engineering.

    PubMed

    Guleria, Apurav; Rath, Madhab C; Singh, Ajay K; Adhikari, Soumyakanti

    2015-12-01

    We report a simple, rapid and one step method for the synthesis and in situ functionalization of CdSe quantum dots (QDs) with β-cyclodextrin (β-CD) in aqueous solution via electron beam (EB) irradiation technique. A probable mechanism has been elucidated for the formation of the QDs using pulse radiolysis technique. The average size of the QDs was found to be in the range of 2-3 nm with a size distribution of -14%. XPS measurements indicate that the -OH groups of the β-CD molecules binds predominantly with the Cd atoms present on the surface of the QDs. These QDs displayed broad photoluminescence (PL) with two emission peaks at 525 nm and 600 nm, which could be tuned by varying the experimental parameters. The broad PL spectrum has been attributed to the polydispersity in the density and the distribution of trap/defects states. Time resolved PL decay measurements further substantiated the domination of surface state originated carrier relaxation processes in the overall PL decay dynamics of QDs synthesized at higher doses and dose rates. The present study reveals that β-CD passivate the QDs by a non-inclusion complex, induces the self-assembling process into a networking architecture and simultaneously reduces their cytotoxicity as compared to the bare nanoparticles. The methodology described in this article may provide unique and interesting aspects to regulate and fine tune the formation of superstructures of nanomaterials vis-à-vis their optoelectronic properties.

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

    NASA Astrophysics Data System (ADS)

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

    2006-09-01

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

  10. A highly sensitive differential pulse anodic stripping voltammetry for determination of 17β-estradiol (E2) using CdSe quantum dots based on indirect competitive immunoassay.

    PubMed

    Chaisuwan, Nuanapa; Xu, He; Wu, Genying; Liu, Jianshe

    2013-08-15

    In this study a new and fast procedure was developed to determine trace 17β-estradiol (E2) concentrations using CdSe quantum dots (QDs) conjugation with bovine serum albumin (BSA)-E2. To increase the high efficiency of the method, the immunoassay design was restricted to an indirect competitive format. The E2 antigen and bioconjugate were incubated in a microtiter plate with an anti-E2 antibody and competition for antibody binding sites was established. The in situ bismuth-coated carbon electrodes were used for detecting the cadmium ions (Cd(2+)) released during the acid dissolution step. After optimization, the well-defined sharp anodic stripping voltammograms curves of the E2 concentration ranging from 50 to 1000 pg/mL was recorded, and the lowest detection limit was 50 pg/mL with 6% reproducibility and 7% repeatability. Finally, the assay was applied to tap water and wastewater samples. The detection limits were 52.56 ± 0.125 pg/mL for tap water and 51.42 ± 0.453 pg/mL for wastewater. These results show that the assay exhibited sensitive analytical performance in E2 detection with high sensitivity and accuracy with satisfactory results. PMID:23542084

  11. Partitioning of hydrophobic CdSe quantum dots into aqueous dispersions of humic substances: influence of capping-group functionality on the phase-transfer mechanism.

    PubMed

    Navarro, Divina A; Banerjee, Sarbajit; Aga, Diana S; Watson, David F

    2010-08-01

    Studies of the fate and transport of engineered nanomaterials are invaluable in predicting environmental impact, bioavailability, and toxicity. We report on the influence of humic and fulvic acids (models of natural organic matter) on the phase transfer of organic-capped CdSe quantum dots (QDs) from hexane to water. QDs capped with tri-n-octylphosphine oxide, tetradecylphosphonic acid, and oleic acid, which were otherwise insoluble in water, were transferred into aqueous solutions of humic substances (HS) (Suwannee River humic acid and fulvic acid standards) within 1-10 days after mixing. Phase transfer was characterized by infrared and UV/Vis absorption spectroscopy, emission spectroscopy, dynamic light scattering, electron microscopy, and inductively coupled plasma mass spectrometry. Phase-transferred QDs were intact and temporarily stabilized by HS. On longer timescales, Cd(2+) leached into aqueous solution. Our data suggest that two mechanisms promote the phase transfer of QD-HS agglomerates: (1) an overcoating mechanism involving dispersion interactions between non-polar moieties of HS and hydrocarbon chains of organic capping groups and (2) a coordinative mechanism involving displacement of capping groups by Lewis basic functionalities of HS. The structure of the capping group of QDs influenced the relative contributions of the two mechanisms and the extent to which Cd(2+) leached into water.

  12. Bulk transport and interfacial transfer dynamics of photogenerated carriers in CdSe quantum dot solid electrodes.

    PubMed

    Yang, Ye; Liu, Zheng; Lian, Tianquan

    2013-08-14

    Practical solar-to-fuel conversion applications of quantum-confined semiconductor crystals require their integration into electrodes. We show that photogenerated electrons in quantum dot solid electrodes can be transported to the aqueous interface to reduce methyl viologen with 100% quantum efficiency and an effective time constant of 12 ± 2 ps. The charge separated state had a half-life of 200 ± 10 ns, limited by hole transport within the solid.

  13. Seed-mediated synthesis, properties and application of {gamma}-Fe{sub 2}O{sub 3}-CdSe magnetic quantum dots

    SciTech Connect

    Lin, Alex W.H.; Ang, Chung Yen; Patra, Pranab K.; Han Yu; Gu Hongwei; Le Breton, Jean-Marie; Juraszek, Jean; Chiron, Hubert; Papaefthymiou, Georgia C.; Tamil Selvan, Subramanian; Ying, Jackie Y.

    2011-08-15

    Seed-mediated growth of fluorescent CdSe quantum dots (QDs) around {gamma}-Fe{sub 2}O{sub 3} magnetic cores was performed at high temperature (300 deg. C) in the presence of organic surfactants. Bi-functional magnetic quantum dots (MQDs) with tunable emission properties were successfully prepared. The as-synthesized MQDs were characterized by high-resolution transmission electron microscopy (HRTEM) and dynamic light scattering (DLS), which confirmed the assembly of heterodimers. When a longer growth period was employed, a homogeneous dispersion of QDs around a magnetic nanoparticle was obtained. The magnetic properties of these nanocomposites were examined. The MQDs were superparamagnetic with a saturation magnetization of 0.40 emu/g and a coercivity of 138 Oe at 5 K. To demonstrate their potential application in bio-labeling, these MQDs were coated with a thin silica shell, and functionalized with a polyethylene glycol (PEG) derivative. The functionalized MQDs were effectively used for the labeling of live cell membranes of 4T1 mouse breast cancer cells and HepG2 human liver cancer cells. - Graphical abstract: (a) HRTEM image of oleic acid capped MPs. The size of MPs ranges from 8 to 10 nm. (b) XRD pattern of {gamma}-Fe{sub 2}O{sub 3} MPs. Highlights: > The fabrication of MQDs through a seed-mediated approach has been demonstrated. > The formation and assembly of these bi-functional nanocomposites have been elucidated. > The MQDs exhibit superparamagnetism and tunable emissions characteristic of the components. > MQDs with thin silica coating were successfully employed in the labeling of cancer cell membranes.

  14. Electron beam induced and microemulsion templated synthesis of CdSe quantum dots: tunable broadband emission and charge carrier recombination dynamics

    NASA Astrophysics Data System (ADS)

    Guleria, Apurav; Singh, Ajay K.; Rath, Madhab C.; Adhikari, Soumyakanti

    2015-04-01

    CdSe quantum dots (QDs) were synthesized by a rapid and one step templated approach inside the water pool of AOT (sodium bis(2-ethylhexyl) sulfosuccinate) based water-in-oil microemulsions (MEs) via electron beam (EB) irradiation technique with high dose rate, which favours high nucleation rate. The interplay of different experimental parameters such as precursor concentration, absorbed dose and {{W}0} values (aqueous phase to surfactant molar ratio) of MEs were found to have interesting consequences on the morphology, photoluminescence (PL), surface composition and carrier recombination dynamics of as-grown QDs. For instance, highly stable ultrasmall (∼1.7 nm) bluish-white light emitting QDs were obtained with quantum efficiency (η) of ∼9%. Furthermore, QDs were found to exhibit tunable broadband light emission extending from 450 to 750 nm (maximum FWHM ∼180 nm). This could be realized from the CIE (Commission Internationale d’Eclairage) chromaticity co-ordinates, which varied across the blue region to the orange region thereby, conferring their potential application in white light emitting diodes. Additionally, the average PL lifetime ≤ft( ≤ft< τ \\right> \\right) values could be varied from 18 ns to as high as 74 ns, which reflect the role of surface states in terms of their density and distribution. Another interesting revelation was the self-assembling of the initially formed QDs into nanorods with high aspect ratios ranging from 7 to 20, in correspondence with the {{W}0} values. Besides, the fundamental roles of the chemical nature of water pool and the interfacial fluidity of AOT MEs in influencing the photophysical properties of QDs were investigated by carrying out a similar study in CTAB (cetyltrimethylammonium bromide; cationic surfactant) based MEs. Surprisingly, very profound and contrasting results were observed wherein ≤ft< τ \\right> and η of the QDs in case of CTAB MEs were found to be at least three times lower as compared to

  15. Effect of metal oxide morphology on electron injection from CdSe quantum dots to ZnO

    NASA Astrophysics Data System (ADS)

    Zheng, Kaibo; Žídek, Karel; Abdellah, Mohamed; Chábera, Pavel; Abd El-sadek, Mahmoud S.; Pullerits, Tõnu

    2013-04-01

    Performance of quantum dot sensitized solar cells relies on a rapid electron injection from quantum dot to metal oxide. We studied the injection process in CdSe-ZnO system by ultrafast time-resolved absorption spectroscopy for two types of acceptor morphologies—nanowires and nanoparticles' films. Based on comparison between experimental data and Marcus theory, we demonstrate that the acceptor morphology has a significant impact on electron injection due to (i) change in material permittivity and (ii) different density of the band-edge states. The results open a reference to improve injection efficiency in quantum dot-metal oxide system by selection of the acceptor morphology.

  16. Photoluminescence response of colloidal quantum dots on VO2 film across metal to insulator transition

    PubMed Central

    2014-01-01

    We have proposed a method to probe metal to insulator transition in VO2 measuring photoluminescence response of colloidal quantum dots deposited on the VO2 film. In addition to linear luminescence intensity decrease with temperature that is well known for quantum dots, temperature ranges with enhanced photoluminescence changes have been found during phase transition in the oxide. Corresponding temperature derived from luminescence dependence on temperature closely correlates with that from resistance measurement during heating. The supporting reflectance data point out that photoluminescence response mimics a reflectance change in VO2 across metal to insulator transition. Time-resolved photoluminescence study did not reveal any significant change of luminescence lifetime of deposited quantum dots under metal to insulator transition. It is a strong argument in favor of the proposed explanation based on the reflectance data. PACS 71.30. + h; 73.21.La; 78.47.jd PMID:25404877

  17. Picosecond Lifetimes with High Quantum Yields from Single-Photon-Emitting Colloidal Nanostructures at Room Temperature.

    PubMed

    Bidault, Sébastien; Devilez, Alexis; Maillard, Vincent; Lermusiaux, Laurent; Guigner, Jean-Michel; Bonod, Nicolas; Wenger, Jérôme

    2016-04-26

    Minimizing the luminescence lifetime while maintaining a high emission quantum yield is paramount in optimizing the excitation cross-section, radiative decay rate, and brightness of quantum solid-state light sources, particularly at room temperature, where nonradiative processes can dominate. We demonstrate here that DNA-templated 60 and 80 nm diameter gold nanoparticle dimers, featuring one fluorescent molecule, provide single-photon emission with lifetimes that can fall below 10 ps and typical quantum yields in a 45-70% range. Since these colloidal nanostructures are obtained as a purified aqueous suspension, fluorescence spectroscopy can be performed on both fixed and freely diffusing nanostructures to quantitatively estimate the distributions of decay rate and fluorescence intensity enhancements. These data are in excellent agreement with theoretical calculations and demonstrate that millions of bright fluorescent nanostructures, with radiative lifetimes below 100 ps, can be produced in parallel. PMID:26972678

  18. Photoinduced band filling in strongly confined colloidal PbS quantum dots

    SciTech Connect

    Ullrich, B.; Xi, H.; Wang, J. S.

    2014-06-21

    Increase in continuous wave laser excitation (6 W/cm{sup 2} to 120 W/cm{sup 2}) of colloidal PbS quantum dots in the strongly quantized regime (diameters 2.0 nm and 4.7 nm) deposited on semi-insulating GaAs and glass causes a clear blue shift (0.019 eV and 0.080 eV) of the emission spectra. Proof of the applicability of a dynamic three-dimensional band filling model is the significance of the presented results and demonstrates the effective electronic coupling in quantum dot arrays similar to superlattices. The work also reveals the influence of quantum dot sizes on photo-doping effects.

  19. TCNQ Interlayers for Colloidal Quantum Dot Light-Emitting Diodes.

    PubMed

    Koh, Weon-kyu; Shin, Taeho; Jung, Changhoon; Cho, Dr-Kyung-Sang

    2016-04-18

    CdSe/CdS/ZnS quantum dot light-emitting diodes (QD-LEDs) show increased brightness (from ca. 18 000 to 27 000 cd m(-2) ) with 7,7,8,8-tetracyanoquinodimethane (TCNQ) between the QD and electron-transfer layers of ZnO nanoparticles. As QD/ZnO layers are known to have interface defects, our finding leads to the importance of interface engineering for QD-LEDs. Although the photoluminescent intensity and decay lifetime of ZnO/TCNQ/QD layers are similar to those of ZnO/QD layers, cyclic voltammetry suggests improved charge transfer of TCNQ/ZnO layers compared to that of pure ZnO layers. This helps us to understand the mechanism of electrically driven QD-LED behavior, which differs from that of conventional solid-state LEDs, and enables the rational design of QD-based optoelectronic devices.

  20. A study of specific features of the electronic spectrum of quantum dots in CdSe semiconductor

    NASA Astrophysics Data System (ADS)

    Mikhailov, A. I.; Kabanov, V. F.; Gorbachev, I. A.; Glukhovskoi, E. G.

    2016-08-01

    Monolayers of CdSe/CdS/ZnS quantum dots (QDs) formed on the aqueous subphase and transferred to solid substrates by the Langmuir-Blodgett method have been studied. The samples obtained were examined by transmission electron microscopy, atomic-force microscopy, and scanning tunnel microscopy. The structure of the QD monolayer obtained on the substrate was analyzed. Specific features of the electronic spectrum of the quantum objects formed in the samples under study were determined.

  1. Bias-induced photoluminescence quenching of single colloidal quantum dots embedded in organic semiconductors.

    PubMed

    Huang, Hao; Dorn, August; Nair, Gautham P; Bulović, Vladimir; Bawendi, Moungi G

    2007-12-01

    We demonstrate reversible quenching of the photoluminescence from single CdSe/ZnS colloidal quantum dots embedded in thin films of the molecular organic semiconductor N,N'-diphenyl-N,N'-bis(3-methylphenyl)-(1,1'-biphenyl)-4,4'-diamine (TPD) in a layered device structure. Our analysis, based on current and charge carrier density, points toward field ionization as the dominant photoluminescence quenching mechanism. Blinking traces from individual quantum dots reveal that the photoluminescence amplitude decreases continuously as a function of increasing forward bias even at the single quantum dot level. In addition, we show that quantum dot photoluminescence is quenched by aluminum tris(8-hydroxyquinoline) (Alq3) in chloroform solutions as well as in thin solid films of Alq3 whereas TPD has little effect. This highlights the importance of chemical compatibility between semiconductor nanocrystals and surrounding organic semiconductors. Our study helps elucidate elementary interactions between quantum dots and organic semiconductors, knowledge needed for designing efficient quantum dot organic optoelectronic devices. PMID:18034504

  2. Bias-induced photoluminescence quenching of single colloidal quantum dots embedded in organic semiconductors.

    PubMed

    Huang, Hao; Dorn, August; Nair, Gautham P; Bulović, Vladimir; Bawendi, Moungi G

    2007-12-01

    We demonstrate reversible quenching of the photoluminescence from single CdSe/ZnS colloidal quantum dots embedded in thin films of the molecular organic semiconductor N,N'-diphenyl-N,N'-bis(3-methylphenyl)-(1,1'-biphenyl)-4,4'-diamine (TPD) in a layered device structure. Our analysis, based on current and charge carrier density, points toward field ionization as the dominant photoluminescence quenching mechanism. Blinking traces from individual quantum dots reveal that the photoluminescence amplitude decreases continuously as a function of increasing forward bias even at the single quantum dot level. In addition, we show that quantum dot photoluminescence is quenched by aluminum tris(8-hydroxyquinoline) (Alq3) in chloroform solutions as well as in thin solid films of Alq3 whereas TPD has little effect. This highlights the importance of chemical compatibility between semiconductor nanocrystals and surrounding organic semiconductors. Our study helps elucidate elementary interactions between quantum dots and organic semiconductors, knowledge needed for designing efficient quantum dot organic optoelectronic devices.

  3. A Surface Chemistry Approach to Enhancing Colloidal Quantum Dot Solids for Photovoltaics

    NASA Astrophysics Data System (ADS)

    Carey, Graham Hamilton

    Colloidal quantum dot (CQD) photovoltaic devices have improved rapidly over the past decade of research. By taking advantage of the quantum confinement effect, solar cells constructed using films of infrared-bandgap nanoparticles are able to capture previously untapped ranges of the solar energy spectrum. Additionally, films are fabricated using simple, cheap, reproducible solution processing techniques, enabling the creation of low-cost, flexible photovoltaic devices. A key factor limiting the creation of high efficiency CQD solar cells is the short charge carrier diffusion length in films. Driven by a combination of limited carrier mobility, poor nanoparticle surface passivation, and the presence of unexamined electrically active impurities throughout the film, the poor diffusion length limits the active layer thickness in CQD solar cells, leading to lower-than-desired light absorption, and curtailing the photocurrent generated by such devices. This thesis seeks to address poor diffusion length by addressing each of the limiting factors in turn. Electrical transport in quantum dot solids is examined in the context of improved quantum dot packing; methods are developed to improve packing by using actively densifying components, or by dramatically lowering the volume change required between quantum dots in solution and in solid state. Quantum dot surface passivation is improved by introducing a crucial secondary, small halide ligand source, and by surveying the impact of the processing environment on the final quality of the quantum dot surface. A heretofore unidentified impurity present in quantum dot solids is identified, characterized, and chemically eliminated. Finally, lessons learned through these experiments are combined into a single, novel materials system, leading to quantum dot devices with a significantly improved diffusion length (enhanced from 70 to 230 nm). This enabled thick, high current density (30 mA cm -2, compared to typical values in the 20

  4. Secondary treatment of films of colloidal quantum dots for optoelectronics and devices produced thereby

    DOEpatents

    Semonin, Octavi Escala; Luther, Joseph M; Beard, Matthew C; Chen, Hsiang-Yu

    2014-04-01

    A method of forming an optoelectronic device. The method includes providing a deposition surface and contacting the deposition surface with a ligand exchange chemical and contacting the deposition surface with a quantum dot (QD) colloid. This initial process is repeated over one or more cycles to form an initial QD film on the deposition surface. The method further includes subsequently contacting the QD film with a secondary treatment chemical and optionally contacting the surface with additional QDs to form an enhanced QD layer exhibiting multiple exciton generation (MEG) upon absorption of high energy photons by the QD active layer. Devices having an enhanced QD active layer as described above are also disclosed.

  5. White/blue-emitting, water-dispersible CdSe quantum dots prepared by counter ion-induced polymer collapse

    NASA Astrophysics Data System (ADS)

    Wang, Jing; Goh, Jane Betty; Goh, M. Cynthia; Giri, Neeraj Kumar; Paige, Matthew F.

    2015-09-01

    The synthesis and characterization of water-dispersible, luminescent CdSe/ZnS semiconductor quantum dots that exhibit nominal "white" fluorescence emission and have potential applications in solid-state lighting is described. The nanomaterials, prepared through counter ion-induced collapse and UV cross-linking of high-molecular weight polyacrylic acid in the presence of appropriate aqueous inorganic ions, were of ∼2-3 nm diameter and could be prepared in gram quantities. The quantum dots exhibited strong luminescence emission in two bands, the first in the blue-region (band edge) of the optical spectrum and the second, a broad emission in the red-region (attributed to deep trap states) of the optical spectrum. Because of the relative strength of emission of the band edge and deep trap state luminescence, it was possible to achieve visible white luminescence from the quantum dots in aqueous solution and in dried, solid films. The optical spectroscopic properties of the nanomaterials, including ensemble and single-molecule spectroscopy, was performed, with results compared to other white-emitting quantum dot systems described previously in the literature.

  6. Towards bulk based preconditioning for quantum dotcomputations

    SciTech Connect

    Dongarra, Jack; Langou, Julien; Tomov, Stanimire; Channing,Andrew; Marques, Osni; Vomel, Christof; Wang, Lin-Wang

    2006-05-25

    This article describes how to accelerate the convergence of Preconditioned Conjugate Gradient (PCG) type eigensolvers for the computation of several states around the band gap of colloidal quantum dots. Our new approach uses the Hamiltonian from the bulk materials constituent for the quantum dot to design an efficient preconditioner for the folded spectrum PCG method. The technique described shows promising results when applied to CdSe quantum dot model problems. We show a decrease in the number of iteration steps by at least a factor of 4 compared to the previously used diagonal preconditioner.

  7. Directional charge transfer mediated by mid-gap states: A transient absorption spectroscopy study of CdSe quantum dot/β-Pb0.33V2O5 heterostructures

    DOE PAGES

    Milleville, Christopher C.; Pelcher, Kate E.; Sfeir, Matthew Y.; Banerjee, Sarbajit; Watson, David F.

    2016-02-15

    For solar energy conversion, not only must a semiconductor absorb incident solar radiation efficiently but also its photoexcited electron—hole pairs must further be separated and transported across interfaces. Charge transfer across interfaces requires consideration of both thermodynamic driving forces as well as the competing kinetics of multiple possible transfer, cooling, and recombination pathways. In this work, we demonstrate a novel strategy for extracting holes from photoexcited CdSe quantum dots (QDs) based on interfacing with β-Pb0.33V2O5 nanowires that have strategically positioned midgap states derived from the intercalating Pb2+ ions. Unlike midgap states derived from defects or dopants, the states utilized heremore » are derived from the intrinsic crystal structure and are thus homogeneously distributed across the material. CdSe/β-Pb0.33V2O5 heterostructures were assembled using two distinct methods: successive ionic layer adsorption and reaction (SILAR) and linker-assisted assembly (LAA). Transient absorption spectroscopy measurements indicate that, for both types of heterostructures, photoexcitation of CdSe QDs was followed by the transfer of electrons to the conduction band of β-Pb0.33V2O5 nanowires and holes to the midgap states of β-Pb0.33V2O5 nanowires. Holes were transferred on time scales less than 1 ps, whereas electrons were transferred more slowly on time scales of ~2 ps. In contrast, for analogous heterostructures consisting of CdSe QDs interfaced with V2O5 nanowires (wherein midgap states are absent), only electron transfer was observed. Interestingly, electron transfer was readily achieved for CdSe QDs interfaced with V2O5 nanowires by the SILAR method; however, for interfaces incorporating molecular linkers, electron transfer was observed only upon excitation at energies substantially greater than the bandgap absorption threshold of CdSe. Furthermore, transient absorbance decay traces reveal longer excited-state lifetimes (1–3

  8. Carrier dynamics in highly quantum-confined, colloidal indium antimonide nanocrystals.

    PubMed

    Chang, Angela Y; Liu, Wenyong; Talapin, Dmitri V; Schaller, Richard D

    2014-08-26

    Nanometer-sized particles of indium antimonide (InSb) offer opportunities in areas such as solar energy conversion and single photon sources. Here, we measure electron-hole pair dynamics, spectra, and absorption cross sections of strongly quantum-confined colloidal InSb nanocrystal quantum dots using femtosecond transient absorption. For all samples, we observe a bleach feature that develops on ultrafast time scales, which notably moves to lower energy during the first several picoseconds following excitation. We associate this unusual red shift, which becomes larger for larger particles and more distinct at lower sample temperatures, with hot exciton cooling through states that we suggest arise from energetically proximal conduction band levels. From controlled optical excitation intensities, we determine biexciton lifetimes, which range from 2 to 20 ps for the studied 3-6 nm diameter particle sizes. PMID:25106893

  9. Model of fluorescence intermittency of single colloidal semiconductor quantum dots using multiple recombination centers.

    PubMed

    Frantsuzov, Pavel A; Volkán-Kacsó, Sándor; Jankó, Bolizsár

    2009-11-13

    We present a new physical model resolving a long-standing mystery of the power-law distributions of the blinking times in single colloidal quantum dot fluorescence. The model considers the nonradiative relaxation of the exciton through multiple recombination centers. Each center is allowed to switch between two quasistationary states. We point out that the conventional threshold analysis method used to extract the exponents of the distributions for the on times and off times has a serious flaw: the qualitative properties of the distributions strongly depend on the threshold value chosen for separating the on and off states. Our new model explains naturally this threshold dependence, as well as other key experimental features of the single quantum dot fluorescence trajectories, such as the power-law power spectrum (1/f noise).

  10. Organic/inorganic hybrid pn-junction between copper phthalocyanine and CdSe quantum dot layers as solar cells

    NASA Astrophysics Data System (ADS)

    Saha, Sudip K.; Guchhait, Asim; Pal, Amlan J.

    2012-08-01

    We have introduced an organic/inorganic hybrid pn-junction for solar cell applications. Layers of II-VI quantum dots and a metal-phthalocyanine in sequence have been used as n- and p-type materials, respectively, to form a junction. The film of quantum dots has been formed through a layer-by-layer process by replacing the long-chain ligands of the nanoparticles in each ultrathin layer or a monolayer with short-chain ones so that interparticle distance becomes small leading to a decrease in resistance of the quantum dot layer. With indium tin oxide and Au as electrodes, we have formed an inverted sandwiched structure. These electrodes formed ohmic contacts with the neighboring materials. From the current-voltage characteristics of the hybrid heterostructure, we have inferred formation of a depletion region at the pn-junction that played a key role in charge separation and correspondingly a photocurrent in the external circuit. For comparison, we have also formed and characterized Schottky devices based on components of the pn-junction keeping the electrode combination same. From capacitance-voltage characteristics, we have observed that the depletion region of the hybrid pn-junction was much wider as compared to that in Schottky devices based on components of the junction.

  11. Colloidal quantum-dot-based silica gel glass: two-photon absorption, emission, and quenching mechanism.

    PubMed

    Li, Jingzhou; Dong, Hongxing; Zhang, Saifeng; Ma, Yunfei; Wang, Jun; Zhang, Long

    2016-09-28

    Two-photon (TP) three-dimensional solid matrices have potential applications in high density optical data reading and storage, infrared-pumped visible displays, lasers, etc. Such technologies will benefit greatly from the advantageous properties of TP materials including tunable emission wavelength, photostability, and simple chemical processing. Here, this ideal TP solid is made possible by using a facile sol-gel process to engineer colloid quantum dots into silica gel glass. Characterization using an open-aperture Z-scan technique shows that the solid matrices exhibited significant TP optical properties with a TP absorption coefficient of (9.41 ± 0.39) × 10(-2) cm GW(-1) and a third-order nonlinear figure of merit of (7.30 ± 0.30) × 10(-14) esu cm. In addition, the dependence of the TP properties on high-temperature thermal treatment is studied in detail to obtain a clear insight for practical applications. The results illustrate that the sample can maintain stable TP performance below the synthesis temperature of the CdTe/CdS colloidal quantum dots. Furthermore, the mechanisms for thermal quenching of photoluminescence under different temperature regimes are clarified as a function of the composition.

  12. Colloidal quantum dot lasers built on a passive two-dimensional photonic crystal backbone

    NASA Astrophysics Data System (ADS)

    Chang, Hojun; Min, Kyungtaek; Lee, Myungjae; Kang, Minsu; Park, Yeonsang; Cho, Kyung-Sang; Roh, Young-Geun; Woo Hwang, Sung; Jeon, Heonsu

    2016-03-01

    We report the room-temperature lasing action from two-dimensional photonic crystal (PC) structures composed of a passive Si3N4 backbone with an over-coat of CdSe/CdS/ZnS colloidal quantum dots (CQDs) for optical gain. When optically excited, devices lased in dual PC band-edge modes, with the modal dominance governed by the thickness of the CQD over-layer. The demonstrated laser platform should have an impact on future photonic integrated circuits as the on-chip coupling between active and passive components is readily achievable.We report the room-temperature lasing action from two-dimensional photonic crystal (PC) structures composed of a passive Si3N4 backbone with an over-coat of CdSe/CdS/ZnS colloidal quantum dots (CQDs) for optical gain. When optically excited, devices lased in dual PC band-edge modes, with the modal dominance governed by the thickness of the CQD over-layer. The demonstrated laser platform should have an impact on future photonic integrated circuits as the on-chip coupling between active and passive components is readily achievable. Electronic supplementary information (ESI) available. See DOI: 10.1039/c5nr08544f

  13. Colloidal quantum-dot-based silica gel glass: two-photon absorption, emission, and quenching mechanism.

    PubMed

    Li, Jingzhou; Dong, Hongxing; Zhang, Saifeng; Ma, Yunfei; Wang, Jun; Zhang, Long

    2016-09-28

    Two-photon (TP) three-dimensional solid matrices have potential applications in high density optical data reading and storage, infrared-pumped visible displays, lasers, etc. Such technologies will benefit greatly from the advantageous properties of TP materials including tunable emission wavelength, photostability, and simple chemical processing. Here, this ideal TP solid is made possible by using a facile sol-gel process to engineer colloid quantum dots into silica gel glass. Characterization using an open-aperture Z-scan technique shows that the solid matrices exhibited significant TP optical properties with a TP absorption coefficient of (9.41 ± 0.39) × 10(-2) cm GW(-1) and a third-order nonlinear figure of merit of (7.30 ± 0.30) × 10(-14) esu cm. In addition, the dependence of the TP properties on high-temperature thermal treatment is studied in detail to obtain a clear insight for practical applications. The results illustrate that the sample can maintain stable TP performance below the synthesis temperature of the CdTe/CdS colloidal quantum dots. Furthermore, the mechanisms for thermal quenching of photoluminescence under different temperature regimes are clarified as a function of the composition. PMID:27602563

  14. Structural and optical characterization of electrodeposited CdSe in mesoporous anatase TiO2 for regenerative quantum-dot-sensitized solar cells.

    PubMed

    Sauvage, Frédéric; Davoisne, Carine; Philippe, Laetitia; Elias, Jamil

    2012-10-01

    We investigated CdSe-sensitized TiO(2) solar cells by means of electrodeposition under galvanostatic control. The electrodeposition of CdSe within the mesoporous film of TiO(2) gives rise to a uniform, thickness controlled, conformal layer of nanostructured CdSe particles intimately wrapping the anatase TiO(2) nanoparticles. This technique has the advantage of providing not only a fast method for sensitization ( < 5 min) but also being easily scalable to the sensitization of large-area panels. XRD together with SAED analysis highlight that the deposit of CdSe is exclusively constituted of the hexagonal polymorph. In addition, hierarchical growth has also been shown, starting from the formation of a TiO(2)-CdSe core-shell structure followed by the growth of an assembly of CdSe nanoparticles resembling cauliflowers. This assembly exhibits at its core a mosaic texture with crystallites of about 3 nm in size, in contrast to a shell composed of well-crystallized single crystals between 5 and 10 nm in size. Preliminary results on the photovoltaic performance of such a nanostructured composite of TiO(2) and CdSe show 0.8% power conversion efficiency under A.M.1.5 G conditions-100 mW cm(-2) in association with a new regenerative redox couple based on cobalt(+III/+II) polypyridil complex (V(oc ) = 485 mV, J(sc ) = 4.26 mA cm (-2), ff=0.37).

  15. Structural and optical characterization of electrodeposited CdSe in mesoporous anatase TiO2 for regenerative quantum-dot-sensitized solar cells.

    PubMed

    Sauvage, Frédéric; Davoisne, Carine; Philippe, Laetitia; Elias, Jamil

    2012-10-01

    We investigated CdSe-sensitized TiO(2) solar cells by means of electrodeposition under galvanostatic control. The electrodeposition of CdSe within the mesoporous film of TiO(2) gives rise to a uniform, thickness controlled, conformal layer of nanostructured CdSe particles intimately wrapping the anatase TiO(2) nanoparticles. This technique has the advantage of providing not only a fast method for sensitization ( < 5 min) but also being easily scalable to the sensitization of large-area panels. XRD together with SAED analysis highlight that the deposit of CdSe is exclusively constituted of the hexagonal polymorph. In addition, hierarchical growth has also been shown, starting from the formation of a TiO(2)-CdSe core-shell structure followed by the growth of an assembly of CdSe nanoparticles resembling cauliflowers. This assembly exhibits at its core a mosaic texture with crystallites of about 3 nm in size, in contrast to a shell composed of well-crystallized single crystals between 5 and 10 nm in size. Preliminary results on the photovoltaic performance of such a nanostructured composite of TiO(2) and CdSe show 0.8% power conversion efficiency under A.M.1.5 G conditions-100 mW cm(-2) in association with a new regenerative redox couple based on cobalt(+III/+II) polypyridil complex (V(oc ) = 485 mV, J(sc ) = 4.26 mA cm (-2), ff=0.37). PMID:22972037

  16. Self-organized colloidal quantum dots and metal nanoparticles for plasmon-enhanced intermediate-band solar cells.

    PubMed

    Mendes, Manuel J; Hernández, Estela; López, Esther; García-Linares, Pablo; Ramiro, Iñigo; Artacho, Irene; Antolín, Elisa; Tobías, Ignacio; Martí, Antonio; Luque, Antonio

    2013-08-30

    A colloidal deposition technique is presented to construct long-range ordered hybrid arrays of self-assembled quantum dots and metal nanoparticles. Quantum dots are promising for novel opto-electronic devices but, in most cases, their optical transitions of interest lack sufficient light absorption to provide a significant impact in their implementation. A potential solution is to couple the dots with localized plasmons in metal nanoparticles. The extreme confinement of light in the near-field produced by the nanoparticles can potentially boost the absorption in the quantum dots by up to two orders of magnitude.In this work, light extinction measurements are employed to probe the plasmon resonance of spherical gold nanoparticles in lead sulfide colloidal quantum dots and amorphous silicon thin-films. Mie theory computations are used to analyze the experimental results and determine the absorption enhancement that can be generated by the highly intense near-field produced in the vicinity of the gold nanoparticles at their surface plasmon resonance.The results presented here are of interest for the development of plasmon-enhanced colloidal nanostructured photovoltaic materials, such as colloidal quantum dot intermediate-band solar cells. PMID:23912379

  17. Self-organized colloidal quantum dots and metal nanoparticles for plasmon-enhanced intermediate-band solar cells.

    PubMed

    Mendes, Manuel J; Hernández, Estela; López, Esther; García-Linares, Pablo; Ramiro, Iñigo; Artacho, Irene; Antolín, Elisa; Tobías, Ignacio; Martí, Antonio; Luque, Antonio

    2013-08-30

    A colloidal deposition technique is presented to construct long-range ordered hybrid arrays of self-assembled quantum dots and metal nanoparticles. Quantum dots are promising for novel opto-electronic devices but, in most cases, their optical transitions of interest lack sufficient light absorption to provide a significant impact in their implementation. A potential solution is to couple the dots with localized plasmons in metal nanoparticles. The extreme confinement of light in the near-field produced by the nanoparticles can potentially boost the absorption in the quantum dots by up to two orders of magnitude.In this work, light extinction measurements are employed to probe the plasmon resonance of spherical gold nanoparticles in lead sulfide colloidal quantum dots and amorphous silicon thin-films. Mie theory computations are used to analyze the experimental results and determine the absorption enhancement that can be generated by the highly intense near-field produced in the vicinity of the gold nanoparticles at their surface plasmon resonance.The results presented here are of interest for the development of plasmon-enhanced colloidal nanostructured photovoltaic materials, such as colloidal quantum dot intermediate-band solar cells.

  18. Electro-optical and dielectric properties of CdSe quantum dots and 6CHBT liquid crystals composites

    SciTech Connect

    Singh, U. B.; Pandey, M. B.; Dhar, R; Pandey, A. S.; Kumar, S.; Dabrowski, R.

    2014-11-15

    We have prepared the composites of a room temperature nematic liquid crystal namely 4-(trans-4-n-hexylcyclohexyl) isothiocyanatobenzoate (6CHBT) and Cadmium Selenide Quantum Dots (CdSe-QDs) and investigated their electro-optical and dielectric properties. Effect of dispersion of CdSe-QDs on various electro-optical and display parameters of host liquid crystalline material have been studied. Physical parameters, such as switching threshold voltage and splay elastic constant have been altered drastically for composites. Dispersion of QDs in a liquid crystals medium destabilizes nematic ordering of the host and decreases the nematic-to-isotropic transition temperature.

  19. Surface passivated colloidal CuIn(S,Se)2 quantum dots for quantum dot heterojunction solar cells (Presentation Recording)

    NASA Astrophysics Data System (ADS)

    Yassitepe, Emre; Voznyy, Oleksandr; Sargent, Edward; Nogueira, Ana Flavia F.

    2015-10-01

    Colloidal quantum dot heterojunction thin film solar cells (CQD-TFSC) utilize facile thin film deposition methods and promise high photon conversion efficiencies (PCE) to cost ratio which is highly desired for commercialization. So far, surface passivated PbS CQD-TFSCs show the highest PCE results, reaching 9.2% with good stability. Among other potential candidates, CuInSe2 CQDs stand out as a non-toxic material with high potential for performance, judging on bulk Cu(Ga,In)(S,Se)2 TFSCs reaching 20% PCE, with high stability. CuInSe2 CQDs has advantage over bulk films, mainly the much less expensive manufacturing cost of uniform deposition on large areas. Ga is known to cause phase separation in the bulk CIGS system. In a CQD form, CuInSe2 band gap can be tuned between 1 to 1.6 eV by quantum confinement without need for Ga and this eliminates the phase separation issue. Within our best knowledge, there are no reports on surface trap passivated CuInSe2 CQD-TFSCs. However Cu(In,Ga)(S,Se)2 colloidal particles were cast in thin film form and fused to form bulk-like crystals by various annealing conditions for solar cell devices. In this work, we investigated well-passivated CuInSe2 CQDs on n-type TiO2 and ZnO layers to form depleted heterojunction structure. We prepared luminescent CuInSe2 CQDs by synthetic wet chemistry methods and passivated the surface with 3-mercaptopropionic acid or tetrabutylammonium iodide using solid-state ligand exchange. X-ray photoelectron spectroscopy was used to confirm the ligand boding and surface coverage of the quantum dots. We will present the effect of synthesis and thin film preparation conditions on the solar cell device performance

  20. Correlated blinking via time dependent energy transfer in single CdSe quantum dot-dye nanoassemblies

    NASA Astrophysics Data System (ADS)

    Gerlach, Frank; Täuber, Daniela; von Borczyskowski, Christian

    2013-05-01

    Optical confocal spectroscopy on self-assembled single nanoassemblies from CdSe/ZnS quantum dots (QD) and perylene diimide dye molecules demonstrates efficient Förster resonance energy transfer (FRET). Intramolecular dynamics of the flexible dye molecule change the FRET efficiency in course of the detection period of several minutes. This can be followed by correlated observations of luminescence intensities and related spectral shifts of both constituents. Contrary to several experiments on similar assemblies, the FRET efficiencies are by almost one order of magnitude larger in the non-polar liquid solvent TEHOS as compared e.g. to toluene. Experimental and theoretically expected efficiencies are in close agreement with each other.

  1. Nanoscale Interfaces in Colloidal Quantum Dot Solar Cells: Physical Insights and Materials Engineering Strategies

    NASA Astrophysics Data System (ADS)

    Kemp, Kyle Wayne

    With growing global energy demand there will be an increased need for sources of renewable energy such as solar cells. To make these photovoltaic technologies more competitive with conventional energy sources such as coal and natural gas requires further reduction in manufacturing costs that can be realized by solution processing and roll-to-roll printing. Colloidal quantum dots are a bandgap tunable, solution processible, semiconductor material which may offer a path forward to efficient, inexpensive photovoltaics. Despite impressive progress in performance with these materials, there remain limitations in photocarrier collection that must be overcome. This dissertation focuses on the characterization of charge recombination and transport in colloidal quantum dot photovoltaics, and the application of this knowledge to the development of new and better materials. Core-shell, PbS-CdS, quantum dots were investigated in an attempt to achieve better surface passivation and reduce electronic defects which can limit performance. Optimization of this material led to improved open circuit voltage, exceeding 0.6 V for the first time, and record published performance of 6% efficiency. Using temperature-dependent and transient photovoltage measurements we explored the significance of interface recombination on the operation of these devices. Careful engineering of the electrode using atomic layer deposition of ZnO helped lead to better TiO2 substrate materials and allowed us to realize a nearly two-fold reduction in recombination rate and an enhancement upwards of 50 mV in open circuit voltage. Carrier extraction efficiency was studied in these devices using intensity dependent current-voltage data of an operational solar cell. By developing an analytical model to describe recombination loss within the active layer of the device we were able to accurately determine transport lengths ranging up to 90 nm. Transient absorption and photoconductivity techniques were used to study

  2. Infrared Colloidal Quantum Dot Photovoltaics via Coupling Enhancement and Agglomeration Suppression.

    PubMed

    Ip, Alexander H; Kiani, Amirreza; Kramer, Illan J; Voznyy, Oleksandr; Movahed, Hamidreza F; Levina, Larissa; Adachi, Michael M; Hoogland, Sjoerd; Sargent, Edward H

    2015-09-22

    Materials optimized for single-junction solar spectral harvesting, such as silicon, perovskites, and large-band-gap colloidal quantum dot solids, fail to absorb the considerable infrared spectral energy that lies below their respective band gap. Here we explore through modeling and experiment the potential for colloidal quantum dots (CQDs) to augment the performance of solar cells by harnessing transmitted light in the infrared. Through detailed balance modeling, we identify the CQD band gap that is best able to augment wafer-based, thin-film, and also solution-processed photovoltaic (PV) materials. The required quantum dots, with an excitonic peak at 1.3 μm, have not previously been studied in depth for solar performance. Using computational studies we find that a new ligand scheme distinct from that employed in better-explored 0.95 μm band gap PbS CQDs is necessary; only via the solution-phase application of a short bromothiol can we prevent dot fusion during ensuing solid-state film treatments and simultaneously offer a high valence band-edge density of states to enhance hole transport. Photoluminescence spectra and transient studies confirm the desired narrowed emission peaks and reduced surface-trap-associated decay. Electronic characterization reveals that only through the use of the bromothiol ligands is strong hole transport retained. The films, when used to make PV devices, achieve the highest AM1.5 power conversion efficiency yet reported in a solution-processed material having a sub-1 eV band gap.

  3. Luminescence properties of II/VI semiconductor colloidal nanocrystals at collective and single scales

    NASA Astrophysics Data System (ADS)

    Vion, Céline; Barthou, Carlos; Coolen, Laurent; Bennaloul, Paul; Chinh, Vu Duc; Thuy Linh, Pham; Thi Bich, Vu; Thu Nga, Pham; Maître, Agnès

    2009-09-01

    Colloidal nanocrystals are crystalline spheres of semiconductors of a few nanometers, obtained by chemical synthesis. At this size scale, lower than Bohr radius of the exciton, emission properties are dominated by quantum confinement effects and depend crucially on the nanocrystal radius, which can be controlled by adjusting the synthesis parameters. Nanocrystals present high photostability and good quantum efficiency, even at room temperature. Their emission wavelength can be tuned over the whole visible range, making them very attractive solid state light sources which are already used in optoelectronic devices or for biological labeling. The luminescence properties of CdSe colloidal nanocrystals synthesized at the Institute of Materials Science in Hanoi are presented. At collective scale, the emission properties reveal the synthesis quality. Temperature effects from ambient to 4 K on spectra and decay rates will be presented and analyzed in terms of emitting level fine structure. The study of CdSe colloidal quantum dots at the single emitter scale is of great interest as it reveals properties which are hidden by collective studies, such as luminescence "blinking", a random switching from a fluorescent to a non fluorescent state, which is closely related to the crystalline defects of a nanocrystal and its interaction with its environment. We will present the blinking properties of the prepared nanocrystals, and relate them to the nanocrystals synthesis quality and shell quality.

  4. Study of colloidal quantum-dot surfaces using an innovative thin-film positron 2D-ACAR method

    NASA Astrophysics Data System (ADS)

    Eijt, Stephan W. H.; van Veen, Anton (Tom); Schut, Henk; Mijnarends, Peter E.; Denison, Art B.; Barbiellini, Bernardo; Bansil, Arun

    2006-01-01

    Nanosized inorganic particles are of great interest because their electronic properties can be easily tailored, providing a tremendous potential for applications in optoelectronic devices, light-emitting diodes, solar cells and hydrogen storage. Confinement of electrons and holes to dimensions comparable to their wavelength leads to quantum-well states with modified wavefunctions and density of states. Surface phenomena are crucial in determining nanoparticle properties in view of their large surface-to-volume ratio. Despite a wealth of information, many fundamental questions about the nature of the surface and its relationship with the electronic structure remain unsolved. Ab initio calculations on CdSe nanocrystals suggest that passivating the ligands does not produce the ideal wurtzite structure and that Se atoms relax outwards irrespective of passivation. Here we show that implanted positrons are trapped at the surface of CdSe nanocrystals. They annihilate mostly with the Se electrons, monitor changes in composition and structure of the surface while hardly sensing the ligand molecules, and we thus unambiguously confirm the predicted strong surface relaxation.

  5. Narrow bandgap colloidal metal chalcogenide quantum dots: synthetic methods, heterostructures, assemblies, electronic and infrared optical properties.

    PubMed

    Kershaw, Stephen V; Susha, Andrei S; Rogach, Andrey L

    2013-04-01

    The chemistry, material processing and fundamental understanding of colloidal semiconductor nanocrystals (quantum dots) are advancing at an astounding rate, bringing the prospects of widespread commercialization of these novel and exciting materials ever closer. Interest in narrow bandgap nanocrystals in particular has intensified in recent years, and the results of research worldwide point to the realistic prospects of applications for these materials in solar cells, infrared optoelectronics (e.g. lasers, optical modulators, photodetectors and photoimaging devices), low cost/large format microelectronics, and in biological imaging and biosensor systems to name only some technologies. Improvements in fundamental understanding and material quality are built on a vast body of experience spread over many different methods of colloidal synthetic growth, each with their own strengths and weaknesses for different materials and sometimes with regard to particular applications. The nanocrystal growth expertise is matched by a rapidly expanding, and highly interdisciplinary, understanding of how best to assemble these materials into films or hybrid composites and thereby into useful devices, and again there are many different strategies that can be adopted. In this review we have attempted to survey and compare the recent work on colloidal synthesis, film and nanocrystal composite material fabrication, concentrating on narrow bandgap chalcogenide materials and some of their topical applications in the solar energy and biological fields. Since these applications are attracting rising interest across a wide range of disciplines, from the biological sciences, device engineering, and materials processing fields as well as the physics and synthetic chemistry communities, we have endeavoured to make the review of these narrow bandgap nanomaterials both comprehensive and accessible to newcomers to the area. PMID:23361653

  6. Narrow bandgap colloidal metal chalcogenide quantum dots: synthetic methods, heterostructures, assemblies, electronic and infrared optical properties.

    PubMed

    Kershaw, Stephen V; Susha, Andrei S; Rogach, Andrey L

    2013-04-01

    The chemistry, material processing and fundamental understanding of colloidal semiconductor nanocrystals (quantum dots) are advancing at an astounding rate, bringing the prospects of widespread commercialization of these novel and exciting materials ever closer. Interest in narrow bandgap nanocrystals in particular has intensified in recent years, and the results of research worldwide point to the realistic prospects of applications for these materials in solar cells, infrared optoelectronics (e.g. lasers, optical modulators, photodetectors and photoimaging devices), low cost/large format microelectronics, and in biological imaging and biosensor systems to name only some technologies. Improvements in fundamental understanding and material quality are built on a vast body of experience spread over many different methods of colloidal synthetic growth, each with their own strengths and weaknesses for different materials and sometimes with regard to particular applications. The nanocrystal growth expertise is matched by a rapidly expanding, and highly interdisciplinary, understanding of how best to assemble these materials into films or hybrid composites and thereby into useful devices, and again there are many different strategies that can be adopted. In this review we have attempted to survey and compare the recent work on colloidal synthesis, film and nanocrystal composite material fabrication, concentrating on narrow bandgap chalcogenide materials and some of their topical applications in the solar energy and biological fields. Since these applications are attracting rising interest across a wide range of disciplines, from the biological sciences, device engineering, and materials processing fields as well as the physics and synthetic chemistry communities, we have endeavoured to make the review of these narrow bandgap nanomaterials both comprehensive and accessible to newcomers to the area.

  7. Composition-dependent trap distributions in CdSe and InP quantum dots probed using photoluminescence blinking dynamics

    NASA Astrophysics Data System (ADS)

    Chung, Heejae; Cho, Kyung-Sang; Koh, Weon-Kyu; Kim, Dongho; Kim, Jiwon

    2016-07-01

    Although Group II-VI quantum dots (QDs) have attracted much attention due to their wide range of applications in QD-based devices, the presence of toxic ions in II-VI QDs raises environmental concerns. To fulfill the demands of nontoxic QDs, synthetic routes for III-V QDs have been developed. However, only a few comparative analyses on optical properties of III-V QDs have been performed. In this study, the composition-related energetic trap distributions have been explored by using three different types of core/multishell QDs: CdSe-CdS (CdSe/CdS/ZnS), InP-ZnSe (InP/ZnSe/ZnS), and InP-GaP (InP/GaP/ZnS). It was shown that CdSe-CdS QDs have much larger trap densities than InP-shell QDs at higher energy states (at least 1Eg (band gap energy) above the lowest conduction band edge) based on probability density plots and Auger ionization efficiencies which are determined by analyses of photoluminescence blinking dynamics. This result suggests that the composition of encapsulated QDs is closely associated with the charge trapping processes, and also provides an insight into the development of more environmentally friendly QD-based devices.Although Group II-VI quantum dots (QDs) have attracted much attention due to their wide range of applications in QD-based devices, the presence of toxic ions in II-VI QDs raises environmental concerns. To fulfill the demands of nontoxic QDs, synthetic routes for III-V QDs have been developed. However, only a few comparative analyses on optical properties of III-V QDs have been performed. In this study, the composition-related energetic trap distributions have been explored by using three different types of core/multishell QDs: CdSe-CdS (CdSe/CdS/ZnS), InP-ZnSe (InP/ZnSe/ZnS), and InP-GaP (InP/GaP/ZnS). It was shown that CdSe-CdS QDs have much larger trap densities than InP-shell QDs at higher energy states (at least 1Eg (band gap energy) above the lowest conduction band edge) based on probability density plots and Auger ionization

  8. Modeling of self-diffraction from the induced aperture in colloidal quantum dots

    NASA Astrophysics Data System (ADS)

    Ezhova, K.; Smirnov, A.

    2015-05-01

    Modeling of self-diffraction pattern formation from the induced diaphragm, arising in the case of the transparency channel saturation by one-photon resonant non-stationary excitation of the basic exciton transition in colloidal quantum dots (QDs) is realized. The simulation results allow us to obtain the reference image of self-diffraction pattern and dependence of the intensity transverse distribution of the output beam from the intensity of the excitation beam, forming a transparency channel. A powerful laser pulse creates a transparency channel, so that it self-diffracts on the induced diaphragm. The possibility to apply the obtained simulation results for intensity estimation of the laser radiation and for the possible application in the technique (nonlinear-optical limiters of intense laser radiation in the visible and nearinfrared region, optical switches) are discussed.

  9. Random lasing in a colloidal quantum dot-doped disordered polymer.

    PubMed

    Cao, Mingxuan; Zhang, Yating; Song, Xiaoxian; Che, Yongli; Zhang, Haiting; Dai, Haitao; Zhang, Guizhong; Yao, Jianquan

    2016-05-01

    We report random lasing in colloidal quantum dots (CQDs) doped disordered polymer. The CdSe/ZnS core-shell CQDs are dispersed in hybrid polymer including two types of monomers with different rates of polymerization. After UV curing, spatially localized random resonators are formed owing to long range refractive-index fluctuations in inhomogeneous polymer with gain. Upon the optical excitation, random lasing action is triggered above the threshold of 7mJ/cm2. Through the investigation on the spectral characteristics of random laser, the wavelengths of random lasers strongly depend on pump position, which confirms that random laser modes originate from spatially localized resnonators. According to power Fourier transform of emission spectrum, the average size of equivalent micro resonators is attributed to be 50 μm. The proposed method provides a facile route to develop random lasers based on CQDs, showing potential applications on random fiber laser and laser displays. PMID:27137548

  10. 10.6% Certified Colloidal Quantum Dot Solar Cells via Solvent-Polarity-Engineered Halide Passivation.

    PubMed

    Lan, Xinzheng; Voznyy, Oleksandr; García de Arquer, F Pelayo; Liu, Mengxia; Xu, Jixian; Proppe, Andrew H; Walters, Grant; Fan, Fengjia; Tan, Hairen; Liu, Min; Yang, Zhenyu; Hoogland, Sjoerd; Sargent, Edward H

    2016-07-13

    Colloidal quantum dot (CQD) solar cells are solution-processed photovoltaics with broad spectral absorption tunability. Major advances in their efficiency have been made via improved CQD surface passivation and device architectures with enhanced charge carrier collection. Herein, we demonstrate a new strategy to improve further the passivation of CQDs starting from the solution phase. A cosolvent system is employed to tune the solvent polarity in order to achieve the solvation of methylammonium iodide (MAI) and the dispersion of hydrophobic PbS CQDs simultaneously in a homogeneous phase, otherwise not achieved in a single solvent. This process enables MAI to access the CQDs to confer improved passivation. This, in turn, allows for efficient charge extraction from a thicker photoactive layer device, leading to a certified solar cell power conversion efficiency of 10.6%, a new certified record in CQD photovoltaics.

  11. Colloidal quantum dots as probes of excitation field enhancement in photonic antennas.

    PubMed

    Aouani, Heykel; Itzhakov, Stella; Gachet, David; Devaux, Eloïse; Ebbesen, Thomas W; Rigneault, Hervé; Oron, Dan; Wenger, Jérôme

    2010-08-24

    Optical antennas are essential devices to interface light to nanoscale volumes and locally enhance the electromagnetic intensity. Various experimental methods can be used to quantify the antenna amplification on the emission process, yet characterizing the antenna amplification at the excitation frequency solely is a challenging task. Such experimental characterization is highly needed to fully understand and optimize the antenna response. Here, we describe a novel experimental tool to directly measure the antenna amplification on the excitation field independently of the emission process. We monitor the transient emission dynamics of colloidal quantum dots and show that the ratio of doubly to singly excited state photoluminescence decay amplitudes is an accurate tool to quantify the local excitation intensity amplification. This effect is demonstrated on optical antennas made of polystyrene microspheres and gold nanoapertures, and supported by numerical computations. The increased doubly excited state formation on nanoantennas realizes a new demonstration of enhanced light-matter interaction at the nanoscale.

  12. Lasing and magnetic microbeads loaded with colloidal quantum dots and iron oxide nanocrystals

    NASA Astrophysics Data System (ADS)

    Li, Minxu; You, Guanjun; Wang, Andrew Y.; Hu, Wenjia; Wang, Jingkang; Sun, Fengqing; Zhu, Yiming; Henderson, Ron; Xu, Jian

    2013-09-01

    This study investigates the feasibility of loading nanostructured lasing medium and magnetic nanocrystals in the same microbead for potential applications in bio- and chemical sensing. A sequential infiltration process is proposed and tested for the preparation of magnetic and lasing microbeads by incorporating, respectively, iron oxide nanocrystals in the inner cores and colloidal quantum dots (CQDs) in the periphery regions of mesoporous silica microbeads. The co-doped bead structure was confirmed by electron microscopy and energy dispersive spectroscopy. The lasing action of the CQD gain medium in the mesoporous beads was characterized with micro-photoluminescence, revealing sharp whispering gallery mode lasing signatures, whereas the distinguishing superparamagnetic property was measured from the co-doped microbeads with vibrating sample magnetometry.

  13. Resonance-induced absorption enhancement in colloidal quantum dot solar cells using nanostructured electrodes.

    PubMed

    Mahpeykar, Seyed Milad; Xiong, Qiuyang; Wang, Xihua

    2014-10-20

    The application of nanostructured indium-doped tin oxide (ITO) electrodes as diffraction gratings for light absorption enhancement in colloidal quantum dot solar cells is numerically investigated using finite-difference time-domain (FDTD) simulation. Resonant coupling of the incident diffracted light with supported waveguide modes in light absorbing layer at particular wavelengths predicted by grating far-field projection analysis is shown to provide superior near-infrared light trapping for nanostructured devices as compared to the planar structure. Among various technologically feasible nanostructures, the two-dimensional nano-branch array is demonstrated as the most promising polarization-independent structure and proved to be able to maintain its performance despite structural imperfections common in fabrication. PMID:25607315

  14. Resonance-induced absorption enhancement in colloidal quantum dot solar cells using nanostructured electrodes.

    PubMed

    Mahpeykar, Seyed Milad; Xiong, Qiuyang; Wang, Xihua

    2014-10-20

    The application of nanostructured indium-doped tin oxide (ITO) electrodes as diffraction gratings for light absorption enhancement in colloidal quantum dot solar cells is numerically investigated using finite-difference time-domain (FDTD) simulation. Resonant coupling of the incident diffracted light with supported waveguide modes in light absorbing layer at particular wavelengths predicted by grating far-field projection analysis is shown to provide superior near-infrared light trapping for nanostructured devices as compared to the planar structure. Among various technologically feasible nanostructures, the two-dimensional nano-branch array is demonstrated as the most promising polarization-independent structure and proved to be able to maintain its performance despite structural imperfections common in fabrication.

  15. Solution-processed high-performance colloidal quantum dot tandem photodetectors on flexible substrates

    SciTech Connect

    Jiang, Zhenyu; You, Guanjun; Wang, Li; Liu, Jie; Xu, Jian; Hu, Wenjia; Zhang, Yu

    2014-08-28

    We report a high-performance colloidal quantum dot (CQD)-based near-infrared tandem photodetector fabricated on flexible substrates via solution-processed method. The tandem photodetector on poly(ethylene terephthalate) substrates exhibited low dark current and high detectivities over ∼8.8 × 10{sup 11} Jones at near infrared range at −0.5 V bias and over ∼10{sup 13} Jones near 0 bias. The critical bend radii of ∼8 mm and ∼3 mm have been demonstrated for tensile and compressive bending, respectively. The performance of photodetectors remains stable under mechanical stress, making PbSe CQD material a promise candidate for flexible infrared sensing applications.

  16. Statistical interpretation of transient current power-law decay in colloidal quantum dot arrays

    NASA Astrophysics Data System (ADS)

    Sibatov, R. T.

    2011-08-01

    A new statistical model of the charge transport in colloidal quantum dot arrays is proposed. It takes into account Coulomb blockade forbidding multiple occupancy of nanocrystals and the influence of energetic disorder of interdot space. The model explains power-law current transients and the presence of the memory effect. The fractional differential analogue of the Ohm law is found phenomenologically for nanocrystal arrays. The model combines ideas that were considered as conflicting by other authors: the Scher-Montroll idea about the power-law distribution of waiting times in localized states for disordered semiconductors is applied taking into account Coulomb blockade; Novikov's condition about the asymptotic power-law distribution of time intervals between successful current pulses in conduction channels is fulfilled; and the carrier injection blocking predicted by Ginger and Greenham (2000 J. Appl. Phys. 87 1361) takes place.

  17. 10.6% Certified Colloidal Quantum Dot Solar Cells via Solvent-Polarity-Engineered Halide Passivation.

    PubMed

    Lan, Xinzheng; Voznyy, Oleksandr; García de Arquer, F Pelayo; Liu, Mengxia; Xu, Jixian; Proppe, Andrew H; Walters, Grant; Fan, Fengjia; Tan, Hairen; Liu, Min; Yang, Zhenyu; Hoogland, Sjoerd; Sargent, Edward H

    2016-07-13

    Colloidal quantum dot (CQD) solar cells are solution-processed photovoltaics with broad spectral absorption tunability. Major advances in their efficiency have been made via improved CQD surface passivation and device architectures with enhanced charge carrier collection. Herein, we demonstrate a new strategy to improve further the passivation of CQDs starting from the solution phase. A cosolvent system is employed to tune the solvent polarity in order to achieve the solvation of methylammonium iodide (MAI) and the dispersion of hydrophobic PbS CQDs simultaneously in a homogeneous phase, otherwise not achieved in a single solvent. This process enables MAI to access the CQDs to confer improved passivation. This, in turn, allows for efficient charge extraction from a thicker photoactive layer device, leading to a certified solar cell power conversion efficiency of 10.6%, a new certified record in CQD photovoltaics. PMID:27351104

  18. Silanization of Low-Temperature-Plasma Synthesized Silicon Quantum Dots for Production of a Tunable, Stable, Colloidal Solution

    SciTech Connect

    Anderson, I. E.; Shircliff, R. A.; Macauley, C.; Smith, D. K.; Lee, B. G.; Agrawal, S.; Stradins, P.; Collins, R. T.

    2012-02-16

    We present a method for grafting silanes onto low-temperature-plasma synthesized silicon quantum dots. The resulting solution of dots is characterized with Fourier transform infrared spectroscopy and transmission electron microscopy, and determined to be a colloidal suspension. The silane is attached at a single point on the quantum dot surface to avoid cross-linking and multilayer formation, and photoluminescence spectroscopy shows the colloidal suspension of dots is stable for over two months in air. The hydroxyl-terminated surfaces required for silanization are created by wet chemical etch, which can be used to tune the luminescence of the silicon dots in the green- to red-wavelength range. We find, however, that the wet etch cannot move the emission into the blue-wavelength range and discuss this observation in terms of the nature of etching process and origin of the emission. In addition, we discuss the photoluminescence quantum yield in the context of other passivation and synthetic techniques.

  19. Surface Induced Magnetism in Quantum Dots

    SciTech Connect

    Meulenberg, R W; Lee, J I

    2009-08-20

    The study of nanometer sized semiconductor crystallites, also known as quantum dots (QDs), has seen rapid advancements in recent years in scientific disciplines ranging from chemistry, physics, biology, materials science, and engineering. QD materials of CdSe, ZnSe, InP, as well as many others, can be prepared in the size range of 1-10 nm producing uniform, nearly monodisperse materials that are typically coated with organic molecules [1-3]. The strength of charge carrier confinement, which dictates the size-dependent properties, in these QDs depends on the nature of the material and can be correlated to the Bohr radius for the system of interest. For instance, the Bohr radius for CdSe is {approx} 5 nm, while in the more covalent structure of InP, the Bohr radius approaches {approx} 10 nm. The study of CdSe QDs has been particularly extensive during the last decade because they exhibit unique and tunable optical properties and are readily synthesized with high-crystallinity and narrow size dispersions. Although the core electronic properties of CdSe are explained in terms of the quantum confinement model, experimental efforts to elucidate the surface structure of these materials have been limited. Typically, colloidal CdSe QDs are coated with an organic surfactant, which typically consists of an organo-phosphine, -thiol, or -amine, that has the function of energetically relaxing defect states via coordination to partially coordinated surface atoms. The organic surfactant also acts to enhance carrier confinement and prevent agglomeration of the particles. Chemically, it has been shown that the bonding of the surfactant to the CdSe QD occurs through Cd atoms resulting cleavage of the Se atoms and formation of a Cd-rich (i.e. non-stoichiometric) particle [5].

  20. Non-blinking single-photon generation with anisotropic colloidal nanocrystals: towards room-temperature, efficient, colloidal quantum sources.

    PubMed

    Pisanello, Ferruccio; Leménager, Godefroy; Martiradonna, Luigi; Carbone, Luigi; Vezzoli, Stefano; Desfonds, Pascal; Cozzoli, Pantaleo Davide; Hermier, Jean-Pierre; Giacobino, Elisabeth; Cingolani, Roberto; De Vittorio, Massimo; Bramati, Alberto

    2013-04-11

    Blinking and single-photon emission can be tailored in CdSe/CdS core/shell colloidal dot-in-rods. By increasing the shell thickness it is possible to obtain almost non-blinking nanocrystals, while the shell length can be used to control single-photon emission probability.

  1. Multi-branched CdSe nanocrystals stabilized by weak ligand for hybrid solar cell application.

    PubMed

    Liu, Jincheng; Tao, Hong; Cao, Yong; Ackermann, Jorg

    2014-04-01

    In this article, multi-branched CdSe nanocrystals were produced by a facile colloidal approach stabilized by oleylamine at a relative low temperature. The as-prepared multi-branched CdSe nanocrystals after simple washing process were used in the fabrication of poly(3-hexylthiophene)/CdSe bulk heterojunction photovoltaic device. The effective charge separation in the poly(3-hexylthiophene)/ CdSe nanocomposites have been confirmed by the strong photoluminescence quenching. The films of the blends of P3HT and simply-washed CdSe nanocrystals show more uniform morphology and flatter surface than the film of the bends of P3HT and pyridine-refluxed CdSe nanocrystals. The corresponding power conversion efficiency under 1 sun is about 0.66% for the P3HT/pyridine-washed CdSe hybrid device. Our work did a preliminary study in the hybrid solar cell application of branched blenze CdSe nanocrystals prepared by an easier way, and will be interesting and helpful for making the high-efficiency hybrid solar cells with branched CdSe acceptors.

  2. Novel Colloidal MoS2 Quantum Dot Heterojunctions on Silicon Platforms for Multifunctional Optoelectronic Devices.

    PubMed

    Mukherjee, Subhrajit; Maiti, Rishi; Katiyar, Ajit K; Das, Soumen; Ray, Samit K

    2016-01-01

    Silicon compatible wafer scale MoS2 heterojunctions are reported for the first time using colloidal quantum dots. Size dependent direct band gap emission of MoS2 dots are presented at room temperature. The temporal stability and decay dynamics of excited charge carriers in MoS2 quantum dots have been studied using time correlated single photon counting spectroscopy technique. Fabricated n-MoS2/p-Si 0D/3D heterojunctions exhibiting excellent rectification behavior have been studied for light emission in the forward bias and photodetection in the reverse bias. The electroluminescences with white light emission spectra in the range of 450-800 nm are found to be stable in the temperature range of 10-350 K. Size dependent spectral responsivity and detectivity of the heterojunction devices have been studied. The peak responsivity and detectivity of the fabricated heterojunction detector are estimated to be ~0.85 A/W and ~8 × 10(11) Jones, respectively at an applied bias of -2 V for MoS2 QDs of 2 nm mean diameter. The above values are found to be superior to the reported results on large area photodetector devices fabricated using two dimensional materials. PMID:27357596

  3. Conformal fabrication of colloidal quantum dot solids for optically enhanced photovoltaics.

    PubMed

    Labelle, André J; Thon, Susanna M; Kim, Jin Young; Lan, Xinzheng; Zhitomirsky, David; Kemp, Kyle W; Sargent, Edward H

    2015-05-26

    Colloidal quantum dots (CQD) are an attractive thin-film material for photovoltaic applications due to low material costs, ease of fabrication, and size-tunable band gap. Unfortunately, today they suffer from a compromise between light absorption and photocarrier extraction, a fact that currently prevents the complete harvest of incoming above-band-gap solar photons. We have investigated the use of structured substrates and/or electrodes to increase the effective light path through the active material and found that these designs require highly conformal application of the light-absorbing films to achieve the greatest enhancement. This conformality requirement derives from the need for maximal absorption enhancement combined with shortest-distance charge transport. Here we report on a means of processing highly conformal layer-by-layer deposited CQD absorber films onto microstructured, light-recycling electrodes. Specifically, we engineer surface hydrophilicity to achieve conformal deposition of upper layers atop underlying ones. We show that only with the application of conformal coating can we achieve optimal quantum efficiency and enhanced power conversion efficiency in structured-electrode CQD cells.

  4. High-Efficiency Colloidal Quantum Dot Photovoltaics via Robust Self-Assembled Monolayers.

    PubMed

    Kim, Gi-Hwan; García de Arquer, F Pelayo; Yoon, Yung Jin; Lan, Xinzheng; Liu, Mengxia; Voznyy, Oleksandr; Jagadamma, Lethy Krishnan; Abbas, Abdullah Saud; Yang, Zhenyu; Fan, Fengjia; Ip, Alexander H; Kanjanaboos, Pongsakorn; Hoogland, Sjoerd; Kim, Jin Young; Sargent, Edward H

    2015-11-11

    The optoelectronic tunability offered by colloidal quantum dots (CQDs) is attractive for photovoltaic applications but demands proper band alignment at electrodes for efficient charge extraction at minimal cost to voltage. With this goal in mind, self-assembled monolayers (SAMs) can be used to modify interface energy levels locally. However, to be effective SAMs must be made robust to treatment using the various solvents and ligands required for to fabricate high quality CQD solids. We report robust self-assembled monolayers (R-SAMs) that enable us to increase the efficiency of CQD photovoltaics. Only by developing a process for secure anchoring of aromatic SAMs, aided by deposition of the SAMs in a water-free deposition environment, were we able to provide an interface modification that was robust against the ensuing chemical treatments needed in the fabrication of CQD solids. The energy alignment at the rectifying interface was tailored by tuning the R-SAM for optimal alignment relative to the CQD quantum-confined electron energy levels. This resulted in a CQD PV record power conversion efficiency (PCE) of 10.7% with enhanced reproducibility relative to controls.

  5. Spin dynamics in colloidal n-type and Mn^2+-doped ZnO quantum dots

    NASA Astrophysics Data System (ADS)

    Ochsenbein, Stefan; Gamelin, Daniel

    2010-03-01

    Spins in semiconductor quantum dots (QDs) have been proposed as qubits for quantum computing. We have explored the reversible introduction of additional unpaired electrons into colloidal QDs, and have examined the spin properties of these electrons by electron paramagnetic resonance (EPR) spectroscopies. These experiments have revealed that the added electron resides in the conduction band and is delocalized over the entire QD. EPR linewidth analysis has allowed the transverse spin relaxation time constant, T2, to be determined. Reducing the concentration of spin active ^67Zn nuclei in the QDs is shown to increase T2 substantially. The spins of Mn^2+ dopants in ZnO QDs have also been explored. Pulsed EPR experiments show that Mn^2+ spins additionally interact with nuclear spins of the QD surface capping ligands, despite large spatial separation. This study quantifies the interactions that determine T2 of electron and dopant spins in ZnO QDs, and demonstrates manipulation of these interactions by chemical means. These results have bearing on consideration of spins in semiconductor nanostructures for information processing. Relevant references: K. M. Whitaker, S. T. Ochsenbein, V. Z. Polinger, and D. R. Gamelin, J. Phys. Chem. C 112, 14331 (2008). W. K. Liu, K. M. Whitaker, A. L. Smith, K. R. Kittilstved, B. H. Robinson, and D. R. Gamelin, Phys. Rev. Lett. 98, 186804 (2007).

  6. Counterion-Mediated Ligand Exchange for PbS Colloidal Quantum Dot Superlattices

    PubMed Central

    2015-01-01

    In the past years, halide capping became one of the most promising strategies to passivate the surface of colloidal quantum dots (CQDs) in thin films to be used for electronic and optoelectronic device fabrication. This is due to the convenient processing, strong n-type characteristics, and ambient stability of the devices. Here, we investigate the effect of three counterions (ammonium, methylammonium, and tetrabutylammonium) in iodide salts used for treating CQD thin films and shed light on the mechanism of the ligand exchange. We obtain two- and three-dimensional square-packed PbS CQD superlattices with epitaxial merging of nearest neighbor CQDs as a direct outcome of the ligand-exchange reaction and show that the order in the layer can be controlled by the nature of the counterion. Furthermore, we demonstrate that the acidity of the environment plays an important role in the substitution of the carboxylates by iodide ions at the surface of lead chalcogenide quantum dots. Tetrabutylammonium iodide shows lower reactivity compared to methylammonium and ammonium iodide due to the nonacidity of the cation, which eventually leads to higher order but also poorer carrier transport due to incomplete removal of the pristine ligands in the QD thin film. Finally, we show that single-step blade-coating and immersion in a ligand exchange solution such as the one containing methylammonium iodide can be used to fabricate well performing bottom-gate/bottom-contact PbS CQD field effect transistors with record subthreshold swing. PMID:26512884

  7. Novel Colloidal MoS2 Quantum Dot Heterojunctions on Silicon Platforms for Multifunctional Optoelectronic Devices.

    PubMed

    Mukherjee, Subhrajit; Maiti, Rishi; Katiyar, Ajit K; Das, Soumen; Ray, Samit K

    2016-06-30

    Silicon compatible wafer scale MoS2 heterojunctions are reported for the first time using colloidal quantum dots. Size dependent direct band gap emission of MoS2 dots are presented at room temperature. The temporal stability and decay dynamics of excited charge carriers in MoS2 quantum dots have been studied using time correlated single photon counting spectroscopy technique. Fabricated n-MoS2/p-Si 0D/3D heterojunctions exhibiting excellent rectification behavior have been studied for light emission in the forward bias and photodetection in the reverse bias. The electroluminescences with white light emission spectra in the range of 450-800 nm are found to be stable in the temperature range of 10-350 K. Size dependent spectral responsivity and detectivity of the heterojunction devices have been studied. The peak responsivity and detectivity of the fabricated heterojunction detector are estimated to be ~0.85 A/W and ~8 × 10(11) Jones, respectively at an applied bias of -2 V for MoS2 QDs of 2 nm mean diameter. The above values are found to be superior to the reported results on large area photodetector devices fabricated using two dimensional materials.

  8. Novel Colloidal MoS2 Quantum Dot Heterojunctions on Silicon Platforms for Multifunctional Optoelectronic Devices

    PubMed Central

    Mukherjee, Subhrajit; Maiti, Rishi; Katiyar, Ajit K.; Das, Soumen; Ray, Samit K.

    2016-01-01

    Silicon compatible wafer scale MoS2 heterojunctions are reported for the first time using colloidal quantum dots. Size dependent direct band gap emission of MoS2 dots are presented at room temperature. The temporal stability and decay dynamics of excited charge carriers in MoS2 quantum dots have been studied using time correlated single photon counting spectroscopy technique. Fabricated n-MoS2/p-Si 0D/3D heterojunctions exhibiting excellent rectification behavior have been studied for light emission in the forward bias and photodetection in the reverse bias. The electroluminescences with white light emission spectra in the range of 450–800 nm are found to be stable in the temperature range of 10–350 K. Size dependent spectral responsivity and detectivity of the heterojunction devices have been studied. The peak responsivity and detectivity of the fabricated heterojunction detector are estimated to be ~0.85 A/W and ~8 × 1011 Jones, respectively at an applied bias of −2 V for MoS2 QDs of 2 nm mean diameter. The above values are found to be superior to the reported results on large area photodetector devices fabricated using two dimensional materials. PMID:27357596

  9. Process-Dependent Properties in Colloidally Synthesized “Giant” Core/Shell Nanocrystal Quantum Dots

    SciTech Connect

    Hollingsworth, Jennifer A.; Ghosh, Yagnaseni; Dennis, Allison M.; Mangum, Benjamin D.; Park, Young-Shin; Kundu, Janardan; Htoon, Han

    2012-06-07

    Due to their characteristic bright and stable photoluminescence, semiconductor nanocrystal quantum dots (NQDs) have attracted much interest as efficient light emitters for applications from single-particle tracking to solid-state lighting. Despite their numerous enabling traits, however, NQD optical properties are frustratingly sensitive to their chemical environment, exhibit fluorescence intermittency ('blinking'), and are susceptible to Auger recombination, an efficient nonradiative decay process. Previously, we showed for the first time that colloidal CdSe/CdS core/shell nanocrystal quantum dots (NQDs) comprising ultrathick shells (number of shell monolayers, n, > 10) grown by protracted successive ionic layer adsorption and reaction (SILAR) leads to remarkable photostability and significantly suppressed blinking behavior as a function of increasing shell thickness. We have also shown that these so-called 'giant' NQDs (g-NQDs) afford nearly complete suppression of non-radiative Auger recombination, revealed in our studies as long biexciton lifetimes and efficient multiexciton emission. The unique behavior of this core/shell system prompted us to assess correlations between specific physicochemical properties - beyond shell thickness - and functionality. Here, we demonstrate the ability of particle shape/faceting, crystalline phase, and core size to determine ensemble and single-particle optical properties (quantum yield/brightness, blinking, radiative lifetimes). Significantly, we show how reaction process parameters (surface-stabilizing ligands, ligand:NQD ratio, choice of 'inert' solvent, and modifications to the SILAR method itself) can be tuned to modify these function-dictating NQD physical properties, ultimately leading to an optimized synthetic approach that results in the complete suppression of blinking. We find that the resulting 'guiding principles' can be applied to other NQD compositions, allowing us to achieve non-blinking behavior in the near

  10. The Colloidal Stabilization of Quantum Dots: Towards Manufacturable, Efficient Solution-Processed Solar Cells

    NASA Astrophysics Data System (ADS)

    Rollny, Lisa

    Understanding colloidal stabilization can influence the design of optoelectronic devices and enable improvements to their performance and stability. For photovoltaics, important characteristics of the active layer material are high conductivity along with a minimum of recombination centers. In order to capitalize on the benefits of solution-processed materials, it is important to minimize the number of processing steps: ideally, to achieve a low-cost solution, materials would be deposited using a single process step compatible with roll-to-roll manufacturing. Prior to this work, the highest-performing colloidal quantum dots (CQD) solar cells have relied on several deposition steps that are repeated in a layer-by-layer (LBL) fashion. The purpose of these process steps has been to remove the long insulating ligands used in synthesis and replace them with short ligands that allow electrical conduction. The large number of steps combined, typically implemented via spin coating, leads to inefficient materials utilization and fails to show a path to a manufacturable solution. In this work, the first CQD solar cells were designed, built, and characterized combining state-of-art performance with scalable manufacture. Firstly, I report the first automated CQD synthesis to result in CQDs that form high-performance CQD solar cells. I analyze the CQD synthesis and by separating it into two phases---nucleation and growth phase---my insights are used to create higher-quality CQDs exhibiting enhanced monodispersity. I then proceed to develop a CQD ink: a CQD solution ready for direct deposition to form a semiconducting film exhibiting low trap state density. In early trials the CQD ink showed only limited power conversion efficiencies of 2%. I designed a new ink strategy, which I term cleavable hemiketal ligands. This novel two-component ligand strategy enables the combination of colloidal stabilization (via this longer two-component ligand) and cleavability (enabling excellent

  11. Colloidal silicon quantum dots: from preparation to the modification of self-assembled monolayers (SAMs) for bio-applications.

    PubMed

    Cheng, Xiaoyu; Lowe, Stuart B; Reece, Peter J; Gooding, J Justin

    2014-04-21

    Concerns over possible toxicities of conventional metal-containing quantum dots have inspired growing research interests in colloidal silicon nanocrystals (SiNCs), or silicon quantum dots (SiQDs). This is related to their potential applications in a number of fields such as solar cells, optoelectronic devices and fluorescent bio-labelling agents. The past decade has seen significant progress in the understanding of fundamental physics and surface properties of silicon nanocrystals. Such understanding is based on the advances in the preparation and characterization of surface passivated colloidal silicon nanocrystals. In this critical review, we summarize recent advances in the methods of preparing high quality silicon nanocrystals and strategies for forming self-assembled monolayers (SAMs), with a focus on their bio-applications. We highlight some of the major challenges that remain, as well as lessons learnt when working with silicon nanocrystals (239 references).

  12. Optical and structural properties of ensembles of colloidal Ag{sub 2}S quantum dots in gelatin

    SciTech Connect

    Ovchinnikov, O. V. Smirnov, M. S.; Shapiro, B. I.; Shatskikh, T. S.; Perepelitsa, A. S.; Korolev, N. V.

    2015-03-15

    The size dependences of the absorption and luminescence spectra of ensembles of hydrophilic colloidal Ag{sub 2}S quantum dots produced by the sol-gel method and dispersed in gelatin are analyzed. By X-ray diffraction analysis and transmission electron microscopy, the formation of core/shell nanoparticles is detected. The characteristic feature of the nanoparticles is the formation of crystalline cores, 1.5–2.0 nm in dimensions, and shells of gelatin and its complexes with the components of synthesis. The observed slight size dependence of the position of infrared photoluminescence bands (in the range 1000–1400 nm) in the ensembles of hydrophilic colloidal Ag{sub 2}S quantum dots is explained within the context of the model of the radiative recombination of electrons localized at structural and impurity defects with free holes.

  13. Group velocity dispersion of CdSSe/ZnS core-shell colloidal quantum dots measured with white light interferometry

    NASA Astrophysics Data System (ADS)

    VanEngen Spivey, Amelia G.

    2016-03-01

    We measure the group velocity dispersion coefficient of CdSSe/ZnS core-shell colloidal quantum dots in liquid suspension in the ∼700-900 nm wavelength range using a white-light Michelson interferometer. Two different sizes of dots are investigated. In both cases, the group velocity dispersion coefficient decreases with increasing wavelength above the absorption edge in the dots. For quantum dots in which the linear absorption spectrum shows clear peaks, the absorption characteristics of the dots can be used to accurately model the wavelength-dependence of the group velocity dispersion coefficient.

  14. Synthesis of colloidal InAs/ZnSe quantum dots and their quantum dot sensitized solar cell (QDSSC) application

    NASA Astrophysics Data System (ADS)

    Lee, S. H.; Jung, C.; Jun, Y.; Kim, S.-W.

    2015-11-01

    We report the synthesis of colloidal InAs/ZnSe core/shell quantum dots (QDs) by the hot injection method. InAs nanocrystals have a narrow band gap of 0.38 eV, a high absorption coefficient, and multiple exciton generation; hence, they are promising candidates for application in solar cells. However, poor coverage of the titania layer causes a low solar efficiency of ∼1.74%. We synthesized type-I InAs/ZnSe core/shell QDs as an effective solution; they are expected to have enhanced solar cell efficiency because of the different wettability of the ZnSe shell and their superior stability as compared to that of the unstable InAs core. We characterized the QDs by powder X-ray diffraction, transmission electron microscopy, and absorption and emission spectroscopy. The particle size increased from 2.6 nm to 5 nm, whereas the absorption and emission spectra exhibited a slight red shift, which is typical of type-I structured core/shell QDs. We then fabricated QD-based solar cells and investigated the cell properties, obtaining an open-circuit voltage (VOC) of 0.51 V, a short-circuit current density (JSC) of 12.4 mA/cm2, and a fill factor (FF) of 44%; the efficiency of 2.7% shows an improvement of more than 50% as compared to the values in previous reports.

  15. Description of the fluorescence intensity time trace of collections of CdSe nanocrystal quantum dots based on single quantum dot fluorescence blinking statistics.

    PubMed

    Chung, Inhee; Witkoskie, James B; Cao, Jianshu; Bawendi, Moungi G

    2006-01-01

    This paper analyzes the observed phenomenology of the fluorescence time trace of collections of quantum dots (QDs) in terms of the model parameters that characterize the fluorescence blinking statistics of single QDs. We demonstrate that the non-universal dynamics that appear in fluorescence time traces of collections of QDs at short time scales are related to the universal dynamics that appear at longer time scales. We explore how the extent of time separation between the short and long dynamics affects the transition region and the dynamics at longer time scales. We suggest a methodology to extract single QD statistical model parameters from experimental fluorescence time traces of collections of QDs. We explore theoretical time traces and their experimental analogs for three different cases that span the diverse nonuniversal dynamics that appear at short time scales.

  16. Organic light-emitting diode with an emitter based on a planar layer of CdSe semiconductor nanoplatelets

    NASA Astrophysics Data System (ADS)

    Vashchenko, A. A.; Vitukhnovskii, A. G.; Lebedev, V. S.; Selyukov, A. S.; Vasiliev, R. B.; Sokolikova, M. S.

    2014-09-01

    Colloidal CdSe semiconductor nanoplatelets with characteristic longitudinal sizes of 20-70 nm and thicknesses of several atomic layers are synthesized. The spectra and kinetics of the photoluminescence of these quasi-two-dimensional nanostructures (quantum wells) at room and cryogenic temperatures are investigated. A hybrid light-emitting diode with the electron and hole transport layers based on TAZ and TPD organic compounds, respectively, and the active "emissive" element based on a layer of such single-component nanoplatelets is designed. The spectral and electrical characteristics of the fabricated device, emitting at a wavelength of λ = 515 nm, are determined. The use of quasi-two-dimensional nanostructures of this kind (nanoplatelets) is promising for the fabrication of hybrid light-emitting diodes with pure colors.

  17. Engineering of Doping and Transport for Enhanced Colloidal Quantum Dot Photovoltaics

    NASA Astrophysics Data System (ADS)

    Zhitomirsky, David

    Colloidal Quantum Dots (CQDs) are nanoscale quantum-tuned semiconductor particles suspended in solution. When deployed as optoelectronic materials, CQDs are closely packed together into thin films enabling charge transport. This also enables the formation of semiconductor junctions and contacts with other bulk semiconductor materials and metals, respectively. However, limited attention has been given to understanding the fundamental electronic behavior of these materials as bulk-like films, gaining fine control over their semiconducting properties, and then leveraging these insights to make better semiconductor devices. In this thesis, I explore two of the most fundamental concepts to CQD semiconductor device physics: charge carrier doping density and charge carrier transport. With the aid of optoelectronic simulation, I show that these are the most important paths to pursue in order to improve the photovoltaic device performance. I develop a doping density theory that I then rigorously test for the PbS CQD materials system; this theory is also applicable to other types of CQD materials. I demonstrate doping densities on the order of 10 16 cm-3 to 1018 cm-3 for both p- and n-type films. My work enables a previously unavailable p-n homojunction within one CQD materials system, and furthermore allows to grade the doping within the active absorber layer to reach power conversion efficiencies (PCEs) exceeding 7%. I then study CQD size polydispersity, and use it to investigate the details of charge transport in the rough energetic landscapes inherent to these materials. Here, I find that midgap trap elimination is the most important concept in rapidly obtaining dramatic photovoltaic performance gains. By directly measuring the diffusion length in highly coupled CQD films, and combined with optoelectronic modeling, I was able to develop a new passivation strategy achieving a record 8.5% PCE. My research serves as a roadmap for future performance improvements in CQD

  18. Crystal symmetry breaking and vacancies in colloidal lead chalcogenide quantum dots.

    PubMed

    Bertolotti, Federica; Dirin, Dmitry N; Ibáñez, Maria; Krumeich, Frank; Cervellino, Antonio; Frison, Ruggero; Voznyy, Oleksandr; Sargent, Edward H; Kovalenko, Maksym V; Guagliardi, Antonietta; Masciocchi, Norberto

    2016-09-01

    Size and shape tunability and low-cost solution processability make colloidal lead chalcogenide quantum dots (QDs) an emerging class of building blocks for innovative photovoltaic, thermoelectric and optoelectronic devices. Lead chalcogenide QDs are known to crystallize in the rock-salt structure, although with very different atomic order and stoichiometry in the core and surface regions; however, there exists no convincing prior identification of how extreme downsizing and surface-induced ligand effects influence structural distortion. Using forefront X-ray scattering techniques and density functional theory calculations, here we have identified that, at sizes below 8 nm, PbS and PbSe QDs undergo a lattice distortion with displacement of the Pb sublattice, driven by ligand-induced tensile strain. The resulting permanent electric dipoles may have implications on the oriented attachment of these QDs. Evidence is found for a Pb-deficient core and, in the as-synthesized QDs, for a rhombic dodecahedral shape with nonpolar {110} facets. On varying the nature of the surface ligands, differences in lattice strains are found. PMID:27295101

  19. Photojunction field-effect transistor based on a colloidal quantum dot absorber channel layer.

    PubMed

    Adinolfi, Valerio; Kramer, Illan J; Labelle, André J; Sutherland, Brandon R; Hoogland, S; Sargent, Edward H

    2015-01-27

    The performance of photodetectors is judged via high responsivity, fast speed of response, and low background current. Many previously reported photodetectors based on size-tuned colloidal quantum dots (CQDs) have relied either on photodiodes, which, since they are primary photocarrier devices, lack gain; or photoconductors, which provide gain but at the expense of slow response (due to delayed charge carrier escape from sensitizing centers) and an inherent dark current vs responsivity trade-off. Here we report a photojunction field-effect transistor (photoJFET), which provides gain while breaking prior photoconductors' response/speed/dark current trade-off. This is achieved by ensuring that, in the dark, the channel is fully depleted due to a rectifying junction between a deep-work-function transparent conductive top contact (MoO3) and a moderately n-type CQD film (iodine treated PbS CQDs). We characterize the rectifying behavior of the junction and the linearity of the channel characteristics under illumination, and we observe a 10 μs rise time, a record for a gain-providing, low-dark-current CQD photodetector. We prove, using an analytical model validated using experimental measurements, that for a given response time the device provides a two-orders-of-magnitude improvement in photocurrent-to-dark-current ratio compared to photoconductors. The photoJFET, which relies on a junction gate-effect, enriches the growing family of CQD photosensitive transistors. PMID:25558809

  20. Crystal symmetry breaking and vacancies in colloidal lead chalcogenide quantum dots

    NASA Astrophysics Data System (ADS)

    Bertolotti, Federica; Dirin, Dmitry N.; Ibáñez, Maria; Krumeich, Frank; Cervellino, Antonio; Frison, Ruggero; Voznyy, Oleksandr; Sargent, Edward H.; Kovalenko, Maksym V.; Guagliardi, Antonietta; Masciocchi, Norberto

    2016-09-01

    Size and shape tunability and low-cost solution processability make colloidal lead chalcogenide quantum dots (QDs) an emerging class of building blocks for innovative photovoltaic, thermoelectric and optoelectronic devices. Lead chalcogenide QDs are known to crystallize in the rock-salt structure, although with very different atomic order and stoichiometry in the core and surface regions; however, there exists no convincing prior identification of how extreme downsizing and surface-induced ligand effects influence structural distortion. Using forefront X-ray scattering techniques and density functional theory calculations, here we have identified that, at sizes below 8 nm, PbS and PbSe QDs undergo a lattice distortion with displacement of the Pb sublattice, driven by ligand-induced tensile strain. The resulting permanent electric dipoles may have implications on the oriented attachment of these QDs. Evidence is found for a Pb-deficient core and, in the as-synthesized QDs, for a rhombic dodecahedral shape with nonpolar {110} facets. On varying the nature of the surface ligands, differences in lattice strains are found.

  1. High performance PbSe colloidal quantum dot vertical field effect phototransistors.

    PubMed

    Zhang, Haiting; Zhang, Yating; Song, Xiaoxian; Yu, Yu; Cao, Mingxuan; Che, Yongli; Wang, Jianlong; Yang, Junbo; Dai, Haitao; Zhang, Guizhong; Yao, Jianquan

    2016-10-21

    Here, vertical field effect phototransistors (VFEPTs) based on lead selenide colloidal quantum dots (PbSe CQDs) for infrared photo detection were investigated, using Au/Ag nanowires as the source transparent electrode. VFEPTs have the advantage of easy fabrication of ultrashort channel length devices, as the channel length is simply determined here by the PbSe CQDs active layer's thickness (260 nm). In ultrashort channels, photo-excited carriers quickly (in nanoseconds) transfer to the drain. As soon as a hole (electron) reaches the drain, a hole (electron) is replenished from the source. Accordingly, multiple holes circulate in the ultrashort channel following a single electron-hole photo generation. As a result, the device exhibits superior photoconductive properties over the lateral structure. PbSe CQD VFEPTs show ambipolar operation under low voltage down to one volt at room temperature. Moreover, high photo responsivity and high specific detectivity of 2 × 10(4) A W(-1) and 7 × 10(12) Jones are also achieved in the devices under 808 nm laser illumination. The transparent electrode-based near infrared VFEPTs prepared through this self-assembly solution process show promise for applications in electronics and photoelectronics. PMID:27623533

  2. Carrier dynamics in colloidal indium arsenide quantum dots in the weak excitation limit

    NASA Astrophysics Data System (ADS)

    Spencer, Austin; Peters, William; Tiwari, Vivek; Cho, Byungmoon; Neale, Nathan; Jonas, David

    2014-03-01

    The dynamics of photo-excited carriers in colloidal indium arsenide (InAs) quantum dots are characterized by degenerate pump-probe spectroscopy at 1.5 times the band gap. This material is of particular interest due to reports of efficient multiple exciton generation and its potential application in third-generation photovoltaic devices. Use of a sample renewal technique based on laser beam scanning enables long resampling times (>0.5 s) with minimal spatial overlap between successive laser shots thereby minimizing repetitive excitation. Pump-probe transients at a range of excitation probabilities are reported, from 2.6%, where signal from biexcitons is small (1.9%), to 36%, where the biexcitons contribute 45% of the signal. These transients are well described by a tri-exponential fit which includes time constants of approximately 1 ps, 16 ps, and 750 ps tentatively attributed to carrier cooling, multi-exciton recombination, and single exciton recombination respectively. By an excitation probability of 10%, biexciton dynamics are detectable and continue to grow in magnitude as the excitation probability increases. The pump power dependence of the signal at 20 ps, which deviates from linearity at an excitation probability of 10%, reflects biexciton recombination.

  3. High performance PbSe colloidal quantum dot vertical field effect phototransistors

    NASA Astrophysics Data System (ADS)

    Zhang, Haiting; Zhang, Yating; Song, Xiaoxian; Yu, Yu; Cao, Mingxuan; Che, Yongli; Wang, Jianlong; Yang, Junbo; Dai, Haitao; Zhang, Guizhong; Yao, Jianquan

    2016-10-01

    Here, vertical field effect phototransistors (VFEPTs) based on lead selenide colloidal quantum dots (PbSe CQDs) for infrared photo detection were investigated, using Au/Ag nanowires as the source transparent electrode. VFEPTs have the advantage of easy fabrication of ultrashort channel length devices, as the channel length is simply determined here by the PbSe CQDs active layer’s thickness (260 nm). In ultrashort channels, photo-excited carriers quickly (in nanoseconds) transfer to the drain. As soon as a hole (electron) reaches the drain, a hole (electron) is replenished from the source. Accordingly, multiple holes circulate in the ultrashort channel following a single electron-hole photo generation. As a result, the device exhibits superior photoconductive properties over the lateral structure. PbSe CQD VFEPTs show ambipolar operation under low voltage down to one volt at room temperature. Moreover, high photo responsivity and high specific detectivity of 2 × 104 A W-1 and 7 × 1012 Jones are also achieved in the devices under 808 nm laser illumination. The transparent electrode-based near infrared VFEPTs prepared through this self-assembly solution process show promise for applications in electronics and photoelectronics.

  4. Temperature and magnetic-field dependence of radiative decay in colloidal germanium quantum dots.

    PubMed

    Robel, István; Shabaev, Andrew; Lee, Doh C; Schaller, Richard D; Pietryga, Jeffrey M; Crooker, Scott A; L Efros, Alexander; Klimov, Victor I

    2015-04-01

    We conduct spectroscopic and theoretical studies of photoluminescence (PL) from Ge quantum dots (QDs) fabricated via colloidal synthesis. The dynamics of late-time PL exhibit a pronounced dependence on temperature and applied magnetic field, which can be explained by radiative decay involving two closely spaced, slowly emitting exciton states. In 3.5 nm QDs, these states are separated by ∼1 meV and are characterized by ∼82 μs and ∼18 μs lifetimes. By using a four-band formalism, we calculate the fine structure of the indirect band-edge exciton arising from the electron-hole exchange interaction and the Coulomb interaction of the Γ-point hole with the anisotropic charge density of the L-point electron. The calculations suggest that the observed PL dynamics can be explained by phonon-assisted recombination of excitons thermally distributed between the lower-energy "dark" state with the momentum projection J = ± 2 and a higher energy "bright" state with J = ± 1. A fairly small difference between lifetimes of these states is due to their mixing induced by the exchange term unique to crystals with a highly symmetric cubic lattice such as Ge.

  5. Crystal symmetry breaking and vacancies in colloidal lead chalcogenide quantum dots.

    PubMed

    Bertolotti, Federica; Dirin, Dmitry N; Ibáñez, Maria; Krumeich, Frank; Cervellino, Antonio; Frison, Ruggero; Voznyy, Oleksandr; Sargent, Edward H; Kovalenko, Maksym V; Guagliardi, Antonietta; Masciocchi, Norberto

    2016-09-01

    Size and shape tunability and low-cost solution processability make colloidal lead chalcogenide quantum dots (QDs) an emerging class of building blocks for innovative photovoltaic, thermoelectric and optoelectronic devices. Lead chalcogenide QDs are known to crystallize in the rock-salt structure, although with very different atomic order and stoichiometry in the core and surface regions; however, there exists no convincing prior identification of how extreme downsizing and surface-induced ligand effects influence structural distortion. Using forefront X-ray scattering techniques and density functional theory calculations, here we have identified that, at sizes below 8 nm, PbS and PbSe QDs undergo a lattice distortion with displacement of the Pb sublattice, driven by ligand-induced tensile strain. The resulting permanent electric dipoles may have implications on the oriented attachment of these QDs. Evidence is found for a Pb-deficient core and, in the as-synthesized QDs, for a rhombic dodecahedral shape with nonpolar {110} facets. On varying the nature of the surface ligands, differences in lattice strains are found.

  6. Saturation behaviour of colloidal PbSe quantum dot exciton emission coupled into silicon photonic circuits.

    PubMed

    Foell, Charles A; Schelew, Ellen; Qiao, Haijun; Abel, Keith A; Hughes, Stephen; van Veggel, Frank C J M; Young, Jeff F

    2012-05-01

    We report coupling of the excitonic photon emission from photoexcited PbSe colloidal quantum dots (QDs) into an optical circuit that was fabricated in a silicon-on-insulator wafer using a CMOS-compatible process. The coupling between excitons and sub-μm sized silicon channel waveguides was mediated by a photonic crystal microcavity. The intensity of the coupled light saturates rapidly with the optical excitation power. The saturation behaviour was quantitatively studied using an isolated photonic crystal cavity with PbSe QDs site-selectively located at the cavity mode antinode position. Saturation occurs when a few μW of continuous wave HeNe pump power excites the QDs with a Gaussian spot size of 2 μm. By comparing the results with a master equation analysis that rigorously accounts for the complex dielectric environment of the QD excitons, the saturation is attributed to ground state depletion due to a non-radiative exciton decay channel with a trap state lifetime ~ 3 μs.

  7. The Influence of Doping on the Optoelectronic Properties of PbS Colloidal Quantum Dot Solids

    PubMed Central

    Papagiorgis, P.; Stavrinadis, A.; Othonos, A.; Konstantatos, G.; Itskos, G.

    2016-01-01

    We report on an extensive spectroscopic investigation of the impact of substitutional doping on the optoelectronic properties of PbS colloidal quantum dot (CQD) solids. N-doping is provided by Bi incorporation during CQD synthesis as well as post-synthetically via cation exchange reactions. The spectroscopic data indicate a systematic quenching of the excitonic absorption and luminescence and the appearance of two dopant-induced contributions at lower energies to the CQD free exciton. Temperature-dependent photoluminescence indicates the presence of temperature-activated detrapping and trapping processes of photoexcitations for the films doped during and after synthesis, respectively. The data are consistent with a preferential incorporation of the dopants at the QDs surface in the case of the cation-exchange treated films versus a more uniform doping profile in the case of in-situ Bi incorporation during synthesis. Time-resolved experiments indicate the presence of fast dopant- and excitation-dependent recombination channels attributed to Auger recombination of negatively charged excitons, formed due to excess of dopant electrons. The data indicate that apart from dopant compensation and filling of dopant induced trap states, a fraction of the Bi ionized electrons feeds the QD core states resulting in n-doping of the semiconductor, confirming reported work on devices based on such doped CQD material. PMID:26743934

  8. Enhanced trion emission from colloidal quantum dots with photonic crystals by two-photon excitation

    NASA Astrophysics Data System (ADS)

    Xu, Xingsheng

    2013-11-01

    For colloidal quantum dots, the ongoing biggest problem is their fluorescence blinking. Until now, there is no generally accepted model for this fluorescence blinking. Here, two-photon excited fluorescence from CdSe/ZnS nanocrystals on silicon nitride photonic crystals is studied using a femtosecond laser. From analysis of the spectra and decay processes, most of the relative trion efficiency is larger than 10%, and the largest relative trion efficiency reaches 46.7%. The photonic crystals enhance the trion emission of CdSe/ZnS nanocrystals, where the enhancement is due to the coupling of the trion emission to the leaky mode of the photonic crystal slab. Moreover, the photonic crystals enhance the Auger-assisted trapping efficiency of electrons/holes to surface states, and then enhance the efficiency of the generations of charge separation and DC electric field, which modifies the trion spectrum. Therefore, a model is present for explaining the mechanism of fluorescence blinking including the effect of the environment.

  9. Energy Gap Tuning and Carrier Dynamics in Colloidal Ge1-xSnx Quantum Dots.

    PubMed

    Hafiz, Shopan A; Esteves, Richard J Alan; Demchenko, Denis O; Arachchige, Indika U; Özgür, Ümit

    2016-09-01

    Optical transition energies and carrier dynamics in colloidally synthesized 2.0 ± 0.8 nm Ge1-xSnx quantum dots (x = 0.055-0.236) having visible luminescence were investigated using steady-state and time-resolved photoluminescence (PL) spectroscopy supported by first-principles calculations. By changing Sn content from x = 0.055 to 0.236, experimentally determined HOMO-LUMO gap at 15 K was tuned from 1.88 to 1.61 eV. Considering the size and compositional variations, these values were consistent with theoretically calculated ones. At 15 K, time-resolved PL revealed slow decay of luminescence (3-27 μs), likely due to the recombination of spin-forbidden dark excitons and recombination of carriers trapped at surface states. Increasing Sn concentration to 23.6% led to 1 order of magnitude faster recombination. At 295 K, PL decays were 3 orders of magnitude faster (9-28 ns) owing to the thermal activation of bright excitons and carrier detrapping from surface states. PMID:27513723

  10. Saturation behaviour of colloidal PbSe quantum dot exciton emission coupled into silicon photonic circuits.

    PubMed

    Foell, Charles A; Schelew, Ellen; Qiao, Haijun; Abel, Keith A; Hughes, Stephen; van Veggel, Frank C J M; Young, Jeff F

    2012-05-01

    We report coupling of the excitonic photon emission from photoexcited PbSe colloidal quantum dots (QDs) into an optical circuit that was fabricated in a silicon-on-insulator wafer using a CMOS-compatible process. The coupling between excitons and sub-μm sized silicon channel waveguides was mediated by a photonic crystal microcavity. The intensity of the coupled light saturates rapidly with the optical excitation power. The saturation behaviour was quantitatively studied using an isolated photonic crystal cavity with PbSe QDs site-selectively located at the cavity mode antinode position. Saturation occurs when a few μW of continuous wave HeNe pump power excites the QDs with a Gaussian spot size of 2 μm. By comparing the results with a master equation analysis that rigorously accounts for the complex dielectric environment of the QD excitons, the saturation is attributed to ground state depletion due to a non-radiative exciton decay channel with a trap state lifetime ~ 3 μs. PMID:22565670

  11. High performance PbSe colloidal quantum dot vertical field effect phototransistors.

    PubMed

    Zhang, Haiting; Zhang, Yating; Song, Xiaoxian; Yu, Yu; Cao, Mingxuan; Che, Yongli; Wang, Jianlong; Yang, Junbo; Dai, Haitao; Zhang, Guizhong; Yao, Jianquan

    2016-10-21

    Here, vertical field effect phototransistors (VFEPTs) based on lead selenide colloidal quantum dots (PbSe CQDs) for infrared photo detection were investigated, using Au/Ag nanowires as the source transparent electrode. VFEPTs have the advantage of easy fabrication of ultrashort channel length devices, as the channel length is simply determined here by the PbSe CQDs active layer's thickness (260 nm). In ultrashort channels, photo-excited carriers quickly (in nanoseconds) transfer to the drain. As soon as a hole (electron) reaches the drain, a hole (electron) is replenished from the source. Accordingly, multiple holes circulate in the ultrashort channel following a single electron-hole photo generation. As a result, the device exhibits superior photoconductive properties over the lateral structure. PbSe CQD VFEPTs show ambipolar operation under low voltage down to one volt at room temperature. Moreover, high photo responsivity and high specific detectivity of 2 × 10(4) A W(-1) and 7 × 10(12) Jones are also achieved in the devices under 808 nm laser illumination. The transparent electrode-based near infrared VFEPTs prepared through this self-assembly solution process show promise for applications in electronics and photoelectronics.

  12. High-Power Genuine Ultraviolet Light-Emitting Diodes Based On Colloidal Nanocrystal Quantum Dots.

    PubMed

    Kwak, Jeonghun; Lim, Jaehoon; Park, Myeongjin; Lee, Seonghoon; Char, Kookheon; Lee, Changhee

    2015-06-10

    Thin-film ultraviolet (UV) light-emitting diodes (LEDs) with emission wavelengths below 400 nm are emerging as promising light sources for various purposes, from our daily lives to industrial applications. However, current thin-film UV-emitting devices radiate not only UV light but also visible light. Here, we introduce genuine UV-emitting colloidal nanocrystal quantum dot (NQD) LEDs (QLEDs) using precisely controlled NQDs consisting of a 2.5-nm-sized CdZnS ternary core and a ZnS shell. The effective core size is further reduced during the shell growth via the atomic diffusion of interior Cd atoms to the exterior ZnS shell, compensating for the photoluminescence red shift. This design enables us to develop CdZnS@ZnS UV QLEDs with pure UV emission and minimal parasitic peaks. The irradiance is as high as 2.0-13.9 mW cm(-2) at the peak wavelengths of 377-390 nm, several orders of magnitude higher than that of other thin-film UV LEDs.

  13. Colloidal atomic layer deposition (c-ALD) using self-limiting reactions at nanocrystal surface coupled to phase transfer between polar and nonpolar media.

    PubMed

    Ithurria, Sandrine; Talapin, Dmitri V

    2012-11-14

    Atomic layer deposition (ALD) is widely used for gas-phase deposition of high-quality dielectric, semiconducting, or metallic films on various substrates. In this contribution we propose the concept of colloidal ALD (c-ALD) for synthesis of colloidal nanostructures. During the c-ALD process, either nanoparticles or molecular precursors are sequentially transferred between polar and nonpolar phases to prevent accumulation of unreacted precursors and byproducts in the reaction mixture. We show that binding of inorganic ligands (e.g., S(2-)) to the nanocrystal surface can be used as a half-reaction in c-ALD process. The utility of this approach has been demonstrated by growing CdS layers on colloidal CdSe nanocrystals, nanoplatelets, and CdS nanorods. The CdS/CdSe/CdS nanoplatelets represent a new example of colloidal nanoheterostructures with mixed confinement regimes for electrons and holes. In these materials holes are confined to a thin (∼1.8 nm) two-dimensional CdSe quantum well, while the electron confinement can be gradually relaxed in all three dimensions by growing epitaxial CdS layers on both sides of the quantum well. The relaxation of the electron confinement energy caused a shift of the emission band from 510 to 665 nm with unusually small inhomogeneous broadening of the emission spectra.

  14. Sensitive and selective determining ascorbic acid and activity of alkaline phosphatase based on electrochemiluminescence of dual-stabilizers-capped CdSe quantum dots in carbon nanotube-nafion composite.

    PubMed

    Ma, Xiaolong; Zhang, Xin; Guo, Xinli; Kang, Qi; Shen, Dazhong; Zou, Guizheng

    2016-07-01

    Sensitive and selective determining bio-related molecule and enzyme play an important role in designing novel procedure for biological sensing and clinical diagnosis. Herein, we found that dual-stabilizers-capped CdSe quantum dots (QDs) in composite film of multi-walled carbon nanotubes (CNTs) and Nafion, displaying eye-visible monochromatic electrochemiluminescence (ECL) with fwhm of 37nm, which offers promising ECL signal for detecting ascorbic acid (AA) as well as the activity of alkaline phosphatase (ALP) in biological samples. It was also shown that the dual-stabilizers-capped CdSe QDs can preserve their highly passivated surface states with prolonged lifetime of excited states in Nafion mixtures, and facilitate electron-transfer ability of Nafion film along with CNTs. Compared with the QDs/GCE, the ECL intensity is enhanced 1.8 times and triggering potential shifted to lower energy by 0.12V on the CdSe-CNTs-Nafion/GCE. The ECL quenching degree increases with increasing concentration of AA in the range of 0.01-30nM with a limit of detection (LOD) of 5pM. The activity of ALP was determined indirectly according to the concentration of AA, generated in the hydrolysis reaction of l-ascorbic acid 2-phosphate sesquimagnesium (AA-P) in the presence of ALP as a catalyst, with an LOD of 1μU/L. The proposed strategy is favorable for developing simple ECL sensor or device with high sensitivity, spectral resolution and less electrochemical interference. PMID:27154663

  15. The use of bulk states to accelerate the band edge statecalculation of a semiconductor quantum dot

    SciTech Connect

    Vomel, Christof; Tomov, Stanimire Z.; Wang, Lin-Wang; Marques,Osni A.; Dongarra, Jack J.

    2006-05-10

    We present a new technique to accelerate the convergence of the folded spectrum method in empirical pseudopotential band edge state calculations for colloidal quantum dots. We use bulk band states of the materials constituent of the quantum dot to construct initial vectors and a preconditioner. We apply these to accelerate the convergence of the folded spectrum method for the interior states at the top of the valence and the bottom of the conduction band. For large CdSe quantum dots, the number of iteration steps until convergence decreases by about a factor of 4 compared to previous calculations.

  16. Flower-like CdSe ultrathin nanosheet assemblies for enhanced visible-light-driven photocatalytic H2 production.

    PubMed

    Peng, Yong; Shang, Lu; Bian, Tong; Zhao, Yufei; Zhou, Chao; Yu, Huijun; Wu, Li-Zhu; Tung, Chen-Ho; Zhang, Tierui

    2015-03-18

    Flower-like CdSe architectures composed of ultrathin nanosheets were prepared via a facile solvothermal method. A relationship was established between the solvothermal temperature and the product structure, and thus the photocatalytic activity. When compared with well-studied CdSe quantum dots, the ultrathin nanosheet assemblies exhibited a better photocatalytic H2 evolution activity under visible light irradiation.

  17. Probing the structural dependency of photoinduced properties of colloidal quantum dots using metal-oxide photo-active substrates

    SciTech Connect

    Patty, Kira; Campbell, Quinn; Hamilton, Nathan; West, Robert G.; Sadeghi, Seyed M.; Mao, Chuanbin

    2014-09-21

    We used photoactive substrates consisting of about 1 nm coating of a metal oxide on glass substrates to investigate the impact of the structures of colloidal quantum dots on their photophysical and photochemical properties. We showed during irradiation these substrates can interact uniquely with such quantum dots, inducing distinct forms of photo-induced processes when they have different cores, shells, or ligands. In particular, our results showed that for certain types of core-shell quantum dot structures an ultrathin layer of a metal oxide can reduce suppression of quantum efficiency of the quantum dots happening when they undergo extensive photo-oxidation. This suggests the possibility of shrinking the sizes of quantum dots without significant enhancement of their non-radiative decay rates. We show that such quantum dots are not influenced significantly by Coulomb blockade or photoionization, while those without a shell can undergo a large amount of photo-induced fluorescence enhancement via such blockade when they are in touch with the metal oxide.

  18. An easy shortcut synthesis of size-controlled bismuth nanoparticles and their use in the SLS growth of high-quality colloidal cadmium selenide quantum wires.

    PubMed

    Wang, Fudong; Buhro, William E

    2010-02-22

    An easy shortcut synthesis of thermally stable, near-monodisperse Bi nanoparticles from BiCl(3) and Na[N(SiMe(3))(2)] is described. The diameters of the Bi nanoparticles are controlled in the range of 4-29 nm by varying the amounts of BiCl(3) and Na[N(SiMe(3))(2)] employed. Standard deviations in their diameter distributions are 5-15% of the mean diameters, consistent with near monodispersity. These Bi nanoparticles are shown to be the best currently available catalysts for the solution-liquid-solid (SLS) growth of high-quality CdSe quantum wires.

  19. Origins of photoluminescence decay kinetics in CdTe colloidal quantum dots.

    PubMed

    Califano, Marco

    2015-03-24

    Recent experimental studies have identified at least two nonradiative components in the fluorescence decay of solutions of CdTe colloidal quantum dots (CQDs). The lifetimes reported by different groups, however, differed by orders of magnitude, raising the question of whether different types of traps were at play in the different samples and experimental conditions and even whether different types of charge carriers were involved in the different trapping processes. Considering that the use of these nanomaterials in biology, optoelectronics, photonics, and photovoltaics is becoming widespread, such a gap in our understanding of carrier dynamics in these systems needs addressing. This is what we do here. Using the state-of-the-art atomistic semiempirical pseudopotential method, we calculate trapping times and nonradiative population decay curves for different CQD sizes considering up to 268 surface traps. We show that the seemingly discrepant experimental results are consistent with the trapping of the hole at unsaturated Te bonds on the dot surface in the presence of different dielectric environments. In particular, the observed increase in the trapping times following air exposure is attributed to the formation of an oxide shell on the dot surface, which increases the dielectric constant of the dot environment. Two types of traps are identified, depending on whether the unsaturated bond is single (type I) or part of a pair of dangling bonds on the same Te atom (type II). The energy landscape relative to transitions to these traps is found to be markedly different in the two cases. As a consequence, the trapping times associated with the different types of traps exhibit a strikingly contrasting sensitivity to variations in the dot environment. Based on these characteristics, we predict the presence of a sub-nanosecond component in all photoluminescence decay curves of CdTe CQDs in the size range considered here if both trap types are present. The absence of such a

  20. Microscopic theory of the optical properties of colloidal graphene quantum dots

    NASA Astrophysics Data System (ADS)

    Ozfidan, Isil; Korkusinski, Marek; Güçlü, A. Devrim; McGuire, John A.; Hawrylak, Pawel

    2014-02-01

    We present a microscopic theory of electronic and optical properties of colloidal graphene quantum dots (CGQDs). The single-particle properties are described in the tight-binding model based on the pz carbon orbitals. Electron-electron screened Coulomb direct, exchange, and scattering matrix elements are calculated using Slater pz orbitals. The many-body ground state and excited states are constructed as a linear combination of a finite number of excitations from the Hartree-Fock (HF) ground state (GS) by exact diagonalization techniques. HF ground states corresponding to semiconductor, Mott-insulator, and spin-polarized phases are obtained as a function of the strength of the screened interaction versus the tunneling matrix element. In the semiconducting phase of a triangular CGQD, the top of the valence band and the bottom of the conduction band are found to be degenerate due to rotational symmetry. The singlet and triplet exciton spectra from the HF GS are obtained by solving the Bethe-Salpeter equation. The low-energy exciton spectrum is predicted to consist of two bright-singlet exciton states corresponding to two circular polarizations of light and a lower-energy band of two dark singlets and 12 dark triplets. The robustness of the bright degenerate singlet pair against correlations in the many-body state is demonstrated as well as the breaking of the degeneracy by the lowering of symmetry of the CGQD. The band-gap renormalization, electron-hole attraction, fine structure, oscillator strength, and polarization of the exciton are analyzed as a function of the size, shape, screening, and symmetry of the CGQD. The theoretical results are compared with experimental absorption spectra.

  1. Highly efficient large-area colourless luminescent solar concentrators using heavy-metal-free colloidal quantum dots

    NASA Astrophysics Data System (ADS)

    Meinardi, Francesco; McDaniel, Hunter; Carulli, Francesco; Colombo, Annalisa; Velizhanin, Kirill A.; Makarov, Nikolay S.; Simonutti, Roberto; Klimov, Victor I.; Brovelli, Sergio

    2015-10-01

    Luminescent solar concentrators serving as semitransparent photovoltaic windows could become an important element in net zero energy consumption buildings of the future. Colloidal quantum dots are promising materials for luminescent solar concentrators as they can be engineered to provide the large Stokes shift necessary for suppressing reabsorption losses in large-area devices. Existing Stokes-shift-engineered quantum dots allow for only partial coverage of the solar spectrum, which limits their light-harvesting ability and leads to colouring of the luminescent solar concentrators, complicating their use in architecture. Here, we use quantum dots of ternary I-III-VI2 semiconductors to realize the first large-area quantum dot-luminescent solar concentrators free of toxic elements, with reduced reabsorption and extended coverage of the solar spectrum. By incorporating CuInSexS2-x quantum dots into photo-polymerized poly(lauryl methacrylate), we obtain freestanding, colourless slabs that introduce no distortion to perceived colours and are thus well suited for the realization of photovoltaic windows. Thanks to the suppressed reabsorption and high emission efficiencies of the quantum dots, we achieve an optical power efficiency of 3.2%. Ultrafast spectroscopy studies suggest that the Stokes-shifted emission involves a conduction-band electron and a hole residing in an intragap state associated with a native defect.

  2. Highly efficient large-area colourless luminescent solar concentrators using heavy-metal-free colloidal quantum dots.

    PubMed

    Meinardi, Francesco; McDaniel, Hunter; Carulli, Francesco; Colombo, Annalisa; Velizhanin, Kirill A; Makarov, Nikolay S; Simonutti, Roberto; Klimov, Victor I; Brovelli, Sergio

    2015-10-01

    Luminescent solar concentrators serving as semitransparent photovoltaic windows could become an important element in net zero energy consumption buildings of the future. Colloidal quantum dots are promising materials for luminescent solar concentrators as they can be engineered to provide the large Stokes shift necessary for suppressing reabsorption losses in large-area devices. Existing Stokes-shift-engineered quantum dots allow for only partial coverage of the solar spectrum, which limits their light-harvesting ability and leads to colouring of the luminescent solar concentrators, complicating their use in architecture. Here, we use quantum dots of ternary I-III-VI2 semiconductors to realize the first large-area quantum dot-luminescent solar concentrators free of toxic elements, with reduced reabsorption and extended coverage of the solar spectrum. By incorporating CuInSexS2-x quantum dots into photo-polymerized poly(lauryl methacrylate), we obtain freestanding, colourless slabs that introduce no distortion to perceived colours and are thus well suited for the realization of photovoltaic windows. Thanks to the suppressed reabsorption and high emission efficiencies of the quantum dots, we achieve an optical power efficiency of 3.2%. Ultrafast spectroscopy studies suggest that the Stokes-shifted emission involves a conduction-band electron and a hole residing in an intragap state associated with a native defect. PMID:26301902

  3. Optical systems modeling and experimental realization of pump and probe technique: investigation of nonlinear absorption in colloidal quantum dots

    NASA Astrophysics Data System (ADS)

    Smirnov, A.; Golinskaya, A.; Ezhova, K.; Kozlova, M.; Dneprovskii, V.

    2016-04-01

    Two optical systems modeling of laser and broadband radiation focusing, that is necessary for realization of the pump and probe method, was carried out in this work. Modeling was utilized to construct experimental setup for transmission spectra measuring of studied sample by probe nanosecond broadband radiation (coumarin photoluminescence) depending on the intensity of the nanosecond laser pump pulses. The saturation effect of absorption and the induced charge Stark-effect coexistence and predominate issue of these effects are determined by power of optical excitation. In dependence of tuning of excitation radiation frequency from basic exciton transition frequency nonlinear effects in colloidal CdSe/ZnS quantum dots has been investigated.

  4. Efficient, air-stable colloidal quantum dot solar cells encapsulated using atomic layer deposition of a nanolaminate barrier

    SciTech Connect

    Ip, Alexander H.; Labelle, André J.; Sargent, Edward H.

    2013-12-23

    Atomic layer deposition was used to encapsulate colloidal quantum dot solar cells. A nanolaminate layer consisting of alternating alumina and zirconia films provided a robust gas permeation barrier which prevented device performance degradation over a period of multiple weeks. Unencapsulated cells stored in ambient and nitrogen environments demonstrated significant performance losses over the same period. The encapsulated cell also exhibited stable performance under constant simulated solar illumination without filtration of harsh ultraviolet photons. This monolithically integrated thin film encapsulation method is promising for roll-to-roll processed high efficiency nanocrystal solar cells.

  5. Suppression of dark current through barrier engineer for solution-processed colloidal quantum-dots infrared photodetectors

    SciTech Connect

    Jiang, Zhenyu E-mail: jianxu@engr.psu.edu; Liu, Yan; Mo, Chen; Wang, Li; Atalla, Mahmoud R. M.; Liu, Jie; Kurhade, Kandhar K.; Xu, Jian E-mail: jianxu@engr.psu.edu; Hu, Wenjia; Zhang, Wenjun; You, Guanjun; Zhang, Yu

    2015-08-31

    In an attempt to suppress the dark current, the barrier layer engineer for solution-processed PbSe colloidal quantum-dot (CQD) photodetectors has been investigated in the present study. It was found that the dark current can be significantly suppressed by implementing two types of carrier blocking layers, namely, hole blocking layer and electron blocking layer, sandwiched in between two active PbSe CQD layers. Meanwhile no adverse impact has been observed for the photo current. Our study suggests that this improvement resides on the transport pathway created via carrier recombination at intermediate layer, which provides wide implications for the suppression of dark current for infrared photodetectors.

  6. Toxicity of CdSe Nanoparticles in Caco-2 Cell Cultures

    PubMed Central

    Wang, Lin; Nagesha, Dattatri K; Selvarasah, Selvapraba; Dokmeci, Mehmet R; Carrier, Rebecca L

    2008-01-01

    Background Potential routes of nanomaterial exposure include inhalation, dermal contact, and ingestion. Toxicology of inhalation of ultra-fine particles has been extensively studied; however, risks of nanomaterial exposure via ingestion are currently almost unknown. Using enterocyte-like Caco-2 cells as a small intestine epithelial model, the possible toxicity of CdSe quantum dot (QD) exposure via ingestion was investigated. Effect of simulated gastric fluid treatment on CdSe QD cytotoxicity was also studied. Results Commercially available CdSe QDs, which have a ZnS shell and poly-ethylene glycol (PEG) coating, and in-house prepared surfactant coated CdSe QDs were dosed to Caco-2 cells. Cell viability and attachment were studied after 24 hours of incubation. It was found that cytotoxicity of CdSe QDs was modulated by surface coating, as PEG coated CdSe QDs had less of an effect on Caco-2 cell viability and attachment. Acid treatment increased the toxicity of PEG coated QDs, most likely due to damage or removal of the surface coating and exposure of CdSe core material. Incubation with un-dialyzed in-house prepared CdSe QD preparations, which contained an excess amount of free Cd2+, resulted in dramatically reduced cell viability. Conclusion Exposure to CdSe QDs resulted in cultured intestinal cell detachment and death; cytotoxicity depended largely, however, on the QD coating and treatment (e.g. acid treatment, dialysis). Experimental results generally indicated that Caco-2 cell viability correlated with concentration of free Cd2+ ions present in cell culture medium. Exposure to low (gastric) pH affected cytotoxicity of CdSe QDs, indicating that route of exposure may be an important factor in QD cytotoxicity. PMID:18947410

  7. Efficient cw lasing in a Cr{sup 2+}:CdSe crystal

    SciTech Connect

    Akimov, V A; Kozlovskii, V I; Korostelin, Yu V; Landman, A I; Podmar'kov, Yu P; Skasyrsky, Ya K; Frolov, M P

    2007-11-30

    Continuous wave lasing in a Cr{sup 2+}:CdSe crystal is obtained for the first time. The Cr{sup 2+}:CdSe crystal pumped by a 1.908-{mu}m thulium fibre laser generated 1.07 W at 2.623 {mu}m with the quantum slope efficiency with respect to the absorbed power equal to 60%. (letters)

  8. Purification non-aqueous solution of quantum dots CdSe- CdS-ZnS from excess organic substance-stabilizer by use PE- HD membrane

    NASA Astrophysics Data System (ADS)

    Kosolapova, K.; Al-Alwani, A.; Gorbachev, I.; Glukhovskoy, E.

    2015-11-01

    Recently, a new simple method for the purification of CdSe-CdS-ZnS quantum dots by using membrane filtration, the filtration process, successfully separated the oleic acid from quantum dots through membranes purification after synthesis; purification of quantum dots is a very significant part of post synthetical treatment that determines the properties of the material. We explore the possibilities of the Langmuir-Blodgett technique to make such layers, using quantum dots as a model system. The Langmuir monolayer of quantum dots were then investigated the surface pressure-area isotherm. From isotherm, we found the surface pressure monolayer changed with time.

  9. Uniform Thin Films of CdSe and CdSe(ZnS) Core(shell) Quantum Dots by Sol-Gel Assembly: Enabling Photoelectrochemical Characterization and Electronic Applications

    PubMed Central

    Korala, Lasantha; Wang, Zhijie; Liu, Yi; Maldonado, Stephen; Brock, Stephanie L.

    2013-01-01

    Optoelectronic properties of quantum dot (QD) films are limited by (1) poor interfacial chemistry and (2) non-radiative recombination due to surface traps. To address these performance issues, sol-gel methods are applied to fabricate thin films of CdSe and core(shell) CdSe(ZnS) QDs. High-angle annular dark-field scanning transmission electron microscopy (HAADF-STEM) imaging with chemical analysis confirms that the surface of the QDs in the sol-gel thin films are chalcogen-rich, consistent with an oxidative-induced gelation mechanism in which connectivity is achieved by formation of dichalcogenide covalent linkages between particles. The ligand removal and assembly process is probed by thermogravimetric, spectroscopic and microscopic studies. Further enhancement of inter-particle coupling via mild thermal annealing, which removes residual ligands and reinforces QD connectivity, results in QD sol-gel thin films with superior charge transport properties, as shown by a dramatic enhancement of electrochemical photocurrent under white light illumination relative to thin films composed of ligand-capped QDs. A more than 2-fold enhancement in photocurrent, and a further increase in photovoltage can be achieved by passivation of surface defects via overcoating with a thin ZnS shell. The ability to tune interfacial and surface characteristics for the optimization of photophysical properties suggests that the sol-gel approach may enable formation of QD thin films suitable for a range of optoelectronic applications. PMID:23350924

  10. Use of colloidal quantum dots as a digitally switched swept light source for gold nanoparticle based hyperspectral microscopy

    PubMed Central

    Hoshino, Kazunori; Joshi, Pratixa. P.; Bhave, Gauri.; Sokolov, Konstantin V.; Zhang, Xiaojing

    2014-01-01

    We propose a method to utilize colloidal quantum dots (QDs) as a swept light source for hyperspectral microscopy. The use of QD allows for uniform multicolor emission which covers visible-NIR wavelengths. We used 8 colors of CdSe/ZnS and CdTe/ZnS colloidal quantum dots with the peak emission wavelengths from 520 nm to 800 nm. The QDs are packed in a compact enclosure, composing a low-cost, solid-state swept light source that can be easily used in most microscopes. Multicolor emission from the QDs is simply controlled by digitally switching excitation UVLEDs, eliminating the use of mechanically-driven gratings or filters. We used gold nanoparticles as optical markers for hyperspectral microscopy. Due to the effect of localized surface plasmon resonance, gold nanoparticles demonstrate size and shape-dependent absorption spectra. Employed in a standard microscope, the QD light source enabled multispectral absorption imaging of macrophage cells labeled with gold nanorods and nanospheres. PMID:24877018

  11. Low-cost photovoltaics: Luminescent solar concentrators and colloidal quantum dot solar cells

    NASA Astrophysics Data System (ADS)

    Leow, Shin Woei

    /emission spectra of an organic luminescent dye (LR305), the transmission coefficient and refractive index of acrylic as parameters that describe the system. Simulations suggest that for LR305, 8-10cm of luminescent material surrounding the PV cell yields the highest increase in power gain per unit area of LSC added, thereby determining the ideal spacing between PV cells in the panel. The model also predicts that for different PV cell dimensions, there exists an optimum waveguide thickness which efficiently transports photon collected by the waveguide to the PV cell with minimal loss, and maintains an even distribution of photons across the cell surface. For the case of the 12.5 by 1cm rectangular cells used in this work, the calculated waveguide thickness is 3mm. For larger cells, every 1cm increment in PV cell width should be accompanied by a 0.75mm increase in waveguide thickness to preserve peak performance. In line with the goal of pushing for cost competitive photovoltaics, the last part of this work shifts to the study of colloidal quantum dot solar cells. A combination of low temperature, highly scalable fabrication process and reduced material usage for thin films offers us a means to produce flexible and cheap solar cells. Tagging on to existing work already performed on germanium quantum dot solar cells, additional work was carried out to further characterize the material. The effect of film thickness, nano-particle surface conditions and thermal anneal were investigated. There is evidence to suggest that the quantum dot devices contain high levels of parasitic resistances. Short circuit current densities increase by up to two times with two spin-cast layers compared to four, leading to the conjecture that charge carrier life time is low with high levels of recombination. Annealing to improve carrier mobility produces devices with current densities up to 301microA, a fourfold increase, but output voltages saw a sharp decrease from 0.12V to 0.015V. In tandem with the work

  12. Low-cost photovoltaics: Luminescent solar concentrators and colloidal quantum dot solar cells

    NASA Astrophysics Data System (ADS)

    Leow, Shin Woei

    /emission spectra of an organic luminescent dye (LR305), the transmission coefficient and refractive index of acrylic as parameters that describe the system. Simulations suggest that for LR305, 8-10cm of luminescent material surrounding the PV cell yields the highest increase in power gain per unit area of LSC added, thereby determining the ideal spacing between PV cells in the panel. The model also predicts that for different PV cell dimensions, there exists an optimum waveguide thickness which efficiently transports photon collected by the waveguide to the PV cell with minimal loss, and maintains an even distribution of photons across the cell surface. For the case of the 12.5 by 1cm rectangular cells used in this work, the calculated waveguide thickness is 3mm. For larger cells, every 1cm increment in PV cell width should be accompanied by a 0.75mm increase in waveguide thickness to preserve peak performance. In line with the goal of pushing for cost competitive photovoltaics, the last part of this work shifts to the study of colloidal quantum dot solar cells. A combination of low temperature, highly scalable fabrication process and reduced material usage for thin films offers us a means to produce flexible and cheap solar cells. Tagging on to existing work already performed on germanium quantum dot solar cells, additional work was carried out to further characterize the material. The effect of film thickness, nano-particle surface conditions and thermal anneal were investigated. There is evidence to suggest that the quantum dot devices contain high levels of parasitic resistances. Short circuit current densities increase by up to two times with two spin-cast layers compared to four, leading to the conjecture that charge carrier life time is low with high levels of recombination. Annealing to improve carrier mobility produces devices with current densities up to 301microA, a fourfold increase, but output voltages saw a sharp decrease from 0.12V to 0.015V. In tandem with the work

  13. Spectroscopic Identification of Tri-n-octylphosphine Oxide (TOPO) Impurities and Elucidation of Their Roles in Cadmium Selenide Quantum-Wire Growth

    PubMed Central

    Wang, Fudong; Tang, Rui; Kao, Jeff L.-F.; Dingman, Sean D.; Buhro, William E.

    2009-01-01

    Tri-n-octylphosphine oxide (TOPO) is the most commonly used solvent for the synthesis of colloidal nanocrystals. Here we show that the use of different batches of commercially obtained TOPO solvent introduces significant variability into the outcomes of CdSe quantum-wire syntheses. This irreproducibility is attributed to varying amounts of phosphorus-containing impurities in the different TOPO batches. We employ 31P NMR to identify 10 of the common TOPO impurities. Their beneficial, harmful, or negligible effects on quantum-wire growth are determined. The impurity di-n-octylphosphinic acid (DOPA) is found to be the important beneficial TOPO impurity for the reproducible growth of high-quality CdSe quantum wires. DOPA is shown to beneficially modify precursor reactivity through ligand substitution. The other significant TOPO impurities are ranked according to their abilities to similarly influence precursor reactivity. The results are likely of general relevance to most nanocrystal syntheses conducted in TOPO. PMID:19296595

  14. Colloidal PbSe quantum dot-solution-filled liquid-core optical fiber for 1.55 μm telecommunication wavelengths.

    PubMed

    Zhang, Lei; Zhang, Yu; Kershaw, Steve V; Zhao, Yanhui; Wang, Yu; Jiang, Yongheng; Zhang, Tieqiang; Yu, William W; Gu, Pengfei; Wang, Yiding; Zhang, Hanzhuang; Rogach, Andrey L

    2014-03-14

    We have studied the optical properties of PbSe colloidal quantum dot-solution filled hollow core multimode silica waveguides as a function of quantum dot-solution concentration, waveguide length, optical pump power and choice of organic solvent in order to establish the conditions to maximize near infrared spontaneous emission intensities. The optical performance was compared and showed good agreement with a simple three level system model for the quantum dots confined in an optical waveguide. Near infrared absorption-free solvent of tetrachlorethylene was confirmed to be a good candidate for the waveguide medium due to the enhancement of output intensity from the liquid-core fiber compared to the performance in toluene-based fiber. This approach demonstrates a useful method for early characterization of quantum dot materials in a waveguide test-bed with minimal material processing on the colloidal nanoparticles.

  15. Surface structure of CdSe Nanorods revealed by combined X-rayabsorption fine structure measurements and ab-initio calculations

    SciTech Connect

    Aruguete, Deborah A.; Marcus, Matthew A.; Li, Liang-shi; Williamson, Andrew; Fakra, Sirine; Gygi, Francois; Galli, Giulia; Alivisatos, A. Paul

    2006-01-27

    We report orientation-specific, surface-sensitive structural characterization of colloidal CdSe nanorods with extended X-ray absorption fine structure spectroscopy and ab-initio density functional theory calculations. Our measurements of crystallographically-aligned CdSe nanorods show that they have reconstructed Cd-rich surfaces. They exhibit orientation-dependent changes in interatomic distances which are qualitatively reproduced by our calculations. These calculations reveal that the measured interatomic distance anisotropy originates from the nanorod surface.

  16. One-step colloidal synthesis of biocompatible water-soluble ZnS quantum dot/chitosan nanoconjugates

    NASA Astrophysics Data System (ADS)

    Ramanery, Fábio P.; Mansur, Alexandra AP; Mansur, Herman S.

    2013-12-01

    Quantum dots (QDs) are luminescent semiconductor nanocrystals with great prospective for use in biomedical and environmental applications. Nonetheless, eliminating the potential cytotoxicity of the QDs made with heavy metals is still a challenge facing the research community. Thus, the aim of this work was to develop a novel facile route for synthesising biocompatible QDs employing carbohydrate ligands in aqueous colloidal chemistry with optical properties tuned by pH. The synthesis of ZnS QDs capped by chitosan was performed using a single-step aqueous colloidal process at room temperature. The nanobioconjugates were extensively characterised by several techniques, and the results demonstrated that the average size of ZnS nanocrystals and their fluorescent properties were influenced by the pH during the synthesis. Hence, novel 'cadmium-free' biofunctionalised systems based on ZnS QDs capped by chitosan were successfully developed exhibiting luminescent activity that may be used in a large number of possible applications, such as probes in biology, medicine and pharmacy.

  17. Sub-picosecond spin relaxation of bright excitons and imbalance suppression in asymmetric Cdse/Zns nanocrystal quantum dots under an applied magnetic field.

    PubMed

    Kyhm, Kwangseuk; Kim, Jihoon; Yang, Ho-Soon; Je, Koo-Chul; Murayama, Akihiro

    2012-03-01

    The ultrafast spin dynamics of the bright exciton in CdSe/ZnS nanocrystal quantum dots has been investigated using a circularly polarized pump-probe experiment. A remarkably fast spin flip (-500 fs) of the bright exciton was observed at 4 K, which is attributed to the anisotropic electron-hole exchange interaction and the random positioning of nanocrystal quantum dots. In the presence of an applied magnetic field (5 T), the exciton spin parallel to the external magnetic field was favored due to Zeeman splitting. We found that this imbalance can possibly be suppressed by the state-blocking and the mixing of the 1(L) and 1(U) states in asymmetric quantum dots.

  18. Dynamics of electronic excitations relaxation in hydrophilic colloidal CdS quantum dots in gelatin with involvement of localized states

    NASA Astrophysics Data System (ADS)

    Smirnov, M. S.; Buganov, O. V.; Shabunya-Klyachkovskaya, E. V.; Tikhomirov, S. A.; Ovchinnikov, O. V.; Vitukhnovsky, A. G.; Perepelitsa, A. S.; Matsukovich, A. S.; Katsaba, A. V.

    2016-10-01

    Dynamics of the 1Se-1S3/2 exciton in colloidal CdS quantum dots with diameter of 3.1 ÷ 4.5 nm in gelatin with involvement of localized states was studied by means of femtosecond photoinduced absorption spectroscopy (pump-probe), thermally stimulated luminescence (TSL) observed under permanently excited luminescence. It was found that the bleaching band occurs in the energy region of exciton ground state under excitation by femtosecond laser pulses. The complex dynamics of bleaching recovery is caused by the capture of electron on localized states, found using TSL. The stochastic model describing the dynamics of bleaching recovery is discussed. It is shown that the low efficiency of exciton luminescence is caused by the rapid capture of holes by luminescence centers.

  19. Trap State Effects in PbS Colloidal Quantum Dot Exciton Kinetics Using Photocarrier Radiometry Intensity and Temperature Measurements

    NASA Astrophysics Data System (ADS)

    Wang, Jing; Mandelis, Andreas; Melnikov, Alexander; Sun, Qiming

    2016-06-01

    Colloidal quantum dots (CQDs) have attracted significant interest for applications in electronic and optoelectronic devices such as photodetectors, light-emitting diodes, and solar cells. However, a poor understanding of charge transport in these nanocrystalline films hinders their practical applications. The photocarrier radiometry (PCR) technique, a frequency-domain photoluminescence method spectrally gated for monitoring radiative recombination photon emissions while excluding thermal infrared photons due to non-radiative recombination, has been applied to PbS CQD thin films for the analysis of charge transport properties. Linear excitation intensity responses of PCR signals were found in the reported experimental conditions. The type and influence of trap states in the coupled PbS CQD thin film were analyzed with PCR temperature- and time-dependent results.

  20. Brightly Luminescent and Color-Tunable Colloidal CH3NH3PbX3 (X = Br, I, Cl) Quantum Dots: Potential Alternatives for Display Technology.

    PubMed

    Zhang, Feng; Zhong, Haizheng; Chen, Cheng; Wu, Xian-gang; Hu, Xiangmin; Huang, Hailong; Han, Junbo; Zou, Bingsuo; Dong, Yuping

    2015-04-28

    Organometal halide perovskites are inexpensive materials with desirable characteristics of color-tunable and narrow-band emissions for lighting and display technology, but they suffer from low photoluminescence quantum yields at low excitation fluencies. Here we developed a ligand-assisted reprecipitation strategy to fabricate brightly luminescent and color-tunable colloidal CH3NH3PbX3 (X = Br, I, Cl) quantum dots with absolute quantum yield up to 70% at room temperature and low excitation fluencies. To illustrate the photoluminescence enhancements in these quantum dots, we conducted comprehensive composition and surface characterizations and determined the time- and temperature-dependent photoluminescence spectra. Comparisons between small-sized CH3NH3PbBr3 quantum dots (average diameter 3.3 nm) and corresponding micrometer-sized bulk particles (2-8 μm) suggest that the intense increased photoluminescence quantum yield originates from the increase of exciton binding energy due to size reduction as well as proper chemical passivations of the Br-rich surface. We further demonstrated wide-color gamut white-light-emitting diodes using green emissive CH3NH3PbBr3 quantum dots and red emissive K2SiF6:Mn(4+) as color converters, providing enhanced color quality for display technology. Moreover, colloidal CH3NH3PbX3 quantum dots are expected to exhibit interesting nanoscale excitonic properties and also have other potential applications in lasers, electroluminescence devices, and optical sensors. PMID:25824283

  1. Effective improvement in optical properties of colloidal CdTe@ZnS quantum dots synthesized from aqueous solution

    NASA Astrophysics Data System (ADS)

    Wang, Yongbo; Si, Boni; Lu, Siwu; Ma, Xuan; Liu, Enzhou; Fan, Jun; Li, Xinghua; Hu, Xiaoyun

    2016-09-01

    Efficient synthesis of high-quality quantum dots (QDs) with excellent optical properties by aqueous synthesis is still of great significance for extended optical applications. Herein we highlight the advantages in optical properties of colloidal CdTe@ZnS QDs prepared by a facile and highly effective aqueous synthesis method. These achievements were realized by delicate manipulation of the conditions involved in nucleation and the growth process. Transmission electron microscopy (TEM) images indicated the QDs were uniform size and well dispersible. The emission peaks of the as-prepared QDs could shift from 496 to 698 nm with narrow full width at half maximum (FWHM), and the corresponding fluorescent color changed from green to red. Moreover, the emission could even reach to the near-infrared (NIR) region (706-796 nm) by extending the reaction time. The highest photoluminescence (PL) quantum yield (QY) of the QDs could reach to 60%, and the average of FWHM was about 55 nm. To address the problem of wide size-distribution in PL QY decrease and FWHM broadening, the colloids of QDs prepared at long reaction time (above 3 h) were centrifuged (12 000 r min-1). In addition, the assessment of QD cytotoxicity indicated the CdTe@ZnS QDs were much less cytotoxic and showed good biocompatibility. Compared with organic synthesis, our aqueous synthesis of QDs could be carried out efficiently on a large scale and showed good batch-to-batch reproducibility. The as-prepared CdTe@ZnS QDs exhibited excellent optical properties and hold a good potential to be applied in optoelectronic and biological applications.

  2. Effective improvement in optical properties of colloidal CdTe@ZnS quantum dots synthesized from aqueous solution.

    PubMed

    Wang, Yongbo; Si, Boni; Lu, Siwu; Ma, Xuan; Liu, Enzhou; Fan, Jun; Li, Xinghua; Hu, Xiaoyun

    2016-09-01

    Efficient synthesis of high-quality quantum dots (QDs) with excellent optical properties by aqueous synthesis is still of great significance for extended optical applications. Herein we highlight the advantages in optical properties of colloidal CdTe@ZnS QDs prepared by a facile and highly effective aqueous synthesis method. These achievements were realized by delicate manipulation of the conditions involved in nucleation and the growth process. Transmission electron microscopy (TEM) images indicated the QDs were uniform size and well dispersible. The emission peaks of the as-prepared QDs could shift from 496 to 698 nm with narrow full width at half maximum (FWHM), and the corresponding fluorescent color changed from green to red. Moreover, the emission could even reach to the near-infrared (NIR) region (706-796 nm) by extending the reaction time. The highest photoluminescence (PL) quantum yield (QY) of the QDs could reach to 60%, and the average of FWHM was about 55 nm. To address the problem of wide size-distribution in PL QY decrease and FWHM broadening, the colloids of QDs prepared at long reaction time (above 3 h) were centrifuged (12 000 r min(-1)). In addition, the assessment of QD cytotoxicity indicated the CdTe@ZnS QDs were much less cytotoxic and showed good biocompatibility. Compared with organic synthesis, our aqueous synthesis of QDs could be carried out efficiently on a large scale and showed good batch-to-batch reproducibility. The as-prepared CdTe@ZnS QDs exhibited excellent optical properties and hold a good potential to be applied in optoelectronic and biological applications. PMID:27482982

  3. Effective improvement in optical properties of colloidal CdTe@ZnS quantum dots synthesized from aqueous solution

    NASA Astrophysics Data System (ADS)

    Wang, Yongbo; Si, Boni; Lu, Siwu; Ma, Xuan; Liu, Enzhou; Fan, Jun; Li, Xinghua; Hu, Xiaoyun

    2016-09-01

    Efficient synthesis of high-quality quantum dots (QDs) with excellent optical properties by aqueous synthesis is still of great significance for extended optical applications. Herein we highlight the advantages in optical properties of colloidal CdTe@ZnS QDs prepared by a facile and highly effective aqueous synthesis method. These achievements were realized by delicate manipulation of the conditions involved in nucleation and the growth process. Transmission electron microscopy (TEM) images indicated the QDs were uniform size and well dispersible. The emission peaks of the as-prepared QDs could shift from 496 to 698 nm with narrow full width at half maximum (FWHM), and the corresponding fluorescent color changed from green to red. Moreover, the emission could even reach to the near-infrared (NIR) region (706–796 nm) by extending the reaction time. The highest photoluminescence (PL) quantum yield (QY) of the QDs could reach to 60%, and the average of FWHM was about 55 nm. To address the problem of wide size-distribution in PL QY decrease and FWHM broadening, the colloids of QDs prepared at long reaction time (above 3 h) were centrifuged (12 000 r min‑1). In addition, the assessment of QD cytotoxicity indicated the CdTe@ZnS QDs were much less cytotoxic and showed good biocompatibility. Compared with organic synthesis, our aqueous synthesis of QDs could be carried out efficiently on a large scale and showed good batch-to-batch reproducibility. The as-prepared CdTe@ZnS QDs exhibited excellent optical properties and hold a good potential to be applied in optoelectronic and biological applications.

  4. Optical properties of colloidal aqueous synthesized 3 mercaptopropionic acid stabilized CdS quantum dots

    NASA Astrophysics Data System (ADS)

    Sumanth Kumar, D.; Jai Kumar, B.; Mahesh H., M.

    2016-05-01

    We have explored an easiest and simplest aqueous route to synthesize bright green luminescent CdS QDs using 3-Mercaptopropionic acid (MPA) as a stabilizer in air ambient for solar cell applications. The CdS quantum dots showed a strong quantum confinement effect with good stability, size and excellent photoluminescence. MPA Capping on CdS QDs was confirmed through FTIR. The Optical absorption spectrum revealed the CdS quantum dots are highly transparent in the visible region with absorption peak at 380 nm, confirming the quantum confinement. Photoluminescence showed an emission peak at 525 nm wavelength. The optical band gap energy was found to be 3.19 eV and CdS quantum dots radius calculated using Brus equation is 1.5 nm. The results are presented and discussed in detail.

  5. Fluorescence resonance energy transfer measured by spatial photon migration in CdSe-ZnS quantum dots colloidal systems as a function of concentration

    SciTech Connect

    Azevedo, G.; Monte, A. F. G.; Reis, A. F.; Messias, D. N.

    2014-11-17

    The study of the spatial photon migration as a function of the concentration brings into attention the problem of the energy transfer in quantum dot embedded systems. By measuring the photon propagation and its spatial dependence, it is possible to understand the whole dynamics in a quantum dot system, and also improve their concentration dependence to maximize energy propagation due to radiative and non-radiative processes. In this work, a confocal microscope was adapted to scan the spatial distribution of photoluminescence from CdSe-ZnS core-shell quantum dots in colloidal solutions. The energy migration between the quantum dots was monitored by the direct measurement of the photon diffusion length, according to the diffusion theory. We observed that the photon migration length decreases by increasing the quantum dot concentration, this kind of behavior has been regarded as a signature of Förster resonance energy transfer in the system.

  6. High reduction of interfacial charge recombination in colloidal quantum dot solar cells by metal oxide surface passivation

    NASA Astrophysics Data System (ADS)

    Chang, Jin; Kuga, Yuki; Mora-Seró, Iván; Toyoda, Taro; Ogomi, Yuhei; Hayase, Shuzi; Bisquert, Juan; Shen, Qing

    2015-03-01

    Bulk heterojunction (BHJ) solar cells based on colloidal QDs and metal oxide nanowires (NWs) possess unique and outstanding advantages in enhancing light harvesting and charge collection in comparison to planar architectures. However, the high surface area of the NW structure often brings about a large amount of recombination (especially interfacial recombination) and limits the open-circuit voltage in BHJ solar cells. This problem is solved here by passivating the surface of the metal oxide component in PbS colloidal quantum dot solar cells (CQDSCs). By coating thin TiO2 layers onto ZnO-NW surfaces, the open-circuit voltage and power conversion efficiency have been improved by over 40% in PbS CQDSCs. Characterization by transient photovoltage decay and impedance spectroscopy indicated that the interfacial recombination was significantly reduced by the surface passivation strategy. An efficiency as high as 6.13% was achieved through the passivation approach and optimization for the length of the ZnO-NW arrays (device active area: 16 mm2). All solar cells were tested in air, and exhibited excellent air storage stability (without any performance decline over more than 130 days). This work highlights the significance of metal oxide passivation in achieving high performance BHJ solar cells. The charge recombination mechanism uncovered in this work could shed light on the further improvement of PbS CQDSCs and/or other types of solar cells.Bulk heterojunction (BHJ) solar cells based on colloidal QDs and metal oxide nanowires (NWs) possess unique and outstanding advantages in enhancing light harvesting and charge collection in comparison to planar architectures. However, the high surface area of the NW structure often brings about a large amount of recombination (especially interfacial recombination) and limits the open-circuit voltage in BHJ solar cells. This problem is solved here by passivating the surface of the metal oxide component in PbS colloidal quantum dot solar

  7. Biodistribution and stability of CdSe core quantum dots in mouse digestive tract following per os administration: Advantages of double polymer/silica coated nanocrystals

    SciTech Connect

    Loginova, Y.F.; Dezhurov, S.V.; Zherdeva, V.V.; Kazachkina, N.I.; Wakstein, M.S.; Savitsky, A.P.

    2012-03-02

    Highlights: Black-Right-Pointing-Pointer New QDs coated with combination of polythiol ligands and silica shell were synthesized. Black-Right-Pointing-Pointer We examine the QDs stability in digestive tract of mice after per os administration. Black-Right-Pointing-Pointer The polymer/silica shell prevents QDs degradation and fluorescence quenching in vivo. -- Abstract: CdSe-core, ZnS-capped semiconductor quantum dots (QDs) are of great potential for biomedical applications. However, applications in the gastrointestinal tract for in vivo imaging and therapeutic purposes are hampered by their sensitivity to acidic environments and potential toxicity. Here we report the use of coatings with a combination of polythiol ligands and silica shell (QDs PolyT-APS) to stabilize QDs fluorescence under acidic conditions. We demonstrated the stability of water-soluble QDs PolyT-APS both in vitro, in strong acidic solutions, and in vivo. The biodistribution, stability and photoluminescence properties of QDs in the gastrointestinal tract of mice after per os administration were assessed. We demonstrated that QDs coated with current traditional materials - mercapto compounds (QDs MPA) and pendant thiol group (QDs PolyT) - are not capable of protecting QDs from chemically induced degradation and surface modification. Polythiol ligands and silica shell quantum dots (QDs PolyT-APS) are suitable for biological and biomedical applications in the gastrointestinal tract.

  8. 'Giant' multishell CdSe nanocrystal quantum dots with supporessed blinking: novel fluorescent probes for real-time detection of single-molecule events

    SciTech Connect

    Hollingsworth, Jennifer A; Vela, Javier; Htoon, Han; Klimov, Victor I; Casson, Amy R; Chen, Yongfen

    2009-01-01

    We reported for the first time that key nanocrystal quantum dot (NQD) optical properties-quantum yield, photobleaching and blinking-can be rendered independent ofNQD surface chemistry and environment by growth of a very thick, defect-free inorganic shell. Here, we show the precise shell-thickness dependence of these effects. We demonstrate that 'giant-shell' NQDs can be largely non-blinking for observation times as long as 54 minutes and lhat on-time fractions are independent of experimental time-resolution from 1-200 ms. These effects are primarily demonstrated on (CdSe)CdS (core)shell NQDs, but we also show that alloyed shells comprising Cd.Znl.'S and terminated with a non-cytotoxic ZnS layer exhibit similar properties. The mechanism for suppressed blinking and dramatically enhanced stability is attributed to both effective isolation of the NQD core excitonic wavefunction from the NQD surface, as well as a quasi-Type II electronic structure. The unusual electronic structure provides for effective spatial separation of the electron and hole into the shell and core, respectively, and, thereby, for reduced efficiencies in non-radiative Auger recombination.

  9. 'Giant' multishell CdSe nanocrystal quantum dots with suppressed blinking: Novel fluorescent probes for real-time detection of single-molecule events.

    PubMed

    Hollingsworth, Jennifer A; Vela, Javier; Chen, Yongfen; Htoon, Han; Klimov, Victor I; Casson, Amy R

    2009-03-01

    We reported for the first time that key nanocrystal quantum dot (NQD) optical properties-quantum yield, photobleaching and blinking-can be rendered independent of NQD surface chemistry and environment by growth of a very thick, defect-free inorganic shell (Chen, et al. J. Am. Chem. Soc. 2008). Here, we show the precise shell-thickness dependence of these effects. We demonstrate that 'giant-shell' NQDs can be largely non-blinking for observation times as long as 54 minutes and that on-time fractions are independent of experimental time-resolution from 1-200 ms. These effects are primarily demonstrated on (CdSe)CdS (core)shell NQDs, but we also show that alloyed shells comprising Cd(x)Zn(1-x)S and terminated with a non-cytotoxic ZnS layer exhibit similar properties. The mechanism for suppressed blinking and dramatically enhanced stability is attributed to both effective isolation of the NQD core excitonic wavefunction from the NQD surface, as well as a quasi-Type II electronic structure. The unusual electronic structure provides for effective spatial separation of the electron and hole into the shell and core, respectively, and, thereby, for reduced efficiencies in non-radiative Auger recombination.

  10. Multiple Exciton Generation in Colloidal Silicon Nanocrystals

    SciTech Connect

    Beard, M. C.; Knutsen, K. P.; Yu, P.; Luther, J. M.; Song, Q.; Metzger, W. K.; Ellingson, R. J.; Nozik, A. M.

    2007-01-01

    Multiple exciton generation (MEG) is a process whereby multiple electron-hole pairs, or excitons, are produced upon absorption of a single photon in semiconductor nanocrystals (NCs) and represents a promising route to increased solar conversion efficiencies in single-junction photovoltaic cells. We report for the first time MEG yields in colloidal Si NCs using ultrafast transient absorption spectroscopy. We find the threshold photon energy for MEG in 9.5 nm diameter Si NCs (effective band gap {identical_to} Eg = 1.20 eV) to be 2.4 {+-} 0.1E{sub g} and find an exciton-production quantum yield of 2.6 {+-} 0.2 excitons per absorbed photon at 3.4E{sub g}. While MEG has been previously reported in direct-gap semiconductor NCs of PbSe, PbS, PbTe, CdSe, and InAs, this represents the first report of MEG within indirect-gap semiconductor NCs. Furthermore, MEG is found in relatively large Si NCs (diameter equal to about twice the Bohr radius) such that the confinement energy is not large enough to produce a large blue-shift of the band gap (only 80 meV), but the Coulomb interaction is sufficiently enhanced to produce efficient MEG. Our findings are of particular importance because Si dominates the photovoltaic solar cell industry, presents no problems regarding abundance and accessibility within the Earth's crust, and poses no significant environmental problems regarding toxicity.

  11. Plasmonic emission enhancement of colloidal quantum dots in the presence of bimetallic nanoparticles

    SciTech Connect

    Sadeghi, S. M.; Hatef, A.; Meunier, M.; Nejat, A.; Campbell, Q.

    2014-04-07

    We studied plasmonic features of bimetallic nanostructures consisting of gold nanoisland cores semi-coated with a chromium layer and explored how they influence emission of CdSe/ZnS quantum dots. We showed that, compared with chromium-covered glass substrates without the gold cores, the bimetallic nanostructures could significantly enhance the emission of the quantum dots. We studied the impact of the excitation intensity and thickness of the chromium layer on this process and utilized numerical means to identify the mechanisms behind it. Our results suggest that when the chromium layer is thin, the enhancement process is the result of the bimetallic plasmonic features of the nanostructures. As the chromium layer becomes thick, the impact of the gold cores is screened and the enhancement mostly happens mostly via the field enhancement of chromium nanoparticles in the absence of significant energy transfer from the quantum dots to these nanoparticles.

  12. Evidence for a diffusion-controlled mechanism for fluorescence blinking of colloidal quantum dots.

    PubMed

    Pelton, Matthew; Smith, Glenna; Scherer, Norbert F; Marcus, Rudolph A

    2007-09-01

    Fluorescence blinking in nanocrystal quantum dots is known to exhibit power-law dynamics, and several different mechanisms have been proposed to explain this behavior. We have extended the measurement of quantum-dot blinking by characterizing fluctuations in the fluorescence of single dots over time scales from microseconds to seconds. The power spectral density of these fluctuations indicates a change in the power-law statistics that occurs at a time scale of several milliseconds, providing an important constraint on possible mechanisms for the blinking. In particular, the observations are consistent with the predictions of models wherein blinking is controlled by diffusion of the energies of electron or hole trap states.

  13. Evidence for a diffusion-controlled mechanism for fluorescence blinking of colloidal quantum dots.

    SciTech Connect

    Pelton, M.; Smith, G.; Scherer, N. F.; Marcus, R. A.; Univ. of Chicago; California Inst. of Tech.

    2007-09-04

    Fluorescence blinking in nanocrystal quantum dots is known to exhibit power-law dynamics, and several different mechanisms have been proposed to explain this behavior. We have extended the measurement of quantum-dot blinking by characterizing fluctuations in the fluorescence of single dots over time scales from microseconds to seconds. The power spectral density of these fluctuations indicates a change in the power-law statistics that occurs at a time scale of several milliseconds, providing an important constraint on possible mechanisms for the blinking. In particular, the observations are consistent with the predictions of models wherein blinking is controlled by diffusion of the energies of electron or hole trap states.

  14. Electrochemical control over photoinduced electron transfer and trapping in CdSe-CdTe quantum-dot solids.

    PubMed

    Boehme, Simon C; Walvis, T Ardaan; Infante, Ivan; Grozema, Ferdinand C; Vanmaekelbergh, Daniël; Siebbeles, Laurens D A; Houtepen, Arjan J

    2014-07-22

    Understanding and controlling charge transfer between different kinds of colloidal quantum dots (QDs) is important for devices such as light-emitting diodes and solar cells and for thermoelectric applications. Here we study photoinduced electron transfer between CdTe and CdSe QDs in a QD film. We find that very efficient electron trapping in CdTe QDs obstructs electron transfer to CdSe QDs under most conditions. Only the use of thiol ligands results in somewhat slower electron trapping; in this case the competition between trapping and electron transfer results in a small fraction of electrons being transferred to CdSe. However, we demonstrate that electron trapping can be controlled and even avoided altogether by using the unique combination of electrochemistry and transient absorption spectroscopy. When the Fermi level is raised electrochemically, traps are filled with electrons and electron transfer from CdTe to CdSe QDs occurs with unity efficiency. These results show the great importance of knowing and controlling the Fermi level in QD films and open up the possibility of studying the density of trap states in QD films as well as the systematic investigation of the intrinsic electron transfer rates in donor-acceptor films. PMID:24883930

  15. 3D Assembly of All-Inorganic Colloidal Nanocrystals into Gels and Aerogels.

    PubMed

    Sayevich, Vladimir; Cai, Bin; Benad, Albrecht; Haubold, Danny; Sonntag, Luisa; Gaponik, Nikolai; Lesnyak, Vladimir; Eychmüller, Alexander

    2016-05-17

    We report an efficient approach to assemble a variety of electrostatically stabilized all-inorganic semiconductor nanocrystals (NCs) by their linking with appropriate ions into multibranched gel networks. These all-inorganic non-ordered 3D assemblies benefit from strong interparticle coupling, which facilitates charge transport between the NCs with diverse morphologies, compositions, sizes, and functional capping ligands. Moreover, the resulting dry gels (aerogels) are highly porous monolithic structures, which preserve the quantum confinement of their building blocks. The inorganic semiconductor aerogel made of 4.5 nm CdSe colloidal NCs capped with I(-) ions and bridged with Cd(2+) ions had a large surface area of 146 m(2)  g(-1) . PMID:27100131

  16. Quantum confinement and dielectric profiles of colloidal nanoplatelets of halide inorganic and hybrid organic-inorganic perovskites.

    PubMed

    Sapori, Daniel; Kepenekian, Mikaël; Pedesseau, Laurent; Katan, Claudine; Even, Jacky

    2016-03-28

    Quantum confinement as well as high frequency ε∞ and static εs dielectric profiles are described for nanoplatelets of halide inorganic perovskites CsPbX3 (X = I, Br, Cl) and hybrid organic-inorganic perovskites (HOP) in two-dimensional (2D) and three-dimensional (3D) structures. 3D HOP are currently being sought for their impressive photovoltaic ability. Prior to this sudden popularity, 2D HOP materials were driving intense activity in the field of optoelectronics. Such developments have been enriched by the recent ability to synthesize colloidal nanostructures of controlled sizes of 2D and 3D HOP. This raises the need to achieve a thorough description of the electronic structure and dielectric properties of these systems. In this work, we go beyond the abrupt dielectric interface model and reach the atomic scale description. We examine the influence of the nature of the halogen and of the cation on the band structure and dielectric constants. Similarly, we survey the effect of dimensionality and shape of the perovskite. In agreement with recent experimental results, we show an increase of the band gap and a decrease of ε∞ when the size of a nanoplatelet reduces. By inspecting 2D HOP, we find that it cannot be described as a simple superposition of independent inorganic and organic layers. Finally, the dramatic impact of ionic contributions on the dielectric constant εs is analysed. PMID:26705549

  17. Synthesis of size-controlled colloidal InAs quantum dots using triphenylarsine as a stable arsenic source

    NASA Astrophysics Data System (ADS)

    Uesugi, Hideo; Kita, Masao; Omata, Takahisa

    2015-04-01

    Colloidal indium arsenide (InAs) quantum dots (QDs) were synthesized by heating an organometallic solution containing the easy-to-handle arsenic source triphenylarsine and indium tribromide in a mixture of oleylamine, tri-n-octylphosphine and octadecene. The one-pot reaction was heated at 320 °C to give spherical, monodisperse QDs in less than 15 min; the size of the QDs was controlled in the range from 3 to 6 nm by changing the reaction time. Tetrahedral QDs composed of four enclosed {111} faces of zincblende InAs were obtained after reaction for 30 min. The dependence of the shape of the QDs on reaction time was rationalized in terms of the adsorption strength of the capping ligand. The obtained QDs exhibited size-dependent optical gaps and PL emission, indicating narrow size distribution and good crystal quality. Because the PL emission exhibited a large Stokes shift of 100-200 meV, the electronic transition responsible for the PL emission was related to defects inside the QDs, and must involve the relaxation of excited electrons at the quantized electron state 1Se because of the large size-dependent energy variation.

  18. Conjugated assembly of colloidal zinc oxide quantum dots and multiwalled carbon nanotubes for an excellent photosensitive ultraviolet photodetector.

    PubMed

    Boruah, Buddha Deka; Misra, Abha

    2016-09-01

    Conjugation of highly dense colloidal zinc oxide quantum dots (ZnO QDs) on multiwalled carbon nanotubes (ZnO QDs@MWCNTs) is achieved for high performance ultraviolet (UV) photodetection. Significant improvement in the photoresponse of the ZnO QDs@MWCNTs photodetector (PD) is established as compared to a pristine ZnO QDs PD. The conjugation of two constituents allows the direct transfer of photoinduced charge carriers in ZnO QDs to MWCNTs for an efficient electrical path that considerably reduces charge recombination during UV exposure. Linearity in the response current with both the UV illumination intensity as well as external bias voltage reveals the photoelastic behavior of the ZnO QDs@MWCNTs PD. Moreover, the PD displays faster response and recovery times of 1.6 s and 1.9 s, respectively, than the most conventional PDs. In addition, spectral photoresponse analysis of the PD presents visible-blind behavior. Overall, conjugation of the hybrid heterostructure presented excellent photoelastic, high performance and visible-blind UV photodetection. PMID:27454746

  19. Conjugated assembly of colloidal zinc oxide quantum dots and multiwalled carbon nanotubes for an excellent photosensitive ultraviolet photodetector

    NASA Astrophysics Data System (ADS)

    Deka Boruah, Buddha; Misra, Abha

    2016-09-01

    Conjugation of highly dense colloidal zinc oxide quantum dots (ZnO QDs) on multiwalled carbon nanotubes (ZnO QDs@MWCNTs) is achieved for high performance ultraviolet (UV) photodetection. Significant improvement in the photoresponse of the ZnO QDs@MWCNTs photodetector (PD) is established as compared to a pristine ZnO QDs PD. The conjugation of two constituents allows the direct transfer of photoinduced charge carriers in ZnO QDs to MWCNTs for an efficient electrical path that considerably reduces charge recombination during UV exposure. Linearity in the response current with both the UV illumination intensity as well as external bias voltage reveals the photoelastic behavior of the ZnO QDs@MWCNTs PD. Moreover, the PD displays faster response and recovery times of 1.6 s and 1.9 s, respectively, than the most conventional PDs. In addition, spectral photoresponse analysis of the PD presents visible-blind behavior. Overall, conjugation of the hybrid heterostructure presented excellent photoelastic, high performance and visible-blind UV photodetection.

  20. Inverted organic solar cells using a solution-processed TiO2/CdSe electron transport layer to improve performance

    NASA Astrophysics Data System (ADS)

    Ma, Xiaoxiao; Xiong, Zhicheng; Wang, Wen; Zhang, Luming; Wu, Sujuan; Lu, Xubing; Gao, Xingsen; Shui, Lingling; Liu, Jun-Ming

    2016-04-01

    In the present work, cadmium selenide (CdSe) nanoparticles are deposited directly on TiO2 film to fabricate the TiO2/CdSe interlayer by a chemical bath deposition method. The inverted organic solar cells using poly(3-hexylthiophene) (P3HT) and [6,6]-phenyl C61 butyric acid methyl ester (PCBM) bulk heterojunction as an active layer and TiO2/CdSe interlayer as an electron transport layer (ETL) are fabricated in air. A series of microstructural, photo-electronic, and electrochemical characterizations on these cells are performed. The TiO2/CdSe structure with respect to either the TiO2 layer or the CdSe layer as the ETL exhibits significantly enhanced external quantum efficiency (EQE) in the visible region. The photoluminescence (PL) measurement shows that the exciton dissociation in the TiO2/CdSe structure is more effective than that in either the TiO2 or CdSe structure. The Nyquist plots obtained from electrochemical impedance spectroscopy (EIS) implies that the charge recombination in the TiO2/CdSe structure can be suppressed with respect to that in either the CdSe or TiO2 structure. The photovoltaic performances of the cells with the TiO2/CdSe ETL are clearly improved compared with the reference cells only with the TiO2 layer or CdSe layer as the ETL.

  1. A novel "green" synthesis of starch-capped CdSe nanostructures.

    PubMed

    Oluwafemi, Oluwatobi S

    2009-10-15

    This paper reports a "green" facile, room temperature, one-pot synthesis of starch-capped CdSe nanostructures with an obvious quantum confinement effect via a novel non-organometallic method. It is found that by simply tuning the Cd:Se molar ratio, dots and elongated particles of high aspect ratio could be prepared selectively in the presence of the same ligand concentration without any post-treatment. Spherical particles were produced at 1:1 ratio, while elongated particles were produced at 0.5:1 Cd:Se ratio. The X-ray diffraction (XRD) analysis showed that the particles were predominantly of wurtzite structure, with sharp diffraction patterns regardless of their size and shapes. We inferred that the elongated particles are formed by self-reorganisation occurring via adhesion between the spherical nanoparticles as a result of dipole-dipole interactions. PMID:19577905

  2. Photogeneration of hydrogen from water using CdSe nanocrystals demonstrating the importance of surface exchange

    PubMed Central

    Das, Amit; Han, Zhiji; Haghighi, Mohsen Golbon; Eisenberg, Richard

    2013-01-01

    Unique tripodal S-donor capping agents with an attached carboxylate are found to bind tightly to the surface of CdSe nanocrystals (NCs), making the latter water soluble. Unlike that in similarly solubilized CdSe NCs with one-sulfur or two-sulfur capping agents, dissociation from the NC surface is greatly reduced. The impact of this behavior is seen in the photochemical generation of H2 in which the CdSe NCs function as the light absorber with metal complexes in aqueous solution as the H2-forming catalyst and ascorbic acid as the electron donor source. This precious-metal–free system for H2 generation from water using [Co(bdt)2]− (bdt, benzene-1,2-dithiolate) as the catalyst exhibits excellent activity with a quantum yield for H2 formation of 24% at 520 nm light and durability with >300,000 turnovers relative to catalyst in 60 h. PMID:24082134

  3. Nanostructured TiO2 Films Attached CdSe QDs Toward Enhanced Photoelectrochemical Performance.

    PubMed

    Du, Yingying; Yang, Ping; Liu, Yunshi; Zhao, Jie; He, Haiyan; Miao, Yanping

    2016-06-01

    TiO2 films consisted of small nanoparticles were fabricated via a spinning coating method on fluorine doped in tin oxide (FTO) slide glass. After calcination, the films were subsequently sensitized by CdSe quantum dots (QDs) using mercaptopropionic acid (MPA) as a bifunctional surface modifier. Upon UV light irradiation, CdSe QDs inject electrons into TiO2 nanoparticles, thus resulting in the generation of photocurrent in QD-sensitized solar cell. The results indicate that TiO2 films sensitized by CdSe QDs have achieved 1.5-fold enhancement in photocurrent compared with pure TiO2 films, indicating that CdSe QDs can improve the photocurrent by promoting the separation of photoinduced charge carriers. In addition, the photocurrent enhances as the thickness of TiO2 films increased. Such improved photoelectrochemical performance is ascribed to the basis of improved interfacial charge transport of the TiO2-CdSe composite films. Combining QDs on TiO2 thin films is a promising and effective way to enhance the photoelectrochemical performance, which is important in QD-sensitized solar cell application. PMID:27427714

  4. Strong exciton-photon coupling with colloidal quantum dots in a high-Q bilayer microcavity

    NASA Astrophysics Data System (ADS)

    Giebink, Noel C.; Wiederrecht, Gary P.; Wasielewski, Michael R.

    2011-02-01

    We demonstrate evanescently coupled bilayer microcavities with Q-factors exceeding 250 fabricated by a simple spin-coating process. The cavity architecture consists of a slab waveguide lying upon a low refractive index spacer layer supported by a glass substrate. For a lossless guide layer, the cavity Q depends only on the thickness of the low index spacer and in principle can reach arbitrarily high values. We demonstrate the versatility of this approach by constructing cavities with a guide layer incorporating CdSe/ZnS core/shell quantum dots, where we observe strong coupling and hybridization between the 1S(e)-1S3/2(h) and 1S(e)-2S3/2(h) exciton states mediated by the cavity photon. This technique greatly simplifies the fabrication of high-Q planar microcavities for organic and inorganic quantum dot thin films and opens up new opportunities for the study of nonlinear optical phenomena in these materials.

  5. Multiplexed measurements by time resolved spectroscopy using colloidal CdSe/ZnS quantum dots

    SciTech Connect

    Kaiser, U.; Jimenez de Aberasturi, D.; Malinowski, R.; Amin, F.; Parak, W. J.; Heimbrodt, W.

    2014-01-27

    Multiplexed measurements of analytes in parallel is a topical demand in bioanalysis and bioimaging. An interesting alternative to commonly performed spectral multiplexing is lifetime multiplexing. In this Letter, we present a proof of principle of single-color lifetime multiplexing by coupling the same fluorophore to different nanoparticles. The effective lifetime of the fluorophores can be tuned by more than one order of magnitude due to resonance energy transfer from donor states. Measurements have been done on a model systems consisting of ATTO-590 dye molecules linked to either gold particles or to CdSe/ZnS core shell quantum dots. Both systems show the same luminescence spectrum of ATTO-590 dye emission in continuous wave excitation, but can be distinguished by means of time resolved measurements. The dye molecules bound to gold particles exhibit a mono-exponential decay with a lifetime of 4.5 ns, whereas the dye molecules bound to CdSe/ZnS dots show a nonexponential decay with a slow component of about 135 ns due to the energy transfer from the quantum dots. We demonstrate the fundamental possibility to determine the mixing ratio for dyes with equal luminescence spectra but very different transients. This opens up a pathway independent of the standard optical multiplexing with many different fluorophores emitting from the near ultraviolet to the near infrared spectral region.

  6. Multiplexed measurements by time resolved spectroscopy using colloidal CdSe/ZnS quantum dots

    NASA Astrophysics Data System (ADS)

    Kaiser, U.; Jimenez de Aberasturi, D.; Malinowski, R.; Amin, F.; Parak, W. J.; Heimbrodt, W.

    2014-01-01

    Multiplexed measurements of analytes in parallel is a topical demand in bioanalysis and bioimaging. An interesting alternative to commonly performed spectral multiplexing is lifetime multiplexing. In this Letter, we present a proof of principle of single-color lifetime multiplexing by coupling the same fluorophore to different nanoparticles. The effective lifetime of the fluorophores can be tuned by more than one order of magnitude due to resonance energy transfer from donor states. Measurements have been done on a model systems consisting of ATTO-590 dye molecules linked to either gold particles or to CdSe/ZnS core shell quantum dots. Both systems show the same luminescence spectrum of ATTO-590 dye emission in continuous wave excitation, but can be distinguished by means of time resolved measurements. The dye molecules bound to gold particles exhibit a mono-exponential decay with a lifetime of 4.5 ns, whereas the dye molecules bound to CdSe/ZnS dots show a nonexponential decay with a slow component of about 135 ns due to the energy transfer from the quantum dots. We demonstrate the fundamental possibility to determine the mixing ratio for dyes with equal luminescence spectra but very different transients. This opens up a pathway independent of the standard optical multiplexing with many different fluorophores emitting from the near ultraviolet to the near infrared spectral region.

  7. Multimodal optical studies of single and clustered colloidal quantum dots for the long-term optical property evaluation of quantum dot-based molecular imaging phantoms

    PubMed Central

    Kang, HyeongGon; Clarke, Matthew L.; Lacerda, Silvia H. De Paoli; Karim, Alamgir; Pease, Leonard F.; Hwang, Jeeseong

    2012-01-01

    Understanding the optical properties of clustered quantum dots (QDs) is essential to the design of QD-based optical phantoms for molecular imaging. Single and clustered core/shell colloidal QDs of dimers, trimers, and tetramers are self-assembled, separated, and preferentially collected using electrospray differential mobility analysis (ES-DMA) with electrostatic deposition. Multimodal optical characterization and analysis of their dynamical photoluminescence (PL) properties enables the long-term evaluation of the physicochemical and optical properties of QDs in a single or a clustered state. A multimodal time-correlated spectroscopic confocal microscope capable of simultaneously measuring the time evolution of PL intensity fluctuation, PL lifetime, and emission spectra reveals the long-term dynamic optical properties of interacting QDs in individual dimeric clusters of QDs. This new method will benefit research into the quantitative interpretation of fluorescence intensity and lifetime results in QD-based molecular imaging techniques. The process of photooxidation leads to coupling of the QDs in a dimer, leading to unique optical properties when compared to an isolated QD. These results guide the design and evaluation of QD-based phantom materials for the validation of the PL measurements for quantitative molecular imaging of biological samples labeled with QD probes. PMID:22741078

  8. Superresolution optical fluctuation imaging (SOFI) aided nanomanipulation of quantum dots using AFM for novel artificial arrangements of chemically functionalized colloidal quantum dots and plasmonic structures

    NASA Astrophysics Data System (ADS)

    Dopf, Katja; Heunisch, Sebastian; Schwab, Patrick; Moosmann, Carola; Habermehl, Anne; Lemmer, Uli; Eisler, Hans-Jürgen

    2014-05-01

    For single photon experiments or research on novel hybrid structures consisting of several colloidal quantum dots (Qdots) and plasmonic nanoparticles both the precise localization and the optical behavior of the emitters need to be correlated. Therefore, the gap between the high spatial resolution topography information that provides detailed localization of single Qdots and the diffraction limited fluorescence image needs to be overcome. In this paper, we demonstrate the combination of atomic force microscopy (AFM) with wide-field fluorescence microscopy improved by superresolution optical fluctuation imaging (SOFI). With this approach the topography and the superresolution image can be overlaid with sub-diffraction precision. Consequently, we discriminate between single Qdots that are optically active and dark ones. Additionally, the optical time-dependent behavior of molecular emitters can be selectively investigated. This method is, furthermore, useful for an advanced manipulation and characterization toolbox of Qdots in general. In summary, our findings represent an easily adaptable, highly reproducible and comparatively cheap subdiffraction limit imaging method and they facilitate the efficient selection of bright Qdots in a standard lab environment for proof-of-principle nanostructures containing Qdots and for nanomanipulation experiments.

  9. Mechanisms of fluorescence decays of colloidal CdSe-CdS/ZnS quantum dots unraveled by time-resolved fluorescence measurement.

    PubMed

    Xu, Hao; Chmyrov, Volodymyr; Widengren, Jerker; Brismar, Hjalmar; Fu, Ying

    2015-11-01

    By narrowing the detection bandpass and increasing the signal-to-noise ratio in measuring the time-resolved fluorescence decay spectrum of colloidal CdSe-CdS/ZnS quantum dots (QDs), we show that directly after the photoexcitation, the fluorescence decay spectrum is characterized by a single exponential decay, which represents the energy relaxation of the photogenerated exciton from its initial high-energy state to the ground exciton state. The fluorescence decay spectrum of long decay time is in the form of β/t(2), where β is the radiative recombination time of the ground-state exciton and t is the decay time. Our findings provide us with a direct and quantitative link between fluorescence decay measurement data and fundamental photophysics of QD exciton, thereby leading to a novel way of applying colloidal QDs to study microscopic, physical and chemical processes in many fields including biomedicine. PMID:26426293

  10. Mechanisms of fluorescence decays of colloidal CdSe-CdS/ZnS quantum dots unraveled by time-resolved fluorescence measurement.

    PubMed

    Xu, Hao; Chmyrov, Volodymyr; Widengren, Jerker; Brismar, Hjalmar; Fu, Ying

    2015-11-01

    By narrowing the detection bandpass and increasing the signal-to-noise ratio in measuring the time-resolved fluorescence decay spectrum of colloidal CdSe-CdS/ZnS quantum dots (QDs), we show that directly after the photoexcitation, the fluorescence decay spectrum is characterized by a single exponential decay, which represents the energy relaxation of the photogenerated exciton from its initial high-energy state to the ground exciton state. The fluorescence decay spectrum of long decay time is in the form of β/t(2), where β is the radiative recombination time of the ground-state exciton and t is the decay time. Our findings provide us with a direct and quantitative link between fluorescence decay measurement data and fundamental photophysics of QD exciton, thereby leading to a novel way of applying colloidal QDs to study microscopic, physical and chemical processes in many fields including biomedicine.

  11. Self-diffraction of ultrashort laser pulses under resonant excitation of excitons in a colloidal solution of CdSe/ZnS quantum dots

    NASA Astrophysics Data System (ADS)

    Dneprovskii, V. S.; Kozlova, M. V.; Smirnov, A. M.

    2013-10-01

    We report self-diffraction processes of two types under resonant excitation of the fundamental electron - hole (exciton) transition in a strongly absorbing colloidal solution of CdSe/ZnS quantum dots (QDs) by high-power picosecond laser pulses. In the first case the absorption saturation (bleaching) at the exciton transition frequency and the Stark shift of exciton absorption line lead to the formation of a transparency channel and self-diffraction of the laser beam from the thus induced round diaphragm. In the second case, self-diffraction of two laser beams, intersecting in a cell with a colloidal QD solution, occurs on the diffraction grating induced by these beams. The physical processes responsible for the nonlinear optical properties of CdSe/ZnS QDs and the found selfaction effects are analysed.

  12. Self-diffraction of ultrashort laser pulses under resonant excitation of excitons in a colloidal solution of CdSe/ZnS quantum dots

    SciTech Connect

    Dneprovskii, V S; Kozlova, M V; Smirnov, A M

    2013-10-31

    We report self-diffraction processes of two types under resonant excitation of the fundamental electron – hole (exciton) transition in a strongly absorbing colloidal solution of CdSe/ZnS quantum dots (QDs) by high-power picosecond laser pulses. In the first case the absorption saturation (bleaching) at the exciton transition frequency and the Stark shift of exciton absorption line lead to the formation of a transparency channel and self-diffraction of the laser beam from the thus induced round diaphragm. In the second case, self-diffraction of two laser beams, intersecting in a cell with a colloidal QD solution, occurs on the diffraction grating induced by these beams. The physical processes responsible for the nonlinear optical properties of CdSe/ZnS QDs and the found selfaction effects are analysed. (nonlinear optical phenomena)

  13. Detailed Observation of Multiphoton Emission Enhancement from a Single Colloidal Quantum Dot Using a Silver-Coated AFM Tip.

    PubMed

    Takata, Hiroki; Naiki, Hiroyuki; Wang, Li; Fujiwara, Hideki; Sasaki, Keiji; Tamai, Naoto; Masuo, Sadahiro

    2016-09-14

    The enhancement of multiphoton emission from a single colloidal nanocrystal quantum dot (NQD) interacting with a plasmonic nanostructure was investigated using a silver-coated atomic force microscopy tip (AgTip) as the plasmonic nanostructure. Using the AgTip, which exhibited a well-defined localized surface plasmon (LSP) resonance band, we controlled the spectral overlap and the distance between the single NQD and the AgTip. The emission behavior of the single NQD when approaching the AgTip at the nanometer scale was measured using off-resonance (405 nm) and resonance (465 nm) excitation of the LSP. We directly observed the conversion of the single-photon emission from a single NQD to multiphoton emission with reduction of the emission lifetime at both excitation wavelengths as the NQD-AgTip distance decreased, whereas a decrease and increase in the emission intensity were observed at 405 and 465 nm excitation, respectively. By combining theoretical analysis and the numerical simulation of the AgTip, we deduced that the enhancement of the multiphoton emission was caused by the quenching of the single-exciton state due to the energy transfer from the NQD to the AgTip and that the emission intensity was increased by enhancement of the excitation rate due to the electric field of the LSP on the AgTip. These results provide evidence that the photon statistics and the photon flux from the single NQD can be manipulated by the plasmonic nanostructure through control of the spectral overlap and the distance.

  14. Detailed Observation of Multiphoton Emission Enhancement from a Single Colloidal Quantum Dot Using a Silver-Coated AFM Tip.

    PubMed

    Takata, Hiroki; Naiki, Hiroyuki; Wang, Li; Fujiwara, Hideki; Sasaki, Keiji; Tamai, Naoto; Masuo, Sadahiro

    2016-09-14

    The enhancement of multiphoton emission from a single colloidal nanocrystal quantum dot (NQD) interacting with a plasmonic nanostructure was investigated using a silver-coated atomic force microscopy tip (AgTip) as the plasmonic nanostructure. Using the AgTip, which exhibited a well-defined localized surface plasmon (LSP) resonance band, we controlled the spectral overlap and the distance between the single NQD and the AgTip. The emission behavior of the single NQD when approaching the AgTip at the nanometer scale was measured using off-resonance (405 nm) and resonance (465 nm) excitation of the LSP. We directly observed the conversion of the single-photon emission from a single NQD to multiphoton emission with reduction of the emission lifetime at both excitation wavelengths as the NQD-AgTip distance decreased, whereas a decrease and increase in the emission intensity were observed at 405 and 465 nm excitation, respectively. By combining theoretical analysis and the numerical simulation of the AgTip, we deduced that the enhancement of the multiphoton emission was caused by the quenching of the single-exciton state due to the energy transfer from the NQD to the AgTip and that the emission intensity was increased by enhancement of the excitation rate due to the electric field of the LSP on the AgTip. These results provide evidence that the photon statistics and the photon flux from the single NQD can be manipulated by the plasmonic nanostructure through control of the spectral overlap and the distance. PMID:27501388

  15. Optical nonlinearities of colloidal InP@ZnS core-shell quantum dots probed by Z-scan and two-photon excited emission

    SciTech Connect

    Wawrzynczyk, Dominika; Szeremeta, Janusz; Samoc, Marek; Nyk, Marcin

    2015-11-01

    Spectrally resolved nonlinear optical properties of colloidal InP@ZnS core-shell quantum dots of various sizes were investigated with the Z-scan technique and two-photon fluorescence excitation method using a femtosecond laser system tunable in the range from 750 nm to 1600 nm. In principle, both techniques should provide comparable results and can be interchangeably used for determination of the nonlinear optical absorption parameters, finding maximal values of the cross sections and optimizing them. We have observed slight differences between the two-photon absorption cross sections measured by the two techniques and attributed them to the presence of non-radiative paths of absorption or relaxation. The most significant value of two-photon absorption cross section σ{sub 2} for 4.3 nm size InP@ZnS quantum dot was equal to 2200 GM, while the two-photon excitation action cross section σ{sub 2}Φ was found to be 682 GM at 880 nm. The properties of these cadmium-free colloidal quantum dots can be potentially useful for nonlinear bioimaging.

  16. Spectroscopic manifestations of hybrid association of CdS colloidal quantum dots with J-aggregates of a thiatrimethine cyanine dye

    NASA Astrophysics Data System (ADS)

    Ovchinnikov, O. V.; Smirnov, M. S.; Shapiro, B. I.; Dedikova, A. O.; Shatskikh, T. S.

    2015-11-01

    We have found spectroscopic manifestations of hybrid association in mixtures of CdS colloidal quantum dots with an average size of 2.5-4.2 nm with J-aggregates of pyridinium salt of the 3,3'-di-(γ- sulfopropyl)-9-ethyl-4,5,4',5'-dibenzo-thiacarbocyanine betaine dye that were prepared by the sol-gel method in gelatin. Observed changes of the spectral properties of J-aggregates of dye molecules due to their hybrid association with CdS quantum dots are ensured by steric transformations of dye molecules, which lead to the formation of luminescent trans-J-aggregates. The hybrid association is accompanied by the quenching of the recombination luminescence band of CdS quantum dots (540-640 nm) and by an increase in the luminescence intensity of J-aggregates of dye molecules (670-680 nm). This regularity becomes enhanced with an increase in the ratio of the number of dye molecules to the number of quantum dots [ n dye]: [ n QD] and in the degree of overlap between the luminescence spectrum of quantum dots and the absorption spectrum of J-aggregates, which indicates that there is a resonant nonradiative transfer of the electronic excitation energy from recombination luminescence centers in CdS quantum dots to trans-J-aggregates of dye molecules conjugated to them.

  17. Photoluminescence properties of cadmium-selenide quantum dots embedded in a liquid-crystal polymer matrix

    SciTech Connect

    Tselikov, G. I. Timoshenko, V. Yu.; Plenge, J.; Ruehl, E.; Shatalova, A. M.; Shandryuk, G. A.; Merekalov, A. S.; Tal'roze, R. V.

    2013-05-15

    The photoluminescence properties of cadmium-selenide (CdSe) quantum dots with an average size of {approx}3 nm, embedded in a liquid-crystal polymer matrix are studied. It was found that an increase in the quantum-dot concentration results in modification of the intrinsic (exciton) photoluminescence spectrum in the range 500-600 nm and a nonmonotonic change in its intensity. Time-resolved measurements show the biexponential decay of the photoluminescence intensity with various ratios of fast and slow components depending on the quantum-dot concentration. In this case, the characteristic lifetimes of exciton photoluminescence are 5-10 and 35-50 ns for the fast and slow components, respectively, which is much shorter than the times for colloidal CdSe quantum dots of the same size. The observed features of the photoluminescence spectra and kinetics are explained by the effects of light reabsorption, energy transfer from quantum dots to the liquid-crystal polymer matrix, and the effect of the electronic states at the CdSe/(liquid crystal) interface.

  18. Continuous-wave pumping of multiexciton bands in the photoluminescence spectrum of a single CdTe-CdSe core-shell colloidal quantum dot.

    PubMed

    Osovsky, Ruth; Cheskis, Dima; Kloper, Viki; Sashchiuk, Aldona; Kroner, Martin; Lifshitz, Efrat

    2009-05-15

    Single-exciton, biexciton, triexciton, and quadraexciton bands were resolved in the microphotoluminescence spectrum of a single CdTe/CdSe core-shell colloidal quantum dot, revealing nearly blinking-free behavior. Multiexcitons were generated by a sequential filling of electronic shells with the increase of a continuous-wave excitation power, and their probability was evaluated under steady-state conditions. A partial carriers' delocalization was determined at the core-shell interface, and an exciton binding energy was estimated by a second-order perturbation theory.

  19. Resonant surface-enhanced Raman scattering by optical phonons in a monolayer of CdSe nanocrystals on Au nanocluster arrays

    NASA Astrophysics Data System (ADS)

    Milekhin, Alexander G.; Sveshnikova, Larisa L.; Duda, Tatyana A.; Rodyakina, Ekaterina E.; Dzhagan, Volodymyr M.; Sheremet, Evgeniya; Gordan, Ovidiu D.; Himcinschi, Cameliu; Latyshev, Alexander V.; Zahn, Dietrich R. T.

    2016-05-01

    Here we present the results on an investigation of resonant Stokes and anti- Stokes surface-enhanced Raman scattering (SERS) by optical phonons in colloidal CdSe nanocrystals (NCs) homogeneously deposited on arrays of Au nanoclusters using the Langmuir-Blodgett technology. The thickness of deposited NCs, determined by transmission and scanning electron microscopy, amounts to approximately 1 monolayer. Special attention is paid to the determination of the localized surface plasmon resonance (LSPR) energy in the arrays of Au nanoclusters as a function of the nanocluster size by means of micro-ellipsometry. SERS by optical phonons in CdSe NCs shows a significant enhancement factor with a maximal value of 2 × 103 which depends resonantly on the Au nanocluster size and thus on the LSPR energy. The deposition of CdSe NCs on the arrays of Au nanocluster dimers enabled us to study the polarization dependence of SERS. It was found that a maximal SERS signal is observed for the light polarization along the dimer axis. Finally, SERS by optical phonons was observed for CdSe NCs deposited on the structures with a single Au dimer. A difference of the LO phonon energy is observed for CdSe NCs on different single dimers. This effect is explained as the confinement-induced shift which depends on the CdSe nanocrystal size and indicates quasi-single NC Raman spectra being obtained.

  20. Final Report for DE-FG36-08GO18007 "All-Inorganic, Efficient Photovoltaic Solid State Devices Utilizing Semiconducting Colloidal Nanocrystal Quantum Dots"

    SciTech Connect

    Vladimir Bulovic and Moungi Bawendi

    2011-09-30

    We demonstrated robust colloidal quantum dot (QD) photovoltaics with high internal quantum efficiencies. In our structures, device durability is derived from use of all-inorganic atmospherically-stable semiconducting metal-oxide films together with QD photoreceptors. We have shown that both QD and metal-oxide semiconducting films and contacts are amenable to room temperature processing under minimal vacuum conditions, enabling large area processing of PV structures of high internal efficiency. We generated the state of the art devices with power conversion efficiency of more than 4%, and have shown that efficiencies as high as 9% are achievable in the near-term, and as high as 17% in the long-term.

  1. Air-stable short-wave infrared PbS colloidal quantum dot photoconductors passivated with Al{sub 2}O{sub 3} atomic layer deposition

    SciTech Connect

    Hu, Chen; Gassenq, Alban; Chen, Hongtao; Roelkens, Günther; Justo, Yolanda; Hens, Zeger; Devloo-Casier, Kilian; Detavernier, Christophe

    2014-10-27

    A PbS colloidal quantum dot photoconductor with Al{sub 2}O{sub 3} atomic layer deposition (ALD) passivation for air-stable operation is presented. Two different types of inorganic ligands for the quantum dots, S{sup 2−} and OH{sup −}, are investigated. PbS/S{sup 2−} photoconductors with a cut-off wavelength up to 2.4 μm are obtained, and a responsivity up to 50 A/W at 1550 nm is reported. The corresponding specific detectivity is ∼3.4 × 10{sup 8} Jones at 230 K. The 3-dB bandwidth of the PbS/S{sup 2−} and PbS/OH{sup −} photodetectors is 40 Hz and 11 Hz, respectively.

  2. Application of DNA Aptamers and Quantum Dots to Lateral Flow Test Strips for Detection of Foodborne Pathogens with Improved Sensitivity versus Colloidal Gold

    PubMed Central

    Bruno, John G.

    2014-01-01

    Preliminary studies aimed at improving the sensitivity of foodborne pathogen detection via lateral flow (LF) test strips by use of high affinity DNA aptamers for capture and reporter functions when coupled to red-emitting quantum dots (Qdot 655) are reported. A variety of DNA aptamers developed against Escherichia coli, Listeria monocytogenes, and Salmonella enterica were paired in capture and reporter combinations to determine which yielded the strongest detection of their cognate bacteria using a colloidal gold screening system. Several promising sandwich combinations were identified for each of the three bacterial LF strip systems. The best E. coli aptamer-LF system was further studied and yielded a visible limit of detection (LOD) of ~3,000 E. coli 8739 and ~6,000 E. coli O157:H7 in buffer. These LODs were reduced to ~300–600 bacterial cells per test respectively by switching to a Qdot 655 aptamer-LF system. Novel aspects of these assays such as the use of high levels of detergents to avoid quantum dot agglutination and enhance migration in analytical membranes, identification of optimal analytical membrane types, UV-immobilization of capture aptamers, and novel dual biotin/digoxigenin-end labeled aptamer streptavidin-colloidal gold or -Qdot 655 conjugates plus anti-digoxigenin antibody control lines are also discussed. In general, this work provides proof-of-principle for highly sensitive aptamer-Qdot LF strip assays for rapid foodborne pathogen detection. PMID:25437803

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

    NASA Astrophysics Data System (ADS)

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

    2016-02-01

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

  4. Colloidal Phenomena.

    ERIC Educational Resources Information Center

    Russel, William B.; And Others

    1979-01-01

    Described is a graduate level engineering course offered at Princeton University in colloidal phenomena stressing the physical and dynamical side of colloid science. The course outline, reading list, and requirements are presented. (BT)

  5. Photo-stability and time-resolved photoluminescence study of colloidal CdSe/ZnS quantum dots passivated in Al2O3 using atomic layer deposition

    NASA Astrophysics Data System (ADS)

    Cheng, Chih-Yi; Mao, Ming-Hua

    2016-08-01

    We report photo-stability enhancement of colloidal CdSe/ZnS quantum dots (QDs) passivated in Al2O3 thin film using the atomic layer deposition (ALD) technique. 62% of the original peak photoluminescence (PL) intensity remained after ALD. The photo-oxidation and photo-induced fluorescence enhancement effects of both the unpassivated and passivated QDs were studied under various conditions, including different excitation sources, power densities, and environment. The unpassivated QDs showed rapid PL degradation under high excitation due to strong photo-oxidation in air while the PL intensity of Al2O3 passivated QDs was found to remain stable. Furthermore, recombination dynamics of the unpassivated and passivated QDs were investigated by time-resolved measurements. The average lifetime of the unpassivated QDs decreases with laser irradiation time due to photo-oxidation. Photo-oxidation creates surface defects which reduces the QD emission intensity and enhances the non-radiative recombination rate. From the comparison of PL decay profiles of the unpassivated and passivated QDs, photo-oxidation-induced surface defects unexpectedly also reduce the radiative recombination rate. The ALD passivation of Al2O3 protects QDs from photo-oxidation and therefore avoids the reduction of radiative recombination rate. Our experimental results demonstrated that passivation of colloidal QDs by ALD is a promising method to well encapsulate QDs to prevent gas permeation and to enhance photo-stability, including the PL intensity and carrier lifetime in air. This is essential for the applications of colloidal QDs in light-emitting devices.

  6. Effect of amine addition on the synthesis of CdSe nanocrystals in liquid paraffin via one-pot method

    NASA Astrophysics Data System (ADS)

    Jia, Jinqian; Tian, Jintao; Tian, Weiguo; Mi, Wen; Liu, Xiaoyun; Dai, Jinhui; Wang, Xin

    2014-02-01

    The effect of n-octylamine (OA) and octadecylamine (ODA) addition on the synthesis of CdSe nanocrystals in liquid paraffin via one-pot method is investigated via the measurements of their ultraviolet-visible absorption and fluorescence emission spectra. Our results showed that the in situ added amines can activate the formation reaction of Cd precursor and, as a result, substantially decrease the initial reaction temperature and accelerate the particle growth. By adding OA at high temperature of 200 °C, remarkable improvement on particle quality is achieved, giving relatively narrow size distribution of 33.1 nm and high photoluminescence quantum yield (PLQY) of 81.9% for the CdSe nanoparticles. OA addition at low temperature shows also good quality improvement for the nanoparticles. With regard to the primary amine of ODA, it may be inappropriate for quality improvement of the CdSe nanoparticles from liquid paraffin via one-pot method.

  7. In situ investigation of energy transfer in hybrid organic/colloidal quantum dot light-emitting diodes via magneto-electroluminescence.

    PubMed

    Chen, Lixiang; Chen, Qiusong; Lei, Yanlian; Jia, Weiyao; Yuan, De; Xiong, Zuhong

    2016-08-10

    Energy transfer (ET) and charge injection (CI) in the hybrid organic/colloidal quantum dot light-emitting diodes (QD-LEDs) have been investigated by using magneto-electroluminescence (MEL) as an in situ tool. The feasibility and availability of MEL as an in situ tool were systematically demonstrated in the typical QD-LEDs based on CdSe-ZnS core-shell QDs. Our results suggest that the ET and CI processes can be well discerned by MEL measurements since these two processes exhibit distinct responses to the applied magnetic field. Through measurement of the MEL and current efficiency, we indicated that ET would be the main mechanism for light emission in the present hybrid QD-LEDs. This study strongly suggests that MEL could be a highly sensitive fingerprint for ET, which provides a facile and efficient method for the in situ investigation of fundamental processes in hybrid organic/colloidal QD-LEDs and other organic/inorganic composites. PMID:27461412

  8. White light emitting diode based on InGaN chip with core/shell quantum dots

    NASA Astrophysics Data System (ADS)

    Shen, Changyu; Hong, Yan; Ma, Jiandong; Ming, Jiangzhou

    2009-08-01

    Quantum dots have many applications in optoelectronic device such as LEDs for its many superior properties resulting from the three-dimensional confinement effect of its carrier. In this paper, single chip white light-emitting diodes (WLEDs) were fabricated by combining blue InGaN chip with luminescent colloidal quantum dots (QDs). Two kinds of QDs of core/shell CdSe /ZnS and core/shell/shell CdSe /ZnS /CdS nanocrystals were synthesized by thermal deposition using cadmium oxide and selenium as precursors in a hot lauric acid and hexadecylamine trioctylphosphine oxide hybrid. This two kinds of QDs exhibited high photoluminescence efficiency with a quantum yield more than 41%, and size-tunable emission wavelengths from 500 to 620 nm. The QDs LED mainly consists of flip luminescent InGaN chip, glass ceramic protective coating, glisten cup, QDs using as the photoluminescence material, pyroceram, gold line, electric layer, dielectric layer, silicon gel and bottom layer for welding. The WLEDs had the CIE coordinates of (0.319, 0.32). The InGaN chip white-light-emitting diodes with quantum dots as the emitting layer are potentially useful in illumination and display applications.

  9. Colloidal Synthesis of Quantum Confined Single Crystal CsPbBr3 Nanosheets with Lateral Size Control up to the Micrometer Range

    PubMed Central

    2016-01-01

    We report the nontemplated colloidal synthesis of single crystal CsPbBr3 perovskite nanosheets with lateral sizes up to a few micrometers and with thickness of just a few unit cells (i.e., below 5 nm), hence in the strong quantum confinement regime, by introducing short ligands (octanoic acid and octylamine) in the synthesis together with longer ones (oleic acid and oleylamine). The lateral size is tunable by varying the ratio of shorter ligands over longer ligands, while the thickness is mainly unaffected by this parameter and stays practically constant at 3 nm in all the syntheses conducted at short-to-long ligands volumetric ratio below 0.67. Beyond this ratio, control over the thickness is lost and a multimodal thickness distribution is observed. PMID:27228475

  10. Colloidal Synthesis of Quantum Confined Single Crystal CsPbBr3 Nanosheets with Lateral Size Control up to the Micrometer Range.

    PubMed

    Shamsi, Javad; Dang, Zhiya; Bianchini, Paolo; Canale, Claudio; Stasio, Francesco Di; Brescia, Rosaria; Prato, Mirko; Manna, Liberato

    2016-06-15

    We report the nontemplated colloidal synthesis of single crystal CsPbBr3 perovskite nanosheets with lateral sizes up to a few micrometers and with thickness of just a few unit cells (i.e., below 5 nm), hence in the strong quantum confinement regime, by introducing short ligands (octanoic acid and octylamine) in the synthesis together with longer ones (oleic acid and oleylamine). The lateral size is tunable by varying the ratio of shorter ligands over longer ligands, while the thickness is mainly unaffected by this parameter and stays practically constant at 3 nm in all the syntheses conducted at short-to-long ligands volumetric ratio below 0.67. Beyond this ratio, control over the thickness is lost and a multimodal thickness distribution is observed.

  11. Colloidal Organometal Halide Perovskite (MAPbBrxI3−x, 0≤x≤3) Quantum Dots: Controllable Synthesis and Tunable Photoluminescence

    PubMed Central

    Zhao, Ying; Xu, Xiangxing; You, Xiaozeng

    2016-01-01

    Organic-inorganic perovskite materials, typically methylammonium lead trihalide (MAPbX3: MA = methylammonium; X = Br, I), are recently attract enormous attention for their distinguished photo-electronic properties. The control of morphology, composition and dispersability of MAPbX3 perovskite nanocrystals is crucial for the property tailoring and still a major challenge. Here we report the synthesis of colloidal MAPbBrxI3−x(0 ≤ x ≤ 3) nanocrystals at room temperature by using alkyl carboxylate as capping ligands. These nanocrystals exhibit continuously tunable UV-vis absorption and photoluminescence (PL) across the visible spectrum, which is attributed to the quantum confinement effect with certain stoichiometry. Their unique exciton recombination dynamics was investigated and discussed. PMID:27775023

  12. The design and synthesis of heterostructured quantum dots with dual emission in the visible and infrared

    SciTech Connect

    Lin, Qianglu; Makarov, Nikolay S.; Koh, Weon-kyu; Velizhanin, Kirill A.; Cirloganu, Claudiu M.; Luo, Hongmei; Klimov, Victor I.; Pietryga, Jeffrey M.

    2014-11-26

    The unique optical properties exhibited by visible emitting core/shell quantum dots with especially thick shells are the focus of widespread study, but have yet to be realized in infrared (IR) -active nanostructures. We apply an effective-mass model to identify PbSe/CdSe core/shell quantum dots as a promising system for achieving this goal. We then synthesize colloidal PbSe/CdSe quantum dots with shell thicknesses of up to 4 nm that exhibit unusually slow hole intra-band relaxation from shell to core states, as evidenced by the emergence of dual emission, i.e., IR photoluminescence from the PbSe core observed simultaneously with visible emission from the CdSe shell. In addition to the large shell thickness, the development of slowed intraband relaxation is facilitated by the existence of a sharp core-shell interface without discernible alloying. Growth of thick shells without interfacial alloying or incidental formation of homogenous CdSe nanocrystals was accomplished using insights attained via a systematic study of the dynamics of the cation-exchange synthesis of both PbSe/CdSe as well as the related system PbS/CdS. Finally, we show that the efficiency of the visible photoluminescence can be greatly enhanced by inorganic passivation.

  13. The design and synthesis of heterostructured quantum dots with dual emission in the visible and infrared

    DOE PAGES

    Lin, Qianglu; Makarov, Nikolay S.; Koh, Weon-kyu; Velizhanin, Kirill A.; Cirloganu, Claudiu M.; Luo, Hongmei; Klimov, Victor I.; Pietryga, Jeffrey M.

    2014-11-26

    The unique optical properties exhibited by visible emitting core/shell quantum dots with especially thick shells are the focus of widespread study, but have yet to be realized in infrared (IR) -active nanostructures. We apply an effective-mass model to identify PbSe/CdSe core/shell quantum dots as a promising system for achieving this goal. We then synthesize colloidal PbSe/CdSe quantum dots with shell thicknesses of up to 4 nm that exhibit unusually slow hole intra-band relaxation from shell to core states, as evidenced by the emergence of dual emission, i.e., IR photoluminescence from the PbSe core observed simultaneously with visible emission from themore » CdSe shell. In addition to the large shell thickness, the development of slowed intraband relaxation is facilitated by the existence of a sharp core-shell interface without discernible alloying. Growth of thick shells without interfacial alloying or incidental formation of homogenous CdSe nanocrystals was accomplished using insights attained via a systematic study of the dynamics of the cation-exchange synthesis of both PbSe/CdSe as well as the related system PbS/CdS. Finally, we show that the efficiency of the visible photoluminescence can be greatly enhanced by inorganic passivation.« less

  14. Studying quantum dot blinking through the addition of an engineered inorganic hole trap.

    PubMed

    Tenne, Ron; Teitelboim, Ayelet; Rukenstein, Pazit; Dyshel, Maria; Mokari, Taleb; Oron, Dan

    2013-06-25

    An all-inorganic compound colloidal quantum dot incorporating a highly emissive CdSe core, which is linked by a CdS tunneling barrier to an engineered charge carrier trap composed of PbS, is designed, and its optical properties are studied in detail at the single-particle level. Study of this structure enables a deeper understanding of the link between photoinduced charging and surface trapping of charge carriers and the phenomenon of quantum dot blinking. In the presence of the hole trap, a "gray" emissive state appears, associated with charging of the core. Rapid switching is observed between the "on" and the "gray" state, although the switching dynamics in and out of the dark "off" state remain unaffected. This result completes the links in the causality chain connecting charge carrier trapping, charging of QDs, and the appearance of a "gray" emission state.

  15. Mapping the 3D distribution of CdSe nanocrystals in highly oriented and nanostructured hybrid P3HT-CdSe films grown by directional epitaxial crystallization.

    PubMed

    Roiban, L; Hartmann, L; Fiore, A; Djurado, D; Chandezon, F; Reiss, P; Legrand, J-F; Doyle, S; Brinkmann, M; Ersen, O

    2012-11-21

    Highly oriented and nanostructured hybrid thin films made of regioregular poly(3-hexylthiophene) and colloidal CdSe nanocrystals are prepared by a zone melting method using epitaxial growth on 1,3,5-trichlorobenzene oriented crystals. The structure of the films has been analyzed by X-ray diffraction using synchrotron radiation, electron diffraction and 3D electron tomography to afford a multi-scale structural and morphological description of the highly structured hybrid films. A quantitative analysis of the reconstructed volumes based on electron tomography is used to establish a 3D map of the distribution of the CdSe nanocrystals in the bulk of the films. In particular, the influence of the P3HT-CdSe ratio on the 3D structure of the hybrid layers has been analyzed. In all cases, a bi-layer structure was observed. It is made of a first layer of pure oriented semi-crystalline P3HT grown epitaxially on the TCB substrate and a second P3HT layer containing CdSe nanocrystals uniformly distributed in the amorphous interlamellar zones of the polymer. The thickness of the P3HT layer containing CdSe nanoparticles increases gradually with increasing content of NCs in the films. A growth model is proposed to explain this original transversal organization of CdSe NCs in the oriented matrix of P3HT.

  16. Analysis of the effects of surface chemistry on the XAS spectra of CdSe nanomaterials

    NASA Astrophysics Data System (ADS)

    Whitley, Heather; Prendergast, David; Ogitsu, Tadashi; Schwegler, Eric

    2010-03-01

    X-ray absorption spectroscopy (XAS) is an element-specific probe of local electronic structure, and is an ideal method to analyze chemical bonding. We investigate the consistency of theoretically predicted structures of CdSe nanomaterials with recently measured XAS via ab initio calculations. Using plane-wave DFT, the x-ray absorption cross-section for the Cd L3-edge of small CdSe clusters with a variety of surface ligands is calculated. We also highlight the importance of including excitonic effects in our simulations of core excitation spectra. We compare our simulations to existing experimental data on the ligand dependence of XAS for ligated quantum dots up to ˜3nm in diameter. Based on the favorable comparison of our theoretical spectra with experimental measurements, we infer the validity of our DFT-derived structure and surface passivation for these quantum dots and its relevance to understanding optoelectronic properties of solution-synthesized CdSe nanocrystals. Prepared by LLNL under Contract DE-AC52-07NA27344.

  17. Electric field-induced emission enhancement and modulation in individual CdSe nanowires.

    PubMed

    Vietmeyer, Felix; Tchelidze, Tamar; Tsou, Veronica; Janko, Boldizsar; Kuno, Masaru

    2012-10-23

    CdSe nanowires show reversible emission intensity enhancements when subjected to electric field strengths ranging from 5 to 22 MV/m. Under alternating positive and negative biases, emission intensity modulation depths of 14 ± 7% are observed. Individual wires are studied by placing them in parallel plate capacitor-like structures and monitoring their emission intensities via single nanostructure microscopy. Observed emission sensitivities are rationalized by the field-induced modulation of carrier detrapping rates from NW defect sites responsible for nonradiative relaxation processes. The exclusion of these states from subsequent photophysics leads to observed photoluminescence quantum yield enhancements. We quantitatively explain the phenomenon by developing a kinetic model to account for field-induced variations of carrier detrapping rates. The observed phenomenon allows direct visualization of trap state behavior in individual CdSe nanowires and represents a first step toward developing new optical techniques that can probe defects in low-dimensional materials.

  18. Distance-Dependent Triplet Energy Transfer between CdSe Nanocrystals and Surface Bound Anthracene.

    PubMed

    Li, Xin; Huang, Zhiyuan; Zavala, Ramsha; Tang, Ming Lee

    2016-06-01

    We investigate triplet energy transfer (TET) across variable-length aromatic oligo-p-phenylene and aliphatic bridges in a covalently linked CdSe nanocrystal (NC)-bridge-anthracene hybrid system. Photon upconversion measurements in saturated 9,10-diphenylanthracene hexane solutions under air-free conditions at room temperature provided the steady-state rate of TET (ket) across this interface. For flexible transmitters, ket is similar for different lengths of aliphatic bridges, suggesting that the ligands bend backward. For the rigid phenylene spacer, triplet sensitization of anthracene transmitter molecules by CdSe NCs shows a strong distance dependence, with a Dexter damping coefficient of 0.43 ± 0.07 Å(-1). The anthracene transmitter bound closest to the NC surface gave the highest quantum yield of 14.3% for the conversion of green to violet light, the current record for a hybrid platform. PMID:27164056

  19. Fingerprint detection and using intercalated CdSe nanoparticles on non-porous surfaces.

    PubMed

    Algarra, Manuel; Radotić, Ksenija; Kalauzi, Aleksandar; Mutavdžić, Dragosav; Savić, Aleksandar; Jiménez-Jiménez, José; Rodríguez-Castellón, Enrique; da Silva, Joaquim C G Esteves; Guerrero-González, Juan José

    2014-02-17

    A fluorescent nanocomposite based on the inclusion of CdSe quantum dots in porous phosphate heterostructures, functionalized with amino groups (PPH-NH2@CdSe), was synthesized, characterized and used for fingerprint detection. The main scopes of this work were first to develop a friendly chemical powder for detecting latent fingerprints, especially in non-porous surfaces; their further intercalation in PPH structure enables not to spread the fluorescent nanoparticles, for that reason very good fluorescent images can be obtained. The fingerprints, obtained on different non-porous surfaces such as iron tweezers, mobile telephone screen and magnetic band of a credit card, treated with this powder emit a pale orange luminescence under ultraviolet excitation. A further image processing consists of contrast enhancement that allows obtaining positive matches according to the information supplied from a police database, and showed to be more effective than that obtained with the non-processed images. Experimental results illustrate the effectiveness of proposed methods.

  20. Cryogenic spectroscopy of ultra-low density colloidal lead chalcogenide quantum dots on chip-scale optical cavities towards single quantum dot near-infrared cavity QED

    SciTech Connect

    Bose, Ranojoy; Gao, Feng; McMillan, James F.; Williams, Alex D.; Wong, Chee Wei

    2009-01-01

    We present evidence of cavity quantum electrodynamics from a sparse density of strongly quantum-confined Pb-chalcogenide nanocrystals (between 1 and 10) approaching single-dot levels on moderately high-Q mesoscopic silicon optical cavities. Operating at important near-infrared (1500-nm) wavelengths, large enhancements are observed from devices and strong modifications of the QD emission are achieved. Saturation spectroscopy of coupled QDs is observed at 77K, highlighting the modified nanocrystal dynamics for quantum information processing.

  1. Air-Stable, Near- to Mid-Infrared Emitting Solids of PbTe/CdTe Core-Shell Colloidal quantum dots.

    PubMed

    Protesescu, Loredana; Zünd, Tanja; Bodnarchuk, Maryna I; Kovalenko, Maksym V

    2016-03-01

    Light emitters and detectors operating in the near- and mid-infrared spectral regions are important to many applications, such as telecommunications, high-resolution gas analysis, atmospheric pollution monitoring, medical diagnostics, and night vision. Various lead chalcogenides (binary, ternary, and quaternary alloys) in the form of quantum dots (QDs) or quantum wells provide narrow bandgap energies that cover the broad infrared region corresponding to wavelengths of 1-30 μm. Here, we report an inexpensive, all-solution-based synthesis strategy to thin-film solids consisting of 5-16 nm PbTe QDs encapsulated by CdTe shells. Colloidally synthesized PbTe QDs were first converted into core-shell PbTe/CdTe QDs, and then deposited as thin films. The subsequent fusion of the CdTe shells is achieved by ligand removal and annealing in the presence of CdCl2 . Contrary to highly unstable bare PbTe QDs, PbTe/CdTe QD solids exhibit bright and stable near- to mid-infrared emission at wavelengths of 1-3 μm, which is also retained upon prolonged storage at ambient conditions for one year.

  2. Hybrid nanostructures of well-organized arrays of colloidal quantum dots and a self-assembled monolayer of gold nanoparticles for enhanced fluorescence

    NASA Astrophysics Data System (ADS)

    Liu, Xiaoying; McBride, Sean P.; Jaeger, Heinrich M.; Nealey, Paul F.

    2016-07-01

    Hybrid nanomaterials comprised of well-organized arrays of colloidal semiconductor quantum dots (QDs) in close proximity to metal nanoparticles (NPs) represent an appealing system for high-performance, spectrum-tunable photon sources with controlled photoluminescence. Experimental realization of such materials requires well-defined QD arrays and precisely controlled QD–metal interspacing. This long-standing challenge is tackled through a strategy that synergistically combines lateral confinement and vertical stacking. Lithographically generated nanoscale patterns with tailored surface chemistry confine the QDs into well-organized arrays with high selectivity through chemical pattern directed assembly, while subsequent coating with a monolayer of close-packed Au NPs introduces the plasmonic component for fluorescence enhancement. The results show uniform fluorescence emission in large-area ordered arrays for the fabricated QD structures and demonstrate five-fold fluorescence amplification for red, yellow, and green QDs in the presence of the Au NP monolayer. Encapsulation of QDs with a silica shell is shown to extend the design space for reliable QD/metal coupling with stronger enhancement of 11 times through the tuning of QD–metal spatial separation. This approach provides new opportunities for designing hybrid nanomaterials with tailored array structures and multiple functionalities for applications such as multiplexed optical coding, color display, and quantum transduction.

  3. Hybrid nanostructures of well-organized arrays of colloidal quantum dots and a self-assembled monolayer of gold nanoparticles for enhanced fluorescence

    NASA Astrophysics Data System (ADS)

    Liu, Xiaoying; McBride, Sean P.; Jaeger, Heinrich M.; Nealey, Paul F.

    2016-07-01

    Hybrid nanomaterials comprised of well-organized arrays of colloidal semiconductor quantum dots (QDs) in close proximity to metal nanoparticles (NPs) represent an appealing system for high-performance, spectrum-tunable photon sources with controlled photoluminescence. Experimental realization of such materials requires well-defined QD arrays and precisely controlled QD-metal interspacing. This long-standing challenge is tackled through a strategy that synergistically combines lateral confinement and vertical stacking. Lithographically generated nanoscale patterns with tailored surface chemistry confine the QDs into well-organized arrays with high selectivity through chemical pattern directed assembly, while subsequent coating with a monolayer of close-packed Au NPs introduces the plasmonic component for fluorescence enhancement. The results show uniform fluorescence emission in large-area ordered arrays for the fabricated QD structures and demonstrate five-fold fluorescence amplification for red, yellow, and green QDs in the presence of the Au NP monolayer. Encapsulation of QDs with a silica shell is shown to extend the design space for reliable QD/metal coupling with stronger enhancement of 11 times through the tuning of QD-metal spatial separation. This approach provides new opportunities for designing hybrid nanomaterials with tailored array structures and multiple functionalities for applications such as multiplexed optical coding, color display, and quantum transduction.

  4. Air-Stable, Near- to Mid-Infrared Emitting Solids of PbTe/CdTe Core-Shell Colloidal quantum dots.

    PubMed

    Protesescu, Loredana; Zünd, Tanja; Bodnarchuk, Maryna I; Kovalenko, Maksym V

    2016-03-01

    Light emitters and detectors operating in the near- and mid-infrared spectral regions are important to many applications, such as telecommunications, high-resolution gas analysis, atmospheric pollution monitoring, medical diagnostics, and night vision. Various lead chalcogenides (binary, ternary, and quaternary alloys) in the form of quantum dots (QDs) or quantum wells provide narrow bandgap energies that cover the broad infrared region corresponding to wavelengths of 1-30 μm. Here, we report an inexpensive, all-solution-based synthesis strategy to thin-film solids consisting of 5-16 nm PbTe QDs encapsulated by CdTe shells. Colloidally synthesized PbTe QDs were first converted into core-shell PbTe/CdTe QDs, and then deposited as thin films. The subsequent fusion of the CdTe shells is achieved by ligand removal and annealing in the presence of CdCl2 . Contrary to highly unstable bare PbTe QDs, PbTe/CdTe QD solids exhibit bright and stable near- to mid-infrared emission at wavelengths of 1-3 μm, which is also retained upon prolonged storage at ambient conditions for one year. PMID:26676076

  5. Optical and electrical characterizations of a single step ion beam milling mesa devices of chloride passivated PbS colloidal quantum dots based film

    NASA Astrophysics Data System (ADS)

    Hechster, Elad; Shapiro, Arthur; Lifshitz, Efrat; Sarusi, Gabby

    2016-07-01

    Colloidal Quantum Dots (CQDs) are of increasing interest, thanks to their quantum size effect that gives rise to their usage in various applications, such as biological tagging, solar cells and as the sensitizing layer of night vision devices. Here, we analyze the optical absorbance of chloride passivated PbS CQDs as well as revealing a correlation between their photoluminescence and sizes distribution, using theoretical models and experimental results from the literature. Next, we calculate the CQDs resistivity as a film. Although resistivity can be calculated from sheet resistance measurement using four point probes, such measurement is usually carried-out on the layer's surface that in most cases has dangling bonds and surface states, which might affect the charges flow and modify the resistivity. Therefore; our approach, which was applied in this work, is to extract the actual resistivity from measurements that are performed along the film's thickness (z-direction). For this intent, we fabricated gold capped PbS mesas devices using a single step Ion Beam Milling (IBM) process where we milled the gold and the PbS film continually, and then measured the vertical resistance. Knowing the mesas' dimensions, we calculate the resistivity. To the best of our knowledge, no previous work has extracted, vertically, the resistivity of chloride passivated PbS CQDs using the above method.

  6. A simple and facile synthesis of MPA capped CdSe and CdSe/CdS core/shell nanoparticles

    SciTech Connect

    Sukanya, D.; Sagayaraj, P.

    2015-06-24

    II-VI semiconductor nanostructures, in particular, CdSe quantum dots have drawn a lot of attention because of their promising potential applications in biological tagging, photovoltaic, display devices etc. due to their excellent optical properties, high emission quantum yield, size dependent emission wavelength and high photostability. In this paper, we describe the synthesis and properties of mercaptopropionic acid capped CdSe and CdSe/CdS nanoparticles through a simple and efficient co-precipitation method followed by hydrothermal treatment. The growth process, characterization and the optical absorption as a function of wavelength for the synthesized MPA capped CdSe and CdSe/CdS nanoparticles have been determined using X-ray diffraction study (XRD), Ultraviolet-Visible spectroscopy (UV-Vis), Fourier transform infrared spectroscopy (FT-IR) and High Resolution Transmission Electron Microscopy (HRTEM)

  7. Colloid update.

    PubMed

    Argalious, Maged Y

    2012-01-01

    This update aims to provide an evidence based review of natural and synthetic colloids with a special emphasis on the various generations of the synthetic colloid hydroxyethyl starch. The effect of 1(st), 2(nd) and 3(rd) generation hetastarches on bleeding, coagulopathy, acute kidney injury and mortality will be discussed. The results of randomised controlled trials addressing morbidity and mortality outcomes of colloid versus crystalloid resuscitation in critically ill patients will be described. In addition, the rationale and evidence behind early goal directed fluid therapy (EGDFT) including a practical approach to assessment of dynamic measures of fluid responsiveness will be presented.

  8. Colloidal polypyrrole

    DOEpatents

    Armes, Steven P.; Aldissi, Mahmoud

    1990-01-01

    Processable electrically conductive latex polymer compositions including colloidal particles of an oxidized, polymerized aromatic heterocyclic monomer, a stabilizing effective amount of a vinyl pyridine-containing polymer and dopant anions and a method of preparing such polymer compositions are disclosed.

  9. Hexadecapolar Colloids

    DOE PAGES

    Senyuk, Bohdan; Puls, Owen; Tovkach, Oleh M.; Chernyshuk, Stanislav B.; Smalyukh, Ivan I.

    2016-02-11

    Outermost occupied electron shells of chemical elements can have symmetries resembling that of monopoles, dipoles, quadrupoles and octupoles corresponding to filled s-, p-, d- and forbitals. Theoretically, elements with hexadecapolar outer shells could also exist, but none of the known elements have filled g-orbitals. On the other hand, the research paradigm of ‘colloidal atoms’ displays complexity of particle behaviour exceeding that of atomic counterparts, which is driven by DNA functionalization, geometric shape and topology and weak external stimuli. We describe elastic hexadecapoles formed by polymer microspheres dispersed in a liquid crystal, a nematic fluid of orientationally ordered molecular rods. Becausemore » of conically degenerate boundary conditions, the solid microspheres locally perturb the alignment of the nematic host, inducing hexadecapolar distortions that drive anisotropic colloidal interactions. We uncover physical underpinnings of formation of colloidal elastic hexadecapoles and report the ensuing bonding inaccessible to elastic dipoles, quadrupoles and other nematic colloids studied previously.« less

  10. Hexadecapolar colloids

    PubMed Central

    Senyuk, Bohdan; Puls, Owen; Tovkach, Oleh M.; Chernyshuk, Stanislav B.; Smalyukh, Ivan I.

    2016-01-01

    Outermost occupied electron shells of chemical elements can have symmetries resembling that of monopoles, dipoles, quadrupoles and octupoles corresponding to filled s-, p-, d- and f-orbitals. Theoretically, elements with hexadecapolar outer shells could also exist, but none of the known elements have filled g-orbitals. On the other hand, the research paradigm of ‘colloidal atoms' displays complexity of particle behaviour exceeding that of atomic counterparts, which is driven by DNA functionalization, geometric shape and topology and weak external stimuli. Here we describe elastic hexadecapoles formed by polymer microspheres dispersed in a liquid crystal, a nematic fluid of orientationally ordered molecular rods. Because of conically degenerate boundary conditions, the solid microspheres locally perturb the alignment of the nematic host, inducing hexadecapolar distortions that drive anisotropic colloidal interactions. We uncover physical underpinnings of formation of colloidal elastic hexadecapoles and describe the ensuing bonding inaccessible to elastic dipoles, quadrupoles and other nematic colloids studied previously. PMID:26864184

  11. Ultrafast exciton dynamics and light-driven H2 evolution in colloidal semiconductor nanorods and Pt-tipped nanorods.

    PubMed

    Wu, Kaifeng; Zhu, Haiming; Lian, Tianquan

    2015-03-17

    Colloidal quantum confined one-dimensional (1D) semiconductor nanorods (NRs) and related semiconductor-metal heterostructures are promising new materials for efficient solar-to-fuel conversion because of their unique physical and chemical properties. NRs can simultaneously exhibit quantum confinement effects in the radial direction and bulk like carrier transport in the axial direction. The former implies that concepts well-established in zero-dimensional quantum dots, such as size-tunable energetics and wave function engineering through band alignment in heterostructures, can also be applied to NRs; while the latter endows NRs with fast carrier transport to achieve long distance charge separation. Selective growth of catalytic metallic nanoparticles, such as Pt, at the tips of NRs provides convenient routes to multicomponent heterostructures with photocatalytic capabilities and controllable charge separation distances. The design and optimization of such materials for efficient solar-to-fuel conversion require the understanding of exciton and charge carrier dynamics. In this Account, we summarize our recent studies of ultrafast charge separation and recombination kinetics and their effects on steady-state photocatalytic efficiencies of colloidal CdS and CdSe/CdS NRs and related NR-Pt heterostructures. After a brief introduction of their electronic structure, we discuss exciton dynamics of CdS NRs. By transient absorption and time-resolved photoluminescence decay, it is shown that although the conduction band electrons are long-lived, photogenerated holes in CdS NRs are trapped on an ultrafast time scale (∼0.7 ps), which forms localized excitons due to strong Coulomb interaction in 1D NRs. In quasi-type II CdSe/CdS dot-in-rod NRs, a large valence band offset drives the ultrafast localization of holes to the CdSe core, and the competition between this process and ultrafast hole trapping on a CdS rod leads to three types of exciton species with distinct spatial

  12. Conduction band offset determination between strained CdSe and ZnSe layers using DLTS

    SciTech Connect

    Rangel-Kuoppa, Victor-Tapio

    2013-12-04

    The conduction band offset between strained CdSe layers embedded in unintentionally n-type doped ZnSe is measured and reported. Two samples, consisting of thirty Ultra Thin Quantum Wells (UTQWs) of CdSe embedded in ZnSe, grown by Atomic Layer Epitaxy, are used for this study. The thicknesses of the UTQWs are one and three monolayers (MLs) in each sample, respectively. As expected, the sample with one ML UTQWs does not show any energy level in the UTQWs due to the small thickness of the UTQWs, while the thickness of the sample with 3 ML UTQWs is large enough to form an energy level inside the UTQWs. This energy level appears as a majority trap with an activation energy of 223.58 ± 9.54 meV. This corresponds to UTQWs with barrier heights (the conduction band offset) between 742 meV and 784 meV. These values suggest that the band gap misfit between strained CdSe and ZnSe is around 70.5 to 74 % in the conduction band.

  13. Enhanced emission of charged-exciton polaritons from colloidal quantum dots on a SiN/SiO2 slab waveguide

    PubMed Central

    Xu, Xingsheng; Li, Xingyun

    2015-01-01

    We investigate the photoluminescence (PL) spectra and the time-resolved PL decay process from colloidal quantum dots on SiN/SiO2 wet etched via BOE (HF:NH4F:H2O). The spectrum displays multi-peak shapes that vary with irradiation time. The evolution of the spectral peaks with irradiation time and collection angle demonstrates that the strong coupling of the charged-exciton emission to the leaky modes of the SiN/SiO2 slab waveguide predominantly produces short-wavelength spectral peaks, resulting in multi-peak spectra. We conclude that BOE etching enhances the charged-exciton emission efficiency and its contribution to the total emission compared with the unetched case. BOE etching smoothes the electron confinement potential, thus decreasing the Auger recombination rate. Therefore, the charged-exciton emission efficiency is high, and the charged-exciton-polariton emission can be further enhanced through strong coupling to the leaky mode of the slab waveguide. PMID:25988709

  14. Field-effect transistor-based solution-processed colloidal quantum dot photodetector with broad bandwidth into near-infrared region.

    PubMed

    Yang, Shengyi; Zhao, Na; Zhang, Li; Zhong, Haizheng; Liu, Ruibin; Zou, Bingsuo

    2012-06-29

    We demonstrate a solution-processed colloidal quantum dot (CQDs) photodetector with the configuration of a field-effect transistor (FET), in which the drain and source electrodes are fabricated by a shadow mask. By blending PbS CQDs into the hybrid blend, poly(3-hexylthiophene) (P3HT) and [6,6]-phenyl-C(61)-butyric acid methylester (PCBM), the photosensitive spectrum of the nanocomposite blend is extended into the near-infrared region. A FET-based photodetector ITO/PMMA (180 nm)/P3HT:PCBM:PbS (110 nm)/Al, in which PMMA (polymethylmethacrylate) acts as the dielectric layer and P3HT:PCBM:PbS (in weight ratio of 1:1:1) as the active layer, shows a broad spectral bandwidth, a responsivity of 0.391 mA W(-1) and a specific detectivity of 1.31 × 10(11) Jones are obtained at V(GS) = 1 V under 600 nm illumination with an intensity of 30 μW cm(-2). Therefore, it provides an easy way to fabricate such a FET-based photodetector with a channel length of some hundreds of micrometers by a shadow mask.

  15. Synthesis of CdSe nanocrystals in a noncoordinating solvent: effect of reaction temperature on size and optical properties.

    PubMed

    Nag, Angshuman; Sapra, Sameer; Chakraborty, S; Basu, S; Sarma, D D

    2007-06-01

    Colloidal synthesis of high quality CdSe nanocrystals with controllable size and tunable properties have been one of the most important topics of research over the last decade, in view of its huge technological potentials. CdSe is one of the most studied nanocrystals of this category because of its photoluminescence tunability across the visible spectrum. We have synthesized CdSe nanocrystals using CdO precursor in a noncoordinating solvent and studied the effect of the reaction temperature on the size and optical properties of the nanocrystals. The size of the nanocrystals could be varied systematically in the range of 3.5 to 6.6 nm diameter with a remarkably narrow size distribution by controlling only the reaction temperature, without any need for a post-synthesis processing. The band gap and the corresponding band edge emission could be tuned across the entire visible range by tuning the size of the nanocrystals. The narrow width of the photoluminescence emissions of different colours (blue to red) make these nanocrystals a potential candidate for different optical and optoelectronic devices. PMID:17654973

  16. Influence of pH on the thermo-optic properties of CdSe QDs prepared by a microwave irradiation method

    NASA Astrophysics Data System (ADS)

    Augustine, Anju K.; Girijavallabhan, C. P.; Nampoori, V. P. N.; Kailasnath, M.

    2014-11-01

    In this letter the optical behavior as well as the thermal properties of CdSe quantum dots (QDs) capped with mercapto succinic acid (MSA) are studied and analyzed. CdSe QDs with an average particle size of 7.0 nm are prepared by a microwave irradiation method. The unique structure of MSA plays an important role in determining the PL intensity and better stability by controlling the pH of the medium. A significant increase in thermal diffusivity with pH values is observed with a mode matched thermal lens method. At the optimum value of pH, the surface charge of nanoparticles increases, which increases the repulsive forces. The resulting reduced agglomeration of QDs enhances mobility and improves heat transport. There is a clear correlation between luminous intensity and thermal diffusivity in these nano fluids containing CdSe QDs.

  17. Size effects on Raman spectra of small CdSe nanoparticles in polymer films

    NASA Astrophysics Data System (ADS)

    Dzhagan, V. M.; Valakh, M. Ya; Raevskaya, A. E.; Stroyuk, A. L.; Kuchmiy, S. Ya; Zahn, D. R. T.

    2008-07-01

    The results of a resonant Raman scattering (RRS) study of polymer-stabilized colloidal CdSe nanoparticles (NPs) are reported. The size-selective nature of the RRS is demonstrated by analysing the NP ensembles with different average size \\bar {d} and size distribution Δd using a set of excitation wavelengths. The effect of size selection on the estimation of \\bar {d} and Δd values from the RRS spectra is discussed, as well as some peculiarities of RRS on surface optical phonons. From the experimentally observed small variation of the I2LO/ILO ratio for 2-5 nm NPs a minor effect of \\bar {d} on the electron-phonon coupling strength in this \\bar {d} range is supposed.

  18. Ultralow thermal conductivity in polycrystalline CdSe thin films with controlled grain size.

    PubMed

    Feser, Joseph P; Chan, Emory M; Majumdar, Arun; Segalman, Rachel A; Urban, Jeffrey J

    2013-05-01

    Polycrystallinity leads to increased phonon scattering at grain boundaries and is known to be an effective method to reduce thermal conductivity in thermoelectric materials. However, the fundamental limits of this approach are not fully understood, as it is difficult to form uniform sub-20 nm grain structures. We use colloidal nanocrystals treated with functional inorganic ligands to obtain nanograined films of CdSe with controlled characteristic grain size between 3 and 6 nm. Experimental measurements demonstrate that thermal conductivity in these composites can fall beneath the prediction of the so-called minimum thermal conductivity for disordered crystals. The measurements are consistent, however, with diffuse boundary scattering of acoustic phonons. This apparent paradox can be explained by an overattribution of transport to high-energy phonons in the minimum thermal conductivity model where, in compound semiconductors, optical and zone edge phonons have low group velocity and high scattering rates.

  19. Colloidal polyaniline

    DOEpatents

    Armes, Steven P.; Aldissi, Mahmoud

    1990-01-01

    Processable electrically conductive latex polymer compositions including colloidal particles of an oxidized, polymerized amino-substituted aromatic monomer, a stabilizing effective amount of a random copolymer containing amino-benzene type moieties as side chain constituents, and dopant anions, and a method of preparing such polymer compositions are provided.

  20. Digital Doping in Magic-Sized CdSe Clusters.

    PubMed

    Muckel, Franziska; Yang, Jiwoong; Lorenz, Severin; Baek, Woonhyuk; Chang, Hogeun; Hyeon, Taeghwan; Bacher, Gerd; Fainblat, Rachel

    2016-07-26

    Magic-sized semiconductor clusters represent an exciting class of materials located at the boundary between quantum dots and molecules. It is expected that replacing single atoms of the host crystal with individual dopants in a one-by-one fashion can lead to unique modifications of the material properties. Here, we demonstrate the dependence of the magneto-optical response of (CdSe)13 clusters on the discrete number of Mn(2+) ion dopants. Using time-of-flight mass spectrometry, we are able to distinguish undoped, monodoped, and bidoped cluster species, allowing for an extraction of the relative amount of each species for a specific average doping concentration. A giant magneto-optical response is observed up to room temperature with clear evidence that exclusively monodoped clusters are magneto-optically active, whereas the Mn(2+) ions in bidoped clusters couple antiferromagnetically and are magneto-optically passive. Mn(2+)-doped clusters therefore represent a system where magneto-optical functionality is caused by solitary dopants, which might be beneficial for future solotronic applications. PMID:27420556

  1. Digital Doping in Magic-Sized CdSe Clusters.

    PubMed

    Muckel, Franziska; Yang, Jiwoong; Lorenz, Severin; Baek, Woonhyuk; Chang, Hogeun; Hyeon, Taeghwan; Bacher, Gerd; Fainblat, Rachel

    2016-07-26

    Magic-sized semiconductor clusters represent an exciting class of materials located at the boundary between quantum dots and molecules. It is expected that replacing single atoms of the host crystal with individual dopants in a one-by-one fashion can lead to unique modifications of the material properties. Here, we demonstrate the dependence of the magneto-optical response of (CdSe)13 clusters on the discrete number of Mn(2+) ion dopants. Using time-of-flight mass spectrometry, we are able to distinguish undoped, monodoped, and bidoped cluster species, allowing for an extraction of the relative amount of each species for a specific average doping concentration. A giant magneto-optical response is observed up to room temperature with clear evidence that exclusively monodoped clusters are magneto-optically active, whereas the Mn(2+) ions in bidoped clusters couple antiferromagnetically and are magneto-optically passive. Mn(2+)-doped clusters therefore represent a system where magneto-optical functionality is caused by solitary dopants, which might be beneficial for future solotronic applications.

  2. Quantum chemistry of quantum dots: Effects of ligands and oxidation

    NASA Astrophysics Data System (ADS)

    Inerbaev, Talgat M.; Masunov, Artëm E.; Khondaker, Saiful I.; Dobrinescu, Alexandra; Plamadǎ, Andrei-Valentin; Kawazoe, Yoshiyuki

    2009-07-01

    We report Gaussian basis set density functional theory (DFT) calculations of the structure and spectra of several colloidal quantum dots (QDs) with a (CdSe)n core (n =6,15,17), that are either passivated by trimethylphosphine oxide ligands, or unpassivated and oxidized. From the ground state geometry optimization results we conclude that trimethylphosphine oxide ligands preserve the wurtzite structure of the QDs. Evaporation of the ligands may lead to surface reconstruction. We found that the number of two-coordinated atoms on the nanoparticle's surface is the critical parameter defining the optical absorption properties. For (CdSe)15 wurtzite-derived QD this number is maximal among all considered QDs and the optical absorption spectrum is strongly redshifted compared to QDs with threefold coordinated surface atoms. According to the time-dependent DFT results, surface reconstruction is accompanied by a significant decrease in the linear absorption. Oxidation of QDs destroys the perfection of the QD surface, increases the number of two-coordinated atoms and results in the appearance of an infrared absorption peak close to 700 nm. The vacant orbitals responsible for this near infrared transition have strong Se-O antibonding character. Conclusions of this study may be used in optimization of engineered nanoparticles for photodetectors and photovoltaic devices.

  3. Magnetic study of Fe-doped CdSe nanomaterials

    NASA Astrophysics Data System (ADS)

    Das, Sayantani; Banerjee, Sourish; Sinha, T. P.

    2016-05-01

    Nanoparticles of pure and iron (50 %) doped cadmium selenide (CdSe) have been synthesized by soft chemical route. EDAX analysis supports the inclusion of Fe into CdSe nanoparticles. The average particle size of pure and doped CdSe is found to be ˜50 nm from scanning electron microscopy (SEM). Magnetization of the samples are measured under the field cooled (FC) and zero field cooled (ZFC) modes in the temperature range from 5K to 300K applying a magnetic field of 500Oe. Field dependent magnetization (M-H) measurement indicates presence of room temperature (RT) paramagnetism and low temperature (5K) ferromagnetism of the sample.

  4. Synthesis of Colloidal Quantum Dots Coated with Mercaptosuccinic Acid for Early Detection and Therapeutics of Oral Cancers

    NASA Astrophysics Data System (ADS)

    Jocelin, G.; Arivarasan, A.; Ganesan, M.; Prasad, N. Rajendra; Sasikala, G.

    2016-04-01

    Quantum dots (QDs) are gaining widespread recognition for its luminescence behavior and unique photo physical properties as a bio-marker and inorganic fluorophore. In spite of such rampant advantages, its application is clinically hampered depending on the surface coating decreasing its luminescence efficiency. The present study reports preparation of CdTe QDs capped with biologically active thiol based material, mercaptosuccinic acid (MSA) for diagnosis of oral cancer (KB) cells by acting as a fluorophore marking targeted tumor cells and at the same time exhibiting certain cytotoxic effects. Synthesized MSA coated CdTe QDs is spherical in shape with an average particle size of 3-5nm. In vitro, the rapid uptake of MSA CdTe QDs in oral cancer cell lines were assessed through fluorescence microscopy. Further, this study evaluates the therapeutic efficiency of MSA CdTe QDs in human oral cancer cell lines using MTT analysis. MSA CdTe QDs exhibit significant cytotoxicity in oral cancer cells in a dose dependent manner with low IC50 when compared with other raw CdTe QDs. MSA CdTe QDs were also treated with human lymphocytes (normal cells) to assess and compare the toxicity profile of QDs in normal and oral tumors. The results of our present study strengthen our hypothesis of using MSA CdTe QDs as detector for tracking and fluorescence imaging of oral cancer cells and exhibiting sufficient cytotoxicity in them.

  5. Single-mode lasing from colloidal water-soluble CdSe/CdS quantum dot-in-rods.

    PubMed

    Di Stasio, Francesco; Grim, Joel Q; Lesnyak, Vladimir; Rastogi, Prachi; Manna, Liberato; Moreels, Iwan; Krahne, Roman

    2015-03-18

    Core-shell CdSe/CdS nanocrystals are a very promising material for light emitting applications. Their solution-phase synthesis is based on surface-stabilizing ligands that make them soluble in organic solvents, like toluene or chloroform. However, solubility of these materials in water provides many advantages, such as additional process routes and easier handling. So far, solubilization of CdSe/CdS nanocrystals in water that avoids detrimental effects on the luminescent properties poses a major challenge. This work demonstrates how core-shell CdSe/CdS quantum dot-in-rods can be transferred into water using a ligand exchange method employing mercaptopropionic acid (MPA). Key to maintaining the light-emitting properties is an enlarged CdS rod diameter, which prevents potential surface defects formed during the ligand exchange from affecting the photophysics of the dot-in-rods. Films made from water-soluble dot-in-rods show amplified spontaneous emission (ASE) with a similar threshold (130 μJ/cm(2)) as the pristine material (115 μJ/cm(2)). To demonstrate feasibility for lasing applications, self-assembled microlasers are fabricated via the "coffee-ring effect" that display single-mode operation and a very low threshold of ∼10 μJ/cm(2). The performance of these microlasers is enhanced by the small size of MPA ligands, enabling a high packing density of the dot-in-rods.

  6. Single-mode lasing from colloidal water-soluble CdSe/CdS quantum dot-in-rods.

    PubMed

    Di Stasio, Francesco; Grim, Joel Q; Lesnyak, Vladimir; Rastogi, Prachi; Manna, Liberato; Moreels, Iwan; Krahne, Roman

    2015-03-18

    Core-shell CdSe/CdS nanocrystals are a very promising material for light emitting applications. Their solution-phase synthesis is based on surface-stabilizing ligands that make them soluble in organic solvents, like toluene or chloroform. However, solubility of these materials in water provides many advantages, such as additional process routes and easier handling. So far, solubilization of CdSe/CdS nanocrystals in water that avoids detrimental effects on the luminescent properties poses a major challenge. This work demonstrates how core-shell CdSe/CdS quantum dot-in-rods can be transferred into water using a ligand exchange method employing mercaptopropionic acid (MPA). Key to maintaining the light-emitting properties is an enlarged CdS rod diameter, which prevents potential surface defects formed during the ligand exchange from affecting the photophysics of the dot-in-rods. Films made from water-soluble dot-in-rods show amplified spontaneous emission (ASE) with a similar threshold (130 μJ/cm(2)) as the pristine material (115 μJ/cm(2)). To demonstrate feasibility for lasing applications, self-assembled microlasers are fabricated via the "coffee-ring effect" that display single-mode operation and a very low threshold of ∼10 μJ/cm(2). The performance of these microlasers is enhanced by the small size of MPA ligands, enabling a high packing density of the dot-in-rods. PMID:25335769

  7. Properties of electrospun CdS and CdSe filled poly(methyl methacrylate) (PMMA) nanofibres

    SciTech Connect

    Mthethwa, T.P.; Moloto, M.J.; De Vries, A.; Matabola, K.P.

    2011-04-15

    Graphical abstract: SEM images of CdS/PMMA showing coiling as loading of CdS nanoparticles is increased. Thermal stability is increased with increase in %loading of both CdS and CdSe nanoparticles. Research highlights: {yields} TOPO-capped CdS and HDA-capped CdSe nanoparticles were synthesized and fully characterized. {yields} The nanoparticles were mixed with the polymer, PMMA using electrospinning technique using 2, 5 and 10% weight loadings. {yields} The mixture was spun to produce fibres with optical and thermal properties showing significant change and also the increase in loading causing bending or spiraling. {yields} Both TEM images for nanoparticles and SEM for fibres shows the morphology and sizes of the particles. -- Abstract: Electrospinning technique was used to fabricate poly(methyl methacrylate) (PMMA) fibres incorporating CdS and CdSe quantum dots (nanoparticles). Different nanoparticle loadings (2, 5 and 10 wt% with respect to PMMA) were used and the effect of the quantum dots on the properties of the fibres was studied. The optical properties of the hybrid composite fibres were investigated by photoluminescence and UV-vis spectrophotometry. Scanning electron microscopy (SEM), X-ray diffraction and FTIR spectrophotometry were also used to investigate the morphology and structure of the fibres. The optical studies showed that the size-tunable optical properties can be achieved in the polymer fibres by addition of quantum dots. SEM images showed that the morphologies of the fibres were dependent on the added amounts of quantum dots. A spiral type of morphology was observed with an increase in the concentration of CdS and CdSe nanoparticles. Less beaded structures and bigger diameter fibres were obtained at higher quantum dot concentrations. X-ray diffractometry detected the amorphous peaks of the polymer and even after the quantum dots were added and the FTIR analysis shows that there was no considerable interaction between the quantum dots and the

  8. Probing structure-induced optical behavior in a new class of self-activated luminescent 0D/1D CaWO₄ metal oxide – CdSe nanocrystal composite heterostructures

    SciTech Connect

    Han, Jinkyu; McBean, Coray; Wang, Lei; Hoy, Jessica; Jaye, Cherno; Liu, Haiqing; Li, Zhuo-Qun; Sfeir, Matthew Y.; Fischer, Daniel A.; Taylor, Gordon T.; Misewich, James A.; Wong, Stanislaus S.

    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 complementary 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.

  9. Electronic doping and trap reduction of quantum dots

    NASA Astrophysics Data System (ADS)

    Thorsen, Amanda Leigh

    Both undoped and doped semiconductor quantum dots (QDs) offer unique opportunities for studying the fundamental physics of quantum confinement. Obtaining a thorough understanding of their physical properties is necessary for development of efficient and robust materials for use in a wide range of applications such as optoelectronics (optical switches, light emitting diodes (LEDs), photovoltaics, and lasers), biosensing, and nanoelectronics. This thesis involves studies that look specifically at the effects of electronic doping and trap reduction in undoped and Mn2+ -doped QDs. Investigation of the effect of electron-Mn2+ exchange interactions on Mn 2+ luminescence in Mn2+:CdS nanocrystal films through an electrochemical method reveals effective Auger de-excitation of photoexcited Mn2+. The doped QDs demonstrate increased sensitivity to Auger de-excitation versus undoped QDs due to the long lifetime of the Mn2+ excited state. Photochemical electronic doping of colloidal CdSe nanocrystals is achieved for the first time through the use of a borohydride hole quencher, Li[Et3BH], and the high spectroscopic quality of the resulting n-type nanocrystals allows for advanced characterization by absorption and photoluminescence. Additionally, chemical titrations of the n-type nanocrystals confirm electron accumulation and suggest significant electron trapping for some of the nanocrystals. Spectroelectrochemical measurements on undoped and Mn2+-doped ZnSe QDs target charge injection into traps within the semiconductor bandgap. In both the undoped and doped QDs, transfer of electrons into the nanocrystal film is directly correlated with enhanced photoluminescence quantum yield and dubbed "electrobrightening." This method of brightening through trap passivation is extended to colloidal systems through the use of outer-sphere reductants and ultimately improves the ensemble photoluminescence quantum yield of Mn2+ -doped ZnSe QDs from 14% to 80%.

  10. Bioelectric and Morphological Response of Liquid-Covered Human Airway Epithelial Calu-3 Cell Monolayer to Periodic Deposition of Colloidal 3-Mercaptopropionic-Acid Coated CdSe-CdS/ZnS Core-Multishell Quantum Dots.

    PubMed

    Turdalieva, Aizat; Solandt, Johan; Shambetova, Nestan; Xu, Hao; Blom, Hans; Brismar, Hjalmar; Zelenina, Marina; Fu, Ying

    2016-01-01

    Lung epithelial cells are extensively exposed to nanoparticles present in the modern urban environment. Nanoparticles, including colloidal quantum dots (QDs), are also considered to be potentially useful carriers for the delivery of drugs into the body. It is therefore important to understand the ways of distribution and the effects of the various types of nanoparticles in the lung epithelium. We use a model system of liquid-covered human airway epithelial Calu-3 cell cultures to study the immediate and long-term effects of repeated deposition of colloidal 3-mercaptopropionic-acid coated CdSe-CdS/ZnS core-multishell QDs on the lung epithelial cell surface. By live confocal microscope imaging and by QD fluorescence measurements we show that the QD permeation through the mature epithelial monolayers is very limited. At the time of QD deposition, the transepithelial electrical resistance (TEER) of the epithelial monolayers transiently decreased, with the decrement being proportional to the QD dose. Repeated QD deposition, once every six days for two months, lead to accumulation of only small amounts of the QDs in the cell monolayer. However, it did not induce any noticeable changes in the long-term TEER and the molecular morphology of the cells. The colloidal 3-mercaptopropionic-acid coated CdSe-CdS/ZnS core-multishell QDs could therefore be potentially used for the delivery of drugs intended for the surface of the lung epithelia during limited treatment periods. PMID:26913754

  11. Bioelectric and Morphological Response of Liquid-Covered Human Airway Epithelial Calu-3 Cell Monolayer to Periodic Deposition of Colloidal 3-Mercaptopropionic-Acid Coated CdSe-CdS/ZnS Core-Multishell Quantum Dots.

    PubMed

    Turdalieva, Aizat; Solandt, Johan; Shambetova, Nestan; Xu, Hao; Blom, Hans; Brismar, Hjalmar; Zelenina, Marina; Fu, Ying

    2016-01-01

    Lung epithelial cells are extensively exposed to nanoparticles present in the modern urban environment. Nanoparticles, including colloidal quantum dots (QDs), are also considered to be potentially useful carriers for the delivery of drugs into the body. It is therefore important to understand the ways of distribution and the effects of the various types of nanoparticles in the lung epithelium. We use a model system of liquid-covered human airway epithelial Calu-3 cell cultures to study the immediate and long-term effects of repeated deposition of colloidal 3-mercaptopropionic-acid coated CdSe-CdS/ZnS core-multishell QDs on the lung epithelial cell surface. By live confocal microscope imaging and by QD fluorescence measurements we show that the QD permeation through the mature epithelial monolayers is very limited. At the time of QD deposition, the transepithelial electrical resistance (TEER) of the epithelial monolayers transiently decreased, with the decrement being proportional to the QD dose. Repeated QD deposition, once every six days for two months, lead to accumulation of only small amounts of the QDs in the cell monolayer. However, it did not induce any noticeable changes in the long-term TEER and the molecular morphology of the cells. The colloidal 3-mercaptopropionic-acid coated CdSe-CdS/ZnS core-multishell QDs could therefore be potentially used for the delivery of drugs intended for the surface of the lung epithelia during limited treatment periods.

  12. Bioelectric and Morphological Response of Liquid-Covered Human Airway Epithelial Calu-3 Cell Monolayer to Periodic Deposition of Colloidal 3-Mercaptopropionic-Acid Coated CdSe-CdS/ZnS Core-Multishell Quantum Dots

    PubMed Central

    Turdalieva, Aizat; Solandt, Johan; Shambetova, Nestan; Xu, Hao; Blom, Hans; Brismar, Hjalmar; Zelenina, Marina; Fu, Ying

    2016-01-01

    Lung epithelial cells are extensively exposed to nanoparticles present in the modern urban environment. Nanoparticles, including colloidal quantum dots (QDs), are also considered to be potentially useful carriers for the delivery of drugs into the body. It is therefore important to understand the ways of distribution and the effects of the various types of nanoparticles in the lung epithelium. We use a model system of liquid-covered human airway epithelial Calu-3 cell cultures to study the immediate and long-term effects of repeated deposition of colloidal 3-mercaptopropionic-acid coated CdSe-CdS/ZnS core-multishell QDs on the lung epithelial cell surface. By live confocal microscope imaging and by QD fluorescence measurements we show that the QD permeation through the mature epithelial monolayers is very limited. At the time of QD deposition, the transepithelial electrical resistance (TEER) of the epithelial monolayers transiently decreased, with the decrement being proportional to the QD dose. Repeated QD deposition, once every six days for two months, lead to accumulation of only small amounts of the QDs in the cell monolayer. However, it did not induce any noticeable changes in the long-term TEER and the molecular morphology of the cells. The colloidal 3-mercaptopropionic-acid coated CdSe-CdS/ZnS core-multishell QDs could therefore be potentially used for the delivery of drugs intended for the surface of the lung epithelia during limited treatment periods. PMID:26913754

  13. Soil colloidal behavior

    Technology Transfer Automated Retrieval System (TEKTRAN)

    Recent understanding that organic and inorganic contaminants are often transported via colloidal particles has increased interest in colloid science. The primary importance of colloids in soil science stems from their surface reactivity and charge characteristics. Characterizations of size, shape,...

  14. Ionic Functionalization of Hydrophobic Colloidal Nanoparticles To Form Ionic Nanoparticles with Enzymelike Properties.

    PubMed

    Liu, Yuan; Purich, Daniel L; Wu, Cuichen; Wu, Yuan; Chen, Tao; Cui, Cheng; Zhang, Liqin; Cansiz, Sena; Hou, Weijia; Wang, Yanyue; Yang, Shengyuan; Tan, Weihong

    2015-12-01

    Inorganic colloidal nanoparticles (NPs) stabilized by a layer of hydrophobic surfactant on their surfaces have poor solubility in the aqueous phase, thus limiting their application as biosensors under physiological conditions. Here we report a simple model to ionize various types of hydrophobic colloidal NPs, including FePt, cubic Fe3O4, Pd, CdSe, and NaYF4 (Yb 30%, Er 2%, Nd 1%) NPs, to multicharged (positive and negative) NPs via ligand exchange. Surfaces of neutral hydrophobic NPs were converted to multicharged ions, thus making them soluble in water. Furthermore, peroxidase-like activity was observed for ionic FePt, Fe3O4, Pd, and CdSe NPs, of which FePt and CdSe catalyzed the oxidation of the colorless substrate 3,3',5,5'-tetramethylbenzidine (TMB) to the blue-colored product in the absence of H2O2, while Pd and Fe3O4 catalyzed the oxidization of TMB in the presence of H2O2. With the benefit of the ionic functionalization protocols described herein, colloidal NPs should gain wider use as biomarkers, nanozymes, and biosensors.

  15. Kinetic analysis of the temperature dependence of PbSe colloidal quantum dot photoluminescence: Effects of synthesis process and oxygen exposure

    NASA Astrophysics Data System (ADS)

    Foell, Charles A.; Abel, Keith A.; van Veggel, Frank C. J. M.; Young, Jeff F.

    2014-01-01

    A kinetic model is derived and used to analyze recently published works and new data on the temperature dependence of the spectrally integrated photoluminescence (PL) from thick-film formulations of PbSe colloidal quantum dots (QDs), with particular attention to the effects of air exposure. The model assumes that the excitons thermalize within a ground-state manifold of states and treats the distribution of radiative and nonradiative decay rates within the distribution as generally as possible, while using a minimal number of free parameters. By adjusting the parameters of the model, good fits are obtained for the wide range of integrated PL behaviors reported in [J. Phys. Chem. Lett. 2, 889 (2011), 10.1021/jz2001979; ACS Nano 6, 5498 (2012), 10.1021/nn301405j; Phys. Rev. B 82, 165435 (2010), 10.1103/PhysRevB.82.165435] and the new data presented in this manuscript. By comparing the extracted parameters we deduce the following: (i) All of the samples in the first two references emit from two distinct clusters of states separated by an energy of 55 to 80 meV regardless of air exposure, while there is only one cluster of emissive states that contributes to the emission reported in the third reference. (ii) In the absence of intentional air exposure, the nonradiative decay from all samples can be described by a single Arrhenius-like process. (iii) Although air-exposure effects are reversible in some samples and irreversible in others, the changes in integrated PL behavior brought about by air-exposure forces the introduction of a common, low-activation-energy nonradiative pathway in all cases. (iv) The low-lying emissive cluster of the two-emissive-cluster samples exhibits behavior similar to the single emissive cluster of the other samples. (v) Many hours of air exposure do not trend either the radiative or nonradiative behavior of the dual-emissive-cluster samples towards the behavior of the single-emissive-cluster samples.

  16. Synthesis and Optical Properties of Thiol Functionalized CdSe/ZnS (Core/Shell) Quantum Dots by Ligand Exchange

    SciTech Connect

    Zhu, Huaping; Hu, Michael Z.; Shao, Lei; Yu, Kui; Dabestani, Reza T; Zaman, Md. Badruz; Liao, Dr. Shijun

    2014-03-20

    The colloidal photoluminescent quantum dots (QDs) of CdSe (core) and CdSe/ZnS (core/shell) were synthesized at different temperatures with different growth periods. The optical properties (i.e., UV/Vis spectra and photoluminescent emission spectra) of the resulting QDs were investigated. The CdSe/ZnS QDs exhibited higher photoluminescent (PL) efficiency and stability than their corresponding CdSe core QDs. Ligand exchange with various thiol molecules was performed to replace the initial surface passivation ligands, that is, trioctylphosphine oxide (TOPO) and trioctylphosphine (TOP), and the optical properties of the surface-modified QDs were studied. The thiol ligand molecules used included 1,4-benzenedimethanethiol, 1,16-hexadecanedithiol, 1,11-undecanedithiol, 11-mercapto-1-undecanol, and 1,8 octanedithiol. After the thiol functionalization, the CdSe/ZnS QDs exhibited significantly enhanced PL efficiency and storage stability. Besides surface passivation effect, such enhanced performance of thiol-functionalized QDs could be due to self-assembly formation of dimer/trimer clusters, in which QDs are linked by dithiol molecules. Effects of ligand concentration, type of ligand, and heating on the thiol stabilization of QDs were also discussed.

  17. Synthesis of Colloidal Nanocrystal Heterostructures for High-Efficiency Light Emission

    NASA Astrophysics Data System (ADS)

    Lu, Yifei

    Group II-VI semiconductor nanocrystals, particularly those based on ZnCdS(Se), can be synthesized using well established chemical colloidal processes, and have been a subject of extensive research over the past decade. Their optical properties can be easily tuned through size and composition variations, making them very attractive for many optoelectronic applications including light-emitting diodes (LEDs) and solar cells. Incorporation of diverse internal heterostructures provides an additional means for tuning the optical and electronic properties of conventional ZnCdS(Se) nanocrystals. Extensive bandgap and strain engineering may be applied to the resultant nanocrystal heterostructures to achieve desirable properties and enhanced performance. Despite the high scientific and practical interests of this unique class of nanomaterials, limited efforts have been made to explore their synthesis and potential device applications. This thesis focuses on the synthesis, engineering, characterization, and device demonstration of two types of CdSe-based nanocrystal heterostructures: core/multishell quantum dots (QDs) and QD quantum wells (QDQWs). Their optical properties have been tuned by bandgap and strain engineering to achieve efficient photoluminescence (PL) and electroluminescence (EL).Firstly, yellow light-emitting CdSe QDs with a strain-compensated ZnS/ZnCdS bilayer shell were synthesized using the successive ion layer adsorption and reaction technique and the effects of the shell on the luminescent properties were investigated. The core/shell/shell QDs enjoyed the benefits of excellent exciton confinement by the ZnS intermediate shell and strain compensation by the ZnCdS outer shell, and exhibited 40% stronger PL and a smaller peak redshift upon shell growth compared to conventional CdSe/ZnCdS/ZnS core/shell/shell QDs with an intermediate lattice adaptor. CdSe/ZnS/ZnCdS QD-LEDs had a luminance of 558 cd/m2 at 20 mA/cm 2, 28% higher than that of CdSe/ZnCdS/ZnS QD

  18. Effect of Different Ligands on Carrier Dynamics of CdSe Quatum Dots for Solar Cells Applications

    NASA Astrophysics Data System (ADS)

    Yakami, Baichhabi R.; Togha, Urice; Mahat, Meg; Nandyala, Shashank R.; Balaz, Milan; Pikal, Jon M.; Department of Electrical; Computer Engineering Team; Department of Chemistry Team; Department of Physics Team

    2015-03-01

    We have carried out steady state absorption and photoluminescence (PL), as well as time resolved PL and ultrafast transient absorption (TA) studies of CdSe quantum dots (QD) with five different capping ligands: trioctylphosphine oxide (TOPO), oleic acid (OA), dodecanethiol (DDT), mercaptopropionic acid (MPA), and L-cysteine (Cys). These ligands have different chemical structures and which effects the optical properties of the QDs. Measurements were conducted on QD sizes ranging from Ø = 2.5nm to 4.6nm with smaller QDs showing an excitonic PL and a broad surface trap state PL. The ligand exchange of OA CdSe QDs with MPA, DDT and Cys leads to quenching of excitonic PL intensity accompanied by a larger surface trap state to excitonic PL intensity ratio. This is consistent with the TRPL measurements, which show faster exciton PL decays for CdSe QDs with MPA, DDT and Cys ligands compared to OA and TOPO. The PL decay shows multi-exponential behavior with the average lifetime decreasing with increasing QD size. Data from TA experiments using a white light probe is also used to study the picosecond carrier dynamics. These measurements shed light on the role of capping ligands on the carrier dynamics of the QD used as sensitizers in solar cells. U.S. Department of Energy.

  19. A Rapid and Cost-Effective Laser Based Synthesis of High Purity Cadmium Selenide Quantum Dots.

    PubMed

    Gondall, M A; Qahtan, Talal F; Dastageer, M A; Yamani, Z H; Anjum, D H

    2016-01-01

    A rapid and cost effective method is developed to synthesize high purity cadmium Selenide (CdSe) quantum dots in acetone medium using second harmonic of Nd:YAG nanosecond pulsed laser of 532 nm wavelength. The thermal agglomeration due the nanosecond pulse duration of the laser was successfully eliminated by using unfocussed laser beam and thereby providing a favorable conditions for the synthesis of quantum dots having the grain size of 3 nm. The morphological and optical characterizations like XRD, HRTEM, optical absorption of the synthesized CdSe quantum dots, reveal that the material possesses the similar characteristics of the one synthesized through cumbersome wet chemical methods. Relative to the CdSe bulk material, the synthesized CdSe quantum dots showed a blue shift in the measured band gap energy from near infrared spectral region to visible region, making this material very attractive for many solar energy harvesting applications like photo-catalysis and solar cells. PMID:27398538

  20. Structural and optical properties of solvothermal synthesized nearly monodispersed CdSe nanocrystals

    NASA Astrophysics Data System (ADS)

    Shahi, A. K.; Pandey, B. K.; Singh, B. P.; Gopal, R.

    2016-09-01

    Water soluble nearly monodisperse CdSe nanocrystals have been successfully synthesized via aqueous phase solvothermal route in non ionic surfactant glycolic acid ethoxylate 4-non phenyl ether (GAEPE). X-ray diffraction (XRD), field emission scanning electron microscopy (FESEM) and transmission electron microscopy (TEM) are used to determine the phase, structural parameters such as lattice constants, strain, x-ray density and specific surface area, morphology, shape and size distribution, respectively, whereas optical properties are studied by UV-visible absorption and photoluminescence (PL) spectroscopy. All the diffraction peaks of XRD pattern indexed to wurtzite phase of hexagonal system of CdSe and crystallite sizes estimated to be 13–29 nm along some stronger and narrower peaks which is also consistent with TEM measurement while crystallinity and defects have been analyzed with selective area electron diffraction (SAED) pattern. Optical absorption spectrum shows that the as prepared sample exhibits primary and secondary absorption band centered at 2.15 eV and 1.82 eV, respectively, which is blue shifted as compared to bulk value (1.74 eV) of band gap due to quantum confinement effect. Photoluminescence spectrum shows sharp excitonic emission band centered at 583 nm which is nearer to primary band gap energy.

  1. EDITORIAL: Colloidal suspensions Colloidal suspensions

    NASA Astrophysics Data System (ADS)

    Petukhov, Andrei; Kegel, Willem; van Duijneveldt, Jeroen

    2011-05-01

    Special issue in honour of Henk Lekkerkerker's 65th birthday Professor Henk N W Lekkerkerker is a world-leading authority in the field of experimental and theoretical soft condensed matter. On the occasion of his 65th birthday in the summer of 2011, this special issue celebrates his many contributions to science. Henk Lekkerkerker obtained his undergraduate degree in chemistry at the University of Utrecht (1968) and moved to Calgary where he received his PhD in 1971. He moved to Brussels as a NATO fellow at the Université Libre de Bruxelles and was appointed to an assistant professorship (1974), an associate professorship (1977) and a full professorship (1980) in physical chemistry at the Vrije Universiteit Brussel. In 1985 he returned to The Netherlands to take up a professorship at the Van 't Hoff Laboratory, where he has been ever since. He has received a series of awards during his career, including the Onsager Medal (1999) of the University of Trondheim, the Bakhuys Roozeboom Gold Medal (2003) of the Royal Dutch Academy of Arts and Sciences (KNAW), the ECIS-Rhodia European Colloid and Interface Prize (2003), and the Liquid Matter Prize of the European Physical Society (2008). He was elected a member of KNAW in 1996, was awarded an Academy Chair position in 2005, and has held several visiting lectureships. Henk's work focuses on phase transitions in soft condensed matter, and he has made seminal contributions to both the theoretical and experimental aspects of this field. Here we highlight three major themes running through his work, and a few selected publications. So-called depletion interactions may lead to phase separation in colloid-polymer mixtures, and Henk realised that the partitioning of polymer needs to be taken into account to describe the phase behaviour correctly [1]. Colloidal suspensions can be used as model fluids, with the time- and length-scales involved leading to novel opportunities, notably the direct observation of capillary waves at a

  2. Probing the surface of colloidal nanomaterials with potentiometry in situ.

    PubMed

    Fedin, Igor; Talapin, Dmitri V

    2014-08-13

    Colloidal nanomaterials represent an important branch of modern chemistry. However, we have very little understanding of molecular processes that occur at the nanocrystal (NC) surface during synthesis and post-synthetic modifications. Here we show that potentiometry can be used to study the surface of colloidal NCs under realistic reaction conditions. Potentiometric titrations of CdSe and InP nanostructures provide information on the active surface area, the affinity of ligands to the NC surface, and the surface reaction kinetics. These studies can be carried out at different temperatures in polar and nonpolar media for NCs of different sizes and shapes. In situ potentiometry can provide real-time feedback during synthesis of core-shell nanostructures.

  3. Solution-Processed Transistors Using Colloidal Nanocrystals with Composition-Matched Molecular "Solders": Approaching Single Crystal Mobility.

    PubMed

    Jang, Jaeyoung; Dolzhnikov, Dmitriy S; Liu, Wenyong; Nam, Sooji; Shim, Moonsub; Talapin, Dmitri V

    2015-10-14

    Crystalline silicon-based complementary metal-oxide-semiconductor transistors have become a dominant platform for today's electronics. For such devices, expensive and complicated vacuum processes are used in the preparation of active layers. This increases cost and restricts the scope of applications. Here, we demonstrate high-performance solution-processed CdSe nanocrystal (NC) field-effect transistors (FETs) that exhibit very high carrier mobilities (over 400 cm(2)/(V s)). This is comparable to the carrier mobilities of crystalline silicon-based transistors. Furthermore, our NC FETs exhibit high operational stability and MHz switching speeds. These NC FETs are prepared by spin coating colloidal solutions of CdSe NCs capped with molecular solders [Cd2Se3](2-) onto various oxide gate dielectrics followed by thermal annealing. We show that the nature of gate dielectrics plays an important role in soldered CdSe NC FETs. The capacitance of dielectrics and the NC electronic structure near gate dielectric affect the distribution of localized traps and trap filling, determining carrier mobility and operational stability of the NC FETs. We expand the application of the NC soldering process to core-shell NCs consisting of a III-V InAs core and a CdSe shell with composition-matched [Cd2Se3](2-) molecular solders. Soldering CdSe shells forms nanoheterostructured material that combines high electron mobility and near-IR photoresponse. PMID:26280943

  4. EDITORIAL: Colloidal suspensions Colloidal suspensions

    NASA Astrophysics Data System (ADS)

    Petukhov, Andrei; Kegel, Willem; van Duijneveldt, Jeroen

    2011-05-01

    Special issue in honour of Henk Lekkerkerker's 65th birthday Professor Henk N W Lekkerkerker is a world-leading authority in the field of experimental and theoretical soft condensed matter. On the occasion of his 65th birthday in the summer of 2011, this special issue celebrates his many contributions to science. Henk Lekkerkerker obtained his undergraduate degree in chemistry at the University of Utrecht (1968) and moved to Calgary where he received his PhD in 1971. He moved to Brussels as a NATO fellow at the Université Libre de Bruxelles and was appointed to an assistant professorship (1974), an associate professorship (1977) and a full professorship (1980) in physical chemistry at the Vrije Universiteit Brussel. In 1985 he returned to The Netherlands to take up a professorship at the Van 't Hoff Laboratory, where he has been ever since. He has received a series of awards during his career, including the Onsager Medal (1999) of the University of Trondheim, the Bakhuys Roozeboom Gold Medal (2003) of the Royal Dutch Academy of Arts and Sciences (KNAW), the ECIS-Rhodia European Colloid and Interface Prize (2003), and the Liquid Matter Prize of the European Physical Society (2008). He was elected a member of KNAW in 1996, was awarded an Academy Chair position in 2005, and has held several visiting lectureships. Henk's work focuses on phase transitions in soft condensed matter, and he has made seminal contributions to both the theoretical and experimental aspects of this field. Here we highlight three major themes running through his work, and a few selected publications. So-called depletion interactions may lead to phase separation in colloid-polymer mixtures, and Henk realised that the partitioning of polymer needs to be taken into account to describe the phase behaviour correctly [1]. Colloidal suspensions can be used as model fluids, with the time- and length-scales involved leading to novel opportunities, notably the direct observation of capillary waves at a

  5. An in vitro assessment of the interaction of cadmium selenide quantum dots with DNA, iron, and blood platelets.

    PubMed

    Dunpall, Rekha; Nejo, Adeola Ayodeji; Pullabhotla, Viswanadha Srirama Rajasekhar; Opoku, Andy R; Revaprasadu, Neerish; Shonhai, Addmore

    2012-12-01

    Cadmium selenide (CdSe) quantum dots have gained increased attention for their potential use in biomedical applications. This has raised interest in assessing their toxicity. In this study, water-soluble, cysteine-capped CdSe nanocrystals with an average size of 15 nm were prepared through a one-pot solution-based method. The CdSe nanoparticles were synthesized in batches in which the concentration of the capping agent was varied with the aim of stabilizing the quantum dot core. The effects of the CdSe quantum dots on DNA stability, aggregation of blood platelets, and reducing activity of iron were evaluated in vitro . DNA damage was observed at a concentration of 200 μg/mL of CdSe quantum dots. Furthermore, the CdSe nanocrystals exhibited high reducing power and chelating activity, suggesting that they may impair the function of haemoglobin by interacting with iron. In addition, the CdSe quantum dots promoted aggregation of blood platelets in a dose dependent manner.

  6. Monodispersed spherical colloids of Se@CdSe: synthesis and use as building blocks in fabricating photonic crystals.

    PubMed

    Jeong, Unyong; Kim, Jong-Uk; Xia, Younan; Li, Zhi-Yuan

    2005-05-01

    Monodispersed spherical core-shell colloids of Se@Ag(2)Se have been exploited as a chemical template to synthesize Se@CdSe core-shell particles using a cation-exchange reaction. A small amount of tributylphosphine could facilitate the replacement of Ag(+) by Cd(2+) in methanol at 50 degrees C to complete the conversion within 150 min. The orthorhombic structure of beta-Ag(2)Se changed to a well-defined wurtzite lattice for CdSe. The CdSe shells could be converted back to beta-Ag(2)Se by reacting with AgNO(3) in methanol at room temperature. Because of the uniformity in size and high refractive index associated with the Se@CdSe core-shell colloids, they could serve as a new class of building blocks to fabricate photonic crystals with wide and strong stop bands.

  7. Determining the exact number of dye molecules attached to colloidal CdSe/ZnS quantum dots in Förster resonant energy transfer assemblies

    SciTech Connect

    Kaiser, Uwe; Jimenez de Aberasturi, Dorleta; Vázquez-González, Margarita; Carrillo-Carrion, Carolina; Niebling, Tobias; Parak, Wofgang J.; Heimbrodt, Wolfram

    2015-01-14

    Semiconductor quantum dots functionalized with organic dye molecules are important tools for biological sensor applications. Energy transfer between the quantum dot and the attached dyes can be utilized for sensing. Though important, the determination of the real number of dye molecules attached per quantum dot is rather difficult. In this work, a method will be presented to determine the number of ATTO-590 dye molecules attached to CdSe/ZnS quantum dots based on time resolved spectral analysis. The energy transfer from the excited quantum dot to the attached ATTO-590 dye leads to a reduced lifetime of the quantum dot's excitons. The higher the concentration of dye molecules, the shorter the excitonic lifetime becomes. However, the number of dye molecules attached per quantum dot will vary. Therefore, for correctly explaining the decay of the luminescence upon photoexcitation of the quantum dot, it is necessary to take into account the distribution of the number of dyes attached per quantum dot. A Poisson distribution of the ATTO-590 dye molecules not only leads to excellent agreement between experimental and theoretical decay curves but also additionally yields the average number of dye molecules attached per quantum dot. In this way, the number of dyes per quantum dot can be conveniently determined.

  8. Ligands Slow Down Pure-Dephasing in Semiconductor Quantum Dots.

    PubMed

    Liu, Jin; Kilina, Svetlana V; Tretiak, Sergei; Prezhdo, Oleg V

    2015-09-22

    It is well-known experimentally and theoretically that surface ligands provide additional pathways for energy relaxation in colloidal semiconductor quantum dots (QDs). They increase the rate of inelastic charge-phonon scattering and provide trap sites for the charges. We show that, surprisingly, ligands have the opposite effect on elastic electron-phonon scattering. Our simulations demonstrate that elastic scattering slows down in CdSe QDs passivated with ligands compared to that in bare QDs. As a result, the pure-dephasing time is increased, and the homogeneous luminescence line width is decreased in the presence of ligands. The lifetime of quantum superpositions of single and multiple excitons increases as well, providing favorable conditions for multiple excitons generation (MEG). Ligands reduce the pure-dephasing rates by decreasing phonon-induced fluctuations of the electronic energy levels. Surface atoms are most mobile in QDs, and therefore, they contribute greatly to the electronic energy fluctuations. The mobility is reduced by interaction with ligands. A simple analytical model suggests that the differences between the bare and passivated QDs persist for up to 5 nm diameters. Both low-frequency acoustic and high-frequency optical phonons participate in the dephasing processes in bare QDs, while low-frequency acoustic modes dominate in passivated QDs. The theoretical predictions regarding the pure-dephasing time, luminescence line width, and MEG can be verified experimentally by studying QDs with different surface passivation. PMID:26284384

  9. Piezo-phototronic effect of CdSe nanowires.

    PubMed

    Dong, Lin; Niu, Simiao; Pan, Caofeng; Yu, Ruomeng; Zhang, Yan; Wang, Zhong Lin

    2012-10-23

    The piezo-phototronic effect on transport properties of flexible CdSe NW devices is investigated. An optimum sensitivity of the flexible CdSe NW devices can be achieved by adjusting the applied strain and illumination intensity. The piezo-phototronic effect under compressive strain increases the internal electric field of the Schottky barrier, and assists the separation of the photo-excited electron-hole pairs, resulting in the increase of photocurrent. A trap-mediated mechanism is responsible for the decreased hole separation when the strain is larger than the critical strain.

  10. Colloidal Dispersions

    NASA Astrophysics Data System (ADS)

    Russel, W. B.; Saville, D. A.; Schowalter, W. R.

    1992-03-01

    The book covers the physical side of colloid science from the individual forces acting between submicron particles suspended in a liquid through the resulting equilibrium and dynamic properties. The relevant forces include Brownian motion, electrostatic repulsion, dispersion attraction, both attraction and repulsion due to soluble polymer, and viscous forces due to relative motion between the particles and the liquid. The balance among Brownian motion and the interparticle forces decides the questions of stability and phase behavior. Imposition of external fields produces complex effects, i.e. electrokinetic phenomena (electric field), sedimentation (gravitational field), diffusion (concentration/chemical potential gradient), and non-Newtonian rheology (shear field). The treatment aims to impart a sound, quantitative understanding based on fundamental theory and experiments with well-characterized model systems. This broad grasp of the fundamentals lends insight and helps to develop the intuitive sense needed to isolate essential features of technological problems and design critical experiments. Some exposure to fluid mechanics, statistical mechanics, and electricity and magnetism is assumed, but each subject is reintroduced in a self-contained manner.

  11. Microwave synthesis of CdSe and CdTe nanocrystals in nonabsorbing alkanes.

    PubMed

    Washington, Aaron L; Strouse, Geoffrey F

    2008-07-16

    Controlling nanomaterial growth via the "specific microwave effect" can be achieved by selective heating of the chalcogenide precursor. The high polarizability of the precursor allows instantaneous activation and subsequent nucleation leading to the synthesis of CdSe and CdTe in nonmicrowave absorbing alkane solvents. Regardless of the desired size, narrow dispersity nanocrystals can be isolated in less than 3 min with high quantum efficiencies and elliptical morphologies. The reaction does not require a high temperature injection step, and the alkane solvent can be easily removed. In addition, batch-to-batch variance in size is 4.2 +/- 0.14 nm for 10 repeat experimental runs. The use of a stopped-flow reactor allows near continuous automation of the process leading to potential industrial benefits.

  12. Microwave synthesis of CdSe and CdTe nanocrystals in nonabsorbing alkanes.

    PubMed

    Washington, Aaron L; Strouse, Geoffrey F

    2008-07-16

    Controlling nanomaterial growth via the "specific microwave effect" can be achieved by selective heating of the chalcogenide precursor. The high polarizability of the precursor allows instantaneous activation and subsequent nucleation leading to the synthesis of CdSe and CdTe in nonmicrowave absorbing alkane solvents. Regardless of the desired size, narrow dispersity nanocrystals can be isolated in less than 3 min with high quantum efficiencies and elliptical morphologies. The reaction does not require a high temperature injection step, and the alkane solvent can be easily removed. In addition, batch-to-batch variance in size is 4.2 +/- 0.14 nm for 10 repeat experimental runs. The use of a stopped-flow reactor allows near continuous automation of the process leading to potential industrial benefits. PMID:18576624

  13. Effect of cadmium selenide quantum dots on the dielectric and physical parameters of ferroelectric liquid crystal

    SciTech Connect

    Singh, D. P.; Gupta, S. K.; Manohar, R.; Varia, M. C.; Kumar, S.; Kumar, A.

    2014-07-21

    The effect of cadmium selenide quantum dots (CdSe QDs) on the dielectric relaxation and material constants of a ferroelectric liquid crystal (FLC) has been investigated. Along with the characteristic Goldstone mode, a new relaxation mode has been induced in the FLC material due to the presence of CdSe QDs. This new relaxation mode is strongly dependent on the concentration of CdSe QDs but is found to be independent of the external bias voltage and temperature. The material constants have also been modified remarkably due to the presence of CdSe QDs. The appearance of this new relaxation phenomenon has been attributed to the concentration dependent interaction between CdSe QDs and FLC molecules.

  14. Million Atom Pseudopotential Manybody Theory of Electronic Structure and Spectroscopy of Semiconductor Quantum Dots

    NASA Astrophysics Data System (ADS)

    Zunger, Alex

    2003-03-01

    Semiconductor Quantum Dots that are of sufficient structural quality (good crystallinity, surface passivation, size uniformity) to produce ultra sharp spectroscopic lines worthy of a detailed theoretical effort tend to be rather BIG, containing thousands to million atoms. Yet, in this size regime, the only theoretical methods available are effective-mass based, particle-in-a-box approaches, that neglect multi-band and inter-valley coupling, leading to significant qualitative errors.(A. Zunger,Phys. Stat. Sol. (a) 190), 467 (2002). While LDA-based methods are capable of solving the Single-Particle problem even for ˜1,000 atom dots, the all important many-body problem can be currently addressed only for considerably smaller dots. I will present here a computational alternative which addresses both the single-particle and the Manybody parts of the problem for 10^3 to 10^6 atom dots .The method is applicable both to ``free Standing" (e.g. colloidal) dots of CdSe, InP, InAs and Si, as well as to the strained, ``self-assembled" epitaxial dots of, e.g., InGaAs/GaAs. It is based on a ``Linear Combination of Bulk Bands" (LCBB) approach that expands the dot states in terms of plane wave based (pseudopotential) Bloch states throughout the Brillouin zone. The manybody part is treated via Configuration Interaction. I will illustrate how this method addresses some of the recent striking experimental observations on semiconductor quantum dots:(i) Scaling laws for band gaps and exchange interactions (ii) Rapid Auger transitions in colloidal dots (iii) Coulomb Blocade and Spin Blockade in colloidal dots (iv) Charged Excitons (e.g. Trions) in Self-assembled dots, and (v) excitonic Fine-Structure in self assembled dots.

  15. Colloids: current recommendations.

    PubMed

    Chan, Daniel L

    2008-05-01

    Colloids are increasingly becoming considered indispensable in the management of critically ill patients. Typical indications for colloid administration include patients with tissue edema, hypovolemia, and low oncotic pressure. Current guidelines for the use of colloids in veterinary patients balance the purported benefits of colloid fluid administration with the potential risks, such as volume overload and coagulation disturbances. This article focuses primarily on hydroxyethyl starches, because they are the most commonly used colloid in veterinary practice, and because recent advances in colloid therapy have been achieved with this colloid. Newer colloids have been modified to limit effects on the coagulation system, and they may be used to modulate the inflammatory response, which could prove to be particularly useful in the management of critically ill patients. A better understanding of how different fluids influence the host response may enable us to explore new applications of fluid replacement therapy beyond simply replenishing volume deficits.

  16. Atomistic description of thiostannate-capped CdSe nanocrystals: retention of four-coordinate SnS4 motif and preservation of Cd-rich stoichiometry.

    PubMed

    Protesescu, Loredana; Nachtegaal, Maarten; Voznyy, Oleksandr; Borovinskaya, Olga; Rossini, Aaron J; Emsley, Lyndon; Copéret, Christophe; Günther, Detlef; Sargent, Edward H; Kovalenko, Maksym V

    2015-02-11

    Colloidal semiconductor nanocrystals (NCs) are widely studied as building blocks for novel solid-state materials. Inorganic surface functionalization, used to displace native organic capping ligands from NC surfaces, has been a major enabler of electronic solid-state devices based on colloidal NCs. At the same time, very little is known about the atomistic details of the organic-to-inorganic ligand exchange and binding motifs at the NC surface, severely limiting further progress in designing all-inorganic NCs and NC solids. Taking thiostannates (K4SnS4, K4Sn2S6, K6Sn2S7) as typical examples of chalcogenidometallate ligands and oleate-capped CdSe NCs as a model NC system, in this study we address these questions through the combined application of solution (1)H NMR spectroscopy, solution and solid-state (119)Sn NMR spectroscopy, far-infrared and X-ray absorption spectroscopies, elemental analysis, and by DFT modeling. We show that through the X-type oleate-to-thiostannate ligand exchange, CdSe NCs retain their Cd-rich stoichiometry, with a stoichiometric CdSe core and surface Cd adatoms serving as binding sites for terminal S atoms of the thiostannates ligands, leading to all-inorganic (CdSe)core[Cdm(Sn2S7)yK(6y-2m)]shell (taking Sn2S7(6-) ligand as an example). Thiostannates SnS4(4-) and Sn2S7(6-) retain (distorted) tetrahedral SnS4 geometry upon binding to NC surface. At the same time, experiments and simulations point to lower stability of Sn2S6(4-) (and SnS3(2-)) in most solvents and its lower adaptability to the NC surface caused by rigid Sn2S2 rings.

  17. Atomistic Description of Thiostannate-Capped CdSe Nanocrystals: Retention of Four-Coordinate SnS4 Motif and Preservation of Cd-Rich Stoichiometry

    PubMed Central

    2016-01-01

    Colloidal semiconductor nanocrystals (NCs) are widely studied as building blocks for novel solid-state materials. Inorganic surface functionalization, used to displace native organic capping ligands from NC surfaces, has been a major enabler of electronic solid-state devices based on colloidal NCs. At the same time, very little is known about the atomistic details of the organic-to-inorganic ligand exchange and binding motifs at the NC surface, severely limiting further progress in designing all-inorganic NCs and NC solids. Taking thiostannates (K4SnS4, K4Sn2S6, K6Sn2S7) as typical examples of chalcogenidometallate ligands and oleate-capped CdSe NCs as a model NC system, in this study we address these questions through the combined application of solution 1H NMR spectroscopy, solution and solid-state 119Sn NMR spectroscopy, far-infrared and X-ray absorption spectroscopies, elemental analysis, and by DFT modeling. We show that through the X-type oleate-to-thiostannate ligand exchange, CdSe NCs retain their Cd-rich stoichiometry, with a stoichiometric CdSe core and surface Cd adatoms serving as binding sites for terminal S atoms of the thiostannates ligands, leading to all-inorganic (CdSe)core[Cdm(Sn2S7)yK(6y-2m)]shell (taking Sn2S76– ligand as an example). Thiostannates SnS44– and Sn2S76– retain (distorted) tetrahedral SnS4 geometry upon binding to NC surface. At the same time, experiments and simulations point to lower stability of Sn2S64– (and SnS32–) in most solvents and its lower adaptability to the NC surface caused by rigid Sn2S2 rings. PMID:25597625

  18. What Is a Colloid?

    ERIC Educational Resources Information Center

    Lamb, William G.

    1985-01-01

    Describes the properties of colloids, listing those commonly encountered (such as whipped cream, mayonnaise, and fog). Also presents several experiments using colloids and discusses "Silly Putty," a colloid with viscoelastic properties whose counterintuitive properties result from its mixture of polymers. (DH)

  19. Photogenerated excitons in plain core CdSe nanocrystals with unity radiative decay in single channel: the effects of surface and ligands.

    PubMed

    Gao, Yuan; Peng, Xiaogang

    2015-04-01

    A systematic and reproducible method was developed to study the decay dynamics of an exciton, a photogenerated electron-hole pair, in semiconductor nanocrystals in solution. Results revealed that the excitons in plain core CdSe nanocrystals in either zinc-blende or wurtzite or mixed lattice structures could be reproducibly prepared to decay radiatively in unity quantum yield and in single channel. The single-channel lifetime was found to increase monotonically by increasing size of the CdSe nanocrystals, with zinc-blende ones increasing in a relatively slow pace. Surface inorganic stoichiometry was found to be a sensitive parameter to affect the exciton decay dynamics for all crystal structures with different sizes. Excess Se (Cd) sites on the surface were found to induce short (long) lifetime channels for the excitons. Both types of traps reduced the quantum yield of the radiative decay of the excitons, and the hole traps associated with Se sites were nearly not emissive. With optimal surface inorganic stoichiometry, primary amines were identified as "ideal" organic ligands for CdSe core nanocrystals to achieve unity radiative decay of excitons in single channel in comparison to other types of neutral ligands commonly applied in the field.

  20. The influence of applied magnetic fields on the optical properties of zero- and one-dimensional CdSe nanocrystals.

    PubMed

    Blumling, Daniel E; McGill, Stephen; Knappenberger, Kenneth L

    2013-10-01

    Shape-dependent exciton relaxation dynamics of CdSe 0-D nanocrystals and 1-D nanorods were studied using low-temperature (4.2 K), time-resolved and intensity-integrated magneto-photoluminscence (MPL) spectroscopy. Analysis of the average MPL rate constants from several different nanocrystal quantum dots and rods excited by 400 nm light in applied magnetic fields up to 17.5 T revealed size-dependent energy gaps separating bright and dark exciton fine-structure states. For 1-D nanorods under strong cross-sectional confinement and large length-to-diameter aspect ratios, efficient mixing of bright and dark exciton states was achieved using relatively low applied field strengths (≤4 T). The effect was attributed, in part, to decreased confinement of CdSe hole states associated with the long axis of the nanorod, which resulted in reduction of the energy gaps separating the bright and dark states. Increased control over the angle formed between the applied field vectors and the nanocrystal c-axis led to more efficient and uniform mixing of nanorod exciton states than for quantum dots. The findings suggest 1-D nanostructures are advantageous over 0-D ones for field-responsive applications. PMID:23945622

  1. Electrohydrodynamically patterned colloidal crystals

    NASA Technical Reports Server (NTRS)

    Hayward, Ryan C. (Inventor); Poon, Hak F. (Inventor); Xiao, Yi (Inventor); Saville, Dudley A. (Inventor); Aksay, Ilhan A. (Inventor)

    2003-01-01

    A method for assembling patterned crystalline arrays of colloidal particles using ultraviolet illumination of an optically-sensitive semiconducting anode while using the anode to apply an electronic field to the colloidal particles. The ultraviolet illumination increases current density, and consequently, the flow of the colloidal particles. As a result, colloidal particles can be caused to migrate from non-illuminated areas of the anode to illuminated areas of the anode. Selective illumination of the anode can also be used to permanently affix colloidal crystals to illuminated areas of the anode while not affixing them to non-illuminated areas of the anode.

  2. Microfluidic colloid filtration

    PubMed Central

    Linkhorst, John; Beckmann, Torsten; Go, Dennis; Kuehne, Alexander J. C.; Wessling, Matthias

    2016-01-01

    Filtration of natural and colloidal matter is an essential process in today’s water treatment processes. The colloidal matter is retained with the help of micro- and nanoporous synthetic membranes. Colloids are retained in a “cake layer” – often coined fouling layer. Membrane fouling is the most substantial problem in membrane filtration: colloidal and natural matter build-up leads to an increasing resistance and thus decreasing water transport rate through the membrane. Theoretical models exist to describe macroscopically the hydrodynamic resistance of such transport and rejection phenomena; however, visualization of the various phenomena occurring during colloid retention is extremely demanding. Here we present a microfluidics based methodology to follow filter cake build up as well as transport phenomena occuring inside of the fouling layer. The microfluidic colloidal filtration methodology enables the study of complex colloidal jamming, crystallization and melting processes as well as translocation at the single particle level. PMID:26927706

  3. Saturated Zone Colloid Transport

    SciTech Connect

    H. Viswanathan; P. Reimus

    2003-09-05

    Colloid retardation is influenced by the attachment and detachment of colloids from immobile surfaces. This analysis demonstrates the development of parameters necessary to estimate attachment and detachment of colloids and, hence, retardation in both fractured tuff and porous alluvium. Field and experimental data specific to fractured tuff are used for the analysis of colloid retardation in fractured tuff. Experimental data specific to colloid transport in alluvial material from Yucca Mountain as well as bacteriophage field studies in alluvial material, which are thought to be good analogs for colloid transport, are used to estimate attachment and detachment of colloids in the alluvial material. There are no alternative scientific approaches or technical methods for calculating these retardation factors.

  4. Microfluidic colloid filtration

    NASA Astrophysics Data System (ADS)

    Linkhorst, John; Beckmann, Torsten; Go, Dennis; Kuehne, Alexander J. C.; Wessling, Matthias

    2016-03-01

    Filtration of natural and colloidal matter is an essential process in today’s water treatment processes. The colloidal matter is retained with the help of micro- and nanoporous synthetic membranes. Colloids are retained in a “cake layer” – often coined fouling layer. Membrane fouling is the most substantial problem in membrane filtration: colloidal and natural matter build-up leads to an increasing resistance and thus decreasing water transport rate through the membrane. Theoretical models exist to describe macroscopically the hydrodynamic resistance of such transport and rejection phenomena; however, visualization of the various phenomena occurring during colloid retention is extremely demanding. Here we present a microfluidics based methodology to follow filter cake build up as well as transport phenomena occuring inside of the fouling layer. The microfluidic colloidal filtration methodology enables the study of complex colloidal jamming, crystallization and melting processes as well as translocation at the single particle level.

  5. Microfluidic colloid filtration.

    PubMed

    Linkhorst, John; Beckmann, Torsten; Go, Dennis; Kuehne, Alexander J C; Wessling, Matthias

    2016-01-01

    Filtration of natural and colloidal matter is an essential process in today's water treatment processes. The colloidal matter is retained with the help of micro- and nanoporous synthetic membranes. Colloids are retained in a "cake layer"--often coined fouling layer. Membrane fouling is the most substantial problem in membrane filtration: colloidal and natural matter build-up leads to an increasing resistance and thus decreasing water transport rate through the membrane. Theoretical models exist to describe macroscopically the hydrodynamic resistance of such transport and rejection phenomena; however, visualization of the various phenomena occurring during colloid retention is extremely demanding. Here we present a microfluidics based methodology to follow filter cake build up as well as transport phenomena occuring inside of the fouling layer. The microfluidic colloidal filtration methodology enables the study of complex colloidal jamming, crystallization and melting processes as well as translocation at the single particle level. PMID:26927706

  6. Spontaneous emission of semiconductor quantum dots in inverse opal SiO2 photonic crystals at different temperatures.

    PubMed

    Yang, Peng; Yang, Yingshu; Wang, Yinghui; Gao, Jiechao; Sui, Ning; Chi, Xiaochun; Zou, Lu; Zhang, Han-Zhuang

    2016-02-01

    The photoluminescence (PL) characteristics of CdSe quantum dots (QDs) infiltrated into inverse opal SiO2 photonic crystals (PCs) are systemically studied. The special porous structure of inverse opal PCs enhanced the thermal exchange rate between the CdSe QDs and their surrounding environment. Finally, inverse opal SiO2 PCs suppressed the nonlinear PL enhancement of CdSe QDs in PCs excited by a continuum laser and effectively modulated the PL characteristics of CdSe QDs in PCs at high temperatures in comparison with that of CdSe QDs out of PCs. The final results are of benefit in further understanding the role of inverse opal PCs on the PL characteristics of QDs. PMID:26781789

  7. Spontaneous emission of semiconductor quantum dots in inverse opal SiO2 photonic crystals at different temperatures.

    PubMed

    Yang, Peng; Yang, Yingshu; Wang, Yinghui; Gao, Jiechao; Sui, Ning; Chi, Xiaochun; Zou, Lu; Zhang, Han-Zhuang

    2016-02-01

    The photoluminescence (PL) characteristics of CdSe quantum dots (QDs) infiltrated into inverse opal SiO2 photonic crystals (PCs) are systemically studied. The special porous structure of inverse opal PCs enhanced the thermal exchange rate between the CdSe QDs and their surrounding environment. Finally, inverse opal SiO2 PCs suppressed the nonlinear PL enhancement of CdSe QDs in PCs excited by a continuum laser and effectively modulated the PL characteristics of CdSe QDs in PCs at high temperatures in comparison with that of CdSe QDs out of PCs. The final results are of benefit in further understanding the role of inverse opal PCs on the PL characteristics of QDs.

  8. van der Waals epitaxy and photoresponse of two-dimensional CdSe plates

    NASA Astrophysics Data System (ADS)

    Zhu, Dan-Dan; Xia, Jing; Wang, Lei; Li, Xuan-Ze; Tian, Li-Feng; Meng, Xiang-Min

    2016-06-01

    Here we demonstrate the first growth of two-dimensional (2D) single-crystalline CdSe plates on mica substrates via van der Waals epitaxy. The as-synthesized 2D plates exhibit hexagonal, truncated triangular and triangular shapes with the lateral size around several microns. Photodetectors based on 2D CdSe plates present a fast response time of 24 ms, revealing that 2D CdSe is a promising building block for ultrathin optoelectronic devices.

  9. Saturated Zone Colloid Transport

    SciTech Connect

    H. S. Viswanathan

    2004-10-07

    This scientific analysis provides retardation factors for colloids transporting in the saturated zone (SZ) and the unsaturated zone (UZ). These retardation factors represent the reversible chemical and physical filtration of colloids in the SZ. The value of the colloid retardation factor, R{sub col} is dependent on several factors, such as colloid size, colloid type, and geochemical conditions (e.g., pH, Eh, and ionic strength). These factors are folded into the distributions of R{sub col} that have been developed from field and experimental data collected under varying geochemical conditions with different colloid types and sizes. Attachment rate constants, k{sub att}, and detachment rate constants, k{sub det}, of colloids to the fracture surface have been measured for the fractured volcanics, and separate R{sub col} uncertainty distributions have been developed for attachment and detachment to clastic material and mineral grains in the alluvium. Radionuclides such as plutonium and americium sorb mostly (90 to 99 percent) irreversibly to colloids (BSC 2004 [DIRS 170025], Section 6.3.3.2). The colloid retardation factors developed in this analysis are needed to simulate the transport of radionuclides that are irreversibly sorbed onto colloids; this transport is discussed in the model report ''Site-Scale Saturated Zone Transport'' (BSC 2004 [DIRS 170036]). Although it is not exclusive to any particular radionuclide release scenario, this scientific analysis especially addresses those scenarios pertaining to evidence from waste-degradation experiments, which indicate that plutonium and americium may be irreversibly attached to colloids for the time scales of interest. A section of this report will also discuss the validity of using microspheres as analogs to colloids in some of the lab and field experiments used to obtain the colloid retardation factors. In addition, a small fraction of colloids travels with the groundwater without any significant retardation

  10. Photodoping of Colloidal Nanocrystals

    NASA Astrophysics Data System (ADS)

    Cohn, Alicia W.

    This dissertation addresses various aspects of photodoping colloidal nanocrystals. Photodoped ZnO nanocrystals were found to be versatile tuneable reducers using both quantum confinement and band-gap engineering with Mg2+ doping to change the conduction band potential. Using photoluminescence of the visible trap and magnetic circular dichroism spectroscopy of Mg2+ and Mn2+ co-doped ZnO, Mg2+ was shown to change the potential of both the conduction and valence band in a ratio of 0.68:0.32. The hole scavenging reaction using ethanol as the hole scavenger was investigated using continuous-wave and time resolved photoluminescence of the visible trap state of ZnO. The reaction was found to occur between the valence band hole and with a rate of > 15 ps-1. Quenching of the ZnO visible trap luminescence upon photodoping was shown to be due to trap/electron Auger process while the concomitant enhancement of the UV band-gap emission was hypothesized to be due to a reduction in non-radiative processes due to extra electrons in the conduction-band. The trap/electron Auger process in ZnO nanocrystals was further characterized by a size-dependence and shown to scale with R2. Another previously unknown Auger size dependence was measured in CdSe/ZnS trions and shown to scale with R4.3.

  11. A detailed examination of the growth of CdSe thin films through structural and optical characterization

    SciTech Connect

    Yükselici, M.H.; Aşıkoğlu Bozkurt, A.; Ömür, B. Can

    2013-07-15

    Highlights: ► Urbach tail width decreases by about 200 meV with the film thickness. ► A coefficient of strain of around 3 × 10{sup −3} along [0 0 2] axis was predicted. ► Compressive strain gives rise to about 11 meV red shift in the band gap energy. ► A relative shift of about 2 cm{sup −1} of LO{sub 1} phonon mode in Raman spectra was observed between different thickness films. - Abstract: Different thickness CdSe thin films were grown on glass substrates by physical vapor deposition and characterized by optical and structural investigations. Urbach energy related to the width of the optical absorption tail decreases from 430 meV for a film thickness of 50 nm to 200 meV for 450 nm. The film thickness dependent grain sizes were estimated by using effective mass model under quantum size effect from the shift of around 500 meV in the asymptotic absorption edge. The X-ray diffraction (XRD) pattern is consistent with CdSe hexagonal crystal structure which indicates crystal growth mode along c axis. XRD peaks broaden and shift depending on film thicknesses which are presumably due to strain and size effect. We observe both blue and red shift depending on thickness in Longitudinal Optical phonon frequency in Raman spectra with respect to that of the source CdSe powder which could also be due to strain on thin films and/or finite crystallite size. In this work we combine the results of optical absorption, Raman and XRD spectroscopies to study the evolution of grain size, strain and structural disorder depending on film thickness.

  12. Structure and optical properties of CdSe chalcogenide semiconductors

    NASA Astrophysics Data System (ADS)

    Ganaie, Mohsin; Prince, Zulfequar, M.

    2015-08-01

    CdSe bulk sample has been prepared by melt-quenching technique and were characterized with XRD, SEM, FTIR, and electrical measurements. Thin films were deposited by thermal evaporation technique on ultra clean glass substrates under a high vacuum of 10-6 Torr. An XRD measurement reveals the coexistence of glassy and crystalline phase in bulk sample. SEM studies shows single phase, porous, and granular surface morphology of powder CdSe alloy. Optical properties (optical gap, absorption coefficient, extinction coefficient, refractive index) are calculated in the range of 190-1100nm. Analysis of the optical measurement shows that the non-direct transition is predominant and the band gap come outs to be 1.751eV. Dc conductivity measurement is thermally activated process which shows the semiconducting nature of the sample having activation energy 0.31eV.

  13. A Resonance-Shifting Hybrid n-Type Layer for Boosting Near-Infrared Response in Highly Efficient Colloidal Quantum Dots Solar Cells.

    PubMed

    Baek, Se-Woong; Song, Jung Hoon; Choi, Woong; Song, Hyunjoon; Jeong, Sohee; Lee, Jung-Yong

    2015-12-22

    A new configuration of a plasmonic quantum dots solar structure is proposed. Gold-silver core-shell metal nanoparticles (Au@Ag NCs) are incorporated into the TiO2 layer (Au@Ag NCs-HL) of PbS-based solar cells. The TiO2 layer enables the Au@Ag NCs to have broad plasmonic responses and the external quantum efficiency and absorption of the plasmonic devices are significantly enhanced. The electrical performance of the solar cells is also improved. PMID:26523933

  14. Deposition of CdSe by EC-ALE

    NASA Astrophysics Data System (ADS)

    Mathe, Mkhulu K.; Cox, Stephen M.; Flowers, Billy H.; Vaidyanathan, R.; Pham, Long; Srisook, Nattapong; Happek, Uwe; Stickney, John L.

    2004-10-01

    The optimization of a program for CdSe thin film deposition using electrochemical atomic layer epitaxy (EC-ALE) is reported. EC-ALE uses surface limited reactions, underpotential deposition, to form compound thin film deposits one atomic layer at a time on Au substrates. Cyclic voltammograms showing deposition of Cd and Se on the Au substrate were first performed to identify cycle potentials. CdSe thin films were formed using an automated flow deposition system, by alternately depositing Se and Cd atomic layers, forming a compound monolayer each cycle. In total, 200 cycle deposits were formed using a series of different potentials, to better optimize the deposition conditions. Electron probe microanalysis of the deposits showed Cd/Se ratio between 1.01 and 1.13. X-ray diffraction indicated the deposits were zinc blende, with a (1 1 1) preferred orientation. The thickness of the deposits were determined using ellipsometry, and found to be around 70 nm. AFM studies of the morphology of substrates and deposits indicated that conformal films were formed. The band gaps of the deposits was determined using UV-VIS absorption measurements, photoconductivity and reflection adsorption FTIR, and all suggested a value of 1.74 eV, consistent with literature values.

  15. Photoluminescence spectral study of single cadmium selenide/zinc sulfide colloidal nanocrystals in poly(methyl methacrylate) and quantum dots molecules

    NASA Astrophysics Data System (ADS)

    Shen, Yaoming

    Quantum dots (QDs)and Nano-crystals (NCs) have been studies for decades. Because of the nanoscale quantum confinement, delta shape like energy density states and narrowband emitters properties, they hold great promise for numerous optoelectronics and photonics applications. They could be used for tunable lasers, white LED, Nano-OLED, non-volatile memory and solar cells. They are also the most promising candidates for the quantum computing. The benefits for NCs over QDs is that NCs can be incorporated into a variety of polymers as well as thin films of bulk semiconductors. These exceptional flexibility and structural control distinguish NCs from the more traditional QD structures fabricated using epitaxial growth techniques. In my research of work, I studied the photoluminescence (PL) and absorption character of ensemble NCs incorporated in Polymethyl methacrylate (PMMA). To understand the behavior of the NCs in PMMA, it is important to measure a singe NC to avoid the inhomogenous broading of many NCs. So I particularly studied the behavior of a single NC in PMMA matrix. A microphotoluminescence setup to optically isolate a single nanocrystal is used. Random spectral shift and blinking behavior (on and off) are found. Addition to that, two color spectral shifting, is a major phenomena found in the system. Other interesting results such as PL intensity changes (decreasing or increasing with time) and quenching effect are observed and explained too. From the correlation function, we can distinguish the phonon replicas. The energy of these phonons can be calculated very accurately from the experiment result. The Huang-Rhys factors can be estimated too. Self-assembled semiconductor quantum dots (QDs), from highly strained-layer heteroepitaxy in the Stranski-Krastanow (S-K) growth mode, have been intensively studied because of the delta-function-like density of states, which is significant for optoelectronic applications. Spontaneous formation of semiconductor quantum

  16. Analysis of colloid transport

    SciTech Connect

    Travis, B.J.; Nuttall, H.E.

    1985-12-31

    The population balance methodology is described and applied to the transport and capture of polydispersed colloids in packed columns. The transient model includes particle growth, capture, convective transport, and dispersion. We also follow the dynamic accumulation of captured colloids on the solids. The multidimensional parabolic partial differential equation was solved by a recently enhanced method of characteristics technique. This computational technique minimized numerical dispersion and is computationally very fast. The FORTRAN 77 code ran on a VAX-780 in less than a minute and also runs on an IBM-AT using the Professional FORTRAN compiler. The code was extensively tested against various simplified cases and against analytical models. The packed column experiments by Saltelli et al. were re-analyzed incorporating the experimentally reported size distribution of the colloid feed material. Colloid capture was modeled using a linear size dependent filtration function. The effects of a colloid size dependent filtration factor and various initial colloid size distributions on colloid migration and capture were investigated. Also, we followed the changing colloid size distribution as a function of position in the column. Some simple arguments are made to assess the likelihood of colloid migration at a potential NTS Yucca Mountain waste disposal site. 10 refs., 3 figs., 1 tab.

  17. UZ Colloid Transport Model

    SciTech Connect

    M. McGraw

    2000-04-13

    The UZ Colloid Transport model development plan states that the objective of this Analysis/Model Report (AMR) is to document the development of a model for simulating unsaturated colloid transport. This objective includes the following: (1) use of a process level model to evaluate the potential mechanisms for colloid transport at Yucca Mountain; (2) Provide ranges of parameters for significant colloid transport processes to Performance Assessment (PA) for the unsaturated zone (UZ); (3) Provide a basis for development of an abstracted model for use in PA calculations.

  18. Probing structure-induced optical behavior in a new class of self-activated luminescent 0D/1D CaWO₄ metal oxide – CdSe nanocrystal composite heterostructures

    DOE PAGES

    Han, Jinkyu; McBean, Coray; Wang, Lei; Hoy, Jessica; Jaye, Cherno; Liu, Haiqing; Li, Zhuo-Qun; Sfeir, Matthew Y.; Fischer, Daniel A.; Taylor, Gordon T.; et al

    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

  19. The role of ligands in the optical and electronic spectra of CdSe nanoclusters

    SciTech Connect

    Kilina, Svletana; Sergei, Ivanov A; Victor, Klimov I; Sergei, Tretiak

    2008-01-01

    We investigate the impact of ligands on morphology, electronic structure, and optical response of the Cd33Se33 cluster, which already overlapps in size with the smallest synthesized CdSe quantum dots (QDs). Our Density Functional Theory (DFT) calculations demonstrate significant surface reorganization both for the bare cluster and for the cluster capped by amine and phosphine oxide ligand models. We observe strong surface-ligand interactions leading to substantial charge redistribution and polarization effects on the surface. This effect results in the appearance of hybridized states, where the electronic density is spread over the cluster and the ligands. Neither the ligand's nor hybridized molecular orbitals appear as trap states inside or near the band gap of the QD. Instead, being optically dark, dense hybridized states from the edges of the valence and the conduction bands could open new relaxation channels for high energy photoexcitations. Comparing quantum dots passivated by different ligands, we found that hybridized states are denser in at the edge of the conduction band of the cluster ligated with phosphine oxide molecules than that with primary amines. Such a different manifestation of ligand binding may potentially lead to the faster electron relaxation in dots passivated by phosphine oxide than by amine ligands, which is in agreement with experimental data.

  20. Photoinduced Electron Transfer to Engineered Surface Traps in CdSe Nanocrystals

    NASA Astrophysics Data System (ADS)

    Califano, Marco; Zhu, Haiming; Yang, Ye; Hyeon-Deuk, Kim; Song, Nianhui; Wang, Youwei; Zhang, Wenqing; Prezhdo, Oleg; Lian, Tianquan

    2014-03-01

    Quantum confined nanomaterials, such as semiconductor nanocrystals (NCs), have emerged in the past decade as a new class of materials for solar energy conversion. An appropriate model for describing photoinduced charge transfer in these systems is, however, still lacking. Recently we observed that the rate of photoinduced electron transfer from CdSe NCs to molecular acceptors increased with decreasing NC size (and increasing driving force) exhibiting a lack of Marcus inverted regime behaviour over an apparent driving force range of 0-1.3 V. Our atomistic semiempirical pseudopotential calculations show that an Auger assisted ET mechanism, in which the transfer of the electron is coupled to the excitation of the hole, can circumvent the unfavourable Frank-Condon overlap (that is a signature of inter- or intra- molecular electron transfer) in the Marcus inverted regime, reproducing our observed ET rates with remarkable accuracy. We conclude that electron transfer from quantum dots differs from electron transfer originating from both molecules and bulk semiconductors. It proceeds via a novel Auger-assisted pathway which we believe is available to most excitonic nanomaterials. This new finding will have a major impact on the design of next generation solar energy harvesting devices.