Nearly Efficiency-Droop-Free AlGaN-Based Ultraviolet Light-Emitting Diodes with a Specifically Designed Superlattice p-Type Electron Blocking Layer for High Mg Doping Efficiency

NASA Astrophysics Data System (ADS)

Zhang, Zi-Hui; Huang Chen, Sung-Wen; Chu, Chunshuang; Tian, Kangkai; Fang, Mengqian; Zhang, Yonghui; Bi, Wengang; Kuo, Hao-Chung

2018-04-01

This work reports a nearly efficiency-droop-free AlGaN-based deep ultraviolet light-emitting diode (DUV LED) emitting in the peak wavelength of 270 nm. The DUV LED utilizes a specifically designed superlattice p-type electron blocking layer (p-EBL). The superlattice p-EBL enables a high hole concentration in the p-EBL which correspondingly increases the hole injection efficiency into the multiple quantum wells (MQWs). The enhanced hole concentration within the MQW region can more efficiently recombine with electrons in the way of favoring the radiative recombination, leading to a reduced electron leakage current level. As a result, the external quantum efficiency for the proposed DUV LED structure is increased by 100% and the nearly efficiency-droop-free DUV LED structure is obtained experimentally.

Multi-Dimensional Quantum Tunneling and Transport Using the Density-Gradient Model

NASA Technical Reports Server (NTRS)

Biegel, Bryan A.; Yu, Zhi-Ping; Ancona, Mario; Rafferty, Conor; Saini, Subhash (Technical Monitor)

1999-01-01

We show that quantum effects are likely to significantly degrade the performance of MOSFETs (metal oxide semiconductor field effect transistor) as these devices are scaled below 100 nm channel length and 2 nm oxide thickness over the next decade. A general and computationally efficient electronic device model including quantum effects would allow us to monitor and mitigate these effects. Full quantum models are too expensive in multi-dimensions. Using a general but efficient PDE solver called PROPHET, we implemented the density-gradient (DG) quantum correction to the industry-dominant classical drift-diffusion (DD) model. The DG model efficiently includes quantum carrier profile smoothing and tunneling in multi-dimensions and for any electronic device structure. We show that the DG model reduces DD model error from as much as 50% down to a few percent in comparison to thin oxide MOS capacitance measurements. We also show the first DG simulations of gate oxide tunneling and transverse current flow in ultra-scaled MOSFETs. The advantages of rapid model implementation using the PDE solver approach will be demonstrated, as well as the applicability of the DG model to any electronic device structure.

Silicon coupled with plasmon nanocavities generates bright visible hot luminescence

NASA Astrophysics Data System (ADS)

Cho, Chang-Hee; Aspetti, Carlos O.; Park, Joohee; Agarwal, Ritesh

2013-04-01

To address the limitations in device speed and performance in silicon-based electronics, there have been extensive studies on silicon optoelectronics with a view to achieving ultrafast optical data processing. The biggest challenge has been to develop an efficient silicon-based light source, because the indirect bandgap of silicon gives rise to extremely low emission efficiencies. Although light emission in quantum-confined silicon at sub-10 nm length scales has been demonstrated, there are difficulties in integrating quantum structures with conventional electronics. It is desirable to develop new concepts to obtain emission from silicon at length scales compatible with current electronic devices (20-100 nm), which therefore do not utilize quantum-confinement effects. Here, we demonstrate an entirely new method to achieve bright visible light emission in `bulk-sized' silicon coupled with plasmon nanocavities at room temperature, from non-thermalized carrier recombination. The highly enhanced emission (internal quantum efficiency of >1%) in plasmonic silicon, together with its size compatibility with current silicon electronics, provides new avenues for developing monolithically integrated light sources on conventional microchips.

Enhancing the photon-extraction efficiency of site-controlled quantum dots by deterministically fabricated microlenses

NASA Astrophysics Data System (ADS)

Kaganskiy, Arsenty; Fischbach, Sarah; Strittmatter, André; Rodt, Sven; Heindel, Tobias; Reitzenstein, Stephan

2018-04-01

We report on the realization of scalable single-photon sources (SPSs) based on single site-controlled quantum dots (SCQDs) and deterministically fabricated microlenses. The fabrication process comprises the buried-stressor growth technique complemented with low-temperature in-situ electron-beam lithography for the integration of SCQDs into microlens structures with high yield and high alignment accuracy. The microlens-approach leads to a broadband enhancement of the photon-extraction efficiency of up to (21 ± 2)% and a high suppression of multi-photon events with g (2)(τ = 0) < 0.06 without background subtraction. The demonstrated combination of site-controlled growth of QDs and in-situ electron-beam lithography is relevant for arrays of efficient SPSs which, can be applied in photonic quantum circuits and advanced quantum computation schemes.

Ultrashort electromagnetic pulse control of intersubband quantum well transitions

PubMed Central

2012-01-01

We study the creation of high-efficiency controlled population transfer in intersubband transitions of semiconductor quantum wells. We give emphasis to the case of interaction of the semiconductor quantum well with electromagnetic pulses with a duration of few cycles and even a single cycle. We numerically solve the effective nonlinear Bloch equations for a specific double GaAs/AlGaAs quantum well structure, taking into account the ultrashort nature of the applied field, and show that high-efficiency population inversion is possible for specific pulse areas. The dependence of the efficiency of population transfer on the electron sheet density and the carrier envelope phase of the pulse is also explored. For electromagnetic pulses with a duration of several cycles, we find that the change in the electron sheet density leads to a very different response of the population in the two subbands to pulse area. However, for pulses with a duration equal to or shorter than 3 cycles, we show that efficient population transfer between the two subbands is possible, independent of the value of electron sheet density, if the pulse area is Π. PMID:22916956

Ultrashort electromagnetic pulse control of intersubband quantum well transitions.

PubMed

Paspalakis, Emmanuel; Boviatsis, John

2012-08-23

: We study the creation of high-efficiency controlled population transfer in intersubband transitions of semiconductor quantum wells. We give emphasis to the case of interaction of the semiconductor quantum well with electromagnetic pulses with a duration of few cycles and even a single cycle. We numerically solve the effective nonlinear Bloch equations for a specific double GaAs/AlGaAs quantum well structure, taking into account the ultrashort nature of the applied field, and show that high-efficiency population inversion is possible for specific pulse areas. The dependence of the efficiency of population transfer on the electron sheet density and the carrier envelope phase of the pulse is also explored. For electromagnetic pulses with a duration of several cycles, we find that the change in the electron sheet density leads to a very different response of the population in the two subbands to pulse area. However, for pulses with a duration equal to or shorter than 3 cycles, we show that efficient population transfer between the two subbands is possible, independent of the value of electron sheet density, if the pulse area is Π.

Semiconducting Nanocrystals in Mesostructured Thin Films for Optical and Opto-Electronic Device Applications

DTIC Science & Technology

2007-03-01

with HF in methanol. For example, for 4.5 nm In0.91Ga0.09P nanoparticles in toluene, there is a dramatic increase in PL quantum efficiency from 8...opto-electronic device applications, for which quantum efficiencies above 50% are typically required for commercial cost-effectiveness. For the...InGaP nanocrystals……… 14 Figure 4: 2D double- quantum 31P NMR spectrum, 4.5 nm InGaP nanocrystals………….…… 15 Figure 5: TEM of of 10 nm, 5 nm

Maximizing the quantum efficiency of microchannel plate detectors - The collection of photoelectrons from the interchannel web using an electric field

NASA Technical Reports Server (NTRS)

Taylor, R. C.; Hettrick, M. C.; Malina, R. F.

1983-01-01

High quantum efficiency and two-dimensional imaging capabilities make the microchannel plate (MCP) a suitable detector for a sky survey instrument. The Extreme Ultraviolet Explorer satellite, to be launched in 1987, will use MCP detectors. A feature which limits MCP efficiency is related to the walls of individual channels. The walls are of finite thickness and thus form an interchannel web. Under normal circumstances, this web does not contribute to the detector's quantum efficiency. Panitz and Foesch (1976) have found that in the case of a bombardment with ions, electrons were ejected from the electrode material coating the web. By applying a small electric field, the electrons were returned to the MCP surface where they were detected. The present investigation is concerned with the enhancement of quantum efficiencies in the case of extreme UV wavelengths. Attention is given to a model and a computer simulation which quantitatively reproduce the experimental results.

Photovoltaic devices based on quantum dot functionalized nanowire arrays embedded in an organic matrix

NASA Astrophysics Data System (ADS)

Kung, Patrick; Harris, Nicholas; Shen, Gang; Wilbert, David S.; Baughman, William; Balci, Soner; Dawahre, Nabil; Butler, Lee; Rivera, Elmer; Nikles, David; Kim, Seongsin M.

2012-01-01

Quantum dot (QD) functionalized nanowire arrays are attractive structures for low cost high efficiency solar cells. QDs have the potential for higher quantum efficiency, increased stability and lifetime compared to traditional dyes, as well as the potential for multiple electron generation per photon. Nanowire array scaffolds constitute efficient, low resistance electron transport pathways which minimize the hopping mechanism in the charge transport process of quantum dot solar cells. However, the use of liquid electrolytes as a hole transport medium within such scaffold device structures have led to significant degradation of the QDs. In this work, we first present the synthesis uniform single crystalline ZnO nanowire arrays and their functionalization with InP/ZnS core-shell quantum dots. The structures are characterized using electron microscopy, optical absorption, photoluminescence and Raman spectroscopy. Complementing photoluminescence, transmission electron microanalysis is used to reveal the successful QD attachment process and the atomistic interface between the ZnO and the QD. Energy dispersive spectroscopy reveals the co-localized presence of indium, phosphorus, and sulphur, suggestive of the core-shell nature of the QDs. The functionalized nanowire arrays are subsequently embedded in a poly-3(hexylthiophene) hole transport matrix with a high degree of polymer infiltration to complete the device structure prior to measurement.

Spin-photon interface and spin-controlled photon switching in a nanobeam waveguide

NASA Astrophysics Data System (ADS)

Javadi, Alisa; Ding, Dapeng; Appel, Martin Hayhurst; Mahmoodian, Sahand; Löbl, Matthias Christian; Söllner, Immo; Schott, Rüdiger; Papon, Camille; Pregnolato, Tommaso; Stobbe, Søren; Midolo, Leonardo; Schröder, Tim; Wieck, Andreas Dirk; Ludwig, Arne; Warburton, Richard John; Lodahl, Peter

2018-05-01

The spin of an electron is a promising memory state and qubit. Connecting spin states that are spatially far apart will enable quantum nodes and quantum networks based on the electron spin. Towards this goal, an integrated spin-photon interface would be a major leap forward as it combines the memory capability of a single spin with the efficient transfer of information by photons. Here, we demonstrate such an efficient and optically programmable interface between the spin of an electron in a quantum dot and photons in a nanophotonic waveguide. The spin can be deterministically prepared in the ground state with a fidelity of up to 96%. Subsequently, the system is used to implement a single-spin photonic switch, in which the spin state of the electron directs the flow of photons through the waveguide. The spin-photon interface may enable on-chip photon-photon gates, single-photon transistors and the efficient generation of a photonic cluster state.

Model of biological quantum logic in DNA.

PubMed

Mihelic, F Matthew

2013-08-02

The DNA molecule has properties that allow it to act as a quantum logic processor. It has been demonstrated that there is coherent conduction of electrons longitudinally along the DNA molecule through pi stacking interactions of the aromatic nucleotide bases, and it has also been demonstrated that electrons moving longitudinally along the DNA molecule are subject to a very efficient electron spin filtering effect as the helicity of the DNA molecule interacts with the spin of the electron. This means that, in DNA, electrons are coherently conducted along a very efficient spin filter. Coherent electron spin is held in a logically and thermodynamically reversible chiral symmetry between the C2-endo and C3-endo enantiomers of the deoxyribose moiety in each nucleotide, which enables each nucleotide to function as a quantum gate. The symmetry break that provides for quantum decision in the system is determined by the spin direction of an electron that has an orbital angular momentum that is sufficient to overcome the energy barrier of the double well potential separating the C2-endo and C3-endo enantiomers, and that enantiomeric energy barrier is appropriate to the Landauer limit of the energy necessary to randomize one bit of information.

Hot electron dynamics at semiconductor surfaces: Implications for quantum dot photovoltaics

NASA Astrophysics Data System (ADS)

Tisdale, William A., III

Finding a viable supply of clean, renewable energy is one of the most daunting challenges facing the world today. Solar cells have had limited impact in meeting this challenge because of their high cost and low power conversion efficiencies. Semiconductor nanocrystals, or quantum dots, are promising materials for use in novel solar cells because they can be processed with potentially inexpensive solution-based techniques and because they are predicted to have novel optoelectronic properties that could enable the realization of ultra-efficient solar power converters. However, there is a lack of fundamental understanding regarding the behavior of highly-excited, or "hot," charge carriers near quantum-dot and semiconductor interfaces, which is of paramount importance to the rational design of high-efficiency devices. The elucidation of these ultrafast hot electron dynamics is the central aim of this Dissertation. I present a theoretical framework for treating the electronic interactions between quantum dots and bulk semiconductor surfaces and propose a novel experimental technique, time-resolved surface second harmonic generation (TR-SHG), for probing these interactions. I then describe a series of experimental investigations into hot electron dynamics in specific quantum-dot/semiconductor systems. A two-photon photoelectron spectroscopy (2PPE) study of the technologically-relevant ZnO(1010) surface reveals ultrafast (sub-30fs) cooling of hot electrons in the bulk conduction band, which is due to strong electron-phonon coupling in this highly polar material. The presence of a continuum of defect states near the conduction band edge results in Fermi-level pinning and upward (n-type) band-bending at the (1010) surface and provides an alternate route for electronic relaxation. In monolayer films of colloidal PbSe quantum dots, chemical treatment with either hydrazine or 1,2-ethanedithiol results in strong and tunable electronic coupling between neighboring quantum dots. A TR-SHG study of these electronically-coupled quantum-dot films reveals temperature-activated cooling of hot charge carriers and coherent excitation of a previously-unidentified surface optical phonon. Finally, I report the first experimental observation of ultrafast electron transfer from the higher excited states of a colloidal quantum dot (PbSe) to delocalized conduction band states of a widely-used electron acceptor (TiO2). The electric field resulting from ultrafast (<50fs) separation of charge carriers across the PbSe/TiO2(110) interface excites coherent vibration of the TiO2 surface atoms, whose collective motions can be followed in real time.

Improving hole injection and carrier distribution in InGaN light-emitting diodes by removing the electron blocking layer and including a unique last quantum barrier

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

Cheng, Liwen, E-mail: lwcheng@yzu.edu.cn; Chen, Haitao; Wu, Shudong

2015-08-28

The effects of removing the AlGaN electron blocking layer (EBL), and using a last quantum barrier (LQB) with a unique design in conventional blue InGaN light-emitting diodes (LEDs), were investigated through simulations. Compared with the conventional LED design that contained a GaN LQB and an AlGaN EBL, the LED that contained an AlGaN LQB with a graded-composition and no EBL exhibited enhanced optical performance and less efficiency droop. This effect was caused by an enhanced electron confinement and hole injection efficiency. Furthermore, when the AlGaN LQB was replaced with a triangular graded-composition, the performance improved further and the efficiency droopmore » was lowered. The simulation results indicated that the enhanced hole injection efficiency and uniform distribution of carriers observed in the quantum wells were caused by the smoothing and thinning of the potential barrier for the holes. This allowed a greater number of holes to tunnel into the quantum wells from the p-type regions in the proposed LED structure.« less

Nano-scale engineering using lead chalcogenide nanocrystals for opto-electronic applications

NASA Astrophysics Data System (ADS)

Xu, Fan

Colloidal quantum dots (QDs) or nanocrystals of inorganic semiconductors exhibit exceptional optoelectronic properties such as tunable band-gap, high absorption cross-section and narrow emission spectra. This thesis discusses the characterizations and physical properties of lead-chalcogenide nanocrystals, their assembly into more complex nanostructures and applications in solar cells and near-infrared light-emitting devices. In the first part of this work, we demonstrate that the band edge emission of PbS quantum dots can be tuned from the visible to the mid-infrared region through size control, while the self-attachment of PbS nanocrystals can lead to the formation of 1-D nanowires, 2-D quantum dot monolayers and 3-D quantum dot solids. In particular, the assembly of closely-packed quantum dot solids has attracted enormous attention. A series of distinctive optoelectronic properties has been observed, such as superb multiple exciton generation efficiencies, efficient hot-electron transfer and cold-exciton recycling. Since the surfactant determines the quantum dot surface passivation and inter dot electronic coupling, we examine the influence of different cross-linking surfactants on the optoelectronic properties of the quantum dot solids. Then, we discuss the ability to tune the quantum dot band-gap combined with the controllable assembly of lead-chalcogenide quantum dots, which opens new possibilities to engineer the properties of quantum dot solids. The PbS and PbSe quantum dot cascade structures and PbS/PbSe quantum dot heterojunctions are assembled using the layer-by-layer deposition method. We show that exciton funnelling and trap state-bound exciton recycling in the quantum dot cascade structure dramatically enhances the quantum dots photoluminescence. Moreover, we show that both type-I and type-II PbS/PbSe quantum dot heterojunctions can be assembled by carefully choosing the quantum dot sizes. In type-I heterojunctions, the excited electron-hole pairs tend to localize in narrower band-gap quantum dots, leading to significant photoluminescence enhancement. In contrast, the staggered energy bands in type-II heterojunctions lead to rapid exciton separation at the junctions that considerably quenches the photoluminescence. As such, this strategy can be fruitfully employed to enhance performances in nanocrystal-based photovoltaic devices. Using this approach, we achieve efficient PbS nanocrystal-based solar cells using an ITO/ TiO2/ PbS QDs/Au architecture, where a porous TiO2 nanowire network is employed as electron transporting layer. Our best heterojunction solar cells exhibit a decent short circuit current of 2.5 mA/cm2, a large open circuit voltage of 0.6 V and a power converting efficiency of 5.4 % under 8.5 mW/cm2 low-light illumination. On the other hand, nanocrystal-based near infrared LED devices are fabricated using a simple ITO-PbS QDs-Al device structure. There, the active quantum dot layer serves as both the electron- and hole-transporting layer. With appropriate surface chemistry treatment on quantum dots, a high-brightness near-infrared LED device is achieved.

Purely organic electroluminescent material realizing 100% conversion from electricity to light

PubMed Central

Kaji, Hironori; Suzuki, Hajime; Fukushima, Tatsuya; Shizu, Katsuyuki; Suzuki, Katsuaki; Kubo, Shosei; Komino, Takeshi; Oiwa, Hajime; Suzuki, Furitsu; Wakamiya, Atsushi; Murata, Yasujiro; Adachi, Chihaya

2015-01-01

Efficient organic light-emitting diodes have been developed using emitters containing rare metals, such as platinum and iridium complexes. However, there is an urgent need to develop emitters composed of more abundant materials. Here we show a thermally activated delayed fluorescence material for organic light-emitting diodes, which realizes both approximately 100% photoluminescence quantum yield and approximately 100% up-conversion of the triplet to singlet excited state. The material contains electron-donating diphenylaminocarbazole and electron-accepting triphenyltriazine moieties. The typical trade-off between effective emission and triplet-to-singlet up-conversion is overcome by fine-tuning the highest occupied molecular orbital and lowest unoccupied molecular orbital distributions. The nearly zero singlet–triplet energy gap, smaller than the thermal energy at room temperature, results in an organic light-emitting diode with external quantum efficiency of 29.6%. An external quantum efficiency of 41.5% is obtained when using an out-coupling sheet. The external quantum efficiency is 30.7% even at a high luminance of 3,000 cd m−2. PMID:26477390

Generation of heralded entanglement between distant quantum dot hole spins

NASA Astrophysics Data System (ADS)

Delteil, Aymeric

Entanglement plays a central role in fundamental tests of quantum mechanics as well as in the burgeoning field of quantum information processing. Particularly in the context of quantum networks and communication, some of the major challenges are the efficient generation of entanglement between stationary (spin) and propagating (photon) qubits, the transfer of information from flying to stationary qubits, and the efficient generation of entanglement between distant stationary (spin) qubits. In this talk, I will present such experimental implementations achieved in our team with semiconductor self-assembled quantum dots.Not only are self-assembled quantum dots good single-photon emitters, but they can host an electron or a hole whose spin serves as a quantum memory, and then present spin-dependent optical selection rules leading to an efficient spin-photon quantum interface. Moreover InGaAs quantum dots grown on GaAs substrate can profit from the maturity of III-V semiconductor technology and can be embedded in semiconductor structures like photonic cavities and Schottky diodes.I will report on the realization of heralded quantum entanglement between two semiconductor quantum dot hole spins separated by more than five meters. The entanglement generation scheme relies on single photon interference of Raman scattered light from both dots. A single photon detection projects the system into a maximally entangled state. We developed a delayed two-photon interference scheme that allows for efficient verification of quantum correlations. Moreover the efficient spin-photon interface provided by self-assembled quantum dots allows us to reach an unprecedented rate of 2300 entangled spin pairs per second, which represents an improvement of four orders of magnitude as compared to prior experiments carried out in other systems.Our results extend previous demonstrations in single trapped ions or neutral atoms, in atom ensembles and nitrogen vacancy centers to the domain of artificial atoms in semiconductor nanostructures that allow for on-chip integration of electronic and photonic elements. This work lays the groundwork for the realization of quantum repeaters and quantum networks on a chip.

Performance improvement of AlGaN-based deep-ultraviolet light-emitting diodes via Al-composition graded quantum wells

NASA Astrophysics Data System (ADS)

Lu, Lin; Zhang, Yu; Xu, Fujun; Ding, Gege; Liu, Yuhang

2018-06-01

Characteristics of AlGaN-based deep-ultraviolet light-emitting diodes (DUV-LEDs) with step-like and Al-composition graded quantum wells have been investigated. The simulation results show that compared to DUV-LEDs with the conventional AlGaN multiple quantum wells (MQWs) structure, the light output power (LOP) and efficiency droop of DUV-LEDs with the Al-composition graded wells were remarkably improved. The key factor accounting for the improved performance is ascribed to the better modulation of carrier distribution in the quantum wells to increase the overlap between electron and hole wavefunctions, which contributes to more efficient recombination of electrons and holes, and thereby a significant enhancement in the LOP.

Cooper pair splitter realized in a two-quantum-dot Y-junction.

PubMed

Hofstetter, L; Csonka, S; Nygård, J; Schönenberger, C

2009-10-15

Non-locality is a fundamental property of quantum mechanics that manifests itself as correlations between spatially separated parts of a quantum system. A fundamental route for the exploration of such phenomena is the generation of Einstein-Podolsky-Rosen (EPR) pairs of quantum-entangled objects for the test of so-called Bell inequalities. Whereas such experimental tests of non-locality have been successfully conducted with pairwise entangled photons, it has not yet been possible to realize an electronic analogue of it in the solid state, where spin-1/2 mobile electrons are the natural quantum objects. The difficulty stems from the fact that electrons are immersed in a macroscopic ground state-the Fermi sea-which prevents the straightforward generation and splitting of entangled pairs of electrons on demand. A superconductor, however, could act as a source of EPR pairs of electrons, because its ground-state is composed of Cooper pairs in a spin-singlet state. These Cooper pairs can be extracted from a superconductor by tunnelling, but, to obtain an efficient EPR source of entangled electrons, the splitting of the Cooper pairs into separate electrons has to be enforced. This can be achieved by having the electrons 'repel' each other by Coulomb interaction. Controlled Cooper pair splitting can thereby be realized by coupling of the superconductor to two normal metal drain contacts by means of individually tunable quantum dots. Here we demonstrate the first experimental realization of such a tunable Cooper pair splitter, which shows a surprisingly high efficiency. Our findings open a route towards a first test of the EPR paradox and Bell inequalities in the solid state.

Highly efficient exciplex organic light-emitting diodes incorporating a heptazine derivative as an electron acceptor.

PubMed

Li, Jie; Nomura, Hiroko; Miyazaki, Hiroshi; Adachi, Chihaya

2014-06-11

Highly efficient exciplex systems incorporating a heptazine derivative () as an electron acceptor and 1,3-di(9H-carbazol-9-yl)benzene () as an electron donor are developed. An organic light-emitting diode containing 8 wt% : as an emitting layer exhibits a maximum external quantum efficiency of 11.3%.

Tuning direct bandgap GeSn/Ge quantum dots' interband and intraband useful emission wavelength: Towards CMOS compatible infrared optical devices

NASA Astrophysics Data System (ADS)

Baira, Mourad; Salem, Bassem; Madhar, Niyaz Ahamad; Ilahi, Bouraoui

2018-05-01

In this work, interband and intraband optical transitions from direct bandgap strained GeSn/Ge quantum dots are numerically tuned by evaluating the confined energies for heavy holes and electrons in D- and L-valley. The practically exploitable emission wavelength ranges for efficient use in light emission and sensing should fulfill specific criteria imposing the electrons confined states in D-valley to be sufficiently below those in L-valley. This study shows that GeSn quantum dots offer promising opportunity towards high efficient group IV based infrared optical devices operating in the mid-IR and far-IR wavelength regions.

Investigating the origin of efficiency droop by profiling the voltage across the multi-quantum well of an operating light-emitting diode

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

Kim, Taewoong; Seong, Tae-Yeon; School of Materials Science and Engineering, Korea University, Seoul 136-713

Efficiency droop is a phenomenon in which the efficiency of a light-emitting diode (LED) decreases with the increase in current density. To analyze efficiency droop, direct experimental observations on the energy conversion occurring inside the LED is required. Here, we present the measured voltage profiles on the cross section of an operating LED and analyze them with the cross-sectional temperature profiles obtained in a previous study under the same operation conditions. The measured voltage profiles suggest that with increases in the injection current density, electron depletion shifts from the multi-quantum well through an electron blocking layer to the p-GaN region.more » This is because electron leakage increases with increases in current density.« less

Optical studies of current-induced magnetization switching and photonic quantum states

NASA Astrophysics Data System (ADS)

Lorenz, Virginia

2017-04-01

The ever-decreasing size of electronic components is leading to a fundamental change in the way computers operate, as at the few-nanometer scale, resistive heating and quantum mechanics prohibit efficient and stable operation. One of the most promising next-generation computing paradigms is Spintronics, which uses the spin of the electron to manipulate and store information in the form of magnetic thin films. I will present our optical studies of the fundamental mechanisms by which we can efficiently manipulate magnetization using electrical current. Although electron spin is a quantum-mechanical property, Spintronics relies on macroscopic magnetization and thus does not take advantage of quantum mechanics in the algorithms used to encode and transmit information. For the second part of my talk, I will present our work under the umbrella of new computing and communication technologies based on the quantum mechanical properties of photons. Quantum technologies often require the carriers of information, or qubits, to have specific properties. Photonic quantum states are good information carriers because they travel fast and are robust to environmental fluctuations, but characterizing and controlling photonic sources so the photons have just the right properties is still a challenge. I will describe our work towards enabling quantum-physics-based secure long-distance communication using photons.

Reversible quantum heat engines for electrons

NASA Astrophysics Data System (ADS)

Linke, Heiner; Humphrey, Tammy E.; Newbury, Richard; Taylor, Richard P.

2002-03-01

Brownian heat engines use local temperature gradients in asymmetric potentials to move particles against an external force. The energy efficiency of such machines is generally limited by irreversible heat flow carried by particles that make contact with different heat baths. Here we show that, by using a suitably chosen energy filter, electrons can be transferred reversibly between reservoirs that have different temperatures and electrochemical potentials. We apply this result to propose heat engines based on quantum ratchets, which can quasistatically operate at Carnot efficiency.

Direct Printing of Organic Electronics at the Nanometer Scale

DTIC Science & Technology

2006-02-01

patterning as seen in Figure 3. Also, a flat film OVJP grown Alq3 NPD OLED was shown to be competitive with VTE with quantum efficiencies of 0.84%. 0 0...a tris(8-hydroxyquinoline)- aluminum ( Alq3 ) electron transport and emitting layer. The OLEDs exhibited an external 8 quantum efficiency of (0.84...parameter analyzer and a Newport Model 2932-C dual-channel power meter. An OLED having the layer structure: ITO/60nm NPD/60nm Alq3 /LiF:Al was deposited

Highly Efficient Flexible Quantum Dot Solar Cells with Improved Electron Extraction Using MgZnO Nanocrystals.

PubMed

Zhang, Xiaoliang; Santra, Pralay Kanti; Tian, Lei; Johansson, Malin B; Rensmo, Håkan; Johansson, Erik M J

2017-08-22

Colloidal quantum dot (CQD) solar cells have high potential for realizing an efficient and lightweight energy supply for flexible or wearable electronic devices. To achieve highly efficient and flexible CQD solar cells, the electron transport layer (ETL), extracting electrons from the CQD solid layer, needs to be processed at a low-temperature and should also suppress interfacial recombination. Herein, a highly stable MgZnO nanocrystal (MZO-NC) layer is reported for efficient flexible PbS CQD solar cells. Solar cells fabricated with MZO-NC ETL give a high power conversion efficiency (PCE) of 10.4% and 9.4%, on glass and flexible plastic substrates, respectively. The reported flexible CQD solar cell has the record efficiency to date of flexible CQD solar cells. Detailed theoretical simulations and extensive characterizations reveal that the MZO-NCs significantly enhance charge extraction from CQD solids and diminish the charge accumulation at the ETL/CQD interface, suppressing charge interfacial recombination. These important results suggest that the low-temperature processed MZO-NCs are very promising for use in efficient flexible solar cells or other flexible optoelectronic devices.

Non-linear effects and thermoelectric efficiency of quantum dot-based single-electron transistors.

PubMed

Talbo, Vincent; Saint-Martin, Jérôme; Retailleau, Sylvie; Dollfus, Philippe

2017-11-01

By means of advanced numerical simulation, the thermoelectric properties of a Si-quantum dot-based single-electron transistor operating in sequential tunneling regime are investigated in terms of figure of merit, efficiency and power. By taking into account the phonon-induced collisional broadening of energy levels in the quantum dot, both heat and electrical currents are computed in a voltage range beyond the linear response. Using our homemade code consisting in a 3D Poisson-Schrödinger solver and the resolution of the Master equation, the Seebeck coefficient at low bias voltage appears to be material independent and nearly independent on the level broadening, which makes this device promising for metrology applications as a nanoscale standard of Seebeck coefficient. Besides, at higher voltage bias, the non-linear characteristics of the heat current are shown to be related to the multi-level effects. Finally, when considering only the electronic contribution to the thermal conductance, the single-electron transistor operating in generator regime is shown to exhibit very good efficiency at maximum power.

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

PubMed

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

2013-04-10

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

Towards efficient solar hydrogen production by intercalated carbon nitride photocatalyst.

PubMed

Gao, Honglin; Yan, Shicheng; Wang, Jiajia; Huang, Yu An; Wang, Peng; Li, Zhaosheng; Zou, Zhigang

2013-11-07

The development of efficient photocatalytic material for converting solar energy to hydrogen energy as viable alternatives to fossil-fuel technologies is expected to revolutionize energy shortage and environment issues. However, to date, the low quantum yield for solar hydrogen production over photocatalysts has hindered advances in the practical applications of photocatalysis. Here, we show that a carbon nitride intercalation compound (CNIC) synthesized by a simple molten salt route is an efficient polymer photocatalyst with a high quantum yield. We found that coordinating the alkali metals into the C-N plane of carbon nitride will induce the un-uniform spatial charge distribution. The electrons are confined in the intercalated region while the holes are in the far intercalated region, which promoted efficient separation of photogenerated carriers. The donor-type alkali metal ions coordinating into the nitrogen pots of carbon nitrides increase the free carrier concentration and lead to the formation of novel nonradiative paths. This should favor improved transport of the photogenerated electron and hole and decrease the electron-hole recombination rate. As a result, the CNIC exhibits a quantum yield as high as 21.2% under 420 nm light irradiation for solar hydrogen production. Such high quantum yield opens up new opportunities for using cheap semiconducting polymers as energy transducers.

Resonantly driven CNOT gate for electron spins

NASA Astrophysics Data System (ADS)

Zajac, D. M.; Sigillito, A. J.; Russ, M.; Borjans, F.; Taylor, J. M.; Burkard, G.; Petta, J. R.

2018-01-01

To build a universal quantum computer—the kind that can handle any computational task you throw at it—an essential early step is to demonstrate the so-called CNOT gate, which acts on two qubits. Zajac et al. built an efficient CNOT gate by using electron spin qubits in silicon quantum dots, an implementation that is especially appealing because of its compatibility with existing semiconductor-based electronics (see the Perspective by Schreiber and Bluhm). To showcase the potential, the authors used the gate to create an entangled quantum state called the Bell state.

A simple quantum mechanical treatment of scattering in nanoscale transistors

NASA Astrophysics Data System (ADS)

Venugopal, R.; Paulsson, M.; Goasguen, S.; Datta, S.; Lundstrom, M. S.

2003-05-01

We present a computationally efficient, two-dimensional quantum mechanical simulation scheme for modeling dissipative electron transport in thin body, fully depleted, n-channel, silicon-on-insulator transistors. The simulation scheme, which solves the nonequilibrium Green's function equations self consistently with Poisson's equation, treats the effect of scattering using a simple approximation inspired by the "Büttiker probes," often used in mesoscopic physics. It is based on an expansion of the active device Hamiltonian in decoupled mode space. Simulation results are used to highlight quantum effects, discuss the physics of scattering and to relate the quantum mechanical quantities used in our model to experimentally measured low field mobilities. Additionally, quantum boundary conditions are rigorously derived and the effects of strong off-equilibrium transport are examined. This paper shows that our approximate treatment of scattering, is an efficient and useful simulation method for modeling electron transport in nanoscale, silicon-on-insulator transistors.

A Biomimetic-Computational Approach to Optimizing the Quantum Efficiency of Photovoltaics

NASA Astrophysics Data System (ADS)

Perez, Lisa M.; Holzenburg, Andreas

The most advanced low-cost organic photovoltaic cells have a quantum efficiency of 10%. This is in stark contrast to plant/bacterial light-harvesting systems which offer quantum efficiencies close to unity. Of particular interest is the highly effective quantum coherence-enabled energy transfer (Fig. 1). Noting that quantum coherence is promoted by charged residues and local dielectrics, classical atomistic simulations and time-dependent density functional theory (DFT) are used to identify charge/dielectric patterns and electronic coupling at exactly defined energy transfer interfaces. The calculations make use of structural information obtained on photosynthetic protein-pigment complexes while still in the native membrane making it possible to establish a link between supramolecular organization and quantum coherence in terms of what length scales enable fast energy transport and prevent quenching. Calculating energy transfer efficiencies between components based on different proximities will permit the search for patterns that enable defining material properties suitable for advanced photovoltaics.

On the effect of ballistic overflow on the temperature dependence of the quantum efficiency of InGaN/GaN multiple quantum well light-emitting diodes

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

Prudaev, I. A., E-mail: funcelab@gmail.com; Kopyev, V. V.; Romanov, I. S.

The dependences of the quantum efficiency of InGaN/GaN multiple quantum well light-emitting diodes on the temperature and excitation level are studied. The experiment is performed for two luminescence excitation modes. A comparison of the results obtained during photo- and electroluminescence shows an additional (to the loss associated with Auger recombination) low-temperature loss in the high-density current region. This causes inversion of the temperature dependence of the quantum efficiency at temperatures lower than 220–300 K. Analysis shows that the loss is associated with electron leakage from the light-emitting-diode active region. The experimental data are explained using the ballistic-overflow model. The simulationmore » results are in qualitative agreement with the experimental dependences of the quantum efficiency on temperature and current density.« less

Scalable quantum computing based on stationary spin qubits in coupled quantum dots inside double-sided optical microcavities

NASA Astrophysics Data System (ADS)

Wei, Hai-Rui; Deng, Fu-Guo

2014-12-01

Quantum logic gates are the key elements in quantum computing. Here we investigate the possibility of achieving a scalable and compact quantum computing based on stationary electron-spin qubits, by using the giant optical circular birefringence induced by quantum-dot spins in double-sided optical microcavities as a result of cavity quantum electrodynamics. We design the compact quantum circuits for implementing universal and deterministic quantum gates for electron-spin systems, including the two-qubit CNOT gate and the three-qubit Toffoli gate. They are compact and economic, and they do not require additional electron-spin qubits. Moreover, our devices have good scalability and are attractive as they both are based on solid-state quantum systems and the qubits are stationary. They are feasible with the current experimental technology, and both high fidelity and high efficiency can be achieved when the ratio of the side leakage to the cavity decay is low.

Scalable quantum computing based on stationary spin qubits in coupled quantum dots inside double-sided optical microcavities.

PubMed

Wei, Hai-Rui; Deng, Fu-Guo

2014-12-18

Quantum logic gates are the key elements in quantum computing. Here we investigate the possibility of achieving a scalable and compact quantum computing based on stationary electron-spin qubits, by using the giant optical circular birefringence induced by quantum-dot spins in double-sided optical microcavities as a result of cavity quantum electrodynamics. We design the compact quantum circuits for implementing universal and deterministic quantum gates for electron-spin systems, including the two-qubit CNOT gate and the three-qubit Toffoli gate. They are compact and economic, and they do not require additional electron-spin qubits. Moreover, our devices have good scalability and are attractive as they both are based on solid-state quantum systems and the qubits are stationary. They are feasible with the current experimental technology, and both high fidelity and high efficiency can be achieved when the ratio of the side leakage to the cavity decay is low.

Polynomial-time quantum algorithm for the simulation of chemical dynamics

PubMed Central

Kassal, Ivan; Jordan, Stephen P.; Love, Peter J.; Mohseni, Masoud; Aspuru-Guzik, Alán

2008-01-01

The computational cost of exact methods for quantum simulation using classical computers grows exponentially with system size. As a consequence, these techniques can be applied only to small systems. By contrast, we demonstrate that quantum computers could exactly simulate chemical reactions in polynomial time. Our algorithm uses the split-operator approach and explicitly simulates all electron-nuclear and interelectronic interactions in quadratic time. Surprisingly, this treatment is not only more accurate than the Born–Oppenheimer approximation but faster and more efficient as well, for all reactions with more than about four atoms. This is the case even though the entire electronic wave function is propagated on a grid with appropriately short time steps. Although the preparation and measurement of arbitrary states on a quantum computer is inefficient, here we demonstrate how to prepare states of chemical interest efficiently. We also show how to efficiently obtain chemically relevant observables, such as state-to-state transition probabilities and thermal reaction rates. Quantum computers using these techniques could outperform current classical computers with 100 qubits. PMID:19033207

Full Quantum Dynamics Simulation of a Realistic Molecular System Using the Adaptive Time-Dependent Density Matrix Renormalization Group Method.

PubMed

Yao, Yao; Sun, Ke-Wei; Luo, Zhen; Ma, Haibo

2018-01-18

The accurate theoretical interpretation of ultrafast time-resolved spectroscopy experiments relies on full quantum dynamics simulations for the investigated system, which is nevertheless computationally prohibitive for realistic molecular systems with a large number of electronic and/or vibrational degrees of freedom. In this work, we propose a unitary transformation approach for realistic vibronic Hamiltonians, which can be coped with using the adaptive time-dependent density matrix renormalization group (t-DMRG) method to efficiently evolve the nonadiabatic dynamics of a large molecular system. We demonstrate the accuracy and efficiency of this approach with an example of simulating the exciton dissociation process within an oligothiophene/fullerene heterojunction, indicating that t-DMRG can be a promising method for full quantum dynamics simulation in large chemical systems. Moreover, it is also shown that the proper vibronic features in the ultrafast electronic process can be obtained by simulating the two-dimensional (2D) electronic spectrum by virtue of the high computational efficiency of the t-DMRG method.

Study on Locally Confined Deposition of Si Nanocrystals in High-Aspect-Ratio Si Nano-Pillar Array for Nano-Electronic and Nano-Photonic Applications

DTIC Science & Technology

2010-02-23

reflection, thus increasing the quantum efficiency by one order of magnitude and improving the light extraction from the nano-roughened device surface by...respectively. At a biased current of 400 A, the highest external quantum efficiency is over 0.2% to obtain the maximum EL power of >1 W. In...processing techniques for improving the internal and external quantum efficiencies of Si MOSLEDs via detuning the size and density of high-aspect-ratio Si

CdS/CdSe co-sensitized SnO2 photoelectrodes for quantum dots sensitized solar cells

NASA Astrophysics Data System (ADS)

Lin, Yibing; Lin, Yu; Meng, Yongming; Tu, Yongguang; Zhang, Xiaolong

2015-07-01

SnO2 nanoparticles were synthesized by hydrothermal method and applied to photo-electrodes of quantum dots-sensitized solar cells (QDSSCs). After sensitizing SnO2 films via CdS quantum dots, CdSe quantum dots was decorated on the surface of CdS/SnO2 photo-electrodes to further improve the power conversion efficiency. CdS and CdSe quantum dots were deposited by successive ionic layer absorption and reaction method (SILAR) and chemical bath deposition method (CBD) respectively. Scanning electron microscopy (SEM), transmission electron microscopy (TEM) and X-ray diffraction (XRD) were used to identify the surface profile and crystal structure of SnO2 photo-electrodes before and after deposited quantum dots. After CdSe co-sensitized process, an overall power conversion efficiency of 1.78% was obtained in CdSe/CdS/SnO2 QDSSC, which showed 66.4% improvement than that of CdS/SnO2 QDSSC.

Electrical control of optical orientation of neutral and negatively charged excitons in an n -type semiconductor quantum well

NASA Astrophysics Data System (ADS)

Dzhioev, R. I.; Korenev, V. L.; Lazarev, M. V.; Sapega, V. F.; Gammon, D.; Bracker, A. S.

2007-01-01

We report electric field induced increase of spin orientation of negatively charged excitons (trions) localized in n -type GaAs/AlGaAs quantum well. Under resonant excitation of free neutral heavy-hole excitons, the polarization of trions increases dramatically with electrical injection of electrons. The polarization enhancement correlates strongly with trion/exciton luminescence intensity ratio. This effect results from a very efficient trapping of free neutral excitons by the quantum well interfacial fluctuations (“natural” quantum dots) containing resident electrons.

Quantum-circuit refrigerator

NASA Astrophysics Data System (ADS)

Tan, Kuan Yen; Partanen, Matti; Lake, Russell E.; Govenius, Joonas; Masuda, Shumpei; Möttönen, Mikko

2017-05-01

Quantum technology promises revolutionizing applications in information processing, communications, sensing and modelling. However, efficient on-demand cooling of the functional quantum degrees of freedom remains challenging in many solid-state implementations, such as superconducting circuits. Here we demonstrate direct cooling of a superconducting resonator mode using voltage-controllable electron tunnelling in a nanoscale refrigerator. This result is revealed by a decreased electron temperature at a resonator-coupled probe resistor, even for an elevated electron temperature at the refrigerator. Our conclusions are verified by control experiments and by a good quantitative agreement between theory and experimental observations at various operation voltages and bath temperatures. In the future, we aim to remove spurious dissipation introduced by our refrigerator and to decrease the operational temperature. Such an ideal quantum-circuit refrigerator has potential applications in the initialization of quantum electric devices. In the superconducting quantum computer, for example, fast and accurate reset of the quantum memory is needed.

Extremely efficient internal exciton dissociation through edge states in layered 2D perovskites

NASA Astrophysics Data System (ADS)

Blancon, J.-C.; Tsai, H.; Nie, W.; Stoumpos, C. C.; Pedesseau, L.; Katan, C.; Kepenekian, M.; Soe, C. M. M.; Appavoo, K.; Sfeir, M. Y.; Tretiak, S.; Ajayan, P. M.; Kanatzidis, M. G.; Even, J.; Crochet, J. J.; Mohite, A. D.

2017-03-01

Understanding and controlling charge and energy flow in state-of-the-art semiconductor quantum wells has enabled high-efficiency optoelectronic devices. Two-dimensional (2D) Ruddlesden-Popper perovskites are solution-processed quantum wells wherein the band gap can be tuned by varying the perovskite-layer thickness, which modulates the effective electron-hole confinement. We report that, counterintuitive to classical quantum-confined systems where photogenerated electrons and holes are strongly bound by Coulomb interactions or excitons, the photophysics of thin films made of Ruddlesden-Popper perovskites with a thickness exceeding two perovskite-crystal units (>1.3 nanometers) is dominated by lower-energy states associated with the local intrinsic electronic structure of the edges of the perovskite layers. These states provide a direct pathway for dissociating excitons into longer-lived free carriers that substantially improve the performance of optoelectronic devices.

Exciton multiplication from first principles.

PubMed

Jaeger, Heather M; Hyeon-Deuk, Kim; Prezhdo, Oleg V

2013-06-18

Third-generation photovolatics require demanding cost and power conversion efficiency standards, which may be achieved through efficient exciton multiplication. Therefore, generating more than one electron-hole pair from the absorption of a single photon has vast ramifications on solar power conversion technology. Unlike their bulk counterparts, irradiated semiconductor quantum dots exhibit efficient exciton multiplication, due to confinement-enhanced Coulomb interactions and slower nonradiative losses. The exact characterization of the complicated photoexcited processes within quantum-dot photovoltaics is a work in progress. In this Account, we focus on the photophysics of nanocrystals and investigate three constituent processes of exciton multiplication, including photoexcitation, phonon-induced dephasing, and impact ionization. We quantify the role of each process in exciton multiplication through ab initio computation and analysis of many-electron wave functions. The probability of observing a multiple exciton in a photoexcited state is proportional to the magnitude of electron correlation, where correlated electrons can be simultaneously promoted across the band gap. Energies of multiple excitons are determined directly from the excited state wave functions, defining the threshold for multiple exciton generation. This threshold is strongly perturbed in the presence of surface defects, dopants, and ionization. Within a few femtoseconds following photoexcitation, the quantum state loses coherence through interactions with the vibrating atomic lattice. The phase relationship between single excitons and multiple excitons dissipates first, followed by multiple exciton fission. Single excitons are coupled to multiple excitons through Coulomb and electron-phonon interactions, and as a consequence, single excitons convert to multiple excitons and vice versa. Here, exciton multiplication depends on the initial energy and coupling magnitude and competes with electron-phonon energy relaxation. Multiple excitons are generated through impact ionization within picoseconds. The basis of exciton multiplication in quantum dots is the collective result of photoexcitation, dephasing, and nonadiabatic evolution. Each process is characterized by a distinct time-scale, and the overall multiple exciton generation dynamics is complete by about 10 ps. Without relying on semiempirical parameters, we computed quantum mechanical probabilities of multiple excitons for small model systems. Because exciton correlations and coherences are microscopic, quantum properties, results for small model systems can be extrapolated to larger, realistic quantum dots.

Balancing the Electron and Hole Transfer for Efficient Quantum Dot Light-Emitting Diodes by Employing a Versatile Organic Electron-Blocking Layer.

PubMed

Jin, Xiao; Chang, Chun; Zhao, Weifeng; Huang, Shujuan; Gu, Xiaobing; Zhang, Qin; Li, Feng; Zhang, Yubao; Li, Qinghua

2018-05-09

The electron-blocking layer (EBL) is important to balance the charge carrier transfer and achieve highly efficient quantum dot light-emitting diodes (QLEDs). Here, we report the utilization of a soluble tert-butyldimethylsilyl chloride-modified poly( p-phenylene benzobisoxazole) (TBS-PBO) as an EBL for simultaneous good charge carrier transfer balance while maintaining a high current density. We show that the versatile TBS-PBO blocks excess electron injection into the quantum dots (QDs), thus leading to better charge carrier transfer balance. It also restricts the undesired QD-to-EBL electron-transfer process, which preserves the superior emission capabilities of the emitter. As a consequence, the TBS-PBO device delivers an external quantum efficiency (EQE) maximum of 16.7% along with a remarkable current density as high as 139 mA/cm 2 with a brightness of 5484 cd/m 2 . The current density of our device is higher than those of insulator EBL-based devices because of the higher conductivity of the TBS-PBO versus insulator EBL, thus helping achieve high luminance values ranging from 1414 to 20 000 cd/cm 2 with current densities ranging from 44 to 648 mA/cm 2 and EQE > 14%. We believe that these unconventional features of the present TBS-PBO-based QLEDs will expand the wide use of TBS-PBO as buffer layers in other advanced QLED applications.

A New Proxy Electronic Voting Scheme Achieved by Six-Particle Entangled States

NASA Astrophysics Data System (ADS)

Cao, Hai-Jing; Ding, Li-Yuan; Jiang, Xiu-Li; Li, Peng-Fei

2018-03-01

In this paper, we use quantum proxy signature to construct a new secret electronic voting scheme. In our scheme, six particles entangled states function as quantum channels. The voter Alice, the Vote Management Center Bob, the scrutineer Charlie only perform two particles measurements on the Bell bases to realize the electronic voting process. So the scheme reduces the technical difficulty and increases operation efficiency. We use quantum key distribution and one-time pad to guarantee its unconditional security. The significant advantage of our scheme is that transmitted information capacity is twice as much as the capacity of other schemes.

Natural occupation numbers in two-electron quantum rings.

PubMed

Tognetti, Vincent; Loos, Pierre-François

2016-02-07

Natural orbitals (NOs) are central constituents for evaluating correlation energies through efficient approximations. Here, we report the closed-form expression of the NOs of two-electron quantum rings, which are prototypical finite-extension systems and new starting points for the development of exchange-correlation functionals in density functional theory. We also show that the natural occupation numbers for these two-electron paradigms are in general non-vanishing and follow the same power law decay as atomic and molecular two-electron systems.

Natural occupation numbers in two-electron quantum rings

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

Tognetti, Vincent, E-mail: vincent.tognetti@univ-rouen.fr; Loos, Pierre-François

2016-02-07

Natural orbitals (NOs) are central constituents for evaluating correlation energies through efficient approximations. Here, we report the closed-form expression of the NOs of two-electron quantum rings, which are prototypical finite-extension systems and new starting points for the development of exchange-correlation functionals in density functional theory. We also show that the natural occupation numbers for these two-electron paradigms are in general non-vanishing and follow the same power law decay as atomic and molecular two-electron systems.

The ABC model of recombination reinterpreted: Impact on understanding carrier transport and efficiency droop in InGaN/GaN light emitting diodes

NASA Astrophysics Data System (ADS)

Hopkins, M. A.; Allsopp, D. W. E.; Kappers, M. J.; Oliver, R. A.; Humphreys, C. J.

2017-12-01

The efficiency of light emitting diodes (LEDs) remains a topic of great contemporary interest due to their potential to reduce the amount of energy consumed in lighting. The current consensus is that electrons and holes distribute themselves through the emissive region by a drift-diffusion process which results in a highly non-uniform distribution of the light emission and can reduce efficiency. In this paper, the measured variations in the external quantum efficiency of a range of InGaN/GaN LEDs with different numbers of quantum wells (QWs) are shown to compare closely with the predictions of a revised ABC model, in which it is assumed that the electrically injected electrons and holes are uniformly distributed through the multi-quantum well (MQW) region, or nearly so, and hence carrier recombination occurs equally in all the quantum wells. The implications of the reported results are that drift-diffusion plays a far lesser role in cross-well carrier transport than previously thought; that the dominant cause of efficiency droop is intrinsic to the quantum wells and that reductions in the density of non-radiative recombination centers in the MQW would enable the use of more QWs and thereby reduce Auger losses by spreading carriers more evenly across a wider emissive region.

"Double-Cable" Conjugated Polymers with Linear Backbone toward High Quantum Efficiencies in Single-Component Polymer Solar Cells.

PubMed

Feng, Guitao; Li, Junyu; Colberts, Fallon J M; Li, Mengmeng; Zhang, Jianqi; Yang, Fan; Jin, Yingzhi; Zhang, Fengling; Janssen, René A J; Li, Cheng; Li, Weiwei

2017-12-27

A series of "double-cable" conjugated polymers were developed for application in efficient single-component polymer solar cells, in which high quantum efficiencies could be achieved due to the optimized nanophase separation between donor and acceptor parts. The new double-cable polymers contain electron-donating poly(benzodithiophene) (BDT) as linear conjugated backbone for hole transport and pendant electron-deficient perylene bisimide (PBI) units for electron transport, connected via a dodecyl linker. Sulfur and fluorine substituents were introduced to tune the energy levels and crystallinity of the conjugated polymers. The double-cable polymers adopt a "face-on" orientation in which the conjugated BDT backbone and the pendant PBI units have a preferential π-π stacking direction perpendicular to the substrate, favorable for interchain charge transport normal to the plane. The linear conjugated backbone acts as a scaffold for the crystallization of the PBI groups, to provide a double-cable nanophase separation of donor and acceptor phases. The optimized nanophase separation enables efficient exciton dissociation as well as charge transport as evidenced from the high-up to 80%-internal quantum efficiency for photon-to-electron conversion. In single-component organic solar cells, the double-cable polymers provide power conversion efficiency up to 4.18%. This is one of the highest performances in single-component organic solar cells. The nanophase-separated design can likely be used to achieve high-performance single-component organic solar cells.

Logical spin-filtering in a triangular network of quantum nanorings with a Rashba spin-orbit interaction

NASA Astrophysics Data System (ADS)

Dehghan, E.; Sanavi Khoshnoud, D.; Naeimi, A. S.

2018-01-01

The spin-resolved electron transport through a triangular network of quantum nanorings is studied in the presence of Rashba spin-orbit interaction (RSOI) and a magnetic flux using quantum waveguide theory. This study illustrates that, by tuning Rashba constant, magnetic flux and incoming electron energy, the triangular network of quantum rings can act as a perfect logical spin-filtering with high efficiency. By changing in the energy of incoming electron, at a proper value of the Rashba constant and magnetic flux, a reverse in the direction of spin can take place in the triangular network of quantum nanorings. Furthermore, the triangular network of quantum nanorings can be designed as a device and shows several simultaneous spintronic properties such as spin-splitter and spin-inverter. This spin-splitting is dependent on the energy of the incoming electron. Additionally, different polarizations can be achieved in the two outgoing leads from an originally incoming spin state that simulates a Stern-Gerlach apparatus.

Highly Efficient Room Temperature Spin Injection Using Spin Filtering in MgO

NASA Astrophysics Data System (ADS)

Jiang, Xin

2007-03-01

Efficient electrical spin injection into GaAs/AlGaAs quantum well structures was demonstrated using CoFe/MgO tunnel spin injectors at room temperature. The spin polarization of the injected electron current was inferred from the circular polarization of electroluminescence from the quantum well. Polarization values as high as 57% at 100 K and 47% at 290 K were obtained in a perpendicular magnetic field of 5 Tesla. The interface between the tunnel spin injector and the GaAs interface remained stable even after thermal annealing at 400 ^oC. The temperature dependence of the electron-hole recombination time and the electron spin relaxation time in the quantum well was measured using time-resolved optical techniques. By taking into account of these properties of the quantum well, the intrinsic spin injection efficiency can be deduced. We conclude that the efficiency of spin injection from a CoFe/MgO spin injector is nearly independent of temperature and, moreover, is highly efficient with an efficiency of ˜ 70% for the temperature range studied (10 K to room temperature). Tunnel spin injectors are thus highly promising components of future semiconductor spintronic devices. Collaborators: Roger Wang^1, 3, Gian Salis^2, Robert Shelby^1, Roger Macfarlane^1, Seth Bank^3, Glenn Solomon^3, James Harris^3, Stuart S. P. Parkin^1 ^1 IBM Almaden Research Center, San Jose, CA 95120 ^2 IBM Zurich Research Laboratory, S"aumerstrasse 4, 8803 R"uschlikon, Switzerland ^3 Solid States and Photonics Laboratory, Stanford University, Stanford, CA 94305

Nano-patterned superconducting surface for high quantum efficiency cathode

DOEpatents

Hannon, Fay; Musumeci, Pietro

2017-03-07

A method for providing a superconducting surface on a laser-driven niobium cathode in order to increase the effective quantum efficiency. The enhanced surface increases the effective quantum efficiency by improving the laser absorption of the surface and enhancing the local electric field. The surface preparation method makes feasible the construction of superconducting radio frequency injectors with niobium as the photocathode. An array of nano-structures are provided on a flat surface of niobium. The nano-structures are dimensionally tailored to interact with a laser of specific wavelength to thereby increase the electron yield of the surface.

Extremely efficient internal exciton dissociation through edge states in layered 2D perovskites

DOE PAGES

Blancon, Jean -Christophe Robert; Tsai, Hsinhan; Nie, Wanyi; ...

2017-03-09

Understanding and controlling charge and energy flow in state-of-the-art semiconductor quantum wells has enabled high-efficiency optoelectronic devices. Two-dimensional (2D) Ruddlesden-Popper perovskites are solution-processed quantum wells wherein the band gap can be tuned by varying the perovskite-layer thickness, which modulates the effective electron-hole confinement. We report that, counterintuitive to classical quantum-confined systems where photogenerated electrons and holes are strongly bound by Coulomb interactions or excitons, the photophysics of thin films made of Ruddlesden-Popper perovskites with a thickness exceeding two perovskite-crystal units (>1.3 nanometers) is dominated by lower-energy states associated with the local intrinsic electronic structure of the edges of the perovskitemore » layers. Furthermore, these states provide a direct pathway for dissociating excitons into longer-lived free carriers that substantially improve the performance of optoelectronic devices.« less

Optical pumping of the electronic and nuclear spin of single charge-tunable quantum dots.

PubMed

Bracker, A S; Stinaff, E A; Gammon, D; Ware, M E; Tischler, J G; Shabaev, A; Efros, Al L; Park, D; Gershoni, D; Korenev, V L; Merkulov, I A

2005-02-04

We present a comprehensive examination of optical pumping of spins in individual GaAs quantum dots as we change the net charge from positive to neutral to negative with a charge-tunable heterostructure. Negative photoluminescence polarization memory is enhanced by optical pumping of ground state electron spins, which we prove with the first measurements of the Hanle effect on an individual quantum dot. We use the Overhauser effect in a high longitudinal magnetic field to demonstrate efficient optical pumping of nuclear spins for all three charge states of the quantum dot.

Optical Pumping of the Electronic and Nuclear Spin of Single Charge-Tunable Quantum Dots

NASA Astrophysics Data System (ADS)

Bracker, A. S.; Stinaff, E. A.; Gammon, D.; Ware, M. E.; Tischler, J. G.; Shabaev, A.; Efros, Al. L.; Park, D.; Gershoni, D.; Korenev, V. L.; Merkulov, I. A.

2005-02-01

We present a comprehensive examination of optical pumping of spins in individual GaAs quantum dots as we change the net charge from positive to neutral to negative with a charge-tunable heterostructure. Negative photoluminescence polarization memory is enhanced by optical pumping of ground state electron spins, which we prove with the first measurements of the Hanle effect on an individual quantum dot. We use the Overhauser effect in a high longitudinal magnetic field to demonstrate efficient optical pumping of nuclear spins for all three charge states of the quantum dot.

Plasmon-resonance-enhanced visible-light photocatalytic activity of Ag quantum dots/TiO2 microspheres for methyl orange degradation

NASA Astrophysics Data System (ADS)

Yu, Xin; Shang, Liwei; Wang, Dongjun; An, Li; Li, Zhonghua; Liu, Jiawen; Shen, Jun

2018-06-01

We successfully prepared Ag quantum dots modified TiO2 microspheres by facile solvothermal and calcination method. The as-prepared Ag quantum dots/TiO2 microspheres were characterized by scanning electron microscope, transmission electron microscope, X-ray diffraction, X-ray photoelectron spectroscopy and UV-vis diffuse reflectance spectroscopy. The Ag quantum dots/TiO2 photocatalyst showed excellent visible light absorption and efficient photocatalytic activity for methyl orange degradation. And the sample with the molar ratio of 0.05 (Ag to Ti) showed the best visible light photocatalytic activity for methyl orange degradation, mainly because of the surface plasmon resonance (SPR) effects of Ag quantum dots to generate electron and hole pairs for enhanced visible light photocatalysis. Finally, possible visible light photocatalytic mechanism of Ag quantum dots/TiO2 microspheres for methyl orange degradation was proposed in detail.

Electron-Phonon Coupling and Resonant Relaxation from 1D and 1P States in PbS Quantum Dots.

PubMed

Kennehan, Eric R; Doucette, Grayson S; Marshall, Ashley R; Grieco, Christopher; Munson, Kyle T; Beard, Matthew C; Asbury, John B

2018-05-31

Observations of the hot-phonon bottleneck, which is predicted to slow the rate of hot carrier cooling in quantum confined nanocrystals, have been limited to date for reasons that are not fully understood. We used time-resolved infrared spectroscopy to directly measure higher energy intraband transitions in PbS colloidal quantum dots. Direct measurements of these intraband transitions permitted detailed analysis of the electronic overlap of the quantum confined states that may influence their relaxation processes. In smaller PbS nanocrystals, where the hot-phonon bottleneck is expected to be most pronounced, we found that relaxation of parity selection rules combined with stronger electron-phonon coupling led to greater spectral overlap of transitions among the quantum confined states. This created pathways for fast energy transfer and relaxation that may bypass the predicted hot-phonon bottleneck. In contrast, larger, but still quantum confined nanocrystals did not exhibit such relaxation of the parity selection rules and possessed narrower intraband states. These observations were consistent with slower relaxation dynamics that have been measured in larger quantum confined systems. These findings indicated that, at small radii, electron-phonon interactions overcome the advantageous increase in energetic separation of the electronic states for PbS quantum dots. Selection of appropriately sized quantum dots, which minimize spectral broadening due to electron-phonon interactions while maximizing electronic state separation, is necessary to observe the hot-phonon bottleneck. Such optimization may provide a framework for achieving efficient hot carrier collection and multiple exciton generation.

Nonplasmonic Hot-Electron Photocurrents from Mn-Doped Quantum Dots in Photoelectrochemical Cells.

PubMed

Dong, Yitong; Rossi, Daniel; Parobek, David; Son, Dong Hee

2016-03-03

We report the measurement of the hot-electron current in a photoelectrochemical cell constructed from a glass/ITO/Al2 O3 (ITO=indium tin oxide) electrode coated with Mn-doped quantum dots, where hot electrons with a large excess kinetic energy were produced through upconversion of the excitons into hot electron hole pairs under photoexcitation at 3 eV. In our recent study (J. Am. Chem. Soc. 2015, 137, 5549), we demonstrated the generation of hot electrons in Mn-doped II-VI semiconductor quantum dots and their usefulness in photocatalytic H2 production reaction, taking advantage of the more efficient charge transfer of hot electrons compared with band-edge electrons. Here, we show that hot electrons produced in Mn-doped CdS/ZnS quantum dots possess sufficient kinetic energy to overcome the energy barrier from a 5.4-7.5 nm thick Al2 O3 layer producing a hot-electron current in photoelectrochemical cell. This work demonstrates the possibility of harvesting hot electrons not only at the interface of the doped quantum dot surface, but also far away from it, thus taking advantage of the capability of hot electrons for long-range electron transfer across a thick energy barrier. © 2016 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Ligand-Asymmetric Janus Quantum Dots for Efficient Blue-Quantum Dot Light-Emitting Diodes.

PubMed

Cho, Ikjun; Jung, Heeyoung; Jeong, Byeong Guk; Hahm, Donghyo; Chang, Jun Hyuk; Lee, Taesoo; Char, Kookheon; Lee, Doh C; Lim, Jaehoon; Lee, Changhee; Cho, Jinhan; Bae, Wan Ki

2018-06-19

We present ligand-asymmetric Janus quantum dots (QDs) to improve the device performance of quantum dot light-emitting diodes (QLEDs). Specifically, we devise blue QLEDs incorporating blue QDs with asymmetrically modified ligands, in which the bottom ligand of QDs in contact with ZnO electron-transport layer serves as a robust adhesive layer and an effective electron-blocking layer and the top ligand ensures uniform deposition of organic hole transport layers with enhanced hole injection properties. Suppressed electron overflow by the bottom ligand and stimulated hole injection enabled by the top ligand contribute synergistically to boost the balance of charge injection in blue QDs and therefore the device performance of blue QLEDs. As an ultimate achievement, the blue QLED adopting ligand-asymmetric QDs displays 2-fold enhancement in peak external quantum efficiency (EQE = 3.23%) compared to the case of QDs with native ligands (oleic acid) (peak EQE = 1.49%). The present study demonstrates an integrated strategy to control over the charge injection properties into QDs via ligand engineering that enables enhancement of the device performance of blue QLEDs and thus promises successful realization of white light-emitting devices using QDs.

Nonadiabatic dynamics of photo-induced proton-coupled electron transfer reactions via ring-polymer surface hopping

NASA Astrophysics Data System (ADS)

Shakib, Farnaz; Huo, Pengfei

Photo-induced proton-coupled electron transfer reactions (PCET) are at the heart of energy conversion reactions in photocatalysis. Here, we apply the recently developed ring-polymer surface-hopping (RPSH) approach to simulate the nonadiabatic dynamics of photo-induced PCET. The RPSH method incorporates ring-polymer (RP) quantization of the proton into the fewest-switches surface-hopping (FSSH) approach. Using two diabatic electronic states, corresponding to the electron donor and acceptor states, we model photo-induced PCET with the proton described by a classical isomorphism RP. From the RPSH method, we obtain numerical results that are comparable to those obtained when the proton is treated quantum mechanically. This accuracy stems from incorporating exact quantum statistics, such as proton tunnelling, into approximate quantum dynamics. Additionally, RPSH offers the numerical accuracy along with the computational efficiency. Namely, compared to the FSSH approach in vibronic representation, there is no need to calculate a massive number of vibronic states explicitly. This approach opens up the possibility to accurately and efficiently simulate photo-induced PCET with multiple transferring protons or electrons.

Deriving the exact nonadiabatic quantum propagator in the mapping variable representation.

PubMed

Hele, Timothy J H; Ananth, Nandini

2016-12-22

We derive an exact quantum propagator for nonadiabatic dynamics in multi-state systems using the mapping variable representation, where classical-like Cartesian variables are used to represent both continuous nuclear degrees of freedom and discrete electronic states. The resulting Liouvillian is a Moyal series that, when suitably approximated, can allow for the use of classical dynamics to efficiently model large systems. We demonstrate that different truncations of the exact Liouvillian lead to existing approximate semiclassical and mixed quantum-classical methods and we derive an associated error term for each method. Furthermore, by combining the imaginary-time path-integral representation of the Boltzmann operator with the exact Liouvillian, we obtain an analytic expression for thermal quantum real-time correlation functions. These results provide a rigorous theoretical foundation for the development of accurate and efficient classical-like dynamics to compute observables such as electron transfer reaction rates in complex quantized systems.

Coupled-Double-Quantum-Dot Environmental Information Engines: A Numerical Analysis

NASA Astrophysics Data System (ADS)

Tanabe, Katsuaki

2016-06-01

We conduct numerical simulations for an autonomous information engine comprising a set of coupled double quantum dots using a simple model. The steady-state entropy production rate in each component, heat and electron transfer rates are calculated via the probability distribution of the four electronic states from the master transition-rate equations. We define an information-engine efficiency based on the entropy change of the reservoir, implicating power generators that employ the environmental order as a new energy resource. We acquire device-design principles, toward the realization of corresponding practical energy converters, including that (1) higher energy levels of the detector-side reservoir than those of the detector dot provide significantly higher work production rates by faster states' circulation, (2) the efficiency is strongly dependent on the relative temperatures of the detector and system sides and becomes high in a particular Coulomb-interaction strength region between the quantum dots, and (3) the efficiency depends little on the system dot's energy level relative to its reservoir but largely on the antisymmetric relative amplitudes of the electronic tunneling rates.

Improving the performance of AlGaN-based deep-ultraviolet light-emitting diodes using electron blocking layer with a heart-shaped graded Al composition

NASA Astrophysics Data System (ADS)

Kwon, M. R.; Park, T. H.; Lee, T. H.; Lee, B. R.; Kim, T. G.

2018-04-01

We propose a design for highly efficient AlGaN-based deep-ultraviolet light-emitting diodes (DUV LEDs) using a heart-shaped graded Al composition electron-blocking layer (EBL). This novel structure reduced downward band bending at the interface between the last quantum barrier and the EBL and flattened the electrostatic field in the interlayer between the barriers of the multi-quantum barrier EBL. Consequently, electron leakage was significantly suppressed and hole injection efficiency was found to have improved. The parameter values of simulation were extracted from the experimental data of the reference DUV LEDs. Using the SimuLED, we compared the electrical and optical properties of three structures with different Al compositions in the active region and the EBL. The internal quantum efficiency of the proposed structure was shown to exceed those of the reference DUV LEDs by a factor of 1.9. Additionally, the output power at 20 mA was found to increase by a factor of 2.1.

Efficient analysis of mode profiles in elliptical microcavity using dynamic-thermal electron-quantum medium FDTD method.

PubMed

Khoo, E H; Ahmed, I; Goh, R S M; Lee, K H; Hung, T G G; Li, E P

2013-03-11

The dynamic-thermal electron-quantum medium finite-difference time-domain (DTEQM-FDTD) method is used for efficient analysis of mode profile in elliptical microcavity. The resonance peak of the elliptical microcavity is studied by varying the length ratio. It is observed that at some length ratios, cavity mode is excited instead of whispering gallery mode. This depicts that mode profiles are length ratio dependent. Through the implementation of the DTEQM-FDTD on graphic processing unit (GPU), the simulation time is reduced by 300 times as compared to the CPU. This leads to an efficient optimization approach to design microcavity lasers for wide range of applications in photonic integrated circuits.

Kelvin probe imaging of photo-injected electrons in metal oxide nanosheets from metal sulfide quantum dots under remote photochromic coloration

NASA Astrophysics Data System (ADS)

Kondo, A.; Yin, G.; Srinivasan, N.; Atarashi, D.; Sakai, E.; Miyauchi, M.

2015-07-01

Metal oxide and quantum dot (QD) heterostructures have attracted considerable recent attention as materials for developing efficient solar cells, photocatalysts, and display devices, thus nanoscale imaging of trapped electrons in these heterostructures provides important insight for developing efficient devices. In the present study, Kelvin probe force microscopy (KPFM) of CdS quantum dot (QD)-grafted Cs4W11O362- nanosheets was performed before and after visible-light irradiation. After visible-light excitation of the CdS QDs, the Cs4W11O362- nanosheet surface exhibited a decreased work function in the vicinity of the junction with CdS QDs, even though the Cs4W11O362- nanosheet did not absorb visible light. X-ray photoelectron spectroscopy revealed that W5+ species were formed in the nanosheet after visible-light irradiation. These results demonstrated that excited electrons in the CdS QDs were injected and trapped in the Cs4W11O362- nanosheet to form color centers. Further, the CdS QDs and Cs4W11O362- nanosheet composite films exhibited efficient remote photochromic coloration, which was attributed to the quantum nanostructure of the film. Notably, the responsive wavelength of the material is tunable by adjusting the size of QDs, and the decoloration rate is highly efficient, as the required length for trapped electrons to diffuse into the nanosheet surface is very short owing to its nanoscale thickness. The unique properties of this photochromic device make it suitable for display or memory applications. In addition, the methodology described in the present study for nanoscale imaging is expected to aid in the understanding of electron transport and trapping processes in metal oxide and metal chalcogenide heterostructure, which are crucial phenomena in QD-based solar cells and/or photocatalytic water-splitting systems.Metal oxide and quantum dot (QD) heterostructures have attracted considerable recent attention as materials for developing efficient solar cells, photocatalysts, and display devices, thus nanoscale imaging of trapped electrons in these heterostructures provides important insight for developing efficient devices. In the present study, Kelvin probe force microscopy (KPFM) of CdS quantum dot (QD)-grafted Cs4W11O362- nanosheets was performed before and after visible-light irradiation. After visible-light excitation of the CdS QDs, the Cs4W11O362- nanosheet surface exhibited a decreased work function in the vicinity of the junction with CdS QDs, even though the Cs4W11O362- nanosheet did not absorb visible light. X-ray photoelectron spectroscopy revealed that W5+ species were formed in the nanosheet after visible-light irradiation. These results demonstrated that excited electrons in the CdS QDs were injected and trapped in the Cs4W11O362- nanosheet to form color centers. Further, the CdS QDs and Cs4W11O362- nanosheet composite films exhibited efficient remote photochromic coloration, which was attributed to the quantum nanostructure of the film. Notably, the responsive wavelength of the material is tunable by adjusting the size of QDs, and the decoloration rate is highly efficient, as the required length for trapped electrons to diffuse into the nanosheet surface is very short owing to its nanoscale thickness. The unique properties of this photochromic device make it suitable for display or memory applications. In addition, the methodology described in the present study for nanoscale imaging is expected to aid in the understanding of electron transport and trapping processes in metal oxide and metal chalcogenide heterostructure, which are crucial phenomena in QD-based solar cells and/or photocatalytic water-splitting systems. Electronic supplementary information (ESI) available. See DOI: 10.1039/c5nr02405f

New Molecular Design Concurrently Providing Superior Pure Blue, Thermally Activated Delayed Fluorescence and Optical Out-Coupling Efficiencies.

PubMed

Rajamalli, P; Senthilkumar, N; Huang, P-Y; Ren-Wu, C-C; Lin, H-W; Cheng, C-H

2017-08-16

Simultaneous enhancement of out-coupling efficiency, internal quantum efficiency, and color purity in thermally activated delayed fluorescence (TADF) emitters is highly desired for the practical application of these materials. We designed and synthesized two isomeric TADF emitters, 2DPyM-mDTC and 3DPyM-pDTC, based on di(pyridinyl)methanone (DPyM) cores as the new electron-accepting units and di(tert-butyl)carbazole (DTC) as the electron-donating units. 3DPyM-pDTC, which is structurally nearly planar with a very small ΔE ST , shows higher color purity, horizontal ratio, and quantum yield than 2DPyM-mDTC, which has a more flexible structure. An electroluminescence device based on 3DPyM-pDTC as the dopant emitter can reach an extremely high external quantum efficiency of 31.9% with a pure blue emission. This work also demonstrates a way to design materials with a high portion of horizontal molecular orientation to realize a highly efficient pure-blue device based on TADF emitters.

High-Performance, Solution-Processed Quantum Dot Light-Emitting Field-Effect Transistors with a Scandium-Incorporated Indium Oxide Semiconductor.

PubMed

He, Penghui; Jiang, Congbiao; Lan, Linfeng; Sun, Sheng; Li, Yizhi; Gao, Peixiong; Zhang, Peng; Dai, Xingqiang; Wang, Jian; Peng, Junbiao; Cao, Yong

2018-05-22

Light-emitting field-effect transistors (LEFETs) have attained great attention due to their special characteristics of both the switching capacity and the electroluminescence capacity. However, high-performance LEFETs with high mobility, high brightness, and high efficiency have not been realized due to the difficulty in developing high electron and hole mobility materials with suitable band structures. In this paper, quantum dot hybrid LEFETs (QD-HLEFETs) combining high-luminous-efficiency quantum dots (QDs) and a solution-processed scandium-incorporated indium oxide (Sc:In 2 O 3 ) semiconductor were demonstrated. The red QD-HLEFET showed high electrical and optical performance with an electron mobility of 0.8 cm 2 V -1 s -1 , a maximum brightness of 13 400 cd/m 2 , and a maximum external quantum efficiency of 8.7%. The high performance of the QD-HLEFET is attributed to the good energy band matching between Sc:In 2 O 3 and QDs and the balanced hole and electron injection (less exciton nonradiative recombination). In addition, incorporation of Sc into In 2 O 3 can suppress the oxygen vacancy and free carrier generation and brings about excellent current and optical modulation (the on/off current ratio is 10 5 and the on/off brightness ratio is 10 6 ).

Measurement of Quantum Yield, Quantum Requirement, and Energetic Efficiency of the O2-Evolving System of Photosynthesis by a Simple Dye Reaction

NASA Astrophysics Data System (ADS)

Ros Barcelò, A.; Zapata, J. M.

1996-11-01

Photosynthesis is the conversion of absorbed radiant energy from sunlight into various forms of chemical energy by the chloroplasts of higher green plants. The overall process of photosynthesis consists of the oxidation of water (with the release of O2 as a product) and the reduction of CO2 to form carbohydrates. In the test tube electrons produced by the photolytic cleavage of H2) may be deviated from their true acceptor by inserting a suitable dye in the electron chain; i.e.; 2,6-dichlorophenol indophenol (DCPIP) (E'o = + 0.217 V), which is blue in the oxidized quinone form and which becomes colorless when reduced to the phenolic form. This dye-electrom acceptor also has the advantage that it accepts electroms directly from the quinone (Qa) electron-acceptor of the photosystem II< the reaction center associated with the O2-evolving (or water-slplitting) system. Based in the bleaching of DCPIP by illuminated spinach leaf chloroplasts, a classroom laboratory protocol has been developed to determine the quantum yield (QY = micromol O2 s-1 / micromol photons s-1, the quantum requirement (1/QY) and the energetic efficiency (f = chemical energy stored / light energy supplied) of the O2-evolving system of photosynthesis. Although values for the quantum yield, the quantum requirement and the energetic efficiency calculated in the classroom laboratory differ widely from those expected theoretically, these calculations are useful for illustrating the transformation of light energy into chemical energy by the chloroplasts of green plants.

Photoinduced Electron Transfer-based Halogen-free Photosensitizers: Covalent meso-Aryl (Phenyl, Naphthyl, Anthryl, and Pyrenyl) as Electron Donors to Effectively Induce the Formation of the Excited Triplet State and Singlet Oxygen for BODIPY Compounds.

PubMed

Zhang, Xian-Fu; Feng, Nan

2017-09-19

Pristine BODIPY compounds have negligible efficiency to generate the excited triplet state and singlet oxygen. In this report, we show that attaching a good electron donor to the BODIPY core can lead to singlet oxygen formation with up to 58 % quantum efficiency. For this purpose, BODIPYs with meso-aryl groups (phenyl, naphthyl, anthryl, and pyrenyl) were synthesized and characterized. The fluorescence, excited triplet state, and singlet oxygen formation properties for these compounds were measured in various solvents by UV/Vis absorption, steady-state and time-resolved fluorescence methods, as well as laser flash photolysis technique. In particular, the presence of anthryl and pyrenyl showed substantial enhancement on the singlet oxygen formation ability of BODIPY with up to 58 % and 34 % quantum efficiency, respectively, owing to their stronger electron-donating ability. Upon the increase in singlet oxygen formation, the fluorescence quantum yield and lifetime values of the aryl-BODIPY showed a concomitant decrease. The increase in solvent polarity enhances the singlet oxygen generation but decreases the fluorescence quantum yield. The results are explained by the presence of intramolecular photoinduced electron transfer from the aryl moiety to BODIPY core. This method of promoting T 1 formation is very different from the traditional heavy atom effect by I, Br, or transition metal atoms. This type of novel photosensitizers may find important applications in organic oxygenation reactions and photodynamic therapy of tumors. © 2017 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.

Characterization and Analysis of Integrated Silicon Photonic Detectors for High-Speed Communications

DTIC Science & Technology

2015-03-26

17 2.2.1.1 Depletion Region and Dark Current . . . . . . . . . . . . . . . . . 18 2.2.1.2 Photocurrent, Quantum ...facilitate a greater consciousness for the RF spectrum from MHz to ∼1 THz demonstrating an advantage over any purely electronic approach. Electronic... Quantum Efficiency and Responsivity. Extrapolating the established model from the dark current section provides the photodiode’s response when light

Conditional Dispersive Readout of a CMOS Single-Electron Memory Cell

NASA Astrophysics Data System (ADS)

Schaal, S.; Barraud, S.; Morton, J. J. L.; Gonzalez-Zalba, M. F.

2018-05-01

Quantum computers require interfaces with classical electronics for efficient qubit control, measurement, and fast data processing. Fabricating the qubit and the classical control layer using the same technology is appealing because it will facilitate the integration process, improving feedback speeds and offering potential solutions to wiring and layout challenges. Integrating classical and quantum devices monolithically, using complementary metal-oxide-semiconductor (CMOS) processes, enables the processor to profit from the most mature industrial technology for the fabrication of large-scale circuits. We demonstrate a CMOS single-electron memory cell composed of a single quantum dot and a transistor that locks charge on the quantum-dot gate. The single-electron memory cell is conditionally read out by gate-based dispersive sensing using a lumped-element L C resonator. The control field-effect transistor (FET) and quantum dot are fabricated on the same chip using fully depleted silicon-on-insulator technology. We obtain a charge sensitivity of δ q =95 ×10-6e Hz-1 /2 when the quantum-dot readout is enabled by the control FET, comparable to results without the control FET. Additionally, we observe a single-electron retention time on the order of a second when storing a single-electron charge on the quantum dot at millikelvin temperatures. These results demonstrate first steps towards time-based multiplexing of gate-based dispersive readout in CMOS quantum devices opening the path for the development of an all-silicon quantum-classical processor.

Theory of electronic and optical properties for different shapes of InAs/In0.52Al0.48As quantum wires

NASA Astrophysics Data System (ADS)

Bouazra, A.; Nasrallah, S. Abdi-Ben; Said, M.

2016-01-01

In this work, we propose an efficient method to investigate optical properties as well as their dependence on geometrical parameters in InAs/InAlAs quantum wires. The used method is based on the coordinate transformation and the finite difference method. It provides sufficient accuracy, stability and flexibility with respect to the size and shape of the quantum wire. The electron and hole energy levels as well as their corresponding wave functions are investigated for different shape of quantum wires. The optical transition energies, the emission wavelengths and the oscillator strengths are also studied.

A Synthetic Approach to the Transfer Matrix Method in Classical and Quantum Physics

ERIC Educational Resources Information Center

Pujol, O.; Perez, J. P.

2007-01-01

The aim of this paper is to propose a synthetic approach to the transfer matrix method in classical and quantum physics. This method is an efficient tool to deal with complicated physical systems of practical importance in geometrical light or charged particle optics, classical electronics, mechanics, electromagnetics and quantum physics. Teaching…

Photoinduced electron transfer from semiconductor quantum dots to metal oxide nanoparticles

PubMed Central

Tvrdy, Kevin; Frantsuzov, Pavel A.; Kamat, Prashant V.

2011-01-01

Quantum dot-metal oxide junctions are an integral part of next-generation solar cells, light emitting diodes, and nanostructured electronic arrays. Here we present a comprehensive examination of electron transfer at these junctions, using a series of CdSe quantum dot donors (sizes 2.8, 3.3, 4.0, and 4.2 nm in diameter) and metal oxide nanoparticle acceptors (SnO2, TiO2, and ZnO). Apparent electron transfer rate constants showed strong dependence on change in system free energy, exhibiting a sharp rise at small driving forces followed by a modest rise further away from the characteristic reorganization energy. The observed trend mimics the predicted behavior of electron transfer from a single quantum state to a continuum of electron accepting states, such as those present in the conduction band of a metal oxide nanoparticle. In contrast with dye-sensitized metal oxide electron transfer studies, our systems did not exhibit unthermalized hot-electron injection due to relatively large ratios of electron cooling rate to electron transfer rate. To investigate the implications of these findings in photovoltaic cells, quantum dot-metal oxide working electrodes were constructed in an identical fashion to the films used for the electron transfer portion of the study. Interestingly, the films which exhibited the fastest electron transfer rates (SnO2) were not the same as those which showed the highest photocurrent (TiO2). These findings suggest that, in addition to electron transfer at the quantum dot-metal oxide interface, other electron transfer reactions play key roles in the determination of overall device efficiency. PMID:21149685

Photoinduced electron transfer from semiconductor quantum dots to metal oxide nanoparticles.

PubMed

Tvrdy, Kevin; Frantsuzov, Pavel A; Kamat, Prashant V

2011-01-04

Quantum dot-metal oxide junctions are an integral part of next-generation solar cells, light emitting diodes, and nanostructured electronic arrays. Here we present a comprehensive examination of electron transfer at these junctions, using a series of CdSe quantum dot donors (sizes 2.8, 3.3, 4.0, and 4.2 nm in diameter) and metal oxide nanoparticle acceptors (SnO(2), TiO(2), and ZnO). Apparent electron transfer rate constants showed strong dependence on change in system free energy, exhibiting a sharp rise at small driving forces followed by a modest rise further away from the characteristic reorganization energy. The observed trend mimics the predicted behavior of electron transfer from a single quantum state to a continuum of electron accepting states, such as those present in the conduction band of a metal oxide nanoparticle. In contrast with dye-sensitized metal oxide electron transfer studies, our systems did not exhibit unthermalized hot-electron injection due to relatively large ratios of electron cooling rate to electron transfer rate. To investigate the implications of these findings in photovoltaic cells, quantum dot-metal oxide working electrodes were constructed in an identical fashion to the films used for the electron transfer portion of the study. Interestingly, the films which exhibited the fastest electron transfer rates (SnO(2)) were not the same as those which showed the highest photocurrent (TiO(2)). These findings suggest that, in addition to electron transfer at the quantum dot-metal oxide interface, other electron transfer reactions play key roles in the determination of overall device efficiency.

A linear triple quantum dot system in isolated configuration

NASA Astrophysics Data System (ADS)

Flentje, Hanno; Bertrand, Benoit; Mortemousque, Pierre-André; Thiney, Vivien; Ludwig, Arne; Wieck, Andreas D.; Bäuerle, Christopher; Meunier, Tristan

2017-06-01

The scaling up of electron spin qubit based nanocircuits has remained challenging up till date and involves the development of efficient charge control strategies. Here, we report on the experimental realization of a linear triple quantum dot in a regime isolated from the reservoir. We show how this regime can be reached with a fixed number of electrons. Charge stability diagrams of the one, two, and three electron configurations where only electron exchange between the dots is allowed are observed. They are modeled with the established theory based on a capacitive model of the dot systems. The advantages of the isolated regime with respect to experimental realizations of quantum simulators and qubits are discussed. We envision that the results presented here will make more manipulation schemes for existing qubit implementations possible and will ultimately allow to increase the number of tunnel coupled quantum dots which can be simultaneously controlled.

QUANTUM ESPRESSO: a modular and open-source software project for quantum simulations of materials.

PubMed

Giannozzi, Paolo; Baroni, Stefano; Bonini, Nicola; Calandra, Matteo; Car, Roberto; Cavazzoni, Carlo; Ceresoli, Davide; Chiarotti, Guido L; Cococcioni, Matteo; Dabo, Ismaila; Dal Corso, Andrea; de Gironcoli, Stefano; Fabris, Stefano; Fratesi, Guido; Gebauer, Ralph; Gerstmann, Uwe; Gougoussis, Christos; Kokalj, Anton; Lazzeri, Michele; Martin-Samos, Layla; Marzari, Nicola; Mauri, Francesco; Mazzarello, Riccardo; Paolini, Stefano; Pasquarello, Alfredo; Paulatto, Lorenzo; Sbraccia, Carlo; Scandolo, Sandro; Sclauzero, Gabriele; Seitsonen, Ari P; Smogunov, Alexander; Umari, Paolo; Wentzcovitch, Renata M

2009-09-30

QUANTUM ESPRESSO is an integrated suite of computer codes for electronic-structure calculations and materials modeling, based on density-functional theory, plane waves, and pseudopotentials (norm-conserving, ultrasoft, and projector-augmented wave). The acronym ESPRESSO stands for opEn Source Package for Research in Electronic Structure, Simulation, and Optimization. It is freely available to researchers around the world under the terms of the GNU General Public License. QUANTUM ESPRESSO builds upon newly-restructured electronic-structure codes that have been developed and tested by some of the original authors of novel electronic-structure algorithms and applied in the last twenty years by some of the leading materials modeling groups worldwide. Innovation and efficiency are still its main focus, with special attention paid to massively parallel architectures, and a great effort being devoted to user friendliness. QUANTUM ESPRESSO is evolving towards a distribution of independent and interoperable codes in the spirit of an open-source project, where researchers active in the field of electronic-structure calculations are encouraged to participate in the project by contributing their own codes or by implementing their own ideas into existing codes.

Quantum Otto engine using a single ion and a single thermal bath

NASA Astrophysics Data System (ADS)

Biswas, Asoka; Chand, Suman

2016-05-01

Quantum heat engines employ a quantum system as the working fluid, that gives rise to large work efficiency, beyond the limit for classical heat engines. Existing proposals for implementing quantum heat engines require that the system interacts with the hot bath and the cold bath (both modelled as a classical system) in an alternative fashion and therefore assumes ability to switch off the interaction with the bath during a certain stage of the heat-cycle. However, it is not possible to decouple a quantum system from its always-on interaction with the bath without use of complex pulse sequences. It is also hard to identify two different baths at two different temperatures in quantum domain, that sequentially interact with the system. Here, we show how to implement a quantum Otto engine without requiring to decouple the bath in a sequential manner. This is done by considering a single thermal bath, coupled to a single trapped ion. The electronic degree of freedom of the ion is chosen as a two-level working fluid while the vibrational degree of freedom plays the role of the cold bath. Measuring the electronic state mimics the release of heat into the cold bath. Thus, our model is fully quantum and exhibits very large work efficiency, asymptotically close to unity.

High-fidelity quantum gates on quantum-dot-confined electron spins in low-Q optical microcavities

NASA Astrophysics Data System (ADS)

Li, Tao; Gao, Jian-Cun; Deng, Fu-Guo; Long, Gui-Lu

2018-04-01

We propose some high-fidelity quantum circuits for quantum computing on electron spins of quantum dots (QD) embedded in low-Q optical microcavities, including the two-qubit controlled-NOT gate and the multiple-target-qubit controlled-NOT gate. The fidelities of both quantum gates can, in principle, be robust to imperfections involved in a practical input-output process of a single photon by converting the infidelity into a heralded error. Furthermore, the influence of two different decay channels is detailed. By decreasing the quality factor of the present microcavity, we can largely increase the efficiencies of these quantum gates while their high fidelities remain unaffected. This proposal also has another advantage regarding its experimental feasibility, in that both quantum gates can work faithfully even when the QD-cavity systems are non-identical, which is of particular importance in current semiconductor QD technology.

Electrical control of charged carriers and excitons in atomically thin materials

NASA Astrophysics Data System (ADS)

Wang, Ke; De Greve, Kristiaan; Jauregui, Luis A.; Sushko, Andrey; High, Alexander; Zhou, You; Scuri, Giovanni; Taniguchi, Takashi; Watanabe, Kenji; Lukin, Mikhail D.; Park, Hongkun; Kim, Philip

2018-02-01

Electrical confinement and manipulation of charge carriers in semiconducting nanostructures are essential for realizing functional quantum electronic devices1-3. The unique band structure4-7 of atomically thin transition metal dichalcogenides (TMDs) offers a new route towards realizing novel 2D quantum electronic devices, such as valleytronic devices and valley-spin qubits8. 2D TMDs also provide a platform for novel quantum optoelectronic devices9-11 due to their large exciton binding energy12,13. However, controlled confinement and manipulation of electronic and excitonic excitations in TMD nanostructures have been technically challenging due to the prevailing disorder in the material, preventing accurate experimental control of local confinement and tunnel couplings14-16. Here we demonstrate a novel method for creating high-quality heterostructures composed of atomically thin materials that allows for efficient electrical control of excitations. Specifically, we demonstrate quantum transport in the gate-defined, quantum-confined region, observing spin-valley locked quantized conductance in quantum point contacts. We also realize gate-controlled Coulomb blockade associated with confinement of electrons and demonstrate electrical control over charged excitons with tunable local confinement potentials and tunnel couplings. Our work provides a basis for novel quantum opto-electronic devices based on manipulation of charged carriers and excitons.

Quantum Dot Sensitized Solar Cells Based on TiO2/AgInS2

NASA Astrophysics Data System (ADS)

Pawar, Sachin A.; Jeong, Jae Pil; Patil, Dipali S.; More, Vivek M.; Lee, Rochelle S.; Shin, Jae Cheol; Choi, Won Jun

2018-05-01

Quantum dot heterojunctions with type-II band alignment can efficiently separate photogenerated electron-hole pairs and, hence, are useful for solar cell studies. In this study, a quantum dot sensitized solar cell (QDSSC) made of TiO2/AgInS2 is achieved to boost the photoconversion efficiency for the TiO2-based system by varying the AgInS2 layer's thickness. The TiO2 nanorods array film is prepared by using a simple hydrothermal technique. The formation of a AgInS2 QD-sensitized TiO2-nanorod photoelectrode is carried out by successive ionic layer adsorption and reaction (SILAR) technique. The effect of the QD layer on the performance of the solar cell is studied by varying the SILAR cycles of the QD coating. The synthesized electrode materials are characterized by using X-ray diffraction, X-ray photoelectron spectroscopy, field emission scanning electron microscopy, high resolution transmission electron microscopy and solar cell performances. The results indicate that the nanocrystals have effectively covered the outer surfaces of the TiO2 nanorods. The interfacial structure of quantum dots (QDs)/TiO2 is also investigated, and the growth interface is verified. A careful comparison between TiO2/AgInS2 sensitized cells reveals that the trasfer of electrons and hole proceeds efficiently, the recombination is suppressed for the optimum thickness of the QD layer and light from the entire visible spectrum is utilised. Under AM 1.5G illumination, a high photocurrent of 1.36 mAcm-2 with an improved power conversion efficiency of 0.48% is obtained. The solar cell properties of our photoanodes suggest that the TiO2 nanorod array films co-sensitized by AgInS2 nanoclusters have potential applications in solar cells.

Multiple exciton generation for photoelectrochemical hydrogen evolution reactions with quantum yields exceeding 100%

DOE PAGES

Yan, Yong; Crisp, Ryan W.; Gu, Jing; ...

2017-04-03

Multiple exciton generation (MEG) in quantum dots (QDs) has the potential to greatly increase the power conversion efficiency in solar cells and in solar-fuel production. During the MEG process, two electron-hole pairs (excitons) are created from the absorption of one high-energy photon, bypassing hot-carrier cooling via phonon emission. Here we demonstrate that extra carriers produced via MEG can be used to drive a chemical reaction with quantum efficiency above 100%. We developed a lead sulfide (PbS) QD photoelectrochemical cell that is able to drive hydrogen evolution from aqueous Na 2S solution with a peak external quantum efficiency exceeding 100%. QDmore » photoelectrodes that were measured all demonstrated MEG when the incident photon energy was larger than 2.7 times the bandgap energy. Finally, our results demonstrate a new direction in exploring high-efficiency approaches to solar fuels.« less

Quantum dot solar cells. Tuning photoresponse through size and shape control of CdSe-TiO2 architecture.

PubMed

Kongkanand, Anusorn; Tvrdy, Kevin; Takechi, Kensuke; Kuno, Masaru; Kamat, Prashant V

2008-03-26

Different-sized CdSe quantum dots have been assembled on TiO2 films composed of particle and nanotube morphologies using a bifunctional linker molecule. Upon band-gap excitation, CdSe quantum dots inject electrons into TiO2 nanoparticles and nanotubes, thus enabling the generation of photocurrent in a photoelectrochemical solar cell. The results presented in this study highlight two major findings: (i) ability to tune the photoelectrochemical response and photoconversion efficiency via size control of CdSe quantum dots and (ii) improvement in the photoconversion efficiency by facilitating the charge transport through TiO2 nanotube architecture. The maximum IPCE (photon-to-charge carrier generation efficiency) obtained with 3 nm diameter CdSe nanoparticles was 35% for particulate TiO2 and 45% for tubular TiO2 morphology. The maximum IPCE observed at the excitonic band increases with decreasing particle size, whereas the shift in the conduction band to more negative potentials increases the driving force and favors fast electron injection. The maximum power-conversion efficiency

Improving hole injection efficiency by manipulating the hole transport mechanism through p-type electron blocking layer engineering.

PubMed

Zhang, Zi-Hui; Ju, Zhengang; Liu, Wei; Tan, Swee Tiam; Ji, Yun; Kyaw, Zabu; Zhang, Xueliang; Hasanov, Namig; Sun, Xiao Wei; Demir, Hilmi Volkan

2014-04-15

The p-type AlGaN electron blocking layer (EBL) is widely used in InGaN/GaN light-emitting diodes (LEDs) for electron overflow suppression. However, a typical EBL also reduces the hole injection efficiency, because holes have to climb over the energy barrier generated at the p-AlGaN/p-GaN interface before entering the quantum wells. In this work, to address this problem, we report the enhancement of hole injection efficiency by manipulating the hole transport mechanism through insertion of a thin GaN layer of 1 nm into the p-AlGaN EBL and propose an AlGaN/GaN/AlGaN-type EBL outperforming conventional AlGaN EBLs. Here, the position of the inserted thin GaN layer relative to the p-GaN region is found to be the key to enhancing the hole injection efficiency. InGaN/GaN LEDs with the proposed p-type AlGaN/GaN/AlGaN EBL have demonstrated substantially higher optical output power and external quantum efficiency.

Radio-frequency measurement of an asymmetric single electron transistor

NASA Astrophysics Data System (ADS)

Ji, Zhongqing; Xue, Weiwei; Rimberg, A. J.

2007-03-01

Since the invention of the radio-frequency single-electron transistor (RF-SET) by Schoelkopf et al.,[1] most measurements have focused on the symmetric single electron transistor. It has been shown, however, that the symmetric SET has a rather low measurement efficiency in its normal working regime.[2][3] Recently, it has been pointed out that an asymmetric SET can be considerably more efficient than a symmetric SET as a quantum amplifier. In this case the measurement efficiency of the asymmetric SET becomes similar to that of the quantum point contact (QPC) detector which can approach the quantum limit. We investigate the asymmetric SET by fabricating Al/AlOx SETs with junction areas 40x40 nm^2 and 40x80nm^2 and total resistance of about 25kφ. The results of RF and DC characterization of such asymmetric SETs will be discussed. [1] R. J. Schoelkopf, P. Wahlgren, A. A. Kozhevnikov, P. Delsing, D. E. Prober, Science, 280, 1242 (1998). [2] A. N. Korotkov, Phys. Rev. B, 63, 085312 (2001); 63, 115403 (2001). [3] D. Mozyrsky, I. Martin, and M. B. Hastings, Phys. Rev. Lett., 92, 018303 (2004). [4] S. A. Gurvitz and G. P. Berman, Phys. Rev. B, 72 , 073303(2005).

Quantum efficiencies exceeding unity in amorphous silicon solar cells

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

Vanmaekelbergh, D.; Lagemaat, J. van de; Schropp, R.E.I.

1994-12-31

The experimental observation of internal quantum efficiencies above unity in crystalline silicon solar cells has brought up the question whether the generation of multiple electron/hole pairs has to be taken into consideration also in solar cells based on direct gap amorphous semiconductors. To study photogenerated carrier dynamics, the authors have applied Intensity Modulated Photocurrent Spectroscopy (IMPS) to hydrogenated amorphous silicon p-i-n solar cells. In the reverse voltage bias region at low illumination intensities it has been observed that the low frequency limit of the AC quantum yield Y increases significantly above unit with decreasing light intensity, indicating that more thanmore » one electron per photon is detected in the external circuit. This phenomenon can be explained by considering trapping and thermal emission of photogenerated carriers at intragap atmospheric dangling bond defect centers.« less

Effect of interface roughness on Auger recombination in semiconductor quantum wells

NASA Astrophysics Data System (ADS)

Tan, Chee-Keong; Sun, Wei; Wierer, Jonathan J.; Tansu, Nelson

2017-03-01

Auger recombination in a semiconductor is a three-carrier process, wherein the energy from the recombination of an electron and hole pair promotes a third carrier to a higher energy state. In semiconductor quantum wells with increased carrier densities, the Auger recombination becomes an appreciable fraction of the total recombination rate and degrades luminescence efficiency. Gaining insight into the variables that influence Auger recombination in semiconductor quantum wells could lead to further advances in optoelectronic and electronic devices. Here we demonstrate the important role that interface roughness has on Auger recombination within quantum wells. Our computational studies find that as the ratio of interface roughness to quantum well thickness is increased, Auger recombination is significantly enhanced. Specifically, when considering a realistic interface roughness for an InGaN quantum well, the enhancement in Auger recombination rate over a quantum well with perfect heterointerfaces can be approximately four orders of magnitude.

The influence of annealing temperature on the interface and photovoltaic properties of CdS/CdSe quantum dots sensitized ZnO nanorods solar cells.

PubMed

Qiu, Xiaofeng; Chen, Ling; Gong, Haibo; Zhu, Min; Han, Jun; Zi, Min; Yang, Xiaopeng; Ji, Changjian; Cao, Bingqiang

2014-09-15

Arrays of ZnO/CdS/CdSe core/shell nanocables with different annealing temperatures have been investigated for CdS/CdSe quantum dots sensitized solar cells (QDSSCs). CdS/CdSe quantum dots were synthesized on the surface of ZnO nanorods that serve as the scaffold via a simple ion-exchange approach. The uniform microstructure was verified by scanning electron microscope and transmission electron microscope. UV-Visible absorption spectrum and Raman spectroscopy analysis indicated noticeable influence of annealing temperature on the interface structural and optical properties of the CdS/CdSe layers. Particularly, the relationship between annealing temperatures and photovoltaic performance of the corresponding QDSSCs was investigated employing photovoltaic conversion, quantum efficiency and electrochemical impedance spectra. It is demonstrated that higher cell efficiency can be obtained by optimizing the annealing temperature through extending the photoresponse range and improving QD layer crystal quality. Copyright © 2014 Elsevier Inc. All rights reserved.

Photoinduced Single- and Multiple-Electron Dynamics Processes Enhanced by Quantum Confinement in Lead Halide Perovskite Quantum Dots

DOE PAGES

Vogel, Dayton J.; Kryjevski, Andrei; Inerbaev, Talgat; ...

2017-03-21

Methylammonium lead iodide perovskite (MAPbI 3) is a promising material for photovoltaic devices. A modification of MAPbI 3 into confined nanostructures is expected to further increase efficiency of solar energy conversion. Photoexcited dynamic processes in a MAPbI3 quantum dot (QD) have been modeled by many-body perturbation theory and nonadiabatic dynamics. A photoexcitation is followed by either exciton cooling (EC), its radiative (RR) or nonradiative recombination (NRR), or multiexciton generation (MEG) processes. Computed times of these processes fall in the order of MEG < EC < RR < NRR, where MEG is on the order of a few femtoseconds, EC ismore » in the picosecond range, while RR and NRR are on the order of nanoseconds. Computed time scales indicate which electronic transition pathways can contribute to increase in charge collection efficiency. Simulated mechanisms of relaxation and their rates show that quantum confinement promotes MEG in MAPbI 3 QDs.« less

Nanometer-scale monitoring of quantum-confined Stark effect and emission efficiency droop in multiple GaN/AlN quantum disks in nanowires

NASA Astrophysics Data System (ADS)

Zagonel, L. F.; Tizei, L. H. G.; Vitiello, G. Z.; Jacopin, G.; Rigutti, L.; Tchernycheva, M.; Julien, F. H.; Songmuang, R.; Ostasevicius, T.; de la Peña, F.; Ducati, C.; Midgley, P. A.; Kociak, M.

2016-05-01

We report on a detailed study of the intensity dependent optical properties of individual GaN/AlN quantum disks (QDisks) embedded into GaN nanowires (NW). The structural and optical properties of the QDisks were probed by high spatial resolution cathodoluminescence (CL) in a scanning transmission electron microscope (STEM). By exciting the QDisks with a nanometric electron beam at currents spanning over three orders of magnitude, strong nonlinearities (energy shifts) in the light emission are observed. In particular, we find that the amount of energy shift depends on the emission rate and on the QDisk morphology (size, position along the NW and shell thickness). For thick QDisks (>4 nm), the QDisk emission energy is observed to blueshift with the increase of the emission intensity. This is interpreted as a consequence of the increase of carriers density excited by the incident electron beam inside the QDisks, which screens the internal electric field and thus reduces the quantum confined Stark effect (QCSE) present in these QDisks. For thinner QDisks (<3 nm ), the blueshift is almost absent in agreement with the negligible QCSE at such sizes. For QDisks of intermediate sizes there exists a current threshold above which the energy shifts, marking the transition from unscreened to partially screened QCSE. From the threshold value we estimate the lifetime in the unscreened regime. These observations suggest that, counterintuitively, electrons of high energy can behave ultimately as single electron-hole pair generators. In addition, when we increase the current from 1 to 10 pA the light emission efficiency drops by more than one order of magnitude. This reduction of the emission efficiency is a manifestation of the "efficiency droop" as observed in nitride-based 2D light emitting diodes, a phenomenon tentatively attributed to the Auger effect.

Valley filters, accumulators, and switches induced in graphene quantum dots by lines of adsorbed hydrogen atoms

NASA Astrophysics Data System (ADS)

Azari, Mohammadhadi; Kirczenow, George

2018-06-01

We present electronic structure and quantum transport calculations that predict conducting channels induced in graphene quantum dots by lines of adsorbed hydrogen atoms to function as highly efficient, experimentally realizable valley filters, accumulators, and switches. The underlying physics is an interesting property of graphene Dirac point resonances (DPRs) that is revealed here, namely, that an electric current passing through a DPR-mediated conducting channel in a given direction is carried by electrons of only one of the two graphene valleys. Our predictions apply to lines of hydrogen atoms adsorbed on graphene quantum dots that are either free standing or supported on a hexagonal boron nitride substrate.

Spin-dependent Otto quantum heat engine based on a molecular substance

NASA Astrophysics Data System (ADS)

Hübner, W.; Lefkidis, G.; Dong, C. D.; Chaudhuri, D.; Chotorlishvili, L.; Berakdar, J.

2014-07-01

We explore the potential of single molecules for thermodynamic cycles. To this end we propose two molecular heat engines based on the Ni2 dimer in the presence of a static magnetic field: (a) a quantum Otto engine and (b) a modified quantum Otto engine for which optical excitations induced by a laser pulse substitute for one of the heat-exchange points. For reliable predictions and to inspect the role of spin and electronic correlations we perform fully correlated ab initio calculations of the molecular electronic structure including spin-orbital effects. We analyze the efficiency of the engines in dependence of the electronic level scheme and the entanglement and find a significant possible enhancement connected to the quantum nature and the heat capacity of the dimer, as well as to the zero-field triplet states splitting.

Microscopic model for intersubband gain from electrically pumped quantum-dot structures

DOE PAGES

Michael, Stephan; Chow, Weng Wah; Schneider, Han Christian

2014-10-03

We study theoretically the performance of electrically pumped self-organized quantum dots as a gain material in the mid-infrared range at room temperature. We analyze an AlGaAs/InGaAs based structure composed of dots-in-a-well sandwiched between two quantum wells. We numerically analyze a comprehensive model by combining a many-particle approach for electronic dynamics with a realistic modeling of the electronic states in the whole structure. We investigate the gain both for quasi-equilibrium conditions and current injection. We find, comparing different structures, that steady-state gain can only be realized by an efficient extraction process, which prevents an accumulation of electrons in continuum states, thatmore » make the available scattering pathways through the quantum-dot active region too fast to sustain inversion.« less

Flexible deep-ultraviolet light-emitting diodes for significant improvement of quantum efficiencies by external bending

NASA Astrophysics Data System (ADS)

Shervin, Shahab; Oh, Seung Kyu; Park, Hyun Jung; Lee, Keon-Hwa; Asadirad, Mojtaba; Kim, Seung-Hwan; Kim, Jeomoh; Pouladi, Sara; Lee, Sung-Nam; Li, Xiaohang; Kwak, Joon Seop; Ryou, Jae-Hyun

2018-03-01

We report a new route to improve quantum efficiencies of AlGaN-based deep-ultraviolet light-emitting diodes (DUV LEDs) using mechanical flexibility of recently developed bendable thin-film structures. Numerical studies show that electronic band structures of AlGaN heterostructures and resulting optical and electrical characteristics of the devices can be significantly modified by external bending through active control of piezoelectric polarization. Internal quantum efficiency is enhanced higher than three times, when the DUV LEDs are moderately bent with concave curvatures. Furthermore, an efficiency droop at high injection currents is mitigated and turn-on voltage of diodes decreases with the same bending condition. The concept of bendable DUV LEDs with a controlled external strain can provide a new path for high-output-power and high-efficiency devices.

Comparison of exciplex generation under optical and X-ray excitation

NASA Astrophysics Data System (ADS)

Kipriyanov, A. A.; Melnikov, A. R.; Stass, D. V.; Doktorov, A. B.

2017-09-01

Exciplex generation under optical and X-ray excitation in identical conditions is experimentally compared using a specially chosen model donor-acceptor system, anthracene (electron acceptor) and N,N-dimethylaniline (electron donor) in non-polar solution, and the results are analyzed and interpreted based on analytically calculated luminescence quantum yields. Calculations are performed on the basis of kinetic equations for multistage schemes of bulk exciplex production reaction under optical excitation and combination of bulk and geminate reactions of radical ion pairs under X-ray excitation. These results explain the earlier experimentally found difference in the ratio of the quantum yields of exciplexes and excited electron acceptors (exciplex generation efficiency) and the corresponding change in the exciplex generation efficiency under X-irradiation as compared to the reaction under optical excitation.

Comparison of exciplex generation under optical and X-ray excitation.

PubMed

Kipriyanov, A A; Melnikov, A R; Stass, D V; Doktorov, A B

2017-09-07

Exciplex generation under optical and X-ray excitation in identical conditions is experimentally compared using a specially chosen model donor-acceptor system, anthracene (electron acceptor) and N,N-dimethylaniline (electron donor) in non-polar solution, and the results are analyzed and interpreted based on analytically calculated luminescence quantum yields. Calculations are performed on the basis of kinetic equations for multistage schemes of bulk exciplex production reaction under optical excitation and combination of bulk and geminate reactions of radical ion pairs under X-ray excitation. These results explain the earlier experimentally found difference in the ratio of the quantum yields of exciplexes and excited electron acceptors (exciplex generation efficiency) and the corresponding change in the exciplex generation efficiency under X-irradiation as compared to the reaction under optical excitation.

A comprehensive evaluation of factors that influence the spin polarization of electrons emitted from bulk GaAs photocathodes

DOE PAGES

Liu, Wei; Poelker, Matt; Peng, Xincun; ...

2017-07-19

Here, the degree of polarization of photoemitted electrons extracted from bulk unstrained GaAs photocathodes is usually considerably less than the theoretical maximum value of 50%, as a result of depolarization mechanisms that originate within the photocathode material and at the vacuum surface interface. This paper provides a comprehensive review of depolarization mechanisms and presents a systematic experimental evaluation of polarization sensitivities to temperature, dopant density, quantum efficiency, and crystal orientation. The highest measured polarization was similar to 50%, consistent with the maximum theoretical value, obtained from a photocathode sample with relatively low dopant concentration and cooled to 77 K. Inmore » general, measurements indicate electron spin polarization can be enhanced at the expense of photoelectron yield (or quantum efficiency).« less

A comprehensive evaluation of factors that influence the spin polarization of electrons emitted from bulk GaAs photocathodes

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

Liu, Wei; Poelker, Matt; Peng, Xincun

Here, the degree of polarization of photoemitted electrons extracted from bulk unstrained GaAs photocathodes is usually considerably less than the theoretical maximum value of 50%, as a result of depolarization mechanisms that originate within the photocathode material and at the vacuum surface interface. This paper provides a comprehensive review of depolarization mechanisms and presents a systematic experimental evaluation of polarization sensitivities to temperature, dopant density, quantum efficiency, and crystal orientation. The highest measured polarization was similar to 50%, consistent with the maximum theoretical value, obtained from a photocathode sample with relatively low dopant concentration and cooled to 77 K. Inmore » general, measurements indicate electron spin polarization can be enhanced at the expense of photoelectron yield (or quantum efficiency).« less

Adiabatic quantum simulation of quantum chemistry.

PubMed

Babbush, Ryan; Love, Peter J; Aspuru-Guzik, Alán

2014-10-13

We show how to apply the quantum adiabatic algorithm directly to the quantum computation of molecular properties. We describe a procedure to map electronic structure Hamiltonians to 2-body qubit Hamiltonians with a small set of physically realizable couplings. By combining the Bravyi-Kitaev construction to map fermions to qubits with perturbative gadgets to reduce the Hamiltonian to 2-body, we obtain precision requirements on the coupling strengths and a number of ancilla qubits that scale polynomially in the problem size. Hence our mapping is efficient. The required set of controllable interactions includes only two types of interaction beyond the Ising interactions required to apply the quantum adiabatic algorithm to combinatorial optimization problems. Our mapping may also be of interest to chemists directly as it defines a dictionary from electronic structure to spin Hamiltonians with physical interactions.

Visible light-driven water oxidation promoted by host-guest interaction between photosensitizer and catalyst with a high quantum efficiency.

PubMed

Li, Hua; Li, Fei; Zhang, Biaobiao; Zhou, Xu; Yu, Fengshou; Sun, Licheng

2015-04-08

A highly active supramolecular system for visible light-driven water oxidation was developed with cyclodextrin-modified ruthenium complex as the photosensitizer, phenyl-modified ruthenium complexes as the catalysts, and sodium persulfate as the sacrificial electron acceptor. The catalysts were found to form 1:1 host-guest adducts with the photosensitizer. Stopped-flow measurement revealed the host-guest interaction is essential to facilitate the electron transfer from catalyst to sensitizer. As a result, a remarkable quantum efficiency of 84% was determined under visible light irradiation in neutral aqueous phosphate buffer. This value is nearly 1 order of magnitude higher than that of noninteraction system, indicating that the noncovalent incorporation of sensitizer and catalyst is an appealing approach for efficient conversion of solar energy into fuels.

Will spin-relaxation times in molecular magnets permit quantum information processing?

NASA Astrophysics Data System (ADS)

Ardavan, Arzhang

2007-03-01

Certain computational tasks can be efficiently implemented using quantum logic, in which the information-carrying elements are permitted to exist in quantum superpositions. To achieve this in practice, a physical system that is suitable for embodying quantum bits (qubits) must be identified. Some proposed scenarios employ electron spins in the solid state, for example phosphorous donors in silicon, quantum dots, heterostructures and endohedral fullerenes, motivated by the long electron-spin relaxation times exhibited by these systems. An alternative electron-spin based proposal exploits the large number of quantum states and the non-degenerate transitions available in high spin molecular magnets. Although these advantages have stimulated vigorous research in molecular magnets, the key question of whether the intrinsic spin relaxation times are long enough has hitherto remained unaddressed. Using X-band pulsed electron spin resonance, we measure the intrinsic spin-lattice (T1) and phase coherence (T2) relaxation times in molecular nanomagnets for the first time. In Cr7M heterometallic wheels, with M = Ni and Mn, phase coherence relaxation is dominated by the coupling of the electron spin to protons within the molecule. In deuterated samples T2 reaches 3 μs at low temperatures, which is several orders of magnitude longer than the duration of spin manipulations, satisfying a prerequisite for the deployment of molecular nanomagnets in quantum information applications.

Improvement of Charge Transportation in Si Quantum Dot-Sensitized Solar Cells Using Vanadium Doped TiO2.

PubMed

Seo, Hyunwoong; Ichida, Daiki; Hashimoto, Shinji; Itagaki, Naho; Koga, Kazunori; Shiratani, Masaharu; Nam, Sang-Hun; Boo, Jin-Hyo

2016-05-01

The multiple exciton generation characteristics of quantum dots have been expected to enhance the performance of photochemical solar cells. In previous work, we first introduced Si quantum dot for sensitized solar cells. The Si quantum dots were fabricated by multi-hollow discharge plasma chemical vapor deposition, and were characterized optically and morphologically. The Si quantum dot-sensitized solar cells had poor performance due to significant electron loss by charge recombination. Although the large Si particle size resulted in the exposure of a large TiO2 surface area, there was a limit to ho much the particle size could be decreased due to the reduced absorbance of small particles. Therefore, this work focused on decreasing the internal impedance to improve charge transfer. TiO2 was electronically modified by doping with vanadium, which can improve electron transfer in the TiO2 network, and which is stable in the redox electrolyte. Photogenerated electrons can more easily arrive at the conductive electrode due to the decreased internal impedance. The dark photovoltaic properties confirmed the reduction of charge recombination, and the photon-to-current conversion efficiency reflected the improved electron transfer. Impedance analysis confirmed a decrease in internal impedance and an increased electron lifetime. Consequently, these improvements by vanadium doping enhanced the overall performance of Si quantum dot-sensitized solar cells.

Highly Enhanced Photoelectrochemical Water Oxidation Efficiency Based on Triadic Quantum Dot/Layered Double Hydroxide/BiVO 4 Photoanodes

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

Tang, Yanqun; Wang, Ruirui; Yang, Ye

2016-08-03

The water oxidation half-reaction is considered to be a bottleneck for achieving highly efficient solar-driven water splitting due to its multiproton-coupled four-electron process and sluggish kinetics. Herein, a triadic photoanode consisting of dual-sized CdTe quantum dots (QDs), Co-based layered double hydroxide (LDH) nanosheets, and BiVO4 particles, that is, QD@LDH@BiVO4, was designed. Two sets of consecutive Type-II band alignments were constructed to improve photogenerated electron-hole separation in the triadic structure. The efficient charge separation resulted in a 2-fold enhancement of the photocurrent of the QD@LDH@BiVO4 photoanode. A significantly enhanced oxidation efficiency reaching above 90% in the low bias region (i.e., Emore » < 0.8 V vs RHE) could be critical in determining the overall performance of a complete photoelectrochemical cell. The faradaic efficiency for water oxidation was almost 90%. The conduction band energy of QDs is -1.0 V more negative than that of LDH, favorable for the electron injection to LDH and enabling a more efficient hole separation. The enhanced photon-to-current conversion efficiency and improved water oxidation efficiency of the triadic structure may result from the non-negligible contribution of hot electrons or holes generated in QDs. Such a band-matching and multidimensional triadic architecture could be a promising strategy for achieving high-efficiency photoanodes by sufficiently utilizing and maximizing the functionalities of QDs.« less

Photosensitization of ZnO nanowires with CdSe quantum dots for photovoltaic devices.

PubMed

Leschkies, Kurtis S; Divakar, Ramachandran; Basu, Joysurya; Enache-Pommer, Emil; Boercker, Janice E; Carter, C Barry; Kortshagen, Uwe R; Norris, David J; Aydil, Eray S

2007-06-01

We combine CdSe semiconductor nanocrystals (or quantum dots) and single-crystal ZnO nanowires to demonstrate a new type of quantum-dot-sensitized solar cell. An array of ZnO nanowires was grown vertically from a fluorine-doped tin oxide conducting substrate. CdSe quantum dots, capped with mercaptopropionic acid, were attached to the surface of the nanowires. When illuminated with visible light, the excited CdSe quantum dots injected electrons across the quantum dot-nanowire interface. The morphology of the nanowires then provided the photoinjected electrons with a direct electrical pathway to the photoanode. With a liquid electrolyte as the hole transport medium, quantum-dot-sensitized nanowire solar cells exhibited short-circuit currents ranging from 1 to 2 mA/cm2 and open-circuit voltages of 0.5-0.6 V when illuminated with 100 mW/cm2 simulated AM1.5 spectrum. Internal quantum efficiencies as high as 50-60% were also obtained.

Single-electron-occupation metal-oxide-semiconductor quantum dots formed from efficient poly-silicon gate layout

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

Carroll, Malcolm S.; rochette, sophie; Rudolph, Martin

We introduce a silicon metal-oxide-semiconductor quantum dot structure that achieves dot-reservoir tunnel coupling control without a dedicated barrier gate. The elementary structure consists of two accumulation gates separated spatially by a gap, one gate accumulating a reservoir and the other a quantum dot. Control of the tunnel rate between the dot and the reservoir across the gap is demonstrated in the single electron regime by varying the reservoir accumulation gate voltage while compensating with the dot accumulation gate voltage. The method is then applied to a quantum dot connected in series to source and drain reservoirs, enabling transport down tomore » the single electron regime. Finally, tuning of the valley splitting with the dot accumulation gate voltage is observed. This split accumulation gate structure creates silicon quantum dots of similar characteristics to other realizations but with less electrodes, in a single gate stack subtractive fabrication process that is fully compatible with silicon foundry manufacturing.« less

High power cascade diode lasers emitting near 2 μm

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

Hosoda, Takashi; Feng, Tao; Shterengas, Leon, E-mail: leon.shterengas@stonybrook.edu

2016-03-28

High-power two-stage cascade GaSb-based type-I quantum well diode lasers emitting near 2 μm were designed and fabricated. Coated devices with cavity length of 3 mm generated about 2 W of continuous wave power from 100-μm-wide aperture at the current of 6 A. The power conversion efficiency peaked at 20%. Carrier recycling between quantum well gain stages was realized using band-to-band tunneling in GaSb/AlSb/InAs heterostructure complemented with optimized electron and hole injector regions. Design optimization eliminated parasitic optical absorption and thermionic emission, and included modification of the InAs quantum wells of electron and composition and doping profile of hole injectors. Utilization of the cascade pumpingmore » scheme yielded 2 μm lasers with improved output power and efficiency compared to existing state-of-the-art diodes.« less

Influence of surface states of CuInS2 quantum dots in quantum dots sensitized photo-electrodes

NASA Astrophysics Data System (ADS)

Peng, Zhuoyin; Liu, Yueli; Wu, Lei; Zhao, Yinghan; Chen, Keqiang; Chen, Wen

2016-12-01

Surface states are significant factor for the enhancement of electrochemical performance in CuInS2 quantum dot sensitized photo-electrodes. DDT, OLA, MPA, and S2- ligand capped CuInS2 quantum dot sensitized photo-electrodes are prepared by thermolysis, solvethermal and ligand-exchange processes, respectively, and their optical properties and photoelectrochemical properties are investigated. The S2- ligand enhances the UV-vis absorption and electron-hole separation property as well as the excellent charge transfer performance of the photo-electrodes, which is attributed to the fact that the atomic S2- ligand for the interfacial region of quantum dots may improve the electron transfer rate. These S2--capped CuInS2 quantum dot sensitized photo-electrodes exhibit the excellent photoelectrochemical efficiency and IPCE peak value, which is higher than that of the samples with DDT, OLA and MPA ligands.

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.

Solar cells using quantum funnels.

PubMed

Kramer, Illan J; Levina, Larissa; Debnath, Ratan; Zhitomirsky, David; Sargent, Edward H

2011-09-14

Colloidal quantum dots offer broad tuning of semiconductor bandstructure via the quantum size effect. Devices involving a sequence of layers comprised of quantum dots selected to have different diameters, and therefore bandgaps, offer the possibility of funneling energy toward an acceptor. Here we report a quantum funnel that efficiently conveys photoelectrons from their point of generation toward an intended electron acceptor. Using this concept we build a solar cell that benefits from enhanced fill factor as a result of this quantum funnel. This concept addresses limitations on transport in soft condensed matter systems and leverages their advantages in large-area optoelectronic devices and systems.

Scanning EM of non-heavy metal stained biosamples: Large-field of view, high contrast and highly efficient immunolabeling

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

Kuipers, Jeroen; Boer, Pascal de; Giepmans, Ben N.G., E-mail: b.n.g.giepmans@umcg.nl

Scanning electron microscopy (SEM) is increasing its application in life sciences for electron density measurements of ultrathin sections. These are traditionally analyzed with transmission electron microscopy (TEM); by most labs, SEM analysis still is associated with surface imaging only. Here we report several advantages of SEM for thin sections over TEM, both for structural inspection, as well as analyzing immuno-targeted labels such as quantum dots (QDs) and gold, where we find that QD-labeling is ten times more efficient than gold-labeling. Furthermore, we find that omitting post-staining with uranyl and lead leads to QDs readily detectable over the ultrastructure, but undermore » these conditions ultrastructural contrast was even almost invisible in TEM examination. Importantly, imaging in SEM with STEM detection leads to both outstanding QDs and ultrastructural contrast. STEM imaging is superior over back-scattered electron imaging of these non-contrasted samples, whereas secondary electron detection cannot be used at all. We conclude that examination of ultrathin sections by SEM, which may be immunolabeled with QDs, will allow rapid and straightforward analysis of large fields with more efficient labeling than can be achieved with immunogold. The large fields of view routinely achieved with SEM, but not with TEM, allows straightforward raw data sharing using virtual microscopy, also known as nanotomy when this concerns EM data in the life sciences. - Highlights: • High resolution and large fields of view via nanotomy or virtual microscopy. • Highly relevant for EM‐datasets where information density is high. • Sample preparation with low contrast good for STEM, not TEM. • Quantum dots now stand out in STEM‐based detection. • 10 Times more efficient labeling with quantum dots compared to gold.« less

Sandwiched confinement of quantum dots in graphene matrix for efficient electron transfer and photocurrent production

PubMed Central

Zhu, Nan; Zheng, Kaibo; Karki, Khadga J.; Abdellah, Mohamed; Zhu, Qiushi; Carlson, Stefan; Haase, Dörthe; Žídek, Karel; Ulstrup, Jens; Canton, Sophie E.; Pullerits, Tõnu; Chi, Qijin

2015-01-01

Quantum dots (QDs) and graphene are both promising materials for the development of new-generation optoelectronic devices. Towards this end, synergic assembly of these two building blocks is a key step but remains a challenge. Here, we show a one-step strategy for organizing QDs in a graphene matrix via interfacial self-assembly, leading to the formation of sandwiched hybrid QD-graphene nanofilms. We have explored structural features, electron transfer kinetics and photocurrent generation capacity of such hybrid nanofilms using a wide variety of advanced techniques. Graphene nanosheets interlink QDs and significantly improve electronic coupling, resulting in fast electron transfer from photoexcited QDs to graphene with a rate constant of 1.3 × 109 s−1. Efficient electron transfer dramatically enhances photocurrent generation in a liquid-junction QD-sensitized solar cell where the hybrid nanofilm acts as a photoanode. We thereby demonstrate a cost-effective method to construct large-area QD-graphene hybrid nanofilms with straightforward scale-up potential for optoelectronic applications. PMID:25996307

Sandwiched confinement of quantum dots in graphene matrix for efficient electron transfer and photocurrent production

NASA Astrophysics Data System (ADS)

Zhu, Nan; Zheng, Kaibo; Karki, Khadga J.; Abdellah, Mohamed; Zhu, Qiushi; Carlson, Stefan; Haase, Dörthe; Žídek, Karel; Ulstrup, Jens; Canton, Sophie E.; Pullerits, Tõnu; Chi, Qijin

2015-05-01

Quantum dots (QDs) and graphene are both promising materials for the development of new-generation optoelectronic devices. Towards this end, synergic assembly of these two building blocks is a key step but remains a challenge. Here, we show a one-step strategy for organizing QDs in a graphene matrix via interfacial self-assembly, leading to the formation of sandwiched hybrid QD-graphene nanofilms. We have explored structural features, electron transfer kinetics and photocurrent generation capacity of such hybrid nanofilms using a wide variety of advanced techniques. Graphene nanosheets interlink QDs and significantly improve electronic coupling, resulting in fast electron transfer from photoexcited QDs to graphene with a rate constant of 1.3 × 109 s-1. Efficient electron transfer dramatically enhances photocurrent generation in a liquid-junction QD-sensitized solar cell where the hybrid nanofilm acts as a photoanode. We thereby demonstrate a cost-effective method to construct large-area QD-graphene hybrid nanofilms with straightforward scale-up potential for optoelectronic applications.

Improving the efficiency of water splitting in dye-sensitized solar cells by using a biomimetic electron transfer mediator

PubMed Central

Zhao, Yixin; Swierk, John R.; Megiatto, Jackson D.; Sherman, Benjamin; Youngblood, W. Justin; Qin, Dongdong; Lentz, Deanna M.; Moore, Ana L.; Moore, Thomas A.; Gust, Devens; Mallouk, Thomas E.

2012-01-01

Photoelectrochemical water splitting directly converts solar energy to chemical energy stored in hydrogen, a high energy density fuel. Although water splitting using semiconductor photoelectrodes has been studied for more than 40 years, it has only recently been demonstrated using dye-sensitized electrodes. The quantum yield for water splitting in these dye-based systems has, so far, been very low because the charge recombination reaction is faster than the catalytic four-electron oxidation of water to oxygen. We show here that the quantum yield is more than doubled by incorporating an electron transfer mediator that is mimetic of the tyrosine-histidine mediator in Photosystem II. The mediator molecule is covalently bound to the water oxidation catalyst, a colloidal iridium oxide particle, and is coadsorbed onto a porous titanium dioxide electrode with a Ruthenium polypyridyl sensitizer. As in the natural photosynthetic system, this molecule mediates electron transfer between a relatively slow metal oxide catalyst that oxidizes water on the millisecond timescale and a dye molecule that is oxidized in a fast light-induced electron transfer reaction. The presence of the mediator molecule in the system results in photoelectrochemical water splitting with an internal quantum efficiency of approximately 2.3% using blue light. PMID:22547794

Finding the quantum thermoelectric with maximal efficiency and minimal entropy production at given power output

NASA Astrophysics Data System (ADS)

Whitney, Robert S.

2015-03-01

We investigate the nonlinear scattering theory for quantum systems with strong Seebeck and Peltier effects, and consider their use as heat engines and refrigerators with finite power outputs. This paper gives detailed derivations of the results summarized in a previous paper [R. S. Whitney, Phys. Rev. Lett. 112, 130601 (2014), 10.1103/PhysRevLett.112.130601]. It shows how to use the scattering theory to find (i) the quantum thermoelectric with maximum possible power output, and (ii) the quantum thermoelectric with maximum efficiency at given power output. The latter corresponds to a minimal entropy production at that power output. These quantities are of quantum origin since they depend on system size over electronic wavelength, and so have no analog in classical thermodynamics. The maximal efficiency coincides with Carnot efficiency at zero power output, but decreases with increasing power output. This gives a fundamental lower bound on entropy production, which means that reversibility (in the thermodynamic sense) is impossible for finite power output. The suppression of efficiency by (nonlinear) phonon and photon effects is addressed in detail; when these effects are strong, maximum efficiency coincides with maximum power. Finally, we show in particular limits (typically without magnetic fields) that relaxation within the quantum system does not allow the system to exceed the bounds derived for relaxation-free systems, however, a general proof of this remains elusive.

An integrated approach to realizing high-performance liquid-junction quantum dot sensitized solar cells

PubMed Central

McDaniel, Hunter; Fuke, Nobuhiro; Makarov, Nikolay S.; Pietryga, Jeffrey M.; Klimov, Victor I.

2013-01-01

Solution-processed semiconductor quantum dot solar cells offer a path towards both reduced fabrication cost and higher efficiency enabled by novel processes such as hot-electron extraction and carrier multiplication. Here we use a new class of low-cost, low-toxicity CuInSexS2−x quantum dots to demonstrate sensitized solar cells with certified efficiencies exceeding 5%. Among other material and device design improvements studied, use of a methanol-based polysulfide electrolyte results in a particularly dramatic enhancement in photocurrent and reduced series resistance. Despite the high vapour pressure of methanol, the solar cells are stable for months under ambient conditions, which is much longer than any previously reported quantum dot sensitized solar cell. This study demonstrates the large potential of CuInSexS2−x quantum dots as active materials for the realization of low-cost, robust and efficient photovoltaics as well as a platform for investigating various advanced concepts derived from the unique physics of the nanoscale size regime. PMID:24322379

Boosting the efficiency of quantum dot sensitized solar cells through modulation of interfacial charge transfer.

PubMed

Kamat, Prashant V

2012-11-20

The demand for clean energy will require the design of nanostructure-based light-harvesting assemblies for the conversion of solar energy into chemical energy (solar fuels) and electrical energy (solar cells). Semiconductor nanocrystals serve as the building blocks for designing next generation solar cells, and metal chalcogenides (e.g., CdS, CdSe, PbS, and PbSe) are particularly useful for harnessing size-dependent optical and electronic properties in these nanostructures. This Account focuses on photoinduced electron transfer processes in quantum dot sensitized solar cells (QDSCs) and discusses strategies to overcome the limitations of various interfacial electron transfer processes. The heterojunction of two semiconductor nanocrystals with matched band energies (e.g., TiO(2) and CdSe) facilitates charge separation. The rate at which these separated charge carriers are driven toward opposing electrodes is a major factor that dictates the overall photocurrent generation efficiency. The hole transfer at the semiconductor remains a major bottleneck in QDSCs. For example, the rate constant for hole transfer is 2-3 orders of magnitude lower than the electron injection from excited CdSe into oxide (e.g., TiO(2)) semiconductor. Disparity between the electron and hole scavenging rate leads to further accumulation of holes within the CdSe QD and increases the rate of electron-hole recombination. To overcome the losses due to charge recombination processes at the interface, researchers need to accelerate electron and hole transport. The power conversion efficiency for liquid junction and solid state quantum dot solar cells, which is in the range of 5-6%, represents a significant advance toward effective utilization of nanomaterials for solar cells. The design of new semiconductor architectures could address many of the issues related to modulation of various charge transfer steps. With the resolution of those problems, the efficiencies of QDSCs could approach those of dye sensitized solar cells (DSSC) and organic photovoltaics.

Enhancing the quantum efficiency of InGaN yellow-green light-emitting diodes by growth interruption

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

Du, Chunhua; Ma, Ziguang; Zhou, Junming

2014-08-18

We studied the effect of multiple interruptions during the quantum well growth on emission-efficiency enhancement of InGaN-based yellow-green light emitting diodes on c-plane sapphire substrate. The output power and dominant wavelength at 20 mA are 0.24 mW and 556.3 nm. High resolution x-ray diffraction, photoluminescence, and electroluminescence measurements demonstrate that efficiency enhancement could be partially attributed to crystal quality improvement of the active region resulted from reduced In clusters and relevant defects on the surface of InGaN layer by introducing interruptions. The less tilted energy band in the quantum well is also caused by the decrease of In-content gradient along c-axis resultedmore » from In segregation during the interruptions, which increases spatial overlap of electron-hole wavefunction and thus the internal quantum efficiency. The latter also leads to smaller blueshift of dominant wavelength with current increasing.« less

Quantum tomography of near-unitary processes in high-dimensional quantum systems

NASA Astrophysics Data System (ADS)

Lysne, Nathan; Sosa Martinez, Hector; Jessen, Poul; Baldwin, Charles; Kalev, Amir; Deutsch, Ivan

2016-05-01

Quantum Tomography (QT) is often considered the ideal tool for experimental debugging of quantum devices, capable of delivering complete information about quantum states (QST) or processes (QPT). In practice, the protocols used for QT are resource intensive and scale poorly with system size. In this situation, a well behaved model system with access to large state spaces (qudits) can serve as a useful platform for examining the tradeoffs between resource cost and accuracy inherent in QT. In past years we have developed one such experimental testbed, consisting of the electron-nuclear spins in the electronic ground state of individual Cs atoms. Our available toolkit includes high fidelity state preparation, complete unitary control, arbitrary orthogonal measurements, and accurate and efficient QST in Hilbert space dimensions up to d = 16. Using these tools, we have recently completed a comprehensive study of QPT in 4, 7 and 16 dimensions. Our results show that QPT of near-unitary processes is quite feasible if one chooses optimal input states and efficient QST on the outputs. We further show that for unitary processes in high dimensional spaces, one can use informationally incomplete QPT to achieve high-fidelity process reconstruction (90% in d = 16) with greatly reduced resource requirements.

Adiabatic Quantum Simulation of Quantum Chemistry

PubMed Central

Babbush, Ryan; Love, Peter J.; Aspuru-Guzik, Alán

2014-01-01

We show how to apply the quantum adiabatic algorithm directly to the quantum computation of molecular properties. We describe a procedure to map electronic structure Hamiltonians to 2-body qubit Hamiltonians with a small set of physically realizable couplings. By combining the Bravyi-Kitaev construction to map fermions to qubits with perturbative gadgets to reduce the Hamiltonian to 2-body, we obtain precision requirements on the coupling strengths and a number of ancilla qubits that scale polynomially in the problem size. Hence our mapping is efficient. The required set of controllable interactions includes only two types of interaction beyond the Ising interactions required to apply the quantum adiabatic algorithm to combinatorial optimization problems. Our mapping may also be of interest to chemists directly as it defines a dictionary from electronic structure to spin Hamiltonians with physical interactions. PMID:25308187

High mobility back-gated InAs/GaSb double quantum well grown on GaSb substrate

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

Nguyen, Binh-Minh, E-mail: mbnguyen@hrl.com, E-mail: MSokolich@hrl.com; Yi, Wei; Noah, Ramsey

2015-01-19

We report a backgated InAs/GaSb double quantum well device grown on GaSb substrate. The use of the native substrate allows for high materials quality with electron mobility in excess of 500 000 cm{sup 2}/Vs at sheet charge density of 8 × 10{sup 11} cm{sup −2} and approaching 100 000 cm{sup 2}/Vs near the charge neutrality point. Lattice matching between the quantum well structure and the substrate eliminates the need for a thick buffer, enabling large back gate capacitance and efficient coupling with the conduction channels in the quantum wells. As a result, quantum Hall effects are observed in both electron and hole regimes across the hybridizationmore » gap.« less

Biosynthesis of luminescent CdS quantum dots using plant hairy root culture

NASA Astrophysics Data System (ADS)

Borovaya, Mariya N.; Naumenko, Antonina P.; Matvieieva, Nadia A.; Blume, Yaroslav B.; Yemets, Alla I.

2014-12-01

CdS nanoparticles have a great potential for application in chemical research, bioscience and medicine. The aim of this study was to develop an efficient and environmentally-friendly method of plant-based biosynthesis of CdS quantum dots using hairy root culture of Linaria maroccana L. By incubating Linaria root extract with inorganic cadmium sulfate and sodium sulfide we synthesized stable luminescent CdS nanocrystals with absorption peaks for UV-visible spectrometry at 362 nm, 398 nm and 464 nm, and luminescent peaks at 425, 462, 500 nm. Transmission electron microscopy of produced quantum dots revealed their spherical shape with a size predominantly from 5 to 7 nm. Electron diffraction pattern confirmed the wurtzite crystalline structure of synthesized cadmium sulfide quantum dots. These results describe the first successful attempt of quantum dots synthesis using plant extract.

Towards quantification of vibronic coupling in photosynthetic antenna complexes

NASA Astrophysics Data System (ADS)

Singh, V. P.; Westberg, M.; Wang, C.; Dahlberg, P. D.; Gellen, T.; Gardiner, A. T.; Cogdell, R. J.; Engel, G. S.

2015-06-01

Photosynthetic antenna complexes harvest sunlight and efficiently transport energy to the reaction center where charge separation powers biochemical energy storage. The discovery of existence of long lived quantum coherence during energy transfer has sparked the discussion on the role of quantum coherence on the energy transfer efficiency. Early works assigned observed coherences to electronic states, and theoretical studies showed that electronic coherences could affect energy transfer efficiency—by either enhancing or suppressing transfer. However, the nature of coherences has been fiercely debated as coherences only report the energy gap between the states that generate coherence signals. Recent works have suggested that either the coherences observed in photosynthetic antenna complexes arise from vibrational wave packets on the ground state or, alternatively, coherences arise from mixed electronic and vibrational states. Understanding origin of coherences is important for designing molecules for efficient light harvesting. Here, we give a direct experimental observation from a mutant of LH2, which does not have B800 chromophores, to distinguish between electronic, vibrational, and vibronic coherence. We also present a minimal theoretical model to characterize the coherences both in the two limiting cases of purely vibrational and purely electronic coherence as well as in the intermediate, vibronic regime.

New Diamond Color Center for Quantum Communication

NASA Astrophysics Data System (ADS)

Huang, Ding; Rose, Brendon; Tyryshkin, Alexei; Sangtawesin, Sorawis; Srinivasan, Srikanth; Twitchen, Daniel; Markham, Matthew; Edmonds, Andrew; Gali, Adam; Stacey, Alastair; Wang, Wuyi; D'Haenens-Johansson, Ulrika; Zaitsev, Alexandre; Lyon, Stephen; de Leon, Nathalie

2017-04-01

Color centers in diamond are attractive for quantum communication applications because of their long electron spin coherence times and efficient optical transitions. Previous demonstrations of color centers as solid-state spin qubits were primarily focused on centers that exhibit either long coherence times or highly efficient optical interfaces. Recently, we developed a method to stabilize the neutral charge state of silicon-vacancy center in diamond (SiV0) with high conversion efficiency. We observe spin relaxation times exceeding 1 minute and spin coherence times of 1 ms for SiV0 centers. Additionally, the SiV0 center also has > 90 % of its emission into its zero-phonon line and a narrow inhomogeneous optical linewidth. The combination of a long spin coherence time and efficient optical interface make the SiV0 center a promising candidate for applications in long distance quantum communication.

Highly Efficient and Fully Solution-Processed Inverted Light-Emitting Diodes with Charge Control Interlayers.

PubMed

Fu, Yan; Jiang, Wei; Kim, Daekyoung; Lee, Woosuk; Chae, Heeyeop

2018-05-23

In this work, we developed a charge control sandwich structure around QD layers for the inverted QLEDs, the performance of which is shown to exceed that of the conventional QLEDs in terms of the external quantum efficiency (EQE) and the current efficiency (CE). The QD light-emitting layer (EML) is sandwiched with two ultrathin interfacial layers: one is a poly(9-vinlycarbazole) (PVK) layer to prevent excess electrons, and the other is a polyethylenimine ethoxylated (PEIE) layer to reduce the hole injection barrier. The sandwich structure resolves the imbalance between injected holes and electrons and brings the level of balanced charge carriers to a maximum. We demonstrated the highly improved performance of 89.8 cd/A of current efficiency, 22.4% of external quantum efficiency, and 72 814 cd m -2 of maximum brightness with the solution-processed inverted QLED. This sandwich structure (PVK/QD/PEIE), as a framework, can be applied to various QLED devices for enhancing performance.

Efficient two-step photocarrier generation in bias-controlled InAs/GaAs quantum dot superlattice intermediate-band solar cells.

PubMed

Kada, T; Asahi, S; Kaizu, T; Harada, Y; Tamaki, R; Okada, Y; Kita, T

2017-07-19

We studied the effects of the internal electric field on two-step photocarrier generation in InAs/GaAs quantum dot superlattice (QDSL) intermediate-band solar cells (IBSCs). The external quantum efficiency of QDSL-IBSCs was measured as a function of the internal electric field intensity, and compared with theoretical calculations accounting for interband and intersubband photoexcitations. The extra photocurrent caused by the two-step photoexcitation was maximal for a reversely biased electric field, while the current generated by the interband photoexcitation increased monotonically with increasing electric field intensity. The internal electric field in solar cells separated photogenerated electrons and holes in the superlattice (SL) miniband that played the role of an intermediate band, and the electron lifetime was extended to the microsecond scale, which improved the intersubband transition strength, therefore increasing the two-step photocurrent. There was a trade-off relation between the carrier separation enhancing the two-step photoexcitation and the electric-field-induced carrier escape from QDSLs. These results validate that long-lifetime electrons are key to maximising the two-step photocarrier generation in QDSL-IBSCs.

Dissipative time-dependent quantum transport theory.

PubMed

Zhang, Yu; Yam, Chi Yung; Chen, GuanHua

2013-04-28

A dissipative time-dependent quantum transport theory is developed to treat the transient current through molecular or nanoscopic devices in presence of electron-phonon interaction. The dissipation via phonon is taken into account by introducing a self-energy for the electron-phonon coupling in addition to the self-energy caused by the electrodes. Based on this, a numerical method is proposed. For practical implementation, the lowest order expansion is employed for the weak electron-phonon coupling case and the wide-band limit approximation is adopted for device and electrodes coupling. The corresponding hierarchical equation of motion is derived, which leads to an efficient and accurate time-dependent treatment of inelastic effect on transport for the weak electron-phonon interaction. The resulting method is applied to a one-level model system and a gold wire described by tight-binding model to demonstrate its validity and the importance of electron-phonon interaction for the quantum transport. As it is based on the effective single-electron model, the method can be readily extended to time-dependent density functional theory.

Large enhancement in photocurrent by Mn doping in CdSe/ZTO quantum dot sensitized solar cells.

PubMed

Pimachev, Artem; Poudyal, Uma; Proshchenko, Vitaly; Wang, Wenyong; Dahnovsky, Yuri

2016-09-29

We find a large enhancement in the efficiency of CdSe quantum dot sensitized solar cells by doping with manganese. In the presence of Mn impurities in relatively small concentrations (2.3%) the photoelectric current increases by up to 190%. The average photocurrent enhancement is about 160%. This effect cannot be explained by a light absorption mechanism because the experimental and theoretical absorption spectra demonstrate that there is no change in the absorption coefficient in the presence of the Mn impurities. To explain such a large increase in the injection current we propose a tunneling mechanism of electron injection from the quantum dot LUMO state to the Zn 2 SnO 4 (ZTO) semiconductor photoanode. The calculated enhancement is approximately equal to 150% which is very close to the experimental average value of 160%. The relative discrepancy between the calculated and experimentally measured ratios of the IPCE currents is only 6.25%. For other mechanisms (such as electron trapping, etc.) the remaining 6.25% cannot explain the large change in the experimental IPCE. Thus we have indirectly proved that electron tunneling is the major mechanism of photocurrent enhancement. This work proposes a new approach for a significant improvement in the efficiency of quantum dot sensitized solar cells.

NbN single-photon detectors with saturated dependence of quantum efficiency

NASA Astrophysics Data System (ADS)

Smirnov, Konstantin; Divochiy, Alexander; Vakhtomin, Yury; Morozov, Pavel; Zolotov, Philipp; Antipov, Andrey; Seleznev, Vitaliy

2018-07-01

The possibility of creating NbN superconducting single-photon detectors with saturated dependence of quantum efficiency (QE) versus normalized bias current was investigated. It was shown that the saturation increases for the detectors based on finer films with a lower value of R s300/R s20. The decreasing of R s300/R s20 was related to the increasing influence of quantum corrections to conductivity of superconductors and, in turn, to the decrease of the electron diffusion coefficient. The best samples have a constant value of system QE 94% at I b /I c ∼ 0.8 and wavelength 1310 nm.

Miniband-related 1.4–1.8 μm luminescence of Ge/Si quantum dot superlattices

PubMed Central

Cirlin, GE; Tonkikh, AA; Zakharov, ND; Werner, P; Gösele, U; Tomm, JW; Elsaesser, T

2006-01-01

The luminescence properties of highly strained, Sb-doped Ge/Si multi-layer heterostructures with incorporated Ge quantum dots (QDs) are studied. Calculations of the electronic band structure and luminescence measurements prove the existence of an electron miniband within the columns of the QDs. Miniband formation results in a conversion of the indirect to a quasi-direct excitons takes place. The optical transitions between electron states within the miniband and hole states within QDs are responsible for an intense luminescence in the 1.4–1.8 µm range, which is maintained up to room temperature. At 300 K, a light emitting diode based on such Ge/Si QD superlattices demonstrates an external quantum efficiency of 0.04% at a wavelength of 1.55 µm.

Many-Body Theory of Proton-Generated Point Defects for Losses of Electron Energy and Photons in Quantum Wells

NASA Astrophysics Data System (ADS)

Huang, Danhong; Iurov, Andrii; Gao, Fei; Gumbs, Godfrey; Cardimona, D. A.

2018-02-01

The effects of point defects on the loss of either energies of ballistic electron beams or incident photons are studied by using a many-body theory in a multi-quantum-well system. This theory includes the defect-induced vertex correction to a bare polarization function of electrons within the ladder approximation, and the intralayer and interlayer screening of defect-electron interactions is also taken into account in the random-phase approximation. The numerical results of defect effects on both energy-loss and optical-absorption spectra are presented and analyzed for various defect densities, numbers of quantum wells, and wave vectors. The diffusion-reaction equation is employed for calculating distributions of point defects in a layered structure. For completeness, the production rate for Frenkel-pair defects and their initial concentration are obtained based on atomic-level molecular-dynamics simulations. By combining the defect-effect, diffusion-reaction, and molecular-dynamics models with an available space-weather-forecast model, it will be possible in the future to enable specific designing for electronic and optoelectronic quantum devices that will be operated in space with radiation-hardening protection and, therefore, effectively extend the lifetime of these satellite onboard electronic and optoelectronic devices. Specifically, this theory can lead to a better characterization of quantum-well photodetectors not only for high quantum efficiency and low dark current density but also for radiation tolerance or mitigating the effects of the radiation.

Electron gun with a transmission photocathode for the Joint Institute for Nuclear Research photoinjector

NASA Astrophysics Data System (ADS)

Balalykin, N. I.; Minashkin, V. F.; Nozdrin, M. A.; Shirkov, G. D.; Zelenogorskii, V. V.; Gacheva, E. I.; Potemkin, A. K.; Huran, J.

2017-10-01

Photocathode electron guns are key to the generation of high-quality electron bunches, which are currently the primary source of electrons for linear electron accelerators. The photogun test bench built at the Joint Institute for Nuclear Research (JINR) is currently being used to further develop the hollow (backside irradiated) photocathode concept. A major achievement was the replacement of the hollow photocathode by a technologically more feasible transmission photocathode made from a metal mesh that serves as a substrate for films of various photomaterials. A number of thin-film cathodes on quartz glass substrates are fabricated by photolithography. The vectorial photoeffect (related to the surface-normal component of the wave electric field) is observed and found to significantly affect the quantum efficiency. The dependence of the quantum efficiency of diamond-like carbon photocathodes on the manufacturing technology is investigated. The Rutherford backscattering and elastic recoil detection techniques are combined to carry out an elemental analysis of the films. An estimate of the emittance of a 400 pC electron beam is obtained using the cross-section method.

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 distributions. The effect of the exciton dynamics on photoreduction reactions is illustrated using methyl viologen (MV(2+)) as a model electron acceptor. The steady-state MV(2+) photoreduction quantum yield of CdSe/CdS dot-in-rod NRs approaches unity under rod excitation, much larger than CdSe QDs and CdSe/CdS core/shell QDs. Detailed time-resolved studies show that in quasi-type II CdSe/CdS NRs and type II ZnSe/CdS NRs strong quantum confinement in the radial direction facilitates fast electron transfer and hole removal, whereas the fast carrier mobility along the axial direction enables long distance charge separation and slow charge recombination, which is essential for efficient MV(2+) photoreduction. The NR/MV(2+) relay system can be coupled to Pt nanoparticles in solution for light-driven H2 generation. Alternatively, Pt-tipped CdS and CdSe/CdS NRs provide fully integrated all inorganic systems for light-driven H2 generation. In CdS-Pt and CdSe/CdS-Pt hetero-NRs, ultrafast hole trapping on the CdS rod surface or in CdSe core enables efficient electron transfer from NRs to Pt tips by suppressing hole and energy transfer. It is shown that the quantum yields of photodriven H2 generation using these heterostructures correlate well with measured hole transfer rates from NRs to sacrificial donors, revealing that hole removal is the key efficiency-limiting step. These findings provide important insights for designing more efficient quantum confined NR and NR-Pt based systems for solar-to-fuel conversion.

Efficient Multi-Dimensional Simulation of Quantum Confinement Effects in Advanced MOS Devices

NASA Technical Reports Server (NTRS)

Biegel, Bryan A.; Rafferty, Conor S.; Ancona, Mario G.; Yu, Zhi-Ping

2000-01-01

We investigate the density-gradient (DG) transport model for efficient multi-dimensional simulation of quantum confinement effects in advanced MOS devices. The formulation of the DG model is described as a quantum correction to the classical drift-diffusion model. Quantum confinement effects are shown to be significant in sub-100nm MOSFETs. In thin-oxide MOS capacitors, quantum effects may reduce gate capacitance by 25% or more. As a result, the inclusion or quantum effects in simulations dramatically improves the match between C-V simulations and measurements for oxide thickness down to 2 nm. Significant quantum corrections also occur in the I-V characteristics of short-channel (30 to 100 nm) n-MOSFETs, with current drive reduced by up to 70%. This effect is shown to result from reduced inversion charge due to quantum confinement of electrons in the channel. Also, subthreshold slope is degraded by 15 to 20 mV/decade with the inclusion of quantum effects via the density-gradient model, and short channel effects (in particular, drain-induced barrier lowering) are noticeably increased.

Experiments on Quantum Hall Topological Phases in Ultra Low Temperatures

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

Du, Rui-Rui

2015-02-14

This project is to cool electrons in semiconductors to extremely low temperatures and to study new states of matter formed by low-dimensional electrons (or holes). At such low temperatures (and with an intense magnetic field), electronic behavior differs completely from ordinary ones observed at room temperatures or regular low temperature. Studies of electrons at such low temperatures would open the door for fundamental discoveries in condensed matter physics. Present studies have been focused on topological phases in the fractional quantum Hall effect in GaAs/AlGaAs semiconductor heterostructures, and the newly discovered (by this group) quantum spin Hall effect in InAs/GaSb materials.more » This project consists of the following components: 1) Development of efficient sample cooling techniques and electron thermometry: Our goal is to reach 1 mK electron temperature and reasonable determination of electron temperature; 2) Experiments at ultra-low temperatures: Our goal is to understand the energy scale of competing quantum phases, by measuring the temperature-dependence of transport features. Focus will be placed on such issues as the energy gap of the 5/2 state, and those of 12/5 (and possible 13/5); resistive signature of instability near 1/2 at ultra-low temperatures; 3) Measurement of the 5/2 gaps in the limit of small or large Zeeman energies: Our goal is to gain physics insight of 5/2 state at limiting experimental parameters, especially those properties concerning the spin polarization; 4) Experiments on tuning the electron-electron interaction in a screened quantum Hall system: Our goal is to gain understanding of the formation of paired fractional quantum Hall state as the interaction pseudo-potential is being modified by a nearby screening electron layer; 5) Experiments on the quantized helical edge states under a strong magnetic field and ultralow temperatures: our goal is to investigate both the bulk and edge states in a quantum spin Hall insulator under time-reversal symmetry-broken conditions.« less

Security of a discretely signaled continuous variable quantum key distribution protocol for high rate systems.

PubMed

Zhang, Zheshen; Voss, Paul L

2009-07-06

We propose a continuous variable based quantum key distribution protocol that makes use of discretely signaled coherent light and reverse error reconciliation. We present a rigorous security proof against collective attacks with realistic lossy, noisy quantum channels, imperfect detector efficiency, and detector electronic noise. This protocol is promising for convenient, high-speed operation at link distances up to 50 km with the use of post-selection.

Finite element method for calculating spectral and optical characteristics of axially symmetric quantum dots

NASA Astrophysics Data System (ADS)

Gusev, A. A.; Chuluunbaatar, O.; Vinitsky, S. I.; Derbov, V. L.; Hai, L. L.; Kazaryan, E. M.; Sarkisyan, H. A.

2018-04-01

We present new calculation schemes using high-order finite element method implemented on unstructured grids with triangle elements for solving boundary-value problems that describe axially symmetric quantum dots. The efficiency of the algorithms and software is demonstrated by benchmark calculations of the energy spectrum, the envelope eigenfunctions of electron, hole and exciton states, and the direct interband light absorption in conical and spheroidal impenetrable quantum dots.

Exciplex-triplet energy transfer: A new method to achieve extremely efficient organic light-emitting diode with external quantum efficiency over 30% and drive voltage below 3 V

NASA Astrophysics Data System (ADS)

Seo, Satoshi; Shitagaki, Satoko; Ohsawa, Nobuharu; Inoue, Hideko; Suzuki, Kunihiko; Nowatari, Hiromi; Yamazaki, Shunpei

2014-04-01

A novel approach to enhance the power efficiency of an organic light-emitting diode (OLED) by employing energy transfer from an exciplex to a phosphorescent emitter is reported. It was found that excitation energy of an exciplex formed between an electron-transporting material with a π-deficient quinoxaline moiety and a hole-transporting material with aromatic amine structure can be effectively transferred to a phosphorescent iridium complex in an emission layer of a phosphorescent OLED. Moreover, such an exciplex formation increases quantum efficiency and reduces drive voltage. A highly efficient, low-voltage, and long-life OLED based on this energy transfer is also demonstrated. This OLED device exhibited extremely high external quantum efficiency of 31% even without any attempt to enhance light outcoupling and also achieved a low drive voltage of 2.8 V and a long lifetime of approximately 1,000,000 h at a luminance of 1,000 cd/m2.

Efficient broad color luminescence from InGaN/GaN single quantum-well nanocolumn crystals on Si (111) substrate

NASA Astrophysics Data System (ADS)

Zhang, Wei; Zhang, Xuehua; Wang, Yongjin; Hu, Fangren

2017-10-01

Nanocolumn InGaN/GaN single quantum well crystals were deposited on Si (111) substrate with nitrified Ga dots as buffer layer. Transmission electron microscopy image shows the crystals' diameter of 100-130 nm and length of about 900 nm. Nanoscale spatial phase separation of cubic and hexagonal GaN was observed by selective area electron diffraction on the quantum well layer. Raman spectrum of the quantum well crystals proved that the crystals were fully relaxed. Room temperature photoluminescence from 450 to 750 nm and full width at half maximum of about 420 meV indicate broad color luminescence covering blue, green, yellow and red emission, which is helpful for the fabrication of tunable optoelectronic devices and colorful light emitting diodes.

Magneto-optical studies of quantum dots

NASA Astrophysics Data System (ADS)

Russ, Andreas Hans

Significant effort in condensed matter physics has recently been devoted to the field of "spintronics" which seeks to utilize the spin degree of freedom of electrons. Unlike conventional electronics that rely on the electron charge, devices exploiting their spin have the potential to yield new and novel technological applications, including spin transistors, spin filters, and spin-based memory devices. Any such application has the following essential requirements: 1) Efficient electrical injection of spin-polarized carriers; 2) Long spin lifetimes; 3) Ability to control and manipulate electron spins; 4) Effective detection of spin-polarized carriers. Recent work has demonstrated efficient electrical injection from ferromagnetic contacts such as Fe and MnAs, utilizing a spin-Light Emitting Diode (spin-LED) as a method of detection. Semiconductor quantum dots (QDs) are attractive candidates for satisfying requirements 2 and 3 as their zero dimensionality significantly suppresses many spin-flip mechanisms leading to long spin coherence times, as well as enabling the localization and manipulation of a controlled number of electrons and holes. This thesis is composed of three projects that are all based on the optical properties of QD structures including: I) Intershell exchange between spin-polarized electrons occupying adjacent shells in InAs QDs; II) Spin-polarized multiexitons in InAs QDs in the presence of spin-orbit interactions; III) The optical Aharonov-Bohm effect in AlxGa1-xAs/AlyGa1-yAs quantum wells (QWs). In the following we introduce some of the basic optical properties of quantum dots, describe the main tool (spin-LED) employed in this thesis to inject and detect spins in these QDs, and conclude with the optical Aharonov-Bohm effect (OAB) in type-II QDs.

Detection of single electron spin resonance in a double quantum dota)

NASA Astrophysics Data System (ADS)

Koppens, F. H. L.; Buizert, C.; Vink, I. T.; Nowack, K. C.; Meunier, T.; Kouwenhoven, L. P.; Vandersypen, L. M. K.

2007-04-01

Spin-dependent transport measurements through a double quantum dot are a valuable tool for detecting both the coherent evolution of the spin state of a single electron, as well as the hybridization of two-electron spin states. In this article, we discuss a model that describes the transport cycle in this regime, including the effects of an oscillating magnetic field (causing electron spin resonance) and the effective nuclear fields on the spin states in the two dots. We numerically calculate the current flow due to the induced spin flips via electron spin resonance, and we study the detector efficiency for a range of parameters. The experimental data are compared with the model and we find a reasonable agreement.

One-step model of photoemission from single-crystal surfaces

DOE PAGES

Karkare, Siddharth; Wan, Weishi; Feng, Jun; ...

2017-02-28

In our paper, we present a three-dimensional one-step photoemission model that can be used to calculate the quantum efficiency and momentum distributions of electrons photoemitted from ordered single-crystal surfaces close to the photoemission threshold. Using Ag(111) as an example, we also show that the model can not only calculate the quantum efficiency from the surface state accurately without using any ad hoc parameters, but also provides a theoretical quantitative explanation of the vectorial photoelectric effect. This model in conjunction with other band structure and wave function calculation techniques can be effectively used to screen single-crystal photoemitters for use as electronmore » sources for particle accelerator and ultrafast electron diffraction applications.« less

Enhanced photovoltaic performance of a quantum dot-sensitized solar cell using a Nb-doped TiO2 electrode.

PubMed

Jiang, Lei; You, Ting; Deng, Wei-Qiao

2013-10-18

In this work Nb-doped anatase TiO2 nanocrystals are used as the photoanode of quantum-dot-sensitized solar cells. A solar cell with CdS/CdSe quantum dots co-sensitized 2.5 mol% Nb-doped anatase TiO2 nanocrystals can achieve a photovoltaic conversion efficiency of 3.3%, which is almost twice as high as the 1.7% obtained by a cell based on undoped TiO2 nanocrystals. The incident photon-to-current conversion efficiency can reach as high as 91%, which is a record for all quantum-dot-sensitized solar cells. Detailed analysis shows that such an enhancement is due to improved lifetime and diffusion length of electrons in the solar cell.

Suppression of electron overflow in 370-nm InGaN/AlGaN ultraviolet light emitting diodes with different insertion layer thicknesses

NASA Astrophysics Data System (ADS)

Wang, C. K.; Wang, Y. W.; Chiou, Y. Z.; Chang, S. H.; Jheng, J. S.; Chang, S. P.; Chang, S. J.

2017-06-01

In this study, the properties of 370-nm InGaN/AlGaN ultraviolet light emitting diodes (UV LEDs) with different thicknesses of un-doped Al0.3Ga0.7N insertion layer (IL) between the last quantum barrier and electron blocking layer (EBL) have been numerically simulated by Advance Physical Model of Semiconductor Devices (APSYS). The results show that the LEDs using the high Al composition IL can effectively improve the efficiency droop, light output power, and internal quantum efficiency (IQE) compared to the original structure. The improvements of the optical properties are mainly attributed to the energy band discontinuity and offset created by IL, which increase the potential barrier height of conduction band to suppress the electron overflow from the active region to the p-side layer.

Deterministic Placement of Quantum-Size Controlled Quantum Dots for Seamless Top-Down Integration

DOE PAGES

Fischer, Arthur J.; Anderson, P. Duke; Koleske, Daniel D.; ...

2017-08-18

We demonstrate a new route toward the integration and deterministic placement of quantum dots (QDs) within prepatterned nanostructures. Using standard electron-beam lithography (EBL) and inductively coupled plasma reactive-ion etching (ICP-RIE), we fabricate arrays of nanowires on a III-nitride platform. Next, we integrate QDs of controlled size within the prepatterned nanowires using a bandgap-selective, wet-etching technique: quantum-size-controlled photoelectrochemical (QSC-PEC) etching. Low-temperature microphotoluminescence (μ-PL) measurements of individual nanowires reveal sharp spectral signatures, indicative of QD formation. Further, internal quantum efficiency (IQE) measurements reveal a near order of magnitude improvement in emitter efficiency following QSC-PEC etching. Finally, second-order cross-correlation (g(2)(0)) measurements of individualmore » QDs directly confirm nonclassical, antibunching behavior. Lastly, our results illustrate an exciting approach toward the top-down integration of nonclassical light sources within nanophotonic platforms.« less

Deterministic Placement of Quantum-Size Controlled Quantum Dots for Seamless Top-Down Integration

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

Fischer, Arthur J.; Anderson, P. Duke; Koleske, Daniel D.

We demonstrate a new route toward the integration and deterministic placement of quantum dots (QDs) within prepatterned nanostructures. Using standard electron-beam lithography (EBL) and inductively coupled plasma reactive-ion etching (ICP-RIE), we fabricate arrays of nanowires on a III-nitride platform. Next, we integrate QDs of controlled size within the prepatterned nanowires using a bandgap-selective, wet-etching technique: quantum-size-controlled photoelectrochemical (QSC-PEC) etching. Low-temperature microphotoluminescence (μ-PL) measurements of individual nanowires reveal sharp spectral signatures, indicative of QD formation. Further, internal quantum efficiency (IQE) measurements reveal a near order of magnitude improvement in emitter efficiency following QSC-PEC etching. Finally, second-order cross-correlation (g(2)(0)) measurements of individualmore » QDs directly confirm nonclassical, antibunching behavior. Lastly, our results illustrate an exciting approach toward the top-down integration of nonclassical light sources within nanophotonic platforms.« less

Improved photovoltaic performance and stability of quantum dot sensitized solar cells using Mn-ZnSe shell structure with enhanced light absorption and recombination control.

PubMed

Gopi, Chandu V V M; Venkata-Haritha, M; Kim, Soo-Kyoung; Kim, Hee-Je

2015-08-07

To make quantum-dot-sensitized solar cells (QDSSCs) competitive, photovoltaic parameters comparable to those of other emerging solar cell technologies are necessary. In the present study, ZnSe was used as an alternative to ZnS, one of the most widely used passivation materials in QDSSCs. ZnSe was deposited on a TiO2-CdS-CdSe photoanode to form a core-shell structure, which was more efficient in terms of reducing the electron recombination in QDSSCs. The development of an efficient passivation layer is a requirement for preventing recombination processes in order to attain high-performance and stable QDSSCs. A layer of inorganic Mn-ZnSe was applied to a QD-sensitized photoanode to enhance the adsorption and strongly inhibit interfacial recombination processes in QDSSCs, which greatly improved the power conversion efficiency. Impedance spectroscopy revealed that the combined Mn doping with ZnSe treatment reduces interfacial recombination and increases charge collection efficiency compared with Mn-ZnS, ZnS, and ZnSe. A solar cell based on the CdS-CdSe-Mn-ZnSe photoanode yielded excellent performance with a solar power conversion efficiency of 5.67%, Voc of 0.584 V, and Jsc of 17.59 mA cm(-2). Enhanced electron transport and reduced electron recombination are responsible for the improved Jsc and Voc of the QDSSCs. The effective electron lifetime of the device with Mn-ZnSe was higher than those with Mn-ZnS, ZnSe, and ZnS, leading to more efficient electron-hole separation and slower electron recombination.

Modeling quantum yield, emittance, and surface roughness effects from metallic photocathodes

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

Dimitrov, D. A.; Bell, G. I.; Smedley, J.

Here, detailed measurements of momentum distributions of emitted electrons have allowed the investigation of the thermal limit of the transverse emittance from metal photocathodes. Furthermore, recent developments in material design and growth have resulted in photocathodes that can deliver high quantum efficiency and are sufficiently robust to use in high electric field gradient photoinjectors and free electron lasers. The growth process usually produces photoemissive material layers with rough surface profiles that lead to transverse accelerating fields and possible work function variations, resulting in emittance growth. To better understand the effects of temperature, density of states, and surface roughness on themore » properties of emitted electrons, we have developed realistic three-dimensional models for photocathode materials with grated surface structures. They include general modeling of electron excitation due to photon absorption, charge transport, and emission from flat and rough metallic surfaces. The models also include image charge and field enhancement effects. We report results from simulations with flat and rough surfaces to investigate how electron scattering, controlled roughness, work function variation, and field enhancement affect emission properties. Comparison of simulation results with measurements of the quantum yield and transverse emittance from flat Sb emission surfaces shows the importance of including efficient modeling of photon absorption, temperature effects, and the material density of states to achieve agreement with the experimental data.« less

Ab Initio Optimized Effective Potentials for Real Molecules in Optical Cavities: Photon Contributions to the Molecular Ground State

PubMed Central

2018-01-01

We introduce a simple scheme to efficiently compute photon exchange-correlation contributions due to the coupling to transversal photons as formulated in the newly developed quantum-electrodynamical density-functional theory (QEDFT).1−5 Our construction employs the optimized-effective potential (OEP) approach by means of the Sternheimer equation to avoid the explicit calculation of unoccupied states. We demonstrate the efficiency of the scheme by applying it to an exactly solvable GaAs quantum ring model system, a single azulene molecule, and chains of sodium dimers, all located in optical cavities and described in full real space. While the first example is a two-dimensional system and allows to benchmark the employed approximations, the latter two examples demonstrate that the correlated electron-photon interaction appreciably distorts the ground-state electronic structure of a real molecule. By using this scheme, we not only construct typical electronic observables, such as the electronic ground-state density, but also illustrate how photon observables, such as the photon number, and mixed electron-photon observables, for example, electron–photon correlation functions, become accessible in a density-functional theory (DFT) framework. This work constitutes the first three-dimensional ab initio calculation within the new QEDFT formalism and thus opens up a new computational route for the ab initio study of correlated electron–photon systems in quantum cavities. PMID:29594185

Modeling quantum yield, emittance, and surface roughness effects from metallic photocathodes

DOE PAGES

Dimitrov, D. A.; Bell, G. I.; Smedley, J.; ...

2017-10-26

Here, detailed measurements of momentum distributions of emitted electrons have allowed the investigation of the thermal limit of the transverse emittance from metal photocathodes. Furthermore, recent developments in material design and growth have resulted in photocathodes that can deliver high quantum efficiency and are sufficiently robust to use in high electric field gradient photoinjectors and free electron lasers. The growth process usually produces photoemissive material layers with rough surface profiles that lead to transverse accelerating fields and possible work function variations, resulting in emittance growth. To better understand the effects of temperature, density of states, and surface roughness on themore » properties of emitted electrons, we have developed realistic three-dimensional models for photocathode materials with grated surface structures. They include general modeling of electron excitation due to photon absorption, charge transport, and emission from flat and rough metallic surfaces. The models also include image charge and field enhancement effects. We report results from simulations with flat and rough surfaces to investigate how electron scattering, controlled roughness, work function variation, and field enhancement affect emission properties. Comparison of simulation results with measurements of the quantum yield and transverse emittance from flat Sb emission surfaces shows the importance of including efficient modeling of photon absorption, temperature effects, and the material density of states to achieve agreement with the experimental data.« less

Quantum control of topological defects in magnetic systems

NASA Astrophysics Data System (ADS)

Takei, So; Mohseni, Masoud

2018-02-01

Energy-efficient classical information processing and storage based on topological defects in magnetic systems have been studied over the past decade. In this work, we introduce a class of macroscopic quantum devices in which a quantum state is stored in a topological defect of a magnetic insulator. We propose noninvasive methods to coherently control and read out the quantum state using ac magnetic fields and magnetic force microscopy, respectively. This macroscopic quantum spintronic device realizes the magnetic analog of the three-level rf-SQUID qubit and is built fully out of electrical insulators with no mobile electrons, thus eliminating decoherence due to the coupling of the quantum variable to an electronic continuum and energy dissipation due to Joule heating. For a domain wall size of 10-100 nm and reasonable material parameters, we estimate qubit operating temperatures in the range of 0.1-1 K, a decoherence time of about 0.01-1 μ s , and the number of Rabi flops within the coherence time scale in the range of 102-104 .

Quantum-dot-in-perovskite solids.

PubMed

Ning, Zhijun; Gong, Xiwen; Comin, Riccardo; Walters, Grant; Fan, Fengjia; Voznyy, Oleksandr; Yassitepe, Emre; Buin, Andrei; Hoogland, Sjoerd; Sargent, Edward H

2015-07-16

Heteroepitaxy-atomically aligned growth of a crystalline film atop a different crystalline substrate-is the basis of electrically driven lasers, multijunction solar cells, and blue-light-emitting diodes. Crystalline coherence is preserved even when atomic identity is modulated, a fact that is the critical enabler of quantum wells, wires, and dots. The interfacial quality achieved as a result of heteroepitaxial growth allows new combinations of materials with complementary properties, which enables the design and realization of functionalities that are not available in the single-phase constituents. Here we show that organohalide perovskites and preformed colloidal quantum dots, combined in the solution phase, produce epitaxially aligned 'dots-in-a-matrix' crystals. Using transmission electron microscopy and electron diffraction, we reveal heterocrystals as large as about 60 nanometres and containing at least 20 mutually aligned dots that inherit the crystalline orientation of the perovskite matrix. The heterocrystals exhibit remarkable optoelectronic properties that are traceable to their atom-scale crystalline coherence: photoelectrons and holes generated in the larger-bandgap perovskites are transferred with 80% efficiency to become excitons in the quantum dot nanocrystals, which exploit the excellent photocarrier diffusion of perovskites to produce bright-light emission from infrared-bandgap quantum-tuned materials. By combining the electrical transport properties of the perovskite matrix with the high radiative efficiency of the quantum dots, we engineer a new platform to advance solution-processed infrared optoelectronics.

Two-step entanglement concentration for arbitrary electronic cluster state

NASA Astrophysics Data System (ADS)

Zhao, Sheng-Yang; Liu, Jiong; Zhou, Lan; Sheng, Yu-Bo

2013-12-01

We present an efficient protocol for concentrating an arbitrary four-electron less-entangled cluster state into a maximally entangled cluster state. As a two-step entanglement concentration protocol (ECP), it only needs one pair of less-entangled cluster state, which makes this ECP more economical. With the help of electronic polarization beam splitter (PBS) and the charge detection, the whole concentration process is essentially the quantum nondemolition (QND) measurement. Therefore, the concentrated maximally entangled state can be remained for further application. Moreover, the discarded terms in some traditional ECPs can be reused to obtain a high success probability. It is feasible and useful in current one-way quantum computation.

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

Blancon, Jean -Christophe Robert; Tsai, Hsinhan; Nie, Wanyi

Understanding and controlling charge and energy flow in state-of-the-art semiconductor quantum wells has enabled high-efficiency optoelectronic devices. Two-dimensional (2D) Ruddlesden-Popper perovskites are solution-processed quantum wells wherein the band gap can be tuned by varying the perovskite-layer thickness, which modulates the effective electron-hole confinement. We report that, counterintuitive to classical quantum-confined systems where photogenerated electrons and holes are strongly bound by Coulomb interactions or excitons, the photophysics of thin films made of Ruddlesden-Popper perovskites with a thickness exceeding two perovskite-crystal units (>1.3 nanometers) is dominated by lower-energy states associated with the local intrinsic electronic structure of the edges of the perovskitemore » layers. Furthermore, these states provide a direct pathway for dissociating excitons into longer-lived free carriers that substantially improve the performance of optoelectronic devices.« less

Electric-field-induced interferometric resonance of a one-dimensional spin-orbit-coupled electron

PubMed Central

Fan, Jingtao; Chen, Yuansen; Chen, Gang; Xiao, Liantuan; Jia, Suotang; Nori, Franco

2016-01-01

The efficient control of electron spins is of crucial importance for spintronics, quantum metrology, and quantum information processing. We theoretically formulate an electric mechanism to probe the electron spin dynamics, by focusing on a one-dimensional spin-orbit-coupled nanowire quantum dot. Owing to the existence of spin-orbit coupling and a pulsed electric field, different spin-orbit states are shown to interfere with each other, generating intriguing interference-resonant patterns. We also reveal that an in-plane magnetic field does not affect the interval of any neighboring resonant peaks, but contributes a weak shift of each peak, which is sensitive to the direction of the magnetic field. We find that this proposed external-field-controlled scheme should be regarded as a new type of quantum-dot-based interferometry. This interferometry has potential applications in precise measurements of relevant experimental parameters, such as the Rashba and Dresselhaus spin-orbit-coupling strengths, as well as the Landé factor. PMID:27966598

Efficient Multi-Dimensional Simulation of Quantum Confinement Effects in Advanced MOS Devices

NASA Technical Reports Server (NTRS)

Biegel, Bryan A.; Ancona, Mario G.; Rafferty, Conor S.; Yu, Zhiping

2000-01-01

We investigate the density-gradient (DG) transport model for efficient multi-dimensional simulation of quantum confinement effects in advanced MOS devices. The formulation of the DG model is described as a quantum correction ot the classical drift-diffusion model. Quantum confinement effects are shown to be significant in sub-100nm MOSFETs. In thin-oxide MOS capacitors, quantum effects may reduce gate capacitance by 25% or more. As a result, the inclusion of quantum effects may reduce gate capacitance by 25% or more. As a result, the inclusion of quantum effects in simulations dramatically improves the match between C-V simulations and measurements for oxide thickness down to 2 nm. Significant quantum corrections also occur in the I-V characteristics of short-channel (30 to 100 nm) n-MOSFETs, with current drive reduced by up to 70%. This effect is shown to result from reduced inversion charge due to quantum confinement of electrons in the channel. Also, subthreshold slope is degraded by 15 to 20 mV/decade with the inclusion of quantum effects via the density-gradient model, and short channel effects (in particular, drain-induced barrier lowering) are noticeably increased.

Enhanced Electron Injection and Exciton Confinement for Pure Blue Quantum-Dot Light-Emitting Diodes by Introducing Partially Oxidized Aluminum Cathode.

PubMed

Wang, Zhibin; Cheng, Tai; Wang, Fuzhi; Bai, Yiming; Bian, Xingming; Zhang, Bing; Hayat, Tasawar; Alsaedi, Ahmed; Tan, Zhan'ao

2018-05-31

Stable and efficient red (R), green (G), and blue (B) light sources based on solution-processed quantum dots (QDs) play important roles in next-generation displays and solid-state lighting technologies. The brightness and efficiency of blue QDs-based light-emitting diodes (LEDs) remain inferior to their red and green counterparts, due to the inherently unfavorable energy levels of different colors of light. To solve these problems, a device structure should be designed to balance the injection holes and electrons into the emissive QD layer. Herein, through a simple autoxidation strategy, pure blue QD-LEDs which are highly bright and efficient are demonstrated, with a structure of ITO/PEDOT:PSS/Poly-TPD/QDs/Al:Al2O3. The autoxidized Al:Al2O3 cathode can effectively balance the injected charges and enhance radiative recombination without introducing an additional electron transport layer (ETL). As a result, high color-saturated blue QD-LEDs are achieved with a maximum luminance over 13,000 cd m -2 , and a maximum current efficiency of 1.15 cd A -1 . The easily controlled autoxidation procedure paves the way for achieving high-performance blue QD-LEDs.

Single Quantum Dot with Microlens and 3D-Printed Micro-objective as Integrated Bright Single-Photon Source

PubMed Central

2017-01-01

Integrated single-photon sources with high photon-extraction efficiency are key building blocks for applications in the field of quantum communications. We report on a bright single-photon source realized by on-chip integration of a deterministic quantum dot microlens with a 3D-printed multilens micro-objective. The device concept benefits from a sophisticated combination of in situ 3D electron-beam lithography to realize the quantum dot microlens and 3D femtosecond direct laser writing for creation of the micro-objective. In this way, we obtain a high-quality quantum device with broadband photon-extraction efficiency of (40 ± 4)% and high suppression of multiphoton emission events with g(2)(τ = 0) < 0.02. Our results highlight the opportunities that arise from tailoring the optical properties of quantum emitters using integrated optics with high potential for the further development of plug-and-play fiber-coupled single-photon sources. PMID:28670600

Towards scalable quantum communication and computation: Novel approaches and realizations

NASA Astrophysics Data System (ADS)

Jiang, Liang

Quantum information science involves exploration of fundamental laws of quantum mechanics for information processing tasks. This thesis presents several new approaches towards scalable quantum information processing. First, we consider a hybrid approach to scalable quantum computation, based on an optically connected network of few-qubit quantum registers. Specifically, we develop a novel scheme for scalable quantum computation that is robust against various imperfections. To justify that nitrogen-vacancy (NV) color centers in diamond can be a promising realization of the few-qubit quantum register, we show how to isolate a few proximal nuclear spins from the rest of the environment and use them for the quantum register. We also demonstrate experimentally that the nuclear spin coherence is only weakly perturbed under optical illumination, which allows us to implement quantum logical operations that use the nuclear spins to assist the repetitive-readout of the electronic spin. Using this technique, we demonstrate more than two-fold improvement in signal-to-noise ratio. Apart from direct application to enhance the sensitivity of the NV-based nano-magnetometer, this experiment represents an important step towards the realization of robust quantum information processors using electronic and nuclear spin qubits. We then study realizations of quantum repeaters for long distance quantum communication. Specifically, we develop an efficient scheme for quantum repeaters based on atomic ensembles. We use dynamic programming to optimize various quantum repeater protocols. In addition, we propose a new protocol of quantum repeater with encoding, which efficiently uses local resources (about 100 qubits) to identify and correct errors, to achieve fast one-way quantum communication over long distances. Finally, we explore quantum systems with topological order. Such systems can exhibit remarkable phenomena such as quasiparticles with anyonic statistics and have been proposed as candidates for naturally error-free quantum computation. We propose a scheme to unambiguously detect the anyonic statistics in spin lattice realizations using ultra-cold atoms in an optical lattice. We show how to reliably read and write topologically protected quantum memory using an atomic or photonic qubit.

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

Damtie, Fikeraddis A., E-mail: Fikeraddis.Damtie@teorfys.lu.se; Wacker, Andreas, E-mail: Andreas.Wacker@fysik.lu.se; Karki, Khadga J., E-mail: Khadga.Karki@chemphys.lu.se

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.

Theory of the power characteristics of quantum-well lasers with asymmetric barrier layers: Inclusion of asymmetry in electron- and hole-state filling

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

Asryan, L. V., E-mail: asryan@vt.edu; Zubov, F. I.; Kryzhanovskaya, N. V.

2016-10-15

The power characteristics of quantum-well lasers with asymmetric barrier layers, which represent a novel type of injection laser, are calculated on the basis of an extended model taking into account asymmetry in the filling of electron and hole states. The electron–hole asymmetry is shown to have no significant effect on the characteristics of these lasers. Even in the presence of intermediate layers (located between the quantum well and each of the two asymmetric barrier layers), where parasitic electron–hole recombination does occur, the internal differential quantum efficiency of such a laser exhibits only a weak dependence on the pump current andmore » remains close to unity; therefore, the light–current characteristic remains linear up to high pumping levels.« less

Highly efficient gate-tunable photocurrent generation in vertical heterostructures of layered materials

PubMed Central

Yu, Woo Jong; Liu, Yuan; Zhou, Hailong; Yin, Anxiang; Li, Zheng; Huang, Yu

2014-01-01

Layered materials of graphene and MoS2, for example, have recently emerged as an exciting material system for future electronics and optoelectronics. Vertical integration of layered materials can enable the design of novel electronic and photonic devices. Here, we report highly efficient photocurrent generation from vertical heterostructures of layered materials. We show that vertically stacked graphene–MoS2–graphene and graphene–MoS2–metal junctions can be created with a broad junction area for efficient photon harvesting. The weak electrostatic screening effect of graphene allows the integration of single or dual gates under and/or above the vertical heterostructure to tune the band slope and photocurrent generation. We demonstrate that the amplitude and polarity of the photocurrent in the gated vertical heterostructures can be readily modulated by the electric field of an external gate to achieve a maximum external quantum efficiency of 55% and internal quantum efficiency up to 85%. Our study establishes a method to control photocarrier generation, separation and transport processes using an external electric field. PMID:24162001

Metallic tin quantum sheets confined in graphene toward high-efficiency carbon dioxide electroreduction

NASA Astrophysics Data System (ADS)

Lei, Fengcai; Liu, Wei; Sun, Yongfu; Xu, Jiaqi; Liu, Katong; Liang, Liang; Yao, Tao; Pan, Bicai; Wei, Shiqiang; Xie, Yi

2016-09-01

Ultrathin metal layers can be highly active carbon dioxide electroreduction catalysts, but may also be prone to oxidation. Here we construct a model of graphene confined ultrathin layers of highly reactive metals, taking the synthetic highly reactive tin quantum sheets confined in graphene as an example. The higher electrochemical active area ensures 9 times larger carbon dioxide adsorption capacity relative to bulk tin, while the highly-conductive graphene favours rate-determining electron transfer from carbon dioxide to its radical anion. The lowered tin-tin coordination numbers, revealed by X-ray absorption fine structure spectroscopy, enable tin quantum sheets confined in graphene to efficiently stabilize the carbon dioxide radical anion, verified by 0.13 volts lowered potential of hydroxyl ion adsorption compared with bulk tin. Hence, the tin quantum sheets confined in graphene show enhanced electrocatalytic activity and stability. This work may provide a promising lead for designing efficient and robust catalysts for electrolytic fuel synthesis.

Alternating InGaN barriers with GaN barriers for enhancing optical performance in InGaN light-emitting diodes

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

Yang, Yujue; Zeng, Yiping, E-mail: ypzeng@semi.ac.cn

2015-01-21

InGaN-based light-emitting diodes (LEDs) with some specific designs on the quantum barrier layers by alternating InGaN barriers with GaN barriers are proposed and studied numerically. In the proposed structure, simulation results show that the carriers are widely dispersed in the multi-quantum well active region, and the radiative recombination rate is efficiently improved and the electron leakage is suppressed accordingly, due to the appropriate band engineering. The internal quantum efficiency and light-output power are thus markedly enhanced and the efficiency droop is smaller, compared to the original structures with GaN barriers or InGaN barriers. Moreover, the gradually decrease of indium compositionmore » in the alternating quantum barriers can further promote the LED performance because of the more uniform carrier distribution, which provides us a simple but highly effective approach for high-performance LED applications.« less

Organic molecules as tools to control the growth, surface structure, and redox activity of colloidal quantum dots.

PubMed

Weiss, Emily A

2013-11-19

In order to achieve efficient and reliable technology that can harness solar energy, the behavior of electrons and energy at interfaces between different types or phases of materials must be understood. Conversion of light to chemical or electrical potential in condensed phase systems requires gradients in free energy that allow the movement of energy or charge carriers and facilitate redox reactions and dissociation of photoexcited states (excitons) into free charge carriers. Such free energy gradients are present at interfaces between solid and liquid phases or between inorganic and organic materials. Nanostructured materials have a higher density of these interfaces than bulk materials. Nanostructured materials, however, have a structural and chemical complexity that does not exist in bulk materials, which presents a difficult challenge: to lower or eliminate energy barriers to electron and energy flux that inevitably result from forcing different materials to meet in a spatial region of atomic dimensions. Chemical functionalization of nanostructured materials is perhaps the most versatile and powerful strategy for controlling the potential energy landscape of their interfaces and for minimizing losses in energy conversion efficiency due to interfacial structural and electronic defects. Colloidal quantum dots are semiconductor nanocrystals synthesized with wet-chemical methods and coated in organic molecules. Chemists can use these model systems to study the effects of chemical functionalization of nanoscale organic/inorganic interfaces on the optical and electronic properties of a nanostructured material, and the behavior of electrons and energy at interfaces. The optical and electronic properties of colloidal quantum dots have an intense sensitivity to their surface chemistry, and their organic adlayers make them dispersible in solvent. This allows researchers to use high signal-to-noise solution-phase spectroscopy to study processes at interfaces. In this Account, I describe the varied roles of organic molecules in controlling the structure and properties of colloidal quantum dots. Molecules serve as surfactant that determines the mechanism and rate of nucleation and growth and the final size and surface structure of a quantum dot. Anionic surfactant in the reaction mixture allows precise control over the size of the quantum dot core but also drives cation enrichment and structural disordering of the quantum dot surface. Molecules serve as chemisorbed ligands that dictate the energetic distribution of surface states. These states can then serve as thermodynamic traps for excitonic charge carriers or couple to delocalized states of the quantum dot core to change the confinement energy of excitonic carriers. Ligands, therefore, in some cases, dramatically shift the ground state absorption and photoluminescence spectra of quantum dots. Molecules also act as protective layers that determine the probability of redox processes between quantum dots and other molecules. How much the ligand shell insulates the quantum dot from electron exchange with a molecular redox partner depends less on the length or degree of conjugation of the native ligand and more on the density and packing structure of the adlayer and the size and adsorption mode of the molecular redox partner. Control of quantum dot properties in these examples demonstrates that nanoscale interfaces, while complex, can be rationally designed to enhance or specify the functionality of a nanostructured system.

Synergistic doping of fullerene electron transport layer and colloidal quantum dot solids enhances solar cell performance.

PubMed

Yuan, Mingjian; Voznyy, Oleksandr; Zhitomirsky, David; Kanjanaboos, Pongsakorn; Sargent, Edward H

2015-02-04

The spatial location of the predominant source of performance-limiting recombination in today's best colloidal quantum dot (CQD) cells is identified, pinpointing the TiO2:CQD junction; then, a highly n-doped PCBM layer is introduced at the CQD:TiO2 heterointerface. An n-doped PCBM layer is essential to maintain the depletion region and allow for efficient current extraction, thereby producing a record 8.9% in overall power conversion efficiency. © 2014 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Engineering coherence among excited states in synthetic heterodimer systems.

PubMed

Hayes, Dugan; Griffin, Graham B; Engel, Gregory S

2013-06-21

The design principles that support persistent electronic coherence in biological light-harvesting systems are obscured by the complexity of such systems. Some electronic coherences in these systems survive for hundreds of femtoseconds at physiological temperatures, suggesting that coherent dynamics may play a role in photosynthetic energy transfer. Coherent effects may increase energy transfer efficiency relative to strictly incoherent transfer mechanisms. Simple, tractable, manipulable model systems are required in order to probe the fundamental physics underlying these persistent electronic coherences, but to date, these quantum effects have not been observed in small molecules. We have engineered a series of rigid synthetic heterodimers that can serve as such a model system and observed quantum beating signals in their two-dimensional electronic spectra consistent with the presence of persistent electronic coherences.

A universal quantum module for quantum communication, computation, and metrology

NASA Astrophysics Data System (ADS)

Hanks, Michael; Lo Piparo, Nicolò; Trupke, Michael; Schmiedmayer, Jorg; Munro, William J.; Nemoto, Kae

2017-08-01

In this work, we describe a simple module that could be ubiquitous for quantum information based applications. The basic modules comprises a single NV- center in diamond embedded in an optical cavity, where the cavity mediates interactions between photons and the electron spin (enabling entanglement distribution and efficient readout), while the nuclear spins constitutes a long-lived quantum memories capable of storing and processing quantum information. We discuss how a network of connected modules can be used for distributed metrology, communication and computation applications. Finally, we investigate the possible use of alternative diamond centers (SiV/GeV) within the module and illustrate potential advantages.

Evaluation of large format electron bombarded virtual phase CCDs as ultraviolet imaging detectors

NASA Technical Reports Server (NTRS)

Opal, Chet B.; Carruthers, George R.

1989-01-01

In conjunction with an external UV-sensitive cathode, an electron-bombarded CCD may be used as a high quantum efficiency/wide dynamic range photon-counting UV detector. Results are presented for the case of a 1024 x 1024, 18-micron square pixel virtual phase CCD used with an electromagnetically focused f/2 Schmidt camera, which yields excellent simgle-photoevent discrimination and counting efficiency. Attention is given to the vacuum-chamber arrangement used to conduct system tests and the CCD electronics and data-acquisition systems employed.

Solving Boltzmann and Fokker-Planck Equations Using Sparse Representation

DTIC Science & Technology

2011-05-31

material science. We have com- puted the electronic structure of 2D quantum dot system, and compared the efficiency with the benchmark software OCTOPUS . For...one self-consistent iteration step with 512 electrons, OCTOPUS costs 1091 sec, and selected inversion costs 9.76 sec. The algorithm exhibits

Carrier multiplication and charge transport in artificial quantum-dot solids probed by ultrafast photocurrent spectroscopy (Conference Presentation)

NASA Astrophysics Data System (ADS)

Klimov, Victor I.

2017-05-01

Understanding and controlling carrier transport and recombination dynamics in colloidal quantum dot films is key to their application in electronic and optoelectronic devices. Towards this end, we have conducted transient photocurrent measurements to monitor transport through quantum confined band edge states in lead selenide quantum dots films as a function of pump fluence, temperature, electrical bias, and surface treatment. Room temperature dynamics reveal two distinct timescales of intra-dot geminate processes followed by non-geminate inter-dot processes. The non-geminate kinetics is well described by the recombination of holes with photoinjected and pre-existing electrons residing in mid-gap states. We find the mobility of the quantum-confined states shows no temperature dependence down to 6 K, indicating a tunneling mechanism of early time photoconductance. We present evidence of the importance of the exciton fine structure in controlling the low temperature photoconductance, whereby the nanoscale enhanced exchange interaction between electrons and holes in quantum dots introduces a barrier to charge separation. Finally, side-by-side comparison of photocurrent transients using excitation with low- and high-photon energies (1.5 vs. 3.0 eV) reveals clear signatures of carrier multiplication (CM), that is, generation of multiple excitons by single photons. Based on photocurrent measurements of quantum dot solids and optical measurements of solution based samples, we conclude that the CM efficiency is unaffected by strong inter-dot coupling. Therefore, the results of previous numerous spectroscopic CM studies conducted on dilute quantum dot suspensions should, in principle, be reproducible in electronically coupled QD films used in devices.

Photodeposition of Ag2S on TiO2 nanorod arrays for quantum dot-sensitized solar cells

PubMed Central

2013-01-01

Ag2S quantum dots were deposited on the surface of TiO2 nanorod arrays by a two-step photodeposition. The prepared TiO2 nanorod arrays as well as the Ag2S deposited electrodes were characterized by X-ray diffraction, scanning electron microscope, and transmission electron microscope, suggesting a large coverage of Ag2S quantum dots on the ordered TiO2 nanorod arrays. UV–vis absorption spectra of Ag2S deposited electrodes show a broad absorption range of the visible light. The quantum dot-sensitized solar cells (QDSSCs) based on these electrodes were fabricated, and the photoelectrochemical properties were examined. A high photocurrent density of 10.25 mA/cm2 with a conversion efficiency of 0.98% at AM 1.5 solar light of 100 mW/cm2 was obtained with an optimal photodeposition time. The performance of the QDSSC at different incident light intensities was also investigated. The results display a better performance at a lower incident light level with a conversion efficiency of 1.25% at 47 mW/cm2. PMID:23286551

Structural Basis for Near Unity Quantum Yield Core/Shell Nanostructures

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

McBride, James; Treadway, Joe; Pennycook, Stephen J

2006-01-01

Aberration-corrected Z-contrast scanning transmission electron microscopy of core/shell nanocrystals shows clear correlations between structure and quantum efficiency. Uniform shell coverage is obtained only for a graded CdS/ZnS shell material and is found to be critical to achieving near 100% quantum yield. The sublattice sensitivity of the images confirms that preferential growth takes place on the anion-terminated surfaces. This explains the three-dimensional "nanobullet" shape observed in the case of core/shell nanorods.

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

Zhang, Z. D.; Wang, J.; Department of Chemistry, SUNY Stony Brook, New York 11794

We established a theoretical framework in terms of the curl flux, population landscape, and coherence for non-equilibrium quantum systems at steady state, through exploring the energy and charge transport in molecular processes. The curl quantum flux plays the key role in determining transport properties and the system reaches equilibrium when flux vanishes. The novel curl quantum flux reflects the degree of non-equilibriumness and the time-irreversibility. We found an analytical expression for the quantum flux and its relationship to the environmental pumping (non-equilibriumness quantified by the voltage away from the equilibrium) and the quantum tunneling. Furthermore, we investigated another quantum signature,more » the coherence, quantitatively measured by the non-zero off diagonal element of the density matrix. Populations of states give the probabilities of individual states and therefore quantify the population landscape. Both curl flux and coherence depend on steady state population landscape. Besides the environment-assistance which can give dramatic enhancement of coherence and quantum flux with high voltage at a fixed tunneling strength, the quantum flux is promoted by the coherence in the regime of small tunneling while reduced by the coherence in the regime of large tunneling, due to the non-monotonic relationship between the coherence and tunneling. This is in contrast to the previously found linear relationship. For the systems coupled to bosonic (photonic and phononic) reservoirs the flux is significantly promoted at large voltage while for fermionic (electronic) reservoirs the flux reaches a saturation after a significant enhancement at large voltage due to the Pauli exclusion principle. In view of the system as a quantum heat engine, we studied the non-equilibrium thermodynamics and established the analytical connections of curl quantum flux to the transport quantities such as energy (charge) transfer efficiency, chemical reaction efficiency, energy dissipation, heat and electric currents observed in the experiments. We observed a perfect transfer efficiency in chemical reactions at high voltage (chemical potential difference). Our theoretical predicted behavior of the electric current with respect to the voltage is in good agreements with the recent experiments on electron transfer in single molecules.« less

Relationships between the Efficiencies of Photosystems I and II and Stromal Redox State in CO2-Free Air 1

PubMed Central

Harbinson, Jeremy; Foyer, Christine H.

1991-01-01

The responses of the efficiencies of photosystems I and II, stromal redox state (as indicated by NADP-malate dehydrogenase activation state), and activation of the Benson-Calvin cycle enzymes ribulose 1,5-bisphosphate carboxylase and fructose 1,6-bisphosphatase to varying irradiance were measured in pea (Pisum sativum L.) leaves operating close to the CO2 compensation point. A comparison of the relationships among these parameters obtained from leaves in air was made with those obtained when the leaves were maintained in air from which the CO2 had been removed. P700 was more oxidized at any measured irradiance in CO2-free air than in air. The relationship between the quantum efficiencies of the photosystems in CO2-free air was distinctly curvilinear in contrast to the predominantly linear relationship obtained with leaves in air. This nonlinearity may be consistent with the operation of cyclic electron flow around photosystem I because the quantum efficiency of photosystem II was much more restricted than the quantum efficiency of photosystem I. In CO2-free air, measured NADP-malate dehydrogenase activities varied considerably at low irradiances. However, at high irradiance the activity of the enzyme was low, implying that the stroma was oxidized. In contrast, fructose-1,6-bisphosphatase activities tended to increase with increasing electron flux through the photosystems. Ribulose-1,5-bisphosphate carboxylase activity remained relatively constant with respect to irradiance in CO2-free air, with an activation state 50% of maximum. We conclude that, at the CO2 compensation point and high irradiance, low redox states are favored and that cyclic electron flow may be substantial. These two features may be the requirements necessary to trigger and maintain the dissipative processes in the thylakoid membrane. PMID:16668401

Exciton shelves for charge and energy transport in third-generation quantum-dot devices

NASA Astrophysics Data System (ADS)

Goodman, Samuel; Singh, Vivek; Noh, Hyunwoo; Casamada, Josep; Chatterjee, Anushree; Cha, Jennifer; Nagpal, Prashant

2014-03-01

Quantum dots are semiconductor nanocrystallites with size-dependent quantum-confined energy levels. While they have been intensively investigated to utilize hot-carriers for photovoltaic applications, to bridge the mismatch between incident solar photons and finite bandgap of semiconductor photocells, efficient charge or exciton transport in quantum-dot films has proven challenging. Here we show development of new coupled conjugated molecular wires with ``exciton shelves'', or different energy levels, matched with the multiple energy levels of quantum dots. Using single nanoparticle and ensemble device measurements we show successful extraction and transport of both bandedge and high-energy charge carriers, and energy transport of excitons. We demonstrate using measurements of electronic density of states, that careful matching of energy states of quantum-dot with molecular wires is important, and any mismatch can generate midgap states leading to charge recombination and reduced efficiency. Therefore, these exciton-shelves and quantum dots can lead to development of next-generation photovoltaic and photodetection devices using simultaneous transport of bandedge and hot-carriers or energy transport of excitons in these nanostructured solution-processed films.

Quantum heat engine power can be increased by noise-induced coherence

PubMed Central

Scully, Marlan O.; Chapin, Kimberly R.; Dorfman, Konstantin E.; Kim, Moochan Barnabas; Svidzinsky, Anatoly

2011-01-01

Laser and photocell quantum heat engines (QHEs) are powered by thermal light and governed by the laws of quantum thermodynamics. To appreciate the deep connection between quantum mechanics and thermodynamics we need only recall that in 1901 Planck introduced the quantum of action to calculate the entropy of thermal light, and in 1905 Einstein’s studies of the entropy of thermal light led him to introduce the photon. Then in 1917, he discovered stimulated emission by using detailed balance arguments. Half a century later, Scovil and Schulz-DuBois applied detailed balance ideas to show that maser photons were produced with Carnot quantum efficiency (see Fig. 1A). Furthermore, Shockley and Quiesser invoked detailed balance to obtain the efficiency of a photocell illuminated by “hot” thermal light (see Fig. 2A). To understand this detailed balance limit, we note that in the QHE, the incident light excites electrons, which can then deliver useful work to a load. However, the efficiency is limited by radiative recombination in which the excited electrons are returned to the ground state. But it has been proven that radiatively induced quantum coherence can break detailed balance and yield lasing without inversion. Here we show that noise-induced coherence enables us to break detailed balance and get more power out of a laser or photocell QHE. Surprisingly, this coherence can be induced by the same noisy (thermal) emission and absorption processes that drive the QHE (see Fig. 3A). Furthermore, this noise-induced coherence can be robust against environmental decoherence.Fig. 1.(A) Schematic of a laser pumped by hot photons at temperature Th (energy source, blue) and by cold photons at temperature Tc (entropy sink, red). The laser emits photons (green) such that at threshold the laser photon energy and pump photon energy is related by Carnot efficiency (4). (B) Schematic of atoms inside the cavity. Lower level b is coupled to the excited states a and β. The laser power is governed by the average number of hot and cold thermal photons, and . (C) Same as B but lower b level is replaced by two states b1 and b2, which can double the power when there is coherence between the levels.Fig. 2.(A) Schematic of a photocell consisting of quantum dots sandwiched between p and n doped semiconductors. Open circuit voltage and solar photon energy ℏνh are related by the Carnot efficiency factor where Tc is the ambient and Th is the solar temperature. (B) Schematic of a quantum dot solar cell in which state b is coupled to a via, e.g., solar radiation and coupled to the valence band reservoir state β via optical phonons. The electrons in conduction band reservoir state α pass to state β via an external circuit, which contains the load. (C) Same as B but lower level b is replaced by two states b1 and b2, and when coherently prepared can double the output power.Fig. 3.(A) Photocell current j = Γραα (laser photon flux Pl/ℏνl) (in arbitrary units) generated by the photovoltaic cell QHE (laser QHE) of Fig. 1C (Fig. 2C) as a function of maximum work (in electron volts) done by electron (laser photon) Eα - Eβ + kTc log(ραα/ρββ) with full (red line), partial (brown line), and no quantum interference (blue line). (B) Power of a photocell of Fig. 2C as a function of voltage for different decoherence rates , 100γ1c. Upper curve indicates power acquired from the sun. PMID:21876187

Quantum heat engine power can be increased by noise-induced coherence.

PubMed

Scully, Marlan O; Chapin, Kimberly R; Dorfman, Konstantin E; Kim, Moochan Barnabas; Svidzinsky, Anatoly

2011-09-13

Laser and photocell quantum heat engines (QHEs) are powered by thermal light and governed by the laws of quantum thermodynamics. To appreciate the deep connection between quantum mechanics and thermodynamics we need only recall that in 1901 Planck introduced the quantum of action to calculate the entropy of thermal light, and in 1905 Einstein's studies of the entropy of thermal light led him to introduce the photon. Then in 1917, he discovered stimulated emission by using detailed balance arguments. Half a century later, Scovil and Schulz-DuBois applied detailed balance ideas to show that maser photons were produced with Carnot quantum efficiency (see Fig. 1A). Furthermore, Shockley and Quiesser invoked detailed balance to obtain the efficiency of a photocell illuminated by "hot" thermal light (see Fig. 2A). To understand this detailed balance limit, we note that in the QHE, the incident light excites electrons, which can then deliver useful work to a load. However, the efficiency is limited by radiative recombination in which the excited electrons are returned to the ground state. But it has been proven that radiatively induced quantum coherence can break detailed balance and yield lasing without inversion. Here we show that noise-induced coherence enables us to break detailed balance and get more power out of a laser or photocell QHE. Surprisingly, this coherence can be induced by the same noisy (thermal) emission and absorption processes that drive the QHE (see Fig. 3A). Furthermore, this noise-induced coherence can be robust against environmental decoherence.Fig. 1.(A) Schematic of a laser pumped by hot photons at temperature T(h) (energy source, blue) and by cold photons at temperature T(c) (entropy sink, red). The laser emits photons (green) such that at threshold the laser photon energy and pump photon energy is related by Carnot efficiency (4). (B) Schematic of atoms inside the cavity. Lower level b is coupled to the excited states a and β. The laser power is governed by the average number of hot and cold thermal photons, and . (C) Same as B but lower b level is replaced by two states b(1) and b(2), which can double the power when there is coherence between the levels.Fig. 2.(A) Schematic of a photocell consisting of quantum dots sandwiched between p and n doped semiconductors. Open circuit voltage and solar photon energy ℏν(h) are related by the Carnot efficiency factor where T(c) is the ambient and T(h) is the solar temperature. (B) Schematic of a quantum dot solar cell in which state b is coupled to a via, e.g., solar radiation and coupled to the valence band reservoir state β via optical phonons. The electrons in conduction band reservoir state α pass to state β via an external circuit, which contains the load. (C) Same as B but lower level b is replaced by two states b(1) and b(2), and when coherently prepared can double the output power.Fig. 3.(A) Photocell current j = Γρ(αα) (laser photon flux P(l)/ℏ(ν(l))) (in arbitrary units) generated by the photovoltaic cell QHE (laser QHE) of Fig. 1C (Fig. 2C) as a function of maximum work (in electron volts) done by electron (laser photon) E(α) - E(β) + kT(c) log(ρ(αα)/ρ(ββ)) with full (red line), partial (brown line), and no quantum interference (blue line). (B) Power of a photocell of Fig. 2C as a function of voltage for different decoherence rates , 100γ(1c). Upper curve indicates power acquired from the sun.

Relationships between the Efficiencies of Photosystems I and II and Stromal Redox State in CO(2)-Free Air : Evidence for Cyclic Electron Flow in Vivo.

PubMed

Harbinson, J; Foyer, C H

1991-09-01

The responses of the efficiencies of photosystems I and II, stromal redox state (as indicated by NADP-malate dehydrogenase activation state), and activation of the Benson-Calvin cycle enzymes ribulose 1,5-bisphosphate carboxylase and fructose 1,6-bisphosphatase to varying irradiance were measured in pea (Pisum sativum L.) leaves operating close to the CO(2) compensation point. A comparison of the relationships among these parameters obtained from leaves in air was made with those obtained when the leaves were maintained in air from which the CO(2) had been removed. P700 was more oxidized at any measured irradiance in CO(2)-free air than in air. The relationship between the quantum efficiencies of the photosystems in CO(2)-free air was distinctly curvilinear in contrast to the predominantly linear relationship obtained with leaves in air. This nonlinearity may be consistent with the operation of cyclic electron flow around photosystem I because the quantum efficiency of photosystem II was much more restricted than the quantum efficiency of photosystem I. In CO(2)-free air, measured NADP-malate dehydrogenase activities varied considerably at low irradiances. However, at high irradiance the activity of the enzyme was low, implying that the stroma was oxidized. In contrast, fructose-1,6-bisphosphatase activities tended to increase with increasing electron flux through the photosystems. Ribulose-1,5-bisphosphate carboxylase activity remained relatively constant with respect to irradiance in CO(2)-free air, with an activation state 50% of maximum. We conclude that, at the CO(2) compensation point and high irradiance, low redox states are favored and that cyclic electron flow may be substantial. These two features may be the requirements necessary to trigger and maintain the dissipative processes in the thylakoid membrane.

Diffusion lengths in irradiated N/P InP-on-Si solar cells

NASA Technical Reports Server (NTRS)

Wojtczuk, Steven; Colerico, Claudia; Summers, Geoffrey P.; Walters, Robert J.; Burke, Edward A.

1996-01-01

Indium phosphide (InP) solar cells were made on silicon (Si) wafers (InP/Si) by to take advantage of both the radiation-hardness properties of the InP solar cell and the light weight and low cost of Si wafers. The InP/Si cell application is for long duration and/or high radiation orbit space missions. Spire has made N/P InP/Si cells of sizes up to 2 cm by 4 cm with beginning-of-life (BOL) AM0 efficiencies over 13% (one-sun, 28C). These InP/Si cells have higher absolute efficiency and power density after a high radiation dose than gallium arsenide (GaAs) or silicon (Si) solar cells after a fluence of about 2e15 1 MeV electrons/sq. cm. In this work, we investigate the minority carrier (electron) base diffusion lengths in the N/P InP/Si cells. A quantum efficiency model was constructed for a 12% BOL AM0 N/P InP/Si cell which agreed well with the absolutely measured quantum efficiency and the sun-simulator measured AM0 photocurrent (30.1 mA/sq. cm). This model was then used to generate a table of AM0 photocurrents for a range of base diffusion lengths. AM0 photocurrents were then measured for irradiations up to 7.7e16 1 MeV electrons/sq. cm (the 12% BOL cell was 8% after the final irradiation). By comparing the measured photocurrents with the predicted photocurrents, base diffusion lengths were assigned at each fluence level. A damage coefficient K of 4e-8 and a starting (unirradiated) base electron diffusion length of 0.8 microns fits the data well. The quantum efficiency was measured again at the end of the experiment to verify that the photocurrent predicted by the model (25.5 mA/sq. cm) agreed with the simulator-measured photocurrent after irradiation (25.7 mA/sq. cm).

Thermal conductivity engineering in width-modulated silicon nanowires and thermoelectric efficiency enhancement

NASA Astrophysics Data System (ADS)

Zianni, Xanthippi

2018-03-01

Width-modulated nanowires have been proposed as efficient thermoelectric materials. Here, the electron and phonon transport properties and the thermoelectric efficiency are discussed for dimensions above the quantum confinement regime. The thermal conductivity decreases dramatically in the presence of thin constrictions due to their ballistic thermal resistance. It shows a scaling behavior upon the width-modulation rate that allows for thermal conductivity engineering. The electron conductivity also decreases due to enhanced boundary scattering by the constrictions. The effect of boundary scattering is weaker for electrons than for phonons and the overall thermoelectric efficiency is enhanced. A ZT enhancement by a factor of 20-30 is predicted for width-modulated nanowires compared to bulk silicon. Our findings indicate that width-modulated nanostructures are promising for developing silicon nanostructures with high thermoelectric efficiency.

Ultra-bright and highly efficient inorganic based perovskite light-emitting diodes

PubMed Central

Zhang, Liuqi; Yang, Xiaolei; Jiang, Qi; Wang, Pengyang; Yin, Zhigang; Zhang, Xingwang; Tan, Hairen; Yang, Yang (Michael); Wei, Mingyang; Sutherland, Brandon R.; Sargent, Edward H.; You, Jingbi

2017-01-01

Inorganic perovskites such as CsPbX3 (X=Cl, Br, I) have attracted attention due to their excellent thermal stability and high photoluminescence quantum efficiency. However, the electroluminescence quantum efficiency of their light-emitting diodes was <1%. We posited that this low efficiency was a result of high leakage current caused by poor perovskite morphology, high non-radiative recombination at interfaces and perovskite grain boundaries, and also charge injection imbalance. Here, we incorporated a small amount of methylammonium organic cation into the CsPbBr3 lattice and by depositing a hydrophilic and insulating polyvinyl pyrrolidine polymer atop the ZnO electron-injection layer to overcome these issues. As a result, we obtained light-emitting diodes exhibiting a high brightness of 91,000 cd m−2 and a high external quantum efficiency of 10.4% using a mixed-cation perovskite Cs0.87MA0.13PbBr3 as the emitting layer. To the best of our knowledge, this is the brightest and most-efficient green perovskite light-emitting diodes reported to date. PMID:28589960

Ultra-bright and highly efficient inorganic based perovskite light-emitting diodes

NASA Astrophysics Data System (ADS)

Zhang, Liuqi; Yang, Xiaolei; Jiang, Qi; Wang, Pengyang; Yin, Zhigang; Zhang, Xingwang; Tan, Hairen; Yang, Yang (Michael); Wei, Mingyang; Sutherland, Brandon R.; Sargent, Edward H.; You, Jingbi

2017-06-01

Inorganic perovskites such as CsPbX3 (X=Cl, Br, I) have attracted attention due to their excellent thermal stability and high photoluminescence quantum efficiency. However, the electroluminescence quantum efficiency of their light-emitting diodes was <1%. We posited that this low efficiency was a result of high leakage current caused by poor perovskite morphology, high non-radiative recombination at interfaces and perovskite grain boundaries, and also charge injection imbalance. Here, we incorporated a small amount of methylammonium organic cation into the CsPbBr3 lattice and by depositing a hydrophilic and insulating polyvinyl pyrrolidine polymer atop the ZnO electron-injection layer to overcome these issues. As a result, we obtained light-emitting diodes exhibiting a high brightness of 91,000 cd m-2 and a high external quantum efficiency of 10.4% using a mixed-cation perovskite Cs0.87MA0.13PbBr3 as the emitting layer. To the best of our knowledge, this is the brightest and most-efficient green perovskite light-emitting diodes reported to date.

Resonantly driven CNOT gate for electron spins.

PubMed

Zajac, D M; Sigillito, A J; Russ, M; Borjans, F; Taylor, J M; Burkard, G; Petta, J R

2018-01-26

Single-qubit rotations and two-qubit CNOT operations are crucial ingredients for universal quantum computing. Although high-fidelity single-qubit operations have been achieved using the electron spin degree of freedom, realizing a robust CNOT gate has been challenging because of rapid nuclear spin dephasing and charge noise. We demonstrate an efficient resonantly driven CNOT gate for electron spins in silicon. Our platform achieves single-qubit rotations with fidelities greater than 99%, as verified by randomized benchmarking. Gate control of the exchange coupling allows a quantum CNOT gate to be implemented with resonant driving in ~200 nanoseconds. We used the CNOT gate to generate a Bell state with 78% fidelity (corrected for errors in state preparation and measurement). Our quantum dot device architecture enables multi-qubit algorithms in silicon. Copyright © 2018, The Authors, some rights reserved; exclusive licensee American Association for the Advancement of Science. No claim to original U.S. Government Works.

The Bravyi-Kitaev transformation for quantum computation of electronic structure

NASA Astrophysics Data System (ADS)

Seeley, Jacob T.; Richard, Martin J.; Love, Peter J.

2012-12-01

Quantum simulation is an important application of future quantum computers with applications in quantum chemistry, condensed matter, and beyond. Quantum simulation of fermionic systems presents a specific challenge. The Jordan-Wigner transformation allows for representation of a fermionic operator by O(n) qubit operations. Here, we develop an alternative method of simulating fermions with qubits, first proposed by Bravyi and Kitaev [Ann. Phys. 298, 210 (2002), 10.1006/aphy.2002.6254; e-print arXiv:quant-ph/0003137v2], that reduces the simulation cost to O(log n) qubit operations for one fermionic operation. We apply this new Bravyi-Kitaev transformation to the task of simulating quantum chemical Hamiltonians, and give a detailed example for the simplest possible case of molecular hydrogen in a minimal basis. We show that the quantum circuit for simulating a single Trotter time step of the Bravyi-Kitaev derived Hamiltonian for H2 requires fewer gate applications than the equivalent circuit derived from the Jordan-Wigner transformation. Since the scaling of the Bravyi-Kitaev method is asymptotically better than the Jordan-Wigner method, this result for molecular hydrogen in a minimal basis demonstrates the superior efficiency of the Bravyi-Kitaev method for all quantum computations of electronic structure.

Long-wavelength infrared (LWIR) quantum-dot infrared photodetector (QDIP) focal plane array

NASA Astrophysics Data System (ADS)

Gunapala, S. D.; Bandara, S. V.; Hill, C. J.; Ting, D. Z.; Liu, J. K.; Rafol, S. B.; Blazejewski, E. R.; Mumolo, J. M.; Keo, S. A.; Krishna, S.; Chang, Y. C.; Shott, C. A.

2006-05-01

We have exploited the artificial atomlike properties of epitaxially self-assembled quantum dots for the development of high operating temperature long wavelength infrared (LWIR) focal plane arrays. Quantum dots are nanometer-scale islands that form spontaneously on a semiconductor substrate due to lattice mismatch. QDIPs are expected to outperform quantum well infrared detectors (QWIPs) and are expected to offer significant advantages over II-VI material based focal plane arrays. QDIPs are fabricated using robust wide bandgap III-V materials which are well suited to the production of highly uniform LWIR arrays. We have used molecular beam epitaxy (MBE) technology to grow multi-layer LWIR quantum dot structures based on the InAs/InGaAs/GaAs material system. JPL is building on its significant QWIP experience and is basically building a Dot-in-the-Well (DWELL) device design by embedding InAs quantum dots in a QWIP structure. This hybrid quantum dot/quantum well device offers additional control in wavelength tuning via control of dot-size and/or quantum well sizes. In addition the quantum wells can trap electrons and aide in ground state refilling. Recent measurements have shown a 10 times higher photoconductive gain than the typical QWIP device, which indirectly confirms the lower relaxation rate of excited electrons (photon bottleneck) in QDIPs. Subsequent material and device improvements have demonstrated an absorption quantum efficiency (QE) of ~ 3%. Dot-in-the-well (DWELL) QDIPs were also experimentally shown to absorb both 45o and normally incident light. Thus we have employed a reflection grating structure to further enhance the quantum efficiency. JPL has demonstrated wavelength control by progressively growing material and fabricating devices structures that have continuously increased in LWIR response. The most recent devices exhibit peak responsivity out to 8.1 microns. Peak detectivity of the 8.1μm devices has reached ~ 1 x 1010 Jones at 77 K. Furthermore, we have fabricated the first long-wavelength 640x512 pixels QDIP focal plane array. This QDIP focal plane array has produced excellent infrared imagery with noise equivalent temperature difference of 40 mK at 60K operating temperature. In addition, we have managed to increase the quantum efficiency of these devices from 0.1% (according to the data published in literature) to 20% in discrete devices. This is a factor of 200 increase in quantum efficiency. With these excellent results, for the first time QDIP performance has surpassed the QWIP performance. Our goal is to operate these long-wavelength detectors at much higher operating temperature than 77K, which can be passively achieved in space. This will be a huge leap in high performance infrared detectors specifically applicable to space science instruments.

Long-Wavelength Infrared (LWIR) Quantum Dot Infrared Photodetector (QDIP) Focal Plane Array

NASA Technical Reports Server (NTRS)

Gunapala, Sarath D.; Bandara, S. V.; Liu, J. K.; Hill, C. J.; Rafol, S. B.; Mumolo, J. M.; Shott, C. A.

2006-01-01

We have exploited the artificial atomlike properties of epitaxially self-assembled quantum dots for the development of high operating temperature long wavelength infrared (LWIR) focal plane arrays. Quantum dots are nanometer-scale islands that form spontaneously on a semiconductor substrate due to lattice mismatch. QDIPs are expected to outperform quantum well infrared detectors (QWIPs) and are expected to offer significant advantages over II-VI material based focal plane arrays. QDIPs are fabricated using robust wide bandgap III-V materials which are well suited to the production of highly uniform LWIR arrays. We have used molecular beam epitaxy (MBE) technology to grow multi-layer LWIR quantum dot structures based on the InAs/InGaAs/GaAs material system. JPL is building on its significant QWIP experience and is basically building a Dot-in-the-Well (DWELL) device design by embedding InAs quantum dots in a QWIP structure. This hybrid quantum dot/quantum well device offers additional control in wavelength tuning via control of dot-size and/or quantum well sizes. In addition the quantum wells can trap electrons and aide in ground state refilling. Recent measurements have shown a 10 times higher photoconductive gain than the typical QWIP device, which indirectly confirms the lower relaxation rate of excited electrons (photon bottleneck) in QDPs. Subsequent material and device improvements have demonstrated an absorption quantum efficiency (QE) of approx. 3%. Dot-in-the-well (DWELL) QDIPs were also experimentally shown to absorb both 45 deg. and normally incident light. Thus we have employed a reflection grating structure to further enhance the quantum efficiency. JPL has demonstrated wavelength control by progressively growing material and fabricating devices structures that have continuously increased in LWIR response. The most recent devices exhibit peak responsivity out to 8.1 microns. Peak detectivity of the 8.1 micrometer devices has reached approx. 1 x 10(exp 10) Jones at 77 K. Furthermore, we have fabricated the first long-wavelength 640x512 pixels QDP focal plane array. This QDIP focal plane may has produced excellent infrared imagery with noise equivalent temperature difference of 40 mK at 60K operating temperature. In addition, we have managed to increase the quantum efficiency of these devices from 0.1% (according to the data published in literature) to 20% in discrete devices. This is a factor of 200 increase in quantum efficiency. With these excellent results, for the first time QDIP performance has surpassed the QWIP performance. Our goal is to operate these long-wavelength detectors at much higher operating temperature than 77K which can be passively achieved in space. This will be a huge leap in high performance infrared detectors specifically applicable to space science instruments.

Carrier transport dynamics in Mn-doped CdSe quantum dot sensitized solar cells

NASA Astrophysics Data System (ADS)

Poudyal, Uma; Maloney, Francis S.; Sapkota, Keshab; Wang, Wenyong

2017-10-01

In this work quantum dot sensitized solar cells (QDSSCs) were fabricated with CdSe and Mn-doped CdSe quantum dots (QDs) using the SILAR method. QDSSCs based on Mn-doped CdSe QDs exhibited improved incident photon-to-electron conversion efficiency. Carrier transport dynamics in the QDSSCs were studied using the intensity modulated photocurrent/photovoltage spectroscopy technique, from which transport and recombination time constants could be derived. Compared to CdSe QDSSCs, Mn-CdSe QDSSCs exhibited shorter transport time constant, longer recombination time constant, longer diffusion length, and higher charge collection efficiency. These observations suggested that Mn doping in CdSe QDs could benefit the performance of solar cells based on such nanostructures.

Impact of geometric, thermal and tunneling effects on nano-transistors

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

Hu, Langhua; Chen, Duan, E-mail: dchen10@uncc.edu; Wei, Guo-Wei

Electronic transistors are fundamental building blocks of large scale integrated circuits in modern advanced electronic equipments, and their sizes have been down-scaled to nanometers. Modeling and simulations in the framework of quantum dynamics have emerged as important tools to study functional characteristics of these nano-devices. This work explores the effects of geometric shapes of semiconductor–insulator interfaces, phonon–electron interactions, and quantum tunneling of three-dimensional (3D) nano-transistors. First, we propose a two-scale energy functional to describe the electron dynamics in a dielectric continuum of device material. Coupled governing equations, i.e., Poisson–Kohn–Sham (PKS) equations, are derived by the variational principle. Additionally, it ismore » found that at a given channel cross section area and gate voltage, the geometry that has the smallest perimeter of the channel cross section offers the largest channel current, which indicates that ultra-thin nanotransistors may not be very efficient in practical applications. Moreover, we introduce a new method to evaluate quantum tunneling effects in nanotransistors without invoking the comparison of classical and quantum predictions. It is found that at a given channel cross section area and gate voltage, the geometry that has the smallest perimeter of the channel cross section has the smallest quantum tunneling ratio, which indicates that geometric defects can lead to higher geometric confinement and larger quantum tunneling effect. Furthermore, although an increase in the phonon–electron interaction strength reduces channel current, it does not have much impact to the quantum tunneling ratio. Finally, advanced numerical techniques, including second order elliptic interface methods, have been applied to ensure computational accuracy and reliability of the present PKS simulation.« less

Magnetic field induced optical gain in a dilute nitride quaternary semiconductor quantum dot

NASA Astrophysics Data System (ADS)

Mageshwari, P. Uma; Peter, A. John; Lee, Chang Woo

2016-10-01

Effects of magnetic field strength on the electronic and optical properties are brought out in a Ga0.661In0.339N0.0554As0.9446/GaAs quantum dot for the applications of desired wavelength in opto-electronic devices. The band alignment is obtained using band anticrossing model and the model solid theory. The magnetic field dependent electron-heavy hole transition energies with the dot radius in a GaInNAs/GaAs quantum dot are investigated. The magnetic field induced oscillator strength as a function of dot radius is studied. The resonant peak values of optical absorption coefficients and the changes of refractive index with the application of magnetic field strength in a GaInNAs/GaAs quantum dot are obtained. The magnetic field induced threshold current density and the maximum optical gain are found in a GaInNAs/GaAs quantum dot. The results show that the optimum wavelength for fibre optical communication networks can be obtained with the variation of applied magnetic field strength and the outcomes may be useful for the design of efficient lasers based on the group III-N-V semiconductors.

Transmission electron microscopy of AlGaAs/GaAs quantum cascade laser structures.

PubMed

Walther, T; Krysa, A B

2017-12-01

Quantum cascade lasers can be efficient infrared radiation sources and consist of several hundreds of very thin layers arranged in stacks that are repeated periodically. Both the thicknesses of the individual layers as well as the period lengths need to be monitored to high precision. Different transmission electron microscopy methods have been combined to analyse AlGaAs/GaAs quantum cascade laser structures in cross-section. We found a small parabolic variation of the growth rate during deposition, affecting the stack periodicity and a reduced aluminium content of the AlGaAs barriers, whereas their widths as well as those of the GaAs quantum wells agreed with the nominal values within one atomic layer. Growth on an offcut substrate led to facets and steps at the interfaces. © 2017 The Authors Journal of Microscopy © 2017 Royal Microscopical Society.

Has the Sun Set on Quantum Dot-Sensitized Solar Cells?

DOE PAGES

Wrenn, Toshia L.; McBride, James R.; Smith, Nathanael J.; ...

2015-01-01

This is a reminder, a review and a look toward the future prospects for quantum dot-sensitized solar cells - a reminder of the highly viable, energy-efficient solar cells achievable. This is also a review of ground-breaking devices and their similarities to the near unity photon-to-electron mechanisms of photosynthesis; a look toward architectures that capitalize on the advances observed in previous work.

Impact of Alloy Fluctuations on Radiative and Auger Recombination in InGaN Quantum Wells

NASA Astrophysics Data System (ADS)

Jones, Christina; Teng, Chu-Hsiang; Yan, Qimin; Ku, Pei-Cheng; Kioupakis, Emmanouil

Light-emitting diodes (LEDs) based on indium gallium nitride (InGaN) are important for efficient solid-state lighting (2014 Nobel Prize in Physics). Despite its many successes, InGaN suffers from issues that reduce the efficiency of devices at high power, such as the green gap and efficiency droop. The origin of the droop has been attributed to Auger recombination, mediated by carrier scattering due to phonons and alloy disorder. Additionally, InGaN exhibits atomic-scale composition fluctuations that localize carriers and may affect the efficiency. In this work, we study the effect of local composition fluctuations on the radiative recombination rate, Auger recombination rate, and efficiency of InGaN/GaN quantum wells. We apply k.p calculations to simulate band edges and wave functions of quantum wells with fluctuating alloy distributions based on atom probe tomography data, and we evaluate double and triple overlaps of electron and hole wave functions. We compare results for quantum wells with fluctuating alloy distributions to those with uniform alloy compositions and to published work. Our results demonstrate that alloy-composition fluctuations aggravate the efficiency-droop and green-gap problems and further reduce LED efficiency at high power. We acknowledge the NSF CAREER award DMR-1254314, the NSF Graduate Research Fellowship Program DGE-1256260, and the DOE NERSC facility (DE-AC02-05CH11231).

Numerical approach of the quantum circuit theory

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

Silva, J.J.B., E-mail: jaedsonfisica@hotmail.com; Duarte-Filho, G.C.; Almeida, F.A.G.

2017-03-15

In this paper we develop a numerical method based on the quantum circuit theory to approach the coherent electronic transport in a network of quantum dots connected with arbitrary topology. The algorithm was employed in a circuit formed by quantum dots connected each other in a shape of a linear chain (associations in series), and of a ring (associations in series, and in parallel). For both systems we compute two current observables: conductance and shot noise power. We find an excellent agreement between our numerical results and the ones found in the literature. Moreover, we analyze the algorithm efficiency formore » a chain of quantum dots, where the mean processing time exhibits a linear dependence with the number of quantum dots in the array.« less

Graphene oxide quantum dot-sensitized porous titanium dioxide microsphere: Visible-light-driven photocatalyst based on energy band engineering.

PubMed

Zhang, Yu; Qi, Fuyuan; Li, Ying; Zhou, Xin; Sun, Hongfeng; Zhang, Wei; Liu, Daliang; Song, Xi-Ming

2017-07-15

We report a novel graphene oxide quantum dot (GOQD)-sensitized porous TiO 2 microsphere for efficient photoelectric conversion. Electro-chemical analysis along with the Mott-Schottky equation reveals conductivity type and energy band structure of the two semiconductors. Based on their energy band structures, visible light-induced electrons can transfer from the p-type GOQD to the n-type TiO 2 . Enhanced photocurrent and photocatalytic activity in visible light further confirm the enhanced separation of electrons and holes in the nanocomposite. Copyright © 2017 Elsevier Inc. All rights reserved.

Direct correlations of structural and optical properties of three-dimensional GaN/InGaN core/shell micro-light emitting diodes

NASA Astrophysics Data System (ADS)

Sadat Mohajerani, Matin; Müller, Marcus; Hartmann, Jana; Zhou, Hao; Wehmann, Hergo-H.; Veit, Peter; Bertram, Frank; Christen, Jürgen; Waag, Andreas

2016-05-01

Three-dimensional (3D) InGaN/GaN quantum-well (QW) core-shell light emitting diodes (LEDs) are a promising candidate for the future solid state lighting. In this contribution, we study direct correlations of structural and optical properties of the core-shell LEDs using highly spatially-resolved cathodoluminescence spectroscopy (CL) in combination with scanning electron microscopy (SEM) and scanning transmission electron microscopy (STEM). Temperature-dependent resonant photoluminescence (PL) spectroscopy has been performed to understand recombination mechanisms and to estimate the internal quantum efficiency (IQE).

New way for determining electron energy levels in quantum dots arrays using finite difference method

NASA Astrophysics Data System (ADS)

Dujardin, F.; Assaid, E.; Feddi, E.

2018-06-01

Electronic states are investigated in quantum dots arrays, depending on the type of cubic Bravais lattice (primitive, body centered or face centered) according to which the dots are arranged, the size of the dots and the interdot distance. It is shown that the ground state energy level can undergo significant variations when these parameters are modified. The results were obtained by means of finite difference method which has proved to be easily adaptable, efficient and precise. The symmetry properties of the lattice have been used to reduce the size of the Hamiltonian matrix.

Carbon-electroluminescence: An organic approach to lighting

NASA Astrophysics Data System (ADS)

Kumari, Sonali; Chaudhary, Tarun; Chandran, Vivek; Lokeshwari, M.; Shastry, K.

2018-05-01

Over the recent years, quantum dots have garnered massive following and peaked in interest among the scientific community due to their versatility, exotic properties, ease of preparation and low cost. As the demand for faster, reliable and energy efficient electronic devices intensifies, extra emphasis is laid on the development of smart materials capable of satiating this need. Electroluminescent organic quantum dots have emerged as one of the prime contenders in addressing the ecological, economic and technological constraints. Application of such luminescent nanoparticles as fluorescent light converters in LEDs is touted as one of the reliable and easiest avenues in realizing and developing newer energy efficient technologies for the next millennia. One promising candidate is zig-zag graphene quantum dots, which exhibits high electro-luminescence due to a phenomenon known as quantum confinement (where size of the nano-particle is of the same order or less than that of Bohr exciton radius). In this paper, we aim to provide a review of past and present research in the synthesis and development of luminescence using organic quantum dots.

Optoelectronic engineering of colloidal quantum-dot solar cells beyond the efficiency black hole: a modeling approach

NASA Astrophysics Data System (ADS)

Mahpeykar, Seyed Milad; Wang, Xihua

2017-02-01

Colloidal quantum dot (CQD) solar cells have been under the spotlight in recent years mainly due to their potential for low-cost solution-processed fabrication and efficient light harvesting through multiple exciton generation (MEG) and tunable absorption spectrum via the quantum size effect. Despite the impressive advances achieved in charge carrier mobility of quantum dot solids and the cells' light trapping capabilities, the recent progress in CQD solar cell efficiencies has been slow, leaving them behind other competing solar cell technologies. In this work, using comprehensive optoelectronic modeling and simulation, we demonstrate the presence of a strong efficiency loss mechanism, here called the "efficiency black hole", that can significantly hold back the improvements achieved by any efficiency enhancement strategy. We prove that this efficiency black hole is the result of sole focus on enhancement of either light absorption or charge extraction capabilities of CQD solar cells. This means that for a given thickness of CQD layer, improvements accomplished exclusively in optic or electronic aspect of CQD solar cells do not necessarily translate into tangible enhancement in their efficiency. The results suggest that in order for CQD solar cells to come out of the mentioned black hole, incorporation of an effective light trapping strategy and a high quality CQD film at the same time is an essential necessity. Using the developed optoelectronic model, the requirements for this incorporation approach and the expected efficiencies after its implementation are predicted as a roadmap for CQD solar cell research community.

GaN-based light emitting diodes using p-type trench structure for improving internal quantum efficiency

NASA Astrophysics Data System (ADS)

Kim, Garam; Sun, Min-Chul; Kim, Jang Hyun; Park, Euyhwan; Park, Byung-Gook

2017-01-01

In order to improve the internal quantum efficiency of GaN-based LEDs, a LED structure featuring a p-type trench in the multi-quantum well (MQW) is proposed. This structure has effects on spreading holes into the MQW and reducing the quantum-confined stark effect (QCSE). In addition, two simple fabrication methods using electron-beam (e-beam) lithography or selective wet etching for manufacturing the p-type structure are also proposed. From the measurement results of the manufactured GaN-based LEDs, it is confirmed that the proposed structure using e-beam lithography or selective wet etching shows improved light output power compared to the conventional structure because of more uniform hole distribution. It is also confirmed that the proposed structure formed by e-beam lithography has a significant effect on strain relaxation and reduction in the QCSE from the electro-luminescence measurement.

Efficiency of photochemical stages of photosynthesis in purple bacteria (a critical survey).

PubMed

Borisov, A Yu

2014-03-01

Based on currently available data, the energy transfer efficiency in the successive photophysical and photochemical stages has been analyzed for purple bacteria. This analysis covers the stages starting from migration of the light-induced electronic excitations from the bulk antenna pigments to the reaction centers up to irreversible stage of the electron transport along the transmembrane chain of cofactors-carriers. Some natural factors are revealed that significantly increase the rates of efficient processes in these stages. The influence on their efficiency by the "bottleneck" in the energy migration chain is established. The overall quantum yield of photosynthesis in these stages is determined.

Phonon Networks with Silicon-Vacancy Centers in Diamond Waveguides

NASA Astrophysics Data System (ADS)

Lemonde, M.-A.; Meesala, S.; Sipahigil, A.; Schuetz, M. J. A.; Lukin, M. D.; Loncar, M.; Rabl, P.

2018-05-01

We propose and analyze a novel realization of a solid-state quantum network, where separated silicon-vacancy centers are coupled via the phonon modes of a quasi-one-dimensional diamond waveguide. In our approach, quantum states encoded in long-lived electronic spin states can be converted into propagating phonon wave packets and be reabsorbed efficiently by a distant defect center. Our analysis shows that under realistic conditions, this approach enables the implementation of high-fidelity, scalable quantum communication protocols within chip-scale spin-qubit networks. Apart from quantum information processing, this setup constitutes a novel waveguide QED platform, where strong-coupling effects between solid-state defects and individual propagating phonons can be explored at the quantum level.

Phonon Networks with Silicon-Vacancy Centers in Diamond Waveguides.

PubMed

Lemonde, M-A; Meesala, S; Sipahigil, A; Schuetz, M J A; Lukin, M D; Loncar, M; Rabl, P

2018-05-25

We propose and analyze a novel realization of a solid-state quantum network, where separated silicon-vacancy centers are coupled via the phonon modes of a quasi-one-dimensional diamond waveguide. In our approach, quantum states encoded in long-lived electronic spin states can be converted into propagating phonon wave packets and be reabsorbed efficiently by a distant defect center. Our analysis shows that under realistic conditions, this approach enables the implementation of high-fidelity, scalable quantum communication protocols within chip-scale spin-qubit networks. Apart from quantum information processing, this setup constitutes a novel waveguide QED platform, where strong-coupling effects between solid-state defects and individual propagating phonons can be explored at the quantum level.

A multi-band, multi-level, multi-electron model for efficient FDTD simulations of electromagnetic interactions with semiconductor quantum wells

NASA Astrophysics Data System (ADS)

Ravi, Koustuban; Wang, Qian; Ho, Seng-Tiong

2015-08-01

We report a new computational model for simulations of electromagnetic interactions with semiconductor quantum well(s) (SQW) in complex electromagnetic geometries using the finite-difference time-domain method. The presented model is based on an approach of spanning a large number of electron transverse momentum states in each SQW sub-band (multi-band) with a small number of discrete multi-electron states (multi-level, multi-electron). This enables accurate and efficient two-dimensional (2-D) and three-dimensional (3-D) simulations of nanophotonic devices with SQW active media. The model includes the following features: (1) Optically induced interband transitions between various SQW conduction and heavy-hole or light-hole sub-bands are considered. (2) Novel intra sub-band and inter sub-band transition terms are derived to thermalize the electron and hole occupational distributions to the correct Fermi-Dirac distributions. (3) The terms in (2) result in an explicit update scheme which circumvents numerically cumbersome iterative procedures. This significantly augments computational efficiency. (4) Explicit update terms to account for carrier leakage to unconfined states are derived, which thermalize the bulk and SQW populations to a common quasi-equilibrium Fermi-Dirac distribution. (5) Auger recombination and intervalence band absorption are included. The model is validated by comparisons to analytic band-filling calculations, simulations of SQW optical gain spectra, and photonic crystal lasers.

Effect of photoanode surface coverage by a sensitizer on the photovoltaic performance of titania based CdS quantum dot sensitized solar cells.

PubMed

Prasad, Rajendra M B; Pathan, Habib M

2016-04-08

In spite of the promising design and architecture, quantum dot sensitized solar cells (QDSSCs) have a long way to go before they attain the actual projected photoconversion efficiencies. Such an inferior performance displayed by QDSSCs is primarily because of many unwanted recombination losses of charge carriers at various interfaces of the cell. Electron recombination due to back electron transfer at the photoanode/electrolyte interface is an important one that needs to be addressed, to improve the efficiency of these third generation nanostructured solar cells. The present work highlights the importance of conformal coverage of CdS quantum dots (QDs) on the surface of the nanocrystalline titania photoanode in arresting such recombinations, leading to improvement in the performance of the cells. Using the successive ionic layer adsorption and reaction (SILAR) process, photoanodes are subjected to different amounts of CdS QD sensitization by varying the number of cycles of deposition. The sensitized electrodes are characterized using UV-visible spectroscopy, cyclic voltammetry and transmission electron microscopy to evaluate the extent of surface coverage of titania electrodes by QDs. Sandwich solar cells are then fabricated using these electrodes and characterized employing electrochemical impedance spectroscopy and J-V characteristics. It is observed that maximum solar cell efficiency is obtained for photoanodes with conformal coating of QDs and any further deposition of sensitizer leads to QD aggregation and so reduces the performance of the solar cells.

Highly efficient single-layer dendrimer light-emitting diodes with balanced charge transport

NASA Astrophysics Data System (ADS)

Anthopoulos, Thomas D.; Markham, Jonathan P. J.; Namdas, Ebinazar B.; Samuel, Ifor D. W.; Lo, Shih-Chun; Burn, Paul L.

2003-06-01

High-efficiency single-layer-solution-processed green light-emitting diodes based on a phosphorescent dendrimer are demonstrated. A peak external quantum efficiency of 10.4% (35 cd/A) was measured for a first generation fac-tris(2-phenylpyridine) iridium cored dendrimer when blended with 4,4'-bis(N-carbazolyl)biphenyl and electron transporting 1,3,5-tris(2-N-phenylbenzimidazolyl)benzene at 8.1 V. A maximum power efficiency of 12.8 lm/W was measured also at 8.1 V and 550 cd/m2. These results indicate that, by simple blending of bipolar and electron-transporting molecules, highly efficient light-emitting diodes can be made employing a very simple device structure.

Emulation of complex open quantum systems using superconducting qubits

NASA Astrophysics Data System (ADS)

Mostame, Sarah; Huh, Joonsuk; Kreisbeck, Christoph; Kerman, Andrew J.; Fujita, Takatoshi; Eisfeld, Alexander; Aspuru-Guzik, Alán

2017-02-01

With quantum computers being out of reach for now, quantum simulators are alternative devices for efficient and accurate simulation of problems that are challenging to tackle using conventional computers. Quantum simulators are classified into analog and digital, with the possibility of constructing "hybrid" simulators by combining both techniques. Here we focus on analog quantum simulators of open quantum systems and address the limit that they can beat classical computers. In particular, as an example, we discuss simulation of the chlorosome light-harvesting antenna from green sulfur bacteria with over 250 phonon modes coupled to each electronic state. Furthermore, we propose physical setups that can be used to reproduce the quantum dynamics of a standard and multiple-mode Holstein model. The proposed scheme is based on currently available technology of superconducting circuits consist of flux qubits and quantum oscillators.

High-efficiency optical pumping of nuclear polarization in a GaAs quantum well

NASA Astrophysics Data System (ADS)

Mocek, R. W.; Korenev, V. L.; Bayer, M.; Kotur, M.; Dzhioev, R. I.; Tolmachev, D. O.; Cascio, G.; Kavokin, K. V.; Suter, D.

2017-11-01

The dynamic polarization of nuclear spins by photoexcited electrons is studied in a high quality GaAs/AlGaAs quantum well. We find a surprisingly high efficiency of the spin transfer from the electrons to the nuclei as reflected by a maximum nuclear field of 0.9 T in a tilted external magnetic field of 1 T strength only. This high efficiency is due to a low leakage of spin out of the polarized nuclear system, because mechanisms of spin relaxation other than the hyperfine interaction are strongly suppressed, leading to a long nuclear relaxation time of up to 1000 s. A key ingredient to that end is the low impurity concentration inside the heterostructure, while the electrostatic potential from charged impurities in the surrounding barriers becomes screened through illumination by which the spin relaxation time is increased compared to keeping the system in the dark. This finding indicates a strategy for obtaining high nuclear spin polarization as required for long-lasting carrier spin coherence.

Optical Manifestations of the Electron-Electron Interaction

NASA Astrophysics Data System (ADS)

Portengen, Taco

1995-01-01

In this thesis, two optical manifestations of the electron-electron interaction are studied: the Fermi -edge singularity in doped quantum wells and quantum wires, and second-harmonic generation in mixed-valent compounds. First, we construct a theory of the Fermi-edge singularity that can systematically account for the finite mass of a hole created in the valence subband of a quantum well or quantum wire. The dynamical response for finite hole mass depends crucially on the dimensionality of the Fermi sea. Whereas in three dimensions the infrared divergence is suppressed, in two dimensions a one-over-square-root singularity survives, while in one dimension the spectrum is even more singular with recoil than without recoil. This explains the large optical singularities observed in quantum wires. Correlations change the prefactor, but not the exponent of the threshold behaviour in two and in three dimensions, while in one dimension, they affect neither the prefactor nor the exponent. Second, we apply our theory to the Frohlich polaron, a manifestation of the electron-phonon rather than the electron-electron interaction. The new method of calculating the Green's function removes unphysical features of the conventional cumulant expansion that had remained unnoticed in the literature up to now. Third, in an effort to investigate the impact of coherence on optical properties, we calculate the linear and nonlinear optical characteristics of mixed-valent compounds. Second -harmonic generation can only occur for solutions of the theoretical Falicov-Kimball model that have a built-in coherence between the itinerant d-electrons and localized f-holes. By contrast, second-harmonic generation cannot occur for solutions with f-site occupation as a good quantum number. The interaction between optically created quasiparticles leads to a threshold singularity in the absorption spectrum, and greatly enhances the second-harmonic conversion efficiency at half the gap frequency. As an experimental test of coherence we propose the measurement of the second-harmonic susceptibility of SmB_6..

Quantum wavepacket ab initio molecular dynamics: an approach for computing dynamically averaged vibrational spectra including critical nuclear quantum effects.

PubMed

Sumner, Isaiah; Iyengar, Srinivasan S

2007-10-18

We have introduced a computational methodology to study vibrational spectroscopy in clusters inclusive of critical nuclear quantum effects. This approach is based on the recently developed quantum wavepacket ab initio molecular dynamics method that combines quantum wavepacket dynamics with ab initio molecular dynamics. The computational efficiency of the dynamical procedure is drastically improved (by several orders of magnitude) through the utilization of wavelet-based techniques combined with the previously introduced time-dependent deterministic sampling procedure measure to achieve stable, picosecond length, quantum-classical dynamics of electrons and nuclei in clusters. The dynamical information is employed to construct a novel cumulative flux/velocity correlation function, where the wavepacket flux from the quantized particle is combined with classical nuclear velocities to obtain the vibrational density of states. The approach is demonstrated by computing the vibrational density of states of [Cl-H-Cl]-, inclusive of critical quantum nuclear effects, and our results are in good agreement with experiment. A general hierarchical procedure is also provided, based on electronic structure harmonic frequencies, classical ab initio molecular dynamics, computation of nuclear quantum-mechanical eigenstates, and employing quantum wavepacket ab initio dynamics to understand vibrational spectroscopy in hydrogen-bonded clusters that display large degrees of anharmonicities.

Quantum Phenomena in High Energy Density Plasmas

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

Murnane, Margaret; Kapteyn, Henry

The possibility of implementing efficient (phase matched) HHG upconversion of deep- UV lasers in multiply-ionized plasmas, with potentially unprecedented conversion efficiency is a fascinating prospect. HHG results from the extreme nonlinear response of matter to intense laser light:high harmonics are radiated as a result of a quantum coherent electron recollision process that occurs during laser field ionization of an atom. Under current support from this grant in work published in Science in 2015, we discovered a new regime of bright HHG in highly-ionized plasmas driven by intense UV lasers, that generates bright harmonics to photon energies >280eV

Improved Signal Control: An Analysis of the Effects of Automatic Gain Control for Optical Signal Detection.

DTIC Science & Technology

1982-12-01

period f T - switching period a - AGC control parameter q - quantum efficiency of photon to electron conversions "I - binary "one" given in terms of the...of the photons striking the surface of the detector. This rate is defined as: X(t) = (np(t)A) / hf 0 (21) where n - quantum efficiency of the photon...mw to 10 mw [Ref 5, Table 1] for infrared wavelengths. 30 Assuming all of the source’s output power is detected, the rate is calculated to be an order

Tuning charge balance in PHOLEDs with ambipolar host materials to achieve high efficiency

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

Padmaperuma, Asanga B.; Koech, Phillip K.; Cosimbescu, Lelia

2009-08-27

The efficiency and stability of blue organic light emitting devices (OLEDs) continue to be a primary roadblock to developing organic solid state white lighting. For OLEDs to meet the high power conversion efficiency goal, they will require both close to 100% internal quantum efficiency and low operating voltage in a white light emitting device.1 It is generally accepted that such high quantum efficiency, can only be achieved with the use of organometallic phosphor doped OLEDs. Blue OLEDs are particularly important for solid state lighting. The simplest (and therefore likely the lowest cost) method of generating white light is to downmore » convert part of the emission from a blue light source with a system of external phosphors.2 A second method of generating white light requires the superposition of the light from red, green and blue OLEDs in the correct ratio. Either of these two methods (and indeed any method of generating white light with a high color rendering index) critically depends on a high efficiency blue light component.3 A simple OLED generally consists of a hole-injecting anode, a preferentially hole transporting organic layer (HTL), an emissive layer that contains the recombination zone and ideally transports both holes and electrons, a preferentially electron-transporting layer (ETL) and an electron-injecting cathode. Color in state-of-the-art OLEDs is generated by an organometallic phosphor incorporated by co-sublimation into the emissive layer (EML).4 New materials functioning as hosts, emitters, charge transporting, and charge blocking layers have been developed along with device architectures leading to electrophosphorescent based OLEDs with high quantum efficiencies near the theoretical limit. However, the layers added to the device architecture to enable high quantum efficiencies lead to higher operating voltages and correspondingly lower power efficiencies. Achievement of target luminance power efficiencies will require new strategies for lowering operating voltages, particularly if this is to be achieved in a device that can be manufactured at low cost. To avoid the efficiency losses associated with phosphorescence quenching by back-energy transfer from the dopant onto the host, the triplet excited states of the host material must be higher in energy than the triplet excited state of the dopant.5 This must be accomplished without sacrificing the charge transporting properties of the composite.6 Similar problems limit the efficiency of OLED-based displays, where blue light emitters are the least efficient and least stable. We previously demonstrated the utility of organic phosphine oxide (PO) materials as electron transporting HMs for FIrpic in blue OLEDs.7 However, the high reluctance of PO materials to oxidation and thus, hole injection limits the ability to balance charge injection and transport in the EML without relying on charge transport by the phosphorescent dopant. PO host materials were engineered to transport both electrons and holes in the EML and still maintain high triplet exciton energy to ensure efficient energy transfer to the dopant (Figure 1). There are examples of combining hole transporting moieties (mainly aromatic amines) with electron transport moieties (e.g., oxadiazoles, triazines, boranes)8 to develop new emitter and host materials for small molecule and polymer9 OLEDs. The challenge is to combine the two moieties without lowering the triplet energy of the target molecule. For example, coupling of a dimesitylphenylboryl moiety with a tertiary aromatic amine (FIAMBOT) results in intramolecular electron transfer from the amine to the boron atom through the bridging phenyl. The mesomeric effect of the dimesitylphenylboryl unit acts to extend conjugation and lowers triplet exciton energies (< 2.8 eV) rendering such systems inadequate as ambipolar hosts for blue phosphors.« less

Reversible Quantum Brownian Heat Engines for Electrons

NASA Astrophysics Data System (ADS)

Humphrey, T. E.; Newbury, R.; Taylor, R. P.; Linke, H.

2002-08-01

Brownian heat engines use local temperature gradients in asymmetric potentials to move particles against an external force. The energy efficiency of such machines is generally limited by irreversible heat flow carried by particles that make contact with different heat baths. Here we show that, by using a suitably chosen energy filter, electrons can be transferred reversibly between reservoirs that have different temperatures and electrochemical potentials. We apply this result to propose heat engines based on mesoscopic semiconductor ratchets, which can quasistatically operate arbitrarily close to Carnot efficiency.

Efficiency improvement of green light-emitting diodes by employing all-quaternary active region and electron-blocking layer

NASA Astrophysics Data System (ADS)

Usman, Muhammad; Saba, Kiran; Han, Dong-Pyo; Muhammad, Nazeer

2018-01-01

High efficiency of green GaAlInN-based light-emitting diode (LED) has been proposed with peak emission wavelength of ∼510 nm. By introducing quaternary quantum well (QW) along with the quaternary barrier (QB) and quaternary electron blocking layer (EBL) in a single structure, an efficiency droop reduction of up to 29% has been achieved in comparison to the conventional GaN-based LED. The proposed structure has significantly reduced electrostatic field in the active region. As a result, carrier leakage has been minimized and spontaneous emission rate has been doubled.

High Color-Purity Green, Orange, and Red Light-Emitting Didoes Based on Chemically Functionalized Graphene Quantum Dots

NASA Astrophysics Data System (ADS)

Kwon, Woosung; Kim, Young-Hoon; Kim, Ji-Hee; Lee, Taehyung; Do, Sungan; Park, Yoonsang; Jeong, Mun Seok; Lee, Tae-Woo; Rhee, Shi-Woo

2016-04-01

Chemically derived graphene quantum dots (GQDs) to date have showed very broad emission linewidth due to many kinds of chemical bondings with different energy levels, which significantly degrades the color purity and color tunability. Here, we show that use of aniline derivatives to chemically functionalize GQDs generates new extrinsic energy levels that lead to photoluminescence of very narrow linewidths. We use transient absorption and time-resolved photoluminescence spectroscopies to study the electronic structures and related electronic transitions of our GQDs, which reveals that their underlying carrier dynamics is strongly related to the chemical properties of aniline derivatives. Using these functionalized GQDs as lumophores, we fabricate light-emitting didoes (LEDs) that exhibit green, orange, and red electroluminescence that has high color purity. The maximum current efficiency of 3.47 cd A-1 and external quantum efficiency of 1.28% are recorded with our LEDs; these are the highest values ever reported for LEDs based on carbon-nanoparticle phosphors. This functionalization of GQDs with aniline derivatives represents a new method to fabricate LEDs that produce natural color.

Canadian Semiconductor Technology Conference, 6th, Ottawa, Canada, Aug. 11-13, 1992, Proceedings

NASA Astrophysics Data System (ADS)

Baribeau, Jean-Marc

1992-11-01

This volume contains papers on the growth efficiency and distribution coefficient of GaInP-InP epilayers and heterostructures, X-ray photoelectron spectroscopy studies of Ge epilayers on Si(100), and mechanical properties of silicon carbide films for X-ray lithography application. Attention is also given to fine structure in Raman spectroscopy and X-ray reflectometry and its uses for the characterization of superlattices, phase formation in Fe-Si thin-film diffusion couples, process optimization for a micromachined silicon nonreverse valve, and a numerical study of heat transport in thermally isolated flow-rate microsensors. Particular consideration is given to a versatile 2D model for InGaAsP quantum-well semiconductor lasers, gallium arsenide electronics in the marketplace, and optical channel grading in p-type Si/SiGe MOSFETs. Other papers are on ultrafast electron tunneling in a reverse-biased high-efficiency quantum well laser structure, excess currents as a result of trap-assisted tunneling in double-barrier resonant tunneling diodes, and carrier lifetimes in strained InGaAsP multiple quantum-well laser structures.

Increasing the efficiency and accuracy of time-resolved electronic spectra calculations with on-the-fly ab initio quantum dynamics methods

NASA Astrophysics Data System (ADS)

Vanicek, Jiri

2014-03-01

Rigorous quantum-mechanical calculations of coherent ultrafast electronic spectra remain difficult. I will present several approaches developed in our group that increase the efficiency and accuracy of such calculations: First, we justified the feasibility of evaluating time-resolved spectra of large systems by proving that the number of trajectories needed for convergence of the semiclassical dephasing representation/phase averaging is independent of dimensionality. Recently, we further accelerated this approximation with a cellular scheme employing inverse Weierstrass transform and optimal scaling of the cell size. The accuracy of potential energy surfaces was increased by combining the dephasing representation with accurate on-the-fly ab initio electronic structure calculations, including nonadiabatic and spin-orbit couplings. Finally, the inherent semiclassical approximation was removed in the exact quantum Gaussian dephasing representation, in which semiclassical trajectories are replaced by communicating frozen Gaussian basis functions evolving classically with an average Hamiltonian. Among other examples I will present an on-the-fly ab initio semiclassical dynamics calculation of the dispersed time-resolved stimulated emission spectrum of the 54-dimensional azulene. This research was supported by EPFL and by the Swiss National Science Foundation NCCR MUST (Molecular Ultrafast Science and Technology) and Grant No. 200021124936/1.

Time-Dependent Density Functional Theory for Open Systems and Its Applications.

PubMed

Chen, Shuguang; Kwok, YanHo; Chen, GuanHua

2018-02-20

Photovoltaic devices, electrochemical cells, catalysis processes, light emitting diodes, scanning tunneling microscopes, molecular electronics, and related devices have one thing in common: open quantum systems where energy and matter are not conserved. Traditionally quantum chemistry is confined to isolated and closed systems, while quantum dissipation theory studies open quantum systems. The key quantity in quantum dissipation theory is the reduced system density matrix. As the reduced system density matrix is an O(M! × M!) matrix, where M is the number of the particles of the system of interest, quantum dissipation theory can only be employed to simulate systems of a few particles or degrees of freedom. It is thus important to combine quantum chemistry and quantum dissipation theory so that realistic open quantum systems can be simulated from first-principles. We have developed a first-principles method to simulate the dynamics of open electronic systems, the time-dependent density functional theory for open systems (TDDFT-OS). Instead of the reduced system density matrix, the key quantity is the reduced single-electron density matrix, which is an N × N matrix where N is the number of the atomic bases of the system of interest. As the dimension of the key quantity is drastically reduced, the TDDFT-OS can thus be used to simulate the dynamics of realistic open electronic systems and efficient numerical algorithms have been developed. As an application, we apply the method to study how quantum interference develops in a molecular transistor in time domain. We include electron-phonon interaction in our simulation and show that quantum interference in the given system is robust against nuclear vibration not only in the steady state but also in the transient dynamics. As another application, by combining TDDFT-OS with Ehrenfest dynamics, we study current-induced dissociation of water molecules under scanning tunneling microscopy and follow its time dependent dynamics. Given the rapid development in ultrafast experiments with atomic resolution in recent years, time dependent simulation of open electronic systems will be useful to gain insight and understanding of such experiments. This Account will mainly focus on the practical aspects of the TDDFT-OS method, describing the numerical implementation and demonstrating the method with applications.

A new route for degradation of volatile organic compounds under visible light: using the bifunctional photocatalyst Pt/TiO2-xNx in H2-O2 atmosphere.

PubMed

Li, Danzhen; Chen, Zhixin; Chen, Yilin; Li, Wenjuan; Huang, Hanjie; He, Yunhui; Fu, Xianzhi

2008-03-15

The bifunctional photocatalyst Pt/TiO2-xNx has been successfully prepared by wet impregnation. The properties of Pt/ TiO2-xNx have been investigated by diffuse reflectance spectra, X-ray diffraction, transmission electron microscopy, X-ray photoelectron spectroscopy, a photoluminescence technique with terephthalic acid, and electric field induced surface photovoltage spectra. The photocatalytic activity of the sample was evaluated by the decomposition of volatile organic pollutants (VOCs) in a H2-O2 atmosphere under visible light irradiation. The results demonstrated that nitrogen-doped and platinum-modified TiO2 in a H2-O2 atmosphere could enormously increase the quantum efficiency of the photocatalytic system with excellent photocatalytic activity and high catalytic stability. The increased quantum efficiency can be explained by enhanced separation efficiency of photogenerated electron-hole pairs, higher interface electron transfer rate, and an increased number of surface hydroxyl radicals in the photocatalytic process. A mechanism was proposed to elucidate the degradation of VOCs over PtTiO(2-x)Nx in a H2-O2 atmosphere under visible light irradiation.

Coexistence of perfect spin filtering for entangled electron pairs and high magnetic storage efficiency in one setup.

PubMed

Ji, T T; Bu, N; Chen, F J; Tao, Y C; Wang, J

2016-04-14

For Entangled electron pairs superconducting spintronics, there exist two drawbacks in existing proposals of generating entangled electron pairs. One is that the two kinds of different spin entangled electron pairs mix with each other. And the other is a low efficiency of entanglement production. Herein, we report the spin entanglement state of the ferromagnetic insulator (FI)/s-wave superconductor/FI structure on a narrow quantum spin Hall insulator strip. It is shown that not only the high production of entangled electron pairs in wider energy range, but also the perfect spin filtering of entangled electron pairs in the context of no highly spin-polarized electrons, can be obtained. Moreover, the currents for the left and right leads in the antiferromagnetic alignment both can be zero, indicating 100% tunnelling magnetoresistance with highly magnetic storage efficiency. Therefore, the spin filtering for entangled electron pairs and magnetic storage with high efficiencies coexist in one setup. The results may be experimentally demonstrated by measuring the tunnelling conductance and the noise power.

Enhanced Internal Quantum Efficiency in Dye-Sensitized Solar Cells: Effect of Long-Lived Charge-Separated State of Sensitizers.

PubMed

Sun, Haiya; Liu, Dongzhi; Wang, Tianyang; Lu, Ting; Li, Wei; Ren, Siyao; Hu, Wenping; Wang, Lichang; Zhou, Xueqin

2017-03-22

Effective charge separation is one of the key determinants for the photovoltaic performance of the dye-sensitized solar cells (DSSCs). Herein, two charge-separated (CS) sensitizers, MTPA-Pyc and YD-Pyc, have been synthesized and applied in DSSCs to investigate the effect of the CS states of the sensitizers on the device's efficiency. The CS states with lifetimes of 64 and 177 ns for MTPA-Pyc and YD-Pyc, respectively, are formed via the photoinduced electron transfer (PET) from the 4-styryltriphenylamine (MTPA) or 4-styrylindoline (YD) donor to the pyrimidine cyanoacrylic acid (Pyc) acceptor. DSSCs based on MTPA-Pyc and YD-Pyc exhibit high internal quantum efficiency (IQE) values of over 80% from 400 to 600 nm. In comparison, the IQEs of the charge transfer (CT) sensitizer cells are 10-30% lower in the same wavelength range. The enhanced IQE values in the devices based on the CS sensitizers are ascribed to the higher electron injection efficiencies and slower charge recombination. The results demonstrate that taking advantage of the CS states in the sensitizers can be a promising strategy to improve the IQEs and further enhance the overall efficiencies of the DSSCs.

Homojunction GaAs solar cells grown by close space vapor transport

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

Boucher, Jason W.; Ritenour, Andrew J.; Greenaway, Ann L.

2014-06-08

We report on the first pn junction solar cells grown by homoepitaxy of GaAs using close space vapor transport (CSVT). Cells were grown both on commercial wafer substrates and on a CSVT absorber film, and had efficiencies reaching 8.1%, open circuit voltages reaching 909 mV, and internal quantum efficiency of 90%. The performance of these cells is partly limited by the electron diffusion lengths in the wafer substrates, as evidenced by the improved peak internal quantum efficiency in devices fabricated on a CSVT absorber film. Unoptimized highly-doped n-type emitters also limit the photocurrent, indicating that thinner emitters with reduced doping,more » and ultimately wider band gap window or surface passivation layers, are required to increase the efficiency.« less

Enhanced thermoelectric response in the fractional quantum Hall effect

NASA Astrophysics Data System (ADS)

Roura-Bas, Pablo; Arrachea, Liliana; Fradkin, Eduardo

2018-02-01

We study the linear thermoelectric response of a quantum dot embedded in a constriction of a quantum Hall bar with fractional filling factors ν =1 /m within Laughlin series. We calculate the figure of merit Z T for the maximum efficiency at a fixed temperature difference. We find a significant enhancement of this quantity in the fractional filling in relation to the integer-filling case, which is a direct consequence of the fractionalization of the electron in the fractional quantum Hall state. We present simple theoretical expressions for the Onsager coefficients at low temperatures, which explicitly show that Z T and the Seebeck coefficient increase with m .

Synthesis, characterization and photovoltaic performance of Mn-doped ZnS quantum dots- P3HT hybrid bulk heterojunction solar cells

NASA Astrophysics Data System (ADS)

Jabeen, Uzma; Adhikari, Tham; Shah, Syed Mujtaba; Pathak, Dinesh; Nunzi, Jean-Michel

2017-11-01

Zinc sulphide (ZnS) and transition metal-doped ZnS nanocrystals were synthesized by co-precipitation method. Further the synthesized nanocrystals were characterized by Field Emission Scanning Electron Microscope (FESEM), High Resolution Transmission Electron Microscope (HRTEM), Fluorescence, UV-Visible, X-ray diffraction (XRD) and Fourier Transformed Infra-red (FTIR) Spectrometer (FTIR). Scanning electron microscope supplemented with EDAX was employed to attain grain size and chemical composition of the nanomaterials. A considerable blue shift of absorption band was noted by the manganese concentration (0.5 M) in the doped sample in comparison with ZnS quantum dots because of the decrease in the size of nanoparticles which may be due to quantum confinement. The photoluminescence emission observed at 596 nm is due to the emission of divalent manganese and can be ascribed to a 4T1→6A1 transition within the 3d shell. Though, the broad blue emission band was observed at 424 nm which may originates from the radiative recombination comprising defect states in the un-doped zinc sulphide quantum dots. XRD analysis exhibited that the synthesized nanomaterial endured in cubic structure. The synthesized nanomaterial combined with organic polymer P3HT, poly (3-hexyl thiophene) and worked in the construction of inverted solar cells. The photovoltaic devices with un-doped zinc sulphide quantum dots showed power conversion efficiency of 0.48% without annealing and 0.52% with annealing. By doping with manganese, the efficiency was enhanced by a factor of 0.52 without annealing and 0.59 with annealing. The morphology and packing behavior of blend of nanocrystals with organic polymer were explored using Atomic Force Microscopy.

Engineering of lead chalcogenide nanostructures for carrier multiplication: Core/shell, 1D, and 2D

NASA Astrophysics Data System (ADS)

Lin, Qianglu

Near infrared emitting semiconductors have been used widely in industry especially in solar-cell fabrications. The efficiency of single junction solar-cell can reach the Shockley-Queisser limit by using optimum band gap material such as silicon and cadmium telluride. The theoretical efficiency can be further enhanced through carrier multiplication, in which a high energy photon is absorbed and more than one electron-hole pair can be generated, reaching more than 100% quantum efficiency in the high energy region of sunlight. The realization of more than unity external quantum efficiency in lead selenide quantum dots solar cell has motivated vast investigation on lowering the carrier multiplication threshold and further improving the efficiency. This dissertation focuses on synthesis of lead chalcogenide nanostructures for their optical spectroscopy studies. PbSe/CdSe core/shell quantum dots were synthesized by cation exchange to obtain thick shells (up to 14 monolayers) for studies of visible and near infrared dual band emissions and carrier multiplication efficiency. By examining the reaction mechanism, a thermodynamic and a kinetic model are introduced to explain the vacancy driven cation exchange. As indicated by the effective mass model, PbSe/CdSe core/shell quantum dots has quasi-type-II band alignment, possessing electron delocalized through the entire quantum dot and hole localized in the core, which breaks down the symmetry of energy levels in the conduction and valence band, leading to hot-hole-assisted efficient multi-exciton generation and a lower carrier multiplication threshold to the theoretical value. For further investigation of carrier multiplication study, PbTe, possessing the highest efficiency among lead chalcogenides due to slow intraband cooling, is synthesized in one-dimensional and two-dimensional nanostructures. By using dodecanethiol as the surfactant, PbTe NRs can be prepared with high uniformity in width and resulted in fine quantum confinement features. The reaction can be explained by a soft-template assisted process, in which the lamellar lead-thiolate precursor transforms into rod-shape micelle in the existence of telluride anions by electrostatic attraction. Fine tuning the reaction condition by changing the solvent to oleylamine, lead telluride nanowires with length up to 200 nm can be prepared, which bundled together because of the strong dipole-dipole attraction between nanowires. Decreasing the amount of surfactant dodecanethiol in the synthesis produces lead telluride nanorings, which formed by attaching four small particles together, leaving the center void. To prepare two-dimensional nanoplatelets, mixture ligands containing two amines with different carbon chain length were used, which initiate oriented attachment of the nanoparticles to form square-shape nanoplatelets. By further adopting stronger binding ligands such as phosphonic acid, PbTe nanoplatelets with micrometer lateral dimension were prepared with extremely sharp near infrared photoluminescence (less than 40 meV), which has never be achieved in quantum dots and other nanostructures.

Electron Dynamics in Finite Quantum Systems

NASA Astrophysics Data System (ADS)

McDonald, Christopher R.

The multiconfiguration time-dependent Hartree-Fock (MCTDHF) and multiconfiguration time-dependent Hartree (MCTDH) methods are employed to investigate nonperturbative multielectron dynamics in finite quantum systems. MCTDHF is a powerful tool that allows for the investigation of multielectron dynamics in strongly perturbed quantum systems. We have developed an MCTDHF code that is capable of treating problems involving three dimensional (3D) atoms and molecules exposed to strong laser fields. This code will allow for the theoretical treatment of multielectron phenomena in attosecond science that were previously inaccessible. These problems include complex ionization processes in pump-probe experiments on noble gas atoms, the nonlinear effects that have been observed in Ne atoms in the presence of an x-ray free-electron laser (XFEL) and the molecular rearrangement of cations after ionization. An implementation of MCTDH that is optimized for two electrons, each moving in two dimensions (2D), is also presented. This implementation of MCTDH allows for the efficient treatment of 2D spin-free systems involving two electrons; however, it does not scale well to 3D or to systems containing more that two electrons. Both MCTDHF and MCTDH were used to treat 2D problems in nanophysics and attosecond science. MCTDHF is used to investigate plasmon dynamics and the quantum breathing mode for several electrons in finite lateral quantum dots. MCTDHF is also used to study the effects of manipulating the potential of a double lateral quantum dot containing two electrons; applications to quantum computing are discussed. MCTDH is used to examine a diatomic model molecular system exposed to a strong laser field; nonsequential double ionization and high harmonic generation are studied and new processes identified and explained. An implementation of MCTDHF is developed for nonuniform tensor product grids; this will allow for the full 3D implementation of MCTDHF and will provide a means to investigate a wide variety of problems that cannot be currently treated by any other method. Finally, the time it takes for an electron to tunnel from a bound state is investigated; a definition of the tunnel time is established and the Keldysh time is connected to the wavefunction dynamics.

International Workshop on Light Emission and Electronic Properties of Nanoscale Silicon

DTIC Science & Technology

1994-04-01

matrix elements, quantum confinement, surface effects ? CHARLOTFE STANDARD R. Tsu Comparison of Luminescence Efficiency ROLE OF NANOSCALE Si-DEVICES...confinement effects in microcrystalline silicon [2,3] may lead to revolutionary advances in speed and dramatically reduced energy consumption of silicon...Formation: A Quantum Wire Effect ," Avpl. Phys. Lett., 58, 856 (1991). 5. R. Tsu, H. Shen, and M. Dutta, "Correlation of Raman and Photoluminescence

InAs/GaAs p-type quantum dot infrared photodetector with higher efficiency

NASA Astrophysics Data System (ADS)

Lao, Yan-Feng; Wolde, Seyoum; Unil Perera, A. G.; Zhang, Y. H.; Wang, T. M.; Liu, H. C.; Kim, J. O.; Schuler-Sandy, Ted; Tian, Zhao-Bing; Krishna, S. S.

2013-12-01

An InAs/GaAs quantum dot infrared photodetector (QDIP) based on p-type valence-band intersublevel hole transitions as opposed to conventional electron transitions is reported. Two response bands observed at 1.5-3 and 3-10 μm are due to transitions from the heavy-hole to spin-orbit split-off QD level and from the heavy-hole to heavy-hole level, respectively. Without employing optimized structures (e.g., the dark current blocking layer), the demonstrated QDIP displays promising characteristics, including a specific detectivity of 1.8×109 cm.Hz1/2/W and a quantum efficiency of 17%, which is about 5% higher than that of present n-type QDIPs. This study shows the promise of utilizing hole transitions for developing QDIPs.

Harvesting dissipated energy with a mesoscopic ratchet

NASA Astrophysics Data System (ADS)

Roche, B.; Roulleau, P.; Jullien, T.; Jompol, Y.; Farrer, I.; Ritchie, D. A.; Glattli, D. C.

2015-04-01

The search for new efficient thermoelectric devices converting waste heat into electrical energy is of major importance. The physics of mesoscopic electronic transport offers the possibility to develop a new generation of nanoengines with high efficiency. Here we describe an all-electrical heat engine harvesting and converting dissipated power into an electrical current. Two capacitively coupled mesoscopic conductors realized in a two-dimensional conductor form the hot source and the cold converter of our device. In the former, controlled Joule heating generated by a voltage-biased quantum point contact results in thermal voltage fluctuations. By capacitive coupling the latter creates electric potential fluctuations in a cold chaotic cavity connected to external leads by two quantum point contacts. For unequal quantum point contact transmissions, a net electrical current is observed proportional to the heat produced.

Novel multistep BRET-FRET energy transfer using nanoconjugates of firefly proteins, quantum dots, and red fluorescent proteins

NASA Astrophysics Data System (ADS)

Alam, Rabeka; Zylstra, Joshua; Fontaine, Danielle M.; Branchini, Bruce R.; Maye, Mathew M.

2013-05-01

Sequential bioluminescence resonance energy transfer (BRET) and fluorescence resonance energy transfer (FRET) from firefly luciferase to red fluorescent proteins using quantum dot or rod acceptor/donor linkers is described. The effect of morphology and tuned optical properties on the efficiency of this unique BRET-FRET system was evaluated.Sequential bioluminescence resonance energy transfer (BRET) and fluorescence resonance energy transfer (FRET) from firefly luciferase to red fluorescent proteins using quantum dot or rod acceptor/donor linkers is described. The effect of morphology and tuned optical properties on the efficiency of this unique BRET-FRET system was evaluated. Electronic supplementary information (ESI) available: Experimental details, Fig. S1 and Table S1-S4. See DOI: 10.1039/c3nr01842c

Non-Markovian Quantum State Diffusion for temperature-dependent linear spectra of light harvesting aggregates

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

Ritschel, Gerhard; Möbius, Sebastian; Eisfeld, Alexander, E-mail: eisfeld@mpipks-dresden.mpg.de

2015-01-21

Non-Markovian Quantum State Diffusion (NMQSD) has turned out to be an efficient method to calculate excitonic properties of aggregates composed of organic chromophores, taking into account the coupling of electronic transitions to vibrational modes of the chromophores. NMQSD is an open quantum system approach that incorporates environmental degrees of freedom (the vibrations in our case) in a stochastic way. We show in this paper that for linear optical spectra (absorption, circular dichroism), no stochastics is needed, even for finite temperatures. Thus, the spectra can be obtained by propagating a single trajectory. To this end, we map a finite temperature environmentmore » to the zero temperature case using the so-called thermofield method. The resulting equations can then be solved efficiently by standard integrators.« less

Nuclear spin cooling by electric dipole spin resonance and coherent population trapping

NASA Astrophysics Data System (ADS)

Li, Ai-Xian; Duan, Su-Qing; Zhang, Wei

2017-09-01

Nuclear spin fluctuation suppression is a key issue in preserving electron coherence for quantum information/computation. We propose an efficient way of nuclear spin cooling in semiconductor quantum dots (QDs) by the coherent population trapping (CPT) and the electric dipole spin resonance (EDSR) induced by optical fields and ac electric fields. The EDSR can enhance the spin flip-flop rate and may bring out bistability under certain conditions. By tuning the optical fields, we can avoid the EDSR induced bistability and obtain highly polarized nuclear spin state, which results in long electron coherence time. With the help of CPT and EDSR, an enhancement of 1500 times of the electron coherence time can been obtained after a 500 ns preparation time.

InGaAs/GaAsP strain balanced multi-quantum wires grown on misoriented GaAs substrates for high efficiency solar cells

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

Alonso-Álvarez, D.; Thomas, T.; Führer, M.

Quantum wires (QWRs) form naturally when growing strain balanced InGaAs/GaAsP multi-quantum wells (MQW) on GaAs [100] 6° misoriented substrates under the usual growth conditions. The presence of wires instead of wells could have several unexpected consequences for the performance of the MQW solar cells, both positive and negative, that need to be assessed to achieve high conversion efficiencies. In this letter, we study QWR properties from the point of view of their performance as solar cells by means of transmission electron microscopy, time resolved photoluminescence and external quantum efficiency (EQE) using polarised light. We find that these QWRs have longermore » lifetimes than nominally identical QWs grown on exact [100] GaAs substrates, of up to 1 μs, at any level of illumination. We attribute this effect to an asymmetric carrier escape from the nanostructures leading to a strong 1D-photo-charging, keeping electrons confined along the wire and holes in the barriers. In principle, these extended lifetimes could be exploited to enhance carrier collection and reduce dark current losses. Light absorption by these QWRs is 1.6 times weaker than QWs, as revealed by EQE measurements, which emphasises the need for more layers of nanostructures or the use light trapping techniques. Contrary to what we expected, QWR show very low absorption anisotropy, only 3.5%, which was the main drawback a priori of this nanostructure. We attribute this to a reduced lateral confinement inside the wires. These results encourage further study and optimization of QWRs for high efficiency solar cells.« less

InGaAs/GaAsP strain balanced multi-quantum wires grown on misoriented GaAs substrates for high efficiency solar cells

NASA Astrophysics Data System (ADS)

Alonso-Álvarez, D.; Thomas, T.; Führer, M.; Hylton, N. P.; Ekins-Daukes, N. J.; Lackner, D.; Philipps, S. P.; Bett, A. W.; Sodabanlu, H.; Fujii, H.; Watanabe, K.; Sugiyama, M.; Nasi, L.; Campanini, M.

2014-08-01

Quantum wires (QWRs) form naturally when growing strain balanced InGaAs/GaAsP multi-quantum wells (MQW) on GaAs [100] 6° misoriented substrates under the usual growth conditions. The presence of wires instead of wells could have several unexpected consequences for the performance of the MQW solar cells, both positive and negative, that need to be assessed to achieve high conversion efficiencies. In this letter, we study QWR properties from the point of view of their performance as solar cells by means of transmission electron microscopy, time resolved photoluminescence and external quantum efficiency (EQE) using polarised light. We find that these QWRs have longer lifetimes than nominally identical QWs grown on exact [100] GaAs substrates, of up to 1 μs, at any level of illumination. We attribute this effect to an asymmetric carrier escape from the nanostructures leading to a strong 1D-photo-charging, keeping electrons confined along the wire and holes in the barriers. In principle, these extended lifetimes could be exploited to enhance carrier collection and reduce dark current losses. Light absorption by these QWRs is 1.6 times weaker than QWs, as revealed by EQE measurements, which emphasises the need for more layers of nanostructures or the use light trapping techniques. Contrary to what we expected, QWR show very low absorption anisotropy, only 3.5%, which was the main drawback a priori of this nanostructure. We attribute this to a reduced lateral confinement inside the wires. These results encourage further study and optimization of QWRs for high efficiency solar cells.

Quantum Optical Transistor and Other Devices Based on Nanostructures

NASA Astrophysics Data System (ADS)

Li, Jin-Jin; Zhu, Ka-Di

Laser and strong coupling can coexist in a single quantum dot (QD) coupled to nanostructures. This provides an important clue toward the realization of quantum optical devices, such as quantum optical transistor, slow light device, fast light device, or light storage device. In contrast to conventional electronic transistor, a quantum optical transistor uses photons as signal carriers rather than electrons, which has a faster and more powerful transfer efficiency. Under the radiation of a strong pump laser, a signal laser can be amplified or attenuated via passing through a single quantum dot coupled to a photonic crystal (PC) nanocavity system. Such a switching and amplifying behavior can really implement the quantum optical transistor. By simply turning on or off the input pump laser, the amplified or attenuated signal laser can be obtained immediately. Based on this transistor, we further propose a method to measure the vacuum Rabi splitting of exciton in all-optical domain. Besides, we study the light propagation in a coupled QD and nanomechanical resonator (NR) system. We demonstrate that it is possible to achieve the slow light, fast light, and quantum memory for light on demand, which is based on the mechanically induced coherent population oscillation (MICPO) and exciton polaritons. These QD devices offer a route toward the use of all-optical technique to investigate the coupled QD systems and will make contributions to quantum internets and quantum computers.

Scalable photonic quantum computing assisted by quantum-dot spin in double-sided optical microcavity.

PubMed

Wei, Hai-Rui; Deng, Fu-Guo

2013-07-29

We investigate the possibility of achieving scalable photonic quantum computing by the giant optical circular birefringence induced by a quantum-dot spin in a double-sided optical microcavity as a result of cavity quantum electrodynamics. We construct a deterministic controlled-not gate on two photonic qubits by two single-photon input-output processes and the readout on an electron-medium spin confined in an optical resonant microcavity. This idea could be applied to multi-qubit gates on photonic qubits and we give the quantum circuit for a three-photon Toffoli gate. High fidelities and high efficiencies could be achieved when the side leakage to the cavity loss rate is low. It is worth pointing out that our devices work in both the strong and the weak coupling regimes.

Using of Quantum Dots in Biology and Medicine.

PubMed

Pleskova, Svetlana; Mikheeva, Elza; Gornostaeva, Ekaterina

2018-01-01

Quantum dots are nanoparticles, which due to their unique physical and chemical (first of all optical) properties, are promising in biology and medicine. There are many ways for quantum dots synthesis, both in the form of nanoislands self-forming on the surfaces, which can be used as single-photon emitters in electronics for storing information, and in the form of colloidal quantum dots for diagnostic and therapeutic purposes in living systems. The paper describes the main methods of quantum dots synthesis and summarizes medical and biological ways of their use. The main emphasis is laid on the ways of quantum dots surface modification. Influence of the size and form of nanoparticles, charge on the surfaces of quantum dots, and cover type on the efficiency of internalization by cells and cell compartments is shown. The main mechanisms of penetration are considered.

Effects of the capping ligands, linkers and oxide surface on the electron injection mechanism of copper sulfide quantum dot-sensitized solar cells.

PubMed

Suárez, Javier Amaya; Plata, Jose J; Márquez, Antonio M; Sanz, Javier Fdez

2017-06-07

Quantum dot-sensitized solar cells, QDSCs, are a clean and effective alternative to fossil fuels to reduce CO 2 emissions. However, the different components that constitute the QDSCs and the difficulty of isolating experimentally their effects on the performance of the whole system slow down the development of more efficient devices. In this work, DFT calculations are combined with a bottom-up approach to differentiate the effect of each component on the electronic structure and absorption spectra. First, Cu 2 S QDs were built including a U parameter to effectively describe the localization of electrons. The effect of capping agents is addressed using ligands with different electron-donating/withdrawing groups. The role of linkers and their adsorption on the oxide surface are also examined. Finally, we propose a main indirect electron injection mechanism based on the position of the peaks of the spectra.

On the Hole Injection for III-Nitride Based Deep Ultraviolet Light-Emitting Diodes.

PubMed

Li, Luping; Zhang, Yonghui; Xu, Shu; Bi, Wengang; Zhang, Zi-Hui; Kuo, Hao-Chung

2017-10-24

The hole injection is one of the bottlenecks that strongly hinder the quantum efficiency and the optical power for deep ultraviolet light-emitting diodes (DUV LEDs) with the emission wavelength smaller than 360 nm. The hole injection efficiency for DUV LEDs is co-affected by the p-type ohmic contact, the p-type hole injection layer, the p-type electron blocking layer and the multiple quantum wells. In this report, we review a large diversity of advances that are currently adopted to increase the hole injection efficiency for DUV LEDs. Moreover, by disclosing the underlying device physics, the design strategies that we can follow have also been suggested to improve the hole injection for DUV LEDs.

On the Hole Injection for III-Nitride Based Deep Ultraviolet Light-Emitting Diodes

PubMed Central

Li, Luping; Zhang, Yonghui; Kuo, Hao-Chung

2017-01-01

The hole injection is one of the bottlenecks that strongly hinder the quantum efficiency and the optical power for deep ultraviolet light-emitting diodes (DUV LEDs) with the emission wavelength smaller than 360 nm. The hole injection efficiency for DUV LEDs is co-affected by the p-type ohmic contact, the p-type hole injection layer, the p-type electron blocking layer and the multiple quantum wells. In this report, we review a large diversity of advances that are currently adopted to increase the hole injection efficiency for DUV LEDs. Moreover, by disclosing the underlying device physics, the design strategies that we can follow have also been suggested to improve the hole injection for DUV LEDs. PMID:29073738

Simple formalism for efficient derivatives and multi-determinant expansions in quantum Monte Carlo

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

Filippi, Claudia, E-mail: c.filippi@utwente.nl; Assaraf, Roland, E-mail: assaraf@lct.jussieu.fr; Moroni, Saverio, E-mail: moroni@democritos.it

2016-05-21

We present a simple and general formalism to compute efficiently the derivatives of a multi-determinant Jastrow-Slater wave function, the local energy, the interatomic forces, and similar quantities needed in quantum Monte Carlo. Through a straightforward manipulation of matrices evaluated on the occupied and virtual orbitals, we obtain an efficiency equivalent to algorithmic differentiation in the computation of the interatomic forces and the optimization of the orbital parameters. Furthermore, for a large multi-determinant expansion, the significant computational gain afforded by a recently introduced table method is here extended to the local value of any one-body operator and to its derivatives, inmore » both all-electron and pseudopotential calculations.« less

Ab initio quantum chemical calculation of electron transfer matrix elements for large molecules

NASA Astrophysics Data System (ADS)

Zhang, Linda Yu; Friesner, Richard A.; Murphy, Robert B.

1997-07-01

Using a diabatic state formalism and pseudospectral numerical methods, we have developed an efficient ab initio quantum chemical approach to the calculation of electron transfer matrix elements for large molecules. The theory is developed at the Hartree-Fock level and validated by comparison with results in the literature for small systems. As an example of the power of the method, we calculate the electronic coupling between two bacteriochlorophyll molecules in various intermolecular geometries. Only a single self-consistent field (SCF) calculation on each of the monomers is needed to generate coupling matrix elements for all of the molecular pairs. The largest calculations performed, utilizing 1778 basis functions, required ˜14 h on an IBM 390 workstation. This is considerably less cpu time than would be necessitated with a supermolecule adiabatic state calculation and a conventional electronic structure code.

Electron-Poor Thiophene 1,1-Dioxides: Synthesis, Characterization, and Application as Electron Relays in Photocatalytic Hydrogen Generation.

PubMed

Tsai, Chia-Hua; Chirdon, Danielle N; Kagalwala, Husain N; Maurer, Andrew B; Kaur, Aman; Pintauer, Tomislav; Bernhard, Stefan; Noonan, Kevin J T

2015-08-03

The synthesis and characterization of electron-poor thiophene 1,1-dioxides bearing cyanated phenyl groups are reported. The electron-accepting nature of these compounds was evaluated by cyclic voltammetry, and highly reversible and facile reductions were observed for several derivatives. Moreover, some of the reduced thiophene dioxides form colorful anions, which were investigated spectroelectrochemically. Photoluminescence spectra of the electron-deficient sulfones were measured in CH2 Cl2, and they emit in the blue-green region with significant variation in the quantum yield depending on the aryl substituents. By expanding the degree of substitution on the phenyl rings, quantum yields up to 34 % were obtained. X-ray diffraction data are reported for two of the thiophene 1,1-dioxides, and the electronic structure was probed for all synthesized derivatives through DFT calculations. The dioxides were also examined as electron relays in a photocatalytic water reduction reaction, and they showed potential to boost the efficiency. © 2015 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Synthesis and x-ray characterization of sputtered bi-alkali antimonide photocathodes

DOE PAGES

Gaowei, M.; Ding, Z.; Schubert, S.; ...

2017-11-10

Advanced photoinjectors, which are critical to many next generation accelerators, open the door to new ways of material probing, both as injectors for free electron lasers and for ultra-fast electron diffraction. For these applications, the nonuniformity of the electric field near the cathode caused by surface roughness can be the dominant source of beam emittance. Therefore, improving the photocathode roughness while maintaining quantum efficiency is essential to the improvement of beam brightness. Here in this article, we report the demonstration of a bi-alkali antimonide photocathode with an order of magnitude improved roughness by sputter deposition from a K 2CsSb sputtermore » target, using in situ and operando X-ray characterizations. We found that a surface roughness of 0.5 nm for a sputtered photocathode with a final thickness of 42 nm can be achieved while still yielding a quantum efficiency of 3.3% at 530 nm wavelength.« less

Synthesis and x-ray characterization of sputtered bi-alkali antimonide photocathodes

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

Gaowei, M.; Ding, Z.; Schubert, S.

Advanced photoinjectors, which are critical to many next generation accelerators, open the door to new ways of material probing, both as injectors for free electron lasers and for ultra-fast electron diffraction. For these applications, the nonuniformity of the electric field near the cathode caused by surface roughness can be the dominant source of beam emittance. Therefore, improving the photocathode roughness while maintaining quantum efficiency is essential to the improvement of beam brightness. Here in this article, we report the demonstration of a bi-alkali antimonide photocathode with an order of magnitude improved roughness by sputter deposition from a K 2CsSb sputtermore » target, using in situ and operando X-ray characterizations. We found that a surface roughness of 0.5 nm for a sputtered photocathode with a final thickness of 42 nm can be achieved while still yielding a quantum efficiency of 3.3% at 530 nm wavelength.« less

Photon-enhanced thermionic emission for solar concentrator systems.

PubMed

Schwede, Jared W; Bargatin, Igor; Riley, Daniel C; Hardin, Brian E; Rosenthal, Samuel J; Sun, Yun; Schmitt, Felix; Pianetta, Piero; Howe, Roger T; Shen, Zhi-Xun; Melosh, Nicholas A

2010-09-01

Solar-energy conversion usually takes one of two forms: the 'quantum' approach, which uses the large per-photon energy of solar radiation to excite electrons, as in photovoltaic cells, or the 'thermal' approach, which uses concentrated sunlight as a thermal-energy source to indirectly produce electricity using a heat engine. Here we present a new concept for solar electricity generation, photon-enhanced thermionic emission, which combines quantum and thermal mechanisms into a single physical process. The device is based on thermionic emission of photoexcited electrons from a semiconductor cathode at high temperature. Temperature-dependent photoemission-yield measurements from GaN show strong evidence for photon-enhanced thermionic emission, and calculated efficiencies for idealized devices can exceed the theoretical limits of single-junction photovoltaic cells. The proposed solar converter would operate at temperatures exceeding 200 degrees C, enabling its waste heat to be used to power a secondary thermal engine, boosting theoretical combined conversion efficiencies above 50%.

Computational Modeling of Photocatalysts for CO2 Conversion Applications

NASA Astrophysics Data System (ADS)

Tafen, De; Matranga, Christopher

2013-03-01

To make photocatalytic conversion approaches efficient, economically practical, and industrially scalable, catalysts capable of utilizing visible and near infrared photons need to be developed. Recently, a series of CdSe and PbS quantum dot-sensitized TiO2 heterostructures have been synthesized, characterized, and tested for reduction of CO2 under visible light. Following these experiments, we use density functional theory to model these heterostructured catalysts and investigate their CO2 catalytic activity. In particular, we study the nature of the heterostructure interface, charge transport/electron transfer, active sites and the electronic structures of these materials. The results will be presented and compared to experiments. The improvement of our understanding of the properties of these materials will aid not only the development of more robust, visible light active photocatalysts for carbon management applications, but also the development of quantum dot-sensitized semiconductor solar cells with high efficiencies in solar-to-electrical energy conversion.

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

Schaefer, Tim; Institut für Physikalische Chemie, Universität zu Köln, 50939 Köln; Schwab, Tobias

A random scattering approach to enhance light extraction in white top-emitting organic light-emitting diodes (OLEDs) is reported. Through solution processing from fluorinated solvents, a nano-particle scattering layer (NPSL) can be deposited directly on top of small molecule OLEDs without affecting their electrical performance. The scattering length for light inside the NPSL is determined from transmission measurements and found to be in agreement with Mie scattering theory. Furthermore, the dependence of the light outcoupling enhancement on electron transport layer thickness is studied. Depending on the electron transport layer thickness, the NPSL enhances the external quantum efficiency of the investigated white OLEDsmore » by between 1.5 and 2.3-fold. For a device structure that has been optimized prior to application of the NPSL, the maximum external quantum efficiency is improved from 4.7% to 7.4% (1.6-fold improvement). In addition, the scattering layer strongly reduces the undesired shift in emission color with viewing angle.« less

Exceeding Conventional Photovoltaic Efficiency Limits Using Colloidal Quantum Dots

NASA Astrophysics Data System (ADS)

Pach, Gregory F.

Colloidal quantum dots (QDs) are a widely investigated field of research due to their highly tunable nature in which the optical and electronic properties of the nanocrystal can be manipulated by merely changing the nanocrystal's size. Specifically, colloidal quantum dot solar cells (QDSCs) have become a promising candidate for future generation photovoltaic technology. Quantum dots exhibit multiple exciton generation (MEG) in which multiple electron-hole pairs are generated from a single high-energy photon. This process is not observed in bulk-like semiconductors and allows for QDSCs to achieve theoretical efficiency limits above the standard single-junction Shockley-Queisser limit. However, the fast expanding field of QDSC research has lacked standardization of synthetic techniques and device design. Therefore, we sought to detail methodology for synthesizing PbS and PbSe QDs as well as photovoltaic device fabrication techniques as a fast track toward constructing high-performance solar cells. We show that these protocols lead toward consistently achieving efficiencies above 8% for PbS QDSCs. Using the same methodology for building single-junction photovoltaic devices, we incorporated PbS QDs as a bottom cell into a monolithic tandem architecture along with solution-processed CdTe nanocrystals. Modeling shows that near-peak tandem device efficiencies can be achieved across a wide range of bottom cell band gaps, and therefore the highly tunable band gap of lead-chalcogenide QDs lends well towards a bottom cell in a tandem architecture. A fully functioning monolithic tandem device is realized through the development of a ZnTe/ZnO recombination layer that appropriately combines the two subcells in series. Multiple recent reports have shown nanocrystalline heterostructures to undergo the MEG process more efficiency than several other nanostrucutres, namely lead-chalcogenide QDs. The final section of my thesis expands upon a recent publication by Zhang et. al., which details the synthesis of PbS/CdS heterostructures in which the PbS and CdS domains exist on opposite sides of the nanocrystal and are termed "Janus particles". Transient absorption spectroscopy shows MEG quantum yields above unity very the thermodynamic limit of 2Eg for PbS/CdS Janus particles. We further explain a mechanism for enhanced MEG using photoluminescence studies.

Determination of the absolute internal quantum efficiency of photoluminescence in GaN co-doped with Si and Zn

NASA Astrophysics Data System (ADS)

Reshchikov, M. A.; Foussekis, M.; McNamara, J. D.; Behrends, A.; Bakin, A.; Waag, A.

2012-04-01

The optical properties of high-quality GaN co-doped with silicon and zinc are investigated by using temperature-dependent continuous-wave and time-resolved photoluminescence measurements. The blue luminescence band is related to the ZnGa acceptor in GaN:Si,Zn, which exhibits an exceptionally high absolute internal quantum efficiency (IQE). An IQE above 90% was calculated for several samples having different concentrations of Zn. Accurate and reliable values of the IQE were obtained by using several approaches based on rate equations. The concentrations of the ZnGa acceptors and free electrons were also estimated from the photoluminescence measurements.

ZnSe quantum dots modified with a Ni(cyclam) catalyst for efficient visible-light driven CO2 reduction in water.

PubMed

Kuehnel, Moritz F; Sahm, Constantin D; Neri, Gaia; Lee, Jonathan R; Orchard, Katherine L; Cowan, Alexander J; Reisner, Erwin

2018-03-07

A precious metal and Cd-free photocatalyst system for efficient CO 2 reduction in water is reported. The hybrid assembly consists of ligand-free ZnSe quantum dots (QDs) as a visible-light photosensitiser combined with a phosphonic acid-functionalised Ni(cyclam) catalyst, NiCycP. This precious metal-free photocatalyst system shows a high activity for aqueous CO 2 reduction to CO (Ni-based TON CO > 120), whereas an anchor-free catalyst, Ni(cyclam)Cl 2 , produced three times less CO. Additional ZnSe surface modification with 2-(dimethylamino)ethanethiol (MEDA) partially suppresses H 2 generation and enhances the CO production allowing for a Ni-based TON CO of > 280 and more than 33% selectivity for CO 2 reduction over H 2 evolution, after 20 h visible light irradiation ( λ > 400 nm, AM 1.5G, 1 sun). The external quantum efficiency of 3.4 ± 0.3% at 400 nm is comparable to state-of-the-art precious metal photocatalysts. Transient absorption spectroscopy showed that band-gap excitation of ZnSe QDs is followed by rapid hole scavenging and very fast electron trapping in ZnSe. The trapped electrons transfer to NiCycP on the ps timescale, explaining the high performance for photocatalytic CO 2 reduction. With this work we introduce ZnSe QDs as an inexpensive and efficient visible light-absorber for solar fuel generation.

Optical rectenna operation: where Maxwell meets Einstein

NASA Astrophysics Data System (ADS)

Joshi, Saumil; Moddel, Garret

2016-07-01

Optical rectennas are antenna-coupled diode rectifiers that receive and convert optical-frequency electromagnetic radiation into DC output. The analysis of rectennas is carried out either classically using Maxwell’s wave-like approach, or quantum-mechanically using Einstein’s particle-like approach for electromagnetic radiation. One of the characteristics of classical operation is that multiple photons transfer their energy to individual electrons, whereas in quantum operation each photon transfers its energy to each electron. We analyze the correspondence between the two approaches by comparing rectenna response first to monochromatic illumination obtained using photon-assisted tunnelling theory and classical theory. Applied to broadband rectenna operation, this correspondence provides clues to designing a rectenna solar cell that has the potential to exceed the 44% quantum-limited conversion efficiency. The comparison of operating regimes shows how optical rectenna operation differs from microwave rectenna operation.

The role of the tunneling matrix element and nuclear reorganization in the design of quantum-dot cellular automata molecules

NASA Astrophysics Data System (ADS)

Henry, Jackson; Blair, Enrique P.

2018-02-01

Mixed-valence molecules provide an implementation for a high-speed, energy-efficient paradigm for classical computing known as quantum-dot cellular automata (QCA). The primitive device in QCA is a cell, a structure with multiple quantum dots and a few mobile charges. A single mixed-valence molecule can function as a cell, with redox centers providing quantum dots. The charge configuration of a molecule encodes binary information, and device switching occurs via intramolecular electron transfer between dots. Arrays of molecular cells adsorbed onto a substrate form QCA logic. Individual cells in the array are coupled locally via the electrostatic electric field. This device networking enables general-purpose computing. Here, a quantum model of a two-dot molecule is built in which the two-state electronic system is coupled to the dominant nuclear vibrational mode via a reorganization energy. This model is used to explore the effects of the electronic inter-dot tunneling (coupling) matrix element and the reorganization energy on device switching. A semi-classical reduction of the model also is made to investigate the competition between field-driven device switching and the electron-vibrational self-trapping. A strong electron-vibrational coupling (high reorganization energy) gives rise to self-trapping, which inhibits the molecule's ability to switch. Nonetheless, there remains an expansive area in the tunneling-reorganization phase space where molecules can support adequate tunneling. Thus, the relationship between the tunneling matrix element and the reorganization energy affords significant leeway in the design of molecules viable for QCA applications.

Role of electron transfer in Ce{sup 3+} sensitized Yb{sup 3+} luminescence in borate glass

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

Sontakke, Atul D., E-mail: sontakke.atul.55a@st.kyoto-u.ac.jp; Katayama, Yumiko; Zhuang, Yixi

2015-01-07

In a Ce{sup 3+}-Yb{sup 3+} system, two mechanisms are proposed so far namely, the quantum cutting mechanism and the electron transfer mechanism explaining Yb{sup 3+} infrared luminescence under Ce{sup 3+} excitation. Among them, the quantum cutting mechanism, where one Ce{sup 3+} photon (ultraviolet/blue) gives rise to two Yb{sup 3+} photons (near infrared) is widely sought for because of its huge potential in enhancing the solar cell efficiency. In present study on Ce{sup 3+}-Yb{sup 3+} codoped borate glasses, Ce{sup 3+} sensitized Yb{sup 3+} luminescence at ∼1 μm have been observed on Ce{sup 3+} 5d state excitation. However, the intensity of sensitized Yb{supmore » 3+} luminescence is found to be very weak compared to the strong quenching occurred in Ce{sup 3+} luminescence in Yb{sup 3+} codoped glasses. Moreover, the absolute luminescence quantum yield also showed a decreasing trend with Yb{sup 3+} codoping in the glasses. The overall behavior of the luminescence properties and the quantum yield is strongly contradicting with the quantum cutting phenomenon. The results are attributed to the energetically favorable electron transfer interactions followed by Ce{sup 3+}-Yb{sup 3+} ⇌ Ce{sup 4+}-Yb{sup 2+} inter-valence charge transfer and successfully explained using the absolute electron binding energies of dopant ions in the studied borate glass. Finally, an attempt has been presented to generalize the electron transfer mechanism among opposite oxidation/reduction property dopant ions using the vacuum referred electron binding energy (VRBE) scheme for lanthanide series.« less

Direct Measurement of Polarization-Induced Fields in GaN/AlN by Nano-Beam Electron Diffraction

NASA Astrophysics Data System (ADS)

Carvalho, Daniel; Müller-Caspary, Knut; Schowalter, Marco; Grieb, Tim; Mehrtens, Thorsten; Rosenauer, Andreas; Ben, Teresa; García, Rafael; Redondo-Cubero, Andrés; Lorenz, Katharina; Daudin, Bruno; Morales, Francisco M.

2016-06-01

The built-in piezoelectric fields in group III-nitrides can act as road blocks on the way to maximizing the efficiency of opto-electronic devices. In order to overcome this limitation, a proper characterization of these fields is necessary. In this work nano-beam electron diffraction in scanning transmission electron microscopy mode has been used to simultaneously measure the strain state and the induced piezoelectric fields in a GaN/AlN multiple quantum well system.

Deep Blue Phosphorescent Organic Light-Emitting Diodes with CIEy Value of 0.11 and External Quantum Efficiency up to 22.5.

PubMed

Li, Xiaoyue; Zhang, Juanye; Zhao, Zifeng; Wang, Liding; Yang, Hannan; Chang, Qiaowen; Jiang, Nan; Liu, Zhiwei; Bian, Zuqiang; Liu, Weiping; Lu, Zhenghong; Huang, Chunhui

2018-03-01

Organic light-emitting diodes (OLEDs) based on red and green phosphorescent iridium complexes are successfully commercialized in displays and solid-state lighting. However, blue ones still remain a challenge on account of their relatively dissatisfactory Commission International de L'Eclairage (CIE) coordinates and low efficiency. After analyzing the reported blue iridium complexes in the literature, a new deep-blue-emitting iridium complex with improved photoluminescence quantum yield is designed and synthesized. By rational screening host materials showing high triplet energy level in neat film as well as the OLED architecture to balance electron and hole recombination, highly efficient deep-blue-emission OLEDs with a CIE at (0.15, 0.11) and maximum external quantum efficiency (EQE) up to 22.5% are demonstrated. Based on the transition dipole moment vector measurement with a variable-angle spectroscopic ellipsometry method, the ultrahigh EQE is assigned to a preferred horizontal dipole orientation of the iridium complex in doped film, which is beneficial for light extraction from the OLEDs. © 2018 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

New Detector Developments for Future UV Space Missions

NASA Astrophysics Data System (ADS)

Werner, Klaus; Kappelmann, Norbert

Ultraviolet (UV) astronomy is facing “dark ages”: After the shutdown of the Hubble Space Tele-scope only the WSO/UV mission will be operable in the UV wavelength region with efficient instruments. Improved optics and detectors are necessary for future successor missions to tackle new scientific goals. This drives our development of microchannel plate (MCP) UV-detectors with high quantum efficiency, high spatial resolution and low-power readout electronics. To enhance the quantum efficiency and the lifetime of the MCP detectors we are developing new cathodes and new anodes for these detectors. To achieve high quantum efficiency, we will use caesium-activated gallium nitride as semitransparent photocathodes with a much higher efficiency than default CsI/CsTe cathodes in this wavelength range. The new anodes will be cross-strip anodes with 64 horizontal and 64 vertical electrodes. This type of anode requires a lower gain and leads to an increased lifetime of the detector, compared to MCP detectors with other anode types. The heart of the new developed front-end-electronic for such type of anode is the so called “BEETLE chip”, which was designed by the MPI für Kernphysik Heidelberg for the LHCb ex-periment at CERN. This chip provides 128 input channels with charge-sensitive preamplifiers and shapers. Our design of the complete front-end readout electronics enables a total power con-sumption of less than 10 W. The MCP detector is intrinsically solar blind, single photon counting and has a very low read-out noise. To qualify this new type of detectors we are presently planning to build a small UV telescope for the usage on the German Technology Experimental Carrier (TET). Furthermore we are involved in the new German initiative for a Public Telescope, a space telescope equipped with an 80 cm mirror. One of the main instruments will be a high-resolution UV-Echelle Spectrograph that will be built by the University of Tübingen. The launch of this mission is scheduled for 2017.

Effects of heteroatom substitution in conjugated heterocyclic compounds on photovoltaic performance: from sulfur to tellurium.

PubMed

Park, Y S; Kale, T S; Nam, C-Y; Choi, D; Grubbs, R B

2014-07-28

We report a general strategy for fine-tuning the bandgap of donor-acceptor-donor based organic molecules by modulating the electron-donating ability of the donor moiety by changing the benzochalcogenophene donor groups from benzothiophenes to benzoselenophenes to benzotellurophenes. These molecules show red-shifts in absorption and external quantum efficiency maxima from sulfur to selenium to tellurium. In bulk heterojunction solar cell devices, the benzoselenophene derivative shows a power conversion efficiency as high as 5.8% with PC61BM as the electron acceptor.

Large tunable valley splitting in edge-free graphene quantum dots on boron nitride

NASA Astrophysics Data System (ADS)

Freitag, Nils M.; Reisch, Tobias; Chizhova, Larisa A.; Nemes-Incze, Péter; Holl, Christian; Woods, Colin R.; Gorbachev, Roman V.; Cao, Yang; Geim, Andre K.; Novoselov, Kostya S.; Burgdörfer, Joachim; Libisch, Florian; Morgenstern, Markus

2018-05-01

Coherent manipulation of the binary degrees of freedom is at the heart of modern quantum technologies. Graphene offers two binary degrees: the electron spin and the valley. Efficient spin control has been demonstrated in many solid-state systems, whereas exploitation of the valley has only recently been started, albeit without control at the single-electron level. Here, we show that van der Waals stacking of graphene onto hexagonal boron nitride offers a natural platform for valley control. We use a graphene quantum dot induced by the tip of a scanning tunnelling microscope and demonstrate valley splitting that is tunable from -5 to +10 meV (including valley inversion) by sub-10-nm displacements of the quantum dot position. This boosts the range of controlled valley splitting by about one order of magnitude. The tunable inversion of spin and valley states should enable coherent superposition of these degrees of freedom as a first step towards graphene-based qubits.

Applying Quantum Monte Carlo to the Electronic Structure Problem

NASA Astrophysics Data System (ADS)

Powell, Andrew D.; Dawes, Richard

2016-06-01

Two distinct types of Quantum Monte Carlo (QMC) calculations are applied to electronic structure problems such as calculating potential energy curves and producing benchmark values for reaction barriers. First, Variational and Diffusion Monte Carlo (VMC and DMC) methods using a trial wavefunction subject to the fixed node approximation were tested using the CASINO code.[1] Next, Full Configuration Interaction Quantum Monte Carlo (FCIQMC), along with its initiator extension (i-FCIQMC) were tested using the NECI code.[2] FCIQMC seeks the FCI energy for a specific basis set. At a reduced cost, the efficient i-FCIQMC method can be applied to systems in which the standard FCIQMC approach proves to be too costly. Since all of these methods are statistical approaches, uncertainties (error-bars) are introduced for each calculated energy. This study tests the performance of the methods relative to traditional quantum chemistry for some benchmark systems. References: [1] R. J. Needs et al., J. Phys.: Condensed Matter 22, 023201 (2010). [2] G. H. Booth et al., J. Chem. Phys. 131, 054106 (2009).

Exploring the effect of band alignment and surface states on photoinduced electron transfer from CuInS2/CdS core/shell quantum dots to TiO2 electrodes.

PubMed

Sun, Mingye; Zhu, Dehua; Ji, Wenyu; Jing, Pengtao; Wang, Xiuying; Xiang, Weidong; Zhao, Jialong

2013-12-11

Photoinduced electron transfer (ET) processes from CuInS2/CdS core/shell quantum dots (QDs) with different core sizes and shell thicknesses to TiO2 electrodes were investigated by time-resolved photoluminescence (PL) spectroscopy. The ET rates and efficiencies from CuInS2/CdS QDs to TiO2 were superior to those of CuInS2/ZnS QDs. An enhanced ET efficiency was surprisingly observed for 2.0 nm CuInS2 core QDs after growth of the CdS shell. On the basis of the experimental and theoretical analysis, the improved performances of CuInS2/CdS QDs were attributed to the passivation of nonradiative traps by overcoating shell and enhanced delocalization of electron wave function from core to CdS shell due to lower conduction band offset. These results indicated that the electron distribution regulated by the band alignment between core and shell of QDs and the passivation of surface defect states could improve ET performance between donor and acceptor.

Photochemical synthesis and photophysical properties of coumarins bearing extended polyaromatic rings studied by emission and transient absorption measurements.

PubMed

Yamaji, Minoru; Hakoda, Yuma; Okamoto, Hideki; Tani, Fumito

2017-04-12

We prepared a variety of coumarin derivatives having expanded π-electron systems along the direction crossing the C 3 -C 4 bond of the coumarin skeleton via a photochemical cyclization process and investigated their photophysical features as a function of the number (n) of the added benzene rings based on emission and transient absorption measurements. Upon increasing n, the fluorescence quantum yields of the π-extended coumarins increased. Expanding the π-electron system on the C 3 -C 4 bond of the coumarin skeleton was found to be efficient for increasing the fluorescence ability more than that on the C 7 -C 8 bond. Introducing the methoxy group at the 7-position was also efficient for enhancing the fluorescence quantum yield and rate of the expanded coumarins. The non-radiative process from the fluorescence state was not substantially influenced by the expanded π-electron system. The competitive process with the fluorescence was found to be intersystem crossing to the triplet state based on the observations of the triplet-triplet absorption. The effects of the expanded π-electron systems on the fluorescence ability were investigated with the aid of TD-DFT calculations.

Design, fabrication and characterization of rugged, high-performance quantum dot photocathodes

NASA Astrophysics Data System (ADS)

Pietryga, Jeffrey; Robel, Istvan; Makarov, Nikolay; Lim, Jaehoon; Lin, Qianglu; Lewellen, John; Moody, Nathan

Semiconductor nanocrystal quantum dots (QDs) are bright, tunable fluorophores used as, e.g., biolabels and downcoverting phosphors. Such applications make use of over three decades in advances in techniques for overcoming the natural tendency of these materials toward losing photoexcited carriers to surface defect states or to ionization. Ironically, QDs first gained attention as a material class for use in photocatalysis, which uses QD photoionization to drive redox reactions. Here, we explore the use of QDs in an alternative application that also exploits photoionization, namely within photocathodes for the electron guns that will enable next-generation light sources. We evaluate the efficiency of electron photoemission of conductive, solution-cast QD films of a variety of compositions in a typical electron gun configuration. By quantifying photocurrent as a function of excitation photon energy, excitation intensity and pulse duration, we demonstrate efficiencies superior to standard copper cathodes in films that are more robust against oxidation. Finally, we establish the dominant mechanism responsible for electron emission in the multi-photon excitation regime, which suggests numerous pathways for further enhancements. We gratefully acknowledge the support of the Los Alamos National Laboratory Directed Research and Development (LDRD) program.

Elevated CO2 response of photosynthesis depends on ozone concentration in aspen

Treesearch

Asko Noormets; Olevi Kull; Anu Sober; Mark E. Kubiske; David F. Karnosky

2010-01-01

The effect of elevated CO2 and O3 on apparent quantum yield (ø), maximum photosynthesis (Pmax), carboxylation efficiency (Vcmax) and electron transport capacity (Jmax) at different canopy locations was studied in two aspen (Populus...

Harnessing Sun’s Energy with Quantum Dots Based Next Generation Solar Cell

PubMed Central

Halim, Mohammad A.

2012-01-01

Our energy consumption relies heavily on the three components of fossil fuels (oil, natural gas and coal) and nearly 83% of our current energy is consumed from those sources. The use of fossil fuels, however, has been viewed as a major environmental threat because of their substantial contribution to greenhouse gases which are responsible for increasing the global average temperature. Last four decades, scientists have been searching for alternative sources of energy which need to be environmentally clean, efficient, cost-effective, renewable, and sustainable. One of the promising sustainable sources of energy can be achieved by harnessing sun energy through silicon wafer, organic polymer, inorganic dye, and quantum dots based solar cells. Among them, quantum dots have an exceptional property in that they can excite multiple electrons using only one photon. These dots can easily be synthesized, processed in solution, and incorporated into solar cell application. Interestingly, the quantum dots solar cells can exceed the Shockley-Queisser limit; however, it is a great challenge for other solar cell materials to exceed the limit. Theoretically, the quantum dots solar cell can boost the power conversion efficiency up to 66% and even higher to 80%. Moreover, in changing the size of the quantum dots one can utilize the Sun’s broad spectrum of visible and infrared ranges. This review briefly overviews the present performance of different materials-based solar cells including silicon wafer, dye-sensitized, and organic solar cells. In addition, recent advances of the quantum dots based solar cells which utilize cadmium sulfide/selenide, lead sulfide/selenide, and new carbon dots as light harvesting materials has been reviewed. A future outlook is sketched as to how one could improve the efficiency up to 10% from the current highest efficiency of 6.6%. PMID:28348320

Harnessing Sun's Energy with Quantum Dots Based Next Generation Solar Cell.

PubMed

Halim, Mohammad A

2012-12-27

Our energy consumption relies heavily on the three components of fossil fuels (oil, natural gas and coal) and nearly 83% of our current energy is consumed from those sources. The use of fossil fuels, however, has been viewed as a major environmental threat because of their substantial contribution to greenhouse gases which are responsible for increasing the global average temperature. Last four decades, scientists have been searching for alternative sources of energy which need to be environmentally clean, efficient, cost-effective, renewable, and sustainable. One of the promising sustainable sources of energy can be achieved by harnessing sun energy through silicon wafer, organic polymer, inorganic dye, and quantum dots based solar cells. Among them, quantum dots have an exceptional property in that they can excite multiple electrons using only one photon. These dots can easily be synthesized, processed in solution, and incorporated into solar cell application. Interestingly, the quantum dots solar cells can exceed the Shockley - Queisser limit; however, it is a great challenge for other solar cell materials to exceed the limit. Theoretically, the quantum dots solar cell can boost the power conversion efficiency up to 66% and even higher to 80%. Moreover, in changing the size of the quantum dots one can utilize the Sun's broad spectrum of visible and infrared ranges. This review briefly overviews the present performance of different materials-based solar cells including silicon wafer, dye-sensitized, and organic solar cells. In addition, recent advances of the quantum dots based solar cells which utilize cadmium sulfide/selenide, lead sulfide/selenide, and new carbon dots as light harvesting materials has been reviewed. A future outlook is sketched as to how one could improve the efficiency up to 10% from the current highest efficiency of 6.6%.

Cavity-Enhanced Optical Readout of a Single Solid-State Spin

NASA Astrophysics Data System (ADS)

Sun, Shuo; Kim, Hyochul; Solomon, Glenn S.; Waks, Edo

2018-05-01

We demonstrate optical readout of a single spin using cavity quantum electrodynamics. The spin is based on a single trapped electron in a quantum dot that has a poor branching ratio of 0.43. Selectively coupling one of the optical transitions of the quantum dot to the cavity mode results in a spin-dependent cavity reflectivity that enables spin readout by monitoring the reflected intensity of an incident optical field. Using this approach, we demonstrate spin-readout fidelity of 0.61. Achieving this fidelity using resonance fluorescence from a bare dot would require 43 times improvement in photon collection efficiency.

Encapsulation efficiency of CdSe/ZnS quantum dots by liposomes determined by thermal lens microscopy

PubMed Central

Batalla, Jessica; Cabrera, Humberto; San Martín-Martínez, Eduardo; Korte, Dorota; Calderón, Antonio; Marín, Ernesto

2015-01-01

In this study the encapsulation of core shell carboxyl CdSe/ZnS quantum dots (QDs) by phospholipids liposome complexes is presented. It makes the quantum dots water soluble and photo-stable. Fluorescence self-quenching of the QDs inside the liposomes was observed. Therefore, the thermal lens microscopy (TLM) was found to be an useful tool for measuring the encapsulation efficiency of the QDs by the liposomes, for which an optimum value of 36% was determined. The obtained limit of detection (LOD) for determining QDs concentration by TLM was 0.13 nM. Moreover, the encapsulated QDs showed no prominent cytotoxicity toward Breast cancer cells line MDA-MB-231. This study was supported by UV-visible spectroscopy, high resolution transmission electron microscopy (HRTEM) and dynamic light scattering measurements (DLS). PMID:26504640

Multiphoton luminescent graphene quantum dots for in vivo tracking of human adipose-derived stem cells

NASA Astrophysics Data System (ADS)

Kim, Jin; Song, Sung Ho; Jin, Yoonhee; Park, Hyun-Ji; Yoon, Hyewon; Jeon, Seokwoo; Cho, Seung-Woo

2016-04-01

The applicability of graphene quantum dots (GQDs) for the in vitro and in vivo live imaging and tracking of different types of human stem cells is investigated. GQDs synthesized by the modified graphite intercalated compound method show efficient cellular uptake with improved biocompatibility and highly sensitive optical properties, indicating their feasibility as a bio-imaging probe for stem cell therapy.The applicability of graphene quantum dots (GQDs) for the in vitro and in vivo live imaging and tracking of different types of human stem cells is investigated. GQDs synthesized by the modified graphite intercalated compound method show efficient cellular uptake with improved biocompatibility and highly sensitive optical properties, indicating their feasibility as a bio-imaging probe for stem cell therapy. Electronic supplementary information (ESI) available: Additional results. See DOI: 10.1039/c6nr02143c

Quantum communication and information processing

NASA Astrophysics Data System (ADS)

Beals, Travis Roland

Quantum computers enable dramatically more efficient algorithms for solving certain classes of computational problems, but, in doing so, they create new problems. In particular, Shor's Algorithm allows for efficient cryptanalysis of many public-key cryptosystems. As public key cryptography is a critical component of present-day electronic commerce, it is crucial that a working, secure replacement be found. Quantum key distribution (QKD), first developed by C.H. Bennett and G. Brassard, offers a partial solution, but many challenges remain, both in terms of hardware limitations and in designing cryptographic protocols for a viable large-scale quantum communication infrastructure. In Part I, I investigate optical lattice-based approaches to quantum information processing. I look at details of a proposal for an optical lattice-based quantum computer, which could potentially be used for both quantum communications and for more sophisticated quantum information processing. In Part III, I propose a method for converting and storing photonic quantum bits in the internal state of periodically-spaced neutral atoms by generating and manipulating a photonic band gap and associated defect states. In Part II, I present a cryptographic protocol which allows for the extension of present-day QKD networks over much longer distances without the development of new hardware. I also present a second, related protocol which effectively solves the authentication problem faced by a large QKD network, thus making QKD a viable, information-theoretic secure replacement for public key cryptosystems.

Time reversal and charge conjugation in an embedding quantum simulator.

PubMed

Zhang, Xiang; Shen, Yangchao; Zhang, Junhua; Casanova, Jorge; Lamata, Lucas; Solano, Enrique; Yung, Man-Hong; Zhang, Jing-Ning; Kim, Kihwan

2015-08-04

A quantum simulator is an important device that may soon outperform current classical computations. A basic arithmetic operation, the complex conjugate, however, is considered to be impossible to be implemented in such a quantum system due to the linear character of quantum mechanics. Here, we present the experimental quantum simulation of such an unphysical operation beyond the regime of unitary and dissipative evolutions through the embedding of a quantum dynamics in the electronic multilevels of a (171)Yb(+) ion. We perform time reversal and charge conjugation, which are paradigmatic examples of antiunitary symmetry operators, in the evolution of a Majorana equation without the tomographic knowledge of the evolving state. Thus, these operations can be applied regardless of the system size. Our approach offers the possibility to add unphysical operations to the toolbox of quantum simulation, and provides a route to efficiently compute otherwise intractable quantities, such as entanglement monotones.

Crystal-Phase Quantum Wires: One-Dimensional Heterostructures with Atomically Flat Interfaces.

PubMed

Corfdir, Pierre; Li, Hong; Marquardt, Oliver; Gao, Guanhui; Molas, Maciej R; Zettler, Johannes K; van Treeck, David; Flissikowski, Timur; Potemski, Marek; Draxl, Claudia; Trampert, Achim; Fernández-Garrido, Sergio; Grahn, Holger T; Brandt, Oliver

2018-01-10

In semiconductor quantum-wire heterostructures, interface roughness leads to exciton localization and to a radiative decay rate much smaller than that expected for structures with flat interfaces. Here, we uncover the electronic and optical properties of the one-dimensional extended defects that form at the intersection between stacking faults and inversion domain boundaries in GaN nanowires. We show that they act as crystal-phase quantum wires, a novel one-dimensional quantum system with atomically flat interfaces. These quantum wires efficiently capture excitons whose radiative decay gives rise to an optical doublet at 3.36 eV at 4.2 K. The binding energy of excitons confined in crystal-phase quantum wires is measured to be more than twice larger than that of the bulk. As a result of their unprecedented interface quality, these crystal-phase quantum wires constitute a model system for the study of one-dimensional excitons.

Hybrid quantum gates between flying photon and diamond nitrogen-vacancy centers assisted by optical microcavities

PubMed Central

Wei, Hai-Rui; Lu Long, Gui

2015-01-01

Hybrid quantum gates hold great promise for quantum information processing since they preserve the advantages of different quantum systems. Here we present compact quantum circuits to deterministically implement controlled-NOT, Toffoli, and Fredkin gates between a flying photon qubit and diamond nitrogen-vacancy (NV) centers assisted by microcavities. The target qubits of these universal quantum gates are encoded on the spins of the electrons associated with the diamond NV centers and they have long coherence time for storing information, and the control qubit is encoded on the polarizations of the flying photon and can be easily manipulated. Our quantum circuits are compact, economic, and simple. Moreover, they do not require additional qubits. The complexity of our schemes for universal three-qubit gates is much reduced, compared to the synthesis with two-qubit entangling gates. These schemes have high fidelities and efficiencies, and they are feasible in experiment. PMID:26271899

Time reversal and charge conjugation in an embedding quantum simulator

PubMed Central

Zhang, Xiang; Shen, Yangchao; Zhang, Junhua; Casanova, Jorge; Lamata, Lucas; Solano, Enrique; Yung, Man-Hong; Zhang, Jing-Ning; Kim, Kihwan

2015-01-01

A quantum simulator is an important device that may soon outperform current classical computations. A basic arithmetic operation, the complex conjugate, however, is considered to be impossible to be implemented in such a quantum system due to the linear character of quantum mechanics. Here, we present the experimental quantum simulation of such an unphysical operation beyond the regime of unitary and dissipative evolutions through the embedding of a quantum dynamics in the electronic multilevels of a 171Yb+ ion. We perform time reversal and charge conjugation, which are paradigmatic examples of antiunitary symmetry operators, in the evolution of a Majorana equation without the tomographic knowledge of the evolving state. Thus, these operations can be applied regardless of the system size. Our approach offers the possibility to add unphysical operations to the toolbox of quantum simulation, and provides a route to efficiently compute otherwise intractable quantities, such as entanglement monotones. PMID:26239028

From transistor to trapped-ion computers for quantum chemistry.

PubMed

Yung, M-H; Casanova, J; Mezzacapo, A; McClean, J; Lamata, L; Aspuru-Guzik, A; Solano, E

2014-01-07

Over the last few decades, quantum chemistry has progressed through the development of computational methods based on modern digital computers. However, these methods can hardly fulfill the exponentially-growing resource requirements when applied to large quantum systems. As pointed out by Feynman, this restriction is intrinsic to all computational models based on classical physics. Recently, the rapid advancement of trapped-ion technologies has opened new possibilities for quantum control and quantum simulations. Here, we present an efficient toolkit that exploits both the internal and motional degrees of freedom of trapped ions for solving problems in quantum chemistry, including molecular electronic structure, molecular dynamics, and vibronic coupling. We focus on applications that go beyond the capacity of classical computers, but may be realizable on state-of-the-art trapped-ion systems. These results allow us to envision a new paradigm of quantum chemistry that shifts from the current transistor to a near-future trapped-ion-based technology.

From transistor to trapped-ion computers for quantum chemistry

PubMed Central

Yung, M.-H.; Casanova, J.; Mezzacapo, A.; McClean, J.; Lamata, L.; Aspuru-Guzik, A.; Solano, E.

2014-01-01

Over the last few decades, quantum chemistry has progressed through the development of computational methods based on modern digital computers. However, these methods can hardly fulfill the exponentially-growing resource requirements when applied to large quantum systems. As pointed out by Feynman, this restriction is intrinsic to all computational models based on classical physics. Recently, the rapid advancement of trapped-ion technologies has opened new possibilities for quantum control and quantum simulations. Here, we present an efficient toolkit that exploits both the internal and motional degrees of freedom of trapped ions for solving problems in quantum chemistry, including molecular electronic structure, molecular dynamics, and vibronic coupling. We focus on applications that go beyond the capacity of classical computers, but may be realizable on state-of-the-art trapped-ion systems. These results allow us to envision a new paradigm of quantum chemistry that shifts from the current transistor to a near-future trapped-ion-based technology. PMID:24395054

Effects of interdot hopping and Coulomb blockade on the thermoelectric properties of serially coupled quantum dots

PubMed Central

2012-01-01

We have theoretically studied the thermoelectric properties of serially coupled quantum dots (SCQDs) embedded in an insulator connected to metallic electrodes. In the framework of Keldysh Green’s function technique, the Landauer formula of transmission factor is obtained using the equation of motion method. Based on such analytical expressions of charge and heat currents, we calculate the electrical conductance, Seebeck coefficient, electron thermal conductance, and figure of merit (ZT) of SCQDs in the linear response regime. The effects of interdot hopping and electron Coulomb interactions on ZT are analyzed. We demonstrate that ZT is not a monotonic increasing function of interdot electron hopping strength (tc). We also show that in the absence of phonon thermal conductance, SCQD can reach the Carnot efficiency as tcapproaches zero. PMID:22591807

LASER APPLICATIONS AND OTHER TOPICS IN QUANTUM ELECTRONICS: Hydrodynamic efficiency of laser-induced transfer of matter

NASA Astrophysics Data System (ADS)

Isakov, Vladimir A.; Kanavin, Andrey P.; Nasibov, A. S.

2007-04-01

A one-dimensional analytic hydrodynamic model of the direct laser-induced transfer of matter is considered. The efficiency of pulsed laser radiation energy conversion to the kinetic energy of the ejected matter is determined. It is shown that the hydrodynamic efficiency of the process for the layers of matter of thickness exceeding the laser radiation absorption depth is determined by the adiabatic index of the evaporated matter.

Photonic sources and detectors for quantum information protocols: A trilogy in eight parts

NASA Astrophysics Data System (ADS)

Rangarajan, Radhika

Quantum information processing (QIP) promises to revolutionize existing methods of manipulating data, via truly unique paradigms based on fundamental nonclassical physical phenomenon. However, the eventual success of optical QIP depends critically on the available technologies. Currently, creating multiple-photon states is extremely inefficient because almost no source thus far has been well optimized. Additionally, high-efficiency single-photon detectors can drastically improve multi-photon QIP (typical efficiencies are ˜70%). In fact, it has been shown that scalable linear optical quantum computing is possible only if the product of the source and detector efficiencies exceeds ˜67%. The research presented here focuses on developing optimized source and detector technologies for enabling scalable QIP. The goal of our source research is to develop an ideal " indistinguishable" source of ultrabright polarization-entangled but spatially- and spectrally-unentangled photon pairs. We engineer such an ideal source by first designing spatio-spectrally unentangled photons using optimized and group-velocity matched spontaneous parametric down conversion (SPDC). Next, we generate polarization-entangled photons using the engineered SPDC. Here we present solutions to the various challenges encountered during the indistinguishable source development. We demonstrate high-fidelity ultrafast pulsed and cw-diode laser-pumped sources of polarization-entangled photons, as well as the first production of polarization-entanglement directly from the highly nonlinear biaxial crystal BiB3O6 (BiBO). We also discuss the first experimental confirmation of the emission-angle dependence of the downconversion polarization (the Migdall effect), and a novel scheme for polarization-dependent focusing. The goal of our single-photon detector research is to develop a very high-efficiency detection system that can also resolve incident photon number, a feature absent from the typical detectors employed for QIP. We discuss the various cryogenic, optical and electronic challenges encountered en route to detector development and present details on detector characterization, ultra-short electronics design and photon-number-resolution studies. The source and detector technologies developed here share a common goal: to enhance the efficiency of existing quantum protocols and pave the way for new ones. Here we discuss some of the possible benefits via a popular quantum protocol---teleportation---as well as a novel quantum communication technique---hyper-fingerprinting. Taken as a whole, this dissertation explores viable technological options for enhancing optical quantum information protocols, offers a perspective on the current status and limitations of existing technologies, and highlights the possibilities enabled by optimized photonic sources and detectors.

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

An efficient and accurate molecular alignment and docking technique using ab initio quality scoring

PubMed Central

Füsti-Molnár, László; Merz, Kenneth M.

2008-01-01

An accurate and efficient molecular alignment technique is presented based on first principle electronic structure calculations. This new scheme maximizes quantum similarity matrices in the relative orientation of the molecules and uses Fourier transform techniques for two purposes. First, building up the numerical representation of true ab initio electronic densities and their Coulomb potentials is accelerated by the previously described Fourier transform Coulomb method. Second, the Fourier convolution technique is applied for accelerating optimizations in the translational coordinates. In order to avoid any interpolation error, the necessary analytical formulas are derived for the transformation of the ab initio wavefunctions in rotational coordinates. The results of our first implementation for a small test set are analyzed in detail and compared with published results of the literature. A new way of refinement of existing shape based alignments is also proposed by using Fourier convolutions of ab initio or other approximate electron densities. This new alignment technique is generally applicable for overlap, Coulomb, kinetic energy, etc., quantum similarity measures and can be extended to a genuine docking solution with ab initio scoring. PMID:18624561

Development of an EMCCD for lidar applications

NASA Astrophysics Data System (ADS)

De Monte, B.; Bell, R. T.

2017-11-01

A novel detector, incorporating e2v's L3 CCD (L3Vision™) [1] technology for use in LIDAR (Light Detection And Ranging) applications has been designed, manufactured and characterised. The most critical performance aspect was the requirement to collect charge from a 120μm square detection area for a 667ns temporal sampling window, with low crosstalk between successive samples, followed by signal readout with sub-electron effective noise. Additional requirements included low dark signal, high quantum efficiency at the 355nm laser wavelength and the ability to handle bright laser echoes, without corruption of the much fainter useful signals. The detector architecture used high speed charge binning to combine signal from each sampling window into a single charge packet. This was then passed through a multiplication register (Electron Multiplying Charge Coupled Device) operating with a typical gain of 100X to a conventional charge detection circuit. The detector achieved a typical quantum efficiency of 80% and a total noise in darkness of < 0.5 electrons rms. Development of the detector was supported by ESA (European Space Agency).

RF Photoelectric injectors using needle cathodes

NASA Astrophysics Data System (ADS)

Lewellen, J. W.; Brau, C. A.

2003-07-01

Photocathode RF guns, in various configurations, are the injectors of choice for both current and future applications requiring high-brightness electron beams. Many of these applications, such as single-pass free-electron lasers, require beams with high brilliance but not necessarily high charge per bunch. Field-enhanced photoelectric emission has demonstrated electron-beam current density as high as 10 10 A/m 2, with a quantum efficiency in the UV that approaches 10% at fields on the order of 10 10 V/m. Thus, the use of even a blunt needle holds promise for increasing cathode quantum efficiency without sacrificing robustness. We present an initial study on the use of needle cathodes in photoinjectors to enhance beam brightness while reducing beam charge. Benefits include lower drive-laser power requirements, easier multibunch operation, lower emittance, and lower beam degradation due to charge-dependent effects in the postinjector accelerator. These benefits result from a combination of a smaller cathode emission area, greatly enhanced RF field strength at the cathode, and the charge scaling of detrimental postinjector linac effects, e.g., transverse wakefields and CSR.

Carnot efficiency at divergent power output

NASA Astrophysics Data System (ADS)

Polettini, Matteo; Esposito, Massimiliano

2017-05-01

The widely debated feasibility of thermodynamic machines achieving Carnot efficiency at finite power has been convincingly dismissed. Yet, the common wisdom that efficiency can only be optimal in the limit of infinitely slow processes overlooks the dual scenario of infinitely fast processes. We corroborate that efficient engines at divergent power output are not theoretically impossible, framing our claims within the theory of Stochastic Thermodynamics. We inspect the case of an electronic quantum dot coupled to three particle reservoirs to illustrate the physical rationale.

Improving Density Functionals with Quantum Harmonic Oscillators

NASA Astrophysics Data System (ADS)

Tkatchenko, Alexandre

2013-03-01

Density functional theory (DFT) is the most widely used and successful approach for electronic structure calculations. However, one of the pressing challenges for DFT is developing efficient functionals that can accurately capture the omnipresent long-range electron correlations, which determine the structure and stability of many molecules and materials. Here we show that, under certain conditions, the problem of computing the long-range correlation energy of interacting electrons can be mapped to a system of coupled quantum harmonic oscillators (QHOs). The proposed model allows us to synergistically combine concepts from DFT, quantum chemistry, and the widely discussed random-phase approximation for the correlation energy. In the dipole limit, the interaction energy for a system of coupled QHOs can be calculated exactly, thereby leading to an efficient and accurate model for the many-body dispersion energy of complex molecules and materials. The studied examples include intermolecular binding energies, the conformational hierarchy of DNA structures, the geometry and stability of molecular crystals, and supramolecular host-guest complexes (A. Tkatchenko, R. A. DiStasio Jr., R. Car, M. Scheffler, Phys. Rev. Lett. 108, 236402 (2012); R. A. DiStasio Jr., A. von Lilienfeld, A. Tkatchenko, PNAS 109, 14791 (2012); A. Tkatchenko, D. Alfe, K. S. Kim, J. Chem. Theory and Comp. (2012), doi: 10.1021/ct300711r; A. Tkatchenko, A. Ambrosetti, R. A. DiStasio Jr., arXiv:1210.8343v1).

Colossal photo-conductive gain in low temperature processed TiO2 films and their application in quantum dot solar cells

NASA Astrophysics Data System (ADS)

Mandal, Debranjan; Goswami, Prasenjit N.; Rath, Arup K.

2017-03-01

Colloidal quantum dot (QD) solar cells have seen remarkable progress in recent past to reach the certified efficiency of 10.6%. Anatase titanium oxide (TiO2) is a widely studied n-type widow layer for the collection of photogenerated electrons in QD solar cells. Requirement of high temperature (˜500 °C) processing steps proved to be disadvantageous for its applications in flexible solar cells and roll to roll processing, and it also has adverse commercial implications. Here, we report that solar light exposure to low temperature processed (80 °C-150 °C) TiO2 and niobium doped TiO2 films leads to unprecedented enhancement in their electron densities and electron mobilities, which enables them to be used as efficient n-type layers in quantum dot solar cells. Such photoinduced high conducting states in these films show gradual decay over hours after the light bias is taken off and can be retrieved under solar illumination. On the contrary, TiO2 films processed at 500 °C show marginal photo induced enhancements in their characteristics. In bilayer configuration with PbS QDs, photovoltaic devices based on low temperature processed TiO2 films show improved performance over high temperature processed TiO2 films. The stability of photovoltaic devices also improved in low temperature processed TiO2 films under ambient working conditions.

Towards Efficient and Accurate Description of Many-Electron Problems: Developments of Static and Time-Dependent Electronic Structure Methods

NASA Astrophysics Data System (ADS)

Ding, Feizhi

Understanding electronic behavior in molecular and nano-scale systems is fundamental to the development and design of novel technologies and materials for application in a variety of scientific contexts from fundamental research to energy conversion. This dissertation aims to provide insights into this goal by developing novel methods and applications of first-principle electronic structure theory. Specifically, we will present new methods and applications of excited state multi-electron dynamics based on the real-time (RT) time-dependent Hartree-Fock (TDHF) and time-dependent density functional theory (TDDFT) formalism, and new development of the multi-configuration self-consist field theory (MCSCF) for modeling ground-state electronic structure. The RT-TDHF/TDDFT based developments and applications can be categorized into three broad and coherently integrated research areas: (1) modeling of the interaction between moleculars and external electromagnetic perturbations. In this part we will first prove both analytically and numerically the gauge invariance of the TDHF/TDDFT formalisms, then we will present a novel, efficient method for calculating molecular nonlinear optical properties, and last we will study quantum coherent plasmon in metal namowires using RT-TDDFT; (2) modeling of excited-state charge transfer in molecules. In this part, we will investigate the mechanisms of bridge-mediated electron transfer, and then we will introduce a newly developed non-equilibrium quantum/continuum embedding method for studying charge transfer dynamics in solution; (3) developments of first-principles spin-dependent many-electron dynamics. In this part, we will present an ab initio non-relativistic spin dynamics method based on the two-component generalized Hartree-Fock approach, and then we will generalized it to the two-component TDDFT framework and combine it with the Ehrenfest molecular dynamics approach for modeling the interaction between electron spins and nuclear motion. All these developments and applications will open up new computational and theoretical tools to be applied to the development and understanding of chemical reactions, nonlinear optics, electromagnetism, and spintronics. Lastly, we present a new algorithm for large-scale MCSCF calculations that can utilize massively parallel machines while still maintaining optimal performance for each single processor. This will great improve the efficiency in the MCSCF calculations for studying chemical dissociation and high-accuracy quantum-mechanical simulations.

Study on photoemission surface of varied doping GaN photocathode

NASA Astrophysics Data System (ADS)

Qiao, Jianliang; Du, Ruijuan; Ding, Huan; Gao, Youtang; Chang, Benkang

2014-09-01

For varied doping GaN photocathode, from bulk to surface the doping concentrations are distributed from high to low. The varied doping GaN photocathode may produce directional inside electric field within the material, so the higher quantum efficiency can be obtained. The photoemission surface of varied doping GaN photocathode is very important to the high quantum efficiency, but the forming process of the surface state after Cs activation or Cs/O activation has been not known completely. Encircling the photoemission mechanism of varied GaN photocathode, considering the experiment phenomena during the activation and the successful activation results, the varied GaN photocathode surface model [GaN(Mg):Cs]:O-Cs after activation with cesium and oxygen was given. According to GaN photocathode activation process and the change of electronic affinity, the comparatively ideal NEA property can be achieved by Cs or Cs/O activation, and higher quantum efficiency can be obtained. The results show: The effective NEA characteristic of GaN can be gotten only by Cs. [GaN(Mg):Cs] dipoles form the first dipole layer, the positive end is toward the vacuum side. In the activation processing with Cs/O, the second dipole layer is formed by O-Cs dipoles, A O-Cs dipole includes one oxygen atom and two Cs atoms, and the positive end is also toward the vacuum side thus the escape of electrons can be promoted.

Influence of Shell Thickness on the Performance of NiO-Based All-Inorganic Quantum Dot Light-Emitting Diodes.

PubMed

Wang, Ting; Zhu, Bingyan; Wang, Shuangpeng; Yuan, Qilin; Zhang, Han; Kang, Zhihui; Wang, Rong; Zhang, Hanzhuang; Ji, Wenyu

2018-05-02

The effect of shell thickness on the performance of all-inorganic quantum dot light-emitting diodes (QLEDs) is explored by employing a series of green quantum dots (QDs) (Zn x Cd 1- x Se/ZnS core/shell QDs with different ZnS shell thicknesses) as the emitters. ZnO nanoparticles and sol-gel NiO are employed as the electron and hole transport materials, respectively. Time-resolved and steady-state photoluminescence results indicate that positive charging processes might occur for the QDs deposited on NiO, which results in emission quenching of QDs and poor device performance. The thick shell outside the core in QDs not only largely suppresses the QD emission quenching but also effectively preserves the excitons in QDs from dissociation of electron-hole pairs when they are subjected to an electric field. The peak efficiency of 4.2 cd/A and maximum luminance of 4205 cd/m 2 are achieved for the device based on QDs with the thickest shells (∼4.2 nm). We anticipate that these results will spur progress toward the design and realization of efficient all-inorganic QLEDs as a platform for the QD-based full-colored displays.

Resonance fluorescence revival in a voltage-controlled semiconductor quantum dot

NASA Astrophysics Data System (ADS)

Reigue, Antoine; Lemaître, Aristide; Gomez Carbonell, Carmen; Ulysse, Christian; Merghem, Kamel; Guilet, Stéphane; Hostein, Richard; Voliotis, Valia

2018-02-01

We demonstrate systematic resonance fluorescence recovery with near-unity emission efficiency in single quantum dots embedded in a charge-tunable device in a wave-guiding geometry. The quantum dot charge state is controlled by a gate voltage, through carrier tunneling from a close-lying Fermi sea, stabilizing the resonantly photocreated electron-hole pair. The electric field cancels out the charging/discharging mechanisms from nearby traps toward the quantum dots, responsible for the usually observed inhibition of the resonant fluorescence. Fourier transform spectroscopy as a function of the applied voltage shows a strong increase in the coherence time though not reaching the radiative limit. These charge controlled quantum dots can act as quasi-perfect deterministic single-photon emitters, with one laser pulse converted into one emitted single photon.

An Exciplex Host for Deep-Blue Phosphorescent Organic Light-Emitting Diodes.

PubMed

Lim, Hyoungcheol; Shin, Hyun; Kim, Kwon-Hyeon; Yoo, Seung-Jun; Huh, Jin-Suk; Kim, Jang-Joo

2017-11-01

The use of exciplex hosts is attractive for high-performance phosphorescent organic light-emitting diodes (PhOLEDs) and thermally activated delayed fluorescence OLEDs, which have high external quantum efficiency, low driving voltage, and low efficiency roll-off. However, exciplex hosts for deep-blue OLEDs have not yet been reported because of the difficulties in identifying suitable molecules. Here, we report a deep-blue-emitting exciplex system with an exciplex energy of 3.0 eV. It is composed of a carbazole-based hole-transporting material (mCP) and a phosphine-oxide-based electron-transporting material (BM-A10). The blue PhOLEDs exhibited maximum external quantum efficiency of 24% with CIE coordinates of (0.15, 0.21) and longer lifetime than the single host devices.

Investigation of Stability of Photosynthetic Reaction Center and Quantum Dot Hybrid Films.

PubMed

Lukashev, E P; Knox, P P; Oleinikov, I P; Seifullina, N Kh; Grishanova, N P

2016-01-01

The efficiency of interaction (efficiency of energy transfer) between various quantum dots (QDs) and photosynthetic reaction centers (RCs) from the purple bacterium Rhodobacter sphaeroides and conditions of long-term stability of functioning of such hybrid complexes in film preparations were investigated. It was found that dry films containing RCs and QDs and maintained at atmospheric humidity are capable to keep their functional activity for at least some months as judging by results of measurement of their spectral characteristics, efficiency of energy transfer from QDs to RCs, and RC electron-transport activity. Addition of trehalose to the films giving them still greater stability is especially expressed for films maintained at low humidity. These stable hybrid film structures are promising for further biotechnological studies for developing new phototransformation devices.

High efficiency spin-valve and spin-filter in a doped rhombic graphene quantum dot device

NASA Astrophysics Data System (ADS)

Silva, P. V.; Saraiva-Souza, A.; Maia, D. W.; Souza, F. M.; Filho, A. G. Souza; Meunier, V.; Girão, E. C.

2018-04-01

Spin-polarized transport through a rhombic graphene quantum dot (rGQD) attached to armchair graphene nanoribbon (AGNR) electrodes is investigated by means of the Green's function technique combined with single-band tight-binding (TB) approach including a Hubbard-like term. The Hubbard repulsion was included within the mean-field approximation. Compared to anti-ferromagnetic (AFM), we show that the ferromagnetic (FM) ordering of the rGQD corresponds to a smaller bandgap, thus resulting in an efficient spin injector. As a consequence, the electron transport spectrum reveals a spin valve effect, which is controlled by doping with B/N atoms creating a p-n-type junction. The calculations point out that such systems can be used as spin-filter devices with efficiency close to a 100 % .

Tunneling explains efficient electron transport via protein junctions.

PubMed

Fereiro, Jerry A; Yu, Xi; Pecht, Israel; Sheves, Mordechai; Cuevas, Juan Carlos; Cahen, David

2018-05-15

Metalloproteins, proteins containing a transition metal ion cofactor, are electron transfer agents that perform key functions in cells. Inspired by this fact, electron transport across these proteins has been widely studied in solid-state settings, triggering the interest in examining potential use of proteins as building blocks in bioelectronic devices. Here, we report results of low-temperature (10 K) electron transport measurements via monolayer junctions based on the blue copper protein azurin (Az), which strongly suggest quantum tunneling of electrons as the dominant charge transport mechanism. Specifically, we show that, weakening the protein-electrode coupling by introducing a spacer, one can switch the electron transport from off-resonant to resonant tunneling. This is a consequence of reducing the electrode's perturbation of the Cu(II)-localized electronic state, a pattern that has not been observed before in protein-based junctions. Moreover, we identify vibronic features of the Cu(II) coordination sphere in transport characteristics that show directly the active role of the metal ion in resonance tunneling. Our results illustrate how quantum mechanical effects may dominate electron transport via protein-based junctions.

Efficient photosensitized splitting of the thymine dimer/oxetane unit on its modifying beta-cyclodextrin by a binding electron donor.

PubMed

Tang, Wen-Jian; Song, Qin-Hua; Wang, Hong-Bo; Yu, Jing-Yu; Guo, Qing-Xiang

2006-07-07

Two modified beta-cyclodextrins (beta-CDs) with a thymine dimer and a thymine oxetane adduct respectively, TD-CD and Ox-CD, have been prepared, and utilized to bind an electron-rich chromophore, indole or N,N-dimethylaniline (DMA), to form a supramolecular complex. We have examined the photosensitized splitting of the dimer/oxetane unit in TD-CD/Ox-CD by indole or DMA via an electron-transfer pathway, and observed high splitting efficiencies of the dimer/oxetane unit. On the basis of measurements of fluorescence spectra and splitting quantum yields, it is suggested that the splitting reaction occurs in a supramolecular complex by an inclusion interaction between the modified beta-CDs and DMA or indole. The back electron transfer, which leads low splitting efficiencies for the covalently-linked chromophore-dimer/oxetane compounds, is suppressed in the non-covalently-bound complex, and the mechanism has been discussed.

External quantum efficiency exceeding 100% in a singlet-exciton-fission-based solar cell

NASA Astrophysics Data System (ADS)

Baldo, Marc

2013-03-01

Singlet exciton fission can be used to split a molecular excited state in two. In solar cells, it promises to double the photocurrent from high energy photons, thereby breaking the single junction efficiency limit. We demonstrate organic solar cells that exploit singlet exciton fission in pentacene to generate more than one electron per incident photon in the visible spectrum. Using a fullerene acceptor, a poly(3-hexylthiophene) exciton confinement layer, and a conventional optical trapping scheme, the peak external quantum efficiency is (109 +/-1)% at λ = 670 nm for a 15-nm-thick pentacene film. The corresponding internal quantum efficiency is (160 +/-10)%. Independent confirmation of the high internal efficiency is obtained by analysis of the magnetic field effect on photocurrent, which determines that the triplet yield approaches 200% for pentacene films thicker than 5 nm. To our knowledge, this is the first solar cell to generate quantum efficiencies above 100% in the visible spectrum. Alternative multiple exciton generation approaches have been demonstrated previously in the ultraviolet, where there is relatively little sunlight. Singlet exciton fission differs from these other mechanisms because spin conservation disallows the usual dominant loss process: a thermal relaxation of the high-energy exciton into a single low-energy exciton. Consequently, pentacene is efficient in the visible spectrum at λ = 670 nm because only the collapse of the singlet exciton into twotriplets is spin-allowed. Supported as part of the Center for Excitonics, an Energy Frontier Research Center funded by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences under Award Number DE-SC0001088.

Direct Observation of the Biaxial Stress Effect on Efficiency Droop in GaN-based Light-emitting Diode under Electrical Injection.

PubMed

Zheng, Jinjian; Li, Shuiqing; Chou, Chilun; Lin, Wei; Xun, Feilin; Guo, Fei; Zheng, Tongchang; Li, Shuping; Kang, Junyong

2015-12-04

Light-emitting diode (LED) efficiency has attracted considerable interest because of the extended use of solid-state lighting. Owing to lack of direct measurement, identification of the reasons for efficiency droop has been restricted. A direct measurement technique is developed in this work for characterization of biaxial stress in GaN-based blue LEDs under electrical injection. The Raman shift of the GaN E2 mode evidently decreases by 4.4 cm(-1) as the driving current on GaN-based LEDs increases to 700 mA. Biaxial compressive stress is released initially and biaxial tensile stress builds up as the current increases with respect to the value of stress-free GaN. First-principles calculations reveal that electron accumulation is responsible for the stress variation in InxGa1-xN/GaN quantum wells, and then reduces the transition probability among quantum levels. This behavior is consistent with the measured current-dependent external quantum efficiency. The rule of biaxial stress-dependent efficiency is further validated by controlling the biaxial stress of GaN-based LEDs with different sapphire substrate thicknesses. This work provides a method for direct observation of the biaxial stress effect on efficiency droop in LEDs under electrical injection.

Direct Observation of the Biaxial Stress Effect on Efficiency Droop in GaN-based Light-emitting Diode under Electrical Injection

PubMed Central

Zheng, Jinjian; Li, Shuiqing; Chou, Chilun; Lin, Wei; Xun, Feilin; Guo, Fei; Zheng, Tongchang; Li, Shuping; Kang, Junyong

2015-01-01

Light-emitting diode (LED) efficiency has attracted considerable interest because of the extended use of solid-state lighting. Owing to lack of direct measurement, identification of the reasons for efficiency droop has been restricted. A direct measurement technique is developed in this work for characterization of biaxial stress in GaN-based blue LEDs under electrical injection. The Raman shift of the GaN E2 mode evidently decreases by 4.4 cm−1 as the driving current on GaN-based LEDs increases to 700 mA. Biaxial compressive stress is released initially and biaxial tensile stress builds up as the current increases with respect to the value of stress-free GaN. First-principles calculations reveal that electron accumulation is responsible for the stress variation in InxGa1−xN/GaN quantum wells, and then reduces the transition probability among quantum levels. This behavior is consistent with the measured current-dependent external quantum efficiency. The rule of biaxial stress-dependent efficiency is further validated by controlling the biaxial stress of GaN-based LEDs with different sapphire substrate thicknesses. This work provides a method for direct observation of the biaxial stress effect on efficiency droop in LEDs under electrical injection. PMID:26634816

Photovoltaic efficiency of intermediate band solar cells based on CdTe/CdMnTe coupled quantum dots

NASA Astrophysics Data System (ADS)

Prado, Silvio J.; Marques, Gilmar E.; Alcalde, Augusto M.

2017-11-01

In this work we show the calculation of optimized efficiencies of intermediate band solar cells (IBSCs) based on Mn-doped II-VI CdTe/CdMnTe coupled quantum dot (QD) structures. We focus our attention on the combined effects of geometrical and Mn-doping parameters on optical properties and solar cell efficiency. In the framework of {k \\cdot p} theory, we accomplish detailed calculations of electronic structure, transition energies, optical selection rules and their corresponding intra- and interband oscillator strengths. With these results and by following the intermediate band model, we have developed a strategy which allows us to find optimal photovoltaic efficiency values. We also show that the effects of band admixture which can lead to degradation of optical transitions and reduction of efficiency can be partly minimized by a careful selection of the structural parameters and Mn-concentration. Thus, the improvement of band engineering is mandatory for any practical implementation of QD systems as IBSC hardware. Finally, our calculations show that it is possible to reach significant efficiency, up to  ∼26%, by selecting a restricted space of parameters such as quantum dot size and shape and Mn-concentration effects, to improve the modulation of optical absorption in the structures.

Photovoltaic efficiency of intermediate band solar cells based on CdTe/CdMnTe coupled quantum dots.

PubMed

Prado, Silvio J; Marques, Gilmar E; Alcalde, Augusto M

2017-11-08

In this work we show the calculation of optimized efficiencies of intermediate band solar cells (IBSCs) based on Mn-doped II-VI CdTe/CdMnTe coupled quantum dot (QD) structures. We focus our attention on the combined effects of geometrical and Mn-doping parameters on optical properties and solar cell efficiency. In the framework of [Formula: see text] theory, we accomplish detailed calculations of electronic structure, transition energies, optical selection rules and their corresponding intra- and interband oscillator strengths. With these results and by following the intermediate band model, we have developed a strategy which allows us to find optimal photovoltaic efficiency values. We also show that the effects of band admixture which can lead to degradation of optical transitions and reduction of efficiency can be partly minimized by a careful selection of the structural parameters and Mn-concentration. Thus, the improvement of band engineering is mandatory for any practical implementation of QD systems as IBSC hardware. Finally, our calculations show that it is possible to reach significant efficiency, up to  ∼26%, by selecting a restricted space of parameters such as quantum dot size and shape and Mn-concentration effects, to improve the modulation of optical absorption in the structures.

Effects of electron transport material on blue organ light-emitting diode with fluorescent dopant of BCzVBi.

PubMed

Meng, Mei; Song, Wook; Kim, You-Hyun; Lee, Sang-Youn; Jhun, Chul-Gyu; Zhu, Fu Rong; Ryu, Dae Hyun; Kim, Woo-Young

2013-01-01

High efficiency blue organic light emitting diodes (OLEDs), based on 2-me-thyl-9,10-di(2-naphthyl) anthracene (MADN) doped with 4,4'-bis(9-ethyl-3-carbazovinylene)-1,1'-biphenyl (BCzVBi), were fabricated using two different electron transport layers (ETLs) of tris(8-hydroxyquinolino)-aluminum (Alq3) and 4,7-di-phenyl-1,10-phenanthroline (Bphen). Bphen ETL layers favored the efficient hole-electron recombination in the emissive layer of the BCzVBi-doped blue OLEDs, leading to high luminous efficiency and quantum efficiency of 8.34 cd/A at 100 mA/cm2 and 5.73% at 100 cd/m2, respectively. Maximum luminance of blue OLED with Bphen ETL and Alq3 ETL were 10670 cd/m2, and CIExy coordinates of blue OLEDs were (0.180, 0279) and (0.155, 0.212) at 100 cd/m2.

Novel Design of Iridium Phosphors with Pyridinylphosphinate Ligands for High-Efficiency Blue Organic Light-emitting Diodes

PubMed Central

Wu, Zheng-Guang; Jing, Yi-Ming; Lu, Guang-Zhao; Zhou, Jie; Zheng, You-Xuan; Zhou, Liang; Wang, Yi; Pan, Yi

2016-01-01

Due to the high quantum efficiency and wide scope of emission colors, iridium (Ir) (III) complexes have been widely applied as guest materials for OLEDs (organic light-emitting diodes). Contrary to well-developed Ir(III)-based red and green phosphorescent complexes, the efficient blue emitters are rare reported. Like the development of the LED, the absence of efficient and stable blue materials hinders the widely practical application of the OLEDs. Inspired by this, we designed two novel ancillary ligands of phenyl(pyridin-2-yl)phosphinate (ppp) and dipyridinylphosphinate (dpp) for efficient blue phosphorescent iridium complexes (dfppy)2Ir(ppp) and (dfppy)2Ir(dpp) (dfppy = 2-(2,4-difluorophenyl)pyridine) with good electron transport property. The devices using the new iridium phosphors display excellent electroluminescence (EL) performances with a peak current efficiency of 58.78 cd/A, a maximum external quantum efficiency of 28.3%, a peak power efficiency of 52.74 lm/W and negligible efficiency roll-off ratios. The results demonstrated that iridium complexes with pyridinylphosphinate ligands are potential blue phosphorescent materials for OLEDs. PMID:27929124

Hot carrier-enhanced interlayer electron-hole pair multiplication in 2D semiconductor heterostructure photocells

NASA Astrophysics Data System (ADS)

Barati, Fatemeh; Grossnickle, Max; Su, Shanshan; Lake, Roger K.; Aji, Vivek; Gabor, Nathaniel M.

2017-12-01

Strong electronic interactions can result in novel particle-antiparticle (electron-hole, e-h) pair generation effects, which may be exploited to enhance the photoresponse of nanoscale optoelectronic devices. Highly efficient e-h pair multiplication has been demonstrated in several important nanoscale systems, including nanocrystal quantum dots, carbon nanotubes and graphene. The small Fermi velocity and nonlocal nature of the effective dielectric screening in ultrathin layers of transition-metal dichalcogenides (TMDs) indicates that e-h interactions are very strong, so high-efficiency generation of e-h pairs from hot electrons is expected. However, such e-h pair multiplication has not been observed in 2D TMD devices. Here, we report the highly efficient multiplication of interlayer e-h pairs in 2D semiconductor heterostructure photocells. Electronic transport measurements of the interlayer I-VSD characteristics indicate that layer-indirect e-h pairs are generated by hot-electron impact excitation at temperatures near T = 300 K. By exploiting this highly efficient interlayer e-h pair multiplication process, we demonstrate near-infrared optoelectronic devices that exhibit 350% enhancement of the optoelectronic responsivity at microwatt power levels. Our findings, which demonstrate efficient carrier multiplication in TMD-based optoelectronic devices, make 2D semiconductor heterostructures viable for a new class of ultra-efficient photodetectors based on layer-indirect e-h excitations.

X-ray imaging using avalanche multiplication in amorphous selenium: investigation of intrinsic avalanche noise.

PubMed

Hunt, D C; Tanioka, Kenkichi; Rowlands, J A

2007-12-01

The flat-panel detector (FPD) is the state-of-the-art detector for digital radiography. The FPD can acquire images in real-time, has superior spatial resolution, and is free of the problems of x-ray image intensifiers-veiling glare, pin-cushion and magnetic distortion. However, FPDs suffer from poor signal to noise ratio performance at typical fluoroscopic exposure rates where the quantum noise is reduced to the point that it becomes comparable to the fixed electronic noise. It has been shown previously that avalanche multiplication gain in amorphous selenium (a-Se) can provide the necessary amplification to overcome the electronic noise of the FPD. Avalanche multiplication, however, comes with its own intrinsic contribution to the noise in the form of gain fluctuation noise. In this article a cascaded systems analysis is used to present a modified metric related to the detective quantum efficiency. The modified metric is used to study a diagnostic x-ray imaging system in the presence of intrinsic avalanche multiplication noise independently from other noise sources, such as electronic noise. An indirect conversion imaging system is considered to make the study independent of other avalanche multiplication related noise sources, such as the fluctuations arising from the depth of x-ray absorption. In this case all the avalanche events are initiated at the surface of the avalanche layer, and there are no fluctuations in the depth of absorption. Experiments on an indirect conversion x-ray imaging system using avalanche multiplication in a layer of a-Se are also presented. The cascaded systems analysis shows that intrinsic noise of avalanche multiplication will not have any deleterious influence on detector performance at zero spatial frequency in x-ray imaging provided the product of conversion gain, coupling efficiency, and optical quantum efficiency are much greater than a factor of 2. The experimental results show that avalanche multiplication in a-Se behaves as an intrinsic noise free avalanche multiplication, in accordance with our theory. Provided good coupling efficiency and high optical quantum efficiency are maintained, avalanche multiplication in a-Se has the potential to increase the gain and make negligible contribution to the noise, thereby improving the performance of indirect FPDs in fluoroscopy.

X-ray imaging using avalanche multiplication in amorphous selenium: Investigation of intrinsic avalanche noise

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

Hunt, D. C.; Tanioka, Kenkichi; Rowlands, J. A.

2007-12-15

The flat-panel detector (FPD) is the state-of-the-art detector for digital radiography. The FPD can acquire images in real-time, has superior spatial resolution, and is free of the problems of x-ray image intensifiers--veiling glare, pin-cushion and magnetic distortion. However, FPDs suffer from poor signal to noise ratio performance at typical fluoroscopic exposure rates where the quantum noise is reduced to the point that it becomes comparable to the fixed electronic noise. It has been shown previously that avalanche multiplication gain in amorphous selenium (a-Se) can provide the necessary amplification to overcome the electronic noise of the FPD. Avalanche multiplication, however, comesmore » with its own intrinsic contribution to the noise in the form of gain fluctuation noise. In this article a cascaded systems analysis is used to present a modified metric related to the detective quantum efficiency. The modified metric is used to study a diagnostic x-ray imaging system in the presence of intrinsic avalanche multiplication noise independently from other noise sources, such as electronic noise. An indirect conversion imaging system is considered to make the study independent of other avalanche multiplication related noise sources, such as the fluctuations arising from the depth of x-ray absorption. In this case all the avalanche events are initiated at the surface of the avalanche layer, and there are no fluctuations in the depth of absorption. Experiments on an indirect conversion x-ray imaging system using avalanche multiplication in a layer of a-Se are also presented. The cascaded systems analysis shows that intrinsic noise of avalanche multiplication will not have any deleterious influence on detector performance at zero spatial frequency in x-ray imaging provided the product of conversion gain, coupling efficiency, and optical quantum efficiency are much greater than a factor of 2. The experimental results show that avalanche multiplication in a-Se behaves as an intrinsic noise free avalanche multiplication, in accordance with our theory. Provided good coupling efficiency and high optical quantum efficiency are maintained, avalanche multiplication in a-Se has the potential to increase the gain and make negligible contribution to the noise, thereby improving the performance of indirect FPDs in fluoroscopy.« less

Direct evaluation of boson dynamics via finite-temperature time-dependent variation with multiple Davydov states.

PubMed

Fujihashi, Yuta; Wang, Lu; Zhao, Yang

2017-12-21

Recent advances in quantum optics allow for exploration of boson dynamics in dissipative many-body systems. However, the traditional descriptions of quantum dissipation using reduced density matrices are unable to capture explicit information of bath dynamics. In this work, efficient evaluation of boson dynamics is demonstrated by combining the multiple Davydov Ansatz with finite-temperature time-dependent variation, going beyond what state-of-the-art density matrix approaches are capable to offer for coupled electron-boson systems. To this end, applications are made to excitation energy transfer in photosynthetic systems, singlet fission in organic thin films, and circuit quantum electrodynamics in superconducting devices. Thanks to the multiple Davydov Ansatz, our analysis of boson dynamics leads to clear revelation of boson modes strongly coupled to electronic states, as well as in-depth description of polaron creation and destruction in the presence of thermal fluctuations.

Preparation and photovoltaic properties of CdS quantum dot-sensitized solar cell based on zinc tin mixed metal oxides.

PubMed

Cao, Jiupeng; Zhao, Yifan; Zhu, Yatong; Yang, Xiaoyu; Shi, Peng; Xiao, Hongdi; Du, Na; Hou, Wanguo; Qi, Genggeng; Liu, Jianqiang

2017-07-15

The present study reports a new type of quantum dot sensitized solar cells (QDSSCs) using the zinc tin mixed metal oxides (MMO) as the anode materials, which were obtained from the layered double hydroxide (LDH) precursor. The successive ionic layer adsorption and reaction (SILAR) method is applied to deposit CdS quantum dots. The effects of sensitizing cycles on the performance of CdS QDSSC are studied. Scanning electron microscopy (SEM), Transmission electron microscope (TEM) and X-ray diffraction (XRD) are used to identify the surface profile and crystal structure of the mixed metal oxides anode. The photovoltaic performance of the QDSSC is studied by the electrochemical method. The new CdS QDSSC exhibits power conversion efficiency (PCE) up to 0.48% when the anode was sensitized for eight cycles. Copyright © 2017 Elsevier Inc. All rights reserved.

High efficiency III-nitride light-emitting diodes

DOEpatents

Crawford, Mary; Koleske, Daniel; Cho, Jaehee; Zhu, Di; Noemaun, Ahmed; Schubert, Martin F; Schubert, E. Fred

2013-05-28

Tailored doping of barrier layers enables balancing of the radiative recombination among the multiple-quantum-wells in III-Nitride light-emitting diodes. This tailored doping enables more symmetric carrier transport and uniform carrier distribution which help to reduce electron leakage and thus reduce the efficiency droop in high-power III-Nitride LEDs. Mitigation of the efficiency droop in III-Nitride LEDs may enable the pervasive market penetration of solid-state-lighting technologies in high-power lighting and illumination.

Interfacial Charge Transfer States in Condensed Phase Systems

NASA Astrophysics Data System (ADS)

Vandewal, Koen

2016-05-01

Intermolecular charge transfer (CT) states at the interface between electron-donating (D) and electron-accepting (A) materials in organic thin films are characterized by absorption and emission bands within the optical gap of the interfacing materials. CT states efficiently generate charge carriers for some D-A combinations, and others show high fluorescence quantum efficiencies. These properties are exploited in organic solar cells, photodetectors, and light-emitting diodes. This review summarizes experimental and theoretical work on the electronic structure and interfacial energy landscape at condensed matter D-A interfaces. Recent findings on photogeneration and recombination of free charge carriers via CT states are discussed, and relations between CT state properties and optoelectronic device parameters are clarified.

Laser program. Annual report, 1978

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

Monsler, M.J.; Jarman, B.D.

1979-03-01

This volume documents progress in advanced quantum electronics - primarily the quest for advanced rep-rateable short-wavelength lasers with high efficiency. Application studies in electrical energy production and fissile fuel production are also described. Selected highlights of the advanced isotope separation program are also presented. (MOW)

Carbon quantum dots coated BiVO{sub 4} inverse opals for enhanced photoelectrochemical hydrogen generation

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

Nan, Feng; Shen, Mingrong; Fang, Liang, E-mail: zhkang@suda.edu.cn, E-mail: lfang@suda.edu.cn

Carbon quantum dots (CQDs) coated BiVO{sub 4} inverse opal (io-BiVO{sub 4}) structure that shows dramatic improvement of photoelectrochemical hydrogen generation has been fabricated using electrodeposition with a template. The io-BiVO{sub 4} maximizes photon trapping through slow light effect, while maintaining adequate surface area for effective redox reactions. CQDs are then incorporated to the io-BiVO{sub 4} to further improve the photoconversion efficiency. Due to the strong visible light absorption property of CQDs and enhanced separation of the photoexcited electrons, the CQDs coated io-BiVO{sub 4} exhibit a maximum photo-to-hydrogen conversion efficiency of 0.35%, which is 6 times higher than that of themore » pure BiVO{sub 4} thin films. This work is a good example of designing composite photoelectrode by combining quantum dots and photonic crystal.« less

Giant photocurrent enhancement by transition metal doping in quantum dot sensitized solar cells

NASA Astrophysics Data System (ADS)

Rimal, Gaurab; Pimachev, Artem K.; Yost, Andrew J.; Poudyal, Uma; Maloney, Scott; Wang, Wenyong; Chien, TeYu; Dahnovsky, Yuri; Tang, Jinke

2016-09-01

A huge enhancement in the incident photon-to-current efficiency of PbS quantum dot (QD) sensitized solar cells by manganese doping is observed. In the presence of Mn dopants with relatively small concentration (4 at. %), the photoelectric current increases by an average of 300% (up to 700%). This effect cannot be explained by the light absorption mechanism because both the experimental and theoretical absorption spectra demonstrate several times decreases in the absorption coefficient. To explain such dramatic increase in the photocurrent we propose the electron tunneling mechanism from the LUMO of the QD excited state to the Zn2SnO4 (ZTO) semiconductor photoanode. This change is due to the presence of the Mn instead of Pb atom at the QD/ZTO interface. The ab initio calculations confirm this mechanism. This work proposes an alternative route for a significant improvement of the efficiency for quantum dot sensitized solar cells.

Thermoelectric properties of periodic quantum structures in the Wigner-Rode formalism

NASA Astrophysics Data System (ADS)

Kommini, Adithya; Aksamija, Zlatan

2018-01-01

Improving the thermoelectric Seebeck coefficient, while simultaneously reducing thermal conductivity, is required in order to boost thermoelectric (TE) figure of merit (ZT). A common approach to improve the Seebeck coefficient is electron filtering where ‘cold’ (low energy) electrons are restricted from participating in transport by an energy barrier (Kim and Lundstrom 2011 J. Appl. Phys. 110 034511, Zide et al 2010 J. Appl. Phys. 108 123702). However, the impact of electron tunneling through thin barriers and resonant states on TE properties has been given less attention, despite the widespread use of quantum wells and superlattices (SLs) in TE applications. In our work, we develop a comprehensive transport model using the Wigner-Rode formalism. We include the full electronic bandstructure and all the relevant scattering mechanisms, allowing us to simulate both energy relaxation and quantum effects from periodic potential barriers. We study the impact of barrier shape on TE performance and find that tall, sharp barriers with small period lengths lead to the largest increase in both Seebeck coefficient and conductivity, thus boosting power factor and TE efficiency. Our findings are robust against additional elastic scattering such as atomic-scale roughness at side-walls of SL nanowires.

Ultrafast terahertz snapshots of excitonic Rydberg states and electronic coherence in an organometal halide perovskite

DOE PAGES

Luo, Liang; Men, Long; Liu, Zhaoyu; ...

2017-06-01

How photoexcitations evolve into Coulomb-bound electron and hole pairs, called excitons, and unbound charge carriers is a key cross-cutting issue in photovoltaics and optoelectronics. Until now, the initial quantum dynamics following photoexcitation remains elusive in the hybrid perovskite system. Furthermore we reveal excitonic Rydberg states with distinct formation pathways by observing the multiple resonant, internal quantum transitions using ultrafast terahertz quasi-particle transport. Nonequilibrium emergent states evolve with a complex co-existence of excitons, carriers and phonons, where a delayed buildup of excitons under on- and off-resonant pumping conditions allows us to distinguish between the loss of electronic coherence and hot statemore » cooling processes. The nearly ~1 ps dephasing time, efficient electron scattering with discrete terahertz phonons and intermediate binding energy of ~13.5 meV in perovskites are distinct from conventional photovoltaic semiconductors. In addition to providing implications for coherent energy conversion, these are potentially relevant to the development of light-harvesting and electron-transport devices.« less

Ultrafast terahertz snapshots of excitonic Rydberg states and electronic coherence in an organometal halide perovskite

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

Luo, Liang; Men, Long; Liu, Zhaoyu

How photoexcitations evolve into Coulomb-bound electron and hole pairs, called excitons, and unbound charge carriers is a key cross-cutting issue in photovoltaics and optoelectronics. Until now, the initial quantum dynamics following photoexcitation remains elusive in the hybrid perovskite system. Furthermore we reveal excitonic Rydberg states with distinct formation pathways by observing the multiple resonant, internal quantum transitions using ultrafast terahertz quasi-particle transport. Nonequilibrium emergent states evolve with a complex co-existence of excitons, carriers and phonons, where a delayed buildup of excitons under on- and off-resonant pumping conditions allows us to distinguish between the loss of electronic coherence and hot statemore » cooling processes. The nearly ~1 ps dephasing time, efficient electron scattering with discrete terahertz phonons and intermediate binding energy of ~13.5 meV in perovskites are distinct from conventional photovoltaic semiconductors. In addition to providing implications for coherent energy conversion, these are potentially relevant to the development of light-harvesting and electron-transport devices.« less

Efficient grid-based techniques for density functional theory

NASA Astrophysics Data System (ADS)

Rodriguez-Hernandez, Juan Ignacio

Understanding the chemical and physical properties of molecules and materials at a fundamental level often requires quantum-mechanical models for these substance's electronic structure. This type of many body quantum mechanics calculation is computationally demanding, hindering its application to substances with more than a few hundreds atoms. The supreme goal of many researches in quantum chemistry---and the topic of this dissertation---is to develop more efficient computational algorithms for electronic structure calculations. In particular, this dissertation develops two new numerical integration techniques for computing molecular and atomic properties within conventional Kohn-Sham-Density Functional Theory (KS-DFT) of molecular electronic structure. The first of these grid-based techniques is based on the transformed sparse grid construction. In this construction, a sparse grid is generated in the unit cube and then mapped to real space according to the pro-molecular density using the conditional distribution transformation. The transformed sparse grid was implemented in program deMon2k, where it is used as the numerical integrator for the exchange-correlation energy and potential in the KS-DFT procedure. We tested our grid by computing ground state energies, equilibrium geometries, and atomization energies. The accuracy on these test calculations shows that our grid is more efficient than some previous integration methods: our grids use fewer points to obtain the same accuracy. The transformed sparse grids were also tested for integrating, interpolating and differentiating in different dimensions (n = 1,2,3,6). The second technique is a grid-based method for computing atomic properties within QTAIM. It was also implemented in deMon2k. The performance of the method was tested by computing QTAIM atomic energies, charges, dipole moments, and quadrupole moments. For medium accuracy, our method is the fastest one we know of.

Enhanced charge carrier transport properties in colloidal quantum dot solar cells via organic and inorganic hybrid surface passivation† †Electronic supplementary information (ESI) available. See DOI: 10.1039/c6ta06835a Click here for additional data file.

PubMed Central

Hong, John; Hou, Bo; Lim, Jongchul; Pak, Sangyeon; Kim, Byung-Sung; Cho, Yuljae; Lee, Juwon; Lee, Young-Woo; Giraud, Paul; Lee, Sanghyo; Park, Jong Bae; Morris, Stephen M.; Snaith, Henry J.; Kim, Jong Min

2016-01-01

Colloidal quantum dots (CQDs) are extremely promising as photovoltaic materials. In particular, the tunability of their electronic band gap and cost effective synthetic procedures allow for the versatile fabrication of solar energy harvesting cells, resulting in optimal device performance. However, one of the main challenges in developing high performance quantum dot solar cells (QDSCs) is the improvement of the photo-generated charge transport and collection, which is mainly hindered by imperfect surface functionalization, such as the presence of surface electronic trap sites and the initial bulky surface ligands. Therefore, for these reasons, finding effective methods to efficiently decorate the surface of the as-prepared CQDs with new short molecular length chemical structures so as to enhance the performance of QDSCs is highly desirable. Here, we suggest employing hybrid halide ions along with the shortest heterocyclic molecule as a robust passivation structure to eliminate surface trap sites while decreasing the charge trapping dynamics and increasing the charge extraction efficiency in CQD active layers. This hybrid ligand treatment shows a better coordination with Pb atoms within the crystal, resulting in low trap sites and a near perfect removal of the pristine initial bulky ligands, thereby achieving better conductivity and film structure. Compared to halide ion-only treated cells, solar cells fabricated through this hybrid passivation method show an increase in the power conversion efficiency from 5.3% for the halide ion-treated cells to 6.8% for the hybrid-treated solar cells. PMID:29308200

Ultra low emittance electron beams from multi-alkali antimonide photocathode operated with infrared light

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

Cultrera, L.; Gulliford, C.; Bartnik, A.

2016-03-28

The intrinsic emittance of electron beams generated from a multi-alkali photocathode operated in a high voltage DC gun is reported. The photocathode showed sensitivity extending to the infrared part of the spectrum up to 830 nm. The measured intrinsic emittances of electron beams generated with light having wavelength longer than 800 nm are approaching the limit imposed by the thermal energy of electrons at room temperature with quantum efficiencies comparable to metallic photocathodes used in operation of modern photoinjectors.

Characteristics of gradient-interface-structured ZnCdSSe quantum dots with modified interface and its application to quantum-dot-sensitized solar cells

NASA Astrophysics Data System (ADS)

Jeong, Da-Woon; Kim, Jae-Yup; Seo, Han Wook; Lim, Kyoung-Mook; Ko, Min Jae; Seong, Tae-Yeon; Kim, Bum Sung

2018-01-01

Colloidal quantum dots (QDs) are attractive materials for application in photovoltaics, LEDs, displays, and bio devices owing to their unique properties. In this study, we synthesized gradient-interface-structured ZnCdSSe QDs and modified the interface based on a thermodynamic simulation to investigate its optical and physical properties. In addition, the interface was modified by increasing the molar concentration of Se. QDs at the modified interface were applied to QD-sensitized solar cells, which showed a 25.5% increase in photoelectric conversion efficiency owing to the reduced electron confinement effect. The increase seems to be caused by the excited electrons being relatively easily transferred to the level of TiO2 owing to the reduced electron confinement effect. Consequently, the electron confinement effect was observed to be reduced by increasing the ZnSe (or Zn1-xCdxSe)-rich phase at the interface. This means that, based on the thermodynamic simulation, the interface between the core QDs and the surface of the QDs can be controlled. The improvement of optical and electronic properties by controlling interfaces and surfaces during the synthesis of QDs, as reported in this work, can be useful for many applications beyond solar cells.

InGaN stress compensation layers in InGaN/GaN blue LEDs with step graded electron injectors

NASA Astrophysics Data System (ADS)

Sheremet, V.; Gheshlaghi, N.; Sözen, M.; Elçi, M.; Sheremet, N.; Aydınlı, A.; Altuntaş, I.; Ding, K.; Avrutin, V.; Özgür, Ü.; Morkoç, H.

2018-04-01

We investigate the effect of InGaN stress compensation layer on the properties of light emitting diodes based on InGaN/GaN multiple quantum well (MQW) structures with step-graded electron injectors. Insertion of an InGaN stress compensation layer between n-GaN and the step graded electron injector provides, among others, strain reduction in the MQW region and as a result improves epitaxial quality that can be observed by 15-fold decrease of V-pit density. We observed more uniform distribution of In between quantum wells in MQW region from results of electro- and photoluminescence measurement. These structural improvements lead to increasing of radiant intensity by a factor of 1.7-2.0 and enhancement of LED efficiency by 40%.

Microscopic nonlinear relativistic quantum theory of absorption of powerful x-ray radiation in plasma.

PubMed

Avetissian, H K; Ghazaryan, A G; Matevosyan, H H; Mkrtchian, G F

2015-10-01

The microscopic quantum theory of plasma nonlinear interaction with the coherent shortwave electromagnetic radiation of arbitrary intensity is developed. The Liouville-von Neumann equation for the density matrix is solved analytically considering a wave field exactly and a scattering potential of plasma ions as a perturbation. With the help of this solution we calculate the nonlinear inverse-bremsstrahlung absorption rate for a grand canonical ensemble of electrons. The latter is studied in Maxwellian, as well as in degenerate quantum plasma for x-ray lasers at superhigh intensities and it is shown that one can achieve the efficient absorption coefficient in these cases.

Processing of fullerene-single wall carbon nanotube complex for bulk heterojunction photovoltaic cells

NASA Astrophysics Data System (ADS)

Li, Cheng; Mitra, Somenath

2007-12-01

A fullerene-single wall carbon nanotube (C60-SWCNT) complex is used as a component of the photoactive layer in bulk heterojunction photovoltaic cells. This complex synthesized by microwave-assisted reaction takes advantage of the electron accepting feature of C60 and the high electron transport capability of SWCNTs. In this paper, quantum efficiency enhancement by increasing light absorption and by bringing about appropriate morphological rearrangements via solvent vapor treatment and thermal annealing is presented. The optimum combination of these steps led to an increase in efficiency by as much as 87.5%.

Toward prethreshold gate-based quantum simulation of chemical dynamics: using potential energy surfaces to simulate few-channel molecular collisions

DOE PAGES

Sornborger, Andrew Tyler; Stancil, Phillip; Geller, Michael R.

2018-03-22

Here, one of the most promising applications of an error-corrected universal quantum computer is the efficient simulation of complex quantum systems such as large molecular systems. In this application, one is interested in both the electronic structure such as the ground state energy and dynamical properties such as the scattering cross section and chemical reaction rates. However, most theoretical work and experimental demonstrations have focused on the quantum computation of energies and energy surfaces. In this work, we attempt to make the prethreshold (not error-corrected) quantum simulation of dynamical properties practical as well. We show that the use of precomputedmore » potential energy surfaces and couplings enables the gate-based simulation of few-channel but otherwise realistic molecular collisions. Our approach is based on the widely used Born–Oppenheimer approximation for the structure problem coupled with a semiclassical method for the dynamics. In the latter the electrons are treated quantum mechanically but the nuclei are classical, which restricts the collisions to high energy or temperature (typically above ≈10 eV). By using operator splitting techniques optimized for the resulting time-dependent Hamiltonian simulation problem, we give several physically realistic collision examples, with 3–8 channels and circuit depths < 1000.« less

Toward prethreshold gate-based quantum simulation of chemical dynamics: using potential energy surfaces to simulate few-channel molecular collisions

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

Sornborger, Andrew Tyler; Stancil, Phillip; Geller, Michael R.

Here, one of the most promising applications of an error-corrected universal quantum computer is the efficient simulation of complex quantum systems such as large molecular systems. In this application, one is interested in both the electronic structure such as the ground state energy and dynamical properties such as the scattering cross section and chemical reaction rates. However, most theoretical work and experimental demonstrations have focused on the quantum computation of energies and energy surfaces. In this work, we attempt to make the prethreshold (not error-corrected) quantum simulation of dynamical properties practical as well. We show that the use of precomputedmore » potential energy surfaces and couplings enables the gate-based simulation of few-channel but otherwise realistic molecular collisions. Our approach is based on the widely used Born–Oppenheimer approximation for the structure problem coupled with a semiclassical method for the dynamics. In the latter the electrons are treated quantum mechanically but the nuclei are classical, which restricts the collisions to high energy or temperature (typically above ≈10 eV). By using operator splitting techniques optimized for the resulting time-dependent Hamiltonian simulation problem, we give several physically realistic collision examples, with 3–8 channels and circuit depths < 1000.« less

Toward prethreshold gate-based quantum simulation of chemical dynamics: using potential energy surfaces to simulate few-channel molecular collisions

NASA Astrophysics Data System (ADS)

Sornborger, Andrew T.; Stancil, Phillip; Geller, Michael R.

2018-05-01

One of the most promising applications of an error-corrected universal quantum computer is the efficient simulation of complex quantum systems such as large molecular systems. In this application, one is interested in both the electronic structure such as the ground state energy and dynamical properties such as the scattering cross section and chemical reaction rates. However, most theoretical work and experimental demonstrations have focused on the quantum computation of energies and energy surfaces. In this work, we attempt to make the prethreshold (not error-corrected) quantum simulation of dynamical properties practical as well. We show that the use of precomputed potential energy surfaces and couplings enables the gate-based simulation of few-channel but otherwise realistic molecular collisions. Our approach is based on the widely used Born-Oppenheimer approximation for the structure problem coupled with a semiclassical method for the dynamics. In the latter the electrons are treated quantum mechanically but the nuclei are classical, which restricts the collisions to high energy or temperature (typically above ≈ 10 eV). By using operator splitting techniques optimized for the resulting time-dependent Hamiltonian simulation problem, we give several physically realistic collision examples, with 3-8 channels and circuit depths < 1000.

Evaluation of the basic propertied of the novel 1.5 in. size PMTs from Hamamatsu Photonics and Electron Tubes Enterprises

NASA Astrophysics Data System (ADS)

Toyama, T.; Hanabata, Y.; Hose, J.; Menzel, U.; Mirzoyan, R.; Nakajima, D.; Takahashi, M.; Teshima, M.; Yamamoto, T.

2015-07-01

Currently the standard light sensors for Imaging Atmospheric Cherenkov Telescopes are the classical photo multiplier tubes that are using bialkali photocathodes. About 8 years ago we initiated an improvement program with the Photo Multiplier Tube manufacturers Hamamatsu in Japan, Electron Tubes Enterprises in England and Photonis in France for the needs of Imaging Atmospheric Cherenkov Telescopes. As a result, after about 40 years of "stagnation" of the peak Quantum Efficiency on the level of 25-27%, new PMTs appeared with a peak QE of 35%. These have got the name "super-bialkali". The second significant upgrade has happened very recently, as a result of a dedicated improvement program for the candidate PMT for Cherenkov Telescope Array. The latter is going to be the next generation major instrument in the field of very high energy gamma astrophysics and will consist of over 100 telescopes of three different sizes of 23 m, 12 m and 4-7 m. Now PMTs with average peak Quantum Efficiency of approximately 40% became available. Also, the photo electron collection efficiency of the previous generation PMTs of 80-90% has been enhanced towards 95-98% for the new ones. The after-pulsing of novel PMTs has been reduced towards the level of 0.02% for the set threshold of 4 photo electrons. Hamamatsu produced the PMT R-12992-100 as the final version for Cherenkov Telescope Array project. Electron Tubes produced the latest PMT D569/3SA as intermediate version and will produce the final version in 2015. We will report on the PMT development work by the companies Electron Tubes Enterprises and Hamamatsu Photonics K.K., show the achieved results and the current status.

Investigation of p-type depletion doping for InGaN/GaN-based light-emitting diodes

NASA Astrophysics Data System (ADS)

Zhang, Yiping; Zhang, Zi-Hui; Tan, Swee Tiam; Hernandez-Martinez, Pedro Ludwig; Zhu, Binbin; Lu, Shunpeng; Kang, Xue Jun; Sun, Xiao Wei; Demir, Hilmi Volkan

2017-01-01

Due to the limitation of the hole injection, p-type doping is essential to improve the performance of InGaN/GaN multiple quantum well light-emitting diodes (LEDs). In this work, we propose and show a depletion-region Mg-doping method. Here we systematically analyze the effectiveness of different Mg-doping profiles ranging from the electron blocking layer to the active region. Numerical computations show that the Mg-doping decreases the valence band barrier for holes and thus enhances the hole transportation. The proposed depletion-region Mg-doping approach also increases the barrier height for electrons, which leads to a reduced electron overflow, while increasing the hole concentration in the p-GaN layer. Experimentally measured external quantum efficiency indicates that Mg-doping position is vitally important. The doping in or adjacent to the quantum well degrades the LED performance due to Mg diffusion, increasing the corresponding nonradiative recombination, which is well supported by the measured carrier lifetimes. The experimental results are well numerically reproduced by modifying the nonradiative recombination lifetimes, which further validate the effectiveness of our approach.

New Antimony Selenide/Nickel Oxide Photocathode Boosts the Efficiency of Graphene Quantum-Dot Co-Sensitized Solar Cells.

PubMed

Kolay, Ankita; Kokal, Ramesh K; Kalluri, Ankarao; Macwan, Isaac; Patra, Prabir K; Ghosal, Partha; Deepa, Melepurath

2017-10-11

A novel assembly of a photocathode and a photoanode is investigated to explore their complementary effects in enhancing the photovoltaic performance of a quantum-dot solar cell (QDSC). While p-type nickel oxide (NiO) has been used previously, antimony selenide (Sb 2 Se 3 ) has not been used in a QDSC, especially as a component of a counter electrode (CE) architecture that doubles as the photocathode. Here, near-infrared (NIR) light-absorbing Sb 2 Se 3 nanoparticles (NPs) coated over electrodeposited NiO nanofibers on a carbon (C) fabric substrate was employed as the highly efficient photocathode. Quasi-spherical Sb 2 Se 3 NPs, with a band gap of 1.13 eV, upon illumination, release photoexcited electrons in addition to other charge carriers at the CE to further enhance the reduction of the oxidized polysulfide. The p-type conducting behavior of Sb 2 Se 3 , coupled with a work function at 4.63 eV, also facilitates electron injection to polysulfide. The effect of graphene quantum dots (GQDs) as co-sensitizers as well as electron conduits is also investigated in which a TiO 2 /CdS/GQDs photoanode structure in combination with a C-fabric CE delivered a power-conversion efficiency (PCE) of 5.28%, which is a vast improvement over the 4.23% that is obtained by using a TiO 2 /CdS photoanode (without GQDs) with the same CE. GQDs, due to a superior conductance, impact efficiency more than Sb 2 Se 3 NPs do. The best PCE of a TiO 2 /CdS/GQDs-nS 2- /S n 2- -Sb 2 Se 3 /NiO/C-fabric cell is 5.96% (0.11 cm 2 area), which, when replicated on a smaller area of 0.06 cm 2 , is seen to increase dramatically to 7.19%. The cell is also tested for 6 h of continuous irradiance. The rationalization for the channelized photogenerated electron movement, which augments the cell performance, is furnished in detail in these studies.

Ag2S Quantum Dot-Sensitized Solar Cells by First Principles: The Effect of Capping Ligands and Linkers.

PubMed

Amaya Suárez, Javier; Plata, Jose J; Márquez, Antonio M; Fernández Sanz, Javier

2017-09-28

Quantum dots solar cells, QDSCs, are one of the candidates for being a reliable alternative to fossil fuels. However, the well-studied CdSe and CdTe-based QDSCs present a variety of issues for their use in consumer-goods applications. Silver sulfide, Ag 2 S, is a promising material, but poor efficiency has been reported for QDSCs based on this compound. The potential influence of each component of QDSCs is critical and key for the development of more efficient devices based on Ag 2 S. In this work, density functional theory calculations were performed to study the nature of the optoelectronic properties for an anatase-TiO 2 (101) surface sensitized with different silver sulfide nanoclusters. We demonstrated how it is possible to deeply tune of its electronic properties by modifying the capping ligands and linkers to the surface. Finally, an analysis of the electron injection mechanism for this system is presented.

Charge transfer in photorechargeable composite films of TiO2 and polyaniline

NASA Astrophysics Data System (ADS)

Nomiyama, Teruaki; Sasabe, Kenichi; Sakamoto, Kenta; Horie, Yuji

2015-07-01

A photorechargeable battery (PRB) is a photovoltaic device having an energy storage function in a single cell. The photoactive electrode of PRB is a bilayer film consisting of bare porous TiO2 and a TiO2-polyaniline (PANi) mixture that work as a photovoltaic current generator and an electrochemical energy storage by ion dedoping, respectively. To study the charge transfer between TiO2 and PANi, the photorechargeable quantum efficiency QE ([electron count on discharge]/[incident photon count on photocharge]) was measured by varying the thickness LS of the TiO2-PANi mixture. The quantum efficiency QEuv for UV photons had a maximum of ˜7% at LS ˜ 7 µm. The time constant τTP for the charge transfer was about 10-1 s, which was longer ten times or more than the lifetime of excited electrons within TiO2. These facts reveal that the main rate-limiting factor in the photocharging process is the charge transfer between TiO2 and PANi.

Development of an EMCCD for LIDAR applications

NASA Astrophysics Data System (ADS)

De Monte, B.; Bell, R. T.

2017-11-01

A novel detector, incorporating e2v's EMCCD (L3VisionTM) [1] technology for use in LIDAR (Light Detection And Ranging) applications has been designed, manufactured and characterised. The most critical performance aspect was the requirement to collect charge from a 120μm square detection area for a 667ns temporal sampling window, with low crosstalk between successive samples, followed by signal readout with sub-electron effective noise. Additional requirements included low dark signal, high quantum efficiency at the 355nm laser wavelength and the ability to handle bright laser echoes, without corruption of the much fainter useful signals. The detector architecture used high speed charge binning to combine signal from each sampling window into a single charge packet. This was then passed through a multiplication register (EMCCD) operating with a typical gain of 100X to a conventional charge detection circuit. The detector achieved a typical quantum efficiency of 80% and a total noise in darkness of < 0.5 electrons rms. Development of the detector was supported by ESA.

High-Efficiency InGaN/GaN Quantum Well-Based Vertical Light-Emitting Diodes Fabricated on β-Ga2O3 Substrate.

PubMed

Muhammed, Mufasila M; Alwadai, Norah; Lopatin, Sergei; Kuramata, Akito; Roqan, Iman S

2017-10-04

We demonstrate a state-of-the-art high-efficiency GaN-based vertical light-emitting diode (VLED) grown on a transparent and conductive (-201)-oriented (β-Ga 2 O 3 ) substrate, obtained using a straightforward growth process that does not require a high-cost lift-off technique or complex fabrication process. The high-resolution scanning transmission electron microscopy (STEM) images confirm that we produced high quality upper layers, including a multiquantum well (MQW) grown on the masked β-Ga 2 O 3 substrate. STEM imaging also shows a well-defined MQW without InN diffusion into the barrier. Electroluminescence (EL) measurements at room temperature indicate that we achieved a very high internal quantum efficiency (IQE) of 78%; at lower temperatures, IQE reaches ∼86%. The photoluminescence (PL) and time-resolved PL analysis indicate that, at a high carrier injection density, the emission is dominated by radiative recombination with a negligible Auger effect; no quantum-confined Stark effect is observed. At low temperatures, no efficiency droop is observed at a high carrier injection density, indicating the superior VLED structure obtained without lift-off processing, which is cost-effective for large-scale devices.

Phosphorescent Iridium(III) Complexes Bearing Fluorinated Aromatic Sulfonyl Group with Nearly Unity Phosphorescent Quantum Yields and Outstanding Electroluminescent Properties.

PubMed

Zhao, Jiang; Yu, Yue; Yang, Xiaolong; Yan, Xiaogang; Zhang, Huiming; Xu, Xianbin; Zhou, Guijiang; Wu, Zhaoxin; Ren, Yixia; Wong, Wai-Yeung

2015-11-11

A series of heteroleptic functional Ir(III) complexes bearing different fluorinated aromatic sulfonyl groups has been synthesized. Their photophysical features, electrochemical behaviors, and electroluminescent (EL) properties have been characterized in detail. These complexes emit intense yellow phosphorescence with exceptionally high quantum yields (ΦP > 0.9) at room temperature, and the emission maxima of these complexes can be finely tuned depending upon the number of the fluorine substituents on the pendant phenyl ring of the sulfonyl group. Furthermore, the electrochemical properties and electron injection/transporting (EI/ET) abilities of these Ir(III) phosphors can also be effectively tuned by the fluorinated aromatic sulfonyl group to furnish some desired characters for enhancing the EL performance. Hence, the maximum luminance efficiency (ηL) of 81.2 cd A(-1), corresponding to power efficiency (ηP) of 64.5 lm W(-1) and external quantum efficiency (ηext) of 19.3%, has been achieved, indicating the great potential of these novel phosphors in the field of organic light-emitting diodes (OLEDs). Furthermore, a clear picture has been drawn for the relationship between their optoelectronic properties and chemical structures. These results should provide important information for developing highly efficient phosphors.

High-efficiency red electroluminescent device based on multishelled InP quantum dots.

PubMed

Jo, Jung-Ho; Kim, Jong-Hoon; Lee, Ki-Heon; Han, Chang-Yeol; Jang, Eun-Pyo; Do, Young Rag; Yang, Heesun

2016-09-01

We report on the synthesis of highly fluorescent red-emitting InP quantum dots (QDs) and their application to the fabrication of a high-efficiency QD-light-emitting diode (QLED). The core/shell heterostructure of the QDs is elaborately tailored toward a multishelled structure with a composition-gradient ZnSeS intermediate shell and an outer ZnS shell. Using the resulting InP/ZnSeS/ZnS QDs as an emitting layer, all-solution-processible red InP QLEDs are fabricated with a hybrid multilayered device structure having an organic hole transport layer (HTL) and an inorganic ZnO nanoparticle electron transport layer. Two HTLs of poly(9-vinlycarbazole) or poly[(9,9-dioctylfluorenyl-2,7-diyl)-co-(4,4^'-(N-(4-sec-butylphenyl))diphenyl-amine), whose hole mobilities are different by at least three orders of magnitude, are individually applied for QLED fabrication and such HTL-dependent device performances are compared. Our best red device displays exceptional figures of merit such as a maximum luminance of 2849  cd/m², a current efficiency of 4.2  cd/A, and an external quantum efficiency of 2.5%.

Spin power and efficiency in an Aharnov-Bohm ring with an embedded magnetic impurity quantum dot

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

Yang, Xi; Guo, Yong, E-mail: guoy66@tsinghua.edu.cn; Collaborative Innovation Center of Quantum Matter, Beijing

2015-05-11

Spin thermoelectric effects in an Aharnov-Bohm ring with a magnetic impurity quantum dot (QD) are theoretically investigated by using the nonequilibrium Green's function method. It is found that due to the exchange coupling between the impurity and the electrons in QD, spin output power, and efficiency can be significant and be further modulated by the gate voltage. The spin thermoelectric effect can be modulated effectively by adjusting the Rashba spin-orbit interaction (RSOI) and the magnetic flux. The spin power and efficiency show zigzag oscillations, and thus spin thermoelectric effect can be switched by adjusting the magnetic flux phase factor andmore » RSOI ones. In addition, the spin efficiency can be significantly enhanced by the coexistence of the RSOI and the magnetic flux, and the maximal value of normalized spin efficiency η{sub max}/η{sub C} = 0.35 is obtained. Our results show that such a QD ring device may be used as a manipulative spin thermoelectric generator.« less

High-fidelity spin measurement on the nitrogen-vacancy center

NASA Astrophysics Data System (ADS)

Hanks, Michael; Trupke, Michael; Schmiedmayer, Jörg; Munro, William J.; Nemoto, Kae

2017-10-01

Nitrogen-vacancy (NV) centers in diamond are versatile candidates for many quantum information processing tasks, ranging from quantum imaging and sensing through to quantum communication and fault-tolerant quantum computers. Critical to almost every potential application is an efficient mechanism for the high fidelity readout of the state of the electronic and nuclear spins. Typically such readout has been achieved through an optically resonant fluorescence measurement, but the presence of decay through a meta-stable state will limit its efficiency to the order of 99%. While this is good enough for many applications, it is insufficient for large scale quantum networks and fault-tolerant computational tasks. Here we explore an alternative approach based on dipole induced transparency (state-dependent reflection) in an NV center cavity QED system, using the most recent knowledge of the NV center’s parameters to determine its feasibility, including the decay channels through the meta-stable subspace and photon ionization. We find that single-shot measurements above fault-tolerant thresholds should be available in the strong coupling regime for a wide range of cavity-center cooperativities, using a majority voting approach utilizing single photon detection. Furthermore, extremely high fidelity measurements are possible using weak optical pulses.

Photoresponse Enhancement in Monolayer ReS2 Phototransistor Decorated with CdSe-CdS-ZnS Quantum Dots.

PubMed

Qin, Jing-Kai; Ren, Dan-Dan; Shao, Wen-Zhu; Li, Yang; Miao, Peng; Sun, Zhao-Yuan; Hu, PingAn; Zhen, Liang; Xu, Cheng-Yan

2017-11-15

ReS 2 films are considered as a promising candidate for optoelectronic applications due to their direct band gap character and optical/electrical anisotropy. However, the direct band gap in a narrow spectrum and the low absorption of atomically thin flakes weaken the prospect for light-harvesting applications. Here, we developed an efficient approach to enhance the performance of a ReS 2 -based phototransistor by coupling CdSe-CdS-ZnS core-shell quantum dots. Under 589 nm laser irradiation, the responsivity of the ReS 2 phototransistor decorated with quantum dots could be enhanced by more than 25 times (up to ∼654 A/W) and the rising and recovery time can be also reduced to 3.2 and 2.8 s, respectively. The excellent optoelectronic performance is originated from the coupling effect of quantum dots light absorber and cross-linker ligands 1,2-ethanedithiol. Photoexcited electron-hole pairs in quantum dots can separate and transfer efficiently due to the type-II band alignment and charge exchange process at the interface. Our work shows that the simple hybrid zero- and two-dimensional hybrid system can be employed for photodetection applications.

Comparative Response of Microchannel Plate and Channel Electron Multiplier Detectors to Penetrating Radiation in Space

DOE PAGES

Funsten, Herbert O.; Harper, Ronnie W.; Dors, Eric E.; ...

2015-10-02

Channel electron multiplier (CEM) and microchannel plate (MCP) detectors are routinely used in space instrumentation for measurement of space plasmas. Here, our goal is to understand the relative sensitivities of these detectors to penetrating radiation in space, which can generate background counts and shorten detector lifetime. We use 662 keV γ-rays as a proxy for penetrating radiation such as γ-rays, cosmic rays, and high-energy electrons and protons that are ubiquitous in the space environment. We find that MCP detectors are ~20 times more sensitive to 662 keV γ-rays than CEM detectors. This is attributed to the larger total area ofmore » multiplication channels in an MCP detector that is sensitive to electronic excitation and ionization resulting from the interaction of penetrating radiation with the detector material. In contrast to the CEM detector, whose quantum efficiency ε γ for 662 keVγ -rays is found to be 0.00175 and largely independent of detector bias, the quantum efficiency of the MCP detector is strongly dependent on the detector bias, with a power law index of 5.5. Lastly, background counts in MCP detectors from penetrating radiation can be reduced using MCP geometries with higher pitch and smaller channel diameter.« less

Graphene quantum dot incorporated perovskite films: passivating grain boundaries and facilitating electron extraction.

PubMed

Fang, Xiang; Ding, Jianning; Yuan, Ningyi; Sun, Peng; Lv, Minghang; Ding, Guqiao; Zhu, Chong

2017-02-22

Organic-inorganic halide perovskites have emerged as attractive materials for use in photovoltaic cells. Owing to the existence of dangling bonds at the grain boundaries between perovskite crystals, minimizing the charge recombination at the surface or grain boundaries by passivating these trap states has been identified to be one of the most important strategies for further optimization of device performance. Previous reports have mainly focused on surface passivation by inserting special materials such as graphene or fullerene between the electron transfer layer and the perovskite film. Here, we report an enhanced efficiency of mesoscopic perovskite solar cells by using graphene quantum dots (GQDs) to passivate the grain boundaries of CH 3 NH 3 PbI 3 . The highest efficiency (17.62%) is achieved via decoration with 7% GQDs, which is an 8.2% enhancement with respect to a pure perovskite based device. Various analyses including electrochemical impedance spectroscopy, time-resolved photoluminescence decay and open-circuit voltage decay measurements are employed in investigating the mechanism behind the improvement in device performance. The findings reveal two important roles played by GQDs in promoting the performance of perovskite solar cells - that GQDs are conducive to facilitating electron extraction and can effectively passivate the electron traps at the perovskite grain boundaries.

Synchronized energy and electron transfer processes in covalently linked CdSe-squaraine dye-TiO2 light harvesting assembly.

PubMed

Choi, Hyunbong; Santra, Pralay K; Kamat, Prashant V

2012-06-26

Manipulation of energy and electron transfer processes in a light harvesting assembly is an important criterion to mimic natural photosynthesis. We have now succeeded in sequentially assembling CdSe quantum dot (QD) and squaraine dye (SQSH) on TiO(2) film and couple energy and electron transfer processes to generate photocurrent in a hybrid solar cell. When attached separately, both CdSe QDs and SQSH inject electrons into TiO(2) under visible-near-IR irradiation. However, CdSe QD if linked to TiO(2) with SQSH linker participates in an energy transfer process. The hybrid solar cells prepared with squaraine dye as a linker between CdSe QD and TiO(2) exhibited power conversion efficiency of 3.65% and good stability during illumination with global AM 1.5 solar condition. Transient absorption spectroscopy measurements provided further insight into the energy transfer between excited CdSe QD and SQSH (rate constant of 6.7 × 10(10) s(-1)) and interfacial electron transfer between excited SQSH and TiO(2) (rate constant of 1.2 × 10(11) s(-1)). The synergy of covalently linked semiconductor quantum dots and near-IR absorbing squaraine dye provides new opportunities to harvest photons from selective regions of the solar spectrum in an efficient manner.

Enhancement of the thermoelectric efficiency in a T-shaped quantum dot system in the linear and nonlinear regimes

NASA Astrophysics Data System (ADS)

Gómez-Silva, G.; Orellana, P. A.; Anda, E. V.

2018-02-01

In the present work, we investigate the thermoelectric properties of a T-shaped double quantum dot system coupled to two metallic leads incorporating the intra-dot Coulomb interaction. We explore the role of the interference effects and Coulomb blockade on the thermoelectric efficiency of the system in the linear and nonlinear regimes. We studied as well the effect of a Van-Hove singularity of the leads density of states (DOS) at the neighborhood of the Fermi energy, a situation that can be obtained using a carbon nanotube, a graphene nano-ribbon or other contacts with one-dimensional properties. The system is studied above the Kondo temperature. The Coulomb blockade of the electronic charges is studied using the Hubbard III approximation, which properly describes the transport properties of this regime. In the linear response, our results show an enhancement of the thermopower and the figure of merit of the system. For a nonlinear situation, we calculate the thermoelectric efficiency and power output, concluding that the T-shaped double quantum dot is an efficient thermoelectric device. Moreover, we demonstrate the great importance of the DOS Van-Hove singularity at the neighborhood of the Fermi energy to obtain a very significant increase in the thermoelectric efficiency of the system.

Cosensitized Quantum Dot Solar Cells with Conversion Efficiency over 12.

PubMed

Wang, Wei; Feng, Wenliang; Du, Jun; Xue, Weinan; Zhang, Linlin; Zhao, Leilei; Li, Yan; Zhong, Xinhua

2018-03-01

The improvement of sunlight utilization is a fundamental approach for the construction of high-efficiency quantum-dot-based solar cells (QDSCs). To boost light harvesting, cosensitized photoanodes are fabricated in this work by a sequential deposition of presynthesized Zn-Cu-In-Se (ZCISe) and CdSe quantum dots (QDs) on mesoporous TiO 2 films via the control of the interactions between QDs and TiO 2 films using 3-mercaptopropionic acid bifunctional linkers. By the synergistic effect of ZCISe-alloyed QDs with a wide light absorption range and CdSe QDs with a high extinction coefficient, the incident photon-to-electron conversion efficiency is significantly improved over single QD-based QDSCs. It is found that the performance of cosensitized photoanodes can be optimized by adjusting the size of CdSe QDs introduced. In combination with titanium mesh supported mesoporous carbon as a counterelectrode and a modified polysulfide solution as an electrolyte, a champion power conversion efficiency up to 12.75% (V oc = 0.752 V, J sc = 27.39 mA cm -2 , FF = 0.619) is achieved, which is, as far as it is known, the highest efficiency for liquid-junction QD-based solar cells reported. © 2018 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Focal-Plane Arrays of Quantum-Dot Infrared Photodetectors

NASA Technical Reports Server (NTRS)

Gunapala, Sarath; Wilson, Daniel; Hill, Cory; Liu, John; Bandara, Sumith; Ting, David

2007-01-01

Focal-plane arrays of semiconductor quantum-dot infrared photodetectors (QDIPs) are being developed as superior alternatives to prior infrared imagers, including imagers based on HgCdTe devices and, especially, those based on quantum-well infrared photodetectors (QWIPs). HgCdTe devices and arrays thereof are difficult to fabricate and operate, and they exhibit large nonunformities and high 1/f (where f signifies frequency) noise. QWIPs are easier to fabricate and operate, can be made nearly uniform, and exhibit lower 1/f noise, but they exhibit larger dark currents, and their quantization only along the growth direction prevents them from absorbing photons at normal incidence, thereby limiting their quantum efficiencies. Like QWIPs, QDIPs offer the advantages of greater ease of operation, greater uniformity, and lower 1/f noise, but without the disadvantages: QDIPs exhibit lower dark currents, and quantum efficiencies of QDIPs are greater because the three-dimensional quantization of QDIPs is favorable to the absorption of photons at normal or oblique incidence. Moreover, QDIPs can be operated at higher temperatures (around 200 K) than are required for operation of QWIPs. The main problem in the development of QDIP imagers is to fabricate quantum dots with the requisite uniformity of size and spacing. A promising approach to be tested soon involves the use of electron-beam lithography to define the locations and sizes of quantum dots. A photoresist-covered GaAs substrate would be exposed to the beam generated by an advanced, high-precision electron beam apparatus. The exposure pattern would consist of spots typically having a diameter of 4 nm and typically spaced 20 nm apart. The exposed photoresist would be developed by either a high-contrast or a low-contrast method. In the high-contrast method, the spots would be etched in such a way as to form steep-wall holes all the way down to the substrate. The holes would be wider than the electron beam spots perhaps as wide as 15 to 20 nm, but may be sufficient to control the growth of the quantum dots. In the low-contrast method, the resist would be etched in such a way as to form dimples, the shapes of which would mimic the electron-beam density profile. Then by use of a transfer etching process that etches the substrate faster than it etches the resist, either the pattern of holes or a pattern comprising the narrow, lowest portions of the dimples would be imparted to the substrate. Having been thus patterned, the substrate would be cleaned. The resulting holes or dimples in the substrate would serve as nucleation sites for the growth of quantum dots of controlled size in the following steps. The substrate would be cleaned, then placed in a molecular-beam-epitaxy (MBE) chamber, where native oxide would be thermally desorbed and the quantum dots would be grown.

Microscopic Perspective on Photovoltaic Reciprocity in Ultrathin Solar Cells

NASA Astrophysics Data System (ADS)

Aeberhard, Urs; Rau, Uwe

2017-06-01

The photovoltaic reciprocity theory relates the electroluminescence spectrum of a solar cell under applied bias to the external photovoltaic quantum efficiency of the device as measured at short circuit conditions. Its derivation is based on detailed balance relations between local absorption and emission rates in optically isotropic media with nondegenerate quasiequilibrium carrier distributions. In many cases, the dependence of density and spatial variation of electronic and optical device states on the point of operation is modest and the reciprocity relation holds. In nanostructure-based photovoltaic devices exploiting confined modes, however, the underlying assumptions are no longer justifiable. In the case of ultrathin absorber solar cells, the modification of the electronic structure with applied bias is significant due to the large variation of the built-in field. Straightforward use of the external quantum efficiency as measured at short circuit conditions in the photovoltaic reciprocity theory thus fails to reproduce the electroluminescence spectrum at large forward bias voltage. This failure is demonstrated here by numerical simulation of both spectral quantities at normal incidence and emission for an ultrathin GaAs p -i -n solar cell using an advanced quantum kinetic formalism based on nonequilibrium Green's functions of coupled photons and charge carriers. While coinciding with the semiclassical relations under the conditions of their validity, the theory provides a consistent microscopic relationship between absorption, emission, and charge carrier transport in photovoltaic devices at arbitrary operating conditions and for any shape of optical and electronic density of states.

Microscopic Perspective on Photovoltaic Reciprocity in Ultrathin Solar Cells.

PubMed

Aeberhard, Urs; Rau, Uwe

2017-06-16

The photovoltaic reciprocity theory relates the electroluminescence spectrum of a solar cell under applied bias to the external photovoltaic quantum efficiency of the device as measured at short circuit conditions. Its derivation is based on detailed balance relations between local absorption and emission rates in optically isotropic media with nondegenerate quasiequilibrium carrier distributions. In many cases, the dependence of density and spatial variation of electronic and optical device states on the point of operation is modest and the reciprocity relation holds. In nanostructure-based photovoltaic devices exploiting confined modes, however, the underlying assumptions are no longer justifiable. In the case of ultrathin absorber solar cells, the modification of the electronic structure with applied bias is significant due to the large variation of the built-in field. Straightforward use of the external quantum efficiency as measured at short circuit conditions in the photovoltaic reciprocity theory thus fails to reproduce the electroluminescence spectrum at large forward bias voltage. This failure is demonstrated here by numerical simulation of both spectral quantities at normal incidence and emission for an ultrathin GaAs p-i-n solar cell using an advanced quantum kinetic formalism based on nonequilibrium Green's functions of coupled photons and charge carriers. While coinciding with the semiclassical relations under the conditions of their validity, the theory provides a consistent microscopic relationship between absorption, emission, and charge carrier transport in photovoltaic devices at arbitrary operating conditions and for any shape of optical and electronic density of states.

Tailoring Quantum Dot Assemblies to Extend Exciton Coherence Times and Improve Exciton Transport

NASA Astrophysics Data System (ADS)

Seward, Kenton; Lin, Zhibin; Lusk, Mark

2012-02-01

The motion of excitons through nanostructured assemblies plays a central role in a wide range of physical phenomena including quantum computing, molecular electronics, photosynthetic processes, excitonic transistors and light emitting diodes. All of these technologies are severely handicapped, though, by quasi-particle lifetimes on the order of a nanosecond. The movement of excitons must therefore be as efficient as possible in order to move excitons meaningful distances. This is problematic for assemblies of small Si quantum dots (QDs), where excitons quickly localize and entangle with dot phonon modes. Ensuing exciton transport is then characterized by a classical random walk reduced to very short distances because of efficient recombination. We use a combination of master equation (Haken-Strobl) formalism and density functional theory to estimate the rate of decoherence in Si QD assemblies and its impact on exciton mobility. Exciton-phonon coupling and Coulomb interactions are calculated as a function of dot size, spacing and termination to minimize the rate of intra-dot phonon entanglement. This extends the time over which more efficient exciton transport, characterized by partial coherence, can be maintained.

High efficiency low threshold current 1.3 μm InAs quantum dot lasers on on-axis (001) GaP/Si

NASA Astrophysics Data System (ADS)

Jung, Daehwan; Norman, Justin; Kennedy, M. J.; Shang, Chen; Shin, Bongki; Wan, Yating; Gossard, Arthur C.; Bowers, John E.

2017-09-01

We demonstrate highly efficient, low threshold InAs quantum dot lasers epitaxially grown on on-axis (001) GaP/Si substrates using molecular beam epitaxy. Electron channeling contrast imaging measurements show a threading dislocation density of 7.3 × 106 cm-2 from an optimized GaAs template grown on GaP/Si. The high-quality GaAs templates enable as-cleaved quantum dot lasers to achieve a room-temperature continuous-wave (CW) threshold current of 9.5 mA, a threshold current density as low as 132 A/cm2, a single-side output power of 175 mW, and a wall-plug-efficiency of 38.4% at room temperature. As-cleaved QD lasers show ground-state CW lasing up to 80 °C. The application of a 95% high-reflectivity coating on one laser facet results in a CW threshold current of 6.7 mA, which is a record-low value for any kind of Fabry-Perot laser grown on Si.

PREFACE: Semiconductor Nanostructures towards Electronic and Optoelectronic Device Applications II (Symposium K, E-MRS 2009 Spring Meeting)

NASA Astrophysics Data System (ADS)

Nötzel, Richard

2009-07-01

This volume of IOP Conference Series: Materials Science and Engineering contains papers that were presented at the special symposium K at the EMRS 2009 Spring Meeting held 8-12 June in Strasbourg, France, which was entitled 'Semiconductor Nanostructures towards Electronic and Optoelectronic Device Applications II'. Thanks to the broad interest a large variety of quantum dots and quantum wires and related nanostructures and their application in devices could be covered. There was significant progress in the epitaxial growth of semiconductor quantum dots seen in the operation of high-power, as well as mode locked laser diodes and the lateral positioning of quantum dots on patterned substrates or by selective area growth for future single quantum dot based optoelectronic and electronic devices. In the field of semiconductor nanowires high quality, almost twin free structures are now available together with a new degree of freedom for band structure engineering based on alternation of the crystal structure. In the search for Si based light emitting structures, nanocrystals and miniband-related near infrared luminescence of Si/Ge quantum dot superlattices with high quantum efficiency were reported. These highlights, among others, and the engaged discussions of the scientists, engineers and students brought together at the symposium emphasize how active the field of semiconductor nanostructures and their applications in devices is, so that we can look forward to the progress to come. Guest Editor Richard Nötzel COBRA Research Institute Department of Applied Physics Eindhoven University of Technology 5600 MB Eindhoven The Netherlands Tel.: +31 40 247 2047; fax: +31 40 246 1339 E-mail address: r.noetzel@tue.nl

ZnO Quantum Dot Decorated Zn2SnO4 Nanowire Heterojunction Photodetectors with Drastic Performance Enhancement and Flexible Ultraviolet Image Sensors.

PubMed

Li, Ludong; Gu, Leilei; Lou, Zheng; Fan, Zhiyong; Shen, Guozhen

2017-04-25

Here we report the fabrication of high-performance ultraviolet photodetectors based on a heterojunction device structure in which ZnO quantum dots were used to decorate Zn 2 SnO 4 nanowires. Systematic investigations have shown their ultrahigh light-to-dark current ratio (up to 6.8 × 10 4 ), specific detectivity (up to 9.0 × 10 17 Jones), photoconductive gain (up to 1.1 × 10 7 ), fast response, and excellent stability. Compared with a pristine Zn 2 SnO 4 nanowire, a quantum dot decorated nanowire demonstrated about 10 times higher photocurrent and responsivity. Device physics modeling showed that their high performance originates from the rational energy band engineering, which allows efficient separation of electron-hole pairs at the interfaces between ZnO quantum dots and a Zn 2 SnO 4 nanowire. As a result of band engineering, holes migrate to ZnO quantum dots, which increases electron concentration and lifetime in the nanowire conduction channel, leading to significantly improved photoresponse. The enhancement mechanism found in this work can also be used to guide the design of high-performance photodetectors based on other nanomaterials. Furthermore, flexible ultraviolet photodetectors were fabricated and integrated into a 10 × 10 device array, which constitutes a high-performance flexible ultraviolet image sensor. These intriguing results suggest that the band alignment engineering on nanowires can be rationally achieved using compound semiconductor quantum dots. This can lead to largely improved device performance. Particularly for ZnO quantum dot decorated Zn 2 SnO 4 nanowires, these decorated nanowires may find broad applications in future flexible and wearable electronics.

Double Super-Exchange in Silicon Quantum Dots Connected by Short-Bridged Networks

NASA Astrophysics Data System (ADS)

Li, Huashan; Wu, Zhigang; Lusk, Mark

2013-03-01

Silicon quantum dots (QDs) with diameters in the range of 1-2 nm are attractive for photovoltaic applications. They absorb photons more readily, transport excitons with greater efficiency, and show greater promise in multiple-exciton generation and hot carrier collection paradigms. However, their high excitonic binding energy makes it difficult to dissociate excitons into separate charge carriers. One possible remedy is to create dot assemblies in which a second material creates a Type-II heterojunction with the dot so that exciton dissociation occurs locally. This talk will focus on such a Type-II heterojunction paradigm in which QDs are connected via covalently bonded, short-bridge molecules. For such interpenetrating networks of dots and molecules, our first principles computational investigation shows that it is possible to rapidly and efficiently separate electrons to QDs and holes to bridge units. The bridge network serves as an efficient mediator of electron superexchange between QDs while the dots themselves play the complimentary role of efficient hole superexchange mediators. Dissociation, photoluminescence and carrier transport rates will be presented for bridge networks of silicon QDs that exhibit such double superexchange. This material is based upon work supported by the Renewable Energy Materials Research Science and Engineering Center (REMRSEC) under Grant No. DMR-0820518 and Golden Energy Computing Organization (GECO).

Distinguishing crystallization stages and their influence on quantum efficiency during perovskite solar cell formation in real-time.

PubMed

Wagner, Lukas; Mundt, Laura E; Mathiazhagan, Gayathri; Mundus, Markus; Schubert, Martin C; Mastroianni, Simone; Würfel, Uli; Hinsch, Andreas; Glunz, Stefan W

2017-11-02

Relating crystallization of the absorber layer in a perovskite solar cell (PSC) to the device performance is a key challenge for the process development and in-depth understanding of these types of high efficient solar cells. A novel approach that enables real-time photo-physical and electrical characterization using a graphite-based PSC is introduced in this work. In our graphite-based PSC, the device architecture of porous monolithic contact layers creates the possibility to perform photovoltaic measurements while the perovskite crystallizes within this scaffold. The kinetics of crystallization in a solution based 2-step formation process has been analyzed by real-time measurement of the external photon to electron quantum efficiency as well as the photoluminescence emission spectra of the solar cell. With this method it was in particular possible to identify a previously overlooked crystallization stage during the formation of the perovskite absorber layer. This stage has significant influence on the development of the photocurrent, which is attributed to the formation of electrical pathways between the electron and hole contact, enabling efficient charge carrier extraction. We observe that in contrast to previously suggested models, the perovskite layer formation is indeed not complete with the end of crystal growth.

Rhizopus stolonifer mediated biosynthesis of biocompatible cadmium chalcogenide quantum dots.

PubMed

Mareeswari, P; Brijitta, J; Harikrishna Etti, S; Meganathan, C; Kaliaraj, Gobi Saravanan

2016-12-01

We report an efficient method to biosynthesize biocompatible cadmium telluride and cadmium sulphide quantum dots from the fungus Rhizopus stolonifer. The suspension of the quantum dots exhibited purple and greenish-blue luminescence respectively upon UV light illumination. Photoluminescence spectroscopy, X-ray diffraction, and transmission electron microscopy confirms the formation of the quantum dots. From the photoluminescence spectrum the emission maxima is found to be 424 and 476nm respectively. The X-ray diffraction of the quantum dots matches with results reported in literature. The 3-(4,5-dimethylthiazol-2-yl)-2,5-diphenyltetrazolium bromide assay for cell viability evaluation carried out on 3-days transfer, inoculum 3×10 5 cells, embryonic fibroblast cells lines shows that more than 80% of the cells are viable even after 48h, indicating the biocompatible nature of the quantum dots. A good contrast in imaging has been obtained upon incorporating the quantum dots in human breast adenocarcinoma Michigan Cancer Foundation-7 cell lines. Copyright © 2016 Elsevier Inc. All rights reserved.

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

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

Xu, Xingsheng, E-mail: xsxu@semi.ac.cn

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 decreasedmore » 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.« less

Quantum coherence spectroscopy reveals complex dynamics in bacterial light-harvesting complex 2 (LH2).

PubMed

Harel, Elad; Engel, Gregory S

2012-01-17

Light-harvesting antenna complexes transfer energy from sunlight to photosynthetic reaction centers where charge separation drives cellular metabolism. The process through which pigments transfer excitation energy involves a complex choreography of coherent and incoherent processes mediated by the surrounding protein and solvent environment. The recent discovery of coherent dynamics in photosynthetic light-harvesting antennae has motivated many theoretical models exploring effects of interference in energy transfer phenomena. In this work, we provide experimental evidence of long-lived quantum coherence between the spectrally separated B800 and B850 rings of the light-harvesting complex 2 (LH2) of purple bacteria. Spectrally resolved maps of the detuning, dephasing, and the amplitude of electronic coupling between excitons reveal that different relaxation pathways act in concert for optimal transfer efficiency. Furthermore, maps of the phase of the signal suggest that quantum mechanical interference between different energy transfer pathways may be important even at ambient temperature. Such interference at a product state has already been shown to enhance the quantum efficiency of transfer in theoretical models of closed loop systems such as LH2.

Quantum coherence spectroscopy reveals complex dynamics in bacterial light-harvesting complex 2 (LH2)

PubMed Central

Harel, Elad; Engel, Gregory S.

2012-01-01

Light-harvesting antenna complexes transfer energy from sunlight to photosynthetic reaction centers where charge separation drives cellular metabolism. The process through which pigments transfer excitation energy involves a complex choreography of coherent and incoherent processes mediated by the surrounding protein and solvent environment. The recent discovery of coherent dynamics in photosynthetic light-harvesting antennae has motivated many theoretical models exploring effects of interference in energy transfer phenomena. In this work, we provide experimental evidence of long-lived quantum coherence between the spectrally separated B800 and B850 rings of the light-harvesting complex 2 (LH2) of purple bacteria. Spectrally resolved maps of the detuning, dephasing, and the amplitude of electronic coupling between excitons reveal that different relaxation pathways act in concert for optimal transfer efficiency. Furthermore, maps of the phase of the signal suggest that quantum mechanical interference between different energy transfer pathways may be important even at ambient temperature. Such interference at a product state has already been shown to enhance the quantum efficiency of transfer in theoretical models of closed loop systems such as LH2. PMID:22215585

Generalized non-equilibrium vertex correction method in coherent medium theory for quantum transport simulation of disordered nanoelectronics

NASA Astrophysics Data System (ADS)

Yan, Jiawei; Ke, Youqi

In realistic nanoelectronics, disordered impurities/defects are inevitable and play important roles in electron transport. However, due to the lack of effective quantum transport method, the important effects of disorders remain poorly understood. Here, we report a generalized non-equilibrium vertex correction (NVC) method with coherent potential approximation to treat the disorder effects in quantum transport simulation. With this generalized NVC method, any averaged product of two single-particle Green's functions can be obtained by solving a set of simple linear equations. As a result, the averaged non-equilibrium density matrix and various important transport properties, including averaged current, disordered induced current fluctuation and the averaged shot noise, can all be efficiently computed in a unified scheme. Moreover, a generalized form of conditionally averaged non-equilibrium Green's function is derived to incorporate with density functional theory to enable first-principles simulation. We prove the non-equilibrium coherent potential equals the non-equilibrium vertex correction. Our approach provides a unified, efficient and self-consistent method for simulating non-equilibrium quantum transport through disorder nanoelectronics. Shanghaitech start-up fund.

Recovery of Active and Efficient Photocatalytic H 2 Production for CdSe Quantum Dots

DOE PAGES

Burke, Rebeckah; Cogan, Nicole M. Briglio; Oi, Aidan; ...

2018-05-07

Recently, colloidal semiconductor quantum dots (QDs) have shown great promise as photocatalysts for the production of chemical fuels by sunlight. Here, the efficiency of photocatalytic hydrogen (H 2) production for integrated systems of large diameter (4.4 nm) CdSe QDs as light harvesting nanoparticles with varying concentrations of nickel-dihydrolipoic acid (Ni-DHLA) small molecule catalysts was measured. While exhibiting excellent robustness and longevity, the efficiency of H 2 production for equimolar catalyst and QDs was relatively poor. However, the efficiency was found to increase substantially with increasing Ni-DHLA:QD molar ratios Surprisingly, this high activity was only observed with the use of 3-mercaptopropionicmore » acid (MPA) ligands, while CdSe QDs capped with dihydrolipoic acid (DHLA) exhibited poor performance in comparison, indicating that the QD capping ligand has a substantial impact on the catalytic performance. Finally, ultrafast transient absorption spectroscopic measurements of the electron transfer (ET) dynamics show fast ET to the catalyst. Importantly, an increase in ET efficiency is observed as the catalyst concentration is increased. Together, these results suggest that for these large QDs, tailoring the QD surface environment for facile ET and increasing catalyst concentrations increases the probability of ET from QDs to Ni-DHLA, overcoming the relatively small driving force for ET and decreased surface electron density for large diameter QDs.« less

Recovery of Active and Efficient Photocatalytic H 2 Production for CdSe Quantum Dots

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

Burke, Rebeckah; Cogan, Nicole M. Briglio; Oi, Aidan

Recently, colloidal semiconductor quantum dots (QDs) have shown great promise as photocatalysts for the production of chemical fuels by sunlight. Here, the efficiency of photocatalytic hydrogen (H 2) production for integrated systems of large diameter (4.4 nm) CdSe QDs as light harvesting nanoparticles with varying concentrations of nickel-dihydrolipoic acid (Ni-DHLA) small molecule catalysts was measured. While exhibiting excellent robustness and longevity, the efficiency of H 2 production for equimolar catalyst and QDs was relatively poor. However, the efficiency was found to increase substantially with increasing Ni-DHLA:QD molar ratios Surprisingly, this high activity was only observed with the use of 3-mercaptopropionicmore » acid (MPA) ligands, while CdSe QDs capped with dihydrolipoic acid (DHLA) exhibited poor performance in comparison, indicating that the QD capping ligand has a substantial impact on the catalytic performance. Finally, ultrafast transient absorption spectroscopic measurements of the electron transfer (ET) dynamics show fast ET to the catalyst. Importantly, an increase in ET efficiency is observed as the catalyst concentration is increased. Together, these results suggest that for these large QDs, tailoring the QD surface environment for facile ET and increasing catalyst concentrations increases the probability of ET from QDs to Ni-DHLA, overcoming the relatively small driving force for ET and decreased surface electron density for large diameter QDs.« less

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

Funsten, Herbert O.; Harper, Ronnie W.; Dors, Eric E.

Channel electron multiplier (CEM) and microchannel plate (MCP) detectors are routinely used in space instrumentation for measurement of space plasmas. Here, our goal is to understand the relative sensitivities of these detectors to penetrating radiation in space, which can generate background counts and shorten detector lifetime. We use 662 keV γ-rays as a proxy for penetrating radiation such as γ-rays, cosmic rays, and high-energy electrons and protons that are ubiquitous in the space environment. We find that MCP detectors are ~20 times more sensitive to 662 keV γ-rays than CEM detectors. This is attributed to the larger total area ofmore » multiplication channels in an MCP detector that is sensitive to electronic excitation and ionization resulting from the interaction of penetrating radiation with the detector material. In contrast to the CEM detector, whose quantum efficiency ε γ for 662 keVγ -rays is found to be 0.00175 and largely independent of detector bias, the quantum efficiency of the MCP detector is strongly dependent on the detector bias, with a power law index of 5.5. Lastly, background counts in MCP detectors from penetrating radiation can be reduced using MCP geometries with higher pitch and smaller channel diameter.« less

Silicon based quantum dot hybrid qubits

NASA Astrophysics Data System (ADS)

Kim, Dohun

2015-03-01

The charge and spin degrees of freedom of an electron constitute natural bases for constructing quantum two level systems, or qubits, in semiconductor quantum dots. The quantum dot charge qubit offers a simple architecture and high-speed operation, but generally suffers from fast dephasing due to strong coupling of the environment to the electron's charge. On the other hand, quantum dot spin qubits have demonstrated long coherence times, but their manipulation is often slower than desired for important future applications. This talk will present experimental progress of a `hybrid' qubit, formed by three electrons in a Si/SiGe double quantum dot, which combines desirable characteristics (speed and coherence) in the past found separately in qubits based on either charge or spin degrees of freedom. Using resonant microwaves, we first discuss qubit operations near the `sweet spot' for charge qubit operation. Along with fast (>GHz) manipulation rates for any rotation axis on the Bloch sphere, we implement two independent tomographic characterization schemes in the charge qubit regime: traditional quantum process tomography (QPT) and gate set tomography (GST). We also present resonant qubit operations of the hybrid qubit performed on the same device, DC pulsed gate operations of which were recently demonstrated. We demonstrate three-axis control and the implementation of dynamic decoupling pulse sequences. Performing QPT on the hybrid qubit, we show that AC gating yields π rotation process fidelities higher than 93% for X-axis and 96% for Z-axis rotations, which demonstrates efficient quantum control of semiconductor qubits using resonant microwaves. We discuss a path forward for achieving fidelities better than the threshold for quantum error correction using surface codes. This work was supported in part by ARO (W911NF-12-0607), NSF (PHY-1104660), DOE (DE-FG02-03ER46028), and by the Laboratory Directed Research and Development program at Sandia National Laboratories under contract DE-AC04-94AL85000.

Improved performance of near UV light-emitting diodes with a composition-graded p-AlGaN irregular sawtooth electron-blocking layer

NASA Astrophysics Data System (ADS)

Qin, Ping; Song, Wei-Dong; Hu, Wen-Xiao; Zhang, Yuan-Wen; Zhang, Chong-Zhen; Wang, Ru-Peng; Zhao, Liang-Liang; Xia, Chao; Yuan, Song-Yang; Yin, Yi-an; Li, Shu-Ti; Su, Shi-Chen

2016-08-01

We investigate the performances of the near-ultraviolet (about 350 nm-360 nm) light-emitting diodes (LEDs) each with specifically designed irregular sawtooth electron blocking layer (EBL) by using the APSYS simulation program. The internal quantum efficiencies (IQEs), light output powers, carrier concentrations in the quantum wells, energy-band diagrams, and electrostatic fields are analyzed carefully. The results indicate that the LEDs with composition-graded p-Al x Ga1-x N irregular sawtooth EBLs have better performances than their counterparts with stationary component p-AlGaN EBLs. The improvements can be attributed to the improved polarization field in EBL and active region as well as the alleviation of band bending in the EBL/p-AlGaN interface, which results in less electron leakage and better hole injection efficiency, thus reducing efficiency droop and enhancing the radiative recombination rate. Project supported by the National Natural Science Foundation of China (Grant Nos. 11474105 and 51172079), the Science and Technology Program of Guangdong Province, China (Grant Nos. 2015B090903078 and 2015B010105011), the Program for Changjiang Scholars and Innovative Research Team in University, China (Grant No. IRT13064), the Science and Technology Project of Guangzhou City, China (Grant No. 201607010246), and the Science and Technology Planning Project of Guangdong Province, China (Grant No. 2015A010105025).

New Insights into Sensitization Mechanism of the Doped Ce (IV) into Strontium Titanate

PubMed Central

Wang, Yuan; Liu, Chenglun; Xu, Longjun

2018-01-01

SrTiO3 and Ce4+ doped SrTiO3 were synthesized by a modified sol–gel process. The optimization synthesis parameters were obtained by a series of single factor experiments. Interesting phenomena are observable in Ce4+ doped SrTiO3 systems. Sr2+ in SrTiO3 system was replaced by Ce4+, which reduced the surface segregation of Ti4+, ameliorated agglomeration, increased specific surface area more than four times compared with pure SrTiO3, and enhanced quantum efficiency for SrTiO3. Results showed that Ce4+ doping increased the physical adsorption of H2O and adsorbed oxygen on the surface of SrTiO3, which produced additional catalytic active centers. Electrons on the 4f energy level for Ce4+ produced new energy states in the band gap of SrTiO3, which not only realized the use of visible light but also led to an easier separation between the photogenerated electrons and holes. Ce4+ repeatedly captured photoelectrons to produce Ce3+, which inhibited the recombination between photogenerated electrons and holes as well as prolonged their lifetime; it also enhanced quantum efficiency for SrTiO3. The methylene blue (MB) degradation efficiency reached 98.7% using 3 mol % Ce4+ doped SrTiO3 as a photocatalyst, indicating highly photocatalytic activity. PMID:29690605

Engineering Graphene Quantum Dots for Enhanced Ultraviolet and Visible Light p-Si Nanowire-Based Photodetector.

PubMed

Mihalache, Iuliana; Radoi, Antonio; Pascu, Razvan; Romanitan, Cosmin; Vasile, Eugenia; Kusko, Mihaela

2017-08-30

In this work, a significant improvement of the classical silicon nanowire (SiNW)-based photodetector was achieved through the realization of core-shell structures using newly designed GQD PEI s via simple solution processing. The poly(ethyleneimine) (PEI)-assisted synthesis successfully tuned both optical and electrical properties of graphene quantum dots (GQDs) to fulfill the requirements for strong yellow photoluminescence emission along with large band gap formation and the introduction of electronic states inside the band gap. The fabrication of a GQD PEI -based device was followed by systematic structural and photoelectronic investigation. Thus, the GQD PEI /SiNW photodetector exhibited a large photocurrent to dark current ratio (I ph /I dark up to ∼0.9 × 10 2 under 4 V bias) and a remarkable improvement of the external quantum efficiency values that far exceed 100%. In this frame, GQD PEI s demonstrate the ability to arbitrate both charge-carrier photogeneration and transport inside a heterojunction, leading to simultaneous attendance of various mechanisms: (i) efficient suppression of the dark current governed by the type I alignment in energy levels, (ii) charge photomultiplication determined by the presence of the PEI-induced electron trap levels, and (iii) broadband ultraviolet-to-visible downconversion effects.

Energy relay from an unconventional yellow dye to CdS/CdSe quantum dots for enhanced solar cell performance.

PubMed

Narayanan, Remya; Das, Amrita; Deepa, Melepurath; Srivastava, Avanish Kumar

2013-12-02

A new design for a quasi-solid-state Forster resonance energy transfer (FRET) enabled solar cell with unattached Lucifer yellow (LY) dye molecules as donors and CdS/CdSe quantum dots (QDs) tethered to titania (TiO2 ) as acceptors is presented. The Forster radius is experimentally determined to be 5.29 nm. Sequential energy transfer from the LY dye to the QDs and electron transfer from the QDs to TiO2 is followed by fluorescence quenching and electron lifetime studies. Cells with a donor-acceptor architecture (TiO2 /CdS/CdSe/ZnS-LY/S(2-)-multi-walled carbon nanotubes) show a maximum incident photon-to-current conversion efficiency of 53 % at 530 nm. This is the highest efficiency among Ru-dye free FRET-enabled quantum dot solar cells (QDSCs), and is much higher than the donor or acceptor-only cells. The FRET-enhanced solar cell performance over the majority of the visible spectrum paves the way to harnessing the untapped potential of the LY dye as an energy relay fluorophore for the entire gamut of dye sensitized, organic, or hybrid solar cells. Copyright © 2013 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

High-efficiency tris(8-hydroxyquinoline)aluminum (Alq3) complexes for organic white-light-emitting diodes and solid-state lighting.

PubMed

Pérez-Bolívar, César; Takizawa, Shin-ya; Nishimura, Go; Montes, Victor A; Anzenbacher, Pavel

2011-08-08

Combinations of electron-withdrawing and -donating substituents on the 8-hydroxyquinoline ligand of the tris(8-hydroxyquinoline)aluminum (Alq(3)) complexes allow for control of the HOMO and LUMO energies and the HOMO-LUMO gap responsible for emission from the complexes. Here, we present a systematic study on tuning the emission and electroluminescence (EL) from Alq(3) complexes from the green to blue region. In this study, we explored the combination of electron-donating substituents on C4 and C6. Compounds 1-6 displayed the emission tuning between 478 and 526 nm, and fluorescence quantum yield between 0.15 and 0.57. The compounds 2-6 were used as emitters and hosts in organic light-emitting diodes (OLEDs). The highest OLED external quantum efficiency (EQE) observed was 4.6%, which is among the highest observed for Alq(3) complexes. Also, the compounds 3-5 were used as hosts for red phosphorescent dopants to obtain white light-emitting diodes (WOLED). The WOLEDs displayed high efficiency (EQE up to 19%) and high white color purity (color rendering index (CRI≈85). Copyright © 2011 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

MCTDH on-the-fly: Efficient grid-based quantum dynamics without pre-computed potential energy surfaces

NASA Astrophysics Data System (ADS)

Richings, Gareth W.; Habershon, Scott

2018-04-01

We present significant algorithmic improvements to a recently proposed direct quantum dynamics method, based upon combining well established grid-based quantum dynamics approaches and expansions of the potential energy operator in terms of a weighted sum of Gaussian functions. Specifically, using a sum of low-dimensional Gaussian functions to represent the potential energy surface (PES), combined with a secondary fitting of the PES using singular value decomposition, we show how standard grid-based quantum dynamics methods can be dramatically accelerated without loss of accuracy. This is demonstrated by on-the-fly simulations (using both standard grid-based methods and multi-configuration time-dependent Hartree) of both proton transfer on the electronic ground state of salicylaldimine and the non-adiabatic dynamics of pyrazine.

TRIQS: A toolbox for research on interacting quantum systems

NASA Astrophysics Data System (ADS)

Parcollet, Olivier; Ferrero, Michel; Ayral, Thomas; Hafermann, Hartmut; Krivenko, Igor; Messio, Laura; Seth, Priyanka

2015-11-01

We present the TRIQS library, a Toolbox for Research on Interacting Quantum Systems. It is an open-source, computational physics library providing a framework for the quick development of applications in the field of many-body quantum physics, and in particular, strongly-correlated electronic systems. It supplies components to develop codes in a modern, concise and efficient way: e.g. Green's function containers, a generic Monte Carlo class, and simple interfaces to HDF5. TRIQS is a C++/Python library that can be used from either language. It is distributed under the GNU General Public License (GPLv3). State-of-the-art applications based on the library, such as modern quantum many-body solvers and interfaces between density-functional-theory codes and dynamical mean-field theory (DMFT) codes are distributed along with it.

Demonstration of an ac Josephson junction laser

NASA Astrophysics Data System (ADS)

Cassidy, M. C.; Bruno, A.; Rubbert, S.; Irfan, M.; Kammhuber, J.; Schouten, R. N.; Akhmerov, A. R.; Kouwenhoven, L. P.

2017-03-01

Superconducting electronic devices have reemerged as contenders for both classical and quantum computing due to their fast operation speeds, low dissipation, and long coherence times. An ultimate demonstration of coherence is lasing. We use one of the fundamental aspects of superconductivity, the ac Josephson effect, to demonstrate a laser made from a Josephson junction strongly coupled to a multimode superconducting cavity. A dc voltage bias applied across the junction provides a source of microwave photons, and the circuit’s nonlinearity allows for efficient down-conversion of higher-order Josephson frequencies to the cavity’s fundamental mode. The simple fabrication and operation allows for easy integration with a range of quantum devices, allowing for efficient on-chip generation of coherent microwave photons at low temperatures.

Study of extending carrier lifetime in ZnTe quantum dots coupled with ZnCdSe quantum well

NASA Astrophysics Data System (ADS)

Fan, W. C.; Chou, W. C.; Lee, J. D.; Lee, Ling; Phu, Nguyen Dang; Hoang, Luc Huy

2018-03-01

We demonstrated the growth of a self-assembled type-II ZnTe/ZnSe quantum dot (QD) structure coupled with a type-I Zn0.88Cd0.12Se/ZnSe quantum well (QW) on the (001) GaAs substrate by molecular beam epitaxy (MBE). As the spacer thickness is less than 2 nm, the carrier lifetime increasing from 20 ns to nearly 200 ns was successfully achieved. By utilizing the time-resolved photoluminescence (TRPL) and PL with different excitation power, we identify the PL emission from the coupled QDs consisting of two recombination mechanisms. One is the recombination between electrons in ZnSe barrier and holes confined within ZnTe QDs, and the other is between electrons confined in Zn0.88Cd0.12Se QW and holes confined within ZnTe QDs. According to the band diagram and power-dependent PL, both of the two recombinations reveal the type-II transition. In addition, the second recombination mechanism dominates the whole carrier recombination as the spacer thickness is less than 2 nm. A significant extension of carrier lifetime by increasing the electron and hole separation is illustrated in a type-II ZnTe/ZnSe QD structure coupling with a type-I ZnCdSe/ZnSe QW. Current sample structure could be used to increase the quantum efficient of solar cell based on the II-VI compound semiconductors.

Self-consistent field for fragmented quantum mechanical model of large molecular systems.

PubMed

Jin, Yingdi; Su, Neil Qiang; Xu, Xin; Hu, Hao

2016-01-30

Fragment-based linear scaling quantum chemistry methods are a promising tool for the accurate simulation of chemical and biomolecular systems. Because of the coupled inter-fragment electrostatic interactions, a dual-layer iterative scheme is often employed to compute the fragment electronic structure and the total energy. In the dual-layer scheme, the self-consistent field (SCF) of the electronic structure of a fragment must be solved first, then followed by the updating of the inter-fragment electrostatic interactions. The two steps are sequentially carried out and repeated; as such a significant total number of fragment SCF iterations is required to converge the total energy and becomes the computational bottleneck in many fragment quantum chemistry methods. To reduce the number of fragment SCF iterations and speed up the convergence of the total energy, we develop here a new SCF scheme in which the inter-fragment interactions can be updated concurrently without converging the fragment electronic structure. By constructing the global, block-wise Fock matrix and density matrix, we prove that the commutation between the two global matrices guarantees the commutation of the corresponding matrices in each fragment. Therefore, many highly efficient numerical techniques such as the direct inversion of the iterative subspace method can be employed to converge simultaneously the electronic structure of all fragments, reducing significantly the computational cost. Numerical examples for water clusters of different sizes suggest that the method shall be very useful in improving the scalability of fragment quantum chemistry methods. © 2015 Wiley Periodicals, Inc.

Modeling of Noise and Resistance of Semimetal Hg1-xCdxTe Quantum Well used as a Channel for THz Hot-Electron Bolometer.

PubMed

Melezhik, E O; Gumenjuk-Sichevska, J V; Sizov, F F

2016-12-01

Noise characteristics and resistance of semimetal-type mercury-cadmium-telluride quantum wells (QWs) at the liquid nitrogen temperature are studied numerically, and their dependence on the QW parameters and on the electron concentration is established. The QW band structure calculations are based on the full 8-band k.p Hamiltonian. The electron mobility is simulated by the direct iterative solution of the Boltzmann transport equation, which allows us to include correctly all the principal scattering mechanisms, elastic as well as inelastic.We find that the generation-recombination noise is strongly suppressed due to the very fast recombination processes in semimetal QWs. Hence, the thermal noise should be considered as a main THz sensitivity-limiting mechanism in those structures. Optimization of a semimetal Hg1-xCdxTe QW to make it an efficient THz bolometer channel should include the increase of electron concentration in the well and tuning the molar composition x close to the gapless regime.

Versatile Molecular Functionalization for Inhibiting Concentration Quenching of Thermally Activated Delayed Fluorescence.

PubMed

Lee, Jiyoung; Aizawa, Naoya; Numata, Masaki; Adachi, Chihaya; Yasuda, Takuma

2017-01-01

Concentration quenching of thermally activated delayed fluorescence is found to be dominated by electron-exchange interactions, as described by the Dexter energy-transfer model. Owing to the short-range nature of the electron-exchange interactions, even a small modulation in the molecular geometric structure drastically affects the concentration-quenching, leading to enhanced solid-state photoluminescence and electroluminescence quantum efficiencies. © 2016 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Implementing a quantum cloning machine in separate cavities via the optical coherent pulse as a quantum communication bus

NASA Astrophysics Data System (ADS)

Zhu, Meng-Zheng; Ye, Liu

2015-04-01

An efficient scheme is proposed to implement a quantum cloning machine in separate cavities based on a hybrid interaction between electron-spin systems placed in the cavities and an optical coherent pulse. The coefficient of the output state for the present cloning machine is just the direct product of two trigonometric functions, which ensures that different types of quantum cloning machine can be achieved readily in the same framework by appropriately adjusting the rotated angles. The present scheme can implement optimal one-to-two symmetric (asymmetric) universal quantum cloning, optimal symmetric (asymmetric) phase-covariant cloning, optimal symmetric (asymmetric) real-state cloning, optimal one-to-three symmetric economical real-state cloning, and optimal symmetric cloning of qubits given by an arbitrary axisymmetric distribution. In addition, photon loss of the qubus beams during the transmission and decoherence effects caused by such a photon loss are investigated.

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

Hodgson, P. D., E-mail: pdhodgson@hotmail.co.uk; Hayne, M.; Robson, A. J.

We report the results of continuous and time-resolved photoluminescence measurements on type-II GaSb quantum rings embedded within GaAs/Al{sub x}Ga{sub 1−x}As quantum wells. A range of samples were grown with different well widths, compensation-doping concentrations within the wells, and number of quantum-ring layers. We find that each of these variants have no discernible effect on the radiative recombination, except for the very narrowest (5 nm) quantum well. In contrast, single-particle numerical simulations of the sample predict changes in photoluminescence energy of up to 200 meV. This remarkable difference is explained by the strong Coulomb binding of electrons to rings that are multiply chargedmore » with holes. The resilience of the emission to compensation doping indicates that multiple hole occupancy of the quantum rings is required for efficient carrier recombination, regardless of whether these holes come from doping or excitation.« less

High-efficiency emitting materials based on phenylquinoline/carbazole-based compounds for organic light emitting diode applications

NASA Astrophysics Data System (ADS)

Jin, Sung-Ho

2009-08-01

Highly efficient light-emitting materials based on phenylquinoline-carbazole derivative has been synthesized for organic-light emitting diodes (OLEDs). The materials form high quality amorphous thin films by thermal evaporation and the energy levels can be easily adjusted by the introduction of different electron donating and electron withdrawing groups on carbazoylphenylquinoline. Non-doped deep-blue OLEDs using Et-CVz-PhQ as the emitter show bright emission (CIE coordinates, x=0.156, y=0.093) with an external quantum efficiency of 2.45 %. Furthermore, the material works as an excellent host material for BCzVBi to get high-performance OLEDs with excellent deep-blue CIE coordinates (x=0.155, y=0.157), high power efficiency (5.98 lm/W), and high external quantum efficiency (5.22 %). Cyclometalated Ir(III) μ-chloride bridged dimers were synthesized by iridium trichloride hydrate with an excess of our developed deep-blue emitter, Et-CVz-PhQ. The Ir(III) complexes were prepared by the dimers with the corresponding ancillary ligands. The chloride bridged diiridium complexes can be easily converted to mononuclear Ir(III) complexes by replacing the two bridging chlorides with bidentate monoanionic ancillary ligands. Among the various types of ancillary ligands, we firstly used picolinic acid N-oxide, including picolinic acid and acetylacetone as an ancillary ligands for Ir(III) complexes. The PhOLEDs also shows reasonably high brightness and good luminance efficiency of 20,000 cd/m2 and 12 cd/A, respectively.

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 charge dynamics by identifying states in these quantum dot materials which facilitate carrier transport. Thermal activation energies for transport of 60 meV or lower were measured for different PbS quantum dot bandgaps, representing a relatively small barrier for carrier transport. From these measurements a dark, quantum confined energy level was attributed to the electronic bandedge of these materials which serves to govern their optoelectronic behavior.

Silicon Germanium Quantum Well Thermoelectrics

NASA Astrophysics Data System (ADS)

Davidson, Anthony Lee, III

Today's growing energy demands require new technologies to provide high efficiency clean energy. Thermoelectrics that convert heat to electrical energy directly can provide a method for the automobile industry to recover waste heat to power vehicle electronics, hence improving fuel economy. If large enough efficiencies can be obtained then the internal combustion engine could even be replaced. Exhaust temperature for automotive application range from 400 to 800 K. In this temperature range the current state of the art materials are bulk Si1-xGex alloys. By alternating layers of Si and Si1-xGex alloy device performance may be enhanced through quantum well effects and variations in material thermal properties. In this study, superlattices designed for in-plane operation with varying period and crystallinity are examined to determine the effect on electrical and thermal properties. In-plane electrical resistivity of these materials was found to be below the bulk material at a similar doping at room temperature, confirming the role of quantum wells in electron transport. As period is reduced in the structures boundary scattering limits electron propagation leading to increased resistivity. The Seebeck coefficient measured at room temperature is higher than the bulk material, additionally lending proof to the effects of quantum wells. When examining cross-plane operation the low doping in the Si layers of the device produce high resistivity resulting from boundary scattering. Thermal conductivity was measured from 77 K up to 674 K and shows little variation due to periodicity and temperature, however an order of magnitude reduction over bulk Si1-xGex is shown in all samples. A model is developed that suggests a combination of phonon dispersion effects and strong boundary scattering. Further study of the phonon dispersion effects was achieved through the examination of the heat capacity by combining thermal diffusivity with thermal conductivity. All superlattices show a reduction in heat capacity when compared to Si, suggesting the importance of phonon dispersion effects due to the periodicity. The Debye model does not provide agreement with this result due to the inadequate treatment of optical phonons. Overall the results show that the design of the superlattice structures results in a thermoelectric that has improved efficiency at room temperature to the state of the art materials with the promise of increased efficiency at higher temperatures.

Microscopic models of non-radiative and high-current effects in LEDs: state of the art and future developments

NASA Astrophysics Data System (ADS)

Bertazzi, Francesco; Goano, Michele; Calciati, Marco; Zhou, Xiangyu; Ghione, Giovanni; Bellotti, Enrico

2014-02-01

Auger recombination is at the hearth of the debate on droop, the decline of the internal quantum efficiency at high injection levels. The theory of Auger recombination in quantum wells is reviewed. The proposed microscopic model is based on a full-Brillouin-zone description of the electronic structure obtained by nonlocal empirical pseudopotential calculations and the linear combination of bulk bands. The lack of momentum conservation along the confining direction in InGaN/GaN quantum wells enhances direct (i.e. phononless) Auger transitions, leading to Auger coefficients in the range of those predicted for phonon-dressed processes in bulk InGaN.

Thermoelectric effect in an Aharonov-Bohm ring with an embedded quantum dot.

PubMed

Zheng, Jun; Chi, Feng; Lu, Xiao-Dong; Zhang, Kai-Cheng

2012-02-28

Thermoelectric effect is studied in an Aharonov-Bohm interferometer with an embedded quantum dot (QD) in the Coulomb blockade regime. The electrical conductance, electron thermal conductance, thermopower, and thermoelectric figure-of-merit are calculated by using the Keldysh Green's function method. It is found that the figure-of-merit ZT of the QD ring may be quite high due to the Fano effect originated from the quantum interference effect. Moreover, the thermoelectric efficiency is sensitive to the magnitude of the dot-lead and inter-lead coupling strengthes. The effect of intradot Coulomb repulsion on ZT is significant in the weak-coupling regime, and then large ZT values can be obtained at rather high temperature.

Reducing inhomogeneity in the dynamic properties of quantum dots via self-aligned plasmonic cavities

NASA Astrophysics Data System (ADS)

Demory, Brandon; Hill, Tyler A.; Teng, Chu-Hsiang; Deng, Hui; Ku, P. C.

2018-01-01

A plasmonic cavity is shown to greatly reduce the inhomogeneity of dynamic optical properties such as quantum efficiency and radiative lifetime of InGaN quantum dots. By using an open-top plasmonic cavity structure, which exhibits a large Purcell factor and antenna quantum efficiency, the resulting quantum efficiency distribution for the quantum dots narrows and is no longer limited by the quantum dot inhomogeneity. The standard deviation of the quantum efficiency can be reduced to 2% while maintaining the overall quantum efficiency at 70%, making InGaN quantum dots a viable candidate for high-speed quantum cryptography and random number generation applications.

Reducing inhomogeneity in the dynamic properties of quantum dots via self-aligned plasmonic cavities.

PubMed

Demory, Brandon; Hill, Tyler A; Teng, Chu-Hsiang; Deng, Hui; Ku, P C

2018-01-05

A plasmonic cavity is shown to greatly reduce the inhomogeneity of dynamic optical properties such as quantum efficiency and radiative lifetime of InGaN quantum dots. By using an open-top plasmonic cavity structure, which exhibits a large Purcell factor and antenna quantum efficiency, the resulting quantum efficiency distribution for the quantum dots narrows and is no longer limited by the quantum dot inhomogeneity. The standard deviation of the quantum efficiency can be reduced to 2% while maintaining the overall quantum efficiency at 70%, making InGaN quantum dots a viable candidate for high-speed quantum cryptography and random number generation applications.

Highly Efficient Inverted Perovskite Solar Cells with CdSe QDs/LiF Electron Transporting Layer

NASA Astrophysics Data System (ADS)

Tan, Furui; Xu, Weizhe; Hu, Xiaodong; Yu, Ping; Zhang, Weifeng

2017-12-01

Organic/inorganic hybrid perovskite solar cell has emerged as a very promising candidate for the next generation of near-commercial photovoltaic devices. Here in this work, we focus on the inverted perovskite solar cells and have found that remarkable photovoltaic performance could be obtained when using cadmium selenide (CdSe) quantum dots (QDs) as electron transporting layer (ETL) and lithium fluoride (LiF) as the buffer, with respect to the traditionally applied and high-cost [6,6]-phenyl-C61-butyric acid methyl ester (PCBM). The easily processed and low-cost CdSe QDs/LiF double layer could facilitate convenient electron-transfer and collection at the perovskite/cathode interface, promoting an optoelectric conversion efficiency of as high as 15.1%, very close to that with the traditional PCBM ETL. Our work provides another promising choice on the ETL materials for the highly efficient and low-cost perovskite solar cells.

On the origin of the electron blocking effect by an n-type AlGaN electron blocking layer

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

Zhang, Zi-Hui; Ji, Yun; Liu, Wei

2014-02-17

In this work, the origin of electron blocking effect of n-type Al{sub 0.25}Ga{sub 0.75}N electron blocking layer (EBL) for c+ InGaN/GaN light-emitting diodes has been investigated through dual-wavelength emission method. It is found that the strong polarization induced electric field within the n-EBL reduces the thermal velocity and correspondingly the mean free path of the hot electrons. As a result, the electron capture efficiency of the multiple quantum wells is enhanced, which significantly reduces the electron overflow from the active region and increases the radiative recombination rate with holes.

Detective quantum efficiency of photon-counting x-ray detectors

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

Tanguay, Jesse, E-mail: jessetan@mail.ubc.ca; Yun, Seungman; Kim, Ho Kyung

Purpose: Single-photon-counting (SPC) x-ray imaging has the potential to improve image quality and enable novel energy-dependent imaging methods. Similar to conventional detectors, optimizing image SPC quality will require systems that produce the highest possible detective quantum efficiency (DQE). This paper builds on the cascaded-systems analysis (CSA) framework to develop a comprehensive description of the DQE of SPC detectors that implement adaptive binning. Methods: The DQE of SPC systems can be described using the CSA approach by propagating the probability density function (PDF) of the number of image-forming quanta through simple quantum processes. New relationships are developed to describe PDF transfermore » through serial and parallel cascades to accommodate scatter reabsorption. Results are applied to hypothetical silicon and selenium-based flat-panel SPC detectors including the effects of reabsorption of characteristic/scatter photons from photoelectric and Compton interactions, stochastic conversion of x-ray energy to secondary quanta, depth-dependent charge collection, and electronic noise. Results are compared with a Monte Carlo study. Results: Depth-dependent collection efficiency can result in substantial broadening of photopeaks that in turn may result in reduced DQE at lower x-ray energies (20–45 keV). Double-counting interaction events caused by reabsorption of characteristic/scatter photons may result in falsely inflated image signal-to-noise ratio and potential overestimation of the DQE. Conclusions: The CSA approach is extended to describe signal and noise propagation through photoelectric and Compton interactions in SPC detectors, including the effects of escape and reabsorption of emission/scatter photons. High-performance SPC systems can be achieved but only for certain combinations of secondary conversion gain, depth-dependent collection efficiency, electronic noise, and reabsorption characteristics.« less

Detective quantum efficiency of photon-counting x-ray detectors.

PubMed

Tanguay, Jesse; Yun, Seungman; Kim, Ho Kyung; Cunningham, Ian A

2015-01-01

Single-photon-counting (SPC) x-ray imaging has the potential to improve image quality and enable novel energy-dependent imaging methods. Similar to conventional detectors, optimizing image SPC quality will require systems that produce the highest possible detective quantum efficiency (DQE). This paper builds on the cascaded-systems analysis (CSA) framework to develop a comprehensive description of the DQE of SPC detectors that implement adaptive binning. The DQE of SPC systems can be described using the CSA approach by propagating the probability density function (PDF) of the number of image-forming quanta through simple quantum processes. New relationships are developed to describe PDF transfer through serial and parallel cascades to accommodate scatter reabsorption. Results are applied to hypothetical silicon and selenium-based flat-panel SPC detectors including the effects of reabsorption of characteristic/scatter photons from photoelectric and Compton interactions, stochastic conversion of x-ray energy to secondary quanta, depth-dependent charge collection, and electronic noise. Results are compared with a Monte Carlo study. Depth-dependent collection efficiency can result in substantial broadening of photopeaks that in turn may result in reduced DQE at lower x-ray energies (20-45 keV). Double-counting interaction events caused by reabsorption of characteristic/scatter photons may result in falsely inflated image signal-to-noise ratio and potential overestimation of the DQE. The CSA approach is extended to describe signal and noise propagation through photoelectric and Compton interactions in SPC detectors, including the effects of escape and reabsorption of emission/scatter photons. High-performance SPC systems can be achieved but only for certain combinations of secondary conversion gain, depth-dependent collection efficiency, electronic noise, and reabsorption characteristics.

Interplay between structure, stoichiometry, and electron transfer dynamics in SILAR-based quantum dot-sensitized oxides.

PubMed

Wang, Hai; Barceló, Irene; Lana-Villarreal, Teresa; Gómez, Roberto; Bonn, Mischa; Cánovas, Enrique

2014-10-08

We quantify the rate and efficiency of picosecond electron transfer (ET) from PbS nanocrystals, grown by successive ionic layer adsorption and reaction (SILAR), into a mesoporous SnO2 support. Successive SILAR deposition steps allow for stoichiometry- and size-variation of the QDs, characterized using transmission electron microscopy. Whereas for sulfur-rich (p-type) QD surfaces substantial electron trapping at the QD surface occurs, for lead-rich (n-type) QD surfaces, the QD trapping channel is suppressed and the ET efficiency is boosted. The ET efficiency increase achieved by lead-rich QD surfaces is found to be QD-size dependent, increasing linearly with QD surface area. On the other hand, ET rates are found to be independent of both QD size and surface stoichiometry, suggesting that the donor-acceptor energetics (constituting the driving force for ET) are fixed due to Fermi level pinning at the QD/oxide interface. Implications of our results for QD-sensitized solar cell design are discussed.

QM/QM approach to model energy disorder in amorphous organic semiconductors.

PubMed

Friederich, Pascal; Meded, Velimir; Symalla, Franz; Elstner, Marcus; Wenzel, Wolfgang

2015-02-10

It is an outstanding challenge to model the electronic properties of organic amorphous materials utilized in organic electronics. Computation of the charge carrier mobility is a challenging problem as it requires integration of morphological and electronic degrees of freedom in a coherent methodology and depends strongly on the distribution of polaron energies in the system. Here we represent a QM/QM model to compute the polaron energies combining density functional methods for molecules in the vicinity of the polaron with computationally efficient density functional based tight binding methods in the rest of the environment. For seven widely used amorphous organic semiconductor materials, we show that the calculations are accelerated up to 1 order of magnitude without any loss in accuracy. Considering that the quantum chemical step is the efficiency bottleneck of a workflow to model the carrier mobility, these results are an important step toward accurate and efficient disordered organic semiconductors simulations, a prerequisite for accelerated materials screening and consequent component optimization in the organic electronics industry.

LASER APPLICATIONS AND OTHER TOPICS IN QUANTUM ELECTRONICS: Mechanism for shock wave merging in magnetised plasma: criteria and efficiency of formation of low-frequency magnetosonic waves

NASA Astrophysics Data System (ADS)

Tishchenko, V. N.; Shaikhislamov, I. F.

2010-08-01

The mechanism of merging of shock waves produced by a pulsating energy source is considered for magnetised plasma. The criteria for the emergence of this mechanism are found and its high efficiency for producing low-frequency magnetosonic waves, which have the form of a jet and propagate at large distances without attenuation, is shown.

Quantum interference in plasmonic circuits.

PubMed

Heeres, Reinier W; Kouwenhoven, Leo P; Zwiller, Valery

2013-10-01

Surface plasmon polaritons (plasmons) are a combination of light and a collective oscillation of the free electron plasma at metal/dielectric interfaces. This interaction allows subwavelength confinement of light beyond the diffraction limit inherent to dielectric structures. As a result, the intensity of the electromagnetic field is enhanced, with the possibility to increase the strength of the optical interactions between waveguides, light sources and detectors. Plasmons maintain non-classical photon statistics and preserve entanglement upon transmission through thin, patterned metallic films or weakly confining waveguides. For quantum applications, it is essential that plasmons behave as indistinguishable quantum particles. Here we report on a quantum interference experiment in a nanoscale plasmonic circuit consisting of an on-chip plasmon beamsplitter with integrated superconducting single-photon detectors to allow efficient single plasmon detection. We demonstrate a quantum-mechanical interaction between pairs of indistinguishable surface plasmons by observing Hong-Ou-Mandel (HOM) interference, a hallmark non-classical interference effect that is the basis of linear optics-based quantum computation. Our work shows that it is feasible to shrink quantum optical experiments to the nanoscale and offers a promising route towards subwavelength quantum optical networks.

InGaAs/InP quantum wires grown on silicon with adjustable emission wavelength at telecom bands

NASA Astrophysics Data System (ADS)

Han, Yu; Li, Qiang; Ng, Kar Wei; Zhu, Si; Lau, Kei May

2018-06-01

We report the growth of vertically stacked InGaAs/InP quantum wires on (001) Si substrates with adjustable room-temperature emission at telecom bands. Based on a self-limiting growth mode in selective area metal–organic chemical vapor deposition, crescent-shaped InGaAs quantum wires with variable dimensions are embedded within InP nano-ridges. With extensive transmission electron microscopy studies, the growth transition and morphology change from quantum wires to ridge quantum wells (QWs) have been revealed. As a result, we are able to decouple the quantum wires from ridge QWs and manipulate their dimensions by scaling the growth time. With minimized lateral dimension and their unique positioning, the InGaAs/InP quantum wires are more immune to dislocations and more efficient in radiative processes, as evidenced by their excellent optical quality at telecom-bands. These promising results thus highlight the potential of combining low-dimensional quantum wire structures with the aspect ratio trapping process for integrating III–V nano-light emitters on mainstream (001) Si substrates.

InGaAs/InP quantum wires grown on silicon with adjustable emission wavelength at telecom bands.

PubMed

Han, Yu; Li, Qiang; Ng, Kar Wei; Zhu, Si; Lau, Kei May

2018-06-01

We report the growth of vertically stacked InGaAs/InP quantum wires on (001) Si substrates with adjustable room-temperature emission at telecom bands. Based on a self-limiting growth mode in selective area metal-organic chemical vapor deposition, crescent-shaped InGaAs quantum wires with variable dimensions are embedded within InP nano-ridges. With extensive transmission electron microscopy studies, the growth transition and morphology change from quantum wires to ridge quantum wells (QWs) have been revealed. As a result, we are able to decouple the quantum wires from ridge QWs and manipulate their dimensions by scaling the growth time. With minimized lateral dimension and their unique positioning, the InGaAs/InP quantum wires are more immune to dislocations and more efficient in radiative processes, as evidenced by their excellent optical quality at telecom-bands. These promising results thus highlight the potential of combining low-dimensional quantum wire structures with the aspect ratio trapping process for integrating III-V nano-light emitters on mainstream (001) Si substrates.

Effects of nanoscale vacuum gap on photon-enhanced thermionic emission devices

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

Wang, Yuan; Liao, Tianjun; Zhang, Yanchao

2016-01-28

A new model of the photon-enhanced thermionic emission (PETE) device with a nanoscale vacuum gap is established by introducing the quantum tunneling effect and the image force correction. Analytic expressions for both the thermionic emission and tunneling currents are derived. The electron concentration and the temperature of the cathode are determined by the particle conservation and energy balance equations. The effects of the operating voltage on the maximum potential barrier, cathode temperature, electron concentration and equilibrium electron concentration of the conduction band, and efficiency of the PETE device are discussed in detail for different given values of the vacuum gapmore » length. The influence of the band gap of the cathode and flux concentration on the efficiency is further analyzed. The maximum efficiency of the PETE and the corresponding optimum values of the band gap and the operating voltage are determined. The results obtained here show that the efficiency of the PETE device can be significantly improved by employing a nanoscale vacuum gap.« less

Substantially Enhancing Quantum Coherence of Electrons in Graphene via Electron-Plasmon Coupling.

PubMed

Cheng, Guanghui; Qin, Wei; Lin, Meng-Hsien; Wei, Laiming; Fan, Xiaodong; Zhang, Huayang; Gwo, Shangjr; Zeng, Changgan; Hou, J G; Zhang, Zhenyu

2017-10-13

The interplays between different quasiparticles in solids lay the foundation for a wide spectrum of intriguing quantum effects, yet how the collective plasmon excitations affect the quantum transport of electrons remains largely unexplored. Here we provide the first demonstration that when the electron-plasmon coupling is introduced, the quantum coherence of electrons in graphene is substantially enhanced with the quantum coherence length almost tripled. We further develop a microscopic model to interpret the striking observations, emphasizing the vital role of the graphene plasmons in suppressing electron-electron dephasing. The novel and transformative concept of plasmon-enhanced quantum coherence sheds new insight into interquasiparticle interactions, and further extends a new dimension to exploit nontrivial quantum phenomena and devices in solid systems.

On the front and back side quantum efficiency differences in semi-transparent organic solar cells and photodiodes

NASA Astrophysics Data System (ADS)

Bouthinon, B.; Clerc, R.; Verilhac, J. M.; Racine, B.; De Girolamo, J.; Jacob, S.; Lienhard, P.; Joimel, J.; Dhez, O.; Revaux, A.

2018-03-01

The External Quantum Efficiency (EQE) of semi-transparent Bulk Hetero-Junction (BHJ) organic photodiodes processed in air shows significant differences when measured from the front or back side contacts. This difference was found significantly reduced when decreasing the active layer thickness or by applying a negative bias. This work brings new elements to help understanding this effect, providing a large set of experiments featuring different applied voltages, active layers, process conditions, and electron and hole layers. By means of detailed electrical simulations, all these measurements have been found consistent with the mechanisms of irreversible photo-oxidation, modeled as deep trap states (and not as p-type doping). The EQE measurement from front and back sides is thus a simple and efficient way of monitoring the presence and amplitude of oxygen contamination in BHJ organic solar cells and photodiodes.

A hole accelerator for InGaN/GaN light-emitting diodes

NASA Astrophysics Data System (ADS)

Zhang, Zi-Hui; Liu, Wei; Tan, Swee Tiam; Ji, Yun; Wang, Liancheng; Zhu, Binbin; Zhang, Yiping; Lu, Shunpeng; Zhang, Xueliang; Hasanov, Namig; Sun, Xiao Wei; Demir, Hilmi Volkan

2014-10-01

The quantum efficiency of InGaN/GaN light-emitting diodes (LEDs) has been significantly limited by the insufficient hole injection, and this is caused by the inefficient p-type doping and the low hole mobility. The low hole mobility makes the holes less energetic, which hinders the hole injection into the multiple quantum wells (MQWs) especially when a p-type AlGaN electron blocking layer (EBL) is adopted. In this work, we report a hole accelerator to accelerate the holes so that the holes can obtain adequate kinetic energy, travel across the p-type EBL, and then enter the MQWs more efficiently and smoothly. In addition to the numerical study, the effectiveness of the hole accelerator is experimentally shown through achieving improved optical output power and reduced efficiency droop for the proposed InGaN/GaN LED.

Maximizing the short circuit current of organic solar cells by partial decoupling of electrical and optical properties

NASA Astrophysics Data System (ADS)

Qarony, Wayesh; Hossain, Mohammad I.; Jovanov, Vladislav; Knipp, Dietmar; Tsang, Yuen Hong

2018-03-01

The partial decoupling of electronic and optical properties of organic solar cells allows for realizing solar cells with increased short circuit current and energy conversion efficiency. The proposed device consists of an organic solar cell conformally prepared on the surface of an array of single and double textured pyramids. The device geometry allows for increasing the optical thickness of the organic solar cell, while the electrical thickness is equal to the nominal thickness of the solar cell. By increasing the optical thickness of the solar cell, the short circuit current is distinctly increased. The quantum efficiency and short circuit current are determined using finite-difference time-domain simulations of the 3D solar cell structure. The influence of different solar cell designs on the quantum efficiency and short circuit current is discussed and optimal device dimensions are proposed.

Quantum Dot-Induced Phase Stabilization of ..alpha..-CsPbI3 Perovskite for High-Efficiency Photovoltaics

DOE PAGES

Swarnkar, Abhishek; Marshall, Ashley R.; Sanehira, Erin M.; ...

2016-10-07

Here, we show nanoscale phase stabilization of CsPbI 3 quantum dots (QDs) to low temperatures that can be used as the active component of efficient optoelectronic devices. CsPbI 3 is an all-inorganic analog to the hybrid organic cation halide perovskites, but the cubic phase of bulk CsPbI3 (..alpha..-CsPbI 3) -- the variant with desirable band gap -- is only stable at high temperatures. We also describe the formation of ..alpha..-CsPbI 3 QD films that are phase-stable for months in ambient air. The films exhibit long-range electronic transport and were used to fabricate colloidal perovskite QD photovoltaic cells with an open-circuitmore » voltage of 1.23 volts and efficiency of 10.77%. Furthermore, these devices function as light-emitting diodes with low turn-on voltage and tunable emission.« less

Increase in the Shockley–Read–Hall recombination rate in InGaN/GaN QWs as the main mechanism of the efficiency droop in LEDs at high injection levels

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

Bochkareva, N. I.; Rebane, Yu. T.; Shreter, Yu. G., E-mail: y.shreter@mail.ioffe.ru

It is shown that the efficiency droop observed as the current through a GaN-based light-emitting diode increases is due to a decrease in the Shockley–Read–Hall nonradiative lifetime. The lifetime decreases with increasing current because a steadily growing number of traps in the density-of-states tails of InGaN/GaN quantum wells become nonradiative recombination centers upon the approach of quasi-Fermi levels to the band edges. This follows from the correlation between the efficiency droop and the appearance of negative differential capacitance, observed in the study. The correlation appears due to slow trap recharging via the trap-assisted tunneling of electrons through the n-type barriermore » of the quantum well and to the inductive nature of the diode-current variation with forward bias.« less

Communication: An efficient and accurate perturbative correction to initiator full configuration interaction quantum Monte Carlo

NASA Astrophysics Data System (ADS)

Blunt, Nick S.

2018-06-01

We present a perturbative correction within initiator full configuration interaction quantum Monte Carlo (i-FCIQMC). In the existing i-FCIQMC algorithm, a significant number of spawned walkers are discarded due to the initiator criteria. Here we show that these discarded walkers have a form that allows the calculation of a second-order Epstein-Nesbet correction, which may be accumulated in a trivial and inexpensive manner, yet substantially improves i-FCIQMC results. The correction is applied to the Hubbard model and the uniform electron gas and molecular systems.

Entanglement of atomic qubits using an optical frequency comb.

PubMed

Hayes, D; Matsukevich, D N; Maunz, P; Hucul, D; Quraishi, Q; Olmschenk, S; Campbell, W; Mizrahi, J; Senko, C; Monroe, C

2010-04-09

We demonstrate the use of an optical frequency comb to coherently control and entangle atomic qubits. A train of off-resonant ultrafast laser pulses is used to efficiently and coherently transfer population between electronic and vibrational states of trapped atomic ions and implement an entangling quantum logic gate with high fidelity. This technique can be extended to the high field regime where operations can be performed faster than the trap frequency. This general approach can be applied to more complex quantum systems, such as large collections of interacting atoms or molecules.

Negative Difference Resistance and Its Application to Construct Boolean Logic Circuits

NASA Astrophysics Data System (ADS)

Nikodem, Maciej; Bawiec, Marek A.; Surmacz, Tomasz R.

Electronic circuits based on nanodevices and quantum effect are the future of logic circuits design. Today's technology allows constructing resonant tunneling diodes, quantum cellular automata and nanowires/nanoribbons that are the elementary components of threshold gates. However, synthesizing a threshold circuit for an arbitrary logic function is still a challenging task where no efficient algorithms exist. This paper focuses on Generalised Threshold Gates (GTG), giving the overview of threshold circuit synthesis methods and presenting an algorithm that considerably simplifies the task in case of GTG circuits.

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.

Graphene shield enhanced photocathodes and methods for making the same

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

Moody, Nathan Andrew

Disclosed are graphene shield enhanced photocathodes, such as high QE photocathodes. In certain embodiments, a monolayer graphene shield membrane ruggedizes a high quantum efficiency photoemission electron source by protecting a photosensitive film of the photocathode, extending operational lifetime and simplifying its integration in practical electron sources. In certain embodiments of the disclosed graphene shield enhanced photocathodes, the graphene serves as a transparent shield that does not inhibit photon or electron transmission but isolates the photosensitive film of the photocathode from reactive gas species, preventing contamination and yielding longer lifetime.

Optimal control of universal quantum gates in a double quantum dot

NASA Astrophysics Data System (ADS)

Castelano, Leonardo K.; de Lima, Emanuel F.; Madureira, Justino R.; Degani, Marcos H.; Maialle, Marcelo Z.

2018-06-01

We theoretically investigate electron spin operations driven by applied electric fields in a semiconductor double quantum dot (DQD) formed in a nanowire with longitudinal potential modulated by local gating. We develop a model that describes the process of loading and unloading the DQD taking into account the overlap between the electron wave function and the leads. Such a model considers the spatial occupation and the spin Pauli blockade in a time-dependent fashion due to the highly mixed states driven by the external electric field. Moreover, we present a road map based on the quantum optimal control theory (QOCT) to find a specific electric field that performs two-qubit quantum gates on a faster timescale and with higher possible fidelity. By employing the QOCT, we demonstrate the possibility of performing within high efficiency a universal set of quantum gates {cnot, H, and T } , where cnot is the controlled-not gate, H is the Hadamard gate, and T is the π /8 gate, even in the presence of the loading/unloading process and charge noise effects. Furthermore, by varying the intensity of the applied magnetic field B , the optimized fidelity of the gates oscillates with a period inversely proportional to the gate operation time tf. This behavior can be useful to attain higher fidelity for fast gate operations (>1 GHz) by appropriately choosing B and tf to produce a maximum of the oscillation.

Ultrafast atomic-scale visualization of acoustic phonons generated by optically excited quantum dots

PubMed Central

Vanacore, Giovanni M.; Hu, Jianbo; Liang, Wenxi; Bietti, Sergio; Sanguinetti, Stefano; Carbone, Fabrizio; Zewail, Ahmed H.

2017-01-01

Understanding the dynamics of atomic vibrations confined in quasi-zero dimensional systems is crucial from both a fundamental point-of-view and a technological perspective. Using ultrafast electron diffraction, we monitored the lattice dynamics of GaAs quantum dots—grown by Droplet Epitaxy on AlGaAs—with sub-picosecond and sub-picometer resolutions. An ultrafast laser pulse nearly resonantly excites a confined exciton, which efficiently couples to high-energy acoustic phonons through the deformation potential mechanism. The transient behavior of the measured diffraction pattern reveals the nonequilibrium phonon dynamics both within the dots and in the region surrounding them. The experimental results are interpreted within the theoretical framework of a non-Markovian decoherence, according to which the optical excitation creates a localized polaron within the dot and a travelling phonon wavepacket that leaves the dot at the speed of sound. These findings indicate that integration of a phononic emitter in opto-electronic devices based on quantum dots for controlled communication processes can be fundamentally feasible. PMID:28852685

Design of a high-bunch-charge 112-MHz superconducting RF photoemission electron source

NASA Astrophysics Data System (ADS)

Xin, T.; Brutus, J. C.; Belomestnykh, Sergey A.; Ben-Zvi, I.; Boulware, C. H.; Grimm, T. L.; Hayes, T.; Litvinenko, Vladimir N.; Mernick, K.; Narayan, G.; Orfin, P.; Pinayev, I.; Rao, T.; Severino, F.; Skaritka, J.; Smith, K.; Than, R.; Tuozzolo, J.; Wang, E.; Xiao, B.; Xie, H.; Zaltsman, A.

2016-09-01

High-bunch-charge photoemission electron-sources operating in a continuous wave (CW) mode are required for many advanced applications of particle accelerators, such as electron coolers for hadron beams, electron-ion colliders, and free-electron lasers. Superconducting RF (SRF) has several advantages over other electron-gun technologies in CW mode as it offers higher acceleration rate and potentially can generate higher bunch charges and average beam currents. A 112 MHz SRF electron photoinjector (gun) was developed at Brookhaven National Laboratory to produce high-brightness and high-bunch-charge bunches for the coherent electron cooling proof-of-principle experiment. The gun utilizes a quarter-wave resonator geometry for assuring beam dynamics and uses high quantum efficiency multi-alkali photocathodes for generating electrons.

Pyrimidine-based twisted donor-acceptor delayed fluorescence molecules: a new universal platform for highly efficient blue electroluminescence.

PubMed

Park, In Seob; Komiyama, Hideaki; Yasuda, Takuma

2017-02-01

Deep-blue emitters that can harvest both singlet and triplet excited states to give high electron-to-photon conversion efficiencies are highly desired for applications in full-color displays and white lighting devices based on organic light-emitting diodes (OLEDs). Thermally activated delayed fluorescence (TADF) molecules based on highly twisted donor-acceptor (D-A) configurations are promising emitting dopants for the construction of efficient deep-blue OLEDs. In this study, a simple and versatile D-A system combining acridan-based donors and pyrimidine-based acceptors has been developed as a new platform for high-efficiency deep-blue TADF emitters. The designed pre-twisted acridan-pyrimidine D-A molecules exhibit small singlet-triplet energy splitting and high photoluminescence quantum yields, functioning as efficient deep-blue TADF emitters. The OLEDs utilizing these TADF emitters display bright blue electroluminescence with external quantum efficiencies of up to 20.4%, maximum current efficiencies of 41.7 cd A -1 , maximum power efficiencies of 37.2 lm W -1 , and color coordinates of (0.16, 0.23). The design strategy featuring such acridan-pyrimidine D-A motifs can offer great prospects for further developing high-performance deep-blue TADF emitters and TADF-OLEDs.

Mitigating Structural Defects in Droop-Minimizing InGaN/GaN Quantum Well Heterostructures

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

Zhao, Zhibo; Chesin, Jordan; Singh, Akshay

2016-12-01

Modern commercial InGaN/GaN blue LEDs continue to suffer from efficiency droop, a reduction in efficiency with increasing drive current. External quantum efficiency (EQE) typically peaks at low drive currents (< 10 A cm 2) and drops monotonically at higher current densities, falling to <85% of the peak EQE at a drive current of 100 A cm 2. Mitigating droop-related losses will yield tremendous gains in both luminous efficacy (lumens/W) and cost (lumens/$). Such improvements are critical for continued large-scale market penetration of LED technologies, particularly in high-power and high flux per unit area applications. However, device structures that reduce droopmore » typically require higher indium content and are accompanied by a corresponding degradation in material quality which negates the droop improvement via enhanced Shockley-Read-Hall (SRH) recombination. In this work, we use advanced characterization techniques to identify and classify structural defects in InGaN/GaN quantum well (QW) heterostructures that share features with low-droop designs. Using aberration-corrected scanning transmission electron microscopy (C s-STEM), we find the presence of severe well width fluctuations (WWFs) in a number of low droop device architectures. However, the presence of WWFs does not correlate strongly with external quantum efficiency nor defect densities measured via deep level optical spectroscopy (DLOS). Hence, performance losses in the heterostructures of interest are likely dominated by nanoscale point or interfacial defects rather than large-scale extended defects.« less

Are hot charge transfer states the primary cause of efficient free-charge generation in polymer:fullerene organic photovoltaic devices? A kinetic Monte Carlo study.

PubMed

Jones, Matthew L; Dyer, Reesha; Clarke, Nigel; Groves, Chris

2014-10-14

Kinetic Monte Carlo simulations are used to examine the effect of high-energy, 'hot' delocalised charge transfer (HCT) states for donor:acceptor and mixed:aggregate blends, the latter relating to polymer:fullerene photovoltaic devices. Increased fullerene aggregation is shown to enhance charge generation and short-circuit device current - largely due to the increased production of HCT states at the aggregate interface. However, the instances where HCT states are predicted to give internal quantum efficiencies in the region of 50% do not correspond to HCT delocalisation or electron mobility measured in experiments. These data therefore suggest that HCT states are not the primary cause of high quantum efficiencies in some polymer:fullerene OPVs. Instead it is argued that HCT states are responsible for the fast charge generation seen in spectroscopy, but that regional variation in energy levels are the cause of long-term, efficient free-charge generation.

Recombination zone in white organic light emitting diodes with blue and orange emitting layers

NASA Astrophysics Data System (ADS)

Tsuboi, Taiju; Kishimoto, Tadashi; Wako, Kazuhiro; Matsuda, Kuniharu; Iguchi, Hirofumi

2012-10-01

White fluorescent OLED devices with a 10 nm thick blue-emitting layer and a 31 nm thick orange-emitting layer have been fabricated, where the blue-emitting layer is stacked on a hole transport layer. An interlayer was inserted between the two emitting layers. The thickness of the interlayer was changed among 0.3, 0.4, and 1.0 nm. White emission with CIE coordinates close to (0.33, 0.33) was observed from all the OLEDs. OLED with 0.3 nm thick interlayer gives the highest maximum luminous efficiency (11 cd/A), power efficiency (9 lm/W), and external quantum efficiency (5.02%). The external quantum efficiency becomes low with increasing the interlayer thickness from 0 nm to 1.0 nm. When the location of the blue- and orange-emitting layers is reversed, white emission was not obtained because of too weak blue emission. It is suggested that the electron-hole recombination zone decreases nearly exponentially with a distance from the hole transport layer.

Field-emission from quantum-dot-in-perovskite solids

PubMed Central

García de Arquer, F. Pelayo; Gong, Xiwen; Sabatini, Randy P.; Liu, Min; Kim, Gi-Hwan; Sutherland, Brandon R.; Voznyy, Oleksandr; Xu, Jixian; Pang, Yuangjie; Hoogland, Sjoerd; Sinton, David; Sargent, Edward

2017-01-01

Quantum dot and well architectures are attractive for infrared optoelectronics, and have led to the realization of compelling light sensors. However, they require well-defined passivated interfaces and rapid charge transport, and this has restricted their efficient implementation to costly vacuum-epitaxially grown semiconductors. Here we report solution-processed, sensitive infrared field-emission photodetectors. Using quantum-dots-in-perovskite, we demonstrate the extraction of photocarriers via field emission, followed by the recirculation of photogenerated carriers. We use in operando ultrafast transient spectroscopy to sense bias-dependent photoemission and recapture in field-emission devices. The resultant photodiodes exploit the superior electronic transport properties of organometal halide perovskites, the quantum-size-tuned absorption of the colloidal quantum dots and their matched interface. These field-emission quantum-dot-in-perovskite photodiodes extend the perovskite response into the short-wavelength infrared and achieve measured specific detectivities that exceed 1012 Jones. The results pave the way towards novel functional photonic devices with applications in photovoltaics and light emission. PMID:28337981

Free-Space Quantum Signatures Using Heterodyne Measurements

NASA Astrophysics Data System (ADS)

Croal, Callum; Peuntinger, Christian; Heim, Bettina; Khan, Imran; Marquardt, Christoph; Leuchs, Gerd; Wallden, Petros; Andersson, Erika; Korolkova, Natalia

2016-09-01

Digital signatures guarantee the authorship of electronic communications. Currently used "classical" signature schemes rely on unproven computational assumptions for security, while quantum signatures rely only on the laws of quantum mechanics to sign a classical message. Previous quantum signature schemes have used unambiguous quantum measurements. Such measurements, however, sometimes give no result, reducing the efficiency of the protocol. Here, we instead use heterodyne detection, which always gives a result, although there is always some uncertainty. We experimentally demonstrate feasibility in a real environment by distributing signature states through a noisy 1.6 km free-space channel. Our results show that continuous-variable heterodyne detection improves the signature rate for this type of scheme and therefore represents an interesting direction in the search for practical quantum signature schemes. For transmission values ranging from 100% to 10%, but otherwise assuming an ideal implementation with no other imperfections, the signature length is shorter by a factor of 2 to 10. As compared with previous relevant experimental realizations, the signature length in this implementation is several orders of magnitude shorter.

Controlling heat and particle currents in nanodevices by quantum observation

NASA Astrophysics Data System (ADS)

Biele, Robert; Rodríguez-Rosario, César A.; Frauenheim, Thomas; Rubio, Angel

2017-07-01

We demonstrate that in a standard thermo-electric nanodevice the current and heat flows are not only dictated by the temperature and potential gradient, but also by the external action of a local quantum observer that controls the coherence of the device. Depending on how and where the observation takes place, the direction of heat and particle currents can be independently controlled. In fact, we show that the current and heat flow in a quantum material can go against the natural temperature and voltage gradients. Dynamical quantum observation offers new possibilities for the control of quantum transport far beyond classical thermal reservoirs. Through the concept of local projections, we illustrate how we can create and directionality control the injection of currents (electronic and heat) in nanodevices. This scheme provides novel strategies to construct quantum devices with application in thermoelectrics, spintronic injection, phononics, and sensing among others. In particular, highly efficient and selective spin injection might be achieved by local spin projection techniques.

Enhanced photoluminescence of corrugated Al2O3 film assisted by colloidal CdSe quantum dots.

PubMed

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

2017-05-19

We present the enhanced photoluminescence (PL) of a corrugated Al 2 O 3 film enabled by colloidal CdSe quantum dots. The colloidal CdSe quantum dots are fabricated directly on a corrugated Al 2 O 3 substrate using an electrochemical deposition (ECD) method in a microfluidic system. The photoluminescence is excited by using a 150 nm diameter ultraviolet laser spot of a scanning near-field optical microscope. Owing to the electron transfer from the conduction band of the CdSe quantum dots to that of Al 2 O 3 , the enhanced photoluminescence effect is observed, which results from the increase in the recombination rate of electrons and holes on the Al 2 O 3 surface and the reduction in the fluorescence of the CdSe quantum dots. A periodically-fluctuating fluorescent spectrum was exhibited because of the periodical wire-like corrugated Al 2 O 3 surface serving as an optical grating. The spectral topographic map around the fluorescence peak from the Al 2 O 3 areas covered with CdSe quantum dots was unique and attributed to the uniform deposition of CdSe QDs on the corrugated Al 2 O 3 surface. We believe that the microfluidic ECD system and the surface enhanced fluorescence method described in this paper have potential applications in forming uniform optoelectronic films of colloidal quantum dots with controllable QD spacing and in boosting the fluorescent efficiency of weak PL devices.

Performance Enhancement of Organic Light-Emitting Diodes Using Electron-Injection Materials of Metal Carbonates

NASA Astrophysics Data System (ADS)

Shin, Jong-Yeol; Kim, Tae Wan; Kim, Gwi-Yeol; Lee, Su-Min; Shrestha, Bhanu; Hong, Jin-Woong

2016-05-01

Performance of organic light-emitting diodes was investigated depending on the electron-injection materials of metal carbonates (Li2CO3 and Cs2CO3 ); and number of layers. In order to improve the device efficiency, two types of devices were manufactured by using the hole-injection material (Teflon-amorphous fluoropolymer -AF) and electron-injection materials; one is a two-layer reference device ( ITO/Teflon-AF/Alq3/Al ) and the other is a three-layer device (ITO/Teflon-AF/Alq3/metal carbonate/Al). From the results of the efficiency for the devices with hole-injection layer and electron-injection layer, it was found that the electron-injection layer affects the electrical properties of the device more than the hole-injection layer. The external-quantum efficiency for the three-layer device with Li2CO3 and Cs2CO3 layer is improved by approximately six and eight times, respectively, compared with that of the two-layer reference device. It is thought that a use of electron-injection layer increases recombination rate of charge carriers by the active injection of electrons and the blocking of holes.

A multiscale quantum mechanics/electromagnetics method for device simulations.

PubMed

Yam, ChiYung; Meng, Lingyi; Zhang, Yu; Chen, GuanHua

2015-04-07

Multiscale modeling has become a popular tool for research applying to different areas including materials science, microelectronics, biology, chemistry, etc. In this tutorial review, we describe a newly developed multiscale computational method, incorporating quantum mechanics into electronic device modeling with the electromagnetic environment included through classical electrodynamics. In the quantum mechanics/electromagnetics (QM/EM) method, the regions of the system where active electron scattering processes take place are treated quantum mechanically, while the surroundings are described by Maxwell's equations and a semiclassical drift-diffusion model. The QM model and the EM model are solved, respectively, in different regions of the system in a self-consistent manner. Potential distributions and current densities at the interface between QM and EM regions are employed as the boundary conditions for the quantum mechanical and electromagnetic simulations, respectively. The method is illustrated in the simulation of several realistic systems. In the case of junctionless field-effect transistors, transfer characteristics are obtained and a good agreement between experiments and simulations is achieved. Optical properties of a tandem photovoltaic cell are studied and the simulations demonstrate that multiple QM regions are coupled through the classical EM model. Finally, the study of a carbon nanotube-based molecular device shows the accuracy and efficiency of the QM/EM method.

Quantum coherent optical phase modulation in an ultrafast transmission electron microscope.

PubMed

Feist, Armin; Echternkamp, Katharina E; Schauss, Jakob; Yalunin, Sergey V; Schäfer, Sascha; Ropers, Claus

2015-05-14

Coherent manipulation of quantum systems with light is expected to be a cornerstone of future information and communication technology, including quantum computation and cryptography. The transfer of an optical phase onto a quantum wavefunction is a defining aspect of coherent interactions and forms the basis of quantum state preparation, synchronization and metrology. Light-phase-modulated electron states near atoms and molecules are essential for the techniques of attosecond science, including the generation of extreme-ultraviolet pulses and orbital tomography. In contrast, the quantum-coherent phase-modulation of energetic free-electron beams has not been demonstrated, although it promises direct access to ultrafast imaging and spectroscopy with tailored electron pulses on the attosecond scale. Here we demonstrate the coherent quantum state manipulation of free-electron populations in an electron microscope beam. We employ the interaction of ultrashort electron pulses with optical near-fields to induce Rabi oscillations in the populations of electron momentum states, observed as a function of the optical driving field. Excellent agreement with the scaling of an equal-Rabi multilevel quantum ladder is obtained, representing the observation of a light-driven 'quantum walk' coherently reshaping electron density in momentum space. We note that, after the interaction, the optically generated superposition of momentum states evolves into a train of attosecond electron pulses. Our results reveal the potential of quantum control for the precision structuring of electron densities, with possible applications ranging from ultrafast electron spectroscopy and microscopy to accelerator science and free-electron lasers.

Quantum coherent optical phase modulation in an ultrafast transmission electron microscope

NASA Astrophysics Data System (ADS)

Feist, Armin; Echternkamp, Katharina E.; Schauss, Jakob; Yalunin, Sergey V.; Schäfer, Sascha; Ropers, Claus

2015-05-01

Coherent manipulation of quantum systems with light is expected to be a cornerstone of future information and communication technology, including quantum computation and cryptography. The transfer of an optical phase onto a quantum wavefunction is a defining aspect of coherent interactions and forms the basis of quantum state preparation, synchronization and metrology. Light-phase-modulated electron states near atoms and molecules are essential for the techniques of attosecond science, including the generation of extreme-ultraviolet pulses and orbital tomography. In contrast, the quantum-coherent phase-modulation of energetic free-electron beams has not been demonstrated, although it promises direct access to ultrafast imaging and spectroscopy with tailored electron pulses on the attosecond scale. Here we demonstrate the coherent quantum state manipulation of free-electron populations in an electron microscope beam. We employ the interaction of ultrashort electron pulses with optical near-fields to induce Rabi oscillations in the populations of electron momentum states, observed as a function of the optical driving field. Excellent agreement with the scaling of an equal-Rabi multilevel quantum ladder is obtained, representing the observation of a light-driven `quantum walk' coherently reshaping electron density in momentum space. We note that, after the interaction, the optically generated superposition of momentum states evolves into a train of attosecond electron pulses. Our results reveal the potential of quantum control for the precision structuring of electron densities, with possible applications ranging from ultrafast electron spectroscopy and microscopy to accelerator science and free-electron lasers.

Real-time dynamics of lattice gauge theories with a few-qubit quantum computer

NASA Astrophysics Data System (ADS)

Martinez, Esteban A.; Muschik, Christine A.; Schindler, Philipp; Nigg, Daniel; Erhard, Alexander; Heyl, Markus; Hauke, Philipp; Dalmonte, Marcello; Monz, Thomas; Zoller, Peter; Blatt, Rainer

2016-06-01

Gauge theories are fundamental to our understanding of interactions between the elementary constituents of matter as mediated by gauge bosons. However, computing the real-time dynamics in gauge theories is a notorious challenge for classical computational methods. This has recently stimulated theoretical effort, using Feynman’s idea of a quantum simulator, to devise schemes for simulating such theories on engineered quantum-mechanical devices, with the difficulty that gauge invariance and the associated local conservation laws (Gauss laws) need to be implemented. Here we report the experimental demonstration of a digital quantum simulation of a lattice gauge theory, by realizing (1 + 1)-dimensional quantum electrodynamics (the Schwinger model) on a few-qubit trapped-ion quantum computer. We are interested in the real-time evolution of the Schwinger mechanism, describing the instability of the bare vacuum due to quantum fluctuations, which manifests itself in the spontaneous creation of electron-positron pairs. To make efficient use of our quantum resources, we map the original problem to a spin model by eliminating the gauge fields in favour of exotic long-range interactions, which can be directly and efficiently implemented on an ion trap architecture. We explore the Schwinger mechanism of particle-antiparticle generation by monitoring the mass production and the vacuum persistence amplitude. Moreover, we track the real-time evolution of entanglement in the system, which illustrates how particle creation and entanglement generation are directly related. Our work represents a first step towards quantum simulation of high-energy theories using atomic physics experiments—the long-term intention is to extend this approach to real-time quantum simulations of non-Abelian lattice gauge theories.

Generating free charges by carrier multiplication in quantum dots for highly efficient photovoltaics.

PubMed

Ten Cate, Sybren; Sandeep, C S Suchand; Liu, Yao; Law, Matt; Kinge, Sachin; Houtepen, Arjan J; Schins, Juleon M; Siebbeles, Laurens D A

2015-02-17

CONSPECTUS: In a conventional photovoltaic device (solar cell or photodiode) photons are absorbed in a bulk semiconductor layer, leading to excitation of an electron from a valence band to a conduction band. Directly after photoexcitation, the hole in the valence band and the electron in the conduction band have excess energy given by the difference between the photon energy and the semiconductor band gap. In a bulk semiconductor, the initially hot charges rapidly lose their excess energy as heat. This heat loss is the main reason that the theoretical efficiency of a conventional solar cell is limited to the Shockley-Queisser limit of ∼33%. The efficiency of a photovoltaic device can be increased if the excess energy is utilized to excite additional electrons across the band gap. A sufficiently hot charge can produce an electron-hole pair by Coulomb scattering on a valence electron. This process of carrier multiplication (CM) leads to formation of two or more electron-hole pairs for the absorption of one photon. In bulk semiconductors such as silicon, the energetic threshold for CM is too high to be of practical use. However, CM in nanometer sized semiconductor quantum dots (QDs) offers prospects for exploitation in photovoltaics. CM leads to formation of two or more electron-hole pairs that are initially in close proximity. For photovoltaic applications, these charges must escape from recombination. This Account outlines our recent progress in the generation of free mobile charges that result from CM in QDs. Studies of charge carrier photogeneration and mobility were carried out using (ultrafast) time-resolved laser techniques with optical or ac conductivity detection. We found that charges can be extracted from photoexcited PbS QDs by bringing them into contact with organic electron and hole accepting materials. However, charge localization on the QD produces a strong Coulomb attraction to its counter charge in the organic material. This limits the production of free charges that can contribute to the photocurrent in a device. We show that free mobile charges can be efficiently produced via CM in solids of strongly coupled PbSe QDs. Strong electronic coupling between the QDs resulted in a charge carrier mobility of the order of 1 cm(2) V(-1) s(-1). This mobility is sufficiently high so that virtually all electron-hole pairs escape from recombination. The impact of temperature on the CM efficiency in PbSe QD solids was also studied. We inferred that temperature has no observable effect on the rate of cooling of hot charges nor on the CM rate. We conclude that exploitation of CM requires that charges have sufficiently high mobility to escape from recombination. The contribution of CM to the efficiency of photovoltaic devices can be further enhanced by an increase of the CM efficiency above the energetic threshold of twice the band gap. For large-scale applications in photovoltaic devices, it is important to develop abundant and nontoxic materials that exhibit efficient CM.

Suppressed power saturation due to optimized optical confinement in 9xx nm high-power diode lasers that use extreme double asymmetric vertical designs

NASA Astrophysics Data System (ADS)

Kaul, T.; Erbert, G.; Maaßdorf, A.; Knigge, S.; Crump, P.

2018-03-01

Broad area lasers with novel extreme double asymmetric structure (EDAS) vertical designs featuring increased optical confinement in the quantum well, Γ, are shown to have improved temperature stability without compromising series resistance, internal efficiency or losses. Specifically, we present here vertical design considerations for the improved continuous wave (CW) performance of devices operating at 940 nm, based on systematically increasing Γ from 0.26% to 1.1%, and discuss the impact on power saturation mechanisms. The results indicate that key power saturation mechanisms at high temperatures originate in high threshold carrier densities, which arise in the quantum well at low Γ. The characteristic temperatures, T 0 and T 1, are determined under short pulse conditions and are used to clarify the thermal contribution to power limiting mechanisms. Although increased Γ reduces thermal power saturation, it is accompanied by increased optical absorption losses in the active region, which has a significant impact on the differential external quantum efficiency, {η }{{diff}}. To quantify the impact of internal optical losses contributed by the quantum well, a resonator length-dependent simulation of {η }{{diff}} is performed and compared to the experiment, which also allows the estimation of experimental values for the light absorption cross sections of electrons and holes inside the quantum well. Overall, the analysis enables vertical designs to be developed, for devices with maximized power conversion efficiency at high CW optical power and high temperatures, in a trade-off between absorption in the well and power saturation. The best balance to date is achieved in devices using EDAS designs with {{Γ }}=0.54 % , which deliver efficiencies of 50% at 14 W optical output power at an elevated junction temperature of 105 °C.

Broadband near-infrared downconversion luminescence in Yb3+-doped BaZn2(BO3)2

NASA Astrophysics Data System (ADS)

Yu, Hua; Deng, Degang; Su, Weitao; Li, Chenxia; Xu, Shiqing

2018-06-01

BaZn2(BO3)2 self-activated phosphors were prepared by the conventional high temperature solid-state method. The PL spectra of BaZn2(BO3)2 powders prepared under reductive and air atmosphere consist of a weak ultraviolet emission band (∼410 nm) and a broad emission band which were centered at ∼ 500 and 545 nm, respectively. According to the spectral analysis and EPR results, the green and yellow emissions may arise from the transitions of photo-generated electron close to the conduction band to the deeply trapped hole in single ionized oxygen vacancy (V+ o) centers and single negatively charged interstitial oxygen ion (O- i), respectively. An efficient broadband near-infrared (NIR) quantum cutting was demonstrated in Yb3+ doped BaZn2(BO3)2 phosphor. Upon excitation with an ultraviolet photon at 375 nm, the emissions of two NIR photons at 983 nm from Yb3+ ions were achieved. The dependences of the visible and NIR emissions, the decay lifetime, the energy transfer efficiency, and the quantum efficiency on the Yb3+ doping content were investigated in detail. The results indicated that the maximum energy transfer and the corresponding downconversion quantum efficiency could reach between 68.5% and 168.5%.

Structural, optical, electrochemical and photovoltaic studies of spider web like Silver Indium Diselenide Quantum dots synthesized by ligand mediated colloidal sol-gel approach

NASA Astrophysics Data System (ADS)

Adhikari, Tham; Pathak, Dinesh; Wagner, Tomas; Jambor, Roman; Jabeen, Uzma; Aamir, Muhammad; Nunzi, Jean-Michel

2017-11-01

Silver indium diselenide quantum dots were successively synthesized by colloidal sol-gel method by chelating with organic ligand oleylamine (OLA). The particle size was studied by transmission electron microscopy (TEM) and the size was found about 10 nm. X-ray diffraction (XRD) was used to study crystalline structure of the nanocrystals. The grain size and morphology were further studied by scanning electron microscopy (SEM) and atomic force microscopy (AFM). The elemental composition was studied by X-ray photon electron spectroscopy (XPS) and energy dispersive x-ray spectroscopy (EDAX). The capping property of OLA in nanocrystal was also demonstrated by Fourier Transform Infrared spectroscopy (FTIR). The band gap was calculated from both cyclic voltammetry and optical absorption and suggest quantum confinement. The solution processed bilayer thin film solar cells were fabricated with n-type Zinc oxide using doctor blading/spin coating method and their photovoltaic performance was studied. The best device sintered at 450 °C showed an efficiency 0.75% with current density of 4.54 mAcm-2, open-circuit voltage 0.44 V and fill factor 39.4%.

Quantum Dot Surface Engineering: Toward Inert Fluorophores with Compact Size and Bright, Stable Emission

PubMed Central

Lim, Sung Jun; Ma, Liang; Schleife, André; Smith, Andrew M.

2016-01-01

The surfaces of colloidal nanocrystals are complex interfaces between solid crystals, coordinating ligands, and liquid solutions. For fluorescent quantum dots, the properties of the surface vastly influence the efficiency of light emission, stability, and physical interactions, and thus determine their sensitivity and specificity when they are used to detect and image biological molecules. But after more than 30 years of study, the surfaces of quantum dots remain poorly understood and continue to be an important subject of both experimental and theoretical research. In this article, we review the physics and chemistry of quantum dot surfaces and describe approaches to engineer optimal fluorescent probes for applications in biomolecular imaging and sensing. We describe the structure and electronic properties of crystalline facets, the chemistry of ligand coordination, and the impact of ligands on optical properties. We further describe recent advances in compact coatings that have significantly improved their properties by providing small hydrodynamic size, high stability and fluorescence efficiency, and minimal nonspecific interactions with cells and biological molecules. While major progress has been made in both basic and applied research, many questions remain in the chemistry and physics of quantum dot surfaces that have hindered key breakthroughs to fully optimize their properties. PMID:28344357

Quantum mechanical force field for water with explicit electronic polarization.

PubMed

Han, Jaebeom; Mazack, Michael J M; Zhang, Peng; Truhlar, Donald G; Gao, Jiali

2013-08-07

A quantum mechanical force field (QMFF) for water is described. Unlike traditional approaches that use quantum mechanical results and experimental data to parameterize empirical potential energy functions, the present QMFF uses a quantum mechanical framework to represent intramolecular and intermolecular interactions in an entire condensed-phase system. In particular, the internal energy terms used in molecular mechanics are replaced by a quantum mechanical formalism that naturally includes electronic polarization due to intermolecular interactions and its effects on the force constants of the intramolecular force field. As a quantum mechanical force field, both intermolecular interactions and the Hamiltonian describing the individual molecular fragments can be parameterized to strive for accuracy and computational efficiency. In this work, we introduce a polarizable molecular orbital model Hamiltonian for water and for oxygen- and hydrogen-containing compounds, whereas the electrostatic potential responsible for intermolecular interactions in the liquid and in solution is modeled by a three-point charge representation that realistically reproduces the total molecular dipole moment and the local hybridization contributions. The present QMFF for water, which is called the XP3P (explicit polarization with three-point-charge potential) model, is suitable for modeling both gas-phase clusters and liquid water. The paper demonstrates the performance of the XP3P model for water and proton clusters and the properties of the pure liquid from about 900 × 10(6) self-consistent-field calculations on a periodic system consisting of 267 water molecules. The unusual dipole derivative behavior of water, which is incorrectly modeled in molecular mechanics, is naturally reproduced as a result of an electronic structural treatment of chemical bonding by XP3P. We anticipate that the XP3P model will be useful for studying proton transport in solution and solid phases as well as across biological ion channels through membranes.

Using quantum dynamics simulations to follow the competition between charge migration and charge transfer in polyatomic molecules

NASA Astrophysics Data System (ADS)

Spinlove, K. E.; Vacher, M.; Bearpark, M.; Robb, M. A.; Worth, G. A.

2017-01-01

Recent work, particularly by Cederbaum and co-workers, has identified the phenomenon of charge migration, whereby charge flow occurs over a static molecular framework after the creation of an electronic wavepacket. In a real molecule, this charge migration competes with charge transfer, whereby the nuclear motion also results in the re-distribution of charge. To study this competition, quantum dynamics simulations need to be performed. To break the exponential scaling of standard grid-based algorithms, approximate methods need to be developed that are efficient yet able to follow the coupled electronic-nuclear motion of these systems. Using a simple model Hamiltonian based on the ionisation of the allene molecule, the performance of different methods based on Gaussian Wavepackets is demonstrated.

Control of electron spin and orbital resonances in quantum dots through spin-orbit interactions

NASA Astrophysics Data System (ADS)

Stano, Peter; Fabian, Jaroslav

2008-01-01

The influence of a resonant oscillating electromagnetic field on a single electron in coupled lateral quantum dots in the presence of phonon-induced relaxation and decoherence is investigated. Using symmetry arguments, it is shown that the spin and orbital resonances can be efficiently controlled by spin-orbit interactions. The control is possible due to the strong sensitivity of the Rabi frequency to the dot configuration (the orientation of the dot and the applied static magnetic field); the sensitivity is a result of the anisotropy of the spin-orbit interactions. The so-called easy passage configuration is shown to be particularly suitable for a magnetic manipulation of spin qubits, ensuring long spin relaxation times and protecting the spin qubits from electric field disturbances accompanying on-chip manipulations.

Atomistic mechanisms of rapid energy transport in light-harvesting molecules

NASA Astrophysics Data System (ADS)

Ohmura, Satoshi; Koga, Shiro; Akai, Ichiro; Shimojo, Fuyuki; Kalia, Rajiv K.; Nakano, Aiichiro; Vashishta, Priya

2011-03-01

Synthetic supermolecules such as π-conjugated light-harvesting dendrimers efficiently harvest energy from sunlight, which is of significant importance for the global energy problem. Key to their success is rapid transport of electronic excitation energy from peripheral antennas to photochemical reaction cores, the atomistic mechanisms of which remains elusive. Here, quantum-mechanical molecular dynamics simulation incorporating nonadiabatic electronic transitions reveals the key molecular motion that significantly accelerates the energy transport based on the Dexter mechanism.

Surface Traps in Colloidal Quantum Dots: A Combined Experimental and Theoretical Perspective.

PubMed

Giansante, Carlo; Infante, Ivan

2017-10-19

Surface traps are ubiquitous to nanoscopic semiconductor materials. Understanding their atomistic origin and manipulating them chemically have capital importance to design defect-free colloidal quantum dots and make a leap forward in the development of efficient optoelectronic devices. Recent advances in computing power established computational chemistry as a powerful tool to describe accurately complex chemical species and nowadays it became conceivable to model colloidal quantum dots with realistic sizes and shapes. In this Perspective, we combine the knowledge gathered in recent experimental findings with the computation of quantum dot electronic structures. We analyze three different systems: namely, CdSe, PbS, and CsPbI 3 as benchmark semiconductor nanocrystals showing how different types of trap states can form at their surface. In addition, we suggest experimental healing of such traps according to their chemical origin and nanocrystal composition.

Experimental observation of spatial quantum noise reduction below the standard quantum limit with bright twin beams of light

NASA Astrophysics Data System (ADS)

Kumar, Ashok; Nunley, Hayden; Marino, Alberto

2016-05-01

Quantum noise reduction (QNR) below the standard quantum limit (SQL) has been a subject of interest for the past two to three decades due to its wide range of applications in quantum metrology and quantum information processing. To date, most of the attention has focused on the study of QNR in the temporal domain. However, many areas in quantum optics, specifically in quantum imaging, could benefit from QNR not only in the temporal domain but also in the spatial domain. With the use of a high quantum efficiency electron multiplier charge coupled device (EMCCD) camera, we have observed spatial QNR below the SQL in bright narrowband twin light beams generated through a four-wave mixing (FWM) process in hot rubidium atoms. Owing to momentum conservation in this process, the twin beams are momentum correlated. This leads to spatial quantum correlations and spatial QNR. Our preliminary results show a spatial QNR of over 2 dB with respect to the SQL. Unlike previous results on spatial QNR with faint and broadband photon pairs from parametric down conversion (PDC), we demonstrate spatial QNR with spectrally and spatially narrowband bright light beams. The results obtained will be useful for atom light interaction based quantum protocols and quantum imaging. Work supported by the W.M. Keck Foundation.

Enhancing the performance of blue GaN-based light emitting diodes with double electron blocking layers

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

Guo, Yao; Liang, Meng; Fu, Jiajia

2015-03-15

In this work, novel double Electron Blocking Layers for InGaN/GaN multiple quantum wells light-emitting diodes were proposed to mitigate the efficiency droop at high current density. The band diagram and carriers distributions were investigated numerically. The results indicate that due to a newly formed holes stack in the p-GaN near the active region, the hole injection has been improved and an uniform carriers distribution can be achieved. As a result, in our new structure with double Electron Blocking Layers, the efficiency droop has been reduced to 15.5 % in comparison with 57.3 % for the LED with AlGaN EBL atmore » the current density of 100 A/cm{sup 2}.« less

Thickness dependent thermoelectric properties of SrTiO3/SrLaTiO3 and SrZrO3/SrLaTiO3 heterostructures

NASA Astrophysics Data System (ADS)

Ishii, Masatoshi; Baniecki, John; Schafranek, Robert; Kerman, Kian; Kurihara, Kazuaki

2013-03-01

Thermoelectric power generators will be required for future sensor network systems. SrTiO3 (STO) is one candidate thermoelectric material due to its non-toxicity and comparable power factor to Bismuth telluride. The energy conversion efficiency of SrTiO3-based thermoelectric energy conversion elements has been reported to be enhanced by quantum size effects, such as the two dimensional (2D) electron gas in SrTiO3/SrTi0.8Nb0.2O3/SrTiO3. Nevertheless, a complete understanding of the mechanisms for the reported increase in efficiency are missing owing to a lack of understanding of the thickness dependence of the transport properties. In the talk, we will present a study of the thickness dependence of the transport properties of SrTiO3/SrLaTiO3 and SrZrO3/SrLaTiO3 heterostructures. The SrZrO3/SrLaTiO3 interface has a large conduction band off-set of 1.9 eV which can be utilized to confine electrons in a 2D quantum well. Characterization of the thermopower, conductivity, and Hall effect will be presented as a function of the SrLaTiO3 thickness down to a few unit cells and the implications of the thickness dependence of the transport properties on carrier confinement and increasing the efficiency STO-based 2DEG quantum well structures will be discussed.

Detailed Modeling of Physical Processes in Electron Sources for Accelerator Applications

NASA Astrophysics Data System (ADS)

Chubenko, Oksana; Afanasev, Andrei

2017-01-01

At present, electron sources are essential in a wide range of applications - from common technical use to exploring the nature of matter. Depending on the application requirements, different methods and materials are used to generate electrons. State-of-the-art accelerator applications set a number of often-conflicting requirements for electron sources (e.g., quantum efficiency vs. polarization, current density vs. lifetime, etc). Development of advanced electron sources includes modeling and design of cathodes, material growth, fabrication of cathodes, and cathode testing. The detailed simulation and modeling of physical processes is required in order to shed light on the exact mechanisms of electron emission and to develop new-generation electron sources with optimized efficiency. The purpose of the present work is to study physical processes in advanced electron sources and develop scientific tools, which could be used to predict electron emission from novel nano-structured materials. In particular, the area of interest includes bulk/superlattice gallium arsenide (bulk/SL GaAs) photo-emitters and nitrogen-incorporated ultrananocrystalline diamond ((N)UNCD) photo/field-emitters. Work supported by The George Washington University and Euclid TechLabs LLC.

Polymer Solar Cells with 90% External Quantum Efficiency Featuring an Ideal Light- and Charge-Manipulation Layer.

PubMed

Chen, Jing-De; Li, Yan-Qing; Zhu, Jingshuai; Zhang, Qianqian; Xu, Rui-Peng; Li, Chi; Zhang, Yue-Xing; Huang, Jing-Sheng; Zhan, Xiaowei; You, Wei; Tang, Jian-Xin

2018-03-01

Rapid progress in the power conversion efficiency (PCE) of polymer solar cells (PSEs) is beneficial from the factors that match the irradiated solar spectrum, maximize incident light absorption, and reduce photogenerated charge recombination. To optimize the device efficiency, a nanopatterned ZnO:Al 2 O 3 composite film is presented as an efficient light- and charge-manipulation layer (LCML). The Al 2 O 3 shells on the ZnO nanoparticles offer the passivation effect that allows optimal electron collection by suppressing charge-recombination loss. Both the increased refractive index and the patterned deterministic aperiodic nanostructure in the ZnO:Al 2 O 3 LCML cause broadband light harvesting. Highly efficient single-junction PSCs for different binary blends are obtained with a peak external quantum efficiency of up to 90%, showing certified PCEs of 9.69% and 13.03% for a fullerene blend of PTB7:PC 71 BM and a nonfullerene blend, FTAZ:IDIC, respectively. Because of the substantial increase in efficiency, this method unlocks the full potential of the ZnO:Al 2 O 3 LCML toward future photovoltaic applications. © 2018 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Fabrication of a Combustion-Reacted High-Performance ZnO Electron Transport Layer with Silver Nanowire Electrodes for Organic Solar Cells.

PubMed

Park, Minkyu; Lee, Sang-Hoon; Kim, Donghyuk; Kang, Juhoon; Lee, Jung-Yong; Han, Seung Min

2018-02-28

Herein, a new methodology for solution-processed ZnO fabrication on Ag nanowire network electrode via combustion reaction is reported, where the amount of heat emitted during combustion was minimized by controlling the reaction temperature to avoid damaging the underlying Ag nanowires. The degree of participation of acetylacetones, which are volatile fuels in the combustion reaction, was found to vary with the reaction temperature, as revealed by thermogravimetric and compositional analyses. An optimized processing temperature of 180 °C was chosen to successfully fabricate a combustion-reacted ZnO and Ag nanowire hybrid electrode with a sheet resistance of 30 Ω/sq and transmittance of 87%. A combustion-reacted ZnO on Ag nanowire hybrid structure was demonstrated as an efficient transparent electrode and electron transport layer for the PTB7-Th-based polymer solar cells. The superior electrical conductivity of combustion-reacted ZnO, compared to that of conventional sol-gel ZnO, increased the external quantum efficiency over the entire absorption range, whereas a unique light scattering effect due to the presence of nanopores in the combustion-derived ZnO further enhanced the external quantum efficiency in the 450-550 nm wavelength range. A power conversion efficiency of 8.48% was demonstrated for the PTB7-Th-based polymer solar cell with the use of a combustion-reacted ZnO/Ag NW hybrid transparent electrode.

Universal non-adiabatic geometric manipulation of pseudo-spin charge qubits

NASA Astrophysics Data System (ADS)

Azimi Mousolou, Vahid

2017-01-01

Reliable quantum information processing requires high-fidelity universal manipulation of quantum systems within the characteristic coherence times. Non-adiabatic holonomic quantum computation offers a promising approach to implement fast, universal, and robust quantum logic gates particularly useful in nano-fabricated solid-state architectures, which typically have short coherence times. Here, we propose an experimentally feasible scheme to realize high-speed universal geometric quantum gates in nano-engineered pseudo-spin charge qubits. We use a system of three coupled quantum dots containing a single electron, where two computational states of a double quantum dot charge qubit interact through an intermediate quantum dot. The additional degree of freedom introduced into the qubit makes it possible to create a geometric model system, which allows robust and efficient single-qubit rotations through careful control of the inter-dot tunneling parameters. We demonstrate that a capacitive coupling between two charge qubits permits a family of non-adiabatic holonomic controlled two-qubit entangling gates, and thus provides a promising procedure to maintain entanglement in charge qubits and a pathway toward fault-tolerant universal quantum computation. We estimate the feasibility of the proposed structure by analyzing the gate fidelities to some extent.

Observation of entanglement between a quantum dot spin and a single photon.

PubMed

Gao, W B; Fallahi, P; Togan, E; Miguel-Sanchez, J; Imamoglu, A

2012-11-15

Entanglement has a central role in fundamental tests of quantum mechanics as well as in the burgeoning field of quantum information processing. Particularly in the context of quantum networks and communication, a main challenge is the efficient generation of entanglement between stationary (spin) and propagating (photon) quantum bits. Here we report the observation of quantum entanglement between a semiconductor quantum dot spin and the colour of a propagating optical photon. The demonstration of entanglement relies on the use of fast, single-photon detection, which allows us to project the photon into a superposition of red and blue frequency components. Our results extend the previous demonstrations of single-spin/single-photon entanglement in trapped ions, neutral atoms and nitrogen-vacancy centres to the domain of artificial atoms in semiconductor nanostructures that allow for on-chip integration of electronic and photonic elements. As a result of its fast optical transitions and favourable selection rules, the scheme we implement could in principle generate nearly deterministic entangled spin-photon pairs at a rate determined ultimately by the high spontaneous emission rate. Our observation constitutes a first step towards implementation of a quantum network with nodes consisting of semiconductor spin quantum bits.

Nonadiabatic Molecular Dynamics and Orthogonality Constrained Density Functional Theory

NASA Astrophysics Data System (ADS)

Shushkov, Philip Georgiev

The exact quantum dynamics of realistic, multidimensional systems remains a formidable computational challenge. In many chemical processes, however, quantum effects such as tunneling, zero-point energy quantization, and nonadiabatic transitions play an important role. Therefore, approximate approaches that improve on the classical mechanical framework are of special practical interest. We propose a novel ring polymer surface hopping method for the calculation of chemical rate constants. The method blends two approaches, namely ring polymer molecular dynamics that accounts for tunneling and zero-point energy quantization, and surface hopping that incorporates nonadiabatic transitions. We test the method against exact quantum mechanical calculations for a one-dimensional, two-state model system. The method reproduces quite accurately the tunneling contribution to the rate and the distribution of reactants between the electronic states for this model system. Semiclassical instanton theory, an approach related to ring polymer molecular dynamics, accounts for tunneling by the use of periodic classical trajectories on the inverted potential energy surface. We study a model of electron transfer in solution, a chemical process where nonadiabatic events are prominent. By representing the tunneling electron with a ring polymer, we derive Marcus theory of electron transfer from semiclassical instanton theory after a careful analysis of the tunneling mode. We demonstrate that semiclassical instanton theory can recover the limit of Fermi's Golden Rule rate in a low-temperature, deep-tunneling regime. Mixed quantum-classical dynamics treats a few important degrees of freedom quantum mechanically, while classical mechanics describes affordably the rest of the system. But the interface of quantum and classical description is a challenging theoretical problem, especially for low-energy chemical processes. We therefore focus on the semiclassical limit of the coupled nuclear-electronic dynamics. We show that the time-dependent Schrodinger equation for the electrons employed in the widely used fewest switches surface hopping method is applicable only in the limit of nearly identical classical trajectories on the different potential energy surfaces. We propose a short-time decoupling algorithm that restricts the use of the Schrodinger equation only to the interaction regions. We test the short-time approximation on three model systems against exact quantum-mechanical calculations. The approximation improves the performance of the surface hopping approach. Nonadiabatic molecular dynamics simulations require the efficient and accurate computation of ground and excited state potential energy surfaces. Unlike the ground state calculations where standard methods exist, the computation of excited state properties is a challenging task. We employ time-independent density functional theory, in which the excited state energy is represented as a functional of the total density. We suggest an adiabatic-like approximation that simplifies the excited state exchange-correlation functional. We also derive a set of minimal conditions to impose exactly the orthogonality of the excited state Kohn-Sham determinant to the ground state determinant. This leads to an efficient, variational algorithm for the self-consistent optimization of the excited state energy. Finally, we assess the quality of the excitation energies obtained by the new method on a set of 28 organic molecules. The new approach provides results of similar accuracy to time-dependent density functional theory.

Bio-Photoelectrochemical Solar Cells Incorporating Reaction Center and Reaction Center Plus Light Harvesting Complexes

NASA Astrophysics Data System (ADS)

Yaghoubi, Houman

Harvesting solar energy can potentially be a promising solution to the energy crisis now and in the future. However, material and processing costs continue to be the most important limitations for the commercial devices. A key solution to these problems might lie within the development of bio-hybrid solar cells that seeks to mimic photosynthesis to harvest solar energy and to take advantage of the low material costs, negative carbon footprint, and material abundance. The bio-photoelectrochemical cell technologies exploit biomimetic means of energy conversion by utilizing plant-derived photosystems which can be inexpensive and ultimately the most sustainable alternative. Plants and photosynthetic bacteria harvest light, through special proteins called reaction centers (RCs), with high efficiency and convert it into electrochemical energy. In theory, photosynthetic RCs can be used in a device to harvest solar energy and generate 1.1 V open circuit voltage and ~1 mA cm-2 short circuit photocurrent. Considering the nearly perfect quantum yield of photo-induced charge separation, efficiency of a protein-based solar cell might exceed 20%. In practice, the efficiency of fabricated devices has been limited mainly due to the challenges in the electron transfer between the protein complex and the device electrodes as well as limited light absorption. The overarching goal of this work is to increase the power conversion efficiency in protein-based solar cells by addressing those issues (i.e. electron transfer and light absorption). This work presents several approaches to increase the charge transfer rate between the photosynthetic RC and underlying electrode as well as increasing the light absorption to eventually enhance the external quantum efficiency (EQE) of bio-hybrid solar cells. The first approach is to decrease the electron transfer distance between one of the redox active sites in the RC and the underlying electrode by direct attachment of the of protein complex onto Au electrodes via surface exposed cysteine residues. This resulted in photocurrent densities as large as ~600 nA cm-2 while still the incident photon to generated electron quantum efficiency was as low as %3 x 10-4. 2- The second approach is to immobilize wild type RCs of Rhodobacter sphaeroides on the surface of a Au underlying electrode using self-assembled monolayers of carboxylic acid terminated oligomers and cytochrome c charge mediating layers, with a preferential orientation from the primary electron donor site. This approach resulted in EQE of up to 0.06%, which showed 200 times efficiency improvement comparing to the first approach. In the third approach, instead of isolated protein complexes, RCs plus light harvesting (LH) complexes were employed for a better photon absorption. Direct attachment of RC-LH1 complexes on Au working electrodes, resulted in 0.21% EQE which showed 3.5 times efficiency improvement over the second approach (700 times higher than the first approach). The main impact of this work is the harnessing of biological RCs for efficient energy harvesting in man-made structures. Specifically, the results in this work will advance the application of RCs in devices for energy harvesting and will enable a better understanding of bio and nanomaterial interfaces, thereby advancing the application of biological materials in electronic devices. At the end, this work offers general guidelines that can serve to improve the performance of bio-hybrid solar cells.

Deterministic quantum teleportation with feed-forward in a solid state system.

PubMed

Steffen, L; Salathe, Y; Oppliger, M; Kurpiers, P; Baur, M; Lang, C; Eichler, C; Puebla-Hellmann, G; Fedorov, A; Wallraff, A

2013-08-15

Engineered macroscopic quantum systems based on superconducting electronic circuits are attractive for experimentally exploring diverse questions in quantum information science. At the current state of the art, quantum bits (qubits) are fabricated, initialized, controlled, read out and coupled to each other in simple circuits. This enables the realization of basic logic gates, the creation of complex entangled states and the demonstration of algorithms or error correction. Using different variants of low-noise parametric amplifiers, dispersive quantum non-demolition single-shot readout of single-qubit states with high fidelity has enabled continuous and discrete feedback control of single qubits. Here we realize full deterministic quantum teleportation with feed-forward in a chip-based superconducting circuit architecture. We use a set of two parametric amplifiers for both joint two-qubit and individual qubit single-shot readout, combined with flexible real-time digital electronics. Our device uses a crossed quantum bus technology that allows us to create complex networks with arbitrary connecting topology in a planar architecture. The deterministic teleportation process succeeds with order unit probability for any input state, as we prepare maximally entangled two-qubit states as a resource and distinguish all Bell states in a single two-qubit measurement with high efficiency and high fidelity. We teleport quantum states between two macroscopic systems separated by 6 mm at a rate of 10(4) s(-1), exceeding other reported implementations. The low transmission loss of superconducting waveguides is likely to enable the range of this and other schemes to be extended to significantly larger distances, enabling tests of non-locality and the realization of elements for quantum communication at microwave frequencies. The demonstrated feed-forward may also find application in error correction schemes.

Study on negative incident photon-to-electron conversion efficiency of quantum dot-sensitized solar cells

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

Li, Chunhui; Wu, Huijue; Zhu, Lifeng

2014-02-15

Recently, negative signals are frequently observed during the measuring process of monochromatic incident photon-to-electron conversion efficiency (IPCE) for sensitized solar cells by DC method. This phenomenon is confusing and hindering the reasonable evaluation of solar cells. Here, cause of negative IPCE values is studied by taking quantum dot-sensitized solar cell (QDSC) as an example, and the accurate measurement method to avoid the negative value is suggested. The negative background signals of QDSC without illumination are found the direct cause of the negative IPCE values by DC method. Ambient noise, significant capacitance characteristics, and uncontrolled electrochemical reaction all can lead tomore » the negative background signals. When the photocurrent response of device under monochromatic light illumination is relatively weak, the actual photocurrent signals will be covered by the negative background signals and the resulting IPCE values will appear negative. To improve the signal-to-noise ratio, quasi-AC method is proposed for IPCE measurement of solar cells with weak photocurrent response based on the idea of replacing the absolute values by the relative values.« less

Dynamical photo-induced electronic properties of molecular junctions

NASA Astrophysics Data System (ADS)

Beltako, K.; Michelini, F.; Cavassilas, N.; Raymond, L.

2018-03-01

Nanoscale molecular-electronic devices and machines are emerging as promising functional elements, naturally flexible and efficient, for next-generation technologies. A deeper understanding of carrier dynamics in molecular junctions is expected to benefit many fields of nanoelectronics and power devices. We determine time-resolved charge current flowing at the donor-acceptor interface in molecular junctions connected to metallic electrodes by means of quantum transport simulations. The current is induced by the interaction of the donor with a Gaussian-shape femtosecond laser pulse. Effects of the molecular internal coupling, metal-molecule tunneling, and light-donor coupling on photocurrent are discussed. We then define the time-resolved local density of states which is proposed as an efficient tool to describe the absorbing molecule in contact with metallic electrodes. Non-equilibrium reorganization of hybridized molecular orbitals through the light-donor interaction gives rise to two phenomena: the dynamical Rabi shift and the appearance of Floquet-like states. Such insights into the dynamical photoelectronic structure of molecules are of strong interest for ultrafast spectroscopy and open avenues toward the possibility of analyzing and controlling the internal properties of quantum nanodevices with pump-push photocurrent spectroscopy.

Luminescent ZnO quantum dots as an efficient sensor for free chlorine detection in water.

PubMed

Singh, Kulvinder; Mehta, S K

2016-04-21

Highly luminescent ZnO quantum dots (QDs) synthesized via a simple and facile route are used for the preparation of an optical sensor for the detection of free chlorine. The concentration of free chlorine greatly affects the PL emission of the ZnO QDs at 525 nm. Since hypochlorite gains electrons with high efficiency, it takes electrons from the oxygen vacancies of ZnO QDs, which gives rise to defect emission in ZnO QDs. UV-vis data analysis shows that free chlorine does not affect the optical absorption spectra of ZnO QDs. The optical sensing of free chlorine using ZnO QDs has several advantages, like quick response time, good selectivity and of course high sensitivity. The pH has very little effect on the PL emission of ZnO QDs. It does not interfere in the sensing mechanism for free chlorine. After 60 s, the response of the ZnO QDs remains stable. The present sensor shows high selectivity with respect to various common cations, as well as anions.

Nanostructured organosilicon luminophores and their application in highly efficient plastic scintillators

NASA Astrophysics Data System (ADS)

Ponomarenko, Sergei A.; Surin, Nikolay M.; Borshchev, Oleg V.; Luponosov, Yuriy N.; Akimov, Dmitry Y.; Alexandrov, Ivan S.; Burenkov, Alexander A.; Kovalenko, Alexey G.; Stekhanov, Viktor N.; Kleymyuk, Elena A.; Gritsenko, Oleg T.; Cherkaev, Georgiy V.; Kechek'yan, Alexander S.; Serenko, Olga A.; Muzafarov, Aziz M.

2014-10-01

Organic luminophores are widely used in various optoelectronic devices, which serve for photonics, nuclear and particle physics, quantum electronics, medical diagnostics and many other fields of science and technology. Improving their spectral-luminescent characteristics for particular technical requirements of the devices is a challenging task. Here we show a new concept to universal solution of this problem by creation of nanostructured organosilicon luminophores (NOLs), which are a particular type of dendritic molecular antennas. They combine the best properties of organic luminophores and inorganic quantum dots: high absorption cross-section, excellent photoluminescence quantum yield, fast luminescence decay time and good processability. A NOL consists of two types of covalently bonded via silicon atoms organic luminophores with efficient Förster energy transfer between them. Using NOLs in plastic scintillators, widely utilized for radiation detection and in elementary particles discoveries, led to a breakthrough in their efficiency, which combines both high light output and fast decay time. Moreover, for the first time plastic scintillators, which emit light in the desired wavelength region ranging from 370 to 700 nm, have been created. We anticipate further applications of NOLs as working elements of pulsed dye lasers in photonics, optoelectronics and as fluorescent labels in biology and medical diagnostics.

Quaternary Cu2ZnSnS4 quantum dot-sensitized solar cells: Synthesis, passivation and ligand exchange

NASA Astrophysics Data System (ADS)

Bai, Bing; Kou, Dongxing; Zhou, Wenhui; Zhou, Zhengji; Tian, Qingwen; Meng, Yuena; Wu, Sixin

2016-06-01

The quaternary Cu2ZnSnS4 (CZTS) QDs had been successfully introduced into quantum dot-sensitized solar cells (QDSC) via hydrolysis approach in our previous work [Green Chem. 2015, vol. 17, p. 4377], but the obtained cell efficiency was still limited by low open-circuit voltage and fill factor. Herein, we use 1-dodecanethiol (DDT) as capping ligand for fairly small-sized CZTS QDs synthesis to improve their intrinsic properties. Since this strong bonded capping ligand can not be replaced by 3-mercaptopropionic acid (MPA) directly, the nature cation (Cu, Zn or Sn)-DDT units of QDs are first exchanged by the preconjugated Cd-oleate via successive ionic layer adsorption and reaction (SILAR) procedure accompanied with the formation of a core/shell structure. The weak bonded oleic acid (OA) can be finally replaced by MPA and the constructed water soluble CZTS/CdSe QDSC achieves an impressive conversion efficiency of 4.70%. The electron transport and recombination dynamic processes are confirmed by intensity-modulated photocurrent spectroscopy (IMPS)/intensity-modulated photovoltage spectroscopy (IMVS) measurements. It is found that the removal of long alkyl chain is conducive to improve the electron transport process and the type-II core/shell structure is beneficial to accelerate electron transport and retard charge recombination. This effective ligand removal strategy is proved to be more convenient for the applying of quaternary QDs in QDSC and would boost a more powerful efficiency in the future work.

Dynamics and mechanism of UV-damaged DNA repair in indole-thymine dimer adduct: molecular origin of low repair quantum efficiency.

PubMed

Guo, Xunmin; Liu, Zheyun; Song, Qinhua; Wang, Lijuan; Zhong, Dongping

2015-02-26

Many biomimetic chemical systems for repair of UV-damaged DNA showed very low repair efficiency, and the molecular origin is still unknown. Here, we report our systematic characterization of the repair dynamics of a model compound of indole-thymine dimer adduct in three solvents with different polarity. By resolving all elementary steps including three electron-transfer processes and two bond-breaking and bond-formation dynamics with femtosecond resolution, we observed the slow electron injection in 580 ps in water, 4 ns in acetonitrile, and 1.38 ns in dioxane, the fast back electron transfer without repair in 120, 150, and 180 ps, and the slow bond splitting in 550 ps, 1.9 ns, and 4.5 ns, respectively. The dimer bond cleavage is clearly accelerated by the solvent polarity. By comparing with the biological repair machine photolyase with a slow back electron transfer (2.4 ns) and a fast bond cleavage (90 ps), the low repair efficiency in the biomimetic system is mainly determined by the fast back electron transfer and slow bond breakage. We also found that the model system exists in a dynamic heterogeneous C-clamped conformation, leading to a stretched dynamic behavior. In water, we even identified another stacked form with ultrafast cyclic electron transfer, significantly reducing the repair efficiency. Thus, the comparison of the repair efficiency in different solvents is complicated and should be cautious, and only the dynamics by resolving all elementary steps can finally determine the total repair efficiency. Finally, we use the Marcus electron-transfer theory to analyze all electron-transfer reactions and rationalize all observed electron-transfer dynamics.

Efficient and accurate treatment of electron correlations with correlation matrix renormalization theory

DOE PAGES

Yao, Y. X.; Liu, J.; Liu, C.; ...

2015-08-28

We present an efficient method for calculating the electronic structure and total energy of strongly correlated electron systems. The method extends the traditional Gutzwiller approximation for one-particle operators to the evaluation of the expectation values of two particle operators in the many-electron Hamiltonian. The method is free of adjustable Coulomb parameters, and has no double counting issues in the calculation of total energy, and has the correct atomic limit. We demonstrate that the method describes well the bonding and dissociation behaviors of the hydrogen and nitrogen clusters, as well as the ammonia composed of hydrogen and nitrogen atoms. We alsomore » show that the method can satisfactorily tackle great challenging problems faced by the density functional theory recently discussed in the literature. The computational workload of our method is similar to the Hartree-Fock approach while the results are comparable to high-level quantum chemistry calculations.« less

Three-dimensional imaging for precise structural control of Si quantum dot networks for all-Si solar cells

NASA Astrophysics Data System (ADS)

Kourkoutis, Lena F.; Hao, Xiaojing; Huang, Shujuan; Puthen-Veettil, Binesh; Conibeer, Gavin; Green, Martin A.; Perez-Wurfl, Ivan

2013-07-01

All-Si tandem solar cells based on Si quantum dots (QDs) are a promising approach to future high-performance, thin film solar cells using abundant, stable and non-toxic materials. An important prerequisite to achieve a high conversion efficiency in such cells is the ability to control the geometry of the Si QD network. This includes the ability to control both, the size and arrangement of Si QDs embedded in a higher bandgap matrix. Using plasmon tomography we show the size, shape and density of Si QDs, that form in Si rich oxide (SRO)/SiO2 multilayers upon annealing, can be controlled by varying the SRO stoichiometry. Smaller, more spherical QDs of higher densities are obtained at lower Si concentrations. In richer SRO layers ellipsoidal QDs tend to form. Using electronic structure calculations within the effective mass approximation we show that ellipsoidal QDs give rise to reduced inter-QD coupling in the layer. Efficient carrier transport via mini-bands is in this case more likely across the multilayers provided the SiO2 spacer layer is thin enough to allow coupling in the vertical direction.All-Si tandem solar cells based on Si quantum dots (QDs) are a promising approach to future high-performance, thin film solar cells using abundant, stable and non-toxic materials. An important prerequisite to achieve a high conversion efficiency in such cells is the ability to control the geometry of the Si QD network. This includes the ability to control both, the size and arrangement of Si QDs embedded in a higher bandgap matrix. Using plasmon tomography we show the size, shape and density of Si QDs, that form in Si rich oxide (SRO)/SiO2 multilayers upon annealing, can be controlled by varying the SRO stoichiometry. Smaller, more spherical QDs of higher densities are obtained at lower Si concentrations. In richer SRO layers ellipsoidal QDs tend to form. Using electronic structure calculations within the effective mass approximation we show that ellipsoidal QDs give rise to reduced inter-QD coupling in the layer. Efficient carrier transport via mini-bands is in this case more likely across the multilayers provided the SiO2 spacer layer is thin enough to allow coupling in the vertical direction. Electronic supplementary information (ESI) available: Electron tomography reconstruction movies. See DOI: 10.1039/c3nr01998e

A divide-conquer-recombine algorithmic paradigm for large spatiotemporal quantum molecular dynamics simulations

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

Shimojo, Fuyuki; Hattori, Shinnosuke; Department of Physics, Kumamoto University, Kumamoto 860-8555

We introduce an extension of the divide-and-conquer (DC) algorithmic paradigm called divide-conquer-recombine (DCR) to perform large quantum molecular dynamics (QMD) simulations on massively parallel supercomputers, in which interatomic forces are computed quantum mechanically in the framework of density functional theory (DFT). In DCR, the DC phase constructs globally informed, overlapping local-domain solutions, which in the recombine phase are synthesized into a global solution encompassing large spatiotemporal scales. For the DC phase, we design a lean divide-and-conquer (LDC) DFT algorithm, which significantly reduces the prefactor of the O(N) computational cost for N electrons by applying a density-adaptive boundary condition at themore » peripheries of the DC domains. Our globally scalable and locally efficient solver is based on a hybrid real-reciprocal space approach that combines: (1) a highly scalable real-space multigrid to represent the global charge density; and (2) a numerically efficient plane-wave basis for local electronic wave functions and charge density within each domain. Hybrid space-band decomposition is used to implement the LDC-DFT algorithm on parallel computers. A benchmark test on an IBM Blue Gene/Q computer exhibits an isogranular parallel efficiency of 0.984 on 786 432 cores for a 50.3 × 10{sup 6}-atom SiC system. As a test of production runs, LDC-DFT-based QMD simulation involving 16 661 atoms is performed on the Blue Gene/Q to study on-demand production of hydrogen gas from water using LiAl alloy particles. As an example of the recombine phase, LDC-DFT electronic structures are used as a basis set to describe global photoexcitation dynamics with nonadiabatic QMD (NAQMD) and kinetic Monte Carlo (KMC) methods. The NAQMD simulations are based on the linear response time-dependent density functional theory to describe electronic excited states and a surface-hopping approach to describe transitions between the excited states. A series of techniques are employed for efficiently calculating the long-range exact exchange correction and excited-state forces. The NAQMD trajectories are analyzed to extract the rates of various excitonic processes, which are then used in KMC simulation to study the dynamics of the global exciton flow network. This has allowed the study of large-scale photoexcitation dynamics in 6400-atom amorphous molecular solid, reaching the experimental time scales.« less

Thermoelectric effect in an Aharonov-Bohm ring with an embedded quantum dot

PubMed Central

2012-01-01

Thermoelectric effect is studied in an Aharonov-Bohm interferometer with an embedded quantum dot (QD) in the Coulomb blockade regime. The electrical conductance, electron thermal conductance, thermopower, and thermoelectric figure-of-merit are calculated by using the Keldysh Green's function method. It is found that the figure-of-merit ZT of the QD ring may be quite high due to the Fano effect originated from the quantum interference effect. Moreover, the thermoelectric efficiency is sensitive to the magnitude of the dot-lead and inter-lead coupling strengthes. The effect of intradot Coulomb repulsion on ZT is significant in the weak-coupling regime, and then large ZT values can be obtained at rather high temperature. PMID:22369454

Photocurrent spectrum study of a quantum dot single-photon detector based on resonant tunneling effect with near-infrared response

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

Weng, Q. C.; Key Laboratory of Polar Materials and Devices, Ministry of Education, East China Normal University, Shanghai 200241; An, Z. H., E-mail: anzhenghua@fudan.edu.cn, E-mail: luwei@mail.sitp.ac.cn

We present the photocurrent spectrum study of a quantum dot (QD) single-photon detector using a reset technique which eliminates the QD's “memory effect.” By applying a proper reset frequency and keeping the detector in linear-response region, the detector's responses to different monochromatic light are resolved which reflects different detection efficiencies. We find the reset photocurrent tails up to 1.3 μm wavelength and near-infrared (∼1100 nm) single-photon sensitivity is demonstrated due to interband transition of electrons in QDs, indicating the device a promising candidate both in quantum information applications and highly sensitive imaging applications operating in relative high temperatures (>80 K).

Suppression of Zeeman gradients by nuclear polarization in double quantum dots.

PubMed

Frolov, S M; Danon, J; Nadj-Perge, S; Zuo, K; van Tilburg, J W W; Pribiag, V S; van den Berg, J W G; Bakkers, E P A M; Kouwenhoven, L P

2012-12-07

We use electric dipole spin resonance to measure dynamic nuclear polarization in InAs nanowire quantum dots. The resonance shifts in frequency when the system transitions between metastable high and low current states, indicating the presence of nuclear polarization. We propose that the low and the high current states correspond to different total Zeeman energy gradients between the two quantum dots. In the low current state, dynamic nuclear polarization efficiently compensates the Zeeman gradient due to the g-factor mismatch, resulting in a suppressed total Zeeman gradient. We present a theoretical model of electron-nuclear feedback that demonstrates a fixed point in nuclear polarization for nearly equal Zeeman splittings in the two dots and predicts a narrowed hyperfine gradient distribution.

Electron Tunneling, a Quantum Probe for the Quantum World of Nanotechnology

ERIC Educational Resources Information Center

Hipps, K. W.; Scudiero, L.

2005-01-01

A quantum-mechanical probe is essential to study the quantum world, which is provided by electron tunneling. A spectroscopic mapping to image the electron-transport pathways on a sub-molecular scale is used.

SINIS bolometer with a suspended absorber

NASA Astrophysics Data System (ADS)

Tarasov, M.; Edelman, V.; Mahashabde, S.; Fominsky, M.; Lemzyakov, S.; Chekushkin, A.; Yusupov, R.; Winkler, D.; Yurgens, A.

2018-03-01

We have developed a Superconductor-Insulator-Normal Metal-Insulator-Superconductor (SINIS) bolometer with a suspended normal metal bridge. The suspended bridge acts as a bolometric absorber with reduced heat losses to the substrate. Such bolometers were characterized at 100-350 mK bath temperatures and electrical responsivity of over 109 V/W was measured by dc heating the absorber through additional contacts. Suspended bolometers were also integrated in planar twin-slot and log-periodic antennas for operation in the submillimetre-band of radiation. The measured voltage response to radiation at 300 GHz and at 100 mK bath temperature is 3*108 V/W and a current response is 1.1*104 A/W which corresponds to a quantum efficiency of ~15 electrons per photon. An important feature of such suspended bolometers is the thermalization of electrons in the absorber heated by optical radiation, which in turn provides better quantum efficiency. This has been confirmed by comparison of bolometric response to dc and rf heating. We investigate the performance of direct SN traps and NIS traps with a tunnel barrier between the superconductor and normal metal trap. Increasing the volume of superconducting electrode helps to reduce overheating of superconductor. Influence of Andreev reflection and Kapitza resistance, as well as electron-phonon heat conductivity and thermal conductivity of N-wiring are estimated for such SINIS devices.

Optically programmable electron spin memory using semiconductor quantum dots.

PubMed

Kroutvar, Miro; Ducommun, Yann; Heiss, Dominik; Bichler, Max; Schuh, Dieter; Abstreiter, Gerhard; Finley, Jonathan J

2004-11-04

The spin of a single electron subject to a static magnetic field provides a natural two-level system that is suitable for use as a quantum bit, the fundamental logical unit in a quantum computer. Semiconductor quantum dots fabricated by strain driven self-assembly are particularly attractive for the realization of spin quantum bits, as they can be controllably positioned, electronically coupled and embedded into active devices. It has been predicted that the atomic-like electronic structure of such quantum dots suppresses coupling of the spin to the solid-state quantum dot environment, thus protecting the 'spin' quantum information against decoherence. Here we demonstrate a single electron spin memory device in which the electron spin can be programmed by frequency selective optical excitation. We use the device to prepare single electron spins in semiconductor quantum dots with a well defined orientation, and directly measure the intrinsic spin flip time and its dependence on magnetic field. A very long spin lifetime is obtained, with a lower limit of about 20 milliseconds at a magnetic field of 4 tesla and at 1 kelvin.

Intermolecular interaction approach for TADF (Conference Presentation)

NASA Astrophysics Data System (ADS)

Wong, Ken-Tsung

2016-09-01

Materials with thermally activated delayed fluorescence (TADF) have recently emerged as new fluorescent emitters for highly efficient organic light-emitting diodes (OLEDs). Molecule with TADF behavior needs to have a small singlet-triplet energy difference (ΔES-T) that allows the up-conversion from nonradiative triplet state (T1) to radiative singlet state (S1) via reverse intersystem crossing (RISC) process. Generally, molecules with small ΔES-T can be obtained via carefully manipulate the degree of "intramolecular" charge transfer (ICT) between electron-donating and -accepting components, such that the electron exchange energy that contributes to ΔES-T, can be minimized. Alternatively, excited state with small ΔES-T can be feasibly realized via "intermolecular" charge transfer occurring at the interface between spatially separating donor (D) and acceptor (A) molecules. Because the exchange energy decreases as the HOMO-LUMO separation distance increases, theoretically, the intermolecular D/A charge transfer state (or exciplex) should have rather small ΔES-T, leading to efficient TADF. However, it is still a challenge to access highly efficient exciplex systems. This is mainly because exciplex formation is commonly accompanied with a large red shift of emission spectra and long radiative lifetime, which tend to diminish photoluminescence quantum yield (PLQY) as well as electroluminescence (EL) performance. Until now, exciplex-based OLEDs with external quantum efficiency (EQE) above 10% are still limited. By judicious selection of donor and acceptor, the formation of efficient exciplex can be feasibly achieved. In this conference, our recent efforts on highly efficient exciplexes using C3-symmetry triazine acceptors and various donors, and their device characteristics will be presented.

Efficient Color-Stable Inverted White Organic Light-Emitting Diodes with Outcoupling-Enhanced ZnO Layer.

PubMed

Zhao, Xin-Dong; Li, Yan-Qing; Xiang, Heng-Yang; Zhang, Yi-Bo; Chen, Jing-De; Xu, Lu-Hai; Tang, Jian-Xin

2017-01-25

Inverted organic light-emitting diode (OLED) has attracted extensive attention due to the demand in active-matrix OLED display panels as its geometry enables the direct connection with n-channel transistor backplane on the substrate. One key challenge of high-performance inverted OLED is an efficient electron-injection layer with superior electrical and optical properties to match the indium tin oxide cathode on substrate. We here propose a synergistic electron-injection architecture using surface modification of ZnO layer to simultaneously promote electron injection into organic emitter and enhance out-coupling of waveguided light. An efficient inverted white OLED is realized by introducing the nanoimprinted aperiodic nanostructure of ZnO for broadband and angle-independent light out-coupling and inserting an n-type doped interlayer for energy level tuning and injection barrier lowering. As a result, the optimized inverted white OLEDs have an external quantum efficiency of 42.4% and a power efficiency of 85.4 lm W 1- , which are accompanied by the superiority of angular color stability over the visible wavelength range. Our results may inspire a promising approach to fabricate high-efficiency inverted OLEDs for large-scale display panels.

Physics of lateral triple quantum-dot molecules with controlled electron numbers.

PubMed

Hsieh, Chang-Yu; Shim, Yun-Pil; Korkusinski, Marek; Hawrylak, Pawel

2012-11-01

We review the recent progress in theory and experiments with lateral triple quantum dots with controlled electron numbers down to one electron in each dot. The theory covers electronic and spin properties as a function of topology, number of electrons, gate voltage and external magnetic field. The orbital Hund's rules and Nagaoka ferromagnetism, magnetic frustration and chirality, interplay of quantum interference and electron-electron interactions and geometrical phases are described and related to charging and transport spectroscopy. Fabrication techniques and recent experiments are covered, as well as potential applications of triple quantum-dot molecule in coherent control, spin manipulation and quantum computation.

Thermally activated delayed fluorescent phenothiazine–dibenzo[a,j]phenazine–phenothiazine triads exhibiting tricolor-changing mechanochromic luminescence† †Electronic supplementary information (ESI) available: Synthetic procedures, spectroscopic data, copies of NMR charts, physicochemical properties, and device fabrication and performances. CCDC 1452024. For ESI and crystallographic data in CIF or other electronic format see DOI: 10.1039/c6sc04863c Click here for additional data file. Click here for additional data file.

PubMed Central

Okazaki, Masato; Pander, Piotr; Higginbotham, Heather; Monkman, Andrew P.

2017-01-01

Novel U-shaped donor–acceptor–donor (D–A–D) π-conjugated multi-functional molecules comprising dibenzo[a,j]phenazine (DBPHZ) as an acceptor and phenothiazines (PTZ) as donors have been developed. Most importantly, the D–A–D compounds exhibit not only distinct tricolor-changeable mechanochromic luminescence (MCL) properties but also efficient thermally activated delayed fluorescence (TADF). Quantum chemical calculations, X-ray diffraction analysis, and systematic studies on the photophysical properties indicated that the “two-conformation-switchable” PTZ units play a highly important role in achieving multi-color-changing MCL. Time-resolved photophysical measurements revealed that the developed D–A–D compounds also exhibit efficient orange-TADF. Furthermore, organic light-emitting diode (OLED) devices fabricated with the new TADF emitters have achieved high external quantum efficiencies (EQEs) up to 16.8%, which significantly exceeds the theoretical maximum (∼5%) of conventional fluorescent emitters. PMID:28553504

Multiple Exciton Generation in Semiconductor Nanostructures: DFT-based Computation

NASA Astrophysics Data System (ADS)

Mihaylov, Deyan; Kryjevski, Andrei; Kilin, Dmitri; Kilina, Svetlana; Vogel, Dayton

Multiple exciton generation (MEG) in nm-sized H-passivated Si nanowires (NWs), and quasi 2D nanofilms depends strongly on the degree of the core structural disorder as shown by the perturbation theory calculations based on the DFT simulations. In perturbation theory, we work to the 2nd order in the electron-photon coupling and in the (approximate) RPA-screened Coulomb interaction. We also include the effect of excitons for which we solve Bethe-Salpeter Equation. To describe MEG we calculate exciton-to-biexciton as well as biexciton-to-exciton rates and quantum efficiency (QE). We consider 3D arrays of Si29H36 quantum dots, NWs, and quasi 2D silicon nanofilms, all with both crystalline and amorphous core structures. Efficient MEG with QE of 1.3 up to 1.8 at the photon energy of about 3Egap is predicted in these nanoparticles except for the crystalline NW and film where QE ~=1. MEG in the amorphous nanoparticles is enhanced by the electron localization due to structural disorder. The exciton effects significantly red-shift QE vs. photon energy curves. Nm-sized a-Si NWs and films are predicted to have effective MEG within the solar spectrum range. Also, we find efficient MEG in the chiral single-wall Carbon nanotubes and in a perovskite nanostructure.

Fundamental aspects of steady-state conversion of heat to work at the nanoscale

NASA Astrophysics Data System (ADS)

Benenti, Giuliano; Casati, Giulio; Saito, Keiji; Whitney, Robert S.

2017-06-01

In recent years, the study of heat to work conversion has been re-invigorated by nanotechnology. Steady-state devices do this conversion without any macroscopic moving parts, through steady-state flows of microscopic particles such as electrons, photons, phonons, etc. This review aims to introduce some of the theories used to describe these steady-state flows in a variety of mesoscopic or nanoscale systems. These theories are introduced in the context of idealized machines which convert heat into electrical power (heat-engines) or convert electrical power into a heat flow (refrigerators). In this sense, the machines could be categorized as thermoelectrics, although this should be understood to include photovoltaics when the heat source is the sun. As quantum mechanics is important for most such machines, they fall into the field of quantum thermodynamics. In many cases, the machines we consider have few degrees of freedom, however the reservoirs of heat and work that they interact with are assumed to be macroscopic. This review discusses different theories which can take into account different aspects of mesoscopic and nanoscale physics, such as coherent quantum transport, magnetic-field induced effects (including topological ones such as the quantum Hall effect), and single electron charging effects. It discusses the efficiency of thermoelectric conversion, and the thermoelectric figure of merit. More specifically, the theories presented are (i) linear response theory with or without magnetic fields, (ii) Landauer scattering theory in the linear response regime and far from equilibrium, (iii) Green-Kubo formula for strongly interacting systems within the linear response regime, (iv) rate equation analysis for small quantum machines with or without interaction effects, (v) stochastic thermodynamic for fluctuating small systems. In all cases, we place particular emphasis on the fundamental questions about the bounds on ideal machines. Can magnetic-fields change the bounds on power or efficiency? What is the relationship between quantum theories of transport and the laws of thermodynamics? Does quantum mechanics place fundamental bounds on heat to work conversion which are absent in the thermodynamics of classical systems?

Ultrafast electronic dynamics in unipolar n-doped indium gallium arsenide/gallium arsenide self-assembled quantum dots

NASA Astrophysics Data System (ADS)

Wu, Zong-Kwei J.

2006-12-01

Photodetectors based on intraband infrared absorption in the quantum dots have demonstrated improved performance over its quantum well counterpart by lower dark current, relative temperature insensitivity, and its ability for normal incidence operation. Various scattering processes, including phonon emission/absorption and carrier-carrier scattering, are critical in understanding device operation on the fundamental level. In previous studies, our group has investigated carrier dynamics in both low- and high-density regime. Ultrafast electron-hole scattering and the predicted phonon bottleneck effect in intrinsic quantum dots have been observed. Further examination on electron dynamics in unipolar structures is presented in this thesis. We used n-doped quantum dot in mid-infrared photodetector device structure to study the electron dynamics in unipolar structure. Differential transmission spectroscopy with mid-infrared intraband pump and optical interband probe was implemented to measure the electron dynamics directly without creating extra electron-hole pair, Electron relaxation after excitation was measured under various density and temperature conditions. Rapid capture into quantum dot within ˜ 10 ps was observed due to Auger-type electron-electron scattering. Intradot relaxation from the quantum dot excited state to the ground state was also observed on the time scale of 100 ps. With highly doped electron density in the structure, the inter-sublevel relaxation is dominated by Auger-type electron-electron scattering and the phonon bottleneck effect is circumvented. Nanosecond-scale recovery in larger-sized quantum dots was observed, not intrinsic to electron dynamics but due to band-bending and built-in voltage drift. An ensemble Monte Carlo simulation was also established to model the dynamics in quantum dots and in goad agreement with the experimental results. We presented a comprehensive picture of electron dynamics in the unipolar quantum dot structure. Although the phonon bottleneck is circumvented with high doped electron density, relaxation processes in unipolar quantum dots have been measured with time scales longer than that of bipolar systems. The results explain the operation principles of the quantum dot infrared photodetector on a microscopic level and provide basic understanding for future applications and designs.

Growth of high-quality InGaN/GaN LED structures on (1 1 1) Si substrates with internal quantum efficiency exceeding 50%

NASA Astrophysics Data System (ADS)

Lee, JaeWon; Tak, Youngjo; Kim, Jun-Youn; Hong, Hyun-Gi; Chae, Suhee; Min, Bokki; Jeong, Hyungsu; Yoo, Jinwoo; Kim, Jong-Ryeol; Park, Youngsoo

2011-01-01

GaN-based light-emitting-diodes (LEDs) on (1 1 1) Si substrates with internal quantum efficiency (IQE) exceeding 50% have been successfully grown by metal organic vapor phase epitaxy (MOVPE). 3.5 μm thick crack-free GaN epitaxial layers were grown on the Si substrates by the re-growth method on patterned templates. Series of step-graded Al xGa 1- xN epitaxial layers were used as the buffer layers to compensate thermal tensile stresses produced during the post-growth cooling process as well as to reduce the density of threading dislocations (TDs) generated due to the lattice mismatches between III-nitride layers and the silicon substrates. The light-emitting region consisted of 1.8 μm thick n-GaN, 3 periods of InGaN/GaN superlattice, InGaN/GaN multiple quantum wells (MQWs) designed for a peak wavelength of about 455 nm, an electron blocking layer (EBL), and p-GaN. The full-widths at half-maximum (FWHM) of (0 0 0 2) and (1 0 -1 2) ω-rocking curves of the GaN epitaxial layers were 410 and 560 arcsec, respectively. Cross-sectional transmission electron microscopy (TEM) investigation revealed that the propagation of the threading dislocations was mostly limited to the interface between the last Al xGa 1- xN buffer and n-GaN layers. The density of the threading dislocations induced pits of n-GaN, as estimated by atomic force microscopy (AFM), was about 5.5×10 8 cm -2. Temperature dependent photoluminescence (PL) measurements with a relative intensity integration method were carried out to estimate the internal quantum efficiency (IQE) of the light-emitting structures grown on Si, which reached up to 55%.

Intrachain versus interchain electron transport in poly(fluorene-alt-benzothiadiazole): a quantum-chemical insight.

PubMed

Van Vooren, Antoine; Kim, Ji-Seon; Cornil, Jérôme

2008-05-16

Poly(9,9-di-n-octylfluorene-alt-benzothiadiazole) [F8BT], displays very different charge-transport properties for holes versus electrons when comparing annealed and pristine thin films and transport parallel (intrachain) and perpendicular (interchain) to the polymer axes. The present theoretical contribution focuses on the electron-transport properties of F8BT chains and compares the efficiency of intrachain versus interchain transport in the hopping regime. The theoretical results rationalize significantly lowered electron mobility in annealed F8BT thin films and the smaller mobility anisotropy (mu( parallel)/mu( perpendicular)) measured for electrons in aligned films (i.e. 5-7 compared to 10-15 for holes).

Electronic Materials and Processing: Proceedings of the First Electronic Materials and Processing Congress Held in Conjunction with the 1988 World Materials Congress, Chicago, Illinois, USA, 24-30 September 1988

DTIC Science & Technology

1988-01-01

usually be traced to a combination of new semiconductors one on top of the other, then concepts, materials, and device principles, the process is called...example, growth techniques. New combinations of compound semiconductors such as GaAs have an materials called heterostructures can be made intrinsically...of combinations of metals, have direct energy band gaps that facilitate semiconductor, and insulators. Quantum the efficient recombination of

Protein's electronic polarization contributes significantly to its catalytic function

NASA Astrophysics Data System (ADS)

Xiang, Yun; Duan, Lili; Zhang, John Z. H.

2011-05-01

Ab initio quantum mechanical/molecular mechanical method is combined with the polarized protein-specific charge to study the chemical reactions catalyzed by protein enzymes. Significant improvement in the accuracy and efficiency of free-energy simulation is demonstrated by calculating the free-energy profile of the primary proton transfer reaction in triosephosphate isomerase. Quantitative agreement with experimental results is achieved. Our simulation results indicate that electronic polarization makes important contribution to enzyme catalysis by lowering the energy barrier by as much as 3 kcal/mol.

Feedback quantum control of molecular electronic population transfer

NASA Astrophysics Data System (ADS)

Bardeen, Christopher J.; Yakovlev, Vladislav V.; Wilson, Kent R.; Carpenter, Scott D.; Weber, Peter M.; Warren, Warren S.

1997-11-01

Feedback quantum control, where the sample `teaches' a computer-controlled arbitrary lightform generator to find the optimal light field, is experimentally demonstrated for a molecular system. Femtosecond pulses tailored by a computer-controlled acousto-optic pulse shaper excite fluorescence from laser dye molecules in solution. Fluorescence and laser power are monitored, and the computer uses the experimental data and a genetic algorithm to optimize population transfer from ground to first excited state. Both efficiency (the ratio of excited state population to laser energy) and effectiveness (total excited state population) are optimized. Potential use as an `automated theory tester' is discussed.

Quantum-dot light-emitting diodes utilizing CdSe /ZnS nanocrystals embedded in TiO2 thin film

NASA Astrophysics Data System (ADS)

Kang, Seung-Hee; Kumar, Ch. Kiran; Lee, Zonghoon; Kim, Kyung-Hyun; Huh, Chul; Kim, Eui-Tae

2008-11-01

Quantum-dot (QD) light-emitting diodes (LEDs) are demonstrated on Si wafers by embedding core-shell CdSe /ZnS nanocrystals in TiO2 thin films via plasma-enhanced metallorganic chemical vapor deposition. The n-TiO2/QDs /p-Si LED devices show typical p-n diode current-voltage and efficient electroluminescence characteristics, which are critically affected by the removal of QD surface ligands. The TiO2/QDs /Si system we presented can offer promising Si-based optoelectronic and electronic device applications utilizing numerous nanocrystals synthesized by colloidal solution chemistry.

Calculation of transmission probability by solving an eigenvalue problem

NASA Astrophysics Data System (ADS)

Bubin, Sergiy; Varga, Kálmán

2010-11-01

The electron transmission probability in nanodevices is calculated by solving an eigenvalue problem. The eigenvalues are the transmission probabilities and the number of nonzero eigenvalues is equal to the number of open quantum transmission eigenchannels. The number of open eigenchannels is typically a few dozen at most, thus the computational cost amounts to the calculation of a few outer eigenvalues of a complex Hermitian matrix (the transmission matrix). The method is implemented on a real space grid basis providing an alternative to localized atomic orbital based quantum transport calculations. Numerical examples are presented to illustrate the efficiency of the method.

Exciton Scattering approach for conjugated macromolecules: from electronic spectra to electron-phonon coupling

NASA Astrophysics Data System (ADS)

Tretiak, Sergei

2014-03-01

The exciton scattering (ES) technique is a multiscale approach developed for efficient calculations of excited-state electronic structure and optical spectra in low-dimensional conjugated macromolecules. Within the ES method, the electronic excitations in the molecular structure are attributed to standing waves representing quantum quasi-particles (excitons), which reside on the graph. The exciton propagation on the linear segments is characterized by the exciton dispersion, whereas the exciton scattering on the branching centers is determined by the energy-dependent scattering matrices. Using these ES energetic parameters, the excitation energies are then found by solving a set of generalized ``particle in a box'' problems on the graph that represents the molecule. All parameters can be extracted from quantum-chemical computations of small molecular fragments and tabulated in the ES library for further applications. Subsequently, spectroscopic modeling for any macrostructure within considered molecular family could be performed with negligible numerical effort. The exciton scattering properties of molecular vertices can be further described by tight-binding or equivalently lattice models. The on-site energies and hopping constants are obtained from the exciton dispersion and scattering matrices. Such tight-binding model approach is particularly useful to describe the exciton-phonon coupling, energetic disorder and incoherent energy transfer in large branched conjugated molecules. Overall the ES applications accurately reproduce the optical spectra compared to the reference quantum chemistry results, and make possible to predict spectra of complex macromolecules, where conventional electronic structure calculations are unfeasible.

Low intensity, continuous wave photodoping of ZnO quantum dots - photon energy and particle size effects.

PubMed

Aguirre, Matías E; Municoy, S; Grela, M A; Colussi, A J

2017-02-08

The unique properties of semiconductor quantum dots (QDs) have found application in the conversion of solar to chemical energy. How the relative rates of the redox processes that control QD photon efficiencies depend on the particle radius (r) and photon energy (E λ ), however, is not fully understood. Here, we address these issues and report the quantum yields (Φs) of interfacial charge transfer and electron doping in ZnO QDs capped with ethylene glycol (EG) as a function of r and E λ in the presence and absence of methyl viologen (MV 2+ ) as an electron acceptor, respectively. We found that Φs for the oxidation of EG are independent of E λ and photon fluence (φ λ ), but markedly increase with r. The independence of Φs on φ λ ensures that QDs are never populated by more than one electron-hole pair, thereby excluding Auger-type terminations. We show that these findings are consistent with the operation of an interfacial redox process that involves thermalized carriers in the Marcus inverted region. In the absence of MV 2+ , QDs accumulate electrons up to limiting volumetric densities ρ e,∞ that depend sigmoidally on excess photon energy E* = E λ - E BG (r), where E BG (r) is the r-dependent bandgap energy. The maximum electron densities: ρ ev,∞ ∼ 4 × 10 20 cm -3 , are reached at E* > 0.5 eV, independent of the particle radius.

Excited-state relaxation in PbSe quantum dots

NASA Astrophysics Data System (ADS)

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

2008-04-01

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

A tunable few electron triple quantum dot

NASA Astrophysics Data System (ADS)

Gaudreau, L.; Kam, A.; Granger, G.; Studenikin, S. A.; Zawadzki, P.; Sachrajda, A. S.

2009-11-01

In this paper, we report on a tunable few electron lateral triple quantum dot design. The quantum dot potentials are arranged in series. The device is aimed at studies of triple quantum dot properties where knowing the exact number of electrons is important as well as quantum information applications involving electron spin qubits. We demonstrate tuning strategies for achieving required resonant conditions such as quadruple points where all three quantum dots are on resonance. We find that in such a device resonant conditions at specific configurations are accompanied by complex charge transfer behavior.

Trap-assisted hole injection and quantum efficiency enhancement in poly(9,9' dioctylfluorene-alt-benzothiadiazole) polymer light-emitting diodes

NASA Astrophysics Data System (ADS)

Seeley, Alexander J. A. B.; Friend, Richard H.; Kim, Ji-Seon; Burroughes, Jeremy H.

2004-12-01

We report a reversible many-fold quantum efficiency enhancement during electrical driving of polymer light-emitting diodes (LEDs) containing poly(9,9' dioctylfluorene-alt-benzothiadiazole) (F8BT), developing over several minutes or hours at low applied bias and recovering on similar time scales after driving. This phenomenon is observed only in devices containing F8BT as an emissive layer in pure or blended form, regardless of anode and cathode choices and even in the absence of a poly(styrene-sulphonate)-doped poly(3,4-ethylene-dioxythiophene) (PEDOT:PSS) layer. We report detailed investigations using a standardized device structure containing PEDOT:PSS and a calcium cathode. Direct measurements of trapped charge recovered from the device after driving significantly exceed the unipolar limit, and thermally activated relaxation suggests a maximum trap depth around 0.6eV. Neither photoluminescence nor electroluminescence spectra reveal any change in the bulk optoelectronic properties of the emissive polymer nor any new emissive species. During the quantum efficiency (QE) enhancement process, the bulk conduction of the device increases. Reverse bias treatment of the device significantly reinforces the QE enhancement. Based on these observations, we propose a simple model in which interfacial dipoles are generated by trapped holes near the anode combining with injected electrons, to produce a narrow tunneling barrier for easy hole injection. The new injection pathway leads to a higher hole current density and thus a better charge injection balance. This produces the relatively high quantum efficiency observed in all F8BT LEDs.

Electronic and Optical Properties of Two-Dimensional GaN from First-Principles.

PubMed

Sanders, Nocona; Bayerl, Dylan; Shi, Guangsha; Mengle, Kelsey A; Kioupakis, Emmanouil

2017-12-13

Gallium nitride (GaN) is an important commercial semiconductor for solid-state lighting applications. Atomically thin GaN, a recently synthesized two-dimensional material, is of particular interest because the extreme quantum confinement enables additional control of its light-emitting properties. We performed first-principles calculations based on density functional and many-body perturbation theory to investigate the electronic, optical, and excitonic properties of monolayer and bilayer two-dimensional (2D) GaN as a function of strain. Our results demonstrate that light emission from monolayer 2D GaN is blueshifted into the deep ultraviolet range, which is promising for sterilization and water-purification applications. Light emission from bilayer 2D GaN occurs at a similar wavelength to its bulk counterpart due to the cancellation of the effect of quantum confinement on the optical gap by the quantum-confined Stark shift. Polarized light emission at room temperature is possible via uniaxial in-plane strain, which is desirable for energy-efficient display applications. We compare the electronic and optical properties of freestanding two-dimensional GaN to atomically thin GaN wells embedded within AlN barriers in order to understand how the functional properties are influenced by the presence of barriers. Our results provide microscopic understanding of the electronic and optical characteristics of GaN at the few-layer regime.

V-doped SnS2: a new intermediate band material for a better use of the solar spectrum.

PubMed

Wahnón, Perla; Conesa, José C; Palacios, Pablo; Lucena, Raquel; Aguilera, Irene; Seminovski, Yohanna; Fresno, Fernando

2011-12-07

Intermediate band materials can boost photovoltaic efficiency through an increase in photocurrent without photovoltage degradation thanks to the use of two sub-bandgap photons to achieve a full electronic transition from the valence band to the conduction band of a semiconductor structure. After having reported in previous works several transition metal-substituted semiconductors as able to achieve the electronic structure needed for this scheme, we propose at present carrying out this substitution in sulfides that have bandgaps of around 2.0 eV and containing octahedrally coordinated cations such as In or Sn. Specifically, the electronic structure of layered SnS(2) with Sn partially substituted by vanadium is examined here with first principles quantum methods and seen to give favourable characteristics in this respect. The synthesis of this material in nanocrystalline powder form is then undertaken and achieved using solvothermal chemical methods. The insertion of vanadium in SnS(2) is found to produce an absorption spectrum in the UV-Vis-NIR range that displays a new sub-bandgap feature in agreement with the quantum calculations. A photocatalytic reaction-based test verifies that this sub-bandgap absorption produces highly mobile electrons and holes in the material that may be used for the solar energy conversion, giving experimental support to the quantum calculations predictions.

Fundamental Challenges for Modeling Electrochemical Energy Storage Systems at the Atomic Scale.

PubMed

Groß, Axel

2018-04-23

There is a strong need to improve the efficiency of electrochemical energy storage, but progress is hampered by significant technological and scientific challenges. This review describes the potential contribution of atomic-scale modeling to the development of more efficient batteries, with a particular focus on first-principles electronic structure calculations. Numerical and theoretical obstacles are discussed, along with ways to overcome them, and some recent examples are presented illustrating the insights into electrochemical energy storage that can be gained from quantum chemical studies.

LASER APPLICATIONS AND OTHER TOPICS IN QUANTUM ELECTRONICS: Study of a volume discharge in inert-gas halides without preionisation

NASA Astrophysics Data System (ADS)

Erofeev, M. V.; Tarasenko, V. F.

2008-04-01

The energy characteristics of radiation of halides of inert gases excited by a volume discharge without additional preionisation are studied. The pressures of working mixtures and relations between the inert gas and halogen optimal for obtaining the maximum pulsed power and radiation efficiency are determined. The peak UV radiation power density achieved 5 kW cm-2 and the radiation efficiency was ≈5.5%. The pulse FWHM was 30—40 ns.

Adsorption characteristics of green 5-arylaminomethylene pyrimidine-2,4,6-triones on mild steel surface in acidic medium: Experimental and computational approach

NASA Astrophysics Data System (ADS)

Verma, Chandrabhan; Olasunkanmi, Lukman O.; Ebenso, Eno E.; Quraishi, M. A.

2018-03-01

The effect of electron withdrawing nitro (-NO2) and electron releasing hydroxyl (-OH) groups on corrosion inhibition potentials of 5-arylaminomethylenepyrimidine-2,4,6-trione (AMP) had been studied. Four AMPs tagged AMP-1, AMP-2, AMP-3 and AMP-4 were studied for their ability to inhibit mild steel corrosion in 1 M HCl using experimental and theoretical methods. Gravimetric results showed that inhibition efficiency of the studied inhibitors increases with increasing concentration. The results further revealed that that electron withdrawing nitro (-NO2) group decreases the inhibition efficiency of AMP, while electron donating hydroxyl (-OH) group increases the inhibition efficiency of AMP. SEM and AFM studies showed that the studied compounds inhibit mild steel corrosion by adsorbing at the metal/electrolyte interface and their adsorption obeyed the Temkin adsorption isotherm. Potentiodynamic polarization study revealed that studied inhibitors act as mixed type inhibitors with predominant effect on cathodic reaction. The inhibitive strength of the compounds might have direct relationship electron donating ability of the molecules as revealed by quantum chemical parameters. The order of interaction energies derived from Monte Carlo simulations is AMP-4 > AMP-3 > AMP-2 > AMP-1, which is in agreement with the order of inhibition efficiencies obtained from experimental measurements.

Investigating and Optimizing Carrier Transport, Carrier Distribution, and Efficiency Droop in GaN-based Light-emitting Diodes

NASA Astrophysics Data System (ADS)

Zhu, Di

2011-12-01

The recent tremendous boost in the number and diversity of applications for light-emitting diodes (LEDs) indicates the emergence of the next-generation lighting and illumination technology. The rapidly improving LED technology is becoming increasingly viable especially for high-power applications. However, the greatest roadblock before finally breaching the main defensive position of conventional fluorescent and incandescent lamps still remains: GaN-based LEDs encounter a significant decrease in efficiency as the drive current increases, and this phenomenon is known as the efficiency droop. This dissertation focuses on uncovering the physical cause of efficiency droop in GaN-based LEDs and looks for solutions to it. GaN-based multiple-quantum-well (MQW) LEDs usually have abnormally high diode-ideality factors. Investigating the origin of the high diode-ideality factors could help to better understand the carrier transport in the LED MQW active region. We investigate the ideality factors of GaInN LEDs with different numbers of doped quantum barriers (QBs). Consistent with the theory, a decrease of the ideality factor as well as a reduction in forward voltage is found with increasing number of doped QBs. Experimental and simulation results indicate that the band profiles of QBs in the active region have a significant impact on the carrier transport mechanism, and the unipolar heterojunctions inside the active region play an important role in determining the diode-ideality factor. This dissertation will discuss several mechanisms leading to electron leakage which could be responsible for the efficiency droop. We show that the inefficient electron capture, the electron-attracting properties of polarized EBL, the inherent asymmetry in electron and hole transport and the inefficient EBL p-doping at high Al contents severely limit the ability to confine electrons to the MQWs. We demonstrate GaInN LEDs employing tailored Si doping in the QBs with strongly enhanced high-current efficiency and reduced efficiency droop. Compared with 4-QB-doped LEDs, 1-QB-doped LEDs show a 37.5% increase in light-output power at high currents. Consistent with the measurements, simulation shows a shift of radiative recombination among the MQWs and a reduced electron leakage current into the p-type GaN when fewer QBs are doped. The results can be attributed to a more symmetric carrier transport and uniform carrier distribution which help to reduce electron leakage and thus reduce the efficiency droop. In this dissertation, artificial evolution is introduced to the LED optimization process which combines a genetic algorithm (GA) and device-simulation software. We show that this approach is capable of generating novel concepts in designing and optimizing LED devices. Application of the GA to the QB-doping in the MQWs yields optimized structures which is consistent with the tailored QB doping experiments. Application of the GA to the EBL region suggests a novel structure with an inverted sheet charge at the spacer-EBL interface. The resulting repulsion of electrons can significantly reduce electron leakage and enhance the efficiency. Finally, dual-wavelength LEDs, which have two types of quantum wells (QWs) emitting at two different wavelengths, are experimentally characterized and compared with numerical simulations. These dual-wavelength LEDs allow us to determine which QW emits most of the light. An experimental observation and a quantitative analysis of the radiative recombination shift within the MQW active region are obtained. In addition, an injection-current dependence of the radiative recombination shift is predicted by numerical simulations and indeed observed in dual-wavelength LEDs. This injection-current dependence of the radiative recombination distribution can be explained very well by incorporating quantum-mechanical tunneling of carriers into and through the QBs into to the classical drift-diffusion model. In summary, using the LEDs with tailored QB doping and dual-wavelength LEDs, we investigate the origin of the high diode-ideality factor of LEDs and gain insight on the control of carrier transport, carrier distribution, and radiative recombination in the LED MQW active region. Our results provide solid evidence on the effectiveness of the GA in the LED device optimization process. In addition, the innovative EBL structure optimized by the GA sheds light on further paths for the optimization of LED design. Our results are the starting point of applying artificial evolution to practical semiconductor devices, opening new perspectives for complex semiconductor device optimization and enabling breakthroughs in high-performance LED design.

Transport properties of a quantum dot and a quantum ring in series

NASA Astrophysics Data System (ADS)

Seo, Minky; Chung, Yunchul

2018-01-01

The decoherence mechanism of an electron interferometer is studied by using a serial quantum dot and ring device. By coupling a quantum dot to a quantum ring (closed-loop electron interferometer), we were able to observe both Coulomb oscillations and Aharonov-Bohm interference simultaneously. The coupled device behaves like an ordinary double quantum dot at zero magnetic field while the conductance of the Coulomb blockade peak is modulated by the electron interference at finite magnetic fields. By injecting one electron at a time (by exploiting the sequential tunneling of a quantum dot) into the interferometer, we were able to study the visibility of the electron interference at non-zero bias voltage. The visibility was found to decay rapidly as the electron energy was increased, which was consistent with the recently reported result for an electron interferometer. However, the lobe pattern and the sudden phase jump became less prominent. These results imply that the lobe pattern and the phase jump in an electron interferometer may be due to electron interactions inside the interferometer, as is predicted by the theory.