Number Of Excitons Research Articles

Coupled exciton-photon Bose condensate in path integral formalism

We study the behavior of exciton polaritons in an optical microcavity with an embedded semiconductor quantum well. We use two-component exciton-photon approach formulated in terms of path integral formalism. In order to describe spatial distributions of the exciton and photon condensate densities, the two coupled equations of the Gross-Pitaevskii type are derived. For a homogeneous system, we find the noncondensate photon and exciton spectra, calculate the coefficients of transformation from the exciton-photon basis to the lower-upper polariton basis, and obtain the exciton and photon occupation numbers of the lower and upper polariton branches for nonzero temperatures. For an inhomogeneous system, the set of coupled equations of the Bogoliubov-de-Gennes type is derived. The equations govern the spectra and spatial distributions of noncondensate photons and excitons.

Photo-reactive charge trapping memory based on lanthanide complex.

Traditional utilization of photo-induced excitons is popularly but restricted in the fields of photovoltaic devices as well as photodetectors, and efforts on broadening its function have always been attempted. However, rare reports are available on organic field effect transistor (OFET) memory employing photo-induced charges. Here, we demonstrate an OFET memory containing a novel organic lanthanide complex Eu(tta)3ppta (Eu(tta)3 = Europium(III) thenoyltrifluoroacetonate, ppta = 2-phenyl-4,6-bis(pyrazol-1-yl)-1,3,5-triazine), in which the photo-induced charges can be successfully trapped and detrapped. The luminescent complex emits intense red emission upon ultraviolet (UV) light excitation and serves as a trapping element of holes injected from the pentacene semiconductor layer. Memory window can be significantly enlarged by light-assisted programming and erasing procedures, during which the photo-induced excitons in the semiconductor layer are separated by voltage bias. The enhancement of memory window is attributed to the increasing number of photo-induced excitons by the UV light. The charges are stored in this luminescent complex for at least 104 s after withdrawing voltage bias. The present study on photo-assisted novel memory may motivate the research on a new type of light tunable charge trapping photo-reactive memory devices.

Multistate Blinking and Scaling of Recombination Rates in Individual Silica-Coated CdSe/CdS Nanocrystals

Nonradiative Auger recombination is the primary exciton loss mechanism in colloidal nanocrystals and an impediment for prospective optoelectronic applications. Recent development of new core/shell nanocrystals with suppressed Auger recombination rates has opened the possibility for studying multicarrier states using time-resolved photoluminescence (PL) spectroscopy. An important aspect not addressed in previous works is the scaling of radiative and nonradiative decay rates with the increasing number and type of excitons in individual nanocrystals. Here we conduct extensive single-dot PL spectroscopy of emissive states in PL blinking trajectories of giant silica-coated CdSe/CdS nanocrystals. At low fluences, we observe the appearance of neutral and charged exciton (trion) states. Both negative and positive trions show strongly suppressed Auger recombination rates resulting in PL quantum yields close to 50%. At higher excitation powers, we observe consecutive emergence of lower efficiency states, indicative...

Temperature effects on carrier formation dynamics in organic heterojunction solar cell

The femto-second time-resolved spectroscopy was performed on the heterojunction (HJ) solar cell which consists of prototypical low-band gap donor (D), poly[[4,8-bis[(2-ethylhexyl)oxy]benzo[1,2-b:4,5-b′] dithiophene-2,6-diyl][3-fluoro-2-[(2-ethylhexyl)carbonyl]thieno[3,4-b] thiophenediyl]] (PTB7), and the C70 acceptor (A). We spectroscopically determined the absolute number of donor exciton (nD*), acceptor exciton (nA*), and carrier (nD+) per an absorbed photon against the delay time (t). At 300 K, we found that the decay time (τdecay = 3.5 ps) of A* is much longer than the carrier formation time (τform = 1.1 ps), indicating that the late A* component does not contribute to the carrier formation process. The elongated τform (=1.5 ps) at 80 K is ascribed to the exciton migration process, not to the exciton dissociation process.

Enhanced multiple exciton generation in amorphous silicon nanowires and films

ABSTRACTMultiple exciton generation (MEG) in nanometer-sized hydrogen-passivated silicon nanowires (NWs), and quasi two-dimensional nanofilms depends strongly on the degree of the core structural disorder as shown by the perturbative many-body quantum mechanics calculations based on the density functional theory simulations. Working to the second order in the electron–photon coupling and in the screened Coulomb interaction, we calculate quantum efficiency (QE), the average number of excitons created by a single absorbed photon, in the Si29H36 quantum dots (QDs) with crystalline and amorphous core structures, simple cubic three-dimensional arrays constructed from these QDs, crystalline and amorphous NWs, and quasi two-dimensional silicon nanofilms, also both crystalline and amorphous. Efficient MEG with QE ranging from 1.3 up to 1.8 at the photon energy of about 3Eg, where Eg is the electronic gap, is predicted in these nanoparticles except for the crystalline NW and crystalline film where QE ≃ 1. MEG in the amorphous nanoparticles is enhanced by the electron localisation due to structural disorder. Combined with the lower gaps, the nanometer-sized amorphous silicon NWs and films are predicted to have effective carrier multiplication within the solar spectrum range.

Enhancement of light absorption by using light scattering and emitting dyes in organic photovoltaics

To enhance the power conversion efficiency of organic photovoltaics (OPVs), sufficient light absorption in the active layer is necessary to generate a greater number of excitons. We propose incorporating luminescent dyes into hole transport layer of OPVs as a route of enhancing light absorption, minimizing changes in the morphology and structure of the active layer; dyes scatter incoming collimated light isotropically, thereby increasing the distance light travels in the active layer, which leads to enhanced light absorption. In addition, dyes can absorb light in the portion of the spectrum where the active layer is transparent and re‐emit light in the portion of the spectrum corresponding to the absorption peak of the active layer. Coumarin 102 (C102) is a dye that has an absorption wavelength of 389 nm, which corresponds to the weakest absorption region of P3HT:PCBM blends. C102 is then able to isotropically re‐emit visible light, in the region that corresponds to the absorption spectrum of P3HT, into the active layer. Based on this effect, we demonstrate that the short circuit current density can be increased by 22.8% compared to the reference sample without any dye.

Measurement of scintillation and ionization yield and scintillation pulse shape from nuclear recoils in liquid argon

We have measured the scintillation and ionization yield of recoiling nuclei in liquid argon as a function of applied electric field by exposing a dual-phase liquid argon time projection chamber (LAr-TPC) to a low energy pulsed narrow band neutron beam produced at the Notre Dame Institute for Structure and Nuclear Astrophysics. Liquid scintillation counters were arranged to detect and identify neutrons scattered in the TPC and to select the energy of the recoiling nuclei. We report measurements of the scintillation yields for nuclear recoils with energies from 10.3 to 57.3 keV and for median applied electric fields from 0 to 970 V/cm. For the ionization yields, we report measurements from 16.9 to 57.3 keV and for electric fields from 96.4 to 486 V/cm. We also report the observation of an anticorrelation between scintillation and ionization from nuclear recoils, which is similar to the anticorrelation between scintillation and ionization from electron recoils. Assuming that the energy loss partitions into excitons and ion pairs from $^{83m}$Kr internal conversion electrons is comparable to that from $^{207}$Bi conversion electrons, we obtained the numbers of excitons ($N_{ex}$) and ion pairs ($N_i$) and their ratio ($N_{ex}/N_i$) produced by nuclear recoils from 16.9 to 57.3 keV. Motivated by arguments suggesting direction sensitivity in LAr-TPC signals due to columnar recombination, a comparison of the light and charge yield of recoils parallel and perpendicular to the applied electric field is presented for the first time.

Optimizing the fabrication process and interplay of device components of polymer solar cells using a field-based multiscale solar-cell algorithm.

Both the device composition and fabrication process are well-known to crucially affect the power conversion efficiency of polymer solar cells. Major advances have recently been achieved through the development of novel device materials and inkjet printing technologies, which permit to improve their durability and performance considerably. In this work, we demonstrate the usefulness of a recently developed field-based multiscale solar-cell algorithm to investigate the influence of the material characteristics, like, e.g., electrode surfaces, polymer architectures, and impurities in the active layer, as well as post-production treatments, like, e.g., electric field alignment, on the photovoltaic performance of block-copolymer solar-cell devices. Our study reveals that a short exposition time of the polymer bulk heterojunction to the action of an external electric field can lead to a low photovoltaic performance due to an incomplete alignment process, leading to undulated or disrupted nanophases. With increasing exposition time, the nanophases align in direction to the electric field lines, resulting in an increase of the number of continuous percolation paths and, ultimately, in a reduction of the number of exciton and charge-carrier losses. Moreover, we conclude by modifying the interaction strengths between the electrode surfaces and active layer components that a too low or too high affinity of an electrode surface to one of the components can lead to defective contacts, causing a deterioration of the device performance. Finally, we infer from the study of block-copolymer nanoparticle systems that particle impurities can significantly affect the nanostructure of the polymer matrix and reduce the photovoltaic performance of the active layer. For a critical volume fraction and size of the nanoparticles, we observe a complete phase transformation of the polymer nanomorphology, leading to a drop of the internal quantum efficiency. For other particle-numbers and -sizes, we observe only a local perturbation of the nanostructure, diminishing the number of continuous percolation paths to the electrodes and, therefore, reducing the device performance. From these investigations, we conclude that our multiscale solar-cell algorithm is an effective approach to investigate the impact of device materials and post-production treatments on the photovoltaic performance of polymer solar cells.

Ultrafast photoinduced dynamics in quantum dot-based systems for light harvesting

Colloidal semiconductor nanocrystals, referred to as quantum dots, offer simple low-temperature solution-based methods for constructing optoelectronic devices such as light emitting diodes and solar cells. We review recent progress in the understanding of photoinduced processes in key components of a certain type of quantum dot solar cells where the dots sensitize a suitable metal oxide, such as ZnO or TiO2, for electron injection, and NiO for hole injection. The electron and hole injection dynamics are discussed in detail as a function of the quantum dot size and core-shell structure, the linker molecule type, and the morphology of the accepting metal oxide. Hole trapping is identified as a major factor limiting the performance of quantum dot-based devices. We review possible strategies for improvement that use core-shell structures and directed excitation energy transfer between quantum dots. Finally, the generation and injection of multiple excitons are revisited. We show that the assumption of a linear relationship between the intensity of transient absorption signal and the number of excitons does not generally hold, and this observation can partially explain highly disparate results for the efficiency of generating multiple excitons. A consistent calculation procedure for studies of multiple exciton generation is provided. Finally, we offer a brief personal outlook on the topic.

Systematic investigation of effects of exciton–acoustic-phonon scattering on photoluminescence rise times of free excitons in GaAs/Al0.3Ga0.7As single quantum wells

We have systematically investigated the photoluminescence (PL) dynamics of free excitons in GaAs/Al0.3Ga0.7As single quantum wells, focusing on the energy relaxation process due to exciton–acoustic-phonon scattering under non-resonant and weak excitation conditions as a function of GaAs-layer thickness from 3.6 to 12.0 nm and temperature from 30 to 50 K. The free exciton characteristics were confirmed by observation that the PL decay time has a linear dependence with temperature. We found that the free exciton PL rise rate, which is the reciprocal of the rise time, is inversely linear with the GaAs-layer thickness and linear with temperature. This is consistent with a reported theoretical study of the exciton–acoustic-phonon scattering rate in the energy relaxation process in quantum wells. Consequently, it is conclusively verified that the PL rise rate is dominated by the exciton–acoustic-phonon scattering rate. In addition, from quantitative analysis of the GaAs-layer thickness and temperature dependences, we suggest that the PL rise rate reflects the number of exciton–acoustic-phonon scattering events.

Kinetic Monte Carlo study of triplet-triplet annihilation in organic phosphorescent emitters

The triplet-triplet annihilation (TTA) rate in organic phosphorescent materials such as used in organic light-emitting diodes is determined predominantly either by the rate of single-step Förster-type triplet-triplet interactions, or by multi-step triplet diffusion. We show how kinetic Monte Carlo simulations may be used to analyze the role of both processes. Under steady state conditions, the effective triplet-triplet interaction rate coefficient, kTT, which is often regarded as a constant, is found to depend actually on the number of excitons lost upon a triplet-triplet interaction process and to show a significant higher-order dependence on the triplet volume density. Under the conditions encountered in transient photoluminescence (PL) studies, kTT is found to be effectively constant in the case of diffusion-dominated TTA. However, for the case of single-step TTA, a strongly different decay of the emission intensity is found, which also deviates from an analytic expression proposed in the literature. We discuss how the transient PL response may be used to make a distinction between both mechanisms. The simulations are applied to recently published work on the dye concentration dependence of the TTA rate in materials based on the archetypal green emitter tris[2-phenylpyridine]iridium (Ir(ppy)3).

Releasing confined holes from type-II quantum dots by inelastic scattering with hot photoelectrons

We study a novel architecture for quantum dot (QD) solar cells. While all models and experiments on QD solar cells studied QDs located in the depletion region, we focused on the solar cell structure in which an electron-blocking barrier spatially separates type-II QD absorber from the depletion region. It is important that these QDs are still within the diffusion length from the depletion region. Inter-band QD absorption of the part of solar spectrum with the photon energy less than the energy band gap in the spacers generates a large number of localized excitons in type-II QDs solar cells. The energy of such photons is not utilized in conventional solar cells. However, the proposed architecture enables QD solar cells to benefit from additional photocurrent generated by disintegrating of localized excitons.Hereby we show that hot photoelectron collision with QDs facilitates exciton disintegration. One fifth of solar photons have energy exceeding GaAs bandgap by more than 0.5eV. They generate hot photoelectrons that usually relax by releasing the excess energy to optical phonons in 1ps time scale by multiple electron–phonon scattering. Our study has shown that collisions with QDs may compete with the scattering with optical phonons in GaSb/GaAs type-II QD absorber. The excess energy is transferred to confined holes. Such collisions enable confined holes to escape from QDs into mobile states in the valence band of absorber and dissociate excitons into mobile electrons and holes. Collection of these mobile carriers will increase both photocurrent and conversion efficiency limit of GaAs solar cells by estimated 50%, well above the Shockley–Queisser limit.

Three-pulse femtosecond spectroscopy of PbSe nanocrystals: 1S bleach nonlinearity and sub-band-edge excited-state absorption assignment.

Above band-edge photoexcitation of PbSe nanocrystals induces strong below band gap absorption as well as a multiphased buildup of bleaching in the 1Se1Sh transition. The amplitudes and kinetics of these features deviate from expectations based on biexciton shifts and state filling, which are the mechanisms usually evoked to explain them. To clarify these discrepancies, the same transitions are investigated here by double-pump-probe spectroscopy. Re-exciting in the below band gap induced absorption characteristic of hot excitons is shown to produce additional excitons with high probability. In addition, pump-probe experiments on a sample saturated with single relaxed excitons prove that the resulting 1Se1Sh bleach is not linear with the number of excitons per nanocrystal. This finding holds for two samples differing significantly in size, demonstrating its generality. Analysis of the results suggests that below band edge induced absorption in hot exciton states is due to excited-state absorption and not to shifted absorption of cold carriers and that 1Se1Sh bleach signals are not an accurate counter of sample excitons when their distribution includes multiexciton states.

Photoluminescence spectra of 1 MeV electron beam irradiated In0.53Ga0.47As/InP quantum well and bulk materials

Minimizing the impact of radiation-induced degradation on optoelectronic devices is important in several applications. Satellites and other spacecraft that fly in near-earth orbits (below 3.8 earth radius) are extremely susceptible to radiation damage caused by the high flux of electrons trapped in the earth’s magnetosphere. Optoelectronic devices are particularly vulnerable to displacement damage caused by electrons and protons. Effects of 1 MeV electron beam irradiation on the photoluminescence properties of In0.53Ga0.47As/InP quantum well (QW) and bulk structures, which are grown by metal-organic vapor phase epitaxy, are investigated. Samples are irradiated at room temperature using an ELV-8II accelerator with 1 MeV electron at doses ranging from 5×1012 to 9×1014 cm-2, and a dose rate of 1.075×1010 cm-2·s-1. Photoluminescence measurements are made using a 532 nm laser for excitation and a cooled Ge detector with lock-in techniques for signal detection. Photoluminescence intensity of all the structures is degraded after irradiation, and its reduction increases with increasing total dose of irradiation. Electron beam irradiation causes a larger reduction in the photoluminescence intensity and carrier lifetime of the bulk than that of quantum well. Photoluminescence intensity of five-layer quantum wells degenerates to 9% that before irradiation as the fluence reaches 6×1014 cm-2. As the electron beams bombard into the sample, the destruction of the lattice integrity will cause the decrease in the number of excitons and intensity of photoluminescence. Electron beam irradiation introduces defects in the samples, increases the density of the nonradiative recombination centers, and results in the decrease of carrier mobility. In a quantum well structure, due to the two-dimensional confinement, the probability of carrier nonradiative recombination at radiation-induced defect centers will be reduced. The reduction of photoluminescence intensity in the bulk is severer than in the quantum well while the cross-sectional area which is sensitive to radiation is kept the same. The number of interface defects which are produced by electron irradiation will increase with the number of layers in quantum well and the heterojunction interface of quantum wells, so is the degration of photoluminescence intensity. The degration is mainly due to the increase of non-radiative centers in the samples. By comparing the different structures, the quantum well structure shows a better radiation resistance.

Effect of exciton oscillator strength on upconversion photoluminescence in GaAs/AlAs multiple quantum wells

We report upconversion photoluminescence (UCPL) in GaAs/AlAs multiple quantum wells. UCPL from the AlAs barrier is caused by the resonant excitation of the excitons in the GaAs well. When the quantum well has sufficient miniband width, UCPL is hardly observed because of the small exciton oscillator strength. The excitation-energy and excitation-density dependences of UCPL intensity show the exciton resonant profile and a linear increase, respectively. These results demonstrate that the observed UCPL caused by the saturated two-step excitation process requires a large number of excitons.

Quantum correlations of quadratic optomechanical oscillator

The quantum optomechanical system serves as an interface for coupling between photons, excitons, and mechanical oscillations. We use the quantum Langevin approach to study a hybrid optomechanical system that contains a single undoped semiconductor quantum well in a cavity, where one of its mirrors is a thin dielectric membrane having quadratic response to the cavity fields. A decorrelation method is employed to solve for a large number of coupled equations. Transient mean numbers of cavity photons, moving membranes, and excitons that provide dynamical behavior are computed. We obtain the two-boson second-order correlation functions for the cavity field and the membrane oscillator, and their cross correlations that provide nonclassical quantum statistical properties and useful insights into the quadratic optomechanical system.

Electrodeposited polymer encapsulated nickel sulphide thin films: frequency switching material

Polyvinylpyrrolidone (PVP) encapsulated nickel sulfide (NiS) thin films have been synthesized electrochemically from aqueous solution of hydrated nickel chloride (NiCl2, 6H2O), thioacetamide (CH3C(S) NH2) (TAA) and polyvinylpyrrolidone (PVP). Surface modification of nickel sulfide (NiS) thin films was achieved by this polymer encapsulation. X-ray diffraction (XRD), high resolution transmission electron microscope (HRTEM), field emission scanning electron microscopy (FESEM) and Energy dispersive X-radiation (EDAX) techniques were used for the characterization of thin films. Infrared spectroscopy (IR) confirmed the formation of polymer encapsulated semiconductor. Frequency switching generation study shows that the encapsulated material could be used as a frequency switching device that generates a frequency ∼ 50Hz under 1 Sun illumination. Encapsulation with PVP causes surface modification that reduces the surface states and barrier height. As a result, the width of the depletion region decreases. So the number of electron-hole pairs increases. Consequently, the number of excitons and exciton related emission increases and this leads to reduction of recombination process and shows photo induced frequency switching phenomenon.

A comparison between experiment and theory on few-quantum-dot nanolasing in a photonic-crystal cavity

We present an experimental and theoretical study on the gain mechanism in a photonic-crystal-cavity nanolaser with embedded quantum dots. From time-resolved measurements at low excitation power we find that four excitons are coupled to the cavity. At high excitation power we observe a smooth low-threshold transition from spontaneous emission to lasing. Before lasing emission sets in, however, the excitons are observed to saturate, and the gain required for lasing originates rather from multi-excitonic transitions, which give rise to a broad emission background. We compare the experiment to a model of quantum-dot microcavity lasers and find that the number of excitons that must be included to fit the data largely exceeds the measured number, which shows that transitions involving the wetting layer can provide a surprisingly large contribution to the gain.

Simulation of ultraviolet- and soft X-ray-pulse generation as a result of cooperative recombination of excitons in diamond nanocrystals embedded in a polymer film

Using numerical simulation, it is shown that the recombination of free excitons photoexcited in diamond nanocrystals embedded in a polymer film can occur in the cooperative mode. It is found that this mode can be implemented despite the fact that diamond is an “indirect” semiconductor. It is shown that the power of the generated radiation at the pulse peak during the cooperative recombination of free excitons can exceed that of the incoherent spontaneous emission of the same initial number of free excitons by more than an order of magnitude. Finally, it is shown that the process under consideration can be used to generate picosecond pulses of ultraviolet and soft X-ray electromagnetic field at a wavelength of 235 nm.

New Insights into Bi2WO6 Properties as a Visible-Light Photocatalyst

Bismuth tungstate has attractive photocatalytic properties under visible light. A better understanding of the origin of that good activity should allow its control and its optimization. An improved photocatalytic activity to different pollutants was obtained using bismuth-based oxide obtained by microwave-assisted synthesis combined with the addition of sodium dodecylsulfate as a size tailoring agent. It is shown using electron paramagnetic resonance that bismuth tungstate is able to generate hydroxyl radicals in aqueous aerated solution, but no superoxide radical anions are formed. The catalytic efficiency relative to TiO2 could be associated to differences in the number of excitons generated, to their lifetimes as holes and electrons in the semiconductor, and to valence and conduction band positions.