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We explore the dynamics of energy transfer between two nanocrystal quantum dots placed within an optical microcavity. By adjusting the coupling strength between the cavity photon mode and the quantum dots, we have the capacity to fine-tune the effective coupling between the donor and acceptor. Introducing a non-adiabatic parameter, γ, governed by the coupling to the cavity mode, we demonstrate the system's capability to shift from the overdamped Förster regime (γ ≪ 1) to an underdamped coherent regime (γ ≫ 1). In the latter regime, characterized by swift energy transfer rates, the dynamics are influenced by decoherence time. To illustrate this, we study the exciton energy transfer dynamics between two closely positioned CdSe/CdS core/shell quantum dots with sizes and separations relevant to experimental conditions. Employing an atomistic approach, we calculate the excitonic level arrangement, exciton–phonon interactions, and transition dipole moments of the quantum dots within the microcavity. These parameters are then utilized to define a model Hamiltonian. Subsequently, we apply a generalized non-Markovian quantum Redfield equation to delineate the dynamics within the polaritonic framework. [ABSTRACT FROM AUTHOR]

Plasmonic catalysis holds the promise of opening new reaction pathways that are inaccessible thermally or via direct UV–vis electronic transitions. Here, energetic carriers produced via the decay of surface plasmons excited by visible light at 532 nm (2.33 eV, green) on a Ag-grating-bearing pyrolytic carbon residue drive its transformation into light-emitting graphitized carbon dots. The pyrolytic carbon residue is detectable via high-magnification surface-enhanced Raman scattering but cannot be directly observed using optical, electron, atomic force, or helium ion microscopy. When a Ag-grating-bearing pyrolyzed residue is introduced into a high-purity O2-depleted gas environment (Ar, N2, and CO2) and excited with 532 nm light, bright yellow luminescence emerges and is readily observed. Light emission is not observed without the pyrolytic carbon, without the excitation of plasmons, or in air or an Ar/O2 gas mixture. This process, driven by visible light and a nanostructured Ag surface bearing pyrolytic carbon, will be of interest to researchers involved in plasmonic catalysis, catalytic processes involving carbon, and luminescent plasmonic surfaces. [ABSTRACT FROM AUTHOR]

Room temperature 6 μm intraband cascade electroluminescence (EL) is demonstrated with lightly n-doped HgTe colloidal quantum dots of ∼8 nm diameter deposited on interdigitated electrodes in a metal–insulator–metal device. With quantum dot films of ∼150 nm thickness made by solid-state-ligand-exchange, the devices emit at 1600 cm−1 (6.25 μm), with a spectral width of 200 cm−1, determined by the overlap of the 1Se–1Pe intraband transition of the quantum dots and the substrate photonic resonance. At the maximum current used of 20 mA, the bias was 30 V, the external quantum efficiency was 2.7%, and the power conversion efficiency was 0.025%. Adding gold nano-antennas between the electrodes broadened the emission and increased the quantum efficiency to 4.4% and the power efficiency to 0.036%. For these films, the doping was about 0.1 electron/dot, the electron mobility was 0.02 cm2 V−1 s−1, and the maximum current density was 0.04 kA cm−2. Higher mobility films made by solution ligand exchange show a 20-fold increase in current density and a 10-fold decrease in EL efficiencies. Electroluminescence with weak doping is interesting for eventually achieving electrically driven stimulated emission, and the requirements for population inversion and lasing are discussed. [ABSTRACT FROM AUTHOR]

Scintillators are materials that convert ionizing radiation in the form of particles or photons into low-energy photons in the ultraviolet to near-infrared spectral range. This work reviews efforts to use colloidal nanocrystals as scintillator materials. To date, research on colloidal nanocrystals as scintillators has focused on doped phosphor systems, quantum dots and related structures, and perovskite-based nanocrystals. Among various material classes and forms, colloidal semiconductor nanocrystals stand out thanks to their appealing fluorescence properties, yet understanding of their radioluminescence and cathodoluminescence is incomplete. This review discusses fundamental limits and material design challenges toward achieving high brightness, fast speed, and durable scintillator performance with nanocrystal scintillators. First, this review describes the basic principles and efficiency limitations of scintillation, particularly the large influence of multiple exciton generation in many nanocrystal species, as well as performance metrics. Second, methods for measurement are described. Third, we review the results of the main classes of nanocrystal scintillators, including quantum dots and related particles, perovskites, and doped-phosphor particles. Fourth, scintillation imaging is discussed in terms of the relevant performance metrics and results obtained using nanocrystal materials. Finally, we note the strengths and weaknesses of nanocrystal scintillators and discuss potential areas of further development. [ABSTRACT FROM AUTHOR]

We have synthesized L-cysteine and oleylamine stabilized CsPbBr3 perovskite quantum dots (PQDs) and coupled them with gold nanoparticles (AuNPs). The PQDs and AuNPs, as well as their hybrid nanostructures (HNS), were characterized using UV–visible (UV–vis) and photoluminescence (PL) spectroscopy. The UV–vis spectra show absorption bands of the HNS at 503 and 520 nm, attributed mainly to PQDs and AuNPs, respectively. The PQDs show a strong excitonic PL band peaked at 513 nm from PQDs. The HR-TEM results show the formation of hybrid structures between PQDs and AuNPs, which is also supported by the PL quenching of the PQDs by the coupled AuNPs. Ultrafast dynamics of the exciton and charge carriers in the HNS and pristine PQD were studied using femtosecond transient absorption. Multiexponential fitting of the dynamic data revealed the existence of shallow and deep trap states in pristine PQDs and ultrafast electron transfer from PQDs to AuNPs in the HNS. A kinetic model was proposed to account for the key dynamic processes involved and to extract the time for electron transfer from PQDs to AuNPs in the HNS, found to be ∼2 ps. Dynamic processes in pristine PQDs are largely unchanged by HNS formation with AuNPs. [ABSTRACT FROM AUTHOR]

We have observed a transition from single to double hysteresis of nuclear spin polarization (NSP) with increasing magnetic field in a single InAlAs self-assembled quantum dot, which means the birth of a third stable branch that depends on the field strength. This NSP transition behavior could not be reproduced by standard model calculations using a fixed electron–nuclear spin correlation time τ c under different external field conditions. By introducing the field dependence of τ c , we were able to successfully reproduce the observed NSP transition. This finding on the phenomenological description of the magnetic field dependence will be a future highlight of τ c . [ABSTRACT FROM AUTHOR]

Quantum-dot Cellular Automata (QCA) has become one of the promising studies for nano-scale computing. QCA is one of the candidate technologies to be replaced with CMOS technology. QCA technology not only reduces power consumption and delay but also increases operating frequency and speed. The arithmetic logic unit is the essential component in a processor that performs arithmetic and logical operations. This paper presents a novel 5 × 5 reversible logic gate called the NRRG (Norouzi_Rasouli Reversible Gate) which can be used as the basic building block of 4:1 and 8:1 reversible multiplexers. Then, we have designed a RALU (reversible arithmetic and logic unit) using this gate. Our design can perform 20 operations such as AND, NAND, OR, XOR, XNOR, COPY, addition, and increment. The proposed QCA RALU requires 0.44 μm2 area, 480 QCA cells, and 10 clock phases. The proposed design needs less cell count, delay, and cost of QCA compared to previous works. The structure is implemented without any rotated cells and only uses one layer which improves the manufacturability of the design. The architectures are designed and simulated using QCA Designer 2.0.3. [ABSTRACT FROM AUTHOR]

Recently, deep-ultraviolet (DUV) light-emitting devices have attracted attention for various applications. GaN/AlN superlattices have emerged as a promising alternative for achieving high-efficiency DUV emission. To fabricate superlattices with high crystal quality and abrupt interfaces, we have utilized face-to-face-annealed sputter-deposited AlN template substrates characterized by a flat surface and low dislocation density. Furthermore, radio-frequency plasma-assisted molecular beam epitaxy with in situ reflection high-energy electron diffraction monitoring was employed for the growth process. The growth of the superlattices follows a specific sequence. Step 1: AlN growth, Step 2: conversion of Al droplets to AlN, Step 3: GaN growth, and Step 4: evaporation of Ga droplets. This study explored the impact of GaN thickness on the GaN/AlN superlattice. The GaN thickness was linearly controlled by changing the duration of Step 3. This approach allowed for the growth of a flat GaN layer up to 1 monolayer (ML) and achieved superlattices with abrupt interfaces. Single-peak cathodoluminescence (CL) emission at 240–245 nm was observed from the superlattices, with the peak shift toward longer wavelengths as the GaN thickness increased. In contrast, quantum dot-like GaN islands were generated with a thickness of over 1 ML, induced by compressive strain. Superlattices with thicker GaN exhibited broad CL emission with multiple peaks. However, the AlN barrier layer reduced the surface roughness and maintained abrupt interfaces within the superlattices. Therefore, to obtain sharp single-peak UV emission from GaN/AlN superlattices, the growth sequence should be controlled to obtain flat GaN layers without dots. [ABSTRACT FROM AUTHOR]

This paper addresses the challenge of efficiently designing multiplexer structures in quantum-dot technology circuits. Specifically, it introduces a novel approach to constructing a 2-to-1 multiplexer through a unique gate design that relies on the interaction between cells. The key focus of this design is to minimize the utilization of cells, thereby conserving space and facilitating the creation of more complex combinational and sequential circuits. The methodology involves developing a gate structure that requires the least number of cells compared to existing designs. This reduction in cell usage not only optimizes space utilization but also enhances the scalability of the multiplexer for integration into larger circuits. The proposed gate structure demonstrates a significant improvement, achieving a 15% reduction in the number of cells compared to the previously best-known design. To further evaluate the effectiveness of this novel gate design, the study extends its analysis to include the implementation of various complex circuits such as a 4-to-1 multiplexer, D latch, and T latch. These structures are synthesized using the newly proposed gate design as a fundamental building block. To validate the functionality and performance of these circuits, simulations are conducted using the QCADesigner simulation tool. This comprehensive simulation enables a thorough assessment of the proposed structures across different circuit configurations, providing insights into their operational efficiency and suitability for practical applications in quantum-dot technology. [ABSTRACT FROM AUTHOR]

We present a detailed study on the effects of oxygen on the photoluminescence properties of CdSe/CdS quantum dots (QDs). We investigated the role of oxygen by performing confocal measurements on thin films as well as on single particles while rapidly exchanging the gaseous environment between oxygen and an inert gas atmosphere. We found that the deionization of negatively charged particles by oxygen depends on both the excitation power and the shell thickness of the QDs. For QDs with thin shells, which exhibit strong photoluminescence blinking, we observed that the presence of oxygen affects both band-edge carrier blinking and hot-carrier blinking. [ABSTRACT FROM AUTHOR]

The efficient and stable electroluminescence of quantum dots (QDs) is of great importance in their applications in new display technologies. The short service life of blue QDs, however, hinders their development and commercialization. Different mechanisms have been proposed for the destabilization of QDs in electroluminescent processes. Based on real-time time-dependent density functional theory studies on the QD models covered by Z-type ligands (XAc2, X = Cd, Zn, Mg), the structural evolution is simulated to reveal the mechanism of the reduction reactions induced by electron injection. Our simulations reproduce the experimental observations that the reduction reactions occur at the QD–ligand interface, and the reduced Cd atom is almost in a zero valence state. However, different sites are predicted for the reactions in which the surface metal atom of the QD instead of the metal atom in the ligands is reduced. As a result, one of the arms of the chelate ligand leaves the QD, which tends to cause damage to its electroluminescent performance. Our findings contribute to a mechanistic understanding of the reduction reactions that occurred at the QD–ligand interface. [ABSTRACT FROM AUTHOR]

The doping of CdS quantum dots (QDs) with Cu(I) disrupts electron–hole correlation due to hole trapping by the dopant ion, post-photoexcitation. The present paper examines the effect of such disruption on the rate of photoinduced electron transfer (PET) from the QDs to methyl viologen (MV2+), with implications in their photocatalytic activity. A significantly greater efficiency of PL quenching by MV2+ is observed for the doped QDs than for the undoped ones. Interestingly, the Stern–Volmer plots constructed using PL intensities exhibit an upward curvature for both the cases, while the PL lifetimes remain unaffected. This observation is rationalized by considering the adsorption of the quencher on the surface of the QDs and ultrafast PET post-photoexcitation. Ultrafast transient absorption experiments confirm a faster electron transfer for the doped QDs. It is also realized that the transient absorption experiment yields a more accurate estimate of the binding constant of the quencher with the QDs, than the PL experiment. [ABSTRACT FROM AUTHOR]

This article explores the shift in chemical physics research towards studying single molecules and nanoparticles instead of bulk samples. Advancements in experimental techniques, such as single-molecule absorption and fluorescence spectroscopy, have made this shift possible. The article discusses various observations made through single-molecule spectroscopy, as well as theoretical considerations and applications in biology, materials science, and nanophotonics. It provides a summary of studies conducted using single-molecule spectroscopy in different disciplinary categories, demonstrating its interdisciplinary nature. The article concludes by discussing the challenges and future directions in the field, including integrating particle tracking with time-dependent spectroscopy and actively manipulating nanoscale objects. [Extracted from the article]

A comprehensive study on the photo-excited relaxation dynamics in semiconducting perovskite quantum dots (PQDs) is pivotal in realizing their extensive potential for optoelectronics applications. Among different competing photoinduced relaxation kinetics, energy transfer and charge transfer (CT) in PQDs need special attention, as they often influence the device efficacy, particularly with the donor–acceptor hybrid architecture. In this work, we explore a detailed investigation into photoinduced CT dynamics in mixed halide undoped CsPb(Br/Cl)3 and Mn2+ doped CsPb(Br/Cl)3 PQDs with a quinone molecule, p-benzoquinone (BQ). The energy level alignment of undoped PQDs with BQ allows an efficient CT, whereas Mn2+ doping reduces the CT efficiency, experiencing a competition between energy transfer from host to dopant and CT to BQ. The conductive atomic force microscopy measurements unveil a direct correlation with the spectroscopic studies by showing a significant improvement in the conductance of undoped PQDs in the presence of BQ, while an inappreciable change is observed for doped PQDs. A much-reduced transition voltage and barrier height in the presence of BQ further validate faster CT for undoped PQD than the doped one. Furthermore, Mn2+ doping in PQDs is observed to enhance their stability, showing better air and thermal stability compared to their undoped counterparts. These results reveal that doping strategy can regulate the CT dynamics in these PQDs and increase their stability, which will be beneficial for the development of desired optoelectronic devices with long-term stability. [ABSTRACT FROM AUTHOR]

Photocurrent measurements are widely used to study the intrinsic optoelectronic properties of semiconductors, such as photocarrier generation efficiency and carrier mobility, as well as evaluate the performance of optoelectronic devices, such as solar cells and photodetectors. Interferometric spectroscopy precisely measures optical properties and gathers optical spectra information on semiconductors. Consequently, photocurrent-based interferometric measurements, with high signal-to-noise ratios, high resolution, and broad frequency bandwidths, can probe the energy distributions of low-density defects and impurities and investigate charge transport in materials and devices. Here, we demonstrate that photocurrent interference spectroscopy reveals the intrinsic properties of solar-cell materials: bulk crystals of GaAs and halide perovskite, and thin films of halide perovskite and quantum dot. We show that homodyne interference spectroscopy of photocurrent can monitor low-density localized states in semiconductors and that it can be used in combination with other spectroscopy techniques, such as photoluminescence measurements, to provide a deep understanding of photocurrent generation processes. Furthermore, we show that heterodyne interference spectroscopy of photocurrent can be used to investigate the frequency dependence of material parameters, such as the dielectric constant, absorption coefficient, and reflectance. As an application, we used interference spectroscopy of photocurrent to show the impact of multiexcitons on the photoabsorption and photocarrier generation processes in quantum dot solar cells. Finally, we used it to reveal the distinctive spectral characteristics at the band edge of a halide perovskite, which is considered to be an exceptional solar-cell material with high energy conversion efficiency. [ABSTRACT FROM AUTHOR]

Chiral perovskite materials are being extensively studied as one of the most promising candidates for circularly polarized luminescence (CPL)-related applications. Balancing chirality and photoluminescence (PL) properties is of great importance for enhancing the value of the dissymmetry factor (glum), and a higher glum value indicates better CPL. Chiral perovskite/quantum dot (QD) composites emerge as an effective strategy for overcoming the dilemma that achieving strong chirality and PL in chiral perovskite while at the same time achieving high glum in this composite is very crucial. Here, we choose diphenyl sulfoxide (DPSO) as an additive in the precursor solution of chiral perovskite to regulate the lattice distortion. How structural variation affects the chiral optoelectronic properties of the chiral perovskite has been further investigated. We find that chiral perovskite/CdSe–ZnS QD composites with strong CPL have been achieved, and the calculated maximum |glum| of the composites increased over one order of magnitude after solvent-additive modulation (1.55 × 10−3 for R-DMF/QDs, 1.58 × 10−2 for R-NMP-DPSO/QDs, −2.63 × 10−3 for S-DMF/QDs, and −2.65 × 10−2 for S-NMP-DPSO/QDs), even at room temperature. Our findings suggest that solvent-additive modulation can effectively regulate the lattice distortion of chiral perovskite, enhancing the value of glum for chiral perovskite/CdSe–ZnS QD composites. [ABSTRACT FROM AUTHOR]

Quantum Dot Cellular Automata (QCA) is an emerging trend in the field of nanoelectronics, and computing can be regarded as an alternative to the traditional complementary metal–oxide–semiconductor technology. The paper is devoted to the study of the key functional properties of the cells for molecular QCA based on mixed valence molecules. The theoretical results for the heat dissipation under the conditions of the fast nonadiabatic switching event and cell–cell response function are obtained in the framework of the quantum-mechanical vibronic approach. These results are parameterized using the previous reliable ab initio calculations performed for oxidized norbornadiene and its polycyclic derivatives with variable lengths of the bridge. The comparative analysis of the dimeric and bidimeric molecular cells composed of these compounds is given. It is underlined that the conditions of a strong non-linear response and a low heat release are contradictory. However, despite this problem, a parametric regime is proposed, which provides a low heat release in combination with a strong nonlinear response of the working cell to the electric field induced by the polarized driver cell. [ABSTRACT FROM AUTHOR]

Carbon quantum dots have become attractive in various applications, such as drug delivery, biological sensing, photocatalysis, and solar cells. Among these, pH sensing via luminescence lifetime measurements of surface-functionalized carbon dots is one application currently investigated for their long lifetime and autonomous operation. In this article, we explore the theoretical connection between excitation lifetimes and the pH value of the surrounding liquid via the protonation and deprotonation of functional groups. Example calculations applied to m-phenylenediamine, phloroglucinol, and tethered disperse blue 1 are shown by applying a separation approach treating the electronic wave function of functional groups separately from the internal electronic structure of the (large) carbon dot. The bulk of the carbon dot is treated as an environment characterized by its optical spectrum that shifts the transition rates of the functional group. A simple relationship between pH, pKa, and mixed fluorescence lifetime is derived from the transition rates of the protonated and deprotonated states. pH sensitivity improves when the difference in the transition rates is greatest between protonated and deprotonated species, with the greatest sensitivity found where the pKa is close to the pH region of interest. The introduced model can directly be extended to consider multicomponent liquids and multiple protonation states. [ABSTRACT FROM AUTHOR]

In this paper, we study theoretically the electron and spectral properties of Ge 1 − x Sn x systems, including alloys, cubic- and spherical quantum dots. The single-particle electron and hole states are calculated within the s p 3 d 5 s ∗ tight-binding approach and used in further modeling of the optical properties. We systematically study the interplay of Sn-driven indirect–direct bandgap transition and the quantum confinement effect in systems of reduced dimensionality. We demonstrate the regime of sizes and compositions, where the ground state in Ge 1 − x Sn x quantum dots is optically active. Finally, we calculate absorbance spectra in experimentally relevant colloidal quantum dots and demonstrate satisfactory agreement with experimental data. [ABSTRACT FROM AUTHOR]

High fidelity single photon sources are required for the implementation of quantum information processing and communications protocols. Although colloidal quantum dots (CQDs) are single photon sources, their efficacy is limited by their tendency to show finite multiphoton emission at higher excitation powers. Here, we show that wave function engineering of CQDs enables the realization of emitters with significantly improved single photon emission performance. We study the ZnS/CdSe/CdS system. It is shown that this system offers significantly improved probabilities of single photon emission. While conventional CQDs such as CdSe/CdS exhibit a g2(0) > 0.5 ± 0.02 at ⟨N⟩ = 2.17, ZnS/CdSe/CdS show a greatly improved g2(0) ≈ 0.04 ± 0.01. Improved single photon emission performance encourages the use of colloidal materials as quantum light sources in emerging quantum devices. [ABSTRACT FROM AUTHOR]

Colloidal quantum dots are of increasing interest for mid-infrared detection and emission, but device performances will vastly benefit from reducing the non-radiative recombination. Empirically, the photoluminescence quantum yield decreases exponentially toward the mid-infrared, which appears similar to the energy gap law known for molecular fluorescence in the near-infrared. For molecules, the mechanism is electron–vibration coupling and fast internal vibrational relaxation. Here, we explore the possible mechanisms for inorganic quantum dots. The primary mechanism is assigned to an electric dipole near-field energy transfer from the quantum dot electronic transitions to the infrared absorption of surface organic ligands and then to the multiphonon absorption of the quantum dot inorganic core or the surrounding inorganic matrix. In order to obtain luminescent quantum dots in the 3–10 μm range, we motivate the importance of using inorganic matrices, which have a higher infrared transparency compared to organic materials. At longer wavelengths, inter-quantum dot energy transfer is noted to be much faster than radiative relaxation, indicating that bright mid-infrared colloidal quantum dot films might then benefit from dilution. [ABSTRACT FROM AUTHOR]

The efficient conversion of solar energy to chemical energy represents a critical bottleneck to the energy transition. Photocatalytic splitting of water to generate solar fuels is a promising solution. Semiconductor quantum dots (QDs) are prime candidates for light-harvesting components of photocatalytic heterostructures, given their size-dependent photophysical properties and band-edge energies. A promising series of heterostructured photocatalysts interface QDs with transition-metal oxides which embed midgap electronic states derived from the stereochemically active electron lone pairs of p-block cations. Here, we examine the thermodynamic driving forces and dynamics of charge separation in Sb2VO5/CdSe QD heterostructures, wherein a high density of Sb 5s2-derived midgap states are prospective acceptors for photogenerated holes. Hard-x-ray valence band photoemission spectroscopy measurements of Sb2VO5/CdSe QD heterostructures were used to deduce thermodynamic driving forces for charge separation. Interfacial charge transfer dynamics in the heterostructures were examined as a function of the mode of interfacial connectivity, contrasting heterostructures with direct interfaces assembled by successive ion layer adsorption and reaction (SILAR) and interfaces comprising molecular bridges assembled by linker-assisted assembly (LAA). Transient absorption spectroscopy measurements indicate ultrafast (<2 ps) electron and hole transfer in SILAR-derived heterostructures, whereas LAA-derived heterostructures show orders of magnitude differentials in the kinetics of hole (<100 ps) and electron (∼1 ns) transfer. The interface-modulated kinetic differentials in electron and hole transfer rates underpin the more effective charge separation, reduced charge recombination, and greater photocatalytic efficiency observed for the LAA-derived Sb2VO5/CdSe QD heterostructures. [ABSTRACT FROM AUTHOR]

Metal ion-induced water pollution is attracting increasing public attention. Perovskite quantum dots and metal–organic frameworks (MOFs), owing to their outstanding properties, hold promise as ideal probes for detecting metal ions. In this study, a composite material, MAPbBr3@PCN-221(Fe), was prepared by encapsulating MAPbBr3 quantum dots with PCN-221(Fe), demonstrating high chemical stability and good reusability. The composite material shows a sensitive fluorescence turn-on signal in the presence of silver ions. The fluorescence intensity of the composite material exhibits a linear relationship with the concentration of Ag+ in the solution, with a low detection limit of 8.68 µM. Moreover, the fluorescence signal exhibits a strong selectivity for Ag+, enabling the detection of Ag+ concentration. This fluorescence turn-on signal originates from the Ag+-bridged energy transfer from the conductive band of MAPbBr3 to the excited state of the MOF, which is directly proportional to the concentration of silver ions. Simultaneously, this finding may open up a new possibility in artificial controlled energy transfer from perovskite to MOF for future development. [ABSTRACT FROM AUTHOR]

Determining the correlation between the size of a single quantum dot (QD) and its photoluminescence (PL) properties is a challenging task. In the study, we determine the size of each QD by measuring its absorption cross section, which allows for accurate investigation of size-dependent PL blinking mechanisms and volume scaling of the biexciton Auger recombination at the single-particle level. A significant correlation between the blinking mechanism and QD size is observed under low excitation conditions. When the QD size is smaller than their Bohr diameter, single CsPbI3 perovskite QDs tend to exhibit BC-blinking, whereas they tend to exhibit Auger-blinking when the QD size exceeds their Bohr diameter. In addition, by extracting bright-state photons from the PL intensity trajectories, the effects of QD charging and surface defects on the biexcitons are effectively reduced. This allows for a more accurate measurement of the volume scaling of biexciton Auger recombination in weakly confined CsPbI3 perovskite QDs at the single-dot level, revealing a superlinear volume scaling (τXX,Auger ∝ σ1.96). [ABSTRACT FROM AUTHOR]

The non-equilibrium Green's function (NEGF) and quantum master equation (QME) are two main classes of approaches for electronic transport. We discuss various Floquet variances of these formalisms for transport properties of a quantum dot driven via interaction with an external periodic field. We first derived two versions of the Floquet NEGF. We also explore an ansatz of the Floquet NEGF formalism for the interacting systems. In addition, we derived two versions of Floquet QME in the weak interaction regime. With each method, we elaborate on the evaluation of the expectation values of the number and current operators. We examined these methods for transport through a two-level system that is subject to periodic driving. The numerical results of all four methods show good agreement for non-interacting systems in the weak regime. Furthermore, we have observed that circular light can introduce spin current. We expect these Floquet quantum transport methods to be useful in studying molecular junctions exposed to light. [ABSTRACT FROM AUTHOR]

Chiral quantum dots (QDs) are promising materials applied in many areas, such as chiral molecular recognition and spin selective filter for charge transport, and can be prepared by facile ligand exchange approaches. However, ligand exchange leads to an increase in surface defects and reduces the efficiencies of radiative recombination and charge transport, which restricts further applications. Here, we investigate the light-induced photoluminescence (PL) enhancement in chiral L- and D-cysteine CdSe QD thin films, providing a strategy to increase the PL. The PL intensity of chiral CdSe QD films can be significantly enhanced over 100 times by continuous UV laser irradiation, indicating a strong passivation of surface defects upon laser irradiation. From the comparative measurements of the PL intensity evolutions in vacuum, dry oxygen, air, and humid nitrogen atmospheres, we conclude that the mechanism of PL enhancement is photo-induced surface passivation with the assistance of water molecules. [ABSTRACT FROM AUTHOR]

This study explored the interplay between the ligand–surface chemistry of colloidal CsPbBr3 nanowires (NWs) and their optical properties. The ligand equilibrium was probed using nuclear magnetic resonance spectroscopy, and by perturbing the equilibrium via dilution, the gradual removal of ligands from the CsPbBr3 surface was observed. This removal was correlated with an increase in the surface defect density, as suggested by a broadening of the photoluminescence (PL) spectrum, a decrease in the PL quantum yield (PLQY), and quenching of the PL decay. These results highlight similar surface binding between the traditional CsPbBr3 quantum dots and our NWs, thereby expanding the scope of well-established ligand chemistry to a relatively unexplored nanocrystal morphology. By controlling the dilution factor, it was revealed that CsPbBr3 NWs achieve a PLQY of 72% ± 2% and a relatively long average PL lifetime of 400 ± 10 ns, without relying on additional surface passivation techniques, such as ligand exchange. [ABSTRACT FROM AUTHOR]

We investigate the entanglement between the spins of two quantum dots that are not simultaneously connected to the same system. Quantum entanglement among localized spins is a crucial property for the advancement of quantum computing and quantum information. Generating and controlling an entangled state between quantum dots have garnered significant attention in recent years for this reason. In this study, we demonstrate that information about the spin orientation of a quantum dot can be preserved, utilizing Kondo entanglement, within a reservoir of electrons. Subsequently, this information can be transmitted to another dot after the initial dot has been decoupled from the reservoirs. We employ a double quantum dot system in a parallel geometry to establish the initial state, where each dot interacts with reservoirs of different symmetries. A specific phase in the couplings is chosen to induce antiferromagnetic spin correlation between the dots. The time evolution of the initial state is analyzed using the time-dependent density matrix renormalization group method. Our findings reveal that a partially entangled state between the dots can be achieved, even when they are not simultaneously connected. This entangled state arises transiently and dissipates in the stationary state. The stability of the state observed during the transient phase is demonstrated. To comprehend the details of these phenomena, we employ a canonical transformation of real space. [ABSTRACT FROM AUTHOR]

A unique on-chip method for the direct correlation of optical properties, with atomic-scale chemical–structural characteristics for a single quantum dot (QD), is developed and utilized in various examples. This is based on performing single QD optical characterization on a modified glass substrate, followed by the extraction of the relevant region of interest by focused-ion-beam–scanning electron microscope processing into a lamella for high resolution scanning transmission electron microscopy (STEM) characterization with atomic scale resolution. The direct correlation of the optical response under an electric field with STEM analysis of the same particle allows addressing several single particle phenomena: first, the direct correlation of single QD photoluminescence (PL) polarization and its response to the external field with the QD crystal lattice alignment, so far inferred indirectly; second, the identification of unique yet rare few-QD assemblies, correlated directly with their special spectroscopic optical characteristics, serving as a guide for future designed assemblies; and third, the study on the effect of metal island growth on the PL behavior of hybrid semiconductor–metal nanoparticles, with relevance for their possible functionality in photocatalysis. This work, therefore, establishes the use of the direct on-chip optical–structural correlation method for numerous scenarios and timely questions in the field of QD research. [ABSTRACT FROM AUTHOR]

This article reports the superparamagnetic behavior of metal-free nitrogen-doped graphene quantum dots (N-GQDs). The pulsed laser ablation (PLA) method was utilized to synthesize N-GQDs with an average diameter of 3.45 nm and a high doping level (N/C) of 1.4. Magnetic properties of as-synthesized N-GQDs were explored by performing magnetization vs magnetic field (M–H) and magnetization vs temperature (M–T) measurements. M–H plots measured in a temperature range of 2–300 K revealed the superparamagnetic behavior of N-GQDs. The value of saturation magnetization was found to be directly correlated to nitrogen concentration and a saturation magnetization up to 28.7 emu/g was obtained at room temperature (300 K). M–T measurements with zero-field-cooled (ZFC) and field-cooled (FC) conditions were employed to study anisotropy energy barriers and blocking temperature. A variation in the blocking temperature (TB) from 288 to 61 K was observed when the external magnetic field (H) was changed from 0.1 to 0.6 T. The origin of superparamagnetism was attributed to the presence of graphitic nitrogen bonding configuration and defect states. The observed superparamagnetic properties along with the optical properties of N-GQDs create an opportunity for developing materials for biomedical applications and data recording devices. [ABSTRACT FROM AUTHOR]

We present a systematic investigation of the optical losses in GaAs photonic crystal cavities with and without embedded self-assembled In(Ga)As quantum dots (QDs) to shed light on additional loss mechanisms related to the presence of the QDs. To clarify the role of the measurement method, we propose an experimental configuration where the optical properties can be evaluated simultaneously through reflection and photoluminescence measurements. Independently of the measurement method, we observe a reduced quality (Q) factor in cavities with embedded QDs when compared to the passive counterparts. Our analysis indicates that these additional losses—about 7 GHz—are unrelated to direct excitonic absorption for the investigated areal QD densities of 175 μ m − 2 . We analyze several mechanisms which could explain our observations and suggest that a possible origin could be unsaturable absorption from midgap defects introduced by the QD growth. [ABSTRACT FROM AUTHOR]

Semiconductor quantum dots (QDs) are one of the leading candidates for realizable qubits, as well as for many other advances in quantum computing and quantum communication. The spatial overlapping of wavefunctions describing each single electron in these nanoscale devices results in tunable spatial entanglement. In this article, we explore the case of two electrons in two-dimensional double quantum dot systems. We compute the two-particle wavefunction through a variational method combined with Hermite finite elements and study the spatial entanglement of electrons. We show that symmetry in the geometry of the double quantum dots plays a role in obtaining optimal entanglement, while a broken symmetry can lead to additional resonances in entanglement that are associated with the crossings of states. We also show that one can finely tune the level of spatial entanglement by altering the geometry of the quantum dots or by applying external fields, which corresponds to an "entanglement spectroscopy." Finally, we study how impurities in the potential profile of the QDs affect the level of entanglement. [ABSTRACT FROM AUTHOR]

Limited stability of blue quantum dot light-emitting diodes (QLEDs) under current stress impedes commercialization. Multi-layer structures of the state-of-the-art blue QLEDs pose significant difficulty in the fundamental understanding of degradation mechanisms. Here, by applying transient electroluminescence measurements, we disentangle charge transport in both pristine and degraded blue QLEDs. By varying thicknesses of the charge transport layers and the emissive layer, respectively, we show that the charge transport in pristine QLEDs is primarily dominated by holes. Furthermore, the degradation of QLEDs under electrical stress is governed by the decrease of hole transport in the emissive quantum dot layer due to the formation of hole traps. [ABSTRACT FROM AUTHOR]

Using the novel process of hot N+-ion implantation at 800 °C into Si quantum dots (Si-QDs) with approximately 3.2 nm fabricated by hot Si+-ion implantation into an SiO2 layer and post-Ar annealing, we experimentally demonstrated that the photoluminescence intensity (IPL) of the Si-QDs increased with increasing N+-ion dose (D N + ). Post-N2 high-temperature annealing without hot N+-ion implantation, as a reference process, also increased the IPL of Si-QDs, because N atoms trapped within Si-QDs, which was evaluated by secondary ion mass spectrometry, terminate the dangling bonds within Si-QDs and at the Si/SiO2 interface. Additionally, the IPL of Si-QDs showed the maximum value at the optimal D N + of 5 × 1015 cm−2, which was 1.4-fold higher than that observed without hot N+-ion implantation. With a short post-annealing time (<60 min), the increase in IPL owing to N+-ion implantation was considerably larger than that caused by N2 annealing, which is likely due to the efficiency of the termination of the dangling bonds of the Si-QDs by the N+-ions. This is an advantage of the hot N+-ion implantation technique. Forming gas annealing after furnace annealing also induced a larger IPL than that observed before forming gas annealing. However, the maximum IPL observed after forming gas annealing was completely independent of the conditions of furnace annealing and D N + . This suggests that the perfect termination of the dangling bonds of the Si-QDs may be realized via forming gas annealing after furnace annealing. [ABSTRACT FROM AUTHOR]

Transient absorption (TA) spectroscopy of semiconductor nanocrystals (NCs) is often used for excited state population analysis, but recent results suggest that TA bleach signals associated with multiexcitons in NCs do not scale linearly with exciton multiplicity. In this manuscript, we probe the factors that determine the intensities and spectral positions of exciton and biexciton components in the TA spectra of CdSe quantum dots (QDs) of five diameters. We find that, in all cases, the peak intensity of the biexciton TA spectrum is less than 1.5 times that of the single exciton TA spectrum, in stark contrast to a commonly made assumption that this ratio is 2. The relative intensities of the biexciton and exciton TA signals at each wavelength are determined by at least two factors: the TA spectral intensity and the spectral offset between the two signals. We do not observe correlations between either of these factors and the particle diameter, but we find that both are strongly impacted by replacing the native organic surface-capping ligands with a hole-trapping ligand. These results suggest that surface trapping plays an important role in determining the absolute intensities of TA features for CdSe QDs and not just their decay kinetics. Our work highlights the role of spectral offsets and the importance of surface trapping in governing absolute TA intensities. It also conclusively demonstrates that the biexciton TA spectra of CdSe QDs at the band gap energy are less than twice as intense as those of the exciton. [ABSTRACT FROM AUTHOR]

We investigate the optical properties appearing in a nanostructure that is composed of an asymmetric double semiconductor quantum dot (SQD) molecule and a metal nanoparticle (MNP). The profile of the total linear absorption spectrum is proportional to the SQD contribution, while the MNP contribution is important. The profile of the doublet of resonances detected on the total linear absorption spectrum creates a transparency window. The doublet is asymmetric for small SQD-MNP distances and has a narrow peak and a wide peak. The width of the transparency window is increased, either with the enhancement of the rate at which the electron tunneling effect takes place within the double SQD molecule or with the decrease of the distance that separates the SQD molecule from the center of the MNP. The steep slope detected on the linear dispersion spectrum for frequencies laying within the transparency window owes its presence to the tunneling induced transparency and leads to slow light production. The corresponding value of the slow down factor is maximized for low values of the electron tunneling rate as well as for low center-to-center distances between the components of the hybrid nanostructure. [ABSTRACT FROM AUTHOR]

The biological reduction of N2 to ammonia requires the ATP-dependent, sequential delivery of electrons from the Fe protein to the MoFe protein of nitrogenase. It has been demonstrated that CdS nanocrystals can replace the Fe protein to deliver photoexcited electrons to the MoFe protein. Herein, light-activated electron delivery within the CdS:MoFe protein complex was achieved in the frozen state, revealing that all the electron paramagnetic resonance (EPR) active E-state intermediates in the catalytic cycle can be trapped and characterized by EPR spectroscopy. Prior to illumination, the CdS:MoFe protein complex EPR spectrum was composed of a S = 3/2 rhombic signal (g = 4.33, 3.63, and 2.01) consistent with the FeMo-cofactor in the resting state, E0. Illumination for sequential 1-h periods at 233 K under 1 atm of N2 led to a cumulative attenuation of E0 by 75%. This coincided with the appearance of S = 3/2 and S = 1/2 signals assigned to two-electron (E2) and four-electron (E4) reduced states of the FeMo-cofactor, together with additional S = 1/2 signals consistent with the formation of E6 and E8 states. Simulations of EPR spectra allowed quantification of the different E-state populations, along with mapping of these populations onto the Lowe–Thorneley kinetic scheme. The outcome of this work demonstrates that the photochemical delivery of electrons to the MoFe protein can be used to populate all of the EPR active E-state intermediates of the nitrogenase MoFe protein cycle. [ABSTRACT FROM AUTHOR]

The temperature dependence of the optical properties of In0.4Ga0.6As0.98N0.02 quantum dots (QDs) was investigated using continuous-wave and time-resolved photoluminescence (PL). Significant increases in the PL peak energy and the PL linewidth were observed at temperatures above 200 K, which reflected the high luminescence efficiency of ground and excited states at high temperatures. The PL decay times of the ground state were almost constant between 200 and 300 K at 200–220 ps, which were significantly longer than that of 38 ps for the In0.4Ga0.6As QDs at 300 K. The temperature independence of the PL decay time represents significant suppression of the thermal escape and the thermal excitation of electrons because the electron ground-state localization energy is much larger than the thermal energy. The PL intensity of the In0.4Ga0.6As0.98N0.02 QDs was seven times stronger than that of the In0.4Ga0.6As QDs at 300 K, and this tendency was maintained up to 400 K with a PL intensity one order of magnitude stronger. These findings demonstrate that lowering the QD conduction band by nitrogen incorporation is an effective approach for achieving strong QD luminescence above room temperature. [ABSTRACT FROM AUTHOR]

Precise positioning of single site-controlled inverted pyramidal InGaAs quantum dots (QDs) at the antinode of a GaAs photonic crystal cavity with nanometer-scale accuracy holds unique advantages compared to self-assembled QDs and offers great promise for practical on-chip photonic quantum information processing. However, the strong coupling regime in this geometry has not yet been achieved due to the low cavity Q-factor based on the (111)B-oriented membrane structures. Here, we reveal the onset of phonon-mediated coherent exciton–photon interaction on our tailored single site-controlled InGaAs QD–photonic crystal cavity. Our results present the Rabi-like oscillation of luminescence intensity between excitonic and photonic components correlated with their energy splitting pronounced at small detuning. Such Rabi-like oscillation is well reproduced by modeling the coherent exchange of the exciton-photon population. The modeling further reveals an oscillatory two-time covariance at QD-cavity resonance, which indicates that the system operates at the onset of the strong coupling regime. Moreover, by using the cavity mode as a probe of the virtual state of the QD induced by phonon scattering, it reveals an increase in phonon scattering rates near the QD–cavity resonance and asymmetric phonon emission and absorption rate of even around 50 K. [ABSTRACT FROM AUTHOR]

Prolonging the lifetime of photoinduced hot carriers in lead–halide perovskite quantum dots (QDs) is highly desirable because it can help improve the photovoltaic conversion efficiency. Ligand engineering has recently become a promising strategy to achieve this; nevertheless, mechanistic studies in this field remain limited. Herein, we propose a new scenario of ligand engineering featuring Pb2+/Br− site-selective capping on the surface of CsPbBr3 QDs. Through joint observations of temperature-dependent photoluminescence, ultrafast transient absorption, and Raman spectroscopy of the two contrasting model systems of CsPbBr3 QDs (i.e., capping with organic ligand only vs hybrid organic/inorganic ligands), we reveal that the phononic regulation of Pb–Br stretching at the Br-site (relative to Pb-site) leads to a larger suppression of charge–phonon coupling due to a stronger polaronic screening effect, thereby more effectively retarding the hot-carrier cooling process. This work opens a new route for the manipulation of hot-carrier cooling dynamics in perovskite systems via site-selective ligand engineering. [ABSTRACT FROM AUTHOR]

Spin qubit systems are one of the promising candidates for quantum computing. The quantum dot (QD) arrays are intensively investigated by many researchers. Because the energy-difference between the up-spin and down-spin states is very small, the detection of the qubit state is of prime importance in this field. Moreover, many wires are required to control qubit systems. Therefore, the integration of qubits and wires is also an important issue. In this study, the measurement process of QD arrays is theoretically investigated using resonant tunneling, controlled by a conventional transistor. It is shown that the number of possible measurements during coherence time can exceed a hundred under the backaction of the measurements owing to the nonlinear characteristics of resonant tunneling. It is also discussed to read out the measurement results by the conventional transistor. [ABSTRACT FROM AUTHOR]

The luminescence efficiency of AlxGa1−xN quantum dots (QDs) and quantum wells (QWs), buried in AlN cladding layers and emitting in the ultraviolet range between 234 and 310 nm, has been investigated. The growth and optical properties have been done using similar aluminum composition (varying from 0.4 to 0.75) for both QDs and QWs. In order to compare as much as possible the optical properties, the QWs were fabricated with a growth time tuned such that the QW width is similar to the average height of the QDs. The photoluminescence (PL) showed emission ranging from 4 to 5.4 eV, putting into evidence differences in terms of full width at half maximum, PL intensity, and asymmetry of the line shape between QDs and QWs. The results show shorter wavelengths and a slightly narrower PL linewidth for QWs. To determine the light emission dependence with the electric field direction in the crystal, the evolutions of the emission diagrams for all samples were recorded along two orthogonal directions, namely, the "in-plane" (growth) and the "on-side" directions, from which the light emission was collected. For the whole QDs and QWs samples' series, the shapes of the emission diagram indicate emission in both in-plane and on-side directions, as evidenced by intra-valence band mixings caused by strain effects combined with the anisotropic Coulomb interactions that are particularly contributing to the polarization at wavelengths below 260 nm. Furthermore, the degree of polarization, determined for each sample, showed good agreement with results from the literature. [ABSTRACT FROM AUTHOR]

The lead halide perovskites have emerged as promising materials with intriguing photo-physical properties and have immense potential for photovoltaic applications. A comprehensive study on the kinetics of charge carrier (electron/hole) generation and transfer across the interface is key to realizing their future scope for efficient device engineering. Herein, we investigate the interfacial charge transfer (CT) dynamics in cesium lead halide (CsPbBr3) perovskite quantum dots (PQDs) with energetically favorable electron acceptors, anthraquinone (AQ) and p-benzoquinone (BQ), and hole acceptors such as pyrene and 4-(dimethylamino)pyridine (DMAP). With various steady-state and time-resolved spectroscopic and microscopic measurements, a faster electron transfer rate is estimated for CsPbBr3 PQDs with BQ compared to that of AQ, while a superior hole transfer for DMAP is divulged compared to pyrene. In concurrence with the spectroscopic measurements, conducting atomic force microscopic studies across the electrode-PQD-electrode junction reveals an increment in the conductance of the PQD in the presence of both the electron and hole acceptors. The variation of the density of states calculation in the presence of the hole acceptors offers strong support and validation for faster CT efficiency. The above findings suggest that a careful selection of simple yet efficient molecular arrangements can facilitate rapid carrier transfer, which can be designed as auxiliary layers for smooth CT and help in the engineering of cost-effective photovoltaic devices. [ABSTRACT FROM AUTHOR]

Quantum dots (QDs) have attracted much attention and exhibit many attractive properties, including high absorption coefficient, adjustable bandgap, high brightness, long-term stability, and size-dependent emission. It is known that to obtain high-quality luminescent properties (i.e. emission color, color purity, quantum yield, and stability), the synthesis parameters must be precisely controlled. In this work, we have constructed a database with CdTe aqueous synthesis parameters and spectroscopic results and applied machine learning algorithms to better understand the influence of the main synthesis parameters of CdTe QDs on their final emission properties. A strong dependence of the final emission wavelength with the reaction time and surface ligands and precursors concentrations was demonstrated. These parameters adjusted synchronously were shown to be very useful for provide ideal synthesis conditions for the preparation of CdTe QDs with desirable emission wavelengths. Moreover, applying the algorithms correctly allows for obtaining information and insights into the growth kinetics of QDs under different synthetic conditions. [ABSTRACT FROM AUTHOR]

In order to explore the interplay among heat, charge, and spin, we investigate the spin-related thermoelectricity of a hybrid double quantum dot Aharonov–Bohm interferometer with Rashba spin–orbit coupling (RSOC). Interestingly, the nonzero RSOC phase difference can induce significant spin-dependent thermoelectric transport. Not only can the strong violation of the Wiedemann-Franz law be obtained, but also a pure spin-Seebeck effect can be produced, which may serve as a pure spin-current generator. The influence of system parameters on thermoelectric coefficients (especially for spin counterparts) are analyzed in detail, and the underlying physics is further elucidated. Furthermore, the spin figure of merit can be much larger than the charge one, which, thus, provides a realistic possibility of engineering spin thermoelectric devices with high performance. These results obtained may be of interest for developing spin thermoelectric devices in the field of spin caloritronics. [ABSTRACT FROM AUTHOR]

The Zeeman-split spin states of a single quantum dot can be used together with its optical trion transitions to form a spin–photon interface between a stationary (the spin) and a flying (the photon) quantum bit. In addition to long coherence times of the spin state itself, the limiting decoherence mechanisms of the trion states are of central importance. Here, we investigate in time-resolved resonance fluorescence the electron spin and trion dynamics in a single self-assembled quantum dot in an applied magnetic field of up to B = 10 T. The quantum dot is only weakly coupled to an electron reservoir with tunneling rates of about 1 ms − 1 . Using this sample structure, we can measure, in addition to the spin-flip rate of the electron and the spin-flip Raman rate of the trion transition, the Auger recombination process that scatters an Auger electron into the conduction band. The Auger effect destroys the radiative trion transition and leaves the quantum dot empty until an electron tunnels from the reservoir into the dot. The combination of an Auger recombination event with subsequent electron tunneling from the reservoir can flip the electron spin and thus constitutes another mechanism that limits the spin lifetime. [ABSTRACT FROM AUTHOR]

We fabricated a photoconductive antenna (PCA) with Er-doped InAs quantum dot (QD) layers on a GaAs substrate and demonstrated THz wave generation with 1.5 μm pump. In terahertz time-domain spectroscopy (THz-TDS), PCAs require high mobility and short lifetimes of photocarriers since the carriers need to respond rapidly to optical pulses for broad THz generation and detection with a high time resolution. In this study, to achieve PCA operation at an optical communication wavelength band of 1.5 μm, a substrate for a PCA was fabricated using stacked Er-doped-InAs QD layers. Then, photocurrent measurements were performed to observe optical absorption in the 1.5 μm band. The results indicated the high capability of the PCA for THz wave generation and detection, in fact, which enabled us to generate the THz wave in the 1.5 μm band optical system. [ABSTRACT FROM AUTHOR]

InP-based quantum dots (QDs) have Stokes shifts and photoluminescence (PL) line widths that are larger than in II–VI semiconductor QDs with comparable exciton energies. The mechanisms responsible for these spectral characteristics are investigated in this paper. Upon comparing different semiconductors, we find the Stokes shift decreases in the following order: InP > CdTe > CdSe. We also find that the Stokes shift decreases with core size and decreases upon deposition of a ZnSe shell. We suggest that the Stokes shift is largely due to different absorption and luminescent states in the angular momentum fine structure. The energy difference between the fine structure levels, and hence the Stokes shifts, are controlled by the electron–hole exchange interaction. Luminescence polarization results are reported and are consistent with this assignment. Spectral widths are controlled by the extent of homogeneous and inhomogeneous broadening. We report PL and PL excitation (PLE) spectra that facilitate assessing the roles of homogeneous and different inhomogeneous broadening mechanisms in the spectra of zinc-treated InP and InP/ZnSe/ZnS particles. There are two distinct types of inhomogeneous broadening: size inhomogeneity and core–shell interface inhomogeneity. The latter results in a distribution of core–shell band offsets and is caused by interfacial dipoles associated with In–Se or P–Zn bonding. Quantitative modeling of the spectra shows that the offset inhomogeneity is comparable to but somewhat smaller than the size inhomogeneity. The combination of these two types of inhomogeneity also explains several aspects of reversible hole trapping dynamics involving localized In3+/VZn2− impurity states in the ZnSe shells. [ABSTRACT FROM AUTHOR]