Hole Wave Functions Research Articles

UNTANGLING THE VALLEY STRUCTURE OF STATES FOR INTRAVALLEY EXCHANGE ANISOTROPY IN LEAD CHALCOGENIDES QUANTUM DOTS

We put forward a generalized procedure which allows to restore the bulk-like electron and hole wave functions localized in certain valleys from the wave functions of quantum confined electron/hole states obtained in atomistic calculations of nanostructures. The procedure is applied to the lead chalcogenide quantum dots to accurately extract the intravalley velocity matrix elements and the constants of the effective intravalley Hamiltonian of the exchange interaction for the ground exciton state in PbS and PbSe quantum dots. Our results suggest that intravalley parameters in PbS quantum dots are much more anisotropic than the ones in PbSe. Renormalization of the velocity matrix elements, forbidden band gap, valley and exchange splittings of exciton and exciton binding energy are also calculated.

Strain fingerprinting of exciton valley character in 2D semiconductors

Intervalley excitons with electron and hole wavefunctions residing in different valleys determine the long-range transport and dynamics observed in many semiconductors. However, these excitons with vanishing oscillator strength do not directly couple to light and, hence, remain largely unstudied. Here, we develop a simple nanomechanical technique to control the energy hierarchy of valleys via their contrasting response to mechanical strain. We use our technique to discover previously inaccessible intervalley excitons associated with K, Γ, or Q valleys in prototypical 2D semiconductors WSe2 and WS2. We also demonstrate a new brightening mechanism, rendering an otherwise “dark” intervalley exciton visible via strain-controlled hybridization with an intravalley exciton. Moreover, we classify various localized excitons from their distinct strain response and achieve large tuning of their energy. Overall, our valley engineering approach establishes a new way to identify intervalley excitons and control their interactions in a diverse class of 2D systems.

Metamorphic InGaAs/InAsPSb Quantum Well Light Emitting Diodes for Operation in the Short‐Wave Infrared Region

AbstractSolid‐state infrared sources designed to emit wavelengths above 2 µm often face challenges in achieving high emission efficiency, minimizing power consumption, and reducing fabrication costs. In response, a 2.4 µm wavelength light emitting diode (LED) is developed using metamorphic In0.83Ga0.17As/InAs0.3P0.65Sb0.05 multiple quantum well (MQW) heterostructures. The substantial conduction (94 meV) and valence band offsets (300 meV) within this type‐I MQW LED architecture result in strong carrier confinement, improving electron and hole wavefunction overlap. Despite a notable lattice mismatch of 2.0% between the MQWs and InP substrate, the resulting LED wafer exhibits exceptionally low surface roughness (1.1 nm) and well‐defined, sharp interfaces within the heterostructures. Furthermore, this MQW LED exhibits favorable emission properties, including a low turn‐on field, minimal efficiency droop, and stable emission wavelength across varying injection currents. These advancements underscore the potential of such short‐wave infrared emitters for scalable applications in fields such as inspection, optical on‐chip communication, and biomedical diagnostics.

Tunable superconductivity in electron- and hole-doped Bernal bilayer graphene.

Graphene-based, high-quality, two-dimensional electronic systems have emerged as a highly tunable platform for studying superconductivity1-21. Specifically, superconductivity has been observed in both electron- and hole-doped twisted graphene moiré systems1-17, whereas in crystalline graphene systems, superconductivity has so far been observed onlyin hole-doped rhombohedral trilayer graphene(RTG)18 and hole-doped Bernal bilayer graphene (BBG)19-21. Recently, enhanced superconductivity has been demonstrated20,21 in BBG because of the proximity to a monolayer WSe2. Here we report the observation of superconductivity and a series of flavour-symmetry-breaking phases in electron- and hole-doped BBG/WSe2 devices by electrostatic doping. The strength of the observed superconductivity is tunable by applied vertical electric fields. The maximum Berezinskii-Kosterlitz-Thouless transition temperature for the electron- and hole-doped superconductivity is about 210 mK and 400 mK, respectively. Superconductivities emerge only when the applied electric fields drive the BBG electron or hole wavefunctions towards the WSe2 layer, underscoring the importance of the WSe2 layer in the observed superconductivity. The hole-doped superconductivity violates the Pauli paramagnetic limit, consistent with an Ising-like superconductor. By contrast, the electron-doped superconductivity obeys the Pauli limit, although the proximity-induced Ising spin-orbit coupling is also notable in the conduction band. Our findings highlight the rich physics associated with the conduction band in BBG, paving the way for further studies into the superconducting mechanisms of crystalline graphene and the development of superconductor devices based on BBG.

Black hole wavefunctions and microcanonical states

We consider the problem of defining a microcanonical thermofield double state at fixed energy and angular momentum from the gravitational path integral. A semiclassical approximation to this state is obtained by imposing a mixed boundary condition on an initial time surface. We analyze the corresponding boundary value problem and gravitational action. The overlap of this state with the canonical thermofield double state, which is interpreted as the Hartle-Hawking wavefunction of an eternal black hole in a mini-superspace approximation, is calculated semiclassically. The relevant saddlepoint is a higher-dimensional, rotating generalization of the wedge geometry that has been studied in two-dimensional gravity. Along the way we discuss a new corner term in the gravitational action that arises at a rotating horizon.

Endothermic Charge Separation Occurs Spontaneously in Non-Fullerene Acceptor/Polymer Bulk Heterojunction.

Organic photovoltaics (OPVs) based on non-fullerene acceptors (NFAs) have achieved a power conversion efficiency close to 20%. These NFA OPVs can generate free carriers efficiently despite a very small energy level offset at the donor/acceptor interface. Why these NFAs can enable efficient charge separation (CS) with low energy losses remains an open question. Here, the CS process in the PM6:Y6 bulk heterojunction is probed by time-resolved two-photon photoemission spectroscopy. It is found that the CS, the conversion from bound charge transfer (CT) excitons to free carriers, is an endothermic process with an enthalpy barrier of 0.15eV. The CS can occur spontaneously despite being an endothermic process, which implies that it is driven by entropy. It is further argued that the morphology of the PM6:Y6 film and the anisotropic electron delocalization restrict the electron and hole wavefunctions within the CT exciton such that they can primarily contact each other through point-like junctions. This configuration can maximize the entropic driving force.

Gain Characteristics of Optically Pumped UVC Lasers with Wide AlGaN Single‐Quantum‐Well Active Regions

Herein, the lasing threshold and gain characteristics of ultraviolet‐C optically pumped edge‐emitting lasers with thick single‐quantum‐well (SQW) active regions are investigated by the variable‐stripe length method. Positive net modal gain is observed in lasers with AlGaN‐based SQWs with thicknesses up to 12 nm. The lasers show a reduction of the threshold power density with increasing SQW thickness, with the lowest threshold of 1.3 MW cm−2 achieved for a 9 nm SQW laser. The high gain and low threshold in lasers with thick quantum wells are attributed to lasing from excited states, where the polarization fields are screened by the carriers in the fundamental state and the barriers, thus recovering larger electron and hole wavefunctions overlap. These findings are supported by k · p simulations, and for a 9 nm SQW, the calculation predicts a contribution of the fundamental transition to the gain of 75% for non‐resonant optical excitation and below 1% for resonant optical or electrical excitation.

Removing Cadmium Impurities from Cation‐Exchange‐Derived CuInSe2/CuInS2 Nanorods for Enhanced Infrared Emission and Photodetection

AbstractMetal chalcogenide nanocrystals with variable composition and shape can conveniently be produced using cation exchange synthesis; however, the presence of cation‐containing ligands inherited from the starting material often results in contamination of the final product. To address this issue, a two‐step ligand replacement strategy is developed to fabricate CuInSe2/CuInS2 nanorods from CdSe/CdS nanorods via removal of Cd‐phosphonates from an intermediate Cu2‐xSe/Cu2‐xS phase used in the cation exchange conversion. This synthetic approach furnishes CuInSe2/CuInS2 nanorods with cadmium content below 1 at.%, and high photoluminescence quantum yields reaching 40% in the near‐infrared spectral range. Transient absorption studies reveal that the band alignment in the CuInSe2/CuInS2 heterostructure features a quasi‐type II character, with an electron localized in the core and a hole wavefunction spread over the entire nanorod. The efficient passivation of the core and the reduced Cd content leads to excitonic emission with full width at half maximum down to 110 meV, superimposed with a broad emission band from copper‐induced defects. Field‐effect transistors based on cadmium‐free CuInSe2/CuInS2 nanorods show two orders of magnitude lower noise current density compared with the cadmium‐rich devices. The responsivity and specific detectivity of these devices reach 230 mA W−1 and 108 Jones, respectively, under near‐infrared excitation at room temperature.

Silver‐Nanoclusters and Vacancies Influence the Optical Properties of Spherical Cs2AgBiCl6 Nanocrystals

AbstractHalide double perovskites (DPs), such as Cs2AgBiX6 (X = Br/Cl), are emerging semiconductors for optoelectronic applications, offering less toxic alternatives compared to lead halide perovskites. Although exhibiting an indirect bandgap, Cs2AgBiCl6 DP nanocrystals (NCs) show bright photoluminescence spectra characterized by a spectrally broad red emission centered ≈650 nm and a narrower blue emission band centered at 425 nm. However, the origin of both emission bands is still under debate. In this paper, it is shown that silver (Ag) plays a crucial role in the explanation of both emission bands observed in these DP NCs. The trapping of holes in Ag vacancies leads to a spatial localization of the hole wave function on the scale of the lattice constant. This provides k‐values for the hole wave function at all boundaries of the Brillouin zone and thus favors the recombination with electrons at the L‐point. Accordingly, a thermally activated behavior of the red photoluminescence with an activation energy of 56 meV is observed. It is further shown that the high‐energetic blue emission band originates from lecithin ligands attached to the NC surface. Surprisingly, their emission spectrum coincides exactly with the plasmon resonance of Ag nanoclusters, located on the surface of the DP NCs.

Molecular beam epitaxy of GaN/AlGaN quantum wells on bulk GaN substrate in the step-flow or step meandering regime: Influence on indirect exciton diffusion

GaN/AlxGa1−xN quantum wells were grown by molecular beam epitaxy on high quality bulk (0001) GaN substrates. The quantum well thickness was set in the 6–8 nm range to favor the photoluminescence emission of indirect excitons. Indeed, such excitons are known to be spatially indirect due to the presence of the internal electric field which spatially separates the electron and hole wave functions. The growth conditions were optimized in view of minimizing the photoluminescence peak broadening. In particular, the impact of growth temperature (up to 900 °C) on the surface morphology, structural, and photoluminescence properties was studied. The diffusion of indirect excitons on the scale of tens of micrometers was measured with a micro-photoluminescence setup equipped with a spatially resolved detection. A dedicated model and its analysis allow us to extract from these measurements the exciton diffusion constant and to conclude on the optimum growth conditions for the GaN/AlxGa1−xN quantum well structures suited for studies of quantum collective effects in indirect exciton liquids.

Temperature and pressure dependent tunable GaAsSb/InGaAs QW heterostructure for application in IR-photodetector

A temperature and pressure dependent tunable type-II DQW (double quantum well) heterostructure with the specific composition and combination of In0.1Ga0.9As, In0.55Ga0.45As and GaAs0.15Sb0.85 layers have been designed and analyzed for the purpose of designing the QW infrared photodetector. Using k.p. theory, the optical response for the optimized heterostructure is investigated as optical absorption. The electronic and hole wavefunctions, as well as the conduction and valence band E-K curves, are computed and examined using the k.p. technique. Furthermore, the dipole matrix elements are also computed in order to comprehend the optical absorption-causing transition process. The partial and total optical absorption are computed in the X- and Y-polarization modes for the proposed QW heterostructure. The maximal optical absorption was found to meet at two wavelengths, around 2700 and 3600 nm, under the X-polarization mode. The absorption peak is stronger and significantly greater at 2700 nm than it is at about 3600 nm. The maximal absorption in the Y-polarization mode meets between about 2550 and 3350 nm. To examine the tunability, the optical absorption spectra have also been studied with variable temperature (rang: 273K–350K) and pressure (range: 0–12 GPa). With increasing temperature and pressure, the absorption peaks have been found to enhance pointedly. It may be argued that the suggested QW heterostructure may be appropriate for developing QW photodetectors to detect radiation in the shortwave infrared (SWIR) area based on the findings of the simulations.

Theoretical Analysis of GeSn Quantum Dots for Photodetection Applications.

GeSn alloys have recently emerged as complementary metal-oxide-semiconductor (CMOS)-compatible materials for optoelectronic applications. Although various photonic devices based on GeSn thin films have been developed, low-dimensional GeSn quantum structures with improved efficiencies hold great promise for optoelectronic applications. This study theoretically analyses Ge-capped GeSn pyramid quantum dots (QDs) on Ge substrates to explore their potential for such applications. Theoretical models are presented to calculate the effects of the Sn content and the sizes of the GeSn QDs on the strain distributions caused by lattice mismatch, the band structures, transition energies, wavefunctions of confined electrons and holes, and transition probabilities. The bandgap energies of the GeSn QDs decrease with the increasing Sn content, leading to higher band offsets and improved carrier confinement, in addition to electron-hole wavefunction overlap. The GeSn QDs on the Ge substrate provide crucial type-I alignment, but with a limited band offset, thereby decreasing carrier confinement. However, the GeSn QDs on the Ge substrate show a direct bandgap at higher Sn compositions and exhibit a ground-state transition energy of ~0.8 eV, rendering this system suitable for applications in the telecommunication window (1550 nm). These results provide important insights into the practical feasibility of GeSn QD systems for optoelectronic applications.

Auger‐Assisted Secondary Hot Carrier Transfer in a Type I MoS2/PtSe2 Heterostructure

AbstractCharge transfer is vital in determining the optoelectronic properties of atomically thin materials, yet remains elusive in type I heterostructures. Here, distinct two‐step charge transfer processes in a type I MoS2/PtSe2 heterostructure are reported. By exclusively exciting the smaller bandgap PtSe2, strong exciton photobleaching peaks of the larger bandgap MoS2 are observed, indicating primary hot carrier transfer from PtSe2 to MoS2 within 70 fs. More importantly, the amplitude of the exciton peaks shows a secondary increase after the initial rapid decay. These dynamics are distinctly different from the monotonic decrease in monolayer MoS2 and indicate a secondary charge transfer process that is attributed to hot carriers re‐generated in PtSe2 by intralayer Auger recombination. Concurrently, the exciton energy blue shifts within 100 ps, probing the dynamic buildup of a charge‐transfer induced electric field across the heterostructure interface, which displaces electron and hole wavefunctions of MoS2 excitons and reduces the exciton binding energy. The results are corroborated by carrier dynamics and transient absorption spectra simulations by considering the two‐step charge transfer processes. The work reveals Auger‐assisted hot carrier transfer processes in type I heterostructures and suggests the possibility for optoelectronic and photocatalytic applications by optical sub‐bandgap excitation.

Mapping charge excitations in generalized Wigner crystals.

Transition metal dichalcogenide-based moiré superlattices exhibit strong electron-electron correlations, thus giving rise to strongly correlated quantum phenomena such as generalized Wigner crystal states. Evidence of Wigner crystals in transition metal dichalcogenide moire superlattices has been widely reported from various optical spectroscopy and electrical conductivity measurements, while their microscopic nature has been limited to the basic lattice structure. Theoretical studies predict that unusual quasiparticle excitations across the correlated gap between upper and lower Hubbard bands can arise due to long-range Coulomb interactions in generalized Wigner crystal states. However, the microscopic proof of such quasiparticle excitations is challenging because of the low excitation energy of the Wigner crystal. Here we describe a scanning single-electron charging spectroscopy technique with nanometre spatial resolution and single-electron charge resolution that enables us to directly image electron and hole wavefunctions and to determine the thermodynamic gap of generalized Wigner crystal states in twisted WS2 moiré heterostructures. High-resolution scanning single-electron charging spectroscopy combines scanning tunnelling microscopy with a monolayer graphene sensing layer, thus enabling the generation of individual electron and hole quasiparticles in generalized Wigner crystals. We show that electron and hole quasiparticles have complementary wavefunction distributions and that thermodynamic gaps of ∼50 meV exist for the 1/3 and 2/3 generalized Wigner crystal states in twisted WS2.

Dielectric and Wavefunction Engineering of Electron Spin Lifetime in Colloidal Nanoplatelet Heterostructures.

Colloidal semiconductor nanoplatelets (NPLs) have emerged as low-cost and free-standing alternates of traditional quantum wells. The giant heavy- and light-hole splitting in NPLs allows for efficient optical spin injection. However, the electron spin lifetimes for prototypical CdSe NPLs are within a few picoseconds, likely limited by strong electron-hole exchange in these quantum- and dielectric-confined materials. Here how this hurdle can be overcome with engineered NPL-heterostructures is demonstrated. By constructing type-I CdSe/ZnS core/shell NPLs, dielectric screening inside the core is strongly enhanced, prolonging the electron spin polarization time (τesp) to over 30ps (or 60ps electron spin-flip time). Alternatively, by growing type-II CdSe/CdTe core/crown NPLs to spatially separate electron and hole wavefunctions, the electron-hole exchange is strongly suppressed, resulting in τesp as long as 300ps at room temperature. This study not only exemplifies how the well-established synthetic chemistry of colloidal heterostructures can aid in spin dynamics control but also establishes the feasibility of room-temperature coherent spin manipulation in colloidal NPLs.

Design of AlGaN-Zn(Si,Ge)N2 quantum wells for high-efficiency ultraviolet light emitters

The effect of inserting a nm-scale layer of Zn(Si,Ge)N2 into an AlGaN quantum well structure designed for light emission in the wavelength range from 255 to 305 nm is investigated here. The enhanced confinement of the hole within the quantum well results in an enhancement of the overlap of the hole and electron wave functions, resulting in an enhancement of the radiative recombination rate. In this theoretical calculation, for emission at a 270 nm wavelength, the enhancement in the wavefunction overlap can reach a factor of 7 when compared to an AlGaN quantum well device specifically engineered for optimal emission at the identical wavelength. Increases of almost an order of magnitude in both the peak spontaneous emission intensity and the radiative recombination rate are predicted. The peak emission wavelength can be tuned from 255 to 305 nm by adjusting the width and/or the composition of the inserted layer. The proposed structures provide a route to higher efficiency ultraviolet practical light emitting diodes and lasers.

Spin relaxation of electron and hole polarons in ambipolar conjugated polymers

The charge-transport properties of conjugated polymers have been studied extensively for opto-electronic device applications. Some polymer semiconductors not only support the ambipolar transport of electrons and holes, but do so with comparable carrier mobilities. This opens the possibility of gaining deeper insight into the charge-transport physics of these complex materials via comparison between electron and hole dynamics while keeping other factors, such as polymer microstructure, equal. Here, we use field-induced electron spin resonance spectroscopy to compare the spin relaxation behavior of electron and hole polarons in three ambipolar conjugated polymers. Our experiments show unique relaxation regimes as a function of temperature for electrons and holes, whereby at lower temperatures electrons relax slower than holes, but at higher temperatures, in the so-called spin-shuttling regime, the trend is reversed. On the basis of theoretical simulations, we attribute this to differences in the delocalization of electron and hole wavefunctions and show that spin relaxation in the spin shuttling regimes provides a sensitive probe of the intimate coupling between charge and structural dynamics.

Strain modulation effect of superlattice interlayer on InGaN/GaN multiple quantum well

The strong piezoelectric field in InGaN/GaN heterostructure quantum wells severely reduces the light emission efficiency of multiple quantum well (MQW) structures. To address this issue, a strain modulation interlayer is commonly used to mitigate the piezoelectric polarization field and improve the luminescence performance of the devices. To investigate the influence and mechanism of strain modulation in the InGaN/GaN superlattice (SL), epitaxial wafers with an n-type InGaN/GaN SL interlayer sample, and their corresponding control samples are prepared. The measured temperature-dependent photoluminescence (PL) spectra of the epitaxial wafers, show that the introduction of an SL interlayer leads to a shorter-wavelength emission and enhancement of internal quantum efficiency. As the temperature increases, a blue shift of the PL peak is observed. However, for the sample with an SL interlayer, the blue shift of the PL peak with temperature increasing is relatively small. Electroluminescence (EL) experiments indicate that the introduction of an SL interlayer significantly increases the integrated intensity of the EL peak and reduces its full width at half maximum. These phenomena collectively indicate that the incorporation of a superlattice interlayer can partly suppress the quantum-confined Stark effect (QCSE) that affects the light emission efficiency. Theoretical calculations show that the introduction of a superlattice strain layer before growing an active multiple quantum well can weaken the polarization-induced built-in electric field in the active quantum well, reduce the tilt of the energy band in the multiple quantum well active region, increase the overlap of electron and hole wave functions, enhance the emission probability, shorten the radiative recombination lifetime, and promote competition between radiative recombination and non-radiative recombination, thereby achieving higher recombination efficiency and improving light emission intensity. This study provides experimental and theoretical evidence that the strain modulation SL interlayer can effectively improve the device performance and offer guidance for optimizing the structural design of devices.

Study of Nano-Hetrostructure of Type-Ii Compound Semiconductors:Their Electronic and Hole Wave Function Action in Mid Infrared Region

Study of Nano-Hetrostructure of Type-Ii Compound Semiconductors:Their Electronic and Hole Wave Function Action in Mid Infrared Region

Ab Initio Quantum Dynamics Simulation of the Impact of Graphene on the Carrier Lifetime of the ZnV2O6 Photocatalyst.

We used a nonadiabatic molecular dynamics simulation to determine the carrier dynamics of a graphene/ZnV2O6 heterostructure in the search for an effective photocatalyst material. The C-2p orbital promotes the wave function overlap, guiding electrons to move between graphene and ZnV2O6, successfully achieving good mixing with the valence and conduction bands in ZnV2O6 materials, which is conducive to supporting carrier migration. The overlap between graphene/ZnV2O6 electrons and hole wave functions is less than that of ZnV2O6, and there is small absolute nonadiabatic coupling. The charge separation caused by graphene increases the carrier lifetime and prevents nonradiative electron-hole recombination. This study reveals the microscopic mechanism of extending the carrier lifetime of ZnV2O6 by introducing graphene, providing useful insights for regulating the electronic structure, promoting electron transfer and ultrafast electron and hole transfer. This strategy provides design considerations for advanced photocatalytic materials.