Effect of electron-electron interaction on polarization process of exciton and biexciton in conjugated polymer

By using one-dimensional tight-binding model modified to include electron-electric field interaction and electron-electron interaction,we theoretically explore the polarization process of exciton and biexciton in cis-polyacetylene.The dynamical simulation is performed by adopting the non-adiabatic evolution approach.The results show that under the effect of moderate electric field,when the strength of electron-electron interaction is weak,the singlet exciton is stable but its polarization presents obvious oscillation.With the enhancement of interaction,it is dissociated into polaron pairs,the spin-flip of which can be observed through modulating the interaction strength.For the triplet exciton,the strong electron-electron interaction restrains its normal polarization,but it is still stable.In the case of biexciton,the strong electron-electron interaction not only dissociate it,but also flip its charge distribution.The yield of the possible states formed after the dissociation of exciton and biexciton is also calculated.

Efficient energy transfer from self-trapped excitons to Mn^(2+) dopants in CsCdCl_(3):Mn^(2+) perovskite nanocrystals

Mn^(2+)doping has been adopted as an efficient approach to regulating the luminescence properties of halide perovskite nano-crystals(NCs).However,it is still difficult to understand the interplay of Mn^(2+)luminescence and the matrix self-trapped exciton(STE)emission therein.In this study,Mn^(2+)-doped CsCdCl_(3) NCs are prepared by hot injection,in which CsCdCl_(3) is selected because of its unique crystal structure suitable for STE emission.The blue emission at 441 nm of undoped CsCdCl_(3) NCs originates from the defect states in the NCs.Mn^(2+)doping promotes lattice distortion of CsCdCl_(3) and generates bright orange-red light emission at 656 nm.The en-ergy transfer from the STEs of CsCdCl_(3) to the excited levels of the Mn^(2+)ion is confirmed to be a significant factor in achieving efficient luminescence in CsCdCl_(3):Mn^(2+)NCs.This work highlights the crucial role of energy transfer from STEs to Mn^(2+)dopants in Mn^(2+)-doped halide NCs and lays the groundwork for modifying the luminescence of other metal halide perovskite NCs.

Strain tunable excitonic optical properties in monolayer Ga_(2)O_(3)

Two-dimensional(2D)Ga_(2)O_(3)has been confirmed to be a stable structure with five atomic layer thickness configuration.In this work,we study the quasi-particle electronic band structures and then access the excitonic optical properties through solving the Bethe-Salpeter equation(BSE).The results reveal that the exciton dominates the optical absorption in the visible light region with the binding energy as large as~1.0 eV,which is highly stable at room temperature.Importantly,both the dominant absorption P_(1)and P_(2)peaks are optically bright without dark exciton between them,and thus is favorable for luminescence process.The calculated radiative lifetime of the lowest-energy exciton is 2.0×10^(-11)s at 0 K.Furthermore,the radiative lifetime under+4%tensile strain is one order of magnitude shorter than that of the strainfree case,while it is less insensitive under the compressive strain.Our findings set the stage for future theoretical and experimental investigation on monolayer Ga_(2)O_(3).

Excitonic optical properties in monolayer SnP_(2)S_(6)

Quantum confinement effect and reduced dielectric screening in two-dimensional(2D)dramatically enhance theelectron-hole interactions.In this work,we use many-body perturbation theory and Bethe-Salpeter equation(BSE)toinvestigate the electronic and excitonic optical properties of monolayer SnP_(2)S_(6).Our findings reveal that the excitoniceffect dominates the optical absorption spectra in the visible light range,and the lowest-energy exciton X0 in monolayerSnP_(2)S_(6)is optically bright with the binding energy of 0.87 eV and the radiative lifetime of~10^(-11)s,which is highly advantageousto the photo-luminescence.Most importantly,the absence of optically forbidden states below the bright statesX0 would give rise to a high quantum efficiency of 2D SnP_(2)S_(6).We also find that applied biaxial strain can further shortenthe radiative lifetime of the bright states.These results imply that 2D SnP_(2)S_(6)is a promising candidate for the optoelectronicdevices.

Behavior of exciton in direct−indirect band gap Al_(x)Ga_(1−x)As crystal lattice quantum wells

Excitons have significant impacts on the properties of semiconductors.They exhibit significantly different properties when a direct semiconductor turns in to an indirect one by doping.Huybrecht variational method is also found to influence the study of exciton ground state energy and ground state binding energy in Al_(x)Ga_(1−x)As semiconductor spherical quantum dots.The Al_(x)Ga_(1−x)As is considered to be a direct semiconductor at AI concentration below 0.45,and an indirect one at the concentration above 0.45.With regards to the former,the ground state binding energy increases and decreases with AI concentration and eigenfrequency,respectively;however,while the ground state energy increases with AI concentration,it is marginally influenced by eigenfrequency.On the other hand,considering the latter,while the ground state binding energy increases with AI concentration,it decreases with eigenfrequency;nevertheless,the ground state energy increases both with AI concentration and eigenfrequency.Hence,for the better practical performance of the semiconductors,the properties of the excitons are suggested to vary by adjusting AI concentration and eigenfrequency.

Interaction of moiréexcitons with cavity photons in two-dimensional semiconductor hetero-bilayers

Moirématerials,composed of two single-layer two-dimensional semiconductors,are important because they are good platforms for studying strongly correlated physics.Among them,moirématerials based on transition metal dichalcogenides(TMDs)have been intensively studied.The hetero-bilayer can support moiréinterlayer excitons if there is a small twist angle or small lattice constant difference between the TMDs in the hetero-bilayer and form a type-Ⅱ band alignment.The coupling of moiréinterlayer excitons to cavity modes can induce exotic phenomena.Here,we review recent advances in the coupling of moiréinterlayer excitons to cavities,and comment on the current difficulties and possible future research directions in this field.

Melting of electronic/excitonic crystals in 2D semiconductor moirépatterns:A perspective from the Lindemann criterion

Using the Lindemann criterion,we analyzed the quantum and thermal melting of electronic/excitonic crystals recently discovered in two-dimensional(2D)semiconductor moirépatterns.We show that the finite 2D screening of the atomically thin material can suppress(enhance)the inter-site Coulomb(dipolar)interaction strength,thus inhibits(facilitates)the formation of the electronic(excitonic)crystal.Meanwhile,a strong enough moiréconfinement is found to be essential for realizing the crystal phase with a wavelength near 10 nm or shorter.From the calculated Lindemann ratio which quantifies the fluctuation of the site displacement,we estimate that the crystal will melt into a liquid above a critical temperature ranging from several tens Kelvin to above 100 K(depending on the system parameters).

Thickness-dependent exciton relaxation dynamics of few-layer rhenium diselenide

Rhenium diselenide(ReSe_(2))has gathered much attention due to its low symmetry of lattice structure,which makes it possess in-plane anisotropic optical,electrical as well as excitonic properties and further enables ReSe_(2)have an important application in optoelectronic devices.Here,we report the thickness-dependent exciton relaxation dynamics of mechanically exfoliated few-layer ReSe_(2)flakes by using time-resolved pump–probe transient transmission spectroscopies.The results reveal two thickness-dependent relaxation processes of the excitons.The fast one correlates with the exciton formation(i.e.,the conversion of hot carriers to excitons),while the slow one is attributed to the exciton recombination dominated by defect-assisted exciton trapping besides photon emission channel.The decrease of scattering probability caused by defects leads to the increase of fast lifetime with thickness,and the increase of slow lifetime with thickness is related to the trap-mediated exciton depopulation induced by surface defects.Polarization-dependent transient spectroscopy indicates the isotropic exciton dynamics in the two-dimensional(2D)plane.These results are insightful for better understanding of excitonic dynamics of ReSe_(2)materials and its application in future optoelectronic and electronic devices.

Efficient transfer of metallophosphor excitons via confined polaritons in organic nanocrystals

We investigate the transfer of phosphorescent energy between co-assembled metallophosphors in crystalline nanostructures [Angew. Chem. Int. Ed. 57 7820(2018) and J. Am. Chem. Soc. 140 4269(2018)]. Neither Dexter's nor Forster's mechanism of resonance energy transfer(RET) could account fully for the observed rates, which exceed 85% with significant temperature dependence. But there exists an alternative pathway on RET mediated by intermediate states of resonantly confined exciton–polaritons. Such a mechanism was used to analyze artificial photosynthesis in organic fluorescents [Phys.Rev. Lett. 122 257402(2019)]. For metallophosphors, the confined modes act as extended states lying between the molecular S_(1) and T_(1) states, offering a bridge for the long-lived T_(1) excitons to migrate from donors to acceptors. Population dynamics with parameters taken entirely based on experiments fits the observed lifetimes of phosphorescence across a broad range of doping and temperature.

Exciton radiative lifetime in CdSe quantum dots

Colloidal CdSe quantum dots(QDs)are promising materials for solar cells because of their simple preparation pro-cess and compatibility with flexible substrates.The QD radiative recombination lifetime has attracted enormous attention as it affects the probability of photogenerated charges leaving the QDs and being collected at the battery electrodes.However,the scaling law for the exciton radiative lifetime in CdSe QDs is still a puzzle.This article presents a novel explanation that recon-ciles this controversy.Our calculations agree with the experimental measurements of all three divergent trends in a broadened energy window.Further,we proved that the exciton radiative lifetime is a consequence of the thermal average of decays for all thermally accessible exciton states.Each of the contradictory size-dependent patterns reflects this trend in a specific size range.As the optical band gap increases,the radiative lifetime decreases in larger QDs,increases in smaller QDs,and is weakly depend-ent on size in the intermediate energy region.This study addresses the inconsistencies in the scaling law of the exciton life-time and gives a unified interpretation over a widened framework.Moreover,it provides valuable guidance for carrier separa-tion in the thin film solar cell of CdSe QDs.

The Role of Radiative Surface Modes and Longitudinal Excitons in the Formation of Exciton-Polariton Luminescence Spectra of CdS-Type Crystals

The low-temperature (T = 2 K) exciton-polariton luminescence (EPL) spectra in the vicinity of the exciton-resonance frequency An=1 for CdS-type crystals have been theoretically and experimentally investigated with allowance for the mechanical exciton decay . The results of the numerical calculations of the partial and interference contributions of the bulk and radiative surface spectral modes to the EPL in the geometry of additional s- and p-polarized waves emitted into vacuum are analyzed. It is shown that the contributions of purely longitudinal excitons and their interference with polaritons of the upper dispersion branch near the longitudinal frequency ωL to the EPL are small (∼10% - 30%);nevertheless, they must be taken into account to obtain quantitative agreement with experimental data. Specifically these contributions are responsible for the formation of an additional line (along with the fundamental AT line) in the case of oblique incidence of radiation.

Binding Energies of Screened Excitons in a Strained(111)-Oriented Zinc-Blende GaN/AlGaN Quantum Well Under Hydrostatic Pressure

We investigate the binding energies of excitons in a strained （111）-oriented zinc-blende GaN/Al0.3 Ga0.7 N quantum well screened by the electron-hole （e-h） gas under hydrostatic pressure by combining a variational method and a selfconsistent procedure. A built-in electric field produced by the strain-induced piezoelectric polarization is considered in our calculations. The result indicates that the binding energies of excitons increase nearly linearly with pressure,even though the modification of strain with hydrostatic pressure is considered, and the influence of pressure is more apparent under higher e-h densities. It is also found that as the density of an e-h gas increases,the binding energies first increase slowly to a maximum and then decrease rapidly when the e-h density is larger than about 1 ×10^11 cm^-2. The excitonic binding energies increase obviously as the barrier thickness decreases due to the decrease of the built-in electric field.

Exciton optical absorption in asymmetric ZnO/ZnMgO double quantum wells with mixed phases

The optical absorption of exciton interstate transition in Zn1-xlMgxlO/ZnO/Zn1-xcMgxcO/ZnO/Zn1-xrMgxrO asymmetric double quantum wells(ADQWs)with mixed phases of zinc-blende and wurtzite in Zn1-xMgxO for 0.37<x<0.62 is discussed.The mixed phases are taken into account by our weight model of fitting.The states of excitons are obtained by a finite difference method and a variational procedure in consideration of built-in electric fields(BEFs)and the Hartree potential.The optical absorption coefficients(OACs)of exciton interstate transition are obtained by the density matrix method.The results show that Hartree potential bends the conduction and valence bands,whereas a BEF tilts the bands and the combined effect enforces electrons and holes to approach the opposite interfaces to decrease the Coulomb interaction effects between electrons and holes.Furthermore,the OACs indicate a transformation between direct and indirect excitons in zinc-blende ADQWs due to the quantum confinement effects.There are two kinds of peaks corresponding to wurtzite and zinc-blende structures respectively,and the OACs merge together under some special conditions.The computed result of exciton interband emission energy agrees well with a previous experiment.Our conclusions are helpful for further relative theoretical studies,experiments,and design of devices consisting of these quantum well structures.

Impact of Structural Disorder on Excitonic Behaviors and Dynamics in 2D Organic-Inorganic Hybrid Perovskites

Two thin-film 2 D organic-inorganic hybrid perovskites,i.e.,2-phenylethylammonium lead iodide(PEPI)and 4-phenyl-1-butylammonium lead iodide(PBPI)were synthesized and investigated by steady-state absorption,temperature-dependent photoluminescence,and temperature-dependent ultrafast transient absorption spectroscopy.PBPI has a longer organic chain(via introducing extra ethyl groups)than PEPI,thus its inorganic skeleton can be distorted,bringing on structural disorder.The comparative analyses of spectral profiles and temporal dynamics revealed that the greater structural disorder in PBPI results in more defect states serving as trap states to promote exciton dynamics.In addition,the fine-structuring of excitonic resonances was unveiled by temperature-dependent ultrafast spectroscopy,suggesting its correlation with inorganic skeleton rather than organic chain.Moreover,the photoexcited coherent phonons were observed in both PEPI and PBPI,pointing to a subtle impact of structural disorder on the low-frequency Raman-active vibrations of inorganic skeleton.This work provides valuable insights into the optical properties,excitonic behaviors and dynamics,as well as coherent phonon effects in 2 D hybrid perovskites.

Exciton luminescence and many-body effect of monolayer WS2 at room temperature

Monolayer transition metal dichalcogenides favor the formation of a variety of excitonic quasiparticles,and can serve as an ideal material for exploring room-temperature many-body effects in two-dimensional systems.Here,using mechanically exfoliated monolayer WS;and photoluminescence(PL)spectroscopy,exciton emission peaks are confirmed through temperature-dependent and electric-field-tuned PL spectroscopy.The dependence of exciton concentration on the excitation power density at room temperature is quantitatively analyzed.Exciton concentrations covering four orders of magnitude are divided into three stages.Within the low carrier concentration stage,the system is dominated by excitons,with a small fraction of trions and localized excitons.At the high carrier concentration stage,the localized exciton emission from defects coincides with the emission peak position of trions,resulting in broad spectral characteristics at room temperature.

Long-lived Single Excitons, Trions, and Biexcitons in CdSe/CdTe Type-II Colloidal Quantum Wells

Light-harvesters with long-lived excited states are desired for efficient solar energy conversion systems. Many solar-to-fuel conversion reactions, such as H2 evolution and CO2 reduction, require multiple sequential electron transfer processes, which leads to a complicated situation that excited states involves not only excitons （electron-hole pairs） but also multi-excitons and charged excitons. While long-lived excitons can be obtained in various systems （e.g., semiconductor nanocrystals）, multi-excitons and charged excitons are typically shorted-lived due to nonradiative Auger recombination pathways whereby the recombination energy of an exciton is quickly transferred to the third carrier on a few to hundreds of picoseconds timescale. In this work, we report a study of excitons, trions （an exciton plus an additional charge）, and biexcitons in CdSe/CdTe colloidal quantum wells or nanoplatelets. The type- II band alignment effectively separates electrons and holes in space, leading to a single exciton lifetime of 340 ns which is -2 order of magnitudes longer than that in plane CdSe nanoplatelets. More importantly, the electron-hole separation also dramatically slows down Auger decay, giving rise to a trion lifetime of 70 ns and a biexciton lifetime of 11 ns, among the longest values ever reported for colloidal nanocrystals. The long-lived exciton, trion, and biexciton states, combined with the intrinsically strong light-absorption capability of two-dimensional systems, enable the CdSe/CdTe type-II nanoplatelets as promising light harvesters for efficient solar-to-fuel conversion reactions.

Phase control of group-velocity-based biexciton coherence in a multiple quantum well nanostructure

A double cascade-type four-level multiple-quantum-well-based exciton-biexciton transitions are proposed. The study is carried out on a 4.8-rim ZnSe single-quantum well which is embedded into ZnMgSSe cladding layers and pseudomor- phically grown by molecular beam epitaxy on a （0 0 1） GaAs substrate. It is displayed that the exciton spin relaxation and relative phases between applied fields can influence the transient and steady-state behaviors of absorption, dispersion, and group velocity of two weak probe and signal fields. Also, transient behaviors of electron population of different levels are discussed. It is found that the probe or signal amplification occurs in the absence of population inversion.

Exciton Condensation and Superfluidity in TmSe_0.45Te_0.55

In this publication details of the calculation of heat conductivity and thermal diffusivity, compressibility, sound velocity and exciton-polaron dispersion of TmSe0.45Te0.55 will be shown. The properties of excitons, coupling to phonons, producing thus polarons, but also blocking the phonons as running waves lead to an exciton condensation or exciton liquid. Surprisingly this exciton liquid is contained in a macroscopic crystal, a solid nevertheless, which becomes extremely hard due to the exciton liquid and finally exhibits a strange type of superfluid in a two fluid model, where the superfluid phase increases more and more below about 20 K until the whole exciton liquid becomes a superfluid at zero temperature. Never else a superfluid phase has been observed at such high temperatures.

Investigation of Dynamical Parameters of Exciton Confined in CdS Spherical Quantum Dots with a B—Spline Technique

Exciton energies as a function of radii of quantum dots in the range of 5–35 ? are calculated based on effective mass approximation model with the B-spline technique and compared with experimental and other theoretical data for the CdS dots. This method leads to accurate and fast convergent exciton energy, which are in good agreement with experimental data in the whole confinement regime. The effect of penetration of wave function from the inside to the outside of the dots and the effect of dielectric constants are taken into account. The magnitudes of dynamical parameters are discussed. It is found that the different materials surrounding the CdS quantum dot affect not only the potential energy and Coulomb interaction energy of the system, but also the effective masses. The comparison shows that the effective mass approximation model can describe very well the quantum size effects observed experimentally on the exciton ground state energy.

Light-emitting diodes based on all-inorganic copper halide perovskite with self-trapped excitons

Light-emitting diodes based on lead halide perovskite have attracted great attention due to their outstanding performance.However,their application is plagued by the toxicity of Pb and the poor stability.Herein novel copper-based all inorganic perovskite CsCu2I3 with much enhanced stability has been reported with a potential photoluminescence quantum yield(PLQY)over 20%and self-trapped excitons(STE).By taking advantage of its extraordinary thermal stability,we successfully fabricate high-quality CsCu2I3 film through direct vacuum-based deposition(VBD)of CsCu2I3 powder.The resulting film shows almost the same PLQY with the synthesized powder,as well as excellent uniformity and stability.The perovskite light-emitting diodes(Pe-LED)based on the evaporated CsCu2I3 emitting layer achieve a luminescence of 10 cd/m2 and an external quantum efficiency(EQE)of 0.02%.To the best of our knowledge,this is the first CsCu2I3 Pe-LED fabricated by VBD with STE property,which offers a new avenue for lead-free Pe-LED.