Exciton binding energy(E_(b))has been regarded as a critical parameter in charge separation during photovoltaic conversion.Minimizing the E_(b) of the photovoltaic materials can facilitate the exciton dissociation in ...Exciton binding energy(E_(b))has been regarded as a critical parameter in charge separation during photovoltaic conversion.Minimizing the E_(b) of the photovoltaic materials can facilitate the exciton dissociation in low-driving force organic solar cells(OSCs)and thus improve the power conversion efficiency(PCE);nevertheless,diminishing the E_(b) with deliberate design principles remains a significant challenge.Herein,bulky side chain as steric hindrance structure was inserted into Y-series acceptors to minimize the E_(b) by modulating the intra-and intermolecular interaction.Theoretical and experimental results indicate that steric hindrance-induced optimal intra-and intermolecular interaction can enhance molecular polarizability,promote electronic orbital overlap between molecules,and facilitate delocalized charge trans-fer pathways,thereby resulting in a low E_(b).The conspicuously reduced E_(b) obtained in Y-ChC5 with pinpoint steric hindrance modulation can minimize the detrimental effects on exciton dissociation in low-driving-force OSCs,achieving a remarkable PCE of 19.1%with over 95%internal quantum efficiency.Our study provides a new molecular design rationale to reduce the E_(b).展开更多
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-...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.展开更多
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+)luminescenc...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.展开更多
Ternary metal halides based on Cu(I)and Ag(I)have attracted intensive attention in optoelectronic applications due to their excellent luminescent properties,low toxicity,and robust stability.While the self-trapped exc...Ternary metal halides based on Cu(I)and Ag(I)have attracted intensive attention in optoelectronic applications due to their excellent luminescent properties,low toxicity,and robust stability.While the self-trapped excitons(STEs)emission mechanisms of Cu(I)halides are well understood,the STEs in Ag(I)halides remain less thoroughly explored.This study explores the STE emission efficiency within the A_(2)AgX_(3)(A=Rb,Cs;X=Cl,Br,I)system by identifying three distinct STE states in each material and calculating their configuration coordinate diagrams.We find that the STE emission efficiency in this system is mainly determined by STE stability and influenced by self-trapping and quenching barriers.Moreover,we investigate the impact of structural compactness on emission efficiency and find that the excessive electron–phonon coupling in this system can be reduced by increasing the structural compactness.The atomic packing factor is identified as a low-cost and effective descriptor for predicting STE emission efficiency in both Cs_(2)AgX_(3) and Rb_(2)AgX_(3) systems.These findings can deepen our understanding of STE behavior in metal halide materials and offer valuable insights for the design of efficient STE luminescent materials.The datasets presented in this paper are openly available in Science Data Bank at https://doi.org/10.57760/sciencedb.12094.展开更多
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 excitoni...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).展开更多
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)to...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.展开更多
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 a...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.展开更多
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...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.展开更多
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 screenin...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).展开更多
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 R...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.展开更多
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...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.展开更多
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 eno...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.展开更多
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 all...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.展开更多
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...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.展开更多
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<...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.展开更多
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...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.展开更多
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.He...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.展开更多
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 e...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.展开更多
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 an...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.展开更多
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, ...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.展开更多
基金National Natural Science Foundation of China,Grant/Award Numbers:52203225,52073122,22375077,22008184Key R&D Project of Hubei Province,Grant/Award Number:2022BAA095+3 种基金Hubei Natural Science Foundation,Grant/Award Number:2022CFB903Special Project from Jianghan University,Grant/Award Number:2022XKZX02Ministry of Science and Technology of China,Grant/Award Number:2021YFE0113600Excellent Discipline Cultivation Project by JHUN,Grant/Award Numbers:2023XKZ010,2023XKZ014。
文摘Exciton binding energy(E_(b))has been regarded as a critical parameter in charge separation during photovoltaic conversion.Minimizing the E_(b) of the photovoltaic materials can facilitate the exciton dissociation in low-driving force organic solar cells(OSCs)and thus improve the power conversion efficiency(PCE);nevertheless,diminishing the E_(b) with deliberate design principles remains a significant challenge.Herein,bulky side chain as steric hindrance structure was inserted into Y-series acceptors to minimize the E_(b) by modulating the intra-and intermolecular interaction.Theoretical and experimental results indicate that steric hindrance-induced optimal intra-and intermolecular interaction can enhance molecular polarizability,promote electronic orbital overlap between molecules,and facilitate delocalized charge trans-fer pathways,thereby resulting in a low E_(b).The conspicuously reduced E_(b) obtained in Y-ChC5 with pinpoint steric hindrance modulation can minimize the detrimental effects on exciton dissociation in low-driving-force OSCs,achieving a remarkable PCE of 19.1%with over 95%internal quantum efficiency.Our study provides a new molecular design rationale to reduce the E_(b).
基金Project supported by the Natural Science Foundation of Shandong Province,China(Grant No.ZR2020MA070).
文摘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.
基金supported by the Guangdong Provincial Science&Technology Project(No.2023A0505050084)the National Natural Science Foundation of China(No.22361132525)+1 种基金the Fundamental Research Funds for the Central Universities(No.2023ZYGXZR002)the Local Innovative and Research Teams Project of Guangdong Pearl River Talents Program(No.2017BT01X137).
文摘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.
基金Project supported by the National Natural Science Foundation of China(Grant Nos.62125402 and 62321166653).
文摘Ternary metal halides based on Cu(I)and Ag(I)have attracted intensive attention in optoelectronic applications due to their excellent luminescent properties,low toxicity,and robust stability.While the self-trapped excitons(STEs)emission mechanisms of Cu(I)halides are well understood,the STEs in Ag(I)halides remain less thoroughly explored.This study explores the STE emission efficiency within the A_(2)AgX_(3)(A=Rb,Cs;X=Cl,Br,I)system by identifying three distinct STE states in each material and calculating their configuration coordinate diagrams.We find that the STE emission efficiency in this system is mainly determined by STE stability and influenced by self-trapping and quenching barriers.Moreover,we investigate the impact of structural compactness on emission efficiency and find that the excessive electron–phonon coupling in this system can be reduced by increasing the structural compactness.The atomic packing factor is identified as a low-cost and effective descriptor for predicting STE emission efficiency in both Cs_(2)AgX_(3) and Rb_(2)AgX_(3) systems.These findings can deepen our understanding of STE behavior in metal halide materials and offer valuable insights for the design of efficient STE luminescent materials.The datasets presented in this paper are openly available in Science Data Bank at https://doi.org/10.57760/sciencedb.12094.
基金supported by the National Natural Science Foundation of China(Grant No.12064032).
文摘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).
基金support by the National Natural Science Foundation of China(Grant No.12064032).
文摘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.
基金supported by the National Natural Science Foundation of China(Nos.12164032 and 11964026)the Natural Science Foundation of Inner Mongolia(No.2019MS01010)+3 种基金Scientific Research Projects in Colleges and Universities in Inner Mongolia(No.NJZZ19145)Graduate Science Innovative Research Projects(No.S20210281Z)the Natural Science Foundation of Inner Mongolia(No.2022MS01014)Doctor Research Start-up Fund of Inner Mongolia Minzu University(No.BS625).
文摘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.
基金supported by the National Key R&D Program of China(Grant No.2018YFA036900)the Beijing Natural Science Foundation(Grant No.JQ21018)。
文摘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.
基金support by the National Natural Science Foundation of China(Grant No.12274477)the Department of Science and Technology of Guangdong Province of China(Grant No.2019QN01X061)。
文摘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).
基金Project supported by the National Natural Science Foundation of China(Grant Nos.12074202,12174207,and 11974190)the Natural Science Foundation of Tianjin City(Grant Nos.20JCQNJC00020 and 22JCYBJC00390)。
文摘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.
基金Project supported by the National Natural Science Foundation of China (Grant No. 16Z103060007) (PA)。
文摘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.
基金supported by the National Key Research and Development Program of China under Grant No.2021YFB2800304.
文摘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.
文摘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.
文摘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.
基金Project supported by the National Natural Science Foundation of China(Grant No.61764012).
文摘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.
基金supported by the National Key Research and Development Program on Nano Science and Technology of the Ministry of Science and Technology of China(No.2016YFA0200602 and No.2018YFA0208702)the National Natural Science Foundation of China(No.21573211 and No.21633007)the Anhui Initiative in Quantum Information Technologies(No.AHY090200)。
文摘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.
基金Project supported by the National Natural Science Foundation of China(Grant Nos.61635001,52072117,and 51972105)。
文摘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.
文摘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.
文摘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.
文摘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.
