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
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 ...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.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
Metal halides have attracted worldwide attention as exceptional optoelectronic materials.Over the past decade,research on metal halides has yielded remarkable progress,and their color-conversion applications have show...Metal halides have attracted worldwide attention as exceptional optoelectronic materials.Over the past decade,research on metal halides has yielded remarkable progress,and their color-conversion applications have shown considerable promise for commercialization.With the reporting of self-trapped exciton(STE)emission in perovskites,the application of metal halides as broadband emitting materials in the lighting field has gained increas-ing interest.Herein,we provide a comprehensive review of metal halide STE emitters,especially for lighting applica-tions.We begin with highlighting the ideal spectral characteristics and corresponding performance metrics for light-ing.This is followed by a systematic summary of the mechanisms,optimization strategies,and recent advances of STE emission in metal halides.Finally,we outline the major challenges and prospective trends for metal halide STE emitters.This review aims to offer valuable insights into metal halide STE emitters and their lighting applications for facilitating the future commercialization.展开更多
Zero-dimensional perovskite materials,characterized by broadband emission caused by self-trapped excitons,are promising materials for stimuli-responsive and photo-writeable encryption.However,existing research is focu...Zero-dimensional perovskite materials,characterized by broadband emission caused by self-trapped excitons,are promising materials for stimuli-responsive and photo-writeable encryption.However,existing research is focused on the effects of structural phase transitions on photophysical properties,and lacks in-depth understanding of the mechanisms of self-trapped excitons emission.Here,we demonstrate that the dehydration reaction in zero-dimensional antimony halide clusters significantly enhances the self-trapped excitons emission without inducing structural phase transition,resulting in a substantial increase in photoluminescence(PL)quantum yield from 3.5%to 91.4%.In-situ X-ray diffraction and PL techniques were employed to shed light on the relationship between the crystal structure and radiative recombination,demonstrating the introduction of rich lattice distortion during the dehydration process.Temperature-dependent PL spectra and transient absorption spectra suggest that the lattice distortion causes the moderate electron-phonon coupling strength and high exciton binding energy,facilitating self-trapped excitons to relax from the non-radiative recombination singlet state to the radiative recombination triplet state,corresponding to the enhanced emission intensity.As a proof of concept,several switchable PL applications have been established in scenarios such as anti-counterfeiting,rewritable luminescent paper,and humidity sensing.This finding elucidates the emission mechanism of self-trapped excitons and provides a novel avenue for designing switchable luminescent materials.展开更多
Two-dimensional(2D)perovskites exhibit broadband emission due to strong exciton–phonon coupling-induced self-trapped excitons and thus would find important applications in the field of white-light emitting devices.Ho...Two-dimensional(2D)perovskites exhibit broadband emission due to strong exciton–phonon coupling-induced self-trapped excitons and thus would find important applications in the field of white-light emitting devices.However,the available identifying methods for self-trapped excitons are currently rather limited and complex.Here,we identify the existence of self-trapped excitons by Raman spectroscopy in both excited and non-excited states.Under excited states,the shifting of the Raman peak indicates the presence of the lattice distortion,which together with the extra Raman scattering peak reveals the presence of self-trapped excitons.Our work provides an alternative simple method to study self-trapped excitons in 2 D perovskites.展开更多
The vacancy-ordered quadruple perovskite Cs_(4)CdBi_(2)Cl_(12),as a newly-emerging lead-free perovskite system,has attracted great research interest due to its excellent stability and direct band gap.However,the poor ...The vacancy-ordered quadruple perovskite Cs_(4)CdBi_(2)Cl_(12),as a newly-emerging lead-free perovskite system,has attracted great research interest due to its excellent stability and direct band gap.However,the poor luminescence performance limits its application in light-emitting diodes(LEDs)and other fields.Herein,for the first time,an Ag^(+)ion doping strategy was proposed to greatly improve the emission performance of Cs_(4)CdBi_(2)Cl_(12) synthesized by hydrothermal method.Density functional theory calculations combined with experimental results evidence that the weak orange emission from Cs_(4)CdBi_(2)Cl_(12) is attributed to the phonon scattering and energy level crossing due to the large lattice distortion under excited states.Fortunately,Ag^(+)ion doping breaks the intrinsic crystal field environment of Cs_(4)CdBi_(2)Cl_(12),suppresses the crossover between ground and excited states,and reduces the energy loss in the form of nonradiative recombination.At a critical doping amount of 0.8%,the emission intensity of Cs_(4)CdBi_(2)Cl_(12):Ag^(+)reaches the maximum,about eight times that of the pristine sample.Moreover,the doped Cs_(4)CdBi_(2)Cl_(12) still maintains excellent stability against heat,ultraviolet irradiation,and environmental oxygen/moisture.The above advantages make it possible for this material to be used as solid-state phosphors for white LEDs applications,and the Commission International de I’Eclairage color coordinates of(0.31,0.34)and high color rendering index of 90.6 were achieved.More importantly,the white LED demonstrates remarkable operation stability in air ambient,showing almost no emission decay after a long working time for 48 h.We believe that this study puts forward an effective ion-doping strategy for emission enhancement of vacancy-ordered quadruple perovskite Cs_(4)CdBi_(2)Cl_(12),highlighting its great potential as efficient emitter compatible for practical applications.展开更多
With strong electron-phonon coupling,the self-trapped excitons are usually formed in materials,which leads to the local lattice distortion and localized excitons.The self-trapping strongly depends on the dimensionalit...With strong electron-phonon coupling,the self-trapped excitons are usually formed in materials,which leads to the local lattice distortion and localized excitons.The self-trapping strongly depends on the dimensionality of the materials.In the three dimensional case,there is a potential barrier for self-trapping,whereas no such barrier is present for quasi-one-dimensional systems.Two-dimensional(2D)systems are marginal cases with a much lower potential barrier or nonex istent potential barrier for the self-trapping,leading to the easier formation of self-trapped states.Self-trapped excitons emission exhibits a broadband emission with a large Stokes shift below the bandgap.2D perovskites are a class of layered structure material with unique optical properties and would find potential promising optoelectronic.In particular,self-trapped excitons are present in 2D per-ovskites and can significantly influence the optical and electrical properties of 2D perovskites due to the soft characteristic and strong electron-phonon interaction.Here,we summarized the luminescence characteristics,origins,and characterizations of self-trapped excitons in 2D perovskites and finally gave an introduction to their applications in optoelectronics.展开更多
We investigate the interactions of lattice pbonons with Wannier-Mott exciton, the exciton that has a large radius in two-dimensional molecular lattice, by the method of continuum limit approximation, and obtain that t...We investigate the interactions of lattice pbonons with Wannier-Mott exciton, the exciton that has a large radius in two-dimensional molecular lattice, by the method of continuum limit approximation, and obtain that the self-trapping can also appear in two-dimensional molecular lattice with a harmonic and nonlinear potential. The exciton effect on molecular lattice does not distort the molecular lattice but only makes it localized and the localization can also react, again through phonon coupling, to trap the energy and prevents its dispersion.展开更多
We investigate the interactions of lattice phonons with Frenkel exciton, which has a small radius in a twodimensional discrete molecular lattice, by the virtue of the quasi-discreteness approximation and the method of...We investigate the interactions of lattice phonons with Frenkel exciton, which has a small radius in a twodimensional discrete molecular lattice, by the virtue of the quasi-discreteness approximation and the method of multiplescale, and obtain that the self-trapping can also appear in the two-dimensional discrete molecular lattice with harmonic and nonlinear potential. The excitons＇ effect on the molecular lattice does not distort it but only causes it to localize which enables it to react again through phonon coupling to trap the energy and prevent its dispersion.展开更多
Twist,the very degree of freedom in van der Waals heterostructures,offers a compelling avenue to manipulate and tailor their electrical and optical characteristics.In particular,moirépatterns in twisted homobilay...Twist,the very degree of freedom in van der Waals heterostructures,offers a compelling avenue to manipulate and tailor their electrical and optical characteristics.In particular,moirépatterns in twisted homobilayer transition metal dichalcogenides(TMDs)lead to zone folding and miniband formation in the resulting electronic bands,holding the promise to exhibit inter-layer excitonic optical phenomena.Although some experiments have shown the existence of twist-angle-dependent intra-and inter-layer excitons in twisted MoSe2 homobilayers,electrical control of the interlayer excitons in MoSe_(2) is relatively under-explored.Here,we show the signatures of the moiréeffect on intralayer and interlayer excitons in 2H-stacked twisted MoSe2 homobilayers.Doping-and electric field-dependent photoluminescence mea-surements at low temperatures give evidence of the momentum-direct K-K intralayer excitons,and the momentum-indirect Г-K and Г-Q interlayer excitons.Our results suggest that twisted MoSe_(2) homobilayers are an intriguing platform for engineering interlayer exciton states,which may shed light on future atomically thin optoelectronic applications.展开更多
Semiconductor moirésuperlattices provide great platforms for exploring exotic collective excitations.Optical Stark effect,a shift of the electronic transition in the presence of a light field,provides an ultrafas...Semiconductor moirésuperlattices provide great platforms for exploring exotic collective excitations.Optical Stark effect,a shift of the electronic transition in the presence of a light field,provides an ultrafast and coherent method of manipulating matter states,which,however,has not been demonstrated in moirématerials.Here,we report the valleyselective optical Stark effect of moiréexcitons in the WSe_(2)/WS_(2)superlattice by using transient reflection spectroscopy.Prominent valley-selective energy shifts up to 7.8 meV have been observed for moiréexcitons,corresponding to pseudomagnetic fields as large as 34 T.Our results provide a route to coherently manipulate exotic states in moirésuperlattices.展开更多
Two-dimensional(2D)transition metal dichalcogenides(TMDs),endowed with exceptional light-matter interaction strength,have become a pivotal platform in advanced optoelectronics,enabling atomically precise control of ex...Two-dimensional(2D)transition metal dichalcogenides(TMDs),endowed with exceptional light-matter interaction strength,have become a pivotal platform in advanced optoelectronics,enabling atomically precise control of excitonic phenomena and offering transformative potential for engineering next-generation optoelectronic devices.In contrast to the narrowband absorption characteristics of conventional band-edge excitons,which are limited by the bandgap energy,highenergy excitons not only demonstrate broad momentum matching capability in the ultraviolet regime due to band nesting effects,but also exhibit distinct absorption peak signatures owing to robust excitonic stabilization under 2D confinement.These unique photophysical properties have established such systems as a prominent research frontier in contemporary exciton physics.This review primarily outlines the distinctive physical characteristics of high-energy excitons in TMDs from the perspectives of band structure,excitonic characteristics,and optical properties.Subsequently,we systematically delineate cutting-edge developments in TMD-based photonic devices exploiting high-energy excitonic band-nesting phenomena,with dedicated emphasis on the strategic engineering of nanoscale heterostructures for tailored optoelectronic functionality.Finally,the discussion concludes with an examination of the challenges associated with the design of high-energy exciton devices and their potential future applications.展开更多
Electron–hole(e–h)recombination is a fundamental process that governs energy dissipation and device efficiency in semiconductors.In two-dimensional(2D)materials,the formation of tightly bound excitons makes exciton-...Electron–hole(e–h)recombination is a fundamental process that governs energy dissipation and device efficiency in semiconductors.In two-dimensional(2D)materials,the formation of tightly bound excitons makes exciton-mediated e–h recombination the dominant decay pathway.In this work,nonradiative e–h recombination within excitons in monolayer MoS_(2) is investigated using first-principles simulations that combine nonadiabatic molecular dynamics with GW and real-time Bethe–Salpeter equation(BSE)propagation.A two-step process is identified:rapid intervalley redistribution induced by exchange interaction,followed by slower phonon-assisted recombination facilitated by exciton binding.By selectively removing the screened Coulomb and exchange terms from the BSE Hamiltonian,their respective contributions are disentangled—exchange interaction is found to increase the number of accessible recombination pathways,while binding reduces the excitation energy and enhances nonradiative decay.A reduction in recombination lifetime by over an order of magnitude is observed due to the excitonic many-body effects.These findings provide microscopic insights for understanding and tuning exciton lifetimes in 2D transition-metal dichalcogenides.展开更多
Organic photovoltaics(OPVs)have achieved remarkable progress,with laboratory-scale single-junction devices now demonstrating power conversion efficiencies(PCEs)exceeding 20%.However,these efficiencies are highly depen...Organic photovoltaics(OPVs)have achieved remarkable progress,with laboratory-scale single-junction devices now demonstrating power conversion efficiencies(PCEs)exceeding 20%.However,these efficiencies are highly dependent on the thickness of the photoactive layer,which is typically around 100 nm.This sensitivity poses a challenge for industrial-scale fabrication.Achieving high PCEs in thick-film OPVs is therefore essential.This review systematically examines recent advancements in thick-film OPVs,focusing on the fundamental mechanisms that lead to efficiency loss and strategies to enhance performance.We provide a comprehensive analysis spanning the complete photovoltaic process chain:from initial exciton generation and diffusion dynamics,through dissociation mechanisms,to subsequent charge-carrier transport,balance optimization,and final collection efficiency.Particular emphasis is placed on cutting-edge solutions in molecular engineering and device architecture optimization.By synthesizing these interdisciplinary approaches and investigating the potential contributions in stability,cost,and machine learning aspects,this work establishes comprehensive guidelines for designing high-performance OPVs devices with minimal thickness dependence,ultimately aiming to bridge the gap between laboratory achievements and industrial manufacturing requirements.展开更多
Correction to:Nano-Micro Letters(2026)18:10.https://doi.org/10.1007/s40820-025-01852-8 Following publication of the original article[1],the authors reported that the last author’s name was inadvertently misspelled.Th...Correction to:Nano-Micro Letters(2026)18:10.https://doi.org/10.1007/s40820-025-01852-8 Following publication of the original article[1],the authors reported that the last author’s name was inadvertently misspelled.The published version showed“Hongzhen Chen”,whereas the correct spelling should be“Hongzheng Chen”.The correct author name has been provided in this Correction,and the original article[1]has been corrected.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
Atoms under optical and magnetic trapping in a limited space at a very low temperature can lead to Bose-Einstein condensation （BEC）, even in a one-dimensional （1D） optical lattice. However, can the confinment of d...Atoms under optical and magnetic trapping in a limited space at a very low temperature can lead to Bose-Einstein condensation （BEC）, even in a one-dimensional （1D） optical lattice. However, can the confinment of dense excitons in a 1D semiconductor microstructure easily reach the excitonic BEC？ A lightly Mn（II）-doped ZnO nanowire under a femtosecond laser pulse pump at room temperature produces single-mode lasing from coherent bipolaronic excitons, which is much like a macroscopic quantum state due to the condensation of the bipoaronic excitons if not real BEC. In this process, longitudinal biphonon binding with the exciton plays an important role. We revisit this system and propose possibility of bipolaronic exciton condensation. More studies are needed for this condensation phenomenon in 1D microcavity systems.展开更多
The binding energies of excitons in quantum well structures subjected to an applied uniform electric field by taking into account the exciton longitudinal optical phonon interaction is calculated. The binding energies...The binding energies of excitons in quantum well structures subjected to an applied uniform electric field by taking into account the exciton longitudinal optical phonon interaction is calculated. The binding energies and corresponding Stark shifts for Ⅲ-Ⅴ and Ⅱ-Ⅵ compound semiconductor quantum well structures have been numerically computed. The results for GaAs/A1GaAs and ZnCdSe/ZnSe quantum wells are given and discussed. Theoretical results show that the exciton-phonon coupling reduces both the exciton binding energies and the Stark shifts by screening the Coulomb interaction. This effect is observable experimentally and cannot be neglected.展开更多
In this work, the effects of quantum confinement on the ground state energy of a correlated electron-hole pair in a spherical and in a disc-like quantum dot have been investigated as a function of quantum dot size. Un...In this work, the effects of quantum confinement on the ground state energy of a correlated electron-hole pair in a spherical and in a disc-like quantum dot have been investigated as a function of quantum dot size. Under parabolic confinement potential and within effective mass approximation Ritz＇s variational method is applied to Hylleraas-like trial wavefunction. An efficient method for reducing the main effort of the calculation of terms like τekh exp （-λτeh） is introduced. The main contribution of the present work is the introduction of integral transforms which provide the calculation of expectation value of energy and the related matrix elements to be done analytically over single-particle coordinates instead of Hvlleraas coordinates.展开更多
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supported by the National Key R&D Program of China(2016YFB070700702)the National Natural Science Foundation of China(51761145048)+1 种基金the Fundamental Research Funds for the Central Universities(HUST:2019421JYCXJJ004)the China Postdoctoral Science Foundation Grant(2019M662624).
文摘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.
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.
文摘Metal halides have attracted worldwide attention as exceptional optoelectronic materials.Over the past decade,research on metal halides has yielded remarkable progress,and their color-conversion applications have shown considerable promise for commercialization.With the reporting of self-trapped exciton(STE)emission in perovskites,the application of metal halides as broadband emitting materials in the lighting field has gained increas-ing interest.Herein,we provide a comprehensive review of metal halide STE emitters,especially for lighting applica-tions.We begin with highlighting the ideal spectral characteristics and corresponding performance metrics for light-ing.This is followed by a systematic summary of the mechanisms,optimization strategies,and recent advances of STE emission in metal halides.Finally,we outline the major challenges and prospective trends for metal halide STE emitters.This review aims to offer valuable insights into metal halide STE emitters and their lighting applications for facilitating the future commercialization.
基金financially supported by the National Ten Thousand Talent Program for Young Top-notch TalentNational Natural Science Foundation of China (22379044 and 52203330)+8 种基金Shanghai Pilot Program for Basic Research (22TQ1400100-5)“Dawn”Program of Shanghai Education Commission (22SG28)Shanghai Municipal Natural Science Foundation (22ZR1418000)Shanghai Sailing Program(22YF1410000)Postdoctoral Research Foundation of China(2021M701190)Fundamental Research Funds for the Central Universities (JKD01241607 and JKVD1241041)Major Science and Technology Projects of Inner Mongolia Autonomous Region (2021ZD0042)Shanghai Engineering Research Center of Hierarchical Nanomaterials(18DZ2252400)Shanghai Frontiers Science Center of Optogenetic Techniques for Cell Metabolism。
文摘Zero-dimensional perovskite materials,characterized by broadband emission caused by self-trapped excitons,are promising materials for stimuli-responsive and photo-writeable encryption.However,existing research is focused on the effects of structural phase transitions on photophysical properties,and lacks in-depth understanding of the mechanisms of self-trapped excitons emission.Here,we demonstrate that the dehydration reaction in zero-dimensional antimony halide clusters significantly enhances the self-trapped excitons emission without inducing structural phase transition,resulting in a substantial increase in photoluminescence(PL)quantum yield from 3.5%to 91.4%.In-situ X-ray diffraction and PL techniques were employed to shed light on the relationship between the crystal structure and radiative recombination,demonstrating the introduction of rich lattice distortion during the dehydration process.Temperature-dependent PL spectra and transient absorption spectra suggest that the lattice distortion causes the moderate electron-phonon coupling strength and high exciton binding energy,facilitating self-trapped excitons to relax from the non-radiative recombination singlet state to the radiative recombination triplet state,corresponding to the enhanced emission intensity.As a proof of concept,several switchable PL applications have been established in scenarios such as anti-counterfeiting,rewritable luminescent paper,and humidity sensing.This finding elucidates the emission mechanism of self-trapped excitons and provides a novel avenue for designing switchable luminescent materials.
基金supported by the National Key Research and Development Program of China(No.2018YFA0704403)National Natural Science Foundation of China(NSFC)(No.62074064)+2 种基金Innovation Fund of WNLO,Key Laboratory of Nanodevices and Applications,Suzhou Institute of NanoTech and Nano-Bionics,Chinese Academy of Sciences(No.19ZS03)China Postdoctoral Science Foundation(No.2020M682399)Postdoctoral Innovation Fund of Hubei Province。
文摘Two-dimensional(2D)perovskites exhibit broadband emission due to strong exciton–phonon coupling-induced self-trapped excitons and thus would find important applications in the field of white-light emitting devices.However,the available identifying methods for self-trapped excitons are currently rather limited and complex.Here,we identify the existence of self-trapped excitons by Raman spectroscopy in both excited and non-excited states.Under excited states,the shifting of the Raman peak indicates the presence of the lattice distortion,which together with the extra Raman scattering peak reveals the presence of self-trapped excitons.Our work provides an alternative simple method to study self-trapped excitons in 2 D perovskites.
基金support from the National Key R&D Program of China(No.2022YFB2803900)the National Natural Science Foundation of China(Nos.12074347,12004346,12204426,and 61935009)+1 种基金Science Foundation for Distinguished Young Scholars of Henan Province(No.212300410019)the Support Program for Scientific and Technological Innovation Teams of Higher Education in Henan Province(No.231RTSTHN012).
文摘The vacancy-ordered quadruple perovskite Cs_(4)CdBi_(2)Cl_(12),as a newly-emerging lead-free perovskite system,has attracted great research interest due to its excellent stability and direct band gap.However,the poor luminescence performance limits its application in light-emitting diodes(LEDs)and other fields.Herein,for the first time,an Ag^(+)ion doping strategy was proposed to greatly improve the emission performance of Cs_(4)CdBi_(2)Cl_(12) synthesized by hydrothermal method.Density functional theory calculations combined with experimental results evidence that the weak orange emission from Cs_(4)CdBi_(2)Cl_(12) is attributed to the phonon scattering and energy level crossing due to the large lattice distortion under excited states.Fortunately,Ag^(+)ion doping breaks the intrinsic crystal field environment of Cs_(4)CdBi_(2)Cl_(12),suppresses the crossover between ground and excited states,and reduces the energy loss in the form of nonradiative recombination.At a critical doping amount of 0.8%,the emission intensity of Cs_(4)CdBi_(2)Cl_(12):Ag^(+)reaches the maximum,about eight times that of the pristine sample.Moreover,the doped Cs_(4)CdBi_(2)Cl_(12) still maintains excellent stability against heat,ultraviolet irradiation,and environmental oxygen/moisture.The above advantages make it possible for this material to be used as solid-state phosphors for white LEDs applications,and the Commission International de I’Eclairage color coordinates of(0.31,0.34)and high color rendering index of 90.6 were achieved.More importantly,the white LED demonstrates remarkable operation stability in air ambient,showing almost no emission decay after a long working time for 48 h.We believe that this study puts forward an effective ion-doping strategy for emission enhancement of vacancy-ordered quadruple perovskite Cs_(4)CdBi_(2)Cl_(12),highlighting its great potential as efficient emitter compatible for practical applications.
基金D.L.acknowledges the support from the National Basic Research Program of China(No.2018YFA0704403)the National Natural Science Foundation of China(NSFC)(Grant No.61674060)Innovation Fund of Wuhan National Laboratory for Optoelectronics(WNLO).
文摘With strong electron-phonon coupling,the self-trapped excitons are usually formed in materials,which leads to the local lattice distortion and localized excitons.The self-trapping strongly depends on the dimensionality of the materials.In the three dimensional case,there is a potential barrier for self-trapping,whereas no such barrier is present for quasi-one-dimensional systems.Two-dimensional(2D)systems are marginal cases with a much lower potential barrier or nonex istent potential barrier for the self-trapping,leading to the easier formation of self-trapped states.Self-trapped excitons emission exhibits a broadband emission with a large Stokes shift below the bandgap.2D perovskites are a class of layered structure material with unique optical properties and would find potential promising optoelectronic.In particular,self-trapped excitons are present in 2D per-ovskites and can significantly influence the optical and electrical properties of 2D perovskites due to the soft characteristic and strong electron-phonon interaction.Here,we summarized the luminescence characteristics,origins,and characterizations of self-trapped excitons in 2D perovskites and finally gave an introduction to their applications in optoelectronics.
基金supported by the National Natural Science Foundation of China (Grant No.1057400)the Natural Science Foundation of Heilongjiang Province,China (Grant No.A200506)
文摘We investigate the interactions of lattice pbonons with Wannier-Mott exciton, the exciton that has a large radius in two-dimensional molecular lattice, by the method of continuum limit approximation, and obtain that the self-trapping can also appear in two-dimensional molecular lattice with a harmonic and nonlinear potential. The exciton effect on molecular lattice does not distort the molecular lattice but only makes it localized and the localization can also react, again through phonon coupling, to trap the energy and prevents its dispersion.
基金supported by the National Natural Science Foundation of China (Grant No 1057400)the Natural Science Foundation of Heilongjiang Province of China (Grant No A200506)
文摘We investigate the interactions of lattice phonons with Frenkel exciton, which has a small radius in a twodimensional discrete molecular lattice, by the virtue of the quasi-discreteness approximation and the method of multiplescale, and obtain that the self-trapping can also appear in the two-dimensional discrete molecular lattice with harmonic and nonlinear potential. The excitons＇ effect on the molecular lattice does not distort it but only causes it to localize which enables it to react again through phonon coupling to trap the energy and prevent its dispersion.
基金supported by the National Key R&D Program of China(No.2023YFF1500600)the National Natural Science Foun-dation of China(Nos.12004259,12204287)+3 种基金China Postdoc-toral Science Foundation(Grant No.2022M723215)Zheng Vitto Han acknowledges the support of the Fund for Shanxi“1331 Project”Key Subjects Construction,and the Innovation Program for Quantum Science and Technology(Grant No.2021ZD0302003)Kenji Watanabe and Takashi Taniguchi acknowledge support from the JSPS KAKENHI(Grant Nos.20H00354 and 23H02052)the World Premier International Research Center Initiative(WPI),MEXT,Japan.
文摘Twist,the very degree of freedom in van der Waals heterostructures,offers a compelling avenue to manipulate and tailor their electrical and optical characteristics.In particular,moirépatterns in twisted homobilayer transition metal dichalcogenides(TMDs)lead to zone folding and miniband formation in the resulting electronic bands,holding the promise to exhibit inter-layer excitonic optical phenomena.Although some experiments have shown the existence of twist-angle-dependent intra-and inter-layer excitons in twisted MoSe2 homobilayers,electrical control of the interlayer excitons in MoSe_(2) is relatively under-explored.Here,we show the signatures of the moiréeffect on intralayer and interlayer excitons in 2H-stacked twisted MoSe2 homobilayers.Doping-and electric field-dependent photoluminescence mea-surements at low temperatures give evidence of the momentum-direct K-K intralayer excitons,and the momentum-indirect Г-K and Г-Q interlayer excitons.Our results suggest that twisted MoSe_(2) homobilayers are an intriguing platform for engineering interlayer exciton states,which may shed light on future atomically thin optoelectronic applications.
基金Project supported by the National Key R&D Program of China(Grant Nos.2022YFA1402400 and 2022YFA1405400)the National Natural Science Foundation of China(Grant Nos.11934011 and 12274365)+3 种基金Zhejiang Provincial Natural Science Foundation of China(Grant No.LR24A040001)Open project of Key Laboratory of Artificial Structures and Quantum Control(Ministry of Education)of Shanghai Jiao Tong Universitysupport from the JSPS KAKENHI(Grant Nos.20H00354 and 23H02052)World Premier International Research Center Initiative(WPI),MEXT,Japan。
文摘Semiconductor moirésuperlattices provide great platforms for exploring exotic collective excitations.Optical Stark effect,a shift of the electronic transition in the presence of a light field,provides an ultrafast and coherent method of manipulating matter states,which,however,has not been demonstrated in moirématerials.Here,we report the valleyselective optical Stark effect of moiréexcitons in the WSe_(2)/WS_(2)superlattice by using transient reflection spectroscopy.Prominent valley-selective energy shifts up to 7.8 meV have been observed for moiréexcitons,corresponding to pseudomagnetic fields as large as 34 T.Our results provide a route to coherently manipulate exotic states in moirésuperlattices.
基金Project supported by the National Natural Science Foundation Fund for Distinguished Young Scholars(Grant No.52025022)the National Natural Science Foundation of China(Grant Nos.62574038,12474421,62275045,and 12074060)+1 种基金the National Key R&D Program of China(Grant No.2023YFB3610200)the Fund from Jilin Province(Grant Nos.JJKH20241413KJ and 20240601049RC)。
文摘Two-dimensional(2D)transition metal dichalcogenides(TMDs),endowed with exceptional light-matter interaction strength,have become a pivotal platform in advanced optoelectronics,enabling atomically precise control of excitonic phenomena and offering transformative potential for engineering next-generation optoelectronic devices.In contrast to the narrowband absorption characteristics of conventional band-edge excitons,which are limited by the bandgap energy,highenergy excitons not only demonstrate broad momentum matching capability in the ultraviolet regime due to band nesting effects,but also exhibit distinct absorption peak signatures owing to robust excitonic stabilization under 2D confinement.These unique photophysical properties have established such systems as a prominent research frontier in contemporary exciton physics.This review primarily outlines the distinctive physical characteristics of high-energy excitons in TMDs from the perspectives of band structure,excitonic characteristics,and optical properties.Subsequently,we systematically delineate cutting-edge developments in TMD-based photonic devices exploiting high-energy excitonic band-nesting phenomena,with dedicated emphasis on the strategic engineering of nanoscale heterostructures for tailored optoelectronic functionality.Finally,the discussion concludes with an examination of the challenges associated with the design of high-energy exciton devices and their potential future applications.
基金supported by the National Key Research and Development Program of China (Grant Nos.2024YFA1409800 for J.Z.and2024YFA1408603 for Q.Z.)the National Natural Science Foundation of China (Grant Nos.12125408,12334004for J.Z.,and 12174363 for Q.Z.)+1 种基金the Innovation Program for Quantum Science and Technology (Grant No.2021ZD0303306 for J.Z.)the Strategic Priority Research Program of the Chinese Academy of Sciences(Grant No.XDB0450101 for J.Z.)。
文摘Electron–hole(e–h)recombination is a fundamental process that governs energy dissipation and device efficiency in semiconductors.In two-dimensional(2D)materials,the formation of tightly bound excitons makes exciton-mediated e–h recombination the dominant decay pathway.In this work,nonradiative e–h recombination within excitons in monolayer MoS_(2) is investigated using first-principles simulations that combine nonadiabatic molecular dynamics with GW and real-time Bethe–Salpeter equation(BSE)propagation.A two-step process is identified:rapid intervalley redistribution induced by exchange interaction,followed by slower phonon-assisted recombination facilitated by exciton binding.By selectively removing the screened Coulomb and exchange terms from the BSE Hamiltonian,their respective contributions are disentangled—exchange interaction is found to increase the number of accessible recombination pathways,while binding reduces the excitation energy and enhances nonradiative decay.A reduction in recombination lifetime by over an order of magnitude is observed due to the excitonic many-body effects.These findings provide microscopic insights for understanding and tuning exciton lifetimes in 2D transition-metal dichalcogenides.
基金supported by Natural Science Foundation of Zhejiang Province(Nos.LQ23E030002,LZ23B040001)the National Natural Science Foundation of China(Nos.52303226,21971049)L.Zhan acknowledges the research start-up fund from Hangzhou Normal University(4095C50222204002).
文摘Organic photovoltaics(OPVs)have achieved remarkable progress,with laboratory-scale single-junction devices now demonstrating power conversion efficiencies(PCEs)exceeding 20%.However,these efficiencies are highly dependent on the thickness of the photoactive layer,which is typically around 100 nm.This sensitivity poses a challenge for industrial-scale fabrication.Achieving high PCEs in thick-film OPVs is therefore essential.This review systematically examines recent advancements in thick-film OPVs,focusing on the fundamental mechanisms that lead to efficiency loss and strategies to enhance performance.We provide a comprehensive analysis spanning the complete photovoltaic process chain:from initial exciton generation and diffusion dynamics,through dissociation mechanisms,to subsequent charge-carrier transport,balance optimization,and final collection efficiency.Particular emphasis is placed on cutting-edge solutions in molecular engineering and device architecture optimization.By synthesizing these interdisciplinary approaches and investigating the potential contributions in stability,cost,and machine learning aspects,this work establishes comprehensive guidelines for designing high-performance OPVs devices with minimal thickness dependence,ultimately aiming to bridge the gap between laboratory achievements and industrial manufacturing requirements.
文摘Correction to:Nano-Micro Letters(2026)18:10.https://doi.org/10.1007/s40820-025-01852-8 Following publication of the original article[1],the authors reported that the last author’s name was inadvertently misspelled.The published version showed“Hongzhen Chen”,whereas the correct spelling should be“Hongzheng Chen”.The correct author name has been provided in this Correction,and the original article[1]has been corrected.
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supported by the National Natural Science Foundation of China (Grant Nos. 90606001,20873039,and 51002011)the Excellent Young Scholars Research Fund of Beijing Institute of Technology
文摘Atoms under optical and magnetic trapping in a limited space at a very low temperature can lead to Bose-Einstein condensation （BEC）, even in a one-dimensional （1D） optical lattice. However, can the confinment of dense excitons in a 1D semiconductor microstructure easily reach the excitonic BEC？ A lightly Mn（II）-doped ZnO nanowire under a femtosecond laser pulse pump at room temperature produces single-mode lasing from coherent bipolaronic excitons, which is much like a macroscopic quantum state due to the condensation of the bipoaronic excitons if not real BEC. In this process, longitudinal biphonon binding with the exciton plays an important role. We revisit this system and propose possibility of bipolaronic exciton condensation. More studies are needed for this condensation phenomenon in 1D microcavity systems.
基金Project supported in part by the National Natural Science Foundation of China （Grant No 10164003） and the Natural Science Foundation of Inner Mongol of China （Grant No 200408020101）.
文摘The binding energies of excitons in quantum well structures subjected to an applied uniform electric field by taking into account the exciton longitudinal optical phonon interaction is calculated. The binding energies and corresponding Stark shifts for Ⅲ-Ⅴ and Ⅱ-Ⅵ compound semiconductor quantum well structures have been numerically computed. The results for GaAs/A1GaAs and ZnCdSe/ZnSe quantum wells are given and discussed. Theoretical results show that the exciton-phonon coupling reduces both the exciton binding energies and the Stark shifts by screening the Coulomb interaction. This effect is observable experimentally and cannot be neglected.
文摘In this work, the effects of quantum confinement on the ground state energy of a correlated electron-hole pair in a spherical and in a disc-like quantum dot have been investigated as a function of quantum dot size. Under parabolic confinement potential and within effective mass approximation Ritz＇s variational method is applied to Hylleraas-like trial wavefunction. An efficient method for reducing the main effort of the calculation of terms like τekh exp （-λτeh） is introduced. The main contribution of the present work is the introduction of integral transforms which provide the calculation of expectation value of energy and the related matrix elements to be done analytically over single-particle coordinates instead of Hvlleraas coordinates.
