The influence of the pressure transmission medium(PTM)on the excitonic interband transitions in monolayer tungsten diselenide(WSe2)is investigated using photoluminescence(PL)spectra under hydrostatic pressure up...The influence of the pressure transmission medium(PTM)on the excitonic interband transitions in monolayer tungsten diselenide(WSe2)is investigated using photoluminescence(PL)spectra under hydrostatic pressure up to 5GPa.Three kinds of PTMs,condensed argon(Ar),1:1 n-pentane and isopentane mixture(PM),and4:1 methanol and ethanol mixture(MEM,a PTM with polarity),are used.It is found that when either Ar or PM is used as the PTM,the PL peak of exciton related to the direct K-K interband transition shows a pressure-induced blue-shift at a rate of 32±4 or 32±1 meV/GPa,while it turns to be 50±9meV/GPa when MEM is used as the PTM.The indirect A-K interband transition presents almost no shift with increasing pressure up to approximatel.y 5 GPa when Ar and PM are used as the PTM,while it shows a red-shift at the rate of-17±7meV/GPa by using MEM as the PTM.These results reveal that the optical interband transitions of monolayer WSe2 are very sensitive to the polarity of the PTM.The anomalous pressure coefficient obtained using the polar PTM of MEM is ascribed to the existence of hydrogen-like bonds between hydroxyl in MEM and Se atoms under hydrostatic pressure.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
The in.jection of charge carriers from the electron/hole injection or transport layers in polymer light-emitting diodes potentially increases the device efficiency not by changing of charge intensity but by lattice di...The in.jection of charge carriers from the electron/hole injection or transport layers in polymer light-emitting diodes potentially increases the device efficiency not by changing of charge intensity but by lattice distortion variation and quasi-particle interactions. From the low-dimensional condensed matter physics perspective, a valid mechanism is proposed to bring a type of novel channels that, under a proper external electric field, transition- forbidden triplet excitons are transformed and partially charged by charge carriers (polarons/bipolarons), thus are able to emit light and to enhance fluorescence greatly.展开更多
The light absorption properties of semiconductor-based photocatalysts to a large extent determine the relevant catalytic performance.Traditional strategies in broadening the light absorption range are usually accompan...The light absorption properties of semiconductor-based photocatalysts to a large extent determine the relevant catalytic performance.Traditional strategies in broadening the light absorption range are usually accompanied with unfavorable changes in redox ability and dynamics of photoinduced species that would confuse the comprehensive optimization.In this work,we propose a nontrivial excitonic transition regulation strategy for gaining sub-bandgap light absorption in low-dimensional semiconductor-based photocatalysts.Using bismuth oxybromide(BiOBr)as a model system,we highlight that the light absorption cut-off edge could be effectively extended up to 500 nm by introducing Bi vacancies.On the basis of theoretical simulations and spectroscopic analyses,we attributed the broadening of light absorption to the promotion of excitonic transition that is generally forbidden in pristine BiOBr system,associated with Bi-vacancy-induced excited-state symmetry breaking.In addition,Bi vacancy was demonstrated to implement negligible effects on other photoexcitation properties like excited-state energy-level profiles and kinetics.Benefiting from these features,the defective sample exhibits a notable advantage in gaining visible-light-driven photocatalytic reactions.展开更多
Buckybowl structures as non-uniform electrostatic potential distributions of poly-cyclic aromatic materials show a unique photoelectric performance.In this work,OTC was utilized for dynamic modulation of triplet excit...Buckybowl structures as non-uniform electrostatic potential distributions of poly-cyclic aromatic materials show a unique photoelectric performance.In this work,OTC was utilized for dynamic modulation of triplet exciton transition processes.Five host molecules with different functional units were selected,thus providing dif-ferent intermolecular interactions in the host/guest systems.Therefore,the delayed emissions were regulated from 536 to 624 nm via the tuning of the triplet exciton transition processes of OTC in different hosts.Experimental data and theoretical calculations revealed that the varied triplet transition behaviors resulted from the competition between the intersystem crossing(ISC)process of OTC-monomer and the reverse intersystem crossing(RISC)process of OTC-aggregates.This work proves the superior structure of buckybowl-based luminophore for controlling triplet exciton transition processes and supplies a new perspective for persistent afterglow luminophore design.展开更多
The electron and heavy hole energy levels of two vertically coupled In As hemispherical quantum dots/wetting layers embedded in a Ga As barrier are calculated numerically. As the radius increases, the electronic energ...The electron and heavy hole energy levels of two vertically coupled In As hemispherical quantum dots/wetting layers embedded in a Ga As barrier are calculated numerically. As the radius increases, the electronic energies increase for the small base radii and decrease for the larger ones. The energies decrease as the dot height increases. The intersubband and interband transitions of the system are also studied. For both, a spectral peak position shift to lower energies is seen due to the vertical coupling of dots. The interband transition energy decreases as the dot size increases, decreases for the dot shapes with larger heights, and reaches a minimum for coupled semisphere dots.展开更多
基金Supported by the National Key Research and Development Program of China under Grant No 2016YFA0301202the National Natural Science Foundation of China under Grant Nos 11474275,61674135 and 91536101+1 种基金the Strategic Priority Research Program of the Chinese Academy of Sciences under Grant No XDPB0603the China Postdoctoral Science Foundation under Grant No 2017M622400
文摘The influence of the pressure transmission medium(PTM)on the excitonic interband transitions in monolayer tungsten diselenide(WSe2)is investigated using photoluminescence(PL)spectra under hydrostatic pressure up to 5GPa.Three kinds of PTMs,condensed argon(Ar),1:1 n-pentane and isopentane mixture(PM),and4:1 methanol and ethanol mixture(MEM,a PTM with polarity),are used.It is found that when either Ar or PM is used as the PTM,the PL peak of exciton related to the direct K-K interband transition shows a pressure-induced blue-shift at a rate of 32±4 or 32±1 meV/GPa,while it turns to be 50±9meV/GPa when MEM is used as the PTM.The indirect A-K interband transition presents almost no shift with increasing pressure up to approximatel.y 5 GPa when Ar and PM are used as the PTM,while it shows a red-shift at the rate of-17±7meV/GPa by using MEM as the PTM.These results reveal that the optical interband transitions of monolayer WSe2 are very sensitive to the polarity of the PTM.The anomalous pressure coefficient obtained using the polar PTM of MEM is ascribed to the existence of hydrogen-like bonds between hydroxyl in MEM and Se atoms under hydrostatic pressure.
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.
文摘The in.jection of charge carriers from the electron/hole injection or transport layers in polymer light-emitting diodes potentially increases the device efficiency not by changing of charge intensity but by lattice distortion variation and quasi-particle interactions. From the low-dimensional condensed matter physics perspective, a valid mechanism is proposed to bring a type of novel channels that, under a proper external electric field, transition- forbidden triplet excitons are transformed and partially charged by charge carriers (polarons/bipolarons), thus are able to emit light and to enhance fluorescence greatly.
基金supported by the National Key Research and Development Program of China(Nos.2022YFA1502903 and 2021YFA1501502)the Strategic Priority Research Program of Chinese Academy of Sciences(Nos.XDB36000000 and XDB0450102)+3 种基金the National Natural Science Foundation of China(22275179)the Anhui Provincial Key Research and Development Program(No.2022a05020054)the Youth Innovation Promotion Association of CAS(No.Y2021123)the Fundamental Research Funds for the Central Universities(No.WK2060000039)。
文摘The light absorption properties of semiconductor-based photocatalysts to a large extent determine the relevant catalytic performance.Traditional strategies in broadening the light absorption range are usually accompanied with unfavorable changes in redox ability and dynamics of photoinduced species that would confuse the comprehensive optimization.In this work,we propose a nontrivial excitonic transition regulation strategy for gaining sub-bandgap light absorption in low-dimensional semiconductor-based photocatalysts.Using bismuth oxybromide(BiOBr)as a model system,we highlight that the light absorption cut-off edge could be effectively extended up to 500 nm by introducing Bi vacancies.On the basis of theoretical simulations and spectroscopic analyses,we attributed the broadening of light absorption to the promotion of excitonic transition that is generally forbidden in pristine BiOBr system,associated with Bi-vacancy-induced excited-state symmetry breaking.In addition,Bi vacancy was demonstrated to implement negligible effects on other photoexcitation properties like excited-state energy-level profiles and kinetics.Benefiting from these features,the defective sample exhibits a notable advantage in gaining visible-light-driven photocatalytic reactions.
基金National Natural Scientific Foundation of China,Grant/Award Numbers:21975021,21975020,21875019,21871119,22105019,22175023Beijing National Laboratory for Molecular Sciences,Grant/Award Number:BNLMS192007BIT Research and Innovation Promoting Project,Grant/Award Number:2022YCXZ035。
文摘Buckybowl structures as non-uniform electrostatic potential distributions of poly-cyclic aromatic materials show a unique photoelectric performance.In this work,OTC was utilized for dynamic modulation of triplet exciton transition processes.Five host molecules with different functional units were selected,thus providing dif-ferent intermolecular interactions in the host/guest systems.Therefore,the delayed emissions were regulated from 536 to 624 nm via the tuning of the triplet exciton transition processes of OTC in different hosts.Experimental data and theoretical calculations revealed that the varied triplet transition behaviors resulted from the competition between the intersystem crossing(ISC)process of OTC-monomer and the reverse intersystem crossing(RISC)process of OTC-aggregates.This work proves the superior structure of buckybowl-based luminophore for controlling triplet exciton transition processes and supplies a new perspective for persistent afterglow luminophore design.
文摘The electron and heavy hole energy levels of two vertically coupled In As hemispherical quantum dots/wetting layers embedded in a Ga As barrier are calculated numerically. As the radius increases, the electronic energies increase for the small base radii and decrease for the larger ones. The energies decrease as the dot height increases. The intersubband and interband transitions of the system are also studied. For both, a spectral peak position shift to lower energies is seen due to the vertical coupling of dots. The interband transition energy decreases as the dot size increases, decreases for the dot shapes with larger heights, and reaches a minimum for coupled semisphere dots.