We theoretically analyze the steady state emission spectrum and transient temporal dynamics in a coupled biexciton quantum dot（QD）–cavity system. For steady state, a phonon-assisted biexciton–exciton cascade model...We theoretically analyze the steady state emission spectrum and transient temporal dynamics in a coupled biexciton quantum dot（QD）–cavity system. For steady state, a phonon-assisted biexciton–exciton cascade model under continuous wave（CW） excitation is presented to explain the asymmetric QD–cavity emission spectrum intensities（intensities of cavity,exciton, and biexciton emission peak） in off-resonance condition. Results demonstrate that the electron–phonon process is crucial to the asymmetry of emission spectrum intensity. Moreover the transient characteristics of the biexciton–exciton cascade system under pulse excitation show abundant nonlinear temporal dynamic behaviors, including complicated oscillations which are caused by the four-level structure of QD model. We also reveal that under off-resonance condition the cavity outputs are slightly reduced due to the electron–phonon interaction.展开更多
Nanowires have recently attracted more attention because of their low-dimensional structure, tunable optical and electrical properties for next-generation nanoscale optoelectronic devices. Cd S nanowire array, which i...Nanowires have recently attracted more attention because of their low-dimensional structure, tunable optical and electrical properties for next-generation nanoscale optoelectronic devices. Cd S nanowire array, which is(002)-orientation growth and approximately perpendicular to Cd foil substrate, has been fabricated by the solvothermal method. In the temperature-dependent photoluminescence, from short wavelength to long wavelength, four peaks can be ascribed to the emissions from the bandgap, the transition from the holes being bound to the donors or the electrons being bound to the acceptors, the transition from Cd interstitials to Cd vacancies, and the transition from S vacancies to the valence band,respectively. In the photoluminescence of 10 K, the emission originated from the bandgap appears in the form of multiple peaks. Two stronger peaks and five weaker peaks can be observed. The energy differences of the adjacent peaks are close to 38 me V, which is ascribed to the LO phonon energy of Cd S. For the multiple peaks of bandgap emission, from low energy to high energy, the first, second, and third peaks are contributed to the third-order, second-order, and first-order phonon replica of the free exciton A, respectively;the fourth peak is originated from the free exciton A;the fifth peak is contributed to the first-order phonon replica of the excitons bound to neutral donors;the sixth and seventh peaks are originated from the excitons bound to neutral donors and the light polarization parallel to the c axis of hexagonal Cd S, respectively.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
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
Based on the framework of the effective-mass approximation,the ionized acceptor bound exciton(A-,X) binding energy and the emission wavelength are investigated for a cylindrical wurtzite(WZ) GaN/Al x Ga1-x N quantum d...Based on the framework of the effective-mass approximation,the ionized acceptor bound exciton(A-,X) binding energy and the emission wavelength are investigated for a cylindrical wurtzite(WZ) GaN/Al x Ga1-x N quantum dot(QD) with finite potential barriers by means of a variational method.Numerical results show that the binding energy and the emission wavelength highly depend on the QD size,the position of the ionized acceptor and the Al composition x of the barrier material Al x Ga1-x N.The binding energy and the emission wavelength are larger when the acceptor is located in the vicinity of the left interface of the QD.In particular,the binding energy of(A-,X) complex is insensitive to the dot height when the acceptor is located at the left boundary of the QD.The ionized acceptor bound exciton binding energy and the emission wavelength are both increased if Al composition x is increased.展开更多
基金Project supported by the National Natural Science Foundation of China(Grant Nos.61275201 and 61372037)the Beijing Municipal Excellent Ph.D. Thesis Guidance Foundation(Grant No.20131001301)the Fund of State Key Laboratory of Information Photonics and Optical Communications(Beijing University of Posts and Telecommunications),China
文摘We theoretically analyze the steady state emission spectrum and transient temporal dynamics in a coupled biexciton quantum dot（QD）–cavity system. For steady state, a phonon-assisted biexciton–exciton cascade model under continuous wave（CW） excitation is presented to explain the asymmetric QD–cavity emission spectrum intensities（intensities of cavity,exciton, and biexciton emission peak） in off-resonance condition. Results demonstrate that the electron–phonon process is crucial to the asymmetry of emission spectrum intensity. Moreover the transient characteristics of the biexciton–exciton cascade system under pulse excitation show abundant nonlinear temporal dynamic behaviors, including complicated oscillations which are caused by the four-level structure of QD model. We also reveal that under off-resonance condition the cavity outputs are slightly reduced due to the electron–phonon interaction.
基金Project supported by the Natural Science Foundation of Henan Province,China(Grant No.202300410304)Key Research Project for Science and Technology of the Education Department of Henan Province,China(Grant No.21A140021)。
文摘Nanowires have recently attracted more attention because of their low-dimensional structure, tunable optical and electrical properties for next-generation nanoscale optoelectronic devices. Cd S nanowire array, which is(002)-orientation growth and approximately perpendicular to Cd foil substrate, has been fabricated by the solvothermal method. In the temperature-dependent photoluminescence, from short wavelength to long wavelength, four peaks can be ascribed to the emissions from the bandgap, the transition from the holes being bound to the donors or the electrons being bound to the acceptors, the transition from Cd interstitials to Cd vacancies, and the transition from S vacancies to the valence band,respectively. In the photoluminescence of 10 K, the emission originated from the bandgap appears in the form of multiple peaks. Two stronger peaks and five weaker peaks can be observed. The energy differences of the adjacent peaks are close to 38 me V, which is ascribed to the LO phonon energy of Cd S. For the multiple peaks of bandgap emission, from low energy to high energy, the first, second, and third peaks are contributed to the third-order, second-order, and first-order phonon replica of the free exciton A, respectively;the fourth peak is originated from the free exciton A;the fifth peak is contributed to the first-order phonon replica of the excitons bound to neutral donors;the sixth and seventh peaks are originated from the excitons bound to neutral donors and the light polarization parallel to the c axis of hexagonal Cd S, respectively.
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Supported by Technology Projects of the Education Bureau of Fujian Province umder Grant No. JK2009038
文摘Based on the framework of the effective-mass approximation,the ionized acceptor bound exciton(A-,X) binding energy and the emission wavelength are investigated for a cylindrical wurtzite(WZ) GaN/Al x Ga1-x N quantum dot(QD) with finite potential barriers by means of a variational method.Numerical results show that the binding energy and the emission wavelength highly depend on the QD size,the position of the ionized acceptor and the Al composition x of the barrier material Al x Ga1-x N.The binding energy and the emission wavelength are larger when the acceptor is located in the vicinity of the left interface of the QD.In particular,the binding energy of(A-,X) complex is insensitive to the dot height when the acceptor is located at the left boundary of the QD.The ionized acceptor bound exciton binding energy and the emission wavelength are both increased if Al composition x is increased.
