The exciton relaxation kinetics of ZnCuInS/ZnSe/ZnS quantum dots (QDs) is investigated by time-resolved spectroscopy techniques in detail. Based on the rate distribution model, the wavelength-dependent emission dyna...The exciton relaxation kinetics of ZnCuInS/ZnSe/ZnS quantum dots (QDs) is investigated by time-resolved spectroscopy techniques in detail. Based on the rate distribution model, the wavelength-dependent emission dynamics shows that the intrinsic exciton, the exciton in the interface defect state and that in donor-acceptor pair state (DAPS) together participate in the photoluminescence process of QDs, and the whole emission process is mainly dependent on the DAPS emission. Transient absorption data show that the intrinsic exciton and the interface defect species maybe together appear after excitation and the intensity-dependent Auger recombination process also exists in QDs at high excitation intensity.展开更多
All-optical coherent control of optical bistability (013) and optical multistability (OM) in the 4.8 nm ZnSe single-quantum well based on excitons and biexciton transitions is investigated. By applying a pair of p...All-optical coherent control of optical bistability (013) and optical multistability (OM) in the 4.8 nm ZnSe single-quantum well based on excitons and biexciton transitions is investigated. By applying a pair of phase-locked laser pulses all-optical coherent control can be obtained. Theoretical analysis with density matrix and Maxwell equations then yield the optical bistability ~nd optical multistability. It is shown that by controlling the coherent and incoherent processes, the intensity threshold of OB and OM can be modified. Also, it is found that the switching between OB and OM or vice versa can be occurred for some controllable parameters.展开更多
Optical selection rules fundamentally determine the optical transitions between energy states in a variety of physical systems,from hydrogen atoms to bulk crystals such as gallium arsenide.These rules are important fo...Optical selection rules fundamentally determine the optical transitions between energy states in a variety of physical systems,from hydrogen atoms to bulk crystals such as gallium arsenide.These rules are important for optoelectronic applications such as lasers,energy-dispersive X-ray spectroscopy,and quantum computation.Recently,single-layer transition metal dichalcogenides have been found to exhibit valleys in momentum space with nontrivial Berry curvature and excitons with large binding energy.However,there has been little study of how the unique valley degree of freedom combined with the strong excitonic effect influences the nonlinear optical excitation.Here,we report the discovery of nonlinear optical selection rules in monolayer WS2,an important candidate for visible 2D optoelectronics because of its high quantum yield and large direct bandgap.We experimentally demonstrated this principle for second-harmonic generation and two-photon luminescence(TPL).Moreover,the circularly polarized TPL and the study of its dynamics evince a sub-ps interexciton relaxation(2p R 1s).The discovery of this new optical selection rule in a valleytronic 2D system not only considerably enhances knowledge in this area but also establishes a foundation for the control of optical transitions that will be crucial for valley optoelectronic device applications such as 2D valley-polarized THz sources with 2p–1s transitions,optical switches,and coherent control for quantum computing.展开更多
Two dimensional excitonic devices are of great potential to overcome the dilemma of response time and integration in current generation of electron or/and photon based systems.The ultrashort diffusion length of excito...Two dimensional excitonic devices are of great potential to overcome the dilemma of response time and integration in current generation of electron or/and photon based systems.The ultrashort diffusion length of exciton arising from ultrafast relaxation and low carrier mobility greatly discounts the performance of excitonic devices.Phonon scattering and exciton localization are crucial to understand the modulation of exciton flux in two dimensional disorder energy landscape,which still remain elusive.Here,we report an optimized scheme for exciton diffusion and relaxation dominated by phonon scattering and disorder potentials in WSe2 monolayers.The effective diffusion coefficient is enhanced by>200%at 280 K.The excitons tend to be localized by disorder potentials accompanied by the steadily weakening of phonon scattering when temperature drops to 260 K,and the onset of exciton localization brings forward as decreasing temperature.These findings identify that phonon scattering and disorder potentials are of great importance for long-range exciton diffusion and thermal management in exciton based systems,and lay a firm foundation for the development of functional excitonic devices.展开更多
文摘The exciton relaxation kinetics of ZnCuInS/ZnSe/ZnS quantum dots (QDs) is investigated by time-resolved spectroscopy techniques in detail. Based on the rate distribution model, the wavelength-dependent emission dynamics shows that the intrinsic exciton, the exciton in the interface defect state and that in donor-acceptor pair state (DAPS) together participate in the photoluminescence process of QDs, and the whole emission process is mainly dependent on the DAPS emission. Transient absorption data show that the intrinsic exciton and the interface defect species maybe together appear after excitation and the intensity-dependent Auger recombination process also exists in QDs at high excitation intensity.
文摘All-optical coherent control of optical bistability (013) and optical multistability (OM) in the 4.8 nm ZnSe single-quantum well based on excitons and biexciton transitions is investigated. By applying a pair of phase-locked laser pulses all-optical coherent control can be obtained. Theoretical analysis with density matrix and Maxwell equations then yield the optical bistability ~nd optical multistability. It is shown that by controlling the coherent and incoherent processes, the intensity threshold of OB and OM can be modified. Also, it is found that the switching between OB and OM or vice versa can be occurred for some controllable parameters.
基金This work was supported by the“Light-Material Interactions in Energy Conversion”Energy Frontier Research Center funded by the U.S.Department of Energy,Office of Science,Office of Basic Energy Sciences under Award Number DE-AC02-05CH11231.
文摘Optical selection rules fundamentally determine the optical transitions between energy states in a variety of physical systems,from hydrogen atoms to bulk crystals such as gallium arsenide.These rules are important for optoelectronic applications such as lasers,energy-dispersive X-ray spectroscopy,and quantum computation.Recently,single-layer transition metal dichalcogenides have been found to exhibit valleys in momentum space with nontrivial Berry curvature and excitons with large binding energy.However,there has been little study of how the unique valley degree of freedom combined with the strong excitonic effect influences the nonlinear optical excitation.Here,we report the discovery of nonlinear optical selection rules in monolayer WS2,an important candidate for visible 2D optoelectronics because of its high quantum yield and large direct bandgap.We experimentally demonstrated this principle for second-harmonic generation and two-photon luminescence(TPL).Moreover,the circularly polarized TPL and the study of its dynamics evince a sub-ps interexciton relaxation(2p R 1s).The discovery of this new optical selection rule in a valleytronic 2D system not only considerably enhances knowledge in this area but also establishes a foundation for the control of optical transitions that will be crucial for valley optoelectronic device applications such as 2D valley-polarized THz sources with 2p–1s transitions,optical switches,and coherent control for quantum computing.
基金National Key Research and Development Program of China(Grant No.2017YFA0206000)eijing Natural Science Foundation(Grant No.Z180011)+1 种基金National Science Foundation of China(Grant Nos.12027807,12104241 and 61521004)roject funded by China Postdoctoral Science Foundation(Grant No.2019M660283)。
文摘Two dimensional excitonic devices are of great potential to overcome the dilemma of response time and integration in current generation of electron or/and photon based systems.The ultrashort diffusion length of exciton arising from ultrafast relaxation and low carrier mobility greatly discounts the performance of excitonic devices.Phonon scattering and exciton localization are crucial to understand the modulation of exciton flux in two dimensional disorder energy landscape,which still remain elusive.Here,we report an optimized scheme for exciton diffusion and relaxation dominated by phonon scattering and disorder potentials in WSe2 monolayers.The effective diffusion coefficient is enhanced by>200%at 280 K.The excitons tend to be localized by disorder potentials accompanied by the steadily weakening of phonon scattering when temperature drops to 260 K,and the onset of exciton localization brings forward as decreasing temperature.These findings identify that phonon scattering and disorder potentials are of great importance for long-range exciton diffusion and thermal management in exciton based systems,and lay a firm foundation for the development of functional excitonic devices.