Full quantum calculations are performed to investigate the broadening profiles of the atomic lithium Li（2s-2p） resonance line induced by interactions with ground Ne（2s^22p^6） perturbers in the spectral wings and c...Full quantum calculations are performed to investigate the broadening profiles of the atomic lithium Li（2s-2p） resonance line induced by interactions with ground Ne（2s^22p^6） perturbers in the spectral wings and core. The X^2Σ~＋, A^2Π,and B^2Σ~＋ potential-energy curves of the two first low lying Li Ne molecular states, as well as the corresponding transition dipole moments, are determined with ab initio methods based on the SA-CASSCF-MRCI calculations. The emission and absorption coefficients in the wavelength range 550-800 nm and the line-core width and shift are investigated theoretically for temperatures ranging from 130 K to 3000 K. Their temperature dependence is analyzed, and the obtained results are compared with the previous experimental measurements and theoretical works.展开更多
The realization of colloidal alloy quantum dots(QDs)with narrow spectral linewidths requires minimization of the contributions of inhomogeneous and homogeneous broadening to the ensemble spectrum.Recently,there has be...The realization of colloidal alloy quantum dots(QDs)with narrow spectral linewidths requires minimization of the contributions of inhomogeneous and homogeneous broadening to the ensemble spectrum.Recently,there has been remarkable progress in eliminating the inhomogeneous contribution by controlling the size distribution of the QDs.However,considerable challenges remain in suppressing the homogeneous broadening,in terms of both intrinsic principles and rational synthetic routes.We find that ground-state exciton fine structure splitting and exciton-phonon coupling play a pivotal role in the homogeneous broadening mechanism.Here we demonstrate that the elimination of the lattice mismatch strain by using a coherent strain structure can decrease the light-heavy hole splitting,thus suppressing the asymmetric broadening of the emission on the high energy side.Besides,the improvement of the uniformity of the alloy by using a stepwise ion exchange strategy can weaken the exciton-longitudinal optical(LO)-phonon interactions,further minimizing the homogeneous broadening.As a result,the final alloy QD products exhibit a widely tunable blue emission wavelength(445-470 nm)with the narrowest ensemble photoluminescence full width at half maximum(FWHM)of 10.1-13.5 nm(or 58.4-75.3 meV).Our study provides a potential strategy for other semiconductor nanocrystals with ultranarrow spectral linewidths.展开更多
文摘Full quantum calculations are performed to investigate the broadening profiles of the atomic lithium Li（2s-2p） resonance line induced by interactions with ground Ne（2s^22p^6） perturbers in the spectral wings and core. The X^2Σ~＋, A^2Π,and B^2Σ~＋ potential-energy curves of the two first low lying Li Ne molecular states, as well as the corresponding transition dipole moments, are determined with ab initio methods based on the SA-CASSCF-MRCI calculations. The emission and absorption coefficients in the wavelength range 550-800 nm and the line-core width and shift are investigated theoretically for temperatures ranging from 130 K to 3000 K. Their temperature dependence is analyzed, and the obtained results are compared with the previous experimental measurements and theoretical works.
基金We gratefully acknowledge the financial support of the Natural Science Foundation of China(No.12174169)the Natural Science Foundation of Guangdong Province(Nos.2021A1515012292 and 2022A1515012448)+5 种基金the Scientific Research Foundation of the Higher Education Institutions of Guangdong Province(Nos.2019KCXTD012,2020ZDZX3034,2019KZDZX2008,and 2020ZDZX2055)the Natural Science Foundation of Jiangxi Province(Nos.20192ACBL21045 and 20181BBE50022)the Talent Project of Lingnan Normal University(Nos.ZL2021029 and ZL2021030)the Science and Technology Plan Project of Zhanjiang(Nos.2020B01085,2021A05233,2020A03003,and 2021A05042)the Young Innovative Talents Project of University of Guangdong Province(No.2018KQNCX153)the Yanling Outstanding Yong Teacher Training Program Funded Project of Lingnan Normal University(No.YL20200102).
文摘The realization of colloidal alloy quantum dots(QDs)with narrow spectral linewidths requires minimization of the contributions of inhomogeneous and homogeneous broadening to the ensemble spectrum.Recently,there has been remarkable progress in eliminating the inhomogeneous contribution by controlling the size distribution of the QDs.However,considerable challenges remain in suppressing the homogeneous broadening,in terms of both intrinsic principles and rational synthetic routes.We find that ground-state exciton fine structure splitting and exciton-phonon coupling play a pivotal role in the homogeneous broadening mechanism.Here we demonstrate that the elimination of the lattice mismatch strain by using a coherent strain structure can decrease the light-heavy hole splitting,thus suppressing the asymmetric broadening of the emission on the high energy side.Besides,the improvement of the uniformity of the alloy by using a stepwise ion exchange strategy can weaken the exciton-longitudinal optical(LO)-phonon interactions,further minimizing the homogeneous broadening.As a result,the final alloy QD products exhibit a widely tunable blue emission wavelength(445-470 nm)with the narrowest ensemble photoluminescence full width at half maximum(FWHM)of 10.1-13.5 nm(or 58.4-75.3 meV).Our study provides a potential strategy for other semiconductor nanocrystals with ultranarrow spectral linewidths.
