The A^1Π→ X^1Σ^+ transition system of aluminium monochloride is determined by using ab initio quantum chemistry.Based on the multi-reference configuration interaction method in conjugate to the Davidson correction(...The A^1Π→ X^1Σ^+ transition system of aluminium monochloride is determined by using ab initio quantum chemistry.Based on the multi-reference configuration interaction method in conjugate to the Davidson correction(MRCI + Q), the potential energy curves(PECs) of the three electronic states are obtained. Transition dipole moments(TDMs) and the vibrational energy levels are studied by employing the aug-cc-pwCV5Z-DK basis set with 4220-active space. The rovibrational constants are first determined from the analytic potential by solving the rovibrational Schr ¨odinger equation, and then the spectroscopic constants are determined by fitting the vibrational levels, and these values are well consistent with the experimental data. The effect of spin–orbit coupling(SOC) on the spectra and vibrational properties are evaluated.The results show that the SOC effect has almost no influence on the spectroscopic constants of AlCl molecules. For the A^1Π→ X^1Σ^+transition, the highly diagonalized Frank–Condon factor(FCF) is f(00)=0.9988. Additionally, Einstein coefficients and radiative lifetimes are studied, where the vibrational bands include ν''= 0–19→ν'=0–9. The ro-vibrational intensity is calculated at a temperature of 296 K, which can have certain astrophysical applications. At present, there is no report on the calculation of Al Cl ro-vibrational intensity, so we hope that our results will be useful in analyzing the interstellar Al Cl based on the absorption from A^1Π→ X^1Σ^+.展开更多
Two-photon fluorescence dyes have shown promising applications in biomedical imaging.However,the substitution site effect on geometric structures and photophysical properties of fluorescence dyes is rarely illustrated...Two-photon fluorescence dyes have shown promising applications in biomedical imaging.However,the substitution site effect on geometric structures and photophysical properties of fluorescence dyes is rarely illustrated in detail.In this work,a series of new lipid droplets detection dyes are designed and studied,molecular optical properties and non-radiative transitions are analyzed.The intramolecular weak interaction and electron-hole analysis reveal its inner mechanisms.All dyes are proven to possess excellent photophysical properties with high fluorescence quantum efficiency and large stokes shift as well as remarkable two-photon absorption cross section.Our work reasonably elucidates the experimental measurements and the effects of substitution site on two-photon absorption and excited states properties of lipid droplets detection NAPBr dyes are highlighted,which could provide a theoretical perspective for designing efficient organic dyes for lipid droplets detection in biology and medicine fields.展开更多
Correlation and relativistic effects are both needed for accurate atomic structure calculations of energy levels and their atomic properties. For transition probabilities of radiative transitions between low-lying lev...Correlation and relativistic effects are both needed for accurate atomic structure calculations of energy levels and their atomic properties. For transition probabilities of radiative transitions between low-lying levels of an atom or ion, accurate wave functions for the outer region of are required. For lighter atoms, relativistic effects can be included through the Breit-Pauli approximation. This paper outlines the advances in the treatment of correlation and describes the current state of Breit-Pauli calculations for complex systems.展开更多
基金Project supported by the National Natural Science Foundation of China(Grant No.61705182)。
文摘The A^1Π→ X^1Σ^+ transition system of aluminium monochloride is determined by using ab initio quantum chemistry.Based on the multi-reference configuration interaction method in conjugate to the Davidson correction(MRCI + Q), the potential energy curves(PECs) of the three electronic states are obtained. Transition dipole moments(TDMs) and the vibrational energy levels are studied by employing the aug-cc-pwCV5Z-DK basis set with 4220-active space. The rovibrational constants are first determined from the analytic potential by solving the rovibrational Schr ¨odinger equation, and then the spectroscopic constants are determined by fitting the vibrational levels, and these values are well consistent with the experimental data. The effect of spin–orbit coupling(SOC) on the spectra and vibrational properties are evaluated.The results show that the SOC effect has almost no influence on the spectroscopic constants of AlCl molecules. For the A^1Π→ X^1Σ^+transition, the highly diagonalized Frank–Condon factor(FCF) is f(00)=0.9988. Additionally, Einstein coefficients and radiative lifetimes are studied, where the vibrational bands include ν''= 0–19→ν'=0–9. The ro-vibrational intensity is calculated at a temperature of 296 K, which can have certain astrophysical applications. At present, there is no report on the calculation of Al Cl ro-vibrational intensity, so we hope that our results will be useful in analyzing the interstellar Al Cl based on the absorption from A^1Π→ X^1Σ^+.
基金This work was supported by the National Natural Science Foundation of China(No.11804196 and No.11904210)the Project funded by China Postdoctoral Science Foundation(No.2018M642689)the Open Fund of Guangdong Provincial Key Laboratory of Luminescence from Molecular Aggregates,(South China University of Technology)(No.2019B030301003).
文摘Two-photon fluorescence dyes have shown promising applications in biomedical imaging.However,the substitution site effect on geometric structures and photophysical properties of fluorescence dyes is rarely illustrated in detail.In this work,a series of new lipid droplets detection dyes are designed and studied,molecular optical properties and non-radiative transitions are analyzed.The intramolecular weak interaction and electron-hole analysis reveal its inner mechanisms.All dyes are proven to possess excellent photophysical properties with high fluorescence quantum efficiency and large stokes shift as well as remarkable two-photon absorption cross section.Our work reasonably elucidates the experimental measurements and the effects of substitution site on two-photon absorption and excited states properties of lipid droplets detection NAPBr dyes are highlighted,which could provide a theoretical perspective for designing efficient organic dyes for lipid droplets detection in biology and medicine fields.
文摘Correlation and relativistic effects are both needed for accurate atomic structure calculations of energy levels and their atomic properties. For transition probabilities of radiative transitions between low-lying levels of an atom or ion, accurate wave functions for the outer region of are required. For lighter atoms, relativistic effects can be included through the Breit-Pauli approximation. This paper outlines the advances in the treatment of correlation and describes the current state of Breit-Pauli calculations for complex systems.
