A singlet diatomic molecule naturally carries doubly degenerate ±Λ states when the projection of the total electronic angular momentum onto the internuclear axis is nonzero. These doubly degenerate states contri...A singlet diatomic molecule naturally carries doubly degenerate ±Λ states when the projection of the total electronic angular momentum onto the internuclear axis is nonzero. These doubly degenerate states contribute equally in conventional measurements and are thus treated the same in corresponding simulations. In this study, we demonstrate that in resonant excitation by intense laser pulses, the doubly degenerate ±Λ states must be clearly identified. This is exemplified in the X^(1)Σ → A^(1)Π transition of CO molecules. This distinction becomes especially important in the case of circularly polarized radiation. We attribute this phenomenon to the interference of electron-rotational pathways in the strong-field coupled transition with the ±Λ-state of the excited Π state. This research sheds light on the fundamental aspects of intense laser-molecule interactions when extending conventional theories.展开更多
It has been reported that electron-rotation coupling plays a significant role in diatomic nuclear dynamics induced by intense VUV pulses [Phys. Rev. A 102(2020) 033114;Phys. Rev. Res. 2(2020) 043348]. As a further ste...It has been reported that electron-rotation coupling plays a significant role in diatomic nuclear dynamics induced by intense VUV pulses [Phys. Rev. A 102(2020) 033114;Phys. Rev. Res. 2(2020) 043348]. As a further step, we present here investigations of the electron-rotation coupling effect in the presence of Auger decay channel for core-excited molecules, based on theoretical modeling of the total electron yield(TEY), resonant Auger scattering(RAS) and x-ray absorption spectra(XAS) for two showcases of CO and CH^(+) molecules excited by resonant intense x-ray pulses. The Wigner D-functions and the universal transition dipole operators are introduced to include the electron-rotation coupling for the core-excitation process. It is shown that with the pulse intensity up to 10^(16) W/cm^(2), no sufficient influence of the electron-rotation coupling on the TEY and RAS spectra can be observed. This can be explained by a suppression of the induced electron-rotation dynamics due to the fast Auger decay channel, which does not allow for effective Rabi cycling even at extreme field intensities,contrary to transitions in optical or VUV range. For the case of XAS, however, relative errors of about 10% and 30% are observed for the case of CO and CH^(+), respectively, when the electron-rotation coupling is neglected.It is concluded that conventional treatment of the photoexcitation, neglecting the electron-rotation coupling,can be safely and efficiently employed to study dynamics at the x-ray transitions by means of electron emission spectroscopy, yet the approximation breaks down for nonlinear processes as stimulated emission, especially for systems with light atoms.展开更多
As x-ray probe pulses approach the subfemtosecond range,conventional x-ray photoelectron spectroscopy(XPS)is expected to experience a reduction in spectral resolution due to the effects of the pulse broadening.However...As x-ray probe pulses approach the subfemtosecond range,conventional x-ray photoelectron spectroscopy(XPS)is expected to experience a reduction in spectral resolution due to the effects of the pulse broadening.However,in the case of resonant x-ray photoemission,also known as resonant Auger scattering(RAS),the spectroscopic technique maintains spectral resolution when an x-ray pulse is precisely tuned to a core-excited state.We present theoretical simulations of XPS and RAS spectra on a showcased CO molecule using ultrashort x-ray pulses,revealing significantly enhanced resolution in the RAS spectra compared to XPS,even in the subfemtosecond regime.These findings provide a novel perspective on potential utilization of attosecond x-ray pulses,capitalizing on the well-established advantages of detecting electron signals for tracking electronic and molecular dynamics.展开更多
基金supported by the National Natural Science Foundation of China(Grant No.12374238)the Postdoctoral Science Foundation of Shaanxi Province (Grant No.2024BSHSDZZ148)Ministry of Science and Higher Education of Russian Federation (Grant No.FSRZ 2023-0006)。
文摘A singlet diatomic molecule naturally carries doubly degenerate ±Λ states when the projection of the total electronic angular momentum onto the internuclear axis is nonzero. These doubly degenerate states contribute equally in conventional measurements and are thus treated the same in corresponding simulations. In this study, we demonstrate that in resonant excitation by intense laser pulses, the doubly degenerate ±Λ states must be clearly identified. This is exemplified in the X^(1)Σ → A^(1)Π transition of CO molecules. This distinction becomes especially important in the case of circularly polarized radiation. We attribute this phenomenon to the interference of electron-rotational pathways in the strong-field coupled transition with the ±Λ-state of the excited Π state. This research sheds light on the fundamental aspects of intense laser-molecule interactions when extending conventional theories.
基金Supported by the National Natural Science Foundation of China (Grant Nos.11934004,11974230,and 11904192)the Education of Russian Federation (Grant No.FSRZ-2020-0008)。
文摘It has been reported that electron-rotation coupling plays a significant role in diatomic nuclear dynamics induced by intense VUV pulses [Phys. Rev. A 102(2020) 033114;Phys. Rev. Res. 2(2020) 043348]. As a further step, we present here investigations of the electron-rotation coupling effect in the presence of Auger decay channel for core-excited molecules, based on theoretical modeling of the total electron yield(TEY), resonant Auger scattering(RAS) and x-ray absorption spectra(XAS) for two showcases of CO and CH^(+) molecules excited by resonant intense x-ray pulses. The Wigner D-functions and the universal transition dipole operators are introduced to include the electron-rotation coupling for the core-excitation process. It is shown that with the pulse intensity up to 10^(16) W/cm^(2), no sufficient influence of the electron-rotation coupling on the TEY and RAS spectra can be observed. This can be explained by a suppression of the induced electron-rotation dynamics due to the fast Auger decay channel, which does not allow for effective Rabi cycling even at extreme field intensities,contrary to transitions in optical or VUV range. For the case of XAS, however, relative errors of about 10% and 30% are observed for the case of CO and CH^(+), respectively, when the electron-rotation coupling is neglected.It is concluded that conventional treatment of the photoexcitation, neglecting the electron-rotation coupling,can be safely and efficiently employed to study dynamics at the x-ray transitions by means of electron emission spectroscopy, yet the approximation breaks down for nonlinear processes as stimulated emission, especially for systems with light atoms.
基金supported by the National Natural Science Foundation of China(Grant Nos.11934004 and 11974230)Russian Science Foundation(Grant No.21-12-00193)。
文摘As x-ray probe pulses approach the subfemtosecond range,conventional x-ray photoelectron spectroscopy(XPS)is expected to experience a reduction in spectral resolution due to the effects of the pulse broadening.However,in the case of resonant x-ray photoemission,also known as resonant Auger scattering(RAS),the spectroscopic technique maintains spectral resolution when an x-ray pulse is precisely tuned to a core-excited state.We present theoretical simulations of XPS and RAS spectra on a showcased CO molecule using ultrashort x-ray pulses,revealing significantly enhanced resolution in the RAS spectra compared to XPS,even in the subfemtosecond regime.These findings provide a novel perspective on potential utilization of attosecond x-ray pulses,capitalizing on the well-established advantages of detecting electron signals for tracking electronic and molecular dynamics.
