报告题目：Electronic coherences built by an attopulse control electron-nuclei entanglement and the forces on the nuclei
报告人：Prof. Françoise Remacle
报告人单位：University of Liege
主持人：李辉 研究员
报告时间：2024年10月23日（周三）上午10:00
报告地点：光学大楼B325会议室
报告内容：
Short attosecond (as) or few femtoseconds (fs) pulses have a broad enough energy bandwidth for exciting a superposition of several electronic states in neutral molecules and molecular cations. This opens the way to engineering electronic coherences to steer charge migration through the selective localization the electronic density on its purely electronic time scale[1]. As the nuclei begin to move, the electronic and nuclear motions are entangled and the engineered electronic coherences can be usefully exploited for control by steering the vibronic density through the network of non adiabatic interactions to specific products.
I will discuss several examples illustrating the role of initial entanglement and the features of the force on the nuclei exerted by the vibronic wave packet after excitation with an attopulse, in the case of the fragmentation of diatomic molecules [2] and in making bonds in the photoinduced isomerization of norbornadiene into quadricyclane[3]. I will then report on the force on the nuclei and the stereodynamics, first in an ensemble of initially randomly oriented LiH molecules photoexcited by a short CEP controlled IR pulse[4]. Next, I will discuss our recent results on the forces driving the ultrafast Jahn-Teller structural rearrangement of the methane cation induced by XUV photoionization of an ensemble of neutral CH4 molecules to a superposition of the three lowest states of the cation[5].
[1] F. Remacle and R. D. Levine, Proc. Natl. Acad. Sci. USA 103, 6793-6798 (2006); F. Remacle, et al., Phys. Rev. Lett. 99 (18), 183902 (2007); B. Mignolet, et al., J. Phys. B: At. Mol. Opt. Phys. 47, 124011 (2014).
[2] M. Blavier, et al., Phys. Chem. Chem. Phys. 24, 17516-17525 (2022); M. Blavier, et al., Chem. Phys. Lett. 804, 139885 (2022);M. Cardosa-Gutierrez, R. D. Levine, and F. Remacle, J. Phys. B At. Mol. Opt. Phys. 57, 133501 (2024).
[3] A. Valentini, S. van den Wildenberg and F. Remacle, Phys. Chem. Chem. Phys. 22 (39), 22302-22313 (2020).
[4] M. Cardosa-Gutierrez, R. D. Levine, F. Remacle, J. Phys. Chem. A. 128, 2937-2947 (2024).
[5] C.E.M. Gonçalves, R.D. Levine, F. Remacle, Phys. Chem. Chem. Phys. 23 (2021) 12051-12059, M. Blavier, et al., J. Phys. Chem. A 125, 9495-9507 (2021)
报告人简介：
Prof. Françoise Remacle, Research Director of Fonds National de la Recherche Scientifique, is the Head of the Theoretical Physical Chemistry (TPC) group of the Chemistry Department of the University of Liège since 2001. She got her PhD at the University of Liège in 1990. She post-doc at the Hebrew University of Jerusalem, 1990-1991. She was elected as an academician of the Royal Belgian Academy of Art and Sciences, Class of Sciences since, 2023 and received the Emmy Noether Distinction for Women in Physic of the European Physical Society, Autumn-Winter 2017. She is a Fellow of the American Physical Society, 2009 since 2009. She is the vice-president of the Research and Valorization Council for Science and Technology of the University of Liege since 2020.Her research focuses on the theory and the modeling of the control of molecular responses to external perturbations (optical, electrical and mechanical), the design of new materials and information processing. In attochemistry, she predicted the existence of an ultrafast attosecond electronic time scale for charge migration and chemical processes that can be initiated and probed with attopulses (Proc. Natl. Acad. Sci. USA 103, 6793-6798 (2006)). Later, she was involved in the theoretical interpretation of experiments in molecular and nanosystems that characterized this attosecond time scale for charge migration (Science350, 790-795 (2015); Phys Rev Lett114, 123004 (2015)). She presently focuses on the control of chemical reactivity and electron-nuclei dynamics in molecular systems through their photoexcitation by atto and few femtosecond optical pulses.