[en] Attopulses have an energy bandwidth broad enough to coherently excite several electronic states of molecules. Towards the control of chemical reactivity by attopulses we derive the quantum mechanical expression for the force exerted on the nuclei in such a vibronic wave packet both during and after the exciting pulse. Tuning the pulse parameters allows accessing specific electronic coherences that determine the force strength and direction during and after the pulse. Following the pulse, the force due to the non adiabatic interactions accelerates or slows down the motion of the vibronic wave packet on the excited electronic states and its sign controls the direction of population transfer. Computational results for the LiH and LiT molecules and the probing by the emission dipole are discussed.
Levine, R.D.; Fritz Haber Center, Institute of Chemistry, The Hebrew University of Jerusalem, Jerusalem, Israel ; Department of Molecular and Medical Pharmacology, David Geffen School of Medicine, University of California, Los Angeles, United States ; Department of Chemistry and Biochemistry, University of California, Los Angeles, United States
Remacle, Françoise ; Université de Liège - ULiège > Département de chimie (sciences) > Laboratoire de chimie physique théorique ; Fritz Haber Center, Institute of Chemistry, The Hebrew University of Jerusalem, Jerusalem, Israel
Language :
English
Title :
Electronic coherences built by an attopulse control the forces on the nuclei
Publication date :
12 July 2024
Journal title :
Journal of Physics : B Atomic Molecular and Optical Physics
F.R.S.-FNRS - Fonds de la Recherche Scientifique COST - European Cooperation in Science and Technology
Funding number :
T0205.20; CA18222
Funding text :
The authors acknowledge support from the COST action ATTOCHEM (CA18222). F R and M C G acknowledge the support of the Fonds National de la Recherche (F.R.S.-FNRS, Belgium), #T0205.20, and of the action of concerted research MECHANOCHEM (ARC 19/23-20, ULiege). Computational resources have been provided by the Consortium des Equipements de Calcul Intensif (CECI), funded by the F.R.S.-FNRS under Grant # 2.5020.11.
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