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Quantum control study of ultrafast isotope-selective vibrational excitations of the cesium iodide (CsI) molecule

Kurosaki, Yuzuru; Yokoyama, Keiichi  ; Yokoyama, Atsushi

We study, using quantum optimal control theory (OCT), isotope-selective vibrational excitations on the ground-state potential energy curve for the mixture of two pure ensembles for $$^{133}$$CsI and $$^{135}$$CsI. Initial states are set to the condition that both $$^{133}$$CsI and $$^{135}$$CsI are in the vibrational ground level, i.e., ($$v$$$$_{133}$$, $$v$$$$_{135}$$) = (0, 0), and target states are set to three: ($$v$$$$_{133}$$, $$v$$$$_{135}$$) = (0, 2), (0, 3), and (0, 4), where molecular orientations are fixed parallel to the field polarization vector. Three total times (i.e., pulse durations), T = 460,000 au, 920,000 au, and 1,840,000 au, are set in the calculations and nine cases for the combination of target state and total time are investigated. It is suggested from the computational results that even when T is short, high-yield transitions into energetically-separated target states are possible through excitations skipping over more than one vibrational level at a time with intense fields including high overtones.

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Category:Chemistry, Physical

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