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We investigated the roles of one-photon and two-photon processes in the laser-controlled rovibrational transitions of the diatomic alkali halide, 7Li37Cl. Optimal control theory calculations were carried out using the Hamiltonian, including both the one-photon and two-photon field-molecule interaction terms. Time-dependent wave packet propagation was performed with both the radial and angular motions being treated quantum mechanically. The targeted processes were pure rotational and vibrational–rotational excitations: (v = 0, J = 0) → (v = 0, J = 2); (v = 0, J = 0) → (v = 1, J = 2). Total time of the control pulse was set to 2,000,000 atomic units (48.4 ps). In each control excitation process, weak and strong optimal fields were obtained by means of giving weak and strong field amplitudes, respectively, to the initial guess for the optimal field. It was found that when the field is weak, the control mechanism is dominated exclusively by a one-photon process, as expected, in both the targeted processes. When the field is strong, we obtained two kinds of optimal fields, one causing two-photon absorption and the other causing a Raman process. It was revealed, however, that the mechanisms for strong fields are not simply characterized by one process but rather by multiple one- and two-photon processes. It was also found that in the rotational excitation, (v = 0, J = 0) → (v = 0, J = 2), the roles of one- and two-photon processes are relatively distinct but in the vibrational–rotational excitation, (v = 0, J = 0) → (v = 1, J = 2), these roles are ambiguous and the cooperative effect associated with these two processes is quite large.

Quantum Optimal Control of Rovibrational Excitations of a Diatomic Alkali Halide: One-Photon vs. Two-Photon Processes