Abstract
ABSTRACTA theoretical approach for simulating the laser-induced alignment dynamics of non-rigid polyatomic molecules is introduced, in which the time-dependent Schrödinger equation (TDSE) is solved by expanding the laser-induced wavepacket with the field-free rovibrational eigenstates of the system. It is shown that not only the exact solution of the TDSE but also its approximated solution can be obtained, depending on the choices of the method for determining the field-free eigenstates. Laser-induced alignment of weakly bound H2He+ is investigated by adopting the present approach with high-accuracy full-dimensional variational calculations of the nuclear dynamics.
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