Isomerization HCN → HNC in the electronic ground state using chirp-optimized mid-IR laser pulses: 4D quantum dynamics

This Hamiltonian reproduces the known exact quantized rovibrational states, including Coriolis coupling. We study the laser-induced dynamics using linearly chirped mid-IR laser pulses with a temporal duration of ≃ 1 picosecond.

The initial state is the vibrational ground state of HCN with J = K = 0, where K is the quantum number associated with vibrational angular momentum and the rotation of H around the CN axis. Over-barrier excitation via fundamental or first overtone bending modes is studied. An optimized pump-dump pulse, which is fully tailored for a fixed χ angle is also employed and leads to considerable isomerization.