Rovibrational laser control targeting a dark state in acetylene. Simulation in the Ns = 1, Nr = 5 Ns=1,Nr=5 polyad

Optimal control theory in the Liouville space is used to perform rovibrational control by means of a
laser pulse in a polyad of acetylene in order to populate a dark vibrational state. The initial mixed state
is a truncated Boltzmann distribution of rotational levels from J=27 to J=31 of the ground vibrational
state. The target state is a rotational equidistribution of levels ranging from J=28 to J=32 of
the first excited vibrational dark state including quanta of energy in each bending modes, with positive
vibrational angular momenta. The simulation is performed by using a manifold of eigenstates of
a full-dimensional Hamiltonian calibrated by high precision spectroscopy known as the global acetylene
Hamiltonian [B. Amyay et al., J. Chem. Phys. 131, 114301 (2009)]. The control is successful as an
Uhlmann’s fidelity of 0.98 is reached.