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

ABSTRACT

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.

GRAPHICAL ABSTRACT

KEYWORDS:

• Acetylene
• polyad
• optimal control
• rovibrational
• Liouville space

Acknowledgements

L.S. is grateful to M. Godefroid for helpful suggestions and S. Gorza for helpful discussions. We also thank the COST XLIC and MOLIM actions. This work has been performed within the French GDR 3575 THEMS.

Disclosure statement

No potential conflict of interest was reported by the authors.

ORCID

L. Santos http://orcid.org/0000-0003-2484-9503

M. Desouter-Lecomte http://orcid.org/0000-0002-6199-7401

N. Vaeck http://orcid.org/0000-0003-0590-9646

Additional information

Funding

This work was supported by the Fonds De La Recherche Scientifique (FRS-FNRS) of Belgium [grant number I.I.S.N. 4.4504.10]. L.S. acknowledges an Fonds pour la Formation à la Recherche dans l'Industrie et dans l'Agriculture (F.R.I.A). research grant from the FRS-FNRS of Belgium. This institution is also thanked by M.D.-L. for a grant.