A test of optimal laser impulsion for controlling population within the $N_s=1$, $N_r=5$ polyad of $^{12}C_2H_2$

TL;DR

This study uses optimal control theory to design simple laser pulses that effectively populate dark states in the acetylene polyad, highlighting a promising target for experimental realization due to high population stability and low decoherence.

Contribution

It demonstrates the application of optimal control to selectively excite dark states in a polyad of acetylene using experimentally derived parameters.

Findings

Optimal pulses are simple and effective.

One dark state maintains high population with minimal decoherence.

Potential for experimental validation of the targeted dark state.

Abstract

Optimal control theory has been employed to populate separately two dark states of the acetylene polyad $N_s=1$, $N_r=5$ by indirect coupling via the ground state. Relevant level energies and transition dipole moments are extracted from the experimental literature. The optimal pulses are rather simple. The evolution of the populations is shown for the duration of the control process and also for the field free-evolution that follows the control. One of the dark states appears to be a potential target for realistic experimental investigation because the average population of the Rabi oscillation remains high and decoherence is expected to be weak.