Optimal single-pulse excitation of rotational impulsive molecular phase modulation.
The full transient macroscopic linear optical susceptibility tensor induced in a transiently aligned molecular gas by a single, linearly polarized intense alignment pulse is studied. We determine the optimal properties of the pulse that forms the rotational wave packet. Significantly, we demonstrate that the optimal pulse for phase modulation differs from the optimal alignment pulse. Finally, we show that the limited information about rotational wave packets obtained by measuring the linear optical susceptibility can be augmented by also measuring the time-varying nonlinear optical susceptibilities.
Masihzadeh
Omid
O
Baertschy
Mark
M
Bartels
Randy A
RA