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Optics Communications

Theory of molecular pulsed excitation with spontaneous emission

Wai Keung Lai, Stig Stenholm

Published Jan 1, 1994• 6 citations
Publisher
DOI
10.1016/0030-4018(94)90562-2

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Laser cooling of molecules employing broadband optical pumping involves a timescale separation between laser excitation and spontaneous emission. Here, we optimize the optical pumping step using shaped laser pulses. We derive two optimization functionals to drive population into those excited state levels that have the largest spontaneous emission rates to the target state. We show that, when using optimal control, laser cooling of molecules works even if the Franck–Condon map governing the transitions is preferential to heating rather than cooling. Our optimization functional is also applicable to the laser cooling of other degrees of freedom provided the cooling cycle consists of coherent excitation and dissipative de-excitation steps whose timescales are separated.
We present an experimentally viable approach for suppressing the spontaneous emission in several atomic and molecular systems. We have shown [E. Frishman and M. Shapiro, Phys. Rev. Lett. 87, 253001 (2001)] that a coherent excitation of overlapping resonances followed by the application of infrequent interruptions can result in complete suppression of spontaneous emission. In the present work, the overlapping resonances result from splitting a single resonance with an external (spectator) field. An optimized superposition of the two components is formed by a shaped pulse excitation from the ground state.
Optimal control theory is applied to laser cooling of molecules. The objective is to cool vibrations, using shaped pulses synchronized with the spontaneous emission. The optimal mechanism is found to operate by a “vibrationally selective coherent population trapping”. The trapping condition is that the instantaneous phase of the laser is locked to the phase of the transition dipole moment of v=0 with the excited population. The molecules that reach v=0 by spontaneous emission are then trapped, while the others are continually repumped.