Cooling molecular vibrations with shaped laser pulses: Optimal control theory exploiting the timescale separation between coherent excitation and spontaneous emission

Abstract

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 deexcitation steps whose timescales are separated.

References in corpus (10)

• Optical pumping and vibrational cooling of molecules
• Monotonically convergent optimization in quantum control using Krotov's method
• The X${}^1{\Sigma }^{+}$ and a${}^3{\Sigma }^{+}$ states of LiCs studied by Fourier-transform spectroscopy
• Rovibrational cooling of molecules by optical pumping
• Steering the optimization pathway in the control landscape using constraints
• Optical pulse-shaping for internal cooling of molecules
• Triplet-singlet conversion by broadband optical pumping
• Laser cooling of rotation and vibration by optical pumping
• The dynamics of three-level $\Lambda$-type system driven by the trains of ultrashort laser pulses
• Impact of Decoherence on Internal State Cooling using Optical Frequency Combs

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