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Journal of Modern Optics

Phase control in coherent population distribution in molecules

Avijit Datta

Published Jan 30, 2018• 4 citations
Publisher

Abstract

A chirped laser pulse transfers population from one level to another level accessible by one photon dipole transition. We have used a pair of phase-locked chirped pulses of same frequency instead of a single chirped pulse to achieve phase control over the population transfer and thus creating coherent population distribution in hydrogen molecule. Simultaneous actions of the phase controlled interference and rapid adiabatic passages due to chirped pulses lead to the control in population transfer from the ground X(v = 0, j = 0) level to the C(v = 2, j = 1) level. We have extended this two-level system to a three-level 1 + 1 ladder system for population transfer from the X level to the J(v = 2, j = 2) level via the C intermediate level using two pairs of phase-locked laser chirped pulses and have achieved laudable control over the coherent population distribution.

DOI
10.1080/09500340.2018.1427289

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We propose and experimentally demonstrate the method of population transfer by piecewise adiabatic passage between two quantum states. Coherent excitation of a two-level system with a train of ultrashort laser pulses is shown to reproduce the effect of an adiabatic passage, conventionally achieved with a single frequency-chirped pulse. By properly adjusting the amplitudes and phases of the pulses in the excitation pulse train, we achieve complete and robust population transfer to the target state. The piecewise nature of the process suggests a possibility for the selective population transfer in complex quantum systems.
We propose a selective, efficient, and robust way to realize control of coherent population transfer in a $\ensuremath{\Lambda}$-type four-level system with a closely spaced doublet in the final state with time-separated chirped pump pulse and Stokes pulse pair by merging stimulated Raman adiabatic passage, temporal coherent control, and chirped adiabatic passage techniques. Moreover, an arbitrary coherent superposition between the final doublet, or between the intermediate state and either of the doublets can be created. This method holds the ability to ``control with control'' and has potential applications in coherent control of chemical reactions and quantum information processing.