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Physical Review A

Quantum control in two-dimensional Fourier-transform spectroscopy

Jongseok Lim, Han-gyeol Lee, Sangkyung Lee, Jaewook Ahn

Published Jul 28, 2011• 9 citations
Publisher

Abstract

We present a method that harnesses coherent control capability to two-dimensional Fourier-transform optical spectroscopy. For this, three ultrashort laser pulses are individually shaped to prepare and control the quantum interference involved in two-photon interexcited-state transitions of a $\mathsf{V}$-type quantum system. In experiments performed with atomic rubidium, quantum control for the enhancement and reduction of the 5$P$${}_{1/2}\ensuremath{\rightarrow}$ 5$P$${}_{3/2}$ transition was successfully tested in which the engineered transitions were distinguishably extracted in the presence of dominant one-photon transitions.

DOI
10.1103/physreva.84.013425

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We present a method that harnesses coherent control capability to two-dimensional Fourier-transform optical spectroscopy. For this, three ultrashort laser pulses are individually shaped to prepare and control the quantum interference involved in two-photon interexcited-state transitions of a V\mathsf{V}V-type quantum system. In experiments performed with atomic rubidium, quantum control for the enhancement and reduction of the 5P$${}_{1/2}\ensuremath{\rightarrow} 5P$${}_{3/2} transition was successfully tested in which the engineered transitions were distinguishably extracted in the presence of dominant one-photon transitions.
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We investigate coherent control of the two-photon transition pathways of a four-level atomic system in a diamond configuration. When an ultrashort laser pulse interacts with this system in the ground state 5S1/25{S}_{1/2}5S1/2​ of rubidium, the two-photon transition probability amplitude of 5D3/25{D}_{3/2}5D3/2​ is obtained by a summation of all possible resonant and nonresonant two-photon transition probability amplitudes via 5P1/25{P}_{1/2}5P1/2​ and 5P3/25{P}_{3/2}5P3/2​. Second-order perturbation theory predicts that the maximal constructive interference of the transition probability amplitudes occurs when the phases of eight different spectrum blocks satisfy four different phase relations. Experiments carried out with spectrally phase-coded laser pulses show good agreement with the theoretical prediction.