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Conference on Lasers and Electro-Optics

Two-Dimensional Fourier-Transform Spectroscopy of Potassium Vapor

Xingcan Dai, Alan D. Bristow, D. Karaiskaj, Steven T. Cundiff

Published Jan 1, 2010• 21 citations
Publisher

Abstract

Various two-dimensional Fourier-transform spectra of potassium vapor have been obtained to show coherent interactions and isolate Raman-like coherences. The experimental results agree well with numerical calculation based on optical Bloch equations.
DOI
10.1364/qels.2010.qfj7

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Optical two-dimensional Fourier-transform (2DFT) spectroscopy is used to study the coherent optical response of potassium vapor in a thin transmission cell. Rephasing and nonrephasing spectra of the D1{D}_{1}D1​ and D2{D}_{2}D2​ transitions are obtained and compared to numerical simulations. Non-perturbative calculations using the optical Bloch equations give very good agreement with the experimental peak strengths and line shapes. Nonradiative Raman-like coherences are isolated using a different 2DFT projection. Comparison between the optical and Raman linewidths shows that dephasing is due to partially correlated energy fluctuations. Density-dependent measurements show distortion of 2DFT spectra due to pulse propagation effects.
Electronic structure and dynamics are captured by optical 2D-Fourier-transform (2DFT) spectroscopy, which tracks the phase of the nonlinear signal during two time delays of a multi-pulse excitation sequence. These Fourier-transformed spectra separate and isolate overlapping and competing contributions to the coherent response. We have developed an ultra-stable platform consisting of nested interferometers with active phase control, allowing for exploration of single- and two-quantum coherences. Phase-resolved spectra are retrieved by all-optical determination of experimental phase ambiguities. GaAs quantum wells show suppression of many-body interactions in cross-linear polarized 2DFT spectra and many-body two-quantum coherences. Potassium vapor also shows unexpected two-quantum coherences.