Frequency combs enable rapid and high-resolution multidimensional coherent spectroscopy

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Science  29 Sep 2017:
Vol. 357, Issue 6358, pp. 1389-1391
DOI: 10.1126/science.aao1090

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Comb quickly through a spectral zoo

Dual-comb spectroscopy relies on a pair of laser pulses with multiple frequencies distributed like tines in a comb. It is a rapid means of characterizing atoms and molecules in fine detail, but, when applied to complex mixtures, it can produce a sea of peaks that are hard to discriminate. Lomsadze and Cundiff present a protocol to extend dual comb spectroscopy into the nonlinear regime. The cross-peaks that appear in the resulting two-dimensional spectra allow assignment of crowded features to common sources, as demonstrated for an isotopic mixture of 87Rb and 85Rb.

Science, this issue p. 1389


Dual laser frequency combs can rapidly measure high-resolution linear absorption spectra. However, one-dimensional linear techniques cannot distinguish the sources of resonances in a mixture of different analytes, nor can they separate inhomogeneous and homogeneous broadening. Here, we overcame these limitations by acquiring high-resolution multidimensional nonlinear coherent spectra with frequency combs. We experimentally differentiated and assigned the Doppler-broadened features of two naturally occurring isotopes of rubidium atoms (87Rb and 85Rb) according to the placement of their hyperfine energy states in a two-dimensional spectrum.

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