Frequency combs enable rapid and high-resolution multidimensional coherent spectroscopy

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.