Dual-comb spectroscopy of molecular electronic transitions in condensed phases

Dual-comb spectroscopy (DCS) utilizes two phase-locked optical frequency combs to allow scanless acquisition of spectra using only a single point detector. Although recent DCS measurements demonstrate rapid acquisition of absolutely calibrated spectral lines with unprecedented precision and accuracy, complex phase-locking schemes and multiple coherent averaging present significant challenges for widespread adoption of DCS. Here, we demonstrate Global Positioning System (GPS) disciplined DCS of a molecular electronic transition in solution at around 800 nm, where the absorption spectrum is recovered by using a single time-domain interferogram. We anticipate that this simplified dual-comb technique with absolute time interval measurement and ultrabroad bandwidth will allow adoption of DCS to tackle molecular dynamics investigation through its implementation in time-resolved nonlinear spectroscopic studies and coherent multidimensional spectroscopy of coupled chromophore systems.