Rapid acquisition of broadband two-dimensional electronic spectra by continuous scanning with conventional delay...

A passively phase-stable, broadband (∼7fs, >2000cm^-1) two-dimensional (2D) electronic spectroscopy apparatus that achieves rapid acquisition rates by continuously-rather than step-wise-scanning the Fourier-transform dimension is demonstrated for the first time, to the best of our knowledge. This is made possible through use of a partially common path interferometer design in which the coherence time τ is sampled in a "rotating frame." Rapid, continuous scanning of τ increases the duty cycle of signal collection, rejects the majority of excitation pulse scatter, and enables the measurement of a complete 2D spectrum in 92 ms, which minimizes the influence of pulse intensity and delay fluctuations on the 2D spectrum. In practice, these improvements make possible the acquisition of hundreds of 2D spectra in tens of minutes, which opens the door to dense sampling of ultrafast relaxation dynamics and to generating extremely broadband 3D Fourier-transform spectra.