Broadband two-dimensional spectrochronography with ultrashort pulses in the mid-infrared

A novel, 2.6-to-10-μm wavelength-tunable laser source of sub-70-fs pulses is combined with mid-IR heterodyne detection to provide a versatile laser platform for broadband two-dimensional Fourier-transform infrared spectrochronography. The mid-infrared laser output serves as both a shortpulse driver and a broadband probe for time-resolved studies of ultrafast molecular coherence, population dynamics, and multimodal energy transfer in a vast class of complex molecular systems.