Temporal resolution beyond the average pulse duration in shaped noisy-pulse transient absorption spectroscopy.

In time-resolved spectroscopy, it is a widespread belief that the temporal resolution is determined by the laser pulse duration. Recently, it was observed and shown that partially coherent laser pulses as they are provided by free-electron-laser (FEL) sources offer an alternative route to reach a temporal resolution below the average pulse duration. Here, we demonstrate the generation of partially coherent light in the laboratory like we observe it at FELs. We present the successful implementation of such statistically fluctuating pulses by using the pulse-shaping technique. These pulses exhibit an average pulse duration about 10 times larger than their bandwidth limit. The shaped pulses are then applied to transient-absorption measurements in the dye IR144. Despite the noisy characteristics of the laser pulses, features in the measured absorption spectra occurring on time scales much faster than the average pulse duration are resolved, thus proving the universality of the described noisy-pulse concept.