Room-temperature ultrafast nonlinear spectroscopy of single molecules with broadband detection

Summary form only given. Our understanding of the dynamical processes such as light harvesting or single fission crucially relies on ultrafast nonlinear measurement modalities [1,2]. Such techniques are routinely applied to bulk materials but their extension to individual quantum systems in condensed phase at room temperature has thus far remained elusive but is highly sought after due to the ongoing device miniaturisation down to the single molecule (SM) level [3]. Even the mere detection of a SM under these conditions has only been achieved under great experimental efforts and only recently have nonlinear SM-experiments under cryogenic conditions been reported for the first time [4-6]. Here, we introduce a novel experimental technique that allows for the direct recording of ultrafast transient absorption spectra of SMs in a broadband fashion and a temporal resolution of 25 fs at room temperature in condensed phase.