| Summary: | Single-molecule spectroscopy has been extensively used to investigate heterogeneity in static and dynamic behaviors on millisecond and second timescales. More recently, single-molecule pump-probe spectroscopy emerged as a method to access heterogeneity on the femtosecond and picosecond timescales. Here, we develop a single-molecule pump-probe apparatus that is easily tunable across the visible region and demonstrate its utility on the widely-used fluorescent dye, Atto647N. A spectrally-independent, bimodal distribution of energetic relaxation time constants is found, where one peak corresponds to electronic dephasing (∼ 100 fs) and the other to intravibrational relaxation (∼ 300 fs). The bimodal nature indicates that relaxation within each individual molecule is dominated by only one of these processes. Both peaks of the distribution are narrow, suggesting little heterogeneity is present for either process. As illustrated here, spectrally-tunable single-molecule pump-probe spectroscopy will enable investigation of the heterogeneity in a wide range of biological and material systems.
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