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Updated: May 12, 2025

High Resolution Phonon-assisted Quasi-resonance Fluorescence Spectroscopy
Published on: June 28, 2016
Overcoming experimental obstacles in two-dimensional spectroscopy of a single molecule
Sanchayeeta Jana1, Simon Durst1, Lucas Ludwig1
1Experimental Physics III, University of Bayreuth, 95447 Bayreuth, Germany.
Abstract:
Two-dimensional electronic spectroscopy provides information on coupling and energy transfer between excited states on ultrafast timescales. Only recently, incoherent fluorescence detection has made it possible to combine this method with single-molecule optical spectroscopy to reach the ultimate limit of sensitivity. The main obstacle has been the low number of photons detected due to limited photostability. Here, we discuss the key experimental choices that allowed us to overcome these obstacles: broadband acousto-optic modulation, accurate phase-locked loops, photon-counting lock-in detection, delay stage linearization, and detector dead-time compensation. We demonstrate how the acquired photon stream data can be used to post-select detection events according to specific criteria.
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