Work

Overcoming experimental obstacles in two-dimensional spectroscopy of a single molecule

Year: 2025

Type: article

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.

Source: The Journal of Chemical Physics

DOI: 10.1063/5.0261813

Authors: Sanchayeeta Jana, Simon Durst, Lucas Ludwig, Markus Lippitz

Institution: University of Bayreuth

Language: English

Topic: Spectroscopy and Quantum Chemical Studies

Subfield: Atomic and Molecular Physics, and Optics

Field: Physics and Astronomy

Domain: Physical Sciences

Open Access status: hybrid

Estimated APC paid: $3,500

Funder: Deutsche Forschungsgemeinschaft