Broadband single-molecule excitation spectroscopy

Nature Communications
Lukasz PiatkowskiNiek F van Hulst

Abstract

Over the past 25 years, single-molecule spectroscopy has developed into a widely used tool in multiple disciplines of science. The diversity of routinely recorded emission spectra does underpin the strength of the single-molecule approach in resolving the heterogeneity and dynamics, otherwise hidden in the ensemble. In early cryogenic studies single molecules were identified by their distinct excitation spectra, yet measuring excitation spectra at room temperature remains challenging. Here we present a broadband Fourier approach that allows rapid recording of excitation spectra of individual molecules under ambient conditions and that is robust against blinking and bleaching. Applying the method we show that the excitation spectra of individual molecules exhibit an extreme distribution of solvatochromic shifts and distinct spectral shapes. Importantly, we demonstrate that the sensitivity and speed of the broadband technique is comparable to that of emission spectroscopy putting both techniques side-by-side in single-molecule spectroscopy.

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Citations

Nov 4, 2016·The Journal of Physical Chemistry Letters·Martin StreiterCarsten Deibel
Jan 25, 2017·The Journal of Physical Chemistry. a·Sean A FischerPatrick Z El-Khoury
Jan 17, 2017·Nano Letters·Matz LiebelNiek F van Hulst
Mar 17, 2017·Physical Chemistry Chemical Physics : PCCP·Yu Akimov, S Sun
Dec 7, 2019·Science·Lukasz PiatkowskiNiek F van Hulst
Feb 17, 2019·Proceedings of the National Academy of Sciences of the United States of America·Erling ThyrhaugJürgen Hauer
May 6, 2019·Optics Express·S Krause, T Vosch
Mar 10, 2017·Light, Science & Applications·Nicolò AccantoNiek F van Hulst
Dec 5, 2018·Proceedings of the National Academy of Sciences of the United States of America·Pablo A Gómez-GarcíaMelike Lakadamyali
Feb 5, 2021·Nano Letters·Matz LiebelNiek F van Hulst
Jun 22, 2021·Angewandte Chemie·Pavel Malý, Tobias Brixner
Feb 23, 2018·The Journal of Physical Chemistry Letters·Lukasz PiatkowskiJacek Waluk
Jan 25, 2018·Chemical Reviews·Sujay RayNils G Walter
Oct 18, 2019·The Journal of Physical Chemistry Letters·Lorenzo SansaloneFrançisco M Raymo
May 14, 2020·Nano Letters·Lisa SaemischNiek F van Hulst
Mar 7, 2020·The Journal of Physical Chemistry Letters·Esther GellingsNiek F van Hulst

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