Two-dimensional bond-selective fluorescence spectroscopy: violations of the resonance condition, vibrational cooling rate dispersion, and super-multiplex imaging.

ABSTRACT: Multidimensional spectroscopies have shaped our understanding of molecular phenomena, but they are often limited in sensitivity. In this work, we describe two-dimensional bond-selective fluorescence-detected infrared-excited (2D-BonFIRE) spectro-microscopy: an ultrasensitive two-dimensional spectroscopy and hyperspectral imaging technique. 2D-BonFIRE spectra are richly detailed, allowing for direct measurement of vibronic coupling and strong evidence of combination modes in congested spectral regions. Additionally, 2D-BonFIRE provides new insights into the nature of vibrational relaxation, including direct experimental observation of vibrational cooling rate dispersion, illuminating the inherent heterogeneity of vibrational decays in large molecules. Finally, we demonstrate that the high s

SUBMITTER: Kocheril PA 

PROVIDER: S-EPMC12336853 | biostudies-literature | 2025 Aug

REPOSITORIES: biostudies-literature