Toward accurate predictions of bond-selective fluorescence spectra

Area of Science:

• Molecular spectroscopy
• Chemical physics
• Biophysical chemistry

Background:

• Vibrational-encoded fluorescence spectro-microscopies combine molecular vibration analysis with fluorescence sensitivity.
• Bond-selective fluorescence-detected infrared-excited (BonFIRE) spectro-microscopy is a recently developed technique.
• Current applications of BonFIRE for rational molecular design are limited but show potential with computational assistance.

Purpose of the Study:

• To provide a theoretical overview of BonFIRE spectroscopy.
• To present a computational pipeline for calculating BonFIRE spectra.
• To explore potential applications of computational methods in vibrational-encoded fluorescence spectro-microscopies.

Main Methods:

• Overview of the theoretical principles behind BonFIRE spectroscopy.
• Development and description of a fully automated computational pipeline for BonFIRE spectra calculation.
• Validation of the computational pipeline by reproducing experimental results.

Main Results:

• The computational pipeline successfully calculates BonFIRE spectra.
• Key features of experimental BonFIRE spectra were reproduced using the computational method.
• The study highlights the potential of computational tools to enhance BonFIRE capabilities.

Conclusions:

• Computational methods can significantly assist in the application of BonFIRE spectro-microscopy.
• The developed pipeline offers a pathway for rational molecular design.
• Vibrational-encoded fluorescence spectro-microscopies, aided by computation, have broad implications for chemistry and biology.