An ultrafast algorithm for ultrafast time-resolved coherent Raman spectroscopy

Francesco Mazza, Dirk van den Bekerom*

*Corresponding author for this work

Research output: Contribution to journalArticleScientificpeer-review

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Abstract

Time-resolved coherent Raman spectroscopy (CRS) is a powerful non-linear optical technique for quantitative, in-situ analysis of chemically reacting flows, offering unparalleled accuracy and exceptional spatiotemporal resolution. Its application to large polyatomic molecules, crucial for understanding reaction dynamics, has thus far been limited by the complexity of their rotational-vibrational Raman spectra. Progress in developing comprehensive spectral codes for these molecules, a longstanding goal, has been hindered by prohibitively long computation times required for their spectral synthesis. Here, we present an algorithm that achieves a million-fold improvement in computation time compared to existing methods. The algorithm demonstrates remarkable accuracy, with an approximation error below 0.1% across all tested probe delays, at both room temperature (296 K) and elevated temperatures (1500 K). This result could greatly expand the application of time-resolved CRS, particularly in plasma research, as well as in broader atmospheric and astrophysical sciences. (Figure presented.)

Original languageEnglish
Article number3
Number of pages9
JournalCommunications Chemistry
Volume8
Issue number1
DOIs
Publication statusPublished - 2025

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