An ultrafast algorithm for ultrafast time-resolved coherent Raman spectroscopy

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 un...

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Main Authors: Francesco Mazza, Dirk van den Bekerom
Format: Article
Language:English
Published: Nature Portfolio 2025-01-01
Series:Communications Chemistry
Online Access:https://doi.org/10.1038/s42004-024-01397-8
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author Francesco Mazza
Dirk van den Bekerom
author_facet Francesco Mazza
Dirk van den Bekerom
author_sort Francesco Mazza
collection DOAJ
description 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.
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institution Kabale University
issn 2399-3669
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spelling doaj-art-7387685b6068428a8ee8e806b62105072025-01-05T12:10:51ZengNature PortfolioCommunications Chemistry2399-36692025-01-01811910.1038/s42004-024-01397-8An ultrafast algorithm for ultrafast time-resolved coherent Raman spectroscopyFrancesco Mazza0Dirk van den Bekerom1Faculty of Aerospace Engineering, Delft University of TechnologyEnergy & Materials Transition, Netherlands Organization for Applied Scientific Research (TNO)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.https://doi.org/10.1038/s42004-024-01397-8
spellingShingle Francesco Mazza
Dirk van den Bekerom
An ultrafast algorithm for ultrafast time-resolved coherent Raman spectroscopy
Communications Chemistry
title An ultrafast algorithm for ultrafast time-resolved coherent Raman spectroscopy
title_full An ultrafast algorithm for ultrafast time-resolved coherent Raman spectroscopy
title_fullStr An ultrafast algorithm for ultrafast time-resolved coherent Raman spectroscopy
title_full_unstemmed An ultrafast algorithm for ultrafast time-resolved coherent Raman spectroscopy
title_short An ultrafast algorithm for ultrafast time-resolved coherent Raman spectroscopy
title_sort ultrafast algorithm for ultrafast time resolved coherent raman spectroscopy
url https://doi.org/10.1038/s42004-024-01397-8
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