Mazza Francesco, van den Bekerom Dirk
Faculty of Aerospace Engineering, Delft University of Technology, Kluyverweg 1, Delft, 2629HS, The Netherlands.
Energy & Materials Transition, Netherlands Organization for Applied Scientific Research (TNO), Urmonderbaan 22, Geleen, 6167RD, The Netherlands.
Commun Chem. 2025 Jan 4;8(1):3. doi: 10.1038/s42004-024-01397-8.
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.
时间分辨相干拉曼光谱（CRS）是一种强大的非线性光学技术，用于对化学反应流进行定量原位分析，具有无与伦比的准确性和出色的时空分辨率。它在理解反应动力学方面至关重要的对大型多原子分子的应用，迄今为止一直受到其旋转 - 振动拉曼光谱复杂性的限制。为这些分子开发全面光谱代码这一长期目标的进展，一直受到其光谱合成所需的极长计算时间的阻碍。在此，我们提出一种算法，与现有方法相比，其计算时间提高了一百万倍。该算法显示出卓越的准确性，在室温（296K）和高温（1500K）下，所有测试的探测延迟的近似误差均低于0.1%。这一结果可能会极大地扩展时间分辨CRS的应用，特别是在等离子体研究以及更广泛的大气和天体物理学领域。
