Huber Marinus, Trubetskov M, Schweinberger W, Jacob P, Zigman M, Krausz F, Pupeza I
Max Planck Institute of Quantum Optics, 85748 Garching, Germany.
Department of Physics, Ludwig Maximilian University of Munich, 85748 Garching, Germany.
Anal Chem. 2024 Aug 13;96(32):13110-13119. doi: 10.1021/acs.analchem.4c01745. Epub 2024 Jul 29.
Field-resolved infrared spectroscopy (FRS) of impulsively excited molecular vibrations can surpass the sensitivity of conventional time-integrating spectroscopies, owing to a temporal separation of the molecular signal from the noisy excitation. However, the resonant response carrying the molecular signal of interest depends on both the amplitude and phase of the excitation, which can vary over time and across different instruments. To date, this has compromised the accuracy with which FRS measurements could be compared, which is a crucial factor for practical applications. Here, we utilize a data processing procedure that overcomes this shortcoming while preserving the sensitivity of FRS. We validate the approach for aqueous solutions of molecules. The employed approach is compatible with established processing and evaluation methods for the analysis of infrared spectra and can be applied to existing spectra from databases, facilitating the spread of FRS to new molecular analytical applications.
脉冲激发分子振动的场分辨红外光谱（FRS）能够超越传统时间积分光谱的灵敏度，这得益于分子信号与噪声激发在时间上的分离。然而，携带感兴趣分子信号的共振响应取决于激发的幅度和相位，而这两者可能随时间以及不同仪器而变化。迄今为止，这影响了FRS测量结果可比的准确性，而这对于实际应用来说是一个关键因素。在此，我们采用一种数据处理程序，该程序在保留FRS灵敏度的同时克服了这一缺点。我们对分子水溶液验证了该方法。所采用的方法与用于红外光谱分析的既定处理和评估方法兼容，并且可以应用于来自数据库的现有光谱，从而促进FRS在新的分子分析应用中的推广。
