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首页> 外文期刊>The journal of physical chemistry, A. Molecules, spectroscopy, kinetics, environment, & general theory >Facile Background Discrimination in Femtosecond Stimulated Raman Spectroscopy Using a Dual-Frequency Raman Pump Technique
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Facile Background Discrimination in Femtosecond Stimulated Raman Spectroscopy Using a Dual-Frequency Raman Pump Technique

机译：使用双频拉曼泵技术，Femtosecond刺激拉曼光谱中的容易背景辨别

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摘要

Femtosecond stimulated Raman spectroscopy (FSRS) is a useful technique for uncovering chemical reaction dynamics by acquiring high-resolution Raman spectra with ultrafast time resolution. However, in FSRS, it can be challenging to discern Raman features from signals arising from transient absorption and other four-wave mixing pathways. To overcome this difficulty, we combine the principles of shifted excitation Raman difference spectroscopy with a simple fixed frequency comb to perform dual frequency Raman pump FSRS. Through the addition of only two mirrors and a slit to the standard FSRS setup, this method provides Raman spectra at two different excitation wavelengths that can be processed by an automated algorithm to reconstruct the Raman spectrum. Here, we demonstrate the utility of dual-frequency Raman pump FSRS to easily identify Raman signatures by visual inspection for excited-state and ground-state spectra, both on- and off-resonance. We show that previously assigned short-lived vibrations of photoexcited beta-carotene are actually not vibrational in nature. We also use crystalline betaine-30 as a challenging test case for this method, as the FSRS spectra contain a number of narrow transient vibronic and non-SRS features. By reliably reducing interference from background signals, the interpretation is substantially more quantitative and enables the future study of new systems, particularly those with small Raman cross-sections or solid-state samples with narrow vibronic features.
机译：FemtOSecond刺激的拉曼光谱（FSRS）是通过通过超快时间分辨率获取高分辨率拉曼光谱来揭示化学反应动力学的有用技术。然而，在FSRS中，它可能挑战从瞬态吸收和其他四波混合途径产生的信号中辨别拉曼特征。为了克服这种困难，我们将换档激励拉曼差异光谱的原理与简单的固定频率梳相结合，以执行双频拉曼泵FSR。通过添加两个镜子和狭缝到标准FSRS设置，该方法在两个不同的激励波长下提供可以通过自动算法处理的两个不同的激励波长来重建拉曼频谱。在这里，我们展示了双频拉曼泵FSR的效用，通过目视检查兴奋状态和地态光谱的视觉检查，既可以轻松识别拉曼签名。我们表明，先前分配了相磷β-胡萝卜素的短暂振动实际上并不振动。我们还将Crystalline Betaine-30用作该方法的具有挑战性的测试用例，因为FSRS光谱含有许多窄的瞬态振动和非SRS特征。通过可靠地减少背景信号的干扰，解释基本上更加定量并且能够实现新系统的未来研究，特别是那些具有窄振动特征的小拉曼横截面或固态样本的研究。

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