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  • 主管单位:
  • 中国科学技术协会
  • 主办单位:
  • 中国仪器仪表学会、上海光学仪器研究所、中国光学学会工程光学专业委员会
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  • 国际标准刊号:
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  • 国内统一刊号:
  • 31-1504/TH
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  • 单  价:
  • 15.00
  • 定  价:
  • 90.00
振动强耦合下光学腔长的拉曼散射判定及应用
Raman-scattering-based determination and applications of optical cavity length in vibrational strong coupling
投稿时间:2024-03-08  
DOI:10.3969/j.issn.1005-5630.202403080042
中文关键词:  振动强耦合  光学腔长  水解反应
英文关键词:vibrational strong coupling  optical cavity length  hydrolysis reaction
基金项目:国家自然科学基金(61875126)
作者单位E-mail
刘言 上海理工大学 光电信息与计算机工程学院上海 200093  
张玲 上海理工大学 光电信息与计算机工程学院上海 200093 lzhang@isst.edu.cn 
摘要点击次数: 87
全文下载次数: 61
中文摘要:
      在振动强耦合(vibrational strong coupling,VSC)条件下,出现拉比分裂现象时,拉曼背底会呈现出与腔长相关的周期性波纹。经过分析发现,这种波纹的周期可用于腔长的计算,且周期性波峰数量与腔长成正比,由此提供了一种间接测量腔长的手段。虽然拉曼光谱中自由光谱范围(free spectral range,FSR)模式峰的展宽会在腔长测定中引入约10-2量级的系统误差,但这一偏差显著低于VSC效应所要求的腔长调制灵敏度阈值(10-1量级),因此不会对VSC的探测产生实质性影响。因此,在测量VSC 时,可同步计算腔长,从而使原位探测更便捷。同时在腔长固定时,若腔内物质发生变化,拉曼散射光谱中的 FSR 模式峰会随之频移,从而可以实时监测化学反应的速率。研究结果显示,VSC 能够催化硝基苯乙酸酯的水解反应。研究不仅定性地分析了该反应的进程,还定量评估了 VSC 对硝基苯乙酸酯水解反应的催化速率,可将其提升1至2个量级。这一研究结果对 VSC 条件下分子反应过程的探测具有借鉴意义。
英文摘要:
      Under vibrational strong coupling (VSC) conditions, Rabi splitting coincides with periodic ripples in the Raman background, which are indicative of cavity length. Analytical findings suggest that the frequency of these ripples can estimate cavity length. A proportional relationship exists between the number of periodic peaks and the optical cavity length, providing an indirect measurement method. Although the broadening of mode peaks in the free spectral range (FSR) of Raman spectra introduces systematic errors at the level of 10-2 in cavity length determination, this deviation is significantly below the sensitivity threshold (10-1 level) required for cavity length modulation in VSC detection. Therefore, it does not substantially affect the probing of VSC effects. During VSC measurements, cavity length is calculated concurrently, facilitating in situ detection. Additionally, when the cavity length was fixed, any changes in the cavity contents led to frequency shifts in the FSR mode peaks of the Raman spectrum, enabling real-time monitoring of chemical reaction rates. Research findings revealed that VSC could catalyze the hydrolysis of para-nitrophenyl acetate (PNPA), offering both qualitative and quantitative insights into the reaction process, and significantly enhancing the hydrolysis rate of PNPA by one to two orders of magnitude. These observations have significant implications for detecting molecular reaction processes under VSC conditions.
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