论文标题

频率搅动傅里叶变换光谱法

Frequency chirped Fourier-Transform spectroscopy

论文作者

Markmann, Sergej, Frankié, Martin, Bertrand, Mathieu, Shahmohammadi, Mehran, Forrer, Andres, Jouy, Pierre, Beck, Mattias, Faist, Jérôme, Scalari, Giacomo

论文摘要

具有高光谱分辨率的快速(下秒)光谱对于揭示复杂化学和生物学反应的量子化学动力学至关重要。傅立叶变换(FT)光谱仪可以实现高光谱分辨率,并在快速扫描模式下以数百个MS时间尺度运行。但是,扫描镜的线性翻译对这些系统施加了严格的时间分辨率限制,这使得不可能同时进行高光谱和时间分辨率。在这里,我们展示了一个FT光谱仪,其操作原理基于扫描镜的连续旋转而不是线性运动,从而将光谱分辨率与时间段的分辨率解耦。这启用了0.5 cm $ {}^{ - 1} $在子-MS时尺度上的分辨率。此外,我们表明这种旋转FT光谱仪可以用单个梳子源执行双弯曲光谱,因为梳子的多普勒移位版本是第二个梳子。通过这种方式,我们使用单个量子级联激光频率梳子将双弯曲和FT光谱的优势结合在一起。我们的技术不需要任何衍射或色散的光学元素,因此可以保留ft光谱仪的jacquinot's-,fellgett's-和Connes'-Advantages。该系统支持从可见频率到THZ频率的大型光带宽。旋转延迟线与准确的相干或非连贯的光源的组合为在高速,大光带宽和高光谱分辨率的应用中为FT光谱仪铺平了道路。

Fast (sub-second) spectroscopy with high spectral resolution is of vital importance for revealing quantum chemistry kinetics of complex chemical and biological reactions. Fourier transform (FT) spectrometers can achieve high spectral resolution and operate at hundreds of ms time scales in rapid-scan mode. However, the linear translation of a scanning mirror imposes stringent time-resolution limitations to these systems, which makes simultaneous high spectral and temporal resolution impossible. Here, we demonstrate an FT spectrometer whose operational principle is based on continuous rotational, rather than linear, motion of the scanning mirror, decoupling the spectral resolution from the temporal one. This enables 0.5 cm${}^{-1}$ resolution on sub-ms time scales. Furthermore, we show that such rotational FT spectrometers can perform dual-comb spectroscopy with a single comb source, since the Doppler-shifted version of the comb serves as the second comb. In this way, we combine the advantages of dual-comb and FT spectroscopy using a single quantum cascade laser frequency comb as a light source. Our technique does not require any diffractive or dispersive optical elements and hence preserve the Jacquinot's-, Fellgett's-, and Connes'-advantages of FT spectrometers. The system supports a large optical bandwidth from visible to THz frequencies. The combination of a rotational delay line with collimated coherent or non-coherent light sources pave the way for FT spectrometers in applications where high speed, large optical bandwidth, and high spectral resolution are desired.

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