Measuring absorptive two-dimensional infrared spectra using chirped-pulse upconversion detection
Measuring absorptive two-dimensional infrared spectra using chirped-pulse upconversion detection
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DOI：
10.1364/josab.27.000382
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发表时间：
2010-03-01
影响因子：
1.9
通讯作者：
Kubarych, Kevin J.
中科院分区：
文献类型：
--
作者：
Anna, Jessica M.;Nee, Matthew J.;Kubarych, Kevin J.
啁啾脉冲上转换（CPU），使中红外光谱的检测使用硅CCD相机的和频混合的中红外领域的高度啁啾近红外（800 nm）领域。虽然大量的啁啾限制了由固有的交叉相位调制引起的光谱展宽和相位失真，但是测量完全吸收的二维IR光谱所需的精细相位保真度要求相位失真的校正。我们演示了如何纠正所有的相位失真，包括延迟级校准，以及必要的非线性信号记录的吸收2D光谱。除了上转换过程本身的额外实验步骤之外，相位校正过程仅需要啁啾脉冲的频谱或时间相位的知识。在金属羰基络合物Mn-2（CO）（10）中，在正己烷和甲醇溶剂中证明了该方法，表明该方法在均匀和不均匀加宽的情况下都能很好地操作。(C)2010年美国光学学会
Chirped-pulse upconversion (CPU) enables the detection of mid-infrared spectra using a silicon CCD camera by sum-frequency mixing a mid-IR field with a highly chirped near-IR ( 800 nm) field. Although the substantial chirp limits the spectral broadening and phase distortions caused by the inherent cross-phase modulation, the exquisite phase fidelity needed to measure a fully absorptive two-dimensional IR spectrum demands the correction of the phase distortions. We demonstrate how to correct all of the phase distortions involved in recording an absorptive 2DIR spectrum including delay stage calibrations as well as the requisite nonlinear signals. Besides the extra experimental step of the upconversion process itself, the phase correction procedure requires only the knowledge of the spectral or temporal phase of the chirped pulse. The method is demonstrated in a metal carbonyl complex, Mn-2(CO)(10), in n-hexane and methanol solvents showing that the method operates well in cases of both homogeneous and inhomogeneous broadening. (C) 2010 Optical Society of America