Double-resonance versus pulsed Fourier transform two-dimensional infrared spectroscopy: An experimental and theoretical comparison
Double-resonance versus pulsed Fourier transform two-dimensional infrared spectroscopy: An experimental and theoretical comparison
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DOI：
10.1063/1.1778163
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发表时间：
2004-09-22
影响因子：
4.4
通讯作者：
Hamm, P
中科院分区：
文献类型：
--
作者：
Cervetto, V;Helbing, J;Hamm, P
在这项研究中，我们重点研究了二维红外光谱的两种实验实现的差异和相似之处：双共振或动态孔燃烧二维红外光谱和脉冲傅立叶变换或外差探测光子回波光谱。通过对比两种方法得到的数据，在理论上和实验上进行了比较。作为一个例子，我们研究了溶解在己烷中的二羰基乙酰丙酮铑的强耦合不对称和对称羰基拉伸振动。两种方法在2D-IR光谱中产生相同的峰。在一定近似范围内，我们推导出二维红外光谱在双共振实验中通过与泵浦脉冲谱宽的卷积在一个频率维度上展宽，而在另一个频率方向上的光谱分辨率在两种情况下是相同的。(C) 2004年美国物理研究所。
In this study we focus on the differences and analogies of two experimental implementations of two-dimensional infrared (2D-IR) spectroscopy: double-resonance or dynamic hole burning 2D-IR spectroscopy and pulsed Fourier transform or heterodyne detected photon echo spectroscopy. A comparison is done theoretically as well as experimentally by contrasting data obtained from both methods. As an example we have studied the strongly coupled asymmetric and symmetric carbonyl stretching vibrations of dicarbonylacetylacetonato rhodium dissolved in hexane. Both methods yield the same peaks in a 2D-IR spectrum. Within certain approximations we derive an analytic expression which shows that the 2D-IR spectra are broadened in one frequency dimension in the double-resonance experiment by convolution with the pump pulse spectral width, while the spectral resolution in the other frequency direction is the same in both cases. (C) 2004 American Institute of Physics.