How to turn your pump-probe instrument into a multidimensional spectrometer: 2D IR and Vis spectroscopies via pulse shaping.

How to turn your pump-probe instrument into a multidimensional spectrometer: 2D IR and Vis spectroscopies via pulse shaping.
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DOI:
10.1039/b813817f
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发表时间:
2009-02-07
期刊:
Physical chemistry chemical physics : PCCP
影响因子:
--
通讯作者:
Zanni MT
Zanni MT
中科院分区:
其他
文献类型:
--
作者:
Shim SH;Zanni MT

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我们最近开发了一种新的和简单的方法来收集二维红外和可见光谱,利用脉冲整形器和部分共线的光束几何形状。二维红外和维斯光谱是研究分子结构及其动力学的有力工具。它们可以用来关联振动或电子本征态,测量能量转移速率,量化线形的动力学,例如,所有这些都具有飞秒时间分辨率。因此,它们被用于表现出快速动态的系统,如亚毫秒化学和生物动态,以及难以研究的环境,如膜。虽然功能强大,但这些技术一直难以实现,因为它们需要一系列飞秒脉冲在空间和时间上重叠,具有精确的时间分辨率和干涉相位稳定性。然而,通过使用脉冲整形器和简单的光束几何形状,消除了与实现2D光谱相关的许多困难,这大大降低了研究人员进入这一令人兴奋的领域所需的技术障碍,同时提供了许多新的能力。本文的目的是提供一个概述的方法收集2D光谱,使局外人考虑使用2D光谱在自己的研究可以判断哪种方法将是最适合他们的研究目标。本文主要集中在二维红外光谱,但也包括我们最近的工作,适应这项技术,以收集二维维斯光谱。我们回顾了已经发表的工作,以及涵盖了我们以前没有报道过的几个主题,包括相位循环方法来去除背景信号,消除不必要的散射,并将数据收集转移到旋转框架中。
We have recently developed a new and simple way of collecting 2D infrared and visible spectra that utilizes a pulse shaper and a partly collinear beam geometry. 2D IR and Vis spectroscopies are powerful tools for studying molecular structures and their dynamics. They can be used to correlate vibrational or electronic eigenstates, measure energy transfer rates, and quantify the dynamics of lineshapes, for instance, all with femtosecond time-resolution. As a result, they are finding use in systems that exhibit fast dynamics, such as sub-millisecond chemical and biological dynamics, and in hard-to-study environments, such as in membranes. While powerful, these techniques have been difficult to implement because they require a series of femtosecond pulses to be spatially and temporally overlapped with precise time-resolution and interferometric phase stability. However, many of the difficulties associated with implementing 2D spectroscopies are eliminated by using a pulse shaper and a simple beam geometry, which substantially lowers the technical barriers required for researchers to enter this exciting field while simultaneously providing many new capabilities. The aim of this paper is to provide an overview of the methods for collecting 2D spectra so that an outsider considering using 2D spectroscopy in their own research can judge which approach would be most suitable for their research aims. This paper focuses primarily on 2D IR spectroscopy, but also includes our recent work on adapting this technology to collecting 2D Vis spectra. We review work that has already been published as well as cover several topics that we have not reported previously, including phase cycling methods to remove background signals, eliminate unwanted scatter, and shift data collection into the rotating frame.
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发表时间: 2002-02-14
影响因子: 2.9
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