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首页> 外文期刊>The Journal of Chemical Physics >Nonadiabatic laser-induced alignment of molecules: Reconstructing < cos(2)theta > directly from < cos(2)theta(2D)> by Fourier analysis
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Nonadiabatic laser-induced alignment of molecules: Reconstructing < cos(2)theta > directly from < cos(2)theta(2D)> by Fourier analysis

机译：非等离激光诱导的分子对准：通过傅立叶分析直接从重建

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摘要

We present an efficient, noise-robust method based on Fourier analysis for reconstructing the three-dimensional measure of the alignment degree, < cos(2)theta >, directly from its two-dimensional counterpart, < cos(2)theta(2D)>. The method applies to nonadiabatic alignment of linear molecules induced by a linearly polarized, nonresonant laser pulse. Our theoretical analysis shows that the Fourier transform of the time-dependent < cos(2)theta(2D)> trace over one molecular rotational period contains additional frequency components compared to the Fourier transform of < cos(2)theta >. These additional frequency components can be identified and removed from the Fourier spectrum of < cos(2)theta(2D)>. By rescaling of the remaining frequency components, the Fourier spectrum of < cos(2)theta > is obtained and, finally, < cos(2)theta > is reconstructed through inverse Fourier transformation. The method allows the reconstruction of the < cos(2)theta > trace from a measured < cos(2)theta(2D)> trace, which is the typical observable of many experiments, and thereby provides direct comparison to calculated < cos(2)theta > traces, which is the commonly used alignment metric in theoretical descriptions. We illustrate our method by applying it to the measurement of nonadiabatic alignment of I-2 molecules. In addition, we present an efficient algorithm for calculating the matrix elements of < cos(2)theta(2D)> and any other observable in the symmetric top basis. These matrix elements are required in the rescaling step, and they allow for highly efficient numerical calculation of < cos(2)theta > and < cos(2)theta > in general.
机译：我们提出了一种基于傅里叶分析的高效，噪声稳健方法，用于重建对准程度的三维度量，，直接从其二维对应物，。该方法适用于线性偏振，非族聚合物激光脉冲引起的线性分子的非分子对准。我们的理论分析表明，与的傅立叶变换相比，在一个分子旋转时段的时间依赖性迹线的傅里叶变换包含额外的频率分量。可以从的傅里叶频谱中识别和去除这些附加频率分量。通过重新扫描剩余频率分量，获得了的傅里叶谱，最后，通过逆傅里叶变换重建迹线重建痕迹，这是许多实验的典型可观察，从而提供与计算的直接比较（2 ）Theta>迹线，这是理论描述中的常用对齐度量。我们通过将其施加到I-2分子的非分配对准来说明我们的方法。另外，我们介绍了一种用于计算的矩阵元素和对称顶部的任何其他可观察到的算法。在重新缩放步骤中需要这些基质元素，并且它们通常允许高效地计算和。

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