A theory and method for a matrix-based reconstruction of molecular frame (MF) photoelectron angular distributions (MFPADs) from laboratory frame (LF) measurements (LFPADs) is developed and basic applications are explored. As with prior studies of MF reconstruction, the experimental side of this protocol is based upon time-resolved LF measurements in which a rotational wavepacket is prepared and probed as a function of time via photoionization, followed by a numerical reconstruction routine. In contrast to other methodologies, the protocol presented here does not require determination of the photoionization matrix elements, and consequently takes the relatively simple numerical form of a matrix equation. Significantly, this simplicity allows the successful reconstruction of MFPADs for nonlinear polyatomic molecules with D _nh point group symmetry. We numerically demonstrate this scheme for two realistic molecular photoionization cases: N₂ and C₂H₄. This new technique is expected to be generally applicable to a broad range of MF reconstruction problems involving photoionization of polyatomic molecules.

开发了一种基于矩阵重建从实验室框架 (LF) 测量 (LFPADs) 的分子框架 (MF) 光电子角分布 (MFPADs) 的理论和方法，并探索了基本应用。与先前对 MF 重建的研究一样，该协议的实验方面基于时间分辨 LF 测量，其中通过光电离准备和探测旋转波包作为时间的函数，然后是数值重建程序。与其他方法相比，此处介绍的协议不需要确定光电离矩阵元素，因此采用矩阵方程的相对简单的数值形式。值得注意的是，这种简单性允许成功重建具有D 的非线性多原子分子的 MFPAD _nh 点群对称。我们针对两个现实的分子光电离情况用数值方法证明了该方案：N ₂和 C ₂ H ₄。预计这种新技术将普遍适用于涉及多原子分子光电离的广泛 MF 重建问题。