Nonadiabatic laser-induced alignment of molecules: Reconstructing ⟨������^�� θ⟩ directly from ⟨������^�� θ_2D⟩ by...

We present an efficient, noise-robust method based on Fourier analysis for reconstructing the three-dimensional measure of the alignment degree, ⟨cos²θ⟩, directly from its two-dimensional counterpart, ⟨cos²θ_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 ⟨cos²θ_2D⟩ trace over one molecular rotational period contains additional frequency components compared to the Fourier transform of ⟨cos²θ⟩. These additional frequency components can be identified and removed from the Fourier spectrum of ⟨cos²θ_2D⟩. By rescaling of the remaining frequency components, the Fourier spectrum of ⟨cos²θ⟩ is obtained and, finally, ⟨cos²θ⟩ is reconstructed through inverse Fourier transformation. The method allows the reconstruction of the ⟨cos²θ⟩ trace from a measured ⟨cos²θ_2D⟩ trace, which is the typical observable of many experiments, and thereby provides direct comparison to calculated ⟨cos²θ⟩ 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 I₂ molecules. In addition, we present an efficient algorithm for calculating the matrix elements of cos²θ_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 ⟨cos²θ_2D⟩ and ⟨cos²θ⟩ in general.