Theory of retrieving orientation-resolved molecular information using time-domain rotational coherence spectroscopy

Abstract

We provide a unified theoretical framework for recently emerging experiments that retrieve fixedin-space molecular information through time-domain rotational coherence spectroscopy. Unlike a previous approach by Makhija et al. [arXiv: 1611.06476 (2016], our method can be applied to the retrieval of both real-valued (e.g., ionization yield) and complex-valued (e.g., induced dipole moment) molecular response information. It is also a direct retrieval method without using iterations. We also demonstrate that experimental parameters, such as the fluence of the aligning laser pulse and the rotational temperature of the molecular ensemble, can be quite accurately determined using a statistical method.

Filming movies of attosecond charge migration in single molecules with high harmonic spectroscopy

“…For a given harmonic order, Eq. ( 1 ) can be expanded as 49 , 50 Let and discretize θ 1 , θ 2 in the range of [0, π ] with a step of 0.01 rad, the S ( τ ) then can be rewritten as Note that in Eq. ( 3 ), the imaginary part of D * ( θ 1 ) D ( θ 2 ) is omitted due to its asymmetry upon the exchange of θ 1 and θ 2 , which will vanish after the convolution.…”

Topical Review: Extracting molecular frame photoionization dynamics from experimental data

“…The time resolved signal ⟨S⟩(t) being measured, the unknown coefficients C jk can be determined by linear regression, and the MF signal in equation ( 24) constructed. In this form the method was initially applied to strong field ionization and dubbed Orientation Reconstruction through Rotational Coherence Spectroscopy [77,78]. It has since been applied to strong field ionization of various molecules [79][80][81], strong field dissociation [82] and few-photon ionization [83].…”

Molecular Frame Photoelectron Angular Distributions in Polyatomic Molecules from Lab Frame Coherent Rotational Wavepacket Evolution

“…This time dependent signal provides sufficient information in some cases to reconstruct the signal for a perfectly oriented molecule, at an arbitrary orientation with respect to the LF. This has been demonstrated for the case of strong field ionization of linear [63] and non-linear polyatomic [5,64,65] molecules, strong field photodissociation of linear molecules [4], molecular high harmonic generation spectroscopy [51,68,69], and MFPADs for one-photon ionization of a homonuclear diatomic molecule. [3].…”