Alignment dependence of photoelectron angular distributions in the few-photon ionization of molecules by ultraviolet pulses

Lam, Huynh Van Sa; Wangjam, Tomthin Nganba; Kumarappan, Vinod

doi:10.1103/physreva.105.053109

Cited by 5 publications

(1 citation statement)

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“…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].…”

Section: Freely Rotating Molecules: Mf Via Time Evolutionmentioning

confidence: 99%

Topical Review: Extracting molecular frame photoionization dynamics from experimental data

Hockett

Makhija

2023

J. Phys. B: At. Mol. Opt. Phys.

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Methods for experimental reconstruction of molecular frame (MF) photoionization dynamics, and related properties - specifically MF photoelectron angular distributions (PADs) and continuum density matrices - are outlined and discussed. General concepts are introduced for the non-expert reader, and experimental and theoretical techniques are further outlined in some depth. Particular focus is placed on a detailed example of numerical reconstruction techniques for matrix-element retrieval from time-domain experimental measurements making use of rotational-wavepackets (i.e. aligned frame measurements) - the ``bootstrapping to the MF" methodology - and a matrix-inversion technique for direct MF-PAD recovery. Ongoing resources for interested researchers are also introduced, including sample data, reconstruction codes (the \textit{Photoelectron Metrology Toolkit}, written in python, and associated \textit{Quantum Metrology with Photoelectrons} platform/ecosystem), and literature via online repositories; it is hoped these resources will be of ongoing use to the community.

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Section: Freely Rotating Molecules: Mf Via Time Evolutionmentioning

confidence: 99%

Topical Review: Extracting molecular frame photoionization dynamics from experimental data

Hockett

Makhija

2023

J. Phys. B: At. Mol. Opt. Phys.

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Time Resolved Quantum Tomography in Molecular Spectroscopy by the Maximal Entropy Approach

Makhija,

Gupta,

Neville

et al. 2024

J. Phys. Chem. Lett.

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Attosecond science offers unprecedented precision in probing the initial moments of chemical reactions, revealing the dynamics of molecular electrons that shape reaction pathways. A fundamental question emerges: what role, if any, do quantum coherences between molecular electron states play in photochemical reactions? Answering this question necessitates quantum tomographythe determination of the electronic density matrix from experimental data, where the off-diagonal elements represent these coherences. The Maximal Entropy (MaxEnt) based Quantum State Tomography (QST) approach offers unique advantages in studying molecular dynamics, particularly with partial tomographic data. Here, we explore the application of MaxEnt-based QST on photoexcited ammonia, necessitating the operator form of observables specific to the performed measurements. We present two methodologies for constructing these operators: one leveraging Molecular Angular Distribution Moments (MADMs) which accurately capture the orientation-dependent vibronic dynamics of molecules and another utilizing Angular Momentum Coherence Operators to construct measurement operators for the full rovibronic density matrix in the symmetric top basis. A key revelation of our study is the direct link between Lagrange multipliers in the MaxEnt formalism and the unique set of MADMs. Additionally, we visualize the electron density within the molecular frame, demonstrating charge migration across the molecule. Furthermore, we achieve a groundbreaking milestone by constructing, for the first time, the entanglement entropy of the electronic subsystema metric that was previously inaccessible. The entropy vividly reveals and quantifies the effects of coupling between the excited electron and nuclear degrees of freedom. Consequently, our findings open new avenues for research in ultrafast molecular spectroscopy within the broader domain of quantum information science, offering profound implications for the study of molecular systems under excitation using quantum tomographic schemes.

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Orientation-angle-resolved photoelectron angular distribution in dissociative ionization of methanol induced by an intense ultraviolet laser pulse

et al. 2023

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Alignment dependence of photoelectron angular distributions in the few-photon ionization of molecules by ultraviolet pulses

Cited by 5 publications

References 50 publications

Topical Review: Extracting molecular frame photoionization dynamics from experimental data

Topical Review: Extracting molecular frame photoionization dynamics from experimental data

Time Resolved Quantum Tomography in Molecular Spectroscopy by the Maximal Entropy Approach

Orientation-angle-resolved photoelectron angular distribution in dissociative ionization of methanol induced by an intense ultraviolet laser pulse

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