Computational studies of x-ray scattering from three-dimensionally-aligned asymmetric-top molecules

Abstract

We theoretically and numerically analyze x-ray scattering from asymmetric-top molecules three-dimensionally aligned using elliptically polarized laser light. A rigid-rotor model is assumed. The principal axes of the polarizability tensor are assumed to coincide with the principal axes of the moment of inertia tensor. Several symmetries in the Hamiltonian are identified and exploited to enhance the efficiency of solving the time-dependent Schrödinger equation for each rotational state initially populated in a thermal ensemble. Using a phase-retrieval algorithm, the feasibility of structure reconstruction from a quasi-adiabatically-aligned sample is illustrated for the organic molecule naphthalene. The spatial resolution achievable strongly depends on the laser parameters, the initial rotational temperature, and the x-ray pulse duration. We demonstrate that for a laser peak intensity of 5 TW/cm^2, a laser pulse duration of 100 ps, a rotational temperature of 10 mK, and an x-ray pulse duration of 1 ps, the molecular structure may be probed at a resolution of 1 Å.

18 pages, 9 figures, accepted by Physical Review A

References in corpus (17)

• X-ray image reconstruction from a diffraction pattern alone
• High-resolution ab initio three-dimensional X-ray diffraction microscopy
• A unified evaluation of iterative projection algorithms for phase retrieval
• Relaxed Averaged Alternating Reflections for Diffraction Imaging
• An assessment of the resolution limitation due to radiation-damage in x-ray diffraction microscopy
• Laser-induced alignment and orientation of quantum-state-selected large molecules
• Field-free orientation of CO molecules by femtosecond two-color laser fields
• Quantum-state selection, alignment, and orientation of large molecules using static electric and laser fields
• Droplet beams for serial crystallography of proteins
• Field-free two-direction alignment alternation of linear molecules by elliptic laser pulses
• Ultimate field-free molecular alignment by combined adiabatic-impulsive field design
• An x-ray probe of laser-aligned molecules
• Laser Induced Selective Alignment of Water Spin Isomers
• Optical gratings induced by field-free alignment of molecules
• Theory of x-ray absorption by laser-aligned symmetric-top molecules
• Rotational molecular dynamics of laser-manipulated bromotrifluoromethane studied by x-ray absorption
• Phasing diffuse scattering. Application of the SIR2002 algorithm to the non-crystallographic phase problem

Cited by in corpus (17)

• Manipulation of Molecules with Electromagnetic Fields
• X-ray diffraction from isolated and strongly aligned gas-phase molecules with a free-electron laser
• Impact of hollow-atom formation on coherent x-ray scattering at high intensity
• State- and conformer-selected beams of aligned and oriented molecules for ultrafast diffraction studies
• Strongly aligned and oriented molecular samples at a kHz repetition rate
• Atomic and molecular dynamics triggered by ultrashort light pulses on the atto- to picosecond time scale
• Strongly aligned gas-phase molecules at Free-Electron Lasers
• Strong Field Ionization of Water: Nuclear Dynamics Revealed by Varying the Pulse Duration
• Quantum state tomography of molecules by ultrafast diffraction
• Alignment of asymmetric-top molecules using multiple-pulse trains
• Molecular Frame Photoelectron Angular Distributions in Polyatomic Molecules from Lab Frame Coherent Rotational Wavepacket Evolution
• Topological charges of periodically kicked molecules
• Applying Bayesian Inference and deterministic anisotropy to retrieve the molecular structure $|\Psi (\mathbf{R}){|}^2$ distribution from gas-phase diffraction experiments
• Ultraintense, ultrashort pulse x-ray scattering in small molecules
• Dynamics of fluctuations in a quantum system
• Machine learning for predicting control landscape maps of quantum molecular dynamics: Laser-induced three-dimensional alignment of asymmetric top molecules
• Electron gun for diffraction experiments off controlled molecules