Phase Cycling RT-TDDFT Simulation Protocol for Nonlinear XUV and X-ray Molecular Spectroscopy.
Daeheum ChoJérémy R RouxelMarkus KowalewskiPrasoon SaurabhJin Yong LeeShaul MukamelPublished in: The journal of physical chemistry letters (2018)
Real-time time-dependent density functional theory (RT-TDDFT) provides a practical algorithm for propagating a many-electron system driven by external laser fields. The fields are included nonperturbatively in the propagation, and the molecular reduced single-electron density operator and various spectroscopic and diffraction signals can be computed directly, avoiding the expensive calculation of many-body states. Nonlinear optical signals contain contributions of multiple pathways. A phase cycling protocol is implemented in order to separate these pathways. Simulations of XUV four-wave mixing signals in the CO molecule are compared with ab initio sum-over-states calculations.
Keyphrases
- density functional theory
- molecular dynamics
- high resolution
- electron microscopy
- randomized controlled trial
- single molecule
- monte carlo
- high intensity
- high speed
- machine learning
- molecular docking
- deep learning
- magnetic resonance imaging
- solar cells
- molecular dynamics simulations
- solid state
- magnetic resonance
- computed tomography
- electron transfer
- mass spectrometry
- diffusion weighted imaging