Title :

Time evolution of natural orbitals in ab initio molecular dynamics

Author(s) :

Rivero Santamaria, Alejandro [Auteur]
Physico-Chimie Moléculaire Théorique [PCMT]
Piris, Mario [Auteur]
Donostia International Physics Center - DIPC (SPAIN)

Journal title :

The Journal of Chemical Physics

Publisher :

American Institute of Physics

Publication date :

2024

ISSN :

0021-9606

HAL domain(s) :

Chimie/Chimie théorique et/ou physique
Physique [physics]/Physique [physics]/Chimie-Physique [physics.chem-ph]

English abstract : [en]

This work combines for the first time ab initio molecular dynamics (AIMD) within the Born–Oppenheimer approximation with a global natural orbital functional (GNOF), an approximate functional of the one-particle reduced ...
Show more >This work combines for the first time ab initio molecular dynamics (AIMD) within the Born–Oppenheimer approximation with a global natural orbital functional (GNOF), an approximate functional of the one-particle reduced density matrix. The most prominent feature of GNOF-AIMD is its ability to display the real-time evolution of natural orbitals, providing detailed information on the time-dependent electronic structure of complex systems and processes, including reactive collisions. The quartet ground-state reaction N(⁴S) + H₂(¹Σ) → NH(³Σ) + H(²S) is taken as a validation test. Collision energy influences on integral cross sections for different initial rovibrational states of H₂ and rotational-state distributions of the NH product are discussed, showing a good agreement with previous high-quality theoretical results.Show less >

Language :

Anglais

Popular science :

Non

Collections :

• Laboratoire de Physique des Lasers, Atomes et Molécules (PhLAM) - UMR 8523

Source :

Harvested from HAL