Details
| Original language | English |
|---|---|
| Article number | 4509 |
| Number of pages | 13 |
| Journal | Molecules (Basel, Switzerland) |
| Volume | 29 |
| Issue number | 18 |
| Publication status | Published - 23 Sept 2024 |
Abstract
It is a well-established standard to describe ground-state chemical reactions at an ab initio level of multi-electron theory. Fast reactions can be directly simulated. The most widely used approach is density functional theory for the electronic structure in combination with molecular dynamics for the nuclear motion. This approach is known as ab initio molecular dynamics. In contrast, the simulation of excited-state reactions at this level of theory is significantly more difficult. It turns out that the self-consistent solution of the Kohn-Sham equations is not easily reached in excited-state simulations. The first program that solved this problem was the Car-Parrinello molecular dynamics code, using restricted open-shell Kohn-Sham theory. Meanwhile, there are alternatives, most prominently the Q-Chem code, which widens the range of applications. The present study investigates the suitability of both codes for the molecular dynamics simulation of excited-state motion and presents applications to photoreactions.
Keywords
- ab initio molecular dynamics, excited-state self-consistent-field theory, photochemistry
ASJC Scopus subject areas
- Pharmacology, Toxicology and Pharmaceutics(all)
- Drug Discovery
- Chemistry(all)
- Analytical Chemistry
- Chemistry(all)
- Chemistry (miscellaneous)
- Biochemistry, Genetics and Molecular Biology(all)
- Molecular Medicine
- Chemistry(all)
- Physical and Theoretical Chemistry
- Pharmacology, Toxicology and Pharmaceutics(all)
- Pharmaceutical Science
- Chemistry(all)
- Organic Chemistry
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In: Molecules (Basel, Switzerland), Vol. 29, No. 18, 4509, 23.09.2024.
Research output: Contribution to journal › Article › Research › peer review
}
TY - JOUR
T1 - On the Simulation of Photoreactions Using Restricted Open-Shell Kohn-Sham Theory
AU - Büchel, Ralf
AU - Grage, Jan
AU - Maniscalco, Dominykas
AU - Frank, Irmgard
AU - Alvarez, Luis
N1 - Publisher Copyright: © 2024 by the authors.
PY - 2024/9/23
Y1 - 2024/9/23
N2 - It is a well-established standard to describe ground-state chemical reactions at an ab initio level of multi-electron theory. Fast reactions can be directly simulated. The most widely used approach is density functional theory for the electronic structure in combination with molecular dynamics for the nuclear motion. This approach is known as ab initio molecular dynamics. In contrast, the simulation of excited-state reactions at this level of theory is significantly more difficult. It turns out that the self-consistent solution of the Kohn-Sham equations is not easily reached in excited-state simulations. The first program that solved this problem was the Car-Parrinello molecular dynamics code, using restricted open-shell Kohn-Sham theory. Meanwhile, there are alternatives, most prominently the Q-Chem code, which widens the range of applications. The present study investigates the suitability of both codes for the molecular dynamics simulation of excited-state motion and presents applications to photoreactions.
AB - It is a well-established standard to describe ground-state chemical reactions at an ab initio level of multi-electron theory. Fast reactions can be directly simulated. The most widely used approach is density functional theory for the electronic structure in combination with molecular dynamics for the nuclear motion. This approach is known as ab initio molecular dynamics. In contrast, the simulation of excited-state reactions at this level of theory is significantly more difficult. It turns out that the self-consistent solution of the Kohn-Sham equations is not easily reached in excited-state simulations. The first program that solved this problem was the Car-Parrinello molecular dynamics code, using restricted open-shell Kohn-Sham theory. Meanwhile, there are alternatives, most prominently the Q-Chem code, which widens the range of applications. The present study investigates the suitability of both codes for the molecular dynamics simulation of excited-state motion and presents applications to photoreactions.
KW - ab initio molecular dynamics
KW - excited-state self-consistent-field theory
KW - photochemistry
UR - http://www.scopus.com/inward/record.url?scp=85205066810&partnerID=8YFLogxK
U2 - 10.3390/molecules29184509
DO - 10.3390/molecules29184509
M3 - Article
C2 - 39339507
VL - 29
JO - Molecules (Basel, Switzerland)
JF - Molecules (Basel, Switzerland)
SN - 1420-3049
IS - 18
M1 - 4509
ER -