Details
| Original language | English |
|---|---|
| Article number | e26902 |
| Journal | International Journal of Quantum Chemistry |
| Volume | 122 |
| Issue number | 12 |
| Publication status | Published - 27 Apr 2022 |
Abstract
Is a classical description of nuclear motion sufficient when describing chemical reactions and spectra? This question is interesting because many researchers use a classical description of nuclear motion in molecular dynamics simulations. The present paper investigates some phenomena that were previously attributed to nuclear quantum effects. The question is if these phenomena can be modeled with traditional Car–Parrinello molecular dynamics, that is, with a method which treats nuclear motion classically and which is widely applied to the simulation of chemical reactions and spectra. We find that for the investigated system no additional paradigm is needed for describing chemical reactions. The special reactivity observed for carbenes can be attributed to the special environment represented by a noble gas matrix and to an additional transition state that was not considered before. Also the infrared spectrum of porphycene is perfectly modeled by traditional Car–Parrinello molecular dynamics. More studies are necessary to decide to what extent classical nuclear motion can replace the quantum mechanical description.
Keywords
- Car–Parrinello molecular dynamics, reaction mechanisms
ASJC Scopus subject areas
- Physics and Astronomy(all)
- Atomic and Molecular Physics, and Optics
- Physics and Astronomy(all)
- Condensed Matter Physics
- Chemistry(all)
- Physical and Theoretical Chemistry
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In: International Journal of Quantum Chemistry, Vol. 122, No. 12, e26902, 27.04.2022.
Research output: Contribution to journal › Article › Research › peer review
}
TY - JOUR
T1 - Classical nuclear motion
T2 - Does it fail to explain reactions and spectra in certain cases?
AU - Rohloff, Erik
AU - Rudolph, Dominik A.
AU - Strolka, Onno
AU - Frank, Irmgard
N1 - Funding Information: The study was supported by the Deutsche Forschungsgemeinschaft (DFG), grant FR1246/10‐1. Funding information
PY - 2022/4/27
Y1 - 2022/4/27
N2 - Is a classical description of nuclear motion sufficient when describing chemical reactions and spectra? This question is interesting because many researchers use a classical description of nuclear motion in molecular dynamics simulations. The present paper investigates some phenomena that were previously attributed to nuclear quantum effects. The question is if these phenomena can be modeled with traditional Car–Parrinello molecular dynamics, that is, with a method which treats nuclear motion classically and which is widely applied to the simulation of chemical reactions and spectra. We find that for the investigated system no additional paradigm is needed for describing chemical reactions. The special reactivity observed for carbenes can be attributed to the special environment represented by a noble gas matrix and to an additional transition state that was not considered before. Also the infrared spectrum of porphycene is perfectly modeled by traditional Car–Parrinello molecular dynamics. More studies are necessary to decide to what extent classical nuclear motion can replace the quantum mechanical description.
AB - Is a classical description of nuclear motion sufficient when describing chemical reactions and spectra? This question is interesting because many researchers use a classical description of nuclear motion in molecular dynamics simulations. The present paper investigates some phenomena that were previously attributed to nuclear quantum effects. The question is if these phenomena can be modeled with traditional Car–Parrinello molecular dynamics, that is, with a method which treats nuclear motion classically and which is widely applied to the simulation of chemical reactions and spectra. We find that for the investigated system no additional paradigm is needed for describing chemical reactions. The special reactivity observed for carbenes can be attributed to the special environment represented by a noble gas matrix and to an additional transition state that was not considered before. Also the infrared spectrum of porphycene is perfectly modeled by traditional Car–Parrinello molecular dynamics. More studies are necessary to decide to what extent classical nuclear motion can replace the quantum mechanical description.
KW - Car–Parrinello molecular dynamics
KW - reaction mechanisms
UR - http://www.scopus.com/inward/record.url?scp=85126029934&partnerID=8YFLogxK
U2 - 10.1002/qua.26902
DO - 10.1002/qua.26902
M3 - Article
AN - SCOPUS:85126029934
VL - 122
JO - International Journal of Quantum Chemistry
JF - International Journal of Quantum Chemistry
SN - 0020-7608
IS - 12
M1 - e26902
ER -