Details
| Original language | English |
|---|---|
| Article number | 194105 |
| Number of pages | 1 |
| Journal | The journal of chemical physics |
| Volume | 152 |
| Issue number | 19 |
| Early online date | 19 May 2020 |
| Publication status | Published - 21 May 2020 |
Abstract
We present a combination of the recently developed double incremental expansion of potential energy surfaces with the well-established adaptive density-guided approach to grid construction. This unique methodology is based on the use of an incremental expansion for potential energy surfaces, known as n-mode expansion; an incremental many-body representation of the electronic energy; and an efficient vibrational density-guided approach to automated determination of grid dimensions and granularity. The reliability of the method is validated calculating potential energy surfaces and obtaining fundamental excitation energies for three moderate-size chain-like molecular systems. The use of our methodology leads to considerable computational savings for potential energy surface construction compared to standard approaches while maintaining a high level of accuracy in the resulting potential energy surfaces. Additional investigations indicate that our method can be applied to covalently bound and strongly interacting molecular systems, even though these cases are known to be very unfavorable for fragmentation schemes. We therefore conclude that the presented methodology is a robust and flexible approach to potential energy surface construction, which introduces considerable computational savings without compromising the accuracy of vibrational spectra calculations.
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In: The journal of chemical physics, Vol. 152, No. 19, 194105, 21.05.2020.
Research output: Contribution to journal › Article › Research › peer review
}
TY - JOUR
T1 - Adaptive density-guided approach to double incremental potential energy surface construction
AU - Artiukhin, Denis G.
AU - Klinting, Emil L.
AU - König, Carolin
AU - Christiansen, Ove
N1 - Funding Information: We thank Diana Madsen for providing us with the tetraphenyl and hexaphenyl FALCON coordinates and Leila Dzabbarova for exploratory computations on convergence of double incremental expansions. D.G.A. acknowledges funding from the European Union’s Horizon 2020 research and innovation programme under the Marie Skłodowska–Curie Grant Agreement No. 835776. C.K. acknowledges support from the Deutsche Forschungsgemeinschaft (DFG) through the Emmy Noether Young Group Leader Programme (Project No. KO 5423/1-1). O.C. acknowledges support from the Danish Council for Independent Research through a Sapere Aude III Grant (No. DFF-4002-00015).
PY - 2020/5/21
Y1 - 2020/5/21
N2 - We present a combination of the recently developed double incremental expansion of potential energy surfaces with the well-established adaptive density-guided approach to grid construction. This unique methodology is based on the use of an incremental expansion for potential energy surfaces, known as n-mode expansion; an incremental many-body representation of the electronic energy; and an efficient vibrational density-guided approach to automated determination of grid dimensions and granularity. The reliability of the method is validated calculating potential energy surfaces and obtaining fundamental excitation energies for three moderate-size chain-like molecular systems. The use of our methodology leads to considerable computational savings for potential energy surface construction compared to standard approaches while maintaining a high level of accuracy in the resulting potential energy surfaces. Additional investigations indicate that our method can be applied to covalently bound and strongly interacting molecular systems, even though these cases are known to be very unfavorable for fragmentation schemes. We therefore conclude that the presented methodology is a robust and flexible approach to potential energy surface construction, which introduces considerable computational savings without compromising the accuracy of vibrational spectra calculations.
AB - We present a combination of the recently developed double incremental expansion of potential energy surfaces with the well-established adaptive density-guided approach to grid construction. This unique methodology is based on the use of an incremental expansion for potential energy surfaces, known as n-mode expansion; an incremental many-body representation of the electronic energy; and an efficient vibrational density-guided approach to automated determination of grid dimensions and granularity. The reliability of the method is validated calculating potential energy surfaces and obtaining fundamental excitation energies for three moderate-size chain-like molecular systems. The use of our methodology leads to considerable computational savings for potential energy surface construction compared to standard approaches while maintaining a high level of accuracy in the resulting potential energy surfaces. Additional investigations indicate that our method can be applied to covalently bound and strongly interacting molecular systems, even though these cases are known to be very unfavorable for fragmentation schemes. We therefore conclude that the presented methodology is a robust and flexible approach to potential energy surface construction, which introduces considerable computational savings without compromising the accuracy of vibrational spectra calculations.
UR - http://www.scopus.com/inward/record.url?scp=85090131521&partnerID=8YFLogxK
U2 - 10.1063/5.0004686
DO - 10.1063/5.0004686
M3 - Article
VL - 152
JO - The journal of chemical physics
JF - The journal of chemical physics
SN - 0021-9606
IS - 19
M1 - 194105
ER -