Empirical Self-Consistent Correction for the Description of Hydrogen Bonds in DFTB3

Kód výsledku v IS VaVaI

<a href="https://www.isvavai.cz/riv?ss=detail&h=RIV%2F61388963%3A_____%2F17%3A00480913" target="_blank" >RIV/61388963:_____/17:00480913 - isvavai.cz</a>

Výsledek na webu

<a href="http://dx.doi.org/10.1021/acs.jctc.7b00629" target="_blank" >http://dx.doi.org/10.1021/acs.jctc.7b00629</a>

DOI - Digital Object Identifier

<a href="http://dx.doi.org/10.1021/acs.jctc.7b00629" target="_blank" >10.1021/acs.jctc.7b00629</a>

Jazyk výsledku

angličtina

Název v původním jazyce

Empirical Self-Consistent Correction for the Description of Hydrogen Bonds in DFTB3

Popis výsledku v původním jazyce

The description of hydrogen bonds in the density-functional tight-binding (DFTB) method continues to be a challenging task because the approximations that make the method computationally efficient compromise already the first-order electrostatic contribution to the interaction. So far, the best results have been achieved with fully empirical corrections such as the recently reparametrized DFTB3-D3H4 method. This approach has, however, important limitations that arise from its independence of the actual electronic structure. Here, we present a novel correction denoted as D3H5, which is integrated deeper in the DFTB method, correcting the problem at the place of its origin. It is applied within the self-consistent evaluation of electrostatic interactions, where it empirically models the missing contributions of atomic multipoles and polarization. Despite being very simple and using fewer parameters than D3H4, it is both more accurate and more robust. In data sets of small model systems, it yields errors below 1 kcal/mol, and it performs comparably well in larger systems. Unlike D3H4, it can describe cooperativity in H-bond networks, which makes it more transferable to more complex systems.

Název v anglickém jazyce

Empirical Self-Consistent Correction for the Description of Hydrogen Bonds in DFTB3

Popis výsledku anglicky

The description of hydrogen bonds in the density-functional tight-binding (DFTB) method continues to be a challenging task because the approximations that make the method computationally efficient compromise already the first-order electrostatic contribution to the interaction. So far, the best results have been achieved with fully empirical corrections such as the recently reparametrized DFTB3-D3H4 method. This approach has, however, important limitations that arise from its independence of the actual electronic structure. Here, we present a novel correction denoted as D3H5, which is integrated deeper in the DFTB method, correcting the problem at the place of its origin. It is applied within the self-consistent evaluation of electrostatic interactions, where it empirically models the missing contributions of atomic multipoles and polarization. Despite being very simple and using fewer parameters than D3H4, it is both more accurate and more robust. In data sets of small model systems, it yields errors below 1 kcal/mol, and it performs comparably well in larger systems. Unlike D3H4, it can describe cooperativity in H-bond networks, which makes it more transferable to more complex systems.

Druh

J_imp - Článek v periodiku v databázi Web of Science

CEP obor

—

OECD FORD obor

10403 - Physical chemistry

Projekt

<a href="/cs/project/GJ16-11321Y" target="_blank" >GJ16-11321Y: Rychlý kvantově-mechanický model pro popis nekovalentních interakcí ce velkých molekulárních systémech</a><br>

Návaznosti

P - Projekt vyzkumu a vyvoje financovany z verejnych zdroju (s odkazem do CEP)

Rok uplatnění

2017

Kód důvěrnosti údajů

S - Úplné a pravdivé údaje o projektu nepodléhají ochraně podle zvláštních právních předpisů

Název periodika

Journal of Chemical Theory and Computation

ISSN

1549-9618

e-ISSN

—

Svazek periodika

13

Číslo periodika v rámci svazku

10

Stát vydavatele periodika

US - Spojené státy americké

Počet stran výsledku

14

Strana od-do

4804-4817

Kód UT WoS článku

000412965700017

EID výsledku v databázi Scopus

2-s2.0-85032221772