Atomistic simulations of the free-energy landscapes of interstellar chemical reactions: the case of methyl isocyanate

Kód výsledku v IS VaVaI

<a href="https://www.isvavai.cz/riv?ss=detail&h=RIV%2F68081707%3A_____%2F21%3A00555333" target="_blank" >RIV/68081707:_____/21:00555333 - isvavai.cz</a>

Výsledek na webu

<a href="https://academic.oup.com/mnras/article-abstract/504/2/1565/6219088?redirectedFrom=fulltext" target="_blank" >https://academic.oup.com/mnras/article-abstract/504/2/1565/6219088?redirectedFrom=fulltext</a>

DOI - Digital Object Identifier

<a href="http://dx.doi.org/10.1093/mnras/stab958" target="_blank" >10.1093/mnras/stab958</a>

Jazyk výsledku

angličtina

Název v původním jazyce

Atomistic simulations of the free-energy landscapes of interstellar chemical reactions: the case of methyl isocyanate

Popis výsledku v původním jazyce

Although complex organic molecules are observed in a wide variety of environments, chemical reaction networks heading to their formation are higly debated. It is a major endeavour to model the rates of reactions and incorporate them into chemical networks. The vast majority of the computational investigations in astrochemistry take into consideration oversimplified molecular models where chemical reactions are simulated under vacuum conditions (gas phase) and with crudely approximated entropic contributions to the free energy. We use density functional theory-based molecular dynamics techniques coupled with state-of-the-art metadynamics methods to investigate the role of ices embedding the reactants in shaping the free-energy landscape of selected reactions. Ices are chemically defined at the same level of theory of the reactants themselves. We consider as test case the transformation of methane and isocyanic acid into molecular hydrogen and methyl isocyanate, a species bearing similarities with peptide bonds. We examine the thermodynamically unfavoured case of very stable reactants to magnify modifications in the energy configuration induced by a solid amorphous water ice, either pure or mixed with CO. The presence of an active medium modifies significantly the free-energy surface, widening the path connecting reactants and products, and decreasing substantially the energy barriers. Ices not only act as gatherers of reactants, but also create thermodynamic conditions favouring chemical evolution.

Název v anglickém jazyce

Atomistic simulations of the free-energy landscapes of interstellar chemical reactions: the case of methyl isocyanate

Popis výsledku anglicky

Although complex organic molecules are observed in a wide variety of environments, chemical reaction networks heading to their formation are higly debated. It is a major endeavour to model the rates of reactions and incorporate them into chemical networks. The vast majority of the computational investigations in astrochemistry take into consideration oversimplified molecular models where chemical reactions are simulated under vacuum conditions (gas phase) and with crudely approximated entropic contributions to the free energy. We use density functional theory-based molecular dynamics techniques coupled with state-of-the-art metadynamics methods to investigate the role of ices embedding the reactants in shaping the free-energy landscape of selected reactions. Ices are chemically defined at the same level of theory of the reactants themselves. We consider as test case the transformation of methane and isocyanic acid into molecular hydrogen and methyl isocyanate, a species bearing similarities with peptide bonds. We examine the thermodynamically unfavoured case of very stable reactants to magnify modifications in the energy configuration induced by a solid amorphous water ice, either pure or mixed with CO. The presence of an active medium modifies significantly the free-energy surface, widening the path connecting reactants and products, and decreasing substantially the energy barriers. Ices not only act as gatherers of reactants, but also create thermodynamic conditions favouring chemical evolution.

Druh

J_imp - Článek v periodiku v databázi Web of Science

CEP obor

—

OECD FORD obor

10308 - Astronomy (including astrophysics,space science)

Projekt

—

Návaznosti

I - Institucionalni podpora na dlouhodoby koncepcni rozvoj vyzkumne organizace

Rok uplatnění

2021

Kód důvěrnosti údajů

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

Název periodika

Monthly Notices of the Royal Astronomical Society

ISSN

0035-8711

e-ISSN

1365-2966

Svazek periodika

504

Číslo periodika v rámci svazku

2

Stát vydavatele periodika

GB - Spojené království Velké Británie a Severního Irska

Počet stran výsledku

6

Strana od-do

1565-1570

Kód UT WoS článku

000659453800002

EID výsledku v databázi Scopus

2-s2.0-85106630758