posted on 2024-01-31, 05:13authored byAlexandra Stan-Bernhardt, Liubov Glinkina, Andreas Hulm, Christian Ochsenfeld
In recent years,
first-principles exploration of chemical reaction
space has provided valuable insights into intricate reaction networks.
Here, we introduce ab initio hyperreactor dynamics,
which enables rapid screening of the accessible chemical space from
a given set of initial molecular species, predicting new synthetic
routes that can potentially guide subsequent experimental studies.
For this purpose, different hyperdynamics derived bias potentials
are applied along with pressure-inducing spherical confinement of
the molecular system in ab initio molecular dynamics
simulations to efficiently enhance reactivity under mild conditions.
To showcase the advantages and flexibility of the hyperreactor approach,
we present a systematic study of the method’s parameters on
a HCN toy model and apply it to a recently introduced experimental
model for the prebiotic formation of glycinal and acetamide in interstellar
ices, which yields results in line with experimental findings. In
addition, we show how the developed framework enables the study of
complicated transitions like the first step of a nonenzymatic DNA
nucleoside synthesis in an aqueous environment, where the molecular
fragmentation problem of earlier nanoreactor approaches is avoided.