  Quantum chemical calculations on atomistic systems have evolved into a
standard approach to study molecular matter. These calculations often involve a
significant amount of manual input and expertise although most of this effort
could be automated, which would alleviate the need for expertise in software
and hardware accessibility. Here, we present the AutoRXN workflow, an automated
workflow for exploratory high-throughput lectronic structure calculations of
molecular systems, in which (i) density functional theory methods are exploited
to deliver minimum and transition-state structures and corresponding energies
and properties, (ii) coupled cluster calculations are then launched for
optimized structures to provide more accurate energy and property estimates,
and (iii) multi-reference diagnostics are evaluated to back check the coupled
cluster results and subject hem to automated multi-configurational calculations
for potential multi-configurational cases. All calculations are carried out in
a cloud environment and support massive computational campaigns. Key features
of all omponents of the AutoRXN workflow are autonomy, stability, and minimum
operator interference. We highlight the AutoRXN workflow at the example of an
autonomous reaction mechanism exploration of the mode of action of a
homogeneous catalyst for the asymmetric reduction of ketones.
