Addressing Dynamics at Catalytic Heterogeneous Interfaces with DFT-MD: Anomalous Temperature Distributions from Commonly Used Thermostats.

Density functional theory-based molecular dynamics (DFT-MD) has been widely used for studying the chemistry of heterogeneous interfacial systems under operational conditions. We report frequently overlooked errors in thermostated or constant-temperature DFT-MD simulations applied to study (electro)catalytic chemistry. Our results demonstrate that commonly used thermostats such as Nosé-Hoover, Berendsen, and simple velocity-rescaling methods fail to provide a reliable temperature description for systems considered.