TimeSOAP: Tracking high-dimensional fluctuations in complex molecular systems via time-variations of SOAP spectra (2302.09673v2)

Abstract: Many molecular systems and physical phenomena are controlled by local fluctuations and microscopic dynamical rearrangements of the constitutive interacting units that are often difficult to detect. This is the case, for example, of phase transitions, phase equilibria, nucleation events, and defect propagation, to mention a few. A detailed comprehension of local atomic environments and of their dynamic rearrangements is essential to understand such phenomena, and also to draw structure-property relationships useful to unveil how to control complex molecular systems. Considerable progresses in the development of advanced high-dimensional structural descriptors (e.g., Smooth Overlap of Atomic Position (SOAP), etc.) have certainly enhanced the representation of atomic-scale simulations data. However, despite such efforts, local dynamic environment rearrangements remain still difficult to elucidate. Here, exploiting the structural-rich description of atomic environments of SOAP and building on the concept of time-dependent local variations, we developed a time-dependent SOAP-based descriptor, TimeSOAP (tSOAP), which essentially tracks the time variations in the local SOAP environments surrounding each molecule (i.e., each SOAP center) in complex molecular systems along ensemble trajectories. We demonstrate how analysis of the time-series {tSOAP data and of their time-derivatives allows detecting dynamics domains and tracking instantaneous changes of local atomic arrangements (i.e., local fluctuations) in a variety of molecular systems. The approach is simple and general, and we expect will help to shed light on a variety of complex dynamical phenomena.