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As popular mixed quantum–classical dynamics methods, trajectory surface hopping and Ehrenfest mean field have been widely utilized to simulate nonadiabatic dynamics. Recently, we have proposed the branching-corrected surface hopping and the branching-corrected mean field methods, both of which closely reproduce the exact quantum dynamics in a series of standard scattering models. Here, the mixed surface hopping and mean field with branching correction (BCSHMF) is presented as a unified framework of mixed quantum–classical dynamics. As benchmarked in thousands of diverse three-level and four-level scattering models, BCSHMF achieves high reliability and flexibility, implying that surface hopping and mean field are compatible with each other in nature, and trajectory branching is essential for the mixed quantum–classical description of nonadiabatic dynamics. [ABSTRACT FROM AUTHOR]

Since the seminal work of Tully [J. Chem. Phys. 93, 1061 (1990)], two-level scattering models have been extensively adopted as the standard benchmark systems to assess the performance of different trajectory surface hopping methods for nonadiabatic dynamics simulations. Here, we extend the branching and phase corrections to multilevel systems and combine them with both the traditional fewest switches surface hopping (FSSH) and its variant global flux surface hopping (GFSH) algorithms. To get a comprehensive evaluation of the proposed methods, we construct a series of more challenging and diverse three-level and four-level scattering models and use exact quantum solutions as references. Encouragingly, both FSSH and GFSH with the branching and phase corrections produce excellent and nearly identical results in all investigated systems, indicating that the new surface hopping methods are robust to describe multilevel problems and the reliability is insensitive to the definition of self-consistent hopping probabilities in the adiabatic representation. Furthermore, the branching correction is found to be especially important when dealing with strongly repulsive potential energy surfaces, which are common in realistic systems, thus promising for general applications. [ABSTRACT FROM AUTHOR]

Cooling based on the electrocaloric effect (ECE) is a promising solution to environmental and energy efficiency problems of vapor-compression refrigeration. Ferroelectric polymer-ceramics nanocomposites, integrating high electric breakdown of organic ferroelectrics and large EC strength of ceramics, are attractive EC materials. Here, we tuned the orientation of Ba 0.67 Sr 0.33 TiO 3 nanofibers (BST nfs) in the P(VDF-TrFE-CFE) polymer. When the nfs were aligned parallel to the field, a Δ T of 11.3 K with an EC strength of 0.16 K·m/MV was achieved in the blends. The EC strength not only surpasses advanced nanocomposites but also is comparable to ferroelectric ceramics. The simulation indicates that a significantly higher electric field is concentrated in polymer regions around the ends of the orientated nfs, contributing to easier flipping of polymer chains for large ECE. This work provides a new method to obtain large ECE in composites for next-generation refrigeration.