Abstract
We present NEXMD version 2.0, the second release of the NEXMD (Nonadiabatic EXcited-state Molecular Dynamics) software package. Across a variety of new features, NEXMD v2.0 incorporates new implementations of two hybrid quantum-classical dynamics methods, namely, Ehrenfest dynamics (EHR) and the Ab-Initio Multiple Cloning sampling technique for Multiconfigurational Ehrenfest quantum dynamics (MCE-AIMC or simply AIMC), which are alternative options to the previously implemented trajectory surface hopping (TSH) method. To illustrate these methodologies, we outline a direct comparison of these three hybrid quantum-classical dynamics methods as implemented in the same NEXMD framework, discussing their weaknesses and strengths, using the modeled photodynamics of a polyphenylene ethylene dendrimer building block as a representative example. We also describe the expanded normal-mode analysis and constraints for both the ground and excited states, newly implemented in the NEXMD v2.0 framework, which allow for a deeper analysis of the main vibrational motions involved in vibronic dynamics. Overall, NEXMD v2.0 expands the range of applications of NEXMD to a larger variety of multichromophore organic molecules and photophysical processes involving quantum coherences and persistent couplings between electronic excited states and nuclear velocity.
| Original language | English |
|---|---|
| Pages (from-to) | 5356-5368 |
| Number of pages | 13 |
| Journal | Journal of Chemical Theory and Computation |
| Volume | 19 |
| Issue number | 16 |
| DOIs | |
| State | Published - Aug 22 2023 |
| Externally published | Yes |
Funding
S.T. and V.M.F. acknowledges support from the U.S. DOE, Office of Science, Office of Basic Energy Sciences under Triad National Security, LLC (“Triad”) contract grant # 89233218CNA000001 (FWP: LANLE3T1). This work was performed in part at the Center for Integrated Nanotechnology (CINT) at the Los Alamos National Laboratory (LANL), a U.S. DOE and Office of Basic Energy Sciences user facility. This research used resources provided by the LANL Institutional Computing Program. Y.Z. and T.G. acknowledges the support from the Laboratory Directed Research and Development (LDRD) program of LANL. S.F.-A. and H.N.-Y. acknowledge the support of CONICET, UNQ, and ANPCyT (PICT 2018-02360). The work was supported by the Chemical Sciences, Geosciences, and Biosciences Division, Office of Basic Energy Sciences, Office of Science, U.S. DOE through Award DE-SC0022225. S.M. also acknowledges the Hagler Institute for Advanced Study at Texas A&M University, from which he is a fellow. L.N.M. and S.S. acknowledge the support from the National Science Foundation (NSF) under grant no. DMR-1847774 and from the Center for Complex and Active Materials at the University of California, Irvine (DMR-2011967). D.M. and D.S. acknowledge the support from EPSRC grant EP/P021123/1.