Non-adiabatic molecular dynamics (NA-MD) within the neglect-of-back-reaction approximation (NBRA) enables simulating NA processes in systems that are prohibitively too large to be studied using traditional NA-MD methods, such as Tully’s fewest switches surface hopping. However, NA-MD within the NBRA framework is still limited in its application, mostly due to the need to compute time-derivative NA couplings and form the vibrionic Hamiltonian. An alternative NA-MD method that does not require such computations is the Landau-Zener formulation of NAD, in which a surface hopping variant was developed by Tully and Preston. A reformulation of this method by Belyaev and Lebedev, dubbed Belyaev-Lebedev surface hopping (BLSH), allows for such dynamics to occur in the adiabatic basis, making it compatible with outputs of many community support electronic structure packages. In this work, we incorporate the BLSH method into the NBRA framework, and apply it to study the cooling of a hot electron in a series of hydrogen and fluorine capped silicon quantum dots. The electronic structure is carried out using the density functional tight binding plus software package, and the dynamics algorithms and post-processing routines are handling using the Libra software package.  Our results show that the NBRA-BLSH method can serve as an inexpensive and promising option for simulating NA processes in large atomistic system, as the method is able to capture expected trends in the NAD in agreement with experiments and previous theoretical studies.    <br/>

Simulating hot electron cooling in hydrogen and fluorine capped silicon quantum dots with Belyaev-Lebedev non-adiabatic dynamics within the neglect-of-back-reaction approximation

Macromolecular Chemistry: The Second Century

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ACS Spring 2020 National Meeting & Expo

The official archive and repository for all ACS Meetings & Expositions abstracts and select posters or presentations.