A variety of interesting chemical phenomena require the accurate modeling of electronic and nuclear dynamics over a broad range of configuration space.  For example, strong and/or shaped laser pulses can be used to selectively initiate chemical reactions (i.e. break chemical bonds).  Accurately modeling these processes requires time-dependent electronic structure tools capable of accurately and efficiently describing statically correlated chemical systems.  Toward this end, we have developed graphics processing unit accelerated time-dependent complete active space configuration interaction (TD-CASCI) and multireference configuration interaction singles (TD-MRCIS) tools.  Akin to time-independent direct configuration interaction methods, our algorithm does not require formation or storage of any data structures with the full dimension of the Hamiltonian, enabling choice of large configuration spaces.  These tools have been applied to predict the response of large, strongly correlated molecules (up to decacene; C<sub>42</sub>H<sub>24</sub>) in strong laser fields.  Numerical issues, choice of orbitals, coupling to nuclear dynamics, and possible pitfalls of self-consistent orbital calculation will be discussed.

Modeling dynamics of strongly correlated systems with graphics processing unit–accelerated time-dependent multireference methods

2019 Spring National Meeting

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