The first principles molecular dynamics simulation of complex molecular fluids places severe demands on computational resources.  In this work, we study the structure of benzene liquids at ambient and elevated temperatures using Kohn-Sham density functional theory.  We compare results for the simulated radial and angular dependent structure of the fluid using numerical basis sets at the single zeta, double zeta, and triple zeta levels.  We find that single zeta results without orbital optimization yield results in poor agreement with experiment and with simulations employing larger basis sets.  By using numerical basis sets optimized specifically for benzene, we get results at the single zeta level comparable to what we find at the double and triple zeta levels.  Orbitals determined at ambient temperature also work well at elevated temperature. We find that we are able to subtantially accelerate our simulations of benzene while increasing the system simulation size by using the orbital optimization technique.

Efficient first principles molecular dynamics of benzene using orbital optimization

248th National Meeting (2014)

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