Two zero-carbon technologies that ultimately may be among civilization’s main sources of electricity and fuels are fusion for electricity and photocatalytic production of fuels. Computational science has an important role to play in testing out concepts and materials difficult to probe experimentally. This lecture briefly reviews two quantum mechanics methods developed in my research group over the past 20+ years – embedded correlated wavefunction (ECW) theory and orbital-free density functional theory (OFDFT). ECW theory locally refines the description of electrons to go beyond DFT approximations and their attendant errors in describing certain phenomena and classes of materials. As a result, ECW theory can accurately simulate, e.g., charge transfer and excited states at a metal catalyst surface. Here, we discuss how ECW ground and excited state potential energy surfaces provide insights into a novel photocatalysis process - plasmon-induced chemistry on metal nanoparticles – for production of fuels and chemicals.   Moving on to a simpler theory applicable to many thousands of atoms, OFDFT employs density functionals to evaluate not only the exchange-correlation energy but also the kinetic energy. The physics contained in the kinetic energy density functional largely determines OFDFT’s accuracy.  Current functionals – primarily developed in my group - are reliable for main group metals and semiconductors, and recent extensions to transition metals promise further generality.  Here, we discuss both first principles and classical MD simulations of liquid metals, with a focus on first wall materials under development for fusion reactors.<br/>

Insights from Ab initio potential energy surfaces and molecular dynamics for sustainable energy technologies

255th National Meeting (2018)

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