Assessing weak hydrogen binding on Ca+ centers: An accurate many-body study with large basis sets
Abstract
Weak H2 physisorption energies present a significant challenge to even the best correlated theoretical many-body methods. We use the phaseless auxiliary-field quantum Monte Carlo method to accurately predict the binding energy of Ca+– 4H2. Attention has recently focused on this model chemistry to test the reliability of electronic structure methods for H2 binding on dispersed alkaline earth metal centers. A modified Cholesky decomposition is implemented to realize the Hubbard-Stratonovich transformation efficiently with large Gaussian basis sets. We employ the largest correlation-consistent Gaussian type basis sets available, up to cc-pCV5Z for Ca, to accurately extrapolate to the complete basis limit. The calculated potential energy curve exhibits binding with a double-well structure.
Document Details
- Document Type
- Pub Defense Publication
- Publication Date
- Oct 28, 2011
- Source ID
- 10.1063/1.3654002
Entities
People
- Henry Krakauer
- Shiwei Zhang
- Wirawan Purwanto
- Yudistira Virgus
Organizations
- College of William & Mary
- National Science Foundation
- Office of Naval Research
- United States Department of Energy