Accurate calculation of hydrogen abstraction reaction barriers is a challenging problem, often requiring high level quantum chemistry methods that scale poorly with system size. Quantum Monte Carlo (QMC) methods provide an alternative approach that exhibit much better scaling, but these methods are still computationally expensive. We describe approaches that can significantly reduce the cost of QMC calculations of barrier heights, using the hydrogen abstraction of methanol by a hydrogen atom as an illustrative example. By analysing the combined influence of trial wavefunctions and pseudopotential quadrature settings on the barrier heights, variance, and timestep errors, we devise a simple protocol that minimizes the cost of the QMC calculations while retaining accuracy comparable to large-basis coupled cluster theory. We demonstrate that this protocol is transferable to other hydrogen abstraction reactions.
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North Carolina State Univ, Dept Phys, Raleigh, NC 27695 USA
North Carolina State Univ, CHiPS, Raleigh, NC 27695 USAUniv Ostrava, Dept Phys, 30 Dubna 22, Ostrava 70103, Czech Republic
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Univ Trento, Phys Dept, Via Sommarive 14, I-38123 Trento, ItalyUniv Trento, Phys Dept, Via Sommarive 14, I-38123 Trento, Italy
Massella, P.
Barranco, F.
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Univ Seville, Dept Fis Aplicada 3, Escuela Super Ingn, Camino Descubrimientos, Seville, SpainUniv Trento, Phys Dept, Via Sommarive 14, I-38123 Trento, Italy
Barranco, F.
Lonardoni, D.
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Michigan State Univ, Facil Rare Isotope Beams, E Lansing, MI 48824 USA
Los Alamos Natl Lab, Theoret Div, Los Alamos, NM 87545 USAUniv Trento, Phys Dept, Via Sommarive 14, I-38123 Trento, Italy
Lonardoni, D.
Lovato, A.
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INFN TIFPA Trento Inst Fundamental Phys & Applica, I-38123 Trento, Italy
Argonne Natl Lab, Phys Div, 9700 S Cass Ave, Argonne, IL 60439 USAUniv Trento, Phys Dept, Via Sommarive 14, I-38123 Trento, Italy
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Imperial Coll London, Dept Mat Sci, Royal Sch Mines, Thomas Young Ctr,London Ctr Nanotechnol, London SW7 2AZ, EnglandImperial Coll London, Dept Mat Sci, Royal Sch Mines, Thomas Young Ctr,London Ctr Nanotechnol, London SW7 2AZ, England
Azadi, Sam
Kuhne, Thomas D.
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Univ Paderborn, Dept Chem, Dynam Condensed Matter, Warburger Str 100, D-33098 Paderborn, Germany
Univ Paderborn, Paderborn Ctr Parallel Comp, Warburger Str 100, D-33098 Paderborn, Germany
Univ Paderborn, Inst Lightweight Design Hybrid Syst, Warburger Str 100, D-33098 Paderborn, GermanyImperial Coll London, Dept Mat Sci, Royal Sch Mines, Thomas Young Ctr,London Ctr Nanotechnol, London SW7 2AZ, England
机构:
North Carolina State Univ, Dept Phys, Raleigh, NC 27695 USA
North Carolina State Univ, CHiPS, Raleigh, NC 27695 USAUniv Ostrava, Dept Phys, 30 Dubna 22, Ostrava 70103, Czech Republic
机构:
Univ Trento, Phys Dept, Via Sommarive 14, I-38123 Trento, ItalyUniv Trento, Phys Dept, Via Sommarive 14, I-38123 Trento, Italy
Massella, P.
Barranco, F.
论文数: 0引用数: 0
h-index: 0
机构:
Univ Seville, Dept Fis Aplicada 3, Escuela Super Ingn, Camino Descubrimientos, Seville, SpainUniv Trento, Phys Dept, Via Sommarive 14, I-38123 Trento, Italy
Barranco, F.
Lonardoni, D.
论文数: 0引用数: 0
h-index: 0
机构:
Michigan State Univ, Facil Rare Isotope Beams, E Lansing, MI 48824 USA
Los Alamos Natl Lab, Theoret Div, Los Alamos, NM 87545 USAUniv Trento, Phys Dept, Via Sommarive 14, I-38123 Trento, Italy
Lonardoni, D.
Lovato, A.
论文数: 0引用数: 0
h-index: 0
机构:
INFN TIFPA Trento Inst Fundamental Phys & Applica, I-38123 Trento, Italy
Argonne Natl Lab, Phys Div, 9700 S Cass Ave, Argonne, IL 60439 USAUniv Trento, Phys Dept, Via Sommarive 14, I-38123 Trento, Italy
机构:
Imperial Coll London, Dept Mat Sci, Royal Sch Mines, Thomas Young Ctr,London Ctr Nanotechnol, London SW7 2AZ, EnglandImperial Coll London, Dept Mat Sci, Royal Sch Mines, Thomas Young Ctr,London Ctr Nanotechnol, London SW7 2AZ, England
Azadi, Sam
Kuhne, Thomas D.
论文数: 0引用数: 0
h-index: 0
机构:
Univ Paderborn, Dept Chem, Dynam Condensed Matter, Warburger Str 100, D-33098 Paderborn, Germany
Univ Paderborn, Paderborn Ctr Parallel Comp, Warburger Str 100, D-33098 Paderborn, Germany
Univ Paderborn, Inst Lightweight Design Hybrid Syst, Warburger Str 100, D-33098 Paderborn, GermanyImperial Coll London, Dept Mat Sci, Royal Sch Mines, Thomas Young Ctr,London Ctr Nanotechnol, London SW7 2AZ, England