Trail-Needs pseudopotentials in quantum Monte Carlo calculations with plane-wave/blip basis sets

Physics

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1607.01544v2
Rights statement: © 2016 American Physical Society
Accepted author manuscript, 293 KB, PDF document

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Trail-Needs pseudopotentials in quantum Monte Carlo calculations with plane-wave/blip basis sets. / Drummond, Neil David; Trail, J. R.; Needs, Richard.
In: Physical review B, Vol. 94, No. 16, 165170, 15.10.2016.

Research output: Contribution to Journal/Magazine › Journal article › peer-review

Bibtex

@article{5f7a368030df43ec939ef7748d199d02,

title = "Trail-Needs pseudopotentials in quantum Monte Carlo calculations with plane-wave/blip basis sets",

abstract = "We report a systematic analysis of the performance of a widely used set of Dirac-Fock pseudopotentials for quantum Monte Carlo (QMC) calculations. We study each atom in the periodic table from hydrogen (Z = 1) to mercury (Z = 80), with the exception of the 4f elements (57 ≤ Z ≤ 70).We demonstrate that ghost states are a potentially serious problem when plane-wave basis sets are used in density functional theory (DFT) orbital-generation calculations, but that this problem can be almost entirely eliminated by choosing the s channel to be local in the DFT calculation; thed channel can then be chosen to be local in subsequent QMC calculations, which generally leadsto more accurate results. We investigate the achievable energy variance per electron with differentlevels of trial wave function and we determine appropriate plane-wave cutoff energies for DFT calculations for each pseudopotential. We demonstrate that the so-called “T-move” scheme in diffusion Monte Carlo is essential for many elements. We investigate the optimal choice of spherical integration rule for pseudopotential projectors in QMC calculations. The information reported here will prove crucial in the planning and execution of QMC projects involving beyond-first-row elements.",

author = "Drummond, {Neil David} and Trail, {J. R.} and Richard Needs",

note = "{\textcopyright} 2016 American Physical Society",

year = "2016",

month = oct,

day = "15",

language = "English",

volume = "94",

journal = "Physical review B",

issn = "1098-0121",

publisher = "AMER PHYSICAL SOC",

number = "16",

}

RIS

TY - JOUR

T1 - Trail-Needs pseudopotentials in quantum Monte Carlo calculations with plane-wave/blip basis sets

AU - Drummond, Neil David

AU - Trail, J. R.

AU - Needs, Richard

PY - 2016/10/15

Y1 - 2016/10/15

N2 - We report a systematic analysis of the performance of a widely used set of Dirac-Fock pseudopotentials for quantum Monte Carlo (QMC) calculations. We study each atom in the periodic table from hydrogen (Z = 1) to mercury (Z = 80), with the exception of the 4f elements (57 ≤ Z ≤ 70).We demonstrate that ghost states are a potentially serious problem when plane-wave basis sets are used in density functional theory (DFT) orbital-generation calculations, but that this problem can be almost entirely eliminated by choosing the s channel to be local in the DFT calculation; thed channel can then be chosen to be local in subsequent QMC calculations, which generally leadsto more accurate results. We investigate the achievable energy variance per electron with differentlevels of trial wave function and we determine appropriate plane-wave cutoff energies for DFT calculations for each pseudopotential. We demonstrate that the so-called “T-move” scheme in diffusion Monte Carlo is essential for many elements. We investigate the optimal choice of spherical integration rule for pseudopotential projectors in QMC calculations. The information reported here will prove crucial in the planning and execution of QMC projects involving beyond-first-row elements.

AB - We report a systematic analysis of the performance of a widely used set of Dirac-Fock pseudopotentials for quantum Monte Carlo (QMC) calculations. We study each atom in the periodic table from hydrogen (Z = 1) to mercury (Z = 80), with the exception of the 4f elements (57 ≤ Z ≤ 70).We demonstrate that ghost states are a potentially serious problem when plane-wave basis sets are used in density functional theory (DFT) orbital-generation calculations, but that this problem can be almost entirely eliminated by choosing the s channel to be local in the DFT calculation; thed channel can then be chosen to be local in subsequent QMC calculations, which generally leadsto more accurate results. We investigate the achievable energy variance per electron with differentlevels of trial wave function and we determine appropriate plane-wave cutoff energies for DFT calculations for each pseudopotential. We demonstrate that the so-called “T-move” scheme in diffusion Monte Carlo is essential for many elements. We investigate the optimal choice of spherical integration rule for pseudopotential projectors in QMC calculations. The information reported here will prove crucial in the planning and execution of QMC projects involving beyond-first-row elements.

M3 - Journal article

VL - 94

JO - Physical review B

JF - Physical review B

SN - 1098-0121

IS - 16

M1 - 165170

ER -

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