Projection-Based Correlated Wave Function in Density Functional Theory Embedding for Periodic Systems

Dhabih V. Chulhai; Jason D. Goodpaster

doi:10.1021/acs.jctc.7b01154

Projection-Based Correlated Wave Function in Density Functional Theory Embedding for Periodic Systems

Dhabih V. Chulhai, Jason D. Goodpaster

Research output: Contribution to journal › Article › peer-review

69 Scopus citations

Abstract

We present a level shift projection operator-based embedding method for systems with periodic boundary conditions - where the "active" subsystem can be described using either density functional theory (DFT) or correlated wave function (WF) methods and the "environment" is described using DFT. Our method allows for k-point sampling, is shown to be exactly equal to the canonical DFT solution of the full system under the limit that we use the full system basis to describe each subsystem, and can treat the active subsystem either with periodic boundary conditions - in what we term "periodic-in-periodic" embedding - or as a molecular cluster - in "cluster-in-periodic" embedding. We explore each of these methods and show that cluster WF-in-periodic DFT embedding can accurately calculate the absorption energy of CO on to a Si(100)-2×1 surface.

Original language	English (US)
Pages (from-to)	1928-1942
Number of pages	15
Journal	Journal of Chemical Theory and Computation
Volume	14
Issue number	4
DOIs	https://doi.org/10.1021/acs.jctc.7b01154
State	Published - Apr 10 2018

Bibliographical note

Funding Information:
This research was carried out within the Nanoporous Materials Genome Center, which is supported by the U.S. Department of Energy, Office of Basic Energy Sciences, Division of Chemical Sciences, Geosciences, and Biosciences under Award DE-FG02-12ER16362. The authors acknowledge the Minnesota Supercomputing Institute (MSI) at the University of Minnesota and the National Energy Research Scientific Computing Center (NERSC), a DOE Office of Science User Facility supported by the Office of Science of the U.S. Department of Energy under Contract No. DE-AC02-05CH11231, for providing resources that contributed to the results reported within this paper.

Funding Information:
This research was carried out within the Nanoporous Materials Genome Center, which is supported by the U.S. Department of Energy, Office of Basic Energy Sciences, Division of Chemical Sciences Geosciences, and Biosciences under Award DE-FG02-12ER16362. The authors acknowledge the Minnesota Supercomputing Institute (MSI) at the University of Minnesota and the National Energy Research Scientific Computing Center (NERSC), a DOE Office of Science User Facility supported by the Office of Science of the U.S. Department of Energy under Contract No. DE-AC02-05CH11231, for providing resources that contributed to the results reported within this paper.

Publisher Copyright:
© 2018 American Chemical Society.

Access

10.1021/acs.jctc.7b01154

OpenUrl availability

Full text

Cite this

@article{cbf525b87b6e4589a122b9dc5fc8586b,

title = "Projection-Based Correlated Wave Function in Density Functional Theory Embedding for Periodic Systems",

abstract = "We present a level shift projection operator-based embedding method for systems with periodic boundary conditions - where the {"}active{"} subsystem can be described using either density functional theory (DFT) or correlated wave function (WF) methods and the {"}environment{"} is described using DFT. Our method allows for k-point sampling, is shown to be exactly equal to the canonical DFT solution of the full system under the limit that we use the full system basis to describe each subsystem, and can treat the active subsystem either with periodic boundary conditions - in what we term {"}periodic-in-periodic{"} embedding - or as a molecular cluster - in {"}cluster-in-periodic{"} embedding. We explore each of these methods and show that cluster WF-in-periodic DFT embedding can accurately calculate the absorption energy of CO on to a Si(100)-2×1 surface.",

author = "Chulhai, {Dhabih V.} and Goodpaster, {Jason D.}",

note = "Funding Information: This research was carried out within the Nanoporous Materials Genome Center, which is supported by the U.S. Department of Energy, Office of Basic Energy Sciences, Division of Chemical Sciences, Geosciences, and Biosciences under Award DE-FG02-12ER16362. The authors acknowledge the Minnesota Supercomputing Institute (MSI) at the University of Minnesota and the National Energy Research Scientific Computing Center (NERSC), a DOE Office of Science User Facility supported by the Office of Science of the U.S. Department of Energy under Contract No. DE-AC02-05CH11231, for providing resources that contributed to the results reported within this paper. Funding Information: This research was carried out within the Nanoporous Materials Genome Center, which is supported by the U.S. Department of Energy, Office of Basic Energy Sciences, Division of Chemical Sciences Geosciences, and Biosciences under Award DE-FG02-12ER16362. The authors acknowledge the Minnesota Supercomputing Institute (MSI) at the University of Minnesota and the National Energy Research Scientific Computing Center (NERSC), a DOE Office of Science User Facility supported by the Office of Science of the U.S. Department of Energy under Contract No. DE-AC02-05CH11231, for providing resources that contributed to the results reported within this paper. Publisher Copyright: {\textcopyright} 2018 American Chemical Society.",

year = "2018",

month = apr,

day = "10",

doi = "10.1021/acs.jctc.7b01154",

language = "English (US)",

volume = "14",

pages = "1928--1942",

journal = "Journal of Chemical Theory and Computation",

issn = "1549-9618",

publisher = "American Chemical Society",

number = "4",

}

TY - JOUR

T1 - Projection-Based Correlated Wave Function in Density Functional Theory Embedding for Periodic Systems

AU - Chulhai, Dhabih V.

AU - Goodpaster, Jason D.

N1 - Funding Information: This research was carried out within the Nanoporous Materials Genome Center, which is supported by the U.S. Department of Energy, Office of Basic Energy Sciences, Division of Chemical Sciences, Geosciences, and Biosciences under Award DE-FG02-12ER16362. The authors acknowledge the Minnesota Supercomputing Institute (MSI) at the University of Minnesota and the National Energy Research Scientific Computing Center (NERSC), a DOE Office of Science User Facility supported by the Office of Science of the U.S. Department of Energy under Contract No. DE-AC02-05CH11231, for providing resources that contributed to the results reported within this paper. Funding Information: This research was carried out within the Nanoporous Materials Genome Center, which is supported by the U.S. Department of Energy, Office of Basic Energy Sciences, Division of Chemical Sciences Geosciences, and Biosciences under Award DE-FG02-12ER16362. The authors acknowledge the Minnesota Supercomputing Institute (MSI) at the University of Minnesota and the National Energy Research Scientific Computing Center (NERSC), a DOE Office of Science User Facility supported by the Office of Science of the U.S. Department of Energy under Contract No. DE-AC02-05CH11231, for providing resources that contributed to the results reported within this paper. Publisher Copyright: © 2018 American Chemical Society.

PY - 2018/4/10

Y1 - 2018/4/10

N2 - We present a level shift projection operator-based embedding method for systems with periodic boundary conditions - where the "active" subsystem can be described using either density functional theory (DFT) or correlated wave function (WF) methods and the "environment" is described using DFT. Our method allows for k-point sampling, is shown to be exactly equal to the canonical DFT solution of the full system under the limit that we use the full system basis to describe each subsystem, and can treat the active subsystem either with periodic boundary conditions - in what we term "periodic-in-periodic" embedding - or as a molecular cluster - in "cluster-in-periodic" embedding. We explore each of these methods and show that cluster WF-in-periodic DFT embedding can accurately calculate the absorption energy of CO on to a Si(100)-2×1 surface.

AB - We present a level shift projection operator-based embedding method for systems with periodic boundary conditions - where the "active" subsystem can be described using either density functional theory (DFT) or correlated wave function (WF) methods and the "environment" is described using DFT. Our method allows for k-point sampling, is shown to be exactly equal to the canonical DFT solution of the full system under the limit that we use the full system basis to describe each subsystem, and can treat the active subsystem either with periodic boundary conditions - in what we term "periodic-in-periodic" embedding - or as a molecular cluster - in "cluster-in-periodic" embedding. We explore each of these methods and show that cluster WF-in-periodic DFT embedding can accurately calculate the absorption energy of CO on to a Si(100)-2×1 surface.

UR - http://www.scopus.com/inward/record.url?scp=85045202883&partnerID=8YFLogxK

UR - http://www.scopus.com/inward/citedby.url?scp=85045202883&partnerID=8YFLogxK

U2 - 10.1021/acs.jctc.7b01154

DO - 10.1021/acs.jctc.7b01154

M3 - Article

C2 - 29494155

AN - SCOPUS:85045202883

SN - 1549-9618

VL - 14

SP - 1928

EP - 1942

JO - Journal of Chemical Theory and Computation

JF - Journal of Chemical Theory and Computation

IS - 4

ER -

Projection-Based Correlated Wave Function in Density Functional Theory Embedding for Periodic Systems

Abstract

Bibliographical note

Access

OpenUrl availability

Other files and links

Fingerprint

NMGC: Nanoporous Materials Genome: Methods and Software to Optimize Gas Storage, Separations, and Catalysis (Phase 2)

Cite this

Projection-Based Correlated Wave Function in Density Functional Theory Embedding for Periodic Systems

Abstract

Bibliographical note

Access

OpenUrl availability

Other files and links

Fingerprint

Projects

NMGC: Nanoporous Materials Genome: Methods and Software to Optimize Gas Storage, Separations, and Catalysis (Phase 2)

Cite this