Electronic structure of water from Koopmans-compliant functionals
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{
"revision": 2,
"id": "953",
"created": "2021-07-19T22:44:56.653284+00:00",
"metadata": {
"doi": "10.24435/materialscloud:76-zf",
"status": "published",
"title": "Electronic structure of water from Koopmans-compliant functionals",
"mcid": "2021.114",
"license_addendum": null,
"_files": [
{
"description": "Description of each file",
"key": "README.txt",
"size": 1322,
"checksum": "md5:93545562fc26f71537d691c3c28935f7"
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{
"description": "Snapshot used for rescaling the O-H bond lengths of water molecules, being the 11th step the non-rescaled one, 1 to 10 with lower O-H bond lengths, and 12 to 21 with longer O-H bond lengths. Cubic box of side 9.8667 Angstroms.",
"key": "Rescaled-Snapshot.tgz",
"size": 32883,
"checksum": "md5:430cd1b617e67f05e4297cba867f747c"
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{
"description": "20 snapshots collected from a classical molecular dynamics with 64 water molecules, using the SPCE-FH force field. Simulation at 300 K with a cubic box with a side of 12.415 Angstroms.\nSimulation at 300 K with a cubic box with a side of 12.415 Angstroms.",
"key": "SPCE-FH.tgz",
"size": 57709,
"checksum": "md5:849cd271cc4bdcb57de40a69bbe46d82"
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{
"description": "20 snapshots collected from a classical molecular dynamics with 64 water molecules, using the TIP4P force field. Simulation at 300 K with a cubic box with a side of 12.415 Angstroms.",
"key": "TIP4P.tgz",
"size": 11400522,
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"owner": 438,
"_oai": {
"id": "oai:materialscloud.org:953"
},
"keywords": [
"water",
"band gap",
"molecular dynamics",
"nuclear quantum effects",
"MARVEL"
],
"conceptrecid": "924",
"is_last": true,
"references": [
{
"type": "Journal reference",
"doi": "10.1021/acs.jctc.1c00063",
"url": "https://doi.org/10.1021/acs.jctc.1c00063",
"citation": "James M. de Almeida, et al., J. Chem. Theory Comput. 2021, 17, 7, 3923\u20133930"
},
{
"type": "Preprint",
"url": "https://arxiv.org/abs/2106.11994",
"citation": "James M. Almeida, et al., eprint arXiv:2106.11994"
},
{
"type": "Website",
"doi": "10.24435/materialscloud:2018.0023/v1",
"url": "https://doi.org/10.24435/materialscloud:2018.0023/v1",
"comment": "Includes the ab initio trajectories",
"citation": "Wei Chen, Francesco Ambrosio, Giacomo Miceli, Alfredo Pasquarello, materialscloud:2018.0023/v1"
}
],
"publication_date": "Jul 20, 2021, 10:54:53",
"license": "Creative Commons Attribution 4.0 International",
"id": "953",
"description": "Obtaining a precise theoretical description of the spectral properties of liquid water poses challenges for both molecular dynamics (MD) and electronic structure methods. The lower computational cost of the Koopmans-compliant functionals with respect to Green\u2019s function methods allows the simulations of many MD trajectories, with a description close to the state-of-art quasi-particle self-consistent GW plus vertex corrections method (QSGW + fxc). Thus, we explore water spectral properties when different MD approaches are used, ranging from classical MD to first-principles MD, and including nuclear quantum effects. We have observed that different MD approaches lead to up to 1 eV change in the average band gap; thus, we focused on the band gap dependence with the geometrical properties of a system to explain such spread. We have evaluated the changes in the band gap due to variations in the intramolecular O\u2013H bond distance and HOH angle, as well as the intermolecular hydrogen bond O\u00b7\u00b7\u00b7O distance and the OHO angles. We have observed that the dominant contribution comes from the O\u2013H bond length; the O\u00b7\u00b7\u00b7O distance plays a secondary role, and the other geometrical properties do not significantly influence the gap. Furthermore, we analyze the electronic density of states (DOS), where the KIPZ functional shows good agreement with the DOS obtained with state-of-art approaches employing quasi-particle self-consistent GW plus vertex corrections. The O\u2013H bond length also significantly influences the DOS. When nuclear quantum effects are considered, broadening of the peaks driven by the broader distribution of the O\u2013H bond lengths is observed, leading to a closer agreement with the experimental photoemission spectra.",
"version": 2,
"contributors": [
{
"email": "james.almeida@ufabc.edu.br",
"affiliations": [
"Universidade Federal do ABC, Centro de Ci\u00eancias Naturais e Humanas, Santo Andr\u00e9, 09210-580 SP, Brazil",
"Theory and Simulation of Materials (THEOS) and National Centre for Computational Design and Discovery of Novel Materials (MARVEL), Ecole Polytechnique F\u00e9d\u00e9rale de Lausanne (EPFL), CH-1015 Lausanne, Switzerland"
],
"familyname": "Moraes de Almeida",
"givennames": "James"
},
{
"affiliations": [
"Theory and Simulation of Materials (THEOS) and National Centre for Computational Design and Discovery of Novel Materials (MARVEL), Ecole Polytechnique F\u00e9d\u00e9rale de Lausanne (EPFL), CH-1015 Lausanne, Switzerland"
],
"familyname": "Linh Nguyen",
"givennames": "Ngoc"
},
{
"affiliations": [
"Laboratory for Neutron Scattering and Imaging, Paul Scherrer Institute, CH-5232 Villigen-PSI, Switzerland",
"National Centre for Computational Design and Discovery of Novel Materials (MARVEL), \u00c9cole Polytechnique F\u00e9d\u00e9rale de Lausanne, CH-1015 Lausanne, Switzerland"
],
"familyname": "Colonna",
"givennames": "Nicola"
},
{
"affiliations": [
"Institute of Condensed Matter and Nanoscience, Universit\u00e9 Catholique de Louvain, B-1348 Louvain-la-Neuve, Belgium"
],
"familyname": "Chen",
"givennames": "Wei"
},
{
"affiliations": [
"Instituto de F\u00edsica, Universidade de S\u00e3o Paulo, S\u00e3o Paulo, 05508-090 SP, Brazil"
],
"familyname": "Rodrigues Miranda",
"givennames": "Caetano"
},
{
"affiliations": [
"Chaire de Simulation \u00e0 l\u2019Echelle Atomique (CSEA), Ecole Polytechnique F\u00e9d\u00e9rale de Lausanne (EPFL), CH-1015 Lausanne, Switzerland"
],
"familyname": "Pasquarello",
"givennames": "Alfredo"
},
{
"affiliations": [
"Theory and Simulation of Materials (THEOS) and National Centre for Computational Design and Discovery of Novel Materials (MARVEL), Ecole Polytechnique F\u00e9d\u00e9rale de Lausanne (EPFL), CH-1015 Lausanne, Switzerland"
],
"familyname": "Marzari",
"givennames": "Nicola"
}
],
"edited_by": 100
},
"updated": "2021-07-20T08:54:53.216925+00:00"
}