Transferable Machine-Learning Model of the Electron Density.
Journal
ACS central science
ISSN: 2374-7943
Titre abrégé: ACS Cent Sci
Pays: United States
ID NLM: 101660035
Informations de publication
Date de publication:
23 Jan 2019
23 Jan 2019
Historique:
received:
10
08
2018
entrez:
30
1
2019
pubmed:
30
1
2019
medline:
30
1
2019
Statut:
ppublish
Résumé
The electronic charge density plays a central role in determining the behavior of matter at the atomic scale, but its computational evaluation requires demanding electronic-structure calculations. We introduce an atom-centered, symmetry-adapted framework to machine-learn the valence charge density based on a small number of reference calculations. The model is highly transferable, meaning it can be trained on electronic-structure data of small molecules and used to predict the charge density of larger compounds with low, linear-scaling cost. Applications are shown for various hydrocarbon molecules of increasing complexity and flexibility, and demonstrate the accuracy of the model when predicting the density on octane and octatetraene after training exclusively on butane and butadiene. This transferable, data-driven model can be used to interpret experiments, accelerate electronic structure calculations, and compute electrostatic interactions in molecules and condensed-phase systems.
Identifiants
pubmed: 30693325
doi: 10.1021/acscentsci.8b00551
pmc: PMC6346381
doi:
Types de publication
Journal Article
Langues
eng
Pagination
57-64Déclaration de conflit d'intérêts
The authors declare no competing financial interest.
Références
Acta Crystallogr A. 2011 Mar;67(Pt 2):141-53
pubmed: 21325717
J Chem Phys. 2018 Jun 28;148(24):241401
pubmed: 29960312
Acta Crystallogr A. 2004 May;60(Pt 3):204-8
pubmed: 15103162
J Phys Chem A. 2007 Jul 5;111(26):5678-84
pubmed: 17567110
ACS Cent Sci. 2018 Aug 22;4(8):938-941
pubmed: 30159387
J Chem Theory Comput. 2015 Jul 14;11(7):3225-33
pubmed: 26575759
J Chem Theory Comput. 2018 Sep 11;14(9):4772-4779
pubmed: 30040892
J Am Chem Soc. 2010 May 12;132(18):6498-506
pubmed: 20394428
Proc Natl Acad Sci U S A. 2019 Feb 26;116(9):3401-3406
pubmed: 30733292
J Chem Theory Comput. 2016 Mar 8;12(3):1052-67
pubmed: 26799516
Acta Crystallogr D Biol Crystallogr. 1998 Nov 1;54(Pt 6 Pt 2):1306-18
pubmed: 10089507
Phys Rev Lett. 2018 Apr 6;120(14):143001
pubmed: 29694129
Nat Mater. 2011 Mar;10(3):209-15
pubmed: 21240288
Phys Rev Lett. 2012 Feb 3;108(5):058301
pubmed: 22400967
Chem Sci. 2017 Apr 1;8(4):3192-3203
pubmed: 28507695
Sci Adv. 2017 Dec 13;3(12):e1701816
pubmed: 29242828
J Chem Phys. 2018 Jun 28;148(24):241730
pubmed: 29960368
J Phys Chem A. 2007 Aug 2;111(30):6904-14
pubmed: 17511437
Angew Chem Int Ed Engl. 2005 Oct 28;44(42):6810-1
pubmed: 16187393
Angew Chem Int Ed Engl. 2004 May 10;43(20):2718-21
pubmed: 18629999
Nat Commun. 2017 Oct 11;8(1):872
pubmed: 29021555
Acta Crystallogr A. 2007 Mar;63(Pt 2):108-25
pubmed: 17301471
J Chem Phys. 2017 Mar 28;146(12):120901
pubmed: 28388098
Philos Trans A Math Phys Eng Sci. 2014 Feb 10;372(2011):20120483
pubmed: 24516180
Phys Rev Lett. 2007 Apr 6;98(14):146401
pubmed: 17501293
J Comput Chem. 2016 Jan 5;37(1):83-92
pubmed: 26228927
Phys Rev Lett. 1992 Dec 14;69(24):3547-3550
pubmed: 10046849
Acta Crystallogr B. 2011 Feb;67(Pt 1):63-78
pubmed: 21245542
J Synchrotron Radiat. 2008 May;15(Pt 3):202-3
pubmed: 18421138
Acta Crystallogr D Biol Crystallogr. 2008 May;64(Pt 5):567-88
pubmed: 18453693
J Chem Theory Comput. 2007 Jan;3(1):232-47
pubmed: 26627168
Phys Rev Lett. 2018 Jan 19;120(3):036002
pubmed: 29400528
Acta Crystallogr A. 2012 May;68(Pt 3):337-51
pubmed: 22514066
Chem Soc Rev. 2012 Jul 7;41(13):4671-87
pubmed: 22660008
J Chem Theory Comput. 2014 Sep 9;10(9):3745-3756
pubmed: 25221443
Acta Crystallogr D Biol Crystallogr. 2009 May;65(Pt 5):485-99
pubmed: 19390154
Chem Rev. 2001 Jun;101(6):1583-627
pubmed: 11709993
Proc Natl Acad Sci U S A. 2005 Aug 16;102(33):11635-8
pubmed: 16087868
Acta Crystallogr A. 2002 Sep;58(Pt 5):464-72
pubmed: 12192120
J Chem Phys. 2018 Jun 28;148(24):241727
pubmed: 29960350
Nature. 2018 Jul;559(7715):547-555
pubmed: 30046072
Phys Rev Lett. 2010 Apr 2;104(13):136403
pubmed: 20481899
Acc Chem Res. 2014 Sep 16;47(9):2804-11
pubmed: 25099338
Phys Rev Lett. 1991 Mar 18;66(11):1438-1441
pubmed: 10043209
ACS Cent Sci. 2018 Feb 28;4(2):144-152
pubmed: 29532014
Chem Sci. 2017 Dec 12;9(5):1289-1300
pubmed: 29675175
J Chem Phys. 2008 Jul 14;129(2):024707
pubmed: 18624552
Phys Chem Chem Phys. 2016 May 18;18(20):13754-69
pubmed: 27101873
J Chem Phys. 2007 Sep 21;127(11):114105
pubmed: 17887826