Interplay between Intra- and Intermolecular Charge Transfer in the Optical Excitations of J-Aggregates.
Journal
The journal of physical chemistry. C, Nanomaterials and interfaces
ISSN: 1932-7447
Titre abrégé: J Phys Chem C Nanomater Interfaces
Pays: United States
ID NLM: 101299949
Informations de publication
Date de publication:
21 Mar 2019
21 Mar 2019
Historique:
received:
05
12
2018
revised:
13
02
2019
entrez:
6
4
2019
pubmed:
6
4
2019
medline:
6
4
2019
Statut:
ppublish
Résumé
In a first-principles study based on density functional theory and many-body perturbation theory, we address the interplay between intra- and intermolecular interactions in a J-aggregate formed by push-pull organic dyes by investigating its electronic and optical properties. We find that the most intense excitation dominating the spectral onset of the aggregate, i.e., the J-band, exhibits a combination of intramolecular charge transfer, coming from the push-pull character of the constituting dyes, and intermolecular charge transfer, due to the dense molecular packing. We also show the presence of a pure intermolecular charge-transfer excitation within the J-band, which is expected to play a relevant role in the emission properties of the J-aggregate. Our results shed light on the microscopic character of optical excitations of J-aggregates and offer new perspectives to further understand the nature of collective excitations in organic semiconductors.
Identifiants
pubmed: 30949274
doi: 10.1021/acs.jpcc.8b11709
pmc: PMC6443228
doi:
Types de publication
Journal Article
Langues
eng
Pagination
6831-6838Déclaration de conflit d'intérêts
The authors declare no competing financial interest.
Références
Phys Rev Lett. 1989 Mar 6;62(10):1169-1172
pubmed: 10039594
Phys Rev Lett. 1996 Mar 11;76(11):1900-1903
pubmed: 10060549
Phys Rev Lett. 1996 Oct 28;77(18):3865-3868
pubmed: 10062328
Phys Rev Lett. 2002 May 20;88(20):206403
pubmed: 12005587
Radiat Res. 1963 Sep;20:55-70
pubmed: 14061481
J Am Chem Soc. 2004 Mar 31;126(12):4007-16
pubmed: 15038755
Phys Rev Lett. 2004 Apr 9;92(14):147402
pubmed: 15089572
Chem Rev. 2005 Nov;105(11):4009-37
pubmed: 16277369
Phys Rev Lett. 2007 Jan 19;98(3):037402
pubmed: 17358724
Nano Lett. 2007 May;7(5):1297-303
pubmed: 17455984
J Chem Phys. 2008 Jan 28;128(4):044505
pubmed: 18247967
Nano Lett. 2008 Oct;8(10):3481-7
pubmed: 18729410
Phys Rev Lett. 2008 Sep 26;101(13):133002
pubmed: 18851443
Nat Chem. 2010 Aug;2(8):648-52
pubmed: 20651727
J Am Chem Soc. 2011 Aug 10;133(31):11830-3
pubmed: 21755937
J Phys Condens Matter. 2009 Sep 30;21(39):395502
pubmed: 21832390
Phys Chem Chem Phys. 2011 Dec 28;13(48):21608-14
pubmed: 22071571
J Am Chem Soc. 2011 Dec 14;133(49):19944-52
pubmed: 22084927
Nanoscale Res Lett. 2013 Mar 22;8(1):134
pubmed: 23522305
J Chem Phys. 2013 Mar 21;138(11):114103
pubmed: 23534623
Acc Chem Res. 2013 Jun 18;46(6):1330-8
pubmed: 23656886
Phys Rev Lett. 2013 May 31;110(22):226402
pubmed: 23767738
J Am Chem Soc. 2014 Apr 16;136(15):5755-64
pubmed: 24697685
ACS Nano. 2014 Jul 22;8(7):7377-83
pubmed: 24957197
J Chem Phys. 2014 Aug 21;141(7):074705
pubmed: 25149804
J Phys Condens Matter. 2015 Mar 25;27(11):113204
pubmed: 25738755
J Phys Chem Lett. 2011 Jun 2;2(11):1315-9
pubmed: 26295427
J Phys Chem Lett. 2011 Apr 21;2(8):863-73
pubmed: 26295620
J Chem Theory Comput. 2015 Jan 13;11(1):147-56
pubmed: 26574213
J Chem Theory Comput. 2013 Jan 8;9(1):324-9
pubmed: 26589035
J Chem Phys. 2016 Dec 21;145(23):234701
pubmed: 27984863
J Phys Condens Matter. 2017 Oct 4;29(39):394005
pubmed: 28664870
Methods Appl Fluoresc. 2017 Dec 21;6(1):012001
pubmed: 28914610
Phys Rev Lett. 2017 Dec 29;119(26):267401
pubmed: 29328724
Nat Commun. 2018 Mar 5;9(1):954
pubmed: 29507287
ACS Omega. 2018 Sep 30;3(9):10481-10486
pubmed: 30288457
Phys Chem Chem Phys. 2018 Dec 5;20(47):29724-29736
pubmed: 30462114
Phys Rev B Condens Matter. 1986 Oct 15;34(8):5390-5413
pubmed: 9940372