Switching intramolecular singlet fission in tetracene dimers via subtle changes in bridges

被引：0

作者：

Wang, Ting ^{[1
]}

Zhang, San ^{[2
]}

Ding, Yun-Tao ^{[1
]}

Zhang, Bo-Yang ^{[1
]}

Yu, Buyang ^{[2
]}

Xu, Rong ^{[2
]}

Liu, Zhi-Xing ^{[2
]}

Sun, Chun-Lin ^{[1
]}

Zhang, Chunfeng ^{[2
]}

Wang, Qiang ^{[1
]}

Zhang, Hao-Li ^{[1
]}

机构：

[1] Lanzhou Univ, Coll Chem & Chem Engn, State Key Lab Appl Organ Chem SKLAOC, Key Lab Special Funct Mat & Struct Design MOE, Lanzhou 730000, Peoples R China

[2] Nanjing Univ, Collaborat Innovat Ctr Adv Microstruct, Sch Phys, Natl Lab Solid State Microstruct, Nanjing 210093, Peoples R China

来源：

JOURNAL OF MATERIALS CHEMISTRY C | 2025年 / 13卷 / 19期

基金：

中国国家自然科学基金;

关键词：

EXCITON FISSION; THIN-FILM; PENTACENE; DELOCALIZATION; DYNAMICS; SILICON; STATES;

D O I：

10.1039/d4tc05184j

中图分类号：

T [工业技术];

学科分类号：

08 ;

摘要：

Singlet fission has attracted great attention in recent years owing to the potential of enhancing photoenergy conversion efficiency through exciton multiplication. Herein, we designed tetracene dimers bridged by two regio-isomers, namely 2T-DPP and 2T-DOP, in which 2T-DPP has a C2 symmetry, while 2T-DOP is asymmetric. Femtosecond transient absorption spectroscopy reveals that 2T-DPP undergoes singlet fission with a triplet yield of 125% in dichloromethane. In contrast, 2T-DOP undergoes no singlet fission. Theoretical investigation indicates that 2T-DPP features a delocalized exciton, whereas localized exciton resides in the dimer 2T-DOP due to low symmetry. This work demonstrates that subtle changes in the bridge structure could significantly alter the efficiency of intramolecular singlet fission and highlights the importance of molecular symmetry in modulating the exciton delocalization and thus in switching intramolecular singlet fission.

引用

页码：9576 / 9583

页数：8

共 57 条

[41] A Silicon-Singlet Fission Tandem Solar Cell Exceeding 100% External Quantum Efficiency with High Spectral Stability [J].

Pazos-Outon, Luis M. ;

Lee, Ju Min ;

Futscher, Moritz H. ;

Kirch, Anton ;

Tabachnyk, Maxim ;

Friend, Richard H. ;

Ehrler, Bruno .

ACS ENERGY LETTERS, 2017, 2 (02) :476-480

[42] Exciton Delocalization Drives Rapid Singlet Fission in Nanoparticles of Acene Derivatives [J].

Pensack, Ryan D. ;

Tilley, Andrew J. ;

Parkin, Sean R. ;

Lee, Tia S. ;

Payne, Marcia M. ;

Gao, Dong ;

Jahnke, Ashlee A. ;

Oblinsky, Daniel G. ;

Li, Peng-Fei ;

Anthony, John E. ;

Seferos, Dwight S. ;

Scholes, Gregory D. .

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2015, 137 (21) :6790-6803

[43] Towards more sustainable synthesis of diketopyrrolopyrroles [J].

Pop, Flavia ;

Humphreys, Joshua ;

Schwarz, Jesper ;

Brown, Liam ;

van den Berg, Ashmiani ;

Amabilino, David B. .

NEW JOURNAL OF CHEMISTRY, 2019, 43 (15) :5783-5790

[44] Ultra-fast intramolecular singlet fission to persistent multiexcitons by molecular design [J].

Pun, Andrew B. ;

Asadpoordarvish, Amir ;

Kumarasamy, Elango ;

Tayebjee, Murad J. Y. ;

Niesner, Daniel ;

McCamey, Dane R. ;

Sanders, Samuel N. ;

Campos, Luis M. ;

Sfeir, Matthew Y. .

NATURE CHEMISTRY, 2019, 11 (09) :821-828

[45] Controlling Singlet Fission with Coordination Chemistry-Induced Assembly of Dipyridyl Pyrrole Bipentacenes [J].

Ribson, Ryan D. ;

Choi, Gyeongshin ;

Hadt, Ryan G. ;

Agapie, Theodor .

ACS CENTRAL SCIENCE, 2020, 6 (11) :2088-2096

[46] Long-Lived Triplet Excited States of Bent-Shaped Pentacene Dimers by Intramolecular Singlet Fission [J].

Sakuma, Takao ;

Sakai, Hayato ;

Araki, Yasuyuki ;

Mori, Tadashi ;

Wada, Takehiko ;

Tkachenko, Nikolai V. ;

Hasobe, Taku .

JOURNAL OF PHYSICAL CHEMISTRY A, 2016, 120 (11) :1867-1875

[47] Exciton Correlations in Intramolecular Singlet Fission [J].

Sanders, Samuel N. ;

Kumarasamy, Elango ;

Pun, Andrew B. ;

Appavoo, Kannatassen ;

Steigerwald, Michael L. ;

Campos, Luis M. ;

Sfeir, Matthew Y. .

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2016, 138 (23) :7289-7297

[48] Intramolecular Singlet Fission in Oligoacene Heterodimers [J].

Sanders, Samuel N. ;

Kumarasamy, Elango ;

Pun, Andrew B. ;

Steigerwald, Michael L. ;

Sfeir, Matthew Y. ;

Campos, Luis M. .

ANGEWANDTE CHEMIE-INTERNATIONAL EDITION, 2016, 55 (10) :3373-3377

[49] Quantitative Intramolecular Singlet Fission in Bipentacenes [J].

Sanders, Samuel N. ;

Kumarasamy, Elango ;

Pun, Andrew B. ;

Trinh, M. Tuan ;

Choi, Bonnie ;

Xia, Jianlong ;

Taffet, Elliot J. ;

Low, Jonathan Z. ;

Miller, John R. ;

Roy, Xavier ;

Zhu, X. -Y. ;

Steigerwald, Michael L. ;

Sfeir, Matthew Y. ;

Campos, Luis M. .

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2015, 137 (28) :8965-8972

[50]

Tayebjee MJY, 2017, NAT PHYS, V13, P182, DOI [10.1038/NPHYS3909, 10.1038/nphys3909]

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