globalchange  > 气候变化与战略
DOI: 10.1073/pnas.1722229115
论文题名:
Molecular excitonic seesaws
作者: Wilhelm P.; Schedlbauer J.; Hinderer F.; Hennen D.; Höger S.; Vogelsang J.; Lupton J.M.
刊名: Proceedings of the National Academy of Sciences of the United States of America
ISSN: 0027-8424
出版年: 2018
卷: 115, 期:16
起始页码: E3626
结束页码: E3634
语种: 英语
英文关键词: Bodipys ; Excited-state molecular dynamics ; Excitonics ; Light harvesting ; Single-molecule spectroscopy
Scopus关键词: oligomer ; Article ; chemical structure ; conjugation ; controlled study ; energy transfer ; field emission ; fluorescence correlation spectroscopy ; fluorescence polarization ; light absorption ; light harvesting system ; light scattering ; molecular dynamics ; photon correlation spectroscopy ; priority journal ; synthesis
英文摘要: The breaking of molecular symmetry through photoexcitation is a ubiquitous but rather elusive process, which, for example, controls the microscopic efficiency of light harvesting in molecular aggregates. A molecular excitation within a π-conjugated segment will self-localize due to strong coupling to molecular vibrations, locally changing bond alternation in a process which is fundamentally nondeterministic. Probing such symmetry breaking usually relies on polarization-resolved fluorescence, which is most powerful on the level of single molecules. Here, we explore symmetry breaking by designing a large, asymmetric acceptor-donor-acceptor (A1-DA2) complex 10 nm in length, where excitation energy can flow from the donor, a π-conjugated oligomer, to either one of the two boron-dipyrromethene (bodipy) dye acceptors of different color. Fluorescence correlation spectroscopy (FCS) reveals a nondeterministic switching between the energy-transfer pathways from the oligomer to the two acceptor groups on the submillisecond timescale. We conclude that excitation energy transfer, and light harvesting in general, are fundamentally nondeterministic processes, which can be strongly perturbed by external stimuli. A simple demonstration of the relation between exciton localization within the extended π-system and energy transfer to the endcap is given by considering the selectivity of endcap emission through the polarization of the excitation light in triads with bent oligomer backbones. Bending leads to increased localization so that the molecule acquires bichromophoric characteristics in terms of its fluorescence photon statistics. © 2018 National Academy of Sciences. All rights reserved.
Citation statistics:
资源类型: 期刊论文
标识符: http://119.78.100.158/handle/2HF3EXSE/163752
Appears in Collections:气候变化与战略

Files in This Item:

There are no files associated with this item.


作者单位: Wilhelm, P., Institut für Experimentelle und Angewandte Physik, Universität Regensburg, Regensburg, 93053, Germany; Schedlbauer, J., Institut für Experimentelle und Angewandte Physik, Universität Regensburg, Regensburg, 93053, Germany; Hinderer, F., Kekulé-Institut für Organische Chemie und Biochemie, Universität Bonn, Bonn, 53121, Germany; Hennen, D., Kekulé-Institut für Organische Chemie und Biochemie, Universität Bonn, Bonn, 53121, Germany; Höger, S., Kekulé-Institut für Organische Chemie und Biochemie, Universität Bonn, Bonn, 53121, Germany; Vogelsang, J., Institut für Experimentelle und Angewandte Physik, Universität Regensburg, Regensburg, 93053, Germany; Lupton, J.M., Institut für Experimentelle und Angewandte Physik, Universität Regensburg, Regensburg, 93053, Germany

Recommended Citation:
Wilhelm P.,Schedlbauer J.,Hinderer F.,et al. Molecular excitonic seesaws[J]. Proceedings of the National Academy of Sciences of the United States of America,2018-01-01,115(16)
Service
Recommend this item
Sava as my favorate item
Show this item's statistics
Export Endnote File
Google Scholar
Similar articles in Google Scholar
[Wilhelm P.]'s Articles
[Schedlbauer J.]'s Articles
[Hinderer F.]'s Articles
百度学术
Similar articles in Baidu Scholar
[Wilhelm P.]'s Articles
[Schedlbauer J.]'s Articles
[Hinderer F.]'s Articles
CSDL cross search
Similar articles in CSDL Cross Search
[Wilhelm P.]‘s Articles
[Schedlbauer J.]‘s Articles
[Hinderer F.]‘s Articles
Related Copyright Policies
Null
收藏/分享
所有评论 (0)
暂无评论
 

Items in IR are protected by copyright, with all rights reserved, unless otherwise indicated.