Supertransport of excitons in atomically thin organic semiconductors at the 2D quantum limit.

Sharma, A; Zhang, L; Tollerud, JO; Dong, M; Zhu, Y; Halbich, R; Vogl, T; Liang, K; Nguyen, HT; Wang, F; Sanwlani, S; Earl, SK; Macdonald, D; Lam, PK; Davis, JA; Lu, Y

Supertransport of excitons in atomically thin organic semiconductors at the 2D quantum limit.

Sharma, A Zhang, L Tollerud, JO Dong, M Zhu, Y Halbich, R Vogl, T Liang, K Nguyen, HT Wang, F

Sanwlani, S Earl, SK Macdonald, D Lam, PK Davis, JA Lu, Y

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Publisher:: Springer Science and Business Media LLC
Publication Type:: Journal Article
Citation:: Light, science & applications, 2020, 9, (1)
Issue Date:: 2020-01

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Field	Value	Language
dc.contributor.author	Sharma, A
dc.contributor.author	Zhang, L
dc.contributor.author	Tollerud, JO
dc.contributor.author	Dong, M
dc.contributor.author	Zhu, Y
dc.contributor.author	Halbich, R
dc.contributor.author	Vogl, T
dc.contributor.author	Liang, K
dc.contributor.author	Nguyen, HT
dc.contributor.author	Wang, F https://orcid.org/0000-0001-7403-3305
dc.contributor.author	Sanwlani, S
dc.contributor.author	Earl, SK
dc.contributor.author	Macdonald, D
dc.contributor.author	Lam, PK
dc.contributor.author	Davis, JA
dc.contributor.author	Lu, Y
dc.date.accessioned	2021-03-09T03:23:21Z
dc.date.available	2020-06-09
dc.date.available	2021-03-09T03:23:21Z
dc.date.issued	2020-01
dc.identifier.citation	Light, science & applications, 2020, 9, (1)
dc.identifier.issn	2095-5545
dc.identifier.issn	2047-7538
dc.identifier.uri	http://hdl.handle.net/10453/146958
dc.description.abstract	Long-range and fast transport of coherent excitons is important for the development of high-speed excitonic circuits and quantum computing applications. However, most of these coherent excitons have only been observed in some low-dimensional semiconductors when coupled with cavities, as there are large inhomogeneous broadening and dephasing effects on the transport of excitons in their native states in materials. Here, by confining coherent excitons at the 2D quantum limit, we first observed molecular aggregation-enabled 'supertransport' of excitons in atomically thin two-dimensional (2D) organic semiconductors between coherent states, with a measured high effective exciton diffusion coefficient of ~346.9 cm<sup>2</sup>/s at room temperature. This value is one to several orders of magnitude higher than the values reported for other organic molecular aggregates and low-dimensional inorganic materials. Without coupling to any optical cavities, the monolayer pentacene sample, a very clean 2D quantum system (~1.2 nm thick) with high crystallinity (J-type aggregation) and minimal interfacial states, showed superradiant emission from Frenkel excitons, which was experimentally confirmed by the temperature-dependent photoluminescence (PL) emission, highly enhanced radiative decay rate, significantly narrowed PL peak width and strongly directional in-plane emission. The coherence in monolayer pentacene samples was observed to be delocalised over ~135 molecules, which is significantly larger than the values (a few molecules) observed for other organic thin films. In addition, the supertransport of excitons in monolayer pentacene samples showed highly anisotropic behaviour. Our results pave the way for the development of future high-speed excitonic circuits, fast OLEDs, and other optoelectronic devices.
dc.format	Electronic-eCollection
dc.language	eng
dc.publisher	Springer Science and Business Media LLC
dc.relation	http://purl.org/au-research/grants/arc/CE170100012
dc.relation.ispartof	Light, science & applications
dc.relation.isbasedon	10.1038/s41377-020-00347-y
dc.rights	This is a post-peer-review, pre-copyedit version of an article published in Light, science & applications. The final authenticated version is available online at: https://dx.doi.org/10.1038/s41377-020-00347-y.	en_US
dc.rights	info:eu-repo/semantics/openAccess
dc.subject	0205 Optical Physics
dc.title	Supertransport of excitons in atomically thin organic semiconductors at the 2D quantum limit.
dc.type	Journal Article
utslib.citation.volume	9
utslib.location.activity	England
utslib.for	0205 Optical Physics
pubs.organisational-group	/University of Technology Sydney/Faculty of Engineering and Information Technology
pubs.organisational-group	/University of Technology Sydney/Strength - GBDTC - Global Big Data Technologies
pubs.organisational-group	/University of Technology Sydney/Strength - IBMD - Initiative for Biomedical Devices
pubs.organisational-group	/University of Technology Sydney/Faculty of Engineering and Information Technology/School of Electrical and Data Engineering
pubs.organisational-group	/University of Technology Sydney
utslib.copyright.status	open_access	*
pubs.consider-herdc	false
dc.date.updated	2021-03-09T03:23:16Z
pubs.issue	1
pubs.publication-status	Published
pubs.volume	9
utslib.citation.issue	1

Abstract:

Long-range and fast transport of coherent excitons is important for the development of high-speed excitonic circuits and quantum computing applications. However, most of these coherent excitons have only been observed in some low-dimensional semiconductors when coupled with cavities, as there are large inhomogeneous broadening and dephasing effects on the transport of excitons in their native states in materials. Here, by confining coherent excitons at the 2D quantum limit, we first observed molecular aggregation-enabled 'supertransport' of excitons in atomically thin two-dimensional (2D) organic semiconductors between coherent states, with a measured high effective exciton diffusion coefficient of ~346.9 cm²/s at room temperature. This value is one to several orders of magnitude higher than the values reported for other organic molecular aggregates and low-dimensional inorganic materials. Without coupling to any optical cavities, the monolayer pentacene sample, a very clean 2D quantum system (~1.2 nm thick) with high crystallinity (J-type aggregation) and minimal interfacial states, showed superradiant emission from Frenkel excitons, which was experimentally confirmed by the temperature-dependent photoluminescence (PL) emission, highly enhanced radiative decay rate, significantly narrowed PL peak width and strongly directional in-plane emission. The coherence in monolayer pentacene samples was observed to be delocalised over ~135 molecules, which is significantly larger than the values (a few molecules) observed for other organic thin films. In addition, the supertransport of excitons in monolayer pentacene samples showed highly anisotropic behaviour. Our results pave the way for the development of future high-speed excitonic circuits, fast OLEDs, and other optoelectronic devices.

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http://hdl.handle.net/10453/146958