Defect-Free, Few-Atomic-Layer Thin ZnO Nanosheets with Superior Excitonic Properties for Optoelectronic Devices.

Singh, M; Zakria, M; Pannu, AS; Sonar, P; Smith, C; Mahasivam, S; Ramanathan, R; Tran, K; Tawfik, S; Murdoch, BJ; Mayes, ELH; Spencer, MJS; Phillips, MR; Bansal, V; Ton-That, C

Defect-Free, Few-Atomic-Layer Thin ZnO Nanosheets with Superior Excitonic Properties for Optoelectronic Devices.

Singh, M Zakria, M Pannu, AS Sonar, P Smith, C Mahasivam, S Ramanathan, R Tran, K Tawfik, S Murdoch, BJ Mayes, ELH Spencer, MJS Phillips, MR Bansal, V Ton-That, C

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Publisher:: AMER CHEMICAL SOC
Publication Type:: Journal Article
Citation:: ACS Nano, 2024, 18, (26), pp. 16947-16957
Issue Date:: 2024-07-02

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Field	Value	Language
dc.contributor.author	Singh, M
dc.contributor.author	Zakria, M
dc.contributor.author	Pannu, AS
dc.contributor.author	Sonar, P
dc.contributor.author	Smith, C
dc.contributor.author	Mahasivam, S
dc.contributor.author	Ramanathan, R
dc.contributor.author	Tran, K
dc.contributor.author	Tawfik, S
dc.contributor.author	Murdoch, BJ
dc.contributor.author	Mayes, ELH
dc.contributor.author	Spencer, MJS
dc.contributor.author	Phillips, MR
dc.contributor.author	Bansal, V
dc.contributor.author	Ton-That, C https://orcid.org/0000-0003-3276-1739
dc.date.accessioned	2024-07-26T08:33:21Z
dc.date.available	2024-07-26T08:33:21Z
dc.date.issued	2024-07-02
dc.identifier.citation	ACS Nano, 2024, 18, (26), pp. 16947-16957
dc.identifier.issn	1936-0851
dc.identifier.issn	1936-086X
dc.identifier.uri	http://hdl.handle.net/10453/179853
dc.description.abstract	Two-dimensional (2D) wide bandgap materials are gaining significant interest for next-generation optoelectronic devices. However, fabricating electronic-grade 2D nanosheets from non-van der Waals (n-vdW) oxide semiconductors poses a great challenge due to their stronger interlayer coupling compared with vdW crystals. This strong coupling typically introduces defects during exfoliation, impairing the optoelectronic properties. Herein, we report the liquid-phase exfoliation of few-atomic-layer thin, defect-free, free-standing ZnO nanosheets. These micron-sized, ultrathin ZnO structures exhibit three different orientations aligned along both the polar c-plane as well as the nonpolar a- and m-planes. The superior crystalline quality of the ZnO nanosheets is validated through comprehensive characterization techniques. This result is supported by density functional theory (DFT) calculations, which reveals that the formation of oxygen vacancies is energetically less favorable in 2D ZnO and that the c-plane loses its polarity upon exfoliation. Unlike bulk ZnO, which is typically dominated by defect-induced emission, the exfoliated nanosheets exhibit a strong, ambient-stable excitonic UV emission. We further demonstrate the utility of solution processing of ZnO nanosheets by their hybrid integration with organic components to produce stable light emitting diodes (LEDs) for display applications.
dc.format	Print-Electronic
dc.language	eng
dc.publisher	AMER CHEMICAL SOC
dc.relation	http://purl.org/au-research/grants/arc/DP210101146
dc.relation.ispartof	ACS Nano
dc.relation.isbasedon	10.1021/acsnano.4c03098
dc.rights	info:eu-repo/semantics/restrictedAccess
dc.subject.classification	Nanoscience & Nanotechnology
dc.title	Defect-Free, Few-Atomic-Layer Thin ZnO Nanosheets with Superior Excitonic Properties for Optoelectronic Devices.
dc.type	Journal Article
utslib.citation.volume	18
utslib.location.activity	United States
pubs.organisational-group	University of Technology Sydney
pubs.organisational-group	University of Technology Sydney/Faculty of Science
pubs.organisational-group	University of Technology Sydney/Faculty of Science/School of Mathematical and Physical Sciences
utslib.copyright.status	recently_added	*
dc.date.updated	2024-07-26T08:33:20Z
pubs.issue	26
pubs.publication-status	Published
pubs.volume	18
utslib.citation.issue	26

Abstract:

Two-dimensional (2D) wide bandgap materials are gaining significant interest for next-generation optoelectronic devices. However, fabricating electronic-grade 2D nanosheets from non-van der Waals (n-vdW) oxide semiconductors poses a great challenge due to their stronger interlayer coupling compared with vdW crystals. This strong coupling typically introduces defects during exfoliation, impairing the optoelectronic properties. Herein, we report the liquid-phase exfoliation of few-atomic-layer thin, defect-free, free-standing ZnO nanosheets. These micron-sized, ultrathin ZnO structures exhibit three different orientations aligned along both the polar c-plane as well as the nonpolar a- and m-planes. The superior crystalline quality of the ZnO nanosheets is validated through comprehensive characterization techniques. This result is supported by density functional theory (DFT) calculations, which reveals that the formation of oxygen vacancies is energetically less favorable in 2D ZnO and that the c-plane loses its polarity upon exfoliation. Unlike bulk ZnO, which is typically dominated by defect-induced emission, the exfoliated nanosheets exhibit a strong, ambient-stable excitonic UV emission. We further demonstrate the utility of solution processing of ZnO nanosheets by their hybrid integration with organic components to produce stable light emitting diodes (LEDs) for display applications.

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http://hdl.handle.net/10453/179853