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Colloidal Two-Dimensional Metal Chalcogenides: Realization and Application of the Structural Anisotropy

Ziyi Hu, Ryan O'Neill, Rostyslav Lesyuk, Christian Klinke Orcid Logo

Accounts of Chemical Research, Volume: 54, Issue: 20, Pages: 3792 - 3803

Swansea University Authors: Ziyi Hu, Ryan O'Neill, Christian Klinke Orcid Logo

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DOI (Published version): 10.1021/acs.accounts.1c00209

Abstract

Due to the spatial confinement, two-dimensional metal chalcogenides display an extraordinary optical response and carrier transport ability. Solution-based synthesis techniques such as colloidal hot injection and ion exchange provide a cost-effective way to fabricate such low-dimensional semiconduct...

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Published in: Accounts of Chemical Research
ISSN: 0001-4842 1520-4898
Published: American Chemical Society (ACS) 2021
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URI: https://cronfa.swan.ac.uk/Record/cronfa58384
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Solution-based synthesis techniques such as colloidal hot injection and ion exchange provide a cost-effective way to fabricate such low-dimensional semiconducting nanocrystals. Over the years, developments in colloidal chemistry made it possible to synthesize various kinds of ultrathin colloidal nanoplatelets, including wurtzite- and zinc blende-type CdSe, rock salt PbS, black phosphorus-like SnX (X = S or Se), hexagonal copper sulfides, selenides, and even transition metal dichalcogenides like MoS2. By altering experimental conditions and applying capping ligands with specific functional groups, it is possible to accurately tune the dimensionality, geometry, and consequently the optical properties of these colloidal metal chalcogenide crystals. Here, we review recent progress in the syntheses of two-dimensional colloidal metal chalcogenides (CMCs) and property characterizations based on optical spectroscopy or device-related measurements. The discoveries shine a light on their huge prospect for applications in areas such as photovoltaics, optoelectronics, and spintronics. In specific, the formation mechanisms of two-dimensional CMCs are discussed. The growth of colloidal nanocrystals into a two-dimensional shape is found to require either an intrinsic structural asymmetry or the assist of coexisted ligand molecules, which act as lamellar double-layer templates or &#x201C;facet&#x201D; the crystals via selective adsorption. By performing optical characterizations and especially ultrafast spectroscopic measurements on these two-dimensional CMCs, their unique electronic and excitonic features are revealed. A strong dependence of optical transition energies linked to both interband and inter-subband processes on the crystal geometry can be verified, highlighting a tremendous confinement effect in such nanocrystals. With the self-assembly of two-dimensional nanocrystals or coupling of different phases by growing heterostructures, unconventional optical performances such as charge transfer state generation or efficient F&#xF6;rster resonance energy transfer are discovered. The growth of large-scale individualized PbS and SnS nanosheets can be realized by facile hot injection techniques, which gives the opportunity to investigate the charge carrier behavior within a single nanocrystal. According to the results of the device-based measurements on these individualized crystals, structure asymmetry-induced anisotropic electrical responses and Rashba effects caused by a splitting of spin-resolved bands in the momentum space due to strong spin&#x2013;orbit-coupling are demonstrated. 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spelling 2021-12-06T17:14:22.6222478 v2 58384 2021-10-18 Colloidal Two-Dimensional Metal Chalcogenides: Realization and Application of the Structural Anisotropy 6ce25906e78850bfb7e274dc21d559ea Ziyi Hu Ziyi Hu true false 70b31483c3ce08211ce0ff053234bad0 Ryan O'Neill Ryan O'Neill true false c10c44238eabfb203111f88a965f5372 0000-0001-8558-7389 Christian Klinke Christian Klinke true false 2021-10-18 Due to the spatial confinement, two-dimensional metal chalcogenides display an extraordinary optical response and carrier transport ability. Solution-based synthesis techniques such as colloidal hot injection and ion exchange provide a cost-effective way to fabricate such low-dimensional semiconducting nanocrystals. Over the years, developments in colloidal chemistry made it possible to synthesize various kinds of ultrathin colloidal nanoplatelets, including wurtzite- and zinc blende-type CdSe, rock salt PbS, black phosphorus-like SnX (X = S or Se), hexagonal copper sulfides, selenides, and even transition metal dichalcogenides like MoS2. By altering experimental conditions and applying capping ligands with specific functional groups, it is possible to accurately tune the dimensionality, geometry, and consequently the optical properties of these colloidal metal chalcogenide crystals. Here, we review recent progress in the syntheses of two-dimensional colloidal metal chalcogenides (CMCs) and property characterizations based on optical spectroscopy or device-related measurements. The discoveries shine a light on their huge prospect for applications in areas such as photovoltaics, optoelectronics, and spintronics. In specific, the formation mechanisms of two-dimensional CMCs are discussed. The growth of colloidal nanocrystals into a two-dimensional shape is found to require either an intrinsic structural asymmetry or the assist of coexisted ligand molecules, which act as lamellar double-layer templates or “facet” the crystals via selective adsorption. By performing optical characterizations and especially ultrafast spectroscopic measurements on these two-dimensional CMCs, their unique electronic and excitonic features are revealed. A strong dependence of optical transition energies linked to both interband and inter-subband processes on the crystal geometry can be verified, highlighting a tremendous confinement effect in such nanocrystals. With the self-assembly of two-dimensional nanocrystals or coupling of different phases by growing heterostructures, unconventional optical performances such as charge transfer state generation or efficient Förster resonance energy transfer are discovered. The growth of large-scale individualized PbS and SnS nanosheets can be realized by facile hot injection techniques, which gives the opportunity to investigate the charge carrier behavior within a single nanocrystal. According to the results of the device-based measurements on these individualized crystals, structure asymmetry-induced anisotropic electrical responses and Rashba effects caused by a splitting of spin-resolved bands in the momentum space due to strong spin–orbit-coupling are demonstrated. It is foreseen that such geometry-controlled, large-scale two-dimensional CMCs can be the ideal materials used for designing high-efficiency photonics and electronics. Journal Article Accounts of Chemical Research 54 20 3792 3803 American Chemical Society (ACS) 0001-4842 1520-4898 Colloidal Chemistry, Nanomaterials 19 10 2021 2021-10-19 10.1021/acs.accounts.1c00209 COLLEGE NANME COLLEGE CODE Swansea University Engineering and Physical Sciences Research Council Grant: EP/N509553/1 Identifier: FundRef 10.13039/501100000266 China Scholarship Council Grant: 201808230269 Identifier: FundRef 10.13039/501100004543 2021-12-06T17:14:22.6222478 2021-10-18T10:55:27.7759190 Faculty of Science and Engineering School of Engineering and Applied Sciences - Chemistry Ziyi Hu 1 Ryan O'Neill 2 Rostyslav Lesyuk 3 Christian Klinke 0000-0001-8558-7389 4 58384__21278__b89e3d0f366f49d8953a74537c913206.pdf Hu-Klinke-2D-Nanosheets-InvitedReview.pdf 2021-10-22T11:48:27.2612005 Output 1014365 application/pdf Accepted Manuscript true 2022-10-08T00:00:00.0000000 true eng
title Colloidal Two-Dimensional Metal Chalcogenides: Realization and Application of the Structural Anisotropy
spellingShingle Colloidal Two-Dimensional Metal Chalcogenides: Realization and Application of the Structural Anisotropy
Ziyi Hu
Ryan O'Neill
Christian Klinke
title_short Colloidal Two-Dimensional Metal Chalcogenides: Realization and Application of the Structural Anisotropy
title_full Colloidal Two-Dimensional Metal Chalcogenides: Realization and Application of the Structural Anisotropy
title_fullStr Colloidal Two-Dimensional Metal Chalcogenides: Realization and Application of the Structural Anisotropy
title_full_unstemmed Colloidal Two-Dimensional Metal Chalcogenides: Realization and Application of the Structural Anisotropy
title_sort Colloidal Two-Dimensional Metal Chalcogenides: Realization and Application of the Structural Anisotropy
author_id_str_mv 6ce25906e78850bfb7e274dc21d559ea
70b31483c3ce08211ce0ff053234bad0
c10c44238eabfb203111f88a965f5372
author_id_fullname_str_mv 6ce25906e78850bfb7e274dc21d559ea_***_Ziyi Hu
70b31483c3ce08211ce0ff053234bad0_***_Ryan O'Neill
c10c44238eabfb203111f88a965f5372_***_Christian Klinke
author Ziyi Hu
Ryan O'Neill
Christian Klinke
author2 Ziyi Hu
Ryan O'Neill
Rostyslav Lesyuk
Christian Klinke
format Journal article
container_title Accounts of Chemical Research
container_volume 54
container_issue 20
container_start_page 3792
publishDate 2021
institution Swansea University
issn 0001-4842
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doi_str_mv 10.1021/acs.accounts.1c00209
publisher American Chemical Society (ACS)
college_str Faculty of Science and Engineering
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hierarchy_top_id facultyofscienceandengineering
hierarchy_top_title Faculty of Science and Engineering
hierarchy_parent_id facultyofscienceandengineering
hierarchy_parent_title Faculty of Science and Engineering
department_str School of Engineering and Applied Sciences - Chemistry{{{_:::_}}}Faculty of Science and Engineering{{{_:::_}}}School of Engineering and Applied Sciences - Chemistry
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description Due to the spatial confinement, two-dimensional metal chalcogenides display an extraordinary optical response and carrier transport ability. Solution-based synthesis techniques such as colloidal hot injection and ion exchange provide a cost-effective way to fabricate such low-dimensional semiconducting nanocrystals. Over the years, developments in colloidal chemistry made it possible to synthesize various kinds of ultrathin colloidal nanoplatelets, including wurtzite- and zinc blende-type CdSe, rock salt PbS, black phosphorus-like SnX (X = S or Se), hexagonal copper sulfides, selenides, and even transition metal dichalcogenides like MoS2. By altering experimental conditions and applying capping ligands with specific functional groups, it is possible to accurately tune the dimensionality, geometry, and consequently the optical properties of these colloidal metal chalcogenide crystals. Here, we review recent progress in the syntheses of two-dimensional colloidal metal chalcogenides (CMCs) and property characterizations based on optical spectroscopy or device-related measurements. The discoveries shine a light on their huge prospect for applications in areas such as photovoltaics, optoelectronics, and spintronics. In specific, the formation mechanisms of two-dimensional CMCs are discussed. The growth of colloidal nanocrystals into a two-dimensional shape is found to require either an intrinsic structural asymmetry or the assist of coexisted ligand molecules, which act as lamellar double-layer templates or “facet” the crystals via selective adsorption. By performing optical characterizations and especially ultrafast spectroscopic measurements on these two-dimensional CMCs, their unique electronic and excitonic features are revealed. A strong dependence of optical transition energies linked to both interband and inter-subband processes on the crystal geometry can be verified, highlighting a tremendous confinement effect in such nanocrystals. With the self-assembly of two-dimensional nanocrystals or coupling of different phases by growing heterostructures, unconventional optical performances such as charge transfer state generation or efficient Förster resonance energy transfer are discovered. The growth of large-scale individualized PbS and SnS nanosheets can be realized by facile hot injection techniques, which gives the opportunity to investigate the charge carrier behavior within a single nanocrystal. According to the results of the device-based measurements on these individualized crystals, structure asymmetry-induced anisotropic electrical responses and Rashba effects caused by a splitting of spin-resolved bands in the momentum space due to strong spin–orbit-coupling are demonstrated. It is foreseen that such geometry-controlled, large-scale two-dimensional CMCs can be the ideal materials used for designing high-efficiency photonics and electronics.
published_date 2021-10-19T04:14:52Z
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