Electron localization in rod-shaped triicosahedral gold nanocluster
Atomically precise gold nanocluster based on linear assembly of repeating icosahedrons (clusters of clusters) is a unique type of linear nanostructure, which exhibits strong near-infrared absorption as their free electrons are confined in a one-dimensional quantum box. Little is known about the carr...
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| Veröffentlicht in: | Proceedings of the National Academy of Sciences - PNAS 2017-06, Vol.114 (24), p.E4697-E4705 |
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| creator | Zhou, Meng Jin, Renxi Sfeir, Matthew Y. Chen, Yuxiang Song, Yongbo Jin, Rongchao |
| description | Atomically precise gold nanocluster based on linear assembly of repeating icosahedrons (clusters of clusters) is a unique type of linear nanostructure, which exhibits strong near-infrared absorption as their free electrons are confined in a one-dimensional quantum box. Little is known about the carrier dynamics in these nanoclusters, which limit their energy-related applications. Here, we reported the observation of exciton localization in triicosahedral Au37 nanoclusters (0.5 nm in diameter and 1.6 nm in length) by measuring femtosecond and nanosecond carrier dynamics. Upon photoexcitation to S₁ electronic state, electrons in Au37 undergo ∼100-ps localization from the two vertexes of three icosahedrons to one vertex, forming a long-lived S₁* state. Such phenomenon is not observed in Au25 (dimer) and Au13 (monomer) consisting of two and one icosahedrons, respectively. We have further observed temperature dependence on the localization process, which proves it is thermally driven. Two excited-state vibration modes with frequencies of 20 and 70 cm−1 observed in the kinetic traces are assigned to the axial and radial breathing modes, respectively. The electron localization is ascribed to the structural distortion of Au37 in the excited state induced by the strong coherent vibrations. The observed electron localization phenomenon provides unique physical insight into one-dimensional gold nanoclusters and other nanostructures, which will advance their applications in solar-energy storage and conversion. |
| doi_str_mv | 10.1073/pnas.1704699114 |
| format | Article |
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Center for Functional Nanomaterials (CFN)</creatorcontrib><description>Atomically precise gold nanocluster based on linear assembly of repeating icosahedrons (clusters of clusters) is a unique type of linear nanostructure, which exhibits strong near-infrared absorption as their free electrons are confined in a one-dimensional quantum box. Little is known about the carrier dynamics in these nanoclusters, which limit their energy-related applications. Here, we reported the observation of exciton localization in triicosahedral Au37 nanoclusters (0.5 nm in diameter and 1.6 nm in length) by measuring femtosecond and nanosecond carrier dynamics. Upon photoexcitation to S₁ electronic state, electrons in Au37 undergo ∼100-ps localization from the two vertexes of three icosahedrons to one vertex, forming a long-lived S₁* state. Such phenomenon is not observed in Au25 (dimer) and Au13 (monomer) consisting of two and one icosahedrons, respectively. We have further observed temperature dependence on the localization process, which proves it is thermally driven. Two excited-state vibration modes with frequencies of 20 and 70 cm−1 observed in the kinetic traces are assigned to the axial and radial breathing modes, respectively. The electron localization is ascribed to the structural distortion of Au37 in the excited state induced by the strong coherent vibrations. The observed electron localization phenomenon provides unique physical insight into one-dimensional gold nanoclusters and other nanostructures, which will advance their applications in solar-energy storage and conversion.</description><identifier>ISSN: 0027-8424</identifier><identifier>EISSN: 1091-6490</identifier><identifier>DOI: 10.1073/pnas.1704699114</identifier><identifier>PMID: 28559316</identifier><language>eng</language><publisher>United States: National Academy of Sciences</publisher><subject>Breathing ; cluster ; Clusters ; electron dynamics ; electron localization ; Electron states ; Electrons ; Energy ; Energy storage ; Free electrons ; Frequencies ; Gold ; I.R. radiation ; Icosahedrons ; Infrared absorption ; Localization ; MATERIALS SCIENCE ; Nanoclusters ; Nanoparticles ; Near infrared radiation ; Photoexcitation ; Physical Sciences ; PNAS Plus ; Solar energy ; Temperature dependence ; Vibration ; Vibration mode ; Vibrations</subject><ispartof>Proceedings of the National Academy of Sciences - PNAS, 2017-06, Vol.114 (24), p.E4697-E4705</ispartof><rights>Volumes 1–89 and 106–114, copyright as a collective work only; author(s) retains copyright to individual articles</rights><rights>Copyright National Academy of Sciences Jun 13, 2017</rights><lds50>peer_reviewed</lds50><oa>free_for_read</oa><woscitedreferencessubscribed>false</woscitedreferencessubscribed><citedby>FETCH-LOGICAL-c536t-9d0f6d45d7df5d99702ae16b6d32d4e8bdc3e685e87022a793b0e8e22e2679923</citedby><cites>FETCH-LOGICAL-c536t-9d0f6d45d7df5d99702ae16b6d32d4e8bdc3e685e87022a793b0e8e22e2679923</cites><orcidid>0000-0001-5619-5722 ; 0000-0002-2525-8345 ; 0000000156195722 ; 0000000225258345</orcidid></display><links><openurl>$$Topenurl_article</openurl><openurlfulltext>$$Topenurlfull_article</openurlfulltext><thumbnail>$$Tsyndetics_thumb_exl</thumbnail><linktopdf>$$Uhttps://www.jstor.org/stable/pdf/26484227$$EPDF$$P50$$Gjstor$$H</linktopdf><linktohtml>$$Uhttps://www.jstor.org/stable/26484227$$EHTML$$P50$$Gjstor$$H</linktohtml><link.rule.ids>230,314,723,776,780,799,881,27901,27902,53766,53768,57992,58225</link.rule.ids><backlink>$$Uhttps://www.ncbi.nlm.nih.gov/pubmed/28559316$$D View this record in MEDLINE/PubMed$$Hfree_for_read</backlink><backlink>$$Uhttps://www.osti.gov/biblio/1360862$$D View this record in Osti.gov$$Hfree_for_read</backlink></links><search><creatorcontrib>Zhou, Meng</creatorcontrib><creatorcontrib>Jin, Renxi</creatorcontrib><creatorcontrib>Sfeir, Matthew Y.</creatorcontrib><creatorcontrib>Chen, Yuxiang</creatorcontrib><creatorcontrib>Song, Yongbo</creatorcontrib><creatorcontrib>Jin, Rongchao</creatorcontrib><creatorcontrib>Brookhaven National Laboratory (BNL), Upton, NY (United States). Center for Functional Nanomaterials (CFN)</creatorcontrib><title>Electron localization in rod-shaped triicosahedral gold nanocluster</title><title>Proceedings of the National Academy of Sciences - PNAS</title><addtitle>Proc Natl Acad Sci U S A</addtitle><description>Atomically precise gold nanocluster based on linear assembly of repeating icosahedrons (clusters of clusters) is a unique type of linear nanostructure, which exhibits strong near-infrared absorption as their free electrons are confined in a one-dimensional quantum box. Little is known about the carrier dynamics in these nanoclusters, which limit their energy-related applications. Here, we reported the observation of exciton localization in triicosahedral Au37 nanoclusters (0.5 nm in diameter and 1.6 nm in length) by measuring femtosecond and nanosecond carrier dynamics. Upon photoexcitation to S₁ electronic state, electrons in Au37 undergo ∼100-ps localization from the two vertexes of three icosahedrons to one vertex, forming a long-lived S₁* state. Such phenomenon is not observed in Au25 (dimer) and Au13 (monomer) consisting of two and one icosahedrons, respectively. We have further observed temperature dependence on the localization process, which proves it is thermally driven. Two excited-state vibration modes with frequencies of 20 and 70 cm−1 observed in the kinetic traces are assigned to the axial and radial breathing modes, respectively. The electron localization is ascribed to the structural distortion of Au37 in the excited state induced by the strong coherent vibrations. The observed electron localization phenomenon provides unique physical insight into one-dimensional gold nanoclusters and other nanostructures, which will advance their applications in solar-energy storage and conversion.</description><subject>Breathing</subject><subject>cluster</subject><subject>Clusters</subject><subject>electron dynamics</subject><subject>electron localization</subject><subject>Electron states</subject><subject>Electrons</subject><subject>Energy</subject><subject>Energy storage</subject><subject>Free electrons</subject><subject>Frequencies</subject><subject>Gold</subject><subject>I.R. radiation</subject><subject>Icosahedrons</subject><subject>Infrared absorption</subject><subject>Localization</subject><subject>MATERIALS SCIENCE</subject><subject>Nanoclusters</subject><subject>Nanoparticles</subject><subject>Near infrared radiation</subject><subject>Photoexcitation</subject><subject>Physical Sciences</subject><subject>PNAS Plus</subject><subject>Solar energy</subject><subject>Temperature dependence</subject><subject>Vibration</subject><subject>Vibration mode</subject><subject>Vibrations</subject><issn>0027-8424</issn><issn>1091-6490</issn><fulltext>true</fulltext><rsrctype>article</rsrctype><creationdate>2017</creationdate><recordtype>article</recordtype><recordid>eNpdkc1rVDEUxYModqyuXSkP3bh5bb4_NoIMVQsFN-06ZJI7nQxvkjHJK-hfb4aprXYVwvnl3JN7EHpL8BnBip3vk6tnRGEujSGEP0MLgg0ZJTf4OVpgTNWoOeUn6FWtW4yxERq_RCdUC2EYkQu0vJjAt5LTMGXvpvjbtdgvMQ0lh7Fu3B7C0EqMPle3gVDcNNzmKQzJpeynuTYor9GLtZsqvLk_T9HN14vr5ffx6se3y-WXq9ELJttoAl7LwEVQYS2CMQpTB0SuZGA0cNCr4BlILUB3hTpl2AqDBkqBSmUMZafo89F3P692EDyk1uPYfYk7V37Z7KL9X0lxY2_znRVccU1EN_hwNMi1RVt9bOA3PqfUV2AJk1jLw5RP91NK_jlDbXYXq4dpcgnyXC0xmFOqKFcd_fgE3ea5pL6DTnGhuCBGdur8SPmSay2wfkhMsD20aA8t2scW-4v3_370gf9bWwfeHYFtbbk86pLrQzb2BzUxoog</recordid><startdate>20170613</startdate><enddate>20170613</enddate><creator>Zhou, Meng</creator><creator>Jin, Renxi</creator><creator>Sfeir, Matthew Y.</creator><creator>Chen, Yuxiang</creator><creator>Song, Yongbo</creator><creator>Jin, Rongchao</creator><general>National Academy of Sciences</general><general>National Academy of Sciences, Washington, DC (United States)</general><scope>NPM</scope><scope>AAYXX</scope><scope>CITATION</scope><scope>7QG</scope><scope>7QL</scope><scope>7QP</scope><scope>7QR</scope><scope>7SN</scope><scope>7SS</scope><scope>7T5</scope><scope>7TK</scope><scope>7TM</scope><scope>7TO</scope><scope>7U9</scope><scope>8FD</scope><scope>C1K</scope><scope>FR3</scope><scope>H94</scope><scope>M7N</scope><scope>P64</scope><scope>RC3</scope><scope>7X8</scope><scope>OTOTI</scope><scope>5PM</scope><orcidid>https://orcid.org/0000-0001-5619-5722</orcidid><orcidid>https://orcid.org/0000-0002-2525-8345</orcidid><orcidid>https://orcid.org/0000000156195722</orcidid><orcidid>https://orcid.org/0000000225258345</orcidid></search><sort><creationdate>20170613</creationdate><title>Electron localization in rod-shaped triicosahedral gold nanocluster</title><author>Zhou, Meng ; Jin, Renxi ; Sfeir, Matthew Y. ; Chen, Yuxiang ; Song, Yongbo ; Jin, Rongchao</author></sort><facets><frbrtype>5</frbrtype><frbrgroupid>cdi_FETCH-LOGICAL-c536t-9d0f6d45d7df5d99702ae16b6d32d4e8bdc3e685e87022a793b0e8e22e2679923</frbrgroupid><rsrctype>articles</rsrctype><prefilter>articles</prefilter><language>eng</language><creationdate>2017</creationdate><topic>Breathing</topic><topic>cluster</topic><topic>Clusters</topic><topic>electron dynamics</topic><topic>electron localization</topic><topic>Electron states</topic><topic>Electrons</topic><topic>Energy</topic><topic>Energy storage</topic><topic>Free electrons</topic><topic>Frequencies</topic><topic>Gold</topic><topic>I.R. radiation</topic><topic>Icosahedrons</topic><topic>Infrared absorption</topic><topic>Localization</topic><topic>MATERIALS SCIENCE</topic><topic>Nanoclusters</topic><topic>Nanoparticles</topic><topic>Near infrared radiation</topic><topic>Photoexcitation</topic><topic>Physical Sciences</topic><topic>PNAS Plus</topic><topic>Solar energy</topic><topic>Temperature dependence</topic><topic>Vibration</topic><topic>Vibration mode</topic><topic>Vibrations</topic><toplevel>peer_reviewed</toplevel><toplevel>online_resources</toplevel><creatorcontrib>Zhou, Meng</creatorcontrib><creatorcontrib>Jin, Renxi</creatorcontrib><creatorcontrib>Sfeir, Matthew Y.</creatorcontrib><creatorcontrib>Chen, Yuxiang</creatorcontrib><creatorcontrib>Song, Yongbo</creatorcontrib><creatorcontrib>Jin, Rongchao</creatorcontrib><creatorcontrib>Brookhaven National Laboratory (BNL), Upton, NY (United States). 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Center for Functional Nanomaterials (CFN)</aucorp><format>journal</format><genre>article</genre><ristype>JOUR</ristype><atitle>Electron localization in rod-shaped triicosahedral gold nanocluster</atitle><jtitle>Proceedings of the National Academy of Sciences - PNAS</jtitle><addtitle>Proc Natl Acad Sci U S A</addtitle><date>2017-06-13</date><risdate>2017</risdate><volume>114</volume><issue>24</issue><spage>E4697</spage><epage>E4705</epage><pages>E4697-E4705</pages><issn>0027-8424</issn><eissn>1091-6490</eissn><abstract>Atomically precise gold nanocluster based on linear assembly of repeating icosahedrons (clusters of clusters) is a unique type of linear nanostructure, which exhibits strong near-infrared absorption as their free electrons are confined in a one-dimensional quantum box. Little is known about the carrier dynamics in these nanoclusters, which limit their energy-related applications. Here, we reported the observation of exciton localization in triicosahedral Au37 nanoclusters (0.5 nm in diameter and 1.6 nm in length) by measuring femtosecond and nanosecond carrier dynamics. Upon photoexcitation to S₁ electronic state, electrons in Au37 undergo ∼100-ps localization from the two vertexes of three icosahedrons to one vertex, forming a long-lived S₁* state. Such phenomenon is not observed in Au25 (dimer) and Au13 (monomer) consisting of two and one icosahedrons, respectively. We have further observed temperature dependence on the localization process, which proves it is thermally driven. Two excited-state vibration modes with frequencies of 20 and 70 cm−1 observed in the kinetic traces are assigned to the axial and radial breathing modes, respectively. The electron localization is ascribed to the structural distortion of Au37 in the excited state induced by the strong coherent vibrations. The observed electron localization phenomenon provides unique physical insight into one-dimensional gold nanoclusters and other nanostructures, which will advance their applications in solar-energy storage and conversion.</abstract><cop>United States</cop><pub>National Academy of Sciences</pub><pmid>28559316</pmid><doi>10.1073/pnas.1704699114</doi><orcidid>https://orcid.org/0000-0001-5619-5722</orcidid><orcidid>https://orcid.org/0000-0002-2525-8345</orcidid><orcidid>https://orcid.org/0000000156195722</orcidid><orcidid>https://orcid.org/0000000225258345</orcidid><oa>free_for_read</oa></addata></record> |
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| subjects | Breathing cluster Clusters electron dynamics electron localization Electron states Electrons Energy Energy storage Free electrons Frequencies Gold I.R. radiation Icosahedrons Infrared absorption Localization MATERIALS SCIENCE Nanoclusters Nanoparticles Near infrared radiation Photoexcitation Physical Sciences PNAS Plus Solar energy Temperature dependence Vibration Vibration mode Vibrations |
| title | Electron localization in rod-shaped triicosahedral gold nanocluster |
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