Temperature Dependence of Excitonic Radiative Decay in CdSe Quantum Dots: The Role of Surface Hole Traps
Using atomistic, semiempirical pseudopotential calculations, we show that if one assumes the simplest form of a surface state in a CdSe nanocrystalan unpassivated surface anion siteone can explain theoretically several puzzling aspects regarding the observed temperature dependence of the radiative...
Gespeichert in:
| Veröffentlicht in: | Nano Letters 2005-12, Vol.5 (12), p.2360-2364 |
|---|---|
| Hauptverfasser: | , , |
| Format: | Artikel |
| Sprache: | eng |
| Schlagworte: | |
| Online-Zugang: | Volltext |
| Tags: |
Tag hinzufügen
Keine Tags, Fügen Sie den ersten Tag hinzu!
|
| container_end_page | 2364 |
|---|---|
| container_issue | 12 |
| container_start_page | 2360 |
| container_title | Nano Letters |
| container_volume | 5 |
| creator | Califano, Marco Franceschetti, Alberto Zunger, Alex |
| description | Using atomistic, semiempirical pseudopotential calculations, we show that if one assumes the simplest form of a surface state in a CdSe nanocrystalan unpassivated surface anion siteone can explain theoretically several puzzling aspects regarding the observed temperature dependence of the radiative decay of excitons. In particular, our calculations show that the presence of surface states leads to a mixing of the dark and bright exciton states, resulting in a decrease of 3 orders of magnitude of the dark-exciton radiative lifetime. This result explains the persistence of the zero-phonon emission line at low temperature, for which thermal population of higher-energy bright-exciton states is negligible. Thus, we suggest that surface states are the controlling factor of dark-exciton radiative recombination in currently synthesized colloidal CdSe nanocrystals. |
| doi_str_mv | 10.1021/nl051027p |
| format | Article |
| fullrecord | <record><control><sourceid>acs_osti_</sourceid><recordid>TN_cdi_crossref_primary_10_1021_nl051027p</recordid><sourceformat>XML</sourceformat><sourcesystem>PC</sourcesystem><sourcerecordid>b3776172</sourcerecordid><originalsourceid>FETCH-LOGICAL-a435t-2c62a44a5e3dc93370d7f8a0aa7d9a35a2734c213ddc7537ebe40a2c6b916d63</originalsourceid><addsrcrecordid>eNpt0L1OwzAUBWALgfgpDLwAMgMDQ8CO47hmQ6VQJCREyR7d2jcikDqRnSDYWHlNnoSUVpSBydfSd67lQ8ghZ2ecxfzcVUz2g2o2yC6XgkWp1vHm7zxMdsheCM-MMS0k2yY7PBWSczXcJS8Zzhv00HYe6RU26Cw6g7Qu6PjNlG3tSkOnYEtoy9eFMPBOS0dH9hHpQweu7eb0qm7DxdfHJ82ekE7r6if-2PkC-k2TxT3z0IR9slVAFfBgdQ5Idj3ORpPo7v7mdnR5F0EiZBvFJo0hSUCisEYLoZhVxRAYgLIahIRYicTEXFhrlBQKZ5gw6FMzzVObigE5Xq6tQ1vmof8EmidTO4emzbVKdR8akNOlMb4OwWORN76cg3_POcsXnea_nfb2aGmbbjZHu5arEntwsgIQDFSFB2fKsHZKSB3HfxyYkD_XnXd9C_88-A07SYqr</addsrcrecordid><sourcetype>Open Access Repository</sourcetype><iscdi>true</iscdi><recordtype>article</recordtype></control><display><type>article</type><title>Temperature Dependence of Excitonic Radiative Decay in CdSe Quantum Dots: The Role of Surface Hole Traps</title><source>ACS Publications</source><source>MEDLINE</source><creator>Califano, Marco ; Franceschetti, Alberto ; Zunger, Alex</creator><creatorcontrib>Califano, Marco ; Franceschetti, Alberto ; Zunger, Alex ; National Renewable Energy Lab. (NREL), Golden, CO (United States)</creatorcontrib><description>Using atomistic, semiempirical pseudopotential calculations, we show that if one assumes the simplest form of a surface state in a CdSe nanocrystalan unpassivated surface anion siteone can explain theoretically several puzzling aspects regarding the observed temperature dependence of the radiative decay of excitons. In particular, our calculations show that the presence of surface states leads to a mixing of the dark and bright exciton states, resulting in a decrease of 3 orders of magnitude of the dark-exciton radiative lifetime. This result explains the persistence of the zero-phonon emission line at low temperature, for which thermal population of higher-energy bright-exciton states is negligible. Thus, we suggest that surface states are the controlling factor of dark-exciton radiative recombination in currently synthesized colloidal CdSe nanocrystals.</description><identifier>ISSN: 1530-6984</identifier><identifier>EISSN: 1530-6992</identifier><identifier>DOI: 10.1021/nl051027p</identifier><identifier>PMID: 16351178</identifier><language>eng</language><publisher>Washington, DC: American Chemical Society</publisher><subject>ANIONS ; Basic Sciences ; Cadmium Compounds - analysis ; Cadmium Compounds - chemistry ; Cadmium Compounds - radiation effects ; Colloids - analysis ; Colloids - chemistry ; Colloids - radiation effects ; Condensed matter: electronic structure, electrical, magnetic, and optical properties ; Cross-disciplinary physics: materials science; rheology ; Crystallization - methods ; Electron states and collective excitations in thin films, multilayers, quantum wells, mesoscopic and nanoscale systems ; Electronic structure and electrical properties of surfaces, interfaces, thin films and low-dimensional structures ; Exact sciences and technology ; EXCITONS ; Half-Life ; Kinetics ; LIFETIME ; Light ; Materials science ; Materials Testing ; Nanoscale materials and structures: fabrication and characterization ; NANOSCIENCE AND NANOTECHNOLOGY ; Nanotechnology - methods ; Physics ; QUANTUM DOTS ; Quantum Nanostructures: Boxes, Films, Wires ; Radiation Dosage ; RADIATIVE DECAY ; Radiometry ; RECOMBINATION ; Selenium Compounds - analysis ; Selenium Compounds - chemistry ; Selenium Compounds - radiation effects ; Solid State Theory ; Surface Properties ; Temperature ; TEMPERATURE DEPENDENCE</subject><ispartof>Nano Letters, 2005-12, Vol.5 (12), p.2360-2364</ispartof><rights>Copyright © 2005 American Chemical Society</rights><rights>2006 INIST-CNRS</rights><lds50>peer_reviewed</lds50><woscitedreferencessubscribed>false</woscitedreferencessubscribed><citedby>FETCH-LOGICAL-a435t-2c62a44a5e3dc93370d7f8a0aa7d9a35a2734c213ddc7537ebe40a2c6b916d63</citedby><cites>FETCH-LOGICAL-a435t-2c62a44a5e3dc93370d7f8a0aa7d9a35a2734c213ddc7537ebe40a2c6b916d63</cites></display><links><openurl>$$Topenurl_article</openurl><openurlfulltext>$$Topenurlfull_article</openurlfulltext><thumbnail>$$Tsyndetics_thumb_exl</thumbnail><linktopdf>$$Uhttps://pubs.acs.org/doi/pdf/10.1021/nl051027p$$EPDF$$P50$$Gacs$$H</linktopdf><linktohtml>$$Uhttps://pubs.acs.org/doi/10.1021/nl051027p$$EHTML$$P50$$Gacs$$H</linktohtml><link.rule.ids>314,776,780,881,2752,27053,27901,27902,56713,56763</link.rule.ids><backlink>$$Uhttp://pascal-francis.inist.fr/vibad/index.php?action=getRecordDetail&idt=17359228$$DView record in Pascal Francis$$Hfree_for_read</backlink><backlink>$$Uhttps://www.ncbi.nlm.nih.gov/pubmed/16351178$$D View this record in MEDLINE/PubMed$$Hfree_for_read</backlink><backlink>$$Uhttps://www.osti.gov/biblio/976975$$D View this record in Osti.gov$$Hfree_for_read</backlink></links><search><creatorcontrib>Califano, Marco</creatorcontrib><creatorcontrib>Franceschetti, Alberto</creatorcontrib><creatorcontrib>Zunger, Alex</creatorcontrib><creatorcontrib>National Renewable Energy Lab. (NREL), Golden, CO (United States)</creatorcontrib><title>Temperature Dependence of Excitonic Radiative Decay in CdSe Quantum Dots: The Role of Surface Hole Traps</title><title>Nano Letters</title><addtitle>Nano Lett</addtitle><description>Using atomistic, semiempirical pseudopotential calculations, we show that if one assumes the simplest form of a surface state in a CdSe nanocrystalan unpassivated surface anion siteone can explain theoretically several puzzling aspects regarding the observed temperature dependence of the radiative decay of excitons. In particular, our calculations show that the presence of surface states leads to a mixing of the dark and bright exciton states, resulting in a decrease of 3 orders of magnitude of the dark-exciton radiative lifetime. This result explains the persistence of the zero-phonon emission line at low temperature, for which thermal population of higher-energy bright-exciton states is negligible. Thus, we suggest that surface states are the controlling factor of dark-exciton radiative recombination in currently synthesized colloidal CdSe nanocrystals.</description><subject>ANIONS</subject><subject>Basic Sciences</subject><subject>Cadmium Compounds - analysis</subject><subject>Cadmium Compounds - chemistry</subject><subject>Cadmium Compounds - radiation effects</subject><subject>Colloids - analysis</subject><subject>Colloids - chemistry</subject><subject>Colloids - radiation effects</subject><subject>Condensed matter: electronic structure, electrical, magnetic, and optical properties</subject><subject>Cross-disciplinary physics: materials science; rheology</subject><subject>Crystallization - methods</subject><subject>Electron states and collective excitations in thin films, multilayers, quantum wells, mesoscopic and nanoscale systems</subject><subject>Electronic structure and electrical properties of surfaces, interfaces, thin films and low-dimensional structures</subject><subject>Exact sciences and technology</subject><subject>EXCITONS</subject><subject>Half-Life</subject><subject>Kinetics</subject><subject>LIFETIME</subject><subject>Light</subject><subject>Materials science</subject><subject>Materials Testing</subject><subject>Nanoscale materials and structures: fabrication and characterization</subject><subject>NANOSCIENCE AND NANOTECHNOLOGY</subject><subject>Nanotechnology - methods</subject><subject>Physics</subject><subject>QUANTUM DOTS</subject><subject>Quantum Nanostructures: Boxes, Films, Wires</subject><subject>Radiation Dosage</subject><subject>RADIATIVE DECAY</subject><subject>Radiometry</subject><subject>RECOMBINATION</subject><subject>Selenium Compounds - analysis</subject><subject>Selenium Compounds - chemistry</subject><subject>Selenium Compounds - radiation effects</subject><subject>Solid State Theory</subject><subject>Surface Properties</subject><subject>Temperature</subject><subject>TEMPERATURE DEPENDENCE</subject><issn>1530-6984</issn><issn>1530-6992</issn><fulltext>true</fulltext><rsrctype>article</rsrctype><creationdate>2005</creationdate><recordtype>article</recordtype><sourceid>EIF</sourceid><recordid>eNpt0L1OwzAUBWALgfgpDLwAMgMDQ8CO47hmQ6VQJCREyR7d2jcikDqRnSDYWHlNnoSUVpSBydfSd67lQ8ghZ2ecxfzcVUz2g2o2yC6XgkWp1vHm7zxMdsheCM-MMS0k2yY7PBWSczXcJS8Zzhv00HYe6RU26Cw6g7Qu6PjNlG3tSkOnYEtoy9eFMPBOS0dH9hHpQweu7eb0qm7DxdfHJ82ekE7r6if-2PkC-k2TxT3z0IR9slVAFfBgdQ5Idj3ORpPo7v7mdnR5F0EiZBvFJo0hSUCisEYLoZhVxRAYgLIahIRYicTEXFhrlBQKZ5gw6FMzzVObigE5Xq6tQ1vmof8EmidTO4emzbVKdR8akNOlMb4OwWORN76cg3_POcsXnea_nfb2aGmbbjZHu5arEntwsgIQDFSFB2fKsHZKSB3HfxyYkD_XnXd9C_88-A07SYqr</recordid><startdate>20051201</startdate><enddate>20051201</enddate><creator>Califano, Marco</creator><creator>Franceschetti, Alberto</creator><creator>Zunger, Alex</creator><general>American Chemical Society</general><scope>IQODW</scope><scope>CGR</scope><scope>CUY</scope><scope>CVF</scope><scope>ECM</scope><scope>EIF</scope><scope>NPM</scope><scope>AAYXX</scope><scope>CITATION</scope><scope>OTOTI</scope></search><sort><creationdate>20051201</creationdate><title>Temperature Dependence of Excitonic Radiative Decay in CdSe Quantum Dots: The Role of Surface Hole Traps</title><author>Califano, Marco ; Franceschetti, Alberto ; Zunger, Alex</author></sort><facets><frbrtype>5</frbrtype><frbrgroupid>cdi_FETCH-LOGICAL-a435t-2c62a44a5e3dc93370d7f8a0aa7d9a35a2734c213ddc7537ebe40a2c6b916d63</frbrgroupid><rsrctype>articles</rsrctype><prefilter>articles</prefilter><language>eng</language><creationdate>2005</creationdate><topic>ANIONS</topic><topic>Basic Sciences</topic><topic>Cadmium Compounds - analysis</topic><topic>Cadmium Compounds - chemistry</topic><topic>Cadmium Compounds - radiation effects</topic><topic>Colloids - analysis</topic><topic>Colloids - chemistry</topic><topic>Colloids - radiation effects</topic><topic>Condensed matter: electronic structure, electrical, magnetic, and optical properties</topic><topic>Cross-disciplinary physics: materials science; rheology</topic><topic>Crystallization - methods</topic><topic>Electron states and collective excitations in thin films, multilayers, quantum wells, mesoscopic and nanoscale systems</topic><topic>Electronic structure and electrical properties of surfaces, interfaces, thin films and low-dimensional structures</topic><topic>Exact sciences and technology</topic><topic>EXCITONS</topic><topic>Half-Life</topic><topic>Kinetics</topic><topic>LIFETIME</topic><topic>Light</topic><topic>Materials science</topic><topic>Materials Testing</topic><topic>Nanoscale materials and structures: fabrication and characterization</topic><topic>NANOSCIENCE AND NANOTECHNOLOGY</topic><topic>Nanotechnology - methods</topic><topic>Physics</topic><topic>QUANTUM DOTS</topic><topic>Quantum Nanostructures: Boxes, Films, Wires</topic><topic>Radiation Dosage</topic><topic>RADIATIVE DECAY</topic><topic>Radiometry</topic><topic>RECOMBINATION</topic><topic>Selenium Compounds - analysis</topic><topic>Selenium Compounds - chemistry</topic><topic>Selenium Compounds - radiation effects</topic><topic>Solid State Theory</topic><topic>Surface Properties</topic><topic>Temperature</topic><topic>TEMPERATURE DEPENDENCE</topic><toplevel>peer_reviewed</toplevel><toplevel>online_resources</toplevel><creatorcontrib>Califano, Marco</creatorcontrib><creatorcontrib>Franceschetti, Alberto</creatorcontrib><creatorcontrib>Zunger, Alex</creatorcontrib><creatorcontrib>National Renewable Energy Lab. (NREL), Golden, CO (United States)</creatorcontrib><collection>Pascal-Francis</collection><collection>Medline</collection><collection>MEDLINE</collection><collection>MEDLINE (Ovid)</collection><collection>MEDLINE</collection><collection>MEDLINE</collection><collection>PubMed</collection><collection>CrossRef</collection><collection>OSTI.GOV</collection><jtitle>Nano Letters</jtitle></facets><delivery><delcategory>Remote Search Resource</delcategory><fulltext>fulltext</fulltext></delivery><addata><au>Califano, Marco</au><au>Franceschetti, Alberto</au><au>Zunger, Alex</au><aucorp>National Renewable Energy Lab. (NREL), Golden, CO (United States)</aucorp><format>journal</format><genre>article</genre><ristype>JOUR</ristype><atitle>Temperature Dependence of Excitonic Radiative Decay in CdSe Quantum Dots: The Role of Surface Hole Traps</atitle><jtitle>Nano Letters</jtitle><addtitle>Nano Lett</addtitle><date>2005-12-01</date><risdate>2005</risdate><volume>5</volume><issue>12</issue><spage>2360</spage><epage>2364</epage><pages>2360-2364</pages><issn>1530-6984</issn><eissn>1530-6992</eissn><abstract>Using atomistic, semiempirical pseudopotential calculations, we show that if one assumes the simplest form of a surface state in a CdSe nanocrystalan unpassivated surface anion siteone can explain theoretically several puzzling aspects regarding the observed temperature dependence of the radiative decay of excitons. In particular, our calculations show that the presence of surface states leads to a mixing of the dark and bright exciton states, resulting in a decrease of 3 orders of magnitude of the dark-exciton radiative lifetime. This result explains the persistence of the zero-phonon emission line at low temperature, for which thermal population of higher-energy bright-exciton states is negligible. Thus, we suggest that surface states are the controlling factor of dark-exciton radiative recombination in currently synthesized colloidal CdSe nanocrystals.</abstract><cop>Washington, DC</cop><pub>American Chemical Society</pub><pmid>16351178</pmid><doi>10.1021/nl051027p</doi><tpages>5</tpages></addata></record> |
| fulltext | fulltext |
| identifier | ISSN: 1530-6984 |
| ispartof | Nano Letters, 2005-12, Vol.5 (12), p.2360-2364 |
| issn | 1530-6984 1530-6992 |
| language | eng |
| recordid | cdi_crossref_primary_10_1021_nl051027p |
| source | ACS Publications; MEDLINE |
| subjects | ANIONS Basic Sciences Cadmium Compounds - analysis Cadmium Compounds - chemistry Cadmium Compounds - radiation effects Colloids - analysis Colloids - chemistry Colloids - radiation effects Condensed matter: electronic structure, electrical, magnetic, and optical properties Cross-disciplinary physics: materials science rheology Crystallization - methods Electron states and collective excitations in thin films, multilayers, quantum wells, mesoscopic and nanoscale systems Electronic structure and electrical properties of surfaces, interfaces, thin films and low-dimensional structures Exact sciences and technology EXCITONS Half-Life Kinetics LIFETIME Light Materials science Materials Testing Nanoscale materials and structures: fabrication and characterization NANOSCIENCE AND NANOTECHNOLOGY Nanotechnology - methods Physics QUANTUM DOTS Quantum Nanostructures: Boxes, Films, Wires Radiation Dosage RADIATIVE DECAY Radiometry RECOMBINATION Selenium Compounds - analysis Selenium Compounds - chemistry Selenium Compounds - radiation effects Solid State Theory Surface Properties Temperature TEMPERATURE DEPENDENCE |
| title | Temperature Dependence of Excitonic Radiative Decay in CdSe Quantum Dots: The Role of Surface Hole Traps |
| url | https://sfx.bib-bvb.de/sfx_tum?ctx_ver=Z39.88-2004&ctx_enc=info:ofi/enc:UTF-8&ctx_tim=2025-02-13T07%3A43%3A58IST&url_ver=Z39.88-2004&url_ctx_fmt=infofi/fmt:kev:mtx:ctx&rfr_id=info:sid/primo.exlibrisgroup.com:primo3-Article-acs_osti_&rft_val_fmt=info:ofi/fmt:kev:mtx:journal&rft.genre=article&rft.atitle=Temperature%20Dependence%20of%20Excitonic%20Radiative%20Decay%20in%20CdSe%20Quantum%20Dots:%E2%80%89%20The%20Role%20of%20Surface%20Hole%20Traps&rft.jtitle=Nano%20Letters&rft.au=Califano,%20Marco&rft.aucorp=National%20Renewable%20Energy%20Lab.%20(NREL),%20Golden,%20CO%20(United%20States)&rft.date=2005-12-01&rft.volume=5&rft.issue=12&rft.spage=2360&rft.epage=2364&rft.pages=2360-2364&rft.issn=1530-6984&rft.eissn=1530-6992&rft_id=info:doi/10.1021/nl051027p&rft_dat=%3Cacs_osti_%3Eb3776172%3C/acs_osti_%3E%3Curl%3E%3C/url%3E&disable_directlink=true&sfx.directlink=off&sfx.report_link=0&rft_id=info:oai/&rft_id=info:pmid/16351178&rfr_iscdi=true |