Biexciton and trion energy transfer from CdSe/CdS giant nanocrystals to Si substrates
Observation of energy transfer (ET) from multiexcitonic (MX) complexes in nanocrystal quantum dots (NQDs) has been severely restricted due to efficient nonradiative Auger recombination leading to very low MX emission quantum yields. Here we employed "giant" CdSe/CdS NQDs with suppressed Au...
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| Veröffentlicht in: | Nanoscale 2017-12, Vol.9 (48), p.19398-19407 |
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| container_title | Nanoscale |
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| creator | Guo, Tianle Sampat, Siddharth Rupich, Sara M Hollingsworth, Jennifer A Buck, Matthew Htoon, Han Chabal, Yves J Gartstein, Yuri N Malko, Anton V |
| description | Observation of energy transfer (ET) from multiexcitonic (MX) complexes in nanocrystal quantum dots (NQDs) has been severely restricted due to efficient nonradiative Auger recombination leading to very low MX emission quantum yields. Here we employed "giant" CdSe/CdS NQDs with suppressed Auger recombination to study ET of biexcitons (BX) and charged excitons (trions) into Si substrate. Photoluminescence (PL) measurements of (sub)monolayers of gNQDs controllably assembled on various interacting surfaces and augmented by single gNQD's imaging reveal appearance of BX spectral signatures and progressive acceleration of PL lifetimes of all excitonic species on Si substrates. From statistical analysis of a large number of PL lifetime traces, representative exciton, trion and BX ET efficiencies are measured as ∼75%, 55% and 45% respectively. Detailed analysis of the MX's radiative rates demonstrate the crucial role of the radiative (waveguide) ET in maintaining high overall transfer efficiency despite the prevalent Auger recombination. Our observations point towards practical utilization of MX-bearing nanocrystals in future optoelectronics architectures. |
| doi_str_mv | 10.1039/c7nr06272a |
| format | Article |
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(LANL), Los Alamos, NM (United States)</creatorcontrib><description>Observation of energy transfer (ET) from multiexcitonic (MX) complexes in nanocrystal quantum dots (NQDs) has been severely restricted due to efficient nonradiative Auger recombination leading to very low MX emission quantum yields. Here we employed "giant" CdSe/CdS NQDs with suppressed Auger recombination to study ET of biexcitons (BX) and charged excitons (trions) into Si substrate. Photoluminescence (PL) measurements of (sub)monolayers of gNQDs controllably assembled on various interacting surfaces and augmented by single gNQD's imaging reveal appearance of BX spectral signatures and progressive acceleration of PL lifetimes of all excitonic species on Si substrates. From statistical analysis of a large number of PL lifetime traces, representative exciton, trion and BX ET efficiencies are measured as ∼75%, 55% and 45% respectively. Detailed analysis of the MX's radiative rates demonstrate the crucial role of the radiative (waveguide) ET in maintaining high overall transfer efficiency despite the prevalent Auger recombination. 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From statistical analysis of a large number of PL lifetime traces, representative exciton, trion and BX ET efficiencies are measured as ∼75%, 55% and 45% respectively. Detailed analysis of the MX's radiative rates demonstrate the crucial role of the radiative (waveguide) ET in maintaining high overall transfer efficiency despite the prevalent Auger recombination. Our observations point towards practical utilization of MX-bearing nanocrystals in future optoelectronics architectures.</description><subject>Augers</subject><subject>Cadmium selenides</subject><subject>Cadmium sulfide</subject><subject>Energy transfer</subject><subject>Excitons</subject><subject>Material Science</subject><subject>MATERIALS SCIENCE</subject><subject>Nanocrystals</subject><subject>Optoelectronics</subject><subject>Photoluminescence</subject><subject>Quantum dots</subject><subject>Silicon substrates</subject><subject>Spectral signatures</subject><subject>Statistical analysis</subject><subject>Trions</subject><issn>2040-3364</issn><issn>2040-3372</issn><fulltext>true</fulltext><rsrctype>article</rsrctype><creationdate>2017</creationdate><recordtype>article</recordtype><recordid>eNpdkU1PGzEQhq2qVfloL_0BldVeUKXAjL2xvccQQamEQCpwtrzeWViU2NT2Ss2_xxDgwGW-9MyrGb2MfUM4RJDtkdchgRJauA9sV0ADMym1-PhWq2aH7eV8D6BaqeRntiNagdCg2mU3xyP992OJgbvQ85LGWlGgdLupjQt5oMSHFNd82V_RUQ38dnSh8OBC9GmTi1tlXiK_Gnmeulx3CuUv7NNQ5_T1Je-zm9OT6-XZ7Pzy95_l4nzmpTZlZlD1cwPekQJ0yjns-rlHQpJNC61p3EBSSqO8cvV4r7FRnek6LVEa4VHusx9b3ZjLaHP9g_ydjyGQLxbnGhTqCh1soYcU_02Ui12P2dNq5QLFKVtstWwUGvWk9_Mdeh-nFOoLVgCCMSAUVOrXlvIp5pxosA9pXLu0sQj2yRG71Bd_nx1ZVPj7i-TUral_Q18tkI-_GYQh</recordid><startdate>20171228</startdate><enddate>20171228</enddate><creator>Guo, Tianle</creator><creator>Sampat, Siddharth</creator><creator>Rupich, Sara M</creator><creator>Hollingsworth, Jennifer A</creator><creator>Buck, Matthew</creator><creator>Htoon, Han</creator><creator>Chabal, Yves J</creator><creator>Gartstein, Yuri N</creator><creator>Malko, Anton V</creator><general>Royal Society of Chemistry</general><scope>NPM</scope><scope>AAYXX</scope><scope>CITATION</scope><scope>7SR</scope><scope>7U5</scope><scope>8BQ</scope><scope>8FD</scope><scope>F28</scope><scope>FR3</scope><scope>JG9</scope><scope>L7M</scope><scope>7X8</scope><scope>OIOZB</scope><scope>OTOTI</scope><orcidid>https://orcid.org/0000-0001-6410-7112</orcidid><orcidid>https://orcid.org/0000-0003-3696-2896</orcidid><orcidid>https://orcid.org/0000-0002-6435-0347</orcidid><orcidid>https://orcid.org/0000000264350347</orcidid><orcidid>https://orcid.org/0000000330991215</orcidid><orcidid>https://orcid.org/0000000164107112</orcidid><orcidid>https://orcid.org/0000000336962896</orcidid></search><sort><creationdate>20171228</creationdate><title>Biexciton and trion energy transfer from CdSe/CdS giant nanocrystals to Si substrates</title><author>Guo, Tianle ; Sampat, Siddharth ; Rupich, Sara M ; Hollingsworth, Jennifer A ; Buck, Matthew ; Htoon, Han ; Chabal, Yves J ; Gartstein, Yuri N ; Malko, Anton V</author></sort><facets><frbrtype>5</frbrtype><frbrgroupid>cdi_FETCH-LOGICAL-c378t-816d580cae601a6aa1bd5c1e1e3490984afe33386c6a006c7146b8bb731382c13</frbrgroupid><rsrctype>articles</rsrctype><prefilter>articles</prefilter><language>eng</language><creationdate>2017</creationdate><topic>Augers</topic><topic>Cadmium selenides</topic><topic>Cadmium sulfide</topic><topic>Energy transfer</topic><topic>Excitons</topic><topic>Material Science</topic><topic>MATERIALS SCIENCE</topic><topic>Nanocrystals</topic><topic>Optoelectronics</topic><topic>Photoluminescence</topic><topic>Quantum dots</topic><topic>Silicon substrates</topic><topic>Spectral signatures</topic><topic>Statistical analysis</topic><topic>Trions</topic><toplevel>peer_reviewed</toplevel><toplevel>online_resources</toplevel><creatorcontrib>Guo, Tianle</creatorcontrib><creatorcontrib>Sampat, Siddharth</creatorcontrib><creatorcontrib>Rupich, Sara M</creatorcontrib><creatorcontrib>Hollingsworth, Jennifer A</creatorcontrib><creatorcontrib>Buck, Matthew</creatorcontrib><creatorcontrib>Htoon, Han</creatorcontrib><creatorcontrib>Chabal, Yves J</creatorcontrib><creatorcontrib>Gartstein, Yuri N</creatorcontrib><creatorcontrib>Malko, Anton V</creatorcontrib><creatorcontrib>Los Alamos National Lab. 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(LANL), Los Alamos, NM (United States)</aucorp><format>journal</format><genre>article</genre><ristype>JOUR</ristype><atitle>Biexciton and trion energy transfer from CdSe/CdS giant nanocrystals to Si substrates</atitle><jtitle>Nanoscale</jtitle><addtitle>Nanoscale</addtitle><date>2017-12-28</date><risdate>2017</risdate><volume>9</volume><issue>48</issue><spage>19398</spage><epage>19407</epage><pages>19398-19407</pages><issn>2040-3364</issn><eissn>2040-3372</eissn><abstract>Observation of energy transfer (ET) from multiexcitonic (MX) complexes in nanocrystal quantum dots (NQDs) has been severely restricted due to efficient nonradiative Auger recombination leading to very low MX emission quantum yields. Here we employed "giant" CdSe/CdS NQDs with suppressed Auger recombination to study ET of biexcitons (BX) and charged excitons (trions) into Si substrate. Photoluminescence (PL) measurements of (sub)monolayers of gNQDs controllably assembled on various interacting surfaces and augmented by single gNQD's imaging reveal appearance of BX spectral signatures and progressive acceleration of PL lifetimes of all excitonic species on Si substrates. From statistical analysis of a large number of PL lifetime traces, representative exciton, trion and BX ET efficiencies are measured as ∼75%, 55% and 45% respectively. Detailed analysis of the MX's radiative rates demonstrate the crucial role of the radiative (waveguide) ET in maintaining high overall transfer efficiency despite the prevalent Auger recombination. 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| source | Royal Society Of Chemistry Journals 2008- |
| subjects | Augers Cadmium selenides Cadmium sulfide Energy transfer Excitons Material Science MATERIALS SCIENCE Nanocrystals Optoelectronics Photoluminescence Quantum dots Silicon substrates Spectral signatures Statistical analysis Trions |
| title | Biexciton and trion energy transfer from CdSe/CdS giant nanocrystals to Si substrates |
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