Ultrafast Electron Trapping at the Surface of Semiconductor Nanocrystals: Excitonic and Biexcitonic Processes
Aging of semiconductor nanocrystals (NCs) is well-known to attenuate the spontaneous photoluminescence from the band edge excitonic state by introduction of nonradiative trap states formed at the NC surface. In order to explore charge carrier dynamics dictated by the surface of the NC, femtosecond p...
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Veröffentlicht in: | The journal of physical chemistry. B 2013-04, Vol.117 (16), p.4412-4421 |
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creator | Saari, Jonathan I Dias, Eva A Reifsnyder, Danielle Krause, Michael M Walsh, Brenna R Murray, Christopher B Kambhampati, Patanjali |
description | Aging of semiconductor nanocrystals (NCs) is well-known to attenuate the spontaneous photoluminescence from the band edge excitonic state by introduction of nonradiative trap states formed at the NC surface. In order to explore charge carrier dynamics dictated by the surface of the NC, femtosecond pump/probe spectroscopic experiments are performed on freshly synthesized and aged CdTe NCs. These experiments reveal fast electron trapping for aged CdTe NCs from the single excitonic state (X). Pump fluence dependence with excitonic state-resolved optical pumping enables directly populating the biexcitonic state (XX), which produces further accelerated electron trapping rates. This increase in electron trapping rate triggers coherent acoustic phonons by virtue of the ultrafast impulsive time scale of the surface trapping process. The observed trapping rates are discussed in terms of electron transfer theory. |
doi_str_mv | 10.1021/jp307668g |
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In order to explore charge carrier dynamics dictated by the surface of the NC, femtosecond pump/probe spectroscopic experiments are performed on freshly synthesized and aged CdTe NCs. These experiments reveal fast electron trapping for aged CdTe NCs from the single excitonic state (X). Pump fluence dependence with excitonic state-resolved optical pumping enables directly populating the biexcitonic state (XX), which produces further accelerated electron trapping rates. This increase in electron trapping rate triggers coherent acoustic phonons by virtue of the ultrafast impulsive time scale of the surface trapping process. The observed trapping rates are discussed in terms of electron transfer theory.</description><identifier>ISSN: 1520-6106</identifier><identifier>EISSN: 1520-5207</identifier><identifier>DOI: 10.1021/jp307668g</identifier><identifier>PMID: 23186016</identifier><language>eng</language><publisher>Washington, DC: American Chemical Society</publisher><subject>Cadmium tellurides ; Condensed matter: electronic structure, electrical, magnetic, and optical properties ; Electronic structure and electrical properties of surfaces, interfaces, thin films and low-dimensional structures ; Electronic structure of nanoscale materials : clusters, nanoparticles, nanotubes, and nanocrystals ; Exact sciences and technology ; Excitation ; Femtosecond ; Nanocrystals ; Nanocrystals and nanoparticles ; Optical properties and condensed-matter spectroscopy and other interactions of matter with particles and radiation ; Optical properties of low-dimensional, mesoscopic, and nanoscale materials and structures ; Phonons ; Physics ; Pumps ; Semiconductors ; Trapping</subject><ispartof>The journal of physical chemistry. 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B</title><addtitle>J. Phys. Chem. B</addtitle><description>Aging of semiconductor nanocrystals (NCs) is well-known to attenuate the spontaneous photoluminescence from the band edge excitonic state by introduction of nonradiative trap states formed at the NC surface. In order to explore charge carrier dynamics dictated by the surface of the NC, femtosecond pump/probe spectroscopic experiments are performed on freshly synthesized and aged CdTe NCs. These experiments reveal fast electron trapping for aged CdTe NCs from the single excitonic state (X). Pump fluence dependence with excitonic state-resolved optical pumping enables directly populating the biexcitonic state (XX), which produces further accelerated electron trapping rates. This increase in electron trapping rate triggers coherent acoustic phonons by virtue of the ultrafast impulsive time scale of the surface trapping process. The observed trapping rates are discussed in terms of electron transfer theory.</description><subject>Cadmium tellurides</subject><subject>Condensed matter: electronic structure, electrical, magnetic, and optical properties</subject><subject>Electronic structure and electrical properties of surfaces, interfaces, thin films and low-dimensional structures</subject><subject>Electronic structure of nanoscale materials : clusters, nanoparticles, nanotubes, and nanocrystals</subject><subject>Exact sciences and technology</subject><subject>Excitation</subject><subject>Femtosecond</subject><subject>Nanocrystals</subject><subject>Nanocrystals and nanoparticles</subject><subject>Optical properties and condensed-matter spectroscopy and other interactions of matter with particles and radiation</subject><subject>Optical properties of low-dimensional, mesoscopic, and nanoscale materials and structures</subject><subject>Phonons</subject><subject>Physics</subject><subject>Pumps</subject><subject>Semiconductors</subject><subject>Trapping</subject><issn>1520-6106</issn><issn>1520-5207</issn><fulltext>true</fulltext><rsrctype>article</rsrctype><creationdate>2013</creationdate><recordtype>article</recordtype><recordid>eNqF0UtLHEEQAOBGIrpZPeQPhL4EzGG1H9uPyS2RjQpiArueh5p-mFlmuifdPaD_PiOu6yUgVFFd8FENVQh9ouScEkYvtgMnSkr9cIBmVDCymFJ92L0lJfIYfcx5SwgTTMsjdMw41ZJQOUP9fVcSeMgFrzpnSooBbxIMQxseMBRc_ji8HpMH43D0eO361sRgR1NiwncQoklPuUCXv-HVo2lLDK3BECz-0bp9_ztF43J2-QQd-sm6012do_ufq83l9eL219XN5ffbBXCly0JproFVjC0rbxrC7FLYRnJhdWO8ZNw3SvKG6opKK5hbgmHcWmknrUAKyefo7GXukOLf0eVS9202rusguDjmmirBBSV8incpX0qhieJ8ol9fqEkx5-R8PaS2h_RUU1I_H6LeH2Kyn3djx6Z3di9fNz-BLzsA2UDnEwTT5jenOFWyqt4cmFxv45jCtLj_fPgPy9icnw</recordid><startdate>20130425</startdate><enddate>20130425</enddate><creator>Saari, Jonathan I</creator><creator>Dias, Eva A</creator><creator>Reifsnyder, Danielle</creator><creator>Krause, Michael M</creator><creator>Walsh, Brenna R</creator><creator>Murray, Christopher B</creator><creator>Kambhampati, Patanjali</creator><general>American Chemical Society</general><scope>IQODW</scope><scope>NPM</scope><scope>AAYXX</scope><scope>CITATION</scope><scope>7X8</scope><scope>7SR</scope><scope>7U5</scope><scope>8BQ</scope><scope>8FD</scope><scope>JG9</scope><scope>L7M</scope></search><sort><creationdate>20130425</creationdate><title>Ultrafast Electron Trapping at the Surface of Semiconductor Nanocrystals: Excitonic and Biexcitonic Processes</title><author>Saari, Jonathan I ; Dias, Eva A ; Reifsnyder, Danielle ; Krause, Michael M ; Walsh, Brenna R ; Murray, Christopher B ; Kambhampati, Patanjali</author></sort><facets><frbrtype>5</frbrtype><frbrgroupid>cdi_FETCH-LOGICAL-a378t-7838a292249fcb02d45db635d8bcf623fb763b18916d52e4ac23dd6d9fc7a6563</frbrgroupid><rsrctype>articles</rsrctype><prefilter>articles</prefilter><language>eng</language><creationdate>2013</creationdate><topic>Cadmium tellurides</topic><topic>Condensed matter: electronic structure, electrical, magnetic, and optical properties</topic><topic>Electronic structure and electrical properties of surfaces, interfaces, thin films and low-dimensional structures</topic><topic>Electronic structure of nanoscale materials : clusters, nanoparticles, nanotubes, and nanocrystals</topic><topic>Exact sciences and technology</topic><topic>Excitation</topic><topic>Femtosecond</topic><topic>Nanocrystals</topic><topic>Nanocrystals and nanoparticles</topic><topic>Optical properties and condensed-matter spectroscopy and other interactions of matter with particles and radiation</topic><topic>Optical properties of low-dimensional, mesoscopic, and nanoscale materials and structures</topic><topic>Phonons</topic><topic>Physics</topic><topic>Pumps</topic><topic>Semiconductors</topic><topic>Trapping</topic><toplevel>peer_reviewed</toplevel><toplevel>online_resources</toplevel><creatorcontrib>Saari, Jonathan I</creatorcontrib><creatorcontrib>Dias, Eva A</creatorcontrib><creatorcontrib>Reifsnyder, Danielle</creatorcontrib><creatorcontrib>Krause, Michael M</creatorcontrib><creatorcontrib>Walsh, Brenna R</creatorcontrib><creatorcontrib>Murray, Christopher B</creatorcontrib><creatorcontrib>Kambhampati, Patanjali</creatorcontrib><collection>Pascal-Francis</collection><collection>PubMed</collection><collection>CrossRef</collection><collection>MEDLINE - Academic</collection><collection>Engineered Materials Abstracts</collection><collection>Solid State and Superconductivity Abstracts</collection><collection>METADEX</collection><collection>Technology Research Database</collection><collection>Materials Research Database</collection><collection>Advanced Technologies Database with Aerospace</collection><jtitle>The journal of physical chemistry. B</jtitle></facets><delivery><delcategory>Remote Search Resource</delcategory><fulltext>fulltext</fulltext></delivery><addata><au>Saari, Jonathan I</au><au>Dias, Eva A</au><au>Reifsnyder, Danielle</au><au>Krause, Michael M</au><au>Walsh, Brenna R</au><au>Murray, Christopher B</au><au>Kambhampati, Patanjali</au><format>journal</format><genre>article</genre><ristype>JOUR</ristype><atitle>Ultrafast Electron Trapping at the Surface of Semiconductor Nanocrystals: Excitonic and Biexcitonic Processes</atitle><jtitle>The journal of physical chemistry. B</jtitle><addtitle>J. Phys. Chem. B</addtitle><date>2013-04-25</date><risdate>2013</risdate><volume>117</volume><issue>16</issue><spage>4412</spage><epage>4421</epage><pages>4412-4421</pages><issn>1520-6106</issn><eissn>1520-5207</eissn><abstract>Aging of semiconductor nanocrystals (NCs) is well-known to attenuate the spontaneous photoluminescence from the band edge excitonic state by introduction of nonradiative trap states formed at the NC surface. In order to explore charge carrier dynamics dictated by the surface of the NC, femtosecond pump/probe spectroscopic experiments are performed on freshly synthesized and aged CdTe NCs. These experiments reveal fast electron trapping for aged CdTe NCs from the single excitonic state (X). Pump fluence dependence with excitonic state-resolved optical pumping enables directly populating the biexcitonic state (XX), which produces further accelerated electron trapping rates. This increase in electron trapping rate triggers coherent acoustic phonons by virtue of the ultrafast impulsive time scale of the surface trapping process. The observed trapping rates are discussed in terms of electron transfer theory.</abstract><cop>Washington, DC</cop><pub>American Chemical Society</pub><pmid>23186016</pmid><doi>10.1021/jp307668g</doi><tpages>10</tpages></addata></record> |
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subjects | Cadmium tellurides Condensed matter: electronic structure, electrical, magnetic, and optical properties Electronic structure and electrical properties of surfaces, interfaces, thin films and low-dimensional structures Electronic structure of nanoscale materials : clusters, nanoparticles, nanotubes, and nanocrystals Exact sciences and technology Excitation Femtosecond Nanocrystals Nanocrystals and nanoparticles Optical properties and condensed-matter spectroscopy and other interactions of matter with particles and radiation Optical properties of low-dimensional, mesoscopic, and nanoscale materials and structures Phonons Physics Pumps Semiconductors Trapping |
title | Ultrafast Electron Trapping at the Surface of Semiconductor Nanocrystals: Excitonic and Biexcitonic Processes |
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