Dynamic Hole Blockade Yields Two-Color Quantum and Classical Light from Dot-in-Bulk Nanocrystals
Semiconductor nanocrystals (NCs) are an emerging class of color-tunable, solution-processable, room-temperature single-photon sources. Photon antibunching in NCs arises from suppression of multiphoton emission by nonradiative Auger recombination. Here, we demonstrate a new antibunching mechanismdyn...
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| Veröffentlicht in: | Nano Lett 2013-01, Vol.13 (1), p.321-328 |
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| creator | Galland, Christophe Brovelli, Sergio Bae, Wan Ki Padilha, Lazaro A Meinardi, Francesco Klimov, Victor I |
| description | Semiconductor nanocrystals (NCs) are an emerging class of color-tunable, solution-processable, room-temperature single-photon sources. Photon antibunching in NCs arises from suppression of multiphoton emission by nonradiative Auger recombination. Here, we demonstrate a new antibunching mechanismdynamic Coulomb blockadewhich allows for generating both quantum and classical light from the same NC without detrimental effects of Auger decay. This mechanism is realized in novel dot-in-bulk (DiB) nanostructures comprising a quantum-confined CdSe core overcoated with a thick, bulk-like CdS shell. The presence of one hole in the core suppresses the capture of the second hole forcing it to recombine in the shell region. Under weak excitation, these NCs emit red antibunched light (core emission). At higher pump levels they exhibit an additional green band (shell emission) with bulk-like, Poissonian photon statistics. The unusual versatility of these novel nanoscale light sources, that combine mutually correlated channels for quantum and classical emission and additionally allow for facile tunability of effective color, opens new interesting opportunities for a range of applications from quantum optics to sensing and nanoscale imaging. |
| doi_str_mv | 10.1021/nl3045316 |
| format | Article |
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Photon antibunching in NCs arises from suppression of multiphoton emission by nonradiative Auger recombination. Here, we demonstrate a new antibunching mechanismdynamic Coulomb blockadewhich allows for generating both quantum and classical light from the same NC without detrimental effects of Auger decay. This mechanism is realized in novel dot-in-bulk (DiB) nanostructures comprising a quantum-confined CdSe core overcoated with a thick, bulk-like CdS shell. The presence of one hole in the core suppresses the capture of the second hole forcing it to recombine in the shell region. Under weak excitation, these NCs emit red antibunched light (core emission). At higher pump levels they exhibit an additional green band (shell emission) with bulk-like, Poissonian photon statistics. The unusual versatility of these novel nanoscale light sources, that combine mutually correlated channels for quantum and classical emission and additionally allow for facile tunability of effective color, opens new interesting opportunities for a range of applications from quantum optics to sensing and nanoscale imaging.</description><identifier>ISSN: 1530-6984</identifier><identifier>EISSN: 1530-6992</identifier><identifier>DOI: 10.1021/nl3045316</identifier><identifier>PMID: 23252581</identifier><language>eng</language><publisher>Washington, DC: American Chemical Society</publisher><subject>Augers ; Blocking ; Channels ; Condensed matter: structure, mechanical and thermal properties ; Cross-disciplinary physics: materials science; rheology ; Emission ; Exact sciences and technology ; Low-dimensional structures (superlattices, quantum well structures, multilayers): structure, and nonelectronic properties ; Materials science ; Nanocrystalline materials ; Nanocrystals ; Nanoscale materials and structures: fabrication and characterization ; Nanostructure ; Photons ; Physics ; Semiconductors ; solar (photovoltaic), solar (fuels), solid state lighting, bio-inspired, electrodes - solar, defects, charge transport, materials and chemistry by design, optics, synthesis (novel materials), synthesis (scalable processing) ; Statistics ; Surfaces and interfaces; thin films and whiskers (structure and nonelectronic properties)</subject><ispartof>Nano Lett, 2013-01, Vol.13 (1), p.321-328</ispartof><rights>Copyright © 2012 American Chemical Society</rights><rights>2014 INIST-CNRS</rights><lds50>peer_reviewed</lds50><woscitedreferencessubscribed>false</woscitedreferencessubscribed><citedby>FETCH-LOGICAL-a471t-99b1382725ea92e1b5f9a2aa8d85e08808a526af9abd2adef644ec8a1827f3a93</citedby><cites>FETCH-LOGICAL-a471t-99b1382725ea92e1b5f9a2aa8d85e08808a526af9abd2adef644ec8a1827f3a93</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/nl3045316$$EPDF$$P50$$Gacs$$H</linktopdf><linktohtml>$$Uhttps://pubs.acs.org/doi/10.1021/nl3045316$$EHTML$$P50$$Gacs$$H</linktohtml><link.rule.ids>314,780,784,885,2765,27076,27924,27925,56738,56788</link.rule.ids><backlink>$$Uhttp://pascal-francis.inist.fr/vibad/index.php?action=getRecordDetail&idt=27145490$$DView record in Pascal Francis$$Hfree_for_read</backlink><backlink>$$Uhttps://www.ncbi.nlm.nih.gov/pubmed/23252581$$D View this record in MEDLINE/PubMed$$Hfree_for_read</backlink><backlink>$$Uhttps://www.osti.gov/biblio/1105283$$D View this record in Osti.gov$$Hfree_for_read</backlink></links><search><creatorcontrib>Galland, Christophe</creatorcontrib><creatorcontrib>Brovelli, Sergio</creatorcontrib><creatorcontrib>Bae, Wan Ki</creatorcontrib><creatorcontrib>Padilha, Lazaro A</creatorcontrib><creatorcontrib>Meinardi, Francesco</creatorcontrib><creatorcontrib>Klimov, Victor I</creatorcontrib><creatorcontrib>Center for Advanced Solar Photophysics (CASP)</creatorcontrib><creatorcontrib>Energy Frontier Research Centers (EFRC)</creatorcontrib><title>Dynamic Hole Blockade Yields Two-Color Quantum and Classical Light from Dot-in-Bulk Nanocrystals</title><title>Nano Lett</title><addtitle>Nano Lett</addtitle><description>Semiconductor nanocrystals (NCs) are an emerging class of color-tunable, solution-processable, room-temperature single-photon sources. Photon antibunching in NCs arises from suppression of multiphoton emission by nonradiative Auger recombination. Here, we demonstrate a new antibunching mechanismdynamic Coulomb blockadewhich allows for generating both quantum and classical light from the same NC without detrimental effects of Auger decay. This mechanism is realized in novel dot-in-bulk (DiB) nanostructures comprising a quantum-confined CdSe core overcoated with a thick, bulk-like CdS shell. The presence of one hole in the core suppresses the capture of the second hole forcing it to recombine in the shell region. Under weak excitation, these NCs emit red antibunched light (core emission). At higher pump levels they exhibit an additional green band (shell emission) with bulk-like, Poissonian photon statistics. The unusual versatility of these novel nanoscale light sources, that combine mutually correlated channels for quantum and classical emission and additionally allow for facile tunability of effective color, opens new interesting opportunities for a range of applications from quantum optics to sensing and nanoscale imaging.</description><subject>Augers</subject><subject>Blocking</subject><subject>Channels</subject><subject>Condensed matter: structure, mechanical and thermal properties</subject><subject>Cross-disciplinary physics: materials science; rheology</subject><subject>Emission</subject><subject>Exact sciences and technology</subject><subject>Low-dimensional structures (superlattices, quantum well structures, multilayers): structure, and nonelectronic properties</subject><subject>Materials science</subject><subject>Nanocrystalline materials</subject><subject>Nanocrystals</subject><subject>Nanoscale materials and structures: fabrication and characterization</subject><subject>Nanostructure</subject><subject>Photons</subject><subject>Physics</subject><subject>Semiconductors</subject><subject>solar (photovoltaic), solar (fuels), solid state lighting, bio-inspired, electrodes - solar, defects, charge transport, materials and chemistry by design, optics, synthesis (novel materials), synthesis (scalable processing)</subject><subject>Statistics</subject><subject>Surfaces and interfaces; 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Brovelli, Sergio ; Bae, Wan Ki ; Padilha, Lazaro A ; Meinardi, Francesco ; Klimov, Victor I</author></sort><facets><frbrtype>5</frbrtype><frbrgroupid>cdi_FETCH-LOGICAL-a471t-99b1382725ea92e1b5f9a2aa8d85e08808a526af9abd2adef644ec8a1827f3a93</frbrgroupid><rsrctype>articles</rsrctype><prefilter>articles</prefilter><language>eng</language><creationdate>2013</creationdate><topic>Augers</topic><topic>Blocking</topic><topic>Channels</topic><topic>Condensed matter: structure, mechanical and thermal properties</topic><topic>Cross-disciplinary physics: materials science; rheology</topic><topic>Emission</topic><topic>Exact sciences and technology</topic><topic>Low-dimensional structures (superlattices, quantum well structures, multilayers): structure, and nonelectronic properties</topic><topic>Materials science</topic><topic>Nanocrystalline materials</topic><topic>Nanocrystals</topic><topic>Nanoscale materials and structures: fabrication and characterization</topic><topic>Nanostructure</topic><topic>Photons</topic><topic>Physics</topic><topic>Semiconductors</topic><topic>solar (photovoltaic), solar (fuels), solid state lighting, bio-inspired, electrodes - solar, defects, charge transport, materials and chemistry by design, optics, synthesis (novel materials), synthesis (scalable processing)</topic><topic>Statistics</topic><topic>Surfaces and interfaces; thin films and whiskers (structure and nonelectronic properties)</topic><toplevel>peer_reviewed</toplevel><toplevel>online_resources</toplevel><creatorcontrib>Galland, Christophe</creatorcontrib><creatorcontrib>Brovelli, Sergio</creatorcontrib><creatorcontrib>Bae, Wan Ki</creatorcontrib><creatorcontrib>Padilha, Lazaro A</creatorcontrib><creatorcontrib>Meinardi, Francesco</creatorcontrib><creatorcontrib>Klimov, Victor I</creatorcontrib><creatorcontrib>Center for Advanced Solar Photophysics (CASP)</creatorcontrib><creatorcontrib>Energy Frontier Research Centers (EFRC)</creatorcontrib><collection>Pascal-Francis</collection><collection>PubMed</collection><collection>CrossRef</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><collection>OSTI.GOV</collection><jtitle>Nano Lett</jtitle></facets><delivery><delcategory>Remote Search Resource</delcategory><fulltext>fulltext</fulltext></delivery><addata><au>Galland, Christophe</au><au>Brovelli, Sergio</au><au>Bae, Wan Ki</au><au>Padilha, Lazaro A</au><au>Meinardi, Francesco</au><au>Klimov, Victor I</au><aucorp>Center for Advanced Solar Photophysics (CASP)</aucorp><aucorp>Energy Frontier Research Centers (EFRC)</aucorp><format>journal</format><genre>article</genre><ristype>JOUR</ristype><atitle>Dynamic Hole Blockade Yields Two-Color Quantum and Classical Light from Dot-in-Bulk Nanocrystals</atitle><jtitle>Nano Lett</jtitle><addtitle>Nano Lett</addtitle><date>2013-01-09</date><risdate>2013</risdate><volume>13</volume><issue>1</issue><spage>321</spage><epage>328</epage><pages>321-328</pages><issn>1530-6984</issn><eissn>1530-6992</eissn><abstract>Semiconductor nanocrystals (NCs) are an emerging class of color-tunable, solution-processable, room-temperature single-photon sources. Photon antibunching in NCs arises from suppression of multiphoton emission by nonradiative Auger recombination. Here, we demonstrate a new antibunching mechanismdynamic Coulomb blockadewhich allows for generating both quantum and classical light from the same NC without detrimental effects of Auger decay. This mechanism is realized in novel dot-in-bulk (DiB) nanostructures comprising a quantum-confined CdSe core overcoated with a thick, bulk-like CdS shell. The presence of one hole in the core suppresses the capture of the second hole forcing it to recombine in the shell region. Under weak excitation, these NCs emit red antibunched light (core emission). At higher pump levels they exhibit an additional green band (shell emission) with bulk-like, Poissonian photon statistics. The unusual versatility of these novel nanoscale light sources, that combine mutually correlated channels for quantum and classical emission and additionally allow for facile tunability of effective color, opens new interesting opportunities for a range of applications from quantum optics to sensing and nanoscale imaging.</abstract><cop>Washington, DC</cop><pub>American Chemical Society</pub><pmid>23252581</pmid><doi>10.1021/nl3045316</doi><tpages>8</tpages></addata></record> |
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| subjects | Augers Blocking Channels Condensed matter: structure, mechanical and thermal properties Cross-disciplinary physics: materials science rheology Emission Exact sciences and technology Low-dimensional structures (superlattices, quantum well structures, multilayers): structure, and nonelectronic properties Materials science Nanocrystalline materials Nanocrystals Nanoscale materials and structures: fabrication and characterization Nanostructure Photons Physics Semiconductors solar (photovoltaic), solar (fuels), solid state lighting, bio-inspired, electrodes - solar, defects, charge transport, materials and chemistry by design, optics, synthesis (novel materials), synthesis (scalable processing) Statistics Surfaces and interfaces thin films and whiskers (structure and nonelectronic properties) |
| title | Dynamic Hole Blockade Yields Two-Color Quantum and Classical Light from Dot-in-Bulk Nanocrystals |
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