Role of Symmetry Breaking on the Optical Transitions in Lead-Salt Quantum Dots
The influence of quantum confinement on the one- and two-photon absorption spectra (1PA and 2PA) of PbS and PbSe semiconductor quantum dots (QDs) is investigated. The results show 2PA peaks at energies where only 1PA transitions are predicted and 1PA peaks where only 2PA transitions are predicted by...
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| Veröffentlicht in: | Nano letters 2010-09, Vol.10 (9), p.3577-3582 |
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| creator | Nootz, Gero Padilha, Lazaro A Olszak, Peter D Webster, Scott Hagan, David J Van Stryland, Eric W Levina, Larissa Sukhovatkin, Vlad Brzozowski, Lukasz Sargent, Edward H |
| description | The influence of quantum confinement on the one- and two-photon absorption spectra (1PA and 2PA) of PbS and PbSe semiconductor quantum dots (QDs) is investigated. The results show 2PA peaks at energies where only 1PA transitions are predicted and 1PA peaks where only 2PA transitions are predicted by the often used isotropic k·p four-band envelope function formalism. The first experimentally identified two-photon absorption peak coincides with the energy of the first one photon allowed transition. This first two-photon peak cannot be explained by band anisotropy, verifying that the inversion symmetry of the wave functions is broken and relaxation of the parity selection rules has to be taken into account to explain optical transitions in lead-salt QDs. Thus, while the band anisotropy of the bulk semiconductor plays a role in the absorption spectra, especially for the more anisotropic PbSe QDs, a complete model of the absorption spectra, for both 1PA and 2PA, must also include symmetry breaking of the quantum confined wave functions. These studies clarify the controversy of the origin of spectral features in lead-salt QDs. |
| doi_str_mv | 10.1021/nl1018673 |
| format | Article |
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The results show 2PA peaks at energies where only 1PA transitions are predicted and 1PA peaks where only 2PA transitions are predicted by the often used isotropic k·p four-band envelope function formalism. The first experimentally identified two-photon absorption peak coincides with the energy of the first one photon allowed transition. This first two-photon peak cannot be explained by band anisotropy, verifying that the inversion symmetry of the wave functions is broken and relaxation of the parity selection rules has to be taken into account to explain optical transitions in lead-salt QDs. Thus, while the band anisotropy of the bulk semiconductor plays a role in the absorption spectra, especially for the more anisotropic PbSe QDs, a complete model of the absorption spectra, for both 1PA and 2PA, must also include symmetry breaking of the quantum confined wave functions. These studies clarify the controversy of the origin of spectral features in lead-salt QDs.</description><identifier>ISSN: 1530-6984</identifier><identifier>EISSN: 1530-6992</identifier><identifier>DOI: 10.1021/nl1018673</identifier><identifier>PMID: 20734976</identifier><language>eng</language><publisher>Washington, DC: American Chemical Society</publisher><subject>Applied sciences ; Condensed matter: electronic structure, electrical, magnetic, and optical properties ; Cross-disciplinary physics: materials science; rheology ; Electronics ; Exact sciences and technology ; Fullerenes and related materials ; Materials science ; Molecular electronics, nanoelectronics ; Nanocrystalline materials ; Nanoscale materials and structures: fabrication and characterization ; Optical properties and condensed-matter spectroscopy and other interactions of matter with particles and radiation ; Physics ; Quantum dots ; Semiconductor electronics. Microelectronics. Optoelectronics. Solid state devices ; Visible and ultraviolet spectra</subject><ispartof>Nano letters, 2010-09, Vol.10 (9), p.3577-3582</ispartof><rights>Copyright © 2010 American Chemical Society</rights><rights>2015 INIST-CNRS</rights><lds50>peer_reviewed</lds50><woscitedreferencessubscribed>false</woscitedreferencessubscribed><citedby>FETCH-LOGICAL-a410t-f511b183f92021c357e5d3778d41439841a928eafd8de777d741b3a599f8c5703</citedby><cites>FETCH-LOGICAL-a410t-f511b183f92021c357e5d3778d41439841a928eafd8de777d741b3a599f8c5703</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/nl1018673$$EPDF$$P50$$Gacs$$H</linktopdf><linktohtml>$$Uhttps://pubs.acs.org/doi/10.1021/nl1018673$$EHTML$$P50$$Gacs$$H</linktohtml><link.rule.ids>314,776,780,2752,27053,27901,27902,56713,56763</link.rule.ids><backlink>$$Uhttp://pascal-francis.inist.fr/vibad/index.php?action=getRecordDetail&idt=23218143$$DView record in Pascal Francis$$Hfree_for_read</backlink><backlink>$$Uhttps://www.ncbi.nlm.nih.gov/pubmed/20734976$$D View this record in MEDLINE/PubMed$$Hfree_for_read</backlink></links><search><creatorcontrib>Nootz, Gero</creatorcontrib><creatorcontrib>Padilha, Lazaro A</creatorcontrib><creatorcontrib>Olszak, Peter D</creatorcontrib><creatorcontrib>Webster, Scott</creatorcontrib><creatorcontrib>Hagan, David J</creatorcontrib><creatorcontrib>Van Stryland, Eric W</creatorcontrib><creatorcontrib>Levina, Larissa</creatorcontrib><creatorcontrib>Sukhovatkin, Vlad</creatorcontrib><creatorcontrib>Brzozowski, Lukasz</creatorcontrib><creatorcontrib>Sargent, Edward H</creatorcontrib><title>Role of Symmetry Breaking on the Optical Transitions in Lead-Salt Quantum Dots</title><title>Nano letters</title><addtitle>Nano Lett</addtitle><description>The influence of quantum confinement on the one- and two-photon absorption spectra (1PA and 2PA) of PbS and PbSe semiconductor quantum dots (QDs) is investigated. The results show 2PA peaks at energies where only 1PA transitions are predicted and 1PA peaks where only 2PA transitions are predicted by the often used isotropic k·p four-band envelope function formalism. The first experimentally identified two-photon absorption peak coincides with the energy of the first one photon allowed transition. This first two-photon peak cannot be explained by band anisotropy, verifying that the inversion symmetry of the wave functions is broken and relaxation of the parity selection rules has to be taken into account to explain optical transitions in lead-salt QDs. Thus, while the band anisotropy of the bulk semiconductor plays a role in the absorption spectra, especially for the more anisotropic PbSe QDs, a complete model of the absorption spectra, for both 1PA and 2PA, must also include symmetry breaking of the quantum confined wave functions. These studies clarify the controversy of the origin of spectral features in lead-salt QDs.</description><subject>Applied sciences</subject><subject>Condensed matter: electronic structure, electrical, magnetic, and optical properties</subject><subject>Cross-disciplinary physics: materials science; rheology</subject><subject>Electronics</subject><subject>Exact sciences and technology</subject><subject>Fullerenes and related materials</subject><subject>Materials science</subject><subject>Molecular electronics, nanoelectronics</subject><subject>Nanocrystalline materials</subject><subject>Nanoscale materials and structures: fabrication and characterization</subject><subject>Optical properties and condensed-matter spectroscopy and other interactions of matter with particles and radiation</subject><subject>Physics</subject><subject>Quantum dots</subject><subject>Semiconductor electronics. Microelectronics. Optoelectronics. Solid state devices</subject><subject>Visible and ultraviolet spectra</subject><issn>1530-6984</issn><issn>1530-6992</issn><fulltext>true</fulltext><rsrctype>article</rsrctype><creationdate>2010</creationdate><recordtype>article</recordtype><recordid>eNptkM1OAyEURonR2Fpd-AKGjTEuRmEYCiy1_iaNjbauJ3QGlDoDFZhF315Ma7txde_i5LvfPQCcYnSFUY6vbYMR5kNG9kAfU4KyoRD5_nbnRQ8chbBACAlC0SHo5YiRQrBhH7y8uUZBp-F01bYq-hW89Up-GfsBnYXxU8HJMppKNnDmpQ0mGmcDNBaOlayzqWwifO2kjV0L71wMx-BAyyaok80cgPeH-9noKRtPHp9HN-NMFhjFTFOM55gTLfLUvyKUKVoTxnhd4IKkwliKnCupa14rxljNCjwnkgqheUUZIgNwsc5devfdqRDL1oRKNY20ynWhZLRAecriibxck5V3IXily6U3rfSrEqPy1165tZfYs01qN29VvSX_dCXgfAPIkJzopKQyYceRHPP0wI6TVSgXrvM2yfjn4A-cuYB_</recordid><startdate>20100908</startdate><enddate>20100908</enddate><creator>Nootz, Gero</creator><creator>Padilha, Lazaro A</creator><creator>Olszak, Peter D</creator><creator>Webster, Scott</creator><creator>Hagan, David J</creator><creator>Van Stryland, Eric W</creator><creator>Levina, Larissa</creator><creator>Sukhovatkin, Vlad</creator><creator>Brzozowski, Lukasz</creator><creator>Sargent, Edward H</creator><general>American Chemical Society</general><scope>IQODW</scope><scope>NPM</scope><scope>AAYXX</scope><scope>CITATION</scope><scope>7X8</scope></search><sort><creationdate>20100908</creationdate><title>Role of Symmetry Breaking on the Optical Transitions in Lead-Salt Quantum Dots</title><author>Nootz, Gero ; Padilha, Lazaro A ; Olszak, Peter D ; Webster, Scott ; Hagan, David J ; Van Stryland, Eric W ; Levina, Larissa ; Sukhovatkin, Vlad ; Brzozowski, Lukasz ; Sargent, Edward H</author></sort><facets><frbrtype>5</frbrtype><frbrgroupid>cdi_FETCH-LOGICAL-a410t-f511b183f92021c357e5d3778d41439841a928eafd8de777d741b3a599f8c5703</frbrgroupid><rsrctype>articles</rsrctype><prefilter>articles</prefilter><language>eng</language><creationdate>2010</creationdate><topic>Applied sciences</topic><topic>Condensed matter: electronic structure, electrical, magnetic, and optical properties</topic><topic>Cross-disciplinary physics: materials science; rheology</topic><topic>Electronics</topic><topic>Exact sciences and technology</topic><topic>Fullerenes and related materials</topic><topic>Materials science</topic><topic>Molecular electronics, nanoelectronics</topic><topic>Nanocrystalline materials</topic><topic>Nanoscale materials and structures: fabrication and characterization</topic><topic>Optical properties and condensed-matter spectroscopy and other interactions of matter with particles and radiation</topic><topic>Physics</topic><topic>Quantum dots</topic><topic>Semiconductor electronics. Microelectronics. Optoelectronics. Solid state devices</topic><topic>Visible and ultraviolet spectra</topic><toplevel>peer_reviewed</toplevel><toplevel>online_resources</toplevel><creatorcontrib>Nootz, Gero</creatorcontrib><creatorcontrib>Padilha, Lazaro A</creatorcontrib><creatorcontrib>Olszak, Peter D</creatorcontrib><creatorcontrib>Webster, Scott</creatorcontrib><creatorcontrib>Hagan, David J</creatorcontrib><creatorcontrib>Van Stryland, Eric W</creatorcontrib><creatorcontrib>Levina, Larissa</creatorcontrib><creatorcontrib>Sukhovatkin, Vlad</creatorcontrib><creatorcontrib>Brzozowski, Lukasz</creatorcontrib><creatorcontrib>Sargent, Edward H</creatorcontrib><collection>Pascal-Francis</collection><collection>PubMed</collection><collection>CrossRef</collection><collection>MEDLINE - Academic</collection><jtitle>Nano letters</jtitle></facets><delivery><delcategory>Remote Search Resource</delcategory><fulltext>fulltext</fulltext></delivery><addata><au>Nootz, Gero</au><au>Padilha, Lazaro A</au><au>Olszak, Peter D</au><au>Webster, Scott</au><au>Hagan, David J</au><au>Van Stryland, Eric W</au><au>Levina, Larissa</au><au>Sukhovatkin, Vlad</au><au>Brzozowski, Lukasz</au><au>Sargent, Edward H</au><format>journal</format><genre>article</genre><ristype>JOUR</ristype><atitle>Role of Symmetry Breaking on the Optical Transitions in Lead-Salt Quantum Dots</atitle><jtitle>Nano letters</jtitle><addtitle>Nano Lett</addtitle><date>2010-09-08</date><risdate>2010</risdate><volume>10</volume><issue>9</issue><spage>3577</spage><epage>3582</epage><pages>3577-3582</pages><issn>1530-6984</issn><eissn>1530-6992</eissn><abstract>The influence of quantum confinement on the one- and two-photon absorption spectra (1PA and 2PA) of PbS and PbSe semiconductor quantum dots (QDs) is investigated. The results show 2PA peaks at energies where only 1PA transitions are predicted and 1PA peaks where only 2PA transitions are predicted by the often used isotropic k·p four-band envelope function formalism. The first experimentally identified two-photon absorption peak coincides with the energy of the first one photon allowed transition. This first two-photon peak cannot be explained by band anisotropy, verifying that the inversion symmetry of the wave functions is broken and relaxation of the parity selection rules has to be taken into account to explain optical transitions in lead-salt QDs. Thus, while the band anisotropy of the bulk semiconductor plays a role in the absorption spectra, especially for the more anisotropic PbSe QDs, a complete model of the absorption spectra, for both 1PA and 2PA, must also include symmetry breaking of the quantum confined wave functions. 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| subjects | Applied sciences Condensed matter: electronic structure, electrical, magnetic, and optical properties Cross-disciplinary physics: materials science rheology Electronics Exact sciences and technology Fullerenes and related materials Materials science Molecular electronics, nanoelectronics Nanocrystalline materials Nanoscale materials and structures: fabrication and characterization Optical properties and condensed-matter spectroscopy and other interactions of matter with particles and radiation Physics Quantum dots Semiconductor electronics. Microelectronics. Optoelectronics. Solid state devices Visible and ultraviolet spectra |
| title | Role of Symmetry Breaking on the Optical Transitions in Lead-Salt Quantum Dots |
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