Many-body levels of optically excited and multiply charged InAs nanocrystals modeled by semiempirical tight binding
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Abstract
Many-body levels of optically excited and multiply charged InAs nanocrystals are studied with the semiempirical tight-binding model. Single-particle levels of unstrained spherical InAs nanocrystals are described by the sp3d5s* nearest-neighbor tight-binding model including spin-orbit coupling. For optically excited InAs nanocrystals, first-order corrections of electron-hole Coulomb and exchange interaction to exciton levels and the oscillator strengths of the exciton levels determine several low-lying, bright-exciton levels. The origin of the large oscillator strengths of the bright exciton levels is explained by the analysis of dominant angular momenta of exciton envelope functions. Good agreement with photoluminescence excitation experiments is achieved for the size dependence of the three lowest bright-exciton energies of InAs nanocrystals with radius larger than 20 Å. For multiply charged InAs nanocrystals, polarization of the nanocrystal environment is approximated by modeling the environment with a uniform dielectric medium. This polarization model incorporated into the tight-binding model provides a reasonable description of electron and hole addition energies in scanning tunneling spectroscopy experiments.
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<record><TEI><teiHeader><fileDesc><titleStmt><title xml:lang="en" level="a">Many-body levels of optically excited and multiply charged InAs nanocrystals modeled by semiempirical tight binding</title><author><name sortKey="Lee, Seungwon" uniqKey="Lee S">Seungwon Lee</name><affiliation wicri:level="2"><inist:fA14 i1="01"><s1>Department of Physics, Ohio State University, Columbus, Ohio 43210</s1><sZ>1 aut.</sZ><sZ>4 aut.</sZ><sZ>5 aut.</sZ><sZ>6 aut.</sZ></inist:fA14><country xml:lang="fr">États-Unis</country><placeName><region type="state">Ohio</region></placeName><wicri:cityArea>Department of Physics, Ohio State University, Columbus</wicri:cityArea></affiliation><affiliation wicri:level="2"><inist:fA14 i1="02"><s1>National Center for Supercomputing Applications, University of Illinois at Urbana-Champaign, Urbana, Illinois 61801</s1><sZ>1 aut.</sZ><sZ>2 aut.</sZ><sZ>3 aut.</sZ></inist:fA14><country xml:lang="fr">États-Unis</country><placeName><region type="state">Illinois</region></placeName><wicri:cityArea>National Center for Supercomputing Applications, University of Illinois at Urbana-Champaign, Urbana</wicri:cityArea></affiliation><affiliation wicri:level="2"><inist:fA14 i1="03"><s1>National Institute of Standards and Technology, Gaithersburg, Maryland 20899</s1></inist:fA14><country xml:lang="fr">États-Unis</country><placeName><region type="state">Maryland</region></placeName><wicri:cityArea>National Institute of Standards and Technology, Gaithersburg</wicri:cityArea></affiliation><affiliation wicri:level="2"><inist:fA14 i1="04"><s1>Jet Propulsion Laboratory, California Institute of Technology, Pasadena, California 91109</s1></inist:fA14><country xml:lang="fr">États-Unis</country><placeName><region type="state">Californie</region></placeName><wicri:cityArea>Jet Propulsion Laboratory, California Institute of Technology, Pasadena</wicri:cityArea></affiliation></author><author><name sortKey="Kim, Jeongnim" uniqKey="Kim J">Jeongnim Kim</name><affiliation wicri:level="2"><inist:fA14 i1="02"><s1>National Center for Supercomputing Applications, University of Illinois at Urbana-Champaign, Urbana, Illinois 61801</s1><sZ>1 aut.</sZ><sZ>2 aut.</sZ><sZ>3 aut.</sZ></inist:fA14><country xml:lang="fr">États-Unis</country><placeName><region type="state">Illinois</region></placeName><wicri:cityArea>National Center for Supercomputing Applications, University of Illinois at Urbana-Champaign, Urbana</wicri:cityArea></affiliation></author><author><name sortKey="Jonsson, Lars" uniqKey="Jonsson L">Lars Jonsson</name><affiliation wicri:level="2"><inist:fA14 i1="02"><s1>National Center for Supercomputing Applications, University of Illinois at Urbana-Champaign, Urbana, Illinois 61801</s1><sZ>1 aut.</sZ><sZ>2 aut.</sZ><sZ>3 aut.</sZ></inist:fA14><country xml:lang="fr">États-Unis</country><placeName><region type="state">Illinois</region></placeName><wicri:cityArea>National Center for Supercomputing Applications, University of Illinois at Urbana-Champaign, Urbana</wicri:cityArea></affiliation></author><author><name sortKey="Wilkins, John W" uniqKey="Wilkins J">John W. Wilkins</name><affiliation wicri:level="2"><inist:fA14 i1="01"><s1>Department of Physics, Ohio State University, Columbus, Ohio 43210</s1><sZ>1 aut.</sZ><sZ>4 aut.</sZ><sZ>5 aut.</sZ><sZ>6 aut.</sZ></inist:fA14><country xml:lang="fr">États-Unis</country><placeName><region type="state">Ohio</region></placeName><wicri:cityArea>Department of Physics, Ohio State University, Columbus</wicri:cityArea></affiliation></author><author><name sortKey="Bryant, Garnett W" uniqKey="Bryant G">Garnett W. Bryant</name><affiliation wicri:level="2"><inist:fA14 i1="01"><s1>Department of Physics, Ohio State University, Columbus, Ohio 43210</s1><sZ>1 aut.</sZ><sZ>4 aut.</sZ><sZ>5 aut.</sZ><sZ>6 aut.</sZ></inist:fA14><country xml:lang="fr">États-Unis</country><placeName><region type="state">Ohio</region></placeName><wicri:cityArea>Department of Physics, Ohio State University, Columbus</wicri:cityArea></affiliation></author><author><name sortKey="Klimeck, Gerhard" uniqKey="Klimeck G">Gerhard Klimeck</name><affiliation wicri:level="2"><inist:fA14 i1="01"><s1>Department of Physics, Ohio State University, Columbus, Ohio 43210</s1><sZ>1 aut.</sZ><sZ>4 aut.</sZ><sZ>5 aut.</sZ><sZ>6 aut.</sZ></inist:fA14><country xml:lang="fr">États-Unis</country><placeName><region type="state">Ohio</region></placeName><wicri:cityArea>Department of Physics, Ohio State University, Columbus</wicri:cityArea></affiliation></author></titleStmt><publicationStmt><idno type="inist">03-0032680</idno><date when="2002-12-15">2002-12-15</date><idno type="stanalyst">PASCAL 03-0032680 AIP</idno><idno type="RBID">Pascal:03-0032680</idno><idno type="wicri:Area/Main/Corpus">00E034</idno><idno type="wicri:Area/Main/Repository">00DC01</idno></publicationStmt><seriesStmt><idno type="ISSN">1098-0121</idno><title level="j" type="abbreviated">Phys. rev., B, Condens. matter mater. phys.</title><title level="j" type="main">Physical review. B, Condensed matter and materials physics</title></seriesStmt></fileDesc><profileDesc><textClass><keywords scheme="KwdEn" xml:lang="en"><term>Excitons</term><term>III-V semiconductors</term><term>Indium compounds</term><term>Nanostructured materials</term><term>Oscillator strengths</term><term>Photoluminescence</term><term>Scanning tunneling spectroscopy</term><term>Spin-orbit interactions</term><term>Theoretical study</term><term>Tight-binding calculations</term><term>Visible spectra</term><term>many-body problems</term></keywords><keywords scheme="Pascal" xml:lang="fr"><term>7322</term><term>7867</term><term>Etude théorique</term><term>Indium composé</term><term>Nanomatériau</term><term>Calcul liaison forte</term><term>Force oscillateur</term><term>Exciton</term><term>Photoluminescence</term><term>Spectre visible</term><term>Interaction spin orbite</term><term>Spectrométrie tunnel balayage</term><term>Semiconducteur III-V</term></keywords></textClass></profileDesc></teiHeader><front><div type="abstract" xml:lang="en">Many-body levels of optically excited and multiply charged InAs nanocrystals are studied with the semiempirical tight-binding model. Single-particle levels of unstrained spherical InAs nanocrystals are described by the sp<sup>3</sup>d<sup>5</sup>s<sup>*</sup> nearest-neighbor tight-binding model including spin-orbit coupling. For optically excited InAs nanocrystals, first-order corrections of electron-hole Coulomb and exchange interaction to exciton levels and the oscillator strengths of the exciton levels determine several low-lying, bright-exciton levels. The origin of the large oscillator strengths of the bright exciton levels is explained by the analysis of dominant angular momenta of exciton envelope functions. Good agreement with photoluminescence excitation experiments is achieved for the size dependence of the three lowest bright-exciton energies of InAs nanocrystals with radius larger than 20 Å. For multiply charged InAs nanocrystals, polarization of the nanocrystal environment is approximated by modeling the environment with a uniform dielectric medium. This polarization model incorporated into the tight-binding model provides a reasonable description of electron and hole addition energies in scanning tunneling spectroscopy experiments.</div></front></TEI><inist><standard h6="B"><pA><fA01 i1="01" i2="1"><s0>1098-0121</s0></fA01><fA02 i1="01"><s0>PRBMDO</s0></fA02><fA03 i2="1"><s0>Phys. rev., B, Condens. matter mater. phys.</s0></fA03><fA05><s2>66</s2></fA05><fA06><s2>23</s2></fA06><fA08 i1="01" i2="1" l="ENG"><s1>Many-body levels of optically excited and multiply charged InAs nanocrystals modeled by semiempirical tight binding</s1></fA08><fA11 i1="01" i2="1"><s1>LEE (Seungwon)</s1></fA11><fA11 i1="02" i2="1"><s1>KIM (Jeongnim)</s1></fA11><fA11 i1="03" i2="1"><s1>JONSSON (Lars)</s1></fA11><fA11 i1="04" i2="1"><s1>WILKINS (John W.)</s1></fA11><fA11 i1="05" i2="1"><s1>BRYANT (Garnett W.)</s1></fA11><fA11 i1="06" i2="1"><s1>KLIMECK (Gerhard)</s1></fA11><fA14 i1="01"><s1>Department of Physics, Ohio State University, Columbus, Ohio 43210</s1><sZ>1 aut.</sZ><sZ>4 aut.</sZ><sZ>5 aut.</sZ><sZ>6 aut.</sZ></fA14><fA14 i1="02"><s1>National Center for Supercomputing Applications, University of Illinois at Urbana-Champaign, Urbana, Illinois 61801</s1><sZ>1 aut.</sZ><sZ>2 aut.</sZ><sZ>3 aut.</sZ></fA14><fA14 i1="03"><s1>National Institute of Standards and Technology, Gaithersburg, Maryland 20899</s1></fA14><fA14 i1="04"><s1>Jet Propulsion Laboratory, California Institute of Technology, Pasadena, California 91109</s1></fA14><fA20><s2>235307-235307-12</s2></fA20><fA21><s1>2002-12-15</s1></fA21><fA23 i1="01"><s0>ENG</s0></fA23><fA43 i1="01"><s1>INIST</s1><s2>144 B</s2></fA43><fA44><s0>8100</s0><s1>© 2003 American Institute of Physics. All rights reserved.</s1></fA44><fA47 i1="01" i2="1"><s0>03-0032680</s0></fA47><fA60><s1>P</s1></fA60><fA61><s0>A</s0></fA61><fA64 i1="01" i2="1"><s0>Physical review. B, Condensed matter and materials physics</s0></fA64><fA66 i1="01"><s0>USA</s0></fA66><fC01 i1="01" l="ENG"><s0>Many-body levels of optically excited and multiply charged InAs nanocrystals are studied with the semiempirical tight-binding model. Single-particle levels of unstrained spherical InAs nanocrystals are described by the sp<sup>3</sup>d<sup>5</sup>s<sup>*</sup> nearest-neighbor tight-binding model including spin-orbit coupling. For optically excited InAs nanocrystals, first-order corrections of electron-hole Coulomb and exchange interaction to exciton levels and the oscillator strengths of the exciton levels determine several low-lying, bright-exciton levels. The origin of the large oscillator strengths of the bright exciton levels is explained by the analysis of dominant angular momenta of exciton envelope functions. Good agreement with photoluminescence excitation experiments is achieved for the size dependence of the three lowest bright-exciton energies of InAs nanocrystals with radius larger than 20 Å. For multiply charged InAs nanocrystals, polarization of the nanocrystal environment is approximated by modeling the environment with a uniform dielectric medium. This polarization model incorporated into the tight-binding model provides a reasonable description of electron and hole addition energies in scanning tunneling spectroscopy experiments.</s0></fC01><fC02 i1="01" i2="3"><s0>001B70C22</s0></fC02><fC02 i1="02" i2="3"><s0>001B70H67</s0></fC02><fC03 i1="01" i2="3" l="FRE"><s0>7322</s0><s2>PAC</s2><s4>INC</s4></fC03><fC03 i1="02" i2="3" l="FRE"><s0>7867</s0><s2>PAC</s2><s4>INC</s4></fC03><fC03 i1="03" i2="3" l="FRE"><s0>Etude théorique</s0></fC03><fC03 i1="03" i2="3" l="ENG"><s0>Theoretical study</s0></fC03><fC03 i1="04" i2="3" l="FRE"><s0>Indium composé</s0></fC03><fC03 i1="04" i2="3" l="ENG"><s0>Indium compounds</s0></fC03><fC03 i1="05" i2="3" l="FRE"><s0>Nanomatériau</s0></fC03><fC03 i1="05" i2="3" l="ENG"><s0>Nanostructured materials</s0></fC03><fC03 i1="06" i2="3" l="ENG"><s0>many-body problems</s0><s4>INC</s4></fC03><fC03 i1="07" i2="3" l="FRE"><s0>Calcul liaison forte</s0></fC03><fC03 i1="07" i2="3" l="ENG"><s0>Tight-binding calculations</s0></fC03><fC03 i1="08" i2="3" l="FRE"><s0>Force oscillateur</s0></fC03><fC03 i1="08" i2="3" l="ENG"><s0>Oscillator strengths</s0></fC03><fC03 i1="09" i2="3" l="FRE"><s0>Exciton</s0></fC03><fC03 i1="09" i2="3" l="ENG"><s0>Excitons</s0></fC03><fC03 i1="10" i2="3" l="FRE"><s0>Photoluminescence</s0></fC03><fC03 i1="10" i2="3" l="ENG"><s0>Photoluminescence</s0></fC03><fC03 i1="11" i2="3" l="FRE"><s0>Spectre visible</s0></fC03><fC03 i1="11" i2="3" l="ENG"><s0>Visible spectra</s0></fC03><fC03 i1="12" i2="3" l="FRE"><s0>Interaction spin orbite</s0></fC03><fC03 i1="12" i2="3" l="ENG"><s0>Spin-orbit interactions</s0></fC03><fC03 i1="13" i2="3" l="FRE"><s0>Spectrométrie tunnel balayage</s0></fC03><fC03 i1="13" i2="3" l="ENG"><s0>Scanning tunneling spectroscopy</s0></fC03><fC03 i1="14" i2="3" l="FRE"><s0>Semiconducteur III-V</s0></fC03><fC03 i1="14" i2="3" l="ENG"><s0>III-V semiconductors</s0></fC03><fN21><s1>013</s1></fN21><fN47 i1="01" i2="1"><s0>0301M000899</s0></fN47></pA></standard></inist></record>Pour manipuler ce document sous Unix (Dilib)
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