Synthesis and Spectroscopy of Silver-Doped PbSe Quantum Dots

Kroupa, Daniel M.; Hughes, Barbara K.; Miller, Elisa M.; Moore, David T.; Anderson, Nicholas C.; Chernomordik, Boris D.; Nozik, Arthur J.; Beard, Matthew C.

doi:10.1021/jacs.7b04551

Title: Synthesis and Spectroscopy of Silver-Doped PbSe Quantum Dots

Journal Article · Sun Jun 25 00:00:00 EDT 2017 · Journal of the American Chemical Society

DOI:https://doi.org/10.1021/jacs.7b04551· OSTI ID:1374971

^[1]; Hughes, Barbara K. ^[1]; Miller, Elisa M. ^[2]; Moore, David T. ^[2]; Anderson, Nicholas C. ^[2]; Chernomordik, Boris D. ^[2]; Nozik, Arthur J. ^[1];

^[2]

National Renewable Energy Lab. (NREL), Golden, CO (United States); Univ. of Colorado, Boulder, CO (United States)
National Renewable Energy Lab. (NREL), Golden, CO (United States)

Electronic impurity doping of bulk semiconductors is an essential component of semiconductor science and technology. Yet there are only a handful of studies demonstrating control of electronic impurities in semiconductor nanocrystals. Here, we studied electronic impurity doping of colloidal PbSe quantum dots (QDs) using a postsynthetic cation exchange reaction in which Pb is exchanged for Ag. We found that varying the concentration of dopants exposed to the as-synthesized PbSe QDs controls the extent of exchange. The electronic impurity doped QDs exhibit the fundamental spectroscopic signatures associated with injecting a free charge carrier into a QD under equilibrium conditions, including a bleach of the first exciton transition and the appearance of a quantum-confined, low-energy intraband absorption feature. Photoelectron spectroscopy confirms that Ag acts as a p-type dopant for PbSe QDs and infrared spectroscopy is consistent with k • p calculations of the size-dependent intraband transition energy. We find that to bleach the first exciton transition by an average of 1 carrier per QD requires that approximately 10% of the Pb be replaced by Ag. Here, we hypothesize that the majority of incorporated Ag remains at the QD surface and does not interact with the core electronic states of the QD. Instead, the excess Ag at the surface promotes the incorporation of <1% Ag into the QD core where it causes p-type doping behavior.

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Research Organization:: National Renewable Energy Laboratory (NREL), Golden, CO (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: AC36-08GO28308

OSTI ID:: 1374971

Report Number(s):: NREL/JA-5900-67594; TRN: US1702347

Journal Information:: Journal of the American Chemical Society, Vol. 139, Issue 30; ISSN 0002-7863

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 48 works

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References (43)

Controlled Chemical Doping of Semiconductor Nanocrystals Using Redox Buffers Engel, Jesse H.; Surendranath, Yogesh; Alivisatos, A. Paul Journal of the American Chemical Society, Vol. 134, Issue 32 https://doi.org/10.1021/ja305293e	journal	August 2012
Heavily doped n-type PbSe and PbS nanocrystals using ground-state charge transfer from cobaltocene Koh, Weon-kyu; Koposov, Alexey Y.; Stewart, John T. Scientific Reports, Vol. 3, Issue 1 https://doi.org/10.1038/srep02004	journal	June 2013
n-type colloidal semiconductor nanocrystals Shim, Moonsub; Guyot-Sionnest, Philippe Nature, Vol. 407, Issue 6807 https://doi.org/10.1038/35039577	journal	October 2000
Photochemical Electronic Doping of Colloidal CdSe Nanocrystals Rinehart, Jeffrey D.; Schimpf, Alina M.; Weaver, Amanda L. Journal of the American Chemical Society, Vol. 135, Issue 50 https://doi.org/10.1021/ja410825c	journal	December 2013
Electron and Hole Injection in PbSe Quantum Dot Films Wehrenberg, Brian L.; Guyot-Sionnest, Philippe Journal of the American Chemical Society, Vol. 125, Issue 26 https://doi.org/10.1021/ja035369d	journal	July 2003
Electrochromic Nanocrystal Quantum Dots Wang, C. Science, Vol. 291, Issue 5512 https://doi.org/10.1126/science.291.5512.2390	journal	March 2001
n- and p-Type HgTe Quantum Dot Films Liu, Heng; Keuleyan, Sean; Guyot-Sionnest, Philippe The Journal of Physical Chemistry C, Vol. 116, Issue 1 https://doi.org/10.1021/jp2109169	journal	December 2011
Electronic Doping and Redox-Potential Tuning in Colloidal Semiconductor Nanocrystals Schimpf, Alina M.; Knowles, Kathryn E.; Carroll, Gerard M. Accounts of Chemical Research, Vol. 48, Issue 7 https://doi.org/10.1021/acs.accounts.5b00181	journal	June 2015
Doping the undopable Galli, Giulia Nature, Vol. 436, Issue 7047 https://doi.org/10.1038/436032a	journal	July 2005
Doping semiconductor nanocrystals Erwin, Steven C.; Zu, Lijun; Haftel, Michael I. Nature, Vol. 436, Issue 7047 https://doi.org/10.1038/nature03832	journal	July 2005
Exploring the doping effects of Ag in p-type PbSe compounds with enhanced thermoelectric performance Wang, Shanyu; Zheng, Gang; Luo, Tingting Journal of Physics D: Applied Physics, Vol. 44, Issue 47 https://doi.org/10.1088/0022-3727/44/47/475304	journal	November 2011
Chemistry of Doped Colloidal Nanocrystals Buonsanti, Raffaella; Milliron, Delia J. Chemistry of Materials, Vol. 25, Issue 8 https://doi.org/10.1021/cm304104m	journal	March 2013
Heavily Doped Semiconductor Nanocrystal Quantum Dots Mocatta, D.; Cohen, G.; Schattner, J. Science, Vol. 332, Issue 6025 https://doi.org/10.1126/science.1196321	journal	March 2011
Electronic Impurity Doping in CdSe Nanocrystals Sahu, Ayaskanta; Kang, Moon Sung; Kompch, Alexander Nano Letters, Vol. 12, Issue 5 https://doi.org/10.1021/nl300880g	journal	April 2012
Influence of Silver Doping on Electron Transport in Thin Films of PbSe Nanocrystals Kang, Moon Sung; Sahu, Ayaskanta; Frisbie, C. Daniel Advanced Materials, Vol. 25, Issue 5 https://doi.org/10.1002/adma.201203114	journal	November 2012
Heterovalent cation substitutional doping for quantum dot homojunction solar cells Stavrinadis, Alexandros; Rath, Arup K.; de Arquer, F. Pelayo García Nature Communications, Vol. 4, Issue 1 https://doi.org/10.1038/ncomms3981	journal	December 2013
Aliovalent Doping in Colloidal Quantum Dots and Its Manifestation on Their Optical Properties: Surface Attachment versus Structural Incorporation Stavrinadis, Alexandros; Pelli Cresi, Jacopo S.; d’Acapito, Francesco Chemistry of Materials, Vol. 28, Issue 15 https://doi.org/10.1021/acs.chemmater.6b01445	journal	July 2016
Steric-Hindrance-Driven Shape Transition in PbS Quantum Dots: Understanding Size-Dependent Stability Choi, Hyekyoung; Ko, Jae-Hyeon; Kim, Yong-Hyun Journal of the American Chemical Society, Vol. 135, Issue 14 https://doi.org/10.1021/ja400948t	journal	March 2013
The coordination chemistry of nanocrystal surfaces Owen, Jonathan Science, Vol. 347, Issue 6222 https://doi.org/10.1126/science.1259924	journal	February 2015
Composition and Size-Dependent Extinction Coefficient of Colloidal PbSe Quantum Dots Moreels, Iwan; Lambert, Karel; De Muynck, David Chemistry of Materials, Vol. 19, Issue 25 https://doi.org/10.1021/cm071410q	journal	December 2007
Ligand Exchange and the Stoichiometry of Metal Chalcogenide Nanocrystals: Spectroscopic Observation of Facile Metal-Carboxylate Displacement and Binding Anderson, Nicholas C.; Hendricks, Mark P.; Choi, Joshua J. Journal of the American Chemical Society, Vol. 135, Issue 49, p. 18536-18548 https://doi.org/10.1021/ja4086758	journal	November 2013
Pauli blocking versus electrostatic attenuation of optical transition intensities in charged $PbSe$ quantum dots An, J. M.; Franceschetti, A.; Zunger, Alex Physical Review B, Vol. 76, Issue 16 https://doi.org/10.1103/PhysRevB.76.161310	journal	October 2007
Localized surface plasmon resonances arising from free carriers in doped quantum dots Luther, Joseph M.; Jain, Prashant K.; Ewers, Trevor Nature Materials, Vol. 10, Issue 5, p. 361-366 https://doi.org/10.1038/nmat3004	journal	April 2011
Facile Synthesis of Silver Chalcogenide (Ag ₂ E; E = Se, S, Te) Semiconductor Nanocrystals Sahu, Ayaskanta; Qi, Lejun; Kang, Moon Sung Journal of the American Chemical Society, Vol. 133, Issue 17 https://doi.org/10.1021/ja200012e	journal	May 2011
Quantum confinement in silver selenide semiconductor nanocrystals Sahu, Ayaskanta; Khare, Ankur; Deng, Donna D. Chemical Communications, Vol. 48, Issue 44 https://doi.org/10.1039/c2cc30539a	journal	January 2012
Stoichiometric Control of Lead Chalcogenide Nanocrystal Solids to Enhance Their Electronic and Optoelectronic Device Performance Oh, Soong Ju; Berry, Nathaniel E.; Choi, Ji-Hyuk ACS Nano, Vol. 7, Issue 3 https://doi.org/10.1021/nn3057356	journal	February 2013
Revisiting the Valence and Conduction Band Size Dependence of PbS Quantum Dot Thin Films Miller, Elisa M.; Kroupa, Daniel M.; Zhang, Jianbing ACS Nano, Vol. 10, Issue 3 https://doi.org/10.1021/acsnano.5b06833	journal	February 2016
Electronic Band Structure and Optical Properties of PbTe, PbSe, and PbS Kohn, S. E.; Yu, P. Y.; Petroff, Y. Physical Review B, Vol. 8, Issue 4 https://doi.org/10.1103/PhysRevB.8.1477	journal	August 1973
X‐ray photoelectron spectroscopy studies of Ag photodoping in Se‐Ge amorphous films Zembutsu, S. Applied Physics Letters, Vol. 39, Issue 12 https://doi.org/10.1063/1.92629	journal	December 1981
Preparation of Cd/Pb Chalcogenide Heterostructured Janus Particles via Controllable Cation Exchange Zhang, Jianbing; Chernomordik, Boris D.; Crisp, Ryan W. ACS Nano, Vol. 9, Issue 7 https://doi.org/10.1021/acsnano.5b01859	journal	June 2015
Tuning the Synthesis of Ternary Lead Chalcogenide Quantum Dots by Balancing Precursor Reactivity Smith, Danielle K.; Luther, Joseph M.; Semonin, Octavi E. ACS Nano, Vol. 5, Issue 1 https://doi.org/10.1021/nn102878u	journal	December 2010
Self‐Diffusion of Lead‐210 in Single Crystals of Lead Selenide Seltzer, Martin S.; Wagner, J. Bruce The Journal of Chemical Physics, Vol. 36, Issue 1 https://doi.org/10.1063/1.1732282	journal	January 1962
Control of PbSe Quantum Dot Surface Chemistry and Photophysics Using an Alkylselenide Ligand Hughes, Barbara K.; Ruddy, Daniel A.; Blackburn, Jeffrey L. ACS Nano, Vol. 6, Issue 6 https://doi.org/10.1021/nn301405j	journal	May 2012
From Impurity Doping to Metallic Growth in Diffusion Doping: Properties and Structure of Silver-Doped InAs Nanocrystals Amit, Yorai; Li, Yuanyuan; Frenkel, Anatoly I. ACS Nano, Vol. 9, Issue 11 https://doi.org/10.1021/acsnano.5b03044	journal	October 2015
Electronic structure and transport properties of doped PbSe Peng, Haowei; Song, Jung-Hwan; Kanatzidis, M. G. Physical Review B, Vol. 84, Issue 12 https://doi.org/10.1103/PhysRevB.84.125207	journal	September 2011
Suppression of Auger Processes in Confined Structures Cragg, George E.; Efros, Alexander L. Nano Letters, Vol. 10, Issue 1 https://doi.org/10.1021/nl903592h	journal	January 2010
Origin and control of blinking in quantum dots Efros, Alexander L.; Nesbitt, David J. Nature Nanotechnology, Vol. 11, Issue 8 https://doi.org/10.1038/nnano.2016.140	journal	August 2016
Surface Chemistry of Colloidal PbSe Nanocrystals Moreels, Iwan; Fritzinger, Bernd; Martins, José C. Journal of the American Chemical Society, Vol. 130, Issue 45 https://doi.org/10.1021/ja803994m	journal	November 2008
Absolute Photoluminescence Quantum Yields of IR-26 Dye, PbS, and PbSe Quantum Dots Semonin, Octavi E.; Johnson, Justin C.; Luther, Joseph M. The Journal of Physical Chemistry Letters, Vol. 1, Issue 16 https://doi.org/10.1021/jz100830r	journal	July 2010
Surfactant-assisted growth of CdS thin films for photovoltaic applications Perkins, Craig L.; Hasoon, Falah S. Journal of Vacuum Science & Technology A: Vacuum, Surfaces, and Films, Vol. 24, Issue 3 https://doi.org/10.1116/1.2194929	journal	May 2006
Electronic structure and optical properties of PbS and PbSe quantum dots Kang, Inuk; Wise, Frank W. Journal of the Optical Society of America B, Vol. 14, Issue 7 https://doi.org/10.1364/JOSAB.14.001632	journal	January 1997
Measurement and assignment of the size-dependent optical spectrum in CdSe quantum dots Norris, D. J.; Bawendi, M. G. Physical Review B, Vol. 53, Issue 24 https://doi.org/10.1103/PhysRevB.53.16338	journal	June 1996
Measurement of Electronic States of PbS Nanocrystal Quantum Dots Using Scanning Tunneling Spectroscopy: The Role of Parity Selection Rules in Optical Absorption Diaconescu, Bogdan; Padilha, Lazaro A.; Nagpal, Prashant Physical Review Letters, Vol. 110, Issue 12 https://doi.org/10.1103/PhysRevLett.110.127406	journal	March 2013

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71 CLASSICAL AND QUANTUM MECHANICS
GENERAL PHYSICS
quantum dots
doping
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Title: Synthesis and Spectroscopy of Silver-Doped PbSe Quantum Dots

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