Energy band structure of CuInS2 and optical spectra of CuInS2 nanocrystals

Shabaev, A.; Mehl, M. J.; Efros, Al. L.

doi:10.1103/PhysRevB.92.035431

Title: Energy band structure of ${CuInS}_{2}$ and optical spectra of ${CuInS}_{2}$ nanocrystals

Journal Article · Mon Jul 27 00:00:00 EDT 2015 · Physical Review. B, Condensed Matter and Materials Physics

DOI:https://doi.org/10.1103/PhysRevB.92.035431· OSTI ID:1371348

Shabaev, A. ^[1]; Mehl, M. J. ^[2]; Efros, Al. L. ^[2]

George Mason Univ., Fairfax, VA (United States)
Naval Research Lab. (NRL), Washington, DC (United States)

Using first principles calculations we describe the energy band structure of bulk CuInS₂. The energy band parameters for the multiband effective mass approximation that describes the band edges of this semiconductor are obtained by fitting them to the first principles spectra. Within the multiband effective mass approximation we develop a theoretical description for the structure of band-edge levels and optical properties of the CuInS₂ nanocrystals. For the nanocrystals of spherical shape, the optical transitions are weakly allowed between the electron and hole ground states due to the tetragonal symmetry of the crystal lattice, resulting in a large Stokes shift of photoluminescence up to 300 meV in the smallest nanocrystals. In conclusion, this theory of the band-edge optical transitions in CuInS₂ NCs can be applied to spherical NCs made of other chalcopyrite compounds.

View Accepted Manuscript (DOE)

View Accepted Manuscript (Publisher)

Cite

Export

Save

Research Organization:: Energy Frontier Research Centers (EFRC) (United States). Center for Advanced Solar Photophysics (CASP)

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

Grant/Contract Number:: AC52-06NA25396

OSTI ID:: 1371348

Alternate ID(s):: OSTI ID: 1203806

Journal Information:: Physical Review. B, Condensed Matter and Materials Physics, Vol. 92, Issue 3; Related Information: CASP partners with Los Alamos National Laboratory (lead); University of California, Irvine; University of Colorado; Colorado School of Mines; George Mason University; Los Alamos National Laboratory; University of Minnesota; National Renewable Energy Laboratory; ISSN 1098-0121

Publisher:: American Physical Society (APS)Copyright Statement

Country of Publication:: United States

Language:: English

Citation Metrics:

Cited by: 66 works

Citation information provided by
Web of Science

References (51)

Ternary I−III−VI Quantum Dots Luminescent in the Red to Near-Infrared Allen, Peter M.; Bawendi, Moungi G. Journal of the American Chemical Society, Vol. 130, Issue 29 https://doi.org/10.1021/ja8036349	journal	July 2008
Generalized Gradient Approximation Made Simple Perdew, John P.; Burke, Kieron; Ernzerhof, Matthias Physical Review Letters, Vol. 77, Issue 18, p. 3865-3868 https://doi.org/10.1103/PhysRevLett.77.3865	journal	October 1996
Stability Assessment on a 3% Bilayer PbS/ZnO Quantum Dot Heterojunction Solar Cell Luther, Joseph M.; Gao, Jianbo; Lloyd, Matthew T. Advanced Materials, Vol. 22, Issue 33, p. 3704-3707 https://doi.org/10.1002/adma.201001148	journal	August 2010
Emergence of colloidal quantum-dot light-emitting technologies Shirasaki, Yasuhiro; Supran, Geoffrey J.; Bawendi, Moungi G. Nature Photonics, Vol. 7, Issue 1 https://doi.org/10.1038/nphoton.2012.328	journal	December 2012
Highly Luminescent, Size- and Shape-Tunable Copper Indium Selenide Based Colloidal Nanocrystals Yarema, Olesya; Bozyigit, Deniz; Rousseau, Ian Chemistry of Materials, Vol. 25, Issue 18 https://doi.org/10.1021/cm402306q	journal	August 2013
Processes for chalcopyrite-based solar cells Lux-Steiner, M. Ch; Ennaoui, A.; Fischer, Ch. -H Thin Solid Films, Vol. 361-362 https://doi.org/10.1016/S0040-6090(99)00826-3	journal	February 2000
Structural, Optical, and Electrical Properties of Self-Assembled Films of PbSe Nanocrystals Treated with 1,2-Ethanedithiol Luther, Joseph M.; Law, Matt; Song, Qing ACS Nano, Vol. 2, Issue 2 https://doi.org/10.1021/nn7003348	journal	January 2008
Landau levels of the C-exciton in CuInSe ₂ studied by magneto-transmission Yakushev, M. V.; Rodina, A. V.; Shuchalin, G. M. Applied Physics Letters, Vol. 105, Issue 14 https://doi.org/10.1063/1.4897995	journal	October 2014
The Electronic Structure of Semiconductor Nanocrystals Efros, Al. L.; Rosen, M. Annual Review of Materials Science, Vol. 30, Issue 1 https://doi.org/10.1146/annurev.matsci.30.1.475	journal	August 2000
Role of mid-gap states in charge transport and photoconductivity in semiconductor nanocrystal films Nagpal, Prashant; Klimov, Victor I. Nature Communications, Vol. 2, Issue 1 https://doi.org/10.1038/ncomms1492	journal	September 2011
Direct Observation of Cu $d$ Levels in I-III- ${VI}_{2}$ Compounds Shay, J. L.; Kasper, H. M. Physical Review Letters, Vol. 29, Issue 17 https://doi.org/10.1103/PhysRevLett.29.1162	journal	October 1972
Quantum Theory of Cyclotron Resonance in Semiconductors: General Theory Luttinger, J. M. Physical Review, Vol. 102, Issue 4 https://doi.org/10.1103/PhysRev.102.1030	journal	May 1956
Efficient Synthesis of Highly Luminescent Copper Indium Sulfide-Based Core/Shell Nanocrystals with Surprisingly Long-Lived Emission Li, Liang; Pandey, Anshu; Werder, Donald J. Journal of the American Chemical Society, Vol. 133, Issue 5, p. 1176-1179 https://doi.org/10.1021/ja108261h	journal	February 2011
Development of CuInSe ₂ Nanocrystal and Nanoring Inks for Low-Cost Solar Cells Guo, Qijie; Kim, Suk Jun; Kar, Mahaprasad Nano Letters, Vol. 8, Issue 9 https://doi.org/10.1021/nl802042g	journal	September 2008
Photoreflectance of CuInS2 single crystal prepared by traveling heater method Shirakata, Sho; Miyake, Hideto Journal of Physics and Chemistry of Solids, Vol. 64, Issue 9-10 https://doi.org/10.1016/S0022-3697(03)00123-9	journal	September 2003
Angular Momentum Theory and Localized States in Solids. Investigation of Shallow Acceptor States in Semiconductors Lipari, Nunzio O.; Baldereschi, A. Physical Review Letters, Vol. 25, Issue 24 https://doi.org/10.1103/PhysRevLett.25.1660	journal	December 1970
Tuning the Luminescence Properties of Colloidal I–III–VI Semiconductor Nanocrystals for Optoelectronics and Biotechnology Applications Zhong, Haizheng; Bai, Zelong; Zou, Bingsuo The Journal of Physical Chemistry Letters, Vol. 3, Issue 21, p. 3167-3175 https://doi.org/10.1021/jz301345x	journal	October 2012
Ternary and quaternary metal chalcogenide nanocrystals: synthesis, properties and applications Aldakov, Dmitry; Lefrançois, Aurélie; Reiss, Peter Journal of Materials Chemistry C, Vol. 1, Issue 24 https://doi.org/10.1039/c3tc30273c	journal	January 2013
$p - d$ Hybridization of the Valence Bands of I-III- ${VI}_{2}$ Compounds Shay, J. L.; Tell, B.; Kasper, H. M. Physical Review B, Vol. 5, Issue 12 https://doi.org/10.1103/PhysRevB.5.5003	journal	June 1972
Efficient CuInSe ₂ /CdS solar cells Shay, J. L.; Wagner, Sigurd; Kasper, H. M. Applied Physics Letters, Vol. 27, Issue 2 https://doi.org/10.1063/1.88372	journal	July 1975
Band structure of ${CdGeAs}_{2}$ near the fundamental gap Limpijumnong, Sukit; Lambrecht, Walter R. L. Physical Review B, Vol. 65, Issue 16 https://doi.org/10.1103/PhysRevB.65.165204	journal	April 2002
Self-Consistent Equations Including Exchange and Correlation Effects Kohn, W.; Sham, L. J. Physical Review, Vol. 140, Issue 4A, p. A1133-A1138 https://doi.org/10.1103/PhysRev.140.A1133	journal	November 1965
Excited states of the A free exciton in CuInS2 Yakushev, M. V.; Martin, R. W.; Mudryi, A. V. Applied Physics Letters, Vol. 92, Issue 11 https://doi.org/10.1063/1.2896301	journal	March 2008
Simple yet Versatile Synthesis of CuInSe _x S _{2– x} Quantum Dots for Sunlight Harvesting McDaniel, Hunter; Koposov, Alexey Y.; Draguta, Sergiu The Journal of Physical Chemistry C, Vol. 118, Issue 30 https://doi.org/10.1021/jp5004903	journal	May 2014
Diamagnetic shifts of free excitons in CuInS2 in magnetic fields Yakushev, M. V.; Martin, R. W.; Mudryi, A. V. Applied Physics Letters, Vol. 94, Issue 4 https://doi.org/10.1063/1.3077022	journal	January 2009
Anisotropy of effective masses in CuInSe ₂ Yakushev, M. V.; Luckert, F.; Rodina, A. V. Applied Physics Letters, Vol. 101, Issue 26 https://doi.org/10.1063/1.4773480	journal	December 2012
Materials Availability Expands the Opportunity for Large-Scale Photovoltaics Deployment Wadia, Cyrus; Alivisatos, A. Paul; Kammen, Daniel M. Environmental Science & Technology, Vol. 43, Issue 6 https://doi.org/10.1021/es8019534	journal	March 2009
Electronic structure of the ternary chalcopyrite semiconductors CuAl $S_{2}$ , CuGa $S_{2}$ , CuIn $S_{2}$ , CuAl ${Se}_{2}$ , CuGa ${Se}_{2}$ , and CuIn ${Se}_{2}$ Jaffe, J. E.; Zunger, Alex Physical Review B, Vol. 28, Issue 10 https://doi.org/10.1103/PhysRevB.28.5822	journal	November 1983
PbSe Quantum Dot Solar Cells with More than 6% Efficiency Fabricated in Ambient Atmosphere Zhang, Jianbing; Gao, Jianbo; Church, Carena P. Nano Letters, Vol. 14, Issue 10 https://doi.org/10.1021/nl503085v	journal	September 2014
New world record efficiency for Cu(In,Ga)Se2 thin-film solar cells beyond 20% Jackson, Philip; Hariskos, Dimitrios; Lotter, Erwin Progress in Photovoltaics: Research and Applications, Vol. 19, Issue 7 https://doi.org/10.1002/pip.1078	journal	January 2011
Influence of the exchange screening parameter on the performance of screened hybrid functionals Krukau, Aliaksandr V.; Vydrov, Oleg A.; Izmaylov, Artur F. The Journal of Chemical Physics, Vol. 125, Issue 22 https://doi.org/10.1063/1.2404663	journal	December 2006
Ab initio molecular dynamics for open-shell transition metals Kresse, G.; Hafner, J. Physical Review B, Vol. 48, Issue 17 https://doi.org/10.1103/PhysRevB.48.13115	journal	November 1993
Electron and hole conductivity in CuInS2 Look, D. C.; Manthuruthil, J. C. Journal of Physics and Chemistry of Solids, Vol. 37, Issue 2 https://doi.org/10.1016/0022-3697(76)90157-8	journal	January 1976
Highly efficient Cu(In,Ga)Se2 solar cells grown on flexible polymer films Chirilă, Adrian; Buecheler, Stephan; Pianezzi, Fabian Nature Materials, Vol. 10, Issue 11 https://doi.org/10.1038/nmat3122	journal	September 2011
Ab initio molecular-dynamics simulation of the liquid-metal–amorphous-semiconductor transition in germanium Kresse, G.; Hafner, J. Physical Review B, Vol. 49, Issue 20, p. 14251-14269 https://doi.org/10.1103/PhysRevB.49.14251	journal	May 1994
n-Type Transition Metal Oxide as a Hole Extraction Layer in PbS Quantum Dot Solar Cells Gao, Jianbo; Perkins, Craig L.; Luther, Joseph M. Nano Letters, Vol. 11, Issue 8, p. 3263-3266 https://doi.org/10.1021/nl2015729	journal	August 2011
Synthesis of CuInS ₂ , CuInSe ₂ , and Cu(In _x Ga _{1- x} )Se ₂ (CIGS) Nanocrystal “Inks” for Printable Photovoltaics Panthani, Matthew G.; Akhavan, Vahid; Goodfellow, Brian Journal of the American Chemical Society, Vol. 130, Issue 49 https://doi.org/10.1021/ja805845q	journal	December 2008
Energy of excitons in CuInS2 single crystals Yakushev, M. V.; Mudryi, A. V.; Victorov, I. V. Applied Physics Letters, Vol. 88, Issue 1 https://doi.org/10.1063/1.2152114	journal	January 2006
Inhomogeneous Electron Gas Hohenberg, P.; Kohn, W. Physical Review, Vol. 136, Issue 3B, p. B864-B871 https://doi.org/10.1103/PhysRev.136.B864	journal	November 1964
Electrical Properties, Optical Properties, and Band Structure of CuGa $S_{2}$ and CuIn $S_{2}$ Tell, B.; Shay, J. L.; Kasper, H. M. Physical Review B, Vol. 4, Issue 8 https://doi.org/10.1103/PhysRevB.4.2463	journal	October 1971
Efficient Spray-Coated Colloidal Quantum Dot Solar Cells Kramer, Illan J.; Minor, James C.; Moreno-Bautista, Gabriel Advanced Materials, Vol. 27, Issue 1 https://doi.org/10.1002/adma.201403281	journal	November 2014
Improved performance and stability in quantum dot solar cells through band alignment engineering Chuang, Chia-Hao M.; Brown, Patrick R.; Bulović, Vladimir Nature Materials, Vol. 13, Issue 8, p. 796-801 https://doi.org/10.1038/nmat3984	journal	May 2014
Luminescence of CuInS2 Binsma, J. J. M.; Giling, L. J.; Bloem, J. Journal of Luminescence, Vol. 27, Issue 1 https://doi.org/10.1016/0022-2313(82)90029-1	journal	June 1982
Theory of the band-gap anomaly in $AB C_{2}$ chalcopyrite semiconductors Jaffe, J. E.; Zunger, Alex Physical Review B, Vol. 29, Issue 4 https://doi.org/10.1103/PhysRevB.29.1882	journal	February 1984
An integrated approach to realizing high-performance liquid-junction quantum dot sensitized solar cells McDaniel, Hunter; Fuke, Nobuhiro; Makarov, Nikolay S. Nature Communications, Vol. 4, Issue 1 https://doi.org/10.1038/ncomms3887	journal	December 2013
Absorption and intensity-dependent photoluminescence measurements on CdSe quantum dots: assignment of the first electronic transitions Ekimov, A. I.; Kudryavtsev, I. A.; Efros, Al. L. Journal of the Optical Society of America B, Vol. 10, Issue 1 https://doi.org/10.1364/JOSAB.10.000100	journal	January 1993
Engineered CuInSe _x S _{2– x} Quantum Dots for Sensitized Solar Cells McDaniel, Hunter; Fuke, Nobuhiro; Pietryga, Jeffrey M. The Journal of Physical Chemistry Letters, Vol. 4, Issue 3 https://doi.org/10.1021/jz302067r	journal	January 2013
Exciton binding energies in chalcopyrite semiconductors Gil, Bernard; Felbacq, Didier; Chichibu, Shigefusa F. Physical Review B, Vol. 85, Issue 7 https://doi.org/10.1103/PhysRevB.85.075205	journal	February 2012
ESR and x-ray analysis of the ternary semiconductors CuAlS2, CuInS2 and AgGaS2 Brandt, G.; Räuber, A.; Schneider, J. Solid State Communications, Vol. 12, Issue 6 https://doi.org/10.1016/0038-1098(73)90638-8	journal	March 1973
Electron and hole conductivity in CuInS2 Look, D. C.; Manthuruthil, J. C. Solid State Communications, Vol. 17, Issue 7 https://doi.org/10.1016/0038-1098(75)90766-8	journal	October 1975
An ultrasensitive molybdenum-based double-heterojunction phototransistor Zenodo https://doi.org/10.5281/zenodo.4835973	text	January 2021

Cited By (7)

Evidence for the Band‐Edge Exciton of CuInS ₂ Nanocrystals Enables Record Efficient Large‐Area Luminescent Solar Concentrators Anand, Abhinav; Zaffalon, Matteo L.; Gariano, Graziella Advanced Functional Materials, Vol. 30, Issue 4 https://doi.org/10.1002/adfm.201906629	journal	November 2019
Near-Infrared, Heavy Metal-Free Colloidal “Giant” Core/Shell Quantum Dots Tong, Xin; Kong, Xiang-Tian; Zhou, Yufeng Advanced Energy Materials, Vol. 8, Issue 2 https://doi.org/10.1002/aenm.201701432	journal	September 2017
Rational Construction of Z‐Scheme CuInS ₂ /Au/g‐C ₃ N ₄ Heterostructure: Experimental Results and Theoretical Calculation Ye, Wenhua; Hu, Jisong; Hu, Xiaofeng ChemCatChem, Vol. 11, Issue 24 https://doi.org/10.1002/cctc.201901227	journal	October 2019
Prospects of Colloidal Copper Chalcogenide Nanocrystals van der Stam, Ward; Berends, Anne C.; de Mello Donega, Celso ChemPhysChem, Vol. 17, Issue 5 https://doi.org/10.1002/cphc.201500976	journal	February 2016
Electronic energy band parameters of $CuInS e_{2}$ : Landau levels in magnetotransmission spectra Yakushev, M. V.; Rodina, A. V.; Seisyan, R. P. Physical Review B, Vol. 100, Issue 23 https://doi.org/10.1103/physrevb.100.235202	journal	December 2019
Investigation of AgInS2/ZnS Quantum Dots by Magnetic Circular Dichroism Spectroscopy Gromova, Yulia; Sokolova, Anastasiia; Kurshanov, Danil Materials, Vol. 12, Issue 21 https://doi.org/10.3390/ma12213616	journal	November 2019
Prospects of Colloidal Copper Chalcogenide Nanocrystals van der Stam, Ward; Berends, Anne C.; de Mello Donega, Celso ChemPhysChem, Vol. 17, Issue 5 https://doi.org/10.1002/cphc.201600094	journal	February 2016

Similar Records

Evidence for the Band-Edge Exciton of CuInS₂ Nanocrystals Enables Record Efficient Large-Area Luminescent Solar Concentrators

Journal Article · Fri Nov 15 00:00:00 EST 2019 · Advanced Functional Materials · OSTI ID:1371348

Anand, Abhinav; Zaffalon, Matteo L.; Gariano, Graziella; +10 more

Synthesis and characteristics of spray deposited CuInS{sub 2} nanocrystals thin films for photovoltaic applications

Journal Article · Tue Oct 15 00:00:00 EDT 2013 · Materials Research Bulletin · OSTI ID:1371348

Kumar, Sushil; AlSalhi, Mohamad S.

Intrinsic and Extrinsic Exciton Recombination Pathways in AgInS ₂ Colloidal Nanocrystals

Journal Article · Mon Apr 05 00:00:00 EDT 2021 · Energy Material Advances · OSTI ID:1371348

Zaffalon, Matteo L.; Pinchetti, Valerio; Camellini, Andrea; +10 more

Related Subjects

36 MATERIALS SCIENCE
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)

Title: Energy band structure of CuInS 2 and optical spectra of CuInS 2 nanocrystals

Citation Formats

References (51)

Cited By (7)

Similar Records

Related Subjects

Title: Energy band structure of ${CuInS}_{2}$ and optical spectra of ${CuInS}_{2}$ nanocrystals