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Title: Intragrain charge transport in kesterite thin films—Limits arising from carrier localization

Abstract

Intragrain charge carrier mobilities measured by time-resolved terahertz spectroscopy in state of the art Cu 2ZnSn(S,Se) 4 kesterite thin films are found to increase from 32 to 140 cm 2V -1s -1 with increasing Se content. The mobilities are limited by carrier localization on the nanometer-scale, which takes place within the first 2 ps after carrier excitation. The localization strength obtained from the Drude-Smith model is found to be independent of the excited photocarrier density. This is in accordance with bandgap fluctuations as a cause of the localized transport. Lastly, charge carrier localization is a general issue in the probed kesterite thin films, which were deposited by coevaporation, colloidal inks, and sputtering followed by annealing with varying Se/S contents and yield 4.9%-10.0% efficiency in the completed device.

Authors:
 [1];  [2];  [3];  [4];  [4];  [4];  [5];  [5]; ORCiD logo [6];  [2]
  1. Helmholtz-Zentrum Berlin (HZB), (Germany). German Research Centre for Materials and Energy, Dept. of Structure and Dynamics of Energy Materials
  2. Helmholtz-Zentrum Berlin (HZB), (Germany). German Research Centre for Materials and Energy, Dept. of Structure and Dynamics of Energy Materials
  3. National Renewable Energy Lab. (NREL), Golden, CO (United States)
  4. Inst. Minoru de Recherche Avancee (IMRA), Sophia Antipolis, Cedex (France)
  5. Humboldt Univ. of Berlin (Germany)
  6. Helmholtz-Zentrum Berlin (HZB), (Germany). German Research Centre for Materials and Energy, Inst. for Solar Fuels
Publication Date:
Research Org.:
National Renewable Energy Lab. (NREL), Golden, CO (United States)
Sponsoring Org.:
USDOE Office of Energy Efficiency and Renewable Energy (EERE)
OSTI Identifier:
1334597
Report Number(s):
NREL/JA-5J00-67507
Journal ID: ISSN 0021-8979; JAPIAU
Grant/Contract Number:  
AC36-08GO28308
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Applied Physics
Additional Journal Information:
Journal Volume: 120; Journal Issue: 17; Journal ID: ISSN 0021-8979
Publisher:
American Institute of Physics (AIP)
Country of Publication:
United States
Language:
English
Subject:
14 SOLAR ENERGY; 71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSICS; band gap; grain boundaries; hole mobility; hall mobility; solar cells

Citation Formats

Hempel, Hannes, Redinger, Alex, Repins, Ingrid, Moisan, Camille, Larramona, Gerardo, Dennler, Gilles, Handwerg, Martin, Fischer, Saskia F., Eichberger, Rainer, and Unold, Thomas. Intragrain charge transport in kesterite thin films—Limits arising from carrier localization. United States: N. p., 2016. Web. doi:10.1063/1.4965868.
Hempel, Hannes, Redinger, Alex, Repins, Ingrid, Moisan, Camille, Larramona, Gerardo, Dennler, Gilles, Handwerg, Martin, Fischer, Saskia F., Eichberger, Rainer, & Unold, Thomas. Intragrain charge transport in kesterite thin films—Limits arising from carrier localization. United States. doi:10.1063/1.4965868.
Hempel, Hannes, Redinger, Alex, Repins, Ingrid, Moisan, Camille, Larramona, Gerardo, Dennler, Gilles, Handwerg, Martin, Fischer, Saskia F., Eichberger, Rainer, and Unold, Thomas. Thu . "Intragrain charge transport in kesterite thin films—Limits arising from carrier localization". United States. doi:10.1063/1.4965868. https://www.osti.gov/servlets/purl/1334597.
@article{osti_1334597,
title = {Intragrain charge transport in kesterite thin films—Limits arising from carrier localization},
author = {Hempel, Hannes and Redinger, Alex and Repins, Ingrid and Moisan, Camille and Larramona, Gerardo and Dennler, Gilles and Handwerg, Martin and Fischer, Saskia F. and Eichberger, Rainer and Unold, Thomas},
abstractNote = {Intragrain charge carrier mobilities measured by time-resolved terahertz spectroscopy in state of the art Cu2ZnSn(S,Se)4 kesterite thin films are found to increase from 32 to 140 cm2V-1s-1 with increasing Se content. The mobilities are limited by carrier localization on the nanometer-scale, which takes place within the first 2 ps after carrier excitation. The localization strength obtained from the Drude-Smith model is found to be independent of the excited photocarrier density. This is in accordance with bandgap fluctuations as a cause of the localized transport. Lastly, charge carrier localization is a general issue in the probed kesterite thin films, which were deposited by coevaporation, colloidal inks, and sputtering followed by annealing with varying Se/S contents and yield 4.9%-10.0% efficiency in the completed device.},
doi = {10.1063/1.4965868},
journal = {Journal of Applied Physics},
number = 17,
volume = 120,
place = {United States},
year = {2016},
month = {11}
}

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Works referenced in this record:

A low-temperature order-disorder transition in Cu 2 ZnSnS 4 thin films
journal, January 2014

  • Scragg, Jonathan J. S.; Choubrac, Léo; Lafond, Alain
  • Applied Physics Letters, Vol. 104, Issue 4
  • DOI: 10.1063/1.4863685

Effects of deposition termination on Cu2ZnSnSe4 device characteristics
journal, May 2015


8.6% Efficient CZTSSe Solar Cells Sprayed from Water–Ethanol CZTS Colloidal Solutions
journal, October 2014

  • Larramona, Gerardo; Bourdais, Stéphane; Jacob, Alain
  • The Journal of Physical Chemistry Letters, Vol. 5, Issue 21
  • DOI: 10.1021/jz501864a

Generalized quantum efficiency analysis for non-ideal solar cells: Case of Cu 2 ZnSnSe 4
journal, January 2016

  • Hages, Charles J.; Carter, Nathaniel J.; Agrawal, Rakesh
  • Journal of Applied Physics, Vol. 119, Issue 1
  • DOI: 10.1063/1.4939487

Deep Defects in Cu 2 ZnSn ( S , Se ) 4 Solar Cells with Varying Se Content
journal, February 2016


Pulsed laser deposition of quaternary Cu 2 ZnSnSe 4 thin films
journal, October 2007

  • Adhi Wibowo, Rachmat; Soo Lee, Eun; Munir, Badrul
  • physica status solidi (a), Vol. 204, Issue 10
  • DOI: 10.1002/pssa.200723144

Minority carrier diffusion length extraction in Cu 2 ZnSn(Se,S) 4 solar cells
journal, September 2013

  • Gokmen, Tayfun; Gunawan, Oki; Mitzi, David B.
  • Journal of Applied Physics, Vol. 114, Issue 11
  • DOI: 10.1063/1.4821841

Electronic and optical properties of Cu2ZnSnS4 and Cu2ZnSnSe4
journal, March 2010


Carrier dynamics in semiconductors studied with time-resolved terahertz spectroscopy
journal, June 2011


Cu-Zn disorder and band gap fluctuations in Cu 2 ZnSn(S,Se) 4 : Theoretical and experimental investigations : Cu-Zn disorder and band gap fluctuations in Cu
journal, September 2015

  • Scragg, Jonathan J. S.; Larsen, Jes K.; Kumar, Mukesh
  • physica status solidi (b), Vol. 253, Issue 2
  • DOI: 10.1002/pssb.201552530

Cu2ZnSnS4 thin film solar cells by fast coevaporation
journal, December 2010

  • Schubert, Björn-Arvid; Marsen, Björn; Cinque, Sonja
  • Progress in Photovoltaics: Research and Applications, Vol. 19, Issue 1
  • DOI: 10.1002/pip.976

The crystal structure of kesterite type compounds: A neutron and X-ray diffraction study
journal, June 2011


Transient photoconductivity in GaAs as measured by time-resolved terahertz spectroscopy
journal, December 2000

  • Beard, Matthew C.; Turner, Gordon M.; Schmuttenmaer, Charles A.
  • Physical Review B, Vol. 62, Issue 23
  • DOI: 10.1103/PhysRevB.62.15764

Luminescence of Cu 2 ZnSnS 4 polycrystals described by the fluctuating potential model
journal, June 2013

  • Halliday, D. P.; Claridge, R.; Goodman, M. C. J.
  • Journal of Applied Physics, Vol. 113, Issue 22
  • DOI: 10.1063/1.4810846

Propagation of terahertz pulses in photoexcited media: Analytical theory for layered systems
journal, July 2007

  • Kužel, P.; Kadlec, F.; Němec, H.
  • The Journal of Chemical Physics, Vol. 127, Issue 2
  • DOI: 10.1063/1.2748402

Universality of ac conduction in disordered solids
journal, July 2000


Fine-Tuning the Sn Content in CZTSSe Thin Films to Achieve 10.8% Solar Cell Efficiency from Spray-Deposited Water-Ethanol-Based Colloidal Inks
journal, October 2015

  • Larramona, Gerardo; Levcenko, Sergiu; Bourdais, Stéphane
  • Advanced Energy Materials, Vol. 5, Issue 24
  • DOI: 10.1002/aenm.201501404

Exploring Dynamics in the Far-Infrared with Terahertz Spectroscopy
journal, April 2004

  • Schmuttenmaer, Charles A.
  • Chemical Reviews, Vol. 104, Issue 4
  • DOI: 10.1021/cr020685g

Effects of sodium on electrical properties in Cu 2 ZnSnS 4 single crystal
journal, April 2014

  • Nagaoka, Akira; Miyake, Hideto; Taniyama, Tomoyasu
  • Applied Physics Letters, Vol. 104, Issue 15
  • DOI: 10.1063/1.4871208

Cation ratio fluctuations in Cu 2 ZnSnS 4 at the 20 nm length scale investigated by analytical electron microscopy : Cation ratio fluctuations in Cu
journal, April 2016

  • Aguiar, Jeffery A.; Erkan, Mehmet E.; Pruzan, Dennis S.
  • physica status solidi (a), Vol. 213, Issue 9
  • DOI: 10.1002/pssa.201600060

Dielectric function spectra and critical-point energies of Cu 2 ZnSnSe 4 from 0.5 to 9.0 eV
journal, February 2012

  • Choi, S. G.; Zhao, H. Y.; Persson, C.
  • Journal of Applied Physics, Vol. 111, Issue 3
  • DOI: 10.1063/1.3681814

A Review of the Terahertz Conductivity of Bulk and Nano-Materials
journal, May 2012

  • Lloyd-Hughes, James; Jeon, Tae-In
  • Journal of Infrared, Millimeter, and Terahertz Waves, Vol. 33, Issue 9
  • DOI: 10.1007/s10762-012-9905-y

High Efficiency Cu 2 ZnSn(S,Se) 4 Solar Cells by Applying a Double In 2 S 3 /CdS Emitter
journal, August 2014

  • Kim, Jeehwan; Hiroi, Homare; Todorov, Teodor K.
  • Advanced Materials, Vol. 26, Issue 44
  • DOI: 10.1002/adma.201402373

Comparison between multiple trapping and multiple hopping transport in a random medium
journal, September 1996


Intrinsic femtosecond charge generation dynamics in single crystal CH 3 NH 3 PbI 3
journal, January 2015

  • Valverde-Chávez, David A.; Ponseca, Carlito S.; Stoumpos, Constantinos C.
  • Energy & Environmental Science, Vol. 8, Issue 12
  • DOI: 10.1039/C5EE02503F

Correlation between intrinsic defects and electrical properties in the high-quality Cu 2 ZnSnS 4 single crystal
journal, September 2013

  • Nagaoka, Akira; Miyake, Hideto; Taniyama, Tomoyasu
  • Applied Physics Letters, Vol. 103, Issue 11
  • DOI: 10.1063/1.4821279

Determination of secondary phases in kesterite Cu 2 ZnSnS 4 thin films by x-ray absorption near edge structure analysis
journal, December 2011

  • Just, Justus; Lützenkirchen-Hecht, Dirk; Frahm, Ronald
  • Applied Physics Letters, Vol. 99, Issue 26
  • DOI: 10.1063/1.3671994

Growth of Cu2ZnSnSe4 single crystals from Sn solutions
journal, September 2012


Classical generalization of the Drude formula for the optical conductivity
journal, September 2001


Direct observation of Cu, Zn cation disorder in Cu 2 ZnSnS 4 solar cell absorber material using aberration corrected scanning transmission electron microscopy : Aberration corrected STEM in Cu, Zn cation disorder in CZTS
journal, September 2012

  • Mendis, Budhika G.; Shannon, Mervyn D.; Goodman, Max CJ
  • Progress in Photovoltaics: Research and Applications, Vol. 22, Issue 1
  • DOI: 10.1002/pip.2279

Employing time-resolved terahertz spectroscopy to analyze carrier dynamics in thin-film Cu2ZnSn(S,Se)4 absorber layers
journal, June 2014

  • Guglietta, Glenn W.; Choudhury, Kaushik Roy; Caspar, Jonathan V.
  • Applied Physics Letters, Vol. 104, Issue 25
  • DOI: 10.1063/1.4884817

Terahertz spectroscopy and imaging - Modern techniques and applications
journal, October 2010

  • Jepsen, P. U.; Cooke, D. G.; Koch, M.
  • Laser & Photonics Reviews, Vol. 5, Issue 1
  • DOI: 10.1002/lpor.201000011

Charge transport in nanostructured materials for solar energy conversion studied by time-resolved terahertz spectroscopy
journal, September 2010

  • Němec, Hynek; Kužel, Petr; Sundström, Villy
  • Journal of Photochemistry and Photobiology A: Chemistry, Vol. 215, Issue 2-3
  • DOI: 10.1016/j.jphotochem.2010.08.006

Band tailing and efficiency limitation in kesterite solar cells
journal, September 2013

  • Gokmen, Tayfun; Gunawan, Oki; Todorov, Teodor K.
  • Applied Physics Letters, Vol. 103, Issue 10
  • DOI: 10.1063/1.4820250

Microscopic mobilities and cooling dynamics of photoexcited carriers in polycrystalline CuInSe 2
journal, March 2014