Limits of Carrier Diffusion in n-Type and p-Type CH3NH3PbI3 Perovskite Single Crystals

Octavi E. Semonin, Giselle A. Elbaz, Daniel B. Straus, Trevor D. Hull, Daniel W. Paley, Arend M. Van Der Zande, James C. Hone, Ioannis Kymissis, Cherie R. Kagan, Xavier Roy, Jonathan S. Owen

Research output: Contribution to journalArticle

Abstract

Using a combination of scanning photocurrent microscopy (SPCM) and time-resolved microwave conductivity (TRMC) measurements, we monitor the diffusion and recombination of photoexcited charges in CH3NH3PbI3 perovskite single crystals. The majority carrier type was controlled by growing crystals in the presence or absence of air, allowing the diffusion lengths of electrons (LD e-) and holes (LD h+) to be directly imaged with SPCM (LD e- = 10-28 μm, LD h+ = 27-65 μm). TRMC measurements reveal a photogenerated carrier mobility (μh + μe) of 115 ± 15 cm2 V-1 s-1 and recombination that depends on the excitation intensity. From the intensity dependence of the recombination kinetics and by accounting for carrier diffusion away from the point of photogeneration, we extract a second-order recombination rate constant (krad = 5 ± 3 × 10-10 cm3/s) that is consistent with the predicted radiative rate. First-order recombination at low photoexcited carrier density (knr p-type = 1.0 ± 0.3 × 105 s-1, knr n-type = 1.5 ± 0.3 × 105 s-1) is slower than that observed in CH3NH3PbI3 thin films or in GaAs single crystals with AlGaAs passivation layers. By accounting for the dilution of photogenerated carriers upon diffusion, and by combining SPCM and TRMC measurements, we resolve disagreement between previous reports of carrier diffusion length.

Original languageEnglish (US)
Pages (from-to)3510-3518
Number of pages9
JournalJournal of Physical Chemistry Letters
Volume7
Issue number17
DOIs
StatePublished - Sep 1 2016

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Perovskite
photocurrents
Single crystals
diffusion length
microscopy
microwaves
conductivity
Photocurrents
scanning
single crystals
Microscopic examination
Microwaves
Scanning
majority carriers
carrier mobility
passivity
aluminum gallium arsenides
dilution
Carrier mobility
Crystal growth

ASJC Scopus subject areas

  • Materials Science(all)
  • Physical and Theoretical Chemistry

Cite this

Limits of Carrier Diffusion in n-Type and p-Type CH3NH3PbI3 Perovskite Single Crystals. / Semonin, Octavi E.; Elbaz, Giselle A.; Straus, Daniel B.; Hull, Trevor D.; Paley, Daniel W.; Van Der Zande, Arend M.; Hone, James C.; Kymissis, Ioannis; Kagan, Cherie R.; Roy, Xavier; Owen, Jonathan S.

In: Journal of Physical Chemistry Letters, Vol. 7, No. 17, 01.09.2016, p. 3510-3518.

Research output: Contribution to journalArticle

Semonin, OE, Elbaz, GA, Straus, DB, Hull, TD, Paley, DW, Van Der Zande, AM, Hone, JC, Kymissis, I, Kagan, CR, Roy, X & Owen, JS 2016, 'Limits of Carrier Diffusion in n-Type and p-Type CH3NH3PbI3 Perovskite Single Crystals', Journal of Physical Chemistry Letters, vol. 7, no. 17, pp. 3510-3518. https://doi.org/10.1021/acs.jpclett.6b01308
Semonin, Octavi E. ; Elbaz, Giselle A. ; Straus, Daniel B. ; Hull, Trevor D. ; Paley, Daniel W. ; Van Der Zande, Arend M. ; Hone, James C. ; Kymissis, Ioannis ; Kagan, Cherie R. ; Roy, Xavier ; Owen, Jonathan S. / Limits of Carrier Diffusion in n-Type and p-Type CH3NH3PbI3 Perovskite Single Crystals. In: Journal of Physical Chemistry Letters. 2016 ; Vol. 7, No. 17. pp. 3510-3518.
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AU - Hull, Trevor D.

AU - Paley, Daniel W.

AU - Van Der Zande, Arend M.

AU - Hone, James C.

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AU - Roy, Xavier

AU - Owen, Jonathan S.

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AB - Using a combination of scanning photocurrent microscopy (SPCM) and time-resolved microwave conductivity (TRMC) measurements, we monitor the diffusion and recombination of photoexcited charges in CH3NH3PbI3 perovskite single crystals. The majority carrier type was controlled by growing crystals in the presence or absence of air, allowing the diffusion lengths of electrons (LD e-) and holes (LD h+) to be directly imaged with SPCM (LD e- = 10-28 μm, LD h+ = 27-65 μm). TRMC measurements reveal a photogenerated carrier mobility (μh + μe) of 115 ± 15 cm2 V-1 s-1 and recombination that depends on the excitation intensity. From the intensity dependence of the recombination kinetics and by accounting for carrier diffusion away from the point of photogeneration, we extract a second-order recombination rate constant (krad = 5 ± 3 × 10-10 cm3/s) that is consistent with the predicted radiative rate. First-order recombination at low photoexcited carrier density (knr p-type = 1.0 ± 0.3 × 105 s-1, knr n-type = 1.5 ± 0.3 × 105 s-1) is slower than that observed in CH3NH3PbI3 thin films or in GaAs single crystals with AlGaAs passivation layers. By accounting for the dilution of photogenerated carriers upon diffusion, and by combining SPCM and TRMC measurements, we resolve disagreement between previous reports of carrier diffusion length.

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