Effect of Water Addition during Preparation on the Early-Time Photodynamics of CH3NH3PbI3 Perovskite Layers

S. Aphrham, Q. Pan, S. F. Zaccarine, K. M. Felter, J. Thieme, Karin van den Nieuwenhuijzen, Johan E. ten Elshof, A. Huijser*

*Corresponding author for this work

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Abstract

The effect of water addition during preparation of a CH3NH3PbI3 layer on the photodynamics is studied by femtosecond transient absorption. Both the regular perovskite and the aqueous analogue show charge thermalisation on a timescale of about 500fs. This process is, however, less pronounced in the latter layer. The spectral feature associated with hot charges does not fully decay on this timescale, but also shows a long-lived (sub-ns) component. As water molecules may interfere with the hydrogen bonding between the CH3NH3 + cations and the inorganic cage, this effect is possibly caused by immobilisation of cation motion, suggesting a key role of CH3NH3 + dipole reorientation in charge thermalisation. This effect shows the possibility of controlling hot charge carrier cooling to overcome the Shockley-Queisser limit.

Original languageEnglish
Pages (from-to)3320-3324
JournalChemPhysChem
Volume18
Issue number23
DOIs
Publication statusPublished - 6 Dec 2017

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Cations
preparation
Water
Charge carriers
water
cations
Hydrogen bonds
Cooling
immobilization
Molecules
retraining
charge carriers
analogs
dipoles
cooling
decay
hydrogen
perovskite
molecules

Keywords

  • Cation immobilisation
  • Hybrid perovskites
  • Photodynamics
  • Transient absorption
  • Water addition

Cite this

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title = "Effect of Water Addition during Preparation on the Early-Time Photodynamics of CH3NH3PbI3 Perovskite Layers",
abstract = "The effect of water addition during preparation of a CH3NH3PbI3 layer on the photodynamics is studied by femtosecond transient absorption. Both the regular perovskite and the aqueous analogue show charge thermalisation on a timescale of about 500fs. This process is, however, less pronounced in the latter layer. The spectral feature associated with hot charges does not fully decay on this timescale, but also shows a long-lived (sub-ns) component. As water molecules may interfere with the hydrogen bonding between the CH3NH3 + cations and the inorganic cage, this effect is possibly caused by immobilisation of cation motion, suggesting a key role of CH3NH3 + dipole reorientation in charge thermalisation. This effect shows the possibility of controlling hot charge carrier cooling to overcome the Shockley-Queisser limit.",
keywords = "Cation immobilisation, Hybrid perovskites, Photodynamics, Transient absorption, Water addition",
author = "S. Aphrham and Q. Pan and Zaccarine, {S. F.} and Felter, {K. M.} and J. Thieme and {van den Nieuwenhuijzen}, Karin and {ten Elshof}, {Johan E.} and A. Huijser",
year = "2017",
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language = "English",
volume = "18",
pages = "3320--3324",
journal = "ChemPhysChem",
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}

Effect of Water Addition during Preparation on the Early-Time Photodynamics of CH3NH3PbI3 Perovskite Layers. / Aphrham, S.; Pan, Q.; Zaccarine, S. F.; Felter, K. M.; Thieme, J.; van den Nieuwenhuijzen, Karin; ten Elshof, Johan E.; Huijser, A.

In: ChemPhysChem, Vol. 18, No. 23, 06.12.2017, p. 3320-3324.

Research output: Contribution to journalArticleAcademicpeer-review

TY - JOUR

T1 - Effect of Water Addition during Preparation on the Early-Time Photodynamics of CH3NH3PbI3 Perovskite Layers

AU - Aphrham, S.

AU - Pan, Q.

AU - Zaccarine, S. F.

AU - Felter, K. M.

AU - Thieme, J.

AU - van den Nieuwenhuijzen, Karin

AU - ten Elshof, Johan E.

AU - Huijser, A.

PY - 2017/12/6

Y1 - 2017/12/6

N2 - The effect of water addition during preparation of a CH3NH3PbI3 layer on the photodynamics is studied by femtosecond transient absorption. Both the regular perovskite and the aqueous analogue show charge thermalisation on a timescale of about 500fs. This process is, however, less pronounced in the latter layer. The spectral feature associated with hot charges does not fully decay on this timescale, but also shows a long-lived (sub-ns) component. As water molecules may interfere with the hydrogen bonding between the CH3NH3 + cations and the inorganic cage, this effect is possibly caused by immobilisation of cation motion, suggesting a key role of CH3NH3 + dipole reorientation in charge thermalisation. This effect shows the possibility of controlling hot charge carrier cooling to overcome the Shockley-Queisser limit.

AB - The effect of water addition during preparation of a CH3NH3PbI3 layer on the photodynamics is studied by femtosecond transient absorption. Both the regular perovskite and the aqueous analogue show charge thermalisation on a timescale of about 500fs. This process is, however, less pronounced in the latter layer. The spectral feature associated with hot charges does not fully decay on this timescale, but also shows a long-lived (sub-ns) component. As water molecules may interfere with the hydrogen bonding between the CH3NH3 + cations and the inorganic cage, this effect is possibly caused by immobilisation of cation motion, suggesting a key role of CH3NH3 + dipole reorientation in charge thermalisation. This effect shows the possibility of controlling hot charge carrier cooling to overcome the Shockley-Queisser limit.

KW - Cation immobilisation

KW - Hybrid perovskites

KW - Photodynamics

KW - Transient absorption

KW - Water addition

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