Impact of Organic Spacers on the Carrier Dynamics in 2D Hybrid Lead-Halide Perovskites

Shou Feng Zhang, Xian Kai Chen, Ai Min Ren, Hong Li, Jean Luc Bredas

Research output: Contribution to journalArticlepeer-review

42 Scopus citations


We have carried out nonadiabatic molecular dynamics simulations combined with time-dependent density functional theory calculations to compare the properties of the two-dimensional (2D) (BA)2(MA)Pb2I7 and three-dimensional (3D) MAPbI3 (where MA = methylammonium and BA = butylammonium) materials. We evaluate the different impacts that the 2D-confined spacer layer of butylammonium cations and the 3D-confined methylammonium cations have on the charge carrier dynamics in the two systems. Our results indicate that, while both the MA+ and BA+ cations play important roles in determining the carrier dynamics, the BA+ cations exhibit stronger nonadiabatic couplings with the 2D perovskite framework. The consequence is a faster hot-carrier decay rate in 2D (BA)2(MA)Pb2I7 than in 3D MAPbI3. Thus, tuning of the functional groups of the organic spacer cations in order to reduce the vibronic couplings between the cations and the Pb-I framework can offer the opportunity to slow down the hot-carrier relaxations and increase the carrier lifetimes in 2D lead-halide perovskites.

Original languageEnglish (US)
Pages (from-to)17-25
Number of pages9
JournalACS Energy Letters
Issue number1
StatePublished - Jan 11 2019
Externally publishedYes

ASJC Scopus subject areas

  • Chemistry (miscellaneous)
  • Renewable Energy, Sustainability and the Environment
  • Fuel Technology
  • Energy Engineering and Power Technology
  • Materials Chemistry


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