The effect of the magnitude and direction of the dipoles of organic cations on the electronic structure of hybrid halide perovskites

Sudeep Maheshwari, Sameer Patwardhan, George C Schatz, Nicolas Renaud, Ferdinand C. Grozema

Research output: Contribution to journalArticle

Abstract

We present ab initio calculations (DFT and SOC-G0W0) of the optoelectronic properties of different hybrid-halide perovskites, namely X-PbI3 (X = methylamonimum, formamidinium, guanidinium, hydrazinium, and hydroxylammonium). These calculations shed new light on how the substitution of different organic cations in the material influences its optoelectronic properties. Our simulations show a significant modification of the lattice parameter and band gap of the material upon cation substitution. These modifications are not only due to steric effects but also due to electrostatic interactions between the organic and inorganic parts of the material. In addition to this, we demonstrate how the relative orientations of neighboring cations in the material modify the local electrostatic potential of the system and its fundamental band gap. This change in the band gap is accompanied by the formation of localized and spatially separated electronic states. These localized states modify the carrier mobility in the materials and can be a reason for the formation and recombination of the charge carriers in these very promising materials.

Original languageEnglish
Pages (from-to)16564-16572
Number of pages9
JournalPhysical chemistry chemical physics : PCCP
Volume21
Issue number30
DOIs
Publication statusPublished - Aug 14 2019

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perovskites
Electronic structure
halides
Cations
dipoles
electronic structure
cations
substitutes
electrostatics
Energy gap
carrier mobility
Optoelectronic devices
charge carriers
lattice parameters
Substitution reactions
Carrier mobility
Guanidine
Electronic states
Coulomb interactions
Charge carriers

ASJC Scopus subject areas

  • Physics and Astronomy(all)
  • Physical and Theoretical Chemistry

Cite this

The effect of the magnitude and direction of the dipoles of organic cations on the electronic structure of hybrid halide perovskites. / Maheshwari, Sudeep; Patwardhan, Sameer; Schatz, George C; Renaud, Nicolas; Grozema, Ferdinand C.

In: Physical chemistry chemical physics : PCCP, Vol. 21, No. 30, 14.08.2019, p. 16564-16572.

Research output: Contribution to journalArticle

Maheshwari, Sudeep ; Patwardhan, Sameer ; Schatz, George C ; Renaud, Nicolas ; Grozema, Ferdinand C. / The effect of the magnitude and direction of the dipoles of organic cations on the electronic structure of hybrid halide perovskites. In: Physical chemistry chemical physics : PCCP. 2019 ; Vol. 21, No. 30. pp. 16564-16572.
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