TY - JOUR
T1 - The effect of the magnitude and direction of the dipoles of organic cations on the electronic structure of hybrid halide perovskites
AU - Maheshwari, Sudeep
AU - Patwardhan, Sameer
AU - Schatz, George C.
AU - Renaud, Nicolas
AU - Grozema, Ferdinand C.
PY - 2019
Y1 - 2019
N2 - 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.
AB - 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.
UR - http://www.scopus.com/inward/record.url?scp=85070789427&partnerID=8YFLogxK
U2 - 10.1039/c9cp02866h
DO - 10.1039/c9cp02866h
M3 - Article
C2 - 31313778
AN - SCOPUS:85070789427
SN - 1463-9076
VL - 21
SP - 16564
EP - 16572
JO - Physical chemistry chemical physics : PCCP
JF - Physical chemistry chemical physics : PCCP
IS - 30
ER -