TY - JOUR
T1 - Theoretical investigation of octahedral tilting and bandgap non-linearity in monolayer Ruddlesden-Popper A2Pb1-xGexI4 perovskites
AU - Javed, Mehreen
AU - Benkraouda, Maamar
AU - Amrane, Noureddine
N1 - Funding Information:
This research was supported under the United Arab Emirates University Program for Advanced Research (UPAR) Grant Number 31R109 under Research Project number ECEER‐9‐2016.
Publisher Copyright:
© 2022 John Wiley & Sons Ltd.
PY - 2022
Y1 - 2022
N2 - 2D Ruddlesden-Popper (RP) perovskites (R-NH3)2An−1BnX3n+1 with tailorable photovoltaic features of low toxicity, reduced dimensionality, and defect tolerance hold promise to overcome the main constraints of perovskite solar cells (PSCs). A systematic investigation of the structural and electronic properties of pure and mixed (R-NH3)2Pb1−xGexI4 systems was performed with and without spin-orbit coupling (SOC), by using density functional theory (DFT). The organic spacer cations (R-NH3+)2 of methylammonium (MA-CH3NH3+) and Phenylethyl ammonium (PEA-C6H5[CH2]2NH3+) with x = 0.0, 0.25, 0.50, 0.75, 1.0, resulted in the compositionally modified 32-permutations by systematically substituting the inorganic cations. Short-range ordering has categorized all studied compositions of (R-NH3)2Pb0.50Ge0.50I4 into column and battenberg schemes depending on the Ge defect site. The competing effects of octahedral tilting and lattice distortion with bandgap bowing and SOC, across Pb-Ge compositional systems, provide a systematic strategy to tune bandgaps. By controlling the cations' composition, these mixed 2D-perovskites outlined the strategy to achieve the desired bandgap and band positions. A rational design approach of low dimensional perovskites was adopted to tune the electronic properties through the spacer and inorganic cation engineering. Our findings expose the scope of monolayer-based systems as an ideal choice of absorber for the bottom sub-cell in all-perovskites 2D-3D tandem solar cell, harvesting light from visible (2.4 eV) up to infrared (1.2 eV) in the solar spectrum with features of defect tolerance, quantum and dielectric confinement, low bandgap, low effective masses, and high mobility.
AB - 2D Ruddlesden-Popper (RP) perovskites (R-NH3)2An−1BnX3n+1 with tailorable photovoltaic features of low toxicity, reduced dimensionality, and defect tolerance hold promise to overcome the main constraints of perovskite solar cells (PSCs). A systematic investigation of the structural and electronic properties of pure and mixed (R-NH3)2Pb1−xGexI4 systems was performed with and without spin-orbit coupling (SOC), by using density functional theory (DFT). The organic spacer cations (R-NH3+)2 of methylammonium (MA-CH3NH3+) and Phenylethyl ammonium (PEA-C6H5[CH2]2NH3+) with x = 0.0, 0.25, 0.50, 0.75, 1.0, resulted in the compositionally modified 32-permutations by systematically substituting the inorganic cations. Short-range ordering has categorized all studied compositions of (R-NH3)2Pb0.50Ge0.50I4 into column and battenberg schemes depending on the Ge defect site. The competing effects of octahedral tilting and lattice distortion with bandgap bowing and SOC, across Pb-Ge compositional systems, provide a systematic strategy to tune bandgaps. By controlling the cations' composition, these mixed 2D-perovskites outlined the strategy to achieve the desired bandgap and band positions. A rational design approach of low dimensional perovskites was adopted to tune the electronic properties through the spacer and inorganic cation engineering. Our findings expose the scope of monolayer-based systems as an ideal choice of absorber for the bottom sub-cell in all-perovskites 2D-3D tandem solar cell, harvesting light from visible (2.4 eV) up to infrared (1.2 eV) in the solar spectrum with features of defect tolerance, quantum and dielectric confinement, low bandgap, low effective masses, and high mobility.
KW - 2D-monolayer perovskites
KW - bandgap non-linearity
KW - defect tolerance
KW - lattice distortion
KW - octahedral tilting
KW - quantum confinement
KW - spin-orbit coupling
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U2 - 10.1002/er.8474
DO - 10.1002/er.8474
M3 - Article
AN - SCOPUS:85135794048
SN - 0363-907X
JO - International Journal of Energy Research
JF - International Journal of Energy Research
ER -