Symmetry-Based Tight Binding Modeling of Halide Perovskite Semiconductors

Boyer‐Richard, Soline; Katan, Claudine; Traoré, Boubacar; Scholz, Reinhard; Jancu, Jean–Marc; Even, Jacky

doi:10.1021/acs.jpclett.6b01749

Cited by 68 publications

(88 citation statements)

References 58 publications

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“…Spin-orbit coupling (SOC) is also included in the model, which adds two more parameters to the model, namely the SOC strengths for Pb and I. Treating the orbital energies and overlaps as fitting parameters, Boyer-Richard et al obtained system parameters that reproduce the main features in the electronic band structure of MAPbI 3 [21]. It is worth mentioning here that a recent study used a somewhat similar tight-binding model to investigate SOC effects in a different family of halide perovskite materials [22].…”

Section: Tight-binding Modelmentioning

confidence: 99%

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Effect of disorder on transport properties in a tight-binding model for lead halide perovskites

Ashhab

Voznyy

Hoogland

et al. 2017

Sci Rep

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The hybrid organic-inorganic lead halide perovskite materials have emerged as remarkable materials for photovoltaic applications. Their strengths include good electric transport properties in spite of the disorder inherent in them. Motivated by this observation, we analyze the effects of disorder on the energy eigenstates of a tight-binding model of these materials. In particular, we analyze the spatial extension of the energy eigenstates, which is quantified by the inverse participation ratio. This parameter exhibits a tendency, and possibly a phase transition, to localization as the on-site energy disorder strength is increased. However, we argue that the disorder in the lead halide perovskites corresponds to a point in the regime of highly delocalized states. Our results also suggest that the electronic states of mixed-halide materials tend to be more localized than those of pure materials, which suggests a weaker tendency to form extended bonding states in the mixed-halide materials and is therefore not favourable for halide mixing.

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Section: Tight-binding Modelmentioning

confidence: 99%

“…We take the model developed in Ref. [21], including the parameters obtained there, as the starting point for our calculations. This simplification allows us to perform systematic simulations on systems containing 512 unit cells (effectively containing ∼6000 atoms) at a rather low computational cost.…”

Section: Introductionmentioning

confidence: 99%

Effect of disorder on transport properties in a tight-binding model for lead halide perovskites

Ashhab

Voznyy

Hoogland

et al. 2017

Sci Rep

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“…Here, we take a major step in this direction via the formulation and theoretical investigation of a fully microscopic model describing the interplay between electronic structure and nuclear motion Our model aims to simulate very large system sizes and thus begins with a computationally efficient tight-binding (TB) parameterization of the band structure, as previously done, see, e.g., Refs. 26,27 . It includes real-space descriptions of the on-site energies associated with occupancy of the relevant s-and p-orbitals of Pb and I, as well as the kinetic energy arising from  and  overlaps of these orbitals, which determine the hopping parameters in the TB scheme.…”

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confidence: 99%

How Lattice and Charge Fluctuations Control Carrier Dynamics in Halide Perovskites

et al. 2018

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Here we develop a microscopic approach aimed at the description of a suite of physical effects related to carrier transport in, and the optical properties of, halide perovskites. Our theory is based on the description of the nuclear dynamics to all orders and goes beyond the common assumption of linear electron-phonon coupling in describing the carrier dynamics and band gap characteristics.When combined with first-principles calculations and applied to the prototypical MAPbI3 system, our theory explains seemingly disparate experimental findings associated with both the chargecarrier mobility and optical absorption properties, including their temperature dependencies. Our findings demonstrate that orbital overlap fluctuations in the lead-halide structure plays a significant role in determining the optoelectronic features of halide perovskites.

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“…This approximation precludes a study of the Rashba effect, 25,26 arising from the inversion symmetry breaking of the typical orthorhombic structure, 7 although this effect could be straightforwardly included along the lines of Ref. 27. Henceforth, we will focus our attention on the specific case of layered HOIPs made from the popular parent compounds of ammonium or methylammonium (MA) lead iodide using butylammonium spacers, i.e.…”

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confidence: 99%

“…41 The spin-orbit coupling constants are determined to be ∆ Pb SOC = 1.18 eV and ∆ I SOC = 1.06 eV, which are similar to the values used in a previous tight-binding study. 27 Moving on to layered HOIPs, we model the system as a stack of alternating organic and inorganic slabs, each with a uniform dielectric constant as shown in Fig. 1.…”

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confidence: 99%

Optical Properties of Layered Hybrid Organic–Inorganic Halide Perovskites: A Tight-Binding GW-BSE Study

Cho

Berkelbach

2019

J. Phys. Chem. Lett.

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We present a many-body calculation of the band structure and optical spectrum of the layered hybrid organicinorganic halide perovskites in the Ruddlesden-Popper phase with the general formula A 2 A n−1 M n X 3n+1 , focusing specifically on the lead iodide family. We calculate the mean-field band structure with spin-orbit coupling, quasiparticle corrections within the GW approximation, and optical spectra using the Bethe-Salpeter equation. The model is parameterized by first-principles calculations and classical electrostatic screening, enabling an accurate but cost-effective study of large unit cells and corresponding thickness-dependent properties. A transition of the electronic and optical properties from quasi-two-dimensional behavior to three-dimensional behavior is shown for increasing n and the nonhydrogenic character of the excitonic Rydberg series is analyzed. The thickness-dependent 1s and 2s exciton energy levels are in good agreement with recently reported experiments and the 1s exciton binding energy is calculated to be 302 meV for n = 1, 97 meV for n = 5, and 37 meV for n = ∞ (bulk MAPbI 3 ).Hybrid organic-inorganic perovskites (HOIPs) are promising photovoltaic materials, most recently showing a high power conversion efficiency of over 24%. 1 A three dimensional bulk HOIP AMX 3 can be transformed into a layered HOIP in the Ruddlesden-Popper phase A 2 A n−1 M n X 3n+1 by substituting a small organic cation A + by a bulkier one A + .Common choices for the small organic cation are A + =CH 3 NH + 3 , NH + 4 ; for the bulkier cation are A + =C 4 H 9 NH + 3 , C 6 H 5 C 2 H 4 NH + 3 ; for the metal are M 2+ =Sn 2+ , Pb 2+ ; and for the halide are X − =Cl − , I − , Br − . A major drawback of the 3D HOIPs for photovoltaics is their relatively fast degradation when exposed to air, moisture, and light; in contrast, the layered HOIPs are more stable while maintaining high power conversion efficiencies under working conditions. 2,3 The optical properties of layered HOIPs can also be easily controlled by composition, 4 enhancing their flexibility for a variety of optoelectronic applications. Unlike the van der Waals materials -a prototypical family of layered materials including graphene, hexagonal boron nitride, and the transition-metal dichalcogenides -the layered HOIPs have sublayers that are covalently bonded. This distinct property makes the layered HOIPs an insightful mixeddimensional platform for investigating the transition of optoelectronic properties from two dimensional to three dimensional.The n-dependent properties of layered HOIPs have been experimentally investigated, especially during the last five years, 5-9 including mechanically exfoliated thin sheets of a layered HOIP. 10,11 Early theoretical investigations of the optical properties of layered HOIPs were performed using the effective mass approximation, giving good estimates for the exciton binding energy and a qualitative explanation of the essential physics. 5,12-14 For a quantitative analysis, ab initio approaches such as density functional...

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Symmetry-Based Tight Binding Modeling of Halide Perovskite Semiconductors

Cited by 68 publications

References 58 publications

Effect of disorder on transport properties in a tight-binding model for lead halide perovskites

Effect of disorder on transport properties in a tight-binding model for lead halide perovskites

How Lattice and Charge Fluctuations Control Carrier Dynamics in Halide Perovskites

Optical Properties of Layered Hybrid Organic–Inorganic Halide Perovskites: A Tight-Binding GW-BSE Study

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