First-Principles Study of Lead Iodide Perovskite Tetragonal and Orthorhombic Phases for Photovoltaics

Wang, Geng; Zhang, Le; Zhang, Yanning; Lau, Woon‐Ming; Liu, Li-Min

doi:10.1021/jp504951h

Cited by 224 publications

(202 citation statements)

References 43 publications

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“…53 which agrees with the experimental results. It is well-known that the spin-orbit coupling (SOC) effect has great effect on the calculated band gap, as shown in the previous work [29]…”

supporting

confidence: 91%

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Effect of surface composition on electronic properties of methylammonium lead iodide perovskite

Wang

Tong

Tang

et al. 2015

Journal of Materiomics

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Methylammonium lead iodide perovskite, CH 3 NH 3 PbI 3 , is one of the most promising photovoltaic materials for low-cost and clean source of energy. In this work, the first-principles calculations were carried out to investigate the different composition of CH 3 NH 3 PbI 3 (001), including both methylammonium iodide terminated (MAI-T) and PbI 2 terminated (PBI 2 -T) surfaces. The calculated surface energies show that the MAI-T is thermodynamical more stable than the PBI 2 -T one under the equilibrium growth condition. The electronic properties of the two types of surfaces are also different. The band gap of PBI 2 -T is obviously smaller than that of MAI-T due to the surface Pb states. Band gaps of MAI-T decrease with increasing thickness, while band gaps of PBI 2 -T are insensitive to the slab thickness. The calculated optical absorption coefficients suggest that both terminations are effective solar energy absorbers in the visible light spectrum.

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“…53 which agrees with the experimental results. It is well-known that the spin-orbit coupling (SOC) effect has great effect on the calculated band gap, as shown in the previous work [29]…”

supporting

confidence: 91%

“…In our previous work, the band gap of bulk tetragonal phase CH 3 NH 3 PbI 3 was found to be about 1.6 eV ( Fig. 4(b)), [53] [53] 53 [53] 53 …”

Section: The Electronic Propertiesmentioning

confidence: 99%

Effect of surface composition on electronic properties of methylammonium lead iodide perovskite

Wang

Tong

Tang

et al. 2015

Journal of Materiomics

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“…42,[46][47][48][49][50]54,55,[60][61][62][63][64] Furthermore, there are certain publications describing direct evidences to the existence of two phases at low temperatures, 48,[65][66][67] which are also supported by our own lowtemperature TEM electron diffraction experiments reported in the supplementary information. Hence, the most significant finding of this work is the inhibition of the phase transition in 1D perovskite nanorods having diameter below ~ 100-150 nm.…”

Section: Discussionsupporting

confidence: 75%

“…Similar phase-transition characteristics of 3D (bulk) perovskites has been observed by others [46][47][48][49][50] and supported by theoretical calculations. 54,55 This implies that, as far as the PL spectroscopy is concerned, both the microwires and the 175 nm nanorods behave as 3D perovskites. On the other hand, only the low-energy emission group has been observed for the 70 nm and the 30 nm nanorods over all temperatures, indicating that the tetragonal phase dominates throughout the entire temperature range and the phase-transition is inhibited in these essentially 1D perovskite nanorods.…”

Section: Methodsmentioning

confidence: 99%

Inhibition of a structural phase transition in one-dimensional organometal halide perovskite nanorods grown inside porous silicon nanotube templates

et al. 2017

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One-dimensional organo-metal halide Perovskite (CH 3 NH 3 PbI 3 ) nanorods whose diameter and length are dictated by the inner size of porous silicon nanotube templates have been grown, characterized and compared to bulk perovskites in the form of microwires. We have observed a structural phase transition for bulk perovskites, where the crystal structure changes from tetragonal to orthorhombic at about 150K, as opposed to small diameter one-dimensional perovskite nanorods, of the order of 30-70 nm in diameter, where the phase transition is inhibited and the dominant phase remains tetragonal. Two major experimental techniques, infrared absorption spectroscopy and photoluminescence, were utilized to probe the temperature dependence of the perovskite phases over the 4-300K temperature range.Yet, different characteristics of the phase transition were measured by the two spectroscopic methods and explained by the presence of small, tetragonal inclusions embedded in the orthorhombic phase. The inhibition of the phase transition is attributed to the large surface area of these one-dimensional perovskite nanorods, which gives rise to a large stress that, in turn, prevents the formation of the orthorhombic phase. The absence of phase transition enables the measurement of the tetragonal bandgap energy down to low temperatures. *

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“…Side-views of the resulting structures of tetragonal CH 3 In the optimized crystal structure, the Pb−I bond lengths were estimated to be 3.155, 3.258 and 3.278 Å, which compare well with crystal parameters of the same phase of CH 3 NH 3 PbI 3 calculated previously without considering spin−orbit coupling (SOC). [20][21] The band structure calculated using van der Waals density functional (vdW-DF2) for the optimized geometry shows a direct band gap energy of E g =1.60 eV at the Γ point ( Figure 1d). This value is slightly higher than the optical bandgap determined from the Tauc plot of experimental absorbance (E g =1.58 eV), but in good agreement with previous theoretical predictions.…”

mentioning

confidence: 99%

Interfacial Charge Transfer Anisotropy in Polycrystalline Lead Iodide Perovskite Films

Yin

Cortecchia

Krishna

et al. 2015

J. Phys. Chem. Lett.

145

141

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Solar cells based on organic-inorganic lead iodide perovskite (CH3NH3PbI3) exhibit remarkably high power conversion efficiency (PCE). One of the key issues in solution-processed films is that often the polycrystalline domain orientation is not well-defined, which makes it difficult to predict energy alignment and charge transfer efficiency. Here we combine ab initio calculations and photoelectron spectroscopy to unravel the electronic structure and charge redistribution at the interface between different surfaces of CH3NH3PbI3 and typical organic hole acceptor Spiro-OMeTAD and electron acceptor PCBM. We find that both hole and electron interfacial transfer depend strongly on the CH3NH3PbI3 surface orientation: while the (001) and (110) surfaces tend to favor hole injection to Spiro-OMeTAD, the (100) surface facilitates electron transfer to PCBM due to surface delocalized charges and hole/electron accumulation at the CH3NH3PbI3/organic interfaces. Molecular dynamic simulations indicate that this is due to strong orbital interactions under thermal fluctuations at room temperature, suggesting the possibility to further improve charge separation and extraction in perovskite-based solar cells by controlling perovskite film crystallization and surface orientation.

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First-Principles Study of Lead Iodide Perovskite Tetragonal and Orthorhombic Phases for Photovoltaics

Cited by 224 publications

References 43 publications

Effect of surface composition on electronic properties of methylammonium lead iodide perovskite

Effect of surface composition on electronic properties of methylammonium lead iodide perovskite

Inhibition of a structural phase transition in one-dimensional organometal halide perovskite nanorods grown inside porous silicon nanotube templates

Interfacial Charge Transfer Anisotropy in Polycrystalline Lead Iodide Perovskite Films

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