Limits to Electrical Mobility in Lead-Halide Perovskite Semiconductors

Xia, Chelsea Q.; Peng, Jiali; Poncé, Samuel; Patel, Jay B.; Wright, Adam D.; Crothers, Timothy; Rothmann, Mathias Uller; Borchert, Juliane; Milot, Rebecca L.; Kraus, H.; Lin, Qianqian; Giustino, Feliciano; Herz, Laura; Johnston, Michael B.

doi:10.1021/acs.jpclett.1c00619

Cited by 49 publications

(53 citation statements)

References 87 publications

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“…[27,62] Given that charge-carrier localization has been shown to depend on the dimension of a system, [21,73,86,87] with lower-dimensional systems having faster localization with lower or nonexistent energetic barriers, this finding agrees well with the theoretical predictions. However, we note that the effect is quite small, that is, we do not see an order-of-magnitude change in localization rate, and this could be linked to the general low electronic dimensionality of silverbismuth materials, [21,55,88] which might dominate over any changes in structural dimensionality.…”

Section: (10 Of 15)mentioning

confidence: 71%

Interplay of Structure, Charge‐Carrier Localization and Dynamics in Copper‐Silver‐Bismuth‐Halide Semiconductors

Buizza

Sansom

Wright

et al. 2021

Adv Funct Materials

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Silver-bismuth based semiconductors represent a promising new class of materials for optoelectronic applications because of their high stability, all-inorganic composition, and advantageous optoelectronic properties. In this study, charge-carrier dynamics and transport properties are investigated across five compositions along the AgBiI 4 -CuI solid solution line (stoichiometry Cu 4x (AgBi) 1−x I 4 ). The presence of a close-packed iodide sublattice is found to provide a good backbone for general semiconducting properties across all of these materials, whose optoelectronic properties are found to improve markedly with increasing copper content, which enhances photoluminescence intensity and charge-carrier transport. Photoluminescence and photoexcitation-energy-dependent terahertz photoconductivity measurements reveal that this enhanced charge-carrier transport derives from reduced cation disorder and improved electronic connectivity owing to the presence of Cu + . Further, increased Cu + content enhances the band curvature around the valence band maximum, resulting in lower charge-carrier effective masses, reduced exciton binding energies, and higher mobilities. Finally, ultrafast charge-carrier localization is observed upon pulsed photoexcitation across all compositions investigated, lowering the charge-carrier mobility and leading to Langevin-like bimolecular recombination. This process is concluded to be intrinsically linked to the presence of silver and bismuth, and strategies to tailor or mitigate the effect are proposed and discussed.

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Section: (10 Of 15)mentioning

confidence: 71%

Interplay of Structure, Charge‐Carrier Localization and Dynamics in Copper‐Silver‐Bismuth‐Halide Semiconductors

Buizza

Sansom

Wright

et al. 2021

Adv Funct Materials

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“…In Figure 6a, we show the isokinetic prefactor σ 00 as a function of the reciprocal of T iso as obtained from Figure 1, and approximate the relationship between the two constants [47] E k T σ σ = ′ − ln ln 00 00 n B iso (5) where 00 σ ′ and E n are empirical constants that we will explain below. The proton conductivity in Figure 6 follows Equation (5) (shown as the solid fitting line), as observed previously in semiconductors, [48] and in the proton conductivity in minerals.…”

Section: Tuning the Isokinetic Temperature According To Mnrmentioning

confidence: 99%

“…proton-conducting electrolytes for intermediate temperature (450-700 °C) protonconducting ceramic fuel cells (IT-PCFCs). [1][2][3][4][5][6][7] Fully understanding the proton transport mechanisms is vital for the improvement of proton conductivity. To form protonic defects, BaMO 3 is doped with trivalent elements to create oxygen vacancies.…”

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confidence: 99%

Optimizing the Proton Conductivity with the Isokinetic Temperature in Perovskite‐Type Proton Conductors According to Meyer–Neldel Rule

Ling

et al. 2021

Advanced Energy Materials

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Perovskite‐type metal oxides such as Y‐doped BaMO3 (M = Zr/Ce) have drawn considerable attention as proton‐conducting electrolytes for intermediate temperature ceramic electrochemical cells. Improving the proton conductivity at lower temperatures requires a comprehensive understanding of the proton conduction mechanism. By applying high pressure or varying the Ce content of Y‐doped BaMO3, it is demonstrated that the proton conductivity follows the Meyer–Neldel rule (MNR) well. In the Arrhenius plot, the conductivities intersect at an isokinetic temperature, where the proton conductivity is independent of activation energy. Considering the relationship between isokinetic temperature and lattice vibration frequency, a high isokinetic temperature is observed in materials with stiff lattices, consisting of light atoms and small MO bond length. Based on consideration of the MNR, it is suggested that the enhancement of proton conductivity at low temperature can be well achieved by tuning lattice vibration frequency toward a desired isokinetic temperature.

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“…Of polycrystalline film (not single-crystal) [62,[73][74][75] ; f ) At high frequency avoiding ionic diffusion; [76,77] g) Density-of-state at conduction band and valence band [78] ; h) Bimolecular recombination coefficient [66] ; i) Auger recombination coefficient [79] ; j)…”

Section: Impact Of Grain Boundary Recombination To Qflsmentioning

confidence: 99%

Understanding the Impacts of Grain Size Variation, Distribution, and Recombination Losses in Halide Perovskites: A Generalized Semi‐Analytical Model from Thin‐Film to Photovoltaics

Adhyaksa

2022

Energy Tech

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Halide-perovskites have rapidly emerged as one promising class of materials for lowcost and efficient photovoltaics (PVs). [1,2] A record cell efficiency of more than 25% made by a relatively low-cost solution-based fabrication process has been the main characteristic pointing that this technology may offer a solution to maintain sustainable cost per-kWh of power generation by PVs. [3] While at the material level, there is still a serious concern for the long-term stability, recent terrific efforts show that at the device level, the stability issue can already be resolved some of which led to great success. [4][5][6] For example, low-bandgap perovskite thin-films usually degrades within seconds to minutes, but after encapsulation with the device stacks, the PV efficiency can be retained at 95% for over 1000 h. [4][5][6][7][8] However, there are growing suspicions that the presence of material defects formed during the fabrication process and device operation is not only detrimental for the device's power conversion efficiency (PCE) but also critical for mitigating its long-term stability. [9][10][11][12][13] In the view of defect, the optoelectronic properties in halide perovskites are relatively tolerant to defect concentration compared to other PV materials. [14,15] However, for high-efficiency devices (e.g., more than 20% PCE), suppressing the concentration of material defects and taming its impact has proven to be the key leading to many recent efficiency records. [16][17][18][19][20] However, defect concentration in halide perovskites is largely influenced by how fast crystallization occurs. [21] The fast crystallization process naturally forms polycrystalline thin-films, whereby defects can occur inside the bulk, on top-and bottom-surfaces, and at the grain boundaries. For PV application, the thickness of perovskite materials is typically 0.25-1 micron, which is already sufficient to absorb 70-90% of incoming sun irradiation with respect to the material bandgap. [22,23] Surprisingly, most high-efficiency perovskite PVs have apparent "grain lateral sizes" rather small which is in the range of sub-micron (e.g., 0.3 microns), but still able to yield an efficiency of more than 20%. [19,20] This indicates that to attain efficiency even higher, for instance, above 25%,

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Limits to Electrical Mobility in Lead-Halide Perovskite Semiconductors

Cited by 49 publications

References 87 publications

Interplay of Structure, Charge‐Carrier Localization and Dynamics in Copper‐Silver‐Bismuth‐Halide Semiconductors

Interplay of Structure, Charge‐Carrier Localization and Dynamics in Copper‐Silver‐Bismuth‐Halide Semiconductors

Optimizing the Proton Conductivity with the Isokinetic Temperature in Perovskite‐Type Proton Conductors According to Meyer–Neldel Rule

Understanding the Impacts of Grain Size Variation, Distribution, and Recombination Losses in Halide Perovskites: A Generalized Semi‐Analytical Model from Thin‐Film to Photovoltaics

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