Tailoring the thermal conductivity of two-dimensional metal halide perovskites

Thakur, Sandip; Dai, Zhenghong; Karna, Pravin; Padture, Nitin P.; Giri, Ashutosh

doi:10.1039/d2mh01070d

Cited by 11 publications

(7 citation statements)

References 49 publications

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“…The thermal conductivities determined via k = D•c p •ρ and shown in Figure 2(d) also feature only minor temperature dependencies. In agreement with recent experimental and theoretical studies, 48,49,57 we observe that both RP materials have lower thermal conductivities than MAPbI 3 . Furthermore, the thermal conductivity of PEA 2 PbI 4 is lower than that of BA 2 PbI 4 .…”

Section: Resultssupporting

confidence: 92%

“…While the dynamic distortions markedly influence the free carrier masses and drift-diffusion transport mechanisms, they do not affect the exciton binding energies and exciton diffusion in quasi-2D RP perovskites . Thermal transport properties of quasi-2D RP perovskites have come into focus only recently, when several experimental and theoretical studies ,, reported ultralow thermal conductivities in A 2 PbX 4 (A = BA, PEA, X = I, Br) using thermal reflectance measurements combined with molecular dynamics simulations based on a classical force field. A theoretical study using a similar force field by Fridriksson et al also showed that length and aromaticity of the interlayer molecule significantly affect the structural rigidity of the perovskite sublattice .…”

Section: Introductionmentioning

confidence: 99%

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Dynamic Distortions of Quasi-2D Ruddlesden–Popper Perovskites at Elevated Temperatures: Influence on Thermal and Electronic Properties

et al. 2023

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Ruddlesden−Popper hybrid halide perovskites are quasi-two-dimensional materials with a layered structure and structural dynamics that are determined by the interplay between the organic and inorganic layers. While their optical properties are governed by confinement effects, the atomistic origin of thermal and electronic properties of these materials is yet to be fully established. Here we combine computational and experimental techniques to study A 2 PbI 4 (A = butylammonium (BA), phenethylammonium (PEA)) Ruddlesden−Popper perovskites and compare them with the quintessential perovskite CH 3 NH 3 PbI 3 . We use first-principles density functional theory, molecular dynamics simulations based on machine-learned interatomic potentials, thermal measurements, temperature-dependent Raman spectroscopy, and ultraviolet photoelectron spectroscopy to probe the thermal and electronic properties of these materials at elevated temperatures. Our molecular dynamics simulations demonstrate that dynamic fluctuations in the organic sublattice determine the bulk-average distortions of these materials at room temperature, explaining significant differences in their electronic density of states close to the Fermi level. Furthermore, by analyzing the organic layer dynamics in BA 2 PbI 4 we provide a mechanistic explanation for the phase transition of this material at 274 K and observations from Raman measurements. Our results highlight the role of the organic interlayer for the electronic and thermal transport properties of Ruddlesden−Popper perovskites, paving the way for the design of new hybrid materials for tailored applications.

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Section: Resultssupporting

confidence: 92%

Section: Introductionmentioning

confidence: 99%

Dynamic Distortions of Quasi-2D Ruddlesden–Popper Perovskites at Elevated Temperatures: Influence on Thermal and Electronic Properties

et al. 2023

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“…Particularly remarkable is the case of K 3 ITe, as its κ L at room temperature is much lower than that of leading thermoelectric materials such as PbTe and Bi 2 Te 3 (with κ L values of ∼1 W m −1 K −1 ). Moreover, K 3 ITe stands out with a κ L value that is lower than those of currently popular metal halide perovskites, such as CsCdBr 3 (∼0.42 W m −1 K −1 ), 52 CsSrF 3 (∼0.90 W m −1 K −1 ), 51 and CsPbI 3 (∼0.56 W m −1 K −1 ), 53 antiperovskites such as K 3 BrO (∼1.7 W m −1 K −1 ) and Rb 3 BrO (∼0.8 W m −1 K −1 ), 54 and alloy materials. 55 To assess the temperature dependence of κ L , we fit the κ L with the relation κ L ∝ T −α .…”

Section: Chemistry Of Materialsmentioning

confidence: 87%

Anomalous Thermal Conductivity and High Thermoelectric Performance of Cubic Antiperovskites K₃IX(Se & Te)

Zeng,

Guo,

Huang

et al. 2023

Chem. Mater.

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The performance of thermoelectric (TE) materials is restricted by the coupling between electronic and phonon transport. On the basis of first-principles calculations, self-consistent phonon theory, and the Boltzmann transport equation, this study proposes a novel class of cubic weak-bonding antiperovskites, K 3 IX(Se & Te), which has not been synthesized thus far. These materials exhibit strong lattice anharmonicity and enable the separation of electronic and phonon transport at the atomic level. With quartic anharmonicity correction, antiperovskites K 3 I(Se & Te) are predicted to exhibit remarkably low lattice thermal conductivities κ L . At room temperature, the calculated κ L values of K 3 ISe and K 3 ITe are only 0.60 and 0.18 W m −1 K −1 , respectively. Additionally, these types of materials demonstrate an anomalously weak temperature dependence of κ L , approximately conforming to a power-law relationship where κ L ∼ T −0.3 for K 3 ITe. Simultaneously, the high degeneracy and nearly flat band structure endow K 3 IX(Se & Te) with large power factors when doped. At 800 K, under p-type doping, the calculated ZT values of K 3 ISe and K 3 ITe can reach 1.33 and 2.61, respectively, surpassing those of the leading traditional TE materials. The results have revealed that K 3 IX(Se & Te) represent a promising class of TE materials exhibiting excellent performance, and the structural features that effectively decouple phonon and electron transport also offer novel perspectives for the investigation of highperformance TE materials.

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“…16 Similarly, the thermal conductivity of COFs can be effectively modulated through strain engineering. 17,18 Besides, mechanical stimuli are also inevitable in many applications of 2D materials. For instance, in the thermal catalysis applications of 2D materials, such as 2D MXenes, the operational conditions typically encompass elevated temperatures and pressures.…”

Section: Introductionmentioning

confidence: 99%

The thermoelastic properties of monolayer covalent organic frameworks studied by machine-learning molecular dynamics

Wang,

Ying,

Zhang

2024

Nanoscale

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Tailoring the thermal conductivity of two-dimensional metal halide perovskites

Abstract: Proper thermal management of solar cells based on metal halide perovskites (MHPs) is key to increasing their efficiency as well as their durability. Although two-dimensional (2D) MHPs possess enhanced thermal...

Cited by 11 publications

References 49 publications

Dynamic Distortions of Quasi-2D Ruddlesden–Popper Perovskites at Elevated Temperatures: Influence on Thermal and Electronic Properties

Dynamic Distortions of Quasi-2D Ruddlesden–Popper Perovskites at Elevated Temperatures: Influence on Thermal and Electronic Properties

Anomalous Thermal Conductivity and High Thermoelectric Performance of Cubic Antiperovskites K₃IX(Se & Te)

The thermoelastic properties of monolayer covalent organic frameworks studied by machine-learning molecular dynamics

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Tailoring the thermal conductivity of two-dimensional metal halide perovskites

Abstract: Proper thermal management of solar cells based on metal halide perovskites (MHPs) is key to increasing their efficiency as well as their durability. Although two-dimensional (2D) MHPs possess enhanced thermal...

Cited by 11 publications

References 49 publications

Dynamic Distortions of Quasi-2D Ruddlesden–Popper Perovskites at Elevated Temperatures: Influence on Thermal and Electronic Properties

Dynamic Distortions of Quasi-2D Ruddlesden–Popper Perovskites at Elevated Temperatures: Influence on Thermal and Electronic Properties

Anomalous Thermal Conductivity and High Thermoelectric Performance of Cubic Antiperovskites K3IX(Se & Te)

The thermoelastic properties of monolayer covalent organic frameworks studied by machine-learning molecular dynamics

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Anomalous Thermal Conductivity and High Thermoelectric Performance of Cubic Antiperovskites K₃IX(Se & Te)