Observation of Extraordinary Vibration Scatterings Induced by Strong Anharmonicity in Lead-Free Halide Double Perovskites

被引:0
作者
Wang, Guang [1 ]
Zheng, Jiongzhi [2 ]
Xue, Jie [3 ]
Xu, Yixin [1 ]
Zheng, Qiye [1 ]
Hautier, Geoffroy [2 ]
Lu, Haipeng [3 ]
Zhou, Yanguang [1 ]
机构
[1] Hong Kong Univ Sci & Technol, Dept Mech & Aerosp Engn, Kowloon, Clear Water Bay, Hong Kong, Peoples R China
[2] Dartmouth Coll, Thayer Sch Engn, Hanover, NH 03755 USA
[3] Hong Kong Univ Sci & Technol, Dept Chem, Kowloon, Clear Water Bay, Hong Kong, Peoples R China
关键词
Double perovskite; FDTR; lattice vibrations; Raman and DFT; strong anharmonicity; two-channel thermal transport; THERMAL-CONDUCTIVITY; CRYSTAL; TRANSPORT; MOBILITIES; PHONONS; BLUE;
D O I
10.1002/advs.202408149
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
Lead-free halide double perovskites provide a promising solution for the long-standing issues of lead-containing halide perovskites, i.e., the toxicity of Pb and the low stability under ambient conditions and high-intensity illumination. Their light-to-electricity or thermal-to-electricity conversion is strongly determined by the dynamics of the corresponding lattice vibrations. Here, the measurement of lattice dynamics is presented in a prototypical lead-free halide double perovskite(Cs2NaInCl6). The quantitative measurements and first-principles calculations show that the scatterings among lattice vibrations at room temperature are at the timescale of approximate to 1 ps, which stems from the extraordinarily strong anharmonicity in Cs2NaInCl6. Further the degree of anharmonicity of each type of atom is quantitatively characterized in the Cs2NaInCl6 single crystal, which stems from the interatomic forces, and demonstrate that this strong anharmonicity is synergistically contributed by the bond hierarchy, the tilting of the NaCl6 and InCl6 octahedral units, and the rattling of Cs+ ions. Consequently, the crystalline Cs2NaInCl6 possesses an ultralow thermal conductivity of approximate to 0.43 W mK-1 at room temperature, and a weak temperature dependence of T -0.41. These findings uncovered the underlying mechanisms behind the dynamics of lattice vibrations in double perovskites, which can largely benefit the design of optoelectronics and thermoelectrics based on halide double perovskites.
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页数:12
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共 96 条
  • [1] Glassy thermal conductivity in Cs3Bi2I6Cl3 single crystal
    Acharyya, Paribesh
    Ghosh, Tanmoy
    Pal, Koushik
    Rana, Kewal Singh
    Dutta, Moinak
    Swain, Diptikanta
    Etter, Martin
    Soni, Ajay
    Waghmare, Umesh, V
    Biswas, Kanishka
    [J]. NATURE COMMUNICATIONS, 2022, 13 (01)
  • [2] Intrinsically Ultralow Thermal Conductivity in Ruddlesden-Popper 2D Perovskite Cs2PbI2Cl2: Localized Anharmonic Vibrations and Dynamic Octahedral Distortions
    Acharyya, Paribesh
    Ghosh, Tanmoy
    Pal, Koushik
    Kundu, Kaushik
    Rana, Kewal Singh
    Pandey, Juhi
    Soni, Ajay
    Waghmare, Umesh, V
    Biswas, Kanishka
    [J]. JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2020, 142 (36) : 15595 - 15603
  • [3] THERMAL-CONDUCTIVITY OF DISORDERED HARMONIC SOLIDS
    ALLEN, PB
    FELDMAN, JL
    [J]. PHYSICAL REVIEW B, 1993, 48 (17) : 12581 - 12588
  • [4] Phonons and related crystal properties from density-functional perturbation theory
    Baroni, S
    de Gironcoli, S
    Dal Corso, A
    Giannozzi, P
    [J]. REVIEWS OF MODERN PHYSICS, 2001, 73 (02) : 515 - 562
  • [5] IMPROVED TETRAHEDRON METHOD FOR BRILLOUIN-ZONE INTEGRATIONS
    BLOCHL, PE
    JEPSEN, O
    ANDERSEN, OK
    [J]. PHYSICAL REVIEW B, 1994, 49 (23): : 16223 - 16233
  • [6] Thermal conductivity of diamond under extreme pressure: A first-principles study
    Broido, D. A.
    Lindsay, L.
    Ward, A.
    [J]. PHYSICAL REVIEW B, 2012, 86 (11)
  • [7] Analysis of heat flow in layered structures for time-domain thermoreflectance
    Cahill, DG
    [J]. REVIEW OF SCIENTIFIC INSTRUMENTS, 2004, 75 (12) : 5119 - 5122
  • [8] Strong Anharmonicity at the Origin of Anomalous Thermal Conductivity in Double Perovskite Cs2NaYbCl6
    Cappai, Antonio
    Melis, Claudio
    Marongiu, Daniela
    Quochi, Francesco
    Saba, Michele
    Congiu, Francesco
    He, Yihui
    Slade, Tyler J.
    Kanatzidis, Mercouri G.
    Colombo, Luciano
    [J]. ADVANCED SCIENCE, 2024, 11 (09)
  • [9] Interfacial thermal resistance: Past, present, and future
    Chen, Jie
    Xu, Xiangfan
    Zhou, Jun
    Li, Baowen
    [J]. REVIEWS OF MODERN PHYSICS, 2022, 94 (02)
  • [10] All-solid-state dye-sensitized solar cells with high efficiency
    Chung, In
    Lee, Byunghong
    He, Jiaqing
    Chang, Robert P. H.
    Kanatzidis, Mercouri G.
    [J]. NATURE, 2012, 485 (7399) : 486 - U94