0D Pyramid-intercalated 2D Bimetallic Halides with Tunable Electronic Structures and Enhanced Emission under Pressure

Liu, Yang1; Liang, Jiayuan2; Deng, Zeyu3; Guo, Songhao2; Ji, Xiaoqin1; Chen, Congcong1; Canepa, Pieremanuele3,4,5,6,7; Lue, Xujie2; Mao, Lingling1

2023-11-01

10.1002/anie.202314977

ANGEWANDTE CHEMIE-INTERNATIONAL EDITION   影响因子和分区

1433-7851

1521-3773

["Hybrid metal halides are emerging semiconductors as potential candidates for optoelectronics. The pursuit of hybridizing various dimensions of metal halides remains a desirable yet highly complex endeavor. By utilizing dimension engineering, a diverse array of new materials with intrinsically different electronic and optical properties has been developed. Here, we report a new family of 2D-0D hybrid bimetallic halides, (C6N2H14)2SbCdCl9 & sdot; 2H2O (SbCd) and (C6N2H14)2SbCuCl9 & sdot; 2H2O (SbCu). These compounds adopt a new layered structure, consisting of alternating 0D square pyramidal [SbCl5] and 2D inorganic layers sandwiched by organic layers. SbCd and SbCu have optical band gaps of 3.3 and 2.3 eV, respectively. These compounds exhibit weak photoluminescence (PL) at room temperature, and the PL gradually enhances with decreasing temperature. Density functional theory (DFT) calculations reveal that SbCd and SbCu are direct gap semiconductors, where first-principles band gaps follow the experimental trend. Moreover, given the different pressure responses of 0D and 2D components, these materials exhibit highly tunable electronic structures during compression, where a remarkable 11 times enhancement in PL emission is observed for SbCd at 19 GPa. This work opens new avenues for designing new layered bimetallic halides and further manipulating their structures and optoelectronic properties via pressure.","Here, we report a new unique family of hybrid layered bimetallic halides with Cd/Cu as the MII site and Sb as the MIII site within the layered structure, with intercalated SbCl5 pyramids. These materials exhibit tunable electronic properties and optical band gaps from 2 to 3 eV. Using pressure as an external stimulus, the photoluminescence of the Cd analog is largely enhanced by 11 times.image"]

Electronic Properties Hybrid Metal Halide Perovskite Derivatives Photoluminescence Pressure

SCI ; EI

英语

NI论文

第一 ; 通讯

This work was supported by the National Natural Science Foundation of China (NSFC) under Grant Nos. 22275077 and 22275004, the Stable Support Plan Program of Shenzhen Natural Science Fund (Program Contract No. 20220814233319001), and the Startup Fund of SU["22275077","22275004"] ; National Natural Science Foundation of China (NSFC)[20220814233319001] ; Stable Support Plan Program of Shenzhen Natural Science Fund[R-284-000-186-133] ; Singa-pore Ministry of Education Academic Fund Tier 1[22-5930-A0001]

Chemistry

Chemistry, Multidisciplinary

WOS:001105753100001

WILEY-V C H VERLAG GMBH

20234715100691

Antimony compounds ; Copper compounds ; Density functional theory ; Electronic properties ; Electronic structure ; Energy gap ; Metal halides ; Optical properties ; Photoluminescence ; Structural properties

Structural Design:408 ; Minerals:482.2 ; Light/Optics:741.1 ; Chemical Products Generally:804 ; Probability Theory:922.1 ; Atomic and Molecular Physics:931.3 ; Quantum Theory; Quantum Mechanics:931.4 ; Materials Science:951

CHEMISTRY

2-s2.0-85177596791

Web of Science

1.Southern Univ Sci & Technol, SUSTech Energy Inst Carbon Neutral, Dept Chem, Shenzhen 518055, Guangdong, Peoples R China
2.Ctr High Pressure Sci & Technol Adv Res HPSTAR, Shanghai 201203, Peoples R China
3.Natl Univ Singapore, Dept Mat Sci & Engn, 9 Engn Dr 1, Singapore 117575, Singapore
4.Singapore MIT Alliance Res & Technol, 1 CREATE Way,10-01 CREATE Tower, Singapore 138602, Singapore
5.Natl Univ Singapore, Dept Chem & Biomol Engn, 4 Engn Dr 4, Singapore 117585, Singapore
6.Univ Houston, Dept Elect & Comp Engn, Houston, TX 77204 USA
7.Univ Houston, Texas Ctr Superconduct, Houston, TX 77204 USA

Liu, Yang,Liang, Jiayuan,Deng, Zeyu,et al. 0D Pyramid-intercalated 2D Bimetallic Halides with Tunable Electronic Structures and Enhanced Emission under Pressure[J]. ANGEWANDTE CHEMIE-INTERNATIONAL EDITION,2023,62(52).

Liu, Yang.,Liang, Jiayuan.,Deng, Zeyu.,Guo, Songhao.,Ji, Xiaoqin.,...&Mao, Lingling.(2023).0D Pyramid-intercalated 2D Bimetallic Halides with Tunable Electronic Structures and Enhanced Emission under Pressure.ANGEWANDTE CHEMIE-INTERNATIONAL EDITION,62(52).

Liu, Yang,et al."0D Pyramid-intercalated 2D Bimetallic Halides with Tunable Electronic Structures and Enhanced Emission under Pressure".ANGEWANDTE CHEMIE-INTERNATIONAL EDITION 62.52(2023).