Tunable Vacancy Order and Emergent Functionalities in Half‐Heusler Crystals

Z Ziheng Gao Z Zhongkang Han (State Key Laboratory of Silicon and Advanced Semiconductor Materials and Center of Electron Microscopy, School of Materials Science and Engineering) Y Yue Zhang C Chenguang Fu (State Key Laboratory of Silicon and Advanced Semiconductor Materials, School of Materials Science and Engineering) K Kaiyang Xia (Institute of Wenzhou Zhejiang University Wenzhou 325006 China) Y Yujing Zhang M Mingyuan Piao (State Key Laboratory of Silicon and Advanced Semiconductor Materials School of Materials Science and Engineering Zhejiang University Hangzhou 310058 China) M Mengzhao Chen (State Key Laboratory of Silicon and Advanced Semiconductor Materials School of Materials Science and Engineering Zhejiang University Hangzhou 310058 China) S Shen Han A Airan Li X Xiaojuan Hu P Pengfei Nan (State Key Laboratory of Optoelectronic Information Acquisition and Protection Technology, Leibniz International Joint Research Center of Materials Sciences of Anhui Province, Institutes of Physical Science and Information Technology) J Jiawei Zhang X Xuezhang Xiao B Binghui Ge (State Key Laboratory of Opto-Electronic Information Acquisition and Protection Technology, Anhui University, Hefei, China.) T Tiejun Zhu (State Key Laboratory of Silicon and Advanced Semiconductor Materials, School of Materials Science and Engineering)

Abstract

Abstract Extra chemical order within periodic crystalline lattices offers a promising approach for designing materials with emergent functionalities. However, achieving tunable extra chemical order in crystalline materials remains challenging. Here, it is found that the vacancy order in cation‐deficient half‐Heusler crystals V 1‐ δ CoSb can be tuned from long‐range order (LRO) to short‐range order (SRO), or vice versa. The vacancy LRO and SRO configurations are uncovered by scanning transmission electron microscopy analysis and Monte Carlo simulations. Remarkably, the evolution of vacancy order induces profound changes in electrical, magnetic, and thermal properties, as well as hydrogen storage characteristics. In particular, the electronic density of state effective mass exhibits a nearly threefold increase, while ferromagnetism emerges from infancy when tuning the vacancy order from LRO to SRO. These results elucidate the local chemical order‐property relationship and highlight the great potential of achieving desirable functionalities by designing extra chemical order in crystalline solids.

Article Details

Volume / Issue Vol. 37, Issue 34
Published August 01, 2025
ISSN 0935-9648
Publisher Unknown Publisher

Journal Info

Advanced Materials

Unknown Publisher

ISSN: 0935-9648 Physical Sciences

Authors (16)

Z

Ziheng Gao

Z

Zhongkang Han

State Key Laboratory of Silicon and Advanced Semiconductor Materials and Center of Electron Microscopy, School of Materials Science and Engineering

Y

Yue Zhang

C

Chenguang Fu

State Key Laboratory of Silicon and Advanced Semiconductor Materials, School of Materials Science and Engineering

K

Kaiyang Xia

Institute of Wenzhou Zhejiang University Wenzhou 325006 China

Y

Yujing Zhang

M

Mingyuan Piao

State Key Laboratory of Silicon and Advanced Semiconductor Materials School of Materials Science and Engineering Zhejiang University Hangzhou 310058 China

M

Mengzhao Chen

State Key Laboratory of Silicon and Advanced Semiconductor Materials School of Materials Science and Engineering Zhejiang University Hangzhou 310058 China

S

Shen Han

A

Airan Li

X

Xiaojuan Hu

P

Pengfei Nan

State Key Laboratory of Optoelectronic Information Acquisition and Protection Technology, Leibniz International Joint Research Center of Materials Sciences of Anhui Province, Institutes of Physical Science and Information Technology

J

Jiawei Zhang

X

Xuezhang Xiao

B

Binghui Ge

State Key Laboratory of Opto-Electronic Information Acquisition and Protection Technology, Anhui University, Hefei, China.

T

Tiejun Zhu

State Key Laboratory of Silicon and Advanced Semiconductor Materials, School of Materials Science and Engineering