Pressure-Driven Reversible Switching between n- and p-Type Conduction in Chalcopyrite CuFeS2

Wen, Ting1; Wang, Yonggang1; Li, Nana1; Zhang, Qian1; Zhao, Yongsheng1; Yang, Wenge1; Zhao, Yusheng2,3; Mao, Ho-kwang1

2019-01-09

10.1021/jacs.8b11269

Journal of the American Chemical Society   影响因子和分区

0002-7863

Temperature-dependent switching between p- and n-type conduction is a newly observed phenomenon in very few Ag-based semiconductors, which may promote fascinating applications in modern electronics. Pressure, as an efficient external stimulus that has driven collective phenomena such as spin-crossover and Mott transition, is also expected to initialize a conduction-type switching in transition metal-based semiconductors. Herein, we report the observation of a pressure-driven dramatic switching between p- and n-type conduction in chalcopyrite CuFeS2 associated with a structural phase transition. Under compression around 8 GPa, CuFeS2 undergoes a phase transition with symmetry breakdown from space group I-42d to space group I-4 accompanying with a remarkable volume shrinkage of the FeS4 tetrahedra. A high-to-low spin crossover of Fe2+ (S = 2 to S = 0) is manifested along with this phase transition. Instead of pressure-driven metallization, a surprising semiconductor-to-semiconductor transition is observed associated with the structural and electronic transformations. Significantly, both photocurrent and Hall coefficient measurements confirm that CuFeS2 undergoes a reversible pressure-driven p-n conduction type switching accompanying with the structural phase transition. The absence of cationic charge transfer between copper and iron during the phase transition is confirmed by both X-ray absorption near-edge spectra (Cu/Fe, K-edge) and total-fluorescence-yield X-ray absorption spectra (Fe, K-edge) results, and the valence distribution maintains Cu2+Fe2+S2 in the high-pressure phase. The observation of an abrupt pressure-driven p-n conduction type switching in a transition metal-based semiconductor paves the way to novel pressure-responsive switching devices.

SCI ; EI

英语

NI论文

通讯

DOE-BES[DE-AC02-06CH11357]

Chemistry

Chemistry, Multidisciplinary

WOS:000455561800068

AMER CHEMICAL SOC

20185106270910

Charge transfer ; Copper compounds ; Iron compounds ; Semiconductor devices ; Switching ; Transition metals ; X ray absorption

Metallurgy and Metallography:531 ; Electromagnetic Waves:711 ; Semiconductor Devices and Integrated Circuits:714.2 ; Chemical Reactions:802.2

Web of Science

1.Ctr High Pressure Sci & Technol Adv Res HPSTAR, Beijing 100094, Peoples R China
2.Southern Univ Sci & Technol, Dept Phys, Shenzhen 518055, Peoples R China
3.Southern Univ Sci & Technol, Acad Adv Interdisciplinary Studies, Shenzhen 518055, Peoples R China

Wen, Ting,Wang, Yonggang,Li, Nana,et al. Pressure-Driven Reversible Switching between n- and p-Type Conduction in Chalcopyrite CuFeS2[J]. Journal of the American Chemical Society,2019,141(1):505-510.

Wen, Ting.,Wang, Yonggang.,Li, Nana.,Zhang, Qian.,Zhao, Yongsheng.,...&Mao, Ho-kwang.(2019).Pressure-Driven Reversible Switching between n- and p-Type Conduction in Chalcopyrite CuFeS2.Journal of the American Chemical Society,141(1),505-510.

Wen, Ting,et al."Pressure-Driven Reversible Switching between n- and p-Type Conduction in Chalcopyrite CuFeS2".Journal of the American Chemical Society 141.1(2019):505-510.