期刊
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
卷 137, 期 4, 页码 1673-1678出版社
AMER CHEMICAL SOC
DOI: 10.1021/ja512396m
关键词
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资金
- Office of Science, Office of Basic Energy Sciences, of the U.S. Department of Energy [DE-AC02-05CH11231]
- U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences [DE-AC02-98CH10886]
- COMPRES, the Consortium for Materials Properties Research in Earth Sciences under NSF [EAR 11-57758]
- National Science Foundation CAREER [DMR-1351538]
- Department of Energy through the Stanford Institute for Materials Energy Science [DE-AC02-76SF00515]
- Satre Family through the Stanford Interdisciplinary Graduate Fellowship
- Direct For Mathematical & Physical Scien
- Division Of Materials Research [1351538] Funding Source: National Science Foundation
Pressure-induced changes in the electronic structure of two-dimensional Cu-based materials have been a subject of intense study. In particular, the possibility of suppressing the Jahn-Teller distortion of d(9) Cu centers with applied pressure has been debated over a number of decades. We studied the structural and electronic changes resulting from the application of pressures up to ca. 60 GPa on a two-dimensional copper(II)-chloride perovskite using diamond anvil cells (DACs), through a combination of in situ powder X-ray diffraction, electronic absorption and vibrational spectroscopy, dc resistivity measurements, and optical observations. Our measurements show that compression of this charge-transfer insulator initially yields a first-order structural phase transition at ca. 4 GPa similar to previous reports on other Cu-II-Cl perovskites, during which the originally translucent yellow solid turns red. Further compression induces a previously unreported phase transition at ca. 8 GPa and dramatic piezochromism from translucent red-orange to opaque black. Two-probe dc resistivity measurements conducted within the DAC show the first instance of appreciable conductivity in Cu-II-Cl perovskites. The conductivity increases by 5 orders of magnitude between 7 and 50 GPa, with a maximum measured conductivity of 2.9 x 10(-4) Scm(-1) at 51.4 GPa. Electronic absorption spectroscopy and variable-temperature conductivity measurements indicate that the perovskite behaves as a 1.0 eV band-gap semiconductor at 39.7 GPa and has an activation energy for electronic conduction of 0.232(1) eV at 40.2 GPa. Remarkably, all these changes are reversible: the material reverts to a translucent yellow solid upon decompression, and ambient pressure powder X-ray diffraction data taken before and after compression up to 60 GPa show that the original structure is maintained with minimal hysteresis.
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