Статья

Pressure-Driven Cooperative Spin-Crossover, Large-Volume Collapse, and Semiconductor-to-Metal Transition in Manganese(II) Honeycomb Lattices

Yonggang WangGeophysical LaboratoryZhengyang ZhouCollege of Chemistry and Chemical Engineering, Chongqing University, Chongqing 400044, ChinaTing Bin WenInstitute of Nanostructured Functional Materials, Huanghe Science and Technology College, Zhengzhou, Henan 450006, ChinaYannan ZhouInstitute of Nanostructured Functional Materials, Huanghe Science and Technology College, Zhengzhou, Henan 450006, ChinaNana LiCenter for High Pressure Science and Technology Advanced Research (HPSTAR), Pudong, Shanghai 201203, ChinaFei HanCenter for the Study of Matter at Extreme Conditions, Department of Mechanical and Materials Engineering, Florida International University, Miami, Florida 33199, United StatesYuming XiaoHigh Pressure Collaborative Access Team (HPCAT), Geophysical Laboratory, Carnegie Institution of Washington, Argonne, Illinois 60439, United StatesPaul ChowHigh Pressure Collaborative Access Team (HPCAT), Geophysical Laboratory, Carnegie Institution of Washington, Argonne, Illinois 60439, United StatesJunliang SunCollege of Chemistry and Molecular Engineering, Peking University, Beijing 100871, ChinaMichael PravicaHigh Pressure Science and Engineering Center, University of Nevada, Las Vegas, Nevada 89154, United StatesAndrew CorneliusHigh Pressure Science and Engineering Center, University of Nevada, Las Vegas, Nevada 89154, United StatesWenge YangCenter for High Pressure Science and Technology Advanced Research (HPSTAR), Pudong, Shanghai 201203, ChinaYusheng ZhaoHigh Pressure Science and Engineering Center, University of Nevada, Las Vegas, Nevada 89154, United States

2016en

ABI

Аннотация

Spin-crossover (SCO) is generally regarded as a spectacular molecular magnetism in 3d4–3d7 metal complexes and holds great promise for various applications such as memory, displays, and sensors. In particular, SCO materials can be multifunctional when a classical light- or temperature-induced SCO occurs along with other cooperative structural and/or electrical transport alterations. However, such a cooperative SCO has rarely been observed in condensed matter under hydrostatic pressure (an alternative external stimulus to light or temperature), probably due to the lack of synergy between metal neighbors under compression. Here, we report the observation of a pressure-driven, cooperative SCO in the two-dimensional (2D) honeycomb antiferromagnets MnPS3 and MnPSe3 at room temperature. Applying pressure to this confined 2D system leads to a dramatic magnetic moment collapse of Mn2+ (d5) from S = 5/2 to S = 1/2. Significantly, a number of collective phenomena were observed along with the SCO, including a large lattice collapse (∼20% in volume), the formation of metallic bonding, and a semiconductor-to-metal transition. Experimental evidence shows that all of these events occur in the honeycomb lattice, indicating a strongly cooperative mechanism that facilitates the occurrence of the abrupt pressure-driven SCO. We believe that the observation of this cooperative pressure-driven SCO in a 2D system can provide a rare model for theoretical investigations and lead to the discovery of more pressure-responsive multifunctional materials.

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Идентификаторы

DOI: 10.1021/jacs.6b10225

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Цитирований: 2Использованных источников: 0

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