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

Authors

Yonggang Wang, University of Nevada, Las VegasFollow
Z Zhou, Chongqing University
T Wen, Huanghe Science and Technology CollegeFollow
Y Zhou, Huanghe Science and Technology College
N Li, Center for High Pressure Science and Technology Advanced Research
F Han, Florida International University
Y Xiao, Carnegie Institution of WashingtonFollow
P Chow, Carnegie Institution of WashingtonFollow
J Sun, Peking University
M Pravica, University of Nevada, Las VegasFollow
A L. Cornelius, University of Nevada, Las VegasFollow
W Yang, Center for High Pressure Science and Technology Advanced ResearchFollow
Y Zhao, University of Nevada Las VegasFollow

Document Type

Article

Publication Date

1-1-2016

Publication Title

Journal of the American Chemical Society

Volume

138

Issue

48

First page number:

15751

Last page number:

15757

Abstract

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. © 2016 American Chemical Society.

Language

English

Repository Citation

Wang, Y., Zhou, Z., Wen, T., Zhou, Y., Li, N., Han, F., Xiao, Y., Chow, P., Sun, J., Pravica, M., Cornelius, A. L., Yang, W., Zhao, Y. (2016). Pressure-Driven Cooperative Spin-Crossover, Large-Volume Collapse, and Semiconductor-to-Metal Transition in Manganese(II) Honeycomb Lattices. Journal of the American Chemical Society, 138(48), 15751-15757.
http://dx.doi.org/10.1021/jacs.6b10225