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Design of a One-Dimensional Stacked Spin Peierls System with Room-Temperature Switching from Quantum Mechanical Predictions

Yang, Hao and Cheng, Tao and Goddard, William A., III and Ren, Xiaoming (2019) Design of a One-Dimensional Stacked Spin Peierls System with Room-Temperature Switching from Quantum Mechanical Predictions. Journal of Physical Chemistry Letters, 10 (21). pp. 6432-6437. ISSN 1948-7185. doi:10.1021/acs.jpclett.9b02219.

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Planar bis-1,2-dithiolene complex anions of a transition metal (denoted as [M(dithiolato)₂]− and M = Ni, Pd, or Pt ion) favor forming columnar stacks of anions in the crystal that feature S = 1/2 spin-chains, and such a spin-chain compound often undergoes a spin-Peierls-type transition, making this a promising material for conducting and magnetic switching. However, current examples show the transition temperatures are far too low for most applications. We use quantum mechanics to predict that changing the cation arrangement from the boat-type to the chair-type packing configuration in a spin-Peierls-type [Ni(dithiolato)₂]⁻ complex will substantially stabilize the antiferromagnetic coupling, dramatically increasing the transition temperature. We estimate that the [Ni(mnt)₂]-based complexes (mnt = maleonitriledithiolate) with chair-type packing of cations will lead to critical temperatures of ∼170, ∼252, and ∼310 K for S-, Se-, and Te-based mnt, respectively. We also suggest how to stabilize the chair-type configurations of these systems.

Item Type:Article
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URLURL TypeDescription
Yang, Hao0000-0002-8241-6231
Cheng, Tao0000-0003-4830-177X
Goddard, William A., III0000-0003-0097-5716
Alternate Title:Design of a One-Dimensional Stacked Spin Peierls System with Room Temperature Switching from QM Predictions
Additional Information:© 2019 American Chemical Society. Received: July 30, 2019; Accepted: October 3, 2019; Published: October 3, 2019. We thank the Joint Ph.D. program of China Scholarships Council (Grant CSC No. 201608320161) for financial support of H.Y. This work was partially supported by the Postdoctoral routine program from Office of Human Resources and Social Security in Jiangsu Province of China (Grant No. 2019Z282). We thank the National Nature Science Foundation of China (Grant Nos. 91122011, 21071080, and 21671100), Priority Academic Program Development of the Jiangsu Higher Education Institutions, and the 111 Project of Collaborative Innovation Center of Suzhou Nano Science & Technology; W.A.G. received support from the Department of Energy (DE-SC0014607). We used the computational resources from the Extreme Science and Engineering Discovery Environment, which is supported by National Science Foundation Grant ACI-1548562. The authors declare no competing financial interest.
Funding AgencyGrant Number
China Scholarship Council201608320161
Jiangsu Office of Human Resources and Social Security2019Z282
National Natural Science Foundation of China91122011
National Natural Science Foundation of China21071080
National Natural Science Foundation of China21671100
Jiangsu Higher Education InstitutionsUNSPECIFIED
Suzhou Nano Science and TechnologyUNSPECIFIED
Department of Energy (DOE)DE-SC0014607
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Issue or Number:21
Record Number:CaltechAUTHORS:20191003-113813931
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Official Citation:Design of a One-Dimensional Stacked Spin Peierls System with Room-Temperature Switching from Quantum Mechanical Predictions. Hao Yang, Tao Cheng, William A. Goddard, III, and Xiao-Ming Ren. The Journal of Physical Chemistry Letters 2019 10 (21), 6432-6437. DOI: 10.1021/acs.jpclett.9b02219
Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:99051
Deposited By: George Porter
Deposited On:03 Oct 2019 22:33
Last Modified:16 Nov 2021 17:43

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