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. https://resolver.caltech.edu/CaltechAUTHORS:20191003-113813931
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Abstract
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.
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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. | ||||||||||||||||||||
Group: | JCAP | ||||||||||||||||||||
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Issue or Number: | 21 | ||||||||||||||||||||
DOI: | 10.1021/acs.jpclett.9b02219 | ||||||||||||||||||||
Record Number: | CaltechAUTHORS:20191003-113813931 | ||||||||||||||||||||
Persistent URL: | https://resolver.caltech.edu/CaltechAUTHORS:20191003-113813931 | ||||||||||||||||||||
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 | ||||||||||||||||||||
Collection: | CaltechAUTHORS | ||||||||||||||||||||
Deposited By: | George Porter | ||||||||||||||||||||
Deposited On: | 03 Oct 2019 22:33 | ||||||||||||||||||||
Last Modified: | 16 Nov 2021 17:43 |
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