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

Journal Article · · Journal of Physical Chemistry Letters
 [1]; ORCiD logo [2]; ORCiD logo [2]; ORCiD logo [3]
  1. Nanjing Tech Univ. (China). State Key Lab. of Materials-Oriented Chemical Engineering; California Institute of Technology (CalTech), Pasadena, CA (United States). Materials and Process Simulation Center; Soochow Univ., Suzhou (China). Inst. of Functional Nano & Soft Materials (FUNSOM), Jiangsu Key Lab. for Carbon-Based Functional Materials & Devices, Joint International Research Lab. of Carbon-Based Functional Materials and Devices
  2. California Institute of Technology (CalTech), Pasadena, CA (United States). Materials and Process Simulation Center; Soochow Univ., Suzhou (China). Inst. of Functional Nano & Soft Materials (FUNSOM), Jiangsu Key Lab. for Carbon-Based Functional Materials & Devices, Joint International Research Lab. of Carbon-Based Functional Materials and Devices
  3. Nanjing Tech Univ. (China). State Key Lab. of Materials-Oriented Chemical Engineering; Nanjing Tech Univ. (China)
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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. Furthermore, 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.

Research Organization:
Univ. of Southern California, Los Angeles, CA (United States)
Sponsoring Organization:
USDOE Office of Science (SC); China Scholarship Council (CSC); National Natural Science Foundation of China (NSFC); National Science Foundation (NSF)
Grant/Contract Number:
SC0014607; 201608320161; 91122011; 21071080; 21671100; ACI-1548562
OSTI ID:
1802689
Journal Information:
Journal of Physical Chemistry Letters, Vol. 10, Issue 21; ISSN 1948-7185
Publisher:
American Chemical SocietyCopyright Statement
Country of Publication:
United States
Language:
English

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Related Subjects

36 MATERIALS SCIENCE
Chemical structure
Energy
Anions
Quantum mechanics
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