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Thermally Ultrarobust

Zhimin Yang1, Maren Pink2, Ewa Malgorzata Nowik-Boltyk3

  • 1Department of Chemistry, University of Nebraska, Lincoln, Nebraska 68588-0304, United States.

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|June 7, 2023
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Researchers synthesized stable open-shell organic radicals with potential for advanced technologies. These biphenylene-fused tetrazolinyl radicals exhibit excellent thermal stability and processability, making them promising for molecular spin qubits and electronic devices.

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Area of Science:

  • Organic Chemistry
  • Materials Science
  • Quantum Computing

Background:

  • Open-shell organic molecules, particularly S = 1/2 radicals, offer potential for advanced technologies.
  • Existing radical compounds often lack sufficient thermal stability and processability for practical applications.

Purpose of the Study:

  • To synthesize and characterize novel S = 1/2 biphenylene-fused tetrazolinyl radicals.
  • To evaluate their thermal stability, electrochemical properties, magnetic behavior, and potential as molecular spin qubits.

Main Methods:

  • Synthesis of biphenylene-fused tetrazolinyl radicals.
  • X-ray crystallography and density-functional theory (DFT) for structural analysis.
  • Thermogravimetric analysis (TGA) for thermal stability.
  • Electrochemical measurements for oxidation potentials and energy gaps.
  • Superconducting quantum interference device (SQUID) magnetometry for magnetic properties.
  • Electron paramagnetic resonance (EPR) and X-ray photoelectron spectroscopy (XPS) for radical stability and assembly characterization.

Main Results:

  • Synthesized two novel S = 1/2 biphenylene-fused tetrazolinyl radicals with planar structures.
  • Radical 1 demonstrated outstanding thermal stability (decomposition onset at 269 °C) and low oxidation potential (<0 V vs. SCE).
  • Magnetic studies revealed a 1D S = 1/2 antiferromagnetic Heisenberg chain in radical 1.
  • Radical 1 exhibited a long electron spin coherence time (Tm ≈ 7 μs) and formed stable nanoneedles upon UHV evaporation.
  • Assemblies showed remarkable air stability (64 hours monitored by XPS) and a long radical half-life (50 ± 4 days at ambient conditions via EPR).

Conclusions:

  • The synthesized biphenylene-fused tetrazolinyl radicals possess exceptional thermal stability and processability.
  • These radicals are promising candidates for molecular spin qubits due to their long spin coherence times.
  • Their stability and unique properties suggest potential applications in emerging electronic and quantum technologies.