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Chun-Yi Lin1, Thacien Ngendahimana2, Gareth R Eaton2

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The counterion significantly impacts V(iv) spin properties in ionic complexes. Larger cations affect solution tumbling, while counterion methyl groups influence phase memory time (T_m) in solid-state electron paramagnetic resonance (EPR) studies.

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Area of Science:

  • Inorganic Chemistry
  • Spin Chemistry
  • Materials Science

Background:

  • Transition metal ions are crucial for spin-based technologies like electron paramagnetic resonance imaging (EPRI) and quantum computation.
  • Understanding how local chemical environments affect spin properties is essential for optimizing these applications.
  • The influence of counterions on the spin dynamics of vanadium(IV) complexes has not been systematically investigated.

Purpose of the Study:

  • To systematically investigate the effect of counterions on the spin properties of V(iv) ionic complexes.
  • To elucidate the role of counterion size and nuclear spin density in influencing electron paramagnetic resonance (EPR) parameters.
  • To provide insights into the design of V(iv) complexes for advanced spin-based applications.

Main Methods:

  • Synthesis of four ionic V(iv) complexes with varying trialkylammonium counterions: (Et3NH)2[V(C6H4O2)3] (1), (n-Bu3NH)2[V(C6H4O2)3] (2), (n-Hex3NH)2[V(C6H4O2)3] (3), and (n-Oct3NH)2[V(C6H4O2)3] (4).
  • Characterization using continuous-wave X-band electron paramagnetic resonance (CW-EPR) spectroscopy in solution at room temperature.
  • Investigation of solid-state spin dynamics using variable-temperature X-band pulsed EPR spectroscopy (5-180 K) in an o-terphenyl glass matrix.

Main Results:

  • Solution CW-EPR showed increasing linewidth with larger cations, attributed to counterion-controlled tumbling via ion pairing.
  • Solid-state pulsed EPR revealed no significant effect of counterions on spin-lattice relaxation times (T1) between 5-180 K.
  • Phase memory times (Tm) were significantly shorter for complex 1 (Et3NH+) compared to complexes 2-4 (larger alkyl chains) below 100 K, contrary to expectations based on 1H nuclear spin density.

Conclusions:

  • Counterions play a critical role in modulating the spin properties of V(iv) complexes, particularly influencing solution dynamics and solid-state phase memory.
  • The methyl groups on the counterion appear to be crucial for enhancing phase memory times (Tm) in the solid state.
  • This study demonstrates the potential for tuning spin coherence by controlling counterion structure, offering a new strategy for spin-based molecular materials.