Molecular electronic spin qubits from a spin-frustrated trinuclear copper complex
Chemical Communications Royal Society of Chemistry 54:92 (2018) 12934-12937
Abstract:
The trinuclear copper(II) complex [Cu3(saltag)(py)6]ClO4 (H5saltag = tris(2-hydroxybenzylidene)triaminoguanidine) was synthesized and characterized by experimental as well as theoretical methods. This complex exhibits a strong antiferromagnetic coupling (J = −298 cm−1) between the copper(II) ions, mediated by the N–N diazine bridges of the tritopic ligand, leading to a spin-frustrated system. This compound shows a T2 coherence time of 340 ns in frozen pyridine solution, which extends to 591 ns by changing the solvent to pyridine-d5. Hence, the presented compound is a promising candidate as a building block for molecular spintronics.Implications of bond disorder in a S=1 kagome lattice
Scientific Reports Nature Publishing Group 8:1 (2018) 4745
Abstract:
Strong hydrogen bonds such as F···H···F offer new strategies to fabricate molecular architectures exhibiting novel structures and properties. Along these lines and, to potentially realize hydrogen-bond mediated superexchange interactions in a frustrated material, we synthesized [H2F]2[Ni3F6(Fpy)12][SbF6]2 (Fpy = 3-fluoropyridine). It was found that positionally-disordered H2F+ ions link neutral NiF2(Fpy)4 moieties into a kagome lattice with perfect 3-fold rotational symmetry. Detailed magnetic investigations combined with density-functional theory (DFT) revealed weak antiferromagnetic interactions (J ~ 0.4 K) and a large positive-D of 8.3 K with ms = 0 lying below ms = ±1. The observed weak magnetic coupling is attributed to bond-disorder of the H2F+ ions which leads to disrupted Ni-F···H-F-H···F-Ni exchange pathways. Despite this result, we argue that networks such as this may be a way forward in designing tunable materials with varying degrees of frustration.Endohedral metallofullerene as molecular high spin qubit: diverse Rabi cycles in Gd2@C79N
Journal of the American Chemical Society American Chemical Society 140:3 (2017) 1123-1130
Abstract:
An anisotropic high-spin qubit with long coherence time could scale the quantum system up. It has been proposed that Grover's algorithm can be implemented in such systems. Dimetallic aza[80]fullerenes M2@C79N (M = Y or Gd) possess an unpaired electron located between two metal ions, offering an opportunity to manipulate spin(s) protected in the cage for quantum information processing. Herein, we report the crystallographic determination of Gd2@C79N for the first time. This molecular magnet with a collective high-spin ground state (S = 15/2) generated by strong magnetic coupling (JGd-Rad = 350 ± 20 cm-1) has been unambiguously validated by magnetic susceptibility experiments. Gd2@C79N has quantum coherence and diverse Rabi cycles, allowing arbitrary superposition state manipulation between each adjacent level. The phase memory time reaches 5 μs at 5 K by dynamic decoupling. This molecule fulfills the requirements of Grover's searching algorithm proposed by Leuenberger and Loss.Strong coupling of microwave photons to antiferromagnetic fluctuations in an organic magnet
Physical Review Letters American Physical Society 119:14 (2017) 147701
Abstract:
Coupling between a crystal of di(phenyl)-(2,4,6-trinitrophenyl)iminoazanium (DPPH) radicals and a superconducting microwave resonator is investigated in a circuit quantum electrodynamics (cQED) architecture. The crystal exhibits paramagnetic behavior above 4 K, with antiferromagnetic correlations appearing below this temperature, and we demonstrate strong coupling at base temperature. The magnetic resonance acquires a field angle dependence as the crystal is cooled down, indicating anisotropy of the exchange interactions. These results show that multi-spin modes in organic crystals are suitable for cQED, offering a platform for their coherent manipulation. They also utilize the cQED architecture as a way to probe spin correlations at low temperature.Quantum interference in graphene nanoconstrictions
Nano Letters American Chemical Society 16:7 (2016) 4210-4216