Exploring the Organometallic Route to Molecular Spin Qubits: The [CpTi(cot)] Case

Angew Chem Int Ed Engl. 2021 Feb 1;60(5):2588-2593. doi: 10.1002/anie.202009634. Epub 2020 Nov 26.

Abstract

The coherence time of the 17-electron, mixed sandwich complex [CpTi(cot)], (η8 -cyclooctatetraene)(η5 -cyclopentadienyl)titanium, reaches 34 μs at 4.5 K in a frozen deuterated toluene solution. This is a remarkable coherence time for a highly protonated molecule. The intramolecular distances between the Ti and H atoms provide a good compromise between instantaneous and spin diffusion sources of decoherence. Ab initio calculations at the molecular and crystal packing levels reveal that the characteristic low-energy ring rotations of the sandwich framework do not yield a too detrimental spin-lattice relaxation because of their small spin-phonon coupling. The volatility of [CpTi(cot)] and the accessibility of the semi-occupied, non-bonding d z 2 orbital make this neutral compound an ideal candidate for single-qubit addressing on surface and quantum sensing in combination with scanning probe microscopy.

Keywords: DFT; electron paramagnetic resonance; metallocene complexes; quantum coherence; titanium.