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Broad-band spectroscopy of a vanadyl porphyrin: a model electronuclear spin qudit

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Abstract

We explore how to encode more than a qubit in vanadyl porphyrin molecules hosting a S = 1/2 electronic spin coupled to a I = 7/2 nuclear spin. The spin Hamiltonian and its parameters, as well as the spin dynamics, have been determined via a combination of electron paramagnetic resonance, heat capacity, magnetization and on-chip magnetic spectroscopy experiments performed on single crystals. We find low temperature spin coherence times of micro-seconds and spin relaxation times longer than a second. For sufficiently strong magnetic fields (B > 0.1 T, corresponding to resonance frequencies of 9–10 GHz) these properties make vanadyl porphyrin molecules suitable qubit realizations. The presence of multiple equispaced nuclear spin levels then merely provides 8 alternatives to define the ‘1’ and ‘0’ basis states. For lower magnetic fields (B < 0.1 T), and lower frequencies (<2 GHz), we find spectroscopic signatures of a sizeable electronuclear entanglement. This effect generates a larger set of allowed transitions between different electronuclear spin states and removes their degeneracies. Under these conditions, we show that each molecule fulfills the conditions to act as a universal 4-qubit processor or, equivalently, as a d = 16 qudit. These findings widen the catalogue of chemically designed systems able to implement non-trivial quantum functionalities, such as quantum simulations and, especially, quantum error correction at the molecular level.

Graphical abstract: Broad-band spectroscopy of a vanadyl porphyrin: a model electronuclear spin qudit

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Article information


Submitted
29 Jan 2021
Accepted
09 Mar 2021
First published
17 Mar 2021

This article is Open Access
All publication charges for this article have been paid for by the Royal Society of Chemistry

Chem. Sci., 2021, Advance Article
Article type
Edge Article

Broad-band spectroscopy of a vanadyl porphyrin: a model electronuclear spin qudit

I. Gimeno, A. Urtizberea, J. Román-Roche, D. Zueco, A. Camón, P. J. Alonso, O. Roubeau and F. Luis, Chem. Sci., 2021, Advance Article , DOI: 10.1039/D1SC00564B

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