108397 20230519145437.0 doi 10.1039/d1sc00564b sideral 123407 ART-2021-123407 eng Gimeno, I (orcid)0000-0002-6184-3920 Broad-band spectroscopy of a vanadyl porphyrin: a model electronuclear spin qudit 2021 Access copy available to the general public Unrestricted 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. info:eu-repo/grantAgreement/ES/DGA/E09-17R-Q-MAD info:eu-repo/grantAgreement/ES/DGA/E31-17R info:eu-repo/grantAgreement/EC/H2020/862893/EU/Molecular spin qudits offering new hope for quantum computing/FATMOLS This project has received funding from the European Union’s Horizon 2020 research and innovation program under grant agreement No H2020 862893-FATMOLS info:eu-repo/grantAgreement/ES/MICINN/CTQ2015-64486-R info:eu-repo/grantAgreement/ES/MICINN/CTQ2015-68370-P info:eu-repo/grantAgreement/ES/MICINN/MAT2017-86826-R info:eu-repo/grantAgreement/ES/MICINN/PCI2018-093116 info:eu-repo/grantAgreement/ES/MICINN/PGC2018-098630-B-I00 info:eu-repo/grantAgreement/ES/MICINN/RTI2018-096075-B-C21 info:eu-repo/semantics/openAccess by http://creativecommons.org/licenses/by/3.0/es/ 9.969 2021 CHEMISTRY, MULTIDISCIPLINARY 25 / 180 = 0.139 2021 Q1 T1 2.878 2021 Chemistry (miscellaneous) 2021 Q1 info:eu-repo/semantics/article info:eu-repo/semantics/publishedVersion Urtizberea, A Universidad de Zaragoza (orcid)0000-0002-8424-9780 Roman-Roche, J (orcid)0000-0003-2995-6615 Zueco, D (orcid)0000-0003-4478-1948 Camon, A (orcid)0000-0001-7289-5649 Alonso, PJ (orcid)0000-0003-3449-4929 Roubeau, O (orcid)0000-0003-2095-5843 Luis, F (orcid)0000-0001-6284-0521 5001 065 Universidad de Zaragoza Dpto. Ciencia Tecnol.Mater.Fl. Área Cienc.Mater. Ingen.Metal. 12, 15 (2021), 5621-5630 Chem. sci. CHEMICAL SCIENCE 2041-6520 1755665 http://zaguan.unizar.es/record/108397/files/texto_completo.pdf Versión publicada 2863945 http://zaguan.unizar.es/record/108397/files/texto_completo.jpg?subformat=icon icon Versión publicada oai:zaguan.unizar.es:108397 articulos driver 2023-05-18-14:24:46 ARTICLE