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  Tunable Spin–Superconductor Coupling of Spin 1/2 Vanadyl Phthalocyanine Molecules

Malavolti, L., Briganti, M., Hänze, M., Serrano, G., Cimatti, I., McMurtrie, G., et al. (2018). Tunable Spin–Superconductor Coupling of Spin 1/2 Vanadyl Phthalocyanine Molecules. Nano Letters, 18(12), 7955-7961. doi:10.1021/acs.nanolett.8b03921.

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Item Permalink: http://hdl.handle.net/21.11116/0000-0002-B83D-B Version Permalink: http://hdl.handle.net/21.11116/0000-0002-B83E-A
Genre: Journal Article

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 Creators:
Malavolti, L.1, 2, 3, Author              
Briganti, M.4, Author
Hänze, M.1, 2, 3, Author              
Serrano, G.4, Author
Cimatti, I.4, Author
McMurtrie, G.1, 2, 3, Author              
Otero, E.5, Author
Ohresser, P.5, Author
Totti, F.4, Author
Mannini, M.4, Author
Sessoli, R.4, Author
Loth, S.1, 2, 3, Author              
Affiliations:
1Institute for Functional Matter and Quantum Technologies, ou_persistent22              
2Dynamics of Nanoelectronic Systems, Independent Research Groups, Max Planck Institute for the Structure and Dynamics of Matter, Max Planck Society, ou_1938290              
3Max Planck Institute for Solid State Research, ou_persistent22              
4Dipartimento di Chimica “Ugo Schiff” & INSTM RU, Università degli Studi di Firenze, ou_persistent22              
5Synchrotron SOLEIL, ou_persistent22              

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Free keywords: density functional theory; molecular magnetism; scanning tunneling spectroscopy; superconductivity; X-ray magnetic circular dichroism; Yu−Shiba−Rusinov bound states
 Abstract: Atomic-scale magnetic moments in contact with superconductors host rich physics based on the emergence of Yu–Shiba–Rusinov (YSR) magnetic bound states within the superconducting condensate. Here, we focus on a magnetic bound state induced into Pb nanoislands by individual vanadyl phthalocyanine (VOPc) molecules deposited on the Pb surface. The VOPc molecule is characterized by a spin magnitude of 1/2 arising from a well-isolated singly occupied dxy-orbital and is a promising candidate for a molecular spin qubit with long coherence times. X-ray magnetic circular dichroism (XMCD) measurements show that the molecular spin remains unperturbed even for molecules directly deposited on the Pb surface. Scanning tunneling spectroscopy and density functional theory (DFT) calculations identify two adsorption geometries for this “asymmetric” molecule (i.e., absence of a horizontal symmetry plane): (a) oxygen pointing toward the vacuum with the Pc laying on the Pb, showing negligible spin–superconductor interaction, and (b) oxygen pointing toward the Pb, presenting an efficient interaction with the Pb and promoting a Yu–Shiba–Rusinov bound state. Additionally, we find that in the first case a YSR state can be induced smoothly by exerting mechanical force on the molecules with the scanning tunneling microscope (STM) tip. This allows the interaction strength to be tuned continuously from an isolated molecular spin case, through the quantum critical point (where the bound state energy is zero) and beyond. DFT indicates that a gradual bending of the VO bond relative to the Pc ligand plane promoted by the STM tip can modify the interaction in a continuously tunable manner. The ability to induce a tunable YSR state in the superconductor suggests the possibility of introducing coupled spins on superconductors with switchable interaction.

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Language(s): eng - English
 Dates: 2018-11-072018-09-292018-11-192018-12
 Publication Status: Published in print
 Pages: 7
 Publishing info: -
 Table of Contents: -
 Rev. Method: Peer
 Identifiers: DOI: 10.1021/acs.nanolett.8b03921
 Degree: -

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Title: Nano Letters
  Abbreviation : Nano Lett.
Source Genre: Journal
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Publ. Info: Washington, DC : American Chemical Society
Pages: - Volume / Issue: 18 (12) Sequence Number: - Start / End Page: 7955 - 7961 Identifier: ISSN: 1530-6984
CoNE: https://pure.mpg.de/cone/journals/resource/110978984570403