Metamagnetic transition and a loss of magnetic hysteresis caused by electron trapping in monolayers of single-molecule magnet Tb-2@C79N

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dc.contributor.authorKoutsouflakis, Emmanouilen
dc.contributor.authorKrylov, Denisen
dc.contributor.authorBachellier, Nicolasen
dc.contributor.authorSostina, Dariaen
dc.contributor.authorDubrovin, Vasiliien
dc.contributor.authorLiu, Fupinen
dc.contributor.authorSpree, Lukasen
dc.contributor.authorVelkos, Georgiosen
dc.contributor.authorSchimmel, Sebastianen
dc.contributor.authorWang, Yaofengen
dc.contributor.authorBuechner, Bernden
dc.contributor.authorWesterstrom, Rasmusen
dc.contributor.authorBulbucan, Claudiuen
dc.contributor.authorKirkpatrick, Kyleen
dc.contributor.authorMuntwiler, Matthiasen
dc.contributor.authorDreiser, Janen
dc.contributor.authorGreber, Thomasen
dc.contributor.authorAvdoshenko, Stas M.en
dc.contributor.authorDorn, Harryen
dc.contributor.authorPopov, Alexey A.en
dc.date.accessioned2022-11-10T15:06:00Zen
dc.date.available2022-11-10T15:06:00Zen
dc.date.issued2022-07-14en
dc.description.abstractRealization of stable spin states in surface-supported magnetic molecules is crucial for their applications in molecular spintronics, memory storage or quantum information processing. In this work, we studied the surface magnetism of dimetallo-azafullerene Tb-2@C79N, showing a broad magnetic hysteresis in a bulk form. Surprisingly, monolayers of Tb-2@C79N exhibited a completely different behavior, with the prevalence of a ground state with antiferromagnetic coupling at low magnetic field and a metamagnetic transition in the magnetic field of 2.5-4 T. Monolayers of Tb-2@C79N were deposited onto Cu(111) and Au(111) by evaporation in ultra-high vacuum conditions, and their topography and electronic structure were characterized by scanning tunneling microscopy and spectroscopy (STM/STS). X-ray photoelectron spectroscopy (XPS), in combination with DFT studies, revealed that the nitrogen atom of the azafullerene cage tends to avoid metallic surfaces. Magnetic properties of the (sub)monolayers were then studied by X-ray magnetic circular dichroism (XMCD) at the Tb-M-4,M-5 absorption edge. While in bulk powder samples Tb-2@C79N behaves as a single-molecule magnet with ferromagnetically coupled magnetic moments and blocking of magnetization at 28 K, its monolayers exhibited a different ground state with antiferromagnetic coupling of Tb magnetic moments. To understand if this unexpected behavior is caused by a strong hybridization of fullerenes with metallic substrates, XMCD measurements were also performed for Tb-2@C79N adsorbed on h-BN|Rh(111) and MgO|Ag(100). The co-existence of two forms of Tb-2@C79N was found on these substrates as well, but magnetization curves showed narrow magnetic hysteresis detectable up to 25 K. The non-magnetic state of Tb-2@C79N in monolayers is assigned to anionic Tb-2@C79N- species with doubly-occupied Tb-Tb bonding orbital and antiferromagnetic coupling of the Tb moments. A charge transfer from the substrate or trapping of secondary electrons are discussed as a plausible origin of these species.en
dc.description.notesComputational resources were provided by ZIH/TU Dresden. The work was performed with financial support from Deutsche Forschungsgemeinschaft (grants PO 1602/7-1 and PO 1602/8-1 to A. A. P., LI 3055/3-1 to F. L., and AV 169/3-1 to S. M. A.), the Swedish Research Council (Grant No. 201500455), and Sklodowska Curie Actions cofounding project INCA 600398. We acknowledge the Paul Scherrer Institute for providing synchrotron beamtime at the X-treme and PEARL beamlines of the Swiss Light Source.en
dc.description.sponsorshipDeutsche Forschungsgemeinschaft [PO 1602/7-1, PO 1602/8-1, LI 3055/3-1, AV 169/3-1]; Swedish Research Council [201500455]; Sklodowska Curie Actions [INCA 600398]en
dc.description.versionPublished versionen
dc.format.mimetypeapplication/pdfen
dc.identifier.doihttps://doi.org/10.1039/d1nr08475een
dc.identifier.eissn2040-3372en
dc.identifier.issn2040-3364en
dc.identifier.issue27en
dc.identifier.pmid35781298en
dc.identifier.urihttp://hdl.handle.net/10919/112556en
dc.identifier.volume14en
dc.language.isoenen
dc.publisherRoyal Society of Chemistryen
dc.rightsCreative Commons Attribution 4.0 Internationalen
dc.rights.urihttp://creativecommons.org/licenses/by/4.0/en
dc.subjectendohedral metallofullereneen
dc.subjectphotoelectron-spectroscopyen
dc.subjectexchangeen
dc.subjectspinen
dc.subjectsubmonolayeren
dc.subjectgd-2-at-c79nen
dc.subjectrelaxationen
dc.subjectfullereneen
dc.subjectspectraen
dc.subjectionen
dc.titleMetamagnetic transition and a loss of magnetic hysteresis caused by electron trapping in monolayers of single-molecule magnet Tb-2@C79Nen
dc.title.serialNanoscaleen
dc.typeArticle - Refereeden
dc.type.dcmitypeTexten

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