62 results on '"Valvidares M"'
Search Results
2. Strontium hexaferrite platelets: a comprehensive soft X-ray absorption and Mössbauer spectroscopy study
- Author
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Soria, G. D., Jenus, P., Marco, J. F., Mandziak, A., Sanchez-Arenillas, M., Moutinho, F., Prieto, J. E., Prieto, P., Cerdá, J., Tejera-Centeno, C., Gallego, S., Foerster, M., Aballe, L., Valvidares, M., Vasili, H. B., Pereiro, E., Quesada, A., and de la Figuera, J.
- Published
- 2019
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3. Hybrid Bloch-N\'eel spiral states in Mn$_{1.4}$PtSn probed by resonant soft x-ray scattering
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Sukhanov, A. S., Ukleev, V., Vir, P., Gargiani, P., Valvidares, M., White, J. S., Felser, C., and Inosov, D. S.
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Condensed Matter - Strongly Correlated Electrons - Abstract
Multiple intriguing phenomena have recently been discovered in tetragonal Heusler compounds, where $D_{2d}$ symmetry sets a unique interplay between Dzyaloshinskii-Moriya (DM) and magnetic dipolar interactions. In the prototype $D_{2d}$ compound Mn$_{1.4}$PtSn, this has allowed the stabilization of exotic spin textures such as first-reported anti-skyrmions or elliptic Bloch-type skyrmions. While less attention has so far been given to the low-field spiral state, this remains extremely interesting as a simplest phase scenario on which to investigate the complex hierarchy of magnetic interactions in this materials family. Here, via resonant small-angle soft x-ray scattering experiments on high-quality single crystals of Mn$_{1.4}$PtSn at low temperatures, we evidence how the underlying $D_{2d}$ symmetry of the DMI in this material is reflected in its magnetic texture. Our studies reveal the existence of a novel and complex metastable phase, which possibly has a mixed character of both the N\'{e}el-type cycloid and the Bloch-type helix, that forms at low temperature in zero fields upon the in-plane field training. This hybrid spin-spiral structure has a remarkable tunability, allowing to tilt its orientation beyond high-symmetry crystallographic directions and control its spiral period. These results broaden the reachness of Heusler $D_{2d}$ materials exotic magnetic phase diagram and extend its tunability, thus enhancing a relevant playground for further fundamental explorations and potential applications in energy saving technologies.
- Published
- 2022
4. Absence of Magnetic Proximity Effect at the Interface of Bi2Se3 and (Bi,Sb)2Te3 with EuS
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Figueroa, A. I., Bonell, F., Cuxart, M. G., Valvidares, M., Gargiani, P., van der Laan, G., Mugarza, A., Valenzuela, S. O., ICN2 - Institut Catala de Nanociencia i Nanotecnologia (ICN2), Universitat Autònoma de Barcelona (UAB), ALBA Synchrotron light source [Barcelone], DIAMOND Light source, Institució Catalana de Recerca i Estudis Avançats (ICREA), European Commission, European Research Council, Generalitat de Catalunya, Ministerio de Economía y Competitividad (España), Ministerio de Ciencia, Innovación y Universidades (España), and Agencia Estatal de Investigación (España)
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[PHYS]Physics [physics] ,Condensed Matter::Materials Science ,Condensed Matter - Mesoscale and Nanoscale Physics ,Mesoscale and Nanoscale Physics (cond-mat.mes-hall) ,FOS: Physical sciences - Abstract
We performed x-ray magnetic circular dichroism (XMCD) measurements on heterostructures comprising topological insulators (TIs) of the (Bi,Sb)2(Se,Te)3 family and the magnetic insulator EuS. XMCD measurements allow us to investigate element-selective magnetic proximity effects at the very TI/EuS interface. A systematic analysis reveals that there is neither significant induced magnetism within the TI nor an enhancement of the Eu magnetic moment at such interface. The induced magnetic moments in Bi, Sb, Te, and Se sites are lower than the estimated detection limit of the XMCD measurements of ∼10−3μB/at., This research was supported by the European Union’s Horizon 2020 FET-PROACTIVE project TOCHA under Grant Agreement 824140. The authors acknowledge funding by the European Research Council under Grant Agreement No. 306652 SPINBOUND, by the CERCA Programme/Generalitat de Catalunya 2017 SGR 827, by MINECO (under Contracts No. MAT2016-75952-R, No. MAT2016-78293-C6-2-R, No. PID2019-111773RBI00/AEI/10.13039/501100011033, No. PID2019- 107338RB-C65, and Severo Ochoa No. SEV-2017-0706) and the European Regional Development Fund (ERDF) under the program Interreg V-A España-Francia-Andorra (Contract No. EFA 194/16 TNSI). A. I. F. acknowledges funding from MINECO-Juan de la Cierva fellowship ref. IJCI-2015-25514 and from the European Union’s Horizon 2020 People Programme (Marie Skłodowska Curie Actions) H2020-MSCA-IF-2017 under REA Grant Agreement No. 796925. F. B. acknowledges funding from MINECO Ramón y Cajal Program under Contract No. RYC-2015-18523.
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- 2020
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5. Reversible spin storage in metal oxide—fullerene heterojunctions
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Moorsom, T, Rogers, M, Scivetti, I, Bandaru, S, Teobaldi, G, Valvidares, M, Flokstra, M, Lee, S, Stewart, R, Prokscha, T, Gargiani, P, Alosaimi, N, Stefanou, G, Ali, M, Al Ma'Mari, F, Burnell, G, Hickey, BJ, and Cespedes, O
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Condensed Matter::Strongly Correlated Electrons - Abstract
We show that hybrid MnOx/C60 heterojunctions can be used to design a storage device for spin-polarized charge: a spin capacitor. Hybridization at the carbon-metal oxide interface leads to spin-polarized charge trapping after an applied voltage or photocurrent. Strong electronic structure changes, including a 1-eV energy shift and spin polarization in the C60 lowest unoccupied molecular orbital, are then revealed by x-ray absorption spectroscopy, in agreement with density functional theory simulations. Muon spin spectroscopy measurements give further independent evidence of local spin ordering and magnetic moments optically/electronically stored at the heterojunctions. These spin-polarized states dissipate when shorting the electrodes. The spin storage decay time is controlled by magnetic ordering at the interface, leading to coherence times of seconds to hours even at room temperature.
- Published
- 2020
6. Extremely fast domain wall motion in compensated magnetic insulators
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Zhou, H., Dong, Y., Xu, T., Xu, K., Sánchez-Tejerina, L., Zhao, L., Cai, L., Ba, Y., Gargiani, P., Valvidares, M., Zhao, Y., Carpentieri, M., Tretiakov, O., Zhong, X., Finocchio, G., Kim, S., and Jiang, W.
- Published
- 2020
7. Compensated ferrimagnetic insulators for extremely fast spin-orbitronics
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Zhou, H., Dong, Y., Xu, T., Xu, K., Sánchez-Tejerina, L., Zhao, L., Cai, L., Ba, Y., Gargiani, P., Valvidares, M., Zhao, Y., Carpentieri, M., Tretiakov, O., Zhong, X., Finocchio, G., Kim, S., and Jiang, W.
- Published
- 2020
8. Surface states and Rashba-type spin polarization in antiferromagnetic $MnBi_{2}Te_{4}$ (0001)
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Vidal, R. C., Bentmann, H., Peixoto, T. R. F., Zeugner, A., Moser, S., Min, C.-H., Schatz, S., Kißner, K., Ünzelmann, M., Fornari, C. I., Vasili, H. B., Valvidares, M., Sakamoto, K., Mondal, D., Fujii, J., Vobornik, I., Jung, S., Cacho, C., Kim, T. K., Koch, R. J., Jozwiak, C., Bostwick, A., Denlinger, J. D., Rotenberg, E., Buck, J., Hoesch, M., Diekmann, F., Rohlf, S., Kalläne, M., Rossnagel, K., Otrokov, M. M., Chulkov, E. V., Ruck, M., Isaeva, A., and Reinert, F.
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Engineering ,Fluids & Plasmas ,Physical Sciences ,Chemical Sciences ,ddc:530 - Abstract
Physical review / B covering condensed matter and materials physics 100(12), 121104-1-121104-6 (2019). doi:10.1103/PhysRevB.100.121104, The layered van der Waals antiferromagnet $MnBi_{2}Te_{4}$ (0001) has been predicted to combine the band ordering of archetypical topological insulators such as Bi2Te3 with the magnetism of Mn, making this material a viable candidate for the realization of various magnetic topological states. We have systematically investigated the surface electronic structure of $MnBi_{2}Te_{4}$ (0001)single crystals by use of spin- and angle-resolved photoelectron spectroscopy experiments. In line with theoretical predictions, the results reveal a surface state in the bulk band gap and they provide evidence for the influence of exchange interaction and spin-orbit coupling on the surface electronic structure., Published by Inst., Woodbury, NY
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- 2019
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9. Towards microscopic control of the magnetic exchange coupling at the surface of a topological insulator
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Rüßmann, P. Mahatha, S.K. Sessi, P. Valbuena, M.A. Bathon, T. Fauth, K. Godey, S. Mugarza, A. Kokh, K.A. Tereshchenko, O.E. Gargiani, P. Valvidares, M. Jiménez, E. Brookes, N.B. Bode, M. Bihlmayer, G. Blügel, S. Mavropoulos, P. Carbone, C. Barla, A.
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Condensed Matter::Materials Science - Abstract
Magnetically doped topological insulators may produce novel states of electronic matter, where for instance the quantum anomalous Hall effect state can be realized. Pivotal to this goal is a microscopic control over the magnetic state, defined by the local electronic structure of the dopants and their interactions. We report on the magnetic coupling among Mn or Co atoms adsorbed on the surface of the topological insulator Bi2Te3. Our findings uncover the mechanisms of the exchange coupling between magnetic atoms coupled to the topological surface state in strong topological insulators. The combination of x-ray magnetic circular dichroism and ab initio calculations reveals that the sign of the magnetic coupling at short adatom-adatom distances is opposite for Mn with respect to Co. For both elements, the magnetic exchange reverses its sign at a critical distance between magnetic adatoms, as a result of the interplay between superexchange, double exchange and Ruderman-Kittel-Kasuya-Yoshida interactions. © 2018 The Author(s). Published by IOP Publishing Ltd
- Published
- 2018
10. Layer-dependence of macroscopic and atomic magnetic correlations in Co/Pd multilayers.
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Soriano, N., Mora, B., Rollano, V., Gargiani, P., Quirós, C., Gálvez, F., Redondo, C., del Valle, J., Montoya, I., Gómez, A., González, E. M., Navarro, E., Vélez, M., Alameda, J. M., Valvidares, M., Vicent, J. L., and Morales, R.
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MAGNETIC anisotropy ,MAGNETIC circular dichroism ,NUCLEAR energy ,MAGNETIC moments ,PERPENDICULAR magnetic anisotropy ,MAGNETIC properties ,MAGNETIC materials - Abstract
The development of multilayered materials with engineered magnetic properties compels a deep knowledge of physical properties at the atomic scale. The magnetic anisotropy is a key property in these materials. This work accounts for the magnetic anisotropy energy and its correlation with atomic properties of Co/Pd multilayers with the number of Co/Pd repetitions. Magnetometry measurements confirm stronger perpendicular magnetic anisotropy energies as the number of repetitions increases up to 40. However, the intrinsic anisotropy, related to the Co–Pd orbital hybridization and spin–orbit coupling, saturates at 15 repetitions. This finding is supported by x-ray magnetic circular dichroism analysis that reveals a direct correlation of the atomic Co and Pd orbital magnetic moments and the effective anisotropy of the system. The proximity effect that accounts for the Pd induced magnetization, along with the increasing Co moment, provides a suitable mechanism for the observed anisotropy energy layer dependence. [ABSTRACT FROM AUTHOR]
- Published
- 2020
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11. Mesoscopic electron focusing in topological insulators
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Sessi, P., R����mann, P., Bathon, T., Barla, A., Kokh, K. A., Tereshchenko, O. E., Fauth, K., Mahatha, S. K., Valbuena, M. A., Godey, S., Mugarza, A., Gargiani, P., Valvidares, M., Long, N. H., Carbone, C., Mavropoulos, P., Bl��gel, S., and Bode, M.
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Condensed Matter - Mesoscale and Nanoscale Physics ,Mesoscale and Nanoscale Physics (cond-mat.mes-hall) ,FOS: Physical sciences - Abstract
The particle wave duality sets a fundamental correspondence between optics and quantum mechanics. Within this framework, the propagation of quasiparticles can give rise to superposition phenomena which, like for electromagnetic waves, can be described by the Huygens principle. However, the utilization of this principle by means of propagation and manipulation of quantum information is limited by the required coherence in time and space. Here we show that in topological insulators, which in their pristine form are characterized by opposite propagation directions for the two quasiparticles spin channels, mesoscopic focusing of coherent charge density oscillations can be obtained at large nested segments of constant energy contours by magnetic surface doping. Our findings provide evidence of strongly anisotropic Dirac fermion-mediated interactions. Even more remarkably, the validity of our findings goes beyond topological insulators but applies for systems with spin orbit lifted degeneracy in general. It demonstrates how spin information can be transmitted over long distances, allowing the design of experiments and devices based on coherent quantum effects in this fascinating class of materials.
- Published
- 2016
12. Graphene-based synthetic antiferromagnets and ferrimagnets.
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Gargiani, P., Cuadrado, R., Vasili, H. B., Pruneda, M., and Valvidares, M.
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MAGNETIC films ,REMANENCE ,NANOTECHNOLOGY ,FERRIMAGNETIC materials ,LOW temperatures ,MAGNETIC properties ,NANOELECTRONICS - Abstract
Graphene-spaced magnetic systems with antiferromagnetic exchange-coupling offer exciting opportunities for emerging technologies. Unfortunately, the in-plane graphene-mediated exchange-coupling found so far is not appropriate for realistic exploitation, due to being weak, being of complex nature, or requiring low temperatures. Here we establish that ultra-thin Fe/graphene/Co films grown on Ir(111) exhibit robust perpendicular antiferromagnetic exchange-coupling, and gather a collection of magnetic properties well-suited for applications. Remarkably, the observed exchange coupling is thermally stable above room temperature, strong but field controllable, and occurs in perpendicular orientation with opposite remanent layer magnetizations. Atomistic first-principles simulations provide further ground for the feasibility of graphene-spaced antiferromagnetic coupled structures, confirming graphene's direct role in sustaining antiferromagnetic superexchange-coupling between the magnetic films. These results provide a path for the realization of graphene-based perpendicular synthetic antiferromagnetic systems, which seem exciting for fundamental nanoscience or potential use in spintronic devices. [ABSTRACT FROM AUTHOR]
- Published
- 2017
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13. Absence of Magnetic Proximity Effect at the Interface of Bi 2 Se 3 and ( Bi , Sb ) 2 Te 3 with EuS
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Figueroa, A. I., Bonell, F., Cuxart, M. G., Valvidares, M., Gargiani, P., van der Laan, G., Mugarza, A., and Valenzuela, S. O.
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14. Absence of magnetic proximity effects in magnetoresistive Pt/CoFe2O4 hybrid interfaces.
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Valvidares, M., Dix, N., Isasa, M., Ollefs, K., Wilhelm, F., Rogalev, A., Sánchez, F., Pellegrin, E., Bedoya-Pinto, A., Gargiani, P., Hueso, L. E., Casanova, F., and Fontcuberta, J.
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MAGNETIZATION , *PLATINUM compounds , *SPIN Hall effect - Abstract
Ultrathin Pt films grown on insulating ferrimagnetic CoFe2O4 (111) epitaxial films display a magnetoresistance upon rotating the magnetization of the magnetic layer. We report here x-ray magnetic circular dichroism (XMCD) recorded at Pt-L2,3 and Pt-M3 edges. The results indicate that the Pt magnetic moment, if any, is below the detection limit (<0.001µB/Pt), thus strongly favoring the view that the presence of CoFe2O4 does not induce the formation of magnetic moments in Pt. Therefore, the observed magnetoresistance cannot be attributed to some sort of proximity-induced magnetic moments at Pt ions and subsequent magnetic-field dependent scattering. It thus follows that either bulk (spin Hall and inverse spin Hall effects) or interface (Rashba) spin-orbit related effects dominate the observed magnetoresistance. Furthermore, comparison of bulk magnetization and XMCD data at (Fe,Co)-L2,3 edges suggests the presence of some spin disorder in the CoFe2O4 layer which may be relevant for the observed anomalous nonsaturating field dependence of spin Hall magnetoresistance. [ABSTRACT FROM AUTHOR]
- Published
- 2016
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15. Absence of Magnetic Proximity Effect at the Interface of Bi2Se3 and (Bi,Sb)2Te3 with EuS.
- Author
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Figueroa, A. I., Bonell, F., Cuxart, M. G., Valvidares, M., Gargiani, P., van der Laan, G., Mugarza, A., and Valenzuela, S. O.
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ANTIMONY , *MAGNETIC insulators , *BISMUTH , *MAGNETIC circular dichroism , *TOPOLOGICAL insulators , *MAGNETIC moments , *DETECTION limit - Abstract
We performed x-ray magnetic circular dichroism (XMCD) measurements on heterostructures comprising topological insulators (TIs) of the (Bi,Sb)2(Se,Te)3 family and the magnetic insulator EuS. XMCD measurements allow us to investigate element-selective magnetic proximity effects at the very TI/EuS interface. A systematic analysis reveals that there is neither significant induced magnetism within the TI nor an enhancement of the Eu magnetic moment at such interface. The induced magnetic moments in Bi, Sb, Te, and Se sites are lower than the estimated detection limit of the XMCD measurements of ~10-3 μB/at. [ABSTRACT FROM AUTHOR]
- Published
- 2020
- Full Text
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16. Direct observation of multivalent states and 4f→3d charge transfer in Ce-doped yttrium iron garnet thin films.
- Author
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Vasili, H. B., Casals, B., Cichelero, R., Macià, F., Geshev, J., Gargiani, P., Valvidares, M., Herrero-Martin, J., Pellegrin, E., Fontcuberta, J., and Herranz, G.
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IRON compounds , *PHOTONICS , *X-ray spectroscopy - Abstract
Due to their large magneto-optic responses, rare-earth-doped yttrium iron garnets, Y3Fe5O12 (YIG), are highly regarded for their potential in photonics and magnonics. Here, we consider the case of Ce-doped YIG (Ce-YIG) thin films, in which substitutional Ce3+ ions are magnetic because of their 4f¹ ground state. In order to elucidate the impact of Ce substitution on the magnetization of YIG, we have carried out soft x-ray spectroscopy measurements on Ce-YIG films. In particular, we have used the element specificity of x-ray magnetic circular dichroism to extract the individual magnetization curves linked to Ce and Fe ions. Our results show that Ce doping triggers a selective charge transfer from Ce to the Fe tetrahedral sites in the YIG structure. This, in turn, causes a disruption of the electronic and magnetic properties of the parent compound, reducing the exchange coupling between the Ce and Fe magnetic moments and causing atypical magnetic behavior. Our work is relevant for understanding magnetism in rare-earth-doped YIG and, eventually, may enable a quantitative evaluation of the magneto-optical properties of rare-earth incorporation into YIG. [ABSTRACT FROM AUTHOR]
- Published
- 2017
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17. Superparamagnetism-induced mesoscopic electron focusing in topological insulators.
- Author
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Sessi, P., Rüßmann, P., Bathon, T., Barla, A., Kokh, K. A., Tereshchenko, O. E., Fauth, K., Mahatha, S. K., Valbuena, M. A., Godey, S., Glott, F., Mugarza, A., Gargiani, P., Valvidares, M., Long, N. H., Carbone, C., Mavropoulos, P., Blügel, S., and Bode, M.
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TOPOLOGICAL insulators , *ELECTRONS , *PARAMAGNETISM - Abstract
Recently it has been shown that surface magnetic doping of topological insulators induces backscattering of Dirac states which are usually protected by time-reversal symmetry [Sessi et al., Nat. Commun. 5, 5349 (2014)]. Here we report on quasiparticle interference measurements where, by improved Fermi level tuning, strongly focused interference patterns on surface Mn-doped Bi2Te3 could be directly observed by means of scanning tunneling microscopy at 4 K. Ab initio and model calculations reveal that their mesoscopic coherence relies on two prerequisites: (i) a hexagonal Fermi surface with large parallel segments (nesting) and (ii) magnetic dopants which couple to a high-spin state. Indeed, x-ray magnetic circular dichroism shows superparamagnetism even at very dilute Mn concentrations. Our findings provide evidence of strongly anisotropic Dirac-fermion-mediated interactions and demonstrate how spin information can be transmitted over long distances, allowing the design of experiments and devices based on coherent quantum effects in topological insulators. [ABSTRACT FROM AUTHOR]
- Published
- 2016
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18. Electronic and spin states of SrRuO3 thin films: An x-ray magnetic circular dichroism study.
- Author
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Agrestini, S., Hu, Z., Kuo, C.-Y., Haverkort, M. W., Ko, K.-T., Hollmann, N., Liu, Q., Pellegrin, E., Valvidares, M., Herrero-Martin, J., Gargiani, P., Gegenwart, P., Schneider, M., Esser, S., Tanaka, A., Komarek, A. C., and Tjeng, L. H.
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ELECTRONIC structure , *THIN films , *MAGNETIC circular dichroism , *METAL quenching , *DATA analysis - Abstract
We report a study of the local magnetism in thin films of SrRuO3 grown on (111) and (001) oriented SrTiO3 substrates using x-ray magnetic circular dichroism spectroscopy (XMCD) at the Ru-L2,3 edges. The application of the sum rules to the XMCD data gives an almost quenched orbital moment and a spin moment close to the value expected for the low spin state S=1. Full-multiplet cluster calculations indicate that the low spin state is quite stable and suggest that the occurrence of a transition to the high spin state S=2 in strained thin films of SrRuO3 is unlikely as it would be too expensive in energy. [ABSTRACT FROM AUTHOR]
- Published
- 2015
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19. Band Structure Engineering in 2D Metal-Organic Frameworks.
- Author
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Mearini S, Baranowski D, Brandstetter D, Windischbacher A, Cojocariu I, Gargiani P, Valvidares M, Schio L, Floreano L, Puschnig P, Feyer V, and Schneider CM
- Abstract
The design of 2D metal-organic frameworks (2D MOFs) takes advantage of the combination of the diverse electronic properties of simple organic ligands with different transition metal (TM) centers. The strong directional nature of the coordinative bonds is the basis for the structural stability and the periodic arrangement of the TM cores in these architectures. Here, direct and clear evidence that 2D MOFs exhibit intriguing energy-dispersive electronic bands with a hybrid character and distinct magnetic properties in the metal cores, resulting from the interactions between the TM electronic levels and the organic ligand π-molecular orbitals, is reported. Importantly, a method to effectively tune both the electronic structure of 2D MOFs and the magnetic properties of the metal cores by exploiting the electronic structure of distinct TMs is presented. Consequently, the ionization potential characteristic of selected TMs, particularly the relative energy position and symmetry of the 3d states, can be used to strategically engineer bands within specific metal-organic frameworks. These findings not only provide a rationale for band structure engineering in 2D MOFs but also offer promising opportunities for advanced material design., (© 2024 The Author(s). Advanced Science published by Wiley‐VCH GmbH.)
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- 2024
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20. On-Surface Synthesis of Organolanthanide Sandwich Complexes.
- Author
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Mathialagan SK, Parreiras SO, Tenorio M, Černa L, Moreno D, Muñiz-Cano B, Navío C, Valvidares M, Valbuena MA, Urgel JI, Gargiani P, Miranda R, Camarero J, Martínez JI, Gallego JM, and Écija D
- Abstract
The synthesis of lanthanide-based organometallic sandwich compounds is very appealing regarding their potential for single-molecule magnetism. Here, it is exploited by on-surface synthesis to design unprecedented lanthanide-directed organometallic sandwich complexes on Au(111). The reported compounds consist of Dy or Er atoms sandwiched between partially deprotonated hexahydroxybenzene molecules, thus introducing a distinct family of homoleptic organometallic sandwiches based on six-membered ring ligands. Their structural, electronic, and magnetic properties are investigated by scanning tunneling microscopy and spectroscopy, X-ray absorption spectroscopy, X-ray linear and circular magnetic dichroism, and X-ray photoelectron spectroscopy, complemented by density functional theory-based calculations. Both lanthanide complexes self-assemble in close-packed islands featuring a hexagonal lattice. It is unveiled that, despite exhibiting analogous self-assembly, the erbium-based species is magnetically isotropic, whereas the dysprosium-based compound features an in-plane magnetization., (© 2024 The Authors. Advanced Science published by Wiley‐VCH GmbH.)
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- 2024
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21. 2D Co-Directed Metal-Organic Networks Featuring Strong Antiferromagnetism and Perpendicular Anisotropy.
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Parreiras SO, Martín-Fuentes C, Moreno D, Mathialagan SK, Biswas K, Muñiz-Cano B, Lauwaet K, Valvidares M, Valbuena MA, Urgel JI, Gargiani P, Camarero J, Miranda R, Martínez JI, Gallego JM, and Écija D
- Abstract
Antiferromagnetic spintronics is a rapidly emerging field with the potential to revolutionize the way information is stored and processed. One of the key challenges in this field is the development of novel 2D antiferromagnetic materials. In this paper, the first on-surface synthesis of a Co-directed metal-organic network is reported in which the Co atoms are strongly antiferromagnetically coupled, while featuring a perpendicular magnetic anisotropy. This material is a promising candidate for future antiferromagnetic spintronic devices, as it combines the advantages of 2D and metal-organic chemistry with strong antiferromagnetic order and perpendicular magnetic anisotropy., (© 2023 The Authors. Small published by Wiley‐VCH GmbH.)
- Published
- 2024
- Full Text
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22. Ferromagnetism on an atom-thick & extended 2D metal-organic coordination network.
- Author
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Lobo-Checa J, Hernández-López L, Otrokov MM, Piquero-Zulaica I, Candia AE, Gargiani P, Serrate D, Delgado F, Valvidares M, Cerdá J, Arnau A, and Bartolomé F
- Abstract
Ferromagnetism is the collective alignment of atomic spins that retain a net magnetic moment below the Curie temperature, even in the absence of external magnetic fields. Reducing this fundamental property into strictly two-dimensions was proposed in metal-organic coordination networks, but thus far has eluded experimental realization. In this work, we demonstrate that extended, cooperative ferromagnetism is feasible in an atomically thin two-dimensional metal-organic coordination network, despite only ≈ 5% of the monolayer being composed of Fe atoms. The resulting ferromagnetic state exhibits an out-of-plane easy-axis square-like hysteresis loop with large coercive fields over 2 Tesla, significant magnetic anisotropy, and persists up to T
C ≈ 35 K. These properties are driven by exchange interactions mainly mediated by the molecular linkers. Our findings resolve a two decade search for ferromagnetism in two-dimensional metal-organic coordination networks., (© 2024. The Author(s).)- Published
- 2024
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23. Spectroscopic Evidence of Kondo-Induced Quasiquartet in CeRh_{2}As_{2}.
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Christovam DS, Ferreira-Carvalho M, Marino A, Sundermann M, Takegami D, Melendez-Sans A, Tsuei KD, Hu Z, Rößler S, Valvidares M, Haverkort MW, Liu Y, Bauer ED, Tjeng LH, Zwicknagl G, and Severing A
- Abstract
CeRh_{2}As_{2} is a new multiphase superconductor with strong suggestions for an additional itinerant multipolar ordered phase. The modeling of the low-temperature properties of this heavy-fermion compound requires a quartet Ce^{3+} crystal-field ground state. Here, we provide the evidence for the formation of such a quartet state using x-ray spectroscopy. Core-level photoelectron and x-ray absorption spectroscopy confirm the presence of Kondo hybridization in CeRh_{2}As_{2}. The temperature dependence of the linear dichroism unambiguously reveals the impact of Kondo physics for coupling the Kramer's doublets into an effective quasiquartet. Nonresonant inelastic x-ray scattering data find that the |Γ_{7}^{-}⟩ state with its lobes along the 110 direction of the tetragonal structure (xy orientation) contributes most to the multiorbital ground state of CeRh_{2}As_{2}.
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- 2024
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24. Covalency versus magnetic axiality in Nd molecular magnets: Nd-photoluminescence, strong ligand-field, and unprecedented nephelauxetic effect in fullerenes NdM 2 N@C 80 (M = Sc, Lu, Y).
- Author
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Yang W, Rosenkranz M, Velkos G, Ziegs F, Dubrovin V, Schiemenz S, Spree L, de Souza Barbosa MF, Guillemard C, Valvidares M, Büchner B, Liu F, Avdoshenko SM, and Popov AA
- Abstract
Nd-based nitride clusterfullerenes NdM
2 N@C80 with rare-earth metals of different sizes (M = Sc, Y, Lu) were synthesized to elucidate the influence of the cluster composition, shape and internal strain on the structural and magnetic properties. Single crystal X-ray diffraction revealed a very short Nd-N bond length in NdSc2 N@C80 . For Lu and Y analogs, the further shortening of the Nd-N bond and pyramidalization of the NdM2 N cluster are predicted by DFT calculations as a result of the increased cluster size and a strain caused by the limited size of the fullerene cage. The short distance between Nd and nitride ions leads to a very large ligand-field splitting of Nd3+ of 1100-1200 cm-1 , while the variation of the NdM2 N cluster composition and concomitant internal strain results in the noticeable modulation of the splitting, which could be directly assessed from the well-resolved fine structure in the Nd-based photoluminescence spectra of NdM2 N@C80 clusterfullerenes. Photoluminescence measurements also revealed an unprecedentedly strong nephelauxetic effect, pointing to a high degree of covalency. The latter appears detrimental to the magnetic axiality despite the strong ligand field. As a result, the ground magnetic state has considerable transversal components of the pseudospin g-tensor, and the slow magnetic relaxation of NdSc2 N@C80 could be observed by AC magnetometry only in the presence of a magnetic field. A combination of the well-resolved magneto-optical states and slow relaxation of magnetization suggests that Nd clusterfullerenes can be useful building blocks for magneto-photonic quantum technologies., Competing Interests: There are no conflicts to declare., (This journal is © The Royal Society of Chemistry.)- Published
- 2023
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25. 2D Materials by Design: Intercalation of Cr or Mn between two VSe 2 van der Waals Layers.
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Pathirage V, Khatun S, Lisenkov S, Lasek K, Li J, Kolekar S, Valvidares M, Gargiani P, Xin Y, Ponomareva I, and Batzill M
- Abstract
Insertion of metal layers between layered transition-metal dichalcogenides (TMDs) enables the design of new pseudo-2D nanomaterials. The general premise is that various metal atoms may adopt energetically favorable intercalation sites between two TMD sheets. These covalently bound metals arrange in metastable configurations and thus enable the controlled synthesis of nanomaterials in a bottom-up approach. Here, this method is demonstrated by the insertion of Cr or Mn between VSe
2 layers. Vacuum-deposited transition metals diffuse between VSe2 layers with increasing concentration, arranging in ordered phases. The Cr3+ or Mn2+ ions are in octahedral coordination and thus in a high-spin state. Measured and computed magnetic moments are high for dilute Cr atoms, but with increasing Cr concentration the average magnetic moment decreases, suggesting antiferromagnetic ordering between Cr ions. The many possible combinations of transition metals with TMDs form a library for exploring quantum phenomena in these nanomaterials.- Published
- 2023
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26. Large-Area Synthesis of Ferromagnetic Fe 5- x GeTe 2 /Graphene van der Waals Heterostructures with Curie Temperature above Room Temperature.
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Lv H, da Silva A, Figueroa AI, Guillemard C, Aguirre IF, Camosi L, Aballe L, Valvidares M, Valenzuela SO, Schubert J, Schmidbauer M, Herfort J, Hanke M, Trampert A, Engel-Herbert R, Ramsteiner M, and Lopes JMJ
- Abstract
Van der Waals (vdW) heterostructures combining layered ferromagnets and other 2D crystals are promising building blocks for the realization of ultracompact devices with integrated magnetic, electronic, and optical functionalities. Their implementation in various technologies depends strongly on the development of a bottom-up scalable synthesis approach allowing for realizing highly uniform heterostructures with well-defined interfaces between different 2D-layered materials. It is also required that each material component of the heterostructure remains functional, which ideally includes ferromagnetic order above room temperature for 2D ferromagnets. Here, it is demonstrated that the large-area growth of Fe
5- x GeTe2 /graphene heterostructures is achieved by vdW epitaxy of Fe5- x GeTe2 on epitaxial graphene. Structural characterization confirms the realization of a continuous vdW heterostructure film with a sharp interface between Fe5- x GeTe2 and graphene. Magnetic and transport studies reveal that the ferromagnetic order persists well above 300 K with a perpendicular magnetic anisotropy. In addition, epitaxial graphene on SiC(0001) continues to exhibit a high electronic quality. These results represent an important advance beyond nonscalable flake exfoliation and stacking methods, thus marking a crucial step toward the implementation of ferromagnetic 2D materials in practical applications., (© 2023 The Authors. Small published by Wiley-VCH GmbH.)- Published
- 2023
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27. Spin-Polarization Strategy for Enhanced Acidic Oxygen Evolution Activity.
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Li L, Zhou J, Wang X, Gracia J, Valvidares M, Ke J, Fang M, Shen C, Chen JM, Chang YC, Pao CW, Hsu SY, Lee JF, Ruotolo A, Chin Y, Hu Z, Huang X, and Shao Q
- Abstract
Spin-polarization is known as a promising way to promote the anodic oxygen evolution reaction (OER), since the intermediates and products endow spin-dependent behaviors, yet it is rarely reported for ferromagnetic catalysts toward acidic OER practically used in industry. Herein, the first spin-polarization-mediated strategy is reported to create a net ferromagnetic moment in antiferromagnetic RuO
2 via dilute manganese (Mn2+ ) (S = 5/2) doping for enhancing OER activity in acidic electrolyte. Element-selective X-ray magnetic circular dichroism reveals the ferromagnetic coupling between Mn and Ru ions, fulfilling the Goodenough-Kanamori rule. The ferromagnetism behavior at room temperature can be well interpreted by first principles calculations as the interaction between the Mn2+ impurity and Ru ions. Indeed, Mn-RuO2 nanoflakes exhibit a strongly magnetic field enhanced OER activity, with the lowest overpotential of 143 mV at 10 mA cmgeo -2 and negligible activity decay in 480 h stability (vs 200 mV/195 h without magnetic field) as known for magnetic effects in the literature. The intrinsic turnover frequency is also improved to reach 5.5 s-1 at 1.45 VRHE . This work highlights an important avenue of spin-engineering strategy for designing efficient acidic oxygen evolution catalysts., (© 2023 Wiley-VCH GmbH.)- Published
- 2023
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28. Inducing Single Spin-Polarized Flat Bands in Monolayer Graphene.
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Jugovac M, Cojocariu I, Sánchez-Barriga J, Gargiani P, Valvidares M, Feyer V, Blügel S, Bihlmayer G, and Perna P
- Abstract
Due to the fundamental and technological implications in driving the appearance of non-trivial, exotic topological spin textures and emerging symmetry-broken phases, flat electronic bands in 2D materials, including graphene, are nowadays a relevant topic in the field of spintronics. Here, via europium doping, single spin-polarized bands are generated in monolayer graphene supported by the Co(0001) surface. The doping is controlled by Eu positioning, allowing for the formation of a K ¯ $\bar{\mathrm{K}}$ -valley localized single spin-polarized low-dispersive parabolic band close to the Fermi energy when Eu is on top, and of a π* flat band with single spin character when Eu is intercalated underneath graphene. In the latter case, Eu also induces a bandgap opening at the Dirac point while the Eu 4f states act as a spin filter, splitting the π band into two spin-polarized branches. The generation of flat bands with single spin character, as revealed by the spin- and angle-resolved photoemission spectroscopy (ARPES) experiments, complemented by density functional theory (DFT) calculations, opens up new pathways toward the realization of spintronic devices exploiting such novel exotic electronic and magnetic states., (© 2023 The Authors. Advanced Materials published by Wiley-VCH GmbH.)
- Published
- 2023
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29. Probing of three-dimensional spin textures in multilayers by field dependent X-ray resonant magnetic scattering.
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Burgos-Parra E, Sassi Y, Legrand W, Ajejas F, Léveillé C, Gargiani P, Valvidares M, Reyren N, Cros V, Jaouen N, and Flewett S
- Abstract
In multilayers of magnetic thin films with perpendicular anisotropy, domain walls can take on hybrid configurations in the vertical direction which minimize the domain wall energy, with Néel walls in the top or bottom layers and Bloch walls in some central layers. These types of textures are theoretically predicted, but their observation has remained challenging until recently, with only a few techniques capable of realizing a three dimensional characterization of their magnetization distribution. Here we perform a field dependent X-ray resonant magnetic scattering measurements on magnetic multilayers exploiting circular dichroism contrast to investigate such structures. Using a combination of micromagnetic and X-ray resonant magnetic scattering simulations along with our experimental results, we characterize the three-dimensional magnetic texture of domain walls, notably the thickness resolved characterization of the size and position of the Bloch part in hybrid walls. We also take a step in advancing the resonant scattering methodology by using measurements performed off the multilayer Bragg angle in order to calibrate the effective absorption of the X-rays, and permitting a quantitative evaluation of the out of plane (z) structure of our samples. Beyond hybrid domain walls, this approach can be used to characterize other periodic chiral structures such as skyrmions, antiskyrmions or even magnetic bobbers or hopfions, in both static and dynamic experiments., (© 2023. The Author(s).)
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- 2023
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30. Lanthanide metal-organic network featuring strong perpendicular magnetic anisotropy.
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Parreiras SO, Moreno D, Mathialagan SK, Muñiz-Cano B, Martín-Fuentes C, Tenorio M, Černa L, Urgel JI, Lauwaet K, Valvidares M, Valbuena MA, Gallego JM, Martínez JI, Gargiani P, Miranda R, Camarero J, and Écija D
- Abstract
The coordination of lanthanides atoms in two-dimensional surface-confined metal-organic networks is a promising path to achieve an ordered array of single atom magnets. These networks are highly versatile with plenty of combinations of molecular linkers and metallic atoms. Notably, with an appropriate choice of molecules and lanthanide atoms it should be feasible to tailor the orientation and intensity of the magnetic anisotropy. However, up to now only tilted and almost in-plane easy axis of magnetizations were reported in lanthanide-based architectures. Here we introduce an Er-directed two-dimensional metallosupramolecular network on Cu(111) featuring strong out-of-plane magnetic anisotropy. Our results will contribute to pave avenues for the use of lanthanides in potential applications in nanomagnetism and spintronics.
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- 2023
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31. Intermixing-Driven Surface and Bulk Ferromagnetism in the Quantum Anomalous Hall Candidate MnBi 6 Te 10 .
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Tcakaev AV, Rubrecht B, Facio JI, Zabolotnyy VB, Corredor LT, Folkers LC, Kochetkova E, Peixoto TRF, Kagerer P, Heinze S, Bentmann H, Green RJ, Gargiani P, Valvidares M, Weschke E, Haverkort MW, Reinert F, van den Brink J, Büchner B, Wolter AUB, Isaeva A, and Hinkov V
- Abstract
The recent realizations of the quantum anomalous Hall effect (QAHE) in MnBi
2 Te4 and MnBi4 Te7 benchmark the (MnBi2 Te4 )(Bi2 Te3 )n family as a promising hotbed for further QAHE improvements. The family owes its potential to its ferromagnetically (FM) ordered MnBi2 Te4 septuple layers (SLs). However, the QAHE realization is complicated in MnBi2 Te4 and MnBi4 Te7 due to the substantial antiferromagnetic (AFM) coupling between the SLs. An FM state, advantageous for the QAHE, can be stabilized by interlacing the SLs with an increasing number n of Bi2 Te3 quintuple layers (QLs). However, the mechanisms driving the FM state and the number of necessary QLs are not understood, and the surface magnetism remains obscure. Here, robust FM properties in MnBi6 Te10 (n = 2) with Tc ≈ 12 K are demonstrated and their origin is established in the Mn/Bi intermixing phenomenon by a combined experimental and theoretical study. The measurements reveal a magnetically intact surface with a large magnetic moment, and with FM properties similar to the bulk. This investigation thus consolidates the MnBi6 Te10 system as perspective for the QAHE at elevated temperatures., (© 2023 The Authors. Advanced Science published by Wiley-VCH GmbH.)- Published
- 2023
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32. Giant Exchange-Bias-Like Effect at Low Cooling Fields Induced by Pinned Magnetic Domains in Y 2 NiIrO 6 Double Perovskite.
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Deng Z, Wang X, Wang M, Shen F, Zhang J, Chen Y, Feng HL, Xu J, Peng Y, Li W, Zhao J, Wang X, Valvidares M, Francoual S, Leupold O, Hu Z, Tjeng LH, Li MR, Croft M, Zhang Y, Liu E, He L, Hu F, Sun J, Greenblatt M, and Jin C
- Abstract
Exchange bias (EB) is highly desirable for widespread technologies. Generally, conventional exchange-bias heterojunctions require excessively large cooling fields for sufficient bias fields, which are generated by pinned spins at the interface of ferromagnetic and antiferromagnetic layers. It is crucial for applicability to obtain considerable exchange-bias fields with minimum cooling fields. Here, an exchange-bias-like effect is reported in a double perovskite, Y
2 NiIrO6 , which shows long-range ferrimagnetic ordering below 192 K. It displays a giant bias-like field of 1.1 T with a cooling field of only 15 Oe at 5 K. This robust phenomenon appears below 170 K. This fascinating bias-like effect is the secondary effect of the vertical shifts of the magnetic loops, which is attributed to the pinned magnetic domains due to the combination of strong spin-orbit coupling on Ir, and antiferromagnetically coupled Ni- and Ir-sublattices. The pinned moments in Y2 NiIrO6 are present throughout the full volume, not just at the interface as in conventional bilayer systems., (© 2023 Wiley-VCH GmbH.)- Published
- 2023
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33. Reversal of Anomalous Hall Effect and Octahedral Tilting in SrRuO 3 Thin Films via Hydrogen Spillover.
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Han H, Zhou H, Guillemard C, Valvidares M, Sharma A, Li Y, Sharma AK, Kostanovskiy I, Ernst A, and Parkin SSP
- Abstract
The perovskite SrRuO
3 (SRO) is a strongly correlated oxide whose physical and structural properties are strongly intertwined. Notably, SRO is an itinerant ferromagnet that exhibits a large anomalous Hall effect (AHE) whose sign can be readily modified. Here, a hydrogen spillover method is used to tailor the properties of SRO thin films via hydrogen incorporation. It is found that the magnetization and Curie temperature of the films are strongly reduced and, at the same time, the structure evolves from an orthorhombic to a tetragonal phase as the hydrogen content is increased up to ≈0.9 H per SRO formula unit. The structural phase transition is shown, via in situ crystal truncation rod measurements, to be related to tilting of the RuO6 octahedral units. The significant changes observed in magnetization are shown, via density functional theory (DFT), to be a consequence of shifts in the Fermi level. The reported findings provide new insights into the physical properties of SRO via tailoring its lattice symmetry and emergent physical phenomena via the hydrogen spillover technique., (© 2022 The Authors. Advanced Materials published by Wiley-VCH GmbH.)- Published
- 2023
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34. On-Surface Design of a 2D Cobalt-Organic Network Preserving Large Orbital Magnetic Moment.
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Martín-Fuentes C, Parreiras SO, Urgel JI, Rubio-Giménez V, Muñiz Cano B, Moreno D, Lauwaet K, Valvidares M, Valbuena MA, Gargiani P, Kuch W, Camarero J, Gallego JM, Miranda R, Martínez JI, Martí-Gastaldo C, and Écija D
- Subjects
- Anisotropy, Ligands, Metals, X-Rays, Cobalt chemistry, Magnetics
- Abstract
The design of antiferromagnetic nanomaterials preserving large orbital magnetic moments is important to protect their functionalities against magnetic perturbations. Here, we exploit an archetype H
6 HOTP species for conductive metal-organic frameworks to design a Co-HOTP one-atom-thick metal-organic architecture on a Au(111) surface. Our multidisciplinary scanning probe microscopy, X-ray absorption spectroscopy, X-ray linear dichroism, and X-ray magnetic circular dichroism study, combined with density functional theory simulations, reveals the formation of a unique network design based on threefold Co+2 coordination with deprotonated ligands, which displays a large orbital magnetic moment with an orbital to effective spin moment ratio of 0.8, an in-plane easy axis of magnetization, and large magnetic anisotropy. Our simulations suggest an antiferromagnetic ground state, which is compatible with the experimental findings. Such a Co-HOTP metal-organic network exemplifies how on-surface chemistry can enable the design of field-robust antiferromagnetic materials.- Published
- 2022
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35. Engineering Periodic Dinuclear Lanthanide-Directed Networks Featuring Tunable Energy Level Alignment and Magnetic Anisotropy by Metal Exchange.
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Moreno D, Parreiras SO, Urgel JI, Muñiz-Cano B, Martín-Fuentes C, Lauwaet K, Valvidares M, Valbuena MA, Gallego JM, Martínez JI, Gargiani P, Camarero J, Miranda R, and Écija D
- Abstract
The design of lanthanide multinuclear networks is an emerging field of research due to the potential of such materials for nanomagnetism, spintronics, and quantum information. Therefore, controlling their electronic and magnetic properties is of paramount importance to tailor the envisioned functionalities. In this work, a multidisciplinary study is presented combining scanning tunneling microscopy, scanning tunneling spectroscopy, X-ray absorption spectroscopy, X-ray linear dichroism, X-ray magnetic circular dichroism, density functional theory, and multiplet calculations, about the supramolecular assembly, electronic and magnetic properties of periodic dinuclear 2D networks based on lanthanide-pyridyl interactions on Au(111). Er- and Dy-directed assemblies feature identical structural architectures stabilized by metal-organic coordination. Notably, despite exhibiting the same +3 oxidation state, there is a shift of the energy level alignment of the unoccupied molecular orbitals between Er- and Dy-directed networks. In addition, there is a reorientation of the easy axis of magnetization and an increment of the magnetic anisotropy when the metallic center is changed from Er to Dy. Thus, the results show that it is feasible to tune the energy level alignment and magnetic anisotropy of a lanthanide-based metal-organic architecture by metal exchange, while preserving the network design., (© 2022 The Authors. Small published by Wiley-VCH GmbH.)
- Published
- 2022
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36. Correction to "Disclosing the Nature of Asymmetric Interface Magnetism in Co/Pt Multilayers".
- Author
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Verna A, Alippi P, Offi F, Barucca G, Varvaro G, Agostinelli E, Albrecht M, Rutkowski B, Ruocco A, Paoloni D, Valvidares M, and Laureti S
- Published
- 2022
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37. Control of Oxygen Vacancy Ordering in Brownmillerite Thin Films via Ionic Liquid Gating.
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Han H, Sharma A, Meyerheim HL, Yoon J, Deniz H, Jeon KR, Sharma AK, Mohseni K, Guillemard C, Valvidares M, Gargiani P, and Parkin SSP
- Abstract
Oxygen defects and their atomic arrangements play a significant role in the physical properties of many transition metal oxides. The exemplary perovskite SrCoO
3-δ ( P- SCO) is metallic and ferromagnetic. However, its daughter phase, the brownmillerite SrCoO2.5 ( BM- SCO), is insulating and an antiferromagnet. Moreover, BM- SCO exhibits oxygen vacancy channels (OVCs) that in thin films can be oriented either horizontally ( H -SCO) or vertically ( V -SCO) to the film's surface. To date, the orientation of these OVCs has been manipulated by control of the thin film deposition parameters or by using a substrate-induced strain. Here, we present a method to electrically control the OVC ordering in thin layers via ionic liquid gating (ILG). We show that H -SCO (antiferromagnetic insulator, AFI) can be converted to P -SCO (ferromagnetic metal, FM) and subsequently to V -SCO (AFI) by the insertion and subtraction of oxygen throughout thick films via ILG. Moreover, these processes are independent of substrate-induced strain which favors formation of H -SCO in the as-deposited film. The electric-field control of the OVC channels is a path toward the creation of oxitronic devices.- Published
- 2022
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38. Disclosing the Nature of Asymmetric Interface Magnetism in Co/Pt Multilayers.
- Author
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Verna A, Alippi P, Offi F, Barucca G, Varvaro G, Agostinelli E, Albrecht M, Rutkowski B, Ruocco A, Paoloni D, Valvidares M, and Laureti S
- Abstract
Nowadays, a wide number of applications based on magnetic materials rely on the properties arising at the interface between different layers in complex heterostructures engineered at the nanoscale. In ferromagnetic/heavy metal multilayers, such as the [Co/Pt]
N and [Co/Pd]N systems, the magnetic proximity effect was demonstrated to be asymmetric, thus inducing a magnetic moment on the Pt (Pd) layer that is typically higher at the top Co/Pt(Pd) interface. In this work, advanced spectroscopic and imaging techniques were combined with theoretical approaches to clarify the origin of this asymmetry both in Co/Pt trilayers and, for the first time, in multilayer systems that are more relevant for practical applications. The different magnetic moment induced at the Co/Pt interfaces was correlated to the microstructural features that are in turn affected by the growth processes that induce a different intermixing during the film deposition, thus influencing the interface magnetic profile.- Published
- 2022
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39. Intrinsic 2D-XY ferromagnetism in a van der Waals monolayer.
- Author
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Bedoya-Pinto A, Ji JR, Pandeya AK, Gargiani P, Valvidares M, Sessi P, Taylor JM, Radu F, Chang K, and Parkin SSP
- Abstract
The physics and universality scaling of phase transitions in low-dimensional systems has historically been a topic of great interest. Recently, two-dimensional (2D) materials exhibiting intriguing long-range magnetic order have been in the spotlight. Although an out-of-plane anisotropy has been shown to stabilize 2D magnetic order, the demonstration of a 2D magnet with in-plane rotational symmetry has remained elusive. We constructed a nearly ideal easy-plane system, a single CrCl
3 monolayer on graphene/6H-SiC(0001), and observed robust ferromagnetic ordering with critical scaling characteristic of a 2D-XY system. These observations indicate the realization of a finite-size Berezinskii-Kosterlitz-Thouless phase transition in a large-area, quasi–free-standing van der Waals monolayer magnet with an XY universality class. This offers a material platform to host 2D superfluid spin transport and topological magnetic textures.- Published
- 2021
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40. Correction to "Imaging Nanometer Phase Coexistence at Defects During the Insulator-Metal Phase Transformation in VO 2 Thin Films by Resonant Soft X-ray Holography".
- Author
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Vidas L, Günther CM, Miller TA, Pfau B, Perez-Salinas D, Martínez E, Schneider M, Gührs E, Gargiani P, Valvidares M, Marvel RE, Hallman KA, Haglund RF Jr, Eisebitt S, and Wall S
- Published
- 2021
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41. Voltage control of ferrimagnetic order and voltage-assisted writing of ferrimagnetic spin textures.
- Author
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Huang M, Hasan MU, Klyukin K, Zhang D, Lyu D, Gargiani P, Valvidares M, Sheffels S, Churikova A, Büttner F, Zehner J, Caretta L, Lee KY, Chang J, Wang JP, Leistner K, Yildiz B, and Beach GSD
- Abstract
Voltage control of magnetic order is desirable for spintronic device applications, but 180° magnetization switching is not straightforward because electric fields do not break time-reversal symmetry. Ferrimagnets are promising candidates for 180° switching owing to a multi-sublattice configuration with opposing magnetic moments of different magnitudes. In this study we used solid-state hydrogen gating to control the ferrimagnetic order in rare earth-transition metal thin films dynamically. Electric field-induced hydrogen loading/unloading in GdCo can shift the magnetic compensation temperature by more than 100 K, which enables control of the dominant magnetic sublattice. X-ray magnetic circular dichroism measurements and ab initio calculations indicate that the magnetization control originates from the weakening of antiferromagnetic exchange coupling that reduces the magnetization of Gd more than that of Co upon hydrogenation. We observed reversible, gate voltage-induced net magnetization switching and full 180° Néel vector reversal in the absence of external magnetic fields. Furthermore, we generated ferrimagnetic spin textures, such as chiral domain walls and skyrmions, in racetrack devices through hydrogen gating. With gating times as short as 50 μs and endurance of more than 10,000 cycles, our method provides a powerful means to tune ferrimagnetic spin textures and dynamics, with broad applicability in the rapidly emerging field of ferrimagnetic spintronics., (© 2021. The Author(s), under exclusive licence to Springer Nature Limited.)
- Published
- 2021
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42. Tuning the Magnetic Anisotropy of Lanthanides on a Metal Substrate by Metal-Organic Coordination.
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Parreiras SO, Moreno D, Cirera B, Valbuena MA, Urgel JI, Paradinas M, Panighel M, Ajejas F, Niño MA, Gallego JM, Valvidares M, Gargiani P, Kuch W, Martínez JI, Mugarza A, Camarero J, Miranda R, Perna P, and Écija D
- Abstract
Taming the magnetic anisotropy of lanthanides through coordination environments is crucial to take advantage of the lanthanides properties in thermally robust nanomaterials. In this work, the electronic and magnetic properties of Dy-carboxylate metal-organic networks on Cu(111) based on an eightfold coordination between Dy and ditopic linkers are inspected. This surface science study based on scanning probe microscopy and X-ray magnetic circular dichroism, complemented with density functional theory and multiplet calculations, reveals that the magnetic anisotropy landscape of the system is complex. Surface-supported metal-organic coordination is able to induce a change in the orientation of the easy magnetization axis of the Dy coordinative centers as compared to isolated Dy atoms and Dy clusters, and significantly increases the magnetic anisotropy. Surprisingly, Dy atoms coordinated in the metallosupramolecular networks display a nearly in-plane easy magnetization axis despite the out-of-plane symmetry axis of the coordinative molecular lattice. Multiplet calculations highlight the decisive role of the metal-organic coordination, revealing that the tilted orientation is the result of a very delicate balance between the interaction of Dy with O atoms and the precise geometry of the crystal field. This study opens new avenues to tailor the magnetic anisotropy and magnetic moments of lanthanide elements on surfaces., (© 2021 The Authors. Small published by Wiley-VCH GmbH.)
- Published
- 2021
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43. Large intrinsic anomalous Hall effect in SrIrO 3 induced by magnetic proximity effect.
- Author
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Yoo MW, Tornos J, Sander A, Lin LF, Mohanta N, Peralta A, Sanchez-Manzano D, Gallego F, Haskel D, Freeland JW, Keavney DJ, Choi Y, Strempfer J, Wang X, Cabero M, Vasili HB, Valvidares M, Sanchez-Santolino G, Gonzalez-Calbet JM, Rivera A, Leon C, Rosenkranz S, Bibes M, Barthelemy A, Anane A, Dagotto E, Okamoto S, Te Velthuis SGE, Santamaria J, and Villegas JE
- Abstract
The anomalous Hall effect (AHE) is an intriguing transport phenomenon occurring typically in ferromagnets as a consequence of broken time reversal symmetry and spin-orbit interaction. It can be caused by two microscopically distinct mechanisms, namely, by skew or side-jump scattering due to chiral features of the disorder scattering, or by an intrinsic contribution directly linked to the topological properties of the Bloch states. Here we show that the AHE can be artificially engineered in materials in which it is originally absent by combining the effects of symmetry breaking, spin orbit interaction and proximity-induced magnetism. In particular, we find a strikingly large AHE that emerges at the interface between a ferromagnetic manganite (La
0.7 Sr0.3 MnO3 ) and a semimetallic iridate (SrIrO3 ). It is intrinsic and originates in the proximity-induced magnetism present in the narrow bands of strong spin-orbit coupling material SrIrO3 , which yields values of anomalous Hall conductivity and Hall angle as high as those observed in bulk transition-metal ferromagnets. These results demonstrate the interplay between correlated electron physics and topological phenomena at interfaces between 3d ferromagnets and strong spin-orbit coupling 5d oxides and trace an exciting path towards future topological spintronics at oxide interfaces.- Published
- 2021
- Full Text
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44. Magnetism at the interface of non-magnetic Cu and C 60 .
- Author
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Sharangi P, Gargiani P, Valvidares M, and Bedanta S
- Abstract
The signature of magnetism without a ferromagnet in a non-magnetic heterostructure is novel as well as fascinating from a fundamental research point of view. It has been shown by Al'Mari et al. that magnetism can be induced at the interface of Cu/C
60 due to a change in the density of states. However, the quantification of such an interfacial magnetic moment has not been performed yet. In order to quantify the induced magnetic moment in Cu, we have performed X-ray magnetic circular dichroism (XMCD) measurements on Cu/C60 multilayers. We have observed room temperature ferromagnetism in the Cu/C60 stack. Further XMCD measurements show that a ∼0.01 μB per atom magnetic moment has been induced in Cu at the Cu/C60 interface.- Published
- 2021
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45. Absence of Magnetic Proximity Effect at the Interface of Bi_{2}Se_{3} and (Bi,Sb)_{2}Te_{3} with EuS.
- Author
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Figueroa AI, Bonell F, Cuxart MG, Valvidares M, Gargiani P, van der Laan G, Mugarza A, and Valenzuela SO
- Abstract
We performed x-ray magnetic circular dichroism (XMCD) measurements on heterostructures comprising topological insulators (TIs) of the (Bi,Sb)_{2}(Se,Te)_{3} family and the magnetic insulator EuS. XMCD measurements allow us to investigate element-selective magnetic proximity effects at the very TI/EuS interface. A systematic analysis reveals that there is neither significant induced magnetism within the TI nor an enhancement of the Eu magnetic moment at such interface. The induced magnetic moments in Bi, Sb, Te, and Se sites are lower than the estimated detection limit of the XMCD measurements of ∼10^{-3} μ_{B}/at.
- Published
- 2020
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46. A New Highly Anisotropic Rh-Based Heusler Compound for Magnetic Recording.
- Author
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He Y, Fecher GH, Fu C, Pan Y, Manna K, Kroder J, Jha A, Wang X, Hu Z, Agrestini S, Herrero-Martín J, Valvidares M, Skourski Y, Schnelle W, Stamenov P, Borrmann H, Tjeng LH, Schaefer R, Parkin SSP, Coey JMD, and Felser C
- Abstract
The development of high-density magnetic recording media is limited by superparamagnetism in very small ferromagnetic crystals. Hard magnetic materials with strong perpendicular anisotropy offer stability and high recording density. To overcome the difficulty of writing media with a large coercivity, heat-assisted magnetic recording was developed, rapidly heating the media to the Curie temperature T
c before writing, followed by rapid cooling. Requirements are a suitable Tc , coupled with anisotropic thermal conductivity and hard magnetic properties. Here, Rh2 CoSb is introduced as a new hard magnet with potential for thin-film magnetic recording. A magnetocrystalline anisotropy of 3.6 MJ m-3 is combined with a saturation magnetization of μ0 Ms = 0.52 T at 2 K (2.2 MJ m-3 and 0.44 T at room temperature). The magnetic hardness parameter of 3.7 at room temperature is the highest observed for any rare-earth-free hard magnet. The anisotropy is related to an unquenched orbital moment of 0.42 μB on Co, which is hybridized with neighboring Rh atoms with a large spin-orbit interaction. Moreover, the pronounced temperature dependence of the anisotropy that follows from its Tc of 450 K, together with a thermal conductivity of 20 W m-1 K-1 , make Rh2 CoSb a candidate for the development of heat-assisted writing with a recording density in excess of 10 Tb in.-2 ., (© 2020 The Authors. Published by Wiley-VCH GmbH.)- Published
- 2020
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47. Molecular Approach for Engineering Interfacial Interactions in Magnetic/Topological Insulator Heterostructures.
- Author
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Cuxart MG, Valbuena MA, Robles R, Moreno C, Bonell F, Sauthier G, Imaz I, Xu H, Nistor C, Barla A, Gargiani P, Valvidares M, Maspoch D, Gambardella P, Valenzuela SO, and Mugarza A
- Abstract
Controlling interfacial interactions in magnetic/topological insulator heterostructures is a major challenge for the emergence of novel spin-dependent electronic phenomena. As for any rational design of heterostructures that rely on proximity effects, one should ideally retain the overall properties of each component while tuning interactions at the interface. However, in most inorganic interfaces, interactions are too strong, consequently perturbing, and even quenching, both the magnetic moment and the topological surface states at each side of the interface. Here, we show that these properties can be preserved using ligand chemistry to tune the interaction of magnetic ions with the surface states. By depositing Co-based porphyrin and phthalocyanine monolayers on the surface of Bi
2 Te3 thin films, robust interfaces are formed that preserve undoped topological surface states as well as the pristine magnetic moment of the divalent Co ions. The selected ligands allow us to tune the interfacial hybridization within this weak interaction regime. These results, which are in stark contrast with the observed suppression of the surface state at the first quintuple layer of Bi2 Se3 induced by the interaction with Co phthalocyanines, demonstrate the capability of planar metal-organic molecules to span interactions from the strong to the weak limit.- Published
- 2020
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48. The Synthesis of a Quasi-One-Dimensional Iron-Based Telluride with Antiferromagnetic Chains and a Spin Glass State.
- Author
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Zhang J, Duan L, Wang Z, Wang X, Zhao J, Jin M, Li W, Zhang C, Cao L, Deng Z, Hu Z, Agrestini S, Valvidares M, Lin HJ, Chen CT, Zhu J, and Jin C
- Abstract
The report on the superconductivity of the two-legged spin ladders BaFe
2 S3 and BaFe2 Se3 has established 123-type iron chalcogenides as a novel subgroup in the iron-based superconductor family and has stimulated the continuous exploration of other iron-based materials with new structures and potentially novel properties. In this paper, we report the systematic study of a new quasi-one-dimensional (1D) iron-based compound, Ba9 Fe3 Te15 , including its synthesis and magnetic properties. The high-pressure synthesized Ba9 Fe3 Te15 crystallized in a hexagonal structure that mainly consisted of face-sharing FeTe6 octahedral chains running along the c axis, with a lattice constant of a = 10.23668 Å; this led to weak interchain coupling and an enhanced one-dimensionality. The systematic static and dynamic magnetic properties were comprehensively studied experimentally. The dc magnetic susceptibility showed typical 1D antiferromagnetic characteristics, with a Tmax at 190 K followed by a spin glass (SG) state with freezing at Tf ≈ 6.0 K, which were also unambiguously proved by ac susceptibility measurements. Additionally, X-ray magnetic circular dichroism (XMCD) experiments revealed an unexpected orbital moment for Fe2+ , i.e., 0.84 μB per Fe in Ba9 Fe3 Te15 . The transport property is electrically insulating, with a thermal activation gap of 0.32 eV. These features mark Ba9 Fe3 Te15 as an alternative type of iron-based compound, providing a diverse candidate for high-pressure studies in order to pursue some emerging physics.- Published
- 2020
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49. Reversible spin storage in metal oxide-fullerene heterojunctions.
- Author
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Moorsom T, Rogers M, Scivetti I, Bandaru S, Teobaldi G, Valvidares M, Flokstra M, Lee S, Stewart R, Prokscha T, Gargiani P, Alosaimi N, Stefanou G, Ali M, Al Ma'Mari F, Burnell G, Hickey BJ, and Cespedes O
- Abstract
We show that hybrid MnO
x /C60 heterojunctions can be used to design a storage device for spin-polarized charge: a spin capacitor. Hybridization at the carbon-metal oxide interface leads to spin-polarized charge trapping after an applied voltage or photocurrent. Strong electronic structure changes, including a 1-eV energy shift and spin polarization in the C60 lowest unoccupied molecular orbital, are then revealed by x-ray absorption spectroscopy, in agreement with density functional theory simulations. Muon spin spectroscopy measurements give further independent evidence of local spin ordering and magnetic moments optically/electronically stored at the heterojunctions. These spin-polarized states dissipate when shorting the electrodes. The spin storage decay time is controlled by magnetic ordering at the interface, leading to coherence times of seconds to hours even at room temperature., (Copyright © 2020 The Authors, some rights reserved; exclusive licensee American Association for the Advancement of Science. No claim to original U.S. Government Works. Distributed under a Creative Commons Attribution License 4.0 (CC BY).)- Published
- 2020
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50. Interfacial Dzyaloshinskii-Moriya interaction arising from rare-earth orbital magnetism in insulating magnetic oxides.
- Author
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Caretta L, Rosenberg E, Büttner F, Fakhrul T, Gargiani P, Valvidares M, Chen Z, Reddy P, Muller DA, Ross CA, and Beach GSD
- Abstract
The Dzyaloshinskii-Moriya interaction (DMI) is responsible for exotic chiral and topological magnetic states such as spin spirals and skyrmions. DMI manifests at metallic ferromagnet/heavy-metal interfaces, owing to inversion symmetry breaking and spin-orbit coupling by a heavy metal such as Pt. Moreover, in centrosymmetric magnetic oxides interfaced by Pt, DMI-driven topological spin textures and fast current-driven dynamics have been reported, though the origin of this DMI is unclear. While in metallic systems, spin-orbit coupling arises from a proximate heavy metal, we show that in perpendicularly-magnetized iron garnets, rare-earth orbital magnetism gives rise to an intrinsic spin-orbit coupling generating interfacial DMI at mirror symmetry-breaking interfaces. We show that rare-earth ion substitution and strain engineering can significantly alter the DMI. These results provide critical insights into the origins of chiral magnetism in low-damping magnetic oxides and identify paths toward engineering chiral and topological states in centrosymmetric oxides through rare-earth ion substitution.
- Published
- 2020
- Full Text
- View/download PDF
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