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Inducing magnetism in graphene has been an important challenge since its discovery. In the dilute regime, magnetic impurities are expected to couple to the Dirac electrons via the Kondo effect in a paramagnetic phase. In the less dilute regime, magnetic impurities in graphene may develop long-range magnetic order mediated by the conduction electrons via the Ruderman-Kittel-Kasuya-Yoshida (RKKY) interaction. Today, the Kondo and RKKY-exchange physics of Dirac electrons in graphene is still elusive while theory predicts competition between a non-trivial Kondo unscreened phase against a RKKY-coupled phase. Considerable experimental efforts have been devoted in this context, with the local magnetic moments originating from carbon vacancies, from adsorption and intercalation (of atoms, clusters or molecules), and from substitutional foreign atoms. Here, we report the incorporation of substitutional manganese (Mn) atoms into graphene as a model case of magnetic doping with transition metals. Ultra-low energy (ULE) ion implantation allows us to precisely tune the kinetic energy of Mn ions, providing control over the form of incorporation and concentration while preserving the structural and electronic properties of graphene [1]. Using low-temperature scanning tunneling microscopy (LT-STM) together with density functional theory (DFT), we identified and characterized point defects that are associated with substitutional-Mn in a carbon single vacancy (Fig.1). These results are complemented by synchrotron-based X-ray photoelectron spectroscopy (XPS), angle-resolved photoemission spectroscopy (ARPES), Raman spectroscopy, X-ray magnetic circular dichroism (XMCD), among others. The new insights provided by our work establish a framework for the controlled incorporation of magnetic dopants in graphene and other 2D materials, using ULE ion implantation.References: [1] P. Willke et al., Appl. Phys. Lett. 105, (2014), 111605

MMM 2020

Magnetic doping of graphene with substitutional manganese atoms

The 65th Annual Conference on Magnetism and Magnetic Materials (MMM 2020) was held in a virtual form. The COVID-19 pandemic, with its associated uncertainty about international travel and the ability to gather in large groups, meant that the Steering Committee decided to cancel the face-to-face meeting that had been planned in Palm Beach, Florida November 2-6, 2020.

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technical paper

Ionic modulations of magnetic properties, controlled by a low voltage, are attractive for future energy efficient magnetic devices. [1,2] We study the magneto-ionic control of thin iron films with uniaxial in-plane anisotropy, which is induced by oblique sputtering. The polycrystalline iron films are natively oxidized to yield iron oxide/iron films suitable for magneto-ionic manipulation by electrolytic gating in alkaline electrolyte. [3] Angle resolved magnetic measurements reveal a uniaxial anisotropy (Fig.1 ). In the pristine state (Fig. 1a,b, black curves), the remanence and coercivity along the hard axis are enhanced, due to the formation of a blocked magnetic state resulting from interactions of the charged Néel walls. [4] A voltage-controlled transformation of the FeOx layer into metallic Fe upon electrolytic gating leads to a drastic decrease in coercivity in all directions (Fig. 1a, blue curve). At the same time, the remanence remains unchanged for angles close to the easy axis but almost vanishes in the vicinity of the hard axis upon the reduction process (Fig. 1b, blue curve). Anhysteretic measurements along the hard axis revealed that the anisotropy increases upon voltage application. The unexpected finding of an inverse anisotropy-coercivity relationship is further studied by investigating the magnetic microstructure by in-situ Kerr microscopy. We find a significant increase in domain size by 60% upon reduction. We attribute the observed coarsening of the magnetic microstructure to the anisotropy-related increase in the domain wall energy. At the same time, the anisotropy increase causes a decrease of the Néel wall tails. Both effects will result in a weakening of the Néel wall interactions during voltage application, which can explain the observed magnetic de-blocking, and thus, the collapse of remanence and coercivity. [5]References: [1] C. Navarro-Senent, A. Quintana, E. Menéndez, E. Pellicer, and J. Sort, APL Materials 7, 030701 (2019). [2] A. Molinari, H. Hahn, and R. Kruk, Advanced Materials 31, 1806662 (2019). [3] K. Duschek, M. Uhlemann, H. Schlörb, K. Nielsch, and K. Leistner, Electrochemistry Communications 72, 153 (2016). [4] A. Hubert and R. Schäfer, Magnetic Domains (Springer Berlin Heidelberg, Berlin, Heidelberg, 1998). [5] J. Zehner, I. Soldatov, S. Schneider, R. Heller, N. B. Khojasteh, S. Schiemenz, S. Fähler, K. Nielsch, R. Schäfer, K. Leistner, submitted

Voltage control of Néel wall interaction in thin films with uniaxial in-plane anisotropy

Multiferroics that show coupling between electric and magnetic properties are promising materials for devices that transform information from one state into another, such as spin excitations into charge, phonons or photons. Among them, BiFeO3 (BFO) is one of the very few compound displaying room temperature multiferroicity. BFO leads for example to spectacular THz electromagnetic wave generation and photostriction properties. The prospects for applications in this area such as optically triggered piezotransducers require a perfect knowledge of the elastic properties of materials. Combining Time Resolved Acoustic Measurements (TRAM) with density functional theory (DFT) calculations and volumic and surface mode propagations simulations, we have studied the elastic properties of BiFeO3. Using TRAM, we have measured wave propagation along 3 differents directions in the (110) plane of BFO. Then, we determined three modes speeds : one longitudinal mode, one fast and one slow transverse modes. With DFT, we calculated a set of elastic constants for BiFeO3. We used these elastic constants to simulate the propagation of volumic and surface modes. The comparison between the calculated and measured speeds enables to ajust the elastic constants. In conclusion, we have been able to fully determine the elastic constant of BiFeO3 that are essential for future integration of BFO in acoustic micro/nano-devices.

Elastic properties of the multiferroic BiFeO3 by Time Resolved Acoustic Measurements

We present novel piezo-ionic/magnetostrictive bi-layer composites for energy generation systems. These structures, fabricated with Metglas® 2826MB ferromagnetic alloys and ionic liquid based PVDF-HFP polymer composites, show an induced electric response as a consequence of the coupling between the magnetostrictive properties of the Metglas® 2826MB and the piezo-ionic ones of the ionic liquid based PVDF-HFP polymer composites. These flexible, simple and low cost structures do not need to be polarized to exhibit an electric response, and show an increased induced voltage as the percentage of the ionic liquid in the PVDF-HFP matrix does. This response is a consequence of the asymmetric deformation caused by the magnetostrictive material on the piezo-ionic composite, which induces a non-uniform distribution of the cations and anions in the polymer matrix. The laminates present a maximum response under the application of a low magnetic fields of 9 Oe, and a normalized magneto-ionic coefficient values up to 130 mV/cm.Oe at 60 kHz for the structure with an ionic liquid content of 30 %. These values are even higher than others obtained with piezoelectric materials based ME composites [1][2]. The simple fabrication process and potentiality of these new piezo-ionic/magnetostrictive laminates contributes to broaden and improve the state of the art of the energy generation systems. [1] P. Galizia, M. Algueró, N. Bernier, N. Gambacorti, E. Aza, A. Lappas, M. Venet and C. Galassi, J. Alloys Compd., vol. 783, p.237–45 (2019) [2] Y. Kumar, K.L. Yadav, J. Shah and R.K. Kotnala, J. Adv. Ceram., vol. 8, p.333–44 (2019)

Magneto-Ionic Effect in Piezo-Ionic/Magnetostrictive Composites for Energy Generation Applications

Multiferroics attracts great attention in the present time due to their very promising technological applications. In the so-called multiferroics of spin origin [1] phenomenon of giant magnetoelectric response was observed [2,3]. Two mechanisms of magnetic ordering induced ferroelectricity, namely inverse Dzyaloshinskii-Moriya and spin-dependent p-d hybridization, imply noncollinear magnetic structure [1], which can appear for example due to the frustration of exchange interaction. This makes research on such incommensurate spin structures as helicoids very important since their properties determine electric polarization. Recently we propose a theoretical description of spiral plane flops in anisotropic frustrated helimagnets [4]. Using smallness of anisotropic interactions in comparison with the exchange one, energies of competing spin textures were described perturbatively and simple equations for the flop fields were derived. Notably, formulas have a similar form with the spin-flop field in uniaxial antiferromagnets. Moreover, the theory was successfully applied to the experimental data on several magnets. In the present research, we further proceed with the theoretical study of anisotropic frustrated antiferromagnets [5]. We show, that if there is competing commensurate spin ordering along with two conventional phase transitions at small magnetic fields (spin-flop and spiral pane flop, see Fig.1 (a) and (b)) there appears a possibility to induce helical ordering using an external magnetic field (see Fig.1 (c), (d) and (e)). We propose and describe theoretically three sequences of phase transitions, where at zero field conventional antiferromagnetic ordering is the ground state. We successfully apply our approach for the description of phase transitions in MnWO4 [6] (scenario shown in Fig. 1 (c)). Furthermore, the scenario shown in Fig. 1 (e) was observed experimentally in Ref. [7] after our research was published. To the best of our knowledge, scenario Fig. 1 (d) has not been found yet and it seems to be an interesting experimental problem.References: [1] Y. Tokura, S. Seki, and N. Nagaosa, Rep. Prog. Phys. 77, 076501 (2014), and references therein [2] S.-W. Cheong and M. Mostovoy, Nat. Mater. 6, 13 (2007), and references therein. [3] Y. Tokura and S. Seki, Adv. Mater. 22, 1554 (2009). [4] O. I. Utesov and A. V. Syromyatnikov, Phys. Rev. B 98, 184406 (2018). [5] O. I. Utesov and A. V. Syromyatnikov, Phys. Rev. B 100, 054439 (2019). [6] M. V. Gvozdikova, T. Ziman, and M. E. Zhitomirsky, Phys. Rev. B 94, 020406(R) (2016). [7] J. Lass, et. al., Phys. Rev. B 101, 054415 (2020).

Formation of Spiral Ordering by Magnetic Field in Frustrated Anisotropic Antiferromagnets

LuFeO3 (LFO) a member of the orthoferrite (RFeO3) family, holds the promise of replacing the well-known room temperature multiferroic, BiFeO3 [1]. LFO nanoparticles with and without Ho doping (i.e., Lu1-xHoxFeO3 with 0 ≤ x ≤ 1) were synthesized using the hydrothermal method [2]. Rietveld refinement of the XRD data (Fig.1) for x = 0 (0.05) reveal the presence of both the hexagonal (h) P63cm and orthorhombic (o) Pnma phase fractions as 96% (6%) and 4% (94%), respectively. Further Ho doping resulted in pure o- structure. The lattice parameters (a, b, c) follow Vegard’s law ensuring the replacement of Lu atoms by Ho atoms. The common characteristics of o- RFeO3 are i) negligible ferroelectric polarization, ii) ordering of Fe3+ moments antiferromagnetically via Fe3+-O2--Fe3+ super-exchange interaction in ac plane and net magnetic moment along b direction for T < TN1 ≈ 600 K, iii) ordering of R3+ moments at T < TN2 ≈ 10 K, iv) possible re-orientation of spins (SR) from b to c direction between TN1 and TN2 owing to the R3+-O2--Fe3+ interaction [3, 4]. To understand the effect of Ho doping on the magnetic properties of Lu1-xHoxFeO3 with 0 ≤ x ≤ 1, the magnetization (M) has been measured as a function of temperature at a magnetic field of 100 Oe in both the zero-field-cooled (ZFC) and field-cooled (FC) modes (Fig.2). For x = 0, the SR is observed at 120 K. In this case, the SR is attributed to h- LFO since in o- LFO, no SR has been reported [5, 6]. For x = 0.05, SR could not be observed even at the lowest measurement temperature of 3 K presumably due to the weak R3+-O2--Fe3+ interaction. Further increase in Ho concentration progressively strengthens the R3+-O2--Fe3+ interaction and hence TSR shifts to higher temperatures with increasing x, as shown in Fig.2. When the M due to Fe3+ moments is equal and opposite to M due to Ho3+ moments, compensation (comp) occurs and the net M goes to zero. For x = 0.3 to 0.6, Tcomp is found to increase with Ho concentration. This study establishes that the Ho doping stabilizes O-structure beyond x > 0.05 and increases the TSR from 0 in o-LFO to 57.8 ± 0.2 K in o-HFO.References: 1. Chowdhury, U. et al. 1–12 (2017). 2. Leelashree, S et al.. J. Supercond. Nov. Magn. (2019) doi:10.1007/s10948-019-5114-4. 3. Zhou, Z et al.. J. Alloys Compd. 583, 21–31 (2014). 4. Yamaguchi, T. J. Phys. Chem. Solids 35, 479–500 (1974). 5. Liu, J. et al. Adv. Funct. Mater. 28, 1–7 (2018). 6. Zhu, W, et al.. Appl. Phys. Lett. 100, 4–8 (2012).

Ho doping induced spin reorientation in O- Lu1-xHoxFeO3 (x = 0 to 1)

Europium chromite (EuCrO3) is a multifunctional material presenting physical and chemical properties that are strongly influenced by the rare-earth ion lying on the A-site of an orthorhombic distorted perovskite structure [1]. EuCrO3 does also present a variety of spin interactions that are highly dependent on temperature (T), leading to a spin-canting antiferromagnetic phase with a Néel temperature (TN) close to about 170 K [2]. In the present work, the dynamics of the spins and the structural parameters of as prepared and thermal treated (T = 1073 K, time = 24 h) samples of Eu1−xFexCrO3 (x = 0, 0.10 and 0.20) were investigated. The ac-magnetic susceptibility (χac) was measured near TN for frequencies (f) in the range 10-104 Hz, magnitude of the ac magnetic field of 10 Oe and for 5 ≤ T ≤ 300 K. X-ray diffraction data were used for measuring the lattice parameters (a, b and c) and the bonding angle θB (Cr3+–O(2)–Cr3+), for 100 ≤ T ≤ 300 K. The maximum in χac was found to shift to higher values of T for increasing values of f. The Voguel-Fulcher law was used for analyzing χac yielding values for the characteristic relaxation time τ0, activation energy Ea/kB and TG, respectively, in the ranges 1.1 - 4.2 ns (3.1 - 3.6 ps), 29.4 - 45.5 K (46.5 - 47.2 K) and 159 - 166 K (170 -173 K) for the as prepared (thermal treated) samples. The super-exchange parameter J ~ cos4[(180-θB)/2]/d7, where d is the length of the Cr-O(2) bound [3], was also obtained for both as prepared and thermal treated samples yielding a good correlation of the values of J with the corresponding ones of TG. Work partially supported by CNPq, CAPES, FACEPE and FINEP (Brazilian Agencies).References: 1 - J. M. Marín Ramírez, H. V. S. Pessoni, A. Franco Jr. and F.L.A. Machado, J. Alloys Compd., Vol. 690, p.315 (2017). 2 - D. R. Ratkovski, J. M. Marín Ramírez, P. R. T. Ribeiro et all., J. Alloys Compd., Vol. 724, p.501 (2017). 3 - J. S. Zhou and J. B. Goodenough, Phys. Rev. B, Vol. 77, p.132104 (2008).

On the Correlation of the Magnetic Properties with the Structural Parameters in Fe-doped Europium Chromite

A variety of chemical and physical procedures could be used for synthesis of magnetic nanoparticles. However, these methods are fraught with many problems with the use of toxic solvents, generation of hazardous by-products, and high energy consumption. Accordingly, there is a vital need to develop environmentally benign procedures for the synthesis of nanoferrites. A promising approach to achieve this objective is to exploit the array of biological resources in nature. Indeed, over the past several years, plants, have been used for production of low-cost, energy-efficient, and nontoxic metallic nanoferrites. Plant-mediated synthesis of nanoparticles is a green chemistry approach that connects nanotechnology with plants. This innovation is particularly compensating as far as decreasing the poisonous quality caused by the conventionally integrated NPs. Aloe Vera leaf extract is a medicinal agent with multiple properties including an antibacterial effect. Moreover, the constituents of Aloe Vera leaves include lignin, hemicellulose, and pectins which can be used in the reduction of nanoferrites. The magnetic nanoferrites (Fe, Co, Ni) were prepared by an eco-friendly hydrothermal method using an Aloe Vera plant extract solution as both a reducing and stabilizing agent. Magnetic nanoferrites were characterized using FTIR, XRD, VSM and SEM. Cytotoxicity were obtained using the MTT assay. X-ray diffraction analysis also demonstrated that the size range of the nanoferrites exhibited average diameters of 7- 19 nm. Results showed that all the metallic nanoparticles are magnetic with values Fe= 52 emu/g, Co= 33 emu/g and Ni=7.1 emu/g. The magnetic nanoferrites exhibited high cell viability rate at high concentrations signifying their non-toxic property. The magnetic nanoferrites produced in this study by green synthesis methodology from leaf extract of Aloe Vera needs to be further evaluated and could find greater biomedical application.References: K. Schulze, A. Koch, B. Schopf and A. Petri, Journal of Magnetism and Magnetic Materials, Vol. 293, pp. 419-432, (2005). S. Das, C. Dickinson, F. Lafir and D. Brougham, Green Chemistry, Vol. 14, pp. 1322–1334, (2012). M. Ferrari, Nature Reviews Cancer, Vol. 5, pp.161-171, (2005). M. Venkatachalam, G. Parthasarathy and P. Gowthaman, Imperial Journal of Interdisciplinary Research (IJIR), Vol. 2, pp. 1570-1575, (2016). T. Neuberger, B. Schopf and H. Hofmann, Journal of Magnetism and Magnetic Materials, Vol. 293, pp. 483–496, (2005).

Green Synthesis of Magnetic Fe3O4, CoFe2O4 and NiFe2O4 from Aloe Vera Extract for future Biomedical Applications

Magnetic order at the atomic scale has received considerable attention due to its potential application in spin transistors1-2, quantum computing3-4 , and ultra-dense memories5-6 . Although one dimensional (1D) magnetic systems have been intensely studied theoretically, the experimental determination of the extent and persistence of short- and long-range magnetic interactions, and how these interactions are affected by boundary conditions induced at the end of the chains remain unknown. We report structural and magnetic properties of ultra-short 1D iron chains subject to controlled boundary conditions. These iron chains are grown using iron phthalocyanine (FePc) thin films and FePc/ metal-free-phthalocyanine (H2Pc) superlattices (SLs), in which their length is precisely controlled by the thickness of the deposited FePc layers, and boundary conditions by electronic hybridization at the end of the chains. The electronic hybridization and local bonding environment is observable by element selective X-ray absorption spectroscopy (XAS). Ultra-short 1D iron chains between 7 and 200 atoms long become ferromagnetic below 5 K, and their magnetic response is strongly dependent on the boundary conditions imposed on the end atoms. The coercive field increases with the iron chain length with hybridized boundaries, whereas in chains not subject to hybridization the coercive field remains constant. A quantitative, semi-classical model based on the Dzyaloshinski-Moriya interaction, provides an understanding of these observations, in good agreement with experimental results. Work supported by the National Science Foundation under grants No. 1804414 and 1805585. Prepared by LLNL under Contract DE-AC52-07NA27344.References: 1. S. Datta, B. Das, Appl Phys Lett 56 (7), 665-667 (1990) 2. I, Zutic, J. Fabian, S. Das Sarma, Rev Mod Phys 76 (2), 323-410 (2004) 3. V. A. Dediu, L. E. Hueso, I. Bergenti, C. Taliani, Nat Mater 8 (9), 707-716 (2009) 4. A. J. Leggett, S. Chakravarty, A. T. Dorsey, M. P. A. Fisher, A. Garg, W. Zwerger, Rev Mod Phys 59 (1), 1-85, (1987) 5. Sinitskii, A.; Fursina, A. A.; Kosynkin, D. V.; Higginbotham, A. L.; Natelson, D.; Tour, J. M., Appl Phys Lett 95 (25), 253108 (2009) 6. Sinitskii, A.; Tour, J. M., ACS Nano 3 (9), 2760-2766 (2009)

Twisted Magnetism in Ultra-Short 1D Iron Chains with Hybridized Boundaries

Atomically thin transition metal dichalcogenides (TMD) semiconductors hold enormous potential for modern optoelectronic and ultra-low powered devices. By inducing long-range ferromagnetism (FM) in these semiconductors through the introduction of small amounts of a magnetic dopant, it is possible to extend their potential in emerging spintronic applications [1,2]. Our recent study showed that room temperature magnetism is achieved in V-doped WS2 monolayers [3], while still maintaining its characteristic optical properties. In this work we demonstrate light-mediated, room temperature FM, in V-doped WS2 monolayers. We probe this effect using the principle of magnetic LC resonance [4], which employs a soft ferromagnetic Co-based microwire coil driven near resonance in the radio frequency regime. Combining LC resonance, with an outstanding giant magneto-impedance effect, renders the coil highly sensitive to changes in the magnetic flux through its core. The V-doped WS2 monolayer is placed at the core of the coil where it is excited with a laser, while its magnetic permeability is probed by the coil. We found that the magnetic permeability of the monolayers is dependent on laser intensity, confirming light control of room temperature magnetism in this two-dimension material. Density functional theory calculations lead us to understand that this phenomenon is a consequence of an accumulation of excess holes in the conduction and valence bands, as well as carriers trapped in the magnetic doping states, which in turn mediates the magnetization of V-WS2 monolayers. These findings provide a promising route to exploit light-controlled FM in two-dimensional TMD based spintronic devices.References: [1] Dietl, T. A ten-year perspective on dilute magnetic semiconductors and oxides. Nat. Mater. 9, 965-974 (2010) [2] Dietl, T., Bonanni, A. & Ohno, H. Families of magnetic semiconductors – an overview. Journal of Semiconductors 40, 8 (2019) [3] Zhang, F., et. al. Monolayer Vanadium-doped Tungsten Disulfide: A Room-Temperature Dilute Magnetic Semiconductor. https://arxiv.org/abs/2005.01965 [4] Ortiz Jimenez, V., et. al. A magnetic sensor using a 2D van der Waals ferromagnetic material. Sci. Rep. 10, 4789 (2020)

Light-mediated magnetism in atomically thin vanadium-doped tungsten disulfide semiconductors

Our recent discovery of room-temperature ferromagnetism (FM) in transition metal dichalcogenide (TMD) monolayers of VSe2 has triggered intense research efforts by the scientific community [1,2]. However, the VSe2 monolayers are metallic which may not access the rich electronic and optical phenomena open to semiconductors. In this talk, we present a novel approach to induce long-range FM in TMDs through introducing magnetic dopants to form a dilute magnetic semiconductor. We demonstrate the tunability of room temperature FM in semiconducting TMD monolayers (V-doped WS2 and WSe2) [3,4]. Ferromagnetism peaks at an intermediate vanadium concentration of a few atomic percent (2-4 at.% V) and decreases for higher concentrations, which is consistent with quenching due to orbital hybridization at closer vanadium-vanadium distances. We discover a novel thermally induced spin flipping phenomenon in the V-doped WSe2 monolayers [4], and demonstrate the light-mediated FM in the V-WS2 monolayers at room temperature [5]. These findings pave a new pathway for the development of novel spintronic and valleytronic nanodevices based on atomically thin van der Waals magnetic semiconductors and stimulate further studies in this rapidly expanding research field of 2D magnetism.References: [1] M. Bonilla, M.H. Phan, et al., Strong Room Temperature Ferromagnetism in VSe2 Monolayers on van der Waals substrates, Nature Nanotechnology 13, 289 (2018) [2] V.O. Jimenez, M.H. Phan, et al., A magnetic sensor using a 2D van der Waals ferromagnetic material, Scientific Reports 10, 4789 (2020) [3] F. Zhang, M.H. Phan, et al., Monolayer Vanadium-doped Tungsten Disulfide: An Emerging Room-Temperature Diluted Magnetic Semiconductor, Advanced Science: https://arxiv.org/abs/2005.01965 [4] Y.T.H. Pham, M.H. Phan, et al., Tunable Ferromagnetism and Thermally Induced Spin Flip in Vanadium-doped Tungsten Diselenide Monolayers at Room Temperature, https://arxiv.org/abs/2005.00493 [5] V.O. Jimenez, M.H. Phan, et al., Light-controlled room temperature ferromagnetism in vanadium-doped tungsten diselenide semiconducting monolayers, Nature Communications (submitted).

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Magnetic doping of graphene with substitutional manganese atoms

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Voltage control of Néel wall interaction in thin films with uniaxial in-plane anisotropy

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