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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).

MMM 2020

Tunable Room-Temperature Ferromagnetism and Emergent Phenomena in Atomically Thin Transition Metal Dichalcogenide Semiconductors INVITED

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

The demonstration of efficient manipulation of the antiferromagnetic (AF) order parameter has highlighted its highly attractive properties for spintronics, including lack of magnetic stray fields, robustness against magnetic field perturbations and intrinsic dynamics in the THz regime [1, 2, 3]. Specific functionalities often depend sensitively on the magnetic domain structure [4]. In fully compensated AFs with no demagnetizing fields, magnetoelastic effects are expected to dominate [5,6]. We report direct imaging and analysis of AF domains in patterned epitaxial CuMnAs thin films. A pronounced effect of patterned edges on the domain orientation and domain wall width is demonstrated, which extends over several microns. A local alignment of the Néel vector with microtwin line defects is observed, which, combined with the edge effect, leads to the formation of lens-shaped domains oriented perpendicular to the patterned edges. We observe magneto-structural reconfigurations in which defect lines and surrounding AF domains grow together over the timescale of weeks at room temperature and over minutes 30K above room temperature.References: [1] P. Wadley, B. Howells, J. Zelezny et al., Science., Vol. 351, p. 587 (2016) [2] X.Z. Chen, R. Zarzuela, J. Zhang et al., Physics Review Letters., Vol. 120, p. 207204 (2018) [3] P. Nemec, M. Fiebig, T. Kampfrath and A.V. Kimel, Nature Physics., Vol. 14, p. 229 (2018) [4] A.L. Ross et al., Nano Letters, Vol. 20(1), p. 306 (2020) [5] O. Gomonay and V. Loktev, Journal of Magnetism and Magnetic Materials., Vol. 242(2), p. 1418 (2002) [6] O. Gomonay, V. Baltz, A. Brataas and Y. Tserkovnyak, Nature Physics., Vol. 14, p. 213 (2018)

Antiferromagnetic Domain Structure in CuMnAs Devices

Non-collinear antiferromagnets such as D019-Mn3Sn have attracted much attention owing to their large anomalous Hall effect (AHE) originating from non-vanishing Berry curvature [1-5]. We recently reported a growth of epitaxial D019-Mn3Sn thin films with various orientations by sputtering, where anisotropic AHE was observed [5]. To realize functional devices harnessing the unique features of this material system, it is necessary to clarify the correlation of the physical properties with various factors of thin film. Here, we study the correlation between AHE and crystal structure of Mn-Sn alloy film by changing post-annealing temperature (Ta) and Mn-Sn composition. We prepare two series of Mn3+xSn1-x thin films which are deposited on MgO(110) substrate by sputtering. The first series have a fixed x = +0.06 and Ta is changed from 300 to 600oC. The second series have various x (-0.35 ~ +0.32) with a fixed Ta = 500oC. Crystal structures are characterized by X-ray diffraction (XRD). Transport measurement is performed for microfabricated Hall devices. From XRD measurement, we find that dominant phase of Mn-Sn changes from Mn1.75Sn to D019-Mn3Sn as Ta increases (series 1), and changes from Mn3Sn2 to D019-Mn3Sn as x increases (series 2) in the studied range. Transport measurement for the series 1 reveals that appearance of AHE coincides with the formation of D019-Mn3Sn and the magnitude increases with Ta [Fig. 1]. Meanwhile, for the series 2, the largest AHE is obtained at around the stoichiometric composition [Fig. 2]. We here note that the two series are prepared at different times, leading to different magnitude of AHE. From a comparison with XRD results, we find that magnitude of AHE is well explained by multiple factors of crystalline structure including proportion of D019-Mn3Sn crystallite, crystalline orientation, and the order parameter. The obtained results provide an important insight to deepen the physics of non-collinear antiferromagnet and to realize new-functional devices. This work is partly supported by JSPS Kakenhi No. 19H05622 and No. 19J13405.References: [1] S. Nakastuji, N. Kiyohara and T. Higo, Nature, Vol. 527, p.212 (2015). [2] A. K. Nayak, J. E. Fischer and S. S. P. Parkin, Sci. Adv., Vol. 15, p.e1501870 (2016). [3] T. Higo, D. Qu and S. Nakatsuji, Appl. Phys. Lett., Vol. 113, p.202402 (2018). [4] T. Ikeda, M. Tsunoda and Y. Ando, Appl. Phys. Lett., Vol. 113, p.222405 (2018). [5] J. Yoon, Y. Takeuchi and H. Ohno, Appl. Phys. Express, Vol. 13, p.013001 (2020).

Anomalous Hall Effect in Mn-Sn Thin Films - Correlation with Crystal Structure

In this work, we report on THz emission from FeMnPt-based synthetic antiferromagnetic structures (SAF), originating from the anomalous Hall effect (AHE) [1][2]. The peak amplitude of the THz emission is almost doubled as compared to the respective single layer with the same equivalent thickness. In addition, we demonstrate by both simulation and experiment that the THz emission provides a powerful tool to probe the magnetization reversal process of individual ferromagnetic layers in the SAF structure – an important building block for all types of spintronic devices. By measuring the polarization of the THz wave, we are able to determine the magnetization directions of the individual magnetic layers which are not possible or difficult to obtain by using other magnetic characterization techniques. Fig. 1 shows the shematic of the FeMnPt SAF structure under an in-plane external field. A femtosecond laser pulse is used to excite the sample, thereby generating the THz emission. Fig. 2 shows the temperoal profile of the THz emmission from both the FeMnPt SAF (solide-line: 0 Oe; dashed-line: 200 Oe) and a single layer FeMnPt (dotted-line). At zero field, The AHE in both layers of the SAF contributes to the THz emission, leading to a larger THz amplitude, which is almost doubled that of the single layer. By correalting the simulated and experimental results, the direction of magnetizaion in each FM layer during field sweeping can be determined becasue the THz emission is propotional to the dedection of mangetization in each FM layer. Our results show that THz emission provides a powerful tool to understand the magnetic reversal of SAFs.References: [1] Q. Zhang, Z. Luo, H. Li, et al., Physical Review Applied, vol.12, p.054027, (2019) [2] Q. Zhang, Y. Yang, Z. Luo, et al., Physical Review Applied, vol.13, p.054016, (2020)

Terahertz Emission From an Exchange-Coupled Synthetic Antiferromagnet

Exotic spin torques resulting from reduced symmetry in quantum materials stand out as strong possibilities for advancing the future of MRAM and spin-torque based neuromorphic computing. Magnetic ordering can reduce the symmetry of a material in a manipulatable way, generating customizable spin torques, and is thus an attractive trait in spin source materials. Antiferromagnets are particularly attractive due to the robustness of their magnetic ordering, which can be prepared into a state and remain stable in that state in a wide range of device setups. Iron rhodium (FeRh) exhibits a transition between a low-temperature antiferromagnetic state and a high-temperature ferromagnetic state. For appropriately grown thin film FeRh, this transition can be found close to room temperature, making both of its magnetic states easily accessible. We report large exotic spin torques generated in an antiferromagnetic FeRh spin source layer and investigate the role of magnetic ordering on the size and geometry of generated spin torques. We also show strong temperature dependence of the spin torque efficiency in the antiferromagnetic phase of FeRh. This work was supported as part of Quantum Materials for Energy Efficient Neuromorphic Computing, an Energy Frontier Research Center funded by the U.S. DOE, Office of Science.

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