United States

Combining two materials having different functional properties has become a current research area for biomedical applications. The progress of nanoplatforms brings a new non-invasive imaging and therapeutic tools for cancer. Here, biocompatible and multifunctional magnetic Fe3O4-ZnO core–shell nanostructure has been developed by using a soft chemical approach. Fe3O4-ZnO core–shell is well characterized by various sophisticated characterization techniques such as X-ray diffraction (XRD), Transmission electron microscopy (TEM), X-ray photoelectron spectroscopy (XPS), UV-visible absorption, photo-luminescent spectroscopy and physical properties measurement system (PPMS). X-ray diffraction (XRD) confirms the presence of both Fe3O4 and ZnO phases. XPS analysis confirms the magnetite phase of Fe3O4 nanodots in the core-shell structures. TEM micrograph clearly reveals that 5 nm Fe3O4 nanodots are well decorated with ZnO nanoparticles shell. This multi-functional approach will facilitate magnetic targeting and generation of reactive species under an external AC magnetic field, providing therapy a smart therapeutic agent for cancer. Fe3O4-ZnO core–shell conserves the intrinsic superparamagnetic behaviour of its constituent Fe3O4 with a magnetization value of ~ 36.5 emu/g. The aqueous colloidal stability, optimal magnetization, and good specific absorption rate (under external AC magnetic field) of Fe3O4-ZnO core–shell particles perform as an effective heating source for thermal therapy. Cytotoxicity studies exhibit the reduction of cellular viability for human cervical cancer cells (HeLa). Further, A combined effect of thermo-therapy and generation of reactive oxygen species under AC magnetic field results in a synergistic effect on the cancer cell death. Therefore, these results indicate that core–shell is sufficient materials for magnetic hyperthermia and bio-imaging.References: 1. J. Wan, H. Li, and K. Chen, Materials Chemistry and Physics, 114, 2009, 30-32. 2. H. Zhang, L. Guo, S. Ding, J. Xiong, and B. Chen, Oncotarget. 7, 2016, 36602–36613. 3. K. Patel, B. S. Raj, Y. Chen, and X.Lou,Colloids and Surfaces B: Biointerfaces, 150, 2017, 317–325.

MMM 2020

Core-Shell ZnO@Fe3O4 Nanostructure for Magnetic Hyperthermia and Bio-Imaging Applications

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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Efficient spin injection into semiconductors remains a formidable and elusive challenge even after almost three decades of major scientific effort, studded by obstacles and only partial workarounds. Few years ago, I predicted the possibility of injecting massive ultrashort spin current pulses across a ferromagnetic metal/semiconductor interface [1-2]. We have now proved experimentally the prediction [3]. By injecting strongly out-of-equilibrium sub-picosecond spin current pulses across a bare ferromagnet/semiconductor interface, we have overcome the crippling problem of impedance mismatch and obtained a massive spin transfer. We demonstrated this by producing ultrashort spin current pulses into cobalt and injecting them into monolayer MoS2. The semiconducting MoS2 layer also acts as a selective converter of the spin current into a charge current, whose THz emission is then measured. As predicted, we measured a giant spin current, orders of magnitude larger than typical injected spin current densities in modern devices.References: [1] M. Battiato, K. Held, Phys. Rev. Lett. 116, 196601 (2016) [2] M. Battiato J. Phys. Condens. Matter 29, 174001 (2017). [3] L. Cheng et al., Nature Physics 15, 347 (2019).

Far out-of-equilibrium spin populations trigger giant spin injection into atomically thin MoS2

Tunneling spin injection on graphene is possible by using different materials as barriers1–3. However, the growth of ultra-thin tunnel barriers leads to the creation of pinholes, which in turn causes direct ohmic contact and a large suppression of spin polarization. This occurs due to a fundamental limitation known as the resistance mismatch problem4, which limits spin injection when the resistance of an injector contact, , is lower than the spin resistance of the graphene channel, . This is the result of contact-induced spin relaxation, which greatly decreases the measured spin signals5. In this work, we demonstrate an alternative approach to grow ultra-thin tunnel barrier contacts made by oxidizing aluminium on top of previously functionalized graphene. We show that molecular functionalization of graphene allows the growth of smooth, high quality tunnel barriers, leading to contacts with increased spin injection efficiency and enhanced spin signals by one order of magnitude. The functionalization process consists on the laser activated physisorbtion of benzoyl peroxide (BPO) molecules on graphene. This laser controlled photoreaction enables us to control both the spatial location and the degree of functionalization, as visualized by Raman spectroscopy maps via the intensity ratio of and peaks (ID/IG). We assess the quality of the oxide barriers using atomic force microscopy, charge transport and spin transport measurements. These results open the path towards engineering spintronic devices with spatially controlled functionalization and efficient tunnel contacts.References: Tombros, N. et al, Nature 448, 571–574 (2007). Tombros, N. et al, Phys. Rev. Lett. 101, 2–5 (2008). Han, W. et al, Phys. Rev. Lett. 105, 167202 (2010). Schmidt, G. et al, Phys. Rev. B 62, R4790–R4793 (2000). Maassen, T. et al, Phys. Rev. B 86, 235408 (2012).

Spin Injection Enhancement via ultra-thin Oxide barriers into Molecularly Functionalized Graphene

The non-local spin valve (NLSV) is an important tool in spintronics, primarily due to its ability to isolate pure spin currents1. As such, NLSVs have been instrumental in spin transport measurements of a wide range of materials2. Yet, even in relatively simple systems, questions remain on the impact of interfaces, defects and impurities3–5. Of particular interest is an increase in the “spin-signal”, ΔRNL, under large magnetic fields (up to 9 T) in all-metallic NLSVs6, in stark contrast to the key tenet that ΔRNL is invariant under a magnetic field. This effect, which appears only for certain combinations of FM and normal metals, has been a long-standing mystery and, thus far, has been a challenge to describe with existing models. Our earlier works on similar materials have shown that a low temperature upturn in spin-relaxation rate, 1/τs, originates from magnetic impurity (MI) scattering near the NLSV interfaces5,7, underlining the importance of the Kondo effect in determining spin-relaxation, particularly in Cu devices. In this study we demonstrate MI scattering as the origin of the field enhancement of ΔRNL, and we provide a theoretical framework. By correlating the magnitude of the field enhancement, δRNL, with the NLSV material pairings, we ascertain that δRNL is only present in those materials that can host MI moments (Figure 1). Next, focusing on Cu/Fe NLSVs, we extract spin-transport parameters from the field-enhanced ΔRNL. Under zero-field, we observe the same increase in 1/τs at low temperatures (Figure 2), due to Kondo scattering from MIs, in agreement with our previous work5. Importantly, we show that this mechanism is quenched by a magnetic field and we successfully model the data using a magnetic-field-modified Kondo expression8. This work not only highlights a systematic overestimation of 1/τs in materials containing MIs, including a clear impact on Hanle spin relaxation measurements, but also provides a simple means to quantify and suppress this scattering mechanism.References: 1 F.J. Jedema, M.S. Nijboer, A.T. Filip, and B.J. van Wees, Phys. Rev. B 67, 085319 (2003). 2 I. Zutić, J. Fabian, and S. Das Sarma, Rev. Mod. Phys. 76, 323 (2004). 3 H. Idzuchi, Y. Fukuma, L. Wang, and Y. Otani, Appl. Phys. Lett. 101, 022415 (2012). 4 E. Villamor, M. Isasa, L.E. Hueso, and F. Casanova, Phys. Rev. B 87, 094417 (2013). 5 L. O’Brien, M.J. Erickson, D. Spivak, et al., Nat. Commun. 5, 3927 (2014). 6 K. Výborný, G. Mihajlović, A. Hoffmann, and S.I. Erlingsson, J. Phys. Condens. Matter 25, (2013). 7 J.D. Watts, L. O’Brien, J.S. Jeong, et al., Phys. Rev. Mater. 3, 124409 (2019). 8 V.I. Litvinov, Phys. Status Solidi 77, 71 (1976).

Origin of the Magnetic Field Enhancement of the Spin Signal in Metallic Non-Local Spin Transport Devices

Semiconductors nanowires (NWs) with strong spin-orbital interaction, like InSb and InAs nanowires, are a leading platform for realizing future computing devices, such as Datta-Das spin-transistor1 and topological-superconductor quantum computing devices2 using Majorana zero modes. Coupling nanowires to electrical spin-selective contacts, therefore, is an important step as it can, on the one hand, provide a setting to study spin transport in quantum wires, and on the other hand could enable the realization of Majorana devices that do not require an applied magnetic field, by taking advantage of the magnetic exchange interaction or spin accumulation. Here, we will discuss our measurements on InSb NW devices with iron (Fe) electrical contacts3 (see Figure 1, scanning electron microscopy picture). Conductance measurements show conductance quantization and Fabry–Pérot interference, clearly demonstrating phase-coherent and ballistic electronic transport with spin-polarized currents. Our magnetoconductance study clearly demonstrates spin injection/ transport across the NWs by the observation of hysteretic spin-valve signals (Figure 2a). Moreover, we show that electrostatic gating tunes the observed hysteretic signal and reveals a transport regime where the device acts as a spin filter (Figure 2b). *Supported primarily by the Department of Energy under Award No. DE-SC-0019274. Nanowire growth was supported by the European Research Council (ERC HELENA 617256), and the Dutch Organization for Scientific Research (NWO).References: 1. Datta, S. & Das, B. Electronic analog of the electro-optic modulator. Appl. Phys. Lett., Vol.56, p.665–667 (2016) 2. Mourik, V. et al. Signatures of Majorana Fermions in Hybrid Superconductor-Semiconductor Nanowire Devices. Science., Vol.336, p.1003–1007 (2012) 3. Yang, Z. et al. Spin Transport in Ferromagnet-InSb Nanowire Quantum Devices. Nano Lett., Vol 20, p.3232-3239 (2020)

Ballistic Spin Transport in InSb Nanowires with Strong Rashba Spin-Orbital Interaction

It has been demonstrated that the Kondo effect from iron impurities substantially enhances the spin relaxation rate at low temperature in submicron copper channels of nonlocal spin valves (NLSV) [1,2]. In this work, we explore a long standing question about the physical existence of Kondo screening clouds [3] by examining the relationship between Kondo spin relaxation rate and Kondo resistivity. A systematic method is utilized to extract spin and charge transport parameters from each of the 20 NLSV devices investigated. Figure 1 (a) shows that the spin relaxation length of a NLSV reaches its maximum of 3.0 microns at 30K. Low temperature upturns are clearly observed in the spin relaxation rate versus temperature (Figure 1 (b)) and the Cu resistivity versus temperature (inset of Figure 1 (b)) plots. Both upturns are attributed to the Kondo effect from Fe impurities of several ppm. The Kondo spin relaxation rate and Kondo resistivity are extracted by fitting and plotted in Figure 1 (c) for all 20 NLSVs. Surprisingly, the Kondo spin relaxation rate remains almost constant, while the Kondo resistivity varies by nearly a factor of 10. This is significantly different from the linear relationship predicted by the Elliott-Yafet model. The effective Kondo spin flip probability, shown in Figure 1 (d), is greatly suppressed as the Kondo resistivity (proportional to impurity density) increases. The data can be explained by considering the spin dephasing processes through the Kondo screening clouds around Fe impurities, and support the physical existence of Kondo screening clouds.References: [1] L. O’Brien, et.al, Nat. Commun. 5, 3927 (2014). [2] J. T. Batley, et.al, Phys. Rev. B 92, 220420(R) (2015). [3] V. Borzenets, et.al, Nature 579, 210–213 (2020).

Unusual scaling of Kondo spin relaxation

Topological insulator BiSb is a promising candidate for spin-orbit-torque (SOT) magnetoresistive random-access memory (MRAM), due to its giant spin Hall effect (spin Hall angle θSH ∼ 52 for BiSb(012) surface) [1] and high electrical conductivity (σ ~ 2.5 × 105 Ω-1m-1) [2] at room temperature. Recently, we demonstrated that high-quality BiSb thin films with quasi single crystal structure could be grown by sputtering deposition, underlying its potential for mass production of SOT-MRAM [3]. In this work, we show that in all-sputtered BiSb-(Co/Pt)n multilayers structure, the BiSb layer with (110) surface has large θSH = 12.3 and high σ ~ 1.5 × 105 Ω-1m-1, which lead to ultrahigh efficient SOT magnetization switching of (Co/Pt)n multilayers. We deposited (0.4 nm Co/0.4 nm Pt)2 - 10 nm BiSb multilayers on c-plane sapphire (0001) substrate at room temperature (Fig. 1a). The (Co/Pt)2 multilayers are perpendicularly magnetized with a large anisotropy field, as shown in Fig. 1b. We employed the second harmonic Hall measurement to evaluate θSH in 50 μm × 25 μm Hall bars. A representative 2nd harmonic Hall resistance (R2ω) is plotted as a function of in-plane magnetic field (H) in Fig. 1c, and the antidamping-like field HAD is evaluated by fitting to R2ω at high field. Fig. 1d shows the HAD at various current density JBiSb, from which we obtained θSH = 12.3. Thanks to the large θSH, the magnetization of (Co/Pt)2 can be efficiently switched by a small DC threshold current density JthBiSb = 1.5 × 106 Acm-2 at H = ±2.75 kOe (Fig. 2a and 2b). Fig. 2c shows robust switching by 75 consecutive pulses at ±1.83 kOe (JBiSb = 4.4 × 106 Acm-2, tpulse = 100 μs). Our results demonstrate the feasibility of BiSb for ultralow power SOT-MRAM and other SOT-based spintronics devices.References: [1] N. H. D. Khang, Y. Ueda and P. N. Hai, Nat. Mater. 17, 808-813 (2018). [2] Y. Ueda et al., Appl. Phys. Lett. 110, 062401 (2017). [3] T. Fan et al., Jpn. J. Appl. Phys. 59, 063001 (2020).

Ultrahigh Efficient Spin-Orbit-Torque Magnetization Switching in Sputtered Topological Insulator BiSb and (Co/Pt)2 Multilayers

Spintronics has opened a new paradigm through the use of the spin variable as the vector of information and has been largely applied from hard drives read-heads to the STT-MRAMs. While very recent, the introduction of 2D materials in Magnetic Tunnel Junctions (MTJs) has already shown some promising properties[1]. Graphene and the 2D insulator h-BN have been the first 2D materials to show strong impact on spin transport in MTJs. The recent advent of the wide TMDC family of 2D semiconductors opened new opportunities for further tailoring of spintronics properties. We will present results on the scarcely studied WS2. We will detail a protocol using laser lithography technology to fabricate spin valves based on CVD grown WS2, with step by step characterizations in support (Raman spectroscopy, photoluminescence, and AFM measurements). We will finally show our first spin transport measurements obtained in a CVD WS2 based MTJ. Our measured MR signals, above state of the art for 2D semiconductor based MTJs, validates our integration approach. We observe that the spin signal extracted from a ferromagnetic electrode can be tuned by placing atomically thin WS2 on top of it. Furthermore the thickness of WS2 significantly affects the extracted spin polarization of the 2D/FM interface. We discuss that trend using the peculiar band structure of WS2, supported by DFT calculations, leading to thickness dependent spin filtering. Our work opens the way to the integration of different members of the very large TMDCs family, in order to reveal their spin transport properties in MTJs[2].References: [1] M. Piquemal-Banci, R. Galceran, M-B. Martin et al. J. Phys. D: Appl. Phys., 50 , 203002 (2017). [2] V. Zatko, M. Galbiati, S-M-M. Dubois et al. ACS Nano., 13 , 14468 (2019).

Band-Structure Spin-Filtering in Vertical Spin Valves Based on CVD Grown WS2

Recently, possible applications for thermoelectrics and spin caloritronics utilizing topological materials have been studied. Thermoelectric (TE) conversion that can convert heat into electricity has been attracting attention as a clean power generation technology without greenhouse gases in energy harvesting. The conversion efficiency is evaluated by the dimensionless figure of merit ZT, which is needed to be larger than 1 (energy conversion efficiency is 10%) in practice. Recently, a bismuth chalcogenide which shows the best TE conversion on the nanoscale has been also known as a three-dimensional topological insulator (3D TI). TI has a linear electronic dispersion on the surface. In the presence of a surface gap induced by magnetic dopants, the surface electronic transport strongly depends on the chemical potential, promising very large TE conversion efficiency [1]. Here, we propose a TE energy conversion device based on the surface of 3D TIs that is magnetically gap-opened and ionically disordered [2]. This device can achieve the thermocouple p-n junction by a single TI film, in which a pair of top and bottom surfaces of a 3D TI takes a role of the vertical p-n junction, which can be considered a thermocouple consisting of two dissimilar TE materials (see Fig. 1). Based on the Boltzmann theory at finite temperatures, we compute TE transport coefficients taking into account electron scattering by screened disorder potentials on the surface. By tuning the surface carrier screening by means of electric gating, we find that ZT of the present device achieves more than 1 in the wide temperature-regime from 100 K to 300 K.References: [1] T. Chiba and S. Takahashi, J. Appl. Phys. 126, 245704 (2019). [2] T. Chiba, S. Takahashi, and T. Komine, Appl. Phys. Lett. 115, 083107 (2019).

Spin caloritronic device based on asymmetric surfaces of magnetic topological insulators

Efficient and versatile spin-to-charge current conversion is crucial for the development of spintronic applications, which strongly rely on the ability to electrically generate and detect spin currents. In this context, the spin Hall effect has been widely studied in heavy metals with strong spin-orbit coupling. While the high crystal symmetry in these materials limits the conversion to the orthogonal configuration [1], unusual configurations are expected in low symmetry transition metal dichalcogenide semimetals [2], which could add flexibility to the electrical injection and detection of pure spin currents. Here, we report the observation of spin-to-charge conversion in MoTe2 flakes, which are stacked in graphene lateral spin valves [3]. We detect two distinct contributions arising from the conversion of two different spin orientations. In addition to the conventional conversion where the spin polarization is orthogonal to the charge current, we also detect a conversion where the spin polarization and the charge current are parallel. Both contributions, which could arise either from bulk spin Hall effect or surface Edelstein effect, show large efficiencies comparable to the best spin Hall metals and topological insulators. Our finding enables the simultaneous conversion of spin currents with any in-plane spin polarization in one single experimental configuration [3].References: [1] Sinova, J.; Valenzuela, S. O.; Wunderlich, et al., Rev. Mod. Phys., Vol. 87, p.1213-1260 (2015) [2] MacNeill, D.; Stiehl, G. M.; Guimaraes, et al., Nat. Phys. Vol. 13, p.300-305 (2017) [3] Safeer, C. K.; Ontoso, N.; Ingla-Aynés, et al., Nano Lett., Vol.19, p8758-8766 (2019)

Large multi-directional spin-to-charge conversion in low symmetry semimetal MoTe2 at room temperature

Metallic-based nanoparticles have been investigated extensively for their robustness, effectiveness and the potential functionalization of their surface. Especially, magnetic nanoparticles with their distinctive characteristics are widely used in bioassays and magnetic drug delivery systems in biomedical applications as an anti-cancer agent. In this study, Fe/Fe3O4 core-shell nanoparticles (13-20nm) (Figure 1), coated with PEG, have been successfully synthesized by Y-junction flow tube technique. The room temperature coercivity was found to be 350 Oe. A549 non-small cell lung cancer and NIH3T3 mouse embryonic fibroblast cell lines were used to monitor cellular toxicity (IC50) and proliferation effects of PEG-ylated Fe/Fe3O4 nanoparticles. The inhibitory potential on the cell motility of A549 cancer cells were higher than NIH3T3 cells. The results showed that the toxic effect of particles was higher on cancer cells. Upon examination, IC50 values were found to be 27.5 μg/ml and 1 μg/ml for NIH3T3 cell and A549 cell, respectively. (Figure 1 a and b) The nanoparticles were found to be 100 times more toxic on cells when compared to the previous studies. According to the results, PEG-ylated Fe/Fe3O4 nanoparticles not only have significantly lower IC50 values compared to similar research but also they could be used in diagnosis, magnetic hyperthermia and various drug systems as a treatment method against cancer. This work was supported by BAP.2018-2.05References: Domac, B. H., AlKhatib, S., Zirhli, O., Akdogan, N. G., Öcal Dirican, S. C., Bulut, G., & Akdogan, O., Effects of PEGylated Fe–Fe3O4 core-shell nanoparticles on NIH3T3 and A549 cell lines. Heliyon, 6(1), (2020).

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