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1.
Adv Sci (Weinh) ; 10(28): e2302956, 2023 Oct.
Article in English | MEDLINE | ID: mdl-37530205

ABSTRACT

Their high tunability of electronic and magnetic properties makes transition-metal oxides (TMOs) highly intriguing for fundamental studies and promising for a wide range of applications. TMOs with strong ferrimagnetism provide new platforms for tailoring the anomalous Hall effect (AHE) beyond conventional concepts based on ferromagnets, and particularly TMOs with perpendicular magnetic anisotropy (PMA) are of prime importance for today's spintronics. This study reports on transport phenomena and magnetic characteristics of the ferrimagnetic TMO NiCo2 O4 (NCO) exhibiting PMA. The entire electrical and magnetic properties of NCO films are strongly correlated with their conductivities governed by the cation valence states. The AHE exhibits an unusual sign reversal resulting from a competition between intrinsic and extrinsic mechanisms depending on the conductivity, which can be tuned by the synthesis conditions independent of the film thickness. Importantly, skew-scattering is identified as an AHE contribution for the first time in the low-conductivity regime. Application wise, the robust PMA without thickness limitation constitutes a major advantage compared to conventional PMA materials utilized in today's spintronics. The great potential for applications is exemplified by two proposed novel device designs consisting only of NCO films that open a new route for future spintronics, such as ferrimagnetic high-density memories.

2.
Small ; 19(39): e2302387, 2023 Sep.
Article in English | MEDLINE | ID: mdl-37231567

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 Fe5- 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.

3.
Adv Mater ; 31(3): e1805645, 2019 Jan.
Article in English | MEDLINE | ID: mdl-30461088

ABSTRACT

Phase coherence in nanostructures is at the heart of a wide range of quantum effects such as Josephson oscillations between exciton-polariton condensates in microcavities, conductance quantization in 1D ballistic transport, or the optical (excitonic) Aharonov-Bohm effect in semiconductor quantum rings. These effects only occur in structures of the highest perfection. The 2D semiconductor heterostructures required for the observation of Aharonov-Bohm oscillations have proved to be particularly demanding, since interface roughness or alloy fluctuations cause a loss of the spatial phase coherence of excitons, and ultimately induce exciton localization. Experimental work in this field has so far relied on either self-assembled ring structures with very limited control of shape and dimension or on lithographically defined nanorings that suffer from the detrimental effects of free surfaces. Here, it is demonstrated that nanowires are an ideal platform for studies of the Aharonov-Bohm effect of neutral and charged excitons, as they facilitate the controlled fabrication of nearly ideal quantum rings by combining all-binary radial heterostructures with axial crystal-phase quantum structures. Thanks to the atomically flat interfaces and the absence of alloy disorder, excitonic phase coherence is preserved even in rings with circumferences as large as 200 nm.

4.
Nano Lett ; 18(1): 81-87, 2018 01 10.
Article in English | MEDLINE | ID: mdl-29206466

ABSTRACT

Controlled and reproducible doping is essential for nanowires (NWs) to realize their functions. However, for the widely used self-catalyzed vapor-liquid-solid (VLS) growth mode, the doping mechanism is far from clear, as the participation of the nanoscale liquid phase makes the doping environment highly complex and significantly different from that of the thin film growth. Here, the doping mechanism of self-catalyzed NWs and the influence of self-catalytic droplets on the doping process are systematically studied using beryllium (Be) doped GaAs NWs. Be atoms are found for the first time to be incorporated into NWs predominantly through the Ga droplet that is observed to be beneficial for setting up thermodynamic equilibrium at the growth front. Be dopants are thus substitutional on Ga sites and redundant Be atoms are accumulated inside the Ga droplets when NWs are saturated, leading to the change of the Ga droplet properties and causing the growth of phase-pure zincblende NWs. This study is an essential step toward the design and fabrication of nanowire devices.

5.
Nano Lett ; 17(9): 5213-5221, 2017 09 13.
Article in English | MEDLINE | ID: mdl-28654280

ABSTRACT

We demonstrate an all-epitaxial and scalable growth approach to fabricate single-crystalline GaN nanowires on graphene by plasma-assisted molecular beam epitaxy. As substrate, we explore several types of epitaxial graphene layer structures synthesized on SiC. The different structures differ mainly in their total number of graphene layers. Because graphene is found to be etched under active N exposure, the direct growth of GaN nanowires on graphene is only achieved on multilayer graphene structures. The analysis of the nanowire ensembles prepared on multilayer graphene by Raman spectroscopy and transmission electron microscopy reveals the presence of graphene underneath as well as in between nanowires, as desired for the use of this material as contact layer in nanowire-based devices. The nanowires nucleate preferentially at step edges, are vertical, well aligned, epitaxial, and of comparable structural quality as similar structures fabricated on conventional substrates.

6.
Sci Rep ; 7: 43644, 2017 02 27.
Article in English | MEDLINE | ID: mdl-28240323

ABSTRACT

Van der Waals heterostructures combining hexagonal boron nitride (h-BN) and graphene offer many potential advantages, but remain difficult to produce as continuous films over large areas. In particular, the growth of h-BN on graphene has proven to be challenging due to the inertness of the graphene surface. Here we exploit a scalable molecular beam epitaxy based method to allow both the h-BN and graphene to form in a stacked heterostructure in the favorable growth environment provided by a Ni(111) substrate. This involves first saturating a Ni film on MgO(111) with C, growing h-BN on the exposed metal surface, and precipitating the C back to the h-BN/Ni interface to form graphene. The resulting laterally continuous heterostructure is composed of a top layer of few-layer thick h-BN on an intermediate few-layer thick graphene, lying on top of Ni/MgO(111). Examinations by synchrotron-based grazing incidence diffraction, X-ray photoemission spectroscopy, and UV-Raman spectroscopy reveal that while the h-BN is relaxed, the lattice constant of graphene is significantly reduced, likely due to nitrogen doping. These results illustrate a different pathway for the production of h-BN/graphene heterostructures, and open a new perspective for the large-area preparation of heterosystems combining graphene and other 2D or 3D materials.

7.
Nano Lett ; 17(3): 1529-1537, 2017 03 08.
Article in English | MEDLINE | ID: mdl-28166406

ABSTRACT

GaN nanowires (NWs) doped with Mg as a p-type impurity were grown on Si(111) substrates by plasma-assisted molecular beam epitaxy. In a systematic series of experiments, the amount of Mg supplied during NW growth was varied. The incorporation of Mg into the NWs was confirmed by the observation of donor-acceptor pairs and acceptor-bound excitons in low-temperature photoluminescence spectroscopy. Quantitative information about the Mg concentrations was deduced from Raman scattering by local vibrational modes related to Mg. In order to study the type and density of charge carriers present in the NWs, we employed two photoelectrochemical techniques, open-circuit potential and Mott-Schottky measurements. Both methods showed the expected transition from n-type to p-type conductivity with increasing Mg doping level, and the latter characterization technique allowed us to quantify the charge carrier concentration. Beyond the quantitative information obtained for Mg doping of GaN NWs, our systematic and comprehensive investigation demonstrates the benefit of photoelectrochemical methods for the analysis of doping in semiconductor NWs in general.

8.
Nano Lett ; 17(1): 136-142, 2017 01 11.
Article in English | MEDLINE | ID: mdl-28001430

ABSTRACT

Nanoscale substrates such as nanowires allow heterostructure design to venture well beyond the narrow lattice mismatch range restricting planar heterostructures, owing to misfit strain relaxing at the free surfaces and partitioning throughout the entire nanostructure. In this work, we uncover a novel strain relaxation process in GaAs/InxGa1-xAs core-shell nanowires that is a direct result of the nanofaceted nature of these nanostructures. Above a critical lattice mismatch, plastically relaxed mounds form at the edges of the nanowire sidewall facets. The relaxed mounds and a coherent shell grow simultaneously from the beginning of the deposition with higher lattice mismatches increasingly favoring incoherent mound growth. This is in stark contrast to Stranski-Krastanov growth, where above a critical thickness coherent layer growth no longer occurs. This study highlights how understanding strain relaxation in lattice mismatched nanofaceted heterostructures is essential for designing devices based on these nanostructures.

9.
Nat Commun ; 6: 7632, 2015 Jul 09.
Article in English | MEDLINE | ID: mdl-26158645

ABSTRACT

Scaling graphene down to nanoribbons is a promising route for the implementation of this material into devices. Quantum confinement of charge carriers in such nanostructures, combined with the electric field-induced break of symmetry in AB-stacked bilayer graphene, leads to a band gap wider than that obtained solely by this symmetry breaking. Consequently, the possibility of fabricating AB-stacked bilayer graphene nanoribbons with high precision is very attractive for the purposes of applied and basic science. Here we show a method, which includes a straightforward air annealing, for the preparation of quasi-free-standing AB-bilayer nanoribbons with different widths on SiC(0001). Furthermore, the experiments reveal that the degree of disorder at the edges increases with the width, indicating that the narrower nanoribbons are more ordered in their edge termination. In general, the reported approach is a viable route towards the large-scale fabrication of bilayer graphene nanostructures with tailored dimensions and properties for specific applications.

10.
Nano Lett ; 14(5): 2604-9, 2014 May 14.
Article in English | MEDLINE | ID: mdl-24678901

ABSTRACT

Efficient infrared light emitters integrated on the mature Si technology platform could lead to on-chip optical interconnects as deemed necessary for future generations of ultrafast processors as well as to nanoanalytical functionality. Toward this goal, we demonstrate the use of GaAs-based nanowires as building blocks for the emission of light with micrometer wavelength that are monolithically integrated on Si substrates. Free-standing (In,Ga)As/GaAs coaxial multishell nanowires were grown catalyst-free on Si(111) by molecular beam epitaxy. The emission properties of single radial quantum wells were studied by cathodoluminescence spectroscopy and correlated with the growth kinetics. Controlling the surface diffusivity of In adatoms along the NW side-walls, we improved the spatial homogeneity of the chemical composition along the nanowire axis and thus obtained a narrow emission spectrum. Finally, we fabricated a light-emitting diode consisting of approximately 10(5) nanowires contacted in parallel through the Si substrate. Room-temperature electroluminescence at 985 nm was demonstrated, proving the great potential of this technology.

11.
Nano Lett ; 13(9): 4053-9, 2013 Sep 11.
Article in English | MEDLINE | ID: mdl-24001176

ABSTRACT

An analysis of the strain in an axial nanowire superlattice shows that the dominating strain state can be defined arbitrarily between unstrained and maximum mismatch strain by choosing the segment height ratios. We give experimental evidence for a successful strain design in series of GaN nanowire ensembles with axial InxGa1-xN quantum wells. We vary the barrier thickness and determine the strain state of the quantum wells by Raman spectroscopy. A detailed calculation of the strain distribution and LO phonon frequency shift shows that a uniform in-plane lattice constant in the nanowire segments satisfactorily describes the resonant Raman spectra, although in reality the three-dimensional strain profile at the periphery of the quantum wells is complex. Our strain analysis is applicable beyond the InxGa1-xN/GaN system under study, and we derive universal rules for strain engineering in nanowire heterostructures.

12.
Nano Lett ; 10(1): 36-42, 2010 Jan.
Article in English | MEDLINE | ID: mdl-20028105

ABSTRACT

We report on a method for the fabrication of graphene on a silicon dioxide substrate by solid-state dissolution of an overlying stack of a silicon carbide and a nickel thin film. The carbon dissolves in the nickel by rapid thermal annealing. Upon cooling, the carbon segregates to the nickel surface forming a graphene layer over the entire nickel surface. By wet etching of the nickel layer, the graphene layer was allowed to settle on the original substrate. Scanning tunneling microscopy (STM) as well as Raman spectroscopy has been performed for characterization of the layers. Further insight into the morphology of the layers has been gained by Raman mapping indicating micrometer-size graphene grains. Devices for electrical measurement have been manufactured exhibiting a modulation of the transfer current by backgate electric fields. The presented approach allows for mass fabrication of polycrystalline graphene without transfer steps while using only CMOS compatible process steps.

13.
J Phys Condens Matter ; 18(32): 7703-8, 2006 Aug 16.
Article in English | MEDLINE | ID: mdl-21690881

ABSTRACT

We present the electrical spin injection from room-temperature ferromagnetic (Ga, Mn)N in nitride-based spin-polarized light-emitting diodes. The electroluminescence spectra from the spin LED indicate the existence of the spin polarization via optical polarization of emitted light up to room temperature. This demonstrates that the spin injection from the (Ga, Mn)N layer into (In, Ga)N quantum wells was achieved persisting up to room temperature by comparing it with the magnetic field dependence of the Hall resistance, which is proportional to the out-of-plane magnetization. These results support that (Ga, Mn)N is an appropriate material for a spin injection source in room-temperature operating semiconductor spintronic devices.

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