Confocal Raman spectroscopy has emerged as a major, versatile workhorse for the non-invasive characterization of graphene. Although it is successfully used to determine the number of layers, the ...quality of edges, and the effects of strain, doping and disorder, the nature of the experimentally observed broadening of the most prominent Raman 2D line has remained unclear. Here we show that the observed 2D line width contains valuable information on strain variations in graphene on length scales far below the laser spot size, that is, on the nanometre-scale. This finding is highly relevant as it has been shown recently that such nanometre-scaled strain variations limit the carrier mobility in high-quality graphene devices. Consequently, the 2D line width is a good and easily accessible quantity for classifying the crystalline quality, nanometre-scale flatness as well as local electronic properties of graphene, all important for future scientific and industrial applications.
By successive oxygen treatments of graphene nonlocal spin-valve devices we achieve a gradual increase of the contact-resistance-area products (R sub(c)A) of Co/MgO spin injection and detection ...electrodes and a transition from linear to nonlinear characteristics in the respective differential dV-dI curves. With this manipulation of the contacts, both spin lifetime and the amplitude of the spin signal can significantly be increased by a factor of seven in the same device. This demonstrates that contact-induced spin dephasing is the bottleneck for spin transport in graphene devices with small R sub(c)A values. With increasing R sub(c)A values, we furthermore observe the appearance of a second charge neutrality point (CNR) in gate-dependent resistance measurements. Simultaneously, we observe a decrease of the gate voltage separation between the two CNPs. The strong enhancement of the spin-transport properties as well as the changes in charge transport are explained by a gradual suppression of a Co-graphene interaction by improving the oxide barrier during oxygen treatment.
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•We review the spin and charge transport in graphene-based spin-valve devices.•Challenges and recent advances in the field of device fabrication are summarized.•We discuss ...shortcomings in the determination of spin lifetimes and carrier mobilities.•Spin injection and detection electrodes can be the bottleneck for spin transport.•Contacts can result in a second charge neutrality point in charge transport.
In this review we discuss spin and charge transport properties in graphene-based single-layer and few-layer spin-valve devices. We give an overview of challenges and recent advances in the field of device fabrication and discuss two of our fabrication methods in more detail which result in distinctly different device performances. In the first class of devices, Co/MgO electrodes are directly deposited onto graphene which results in rough MgO-to-Co interfaces and favor the formation of conducting pinholes throughout the MgO layer. We show that the contact resistance area product (RcA) is a benchmark for spin transport properties as it scales with the measured spin lifetime in these devices indicating that contact-induced spin dephasing is the bottleneck for spin transport even in devices with large RcA values. In a second class of devices, Co/MgO electrodes are first patterned onto a silicon substrate. Subsequently, a graphene-hBN heterostructure is directly transferred onto these prepatterned electrodes which provides improved interface properties. This is seen by a strong enhancement of both charge and spin transport properties yielding charge carrier mobilities exceeding 20,000cm2/(Vs) and spin lifetimes up to 3.7ns at room temperature. We discuss several shortcomings in the determination of both quantities which complicates the analysis of both extrinsic and intrinsic spin scattering mechanisms. Furthermore, we show that contacts can be the origin of a second charge neutrality point in gate dependent resistance measurements which is influenced by the quantum capacitance of the underlying graphene layer.
We investigate spin and charge transport in both single and bilayer graphene nonlocal spin-valve devices. An inverse dependence of the spin lifetime taus on the carrier mobility mu is observed in ...devices with large contact-resistance-area products (R sub(c)A > 1 kOmega mu m super(2)). Furthermore, we observe an increase of taus with increasing R sub(c)A values, demonstrating that spin transport is limited by spin dephasing underneath the electrodes. In charge transport, we measure a second contact-induced Dirac peak at negative gate voltages in devices with larger R sub(c)A values, demonstrating different transport properties in contact-covered and bare graphene parts. We argue that the existence of the second Dirac peak complicates the analysis of the carrier mobilities and the spin scattering mechanisms.
The chemical bond is one of the most powerful, yet controversial concepts in chemistry, explaining property trends in solids. Recently, a novel type of chemical bonding has been identified in several ...higher chalcogenides, characterized by a unique property portfolio, unconventional bond breaking and sharing of about one electron between adjacent atoms. Metavalent bonding is a fundamental type of bonding besides covalent, ionic and metallic bonding, raising the pertinent question, if there is a well-defined transition between metavalent and covalent bonding. For three different pseudo-binary lines, namely GeTe1-xSex, Sb2Te3(1-x)Se3x and Bi2-2xSb2xSe3, a sudden drop in several properties, including the optical dielectric constant, the Born effective charge, the electrical conductivity as well as the bond breaking is observed once a critical Se or Sb concentration is reached. This finding provides a blueprint to explore the impact of metavalent bonding on attractive properties utilized in phase change materials and thermoelectrics.
In this review we discuss spin and charge transport properties in graphene-based single-layer and few-layer spin-valve devices. We give an overview of challenges and recent advances in the field of ...device fabrication and discuss two of our fabrication methods in more detail which result in distinctly different device performances. In the first class of devices, Co/MgO electrodes are directly deposited onto graphene which results in rough MgO-to-Co interfaces and favor the formation of conducting pinholes throughout the MgO layer. We show that the contact resistance area product (R\(_c\)A) is a benchmark for spin transport properties as it scales with the measured spin lifetime in these devices indicating that contact-induced spin dephasing is the bottleneck for spin transport even in devices with large R\(_c\)A values. In a second class of devices, Co/MgO electrodes are first patterned onto a silicon substrate. Subsequently, a graphene-hBN heterostructure is directly transferred onto these prepatterned electrodes which provides improved interface properties. This is seen by a strong enhancement of both charge and spin transport properties yielding charge carrier mobilities exceeding 20000 cm\(^2\)/(Vs) and spin lifetimes up to 3.7 ns at room temperature. We discuss several shortcomings in the determination of both quantities which complicates the analysis of both extrinsic and intrinsic spin scattering mechanisms. Furthermore, we show that contacts can be the origin of a second charge neutrality point in gate dependent resistance measurements which is influenced by the quantum capacitance of the underlying graphene layer.
Recently, it has been shown that oxide barriers in graphene-based non-local spin-valve structures can be the bottleneck for spin transport. The barriers may cause spin dephasing during or right after ...electrical spin injection which limit spin transport parameters such as the spin lifetime of the whole device. An important task is to evaluate the quality of the oxide barriers of both spin injection and detection contacts in a fabricated device. To address this issue, we discuss the influence of spatially inhomogeneous oxide barriers and especially conducting pinholes within the barrier on the background signal in non-local measurements of graphene/MgO/Co spin-valve devices. By both simulations and reference measurements on devices with non-ferromagnetic electrodes, we demonstrate that the background signal can be caused by inhomogeneous current flow through the oxide barriers. As a main result, we demonstrate the existence of charge accumulation next to the actual spin accumulation signal in non-local voltage measurements, which can be explained by a redistribution of charge carriers by a perpendicular magnetic field similar to the classical Hall effect. Furthermore, we present systematic studies on the phase of the low frequency non-local ac voltage signal which is measured in non-local spin measurements when applying ac lock-in techniques. This phase has so far widely been neglected in the analysis of non-local spin transport. We demonstrate that this phase is another hallmark of the homogeneity of the MgO spin injection and detection barriers. We link backgate dependent changes of the phase to the interplay between the capacitance of the oxide barrier to the quantum capacitance of graphene.
Ternary (Bi1-xSbx)2Te3 films with an Sb content between 0 and 100% were deposited on a Si(111) substrate by means of molecular beam epitaxy. X-ray diffraction measurements confirm single crystal ...growth in all cases. The Sb content is determined by X-ray photoelectron spectroscopy. Consistent values of the Sb content are obtained from Raman spectroscopy. Scanning Raman spectroscopy reveals that the (Bi1-xSbx)2Te3 layers with an intermediate Sb content show spatial composition inhomogeneities. The observed spectra broadening in angular-resolved photoemission spectroscopy (ARPES) is also attributed to this phenomena. Upon increasing the Sb content from x=0 to 1 the ARPES measurements show a shift of the Fermi level from the conduction band to the valence band. This shift is also confirmed by corresponding magnetotransport measurements where the conductance changes from n- to p-type. In this transition region, an increase of the resistivity is found, indicating a location of the Fermi level within the band gap region. More detailed measurements in the transition region reveals that the transport takes place in two independent channels. By means of a gate electrode the transport can be changed from n- to p-type, thus allowing a tuning of the Fermi level within the topologically protected surface states.
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