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Register a new userSingle Spin Localization and Manipulation in Graphene Open-Shell Nanostructures
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Predictions state that graphene can spontaneously develop magnetism from the Coulomb repulsion of its $pi$-electrons, but its experimental verification has been a challenge. Here, we report on the observation and manipulation of individual magnetic moments localized in graphene nanostructures on a Au(111) surface. Using scanning tunneling spectroscopy, we detected the presence of single electron spins localized around certain zigzag sites of the carbon backbone via the Kondo effect. Two near-by spins were found coupled into a singlet ground state, and the strength of their exchange interaction was measured via singlet-triplet inelastic tunnel electron excitations. Theoretical simulations demonstrate that electron correlations result in spin-polarized radical states with the experimentally observed spatial distributions. Hydrogen atoms bound to these radical sites quench their magnetic moment, permitting us to switch the spin of the nanostructure using the tip of the microscope.
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Two-dimensional (2D) materials for their versatile band structures and strictly 2D nature have attracted considerable attention over the past decade. Graphene is a robust material for spintronics owing to its weak spin-orbit and hyperfine interactions, while monolayer transition metal dichalcogenides (TMDs) possess a Zeeman effect-like band splitting in which the spin and valley degrees of freedom are nondegenerate. The surface states of topological insulators (TIs) exhibit a spin-momentum locking that opens up the possibility of controlling the spin degree of freedom in the absence of an external magnetic field. Nanostructures made of these materials are also viable for use in quantum computing applications involving the superposition and entanglement of individual charge and spin quanta. In this article, we review a selection of transport studies addressing the confinement and manipulation of charges in nanostructures fabricated from various 2D materials. We supply the entry-level knowledge for this field by first introducing the fundamental properties of 2D bulk materials followed by the theoretical background relevant to the physics of nanostructures. Subsequently, a historical review of experimental development in this field is presented, from the early demonstration of graphene nanodevices on SiO2 substrate to more recent progress in utilizing hexagonal boron nitride to reduce substrate disorder. In the second part of this article, we extend our discussion to TMDs and TI nanostructures. We aim to outline the current challenges and suggest how future work will be geared towards developing spin qubits in 2D materials.
Spin Hall effects have surged as promising phenomena for spin logics operations without ferromagnets. However, the magnitude of the detected electric signals at room temperature in metallic systems has been so far underwhelming. Here, we demonstrate a two-order of magnitude enhancement of the signal in monolayer graphene/Pt devices when compared to their fully metallic counterparts. The enhancement stems in part from efficient spin injection and the large resistivity of graphene but we also observe 100% spin absorption in Pt and find an unusually large effective spin Hall angle of up to 0.15. The large spin-to-charge conversion allows us to characterise spin precession in graphene under the presence of a magnetic field. Furthermore, by developing an analytical model based on the 1D diffusive spin-transport, we demonstrate that the effective spin-relaxation time in graphene can be accurately determined using the (inverse) spin Hall effect as a means of detection. This is a necessary step to gather full understanding of the consequences of spin absorption in spin Hall devices, which is known to suppress effective spin lifetimes in both metallic and graphene systems.
Intense efforts have been made in recent years to realize nonlinear optical interactions at the single-photon level. Much of this work has focused on achieving strong third-order nonlinearities, such as by using single atoms or other quantum emitters while the possibility of achieving strong second-order nonlinearities remains unexplored. Here, we describe a novel technique to realize such nonlinearities using graphene, exploiting the strong per-photon fields associated with tightly confined graphene plasmons in combination with spatially nonlocal nonlinear optical interactions. We show that in properly designed graphene nanostructures, these conditions enable extremely strong internal down-conversion between a single quantized plasmon and an entangled plasmon pair, or the reverse process of second harmonic generation. A separate issue is how such strong internal nonlinearities can be observed, given the nominally weak coupling between these plasmon resonances and free-space radiative fields. On one hand, by using the collective coupling to radiation of nanostructure arrays, we show that the internal nonlinearities can manifest themselves as efficient frequency conversion of radiative fields at extremely low input powers. On the other hand, the development of techniques to efficiently couple to single nanostructures would allow these nonlinear processes to occur at the level of single input photons.
Single-molecule memory device based on a single-molecule magnet (SMM) is one of the ultimate goals of semiconductor nanofabrication technologies. Here, we study how to manipulate and readout the SMMs two spin-state of stored information that characterized by the maximum and minimum average value of the $Z$-component of the total spin of the SMM and the conduction-electron, which are recognized as the information bits $1$ and $0$. We demonstrate that the switching time depends on both the sequential tunneling gap $varepsilon_{se}$ and the spin-selection-rule allowed transition-energy $varepsilon_{trans}$, which can be tuned by the gate voltage. In particular, when the external bias voltage is turned off, in the cases of the unoccupied and doubly-occupied ground eigenstates, the time derivative of the transport current can be used to read out the SMMs two spin-state of stored information. Moreover, the tunneling strength of and the asymmetry of the SMM-electrode coupling have a strong influence on the switching time, but that have a slight influence on the readout time that being on the order of nanoseconds. Our results suggest a SMM-based memory device, and provide fundamental insight into the electrical controllable manipulation and readout of the SMMs two spin-state of stored information.
Organometallic hexahapto chromium metal complexation of single layer graphene, which involves constructive rehybridization of the graphene pi-system with the vacant chromium d orbital, leads to field effect devices which retain a high degree of the mobility with enhanced on-off ratio. This hexahapto mode of bonding between metal and graphene is quite distinct from the modification in electronic structure induced by conventional covalent sigma-bond formation with creation of sp3 carbon centers in graphene lattice and this chemistry is reversible.
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