Ultralong 100 ns spin relaxation time in graphite at room temperature.

Graphite has been intensively studied, yet its electron spins dynamics remains an unresolved problem even 70 years after the first experiments. The central quantities, the longitudinal (T1) and transverse (T2) relaxation times were postulated to be equal, mirroring standard metals, but T1 has never been measured for graphite. Here, based on a detailed band structure calculation including spin-orbit coupling, we predict an unexpected behavior of the relaxation times. We find, based on saturation ESR measurements, that T1 is markedly different from T2. Spins injected with perpendicular polarization with respect to the graphene plane have an extraordinarily long lifetime of 100 ns at room temperature. This is ten times more than in the best graphene samples. The spin diffusion length across graphite planes is thus expected to be ultralong, on the scale of ~ 70 µm, suggesting that thin films of graphite - or multilayer AB graphene stacks - can be excellent platforms for spintronics applications compatible with 2D van der Waals technologies. Finally, we provide a qualitative account of the observed spin relaxation based on the anisotropic spin admixture of the Bloch states in graphite obtained from density functional theory calculations.

Stacking Domains and Dislocation Networks in Marginally Twisted Bilayers of Transition Metal Dichalcogenides.

We apply a multiscale modeling approach to study lattice reconstruction in marginally twisted bilayers of transition metal dichalcogenides (TMD). For this, we develop density functional theory parametrized interpolation formulae for interlayer adhesion energies of MoSe_{2}, WSe_{2}, MoS_{2}, and WS_{2}, combine those with elasticity theory, and analyze the bilayer lattice relaxation into mesoscale domain structures. Paying particular attention to the inversion asymmetry of TMD monolayers, we show that 3R and 2H stacking domains, separated by a network of dislocations develop for twist angles θ^{∘}<θ_{P}^{∘}∼2.5° and θ^{∘}<θ_{AP}^{∘}∼1° for, respectively, bilayers with parallel (P) and antiparallel (AP) orientation of the monolayer unit cells and suggest how the domain structures would manifest itself in local probe scanning of marginally twisted P and AP bilayers.

The direct-to-indirect band gap crossover in two-dimensional van der Waals Indium Selenide crystals.

The electronic band structure of van der Waals (vdW) layered crystals has properties that depend on the composition, thickness and stacking of the component layers. Here we use density functional theory and high field magneto-optics to investigate the metal chalcogenide InSe, a recent addition to the family of vdW layered crystals, which transforms from a direct to an indirect band gap semiconductor as the number of layers is reduced. We investigate this direct-to-indirect bandgap crossover, demonstrate a highly tuneable optical response from the near infrared to the visible spectrum with decreasing layer thickness down to 2 layers, and report quantum dot-like optical emissions distributed over a wide range of energy. Our analysis also indicates that electron and exciton effective masses are weakly dependent on the layer thickness and are significantly smaller than in other vdW crystals. These properties are unprecedented within the large family of vdW crystals and demonstrate the potential of InSe for electronic and photonic technologies.

Enhanced NMR relaxation of Tomonaga-Luttinger liquids and the magnitude of the carbon hyperfine coupling in single-wall carbon nanotubes.

Recent transport measurements [Churchill et al. Nature Phys. 5, 321 (2009)] found a surprisingly large, 2-3 orders of magnitude larger than usual (13)C hyperfine coupling (HFC) in (13)C enriched single-wall carbon nanotubes. We formulate the theory of the nuclear relaxation time in the framework of the Tomonaga-Luttinger liquid theory to enable the determination of the HFC from recent data by Ihara et al. [Europhys. Lett. 90, 17,004 (2010)]. Though we find that 1/T(1) is orders of magnitude enhanced with respect to a Fermi-liquid behavior, the HFC has its usual, small value. Then, we reexamine the theoretical description used to extract the HFC from transport experiments and show that similar features could be obtained with HFC-independent system parameters.

Surface relaxation and stress for 5d transition metals.

Using the density functional theory, we present a systematic theoretical study of the layer relaxation and surface stress of 5d transition metals. Our calculations predict layer contractions for all surfaces, except for the (111) surface of face centered cubic Pt and Au, where slight expansions are obtained similarly to the case of the 4d series. We also find that the relaxations of the close packed surfaces decrease with increasing occupation number through the 5d series. The surface stress for the relaxed, most closely packed surfaces shows similar atomic number dependence as the surface energy. Using Cammarata's model and our calculated surface stress and surface energy values, we examine the possibility of surface reconstructions, which is in reasonable agreement with the experimental observations.

Electron spin resonance signal of Luttinger liquids and single-wall carbon nanotubes.

A comprehensive theory of electron spin resonance (ESR) for a Luttinger liquid state of correlated metals is presented. The ESR measurables such as the signal intensity and the linewidth are calculated in the framework of Luttinger liquid theory with broken spin rotational symmetry as a function of magnetic field and temperature. We obtain a significant temperature dependent homogeneous line broadening which is related to the spin-symmetry breaking and the electron-electron interaction. The result crosses over smoothly to the ESR of itinerant electrons in the noninteracting limit. These findings explain the absence of the long-sought ESR signal of itinerant electrons in single-wall carbon nanotubes when considering realistic experimental conditions.

Isotope engineering of carbon nanotube systems.

The synthesis of a unique isotope engineered system, double-wall carbon nanotubes with natural carbon outer and highly 13C enriched inner walls, is reported from isotope enriched fullerenes encapsulated in single-wall carbon nanotubes (SWCNTs). The material allows the observation of the D line of the highly defect-free inner tubes that can be related to a curvature induced enhancement of the electron-phonon coupling. Ab initio calculations explain the inhomogeneous broadening of inner tube Raman modes due to the distribution of different isotopes. Nuclear magnetic resonance shows a significant contrast of the isotope enriched inner SWCNTs compared to other carbon phases and provides a macroscopic measure of the inner tube mass content. The high curvature of the small diameter inner tubes manifests in an increased distribution of the chemical shift tensor components.

Unusual high degree of unperturbed environment in the interior of single-wall carbon nanotubes.

Double wall carbon nanotubes were prepared by vacuum annealing of single wall carbon nanotubes filled with C60. Strong evidence is provided for a highly defect free and unperturbed environment in the interior of the tubes. This is concluded from unusual narrow Raman lines for the radial breathing mode of the inner tubes. Lorentzian linewidths scale down to 0.35 cm(-1) which is almost 10 times smaller than linewidths reported so far for this mode. A splitting is observed for the majority of the Raman lines. It is considered to originate from tube-tube interaction between one inner tube and several different outer tubes. The highest RBM frequency detected is 484 cm(-1) corresponding to a tube diameter of only 0.50 nm. Labeling of the Raman lines with the folding vector is provided for all inner tubes. This labeling is supported by density functional calculations.

Origin of the fine structure of the Raman D band in single-wall carbon nanotubes.

Experiments show that the D bands of bundles of single wall carbon nanotubes have a fine structure, apparently consisting of more than one subband. Using the double resonance theory, we calculate for the first time the D band for a sample of a given diameter distribution for seven different laser excitation energies in a wide range. In addition, a detailed theoretical explanation for the fine structure of the D band is provided. The calculated results agree well with experiments and show that the main factors in determining the fine structure are an enhanced trigonal warping of the phonon dispersion, the presence of a diameter distribution in the sample, and--most importantly--the resonance from the Van Hove singularities.