Dimer Coupling Energies of the Si(001) Surface.

The coupling energies between the buckled dimers of the Si(001) surface were determined through analysis of the anisotropic critical behavior of its order-disorder phase transition. Spot profiles in high-resolution low-energy electron diffraction as a function of temperature were analyzed within the framework of the anisotropic two-dimensional Ising model. The validity of this approach is justified by the large ratio of correlation lengths, ξ_{∥}^{+}/ξ_{⊥}^{+}=5.2 of the fluctuating c(4×2) domains above the critical temperature T_{c}=(190.6±10) K. We obtain effective couplings J_{∥}=(-24.9±1.3) meV along the dimer rows and J_{⊥}=(-0.8±0.1) meV across the dimer rows, i.e., antiferromagneticlike coupling of the dimers with c(4×2) symmetry.

A Raman probe of phonons and electron-phonon interactions in the Weyl semimetal NbIrTe4.

There is tremendous interest in measuring the strong electron-phonon interactions seen in topological Weyl semimetals. The semimetal NbIrTe4 has been proposed to be a Type-II Weyl semimetal with 8 pairs of opposite Chirality Weyl nodes which are very close to the Fermi energy. We show using polarized angular-resolved micro-Raman scattering at two excitation energies that we can extract the phonon mode dependence of the Raman tensor elements from the shape of the scattering efficiency versus angle. This van der Waals semimetal with broken inversion symmetry and 24 atoms per unit cell has 69 possible phonon modes of which we measure 19 modes with frequencies and symmetries consistent with Density Functional Theory calculations. We show that these tensor elements vary substantially in a small energy range which reflects a strong variation of the electron-phonon coupling for these modes.

Ultrafast photoinduced band splitting and carrier dynamics in chiral tellurium nanosheets.

Trigonal tellurium (Te) is a chiral semiconductor that lacks both mirror and inversion symmetries, resulting in complex band structures with Weyl crossings and unique spin textures. Detailed time-resolved polarized reflectance spectroscopy is used to investigate its band structure and carrier dynamics. The polarized transient spectra reveal optical transitions between the uppermost spin-split H4 and H5 and the degenerate H6 valence bands (VB) and the lowest degenerate H6 conduction band (CB) as well as a higher energy transition at the L-point. Surprisingly, the degeneracy of the H6 CB (a proposed Weyl node) is lifted and the spin-split VB gap is reduced upon photoexcitation before relaxing to equilibrium as the carriers decay. Using ab initio density functional theory (DFT) calculations, we conclude that the dynamic band structure is caused by a photoinduced shear strain in the Te film that breaks the screw symmetry of the crystal. The band-edge anisotropy is also reflected in the hot carrier decay rate, which is a factor of two slower along the c-axis than perpendicular to it. The majority of photoexcited carriers near the band-edge are seen to recombine within 30 ps while higher lying transitions observed near 1.2 eV appear to have substantially longer lifetimes, potentially due to contributions of intervalley processes in the recombination rate. These new findings shed light on the strong correlation between photoinduced carriers and electronic structure in anisotropic crystals, which opens a potential pathway for designing novel Te-based devices that take advantage of the topological structures as well as strong spin-related properties.

Temperature-Controlled Rotational Epitaxy of Graphene.

When graphene is placed on a crystalline surface, the periodic structures within the layers superimpose and moiré superlattices form. Small lattice rotations between the two materials in contact strongly modify the moiré lattice parameter, upon which many electronic, vibrational, and chemical properties depend. While precise adjustment of the relative orientation in the degree- and sub-degree-range can be achieved via careful deterministic transfer of graphene, we report on the spontaneous reorientation of graphene on a metallic substrate, Ir(111). We find that selecting a substrate temperature between 1530 and 1000 K during the growth of graphene leads to distinct relative rotational angles of 0°, ± 0.6°, ±1.1°, and ±1.7°. When modeling the moiré superlattices as two-dimensional coincidence networks, we can ascribe the observed rotations to favorable low-strain graphene structures. The dissimilar thermal expansion of the substrate and graphene is regarded as an effective compressive biaxial pressure that is more easily accommodated in graphene by small rotations rather than by compression.

Strong Hot Carrier Effects in Single Nanowire Heterostructures.

We use transient Rayleigh scattering to study the thermalization of hot photoexcited carriers in single GaAs0.7Sb0.3/InP nanowire heterostructures. By comparing the energy loss rate in single core-only GaAs0.7Sb0.3 nanowires which do not show substantial hot carrier effects with the core-shell nanowires, we show that the presence of an InP shell substantially suppresses the longitudinal optical phonon emission rate at low temperatures which then leads to strong hot carrier effects.

Revealing Optical Transitions and Carrier Recombination Dynamics within the Bulk Band Structure of Bi2Se3.

Bismuth selenide (Bi2Se3) is a prototypical 3D topological insulator whose Dirac surface states have been extensively studied theoretically and experimentally. Surprisingly little, however, is known about the energetics and dynamics of electrons and holes within the bulk band structure of the semiconductor. We use mid-infrared femtosecond transient reflectance measurements on a single nanoflake to study the ultrafast thermalization and recombination dynamics of photoexcited electrons and holes within the extended bulk band structure over a wide energy range (0.3 to 1.2 eV). Theoretical modeling of the reflectivity spectral line shapes at 10 K demonstrates that the electrons and holes are photoexcited within a dense and cold electron gas with a Fermi level positioned well above the bottom of the lowest conduction band. Direct optical transitions from the first and the second spin-orbit split valence bands to the Fermi level above the lowest conduction band minimum are identified. The photoexcited carriers thermalize rapidly to the lattice temperature within a couple of picoseconds due to optical phonon emission and scattering with the cold electron gas. The minority carrier holes recombine with the dense electron gas within 150 ps at 10 K and 50 ps at 300 K. Such knowledge of interaction of electrons and holes within the bulk band structure provides a foundation for understanding how such states interact dynamically with the topologically protected Dirac surface states.

Graphene-Complex-Oxide Nanoscale Device Concepts.

The integration of graphene with complex-oxide heterostructures such as LaAlO3/SrTiO3 offers the opportunity to combine the multifunctional properties of an oxide interface with the exceptional electronic properties of graphene. The ability to control interface conduction through graphene and understanding how it affects the intrinsic properties of an oxide interface are critical to the technological development of multifunctional devices. Here we demonstrate several device archetypes in which electron transport at an oxide interface is modulated using a patterned graphene top-gate. Nanoscale devices are fabricated at the oxide interface by conductive atomic force microscope (c-AFM) lithography, and transport measurements are performed as a function of the graphene gate voltage. Experiments are performed with devices written adjacent to or directly underneath the graphene gate. Distinct capabilities of this approach include the ability to create highly flexible device configurations, the ability to modulate carrier density at the oxide interface, and the ability to control electron transport up to the single-electron tunneling regime, while maintaining intrinsic transport properties of the oxide interface. Our results facilitate the design of a variety of nanoscale devices that combine excellent transport properties of these two proximal two-dimensional electron systems.

Room-Temperature Quantum Transport Signatures in Graphene/LaAlO3 /SrTiO3 Heterostructures.

High mobility graphene field-effect devices, fabricated on the complex-oxide heterostructure LaAlO3 /SrTiO3 , exhibit quantum interference signatures up to room temperature. The oxide material is believed to play a critical role in suppressing short-range and phonon contributions to scattering. The ability to maintain pseudospin coherence at room temperature holds promise for the realization of new classical and quantum information technologies.

Observation of Ground- and Excited-State Charge Transfer at the C60/Graphene Interface.

We examine charge transfer interactions in the hybrid system of a film of C60 molecules deposited on single-layer graphene using Raman spectroscopy and Terahertz (THz) time-domain spectroscopy. In the absence of photoexcitation, we find that the C60 molecules in the deposited film act as electron acceptors for graphene, yielding increased hole doping in the graphene layer. Hole doping of the graphene film by a uniform C60 film at a level of 5.6 × 10(12)/cm(2) or 0.04 holes per interfacial C60 molecule was determined by the use of both Raman and THz spectroscopy. We also investigate transient charge transfer occurring upon photoexcitation by femtosecond laser pulses with a photon energy of 3.1 eV. The C60/graphene hybrid exhibits a short-lived (ps) decrease in THz conductivity, followed by a long-lived increase in conductivity. The initial negative photoconductivity transient, which decays within 2 ps, reflects the intrinsic photoresponse of graphene. The longer-lived positive conductivity transient, with a lifetime on the order of 100 ps, is attributed to photoinduced hole doping of graphene by interfacial charge transfer. We discuss possible microscopic pathways for hot carrier processes in the hybrid system.

Interplay between forward and backward scattering of spin-orbit split surface states of Bi(111).

The electronic structure at the surface of Bi(111) enables us to study the effect of defects scattering into multiple channels. By performing scanning tunneling spectroscopy near step edges, we analyze the resulting oscillations in the local density of electronic states (LDOS) as function of position. At a given energy, forward and backward scattering not only occur simultaneously but may contribute to the same scattering vector Δk. If the scattering phase of both processes differs by π and the amplitudes are almost equal, the oscillations cancel out. A sharp dip in the magnitude of the Fourier transform of the LDOS marks the crossover between forward and backward scattering channels.

Observation of a transient decrease in terahertz conductivity of single-layer graphene induced by ultrafast optical excitation.

We have measured the terahertz frequency-dependent sheet conductivity and its transient response following femtosecond optical excitation for single-layer graphene samples grown by chemical vapor deposition. The conductivity of the unexcited graphene sheet, which was spontaneously doped, showed a strong free-carrier response. The THz conductivity matched a Drude model over the available THz spectral range and yielded an average carrier scattering time of 70 fs. Upon photoexcitation, we observed a transient decrease in graphene conductivity. The THz frequency-dependence of the graphene photoresponse differs from that of the unexcited material but remains compatible with a Drude form. We show that the negative photoconductive response arises from an increase in the carrier scattering rate, with a minor offsetting increase in the Drude weight. This behavior, which differs in sign from that reported previously for epitaxial graphene, is expected for samples with relatively high mobilities and doping levels. The photoinduced conductivity transient has a picosecond lifetime and is associated with nonequilibrium excitation conditions in the graphene.

Interplay of wrinkles, strain, and lattice parameter in graphene on iridium.

Following graphene growth by thermal decomposition of ethylene on Ir(111) at high temperatures we analyzed the strain state and the wrinkle formation kinetics as function of temperature. Using the moiré spot separation in a low energy electron diffraction pattern as a magnifying mechanism for the difference in the lattice parameters between Ir and graphene, we achieved an unrivaled relative precision of ±0.1 pm for the graphene lattice parameter. Our data reveals a characteristic hysteresis of the graphene lattice parameter that is explained by the interplay of reversible wrinkle formation and film strain. We show that graphene on Ir(111) always exhibits residual compressive strain at room temperature. Our results provide important guidelines for strategies to avoid wrinkling.