arXiv subjects

Tony F. Heinz

Publications and source records attributed to Tony F. Heinz.

86 records · Page 5Linked to original sources

arXiv2010

Atomically thin MoS2: A new direct-gap semiconductor

The electronic properties of ultrathin crystals of molybdenum disulfide consisting of N = 1, 2, ... 6 S-Mo-S monolayers have been investigated by optical spectroscopy. Through characterization by absorption, photoluminescence, and photoconductivity spectroscopy, we trace the effect of quantum confinement on the material's electronic structure. With decreasing thickness, the indirect band gap, which lies below the direct gap in the bulk material, shifts upwards in energy by more than 0.6 eV. This leads to a crossover to a direct-gap material in the limit of the single monolayer. Unlike the bulk material, the MoS2 monolayer emits light strongly. The freestanding monolayer exhibits an increase in luminescence quantum efficiency by more than a factor of 1000 compared with the bulk material.

cond-mat.mtrl-sci↗

arXiv2010

Electron and optical phonon temperatures in electrically biased graphene

We examine the intrinsic energy dissipation steps in electrically biased graphene channels. By combining in-situ measurements of the spontaneous optical emission with a Raman spectroscopy study of the graphene sample under conditions of current flow, we obtain independent information on the energy distribution of the electrons and phonons. The electrons and holes contributing to light emission are found to obey a thermal distribution, with temperatures in excess of 1500 K in the regime of current saturation. The zone-center optical phonons are also highly excited and are found to be in equilibrium with the electrons. For a given optical phonon temperature, the anharmonic downshift of the Raman G-mode is smaller than expected under equilibrium conditions, suggesting that the electrons and high-energy optical phonons are not fully equilibrated with all of the phonon modes.

cond-mat.mes-hall↗

arXiv2010

Energy Transfer from Individual Semiconductor Nanocrystals to Graphene

Energy transfer from photoexcited zero-dimensional systems to metallic systems plays a prominent role in modern day materials science. A situation of particular interest concerns the interaction between a photoexcited dipole and an atomically thin metal. The recent discovery of graphene layers permits investigation of this phenomenon. Here we report a study of fluorescence from individual CdSe/ZnS nanocrystals in contact with single- and few-layer graphene sheets. The rate of energy transfer is determined from the strong quenching of the nanocrystal fluorescence. For single-layer graphene, we find a rate of ~ 4ns-1, in agreement with a model based on the dipole approximation and a tight-binding description of graphene. This rate increases significantly with the number of graphene layers, before approaching the bulk limit. Our study quantifies energy transfer to and fluorescence quenching by graphene, critical properties for novel applications in photovoltaic devices and as a molecular ruler.

physics.chem-ph↗

arXiv2010

Electronic Structure of Few-Layer Graphene: Experimental Demonstration of Strong Dependence on Stacking Sequence

The electronic structure of few-layer graphene (FLG) samples with crystalline order was investigated experimentally by infrared absorption spectroscopy for photon energies ranging from 0.2 - 1 eV. Distinct optical conductivity spectra were observed for different samples having precisely the same number of layers. The different spectra arise from the existence of two stable polytypes of FLG, namely, Bernal (AB) stacking and rhombohedral (ABC) stacking. The observed absorption features, reflecting the underlying symmetry of the two polytypes and the nature of the associated van Hone singularities, were reproduced by explicit calculations within a tight-binding model. The findings demonstrate the pronounced effect of stacking order on the electronic structure of FLG.

cond-mat.mtrl-sci↗

arXiv2010

Excitons and high-order optical transitions in individual carbon nanotubes

We examine the excitonic nature of high-lying optical transitions in single-walled carbon nanotubes by means of Rayleigh scattering spectroscopy. A careful analysis of the principal transitions of individual semiconducting and metallic nanotubes reveals that in both cases the lineshape is consistent with an excitonic model, but not one of free-carriers. For semiconducting species, side-bands are observed at ~200 meV above the third and fourth optical transitions. These features are ascribed to exciton-phonon bound states. Such side-bands are not apparent for metallic nanotubes,as expected from the reduced strength of excitonic interactions in these systems.

cond-mat.mes-hall↗

arXiv2009

Performance of Monolayer Graphene Nanomechanical Resonators with Electrical Readout

The enormous stiffness and low density of graphene make it an ideal material for nanoelectromechanical (NEMS) applications. We demonstrate fabrication and electrical readout of monolayer graphene resonators, and test their response to changes in mass and temperature. The devices show resonances in the MHz range. The strong dependence of the resonant frequency on applied gate voltage can be fit to a membrane model, which yields the mass density and built-in strain. Upon removal and addition of mass, we observe changes in both the density and the strain, indicating that adsorbates impart tension to the graphene. Upon cooling, the frequency increases; the shift rate can be used to measure the unusual negative thermal expansion coefficient of graphene. The quality factor increases with decreasing temperature, reaching ~10,000 at 5 K. By establishing many of the basic attributes of monolayer graphene resonators, these studies lay the groundwork for applications, including high-sensitivity mass detectors.

cond-mat.mes-hall↗

arXiv2009

Measurement of the Optical Conductivity of Graphene

Optical reflectivity and transmission measurements over photon energies between 0.2 and 1.2 eV were performed on single-crystal graphene samples on a transparent SiO2 substrate. For photon energies above 0.5 eV, graphene yielded a spectrally flat optical absorbance of (2.3 +/- 0.2)%. This result is in agreement with a constant absorbance of pi*alpha, or a sheet conductivity of pi*e^2/2h, predicted within a model of non-interacting massless Dirac Fermions. This simple result breaks down at lower photon energies, where both spectral and sample-to-sample variations were observed. This "non-universal" behavior is explained by including the effects of doping and finite temperature, as well as contributions from intraband transitions.

cond-mat.mtrl-sci↗

arXiv2009

Observation of an Electric-Field Induced Band Gap in Bilayer Graphene by Infrared Spectroscopy

It has been predicted that application of a strong electric field perpendicular to the plane of bilayer graphene can induce a significant band gap. We have measured the optical conductivity of bilayer graphene with an efficient electrolyte top gate for a photon energy range of 0.2 - 0.7 eV. We see the emergence of new transitions as a band gap opens. A band gap approaching 200 meV is observed when an electric field ~ 1 V/nm is applied by an electrolyte gate to the bilayer system, inducing a carrier density of about 10^13 cm-2. The magnitude of the band gap and the features observed in the infrared conductivity spectra are broadly compatible with calculations within a tight-binding model.

cond-mat.mes-hall↗

arXiv2009

The Electronic Structure of Few-Layer Graphene: Probing the Evolution from a 2-Dimensional to a 3-Dimensional Material

While preserving many of the unusual features of single-layer graphene, few-layer graphene (FLG) provides a richness and flexibility of electronic structure that render this set of materials of great interest for both fundamental studies and applications. Essential for progress, however, is an understanding of the evolution of the electronic structure of these materials with increasing layer number. In this report, the evolution of the electronic structure of FLG, for N = 1 - 8 atomic layers, has been characterized by measurements of the optical conductivity spectra. For each layer thickness N, distinctive peaks are found in the infrared range, with positions obeying a simple scaling relation. The observations are explained by a unified zone-folding scheme that generates the electronic structure for all FLG materials from that of bulk graphite.

cond-mat.mes-hall↗

arXiv2009

Probing the Intrinsic Properties of Exfoliated Graphene: Raman Spectroscopy of Free-Standing Monolayers

The properties of pristine, free-standing graphene monolayers prepared by mechanical exfoliation of graphite are investigated. The graphene monolayers, suspended over open trenches, are examined by means of spatially resolved Raman spectroscopy of the G-, D-, and 2D-phonon modes. The G-mode phonons exhibit reduced energies (1580 cm-1) and increased widths (14 cm-1) compared to the response of graphene monolayers supported on the SiO2 covered substrate. From analysis of the G-mode Raman spectra, we deduce that the free-standing graphene monolayers are essentially undoped, with an upper bound of 2x10^11 cm-2 for the residual carrier concentration. On the supported regions, significantly higher and spatially inhomogeneous doping is observed. The free-standing graphene monolayers show little local disorder, based on the very weak Raman D-mode response. The two-phonon 2D mode of the free-standing graphene monolayers is downshifted in frequency compared to that of the supported region of the samples and exhibits a narrowed, positively skewed line shape.

cond-mat.mtrl-sci↗

arXiv2008

Raman Spectroscopy of Graphene under Uniaxial Stress: Phonon Softening and Determination of the Crystallographic Orientation

We present a systematic study of the Raman spectra of optical phonons in graphene monolayers under tunable uniaxial tensile stress. Both the G and 2D bands exhibit significant red shifts. The G band splits into two distinct sub-bands (G+, G-) because of the strain-induced symmetry breaking. Raman scattering from the G+ and G- bands shows a distinctive polarization dependence that reflects the angle between the axis of the stress and the underlying graphene crystal axes. Polarized Raman spectroscopy therefore constitutes a purely optical method for the determination of the crystallographic orientation of graphene.

cond-mat.mtrl-sci↗

arXiv2008

Reversible Basal Plane Hydrogenation of Graphene

We report the chemical reaction of single-layer graphene with hydrogen atoms, generated in situ by electron-induced dissociation of hydrogen silsesquioxane (HSQ). Hydrogenation, forming sp3 C-H functionality on the basal plane of graphene, proceeds at a higher rate for single than for double layers, demonstrating the enhanced chemical reactivity of single sheet graphene. The net H atom sticking probability on single layers at 300 K is at least 0.03, which exceeds that of double layers by at least a factor of 15. Chemisorbed hydrogen atoms, which give rise to a prominent Raman D band, can be detached by thermal annealing at 100~200 degrees C. The resulting dehydrogenated graphene is "activated" when photothermally heated it reversibly binds ambient oxygen, leading to hole doping of the graphene. This functionalization of graphene can be exploited to manipulate electronic and charge transport properties of graphene devices.

cond-mat.mtrl-sci↗

arXiv2007

Variable Electron-Phonon Coupling in Isolated Metallic Carbon Nanotubes Observed by Raman Scattering

We report the existence of broad and weakly asymmetric features in the high-energy (G) Raman modes of freely suspended metallic carbon nanotubes of defined chiral index. A significant variation in peak width (from 12 cm-1 to 110 cm-1) is observed as a function of the nanotube's chiral structure. When the nanotubes are electrostatically gated, the peak widths decrease. The broadness of the Raman features is understood as the consequence of coupling of the phonon to electron-hole pairs, the strength of which varies with the nanotube chiral index and the position of the Fermi energy.

cond-mat.mtrl-sci↗

arXiv2007

High-Resolution Scanning Tunneling Microscopy Imaging of Mesoscopic Graphene Sheets on an Insulating Surface

We present scanning tunneling microscopy (STM) images of single-layer graphene crystals examined under ultrahigh vacuum conditions. The samples, with lateral dimensions on the micron scale, were prepared on a silicon dioxide surface by direct exfoliation of single crystal graphite. The single-layer films were identified using Raman spectroscopy. Topographic images of single-layer samples display the honeycomb structure expected for the full hexagonal symmetry of an isolated graphene monolayer. The absence of observable defects in the STM images is indicative of the high quality of these films. Crystals comprised of a few layers of graphene were also examined. They exhibited dramatically different STM topography, displaying the reduced three-fold symmetry characteristic of the surface of bulk graphite.

cond-mat.mes-hall↗