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Graphene is a model system for the study of electrons confined to a strictly two-dimensional layer1 and a large number of electronic phenomena have been demonstrated in graphene, from the fractional2, 3 quantum Hall effect to superconductivity4. However, the coupling of conduction electrons to local magnetic moments5, 6, a central problem of condensed matter physics, has not been realized in graphene, and, given carbon's lack of d or f electrons, magnetism in graphene would seem unlikely. Nonetheless, magnetism in graphitic carbon in the absence of transition-metal elements has been reported7-10, with explanations ranging from lattice defects11 to edge structures12, 13 to negative curvature regions of the graphene sheet14. Recent experiments suggest that correlated defects in highly-ordered pyrolytic graphite (HOPG) induced by proton irradiation9 or native to grain boundaries7, can give rise to ferromagnetism. Here we show that point defects (vacancies) in graphene15 are local moments which interact strongly with the conduction electrons through the Kondo effect6, 16-18 providing strong evidence that defects in graphene are indeed magnetic. The Kondo temperature TK is tunable with carrier density from 30-90 K; the high TK is a direct consequence of strong coupling of defects to conduction electrons in a Dirac material18. The results indicate that defect engineering in graphene could be used to generate and control carrier-mediated magnetism, and realize all-carbon spintronic devices. Furthermore, graphene should be an ideal system in which to probe Kondo physics in a widely tunable electron system., Comment: 22 pages, 7 figures (4 in main text, 3 in supplementary information), to appear in Nature Physics

Irradiation of graphene on SiO2 by 500 eV Ne and He ions creates defects that cause intervalley scattering as evident from a significant Raman D band intensity. The defect scattering gives a conductivity proportional to charge carrier density, with mobility decreasing as the inverse of the ion dose. The mobility decrease is four times larger than for a similar concentration of singly charged impurities. The minimum conductivity decreases proportional to the mobility to values lower than 4e^2/(pi*h), the minimum theoretical value for graphene free of intervalley scattering. Defected graphene shows a diverging resistivity at low temperature, indicating insulating behavior. The results are best explained by ion-induced formation of lattice defects that result in mid-gap states., Comment: 16 pages, 5 figures

Ultra-thin oxide (UTO) films were grown on Si(111) in ultrahigh vacuum at room temperature and characterized by scanning tunneling microscopy. The ultra-thin oxide films were then used as substrates for room temperature growth of pentacene. The apparent height of the first layer is 1.57 +/- 0.05 nm, indicating standing up pentacene grains in the thin-film phase were formed. Pentacene is molecularly resolved in the second and subsequent molecular layers. The measured in-plane unit cell for the pentacene (001) plane (ab plane) is a=0.76+/-0.01 nm, b=0.59+/-0.01 nm, and gamma=87.5+/-0.4 degrees. The films are unperturbed by the UTO's short-range spatial variation in tunneling probability, and reduce its corresponding effective roughness and correlation exponent with increasing thickness. The pentacene surface morphology follows that of the UTO substrate, preserving step structure, the long range surface rms roughness of ~0.1 nm, and the structural correlation exponent of ~1., Comment: 15 pages, 4 figures

We employ scanning probe microscopy to reveal atomic structures and nanoscale morphology of graphene-based electronic devices (i.e. a graphene sheet supported by an insulating silicon dioxide substrate) for the first time. Atomic resolution STM images reveal the presence of a strong spatially dependent perturbation, which breaks the hexagonal lattice symmetry of the graphitic lattice. Structural corrugations of the graphene sheet partially conform to the underlying silicon oxide substrate. These effects are obscured or modified on graphene devices processed with normal lithographic methods, as they are covered with a layer of photoresist residue. We enable our experiments by a novel cleaning process to produce atomically-clean graphene sheets., Comment: 13 pages, 4 figures

Spatial step edge fluctuations on a multi-component surface of Al/Si(111)-(root3 x root3) were measured via scanning tunneling microscopy over a temperature range of 720K-1070K, for step lengths of L = 65-160 nm. Even though the time scale of fluctuations of steps on this surface varies by orders of magnitude over the indicated temperature ranges, measured first-passage spatial persistence and survival probabilities are temperature independent. The power law functional form for spatial persistence probabilities is confirmed and the symmetric spatial persistence exponent is measured to be theta = 0.498 +/- 0.062 in agreement with the theoretical prediction theta = 1/2. The survival probability is found to scale directly with y/L, where y is the distance along the step edge. The form of the survival probabilities agree quantitatively with the theoretical prediction, which yields exponential decay in the limit of small y/L. The decay constant is found experimentally to be ys/L= 0.076 +/- 0.033 for y/L <= 0.2., Comment: 21 pages, 6 figures

Pentacenequinone (PnQ) impurities have been introduced into a pentacene source material in a controlled manner to quantify the relative effects of the impurity content on grain boundary structure and thin film nucleation. Atomic force microscopy (AFM) has been employed to directly characterize films grown using 0.0-7.5% PnQ by weight in the source material. Analysis of the distribution of capture zones areas of submonolayer islands as a function of impurity content shows that for large PnQ content the critical nucleus size for forming a Pn island is smaller than for low PnQ content. This result indicates a favorable energy for formation of Pn-PnQ complexes, which in turn suggests that the primary effect of PnQ on Pn mobility may arise from homogeneous distribution of PnQ defects., Comment: 16 Pages, 5 figures, 1 Table

The 1/f noise in pentacene thin film transistors has been measured as a function of device thickness from well above the effective conduction channel thickness to only two conducting layers. Over the entire thickness range, the spectral noise form is 1/f, and the noise parameter varies as (gate voltage)-1, confirming that the noise is due to mobility fluctuations, even in the thinnest films. Hooge's parameter varies as an inverse power-law with conductivity for all film thicknesses. The magnitude and transport characteristics of the spectral noise are well explained in terms of percolative effects arising from the grain boundary structure., Comment: 13 pages, 4 figures, Published

Direct correlation between temporal structural fluctuations and electron wind force is demonstrated, for the first time, by STM imaging and analysis of atomically-resolved motion on a thin film surface under large applied current (10e5 Amp/sqare cm). The magnitude of the momentum transfer between current carriers and atoms in the fluctuating structure is at least five to fifteen times (plus or minus one sigma range) larger than for freely diffusing adatoms. The corresponding changes in surface resistivity will contribute significant fluctuation signature to nanoscale electronic properties., Comment: 15 pages

Supported nanoscale lead crystallites with a step emerging from a non-centered screw dislocation on the circular top facet were prepared by rapid cooling from just above the melting temperature. STM observations of the top facet show a nonuniform rotation rate and shape of the spiral step as the crystallite relaxes. These features can be accurately modeled using curvature driven dynamics, as in classical models of spiral growth, with boundary conditions fixing the dislocation core and regions of the step lying along the outer facet edge., Comment: 4 pages, 3 figures, to be published in Physical Review Letters

The effects of sampling rate and total measurement time have been determined for single-point measurements of step fluctuations within the context of first-passage properties. Time dependent STM has been used to evaluate step fluctuations on Ag(111) films grown on mica as a function of temperature (300-410 K), on screw dislocations on the facets of Pb crystallites at 320K, and on Al-terminated Si(111) over the temperature range 770K - 970K. Although the fundamental time constant for step fluctuations on Ag and Al/Si varies by orders of magnitude over the temperature ranges of measurement, no dependence of the persistence amplitude on temperature is observed. Instead, the persistence probability is found to scale directly with t/Dt where Dt is the time interval used for sampling. Survival probabilities show a more complex scaling dependence which includes both the sampling interval and the total measurement time tm. Scaling with t/Dt occurs only when Dt/tm is a constant. We show that this observation is equivalent to theoretical predictions that the survival probability will scale as Dt/L^z, where L is the effective length of a step. This implies that the survival probability for large systems, when measured with fixed values of tm or Dt should also show little or no temperature dependence., Comment: 27 pages, 10 figures

In a recent comment [1], Armitage and Hu have suggested that our experiment observing dichroism in angle resolved photoemission (ARPES) [2] could not be conclusively interpreted as arising from time reversal symmetry breaking, arguing that our observations are likely due to structural effects. The concerns expressed by Armitage and Hu that our results could be due to a change in the mirror plane are as important as they are obvious. In fact the first part of their comment merely restates the results of Simon and Varma [3] about the relationship and contrast of effects due to time reversal symmetry breaking and those caused by crystallographic changes. In any test of time reversal symmetry one must ensure that parity alone is not inducing the observed changes. We have indeed considered this issue very carefully in the course of our study [2] and it is precisely the lack of temperature dependent structural changes significant enough to explain the magnitude of the observed dichroism that forced us to conclude that time reversal symmetry breaking is the only plausible explanation. Furthermore, recent experiments by Borisenko, et al. [4] confirm that changes in the mirror plane are unmeasurably small.

When matter undergoes a phase transition from one state to another, usually a change in symmetry is observed, as some of the symmetries exhibited are said to be spontaneously broken. The superconducting phase transition in the underdoped high-Tc superconductors is rather unusual, in that it is not a mean-field transition as other superconducting transitions are. Instead, it is observed that a pseudo-gap in the electronic excitation spectrum appears at temperatures T* higher than Tc, while phase coherence, and superconductivity, are established at Tc (Refs. 1, 2). One would then wish to understand if T* is just a crossover, controlled by fluctuations in order which will set in at the lower Tc (Refs. 3, 4), or whether some symmetry is spontaneously broken at T* (Refs. 5-10). Here, using angle-resolved photoemission with circularly polarized light, we find that, in the pseudogap state, left-circularly polarized photons give a different photocurrent than right-circularly polarized photons, and therefore the state below T* is rather unusual, in that it breaks time reversal symmetry11. This observation of a phase transition at T* provides the answer to a major mystery of the phase diagram of the cuprates. The appearance of the anomalies below T* must be related to the order parameter that sets in at this characteristic temperature ., Comment: 11 pages, 4 figures