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Floquet theory has spawned many exciting possibilities for electronic structure control with light with enormous potential for future applications. The experimental realization in solids, however, largely remains pending. In particular, the influence of scattering on the formation of Floquet-Bloch states remains poorly understood. Here we combine time- and angle-resolved photoemission spectroscopy with time-dependent density functional theory and a two-level model with relaxation to investigate the survival of Floquet-Bloch states in the presence of scattering. We find that Floquet-Bloch states will be destroyed if scattering -- activated by electronic excitations -- prevents the Bloch electrons from following the driving field coherently. The two-level model also shows that Floquet-Bloch states reappear at high field intensities where energy exchange with the driving field dominates over energy dissipation to the bath. Our results clearly indicate the importance of long scattering times combined with strong driving fields for the successful realization of various Floquet phenomena., Comment: 27 pages, 5 figues

Van-der-Waals heterostructures show many intriguing phenomena including ultrafast charge separation following strong excitonic absorption in the visible spectral range. However, despite the enormous potential for future applications in the field of optoelectronics, the underlying microscopic mechanism remains controversial. Here we use time- and angle-resolved photoemission spectroscopy combined with microscopic many-particle theory to reveal the relevant microscopic charge transfer channels in epitaxial WS$_2$/graphene heterostructures. We find that the timescale for efficient ultrafast charge separation in the material is determined by direct tunneling at those points in the Brillouin zone where WS$_2$ and graphene bands cross, while the lifetime of the charge separated transient state is set by defect-assisted tunneling through localized sulphur vacanices. The subtle interplay of intrinsic and defect-related charge transfer channels revealed in the present work can be exploited for the design of highly efficient light harvesting and detecting devices., Comment: 37 pages, 16 figures

The challenge of next generation datacom and telecom communication is to increase the available bandwidth while reducing the size, cost and power consumption of photonic integrated circuits. Silicon (Si) photonics has emerged as a viable solution to reach these objectives. Graphene, a single-atom thick layer of carbon5, has been recently proposed to be integrated with Si photonics because of its very high mobility, fast carrier dynamics and ultra-broadband optical properties. Here, we focus on graphene photodetectors for high speed datacom and telecom applications. High speed graphene photodetectors have been demonstrated so far, however the most are based on the photo-bolometric (PB) or photo-conductive (PC) effect. These devices are characterized by large dark current, in the order of milli-Amperes , which is an impairment in photo-receivers design, Photo-thermo-electric (PTE) effect has been identified as an alternative phenomenon for light detection. The main advantages of PTE-based photodetectors are the optical power to voltage conversion, zero-bias operation and ultra-fast response. Graphene PTE-based photodetectors have been reported in literature, however high-speed optical signal detection has not been shown. Here, we report on an optimized graphene PTE-based photodetector with flat frequency response up to 65 GHz. Thanks to the optimized design we demonstrate a system test leading to direct detection of 105 Gbit s-1 non-return to zero (NRZ) and 120 Gbit s-1 4-level pulse amplitude modulation (PAM) optical signals

Several works reported increased differentiation of neuronal cells grown on graphene; however, the molecular mechanism driving axon elongation on this material has remained elusive. Here, we study the axonal transport of nerve growth factor (NGF), the neurotrophin supporting development of peripheral neurons, as a key player in the time course of axonal elongation of dorsal root ganglion neurons on graphene. We find that graphene drastically reduces the number of retrogradely transported NGF vesicles in favor of a stalled population in the first two days of culture, in which the boost of axon elongation is observed. This correlates with a mutual charge redistribution, observed via Raman spectroscopy and electrophysiological recordings. Furthermore, ultrastructural analysis indicates a reduced microtubule distance and an elongated axonal topology. Thus, both electrophysiological and structural effects can account for graphene action on neuron development. Unraveling the molecular players underneath this interplay may open new avenues for axon regeneration applications.

The adoption of graphene in electronics, optoelectronics and photonics is hindered by the difficulty in obtaining high quality material on technologically-relevant substrates, over wafer-scale sizes and with metal contamination levels compatible with industrial requirements. To date, the direct growth of graphene on insulating substrates has proved to be challenging, usually requiring metal-catalysts or yielding defective graphene. In this work, we demonstrate a metal-free approach implemented in commercially available reactors to obtain high-quality monolayer graphene on c-plane sapphire substrates via chemical vapour deposition (CVD). We identify via low energy electron diffraction (LEED), low energy electron microscopy (LEEM) and scanning tunneling microscopy (STM) measurements the Al-rich reconstruction root31R9 of sapphire to be crucial for obtaining epitaxial graphene. Raman spectroscopy and electrical transport measurements reveal high-quality graphene with mobilities consistently above 2000 cm2/Vs. We scale up the process to 4-inch and 6-inch wafer sizes and demonstrate that metal contamination levels are within the limits for back-end-of-line (BEOL) integration. The growth process introduced here establishes a method for the synthesis of wafer-scale graphene films on a technologically viable basis., Comment: 15 main text pages, 4 main text figures, 13 supplementary information pages, 12 supplementary figures, 3 supplementary tables

We systematically investigate the chemical vapor deposition growth of graphene on Ge(110) as a function of the deposition temperature close to the Ge melting point. By merging spectroscopic and morphological information, we find that the quality of graphene films depends critically on the growth temperature improving significantly by increasing this temperature in the 910-930 {\deg}C range. We correlate the abrupt improvement of the graphene quality to the formation of a quasi-liquid Ge surface occurring in the same temperature range, which determines increased atom diffusivity and sublimation rate. Being observed for diverse Ge orientations, this process is of general relevance for graphene synthesis on Ge.

We present a micrometer scale, on-chip integrated, plasmonic enhanced graphene photodetector (GPD) for telecom wavelengths operating at zero dark current. The GPD is designed and optimized to directly generate a photovoltage and has an external responsivity~12.2V/W with a 3dB bandwidth~42GHz. We utilize Au split-gates with a$\sim$100nm gap to electrostatically create a p-n-junction and simultaneously guide a surface plasmon polariton gap-mode. This increases light-graphene interaction and optical absorption and results in an increased electronic temperature and steeper temperature gradient across the GPD channel. This paves the way to compact, on-chip integrated, power-efficient graphene based photodetectors for receivers in tele and datacom modules

We use time- and angle-resolved photoemission spectroscopy (tr-ARPES) to investigate ultrafast charge transfer in an epitaxial heterostructure made of monolayer WS$_2$ and graphene. This heterostructure combines the benefits of a direct gap semiconductor with strong spin-orbit coupling and strong light-matter interaction with those of a semimetal hosting massless carriers with extremely high mobility and long spin lifetimes. We find that, after photoexcitation at resonance to the A-exciton in WS$_2$, the photoexcited holes rapidly transfer into the graphene layer while the photoexcited electrons remain in the WS$_2$ layer. The resulting charge transfer state is found to have a lifetime of $\sim1$\,ps. We attribute our findings to differences in scattering phase space caused by the relative alignment of WS$_2$ and graphene bands as revealed by high resolution ARPES. In combination with spin-selective excitation using circularly polarized light the investigated WS$_2$/graphene heterostructure might provide a new platform for efficient optical spin injection into graphene., Comment: 28 pages, 14 figures

By combining scanning probe microscopy with Raman and x-ray photoelectron spectroscopies, we investigate the evolution of CVD-grown graphene/Ge(001) as a function of the deposition temperature in close proximity to the Ge melting point, highlighting an abrupt change of the graphene's quality, morphology, electronic properties and growth mode at 930 degrees. We attribute this discontinuity to the incomplete surface melting of the Ge substrate and show how incomplete melting explains a variety of diverse and long-debated peculiar features of the graphene/Ge(001), including the characteristic nanostructuring of the Ge substrate induced by graphene overgrowth. We find that the quasi-liquid Ge layer formed close to 930 degrees is fundamental to obtain high-quality graphene, while a temperature decrease of 10 degrees already results in a wrinkled and defective graphene film., Comment: in press

The surface structure of Few-Layer Graphene (FLG) epitaxially grown on the C-face of SiC has been investigated by TM-AFM in ambient air and upon interaction with diluted aqueous solutions of bio-organic molecules (dimethyl sulfoxide, DMSO, and L-Methionine). On pristine FLG we observe nicely ordered, three-fold oriented rippled domains, with a 4.7+/-0.2 nm periodicity (small periodicity, SP) and a peak-to-valley distance in the range 0.1-0.2 nm. Upon mild interaction of the FLG surface with the molecular solution, the ripple periodicity relaxes to 6.2+/-0.2 nm (large periodicity, LP), while the peak-to-valley height increases to 0.2-0.3 nm. When additional energy is transferred to the system through sonication in solution, graphene planes are peeled off from FLG, as shown by quantitative analysis of XPS and Raman spectroscopy data which indicate a neat reduction of thickness. Upon sonication rippled domains are no longer observed. Regarding HOPG, we could not observe ripples on cleaved samples in ambient air, while LP ripples develop upon interaction with the molecular solutions. Recent literature on similar systems is not univocal regarding the interpretation of rippling. The complex of our comparative observations on FLG and HOPG can be hardly rationalized solely on the base of surface assembly of molecules, either organic molecules coming from the solution or adventitious species. We propose to consider the ripples as the manifestation of the free-energy minimization of quasi-2D layers, eventually affected by factors such as the interplane stacking, the interaction with molecules and/or with the AFM tip.

In this work we test graphene electrodes in nano-metric channel n-type Organic Field EffectTransistors (OFETs) based on thermally evaporated thin films of perylene-3,4,9,10-tetracarboxylic acid diimide derivative (PDIF-CN2). By a thorough comparison with short channel transistors made with reference gold electrodes, we found that the output characteristics of the graphene-based devices respond linearly to the applied biases, in contrast with the supra-linear trend of gold-based transistors. Moreover, short channel effects are considerably suppressed in graphene electrodes devices. More specifically, current on/off ratios independent of the channel length (L) and enhanced response for high longitudinal biases are demonstrated for L down to ~140 nm. These results are rationalized taking into account the morphological and electronic characteristics of graphene, showing that the use of graphene electrodes may help to overcome the problem of Space Charge Limited Current (SCLC) in short channel OFETs.

Black Phosphorus (bP) has emerged as an interesting addition to the category of two-dimensional materials. Surface-science studies on this material are of great interest, but they are hampered by bP's high reactivity to oxygen and water, a major challenge to scanning tunneling microscopy (STM) experiments. As a consequence, the large majority of these studies were performed by cleaving a bulk crystal in situ. Here we present a study of surface modifications on exfoliated bP flakes upon consecutive annealing steps, up to 550 C, well above the sublimation temperature of bP. In particular, our attention is focused on the temperature range 375 C - 400 C, when sublimation starts, and a controlled desorption from the surface occurs alongside with the formation of characteristic well-aligned craters. There is an open debate in the literature about the crystallographic orientation of these craters, whether they align along the zigzag or the armchair direction. Thanks to the atomic resolution provided by STM, we are able to identify the orientation of the craters with respect to the bP crystal: the long axis of the craters is aligned along the zigzag direction of bP. This allows us to solve the controversy, and, moreover, to provide insight in the underlying desorption mechanism leading to crater formation.

In this work we shed light on the early stage of the chemical vapor deposition of graphene on Ge(001) surfaces. By a combined use of microRaman and x-ray photoelectron spectroscopies, and scanning tunneling microscopy and spectroscopy, we were able to individuate a carbon precursor phase to graphene nucleation which coexists with small graphene domains. This precursor phase is made of C aggregates with different size, shape and local ordering which are not fully sp2 hybridized. In some atomic size regions these aggregates show a linear arrangement of atoms as well as the first signature of the hexagonal structure of graphene. The carbon precursor phase evolves in graphene domains through an ordering process, associated to a re-arrangement of the Ge surface morphology. This surface structuring represents the embryo stage of the hills-and-valleys faceting featured by the Ge(001) surface for longer deposition times, when the graphene domains coalesce to form a single layer graphene film.

Germanium is emerging as the substrate of choice for the growth of graphene in CMOS-compatible processes. For future application in next generation devices the accurate control over the properties of high-quality graphene synthesized on Ge surfaces, such as number of layers and domain size, is of paramount importance. Here we investigate the role of the process gas flows on the CVD growth of graphene on Ge(100). The quality and morphology of the deposited material is assessed by using microRaman spectroscopy, x-ray photoemission spectroscopy, scanning electron and atomic force microscopies. We find that by simply varying the carbon precursor flow different growth regimes - yielding to graphene nanoribbons, graphene monolayer and graphene multilayer - are established. We identify the growth conditions yielding to a layer-by-layer growth regime and report on the achievement of homogeneous monolayer graphene with an average intensity ratio of 2D and G bands in the Raman map larger than 3.

We report on room temperature THz detection by means of antenna-coupled field effect transistors fabricated by using epitaxial graphene grown on silicon carbide substrate. Two independent detection mechanisms are found: plasma wave assisted-detection and thermoelectric effect, which is ascribed to the presence of junctions along the FET channel. The superposition of the calculated functional dependence of both the plasmonic and thermoelectric photovoltages on the gate bias qualitatively well reproduces the measured photovoltages. Additionally, the sign reversal of the measured photovoltage demonstrates the stronger contribution of the plasmonic detection compared to the thermoelectric mechanism. Although responsivity improvement is necessary, these results demonstrate that plasmonic detectors fabricated by epitaxial graphene on silicon carbide are potential candidates for fast large area imaging of macroscopic samples.

This work presents a comparison of the structural, chemical and electronic properties of multi-layer graphene grown on SiC(000-1) by using two different growth approaches: thermal decomposition and chemical vapor deposition (CVD). The topography of the samples was investigated by using atomic force microscopy (AFM), and scanning electron microscopy (SEM) was performed to examine the sample on a large scale. Raman spectroscopy was used to assess the crystallinity and electronic behavior of the multi-layer graphene and to estimate its thickness in a non-invasive way. While the crystallinity of the samples obtained with the two different approaches is comparable, our results indicate that the CVD method allows for a better thickness control of the grown graphene., Comment: 6 pages, 5 figures

For many of the envisioned optoelectronic applications of graphene it is crucial to understand the sub-picosecond carrier dynamics immediately following photoexcitation, as well as the effect on the electrical conductivity - the photoconductivity. Whereas these topics have been studied using various ultrafast experiments and theoretical approaches, controversial and incomplete explanations have been put forward concerning the sign of the photoconductivity, the occurrence and significance of the creation of additional electron-hole pairs, and, in particular, how the relevant processes depend on Fermi energy. Here, we present a unified and intuitive physical picture of the ultrafast carrier dynamics and the photoconductivity, combining optical pump - terahertz probe measurements on a gate-tunable graphene device, with numerical calculations using the Boltzmann equation. We distinguish two types of ultrafast photo-induced carrier heating processes: At low (equilibrium) Fermi energy ($E_{\rm F} \lesssim$ 0.1 eV for our experiments) broadening of the carrier distribution involves interband transitions - interband heating. At higher Fermi energy ($E_{\rm F} \gtrsim$ 0.15 eV) broadening of the carrier distribution involves intraband transitions - intraband heating. Under certain conditions, additional electron-hole pairs can be created (carrier multiplication) for low $E_{\rm F}$, and hot carriers (hot-carrier multiplication) for higher $E_{\rm F}$. The resultant photoconductivity is positive (negative) for low (high) $E_{\rm F}$, which originates from the effect of the heated carrier distributions on the screening of impurities, consistent with the DC conductivity being mostly due to impurity scattering. The importance of these insights is highlighted by a discussion of the implications for graphene photodetector applications.

The pseudospin of Dirac electrons in graphene manifests itself in a peculiar momentum anisotropy for photo-excited electron-hole pairs. These interband excitations are in fact forbidden along the direction of the light polarization, and are maximum perpendicular to it. Here, we use time- and angle-resolved photoemission spectroscopy to investigate the resulting unconventional hot carrier dynamics, sampling carrier distributions as a function of energy and in-plane momentum. We first show that the rapidly-established quasi-thermal electron distribution initially exhibits an azimuth-dependent temperature, consistent with relaxation through collinear electron-electron scattering. Azimuthal thermalization is found to occur only at longer time delays, at a rate that depends on the substrate and the static doping level. Further, we observe pronounced differences in the electron and hole dynamics in n-doped samples. By simulating the Coulomb- and phonon-mediated carrier dynamics we are able to disentangle the influence of excitation fluence, screening, and doping, and develop a microscopic picture of the carrier dynamics in photo-excited graphene. Our results clarify new aspects of hot carrier dynamics that are unique to Dirac materials, with relevance for photo-control experiments and optoelectronic device applications., Comment: 23 pages, 12 figures

Electron-phonon coupling directly determines the stability of cooperative order in solids, including superconductivity, charge and spin density waves. Therefore, the ability to enhance or reduce electron-phonon coupling by optical driving may open up new possibilities to steer materials' functionalities, potentially at high speeds. Here we explore the response of bilayer graphene to dynamical modulation of the lattice, achieved by driving optically-active in-plane bond stretching vibrations with femtosecond mid-infrared pulses. The driven state is studied by two different ultrafast spectroscopic techniques. Firstly, TeraHertz time-domain spectroscopy reveals that the Drude scattering rate decreases upon driving. Secondly, the relaxation rate of hot quasi-particles, as measured by time- and angle-resolved photoemission spectroscopy, increases. These two independent observations are quantitatively consistent with one another and can be explained by a transient three-fold enhancement of the electron-phonon coupling constant. The findings reported here provide useful perspective for related experiments, which reported the enhancement of superconductivity in alkali-doped fullerites when a similar phonon mode was driven., Comment: 12 pages, 4 figures

We report on the transport properties of hybrid devices obtained by depositing graphene on a LaAlO3/SrTiO3 oxide junction hosting a 4 nm-deep two-dimensional electron system. At low graphene-oxide inter-layer bias the two electron systems are electrically isolated, despite their small spatial separation, and very efficient reciprocal gating is shown. A pronounced rectifying behavior is observed for larger bias values and ascribed to the interplay between electrostatic depletion and tunneling across the LaAlO3 barrier. The relevance of these results in the context of strongly-coupled bilayer systems is discussed., Comment: 10 pages, 3 figures

Titanium-island formation on graphene as a function of defect density is investigated. When depositing titanium on pristine graphene, titanium atoms cluster and form islands with an average diameter of about 10nm and an average height of a few atomic layers. We show that if defects are introduced in the graphene by ion bombardment, the mobility of the deposited titanium atoms is reduced and the average diameter of the islands decreases to 5nm with monoatomic height. This results in an optimized coverage for hydrogen storage applications since the actual titanium surface available per unit graphene area is significantly increased.

Quasi-free standing epitaxial graphene is obtained on SiC(0001) by hydrogen intercalation. The hydrogen moves between the 6root3 reconstructed initial carbon layer and the SiC substrate. The topmost Si atoms which for epitaxial graphene are covalently bound to this buffer layer, are now saturated by hydrogen bonds. The buffer layer is turned into a quasi-free standing graphene monolayer with its typical linear pi-bands. Similarly, epitaxial monolayer graphene turns into a decoupled bilayer. The intercalation is stable in air and can be reversed by annealing to around 900 degrees Celsius., Comment: Accepted for publication in Physical Review Letters

We consider the two dimensional version of a drainage network model introduced by Gangopadhyay, Roy and Sarkar, and show that the appropriately rescaled family of its paths converges in distribution to the Brownian web. We do so by verifying the convergence criteria proposed by Fontes, Isopi, Newman and Ravishankar., Comment: 15 pages