Graphene is emerging as a viable alternative to conventional optoelectronic, plasmonic and nanophotonic materials. The interaction of light with charge carriers creates an out-ofequilibrium distribution, which relaxes on an ultrafast timescale to a hot Fermi-Dirac distribution, that subsequently cools emitting phonons. Although the slower relaxation mechanisms have been extensively investigated, the initial stages still pose a challenge. Experimentally, they defy the resolution of most pump-probe setups, due to the extremely fast sub-100 fs carrier dynamics. Theoretically, massless Dirac fermions represent a novel many-body problem, fundamentally different from Schrödinger fermions. Here we combine pump-probe spectroscopy with a microscopic theory to investigate electron-electron interactions during the early stages of relaxation. We identify the mechanisms controlling the ultrafast dynamics, in particular the role of collinear scattering. This gives rise to Auger processes, including charge multiplication, which is key in photovoltage generation and photodetectors.

We study by Raman scattering the shear and layer breathing modes in multilayer MoS2. These are identified by polarization measurements and symmetry analysis. Their positions change with the number of layers, with different scaling for odd and even layers. A chain model explains the results, with general applicability to any layered material, and allows one to monitor their thickness.

We report the exfoliation of graphite in aqueous solutions under high shear rate [∼ 108 s–1] turbulent flow conditions, with a 100% exfoliation yield. The material is stabilized without centrifugation at concentrations up to 100 g/L using carboxymethylcellulose sodium salt to formulate conductive printable inks. The sheet resistance of blade coated films is below ∼2Ω/□. This is a simple and scalable production route for conductive inks for large-area printing in flexible electronics.

We report an on-chip integrated metal graphene–silicon plasmonic Schottky photodetector with 85 mA/W responsivity at 1.55 μm and 7% internal quantum efficiency. This is one order of magnitude higher than metal–silicon Schottky photodetectors operated in the same conditions. At a reverse bias of 3 V, we achieve avalanche multiplication, with 0.37A/W responsivity and avalanche photogain ∼2. This paves the way to graphene integrated silicon photonics.

Graphene is used as the thinnest possible spacer between gold nanoparticles and a gold substrate. This creates a robust, repeatable, and stable subnanometer gap for massive plasmonic field enhancements. White light spectroscopy of single 80 nm gold nanoparticles reveals plasmonic coupling between the particle and its image within the gold substrate. While for a single graphene layer, spectral doublets from coupled dimer modes are observed shifted into the near-infrared, these disappear for increasing numbers of layers. These doublets arise from charger-transfer-sensitive gap plasmons, allowing optical measurement to access out-of-plane conductivity in such layered systems. Gating the graphene can thus directly produce plasmon tuning.

Raman spectroscopy is the prime nondestructive characterization tool for graphene and related layered materials. The shear (C) and layer breathing modes (LBMs) are due to relative motions of the planes, either perpendicular or parallel to their normal. This allows one to directly probe the interlayer interactions in multilayer samples. Graphene and other two-dimensional (2d) crystals can be combined to form various hybrids and heterostructures, creating materials on demand with properties determined by the interlayer interaction. This is the case even for a single material, where multilayer stacks with different relative orientations have different optical and electronic properties. In twisted multilayer graphene there is a significant enhancement of the C modes due to resonance with new optically allowed electronic transitions, determined by the relative orientation of the layers. Here we show that this applies also to the LBMs, which can be now directly measured at room temperature. We find that twisting has a small effect on LBMs, quite different from the case of the C modes. This implies that the periodicity mismatch between two twisted layers mostly affects shear interactions. Our work shows that ultralow-frequency Raman spectroscopy is an ideal tool to uncover the interface coupling of 2d hybrids and heterostructures.

We present flexible photodetectors (PDs) for visible wavelengths fabricated by stacking centimeter-scale chemical vapor deposited (CVD) single layer graphene (SLG) and single layer CVD MoS2, both wet transferred onto a flexible polyethylene terephthalate substrate. The operation mechanism relies on injection of photoexcited electrons from MoS2 to the SLG channel. The external responsivity is 45.5A/W and the internal 570A/W at 642 nm. This is at least 2 orders of magnitude higher than bulk-semiconductor flexible membranes. The photoconductive gain is up to 4 × 105. The photocurrent is in the 0.1–100 μA range. The devices are semitransparent, with 8% absorptance at 642 nm, and are stable upon bending to a curvature of 1.4 cm. These capabilities and the low-voltage operation (<1 V) make them attractive for wearable applications.

Graphene's high mobility and Fermi velocity, combined with its constant light absorption in the visible to far-infrared range, make it an ideal material to fabricate high-speed and ultrabroadband photodetectors. However, the precise mechanism of photodetection is still debated. Here, we report wavelength and polarization-dependent measurements of metal−graphene−metal photodetectors. This allows us to quantify and control the relative contributions of both photothermo-and photoelectric effects, both adding to the overall photoresponse. This paves the way for a more efficient photodetector design for ultrafast operating speeds.KEYWORDS: Graphene, photodetectors, Raman spectroscopy, photoresponse, optoelectronics T he unique optical and electronic properties of graphene make it ideal for photonics and optoelectronics. 1 A variety of prototype devices have already been demonstrated, such as transparent electrodes in displays 2 and photovoltaic modules, 3 optical modulators, 4 plasmonic devices, 4−9 microcavities, 10,11 and ultrafast lasers. 12 Among these, a significant effort is being devoted to photodetectors (PDs). 6,10,11,13−25 Various photodetection schemes and architectures have been proposed to date. The simplest configuration is the metal− graphene−metal (MGM) PD, in which graphene is contacted with metal electrodes as the source and drain. 13−18 These PDs can be combined with metal nanostructures enabling local surface plasmons and increased absorption, realizing an enhancement in responsivity (i.e., the ratio of the lightgenerated electrical current to the incident light power). 6,26 Microcavity based PDs were also used, with increased light absorption at the cavity resonance frequency, again achieving an increase in responsivity. 10,11 Another scheme is the integration of graphene with a waveguide to increase the effective interaction length with light. 25,27 Hybrid approaches employ semiconducting nanodots as light-absorbing media. 22 In this case, light excites electron−hole (e−h) pairs in the nanodots; the electrons are trapped in the nanodot, while the holes are transferred to graphene, thus effectively gating it. 22 Under applied drain−source bias, this results in a shift in the Dirac point, thus a modulation of the drain−source current. 22 Due to the long trapping time of the electrons within the dot, the transferred holes can cycle many times through the phototransistor before relaxation and e−h recombination. This gives a photoconductive gain; i.e., one absorbed photon effectively results in an electrical current of several electrons. Responsivities >10 7 A/W were reported, 22 but with a millisecond time scale, not suitable for, e.g., high-speed optical communications. Devices were also fabricated for detection of THz light. 28,29 In this low energy range, Pauli blocking forbids the direct excitation of e−h pairs due to finite doping. Instead, an antenna coupled to source and gate of the device excites plasma waves within the channel. These are rectified, leading to a detectable dc out...