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Andrea C. Ferrari

Publications and source records attributed to Andrea C. Ferrari.

54 records · Page 3Linked to original sources

Excitonic emission of monolayer semiconductors near-field coupled to high-Q microresonators

We present quantum yield measurements of single layer $\textrm{WSe}_2$ (1L-$\textrm{WSe}_2$) integrated with high-Q ($Q>10^6$) optical microdisk cavities, using an efficient ($η>$90%) near-field coupling scheme based on a tapered optical fiber. Coupling of the excitonic emission is achieved by placing 1L-WSe$_2$ to the evanescent cavity field. This preserves the microresonator high intrinsic quality factor ($Q>10^6$) below the bandgap of 1L-WSe$_2$. The nonlinear excitation power dependence of the cavity quantum yield is in agreement with an exciton-exciton annihilation model. The cavity quantum yield is $\textrm{QY}_\textrm{c}\sim10^{-3}$, consistent with operation in the \textit{broad emitter} regime (i.e. the emission lifetime of 1L-WSe$_2$ is significantly shorter than the bare cavity decay time). This scheme can serve as a precise measurement tool for the excitonic emission of layered materials into cavity modes, for both in plane and out of plane excitation.

cond-mat.mes-hall↗

Photo-Induced Bandgap Renormalization Governs the Ultrafast Response of Single-Layer MoS2

Transition metal dichalcogenides (TMDs) are emerging as promising two-dimensional (2d) semiconductors for optoelectronic and flexible devices. However, a microscopic explanation of their photophysics -- of pivotal importance for the understanding and optimization of device operation -- is still lacking. Here we use femtosecond transient absorption spectroscopy, with pump pulse tunability and broadband probing, to monitor the relaxation dynamics of single-layer MoS2 over the entire visible range, upon photoexcitation of different excitonic transitions. We find that, irrespective of excitation photon energy, the transient absorption spectrum shows the simultaneous bleaching of all excitonic transitions and corresponding red-shifted photoinduced absorption bands. First-principle modeling of the ultrafast optical response reveals that a transient bandgap renormalization, caused by the presence of photo-excited carriers, is primarily responsible for the observed features. Our results demonstrate the strong impact of many-body effects in the transient optical response of TMDs even in the low-excitation-density regime.

cond-mat.mtrl-sci↗

p-wave triggered superconductivity in single layer graphene on an electron-doped oxide superconductor

Electron pairing in the vast majority of superconductors follows the Bardeen-Cooper-Schrieffer theory of superconductivity, which describes the condensation of electrons into pairs with antiparallel spins in a singlet state with an s-wave symmetry. Unconventional superconductivity is predicted in single layer graphene where the electrons pair with a p-wave or chiral d-wave symmetry, depending on the position of the Fermi energy with respect to the Dirac point. By placing single layer graphene on an electron-doped (non-chiral) d-wave superconductor and performing local scanning tunnelling microscopy and spectroscopy, here we show evidence for a p-wave triggered superconducting density of states in single layer graphene. The realization of unconventional superconductivity in single layer graphene offers an exciting new route for the development of p-wave superconductivity using two-dimensional materials with transition temperatures above 4.2 K.

cond-mat.supr-con↗

Large-scale quantum-emitter arrays in atomically thin semiconductors

The flourishing field of two-dimensional (2D) nanophotonics has generated much excitement in the quantum technologies community after the identification of quantum emitters (QEs) in layered materials (LMs). LMs offer many advantages as platforms for quantum circuits, such as integration within hybrid technologies, valley degree of freedom and strong spin-orbit coupling. QEs in LMs, however, suffer from uncontrolled occurrences, added to the uncertainty over their origin, which has been linked to defects and strain gradients. Here, we report a scalable method to create arrays of single-photon emitting QEs in tungsten diselenide (WSe2) and tungsten disulphide (WS2) using a nanopatterned silica substrate. We obtain devices with QE numbers in the range of hundreds, limited only by the flake size, and a QE yield approaching unity. The overall quality of these deterministic QEs surpasses that of their randomly appearing counterparts, with spectral wanderings of around 0.1 meV, an order of magnitude lower than previous reports. Our technique solves the scalability challenge for LM-based quantum photonic devices.

cond-mat.mes-hall↗

Atomically thin quantum light emitting diodes

Transition metal dichalcogenides (TMDs) are optically active layered materials providing potential for fast optoelectronics and on-chip photonics. We demonstrate electrically driven single-photon emission from localised sites in tungsten diselenide (WSe2) and tungsten disulphide (WS2). To achieve this, we fabricate a light emitting diode structure comprising single layer graphene, thin hexagonal boron nitride and TMD mono- and bi-layers. Photon correlation measurements are used to confirm the single-photon nature of the spectrally sharp emission. These results present the TMD family as a platform for hybrid, broadband, atomically precise quantum photonics devices.

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Raman fingerprints of atomically precise graphene nanoribbons

Bottom-up approaches allow the production of ultra-narrow and atomically precise graphene nanoribbons (GNRs), with electronic and optical properties controlled by the specific atomic structure. Combining Raman spectroscopy and ab-initio simulations, we show that GNR width, edge geometry and functional groups all influence their Raman spectra. The low-energy spectral region below 1000 cm-1 is particularly sensitive to edge morphology and functionalization, while the D peak dispersion can be used to uniquely fingerprint the presence of GNRs, and differentiates them from other sp2 carbon nanostructures.

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Interface coupling in twisted multilayer graphene by resonant Raman spectroscopy of layer breathing modes

Raman spectroscopy is the prime non-destructive 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 orientation have different optical and electronic properties. In twisted multilayer graphene samples 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, that can be now directly measured at room temperature. We find that twisting does not affect 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 Raman spectroscopy is an ideal tool to uncover the interface coupling of 2d hybrids and heterostructures.

cond-mat.mtrl-sci↗

On-chip integrated, silicon-graphene plasmonic Schottky photodetector, with high responsivity and avalanche photogain

We report an on-chip integrated metal-graphene-silicon plasmonic Schottky photodetector with 85mA/W responsivity at 1.55 um 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 3V, we achieve avalanche multiplication, with 0.37A/W responsivity and avalanche photogain~2. This paves the way to graphene integrated silicon photonics.

cond-mat.mes-hall↗

The Interlayer Shear Modes in Twisted Multi-layer Graphenes: Interlayer coupling, Davydov Splitting and Intensity Resonance

Graphene and other two-dimensional crystals can be combined to form various hybrids and heterostructures, creating materials on demand, in which the interlayer coupling at the interface leads to modified physical properties as compared to their constituents. Here, by measuring Raman spectra of shear modes, we probe the coupling at the interface between two artificially-stacked few-layer graphenes rotated with respect to each other. The strength of interlayer coupling between the two interface layers is found to be only 20% of that between Bernal-stacked layers. Nevertheless, this weak coupling manifests itself in a Davydov splitting of the shear mode frequencies in systems consisting of two equivalent graphene multilayers, and in the intensity enhancement of shear modes due to the optical resonance with several optically allowed electronic transitions between conduction and valence bands in the band structures. This study paves way for fundamental understanding into the interface coupling of two-dimensional hybrids and heterostructures.

cond-mat.mtrl-sci↗

High performance bilayer-graphene Terahertz detectors

We report bilayer-graphene field effect transistors operating as THz broadband photodetectors based on plasma-waves excitation. By employing wide-gate geometries or buried gate configurations, we achieve a responsivity $\sim 1.2V/W (1.3 mA/W)$ and a noise equivalent power $\sim 2\times 10^{-9} W/Hz^{-1/2}$ in the 0.29-0.38 THz range, in photovoltage and photocurrent mode. The potential of this technology for scalability to higher frequencies and the development of flexible devices makes our approach competitive for a future generation of THz detection systems.

cond-mat.mes-hall↗

Raman spectroscopy as a versatile tool for studying the properties of graphene

Raman spectroscopy is an integral part of graphene research. It is used to determine the number and orientation of layers, the quality and types of edge, and the effects of perturbations, such as electric and magnetic fields, strain, doping, disorder and functional groups. This, in turn, provides insight into all $sp^2$-bonded carbon allotropes, because graphene is their fundamental building block. Here we review the state of the art, future directions and open questions in Raman spectroscopy of graphene. We describe essential physical processes whose importance has only recently been recognized, such as the various types of resonance at play, and the role of quantum interference. We update all basic concepts and notations, and propose a terminology that is able to describe any result in literature. We finally highlight the potential of Raman spectroscopy for layered materials other than graphene.

cond-mat.mtrl-sci↗

Non-equilibrium dynamics of photo-excited electrons in graphene: collinear scattering, Auger processes, and the impact of screening

We present a combined analytical and numerical study of the early stages (sub-100fs) of the non-equilibrium dynamics of photo-excited electrons in graphene. We employ the semiclassical Boltzmann equation with a collision integral that includes contributions from electron-electron (e-e) and electron-optical phonon interactions. Taking advantage of circular symmetry and employing the massless Dirac Fermion (MDF) Hamiltonian, we are able to perform an essentially analytical study of the e-e contribution to the collision integral. This allows us to take particular care of subtle collinear scattering processes - processes in which incoming and outgoing momenta of the scattering particles lie on the same line - including carrier multiplication (CM) and Auger recombination (AR). These processes have a vanishing phase space for two dimensional MDF bare bands. However, we argue that electron-lifetime effects, seen in experiments based on angle-resolved photoemission spectroscopy, provide a natural pathway to regularize this pathology, yielding a finite contribution due to CM and AR to the Coulomb collision integral. Finally, we discuss in detail the role of physics beyond the Fermi golden rule by including screening in the matrix element of the Coulomb interaction at the level of the Random Phase Approximation (RPA), focusing in particular on the consequences of various approximations including static RPA screening, which maximizes the impact of CM and AR processes, and dynamical RPA screening, which completely suppresses them.

cond-mat.mes-hall↗

Controlling Sub-nm Gaps in Plasmonic Dimers using Graphene

Graphene is used as the thinnest possible spacer between gold nanoparticles and a gold substrate. This creates a robust, repeatable, and stable sub-nanometre 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 infra-red, these disappear for increasing numbers of layers. These doublets arise from plasmonic charge transfer, allowing the direct optical measurement of out-of-plane conductivity in such layered systems. Gating the graphene can thus directly produce plasmon tuning.

cond-mat.mes-hall↗

Light-matter interaction in a microcavity-controlled graphene transistor

Graphene has extraordinary electronic and optical properties and holds great promise for applications in photonics and optoelectronics. Demonstrations including high-speed photodetectors, optical modulators, plasmonic devices, and ultrafast lasers have now been reported. More advanced device concepts would involve photonic elements such as cavities to control light-matter interaction in graphene. Here we report the first monolithic integration of a graphene transistor and a planar, optical microcavity. We find that the microcavity-induced optical confinement controls the efficiency and spectral selection of photocurrent generation in the integrated graphene device. A twenty-fold enhancement of photocurrent is demonstrated. The optical cavity also determines the spectral properties of the electrically excited thermal radiation of graphene. Most interestingly, we find that the cavity confinement modifies the electrical transport characteristics of the integrated graphene transistor. Our experimental approach opens up a route towards cavity-quantum electrodynamics on the nanometre scale with graphene as a current-carrying intra-cavity medium of atomic thickness.

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From Graphene to Carbon Fibres: Mechanical Deformation and Development of a Universal Stress Sensor

Carbon fibres (CF) represent a significant volume fraction of modern structural airframes. Embedded into polymer matrices, they provide significant strength and stiffness gains over unit weight as compared to other competing structural materials. Nevertheless, no conclusive structural model yet exists to account for their extraordinary properties. In particular, polyacrynonitrile (PAN) derived CF are known to be fully turbostratic: the graphene layers are slipped sideways relative to each other, which leads to an inter-graphene distance much greater than graphite. Here, we demonstrate that CF derive their mechanical properties from those of graphene itself. By monitoring the Raman G peak shift with strain for both CF and graphene, we develop a universal master plot relating the G peak strain sensitivity of all types of CF to graphene over a wide range of tensile moduli. A universal value of - average- shift rate with axial stress of ~ -5ω0^-1 (cm^-1 MPa^-1)is calculated for both graphene and all CF exhibiting annular ("onion-skin") morphology.

cond-mat.mtrl-sci↗

Subjecting a graphene monolayer to tension and compression

The mechanical behaviour of graphene flakes under both tension and compression is examined using a cantilever-beam arrangement. Two different sets of samples were employed involving flakes just supported on a plastic bar but also embedded within the plastic substrate. By monitoring the shift of the 2D Raman line with strain, information on the stress transfer efficiency as a function of stress sign and monolayer support were obtained. In tension, the embedded flake seems to sustain strains up to 1.3%, whereas in compression there is an indication of flake buckling at about 0.7% strain. The retainment of such a high critical buckling strain confirms the relative high flexural rigidity of the embedded monolayer.

cond-mat.mes-hall↗

Dielectrophoretic Assembly of High-Density Arrays of Individual Graphene Devices for Rapid Screening

We establish the use of dielectrophoresis for the directed parallel assembly of individual flakes and nanoribbons of few-layer graphene into electronic devices. This is a bottom-up approach where source and drain electrodes are prefabricated and the flakes are deposited from a solution using an alternating electric field applied between the electrodes. These devices are characterized by scanning electron microscopy, atomic force microscopy, Raman spectroscopy and electron transport measurements. They are shown to be electrically active and their current carrying capacity and subsequent failure mechanism is revealed. Akin to carbon nanotubes, we show that the dielectrophoretic deposition is self-limiting to one flake per device and is scalable to ultra-large-scale integration densities, thereby enabling the rapid screening of a large number of devices.

cond-mat.mes-hall↗

Born-Oppenheimer Breakdown in Graphene

The Born-Oppenheimer approximation (BO) has proven effective for the accurate determination of chemical reactions, molecular dynamics and phonon frequencies in a wide range of metallic systems. Graphene, recently discovered in the free state, is a zero band-gap semiconductor, which becomes a metal if the Fermi energy is tuned applying a gate-voltage Vg. Graphene electrons near the Fermi energy have twodimensional massless dispersions, described by Dirac cones. Here we show that a change in Vg induces a stiffening of the Raman G peak (i.e. the zone-center E2g optical phonon), which cannot be described within BO. Indeed, the E2g vibrations cause rigid oscillations of the Dirac-cones in the reciprocal space. If the electrons followed adiabatically the Dirac-cone oscillations, no change in the phonon frequency would be observed. Instead, since the electron-momentum relaxation near the Fermi level is much slower than the phonon motion, the electrons do not follow the Dirac-cone displacements. This invalidates BO and results in the observed phonon stiffening. This spectacular failure of BO is quite significant since BO has been the fundamental paradigm to determine crystal vibrations from the early days of quantum mechanics.

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