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Optical-microcavity-enhanced light-matter interaction offers a powerful tool to develop fast and precise sensing techniques, spurring applications in the detection of biochemical targets ranging from cells, nanoparticles, and large molecules. However, the intrinsic inertness of such pristine microresonators limits their spread in new fields such as gas detection. Here, a functionalized microlaser sensor is realized by depositing graphene in an erbium-doped over-modal microsphere. By using a 980 nm pump, multiple laser lines excited in different mode families of the microresonator are co-generated in a single device. The interference between these splitting mode lasers produce beat notes in the electrical domain (0.2-1.1 MHz) with sub-kHz accuracy, thanks to the graphene-induced intracavity backward scattering. This allows for lab-free multispecies gas identification from a mixture, and ultrasensitive gas detection down to individual molecule.

Mixed dimensional hybrid structures have recently gained increasing attention as promising building blocks for novel electronic and optoelectronic devices. In this context, hybridization of semiconductor nanowires with two-dimensional materials could offer new ways to control and modulate lasing at the nanoscale. In this work, we deterministically fabricate hybrid mixed-dimensional heterostructures composed of ZnO nanowires and MoS2 monolayers with micrometer control over their relative position. First, we show that our deterministic fabrication method does not degrade the optical properties of the ZnO nanowires. Second, we demonstrate that the lasing wavelength of ZnO nanowires can be tuned by several nanometers by hybridization with CVD-grown MoS2 monolayers. We assign this spectral shift of the lasing modes to an efficient carrier transfer at the heterointerface and the subsequent increase of the optical band gap in ZnO (Moss-Burstein effect).

Mixed-dimensional hybrid structures have recently gained increasing attention as promising building blocks for novel electronic and optoelectronic devices. In this context, hybridization of semiconductor nanowires with two-dimensional materials could offer new ways to control and modulate lasing at the nanoscale. In this work, we deterministically fabricate hybrid mixed-dimensional heterostructures composed of ZnO nanowires and MoS

Single-layer transition metal dichalcogenides are at the center of an ever increasing research effort both in terms of fundamental physics and applications. Exciton–phonon coupling plays a key role in determining the (opto)electronic properties of these materials. However, the exciton–phonon coupling strength has not been measured at room temperature. Here, we use two-dimensional micro-spectroscopy to determine exciton–phonon coupling of single-layer MoSe2. We detect beating signals as a function of waiting time induced by the coupling between A excitons and A′1 optical phonons. Analysis of beating maps combined with simulations provides the exciton–phonon coupling. We get a Huang–Rhys factor ~1, larger than in most other inorganic semiconductor nanostructures. Our technique offers a unique tool to measure exciton–phonon coupling also in other heterogeneous semiconducting systems, with a spatial resolution ~260 nm, and provides design-relevant parameters for the development of optoelectronic devices. The exciton–phonon coupling (EXPC) affects the opto-electronic properties of atomically thin semiconductors. Here, the authors develop two-dimensional micro-spectroscopy to determine the EXPC of monolayer MoSe2.

Surface plasmons in graphene provide a compelling strategy for advanced photonic technologies thanks to their tight confinement, fast response and tunability. Recent advances in the field of all-optical generation of graphene’s plasmons in planar waveguides offer a promising method for high-speed signal processing in nanoscale integrated optoelectronic devices. Here, we use two counter propagating frequency combs with temporally synchronized pulses to demonstrate deterministic all-optical generation and electrical control of multiple plasmon polaritons, excited via difference frequency generation (DFG). Electrical tuning of a hybrid graphene-fiber device offers a precise control over the DFG phase-matching, leading to tunable responses of the graphene’s plasmons at different frequencies and provides a powerful tool for high-speed logic operations. Our results offer new insights for plasmonics on hybrid photonic devices based on layered materials and pave the way to high-speed integrated optoelectronic computing circuits.

Graphene is ideally suited for optoelectronics. It offers absorption at telecom wavelengths, high-frequency operation and CMOS-compatibility. We show how high speed optoelectronic mixing can be achieved with high frequency (~20 GHz bandwidth) graphene field effect transistors (GFETs). These devices mix an electrical signal injected into the GFET gate and a modulated optical signal onto a single layer graphene (SLG) channel. The photodetection mechanism and the resulting photocurrent sign depend on the SLG Fermi level (E

Hard disk drives (HDDs) are used as secondary storage in digital electronic devices owing to low cost and large data storage capacity. Due to the exponentially increasing amount of data, there is a need to increase areal storage densities beyond ~1 Tb/in2. This requires the thickness of carbon overcoats (COCs) to be, The main limitation to the areal storage density of hard disk drives (HDDs) is the thickness of carbon overcoats protecting the disk media. Here

Hot charge carriers in graphene exhibit fascinating physical phenomena, whose understanding has improved greatly over the past decade. They have distinctly different physical properties compared to, for example, hot carriers in conventional metals. This is predominantly the result of graphene's linear energy–momentum dispersion, its phonon properties, its all-interface character, and the tunability of its carrier density down to very small values, and from electron- to hole-doping. Since a few years, we have witnessed an increasing interest in technological applications enabled by hot carriers in graphene. Of particular interest are optical and optoelectronic applications, where hot carriers are used to detect (photodetection), convert (nonlinear photonics), or emit (luminescence) light. Graphene-enabled systems in these application areas could find widespread use and have a disruptive impact, for example in the field of data communication, high-frequency electronics, and industrial quality control. The aim of this review is to provide an overview of the most relevant physics and working principles that are relevant for applications exploiting hot carriers in graphene., Hot charge carriers in graphene exhibit fascinating physical phenomena and have great promise for exciting optoelectronic applications. The current understanding of the relevant fundamental physics and the most promising applications are reviewed.

Monolayer transition metal dichalcogenides with direct bandgaps are emerging candidates for microelectronics, nano-photonics, and optoelectronics. Transferred onto photonic integrated circuits (PICs), these semiconductor materials have enabled new classes of light-emitting diodes, modulators and photodetectors, that could be amenable to wafer-scale manufacturing. For integrated photonic devices, the optical losses of the PICs are critical. In contrast to silicon, silicon nitride (Si3N4) has emerged as a low-loss integrated platform with a wide transparency window from ultraviolet to mid-infrared and absence of two-photon absorption at telecommunication bands. Moreover, it is suitable for nonlinear integrated photonics due to its high Kerr nonlinearity and high-power handing capability. These features of Si3N4 are intrinsically beneficial for nanophotonics and optoelectronics applications. Here we report a low-loss integrated platform incorporating monolayer molybdenum ditelluride (1L-MoTe2) with Si3N4 photonic microresonators. We show that, with the 1L-MoTe2, microresonator quality factors exceeding 3 million in the telecommunication O-band to E-band are maintained. We further investigate the change of microresonator dispersion and resonance shift due to the presence of 1L-MoTe2, and extrapolate the optical loss introduced by 1L-MoTe2 in the telecommunication bands, out of the excitonic transition region. Our work presents a key step for low-loss, hybrid PICs with layered semiconductors without using heterogeneous wafer bonding.

Detection of individual molecules is the ultimate goal of any chemical sensor. In the case of gas detection, such resolution has been achieved in advanced nanoscale electronic solid-state sensors, but it has not been possible so far in integrated photonic devices, where the weak light-molecule interaction is typically hidden by noise. Here, we demonstrate a scheme to generate ultrasensitive down-conversion four-wave-mixing (FWM) in a graphene bipolar-junction-transistor heterogeneous D-shaped fiber. In the communication band, the FWM conversion efficiency can change steeply when the graphene Fermi level approaches 0.4 eV. In this condition, we exploit our unique two-step optoelectronic heterodyne detection scheme, and we achieve real-time individual gas molecule detection in vacuum. Such combination of graphene strong nonlinearities, electrical tunability, and all-fiber integration paves the way toward the design of versatile high-performance graphene photonic devices.

Funder: ERC Grants Hetero2D, Funder: GSYNCOR, Funder: EU Graphene Flagship, Black phosphorous (BP) is a layered semiconductor with high carrier mobility, anisotropic optical response and wide bandgap tunability. In view of its application in optoelectronic devices, understanding transient photo-induced effects is crucial. Here, we investigate by time- and angle-resolved photoemission spectroscopy BP in its pristine state and in the presence of Stark splitting, chemically induced by Cs ad-sorption. We show that photo-injected carriers trigger bandgap renormalization, and a concurrent valence band flattening caused by Pauli blocking. In biased samples, photo-excitation leads to a long-lived (ns) surface photovoltage of few hundreds mV that counterbalances the Cs-induced surface band bending. This allows us to disentangle bulk from surface electronic states, and to clarify the mechanism underlying the band inversion observed in bulk samples.

Dual comb spectroscopy enables fast and accurate measurements over broad spectral ranges, offering a powerful tool to identify chemical species with unprecedented spectral resolution. Co-generation of soliton combs in one single microresonator can be used to improve the compactness of multi-comb sources and bridge the lab-to-fab gap. However, the robustness of pristine microresonators to environmental changes limits their potential in broader applications such as biochemical sensing. Here, we realize for the first time a two-dimensional-material functionalized dual-comb spectrometer by asymmetrically depositing graphene in an over-modal microsphere. Spectrally trapped Stokes solitons belonging to distinct transverse mode families are co-generated in one single device. A soliton mode in the graphene-functionalized region is highly sensitive to environmental changes while a second soliton mode in the pristine region serves as reference, thus producing dual-comb ultrasensitive beat notes in the electrical domain. Taking advantage of an advanced optoelectronic heterodyne detection scheme, we trace the frequency shift of the dual-soliton beat-note with uncertainty < 0.2 Hz and we achieve real-time individual gas molecule detection in vacuum. This combination of atomically thin materials and microcombs shows the potential for integrated spectroscopy with unprecedented performances and offers new insights toward the design of versatile functionalized microcavity photonic devices.

Fibrillar amyloids exhibit a fascinating range of mechanical, optical, and electronic properties originating from their characteristic β-sheet-rich structure. Harnessing these functionalities in practical applications has so far been hampered by a limited ability to control the amyloid self-assembly process at the macroscopic scale. Here, we use core-shell electrospinning with microconfinement to assemble amyloid-hybrid fibers, consisting of densely aggregated fibrillar amyloids stabilized by a polymer shell. Up to centimeter-long hybrid fibers with micrometer diameter can be arranged into aligned and ordered arrays and deposited onto substrates or produced as free-standing networks. Properties that are characteristic of amyloids, including their high elastic moduli and intrinsic fluorescence signature, are retained in the hybrid fiber cores, and we show that they fully persist through the macroscopic fiber patterns. Our findings suggest that microlevel confinement is key for the guided assembly of amyloids from monomeric proteins.

We demonstrate the steep EO tunability of four-wave-mixing (FWM) in a graphene bipolar-junction-transistor heterogeneous D-shaped fiber (GhDF). This enables the GhDF ultrasensitive to external molecule adsorption/desorption in vacuum, achieving individual gas molecule detections.

Electron transport across the transition-metal dichalcogenide (TMD)/metal interface plays an important role in determining the performance of TMD-based optoelectronic devices. However, the robustness of this process against structural heterogeneities remains unexplored, to the best of our knowledge. Here, we employ a combination of time-resolved photoemission electron microscopy (TR-PEEM) and atomic force microscopy to investigate the spatially resolved hot-electron-transfer dynamics at the monolayer (1L) MoS

We present a transient absorption setup combining broadband detection over the visible-UV range with high temporal resolution (∼20 fs) which is ideally suited to trigger and detect vibrational coherences in different classes of materials. We generate and detect coherent phonons (CPs) in single-layer (1L)-MoS

International audience; Layered hybrid metal-halide perovskites with non-centrosymmetric crystal structure are predicted to show spin-selective band splitting from Rashba effects. Thus, fabrication of metal-halide perovskites with defined crystal symmetry is desired to control the spin-splitting in their electronic states. Here, we report the influence of halogen para-substituents on the crystal structure of benzylammonium lead iodide perovskites (4-XC6H4CH2NH3)2PbI4 (X = H, F, Cl, Br). Using X-ray diffraction and second-harmonic generation, we study structure and symmetry of single crystal and thin film samples. We report that introduction of a halogen atom lowers the crystal symmetry such that the chlorine- and bromine-substituted structures are non-centrosymmetric. The differences can be attributed to the nature of the intermolecular interactions between the organic molecules. We calculate electronic band structures and find good control of Rashba splittings. Our results present a facile approach to tailor hybrid layered metal halide perovskites with potential for spintronic and non-linear optical applications.

Excitonic interactions determine the photoelectric properties of two-dimensional semiconductors. By using spatially resolved coherent two-dimensional micro-spectroscopy, we are able to determine the strength of exciton–phonon coupling in single-layer MoSe2 at room temperature.

Broadband transient absorption with sub-20fs temporal resolution, supported by ab-initio calculations, quantitatively provides the strength of exciton-coherent phonon coupling in 1L-MoS2, showing a resonant profile around the C exciton.

We investigate the photocatalytic performance of composites prepared in a one-step process by liquid-phase exfoliation of graphite in the presence of TiO

Graphene is an ideal material for integrated nonlinear optics thanks to its strong light-matter interaction and large nonlinear optical susceptibility. Graphene has been used in optical modulators, saturable absorbers, nonlinear frequency converters, and broadband light emitters. For the latter application, a key requirement is the ability to control and engineer the emission wavelength and bandwidth, as well as the electronic temperature of graphene. Here, we demonstrate that the emission wavelength of graphene$'$ s broadband hot carrier photoluminescence can be tuned by integration on photonic cavities, while thermal management can be achieved by out-of-plane heat transfer to hexagonal boron nitride. Our results pave the way to graphene-based ultrafast broadband light emitters with tunable emission.

Atomically thin Transition-metal dichalcogenides (TMDs) have come into the spotlight in optoelectronics thanks to their outstanding physical properties [1,2]. In single-layer (1L) TMDs strong quantum confinement effects cause a weak screening of Coulomb, so that the excitons created by photo-excitation have large binding energy, up to several hundred meVs [3]. While the steady-state properties of TMDCs have been studied in detail by linear optical techniques, the recent application of time-resolved nonlinear spectroscopy (mainly ultrafast pump-probe) has enabled the study of excited-state dynamics on femtosecond timescales [4] opening up questions about the mechanisms of exciton relaxations and exciton-exciton interactions.

The ultrafast relaxation dynamics in single-layer graphene (SLG) is of key importance for its applications in optoelectronic devices which rely on the dynamic response of charge carriers, such as photodetectors, saturable absorbers and modulators[1]. The absorption via interband transitions of a photon of energy in ħω SLG promotes an electron from an energy −ħω/2 in the valence band to an energy ħω/2 in the conduction band. This strongly non-equilibrium distribution thermalizes by electron-electron scattering (t∼ 10–20 fs) to a hot Fermi-Dirac (FD) distribution, which in turn equilibrates with the cold lattice via interaction with strongly-coupled optical phonons (SCOP, t∼200–300 fs) and, on a longer time scale, via anharmonic coupling with acoustic phonons (t∼ 1–2 ps) [2].

Hot-electrons dominate the ultrafast (∼fs-ps) optical and electronic properties of metals and semiconductors [1–2] and they are exploited in a variety of applications including photovoltaics and photodetection. Here we perform power-dependent third harmonic generation (THG) measurements on gated single layer graphene (SLG) and we show that hot-electrons modulate significantly the power-law dependence of THG, inducing a large deviation from the expected cubic power-law. We use a Chemical Vapor Deposition (CVD) SLG sample transferred on Fused Silica (FS) and gated by ionic liquid (IL), Fig.1(a). We excite the sample with the idler beam of an Optical Parametric Oscillator (OPO, Coherent) at a photon energy of ħω0=0.69eV. The OPO is seeded by a mode-locked Ti:Sa laser (Coherent) with 150fs pulse duration and 80MHz repetition rate. The OPO idler spot-size is∼4.7μm and the pulse duration ∼300fs.

We present a transient absorption setup combining broadband detection over the visible-UV range with high temporal resolution ($\sim$20fs) which is ideally suited to trigger and detect vibrational coherences in different classes of materials. We generate and detect coherent phonons (CPs) in single layer (1L) MoS$_2$, as a representative semiconducting 1L-transition metal dichalcogenide (TMD), where the confined dynamical interaction between excitons and phonons is unexplored. The coherent oscillatory motion of the out-of-plane $A'_{1}$ phonons, triggered by the ultrashort laser pulses, dynamically modulates the excitonic resonances on a timescale of few tens fs. We observe an enhancement by almost two orders of magnitude of the CP amplitude when detected in resonance with the C exciton peak, combined with a resonant enhancement of CP generation efficiency. Ab initio calculations of the change in 1L-MoS$_2$ band structure induced by the $A'_{1}$ phonon displacement confirm a strong coupling with the C exciton. The resonant behavior of the CP amplitude follows the same spectral profile of the calculated Raman susceptibility tensor. This demonstrates that CP excitation in 1L-MoS$_2$ can be described as a Raman-like scattering process. These results explain the CP generation process in 1L-TMDs, paving the way for coherent all-optical control of excitons in layered materials in the THz frequency range.

We use helicity-resolved transient absorption spectroscopy to track intravalley scattering dynamics in monolayer WS2. We find that spin-polarized carriers scatter from upper to lower conduction band by reversing their spin orientation on a sub-ps timescale.

Item does not contain fulltext We investigate the photocatalytic performance of composites prepared in a one-step process by liquid-phase exfoliation of graphite in the presence of TiO2 nanoparticles (NPs) at atmospheric pressure and in water, without heating or adding any surfactant, and starting from low-cost commercial reagents. These show enhanced photocatalytic activity, degrading up to 40% more pollutants with respect to the starting TiO2-NPs, in the case of a model dye target, and up to 70% more pollutants in the case of nitrogen oxides. In order to understand the photo-physical mechanisms underlying this enhancement, we investigate the photo-generation of reactive species (trapped holes and electrons) by ultrafast transient absorption spectroscopy. We observe an electron transfer process from TiO2 to the graphite flakes within the first picoseconds of the relaxation dynamics, which causes the decrease of the charge recombination rate, and increases the efficiency of the reactive species photo-production.

Janus crystals represent an exciting class of 2D materials with different atomic species on their upper and lower facets. Theories have predicted that this symmetry breaking induces an electric field and leads to a wealth of novel properties, such as large Rashba spin-orbit coupling and formation of strongly correlated electronic states. Monolayer MoSSe Janus crystals have been synthesized by two methods, via controlled sulfurization of monolayer MoSe2 and via plasma stripping followed thermal annealing of MoS2 . However, the high processing temperatures prevent growth of other Janus materials and their heterostructures. Here, a room-temperature technique for the synthesis of a variety of Janus monolayers with high structural and optical quality is reported. This process involves low-energy reactive radical precursors, which enables selective removal and replacement of the uppermost chalcogen layer, thus transforming classical transition metal dichalcogenides into a Janus structure. The resulting materials show clear mixed character for their excitonic transitions, and more importantly, the presented room-temperature method enables the demonstration of first vertical and lateral heterojunctions of 2D Janus TMDs. The results present significant and pioneering advances in the synthesis of new classes of 2D materials, and pave the way for the creation of heterostructures from 2D Janus layers.

In monolayer (1L) transition metal dichalcogenides (TMDs) the valence and conduction bands are spin-split because of the strong spin-orbit interaction. In tungsten-based TMDs the spin-ordering of the conduction band is such that the so-called dark excitons, consisting of electrons and holes with opposite spin orientation, have lower energy than A excitons. The transition from bright to dark excitons involves the scattering of electrons from the upper to the lower conduction band at the K point of the Brillouin zone, with detrimental effects for the optoelectronic response of 1L-TMDs, since this reduces their light emission efficiency. Here, we exploit the valley selective optical selection rules and use two-color helicity-resolved pump-probe spectroscopy to directly measure the intravalley spin-flip relaxation dynamics in 1L-WS

Nitrophorins (NP) 1–7 are NO-carrying heme proteins found in the saliva of the blood-sucking insect Rhodnius prolixus. The isoform NP7 displays peculiar properties, such as an abnormally high isoelectric point, the ability to bind negatively charged membranes, and a strong pH sensitivity of NO affinity. A unique trait of NP7 is the presence of Glu in position 27, which is occupied by Val in other NPs. Glu27 appears to be important for tuning the heme properties, but its influence on the pH-dependent NO release mechanism, which is assisted by a conformational change in the AB loop, remains unexplored. Here, in order to gain insight into the functional role of Glu27, we examine the effect of Glu27 → Val and Glu27 → Gln mutations on the ligand binding kinetics using CO as a model. The results reveal that annihilation of the negative charge of Glu27 upon mutation reduces the pH sensitivity of the ligand binding rate, a process that in turn depends on the ionization of Asp32. We propose that Glu27 exerts a through-space electrostatic action on Asp32, which shifts the pKa of the latter amino acid towards more acidic values thus reducing the pH sensitivity of the transition between open and closed states.

© 2016 American Chemical Society. We studied by broad-band pump-probe spectroscopy the ultrafast optical response of thin copper films covered by a monolayer of graphene. It is demonstrated that graphene protection does not alter the thermo-modulational nonlinearity of copper in the whole visible range. Also, we provide a quantitative validation of a theoretical model for this optical nonlinearity, derived from a semiclassical description of electron thermalization dynamics and subsequent modulation of copper dielectric function from 450 to 700 nm wavelength. Our results extend to the nonlinear domain the capability of graphene-protected copper nanolayers to serve as a low cost optical grade material, with major potential impact on nonlinear plasmonics and metamaterials.