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The scalable synthesis and transfer of large-area graphene underpins the development of nanoscale photonic devices ideal for new applications in a variety of fields, ranging from biotechnology, to wearable sensors for healthcare and motion detection, to quantum transport, communications, and metrology. We report room-temperature zero-bias thermoelectric photodetectors, based on single- and polycrystal graphene grown by chemical vapor deposition (CVD), tunable over the whole terahertz range (0.1-10 THz) by selecting the resonance of an on-chip patterned nanoantenna. Efficient light detection with noise equivalent powers

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 to directly generate a photovoltage by the photothermoelectric effect. It is made of chemical vapor deposited single layer graphene, and has an external responsivity ∼12.2 V/W with a 3 dB bandwidth ∼42 GHz. We utilize Au split-gates to electrostatically create a p-n-junction and simultaneously guide a surface plasmon polariton gap-mode. This increases the 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.

Resistive-switching memories are alternative to Si-based ones, which face scaling and high power consumption issues. Tetrahedral amorphous carbon (ta-C) shows reversible, non-volatile resistive switching. Here we report polarity independent ta-C resistive memory devices with graphene-based electrodes. Our devices show ON/OFF resistance ratios$\sim$4x$10^5$, ten times higher than with metal electrodes, with no increase in switching power, and low power density$\sim$14$\mu$W/$\mu$m$^2$. We attribute this to a suppressed tunneling current due to the low density of states of graphene near the Dirac point, consistent with the current-voltage characteristics derived from a quantum point contact model. Our devices also have multiple resistive states. This allows storing more than one bit per cell. This can be exploited in a range of signal processing/computing-type operations, such as implementing logic, providing synaptic and neuron-like mimics, and performing analogue signal processing in non-von-Neumann architectures

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.

Ultrafast and sensitive (noise equivalent power, This is the unedited authors' version of the article accepted for publication in Nanophotonics 2020 (Online ISSN: 2192-8614)

It is challenging for conventional top-down lithography to fabricate reproducible devices very close to atomic dimensions, whereas identical molecules and very similar nanoparticles can be made bottom-up in large quantities, and can be self-assembled on surfaces. The challenge is to fabricate electrical contacts to many such small objects at the same time, so that nanocrystals and molecules can be incorporated into conventional integrated circuits. Here, we report a scalable method for contacting a self-assembled monolayer of nanoparticles with a single layer of graphene. This produces single-electron effects, in the form of a Coulomb staircase, with a yield of 87 ± 13% in device areas ranging from, The integration of nano-molecules into microelectronic circuitry is challenging. Here, the authors provide a scalable method for contacting a self-assembled monolayer of nanoparticles with a single layer of graphene that produces single-electron effects, in the form of a Coulomb staircase, with a yield of at least 70%.

Graphene integrated photonics provides several advantages over conventional Si photonics. Single layer graphene (SLG) enables fast, broadband, and energy-efficient electro-optic modulators, optical switches and photodetectors (GPDs), and is compatible with any optical waveguide. The last major barrier to SLG-based optical receivers lies in the low responsivity - electrical output per optical input - of GPDs compared to conventional PDs. Here we overcome this shortfall by integrating a photo-thermoelectric GPD with a Si microring resonator. Under critical coupling, we achieve $>$90% light absorption in a $\sim$6 $��$m SLG channel along the Si waveguide. Exploiting the cavity-enhanced light-matter interaction, causing carriers in SLG to reach $\sim$400 K for an input power of $\sim$0.6 mW, we get a voltage responsivity $\sim$90 V/W, demonstrating the feasibility of our approach. Our device is capable of detecting data rates up to 20 Gbit/s, with a receiver sensitivity enabling it to operate at a 10$^{-9}$ bit-error rate, on par with mature semiconductor technology. The natural generation of a voltage rather than a current, removes the need for transimpedance amplification, with a reduction of the energy-per-bit cost and foot-print, when compared to a traditional semiconductor-based receiver., 11 pages, 5 figures

Interlayer excitons in layered materials constitute a novel platform to study many-body phenomena arising from long-range interactions between quantum particles. Long-lived excitons are required to achieve high particle densities, to mediate thermalisation, and to allow for spatially and temporally correlated phases. Additionally, the ability to confine them in periodic arrays is key to building a solid-state analogue to atoms in optical lattices. Here, we demonstrate interlayer excitons with lifetime approaching 0.2 ms in a layered-material heterostructure made from WS2 and WSe2 monolayers. We show that interlayer excitons can be localised in an array using a nano-patterned substrate. These confined excitons exhibit microsecond-lifetime, enhanced emission rate, and optical selection rules inherited from the host material. The combination of a permanent dipole, deterministic spatial confinement and long lifetime places interlayer excitons in a regime that satisfies one of the requirements for simulating quantum Ising models in optically resolvable lattices. Excitons are quasiparticles consisting of an electron-hole pair and can be used to study many-body phenomenon. Here, the authors demonstrate on-demand quantum confinement of long-lived interlayer excitons in WS2/WSe2 heterostructures deposited on nanopatterned substrates.

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

The diffusion of lithium ions decoupled from a solid polymer electrolyte matrix is the key for high-energy electrochemical devices with the safety needed for commercial use. This Letter reports how the ion mobility in a single-phase hybrid polyelectrolyte (SPHP) matrix can be tuned by changing an inorganic coordinating atom from silicon (Si) to germanium (Ge). Nuclear Magnetic Resonance (NMR) results show that the lithium ion activation barrier in the polyelectrolyte with Si can be modulated from 0.26 eV to the unprecedented value of 0.12 eV in the polyelectrolyte with Ge. Density functional theory is used to show that the electronic structures of both polymers are very different, although their chemical structures are very similar, except for the coordinating atom. This simple chemical substitution route will certainly increase the interest in these polymers for applications in electrochemical devices.

Spontaneous Raman spectroscopy is a powerful characterization tool for graphene research. Its extension to the coherent regime, despite the large nonlinear third-order susceptibility of graphene, has so far proven challenging. Due to its gapless nature, several interfering electronic and phononic transitions concur to generate its optical response, preventing to retrieve spectral profiles analogous to those of spontaneous Raman. Here we report stimulated Raman spectroscopy of the G-phonon in single and multi-layer graphene, through coherent anti-Stokes Raman Scattering. The nonlinear signal is dominated by a vibrationally non-resonant background, obscuring the Raman lineshape. We demonstrate that the vibrationally resonant coherent anti-Stokes Raman Scattering peak can be measured by reducing the temporal overlap of the laser excitation pulses, suppressing the vibrationally non-resonant background. We model the spectra, taking into account the electronically resonant nature of both. We show how coherent anti-Stokes Raman Scattering can be used for graphene imaging with vibrational sensitivity., Coherent anti-Stokes Raman Scattering (CARS) accesses the vibrational properties of a material via nonlinear four-wave mixing (FWM); CARS in graphene has not been observed to date despite its high nonlinear third-order susceptibility. Here, the authors devised a FWM scheme to perform stimulated Raman spectroscopy in single and multi-layer graphene through CARS.

We report high room-temperature mobility in single layer graphene grown by Chemical Vapor Deposition (CVD) after wet transfer on SiO$_2$ and hexagonal boron nitride (hBN) encapsulation. By removing contaminations trapped at the interfaces between single-crystal graphene and hBN, we achieve mobilities up to$\sim70000cm^2 V^{-1} s^{-1}$ at room temperature and$\sim120000cm^2 V^{-1} s^{-1}$ at 9K. These are over twice those of previous wet transferred graphene and comparable to samples prepared by dry transfer. We also investigate the combined approach of thermal annealing and encapsulation in polycrystalline graphene, achieving room temperature mobilities$\sim30000 cm^2 V^{-1} s^{-1}$. These results show that, with appropriate encapsulation and cleaning, room temperature mobilities well above $10000cm^2 V^{-1} s^{-1}$ can be obtained in samples grown by CVD and transferred using a conventional, easily scalable PMMA-based wet approach.

This work describes a multilayer tungsten oxide photoanode synthesized via facile dip-coating deposition solution for sunlight-driven water oxidation reaction. The number of layers (three, five and ten) followed by a successive annealing process at each deposited layer has strongly influenced their performance. The ten-layers tungsten oxide photoanode exhibited the highest photocurrent density around 0.7 mA/cm2 at 1.23 VRHE, under sunlight irradiation. This photocurrent response corresponds to 17% of solar-to-hydrogen conversion efficiency (STH) from the maximum theoretical predicted for tungsten oxide (4.8%). The successive annealing treatment promoted a reduction in the number of grain boundaries, yielding in higher film porosity and surface roughness, which decreased the charge transfer resistance and the electron-hole recombination rate.

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

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.

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.

Multiple studies have reported the observation of electro-synaptic response in different metal/insulator/metal devices; however, most of them analysed large (>1 µm2) devices that do not meet the integration density required by the industry (1010 devices/mm2). Some studies employed a scanning tunnelling microscope (STM) to explore nano-synaptic response in different materials, but in this setup there is a nanogap between the insulator and one of the metallic electrodes (i.e. the STM tip), which is not present in real devices. Here we show how to use a conductive atomic force microscope (CAFM) to explore the presence and quality of nano-synaptic response in confined areas

We report room temperature terahertz detection in hBN/graphene/hBN heterostructures. The obtained record combination of high-speed (response time < 1 ns) and high sensitivity (noise equivalent power ~ 100 pWHz-1/2) is enabled by the photo-thermoelectric effect.

Solution-processed semiconducting transition metal dichalcogenides are at the centre of an ever-increasing research effort in printed (opto)electronics. However, device performance is limited by structural defects resulting from the exfoliation process and poor inter-flake electronic connectivity. Here, we report a new molecular strategy to boost the electrical performance of transition metal dichalcogenide-based devices via the use of dithiolated conjugated molecules, to simultaneously heal sulfur vacancies in solution-processed transition metal disulfides and covalently bridge adjacent flakes, thereby promoting percolation pathways for the charge transport. We achieve a reproducible increase by one order of magnitude in field-effect mobility (µFE), current ratio (ION/IOFF) and switching time (τS) for liquid-gated transistors, reaching 10−2 cm2 V−1 s−1, 104 and 18 ms, respectively. Our functionalization strategy is a universal route to simultaneously enhance the electronic connectivity in transition metal disulfide networks and tailor on demand their physicochemical properties according to the envisioned applications. A defect-engineering strategy exploiting dithiolated molecules enables the formation of covalently interconnected networks based on solution-processed transition metal disulfides, leading to devices with enhanced electrical performance and improved characteristics.

Batteries that extend performance beyond the intrinsic limits of Li-ion batteries are among the most important developments required to continue the revolution promised by electrochemical devices. Of these next-generation batteries, lithium sulfur (Li–S) chemistry is among the most commercially mature, with cells offering a substantial increase in gravimetric energy density, reduced costs and improved safety prospects. However, there remain outstanding issues to advance the commercial prospects of the technology and benefit from the economies of scale felt by Li-ion cells, including improving both the rate performance and longevity of cells. To address these challenges, the Faraday Institution, the UK’s independent institute for electrochemical energy storage science and technology, launched the Lithium Sulfur Technology Accelerator (LiSTAR) programme in October 2019. This Roadmap, authored by researchers and partners of the LiSTAR programme, is intended to highlight the outstanding issues that must be addressed and provide an insight into the pathways towards solving them adopted by the LiSTAR consortium. In compiling this Roadmap we hope to aid the development of the wider Li–S research community, providing a guide for academia, industry, government and funding agencies in this important and rapidly developing research space.

Graphene possesses a peculiar potential for the development of optoelectronic components capable to actively manipulate infrared light [1] . Its electrostatically tunable optical conductivity, band structure and transport characteristics, and the possibility to be grown over large areas, offer an intriguing playground for engineering, at the nanoscale, amplitude modulators, spatial light modulators and switches, combining high efficiency (> 50%) intensity modulation, reasonably high speeds (> s response times), and spectral tunability in the underexploited high (> 1.5 THz) terahertz-frequency range [2] , where frontier applications in quantum communications, quantum computing, adaptive and quantum optics are still at their infancy.

We present Z-Type Dye Sensitized Solar Modules (DSSMs) with screen printed graphene-based vertical interconnects. This prevents corrosion of interconnects in contact with electrolytic species, unlike conventional Ag interconnects. By enlarging the width of single cells, or by increasing the number of cells, we get an enhancement of the aperture power conversion efficiency ∼+12% with respect to Ag-based modules, with 1000 h stability under 85 °C stress test. This paves the way to original design layouts with decreased dead area and increased generated power per aperture area.

Transition metal dichalcogenides (TMDs) have rapidly emerged as one of the most attractive families of two-dimensional materials due to their numerous outstanding electronic and optoelectronic properties. TMDs have layer-dependent band structures, exhibiting a dramatic transition from a direct bandgap in the monolayer (1L) to an indirect bandgap in the multilayer (NL). TMD homojunctions form when a 1L TMD interfaces with an NL TMD of the same chemical composition. Such 1L/NL TMD homojunctions are predicted to have similar properties as heterojunctions, which comprises two different TMDs. In this work, we employ time-resolved photoemission electron microscopy (TR-PEEM) to study the ultrafast carrier dynamics of a WSe2 1L/NL Type-I homojunction with high temporal (50 fs) and spatial (70 nm) resolution. Published version

Energy relaxation of photo-excited charge carriers is of significant fundamental interest and crucial for the performance of monolayer transition metal dichalcogenides in optoelectronics. The primary stages of carrier relaxation affect a plethora of subsequent physical mechanisms. Here we measure light scattering and emission in tungsten diselenide monolayers close to the laser excitation energy (down to ~0.6 meV). We reveal a series of periodic maxima in the hot photoluminescence intensity, stemming from energy states higher than the A-exciton state. We find a period ~15 meV for 7 peaks below (Stokes) and 5 peaks above (anti-Stokes) the laser excitation energy, with a strong temperature dependence. These are assigned to phonon cascades, whereby carriers undergo phonon-induced transitions between real states above the free-carrier gap with a probability of radiative recombination at each step. We infer that intermediate states in the conduction band at the Λ-valley of the Brillouin zone participate in the cascade process of tungsten diselenide monolayers. This provides a fundamental understanding of the first stages of carrier–phonon interaction, useful for optoelectronic applications of layered semiconductors. The primary stages of carrier relaxation in atomically thin transition metal dichalcogenides are hardly accessible due to their fast timescales. Here, the authors measure the first stages of carrier–phonon interaction in monolayer WSe2 via a series of periodic maxima in the hot photoluminescence intensity, assigned to phonon cascades.

We report room temperature terahertz detection in hBN/graphene/hBN heterostructures, integrated in top-gated field effect transistors. The record combination of high-speed (response time < 1 ns) and high sensitivity (noise equivalent power ~ 100 pWHz-1I2) is enabled by the photo-thermoelectric effect and paves the way for the design of ultrafast graphene arrays in the far infrared, opening concrete perspectives for targeting ultrafast applications.

Plasmonic biosensing has emerged as the most sensitive label-free technique to detect various molecular species in solutions and has already proved crucial in drug discovery, food safety and studies of bio-reactions. This technique relies on surface plasmon resonances in ~50 nm metallic films and the possibility to functionalize the surface of the metal in order to achieve selectivity. At the same time, most metals corrode in bio-solutions, which reduces the quality factor and darkness of plasmonic resonances and thus the sensitivity. Furthermore, functionalization itself might have a detrimental effect on the quality of the surface, also reducing sensitivity. Here we demonstrate that the use of graphene and other layered materials for passivation and functionalization broadens the range of metals which can be used for plasmonic biosensing and increases the sensitivity by 3-4 orders of magnitude, as it guarantees stability of a metal in liquid and preserves the plasmonic resonances under biofunctionalization. We use this approach to detect low molecular weight HT-2 toxins (crucial for food safety), achieving phase sensitivity~0.5 fg/mL, three orders of magnitude higher than previously reported. This proves that layered materials provide a new platform for surface plasmon resonance biosensing, paving the way for compact biosensors for point of care testing.

We report compact, scalable, high-performance, waveguide integrated graphene-based photodetectors (GPDs) for telecom and datacom applications, not affected by dark current. To exploit the photothermoelectric (PTE) effect, our devices rely on a graphene-polymer-graphene stack with static top split gates. The polymeric dielectric, poly(vinyl alcohol) (PVA), allows us to preserve graphene quality and to generate a controllable p-n junction. Both graphene layers are fabricated using aligned single-crystal graphene arrays grown by chemical vapor deposition. The use of PVA yields a low charge inhomogeneity 8 x 10$^{10}$ $cm^{-2}$ at the charge neutrality point, and a large Seebeck coefficient 140 ${\mu}$V K$^{-1}$, enhancing the PTE effect. Our devices are the fastest GPDs operating with zero dark current, showing a flat frequency response up to 67 GHz without roll-off. This performance is achieved on a passive, low-cost, photonic platform, and does not rely on nanoscale plasmonic structures. This, combined with scalability and ease of integration, makes our GPDs a promising building block for next-generation optical communication devices., Comment: 15 pages, 11 figures. Published under ACS AuthorChoice license

III-VI post-transition metal chalcogenides (InSe and GaSe) are a new class of layered semiconductors, which feature a strong variation of size and type of their band gaps as a function of number of layers (N). Here, we investigate exfoliated layers of InSe and GaSe ranging from bulk crystals down to monolayer, encapsulated in hexagonal boron nitride, using Raman spectroscopy. We present the N-dependence of both intralayer vibrations within each atomic layer, as well as of the interlayer shear and layer breathing modes. A linear chain model can be used to describe the evolution of the peak positions as a function of N, consistent with first principles calculations., Comment: 6 pages, 5 figures

Uncooled Terahertz (THz) photodetectors (PDs) showing fast (ps) response and high sensitivity (noise equivalent power (NEP) < $nWHz^{-1/2}$) over a broad (0.5THz-10THz) frequency range are needed for applications in high-resolution spectroscopy (relative accuracy ~ $10^{-11}$), metrology, quantum information, security, imaging, optical communications. However, present THz receivers cannot provide the required balance between sensitivity, speed, operation temperature and frequency range. Here, we demonstrate an uncooled THz PD combining the low (~2000 $k_{B}��m^{-2}$) electronic specific heat of high mobility (> 50000 $cm^{2}V^{-1}s^{-1}$) hBN-encapsulated graphene with the asymmetric field-enhancement produced by a bow-tie antenna resonating at 3 THz. This produces a strong photo-thermoelectric conversion, which simultaneously leads to a combination of high sensitivity (NEP $\leq$ 160 $pWHz^{-1/2}$), fast response time ($\leq 3.3 ns$) and a four orders of magnitude dynamic range, making our devices the fastest, broadband, low noise, room temperature THz PD to date., This is the unedited authors' version of the submitted article, published in its final form at http://dx.doi.org/10.1021/acs.nanolett.9b05207 16 Pages, 4 Figures

Layered materials (LMs), such as graphite, hexagonal boron nitride, and transition-metal dichalcogenides, are at the centre of an ever increasing research effort, due to their scientific and technological relevance. Raman and infrared spectroscopies are accurate, non-destructive, approaches to determine a wide range of properties, including the number of layers and the strength of the interlayer interactions. Here, we present a general approach to predict the complete spectroscopic fan diagrams, i.e., the relations between frequencies and number of layers, $N$, for the optically-active shear and layer-breathing modes of any multilayer comprising $N \geq 2$ identical layers. In order to achieve this, we combine a description of the normal modes in terms of a one-dimensional mechanical model, with symmetry arguments that describe the evolution of the point group as a function of $N$. Group theory is then used to identify which modes are Raman and/or infrared active, and to provide diagrams of the optically-active modes for any stack composed of identical layers. We implement the method and algorithms in an open-source tool directly available on the Materials Cloud portal, to assist any researcher in the prediction and interpretation of such diagrams. Our work will underpin all future efforts on Raman and Infrared characterization of known, and yet not investigated, LMs., Comment: 30 pages (including appendices and tables), 7 figures

Funder: Deutsche Forschungsgemeinschaft (German Research Foundation); doi: https://doi.org/10.13039/501100001659, Laser diodes are efficient light sources. However, state-of-the-art laser diode-based lighting systems rely on light-converting inorganic phosphor materials, which strongly limit the efficiency and lifetime, as well as achievable light output due to energy losses, saturation, thermal degradation, and low irradiance levels. Here, we demonstrate a macroscopically expanded, three-dimensional diffuser composed of interconnected hollow hexagonal boron nitride microtubes with nanoscopic wall-thickness, acting as an artificial solid fog, capable of withstanding ~10 times the irradiance level of remote phosphors. In contrast to phosphors, no light conversion is required as the diffuser relies solely on strong broadband (full visible range) lossless multiple light scattering events, enabled by a highly porous (>99.99%) non-absorbing nanoarchitecture, resulting in efficiencies of ~98%. This can unleash the potential of lasers for high-brightness lighting applications, such as automotive headlights, projection technology or lighting for large spaces.

Herein, a detailed investigation of the surface modification of a zinc oxide (ZnO) nanorod electrode with FeOOH nanoparticles dispersed in glycine was conducted to improve the water oxidation reaction assisted by sunlight. The results were systematically analysed in terms of the general parameters (light absorption, charge separation, and surface for catalysis) that govern the photocurrent density response of metal oxide as photoanode in a photoelectrochemical (PEC) cell. ZnO electrodes surface were modified with different concentration of FeOOH nanoparticles using the spin-coating deposition method, and it was found that 6-layer deposition of glycine-FeOOH nanoparticles is the optimum condition. The glycine plays an important role decreasing the agglomeration of FeOOH nanoparticles over the ZnO electrode surface and increasing the overall performance. Comparing bare ZnO electrodes with the ones modified with glycine-FeOOH nanoparticles an enhanced photocurrent density can be observed from 0.27 to 0.57 mA/cm2 at 1.23 VRHE under sunlight irradiation. The impedance spectroscopy data aid us to conclude that the higher photocurrent density is an effect associated with more efficient surface for chemical reaction instead of electronic improvement. Nevertheless, the charge separation efficiency remains low for this system. The present discovery shows that the combination of glycine-FeOOH nanoparticle is suitable and environmentally-friend cocatalyst to enhance the ZnO nanorod electrode activity for the oxygen evolution reaction assisted by sunlight irradiation.

We report vertically-illuminated, resonant cavity enhanced, graphene-Si Schottky photodetectors (PDs) operating at 1550nm. These exploit internal photoemission at the graphene-Si interface. To obtain spectral selectivity and enhance responsivity, the PDs are integrated with an optical cavity, resulting in multiple reflections at resonance, and enhanced absorption in graphene. Our devices have wavelength-dependent photoresponse with external (internal) responsivity~20mA/W (0.25A/W). The spectral-selectivity may be further tuned by varying the cavity resonant wavelength. Our devices pave the way for developing high responsivity hybrid graphene-Si free-space illuminated PDs for free-space optical communications, coherence optical tomography and light-radars

Carbon-based nonvolatile resistive memories are an emerging technology. Switching endurance remains a challenge in carbon memories based on tetrahedral amorphous carbon (ta-C). One way to counter this is by oxygenation to increase the repeatability of reversible switching. Here, we overview the current status of carbon memories. We then present a comparative study of oxygen-free and oxygenated carbon-based memory devices, combining experiments and molecular dynamics (MD) simulations.

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 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.

© 2002-2012 IEEE. Tetrahedral amorphous (ta-C) carbon-based memory devices have recently gained traction due to their good scalability and promising properties like nanosecond switching speeds. However, cycling endurance is still a key challenge. In this paper, we present a model that takes local fluctuations in sp 2 and sp 3 content into account when describing the conductivity of ta-C memory devices. We present a detailed study of the conductivity of ta-C memory devices ranging from ohmic behavior at low electric fields to dielectric breakdown. The study consists of pulsed switching experiments and device-scale simulations, which allows us for the first time to provide insights into the local temperature distribution at the onset of memory switching.

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.

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., Comment: This document is the Accepted Manuscript version of a Published Work that appeared in final form in ACS Nano after peer review and technical editing by the publisher. To access the final edited and published work see: http://pubs.acs.org/articlesonrequest/AOR-fcCuTYn5m6wiDTIg98Kx

We report the angular distribution of the G and 2D Raman scattering from graphene on glass by detecting back focal plane patterns. The G Raman emission can be described by a superposition of two incoherent orthogonal point dipoles oriented in the graphene plane. Due to double resonant Raman scattering, the 2D emission can be represented by the sum of either three incoherent dipoles oriented 120° with respect to each other, or two orthogonal incoherent ones with a 3:1 weight ratio. Parameter-free calculations of the G and 2D intensities are in excellent agreement with the experimental radiation patterns. We show that the 2D polarization ratio and the 2D/G intensity ratio depend on the numerical aperture of the microscope objective. This is due to the depolarization of the emission and excitation light when graphene is on a dielectric substrate, as well as to tight focusing. The polarization contrast decreases substantially for increasing collection angle, due to polarization mixing caused by the air-dielectric interface. This also influences the intensity ratio I(2D)/I(G), a crucial quantity for estimating the doping in graphene. Our results are thus important for the quantitative analysis of the Raman intensities in confocal microscopy. In addition, they are relevant for understanding the influence of signal enhancing plasmonic antenna structures, which typically modify the sample's radiation pattern.

Oligomers and co-oligomers of carbon oxides (CO & CO2) hold considerable potential as high energy density materials (HEDMs) and are of prospective interest to astrochemists. Here, we theoretically investigate the equilibrium geometries, vibrational frequencies, infrared intensities, Raman activities, and energetics of several C2O3 and C2O4 species. Various DFT functionals were employed (BLYP, B3LYP, PBE, PBE0, ωB97X-D) along with Møller-Plesset methods (MP2, SCS-MP2) using the aug-cc-pVQZ basis set. Further calculations (excluding infrared intensities and Raman activities) were performed using Coupled-Cluster methods (CCSD, CCSD(T), CCSD(2)T) with the cc-pVTZ basis set. We discuss the accuracy and suitability of each method for predicting these properties alongside their capability to handle the multi-reference character of these species (through T1 diagnostic, largest T2 amplitudes, %TAE(T), Aλ). The CCSD(2)T and SCS-MP2 approaches provide modest improvements in accuracy over their CCSD(T) and MP2 counterparts, while from the DFT functionals investigated, B3LYP strikes a balance between accuracy and computational cost. Heats of formation and bond dissociation energies were calculated using composite methods (G3MP2, CCCA-CCL, CCCA-S4). The CO2 dimer of D2h symmetry was found to be the best HEDM candidate since its decomposition (to 2CO2), is highly exothermic (by 260.93 kcal/mol at 298 K), alongside high estimated detonation velocities and pressures.

We report soliton rains in a tunable Tm-doped fiber laser mode locked by carbon nanotubes. We also detect their second- and third-harmonics. We achieve a tunability of over 56 nm, from 1877 to 1933 nm, by introducing a polarization-maintaining isolator and two in-line polarization controllers. This makes our system promising as a tunable filter for ultrafast spectroscopy., We acknowledge funding from ERC Grant Hetero2D, EPSRC Grants Nos. EP/L016087/1, EP/K017144/1, EP/K01711X/1 and the China Scholarship Council.

The thermal properties of airless icy surfaces are providing a wealth of information on their regolith structure after eons of space weathering. Numerous observations of the thermal cycles of Jupiter and Saturn icy satellites or Centaurs and TNOs have been acquired in the latest decades thanks to the Galileo and Cassini missions and to the Spitzer and Herschel telescopes. These observations and the latest developments on thermophysical modeling which have been achieved to link the thermal inertia to the regolith structure are reviewed here. Measured thermal inertias of these surfaces covered with water ice are very low, roughly between about 1 and 100 J/m2/K/s1/2. Often interpreted as due to unconsolidated or highly porous regoliths, these low values may result from a composition of amorphous ice or from the roughness of grains defacing contacts in a regolith of normal compaction. Taken together, thermal inertias appear to increase with probed depth and to decrease with heliocentric distance. This latter effect can be easily reproduced if heat transfer is dominated by radiation in pores, despite low temperatures, because the conduction through grains is limited, either due to the presence of amorphous ice or because of the roughness of grains.

We report an environmentally stable nanotube mode-locked fibre laser producing linearly-polarized, nanosecond pulses. A simple all-polarization-maintaining fibre ring cavity is used, including 300 m of highly nonlinear fibre to elongate the cavity and increase intracavity dispersion and nonlinearity. The laser generates scalar pulses with a duration of 1.23 ns at a centre wavelength of 1042 nm, with 1.3-nm bandwidth and at 641-kHz repetition rate. Despite the long cavity, the output characteristics show no significant variation when the cavity is perturbed, and the degree of polarization remains at 97%.

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., ACS Nano, 2015, 9(7), 7440-7449