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In twisted layered materials (t-LMs), an inter-layer rotation can break inversion symmetry and create an interfacial array of staggered out-of-plane polarization due to AB/BA stacking registries. This symmetry breaking can also trigger the formation of edge in-plane polarizations localized along the perimeter of AB/BA regions (i.e., saddle point domains). However, a comprehensive experimental investigation of these features is still lacking. Here, we use piezo force microscopy to probe the electromechanical behavior of twisted hexagonal boron nitride (t-hBN). For a parallel stacking alignment of t-hBN, we reveal very narrow (width ~ 20 nm) saddle point polarizations, which we also measure in the anti-parallel configuration. These localized polarizations can still be found on a multiply-stacked t-hBN structure, determining the formation of a double moir\'e. We also visualize a t-hBN moir\'e superlattice in the topography maps with atomic force microscopy, related to the strain accumulated at the saddle point domains. Our findings imply that polarizations in t-hBN do not only point in the out-of-plane direction, but also show an in-plane component, giving rise to a much more complex 3D polarization field.

Interlayer excitons in transition-metal dichalcogenide heterobilayers combine high binding energy and valley-contrasting physics with long optical lifetime and strong dipolar character. Their permanent electric dipole enables electric-field control of emission energy, lifetime, and location. Device material and geometry impacts the nature of the interlayer excitons via their real- and momentum-space configurations. Here, we show that interlayer excitons in MoS$_{2}$/MoSe$_{2}$ heterobilayers are formed by charge carriers residing at the Brillouin zone edges, with negligible interlayer hybridization. We find that the moir\'e superlattice leads to the reversal of the valley-dependent optical selection rules, yielding a positively valued g-factor and cross-polarized photoluminescence. Time-resolved photoluminescence measurements reveal that the interlayer exciton population retains the optically induced valley polarization throughout its microsecond-long lifetime. The combination of long optical lifetime and valley polarization retention makes MoS$_{2}$/MoSe$_{2}$ heterobilayers a promising platform for studying fundamental bosonic interactions and developing excitonic circuits for optical information processing.

Machine-learned force fields have transformed the atomistic modelling of materials by enabling simulations of ab initio quality on unprecedented time and length scales. However, they are currently limited by: (i) the significant computational and human effort that must go into development and validation of potentials for each particular system of interest; and (ii) a general lack of transferability from one chemical system to the next. Here, using the state-of-the-art MACE architecture we introduce a single general-purpose ML model, trained on a public database of 150k inorganic crystals, that is capable of running stable molecular dynamics on molecules and materials. We demonstrate the power of the MACE-MP-0 model - and its qualitative and at times quantitative accuracy - on a diverse set problems in the physical sciences, including the properties of solids, liquids, gases, chemical reactions, interfaces and even the dynamics of a small protein. The model can be applied out of the box and as a starting or "foundation model" for any atomistic system of interest and is thus a step towards democratising the revolution of ML force fields by lowering the barriers to entry., Comment: 119 pages, 63 figures, 37MB PDF

Next-generation data networks need to support Tb/s rates. In-phase and quadrature (IQ) modulation combine phase and intensity information to increase the density of encoded data, reduce overall power consumption by minimising the number of channels, and increase noise tolerance. To reduce errors when decoding the received signal, intersymbol interference must be minimised. This is achieved with pure phase modulation, where the phase of the optical signal is controlled without changing its intensity. Phase modulators are characterised by the voltage required to achieve a $\pi$ phase shift V$_{\pi}$, the device length L, and their product V$_{\pi}$L. To reduce power consumption, IQ modulators are needed with$<$1V drive voltages and compact (sub-cm) dimensions, which translate in V$_\pi$L$<$1Vcm. Si and LiNbO$_3$ (LN) IQ modulators do not currently meet these requirements, because V$_{\pi}$L$>$1Vcm. Here, we report a double single-layer graphene (SLG) Mach-Zehnder modulator (MZM) with pure phase modulation in the transparent regime, where optical losses are minimised and remain constant with increasing voltage. Our device has $V_{\pi}L\sim$0.3Vcm, matching state-of-the-art SLG-based MZMs and plasmonic LN MZMs, but with pure phase modulation and low insertion loss ($\sim$5dB), essential for IQ modulation. Our $V_\pi L$ is$\sim$5 times lower than the lowest thin-film LN MZMs, and$\sim$3 times lower than the lowest Si MZMs. This enables devices with complementary metal-oxide semiconductor compatible V$_\pi$L ($<$1Vcm) and smaller footprint than LN or Si MZMs, improving circuit density and reducing power consumption by one order of magnitude.

The integration of optoelectronic devices, such as transistors and photodetectors (PDs), into wearables and textiles is of great interest for applications such as healthcare and physiological monitoring. These require flexible/wearable systems adaptable to body motions, thus materials conformable to non-planar surfaces, and able to maintain performance under mechanical distortions. Here, we prepare fibre PDs combining rolled graphene layers and photoactive perovskites. Conductive fibres ($\sim$500$\Omega$/cm) are made by rolling single layer graphene (SLG) around silica fibres, followed by deposition of a dielectric layer (Al$_{2}$O$_{3}$ and parylene C), another rolled SLG as channel, and perovskite as photoactive component. The resulting gate-tunable PDs have response time$\sim$5ms, with an external responsivity$\sim$22kA/W at 488nm for 1V bias. The external responsivity is two orders of magnitude higher and the response time one order of magnitude faster than state-of-the-art wearable fibre based PDs. Under bending at 4mm radius, up to$\sim$80\% photocurrent is maintained. Washability tests show$\sim$72\% of initial photocurrent after 30 cycles, promising for wearable applications.

Robust spin-photon interfaces in solids are essential components in quantum networking and sensing technologies. Ideally, these interfaces combine a long-lived spin memory, coherent optical transitions, fast and high-fidelity spin manipulation, and straightforward device integration and scaling. The tin-vacancy center (SnV) in diamond is a promising spin-photon interface with desirable optical and spin properties at 1.7 K. However, the SnV spin lacks efficient microwave control and its spin coherence degrades with higher temperature. In this work, we introduce a new platform that overcomes these challenges - SnV centers in uniformly strained thin diamond membranes. The controlled generation of crystal strain introduces orbital mixing that allows microwave control of the spin state with 99.36(9) % gate fidelity and spin coherence protection beyond a millisecond. Moreover, the presence of crystal strain suppresses temperature dependent dephasing processes, leading to a considerable improvement of the coherence time up to 223(10) ${\mu}$s at 4 K, a widely accessible temperature in common cryogenic systems. Critically, the coherence of optical transitions is unaffected by the elevated temperature, exhibiting nearly lifetime-limited optical linewidths. Combined with the compatibility of diamond membranes with device integration, the demonstrated platform is an ideal spin-photon interface for future quantum technologies.

Layered material heterostructures (LMHs) can be used to fabricate electroluminescent devices operating in the visible spectral region. A major advantage of LMH-light emitting diodes (LEDs) is that electroluminescence (EL) emission can be tuned across that of different exciton complexes (e.g. biexcitons, trions, quintons) by controlling the charge density. However, these devices have an EL quantum efficiency as low as$\sim$10$^{-4}$\%. Here, we show that the superacid bis-(triuoromethane)sulfonimide (TFSI) treatment of monolayer WS$_2$-LEDs boosts EL quantum efficiency by over one order of magnitude at room temperature. Non-treated devices emit light mainly from negatively charged excitons, while the emission in treated ones predominantly involves radiative recombination of neutral excitons. This paves the way to tunable and efficient LMH-LEDs

Graphene is an ideal platform to study the coherence of quantum interference pathways by tuning doping or laser excitation energy. The latter produces a Raman excitation profile that provides direct insight into the lifetimes of intermediate electronic excitations and, therefore, on quantum interference, which has so far remained elusive. Here, we control the Raman scattering pathways by tuning the laser excitation energy in graphene doped up to 1.05eV, above what achievable with electrostatic doping. The Raman excitation profile of the G mode indicates its position and full width at half maximum are linearly dependent on doping. Doping-enhanced electron-electron interactions dominate the lifetime of Raman scattering pathways, and reduce Raman interference. This paves the way for engineering quantum pathways in doped graphene, nanotubes and topological insulators., Comment: 18 pages, 4 figures

Janus transition-metal dichalcogenide monolayers are fully artificial materials, where one plane of chalcogen atoms is replaced by chalcogen atoms of a different type. Theory predicts an in-built out-of-plane electric field, giving rise to long-lived, dipolar excitons, while preserving direct-bandgap optical transitions in a uniform potential landscape. Previous Janus studies had broad photoluminescence (>15 meV) spectra obfuscating their excitonic origin. Here, we identify the neutral, and negatively charged inter- and intravalley exciton transitions in Janus WSeS monolayer with $\sim 6$ meV optical linewidth. We combine a recently developed synthesis technique, with the integration of Janus monolayers into vertical heterostructures, allowing doping control. Further, magneto-optic measurements indicate that monolayer WSeS has a direct bandgap at the K points. This work provides the foundation for applications such as nanoscale sensing, which relies on resolving excitonic energy shifts, and photo-voltaic energy harvesting, which requires efficient creation of long-lived excitons and integration into vertical heterostructures.

The generation of stable trains of ultra-short (fs-ps), terahertz (THz)-frequency radiation pulses, with large instantaneous intensities, is an underpinning requirement for the investigation of light-matter interactions, for metrology and for ultra-high-speed communications. In solid-state electrically-pumped lasers, the primary route for generating short pulses is through passive mode-locking. However, this has not yet been achieved in the THz range, defining one of the longest standing goals over the last two decades. In fact, the realization of passive mode-locking has long been assumed to be inherently hindered by the fast recovery times associated with the intersubband gain of THz lasers. Here, we demonstrate a self-starting miniaturized ultra-short pulse THz laser, exploiting an original device architecture that includes the surface patterning of multilayer-graphene saturable absorbers distributed along the entire cavity of a double-metal semiconductor 2.30-3.55 THz wire laser. Self-starting pulsed emission with 4.0-ps-long pulses in a compact, all-electronic, all-passive and inexpensive configuration is demonstrated., Comment: 20 pages, 4 figures

The photoluminescence (PL) spectra of monolayer (1L) semiconductors feature peaks ascribed to different charge-carrier complexes. We perform diffusion quantum Monte Carlo simulations of the binding energies of these complexes and examine their response to electric and magnetic fields. We focus on quintons (charged biexcitons), since they are the largest free charge-carrier complexes in transition-metal dichalcogenides (TMDs). We examine the accuracy of the Rytova-Keldysh interaction potential between charges by comparing the binding energies of charge-carrier complexes in 1L-TMDs with results obtained using $\textit{ab initio}$ interaction potentials. Magnetic fields$<8$T change the binding energies (BEs) by$\sim0.2$ meV,T$^{-1}$, in agreement with experiments, with the BE variations of different complexes being very similar. Our results will help identify charge complexes in the PL spectra of 1L-semiconductors

The unique optoelectronic properties of single layer graphene (SLG) are ideal for the development of photonic devices across a broad range of frequencies, from X-rays to microwaves. In the terahertz (THz) range (0.1-10 THz frequency) this has led to the development of optical modulators, non-linear sources, and photodetectors, with state-of-the-art performances. A key challenge is the integration of SLG-based active elements with pre-existing technological platforms in a scalable way, while maintaining performance level unperturbed. Here, we report on the development of room temperature THz detection in large-area SLG, grown by chemical vapor deposition (CVD), integrated in antenna-coupled field effect transistors. We selectively activate the photo-thermoelectric detection dynamics, and we employ different dielectric configurations on SLG on Al2O3 with and without large-area CVD hBN capping to investigate their effect on SLG thermoelectric properties underpinning photodetection. With these scalable architectures, response times ~5ns and noise equivalent powers ~1nWHz-1/2 are achieved under zero-bias operation. This shows the feasibility of scalable, large-area, layered materials heterostructures for THz detection., Comment: 15 pages, 4 Figures. The following article has been accepted by Applied Physics Letters. After it is published, it will be found at the link https://doi.org/10.1063/5.0097726

The ability to tune the optical response of a material via electrostatic gating is crucial for optoelectronic applications, such as electro-optic modulators, saturable absorbers, optical limiters, photodetectors and transparent electrodes. The band structure of single layer graphene (SLG), with zero-gap, linearly dispersive conduction and valence bands, enables an easy control of the Fermi energy E$_F$ and of the threshold for interband optical absorption. Here, we report the tunability of the SLG non-equilibrium optical response in the near-infrared (1000-1700nm/0.729-1.240eV), exploring a range of E$_F$ from -650 to 250 meV by ionic liquid gating. As E$_F$ increases from the Dirac point to the threshold for Pauli blocking of interband absorption, we observe a slow-down of the photobleaching relaxation dynamics, which we attribute to the quenching of optical phonon emission from photoexcited charge carriers. For E$_F$ exceeding the Pauli blocking threshold, photobleaching eventually turns into photoinduced absorption, due to hot electrons' excitation increasing SLG absorption. The ability to control both recovery time and sign of nonequilibrium optical response by electrostatic gating makes SLG ideal for tunable saturable absorbers with controlled dynamics., Comment: 6 figures

Group-IV color centers in diamond are a promising light-matter interface for quantum networking devices. The negatively charged tin-vacancy center (SnV) is particularly interesting, as its large spin-orbit coupling offers strong protection against phonon dephasing and robust cyclicity of its optical transitions towards spin-photon entanglement schemes. Here, we demonstrate multi-axis coherent control of the SnV spin qubit via an all-optical stimulated Raman drive between the ground and excited states. We use coherent population trapping and optically driven electronic spin resonance to confirm coherent access to the qubit at 1.7 K, and obtain spin Rabi oscillations at a rate of $\Omega/2\pi$=3.6(1) MHz. All-optical Ramsey interferometry reveals a spin dephasing time of $T_2^*$=1.3(3)$\mu$s and two-pulse dynamical decoupling already extends the spin coherence time to $T_2$=0.33(14) ms. Combined with transform-limited photons and integration into photonic nanostructures, our results make the SnV a competitive spin-photon building block for quantum networks.

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 develop two-dimensional micro-spectroscopy to determine exciton-phonon coupling of single-layer MoSe2. We detect beating signals as a function of waiting time T, induced by the coupling between the A exciton and the A'1 optical phonon. Analysis of two-dimensional beating maps combined with simulations provides the exciton-phonon coupling. The Huang-Rhys factor of ~1 is 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 will provide design-relevant parameters for the development of optoelectronic devices.

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., Comment: 22 pages, 5 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

The ability to engineer quantum-cascade-lasers (QCLs) with ultrabroad gain spectra and with a full compensation of the group velocity dispersion, at Terahertz (THz) frequencies, is a fundamental need for devising monolithic and miniaturized optical frequency-comb-synthesizers (FCS) in the far-infrared. In a THz QCL four-wave mixing, driven by the intrinsic third-order susceptibility of the intersubband gain medium, self-lock the optical modes in phase, allowing stable comb operation, albeit over a restricted dynamic range (~ 20% of the laser operational range). Here, we engineer miniaturized THz FCSs comprising a heterogeneous THz QCL integrated with a tightly-coupled on-chip solution-processed graphene saturable-absorber reflector that preserves phase-coherence between lasing modes even when four-wave mixing no longer provides dispersion compensation. This enables a high-power (8 mW) FCS with over 90 optical modes to be demonstrated, over more than 55% of the laser operational range. Furthermore, stable injection-locking is showed, paving the way to impact a number of key applications, including high-precision tuneable broadband-spectroscopy and quantum-metrology., Comment: 31 pages, 11 figures, to be published in ACS Photonics

We present an electrically switchable graphene terahertz (THz) modulator with a tunable-by-design optical bandwidth and we exploit it to compensate the cavity dispersion of a quantum cascade laser (QCL). Electrostatic gating is achieved by a metal-grating used as a gate electrode, with an HfO2/AlOx gate dielectric on top. This is patterned on a polyimide layer, which acts as a quarter wave resonance cavity, coupled with an Au reflector underneath. We get 90% modulation depth of the intensity, combined with a 20 kHz electrical bandwidth in the 1.9 _ 2.7 THz range. We then integrate our modulator with a multimode THz QCL. By adjusting the modulator operational bandwidth, we demonstrate that the graphene modulator can partially compensates the QCL cavity dispersion, resulting in an integrated laser behaving as a stable frequency comb over 35% of the laser operational range, with 98 equidistant optical modes and with a spectral coverage of ~ 1.2 THz. This has significant potential for frontier applications in the terahertz, as tunable transformation-optics devices, active photonic components, adaptive and quantum optics, and as a metrological tool for spectroscopy at THz frequencies., Comment: 22 pages, 6 figures

Graphene and related materials can lead to disruptive advances in next generation photonics and optoelectronics. The challenge is to devise growth, transfer and fabrication protocols providing high (>5,000 cm2 V-1 s-1) mobility devices with reliable performance at the wafer scale. Here, we present a flow for the integration of graphene in photonics circuits. This relies on chemical vapour deposition (CVD) of single layer graphene (SLG) matrices comprising up to ~12000 individual single crystals (SCs), grown to match the geometrical configuration of the devices in the photonic circuit. This is followed by a transfer approach which guarantees coverage over ~80% of the device area, and integrity for up to 150 mm wafers, with room temperature mobility ~5000 cm2 V-1 s-1. We use this process flow to demonstrate double SLG electro-absorption modulators with modulation efficiency ~0.25, 0.45, 0.75, 1 dB V-1 for device lengths ~30, 60, 90, 120 {\mu}m. The data rate is up to 20 Gbps. Encapsulation with single-layer hBN is used to protected SLG during plasma-enhanced CVD of Si3N4, ensuring reproducible device performance. Our full process flow (from growth to device fabrication) enables the commercial implementation of graphene-based photonic devices., Comment: 30 pages, 9 Figures

Layered materials (LMs) are at the centre of an ever increasing research effort due to their potential use in a variety of applications. The presence of imperfections, such as bi- or multilayer areas, holes, grain boundaries, isotropic and anisotropic deformations, etc. are detrimental for most (opto)electronic applications. Here, we present a set-up able to transform a conventional scanning electron microscope into a tool for structural analysis of a wide range of LMs. An hybrid pixel electron detector below the sample makes it possible to record two dimensional (2d) diffraction patterns for every probe position on the sample surface (2d), in transmission mode, thus performing a 2d+2d=4d STEM (scanning transmission electron microscopy) analysis. This offers a field of view up to 2 mm2, while providing spatial resolution in the nm range, enabling the collection of statistical data on grain size, relative orientation angle, bilayer stacking, strain, etc. which can be mined through automated open-source data analysis software. We demonstrate this approach by analyzing a variety of LMs, such as mono- and multi-layer graphene, graphene oxide and MoS2, showing the ability of this method to characterize them in the tens of nm to mm scale. This wide field of view range and the resulting statistical information are key for large scale applications of LMs., Comment: A. Orekhov and D. Jannis contributed equally to this work. J. Verbeeck is corresponding author

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.

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

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 attening caused by Pauli blocking. In the biased sample, photoexcitation 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.

Energy relaxation of photo-excited charge carriers is of significant fundamental interest and crucial for the performance of monolayer (1L) transition metal dichaclogenides (TMDs) in optoelectronics. We measure light scattering and emission in 1L-WSe$_2$ close to the laser excitation energy (down to~$\sim$0.6meV). We detect a series of periodic maxima in the hot photoluminescence intensity, stemming from energy states higher than the A-exciton state, in addition to sharp, non-periodic Raman lines related to the phonon modes. We find a period $\sim$15meV for peaks both below (Stokes) and above (anti-Stokes) the laser excitation energy. We detect 7 maxima from 78K to room temperature in the Stokes signal and 5 in the anti-Stokes, of increasing intensity with temperature. We assign these to phonon cascades, whereby carriers undergo phonon-induced transitions between real states in the free-carrier gap with a probability of radiative recombination at each step. We infer that intermediate states in the conduction band at the $\Lambda$-valley of the Brillouin zone participate in the cascade process of 1L-WSe$_2$. The observations explain the primary stages of carrier relaxation, not accessible so far in time-resolved experiments. This is important for optoelectronic applications, such as photodetectors and lasers, because these determine the recovery rate and, as a consequence, the devices' speed and efficiency., Comment: 13 pages, 10 figures

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 $\mu$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., Comment: 11 pages, 5 figures

Ultrafast and sensitive (noise equivalent power <1 nWHz-1/2) light-detection in the Terahertz (THz) frequency range (0.1-10 THz) and at room-temperature is key for applications such as time-resolved THz spectroscopy of gases, complex molecules and cold samples, imaging, metrology, ultra-high-speed data communications, coherent control of quantum systems, quantum optics and for capturing snapshots of ultrafast dynamics, in materials and devices, at the nanoscale. Here, we report room-temperature THz nano-receivers exploiting antenna-coupled graphene field effect transistors integrated with lithographically-patterned high-bandwidth (~100 GHz) chips, operating with a combination of high speed (hundreds ps response time) and high sensitivity (noise equivalent power <120 pWHz-1/2) at 3.4 THz. Remarkably, this is achieved with various antenna and transistor architectures (single-gate, dual-gate), whose operation frequency can be extended over the whole 0.1-10 THz range, thus paving the way for the design of ultrafast graphene arrays in the far infrared, opening concrete perspective for targeting the aforementioned applications., Comment: This is the unedited authors' version of the article accepted for publication in Nanophotonics 2020 (Online ISSN: 2192-8614)

To promote structurally flexible controllers in self-adaptive software systems, this paper proposes the use of micro-controllers. Instead of generic monolithic controllers, like Rainbow, we advocate the use of service-specific micro-controllers which can be based on microservices. Although traditional generic controllers can be configured parametrically according to system needs, their use and reuse are nevertheless restrictive because of the wide range of services expected from the different stages of the feedback control loop.The solution being advocated is to have structurally flexible controllers that can be composed from micro-controllers. Controlling the architectural configuration of these micro-controllers is a meta-controller that is able to configure the controller according to the services required for controlling the target system. The feasibility of the proposed approach of using micro-controllers at the level of the controller is demonstrated in the context of the PhoneAdapter case study in which micro-controllers are configured at run-time depending on changes affecting the system or its environment., Comment: 10 pages, 4 figures

Interlayer excitons in layered materials constitute a novel platform to study many-body phenomena arising from long-range interactions between quantum particles. The ability to localise individual interlayer excitons in potential energy traps is a key step towards simulating Hubbard physics in artificial lattices. Here, we demonstrate spatial localisation of long-lived interlayer excitons in a strongly confining trap array using a WS$_{2}$/WSe$_{2}$ heterostructure on a nanopatterned substrate. We detect long-lived interlayer excitons with lifetime approaching 0.2 ms and show that their confinement results in a reduced lifetime in the microsecond range and stronger emission rate with sustained optical selection rules. The combination of a permanent dipole moment, spatial confinement and long lifetime places interlayer excitons in a regime that satisfies one of the requirements for observing long-range dynamics in an optically resolvable trap lattice.

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 $k_{B}{\mu}m^{-2}$) 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., Comment: 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

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

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.

Electromagnetic interference (EMI) shielding coating materials with thicknesses in the microscale are required in many sectors, including communications, medical, aerospace and electronics, to isolate the electromagnetic radiation emitted from electronic equipment. We report a spray, layer-by-layer (LbL) coating approach to fabricate micron thick, highly-ordered and electrically-conductive coatings with exceptional EMI shielding effectiveness (EMI SE >4830 dB/mm), through the alternating self-assembly of negatively-charged reduced graphene oxide (RGO) and a positively-charged polyelectrolyte (PEI). The microstructure and resulting electrical properties of the (PEI/RGO)n LbL structures are studied as function of increasing mass of graphene deposited per cycle (keeping the PEI content constant), number of deposited layers (n), flake diameter and type of RGO. A strong effect of the lateral flake dimensions on the electrical properties is observed, which also influences the EMI SE. A maximum EMI SE of 29 dB is obtained for a 6 um thick (PEI/RGO)10 coating with 19 vol.% loading of reduced electrochemically-exfoliated graphene oxide flakes with diameters ~3um. This SE performance exceeds those previously reported for thicker graphene papers and bulk graphene/polymer composite films with higher RGO or graphene nanoplatelets contents, which represents an important step towards the fabrication of thin and light-weight high-performance EMI shielding structures., Comment: 34 pages,7 figures

Graphene is an ideal material for optoelectronic applications. Its photonic properties give several advantages and complementarities over Si photonics. For example, graphene enables both electro-absorption and electro-refraction modulation with an electro-optical index change exceeding 10$^{-3}$. It can be used for optical add-drop multiplexing with voltage control, eliminating the current dissipation used for the thermal detuning of microresonators, and for thermoelectric-based ultrafast optical detectors that generate a voltage without transimpedance amplifiers. Here, we present our vision for grapheme-based integrated photonics. We review graphene-based transceivers and compare them with existing technologies. Strategies for improving power consumption, manufacturability and wafer-scale integration are addressed. We outline a roadmap of the technological requirements to meet the demands of the datacom and telecom markets. We show that graphene based integrated photonics could enable ultrahigh spatial bandwidth density , low power consumption for board connectivity and connectivity between data centres, access networks and metropolitan, core, regional and long-haul optical communications.