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We introduce a two-step, fully reversible process designed to project the outer shape of a generic droplet onto a lower-dimensional space. The initial step involves representing the droplet's shape as a Fourier series. Subsequently, the Fourier coefficients are reduced to lower-dimensional vectors by using autoencoder models. The exploitation of the domain knowledge of the droplet shapes allows us to map generic droplet shapes to just 2D space in contrast to previous direct methods involving autoencoders that could map it on minimum 8D space. This 6D reduction in the dimensionality of the droplet's description opens new possibilities for applications, such as automated droplet generation via reinforcement learning, the analysis of droplet shape evolution dynamics and the prediction of droplet breakup. Our findings underscore the benefits of incorporating domain knowledge into autoencoder models, highlighting the potential for increased accuracy in various other scientific disciplines., Comment: 7 pages, 8 figures

In microfluidic systems, droplets undergo intricate deformations as they traverse flow-focusing junctions, posing a challenging task for accurate measurement, especially during short transit times. This study investigates the physical behavior of droplets within dense emulsions in diverse microchannel geometries, specifically focusing on the impact of varying opening angles within the primary channel and injection rates of fluid components. Employing a sophisticated droplet tracking tool based on deep-learning techniques, we analyze multiple frames from flow-focusing experiments to quantitatively characterize droplet deformation in terms of ratio between maximum width and height and propensity to form liquid with hexagonal crystalline order. Our findings reveal the existence of an optimal opening angle where shape deformations are minimal and crystal-like arrangement is maximal. Variations of fluid injection rates are also found to affect size and packing fraction of the emulsion in the exit channel. This paper offers insights into deformations, size and structure of fluid emulsions relative to microchannel geometry and other flow-related parameters captured through machine learning, with potential implications for the design of microchips utilized in cellular transport and tissue engineering applications., Comment: 11 pages, 7 figures

The integration of 2D nanomaterials with silicon is expected to enrich the applications of 2D functional nanomaterials and to pave the way for next-generation, nanoscale optoelectronics with enhanced performances. Herein, a strategy for rare earth element doping has been utilized for the synthesis of 2D WS$_2$:Er nanosheets to achieve up-conversion and down-conversion emission ranging from visible to the near-infrared region. Moreover, the potential integration of the synthesized 2D nanosheets in silicon platforms is demonstrated by the realization of an infrared photodetector based on a WS$_2$:Er/Si heterojunction. These devices operate at room temperature and show a high photoresponsivity of ~39.8 mA/W (at 980 nm) and a detectivity of 2.79 $\times$ 10$^{10}$ cm Hz$^{1/2}$ W$^{-1}$. Moreover, the dark current and noise power density are suppressed effectively by van der Waals assisted p-n heterojunction. This work fundamentally contributes to establishing infrared detection by rare element doping of 2D materials in heterojunctions with Si, at the forefront of infrared 2D materials-based photonics., Comment: 34 pages, 9 Figures, Advanced Materials Interfaces, 2022

The optical gain of blue light-emitting electrospun polystyrene fibers doped with a linear multi-fragment molecular dye based on the combination of fluorine-carbazole functional units is investigated, with the aim of correlating emission properties and the specific material architecture made of either aligned or disordered fibers. Enhanced performance is found in aligned fibers, whose gain spectrum can be finely tuned by varying the dye concentration. Instead, randomly oriented fibers show a manifold spectral line narrowing, resulting in sharp laser peaks superimposed on top of a broad emission band, ascribable to random lasing. In these systems, the increase of the dye content turns out to be effective for both decreasing the lasing threshold by about a factor 6 and for varying the laser emission wavelength. These results make these arrays and disordered architectures of fibers valuable active media for variable-gain, broadband lasing, which is remarkably important in optical sensing and tunable microlaser devices., Comment: 24 pages, 12 Figures, 1 Table, Journal of Materials Chemistry C, 2022

Fluid flows hosting electrical phenomena make the subject of a fascinating and highly interdisciplinary scientific field. In recent years, the extraordinary success of electrospinning and solution blowing technologies for the generation of polymer nanofibers has motivated vibrant research aiming at rationalizing the behavior of viscoelastic jets under applied electric fields or other stretching fields including gas streams. Theoretical models unveiled many original aspects in the underpinning physics of polymer solutions in jets, and provided useful information to improve experimental platforms. This article reviews advances in the theoretical description and numerical simulation of polymer solution jets in electrospinning and solution blowing. Instability phenomena of electrical and hydrodynamic origin are highlighted, which play a crucial role in the relevant flow physics. Specifications leading to accurate and computationally viable models are formulated. Electrohydrodynamic modeling, theories for the jet bending instability, recent advances in Lagrangian approaches to describe the jet flow, including strategies for dynamic refinement of simulations, and effects of strong elongational flow on polymer networks are reviewed. Finally, the current challenges and future perspectives of the field are outlined and discussed, including the task of correlating the physics of the jet flows with the properties of realized materials, as well as the development of multiscale techniques for modelling viscoelastic jets., Comment: 135 pages, 42 figures

Tracking droplets in microfluidics is a challenging task. The difficulty arises in choosing a tool to analyze general microfluidic videos to infer physical quantities. The state-of-the-art object detector algorithm You Only Look Once (YOLO) and the object tracking algorithm Simple Online and Realtime Tracking with a Deep Association Metric (DeepSORT) are customizable for droplet identification and tracking. The customization includes training YOLO and DeepSORT networks to identify and track the objects of interest. We trained several YOLOv5 and YOLOv7 models and the DeepSORT network for droplet identification and tracking from microfluidic experimental videos. We compare the performance of the droplet tracking applications with YOLOv5 and YOLOv7 in terms of training time and time to analyze a given video across various hardware configurations. Despite the latest YOLOv7 being 10% faster, the real-time tracking is only achieved by lighter YOLO models on RTX 3070 Ti GPU machine due to additional significant droplet tracking costs arising from the DeepSORT algorithm. This work is a benchmark study for the YOLOv5 and YOLOv7 networks with DeepSORT in terms of the training time and inference time for a custom dataset of microfluidic droplets., Comment: 13 pages, 4 figures, 3 tables

The delivery of optical signals from an external light source to a nanoscale waveguide is highly important for the development of nanophotonic circuits. However, the efficient coupling of external light energy into nanophotonic components is difficult and still remains a challenge. Herein, we use an external silica nanofiber to light up an organic-inorganic hybrid nano-waveguide, namely a system composed of a polymer filament doped with MoS$_{2}$ quantum dots. Nanofiber-excited nano-waveguides in a crossed geometry are found to asymmetrically couple excitation signals along two opposite directions, with different energy dissipation resulting in different colors of the light emitted by MoS$_{2}$ quantum dots and collected from the waveguide terminals. Interestingly, rainbow-like light in the hybrid waveguide is achieved by three-in-one mixing of red, green, and blue components. This hetero-dimensional system of dots-in-waveguide represents a significant advance towards all-optical routing and full-color display in integrated nanophotonic devices., Comment: 26 pages, 11 Figures, Journal of Physical Chemistry Letters, 2021

Photopolymerization processes are exploited in light exposure-based 3D printing technologies, where either a focused laser beam or a patterned light sheet allows layers of a UV curable, liquid pre-polymer to be solidified. Here we focus on the crucial, though often neglected, role of the layer thickness on photopolymerization. The temporal evolution of polymerization reactions occurring in droplets of acrylate-based oligomers and in photoresist films with varied thickness is investigated by means of an optical system, which is specifically designed for in-situ and real-time monitoring. The time needed for complete curing is found to increase as the polymerization volume is decreased below a characteristic threshold that depends on the specific reaction pathway. This behavior is rationalized by modelling the process through a size-dependent polymerization rate. Our study highlights that the formation of photopolymerized networks might be affected by the involved volumes regardless of the specific curing mechanisms, which could play a crucial role in optimizing photocuring-based additive manufacturing., Comment: 31 pages, 10 figures, 1 table

Refractive freeform components are becoming increasingly relevant for generating controlled patterns of light, because of their capability to spatially-modulate optical signals with high efficiency and low background. However, the use of these devices is still limited by difficulties in manufacturing macroscopic elements with complex, 3-dimensional (3D) surface reliefs. Here, 3D-printed and stretchable magic windows generating light patterns by refraction are introduced. The shape and, consequently, the light texture achieved can be changed through controlled device strain. Cryptographic magic windows are demonstrated through exemplary light patterns, including micro-QR-codes, that are correctly projected and recognized upon strain gating while remaining cryptic for as-produced devices. The light pattern of micro-QR-codes can also be projected by two coupled magic windows, with one of them acting as the decryption key. Such novel, freeform elements with 3D shape and tailored functionalities is relevant for applications in illumination design, smart labels, anti-counterfeiting systems, and cryptographic communication., Comment: 31 pages, 22 figures, Advanced Materials Technologies 2022

Recently, random lasing in complex networks has shown efficient lasing over more than 50 localised modes, promoted by multiple scattering over the underlying graph. If controlled, these network lasers can lead to fast-switching multifunctional light sources with synthesised spectrum. Here, we observe both in experiment and theory high sensitivity of the network laser to the spatial shape of the pump profile, with mode intensity variation of up to 280% for a non-homogeneous 7% pump decrease. We solve the nonlinear equations within the steady state ab-initio laser theory (SALT) approximation over a graph and we show selective lasing of around 90% of the top modes, effectively programming the spectrum of the lasing networks. In our experiments with polymer networks, this high sensitivity enables control of the lasing spectrum through non-uniform pump patterns. We propose the underlying complexity of the network modes as the key element behind efficient spectral control opening the way for the development of optical devices with wide impact for on-chip photonics for communication, sensing and computation., Comment: 22 pages, 14 figures

In the past decade, complex networks of light emitters are proposed as novel platforms for photonic circuits and lab-on-chip active devices. Lasing networks made by connected multiple gain components and graphs of nanoscale random lasers (RLs) obtained from complex meshes of polymeric nanofibers are successful prototypes. However, in the reported research, mainly collective emission from a whole network of resonators is investigated, and only in a few cases, the emission from single points showing, although homogeneous and broad, spatial emission. In all cases, simultaneous activation of the miniaturized lasers is observed. Here, differently, we realize heterogeneous random lasers made of ribbon-like and highly porous fibers with evident RL action from separated micrometric domains that alternatively switch on and off by tuning the pumping light intensity. We visualize this novel effect by building for the first time replica symmetry breaking (RSB) maps of the emitting fibers with 2 {\mu}m spatial resolution. In addition, we calculate the spatial correlations of the laser regions showing clearly an average extension of 50 {\mu}m. The observed blinking effect is due to mode interaction along light guiding fibers and opens new avenues in the fabrication of flexible photonic networks with specific and adaptable activity., Comment: 22 pages, 7 Figures, ACS Photonics, 2021

Technologies operating on the basis of quantum mechanical laws and resources such as phase coherence and entanglement are expected to revolutionize our future. Quantum technologies are often divided into four main pillars: computing, simulation, communication, and sensing & metrology. Moreover, a great deal of interest is currently also nucleating around energy-related quantum technologies. In this Perspective, we focus on advanced superconducting materials, van der Waals materials, and moir\'e quantum matter, summarizing recent exciting developments and highlighting a wealth of potential applications, ranging from high-energy experimental and theoretical physics to quantum materials science and energy storage., Comment: 19 pages, 4 figures, 215 references, Perspective article on solid-state quantum technologies

We demonstrate a graphene-MoS2 architecture integrating multiple field-effect transistors and we independently probe and correlate the conducting properties of van der Waals coupled graphene-MoS2 contacts with the ones of the MoS2 channels. Devices are fabricated starting from high-quality single-crystal monolayers grown by chemical vapor deposition and characterized by scanning Raman and photoluminescence spectroscopies. Transconductance curves of MoS2 are compared with the current-voltage characteristics of graphene contact stripes, revealing a significant suppression of transport on the n-side of the transconductance curve. Based on ab-initio modeling, the effect is understood in terms of trapping by sulfur vacancies, which counter-intuitively depends on the field-effect, even though the graphene contact layer is positioned between the backgate and the MoS2 channel.

We introduce a mesoscale approach for the simulation of multicomponent flows to model the direct-writing printing process, along with the early stage of ink deposition. As an application scenario, alginate solutions at different concentrations are numerically investigated alongside processing parameters, such as apparent viscosity, extrusion rate, and print head velocity. The present approach offers useful insights on the ink rheological effects upon printed products, susceptible to geometric accuracy and shear stress, by manufacturing processes such as the direct-writing printing for complex photonic circuitry, bio-scaffold fabrication, and tissue engineering., Comment: 14 pages, 5 figures

Combined dry-wet transient materials and devices are introduced, which are based on water-dissolvable dye-doped polymers layered onto non-polar cyclic hydrocarbon sublimating substrates. Light-emitting heterostructures showing amplified spontaneous emission are used as illumination sources for speckle-free, full-field imaging, and transient optical labels are realized that incorporate QR codes with stably encoded information. The transient behavior is also studied at the microscopic scale, highlighting the real time evolution of material domains in the sublimating compound. Finally, the exhausted components are fully soluble in water thus being naturally degradable., Comment: 30 pages, 15 figures

Lasers based on biological materials are attracting an increasing interest in view of their use in integrated and transient photonics. DNA as optical biopolymer in combination with highly-emissive dyes has been reported to have excellent potential in this respect, however achieving miniaturized lasing systems based on solid-state DNA shaped in different geometries to confine and enhance emission is still a challenge, and physico-chemical mechanisms originating fluorescence enhancement are not fully understood. Herein, a class of wavelength-tunable lasers based on DNA nanofibers is demonstrated, for which optical properties are highly controlled through the system morphology. A synergistic effect is highlighted at the basis of lasing action. Through a quantum chemical investigation, we show that the interaction of DNA with the encapsulated dye leads to hindered twisting and suppressed channels for the non-radiative decay. This is combined with effective waveguiding, optical gain, and tailored mode confinement to promote morphologically-controlled lasing in DNA-based nanofibers. The results establish design rules for the development of bright and tunable nanolasers and optical networks based on DNA nanostructures., Comment: 31 pages, 11 figures and 2 tables

Anthracene derivative compounds are currently investigated because of their unique physical properties (e.g., bright luminescence and emission tunability), which make them ideal candidates for advanced optoelectronic devices. Intermolecular interactions are the basis of the tunability of the optical and electronic properties of these compounds, whose prediction and exploitation benefit from the knowledge of the crystal structure and the packing architecture. Polymorphism can occur due to the weak intermolecular interactions, asking for detailed structural analysis clarifying the origin of observed material property modifications. Here, two silylethyne-substituted anthracene compounds are characterized by single-crystal synchrotron X-ray diffraction, identifying a new polymorph. Additionally, laser confocal microscopy and fluorescence lifetime imaging microscopy confirm the results obtained by the X-ray diffraction characterization, i.e., shifting the substituents towards the external benzene rings of the anthracene unit favours {\pi}-{\pi} interactions, impacting on both the morphology and the microscopic optical properties of the crystals. The compounds with more isolated anthracene units feature shorter lifetime and emission spectra more similar to those ones of isolated molecules. The crystallographic study, supported by the optical investigation, sheds light on the influence of non-covalent interactions on the crystal packing and luminescence properties of anthracene derivatives, providing a further step towards their efficient use as building blocks in active components of light sources and photonic networks., Comment: 39 pages, 16 figures, 3 tables

The mechanisms governing mechanical dissipation in amorphous tantala are studied at microscopic scale via Molecular Dynamics simulations, namely by mechanical spectroscopy in a wide range of temperature and frequency. We find that dissipation is associated with irreversible atomic rearrangements with a sharp cooperative character, involving tens to hundreds of atoms arranged in spatially extended clusters of polyhedra. Remarkably, at low temperature we observe an excess of plastically rearranging oxygen atoms which correlates with the experimental peak in the macroscopic mechanical losses. A detailed structural analysis reveals preferential connections of the irreversibly rearranging polyhedra, corresponding to edge and face sharing. These results might lead to microscopically informed design rules for reducing mechanical losses in relevant materials for structural, optical, and sensing applications.

The miniaturization of diagnostic devices that exploit optical detection schemes requires the design of light-sources combining small size, high performance for effective excitation of chromophores, and mechanical flexibility for easy coupling to components with complex and non-planar shapes. Here, ZnO nanowire-in-fiber hybrids with internal architectural order are introduced, exhibiting a combination of polarized stimulated emission, low propagation losses of light modes, and structural flexibility. Ultrafast transient absorption experiments on the electrospun material show optical gain which gives rise to amplified spontaneous emission, with threshold lower than the value found in films. These systems are highly flexible and can conveniently conform to curved surfaces, which makes them appealing active elements for various device platforms, such as bendable lasers, optical networks and sensors, as well as for application in bioimaging, photo-crosslinking, and optogenetics., Comment: 50 pages, 17 figures, 1 table, ACS Nano, 2020

Wrought by nature's wondrous hand, surface topographies are discovered on all length scales in living creatures and serve a variety of functions. Inspired by floral striations, here we developed a scalable means of fabricating custom-tailored photonic cellulose films that contained both cholesteric organization and microscopic wrinkly surface topography. Free-standing films were prepared by molding cellulose nanocrystal ink onto an oriented wrinkled template through evaporation-assisted nanoimprinting lithography, yielding morphology-induced light scattering at a short wavelength as well as optically tunable structural color derived from the helical cellulose matrix. As a result, the interplay between the two photonic structures, grating-like surface and chiral bulk, led to selective scattering of circularly polarized light with specific handedness. Moreover, the wrinkled surface relief on cholesteric cellulose films could be precisely controlled, enabling engineered printing of microscopic patterned images., Comment: 50 pages, 31 Figures

All-optical switches are introduced which are based on deoxyribonucleic acid (DNA) in the form of electrospun fibers, where DNA is semi-intercalated with a push-pull, luminescent nonlinear pyrazoline derivative. Optical birefringence is found in the organic nanofibers, with fully reversible switching controlled through continuous-wave laser irradiation. The photoinduced signal is remarkably large, with birefringence highlighted by optically-driven refractive index anisotropy approaching 0.001. Sub-millisecond characteristic switching times are found. Integrating dye-intercalated DNA complex systems in organic nanofibers, as convenient and efficient approach to template molecular organization and controlling it by external stimuli, might open new routes for realizing optical logic gates, reconfigurable photonic networks and sensors through physically-transient biopolymer components., Comment: 18 pages, 11 figures. Journal of Materials Chemistry C, 2018

Molybdenum disulfide (MoS2) has been attracting extraordinary attention for its intriguing optical, electronic and mechanical properties. Here we demonstrate hybrid, organic-inorganic light-emitting nanofibers based on MoS2 nanoparticle dopants obtained through a simple and inexpensive sonication process in N-methyl-2-pyrrolidone and successfully encapsulated in polymer filaments. Defectiveness is found to be kept low, and stoichiometry preserved, by the implemented, gentle exfoliation method that allows the MoS2 nanoparticles to be produced. So-achieved hybrid fibers are smooth, uniform, flawless, and exhibit bright and continuous light emission. Moreover, they show significant capability of waveguiding self-emitted light along their longitudinal axis. These findings suggest the use of emissive MoS2 fibers enabled by gentle exfoliation methods as novel and highly promising optical material for building sensing surfaces and as components of photonic circuits., Comment: 22 pages, 9 figures, Nanoscale, 2018

We present stacked organic lasing heterostructures made by different species of light-emitting electrospun fibers, each able to provide optical gain in a specific spectral region. A hierarchical architecture is obtained by conformable layers of fibers with disordered two-dimensional organization and three-dimensional compositional heterogeneity. Lasing polymer fibers are superimposed in layers, showing asymmetric optical behavior from the two sides of the organic heterostructure, and tailored and bichromatic stimulated emission depending on the excitation direction. A marginal role of energy acceptor molecules in determining quenching of high-energy donor species is evidenced by luminescence decay time measurements. These findings show that non-woven stacks of light-emitting electrospun fibers doped with different dyes exhibit critically-suppressed F\"orster resonance energy transfer, limited at joints between different fiber species. This leads to obtain hybrid materials with mostly physically-separated acceptors and donors, thus largely preventing donor quenching and making much easier to achieve simultaneous lasing from multiple spectral bands. Coherent backscattering experiments are also performed on the system, suggesting the onset of random lasing features. These new organic lasing systems might find application in microfluidic devices where flexible and bidirectional excitation sources are needed, optical sensors, and nanophotonics., Comment: 18 pages, 6 figures

Hybrid polymer-plasmonic nanostructures might combine high enhancement of localized fields from metal nanoparticles with light confinement and long-range transport in subwavelength dielectric structures. Here we report on the complex behavior of fluorophores coupling to Au nanoparticles within polymer nanowires, which features localized metal-enhanced fluorescence (MEF) with unique characteristics compared to conventional structures. The intensification effect when the particle is placed in the organic filaments is remarkably higher with respect to thin films of comparable thickness, thus highlighting a specific, nanowire-related enhancement of MEF effects. A dependence on the confinement volume in the dielectric nanowire is also evidenced, with MEF significantly increasing upon reducing the wire diameter. These findings are rationalized by finite element simulations, predicting a position-dependent enhancement of the quantum yield of fluorophores embedded in the fibers. Calculation of the ensemble-averaged fluorescence enhancement unveils the possibility of strongly enhancing the overall emission intensity for structures with size twice the diameter of the embedded metal particles. These new, hybrid fluorescent systems with localized enhanced emission, as well as the general Nanowire-Intensified MEF effect associated to them, are highly relevant for developing nanoscale light-emitting devices with high efficiency and inter-coupled through nanofiber networks, highly sensitive optical sensors, and novel laser architectures., Comment: 29 pages, 12 figures, Small (2018)

Hybrid conjugated polymer/fullerene filaments based on MEH-PPV/PVP/PCBM are prepared by electrospinning, and their properties assessed by scanning electron, atomic and lateral force, tunnelling, and confocal microscopy, as well as by attenuated total reflection Fourier transform-infrared spectroscopy, photoluminescence quantum yield and spatially-resolved fluorescence. Highlighted features include ribbon-shape of the realized fibers, and the persistence of a network serving as a template for heterogeneous active layers in solar cell devices. A set of favorable characteristics is evidenced in this way in terms of homogeneous charge transport behavior and formation of effective interfaces for diffusion and dissociation of photogenerated excitons. The interaction of the organic filaments with light, exhibiting specific light-scattering properties of the nanofibrous mat, might also contribute to spreading incident radiation across the active layers, thus potentially enhancing photovoltaic performance. This method might be applied to other electron donor-electron acceptor material systems for the fabrication of solar cell devices enhanced by nanofibrillar morphologies embedding conjugated polymers and fullerene compounds., Comment: 35 pages, 9 figures

Concomitant amplified spontaneous emission (ASE) and F\"orster resonance energy transfer (FRET) are investigated in electrospun light-emitting fibers. Upon dye-doping with a proper FRET couple system, free-standing fibrous mats exhibit tunable FRET efficiency and, more importantly, tailorable threshold conditions for stimulated emission. In addition, effective scattering of light is found in the fibrous material by measuring the transport mean free path of photons by coherent backscattering experiments. The interplay of ASE and FRET leads to high control in designing optical properties from electrospun fibers, including the occurrence of simultaneous stimulated emission from both donor and acceptor components. All tunable-optical properties are highly interesting in view of applying electrospun light-emitting materials in lightening, display, and sensing technologies., Comment: 32 pages, 13 figures

Random lasers are based on disordered materials with optical gain. These devices can exhibit either intensity or resonant feedback, relying on diffusive or interference behaviour of light, respectively, which leads to either coupling or independent operation of lasing modes. We study for the first time these regimes in complex, solid-state nanostructured materials. The number of lasing modes and their intensity correlation features are found to be tailorable in random lasers made of light-emitting, electrospun polymer fibers upon nanoparticle doping. By material engineering, directional waveguiding along the length of fibers is found to be relevant to enhance mode correlation in both intensity feedback and resonant feedback random lasing. The here reported findings can be used to establish new design rules for tuning the emission of nano-lasers and correlation properties by means of the compositional and morphological properties of complex nanostructured materials., Comment: 30 pages, 10 figures

The control of strain in two-dimensional materials opens exciting perspectives for the engineering of their electronic properties. While this expectation has been validated by artificial-lattice studies, it remains elusive in the case of atomic lattices. Remarkable results were obtained on nanobubbles and nano-wrinkles, or using scanning probes; microscale strain devices were implemented exploiting deformable substrates or external loads. These devices lack, however, the flexibility required to fully control and investigate arbitrary strain profiles. Here, we demonstrate a novel approach making it possible to induce strain in graphene using polymeric micrometric artificial muscles (MAMs) that contract in a controllable and reversible way under an electronic stimulus. Our method exploits the mechanical response of poly-methyl-methacrylate (PMMA) to electron-beam irradiation. Inhomogeneous anisotropic strain and out-of-plane deformation are demonstrated and studied by Raman, scanning-electron and atomic-force microscopy. These can all be easily combined with the present device architecture. The flexibility of the present method opens new opportunities for the investigation of strain and nanomechanics in two-dimensional materials.

New materials aim at exploiting the great control of living organisms over molecular architectures and minerals. Optical biomimetics has been widely developed by microengineering, leading to photonic components with order resembling those found in plants and animals. These systems, however, are realized by complicated and adverse processes. Here we show how biomineralization might enable the one-step generation of components for amorphous photonics, in which light is made to travel through disordered scattering systems, and particularly of active devices such as random lasers, by using electrospun fiber templates. The amount of bio-enzymatically produced silica is related to light-scattering capacity and the resulting organosilica surfaces exhibit a transport mean free path for light as low as 3 micron, and lasing with linewidth below 0.2 nm. The resulting, complex optical material is characterized and modelled to elucidate scattered fields and lasing performance. Tightly-controlled nanofabrication of direct biological inspiration establishes a new concept for the additive manufacturing of engineered light-diffusing materials and photonic components, not addressed by existing technologies., Comment: 37 pages, 11 figures

Conventional nano-photonic schemes minimise multiple scattering to realise a miniaturised version of beam-splitters, interferometers and optical cavities for light propagation and lasing. Here instead, we introduce a nanophotonic network built from multiple paths and interference, to control and enhance light-matter interaction via light localisation. The network is built from a mesh of subwavelength waveguides, and can sustain localised modes and mirror-less light trapping stemming from interference over hundreds of nodes. With optical gain, these modes can easily lase, reaching $\sim$100 pm linewidths. We introduce a graph solution to the Maxwell's equation which describes light on the network, and predicts lasing action. In this framework, the network optical modes can be designed via the network connectivity and topology, and lasing can be tailored and enhanced by the network shape. Nanophotonic networks pave the way for new laser device architectures, which can be used for sensitive biosensing and on-chip optical information processing.

We investigate the effects of nanoparticles on the onset of varicose and whipping instabilities in the dynamics of electrified jets. In particular, we show that the non-linear interplay between the mass of the nanoparticles and electrostatic instabilities, gives rise to qualitative changes of the dynamic morphology of the jet, which in turn, drastically affect the final deposition pattern in electrospinning experiments. It is also shown that even a tiny amount of excess mass, of the order of a few percent, may more than double the radius of the electrospun fiber, with substantial implications for the design of experiments involving electrified jets as well as spun organic fibers., Comment: 8 pages, 7 figures, 1 table

Complex assemblies of light-emitting polymer nanofibers with molecular materials exhibiting optical gain can lead to important advance to amorphous photonics and to random laser science and devices. In disordered mats of nanofibers, multiple scattering and waveguiding might interplay to determine localization or spreading of optical modes as well as correlation effects. Here we study electrospun fibers embedding a lasing fluorene-carbazole-fluorene molecule and doped with titania nanoparticles, which exhibit random lasing with sub-nm spectral width and threshold of about 9 mJ cm^-2 for the absorbed excitation fluence. We focus on the spatial and spectral behavior of optical modes in the disordered and non-woven networks, finding evidence for the presence of modes with very large spatial extent, up to the 100 micrometer-scale. These findings suggest emission coupling into integrated nanofiber transmission channels as effective mechanism for enhancing spectral selectivity in random lasers and correlations of light modes in the complex and disordered material., Comment: 22 pages, 6 figures

Electromechanical coupling through piezoelectric polymer chains allows the emission of organic molecules in active nanowires to be tuned. This effect is evidenced by highly bendable arrays of counter-ion dye-doped nanowires made of a poly(vinylidenefluoride) copolymer. A reversible redshift of the dye emission is found upon the application of dynamic stress during highly accurate bending experiments. By density functional theory calculations it is found that these photophysical properties are associated with mechanical stresses applied to electrostatically interacting molecular systems, namely to counterion-mediated states that involve light-emitting molecules as well as charged regions of piezoelectric polymer chains. These systems are an electrostatic class of supramolecular functional stress-sensitive units, which might impart new functionalities in hybrid molecular nanosystems and anisotropic nanostructures for sensing devices and soft robotics., Comment: 32 pages, 18 figures

We present a lattice Boltzmann model for charged leaky dielectric multiphase fluids in the context of electrified jet simulations, which are of interest for a number of production technologies including electrospinning. The role of non-linear rheology on the dynamics of electrified jets is considered by exploiting the Carreau model for pseudoplastic fluids. We report exploratory simulations of charged droplets at rest and under a constant electric field, and we provide results for charged jet formation under electrospinning conditions., Comment: 29 pages, 10 figures, 1 table

Conjugated polymers are complex multi-chromophore systems, with emission properties strongly dependent on the electronic energy transfer through active sub-units. Although the packing of the conjugated chains in the solid state is known to be a key factor to tailor the electronic energy transfer and the resulting optical properties, most of the current solution-based processing methods do not allow for effectively controlling the molecular order, thus making the full unveiling of energy transfer mechanisms very complex. Here we report on conjugated polymer fibers with tailored internal molecular order, leading to a significant enhancement of the emission quantum yield. Steady state and femtosecond time-resolved polarized spectroscopies evidence that excitation is directed toward those chromophores oriented along the fiber axis, on a typical timescale of picoseconds. These aligned and more extended chromophores, resulting from the high stretching rate and electric field applied during the fiber spinning process, lead to improved emission properties. Conjugated polymer fibers are relevant to develop optoelectronic plastic devices with enhanced and anisotropic properties., Comment: 43 pages, 15 figures, 1 table in Journal of the American Chemical Society, (2016)

Electrospinning is a nanotechnology process whereby an external electric field is used to accelerate and stretch a charged polymer jet, so as to produce fibers with nanoscale diameters. In quest of a further reduction in the cross section of electrified jets hence of a better control on the morphology of the resulting electrospun fibers, we explore the effects of an external rotating electric field orthogonal to the jet direction. Through extensive particle simulations, it is shown that by a proper tuning of the electric field amplitude and frequency, a reduction of up to a $30 \%$ in the aforementioned radius can be obtained, thereby opening new perspectives in the design of future ultra-thin electrospun fibres. Applications can be envisaged in the fields of nanophotonic components as well as for designing new and improved filtration materials., Comment: 22 pages, 8 figures

The intrinsic flexible character of polymeric materials also causes remarkable strain deformations along directions perpendicular to the applied stress. Here the biaxial response in the shear piezoelectricity of polyvinylidenefluoride copolymers is analyzed and their full piezoelectric tensors are provided. The microscopic shear is exploited in single suspended nanowires bent by localized loading to couple flexural deformation and transverse piezoelectric response., Comment: 36 pages, 10 figures, 2 tables, 49 references, Advanced Materials, 2016

We study the effects of a controlled gas flow on the dynamics of electrified jets in the electrospinning process. The main idea is to model the air drag effects of the gas flow by using a non-linear Langevin-like approach. The model is employed to investigate the dynamics of electrified polymer jets at different conditions of air drag force, showing that a controlled gas counterflow can lead to a decrease of the average diameter of electrospun fibers, and potentially to an improvement of the quality of electrospun products. We probe the influence of air drag effects on the bending instabilities of the jet and on its angular fluctuations during the process. The insights provided by this study might prove useful for the design of future electrospinning experiments and polymer nanofiber materials., Comment: 16 pages, 8 figures in J. Phys. Chem. A, Article ASAP, 2016

Efficient manipulation and long distance transport of single-photons is a key component in nanoscale quantum optics. In this letter, we study the emission properties of an individual light emitter placed into a nanofiber and coupled to a metallic nanoparticle. We find that plasmonic field enhancement together with the nanofiber optical confinement uniquely and synergistically contribute to an overall increase of emission rates as well as quantum yields.

Nowadays, several models of unidimensional fluid jets exploit discrete element methods. In some cases, as for models aiming at describing the electrospinning nanofabrication process of polymer fibers, discrete element methods suffer a non constant resolution of the jet representation. We develop a dynamic mesh-refinement method for the numerical study of the electro-hydrodynamic behavior of charged jets using discrete element methods. To this purpose, we import ideas and techniques from the string method originally developed in the framework of free-energy landscape simulations. The mesh-refined discrete element method is demonstrated for the case of electrospinning applications., Comment: 16 pages, 7 figures in Journal of Computational Science, 2016

A fundamental issue in biomedical and environmental sciences is the development of sensitive and robust sensors able to probe the analyte of interest, under physiological and pathological conditions or in environmental samples, and with very high spatial resolution. In this work, novel hybrid organic fibers that can effectively report the analyte concentration within the local microenvironment are reported. The nanostructured and flexible wires are prepared by embedding fluorescent pH sensors based on seminaphtho-rhodafluor-1-dextran conjugate. By adjusting capsule/polymer ratio and spinning conditions, the diameter of the fibers and the alignment of the reporting capsules are both tuned. The hybrid wires display excellent stability, high sensitivity, as well as reversible response, and their operation relies on effective diffusional kinetic coupling of the sensing regions and the embedding polymer matrix. These devices are believed to be a powerful new sensing platform for clinical diagnostics, bioassays and environmental monitoring., Comment: 32 pages, 14 figures, Small, 2015

Electrospinning in controlled nitrogen atmosphere is developed for the realization of active polymer nanofibers. Fibers electrospun under controlled atmospheric conditions are found to be smoother and more uniform than samples realized by conventional electrospinning processes performed in air. In addition, they exhibit peculiar composition, incorporating a greatly reduced oxygen content during manufacturing, which favors enhanced optical properties and increases emission quantum yield. Active waveguides with optical losses coefficients lowered by ten times with respect to fibers spun in air are demonstrated through this method. These findings make the process very promising for the highly-controlled production of active polymer nanostructures for photonics, electronics and sensing., Comment: 26 pages, 11 figures

The use of UV light sources is highly relevant in many fields of science, being directly related to all those detection and diagnosis procedures which are based on fluorescence spectroscopy. Depending on the specific application, UV light-emitting materials are desired to feature a number of opto-mechanical properties, including brightness, optical gain for being used in laser devices, flexibility to conform with different lab-on-chip architectures, and tailorable wettability to control and minimize their interaction with ambient humidity and fluids. In this work, we introduce multifunctional, UV-emitting electrospun fibers with both optical gain and anisotropic hydrophobicity greatly enhanced compared to films. Fibers are described by the onset of a composite wetting state and their arrangement in uniaxial arrays further favours liquid directional control. The low gain threshold and optical losses, the plastic nature and the flexibility and stability of these UV-emitting fibers make them interesting for building light-emitting devices and microlasers. Furthermore, the found anisotropic hydrophobicity is strongly synergic with optical properties, reducing interfacial interactions with liquids and enabling smart functional surfaces for droplet microfluidic and wearable applications., Comment: 25 pages, 11 figures

In metal-enhanced fluorescence (MEF), the localized surface plasmon resonances of metallic nanostructures amplify the absorption of excitation light and assist in radiating the consequent fluorescence of nearby molecules to the far-field. This effect is at the base of various technologies that have strong impact on fields such as optics, medical diagnostics and biotechnology. Among possible emission bands, those in the near-infrared (NIR) are particularly intriguing and widely used in proteomics and genomics due to its noninvasive character for biomolecules, living cells, and tissues, which greatly motivates the development of effective, and eventually multifunctional NIR-MEF platforms. Here we demonstrate NIR-MEF substrates based on Au nanocages micropatterned with a tight spatial control. The dependence of the fluorescence enhancement on the distance between the nanocage and the radiating dipoles is investigated experimentally and modeled by taking into account the local electric field enhancement and the modified radiation and absorption rates of the emitting molecules. At a distance around 80 nm, a maximum enhancement up to 2-7 times with respect to the emission from pristine dyes (in the region 660 nm-740 nm) is estimated for films and electrospun nanofibers. Due to their chemical stability, finely tunable plasmon resonances, and large light absorption cross sections, Au nanocages are ideal NIR-MEF agents. When these properties are integrated with the hollow interior and controllable surface porosity, it is feasible to develop a nanoscale system for targeted drug delivery with the diagnostic information encoded in the fluorophore., Comment: 41 pages, 18 figures

We present the open-source computer program JETSPIN, specifically designed to simulate the electrospinning process of nanofibers. Its capabilities are shown with proper reference to the underlying model, as well as a description of the relevant input variables and associated test-case simulations. The various interactions included in the electrospinning model implemented in JETSPIN are discussed in detail. The code is designed to exploit different computational architectures, from single to parallel processor workstations. This paper provides an overview of JETSPIN, focusing primarily on its structure, parallel implementations, functionality, performance, and availability., Comment: 22 pages, 11 figures. arXiv admin note: substantial text overlap with arXiv:1507.07015

Nanoscale generation of individual photons in confined geometries is an exciting research field aiming at exploiting localized electromagnetic fields for light manipulation. One of the outstanding challenges of photonic systems combining emitters with nanostructured media is the selective channelling of photons emitted by embedded sources into specific optical modes and their transport at distant locations in integrated systems. Here, we show that soft-matter nanofibers, electrospun with embedded emitters, combine subwavelength field localization and large broadband near-field coupling with low propagation losses. By momentum spectroscopy, we quantify the modal coupling efficiency identifying the regime of single-mode coupling. These nanofibers do not rely on resonant interactions, making them ideal for room-temperature operation, and offer a scalable platform for future quantum information technology.