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Nanoporous carbon materials containing small domains of sp2-carbon with highly disordered structures are promising for supercapacitor applications. Herein, we synthesize amorphous carbon nanofoam with 98% volumetric void fraction and low mass density of around 30 mg/cm3 by pulsed laser deposition at room temperature. With the unavoidable oxygen functional groups on the nanoporous surface, pristine and nitrogen-functionalized carbon nanofoams are directly grown on the desired substrate under background gas of Ar, N2 and N2-H2employed as supercapacitor electrodes. Among the background gases used in synthesis, the use of nitrogen yields nanofoam with higher thickness and more N-content with higher graphitic-N, which is correlated with plasma plume behaviour. From the test of amorphous carbon nanofoam supercapacitor device, nitrogenated amorphous carbon show a higher areal capacitance of 4.1 mF/cm2 at 20 mV/s in aqueous electrolyte, a better capacitance retention at higher current, and excellent cycle stability (98%) over prolonged 10000 charge-discharge cycles are achieved for compared to pristine counterpart prepared under Ar background gas (2.7 mF/cm2 and cycle stability of 88%)., Comment: 14 pages main article, 2 pages supporting material, 5 figures, 3 supporting figures, 1 table

Carbon atomic wires, a linear atomic chain of sp-carbon, is theoretically predicted to have around five times higher surface area than graphene, notable charge mobilities, as well as excellent optical and thermal properties. Despite these impressive properties, the properties of sp-carbon as an electrochemical energy-storage electrode have not been reported so far. Herein, we prepare solution processed thin films of tetraphenyl[3]cumulenic sp-carbon atomic wires embedded in a polymer matrix, in which sp-carbon atomic wires feature three cumulated carbon-carbon double bonds terminated at each end by two phenyl groups. Raman and UV-visible spectroscopy are used to confirm the presence and possible degradation of sp-carbons inside the polymeric matrix. Finally, we investigate the supercapacitor performance of cumulenic sp-carbon atomic wires embedded polymer in three aqueous mediums, namely 1M Na2SO4 (neutral), 1M H2SO4 (acidic), and 6M KOH (basic). The results suggest 6M KOH is the best electrolyte to obtain high charge-storage performance of device with areal capacitance of 2.4 mF/cm2 at 20 mV/s, 85% cycle stability after 10000 charge-discharge cycles, and excellent frequency response., Comment: 15 pages, 2 supplementary pages, 5 figures, 2 supporting figures

Carbyne, an infinite linear chain of carbon atoms, is the truly one-dimensional allotrope of carbon. While ideal carbyne and its fundamental properties have remained elusive, carbyne-like materials like carbyne chains confined inside carbon nanotubes are available for study. Here, we probe the longitudinal optical phonon (C-mode) of confined carbyne chains by Raman spectroscopy up to the third overtone. We observe a strong vibrational anharmonicity that increases with decreasing C-mode frequency, reaching up to 8% for the third overtone. Moreover, we find that the relation between vibrational anharmonicity and C-mode frequency is universal to carbyne-like materials, including ideal carbyne. This establishes experimentally that carbyne and related materials have pronounced anharmonic potential landscapes which must be included in the theoretical description of their structure and properties.

Advanced material composite of nanocarbons and metal-based materials provides a synergistic effect to obtain excellent electrochemical charge-storage performance and other properties. Herein, 3D porous carbon-metal oxynitride nanocomposites with tunable carbon/metal and oxygen/nitrogen ratio are synthesized uniquely by simultaneous ablation from two different targets by single-step pulsed laser deposition at room temperature. Co-ablation of titanium and vanadium nitride targets together with graphite allowed us to synthesize carbon-metal oxynitride porous nanocomposite and exploit them as a binder-free thin film supercapacitor electrode in aqueous electrolyte. We show that the elemental composition ratio and hence the structural properties can be tuned by selecting target configuration and by manipulating the ablation position. We investigate how this tuning capability impacts their charge-storage performances. We anticipate the utilization of as-synthesized various composites in a single PLD production run as next-generation active materials for flexible energy storage and optoelectronic applications., Comment: 18 pages, 8 Figures, 1 table, 9 figures in supplementary figures

In pulsed laser deposition, along the traditionally exploited deposition on the front-side of the plasma-plume, a coating forms on the surface of the target as well. For reproducibility, this residue is usually cleaned and discarded. Here we instead investigate the target-side coated materials and employ them as a binder-free supercapacitor electrode. The ballistic-aggregated, target-side nanofoam is compact and features a larger fraction of sp2-carbon, higher nitrogen content with higher graphitic-N and lower oxygen content with fewer COOH groups than that of diffusive-aggregated conventional nanofoams. They are highly hydrogenated graphite-like amorphous carbon and superhydrophilic. The resulting symmetric micro-supercapacitor delivers higher volumetric capacitance of 522 mF/cm3 at 100 mV/s and 104% retention after 10000 charge-discharge cycles over conventional nanofoam (215 mF/cm3 and 85% retention) with an areal capacitance of 134 {\mu}F/cm2 at 120 Hz and ultrafast frequency response. Utilizing the normally discarded target-side material can therefore enable high performing devices while reducing waste, cost and energy input per usable product. leading towards a greater sustainability on nanomaterials synthesis and deposition techniques., Comment: 22 pages, 8 figures in text, 8 figures in supplementary, 1 table

The quest for safer and more efficient transportation through cooperative, connected and automated mobility (CCAM) calls for realistic performance analysis tools, especially with respect to wireless communications. While the simulation of existing and emerging communication technologies is an option, the most realistic results can be obtained by employing real hardware, as done for example in field operational tests (FOTs). For CCAM, however, performing FOTs requires vehicles, which are generally expensive. and performing such tests can be very demanding in terms of manpower, let alone considering safety issues. Mobility simulation with hardware-in-the-loop (HIL) serves as a middle ground, but current solutions lack flexibility and reconfigurability. This work thus proposes ColosSUMO as a way to couple Colosseum, the world's largest wireless network emulator, with the SUMO mobility simulator, showing its design concept, how it can be exploited to simulate realistic vehicular environments, and its flexibility in terms of communication technologies.

Graphdiyne-based carbon systems generate intriguing layered sp-sp$^2$ organometallic lattices, characterized by flexible acetylenic groups connecting planar carbon units through metal centers. At their thinnest limit, they can result in two-dimensional (2D) organometallic networks exhibiting unique quantum properties and even confining the surface states of the substrate, which is of great importance for fundamental studies. In this work, we present the on-surface synthesis of a highly crystalline 2D organometallic network grown on Ag(111). The electronic structure of this mixed honeycomb-kagome arrangement - investigated by angle-resolved photoemission spectroscopy and scanning tunneling spectroscopy - reveals a strong electronic conjugation within the network, leading to the formation of two intense electronic band-manifolds. In comparison to theoretical density functional theory calculations, we observe that these bands exhibit a well-defined orbital character that can be associated with distinct regions of the sp-sp$^2$ monomers. Moreover, we find that the halogen by-products resulting from the network formation locally affect the pore-confined states, causing a significant energy shift. This work contributes to the understanding of the growth and electronic structure of graphdiyne-like 2D networks, providing insights into the development of novel carbon materials beyond graphene with tailored properties., Comment: 11 pages, 4 figures + supporting information (5 pages, 10 figures)

Invisible labor is work that is either not fully visible or not appropriately compensated. In open source software (OSS) ecosystems, essential tasks that do not involve code (like content moderation) often become invisible to the detriment of individuals and organizations. However, invisible labor is sufficiently difficult to measure that we do not know how much of OSS activities are invisible. Our study addresses this challenge, demonstrating that roughly half of OSS work is invisible. We do this by developing a cognitive anchoring survey technique that measures OSS developer self-assessments of labor visibility and attribution. Survey respondents (n=142) reported that their work is more likely to be invisible (2 in 3 tasks) than visible, and that half (50.1%) is uncompensated. Priming participants with the idea of visibility caused participants to think their work was more visible, and that visibility was less important, than those primed with invisibility. We also found evidence that tensions between attribution motivations probably increase how common invisible labor is. This suggests that advertising OSS activities as "open" may lead contributors to overestimate how visible their labor actually is. Our findings suggest benefits to working with varied stakeholders to make select, collectively valued activities visible, and increasing compensation in valued forms (like attribution, opportunities, or pay) when possible. This could improve fairness in software development while providing greater transparency into work designs that help organizations and communities achieve their goals., Comment: 31 pages, 7 figures, 1 table

The quasi-optical propagation of millimeter-wave signals enables high-accuracy localization algorithms that employ geometric approaches or machine learning models. However, most algorithms require information on the indoor environment, may entail the collection of large training datasets, or bear an infeasible computational burden for commercial off-the-shelf (COTS) devices. In this work, we propose to use tiny neural networks (NNs) to learn the relationship between angle difference-of-arrival (ADoA) measurements and locations of a receiver in an indoor environment. To relieve training data collection efforts, we resort to a self-supervised approach by bootstrapping the training of our neural network through location estimates obtained from a state-of-the-art localization algorithm. We evaluate our scheme via mmWave measurements from indoor 60-GHz double-directional channel sounding. We process the measurements to yield dominant multipath components, use the corresponding angles to compute ADoA values, and finally obtain location fixes. Results show that the tiny NN achieves sub-meter errors in 74% of the cases, thus performing as good as or even better than the state-of-the-art algorithm, with significantly lower computational complexity., Comment: 13 pages, 12 figures

In the last years, transition metal dichalcogenides (TMDs), especially at the two-dimensional (2D) limit, gained a large interest due to their unique optical and electronic properties. Among them, MoS2 received great attention from the scientific community due to its versatility, workability, and applicability in a large number of fields such as electronics, optoelectronics and electrocatalysis. To open the possibility of 2D-MoS2 exploitation, its synthesis over large macroscopic areas using cost-effective methods is fundamental. In this study, we report a method for the synthesis of large-area (~ cm2) few-layers MoS2 via liquid precursor CVD (L-CVD), where the Mo precursor (i.e. ammonium heptamolybdate AHM) is provided via a solution that is spin-coated over the substrate. Given the capability of organic and inorganic molecules, such as alkaline salts, to enhance MoS2 growth, we investigated the action of different inorganic salts as seed promoters. In particular, by using visible Raman spectroscopy, we focused on the effect of Na(OH), KCl, KI, and Li(OH) on the thickness, morphology, uniformity and degree of coverage of the grown MoS2. We optimized the process tuning parameters such as the volume of spin-coated solution, the growth temperature, and the seed promoter concentration, to synthesise the lowest possible thickness which resulted to be 2 layers (2L) of the highest quality. We witnessed that the addition of an inorganic seed promoter in the solution improves the extension of the grown MoS2 promoting lateral growth front, and therefore the degree of coverage. From this study, we conclude that, amongst the investigated seed promoters, K-based salts proved to grant the growth of high-quality two-layer MoS2 with optimal and uniform coverage of the SiO2/Si substrate surface.

The interest in tellurium nanostructures is on the rise due to their outstanding physical properties including high carrier mobility, anisotropic charge conduction, photoconductivity, thermoelectricity, and piezoelectricity. Applications in related technologies require tailoring the synthesis of tellurium from its preferred vertical growth toward the lateral growth. Here, the synthesis of pillar-like and pennette-like structures of tellurium through a powder vapor deposition technique has been discussed. It has been shown that exploiting salt additives such as NaCl in vapor deposition technique can enhance tellurium pillar dimensionality toward large planar grains. Further, we report on the synthesis of hexagonal ultrathin tellurium nanoflakes, namely tellurene, from few-layer to monolayer thickness by optimizing the growth kinetics without the usage of any additives. In addition, we explore the surface quality and physical properties of as-grown two-dimensional (2D) tellurium, using a variety of characterization techniques, including Raman spectroscopy, scanning electron microscopy, atomic force microscopy, and Kelvin probe force microscopy. This study provides a pivotal scheme for enabling scalable 2D tellurium integration in numerous potential applications for electronics and optoelectronic devices., Comment: 17 pages, 13 figures

One-dimensional (1D) linear nanostructures comprising sp-hybridized carbon atoms, as derivatives of the prototypical allotrope known as carbyne, are predicted to possess outstanding mechanical, thermal, and electronic properties. Despite recent advances in the synthesis, their chemical and physical properties are still poorly understood. Here, we investigate the photophysics of a prototypical polyyne (i.e., 1D chain with alternating single and triple carbon bonds), as the simplest model of finite carbon wire and as a prototype of sp-carbon-based chains. We perform transient absorption experiments with high temporal resolution (<30 fs) on monodispersed hydrogen-capped hexayne H$-$(C$\equiv$C)$_6-$H synthesized by laser ablation in liquid. With the support of detailed computational studies based on ground state density functional theory (DFT) and excited state time-dependent (TD)-DFT calculations, we provide a comprehensive description of the excited state relaxation processes at early times following photoexcitation. We show that the internal conversion from a bright high-energy singlet excited state to a low-lying singlet dark state is ultrafast and takes place with a 200-fs time constant, followed by thermalization on the picosecond timescale and decay of the low-energy singlet state with hundreds of picoseconds time constant. We also show that the timescale of these processes does not depend on the end groups capping the sp-carbon chain. The understanding of the primary photo-induced events in polyynes is of key importance both for fundamental knowledge and for potential optoelectronic and light-harvesting applications of low dimensional nanostructured carbon-based materials., Comment: 24 pages, 6 figures

Millimeter wave (mmWave) radar sensors are emerging as valid alternatives to cameras for the pervasive contactless monitoring of people in indoor spaces. However, commercial mmWave radars feature a limited range (up to $6$-$8$ m) and are subject to occlusion, which may constitute a significant drawback in large, crowded rooms characterized by a challenging multipath environment. Thus, covering large indoor spaces requires multiple radars with known relative position and orientation and algorithms to combine their outputs. In this work, we present ORACLE, an autonomous system that (i) integrates automatic relative position and orientation estimation from multiple radar devices by exploiting the trajectories of people moving freely in the radars' common fields of view, and (ii) fuses the tracking information from multiple radars to obtain a unified tracking among all sensors. Our implementation and experimental evaluation of ORACLE results in median errors of $0.12$ m and $0.03^\circ$ for radars location and orientation estimates, respectively. Fused tracking improves the mean target tracking accuracy by $27\%$, and the mean tracking error is $23$ cm in the most challenging case of $3$ moving targets. Finally, ORACLE does not show significant performance reduction when the fusion rate is reduced to up to 1/5 of the frame rate of the single radar sensors, thus being amenable to a lightweight implementation on a resource-constrained fusion center.

We propose a technique to authenticate received packets in underwater acoustic networks based on the physical layer features of the underwater acoustic channel (UWAC). Several sensors a) locally estimate features (e.g., the number of taps or the delay spread) of the UWAC over which the packet is received, b) obtain a compressed feature representation through a neural network (NN), and c) transmit their representations to a central sink node that, using a NN, decides whether the packet has been transmitted by the legitimate node or by an impersonating attacker. Although the purpose of the system is to make a binary decision as to whether a packet is authentic or not, we show the importance of having a rich set of compressed features, while still taking into account transmission rate limits among the nodes. We consider both global training, where all NNs are trained together, and local training, where each NN is trained individually. For the latter scenario, several alternatives for the NN structure and loss function were used for training., Comment: Conference paper accepted to UCOMMS22

Polyynes are linear carbon chains characterized by alternated single and triple bonds and terminated by hydrogen or other terminal substituents. They can be synthesized by pulsed laser ablation in liquid (PLAL) as a scalable, cost-effective, and fast physical technique. Water can be employed as a solvent for PLAL to avoid toxicity problems and to reduce costs compared to organic solvents. However, in this case, the production yield of polyynes reached is extremely low and prevents further characterization and implementation in new functional materials. In this work, we synthesized polyynes by pulsed laser ablation in water and we optimized the process parameters to improve the yield of polyynes by PLAL. Then, we developed a procedure entirely based on reversed-phase high-performance liquid chromatography (RP-HPLC) which effectively enables the concentration, separation and collection of polyynes according to their length. Since the polyynes sample is an aqueous solution, we could inject it directly into the RP-HPLC column without the dilution step required in the case of a sample in an organic solvent. Thanks to our single RP-HPLC procedure, it is possible to highly increase the concentration and separately characterize different size-selected polyynes for further use in functional materials., Comment: 8 pages, 4 figures

This review provides a discussion of the current state of research on sp-carbon chains synthesized by pulsed laser ablation in liquid. In recent years, pulsed laser ablation in liquid (PLAL) has been widely employed for polyynes synthesis thanks to its flexibility with varying laser parameters, solvents, and targets. This allows the control of sp-carbon chains properties as yield, length, termination and stability. Although many reviews related to PLAL have been published, a comprehensive work reporting the current status and advances related to the synthesis of sp-carbon chains by PLAL is still missing. Here we first review the principle of PLAL and the mechanisms of formation of sp-carbon chains. Then we discuss the role of laser fluence (i.e. energy density), solvent, and target for sp-carbon chains synthesis. Lastly, we report the progress related to the prolonged stability of sp-carbon chains by PLAL encapsulated in polymeric matrices. This review will be a helpful guide for researchers interested in synthesizing sp-carbon chains by PLAL.

Communication surrounding the development of an open source project largely occurs outside the software repository itself. Historically, large communities often used a collection of mailing lists to discuss the different aspects of their projects. Multimodal tool use, with software development and communication happening on different channels, complicates the study of open source projects as a sociotechnical system. Here, we combine and standardize mailing lists of the Python community, resulting in 954,287 messages from 1995 to the present. We share all scraping and cleaning code to facilitate reproduction of this work, as well as smaller datasets for the Golang (122,721 messages), Angular (20,041 messages) and Node.js (12,514 messages) communities. To showcase the usefulness of these data, we focus on the CPython repository and merge the technical layer (which GitHub account works on what file and with whom) with the social layer (messages from unique email addresses) by identifying 33% of GitHub contributors in the mailing list data. We then explore correlations between the valence of social messaging and the structure of the collaboration network. We discuss how these data provide a laboratory to test theories from standard organizational science in large open source projects., Comment: Accepted for the 19th International Conference on Mining Software Repositories (MSR '22), May 23--24, 2022, Pittsburgh, PA, USA

Two-dimensional (2D) hybrid sp-sp2 carbon systems are an appealing subject for science and technology. For these materials, topology and structure significantly affect electronic and vibrational properties. We investigate here by periodic density-functional theory (DFT) calculations we here investigate the Raman and IR spectra of 2D carbon crystals belonging to the family of graphdiynes (GDYs) and having different structures and topologies. By joining DFT calculations with symmetry analysis, we assign the IR and Raman modes in the spectra of all the investigated systems. On this basis, we discuss how the modulation of the Raman and IR active bands depends on the different interactions between sp and sp2 domains. The symmetry-based classification allows identifying the marker bands sensitive to the different peculiar topologies. These results show the effectiveness of vibrational spectroscopy for the characterization of new nanostructures, deepening the knowledge of the subtle interactions that take place in these 2D materials.

Hybrid sp-sp2 structures can be efficiently obtained on metal substrates via on-surface synthesis. The choice of both the precursor and of the substrate impacts on the effectiveness of the process and the stability of the formed structures. Here we demonstrate that using anthracene-based molecules as precursor, the formation on Au(111) of polymers hosting sp carbon chains is affected by the steric hindrance between aromatic groups. In particular, by scanning tunneling microscopy and density functional theory calculations we show that the de-metalation of organometallic structures induces a lateral separation of adjacent polymers preventing the formation of ordered domains.

Solution-processed, large-area, and flexible electronics largely relies on the excellent electronic properties of sp$^2$-hybridized carbon molecules, either in the form of $\pi$-conjugated small molecules and polymers or graphene and carbon nanotubes. Carbon with sp-hybridization, the foundation of the elusive allotrope carbyne, offers vast opportunities for functionalized molecules in the form of linear carbon atomic wires (CAWs), with intriguing and even superior predicted electronic properties. While CAWs represent a vibrant field of research, to date, they have only been applied sparingly to molecular devices. The recent observation of the field-effect in microcrystalline cumulenes suggests their potential applications in solution-processed thin-film transistors but concerns surrounding the stability and electronic performance have precluded developments in this direction. In the present study, ideal field-effect characteristics are demonstrated for solution-processed thin films of tetraphenyl[3]cumulene, the shortest semiconducting CAW. Films are deposited through a scalable, large-area, meniscus-coating technique, providing transistors with hole mobilities in excess of 0.1 cm$^2$ V$^{-1}$ s$^{-1}$, as well as promising operational stability under dark conditions. These results offer a solid foundation for the exploitation of a vast class of molecular semiconductors for organic electronics based on sp-hybridized carbon systems and create a previously unexplored paradigm.

As renewable energy is becoming a critical energy source to meet the global demand, electrochemical energy storage devices become indispensable for the efficient energy storage and reliable supply. The electrode material is the key factor determining the energy storage capacity and the power delivery of the devices. Carbon-based materials are emerging as a viable candidate for electrodes, yet their low energy densities impede the development of advanced energy storage materials. Nanoparticle decoration of the carbon structures is one of the most promising and easy-to-implement a strategy to enhance the charge-storage performance of carbon-based electrodes. Decoration by nanoparticles of metals, metal oxides, nitrides, carbides, phosphides, chalcogenides, and bimetallic components lead to significant enhancements in the structural and electronic properties, pore refinement, charge storage, and charge transfer kinetics of both pristine and doped carbon structures, thereby making their performance promising for next-generation energy storage devices. This review covers the state-of-art nanoparticle decorated nanocarbons for battery, supercapacitor, and metal-ion capacitor applications. A critical analysis of the elemental composition, structure, associated physico-chemical properties and performance relationships of nanoparticle-decorated nanocarbon electrodes is provided as well to inform the future development of the next generation of advanced energy storage materials, devices, and systems., Comment: 67 pages, 17 figures, 5 tables

The commercial availability of low-cost millimeter wave (mmWave) communication and radar devices is starting to improve the penetration of such technologies in consumer markets, paving the way for large-scale and dense deployments in fifth-generation (5G)-and-beyond as well as 6G networks. At the same time, pervasive mmWave access will enable device localization and device-free sensing with unprecedented accuracy, especially with respect to sub-6 GHz commercial-grade devices. This paper surveys the state of the art in device-based localization and device-free sensing using mmWave communication and radar devices, with a focus on indoor deployments. We first overview key concepts about mmWave signal propagation and system design. Then, we provide a detailed account of approaches and algorithms for localization and sensing enabled by mmWaves. We consider several dimensions in our analysis, including the main objectives, techniques, and performance of each work, whether each research reached some degree of implementation, and which hardware platforms were used for this purpose. We conclude by discussing that better algorithms for consumer-grade devices, data fusion methods for dense deployments, as well as an educated application of machine learning methods are promising, relevant and timely research directions., Comment: 43 pages, 13 figures. Accepted in IEEE Communications Surveys & Tutorials (IEEE COMST)

Millimeter wave (mmWave) localization algorithms exploit the quasi-optical propagation of mmWave signals, which yields sparse angular spectra at the receiver. Geometric approaches to angle-based localization typically require to know the map of the environment and the location of the access points. Thus, several works have resorted to automated learning in order to infer a device's location from the properties of the received mmWave signals. However, collecting training data for such models is a significant burden. In this work, we propose a shallow neural network model to localize mmWave devices indoors. This model requires significantly fewer weights than those proposed in the literature. Therefore, it is amenable for implementation in resource-constrained hardware, and needs fewer training samples to converge. We also propose to relieve training data collection efforts by retrieving (inherently imperfect) location estimates from geometry-based mmWave localization algorithms. Even in this case, our results show that the proposed neural networks perform as good as or better than state-of-the-art algorithms., Comment: 6 pages, 9 figures. The paper was accepted at IEEE WCNC 2022