Fractal superconducting nanowire single-photon detectors working in dual bands and their applications in free-space and underwater hybrid LIDAR.

We demonstrate a fiber-coupled fractal superconducting nanowire single-photon detector (SNSPD) system with minimum polarization dependence of detection efficiency. Its system detection efficiency (SDE) was maximized at the wavelength of 1540 nm, which was measured to be 91 ± 4%; furthermore, we observed the second local maximum of SDE at the wavelength of 520 nm, which was measured to be 61 ± 2%. This dual-band feature of SDE was due to the enhancement of the optical absorptance by two longitudinal resonance modes of the micro-cavity. By using high SDE with minimum polarization dependence in these two bands, we implemented a hybrid LIDAR for imaging the remote objects in free space and under water.

Nanosecond gating of superconducting nanowire single-photon detectors using cryogenic bias circuitry.

Superconducting nanowire single-photon detectors (SNSPDs) show near unity efficiency, low dark count rate, and short recovery time. Combining these characteristics with temporal control of SNSPDs broadens their applications as in active de-latching for higher dynamic range counting or temporal filtering for pump-probe spectroscopy or LiDAR. To that end, we demonstrate active gating of an SNSPD with a minimum off-to-on rise time of 2.4 ns and a total gate length of 5.0 ns. We show how the rise time depends on the inductance of the detector in combination with the control electronics. The gate window is demonstrated to be fully and freely, electrically tunable up to 500 ns at a repetition rate of 1.0 MHz, as well as ungated, free-running operation. Control electronics to generate the gating are mounted on the 2.3 K stage of a closed-cycle sorption cryostat, while the detector is operated on the cold stage at 0.8 K. We show that the efficiency and timing jitter of the detector is not altered during the on-time of the gating window. We exploit gated operation to demonstrate a method to increase in the photon counting dynamic range by a factor 11.2, as well as temporal filtering of a strong pump in an emulated pump-probe experiment.

Gas-phase synthesis of nanoparticles: current application challenges and instrumentation development responses.

Nanoparticles constitute fundamental building blocks required in several fields of application with current global importance. To fully exploit nanoparticle properties specifically determined by the size, shape, chemical composition and interfacial configuration, rigorous nanoparticle growth and deposition control is needed. Gas-phase synthesis, in particular magnetron-sputtering inert-gas condensation, provides unique opportunities to realise engineered nanoparticles optimised for the desired use case. Here, we provide an overview of recent nanoparticle growth experiments via this technique, how the latter can meet application-specific requirements, and what challenges might impede the wide-spread adoption for scalable industrial synthesis. More specifically, we discuss the timely topics of energy, catalysis, and sensing applications enabled by gas-phase synthesised nanoparticles, as well as recently emerging advances in neuromorphic devices for unconventional computing. Having identified the most relevant challenges and limiting factors, we outline how advances in nanoparticle source instrumentation and/or in situ diagnostics can address current shortcomings. Eventually we identify common trends and directions, giving our perspective on the most promising and impactful applications of gas-phase synthesised nanoparticles in the future.

Strain-Controlled Quantum Dot Fine Structure for Entangled Photon Generation at 1550 nm.

Entangled photon generation at 1550 nm in the telecom C-band is of critical importance as it enables the realization of quantum communication protocols over long distance using deployed telecommunication infrastructure. InAs epitaxial quantum dots have recently enabled on-demand generation of entangled photons in this wavelength range. However, time-dependent state evolution, caused by the fine-structure splitting, currently limits the fidelity to a specific entangled state. Here, we show fine-structure suppression for InAs quantum dots using micromachined piezoelectric actuators and demonstrate generation of highly entangled photons at 1550 nm. At the lowest fine-structure setting, we obtain a maximum fidelity of 90.0 ± 2.7% (concurrence of 87.5 ± 3.1%). The concurrence remains high also for moderate (weak) temporal filtering, with values close to 80% (50%), corresponding to 30% (80%) of collected photons, respectively. The presented fine-structure control opens the way for exploiting entangled photons from quantum dots in fiber-based quantum communication protocols.

Reconfigurable photonics with on-chip single-photon detectors.

Integrated quantum photonics offers a promising path to scale up quantum optics experiments by miniaturizing and stabilizing complex laboratory setups. Central elements of quantum integrated photonics are quantum emitters, memories, detectors, and reconfigurable photonic circuits. In particular, integrated detectors not only offer optical readout but, when interfaced with reconfigurable circuits, allow feedback and adaptive control, crucial for deterministic quantum teleportation, training of neural networks, and stabilization of complex circuits. However, the heat generated by thermally reconfigurable photonics is incompatible with heat-sensitive superconducting single-photon detectors, and thus their on-chip co-integration remains elusive. Here we show low-power microelectromechanical reconfiguration of integrated photonic circuits interfaced with superconducting single-photon detectors on the same chip. We demonstrate three key functionalities for photonic quantum technologies: 28 dB high-extinction routing of classical and quantum light, 90 dB high-dynamic range single-photon detection, and stabilization of optical excitation over 12 dB power variation. Our platform enables heat-load free reconfigurable linear optics and adaptive control, critical for quantum state preparation and quantum logic in large-scale quantum photonics applications.

In situ investigation of oxidation across a heterogeneous nanoparticle-support interface during metal support interactions.

Interactions between oxide supports and noble metal nanoparticles (NPs) is an area of intense research interest across all fields of catalysis. Oxygen spillover, metal support interactions (MSIs) and charge transfer are among many mechanisms observed and proposed as to how NP-support interfaces assist and enhance catalysis. This work studies the migration of oxygen across the Pd NP-CuO nanowire (NW) interface and beyond. X-ray photoelectron spectroscopy (XPS) and Kelvin probe force microscopy (KPFM) found an interaction between the Pd NP and CuO NW support, via the formation of PdO at the Pd-CuO interface. It was found, through in situ irradiation at high vacuum transmission electron microscopy (TEM), that oxygen enters the Pd NP lattice from the Pd-CuO interface via amorphization of the NP. Varying the amount of irradiation highlighted the different rates of amorphization of NPs, with full amorphization of a NP leading to the formation of an epitaxially driven PdO across the NPs. Interestingly, in situ heating in XPS observed a reduction to metallic Pd, found to be similarly amorphous during TEM investigation. On comparison with Pd supported on a non-reducible substrate - in which oxidation was found to proceed from the outer surface in, rather than the support interface (resulting in a PdO shell) - it is theorized that the oxidation and reduction of Pd on CuO forms a PdO NP surface full of Pd-PdO sites allowing for synergistic effects, of great use in the oxidation and hydrogenation of organic species.

On-Demand Generation of Entangled Photon Pairs in the Telecom C-Band with InAs Quantum Dots.

Entangled photons are an integral part in quantum optics experiments and a key resource in quantum imaging, quantum communication, and photonic quantum information processing. Making this resource available on-demand has been an ongoing scientific challenge with enormous progress in recent years. Of particular interest is the potential to transmit quantum information over long distances, making photons the only reliable flying qubit. Entangled photons at the telecom C-band could be directly launched into single-mode optical fibers, enabling worldwide quantum communication via existing telecommunication infrastructure. However, the on-demand generation of entangled photons at this desired wavelength window has been elusive. Here, we show a photon pair generation efficiency of 69.9 ± 3.6% in the telecom C-band by an InAs/GaAs semiconductor quantum dot on a metamorphic buffer layer. Using a robust phonon-assisted two-photon excitation scheme we measure a maximum concurrence of 91.4 ± 3.8% and a peak fidelity to the Φ+ state of 95.2 ± 1.1%, verifying on-demand generation of strongly entangled photon pairs and marking an important milestone for interfacing quantum light sources with our classical fiber networks.

Proximitized Josephson junctions in highly-doped InAs nanowires robust to optical illumination.

We have studied the effects of optical-frequency light on proximitized InAs/Al Josephson junctions based on highly n-doped InAs nanowires at varying incident photon flux and at three different photon wavelengths. The experimentally obtained IV curves were modeled using a resistively shunted junction model which takes scattering at the contact interfaces into account. Despite the fact that the InAs weak link is photosensitive, the Josephson junctions were found to be surprisingly robust, interacting with the incident radiation only through heating, whereas above the critical current our devices showed non-thermal effects resulting from photon exposure. Our work indicates that Josephson junctions based on highly-doped InAs nanowires can be integrated in close proximity to photonic circuits. The results also suggest that such junctions can be used for optical-frequency photon detection through thermal processes by measuring a shift in critical current.

Optimizing the stoichiometry of ultrathin NbTiN films for high-performance superconducting nanowire single-photon detectors.

The requirements in quantum optics experiments for high single-photon detection efficiency, low timing jitter, low dark count rate and short dead time have been fulfilled with the development of superconducting nanowire single-photon detectors. Although they offer a detection efficiency above 90%, achieving a high time resolution in devices made of amorphous materials is a challenge, particularly at temperatures above 0.8 K. Devices made from niobium nitride and niobium titanium nitride allow us to reach the best timing jitter but, in turn, have stronger requirements in terms of film quality to achieve a high efficiency. Here we take advantage of the flexibility of reactive co-sputter deposition to tailor the composition of NbxTi1-xN superconducting films and show that a Nb fraction of x = 0.62 allows for the fabrication of detectors from films as thick as 9 nm and covering an active area of 20 µm, with a wide detection saturation plateau at telecom wavelengths and in particular at 1550 nm. This is a signature of an internal detection efficiency saturation, achieved while maintaining the high time resolution associated with NbTiN and operation at 2.5K. With our optimized recipe, we reliably fabricated detectors with high critical current densities reaching a saturation plateau at 1550 nm with 80% system detection efficiency and with a FWHM timing jitter as low as 19.5 ps.

In Situ Observation of Metal to Metal Oxide Progression: A Study of Charge Transfer Phenomenon at Ru-CuO Interfaces.

Surface charge and charge transfer between nanoclusters and oxide supports are of paramount importance to catalysis, surface plasmonics, and optical energy harvesting areas. At present, high-energy X-rays and theoretical investigation are always required to determine the chemical state changes in the nanoclusters and the oxide supports, as well as the underlying transfer charge between them. This work presents the idea of using chrono-conductometric measurements to determine the chemical states of the Ru nanoclusters on CuO supports. Both icosahedral and single-crystal hexagonal close-packed Ru nanoclusters were deposited through gas-phase synthesis. To study the charge transfer phenomenon at the interface, a bias was applied to cupric oxide nanowires with metallic nanocluster decoration. In situ conductometric measurements were performed to observe the evolution of Ru into RuOx under heating conditions. Structural elucidation techniques such as transmission electron microscopy, X-ray photoelectron spectroscopy, and Kelvin probe force microscopy were employed to study the corresponding progression of structure, chemical ordering, and surface potential, respectively, as Ru(0) was oxidized to RuOx on the supporting oxide surface. Experimental and theoretical investigation of charge transfer between the nanocluster and oxide support highlighted the importance of metallic character and structure of the nanoclusters on the interfacial charge transfer, thus allowing the investigation of surface charge behavior on oxide-supported catalysts, in situ, during catalytic operation via conductometric measurements.

Site-Specific Wetting of Iron Nanocubes by Gold Atoms in Gas-Phase Synthesis.

A key challenge in nanotechnology is the rational design of multicomponent materials that beat the properties of their elemental counterparts. At the same time, when considering the material composition of such hybrid nanostructures and the fabrication process to obtain them, one should favor the use of nontoxic, abundant elements in view of the limited availability of critical metals and sustainability. Cluster beam deposition offers a solvent- and, therefore, effluent-free physical synthesis method to achieve nanomaterials with tailored characteristics. However, the simultaneous control of size, shape, and elemental distribution within a single nanoparticle in a small-size regime (sub-10 nm) is still a major challenge, equally limiting physical and chemical approaches. Here, a single-step nanoparticle fabrication method based on magnetron-sputtering inert-gas condensation is reported, which relies on selective wetting of specific surface sites on precondensed iron nanocubes by gold atoms. Using a newly developed Fe-Au interatomic potential, the growth mechanism is decomposed into a multistage model implemented in a molecular dynamics simulation framework. The importance of growth kinetics is emphasized through differences between structures obtained either experimentally or computationally, and thermodynamically favorable configurations determined via global optimization techniques. These results provide a roadmap for engineering complex nanoalloys toward targeted applications.

Nanoscale Heterogeneity of Multilayered Si Anodes with Embedded Nanoparticle Scaffolds for Li-Ion Batteries.

A new approach on the synthesis of Si anodes for Li-ion batteries is reported, combining advantages of both nanoparticulated and continuous Si films. A multilayered configuration prototype is proposed, comprising amorphous Si arranged in nanostructured, mechanically heterogeneous films, interspersed with Ta nanoparticle scaffolds. Particular structural features such as increased surface roughness, nanogranularity, and porosity are dictated by the nanoparticle scaffolds, boosting the lithiation process due to fast Li diffusion and low electrode polarization. Consequently, a remarkable charge/discharge speed is reached with the proposed anode, in the order of minutes (1200 mAh g-1 at 10 C). Moreover, nanomechanical heterogeneity self-limits the capacity at intermediate charge/discharge rates; as a consequence, exceptional cycleability is observed at 0.5 C, with 100% retention over 200 cycles with 700 mAh g-1. Higher capacity can be obtained when the first cycles are performed at 0.2 C, due to the formation of microislands, which facilitate the swelling of the active Si. This study indicates a method to tune the mechanical, morphological, and electrochemical properties of Si electrodes via engineering nanoparticle scaffolds, paving the way for a novel design of nanostructured Si electrodes for high-performance energy storage devices.

In situ chemoresistive sensing in the environmental TEM: probing functional devices and their nanoscale morphology.

In situ transmission electron microscopy provides exciting opportunities to address fundamental questions and technological aspects related to functional nanomaterials, including the structure-property relationships of miniaturized electronic devices. Herein, we report the in situ chemoresistive sensing in the environmental transmission electron microscope (TEM) with a single SnO2 nanowire device, studying the impact of surface functionalization with heterogeneous nanocatalysts. By detecting toxic carbon monoxide (CO) gas at ppm-level concentrations inside the microscope column, the sensing properties of a single SnO2 nanowire were characterized before and after decoration with hybrid Fe-Pd nanocubes. The structural changes of the supported nanoparticles induced by sensor operation were revealed, enabling direct correlation with CO sensing properties. Our novel approach is applicable for a broad range of functional nanomaterials and paves the way for future studies on the relationship between chemoresistive properties and nanoscale morphology.

Formation Mechanism of Fe Nanocubes by Magnetron Sputtering Inert Gas Condensation.

In this work, we study the formation mechanisms of iron nanoparticles (Fe NPs) grown by magnetron sputtering inert gas condensation and emphasize the decisive kinetics effects that give rise specifically to cubic morphologies. Our experimental results, as well as computer simulations carried out by two different methods, indicate that the cubic shape of Fe NPs is explained by basic differences in the kinetic growth modes of {100} and {110} surfaces rather than surface formation energetics. Both our experimental and theoretical investigations show that the final shape is defined by the combination of the condensation temperature and the rate of atomic deposition onto the growing nanocluster. We, thus, construct a comprehensive deposition rate-temperature diagram of Fe NP shapes and develop an analytical model that predicts the temporal evolution of these properties. Combining the shape diagram and the analytical model, morphological control of Fe NPs during formation is feasible; as such, our method proposes a roadmap for experimentalists to engineer NPs of desired shapes for targeted applications.

Single CuO nanowires decorated with size-selected Pd nanoparticles for CO sensing in humid atmosphere.

We report on conductometric gas sensors based on single CuO nanowires and compare the carbon monoxide (CO) sensing properties of pristine as well as Pd nanoparticle decorated devices in humid atmosphere. Magnetron sputter inert gas aggregation combined with a quadrupole mass filter for cluster size selection was used for single-step Pd nanoparticle deposition in the soft landing regime. Uniformly dispersed, crystalline Pd nanoparticles with size-selected diameters around 5 nm were deposited on single CuO nanowire devices in a four point configuration. During gas sensing experiments in humid synthetic air, significantly enhanced CO response for CuO nanowires decorated with Pd nanoparticles was observed, which validates that magnetron sputter gas aggregation is very well suited for the realization of nanoparticle-functionalized sensors with improved performance.

Kinetic parameter estimation and fluctuation analysis of CO at SnO2 single nanowires.

In this work, we present calculated numerical values for the kinetic parameters governing adsorption/desorption processes of carbon monoxide at tin dioxide single-nanowire gas sensors. The response of such sensors to pulses of 50 ppm carbon monoxide in nitrogen is investigated at different temperatures to extract the desired information. A rate-equation approach is used to model the reaction kinetics, which results in the problem of determining coefficients in a coupled system of nonlinear ordinary differential equations. The numerical values are computed by inverse-modeling techniques and are then used to simulate the sensor response. With our model, the dynamic response of the sensor due to the gas-surface interaction can be studied in order to find the optimal setup for detection, which is an important step towards selectivity of these devices. We additionally investigate the noise in the current through the nanowire and its changes due to the presence of carbon monoxide in the sensor environment. Here, we propose the use of a wavelet transform to decompose the signal and analyze the noise in the experimental data. This method indicates that some fluctuations are specific for the gas species investigated here.