Transporting and concentrating vibrational energy to promote isomerization.

Visible-light absorption and transport of the resultant electronic excitations to a reaction centre through Förster resonance energy transfer1-3 (FRET) are critical to the operation of biological light-harvesting systems4, and are used in various artificial systems made of synthetic dyes5, polymers6 or nanodots7,8. The fundamental equations describing FRET are similar to those describing vibration-to-vibration (V-V) energy transfer9, and suggest that transport and localization of vibrational energy should, in principle, also be possible. Although it is known that vibrational excitation can promote reactions10-16, transporting and concentrating vibrational energy has not yet been reported. We have recently demonstrated orientational isomerization enabled by vibrational energy pooling in a CO adsorbate layer on a NaCl(100) surface17. Here we build on that work to show that the isomerization reaction proceeds more efficiently with a thick 12C16O overlayer that absorbs more mid-infrared photons and transports the resultant vibrational excitations by V-V energy transfer to a 13C18O-NaCl interface. The vibrational energy density achieved at the interface is 30 times higher than that obtained with direct excitation of the interfacial CO. We anticipate that with careful system design, these concepts could be used to drive other chemical transformations, providing new approaches to condensed phase chemistry.

Chronic clinical performance of a novel subxiphoidal pacemaker system: Early feasibility study design.

BACKGROUND: Extravascular and leadless pacemakers are a new class of cardiac devices that may reduce the rate of complications common to traditional cardiac pacemakers with intracardiac leads. These devices also have the potential of expanding access to cardiac pacing therapy by simplifying the complexity and cost of implantation. The objective of this study is to evaluate the implantation, chronic safety, and performance of a novel subxiphoidal pacemaker. METHODS: This study is an open-label, non-randomized, early feasibility study. Ten patients indicated for implantation of a single-chamber ventricular pacemaker will be enrolled and implanted with the investigational device. The pacemaker will be inserted underneath the ribcage and clipped to the xiphoid process, with stimulation electrodes positioned on the cardiac pericardium. Patients will be programmed to chronic pacing; pacing capture threshold, sensing amplitude, and lead impedance will be measured at implant and regularly scheduled follow-up visits. 24-h Holter ECG and cardiac troponin will also be periodically measured. Adverse events will be recorded throughout the study period. CONCLUSION: This study is designed to assess the feasibility, safety, and chronic performance of a novel extravascular pacemaker, and will provide valuable data on whether this device has the potential to be a viable alternative to conventional pacemakers.

Superconducting single-photon detectors in the mid-infrared for physical chemistry and spectroscopy.

Applications of vibrational spectroscopy throughout the field of physical chemistry are limited by detectors with poor temporal resolution, low detection efficiency, and high background levels. Up to now, the field has relied upon detectors based on semiconducting materials with small bandgaps, which unavoidably leads to a compromise between good spectral response and noise at long wavelengths. However, a revolution in mid-infrared light detection is underway based on the interactions of photons with superconducting materials, which function under fundamentally different operating principles. Superconducting detectors were first used to detect light at shorter wavelengths. However, recent developments in their sensitivity toward mid-infrared wavelengths up to 10 µm provide new opportunities for applications in molecular science, such as infrared emission experiments, exoplanet spectroscopy and single molecule microscopy. In this tutorial review, we provide background information needed for the non-expert in superconducting light detection to apply these devices in the field of mid-infrared molecular spectroscopy. We present and compare the detection mechanisms and current developments of three types of superconducting detectors: superconducting nanowire single-photon detectors (SNSPDs), transition edge sensors (TESs), and microwave kinetic inductance detectors (MKIDs). We also highlight existing applications of SNSPDs for laser-induced infrared fluorescence experiments and discuss their potential for other molecular spectroscopy applications. Ultimately, superconducting infrared detectors have the potential to approach the sensitivity and characteristics of established single-photon detectors operating in the UV/Vis region, which have existed for almost a century and become an indispensable tool within the field of physical chemistry.

Kilopixel array of superconducting nanowire single-photon detectors.

We present a 1024-element near-infrared imaging array of superconducting nanowire single photon detectors (SNSPDs) using a 32×32 row-column multiplexing architecture. The array has an active area of 0.96 × 0.96 mm, making it the largest SNSPD array reported to date in terms of both active area and pixel count. Using a 64-channel time-tagging readout, we have characterized the array's yield, efficiency, and timing resolution. Large arrays of SNSPDs are desirable for applications such as imaging, spectroscopy, or particle detection.

Detecting Sub-GeV Dark Matter with Superconducting Nanowires.

We propose the use of superconducting nanowires as both target and sensor for direct detection of sub-GeV dark matter. With excellent sensitivity to small energy deposits on electrons and demonstrated low dark counts, such devices could be used to probe electron recoils from dark matter scattering and absorption processes. We demonstrate the feasibility of this idea using measurements of an existing fabricated tungsten-silicide nanowire prototype with 0.8-eV energy threshold and 4.3 ng with 10 000 s of exposure, which showed no dark counts. The results from this device already place meaningful bounds on dark matter-electron interactions, including the strongest terrestrial bounds on sub-eV dark photon absorption to date. Future expected fabrication on larger scales and with lower thresholds should enable probing of new territory in the direct detection landscape, establishing the complementarity of this approach to other existing proposals.

Mid-infrared Laser-Induced Fluorescence with Nanosecond Time Resolution Using a Superconducting Nanowire Single-Photon Detector: New Technology for Molecular Science.

In contrast to UV photomultiplier tubes that are widely used in physical chemistry, mid-infrared detectors are notorious for poor sensitivity and slow time response. This helps explain why, despite the importance of infrared spectroscopy in molecular science, mid-infrared fluorescence is not more widely used. In recent years, several new technologies have been developed that open new experimental possibilities for research in the mid-infrared. In this Account, we present one of the more promising technologies, superconducting nanowire single photon detectors (SNSPDs) by sharing our experience with its use in a typical experiment carried out by physical chemists (laser-induced fluorescence) and comparing the SNSPD to a detector commonly used by physical chemists (InSb at LN Temperature). SNSPDs are fabricated from a thin film of superconducting metal, patterned into a meandering nanowire. The nanowire is cooled below its superconducting temperature, Tc, and held in a constant current circuit below the critical current necessary to destroy superconductivity, Ic. Upon absorption of a photon, the resulting heat is sufficient to destroy superconductivity across the entire width of the nanowire, an event that can be detected as a voltage pulse. In contrast to semiconductor-based detectors, which have a long wavelength cutoff determined by the band gap, the SNSPD exhibits single-photon sensitivity across the entire mid-IR spectrum. As these devices have not been used extensively outside the field of light detection technology research, one important goal of this Account is to provide practical details for the implementation of these devices in a physical chemistry laboratory. We provide extensive Supporting Information describing what is needed. This includes information on a liquid nitrogen cooled monochromator, the optical collection system including mid-infrared fibers, as well as a closed-cycle cryogenic cooler that reaches 0.3 K. We demonstrate the advantages of these detectors in a time-resolved laser-induced infrared fluorescence experiment on the energy pooling in crystalline CO overlayers formed on a NaCl(100) surface. We present dispersed fluorescence spectra recorded from 1.9 to 7.0 µm obtained by single-photon counting. We also estimate the sensitivity of this WSi-based detection system at 3 µm; the system's noise equivalent power (NEP) value is ∼10-3 of a conventional InSb photovoltaic device. Straightforward modifications are expected to provide another 100 000-fold improvement. We demonstrate that the temporal resolution of the experiment is limited only by the pulse duration of the laser used in this work (fwhm = 3.7 ns). The use of SNSPDs enables dramatically improved observations of energy pooling in cryogenic molecular crystals.

Short-wave infrared compressive imaging of single photons.

We present a short-wave infrared (SWIR) single photon camera based on a single superconducting nanowire single photon detector (SNSPD) and compressive imaging. We show SWIR single photon imaging at a megapixel resolution with a low signal-to-background ratio around 0.6, show SWIR video acquisition at 20 frames per second and 64x64 pixel video resolution, and demonstrate sub-nanosecond resolution time-of-flight imaging. All scenes were sampled by detecting only a small number of photons for each compressive sampling matrix. In principle, our technique can be used for imaging faint objects in the mid-IR regime.

Ultra-sensitive mid-infrared emission spectrometer with sub-ns temporal resolution.

We evaluate the performance of a mid-infrared emission spectrometer operating at wavelengths between 1.5 and 6 µm based on an amorphous tungsten silicide (a-WSi) superconducting nanowire single-photon detector (SNSPD). We performed laser induced fluorescence spectroscopy of surface adsorbates with sub-monolayer sensitivity and sub-nanosecond temporal resolution. We discuss possible future improvements of the SNSPD-based infrared emission spectrometer and its potential applications in molecular science.

Optically Addressing Single Rare-Earth Ions in a Nanophotonic Cavity.

We demonstrate optical probing of spectrally resolved single Nd^{3+} rare-earth ions in yttrium orthovanadate. The ions are coupled to a photonic crystal resonator and show strong enhancement of the optical emission rate via the Purcell effect, resulting in near radiatively limited single photon emission. The measured high coupling cooperativity between a single photon and the ion allows for the observation of coherent optical Rabi oscillations. This could enable optically controlled spin qubits, quantum logic gates, and spin-photon interfaces for future quantum networks.

Conclusive Experimental Demonstration of One-Way Einstein-Podolsky-Rosen Steering.

Einstein-Podolsky-Rosen steering is a quantum phenomenon wherein one party influences, or steers, the state of a distant party's particle beyond what could be achieved with a separable state, by making measurements on one-half of an entangled state. This type of quantum nonlocality stands out through its asymmetric setting and even allows for cases where one party can steer the other but where the reverse is not true. A series of experiments have demonstrated one-way steering in the past, but all were based on significant limiting assumptions. These consisted either of restrictions on the type of allowed measurements or of assumptions about the quantum state at hand, by mapping to a specific family of states and analyzing the ideal target state rather than the real experimental state. Here, we present the first experimental demonstration of one-way steering free of such assumptions. We achieve this using a new sufficient condition for nonsteerability and, although not required by our analysis, using a novel source of extremely high-quality photonic Werner states.

Efficient and pure femtosecond-pulse-length source of polarization-entangled photons.

We present a source of polarization entangled photon pairs based on spontaneous parametric downconversion engineered for frequency uncorrelated telecom photon generation. Our source provides photon pairs that display, simultaneously, the key properties for high-performance quantum information and fundamental quantum science tasks. Specifically, the source provides for high heralding efficiency, high quantum state purity and high entangled state fidelity at the same time. Among different tests we apply to our source we observe almost perfect non-classical interference between photons from independent sources with a visibility of (100 ± 5)%.

Heralded amplification of photonic qubits.

We demonstrate postselection free heralded qubit amplification for Time-Bin qubits and single photon states in an all-fibre, telecom-wavelength, scheme that highlights the simplicity, stability and potential for fully integrated photonic solutions. Exploiting high-efficiency superconducting detectors, the gain, fidelity and the performance of the amplifier are studied as a function of loss. We also demonstrate the first heralded single photon amplifier with independent sources. This provides a significant advance towards demonstrating device-independent quantum key distribution as well as fundamental tests of quantum mechanics over extended distances.

Spectral correlation and interference in non-degenerate photon pairs at telecom wavelengths.

We characterize an entangled-photon-pair source that produces signal and idler photons at 1533 nm and 1567 nm using fiber-assisted signal-photon spectroscopy. By erasing the polarization distinguishability, we observe interference between the two down-conversion paths. The observed interference signature is closely related to the spectral correlations between photons in a Hong-Ou-Mandel interferometer. These measurements suggest good indistinguishability between the two down-conversion paths, which is required for high entanglement visibility.

High-efficiency WSi superconducting nanowire single-photon detectors for quantum state engineering in the near infrared.

We report on high-efficiency superconducting nanowire single-photon detectors based on amorphous tungsten silicide and optimized at 1064 nm. At an operating temperature of 1.8 K, we demonstrated a 93% system detection efficiency at this wavelength with a dark noise of a few counts per second. Combined with cavity-enhanced spontaneous parametric downconversion, this fiber-coupled detector enabled us to generate narrowband single photons with a heralding efficiency greater than 90% and a high spectral brightness of 0.6×104 photons/(s·mW·MHz). Beyond single-photon generation at large rate, such high-efficiency detectors open the path to efficient multiple-photon heralding and complex quantum state engineering.

Temporal Multimode Storage of Entangled Photon Pairs.

Multiplexed quantum memories capable of storing and processing entangled photons are essential for the development of quantum networks. In this context, we demonstrate and certify the simultaneous storage and retrieval of two entangled photons inside a solid-state quantum memory and measure a temporal multimode capacity of ten modes. This is achieved by producing two polarization-entangled pairs from parametric down-conversion and mapping one photon of each pair onto a rare-earth-ion-doped (REID) crystal using the atomic frequency comb (AFC) protocol. We develop a concept of indirect entanglement witnesses, which can be used as Schmidt number witnesses, and we use it to experimentally certify the presence of more than one entangled pair retrieved from the quantum memory. Our work puts forward REID-AFC as a platform compatible with temporal multiplexing of several entangled photon pairs along with a new entanglement certification method, useful for the characterization of multiplexed quantum memories.

Telecom-Wavelength Atomic Quantum Memory in Optical Fiber for Heralded Polarization Qubits.

Polarization-encoded photons at telecommunication wavelengths provide a compelling platform for practical realizations of photonic quantum information technologies due to the ease of performing single qubit manipulations, the availability of polarization-entangled photon-pair sources, and the possibility of leveraging existing fiber-optic links for distributing qubits over long distances. An optical quantum memory compatible with this platform could serve as a building block for these technologies. Here we present the first experimental demonstration of an atomic quantum memory that directly allows for reversible mapping of quantum states encoded in the polarization degree of freedom of a telecom-wavelength photon. We show that heralded polarization qubits at a telecom wavelength are stored and retrieved with near-unity fidelity by implementing the atomic frequency comb protocol in an ensemble of erbium atoms doped into an optical fiber. Despite remaining limitations in our proof-of-principle demonstration such as small storage efficiency and storage time, our broadband light-matter interface reveals the potential for use in future quantum information processing.

Strong Loophole-Free Test of Local Realism.

We present a loophole-free violation of local realism using entangled photon pairs. We ensure that all relevant events in our Bell test are spacelike separated by placing the parties far enough apart and by using fast random number generators and high-speed polarization measurements. A high-quality polarization-entangled source of photons, combined with high-efficiency, low-noise, single-photon detectors, allows us to make measurements without requiring any fair-sampling assumptions. Using a hypothesis test, we compute p values as small as 5.9×10^{-9} for our Bell violation while maintaining the spacelike separation of our events. We estimate the degree to which a local realistic system could predict our measurement choices. Accounting for this predictability, our smallest adjusted p value is 2.3×10^{-7}. We therefore reject the hypothesis that local realism governs our experiment.

A 64-pixel mid-infrared single-photon imager based on superconducting nanowire detectors.

A large-format mid-infrared single-photon imager with very low dark count rates would enable a broad range of applications in fields like astronomy and chemistry. Superconducting nanowire single-photon detectors (SNSPDs) are a mature photon-counting technology as demonstrated by their figures of merit such as high detection efficiencies and very low dark count rates. However, scaling SNSPDs to large array sizes for mid-infrared applications requires sophisticated readout architectures in addition to superconducting materials development. In this work, an SNSPD array design that combines a thermally coupled row-column multiplexing architecture with a thermally coupled time-of-flight transmission line was developed for mid-infrared applications. The design requires only six cables and can be scaled to larger array sizes. The demonstration of a 64-pixel array shows promising results for wavelengths between 3.4 µm and 10 µm, which will enable the use of this single-photon detector technology for a broad range of new applications.

First-in-man clinical implantation and acute pacing performance of a novel subxiphoidal pacemaker system.

BACKGROUND: Intravascular cardiac pacemakers are an established therapy for bradycardic indications. Recently, a new class of leadless pacemakers have mitigated some of the complications related to pacemaker leads. In this study, we evaluate the implantation and performance of a novel extravascular technology that delivers epicardial pacing through a subxiphoidal approach. METHODS: Fifteen patients undergoing non-emergent open-heart surgery were enrolled. A midline incision was made just below the xiphoid process, and substernal tunneling was used to create a pocket for the device and to access the anterior pericardium over the right ventricle. The test device (Calyan Technologies, Oakdale, MN) was temporarily inserted underneath the ribcage and clipped to the xiphoid process. The sensing and pacing electrode (FlexArm) was positioned on the anterior pericardium. Ventricular sensing and pacing capture thresholds were measured. RESULTS: The test device was successfully implanted in all 15 patients. There were no device or procedure-related adverse events. The first five implanted patients had no pacing capture at maximum stimulation intensity. Design changes were made to the device, including different electrode size and shape, and successful ventricular capture was achieved in 9 of the subsequent 10 patients. In these patients, pacing threshold was 3.8 ± 1.6 mA with a pulse width of 0.5 ms. All devices were successfully explanted at the end of the procedure. CONCLUSIONS: In a first-in-human experience with a novel extravascular pacemaker, this study demonstrated the feasibility of pericardial ventricular pacing via a subxiphoidal approach. Further chronic studies are required to evaluate the safety and performance of this novel pacing technology.

Safety and performance of a novel subxiphoidal pacemaker system.

BACKGROUND: Traditional cardiac pacemakers commonly have a range of complications related to the presence of intracardiac leads. A new class of extravascular and leadless pacemakers has recently emerged with the potential to mitigate these complications and expand access to cardiac pacing. The objective of this study is to evaluate the implantation, short-term chronic safety, and performance of a novel subxiphoidal extracardiac pacemaker. METHODS: Normal Yorkshire Cross swine (n = 16) were implanted with the subxiphoidal pacemaker. The pacemaker was inserted through a midline chest incision and clipped to the underside of the sternum, with the stimulation electrode placed on the anterior pericardium. Animals were chronically paced and followed for 90 days post-implant, with periodic measurement of pacing capture threshold (PCT) and electrode impedance. RESULTS: All 16 animals were successfully implanted with the study device. At implant, a consistent average PCT of 2.2 ± 0.4 V at a pulse width of 1.0 ms was observed in all animals, with an average implant impedance of 648 ± 44 Ω. Chronic pacing was programmed at a rate of 60 bpm, an amplitude of 3.4 ± 0.7 V, and a pulse width of 1.0 ms. PCT rose to 4.6 ± 0.8 V at 14 days and stabilized; at 90 days, PCT was 3.8 ± 1.2 V and electrode impedance was 533 ± 105 Ω. All implanted animals completed the study with no clinically significant findings, no clinically significant abnormalities, and with no adverse events that affected animal welfare. CONCLUSIONS: This study demonstrated the safety and feasibility of a novel subxiphoidal extracardiac pacemaker to deliver short-term chronic extravascular therapy. Further studies are required to assess the safety, feasibility, and long-term chronic pacing performance in human subjects.