An optimal single-photon source should deterministically deliver one and only one photon at a time, with no trade-off between the source's efficiency and the photon indistinguishability. However, all reported solid-state sources of indistinguishable single photons had to rely on polarization filtering which reduced the efficiency by 50%, which fundamentally limited the scaling of photonic quantum technologies. Here, we overcome this final long-standing challenge by coherently driving quantum dots deterministically coupled to polarization-selective Purcell microcavities-two examples are narrowband, elliptical micropillars and broadband, elliptical Bragg gratings. A polarization-orthogonal excitation-collection scheme is designed to minimize the polarization-filtering loss under resonant excitation. We demonstrate a polarized single-photon efficiency of 0.60(2), a single-photon purity of 0.991(3), and an indistinguishability of 0.973(5). Our work provides promising solutions for truly optimal single-photon sources combining near-unity indistinguishability and near-unity system efficiency simultaneously.Single photons are appealing candidates for quantum communications 1,2 , quantumenhanced metrology 3,4 and quantum computing 5,6 . In view of the quantum information applications, the single photons are required to be controllably prepared with a high efficiency into a given quantum state. Specifically, the single photons should possess the same polarization, spatial mode, and transform-limited spectro-temporal profile for a high-visibility Hong-Ou-Mandel-type quantum interference 1,7 .Self-assembled quantum dots show so far the highest quantum efficiency among solid-state quantum emitters and thus can potentially serve as an ideal single-photon source 8-15 . There has been encouraging progress in recent years in developing highperformance single-photon sources 11 . Pulsed resonant excitation on single quantum dots has been developed to eliminate dephasing and time jitter, which created single photons with near-unity indistinguishability 15 . Further, by combining the resonant excitation with Purcell-enhanced micropillar 16,17 or photonic crystals 18,19 , the generated transform-limited 20,21 single photons have been efficiently extracted out of the bulk and funneled into a single mode at far field. Despite the recent progress 16-22 , the experimentally achieved polarized-single-photon efficiency (defined as the number of single-polarized photons extracted from the bulk semiconductor and collected by the first lens per pumping pulse) is ~33% in ref. 16 and ~15% in ref. 17, still fell short of the minimally required efficiency of 50% for boson sampling to show computational advantage to classical algorithms 23 , and was below the efficiency threshold of 67% for photon-loss-tolerant encoding in cluster-state models of optical quantum computing 24 . It should be noted that a <50% single-photon efficiency would render nearly all linear optical quantum computing schemes 1,5 not scalable.The indistinguishable single-photon...

Infrared spectroscopy, especially for molecular vibrations in the fingerprint region between 600 and 1,500 cm−1, is a powerful characterization method for bulk materials. However, molecular fingerprinting at the nanoscale level still remains a significant challenge, due to weak light–matter interaction between micron-wavelengthed infrared light and nano-sized molecules. Here we demonstrate molecular fingerprinting at the nanoscale level using our specially designed graphene plasmonic structure on CaF2 nanofilm. This structure not only avoids the plasmon–phonon hybridization, but also provides in situ electrically-tunable graphene plasmon covering the entire molecular fingerprint region, which was previously unattainable. In addition, undisturbed and highly confined graphene plasmon offers simultaneous detection of in-plane and out-of-plane vibrational modes with ultrahigh detection sensitivity down to the sub-monolayer level, significantly pushing the current detection limit of far-field mid-infrared spectroscopies. Our results provide a platform, fulfilling the long-awaited expectation of high sensitivity and selectivity far-field fingerprint detection of nano-scale molecules for numerous applications.

IntroductionOver the past decade, optical near-field techniques, especially scattering-type scanning near-field optical microscopy Infrared and optical spectroscopy represents one of the most informative methods in advanced materials research. As an important branch of modern optical techniques that has blossomed in the past decade, scattering-type scanning near-field optical microscopy (s-SNOM) promises deterministic characterization of optical properties over a broad spectral range at the nanoscale. It allows ultrabroadband optical (0.5-3000 µm) nanoimaging, and nanospectroscopy with fine spatial (<10 nm), spectral (<1 cm −1 ), and temporal (<10 fs) resolution. The history of s-SNOM is briefly introduced and recent advances which broaden the horizons of this technique in novel material research are summarized. In particular, this includes the pioneering efforts to study the nanoscale electrodynamic properties of plasmonic metamaterials, strongly correlated quantum materials, and polaritonic systems at room or cryogenic temperatures. Technical details, theoretical modeling, and new experimental methods are also discussed extensively, aiming to identify clear technology trends and unsolved challenges in this exciting field of research. and Astronomy. His research interests cover nanoscale and ultrafast electromagnetic responses of strongly correlated electron materials, 2D materials, and metamaterials that span from the near-infrared to terahertz frequencies.tip-sample interactions. In s-SNOM, these difficulties result from at least three factors. First, the well-known antenna effect [48] causes light to be highly confined between the probe apex and the sample surface. The specific geometry of the tip shank plays a significant role in determining the intensity of the scattered signal. [49] Second, in addition to the local optical information, a strong but undesired background signal can be detected. This background signal can be mainly attributed to the light scattering from the tip shank, cantilever, and sample surface. Third, due to the broad momentum distribution of the localized radiation, in some cases, nominally "far-field trivial" Adv. Mater. 2019, 31, 1804774 Figure 1. Far-field (blue) and near-field (yellow) measurements, accessing the propagating field and the evanescent field, respectively.The authors declare no conflict of interest.

An outstanding goal in quantum optics and scalable photonic quantum technology is to develop a source that each time emits one and only one entangled photon pair with simultaneously high entanglement fidelity, extraction efficiency, and photon indistinguishability. By coherent two-photon excitation of a single InGaAs quantum dot coupled to a circular Bragg grating bullseye cavity with broadband high Purcell factor up to 11.3, we generate entangled photon pairs with a state fidelity of 0.90(1), pair generation rate of 0.59(1), pair extraction efficiency of 0.62(6), and photon indistinguishability of 0.90(1) simultaneously. Our work will open up many applications in high-efficiency multi-photon experiments and solid-state quantum repeaters.

Identification of gas molecules plays a key role a wide range of applications extending from healthcare to security. However, the most widely used gas nano-sensors are based on electrical approaches or refractive index sensing, which typically are unable to identify molecular species. Here, we report label-free identification of gas molecules SO 2 , NO 2 , N 2 O, and NO by detecting their rotational-vibrational modes using graphene plasmon. The detected signal corresponds to a gas molecule layer adsorbed on the graphene surface with a concentration of 800 zeptomole per μm 2 , which is made possible by the strong field confinement of graphene plasmons and high physisorption of gas molecules on the graphene nanoribbons. We further demonstrate a fast response time (<1 min) of our devices, which enables real-time monitoring of gaseous chemical reactions. The demonstration and understanding of gas molecule identification using graphene plasmonic nanostructures open the door to various emerging applications, including in-breath diagnostics and monitoring of volatile organic compounds.