Volume 12, Issue 3 - Special Issue: Quantum Nanophotonics

At the core of quantum photonic information processing and sensing, two major building pillars are single-photon emitters and single-photon detectors. In this review, we systematically summarize the working theory, material platform, fabrication process, and game-changing applications enabled by state-of-the-art quantum dots in nanowire emitters and superconducting nanowire single-photon detectors. Such nanowire-based quantum hardware offers promising properties for modern quantum optics experiments. We highlight several burgeoning quantum photonics applications using nanowires and discuss development trends of integrated quantum photonics. Also, we propose quantum information processing and sensing experiments for the quantum optics community, and future interdisciplinary applications.

Solid-state defects acting as single photon sources and quantum bits are leading contenders in quantum technologies. Despite great efforts, not all the properties and behaviours of the presently known solid-state defect quantum bits are understood. Furthermore, various quantum technologies require novel solutions, thus new solid-state defect quantum bits should be explored to this end. These issues call to develop ab initio methods which accurately yield the key parameters of solid-state defect quantum bits and vastly accelerate the identification of novel ones for a target quantum technology application. In this review, we describe recent developments in the field including the calculation of excited states with quantum mechanical forces, treatment of spatially extended wavefunctions in supercell models, methods for temperature-dependent Herzberg–Teller fluorescence spectrum and photo-ionisation thresholds, accurate calculation of magneto-optical parameters of defects consisting of heavy atoms, as well as spin-phonon interaction responsible for temperature dependence of the longitudonal spin relaxation T 1 time and magneto-optical parameters, and finally the calculation of spin dephasing and spin-echo times. We highlight breakthroughs including the description of effective-mass like excited states of deep defects and understanding the leading microscopic effect in the spin-relaxation of isolated nitrogen-vacancy centre in diamond.

The chemically synthesizable quantum emitters such as quantum dots (QDs), fluorescent nanodiamonds (FNDs), and organic fluorescent dyes can be integrated with an easy-to-craft quantum nanophotonic device, which would be readily developed by non-lithographic solution process. As a representative example, the solution dipping or casting of such soft quantum emitters on a flat metal layer and subsequent drop-casting of plasmonic nanoparticles can afford the quantum emitter-coupled plasmonic nanocavity (referred to as a nanoparticle-on-mirror (NPoM) cavity), allowing us for exploiting various quantum mechanical behaviors of light–matter interactions such as quantum electrodynamics (QED), strong coupling (e.g., Rabi splitting), and quantum mirage. This versatile, yet effective soft quantum nanophotonics would be further benefitted from a deterministic control over the positions and orientations of each individual quantum emitter, particularly at the molecule level of resolution. In this review, we will argue that DNA nanotechnology can provide a gold vista toward this end. A collective set of exotic characteristics of DNA molecules, including Watson-Crick complementarity and helical morphology, enables reliable grabbing of quantum emitters at the on-demand position and steering of their directors at the single molecular level. More critically, the recent advances in large-scale integration of DNA origami have pushed the reliance on the distinctly well-formed single device to the regime of the ultra-scale device arrays, which is critical for promoting the practically immediate applications of such soft quantum nanophotonics.

The fundamental understanding of molecular quantum electrodynamics via the strong light–matter interactions between a nanophotonic cavity and quantum emitters opens various applications in quantum biology, biophysics, and chemistry. However, considerable obstacles to obtaining a clear understanding of coupling mechanisms via reliable experimental quantifications remain to be resolved before this field can truly blossom toward practical applications in quantitative life science and photochemistry. Here, we provide recent advancements of state-of-the-art demonstrations in plexcitonic and vibro-polaritonic strong couplings and their applications. We highlight recent studies on various strong coupling systems for altering chemical reaction landscapes. Then, we discuss reports dedicated to the utilization of strong coupling methods for biomolecular sensing, protein functioning studies, and the generation of hybrid light–matter states inside living cells. The strong coupling regime provides a tool for investigating and altering coherent quantum processes in natural biological processes. We also provide an overview of new findings and future avenues of quantum biology and biochemistry.

Nitrogen vacancy centers in diamond provide a spin-based qubit system with long coherence time even at room temperature, making them suitable ambient-condition quantum sensors for quantities including electromagnetic fields, temperature, and rotation. The optically addressable level structures of NV spins allow transduction of spin information onto light-field intensity. The sub-optimal readout fidelity of conventional fluorescence measurement remains a significant drawback for room-temperature ensemble sensing. Here, we discuss nanophotonic interfaces that provide opportunities to achieve near-unity readout fidelity based on IR absorption via resonantly enhanced spin-optic coupling. Spin-coupled resonant nanophotonic devices are projected to particularly benefit applications that utilize micro- to nanoscale sensing volume and to outperform present methods in their volume-normalized sensitivity.

Metal-halide perovskite light-emitting diodes (PeLEDs) are considered as new-generation highly efficient luminescent materials for application in displays and solid-state lighting. Since the first successful demonstration of PeLEDs in 2014, the research on the development of efficient PeLEDs has progressed significantly. Although the device efficiency has significantly improved over a short period of time, their overall performance has not yet reached the levels of mature technologies for practical applications. Various degradation processes are the major impediment to improving the performance and stability of PeLED devices. In this review, we discuss various analysis techniques that are necessary to gain insights into the effects of various degradation mechanisms on the performance and stability of PeLEDs. Based on the causes and effects of external and internal factors, the degradation processes and associated mechanisms are examined in terms of critical physical and chemical parameters. Further, according to the progress of the current research, the challenges faced in studying degradation mechanisms are also elucidated. Given the universality of the degradation behavior, an in-depth understanding of the device degradation may promote the development of optimization strategies and further improve the performance and stability of PeLEDs.

Two-dimensional (2D) materials have shown great promise as hosts for high-purity deterministic single-photon sources. In the last few years, the underlying physics of single photon emission in 2D materials have been uncovered, and their optical properties have been improved to meet criteria for a variety of quantum technologies and applications. In this work, we take advantage of the unique characteristics of dielectric nanoantennas in manipulating the electromagnetic response on a sub-wavelength scale to localize and control defect-based single-photon emitters (SPEs) in 2D layered materials. We show that dielectric nanoantennas are capable of inducing high Purcell enhancement >20 and therefore brighter single-photon emission, which is characterized by a reduction of the emitters’ radiative lifetimes and enhancement of their brightness by more than an order of magnitude. We demonstrate that the sub-wavelength-scale dielectric nanoantennas can be designed to also impose a predetermined strain profile that determines the confinement potential of the SPE, leading to robust control over the optical polarization with up to 94% extinction ratio. The combination of large Purcell enhancement, polarization orientation, and site control through strain engineering demonstrates the advantages and unique capabilities of dielectric nanoantennas for enhancing the quantum optical properties of 2D SPEs for quantum information technologies.

Diamond color centers have been widely studied in the field of quantum optics. The negatively charged silicon vacancy (SiV − ) center exhibits a narrow emission linewidth at the wavelength of 738 nm, a high Debye–Waller factor, and unique spin properties, making it a promising emitter for quantum information technologies, biological imaging, and sensing. In particular, nanodiamond (ND)-based SiV − centers can be heterogeneously integrated with plasmonic and photonic nanostructures and serve as in vivo biomarkers and intracellular thermometers. Out of all methods to produce NDs with SiV − centers, ion implantation offers the unique potential to create controllable numbers of color centers in preselected individual NDs. However, the formation of single color centers in NDs with this technique has not been realized. We report the creation of single SiV − centers featuring stable high-purity single-photon emission through Si implantation into NDs with an average size of ∼20 nm. We observe room temperature emission, with zero-phonon line wavelengths in the range of 730–800 nm and linewidths below 10 nm. Our results offer new opportunities for the controlled production of group-IV diamond color centers with applications in quantum photonics, sensing, and biomedicine.

Up-conversion single-photon detectors (UCSPD) are based on sum-frequency generation of the telecom band single-photons to near-infrared wavelengths at which efficient and low-noise silicon single-photon detectors are available. Moreover, because of high dynamic range of silicon single-photon detectors, UCSPD is suitable for high-speed quantum communication. UCSPDs reported to date, however, have a very narrow fixed window of detectable wavelengths, severely limiting their applications in wavelength-multiplexed quantum networks. In this work, we report a tunable UCSPD module that covers the complete telecom C band, making it suitable for quantum communication networks based on sharing wavelength-multiplexed entangled photons.

Common methods to achieve photon number resolution rely on fast on-off single-photon detectors in conjunction with temporal or spatial mode multiplexing. Yet, these methods suffer from an inherent trade-off between the efficiency of photon number discrimination and photon detection rate. Here, we introduce a method of photon number resolving detection that overcomes these limitations by replacing mode multiplexing with coherent absorption of a single optical mode in a distributed detector array. Distributed coherent absorption ensures complete and uniform absorption of light among the constituent detectors, enabling fast and efficient photon number resolution. As a proof-of-concept, we consider the case of a distributed array of superconducting nanowire single-photon detectors with realistic parameters and show that deterministic absorption and arbitrarily high photon number discrimination efficiency can be achieved by increasing the number of detectors in the array. Photon number resolution without optical mode multiplication provides a simple yet effective method to discriminate an arbitrary number of photons in large arrays of on-off detectors or in smaller arrays of mode multiplexed detectors.

Micro-/nanocavities that combine high quality factor ( Q ) and small mode volume ( V ) have been used to enhance light–matter interactions for cavity quantum electrodynamics (cQED). Whispering gallery mode (WGM) geometries such as microdisks and microrings support high- Q and are design- and fabrication-friendly, but V is often limited to tens of cubic wavelengths to avoid WGM radiation. The stronger modal confinement provided by either one-dimensional or two-dimensional photonic crystal defect geometries can yield sub-cubic-wavelength V , yet the requirements on precise design and dimensional control are typically much more stringent to ensure high- Q . Given their complementary features, there has been sustained interest in geometries that combine the advantages of WGM and photonic crystal cavities. Recently, a “microgear” photonic crystal ring (MPhCR) has shown promise in enabling additional defect localization ( > $ > $ 10× reduction of V ) of a WGM, while maintaining high- Q ( ≈ 1 0 6 ) $(\approx 1{0}^{6})$ and other WGM characteristics in ease of coupling and design. However, the unit cell geometry used is unlike traditional PhC cavities, and etched surfaces may be too close to embedded quantum nodes (quantum dots, atomic defect spins, etc.) for cQED applications. Here, we report two novel PhCR designs with “rod” and “slit” unit cells, whose geometries are more traditional and suitable for solid-state cQED. Both rod and slit PhCRs have high- Q ( > 1 0 6 ) $( > 1{0}^{6})$ with WGM coupling properties preserved. A further ≈10× reduction of V by defect localization is observed in rod PhCRs. Moreover, both fundamental and 2nd-order PhC modes co-exist in slit PhCRs with high Q s and good coupling. Our work showcases that high- Q / V PhCRs are in general straightforward to design and fabricate and are a promising platform to explore for cQED.

An on-chip quantum light source based on spontaneous four-wave mixing is an essential element for developing quantum photonic integrated circuit technology, which has the advantage of no connection loss owing to the integration of the source into photonic circuits. The waveguide-based quantum light source inevitably causes propagation loss owing to imperfections in the fabrication process, but the propagation loss effects on photon-pair generation have not been extensively studied. In this study, propagation loss effects were examined using theoretical and experimental methods. In theory, the performance of quantum light sources, such as brightness, heralding efficiency, and coincidence-to-accidental ratio, strongly depend on propagation loss. We fabricate several waveguides with a moderate propagation loss of 2.2 dB/cm to investigate the loss dependence and ascertain that the brightness, heralding efficiency, and coincidence-to-accident ratio strongly correlate with the length of the optical waveguide. The maximum coincidence-count brightness occurred at an optimization length of 1/ α , where α is the absorption coefficient. In contrast, the single-count brightness shows slightly different waveguide length dependence owing to loss-induced one-photon states. We expect that the results obtained in this study will greatly assist in determining the proper waveguide length for photon-pair generation according to the source’s application fields. The results will be helpful in the development of a quantum light source suitable for practical and quantum optical integrated circuits and will lead to the development of high-fidelity quantum technologies.

Temporal metamaterials empower novel forms of wave manipulation with direct applications to quantum state transformations. In this work, we investigate vacuum amplification effects in anisotropic temporal boundaries. Our results theoretically demonstrate that the anisotropy of the temporal boundary provides control over the angular distribution of the generated photons. We analyze several single and multi-layered configurations of anisotropic temporal boundaries, each with a distinct vacuum amplification effect. Examples include the inhibition of photon production along specific directions, resonant and directive vacuum amplification, the generation of angular and frequency photon combs and fast angular variations between inhibition and resonant photon production.

The electromagnetic local density of states (LDOS) is crucial to many aspects of photonics engineering, from enhancing emission of photon sources to radiative heat transfer and photovoltaics. We present a framework for evaluating upper bounds on the LDOS in structured media that can handle arbitrary bandwidths and accounts for critical wave scattering effects. The bounds are solely determined by the bandwidth, material susceptibility, and device footprint, with no assumptions on geometry. We derive an analytical expression for the maximum LDOS consistent with the conservation of energy across the entire design domain, which upon benchmarking with topology-optimized structures is shown to be nearly tight for large devices. Novel scaling laws for maximum LDOS enhancement are found: the bounds saturate to a finite value with increasing susceptibility and scale as the quartic root of the bandwidth for semi-infinite structures made of lossy materials, with direct implications on material selection and design applications.

Percolation, describing critical behaviors of phase transition in a geometrical context, prompts wide investigations in natural and social networks as a fundamental model. The introduction of quantum coherence and superposition brings percolation into quantum regime with more fascinating phenomena and unique features, which, however, has not been experimentally explored yet. Here we successfully map these large-scale porous structures into a photonic chip using femtosecond laser direct writing techniques and present an experimental demonstration of quantum transport in hexagonal percolation lattices, probed by coherent light. A quantum percolation threshold of 80% is observed in the prototyped laser-written lattices with up to 1,600 waveguides, which is significantly larger than the classical counterpart of 63%. We also investigate the spatial confinement by localization parameters and exhibit the transition from ballistic to diffusive propagation with the decrease of the occupation probability. Direct observation of quantum percolation may deepen the understanding of the relation among materials, quantum transport, geometric quenching, disorder and localization, and inspire applications for quantum technologies.

Bell state measurement is vital to quantum information technology. Conventional linear optical elements, however, cannot fully distinguish all polarization Bell states without assisting of additional degrees of freedom. Leveraging on a pair of binary-pixel metasurfaces, we demonstrate direct measurement of all four polarization Bell states. Each metasurface is designed to produce two output modes that linearly superpose three Bell states in the coincidence counting measurement. By rotating the polarizers, the coincidence counting measurement achieves a tunable anticorrelation between one and the other two Bell states, achieving Bell state detection efficiency of 75% in a single measurement. Complete and deterministic Bell state measurement is further realized by performing two measurements. Our work shows the advantage of utilization of metasurfaces in quantum detection schemes and is of great applicative interest for quantum dense coding, entanglement swapping, quantum teleportation protocols, and novel quantum information processing tasks.

Two-photon interference is an important effect that is tightly related to the quantum nature of light. Recently, it has been shown that the photon bunching from the Hong–Ou–Mandel (HOM) effect can be used for quantum imaging in which sample properties (reflection/transmission amplitude, phase delay, or polarization) can be characterized at the pixel-by-pixel level. In this work, we perform Jones matrix imaging for an unknown object based on two-photon interference. By using a reference metasurface with panels of known polarization responses in pairwise coincidence measurements, the object’s polarization responses at each pixel can be retrieved from the dependence of the coincidence visibility as a function of the reference polarization. The post-selection of coincidence images with specific reference polarization in our approach eliminates the need in switching the incident polarization and thus parallelized optical measurements for Jones matrix characterization. The parallelization in preparing input states, prevalent in any quantum algorithms, is an advantage of adopting two-photon interference in Jones matrix imaging. We believe our work points to the usage of metasurfaces in biological and medical imaging in the quantum optical regime.

Nonreciprocity originating from classical interactions among nonlinear scatterers has been attracting increasing attention in the quantum community, offering a promising tool to control excitation transfer for quantum information processing and quantum computing. In this work, we explore the possibility of realizing largely nonreciprocal total cross sections for a pair of quantum metasurfaces formed by two parallel periodic arrays of two-level atoms. We show that large nonreciprocal responses can be obtained in such nonlinear systems by controlling the position of the atoms and their transition frequencies, without requiring that the environment in which the atoms are placed is nonreciprocal. We demonstrate the connection of this effect with the asymmetric population of a slowly decaying dark state, which is critical to obtain large nonreciprocal responses.

Self-powered photodetectors with broadband and polarization-sensitive photoresponse are desirable for many important applications such as wearable electronic devices and wireless communication systems. Recently, two-dimensional (2D) materials have been demonstrated as promising candidates for self-powered photodetectors owing to their advantages in light–matter interaction, transport, electronic properties, and so on. However, their performance in speed, broadband response, and multifunction is still limited. Here, we report a PdSe 2 photodetector with asymmetric van der Waals (vdWs) contacts formed by using a homojunction configuration. This device achieves a high responsivity approaching 53 mA/W, a rise/decay time of about 0.72 ms/0.24 ms, and a detectivity of more than 5.17 × 10 11 Jones in the visible-near infrared regime (532–1470 nm). In addition, a linear polarization-sensitive response can be observed with an anisotropy ratio of 1.11 at 532 nm and 1.62 at 1064 nm. Furthermore, a strong anisotropic response endows this photodetector with outstanding polarization imaging capabilities, realizing a contrast-enhanced degree of linear polarization imaging. Our proposed device architecture demonstrated the great potential of PdSe 2 -based asymmetric vdWs contacts for high-performance photodetectors operating without any external bias.

Plasmonic nanoantennas have been extensively explored to boost nonlinear optical processes due to their capabilities to confine optical fields on the nanoscale. In harmonic generation, nanoantenna array architectures are often employed to increase the number of emitters in order to efficiently enhance the harmonic emission. A small laser focus spot on the nanoantenna array maximizes the harmonic yield since it scales nonlinearly with the incident laser intensity. However, the nonlinear yield of the nanoantennas lying at the boundary of a focused beam may exhibit significant deviations in comparison to those at the center of the beam due to the Gaussian intensity distribution of the beam. This spatial beam inhomogeneity can cause power instability of the emitted harmonics when the lateral beam position is not stable which we observed in plasmon-enhanced third-harmonic generation (THG). Hence, we propose a method for deterministically designing the density of a nanoantenna array to decrease the instability of the beam position-dependent THG yield. This method is based on reducing the ratio between the number of ambiguous nanoantennas located at the beam boundary and the total number of nanoantennas within the beam diameter to increase the plasmon-enhanced THG stability, which we term as the ratio of ambiguity ( ROA ). We find that the coefficient of variation of the measured plasmonic THG yield enhancement decreases with the ROA . Thus, our method is beneficial for designing reliable sensors or nonlinear optical devices consisting of nanoantenna arrays for enhancing output signals.

We have studied reflection spectra of dye-doped and undoped polymers deposited onto Ag and Au substrates and found anomalous dips in the UV spectral range. On top of Ag substrates, the λ ∼ 375 nm dips were observed in undoped PMMA, PVP, and PS polymers as well as PMMA doped with Rh590 and HITC laser dyes. In silver-based samples, the spectral positions of the observed reflection dips were close to singularities in the refractive indexes of surface plasmon polaritons (SPPs) propagating at the interface between Ag and polymer. The latter singularities can tentatively explain the λ ∼ 375 nm reflection dips, if the scattering of Ag and polymeric films is large enough to launch SPP without any prism or grating. The dips observed in reflection of Rh590:PMMA and HITC:PMMA on top of Au, were more pronounced than those on Ag, broader, shifted to shorter wavelengths, and their spectral positions had large standard deviations. Furthermore, no anomalous dips in gold-based samples were observed in the reflection spectra of undoped PMMA, PVP, and PS polymers, and a modest singularity in the SPP refractive index, predicted theoretically at λ ∼ 500 nm, cannot explain the dips in the UV reflection spectra observed experimentally. It appears likely that the origin of the reflection dips on top of Au substrates is different from that on top of Ag substrates.