Double-Pulse Generation of Indistinguishable Single Photons with Optically Controlled Polarization.

Single-photon sources play a key role in photonic quantum technologies. Semiconductor quantum dots can emit indistinguishable single photons under resonant excitation. However, the resonance fluorescence technique typically requires cross-polarization filtering, which causes a loss of the unpolarized quantum dot emission by 50%. To solve this problem, we demonstrate a method for generating indistinguishable single photons with optically controlled polarization by two laser pulses off-resonant with neutral exciton states. This scheme is realized by exciting the quantum dot to the biexciton state and subsequently driving the quantum dot to an exciton eigenstate. By combining with a magnetic field, we demonstrated the generation of photons with optically controlled polarization (the degree of polarization is 101(2)%), laser-neutral exciton detuning up to 0.81 meV, high single-photon purity (99.6(1)%), and indistinguishability (85(4)%). Laser pulses can be blocked using polarization and spectral filtering. Our work makes an important step toward indistinguishable single-photon sources with near-unity collection efficiency.

Rhodium-Catalyzed Reaction of Silacyclobutanes with Unactivated Alkynes to Afford Silacyclohexenes.

A Rh-catalyzed reaction of silacyclobutanes (SCBs) with unactivated alkynes has been developed to form silacyclohexenes with high chemoselectivity. Good enantioselectivity at the stereogenic silicon center was achieved using a chiral phosphoramidite ligand. The resulting silacyclohexenes are useful scaffolds for synthesizing structurally attractive silacyclic compounds.

Controllable Si-C Bond Formation from Trihydrosilanes En Route to Synthesis of 1,4-Azasilinanes with Diverse Silyl Functionalities.

A B(C6F5)3-catalyzed controllable inter/intra-/intermolecular Si-C bond formation process has been developed from trihydrosilane and dienamide with alkenes, anilines, or aryl iodides. A variety of 1,4-azasilinanes have been generated with diverse exo-cyclic heteroleptic disubstitutions on silicon, thereby expanding the range of silaazacyclic rings available for the discovery of silicon-containing drugs.

Telecom-band quantum dot technologies for long-distance quantum networks.

A future quantum internet is expected to generate, distribute, store and process quantum bits (qubits) over the world by linking different quantum nodes via quantum states of light. To facilitate long-haul operations, quantum repeaters must operate at telecom wavelengths to take advantage of both the low-loss optical fibre network and the established technologies of modern optical communications. Semiconductor quantum dots have thus far shown exceptional performance as key elements for quantum repeaters, such as quantum light sources and spin-photon interfaces, but only in the near-infrared regime. Therefore, the development of high-performance telecom-band quantum dot devices is highly desirable for a future solid-state quantum internet based on fibre networks. In this Review, we present the physics and technological developments towards epitaxial quantum dot devices emitting in the telecom O- and C-bands for quantum networks, considering both advanced epitaxial growth for direct telecom emission and quantum frequency conversion for telecom-band down-conversion of near-infrared quantum dot devices. We also discuss the challenges and opportunities for future realization of telecom quantum dot devices with improved performance and expanded functionality through hybrid integration.

Bright semiconductor single-photon sources pumped by heterogeneously integrated micropillar lasers with electrical injections.

The emerging hybrid integrated quantum photonics combines the advantages of different functional components into a single chip to meet the stringent requirements for quantum information processing. Despite the tremendous progress in hybrid integrations of III-V quantum emitters with silicon-based photonic circuits and superconducting single-photon detectors, on-chip optical excitations of quantum emitters via miniaturized lasers towards single-photon sources (SPSs) with low power consumptions, small device footprints, and excellent coherence properties is highly desirable yet illusive. In this work, we present realizations of bright semiconductor SPSs heterogeneously integrated with on-chip electrically-injected microlasers. Different from previous one-by-one transfer printing technique implemented in hybrid quantum dot (QD) photonic devices, multiple deterministically coupled QD-circular Bragg Grating (CBG) SPSs were integrated with electrically-injected micropillar lasers at one time via a potentially scalable transfer printing process assisted by the wide-field photoluminescence (PL) imaging technique. Optically pumped by electrically-injected microlasers, pure single photons are generated with a high-brightness of a count rate of 3.8 M/s and an extraction efficiency of 25.44%. Such a high-brightness is due to the enhancement by the cavity mode of the CBG, which is confirmed by a Purcell factor of 2.5. Our work provides a powerful tool for advancing hybrid integrated quantum photonics in general and boosts the developments for realizing highly-compact, energy-efficient and coherent SPSs in particular.

Efficient second harmonic generation by harnessing bound states in the continuum in semi-nonlinear etchless lithium niobate waveguides.

Integrated photonics provides unprecedented opportunities to pursue advanced nonlinear light sources with low-power consumptions and small footprints in a scalable manner, such as microcombs, chip-scale optical parametric oscillators and integrated quantum light sources. Among a variety of nonlinear optical processes, high-efficiency second harmonic generation (SHG) on-chip is particularly appealing and yet challenging. In this work, we present efficient SHG in highly engineerable semi-nonlinear waveguides consisting of electron-beam resist waveguides and thin-film silicon nitride (SiN)/lithium niobate (LN). By carefully designing octave-separating bound states in the continuum (BICs) for the nonlinear interacting waves in such a hybrid structure, we have simultaneously optimized the losses for both fundamental frequency (FF) and second harmonic (SH) waves and achieved modal phasing matching and maximized the nonlinear modal overlap between the FF and SH waves, which results in an experimental conversion efficiency up to 4.05% W-1cm-2. Our work provides a versatile and fabrication-friendly platform to explore on-chip nonlinear optical processes with high efficiency in the context of nanophotonics and quantum optics.

Tailoring solid-state single-photon sources with stimulated emissions.

The coherent interaction of electromagnetic fields with solid-state two-level systems can yield deterministic quantum light sources for photonic quantum technologies. To date, the performance of semiconductor single-photon sources based on three-level systems is limited mainly due to a lack of high photon indistinguishability. Here we tailor the cavity-enhanced spontaneous emission from a ladder-type three-level system in a single epitaxial quantum dot through stimulated emission. After populating the biexciton (XX) of the quantum dot through two-photon resonant excitation, we use another laser pulse to selectively depopulate the XX state into an exciton (X) state with a predefined polarization. The stimulated XX-X emission modifies the X decay dynamics and improves the characteristics of a polarized single-photon source, such as a source brightness of 0.030(2), a single-photon purity of 0.998(1) and an indistinguishability of 0.926(4). Our method can be readily applied to existing quantum dot single-photon sources and expands the capabilities of three-level systems for advanced quantum photonic functionalities.

Dual-resonance enhanced quantum light-matter interactions in deterministically coupled quantum-dot-micropillars.

Optical microcavities have widely been employed to enhance either the optical excitation or the photon emission processes for boosting light-matter interactions at the nanoscale. When both the excitation and emission processes are simultaneously facilitated by the optical resonances provided by the microcavities, as referred to the dual-resonance condition in this article, the performances of many nanophotonic devices approach to the optima. In this work, we present versatile accessing of dual-resonance conditions in deterministically coupled quantum-dot (QD)-micropillars, which enables emission from neutral exciton (X)-charged exciton (CX) transition with improved single-photon purity. In addition, the rarely observed up-converted single-photon emission process is achieved under dual-resonance conditions. We further exploit the vectorial nature of the high-order cavity modes to significantly improve the excitation efficiency under the dual-resonance condition. The dual-resonance enhanced light-matter interactions in the quantum regime provide a viable path for developing integrated quantum photonic devices based on cavity quantum electrodynamics (QED) effect, e.g., highly efficient quantum light sources and quantum logical gates.

Directional and Fast Photoluminescence from CsPbI3 Nanocrystals Coupled to Dielectric Circular Bragg Gratings.

Lead halide perovskite nanocrystals (NCs), especially the all-inorganic perovskite NCs, have drawn substantial attention for both fundamental research and device applications in recent years due to their unique optoelectronic properties. To build high-performance nanophotonic devices based on perovskite NCs, it is highly desirable to couple the NCs to photonic nanostructures for enhancing the radiative emission rate and improving the emission directionality of the NCs. In this work, we synthesized high-quality CsPbI3 NCs and further coupled them to dielectric circular Bragg gratings (CBGs). The efficient couplings between the perovskite NCs and the CBGs resulted in a 45.9-fold enhancement of the photoluminescence (PL) intensity and 3.2-fold acceleration of the radiative emission rate. Our work serves as an important step for building high-performance nanophotonic light emitting devices by integrating perovskite NCs with photonic nanostructures.

Bright solid-state sources for single photons with orbital angular momentum.

Photons that have a helical phase front, that is, twisted photons, can carry a discrete, in principle, unlimited, but quantized amount of orbital angular momentum (OAM). Hence, twisted single photons constitute a high-dimensional quantum system with information-processing abilities beyond those of two-level single-photon qubits. To date, the generation of single photons carrying OAM has relied on a non-linear process in bulk crystals, for example, spontaneous parametric down-conversion, which limits both the efficiency and the scalability of the source. Here, we present a bright solid-state source of single photons in an OAM superposition state with a single-photon purity of g(2)(0) = 0.115(1) and a collection efficiency of 23(4)%. The mode purity of the single-photon OAM states is further examined via projection measurements. Future developments of integrated quantum photonic devices with pure OAM states as an additional degree of freedom may enable high-dimensional quantum information processing.

ArNMeCH(SiMe3)2: a useful precursor of formal α-aminoalkyl diradicals in visible-light-mediated homo- and hetero-diaddition with alkenes.

ArNMeCH(SiMe3)2 has been developed as a useful precursor of a formal α-aminoalkyl diradical in Ru(bpy)3Cl2-catalzyed addition with alkenes under visible-light-mediated photoredox conditions. This approach leads to homo-diaddition with two identical alkenes in one-pot, or hetero-diaddition with two different alkenes via a sequential operation.

Quantum Frequency Conversion of a Quantum Dot Single-Photon Source on a Nanophotonic Chip.

Single self-assembled InAs/GaAs quantum dots are promising bright sources of indistinguishable photons for quantum information science. However, their distribution in emission wavelength, due to inhomogeneous broadening inherent to their growth, has limited the ability to create multiple identical sources. Quantum frequency conversion can overcome this issue, particularly if implemented using scalable chip-integrated technologies. Here, we report the first demonstration of quantum frequency conversion of a quantum dot single-photon source on a silicon nanophotonic chip. Single photons from a quantum dot in a micropillar cavity are shifted in wavelength with an on-chip conversion efficiency ≈ 12 %, limited by the linewidth of the quantum dot photons. The intensity autocorrelation function g(2)(τ) for the frequency-converted light is antibunched with g(2)(0)=0.290±0.030, compared to the before-conversion value g(2)(0)=0.080±0.003. We demonstrate the suitability of our frequency conversion interface as a resource for quantum dot sources by characterizing its effectiveness across a wide span of input wavelengths (840 nm to 980 nm), and its ability to achieve tunable wavelength shifts difficult to obtain by other approaches.

High-efficiency broadband second harmonic generation in single hexagonal GaAs nanowire.

In this paper, we investigate second harmonic generation in a single hexagonal GaAs nanowire. An excellent frequency converter based on this nanowire excited using a femtosecond laser is demonstrated to operate over a range from 730 nm to 1960 nm, which is wider than previously reported ranges for nanowires in the literature. The converter always operates with a high conversion efficiency of ~10-5 W-1 which is ~103 times higher than that obtained from the surface of bulk GaAs. This nanoscale nolinear optical converter that simultaneously owns high efficiency and broad bandwidth may open a new way for application in imaging, bio-sensing and on-chip all-optical signal processing operations.

A deterministic quantum dot micropillar single photon source with >65% extraction efficiency based on fluorescence imaging method.

We report optical positioning of single quantum dots (QDs) in planar distributed Bragg reflector (DBR) cavity with an average position uncertainty of ≈20 nm using an optimized photoluminescence imaging method. We create single-photon sources based on these QDs in determined micropillar cavities. The brightness of the QD fluorescence is greatly enhanced on resonance with the fundamental mode of the cavity, leading to an high extraction efficiency of 68% ± 6% into a lens with numerical aperture of 0.65, and simultaneously exhibiting low multi-photon probability (g(2)(0) = 0.144 ± 0.012) at this collection efficiency.