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The trigonal planar unit possesses significant hyperpolarizability and polarizability anisotropy, which makes it useful for optimizing nonlinear optical (NLO) materials, however, chalcogenide with this unit has seldom been reported. In this work, a novel approach is introduced by integrating the unprecedented trigonal planar MS 3 (M = Cd/In, Hg/In) motifs into the nearly optically isotropic tetrahedral units, resulting in two novel chalcogenides CsM 2 In 2 S 6 (M = Cd/In, 1; Hg/In, 2). Notably, structures 1 and 2 feature nearly planar triangular units at the center, encircled by three trimers, further interconnecting each other to create 3D frameworks. Importantly, phases 1 and 2 display phase-matching (PM) capabilities, primarily attributed to incorporating trigonal planar MS 3 units that additionally enhance polarizability anisotropy. Furthermore, compounds 1 and 2 demonstrate moderate second-harmonic generation (SHG) signals (0.70 and 0.84 × AgGaS2@1.7 µm). This study pioneers an efficient strategy for the design of infrared NLO crystals with PM capabilities., (© 2024 Wiley‐VCH GmbH.)

The measurement of a laser linewidth is significant in metrology, coherent optical communications, high-resolution sensing, and LIDAR. Firstly, in this study, we theoretically explain why estimating an integrated linewidth via a frequency-noise power spectral density (PSD) is valid. We find that the previous methods estimating the integrated linewidth via the frequency-noise PSD result from Gaussian approximation and obtain a more general consequence. Secondly, according to the theory, we propose the Voigt approximation method to improve the estimation performance. The simulation results show the Voigt approximation estimation error is lower than 5%. Finally, based on the Voigt approximation, the relationship between the interference visibility and laser linewidth is found, providing a possible convenient approach to measuring the linewidth.

The generation of cold molecules is an important topic in the field of cold atoms and molecules and has received relevant advanced research attention in ultracold chemistry, quantum computation, and quantum metrology. With a high atomic phase space density, optical dipole traps have been widely used to prepare, trap, and study cold molecules. In this work, Rb2 molecules were photoassociated in a magneto-optical trap to obtain a precise rovibrational spectrum, which provided accurate numerical references for the realization of multiple frequency photoassociation. By meeting the harsh requirements of photoassociation in optical dipole traps, the cold molecule photoassociation process was well explored, and different photoassociation resonances were simultaneously addressed in a single optical dipole trap. This method can be universally extended to simultaneously photoassociate cold molecules with different internal states or atomic species in a single optical dipole trap, thus advancing generous cold molecule studies such as cold molecule collision dynamics., (© 2024 Author(s). Published under an exclusive license by AIP Publishing.)

In practical sensing tasks, noise is usually regarded as an obstacle that degrades the sensitivity. Fortunately, stochastic resonance can counterintuitively harness noise to notably enhance the output signal-to-noise ratio in a nonlinear system. Although stochastic resonance has been extensively studied in various disciplines, its potential in realistic sensing tasks remains largely unexplored. Here, we propose and demonstrate a noise-enhanced microwave sensor using a thermal ensemble of interacting Rydberg atoms. Using the strong nonlinearity present in the Rydberg ensembles and leveraging stochastic noises in the system, we demonstrate the stochastic resonance driven by a weak microwave signal (from several microvolts per centimeter to millivolts per centimeter). A substantial enhancement in the detection is achieved, with a sensitivity surpassing that of a heterodyne atomic sensor by 6.6 decibels. Our results offer a promising platform for investigating stochastic resonance in practical sensing scenarios.

Efficient removal of acetylene (C 2 H 2 ) impurities from polymer-grade ethylene (C 2 H 4 ) in a simple, clean manner remains a challenging goal in industry. The use of porous materials such as metal-organic frameworks (MOFs) is promising for this aim but the acquisition of high purification performance is still hindered by few knowledge on the purification process because the previous conclusions were derived basically from the non-breakthrough tests or ignored the influence of structural difference (crystal structure, morphology, or defect). Here we propose an unprecedented in situ stimulus response strategy to minimize the influence of structural difference, obtain the gas-loading crystal structures of the same MOF before and after light or heat stimulation, directly observe the evolution of pore charge distribution and pore⋅⋅⋅gas interactions under light/heat induction, and finally summarizes the favorable structure for highly efficient purification of C 2 H 4 . This study opens a new route to understand the relationship between the structure and separation performance for porous materials., (© 2024 Wiley-VCH GmbH.)

Detecting a microwave signal that is emitted or reflected by distant targets is a powerful tool in fundamental science and industrial technology. Solid-state spins provide an opportunity to realize quantum-enhanced remote sensing under ambient conditions. However, the weak interaction between the free-space signal and atomic size sensor limits the sensitivity. This hinders the realization of practical quantum remote sensing. Here, we demonstrate active microwave remote sensing with a diamond-based hybrid quantum receiver by combining electromagnetic field localization at nanoscale with quantum spin manipulation. A method of differential spin refocusing (DSR) is developed to overcome the challenge of reducing the impact of inhomogeneities in spin-signal interaction, while the strength of interaction is enhanced by more than 3 orders with nanostructure. It improves the coherent interaction time of quantum receiver by 30-fold, substantially enhancing the sensitivity and stability. By detecting the reflected microwave with picotesla sensitivity, diamond remote sensing monitors the real-time status of a centimeter-sized target at 2 m distance. Our method is general to various solid-state spins. The results will expand the applications of solid-state spin quantum sensors in areas ranging from medical imaging to resource survey.

The manipulation and transformation of quantum resources are key parts of quantum mechanics. Among them, asymmetry is one of the most useful operational resources, which is widely used in quantum clocks, quantum metrology, and other tasks. Recent studies have shown that the asymmetry of quantum states can be significantly amplified with the assistance of correlating catalysts that are finite-dimensional auxiliaries. In the experiment, we perform translationally invariant operations, ensuring that the asymmetric resources of the entire system remain nonincreasing, on a composite system composed of a catalytic system and a quantum system. The experimental results demonstrate an asymmetry amplification of 0.0172±0.0022 in the system following the catalytic process. Our Letter showcases the potential of quantum catalytic processes and is expected to inspire further research in the field of quantum resource theories.

Quantum networks provide a prospective paradigm to connect separated quantum nodes, which relies on the distribution of long-distance entanglement and active feedforward control of qubits between remote nodes. Such approaches can be utilized to construct nonlocal quantum gates, forming building blocks for distributed quantum computing and other novel quantum applications. However, these gates have only been realized within single nodes or between nodes separated by a few tens of meters, limiting the ability to harness computing resources in large-scale quantum networks. Here, we demonstrate nonlocal photonic quantum gates between two nodes spatially separated by 7.0 km using stationary qubits based on multiplexed quantum memories, flying qubits at telecom wavelengths, and active feedforward control based on field-deployed fibers. Furthermore, we illustrate quantum parallelism by implementing the Deutsch-Jozsa algorithm and the quantum phase estimation algorithm between the two remote nodes. These results represent a proof-of-principle demonstration of quantum gates over metropolitan-scale distances and lay the foundation for the construction of large-scale distributed quantum networks relying on existing fiber channels., (© 2024. The Author(s).)

Infrared birefringent crystals that hold significant importance for optoelectronic application have been rarely reported. Traditional tetrahedral PS 4 , ethane-like P 2 S 6 , and octahedral InS 6 units in thiophosphates typically manifest near isotropy, often resulting in extremely small birefringence. However, this study prepares α-Rb 2 InP 2 S 7 (1), β-Rb 2 InP 2 S 7 (2), and Cs 2 InP 2 S 7 (3), consisting of the aforementioned microstructures, notably exhibiting the highest refractive index difference or birefringence values (0.247, 0.298, and 0.250 at 546 nm, respectively) among thiophosphates, the middle one being larger than that of commercial birefringent materials. This unusual increase in birefringence can be primarily attributed to two key factors: (1) simultaneous stretching and compressing of the P-S and In-S covalent bond interactions, generating high polarizability anisotropy of InS 6 , PS 4 , and P 2 S 6 polyhedral units; (2) the additional incorporation of alkali metals that further reduces the dimensionality of the crystal structure, creating one-dimensional [InP 2 S 7 ] 2- structures with increasing polarizability anisotropy. This study presents an alternative approach to enhance birefringent materials by reconstructing covalent bond interactions and specific spatial arrangements., Competing Interests: The authors declare no competing financial interest., (This journal is © The Royal Society of Chemistry.)

The fluorescence collection from single atoms and emitters has been extensively utilized in quantum information and quantum optics research. Here, we investigated the collection efficiency of an objective lens by drawing an analogy between the free-space beam (FSB) and a waveguide mode. We explored how efficiency is influenced by their thermal motion within a dipole trap. Furthermore, we introduce an effective energy fraction ratio to quantify potential imperfections in the focusing of the objective lens. Our results provide valuable insights for optimizing the fluorescence collection in single-atom experiments and highlight the importance of considering realistic experimental conditions when estimating achievable efficiencies.

Quantum interference is a natural consequence of wave-particle duality in quantum mechanics, and is widely observed at the atomic scale. One interesting manifestation of quantum interference is coherent population trapping (CPT), first proposed in three-level driven atomic systems and observed in quantum optical experiments. Here, we demonstrate CPT in a gate-defined semiconductor double quantum dot (DQD), with some unique twists as compared to the atomic systems. Specifically, we observe CPT in both driven and nondriven situations. We further show that CPT in a driven DQD could be used to generate adiabatic state transfer. Moreover, our experiment reveals a nontrivial modulation to the CPT caused by the longitudinal driving field, yielding an odd-even effect and a tunable CPT. Our results broaden the field of CPT, and open up the possibility of quantum simulation and quantum computation based on adiabatic passage in quantum dot systems.

Metals containing d-orbitals are typically characterized by strong deformation and polarization, yet they tend to induce narrow bandgaps that render them little-appreciated by high-power nonlinear optical (NLO) crystals. Incorporating highly electropositive polycations into d-orbital-containing chalcogenides to modify them into salt-inclusion chalcogenides (SICs) that are competitive in NLO materials, is a viable solution to this predicament. In the present work, two isostructural SICs [K 4 Cl][MGa 9 S 16 ] (M = Mn, 1; Hg, 2) are successfully synthesized by the high-temperature molten-salt growth method. Both compounds demonstrate commendable second-harmonic-generation (SHG) responses (0.6-1.0 × AgGaS 2 @1910 nm), which can be attributed to their well-designed [MGa 9 S 16 ] 3- anionic frameworks; and compound 2 exhibits the widest optical bandgap (3.41 eV) among the Hg-based NLO chalcogenides. Also, an interesting dual-band photoluminescence emission centered at ∼650 and ∼718 nm is detected in 1 at 77 K, with long lifetimes of 0.94 and 1.35 ms, respectively., Competing Interests: There are no conflicts to declare., (This journal is © The Royal Society of Chemistry.)

With an extremely high dimensionality, the spatial degree of freedom of entangled photons is a key tool for quantum foundation and applied quantum techniques. To fully utilize the feature, the essential task is to experimentally characterize the multiphoton spatial wave function including the entangled amplitude and phase information at different evolutionary stages. However, there is no effective method to measure it. Quantum state tomography is costly, and quantum holography requires additional references. Here, we introduce quantum Shack-Hartmann wavefront sensing to perform efficient and reference-free measurement of the biphoton spatial wave function. The joint probability distribution of photon pairs at the back focal plane of a microlens array is measured and used for amplitude extraction and phase reconstruction. In the experiment, we observe that the biphoton amplitude correlation becomes weak while phase correlation shows up during free-space propagation. Our work is a crucial step in quantum physical and adaptive optics and paves the way for characterizing quantum optical fields with high-order correlations or topological patterns.

An approach for continuous tuning of on-chip optical delay with a microring resonator is proposed and demonstrated. By introducing an electro-optically tunable waveguide coupler, the bus waveguide to the resonance coupling can be effectively tuned from the under-coupling regime to the over-coupling regime. The optical delay is experimentally characterized by measuring the relative phase shift between lasers and shows a large dynamic range of delay from -600 to 600 ps and an efficient tuning of delay from -430 to -180 ps and from 40 to 240 ps by only a 5 V voltage.

The construction of secondary building units (SBUs) in versatile metal-organic frameworks (MOFs) represents a promising method for developing multi-functional materials, especially for improving their sensitizing ability. Herein, we developed a dual small molecules auxiliary strategy to construct a high-nuclear transition-metal-based UiO-architecture Co 16 -MOF-BDC with visible-light-absorbing capacity. Remarkably, the N 3 - molecule in hexadecameric cobalt azide SBU offers novel modification sites to precise bonding of strong visible-light-absorbing chromophores via click reaction. The resulting Bodipy@Co 16 -MOF-BDC exhibits extremely high performance for oxidative coupling benzylamine (~100 % yield) via both energy and electron transfer processes, which is much superior to that of Co 16 -MOF-BDC (31.5 %) and Carboxyl @Co 16 -MOF-BDC (37.5 %). Systematic investigations reveal that the advantages of Bodipy@Co 16 -MOF-BDC in dual light-absorbing channels, robust bonding between Bodipy/Co 16 clusters and efficient electron-hole separation can greatly boost photosynthesis. This work provides an ideal molecular platform for synergy between photosensitizing MOFs and chromophores by constructing high-nuclear transition-metal-based SBUs with surface-modifiable small molecules., (© 2024 Wiley-VCH GmbH.)

Measurement device independent quantum key distribution (MDI QKD) has attracted growing attention for its immunity to attacks at the measurement unit, but its unique structure limits the secret key rate. Utilizing the wavelength division multiplexing (WDM) technique and reducing error rates are effective strategies for enhancing the secret key rate. Reducing error rates often requires active feedback control of wavelengths using precise external references. However, for a multiwavelength laser, employing multiple references to stabilize each wavelength output places stringent demands on these references and significantly increases system complexity. Here, we demonstrate a stable, wavelength-tunable multiwavelength laser with an output wavelength ranging from 1270 to 1610 nm. Through precise temperature control and stable drive current, we passively lock the laser wavelength, achieving remarkable wavelength stability. This significantly reduce the error rate, leading to an almost doubling of the secret key rate compared to previous experiments. Furthermore, the exceptional wavelength stability offered by our multiwavelength laser, combined with the WDM technique, has further boosted the secret key rate of MDI QKD. With a wide wavelength tuning range of 5.1 nm, our multiwavelength laser facilitates flexible operation across multiple dense wavelength division multiplexing channels. Coupled with high wavelength stability and multiple wavelength outputs simultaneously, this laser offers a promising solution for a high-rate MDI QKD system., (© 2024 Author(s). Published under an exclusive license by AIP Publishing.)

Einstein-Podolsky-Rosen (EPR) steering, a distinctive quantum correlation, reveals a unique and inherent asymmetry. This research delves into the multifaceted asymmetry of EPR steering within high-dimensional quantum systems, exploring both theoretical frameworks and experimental validations. We introduce the concept of genuine high-dimensional one-way steering, wherein a high Schmidt number of bipartite quantum states is demonstrable in one steering direction but not reciprocally. Additionally, we explore two criteria to certify the lower and upper bounds of the Schmidt number within a one-sided device-independent context. These criteria serve as tools for identifying potential asymmetric dimensionality of EPR steering in both directions. By preparing two-qutrit mixed states with high fidelity, we experimentally observe asymmetric structures of EPR steering in the C^{3}⊗C^{3} Hilbert space. Our Letter offers new perspectives to understand the asymmetric EPR steering beyond qubits and has potential applications in asymmetric high-dimensional quantum information tasks.

Quantum entanglement and decoherence are the two counterforces of many quantum technologies and protocols. For example, while quantum teleportation is fueled by a pair of maximally entangled resource qubits, it is vulnerable to decoherence. Here, we propose an efficient quantum teleportation protocol in the presence of pure decoherence and without entangled resource qubits entering the Bell-state measurement. Instead, we use multipartite hybrid entanglement between the auxiliary qubits and their local environments within the open-quantum system context. With a hybrid-entangled initial state, it is the decoherence that allows us to achieve high fidelities. We demonstrate our protocol in an all-optical experiment.

Photonic integrated quantum memories are essential for the construction of scalable quantum networks. Spin-wave quantum storage, which can support on-demand retrieval with a long lifetime, is indispensable for practical applications, but has never been demonstrated in an integrated solid-state device. Here, we demonstrate spin-wave quantum storage based on a laser-written waveguide fabricated in a 151 Eu 3+ :Y 2 SiO 5 crystal, using both the atomic frequency comb and noiseless photon-echo protocols. Qubits encoded with single-photon-level inputs are stored and retrieved with a fidelity of [Formula: see text], which is far beyond the maximal fidelity that can be obtained with any classical device. Our results underline the potential of laser-written integrated devices for practical applications in large-scale quantum networks, such as the construction of multiplexed quantum repeaters in an integrated configuration and high-density transportable quantum memories., (© The Author(s) 2024. Published by Oxford University Press on behalf of China Science Publishing & Media Ltd.)

Phonon-based frequency combs that can be generated in the optical and microwave frequency domains have attracted much attention due to the small repetition rates and the simple setup. Here, we experimentally demonstrate a new type of phonon-based frequency comb in a silicon optomechanical crystal cavity including both a breathing mechanical mode (∼GHz) and flexural mechanical modes (tens of MHz). We observe strong mode competition between two approximate flexural mechanical modes, i.e., 77.19 and 90.17 MHz, resulting in only one preponderant lasing, while maintaining the lasing of the breathing mechanical mode. These simultaneous observations of two-mode phonon lasing state and significant mode competition are counterintuitive. We have formulated comprehensive theories to elucidate this phenomenon in response to this intriguing outcome. In particular, the self-pulse induced by the free carrier dispersion and thermo-optic effects interacts with two approximate flexural mechanical modes, resulting in the repetition rate of the comb frequency-locked to exact fractions of one of the flexural mechanical modes and the mode hopping between them. This phonon-based frequency comb has at least 260 comblines and a repetition rate as low as a simple fraction of the flexural mechanical frequency. Our demonstration offers an alternative optomechanical frequency comb for sensing, timing, and metrology applications.

Quantum theory allows information to flow through a single device in a coherent superposition of two opposite directions, resulting into situations where the input-output direction is indefinite. Here we introduce a theoretical method to witness input-output indefiniteness in a single quantum device, and we experimentally demonstrate it by constructing a photonic setup that exhibits input-output indefiniteness with a statistical significance exceeding 69 standard deviations. Our results provide a way to characterize input-output indefiniteness as a resource for quantum information and photonic quantum technologies and enable tabletop simulations of hypothetical scenarios exhibiting quantum indefiniteness in the direction of time.

Soliton microcombs are regarded as an ideal platform for applications such as optical communications, optical sensing, low-noise microwave sources, optical atomic clocks, and frequency synthesizers. Many of these applications require a broad comb spectrum that covers an octave, essential for implementing the f - 2f self-referencing techniques. In this work, we have successfully generated an octave-spanning soliton microcomb based on a z-cut thin-film lithium niobate (TFLN) microresonator. This achievement is realized under on-chip optical pumping at 340 mW and through extensive research into the broadening of dual dispersive waves (DWs). Furthermore, the repetition rate of the octave soliton microcomb is accurately measured using an electro-optic comb generated by an x-cut TFLN racetrack microresonator. Our results represent a crucial step toward the realization of practical, integrated, and fully stabilized soliton microcomb systems based on TFLN.

An integrated quantum light source is increasingly desirable in large-scale quantum information processing. Despite recent remarkable advances, a new material platform is constantly being explored for the fully on-chip integration of quantum light generation, active and passive manipulation, and detection. Here, for the first time, we demonstrate a gallium nitride (GaN) microring based quantum light generation in the telecom C-band, which has potential toward the monolithic integration of quantum light source. In our demonstration, the GaN microring has a free spectral range of 330 GHz and a near-zero anomalous dispersion region of over 100 nm. The generation of energy-time entangled photon pair is demonstrated with a typical raw two-photon interference visibility of 95.5±6.5%, which is further configured to generate a heralded single photon with a typical heralded second-order autocorrelation g_{H}^{(2)}(0) of 0.045±0.001. Our results pave the way for developing a chip-scale quantum photonic circuit.

Birefringent materials are of great significance to the development of modern optical technology; however, research on halide birefringent crystals with a wide transparent range remains limited. In this work, mercuric bromide (HgBr 2 ) has been investigated for the first time as a promising birefringent material with a wide transparent window spanning from ultraviolet (UV) to far-infrared (far-IR) spectral regions (0.34-22.9 μm). HgBr 2 has an exceptionally large birefringence (Δ n , 0.235 @ 546 nm), which is 19.6 times that of commercial MgF 2 . The ordered linear motif [Br-Hg-Br] with high polarizability anisotropy within the molecule is the inherent source of excellent birefringence, making it an efficient building block for birefringent materials. In addition, HgBr 2 can be easily grown under mild conditions and remain stable in air for prolonged periods. Studying the birefringent properties of HgBr 2 crystals would provide new ideas for future exploration of wide-spectrum birefringent materials., Competing Interests: There are no conflicts to declare., (This journal is © The Royal Society of Chemistry.)

Reducing the average resource consumption is the central quest in discriminating non-orthogonal quantum states for a fixed admissible error rate ϵ. The globally optimal fixed local projective measurement for this task is found to be different from that for previous minimum-error discrimination tasks [S. Slussarenko et al., Phys. Rev. Lett. 118, 030502 (2017)PRLTAO0031-900710.1103/PhysRevLett.118.030502]. To achieve the ultimate minimum average consumption, here we develop a general globally optimal adaptive strategy (GOA) by subtly using the updated posterior probability, which works under any error rate requirements and any one-way measurement restrictions, and can be solved by a convergent iterative relation. First, under the local measurement restrictions, our GOA is solved to serve as the local bound, which saves 16.6 copies (24%) compared with the previously best globally optimal fixed local projective measurement. When the more powerful two-copy collective measurements are allowed, our GOA is experimentally demonstrated to beat the local bound by 3.9 copies (6.0%). By exploiting both adaptivity and collective measurements, our Letter marks an important step toward minimum-consumption quantum state discrimination.

Noise-enhanced applications in open quantum walk (QW) has recently seen a surge due to their ability to improve performance. However, verifying the success of open QW is challenging, as mixed-state tomography is a resource-intensive process, and implementing all required measurements is almost impossible due to various physical constraints. To address this challenge, we present a neural-network-based method for reconstructing mixed states with a high fidelity (∼97.5%) while costing only 50% of the number of measurements typically required for open discrete-time QW in one dimension. Our method uses a neural density operator that models the system and environment, followed by a generalized natural gradient descent procedure that significantly speeds up the training process. Moreover, we introduce a compact interferometric measurement device, improving the scalability of our photonic QW setup that enables experimental learning of mixed states. Our results demonstrate that highly expressive neural networks can serve as powerful alternatives to traditional state tomography.

Photonic quantum computation plays an important role and offers unique advantages. Two decades after the milestone work of Knill-Laflamme-Milburn, various architectures of photonic processors have been proposed, and quantum advantage over classical computers has also been demonstrated. It is now the opportune time to apply this technology to real-world applications. However, at current technology level, this aim is restricted by either programmability in bulk optics or loss in integrated optics for the existing architectures of processors, for which the resource cost is also a problem. Here we present a von-Neumann-like architecture based on temporal-mode encoding and looped structure on table, which is capable of multimode-universal programmability, resource-efficiency, phase-stability and software-scalability. In order to illustrate these merits, we execute two different programs with varying resource requirements on the same processor, to investigate quantum signature of chaos from two aspects: the signature behaviors exhibited in phase space (13 modes), and the Fermi golden rule which has not been experimentally studied in quantitative way before (26 modes). The maximal program contains an optical interferometer network with 1694 freely-adjustable phases. Considering current state-of-the-art, our architecture stands as the most promising candidate for real-world applications., (© 2024. The Author(s).)

On-chip acousto-optic modulators that operate at an optical wavelength of 780 nm and a microwave frequency of 6.835 GHz are proposed. The modulators are based on a lithium-niobate-on-sapphire platform and efficiently excite surface acoustic waves and exhibit strong interactions with tightly confined optical modes in waveguides. In particular, a high-efficiency phase modulator and single-sideband mode converter are designed. We found that for both microwave and optical wavelengths below 1 µm, the interactions at the cross-sections of photonic waveguides are sensitive to the waveguide width and are significantly different from those in previous studies. Our designed devices have small footprints and high efficiencies, making them suitable for controlling rubidium atoms and realizing hybrid photonic-atomic chips. Furthermore, our devices have the potential to extend the acousto-optic modulators to other visible wavelengths for other atom transitions and for visible light applications, including imaging and sensing.

Reducing the dark current of photodetectors is an important strategy for enhancing the detection sensitivity, but hampered by the manufacturing cost due to the need for controlling the complex material composition and processing intricate interface. This study reports a new single-component photochromic semiconductor, [(HDMA) 4 (Pb 3 Br 10 )(PhSQ) 2 ] n (1, HDMA = dimethylamine cation, PhSQ = 1-(4-sulfophenyl)-4,4'-bipyridinium), by introducing a redox-active monosubstituted viologen zwitterion into inorganic semiconducting skeleton. It features yellow to green coloration after UV irradiation with the sharply dropping intrinsic conductivity of 14.6-fold, and the photodetection detection sensitivity gain successfully doubles. The reason of decreasing conductivity originates from the increasing the band gap of the inorganic semiconducting component and formation of Frenkel excitons with strong Coulomb interactions, thereby decreasing the concentration of thermally excited intrinsic carriers., (© 2023 Wiley‐VCH GmbH.)

Quantum measurements based on mutually unbiased bases (MUBs) play crucial roles in foundational studies and quantum information processing. It is known that there exist inequivalent MUBs, but little is known about their operational distinctions, not to say experimental demonstration. In this Letter, by virtue of a simple estimation problem, we experimentally demonstrate the operational distinctions between inequivalent triples of MUBs in dimension 4 based on high-precision photonic systems. The experimental estimation fidelities coincide well with the theoretical predictions with only 0.16% average deviation, which is 25 times less than the difference (4.1%) between the maximum estimation fidelity and the minimum estimation fidelity. Our experiments clearly demonstrate that inequivalent MUBs have different information extraction capabilities and different merits for quantum information processing.

Uncertainty relations for Hermitian operators have been confirmed through many experiments. However, previous experiments have only tested the special case of non-Hermitian operators, i.e., uncertainty relations for unitary operators. In this study, we explore uncertainty relations for general non-Hermitian operators, which include Hermitian and unitary operators as special cases. We perform experiments with both real and complex non-Hermitian operators for qubit states, and confirm the validity of the uncertainty relations within the experimental error. Our results provide experimental evidence of uncertainty relations for non-Hermitian operators. Furthermore, our methods for realizing and measuring non-Hermitian operators are valuable in characterizing open-system dynamics and enhancing parameter estimation.

The study of facile-synthesis and low-cost X-ray scintillators with high light yield, low detection limit and high X-ray imaging resolution plays a vital role in medical and industrial imaging fields. However, the optimal balance between X-ray absorption, decay lifetime and excitonic utilization efficiency of scintillators to achieve high-resolution imaging is extremely difficult due to the inherent contradiction. Here two thermally activated delayed fluorescence (TADF)-actived coinage-metal clusters M 6 S 6 L 6 (M=Ag or Cu) were synthesized by simple solvothermal reaction, where the cooperation of heavy atom-rich character and TADF mechanism supports strong X-ray absorption and rapid luminescent collection of excitons. Excitingly, Ag 6 S 6 L 6 (SC-Ag) displays a high photoluminescence quantum yield of 91.6 % and scintillating light yield of 17420 photons MeV -1 , as well as a low detection limit of 208.65 nGy s -1 that is 26 times lower than the medical standard (5.5 μGy s -1 ). More importantly, a high X-ray imaging resolution of 16 lp/mm based on SC-Ag screen is demonstrated. Besides, rigid core skeleton reinforced by metallophilicity endows clusters M 6 S 6 L 6 strong resistance to humidity and radiation. This work provides a new view for the design of efficient scintillators and opens the research door for silver clusters in scintillation application., (© 2023 Wiley-VCH GmbH.)

Scalable and addressable integrated manipulation of qubits is crucial for practical quantum information applications. Different waveguides have been used to transport the optical and electrical driving pulses, which are usually required for qubit manipulation. However, the separated multifields may limit the compactness and efficiency of manipulation and introduce unwanted perturbation. Here, we develop a tapered fiber-nanowire-electrode hybrid structure to realize integrated optical and microwave manipulation of solid-state spins at nanoscale. Visible light and microwave driving pulses are simultaneously transported and concentrated along an Ag nanowire. Studied with spin defects in diamond, the results show that the different driving fields are aligned with high accuracy. The spatially selective spin manipulation is realized. And the frequency-scanning optically detected magnetic resonance (ODMR) of spin qubits is measured, illustrating the potential for portable quantum sensing. Our work provides a new scheme for developing compact, miniaturized quantum sensors and quantum information processing devices.

Recently, there has been significant interest in the generation of coherent temporal solitons in optical microresonators. In this Letter, we present a demonstration of dissipative Kerr soliton generation in a microrod resonator using an auxiliary-laser-assisted thermal response control method. In addition, we are able to control the repetition rate of the soliton over a range of 200 kHz while maintaining the pump laser frequency, by applying external stress tuning. Through the precise control of the PZT voltage, we achieve a stability level of 3.9 × 10 -10 for residual fluctuation of the repetition rate when averaged 1 s. Our platform offers precise tuning and locking capabilities for the repetition frequency of coherent mode-locked combs in microresonators. This advancement holds great potential for applications in spectroscopy and precision measurements.

We present a novel micro-fabrication technique for creating concave surfaces on the endfacets of photonic crystal fibers. A fiber fusion splicer is used to generate arc discharges to melt and reshape the fiber endfacet. This technique can produce large spherical concave surfaces with roughness as low as 0.12 nm in various types of photonic crystal fibers. The deviation of fabricated surface and a spherical profile in the region of 70 µ m in diameter is less than 50 nm. The center of the concave surface and the fiber mode field are highly coincident with a deviation less than 500 nm. Finesse measurements have shown that a Fabry-Pérot cavity composed of the fiber fabricated using this method and a plane mirror maintains finesse of 20000. This method is easy to replicate, making it a practical and efficient approach to fabricate concave surface on fibers for open-access fiber Fabry-Pérot cavities.

Noncentrosymmetric phosphides have garnered significant attention as promising systems of infrared (IR) nonlinear optical (NLO) materials. Herein, a new quaternary diamond-like phosphide family I-III-IV 2 -V 4 and its inaugural member, namely, CuInSi 2 P 4 (CISP), were successfully fabricated by isovalent and aliovalent substitution based on ZnGeP 2 . First-principles calculations revealed that CISP has a large NLO coefficient ( d 14 = 110.8 pm/V), which can be attributed to the well-aligned tetrahedral [CuP 4 ], [InP 4 ], and [SiP 4 ] units. Remarkably, the extremely small thermal expansion anisotropy (0.09) of CISP enables it to exhibit a considerable laser-induced damage threshold (LIDT, 5.0 × AgGaS 2 @1.06 μm) despite the relatively narrow band gap (0.81 eV). This work improves the chemical diversity of inorganic phosphide and promotes the development of phosphide systems, which may provide valuable perspectives for future exploration of IR NLO materials.

The typical chalcopyrite AgGaQ 2 (Q = S, Se) are commercial infrared (IR) second-order nonlinear optical (NLO) materials; however, they suffer from unexpected laser-induced damage thresholds (LIDTs) primairy due to their narrow band gaps. Herein, what sets this apart from previously reported chemical substitutions is the utilization of an unusual cationic substitution strategy, represented by [[SZn 4 ]S 12 + [S 4 Zn 13 ]S 24 + 11ZnS 4 ⇒ MS 12 + [M 4 Cl]S 24 + 11GaS 4 ], in which the covalent S x Zn y units in the diamond-like sphalerite ZnS are synergistically replaced by cationic M x Cl y units, resulting in two novel salt-inclusion sulfides, M[M 4 Cl][Ga 11 S 20 ] (M = A/Ba, A = K, 1; Rb, 2). As expected, the introduction of mixed cations in the GaS 4 anionic frameworks of 1 and 2 leads to wide band gaps (3.04 and 3.01 eV), which exceeds the value of AgGaS 2 , facilitating the improvement of high LIDTs (9.4 and 10.3 × AgGaS 2 @1.06 µm, respectively). Furthermore, compounds 1 and 2 exhibit moderate second-harmonic generation intensities (0.84 and 0.78 × AgGaS 2 @2.9 µm, respectively), mainly originating from the orderly packing tetrahedral GaS 4 units. Importantly, this study demonstrates the successful application of the cationic substitution strategy based on diamond-like structures to provide a feasible chemical design insight for constructing high-performance NLO materials., (© 2023 Wiley-VCH GmbH.)

Magnetic-free nonreciprocal optical devices have attracted great attention in recent years. Here, we investigated the magnetic-free polarization rotation of light in an atom vapor cell. Two mechanisms of magnetic-free nonreciprocity have been realized in ensembles of hot atoms, including electromagnetically induced transparency and optically-induced magnetization. For a linearly polarized input probe light, a rotation angle up to 86.4° has been realized with external control and pump laser powers of 10 mW and is mainly attributed to the optically-induced magnetization effect. Our demonstration offers a new approach to realize nonreciprocal devices, which can be applied to solid-state atom ensembles and may be useful in photonic integrated circuits.

An optical frequency comb is a spectrum of optical radiation which consists of evenly spaced and phase-coherent narrow spectral lines and is initially invented in a laser for frequency metrology purposes. A direct analog of frequency combs in the magnonic systems has not been demonstrated to date. In our experiment, we generate a new magnonic frequency comb in the resonator with giant mechanical oscillations through the magnomechanical interaction. We observe the magnonic frequency comb contains up to 20 comb lines, which are separated by the mechanical frequency of 10.08 MHz. The thermal effect based on the strong pump power induces the cyclic oscillation of the magnon frequency shift, which leads to a periodic oscillation of the magnonic frequency comb. Moreover, we demonstrate the stabilization and control of the frequency spacing of the magnonic frequency comb via injection locking. Our Letter lays the groundwork for magnonic frequency combs in the fields of sensing and metrology.