Time Crystal in a Single-Mode Nonlinear Cavity.

Time crystal is a class of nonequilibrium phases with broken time-translational symmetry. Here, we demonstrate the time crystal in a single-mode nonlinear cavity. The time crystal originates from the self-oscillation induced by a linear gain and is stabilized by a nonlinear damping. We show in the time crystal phase there are sharp dissipative gap closing and pure imaginary eigenvalues of the Liouvillian spectrum in the thermodynamic limit. Dynamically, we observe a metastable regime with the emergence of quantum oscillation, followed by a dissipative evolution with a timescale much longer than the oscillating period. Moreover, we show there is a dissipative phase transition at the Hopf bifurcation, which can be characterized by the photon number fluctuation in the steady state. These results pave a new promising way for further experiments and deepen our understanding of time crystals.

Fast Generation of GHZ-like States Using Collective-Spin XYZ Model.

The Greenberger-Horne-Zeilinger (GHZ) state is a key resource for quantum information processing and quantum metrology. The atomic GHZ state can be generated by one-axis twisting (OAT) interaction H_{OAT}=χJ_{z}^{2} with χ the interaction strength, but it requires a long evolution time χt=π/2 and is thus seriously influenced by decoherence and losses. Here we propose a three-body collective-spin XYZ model which creates a GHZ-like state in a very short timescale χt∼lnN/N for N particles. We show that this model can be effectively produced by applying Floquet driving to an original OAT Hamiltonian. Compared with the ideal GHZ state, the GHZ-like state generated using our model can maintain similar metrological properties reaching the Heisenberg-limited scaling, and it shows better robustness to decoherence and particle losses. This Letter opens the avenue for generating GHZ-like states with a large particle number, which holds great potential for the study of macroscopic quantum effects and for applications in quantum metrology and quantum information.

Identifying Driving Factors of Atmospheric N2O5 with Machine Learning.

Dinitrogen pentoxide (N2O5) plays an essential role in tropospheric chemistry, serving as a nocturnal reservoir of reactive nitrogen and significantly promoting nitrate formations. However, identifying key environmental drivers of N2O5 formation remains challenging using traditional statistical methods, impeding effective emission control measures to mitigate NOx-induced air pollution. Here, we adopted machine learning assisted by steady-state analysis to elucidate the driving factors of N2O5 before and during the 2022 Winter Olympics (WO) in Beijing. Higher N2O5 concentrations were observed during the WO period compared to the Pre-Winter-Olympics (Pre-WO) period. The machine learning model accurately reproduced ambient N2O5 concentrations and showed that ozone (O3), nitrogen dioxide (NO2), and relative humidity (RH) were the most important driving factors of N2O5. Compared to the Pre-WO period, the variation in trace gases (i.e., NO2 and O3) along with the reduced N2O5 uptake coefficient was the main reason for higher N2O5 levels during the WO period. By predicting N2O5 under various control scenarios of NOx and calculating the nitrate formation potential from N2O5 uptake, we found that the progressive reduction of nitrogen oxides initially increases the nitrate formation potential before further decreasing it. The threshold of NOx was approximately 13 ppbv, below which NOx reduction effectively reduced the level of night-time nitrate formations. These results demonstrate the capacity of machine learning to provide insights into understanding atmospheric nitrogen chemistry and highlight the necessity of more stringent emission control of NOx to mitigate haze pollution.

The Significant Role of New Particle Composition and Morphology on the HNO3-Driven Growth of Particles down to Sub-10 nm.

New particle formation and growth greatly influence air quality and the global climate. Recent CERN Cosmics Leaving OUtdoor Droplets (CLOUD) chamber experiments proposed that in cold urban atmospheres with highly supersaturated HNO3 and NH3, newly formed sub-10 nm nanoparticles can grow rapidly (up to 1000 nm h-1). Here, we present direct observational evidence that in winter Beijing with persistent highly supersaturated HNO3 and NH3, nitrate contributed less than ∼14% of the 8-40 nm nanoparticle composition, and overall growth rates were only ∼0.8-5 nm h-1. To explain the observed growth rates and particulate nitrate fraction, the effective mass accommodation coefficient of HNO3 (αHNO3) on the nanoparticles in urban Beijing needs to be 2-4 orders of magnitude lower than those in the CLOUD chamber. We propose that the inefficient uptake of HNO3 on nanoparticles is mainly due to the much higher particulate organic fraction and lower relative humidity in urban Beijing. To quantitatively reproduce the observed growth, we show that an inhomogeneous "inorganic core-organic shell" nanoparticle morphology might exist for nanoparticles in Beijing. This study emphasized that growth for nanoparticles down to sub-10 nm was largely influenced by their composition, which was previously ignored and should be considered in future studies on nanoparticle growth.

Comparative analysis for the impacts of VOC subgroups and atmospheric oxidation capacity on O3 based on different observation-based methods at a suburban site in the North China Plain.

The persistent O3 pollution in the Beijing-Tianjin-Hebei (BTH) region remains unresolved, largely due to limited comprehension of O3-precursor relationship and photochemistry drivers. In this work, intraday O3 sensitivity evolution from VOC-limited (volatile organic compound) regime in the forenoon to transition regime in the late afternoon was inferred by relative incremental reactivity (RIR) in summer 2019 at Xianghe, a suburban site in BTH region, suggesting that VOC-focused control policy could combine with stringent afternoon NOx control. Then detailed impacts of VOC subgroups on O3 formation were further comprehensively quantified by parametric OH reactivity (KOH), O3 formation potential (OFP), as well as RIR weighted value and O3 formation path tracing (OFPT) approach based on photochemical box model. O3 episode days corresponded to stronger O3 formation, depicted by higher KOH (10.4 s-1), OFP (331.7 µg m-3), RIR weighted value (1.2), and F(O3)-OFPT (15.5 ppbv h-1). High proportions of isoprene and OVOCs (oxygenated VOCs) to the total KOH and the OFPT method were demonstrated whereas results of OFP and RIR-weighted presented extra great impacts of aromatics on O3 formation. The OFPT approach captured the process that has already happened and included final O3 response to the original VOC, thus reliable for replicating VOC impacts. The comparison results of the four methods showed similarities when utilizing KOH and OFPT methods, which reveals that the potential applicability of simple KOH for contingency VOC control and more complex OFPT method for detailed VOC- and source-oriented control during policy-making. To investigate propulsion of VOC-involved O3 photochemistry, atmospheric oxidation capacity (AOC) was quantified by two atmospheric oxidation indexes (AOI). Both AOIp_G (7.0 × 107 molec cm-3 s-1, potential AOC calculated by oxidation reaction rates) and AOIe_G (8.5 µmol m-3, estimated AOC given redox electron transfer for oxidation products) were stronger on O3 episode days, indicating that AOC promoted the radical cycling initiated from VOC oxidation and subsequent O3 production. Result-oriented AOIe_G reasonably characterized actual AOC inferred by good linear correlation between AOIe_G and O3 concentrations compared to process-oriented AOIp_G. Therefore, with continuous NOx abatement, AOIe_G should be considered to represent actual AOC, also O3-inducing ability.

Health risks and sources of trace elements and black carbon in PM2.5 from 2019 to 2021 in Beijing.

A comprehensive health risk assessment of PM2.5 is meaningful to understand the current status and directions regarding further improving air quality from the perspective of human health. In this study, we evaluated the health risks of PM2.5 as well as highly toxic inorganic components, including heavy metals (HMs) and black carbon (BC) based on long-term observations in Beijing from 2019 to 2021. Our results showed that the relative risks of chronic obstructive pulmonary disease, lung cancer, acute lower respiratory tract infection, ischemic heart disease, and stroke decreased by 4.07%-9.30% in 2020 and 2.12%-6.70% in 2021 compared with 2019. However, they were still at high levels ranging from 1.26 to 1.77, in particular, stroke showed the highest value in 2021. Mn had the highest hazard quotient (HQ, from 2.18 to 2.56) for adults from 2019 to 2021, while Ni, Cr, Pb, As, and BC showed high carcinogenic risks (CR > 1.0×10-6) for adults. The HQ values of Mn and As and the CR values of Pb and As showed constant or slight upwards trends during our observations, which is in contrast to the downward trends of other HMs and PM2.5. Mn, Cr, and BC are crucial toxicants in PM2.5. A significant shrink of southern region sourcesof HMs and BCshrank suggests the increased importance of local sources. Industry, dust, and biomass burning are the major contributors to the non-carcinogenic risks, while traffic emissions and industry are the dominant contributors to the carcinogenic risks in Beijing.

α-Helix-Mediated Protein Adhesion.

Proteins have been adopted by natural living organisms to create robust bioadhesive materials, such as biofilms and amyloid plaques formed in microbes and barnacles. In these cases, ß-sheet stacking is recognized as a key feature that is closely related to the interfacial adhesion of proteins. Herein, we challenge this well-known recognition by proposing an α-helix-mediated interfacial adhesion model for proteins. By using bovine serum albumin (BSA) as a model protein, it was discovered that the reduction of disulfide bonds in BSA results in random coils from unfolded BSA dragging α-helices to gather at the solid/liquid interface (SLI). The hydrophobic residues in the α-helix then expose and break through the hydration layer of the SLI, followed by the random deposition of hydrophilic and hydrophobic residues to achieve interfacial adhesion. As a result, the first assembled layer is enriched in the α-helix secondary structure, which is then strengthened by intermolecular disulfide bonds and further initiates stepwise layering protein assembly. In this process, ß-sheet stacking is transformed from the α-helix in a gradually evolving manner. This finding thus indicates a valuable clue that ß-sheet-featuring amyloid may form after the interfacial adhesion of proteins. Furthermore, the finding of the α-helix-mediated interfacial adhesion model of proteins affords a unique strategy to prepare protein nanofilms with a well-defined layer number, presenting robust and modulable adhesion on various substrates and exhibiting good resistance to acid, alkali, organic solvent, ultrasonic, and adhesive tape peeling.

Observation of Exceptional Points in Thermal Atomic Ensembles.

Exceptional points (EPs) in non-Hermitian systems have recently attracted wide interest and spawned intriguing prospects for enhanced sensing. However, EPs have not yet been realized in thermal atomic ensembles, which is one of the most important platforms for quantum sensing. Here we experimentally observe EPs in multilevel thermal atomic ensembles and realize enhanced sensing of the magnetic field for 1 order of magnitude. We take advantage of the rich energy levels of atoms and construct effective decays for selected energy levels by employing laser coupling with the excited state, yielding unbalanced decay rates for different energy levels, which finally results in the existence of EPs. Furthermore, we propose the optical polarization rotation measurement scheme to detect the splitting of the resonance peaks, which makes use of both the absorption and dispersion properties and shows an advantage with enhanced splitting compared with the conventional transmission measurement scheme. Additionally, in our system both the effective coupling strength and decay rates are flexibly adjustable, and thus the position of the EPs are tunable, which expands the measurement range. Our Letter not only provides a new controllable platform for studying EPs and non-Hermitian physics, but also provide new ideas for the design of EP-enhanced sensors and opens up realistic opportunities for practical applications in the high-precision sensing of magnetic field and other physical quantities.

PT-Symmetric Feedback Induced Linewidth Narrowing.

Narrow linewidth is a long-pursued goal in precision measurement and sensing. We propose a parity-time symmetric (PT-symmetric) feedback method to narrow the linewidths of resonance systems. By using a quadrature measurement-feedback loop, we transform a dissipative resonance system into a PT-symmetric system. Unlike the conventional PT-symmetric systems that typically require two or more modes, here the PT-symmetric feedback system contains only a single resonance mode, which greatly extends the scope of applications. The method enables remarkable linewidth narrowing and enhancement of measurement sensitivity. We illustrate the concept in a thermal ensemble of atoms, achieving a 48-fold narrowing of the magnetic resonance linewidth. By applying the method in magnetometry, we realize a 22-times improvement of the measurement sensitivity. This work opens the avenue for studying non-Hermitian physics and high-precision measurements in resonance systems with feedback.

Constraints on Spin-Spin Velocity-Dependent Interactions.

The existence of exotic spin-dependent forces may shine light on new physics beyond the standard model. We utilize two iron shielded SmCo_{5} electron-spin sources and two optically pumped magnetometers to search for exotic long-range spin-spin velocity-dependent force. The orientations of spin sources and magnetometers are optimized such that the exotic force is enhanced and common-mode noise is effectively subtracted. We set direct limit on proton-electron interaction in the force range from 1 cm to 1 km. Our experiment represents more than 10 orders of magnitude improvement than previous works.

PtSnBi Nanoplates Enable Photoacoustic Imaging-Guided Highly Efficient Photothermal Tumor Ablation.

The development of photothermal agents (PTAs) with robust photostability and high photothermal conversion efficiency is of great importance for cancer photothermal therapy. Herein, a novel PTA was created using two-dimensional intermetallic PtSnBi nanoplates (NPs), which demonstrated excellent photostability and biocompatibility with a high photothermal conversion efficiency of ∼61 % after PEGylation. More importantly, PtSnBi NPs could be employed as photoacoustic imaging contrast agents for tumor visualization due to their strong absorbance in the NIR range. In addition, both in vitro and in vivo experiments confirmed that PtSnBi NPs had a good photothermal efficacy under NIR laser irradiation. Therefore, the remarkable therapeutic characteristics of PtSnBi NPs make them a most promising candidate for cancer theranostics.

Catalytic Oxidation Mechanism of Toluene over CexMn1-xO2: The Role of Oxygen Vacancies in Adsorption and Activation of Toluene.

Catalytic oxidation has been extensively studied as a promising technology for the removal of toluene from industrial waste gases and indoor air. However, the debate regarding the oxidation mechanism is far from resolved. CexMn1-xO2 catalysts with different mixing ratios are prepared by the sol-gel method and found to exhibit better catalytic activities for toluene oxidation than a single oxide. Characterizations and theoretical calculations reveal that the doped Mn increases the number of oxygen vacancies and the ability of oxygen vacancies to activate aromatic rings, which promotes the rate-determining step of toluene oxidation, i.e., ring-opening reactions. The oxidation products detected by in situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) and Vocus proton transfer reaction mass spectrometry (Vocus-PTR-MS) show that the doped Mn significantly improves the ring-opening efficiency and subsequently yields more short-chain products, such as pyruvic acid and acetic acid. A comprehensive oxidation pathway of toluene is refined in this work.

Synthesis of cyclopropanes through gold-catalyzed [2 + 1] cycloaddition of allenamides with sulfoxonium ylides.

Cyclopropyl groups are widely found in pharmaceutical products and their application as precursors or key reaction intermediates benefits the development of a wide range of reactions. Herein, we report a facile protocol for the synthesis of this compound through gold-catalyzed [2 + 1] cycloaddition of allenamides with sulfoxonium ylides. The reaction exhibited good functional group tolerance and high efficiency, affording the products in good to excellent yields with good diastereoisomerism. The steric hindrance between the sulfonamide group and the gold catalyst determined the major configuration of the formed cis-cyclopropane product. Moreover, the aldehyde could be converted to amide under Schmidt reaction conditions and alcohol under reduction conditions.

Reactive Chlorine Species Advancing the Atmospheric Oxidation Capacities of Inland Urban Environments.

Chlorine (Cl) radicals from photolabile chlorine species are highly reactive and can affect the fate of air pollutants in the atmosphere. Although several campaigns have been conducted, typically in coastal environments, long-term observations of reactive chlorine species and their impacts on atmospheric oxidation capacities (AOCs) are lacking. Here, we report nearly full-year observations of Cl2 and ClNO2 levels in Beijing and evaluate their impacts on the AOC with a box model coupled with Cl chemistry. Cl radicals promote the circulation of OH-HO2-RO2 by accelerating the OH chain lengths by up to 12.6% on average, hence boosting the AOC, especially in the winter or spring. This promotion effect is nonlinearly dependent on the VOC and NOx concentrations, thus leading to a slight shift in ozone formation from a VOC-sensitive regime to a transition regime with seasonal differences. Given the ubiquitous reactive chlorines in polluted inland urban regions, the AOCs and the formation of secondary pollutants will be underestimated if the reactive chlorine species are neglected.

The role of NOx in Co-occurrence of O3 and PM2.5 pollution driven by wintertime east Asian monsoon in Hainan.

Clarifying the driving forces of O3 and fine particulate matter (PM2.5) co-pollution is important to perform their synergistic control. This work investigated the co-pollution of O3 and PM2.5 in Hainan Province using an observation-based model and explainable machine learning. The O3 and PM2.5 pollution that occurs in winter is affected by the wintertime East Asian Monsoon. The O3 formation shifts from a NOx-limited regime with a low O3 production rate (PO3) in the non-pollution season to a transition regime with a high PO3 in the pollution season due to an increase in NOx concentrations. Increased O3 and atmospheric oxidation capacity promote the conversion from gas-phase precursors to aerosols. Meanwhile, the high concentration of particulate nitrate favors HONO formation via photolysis, in turn facilitating O3 production. Machine learning reveals that NOx promotes O3 and PM2.5 co-pollution during the pollution period. The PO3 shows an upward trend at the observation site from 2018 to 2022 due to the inappropriate reduction of volatile organic compounds (VOCs) and NOx in the upwind areas. Our results suggest that a deep reduction of NOx should benefit both O3 and PM2.5 pollution control in Hainan and bring new insights into improving air quality in other regions of China in the future.

Heterogeneous kinetics of the OH-initiated degradation of fenthion and parathion.

Fenthion and parathion are two representative kinds of organophosphorus pesticides and widely used in agriculture. They are directly or indirectly released into the atmosphere by spraying or volatilization processes. However, their heterogeneous reactivity toward OH radicals has not yet been well understood. Therefore, this work investigated the heterogeneous kinetics of the OH-initiated degradation of surface-bound fenthion and parathion using a flow reactor. The results showed that OH radicals played an important role in the atmospheric degradation of fenthion and parathion. Their average rate constants were (7.20 ± 0.77) × 10-12 and (10.40 ± 0.60) × 10-12 cm3/(mol· sec) at a relative humidity (RH) and temperature of 35% and 20 °C, respectively, suggesting that they have relatively short lifetimes in the atmosphere. In addition, a negative RH dependence and a positive temperature dependence of the rate constants were observed. The Arrhenius expressions of fenthion and parathion were k2 = (1.34 ± 0.48) × 10-9exp[-(1432.59 ± 105.29)/T] and k2 = (1.96 ± 1.38) × 10-9exp[-(1619.98 ± 222.02)/T], respectively, and their overall activation energy was estimated to be (11.88 ± 0.87) and (13.48 ± 1.83) kJ/mol. The experimental results will update the kinetic data of fenthion and parathion in the atmosphere and be helpful to further understand their atmospheric transportation processes.

Electrocatalytic oxidation of gaseous toluene in an all-solid cell using a foam Ti/Sb-SnO2/ß-PbO2 anode.

Mineralization of benzene, toluene, and xylene (BTX) with high efficiency at room temperature is still a challenge for the purification of indoor air. In this work, a foam Ti/Sb-SnO2/ß-PbO2 anode catalyst was prepared for electrocatalytically oxidizing gaseous toluene in an all-solid cell at ambient temperature. The complex Ti/Sb-SnO2/ß-PbO2 anode, which was prepared by sequentially deposing Sb-SnO2 and ß-PbO2 on a foam Ti substrate, shows high electrocatalytic oxidation efficiency of toluene (80%) at 7 hr of reaction and high CO2 selectivity (94.9%) under an optimized condition, i.e., a cell voltage of 2.0 V, relative humidity of 60% and a flow rate of 100 mL/min. The better catalytic performance can be ascribed to the high production rate of ⋅OH radicals from discharging adsorbed water and the inhibition of oxygen evolution on the surface of foam Ti/Sb-SnO2/ß-PbO2 anode when compared with the foam Ti/Sb-SnO2 anode. Our results demonstrate that prepared complex electrodes can be potentially used for electrocatalytic removal of gaseous toluene at room temperature with a good performance.

Controlling the Structure and Function of Protein Thin Films through Amyloid-like Aggregation.

Protein thin films (PTFs) with tunable structure and function can offer multiple opportunities in various fields such as surface modification, biomaterials, packaging, optics, electronics, separation, energy, and environmental science. Although nature may offer a variety of examples of high-level control of structure and function, e.g., the S layer of cells, synthetic alternatives for large-area protein-based thin films with fine control over both biological function and material structure are a key challenge, especially when aiming for facile, low-cost, green, and large-scale preparation as well as a further extension of function, such as the encapsulation and release of functional building blocks.Therefore, regarding the structure and function of PTFs, we will first briefly comment on the problems associated with PTF fabrication, and then, regarding the basis of our long-term research on protein-based thin films, we will summarize the new strategies that we have developed in recent years to explore and control the structure and function of PTFs for frontier research and practical applications.Inspired by naturally occurring protein amyloid fibrillization, we proposed the amyloid-like protein aggregation strategy to assemble proteins into supramolecular 2D films with extremely large sizes and enduring interfacial adhesion stability. This approach opened a new window for PTF fabrication in which the spontaneous interfacial 2D aggregation of protein oligomers instead of traditional 1D protofibril elongation directs the assembly of proteins. As a result, the film morphology, thickness, porosity, and function can be tailored by simply tuning the interfacial aggregation pathways.We further modified amyloid-like protein aggregation to develop chemoselective reaction-induced protein aggregation (CRIPA). It is well known that chemoselective reactions have been employed for protein modification. However, the application of such reactions in PTF fabrication has been overlooked. We initiated this new strategy by employing thiol-disulfide exchange reactions. These reactions are chemoselective toward proteins containing specific disulfide bonds with high redox potentials, resulting in amyloid-like aggregation and thin film formation. Functional proteins with immunity to such reactions can be encapsulated in thin films and released on demand without a loss of activity, opening a new avenue for the development of functional PTFs and coatings.Finally, the resultant amyloid-inspired PTFs, as a new type of biomimetic materials, provide a good platform for integration with various biomedical functions. Here, the creation of bioactive surfaces on virtually arbitrary substrates by amyloid-like PTFs will be discussed, highlighting antimicrobial, antifouling, molecular separation, and interfacial biomineralization activities that exceed those of their native protein precursors and synthetic alternatives.

Cooling of mechanical resonator in a hybrid intracavity squeezing optomechanical system.

A hybrid intracavity squeezing optomechanical cooling system, in which an auxiliary cavity couples to an optomechanical cavity with a nonlinear medium inside it, is proposed to realize the ground state cooling of the mechanical resonator in the highly unresolved sideband regime. We demonstrate that the quantum backaction heating can be suppressed perfectly by the intracavity squeezing, and the cooling process can be further promoted by adjusting the tunnel coupling between the coupled cavities. The scheme has good performance in resisting the environmental thermal noise and better tolerance for the auxiliary cavity quality factor and provides the possibility for the quantum manipulation of the mechanical resonator with large mass and low frequency.

Gain-Loss-Induced Hybrid Skin-Topological Effect.

Non-Hermitian topological effects are of crucial importance both in fundamental physics and applications. Here we discover the gain-loss-induced hybrid second-order skin-topological effect and the PT phase transition in skin-topological modes. By studying a non-Hermitian Haldane model, we find that the topological edge modes are localized on a special type of corner, while the bulk modes remain extended. Such an effect originates from the interplay between gain, loss, and the chiral edge currents induced by the nonlocal flux, which can be characterized by considering the properties of the edge sites as a one-dimensional chain. We establish a relation between the skin-topological effect and the PT symmetries belonging to different edges. Moreover, we discover the PT phase transition with the emergence of exceptional points between pairs of skin-topological modes. Our results pave the way for the investigation of non-Hermitian topological physics and PT phase transition in higher-dimensional systems.