Observation of Non-Hermitian Edge Burst Effect in One-Dimensional Photonic Quantum Walk.

Non-Hermitian systems can exhibit unique quantum phases without any Hermitian counterparts. For example, the latest theoretical studies predict a new surprising phenomenon that bulk bands can localize and dissipate prominently at the system boundary, which is dubbed the non-Hermitian edge burst effect. Here we realize a one-dimensional non-Hermitian Su-Schrieffer-Heeger lattice with bulk translation symmetry implemented with a photonic quantum walk. Employing time-resolved single-photon detection to characterize the chiral motion and boundary localization of bulk bands, we determine experimentally that the dynamics underlying the non-Hermitian edge burst effect is due to the interplay of non-Hermitian skin effect and imaginary band gap closing. This new non-Hermitian physical effect deepens our understanding of quantum dynamics in open quantum systems.

A brief review of hybrid skin-topological effect.

The finding of non-Hermitian skin effect (NHSE) has revolutionized our understanding of non-Hermitian topological phases, where the usual bulk-boundary correspondence is broken and new topological phases specific to non-Hermitian system are uncovered. Hybrid skin-topological effect (HSTE) is a class of newly discovered non-Hermitian topological states that simultaneously supports skin-localized topological edge states and extended bulk states. Here we provide a brief review of HSTE, starting from different mechanisms that have been used to realize HSTE, including non-reciprocal couplings, onsite gain/loss, and non-Euclidean lattice geometries. We also review some theoretical developments closely related to the HSTE, including the concept of higher-order NHSE, parity-time symmetry engineering, and non-Hermitian chiral skin effect. Finally, we summarize recent experimental exploration of HSTE, including its realization in electric circuits systems, non-Hermitian photonic crystals, and active matter systems. We hope this review can make the concept of hybrid-skin effect clearer and inspire new finding of non-Hermitian topological states in higher dimensional systems.

Occupation-Dependent Particle Separation in One-Dimensional Non-Hermitian Lattices.

We unveil an exotic phenomenon arising from the intricate interplay between non-Hermiticity and many-body physics, namely, an occupation-dependent particle separation for hardcore bosons in a one-dimensional lattice driven by unidirectional non-Hermitian pumping. Taking hardcore bosons as an example, we find that a pair of particles occupying the same unit cell exhibit an opposite non-Hermitian pumping direction to that of unpaired ones occupying different unit cells. By turning on an intracell interaction, many-body eigenstates split in their real energies, forming separable clusters in the complex energy plane with either left-, right-, or bipolar-types of non-Hermitian skin effect (NHSE). The dependency of skin accumulating directions on particle occupation is further justified with local sublattice correlation and entanglement entropy of many-body eigenstates. Dynamically, this occupation-dependent NHSE manifests as uni- or bidirectional pumping for many-body initial states, allowing for spatially separating paired and unpaired particles. Our results unveil the possibility of designing and exploring novel non-Hermitian phases originated from particle nonconservation in subsystems (e.g., orbitals, sublattices, or spin species) and their spatial configurations.

Porous Structure of Polymer Films Optimized by Rationally Tuning Phase Separation for Passive All-Day Radiative Cooling.

Passive all-day radiative cooling (PARC) films with porous structures prepared via nonsolvent-induced phase separation (NIPS) have attracted considerable attention owing to their cost-effectiveness and wide applicability. The PARC performances of the films correlate with their porous structures. However, the porous structure formed using the NIPS process cannot be finely regulated. In this study, we prepared polyvinylidene fluoride-hexafluoropropylene (PVDF-HFP) films with porous structures optimized by rationally tuning the phase separation, which was achieved by adjusting the proportions of two good solvents with varying solubility parameters. The optimized PVDF-HFP film with a hierarchically porous structure exhibited a high solar reflectance of 97.7% and an infrared emissivity of 96.7%. The film with excellent durability achieved an average subambient cooling temperature of approximately 5.4 °C under a solar irradiance of 945 W·m-2 as well as a temperature of 11.2 °C at nighttime, thus demonstrating all-day radiative cooling. The results indicate that the proposed films present a promising platform for large-scale applications in green building cooling and achieving carbon neutrality.

Ligand Promoted Pd-Catalyzed High para-Selective C-H Olefination.

Achieving high para-selective C-H functionalized products of benzoic acid derivatives using a designed template is still a daunting challenge because the carbonyl group also could coordinate with metal to activate the ortho-C-H bond. Herein, we report the ligand promoted high para-selective C-H olefination of benzoic acid derivatives; we screened a series of ligands increasing the ratio of p:others from 62:38 to 96:4. This work may find application in the construction of para-substituted benzoic acid derivatives.

Biomimetic Construction of Degradable DNAzyme-Loaded Nanocapsules for Self-Sufficient Gene Therapy of Pulmonary Metastatic Breast Cancer.

Pulmonary metastasis of breast cancer is the major cause of deaths of breast cancer patients, but the effective treatment of pulmonary metastases is still lacking at present. Herein, a degradable biomimetic DNAzyme biocapsule is developed with the poly(ethylenimine) (PEI)-DNAzyme complex encapsulated in a Mn2+/Zn2+-coordinated inositol hexaphosphate (IP6) capsule modified with the cRGD targeting peptide for high-efficiency gene therapy of both primary and pulmonary metastatic breast tumors. This DNAzyme biocapsule is degradable inside acidic lysosomes, leading to the release of DNAzyme and abundant Mn2+/Zn2+ for catalytic cleavage of EGR-1 mRNA. We find that PEI promotes the lysosomal escape of the released DNAzyme. Both in vitro and in vivo experiments demonstrate the apparent downregulation of EGR-1 and Bcl-2 protein expression after treatment with the DNAzyme biocapsule, thereby inducing apoptotic death of tumor cells. We further verify that the DNAzyme biocapsule exhibits potent therapeutic efficacy against both primary and pulmonary metastatic breast tumors with significant inhibition of peri-pulmonary metastasis. This study provides a promising effective strategy for constructing degradable DNAzyme-based platforms with self-supply of abundant metal ion cofactors for high-efficiency gene therapy of metastatic breast cancer.

An experimental and thermodynamic equilibrium investigation of heavy metals transformation in supercritical water gasification of oily sludge.

Supercritical water gasification (SCWG) is an advanced and highly efficient method for treating oily sludge. However, it is crucial to consider the transformation characteristics of heavy metals (HMs) during the SCWG process to prevent potential secondary pollution. This work studied the transformation and distribution characteristics of Cu, Cr and Zn after SCWG of oily sludge in a batch reactor at temperatures ranging from 550 to 700 °C. Additionally, thermodynamic equilibrium analysis was conducted to assess the distribution of HMs based on the minimization of Gibbs free energy. Experimental results indicated that higher temperatures led to the conversion of HMs into more stable forms, effectively immobilizing them within solid products. Furthermore, the addition of Na2CO3 enhanced this process and contributed to a reduction in HMs pollution in the effluent. Thermodynamic equilibrium results were consistent with our experimental data, indicating that the molar fraction of stable HMs forms followed the order: Cr > Cu > Zn. Besides, it is worth noting that Na2CO3 had a limited impact on the distribution of Cu and Cr. However, it played a significant role in inhibiting the formation of silicate Zn at lower temperatures, promoting the decomposition of ZnO*Al2O3 into unstable Zn. This may explain the higher presence of unstable Zn when Na2CO3 was introduced. In summary, this study offers valuable insights into the transformation characteristics of heavy metals and strategies for pollution control during SCWG of oily sludge.

Experimental study on supercritical water gasification of oily sludge using a continuous two-step method.

Supercritical water gasification (SCWG) technology can convert oily sludge into hydrogen-rich gas. To achieve high gasification efficiency of oily sludge with a high oil concentration under mild conditions, a two-step method involving a desorption process and a catalytic gasification process using Raney-Ni catalyst was investigated. High oil removal efficiency (99.57%) and carbon gasification efficiency (93.87%) were achieved. The lowest wastewater total organic carbon, oil content, and carbon content in the solid residues were 4.88 ppm, 0.08% and 0.88%, respectively, using a gasification temperature of 600 °C, treatment concentration of 1.11 wt%, gasification time of 70.7 s, and the optimal desorption temperature of 390 °C. The main organic carbon component in the solid residues was cellulose, which is environmentally safe. As the treatment concentration increased, the two-step method outperformed the single-step method. The mechanism for the two-step SCWG of oily sludge was revealed. In the first step, supercritical water is used in the desorption unit to achieve a high oil removal efficiency with few liquid products generated. In the second step, the Raney-Ni catalyst promotes efficient gasification of high-concentration oil at a low temperature. This research provides valuable insights into the effective SCWG of oily sludge at a low temperature.

Experimental study on alkali catalytic gasification of oily sludge in supercritical water with a continuous reactor.

Realizing the harmless resource utilization of oily sludge is urgent for petroleum industry and of great significance for environmental management. The treatment of oily sludge was investigated using supercritical water gasification (SCWG) with a continuous fluidized bed reactor. The effect of operating parameters on gasification efficiency and gas yield without catalyst was tested, and then the influences of catalyst type (K2CO3 and Na2CO3) and concentrations (1-8 wt%) were systematically studied. The results indicated that a medium mass flow ratio and low feedstock concentration were beneficial for gas production. Alkali catalyst improved carbon gasification efficiency (CE) prominently, and Na2CO3 showed better performance due to its better stability. A maximum CE of 95.87% was achieved when 5 wt% Na2CO3 was added at 650 °C, 23 MPa with 5 wt% oily sludge concentration. Besides, according to XRD patterns of solid residues, Na2CO3 was more stable than K2CO3 during SCWG. SEM-EDX results also revealed that more K was migrated into solid residues than Na. The analysis of pore structure demonstrated that alkali catalyst promoted the evolution of pore structure, resulting in higher specific surface areas and total pore volumes. Na2CO3 has a more substantial destructive effect on solid matrix, causing the matrix structure to collapse and inhibiting pore structure development. The FTIR spectra of solid products exhibited a lower content of carbohydrates and aromatic structures than the initial oily sludge. NH4-N results demonstrated that SCWG was a potential green treatment process for oily sludge. This work can not only give an insight into the reaction mechanism of alkali catalytic gasification of oily sludge, but also help to guide the optimal design of reactor and the regulation of operating parameters.

Oil diffusion mathematical model in oily sludge particle under supercritical water environment.

Supercritical water (SCW, T > 374.15 °C, P > 22.1 MPa) treatment can achieve volume reduction, harmless disposal, and resource utilization of oily sludge. Herein, we investigated the oil removal efficiency (ORE) and oil diffusion characteristics in oily sludge particles under SCW environment. The experimental results showed that when the treatment duration was extended from 5 min to 60 min, the particle diameter decreased from 4 mm to 2 mm, and the ORE improved considerably; however, the treatment temperature (375 °C ∼ 425 °C) had little influence. Based on these findings, an oil diffusion mechanism in oily sludge particles under SCW environment was proposed. Subsequently, a reasonable mathematical model of diffusion was developed to represent the heat and mass transfer in oily sludge particles characterized by porous, high moisture, and oil content. Finally, by analyzing the oil diffusion process in sludge particles within this model, it was found that the oil concentration in SCW and particle diameter had a considerable influence on ORE, while the effect can be ignored when the diameter < 0.2 mm. This research serves as a guide for effectively using SCW to remove oil from oily sludge.

Non-Hermitian pseudo-gaps.

The notion of a band gap is ubiquitous in the characterization of matter. Particularly interesting are pseudo-gaps, which are enigmatic regions of very low density of states that have been linked to novel phenomena like high temperature superconductivity. In this work, we discover a novel origin for pseudo-gaps when boundaries are introduced in a non-Hermitian lattice. It generically occurs due to the interference between two or more asymmetric pumping channels, and possess no analog in Hermitian systems. Mathematically, it can be visualized as being created by divergences of spectral flow in the complex energy plane, analogous to how sharp edges creates divergent electric fields near an electrical conductor. A non-Hermitian pseudo-gap can host symmetry-protected mid-gap modes like ordinary topological gaps, but the mid-gap modes are extended instead of edge-localized, and exhibit extreme sensitivity to symmetry-breaking perturbations. Surprisingly, pseudo-gaps can also host an integer number of edge modes even though the pseudo-bands possess fractional topological windings, or even no well-defined Chern number at all, in the marginal case of a phase transition point. Challenging conventional notions of topological bulk-boundary correspondences and even the very concept of a band, pseudo-gaps post profound implications that extend to many-body settings, such as fractional Chern insulators.

Designing non-Hermitian real spectra through electrostatics.

Non-hermiticity presents a vast newly opened territory that harbors new physics and applications such as lasing and sensing. However, only non-Hermitian systems with real eigenenergies are stable, and great efforts have been devoted in designing them through enforcing parity-time (PT) symmetry. In this work, we exploit a lesser-known dynamical mechanism for enforcing real-spectra, and develop a comprehensive and versatile approach for designing new classes of parent Hamiltonians with real spectra. Our design approach is based on a new electrostatics analogy for modified non-Hermitian bulk-boundary correspondence, where electrostatic charge corresponds to density of states and electric fields correspond to complex spectral flow. As such, Hamiltonians of any desired spectra and state localization profile can be reverse-engineered, particularly those without any guiding symmetry principles. By recasting the diagonalization of non-Hermitian Hamiltonians as a Poisson boundary value problem, our electrostatics analogy also transcends the gain/loss-induced compounding of floating-point errors in traditional numerical methods, thereby allowing access to far larger system sizes.

Near-infrared II plasmonic porous cubic nanoshells for in vivo noninvasive SERS visualization of sub-millimeter microtumors.

In vivo surface-enhanced Raman scattering (SERS) imaging allows non-invasive visualization of tumors for intraoperative guidance and clinical diagnostics. However, the in vivo utility of SERS is greatly hampered by the strong optical scattering and autofluorescence background of biological tissues and the lack of highly active plasmonic nanostructures. Herein, we report a class of porous nanostructures comprising a cubic AuAg alloy nanoshell and numerous nanopores. Such porous nanostructures exhibit excellent near-infrared II plasmonic properties tunable in a broad spectral range by varying the pore features while maintaining a small dimension. We demonstrate their exceptional near-infrared II SERS performance varying with the porous properties. Additionally, near-infrared II SERS probes created with porous cubic AuAg nanoshells are demonstrated with remarkable capability for in vivo visualization of sub-millimeter microtumors in a living mouse model. Our near-infrared II SERS probes hold great potentials for precise demarcation of tumor margins and identification of microscopic tumors.

Characteristics and mechanisms of nitrogen transformation during chicken manure gasification in supercritical water.

Supercritical water gasification (SCWG) is a clean and efficient method for the energy utilization of biomass waste. Studying the behavior of nitrogen in feedstock during the SCWG process is essential because of its significant potential impact on the environment. In this study, the characteristics and mechanisms of nitrogen transformation during chicken manure gasification in supercritical water were investigated in autoclave reactors. The results revealed that temperature plays an important role in raw material conversion and product distribution, especially for nitrogenous components. In particular, the carbon gasification efficiency was 92.66 % at 700 °C, 10 wt%, and K2CO3 as catalysts, implying that the chicken manure was nearly completely converted. NOx was not identified in the gaseous products. As the temperature increased, nitrogen in the raw material was mainly transferred to the liquid. This process is accompanied by the conversion of organic nitrogen to inorganic nitrogen, which is mainly present as NH3-N in liquids. Finally, the migration pathways of nitrogenous intermediates were investigated. The hydrolysis of proteins and amino acids in the initial phases creates conditions for the Maillard reaction, forming nitrogenous heterocyclic compounds (NHCs). Most NHCs gradually ring-opened and eventually converted to CO2, H2, NH3, and other gases. Only a small number of NHCs undergo a series of polymerization reactions at lower temperatures to form nitrogenous carbon precursors that are challenging to gasify. This study provides a theoretical foundation for the targeted removal of nitrogen components during the SCWG of high-nitrogenous biomass.

Near-Infrared II Plasmonic Phototheranostics with Glutathione Depletion for Multimodal Imaging-Guided Hypoxia-Tolerant Chemodynamic-Photocatalytic-Photothermal Cancer Therapy Triggered by a Single Laser.

Tumor microenvironment (TME)-activatable phototheranostics is highly desirable in cancer management but still remains challenging for clinical applications owing to the lack of multifunctional theranostic agents and the limited tissue penetration depth. Reported here is an "all-in-one" phototheranostic platform based on near-infrared II (NIR-II) dual-plasmonic Au@Cu2-x Se core-shell nanocrystals (dpGCS NCs) for combined photoacoustic (PA)/photothermal (PT) imaging-guided chemodynamic therapy (CDT)/photocatalytic therapy (PCT)/photothermal therapy (PTT) all triggered by a single NIR-II laser. The dpGCS NCs feature excellent NIR-II plasmonic and PT properties, which guarantee their capabilities of NIR-II PA and PT imaging for real-time visual observation of tumor size and location during cancer treatment. Additionally, the TME-activated in situ •OH production via dpGCS NC-catalyzed Fenton-like reaction is further enhanced by the NIR-II irradiation, while photoexcited plasmonic hole-induced formation of extra •OH is also evidenced for PCT. Both in vitro and in vivo experiments confirm remarkable therapeutic efficacy of the present phototheranostic platform under NIR-II laser through the CDT/PCT/PTT trimodal combination therapy, achieving complete inhibition of tumor growth in tumor-bearing mice after administration of dpGCS NCs plus a single NIR-II laser irradiation. This work provides a distinctive paradigm for the development of NIR-II phototheranostic platforms for imaging-guided cancer therapy using a single laser.

Quantized classical response from spectral winding topology.

Topologically quantized response is one of the focal points of contemporary condensed matter physics. While it directly results in quantized response coefficients in quantum systems, there has been no notion of quantized response in classical systems thus far. This is because quantized response has always been connected to topology via linear response theory that assumes a quantum mechanical ground state. Yet, classical systems can carry arbitrarily amounts of energy in each mode, even while possessing the same number of measurable edge states as their topological winding. In this work, we discover the totally new paradigm of quantized classical response, which is based on the spectral winding number in the complex spectral plane, rather than the winding of eigenstates in momentum space. Such quantized response is classical insofar as it applies to phenomenological non-Hermitian setting, arises from fundamental mathematical properties of the Green's function, and shows up in steady-state response, without invoking a conventional linear response theory. Specifically, the ratio of the change in one quantity depicting signal amplification to the variation in one imaginary flux-like parameter is found to display fascinating plateaus, with their quantized values given by the spectral winding numbers as the topological invariants.

Experimental investigation on gasification of cationic ion exchange resin used in nuclear power plants by supercritical water.

Spent ion exchange resins produced by nuclear power plants are radioactive organic waste. Until now, there is no satisfactory industrial treatment. Supercritical water gasification (SCWG) of cationic ion exchange resin (CIER) used in nuclear power plants was carried out in a batch reactor in this study. Results showed that the gasification efficiency increased with the growth of temperature (550-750 °C), addition of alkali homogeneous catalyst (K2CO3), proper ratio loading of catalyst to CIER (1:1), decrease of feed concentration (2-10 wt%) and extension of residence time (10-60 min). Carbon gasification efficiency was up to 97.98% with K2CO3 added and 30 min at 750 °C in the batch reactor. The gaseous products mainly consist of H2, CO, CO2 and CH4. The GC-MS analysis showed that the organic component in liquid products was mainly composed of benzene, monocycle arenes, phenol group and polycyclic aromatic hydrocarbons. Based on the experimental results, the formation and gasification pathways of CIER in SCW were proposed.

Direct dynamical characterization of higher-order topological phases with nested band inversion surfaces.

Higher-order topological phases (HOTPs) are systems with topologically protected in-gap boundary states localized at their (d-n)-dimensional boundaries, with d the system dimension and n the order of the topology. This work proposes a dynamics-based characterization of one large class of Z-type HOTPs without specifically relying on any crystalline symmetry considerations. The key element of our innovative approach is to connect quantum quench dynamics with nested configurations of the so-called band inversion surfaces (BISs) of momentum-space Hamiltonians as a sum of operators from the Clifford algebra (a condition that can be partially relaxed), thereby making it possible to dynamically detect each and every order of topology on an equal footing. Given that experiments on synthetic topological matter can directly measure the winding of certain pseudospin texture to determine topological features of BISs, the topological invariants defined through nested BISs are all within reach of ongoing experiments. Further, the necessity of having nested BISs in defining higher-order topology offers a unique perspective to investigate and engineer higher-order topological phase transitions.

Rationally designed dual-plasmonic gold nanorod@cuprous selenide hybrid heterostructures by regioselective overgrowth for in vivo photothermal tumor ablation in the second near-infrared biowindow.

NIR-II plasmonic materials offer multiple functionalities for in vivo biomedical applications, such as photothermal tumor ablation, surface-enhanced Raman scattering biosensing, photoacoustic imaging, and drug carriers. However, integration of noble metals and plasmonic semiconductors is greatly challenging because of the large lattice-mismatch. This study reports the regioselective overgrowth of Cu2-xSe on gold nanorods (GNRs) for preparation of dual-plasmonic GNR@Cu2-xSe hybrid heterostructures with tunable NIR-II plasmon resonance absorption for in vivo photothermal tumor ablation. Methods: The regioselective deposition of amorphous Se and its subsequent conversion into Cu2-xSe on the GNRs are performed by altering capping agents to produce the GNR@Cu2-xSe heterostructures of various morphologies. Their photothermal performances for NIR-II photothermal tumor ablation are evaluated both in vitro and in vivo. Results: We find that the lateral one- and two-side deposition, conformal core-shell coating and island growth of Cu2-xSe on the GNRs can be achieved using different capping agents. The Cu2-xSe domain size in these hybrids can be effectively adjusted by the SeO2 concentration, thereby tuning the NIR-II plasmon bands. A photothermal conversion efficiency up to 58-85% and superior photostability of these dual-plasmonic hybrids can be achieved under the NIR-II laser. Results also show that the photothermal conversion efficiency is dependent on the proportion of optical absorption converted into heat; however, the temperature rise is tightly related to the concentration of their constituents. The excellent NIR-II photothermal effect is further verified in the following in vitro and in vivo experiments. Conclusions: This study achieves one-side or two-side deposition, conformal core-shell coating, and island deposition of Cu2-xSe on GNRs for GNR@Cu2-xSe heterostructures with NIR-II plasmonic absorption, and further demonstrates their excellent NIR-II photothermal tumor ablation in vivo. This study provides a promising strategy for the rational design of NIR-II dual-plasmonic heterostructures and highlights their therapeutic in vivo potential.