Metal-Coordinated NIR-II Nanoadjuvants with Nanobody Conjugation for Potentiating Immunotherapy by Tumor Metabolism Reprogramming.

Immune checkpoint blockade (ICB) immunotherapy remains hampered by insufficient immunogenicity and a high-lactate immunosuppressive tumor microenvironment (TME). Herein, a nanobody-engineered NIR-II nanoadjuvant with targeting metabolic reprogramming capability is constructed for potentiating NIR-II photothermal-ferroptosis immunotherapy. Specifically, the nanoadjuvant (2DG@FS-Nb) is prepared by metallic iron ion-mediated coordination self-assembly of D-A-D type NIR-II molecules and loading of glycolysis inhibitor, 2-deoxy-D-glucose (2DG), followed by modification with aPD-L1 nanobody (Nb), which can effectively target the immunosuppressive TME and trigger in situ immune checkpoint blockade. The nanoadjuvants responsively release therapeutic components in the acidic TME, enabling the precise tumor location by NIR-II fluorescence/photoacoustic imaging while initiating NIR-II photothermal-ferroptosis therapy. The remarkable NIR-II photothermal efficiency and elevated glutathione (GSH) depletion further sensitize ferroptosis to induce severe lipid peroxidation, provoking robust immunogenic cell death (ICD) to trigger anti-tumor immune response. Importantly, the released 2DG markedly inhibits lactate generation through glycolysis obstruction. Decreased lactate efflux remodels the immunosuppressive TME by suppressing M2 macrophage proliferation and downregulating regulatory T cell levels. This work provides a new paradigm for the integration of NIR-II phototheranostics and lactate metabolism regulation into a single nanoplatform for amplified anti-tumor immunotherapy combined with ICB therapy.

An NIR-II-emitting type-I photosensitizer for efficient hypoxic tumor phototheranostics.

A small molecule-based NIR-II type-I photosensitizer (IT-IC) with a strong push-pull effect and good planar π-conjugated structure was synthesized. The IT-IC NPs exhibited strong light absorption, outstanding NIR-II fluorescence emission, excellent photothermal conversion and efficient type-I/II ROS generation, showing encouraging therapeutic outcomes for hypoxic tumors.

A diketopyrrolopyrrole-based small molecule with an extended conjugated skeleton and J-aggregation behavior for 808 nm laser triggered phototheranostics.

The development of phototheranostic agents, specifically those based on organic small molecules (OSMs) with long wavelength excitation/emission, is an attractive but challenging project. In this contribution, we designed and synthesized a novel conjugate small molecule with a linear structure, named DPP-OPIC. Water-soluble nanoparticle DPP-OPIC NPs were fabricated. They exhibited strong absorption in the region of 600-1000 nm, which was due to the extended conjugate length of the molecular skeleton and J-aggregation behavior. Under 808 nm laser excitation, DPP-OPIC NPs were capable of producing outstanding near-infrared-II (NIR-II, 900-1700 nm) fluorescence. The photoluminescence quantum yield was determined as 0.58%, which enabled high-resolution in vivo tumor imaging. Additionally, a notable photothermal effect with a high photothermal conversion efficiency (41.5%) was achieved by the irradiation of DPP-OPIC NPs. Hence, DPP-OPIC NPs can be used as superior phototheranostic agents, providing valuable contributions to NIR-II fluorescence imaging and photothermal therapy.

Anomalous transport due to Weyl fermions in the chiral antiferromagnets Mn3X, X = Sn, Ge.

The recent discoveries of strikingly large zero-field Hall and Nernst effects in antiferromagnets Mn3X (X = Sn, Ge) have brought the study of magnetic topological states to the forefront of condensed matter research and technological innovation. These effects are considered fingerprints of Weyl nodes residing near the Fermi energy, promoting Mn3X (X = Sn, Ge) as a fascinating platform to explore the elusive magnetic Weyl fermions. In this review, we provide recent updates on the insights drawn from experimental and theoretical studies of Mn3X (X = Sn, Ge) by combining previous reports with our new, comprehensive set of transport measurements of high-quality Mn3Sn and Mn3Ge single crystals. In particular, we report magnetotransport signatures specific to chiral anomalies in Mn3Ge and planar Hall effect in Mn3Sn, which have not yet been found in earlier studies. The results summarized here indicate the essential role of magnetic Weyl fermions in producing the large transverse responses in the absence of magnetization.

Lifshitz transition underlying the metamagnetic transition of UPt3.

Comparing quantum oscillation measurements, dc magnetoresistance measurements, and Fermi surfaces obtained from LDA calculations, we argue that the metamagnetic transition of UPt3, which occurs at an applied field µ ◦ H M ∼ 20 T, coincides with a Lifshitz transition at which an open orbit on the band 2 hole-like Fermi surface becomes closed for one spin direction. At low field, proximity of the Fermi energy to this particular van Hove singularity may have implications for the superconducting pairing potential of UPt3. In our picture the magnetization comes from non-linear spin-splitting of the heavy fermion bands. In support of this, we show that the non-linear field dependence of a particular quantum oscillation frequency can be fitted by assuming that the corresponding extremal Fermi surface area is proportional to the magnetization. In addition, below H M , we find in our LDA calculations a new, non-central orbit on band 1, whose non-linear behaviour explains a field-dependent frequency recently observed in magnetoacoustic quantum oscillation measurements.

Co/FeC core-nitrogen doped hollow carbon shell structure with tunable shell-thickness for oxygen evolution reaction.

Herein, multi-core-shell structure Co/FeC@N-doped hollow carbon (Co/FeC@NHC) with tunable carbon shell thickness is well crafted by a novel and simple strategy. Novel core-shell structure consisting of polydopamine (PDA) shell with different thickness and bimetal-based metal-organic frameworks (MOFs) Co/Fe core with cubic morphology are first prepared, followed by a thermal and etching treatments to fabricate hollow composite materials composed of multiple Co/FeC cores evenly distributed in N-doped carbon shell. PDA acts as a carbon and nitrogen source simultaneously to form N-doped hollow carbon in this procedure. Creatively, the N-doped hollow carbon shell protects Co/FeC core and against the degradation, in addition to enhance the conductivity of Co/FeC@NHC. Through adjusting the PDA shell thickness simply, Co/FeC@NHC with tunable N-doped carbon shell thickness is well crafted. The Co/FeC@NHC-1 with the best electrocatalytic performance is obtained by optimizing the thickness of N-doped hollow carbon shell. The Co/FeC@NHC-1 exhibits the highest activity for the oxygen evolution reaction (OER) and outstanding stability and durability. Hence, this research may establish a promising path for the rational design of metals@carbon composite with controllable structure which can act as highly efficient electrocatalysts for (OER).

Electrochemical chiral amino acid biosensor based on dopamine-localized gold nanoparticles @ left-handed spiral chiral carbon nanotubes.

The high electrocatalytic performance plays a decisive role in the efficient electrochemical sensing of electrocatalysts. A spiral chiral carbon tube (HLCNT) loaded with gold nanoparticles (AuNPs) was prepared by electrochemical methods. Dopamine was first electropolymerized on the surface of the HLCNT, and then it acted as a localizer to uniformly load the AuNPs onto the surface of the HLCNT. The dopamine-localized gold nanoparticles @ left-handed spiral chiral carbon nanotubes (HLCNT-AuNPs-2) material combined the chiral structure of chiral carbon nanotubes and the high conductivity of AuNPs. The HLCNT-AuNPs-2 realized the qualitative and quantitative detection of tyrosine (Tyr) and tryptophan (Trp) isomers by their different oxidation potentials and current signals. Through quantitative detection, the analytical results showed that the detection limit of l-Trp was calculated to be 5.31 µM, and the detection limit of l-Tyr was 9.04 µM. More importantly, the material realized the real sample detection of amino acids, which is of great significance for the practical detection of amino acid isomers in medicine and biology.

Carbon quantum dots encapsulated in super small platinum nanocrystals core-shell architecture/nitrogen doped graphene hybrid nanocomposite for electrochemical biosensing of DNA damage biomarker-8-hydroxy-2'-deoxyguanosine.

In this work, carbon quantum dots (CQD) encapsulated in super small platinum nanocrystals core-shell architecture/nitrogen doped graphene hybrid nanocomposite (CQD@PDA@PtNCs-NGR) was design synthesized. Without using any capping reagent, stabilizer and surfactant, very small CQD was served as template and anchoring point for the synthesis of Pt NCs with a super small size (2.25 nm) and a uniform distribution. Meanwhile, dopamine (DA) was used as bridging agent, positioning agent and weak reducing agent to make Pt2+ grow on the CQD. Combine the high dispersed Pt NCs with high specific surface area and high conductivity of NGR, the CQD@PDA@PtNCs-NGR shows excellent electrocatalytic performance towards the biosensing of DNA damage biomarker- 8-Hydroxy-2'-deoxyguanosine (8-OH-dG). A very low detection limit of 0.45 nM and 0.85 nM (S/N = 3), a wide linear range of 0.013 µM-109.78 µM and a high sensitivity of 7.912 µA µM-1cm-2 and 4.190 µA µM-1cm-2 were obtained. The fabricated CQD@PDA@PtNCs-NGR realized the detection of 8-OH-dG in human urine practical sample. Furthermore, CQD@PDA@PtNCs-NGR was applied for the determination of 8-OH-dG generated from damaged DNA and damaged guanine (G), respectively. This work effectively combines the electrochemical signal of 8-OH-dG with DNA damage, confirms the mechanism of DNA damage, which might pave a new way to establish the associations between degree of DNA damage and 8-OH-dG.

Nitrogen doped chiral carbonaceous nanotube for ultrasensitive DNA direct electrochemistry, DNA hybridization and damage study.

In the interest of developing novel electrocatalyst for high performance DNA biosensing, with distinctive chiral double helix nanostructure, nitrogen doped chiral carbonaceous nanotube (Chiral-CNT) was employed for ultrasensitive label-free DNA biosensing research. Chiral-CNT can quantitative detection of four DNA bases with high sensitivity and selectivity. Without any prehydrolysis and labeling process, direct electrochemistry of single-stranded DNA and double-stranded DNA, qualitative and quantitative detection of DNA hybridization (low detection limit: 0.0268 g L-1) were realized. Moreover, sensitive detection of DNA damage induced by fenton reagent was also realized with low detection limit of 0.0350 mg mL-1 and high sensitivity of 7.42 µA mg-1 mL. The high biosensing performance attributes to the unique chiral structure of Chiral-CNT, leads to efficient interreaction between Chiral-CNT and DNA molecule.

Evidence for a gapped spin-liquid ground state in a kagome Heisenberg antiferromagnet.

The kagome Heisenberg antiferromagnet is a leading candidate in the search for a spin system with a quantum spin-liquid ground state. The nature of its ground state remains a matter of active debate. We conducted oxygen-17 single-crystal nuclear magnetic resonance (NMR) measurements of the spin-1/2 kagome lattice in herbertsmithite [ZnCu3(OH)6Cl2], which is known to exhibit a spinon continuum in the spin excitation spectrum. We demonstrated that the intrinsic local spin susceptibility χ(kagome), deduced from the oxygen-17 NMR frequency shift, asymptotes to zero below temperatures of 0.03J, where J ~ 200 kelvin is the copper-copper superexchange interaction. Combined with the magnetic field dependence of χ(kagome) that we observed at low temperatures, these results imply that the kagome Heisenberg antiferromagnet has a spin-liquid ground state with a finite gap.