Light-cone distribution amplitudes of the baryon octet

We present results of the first ab initio lattice QCD calculation of the normalization constants and first moments of the leading twist distribution amplitudes of the full baryon octet, corresponding to the small transverse distance limit of the associated S-wave light-cone wave functions. The P-wave (higher twist) normalization constants are evaluated as well. The calculation is done using $N_f=2+1$ flavors of dynamical (clover) fermions on lattices of different volumes and pion masses down to 222 MeV. Significant SU(3) flavor symmetry violation effects in the shape of the distribution amplitudes are observed.Comment: Update to the version published in JHE

Topological aspects of multi-k antiferromagnetism in cubic rare-earth compounds

We advertise rare-earth intermetallics with high-symmetry crystal structures and competing interactions as a possible materials platform hosting spin structures with non-trivial topological properties. Focusing on the series of cubic RCu compounds, where R = Ho, Er, Tm, the bulk properties of these systems display exceptionally rich magnetic phase diagrams hosting an abundance of different phase pockets characteristic of antiferromagnetic order in the presence of delicately balanced interactions. The electrical transport properties exhibit large anomalous contributions suggestive of topologically non-trivial winding in the electronic and magnetic structures. Neutron diffraction identifies spontaneous long-range magnetic order in terms of commensurate and incommensurate variations of ππ0 antiferromagnetism with the possibility for various multi-k configurations. Motivated by general trends in these materials, we discuss the possible existence of topologically non-trivial winding in real and reciprocal space in the class of RCu compounds including antiferromagnetic skyrmion lattices. Putatively bringing together different limits of non-trivial topological winding in the same material, the combination of properties in RCu systems promises access to advanced functionalities

Observation of two independent skyrmion phases in a chiral magnetic material

Magnetic materials can host skyrmions, which are topologically non-trivial spin textures. In chiral magnets with cubic lattice symmetry, all previously-observed skyrmion phases require thermal fluctuations to become thermodynamically stable in bulk materials, and therefore exist only at relatively high temperature, close to the helimagnetic transition temperature. Other stabilization mechanisms require a lowering of the cubic crystal symmetry. Here, we report the identification of a second skyrmion phase in Cu$_{2}$OSeO$_{3}$ at low temperature and in the presence of an applied magnetic field. The new skyrmion phase is thermodynamically disconnected from the well-known, nearly-isotropic, high-temperature phase, and exists, in contrast, when the external magnetic field is oriented along the $\langle100\rangle$ crystal axis only. Theoretical modelling provides evidence that the stabilization mechanism is given by well-known cubic anisotropy terms, and accounts for an additional observation of metastable helices tilted away from the applied field. The identification of two distinct skyrmion phases in the same material and the generic character of the underlying mechanism suggest a new avenue for the discovery, design, and manipulation of topological spin textures

Efficient, Near-Infrared Light-Induced Photoclick Reaction Enabled by Upconversion Nanoparticles

Photoclick reactions combine the selectivity of classical click chemistry with the high precision and spatiotemporal control afforded by light, finding diverse utility in surface customization, polymer conjugation, photocross-linking, protein labeling, and bioimaging. Nonetheless, UV light, pivotal in prevailing photoclick reactions, poses issues, especially in biological contexts, due to its limited tissue penetration and cell-toxic nature. Herein, a reliable and versatile strategy of activating the photoclick reactions of 9,10-phenanthrenequinones (PQs) with electron-rich alkenes (ERAs) with near infrared (NIR) light transduced by spectrally and structurally customized upconversion nanoparticles (UCNPs) is introduced. Under NIR irradiation, the UCNPs become UV/blue nanoemitters uniformly distributed in the reaction system. Enabled by the customized UCNPs, 800 or 980 nm light effectively activates the photocycloaddition reactions via radiative energy transfer in both general and triplet–triplet energy transfer (TTET)-mediated PQ-ERA systems. In particular, the novel sandwich structure UCNPs achieve the click reaction with up to 76% production yield in 10 min under NIR light irradiation. Meanwhile, the tricky side effect of photoclick product absorption-induced quenching is successfully circumvented from the fine-tuning of the upconversion spectrum. Moreover, through-tissue irradiation experiments, the authors show that the UCNP-PQ-ERA reaction unlocks the full potential of photoclick reactions for in vivo applications.</p

Absence of bulk charge density wave order in the normal state of UTe2

A spatially modulated superconducting state, known as pair density wave (PDW), is a tantalizing state of matter with unique properties. Recent scanning tunneling microscopy (STM) studies revealed that spin-triplet superconductor UTe$_{2}$ hosts an unprecedented spin-triplet, multi-component PDW whose three wavevectors are indistinguishable from a preceding charge-density wave (CDW) order that survives to temperatures well above the superconducting critical temperature, T$_{c}$. Whether the PDW is the mother or a subordinate order remains unsettled. Here, based on a systematic search for bulk charge order above T$_{c}$ using resonant elastic X-ray scattering (REXS), we show that the structure factor of charge order previously identified by STM is absent in the bulk within the sensitivity of REXS. Our results invite two scenarios: either the density-wave orders condense simultaneously at T$_{c}$ in the bulk, in which case PDW order is likely the mother phase, or the charge modulations are restricted to the surface

Phenylimino Indolinone: A Green-Light-Responsive T-Type Photoswitch Exhibiting Negative Photochromism

Imines are photoaddressable motifs useful in the development of new generations of molecular switches, but their operation with low-energy photons and control over isomer stability remain challenging. Based on a computational design, we developed phenylimino indolinone (PIO), a green-light-addressable T-type photoswitch showing negative photochromism. The isomerization behavior of this photoactuator of the iminothioindoxyl (ITI) class was studied using time-resolved spectroscopies on time scales from femtoseconds to the steady state and by quantum-chemical analyses. The understanding of the isomerization properties and substituent effects governing these photoswitches opens new avenues for the development of novel T-type visible-light-addressable photoactuators based on C=N bonds

Hypothesis-Driven, Structure-Based Design in Photopharmacology:The Case of eDHFR Inhibitors

[Image: see text] Photopharmacology uses light to regulate the biological activity of drugs. This precise control is obtained through the incorporation of molecular photoswitches into bioactive molecules. A major challenge for photopharmacology is the rational design of photoswitchable drugs that show light-induced activation. Computer-aided drug design is an attractive approach toward more effective, targeted design. Herein, we critically evaluated different structure-based approaches for photopharmacology with Escherichia coli dihydrofolate reductase (eDHFR) as a case study. Through the iterative examination of our hypotheses, we progressively tuned the design of azobenzene-based, photoswitchable eDHFR inhibitors in five design–make–switch–test–analyze cycles. Targeting a hydrophobic subpocket of the enzyme and a specific salt bridge only with the thermally metastable cis-isomer emerged as the most promising design strategy. We identified three inhibitors that could be activated upon irradiation and reached potencies in the low-nanomolar range. Above all, this systematic study provided valuable insights for future endeavors toward rational photopharmacology

Long-range magnetic order in CePdAl3_3 enabled by orthorhombic deformation

We investigate the effect of structural deformation on the magnetic properties of orthorhombic CePdAl$_3$ in relation to its tetragonal polymorph. Utilizing x-ray and neutron diffraction we establish that the crystal structure has the $Cmcm$ space group symmetry and exhibits pseudo-tetragonal twinning. According to density-functional calculations the tetragonal-orthorhombic deformation mechanism has its grounds in relatively small free enthalpy difference between the polymorphs, allowing either phase to be quenched and fully accounts for the twinned microstructure of the orthorhombic phase. Neutron diffraction measurements show that orthorhombic CePdAl$_3$ establishes long-range magnetic order below $T_\mathrm{N}$=5.29 (5) K characterized by a collinear, antiferromagnetic arrangement of magnetic moments. Magnetic anisotropies of orthorhombic CePdAl$_3$ arise from strong spin-orbit coupling as evidenced by the crystal-field splitting of the $4f$ multiplet, fully characterised with neutron spectroscopy. We discuss the potential mechanism of frustration posed by antiferromagnetic interactions between nearest neighbours in the tetragonal phase, which hinders the formation of long-range magnetic order in tetragonal CePdAl$_3$. We propose that orthorhombic deformation releases the frustration and allows for long-range magnetic order.Comment: Finalized paper from the splitting of arxiv.org/abs/2106.08194v

Synthesis and preclinical evaluation of novel 18F-vancomycin-based tracers for the detection of bacterial infections using positron emission tomography

IntroductionBacterial infections are a major problem in medicine, and the rapid and accurate detection of such infections is essential for optimal patient outcome. Bacterial infections can be diagnosed by nuclear imaging, but most currently available modalities are unable to discriminate infection from sterile inflammation. Bacteria-targeted positron emission tomography (PET) tracers have the potential to overcome this hurdle. In the present study, we compared three 18F-labelled PET tracers based on the clinically applied antibiotic vancomycin for targeted imaging of Gram-positive bacteria.Methods[18F]FB-NHS and [18F]BODIPY-FL-NHS were conjugated to vancomycin. The resulting conjugates, together with our previously developed [18F]PQ-VE1-vancomycin, were tested for stability, lipophilicity, selective binding to Gram-positive bacteria, antimicrobial activity and biodistribution. For the first time, the pharmacokinetic properties of all three tracers were compared in healthy animals to identify potential binding sites.Results[18F]FB-vancomycin, [18F]BODIPY-FL-vancomycin, and [18F]PQ-VE1-vancomycin were successfully synthesized with radiochemical yields of 11.7%, 2.6%, and 0.8%, respectively. [18F]FB-vancomycin exhibited poor in vitro and in vivo stability and, accordingly, no bacterial binding. In contrast, [18F]BODIPY-FL-vancomycin and [18F]PQ-VE1-vancomycin showed strong and specific binding to Gram-positive bacteria, including methicillin-resistant Staphylococcus aureus (MRSA), which was outcompeted by unlabeled vancomycin only at concentrations exceeding clinically relevant vancomycin blood levels. Biodistribution showed renal clearance of [18F]PQ-VE1-vancomycin and [18F]BODIPY-FL-vancomycin with low non-specific accumulation in muscles, fat and bones.ConclusionHere we present the synthesis and first evaluation of the vancomycin-based PET tracers [18F]BODIPY-FL-vancomycin and [18F]PQ-VE1-vancomycin for image-guided detection of Gram-positive bacteria. Our study paves the way towards real-time bacteria-targeted diagnosis of soft tissue and implant-associated infections that are oftentimes caused by Gram-positive bacteria, even after prophylactic treatment with vancomycin