Ribozymes enhance chemical reaction rates using many of the same catalytic strategies as protein enzymes. In the hepatitis delta virus (HDV) ribozyme, site-specific self-cleavage of the viral RNA ...phosphodiester backbone requires both divalent cations and a cytidine nucleotide. General acid-base catalysis, substrate destabilization and global and local conformational changes have all been proposed to contribute to the ribozyme catalytic mechanism. Here we report ten crystal structures of the HDV ribozyme in its pre-cleaved state, showing that cytidine is positioned to activate the 2′-OH nucleophile in the precursor structure. This observation supports its proposed role as a general base in the reaction mechanism. Comparison of crystal structures of the ribozyme in the pre- and post-cleavage states reveals a significant conformational change in the RNA after cleavage and that a catalytically critical divalent metal ion from the active site is ejected. The HDV ribozyme has remarkable chemical similarity to protein ribonucleases and to zymogens for which conformational dynamics are integral to biological activity. This finding implies that RNA structural rearrangements control the reactivity of ribozymes and ribonucleoprotein enzymes.
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DOBA, IJS, IZUM, KILJ, NUK, PILJ, PNG, SAZU, SIK, UILJ, UKNU, UL, UM, UPUK
Two new gapless quantum spin-liquid candidates with S = 1 (Ni(2+)) moments: the 6H-B phase of Ba(3)NiSb(2)O(9) with a Ni(2+)-triangular lattice and the 3C phase with a ...Ni(2/3)Sb(1/3)-three-dimensional edge-shared tetrahedral lattice were obtained under high pressure. Both compounds show no magnetic order down to 0.35 K despite Curie-Weiss temperatures θ(CW) of -75.5 (6H-B) and -182.5 K (3C), respectively. Below ~25 K, the magnetic susceptibility of the 6H-B phase saturates to a constant value χ(0) = 0.013 emu/mol, which is followed below 7 K by a linear-temperature-dependent magnetic specific heat (C(M)) displaying a giant coefficient γ = 168 mJ/mol K(2). Both observations suggest the development of a Fermi-liquid-like ground state. For the 3C phase, the C(M) perpendicular T(2) behavior indicates a unique S = 1, 3D quantum spin-liquid ground state.
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CMK, CTK, FMFMET, IJS, NUK, PNG, UM
A universal high energy anomaly in the single particle spectral function is reported in three different families of high temperature superconductors by using angle-resolved photoemission ...spectroscopy. As we follow the dispersing peak of the spectral function from the Fermi energy to the valence band complex, we find dispersion anomalies marked by two distinctive high energy scales, E1 approximately 0.38 eV and E2 approximately 0.8 eV. E1 marks the energy above which the dispersion splits into two branches. One is a continuation of the near parabolic dispersion, albeit with reduced spectral weight, and reaches the bottom of the band at the Gamma point at approximately 0.5 eV. The other is given by a peak in the momentum space, nearly independent of energy between E1 and E2. Above E2, a bandlike dispersion reemerges. We conjecture that these two energies mark the disintegration of the low-energy quasiparticles into a spinon and holon branch in the high Tc cuprates.
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Polymer hydrogels formed by rapid thiol-ene coupling of macromolecular gel formers can offer access to versatile new matrices. This paper describes the efficient synthesis of cysteamine vinyl sulfone ...(CVS) trifluoroacetate, and its incorporation into poly(methyl vinyl ether-alt-maleic anhydride) (PMMAn) to form a series of CVS-functionalized poly(methyl vinyl ether-alt-maleic acid) polymers (PMM-CVSx) containing 10 to 30 mol% pendant vinyl sulfone groups. Aqueous mixtures of these PMM-CVS and a dithiol crosslinker, α,ω-dithio-polyethyleneglycol (HS-PEG-SH, Mn = 1 kDa), gelled through crosslinking by Michael addition within seconds to minutes, depending on pH, degree of functionalization, and polymer loading. Gelation efficiency, Young's modulus, equilibrium swelling and hydrolytic stability are described, and step-wise hydrogel post-functionalization with a small molecule thiol, cysteamine, was demonstrated. Cytocompatibility of these crosslinked hydrogels towards entrapped 3T3 fibroblasts was confirmed using a live/dead fluorescence assay.
Self-assembled nanolayering structures have been reported in resin-dentin interfaces created by adhesives that contain 10-methacryloyloxydecyl dihydrogen phosphate (10-MDP). These structures have ...been hypothesized to contribute to bond durability. The objective of the present study was to determine the extent of nanolayering in resin-dentin interfaces after application of commercialized 10-MDP-containing self-etch and universal adhesives to human dentin. Seven commercialized adhesives were examined: Adhese Universal (Ivoclar-Vivadent), All-Bond Universal (Bisco, Inc.), Clearfil SE Bond 2, Clearfil S3 Bond Plus, Clearfil Universal Bond (all from Kuraray Noritake Dental Inc.), G-Premio Bond (GC Corp.), and Scotchbond Universal (3M ESPE). Each adhesive was applied in the self-etch mode on midcoronal dentin according to the respective manufacturer’s instructions. Bonded specimens (n = 6) were covered with flowable resin composite, processed for transmission electron microscopy, and examined at 30 random sites without staining. Thin-film glancing angle X-ray diffraction (XRD) was used to detect the characteristic peaks exhibited by nanolayering (n = 4). The control consisted of 15%wt, 10%wt, and 5%wt 10-MDP (DM Healthcare Products, Inc.) dissolved in a mixed solvent (ethanol and water weight ratio 9:8, with photoinitiators). Experimental primers were applied to dentin for 20 s, covered with hydrophobic resin layer, and examined in the same manner. Profuse nanolayering with highly ordered periodicity (~3.7 nm wide) was observed adjacent to partially dissolved apatite crystallites in dentin treated with the 15% 10-MDP primer. Three peaks in the 2θ range of 2.40° (3.68 nm), 4.78° (1.85 nm), and 7.18° (1.23 nm) were identified from thin-film XRD. Reduction in the extent of nanolayering was observed in the 10% and 5% 10-MDP experimental primer-dentin interface along with lower intensity XRD peaks. Nanolayering and characteristic XRD peaks were rarely observed in specimens prepared from the commercialized adhesives. The sparsity of nanolayering in resin-dentin interfaces created by commercialized adhesives challenges its clinical effectiveness as a mechanism for improving bond longevity in dentin bonding.
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CMK, NUK, OILJ, SAZU, UKNU, UL, UM, UPUK
Itinerant Antiferromagnetism in RuO2 Berlijn, Tom; Snijders, Paul C.; Delaire, Oliver A. ...
Physical review letters,
02/2017, Volume:
118, Issue:
7
Journal Article
Peer reviewed
Open access
Bulk rutile RuO2 has long been considered a Pauli paramagnet. Here, in this article, we report that RuO2 exhibits a hitherto undetected lattice distortion below approximately 900 K. The distortion is ...accompanied by antiferromagnetic order up to at least 300 K with a small room temperature magnetic moment of approximately 0.05μB as evidenced by polarized neutron diffraction. Density functional theory plus U(DFT+U) calculations indicate that antiferromagnetism is favored even for small values of the Hubbard U of the order of 1 eV. The antiferromagnetism may be traced to a Fermi surface instability, lifting the band degeneracy imposed by the rutile crystal field. The combination of high Néel temperature and small itinerant moments make RuO2 unique among ruthenate compounds and among oxide materials in general.
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This paper presents a unified framework of fault diagnosis and fault-tolerant cooperative output regulation (FTCOR) for a linear discrete-time multi-vehicle system with sensor faults. The FTCOR ...control law is designed through three steps. A cooperative output regulation (COR) controller is designed based on the internal mode principle when there are no sensor faults. A sufficient condition on the existence of the COR controller is given based on the discrete-time algebraic Riccati equation (DARE). Then, a decentralised fault diagnosis scheme is designed to cope with sensor faults occurring in followers. A residual generator is developed to detect sensor faults of each follower, and a bank of fault-matching estimators are proposed to isolate and estimate sensor faults of each follower. Unlike the current distributed fault diagnosis for multi-vehicle systems, the presented decentralised fault diagnosis scheme in each vehicle reduces the communication and computation load by only using the information of the vehicle. By combing the sensor fault estimation and the COR control law, an FTCOR controller is proposed. Finally, the simulation results demonstrate the effectiveness of the FTCOR controller.
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BFBNIB, GIS, IJS, KISLJ, NUK, PNG, UL, UM, UPUK
Abstract
A recent focus of quantum spin liquid (QSL) studies is how disorder/randomness in a QSL candidate affects its true magnetic ground state. The ultimate question is whether the QSL survives ...disorder or the disorder leads to a “spin-liquid-like” state, such as the proposed random-singlet (RS) state. Since disorder is a standard feature of most QSL candidates, this question represents a major challenge for QSL candidates. YbMgGaO
4
, a triangular lattice antiferromagnet with effective spin-1/2 Yb
3+
ions, is an ideal system to address this question, since it shows no long-range magnetic ordering with Mg/Ga site disorder. Despite the intensive study, it remains unresolved as to whether YbMgGaO
4
is a QSL or in the RS state. Here, through ultralow-temperature thermal conductivity and magnetic torque measurements, plus specific heat and DC magnetization data, we observed a residual
κ
0
/
T
term and series of quantum spin state transitions in the zero temperature limit for YbMgGaO
4
. These observations strongly suggest that a QSL state with itinerant excitations and quantum spin fluctuations survives disorder in YbMgGaO
4
.
Abstract
A sub-array of the Large High Altitude Air Shower Observatory (LHAASO), KM2A is mainly designed to observe a large fraction of the northern sky to hunt for γ-ray sources at energies above 10 ...TeV. Even though the detector construction is still underway, half of the KM2A array has been operating stably since the end of 2019. In this paper, we present the KM2A data analysis pipeline and the first observation of the Crab Nebula, a standard candle in very high energy γ-ray astronomy. We detect γ-ray signals from the Crab Nebula in both energy ranges of 10
100 TeV and
100 TeV with high significance, by analyzing the KM2A data of 136 live days between December 2019 and May 2020. With the observations, we test the detector performance, including angular resolution, pointing accuracy and cosmic-ray background rejection power. The energy spectrum of the Crab Nebula in the energy range 10-250 TeV fits well with a single power-law function d
N
/d
E
= (1.13
0.05
0.08
)
10
(
E
/20 TeV)
cm
s
TeV
. It is consistent with previous measurements by other experiments. This opens a new window of γ-ray astronomy above 0.1 PeV through which new ultrahigh-energy γ-ray phenomena, such as cosmic PeVatrons, might be discovered.
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