Water oxidation is a key chemical transformation for the conversion of solar energy into chemical fuels. Our review focuses on recent work on robust earth-abundant heterogeneous catalysts for the ...oxygen-evolving reaction (OER). We point out that improvements in the performance of OER catalysts will depend critically on the success of work aimed at understanding reaction barriers based on atomic-level mechanisms. We highlight the challenge of obtaining acid-stable OER catalysts, with proposals for elements that could be employed to reach this goal. We suggest that future advances in solar fuels science will be accelerated by the development of new methods for materials synthesis and characterization, along with in-depth investigations of redox mechanisms at catalytic surfaces.
Post-translational modifications (PTMs) dramatically enhance the capabilities of proteins. They introduce new functionalities and dynamically control protein activity by modulating intra- and ...intermolecular interactions. Traditionally, PTMs have been considered as reversible attachments to nucleophilic functional groups on amino acid side chains, whereas the polypeptide backbone is often thought to be inert. This paradigm is shifting as chemically and functionally diverse alterations of the protein backbone are discovered. Importantly, backbone PTMs can control protein structure and function just as side chain modifications do and operate through unique mechanisms to achieve these features. In this Perspective, I outline the various types of protein backbone modifications discovered so far and highlight their contributions to biology as well as the challenges in studying this versatile yet poorly characterized class of PTMs.
Issues surrounding the synthesis of modified histone peptides are examined. Topics discussed include histone phosphorylation, lysine methylation and arginine methylation.
We construct a complete set of quasi-local integrals of motion for the many-body localized phase of interacting fermions in a disordered potential. The integrals of motion can be chosen to have ...binary spectrum {0,1}, thus constituting exact quasiparticle occupation number operators for the Fermi insulator. We map the problem onto a non-Hermitian hopping problem on a lattice in operator space. We show how the integrals of motion can be built, under certain approximations, as a convergent series in the interaction strength. An estimate of its radius of convergence is given, which also provides an estimate for the many-body localization–delocalization transition. Finally, we discuss how the properties of the operator expansion for the integrals of motion imply the presence or absence of a finite temperature transition.
Ultralight mechanical resonators based on low-dimensional materials are well suited as exceptional transducers of minuscule forces or mass changes. However, the low dimensionality also provides a ...challenge to minimize resistive losses and heating. Here, we report on a novel approach that aims to combine different two-dimensional (2D) materials to tackle this challenge. We fabricated a heterostructure mechanical resonator consisting of few layers of niobium diselenide (NbSe2) encapsulated by two graphene sheets. The hybrid membrane shows high quality factors up to 245,000 at low temperatures, comparable to the best few-layer graphene mechanical resonators. In contrast to few-layer graphene resonators, the device shows reduced electrical losses attributed to the lower resistivity of the NbSe2 layer. The peculiar low-temperature dependence of the intrinsic quality factor points to dissipation over two-level systems which in turn relax over the electronic system. Our high sensitivity readout is enabled by coupling the membrane to a superconducting cavity which allows for the integration of the hybrid mechanical resonator as a sensitive and low loss transducer in future quantum circuits.
The construction of a quantum computer remains a fundamental scientific and technological challenge because of the influence of unavoidable noise. Quantum states and operations can be protected from ...errors through the use of protocols for quantum computing with faulty components. We present a quantum error-correcting code in which one qubit is encoded in entangled states distributed over seven trapped-ion qubits. The code can detect one bit flip error, one phase flip error, or a combined error of both, regardless on which of the qubits they occur. We applied sequences of gate operations on the encoded qubit to explore its computational capabilities. This seven-qubit code represents a fully functional instance of a topologically encoded qubit, or color code, and opens a route toward fault-tolerant quantum computing.
Catalysis is essential to modern life and has a huge economic impact. The development of new catalysts critically depends on synthetic methods that enable the preparation of tailored nanomaterials. ...Pulsed laser in liquids synthesis can produce uniform, multicomponent, nonequilibrium nanomaterials with independently and precisely controlled properties, such as size, composition, morphology, defect density, and atomistic structure within the nanoparticle and at its surface. We cover the fundamentals, unique advantages, challenges, and experimental solutions of this powerful technique and review the state-of-the-art of laser-made electrocatalysts for water oxidation, oxygen reduction, hydrogen evolution, nitrogen reduction, carbon dioxide reduction, and organic oxidations, followed by laser-made nanomaterials for light-driven catalytic processes and heterogeneous catalysis of thermochemical processes. We also highlight laser-synthesized nanomaterials for which proposed catalytic applications exist. This review provides a practical guide to how the catalysis community can capitalize on pulsed laser in liquids synthesis to advance catalyst development, by leveraging the synergies of two fields of intensive research.
To investigate the relationships between history of falls and cholinergic vs dopaminergic denervation in patients with Parkinson disease (PD).
There is a need to explore nondopaminergic mechanisms of ...gait control as the majority of motor impairments associated with falls in PD are resistant to dopaminergic treatment. Alterations in cholinergic neurotransmission in PD may be implicated because of evidence that gait control depends on cholinergic system-mediated higher-level cortical and subcortical processing, including pedunculopontine nucleus (PPN) function.
In this cross-sectional study, 44 patients with PD (Hoehn & Yahr stages I-III) without dementia and 15 control subjects underwent a clinical assessment and (11)Cmethyl-4-piperidinyl propionate (PMP) acetylcholinesterase (AChE) and (11)Cdihydrotetrabenazine (DTBZ) vesicular monoamine transporter type 2 (VMAT2) brain PET imaging.
Seventeen patients (38.6%) reported a history of falls and 27 patients had no falls. Analysis of covariance of the cortical AChE hydrolysis rates demonstrated reduced cortical AChE in the PD fallers group (-12.3%) followed by the PD nonfallers (-6.6%) compared to control subjects (F = 7.22, p = 0.0004). Thalamic AChE activity was lower only in the PD fallers group (-11.8%; F = 4.36, p = 0.008). There was no significant difference in nigrostriatal dopaminergic activity between PD fallers and nonfallers.
Unlike nigrostriatal dopaminergic denervation, cholinergic hypofunction is associated with fall status in Parkinson disease (PD). Thalamic AChE activity in part represents cholinergic output of the pedunculopontine nucleus (PPN), a key node for gait control. Our results are consistent with other data indicating that PPN degeneration is a major factor leading to impaired postural control and gait dysfunction in PD.
An on-demand source of indistinguishable and entangled photon pairs is a fundamental component of various quantum information applications, including optical quantum computing, quantum repeaters, ...quantum teleportation and quantum communication. Parametric downconversion and four-wave mixing sources of entangled photons have shown high degrees of entanglement and indistinguishability, but the probabilistic nature of their generation process also creates zero or multiple photon pairs following a Poissonian distribution. This limits their use in complex algorithms where many qubits and gate operations are required. Here, we simultaneously show ultrahigh purity (g(2) (0) < 0.004), high entanglement fidelity (0.81 ± 0.02), high two-photon interference non-post selective visibilities (0.86 ± 0.03 and 0.71 ± 0.04) and on-demand generation (efficiency straight epsilonpair = 0.86 ± 0.08) of polarization-entangled photon pairs from a single semiconductor quantum dot. Through a two-photon resonant excitation scheme, the biexciton population is deterministically prepared by a π-pulse (straight epsilonbiexciton = 0.98 ± 0.07). Applied on a quantum dot showing no exciton fine-structure splitting, this results in the deterministic generation of indistinguishable entangled photon pairs.
Bioelectrical impedance analysis (BIA) provides noninvasive measures of skeletal muscle mass (SMM) and visceral adipose tissue (VAT). This study (i) analyzes the impact of conventional wrist-ankle vs ...segmental technology and standing vs supine position on BIA equations and (ii) compares BIA validation against magnetic resonance imaging (MRI) and dual X-ray absorptiometry (DXA).
One hundred and thirty-six healthy Caucasian adults (70 men, 66 women; age 40±12 years) were measured by a phase-sensitive multifrequency BIA (seca medical body composition analyzers 515 and 525). Multiple stepwise regression analysis was used to generate prediction equations. Accuracy was tested vs MRI or DXA in an independent multiethnic population.
Variance explained by segmental BIA equations ranged between 97% for total SMM
, 91-94% for limb SMM
and 80-81% for VAT with no differences between supine and standing position. When compared with segmental measurements using conventional wrist-ankle technology. the relationship between measured and predicted SMM was slightly deteriorated (r=0.98 vs r=0.99, P<0.05). Although BIA results correctly identified ethnic differences in muscularity and visceral adiposity, the comparison of bias revealed some ethnical effects on the accuracy of BIA equations. The differences between LST
and SMM
at the arms and legs were sizeable and increased with increasing body mass index.
A high accuracy of phase-sensitive BIA was observed with no difference in goodness of fit between different positions but an improved prediction with segmental compared with conventional wrist-ankle measurement. A correction factor for certain ethnicities may be required. When compared with DXA MRI-based BIA equations are more accurate for predicting muscle mass.
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