Electronic Asymmetry Research Articles

Electronic asymmetry of lattice oxygen sites in ZnO promotes the photocatalytic oxidative coupling of methane

Photocatalytic oxidative coupling of methane with oxygen is promising to obtain valuable muti-carbon products, yet suffering low reactivity. Here, we apply cerium modifications on zinc oxide-supported gold catalysts based on the electronic asymmetry design of lattice oxygen to improve the coupling activity. The methane conversion rate exceeds 16000 μmol g−1 h−1 with muti-carbon selectivity of 94.9% and catalytic durability of 3 days, and it can increase to 34000 μmol g−1 h−1 under more thermal assistance, with a turnover frequency of 507 h−1 for ethane and an apparent quantum efficiency of 33.7% at 350 nm. According to systematic characterizations and theoretical analysis, cerium dopants not only can boost the formation of reactive oxygen species but also intervene in the vivacity of lattice oxygen by manipulating metal-oxygen bond strength, thereby leading to favorable methyl desorption to form ethane and quick water release. This work provides insight into the rational design of efficient photocatalysts for aerobic methane-to-ethane conversion.

Van der Waals GeSe with Strain- and Gate-Tunable Linear Dichroism for Wearable Electronics.

The direct detection of light polarization poses a crucial challenge in the field of optoelectronics and photonics. Herein, the tunable linear dichroism (LD) in GeSe-based polarized photodetectors is presented through electronic and structural asymmetry modulation, and demonstrate their application prospects in wearable electronics. An improvement in the dichroic ratio up to 34% is achieved under a gate voltage of 20V, and the improvement reaches 44% by applying a tensile strain along the zigzag direction. Theoretical calculations reveal that the gate regulation of barrier height between GeSe and Au electrodes is responsible for the electrical-tunable LD, while the anisotropic optical absorption in response to strains leads to the strain-tunable LD. Moreover, flexible GeSe transistors are developed for wearable applications including motion sensors and glucose monitors. This study offers viable approaches for modulating the optical anisotropy of low-dimensional materials and emphasizes the versatility of van der Waals materials for practical applications in wearable electronic devices.

High Voltage Monolithic Active Pixel Sensors for the MOLLER experiment

The MOLLER experiment [1] aims to measure the parity-violating asymmetry (APV) in electron–electron scattering at 11 GeV, and thus determine the weak charge of the electron to a high precision (2.4%). Two of the key sub-systems in the experimental apparatus are the main detector array, consisting of 224 fused silica detector modules and an electron beam Compton polarimeter. The main detector array can be operated in either pulsed mode for particle tracking, or integration mode for the asymmetry measurement at high rate detection. A subset of these detector modules will be equipped with an array of High Voltage Monolithic Active Pixel Sensors (HVMAPS), to be used in particle tracking and allowing for real-time monitoring of the event profile in the main Møller region. HVMAPS are also used for the Compton polarimeter, consisting of four-plane planes of HVMAPS chips, housed in a vacuum chamber upstream of the interaction point. An overview of the implementation of the HVMAPS for the main detectors and Compton polarimeter is provided.

Plasma homogeneity over the extraction beamlet groups at the half size ITER negative ion source at ELISE test facility

The negative ion source for neutral beam injection at ITER has to provide high-intensity and low-divergence negative hydrogen and deuterium ion beams. Extracting the negative ions from the plasma is inevitably accompanied by co-extraction of electrons, which can limit the source performance, especially in deuterium. Reducing the co-extracted electrons is done by applying a magnetic filter field. On the one hand, the filter field reduces the electron temperature and the amount of co-extracted electrons, on the other hand, it introduces × B→ drifts. The drifts create a vertical plasma inhomogeneity in front of the extraction area and, consequently, an asymmetry of the co-extracted electrons. This motivated detailed studies on the vertical plasma inhomogeneity over the beamlet groups in the ELISE ion source using a movable Langmuir probe in deuterium plasma. It is demonstrated that the vertical distribution of the plasma potential changes together with the sheath, forming at the plasma grid – from electron repelling to attracting sheath. A repelling sheath reduces the flux of electrons from the plasma to the grid surface and consequently, more electrons are co-extracted. The attracting sheath collects the majority of electrons on the grid and reduces the co-extracted electrons.

Asymmetric Copper‐Sulphur Sites Promote C–C Coupling for Selective CO2 Electroreduction to C2 Products

AbstractSustainable multicarbon e‐chemicals are of particular interest due to their potential future, high market values, and demand. In the direct electrocatalytic formation of multicarbon e‐chemicals from CO2, the elementary C–C coupling by CO dimerization is considered the rate‐limiting step. Here, a generalized surface structural design principle of asymmetric metal pair sites is proposed, explored, and experimentally tested in order to promote CO dimerization on surfaces. First a computational model of N‐doped Cu2S layers featuring adjacent, electronically asymmetric Cuδ1+‐Cuδ2+ (0 < δ1+ < δ2+ < 1) metal atomic pairs evidenced by their non‐uniform charge distribution is considered. The electronic asymmetry resulted in distinct CO adsorption energies and the associated self‐adjusting structures, which lowered C–C coupling energy barriers significantly. The computational hypotheses are experimentally tested using X‐ray photoelectron spectroscopy of Cu‐N moieties within N‐doped Cu2S layers. In‐situ Fourier‐transform infrared spectroscopy confirms linear *CO and *CO‐CO adsorption configuration by the peaks of ≈2080 and 1920 cm−1, respectively. After N‐doping, the catalytically C2 faradaic efficiency can significantly be elevated to 14.72% due to the promotion of C–C coupling.

Neutron skin of 27Al with Skyrme and Korea-IBS-Daegu-SKKU density functionals

Recent measurement of the parity-violating (PV) asymmetry in the elastic electron scattering on [Formula: see text]Al target evokes the interest in the distribution of the neutron in the nucleus. In this work, we calculate the neutron skin thickness ([Formula: see text]) of [Formula: see text]Al with nonrelativistic nuclear structure models. We focus on the role of the effective mass, symmetry energy and pairing force. Models are selected to have effective masses in the range (0.58–1.05) M where M is the nucleon mass in free space, and stiffness of the symmetry energy is varied by choosing the slope of the symmetry energy in the range 9.4–100.5[Formula: see text]MeV. Effect of pairing force is investigated by calculating nuclear properties with and without pairing. With constant force pairing, we obtain [Formula: see text]–0.013[Formula: see text]fm. The result is independent of the effective mass and symmetry energy. However, [Formula: see text] is negative when the pairing force is switched off, so the pairing force plays an essential role to make [Formula: see text] positive and constrained in a narrow range. We also calculate the PV asymmetry ([Formula: see text]) in the elastic electron-[Formula: see text]Al scattering in the Born approximation at the kinematics of the Qweak experiment. We obtain a very narrow-ranged result [Formula: see text]. The result is consistent with the experiment and insensitive to the effective mass and symmetry energy.

Wash-in leptogenesis after the evaporation of primordial black holes

Wash-in leptogenesis is a powerful mechanism to generate the baryon asymmetry of the Universe that treats right-handed-neutrino interactions on the same footing as electroweak sphaleron processes: as mere spectator processes acting on the background of chemical potentials in the Standard Model plasma. Successful wash-in leptogenesis requires this chemical background to be CP-violating, which can be achieved by violating any of the more than ten global charges that are conserved in the Standard Model at very high temperatures. In this paper, we demonstrate that the primordial charge asymmetries required for wash-in leptogenesis can be readily produced by evaporating primordial black holes (PBHs). Our argument is based on the fact that the Hawking radiation emitted by PBHs contains more or less any state in the particle spectrum. Therefore, if heavy states with CP-violating decays are present in the ultraviolet, PBH evaporation will unavoidably lead to the production of these states. We illustrate this scenario by means of a simple toy model where PBH evaporation leads to the production of heavy particles that we call asymmetrons and whose decay results in a primordial charge asymmetry for right-handed electrons, which in turn sets the initial conditions for wash-in leptogenesis. We focus on the parameter region where the decay of the initial thermal asymmetron abundance occurs long before PBH evaporation and only results in a negligible primordial charge asymmetry. PBH evaporation at later times then serves as a mechanism to resurrect the asymmetron abundance and ensure the successful generation of the baryon asymmetry after all. We conclude that PBHs can act as asymmetry-producing machines that grant access to whatever CP-violating physics may be present in the ultraviolet, rekindling it at lower energies where it can be reprocessed into a baryon asymmetry by right-handed neutrinos.

Heptacyclic aromatic hydrocarbon isomers with two azulene units fused.

Azulene, known for its unique electronic properties and structural asymmetry, serves as a promising building block for the design of novel non-benzenoid polycyclic aromatic hydrocarbons (PAHs). Herein, we present the synthesis, characterization, and physical properties of three diazulene-fused heptacyclic aromatic hydrocarbons, 8,17-dioctyldiazuleno[2,1-a:2',1'-h]anthracene (trans configuration), 16,18-dioctyldiazuleno[2,1-a:1',2'-j]anthracene (cis configuration) and 3,18-dioctyldiazuleno[2,1-a:1',2'-i]phenanthrene (zigzag configuration). Three compounds are configurational isomers with different fusing patterns of aromatic rings. All three isomers exhibit pronounced aromaticity, as revealed by nuclear magnetic resonance spectroscopy and theoretical calculations. They exhibit characteristics of both azulene and benzenoid PAHs and are much more stable than their all-benzene analogues. The optical and electrochemical properties of these three isomers were investigated through UV-vis absorption spectra and cyclic voltammetry, revealing distinct behaviors influenced by their molecular configurations. Furthermore, the isomer in trans configuration exhibits promising semiconducting properties with a hole mobility of up to 0.22 cm2 V-1 s-1, indicating its potential in organic electronics applications.

Homogeneous Dephasing in Photosynthetic Bacterial Reaction Centers: Time Correlation Function Approach.

A new tractable linear electronic transition dipole moment time correlation function (ETDMTCF) that accurately accounts for electronic dephasing, asymmetry, and width of 1-phonon profile, which the zero-phonon line (ZPL) contributes to it, in Rhodopseudomonas viridis bacterial reaction center is derived. This time correlation function proves to be superior to other frequency-domain expressions in case of strong electron-phonon coupling (which is often the case in bacterial RCs and pigment-protein complexes), many vibrational modes involved, and high temperature, whereby more vibronic and electronic (sequence) transitions would arise. The Fourier transform of this ETDMTCF leads to asymmetric multiphonon profiles composed of Lorentzian distribution and Gaussian distribution on the high- and low-energy sides, respectively, whereby the overtone widths fold themselves with that of the one-phonon profile. This ETDMTCF also features expedient computation in large systems using asymmetric phonon profiles to account correctly for dephasing and pigment-protein interaction (electron-phonon coupling). The derived ETDMTCF allows computing all nonlinear optical signals in both time and frequency domains, through the nonlinear dipole moment time correlation functions (as guided by nonlinear optical response theory) in line with the eight Liouville space pathways. The linear transition dipole moment time correlation function is of a central value as the nonlinear transition dipole moment time correlation function is expressed in terms of the linear transition dipole moment time correlation function, derived herein. One of the great advantages of presenting this ETDMTCF is its applicability to nonlinear transition dipole moment time correlation functions in line with the eight Liouville space pathways needed in computing nonlinear signals. As such, there is more to the utility and applicability of the presented ETDMTCF besides computational expediency and efficiency. Results show good agreement with the reported literature. The intimate connection between a one-phonon profile and the corresponding bath spectral density in photosynthetic complexes is discussed.

Dawn‐Dusk Asymmetry of Energetic Electron at LEO During a Storm: Observation by FY3E

AbstractElectrons in Low Earth Orbit (LEO) have been a popular research topic since the early days of space exploration. However, due to the limited pitch angle coverage and energy resolution of past in‐situ measurements, there is still much to uncover about the radiation environment. Fortunately, the recently launched satellite FY3E, which is equipped with the Medium‐Energy Electron Detector, is changing this. FY3E is the world's first early‐morning‐orbit meteorological satellite for civil use. With the ability to provide full pitch angle coverage and discrete energy measurements of 30–600 keV electrons, we now have an unprecedented opportunity to investigate the dynamics of space radiation at LEO and Magnetosphere‐Ionosphere coupling. Using the newly available measurements, we have discovered that during storms, electron precipitation exhibits dawn‐dusk asymmetry up to 100 keV. At dawn sector downward electrons can be similar to trapped electrons, and the loss cone ratio (precipitating flux over trapped flux) can be as high as unity at L‐shell greater than 6. While at dusk barely precipitation can be seen. The flux of trapped, upward, downward and net precipitation are calculated, and separate energy flux spectra of downward, upward, and trapped electrons are presented for the first time. With significant upward electrons up to 200 keV, asymmetric local pitch angle is observed at dawn within intense precipitation. In light of these findings, FY3E reveals critical information for understanding the Magnetosphere‐Ionosphere Coupling process.

Electronic Asymmetry Engineering of Fe-N-C Electrocatalyst via Adjacent Carbon Vacancy for Boosting Oxygen Reduction Reaction.

Single-atomic transition metal-nitrogen-carbon (M-N-C) structures are promising alternatives toward noble-metal-based catalysts for oxygen reduction reaction (ORR) catalysis involved in sustainable energy devices. The symmetrical electronic density distribution of the M─N4 moieties, however, leads to unfavorable intermediate adsorption and sluggish kinetics. Herein, a Fe-N-C catalyst with electronic asymmetry induced by one nearest carbon vacancy adjacent to Fe─N4 is conceptually produced, which induces an optimized d-band center, lowered free energy barrier, and thus superior ORR activity with a half-wave potential (E1/2 ) of 0.934V in a challenging acidic solution and 0.901V in an alkaline solution. When assembled as the cathode of a Zinc-air battery (ZAB), a peak power density of 218mW cm-2 and long-term durability up to 200h are recorded, 1.5 times higher than the noble metal-based Pt/C+RuO2 catalyst. This work provides a new strategy on developing efficient M-N-C catalysts and offers an opportunity for the real-world application of fuel cells and metal-air batteries.

Facile and Scalable Mechanochemical Synthesis of Defective MoS2 with Ru Single Atoms Toward High-Current-Density Hydrogen Evolution.

Designing a facile strategy to prepare catalysts with highly active sites are challenging for large-scale implementation of electrochemical hydrogen production. Herein, a straightforward and eco-friendly method by high-energy mechanochemical ball milling for mass production of atomic Ru dispersive in defective MoS2 catalysts (Ru1 @D-MoS2 ) is developed. It is found that single atomic Ru doping induces the generation of S vacancies, which can break the electronic neutrality around Ru atoms, leading to an asymmetrical distribution of electrons. It is also demonstrated that the Ru1 @D-MoS2 exhibits superb alkaline hydrogen evolution enhancement, possibly attributing to this electronic asymmetry. The overpotential required to deliver a current density of 10mA cm-2 is as low as 107mV, which is much lower than that of commercial MoS2 (C-MoS2 , 364mV). Further density functional theory (DFT) calculations also support that the vacancy-coupled single Ru enables much higher electronic distribution asymmetry degree, which could regulate the adsorption energy of intermediates, favoring the water dissociation and the adsorption/desorption of H*. Besides, the long-term stability test under 500mA cm-2 further confirms the robust performance of Ru1 @D-MoS2 . Ourstrategy provides a promising and practical way towards large-scale preparation of advanced HER catalysts for commercial applications.

Searching for new physics from SMEFT and leptoquarks at the P2 experiment

The P2 experiment aims at high-precision measurements of the parity-violating asymmetry in elastic electron-proton and electron-$^{12}$C scatterings with longitudinally polarized electrons. We discuss here the sensitivity of P2 to leptoquarks, which within the P2 energy range can be described in the language of Standard Model Effective Field Theory (SMEFT). We give the expected P2 limits on the SMEFT operators and on the leptoquark parameters, which will test energy scales up to 15 TeV. In many cases those limits exceed current constraints from LHC and atomic parity violation (APV) experiments. We also demonstrate that degeneracies of different SMEFT operators can partially be resolved by use of APV experiments and different targets (protons and $^{12}$C) at P2. Moreover, we show that P2 could confirm or resolve potential tensions between the theoretical and experimental determinations of the weak charge of $^{133}$Cs.

Electric fields and substrates dramatically accelerate spin relaxation in graphene

Electrons in graphene are theoretically expected to retain spin states much longer than most materials, making graphene a promising platform for spintronics and quantum information technologies. Here, we use first-principles density-matrix (FPDM) dynamics simulations to show that interaction with electric fields and substrates strongly enhance spin relaxation through scattering with phonons. Consequently, the relaxation time at room temperature reduces from microseconds in free-standing graphene to nanoseconds in graphene on hexagonal boron nitride (hBN) substrate, the order of magnitude typically measured in experiments. Further, inversion symmetry breaking by hBN introduces a stronger asymmetry in electron and hole spin lifetimes, than predicted by the conventional D'yakonov-Perel' (DP) model for spin relaxation. Deviations from the conventional DP model are stronger for in-plane spin relaxation, resulting in out-of-plane to in-plane lifetime ratios much greater than 1/2 with a maximum close to the Dirac point. These FPDM results, independent of symmetry-specific assumptions or material-dependent parameters, also validate recent modifications of the DP model to explain such deviations. Overall, our results indicate that spin-phonon relaxation in the presence of substrates may be more important in graphene than typically assumed, requiring consideration for graphene-based spin technologies at room temperature.

Effects of magnetic field on the secondary electron asymmetry effect in capacitively coupled plasmas

The secondary electron asymmetry effect (SEAE) provides the opportunity to generate the dc self-bias voltage and asymmetric plasma response, where secondary electron emission coefficients at both electrodes are unequal. In this work, we use one-dimensional implicit particle-in-cell/Monte Carlo collision simulation to investigate the effects of the homogeneous and inhomogeneous magnetic field on the SEAE. The magnetic field is applied parallel to electrodes, and the discharge is operated in a geometrically and electrically symmetric capacitively coupled argon plasma. By comparing the simulation results of the effects of the homogeneous and inhomogeneous magnetic field on the SEAE, the homogeneous magnetic field can increase the dc self-bias voltage to a certain extent and has little effect on the plasma density distribution. The inhomogeneous magnetic field is more advantageous in generating the dc self-bias but at the cost of uneven plasma density distribution. In addition, by comparing the results of inhomogeneous magnetic fields with opposite gradients, we found that the value of the self-bias voltage can be changed by adjusting the magnetic field gradient. Aside from that the roles of two electrodes can be easily reversed by changing the slopes of the magnetic field gradient. The results suggest that such a configuration could be desired in the microelectronics industry, since the controllable self-bias voltage is needed for deposition and etching processes.

Resonant elastic scattering of polarized electrons on H-like ions

The polarization properties of the elastic electron scattering on H-like ions are investigated within the framework of the relativistic QED theory. The polarization properties are determined by a combination of relativistic effects and spin exchange between the incident and bound electrons. The scattering of a polarized electron on an initially unpolarized ion is fully described by five parameters. We study these parameters for non-resonant scattering, as well as in the vicinity of LL resonances, where scattering occurs through the formation and subsequent decay of intermediate autoionizing states. The study was carried out for ions from $\txt{B}^{4+}$ to $\txt{Xe}^{53+}$. Special attention was paid to the study of asymmetry in electron scattering.

Measurement of the charge asymmetry of electrons from the decays of W bosons produced in pp¯ collisions at s=1.96 TeV

At the Fermilab Tevatron proton-antiproton (pp¯) collider, high-mass electron-neutrino (eν) pairs are produced predominantly in the process pp¯→W(→eν)+X. The asymmetry of the electron and positron yield as a function of their pseudorapidity constrain the slope of the ratio of the u- to d-quark parton distributions versus the fraction of the proton momentum carried by the quarks. This paper reports on the measurement of the electron-charge asymmetry using the full data set recorded by the Collider Detector at Fermilab in 2001–2011 and corresponding to 9.1 fb−1 of integrated luminosity. The measurement significantly improves the precision of the Tevatron constraints on the parton-distribution functions of the proton. Numerical tables of the measurement are provided.18 MoreReceived 9 July 2021Accepted 29 September 2021DOI:https://doi.org/10.1103/PhysRevD.104.092002Published by the American Physical Society under the terms of the Creative Commons Attribution 4.0 International license. Further distribution of this work must maintain attribution to the author(s) and the published article’s title, journal citation, and DOI. Funded by SCOAP3.Published by the American Physical SocietyPhysics Subject Headings (PhySH)Research AreasHadron-hadron interactionsW & Z bosonsPhysical SystemsElectronsParticles & Fields

NNBI for ITER: status of long pulses in deuterium at the test facilities BATMAN Upgrade and ELISE

For the D-T operational phase of the international fusion experiment ITER, starting in 2035, pulses are planned with Q > 10 and a duration of 400 s and pulses with Q = 5 for up to 3600 s. The two neutral beam injection (NBI) systems will deliver 33.3 MW of heating power to the plasma and will also be an important source for non-inductive current drive. An essential part of the NBI systems is a large RF driven source for negative hydrogen or deuterium ions. In order to fulfil the requirements imposed to the NBI system, the ion source has to deliver an intense, stable and homogeneous large negative ion beam over pulse lengths of 400 s or 3600 s. Till now, long pulses in deuterium at the extracted negative ion current density required for ITER could not be demonstrated. The achievable performance is limited by a high current and a pronounced vertical asymmetry of the co-extracted electrons, both strongly increasing with time, whereas the stability of the negative deuterium ions is not an issue. For reduced performance, i.e. reduced negative ion current, lower and more stable co-extracted electron currents are observed, making possible pulses up to 3600 s (using pulsed extraction). One main aim of ongoing investigations at the two test facilities BATMAN Upgrade (Bavarian test machine for negative ions) and ELISE (extraction from a large ion source experiment) is the development of scenarios stabilizing and symmetrizing the co-extracted electron current in deuterium. These investigations are discussed and the current status of hardware upgrades ongoing at BATMAN Upgrade and ELISE towards the ITER scenario of one-hour steady state extraction is presented.

Molecular Alignment of Homoleptic Iridium Phosphors in Organic Light-Emitting Diodes.

The orientation of facial (fac) tris-cyclometalated iridium complexes in doped films prepared by vacuum deposition is investigated by altering the physical shape and electronic asymmetry in the molecular structure. Angle-dependent photoluminescence spectroscopy and Fourier-plane imaging microscopy show that the orientation of roughly spherical fac-tris(2-phenylpyridyl)iridium (Ir(ppy)3 ) is isotropic, whereas complexes that are oblate spheroids, fac-tris(mesityl-2-phenyl-1H-imidazole)iridium (Ir(mi)3 ) and fac-tris((3,5-dimethyl-[1,1'-biphenyl]-4-yl)-2-phenyl-1H-imidazole)iridium (Ir(mip)3 ), have a net horizontal alignment of their transition dipole moments. Optical anisotropy factors of 0.26 and 0.15, respectively, are obtained from the latter complexes when doped into tris(4-(9H-carbazol-9-yl)phenyl)amine host thin films. The horizontal alignment is attributed to the favorable van der Waals interaction between the oblate Ir complexes and host material. Trifluoromethyl groups substituted on one polar face of the Ir(ppy)3 and Ir(mi)3 complexes introduce chemical asymmetries in the molecules at the expense of their oblate shapes. The anisotropy factors of films doped with these substituted derivatives are lower relative to the parent complexes, indicating that the fluorinated patches reinforce horizontal alignment during deposition. High efficiencies obtained from organic light emitting diodes prepared using the Ir dopants is attributed, in part, to improved outcoupling of electroluminescence brought about by molecular alignment.

Beam-normal single-spin asymmetry in elastic scattering of electrons from a spin-0 nucleus

We study the beam-normal single-spin asymmetry (BNSSA) in high-energy elastic electron scattering from several spin-0 nuclei. Existing theoretical approaches work in the plane-wave formalism and predict the BNSSA to scale as $\ensuremath{\sim}A/Z$ with the atomic number $Z$ and nuclear mass number $A$. While this prediction holds for light and intermediate nuclei, a striking disagreement in both the sign and the magnitude of BNSSA was observed by the PREX collaboration for $^{208}\mathrm{Pb}$, coined the ``PREX puzzle.'' To shed light on this disagreement, we go beyond the plane-wave approach which neglects Coulomb distortions known to be significant for heavy nuclei. We explicitly investigate the dependence of BNSSA on $A$ and $Z$ by (i) including inelastic intermediate states' contributions into the Coulomb problem in the form of an optical potential, (ii) by accounting for the experimental information on the $A$-dependence of the Compton slope parameter, and (iii) giving a thorough account of the uncertainties of the calculation. Despite of these improvements, the PREX puzzle remains unexplained. We discuss further strategies to resolve this riddle.