Intertwined spin, charge, and pair correlations in the two-dimensional Hubbard model in the thermodynamic limit.

The high-temperature superconducting cuprates are governed by intertwined spin, charge, and superconducting orders. While various state-of-the-art numerical methods have demonstrated that these phases also manifest themselves in doped Hubbard models, they differ on which is the actual ground state. Finite-cluster methods typically indicate that stripe order dominates, while embedded quantum-cluster methods, which access the thermodynamic limit by treating long-range correlations with a dynamical mean field, conclude that superconductivity does. Here, we report the observation of fluctuating spin and charge stripes in the doped single-band Hubbard model using a quantum Monte Carlo dynamical cluster approximation (DCA) method. By resolving both the fluctuating spin and charge orders using DCA, we demonstrate that they survive in the doped Hubbard model in the thermodynamic limit. This discovery also provides an opportunity to study the influence of fluctuating stripe correlations on the model's pairing correlations within a unified numerical framework. Using this approach, we also find evidence for pair-density-wave correlations whose strength is correlated with that of the stripes.

Polymorph Identification for Flexible Molecules: Linear Regression Analysis of Experimental and Calculated Solution- and Solid-State NMR Data.

The Δδ regression approach of Blade et al. [ J. Phys. Chem. A 2020, 124(43), 8959-8977] for accurately discriminating between solid forms using a combination of experimental solution- and solid-state NMR data with density functional theory (DFT) calculation is here extended to molecules with multiple conformational degrees of freedom, using furosemide polymorphs as an exemplar. As before, the differences in measured 1H and 13C chemical shifts between solution-state NMR and solid-state magic-angle spinning (MAS) NMR (Δδexperimental) are compared to those determined by gauge-including projector augmented wave (GIPAW) calculations (Δδcalculated) by regression analysis and a t-test, allowing the correct furosemide polymorph to be precisely identified. Monte Carlo random sampling is used to calculate solution-state NMR chemical shifts, reducing computation times by avoiding the need to systematically sample the multidimensional conformational landscape that furosemide occupies in solution. The solvent conditions should be chosen to match the molecule's charge state between the solution and solid states. The Δδ regression approach indicates whether or not correlations between Δδexperimental and Δδcalculated are statistically significant; the approach is differently sensitive to the popular root mean squared error (RMSE) method, being shown to exhibit a much greater dynamic range. An alternative method for estimating solution-state NMR chemical shifts by approximating the measured solution-state dynamic 3D behavior with an ensemble of 54 furosemide crystal structures (polymorphs and cocrystals) from the Cambridge Structural Database (CSD) was also successful in this case, suggesting new avenues for this method that may overcome its current dependency on the prior determination of solution dynamic 3D structures.

Multiorbital charge-density wave excitations and concomitant phonon anomalies in Bi2Sr2LaCuO6+δ.

Charge-density waves (CDWs) are ubiquitous in underdoped cuprate superconductors. As a modulation of the valence electron density, CDWs in hole-doped cuprates possess both Cu-3d and O-2p orbital character owing to the strong hybridization of these orbitals near the Fermi level. Here, we investigate underdoped Bi2Sr1.4La0.6CuO6+δ using resonant inelastic X-ray scattering (RIXS) and find that a short-range CDW exists at both Cu and O sublattices in the copper-oxide (CuO2) planes with a comparable periodicity and correlation length. Furthermore, we uncover bond-stretching and bond-buckling phonon anomalies concomitant to the CDWs. Comparing to slightly overdoped Bi2Sr1.8La0.2CuO6+δ, where neither CDWs nor phonon anomalies appear, we highlight that a sharp intensity anomaly is induced in the proximity of the CDW wavevector (QCDW) for the bond-buckling phonon, in concert with the diffused intensity enhancement of the bond-stretching phonon at wavevectors much greater than QCDW Our results provide a comprehensive picture of the quasistatic CDWs, their dispersive excitations, and associated electron-phonon anomalies, which are key for understanding the competing electronic instabilities in cuprates.

Polaronic behavior in a weak-coupling superconductor.

The nature of superconductivity in the dilute semiconductor SrTiO3 has remained an open question for more than 50 y. The extremely low carrier densities ([Formula: see text]-[Formula: see text] cm-3) at which superconductivity occurs suggest an unconventional origin of superconductivity outside of the adiabatic limit on which the Bardeen-Cooper-Schrieffer (BCS) and Migdal-Eliashberg (ME) theories are based. We take advantage of a newly developed method for engineering band alignments at oxide interfaces and access the electronic structure of Nb-doped SrTiO3, using high-resolution tunneling spectroscopy. We observe strong coupling to the highest-energy longitudinal optic (LO) phonon branch and estimate the doping evolution of the dimensionless electron-phonon interaction strength ([Formula: see text]). Upon cooling below the superconducting transition temperature ([Formula: see text]), we observe a single superconducting gap corresponding to the weak-coupling limit of BCS theory, indicating an order of magnitude smaller coupling ([Formula: see text]). These results suggest that despite the strong normal state interaction with electrons, the highest LO phonon does not provide a dominant contribution to pairing. They further demonstrate that SrTiO3 is an ideal system to probe superconductivity over a wide range of carrier density, adiabatic parameter, and electron-phonon coupling strength.

Superconductivity in a Hole-Doped Mott-Insulating Triangular Adatom Layer on a Silicon Surface.

Adsorption of one-third monolayer of Sn on an atomically clean Si(111) substrate produces a two-dimensional triangular adatom lattice with one unpaired electron per site. This dilute adatom reconstruction is an antiferromagnetic Mott insulator; however, the system can be modulation doped and metallized using heavily doped p-type Si(111) substrates. Here, we show that the hole-doped dilute adatom layer on a degenerately doped p-type Si(111) wafer is superconducting with a critical temperature of 4.7±0.3 K. While a phonon-mediated coupling scenario would be consistent with the observed T_{c}, Mott correlations in the Sn-derived dangling-bond surface state could suppress the s-wave pairing channel. The latter suggests that the superconductivity in this triangular adatom lattice may be unconventional.

City Scale Particulate Matter Monitoring Using LoRaWAN Based Air Quality IoT Devices.

Air Quality (AQ) is a very topical issue for many cities and has a direct impact on citizen health. The AQ of a large UK city is being investigated using low-cost Particulate Matter (PM) sensors, and the results obtained by these sensors have been compared with government operated AQ stations. In the first pilot deployment, six AQ Internet of Things (IoT) devices have been designed and built, each with four different low-cost PM sensors, and they have been deployed at two locations within the city. These devices are equipped with LoRaWAN wireless network transceivers to test city scale Low-Power Wide Area Network (LPWAN) coverage. The study concludes that (i) the physical device developed can operate at a city scale; (ii) some low-cost PM sensors are viable for monitoring AQ and for detecting PM trends; (iii) LoRaWAN is suitable for city scale sensor coverage where connectivity is an issue. Based on the findings from this first pilot project, a larger LoRaWAN enabled AQ sensor network is being deployed across the city of Southampton in the UK.

Correlation of Fe-Based Superconductivity and Electron-Phonon Coupling in an FeAs/Oxide Heterostructure.

Interfacial phonons between iron-based superconductors (FeSCs) and perovskite substrates have received considerable attention due to the possibility of enhancing preexisting superconductivity. Using scanning tunneling spectroscopy, we studied the correlation between superconductivity and e-ph interaction with interfacial phonons in an iron-based superconductor Sr_{2}VO_{3}FeAs (T_{c}≈33 K) made of alternating FeSC and oxide layers. The quasiparticle interference measurement over regions with systematically different average superconducting gaps due to the e-ph coupling locally modulated by O vacancies in the VO_{2} layer, and supporting self-consistent momentum-dependent Eliashberg calculations provide a unique real-space evidence of the forward-scattering interfacial phonon contribution to the total superconducting pairing.

Switching Magnetism and Superconductivity with Spin-Polarized Current in Iron-Based Superconductor.

We explore a new mechanism for switching magnetism and superconductivity in a magnetically frustrated iron-based superconductor using spin-polarized scanning tunneling microscopy (SPSTM). Our SPSTM study on single-crystal Sr_{2}VO_{3}FeAs shows that a spin-polarized tunneling current can switch the Fe-layer magnetism into a nontrivial C_{4} (2×2) order, which cannot be achieved by thermal excitation with an unpolarized current. Our tunneling spectroscopy study shows that the induced C_{4} (2×2) order has characteristics of plaquette antiferromagnetic order in the Fe layer and strongly suppresses superconductivity. Also, thermal agitation beyond the bulk Fe spin ordering temperature erases the C_{4} state. These results suggest a new possibility of switching local superconductivity by changing the symmetry of magnetic order with spin-polarized and unpolarized tunneling currents in iron-based superconductors.

3D Histopathology-a Lung Tissue Segmentation Workflow for Microfocus X-ray-Computed Tomography Scans.

Lung histopathology is currently based on the analysis of 2D sections of tissue samples. The use of microfocus X-ray-computed tomography imaging of unstained soft tissue can provide high-resolution 3D image datasets in the range of 2-10 µm without affecting the current diagnostic workflow. Important details of structural features such as the tubular networks of airways and blood vessels are contained in these datasets but are difficult and time-consuming to identify by manual image segmentation. Providing 3D structures permits a better understanding of tissue functions and structural interrelationships. It also provides a more complete picture of heterogeneous samples. In addition, 3D analysis of tissue structure provides the potential for an entirely new level of quantitative measurements of this structure that have previously been based only on extrapolation from 2D sections. In this paper, a workflow for segmenting such 3D images semi-automatically has been created using and extending the ImageJ open-source software and key steps of the workflow have been integrated into a new ImageJ plug-in called LungJ. Results indicate an improved workflow with a modular organization of steps facilitating the optimization for different sample and scan properties with expert input as required. This allows for incremental and independent optimization of algorithms leading to faster segmentation. Representation of the tubular networks in samples of human lung, building on those segmentations, has been demonstrated using this approach.

Host Phenology and Leaf Effects on Susceptibility of California Bay Laurel to Phytophthora ramorum.

Spread of the plant pathogen Phytophthora ramorum, causal agent of the forest disease sudden oak death, is driven by a few competent hosts that support spore production from foliar lesions. The relationship between traits of a principal foliar host, California bay laurel (Umbellularia californica), and susceptibility to P. ramorum infection were investigated with multiple P. ramorum isolates and leaves collected from multiple trees in leaf-droplet assays. We examined whether susceptibility varies with season, leaf age, or inoculum position. Bay laurel susceptibility was highest during spring and summer and lowest in winter. Older leaves (>1 year) were more susceptible than younger ones (8 to 11 months). Susceptibility was greater at leaf tips and edges than the middle of the leaf. Leaf surfaces wiped with 70% ethanol were more susceptible to P. ramorum infection than untreated leaf surfaces. Our results indicate that seasonal changes in susceptibility of U. californica significantly influence P. ramorum infection levels. Thus, in addition to environmental variables such as temperature and moisture, variability in host plant susceptibility contributes to disease establishment of P. ramorum.

A New Generation of Antiplatelet, and Anticoagulant Medication and the Implications for the Dental Surgeon.

The management of dental patients taking either antiplatelet medication, anticoagulant medication or both has been well established in the previous literature. Recently, new generations of drugs have emerged which are becoming increasingly common, including direct thrombin inhibitors, factor X inhibitors and a new class of oral thienopyridines. The implications of these drugs for the dental surgeon are not yet fully known. Awareness remains low and there is very little information available within the literature on safe use during surgery. This review paper aims to provide some guidance for dental practitioners performing invasive procedures. CPD/CLINICAL RELEVANCE: A new generation of anticoagulant and antiplatelet drugs have serious implications for patients undergoing surgery and their use is increasing.

Elucidating the Role of InGaAs and InAlAs Buffers on Carrier Dynamics of Tensile-Strained Ge Double Heterostructures.

Extensive research efforts of strained germanium (Ge) are currently underway due to its unique properties, namely, (i) possibility of band gap and strain engineering to achieve a direct band gap, thus exhibiting superior radiative properties, and (ii) higher electron and hole mobilities than Si for upcoming technology nodes. Realizing lasing structures is vital to leveraging the benefits of tensile-strained Ge (ε-Ge). Here, we use a combination of different analytical tools to elucidate the effect of the underlying InGaAs/InAlAs and InGaAs overlaying heterostructures on the material quality and strain state of ε-Ge grown by molecular beam epitaxy. Using X-ray analysis, we show the constancy of tensile strain in sub-50 nm ε-Ge in a quantum-well (QW) heterostructure. Further, effective carrier lifetime using photoconductive decay as a function of buffer type exhibited a high (low) defect-limited carrier lifetime of ∼68 ns (∼13 ns) in 0.61% (0.66%) ε-Ge grown on an InGaAs (InAlAs) buffer. These results correspond well with the measured surface roughness of 1.289 nm (6.303 nm), consistent with the surface effect of the ε-Ge/III-V heterointerface. Furthermore, a reasonably high effective lifetime of ∼78 ns is demonstrated in a QW of ∼30 nm 1.6% ε-Ge, a moderate reduction from ∼99 ns in uncapped ε-Ge, alluding to the surface effect of the overlying heterointerface. Thus, the above results highlight the prime quality of ε-Ge that can be achieved via III-V heteroepitaxy and paves a path for integrated Ge photonics.

GeSn-on-GaAs with photoconductive carrier lifetime >400 ns: role of substrate orientation and atomistic simulation.

Group IV GeSn quantum material finds application in electronics and silicon-compatible photonics. Synthesizing these materials with low defect density and high carrier lifetime is a potential challenge due to lattice mismatch induced defects and tin segregation at higher growth temperature. Recent advancements in the growth of these GeSn materials on Si, Ge, GaAs, and with substrate orientations, demonstrated different properties using epitaxial and chemical deposition methods. This article addresses the effect of GaAs substrate orientation and misorientation on the materials' properties and carrier lifetimes in epitaxial Ge0.94Sn0.06 layers. With starting GaAs substrates of (100)/2°, (100)/6°, (110) and (111)A orientations, Ge0.94Sn0.06 epitaxial layers were grown with an intermediate Ge buffer layer by molecular beam epitaxy and analyzed by several analytical tools. X-ray analysis displayed good crystalline quality, and Raman spectroscopy measurements showed blue shifts in phonon wavenumber due to biaxial compressive strain in Ge0.94Sn0.06 epilayers. Cross-sectional transmission electron microscopy analysis confirmed the defect-free heterointerface of Ge0.94Sn0.06/Ge/GaAs heterostructure. Minority carrier lifetimes of the unintentionally doped n-type Ge0.94Sn0.06 epilayers displayed photoconductive carrier lifetimes of >400 ns on (100)/6°, 319 ns on (100)/2°, and 434 ns on (110) GaAs substrate at 1500 nm excitation wavelength. On the other hand, Ge0.94Sn0.06 layer showed poor carrier lifetime on (111)A GaAs substrate. The observed differences in carrier lifetimes were correlated with the formation energy of the Ge on (100)/6° and (100)/2° GaAs heterointerface using Stillinger-Weber interatomic potential model-based atomistic simulation with different heterointerfacial bonding by Synopsys QuantumATK tool. Total energy computation of 6280-atom Ge/GaAs supercell on (100)/6° leads to lower formation energy than (100)/2°, making it more thermodynamically stable. Hence, the growth of the GeSn/III-V material system using misoriented (100) substrates that are more thermodynamically stable will enhance the performances of optoelectronic devices.

Investigation of Sub-Bandgap Emission and Unexpected n-Type Behavior in Undoped Polycrystalline CdSexTe1-x.

Se alloying has enabled significantly higher carrier lifetimes and photocurrents in CdTe solar cells, but these benefits can be highly dependent on CdSexTe1-x processing. This work evaluates the optoelectronic, chemical, and electronic properties of thick (3 µm) undoped CdSexTe1-x of uniform composition and varied processing conditions (CdSexTe1-x evaporation rate, CdCl2 anneal, Se content) chosen to reflect various standard device processing conditions. Sub-bandgap defect emission is observed, which increased as Se content increased and with "GrV-optimized CdCl2" (i.e., CdCl2 anneal conditions used for group-V-doped devices). Low carrier lifetime is found for GrV-optimized CdCl2, slow CdSexTe1-x deposition, and low-Se films. Interestingly, all films (including CdTe control) exhibited n-type behavior, where electron density increased with Se up to an estimated ≈1017 cm-3. This behavior appears to originate during the CdCl2 anneal, possibly from Se diffusion leading to anion vacancy (e.g., VSe, VTe) and ClTe generation.

Cooperative catalysis: combining an achiral metal catalyst with a chiral Brønsted acid enables highly enantioselective hydrogenation of imines.

Asymmetric hydrogenation of imines leads directly to chiral amines, one of the most important structural units in chemical products, from pharmaceuticals to materials. However, highly effective catalysts are rare. This article reveals that combining an achiral pentamethylcyclopentadienyl (Cp*)-iridium complex with a chiral phosphoric acid affords a catalyst that allows for highly enantioselective hydrogenation of imines derived from aryl ketones, as well as those derived from aliphatic ones, with ee values varying from 81 to 98 %. A range of achiral iridium complexes containing diamine ligands were examined, for which the ligands were shown to have a profound effect on the reaction rate, enantioselectivity and catalyst deactivation. The chiral phosphoric acid is no less important, inducing enantioselection in the hydrogenation. The induction occurs, however, at the expense of the reaction rate.

Group-equivariant autoencoder for identifying spontaneously broken symmetries.

We introduce the group-equivariant autoencoder (GE autoencoder), a deep neural network (DNN) method that locates phase boundaries by determining which symmetries of the Hamiltonian have spontaneously broken at each temperature. We use group theory to deduce which symmetries of the system remain intact in all phases, and then use this information to constrain the parameters of the GE autoencoder such that the encoder learns an order parameter invariant to these "never-broken" symmetries. This procedure produces a dramatic reduction in the number of free parameters such that the GE-autoencoder size is independent of the system size. We include symmetry regularization terms in the loss function of the GE autoencoder so that the learned order parameter is also equivariant to the remaining symmetries of the system. By examining the group representation by which the learned order parameter transforms, we are then able to extract information about the associated spontaneous symmetry breaking. We test the GE autoencoder on the 2D classical ferromagnetic and antiferromagnetic Ising models, finding that the GE autoencoder (1) accurately determines which symmetries have spontaneously broken at each temperature; (2) estimates the critical temperature in the thermodynamic limit with greater accuracy, robustness, and time efficiency than a symmetry-agnostic baseline autoencoder; and (3) detects the presence of an external symmetry-breaking magnetic field with greater sensitivity than the baseline method. Finally, we describe various key implementation details, including a quadratic-programming-based method for extracting the critical temperature estimate from trained autoencoders and calculations of the DNN initialization and learning rate settings required for fair model comparisons.

Flexible class of exact Hubbard-Stratonovich transformations.

We consider a class of Hubbard-Stratonovich transformations suitable for treating Hubbard interactions in the context of quantum Monte Carlo simulations. A tunable parameter p allows us to continuously vary from a discrete Ising auxiliary field (p=∞) to a compact auxiliary field that couples to electrons sinusoidally (p=0). In tests on the single-band square and triangular Hubbard models, we find that the severity of the sign problem decreases systematically with increasing p. Selecting p finite, however, enables continuous sampling methods such as the Langevin or Hamiltonian Monte Carlo methods. We explore the tradeoffs between various simulation methods through numerical benchmarks.

Robust charge-density-wave correlations in the electron-doped single-band Hubbard model.

There is growing evidence that the hole-doped single-band Hubbard and t - J models do not have a superconducting ground state reflective of the high-temperature cuprate superconductors but instead have striped spin- and charge-ordered ground states. Nevertheless, it is proposed that these models may still provide an effective low-energy model for electron-doped materials. Here we study the finite temperature spin and charge correlations in the electron-doped Hubbard model using quantum Monte Carlo dynamical cluster approximation calculations and contrast their behavior with those found on the hole-doped side of the phase diagram. We find evidence for a charge modulation with both checkerboard and unidirectional components decoupled from any spin-density modulations. These correlations are inconsistent with a weak-coupling description based on Fermi surface nesting, and their doping dependence agrees qualitatively with resonant inelastic x-ray scattering measurements. Our results provide evidence that the single-band Hubbard model describes the electron-doped cuprates.

Dynamical tuning of the chemical potential to achieve a target particle number in grand canonical Monte Carlo simulations.

We present a method to facilitate Monte Carlo simulations in the grand canonical ensemble given a target mean particle number. The method imposes a fictitious dynamics on the chemical potential, to be run concurrently with the Monte Carlo sampling of the physical system. Corrections to the chemical potential are made according to time-averaged estimates of the mean and variance of the particle number, with the latter being proportional to thermodynamic compressibility. We perform a variety of tests, and in all cases find rapid convergence of the chemical potential-inexactness of the tuning algorithm contributes only a minor part of the total measurement error for realistic simulations.

Inhaled methoxyflurane and intranasal fentanyl for prehospital management of visceral pain in an Australian ambulance service.

OBJECTIVE: This study analysed the analgesic effect and changes in vital signs associated with administration of inhaled Methoxyflurane (MTX) and/or intranasal Fentanyl (INF) for prehospital management of visceral pain. METHOD: A retrospective, observational study reviewing 1024 randomly selected records of patients with presumed visceral pain administered MTX (465), INF (397) or both (162) by the Western Australian Ambulance Service between January 2004 and February 2006. Clinical variables assessed included systolic blood pressure, pulse rate, respiration rate and Glasgow Coma Scale score. Pain was assessed utilising Visual/Verbal Analogue Scale pain scores. RESULTS: Overall effects on vital signs appeared favourable 5 min after use and at hospital arrival with either agent alone or in combination. As sole agents, MTX produced the greatest initial pain scores reduction (2.0 (1.7 to 2.2) vs 1.6 (1.4 to 1.8)) (mean (95% CI), and INF provided greater pain reduction by hospital arrival (3.2 (2.9 to 3.5) vs 2.5 (2.1 to 2.9)). While both agents were effective, INF provided a greater pain score reduction for cardiac (3.0 (2.6 to 3.4) vs 2.3 (1.8 to 2.8)), female (3.4 (2.9 to 4.0) v 2.5 (2.0 to 3.0)) and age 75+ patients (3.2 (2.5 to 3.8) vs 1.8 (1.0 to 2.5)). Combined use of agents was not advantageous. CONCLUSIONS: MTX and INF are effective agents for providing visceral pain analgesia in the prehospital setting. While MTX provided a more rapid onset of pain relief, INF provided superior analgesia after subsequent doses and in female, cardiac and older patients.