Probing magnetic fields on crystals of the nanomagnet Mn12-acetate by electron paramagnetic resonance

We report on electron paramagnetic resonance (EPR) probing of magnetic fields and magnetic field gradients near the surface of a single crystal of the nanomagnet [Mn12O12(CH3COO)16(H2O)4].2CH3COOH.4H2O (Mn12-Ac). As the EPR probe, we utilized a 0.7 mm x 30 microm x 30 microm fibrous needle of the organic conductor N-methylphenazinium-tetracyanoquinodimethane (NMP-TCNQ), which yields an exceptionally sharp peak, with a 0.2 G (approximately 20 microT) width. In the presence of Mn12-Ac, the probe's peak exhibits splitting on temperature lowering, which depends on the orientation of the Zeeman field relative to the axis of easy magnetization of the employed Mn12-Ac crystal. The shifted peaks yield the magnitude of the magnetic field from Mn12-Ac crystal to which the various fibers of the probe are subjected. In conjunction with electron microscopy, the shifts yield the field gradient at the crystal surface and its change with temperature. For Mn12-Ac at 10 K, the surface magnetic field was measured to be in the mT range and its gradient on the order of 50 T/m.     

Using Convolutional Neural Network and a Single Heartbeat for ECG Biometric Recognition

The electrocardiogram (ECG) signal has become a popular biometric modality due to characteristics that make it suitable for developing reliable authentication systems. However, the long segment of signal required for recognition is still one of the limitations of existing ECG biometric recognition methods and affects its acceptability as a biometric modality. This paper investigates how a short segment of an ECG signal can be effectively used for biometric recognition, using deep-learning techniques. A small convolutional neural network (CNN) is designed to achieve better generalization capability by entropy enhancement of a short segment of a heartbeat signal. Additionally, it investigates how various blind and feature-dependent segments with different lengths affect the performance of the recognition system. Experiments were carried out on two databases for performance evaluation that included single and multisession records. In addition, a comparison was made between the performance of the proposed classifier and four well-known CNN models: GoogLeNet, ResNet, MobileNet and EfficientNet. Using a time–frequency domain representation of a short segment of an ECG signal around the R-peak, the proposed model achieved an accuracy of 99.90% for PTB, 98.20% for the ECG-ID mixed-session, and 94.18% for ECG-ID multisession datasets. Using the preprinted ResNet, we obtained 97.28% accuracy for 0.5-second segments around the R-peaks for ECG-ID multisession datasets, outperforming existing methods. It was found that the time–frequency domain representation of a short segment of an ECG signal can be feasible for biometric recognition by achieving better accuracy and acceptability of this modality.     

Determination of Atovaquone in Human Plasma by LC-MS-MS and Its Application to a Bioequivalence Study

A sensitive and selective method for the determination of atovaquone in human plasma was developed and validated. The procedure employed the use of an internal standard (chlorothalidone) and a solvent extraction step. Detection was by electrospray ionization tandem mass spectrometry with multiple reaction monitoring. The method showed a linear range from 50 to 2,000 ng mL^?1. The extraction recovery was determined to be 84.91 ± 6.42% (SD), the intra- and inter-day assay accuracy (relative error) was within 7.57% and precision (RSD) was below 6.06%. The method was successfully employed to analyze plasma samples and evaluate the pharmacokinetics of atovaquone in human volunteers.     

Direct evidence from electron paramagnetic resonance for additional configurations in uncommon paddlewheel Re2(7+) units surrounded by an unsymmetrical bicyclic guanidinate

Three rare compounds have been synthesized and structurally characterized; these species have paddlewheel structures and Re(2)(7+) cores surrounded by four bicyclic guanidinates and two axial ligands along the Re-Re axis. Each possesses a formal bond order of 3.5 and a σ(2)π(4)δ(1) electronic configuration that entails the presence of one unpaired electron for each compound. The guanidinate ligands characterized by having CH(2) entities and a central C(N)(3) unit that joins two cyclic units--one having two fused 6-membered rings (hpp) and the other having a 5- and a 6-membered ring fused together (tbn)--allowed the isolation of [Re(2)(tbn)(4)Cl(2)]PF(6), 1, [Re(2)(tbn)(4)Cl(2)]Cl, 2, and [Re(2)(hpp)(4)(O(3)SCF(3))(2)](O(3)SCF(3)), 3. Because of the larger bite angle of the tbn relative to the hpp ligand, the Re-Re bond distances in 1 and 2 (2.2691(14) and 2.2589(14) ?, respectively) are much longer than that in 3 (2.1804(8) ?). Importantly, electron paramagnetic resonance (EPR) studies at both X-band (~9.4 GHz) and W-band (112 GHz) in the solid and in frozen solution show unusually low g-values (~1.75) and the absence of zero-field splitting, providing direct evidence for the presence of one metal-based unpaired electron for both 1 and 3. These spectroscopic data suggest that the unsymmetrical 5-/6-membered ligand leads to the formation of isomers, as shown by significantly broader EPR signals for 1 than for 3, even though both compounds possess what appears to be similar ideal crystallographic axial symmetry on the X-ray time scale.     

Directed Diffusion Approach for Preparing Atomistic Models of Crosslinked Epoxy for Use in Molecular Simulations

A directed diffusion approach is used to create atomistic models of crosslinked epoxy. In polymerization‐based approaches for preparing epoxy model structures, conversions higher than 95% are difficult to achieve due to very slow diffusion of unreacted monomers and crosslinkers in the partially formed network. This problem is overcome by creating very long bonds in the polymerization stage, and then relaxing these to equilibrium values by using a directed‐diffusion‐based relaxation strategy. The method minimizes the use of custom code by relying on the in‐built functionality in LAMMPS package (S. Plimpton, J. Comput. Phys. 1995 , 117, 1). The approach allows for near‐complete conversion (≈99%) and the thermal and volumetric properties of the structures so prepared show good agreement with experimental data.

     

Spin glass transitions in the absence of chemical disorder for the pyrochlores A2Sb2O7 (A=Mn, Co, Ni)

The pyrochlores in the series A₂Sb₂O₇ have been synthesized and characterized as exhibiting spin glass transitions at T_SG=41, 4.5, and 2.6 K (for A=Mn²⁺, Co²⁺ and Ni²⁺S=1, respectively) despite the lack of chemical disorder. Since the Curie-Weiss temperature remains essentially constant for all members in the series (), the frustration index for these materials increases significantly as the moment size is reduced from f=|θ|/T_SG=1.1 (Mn²⁺), to 9.3 (Co²⁺) to 14.6 (Ni²⁺). There is also a corresponding change in the spin dynamics measured by the shift in the AC susceptibility signal as a function of frequency. These new materials provide an avenue to investigate the effect of quantum fluctuations on the Heisenberg pyrochlore lattice in the low spin limit, and show there is a dramatic change in the spin dynamics as the quantum regime is approached.     

Geometric complexity theory III: on deciding nonvanishing of a Littlewood–Richardson coefficient

We point out that the positivity of a Littlewood?CRichardson coefficient $c^{\gamma}_{\alpha, \beta}$ for sl _n can be decided in strongly polynomial time. This means that the number of arithmetic operations is polynomial in n and independent of the bit lengths of the specifications of the partitions ??,??, and ??, and each operation involves numbers whose bitlength is polynomial in n and the bit lengths ??,??, and ??. Secondly, we observe that nonvanishing of a generalized Littlewood?CRichardson coefficient of any type can be decided in strongly polynomial time assuming an analogue of the saturation conjecture for these types, and that for weights ??,??,??, the positivity of $c^{ 2\gamma}_{2\alpha, 2\beta}$ can (unconditionally) be decided in strongly polynomial time.     

3 d metal ions in highly unusual eight-coordination: the phosphate-capped dodecapalladate(II) nanocube

Trapped in a noble cube: A novel family of noble metalates has been discovered in which a 3d metal ion M (M = Mn(II), Fe(III), Co(II), Cu(II), Zn(II)) is encapsulated by a 12 palladium-oxo cage {Pd(12)O(32)}, which is capped by eight phosphate groups. Such discrete nanocubes were further investigated by EPR spectroscopy, electrochemistry, and in homogeneous hydrogenation catalysis.     

Coherent manipulation of electron spins in the {Cu3} spin triangle complex impregnated in nanoporous silicon

We report on coherent manipulation of electron spins in an antiferromagnetically coupled spin triangle {Cu3-X} (X=As, Sb) impregnated in freestanding nanoporous silicon (NS) by using 240 GHz microwave pulses. Rabi oscillations are observed and the spin coherence time is found to be T(2)=1066 ns at 1.5 K. This demonstrates that the {Cu3-X}:NS hybrid material provides a promising scheme for implementing spin-based quantum gates. By measuring the spin relaxation times of samples with different symmetries and environments we give evidence that a spin chirality is the main decoherence source of spin triangle molecules.