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Slowly quenched, high pressure glassy B2O3 at DFT accuracy
Modeling inorganic glasses requires an accurate representation of interatomic interactions, large system sizes to allow for intermediate-range structural order, and slow quenching rates to eliminate kinetically trapped structural motifs. Neither first principles-based nor force field-based molecular dynamics (MD) simulations satisfy these three criteria unequivocally. Herein, we report the development of a machine learning potential (MLP) for a classic glass, B2O3, which meets these goals well. The MLP is trained on condensed phase configurations whose energies and forces on the atoms are obtained using periodic quantum density functional theory. Deep potential MD simulations based on this MLP accurately predict the equation of state and the densification of the glass with slower quenching from the melt. At ambient conditions, quenching rates larger than 1011 K/s are shown to lead to artifacts in the structure. Pressure-dependent x-ray and neutron structure factors from the simulations compare excellently with experimental data. High-pressure simulations of the glass show varied coordination geometries of boron and oxygen, which concur with experimental observations.
Argonaute2 modulates megakaryocyte development and sex-specific control of platelet protein expression and reactivity
Analysis of intramolecular modes of liquid water in two-dimensional spectroscopy: A classical hierarchical equations of motion approach
Two-dimensional (2D) vibrational spectroscopy is a powerful means of investigating the structure and dynamics of complex molecules in condensed phases. However, even in theory, analysis of 2D spectra resulting from complex inter- and intra-molecular motions using only molecular dynamics methods is not easy. This is because molecular motions comprise complex multiple modes and peaks broaden and overlap owing to various relaxation processes and inhomogeneous broadening. On the basis of an anharmonic multimode Brownian oscillator model with nonlinear system–bath coupling, we have developed an approach that simulates 2D spectra, taking into account arbitrary modes of intermolecular and intramolecular vibrations simultaneously. Although only two-mode quantum calculations are feasible with this model, owing to high computational costs, here we restrict ourselves to the classical case and perform three-mode calculations. We demonstrate the applicability of our method by calculating 2D correlation infrared spectra of water for symmetric stretching, antisymmetric stretching, and bending modes. The quantum effects of these results are deduced by comparing 2D quantum spectra previously obtained for two intramolecular modes with those obtained using our classical approach under the same physical conditions. The results show that the 2D spectra calculated by separating the stretching modes into symmetric and asymmetric modes provide better descriptions of peak profiles, such as the splitting of cross-peaks.
Evaluation of ampicillin plus ceftobiprole combination therapy in treating Enterococcus faecalis infective endocarditis and bloodstream infection
Multiple and transforming vibrational identities of atoms in amorphous solids
Identifying the diverse roles of disorderly packed atoms inside an amorphous solid has been a highly pursued but daunting task in glass physics. By analyzing the full-frequency vibrational modes of a model Cu50Zr50 glass, here, we classify the internal atoms into low-, subhigh-, and high-frequency ones that have different tendencies for rearrangements upon excitations. We find that low-frequency atoms are structurally unfavored and tend to aggregate. High-frequency atoms originating from compressed atomic pairs are also mechanically unstable. As yield approaches, shear-transformation rearrangements shift from low-frequency to high-frequency atoms. Subhigh-frequency atoms play the role of stable backbones. Given that atoms can have different identities, multiple identities are observed to overlap in space. Atoms with one vibrational identity often transform to another one, showing different preferences in transformation routes. Our results deepen the understanding of atomic structures for amorphous plasticity beyond the simplified picture of soft vs hard spots.
Triaxial behavior and microstructural insights of loose sandy soil stabilized with alkali activated slag
How to correct Ehrenfest nonadiabatic dynamics in open quantum systems: Ehrenfest plus random force (E + <i>σ</i>) dynamics
One key challenge in the study of nonadiabatic dynamics in open quantum systems is to balance computational efficiency and accuracy. Although Ehrenfest dynamics (ED) is computationally efficient and well-suited for large complex systems, ED often yields inaccurate results. To address these limitations, we improve the accuracy of the traditional ED by adding a random force (E + σ). In this work, the construction of random forces is considered in Markovian and non-Markovian scenarios, and we ensure the dynamics satisfy the detailed balance in both scenarios. By comparing our E + σ with existing methods such as the electronic friction model and surface hopping, we furthermore validate its reliability. In addition, the E + σ model still retains the high efficiency of ED and does not incur much additional computation. We believe that this method provides an alternative to accurately describe the mixed quantum–classical dynamics in open quantum systems, particularly for large complex systems.
Short-term airborne ultrasound induced cell death in tobacco cells and changed their wall components
Structural evolution of particle configurations: Zero-temperature phases under increasing confinement
In this study, we investigate the phase behavior and structural organization of colloidal particles in a two-dimensional (2D) system under isotropic harmonic confinement using overdamped Langevin dynamics simulations. We employ a modified mermaid potential, which introduces an additional short-distance term resulting in a null-force region, distinct from the conventional mermaid potential. This modification facilitates a richer exploration of self-assembled structures, revealing a variety of phases influenced by the interplay between confinement strength V0 and the interaction potential. Our analysis spans a wide range of parameters, resulting in a detailed phase diagram that captures transitions from dispersed clusters to well-ordered patterns, including square, triangular, rhomboidal, and mixed configurations, as the confinement strength increases. The findings underscore the intricate balance of forces governing the self-assembly of colloidal systems and offer valuable insights for future experimental realizations.
Insulator–metal transition in VO2 film on sapphire studied by broadband dielectric spectroscopy
Mixed atomistic–implicit quantum/classical approach to molecular nanoplasmonics
A multiscale quantum mechanical (QM)/classical approach is presented that is able to model the optical properties of complex nanostructures composed of a molecular system adsorbed on metal nanoparticles. The latter is described by a combined atomistic–continuum model, where the core is described using the implicit boundary element method (BEM) and the surface retains a fully atomistic picture and is treated employing the frequency-dependent fluctuating charge and fluctuating dipole (ωFQFμ) approach. The integrated QM/ωFQFμ-BEM model is numerically compared with state-of-the-art fully atomistic approaches, and the quality of the continuum/core partition is evaluated. The method is then extended to compute surface-enhanced Raman scattering within a time-dependent density functional theory framework.
Biomechanical analysis of a newly designed and 3D printed plate-locking interbody cage: an observational study of finite element analysis
Low-energy electron driven reactions in 2-bromo-5-nitrothiazole
Thiazole derivatives are biologically relevant molecules, used also in pharmaceutical applications. Herein, we report results for electron attachment to 2-bromo-5-nitrothiazole (BNT) in the gas phase. Employing two crossed electron–molecule beam experiments, we determined the efficiency curves of various fragment anions as a function of the initial electron energy between about 0 and 10 eV as well as the emission angle and kinetic energy distributions of Br− and NO2− ions formed from a resonance near 4 eV. The experiments were supported by quantum chemical calculations, exploring possible dissociation pathways along with their reaction energies. We also compared the electron attachment characteristics of BNT with those of the native thiazole molecule by performing electron attachment experiments and calculations for this molecule as well. Compared to thiazole, which is primarily degraded only by electrons with kinetic energies between about 5 and 10 eV, BNT is susceptible to low-energy electrons near 0 eV with enhanced cross section for (dissociative) electron attachment. However, although BNT offers two localization sites with high electron affinity (Br and NO2 moieties), we do not find the corresponding anions as the dominant negatively charged species formed upon electron attachment. Instead, the reaction channels with an abstraction of Br and NO2 as neutral radicals prevail, accompanied by the opening of the thiazole ring due to the relatively weak C–S bond.
Association between ethylene oxide exposure and cognitive function in older adults from NHANES data
Exploring low barrier quantum tunneling and structural planarity in 3-methylstyrene conformers: Insights from microwave spectroscopy
The first ground-state rotational spectrum of 3-methylstyrene (3MS) was measured by Fourier transform microwave spectroscopy under supersonic jet-cooled conditions. Transitions were assigned for two conformers: cis-3MS and trans-3MS. In the cis conformer, the vinyl group is oriented toward the methyl group, while in the trans conformer, it is positioned away from the methyl. The energy difference between the two conformers was calculated to be only 2.1 cm−1, with the cis conformer having lower energy. Significant tunneling splitting, caused by the low-barrier internal rotation of the methyl group, was observed and analyzed using the XIAM and BELGI-Cs codes. The BELGI results show that the V3 barrier is 30.6688(87) cm−1 for the cis conformer and 11.0388(88) cm−1 for the trans conformer. The experimental rotational and torsional parameters are compared to their density functional theory counterparts. The planarity of the molecular geometry of cis- and trans-3MS is discussed, contributing to the long-standing topic of discussion about the planarity of styrene derivatives.
Prediction model and real-time diagnostics of hydraulic fracturing pressure for highly deviated wells in deep oil and gas reservoirs
Hydroxysilylene (HSi–OH) in the gas phase
The hydroxysilylene (HSiOH) molecule has been spectroscopically identified in the gas phase for the first time. This highly reactive species was produced in a twin electric discharge jet using separate precursor streams of 16O2/18O2 and Si2H6/Si2D6, both diluted in high pressure argon. The strongest and most stable laser induced fluorescence (LIF) signals were obtained by applying an electric discharge to each of the precursor streams and then merging the discharge products just prior to expansion into vacuum. Bands of the Ã1A–X~1A′ electronic transition of HSiOH were found in the 455–420 nm region, and single vibronic level emission spectra showed only transitions attributable to the trans-hydroxysilylene ground state isomer. High resolution, rotationally resolved spectra were obtained for the 0-0 bands of HSi16OH and HSi18OH. The rotational constants were used to obtain ground and excited state molecular structures of HSiOH, with some necessary constraints. The derived ground state structure is trans-HSiOH, with geometric parameters similar to theoretical predictions from the literature. In the excited state, a skew-HSiOH structure was obtained with a dihedral angle of 102°. Our own CASSCF/aug-cc-pVTZ calculations predict a similar excited state skew geometry. The lack of odd quantum number changes in the torsional mode in emission and our difficulties in obtaining DSiOD spectra, despite considerable effort, all suggest that further experimental and theoretical efforts will be necessary to thoroughly understand the electronic spectrum of hydroxysilylene.
Circularly polarized dual-band resonance in a miniaturized implantable antenna using combined hexagonal and rhombic patches
Abstract The design and characterisation of a novel dual-band implantable antenna with compact size is presented in this research. The antenna, which is $$5 \times 5 \times 0.635 {\text{mm}}^{3}$$ in size and operates at two critical frequencies—0.954 GHz in the UHF band and 2.4 GHz in the ISM band—was fabricated on an RT6010 substrate. The U-shaped slot and shorting pin on the radiating element have been exploited to achieved dual-band and circular polarization. The antenna is noteworthy for achieving circular polarization with a broad axial ratio bandwidth of 24.6%, which enables strong performance throughout its operating frequencies. The proposed antennas SAR values satisfy IEEE safety standards for implantable medical devices with a gain of − 28.1 dB at 2.4 GHz and − 31.2 dB at 0.954 GHz, despite its small size. The design represents a significant advancement in the field of medical implant technology since it prioritizes effective wireless communication capabilities while upholding strict safety regulations.
Alchemical harmonic approximation based potential for iso-electronic diatomics: Foundational baseline for Δ-machine learning
We introduce the alchemical harmonic approximation (AHA) of the absolute electronic energy for charge-neutral iso-electronic diatomics at fixed interatomic distance d0. To account for variations in distance, we combine AHA with this ansatz for the electronic binding potential, E(d)=(Eu−Es)Ec−EsEu−Esd/d0+Es, where Eu, Ec, Es correspond to the energies of the united atom, calibration at d0, and the sum of infinitely separated atoms, respectively. Our model covers the two-dimensional electronic potential energy surface spanned by distances of 0.7–2.5 Å and differences in nuclear charge from which only one single point (with elements of nuclear charge Z1, Z2, and distance d0) is drawn to calibrate Ec. Using reference data from pbe0/cc-pVDZ, we present numerical evidence for the electronic ground-state of all neutral diatomics with 8, 10, 12, and 14 electrons. We assess the validity of our model by comparison to legacy interatomic potentials (harmonic oscillator, Lennard-Jones, and Morse) within the most relevant range of binding (0.7–2.5 Å) and find comparable accuracy if restricted to single diatomics and significantly better predictive power when extrapolating to the entire iso-electronic series. We also investigated Δ-learning of the electronic absolute energy using our model as a baseline. This baseline model results in a systematic improvement, effectively reducing training data needed for reaching chemical accuracy by up to an order of magnitude from ∼1000 to ∼100. By contrast, using AHA+Morse as a baseline hardly leads to any improvement and sometimes even deteriorates the predictive power. Inferring the energy of unseen CO converges to a prediction error of ∼0.1 Ha in direct learning and ∼0.04 Ha with our baseline.