Reaction mechanism between small-sized Ce clusters and water molecules: An ab initio investigation on Ce\u3csub\u3e\u3ci\u3en\u3c/i\u3e\u3c/sub\u3e+H\u3csub\u3e2\u3c/sub\u3eO

Reactions of small-sized cerium clusters Cen (n = 1–3) with a single water molecule are systematically investigated theoretically. The ground state structures of the Cen/H2O complex and the reaction pathways between Cen + H2O are predicted. Our results show the size-dependent reactivity of small-sized Ce clusters. The calculated reaction energies and reaction barriers indicate that the reactivity between Cen and water becomes higher with increasing cluster size. The predicted reaction pathways show that the single Ce atom and the Ce2 and Ce3 clusters can all easily react with H2O and dissociate the water molecule. Under UV-irradiation, the reaction of a Ce atom with a single H2O molecule may even release an H2 molecule. The reaction of either Ce2 or Ce3 with a single H2O molecule can fully dissociate the H2O into H and O atoms while it is bonded with the Ce cluster. The electronic configuration and oxidation states of the Ce atoms in the products and the higher occupied molecular orbitals are analyzed by using the natural bond orbital (NBO) analysis method, from which the high reactivity between the reaction products of Cen + H2O and an additional H2O molecule is predicted. Our results offer deeper molecular insights into the chemical reactivity of Ce, which could be helpful for developing more efficient Ce-doped or Ce-based catalysts. Includes supplementary materials

Topological Atomic Spinwave Lattices by Dissipative Couplings

Recent experimental advance in creating dissipative couplings provides a new route for engineering exotic lattice systems and exploring topological dissipation. Using the spatial lattice of atomic spinwaves in a vacuum vapor cell, where purely dissipative couplings arise from diffusion of atoms, we experimentally realize a dissipative version of the Su-Schrieffer-Heeger (SSH) model. We construct the dissipation spectra of the topological or trivial lattices via electromagnetically-induced-transparency (EIT) spectroscopy. The topological dissipation spectrum is found to exhibit edge modes at dissipation rates within a dissipative gap, decoupled from the bulk. We also validate chiral symmetry of the dissipative SSH couplings. This work paves the way for realizing topology-enabled quantum correlations and non-Hermitian topological quantum optics via dissipative couplings.Comment: 5 pages, 4 figure

Mechanistic study of pressure and temperature dependent structural changes in reactive formation of silicon carbonate

The discovery of the silicon carbonate through chemical reaction between porous SiO2 and gaseous CO2 addressed a long-standing question regarding whether the reaction between CO2 and SiO2 is possible. However, the detailed atomic structure of silicon carbonate and associated reaction mechanism are still largely unknown. We explore structure changes of silicon carbonate with pressure and temperature based on systematic ab initio molecular dynamics simulations. Our simulations suggest that the reaction proceeds at the surface of the porous SiO2. Increasing number of CO2 molecules can take part in the reaction by increasing either the pressure or temperature. The final product of the reaction exhibits amorphous structures, where most C atoms and Si atoms are 3-fold and 6-fold coordinated, respectively. The fraction of differently coordinated C (Si) atoms is pressure dependent, and as a result, the structure of the final product is pressure dependent as well. When releasing the pressure, part of the reaction product decomposes into CO2 molecules and SiO2 tetrahedrons. However more than 50% of C atoms are still in 3-fold coordination, implying that stable silicon carbonate may be obtained via repeated annealing under high pressure. The mechanism underlying this chemical reaction is predicted with two possible reaction pathways identified. Moreover, the reaction transition curve is obtained from the extensive simulation, which can be useful to guide the synthesis of silicon carbonate from the reaction between SiO2 and CO2

Explicit Dynamic DDA Method considering Dynamic Contact Force

This paper proposes an explicit dynamic DDA method considering dynamic contact force, which aims at solving the problems of low efficiency of dynamic contact detection and the simulation of dynamic contact force in the conventional DDA method. The mutual contact between blocks can be regarded as the application of point loading on a single block, and the corresponding contact submatrix can be calculated and the simultaneous equations of the block system can be integrated. The central difference method is adopted to deduce the explicit expression of block displacement containing dynamic contact force. With the relationship between displacement and dynamic contact force, contact constraint equations of a block system are obtained to calculate the dynamic contact force and the corresponding block displacement. The accuracy of the explicit dynamic DDA method is verified using two numerical cases. The calculation results show that the new DDA method can be applied in large-scale geotechnical engineering

Seasonal and spatial variations of heavy metalsin surface sediments collected from the BaoxiangRiver in the Dianchi Watershed, China

To explore potential ecological hazards due to heavy metals in the Dianchi Lake Watershed, a three-stage European Community Bureau of Reference (BCR) sequential extraction procedure was applied to examine the spatial distributions and relative speciation ratios of Zn, Cu, Ni, Pb, and Cr in Baoxiang River sediments during wet and dry seasons. The metal species have similar spatial variations during different seasons. In the upstream reaches of the Baoxiang River, heavy metals reside primarily in the non-extractable residual fraction (72&ndash;90%). In the midstream, the residual fraction (35&ndash;89%) remains dominant, but the extractable fraction increases, featuring especially notable increases in the reducible fraction (5&ndash;40%). Downstream, the Cu, Ni, Pb, and Cr residual fractions remain high (46&ndash;80%) and the extractable fractions increase rapidly; the Zn extractable fraction is quite high (65.5%). Anthropogenic sources drive changes in heavy metal speciation. Changes in the river environment, such as pH and oxidation-reduction potential, also affect speciation. The reducible fraction of heavy metals in Baoxiang River sediments is most sensitive to pH. Potential ecological risk assessments for these five elements indicate that risks from Zn and Pb are mild to moderate in the middle and lower reaches of the river.<br style="line-height: normal; text-align: -webkit-auto; text-size-adjust: auto;" /

AdaptivePose++: A Powerful Single-Stage Network for Multi-Person Pose Regression

Multi-person pose estimation generally follows top-down and bottom-up paradigms. Both of them use an extra stage ($\boldsymbol{e.g.,}$ human detection in top-down paradigm or grouping process in bottom-up paradigm) to build the relationship between the human instance and corresponding keypoints, thus leading to the high computation cost and redundant two-stage pipeline. To address the above issue, we propose to represent the human parts as adaptive points and introduce a fine-grained body representation method. The novel body representation is able to sufficiently encode the diverse pose information and effectively model the relationship between the human instance and corresponding keypoints in a single-forward pass. With the proposed body representation, we further deliver a compact single-stage multi-person pose regression network, termed as AdaptivePose. During inference, our proposed network only needs a single-step decode operation to form the multi-person pose without complex post-processes and refinements. We employ AdaptivePose for both 2D/3D multi-person pose estimation tasks to verify the effectiveness of AdaptivePose. Without any bells and whistles, we achieve the most competitive performance on MS COCO and CrowdPose in terms of accuracy and speed. Furthermore, the outstanding performance on MuCo-3DHP and MuPoTS-3D further demonstrates the effectiveness and generalizability on 3D scenes. Code is available at https://github.com/buptxyb666/AdaptivePose.Comment: Submit to IEEE TCSVT; 11 pages. arXiv admin note: text overlap with arXiv:2112.1363

Better synchronous binarization for machine translation

Binarization of Synchronous Context Free Grammars (SCFG) is essential for achieving polynomial time complexity of decoding for SCFG parsing based machine translation sys-tems. In this paper, we first investigate the excess edge competition issue caused by a left-heavy binary SCFG derived with the method of Zhang et al. (2006). Then we propose a new binarization method to mitigate the problem by exploring other alternative equivalent bi-nary SCFGs. We present an algorithm that ite-ratively improves the resulting binary SCFG, and empirically show that our method can im-prove a string-to-tree statistical machine trans-lations system based on the synchronous bina-rization method in Zhang et al. (2006) on the NIST machine translation evaluation tasks.

Two-dimensional monolayer salt nanostructures can spontaneously aggregate rather than dissolve in dilute aqueous solutions

It is well known that NaCl salt crystals can easily dissolve in dilute aqueous solutions at room temperature. Herein, we reported the first computational evidence of a novel salt nucleation behavior at room temperature, i.e., the spontaneous formation of two-dimensional (2D) alkali chloride crystalline/non-crystalline nanostructures in dilute aqueous solution under nanoscale confinement. Microsecond-scale classical molecular dynamics (MD) simulations showed that NaCl or LiCl, initially fully dissolved in confined water, can spontaneously nucleate into 2D monolayer nanostructures with either ordered or disordered morphologies. Notably, the NaCl nanostructures exhibited a 2D crystalline square-unit pattern, whereas the LiCl nanostructures adopted non-crystalline 2D hexagonal ring and/or zigzag chain patterns. These structural patterns appeared to be quite generic, regardless of the water and ion models used in the MD simulations. The generic patterns formed by 2D monolayer NaCl and LiCl nanostructures were also confirmed by ab initio MD simulations. The formation of 2D salt structures in dilute aqueous solution at room temperature is counterintuitive. Free energy calculations indicated that the unexpected spontaneous salt nucleation behavior can be attributed to the nanoscale confinement and strongly compressed hydration shells of ions. Supplementary files, including 6 movies, attached below