Tweezer-like magnetic tip control of the local spin state in the FeOEP/Pb(111) adsorption system: a preliminary exploration based on first-principles calculations.

The magnetic interactions between the spin-polarized scanning tunnelling microscopy (SP-STM) tip and the localized spin impurities lead to various forms of the Kondo effect. Although these intriguing phenomena enrich Kondo physics, detailed theoretical simulations and explanations are still lacking due to the rather complex formation mechanisms. Here, by combining density functional theory (DFT), complete active space self-consistent field (CASSCF) theory, and hierarchical equations of motion (HEOM) methods, we perform first-principles-based simulation to elaborate the regulation process of the magnetic Co-tip on the spin state and transport behaviour of FeOEP/Pb(111) system. Compared with the non-magnetic tip, the stronger interaction between the magnetic tip and FeOEP molecule results in a more drastic deformation of the molecular structure with more electron transfer from the local environment to Fe-3d orbitals. The magnetic anisotropy of FeOEP changes very drastically from positive values in the tunnelling region to negative values in the contact region. The ferromagnetic electron correlation between the magnetic tip and the molecule induces an asymmetric Kondo line-shape near the Fermi level. This work highlights that the DFT + CASSCF + HEOM approach can not only predict complex quantum phenomena and explain underlying physical mechanisms, but also facilitate the design of more fascinating quantum control experiments.

Unveiling the Decisive Factor for the Sharp Transition in the Scanning Tunneling Spectroscopy of a Single Nickelocene Molecule.

Scanning tunneling microscopy (STM) has been utilized to realize the precise measurement and control of local spin states. Experiments have demonstrated that when a nickelocene (Nc) molecule is attached to the apex of an STM tip, the dI/dV spectra exhibit a sharp or a smooth transition when the tip is displaced toward the substrate. However, what leads to the two distinct types of transitions remains unclear, and more intriguingly, the physical origin of the abrupt change in the line shape of dI/dV spectra remains unclear. To clarify these intriguing issues, we perform first-principles-based simulations on the STM tip control process for the Cu tip/Nc/Cu(100) junction. In particular, we find that the suddenly enhanced hybridization between the d orbitals on the Ni ion and the metallic bands in the substrate leads to Kondo correlation overwhelming spin excitation, which is the main cause of the sharp transition in the dI/dV spectra observed experimentally.

Reduction-Controlled Atomic Migration for Single Atom Alloy Library.

Picturing the atomic migration pathways of catalysts in a reactive atmosphere is of central significance for uncovering the underlying catalytic mechanisms and directing the design of high-performance catalysts. Here, we describe a reduction-controlled atomic migration pathway that converts nanoparticles to single atom alloys (SAAs), which has remained synthetically challenging in prior attempts due to the elusive mechanism. We achieved this by thermally treating the noble-metal nanoparticles M (M = Ru, Rh, Pd, Ag, Ir, Pt, and Au) on metal oxide (CuO) supports with H2/Ar. Atomic-level characterization revealed such conversion as the synergistic consequence of noble metal-promoted H2 dissociation and concomitant CuO reduction. The observed atomic migration pathway offers an understanding of the dynamic mechanisms study of nanomaterials formation and catalyst design.

Origin of Asymmetric Splitting of Kondo Peak in Spin-Polarized Scanning Tunneling Spectroscopy: Insights from First-Principles-Based Simulations.

The spin-polarized scanning tunneling microscope (SP-STM) has served as a versatile tool for probing and manipulating the spintronic properties of atomic and molecular devices with high precision. The interplay between the local spin state and its surrounding magnetic environment significantly affects the transport behavior of the device. Particularly, in the contact regime, the strong hybridization between the SP-STM tip and the magnetic atom or molecule could give rise to unconventional Kondo resonance signatures in the differential conductance (dI/dV) spectra. This poses challenges for the simulation of a realistic tip control process. By combining the density functional theory and the hierarchical equations of motion methods, we achieve first-principles-based simulation of the control of a Ni-tip/Co/Cu(100) junction in both the tunneling and contact regimes. The calculated dI/dV spectra reproduce faithfully the experimental data. A cotunneling mechanism is proposed to elucidate the physical origin of the observed unconventional Kondo signatures.

Effective utilization of dichloromethane by a newly isolated strain Methylobacterium rhodesianum H13.

An effective dichloromethane (DCM) utilizer Methylobacterium rhodesianum H13 was isolated from activated sludge. A response surface methodology was conducted, and the optimal conditions were found to be 4.5 g/L Na2HPO4·12H2O, 0.5 g/L (NH4)2SO4, an initial pH of 7.55, and a temperature of 33.7 °C. The specific growth rate of 0.25 h(-1) on 10 mM DCM was achieved, demonstrating that M. rhodesianum H13 was superior to the other microorganisms in previous investigations of DCM utilization. DCM mineralization paralleled the production of cells, CO2, and water-soluble metabolites, as well as the release of Cl(-), whereas the carbon distribution and Cl(-) yield varied with DCM concentrations. The facts that complete degradation only occurred with DCM concentrations below 15 mM and repetitive degradation of 5 mM DCM could proceed for only three cycles were ascribed to pH decrease (from 7.55 to 3.02) though a buffer system was employed.

[Isolation and degradation characteristics of dichloromethane-degradation bacterial strain by Methylobacterium rhodesianum H13].

A dichloromethane-degrading bacterium Methylobacterium rhodesianum H13 which utilized the DCM as the sole carbon and energy source was isolated. According to the research, M. rhodesianum H13 could completely degrade 5 mmol x L(-1) DCM in 23 h with the initial cell concentration of 0.82 mg x L(-1), pH 7.0, 30 degrees C, and the cell yield rate was about 0.136 g x g(-1) DCM. With the degradation of DCM, Cl- concentration gradually raised (the release of Cl- concentration was about 2 times higher as the DCM), pH value dropped to 6.75, and the solution was weakly acidic. Temperature, pH, DCM concentration, Cl- concentration and other factors were investigated through the shake flask experiments, and the optimal conditions for DCM degradation were: temperature 30 degrees C, pH 7.0. The study also indicated that 5 mmol x L(-1) of DCM was the optimum concentration for M. rhodesianum H13 and high levels of DCM could inhibit the degradation. The research has an important application value for the DCM environmental pollution.