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1. Bayesian learning of chemisorption for bridging the complexity of electronic descriptors

   https://doi.org/10.1038/s41467-020-19524-z  

   Wang, Siwen ; Pillai, Hemanth Somarajan ; Xin, Hongliang ( November 2020 , Nature Communications)

   Building upon thed-band reactivity theory in surface chemistry and catalysis, we develop a Bayesian learning approach to probing chemisorption processes at atomically tailored metal sites. With representative species, e.g., *O and *OH, Bayesian models trained with ab initio adsorption properties of transition metals predict site reactivity at a diverse range of intermetallics and near-surface alloys while naturally providing uncertainty quantification from posterior sampling. More importantly, this conceptual framework sheds light on the orbitalwise nature of chemical bonding at adsorption sites withd-states characteristics ranging from bulk-like semi-elliptic bands to free-atom-like discrete energy levels, bridging the complexity of electronic descriptors for the prediction of novel catalytic materials.

    

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2. Charge state-dependent symmetry breaking of atomic defects in transition metal dichalcogenides

   https://doi.org/10.1038/s41467-024-47039-4  

   Xiang, Feifei ; Huberich, Lysander ; Vargas, Preston A. ; Torsi, Riccardo ; Allerbeck, Jonas ; Tan, Anne Marie Z. ; Dong, Chengye ; Ruffieux, Pascal ; Fasel, Roman ; Gröning, Oliver ; et al ( March 2024 , Nature Communications)

   The functionality of atomic quantum emitters is intrinsically linked to their host lattice coordination. Structural distortions that spontaneously break the lattice symmetry strongly impact their optical emission properties and spin-photon interface. Here we report on the direct imaging of charge state-dependent symmetry breaking of two prototypical atomic quantum emitters in mono- and bilayer MoS₂by scanning tunneling microscopy (STM) and non-contact atomic force microscopy (nc-AFM). By changing the built-in substrate chemical potential, different charge states of sulfur vacancies (Vac_S) and substitutional rhenium dopants (Re_Mo) can be stabilized. Vac$${}_{{{{{{{{\rm{S}}}}}}}}}^{-1}$$${}_S^{-1}$as well as Re$${}_{{{{{{{{\rm{Mo}}}}}}}}}^{0}$$${}_{\mathrm{Mo}}^0$and Re$${}_{{{{{{{{\rm{Mo}}}}}}}}}^{-1}$$${}_{\mathrm{Mo}}^{-1}$exhibit local lattice distortions and symmetry-broken defect orbitals attributed to a Jahn-Teller effect (JTE) and pseudo-JTE, respectively. By mapping the electronic and geometric structure of single point defects, we disentangle the effects of spatial averaging, charge multistability, configurational dynamics, and external perturbations that often mask the presence of local symmetry breaking.

    

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3. Accurate simulation of surfaces and interfaces of ten FCC metals and steel using Lennard–Jones potentials

   https://doi.org/10.1038/s41524-020-00478-1  

   Kanhaiya, Krishan ; Kim, Seonghan ; Im, Wonpil ; Heinz, Hendrik ( January 2021 , npj Computational Materials)

   The earlier integration of validated Lennard–Jones (LJ) potentials for 8 fcc metals into materials and biomolecular force fields has advanced multiple research fields, for example, metal–electrolyte interfaces, recognition of biomolecules, colloidal assembly of metal nanostructures, alloys, and catalysis. Here we introduce 12-6 and 9-6 LJ parameters for classical all-atom simulations of 10 further fcc metals (Ac, Ca (α), Ce (γ), Es (β), Fe (γ), Ir, Rh, Sr (α), Th (α), Yb (β)) and stainless steel. The parameters reproduce lattice constants, surface energies, water interfacial energies, and interactions with (bio)organic molecules in 0.1 to 5% agreement with experiment, as well as qualitative mechanical properties under standard conditions. Deviations are reduced up to a factor of one hundred in comparison to earlier Lennard–Jones parameters, embedded atom models, and density functional theory. We also explain a quantitative correlation between atomization energies from experiments and surface energies that supports parameter development. The models are computationally very efficient and applicable to an exponential space of alloys. Compatibility with a wide range of force fields such as the Interface force field (IFF), AMBER, CHARMM, COMPASS, CVFF, DREIDING, OPLS-AA, and PCFF enables reliable simulations of nanostructures up to millions of atoms and microsecond time scales. User-friendly model building and input generation are available in the CHARMM-GUI Nanomaterial Modeler. As a limitation, deviations in mechanical properties vary and are comparable to DFT methods. We discuss the incorporation of reactivity and features of the electronic structure to expand the range of applications and further increase the accuracy.

    

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4. Ab initio electron-defect interactions using Wannier functions

   https://doi.org/10.1038/s41524-020-0284-y  

   Lu, I-Te ; Park, Jinsoo ; Zhou, Jin-Jian ; Bernardi, Marco ( March 2020 , npj Computational Materials)

   Computing electron–defect (e–d) interactions from first principles has remained impractical due to computational cost. Here we develop an interpolation scheme based on maximally localized Wannier functions (WFs) to efficiently computee–d interaction matrix elements. The interpolated matrix elements can accurately reproduce those computed directly without interpolation and the approach can significantly speed up calculations ofe–d relaxation times and defect-limited charge transport. We show example calculations of neutral vacancy defects in silicon and copper, for which we compute thee–d relaxation times on fine uniform and random Brillouin zone grids (and for copper, directly on the Fermi surface), as well as the defect-limited resistivity at low temperature. Our interpolation approach opens doors for atomistic calculations of charge carrier dynamics in the presence of defects.

    

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5. Substitutional transition metal doping in MoS 2 : a first-principles study

   https://doi.org/10.1088/2632-959X/ab7cb3  

   Yoshimura, Anthony ; Koratkar, Nikhil ; Meunier, Vincent ( March 2020 , Nano Express)

   Single-layer MoS₂is a direct-gap semiconductor whose band edges character is dominated by the d-orbitals of the Mo atoms. It follows that substitutional doping of the Mo atoms has a significant impact on the material’s electronic properties, namely the size of the band gap and the position of the Fermi level. Here, density functional theory is used along with the G₀W₀method to examine the effects of substituting Mo with four different transition metal dopants: Nb, Tc, Ta, and Re. Nb and Ta possess one less valence electron than Mo does and are therefore p-type dopants, while Re and Tc are n-type dopants, having one more valence electron than Mo has. Four types of substitutional structures are considered for each dopant species: isolated atoms, lines, three-atom clusters centered on a S atom (c3s), and three-atom clusters centered on a hole (c3h). The c3h structure is found to be the most stable configuration for all dopant species. However, electronic structure calculations reveal that isolated dopants are preferable for efficient n- or p-type performance. Lastly, it is shown that photoluminescence measurements can provide valuable insight into the atomic structure of the doped material. Understanding these properties of substitutionally-doped MoS₂can allow for its successful implementation into cutting-edge solid state devices.

    

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