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Motivated by the recent observation of superconductivity withT_c ~ 80 K in pressurized La₃Ni₂O₇¹, we explore the structural and electronic properties ofA₃Ni₂O₇bilayer nickelates (A = La-Lu, Y, Sc) as a function of pressure (0–150 GPa) from first principles including a Coulomb repulsion term. At ~ 20 GPa, we observe an orthorhombic-to-tetragonal transition in La₃Ni₂O₇at variance with x-ray diffraction data, which points to so-far unresolved complexities at the onset of superconductivity, e.g., charge doping by variations in the oxygen stoichiometry. We compile a structural phase diagram that establishes chemical and external pressure as distinct and counteracting control parameters. We find unexpected correlations betweenT_cand thein-planeNi-O-Ni bond angles for La₃Ni₂O₇. Moreover, two structural phases with significantc⁺octahedral rotations and in-plane bond disproportionations are uncovered forA = Nd-Lu, Y, Sc that exhibit a pressure-driven electronic reconstruction in the Nie_gmanifold. By disentangling the involvement of basal versus apical oxygen states at the Fermi surface, we identify Tb₃Ni₂O₇as an interesting candidate for superconductivity at ambient pressure. These results suggest a profound tunability of the structural and electronic phases in this novel materials class and are key for a fundamental understanding of the superconductivity mechanism.

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.

All-atom dynamics simulations are an indispensable quantitative tool in physics, chemistry, and materials science, but large systems and long simulation times remain challenging due to the trade-off between computational efficiency and predictive accuracy. To address this challenge, we combine effective two- and three-body potentials in a cubic B-spline basis with regularized linear regression to obtain machine-learning potentials that are physically interpretable, sufficiently accurate for applications, as fast as the fastest traditional empirical potentials, and two to four orders of magnitude faster than state-of-the-art machine-learning potentials. For data from empirical potentials, we demonstrate the exact retrieval of the potential. For data from density functional theory, the predicted energies, forces, and derived properties, including phonon spectra, elastic constants, and melting points, closely match those of the reference method. The introduced potentials might contribute towards accurate all-atom dynamics simulations of large atomistic systems over long-time scales.

The discovery of substrate materials has been dominated by trial and error, opening the opportunity for a systematic search. We generate bonding networks for materials from the Materials Project and systematically break up to three bonds in the networks for three-dimensional crystals. Successful cleavage reduces the bonding network to two periodic dimensions. We identify 4693 symmetrically unique cleavage surfaces across 2133 bulk crystals, 4626 of which have a maximum Miller index of one. We characterize the likelihood of cleavage by creating monolayers of these surfaces and calculating their thermodynamic stability using density functional theory to discover 3991 potential substrates. Following, we identify distinct trends in the work of cleavage and relate them to bonding in the three-dimensional precursor. We illustrate the potential impact of the substrate database by identifying several improved epitaxial substrates for the transparent conductor BaSnO₃. The open-source databases of predicted and commercial substrates are available at MaterialsWeb.org.