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The electrocaloric effect (ECE) offers a promising alternative to the traditional gas compressing refrigeration due to its high efficiency and environmental friendliness. The unusual negative electrocaloric effect refers to the adiabatic temperature drops due to application of electric field, in contrast with the normal (positive) ECE, and provides ways to improve the electrocaloric efficiency in refrigeration cycles. However, negative ECE is unusual and requires a clear understanding of microscopic mechanisms. Here, we found unexpected and extensive negative ECE in nonpolar orthorhombic, tetragonal, and cubic phases of halide and oxide perovskite at wide range of temperature by means of first-principle-based large scale Monte Carlo methods. Such unexpected negative ECE originates from the octahedral tilting related entropy change rather than the polarization entropy change under the application of electric field. Furthermore, a giant negative ECE with temperature change of 8.6 K is found at room temperature. This giant and extensive negative ECE in perovskite opens up new horizon in the research of caloric effects and broadens the electrocaloric refrigeration ways with high efficiency., Comment: 11 pages, 7 figures

The first-principles-based effective Hamiltonian is widely used to predict and simulate the properties of ferroelectrics and relaxor ferroelectrics. However, the parametrization method of the effective Hamiltonian is complicated and hardly can resolve the systems with complex interactions and/or complex components. Here, we developed an on-the-fly machine learning approach to parametrize the effective Hamiltonian based on Bayesian linear regression. The parametrization is completed in molecular dynamics simulations, with the energy, forces and stress predicted at each step along with their uncertainties. First-principles calculations are executed when the uncertainties are large to retrain the parameters. This approach provides a universal and automatic way to compute the effective Hamiltonian parameters for any considered systems including complex systems which previous methods can not handle. BaTiO3 and Pb(Sc,Ta)O3 are taken as examples to show the accurateness of this approach comparing with conventional first-principles parametrization method., Comment: 11 pages, 2 figures

Non-collinear spin order that breaks space inversion symmetry and allows efficient electric-field control of magnetism makes BiFeO$_3$ a promising candidate for applications in low-power spintronic devices. Epitaxial strain effects have been intensively studied and exhibit significant modulation of the magnetic order in BiFeO$_3$, but tuning its spin structure with continuously varied uniaxial strain is still lacking up to date. Here, we apply \emph{in situ} uniaxial strain to a freestanding BiFeO$_3$ film and use scanning NV microscope to image the nanoscale magnetic order in real-space. The strain is continuously increased from 0\% to 1.5\% and four images under different strains are acquired during this period. The images show that the spin cycloid tilts by $\sim 12.6^\circ$ when strain approaches 1.5\%. A first principle calculation has been processed to show that the tilting is energetically favorable under such strain. Our \emph{in situ} strain applying method in combination with scanning NV microscope real-space imaging ability paves a new way in studying the coupling between magnetic order and strain in BiFeO$_3$ films., Comment: 11 pages, 4 figures in main text, 5 figures in SI

Silicon–carbon composites, which exhibit the advantages of both carbon and silicon materials, are regarded as the most promising anode for lithium ion battery. In this work, a composite of 3D graphene-like nanosheets/silicon wrapped by catalytic graphite (G-3DGNs-Si) was prepared via a chemical oxidation–thermal expansion strategy and high-temperature sintering method. The obvious interlinked 3D-layered spaces in 3DGNs arranged orderly can uniformly accommodate silicon nanoparticles (SiNPs). 3DGNs can relieve the volume expansion and improve the electrical conductivity of SiNPs. In addition, the catalytic graphite evenly coated on the 3DGNs-Si can further improve electrochemical performance. The G-3DGNs-Si composite anode can achieve 90% reversible capacity retention (957.2 mAh g−1) at 0.2 A g−1 after 100 cycles (78.9% after 300 cycles). The method is effective and easy to operate. This work provides a novel idea for designing silicon–carbon composites.