Capturing Nucleation at 4D Atomic Resolution

Nucleation plays a critical role in many physical and biological phenomena ranging from crystallization, melting and evaporation to the formation of clouds and the initiation of neurodegenerative diseases. However, nucleation is a challenging process to study in experiments especially in the early stage when several atoms/molecules start to form a new phase from its parent phase. Here, we advance atomic electron tomography to study early stage nucleation at 4D atomic resolution. Using FePt nanoparticles as a model system, we reveal that early stage nuclei are irregularly shaped, each has a core of one to few atoms with the maximum order parameter, and the order parameter gradient points from the core to the boundary of the nucleus. We capture the structure and dynamics of the same nuclei undergoing growth, fluctuation, dissolution, merging and/or division, which are regulated by the order parameter distribution and its gradient. These experimental observations differ from classical nucleation theory (CNT) and to explain them we propose the order parameter gradient (OPG) model. We show the OPG model generalizes CNT and energetically favours diffuse interfaces for small nuclei and sharp interfaces for large nuclei. We further corroborate this model using molecular dynamics simulations of heterogeneous and homogeneous nucleation in liquid-solid phase transitions of Pt. We anticipate that the OPG model is applicable to different nucleation processes and our experimental method opens the door to study the structure and dynamics of materials with 4D atomic resolution.Comment: 42 pages, 5 figures, 12 supplementary figures and one supplementary tabl

Watermark Embedded in Polygonal Line for Copyright Protection of Contour Map

In GIS system, we often use vector contour map to show or locate position on the earth. Since such map data is very worthy of value, it is necessary and important to protect its copyright. In this paper, we propose a new method to embed watermark into the angle parameter of polygonal lines or curves in a contour map after its parameterization. The watermark can be detected as proof of the ownership or authority of the map by hypothesis test. Key words

Experimental Study on the Mechanics Characteristics of CFRP Strengthening of Highway Tunnels at Different Damage States

Cracks and other diseases may occur in the long-term operation of highway tunnels and reduce the structural load-carrying capacity. Strengthening using carbon fiber reinforced polymer (CFRP) sheets and other materials could extend the service time of the tunnels. However, the process of strengthening tunnels is remarkably different from the process of strengthening aboveground structures because of the secondary load. In order to understand the development of stress and deformation of strengthened tunnels under secondary load, a 1 : 10 scaled model was tested to simulate the tunnel strengthened with CFRP under different damage states. The test results show that CFRP strengthening improved the stiffness of the structure and inhibited the propagation of the existing cracks. The peeling of the CFRP sheets made the strengthened structure quickly lose its load-carrying capacity, causing the instability of the structure. The failure loads of the structures strengthened at different damage states were essentially the same, with an average value of 184% of the original failure load. Nevertheless, the early strengthening helped control the structural deformation. The test results also demonstrate that the bonding strength between the CFRP and the lining is essential for strengthening effectiveness. This study provides a theoretical basis for similar engineering reinforcement designs

Out-of-plane ferroelectricity and robust magnetoelectricity in quasi two-dimensional materials

<p>Thin film ferroelectrics have been pursued for capacitive and nonvolatile memory devices. They rely on polarizations that are oriented in an out-of-plane direction to facilitate integration and addressability with CMOS architectures. The internal depolarization field, however, formed by surface charges can suppress the out-of-plane polarization in ultrathin ferroelectric films that could otherwise exhibit lower coercive fields and operate with lower power. Here we unveil stabilization of a polar longitudinal optical (LO) mode in the <em>n</em>=2 Ruddlesden–Popper family that produces out-of-plane ferroelectricity, persists under open-circuit boundary conditions, and is distinct from hyperferroelectricity. Our first-principles calculations show the stabilization of the LO mode is ubiquitous in chalcogenides and halides and relies on anharmonic trilinear mode coupling. We further show that the out-of-plane ferroelectricity can be predicted with a crystallographic tolerance factor, and we use these insights to design a room-temperature multiferroic with strong magnetoelectric coupling suitable for magneto-electric spin-orbit transistors.  </p><p>Funding provided by: National Science Foundation<br>Crossref Funder Registry ID: https://ror.org/021nxhr62<br>Award Number: </p><p>Funding provided by: United States Department of Energy<br>Crossref Funder Registry ID: https://ror.org/01bj3aw27<br>Award Number: </p&gt

High Efficiency Inverted Planar Perovskite Solar Cells with Solution-Processed NiO_<i>x</i> Hole Contact

NiO_<i>x</i> is a promising hole-transporting material for perovskite solar cells due to its high hole mobility, good stability, and easy processability. In this work, we employed a simple solution-processed NiO_<i>x</i> film as the hole-transporting layer in perovskite solar cells. When the thickness of the perovskite layer increased from 270 to 380 nm, the light absorption and photogenerated carrier density were enhanced and the transporting distance of electron and hole would also increase at the same time, resulting in a large charge transfer resistance and a long hole-extracted process in the device, characterized by the UV–vis, photoluminescence, and electrochemical impedance spectroscopy spectra. Combining both of these factors, an optimal thickness of 334.2 nm was prepared with the perovskite precursor concentration of 1.35 M. Moreover, the optimal device fabrication conditions were further achieved by optimizing the thickness of NiO_<i>x</i> hole-transporting layer and PCBM electron selective layer. As a result, the best power conversion efficiency of 15.71% was obtained with a <i>J</i>_sc of 20.51 mA·cm^–2, a <i>V</i>_oc of 988 mV, and a FF of 77.51% with almost no hysteresis. A stable efficiency of 15.10% was caught at the maximum power point. This work provides a promising route to achieve higher efficiency perovskite solar cells based on NiO or other inorganic hole-transporting materials

Capturing Nucleation at 4D Atomic Resolution

Nucleation plays a critical role in many physical and biological phenomena ranging from crystallization, melting and evaporation to the formation of clouds and the initiation of neurodegenerative diseases. However, nucleation is a challenging process to study in experiments especially in the early stage when several atoms/molecules start to form a new phase from its parent phase. Here, we advance atomic electron tomography to study early stage nucleation at 4D atomic resolution. Using FePt nanoparticles as a model system, we reveal that early stage nuclei are irregularly shaped, each has a core of one to few atoms with the maximum order parameter, and the order parameter gradient points from the core to the boundary of the nucleus. We capture the structure and dynamics of the same nuclei undergoing growth, fluctuation, dissolution, merging and/or division, which are regulated by the order parameter distribution and its gradient. These experimental observations differ from classical nucleation theory (CNT) and to explain them we propose the order parameter gradient (OPG) model. We show the OPG model generalizes CNT and energetically favours diffuse interfaces for small nuclei and sharp interfaces for large nuclei. We further corroborate this model using molecular dynamics simulations of heterogeneous and homogeneous nucleation in liquid-solid phase transitions of Pt. We anticipate that the OPG model is applicable to different nucleation processes and our experimental method opens the door to study the structure and dynamics of materials with 4D atomic resolution

Observing crystal nucleation in four dimensions using atomic electron tomography.

Nucleation plays a critical role in many physical and biological phenomena that range from crystallization, melting and evaporation to the formation of clouds and the initiation of neurodegenerative diseases1-3. However, nucleation is a challenging process to study experimentally, especially in its early stages, when several atoms or molecules start to form a new phase from a parent phase. A number of experimental and computational methods have been used to investigate nucleation processes4-17, but experimental determination of the three-dimensional atomic structure and the dynamics of early-stage nuclei has been unachievable. Here we use atomic electron tomography to study early-stage nucleation in four dimensions (that is, including time) at atomic resolution. Using FePt nanoparticles as a model system, we find that early-stage nuclei are irregularly shaped, each has a core of one to a few atoms with the maximum order parameter, and the order parameter gradient points from the core to the boundary of the nucleus. We capture the structure and dynamics of the same nuclei undergoing growth, fluctuation, dissolution, merging and/or division, which are regulated by the order parameter distribution and its gradient. These experimental observations are corroborated by molecular dynamics simulations of heterogeneous and homogeneous nucleation in liquid-solid phase transitions of Pt. Our experimental and molecular dynamics results indicate that a theory beyond classical nucleation theory1,2,18 is needed to describe early-stage nucleation at the atomic scale. We anticipate that the reported approach will open the door to the study of many fundamental problems in materials science, nanoscience, condensed matter physics and chemistry, such as phase transition, atomic diffusion, grain boundary dynamics, interface motion, defect dynamics and surface reconstruction with four-dimensional atomic resolution

Determining the three-dimensional atomic structure of an amorphous solid.

Amorphous solids such as glass, plastics and amorphous thin films are ubiquitous in our daily life and have broad applications ranging from telecommunications to electronics and solar cells1-4. However, owing to the lack of long-range order, the three-dimensional (3D) atomic structure of amorphous solids has so far eluded direct experimental determination5-15. Here we develop an atomic electron tomography reconstruction method to experimentally determine the 3D atomic positions of an amorphous solid. Using a multi-component glass-forming alloy as proof of principle, we quantitatively characterize the short- and medium-range order of the 3D atomic arrangement. We observe that, although the 3D atomic packing of the short-range order is geometrically disordered, some short-range-order structures connect with each other to form crystal-like superclusters and give rise to medium-range order. We identify four types of crystal-like medium-range order-face-centred cubic, hexagonal close-packed, body-centred cubic and simple cubic-coexisting in the amorphous sample, showing translational but not orientational order. These observations provide direct experimental evidence to support the general framework of the efficient cluster packing model for metallic glasses10,12-14,16. We expect that this work will pave the way for the determination of the 3D structure of a wide range of amorphous solids, which could transform our fundamental understanding of non-crystalline materials and related phenomena