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1.
Nano Lett ; 23(4): 1481-1488, 2023 Feb 22.
Artículo en Inglés | MEDLINE | ID: mdl-36723175

RESUMEN

Femtosecond laser pulses drive nonequilibrium phase transitions via reaction paths hidden in thermal equilibrium. This stimulates interest to understand photoinduced ultrafast melting processes, which remains incomplete due to challenges in resolving accompanied kinetics at the relevant space-time resolution. Here, by newly establishing a multiplexing femtosecond X-ray probe, we have successfully revealed ultrafast energy transfer processes in confined Au nanospheres. Real-time images of electron density distributions with the corresponding lattice structures elucidate that the energy transfer begins with subpicosecond melting at the specimen boundary earlier than the lattice thermalization, and proceeds by forming voids. Two temperature molecular dynamics simulations uncovered the presence of both heterogeneous melting with the melting front propagation from surface and grain boundaries and homogeneous melting with random melting seeds and nanoscale voids. Supported by experimental and theoretical results, we provide a comprehensive atomic-scale picture that accounts for the ultrafast laser-induced melting and evaporation kinetics.

2.
Proc Natl Acad Sci U S A ; 115(50): 12654-12661, 2018 12 11.
Artículo en Inglés | MEDLINE | ID: mdl-30530677

RESUMEN

Stories of mega-jams that last tens of hours or even days appear not only in fiction but also in reality. In this context, it is important to characterize the collapse of the network, defined as the transition from a characteristic travel time to orders of magnitude longer for the same distance traveled. In this multicity study, we unravel this complex phenomenon under various conditions of demand and translate it to the travel time of the individual drivers. First, we start with the current conditions, showing that there is a characteristic time τ that takes a representative group of commuters to arrive at their destinations once their maximum density has been reached. While this time differs from city to city, it can be explained by Γ, defined as the ratio of the vehicle miles traveled to the total vehicle distance the road network can support per hour. Modifying Γ can improve τ and directly inform planning and infrastructure interventions. In this study we focus on measuring the vulnerability of the system by increasing the volume of cars in the network, keeping the road capacity and the empirical spatial dynamics from origins to destinations unchanged. We identify three states of urban traffic, separated by two distinctive transitions. The first one describes the appearance of the first bottlenecks and the second one the collapse of the system. This collapse is marked by a given number of commuters in each city and it is formally characterized by a nonequilibrium phase transition.

3.
Proc Natl Acad Sci U S A ; 114(18): 4631-4636, 2017 05 02.
Artículo en Inglés | MEDLINE | ID: mdl-28416689

RESUMEN

Active fluids are a class of nonequilibrium systems where energy is injected into the system continuously by the constituent particles themselves. Many examples, such as bacterial suspensions and actomyosin networks, are intrinsically chiral at a local scale, so that their activity involves torque dipoles alongside the force dipoles usually considered. Although many aspects of active fluids have been studied, the effects of chirality on them are much less known. Here, we study by computer simulation the dynamics of an unstructured droplet of chiral active fluid in three dimensions. Our model considers only the simplest possible combination of chiral and achiral active stresses, yet this leads to an unprecedented range of complex motilities, including oscillatory swimming, helical swimming, and run-and-tumble motion. Strikingly, whereas the chirality of helical swimming is the same as the microscopic chirality of torque dipoles in one regime, the two are opposite in another. Some of the features of these motility modes resemble those of some single-celled protozoa, suggesting that underlying mechanisms may be shared by some biological systems and synthetic active droplets.

4.
Nano Lett ; 17(5): 2994-2998, 2017 05 10.
Artículo en Inglés | MEDLINE | ID: mdl-28394624

RESUMEN

We investigate the dramatic switch of resistance in ordered correlated insulators when they are driven out of equilibrium by a strong voltage bias. Microscopic calculations on a driven-dissipative lattice of interacting electrons explain the main experimental features of resistive switching (RS), such as the hysteretic I-V curves and the formation of hot conductive filaments. The energy-resolved electron distribution at the RS reveals the underlying nonequilibrium electronic mechanism, namely Landau-Zener tunneling, and also justifies a thermal description in which the hot-electron temperature, estimated from the first moment of the distribution, matches the equilibrium-phase transition temperature. We discuss the tangled relationship between filament growth and negative differential resistance and the influence of crystallographic structure and disorder in the RS.

5.
ACS Appl Mater Interfaces ; 11(36): 33043-33053, 2019 Sep 11.
Artículo en Inglés | MEDLINE | ID: mdl-31419106

RESUMEN

It is notoriously difficult to distinguish the stoichiometric LiCoO2 (LCO) with a O3-I structure from its lithium defective O3-II phase because of their similar crystal symmetry. Interestingly, moreover, the O3-II phase shows metallic conductivity, whereas the O3-I phase is an electronic insulator. How to effectively reveal the intrinsic mechanism of the conductivity difference and nonequilibrium phase transition induced by the lithium deintercalation is of vital importance for its practical application and development. Based on the developed technology of in situ peak force tunneling atomic force microscopy (PF-TUNA) in liquids, the phase transition from O3-I to O3-II and consequent insulator-to-metal transition of LCO thin-film electrodes with preferred (003) orientation nanorods designed and prepared via magnetron sputtering were observed under an organic electrolyte for the first time in this work. Then, studying the post-mortem LCO thin-film electrode by using ex situ time-dependent XRD and conductive atomic force microscopy, we find the phase relaxation of LCO electrodes after the nonequilibrium deintercalation, further proving the differences of the electronic conductivity and work function between the O3-I and O3-II phases. Moreover, X-ray absorption spectroscopy results indicate that the oxidation of Co ions and the increasing of O 2p-Co 3d hybridization in the O3-II phase lead to electrical conductivity improvement in Li1-xCoO2. Simultaneously, it is found that the nonequilibrium deintercalation at a high charging rate can result in phase-transition hysteresis and the O3-I/O3-II coexistence at the charging end, which is explained well by an ionic blockade model with an antiphase boundary. At last, this work strongly suggests that PF-TUNA can be used to reveal the unconventional phenomena on the solid/liquid interfaces.

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