Dynamics and control of gold-encapped gallium arsenide nanowires imaged by 4D electron microscopy

Eutectic related reaction is a special chemical/physical reaction involving multiple phases, solid and liquid. Visualization of phase reaction of composite nanomaterials with high spatial and temporal resolution provides a key understanding of alloy growth with important industrial applications. However, it has been a rather challenging task. Here we report the direct imaging and control of the phase reaction dynamics of a single, as-grown free-standing gallium arsenide nanowire encapped with a gold nanoparticle, free from environmental confinement or disturbance, using four-dimensional electron microscopy. The non-destructive preparation of as-grown free-standing nanowires without supporting films allows us to study their anisotropic properties in their native environment with better statistical character. A laser heating pulse initiates the eutectic related reaction at a temperature much lower than the melting points of the composite materials, followed by a precisely time-delayed electron pulse to visualize the irreversible transient states of nucleation, growth and solidification of the complex. Combined with theoretical modeling, useful thermodynamic parameters of the newly formed alloy phases and their crystal structures could be determined. This technique of dynamical control and 4D imaging of phase reaction processes on the nanometer-ultrafast time scale open new venues for engineering various reactions in a wide variety of other systems

Analytical vectorial structure of non-paraxial four-petal Gaussian beams in the far field

The analytical vectorial structure of non-paraxial four-petal Gaussian beams(FPGBs) in the far field has been studied based on vector angular spectrum method and stationary phase method. In terms of analytical electromagnetic representations of the TE and TM terms, the energy flux distributions of the TE term, the TM term, and the whole beam are derived in the far field, respectively. According to our investigation, the FPGBs can evolve into a number of small petals in the far field. The number of the petals is determined by the order of input beam. The physical pictures of the FPGBs are well illustrated from the vectorial structure, which is beneficial to strengthen the understanding of vectorial properties of the FPGBs

Imaging rotational dynamics of nanoparticles in liquid by 4D electron microscopy

In real time and space, four-dimensional electron microscopy (4D EM) has enabled observation of transient structures and morphologies of inorganic and organic materials. We have extended 4D EM to include liquid cells without the time resolution being limited by the response of the detector. Our approach permits the imaging of the motion and morphological dynamics of a single, same particle on nanometer and ultrashort time scales. As a first application, we studied the rotational dynamics of gold nanoparticles in aqueous solution. A full transition from the conventional diffusive rotation to superdiffusive rotation and further to a ballistic rotation was observed with increasing asymmetry of the nanoparticle morphology. We explored the underlying physics both experimentally and theoretically according to the morphological asymmetry of the nanoparticles

Vectorial structure of a hard-edged-diffracted four-petal Gaussian beam in the far field

Based on the vector angular spectrum method and the stationary phase method and the fact that a circular aperture function can be expanded into a finite sum of complex Gaussian functions, the analytical vectorial structure of a four-petal Gaussian beam (FPGB) diffracted by a circular aperture is derived in the far field. The energy flux distributions and the diffraction effect introduced by the aperture are studied and illustrated graphically. Moreover, the influence of the f-parameter and the truncation parameter on the nonparaxiality is demonstrated in detail. In addition, the analytical formulas obtained in this paper can degenerate into un-apertured case when the truncation parameter tends to infinity. This work is beneficial to strengthen the understanding of vectorial properties of the FPGB diffracted by a circular aperture

Photoinduced nanobubble-driven superfast diffusion of nanoparticles imaged by 4D electron microscopy

Dynamics of active or propulsive Brownian particles in nonequilibrium status have recently attracted great interest in many fields including artificial micro/nanoscopic motors and biological entities. Understanding of their dynamics can provide insight into the statistical properties of physical and biological systems far from equilibrium. We report the translational dynamics of photon-activated gold nanoparticles (NPs) in water imaged by liquid-cell four-dimensional electron microscopy (4D-EM) with high spatiotemporal resolution. Under excitation of femtosecond laser pulses, we observed that those NPs exhibit superfast diffusive translation with a diffusion constant four to five orders of magnitude greater than that in the absence of laser excitation. The measured diffusion constant follows a power-law dependence on the laser fluence and a linear increase with the laser repetition rate, respectively. This superfast diffusion of the NPs is induced by a strong random driving force arising from the photoinduced steam nanobubbles (NBs) near the NP surface. In contrast, the NPs exhibit a superfast ballistic translation at a short time scale down to nanoseconds. Combining with a physical model simulation, this study reveals a photoinduced NB propulsion mechanism for propulsive motion, providing physical insights into better design of light-activated artificial micro/nanomotors. The liquid-cell 4D-EM also provides the potential of studying other numerical dynamical behaviors in their native environments

Photoinduced nanobubble-driven superfast diffusion of nanoparticles imaged by 4D electron microscopy

Dynamics of active or propulsive Brownian particles in nonequilibrium status have recently attracted great interest in many fields including artificial micro/nanoscopic motors and biological entities. Understanding of their dynamics can provide insight into the statistical properties of physical and biological systems far from equilibrium. We report the translational dynamics of photon-activated gold nanoparticles (NPs) in water imaged by liquid-cell four-dimensional electron microscopy (4D-EM) with high spatiotemporal resolution. Under excitation of femtosecond laser pulses, we observed that those NPs exhibit superfast diffusive translation with a diffusion constant four to five orders of magnitude greater than that in the absence of laser excitation. The measured diffusion constant follows a power-law dependence on the laser fluence and a linear increase with the laser repetition rate, respectively. This superfast diffusion of the NPs is induced by a strong random driving force arising from the photoinduced steam nanobubbles (NBs) near the NP surface. In contrast, the NPs exhibit a superfast ballistic translation at a short time scale down to nanoseconds. Combining with a physical model simulation, this study reveals a photoinduced NB propulsion mechanism for propulsive motion, providing physical insights into better design of light-activated artificial micro/nanomotors. The liquid-cell 4D-EM also provides the potential of studying other numerical dynamical behaviors in their native environments