Direct mapping of bending and torsional dynamics in individual nanostructures.

Investigating coherent acoustic vibrations in nanostructured materials provides fundamental insights into optomechanical responses and microscopic energy flow. Extensive measurements of vibrational dynamics have been performed for a wide variety of nanoparticles and nanoparticle assemblies. However, virtually all of them show that only the dilation modes are launched after laser excitations, and the acoustic bending and torsional motions, which are commonly observed in photoexcited chemical bonds, are absent. Unambiguous identification and refined characterization of these "missing" modes have been a long-standing issue. In this report, we investigated the acoustic vibrational dynamics of individual Au nanoprisms on free-standing graphene substrates using an ultrafast high-sensitivity dark-field imaging approach in four-dimensional transmission electron microscopy. Following optical excitations, we observed low-frequency multiple-mode oscillations and higher superposition amplitudes at nanoprism corners and edges on the subnanoparticle level. In combination with finite-element simulations, we determined that these vibrational modes correspond to out-of-plane bending and torsional motions, superimposed by an overall tilting effect of the nanoprisms. The launch and relaxation processes of these modes are highly pertinent to substrate effects and nanoparticle geometries. These findings contribute to the fundamental understanding about acoustic dynamics of individual nanostructures and their interaction with substrates.

4D electron microscopy of T cell activation.

T cells can be controllably stimulated through antigen-specific or nonspecific protocols. Accompanying functional hallmarks of T cell activation can include cytoskeletal reorganization, cell size increase, and cytokine secretion. Photon-induced near-field electron microscopy (PINEM) is used to image and quantify evanescent electric fields at the surface of T cells as a function of various stimulation conditions. While PINEM signal strength scales with multiple of the biophysical changes associated with T cell functional activation, it mostly strongly correlates with antigen-engagement of the T cell receptors, even under conditions that do not lead to functional T cell activation. PINEM image analysis suggests that a stimulation-induced reorganization of T cell surface structure, especially over length scales of a few hundred nanometers, is the dominant contributor to these PINEM signal changes. These experiments reveal that PINEM can provide a sensitive label-free probe of nanoscale cellular surface structures.

Visualization of Plasmonic Couplings Using Ultrafast Electron Microscopy.

Hybrids of graphene and metal plasmonic nanostructures are promising building blocks for applications in optoelectronics, surface-enhanced scattering, biosensing, and quantum information. An understanding of the coupling mechanism in these hybrid systems is of vital importance to its applications. Previous efforts in this field mainly focused on spectroscopic studies of strong coupling within the hybrids with no spatial resolution. Here we report direct imaging of the local plasmonic coupling between single Au nanocapsules and graphene step edges at the nanometer scale by photon-induced near-field electron microscopy in an ultrafast electron microscope for the first time. The proximity of a step in the graphene to the nanocapsule causes asymmetric surface charge density at the ends of the nanocapsules. Computational electromagnetic simulations confirm the experimental observations. The results reported here indicate that this hybrid system could be used to manipulate the localized electromagnetic field on the nanoscale, enabling promising future plasmonic devices.

Contactless Discharge-Driven Droplet Motion on a Nonslippery Polymer Surface.

Droplet manipulation is the cornerstone of many modern technologies. It is still challenging to drive the droplet motion on nonslippery surfaces flexibly. We present a droplet manipulation method on nonslippery polymer surfaces based on the corona discharge. With the corona discharge of two-needle electrodes with opposite polarities, the droplet's charge polarity can be switched, which results in the directionally droplet transport on a charged polymer surface with the oscillation. Here, such droplet behaviors are presented in detail. Dependence of the motion on the critical distance and driving distance between the droplet and the needle electrode is revealed. The driving mechanism is verified by experiments and simulations. This work enriches the droplet manipulation techniques on nonslippery surfaces for various applications, such as combinatory chemistry, biochemical, and medical detection.

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 a 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 (4D) electron microscopy. The nondestructive 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 aided by 4D imaging of phase reaction processes on the nanometer-ultrafast time scale opens new venues for engineering various reactions in a wide variety of other systems.

Photon-Induced Near-Field Electron Microscopy of Eukaryotic Cells.

Photon-induced near-field electron microscopy (PINEM) is a technique to produce and then image evanescent electromagnetic fields on the surfaces of nanostructures. Most previous applications of PINEM have imaged surface plasmon-polariton waves on conducting nanomaterials. Here, the application of PINEM on whole human cancer cells and membrane vesicles isolated from them is reported. We show that photons induce time-, orientation-, and polarization-dependent evanescent fields on the surfaces of A431 cancer cells and isolated membrane vesicles. Furthermore, the addition of a ligand to the major surface receptor on these cells and vesicles (epidermal growth factor receptor, EGFR) reduces the intensity of these fields in both preparations. We propose that in the absence of plasmon waves in biological samples, these evanescent fields reflect the changes in EGFR kinase domain polarization upon ligand binding.

4D imaging and diffraction dynamics of single-particle phase transition in heterogeneous ensembles.

In this Letter, we introduce conical-scanning dark-field imaging in four-dimensional (4D) ultrafast electron microscopy to visualize single-particle dynamics of a polycrystalline ensemble undergoing phase transitions. Specifically, the ultrafast metal-insulator phase transition of vanadium dioxide is induced using laser excitation and followed by taking electron-pulsed, time-resolved images and diffraction patterns. The single-particle selectivity is achieved by identifying the origin of all constituent Bragg spots on Debye-Scherrer rings from the ensemble. Orientation mapping and dynamic scattering simulation of the electron diffraction patterns in the monoclinic and tetragonal phase during the transition confirm the observed behavior of Bragg spots change with time. We found that the threshold temperature for phase recovery increases with increasing particle sizes and we quantified the observation through a theoretical model developed for single-particle phase transitions. The reported methodology of conical scanning, orientation mapping in 4D imaging promises to be powerful for heterogeneous ensemble, as it enables imaging and diffraction at a given time with a full archive of structural information for each particle, for example, size, morphology, and orientation while minimizing radiation damage to the specimen.

Dynamic study on the transformation process of gold nanoclusters.

In this paper, the transformation process from Au8 to Au25 nanoclusters (NCs) is investigated with steady state fluorescence spectroscopy and time-resolved fluorescence spectroscopy at various reaction temperatures and solvent diffusivities. Results demonstrate that Au8 NCs, protected by bovine serum albumin, transform into Au25 NCs under controlled pH values through an endothermic reaction with the activation energy of 74 kJ mol(-1). Meanwhile, the characteristic s-shaped curves describing the formation of Au25 NCs suggest this process involves a diffusion controlled growth mechanism.

Time-resolved structural dynamics of thin metal films heated with femtosecond optical pulses.

We utilize 100 fs optical pulses to induce ultrafast disorder of 35- to 150-nm thick single Au(111) crystals and observe the subsequent structural evolution using 0.6-ps, 8.04-keV X-ray pulses. Monitoring the picosecond time-dependent modulation of the X-ray diffraction intensity, width, and shift, we have measured directly electron/phonon coupling, phonon/lattice interaction, and a histogram of the lattice disorder evolution, such as lattice breath due to a pressure wave propagating at sonic velocity, lattice melting, and recrystallization, including mosaic formation. Results of theoretical simulations agree and support the experimental data of the lattice/liquid phase transition process. These time-resolved X-ray diffraction data provide a detailed description of all the significant processes induced by ultrafast laser pulses impinging on thin metallic single crystals.

Nanoscale subparticle imaging of vibrational dynamics using dark-field ultrafast transmission electron microscopy.

An understanding of nanoscale energy transport and acoustic response is important for applications of nanomaterials but hinges on a complete characterization of their structural dynamics. The precise determination of the structural dynamics within nanoparticles, however, is still challenging and requires high spatiotemporal resolution and detection sensitivity. Here we present a centred dark-field imaging approach based on ultrafast transmission electron microscopy that is capable of directly mapping the picosecond-scale evolution of intrananoparticle vibration with a spatial resolution down to 3 nm. Using this approach, we investigated the photo-induced vibrational dynamics in individual gold heterodimers composed of a nanoprism and a nanosphere. We observed not only the retardation of in-plane vibrations in the nanoprisms, which we attribute to thermal and vibrational energy transferred from adjacent nanospheres mediated by surfactants, but also the existence of a complex multimodal oscillation and its spatial variation within individual nanoprisms. This work represents an advance in real-space mapping of vibrational dynamics on the subnanoparticle level with a high detection sensitivity.

Carrier dynamics in InN nanorod arrays.

In this report, we investigated ultrafast carrier dynamics of vertically aligned indium nitride (InN) nanorod (NR) arrays grown by molecular-beam epitaxy on Si(111) substrates. Dominant band filling effects were observed and were attributed to a partial bleaching of absorption at the probe wavelengths near the absorption edge. Carrier relaxation in nanorod samples was strongly dependent on the rod size and length. In particular, a fast initial decay was observed for carriers in NRs with a small diameter (~30 nm), the lifetime of which is much shorter than the carrier cooling time, demonstrating the substantial surface-associated influence on carrier relaxation in semiconductor nanostructures.

Pumping-power-dependent photoluminescence angular distribution from an opal photonic crystal composed of monodisperse Eu3+/SiO2 core/shell nanospheres.

High quality opal photonic crystals (PhCs) were successfully fabricated by self-assembling of monodisperse Eu(3+)/SiO(2) core/shell nanospheres. Angular resolved photoluminescence (PL) spectra of a PhC sample were measured with different pumping powers, and its PL emission strongly depended on spectroscopic position of the photonic stop band and the optical pumping power. Suppression of the PL occurred in the directions where the emission lines aligned with the center of the photonic stop band. Suppression and enhancement of the PL were observed at low- and high-pumping powers, respectively, in the directions where the emission lines were located at the edges of the photonic stop band. When pumping power exceeded 6 µJ/pulse, a super-linear dependence was found between the pumping power and PL intensity. The dramatic enhancement of PL was attributed to the amplification of spontaneous emission resulted from the creation of large population inversion and the slow group velocity of the emitted light inside the PhC. The opal PhC provided highly angular-selective quasi-monochromatic PL output, which can be useful for a variety of optical applications.

Temperature dependent spectral properties of type-I and quasi type-II CdSe/CdS dot-in-rod nanocrystals.

We investigated systematically the temperature dependence of the spectral properties such as the band gap, bandwidth and fluorescence intensity of CdSe/CdS dot-in-rod nanocrystals. These asymmetry nanoparticles were synthesized by seeded growth techniques with band alignment of the type-I and quasi type-II with initial core sizes of 3.3 and 2.3 nm, respectively. With increasing temperature the band gap decreases and bandwidth increases, largely due to exciton-phonon scattering. Anomalous variations of the band gap and bandwidth were observed at 200-240 K, and the variations are attributed to the anisotropic strain in the CdSe/CdS interface due to temperature dependent lattice mismatch. The integrated intensity of fluorescence shows two variation regimes. In the low temperature regime, the intensity remained roughly constant due to the temperature dependent carrier mobility and trapping by the defect states in the CdS shell. However, in the higher temperature regime, the intensity decreased quickly due to thermal/phonon assisted escape from the CdSe dot. The barrier depths are estimated to be about 557 and 285 meV for type-I and quasi type-II samples, respectively.

High-efficiency cascade CdS/CdSe quantum dot-sensitized solar cells based on hierarchical tetrapod-like ZnO nanoparticles.

Quantum dot-sensitized solar cells (QDSCs) constructed using cascade CdS/CdSe sensitizers and the novel tetrapod-like ZnO nanoparticles have been fabricated. The cascade co-sensitized QDSCs manifested good electron transfer dynamics and overall power conversion efficiency, compared to single CdS- or CdSe-sensitized cells. The preliminary CdS layer is not only energetically favorable to electron transfer but behaves as a passivation layer to diminish the formation of interfacial defects during CdSe synthesis. On the other hand, the anisotropic tetrapod-like ZnO nanoparticles, with a high electron diffusion coefficient, can afford a better carrier transport than traditional ZnO nanoparticles. The resultant solar cell yielded an excellent performance with a solar power conversion efficiency of 4.24% under simulated one sun (AM1.5G, 100 mW cm(-2)) illumination.

Mass oscillations and matter wave's phase and amplitude modulations of relativistic quantum particles induced by Heisenberg's uncertainty principle.

We present a flip-flop dual-component model to treat quantum dynamics of relativistic particles with a rest mass and investigate the matter waves' phase and amplitude modulations due to Heisenberg's uncertainty principle. Their matter waves behave like a traveling Gaussian-shaped wave packet accompanied by a guiding pilot wave, and the phase modulations result in mass oscillations. These effects are more prominent for light-weighted elementary particles, such as neutrinos and electrons. This mechanism is solely due to the uncertainty principle and has nothing to do with the flavor-mixing of neutrinos. Simulations using neutrinos and electrons are presented, which indicate an oscillation period on the order of ps. This study primarily focuses on the predicted mass oscillations induced by the uncertainty principle. A slit-type interference experiment using neutrinos and electrons from reactors is proposed to test the predicted behaviors.

Research on the rapid combustion process of butane under microwave discharge.

To study the combustion process of fuel in the microwave plasma torch, we designed a butane microwave plasma device exploiting a tungsten rod as an electrode. Through analysis of the image record by high-speed camera, we found that the discharge of butane microwave plasma torch is a cyclic process at atmospheric pressure at a frequency  of around 100 Hz. During the discharge, the active particles continuously diffuse from the electrode to the outside like the bloom of the flower. Then, the variation of plasma torch of jet height and temperature with microwave power is obtained. In addition, we studied the effects of different butane flow rates on the plasma torch. The results illustrate that excessive butane will lead to carbon deposition on the electrode. All in all, this work provides a new understanding of the combustion of the microwave plasma torch, which is conducive to the further development of microwave plasma in the fields of waste gas treatment, fuel combustion, and plasma engine.

Contactless Discharge-Driven Method for Separation of Oil-Water Mixtures.

Oil-water separation technology has potential applications in wastewater treatment, petroleum refining and edible oil processing. As the ultimate means in oil-water treatment, electrostatic coalescence technology has been widely used in oil fields and refineries. However, the technology has many problems, such as complex processes, electrode corrosion, and the inability to treat high-water-cut crude oil emulsions. Here, we propose a contactless method of oil-water separation by corona discharge. With corona discharge of a needle-plate electrode configuration, the oil droplet diffuses to the ITO glass surface and the water droplet oscillates at the edge of the PET film. Here, such droplet behaviors are described in detail. Based on the motion behavior of the oil and water droplet, we designed an efficient oil-water separation device. After the oil-water mixture passes through the device, the oil content in the oil region can reach 99.25% with a voltage of 8 kV. In addition, the separation speed of the oil-water mixture can also be adjusted by varying the corona discharge voltage. This paper presents a simple and innovative method for oil-water separation.

High-power, passively mode-locked Nd:GdVO4 laser using single-walled carbon nanotubes as saturable absorber.

We use a new (to our knowledge) fabrication method of a single-walled carbon nanotube (SWCNT) absorber without polymer to sustain high-power illumination. Using a series of saturable absorbers (SAs) incorporating different amounts of SWCNTs, we demonstrate mode-locking for a Nd:GdVO4 laser in the 1 µm spectral range. Continuous-wave mode-locking (CWML) pulses with a maximum output power of 3.6 W at 1063 nm and high noise extinction of 61 dB has been achieved to give the highest pulse peak power of 3.6 kW and pulse energy of 30 nJ under 15 W pumping. To our knowledge, this is the highest CWML output power with SWCNT-SAs reported. The measured nonlinear absorption of the SWCNT-SAs shows a modulation depth of ~3% with subpicosecond recovery time.

A highly efficient graphene oxide absorber for Q-switched Nd:GdVO4 lasers.

We demonstrated that graphene oxide material could be used as a highly efficient saturable absorber for the Q-switched Nd:GdVO4 laser. A novel and low-cost graphene oxide (GO) absorber was fabricated by a vertical evaporation technique and high viscosity of polyvinyl alcohol (PVA) aqueous solution. A piece of GO/PVA absorber, a piece of round quartz, and an output coupler mirror were combined to be a sandwich structure passive component. Using such a structure, 104 ns pulses and 1.22 W average output power were obtained with the maximum pulse energy at 2 µJ and a slope efficiency of 17%.

Photoinduced multimode coherent acoustic phonons of metallic nanoprisms and the effects of shape-induced anisotropic electronic stresses.

In this work we reported experimental measurements of ultrafast structural dynamics in metallic nanoprisms induced by a femtosecond laser pulse. The main focus of this study of anisotropic heating in nanoprisms is about laser fluence effects on photoexcitation of two planar coherent acoustic phonon modes, namely, the breathing mode and the totally symmetric mode. We presented a combined two-temperature model and 2-D Fermi-Pasta-Ulam model to explain both the dependence of the initial phases and the mode weight on the excitation power. Our transient optical absorption data for both the initial fast monotonic decay and the subsequent coherent acoustic oscillations clearly indicate the presence of anisotropic thermal expansion in nanoprisms.