Mechanism of Single-Cycle THz Pulse Generation and X-ray Emission: Water-Flow Irradiated by Two Ultra-Short Laser Pulses.

The interaction of two subsequent ultra-short sub-milli-Joule laser pulses with a thin water flow results in an emission of a strong single-cycle THz pulse associated with enhanced soft X-ray emission. In this paper, a chain of processes produced in this interaction is analyzed and compared with other THz generation studies. It is demonstrated that the enhanced THz and X-ray emissions are produced by an energetic electron beam accelerated in the interaction of a main laser pulse with liquid water ejected from the surface by the pre-pulse. This scheme thus provides an efficient laser energy conversion in a THz pulse, avoiding laser self-focusing and filamentation in air.

Computational broadband imaging with laser-driven sequential light source arrays on a water film.

Imaging and computational processing fusion technologies have expanded the wavelength range that can be visualized. However, it is still challenging to realize a system that can image a wide range of wavelengths, including non-visible regions, in a single system. Here, we propose a broadband imaging system based on femtosecond-laser-driven sequential light source arrays. The light source arrays allow us to form ultra-broadband illumination light depending on the excitation target and irradiated pulse energy. We demonstrated X-ray and visible imaging under atmospheric pressure by using a water film as an excitation target. Furthermore, by applying a compressive sensing algorithm, the imaging time was reduced while maintaining the number of pixels in the reconstructed image.

Shockwave-based THz emission in air.

THz emission in air under the irradiation of a pair of tightly-focused femtosecond laser pulses (800nm, 35fs) with nanosecond time delay and micro-meter spatial offsets is studied with polarization-sensitive THz time-domain spectroscopy and time-resolved imaging. The pre-pulse irradiation induces air-breakdown at its focus, which results in the expansion of shockwave front traveling outward. When the main pulse irradiates such shockwave front far from the pre-pulse focus with nanosecond delay, THz emission intensity was enhanced up to ∼13-times and its linear polarization was aligned along the line between the two focus positions of the pre- and the main pulses which is parallel to the expansion direction of the shockwave front. Asymmetric density profiles of the shockwave fronts prepared by the pre-pulse irradiation define the polarization of THz emission. Mechanisms are discussed from the viewpoint of electron diffusion in such asymmetric density profiles.

Feasibility of using bimetallic Au-Ag nanoparticles for organic light-emitting devices.

Matching the resonant wavelength of plasmonic nanoparticles (NPs) and the emission band of organic materials is critical for achieving optimal plasmon-enhanced luminescence in organic light-emitting devices (OLEDs). However, the spectral matching is often unsatisfactory because the interior architecture of OLEDs limits the dimensions of the NPs to support the desired wavelength adjustment. In this article, we proposed a design strategy via AuxAg1-x alloy NPs to enable resonance tuning while preserving the size of the NP to suit the OLED design requirements. The bimetallic NPs, especially for x < 0.6, not only add one more degree of freedom to vary the plasmon wavelength but also provide the benefits of higher scattering and more intense and outspread electric fields over a broader spectrum compared to Au monometallic NPs. These features allow smaller NPs, which are more compatible with OLED interiors, to scatter electric fields more efficiently and increase the density of molecules interacting with the NP plasmons. In the presence of a nearby dipole emitter, the bimetallic NPs can simultaneously increase radiative enhancement and suppress non-radiative losses, which are advantageous for increasing the quantum yield and luminescence efficiency of the emitter. These improvements are associated with lower intraband and interband activities resulting from the higher molar fraction of Ag in the alloy NPs. We provided composition mappings to achieve enhanced luminescence for specified wavelengths at fixed NP sizes. Finally, we theoretically demonstrated that the bimetallic NPs could improve the light-extraction efficiency of OLEDs better than Au monometallic NPs. This work provides essential guidance to enable versatile plasmon-enhanced applications with predefined nanostructural geometries and wavelengths to match the device requirements.

Surface plasmon-enhanced solution-processed phosphorescent organic light-emitting diodes by incorporating gold nanoparticles.

Organic light-emitting diodes (OLEDs) have attracted increasing attention due to their superiority as high quality displays and energy-saving lighting. However, improving the efficiency of solution-processed devices especially based on blue emitter remains a challenge. Excitation of surface plasmons on metallic nanoparticles has potential for increasing the absorption and emission from optoelectronic devices. We demonstrate here that the incorporation of gold nano particles (GNPs) in the hole injection layer of poly(3,4-ethylene dioxythiophene):polystyrene sulfonic acid with an appropriate size and doping concentration can greatly enhance the efficiency OLED device especially at higher voltage. Apparently, the spectral of the multiple plasmon resonances of the GNPs and the luminescence of the emitting materials significantly overlap with each other. At 1000 cd m-2 for example, the power efficiency of a studied green device is increased from 29.0 to 36.2 lm W-1, an increment of 24.8%, and the maximum brightness improved from 21 550 to 27 810  cd m-2, an increment of 29.1%, as 2 wt% of a 12 nm GNP is incorporated. Remarkably, designed blue OLED also exhibited an increment of 50% and 35% in power efficacy at 100 and 1000 cd m-2, respectively, for same device structure. The reason why the enhancement is marked may be attributed to a strong absorption of the short-wavelength emission from the device by the gold nano particles, which in turn initiates a strong surface plasmon resonance effect, leading to a high device efficiency.

Enhancement of X-ray emission from nanocolloidal gold suspensions under double-pulse excitation.

Enhancement of X-ray emission was observed from a micro-jet of a nano-colloidal gold suspension in air under double-pulse excitation of ultrashort (40 fs) near-IR laser pulses. Temporal and spatial overlaps between the pre-pulse and the main pulse were optimized for the highest X-ray emission. The maximum X-ray intensity was obtained at a 1-7 ns delay of the main pulse irradiation after the pre-pulse irradiation with the micro-jet position shifted along the laser beam propagation. It was revealed that the volume around gold nanoparticles where the permittivity is near zero, ε ≈ 0, accounts for the strongest absorption, which leads to the effective enhancements of X-ray emission.

Dual THz Wave and X-ray Generation from a Water Film under Femtosecond Laser Excitation.

Simultaneous emission of the THz wave and hard X-ray from thin water free-flow was induced by the irradiation of tightly-focused femtosecond laser pulses (35 fs, 800 nm, 500 Hz) in air. Intensity measurements of the THz wave and X-ray were carried out at the same time with time-domain spectroscopy (TDS) based on electro-optic sampling with a ZnTe(110) crystal and a Geiger counter, respectively. Intensity profiles of the THz wave and X-ray emission as a function of the solution flow position along the incident laser axis at the laser focus show that the profile width of the THz wave is broader than that of the X-ray. Furthermore, the profiles of the THz wave measured in reflection and transmission directions show different features and indicate that THz wave emission is, under single-pulse excitation, induced mainly in laser-induced plasma on the water flow surface. Under double-pulse excitation with a time separation of 4.6 ns, 5⁻10 times enhancements of THz wave emission were observed. Such dual light sources can be used to characterise materials, as well as to reveal the sequence of material modifications under intense laser pulses.

Photoacoustic signal enhancements from gold nano-colloidal suspensions excited by a pair of time-delayed femtosecond pulses.

Photoacoustic signal enhancements were observed with a pair of time-delayed femtosecond pulses upon excitation of gold nanosphere colloidal suspension. A systematic experimental investigation of photoacoustic intensity within the delay time, Δt = 0 to 15 ns, was carried out. The results revealed a significant enhancement factor of ∼2 when the pre-pulse energy is 20-30% of the total energy. Pre-pulse and main pulse energy ratios, Ep(1):Es(2), were varied to determine the optimal ratio that yields to maximum photoacoustic signal enhancement. This enhancement was ascribed to the initial stage of thermalization and bubble generation in the nanosecond time scale. Pre-pulse scattering intensity measurements and numerical finite-difference time-domain calculations were performed to reveal dynamics and light field enchancement, respectively.

Dynamic position shifts of X-ray emission from a water film induced by a pair of time-delayed femtosecond laser pulses.

Femtosecond double-pulsed laser excitation of a water film in air showed enhancements of X-ray intensity as compared with single pulse irradiation. The position of the highest yield of X-rays strongly depends on temporal separation between the pre-pulse and the main-pulse (energy ratios where ∼ 1 : 10). The strongest X-ray emission was observed at 10-15 ns delay of the main-pulse. Nanoscale roughening of water surface can account for the observation.

Regenerated volume gratings in PMMA after femtosecond laser writing.

Self-regeneration of volume gratings recorded inside polymethyl methacrylate (PMMA) after 70-100 days is demonstrated. First, volume gratings were made inside PMMA by femtosecond laser writing. The diffraction efficiency of the gratings reached the maximum-was regenerated-following an initial slow decrease within the first several days after the fabrication. Time-lapse measurements of the diffraction efficiency in both top-plane (as laser written) and side-plane illumination were used to monitor changes of the diffraction efficiency. The final efficiency was reaching values well in excess of the as-fabricated efficiencies, with a maximum diffraction efficiency of 90% for the side readout illumination. The regenerated volume grating is a possible candidate to achieve high diffraction efficiency in PMMA. The regeneration is consistent with the α-relaxation of the polymer structure and oxidation of the dangling bonds.

Femtosecond laser-induced hard X-ray generation in air from a solution flow of Au nano-sphere suspension using an automatic positioning system.

Femtosecond laser-induced hard X-ray generation in air from a 100-µm-thick solution film of distilled water or Au nano-sphere suspension was carried out by using a newly-developed automatic positioning system with 1-µm precision. By positioning the solution film for the highest X-ray intensity, the optimum position shifted upstream as the laser power increased due to breakdown. Optimized positioning allowed us to control X-ray intensity with high fidelity. X-ray generation from Au nano-sphere suspension and distilled water showed different power scaling. Linear and nonlinear absorption mechanism are analyzed together with numerical modeling of light delivery.

Enhanced photoacoustics from gold nano-colloidal suspensions under femtosecond laser excitation.

Enhanced photoacoustic (PA) intensity from gold nanosphere and nanorod colloidal suspensions in water under tightly-focused femtosecond pulsed laser irradiation was systematically investigated. PA signal amplitudes were measured by ultrasound transducers at frequencies of 5, 10, and 25 MHz. The experimental results revealed a linear-dependence of the relative photoacoustic amplitude on the laser power and the mechanism was attributed to non-radiative relaxation dynamics of surface plasmon oscillations. When gold nanorod with longitudinal absorption/extinction peak at 800 nm coincides with the wavelength of femtosecond laser pulses, the most efficient PA signal is generated. Laser excitation was kept within a thermal stability region of gold nanoparticles, i.e., colloidal suspension can be continuously reused for PA generation.

MHz-ultrasound generation by chirped femtosecond laser pulses from gold nano-colloidal suspensions.

Strong absorption of femtosecond laser pulses in Au nano-colloidal suspensions was used to generate coherent ultrasound signals at 1-20 MHz frequency range. The most efficient ultrasound generation was observed at negative chirp values and was proportional to the pulse duration. Maximization of a dimensionless factor A ≡ αc0tp defined as the ratio of pulse duration tp and the time required for sound at speed c0 to cross the optical energy deposition length (an inverse of the absorption coefficient α) given by 1/(αc0). Chirp controlled pulse duration allows effective enhancement of ultrasound generation at higher frequencies (shorter wavelengths) and is promising for a high spatial resolution acoustic imaging.

Polarization-independent guided-mode resonance filter with cross-integrated waveguide resonators.

A cavity-resonator-integrated guided-mode resonance filter (CRIGF) has been proposed and investigated in order to realize high-efficiency narrowband reflection with a small aperture. The CRIGF consists of a grating coupler integrated in a cavity resonator constructed by a pair of distributed Bragg reflectors on a thin-film waveguide. This time, orthogonally crossed integration of two CRIGFs was demonstrated in order to obtain polarization-independent reflection spectrum. An SiO2-based device with 10 µm aperture was designed and fabricated for around 850 nm wavelength operation, and narrowband polarization-independent reflection was confirmed experimentally.

Cavity-resonator-integrated guided-mode resonance filter for aperture miniaturization.

A guided-mode resonance filter integrated in a waveguide cavity resonator constructed by two distributed Bragg reflectors is designed and fabricated for miniaturization of aperture size. Reflection efficiency of >90% and wavelength selectivity of 0.4 nm are predicted in the designed SiO(2)-based filter with 50-µm aperture by a numerical calculation using the finite-difference time-domain method. A maximum reflectance of 67% with 0.5-nm bandwidth is experimentally demonstrated by the fabricated device at around 850-nm wavelength.

Water expansion dynamics after pulsed IR laser heating.

A nanosecond pulsed IR (1.9 microm) laser rapidly heated water, in an open vessel, to temperatures well below the boiling point. The subsequent dynamics of volume expansion were monitored using time-resolved interferometry in order to measure the increase in the water level in the heated area. The water expanded at less than the speed of sound, taking just less than 100 ns to increase its height by approximately 500 nm at surface temperature jumps of 20 K. The initial expansion was followed by an apparent contraction and then a re-expansion. The first expansion phase occurred more slowly than the timescale for bulk H-bond re-structuring of the water, as determined from vibrational bands in the Raman spectra, and represents the limit to the rate at which the overpressure caused by sudden heating can be released. The second phase of the expansion was caused by hydrodynamic effects and is accompanied by morphological changes resulting in light scattering as well as droplet spallation.

Chirp effect in hard X-ray generation from liquid target when irradiated by femtosecond pulses.

The chirp effect on a X-ray emission intensity from a CsCl aqueous solution jet irradiated by femtosecond pulses was systematically studied. The p-polarized chirped pulses were more efficient as compared with the shortest pulses determined by the spectral bandwidth. The negatively-chirped pulses of approximately 240 fs duration produced up to 10 times larger X-ray intensity as compared with the transform-limited 160 fs pulses. The angular dependence of X-ray generation can be explained by the resonant absorption. Numerical simulations of electron density evolution due to the avalanche and multi-photon absorption supports qualitatively well the experimental observations.

Density changes accompanying wave propagation in the cerium-catalyzed Belousov-Zhabotinsky reaction.

Refractive index measurement using an interferometric imaging system and observation of chemical wave shapes were carried out during chemical wave propagation of a cerium-catalyzed Belousov-Zhabotinsky (BZ) reaction. Densities increased as chemical waves propagated in samples without NaBr, and decreased in samples with NaBr. Concentration changes of malonic acid, bromomalonic acid, and BrO3- were estimated from Raman spectral measurements in a stirred batch BZ reaction, and these also exhibited differences between samples with and without NaBr. It is proposed that a reaction subset yielding low molecular weight carboxylic acids is predominant in samples with NaBr, whereas a pathway leading to dibromoacetic acid or tribromoacetic acid production is the major process in samples without NaBr.

Dynamics of Re(2,2'-bipyridine)(CO)3Cl MLCT formation and decay after picosecond pulsed X-ray excitation and femtosecond UV excitation.

The dynamics of Re(2,2'-bipyridine)(CO)3Cl MLCT state formation and decay were determined after femtosecond UV laser excitation and picosecond pulsed X-ray excitation, in an N,N-dimethylformamide (DMF) solution as well as in its solid form. At room temperature, after UV excitation, this MLCT excited state emits both in DMF solution and in the solid form. Transient absorption spectra were measured in solution at various delay times following excitation by a 160 fs, 390 nm laser pulse. There was a prompt absorption increase at around 460 nm occurring within the pump probe convolution (<1 ps), which was assigned to the formation of the 3MLCT state. This transient absorbance was constant over 100 ps. In contrast to the solution state, in the solid state, the emission maximum slightly red-shifts with increasing time after laser excitation. In both solid and solution the emission rises within the system response time. The solid sample exhibited a 1.4 ns emission decay that was not observed for the solution sample. The emission rise from a solid sample after 20 ps pulsed X-ray excitation was significantly slower than the system's time resolution. It is proposed that kinetically energetic electrons are ejected following X-ray induced ionisation, creating ionised tracks in which energetic cations and electrons take time to recombine yielding delayed 3MLCT states that emit.