Time-resolved Emission Imaging Research Articles

Expansion Dynamic and Characterization of Stagnation Layer in Laterally Colliding Plasmas: Dependence of Observation Bandwidth and Plasma Plume Separation

The colliding laser-produced plasma (CLPP) has a wide range of applications in various contexts, that might start with astrophysical applications or pulsed laser deposition or Laser-Induced Breakdown Spectroscopy (LIBS), which is a powerful analytical technique for elemental analysis and material identification.In CLPP experiments, the stagnation layer might form at the interface region when two dense laser-induced plasmas collide, and the degree of stagnation can be diagnosed by the collisionality parameter that is used to determine what kind of interaction will take place, i.e., soft or hard stagnation.Our experimental work presents the results of the temporal, spatial and semi-spectrally imaging of colliding plasmas of aluminium and silicon targets. The analysis is focused on describing the velocity of the expanding plasma front for the interaction zone. The aim of the work presented here is to further advance and study colliding plasma techniques, as well as other methods to realize and control species density and expansion, with a view to a deep understanding of these complex mechanisms and optimising emission in the visible wavelength range.All investigation sequences were based on a similar experimental setup, where two different focusing lenses were used with an effective focal length (EFL) of approx. 100mm or 125mm to achieve seed separation around 1.66mm or 2.16mm, respectively. Time-resolved emission imaging was employed to track the stagnation layer‛s size and shape, which might act as a signature of hard versus soft stagnation.The study provides a considerable amount of detailed data related to the expansion velocity of the interaction zone which extends the understanding of the behaviour of particular species within colliding laser-produced plasmas.

Influence of surface roughness on nanosecond laser-induced shock wave enhancement effects.

In this paper, an effective method is proposed for improving the energy of the shock waves that are generated by plasma expanding outward and colliding with another gas. Silicon targets are used as the response medium with roughness of 2.3 nm, 457.8 nm, 1.1 µm, and 37.1 µm, respectively. A 532-nm-laser with a pulse duration of 8 ns and a repetition rate of 10 Hz is used as the irradiation source. An intensified charge-coupled device (ICCD) is used to photograph the morphology of the shock waves. The time-resolved emission images of silicon plasma plumes are observed between 20-200 ns. As the surface roughness of the target increases, the intensity of the shock wave gradually increases, and the energy of the shock wave reaches up to 39.45 mJ at a roughness of 37.1 µm.

Mechanisms of graphite ablation by sub-millisecond ytterbium fiber laser pulses

Graphite is a key material in a variety of cross-cutting applications in energy conversion, energy storage, and nuclear energy. Recently, temporally modulated continuous wave lasers have been shown to produce well-defined ablation features in graphite at relatively high processing speeds. In this work, we analyze in detail the laser ablation dynamics of single-pulse ablation in the sub-millisecond time regime to elucidate the origins of the resulting well-defined ablation craters using a combination of time-resolved emission imaging, diffuse reflection/scattering imaging, and optical emission spectroscopy. These multimodal in situ diagnostics revealed three main contributors to achieve well-defined ablation features: (1) rapid ejection of particles with ∼100 m/s speed, (2) ablation of the graphite in the gaseous form, and (3) absence of bulk liquid motion, which is typically observed in laser processing of metals. Plasma plume formation was sustained throughout the duration of the laser pulse (500 μs). This work provides insights into the complex physical and chemical mechanisms of sub-millisecond laser–matter interactions, which are critical for parameter space optimization and tailoring of laser machining and drilling processes.

Long-lived metal complexes open up microsecond lifetime imaging microscopy under multiphoton excitation: from FLIM to PLIM and beyond

Lifetime imaging microscopy with sub-micron resolution provides essential understanding of living systems by allowing both the visualisation of their structure, and the sensing of bio-relevant analytes in vivo using external probes. Chemistry is pivotal for the development of the next generation of bio-tools, where contrast, sensitivity, and molecular specificity facilitate observation of processes fundamental to life. A fundamental limitation at present is the nanosecond lifetime of conventional fluorescent probes which typically confines the sensitivity to sub-nanosecond changes, whilst nanosecond background autofluorescence compromises the contrast. High-resolution visualization with complete background rejection and simultaneous mapping of bio-relevant analytes including oxygen – with sensitivity orders of magnitude higher than that currently attainable – can be achieved using time-resolved emission imaging microscopy (TREM) in conjunction with probes with microsecond (or longer) lifetimes. Yet the microsecond timescale has so far been incompatible with available multiphoton excitation/detection technologies. Here we realize for the first time microsecond-imaging with multiphoton excitation whilst maintaining the essential sub-micron spatial resolution. The new method is background-free and expands available imaging and sensing timescales 1000-fold. Exploiting the first engineered water-soluble member of a family of remarkably emissive platinum-based, microsecond-lived probes amongst others, we demonstrate (i) the first instance of background-free multiphoton-excited microsecond depth imaging of live cells and histological tissues, (ii) over an order-of-magnitude variation in the probe lifetime in vivo in response to the local microenvironment. The concept of two-photon TREM can be seen as “FLIM + PLIM” as it can be used on any timescale, from ultrafast fluorescence of organic molecules to slower emission of transition metal complexes or lanthanides/actinides, and combinations thereof. It brings together transition metal complexes as versatile emissive probes with the new multiphoton-excitation/microsecond-detection approach to create a transformative framework for multiphoton imaging and sensing across biological, medicinal and material sciences.

Stagnation layers at the collision front between two laser-induced plasmas: A study using time-resolved imaging and spectroscopy

When two dense laser-induced plasmas collide a stagnation layer may form at the interface region. The degree of stagnation depends on the so-called collisionality parameter given by the ratio of the geometric scale length of the experiment (in effect the initial plasma–plasma separation) to the ion–ion mean free path. Our experiments confirm that both target geometry and elemental composition strongly influence the collision process and degree of stagnation. In particular, we show that moving from flat to wedge-shaped targets and from aluminium to calcium results in a decrease in the value of the collisionality parameter accompanied by a concomitant reduction in the degree of stagnation. Time-resolved emission imaging was employed to track the size and shape of the stagnation layer which acts as a signature of hard versus soft stagnation. Characterization of the stagnation layer in terms of electron density and temperature has been performed using optical emission spectroscopy.

The time domain in co-stained cell imaging: time-resolved emission imaging microscopy using a protonatable luminescent iridium complex

The intense luminescence of the new complex Ir(ppy)(2)(pybz) (1) within the cytoplasm of live cells can be discriminated from the fluorescence of an organic stain, solely on the basis of the emission timescale {pybzH = 2-pyridyl-benzimidazole}. The protonated form of 1 displays red-shifted emission, and may be implicated in a superior uptake compared to Ir(ppy)(3).

Time-resolved and two-photon emission imaging microscopy of live cells with inert platinum complexes

This work explores time-resolved emission imaging microscopy (TREM) for noninvasive imaging and mapping of live cells on a hitherto uncharted microsecond time scale. Simple robust molecules for this purpose have long been sought. We have developed highly emissive, synthetically versatile, and photostable platinum(II) complexes that make TREM a practicable reality. [PtLCl], {HL = 1,3-di(2-pyridyl)benzene and derivatives}, are charge-neutral, small molecules that have low cytotoxicity and accumulate intracellularly within a remarkably short incubation time of 5 min, apparently under diffusion control. Their microsecond lifetimes and emission quantum yields of up to 70% are exceptionally high for transition metal complexes and permit the application of TREM to be demonstrated in a range of live cell types-normal human dermal fibroblast, neoplastic C8161 and CHO cells. [PtLCl] are thus likely to be suitable emission labels for any eukaryotic cell types. The high photostability of [PtLCl] under intense prolonged irradiation has allowed the development of tissue-friendly NIR two-photon excitation (TPE) in conjunction with transition metal complexes in live cells. A combination of confocal one-photon excitation, nonlinear TPE, and microsecond time-resolved imaging has revealed (i) preferential localization of the complexes to intracellular nucleic acid structures, in particular the nucleoli and (ii) the possibility of measuring intracellular emission lifetimes in the microsecond range. The combination of TREM, TPE, and Pt(II) complexes will be a powerful tool for investigating intracellular processes in vivo, because the long lifetimes allow discrimination from autofluorescence and open up the use of commonplace technology.

Femtosecond laser ablation induced plasma characteristics from submicron craters in thin metal film

The ablation-induced plasma physics at reduced ablation crater dimensions is experimentally investigated. Frequency doubled femtosecond laser pulses are tightly focused through objective lenses onto a Cr thin film coated on quartz wafer in order to obtain ablation craters of submicron lateral dimensions. Side-view time-resolved emission images and the corresponding spectra depict the detailed plasma evolution at the fluence range near the ablation threshold. Collected emission spectra at the laser fluence level of around two to three times of ablation threshold display characteristic atomic transition peaks of the ablated Cr material from submicron ablation craters. This finding confirms that improved spatial resolution for laser-induced breakdown spectroscopy can be achieved.

Optical near-field ablation-induced plasma characteristics

The physics of optical near-field based laser ablation plasmas is studied. A Cr thin metal film is ablated using visible nanosecond laser pulses coupled through an optical near-field fiber probe. The ablated plasma evolution is monitored via time-resolved emission imaging and spectral measurement. Intense plasma formed in the proximity of the near-field gap within the laser pulse duration and decayed after several nanoseconds. Highly directional jetlike material ejection was observed at later time scales. The measured spectra reveal that early stage plasma of short lifetime yields ablated material characteristic emission peaks, supporting possible application to laser-induced breakdown spectroscopy.

Pre-breakdown light emission phenomena in low-pressure argon between parabolic electrodes

An experimental study on pre-breakdown light emission in low-pressure argon gas was performed. In a pulsed discharge, pre-breakdown phenomena were observed for repetition rates between 100 and 2000 Hz and pulse duration of 100 µs. These phenomena were studied with time-resolved emission imaging using an intensified charge coupled device camera. The origin of the pre-breakdown emission was identified as diffusion of volume charges left over from previous discharges. These charges were accelerated towards the anode in small electron avalanches causing excitation of argon atoms. Different spatial distributions of the pre-breakdown light emission for different times between discharges were measured and the effects of the pre-breakdown phenomena on the main breakdown phase were studied using a double voltage pulse. The observed effects were attributed to the distribution of volume charges, left over from previous discharges, in the discharge gap during the pre-breakdown phase.

Influence of Gas Sampling on Analyte Transport within the ICP and Ion Sampling for ICP-MS Studied Using Individual, Isolated Sample Droplets

The effect of gas flow entrainment on the gas sampling, ion sampling, and ion detection processes in inductively coupled plasma mass spectrometry (ICP-MS) has been investigated. Isolated, single droplets of sample from a monodisperse dried microparticulate injector (MDMI) were used in conjunction with time-resolved ICP-MS, photographs of ion cloud movement, and time-gated imaging using a gateable, intensified charge-coupled device (ICCD) detector mounted on an imaging spectrometer. The results indicate that gas flow entrainment into the sampling orifice can have a significant effect on the plasma gas velocities as far as 7 mm from the sampling orifice. The effects are most pronounced within 3 mm of the sampling orifice. The trends in these results are consistent with theoretical calculations. Photographic images show that plasma gas initially as far as 3 mm off axis adopts a curved path into the sampling orifice. Time-resolved emission images of Sr+ ion clouds approaching the sampling orifice demonstrate the entrainment process and significant distortion of the ion cloud as it flows into the sampling orifice. Spatial maps of La+ ICP-MS signals were acquired as a function of distance from the vaporization point and distance from the plasma axis. The results suggest that gas entrainment has a significant effect on the spatial path of ions in the plasma and that accurate radially resolved spatial mapping of plasmas using mass spectrometry may not be possible. The widths of radially resolved La+ ICP-MS signal peaks do not change significantly when ions are sampled 2 mm from the vaporization point compared to 5 mm away. In contrast, ICP-MS signals measured on axis as a function of time clearly show broadening due to diffusion. These observations suggest that some detected ions may have originated from off-axis locations in the plasma.