Development of a fast laser ablation-inductively coupled plasma-mass spectrometry cell for sub-μm scanning of layered materials

Malderen, Stijn J. M. Van; Elteren, Johannes T. van; Vanhaecke, Frank

doi:10.1039/c4ja00137k

Cited by 91 publications

(85 citation statements)

References 45 publications

(53 reference statements)

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“…Moreover, some dyes interfere with biological processes, are only sensitive to the free unbound metal ion, or additionally to other elements than the one under consideration [13–16]. Other trace level analytical techniques such as inductively coupled plasma mass spectrometry (ICP-MS) are powerful in terms of sensitivity, but in case of liquid analysis isolation procedures of target elements are prone to contamination and by using laser ablation systems spatial resolution is restricted to the single micrometer level [17]. Synchrotron radiation induced X-ray fluorescence distinguishes itself due to (ultra) trace level sensitivity (down to 100 ppb in imaging mode) with superior sub-micrometer resolution (currently at the 10 nm scale), deep penetrating nature, low susceptibility for contaminations and non-destructive character.…”

Section: Introductionmentioning

confidence: 99%

Probing Intracellular Element Concentration Changes during Neutrophil Extracellular Trap Formation Using Synchrotron Radiation Based X-Ray Fluorescence

et al. 2016

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High pressure frozen (HPF), cryo-substituted microtome sections of 2 μm thickness containing human neutrophils (white blood cells) were analyzed using synchrotron radiation based X-ray fluorescence (SR nano-XRF) at a spatial resolution of 50 nm. Besides neutrophils from a control culture, we also analyzed neutrophils stimulated for 1–2 h with phorbol myristate acetate (PMA), a substance inducing the formation of so-called Neutrophil Extracellular Traps (or NETs), a defense system again pathogens possibly involving proteins with metal chelating properties. In order to gain insight in metal transport during this process, precise local evaluation of elemental content was performed reaching limits of detection (LODs) of 1 ppb. Mean weight fractions within entire neutrophils, their nuclei and cytoplasms were determined for the three main elements P, S and Cl, but also for the 12 following trace elements: K, Ca, Mn, Fe, Co, Ni, Cu, Zn, Se, Br, Sr and Pb. Statistical analysis, including linear regression provided objective analysis and a measure for concentration changes. The nearly linear Ca and Cl concentration changes in neutrophils could be explained by already known phenomena such as the induction of Ca channels and the uptake of Cl under activation of NET forming neutrophils. Linear concentration changes were also found for P, S, K, Mn, Fe, Co and Se. The observed linear concentration increase for Mn could be related to scavenging of this metal from the pathogen by means of the neutrophil protein calprotectin, whereas the concentration increase of Se may be related to its antioxidant function protecting neutrophils from the reactive oxygen species they produce against pathogens. We emphasize synchrotron radiation based nanoscopic X-ray fluorescence as an enabling analytical technique to study changing (trace) element concentrations throughout cellular processes, provided accurate sample preparation and data-analysis.

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Section: Introductionmentioning

confidence: 99%

Probing Intracellular Element Concentration Changes during Neutrophil Extracellular Trap Formation Using Synchrotron Radiation Based X-Ray Fluorescence

et al. 2016

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“…In Figure 5b, the signal at time 5.47 s clearly contains contributions from both the pyrite and clay domains; this pixel can neither be identified as pyrite or clay but suggests that signals from features below the 1.5-μm spot size used here might be resolvable if a smaller LA spot was used. A possible method to overcome the laser-spot-size resolution limit would be to overlap adjacent LA spots and deconvolute signal intensities, as recently described by Van Malderen et al 29 In Figure 6, we emphasize the information gained with improved LA-ICPMS imaging lateral resolutions by directly comparing the same section of Seymchan pallasite meteorite, which was imaged first with a matrix of 42-μm diameter laser shots and then with 10-μm spots. In both cases, LA was performed at a laser repetition rate of 20 Hz and complete washout was achieved between laser shots so that pulse-topulse mixing did not degrade lateral resolution.…”

Section: Analytical Chemistrymentioning

confidence: 98%

High-Speed, High-Resolution, Multielemental Laser Ablation-Inductively Coupled Plasma-Time-of-Flight Mass Spectrometry Imaging: Part I. Instrumentation and Two-Dimensional Imaging of Geological Samples

et al. 2015

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Low-dispersion laser ablation (LA) has been combined with inductively coupled plasma-time-of-flight mass spectrometry (ICP-TOFMS) to provide full-spectrum elemental imaging at high lateral resolution and fast image-acquisition speeds. The low-dispersion LA cell reported here is capable of delivering 99% of the total LA signal within 9 ms, and the prototype TOFMS instrument enables simultaneous and representative determination of all elemental ions from these fast-transient ablation events. This fast ablated-aerosol transport eliminates the effects of pulse-to-pulse mixing at laser-pulse repetition rates up to 100 Hz. Additionally, by boosting the instantaneous concentration of LA aerosol into the ICP with the use of a low-dispersion ablation cell, signal-to-noise (S/N) ratios, and thus limits of detection (LODs), are improved for all measured isotopes; the lowest LODs are in the single digit parts per million for single-shot LA signal from a 10-μm diameter laser spot. Significantly, high-sensitivity, multielemental and single-shot-resolved detection enables the use of small LA spot sizes to improve lateral resolution and the development of single-shot quantitative imaging, while also maintaining fast image-acquisition speeds. Here, we demonstrate simultaneous elemental imaging of major and minor constituents in an Opalinus clay-rock sample at a 1.5 μm laser-spot diameter and quantitative imaging of a multidomain Pallasite meteorite at a 10 μm LA-spot size.

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“…A custom-built ablation cell assembly described elsewhere 33 was mounted inside an Analyte G2 (Teledyne CETAC Technologies, Omaha, USA) 193 nm ArF* excimer laser ablation system (pulse duration <5 ns, 1% energy Figure 3. The central zone from which the surface roughness data were extracted features a 4-fold larger ablation area than displayed in Figure 3.…”

Section: ■ Experimental Sectionmentioning

confidence: 99%

Submicrometer Imaging by Laser Ablation-Inductively Coupled Plasma Mass Spectrometry via Signal and Image Deconvolution Approaches

2015

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In this work, pre- and postacquisition procedures for enhancing the lateral resolution of laser ablation-inductively coupled plasma mass spectrometry (LA-ICPMS) in two- and three-dimensional (2D, 3D) nuclide distribution mapping beyond the laser beam waist are described. 2D images were constructed by projecting a rectangular grid of discrete LA positions, arranged at interspacings smaller than the dimensions of the laser beam waist, onto the sample surface, thus oversampling the region of interest and producing a 2D image convolved in the spatial domain. The pulse response peaks of a low-dispersion LA cell were isolated via signal deconvolution of the transient mass analyzer response. A 3D stack of 2D images was deconvolved by an iterative Richardson-Lucy algorithm with Total Variance regularization, enabling submicrometer image fidelity, demonstrated in the analysis of trace level features in corroded glass. A point spread function (PSF) could be derived from topography maps of single pulse craters from atomic force microscopy. This experimental PSF allows the approach to take into account the laser beam shape, beam aberrations, and the laser-solid interaction, which in turn enhances the spatial resolution of the reconstructed volume.

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Development of a fast laser ablation-inductively coupled plasma-mass spectrometry cell for sub-μm scanning of layered materials

Cited by 91 publications

References 45 publications

Probing Intracellular Element Concentration Changes during Neutrophil Extracellular Trap Formation Using Synchrotron Radiation Based X-Ray Fluorescence

Probing Intracellular Element Concentration Changes during Neutrophil Extracellular Trap Formation Using Synchrotron Radiation Based X-Ray Fluorescence

High-Speed, High-Resolution, Multielemental Laser Ablation-Inductively Coupled Plasma-Time-of-Flight Mass Spectrometry Imaging: Part I. Instrumentation and Two-Dimensional Imaging of Geological Samples

Submicrometer Imaging by Laser Ablation-Inductively Coupled Plasma Mass Spectrometry via Signal and Image Deconvolution Approaches

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