title: 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.
abstract: 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.
authors.affiliation: †Laboratory of Inorganic Chemistry, ETH Zurich, Vladimir-Prelog-Weg 1, CH-8093 Zurich, Switzerland.
authors.forename: Alexander
authors.initials: A
authors.lastname: Gundlach-Graham
authors.affiliation: †Laboratory of Inorganic Chemistry, ETH Zurich, Vladimir-Prelog-Weg 1, CH-8093 Zurich, Switzerland.
authors.forename: Marcel
authors.initials: M
authors.lastname: Burger
authors.affiliation: †Laboratory of Inorganic Chemistry, ETH Zurich, Vladimir-Prelog-Weg 1, CH-8093 Zurich, Switzerland.
authors.forename: Steffen
authors.initials: S
authors.lastname: Allner
authors.affiliation: †Laboratory of Inorganic Chemistry, ETH Zurich, Vladimir-Prelog-Weg 1, CH-8093 Zurich, Switzerland.
authors.forename: Gunnar
authors.initials: G
authors.lastname: Schwarz
authors.affiliation: †Laboratory of Inorganic Chemistry, ETH Zurich, Vladimir-Prelog-Weg 1, CH-8093 Zurich, Switzerland.
authors.forename: Hao A O
authors.initials: HA
authors.lastname: Wang
authors.affiliation: †Laboratory of Inorganic Chemistry, ETH Zurich, Vladimir-Prelog-Weg 1, CH-8093 Zurich, Switzerland.
authors.forename: Luzia
authors.initials: L
authors.lastname: Gyr
authors.affiliation: ‡microXAS Beamline Project, Swiss Light Source, Paul Scherrer Institute, 5232 Villigen PSI, Switzerland.
authors.forename: Daniel
authors.initials: D
authors.lastname: Grolimund
authors.affiliation: †Laboratory of Inorganic Chemistry, ETH Zurich, Vladimir-Prelog-Weg 1, CH-8093 Zurich, Switzerland.
authors.forename: Bodo
authors.initials: B
authors.lastname: Hattendorf
authors.affiliation: †Laboratory of Inorganic Chemistry, ETH Zurich, Vladimir-Prelog-Weg 1, CH-8093 Zurich, Switzerland.
authors.forename: Detlef
authors.initials: D
authors.lastname: Günther