High-resolution single pulse LA-ICP-MS mapping via 2D sub-pixel oversampling on orthogonal and hexagonal ablation grids – A computational assessment

Laser beam profiles in analytical laser ablation – inductively coupled plasma – mass spectrometry (LA-ICP-MS) instruments are in general homogenized to produce a flat-top beam profile. However, in practice, they are mostly super-Gaussian in nature, and for small laser beam sizes (

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Veröffentlicht in:Talanta (Oxford) 2023-10, Vol.263, p.124699-124699, Article 124699
Hauptverfasser: Metarapi, Dino, van Elteren, Johannes T.
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description Laser beam profiles in analytical laser ablation – inductively coupled plasma – mass spectrometry (LA-ICP-MS) instruments are in general homogenized to produce a flat-top beam profile. However, in practice, they are mostly super-Gaussian in nature, and for small laser beam sizes (
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However, in practice, they are mostly super-Gaussian in nature, and for small laser beam sizes (&lt;5 μm) they even approach a Gaussian profile. This implies that the amount of surface material sampled by the laser (=ablation volume) directly depends on the beam profile and ablation grid. By contraction of the ablation grid (=sub-pixel mapping) not only more accurate surface sampling is realized, but also a higher pixel density, an improved spatial resolution, and a better signal-to-noise ratio. Although LA sampling is predominantly performed on an orthogonal grid, hexagonal or staggered/interleaved sampling may further improve the image quality as regular hexagons are more compact than squares (=lower perimeter/area) and suffer less from orientation bias (=lower anisotropy). Due to the current limitations of LA stages in executing precise hexagonal sampling with small beam sizes, computational protocols were employed to simulate LA-ICP-MS mapping. Simulation was performed by discrete convolution using the crater profile as the kernel, followed by the application/addition of Poisson/Flicker noise related to the local concentration and instrumental sensitivity/noise. A freely accessible online app was developed (https://laicpms-apps.ki.si/webapps/home/) to study the effect of sampling grid contraction (orthogonal and hexagonal) on the image map quality (spatial resolution and signal-to-noise ratio) by virtual ablation of phantoms. Comparison of experimental LA-ICP-MS maps obtained through orthogonal and hexagonal sampling methods could only be performed using a beam size of 150 μm and a macroscale inkjet-printed resolution target. This was due to the unavailability of precise hexagonal sampling stages and microscale resolution targets, which prevented the use of smaller beam sizes. [Display omitted] •Laser ablation crater morphologies are generally not cuboidal or cylindrical.•Closer packing of round/square ablation spots is best done hexagonally/orthogonally.•This offers more accurate surface sampling by reducing “sampling holes”.•Ablation grid contraction also yields higher spatial resolution and reduction of noise.•Implementation in imaging techniques like LA-ICP-MS would offer better image quality.</description><identifier>ISSN: 0039-9140</identifier><identifier>EISSN: 1873-3573</identifier><identifier>DOI: 10.1016/j.talanta.2023.124699</identifier><identifier>PMID: 37267882</identifier><language>eng</language><publisher>Netherlands: Elsevier B.V</publisher><subject>Chirp resolution target ; Contrast-detail diagram ; Hexagonal lattice ; Hexagons ; Simulation ; Visual acuity</subject><ispartof>Talanta (Oxford), 2023-10, Vol.263, p.124699-124699, Article 124699</ispartof><rights>2023 The Authors</rights><rights>Copyright © 2023 The Authors. 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[Display omitted] •Laser ablation crater morphologies are generally not cuboidal or cylindrical.•Closer packing of round/square ablation spots is best done hexagonally/orthogonally.•This offers more accurate surface sampling by reducing “sampling holes”.•Ablation grid contraction also yields higher spatial resolution and reduction of noise.•Implementation in imaging techniques like LA-ICP-MS would offer better image quality.</description><subject>Chirp resolution target</subject><subject>Contrast-detail diagram</subject><subject>Hexagonal lattice</subject><subject>Hexagons</subject><subject>Simulation</subject><subject>Visual acuity</subject><issn>0039-9140</issn><issn>1873-3573</issn><fulltext>true</fulltext><rsrctype>article</rsrctype><creationdate>2023</creationdate><recordtype>article</recordtype><recordid>eNqFkcuOEzEQRS0EYsLAJ4C8ZOPgRz_sFYrCY0YKAglYW3Z3JXHkbje2Oxp2_AMSH8iX4EwCW1Z-1Ll17boIPWd0yShrXh2W2XgzZrPklIsl41Wj1AO0YLIVRNSteIgWlApFFKvoFXqS0oHSQlLxGF2JljetlHyBft243Z5ESMHP2YURJzfuPOBp9gnwZkVu15_Ih894MNNUKvjoDOZvcJotmdwdeByOEJMZJn-qFn2IeR92YTQem7HHe7gzl5P15t5hF12f8O8fP_EKd2GY5nx_f0JSgpQGGPNT9GhrygueXdZr9PXd2y_rG7L5-P52vdqQrmI8k1q2lBvbt1uQjWBKdkbIuuG26qmAulKgrBWclp3qm1qxbV2m0VolhFG2qcU1ennuO8XwbYaU9eBSB75MFsKcNJeci1YqKQpan9EuhpQibPUU3WDid82oPkWiD_oSiT5Fos-RFN2Li8VsB-j_qf5mUIDXZwDKR48Ook6dg7GD3kXosu6D-4_FHzNvoZY</recordid><startdate>20231001</startdate><enddate>20231001</enddate><creator>Metarapi, Dino</creator><creator>van Elteren, Johannes T.</creator><general>Elsevier B.V</general><scope>6I.</scope><scope>AAFTH</scope><scope>NPM</scope><scope>AAYXX</scope><scope>CITATION</scope><scope>7X8</scope><orcidid>https://orcid.org/0000-0003-2237-7821</orcidid></search><sort><creationdate>20231001</creationdate><title>High-resolution single pulse LA-ICP-MS mapping via 2D sub-pixel oversampling on orthogonal and hexagonal ablation grids – A computational assessment</title><author>Metarapi, Dino ; van Elteren, Johannes T.</author></sort><facets><frbrtype>5</frbrtype><frbrgroupid>cdi_FETCH-LOGICAL-c412t-58702abd7fe863198ca38562b4d03e549e9bb3205499d6591f51407b933a9b653</frbrgroupid><rsrctype>articles</rsrctype><prefilter>articles</prefilter><language>eng</language><creationdate>2023</creationdate><topic>Chirp resolution target</topic><topic>Contrast-detail diagram</topic><topic>Hexagonal lattice</topic><topic>Hexagons</topic><topic>Simulation</topic><topic>Visual acuity</topic><toplevel>peer_reviewed</toplevel><toplevel>online_resources</toplevel><creatorcontrib>Metarapi, Dino</creatorcontrib><creatorcontrib>van Elteren, Johannes T.</creatorcontrib><collection>ScienceDirect Open Access Titles</collection><collection>Elsevier:ScienceDirect:Open Access</collection><collection>PubMed</collection><collection>CrossRef</collection><collection>MEDLINE - Academic</collection><jtitle>Talanta (Oxford)</jtitle></facets><delivery><delcategory>Remote Search Resource</delcategory><fulltext>fulltext</fulltext></delivery><addata><au>Metarapi, Dino</au><au>van Elteren, Johannes T.</au><format>journal</format><genre>article</genre><ristype>JOUR</ristype><atitle>High-resolution single pulse LA-ICP-MS mapping via 2D sub-pixel oversampling on orthogonal and hexagonal ablation grids – A computational assessment</atitle><jtitle>Talanta (Oxford)</jtitle><addtitle>Talanta</addtitle><date>2023-10-01</date><risdate>2023</risdate><volume>263</volume><spage>124699</spage><epage>124699</epage><pages>124699-124699</pages><artnum>124699</artnum><issn>0039-9140</issn><eissn>1873-3573</eissn><abstract>Laser beam profiles in analytical laser ablation – inductively coupled plasma – mass spectrometry (LA-ICP-MS) instruments are in general homogenized to produce a flat-top beam profile. However, in practice, they are mostly super-Gaussian in nature, and for small laser beam sizes (&lt;5 μm) they even approach a Gaussian profile. This implies that the amount of surface material sampled by the laser (=ablation volume) directly depends on the beam profile and ablation grid. By contraction of the ablation grid (=sub-pixel mapping) not only more accurate surface sampling is realized, but also a higher pixel density, an improved spatial resolution, and a better signal-to-noise ratio. Although LA sampling is predominantly performed on an orthogonal grid, hexagonal or staggered/interleaved sampling may further improve the image quality as regular hexagons are more compact than squares (=lower perimeter/area) and suffer less from orientation bias (=lower anisotropy). Due to the current limitations of LA stages in executing precise hexagonal sampling with small beam sizes, computational protocols were employed to simulate LA-ICP-MS mapping. Simulation was performed by discrete convolution using the crater profile as the kernel, followed by the application/addition of Poisson/Flicker noise related to the local concentration and instrumental sensitivity/noise. A freely accessible online app was developed (https://laicpms-apps.ki.si/webapps/home/) to study the effect of sampling grid contraction (orthogonal and hexagonal) on the image map quality (spatial resolution and signal-to-noise ratio) by virtual ablation of phantoms. Comparison of experimental LA-ICP-MS maps obtained through orthogonal and hexagonal sampling methods could only be performed using a beam size of 150 μm and a macroscale inkjet-printed resolution target. This was due to the unavailability of precise hexagonal sampling stages and microscale resolution targets, which prevented the use of smaller beam sizes. [Display omitted] •Laser ablation crater morphologies are generally not cuboidal or cylindrical.•Closer packing of round/square ablation spots is best done hexagonally/orthogonally.•This offers more accurate surface sampling by reducing “sampling holes”.•Ablation grid contraction also yields higher spatial resolution and reduction of noise.•Implementation in imaging techniques like LA-ICP-MS would offer better image quality.</abstract><cop>Netherlands</cop><pub>Elsevier B.V</pub><pmid>37267882</pmid><doi>10.1016/j.talanta.2023.124699</doi><tpages>1</tpages><orcidid>https://orcid.org/0000-0003-2237-7821</orcidid><oa>free_for_read</oa></addata></record>
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subjects Chirp resolution target
Contrast-detail diagram
Hexagonal lattice
Hexagons
Simulation
Visual acuity
title High-resolution single pulse LA-ICP-MS mapping via 2D sub-pixel oversampling on orthogonal and hexagonal ablation grids – A computational assessment
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