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Imaging Spectrometry


261

Author(s): Zoriy, MV (Zoriy, Myroslav V.); Dehnhardt, M (Dehnhardt, Markus); Matusch, A (Matusch, Andreas); Becker, JS (Becker, J. Sabine)

Title: Comparative imaging of P, S, Fe, Cu, Zn and C in thin sections of rat brain tumor as well as control tissues by laser ablation inductively coupled plasma mass spectrometry

Source: SPECTROCHIMICA ACTA PART B-ATOMIC SPECTROSCOPY, 63 (3): 375-382 MAR 2008

Abstract:

Laser ablation inductively coupled plasma mass spectrometry (LA-ICP-MS) was used for quantitative imaging of selected elements (P, S, Fe, Cu, Zn and C) in thin sections of rat brain samples (thickness 20 pm). The sample surface was scanned (raster area similar to 2 cm(2)) with a focused laser beam (wavelength 266 nm, diameter of laser crater 50 mu m, and irradiance X 10(9) W cm(-2)). The laser ablation system was coupled to a doublefocusing sector field. The possibility was evaluated of using carbon (via measurement of C-13(+)) as an internal standard element for imaging element distribution as part of this method. The LA-ICP-MS images obtained for P, S, Fe Cu and Zn were quantified using synthetically prepared matrixmatched laboratory standards. Depending on the sample analyzed, concentrations of Cu and Zn in the control, tissue were found to be in the range of 8-10 mu g g(-1) and 10-12 mu g g(-1), while in the tumor tissue these concentrations were in the range of 12-15 mu g g(-1) and 15-17 mu g g(-1) respectively. The measurements of P, S and Fe distribution revealed the depletion of these elements in tumor tissue. In all the samples, the shape of the tumor could be clearly distinguished from the surrounding healthy tissue by the depletion in carbon. Additional experiments were performed in order to study the influence of the water content of the analyzed tissue on the intensity signal of the analyte. The results of these measurements show the linear correlation (R-2 = 0.9604) between the intensity of analyte and amount of water in the sample. The growth of a brain tumor was thus studied for the first time by imaging mass spectrometry. (c) 2008 Published by Elsevier B.V.


Addresses: Res Ctr, Cent Div Anal Chem, D-52425 Julich, Germany

Res Ctr, Inst Med, D-52425 Julich, Germany

Reprint Address: BECKER, JS, RES CTR, CENT DIV ANAL CHEM, D-52425 JULICH, GERMANY

Author's E-mail: s.becker@fz-juelich.de

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262


Author(s): Wiseman, JM (Wiseman, Justin M.); Ifa, DR (Ifa, Demian R.); Cooks, RG (Cooks, R. Graham); Venter, A (Venter, Andre)

Title: Ambient molecular imaging by desorption electrospray ionization mass spectrometry

Source: NATURE PROTOCOLS, 3 (3): 517-524 2008

Abstract:

Desorption electrospray ionization (DESI) allows the direct analysis of ordinary objects or pre-processed samples under ambient conditions. Among other applications, DESI is used to identify and record spatial distributions of lipids and drug molecules in biological tissue sections. This technique does not require sample preparation other than production of microtome tissue slices and does not involve the use of ionization matrices. This greatly simplifies the procedure and prevents the redistribution of analytes during matrix deposition. Images are obtained by continuously moving the sample relative to the DESI sprayer and the inlet of the mass spectrometer. The timing of the protocol depends on the size of the surface to be analyzed and on the desired resolution. Analysis of organ tissue slices at 250 mu m resolution typically takes between 30 min and 2 h.
Addresses: Purdue Univ, Dept Chem, W Lafayette, IN 47907 USA

Reprint Address: COOKS, RG, PURDUE UNIV, DEPT CHEM, W LAFAYETTE, IN 47907 USA

Author's E-mail: cooks@purdue.edu

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263

Author(s): Vaidyanathan, S (Vaidyanathan, Seethararnan); Fietcher, JS (Fietcher, John S.); Goodacre, R (Goodacre, Roy); Lockyer, NP (Lockyer, Nicholas P.); Micklefield, J (Micklefield, Jason); Vickerman, JC (Vickerman, John C.)



Title: Subsurface biomolecular imaging of Streptomyces coelicolor using secondary ion mass spectrometry

Source: ANALYTICAL CHEMISTRY, 80 (6): 1942-1951 MAR 15 2008

Abstract:

Imaging using time-of-flight secondary ion mass spectrometry (TOF-SIMS) with buckministerfullerene (C-60) primary ions offers the possibility of mapping the chemical distribution of molecular species from biological surfaces. Here we demonstrate the capability of the technique to provide biomolecular information from the cell surface as well as from within the surface, as illustrated with the distribution of two antibiotics in Streptomyces coelicolor (a mycelial bacterium). Differential production of the two pigmented antibiotics under salt-stressed and normal conditions in submerged cultivations could be detected from the TOF-SIMS spectra of the bacteria, demonstrating the potential of the technique in studying microbial physiology. Although both the antibiotics were detected on the cell surface, sputter etching with C-60(+) revealed the spectral features of only one of the antibiotics within the cells. Exploratory analysis of the images using principal component analysis assisted in analyzing the spectral information with respect to peak contributions and their spatial distributions. The technique allows the study of not only lateral but also the depthwise distribution of biomolecules, uniquely enabling exploration of the processes within biological systems with minimal system intervention and with little a priori biochemical knowledge of relevance.


Addresses: Univ Manchester, Manchester Interdisciplinary Bioctr, Sch Chem Engn & Analyt Sci, Manchester M1 7DN, Lancs, England

Univ Manchester, Manchester Interdisciplinary Bioctr, Sch Chem, Manchester M1 7DN, Lancs, England

Reprint Address: VAIDYANATHAN, S, UNIV SHEFFIELD, DEPT CHEM & PROC ENGN, MAPPIN ST, SHEFFIELD S1 3JD, S YORKSHIRE, ENGLAND

Author's E-mail: S.Vaidyanathan@sheffield.ac.uk

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264


Author(s): Maltagliati, L (Maltagliati, Luca); Titov, DV (Titov, Dmitry V.); Encrenaz, T (Encrenaz, Threrese); Melchiorri, R (Melchiorri, Riccardo); Forget, F (Forget, Francois); Garcia-Comas, M (Garcia-Comas, Maya); Keller, HU (Keller, Horst U.); Langevin, Y (Langevin, Yves); Bibring, JP (Bibring, Jean-Pierre)

Title: Observations of atmospheric water vapor above the Tharsis volcanoes on Mars with the OMEGA/MEx imaging spectrometer

Source: ICARUS, 194 (1): 53-64 MAR 2008

Abstract:

The OMEGA imaging spectrometer onboard the Mars Express spacecraft is particularly well suited to study in detail specific regions of Mars, thanks to its high spatial resolution and its high signal-to-noise ratio. We investigate the behavior of atmospheric water vapor over the four big volcanoes located on the Tharsis plateau (Olympus, Ascraeus, Pavonis and Arsia Mons) using the 2.6 mu m band, which is the strongest and most sensitive H2O band in the OMEGA spectral range. Our data sample covers the end of MY26 and the whole MY27, with gaps only in the late northern spring and in northern autumn. The most striking result of our retrievals is the increase of water vapor mixing ratio from the valley to the summit of volcanoes. Corresponding column density is often almost constant, despite a factor of similar to 5 decrease in air mass from the bottom to the top. This peculiar water enrichment on the volcanoes is present in 75% of the orbits in our sample. The seasonal distribution of such enrichment hints at a seasonal dependence, with a minimum during the northern summer and a maximum around the northern spring equinox. The enrichment possibly also has a diurnal trend, being the orbits with a high degree of enrichment concentrated in the early morning. However, the season and the solar time of the observations, due to the motion of the spacecraft, are correlated, then the two dependences cannot be clearly disentangled. Several orbits exhibit also spatially localized enrichment structures, usually ring- or crescent-shaped. We retrieve also the height of the saturation level over the volcanoes. The results show a strong minimum around the aphelion season, due to the low temperatures, while it raises quickly before and after this period. The enrichment is possibly generated by the local circulation characteristic of the volcano region, which can transport upslope significant quantities of water vapor. The low altitude of the saturation level during the early summer can then hinder the transport of water during this season. The influence of the coupling between atmosphere and surface, due mainly to the action of the regoliths, can also contribute partially to the observed phenomenon. (C) 2007 Elsevier Inc. All rights reserved.
Addresses: Max Planck Inst Sonnen Syst Forschung, D-37191 Katlenburg Lindau, Germany

IKI, Space Res Inst, Moscow 117810, Russia

Observ Paris, DESPA, F-92195 Meudon, France

Univ Paris 06, CNRS, LMD, F-75252 Paris, France

Univ Paris 11, CNRS, IAS, F-91405 Orsay, France

Reprint Address: MALTAGLIATI, L, MAX PLANCK INST SONNEN SYST FORSCHUNG, MAX PLANCK STR 2, D-37191 KATLENBURG LINDAU, GERMANY

Author's E-mail: maltagliati@mps.mpg.de

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265

Author(s): Chaurand, P (Chaurand, Pierre); Rahman, MA (Rahman, Mohammad A.); Hunt, T (Hunt, Tamela); Mobley, JA (Mobley, James A.); Gu, G (Gu, Guangyu); Latham, JC (Latham, Joey C.); Caprioli, RM (Caprioli, Richard M.); Kasper, S (Kasper, Susan)



Title: Monitoring mouse prostate development by profiling and imaging mass spectrometry

Source: MOLECULAR & CELLULAR PROTEOMICS, 7 (2): 411-423 FEB 2008

Abstract:

Mass spectrometry-based tissue profiling and imaging are technologies that allow identification and visualization of protein signals directly on thin sections cut from fresh frozen tissue specimens. These technologies were utilized to evaluate protein expression profiles in the normal mouse prostate during development (1-5 weeks of age), at sexual maturation (6 weeks of age), and in adult prostate (at 10, 15, or 40 weeks of age). The evolution of protein expression during normal prostate development and maturation were subsequently compared with 15-week prostate tumors derived from genetically engineered mice carrying the Large T antigen gene under regulation of the prostate-specific probasin promoter (LPB-Tag mouse model for prostate cancer). This approach identified proteins differentially expressed at specific time points during prostate development. Furthermore expression of some of these proteins, for example probasin and spermine-binding protein, were associated with prostate maturation, and prostate tumor formation resulted in their loss of expression. Cyclophilin A, a protein found in other cancers, was differentially a-acetylated on the N terminus, and both isoforms appeared during normal prostate and prostate tumor development. Imaging mass spectrometry localized the protein signals to specific prostatic lobes or regions. Thus, tissue profiling and imaging can be utilized to analyze the ontogeny of protein expression during prostate morphogenesis and tumorigenesis and identify proteins that could potentially serve as biomarkers for prostate cancer.


Addresses: Vanderbilt Univ, Dept Urol Surg, Nashville, TN 37232 USA

Vanderbilt Univ, Mass Spectrometry Res Ctr, Nashville, TN 37232 USA

Univ Alabama, Dept Surg, Div Urol, Birmingham, AL 35233 USA

Reprint Address: KASPER, S, VANDERBILT UNIV, DEPT UROL SURG, A-1302 MCN, NASHVILLE, TN 37232 USA

Author's E-mail: susan.kasper@vanderbilt.edu

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266

Author(s): Kertesz, V (Kertesz, Vilmos); van Berkel, GJ (van Berkel, Gary J.)



Title: Scanning and surface alignment considerations in chemical imaging with desorption electrospray mass spectrometry

Source: ANALYTICAL CHEMISTRY, 80 (4): 1027-1032 FEB 15 2008

Abstract:

The effects of surface scanning mode (raster vs unidirectional scanning) and the constancy of spray tip-to-surface and atmospheric sampling interface capillary-to-surface distances on chemical image quality using desorption electrospray ionization mass spectrometry were investigated. Unidirectional scanning was found to provide a spatially and a quantitatively more precise chemical image of the surface as compared to raster scanning. Maintaining constant spray tip-to-surface and atmospheric sampling interface capillary-to-surface distances during an imaging experiment was found to also be critical. An automation process was implemented using a custom image analysis software (HandsFree Surface Analysis) to keep these distances constant during the surface sampling experiment. Improved chemical image quality afforded through this software control was illustrated by imaging printed objects on normal copy paper.


Addresses: Oak Ridge Natl Lab, Organ & biol Mass Spect Grp, Div Chem Sci, Oak Ridge, TN 37831 USA

Reprint Address: KERTESZ, V, OAK RIDGE NATL LAB, ORGAN & BIOL MASS SPECT GRP, DIV CHEM SCI, OAK RIDGE, TN 37831 USA

Author's E-mail: kerteszv@ornl.gov

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267

Author(s): Farquar, GR (Farquar, George R.); Steele, PT (Steele, Paul T.); McJimpsey, EL (McJimpsey, Erica L.); Lebrilla, CB (Lebrilla, Carlito B.); Tobias, HJ (Tobias, Herbert J.); Gard, EE (Gard, Eric E.); Frank, M (Frank, Matthias); Coffee, K (Coffee, Ketith); Riot, V (Riot, Vincent); Fergenson, DP (Fergenson, David P.)



Title: Supramicrometer particle shadowgraph imaging in the ionization region of a single particle aerosol mass spectrometer

Source: JOURNAL OF AEROSOL SCIENCE, 39 (1): 10-18 JAN 2008

Abstract:

An in situ method to image individual aerosol particles upon desorption/ionization in a single particle aerosol mass spectrometer using shadowgraph imaging is presented and applied directly to determine a 2D spatial distribution of 5.0 mu m particles. This new technique is complementary to previously reported methods for the determination of focused particle beam profiles and has several advantages, including a very low particle concentration requirement and the ability to collect the image of an individual particle with a correlated mass spectrum. Images are presented for 1.3, 2.1, 3.0, and 5.0 mu m polystyrene latex spheres. Particle beam profiles are presented in the directions perpendicular and parallel to the particle beam axis. These results are qualitatively compared to those of a complementary particle collection method (dusting) used at Lawrence Livermore National Laboratory to characterize aerosol beam focusing. (C) 2007 Elsevier Ltd. All rights reserved.


Addresses: Lawrence Livermore Natl Lab, Livermore, CA 94551 USA

Univ Calif Davis, Davis, CA 95616 USA

Reprint Address: STEELE, PT, LAWRENCE LIVERMORE NATL LAB, 7000 E AVE,L211, LIVERMORE, CA 94551 USA

Author's E-mail: psteele@llnl.gov

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268


Author(s): Elbast, M (Elbast, Mouhamad); Wu, TD (Wu, Ting-Di); Guiraud-Vitaux, F (Guiraud-Vitaux, Francoise); Petiet, A (Petiet, Anne); Hindie, E (Hindie, Elif); Champion, C (Champion, Christophe); Croisy, A (Croisy, Alain); Guerquin-Kern, JL (Guerquin-Kern, Jean-Luc); Colas-Linhart, N (Colas-Linhart, Nicole)

Title: Kinetics of intracolloidal iodine within the thyroid of newborn rats. Direct imagery using secondary ion mass spectrometry

Source: COMPTES RENDUS BIOLOGIES, 331 (1): 13-22 JAN 2008

Abstract:

The spatiotemporal distribution of cellular uptake site of radiotoxics is essential data for microdosimetric studies. As early as 1950, the heterogeneity of iodine incorporation within the thyroid has been shown using autoradiography. The objective of this study is to describe the kinetic cellular distribution of newly organified iodine in the thyroid of newborn rats using secondary ion mass microscopy (NanoSIMS50). Ionic images obtained at high mass resolution and with a lateral resolution of about 50 nm show that the early distribution of iodine is heterogeneous from one follicle to another, from one thyrocyte to another inside the same follicle, and that this distribution varies as a function of time. The obtained kinetic profile will allow us to refine the studies concerning the aetiopathology of thyroid cancers of the Chernobyl children.
Addresses: Univ Paris 07, Fac Med, Biophys Lab, F-75870 Paris 18, France

INSERM, U759, F-91405 Orsay, France

Inst Curie, Lab Microscop Ion, F-91405 Orsay, France

Univ Paul Verlaine, Inst Phys, Lab Phys Mol & Collis, F-57078 Metz, France

Reprint Address: COLAS-LINHART, N, UNIV PARIS 07, FAC MED, BIOPHYS LAB, BP 416, F-75870 PARIS 18, FRANCE

Author's E-mail: radiobioexp@aol.com

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269


Author(s): Dobrowolska, J (Dobrowolska, J.); Dehnhardt, M (Dehnhardt, M.); Matusch, A (Matusch, A.); Zoriy, M (Zoriy, M.); Palomero-Gallagher, N (Palomero-Gallagher, N.); Koscielniak, P (Koscielniak, P.); Zilles, K (Zilles, K.); Becker, JS (Becker, J. S.)
Title: Quantitative imaging of zinc, copper and lead in three distinct regions of the human brain by laser ablation inductively coupled plasma mass spectrometry

Source: TALANTA, 74 (4): 717-723 JAN 15 2008

Abstract:

Laser ablation inductively coupled plasma mass spectrometry (LA-ICP-MS) was used to determine the distribution of the trace elements zinc, copper and lead in insular, central and hippocampal areas of thin tissue sections (thickness 20 mu m) through an entire human brain hemisphere. For the investigation of the tissue samples, a commercial laser ablation system was coupled to a double-focusing sector field ICP-MS. The regions of interest of healthy brain tissue (thickness 20 mu m) were scanned (raster area similar to 200 mm(2)) with a focused laser beam (wavelength 266 nm, diameter of laser crater 200 mu m and laser power density 3 x 10(9) W cm(-2)). The ion intensities of Zn-64(+), Cu-63(+) and Pb-208(+) were measured by LA-ICP-MS within the ablated area. For quantification purposes, matrix-matched laboratory standards were prepared by means of dosing of each analyte to the pieces of brain tissue. The mass spectrometric analysis yielded inhomogeneous and largely reciprocal distributions of Zn and Cu in the selected areas of investigated brain samples. The highest concentrations of Zn and Cu with the most distinct distribution pattern were found in the hippocampus (up to 15 mu g g(-1)). In contrast to zinc and copper, for lead, a more homogeneous distribution throughout all regions examined was found at a low concentration (in the ng g(-1) range) level within the analytical range of LA-ICP-MS. (c) 2007 Elsevier B.V. All rights reserved.


Addresses: Res Ctr Zulich, Cent Res Analyt Chem, D-52425 Julich, Germany

Res Ctr Zulich, Inst Med, D-52425 Julich, Germany

Jagiellonian Univ, Fac Chem, Lab Forens Chem, PL-30060 Krakow, Poland

Reprint Address: BECKER, JS, RES CTR ZULICH, CENT RES ANALYT CHEM, D-52425 JULICH, GERMANY

Author's E-mail: s.becker@fz-juelich.de

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270

Author(s): Lee, SG (Lee, S. G.); Bak, JG (Bak, J. G.); Bitter, M (Bitter, M.)



Title: Calibration of an imaging crystal spectrometer for low x-ray energies - art. no. 013501

Source: REVIEW OF SCIENTIFIC INSTRUMENTS, 79 (1): 13501-13501 JAN 2008

Abstract:

An x-ray imaging crystal spectrometer was designed for the Hanbit magnetic mirror device to observe spectra of heliumlike neon at 13.4474 angstrom. The spectrometer consists of a spherically bent mica crystal and an x-ray sensitive vacuum charge coupled device camera. This spectrometer can provide spatially resolved spectra, making it possible to obtain profiles of the ion charge state distribution from line ratios and profiles of the plasma rotation velocity from Doppler shift measurements. The paper describes measurements of spectral resolution of this instrument for low x-ray energies. (C) 2008 American Institute of Physics.


Addresses: Natl Fus Res Inst, Taejon 305333, South Korea

Princeton Plasma Phys Lab, Princeton, NJ 08540 USA

Reprint Address: LEE, SG, NATL FUS RES INST, TAEJON 305333, SOUTH KOREA

Author's E-mail: sglee@nfri.re.kr

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271


Author(s): Balter, V (Balter, Vincent); Reynard, B (Reynard, Bruno)

Title: Secondary ionization mass spectrometry imaging of dilute stable strontium labeling in dentin and enamel

Source: BONE, 42 (1): 229-234 JAN 2008

Abstract:

The labeling of the zones of active mineralization in bone and tooth is usually achieved with calcium-binding fluorescent dyes. However, these compounds are labile and mostly lost during the maturation process of the growing tissue. Here we labeled mouse teeth using injections of dilute strontium (SrCl2, 500 mu g/ml), a trace element that is naturally incorporated in hydroxyapatite, and resolve the subtle induced compositional changes using secondary ion mass spectrometry (SIMS) imaging and analysis. Entire hemi-mandibules sampled at 14 and 28 days after birth are embedded in resin and polished along longitudinal sections. SIMS chemical imaging reveals the double Sr labeling both in dentin and enamel of molar teeth as two stripes with excess Sr concentration parallel to the dentino-enamel junction. In order to quantify the variations of the strontium/calcium ratio (Sr/Ca), two international standards were sintered and measured along with the samples. The concentration of Sr in the two stripes is about 300 mu g/g, which corresponds to an enrichment factor of about 1.3-1.4 relative to the natural baseline. These results show that SIMS provides rapid and quantitative imaging of small abundances of stable isotopes in growing mineralized tissues with a sensibility that is at least two orders of magnitude higher than classical X-rays microanalysis. (C) 2007 Elsevier Inc. All rights reserved.
Addresses: CNRS, UMR Paleoenvironm & Paleobiosphere 5125, F-75700 Paris, France

Univ Lyon 1, Ecole Normale Super Lyon, F-69622 Villeurbanne, France

CNRS, UMR 5570, Lab Sci Terre, F-75700 Paris, France

Reprint Address: BALTER, V, CNRS, UMR PALEOENVIRONM & PALEOBIOSPHERE 5125, F-75700 PARIS, FRANCE

Author's E-mail: Vincent.Balter@univ-lyon1.fr

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272

Author(s): Andersson, M (Andersson, Malin); Groseclose, MR (Groseclose, M. Reid); Deutch, AY (Deutch, Ariel Y.); Caprioli, RM (Caprioli, Richard M.)



Title: Imaging mass spectrometry of proteins and peptides: 3D volume reconstruction

Source: NATURE METHODS, 5 (1): 101-108 JAN 2008

Abstract:

As large genomic and proteomic datasets are generated from homogenates of various tissues, the need for information on the spatial localization of their encoded products has become more pressing. Matrix-assisted laser desorption-ionization (MALDI) imaging mass spectrometry (IMS) offers investigators the means with which to unambiguously study peptides and proteins with molecular specificity, and to determine their distribution in two and three dimensions(1,2). In the past few years, several parameters have been optimized for IMS, including sample preparation, matrix application and instrumental acquisition parameters(3,4) (Box 1). These developments have resulted in a high degree of reproducibility in mass accuracy and peak intensities (Supplementary Fig. 1 online). Recently, we have optimized our protocol to be able to increase the number of molecular species analyzed by collecting two sets of sections, covering one set of sections with sinapinic acid for optimal detection of proteins and adjacent sections with 2,5-dihydroxybenzoic acid (DHB) matrix for the optimal detection of low-mass species, including peptides. Approximately 1,000 peaks can be observed in each dataset (Fig. 1). Furthermore, the sections are collected at an equal distance, 200 mu m instead of 400-500 mu m used previously, thus enabling the use of virtual z-stacks and three-dimensional (3D) volume renderings to investigate differential localization patterns in much smaller brain structures such as the substantia nigra and the interpeduncular nucleus. Here we present our optimized step-by-step procedure based on previous work in our laboratory(2), describing how to make 3D volume reconstructions of MALDI IMS data, as applied to the rat brain.


Addresses: Vanderbilt Univ, Med Ctr, Mass Spectrometry Res Ctr, Nashville, TN 37232 USA

Vanderbilt Univ, Med Ctr, Dept Biochem, Nashville, TN 37232 USA

Vanderbilt Univ, Med Ctr, Dept Psychiat, Nashville, TN 37232 USA

Vanderbilt Univ, Med Ctr, Dept Pharmacol, Nashville, TN 37232 USA

Reprint Address: CAPRIOLI, RM, VANDERBILT UNIV, MED CTR, MASS SPECTROMETRY RES CTR, 465 21ST AVE S, NASHVILLE, TN 37232 USA

Author's E-mail: r.caprioli@vanderbilt.edu

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273


Author(s): Tahallah, N (Tahallah, Nora); Brunelle, A (Brunelle, Alain); De La Porte, S (De La Porte, Sabine); Laprevote, O (Laprevote, Olivier)

Title: Lipid mapping in human dystrophic muscle by cluster-time-of-flight secondary ion mass spectrometry imaging

Source: JOURNAL OF LIPID RESEARCH, 49 (2): 438-454 FEB 2008

Abstract:

Human striated muscle samples, from male control and Duchenne muscular dystrophy-affected children, were subjected to cluster-time-of-flight secondary ion mass spectrometry (cluster-ToF-SIMS) imaging using a 25 keV Bi-3(+) liquid metal ion gun under static SIMS conditions. Spectra and ion density maps, or secondary ion images, were acquired in both positive and negative ion mode over several areas of 500 x 500 mu m(2) (image resolution, 256 x 256 pixels). Characteristic distributions of various lipids were observed. Vitamin E and phosphatidylinositols were found to concentrate within the cells, whereas intact phosphocholines accumulated over the most damaged areas of the dystrophic muscles, together with cholesterol and sphingomyelin species. Fatty acyl chain composition varied depending on the region, allowing estimation of the local damage extent.
Addresses: CNRS, Inst Chim Subst Nat, Unite Propre Rech 2301, Lab Spectrometrie Masse, F-91198 Gif Sur Yvette, France

CNRS, Inst Neurobiol Alfred Fessard, Neurobiol Cellulaire & Mol Lab, Unite Propre Rech 9040,FRC2118, F-91198 Gif Sur Yvette, France

Reprint Address: LAPREVOTE, O, CNRS, INST CHIM SUBST NAT, UNITE PROPRE RECH 2301, LAB SPECTROMETRIE MASSE, F-91198 GIF SUR YVETTE, FRANCE

Author's E-mail: olivier.laprevote@icsn.cnrs-gif.fr

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274


Author(s): Li, Y (Li, Yue); Shrestha, B (Shrestha, Bindesh); Vertes, A (Vertes, Akos)

Title: Atmospheric pressure infrared MALDI imaging mass spectrometry for plant metabolomics

Source: ANALYTICAL CHEMISTRY, 80 (2): 407-420 JAN 15 2008

Abstract:

The utility of atmospheric pressure infrared MALDI mass spectrometry (AP IR-MALDI) was assessed for plant metabolomics studies. Tissue sections from plant organs, including flowers, ovaries, aggregate fruits, fruits, leaves, tubers, bulbs, and seeds were studied in both positive and negative ion modes. For leaves, single laser pulses sampled the cuticle and upper epidermal cells, whereas multiple pulses were demonstrated to ablate some mesophyll layers. Tandem mass spectra were obtained with collision-activated dissociation to aid with the identification of some observed ions. In the positive mode, most ions were produced as potassium, proton, or sometimes sodium ion adducts, whereas proton loss was dominant in the negative ion mode. Over 50 small metabolites and various lipids were detected in the spectra including, for example, 7 of the 10 intermediates in the citric acid cycle. Key components of the glycolysis pathway occurring in the plant cytosol were found along with intermediates of phospholipid biosynthesis and reactants or products of amino acid, nucleotide, oligosaccharide, and flavonoid biosynthesis. AP IR-MALDI mass spectrometry was used to follow the fluid transport driven by transpiration and image the spatial distributions of several metabolites in a white lily (Lilium candidum) flower petal.
Addresses: George Washington Univ, Dept Chem, WM Keck Inst Prote Technol & Applicat, Washington, DC 20052 USA

Reprint Address: VERTES, A, GEORGE WASHINGTON UNIV, DEPT CHEM, WM KECK INST PROTE TECHNOL & APPLICAT, WASHINGTON, DC 20052 USA

Author's E-mail: vertes@gwu.edu

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275

Author(s): Taatjes, CA (Taatjes, Craig A.); Hansen, N (Hansen, Nils); Osborn, DL (Osborn, David L.); Kohse-Hoinghaus, K (Kohse-Hoeinghaus, Katharina); Cool, TA (Cool, Terrill A.); Westmoreland, PR (Westmoreland, Phillip R.)



Title: "Imaging" combustion chemistry via multiplexed synchrotron-photoionization mass spectrometry

Source: PHYSICAL CHEMISTRY CHEMICAL PHYSICS, 10 (1): 20-34 2008

Abstract:

The combination of multiplexed mass spectrometry with photoionization by tunable-synchrotron radiation has proved to be a powerful tool to investigate elementary reaction kinetics and the chemistry of low-pressure flames. In both of these applications, multiple-mass detection and the ease of tunability of synchrotron radiation make it possible to acquire full sets of data as a function of mass, photon energy, and of the physical dimension of the system, e. g. distance from the burner or time after reaction initiation. The data are in essence an indirect image of the chemistry. The data can be quantitatively correlated and integrated along any of several dimensions to compare to traditional measurements such as time or distance profiles of individual chemical species, but it can also be directly interpreted in image form. This perspective offers an overview of flame chemistry and chemical kinetics measurements that combine tunable photoionization with multiple-mass detection, emphasizing the overall insight that can be gained from multidimensional data on these systems. The low-pressure flame apparatus is capable of providing isomer-resolved mass spectra of stable and radical species as a function of position in the flame. The overall chemical structure of the flames can be readily seen from images of the evolving mass spectrum as distance from the burner increases, with isomer-specific information given in images of the photoionization efficiency. Several flames are compared in this manner, with a focus on identification of global differences in fuel-decomposition and soot-formation pathways. Differences in the chemistry of flames of isomeric fuels can be discerned. The application of multiplexed synchrotron photoionization to elementary reaction kinetics permits identification of time-resolved isomeric composition in reacting systems. The power of this technique is illustrated by the separation of direct and dissociative ionization signals in the reaction of C2H5 with O-2; by the resolution of isomeric products in reactions of the ethynyl ( C2H) radical; and by preliminary observation of branching to methyl + propargyl products in the self-reaction of vinyl radicals. Finally, prospects for future research using multiplexed photoionization mass spectrometry are explored.


Addresses: Sandia Natl Labs, Combust Res Facil, Livermore, CA 94551 USA

Univ Bielefeld, Dept Chem, D-33615 Bielefeld, Germany

Cornell Univ, Sch Appl & Engn Phys, Ithaca, NY 14853 USA

Univ Massachusetts, Dept Chem Engn, Amherst, MA 01003 USA

Reprint Address: TAATJES, CA, SANDIA NATL LABS, COMBUST RES FACIL, MAIL STOP 9055, LIVERMORE, CA 94551 USA

Author's E-mail: cataatj@sandia.gov

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276


Author(s): Chandra, S (Chandra, S.); Tjarks, W (Tjarks, W.); Lorey, DR (Lorey, D. R., II); Barth, RF (Barth, R. F.)

Title: Quantitative subcellular imaging of boron compounds in individual mitotic and interphase human glioblastoma cells with imaging secondary ion mass spectrometry (SIMS)

Source: JOURNAL OF MICROSCOPY-OXFORD, 229 (1): 92-103 JAN 2008

Abstract:



Boron measurements at subcellular scale are essential in boron neutron capture therapy (BNCT) of cancer as the nuclear localization of boron-10 atoms can enhance the effectiveness of killing individual tumour cells. Since tumours contain a heterogeneous population of cells in interphase as well as in the M phase (mitotic division) of the cell cycle, it is important to evaluate the subcellular distribution of boron in both phases. In this work, the secondary ion mass spectrometry (SIMS) based imaging technique of ion microscopy was used to quantitatively image boron from two BNCT agents, wclinically used p-boronophenylalanine (BPA) and 3-[4-(o-carboran-1-yl) butyl] thymidine (N4), in mitotic metaphase and interphase human glioblastoma T98G cells. N4 belongs to a class of experimental BNCT agents, designated 3- carboranyl thymidine analogues (3CTAs), which presumably accumulate selectively in cancer cells due to a process referred to as kinase-mediated trapping (KMT). The cells were exposed to BPA for 1 h and N4 for 2 h. A CAMECA IMS-3f SIMS ion microscope instrument capable of producing isotopic images with 500 nm spatial resolution was used in the study. Observations were made in cryogenically prepared fast frozen, and freeze-fractured, freeze-dried cells. Three discernible subcellular regions were studied: the nucleus, a characteristic mitochondria-rich perinuclear cytoplasmic region, and the remaining cytoplasm in interphase T98G cells. In metaphase cells, the chromosomes and the cytoplasm were studied for boron localization. Intracellular concentrations of potassium and sodium also were measured in each cell in which the subcellular boron concentrations were imaged. Since the healthy cells maintain a K/Na ratio of approximately 10 due to the presence of Na-K-ATPase in the plasma membrane of mammalian cells, these measurements provided validation for cryogenic sample preparation and indicated the analysis healthy, well preserved cells. The BPA-treated interphase cells revealed significantly lower concentrations of boron in the perinuclear mitochondria-rich cytoplasmic region as compared to the remaining cytoplasm and the nucleus, which were not significantly different from each other. In contrast, the BPA-treated metaphase cells revealed significantly lower concentration of boron in their chromosomes than cytoplasm. In addition, the cytoplasm of metaphase cells contained significantly less boron than the cytoplasm of interphase cells. These observations provide valuable information on the reduced uptake of boron from BPA in mitotic cells for BPA-mediated BNCT. SIMS observations on N4 revealed that boron was distributed throughout the interphase and mitotic cells, including the chromosomes. The presence of boron in chromosomes of metaphase cells treated with N4 is indicative of a possible incorporation of this thymidine analogue into DNA. The 3-DSIMS imaging approach for the analysis of mitotic cells shown in this work should be equally feasible to the evaluation of other BNCT agents.
Addresses: Cornell Univ, Dept Earth & Atmospher Sci, Cornell SIMS Lab, Ithaca, NY 14853 USA

Ohio State Univ, Coll Pharm, Columbus, OH 43210 USA

Cornell Univ, Dept Chem & Chem Biol, Ithaca, NY USA

Ohio State Univ, Dept Pathol, Columbus, OH 43210 USA

Reprint Address: CHANDRA, S, CORNELL UNIV, DEPT EARTH & ATMOSPHER SCI, CORNELL SIMS LAB, ITHACA, NY 14853 USA

Author's E-mail: sc40@cornell.edu


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