Development of capabilities for imaging mass spectrometry under ambient conditions with desorption electrospray ionization (DESI)

Ifa, Demian R.; Wiseman, Justin M.; Song, Qingyu; Cooks, R. Graham

doi:10.1016/j.ijms.2006.08.003

Cited by 250 publications

(237 citation statements)

References 46 publications

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“…Analytes present at the surface are desorbed and ionized by the incoming plume and subsequently transferred to the mass spectrometer inlet by the influence of the applied potential and the pressure differential between atmospheric pressure and the low-pressure region of the mass analyzer. To date, DESI has found many applications including forensic analysis [2][3][4][5], explosives detection [6 -9], chemical warfare agent detection [3, 10 -12], imaging [13][14][15], pharmaceutical analysis [16 -24], natural product characterization [2,25], polymer analysis [26,27], metabolomics [2, 28 -31], proteomics [2,[32][33], and glycomics [34].…”

Section: Esorption Electrospray Ionization (Desi)mentioning

confidence: 99%

The influence of material and mesh characteristics on transmission mode desorption electrospray ionization

Chipuk

Brodbelt

2008

J. Am. Soc. Mass Spectrom.

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Adaptation of desorption electrospray ionization to a transmission mode (TM-DESI) entails passing an electrospray plume through a sample that has been deposited onto a mesh substrate. A combination of mass spectrometry and fluorescence microscopy studies is used to illustrate the critical role material composition, mesh open space, and mesh fiber diameter play on the transmission, desorption, and ionization process. Substrates with open spaces less than 150 m and accompanying minimal strand diameters produce less scattering of the plume and therefore favor transmission. Larger strand diameters typically encompass larger open spaces, but the increase in the surface area of the strand increases plume scattering as well as solvent and analyte spreading on the mesh. Polypropylene (PP), ethylene tetrafluoroethylene (ETFE), and polyetheretherketone (PEEK) materials afford much better desorption than similarly sized polyethylene terephthalate (PETE) or nylon-6,6 (PA66) substrates. Ultimately, the manner in which the electrospray plume interacts with the mesh as it is transmitted through the substrate is shown to be critical to performing and optimizing TM-DESI analyses. In addition, evidence is presented for analyte dependent variations in the desorption mechanisms of dry and solvated samples. . In DESI, ions are produced by directing charged solvent droplets from an electrospray source toward a sample that is either a bulk material in its native state (e.g., pharmaceutical tablet) or one that has been deposited from solution onto a sampling surface. Analytes present at the surface are desorbed and ionized by the incoming plume and subsequently transferred to the mass spectrometer inlet by the influence of the applied potential and the pressure differential between atmospheric pressure and the low-pressure region of the mass analyzer. To date, DESI has found many applications including forensic analysis [2][3][4][5] Recent adaptations of DESI, including geometry independent DESI in gas tight enclosures [35] and transmission mode desorption electrospray ionization (TM-DESI), have been developed to reduce the geometry dependence of DESI experiments [36]. In the transmission DESI mode the sample is not deposited onto a continuous solid surface but rather onto a sampling mesh. In this adaptation, the incident spray angle and collection angle are fixed at 0°and the spray is transmitted through the sample (Figure 1). Along with the simplification of the experimental geometry, the transmission mode also allows convenient analysis of both dry (i.e., following evaporation of the deposition solvent) and wet (i.e., solvated) samples with similar performance characteristics to those achieved using traditional DESI [36].Surface variables including the chemical composition, porosity, texture, and electrical conductivity of the substrate have been reported to affect DESI analyses [2,24,[37][38][39]. Dramatic reductions in response have been noted for high conductivity surfaces due to neutralization of the incoming ion plume at the su...

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Section: Esorption Electrospray Ionization (Desi)mentioning

confidence: 99%

The influence of material and mesh characteristics on transmission mode desorption electrospray ionization

Chipuk

Brodbelt

2008

J. Am. Soc. Mass Spectrom.

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“…In the alternative serial sectioning approach, serial sections of the object are obtained through mechanical sectioning and individually analyzed. Matrix assisted laser desorption ionization (MALDI-MS) [8] is the only technique that have been used to serial sectioning analysis for 3D imaging.SIMS and MALDI are well established techniques that have been widely used for molecular imaging under vacuum but newer ambient ionization methods such as DESI [9,10], LAESI, AP-IR-MALDI and LA-FAPA allow the direct analysis of samples in the open atmosphere. In particular, DESI-MS is an ambient desorption ionization method with the advantages of little or no sample preparation, ease of implementation and simplified analysis [11].…”

mentioning

confidence: 99%

“…Indeed, it has been shown that several experimental parameters can be optimized to improve the quality of DESI data. [9,15] Two distinctive mass spectral patterns were observed in the negative-ion mode for the brain sections analyzed depending on the region of the brain being investigated (Figure 1). The differences are associated with the lipid compositions representative of the gray and white matter of the brain.…”

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confidence: 99%

Three‐Dimensional Vizualization of Mouse Brain by Lipid Analysis Using Ambient Ionization Mass Spectrometry

Eberlin

Ifa

et al. 2010

Angewandte Chemie

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Keywords ambient ionization; molecular imaging; mass spectrometry; mouse brain model; phospholipids; tissue analysis Two-dimensional (2D) imaging mass spectrometry (MS) [1] has emerged as a powerful technique in the biological sciences. It allows direct investigation of the distribution of a variety of lipids, drugs, biological defensive agents, pigments and proteins in plant and animal tissues with high specificity and without the need of fluorescent or radioactive labelling normally used in histochemical protocols. [2,3] In imaging MS, the chemical identity of molecules present on a surface is investigated as a function of their 2D spatial distribution (x and y coordinates).Three-dimensional (3D) images can be constructed from a suitable set of 2D data and they illustrate the spatial distributions of specific biomolecules in substructures of tissues including pathological features [4]. Two basic approaches, depth profiling and serial sectioning, have been described for recording the information needed to create 3D MS-based images. In depth profiling experiments, the desorbing agent is used to remove shallow layers of material from the surface of the object in between recording surface analysis data. Secondary ion mass spectrometry (SIMS) [5], laser ablation electrospray ionization (LAESI) [2,6] and laser ablation flowing atmospheric-pressure afterglow (LA-FAPA) [7] are ionization techniques that have been used to create 3D MS models by depth profiling. In the alternative serial sectioning approach, serial sections of the object are obtained through mechanical sectioning and individually analyzed. Matrix assisted laser desorption ionization (MALDI-MS) [8] is the only technique that have been used to serial sectioning analysis for 3D imaging.SIMS and MALDI are well established techniques that have been widely used for molecular imaging under vacuum but newer ambient ionization methods such as DESI [9,10], LAESI, AP-IR-MALDI and LA-FAPA allow the direct analysis of samples in the open atmosphere. In particular, DESI-MS is an ambient desorption ionization method with the advantages of little or no sample preparation, ease of implementation and simplified analysis [11]. Most importantly, the problem of endogenous compounds dislocation during sample preparation procedures of traditional histochemical analysis can be overcome, because tissue sections are analyzed directly outside the mass spectrometer without any treatments after sectioning. It has been shown that DESI-MS imaging can be used to distinguish between cancerous and non-cancerous tissue samples using multiple marker lipids [12]. DESI-MS imaging has also In order to obtain high quality 2D images, essential to building reliable 3D images, experimental conditions were optimized to maximize the signal intensity and increase image quality (see Supporting Information for Experimental Section). Indeed, it has been shown that several experimental parameters can be optimized to improve the quality of DESI data. [9,15] Two distinctive mass spectral patterns were ob...

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“…In particular, the intensities of certain sphingomyelin species marked the margin between the non-tumor and the tumor portion of the tissue sections. More recently, two-dimensional molecular ion images of thin sections of rat brain tissue have been recorded using 2D rastering of the cryosectioned tissue with a DESI ion source, and characteristically different distributions in lipids have been noted [30,31].…”

mentioning

confidence: 99%

Desorption electrospray ionization (DESI) mass spectrometry and tandem mass spectrometry (MS/MS) of phospholipids and sphingolipids: Ionization, adduct formation, and fragmentation

Manicke

Wiseman

Ifa

et al. 2008

J. Am. Soc. Mass Spectrom.

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Desorption electrospray ionization (DESI) mass spectrometry was evaluated for the characterization of glycerophospholipid standards, including glycerophosphocholine (GPCho), glycerophosphoglycerol (GPGro), glycerophosphoethanolamine (GPEtn), glycerophosphoserine (GPSer), glycerophosphoinositol (GPIns), cardiolipin (CL), and sphingolipid standards, including sulfatides (ST) and sphingomyelin (SM). Of specific interest were the effects of surface and solvent composition on signal stability and intensity, along with the ions observed in the full scan mode and the fragmentations seen upon collisional activation for each of the above classes. These experiments were performed without the addition of matrix compounds to the sample and were conducted in the free ambient environment at atmospheric pressure. The compounds GPSer, GPGro, GPIns, ST, and CL were best analyzed in the negative ion mode while PE was ionized efficiently in both positive and negative ion modes. SM and GPCho, which typically generate more abundant ions in the positive ion mode, could be analyzed in the negative ion mode by the addition of anionic reagents such as acetate to the spray solvent. Full scan DESI mass spectra and tandem (MS/MS) spectra for this representative set of physiological phospho/sphingolipids are presented. Similarities with other ionization methods in terms of fragmentation behavior were strong, although ambient ionization of untreated samples is only available with DESI. The effect of surface and solvent properties on signal intensity and stability were determined by depositing standard compounds on several different surfaces and analyzing with various proportions of methanol in the aqueous spray. Analysis was extended to complex mixtures of phospholipids and sphingolipids by examining the total lipid extract of porcine brain and by direct analysis of rat brain cryotome sections. These types of mixture analyses and molecular imaging studies are likely to represent major areas of application of DESI. (J

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Development of capabilities for imaging mass spectrometry under ambient conditions with desorption electrospray ionization (DESI)

Cited by 250 publications

References 46 publications

The influence of material and mesh characteristics on transmission mode desorption electrospray ionization

The influence of material and mesh characteristics on transmission mode desorption electrospray ionization

Three‐Dimensional Vizualization of Mouse Brain by Lipid Analysis Using Ambient Ionization Mass Spectrometry

Desorption electrospray ionization (DESI) mass spectrometry and tandem mass spectrometry (MS/MS) of phospholipids and sphingolipids: Ionization, adduct formation, and fragmentation

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