Desorption electrospray ionization mass spectrometry: Imaging drugs and metabolites in tissues

Wiseman, Justin M.; Ifa, Demian R.; Zhang, Yongxin; Kissinger, Candice B.; Manicke, Nicholas E.; Kissinger, Peter T.; Cooks, R. Graham

doi:10.1073/pnas.0801066105

Cited by 416 publications

(369 citation statements)

References 43 publications

(39 reference statements)

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“…esorption electrospray ionization (DESI) [1,2] is a widely used ambient ionization technique [3][4][5][6][7][8], which is used for surface sampling [9,10], high throughput analysis [11,12], and chemical imaging [13][14][15][16][17], largely because of its applicability to in situ analyte detection from unmodified surfaces. In DESI, a nebulized electrospray of high-velocity charged microdroplets is directed at a surface from which the solvent extracts analyte and carries it to the mass spectrometer in the form of secondary microdroplets.…”

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Enhanced ion signals in desorption electrospray ionization using surfactant spray solutions

Badu‐Tawiah

Cooks

2010

J. Am. Soc. Mass Spectrom.

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Solvent optimization is an important procedure in desorption electrospray ionization (DESI) and in this study the effects of solvent surface tension are explored. Data are presented for methanol/water/surfactant solvent systems, which show increases in ion signals of more than an order of magnitude when low concentrations of surfactants are added to the standard methanol/water (1:1) spray solvent. Examples of analytes tested include food chemicals, peptides, pharmaceuticals, and drugs of abuse. The improvement in ion intensity is mainly attributed to the effect of surface tension in producing smaller spray droplets, which are shown to cover a larger surface area. Surfactant-containing spray solutions allowed extension of DESI-MS analysis to previously intractable analytes like melamine and highly hydrophobic compounds like the sudan dyes. ( [3][4][5][6][7][8], which is used for surface sampling [9,10], high throughput analysis [11,12], and chemical imaging [13][14][15][16][17], largely because of its applicability to in situ analyte detection from unmodified surfaces. In DESI, a nebulized electrospray of high-velocity charged microdroplets is directed at a surface from which the solvent extracts analyte and carries it to the mass spectrometer in the form of secondary microdroplets. This methodology has been applied in a variety of disciplines including forensics [18,19], environmental science [20], food science [12,21], and pharmaceutical science [22]. With increased interest in ambient desorption mass spectrometry, the need has arisen to develop more versatile solvent systems that are applicable to a wider range of samples than is currently the case. One aspect of this effort is the use of non-aqueous spray solutions [23] and another is the addition of reagents to the spray solvent chosen to react and give ionic derivatives of the analytes of interest [24]. Both are discussed further below. In this work, we explore the special properties of spray solutions containing surfactants, in an attempt to increase the ion intensity and to learn more about the mechanisms of DESI.Three mechanisms have been identified in DESI, all falling under the rubric of droplet pick-up. The first and best established is the droplet micro-extraction mechanism [25,26]. In this mechanism, initial droplets arriving at the surface form a localized and probably discontinuous liquid thin film, which dissolves analyte present on the surface. Subsequent droplet-liquid-thin-film collisions produce secondary microdroplets containing the analyte, which are then sucked into the mass spectrometer for mass/charge analysis. A second mechanism is believed to involve gas-phase ion/molecule reactions [2]. In this case, vaporization of the analyte from the surface is followed by fast charge-transfer reactions with protonated (or other) solvent molecules or droplets to produce charged analytes, which are then transferred into the mass spectrometer for mass analysis. A third mechanism, which also seems to make a limited contribution to ion production in ...

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Enhanced ion signals in desorption electrospray ionization using surfactant spray solutions

Badu‐Tawiah

Cooks

2010

J. Am. Soc. Mass Spectrom.

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“…E.g., a selection of [1,4,5] usually results in the retrieval of a single scalar corresponding to the item with index (1,4,5).…”

Section: Data Selection Basic Slicingmentioning

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“…This means if multiple lists are specified, then the lists must be of equal length and the lists are merged to define specific indexpairs to be selected. E.g, x= [1,2] and y= [4,5] results in the retrieval of the elements [ (1,4), (2,4) ] compared to an all-to-all matching, which would retrieve [ (1,4), (1,5), (2,4), (2,5) ]. This scheme allows for selection of arbitrary regions of interest.…”

Section: Multi-dimensional Slicingmentioning

confidence: 99%

“…#Check and read input parameters if argv is None: argv = sys.argv if len(argv) < 2 : printHelp() exit(0) #If we are a slave process, then read the requested data #subset and exit if len(argv) == 8 : infile = argv [1] xmin = int(argv [2]) xmax = int(argv [3]) ymin = int(argv [4]) ymax = int(argv [5]) zmin = int(argv [6]) zmax = int(argv [7] We compute each test separately so that we have touched #enough data from other files to avoid biases due to data cacheing. #Note: Depending on the file system, a significant amount of data #and in some cases complete files) can be cached by the file #system.…”

Section: Data Readmentioning

confidence: 99%

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OpenMSI: A High-Performance Web-Based Platform for Mass Spectrometry Imaging

et al. 2013

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“…However, these methods require extensive sample preparation, such as the application of matrix molecules to the sample surface, and a vacuum sampling environment, which could introduce artifacts to the data obtained. Ambient techniques such as desorption electrospray ionization (DESI) MS 5 , laser ablation electrospray ionization (LAESI) MS 6 , and nano-DESI MS 7 are capable of MSI of samples with little to no prior preparation under the ambient environment, which is able to produce MS images that potentially reflect the sample in its most native state. However, most of these techniques generally lack the high spatial resolution and detection sensitivity compared with the non-ambient techniques, with experiments typically conducted at around 150 μm per pixel 8 .…”

Section: Introductionmentioning

confidence: 99%

Applications of the Single-probe: Mass Spectrometry Imaging and Single Cell Analysis under Ambient Conditions

Rao

Pan

Yang

2016

JoVE

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Mass spectrometry imaging (MSI) and in-situ single cell mass spectrometry (SCMS) analysis under ambient conditions are two emerging fields with great potential for the detailed mass spectrometry (MS) analysis of biomolecules from biological samples. The single-probe, a miniaturized device with integrated sampling and ionization capabilities, is capable of performing both ambient MSI and in-situ SCMS analysis. For ambient MSI, the single-probe uses surface micro-extraction to continually conduct MS analysis of the sample, and this technique allows the creation of MS images with high spatial resolution (8.5 μm) from biological samples such as mouse brain and kidney sections. Ambient MSI has the advantage that little to no sample preparation is needed before the analysis, which reduces the amount of potential artifacts present in data acquisition and allows a more representative analysis of the sample to be acquired. For in-situ SCMS, the single-probe tip can be directly inserted into live eukaryotic cells such as HeLa cells, due to the small sampling tip size (< 10 μm), and this technique is capable of detecting a wide range of metabolites inside individual cells at near real-time. SCMS enables a greater sensitivity and accuracy of chemical information to be acquired at the single cell level, which could improve our understanding of biological processes at a more fundamental level than previously possible. The single-probe device can be potentially coupled with a variety of mass spectrometers for broad ranges of MSI and SCMS studies.

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Desorption electrospray ionization mass spectrometry: Imaging drugs and metabolites in tissues

Cited by 416 publications

References 43 publications

Enhanced ion signals in desorption electrospray ionization using surfactant spray solutions

Enhanced ion signals in desorption electrospray ionization using surfactant spray solutions

OpenMSI: A High-Performance Web-Based Platform for Mass Spectrometry Imaging

Applications of the Single-probe: Mass Spectrometry Imaging and Single Cell Analysis under Ambient Conditions

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