High Sensitivity and Analyte Capture with Desorption/Ionization Mass Spectrometry on Silylated Porous Silicon

Trauger, Sunia A.; Go, Eden P.; Shen, Zhouxin; Apon, Junefredo V.; Compton, Bruce Jon; Bouvier, Edouard S. P.; Finn, M. G.; Siuzdak, Gary

doi:10.1021/ac049657j

Cited by 220 publications

(252 citation statements)

References 20 publications

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“…To date a number of ionization techniques that belong to SALDI have been proposed,1, 2, 3, 4, 5, 6, 7, 8, 9, 10, 11, 12, 13, 14, 15, 16, 17, 18, 19, 20, 21, 22, 23, 24, 25, 26, 27, 28, 29, 30, 31, 32, 33, 34, 35, 36, 37, 38, 39, 40, 41, 42, 43, 44, 45, 46, 47, 48, 49, 50, 51, 52, 53, 54, 55, 56, 57, 58, 59, 60, 61, 62, 63, 64, 65, 66, 67, 68, 69, 70, 71, 72, 73, 74, 75, ...…”

Section: Introductionmentioning

confidence: 99%

“…The techniques in the other category utilize planar solid substrates with fine structures on the uppermost surface layer as the target plate, so that the photon energies of the laser can reach analytes which are spread over and adsorbed onto the surface and achieve desorption and ionization of analytes 20, 23, 46, 47, 48, 49, 50, 51, 52, 53, 54, 55, 56, 57, 58, 59, 60, 61, 62, 63, 64, 65, 66, 67, 68, 69, 70, 71, 72, 73, 74, 75, 76, 77, 78, 79, 80. Desorption Ionization on Silicon (DIOS) is the representative technique in this category 46.…”

Section: Introductionmentioning

confidence: 99%

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A novel laser desorption/ionization method using through hole porous alumina membranes

Naito

Kotani

Ohmura

2018

Rapid Comm Mass Spectrometry

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RationaleA novel matrix‐free laser desorption/ionization method based on porous alumina membranes was developed. The porous alumina membranes have a two‐dimensional (2D) ordered structure consisting of closely aligned straight through holes of sub‐micron in diameter that are amenable to mass production by industrial fabrication processes.MethodsConsidering a balance between the ion generating efficiency and the mechanical strength of the membranes, the typical values for the hole diameter, open aperture ratio and membrane thickness were set to 200 nm, 50% and 5 μm, respectively. The membranes were coated with platinum on a single side that was exposed to the laser. Evaluation experiments were conducted on the feasibility of this membrane structure for an ionization method using a single peptide and mixed peptides and polyethylene glycol samples and a commercial matrix‐assisted laser desorption/ionization (MALDI) time‐of‐flight mass spectrometer in the positive ion mode.ResultsResults showed a softness of ionization and no sweet spot nature. The capillary action of the through holes with very high aspect ratio enables several loading protocols including sample impregnation from the surface opposite to the laser exposure side.ConclusionsThe feasibility study indicates that the through hole porous alumina membranes have several advantages in terms of usefulness over the conventional surface‐assisted laser desorption ionization (SALDI) methods. The proposed novel ionization method is termed Desorption Ionization Using Through Hole Alumina Membrane (DIUTHAME).

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Section: Introductionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

A novel laser desorption/ionization method using through hole porous alumina membranes

Naito

Kotani

Ohmura

2018

Rapid Comm Mass Spectrometry

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“…Other surfaces have also been shown to generate intact molecular ions into the gas phase, including GaAs and GaN [5], immobilized carbon nanotubes [6], silicon nanowires [7,8], and lithographically patterned and roughened silicon surfaces [9]. In particular, the porous silicon surface has demonstrated unique performance capabilities, allowing the analysis of a wide range of molecules [10] and peptide analysis at the 800 yoctomole level [11]. Given its novel means of generating ions, a more complete understanding on how these ions are transferred intact into the gas phase has practical as well as fundamental scientific implications for surface-based mass analysis.…”

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confidence: 99%

High surface area of porous silicon drives desorption of intact molecules

Northen

Woo

Northen

et al. 2007

J. Am. Soc. Mass Spectrom.

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The surface structure of porous silicon used in desorption/ionization on porous silicon (DIOS) mass analysis is known to play a primary role in the desorption/ionization (D/I) process. In this study, mass spectrometry and scanning electron microscopy (SEM) are used to examine the correlation between intact ion generation with surface ablation and surface morphology. The DIOS process is found to be highly laser energy dependent and correlates directly with the appearance of surface ions (Si n ϩ and OSiH ϩ ). A threshold laser energy for DIOS is observed (10 mJ/cm 2 ), which supports that DIOS is driven by surface restructuring and is not a strictly thermal process. In addition, three DIOS regimes are observed that correspond to surface restructuring and melting. These results suggest that higher surface area silicon substrates may enhance DIOS performance. A recent example that fits into this mechanism is the surface of silicon nanowires, which has a high surface energy and concomitantly requires lower laser energy for analyte desorption. (J Am Soc Mass Spectrom 2007, 18, 1945-1949

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“…Surface functional groups of DIOS substrates are decided by substrate preparation and storage [11,20,21]. For example, surface oxidation occurs immediately after a brief exposure of the substrate in air and has been found to be the culprit for performance degradation of DIOS-MS [22].…”

Section: Analyte Protonation By Porous Si Surfacementioning

confidence: 99%

Quantitative study of solvent and surface effects on analyte ionization in desorption ionization on silicon (DIOS) mass spectrometry

Liu

2008

J. Am. Soc. Mass Spectrom.

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Deuterated solvents and DIOS surfaces derivatized with different functional groups are used to investigate impacts of local chemical environment on analyte ionization. Both solvent molecules and surface functional groups are found to directly participate in analyte protonation in the condensed phase. The corresponding protonation effectiveness is quantitatively estimated based on the relative MS peak intensities of [M ϩ 2] ϩ /[M ϩ 1] ϩ . A direct correlation between ionization of triethylamine and the relative acidities of the surface and the solvent is evident. In addition, the proton donating effectiveness of a solvent is found to be related to its vapor pressure. Improved MS detection of small molecules via proper surface treatment and solvent selection is demonstrated. (J Am Soc Mass Spectrom 2008, 19, 8 -13) © 2008 American Society for Mass Spectrometry E xtensive research in metabolite profiling in recent years has revived interest in desorption ionization on porous silicon mass spectrometry (DIOS-MS). Elimination of matrix molecules in DIOS-MS reduces background noise in the low-mass range and enables direct detection of biologically significant small molecules [1][2][3][4]. It also overcomes matrix-induced analyte redistribution on a sample surface, which allows two-dimensional imaging of tissue samples with good spatial accuracy [5]. Recent studies have shown that the local chemical properties of a DIOS substrate, including the residual solvent on the surface and the surface functional groups, are critical in analyte ionization [6 -9]. Quantitative investigation of these factors, however, is lacking. In this report, we semiquantitatively assessed contributions of various proton sources in DIOS-MS and the feasibility of improving MS detection of lipids and peptides by proper sample treatment. Experimental DIOS Substrate PreparationDIOS substrates were prepared by dipping the wafer into a solution of 5% HF/EtOH for 1 min to remove the oxidized layer, followed by a 1.5-min anodic etching in 25% HF/EtOH at 5 mA/cm 2 [10,11]. Before MS experiments, the DIOS substrates were dipped in 5% HF/ EtOH to regenerate the H-terminated surface. For OHterminated surfaces, the DIOS substrates were dipped in a solution of 15% H 2 O 2 /MeOH (or 15% D 2 O 2 / MeOH-d 4 ) for 30 min. For RNH 2 -terminated surfaces, the same OH-terminated surfaces were refluxed in a solution of 10% APTMS/toluene under N 2 for 4 h. To remove residual solvent molecules, the DIOS or chemically modified DIOS substrates were dried under high vacuum overnight, unless specified otherwise.

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High Sensitivity and Analyte Capture with Desorption/Ionization Mass Spectrometry on Silylated Porous Silicon

Cited by 220 publications

References 20 publications

A novel laser desorption/ionization method using through hole porous alumina membranes

A novel laser desorption/ionization method using through hole porous alumina membranes

High surface area of porous silicon drives desorption of intact molecules

Quantitative study of solvent and surface effects on analyte ionization in desorption ionization on silicon (DIOS) mass spectrometry

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