Application of Black Silicon for Nanostructure-Initiator Mass Spectrometry

Gao, Jian; Raad, Markus de; Bowen, Benjamin P.; Zuckermann, Ronald N.; Northen, Trent

doi:10.1021/acs.analchem.5b03452

Cited by 32 publications

(32 citation statements)

References 43 publications

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“…Surface‐assisted laser desorption/ionization (SALDI) methods, which utilize the optophysical properties of inorganic solid microstructures instead of the spectral properties of organic matrix compounds, can be used on existing MALDI mass spectrometers and would be effective for low‐mass analytes whose detection might be impaired by matrix‐related peaks. Substrate‐type SALDI methods utilize planar solid substrates with microstructures on the uppermost surface layer as the target . In those SALDI methods, analytes are spread and adsorbed onto the target plate that converts photon energies of laser to a driving force for desorption and ionization via interaction with the surface microstructures.…”

Section: Introductionmentioning

confidence: 99%

DIUTHAME enables matrix‐free mass spectrometry imaging of frozen tissue sections

Kuwata

Itou

Kotani

et al. 2020

Rapid Comm Mass Spectrometry

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Rationale:A recently developed matrix-free laser desorption/ionization method, DIUTHAME (desorption ionization using through-hole alumina membrane), was examined for the feasibility of mass spectrometry imaging (MSI) applied to frozen tissue sections. The permeation behavior of DIUTHAME is potentially useful for MSI as positional information may not be distorted during the extraction of analytes from a sample. Methods:The through-hole porous alumina membranes used in the DIUTHAME chips were fabricated by wet anodization, were 5 μm thick, and had the desired values of 200 nm through-hole diameter and 50% open aperture ratio. Mouse brain frozen tissue sections on indium tin oxide (ITO)-coated slides were covered using the DIUTHAME chips and were subjected to MSI experiments in commercial time-offlight mass spectrometers equipped with solid-state UV lasers after thawing and drying without matrix application.Result: Mass spectra and mass images were successfully obtained from the frozen tissue sections using DIUTHAME as the ionization method. The mass spectra contained rich peaks in the phospholipid mass range free from the chemical background owing to there being no matrix-derived peaks in that range. DIUTHAME-MSI delivered high-quality mass images that reflected the anatomy of the brain tissue. Conclusions:Analytes can be extracted from frozen tissue by capillary action of the through-holes in DIUTHAME and moisture contained in the tissue without distorting positional information of the analytes. The sample preparation for frozen tissue sections in DIUTHAME-MSI is simple, requiring no specialized skills or dedicated apparatus for matrix application. DIUTHAME can facilitate MSI at a low mass, as there is no interference from matrix-derived peaks, and should provide high-quality, reproducible mass images more easily than MALDI-MSI.

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Section: Introductionmentioning

confidence: 99%

DIUTHAME enables matrix‐free mass spectrometry imaging of frozen tissue sections

Kuwata

Itou

Kotani

et al. 2020

Rapid Comm Mass Spectrometry

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“…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%

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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“…These porous nanostructures enable large surface area as well as low melting points that allow efficient conversion of analyte molecules into gas-phase ions under low intensity laser irradiation. 3,26,27,46 Spectroscopic ellipsometry was applied to characterize physical parameters of these porous substrates, and adsorption and desorption isotherms of toluene in the silicon surface were obtained under a broad range of relative pressures (sample pressure/saturated pressure) as shown in Supporting Information. The results were fitted by the Kelvin equation and Forouhi−Bloomer's model to extract their pore size distribution from these isotherms (Supporting Information).…”

Section: ■ Results and Discussionmentioning

confidence: 99%

Morphology-Driven Control of Metabolite Selectivity Using Nanostructure-Initiator Mass Spectrometry

et al. 2017

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Nanostructure-initiator mass spectrometry (NIMS) is a laser desorption/ionization analysis technique based on the vaporization of a nanostructure-trapped liquid "initiator" phase. Here we report an intriguing relationship between NIMS surface morphology and analyte selectivity. Scanning electron microscopy and spectroscopic ellipsometry were used to characterize the surface morphologies of a series of NIMS substrates generated by anodic electrochemical etching. Mass spectrometry imaging was applied to compare NIMS sensitivity of these various surfaces toward the analysis of diverse analytes. The porosity of NIMS surfaces was found to increase linearly with etching time where the pore size ranged from 4 to 12 nm with corresponding porosities estimated to be 7-70%. Surface morphology was found to significantly and selectively alter NIMS sensitivity. The small molecule (<2k Da) sensitivity was found to increase with increased porosity, whereas low porosity had the highest sensitivity for the largest molecules examined. Estimation of molecular sizes showed that this transition occurs when the pore size is <3× the maximum of molecular dimensions. While the origins of selectivity are unclear, increased signal from small molecules with increased surface area is consistent with a surface area restructuring-driven desorption/ionization process where signal intensity increases with porosity. In contrast, large molecules show highest signal for the low-porosity and small-pore-size surfaces. We attribute this to strong interactions between the initiator-coated pore structures and large molecules that hinder desorption/ionization by trapping large molecules. This finding may enable us to design NIMS surfaces with increased specificity to molecules of interest.

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Application of Black Silicon for Nanostructure-Initiator Mass Spectrometry

Cited by 32 publications

References 43 publications

DIUTHAME enables matrix‐free mass spectrometry imaging of frozen tissue sections

DIUTHAME enables matrix‐free mass spectrometry imaging of frozen tissue sections

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

Morphology-Driven Control of Metabolite Selectivity Using Nanostructure-Initiator Mass Spectrometry

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