Testing Molecular Homogeneity at the Nanoscale with Massive Cluster Secondary Ion Mass Spectrometry

Eller, Michael J.; Verkhoturov, Stanislav V.; Schweikert, E. A.

doi:10.1021/acs.analchem.6b01466

Cited by 18 publications

(42 citation statements)

References 21 publications

(31 reference statements)

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“…34,35 We used a variant of TOF-SIMS, event-by-event detection mode, that uses individual projectiles to analyze single nanoparticles. 36 The method has two innovative features: (1) the mode of bombardment and recording of the secondary ions and (2) impacting the surface with relatively massive 2 nm projectiles (Au 400 4+ ) that produces abundant secondary ion emissions from the sample. 37 This one-of-a-kind tool is suited for the quantification of the ligand distribution on an individual metal nanoparticle independent of morphology and method of ligand attachment (e.g., covalent or electrostatic bonds).…”

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confidence: 99%

Label Free Particle-by-Particle Quantification of DNA Loading on Sorted Gold Nanostars

et al. 2019

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This paper describes a label free technique for determining ligand loading on metal nanoparticles using a variant of secondary ion mass spectrometry. Au 400 4+ clusters bombard DNAfunctionalized anisotropic gold nanostars and isotropic nanospheres with similar surface areas to determine ligand density. For each projectile impact, co-localized molecules within the emission area of a single impact (diameter of 10-15 nm) were examined for each particle. Individual nanoparticle analysis allows for determination of the relationship between particle geometry and DNA loading. We found that branched particles exhibited increased ligand density versus nanospheres and determined that positive and neutral curvature could facilitate additional loading. This methodology can be applied to optimize loading for any ligand-core interaction independent of nanoparticle core, ligand, or attachment chemistry.

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confidence: 99%

Label Free Particle-by-Particle Quantification of DNA Loading on Sorted Gold Nanostars

et al. 2019

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“…To quantify the relative abundance of CD63 and CD81, we first examined the mass spectra for positive or negative correlations. 37 Briefly, to determine if two ions display a positive or negative correlation, the measured probability of co-detection is divided by the product of their independent detection probabilities (i.e., measured ion yield). A positive correlation (ratio greater than 1) indicates that the two species are co-localized on the surface and a negative correlation (ratio less than 1) indicates that the two species originate from different surface domains.…”

Section: ■ Results and Discussionmentioning

confidence: 99%

“…The abundance of fatty acid co-emitted with F − or I − compared to all measurements (which randomly sample the surface) shows the extent of correlation between tag and fatty acid. 28,37 The correlation coefficients between F − or I − and each fatty acid ion in the nontagged EV sample and tagged EV are listed in Table 4. Additional correlation coefficients are presented in a two-dimensional (2-D) heat map, see Supporting Information Figures S6 and S7.…”

Section: ■ Results and Discussionmentioning

confidence: 99%

“…Surface analysis and mapping of projectile impacts is a custom mass spectrometry data analysis software and was used for mass spectrometry data analysis. 37 Conjugation of Abs to Mass Spectrometry Tags. Abs specific to target proteins were conjugated to halide-containing tags chosen for their high probability of ionization and detection.…”

Section: ■ Materials and Methodsmentioning

confidence: 99%

“…The instrument is operated in the event-by-event bombardment/detection mode, meaning that individual projectile impacts are detected and analyzed separately. Surface analysis and mapping of projectile impacts is a custom mass spectrometry data analysis software and was used for mass spectrometry data analysis …”

Section: Materials and Methodsmentioning

confidence: 99%

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Nanoprojectile Secondary Ion Mass Spectrometry for Analysis of Extracellular Vesicles

et al. 2021

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We describe a technique based on secondary ion mass spectrometry with nanoprojectiles (NP-SIMS) for determining the protein content of extracellular vesicles, EVs, via tagged antibodies. The technique uses individual gold nanoprojectiles (e.g., Au400 4+ and Au2800 8+), separated in time and space, to bombard a surface. For each projectile impact (10–20 nm in diameter), the co-emitted molecules are mass analyzed and recorded as an individual mass spectrum. Examining these individual mass spectra for co-localized species allows for nanoscale mass spectrometry to be performed. The high lateral resolution of this technique is well suited for analyzing nano-objects. SIMS is generally limited to analyzing small molecules (below ∼1500 Da); therefore, we evaluated three molecules (eosin, erythrosine, and BHHTEGST) as prospective mass spectrometry tags. We tested these on a model surface comprising a mixture of all three tags conjugated to antibodies and found that NP-SIMS could detect all three tags from a single projectile impact. Applying the method, we tagged two surface proteins common in urinary EVs, CD63 and CD81, with anti-CD63–erythrosine and anti-CD81–BHHTEGST. We found that NP-SIMS could determine the relative abundance of the two proteins and required only a few hundred or thousand EVs in the analysis region to detect the presence of the tagged antibodies.

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Functional link between plasma membrane spatiotemporal dynamics, cancer biology, and dietary membrane-altering agents

Erazo-Oliveras

Fuentes

Wright

et al. 2018

Cancer Metastasis Rev

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The cell plasma membrane serves as a nexus integrating extra- and intracellular components, which together enable many of the fundamental cellular signaling processes that sustain life. In order to perform this key function, plasma membrane components assemble into well-defined domains exhibiting distinct biochemical and biophysical properties that modulate various signaling events. Dysregulation of these highly dynamic membrane domains can promote oncogenic signaling. Recently, it has been demonstrated that select membrane-targeted dietary bioactives (MTDBs) have the ability to remodel plasma membrane domains and subsequently reduce cancer risk. In this review, we focus on the importance of plasma membrane domain structural and signaling functionalities as well as how loss of membrane homeostasis can drive aberrant signaling. Additionally, we discuss the intricacies associated with the investigation of these membrane domain features and their associations with cancer biology. Lastly, we describe the current literature focusing on MTDBs, including mechanisms of chemoprevention and therapeutics in order to establish a functional link between these membrane-altering biomolecules, tuning of plasma membrane hierarchal organization, and their implications in cancer prevention.

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Testing Molecular Homogeneity at the Nanoscale with Massive Cluster Secondary Ion Mass Spectrometry

Cited by 18 publications

References 21 publications

Label Free Particle-by-Particle Quantification of DNA Loading on Sorted Gold Nanostars

Label Free Particle-by-Particle Quantification of DNA Loading on Sorted Gold Nanostars

Nanoprojectile Secondary Ion Mass Spectrometry for Analysis of Extracellular Vesicles

Functional link between plasma membrane spatiotemporal dynamics, cancer biology, and dietary membrane-altering agents

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