- Mass Spectrometry Techniques and Applications
- Metabolomics and Mass Spectrometry Studies
- Analytical Chemistry and Chromatography
- Advanced Proteomics Techniques and Applications
- Ion-surface interactions and analysis
- Isotope Analysis in Ecology
- Lipid Membrane Structure and Behavior
- Clostridium difficile and Clostridium perfringens research
- Alkaloids: synthesis and pharmacology
- Analytical chemistry methods development
- Chemical Synthesis and Analysis
- X-ray Diffraction in Crystallography
- Crystallization and Solubility Studies
- Bacterial Identification and Susceptibility Testing
- Organometallic Complex Synthesis and Catalysis
- Traditional and Medicinal Uses of Annonaceae
- Gut microbiota and health
- Pesticide Residue Analysis and Safety
- Adipose Tissue and Metabolism
- Eicosanoids and Hypertension Pharmacology
- Microfluidic and Capillary Electrophoresis Applications
- Nuclear Physics and Applications
- Radiation Effects in Electronics
- Coordination Chemistry and Organometallics
- Electrohydrodynamics and Fluid Dynamics
University of Florida
2019-2024
Vanderbilt University
2015-2020
Vanderbilt University Medical Center
2018
RELX Group (United States)
2017
Purdue University West Lafayette
2010-2017
Longwood University
2009
CD8+ T cells are master effectors of antitumor immunity, and their presence at tumor sites correlates with favorable outcomes. However, metabolic constraints imposed by the microenvironment (TME) can dampen ability to control progression. We describe lipid accumulation in TME areas pancreatic ductal adenocarcinoma (PDA) populated infiltrating both murine human tumors. In this lipid-rich but otherwise nutrient-poor TME, access using metabolism becomes particularly valuable for sustaining cell...
Abstract Microorganisms form biofilms containing differentiated cell populations. To determine factors driving differentiation, we herein visualize protein and metal distributions within Pseudomonas aeruginosa using imaging mass spectrometry. These in vitro experiments reveal correlations between differential distribution abundance. Notably, zinc- manganese-depleted portions of the biofilm repress production anti-staphylococcal molecules. Exposure to calprotectin (a host known sequester ions...
A matrix‐assisted laser desorption/ionization time of flight/time flight tandem mass spectrometer (MALDI TOF/TOF) has been used for high‐speed precursor/fragment ion transition image acquisition. High‐throughput analysis is facilitated by an Nd:YLF solid state capable pulse repetition rates up to 5 kHz, a high digitizer acquisition rate (up 50 pixels/s), and continuous raster sampling. MS/MS experiments are enabled through the use precision timed selector, second source acceleration,...
The exposure of electrospray droplets to acid vapors can significantly affect protein charge state distributions (CSDs) derived from unbuffered solutions. Such experiments have been conducted by leaking acidic into the counter-current nitrogen drying gas an interface. On basis changes in CSDs, folding and unfolding phenomena are implicated these studies. Additionally, noncovalently bound complexes preserved, transient intermediates observed, such as high ions holomyoglobin. CSDs proteins...
Matrix-assisted laser desorption/ionization imaging mass spectrometry (MALDI IMS) allows for the visualization of molecular distributions within tissue sections. While providing excellent specificity and spatial information, absolute quantification by MALDI IMS remains challenging. Especially in low weight region spectrum, analysis is complicated matrix interferences ionization suppression. Though tandem (MS/MS) can be used to ensure chemical improve sensitivity eliminating noise, typical...
Multimodal mass spectrometric imaging identifies bacterial and host analytes in intact tissues during invasive infection mice.
Abstract The specific matrix used in matrix‐assisted laser desorption/ionization imaging mass spectrometry (MALDI IMS) can have an effect on the molecules ionized from a tissue sample. sensitivity for distinct classes of biomolecules vary when employing different MALDI matrices. Here, we compare intensities various lipid subclasses measured by Fourier transform ion cyclotron resonance (FT‐ICR) IMS murine liver using 9‐aminoacridine (9AA), 5‐chloro‐2‐mercaptobenzothiazole (CMBT),...
Lipids and metabolites are of interest in many clinical research settings because it is the metabolome that increasingly recognized as a more dynamic sensitive molecular measure phenotype. The enormous diversity lipid structures importance biological structure-function relationships wide variety applications makes accurate identification challenging yet crucial area community. Indeed, subtle differences chemical lipids can have important implications cellular metabolism disease pathologies....
Mass spectrometry imaging (MSI) is an important analytical technique that simultaneously reports the spatial location and abundance of detected ions in biological, chemical, clinical, pharmaceutical studies. As MSI grows popularity, it has become evident data reporting varies among different research groups between techniques. The lack consistency inherently creates additional challenges comparing intra- inter-laboratory data. In this tutorial, we propose a unified system, SMART, based on...
The chemical complexity of biological tissues creates challenges in the analysis lipids via imaging mass spectrometry. presence isobaric and isomeric compounds introduces noise that makes it difficult to unambiguously identify accurately map spatial distributions these compounds. Electron-induced dissociation (EID) has previously been shown profile phosphatidylcholine (PCs) sn-isomers directly from rat brain tissue matrix-assisted laser desorption/ionization (MALDI) However, acquisition true...
Accurate structural identification of lipids in imaging mass spectrometry is critical to properly contextualizing spatial distributions with tissue biochemistry. Gas-phase charge inversion ion/ion reactions alter the ion type prior dissociation allow for more structurally informative fragmentation and improve lipid at isomeric level. In this work, infrared multiphoton (IRMPD) was interfaced a commercial hybrid Qh-FT-ICR spectrometer enable rapid gas-phase reaction products every pixel...
The diverse array of chemical compounds present in tissue samples results many isobaric (i.e., same nominal mass) imaging mass spectrometry experiments. Adequate separation and differentiation these is necessary to ensure accurate analyte identification avoid composite images comprising multiple compounds. High-resolution (HRAM) measurements are able resolve some instances, but HRAM not always feasible depending on the instrument platform desired experimental time scale. Alternatively,...
Abstract The use of mass spectrometry (MS) to acquire molecular images biological tissues and other substrates has developed into an indispensable analytical tool over the past 25 years. Imaging technologies are widely used today study in situ spatial distributions for a variety analytes. Early MS were acquired using secondary ion matrix‐assisted laser desorption/ionization. Researchers have also designed ionization techniques recent years probe surfaces generate images, including desorption...
Gas-phase ion/ion reactions are emerging as useful and flexible means for the manipulation characterization of peptide protein biopolymers. Acid/base-like chemical (i.e., proton transfer reactions) reduction/oxidation (redox) electron represent relatively mature classes gas-phase reactions. Even so, especially in regards to redox chemistry, widespread utility these two types chemistries is undergoing rapid growth development. Additionally, a new class transformations which involves selective...
The molecular identification of species interest is an important part imaging mass spectrometry (IMS) experiment. high resolution accurate capabilities Fourier transform ion cyclotron resonance (FT-ICR MS) have recently been shown to facilitate the proteins in matrix-assisted laser desorption/ionization (MALDI) IMS. However, these experiments are typically limited giving rise ions relatively low m/ z due difficulties transmitting and measuring large weight charge states. Herein we modified...
Gas-phase ion/ion reactions have been enabled on a commercial dual source, hybrid QhFT-ICR mass spectrometer for use during imaging spectrometry experiments. These allow the transformation of ion type most readily generated from tissue surface to an that gives improved chemical structural information upon tandem (MS/MS) without manipulating sample. This process is demonstrated via charge inversion reaction phosphatidylcholine (PC) lipid cations rat brain matrix-assisted laser...
Extended similarity indices facilitate processing complex IMS data and quickly finding correlations between multiple compounds tissue regions.
Accurate structural determination of proteins is critical to understanding their biological functions and the impact disruption on disease progression. Gas-phase cross-linking mass spectrometry (XL-MS) via ion/ion reactions between multiply charged protein cations singly cross-linker anions has previously been developed obtain low-resolution information proteins. This method significantly shortens experimental time relative conventional solution-phase XL-MS but several technical limitations:...
An understanding of how cells respond to perturbation is essential for biological applications; however, most approaches profiling cellular response are limited in scope pre-established targets. Global analysis molecular mechanism will advance our the complex networks constituting and lead advancements areas, such as infectious disease pathogenesis, developmental biology, pathophysiology, pharmacology, toxicology. We have developed a high-throughput multiomics platform comprehensive, de novo...