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This article has been featured for the Most Popular Articles 2025 collection in RSC Chemical Science.

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(selected for front cover graphics)

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(KG and AN contributed equally)

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(AK, VSA, and AN contributed equally)

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Highlighted in the LCGC International News

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(Young Scientist Feature and Cover Article in April 2023 issue) - Read the Interview

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(VSA and SM contributed equally)

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Selected for Spotlights in JACS
"Highly Reactive Carbocations Tamed in Water Microdroplets" by Lučka Bibič
J. Am. Chem. Soc. 2021, 143, 7, 2621.

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(AA and SM contributed equally)
Selected for ACS Editors' Choice

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(M.K, S.V, and A.K contributed equally)

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(#E.N.C, S.S, and S.B contributed equally)
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Invited Review Article

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Mass Spectrometry and aggressiveness of cancer. However, because of heterogeneity in tissue morphology, conventional histopathology-based classification of cancer from benign tissue or determination of grade/score of cancer is often subjective, excessively limiting enrollment in active surveillance. Moreover, an unreliable biopsy report often causes unsuccessful cancer surgery by leaving tumor cells at the resected specimen edge, which has been associated in many cancers with increased local recurrence and decreased overall survival. Therefore, driven by the need for trustworthy detection and classification of cancer margin, an accurate molecular assessment of a biopsy specimen has become indispensable. A number of molecular methods including immunohistochemistry and fluorescence in situ hybridization have improved the efficacy of microscopic examination of biopsy specimens. Both these techniques have been widely adopted into the practice of pathology, indicating that molecular analysis has an enormous power to unravel the diagnostic features. Recently, DESI-MSI has been used [3-5] to rapidly evaluate the tissue metabolome at ambient conditions by simultaneously characterizing hundreds of lipids and metabolites. In the last five years, some reports from Zare laboratory (Stanford Chemistry) [4-7] and others [3, 8-9] have demonstrated the usefulness of DESI-MSI in viewing the metabolite/lipid distribution on tissues in the context of cancer and other disease pathologies. Therefore, DESI-MSI has opened a vast possibility to explore in the area of cancer diagnosis and biochemistry, particularly because of the diversity in cancer clinical behaviors driven from tremendous heterogeneity at the molecular level. In addition to that, DESI-MSI can also offer the best hope for maximizing cancer cures without overtreatment involving precision medicine through molecular evaluation of each individual cancer by understanding its biological nature. Global changes in metabolism are hallmark features of neoplasia. Cancer exhibits alterations in lipid metabolism caused by the-A Journey Towards Cancer Diagnosis.

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Accurate identification of prostate cancer in frozen sections at the time of surgery can be challenging, limiting the surgeon’s ability to best determine resection margins during prostatectomy. We performed desorption electrospray ionization mass spectrometry imaging (DESI-MSI) on 54 banked human cancerous and normal prostate tissue specimens to investigate the spatial distribution of a wide variety of small metabolites, carbohydrates, and lipids. In contrast to several previous studies, our method included Krebs cycle intermediates (m/z <200), which we found to be highly informative in distinguishing cancer from benign tissue. Malignant prostate cells showed marked metabolic derangements compared with their benign counterparts. Using the “Least absolute shrinkage and selection operator” (Lasso), we analyzed all metabolites from the DESI-MS data and identified parsimonious sets of metabolic profiles for distinguishing between cancer and normal tissue. In an independent set of samples, we could use these models to classify prostate cancer from benign specimens with nearly 90% accuracy per patient. Based on previous work in prostate cancer showing that glucose levels are high while citrate is low, we found that measurement of the glucose/citrate ion signal ratio accurately predicted cancer when this ratio exceeds 1.0 and normal prostate when the ratio is less than 0.5. After brief tissue preparation, the glucose/citrate ratio can be recorded on a tissue sample in 1 min or less, which is in sharp contrast to the 20 min or more required by histopathological examination of frozen tissue specimens.

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(Highlighted in Nature Reviews Urology; doi:10.1038/nrurol.2017.46)

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We have investigated the gas-phase production of isoquinoline by performing collisional activation on benzalaminoacetal, the first intermediate in the classic solution-phase Pomeranz–Fritsch synthesis of isoquinoline. We have elucidated the reaction pathways in the gas phase using tandem mass spectrometry. Unlike the corresponding condensed-phase reaction, where catalytic proton exchange between intermediate(s) and solvent (Brønsted–Lowry base) is known to drive the reaction, the gas-phase reaction follows the “mobile proton model” to form the products via a number of intermediates, some the same as in their condensed-phase counterparts. Energy-resolved mass spectrometry, deuterium labeling experiments, and theoretical calculations (B3LYP/6-31G**) identified 27 different reaction routes in the gas phase, forming a complex interlinked reaction network. The experimental measurements and theoretical calculations confirm the proton hopping onto different basic sites of the precursors and intermediates to transform them ultimately into isoquinoline.

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(SB and FL contributed equally)

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(SB, YY, and IDJ contributed equally)

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(Selected for back cover graphics, DOI: 10.1039/C7AN90033C)
C&EN mentioned this work
Ranked in the top 5% of highly cited articles in Analyst in 2018

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(SB and SS contributed equally)
ATLAS of Science mentioned this work

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(JKL and SB contributed equally)

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(SG and SB contributed equally)

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Invited Review Article