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Perspective Patel, Cole, Bradshaw et al.


8 Trim PJ, Francese S, Clench MR. Imaging mass spectrometry for the assessment of drugs and metabolites in tissue. Bioanalysis 1(2), 309–319 (2009).


9 Gessel MM, Norris JL, Caprioli RM. MALDI imaging mass spectrometry: spatial molecular analysis to enable a new age of discovery. J. Proteomics 107, 71–82 (2014).


10 Trim PJ, Djidja MC, Muharib T et al. Instrumentation and software for mass spectrometry imaging‐‐making the most of what you’ve got. J. Proteomics. 75(16), 4931–4940 (2012).


11 Ellis SR, Brown SH, In Het Panhuis M, Blanksby SJ, Mitchell TW. Surface analysis of lipids by mass spectrometry: more than just imaging. Prog. Lipid Res. 52(4), 329–353 (2013).


12 Kafka AP, Kleffmann T, Rades T, McDowell A. The application of MALDI TOF MS in biopharmaceutical research. Int. J. Pharm. 417(1–2), 70–82 (2011).


13 Troendle FJ, Reddick CD, Yost RA. Detection of pharmaceutical compounds in tissue by matrix-assisted laser desorption/ionization and laser desorption/chemical ionization tandem mass spectrometry with a quadrupole ion trap. J. Am. Soc. Mass Spectrom. 10(12), 1315–1321 (1999).


14 Reyzer ML, Hsieh Y, Ng K, Korfmacher WA, Caprioli RM. Direct analysis of drug candidates in tissue by matrix-assisted laser desorption/ionization mass spectrometry. J. Mass Spectrom. 38(10), 1081–1092 (2003).


15 Stoeckli M, Staab D, Schweitzer A. Compound and metabolite distribution measured by MALDI mass spectrometric imaging in whole-body tissue sections. Int. J. Mass Spectrom. 260(2–3), 195–202 (2007).


16 Khatib-Shahidi S, Andersson M, Herman JL, Gillespie TA, Caprioli RM. Direct molecular analysis of whole-body animal tissue sections by imaging MALDI mass spectrometry. Anal. Chem. 78(18), 6448–6456 (2006).


17 Fournier I, Wisztorski M, Salzet M. Tissue imaging using MALDI-MS: a new frontier of histopathology proteomics. Expert Rev. Proteomics 5(3), 413–424 (2008).


18 Groseclose MR, Andersson M, Hardesty WM, Caprioli RM. Identification of proteins directly from tissue: in situ tryptic digestions coupled with imaging mass spectrometry. J. Mass Spectrom. 42(2), 254–262 (2007).


19 Shimma S, Furuta M, Ichimura K, Yoshida Y, Setou M. A novel approach to in situ proteome analysis using chemical inkjet printing technology and MALDI-QIT-TOF tandem mass spectrometer. J. Mass Spectrom. Soc. Jpn 54(4), 133–140 (2006).


20 Lemaire R, Desmons A, Tabet JC, Day R, Salzet M, Fournier I. Direct analysis and MALDI imaging of formalin-fixed, paraffin-embedded tissue sections. J. Proteome Res. 6(4), 1295–1305 (2007).


21 Schwamborn K. Imaging mass spectrometry in biomarker discovery and validation. J. Proteomics 75(16), 4990–4998 (2012).


22 Prideaux B, Stoeckli M. Mass spectrometry imaging for drug distribution studies. J. Proteomics 75(16), 4999–5013 (2012).


23 Nilsson A, Fehniger TE, Gustavsson L et al. Fine mapping the spatial distribution and concentration of unlabeled drugs within tissue micro-compartments using imaging mass spectrometry. PLoS ONE 5(7), e11411 (2010).


24 Marko-Varga G, Végvári A, Rezeli M et al. Understanding drug uptake and binding within targeted disease micro- environments in patients: a new tool for translational medicine. Clin. Transl. Med. 1(1), 8–9 (2012).


25 Cole LM, Djidja MC, Bluff J et al. Investigation of protein induction in tumour vascular targeted strategies by MALDI MSI. Methods 54(4), 442–453 (2011).


26 Atkinson SJ, Loadman PM, Sutton C, Patterson LH, Clench MR. Examination of the distribution of the bioreductive drug AQ4N and its active metabolite AQ4 in solid tumours by imaging matrix-assisted laser desorption/ionisation mass spectrometry. Rapid Commun. Mass Spectrom. 21(7), 1271–1276 (2007).


27 van Kampen JJ, Burgers PC, de Groot R, Gruters RA, Luider TM. Biomedical application of MALDI mass spectrometry for small-molecule analysis. Mass Spectrom. Rev. 30(1), 101–120 (2011).


28 Munteanu B, Meyer B, von Reitzenstein C et al. Label- free in situ monitoring of histone deacetylase drug target engagement by matrix-assisted laser desorption ionization-mass spectrometry biotyping and imaging. Anal. Chem. 86(10), 4642–4647 (2014).


•• The monitoring of drug-induced mass shifts in protein ion fingerprints/images directly corresponding to histone post- transcriptional modifications is a novel pharmacodynamic approach for analyzing engagement of drug targets and intact cell responses via MALDI-MS.


29 Djidja MC, Claude E, Snel MF et al. Novel molecular tumour classification using MALDI-mass spectrometry imaging of tissue micro-array. Anal. Bioanal. Chem. 397(2), 587–601 (2010).


• Potentially a high-throughput method for the classification and interrogation of pancreatic cancer tissue by analyzing formalin-fixed paraffin-embedded tissue microarrays. This would be advantages in a clinical setting.


30 Demichelis F, Magni P, Piergiorgi P, Rubin MA, Bellazzi R. A hierarchical Naive Bayes Model for handling sample heterogeneity in classification problems: an application to tissue microarrays. BMC Bioinformatics 7, 514 (2006).


31 Battifora H, Mehta P. The checkerboard tissue block. An improved multitissue control block. Lab. Invest. 63(5), 722–724 (1990).


32 Kononen J, Bubendorf L, Kallioniemi A et al. Tissue microarrays for high-throughput molecular profiling of tumor specimens. Nat. Med. 4(7), 844–847 (1998).


33 Abd El-Rehim DM, Ball G, Pinder SE et al. High- throughput protein expression analysis using tissue microarray technology of a large well-characterised series identifies biologically distinct classes of breast cancer confirming recent cDNA expression analyses. Int. J. Cancer 116(3), 340–350 (2005).


34 Djidja MC, Francese S, Claude E et al. Targeting of hypoxia in AQ4N-treated tumour xenografts by MALDI-ion mobility separation–mass spectrometry imaging. Curr. Anal. Chem. (9), 212–225 (2013).


35 Cole LM, Bluff JE, Carolan VA, Paley MN, Tozer GM, Clench MR. MALDI-MSI and label-free LC-ESI-MS/


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