A Focus Honoring R. Graham Cooks’ Election to the National Academy of Sciences

Focus: Honoring R. G. Cooks' Election to the National Academy of Sciences: Editorial

Keywords

Paper Spray Ambient Mass Spectrometry Desorption Electrospray Ionization Mass Spectrometry Portable Mass Spectrometer Peptide Disulfide Linkage 
These keywords were added by machine and not by the authors. This process is experimental and the keywords may be updated as the learning algorithm improves.
Congratulations to Graham Cooks, a long-time member of the ASMS and a former president of the society, who was recently elected to the National Academy of Sciences of the U.S.A. He joins other eminent American mass spectrometrists, including John Fenn, Fred McLafferty, Klaus Biemann, Carl Djerassi, John Hayes, and Jack Beauchamp in this honor. This JASMS focus of original science articles, contributed by his many protégés, honors his accomplishments.
Table 1

Titles of a selection of RG Cooks papers that have received at least 100 citations

Year

Title

Journal

1969

Bond Formation upon Electron Impact

Org. Mass Spectrom.

1971

Structure and Fragmentation Mechanisms of Organic Ions in Mass Spectrometer

Org. Mass Spectrom.

1973

Design and Performance of a Mass Analyzed Ion Kinetic-Energy (MIKE) Mass Spectrometer

Anal. Chem.

1974

Kinetic-Energy Distributions from Shapes of Metastable Peaks

Proc. Royal Soc. A

1977

Intrinsic Basicity Determination Using Metastable Ions

J. Am. Chem. Soc.

1978

Direct Analysis of Mixtures by Mass Spectrometry

Anal. Chem.

1981

Proton Affinities from Dissociations of Proton-Bound Dimers

J. Am. Chem. Soc.

1982

Mass Spectrometry of Large, Fragile, and Involatile Molecules

Science

1982

Consecutive Reactions in Triple Analyzer Mass Spectrometry and Applications to Mixture Analysis

Anal. Chem.

1987

Mechanisms in Molecular SIMS

Chem. Rev.

1991

Operation of a Quadrupole Ion Trap Mass Spectrometry to Achieve High Mass Charge Ratios

Int. J. Mass Spectrom.

1994

Reactions of Ions with Organic Surfaces

Accts. Chem. Res.

1997

Soft-Landing of Polyatomic Ions at Fluorinated Self-Assembled Monolayer Surfaces

Science

2000

Copper(II)-Assisted Enantiomeric Analysis Of D,L-Amino Acids Using the Kinetic Method: Chiral Recognition and Quantification in the Gas Phase

J. Am. Chem. Soc.

2000

Miniature Mass Analyzers

J. Mass Spectrom.

2001

Collisions of Ions with Surfaces at Chemically Relevant Energies: Instrumentation and Phenomena

Rev. Sci. Instrum.

2001

Chiroselective Self-Directed Octamerization of Serine: Implications for Homochirogenesis

Anal. Chem.

2003

Preparing Protein Microarrays by Soft-Landing of Mass-Selected Ions

Science

2003

Chiral Analysis by MS

Anal. Chem.

2004

Mass Spectrometry Sampling Under Ambient Conditions with Desorption Electrospray Ionization

Science

2004

Rectilinear Ion Trap: Concepts, Calculations, and Analytical Performance of a New Mass Analyzer

Anal. Chem.

2005

Mass Spectrometric Profiling of Intact Biological Tissue by Using Desorption Electrospray Ionization

Angew. Chem.

2005

Ambient Mass Spectrometry Using Desorption Electrospray Ionization (DESI): Instrumentation, Mechanisms, and Applications in Forensics, Chemistry, and Biology

J. Mass Spectrom.

2006

Droplet Dynamics and Ionization Mechanisms in Desorption Electrospray Ionization Mass Spectrometry

Anal. Chem.

2006

Rapid Trace Detection of Triacetone Triperoxide (TATP) by Complexation Reactions During Desorption Electrospray Ionization

Chem. Commun.

2007

Development of Capabilities for Imaging Mass Spectrometry under Ambient Conditions with DESI

Int. J. Mass Spectrom.

2007

Principal Component Analysis of Urine Metabolites Detected by NMR and DESI-MS in Patients with Inborn Errors of Metabolism

Anal. Bioanal. Chem.

2008

Desorption Electrospray Ionization (DESI) Mass Spectrometry and Tandem Mass Spectrometry (MS/MS) of Phospholipids and Sphingolipids: Ionization, Adduct Formation, and Fragmentation

J. Am. Soc. Mass Spectrom.

2008

Desorption Electrospray Ionization Mass Spectrometry: Imaging Drugs and Metabolites in Tissues

Proc Natl. Acad. Sci. U.S.A.

2008

Latent Fingerprint Chemical Imaging by Mass Spectrometry

Science

2010

Paper Spray for Direct Analysis of Complex Mixtures Using Mass Spectrometry

Anal. Chem.

Figure 1

Graham Cooks

Figure 2

R. G. Cooks at ASMS conferences. Top Row: 2015, 2010, 2015; Middle Row: 2014 (with wife Maria Cooks), 2006 (with Gary Glish), 2000; Bottom Row: 2014 (with fellow ASMS Presidents); 2015 (with Bob Murphy and wife Maria). Photos, except ASMS Presidents, by Sue Weintraub

Figure 3

Top Row: Coventry/Warwick for the Jennings/Scrivens 2012 Birthday Celebration. Middle Two Top: with son Barry, End top: with Pat Williams, wife of the late Dudley Williams; Middle Row: with wife Maria in Kyoto IMSC, 2012; Middle and Right: Coventry; Bottom Row: with Nico Nibbering and Helmut Schwarz at the Berlin Wall, 1984; with Alison Ashcroft and Nico Nibbering, Siena Int’l MS School, 2013. Photos by M. L. Gross

Figure 4

At the 2012 William Nichols Award Symposium and banquet, New York, honoring Alan Marshall. Top Right: with Dick Zare; Bottom Right: with Michael Gross, Alan Marshall, and John Baldeschwieler. Photos by M. L. Gross

I have known Graham, or about him, for 48 years. It was during the winter 1968 as a postdoctoral research associate with Fred McLafferty at Purdue University that Fred was helping me locate an academic position. Since I am a Midwesterner, we were restricting considerations to the Midwest. Fred indicated that he knew of a position at Kansas State University, but then he backed away and reported that Kansas State was about to appoint a “star” who had recently finished his second Ph.D. studies at Cambridge in England. This was my first introduction to the name R. Graham Cooks, and “star quality” was and still is correct. I didn’t apply at KSU, for obvious reasons, and some months later accepted my first independent position at the neighboring University of Nebraska-Lincoln.

Later I met Graham, possibly via a seminar invitation or at a Midwest meeting, before he went to Purdue. I am quite sure he reviewed some of my early papers, where he was immensely helpful and supportive, especially important at the start of one’s career. One communication I submitted to J. Am. Chem. Soc. is entitled “The unusually slow loss of hydrogen from ionized 1,5-hexadiyne” (1973) on the esoteric (by today’s standards) subject of the slow decomposition of a benzene isomeric radical cations. I think it was Graham who wrote “this is what a communication should be – an uncluttered description of a novel result.” I always suspected but never knew for sure that Graham was the reviewer, but even if Graham didn’t write this, he would have, had he been asked. Comments like this are of immense importance to young investigators because they are enthusiastic and supportive. One of Graham’s outstanding virtues is to help and support his students, coworkers, and colleagues.

Ideas flowed from his active mind and continued from his early approaches using MS/MS, collisional and surface activation to understand ion structure. More importantly, Graham put his own touch on this area by conducting complex mixture analysis by MS/MS. Everyone from that era recalls his direct MS/MS analysis of coca leaves and strawberry jam, admiring his boldness to eschew chromatography and advocate putting such complex samples in pristine mass spectrometers. This work is a harbinger of his present efforts on direct mixture analysis, ambient ionization, and small mass spectrometers.

Graham has impacted nearly all aspects of our subject. His kinetic method yields physical chemical properties (e.g., proton affinities) of complex molecules, taking as subjects molecules well beyond the ken of the chemical physicists of the day who remained fascinated by detailed measurements of simple hydrocarbons. His invention of desorption electrospray ionization (DESI) has become an important complement to electrospray ionization and an opportunity to do “ambient mass spectrometry.” Then there are “paper spray” and “leaf spray.” Once he formed ions by various approaches, some by his own methods, he contributed considerably to our understanding of collisional activation and to developing surface-induced dissociation. He promoted extensively ion traps and Orbitraps for mass analysis, recognizing more quickly than most of us the importance of these instruments compared with the large magnetic sectors and Fourier transform ion cyclotron resonance (ICR) instruments that captured our imagination in the 1980s and 1990s. His far-sighted interest has continued with the development of miniature mass spectrometers, even those that can fit in a back pack or a surgical operating theater.

To illustrate the subjects to which he has contributed, I decided to look at his citation record to assess what the community has been “saying” about the importance of his work. I reasoned that if colleagues and competitors thought the work was important, they would cite the paper. The following table is the outcome of my survey and lists a subset of his papers that have received at least 100 citations. It is organized from the beginning of his career to the present. A glance at the titles and years show the interesting evolution of his thinking about our subject. A look to the journal titles reveals that he has supported many journals ranging, from high impact general journals to specialist journals in our field. A long-distance view demonstrates his ongoing contributions that have continued for nearly 50 y.

His work, like that of many in his era, begins with the fundamentals of gas-phase ions, their fragmentation, the release of internal energy as kinetic energy, and their collisional activation. This field, of diminishing attention today, follows from the inherently interesting fragmentation of isolated gas-phase ions that underpins mass spectrometry and physical organic chemistry. The mass spectrometer is a “test tube” for ion reactions.

Accompanying these fundamental studies are studies in instrument design and MS/MS – a theme that runs through all of his work in direct sample introduction in the mass spectrometer and the opportunity for direct and later ambient analysis.

Emerging from his fundamental studies is the kinetic method, which is one of the key ways to measure proton affinities, particularly of molecules that are involatile and not suitable for gas-phase equilibrium. Another subject of interest is the analysis of chiral compounds, culminating in his work on serine oligomers. A follow-up on MS/MS is surface-induced dissociation and the fundamentals of ion–surface interactions and “soft landing” experiments.

Recently, ambient ionization mass spectrometry and small, even portable mass spectrometers have occupied his attention. He has developed new ionization approaches (DESI, DESI imaging, paper spray) that set the stage for rapid analysis in simple instrument settings. Accompanying these fundamental and instrumental advances are papers showing applications.

Graham sees opportunities to use mass spectrometers for many problems, even to do organic synthesis and teach organic synthesis with no hoods or solvent disposal. Preparing interesting materials prompted his development of soft landing ideas and related strategies of synthesis. A summary of his work is captured with some references by: http://en.wikipedia.org/wiki/R._Graham_Cooks.

To honor him, the JASMS editors decided on a Focus to which would be invited his former coworkers, both students and postdoctoral researchers, who are in a position to contribute a scientific article. Graham has educated over 125 Ph.D. students, and a large fraction of them are in academic or related settings wherein they can do mass spectrometry research. JASMS captured 20 articles from Graham’s protégés to comprise this Focus Section. In this way, we draw attention not only to his research accomplishments but also to his human legacy of students and coworkers. A listing of the articles is as follows:

Ion Chemistry Developments

  1. 1.

    Online Monitoring of Methanol Electro-Oxidation Reactions by Ambient Mass Spectrometry by Si Cheng, Qiuhua Wu, Howard D. Dewald, Hao Chen

     
  2. 2.

    Formation of Pyrylium from Aromatic Systems with a Helium:Oxygen Flowing Atmospheric-Pressure Afterglow (FAPA) Plasma Source by Sunil P. Badal, Tyree D. Ratcliff, Yi You, Curt M. Breneman, Jacob T. Shelley

     
  3. 3.

    Charge-Tagged N-Heterocyclic Carbenes (NHC): Direct Transfer from Ionic Liquid Solutions and Long-Lived Nature in the Gas Phase by Thyago S. Rodrigues, Denis Lesage, Wender A. da Silva, Richard B. Cole, Günter Ebeling, Jaïrton Dupont, Heibbe C. B. de Oliveira, Marcos N. Eberlin, Brenno A. D. Neto

     
  4. 4.

    Metal Cationization Extractive Electrospray Ionization Mass Spectrometry of Compounds Containing Multiple Oxygens by Kenneth D. Swanson, Sandra E. Spencer, Gary L. Glish

     
  5. 5.

    Gas-Phase Oxidation via Ion/Ion Reactions: Pathways and Applications by Alice L. Pilo, Feifei Zhao, Scott A. McLuckey

     
  6. 6.

    Investigation and Applications of In-Source Oxidation in Liquid Sampling-Atmospheric Pressure Afterglow Microplasma Ionization (LS-APAG) Source by Xiaobo Xie, Zhenpeng Wang, Yafeng Li, Lingpeng Zhan, Zongxiu Nie

     

Instrumentation Developments

  1. 7.

    Analytical Validation of a Portable Mass Spectrometer Featuring Interchangeable, Ambient Ionization Sources for High Throughput Forensic Evidence Screening by Zachary E. Lawton, Angelica Traub, William L. Fatigante, Jose Mancias, Adam E. O’Leary, Seth E. Hall, Jamie R. Wieland, Herbert Oberacher, Michael C. Gizzi, Christopher C. Mulligan

     
  2. 8.

    A Simple Method for Improving the Spatial Resolution in Infrared Laser Ablation Mass Spectrometry Imaging by Juha-Pekka Hieta, Anu Vaikkinen, Samuli Auno, Heikki Räikkönen, Markus Haapala, Gianmario Scotti, Jaakko Kopra, Petteri Piepponen, Tiina J. Kauppila

     
  3. 9.

    High Mass Ion Detection with Charge Detector Coupled to Rectilinear Ion Trap Mass Spectrometer by Avinash A. Patil, Szu-Wei Chou, Pei-Yu Chang, Chen-Wei Lee, Chun-Yen Cheng, Ming-Lee Chu, Wen-Ping Peng

     
  4. 10.

    Isobar Separation in a Multiple-Reflection Time-of-Flight Mass Spectrometer by Mass-Selective Re-Trapping by Timo Dickel, Wolfgang R. Plaß, Wayne Lippert, Johannes Lang, Mikhail I. Yavor, Hans Geissel, Christoph Scheidenberger

     

Applications

  1. 11.

    Laser-Induced Acoustic Desorption/Electron Ionization of Amino Acids and Small Peptides by Tiffany M. Jarrell, Benjamin C. Owen, James S. Riedeman, Boone M. Prentice, Chris J. Pulliam, Hilkka I. Kenttämaa

     
  2. 12.

    Assigning Peptide Disulfide Linkage Pattern among Regio-Isomers via Methoxy Addition to Disulfide and Tandem Mass Spectrometry by Kirt L. Durand, Lei Tan, Craig A. Stinson, Chasity B. Love-Nkansah, Xiaoxiao Ma, Yu Xia

     
  3. 13.

    Ammonium Bicarbonate Addition Improves the Detection of Proteins by Desorption Electrospray Ionization Mass Spectrometry by Elahe Honarvar, Andre R. Venter

     
  4. 14.

    Characterization of Lipid A Variants by Energy-Resolved Mass Spectrometry: Impact of Acyl Chains by Christopher M. Crittenden, Lucas D. Akin, Lindsay J. Morrison, M. Stephen Trent, Jennifer S. Brodbelt

     
  5. 15.

    Estimating the Efficiency Of Phosphopeptide Identification by Tandem Mass Spectrometry by Chuan-Chih Hsu, Liang Xue, Justine V. Arrington, Pengcheng Wang, Juan Sebastian Paez, Yuan Zhou, Jian-Kang Zhu, W. Andy Tao

     
  6. 16.

    Monitoring Toxic Ionic Liquids in Zebrafish (Danio rerio) with Desorption Electrospray Ionization Mass Spectrometry Imaging (DESI-MSI) by Consuelo J. Perez, Alessandra Tata, Michel L. de Campos, Chun Peng, Demian R. Ifa

     
  7. 17.

    MS/MS-Assisted Design of Sequence-Controlled Synthetic Polymers for Improved Reading of Encoded Information by Laurence Charles, Gianni Cavallo, Valérie Monnier, Laurence Oswald, Roza Szweda, Jean-François Lutz

     
  8. 18.

    Characterization of ZnO Nanoparticles Using Superconducting Tunnel Junction Cryodetection Mass Spectrometry by Logan D. Plath, Zongyu Wang, Jiajun Yan, Krzysztof Matyjaszewski, Mark E. Bier

     
  9. 19.

    Detection of Metastatic Breast and Thyroid Cancer in Lymph Nodes by Desorption Electrospray Ionization Mass Spectrometry Imaging by Jialing Zhang, Clara Feider, Chandandeep Nagi, Wendong Yu, Stacey A. Carter, James Suliburk, Hop S. Tran Cao, Livia S. Eberlin

     
  10. 20.

    Ambient Ionization Mass Spectrometry Measurement of Aminotransferase Activity by Xin Yan, Xin Li, Chengsen Zhang, Yang Xu, R. Graham Cooks

     

Congratulations, Graham, on your election to the U.S. National Academy of Sciences. The ASMS is proud of your accomplishments and history and pleased to regard you as a friend, coworker, and colleague.

Michael L. Gross

Washington University in St. Louis

Department of Chemistry

St. Louis, MO, USA

mgross@wustl.edu

Notes

Acknowledgments

PS. I wish to thank the editorial group of JASMS with their help in reviewing these articles.

Copyright information

© American Society for Mass Spectrometry 2017

Authors and Affiliations

  1. 1.Department of ChemistryWashington University in St. LouisSt. LouisUSA

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