| Fragmentation and reactivity in collisions of protonated diglycine with chemically modified perfluorinated alkylthiolate-self-assembled monolayer surfaces. | |
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MedLine Citation:
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PMID: 21384949 Owner: NLM Status: In-Data-Review |
Abstract/OtherAbstract:
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Direct dynamics simulations are reported for quantum mechanical (QM)/molecular mechanical (MM) trajectories of N-protonated diglycine (gly(2)-H(+)) colliding with chemically modified perfluorinated octanethiolate self-assembled monolayer (SAM) surfaces. The RM1 semiempirical theory is used for the QM component of the trajectories. RM1 activation and reaction energies were compared with those determined from higher-level ab initio theories. Two chemical modifications are considered in which a head group (-COCl or -CHO) is substituted on the terminal carbon of a single chain of the SAM. These surfaces are designated as the COCl-SAM and CHO-SAM, respectively. Fragmentation, peptide reaction with the SAM, and covalent linkage of the peptide or its fragments with the SAM surface are observed. Peptide fragmentation via concerted CH(2)-CO bond breakage is the dominant pathway for both surfaces. HCl formation is the dominant species produced by reaction with the COCl-SAM, while for the CHO-SAM a concerted H-atom transfer from the CHO-SAM to the peptide combined with either a H-atom or radical transfer from the peptide to the surface to form singlet reaction products is the dominant pathway. A strong collision energy dependence is found for the probability of peptide fragmentation, its reactivity, and linkage with the SAM. Surface deposition, i.e., covalent linkage between the surface and the peptide, is compared to recent experimental observations of such bonding by Laskin and co-workers [Phys. Chem. Chem. Phys. 10, 1512 (2008)]. Qualitative differences in reactivity are seen between the COCl-SAM and CHO-SAM showing that chemical identity is important for surface reactivity. The probability of reactive surface deposition, which is most closely analogous to experimental observables, peaks at a value of around 20% for a collision energy of 50 eV. |
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Authors:
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George L Barnes; Kelsey Young; Li Yang; William L Hase |
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Publication Detail:
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Type: Journal Article |
Journal Detail:
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Title: The Journal of chemical physics Volume: 134 ISSN: 1089-7690 ISO Abbreviation: J Chem Phys Publication Date: 2011 Mar |
Date Detail:
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Created Date: 2011-03-09 Completed Date: - Revised Date: - |
Medline Journal Info:
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Nlm Unique ID: 0375360 Medline TA: J Chem Phys Country: United States |
Other Details:
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Languages: eng Pagination: 094106 Citation Subset: IM |
Affiliation:
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Department of Chemistry and Biochemistry, Texas Tech University, Lubbock, Texas 79409, USADepartment of Chemistry and Biochemistry, Abilene Christian University, Abilene, Texas 79699, USA. |
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From MEDLINE®/PubMed®, a database of the U.S. National Library of Medicine
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