Concerted and sequential proton transfer mechanisms in water-separated acid-base encounter pairs

Journal of Physical Chemistry Letters

Volumn 3, Issue 18, 2012, Pages 2633-2637

  Thomas, Vibin ^a   Rivard, Ugo ^a   Maurer, Patrick ^a   Bruhács, Andrew ^b   Siwick, Bradley J ^b   Iftimie, Radu ^a  

^a UNIVERSITÉ DE MONTRÉAL   (Canada)

^b MCGILL UNIVERSITY   (Canada)

Author keywords

Kinetics and Dynamics

Indexed keywords

AB INITIO MOLECULAR DYNAMICS; ACID BASE; BULK TRANSFER; CONCERTED MECHANISM; DONOR AND ACCEPTOR; ENCOUNTER COMPLEX; EXCITED-STATE PROTON TRANSFER; MODEL FRAMEWORK; MOLECULAR LEVELS; PICOSECONDS; PROTON-TRANSFER MECHANISM; TIME-RESOLVED; TRANSFER PATHWAY; ULTRAFAST SPECTROSCOPY; WATER MOLECULE;

HYDROGEN BONDS; MOLECULAR DYNAMICS; PHENOLS; SEPARATION;

PROTON TRANSFER;

EID: 84866596481     PISSN: None     EISSN: 19487185     Source Type: Journal    
DOI: 10.1021/jz3012639     Document Type: Article

References (30)

1. Nibbering, E. T.; Pines, E. In Hydrogen-Transfer Reactions; Hynes, J. T., Klinman, J. P., Limbach, H. H., Schowen, R. L., Eds.; Wiley-VCH: New York, 2007; pp 443 - 458; Vol. 1.
2. Kiefer, P. M.; Hynes, J. T. In Hydrogen-Transfer Reactions; Hynes, J. T., Klinman, J. P., Limbach, H. H., Schowen, R. L., Eds.; Wiley-VCH: New York, 2007; pp 303-348; Vol. 1.
3. Eigen, M. Proton Transfer, Acid-Base Catalysis, and Enzymatic Hydrolysis. Part I: Elementary Processes Angew. Chem., Int. Ed 1964, 3 (1) 1-19
4. Marcus, R. A. Electron Transfer Reactions in Chemistry: Theory and Experiment (Nobel Lecture) Angew. Chem., Int. Ed. 1993, 32 (8) 1111-1121
5. Genosar, L.; Cohen, B.; Huppert, D. Ultrafast Direct Photoacid-Base Reaction J. Phys. Chem. A 2000, 104 (29) 6689-6698
6. Cohen, B.; Huppert, D. Non-Exponential Smoluchowski Dynamics in Fast Acid-Base Reaction J. Am. Chem. Soc. 2000, 122 (40) 9838-9839
7. Rini, M.; Magnes, B. Z.; Pines, E.; Nibbering, E. T. J. Real-Time Observation of Bimodal Proton Transfer in Acid-Base Pairs in Water Science 2003, 301, 349-352
8. Mohammed, O. F.; Pines, D.; Dreyer, J.; Pines, E.; Nibbering, E. T. J. Sequential Proton Transfer Through Water Bridges in Acid-Base Reactions Science 2005, 310, 83-86
9. Mohammed, O. F.; Pines, D.; Nibbering, E. T. J.; Pines, E. Base-Induced Solvent Switches in Acid-Base Reactions Angew. Chem., Int. Ed. 2007, 46, 1458-1461
10. Siwick, B. J.; Bakker, H. J. On the Role of Water in Intermolecular Proton-Transfer Reactions J. Am. Chem. Soc. 2007, 129, 13412-13420
11. Siwick, B. J.; Cox, M. J.; Bakker, H. J. Long-Range Proton Transfer in Aqueous Acid-Base Reactions J. Phys. Chem. B 2008, 112, 378-389
12. Cox, M. J.; Timmer, R. L. A.; Bakker, H. J.; Park, S.; Agmon, N. Distance-Dependent Proton Transfer along Water Wires Connecting Acid-Base Pairs J. Phys. Chem. A 2009, 113, 6599-6606
13. Marx, D.; Hutter, J. Ab Initio Molecular Dynamics; Cambridge University Press: New York, 2009.
14. Maurer, P.; Iftimie, R. Combining Ab Initio Quantum Mechanics with a Dipole-Field Model to Describe Acid Dissociation Reactions in Water: First-Principles Free Energy and Entropy Calculations J. Chem. Phys. 2010, 132, 074112-074116
15. Maurer, P.; Thomas, V.; Rivard, U.; Iftimie, R. a Computational Study of Ultrafast Acid Dissociation and Acid-Base Neutralization Reactions. I. The Model J. Chem. Phys. 2010, 133, 044108
16. Maurer, P.; Thomas, V.; Iftimie, R. a Computational Study of Ultrafast Acid Dissociation and Acid-base Neutralization Reactions. II. The Relationship between the Coordination State of Solvent Molecules and Concerted versus Sequential Acid Dissociation J. Chem. Phys. 2011, 134, 094505-094513
17. Spry, D. B.; Fayer, M. D. Charge Redistribution and Photoacidity: Neutral versus Cationic Photoacids J. Chem. Phys. 2008, 128, 084508
18. Mohammed, O. F.; Pines, D.; Pines, E.; Nibbering, E. T. J. Aqueous Bimolecular Proton Transfer in Acid-base Neutralization Chem. Phys. 2007, 341, 240-257
19. Hynes, J. T. The Peripatetic Proton Nature 2007, 446, 270-273
20. Staib, A.; Borgis, D.; Hynes, J. T. Proton Transfer in Hydrogen-Bonded Acid-base Complexes in Polar Solvents J. Chem. Phys. 1995, 102, 2487
21. Ando, K.; Hynes, J. T. Molecular Mechanism of HF Acid Ionization in Water: An Electronic Structure-Monte Carlo Study J. Phys. Chem. A 1999, 103, 10398-10408
22. Leiderman, P.; Genosar, L.; Huppert, D. Excited-State Proton Transfer: Indication of Three Steps in the Dissociation and Recombination Process J. Phys. Chem. A 2005, 109, 5965
23. Marx, D.; Tuckerman, M. E.; Hutter, J.; Parrinello, M. The Nature of the Hydrated Excess Proton in Water Nature 1999, 397, 601-604
24. Marx, D. Proton Transfer 200 Years after von Grotthuss: Insights from Ab Initio Simulations ChemPhysChem 2006, 7, 1848-1870
25. Markovitch, O.; Chen, H.; Izvekov, S.; Paesani, F.; Voth, G. A.; Agmon, N. Special Pair Dance and Partner Selection: Elementary Steps in Proton Transport in Liquid Water J. Phys. Chem. B 2008, 112, 9456-9466
26. 397, 601-604.
27. CPMD V3; IBM Corp 1990-2006, MPI für Festkörperforschung Stuttgart 1997-2001. www.cpmd.org.
28. Becke, A. D. Density-Functional Exchange-Energy Approximation with Correct Asymptotic Behavior Phys. Rev. A 1988, 38, 3098-3100
29. Lee, C. T.; Yang, W. T.; Parr, R. G. Development of the Colle-Salvetti Conelation Energy Formula into a Functional of the Electron Density Phys. Rev. B 1988, 37, 785-789
30. Troullier, N.; Martins, J. L. Efficient Pseudopotentials for Plane-Wave Calculations Phys. Rev. B 1991, 43, 1993-2006