W. Andrzej SOKALSKI 教授 特別講演会

Intermolecular interactions determine numerous practically important physical and chemical properties of biomolecules with parameters considerably exceeding synthetic materials[1]. Due to the large size of biomolecular systems they are still studied by very crude methods, employing mostly empirical force fields or in the best case by supermolecular variational methods which can not provide any insight into the physical nature of corresponding interactions. However, such data can be obtained now using variation-perturbation partitioning of intermolecular interaction energy into electrostatic, exchange, delocalization and correlation terms for relatively large molecular systems (up to about 100 atoms)[2].

This methodology allowed us to analyze from the first principles of quantum mechanics the physical nature of active site interactions with inhibitors [3-4] or reactants [5] for several enzymes, as well as interactions involving nucleic acids [6] and zeolites [7]. Moreover, these components define entire hierarchy of gradually simplified theoretical models, which can be effectively used in rational design of new molecular materials ? catalysts, drugs, etc.

One of such models - Differential Transition State Stabilization (DTSS) approach [8] describes catalytic activity of molecular environment allowing to determine the most important residues and energy contributions involved. Wherever electrostatic effects are dominant, these results can be generalized in the form of catalytic fields [5,8] aiding rational catalyst design. Corresponding examples related to enzyme systems [5] nucleic acids [9] will be presented and possible dynamic effects discussed.

1. W.A. Sokalski(ed), Molecular Materials with Specific Interactions: Modeling and Design, Vol. 4, Series: Challenges and Advances in Computational Chemistry and Physics, Springer 2007.
2. W.A. Sokalski, S. Roszak, K. Pecul, Chem.Phys.Lett., 153,153 (1988).
3. E. Dyguda-Kazimierowicz, J. Grembecka, W. A. Sokalski, J. Leszczynski, J. Am. Chem. Soc. 127 (6), 1658-1659 (2005).
4. R. Grzywa, E. Dyguda-Kazimierowicz, M. Sie?czyk, M. Feliks, W. A. Sokalski, J. Oleksyszyn, J.Mol.Model., 13, 677 (2007).
5. B. Szefczyk, A.J. Mulholland, K.E. Ranaghan, W.A. Sokalski, J.Am.Chem.Soc., 126, 16148 (2004).
6. K. M. Langner, P. K?dzierski, W. A. Sokalski, J. Leszczynski, J. Phys. Chem. B 110 (19), 9720-9727 (2006).
7. P. Dzieko?ski, W. A. Sokalski, B. Szyja, J. Leszczynski, Chem. Phys. Lett. 364 (1-2), 133-138 (2002)
8. W.A. Sokalski, J.Mol.Catalysis,30, 395 (1985).
9. L. Gorb, Y. Podolyan, P. Dziekonski, W.A. Sokalski, J. Leszczynski, J.Am.Chem.Soc., 126, 10119 (2004).