MICROSCOPIC KINETIC MODEL EXHIBITING CHIRAL SYMMETRY BREAKING Harold W. Hatch, Pablo G. Debenedetti Chemical Engineering Dept., Princeton Frank H. Stillinger.

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Presentation transcript:

MICROSCOPIC KINETIC MODEL EXHIBITING CHIRAL SYMMETRY BREAKING Harold W. Hatch, Pablo G. Debenedetti Chemical Engineering Dept., Princeton Frank H. Stillinger Chemistry Dept., Princeton Acknowledgement: Prof. Donna G. Blackmond, Imperial College, London, and The Scripps Research Institute, La Jolla, CA Financial Support: NSF Collaborative Research in Chemistry Grant ACS Presentation F.H. Stillinger View 1

MOTIVATING MYSTERIES Biological molecules (proteins, DNA, carbohydrates,....) occur overwhelmingly with chiral subunits that exhibit only one of the two possible mirror image forms. How did this broken geometric symmetry arise? Is the spontaneous appearance of life and its subsequent evolution possible only in such a symmetry-broken chemical environment? How far must one search in the universe to find C,N,O,H based life with the opposite chirality? ACS Presentation F.H. Stillinger View 2

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POSSIBLE MECHANISMS (1) Parity-violating weak interactions (2) Illumination with circularly polarized light (3) D,L phase diagram characteristics: enantiomorphic excess amplification resulting from off-symmetry eutectic pairs (4) Mechanically disturbed crystallization with slow liquid-phase D,L interconversion, and "Ostwald ripening" (5) Liquid-phase chemical kinetics with autocatalysis and inhibition ACS Presentation F.H. Stillinger View 4

TWO-DIMENSIONAL LATTICE MODEL Square lattice, two achiral reactants A and B B Rigid chiral reaction products B B and B B A A "Empty" sites represent inert solvent Random nearest-neighbor diffusive jumps before and after reaction ACS Presentation F.H. Stillinger View 5

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CONCLUDING REMARKS Although not present in the model investigated, hydrodynamic convection or mechanical stirring would magnify the effectiveness of inhibition. Conversion of lattice model to a continuum model is feasible, but technically complicated. Chemical reaction reversibility can be included. One possible aspect would be to allow two molecules of the same chirality to bind to (i.e., "gang up on") one molecule of the opposite chirality and cause it to revert to its unbonded precursor reactants. ACS Presentation F.H. Stillinger View 17