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Ultrafast processes in molecules

Ultrafast processes in molecules. X – Case studies of dynamics simulations. Mario Barbatti barbatti@kofo.mpg.de. Case 1: Aminopyrimidine. Aminopyrimidine. Can the Nonadiabatic Photodynamics of Aminopyrimidine Be a Model for the Ultrafast Deactivation of Adenine?. No!.

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Ultrafast processes in molecules

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  1. Ultrafast processes in molecules X – Case studies of dynamics simulations Mario Barbatti barbatti@kofo.mpg.de

  2. Case 1: Aminopyrimidine

  3. Aminopyrimidine Can the Nonadiabatic Photodynamics of Aminopyrimidine Be a Model for the Ultrafast Deactivation of Adenine? No! • Barbatti and Lischka, J Phys Chem A 111, 2852 (2007)

  4. Restricted aminopyrimidine Can the Nonadiabatic Photodynamics of Aminopyrimidine Be a Model for the Ultrafast Deactivation of Adenine? Hum, Maybe !? 1000 amu • Barbatti and Lischka, J Phys Chem A 111, 2852 (2007)

  5. Surface hopping: dynamics example • Nachtigallova, Zeleny, Ruckenbauer, Muller, Barbatti, Hobza, Lischka, JACS 132, 8261 (2010)

  6. Case 2: Azobenzene

  7. Phototrigger

  8. Dynamics • Pederzoli, Pittner, Barbatti, Lischka,J Phys ChemA 115, 11136 (2011)

  9. Dihedral evolution

  10. Chirality

  11. Biased initial conditions Initial velocities biased towards positive projection of the clockwise direction • Pederzoli, Pittner, Barbatti, Lischka,J Phys ChemA 115, 11136 (2011)

  12. Case 3: Cr(CO)6

  13. Cr(CO)6 method assessment O C Cr CC • Crespo-Otero, Barbatti,J Chem Phys 134, 164305 (2011)

  14. Cr(CO)6photochemistry Energy O C Cr Time • Kosma, Trushin, Fuss, Schmid, Schneider, PCCP 12, 13197 (2010) • Crespo-Otero, Barbatti,J Chem Phys 134, 164305 (2011)

  15. Case 4: Formamide

  16. Formamide photolysis 193 nm NH2 + COH Gas phase 193 nm NH3 ••• CO Ar matrix 193 nm H2 + NCOH Xe matrix • Lundell, Krajewska, Rasanen, J Phys Chem A102, 6643 (1998)

  17. Formamide in Ar matrix • QM: formamide • CASSCF(10,8)/6-31G* • MM: Ar matrix • 661 atoms • 18 K • OPLSAA force field • Dynamics • 100 trajectories • 2 ps • 0.5 fs step • Eckert-Maksic, Vazdar, Ruckenbauer, Barbatti, Muller, Lischka, PCCP 12, 12719 (2010)

  18. Formamide in Ar matrix (22%) ..... ..... (15%) * (16%) …. > 2ps 0.5 ps ? (47%) > 2ps 0.5 ps + ? 1 ps > 2ps 2 ps ? • Eckert-Maksic, Vazdar, Ruckenbauer, Barbatti, Muller, Lischka, PCCP 12, 12719 (2010)

  19. Formamide in Ar matrix • Eckert-Maksic, Vazdar, Ruckenbauer, Barbatti, Muller, Lischka, PCCP 12, 12719 (2010)

  20. Me-formamide in the gas phase • Crespo-Otero, Mardyukov, Sanchez-Garcia, Barbatti, Sander, • ChemPhysChem14, 827 (2013)

  21. Case 5: Prebiotic reactions

  22. Prebiotic route for nucleotides • Ferris, Orgel, JACS 88, 1074 (1966) • Powner, Sutherland, Szostak, JACS 132, 16677 (2010)

  23. Computational chemistry in action QM/MM: hot 4HCN in water RRKM Dynamics and Chemical Kinetics revealed the only possible route

  24. Photochem in prebiotic synthesis 4HCN purine nucleotides • Boulanger, Anoop, Nachtigallova, Thiel, MB, ACIE 52, 8000 (2013)

  25. Next lecture: • Surface hopping with single reference methods www.youtube.com/user/mbarbatti Contact barbatti@kofo.mpg.de

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