Organisers

• Nikos Doltsinis (Ruhr-Universit\)
• Sara Bonella (Dip. Di Fisica, Universita' di Roma )

Supports

 CECAM

 SimBioMa

 COST - MolSimu

Description

This workshop will address the challenge of simulating realistic photoactivated processes of interest in biology and materials science [1,2,3]. These phenomena usually involve non-adiabatic transitions among the electronic states of the system induced by the coupled motion of electronic and nuclear degrees of freedom. Consequently, their simulation requires both accurate ab initio calculations of the (many) electronic states of the system and of the couplings among them and the non-adiabatic time evolution of its components. Although several approaches have been developed recently to tackle these problems [4,5,6,7,8], the techniques currently available are generally either not efficient or not accurate enough to provide a reliable tool to study photophysical processes in complex systems (see proposal for further details).

The workshop will bring together experts from the fields of ab initio quantum chemistry and non-adiabatic dynamics calculations to provide an opportunity for the two communities to join forces and accelerate progress towards reliable theoretical studies of photoactivated phenomena. Current approaches to non-adiabatic ab initio molecular dynamics will be examined and compared to assess their strengths and weaknesses. Novel approaches will also be presented and their potential with respect to realistic applications assessed, both in terms of accuracy and efficiency.

Scientific Objectives

The main scientific objective of the workshop is to accelerate progress towards reliable theoretical studies of complex photoactivated processes of relevance, for instance, to biology or materials science. Complementary goals that will be pursued with that intent can be summarized as follows:

(1) identify more clearly the specific issues, both theoretical and numerical, representing the bottlenecks for ab initio nonadiabatic dynamics;

(2) assess the relative merits of available algorithms;

(3) explore possible improvements in the combined treatment of the electronic structure problem and of the description of nonadiabatic dynamical effects;

(4) encourage the interaction and exchange of information among the electronic structure calculation and nonadiabatic dynamics communities.

References

[1] A. H. Zewail Femtochemistry: Ultrafast Dynamics of the ChemicalBond edited by ed., World Scientific Singapore (1994)

[2] M. Klessinger and J. Michl Excited States and Photochemistry of Organic Molecules edited by ed., VCH New York (1995)

[3] C. E. Crespo-Hernandez, B. Cohen, P. M. Hare and B. Kohler , Chem. Rev. 104 1977 (2004)

[4] N. L. Doltsinis and D. Marx , J. Theor. Comp. Chem. 1 319-349 (2002)

[5] W. Domcke, D. R. Yarkony and H. Koppel Conical Intersections: Electronic Structure, Dynamics and Spectroscopy edited by ed., World Scientific, Singapore (2004)

[6] M. A. Robb, M. Garavelli, M. Olivucci and F. Bernardi , Rev. Comp. Ch. 15 87 (2000)

[7] D. F. Coker and S. Bonella, Linearized Path Integral Methods for quantum correlation functions in Computer Simulations in Condensed Matter: From Materials to Chemical Biology, (2006)

[8] G. Stock and M. Thoss , Adv. Chem. Phys. 131 243-375 (2005)