Leiden University, Theoretical Chemistry (LEI)

Principal investigator: 
Geert-Jan Kroes


The goal of the research of the Leiden Theoretical Chemistry group is to predict the dynamics of chemical reactions (mechanisms, outcomes) on the basis of first principles. Kroes has expertise in the use of quantum dynamical methods for molecule-surface reactions [62, 63] and transition state theory [64], and Olsen in the use of electronic structure methods [65], transition state theory, and saddle-point searchers. The Leiden group is a world leading group in quantum dynamics of molecule-surface reactions, having been the first to perform full-dimensional quantum dynamical calculations of activated dissociation of H2 [66] and HD [67] on metal surfaces. The group has now shifted its focus to research on production and storage of hydrogen. Frankcombe, Díaz, and Marashdeh are now performing research on hydrogen storage [68-70], and Olsen and Qu on production of hydrogen [71].

Facilities and infrastructure

The group owns three Beowulfclusters for its computational research, two 32 dual-processor node machines (192 and 170 Gflop/s, respectively), and one 18 dual-processor node machine (61 Gflop/s) which will be replaced with a 200+ Gflop/s computer in the autumn of 2006. The group also has access to three national Dutch supercomputers (TERAS, 1 Tflop/s; ASTER, 2.2 Tflop/s; LISA, 3 Gflop/s), the current yearly grant is 1.2 million TERAS hours, equivalent to a computational capacity of 130 Gflop/s.

Training and tutoring capacity

Kroes and Olsen have extensive experience with supervising and tutoring ESRs and ERs, and teach several courses at the MSc/PhD level that will be useful for the ESR and ER (such as "Dynamics of molecule-surface reactions", "Quantum chemistry"). Kroes is co-developing a MSc/Phd course entitled "Science for the Hydrogen Economy". Leiden is an ideal environment for research on hydrogen, with a modernised chemistry curriculum called "Molecular Science and Technology" which has as one of its BSc tracks "Sustainable Molecular Science and Technology". The presence of several post-docs and of a Ph.D. student in the group already performing research on production and storage of hydrogen will facilitate transfer of knowledge to the ESR and ER who will work in the group.

Experience with international collaboration

Kroes is the coordinator of the Research Training Network "Predicting catalysis" in which Nørskov, Clary, and Jónsson are partners, and which will end in June 2006. The old network focuses on catalysis for ammonia production, which is intimately linked with hydrogen production. Concepts relevant to heterogeneous catalysis will also play an important role in our new research on hydrogen. Of the current PIs, Kroes collaborates and has published with Jónsson, Clary [72], Züttel [68], and Nørskov [73].

Key publications

  • P. Nieto, E. Pijper, D. Barredo, G. Laurent, R. A. Olsen, E.J. Baerends, G.J. Kroes, and D. Farías, Reactive and non-reactive scattering of H2 from a metal surface is electronically adiabatic, Science, 9 February 2006 (10.1126/science.1123057).
  • G.J. Kroes, A. Gross, E.J. Baerends, M. Scheffler, and D.A. McCormack, Quantum theory of dissociative chemisorption on metal surfaces, Acc. Chem. Res. 35, 193 (2002).
  • R.A. Olsen, G.J. Kroes, G. Henkelman, A. Arnoldssen, and H. Jónsson, Comparison of methods for finding saddle points without knowledge of final states, J.Chem.Phys. 121, 9776 (2004).


45. R.A. Olsen, G.J. Kroes, G. Henkelman, A. Arnaldsson, and H. Jónsson, J.Chem.Phys. 121, 9776 (2004).
55. E. Pijper, G.J. Kroes, R.A. Olsen, and E.J. Baerends, J. Chem. Phys. 117, 5885 (2002).
63. D. Farías, C. Díaz, P. Rivière, H.F. Busnengo, P. Nieto, M.F. Somers, G.J. Kroes, A. Salin, and F. Martín, Phys.Rev.Lett. 93, 246104 (2004).
64. R. Valero and G.J. Kroes, J. Chem. Phys. 117, 8736 (2002).
65. R.A. Olsen, H.F. Busnengo, A. Salin, M.F. Somers, G.J. Kroes, and E.J. Baerends, J. Chem. Phys. 116, 3841 (2002).
66. G.J. Kroes, E.J. Baerends, and R.C. Mowrey, Phys.Rev.Lett. 78, 3583 (1997).
67. S.M. Kingma, M.F. Somers, E. Pijper, G.J. Kroes, R.A. Olsen, and E.J. Baerends, J. Chem. Phys. 118, 4190 (2003).
68. T.J. Frankcombe, G.J. Kroes, and A. Züttel, Chem.Phys.Lett. 405, 73 (2005).
69. T.J. Frankcombe, G.J. Kroes, N.I. Choly, and E. Kaxiras, J.Phys.Chem.B 109, 16554 (2005).
70. A. Marashdeh, R.A. Olsen, O.M. Løvvik, and G.J. Kroes, Chem.Phys.Lett. submitted (2006).
71. Z.W. Qu and G.J. Kroes, J.Phys.Chem.B submitted (2006).
72. D.C. Clary and G.J. Kroes, in Scattering, edited by P. Sabatier and E. R. Pike (Academic, London, 2002).
73. C. Díaz, J.K. Vincent, G.P. Krishnamohan, R.A. Olsen, K. Honkala, J.K. Nørskov, and G.J. Kroes, Phys.Rev.Lett. in press (2006).