@article{FuechselTremblayKlamrothetal.2013,
  author    = {F{\"u}chsel, Gernot and Tremblay, Jean Christophe and Klamroth, Tillmann and Saalfrank, Peter},
  title     = {Quantum dynamical simulations of the femtosecond-laser-induced ultrafast desorption of H2 and D2 from Ru(0001)},
  series = {ChemPhysChem : a European journal of chemical physics and physical chemistry},
  volume    = {14},
  journal   = {ChemPhysChem : a European journal of chemical physics and physical chemistry},
  number    = {7},
  publisher = {Wiley-VCH},
  address   = {Weinheim},
  issn      = {1439-4235},
  doi       = {10.1002/cphc.201200940},
  pages     = {1471 -- 1478},
  year      = {2013},
  abstract  = {We investigate the recombinative desorption of hydrogen and deuterium from a Ru(0001) surface initiated by femtosecond laser pulses. We adopt a quantum mechanical two-state model including three molecular degrees of freedom to describe the dynamics within the desorption induced by electronic transition (DIET) limit. The energy distributions as well as the state-resolved and ensemble properties of the desorbed molecules are analyzed in detail by using the time-energy method. Our results shed light on the experimentally observed 1) large isotopic effects regarding desorption yields and translational energies and 2) the nonequal energy partitioning into internal and translational modes. In particular, it is shown that a single temperature is sufficient to characterize the energy distributions for all degrees of freedom. Further, we confirm that quantization effects play an important role in the determination of the energy partitioning.},
  language  = {en}
}
@article{FuechselTremblayKlamrothetal.2012,
  author    = {F{\"u}chsel, Gernot and Tremblay, Jean Christophe and Klamroth, Tillmann and Saalfrank, Peter},
  title     = {Selective excitation of molecule-surface vibrations in H2 and D2 dissociatively adsorbed on Ru(0001)},
  series = {Israel journal of chemistry},
  volume    = {52},
  journal   = {Israel journal of chemistry},
  number    = {5},
  publisher = {Wiley-VCH},
  address   = {Weinheim},
  issn      = {0021-2148},
  doi       = {10.1002/ijch.201100097},
  pages     = {438 -- 451},
  year      = {2012},
  abstract  = {In this contribution we report about the selective vibrational excitation of H2 and D2 on Ru(0001) as an example for nonadiabatic coupling of an open quantum system to a dissipative environment. We investigate the possibility of achieving state-selective vibrational excitations of H2 and D2 adsorbed on a Ru(0001) surface using picosecond infrared laser pulses. The systems behavior is explored using pulses that are rationally designed and others that are optimized using a time-local variant of Optimal Control Theory. The effects of dissipation on the laser-driven dynamics are studied using the reduced-density matrix formalism. The non-adiabatic couplings between adsorbate and surface are computed perturbatively, for which our recently introduced state-resolved anharmonic rate model is used. It is shown that mode- and state-selective excitation can be achieved in the absence of dissipation when using optimized laser pulses. The inclusion of dissipation in the model reduces the state selectivity and the population transfer yield to highly excited states. In this case, mode activation is most effectively realized by a rational pulse of carefully chosen duration rather than by a locally optimized pulse.},
  language  = {en}
}