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  • Articles  (3)
  • American Institute of Physics (AIP)  (3)
  • 1995-1999  (3)
  • Physics  (3)
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  • Articles  (3)
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  • 1
    Electronic Resource
    Electronic Resource
    Real time observation of hydrogen transfer: Femtosecond time-resolved photoelectron spectroscopy in the excited ammonia dimer (1999)
    College Park, Md. : American Institute of Physics (AIP)
    The Journal of Chemical Physics 111 (1999), S. 633-642 
    Details
    ISSN: 1089-7690
    Source: AIP Digital Archive
    Topics: Physics , Chemistry and Pharmacology
    Notes: The energy flow in ammonia dimers excited to the electronic A˜ state is analyzed by combining the femtosecond pump–probe technique and the photoelectron–photoion coincidence detection. We use ∼140 fs laser pulses (200 nm for excitation and 267 nm for ionization). For the dimer ion the photoelectron spectra change drastically from a rather broad shape ((approximately-greater-than)1 eV) at small delay times between pump and probe pulse to a rather narrow peak (0.25 eV) at some picoseconds. This is explained by the dynamics of an internal H-atom transfer in the electronic A˜ state to an NH4...NH2 configuration. The measured photoelectron energies are consistent with ab initio potential energy surface calculations. The observed picosecond lifetime of the hydrogen-transfer state NH4...NH2 can be understood by a conical intersection with the charge-transfer state NH4+...NH2−. © 1999 American Institute of Physics.
    Type of Medium: Electronic Resource
    URL: http://dx.doi.org/10.1063/1.479343
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  • 2
    Electronic Resource
    Electronic Resource
    Ultrafast internal conversion and photodissociation of molecules excited by femtosecond 155 nm laser pulses (1999)
    College Park, Md. : American Institute of Physics (AIP)
    The Journal of Chemical Physics 111 (1999), S. 6264-6270 
    Details
    ISSN: 1089-7690
    Source: AIP Digital Archive
    Topics: Physics , Chemistry and Pharmacology
    Notes: The dynamics of several prototypical molecular systems after excitation with femtosecond laser pulses at 155 nm has been studied in pump–probe experiments. The vacuum ultraviolet (VUV) pump pulses with a pulse width of 350–450 fs were generated by near-resonant four-wave difference frequency mixing in argon. The careful analysis of the time-dependent ion signals has allowed us to determine the lifetime of the excited molecular states down to about 30 fs. The extremely short lifetime of water molecules excited to the repulsive A˜ state has been directly observed for the first time: τD≤20 fs. For molecular oxygen highly excited in the Schumann–Runge band, a decay time of 40±20 fs was obtained. The lifetimes of ethylene and chloroethylenes as well as of benzene and toluene reaching from 40 up to 180 fs are primarily caused by internal conversion. The decay times τD=(1.9±0.1) and τD=(90±20) ps obtained for carbon disulfide and nitric oxide, respectively, are due to predissociation of the VUV excited states. © 1999 American Institute of Physics.
    Type of Medium: Electronic Resource
    URL: http://dx.doi.org/10.1063/1.479932
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  • 3
    Electronic Resource
    Electronic Resource
    Ultrafast predissociation and coherent phenomena in CS2 excited by femtosecond laser pulses at 194–207 nm (1999)
    College Park, Md. : American Institute of Physics (AIP)
    The Journal of Chemical Physics 111 (1999), S. 5338-5343 
    Details
    ISSN: 1089-7690
    Source: AIP Digital Archive
    Topics: Physics , Chemistry and Pharmacology
    Notes: The ultrafast predissociation dynamics of CS2 molecules excited to the 1B2(1Σu+) electronic state by femtosecond laser pulses with 6.0–6.4 eV photon energy has been studied in pump–probe experiments. The analysis of the time-dependent ion signals has revealed lifetimes decreasing from 620 fs down to 180 fs for tuning the excitation wavelength from 207 nm to 194 nm. A nearly constant plateau at about 200 nm in the energy dependence of the lifetime reflects the barrier of the transition from the bent to a quasilinear geometry of the excited CS2 molecule. If two vibrational bands of the 1B2(1Σu+) state were excited simultaneously by the femtosecond laser pulses we observed quantum beats with a modulation frequency corresponding to the energy difference of the two modes. Thus, the coherent excitation process is directly visualized despite the ultrafast decay of the excited molecular states due to predissociation. © 1999 American Institute of Physics.
    Type of Medium: Electronic Resource
    URL: http://dx.doi.org/10.1063/1.479793
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