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Aufsatz
Femtosecond probing of sodium cluster ion Na_n ^+ fragmentation
(1992)
We report on the first femtosecond time-resolved experiments in cluster physics. The photofragmentation
dynamics of small sodium cluster ions Na_n ^+ have been studied with pump-probe techniques. Ultrashort
laser pulses of 60-fs duration are employed to photoionize the sodium clusters and to probe the
photofragments. We find that the ejection of neutral dimer Na_2 and, observed for the first time, neutral
trimer Na_3 photofragments occur on ultrashort time scales of 2.5 and 0.4 ps, respectively. This and the
absence ...
Aufsatz
Femtosecond time-resolved molecular multiphoton ionization: the Na_2 system
(1991)
We report here the first experimental study of femtosecond time-resolved molecular multiphoton ionization.
Femtosecond pump-probe techniques are combined with time-of-flight spectroscopy to measure
transient ionization spectra of Na_2 in a molecular-beam experiment. The wave-packet motions in
different molecular potentials show that incoherent contributions from direct photoionization of a singly
excited state and from excitation and autoionization of a bound doubly excited molecular state determine
the observed ...
Aufsatz
Femtosecond pump-probe study of the spreading and recurrence of a vibrational wave packet in Na_2
(1992)
The motion of a vibrational wave packet in the bound A(^1 \summe^+_u) electronic state of the sodium dimer is detected in a femtosecond pump/probe molecular beam experiment. For short times harmonic motion is seen in the total ion yield of Na^+_2 as a function of delay time between the two laser pulses. The spreading of the wave packet results in the loss of the periodic variation of the ion signal. For longer delay times (47 ps) the wave packet regains its initial form which is reflected in the revival structure of ...
Aufsatz
Femtosecond spectroscopy of molecular autoionization and fragmentation
(1990)
Femtosecond laser pulses are applied to the study of the dynamics and the pathways of multiphoton-induced ionization, autoionization, and fragmentation of Na_2 in molecular-beam experiments. In particular,
we report on first results obtained studying electronic autoionization (leading to Na_2{^+} + {e ^-}) and
autoionization-induced fragmentation (leading to Na{^+} + Na + {e ^-}) of a bound doubly excited molecular state. The final continuum states are analyzed by photoelectron spectroscopy and by measuring the ...
Aufsatz
Femtosecond real-time probing of reactions. 12. Vectorial dynamics of transition states
(1993)
Femtosecond time-resolved techniques with KETOF (kinetic energy time-of-flight) detection in a molecular beam are developed for studies of the vectorial dynamics of transition states. Application to the dissociation reaction of IHgI is presented. For this system, the complex [I---Hg---I](++)* is unstable and, through the symmetric and asymmetric stretch motions, yields different product fragments: [I---Hg---I](++)* -> HgI(X^2/sigma^+) + I(^2P_3/2) [or I*(^2P_l/2)] (1a); [I---Hg---I](++)* -> Hg(^1S_0) + I(^2P_3/2) + ...
Aufsatz
Femtosecond real-time probing of reactions
(1993)
Femtosecond reaction dynamics of OClO in a supersonic molecular beam are reported. The system is excited to the A^2A_2 state with a femtosecond pulse, covering a range of excitation in the symmetric stretch between v_1 = 17 to v_1 = 11 (308-352 nm). A time-delayed femtosecond probe pulse ionizes the OClO, and OClO^+ is detected. This ion has not been observed in previous experiments because of its ultrafast fragmentation. Transients are reported for the mass of the parent OClO as well as the mass of the ClO. Apparent ...
Aufsatz
Femtosecond time-resolved molecular multiphoton ionization and fragmentation of Na_2
(1993)
We present a comparison between experimental and theoretical results for pump/probe multiphoton ionizing transitions of the sodium dimer, initiated by femtosecond laser pulses. It is shown that the motion of vibrational wavepackets in two electronic states is probed simultaneously and their dynamics is reflected in the total Na^+_2 ion signal which is recorded as a function of the time delay between pump and probe pulse. The time dependent quantum calculations demonstrate that two ionization pathways leading to the ...
Aufsatz
Femtosecond two-photon ionization spectroscopy of the B state of Na_3 clusters
(1993)
We report time-resolved experiments studying the dynamics of the Na_3 B-X system. Femtosecond pump-probe techniques combined with ion time-of-flight (TOF) and zero kinetic energy (ZEKE) photoelectron spectroscopy allow us to observe the three-dimensional wavepacket motion in the excited Na_3 B state and in the Na_3 X state. The ground state wavepacket is induced by stimulated emission pumping during the pump pulse. The X-state dynamics is dominated by the three vibrational modes of the Na_3. Furthermore we observed ...
Aufsatz
Molecular photochemistry with femtosecond laser pulses
(1990)
Femtosecond laser pulses generated from an amplified coiliding pulse modelocked ring dye laser have been employed in molecular beam experiments to study the dynamics and the pathways of multiphoton induced ionization, autoionization and fragmentation of Na2 . Energy distributions of photoelectrons arising from these processes and the mass and released kinetic energy of the corresponding fragment ions are measured by time-of-flight spectroscopy.