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Aufsatz
Direct evidence for radiative charge transfer after inner-shell excitation and ionization of large clusters
(2018-01-16)
We directly observe radiative charge transfer (RCT) in Ne clusters by dispersed vacuum-ultraviolet photon detection. The doubly ionized Ne^2+ – Ne_n-1 initial states of RCT are populated after resonant 1s–3p photoexcitation or 1s photoionization of Ne_n clusters with {n} \approx 2800. These states relax further producing Ne^+ – Ne^+ – Ne_n-2 final states, and the RCT photon is emitted. Ab initio calculations assign the observed RCT signal to the Ne^2+(2p^-2 [^1D]) - Ne_n-1 initial state, while transitions from other ...
Aufsatz
Circular Dichroism in Fluorescence Emission Following the C 1s→π* Excitation and Resonant Auger Decay of Carbon Monoxide
(2018-06-26)
Dichroism in angle-resolved spectra of circularly polarized fluorescence from freely-rotating CO molecules was studied experimentally and theoretically. For this purpose, carbon monoxide in the gas phase was exposed to circularly polarized soft X-ray synchrotron radiation. The photon energy was tuned across the C 1s→π* resonant excitation, which decayed via the participator Auger transition into the CO+ A 2Π state. The dichroic parameter β1 of the subsequent CO+ (A 2Π → X 2Σ+) visible fluorescence was measured by ...
Aufsatz
Spatio-temporal resolution studies on a highly compact ultrafast electron diffractometer
(2015)
Time-resolved diffraction with femtosecond electron pulses has become a promising technique to directly provide insights into photo induced primary dynamics at the atomic level in molecules and solids. Ultrashort pulse duration as well as extensive spatial coherence are desired, however, space charge effects complicate the bunching of multiple electrons in a single pulse.Weexperimentally investigate the interplay between spatial and temporal aspects of resolution limits in ultrafast electron diffraction (UED) on our ...
Aufsatz
Detecting ultrafast interatomic electronic processes in media by fluorescence
(In: New journal of physics. - London : IOP, 2014, 16, 102002, 1-9, 2014)
Interatomic coulombic decay (ICD), a radiationless transition in weakly bonded systems, such as solutes or van der Waals bound aggregates, is an effective source for electrons of low kinetic energy. So far, the ICD processes could only be probed in ultra-high vacuum by using electron and/or ion spectroscopy. Here we show that resonant ICD processes can also be detected by measuring the subsequently emitted characteristic fluorescence radiation, which makes their study in dense media possible.
Aufsatz
Asymptotic model for shape resonance control of diatomics by intense non-resonant light: universality in the single-channel approximation
(2015)
Non-resonant light interacting with diatomics via the polarizability anisotropy couples different
rotational states and may lead to strong hybridization of the motion. The modification of shape
resonances and low-energy scattering states due to this interaction can be fully captured by an
asymptotic model, based on the long-range properties of the scattering (Crubellier et al 2015 New J.
Phys. 17 045020). Remarkably, the properties of the field-dressed shape resonances in this asymptotic
multi-channel description ...
Aufsatz
Asymptotic model for shape resonance control of diatomics by intense non-resonant light
(2015)
We derive a universal model for atom pairs interacting with non-resonant light via the polarizability
anisotropy, based on the long range properties of the scattering. The corresponding dynamics can be
obtained using a nodal line technique to solve the asymptotic Schrödinger equation. It consists of
imposing physical boundary conditions at long range and vanishing the wavefunction at a position
separating the inner zone and the asymptotic region. We show that nodal lines which depend on the
intensity of the ...
Aufsatz
Femtosecond wavepacket interferometry using the rotational dynamics of a trapped cold molecular ion
(2015)
A Ramsey-type interferometer is suggested, employing a cold trapped ion and two time-delayed offresonant
femtosecond laser pulses. The laser light couples to the molecular polarization anisotropy,
inducing rotational wavepacket dynamics. An interferogram is obtained from the delay dependent
populations of the final field-free rotational states. Current experimental capabilities for cooling and
preparation of the initial state are found to yield an interferogram visibility of more than 80%. The
interferograms can ...