108 research outputs found
Electron gun for diffraction experiments off controlled molecules
A dc electron gun, generating picosecond pulses with up to
electrons per pulse, was developed. Its applicability for future
time-resolved-diffraction experiments on state- and conformer-selected
laser-aligned or oriented gaseous samples was characterized. The focusing
electrodes were arranged in a velocity-map imaging spectrometer configuration.
This allowed to directly measure the spatial and velocity distributions of the
electron pulses emitted from the cathode. The coherence length and pulse
duration of the electron beam were characterized by these measurements combined
with electron trajectory simulations. Electron diffraction data off a thin
aluminum foil illustrated the coherence and resolution of the electron-gun
setup
Spatially-controlled complex molecules and their applications
The understanding of molecular structure and function is at the very heart of
the chemical and molecular sciences. Experiments that allow for the creation of
structurally pure samples and the investigation of their molecular dynamics and
chemical function have developed tremendously over the last few decades,
although "there's plenty of room at the bottom" for better control as well as
further applications.
Here, we describe the use of inhomogeneous electric fields for the
manipulation of neutral molecules in the gas-phase, \ie, for the separation of
complex molecules according to size, structural isomer, and quantum state. For
these complex molecules, all quantum states are strong-field seeking, requiring
dynamic fields for their confinement. Current applications of these controlled
samples are summarised and interesting future applications discussed.Comment: Accepted by Int. Rev. Phys. Che
Ultrafast light-induced dynamics in solvated biomolecules: The indole chromophore with water
Interactions between proteins and their solvent environment can be studied in
a bottom-up approach using hydrogen-bonded chromophore-solvent clusters. The
ultrafast dynamics following UV-light-induced electronic excitation of the
chromophores, potential radiation-damage, and their dependence on solvation are
important open questions. The microsolvation effect is challenging to study due
to the inherent mix of the produced gas-phase aggregates. We used the deflector
to spatially separate different molecular species in combination with
pump-probe velocity-map-imaging experiments. We demonstrated that this powerful
experimental approach reveals intimate details of the UV-induced dynamics in
the near-UV-absorbing prototypical biomolecular indole-water system. We
determined the time-dependent appearance of the different reaction products and
disentangled the occurring ultrafast processes. This novel approach ensures
that the reactants are well-known and that detailed characteristics of the
specific reaction products are accessible -- paving the way for the complete
chemical-reactivity experiment
Strongly aligned and oriented molecular samples at a kHz repetition rate
We demonstrate strong adiabatic laser alignment and mixed-field orientation
at kHz repetition rates. We observe degrees of alignment as large as
cos\Theta=0.94 at 1 kHz operation for iodobenzene. The experimental setup
consist of a kHz laser system simultaneously producing pulses of 30 fs (1.3 mJ)
and 450 ps (9 mJ). A cold 1 K state-selected molecular beam is produced at the
same rate by appropriate operation of an Even-Lavie valve. Quantum state
selection has been obtained using an electrostatic deflector. A camera and data
acquisition system records and analyzes the images on a single-shot basis. The
system is capable of producing, controlling (translation and rotation) and
analyzing cold molecular beams at kHz repetition rates and is, therefore,
ideally suited for the recording of ultrafast dynamics in so-called "molecular
movies".Comment: 6 pages, 4 figures, in press in Mol. Phys., accepted in February
2013, in final production (galley proofs done) since March 8, 2013, v3 only
adds publication dat
Two-state wave packet for strong field-free molecular orientation
We demonstrate strong laser-field-free orientation of absolute-ground-state
carbonyl sulfide molecules. The molecules are oriented by the combination of a
485-ps-long non-resonant laser pulse and a weak static electric field. The
edges of the laser pulse create a coherent superposition of two rotational
states resulting in revivals of strong transient molecular orientation after
the laser pulse. The experimentally attained degree of orientation of 0.6
corresponds to the theoretical maximum for mixing of the two states. Switching
off the dc field would provide the same orientation completely field-free
Knife edge skimming for improved separation of molecular species by the deflector
A knife edge for shaping a molecular beam is described to improve the spatial
separation of the species in a molecular beam by the electrostatic deflector.
The spatial separation of different molecular species from each other as well
as from atomic seed gas is improved. The column density of the selected
molecular-beam part in the interaction zone, which corresponds to higher signal
rates, was enhanced by a factor of 1.5, limited by the virtual source size of
the molecular beam.Comment: 3 pages, 2 figure
Molecular movie of ultrafast coherent rotational dynamics of OCS
Recording molecular movies on ultrafast timescales has been a longstanding goal for unravelling detailed information about molecular dynamics. Here we present the direct experimental recording of very-high-resolution and -fidelity molecular movies over more than one-and-a-half periods of the laser-induced rotational dynamics of carbonylsulfide (OCS) molecules. Utilising the combination of single quantum-state selection and an optimised two-pulse sequence to create a tailored rotational wavepacket, an unprecedented degree of field-free alignment, 〈cos2θ2D〉 = 0.96 (〈cos2θ〉 = 0.94) is achieved, exceeding the theoretical limit for single-pulse alignment. The very rich experimentally observed quantum dynamics is fully recovered by the angular probability distribution obtained from solutions of the time-dependent Schrödinger equation with parameters refined against the experiment. The populations and phases of rotational states in the retrieved time-dependent three-dimensional wavepacket rationalises the observed very high degree of alignment
Spatial separation of pyrrole and pyrrole-water clusters
We demonstrate the spatial separation of pyrrole and pyrrole(HO) clusters
from the other atomic and molecular species in a supersonically-expanded beam
of pyrrole and traces of water seeded in high-pressure helium gas. The
experimental results are quantitatively supported by simulations. The obtained
pyrrole(HO) cluster beam has a purity of ~100 %. The extracted rotational
temperature of pyrrole and pyrrole(HO) from the original supersonic
expansion is K, whereas the temperature of the
deflected, pure-pyrrole(HO) part of the molecular beam corresponds to
K
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