| 1. |
- Kuepper, Jochen, et al.
(författare)
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X-Ray Diffraction from Isolated and Strongly Aligned Gas-Phase Molecules with a Free-Electron Laser
- 2014
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Ingår i: Physical Review Letters. - 0031-9007 .- 1079-7114. ; 112:8, s. 083002-
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Tidskriftsartikel (refereegranskat)abstract
- We report experimental results on x-ray diffraction of quantum-state-selected and strongly aligned ensembles of the prototypical asymmetric rotor molecule 2,5-diiodobenzonitrile using the Linac Coherent Light Source. The experiments demonstrate first steps toward a new approach to diffractive imaging of distinct structures of individual, isolated gas-phase molecules. We confirm several key ingredients of single molecule diffraction experiments: the abilities to detect and count individual scattered x-ray photons in single shot diffraction data, to deliver state-selected, e.g., structural-isomer-selected, ensembles of molecules to the x-ray interaction volume, and to strongly align the scattering molecules. Our approach, using ultrashort x-ray pulses, is suitable to study ultrafast dynamics of isolated molecules.
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| 2. |
- Boll, Rebecca, et al.
(författare)
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Imaging molecular structure through femtosecond photoelectron diffraction on aligned and oriented gas-phase molecules
- 2014
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Ingår i: Faraday Discussions. - : Royal Society of Chemistry (RSC). - 1364-5498. ; 171, s. 57-80
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Tidskriftsartikel (refereegranskat)abstract
- This paper gives an account of our progress towards performing femtosecond time-resolved photoelectron diffraction on gas-phase molecules in a pump-probe setup combining optical lasers and an X-ray free-electron laser. We present results of two experiments aimed at measuring photoelectron angular distributions of laser-aligned 1-ethynyl-4-fluorobenzene (C8H5F) and dissociating, laser-aligned 1,4-dibromobenzene (C6H4Br2) molecules and discuss them in the larger context of photoelectron diffraction on gas-phase molecules. We also show how the strong nanosecond laser pulse used for adiabatically laser-aligning the molecules influences the measured electron and ion spectra and angular distributions, and discuss how this may affect the outcome of future time-resolved photoelectron diffraction experiments.
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| 3. |
- Ertel, Dominik, et al.
(författare)
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Influence of nuclear dynamics on molecular attosecond photoelectron interferometry
- 2023
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Ingår i: Science Advances. - 2375-2548. ; 9:35
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Tidskriftsartikel (refereegranskat)abstract
- In extreme ultraviolet spectroscopy, the photoionization process occurring in a molecule due to the absorption of a single photon can trigger an ultrafast nuclear motion in the cation. Taking advantage of attosecond photoelectron interferometry, where the absorption of the extreme ultraviolet photon is accompanied by the exchange of an additional infrared quantum of light, one can investigate the influence of nuclear dynamics by monitoring the characteristics of the photoelectron spectra generated by the two-color field. Here, we show that attosecond photoelectron interferometry is sensitive to the nuclear response by measuring the two-color photoionization spectra in a mixture of methane (CH4) and deuteromethane (CD4). The effect of the different nuclear evolution in the two isotopologues manifests itself in the modification of the amplitude and contrast of the oscillations of the photoelectron peaks. Our work indicates that nuclear dynamics can affect the coherence properties of the electronic wave packet emitted by photoionization on a time scale as short as a few femtoseconds.
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| 4. |
- Ranitovic, Predrag, 1974-
(författare)
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Time-Resolved Attosecond Spectroscopy of He Using COLTRIMS
- 2008
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Doktorsavhandling (övrigt vetenskapligt/konstnärligt)abstract
- Tunable ultrafast lasers are becoming a standard tool for probing and controlling the dynamics of atoms, molecules and chemical reactions. This thesis is a contribution to a large, ongoing effort to make spectroscopic tools for inducing and controlling, in real time, the natural processes which occur on the femto and attosecond times scales.Femtosecond lasers, with a fundamental wavelength in the infrared (IR) spectral region, can be used for producing a fascinating spectroscopic tool - extreme ultraviolet (XUV) pulses with typical duration of hundreds of attoseconds. A typical XUV attosecond pulse is produced when an intense ultrafast laser is focused in a gaseous target. The fundamental laser frequency gets upconverted into its higher harmonics through an extreme nonlinear process in which the electron leaves the ion's potential well and oscillates in the laser field emitting a short burst of radiation every time it is driven back into the vicinity of its parent ion by the linearly polarized laser electric field. In this thesis, we present several examples of using IR and XUV pulses to induce and control the excitation and ionization processes in atoms and molecules on the attosecond time scale. A 3D momentum imaging technique called COLTRIMS is used to collect all the reaction products (electrons and ions) in coincidence.The experiments were performed at the J.R.M. lab at the Kansas State University, where the experimental apparatus was designed and built under the supervision of professor C.L. Cocke.
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| 5. |
- Schmid, Georg, et al.
(författare)
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Tracing charge transfer in argon dimers by XUV-pump IR-probe experiments at FLASH
- 2019
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Ingår i: Journal of Chemical Physics. - : AIP Publishing. - 0021-9606 .- 1089-7690. ; 151:8
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Tidskriftsartikel (refereegranskat)abstract
- Charge transfer (CT) at avoided crossings of excited ionized states of argon dimers is observed using a two-color pump-probe experiment at the free-electron laser in Hamburg (FLASH). The process is initiated by the absorption of three 27-eV-photons from the pump pulse, which leads to the population of Ar2+*-Ar states. Due to nonadiabatic coupling between these one-site doubly ionized states and two-site doubly ionized states of the type Ar+*-Ar+, CT can take place leading to the population of the latter states. The onset of this process is probed by a delayed infrared (800 nm) laser pulse. The latter ionizes the dimers populating repulsive Ar2+ -Ar+ states, which then undergo a Coulomb explosion. From the delay-dependent yields of the obtained Ar2+ and Ar+ ions, the lifetime of the charge-transfer process is extracted. The obtained experimental value of (531 ± 136) fs agrees well with the theoretical value computed from Landau-Zener probabilities.
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