| 1. |
- Lever, F., et al.
(författare)
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Ultrafast dynamics of 2-thiouracil investigated by time-resolved Auger spectroscopy
- 2020
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Ingår i: Journal of Physics B: Atomic, Molecular and Optical Physics. - : IOP Publishing. - 0953-4075 .- 1361-6455. ; 54
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Tidskriftsartikel (refereegranskat)abstract
- We present time-resolved ultraviolet-pump x-ray probe Auger spectra of 2-thiouracil. An ultraviolet induced shift towards higher kinetic energies is observed in the sulfur 2p Auger decay. The difference Auger spectra of pumped and unpumped molecules exhibit ultrafast dynamics in the shift amplitude, in which three phases can be recognized. In the first 100 fs, a shift towards higher kinetic energies is observed, followed by a 400 fs shift back to lower kinetic energies and a 1 ps shift again to higher kinetic energies. We use a simple Coulomb-model, aided by quantum chemical calculations of potential energy states, to deduce a C–S bond expansion within the first 100 fs. The bond elongation triggers internal conversion from the photoexcited S2 to the S1 state. Based on timescales, the subsequent dynamics can be interpreted in terms of S1 nuclear relaxation and S1-triplet internal conversion.
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| 2. |
- Mayer, D., et al.
(författare)
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Following excited-state chemical shifts in molecular ultrafast x-ray photoelectron spectroscopy
- 2022
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Ingår i: Nature Communications. - : Springer Science and Business Media LLC. - 2041-1723. ; 13:1
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Tidskriftsartikel (refereegranskat)abstract
- The conversion of photon energy into other energetic forms in molecules is accompanied by charge moving on ultrafast timescales. We directly observe the charge motion at a specific site in an electronically excited molecule using time-resolved x-ray photoelectron spectroscopy (TR-XPS). We extend the concept of static chemical shift from conventional XPS by the excited-state chemical shift (ESCS), which is connected to the charge in the framework of a potential model. This allows us to invert TR-XPS spectra to the dynamic charge at a specific atom. We demonstrate the power of TR-XPS by using sulphur 2p-core-electron-emission probing to study the UV-excited dynamics of 2-thiouracil. The method allows us to discover that a major part of the population relaxes to the molecular ground state within 220–250 fs. In addition, a 250-fs oscillation, visible in the kinetic energy of the TR-XPS, reveals a coherent exchange of population among electronic states. © 2022, The Author(s).
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| 3. |
- Seidel, M., et al.
(författare)
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Multi-pass Cell Based Nonlinear Pulse Compression of Yb : YAG Pump-Probe Lasers at FLASH
- 2023
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Ingår i: X-Ray Free-Electron Lasers : Advances in Source Development and Instrumentation VI - Advances in Source Development and Instrumentation VI. - 1996-756X .- 0277-786X. - 9781510662827 ; 12581
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Konferensbidrag (refereegranskat)abstract
- The majority of user experiments at the high repetition-rate free electron laser (FEL) facility FLASH are of pump-probe type, combining the extreme ultraviolet (XUV) or soft x-ray radiation from the FEL with ultrashort pulses generated by optical lasers. In this contribution, we demonstrate the advantages of using high-power Yb:YAG lasers with subsequent nonlinear pulse compression stages based on multi-pass cells (MPC). The approach enables the combination of hundreds of kHz to MHz repetition-rates, hundreds of watts of average powers and excellent intensity stabilities. We present the characteristics of the MPC-based pump-probe laser at the FLASH plane-grating beamlines. Furthermore, we report pulse compression to 8.2 fs pulse duration and the seeding of an optical parametric amplifier generating mid-IR radiation tunable from 1.4 µm to 16 µm.
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| 4. |
- Viotti, A. L., et al.
(författare)
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Multi-Pass Cell Post-Compression for Pump-Probe Experiments at the FEL Facility FLASH
- 2021
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Ingår i: Laser Applications Conference, LAC 2021. - 9781557528209
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Konferensbidrag (refereegranskat)abstract
- We present high-power Yb:YAG lasers combined with nonlinear pulse compression in multi-pass cells. We show that these are suitable for integration in FEL facilities in terms of pulse stability, jitter, temporal contrast and intra-burst behaviour.
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