Strong-field ionization of molecular iodine traced with XUV pulses from a free-electron laser

Krikunova, Maria; Maltezopoulos, T.; Wessels, Philipp; Schlie, Moritz; Azima, Armin; Gaumnitz, Thomas; Gebert, Thomas-H.; Wieland, Marek; Drescher, Markus

doi:10.1103/physreva.86.043430

Cited by 20 publications

(11 citation statements)

References 35 publications

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“…, clusters and nanoparticles (Krikunova et al 2012a, 2012b, Clark et al 2015, Ferguson et al 2016, Flückiger et al 2016, Gorkhover et al 2016, liquids (Hallmann et al 2010, Wernet et al 2015, Biasin et al 2016, solids (Rajkovic et al 2010, Dell'Angela et al 2013, Siefermann et al 2014, Gleason et al 2015, Öström et al 2015, Rettig et al 2016, and even biological systems such as photoactive proteins (Aquila et al 2012, Tenboer et al 2014, Barends et al 2015, Pande et al 2016. Many of these time-resolved experiments require precise synchronization of an optical femtosecond laser with the FEL.…”

Section: Introductionmentioning

confidence: 99%

Jitter-correction for IR/UV-XUV pump-probe experiments at the FLASH free-electron laser

et al. 2017

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In pump-probe experiments employing a free-electron laser (FEL) in combination with a synchronized optical femtosecond laser, the arrival-time jitter between the FEL pulse and the optical laser pulse often severely limits the temporal resolution that can be achieved. Here, we present a pump-probe experiment on the UV-induced dissociation of 2,6-difluoroiodobenzene (C 6 H 3 F 2 I) molecules performed at the FLASH FEL that takes advantage of recent upgrades of the FLASH timing and synchronization system to obtain high-quality data that are not limited by the FEL arrival-time jitter. We discuss in detail the necessary data analysis steps and describe the origin of the timedependent effects in the yields and kinetic energies of the fragment ions that we observe in the experiment.

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Section: Introductionmentioning

confidence: 99%

Jitter-correction for IR/UV-XUV pump-probe experiments at the FLASH free-electron laser

et al. 2017

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“…It should be noted that the COB model used here is analog to those applied for field-ionization in strong laser fields (e.g., [22,23]) and slow ion-atom collisions [11,12]. Our experimental situation is similar to a collision, with the difference that now the reaction partners start from their closest distance.…”

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confidence: 92%

Electron Rearrangement Dynamics in DissociatingI2n+Molecules Accessed by Extreme Ultraviolet Pump-Probe Experiments

et al. 2014

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The charge rearrangement in dissociating I n+ 2 molecules is measured as a function of the internuclear distance R using XUV pulses delivered by the free-electron laser (FEL) in Hamburg. Within an XUV pump-probe scheme the first pulse initiates dissociation by multiply ionizing I 2 , and the delayed probe pulse further ionizes one of the two fragments at a given time, thus triggering charge rearrangement at a well-defined R. The electron transfer between the fragments is monitored by analyzing the delay-dependent ion kinetic energies and charge states. The experimental results are in very good agreement with predictions of the classical over-the-barrier model demonstrating its validity in a thus far unexplored quasimolecular regime relevant for FEL, plasma and chemistry applications.The dynamics of charge relaxation, rearrangement and equilibration at the transition between chemically bound and unbound systems is essential for understanding many chemical [1, 2] and plasma reactions [3,4]. It is also crucial for the imaging of biomolecules with atomic resolution, a key application of Free-Electron Lasers (FELs). Here, the idea is to take a snapshot of the molecule by irradiating the system with intense ultra-short (< 100 fs) X-ray pulses before it is damaged [5]. Recent experiments on nano-crystalized lysozyme, however, have shown that the photon-induced damage leads to a scattering pattern that is different from what is expected for the intact molecule even for X-ray pulses as short as 70 fs [6]. Photon absorption is strongly localized at constituents with high atomic numbers, often having more than an order of magnitude larger cross sections as compared to H or even C atoms [7]. Therefore, it is crucial to understand the underlying ultrafast electronic and nuclear rearrangement dynamics in order to develop improved damage models that take into account the spatio-temporal spread of the locally induced charge.Localized photon absorption efficiently triggers atomic movement and electron rearrangement across the entire molecular ion, mainly leading to its fragmentation. In a recent study methylselenol [8] and ethylselenol [9] molecules, containing one heavy selenium atom as photoabsorption center, were irradiated with single intense 5 fs X-ray pulses. From the observed charge-state distributions and the fragments' kinetic energies it could be concluded that even for such short pulses ultrafast charge rearrangement takes place, accompanied by considerable atomic displacements which is relevant for imaging with atomic resolution. However, the central question concerning the underlying time and length scales remained open. In this work we present experimental results on the electron transfer between two iodine ions at freely chosen internuclear distances R. A dissociation of the I 2 molecule is triggered by multiple ionization with a femtosecond pump pulse [10]. The evolving system is then further ionized by the delayed probe pulse. Depending on the time delay, or the corresponding internuclear distance, and the charg...

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“…High irradiation intensity combined with short pulse duration provided access to a new parameter regime of nonlinear x-ray physics [4][5][6][7] and has led to the observation of novel phenomena such as x-ray induced transparency [8], collective plasmalike states [9], or interatomic Coulombic decay cascades [10]. Ultrafast time-resolved spectroscopy using FEL pulses is now able to trace the dynamics of electronic and nuclear rearrangement in molecules [11,12]. Another prominent example is the serial time-resolved crystallography that has provided unprecedented insights into the conformational changes triggered by the excitation of Photosystem II with visible light [13].…”

Section: Introductionmentioning

confidence: 99%

Mapping ultrafast ionization of atoms and clusters with terahertz-streaking delay

et al. 2019

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We apply THz-field streaking to temporally resolve the ultrafast ionization of neutral cluster vs atomic targets exposed to intense ultrashort soft x-ray pulses from a free-electron laser (FEL). In the experiment pristine Xe and mixed Xe/Ar clusters as well as Xe atoms are ionized in the vicinity of the 4d → ε f giant resonance of Xe. We compare the relative streaking delay between the center-of-mass oscillations of electrons that have final kinetic energies in the spectral region of the Xe(4d) photoline. Our results show that clusters are ionized at the beginning of the 100 fs FEL pulse as supported by calculations of target frustration in the focal volume. We have identified a significantly larger 40 fs relative streaking delay between mixed Xe-Ar clusters vs Xe atoms compared to a 15 fs relative delay found for pristine Xe clusters. This is attributed to the high sensitivity of our spectroscopic measurement to the degree of condensation of the cluster target. Our results show that THz streaking is a powerful technique to temporally study electron emission from extended targets under intense FEL radiation on time scales that are significantly shorter than the FEL pulse duration.

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Strong-field ionization of molecular iodine traced with XUV pulses from a free-electron laser

Cited by 20 publications

References 35 publications

Jitter-correction for IR/UV-XUV pump-probe experiments at the FLASH free-electron laser

Jitter-correction for IR/UV-XUV pump-probe experiments at the FLASH free-electron laser

Electron Rearrangement Dynamics in DissociatingI2n+Molecules Accessed by Extreme Ultraviolet Pump-Probe Experiments

Mapping ultrafast ionization of atoms and clusters with terahertz-streaking delay

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