12 research outputs found
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Observation of correlated electronic decay in expanding clusters triggered by near-infrared fields
When an excited atom is embedded into an environment, novel relaxation pathways can emerge that are absent for isolated atoms. A well-known example is interatomic Coulombic decay, where an excited atom relaxes by transferring its excess energy to another atom in the environment, leading to its ionization. Such processes have been observed in clusters ionized by extreme-ultraviolet and X-ray lasers. Here, we report on a correlated electronic decay process that occurs following nanoplasma formation and Rydberg atom generation in the ionization of clusters by intense, non-resonant infrared laser fields. Relaxation of the Rydberg states and transfer of the available electronic energy to adjacent electrons in Rydberg states or quasifree electrons in the expanding nanoplasma leaves a distinct signature in the electron kinetic energy spectrum. These so far unobserved electron-correlation-driven energy transfer processes may play a significant role in the response of any nano-scale system to intense laser light
Ultrafast vibrational relaxation dynamics in XUV-excited Polycyclic Aromatic Hydrocarbon molecules
Interstellar matter and star formatio
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XUV excitation followed by ultrafast non-adiabatic relaxation in PAH molecules as a femto-astrochemistry experiment
Highly excited molecular species are at play in the chemistry of interstellar media and are involved in the creation of radiation damage in a biological tissue. Recently developed ultrashort extreme ultraviolet light sources offer the high excitation energies and ultrafast time-resolution required for probing the dynamics of highly excited molecular states on femtosecond (fs) (1 fs=10−15s) and even attosecond (as) (1 as=10−18 s) timescales. Here we show that polycyclic aromatic hydrocarbons (PAHs) undergo ultrafast relaxation on a few tens of femtoseconds timescales, involving an interplay between the electronic and vibrational degrees of freedom. Our work reveals a general property of excited radical PAHs that can help to elucidate the assignment of diffuse interstellar absorption bands in astrochemistry, and provides a benchmark for the manner in which coupled electronic and nuclear dynamics determines reaction pathways in large molecules following extreme ultraviolet excitation
Ultrafast dynamics of correlation bands following XUV molecular photoionization
Interstellar matter and star formatio
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Charge transfer to ground-state ions produces free electrons
Inner-shell ionization of an isolated atom typically leads to Auger decay. In an environment, for example, a liquid or a van der Waals bonded system, this process will be modified, and becomes part of a complex cascade of relaxation steps. Understanding these steps is important, as they determine the production of slow electrons and singly charged radicals, the most abundant products in radiation chemistry. In this communication, we present experimental evidence for a so-far unobserved, but potentially very important step in such relaxation cascades: Multiply charged ionic states after Auger decay may partially be neutralized by electron transfer, simultaneously evoking the creation of a low-energy free electron (electron transfer-mediated decay). This process is effective even after Auger decay into the dicationic ground state. In our experiment, we observe the decay of Ne2+ produced after Ne 1s photoionization in Ne-Kr mixed clusters
Slow interatomic Coulombic decay of multiply excited neon clusters
Ne clusters ( 3c5000 atoms) were resonantly excited (2p\u21923s) by intense free electron laser (FEL) radiation at FERMI. Such multiply excited clusters can decay nonradiatively via energy exchange between at least two neighboring excited atoms. Benefiting from the precise tunability and narrow bandwidth of seeded FEL radiation, specific sites of the Ne clusters were probed. We found that the relaxation of cluster surface atoms proceeds via a sequence of interatomic or intermolecular Coulombic decay (ICD) processes while ICD of bulk atoms is additionally affected by the surrounding excited medium via inelastic electron scattering. For both cases, cluster excitations relax to atomic states prior to ICD, showing that this kind of ICD is rather slow (picosecond range). Controlling the average number of excitations per cluster via the FEL intensity allows a coarse tuning of the ICD rate
PAH under XUV excitation: an ultrafast XUV-photochemistry experiment for astrophysics
Understanding processes induced by XUV excitation of Polycyclic Aromatic Hydrocarbons (PAHs) is at the heart of molecular astrophysics, which aims at understanding molecular evolution in interstellar media. We used ultrashort XUV pulses to produce highly excited PAHs cations. The photo-induced dynamics is probed using a pump-probe XUV-IR spectroscopy. By studying PAH from small (naphthalene) to large (hexabenzocoronene) PAHs, we show that the dynamic is governed by the large density of states, in which many-body quantum effects are dominant
Ultrafast dynamics of correlation bands following XUV molecular photoionization
Laboratory astrophysics and astrochemistr
Coherence of Auger and inter-Coulombic decay processes in the photoionization of Ar@C60 versus Kr@C60
For the asymmetric spherical dimer of an endohedrally confined atom and a
host fullerene, an innershell vacancy of either system can decay through the
continuum of an outer electron hybridized between the systems. Such decays,
viewed as coherent superpositions of the single-center Auger and two-center
inter-Coulombic (ICD) amplitudes, are found to govern leading decay mechanisms
in noble-gas endofullerenes, and are likely omnipresent in this class of
nanomolecules. A comparison between resulting autoionizing resonances
calculated in the photoionization of Ar@C60 and Kr@C60 exhibits details of the
underlying processes.Comment: 7 pages, 3 figures, Submitte