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204 results on '"Di Fraia M"'

1. Time-resolved chiral X-Ray photoelectron spectroscopy with transiently enhanced atomic site-selectivity: a Free Electron Laser investigation of electronically excited fenchone enantiomers

Author

Faccialà, D., Devetta, M., Beauvarlet, S., Besley, N., Calegari, F., Callegari, C., Catone, D., Cinquanta, E., Ciriolo, A. G., Colaizzi, L., Coreno, M., Crippa, G., De Ninno, G., Di Fraia, M., Galli, M., Garcia, G. A., Mairesse, Y., Negro, M., Plekan, O., Geetha, P. Prasannan, Prince, K. C., Pusala, A., Stagira, S., Turchini, S., Ueda, K., You, D., Zema, N., Blanchet, V., Nahon, L., Powis, I., and Vozzi, C.

Subjects
Physics - Chemical Physics
Abstract

Chiral molecules are widespread in nature, playing a fundamental role in bio-chemical processes and in the origin of life itself. The observation of dynamics in chiral molecules is crucial for the understanding and control of the chiral activity of photo-excited states. One of the most promising techniques for the study of photo-excited chiral systems is time-resolved photoelectron circular dichroism (TR-PECD), which offers an intense and sensitive probe for vibronic and geometric molecular structure as well as electronic structures, and their evolution on a femtosecond timescale. However, the non-local character of the PECD effect, which is imprinted during the electron scattering off the molecule, makes the interpretation of TR-PECD experiments challenging. In this respect, core-photoionization is known to allow site- and chemical-sensitivity to photelectron spectroscopy. Here we demonstrate that TR-PECD utilising core-level photoemission enables probing the chiral electronic structure and its relaxation dynamics with atomic site sensitivity. Following UV pumped excitation to a 3s Rydberg state, fenchone enantiomers (C 10 H 16 O) were probed on a femtosecond scale using circularly polarized soft X-ray light pulses provided by the free-electron laser FERMI. C 1s binding energy shifts caused by the redistribution of valence electron density in this 3s-valence-Rydberg excitation allowed us to measure transient PECD chiral responses with an enhanced C-atom site-selectivity compared to that achievable in the ground state molecule. These results represent the first chemical-specific and site-specific, enantio-sensitive observations on the electronic structure of a photo-excited chiral molecule and pave the way towards chiral femtochemistry probed by core-level photoemission.

Published
2022
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2. The photochemical ring-opening reaction of 1,3-cyclohexadiene: complex dynamical evolution of the reactive state

Author

Travnikova, O., Piteša, T., Ponzi, A., Sapunar, M., Squibb, R. J., Richter, R., Finetti, P., Di Fraia, M., De Fanis, A., Mahne, N., Manfredda, M., Zhaunerchyk, V., Marchenko, T., Guillemin, R., Journel, L., Prince, K. C., Callegari, C., Simon, M., Feifel, R., Decleva, P., Došlić, N., and Piancastelli, M. N.

Subjects
Physics - Chemical Physics
Abstract

The photochemically induced ring-opening isomerization reaction of 1,3-cyclohexadiene (CHD) to 1,3,5-hexatriene (HT) is a textbook example of a pericyclic reaction, and has been amply investigated with advanced spectroscopic techniques. The generally accepted description of the isomerization pathway starts with a valence excitation to the lowest-lying bright state, followed by a passage through a conical intersection to a dark doubly excited state, and finally a branching between either the return to the ground state of the cyclic molecule or the actual ring-opening reaction leading to the open-chain isomer. It was traditionally assumed that the dark reactive state corresponds to the second excited state of CHD at the Franck-Condon geometry. Here in a joint experimental and computational effort we demonstrate that the evolution of the excitation-deexcitation process is much more complex than usually described. In particular, we show that an initially high-lying electronic state smoothly decreasing in energy along the reaction path plays a key role in the ring-opening reaction. The conceptual basis of our work is that the dynamics to consider here is determined by diabatic states, whose populations are the ones closely related to the observed photoelectron signal., Comment: Sumbitted to Nature Communications (under review)

Published
2022

3. Time-resolved quantum beats in the fluorescence of helium resonantly excited by XUV radiation

Author

LaForge, AC, Benediktovitch, A, Sukharnikov, V, Krušič, Š, Žitnik, M, Debatin, M, Falcone, RW, Asmussen, JD, Mudrich, M, Michiels, R, Stienkemeier, F, Badano, L, Callegari, C, Di Fraia, M, Ferianis, M, Giannessi, L, Plekan, O, Prince, KC, Spezzani, C, Rohringer, N, and Berrah, N

Subjects
Physics - Atomic Physics
Abstract

We report on the observation of time-resolved quantum beats in the helium fluorescence from the transition 1s3p -> 1s2s, where the initial state is excited by XUV free-electron laser radiation. The quantum beats originate from the Zeeman splitting of the magnetic substates due to an external magnetic field. We perform a systematic study of this effect and discuss the possibilities of studying this phenomenon in the XUV and x-ray regime., Comment: 7 pages, 4 figures

Published
2021
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4. Collective enhancement of above threshold ionization by resonantly excited helium nanodroplets

Author

Michiels, R., Abu-samha, M., Madsen, L. B., Binz, M., Bangert, U., Bruder, L., Duim, R., Wituschek, A., LaForge, A. C., Squibb, R. J., Feifel, R., Callegari, C., Di Fraia, M., Danailov, M., Manfredda, M., Plekan, O., Prince, K. C., Rebernik, P., Zangrando, M., Stienkemeier, F., and Mudrich, M.

Subjects
Physics - Atomic and Molecular Clusters
Abstract

Clusters and nanodroplets hold the promise of enhancing high-order nonlinear optical effects due to their high local density. However, only moderate enhancement has been demonstrated to date. Here, we report the observation of energetic electrons generated by above-threshold ionization (ATI) of helium (He) nanodroplets which are resonantly excited by ultrashort extreme ultraviolet (XUV) free-electron laser pulses and subsequently ionized by near-infrared (NIR) or near-ultraviolet (UV) pulses. The electron emission due to high-order ATI is enhanced by several orders of magnitude compared to He atoms. The crucial dependence of the ATI intensities with the number of excitations in the droplets suggests a local collective enhancement effect.

Published
2021
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5. Evolution and ion kinetics of a XUV-induced nanoplasma in ammonia clusters

Author

Michiels, R., LaForge, A. C., Bohlen, M., Callegari, C., Clark, A., von Conta, A., Coreno, M., Di Fraia, M., Drabbels, M., Finetti, P., Huppert, M., Oliver, V., Plekan, O., Prince, K. C., Stranges, S., Wörner, H. J., and Stienkemeier, F.

Subjects
Physics - Atomic and Molecular Clusters
Abstract

High-intensity extreme ultraviolet (XUV) pulses from a free-electron laser can be used to create a nanoplasma in clusters. In Ref. [Michiels et al. PCCP, 2020; 22: 7828-7834] we investigated the formation of excited states in an XUV-induced nanoplasma in ammonia clusters. In the present article we expand our previous study with a detailed analysis of the nanoplasma evolution and ion kinetics. We use a time-delayed UV laser as probe to ionize excited states of H and H$_2^+$ in the XUV-induced plasma. Employing covariance mapping techniques, we show that the correlated emission of protons plays an important role in the plasma dynamics. The time-dependent kinetic energy of the ions created by the probe laser is measured, revealing the charge neutralization of the cluster happens on a sub-picosecond timescale. Furthermore, we observe ro-vibrationally excited molecular hydrogen ions H$_2^{+*}$ being ejected from the clusters. We rationalize our data through a qualitative model of a finite-size non-thermal plasma.

Published
2020
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6. Time-resolved study of resonant interatomic Coulombic decay in helium nanodroplets

Author

LaForge, A. C., Michiels, R., Ovcharenko, Y., Ngai, A., Escartin, J. M., Berrah, N., Callegari, C., Clark, A., Coreno, M., Cucini, R., Di Fraia, M., Drabbels, M., Fasshauer, E., Finetti, P., Giannessi, L., Grazioli, C., Iablonskyi, D., Langbehn, B., Nishiyama, T., Oliver, V., Piseri, P., Plekan, O., Prince, K. C., Rupp, D., Stranges, S., Ueda, K., Sisourat, N., Eloranta, J., Pi, M., Barranco, M., Stienkemeier, F., Moeller, T., and Mudrich, M.

Subjects
Physics - Atomic and Molecular Clusters
Abstract

When weakly-bound complexes are multiply excited by intense electromagnetic radiation, energy can be exchanged between neighboring atoms through a type of resonant interatomic Coulombic decay (ICD). This decay mechanism due to multiple excitations has been predicted to be relatively slow, typically lasting tens to hundreds of picoseconds. Here, we directly measure the ICD timescale in resonantly excited helium droplets using a high resolution, tunable, extreme ultraviolet free electron laser. Over an extensive range of droplet sizes and laser intensities, we discover the decay to be surprisingly fast, with decay times as fast as 400 femtoseconds, and to only present a weak dependence on the density of the excited states. Using a combination of time dependent density functional theory and ab initio quantum chemistry calculations, we elucidate the mechanisms of this ultrafast decay process where pairs of excited helium atoms in one droplet strongly attract each other and form merging void bubbles which drastically accelerates ICD.

Published
2020
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7. Ultrafast relaxation of photoexcited superfluid He nanodroplets

Author

Mudrich, M., LaForge, A., Stienkemeier, F., Ciavardini, A., O'Keeffe, P., Coreno, M., Ovcharenko, Y., Moeller, T., Ziemkiewicz, M., Devetta, M., Piseri, P., Drabbels, M., Demidovich, A., Grazioli, C., Finetti, P., Plekan, O., Di Fraia, M., Prince, K. C., Richter, R., Callegari, C., Eloranta, J., Hernando, A., Pi, M., and Barranco, M.

Subjects
Physics - Atomic and Molecular Clusters
Abstract

The relaxation of photoexcited nanosystems is a fundamental process of light-matter interaction. Depending on the couplings of the internal degrees of freedom, relaxation can be ultrafast, converting electronic energy in a few fs, or slow, if the energy is trapped in a metastable state that decouples from its environment. Here, helium nanodroplets are resonantly excited by femtosecond extreme-ultraviolet (XUV) pulses from a seeded free-electron laser. Despite their superfluid nature, we find that helium nanodroplets in the lowest electronically excited states undergo ultrafast relaxation. By comparing experimental photoelectron spectra with time-dependent density functional theory simulations, we unravel the full relaxation pathway: Following an ultrafast interband transition, a void nanometer-sized bubble forms around the localized excitation (He*) within 1 ps. Subsequently, the bubble collapses and releases metastable He* at the droplet surface. This study highlights the high level of detail achievable in probing the photodynamics of nanosystems using tunable XUV pulses.

Published
2019
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8. Two-photon resonant excitation of interatomic coulombic decay in neon dimers

Author

Dubrouil, A, Reduzzi, M, Devetta, M, Feng, C, Hummert, J, Finetti, P, Plekan, O, Grazioli, C, Di Fraia, M, Lyamayev, V, La Forge, A, Katzy, R, Stienkemeier, F, Ovcharenko, Y, Coreno, M, Berrah, N, Motomura, K, Mondal, S, Ueda, K, Prince, K C, Callegari, C, Kuleff, A I, Demekhin, Ph V, and Sansone, G

Subjects
Physics - Atomic Physics, Physics - Optics
Abstract

The recent availability of intense and ultrashort extreme ultraviolet sources opens the possibility to investigate ultrafast electronic relaxation processes in matter in an unprecedented regime. In this work we report on the observation of two-photon excitation of interatomic Coulombic decay (ICD) in neon dimers using the tunable intense pulses delivered by the free electron laser FERMI@Elettra. The unique characteristics of FERMI (narrow bandwidth, spectral stability, and tunability) allow one to resonantly excite specific ionization pathways and to observe a clear signature of the ICD mechanism in the ratio of the ion yield created by Coulomb explosion. The present experimental results are explained by \emph{ab initio} electronic structure and nuclear dynamics calculations.

Published
2019

9. Control of H2 Dissociative Ionization in the Nonlinear Regime Using Vacuum Ultraviolet Free-Electron Laser Pulses

Author

Holzmeier, F, Bello, RY, Hervé, M, Achner, A, Baumann, TM, Meyer, M, Finetti, P, Di Fraia, M, Gauthier, D, Roussel, E, Plekan, O, Richter, R, Prince, KC, Callegari, C, Bachau, H, Palacios, A, Martín, F, and Dowek, D

Subjects
Mathematical Sciences, Physical Sciences, Engineering, General Physics
Abstract

The role of the nuclear degrees of freedom in nonlinear two-photon single ionization of H_{2} molecules interacting with short and intense vacuum ultraviolet pulses is investigated, both experimentally and theoretically, by selecting single resonant vibronic intermediate neutral states. This high selectivity relies on the narrow bandwidth and tunability of the pulses generated at the FERMI free-electron laser. A sustained enhancement of dissociative ionization, which even exceeds nondissociative ionization, is observed and controlled as one selects progressively higher vibronic states. With the help of ab initio calculations for increasing pulse durations, the photoelectron and ion energy spectra obtained with velocity map imaging allow us to identify new photoionization pathways. With pulses of the order of 100 fs, the experiment probes a timescale that lies between that of ultrafast dynamical processes and that of steady state excitations.

Published
2018

10. Collective Autoionization in Multiply-Excited Systems: A novel ionization process observed in Helium Nanodroplets

Author

LaForge, A. C., Drabbels, M., Brauer, N., Coreno, M., Devetta, M., Di Fraia, M., Finetti, P., Grazioli, C., Katzy, R., Lyamayev, V., Mazza, T., Mudrich, M., OKeeffe, P., Ovcharenko, Y., Piseri, P., Plekan, O., Prince, K. C., Richter, R., Stranges, S., Callegari, C., Moeller, T., and Stienkemeier, F.

Subjects
Physics - Atomic and Molecular Clusters
Abstract

Free electron lasers (FELs) offer the unprecedented capability to study reaction dynamics and image the structure of complex systems. When multiple photons are absorbed in complex systems, a plasma-like state is formed where many atoms are ionized on a femtosecond timescale. If multiphoton absorption is resonantly-enhanced, the system becomes electronically-excited prior to plasma formation, with subsequent decay paths which have been scarcely investigated to date. Here, we show using helium nanodroplets as an example that these systems can decay by a new type of process, named collective autoionization. In addition, we show that this process is surprisingly efficient, leading to ion abundances much greater than that of direct single-photon ionization. This novel collective ionization process is expected to be important in many other complex systems, e.g. macromolecules and nanoparticles, exposed to high intensity radiation fields.

Published
2013
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11. EUV ionization of pure He nanodroplets: Mass-correlated photoelectron imaging, Penning ionization and electron energy-loss spectra

Author

Buchta, D., Krishnan, S. R., Brauer, N. B., Drabbels, M., O'Keeffe, P., Devetta, M., Di Fraia, M., Callegari, C., Richter, R., Coreno, M., Prince, K. C., Stienkemeier, F., Moshammer, R., and Mudrich, M.

Subjects
Physics - Atomic and Molecular Clusters
Abstract

The ionization dynamics of pure He nanodroplets irradiated by EUV radiation is studied using Velocity-Map Imaging PhotoElectron-PhotoIon COincidence (VMI-PEPICO) spectroscopy. We present photoelectron energy spectra and angular distributions measured in coincidence with the most abundant ions He+, He2+, and He3+. Surprisingly, below the autoionization threshold of He droplets we find indications for multiple excitation and subsequent ionization of the droplets by a Penning-like process. At high photon energies we evidence inelastic collisions of photoelectrons with the surrounding He atoms in the droplets.

Published
2013
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12. Atomic Two-Color XUV Interferometer

Author

Žitnik, M., primary, Mihelič, A., additional, Bučar, K., additional, Krušič, Š, additional, Turnšek, J., additional, Squibb, R., additional, Feifel, R., additional, Ismail, I., additional, Lablanquie, P., additional, Palaudoux, J., additional, Plekan, O., additional, Di Fraia, M., additional, Pal, N., additional, Coreno, M., additional, Manfredda, M., additional, Simoncig, A., additional, Ribič, P. Rebernik, additional, Sottocorona, F., additional, Allaria, E., additional, Prince, K. C., additional, Callegari, C., additional, and Penent, F., additional

Published
2023
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13. Sub-Wavelength Charge Dynamics in Textured Infrared and Free Electron Lasers

Author

Wätzel, J., primary, Ribič, P. R., additional, Coreno, M., additional, Danailov, M. B., additional, David, C., additional, Demidovich, A., additional, Di Fraia, M., additional, Giannessi, L., additional, Hansen, K., additional, Krušič, Š., additional, Manfredda, M., additional, Meyer, M., additional, Mihelič, A., additional, Mirian, N., additional, Plekan, O., additional, Ressel, B., additional, Rösner, B., additional, Simoncig, A., additional, Spampinati, S., additional, Stupar, M., additional, Žitnik, M., additional, Zangrando, M., additional, Callegari, C., additional, De Ninno, G., additional, and Berakdar, J., additional

Published
2023
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15. Time-Resolved Chiral X-Ray Photoelectron Spectroscopy with Transiently Enhanced Atomic Site Selectivity: A Free-Electron Laser Investigation of Electronically Excited Fenchone Enantiomers

Author

Faccialà, D., primary, Devetta, M., additional, Beauvarlet, S., additional, Besley, N., additional, Calegari, F., additional, Callegari, C., additional, Catone, D., additional, Cinquanta, E., additional, Ciriolo, A. G., additional, Colaizzi, L., additional, Coreno, M., additional, Crippa, G., additional, De Ninno, G., additional, Di Fraia, M., additional, Galli, M., additional, Garcia, G. A., additional, Mairesse, Y., additional, Negro, M., additional, Plekan, O., additional, Prasannan Geetha, P., additional, Prince, K. C., additional, Pusala, A., additional, Stagira, S., additional, Turchini, S., additional, Ueda, K., additional, You, D., additional, Zema, N., additional, Blanchet, V., additional, Nahon, L., additional, Powis, I., additional, and Vozzi, C., additional

Published
2023
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18. Controlling Fragmentation of the Acetylene Cation in the Vacuum Ultraviolet via Transient Molecular Alignment

Author

Varvarezos, L., primary, Delgado-Guerrero, J., additional, Di Fraia, M., additional, Kelly, T. J., additional, Palacios, A., additional, Callegari, C., additional, Cavalieri, A. L., additional, Coffee, R., additional, Danailov, M., additional, Decleva, P., additional, Demidovich, A., additional, DiMauro, L., additional, Düsterer, S., additional, Giannessi, L., additional, Helml, W., additional, Ilchen, M., additional, Kienberger, R., additional, Mazza, T., additional, Meyer, M., additional, Moshammer, R., additional, Pedersini, C., additional, Plekan, O., additional, Prince, K. C., additional, Simoncig, A., additional, Schletter, A., additional, Ueda, K., additional, Wurzer, M., additional, Zangrando, M., additional, Martín, F., additional, and Costello, J. T., additional

Published
2022
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19. Diffraction imaging of light induced dynamics in xenon-doped helium nanodroplets

Author

Langbehn, B, primary, Ovcharenko, Y, additional, Clark, A, additional, Coreno, M, additional, Cucini, R, additional, Demidovich, A, additional, Drabbels, M, additional, Finetti, P, additional, Di Fraia, M, additional, Giannessi, L, additional, Grazioli, C, additional, Iablonskyi, D, additional, LaForge, A C, additional, Nishiyama, T, additional, Oliver Álvarez de Lara, V, additional, Peltz, C, additional, Piseri, P, additional, Plekan, O, additional, Sander, K, additional, Ueda, K, additional, Fennel, T, additional, Prince, K C, additional, Stienkemeier, F, additional, Callegari, C, additional, Möller, T, additional, and Rupp, D, additional

Published
2022
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21. Interference of two-photon transitions induced by XUV light

Author

Žitnik, M., primary, Mihelič, A., additional, Bučar, K., additional, Krušič, Š., additional, Squibb, R., additional, Feifel, R., additional, Ismail, I., additional, Lablanquie, P., additional, Palaudoux, J., additional, Plekan, O., additional, Di Fraia, M., additional, Coreno, M., additional, Manfredda, M., additional, Simoncig, A., additional, Rebernik Ribič, P., additional, Sottocorona, F., additional, Allaria, E., additional, Prince, K. C., additional, Callegari, C., additional, and Penent, F., additional

Published
2022
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22. Planet Hunters TESS IV: a massive, compact hierarchical triple star system TIC 470710327

Author

Eisner, N L, primary, Johnston, C, additional, Toonen, S, additional, Frost, A J, additional, Janssens, S, additional, Lintott, C J, additional, Aigrain, S, additional, Sana, H, additional, Abdul-Masih, M, additional, Arellano-Córdova, K Z, additional, Beck, P G, additional, Bordier, E, additional, Cannon, E, additional, Escorza, A, additional, Fabry, M, additional, Hermansson, L, additional, Howell, S B, additional, Miller, G, additional, Sheyte, S, additional, Alhassan, S, additional, Baeten, E M L, additional, Barnet, F, additional, Bean, S J, additional, Bernau, M, additional, Bundy, D M, additional, Di Fraia, M Z, additional, Emralino, F M, additional, Goodwin, B L, additional, Hermes, P, additional, Hoffman, T, additional, Huten, M, additional, Janíček, R, additional, Lee, S, additional, Mazzucato, M T, additional, Rogers, D J, additional, Rout, M P, additional, Sejpka, J, additional, Tanner, C, additional, Terentev, I A, additional, and Urvoy, D, additional

Published
2022
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24. Relaxation dynamics in excited helium nanodroplets probed with high resolution, time-resolved photoelectron spectroscopy

Author

LaForge, A. C., primary, Asmussen, J. D., additional, Bastian, B., additional, Bonanomi, M., additional, Callegari, C., additional, De, S., additional, Di Fraia, M., additional, Gorman, L., additional, Hartweg, S., additional, Krishnan, S. R., additional, Kling, M. F., additional, Mishra, D., additional, Mandal, S., additional, Ngai, A., additional, Pal, N., additional, Plekan, O., additional, Prince, K. C., additional, Rosenberger, P., additional, Aguirre Serrata, E., additional, Stienkemeier, F., additional, Berrah, N., additional, and Mudrich, M., additional

Published
2022
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27. Enhancement of Above Threshold Ionization in Resonantly Excited Helium Nanodroplets

Author

Michiels, R., primary, Abu-samha, M., additional, Madsen, L. B., additional, Binz, M., additional, Bangert, U., additional, Bruder, L., additional, Duim, R., additional, Wituschek, A., additional, LaForge, A. C., additional, Squibb, R. J., additional, Feifel, R., additional, Callegari, C., additional, Di Fraia, M., additional, Danailov, M., additional, Manfredda, M., additional, Plekan, O., additional, Prince, K. C., additional, Rebernik, P., additional, Zangrando, M., additional, Stienkemeier, F., additional, and Mudrich, M., additional

Published
2021
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29. Ultrafast Resonant Interatomic Coulombic Decay Induced by Quantum Fluid Dynamics

Author

LaForge, A. C., primary, Michiels, R., additional, Ovcharenko, Y., additional, Ngai, A., additional, Escartín, J. M., additional, Berrah, N., additional, Callegari, C., additional, Clark, A., additional, Coreno, M., additional, Cucini, R., additional, Di Fraia, M., additional, Drabbels, M., additional, Fasshauer, E., additional, Finetti, P., additional, Giannessi, L., additional, Grazioli, C., additional, Iablonskyi, D., additional, Langbehn, B., additional, Nishiyama, T., additional, Oliver, V., additional, Piseri, P., additional, Plekan, O., additional, Prince, K. C., additional, Rupp, D., additional, Stranges, S., additional, Ueda, K., additional, Sisourat, N., additional, Eloranta, J., additional, Pi, M., additional, Barranco, M., additional, Stienkemeier, F., additional, Möller, T., additional, and Mudrich, M., additional

Published
2021
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30. Analysis of two-color photoelectron spectroscopy for attosecond metrology at seeded free-electron lasers

Author

Maroju, P K, primary, Grazioli, C, additional, Di Fraia, M, additional, Moioli, M, additional, Ertel, D, additional, Ahmadi, H, additional, Plekan, O, additional, Finetti, P, additional, Allaria, E, additional, Giannessi, L, additional, De Ninno, G, additional, Spampinati, S, additional, Lutman, A A, additional, Squibb, R J, additional, Feifel, R, additional, Carpeggiani, P, additional, Reduzzi, M, additional, Mazza, T, additional, Meyer, M, additional, Bengtsson, S, additional, Ibrakovic, N, additional, Simpson, E R, additional, Mauritsson, J, additional, Csizmadia, T, additional, Dumergue, M, additional, Kühn, S, additional, Harshitha, N G, additional, You, D, additional, Ueda, K, additional, Labeye, M, additional, Bækhøj, J E, additional, Schafer, K J, additional, Gryzlova, E V, additional, Grum-Grzhimailo, A N, additional, Prince, K C, additional, Callegari, C, additional, and Sansone, G, additional

Published
2021
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31. Autoionization dynamics of helium nanodroplets resonantly excited by intense XUV laser pulses

Author

Ovcharenko, Y., Laforge, A. C., Langbehn, B., Plekan, O., Cucini, R., Finetti, P., O'Keeffe, P., Iablonskyi, D., Nishiyama, T., Ueda, K., Piseri, P., Di Fraia, M., Richter, R., Coreno, M., Callegari, C., Prince, K. C., Stienkemeier, F., Möller, T., and Mudrich, M.

Subjects
He nanodroplets, nanoplasma, Physics::Atomic and Molecular Clusters, ddc:530, collective autoionization, interatomic Coulombic decay, Physics::Atomic Physics
Abstract

The ionization dynamics of helium droplets irradiated by intense, femtosecond extreme ultraviolet (XUV) pulses is investigated in detail by photoelectron spectroscopy. Helium droplets are resonantly excited to atomic-like 2p states with a photon energy of 21.5 eV and autoionize by interatomic Coulombic decay (ICD). A complex evolution of the electron spectra as a function of droplet size (250 to 106 He atoms per droplet) and XUV intensity (109-1012 W cm-2) is observed, ranging from narrow atomic-like peaks that are due to binary autoionization, to an unstructured feature characteristic of electron emission from a nanoplasma. The experimental results are analyzed and interpreted with the help of a numerical simulation based on rate equations taking into account all relevant processes - multi-step ionization, electronic relaxation, ICD, secondary inelastic collisions, desorption of electronically excited atoms, and collective autoionization (CAI).

Published
2020
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32. Ultrafast relaxation of photoexcited superfluid He nanodroplets

Author

German Research Foundation, National Science Foundation (US), Carl Zeiss Foundation, Ministerio de Ciencia, Innovación y Universidades (España), Agencia Estatal de Investigación (España), European Commission, Swiss National Science Foundation, Department of Energy (US), Mudrich, M., LaForge, A. C., Ciavardini, A., O’Keeffe, P., Callegari, C., Coreno, M., Demidovich, A., Devetta, M., Di Fraia, M., Drabbels, M., Finetti, P., Gessner, O., Grazioli, C., Hernando de Castro, Alberto, Neumark, D. M., Ovcharenko, Y., Piseri, P., Plekan, O., Prince, K. C., Richter, R., Ziemkiewicz, M. P., Möller, T., Eloranta, J., Pi, Martí, Barranco, Manuel, Stienkemeier, F., German Research Foundation, National Science Foundation (US), Carl Zeiss Foundation, Ministerio de Ciencia, Innovación y Universidades (España), Agencia Estatal de Investigación (España), European Commission, Swiss National Science Foundation, Department of Energy (US), Mudrich, M., LaForge, A. C., Ciavardini, A., O’Keeffe, P., Callegari, C., Coreno, M., Demidovich, A., Devetta, M., Di Fraia, M., Drabbels, M., Finetti, P., Gessner, O., Grazioli, C., Hernando de Castro, Alberto, Neumark, D. M., Ovcharenko, Y., Piseri, P., Plekan, O., Prince, K. C., Richter, R., Ziemkiewicz, M. P., Möller, T., Eloranta, J., Pi, Martí, Barranco, Manuel, and Stienkemeier, F.

Abstract

The relaxation of photoexcited nanosystems is a fundamental process of light–matter interaction. Depending on the couplings of the internal degrees of freedom, relaxation can be ultrafast, converting electronic energy in a few fs, or slow, if the energy is trapped in a metastable state that decouples from its environment. Here, we study helium nanodroplets excited resonantly by femtosecond extreme-ultraviolet (XUV) pulses from a seeded free-electron laser. Despite their superfluid nature, we find that helium nanodroplets in the lowest electronically excited states undergo ultrafast relaxation. By comparing experimental photoelectron spectra with time-dependent density functional theory simulations, we unravel the full relaxation pathway: Following an ultrafast interband transition, a void nanometer-sized bubble forms around the localized excitation (He∗) within 1 ps. Subsequently, the bubble collapses and releases metastable He∗ at the droplet surface. This study highlights the high level of detail achievable in probing the photodynamics of nanosystems using tunable XUV pulses.

Published
2020

33. Evolution and ion kinetics of a XUV-induced nanoplasma in ammonia clusters

Author

Michiels, R, primary, LaForge, A C, additional, Bohlen, M, additional, Callegari, C, additional, Clark, A, additional, von Conta, A, additional, Coreno, M, additional, Di Fraia, M, additional, Drabbels, M, additional, Finetti, P, additional, Huppert, M, additional, Oliver, V, additional, Plekan, O, additional, Prince, K C, additional, Stranges, S, additional, Wörner, H J, additional, and Stienkemeier, F, additional

Published
2021
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35. Time-resolved quantum beats in the fluorescence of helium resonantly excited by XUV radiation

Author

LaForge, A C, primary, Benediktovitch, A, additional, Sukharnikov, V, additional, Krušič, Š, additional, Žitnik, M, additional, Debatin, M, additional, Falcone, R W, additional, Asmussen, J D, additional, Mudrich, M, additional, Michiels, R, additional, Stienkemeier, F, additional, Badano, L, additional, Callegari, C, additional, Di Fraia, M, additional, Ferianis, M, additional, Giannessi, L, additional, Plekan, O, additional, Prince, K C, additional, Spezzani, C, additional, Rohringer, N, additional, and Berrah, N, additional

Published
2020
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36. Photoelectron spectra and angular distribution in sequential two-photon double ionization in the region of autoionizing resonances of ArII and KrII

Author

Kiselev, M D, primary, Carpeggiani, P A, additional, Gryzlova, E V, additional, Burkov, S M, additional, Reduzzi, M, additional, Dubrouil, A, additional, Faccialá, D, additional, Negro, M, additional, Ueda, K, additional, Frassetto, F, additional, Stienkemeier, F, additional, Ovcharenko, Y, additional, Meyer, M, additional, Di Fraia, M, additional, Plekan, O, additional, Prince, K C, additional, Callegari, C, additional, Sansone, G, additional, and Grum-Grzhimailo, A N, additional

Published
2020
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37. Autoionization dynamics of helium nanodroplets resonantly excited by intense XUV laser pulses

Author

Ovcharenko, Y, primary, LaForge, A C, additional, Langbehn, B, additional, Plekan, O, additional, Cucini, R, additional, Finetti, P, additional, O’Keeffe, P, additional, Iablonskyi, D, additional, Nishiyama, T, additional, Ueda, K, additional, Piseri, P, additional, Di Fraia, M, additional, Richter, R, additional, Coreno, M, additional, Callegari, C, additional, Prince, K C, additional, Stienkemeier, F, additional, Möller, T, additional, and Mudrich, M, additional

Published
2020
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40. Core-level Time Resolved Spectroscopy of Photoelectron Circular Dichroism in Fenchone

Author

Faccialà, D., primary, Devetta, M., additional, Beauvarlet, S., additional, Besley, N., additional, Calegari, F., additional, Callegari, C., additional, Catone, D., additional, Cinquanta, E., additional, Ciriolo, A., additional, Colaizzi, L., additional, Coreno, M., additional, Crippa, G., additional, De Ninno, G., additional, Di Fraia, M., additional, Galli, M., additional, Garcia, G., additional, Mairesse, Y., additional, Negro, M., additional, Plekan, O., additional, Powis, I., additional, Geetha, P. Prasannan, additional, Prince, K., additional, Pusala, A., additional, Stagira, S., additional, Turchini, S., additional, Ueda, K., additional, You, D., additional, Zema, N., additional, Nahon, L., additional, Blanchet, V., additional, and Vozzi, C., additional

Published
2020
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41. Attosecond delays in photoionization studied with coherent-controlled FEL

Author

You, D, primary, Ueda, K, additional, Tugs, O, additional, Orimo, Y, additional, Sato, T, additional, Ishikawa, K L, additional, Gryzlova, E V, additional, Staroselskaya, E I, additional, Grum-Grzhimailo, A N, additional, Carpeggiani, P A, additional, Csizmadia, T, additional, Füle, M, additional, Harshitha, N G, additional, Sansone, G, additional, Maroju, P K, additional, Meyer, M, additional, Mazza, T, additional, D’Elia, A, additional, Callegari, C, additional, Di Fraia, M, additional, Plekan, O, additional, Giannessi, L, additional, Allaria, E M, additional, De Ninno, G, additional, Trovò, M, additional, Badano, L, additional, Diviacco, B, additional, Gauthier, D, additional, Mirian, N S, additional, Penco, G M, additional, Rebernik, P R, additional, Spampinati, S, additional, Spezzani, C, additional, Gaio, G, additional, and Prince, K C, additional

Published
2020
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42. Acetylacetone photodynamics at a seeded free-electron laser

Author

Squibb, R., Sapunar, M., Ponzi, A., Richter, R., Kivimäki, A., Plekan, O., Finetti, P., Sisourat, N., Zhaunerchyk, V., Marchenko, T., Journel, L., Guillemin, R., Cucini, R., Coreno, M., Grazioli, C., Di Fraia, M., Callegari, C., Prince, K., Decleva, P., Simon, M., Eland, J., Došlić, N., Feifel, R., Piancastelli, M., University of Gothenburg (GU), Centre de Recherche en Cancérologie de Marseille (CRCM), Centre National de la Recherche Scientifique (CNRS)-Institut National de la Santé et de la Recherche Médicale (INSERM)-Institut Paoli-Calmettes, Fédération nationale des Centres de lutte contre le Cancer (FNCLCC)-Fédération nationale des Centres de lutte contre le Cancer (FNCLCC)-Aix Marseille Université (AMU), Laboratoire de Chimie Physique - Matière et Rayonnement (LCPMR), Université Pierre et Marie Curie - Paris 6 (UPMC)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Department of Physics [Gothenburg], Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS), RIKEN - Institute of Physical and Chemical Research [Japon] (RIKEN), LENS and Dip. di Fisica, Università di Firenze, Università degli Studi di Firenze = University of Florence [Firenze] (UNIFI), Istituto di Struttura della Materia, Consiglio Nazionale delle Ricerche [Roma] (CNR), Università degli studi di Trieste, Univ Trieste, Dept Phys, I-34127 Trieste, Italy, Sincrotrone Trieste, Laboratoire pour l'utilisation du rayonnement électromagnétique (LURE), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-MENRT-Centre National de la Recherche Scientifique (CNRS), Aix Marseille Université (AMU)-Institut Paoli-Calmettes, Fédération nationale des Centres de lutte contre le Cancer (FNCLCC)-Fédération nationale des Centres de lutte contre le Cancer (FNCLCC)-Institut National de la Santé et de la Recherche Médicale (INSERM)-Centre National de la Recherche Scientifique (CNRS), Dipartimento di Fisica e Astronomia [Firenze], Università degli Studi di Firenze = University of Florence (UniFI), National Research Council of Italy | Consiglio Nazionale delle Ricerche (CNR), Università degli studi di Trieste = University of Trieste, Squibb, R. J., Sapunar, M., Ponzi, A., Richter, R., Kivimäki, A., Plekan, O., Finetti, P., Sisourat, N., Zhaunerchyk, V., Marchenko, T., Journel, L., Guillemin, R., Cucini, R., Coreno, M., Grazioli, C., Di Fraia, M., Callegari, C., Prince, K. C., Decleva, P., Simon, M., Eland, J. H. D., Došlić, N., Feifel, R., and Piancastelli, M. N.

Subjects
[PHYS]Physics [physics], Science, Acetylacetone, free electron laser, Article, Chemistry, [CHIM]Chemical Sciences, lcsh:Q, Astrophysics::Earth and Planetary Astrophysics, lcsh:Science, photodynamics, ComputingMilieux_MISCELLANEOUS
Abstract

The first steps in photochemical processes, such as photosynthesis or animal vision, involve changes in electronic and geometric structure on extremely short time scales. Time-resolved photoelectron spectroscopy is a natural way to measure such changes, but has been hindered hitherto by limitations of available pulsed light sources in the vacuum-ultraviolet and soft X-ray spectral region, which have insufficient resolution in time and energy simultaneously. The unique combination of intensity, energy resolution, and femtosecond pulse duration of the FERMI-seeded free-electron laser can now provide exceptionally detailed information on photoexcitation–deexcitation and fragmentation in pump-probe experiments on the 50-femtosecond time scale. For the prototypical system acetylacetone we report here electron spectra measured as a function of time delay with enough spectral and time resolution to follow several photoexcited species through well-characterized individual steps, interpreted using state-of-the-art static and dynamics calculations. These results open the way for investigations of photochemical processes in unprecedented detail., The first steps in photochemical processes involve changes in electronic and geometric structure on extremely short timescales. Here, the authors report femtosecond dynamics in prototypical acetylacetone, by pump-probe photoexcitation-photoemission experiments and static and dynamics calculations.

Published
2018
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43. Control of H 2 Dissociative Ionization in the Nonlinear Regime Using Vacuum Ultraviolet Free-Electron Laser Pulses

Author

Holzmeier, F., Bello, R. Y., Hervé, M., Achner, A., Baumann, T. M., Meyer, M., Finetti, P., Di Fraia, M., Gauthier, D., Roussel, E., Plekan, O., Richter, R., Prince, K. C., Callegari, C., Bachau, H., Palacios, A., Martin, F., Dowek, D., INFM-Dipartimento di Fisica-Politecnico di Milano, Istituto Nazionale di Fisica Nucleare (INFN), Museum d'Aquitaine, Laboratoire d'interaction du rayonnement X avec la matière (LIXAM), Université Paris-Sud - Paris 11 (UP11)-Centre National de la Recherche Scientifique (CNRS), Centre de Recherche en Cancérologie de Marseille (CRCM), Aix Marseille Université (AMU)-Institut Paoli-Calmettes, Fédération nationale des Centres de lutte contre le Cancer (FNCLCC)-Fédération nationale des Centres de lutte contre le Cancer (FNCLCC)-Institut National de la Santé et de la Recherche Médicale (INSERM)-Centre National de la Recherche Scientifique (CNRS), Università degli studi di Trieste = University of Trieste, Chimie Et Interdisciplinarité : Synthèse, Analyse, Modélisation (CEISAM), Université de Nantes - UFR des Sciences et des Techniques (UN UFR ST), Université de Nantes (UN)-Université de Nantes (UN)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Biologie et écologie tropicale et méditerranéenne [2007-2010] (BETM), Université de Perpignan Via Domitia (UPVD)-École Pratique des Hautes Études (EPHE), Université Paris sciences et lettres (PSL)-Université Paris sciences et lettres (PSL)-Centre National de la Recherche Scientifique (CNRS), Sincrotrone Trieste, Centre d'Etudes Lasers Intenses et Applications (CELIA), Université de Bordeaux (UB)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Centre National de la Recherche Scientifique (CNRS), Laboratoire des collisions atomiques et moléculaires (LCAM), Centre National de la Recherche Scientifique (CNRS)-Institut National de la Santé et de la Recherche Médicale (INSERM)-Institut Paoli-Calmettes, Fédération nationale des Centres de lutte contre le Cancer (FNCLCC)-Fédération nationale des Centres de lutte contre le Cancer (FNCLCC)-Aix Marseille Université (AMU), Univ Trieste, Dept Phys, I-34127 Trieste, Italy, Université de Nantes (UN)-Université de Nantes (UN)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC), Université de Perpignan Via Domitia (UPVD)-École pratique des hautes études (EPHE), and Centre National de la Recherche Scientifique (CNRS)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université de Bordeaux (UB)

Subjects
[PHYS]Physics [physics], ComputingMilieux_MISCELLANEOUS
Abstract

International audience

Published
2018
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44. Acetylacetone photodynamics at a seeded freeelectron laser

Author

Squibb, R. J., Sapunar, Marin, Ponzi, A., Richter, R., Kivimäki, A., Plekan, O., Finetti, P., Sisourat, N., Zhaunerchyk, V., Marchenko, T., Journel, L., Guillemin, R., Cucini, R., Coreno, M., Grazioli, C., Di Fraia, M., Callegari, C., Prince, K. C., Decleva, P., Simon, M., Eland, J. H. D., Došlić, Nađa, Feifel, R., and Piancastelli, M. N.

Subjects
Chemistry, Acetylacetone, photodynamics, seeded free electron laser
Abstract

The first steps in photochemical processes, such as photosynthesis or animal vision, involve changes in electronic and geometric structure on extremely short time scales. Time-resolved photoelectron spectroscopy is a natural way to measure such changes, but has been hindered hitherto by limitations of available pulsed light sources in the vacuum-ultraviolet and soft Xray spectral region, which have insufficient resolution in time and energy simultaneously. The unique combination of intensity, energy resolution, and femtosecond pulse duration of the FERMI-seeded free-electron laser can now provide exceptionally detailed information on photoexcitation–deexcitation and fragmentation in pump-probe experiments on the 50- femtosecond time scale. For the prototypical system acetylacetone we report here electron spectra measured as a function of time delay with enough spectral and time resolution to follow several photoexcited species through well-characterized individual steps, interpreted using state-of-the-art static and dynamics calculations. These results open the way for investigations of photochemical processes in unprecedented detail.

Published
2018

45. Control of H2 Dissociative Ionization in the Nonlinear Regime Using Vacuum Ultraviolet Free-Electron Laser Pulses

Author

Holzmeier F., Bello R.Y., Hervé M., Achner A., Baumann T.M., Meyer M., Finetti P., Di Fraia M., Gauthier D., Roussel E., Plekan O., Richter R., Prince K.C., Callegari C., Bachau H., Palacios A., Martín F., Dowek D. and This research was supported by 'Investissements d’Avenir' LabEx PALM (ANR-10-LABX-0039-PALM) and EquipEx ATTOLAB (ANR-11-EQPX-0005-ATTOLAB), as well as by the EU-H2020 Laserlab-Europe 654148. This work is supported by the ERC advanced Grant No. 290853—XCHEM—within the seventh framework program of the European Union. We also acknowledge the financial support from the MINECO Project No. FIS2016-77889-R and the European COST Action XLIC CM1204 and the computer time from the CCC-UAM and Marenostrum Supercomputer. A.?P. acknowledges a Ramón y Cajal contract from the Ministerio de Economía y Competitividad (Spain). F.?M. acknowledges support from the 'Severo Ochoa' Program for Centres of Excellence in R&D (MINECO, Grant No. SEV-2016-0686) and the 'María de Maeztu' Program for Units of Excellence in R&D (MDM-2014-0377). D.?D. and M.?H. acknowledge support by Institut de Physique (CNRS). M.?M. acknowledges support by the Deutsche Forschungsgemeinschaft (DFG) under Grants No. SFB925/A3 and CUI, No. DFG-EXC1074. We gratefully acknowledge the members of the FERMI team at Elettra-Sincrotrone Trieste whose work made this experiment possible.

Published
2018

46. Real-Time Dynamics of the Formation of Hydrated Electrons upon Irradiation of Water Clusters with Extreme Ultraviolet Light

Author

LaForge, A. C., primary, Michiels, R., additional, Bohlen, M., additional, Callegari, C., additional, Clark, A., additional, von Conta, A., additional, Coreno, M., additional, Di Fraia, M., additional, Drabbels, M., additional, Huppert, M., additional, Finetti, P., additional, Ma, J., additional, Mudrich, M., additional, Oliver, V., additional, Plekan, O., additional, Prince, K. C., additional, Shcherbinin, M., additional, Stranges, S., additional, Svoboda, V., additional, Wörner, H. J., additional, and Stienkemeier, F., additional

Published
2019
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47. Acetylacetone photodynamics at a seeded free-electron laser

Author

Squibb, R. J., Sapunar, M., Ponzi, A., Richter, R., Kivimaki, A., Plekan, O., Finetti, P., Sisourat, N., Zhaunerchyk, V., Marchenko, T., Journel, L., Guillemin, R., Cucini, R., Coreno, M., Grazioli, C., Di Fraia, M., Callegari, C., Prince, K. C., Decleva, P., Simon, M., Eland, J. H. D., Doslic, N., Feifel, R., Piancastelli, Maria Novella, Squibb, R. J., Sapunar, M., Ponzi, A., Richter, R., Kivimaki, A., Plekan, O., Finetti, P., Sisourat, N., Zhaunerchyk, V., Marchenko, T., Journel, L., Guillemin, R., Cucini, R., Coreno, M., Grazioli, C., Di Fraia, M., Callegari, C., Prince, K. C., Decleva, P., Simon, M., Eland, J. H. D., Doslic, N., Feifel, R., and Piancastelli, Maria Novella

Abstract

The first steps in photochemical processes, such as photosynthesis or animal vision, involve changes in electronic and geometric structure on extremely short time scales. Time-resolved photoelectron spectroscopy is a natural way to measure such changes, but has been hindered hitherto by limitations of available pulsed light sources in the vacuum-ultraviolet and soft Xray spectral region, which have insufficient resolution in time and energy simultaneously. The unique combination of intensity, energy resolution, and femtosecond pulse duration of the FERMI-seeded free-electron laser can now provide exceptionally detailed information on photoexcitation-deexcitation and fragmentation in pump-probe experiments on the 50-femtosecond time scale. For the prototypical system acetylacetone we report here electron spectra measured as a function of time delay with enough spectral and time resolution to follow several photoexcited species through well-characterized individual steps, interpreted using state-of-the-art static and dynamics calculations. These results open the way for investigations of photochemical processes in unprecedented detail.

Published
2018
Full Text
View/download PDF

48. Control of H2 Dissociative Ionization in the Nonlinear Regime Using Vacuum Ultraviolet Free-Electron Laser Pulses

Author

Holzmeier F., Bello R.Y., Hervé M., Achner A., Baumann T.M., Meyer M., Finetti P., Di Fraia M., Gauthier D., Roussel E., Plekan O., Richter R., Prince K.C., Callegari C., Bachau H., Palacios A., Martín, Fernando, Dowek D., Holzmeier F., Bello R.Y., Hervé M., Achner A., Baumann T.M., Meyer M., Finetti P., Di Fraia M., Gauthier D., Roussel E., Plekan O., Richter R., Prince K.C., Callegari C., Bachau H., Palacios A., Martín, Fernando, and Dowek D.

Published
2018

49. Extreme ultraviolet ionization of pure He nanodroplets: Mass-correlated photoelectron imaging, Penning ionization, and electron energy-loss spectra.

Author

Buchta, D., Krishnan, S. R., Brauer, N. B., Drabbels, M., O'Keeffe, P., Devetta, M., Di Fraia, M., Callegari, C., Richter, R., Coreno, M., Prince, K. C., Stienkemeier, F., Ullrich, J., Moshammer, R., and Mudrich, M.

Subjects
PENNING ionization, DROPLETS, ULTRAVIOLET radiation, HELIUM ions, ANGULAR distribution (Nuclear physics), SIMULTANEITY (Physics), AUGER effect, ELECTRON energy loss spectroscopy
Abstract

The ionization dynamics of pure He nanodroplets irradiated by Extreme ultraviolet radiation is studied using Velocity-Map Imaging PhotoElectron-PhotoIon COincidence spectroscopy. We present photoelectron energy spectra and angular distributions measured in coincidence with the most abundant ions He+, He2+, and He3+. Surprisingly, below the autoionization threshold of He droplets, we find indications for multiple excitation and subsequent ionization of the droplets by a Penning-like process. At high photon energies we observe inelastic collisions of photoelectrons with the surrounding He atoms in the droplets. [ABSTRACT FROM AUTHOR]

Published
2013
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