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Forschung an Atomen, Molekülen und Clustern mit hoch intensiven XUV Laserpulsen von Freie-Elektronen-Lasern (FERMI)

Forschung an Atomen, Molekülen und Clustern mit hoch intensiven XUV Laserpulsen von Freie-Elektronen-Lasern (FERMI)


A primary goal in both chemistry and physics is to map reaction dynamics on atomic and electronic timescales. Research in this field includes many topics with various complexity, ranging from the dynamic of a highly complex protein unfolding, which is essential in molecular biology, to a simple proton transfer in water, which is important for radical formation in atmospheric chemistry. The recent development of extreme ultraviolet (XUV) free electron lasers (FELs) has opened up many new and exciting possibilities to study reaction dynamics in real-time. Our research group headed an international collaboration to successfully commission the low density matter (LDM) endstation at the FEL FERMI in Trieste (Fig. 1b). This experimental setup combines ultrashort coherent XUV FEL pulses with neutral and charged particle imaging methods to study a wide array of samples in the gas phase.

An intriguing class of gas-phase samples are atoms and molecules condensed into finite-sized clusters. Depending on the choice of constituents, these nanoparticles provide ideal model systems for the study of fundamental physical, chemical and biological processes. Examples studied in our group are superfluid helium droplets showing peculiar physical properties, or biological systems such as water and ammonia clusters, providing new insights into the nature of solvated electrons (Fig. 1).

Pump probe delay

The coherent XUV radiation from FERMI allows us to design unique experiments where we either induce single-component reactions, like the formation of a solvated electron, or completely destroy the cluster forming a nanometer sized plasma, a nanoplasma. Pump-probe techniques with an additional ultraviolet, visible or infrared laser, or two XUV pulses created by a split-and-delay unit, enable us to time-resolve these processes on a femtosecond timescale. Current and future experiments focus on the study of inner- and intramolecular dynamics of XUV irradiated clusters built of small biomolecules, for example alcohols, ammonia or water.

Figure 1: Formation of a solvated electron after XUV irradiation of water clusters [1].

Luftbild FERMI

Figure 2: Free Electron Laser FERMI and synchrotron Elettra in Trieste, Italy.


Relevante Publikationen:

[11] Ovcharenko Y, Lyamayev V, Katzy R, Devetta M, LaForge A, O’Keeffe P, Plekan O, Finetti P, Di Fraia M, Mudrich M, Krikunova M, Piseri P, Coreno M, Brauer N, Mazza T, Stranges S, Grazioli C, Richter R, Prince K C, Drabbels M, Callegari C, Stienkemeier F, Möller T:
Novel Collective Autoionization Process Observed in Electron Spectra of He Clusters
Phys Rev Lett

[10] García-Alfonso E, Coppens F, Barranco M, Pi M, Stienkemeier F, Halberstadt N
Alkali atoms attached to vortex-hosting helium nanodroplets
Chem Phys, 2020; 152: 194109-1-194109-9.: abstract - pdf

[9] 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, Svoboda V, Wörner H J, Stienkemeier F
Time-resolved formation of excited atomic and molecular states in XUV-induced nanoplasmas in ammonia clusters
Phys Chem Chem Phys, 2020; 22: 7828-7834.: abstract - pdf - arXiv

[8] 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 A, Neumark D M, Ovcharenko Y, Piseri P, Plekan O, Prince K C, Richter R, Ziemkiewicz M P, Möller T, Eloranta J, Pi M, Barranco M, Stienkemeier F:
Ultrafast relaxation of photoexcited superfluid He nanodroplets
Nat Commun, 2020; 11 (112): 1-7.: abstract - pdf - arxiv

[7] Svoboda V, Michiels R, LaForge A C, Med J, Stienkemeier F, Slavíček P, Wörner H J:
Real-time observation of water radiolysis and hydrated electron formation induced by extreme-ultraviolet pulses
Sci Adv, 2020; 6 (3): 1-8.: abstract - pdf

[6] Zimmermann J, Langbehn B, Cucini R, Di Fraia M, Finetti P, LaForge A C, Nishiyama T, Ovcharenko O, Piseri P, Plekan O, Prince K C, Stienkemeier F, Ueda K, Callegari C, Möller T, Rupp D:
Deep neural networks for classifying complex features in diffraction images
Phys Rev E, 2019; 99 (6): 063309-1-063309-20.: abstract - pdf - arXiv

[5] LaForge A, Michiels R, Bohlen M, Callegari C, Clark A, von Conta A, Coreno M, Di Fraia M, Drabbels M, Huppert M, Finetti P, Ma J, Mudrich M, Oliver V, Plekan O, Prince K C, Shcherbinin M, Stranges S, Svoboda V, Wörner H J, Stienkemeier F:
Real-Time Dynamics of the Formation of Hydrated Electrons upon Irradiation of Water Clusters with Extreme Ultraviolet Light
Phys Rev Lett, 2019; 122 (13): 133001-1-133001-5.: abstract - pdf

[4] LaForge A C, Shcherbinin M, Stienkemeier F, Richter R, Moshammer R, Pfeifer T, Mudrich M:
Highly efficient double ionization of mixed alkali dimers by intermolecular Coulombic decay
Nat Phys, 2019; 15: 247-250.: abstract - pdf - arXiv

[3] Langbehn B, Sander K, Ovcharenko Y, Peltz C, Clark A, Coreno M, Cucini R, Drabbels M, Finetti P, Di Fraia M, Giannessi L, Grazioli C, Iablonskyi D, LaForge A, Nishiyama T, Álvarez de Lara V, Piseri P, Plekan O, Ueda K, Zimmermann J, Prince K C, Stienkemeier F, Callegari C, Fennel T, Rupp D, Möller T:
Three-Dimensional Shapes of Spinning Helium Nanodroplets
Phys Rev Lett, 2018; 121 (25): 255301-1-255301-6.: abstract - pdf - arXiv

[2] Shcherbinin M, LaForge A C, Sharma V, Devetta M, Richter R, Moshammer R, Pfeifer S T, Mudrich M:
Interatomic Coulombic decay in helium nanodroplets
Phys Rev A, 2017; 96 (1): 013407-1-013407-5.: abstract - pdf - arXiv

[1] Takanashi T, Golubev N V, Callegari C, Fukuzawa H, Motomura K, Iablonsky D, Kumagai Y, Mondal S, Tachibana T, Nagaya K, Nishiyama T, Matsunami K, Johnsson P, Piseri P, Sansone G, Dubrouil A, Reduzzi M, Carpeggiani P, Vozzi C, Devetta M, Negro M, Faccialà D, Calegari F, Trabattoni A, Castrovilli M C, Ovcharenko Y, Mudrich M, Stienkemeier F, Coreno M, Alagia M, Schütte B, Berrah N, Plekan O, Finetti P, Spezzani C, Ferrari E, Allaria E, Penco G, Serpico C, De Ninno G, Diviacco B, Di Mitri S, Giannessi L, Jabbari G, Prince K C, Cederbaum L S, Demekhin Ph V, Kuleff A I, Ueda K:
Time-Resolved Measurement of Interatomic Coulombic Decay Induced by Two-Photon Double Excitation of Ne2
Phys Rev Lett, 2017; 118 (3): 033202-1-033202-6.: abstract - pdf - arXiv




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