Working Group 4

Deliverable 9. Controlled low-temperature aggregation and substrate-deposition of multicomponent metal nanostructures along with Working Group 3 (M26); Deposition and ex-situ characterization of relevant organo-metallic nanoparticles (M48).

9.1. Synthesis, characterization and surface deposition of technologically relevant prototypes of high-purity materials.

Delivered – Great efforts have been made, both theoretically and experimentally, to explore the aggregation, in-situ characterization, and substrate-deposition of metal nanostructure and other types of high-purity materials in helium nanodroplets, including metal-non-metal complexes, diamondoids, and polycyclic aromatic hydrocarbons, resulting in 10 publications.

  1. “Superfluid helium droplet-mediated surface-deposition of neutral and charged silver atomic species”. B. Fernández, M. Pi, and M. Pilar de Lara-Castells. Physical Chemistry Chemical Physics 25.25, 16699-16706 (2023); https://doi.org/10.1063/5.0205951
  2. “Structure and formation of copper cluster ions in multiply charged He nanodroplets”, O. V. Lushchikova, M. Gatchell, J. Reichegger, S. Kollotzek, F. Zappa, M. Mahmoodi-Darian and P. Scheier, Phys. Chem. Chem. Phys. 25, 8463-8471 (2023); https://doi.org/10.1039/D2CP04569A
  3. ”Solvation of cationic copper clusters in molecular hydrogen”, O. V. Lushchikova, J. Reichegger, S. Kollotzek, F. Zappa, M. Mahmoodi-Darian, M. Bartolomei, J. Campos-Martínez, T. González-Lezana, F. Pirani and P. Scheier , Phys. Chem. Chem. Phys. 25, 25251-25263 (2023); https://doi.org/10.1039/D3CP03452F
  4. “Nanostructured supramolecular networks from self-assembled diamondoid molecules at ultracold conditions”, M. Alešković, F. Küstner, R. Messner, F. Lackner, W. E. Ernst, M. Šekutor, Physical Chemistry Chemical Physics 25, 17869-17876 (2023); https://doi.org/10.1039/D3CP02367B
  5. “Diamondoid ether clusters in helium nanodroplets”, J. Alić, R. Messner, M. Alešković, F. Küstner, M. Rubčić, F. Lackner, W. E. Ernst, M. Šekutor, Phys. Chem. Chem. Phys. 25, 11951-11958 (2023); https://doi.org/10.1039/D3CP00489A
  6. “Nanostructured supramolecular networks from self-assembled diamondoid molecules under ultracold conditions.”, M. Alešković, F. Küstner, R. Messner, F. Lackner, W. E. Ernst, and M. Šekutor. Physical Chemistry Chemical Physics 25, 17869-17876 (2023); https://doi.org/10.1039/D3CP02367B
  7. “An Ab Initio Journey toward the Molecular‐Level Understanding and Predictability of Subnanometric Metal Clusters”, M. P. de Lara‐Castells, Small Structures (2024): 2400147. https://doi.org/10.1002/sstr.202400147
  8. “The role of Na decoration on the hydrogen adsorption on coronene: A combined experimental and computational study”, E. García-Arroyo, A. M. Reider, S. Kollotzek, F. Foitzik, J. Campos-Martínez, M. Bartolomei, F. Pirani, M. I. Hernández, M. Mella, and P. Scheier, International Journal of Hydrogen Energy 83, 387-395 (2024); https://doi.org/ 10.1016/j.ijhydene.2024.07.425
  9. “Mixed cluster ions of magnesium and C60”, A.M. Reider, J. Mayerhofer, P. Martini, P. Scheier, and O.V. Lushchikova, J. Phys. Chem. A 128 (2024) 848 – 857. https//doi.org/ 10.1021/acs.jpca.3c06902
  10. “Spectroscopic Investigation of Size-Dependent CO2 Binding on Cationic Copper Clusters: Analysis of the CO2 Asymmetric Stretch”, A.M. Reider, M. Szalay, J. Reichegger, J. Barabás, M. Schmidt, M. Kappe, T. Höltzl, P. Scheier, and O. Lushchikova, Phys. Chem. Chem. Phys. 26 (2024) 20355 – 20364; https://doi.org/10.1039/D4CP01797H

9.2. Physics of microsolvation. The fundamental dynamics of solvation of charged particles in superfluid He has been studied to expand the knowledge about the property of He nanodroplets to serve as ultracold substrates for aggregation and characterization of tailored molecular complexes and metal nanostructures.

Delivered, see:

  1. “Time-resolved solvation of alkali ions in superfluid helium nanodroplets”, E. García-Alfonso, M. Barranco, N. Halberstadt, M. Pi, J. Chem. Phys. 160, 164308 (2024). https://doi.org/10.1063/5.0205951
  2. “Computational molecular dynamics simulations of cationic alkali dimers solvated in He clusters: the Li2+ case”, Yanes-Rodríguez R, Rodríguez-Segundo R, Villarreal P, Prosmiti R., The European Physical Journal D., 77(6), 116 (2023). https://doi.org/10.1140/epjd/s10053-023-00691-9
  3. “Doubly charged dimers and trimers of heavy noble gases”, G. Schöpfer, S. Bergmeister, M. Ončák, I. Stromberg, M. Mahmoodi-Darian, P. Scheier, O. Echt, and E. Gruber. Physical Chemistry Chemical Physics 26, 11482-11490 (2024). https//doi.org/10.1039/D4CP00465E

Deliverable 10. Spectroscopic characterization of helium droplet-aggregated organic light-harvesting complexes (M48); New routes for enhancing energy conversion using helium droplets (M48).”

10.1. Charge- and energy-transfer processes in He nanodroplets.

Delivered – Energy conversion by light-harvesting complexes has been intensely studied mostly on the fundamental level of charge- and energy-transfer processes occurring in He nanodroplets. By the end of the Action it is expected that this knowledge and expertise will be redirected to the investigation of specific molecular light-harvesting complexes with high potential for applications.

  1. “Secondary ionization of pyrimidine nucleobases and their microhydrated derivatives in helium nanodroplets”, J. D. Asmussen, A. R. Abid, A. Sundaralingam, B. Bastian, K. Sishodia, S. De, L. Ben Ltaief, S. R. Krishnan, H. B. Pedersen, M. Mudrich, Physical Chemistry Chemical Physics 25, 24819 – 24828 (2023). https://doi.org/10.1039/D3CP02879H
  2. “Dopant ionization and efficiency of ion and electron ejection from helium nanodroplets”, J. D. Asmussen, L. Ben Ltaief, K. Sishodia, A. R. Abid, B. Bastian, S. R. Krishnan, H. B. Pedersen, M. Mudrich, The Journal of Chemical Physics 159, 034301 (2023). https://doi.org/10.1063/5.0160171
  3. “Efficient Indirect Interatomic Coulombic Decay Induced by Photoelectron Impact Excitation in Large He Nanodroplets”, L. Ben Ltaief, K. Sishodia, S. Mandal, S. De, S. R. Krishnan, C. Medina, N. Pal, R. Richter, T. Fennel, and M. Mudrich, Physical Review Letters 131, 023001 (2023). https://doi.org/10.1103/PhysRevLett.131.023001
  4. “Electron energy loss and angular asymmetry induced by elastic scattering in helium droplets”, J. D. Asmussen, K. Sishodia, B. Bastian, A. R. Abid, L. Ben Ltaief, H. B. Pedersen, S. De, C. Medina, N. Pal, R. Richter, T. Fennel, S. R. Krishnan, M. Mudrich, Nanoscale 15, 14025-14031 (2023). https://doi.org/10.1039/D3NR03295G
  5. “Long-lasting XUV activation of helium nanodroplets for avalanche ionization”, C. Medina, A. Ø. Lægdsmand, L. Ben Ltaief, Z. Hoque, A. H. Roos, L Jurkovičová, O. Hort, O. Finke, M. Albrecht, J. Nejdl, F. Stienkemeier, J. Andreasson, E. Klimešová, M. Krikunova, A. Heidenreich and M. Mudrich, New Journal of Physics 25, 053030 (2023). https://doi.org/10.1088/1367-2630/acd5f6
  6. “Spectroscopically resolved resonant interatomic Coulombic decay in photoexcited large He nanodroplets”, L. Ben Ltaief, K. Sishodia, R. Richter, B. Bastian, J. D. Asmussen, S. Mandal, N. Pal, C. Medina, S. R. Krishnan, K. von Haeften, and M. Mudrich, Physical Review Research 6, 013019 (2024). https://doi.org/ 10.1103/PhysRevResearch.6.013019
  7. “Observation of interatomic Coulombic decay induced by double excitation of helium in nanodroplets”, B. Bastian, J. D. Asmussen, L. Ben Ltaief, H. B. Pedersen, K. Sishodia, S. De, S. R. Krishnan, C. Medina, N. Pal, R. Richter, N. Sisourat, and M. Mudrich. Physical Review Letters 132, 233001 (2024). https://doi.org/10.1103/PhysRevLett.132.233001
  8. “Non-adiabatic electronic relaxation of tetracene from its brightest singlet excited state”, A. Scognamiglio, K. S. Thalmann, S. Hartweg, N. Rendler, L. Bruder, P. B. Coto, M. Thoss, F. Stienkemeier, J. Chem. Phys. 161, 024302 (2024). https://doi.org/10.1063/5.0214006

10.2. Fundamental properties of superfluid He nanodroplets

Delivered – As a prerequisite of all studies of aggregation, surface-deposition, in-situ characterization of molecular complexes and metal nanostructures in He nanodroplets, the fundamental properties of He nanodroplets have to be further elucidated, in particular with regard to their shape, structure, superfluidity, and relaxation dynamics. Therefore, a series of theoretical and experimental studies on various fundamental aspects of He nanodroplets was carried out, specifically addressing rotation (quantum vortices, rotating cylinders) and flow (jets and filaments).

  1. “Quantized vortex nucleation in collisions of superfluid nanoscopic helium droplets at zero temperature”, García-Alfonso E, Ancilotto F, Barranco M, Pi M, Halberstadt N., The Journal of Chemical Physics. 21, 159(7) (2023). https://doi.org/10.1063/5.0165820
  2. “Breakup of quantum liquid filaments into droplets”, Francesco Ancilotto, Manuel Barranco, and Martí Pi, Phys. Rev. A 107, 063312 (2023). https://doi.org/10.1103/PhysRevA.107.063312
  3. “Nanoscopic jets and filaments of superfluid 4He at zero temperature: A DFT study”, Ancilotto F, Barranco M, Pi M., The Journal of Chemical Physics. 14, 158(14) (2023). https://doi.org/10.1063/5.0143399
  4. “Relaxation dynamics of 3He and 4He clusters and droplets studied using near infrared and visible fluorescence excitation spectroscopy”, Klaus von Haeften, Tim Laarmann, Hubertus Wabnitz and Thomas Möller, Phys. Chem. Chem. Phys. 25, 1863 (2023). https://doi.org/10.1039/D2CP04594J
  5. “Self-sustained deformable rotating liquid He cylinders: The pure normal fluid 3He and superfluid 4He cases”, M. Pi, F. Ancilotto, M. Barranco, S. L. Butler, and J. M. Escartín, Phys. Rev. B 108, 054524 (2023). https://doi.org/10.1103/PhysRevB.108.054524

10.3. Advanced instrumentation and methods

Delivered – As a prerequisite for carrying out sophisticated experimental studies of confined molecular systems in He nanodroplets, new research instrumentation and methodology needs to be developed. To this end, WG4 has developed advanced spectroscopic instrumentation and methods (a continuously-tunable VUV source, stabilization scheme for laser pulses, a method improving mass spectrometry, an expansion of the experimental endstation MAC at ELI Beamlines).

  1. “Bright continuously-tunable VUV source for ultrafast spectroscopy”, L. Jurkovičová, L. Ben Ltaief, A. H. Roos, O. Hort, O. Finke, M. Albrecht, Z. Hoque, E. Klimešová, A. Sundaralingam, R. Antipenkov, A. Grenfell, A. Špaček, W. Szuba, M. Krikunova, M. Mudrich, J. Nejdl, J. Andreasson, Communications Physics 7, 26 (2024). https://doi.org/ 10.1038/s42005-023-01513-5
  2. “Method of kinetic energy reconstruction from time-of-flight mass spectra”, A. Ngai, K. Dulitz, S. Hartweg, J. C. Franz, M. Mudrich, and F. Stienkemeier. Review of Scientific Instruments 95, 033305 (2024). https://doi.org/10.1063/5.0201425
  3. “Update on MAC End-Station at ELI Beamlines Facility”, E. Klimesová, A. Hult Roos, Z. Hoque, N. Smijesh, R. J. Squibb, H. Coudert-Alteirac, R. Feifel, J. Andreasson, and M. Krikunova. Acta Physica Polonica A 145, 118-122 (2024). https://doi.org/10.12693/APhysPolA.145.118
  4. “Generation of interferometrically stable pulse pairs from a free-electron laser using a birefringent interferometer”, B Ardini, F. Richter, L. Uboldi, P. Cinquegrana, M. Danailov, A. Demidovich, S. D. Ganeshamandiram, S. Hartweg, G. Kurdi, F. Landmesser, M. Michelbach, A. Ngai, I. Nikolov, N. Rendler, F. Stienkemeier, D. Uhl, L. Bruder, G. Cerullo and C. Manzoni, J. Phys. B: At. Mol. Opt. Phys. 57, 075402 (2024). https://doi.org/10.1088/1361-6455/ad2e2d

Deliverable 11. Detailed analysis of astrophysically relevant cold reactions using helium droplets along with Working Group 5 (M48); Controlled low-temperature formation of cosmic dust nanoparticles (M48).

11.1. Spectroscopy of astrophysically relevant species.

Partially delivered and to be completely delivered before the end of the Action.

  1. “Spectroscopy of helium-tagged C60 anions”, M. Kappe, P. Martini, A. Schiller, E. Gruber, F. Zappa, S. A. Krasnokutski, P. Scheier, and M. Gatchell. Physical Review Research 6, L012045 (2024). https://doi.org/10.1103/PhysRevResearch.6.L012045