1. Attosecond XUV-pump/IR-probe measurements were conducted on several gas-phase donor-acceptor systems, namely, nitroanilines and biphenyl derivatives. The results were interpreted by means of state-of-the art theoretical calculations. We found that CT can be much faster than anticipated (~10 fs) and even reversible. We also performed measurements in C60 and observed time delays of approximately 300 attoseconds, attributed to electron correlation effects associated with plasmonic resonances.
2. A beamline for soft X-ray generation has been developed, driven by IR pulses with durations down to ~10 fs and tunable wavelengths in the 1.1–2.6 µm range.
3. Ultrashort deep-UV (DUV) and UV pulses tuneable within the 200–350 nm spectral range have been generated using the resonant dispersive wave (RDW) emission process. The minimum pulse duration achieved is 2.4 fs.
4. An attosecond UV-pump/XUV-probe beamline has been implemented with active stabilization of the pump–probe delay. First time-resolved UV-XUV measurements validated a ~3-fs instrumental response via cross-correlation in argon.
5. Time dependent versions of XCHEM and esx-DFT have been developed from the existing time-independent versions. For diatomic and triatomic molecules, the effect of nuclear motion and the coupling of this motion with the electronic one were described in a full quantum mechanical way.
6. A new theoretical method, PFM-TSH, has been developed and successfully tested to properly account for the evolution of the electronic coherences created by few-fs UV pulses in the framework of a classical trajectory approach, which is the only one feasible for large molecules.
7. Time-resolved UV-pump/XUV-probe experiments with ~3-fs time resolution were performed on gas-phase pyrazine and isopropoxy-nitrobenzene. For pyrazine, theoretical calculations using the newly developed computational methods have provided time-resolved photoelectron spectra directly comparable with the experimental ones.
8. Theoretical identification of Graphene/SiC as an ideal substrate for deposition of organic molecules without destroying their donor-acceptor character while keeping them firmly bonded to the substrate.
9. Enantioselective synthesis of molecular nanographenes has been carried out for the first time, thus avoiding the use of expensive and time-consuming HPLC chromatography and paving the way to the preparation of these materials in gram amounts for practical applications.
