Femtosecond X-ray-induced fragmentation of fullerenes

Abstract

A new class of femtosecond, intense, short wavelength lasers -the free electron laser -has opened up new opportunities to investigate the structure and dynamics in many scientific areas. These new lasers, whose performance keeps increasing, enable the understanding of physical and chemical changes at an atomic spatial scale and on the time scale of atomic motion which is essential for a broad range of scientific fields. We describe here the interaction of fullerenes in the multiphoton regime with the Linac Coherent Light Source (LCLS) free electron laser at SLAC National Laboratory. In particular, we report on new data regarding the ionization of Ho 3 N@C 80 molecules and compare the results with our prior C 60 investigation of radiation damage induced by the LCLS pulses. We also discuss briefly the potential impact of newly available instrumentation to physical and chemical sciences when they are coupled with FELs as well as theoretical calculations and modeling.

Fullerene Dynamics with X-Ray Free-Electron Lasers

“…The photoionization with 1530 eV leads to the absorption cross section of Ho to be about 1.55 Mb, while that of C was about 0.013 Mb. Our interpretation of the interaction of Ho 3 N@C 80 with 1530 eV photon energy was that the Ho atom charges up and gets multi-ionized due to the cyclic photoionization and Auger decay [51]. In doing so, it grabs electrons from the carbon cage via electron transfer between the Ho and the cage-resulting in the whole parent molecule charging up and reaching at least Ho 3 N@C 80…”

“…We thank all of the authors of references [40,44,51]. We also thank Ms. Rachel Tshonas for her help with the manuscript.…”

The Role of Super-Atom Molecular Orbitals in Doped Fullerenes in a Femtosecond Intense Laser Field

“…and in refs 52 and 53. The ion-mass spectrum of Ho 3 N@C 80 at 800 nm obtained at a laser intensity of 4 × 10 14  W/cm 2 and 30 fs pulse duration is shown in Fig.…”

“…The experiment was performed using an ion velocity map imaging (VMI) spectrometer used in the time of flight (TOF) mode and details are available in the Supplementary information (S.I.) and in refs 52 and 53 . The ion-mass spectrum of Ho 3 N@C 80 at 800 nm obtained at a laser intensity of 4 × 10 14 W/cm 2 and 30 fs pulse duration is shown in Fig.…”

Fragmentation of endohedral fullerene Ho3N@C80 in an intense femtosecond near-infrared laser field

“…Ionization and fragmentation of molecules in femtosecond laser fields is an important method to understand their electronic and nuclear dynamics [1][2][3][4][5][6][7][8][9][10]. Complex molecular targets, such as carbon based nano-size fullerenes, characterized by their hollow geometric structures, attract a great deal of interest due to their broad range of applications and 'supramolecular' physical and chemical properties [11].…”