TY - JOUR A1 - Xiong, Hui A1 - Mignolet, Benoit A1 - Fang, Li A1 - Osipov, Timur A1 - Wolf, Thomas J. A. A1 - Sistrunk, Emily A1 - Gühr, Markus A1 - Remacle, Francoise A1 - Berrah, Nora T1 - The Role of Super-Atom Molecular Orbitals in Doped Fullerenes in a Femtosecond Intense Laser Field JF - Scientific reports N2 - The interaction of gas phase endohedral fullerene Ho3N@C-80 with intense (0.1-5 x 10(14) W/cm(2)), short (30 fs), 800 nm laser pulses was investigated. The power law dependence of Ho3N@C-80(q+), q = 1-2, was found to be different from that of C-60. Time-dependent density functional theory computations revealed different light-induced ionization mechanisms. Unlike in C-60, in doped fullerenes, the breaking of the cage spherical symmetry makes super atomic molecular orbital (SAMO) states optically active. Theoretical calculations suggest that the fast ionization of the SAMO states in Ho3N@C-80 is responsible for the n = 3 power law for singly charged parent molecules at intensities lower than 1.2 x 10(14) W/cm(2). Y1 - 2017 U6 - https://doi.org/10.1038/s41598-017-00124-9 SN - 2045-2322 VL - 7 PB - Nature Publ. Group CY - London ER - TY - JOUR A1 - Wolf, Thomas J. A. A1 - Holzmeier, Fabian A1 - Wagner, Isabella A1 - Berrah, Nora A1 - Bostedt, Christoph A1 - Bozek, John A1 - Bucksbaum, Phil A1 - Coffee, Ryan A1 - Cryan, James A1 - Farrell, Joe A1 - Feifel, Raimund A1 - Martinez, Todd J. A1 - McFarland, Brian A1 - Mucke, Melanie A1 - Nandi, Saikat A1 - Tarantelli, Francesco A1 - Fischer, Ingo A1 - Gühr, Markus T1 - Observing Femtosecond Fragmentation Using Ultrafast X-ray-Induced Auger Spectra JF - Applied sciences N2 - Molecules often fragment after photoionization in the gas phase. Usually, this process can only be investigated spectroscopically as long as there exists electron correlation between the photofragments. Important parameters, like their kinetic energy after separation, cannot be investigated. We are reporting on a femtosecond time-resolved Auger electron spectroscopy study concerning the photofragmentation dynamics of thymine. We observe the appearance of clearly distinguishable signatures from thymines neutral photofragment isocyanic acid. Furthermore, we observe a time-dependent shift of its spectrum, which we can attribute to the influence of the charged fragment on the Auger electron. This allows us to map our time-dependent dataset onto the fragmentation coordinate. The time dependence of the shift supports efficient transformation of the excess energy gained from photoionization into kinetic energy of the fragments. Our method is broadly applicable to the investigation of photofragmentation processes. KW - ultrafast dynamics KW - Auger electron spectroscopy KW - photofragmentation KW - photochemistry Y1 - 2017 U6 - https://doi.org/10.3390/app7070681 SN - 2076-3417 VL - 7 IS - 7 PB - MDPI CY - Basel ER - TY - JOUR A1 - Xiong, Hui A1 - Fang, Li A1 - Osipov, Timur A1 - Kling, Nora G. A1 - Wolf, Thomas J. A. A1 - Sistrunk, Emily A1 - Obaid, Razib A1 - Gühr, Markus A1 - Berrah, Nora T1 - Fragmentation of endohedral fullerene Ho3N@C-80 in an intense femtosecond near-infrared laser field JF - Physical review : A, Atomic, molecular, and optical physics N2 - The fragmentation of gas phase endohedral fullerene, Ho3N@C-80, was investigated using femtosecond near-infrared laser pulses with an ion velocity map imaging spectrometer. We observed that Ho+ abundance associated with carbon cage opening dominates at an intensity of 1.1 x 10(14) W/cm(2). As the intensity increases, the Ho+ yield associated with multifragmentation of the carbon cage exceeds the prominence of Ho+ associated with the gentler carbon cage opening. Moreover, the power law dependence of Ho+ on laser intensity indicates that the transition of the most likely fragmentation mechanisms occurs around 2.0 x 10(14) W/cm(2). Y1 - 2018 U6 - https://doi.org/10.1103/PhysRevA.97.023419 SN - 2469-9926 SN - 2469-9934 VL - 97 IS - 2 PB - American Physical Society CY - College Park ER - TY - JOUR A1 - Wolf, T. J. A. A1 - Myhre, R. H. A1 - Cryan, J. P. A1 - Coriani, S. A1 - Squibb, R. J. A1 - Battistoni, A. A1 - Berrah, Nora A1 - Bostedt, Christoph A1 - Bucksbaum, Philip H. A1 - Coslovich, G. A1 - Feifel, R. A1 - Gaffney, K. J. A1 - Grilj, J. A1 - Martinez, T. J. A1 - Miyabe, S. A1 - Moeller, S. P. A1 - Mucke, M. A1 - Natan, A. A1 - Obaid, R. A1 - Osipov, T. A1 - Plekan, O. A1 - Wang, S. A1 - Koch, H. A1 - Guehr, Markus T1 - Probing ultrafast pi pi*/n pi* internal conversion in organic chromophores via K-edge resonant absorption JF - Nature Communications Y1 - 2017 U6 - https://doi.org/10.1038/s41467-017-00069-7 SN - 2041-1723 VL - 8 SP - 14317 EP - 14322 PB - Nature Publ. Group CY - London ER - TY - GEN A1 - Wolf, Thomas J. A. A1 - Holzmeier, Fabian A1 - Wagner, Isabella A1 - Berrah, Nora A1 - Bostedt, Christoph A1 - Bozek, John A1 - Bucksbaum, Philip H. A1 - Coffee, Ryan A1 - Cryan, James A1 - Farrell, Joe A1 - Feifel, Raimund A1 - Martinez, Todd J. A1 - McFarland, Brian A1 - Mucke, Melanie A1 - Nandi, Saikat A1 - Tarantelli, Francesco A1 - Fischer, Ingo A1 - Gühr, Markus T1 - Observing Femtosecond Fragmentation Using Ultrafast X-ray-Induced Auger Spectra N2 - Molecules often fragment after photoionization in the gas phase. Usually, this process can only be investigated spectroscopically as long as there exists electron correlation between the photofragments. Important parameters, like their kinetic energy after separation, cannot be investigated. We are reporting on a femtosecond time-resolved Auger electron spectroscopy study concerning the photofragmentation dynamics of thymine. We observe the appearance of clearly distinguishable signatures from thymine′s neutral photofragment isocyanic acid. Furthermore, we observe a time-dependent shift of its spectrum, which we can attribute to the influence of the charged fragment on the Auger electron. This allows us to map our time-dependent dataset onto the fragmentation coordinate. The time dependence of the shift supports efficient transformation of the excess energy gained from photoionization into kinetic energy of the fragments. Our method is broadly applicable to the investigation of photofragmentation processes. T3 - Zweitveröffentlichungen der Universität Potsdam : Mathematisch-Naturwissenschaftliche Reihe - 386 KW - Auger electron spectroscopy KW - photochemistry KW - photofragmentation KW - ultrafast dynamics Y1 - 2017 U6 - http://nbn-resolving.de/urn/resolver.pl?urn:nbn:de:kobv:517-opus4-402692 ER - TY - JOUR A1 - Wolf, Thomas J. A. A1 - Holzmeier, Fabian A1 - Wagner, Isabella A1 - Berrah, Nora A1 - Bostedt, Christoph A1 - Bozek, John A1 - Bucksbaum, Philip H. A1 - Coffee, Ryan A1 - Cryan, James A1 - Farrell, Joe A1 - Feifel, Raimund A1 - Martinez, Todd J. A1 - McFarland, Brian A1 - Mucke, Melanie A1 - Nandi, Saikat A1 - Tarantelli, Francesco A1 - Fischer, Ingo A1 - Gühr, Markus T1 - Observing Femtosecond Fragmentation Using Ultrafast X-ray-Induced Auger Spectra JF - Applied Sciences N2 - Molecules often fragment after photoionization in the gas phase. Usually, this process can only be investigated spectroscopically as long as there exists electron correlation between the photofragments. Important parameters, like their kinetic energy after separation, cannot be investigated. We are reporting on a femtosecond time-resolved Auger electron spectroscopy study concerning the photofragmentation dynamics of thymine. We observe the appearance of clearly distinguishable signatures from thymine′s neutral photofragment isocyanic acid. Furthermore, we observe a time-dependent shift of its spectrum, which we can attribute to the influence of the charged fragment on the Auger electron. This allows us to map our time-dependent dataset onto the fragmentation coordinate. The time dependence of the shift supports efficient transformation of the excess energy gained from photoionization into kinetic energy of the fragments. Our method is broadly applicable to the investigation of photofragmentation processes. KW - ultrafast dynamics KW - Auger electron spectroscopy KW - photofragmentation KW - photochemistry Y1 - 2017 U6 - https://doi.org/10.3390/app7070681 SN - 2076-3417 VL - 7 IS - 7 PB - MDPI CY - Basel ER -