TY - JOUR A1 - Kunnus, Kristjan A1 - Josefsson, I. A1 - Rajkovic, Ivan A1 - Schreck, Simon A1 - Quevedo, Wilson A1 - Beye, Martin A1 - Weniger, C. A1 - Gruebel, S. A1 - Scholz, M. A1 - Nordlund, D. A1 - Zhang, W. A1 - Hartsock, R. W. A1 - Gaffney, K. J. A1 - Schlotter, W. F. A1 - Turner, J. J. A1 - Kennedy, B. A1 - Hennies, F. A1 - de Groot, F. M. F. A1 - Techert, S. A1 - Odelius, Michael A1 - Wernet, Ph. A1 - Föhlisch, Alexander T1 - Identification of the dominant photochemical pathways and mechanistic insights to the ultrafast ligand exchange of Fe(CO)(5) to Fe(CO)(4)EtOH JF - Structural dynamics N2 - We utilized femtosecond time-resolved resonant inelastic X-ray scattering and ab initio theory to study the transient electronic structure and the photoinduced molecular dynamics of a model metal carbonyl photocatalyst Fe(CO)(5) in ethanol solution. We propose mechanistic explanation for the parallel ultrafast intra-molecular spin crossover and ligation of the Fe(CO)(4) which are observed following a charge transfer photoexcitation of Fe(CO)(5) as reported in our previous study [ Wernet et al., Nature 520, 78 (2015)]. We find that branching of the reaction pathway likely happens in the (1)A(1) state of Fe(CO)(4). A sub-picosecond time constant of the spin crossover from B-1(2) to B-3(2) is rationalized by the proposed B-1(2) -> (1)A(1) -> B-3(2) mechanism. Ultrafast ligation of the B-1(2) Fe(CO)(4) state is significantly faster than the spin-forbidden and diffusion limited ligation process occurring from the B-3(2) Fe(CO)(4) ground state that has been observed in the previous studies. We propose that the ultrafast ligation occurs via B-1(2) -> (1)A(1) -> (1)A'Fe(CO)(4)EtOH pathway and the time scale of the (1)A(1) Fe(CO)(4) state ligation is governed by the solute-solvent collision frequency. Our study emphasizes the importance of understanding the interaction of molecular excited states with the surrounding environment to explain the relaxation pathways of photoexcited metal carbonyls in solution. (C) 2016 Author(s). Y1 - 2016 U6 - https://doi.org/10.1063/1.4941602 SN - 2329-7778 VL - 3 PB - American Institute of Physics CY - Washington ER - TY - JOUR A1 - Furniss, A. A1 - Noda, K. A1 - Boggs, S. A1 - Chiang, J. A1 - Christensen, F. A1 - Craig, W. A1 - Giommi, P. A1 - Hailey, C. A1 - Harisson, F. A1 - Madejski, G. A1 - Nalewajko, K. A1 - Perri, M. A1 - Stern, D. A1 - Urry, M. A1 - Verrecchia, F. A1 - Zhang, W. A1 - Ahnen, M. L. A1 - Ansoldi, S. A1 - Antonelli, L. A. A1 - Antoranz, P. A1 - Babic, A. A1 - Banerjee, B. A1 - Bangale, P. A1 - de Almeida, U. Barres A1 - Barrio, J. A. A1 - Becerra Gonzalez, J. A1 - Bednarek, W. A1 - Bernardini, E. A1 - Biasuzzi, B. A1 - Biland, A. A1 - Blanch Bigas, O. A1 - Bonnefoy, S. A1 - Bonnoli, G. A1 - Borracci, F. A1 - Bretz, T. A1 - Carmona, E. A1 - Carosi, A. A1 - Chatterjee, A. A1 - Clavero, R. A1 - Colin, P. A1 - Colombo, E. A1 - Contreras, J. L. A1 - Cortina, J. A1 - Covino, S. A1 - Da Vela, P. A1 - Dazzi, F. A1 - De Angelis, A. A1 - De Caneva, G. A1 - De Lotto, B. A1 - de Ona Wilhelmi, E. A1 - Delgado Mendez, C. A1 - Di Pierro, F. A1 - Prester, Dijana Dominis A1 - Dorner, D. A1 - Doro, M. A1 - Einecke, S. A1 - Eisenacher Glawion, D. A1 - Elsaesser, D. A1 - Fernandez-Barral, A. A1 - Fidalgo, D. A1 - Fonseca, M. V. A1 - Font, L. A1 - Frantzen, K. A1 - Fruck, C. A1 - Galindo, D. A1 - Garcia Lopez, R. J. A1 - Garczarczyk, M. A1 - Garrido Terrats, D. A1 - Gaug, M. A1 - Giammaria, P. A1 - Godinovic, N. A1 - Gonzalez Munoz, A. A1 - Guberman, D. A1 - Hanabata, Y. A1 - Hayashida, M. A1 - Herrera, J. A1 - Hose, J. A1 - Hrupec, D. A1 - Hughes, G. A1 - Idec, W. A1 - Kellermann, H. A1 - Kodani, K. A1 - Konno, Y. A1 - Kubo, H. A1 - Kushida, J. A1 - La Barbera, A. A1 - Lelas, D. A1 - Lewandowska, N. A1 - Lindfors, E. A1 - Lombardi, S. A1 - Longo, F. A1 - Lopez, M. A1 - Lopez-Coto, R. A1 - Lopez-Oramas, A. A1 - Lorenz, E. A1 - Majumdar, P. A1 - Makariev, M. A1 - Mallot, K. A1 - Maneva, G. A1 - Manganaro, M. A1 - Mannheim, K. A1 - Maraschi, L. A1 - Marcote, B. A1 - Mariotti, M. A1 - Martinez, M. A1 - Mazin, D. A1 - Menzel, U. A1 - Miranda, J. M. A1 - Mirzoyan, R. A1 - Moralejo, A. A1 - Nakajima, D. A1 - Neustroev, V. A1 - Niedzwiecki, A. A1 - Nievas Rosillo, M. A1 - Nilsson, K. A1 - Nishijima, K. A1 - Orito, R. A1 - Overkemping, A. A1 - Paiano, S. A1 - Palacio, J. A1 - Palatiello, M. A1 - Paneque, D. A1 - Paoletti, R. A1 - Paredes, J. M. A1 - Paredes-Fortuny, X. A1 - Persic, M. A1 - Poutanen, J. A1 - Moroni, P. G. Prada A1 - Prandini, E. A1 - Puljak, I. A1 - Reinthal, R. A1 - Rhode, W. A1 - Ribo, M. A1 - Rico, J. A1 - Garcia, J. Rodriguez A1 - Saito, T. A1 - Saito, K. A1 - Satalecka, K. A1 - Scapin, V. A1 - Schultz, C. A1 - Schweizer, T. A1 - Shore, S. N. A1 - Sillanpaa, A. A1 - Sitarek, J. A1 - Snidaric, I. A1 - Sobczynska, D. A1 - Stamerra, A. A1 - Steinbring, T. A1 - Strzys, M. A1 - Takalo, L. A1 - Takami, H. A1 - Tavecchio, F. A1 - Temnikov, P. A1 - Terzic, T. A1 - Tescaro, D. A1 - Teshima, M. A1 - Thaele, J. A1 - Torres, D. F. A1 - Toyama, T. A1 - Treves, A. A1 - Verguilov, V. A1 - Vovk, I. A1 - Will, M. A1 - Zanin, R. A1 - Archer, A. A1 - Benbow, W. A1 - Bird, R. A1 - Biteau, Jonathan A1 - Bugaev, V. A1 - Cardenzana, J. V. A1 - Cerruti, M. A1 - Chen, Xuhui A1 - Ciupik, L. A1 - Connolly, M. P. A1 - Cui, W. A1 - Dickinson, H. J. A1 - Dumm, J. A1 - Eisch, J. D. A1 - Falcone, A. A1 - Feng, Q. A1 - Finley, J. P. A1 - Fleischhack, H. A1 - Fortin, P. A1 - Fortson, L. A1 - Gerard, L. A1 - Gillanders, G. H. A1 - Griffin, S. A1 - Griffiths, S. T. A1 - Grube, J. A1 - Gyuk, G. A1 - Hakansson, Nils A1 - Holder, J. A1 - Humensky, T. B. A1 - Johnson, C. A. A1 - Kaaret, P. A1 - Kertzman, M. A1 - Kieda, D. A1 - Krause, M. A1 - Krennrich, F. A1 - Lang, M. J. A1 - Lin, T. T. Y. A1 - Maier, G. A1 - McArthur, S. A1 - McCann, A. A1 - Meagher, K. A1 - Moriarty, P. A1 - Mukherjee, R. A1 - Nieto, D. A1 - Ong, R. A. A1 - Park, N. A1 - Petry, D. A1 - Pohl, Martin A1 - Popkow, A. A1 - Ragan, K. A1 - Ratliff, G. A1 - Reyes, L. C. A1 - Reynolds, P. T. A1 - Richards, G. T. A1 - Roache, E. A1 - Santander, M. A1 - Sembroski, G. H. A1 - Shahinyan, K. A1 - Staszak, D. A1 - Telezhinsky, Igor O. A1 - Tucci, J. V. A1 - Tyler, J. A1 - Vassiliev, V. V. A1 - Wakely, S. P. A1 - Weiner, O. M. A1 - Weinstein, A. A1 - Wilhelm, Alina A1 - Williams, D. A. A1 - Zitzer, B. A1 - Vince, O. A1 - Fuhrmann, L. A1 - Angelakis, E. A1 - Karamanavis, V. A1 - Myserlis, I. A1 - Krichbaum, T. P. A1 - Zensus, J. A. A1 - Ungerechts, H. A1 - Sievers, A. A1 - Bachev, R. A1 - Boettcher, Markus A1 - Chen, W. P. A1 - Damljanovic, G. A1 - Eswaraiah, C. A1 - Guver, T. A1 - Hovatta, T. A1 - Hughes, Z. A1 - Ibryamov, S. I. A1 - Joner, M. D. A1 - Jordan, B. A1 - Jorstad, S. G. A1 - Joshi, M. A1 - Kataoka, J. A1 - Kurtanidze, O. M. A1 - Kurtanidze, S. O. A1 - Lahteenmaki, A. A1 - Latev, G. A1 - Lin, H. C. A1 - Larionov, V. M. A1 - Mokrushina, A. A. A1 - Morozova, D. A. A1 - Nikolashvili, M. G. A1 - Raiteri, C. M. A1 - Ramakrishnan, V. A1 - Readhead, A. C. R. A1 - Sadun, A. C. A1 - Sigua, L. A. A1 - Semkov, E. H. A1 - Strigachev, A. A1 - Tammi, J. A1 - Tornikoski, M. A1 - Troitskaya, Y. V. A1 - Troitsky, I. S. A1 - Villata, M. T1 - First NuSTAR observations of MRK 501 within a radio to TeV multi-instrument campaign JF - The astrophysical journal : an international review of spectroscopy and astronomical physics N2 - We report on simultaneous broadband observations of the TeV-emitting blazar Markarian 501 between 2013 April 1 and August 10, including the first detailed characterization of the synchrotron peak with Swift and NuSTAR. During the campaign, the nearby BL Lac object was observed in both a quiescent and an elevated state. The broadband campaign includes observations with NuSTAR, MAGIC, VERITAS, the Fermi Large Area Telescope, Swift X-ray Telescope and UV Optical Telescope, various ground-based optical instruments, including the GASP-WEBT program, as well as radio observations by OVRO, Metsahovi, and the F-Gamma consortium. Some of the MAGIC observations were affected by a sand layer from the Saharan desert, and had to be corrected using event-by-event corrections derived with a Light Detection and Ranging (LIDAR) facility. This is the first time that LIDAR information is used to produce a physics result with Cherenkov Telescope data taken during adverse atmospheric conditions, and hence sets a precedent for the current and future ground-based gamma-ray instruments. The NuSTAR instrument provides unprecedented sensitivity in hard X-rays, showing the source to display a spectral energy distribution (SED) between 3 and 79 keV consistent with a log-parabolic spectrum and hard X-ray variability on hour timescales. None (of the four extended NuSTAR observations) show evidence of the onset of inverse-Compton emission at hard X-ray energies. We apply a single-zone equilibrium synchrotron self-Compton (SSC) model to five simultaneous broadband SEDs. We find that the SSC model can reproduce the observed broadband states through a decrease in the magnetic field strength coinciding with an increase in the luminosity and hardness of the relativistic leptons responsible for the high-energy emission. KW - BL Lacertae objects: general KW - galaxies: individual (Markarian 501) KW - X-rays: galaxies Y1 - 2015 U6 - https://doi.org/10.1088/0004-637X/812/1/65 SN - 0004-637X SN - 1538-4357 VL - 812 IS - 1 PB - IOP Publ. Ltd. CY - Bristol ER -