TY - JOUR A1 - Yang, Jie A1 - Gühr, Markus A1 - Vecchione, Theodore A1 - Robinson, Matthew Scott A1 - Li, Renkai A1 - Hartmann, Nick A1 - Shen, Xiaozhe A1 - Coffee, Ryan A1 - Corbett, Jeff A1 - Fry, Alan A1 - Gaffney, Kelly A1 - Gorkhover, Tais A1 - Hast, Carsten A1 - Jobe, Keith A1 - Makasyuk, Igor A1 - Reid, Alexander A1 - Robinson, Joseph A1 - Vetter, Sharon A1 - Wang, Fenglin A1 - Weathersby, Stephen A1 - Yoneda, Charles A1 - Centurion, Martin A1 - Wang, Xijie T1 - Diffractive imaging of a rotational wavepacket in nitrogen molecules with femtosecond megaelectronvolt electron pulses JF - Nature Communications N2 - Imaging changes in molecular geometries on their natural femtosecond timescale with sub-Angstrom spatial precision is one of the critical challenges in the chemical sciences, as the nuclear geometry changes determine the molecular reactivity. For photoexcited molecules, the nuclear dynamics determine the photoenergy conversion path and efficiency. Here we report a gas-phase electron diffraction experiment using megaelectronvolt (MeV) electrons, where we captured the rotational wavepacket dynamics of nonadiabatically laser-aligned nitrogen molecules. We achieved a combination of 100 fs root-mean-squared temporal resolution and sub-Angstrom (0.76 angstrom) spatial resolution that makes it possible to resolve the position of the nuclei within the molecule. In addition, the diffraction patterns reveal the angular distribution of the molecules, which changes from prolate (aligned) to oblate (anti-aligned) in 300 fs. Our results demonstrate a significant and promising step towards making atomically resolved movies of molecular reactions. Y1 - 2016 U6 - https://doi.org/10.1038/ncomms11232 SN - 2041-1723 VL - 7 PB - Nature Publ. Group CY - London ER - TY - GEN A1 - Yang, Jie A1 - Guehr, Markus A1 - Vecchione, Theodore A1 - Robinson, Matthew Scott A1 - Li, Renkai A1 - Hartmann, Nick A1 - Shen, Xiaozhe A1 - Coffee, Ryan A1 - Corbett, Jeff A1 - Fry, Alan A1 - Gaffney, Kelly A1 - Gorkhover, Tais A1 - Hast, Carsten A1 - Jobe, Keith A1 - Makasyuk, Igor A1 - Reid, Alexander A1 - Robinson, Joseph A1 - Vetter, Sharon A1 - Wang, Fenglin A1 - Weathersby, Stephen A1 - Yoneda, Charles A1 - Wang, Xijie A1 - Centurion, Martin T1 - Femtosecond gas phase electron diffraction with MeV electrons N2 - We present results on ultrafast gas electron diffraction (UGED) experiments with femtosecond resolution using the MeV electron gun at SLAC National Accelerator Laboratory. UGED is a promising method to investigate molecular dynamics in the gas phase because electron pulses can probe the structure with a high spatial resolution. Until recently, however, it was not possible for UGED to reach the relevant timescale for the motion of the nuclei during a molecular reaction. Using MeV electron pulses has allowed us to overcome the main challenges in reaching femtosecond resolution, namely delivering short electron pulses on a gas target, overcoming the effect of velocity mismatch between pump laser pulses and the probe electron pulses, and maintaining a low timing jitter. At electron kinetic energies above 3 MeV, the velocity mismatch between laser and electron pulses becomes negligible. The relativistic electrons are also less susceptible to temporal broadening due to the Coulomb force. One of the challenges of diffraction with relativistic electrons is that the small de Broglie wavelength results in very small diffraction angles. In this paper we describe the new setup and its characterization, including capturing static diffraction patterns of molecules in the gas phase, finding time-zero with sub-picosecond accuracy and first time-resolved diffraction experiments. The new device can achieve a temporal resolution of 100 fs root-mean-square, and sub-angstrom spatial resolution. The collimation of the beam is sufficient to measure the diffraction pattern, and the transverse coherence is on the order of 2 nm. Currently, the temporal resolution is limited both by the pulse duration of the electron pulse on target and by the timing jitter, while the spatial resolution is limited by the average electron beam current and the signal-to-noise ratio of the detection system. We also discuss plans for improving both the temporal resolution and the spatial resolution. T3 - Zweitveröffentlichungen der Universität Potsdam : Mathematisch-Naturwissenschaftliche Reihe - 326 Y1 - 2016 U6 - http://nbn-resolving.de/urn/resolver.pl?urn:nbn:de:kobv:517-opus4-394989 ER - TY - JOUR A1 - Yang, Jie A1 - Gühr, Markus A1 - Vecchione, Theodore A1 - Robinson, Matthew Scott A1 - Li, Renkai A1 - Hartmann, Nick A1 - Shen, Xiaozhe A1 - Coffee, Ryan A1 - Corbett, Jeff A1 - Fry, Alan A1 - Gaffney, Kelly A1 - Gorkhover, Tais A1 - Hast, Carsten A1 - Jobe, Keith A1 - Makasyuk, Igor A1 - Reid, Alexander A1 - Robinson, Joseph A1 - Vetter, Sharon A1 - Wang, Fenglin A1 - Weathersby, Stephen A1 - Yoneda, Charles A1 - Wang, Xijie A1 - Centurion, Martin T1 - Femtosecond gas phase electron diffraction with MeV electrons JF - Faraday discussions N2 - We present results on ultrafast gas electron diffraction (UGED) experiments with femtosecond resolution using the MeV electron gun at SLAC National Accelerator Laboratory. UGED is a promising method to investigate molecular dynamics in the gas phase because electron pulses can probe the structure with a high spatial resolution. Until recently, however, it was not possible for UGED to reach the relevant timescale for the motion of the nuclei during a molecular reaction. Using MeV electron pulses has allowed us to overcome the main challenges in reaching femtosecond resolution, namely delivering short electron pulses on a gas target, overcoming the effect of velocity mismatch between pump laser pulses and the probe electron pulses, and maintaining a low timing jitter. At electron kinetic energies above 3 MeV, the velocity mismatch between laser and electron pulses becomes negligible. The relativistic electrons are also less susceptible to temporal broadening due to the Coulomb force. One of the challenges of diffraction with relativistic electrons is that the small de Broglie wavelength results in very small diffraction angles. In this paper we describe the new setup and its characterization, including capturing static diffraction patterns of molecules in the gas phase, finding time-zero with sub-picosecond accuracy and first time-resolved diffraction experiments. The new device can achieve a temporal resolution of 100 fs root-mean-square, and sub-angstrom spatial resolution. The collimation of the beam is sufficient to measure the diffraction pattern, and the transverse coherence is on the order of 2 nm. Currently, the temporal resolution is limited both by the pulse duration of the electron pulse on target and by the timing jitter, while the spatial resolution is limited by the average electron beam current and the signal-to-noise ratio of the detection system. We also discuss plans for improving both the temporal resolution and the spatial resolution. Y1 - 2016 U6 - https://doi.org/10.1039/c6fd00071a SN - 1359-6640 SN - 1364-5498 VL - 194 SP - 563 EP - 581 PB - Royal Society of Chemistry CY - Cambridge ER - TY - JOUR A1 - Yang, Jie A1 - Guehr, Markus A1 - Shen, Xiaozhe A1 - Li, Renkai A1 - Vecchione, Theodore A1 - Coffee, Ryan A1 - Corbett, Jeff A1 - Fry, Alan A1 - Hartmann, Nick A1 - Hast, Carsten A1 - Hegazy, Kareem A1 - Jobe, Keith A1 - Makasyuk, Igor A1 - Robinson, Joseph A1 - Robinson, Matthew Scott A1 - Vetter, Sharon A1 - Weathersby, Stephen A1 - Yoneda, Charles A1 - Wang, Xijie A1 - Centurion, Martin T1 - Diffractive Imaging of Coherent Nuclear Motion in Isolated Molecules JF - Physical review letters N2 - Observing the motion of the nuclear wave packets during a molecular reaction, in both space and time, is crucial for understanding and controlling the outcome of photoinduced chemical reactions. We have imaged the motion of a vibrational wave packet in isolated iodine molecules using ultrafast electron diffraction with relativistic electrons. The time-varying interatomic distance was measured with a precision 0.07 angstrom and temporal resolution of 230 fs full width at half maximum. The method is not only sensitive to the position but also the shape of the nuclear wave packet. Y1 - 2016 U6 - https://doi.org/10.1103/PhysRevLett.117.153002 SN - 0031-9007 SN - 1079-7114 VL - 117 PB - American Physical Society CY - College Park ER - TY - JOUR A1 - Tiegs, Scott D. A1 - Costello, David M. A1 - Isken, Mark W. A1 - Woodward, Guy A1 - McIntyre, Peter B. A1 - Gessner, Mark O. A1 - Chauvet, Eric A1 - Griffiths, Natalie A. A1 - Flecker, Alex S. A1 - Acuna, Vicenc A1 - Albarino, Ricardo A1 - Allen, Daniel C. A1 - Alonso, Cecilia A1 - Andino, Patricio A1 - Arango, Clay A1 - Aroviita, Jukka A1 - Barbosa, Marcus V. M. A1 - Barmuta, Leon A. A1 - Baxter, Colden V. A1 - Bell, Thomas D. C. A1 - Bellinger, Brent A1 - Boyero, Luz A1 - Brown, Lee E. A1 - Bruder, Andreas A1 - Bruesewitz, Denise A. A1 - Burdon, Francis J. A1 - Callisto, Marcos A1 - Canhoto, Cristina A1 - Capps, Krista A. A1 - Castillo, Maria M. A1 - Clapcott, Joanne A1 - Colas, Fanny A1 - Colon-Gaud, Checo A1 - Cornut, Julien A1 - Crespo-Perez, Veronica A1 - Cross, Wyatt F. A1 - Culp, Joseph M. A1 - Danger, Michael A1 - Dangles, Olivier A1 - de Eyto, Elvira A1 - Derry, Alison M. A1 - Diaz Villanueva, Veronica A1 - Douglas, Michael M. A1 - Elosegi, Arturo A1 - Encalada, Andrea C. A1 - Entrekin, Sally A1 - Espinosa, Rodrigo A1 - Ethaiya, Diana A1 - Ferreira, Veronica A1 - Ferriol, Carmen A1 - Flanagan, Kyla M. A1 - Fleituch, Tadeusz A1 - Shah, Jennifer J. Follstad A1 - Frainer, Andre A1 - Friberg, Nikolai A1 - Frost, Paul C. A1 - Garcia, Erica A. A1 - Lago, Liliana Garcia A1 - Garcia Soto, Pavel Ernesto A1 - Ghate, Sudeep A1 - Giling, Darren P. A1 - Gilmer, Alan A1 - Goncalves, Jose Francisco A1 - Gonzales, Rosario Karina A1 - Graca, Manuel A. S. A1 - Grace, Mike A1 - Grossart, Hans-Peter A1 - Guerold, Francois A1 - Gulis, Vlad A1 - Hepp, Luiz U. A1 - Higgins, Scott A1 - Hishi, Takuo A1 - Huddart, Joseph A1 - Hudson, John A1 - Imberger, Samantha A1 - Iniguez-Armijos, Carlos A1 - Iwata, Tomoya A1 - Janetski, David J. A1 - Jennings, Eleanor A1 - Kirkwood, Andrea E. A1 - Koning, Aaron A. A1 - Kosten, Sarian A1 - Kuehn, Kevin A. A1 - Laudon, Hjalmar A1 - Leavitt, Peter R. A1 - Lemes da Silva, Aurea L. A1 - Leroux, Shawn J. A1 - Leroy, Carri J. A1 - Lisi, Peter J. A1 - MacKenzie, Richard A1 - Marcarelli, Amy M. A1 - Masese, Frank O. A1 - Mckie, Brendan G. A1 - Oliveira Medeiros, Adriana A1 - Meissner, Kristian A1 - Milisa, Marko A1 - Mishra, Shailendra A1 - Miyake, Yo A1 - Moerke, Ashley A1 - Mombrikotb, Shorok A1 - Mooney, Rob A1 - Moulton, Tim A1 - Muotka, Timo A1 - Negishi, Junjiro N. A1 - Neres-Lima, Vinicius A1 - Nieminen, Mika L. A1 - Nimptsch, Jorge A1 - Ondruch, Jakub A1 - Paavola, Riku A1 - Pardo, Isabel A1 - Patrick, Christopher J. A1 - Peeters, Edwin T. H. M. A1 - Pozo, Jesus A1 - Pringle, Catherine A1 - Prussian, Aaron A1 - Quenta, Estefania A1 - Quesada, Antonio A1 - Reid, Brian A1 - Richardson, John S. A1 - Rigosi, Anna A1 - Rincon, Jose A1 - Risnoveanu, Geta A1 - Robinson, Christopher T. A1 - Rodriguez-Gallego, Lorena A1 - Royer, Todd V. A1 - Rusak, James A. A1 - Santamans, Anna C. A1 - Selmeczy, Geza B. A1 - Simiyu, Gelas A1 - Skuja, Agnija A1 - Smykla, Jerzy A1 - Sridhar, Kandikere R. A1 - Sponseller, Ryan A1 - Stoler, Aaron A1 - Swan, Christopher M. A1 - Szlag, David A1 - Teixeira-de Mello, Franco A1 - Tonkin, Jonathan D. A1 - Uusheimo, Sari A1 - Veach, Allison M. A1 - Vilbaste, Sirje A1 - Vought, Lena B. M. A1 - Wang, Chiao-Ping A1 - Webster, Jackson R. A1 - Wilson, Paul B. A1 - Woelfl, Stefan A1 - Xenopoulos, Marguerite A. A1 - Yates, Adam G. A1 - Yoshimura, Chihiro A1 - Yule, Catherine M. A1 - Zhang, Yixin X. A1 - Zwart, Jacob A. T1 - Global patterns and drivers of ecosystem functioning in rivers and riparian zones JF - Science Advances N2 - River ecosystems receive and process vast quantities of terrestrial organic carbon, the fate of which depends strongly on microbial activity. Variation in and controls of processing rates, however, are poorly characterized at the global scale. In response, we used a peer-sourced research network and a highly standardized carbon processing assay to conduct a global-scale field experiment in greater than 1000 river and riparian sites. We found that Earth’s biomes have distinct carbon processing signatures. Slow processing is evident across latitudes, whereas rapid rates are restricted to lower latitudes. Both the mean rate and variability decline with latitude, suggesting temperature constraints toward the poles and greater roles for other environmental drivers (e.g., nutrient loading) toward the equator. These results and data set the stage for unprecedented “next-generation biomonitoring” by establishing baselines to help quantify environmental impacts to the functioning of ecosystems at a global scale. Y1 - 2019 U6 - https://doi.org/10.1126/sciadv.aav0486 SN - 2375-2548 VL - 5 IS - 1 PB - American Assoc. for the Advancement of Science CY - Washington ER -