TY - JOUR A1 - Yang, Jie A1 - Zhu, Xiaolei A1 - Wolf, Thomas J. A. A1 - Li, Zheng A1 - Nunes, João Pedro Figueira A1 - Coffee, Ryan A1 - Cryan, James P. A1 - Gühr, Markus A1 - Hegazy, Kareem A1 - Heinz, Tony F. A1 - Jobe, Keith A1 - Li, Renkai A1 - Shen, Xiaozhe A1 - Veccione, Theodore A1 - Weathersby, Stephen A1 - Wilkin, Kyle J. A1 - Yoneda, Charles A1 - Zheng, Qiang A1 - Martinez, Todd J. A1 - Centurion, Martin A1 - Wang, Xijie T1 - Imaging CF3I conical intersection and photodissociation dynamics with ultrafast electron diffraction JF - Science N2 - Conical intersections play a critical role in excited-state dynamics of polyatomic molecules because they govern the reaction pathways of many nonadiabatic processes. However, ultrafast probes have lacked sufficient spatial resolution to image wave-packet trajectories through these intersections directly. Here, we present the simultaneous experimental characterization of one-photon and two-photon excitation channels in isolated CF3I molecules using ultrafast gas-phase electron diffraction. In the two-photon channel, we have mapped out the real-space trajectories of a coherent nuclear wave packet, which bifurcates onto two potential energy surfaces when passing through a conical intersection. In the one-photon channel, we have resolved excitation of both the umbrella and the breathing vibrational modes in the CF3 fragment in multiple nuclear dimensions. These findings benchmark and validate ab initio nonadiabatic dynamics calculations. Y1 - 2018 U6 - https://doi.org/10.1126/science.aat0049 SN - 0036-8075 SN - 1095-9203 VL - 361 IS - 6397 SP - 64 EP - 67 PB - American Assoc. for the Advancement of Science CY - Washington ER - TY - JOUR A1 - Wilkin, Kyle J. A1 - Parrish, Robert M. A1 - Yang, Jie A1 - Wolf, Thomas J. A. A1 - Nunes, J. Pedro F. A1 - Gühr, Markus A1 - Li, Renkai A1 - Shen, Xiaozhe A1 - Zheng, Qiang A1 - Wang, Xijie A1 - Martinez, Todd J. A1 - Centurion, Martin T1 - Diffractive imaging of dissociation and ground-state dynamics in a complex molecule JF - Physical review : A, Atomic, molecular, and optical physics N2 - We have investigated the structural dynamics in photoexcited 1,2-diiodotetrafluoroethane molecules (C2F4I2) in the gas phase experimentally using ultrafast electron diffraction and theoretically using FOMO-CASCI excited-state dynamics simulations. The molecules are excited by an ultraviolet femtosecond laser pulse to a state characterized by a transition from the iodine 5p perpendicular to orbital to a mixed 5p parallel to sigma hole and CF2 center dot antibonding orbital, which results in the cleavage of one of the carbon-iodine bonds. We have observed, with sub-Angstrom resolution, the motion of the nuclear wave packet of the dissociating iodine atom followed by coherent vibrations in the electronic ground state of the C2F4I radical. The radical reaches a stable classical (nonbridged) structure in less than 200 fs. Y1 - 2019 U6 - https://doi.org/10.1103/PhysRevA.100.023402 SN - 2469-9926 SN - 2469-9934 VL - 100 IS - 2 PB - American Physical Society CY - College Park 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 - 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 - 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 - 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 - Bonifacio, P. A1 - Rahmani, H. A1 - Whitmore, J. B. A1 - Wendt, Martin A1 - Centurion, Martin A1 - Molaro, P. A1 - Srianand, R. A1 - Murphy, M. T. A1 - Petitjean, P. A1 - Agafonova, I. I. A1 - Evans, T. M. A1 - Levshakov, S. A. A1 - Lopez, S. A1 - Martins, C. J. A. P. A1 - Reimers, D. A1 - Vladilo, G. T1 - Fundamental constants and high-resolution spectroscopy JF - Astronomische Nachrichten = Astronomical notes KW - atomic processes KW - cosmology: observations KW - elementary particles KW - line: formation KW - quasars: absorption lines KW - techniques: spectroscopic Y1 - 2014 U6 - https://doi.org/10.1002/asna.201312005 SN - 0004-6337 SN - 1521-3994 VL - 335 IS - 1 SP - 83 EP - 91 PB - Wiley-VCH CY - Weinheim ER - TY - JOUR A1 - Evans, T. M. A1 - Murphy, M. T. A1 - Whitmore, J. B. A1 - Misawa, T. A1 - Centurion, Martin A1 - Lopez, S. A1 - Martins, C. J. A. P. A1 - Molaro, P. A1 - Petitjean, P. A1 - Rahmani, H. A1 - Srianand, R. A1 - Wendt, Martin T1 - The UVES Large Program for testing fundamental physics - III. Constraints on the fine-structure constant from three telescopes JF - Monthly notices of the Royal Astronomical Society KW - intergalactic medium KW - quasars: absorption lines KW - quasars: individual: HS 1549+1919 KW - cosmology: miscellaneous KW - cosmology: observations Y1 - 2014 U6 - https://doi.org/10.1093/mnras/stu1754 SN - 0035-8711 SN - 1365-2966 VL - 445 IS - 1 SP - 128 EP - 150 PB - Oxford Univ. Press CY - Oxford ER - TY - JOUR A1 - Molaro, P. A1 - Centurion, Martin A1 - Whitmore, J. B. A1 - Evans, T. M. A1 - Murphy, M. T. A1 - Agafonova, I. I. A1 - Bonifacio, P. A1 - D'Odorico, S. A1 - Levshakov, S. A. A1 - Lopez, S. A1 - Martins, C. J. A. P. A1 - Petitjean, P. A1 - Rahmani, H. A1 - Reimers, D. A1 - Srianand, R. A1 - Vladilo, G. A1 - Wendt, Martin T1 - The UVES Large Program for testing fundamental physics I. Bounds on a change in alpha towards quasar HE 221-2818 JF - Astronomy and astrophysics : an international weekly journal N2 - Context. Absorption-line systems detected in quasar spectra can be used to compare the value of the fine-structure constant, alpha, measured today on Earth with its value in distant galaxies. In recent years, some evidence has emerged of small temporal and also spatial variations in alpha on cosmological scales. These variations may reach a fractional level of approximate to 10 ppm (parts per million). Aims. To test these claims we are conducting a Large Program of observations with the Very Large Telescope's Ultraviolet and Visual Echelle Spectrograph (UVES), and are obtaining high-resolution (R approximate to 60 000) and high signal-to-noise ratio (S/N approximate to 100) UVES spectra calibrated specifically for this purpose. Here we analyse the first complete quasar spectrum from this programme, that of HE 2217-2818. Methods. We applied the many multiplet method to measure alpha in five absorption systems towards this quasar: z(abs) = 0.7866, 0.9424, 1.5558, 1.6279, and 1.6919. Results. The most precise result is obtained for the absorber at z(abs) = 1.6919 where 3 Fe II transitions and Al II lambda 1670 have high S/N and provide a wide range of sensitivities to alpha. The absorption profile is complex with several very narrow features, and it requires 32 velocity components to be fitted to the data. We also conducted a range of tests to estimate the systematic error budget. Our final result for the relative variation in alpha in this system is Delta alpha/alpha = +1.3 +/- 2.4(stat) +/- 1.0(sys) ppm. This is one of the tightest current bounds on alpha-variation from an individual absorber. A second, separate approach to the data reduction, calibration, and analysis of this system yielded a slightly different result of -3.8 +/- 2.1(stat) ppm, possibly suggesting a larger systematic error component than our tests indicated. This approach used an additional 3 Fe II transitions, parts of which were masked due to contamination by telluric features. Restricting this analysis to the Fe II transitions alone and using a modified absorption profile model gave a result that is consistent with the first approach, Delta alpha/alpha = +1.1 +/- 2.6(stat) ppm. The four other absorbers have simpler absorption profiles, with fewer and broader features, and offer transitions with a narrower range of sensitivities to alpha. They therefore provide looser bounds on Delta alpha/alpha at the greater than or similar to 10 ppm precision level. Conclusions. The absorbers towards quasar HE 2217-2818 reveal no evidence of any variation in alpha at the 3-ppm precision level (1 sigma confidence). If the recently reported 10-ppm dipolar variation in alpha across the sky is correct, the expectation at this sky position is (3.2-5.4) +/- 1.7 ppm depending on dipole model used. Our constraint of Delta alpha/alpha = +1.3 +/- 2.4(stat) +/- 1.0(sys) ppm is not inconsistent with this expectation. KW - quasars: absorption lines KW - quasars: individual: HE 2217-2818 KW - intergalactic medium KW - cosmology: miscellaneous cosmology KW - observations Y1 - 2013 U6 - https://doi.org/10.1051/0004-6361/201321351 SN - 0004-6361 VL - 555 IS - 4 PB - EDP Sciences CY - Les Ulis ER - TY - JOUR A1 - Rahmani, H. A1 - Wendt, Martin A1 - Srianand, R. A1 - Noterdaeme, P. A1 - Petitjean, P. A1 - Molaro, P. A1 - Whitmore, J. B. A1 - Murphy, M. T. A1 - Centurion, Martin A1 - Fathivavsari, H. A1 - D'Odorico, S. A1 - Evans, T. M. A1 - Levshakov, S. A. A1 - Lopez, S. A1 - Martins, C. J. A. P. A1 - Reimers, D. A1 - Vladilo, G. T1 - The UVES large program for testing fundamental physics - II. Constraints on a change in mu towards quasar HE 0027-1836 JF - Monthly notices of the Royal Astronomical Society N2 - We present an accurate analysis of the H-2 absorption lines from the z(abs) similar to 2.4018 damped Ly alpha system towards HE 0027-1836 observed with the Very Large Telescope Ultraviolet and Visual Echelle Spectrograph (VLT/UVES) as a part of the European Southern Observatory Large Programme 'The UVES large programme for testing fundamental physics' to constrain the variation of proton-to-electron mass ratio, mu m(p)/m(e). We perform cross-correlation analysis between 19 individual exposures taken over three years and the combined spectrum to check the wavelength calibration stability. We notice the presence of a possible wavelength-dependent velocity drift especially in the data taken in 2012. We use available asteroids spectra taken with UVES close to our observations to confirm and quantify this effect. We consider single-and two-component Voigt profiles to model the observed H-2 absorption profiles. We use both linear regression analysis and Voigt profile fitting where Delta mu/mu is explicitly considered as an additional fitting parameter. The two-component model is marginally favoured by the statistical indicators and we get Delta mu/mu = -2.5 +/- 8.1(stat) +/- 6.2(sys) ppm. When we apply the correction to the wavelength-dependent velocity drift, we find Delta mu/mu = -7.6 +/- 8.1(stat) +/- 6.3(sys) ppm. It will be important to check the extent to which the velocity drift we notice in this study is present in UVES data used for previous Delta mu/mu measurements. KW - intergalactic medium KW - quasars: absorption lines KW - quasars: individual: HE 0027-1836 Y1 - 2013 U6 - https://doi.org/10.1093/mnras/stt1356 SN - 0035-8711 SN - 1365-2966 VL - 435 IS - 1 SP - 861 EP - 878 PB - Oxford Univ. Press CY - Oxford ER -