@article{YoungUedaGuehretal.2018,
  author    = {Young, Linda and Ueda, Kiyoshi and G{\"u}hr, Markus and Bucksbaum, Philip H. and Simon, Marc and Mukamel, Shaul and Rohringer, Nina and Prince, Kevin C. and Masciovecchio, Claudio and Meyer, Michael and Rudenko, Artem and Rolles, Daniel and Bostedt, Christoph and Fuchs, Matthias and Reis, David A. and Santra, Robin and Kapteyn, Henry and Murnane, Margaret and Ibrahim, Heide and Legare, Francois and Vrakking, Marc and Isinger, Marcus and Kroon, David and Gisselbrecht, Mathieu and W{\"o}rner, Hans Jakob and Leone, Stephen R.},
  title     = {Roadmap of ultrafast x-ray atomic and molecular physics},
  series = {Journal of physics : B, Atomic, molecular and optical physics},
  volume    = {51},
  journal   = {Journal of physics : B, Atomic, molecular and optical physics},
  number    = {3},
  publisher = {IOP Publ. Ltd.},
  address   = {Bristol},
  issn      = {0953-4075},
  doi       = {10.1088/1361-6455/aa9735},
  pages     = {45},
  year      = {2018},
  abstract  = {X-ray free-electron lasers (XFELs) and table-top sources of x-rays based upon high harmonic generation (HHG) have revolutionized the field of ultrafast x-ray atomic and molecular physics, largely due to an explosive growth in capabilities in the past decade. XFELs now provide unprecedented intensity (10(20) W cm(-2)) of x-rays at wavelengths down to similar to 1 Angstrom, and HHG provides unprecedented time resolution (similar to 50 attoseconds) and a correspondingly large coherent bandwidth at longer wavelengths. For context, timescales can be referenced to the Bohr orbital period in hydrogen atom of 150 attoseconds and the hydrogen-molecule vibrational period of 8 femtoseconds; wavelength scales can be referenced to the chemically significant carbon K-edge at a photon energy of similar to 280 eV (44 Angstroms) and the bond length in methane of similar to 1 Angstrom. With these modern x-ray sources one now has the ability to focus on individual atoms, even when embedded in a complex molecule, and view electronic and nuclear motion on their intrinsic scales (attoseconds and Angstroms). These sources have enabled coherent diffractive imaging, where one can image non-crystalline objects in three dimensions on ultrafast timescales, potentially with atomic resolution. The unprecedented intensity available with XFELs has opened new fields of multiphoton and nonlinear x-ray physics where behavior of matter under extreme conditions can be explored. The unprecedented time resolution and pulse synchronization provided by HHG sources has kindled fundamental investigations of time delays in photoionization, charge migration in molecules, and dynamics near conical intersections that are foundational to AMO physics and chemistry. This roadmap coincides with the year when three new XFEL facilities, operating at Angstrom wavelengths, opened for users (European XFEL, Swiss-FEL and PAL-FEL in Korea) almost doubling the present worldwide number of XFELs, and documents the remarkable progress in HHG capabilities since its discovery roughly 30 years ago, showcasing experiments in AMO physics and other applications. Here we capture the perspectives of 17 leading groups and organize the contributions into four categories: ultrafast molecular dynamics, multidimensional x-ray spectroscopies; high-intensity x-ray phenomena; attosecond x-ray science.},
  language  = {en}
}
@article{YangZhuWolfetal.2018,
  author    = {Yang, Jie and Zhu, Xiaolei and Wolf, Thomas J. A. and Li, Zheng and Nunes, Jo{\~a}o Pedro Figueira and Coffee, Ryan and Cryan, James P. and G{\"u}hr, Markus and Hegazy, Kareem and Heinz, Tony F. and Jobe, Keith and Li, Renkai and Shen, Xiaozhe and Veccione, Theodore and Weathersby, Stephen and Wilkin, Kyle J. and Yoneda, Charles and Zheng, Qiang and Martinez, Todd J. and Centurion, Martin and Wang, Xijie},
  title     = {Imaging CF3I conical intersection and photodissociation dynamics with ultrafast electron diffraction},
  series = {Science},
  volume    = {361},
  journal   = {Science},
  number    = {6397},
  publisher = {American Assoc. for the Advancement of Science},
  address   = {Washington},
  issn      = {0036-8075},
  doi       = {10.1126/science.aat0049},
  pages     = {64 -- 67},
  year      = {2018},
  abstract  = {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.},
  language  = {en}
}
@article{YangGuehrVecchioneetal.2016,
  author    = {Yang, Jie and G{\"u}hr, Markus and Vecchione, Theodore and Robinson, Matthew Scott and Li, Renkai and Hartmann, Nick and Shen, Xiaozhe and Coffee, Ryan and Corbett, Jeff and Fry, Alan and Gaffney, Kelly and Gorkhover, Tais and Hast, Carsten and Jobe, Keith and Makasyuk, Igor and Reid, Alexander and Robinson, Joseph and Vetter, Sharon and Wang, Fenglin and Weathersby, Stephen and Yoneda, Charles and Wang, Xijie and Centurion, Martin},
  title     = {Femtosecond gas phase electron diffraction with MeV electrons},
  series = {Faraday discussions},
  volume    = {194},
  journal   = {Faraday discussions},
  publisher = {Royal Society of Chemistry},
  address   = {Cambridge},
  issn      = {1359-6640},
  doi       = {10.1039/c6fd00071a},
  pages     = {563 -- 581},
  year      = {2016},
  abstract  = {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.},
  language  = {en}
}
@article{YangGuehrVecchioneetal.2016,
  author    = {Yang, Jie and G{\"u}hr, Markus and Vecchione, Theodore and Robinson, Matthew Scott and Li, Renkai and Hartmann, Nick and Shen, Xiaozhe and Coffee, Ryan and Corbett, Jeff and Fry, Alan and Gaffney, Kelly and Gorkhover, Tais and Hast, Carsten and Jobe, Keith and Makasyuk, Igor and Reid, Alexander and Robinson, Joseph and Vetter, Sharon and Wang, Fenglin and Weathersby, Stephen and Yoneda, Charles and Centurion, Martin and Wang, Xijie},
  title     = {Diffractive imaging of a rotational wavepacket in nitrogen molecules with femtosecond megaelectronvolt electron pulses},
  series = {Nature Communications},
  volume    = {7},
  journal   = {Nature Communications},
  publisher = {Nature Publ. Group},
  address   = {London},
  issn      = {2041-1723},
  doi       = {10.1038/ncomms11232},
  pages     = {9},
  year      = {2016},
  abstract  = {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.},
  language  = {en}
}
@article{XiongMignoletFangetal.2017,
  author    = {Xiong, Hui and Mignolet, Benoit and Fang, Li and Osipov, Timur and Wolf, Thomas J. A. and Sistrunk, Emily and G{\"u}hr, Markus and Remacle, Francoise and Berrah, Nora},
  title     = {The Role of Super-Atom Molecular Orbitals in Doped Fullerenes in a Femtosecond Intense Laser Field},
  series = {Scientific reports},
  volume    = {7},
  journal   = {Scientific reports},
  publisher = {Nature Publ. Group},
  address   = {London},
  issn      = {2045-2322},
  doi       = {10.1038/s41598-017-00124-9},
  pages     = {8},
  year      = {2017},
  abstract  = {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).},
  language  = {en}
}
@article{XiongFangOsipovetal.2018,
  author    = {Xiong, Hui and Fang, Li and Osipov, Timur and Kling, Nora G. and Wolf, Thomas J. A. and Sistrunk, Emily and Obaid, Razib and G{\"u}hr, Markus and Berrah, Nora},
  title     = {Fragmentation of endohedral fullerene Ho3N@C-80 in an intense femtosecond near-infrared laser field},
  series = {Physical review : A, Atomic, molecular, and optical physics},
  volume    = {97},
  journal   = {Physical review : A, Atomic, molecular, and optical physics},
  number    = {2},
  publisher = {American Physical Society},
  address   = {College Park},
  issn      = {2469-9926},
  doi       = {10.1103/PhysRevA.97.023419},
  pages     = {7},
  year      = {2018},
  abstract  = {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).},
  language  = {en}
}
@article{WolfSanchezYangetal.2019,
  author    = {Wolf, Thomas J. A. and Sanchez, David M. and Yang, J. and Parrish, R. M. and Nunes, J. P. F. and Centurion, M. and Coffee, R. and Cryan, J. P. and G{\"u}hr, Markus and Hegazy, Kareem and Kirrander, Adam and Li, R. K. and Ruddock, J. and Shen, Xiaozhe and Vecchione, T. and Weathersby, S. P. and Weber, Peter M. and Wilkin, K. and Yong, Haiwang and Zheng, Q. and Wang, X. J. and Minitti, Michael P. and Martinez, Todd J.},
  title     = {The photochemical ring-opening of 1,3-cyclohexadiene imaged by ultrafast electron diffraction},
  series = {Nature chemistry},
  volume    = {11},
  journal   = {Nature chemistry},
  number    = {6},
  publisher = {Nature Publ. Group},
  address   = {London},
  issn      = {1755-4330},
  doi       = {10.1038/s41557-019-0252-7},
  pages     = {504 -- 509},
  year      = {2019},
  abstract  = {The ultrafast photoinduced ring-opening of 1,3-cyclohexadiene constitutes a textbook example of electrocyclic reactions in organic chemistry and a model for photobiological reactions in vitamin D synthesis. Although the relaxation from the photoexcited electronic state during the ring-opening has been investigated in numerous studies, the accompanying changes in atomic distance have not been resolved. Here we present a direct and unambiguous observation of the ring-opening reaction path on the femtosecond timescale and subangstrom length scale using megaelectronvolt ultrafast electron diffraction. We followed the carbon-carbon bond dissociation and the structural opening of the 1,3-cyclohexadiene ring by the direct measurement of time-dependent changes in the distribution of interatomic distances. We observed a substantial acceleration of the ring-opening motion after internal conversion to the ground state due to a steepening of the electronic potential gradient towards the product minima. The ring-opening motion transforms into rotation of the terminal ethylene groups in the photoproduct 1,3,5-hexatriene on the subpicosecond timescale.},
  language  = {en}
}
@article{WolfParrishMyhreetal.2019,
  author    = {Wolf, Thomas J. A. and Parrish, Robert M. and Myhre, Rolf H. and Martinez, Todd J. and Koch, Henrik and G{\"u}hr, Markus},
  title     = {Observation of Ultrafast Intersystem Crossing in Thymine by Extreme Ultraviolet Time-Resolved Photoelectron Spectroscopy},
  series = {The journal of physical chemistry : A, Molecules, spectroscopy, kinetics, environment \& general theory},
  volume    = {123},
  journal   = {The journal of physical chemistry : A, Molecules, spectroscopy, kinetics, environment \& general theory},
  number    = {32},
  publisher = {American Chemical Society},
  address   = {Washington},
  issn      = {1089-5639},
  doi       = {10.1021/acs.jpca.9b05573},
  pages     = {6897 -- 6903},
  year      = {2019},
  abstract  = {We studied the photoinduced ultrafast relaxation dynamics of the nucleobase thymine using gas-phase time-resolved photoelectron spectroscopy. By employing extreme ultraviolet pulses from high harmonic generation for photoionization, we substantially extend our spectral observation window with respect to previous studies. This enables us to follow relaxation of the excited state population all the way to low-lying electronic states including the ground state. In thymine, we observe relaxation from the optically bright (1)pi pi* state of thymine to a dark (1)n pi* state within 80 +/- 30 fs. The (1)n pi* state relaxes further within 3.5 +/- 0.3 ps to a low-lying electronic state. By comparison with quantum chemical simulations, we can unambiguously assign its spectroscopic signature to the (3)pi pi* state. Hence, our study draws a comprehensive picture of the relaxation mechanism of thymine including ultrafast intersystem crossing to the triplet manifold.},
  language  = {en}
}
@article{WolfHolzmeierWagneretal.2017,
  author    = {Wolf, Thomas J. A. and Holzmeier, Fabian and Wagner, Isabella and Berrah, Nora and Bostedt, Christoph and Bozek, John and Bucksbaum, Philip H. and Coffee, Ryan and Cryan, James and Farrell, Joe and Feifel, Raimund and Martinez, Todd J. and McFarland, Brian and Mucke, Melanie and Nandi, Saikat and Tarantelli, Francesco and Fischer, Ingo and G{\"u}hr, Markus},
  title     = {Observing Femtosecond Fragmentation Using Ultrafast X-ray-Induced Auger Spectra},
  series = {Applied Sciences},
  volume    = {7},
  journal   = {Applied Sciences},
  number    = {7},
  publisher = {MDPI},
  address   = {Basel},
  issn      = {2076-3417},
  doi       = {10.3390/app7070681},
  year      = {2017},
  abstract  = {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.},
  language  = {en}
}
@article{WolfHolzmeierWagneretal.2017,
  author    = {Wolf, Thomas J. A. and Holzmeier, Fabian and Wagner, Isabella and Berrah, Nora and Bostedt, Christoph and Bozek, John and Bucksbaum, Phil and Coffee, Ryan and Cryan, James and Farrell, Joe and Feifel, Raimund and Martinez, Todd J. and McFarland, Brian and Mucke, Melanie and Nandi, Saikat and Tarantelli, Francesco and Fischer, Ingo and G{\"u}hr, Markus},
  title     = {Observing Femtosecond Fragmentation Using Ultrafast X-ray-Induced Auger Spectra},
  series = {Applied sciences},
  volume    = {7},
  journal   = {Applied sciences},
  number    = {7},
  publisher = {MDPI},
  address   = {Basel},
  issn      = {2076-3417},
  doi       = {10.3390/app7070681},
  pages     = {11},
  year      = {2017},
  abstract  = {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.},
  language  = {en}
}