Structural Determination of a Transient Isomer of<mml:math xmlns:mml="http://www.w3.org/1998/Math/MathML" display="inline"><mml:msub><mml:mi>CH</mml:mi><mml:mn>2</mml:mn></mml:msub><mml:msub><mml:mi mathvariant="normal">I</mml:mi><mml:mn>2</mml:mn></mml:msub></mml:math>by Picosecond X-Ray Diffraction

Davidsson, Jan; Poulsen, Jens Aage; Cammarata, Marco; Georgiou, Panayiotis G.; Wouts, R.; Katona, Gergely; Jacobson, Frida; Plech, Anton; Wulff, Michaël; Nyman, Gunnar; Neutze, Richard

doi:10.1103/physrevlett.94.245503

Cited by 95 publications

(108 citation statements)

References 29 publications

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“…The main limit of this spectroscopic approach is the possibility of missing intermediate species containing only linear carbonyls (which are buried under the GS signals) and the poor structural sensitivity. TR-XSS is therefore a perfect complement for ultrafast IR characterization since it contains the scattering signal contributions from all the reaction pathways (in proportion to their population and scattering function) and is highly sensitive to intermediate geometries [43,49,58,59,[61][62][63]65,70,[198][199][200].…”

Section: (C) the Solution-phase Photochemistry Of The Transition Metamentioning

confidence: 99%

Synchrotron ultrafast techniques for photoactive transition metal complexes

Borfecchia

Garino

Salassa

et al. 2013

Phil. Trans. R. Soc. A.

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In the last decade, the use of time-resolved X-ray techniques has revealed the structure of lightgenerated transient species for a wide range of samples, from small organic molecules to proteins. Time resolutions of the order of 100 ps are typically reached, allowing one to monitor thermally equilibrated excited states and capture their structure as a function of time. This review aims at providing a general overview of the application of timeresolved X-ray solution scattering (TR-XSS) and time-resolved X-ray absorption spectroscopy (TR-XAS), the two techniques prevalently employed in the investigation of light-triggered structural changes of transition metal complexes. In particular, we herein describe the fundamental physical principles for static XSS and XAS and illustrate the theory of timeresolved XSS and XAS together with data acquisition and analysis strategies. Selected pioneering examples of photoactive transition metal complexes studied by TR-XSS and TR-XAS are discussed in depth.

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Section: (C) the Solution-phase Photochemistry Of The Transition Metamentioning

confidence: 99%

Synchrotron ultrafast techniques for photoactive transition metal complexes

Borfecchia

Garino

Salassa

et al. 2013

Phil. Trans. R. Soc. A.

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“…The method has been applied to follow chemical reactions of small molecules (29)(30)(31) as well as structural dynamics of photoactive proteins (32-41).…”

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confidence: 99%

Ultrafast anisotropic protein quake propagation after CO photodissociation in myoglobin

Brinkmann

Hub

2016

Proc. Natl. Acad. Sci. U.S.A.

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"Protein quake" denotes the dissipation of excess energy across a protein, in response to a local perturbation such as the breaking of a chemical bond or the absorption of a photon. Femtosecond timeresolved small-and wide-angle X-ray scattering (TR-SWAXS) is capable of tracking such ultrafast protein dynamics. However, because the structural interpretation of the experiments is complicated, a molecular picture of protein quakes has remained elusive. In addition, new questions arose from recent TR-SWAXS data that were interpreted as underdamped oscillations of an entire protein, thus challenging the long-standing concept of overdamped global protein dynamics. Based on molecular-dynamics simulations, we present a detailed molecular movie of the protein quake after carbon monoxide (CO) photodissociation in myoglobin. The simulations suggest that the protein quake is characterized by a single pressure peak that propagates anisotropically within 500 fs across the protein and further into the solvent. By computing TR-SWAXS patterns from the simulations, we could interpret features in the reciprocalspace SWAXS signals as specific real-space dynamics, such as CO displacement and pressure wave propagation. Remarkably, we found that the small-angle data primarily detect modulations of the solvent density but not oscillations of the bare protein, thereby reconciling recent TR-SWAXS experiments with the notion of overdamped global protein dynamics.time-resolved SAXS/WAXS | free-electron laser | molecular dynamics F unctional protein dynamics occur on various timescales, ranging from tens of femtoseconds for bond breaking, up to milliseconds and seconds for large-scale conformational transitions or protein folding. Observing and explaining such transitions, if possible in a time-resolved manner, has remained a central goal of molecular biophysics. A popular model system used to study proteins dynamics has been the 18-kDa protein myoglobin (Mb), the protein of first known tertiary structure (1). Mb contains an iron-porphyrin heme group that reversibly binds small gas molecules such as molecular oxygen (O 2 ) or carbon monoxide (CO). Mb is abundant in the muscle tissue of vertebrates, where it plays an important role in the transport and storage of O 2 and in the biochemistry of nitric oxide (2, 3).Because the CO-iron bonds in a Mb ensemble can be coherently photolysed with a laser flash within only 50 fs (4), a range of time-resolved techniques has been applied to probe various aspects of the structural dynamics after CO photodissociation, such as energy dissipation, CO dynamics, or heme doming (5-15). Three-dimensional movies of Mb conformational transitions were derived by means of time-resolved crystallography, which recently reached subpicosecond time resolution (16-19). These experimental studies were complemented by several pioneering molecular-dynamics (MD) simulations that revealed the Mb dynamics with atomic detail, with some focus on heat dissipation, vibrational dynamics, as well as ligand migration (20-28).Time-re...

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“…The X-ray pulse with 3% energy bandwidth of the first harmonics of the undulator has been used for TRXL experiments in the beamline ID09B at ESRF (Cammarata et al, 2008;Cammarata et al, 2006;Christensen et al, 2009;Davidsson et al, 2005;Georgiou et al, 2006;Ichiyanagi et al, 2009;Ihee, 2009;Ihee et al, 2005a;Kim et al, 2006;Kong et al, 2008;Kong et al, 2007;Lee et al, 2008a;Lee et al, 2006;Lee et al, 2008b;Plech et al, 2004;Vincent et al, 2009;Wulff et al, 2006). For example, the structural dynamics of C 2 H 4 I 2 in methanol were studied at the ID09B beamline (Ihee et al, 2005a), and the reaction pathways and associated transient molecular structures in solution were resolved by the combination of theoretical calculations and global fitting analysis.…”

Section: Energy Bandwidth Of the Incident X-ray Beammentioning

confidence: 99%

“…On one hand, time-resolved X-ray diffraction enables us to access to the mechanism of structural transformations at the atomic level in crystalline state (Collet et al, 2003;Schotte et al, 2003;Srajer et al, 1996;Techert et al, 2001). On the other hand, timeresolved X-ray absorption fine structure (XAFS) (Chen et al, 2001;Saes et al, 2003;Sato et al, 2009) and time-resolved solution scattering (Davidsson et al, 2005;Ihee, 2009;Ihee et al, 2005a;Plech et al, 2004) can probe structural dynamics in non-crystalline states of materials, complementing the X-ray diffraction technique.…”

Section: Introductionmentioning

confidence: 99%