The structure of short-lived excited states of molecular complexes by time-resolved X-ray diffraction

Coppens, Philip; Vorontsov, Ivan I.; Graber, Tim; Gembický, Milan; Kovalevsky, Andrey

doi:10.1107/s0108767304029551

Cited by 90 publications

(63 citation statements)

References 42 publications

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“…We collected complete diffraction data, from which structures were solved and refined at different delays with good quality (Lorenc et al, submitted) and in very good agreement with the structures obtained at thermal equilibrium (Floquet et al, 2005). As no phase separation was observed during the process, we could deduce a homogeneous excitation of the molecules in the crystal which, as explained in detail by Coppens (Coppens et al, 2005), modifies the structure factor as the weighted contribution of the fraction of molecules in HS (x HS ) and LS (1-x HS ) states:…”

Section: Photo-excitation Of Spin-crossover Complexes: Towards Picosementioning

confidence: 71%

“…Photocrystallography is a new frontier in the field of structural science (Coppens et al, 2005;Collet et al, 2006), promising direct access to the structural rearrangement driven by cw or pulsed laser irradiation toward a transient, permanent or photo-steady state (steady state maintained by cw laser). Among the different light-driven processes, photoinduced phase transitions (Buron and Collet, 2005;Koshihara and Kuwata-Gonokami, 2006;Nasu, 1997) represent a fascinating perspective to manipulate with light the macroscopic physical properties of a material.…”

Section: Introductionmentioning

confidence: 99%

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State of the art and opportunities in probing photoinduced phase transitions in molecular materials by conventional and picosecond X-ray diffraction

Collet¹,

Cointe²,

Lorenc³

et al. 2008

Zeitschrift Für Kristallographie - Crystalline Materials

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Abstract. The optical control of the macroscopic physical properties (magnetic, optical . . .) of a material by laser irradiation is gaining interest through the emerging field of photoinduced phase transitions. Light-induced changes of the macroscopic state of a material involves subtle coupling between the electronic and structural degrees of freedom, which are essential to stabilize the photo-excited state, different in nature from the stable state. Therefore the new experimental field of photocrystallography plays a key role. It goes far beyond simple structural analysis under laser excitation. By playing on different physical parameters and developing the techniques and analysis, one can investigate new out of equilibrium physics through light-driven cooperative dynamics and transformations in materials. This paper is reviewing different aspects of the use of photocrystallography to investigate the nature, the mechanisms and the dynamics of photoinduced phase transitions for photo-steady or long-lived states, as well as transformations driven by an ultra-short light pulse. We also give a brief overview on recent advances in time-resolved crystallography with 100 ps resolution.

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Section: Photo-excitation Of Spin-crossover Complexes: Towards Picosementioning

confidence: 71%

Section: Introductionmentioning

confidence: 99%

State of the art and opportunities in probing photoinduced phase transitions in molecular materials by conventional and picosecond X-ray diffraction

Collet¹,

Cointe²,

Lorenc³

et al. 2008

Zeitschrift Für Kristallographie - Crystalline Materials

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show abstract

“…Previous reports highlighted a 3 A 2u -symmetry lowest-lying triplet state [204,205], with a measured lifetime of 9.8 µs in deoxygenated water [206][207][208] and a quantum yield of approximately 100% [208]. The geometry of such a long-lived triplet state was thoroughly investigated in the crystal phase using both ultrafast [209][210][211] and stationary-state X-ray methods [212,213]. The crucial structural parameter is the contraction of the Pt-Pt bond distance, which , from analysis of TR-XXS data collected at 100 ps and 1 µs after laser excitation at 267 nm [199].…”

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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“…Before each X-ray pulse a laser pulse excites the molecules of interest. Coppens et al (2005) describe picosecond powder diffraction experiments on molecular excitations to a singlet state, and microsecond experiments on inorganic complexes. The field is rapidly developing and will be an important application of free-electron lasers.…”

Section: Time-resolved Crystallographymentioning

confidence: 99%

The success story of crystallographyThis Laue centennial article has also been published inZeitschrift für Kristallographie[Schwarzenbach (2012).Z. Kristallogr.227, 52–62].

Schwarzenbach

2011

Acta Cryst Sect A

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Diffractionists usually place the birth of crystallography in 1912 with the first X-ray diffraction experiment of Friedrich, Knipping and Laue. This discovery propelled the mathematical branch of mineralogy to global importance and enabled crystal structure determination. Knowledge of the geometrical structure of matter at atomic resolution had revolutionary consequences for all branches of the natural sciences: physics, chemistry, biology, earth sciences and material science. It is scarcely possible for a single person in a single article to trace and appropriately value all of these developments. This article presents the limited, subjective view of its author and a limited selection of references. The bulk of the article covers the history of X-ray structure determination from the NaCl structure to aperiodic structures and macromolecular structures. The theoretical foundations were available by 1920. The subsequent success of crystallography was then due to the development of diffraction equipment, the theory of the solution of the phase problem, symmetry theory and computers. The many structures becoming known called for the development of crystal chemistry and of data banks. Diffuse scattering from disordered structures without and with partial long-range order allows determination of short-range order. Neutron and electron scattering and diffraction are also mentioned.

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The structure of short-lived excited states of molecular complexes by time-resolved X-ray diffraction

Cited by 90 publications

References 42 publications

State of the art and opportunities in probing photoinduced phase transitions in molecular materials by conventional and picosecond X-ray diffraction

State of the art and opportunities in probing photoinduced phase transitions in molecular materials by conventional and picosecond X-ray diffraction

Synchrotron ultrafast techniques for photoactive transition metal complexes

The success story of crystallographyThis Laue centennial article has also been published inZeitschrift für Kristallographie[Schwarzenbach (2012).Z. Kristallogr.227, 52–62].

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