Spatiotemporal kinetics in solution studied by time-resolved X-ray liquidography (solution scattering)

Tae Kyu Kim, Jae Hyuk Lee, Michael Wulff, Qingyu Kong, Hyotcherl Lhee

Research output: Contribution to journalReview article

60 Citations (Scopus)

Abstract

Information about temporally varying molecular structure during chemical processes is crucial for understanding the mechanism and function of a chemical reaction. Using ultrashort optical pulses to trigger a reaction in solution and using time-resolved X-ray diffraction (scattering) to interrogate the structural changes in the molecules, time-resolved X-ray liquidography (TRXL) is a direct tool for probing structural dynamics for chemical reactions in solution. TRXL can provide direct structural information that is difficult to extract from ultrafast optical spectroscopy, such as the time dependence of bond lengths and angles of all molecular species including shortlived intermediates over a wide range of times, from picoseconds to milliseconds. TRXL elegantly complements ultrafast optical spectroscopy because the diffraction signals are sensitive to all chemical species simultaneously and the diffraction signal from each chemical species can be quantitatively calcu-lated from its three-dimensional atomic coordinates and compared with experimental TRXL data. Since X-rays scatter from all the atoms in the solution sample, solutes as well as the solvent, the analysis of TRXL data can provide the temporal behavior of the solvent as well as the structural progression of all the solute molecules in all the reaction pathways, thus providing a global picture of the reactions and accurate branching ratios between multiple reaction pathways. The arrangement of the solvent around the solute molecule can also be extracted. This review summarizes recent developments in TRXL, including technical innovations in synchrotron beamlines and theoretical analysis of TRXL data, as well as several examples from simple molecules to an organometallic complex, nanoparticles, and proteins in solution. Future potential applications of TRXL in femtosecond studies and biologically relevant molecules are also briefly mentioned.

Original languageEnglish
Pages (from-to)1958-1980
Number of pages23
JournalChemPhysChem
Volume10
Issue number12
DOIs
Publication statusPublished - 2009 Aug 24

Fingerprint

Scattering
X rays
Kinetics
kinetics
scattering
x rays
Molecules
solutes
molecules
Chemical reactions
Diffraction
chemical reactions
diffraction
Structural dynamics
Bond length
Organometallics
dynamic structural analysis
Synchrotrons
Molecular structure
progressions

All Science Journal Classification (ASJC) codes

  • Atomic and Molecular Physics, and Optics
  • Physical and Theoretical Chemistry

Cite this

Kim, Tae Kyu ; Lee, Jae Hyuk ; Wulff, Michael ; Kong, Qingyu ; Lhee, Hyotcherl. / Spatiotemporal kinetics in solution studied by time-resolved X-ray liquidography (solution scattering). In: ChemPhysChem. 2009 ; Vol. 10, No. 12. pp. 1958-1980.
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Spatiotemporal kinetics in solution studied by time-resolved X-ray liquidography (solution scattering). / Kim, Tae Kyu; Lee, Jae Hyuk; Wulff, Michael; Kong, Qingyu; Lhee, Hyotcherl.

In: ChemPhysChem, Vol. 10, No. 12, 24.08.2009, p. 1958-1980.

Research output: Contribution to journalReview article

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