Ultrafast x‐ray absorption probing of a chemical reaction

Ultrafast x‐ray techniques can, in principle, allow us to more directly watch the time evolution of matter, with atomic spatial resolution and with time resolution on the scale of atomic motions such as the making and breaking of chemical bonds, in order to more directly observe the fundamental molecular dynamics underlying the concept of ‘‘mechanism’’ in inorganic, organic, and biochemical reactions. As a step toward this goal, we have observed a chemical reaction process, photoinduced dissociation of gas phase SF6 molecules, detected by ultrafast near‐edge x‐ray absorption spectroscopy with time resolutions of 1.5–3 ps, near the sulfur K edge at a photon energy of 2.48 keV (4.98 A).

[1]  Harris,et al.  MeV x-ray generation with a femtosecond laser. , 1992, Physical review letters.

[2]  Wilfried Schildkamp,et al.  Quantitive analysis of Laue diffraction patterns recorded with a 120 ps exposure from an X-ray undulator , 1992 .

[3]  Joseph L. Dehmer,et al.  Evidence of Effective Potential Barriers in the X‐Ray Absorption Spectra of Molecules , 1972 .

[4]  Ying K. Wu,et al.  mm-wave isochronous FEL and hard X-ray inverse Compton source at the Duke storage ring , 1995 .

[5]  Raymond C. Elton,et al.  X-ray lasers , 1990 .

[6]  K. Boyer,et al.  Multiphoton-induced X-ray emission at 4–5 keV from Xe atoms with multiple core vacancies , 1994, Nature.

[7]  Kent R. Wilson,et al.  Transient x‐ray scattering calculated from molecular dynamics , 1986 .

[8]  C. Pellegrini On some methods of x-ray production from relativistic electron beams. , 1994, Journal of X-ray science and technology.

[9]  D. A. Shirley,et al.  High-resolution measurements of near-edge resonances in the core-level photoionization spectra of SF[sub 6] , 1993 .

[10]  R. Frankel,et al.  Nanosecond X-ray diffraction from biological samples with a laser-produced plasma source. , 1979, Science.

[11]  Swapan Chattopadhyay,et al.  Generation of femtosecond X-rays by 90° Thomson scattering , 1994 .

[12]  M. H. Sher,et al.  Picosecond soft-x-ray pulse length measurement by pump - probe absorption spectroscopy. , 1993 .

[13]  Rose,et al.  Experimental observation of ion correlation in a dense laser-produced plasma. , 1988, Physical review letters.

[14]  Gerard Mourou,et al.  Ultrafast x‐ray sources* , 1993 .

[15]  Falcone,et al.  High density plasmas produced by ultrafast laser pulses. , 1989, Physical review letters.

[16]  David M. Hanson,et al.  Photodissociation of SF6 near the F 1s absorption edge , 1994 .

[17]  B. K. Agarwal,et al.  X-Ray Spectroscopy , 1979 .

[18]  Shirley,et al.  Sulfur 1s core-level photoionization of SF6. , 1986, Physical review. A, General physics.

[19]  Frey,et al.  Faraday-rotation spectra of semimagnetic semiconductors. , 1994, Physical review. B, Condensed matter.

[20]  Muller,et al.  Observation of laser-assisted Auger decay in argon. , 1994, Physical review letters.

[21]  Murakami,et al.  Pulsed-laser irradiated silicon studied by time-resolved x-ray absorption (90-300 eV). , 1986, Physical review letters.

[22]  Richard D. Deslattes,et al.  K‐Absorption Fine Structures of Sulfur in Gaseous SF6 , 1966 .

[23]  M. Richardson,et al.  Applications of Laser Plasma Radiation II , 1995 .

[24]  Ivan V. Tomov,et al.  A high repetition rate, picosecond hard x‐ray system, and its application to time‐resolved x‐ray diffraction , 1993 .

[25]  Anders Persson,et al.  Lund high-power laser facility - systems and first results , 1994 .

[26]  H. Nakamatsu,et al.  Theoretical x‐ray absorption spectra of SF6 and H2S , 1991 .