Ferenc Raksi

REGENERATIVE PULSE SHAPING AND AMPLIFICATION OF ULTRABROADBAND OPTICAL PULSES

Regenerative pulse shaping is used to alleviate gain narrowing during ultrashort-pulse amplification. Amplification bandwidths of ~ 100 nm, or nearly three times wider than the traditional gain-narrowing limit, are produced with a modified Ti:sapphire regenerative amplifier. This novel regenerative amplifier has been used to amplify pulses to the 5-mJ level with a bandwidth sufficient to support ~ 10-fs pulses.

Generation of 18-fs, multiterawatt pulses by regenerative pulse shaping and chirped-pulse amplification

Transform-limited, 18-fs pulses of 4.4-TW peak power are produced in a Ti:sapphire-based chirped-pulsed amplification system at a repetition rate of 50 Hz. Regenerative pulse shaping is used to control gain narrowing during amplification, and an optimized, quintic-phase-limited dispersion compensation scheme is used to control higher-order phase distortions over a bandwidth of ~100 nm. Seed pulses are temporally stretched >100,000 times before amplification.

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).

Picosecond-milliangstrom resolution dynamics by ultrafast x-ray diffraction

Optical pump, x-ray diffraction probe measurements have been used to study the lattice dynamics of single crystals with picosecond-milliangstrom resolution by employing a table- top, laser-driven x-ray source. The x-ray source, consisting of an approximately 30 fs, 75 mJ/pulse, 20 Hz repetition rate, terawatt laser system and a moving Cu wire target assembly, generates approximately 5 X 1010 photons (4π steradians s)-1 of Cu Kα radiation. Lattice spacing changes of as small as 1 X 10-3 Å in a few picoseconds have been detected, utilizing Bragg diffraction from GaAs single crystals. Enhancement of the diffraction intensity associated with degradation of the crystals during and after the laser irradiation has been observed, likely due to a transition from dynamic to kinematic diffraction.

Methods for generation of 10-Hz 100-TW optical pulses

Phase and amplitude control during multiterawatt, ultrashort-pulse amplification is discussed. Methods for efficient energy extraction and scaling to 100-TW peak powers are outlined.

Time-gated medical imaging with ultrafast laser-plasma x rays

Laser-generated, hard x-rays are produced in a > 1018 W/cm2 focus of an ultrashort-pulse laser system. The application of ultrashort-duration, laser-generated x-rays to diagnostic medical imaging is discussed. Time-gated detection allows removal of scattered radiation, improved image quality and possible reduction of patient exposure. Methods for improvement of x-ray yield, design of appropriate drive lasers, and applications to mammography and angiography are also discussed.

Ultrafast 2.5-keV x-ray absorption probing of a chemical reaction with 3-ps time resolution

We perform pump-probe measurements in which intense ultrashort optical pulses are the pump pulses that initiate a chemical reaction and ultrafast x-ray pulses are the probe pulses that monitor the response of the system. We present experimental results on the observation of a chemical reaction process, photoinduced dissociation of gas phase SF6 molecules, detected by ultrafast x-ray absorption spectroscopy with 3 ps time resolution near the sulfur K edge at a photon energy of 2.48 keV (4.98 A). High contrast light pulses of 400 fs duration (500 mJ energy and 0.53 micrometers wavelength) from the INRS terawatt laser were focused on high atomic number targets at an intensity of 5 X 1017 W/cm2 in order to generate an x-ray continuum around the sulfur K edge. The SF6 molecule exhibits intense near shape resonances at the sulfur K and L edges, due to the multiple scattering and interference of the emitted photoelectrons by the fluorine atoms that symmetrically surround the central sulfur atom. The shape resonance of the molecule is clearly resolved in the absence of any pump pulse, and the variation of the x-ray absorption spectrum was measured as a function of the delay between the optical pump and x-ray probe pulses. As expected from theory, the reaction process is faster than can be resolved with the 3 picosecond duration x-ray pulses used in this initial experiment. This fast response can, in principle, be used to measure the duration of ultrashort x-ray pulses.

Techniques for controlling gain narrowing during ultrashort-pulse amplification

Regenerative pulse shaping is used to overcome gain narrowing during ultrashort pulse amplification. We have demonstrated multiple spectral filters for broadening the amplified spectrum. We have produced amplified pulses with an energy of approximately 5 mJ and bandwidths of approximately 100 nm, or nearly 3 times wider than the gain narrowing limit of Ti:sapphire.

Ultrafast x-ray absorbtion and diffraction

Our goal is to watch the evolution of matter on the atomic length scale and on the time scale on which elementary chemical reactions take place. We present initial experiments made in collaboration between UCSD and the INRS laboratory in Canada, on time-resolved ultrafast, 3 ps temporal resolution, near-edge x-ray absorption of gas phase SF6 at 2.4 keV (4.89 A). We can see both the initial presence of the F atoms around the S and their absence after photodissociation produced by pumping with an intense optical pulse. Simulations of ultrafast EXAFS and diffraction experiments are presented. We are constructing an ultrahigh intensity laser to generate ultrafast x-ray pulses from laser-produced plasmas. This laser is especially designed to achieve high average power, short pulse duration and high intensity to produce very high temperature solid density plasmas and ultrahot electrons for ultrafast hard x-ray production at high x-ray photon flux, which should enable us to perform a variety of ultrafast x-ray absorption and diffraction experiments. Finally, we discuss several means to measure the duration of subpicosecond x-ray pulses.

Chemical Reaction Observed by Ultrafast X-Ray Absorption

We have used ultrafast hard x-rays pulses (1.5 ps FWHM) from a laser driven plasma to probe a chemical reaction. We observe photoinduced dissociation of SF6 molecules, detected by 5 A ultrafast near-edge x-ray absorption spectroscopy. The “chemical cross-correlation” measures the x-ray duration with ~400 fs resolution.