Ultrafast Laser Synchronization Breakthrough

AMO experiment schematic

Set-up of a nitrogen pulse-pump experiment that uses pulse arrival time information from a cross-correlator mounted downstream from the experiment. Figure courtesy of SLAC National Accelerator Laboratory.

A journal article, just published in Applied Physics Letters, details a major breakthrough for experiments at SLAC’s Linac Coherent Light Source (LCLS).

LCLS delivers intense ultrashort x-ray pulses that can be used to study the motion of atoms as they respond to external triggers, such as an optical laser. In these “pump-probe” experiments, the optical laser “pump” pulse starts a reaction in the material, while the x-ray “probe” pulse investigates the state of the material after a defined time delay. A sequence of x-ray pulses, with different time delays between the laser and x-ray pulses, is used to “film” the reaction in the material.

LCLS ultrafast x-ray pulses basically act like high-speed flashes of a camera strobe, allowing scientists to capture images with a “shutter speed” of less than 100 femtoseconds – the time it takes light to travel the width of a human hair.

In order to be able to “film” optically-induced ultrafast processes, however, scientists need more than just ultrashort x-ray and laser pulses. They also need to synchronize the x-ray pulses to the optical laser pulses with almost femtosecond accuracy, in order to have snapshots with good time resolution (“sharp focus”). This is a major challenge, since the main laser system for the x-ray free electron laser is a kilometer away from the optical laser and experiment.

State-of-the-art synchronization is performed at LCLS by accurately measuring the arrival times of the electron bunches (and corresponding x-ray pulses) relative to the radiofrequency that drives the accelerator, since the optical laser is locked to this reference radiofrequency. The best time resolution so far achieved with this approach is 280 fs (full width at half maximum, FWHM).

Recently, scientists at the LCLS Atomic, Molecular and Optical Science Instrument (AMO) dramatically improved the time resolution for their pump-probe experiments. Their new synchronization strategy is to directly measure the relative arrival time of both the x-ray and optical laser pulses at the experiment on a shot-by-shot basis. They do this by introducing into the x-ray beam what they call a cross-correlator, which is mounted downstream of the main experiment.

AMO scientists split their laser beam, sending it to both a pump-probe experiment and the cross-correlator (with a time delay). In the cross-correlator, the laser beam is reflected off a Si3N4 thin film. The spot of the laser pulse is then imaged with a long-distance microscope on a CCD camera. X-ray pulses also hit the same surface of the Si3N4 film, quasi-instantaneously changing the surface reflectivity.

The x-ray pulse very briefly changes the surface reflectivity. By imaging and measuring the position of this reflectivity change with the reflected laser, AMO scientists can directly measure the relative arrival time of the x-ray and optical laser pulses at their experiment. The scientists then use this pulse arrival time information from the cross-correlator to correct their corresponding experimental data on a shot-by-shot basis.

The AMO team demonstrated their improved time resolution with a nitrogen pump-probe experiment. With the time information from the cross-correlator, they were able to decrease the time resolution of their nitrogen experiment down to only 50 fs (FWHM). That’s almost down to the theoretical limit, allowing scientists to investigate all sorts of new ultrafast science.

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