Femtosecond Resolution Experiments at Third-Generation Light Sources: a Concept Based on the Statistical Properties of Synchrotron Radiation

The paper describes a new concept of visible pump/X-ray probe/slow detector experiments that could be performed at thirdgeneration synchrotron light sources. We propose a technique that would allow time resolution up to femtosecond capabilities to be recovered from a long (100 ps) X-ray probe pulse. The visible pump pulse must be as short as the desired time resolution. The principle of operation of the proposed pump-probe scheme is essentially based on the statistical properties of the synchrotron radiation. These properties are well known in statistical optics as properties of completely chaotic polarized light. Our technique utilizes the fact that, for any synchrotron light beam there exist some characteristic time (coherence time), which determines the time-scale of the random fluctuations. The typical coherence time of soft X-ray synchrotron light at the exit of monochromator is in the femtosecond range. An excited state is prepared with a pump pulse and then projected with a probe pulse onto a final ion state. The first statistical quantity of interest is the variance of the number of photoelectrons detected during synchrotron radiation pulse. The statistics of concern are defined over an ensemble of synchrotron radiation pulses. From a set of variances measured as a function of coherence time (inversely proportional to monochromator bandwidth) it is possible to reconstruct the femtosecond dynamical process.