RESUMEN
X-ray speckle visibility spectroscopy using X-ray free-electron lasers has long been proposed as a probe of fast dynamics in noncrystalline materials. In this paper, numerical modeling is presented to show how the data interpretation of visibility spectroscopy can be impacted by the nonidealities of real-life X-ray detectors. Using simulated detector data, this work provides a detailed analysis of the systematic errors of several contrast extraction algorithms in the context of low-count-rate X-ray speckle visibility spectroscopy and their origins are discussed. Here, it was found that the finite detector charge cloud and pixel size lead to an unavoidable `degeneracy' in photon position determination, and that the contrasts extracted using different algorithms can all be corrected by a simple linear model. The results suggest that experimental calibration of the correction coefficient at the count rate of interest is possible and essential. This allows computationally lightweight algorithms to be implemented for on-the-fly analysis.
RESUMEN
Pump-probe experiments at synchrotrons and free-electron lasers to study ultrafast dynamics in materials far from equilibrium have been well established, but techniques to investigate equilibrium dynamics on the nano- and pico-second timescales remain underdeveloped and experimentally challenging. A promising approach relies on a double-probe X-ray speckle visibility spectroscopy setup at split-and-delay beamlines of X-ray free-electron lasers. However, the logistics in consistently producing two collinear, perfectly overlapping pulses necessary to conduct a faithful experiment is difficult to achieve. In this paper, a method is introduced to extract contrast in the case where an angular misalignment and imperfect overlap exists between the two pulses. Numerical simulations of a dynamical system show that contrast can still be extracted for significant angular misalignments accompanied by partial overlap between the two pulses.
RESUMEN
This paper reports on coherent scattering experiments in the low-count regime with less than one photon per pixel per acquisition on average, conducted with two detectors based on the Eiger single-photon-counting chip. The obtained photon-count distributions show systematic deviations from the expected Poisson-gamma distribution, which result in a strong overestimation of the measured speckle contrast. It is shown that these deviations originate from an artificial increase of double-photon events, which is proportional to the detected intensity and inversely proportional to the exposure time. The observed miscounting effect may have important implications for new coherent scattering experiments emerging with the advent of high-brilliance X-ray sources. Different correction schemes are discussed in order to obtain the correct photon distributions from the data. A successful correction is demonstrated with the measurement of Brownian motion from colloidal particles using X-ray speckle visibility spectroscopy.