sub-picosecond movies of nucleation dynamics

A shortlived SPPS facility is still producing papers – this week it’s the PRL paper by Aaron Lindenberg and some 28 co-authors ” X-Ray Diffuse Scattering Measurements of Nucleation Dynamics at Femtosecond Resolution” Phys. Rev. Lett. 100, 135502 (2008).

This is yet another pump-probe experiment, where pump is a femtosecond laser which ablates/melts a crystal, and a probe is a sub-picosecond x-ray pulse from SPPS. X-ray probe pulse length is still a limiting parameter in overall time resolution of such pump-probe setups. This experiment had a time resolution of 700 fs, but in the near future at XFEL facilities such as LCLS the time resolution will approach tens of femtosecond.

Lindenberg and coworkers were able to look at both high-angle and small-angle diffuse scattering resulting in ablation process in this time-resolved mode. Their data indicates presence of short-lived nanoscale voids (shown in green in the figure on the right) in the liquid state caused by the laser pulse, and these voids merge together to form larger voids over the timescale of 20 ps or so – claims supported by molecular dynamics simulations. While their data was taken in reciprocal space, by recording ensemble-averaged structure factor S(q) at various time delays from the laser pulse, in the future one could envision fully inverting the speckle patterns shown in the figure above, to obtain a real-space images of the nanoscale voids.

Near-Field X-ray Speckle

There is a brand new paper that appeared today in Nature Physics by Cerbino and co-workers that describes a new x-ray coherent technique based on observations of Near-Field Speckle pattern.

Typically x-ray speckles (or visible light speckles) are observed in Fraunhoffer, or far-field diffraction regime, in which parallel beam approximation can be applied.

The other extreme regime is the near-field (aka Fresnel) geometry, where the detector is placed in the relative vicinity of the sample. This regime is often ignored by scientists because of the complicated scattering patterns caused by interference between scattered and transmitted beams.

However, recently it was shown that Fresnel geometry has some advantages – both in terms of performing lensless imaging microscopy: curved wavefronts, resulting from for example focusing Fresnel Zone Plate optics, result in faster convergence of lensless imaging algorythms – see this paper by Williams et al. Phys. Rev. Lett. 97, 025506 (2006) - and now in terms of using near-field x-ray speckle for X-ray Photon Correlation Spectroscopy.

The Near-Field Speckle setup is limited to relatively small Q-range – the example used in the featured paper by Cerbino et. al is covering ultra-small angle scattering range of Q<0.001 inverse nanometers, corresponding to lengthscales on the order of 10 microns. While such low angles are difficult to access with far-field hard x-ray speckle, the same lengthscales can in principle be reached with visible light (laser) speckle – dynamic light scattering techniques. However, one big advantage of x-rays here is their penetrating
ability and no complications due to multiple scattering effects. Therefore, Near Field X-ray Speckle has a lot of potential for use in non-transparent materials and thick specimens where multiple light scattering effects make laser-based measurements difficult.