Serial X-ray Crystallography

Serial crystallography (SX) is an emerging technique to determine macromolecules at room temperature. SX with a pump–probe experiment provides the time-resolved dynamics of target molecules. SX has developed rapidly over the past decade as a technique that not only provides room-temperature structures with biomolecules, but also has the ability to time-resolve their molecular dynamics. The serial femtosecond crystallography (SFX) technique using an X-ray free electron laser (XFEL) has now been extended to serial synchrotron crystallography (SSX) using synchrotron X-rays. The development of a variety of sample delivery techniques and data processing programs is currently accelerating SX research, thereby increasing the research scope. In this editorial, I briefly review some of the experimental techniques that have contributed to advances in the field of SX research and recent major research achievements. This Special Issue will contribute to the field of SX research.

Ultrafast manipulation of magnetic anisotropy in a uniaxial intermetallic heterostructure TbCo2/FeCo

We study experimentally and theoretically the dynamics of spin relaxation motion excited by a femtosecond pulse in the TbCo2/FeCo multilayer structures with different ratios of TbCo2 to FeCo thicknesses rd = dTbCo2 / dFeCo. The main attribute of the structure is in-plane magnetic anisotropy artificially induced during sputtering under DC magnetic field. The optical pump-probe method revealed strongly damped high-frequency oscillations of the dynamical Kerr rotation angle, followed by its slow relaxation to the initial state. Modeling experimental results using the Landau-Lifshitz-Gilbert (LLG) equation showed that the observed entire dynamics is due to destruction and restoration of magnetic anisotropy rather than to demagnetization. For the pumping fluence of 7 mJ/cm2, the maximal photo-induced disruption of the anisotropy field is about 14% for the sample with rd = 1 and decreases when rd increases. The anisotropy relaxation is a three-stage process: the ultrafast one occurs within several picoseconds, and the slow one occurs on a nanosecond time scale. The Gilbert damping in the multilayers is found one order of magnitude higher than that in the constituent monolayers.

Ultrafast laser processing of transparent materials supported by in-situ diagnostics

For the development of industrial NIR ultrafast laser processing of transparent materials, the absorption inside the bulk material has to be controlled. Applications we aim for are front and rear side ablation, drilling and inscription of modifications for cleaving and selective laser etching of glass and sapphire in sheet geometry. We applied pump probe technology and in situ stress birefringence microscopy for fundamental studies on the influence of energy and duration (100 fs – 20 ps), temporal and spatial spacing, focusing and beam shaping of the laser pulses. Applying pump probe technique we are able to visualize differences of spatio-temporal build up of absorption, self focusing, shock wave generation for standard, multispot and beam shaped focusing. Incubation effects and disturbance of beam propagation due to modifications or ablation can be observed. In-situ imaging of stress birefringence gained insight in transient build up of stress with and without translation. The results achieved so far, demonstrate that transient stress has to be taken into account in scaling the laser machining throughput of brittle materials. Furthermore it points out that transient stress birefringence is a good indicator for accumulation effects, supporting tailored processing strategies.Cutting results achieved for selective laser etching by single pass laser modification exemplifies the benefits of process development supported by in situ diagnostics.

Controlling the Pump-Probe Optical Response in Asymmetric Tunneling-Controlled Double Quantum Dot Molecule—Metal Nanoparticle Hybrids

In the present work, we investigate the modified nonlinear pump-probe optical properties due to the excitonic–plasmonic interaction of a double semiconductor quantum dot (SQD) molecule coupled to a metal nanoparticle (MNP). More specifically, we study the absorption and the dispersion spectra of a weak electromagnetic field in a hybrid structure with two counterparts, a molecule of two coupled SQDs, and a spherical MNP driven by a field of high intensity. We solve the relevant density matrix equations, calculate the first-order optical susceptibility of the probe field in the strong pumping regime, and investigate the way in which the distance between the two counterparts modifies the optical response, for a variety of values of the physical constants of the system, including the pump-field detuning, the tunnelling rate, and the energy separation gap associated with the excited states of the coupled SQDs.

Study of Impulsive Stimulated Raman Scattering Effects Using the Femtosecond Pump–Probe Z-Scan Technique

Impulsive stimulated Raman scattering (ISRS) is a nonlinear pump–probe spectroscopy technique particularly suitable to study vibrational intermolecular and intramolecular modes in complex systems. For the latter, recent studies of ISRS microscopy with low-energy laser sources have attracted attention for investigation of photosensitive or biological samples. Following this stream of interest, in this paper, we report an investigation on the relationship between femtosecond ISRS data and pump–probe Z-scan measurements, showing that the latter technique is capable of capturing the Kerr nonlinearities induced by the molecular vibrational modes. To this aim, firstly, spectrally filtered and Raman-induced Kerr ISRS signals were simultaneously acquired to determine the sample nonlinear response and to establish the reference data for the Z-scan analysis. Then, by adopting a suitable experimental arrangement to avoid thermo-optical effects, we were able to unambiguously observe the Raman-induced effects in Z-scan measurements, thus obtaining a consistent picture between ISRS and Z-scan for the first time, to the best of our knowledge. Practical applications of the proposed method include calibrated measurements of the contribution of the internal (Raman) and external molecular modes to the nonlinear refractive index.