A hierarchical view on material formation during pulsed-laser synthesis of nanoparticles in liquid

Pulsed-laser assisted nanoparticle synthesis in liquids (PLAL) is a versatile tool for nanoparticle synthesis. However, fundamental aspects of structure formation during PLAL are presently poorly understood. We analyse the spatio-temporal kinetics during PLAL by means of fast X-ray radiography (XR) and scanning small-angle X-ray scattering (SAXS), which permits us to probe the process on length scales from nanometers to millimeters with microsecond temporal resolution. We find that the global structural evolution, such as the dynamics of the vapor bubble can be correlated to the locus and evolution of silver nanoparticles. The bubble plays an important role in particle formation, as it confines the primary particles and redeposits them to the substrate. Agglomeration takes place for the confined particles in the second bubble. Additionally, upon the collapse of the second bubble a jet of confined material is ejected perpendicularly to the surface. We hypothesize that these kinetics influence the final particle size distribution and determine the quality of the resulting colloids, such as polydispersity and modality through the interplay between particle cloud compression and particle release into the liquid

Temporal broadening of attosecond photoelectron wavepackets from solid surfaces

The response of solids to electromagnetic fields is of crucial importance in many areas of science and technology. Many fundamental questions remain to be answered about the dynamics of the photoexcited electrons that underpin this response, which can evolve on timescales of tens to hundreds of attoseconds. How, for example, is the photoexcited electron affected by the periodic potential as it travels in the solid, and how do the other electrons respond in these strongly correlated systems? Furthermore, control of electronic motion in solids with attosecond precision would pave the way for the development of ultrafast optoelectronics. Attosecond electron dynamics can be traced using streaking, a technique in which a strong near-infrared laser field accelerates an attosecond electron wavepacket photoemitted by an extreme ultraviolet light pulse, imprinting timing information onto it. We present attosecond streaking measurements on the wide-bandgap semiconductor tungsten trioxide, and on gold, a metal used in many nanoplasmonic devices. Information about electronic motion in the solid is encoded on the temporal properties of the photoemitted electron wavepackets, which are consistent with a spread of electron transport times to the surface following photoexcitation

In situ and real-time monitoring of structure formation during non-reactive sputter deposition of lanthanum and reactive sputter deposition of lanthanum nitride

Lanthanum and lanthanum nitride thin films were deposited by magnetron sputtering onto silicon wafers covered by natural oxide. In situ and real-time synchrotron radiation experiments during deposition reveal that lanthanum crystallizes in the face-centred cubic bulk phase. Lanthanum nitride, however, does not form the expected NaCl structure but crystallizes in the theoretically predicted metastable wurtzite and zincblende phases, whereas post-growth nitridation results in zincblende LaN. During deposition of the initial 2-3 nm, amorphous or disordered films with very small crystallites form, while the surface becomes smoother. At larger thicknesses, the La and LaN crystallites are preferentially oriented with the close-packed lattice planes parallel to the substrate surface. For LaN, the onset of texture formation coincides with a sudden increase in roughness. For La, the smoothing process continues even during crystal formation, up to a thickness of about 6 nm. This different growth behaviour is probably related to the lower mobility of the nitride compared with the metal. It is likely that the characteristic void structure of nitride thin films, and the similarity between the crystal structures of wurtzite LaN and La2O3, evoke the different degradation behaviours of La/B and LaN/B multilayer mirrors for off-normal incidence at 6.x nm wavelength

Lattice Dynamics of Laser Excited Ferroelectric BaTiO3BaTiO_3

We investigated the lattice dynamics of the prototypic ferroelectric barium titanate close to its ferroelectric-paraelectric phase transition aiming at a better understanding of the atomistic nature of the transition. The usage of time-resolved X-ray techniques allows to disentangle lattice motion and unit cell changes, which, in part, relate to the ferroelectric polarization. In the quasi-static case both the electrical and the laser excitation show a mean-field, simple thermal behaviour, while for time scales shorter than nanoseconds the impulsive nature of the excitation becomes visible

Lattice Dynamics of Laser Excited Ferroelectric BaTiO 3

We investigated the lattice dynamics of the prototypic ferroelectric barium titanate close to its ferroelectric-paraelectric phase transition aiming at a better understanding of the atomistic nature of the transition. The usage of time-resolved X-ray techniques allows to disentangle lattice motion and unit cell changes, which, in part, relate to the ferroelectric polarization. In the quasi-static case both the electrical and the laser excitation show a mean-field, simple thermal behaviour, while for time scales shorter than nanoseconds the impulsive nature of the excitation becomes visible