Quick X-ray reflectivity using monochromatic synchrotron radiation for time-resolved applications.

A new technique for the parallel collection of X-ray reflectivity (XRR) data, compatible with monochromatic synchrotron radiation and flat substrates, is described and applied to the in situ observation of thin-film growth. The method employs a polycapillary X-ray optic to produce a converging fan of radiation, incident onto a sample surface, and an area detector to simultaneously collect the XRR signal over an angular range matching that of the incident fan. Factors determining the range and instrumental resolution of the technique in reciprocal space, in addition to the signal-to-background ratio, are described in detail. This particular implementation records ∼5° in 2θ and resolves Kiessig fringes from samples with layer thicknesses ranging from 3 to 76 nm. The value of this approach is illustrated by showing in situ XRR data obtained with 100 ms time resolution during the growth of epitaxial La0.7Sr0.3MnO3 on SrTiO3 by pulsed laser deposition at the Cornell High Energy Synchrotron Source (CHESS). Compared with prior methods for parallel XRR data collection, this is the first method that is both sample-independent and compatible with the highly collimated, monochromatic radiation typical of third-generation synchrotron sources. Further, this technique can be readily adapted for use with laboratory-based sources.

Measurements of surface diffusivity and coarsening during pulsed laser deposition.

Pulsed laser deposition (PLD) of homoepitaxial SrTiO(3) 001 was studied with in situ x-ray specular reflectivity and surface diffuse x-ray scattering. Unlike prior reflectivity-based studies, these measurements access both time and length scales of the evolution of the surface morphology during growth. In particular, we show that this technique allows direct measurements of the diffusivity for both inter- and intralayer transport. Our results explicitly limit the possible role of island breakup, demonstrate the key roles played by nucleation and coarsening in PLD, and place an upper bound on the Ehrlich-Schwoebel barrier for downhill interlayer diffusion.

In situ x-ray reflectivity studies of dynamics and morphology during heteroepitaxial complex oxide thin film growth.

We present a method, based on refraction effects in continuous, stratified media, for quantitative analysis of specular x-ray reflectivity from interfaces with atomic-scale roughness. Roughness at interfaces has previously been incorporated into this framework via Fourier transform of a continuous height distribution, but this approach breaks down when roughness approaches the atomic scale and manifests discrete character. By modeling the overall roughness at interfaces as a convolution of discrete and continuous height distributions, we have extended the applicability of this reflectivity model to atomic-scale roughness. The parameterization of thickness and roughness enables quantitative analysis of time-resolved in situ reflectivity studies of thin film growth, modeling step-flow, layer-by-layer and three-dimensional growth within a single framework. We present the application of this model to the analysis of anti-Bragg growth oscillations measured in situ during heteroepitaxial growth of La(0.7)Sr(0.3)MnO(3) on [Formula: see text] SrTiO(3) at different temperatures and pressures, and discuss the evolution of surface morphology.

Multiple time scales in diffraction measurements of diffusive surface relaxation.

We grew SrTiO3 on SrTiO3(001) by pulsed laser deposition, using x-ray scattering to monitor the growth in real time. The time-resolved small-angle scattering exhibits a well-defined length scale associated with the spacing between unit-cell high surface features. This length scale imposes a discrete spectrum of Fourier components and rate constants upon the diffusion equation solution, evident in multiple exponential relaxation of the "anti-Bragg" diffracted intensity. An Arrhenius analysis of measured rate constants confirms that they originate from a single activation energy.

Observed effects of a changing step-edge density on thin-film growth dynamics.

We grew SrTiO(3) on SrTiO(3)(001) by pulsed laser deposition, while observing x-ray diffraction at the (00(1/2)) position. The drop DeltaI in the x-ray intensity following a laser pulse contains information about plume-surface interactions. Kinematic theory predicts DeltaI/I = -4sigma(1 - sigma), so that DeltaI /I depends only on the amount of deposited material sigma. In contrast, we observed experimentally that |DeltaI /I| < 4sigma(1 - sigma) and that DeltaI /I depends on the phase of x-ray growth oscillations. The combined results suggest a fast smoothing mechanism that depends on surface step-edge density.