arXiv subjects

Karl F. Ludwig

Publications and source records attributed to Karl F. Ludwig.

4 recordsLinked to original sources

arXiv2023

Coherent X-ray Spectroscopy Elucidates Nanoscale Dynamics of Plasma-Enhanced Thin-Film Growth

Sophisticated thin film growth techniques increasingly rely on the addition of a plasma component to open or widen a processing window, particularly at low temperatures. However, the addition of the plasma into the growth environment also complicates the surface dynamical evolution. Taking advantage of continued increases in accelerator-based X-ray source brilliance, this real-time study uses X-ray Photon Correlation Spectroscopy (XPCS) to elucidate the nanoscale surface dynamics during Plasma-Enhanced Atomic Layer Deposition (PE-ALD) of an epitaxial indium nitride film. XPCS examines the evolution of the coherent X-ray scattering speckle pattern, which is a fingerprint of the unique sample microstructure at each moment in time. In PE-ALD, ultrathin films are synthesized from repeated cycles of alternating self-limited surface reactions induced by temporally-separated pulses of material precursor and plasma reactant, allowing the influence of each on the evolving morphology to be examined. During the heteroepitaxial 3D growth examined here, sudden changes in surface structure during initial film growth, consistent with numerous overlapping stress-relief events, are observed. When the film becomes continuous, the nanoscale surface morphology abruptly becomes long-lived with correlation time spanning the period of the experiment. Throughout the growth experiment, there is a consistent repeating pattern of correlations associated with the cyclic growth process, which is modeled as transitions between different surface states. The plasma exposure does not simply freeze in a structure that is then built upon in subsequent cycles, but rather there is considerable surface evolution during all phases of the growth cycle.

cond-mat.mtrl-sci↗

arXiv2023

Local step-flow dynamics in thin film growth with desorption

Desorption of deposited species plays a role in determining the evolution of surface morphology during crystal growth when the desorption time constant is short compared to the time to diffuse to a defect site, step edge or kink. However, experiments to directly test the predictions of these effects are lacking. Novel techniques such as \emph{in-situ} coherent X-ray scattering can provide significant new information. Herein we present X-ray Photon Correlation Spectroscopy (XPCS) measurements during diindenoperylene (DIP) vapor deposition on thermally oxidized silicon surfaces. DIP forms a nearly complete two-dimensional first layer over the range of temperatures studied (40 - 120 $^{\circ}$C), followed by mounded growth during subsequent deposition. Local step flow within mounds was observed, and we find that there was a terrace-length-dependent behavior of the step edge dynamics. This led to unstable growth with rapid roughening ($β>0.5$) and deviation from a symmetric error-function-like height profile. At high temperatures, the grooves between the mounds tend to close up leading to nearly flat polycrystalline films. Numerical analysis based on a 1 + 1 dimensional model suggests that terrace-length dependent desorption of deposited ad-molecules is an essential cause of the step dynamics, and it influences the morphology evolution.

cond-mat.mtrl-sci↗

arXiv2021

Early Stage Growth of Amorphous Thin Film: Average Kinetics, Nanoscale Dynamics and Pressure Dependence

We used the Coherent Grazing Incidence Small Angle X-Ray Scattering (Co-GISAXS) technique to study the average kinetics and nanoscale dynamics during early-stage a-WSi$_2$ sputter deposition. The kinetic and dynamic properties are examined as a function of pressure, which is known to be a critical factor in determining final surface roughness. Surface growth kinetics and dynamics are characterized by time parameters extracted from the height-height structure factor and correlation functions. The roughness at a given length scale reaches a maximum before relaxing down to a steady state. The lateral length scale dependence and pressure dependence are then compared among measured kinetics and dynamics time parameters. Surfaces grown at lower pressures are smoother, leading to longer correlation times. The time to reach a dynamic steady state and a kinetic steady state show contrasting pressure dependence. A dynamic steady state is reached earlier than the kinetic steady state at high pressure. A more random deposition direction and lower kinetic energy at higher pressures can explain these phenomena, along with the hypothesis that larger nanoclusters form in vapor before arriving at the surface. A continuum model is applied to simulate the overall behavior with mixed success.

cond-mat.mtrl-sci↗

arXiv2015

Atomic layer deposition-based tuning of the pore size in mesoporous thin films studied by in situ grazing incidence small angle x-ray scattering

Atomic layer deposition (ALD) enables the conformal coating of porous materials, making the technique suitable for pore size tuning at the atomic level, e.g., for applications in catalysis, gas separation and sensing. It is, however, not straightforward to obtain information about the conformality of ALD coatings deposited in pores with diameters in the low mesoporous regime (< 10 nm). In this work, it is demonstrated that in situ synchrotron based grazing incidence small angle x-ray scattering (GISAXS) can provide valuable information on the change in density and internal surface area during ALD of TiO2 in a porous titania film with small mesopores (3-8 nm). The results are shown to be in good agreement with in situ x-ray fluorescence data representing the evolution of the amount of Ti atoms deposited in the porous film. Analysis of both data sets indicates that the minimum pore diameter that can be achieved by ALD is determined by the size of the Ti-precursor molecule.

cond-mat.mtrl-sci↗