Search arXivSearch

arXiv · 2102.05726

cryo-ePDF: Overcoming Electron Beam Damage to Study the Local Atomic Structure of Amorphous ALD Aluminum Oxide Thin Films within a TEM

Abstract

Atomic layer deposition (ALD) provides uniform and conformal thin films that are of interest for a range of applications. To better understand the properties of amorphous ALD films, we need improved understanding of their local atomic structure. Previous work demonstrated measurement of how the local atomic structure of ALD-grown aluminum oxide (AlOx) evolves in operando during growth by employing synchrotron high energy X-ray diffraction (HE-XRD). In this work, we report on efforts to employ electron diffraction pair distribution function (ePDF) measurements using more broadly available transmission electron microscope (TEM) instrumentation to study the atomic structure of amorphous ALD-AlOx. We observe electron beam damage in the ALD-coated samples during ePDF at ambient temperature and successfully mitigate this beam damage using ePDF at cryogenic temperatures (cryo-ePDF). We employ cryo-ePDF and Reverse Monte Carlo (RMC) modeling to obtain structural models of ALD-AlOx coatings formed at a range of deposition temperatures from 150-332{\deg}C. From these model structures, we derive structural metrics including stoichiometry, pair distances, and coordination environments in the ALD-AlOx films as a function of deposition temperature. The structural variations we observe with growth temperature are consistent with temperature-dependent changes in the surface hydroxyl density on the growth surface. The sample preparation and cryo-ePDF procedures we report here can be used for routine measurement of ALD-grown amorphous thin films to improve our understanding of the atomic structure of these materials, establish structure-property relationships, and help accelerate the timescale for the application of ALD to address technological needs.

Explore related subjects

Keep this discovery

BibTeXRIS

Ahmed M. Jasim, Xiaoqing He, Yangchuan Xing, Tommi A. White, Matthias J. Young. 2021-02-10. cryo-ePDF: Overcoming Electron Beam Damage to Study the Local Atomic Structure of Amorphous ALD Aluminum Oxide Thin Films within a TEM. https://arxiv.org/abs/2102.05726

Cite the original work for its findings. Save a collection to share your selection of sources.

KEEP EXPLORING

Related papers

Measuring chiral phonons

Chiral phonons are quantized vibrations where the atomic motion in a solid breaks improper rotation symmetries. In many cases, chiral phonons possess angular momenta and are therefore selective to circularly polarized light. Both fundamental and applied research efforts on chiral phonons have been gaining increasing attention owing to their importance in a variety of fields including spintronics, spin-selective chemical reactions, thermal transport, quantum information processing and biosensing, where the bi-directional spin-lattice coupling enabled by chiral phonons can be harnessed in new ways, and potentially lead to new functionalities. Thus far, the studies of chiral phonons across diverse materials platforms have evolved largely independently within these fields, but the experimental techniques are often interrelated. In this perspective, we present a detailed description, as well as advantages and disadvantages of the current approaches for experimentally measuring chiral phonons in chiral and achiral materials. We conclude with a discussion of new methods for measuring chiral phonons. Ultimately, this work seeks to offer an experimental guide for systematically investigating the properties of chiral phonons in various materials systems and applications.

cond-mat.mtrl-sci

A model of grain growth in UN integrating molecular dynamics, phase-field modeling, and uncertainty quantification

Grain growth kinetics and grain-boundary (GB) properties in uranium mononitride (UN) are investigated through an integrated multiscale framework combining molecular dynamics (MD), phase-field modeling, and surrogate-assisted uncertainty quantification. MD simulations yield GB energies for 27 symmetric tilt boundaries from 0--2000~K, which are consistent with available DFT values. The average GB energy is nearly temperature-independent below 1000~K and increases at higher temperatures. A mechanistic pore-drag model applied to the only available grain growth dataset for actinide nitrides yields a mobility reduction factor of $s \approx 0.93$--$0.99$, statistically indistinguishable from unity, confirming that pore drag is negligible under the experimental conditions. The intrinsic GB mobility is therefore extracted directly from the effective mobility, yielding $M_0 = 2.05\times10^{-15}$~m$^4$/(J$\cdot$s) and $Q_M = 0.89$~eV. Phase-field simulations conducted from 1500--2000~K confirm normal curvature-driven grain growth, with grain size distributions converging to the Hillert-like form. A surrogate-assisted global sensitivity analysis---combining principal component analysis, Gaussian process regression, and Sobol decomposition---reveals that the mobility prefactor $M_0$ dominates output variance at all times, followed by the activation energy $Q_M$, while the GB energy $\gamma$ contributes minimally. These results establish the first quantitative grain growth framework for UN and identify the reduction of uncertainty in $M_0$ and $Q_M$ as the highest-priority target for future experimental efforts.

cond-mat.mtrl-sci

Silicon Solar Cell Design for >30% Efficiency via Singlet Fission

Singlet fission (SF) materials convert high-energy photons into multiple charge carriers, providing a route to exceed the efficiency limits of single-junction silicon solar cells without many of the complexities of multi-junction tandem designs. Following the first demonstration of an SF-enhanced silicon solar cell in 2025, there is a need to understand how SF materials can be effectively integrated into high-efficiency industrial silicon devices and translated from proof of concept to a manufacturable technology. Using coupled optical and electrical simulations, we assess the efficiency potential of several industrially relevant silicon cell architectures combined with SF materials. Interdigitated back-contact (IBC) cells offer the greatest potential for improvement due to unrestricted front-surface access and can achieve efficiencies exceeding 33%. However, performance is highly sensitive to front-surface passivation quality. Appropriate silicon design, particularly controlled surface doping and fixed interfacial charge, can mitigate recombination losses and relax passivation requirements for ultra-thin exciton-transfer layers.

cond-mat.mtrl-sci