arXiv subjects

Ashley R. Head

Publications and source records attributed to Ashley R. Head.

5 recordsLinked to original sources

arXiv2025

Toward the Origins of Binding Energy Shifts and Satellites Formation During Plasma-XPS Measurements

In plasma X ray photoelectron spectroscopy emerges as a powerful platform for real time, in situ chemical analysis under conditions relevant to semiconductor processing and other plasma enabled technologies. This study investigates the origins of binding energy shifts and satellite peaks formation observed during plasma XPS measurements across conductive, dielectric, and gas phase systems. Using a standard laboratory based ambient pressure XPS apparatus coupled with an alternating current driven capacitively coupled plasma source, we show that metastable surface species, such as transient Au oxides, can be detected during plasma exposure, revealing chemical states hardly accessible using conventional ultrahigh vacuum XPS. In dielectric samples, we observe pressure- and plasma type dependent BE shifts up to 50 eV, attributed to X ray induced and plasma mediated surface charging. These shifts are mitigated at higher pressures plasmas or in electronegative plasmas, the latter due to enhanced charge compensation mechanisms involving slow negative ions. For gas phase species, AC plasma excitation leads to spectral broadening and the emergence of satellite peaks with a few eV energy separations, linked to oscillating local plasma potentials in the probing volume. These findings highlight the important and complex interplay of plasma parameters, surface charging, and local electric fields in shaping XPS spectra. Overall, plasma XPS emerges as a critical metrological tool for probing transient surface chemistry, with implications for semiconductor processing, material synthesis, and plasma diagnostics.

physics.plasm-ph↗

arXiv2025

Operando XPS in Reactive Plasmas: The Importance of The Wall Reactions

Advancements in differential pumping and electron optics over the past few decades have enabled x-ray photoelectron spectroscopy (XPS) measurements at (near-)ambient pressures, bridging the pressure gap for characterizing realistic sample chemistries. Recently, we demonstrated the capabilities of an ambient pressure XPS (APXPS) setup for in-situ plasma environment measurements, allowing plasma-surface interactions to be studied in operando rather than using the traditional before-and-after analysis approach. This new plasma-XPS technique facilitates the identification of reaction intermediates critical for understanding plasma-assisted surface processes relevant to semiconductor nanomanufacturing, such as physical vapor deposition, etching, atomic layer deposition, etc. In this report, we apply the plasma-XPS approach to monitor real-time surface chemical changes on a model Ag(111) single crystal exposed to oxidizing and reducing plasmas. We correlate surface-sensitive data with concurrent gas-phase XPS measurements and residual gas mass-spectra analysis of species generated during plasma exposure, highlighting the significant role of plasma-induced chamber wall reactions. Ultimately, we demonstrate that plasma-XPS provides comprehensive insights into both surface and gas-phase chemistry, establishing it as a versatile and dynamic characterization tool with broad applications in microelectronics research.

physics.plasm-ph↗

arXiv2024

Operando Plasma-XPS for Process Monitoring: Hydrogenation of Copper Oxide Confined Under h-BN Case Study

We demonstrate that ambient pressure x-ray photoelectron spectroscopy (APXPS) can be used for in situ studies of dynamic changes in surface chemistry in a plasma environment. Hexagonal boron nitride (h-BN) was used in this study as a model system since it exhibits a wide array of unique chemical, optical, and electrical properties that make it a prospective material for advanced electronics. To better understand the stability and surface chemistry of h-BN during plasma-assisted processing, we used polycrystalline Cu foils with single-layer h-BN, grown via chemical vapor deposition (CVD), and tracked in real-time the plasma-induced reduction of the underlying Cu oxide using APXPS equipped with 22 kHz 75 W discharge plasma source operating at 13 Pa. Residual gas analysis (RGA) mass-spectra were concurrently collected during plasma-XPS to track reaction products formed during plasma exposure. A clear reduction of CuxO is seen, while an h-BN layer remains intact, suggesting H radical species can attack the exposed and h-BN-covered Cu oxide patches and partially reduce the underlying substrate. In addition to the demonstration and discussion of plasma-XPS capabilities, our results indicate the h-BN encapsulated metallic Cu interface might be repaired without significantly damaging the overlaying h-BN, which is of practical importance for the development of h-BN encapsulated devices and interfaces

cond-mat.mtrl-sci↗

arXiv2023

Ultrathin Magnesium-based Coating as an Efficient Oxygen Barrier for Superconducting Circuit Materials

Scaling up superconducting quantum circuits based on transmon qubits necessitates substantial enhancements in qubit coherence time. Among the materials considered for transmon qubits, tantalum (Ta) has emerged as a promising candidate, surpassing conventional counterparts in terms of coherence time. However, the presence of an amorphous surface Ta oxide layer introduces dielectric loss, ultimately placing a limit on the coherence time. In this study, we present a novel approach for suppressing the formation of tantalum oxide using an ultrathin magnesium (Mg) capping layer deposited on top of tantalum. Synchrotron-based X-ray photoelectron spectroscopy (XPS) studies demonstrate that oxide is confined to an extremely thin region directly beneath the Mg/Ta interface. Additionally, we demonstrate that the superconducting properties of thin Ta films are improved following the Mg capping, exhibiting sharper and higher-temperature transitions to superconductive and magnetically ordered states. Based on the experimental data and computational modeling, we establish an atomic-scale mechanistic understanding of the role of the capping layer in protecting Ta from oxidation. This work provides valuable insights into the formation mechanism and functionality of surface tantalum oxide, as well as a new materials design principle with the potential to reduce dielectric loss in superconducting quantum materials. Ultimately, our findings pave the way for the realization of large-scale, high-performance quantum computing systems.

cond-mat.mtrl-sci↗

arXiv2023

Chemical profiles of the oxides on tantalum in state of the art superconducting circuits

Over the past decades, superconducting qubits have emerged as one of the leading hardware platforms for realizing a quantum processor. Consequently, researchers have made significant effort to understand the loss channels that limit the coherence times of superconducting qubits. A major source of loss has been attributed to two level systems that are present at the material interfaces. We recently showed that replacing the metal in the capacitor of a transmon with tantalum yields record relaxation and coherence times for superconducting qubits, motivating a detailed study of the tantalum surface. In this work, we study the chemical profile of the surface of tantalum films grown on c-plane sapphire using variable energy X-ray photoelectron spectroscopy (VEXPS). We identify the different oxidation states of tantalum that are present in the native oxide resulting from exposure to air, and we measure their distribution through the depth of the film. Furthermore, we show how the volume and depth distribution of these tantalum oxidation states can be altered by various chemical treatments. By correlating these measurements with detailed measurements of quantum devices, we can improve our understanding of the microscopic device losses.

cond-mat.mtrl-sci↗