arXiv subjects

C. Cancellieri

Publications and source records attributed to C. Cancellieri.

11 recordsLinked to original sources

arXiv2026

Residual stress gradient in a thin film within the dislocation pile-up theory

A model for predicting the residual stress gradient in a thin film segment is developed on the basis of the theory of dislocation pile-ups. The initial shear stress within the film is relaxed via the formation of a pile-up of screw dislocations against the impenetrable film-substrate interface. Plastic strain is related to the dislocation density, leading to a fundamental equation, which links the residual stress to this density. The distribution of dislocations within the pile-up for an arbitrary, non-uniform residual stress profile is derived analytically by applying the force balance condition. This results in a singular integro-differential equation for the residual stress profile. The equation is solved numerically by a collocation method for various initial stress distributions: constant, linear, parabolic, and exponential functions. The solutions demonstrate that the established residual stress profile strongly depends on the film segment's thickness-to-width ratio and the initial stress distribution. As this ratio increases, stress relaxation becomes more effective away from the film-substrate interface. In all cases, equilibrium requires a pile-up containing dislocations with both positive and negative Burgers vectors. The total number of dislocations and their density distribution vary significantly with the initial stress profile. This model provides a critical step towards more complex models of residual stress formation in constrained material systems, specifically, thin films.

cond-mat.mtrl-sci↗

arXiv2025

Auger parameter analysis for TiN and AlN thin films via combined in-situ XPS and HAXPES

Auger parameter analysis provides in-depth information about the electronic and chemical bonding properties of TiN and AlN thin films, which are relevant across a wide range of technologies. Meaningful interpretation and analysis of the Auger parameter of these materials have been hindered due to, among other reasons, the absence of reliable references. Here we present a comprehensive study of Auger parameters for TiN and AlN thin films using a dual-source lab-based XPS/HAXPES system equipped with Al Ka and Cr Ka x-ray sources. Due to a large spread of excitation x-ray energy, bulk- and surface-sensitive core-level photoelectrons and Auger transitions are probed. This allows us to study a wide range of Auger and core-level emission lines of TiN and AlN. These measurements can serve as references for further identification of chemical state changes, oxidation state or any deviations in the local chemical environment in these materials. UHV sample transfer was employed to minimise surface contamination. Additionally, we demonstrate how common procedures such as ambient air exposure and Ar+ sputter-etching influence the Auger parameters, highlighting the importance of surface preparation in spectroscopic analysis.

cond-mat.mtrl-sci↗

arXiv2024

Computationally-guided discovery and synthesis of the amorphous nitride Y2WN4

Amorphous materials offer unique functional characteristics, which are often not observed in their crystalline counterparts. This makes them invaluable for many technological applications, such as diffusion barriers in semiconductor devices. However, the computationally guided search for new functional amorphous materials with attractive properties represents a major challenge. In this work, we combine theory and experiment to discover and synthesize the amorphous ternary nitride Y2WN4. We show how computational random structure sampling offers a route to robustly identify chemistries which are hard to crystallize. Experiments prove that the predicted nitride is easily synthesized in amorphous phase with no detectable precipitates. The material exhibits remarkable stability against crystallization at high temperature and as well as excellent oxidation resistance and stability against Cu diffusion. Moreover, Y2WN4 exhibits a sharp onset of optical absorption and an indirect band gap of 2.24 eV. These properties make this material promising for the integration in electronic devices as a high-performance diffusion barrier with adjustable band edges.

cond-mat.mtrl-sci↗

arXiv2019

Advanced chemical state studies of oxide films by lab-based HAXPES combining soft and hard X-ray sources

The greater information depth provided in Hard X-ray Photoelectron Spectroscopy (HAXPES) enables non-destructive analyses of the chemistry and electronic structure of buried interfaces. Moreover, for industrially relevant elements like Al, Si and Ti, the combined access to the Al 1s, Si 1s or Ti 1s photoelectron line and its associated Al KLL, Si KLL or Ti KLL Auger transition, as required for local chemical state analysis on the basis of the Auger parameter, is only possible with hard X-rays. Until now, such photoemission studies were only possible at synchrotron facilities. Recently however, the first commercial XPS/HAXPES systems, equipped with both soft and hard X-ray sources, have entered the market, providing unique opportunities for monitoring the local chemical state of all constituent ions in functional oxides at different probing depths, in a routine laboratory environment. Bulk-sensitive shallow core-levels can be excited using either the hard or soft X-ray source, whereas more surface-sensitive deep core-level photoelectron lines and associated Auger transitions can be measured using the hard X-ray source. As demonstrated for thin Al2O3, SiO2 and TiO2 films, the local chemical state of the constituting ions in the oxide may even be probed at near constant probing depth by careful selection of sets of photoelectron and Auger lines, as excited with the combined soft and hard X-ray sources. We highlight the potential of lab-based HAXPES for the research on functional oxides and also discuss relevant technical details regarding the calibration of the kinetic binding energy scale.

cond-mat.mtrl-sci↗

arXiv2019

k-Resolved electronic structure of buried heterostructure and impurity systems by soft-X-ray ARPES

Angle-resolved photoelectron spectroscopy (ARPES) is the main experimental tool to explore electronic structure of solids resolved in the electron momentum k . Soft-X-ray ARPES (SX-ARPES), operating in a photon energy range around 1 keV, benefits from enhanced probing depth compared to the conventional VUV-range ARPES, and elemental/chemical state specificity achieved with resonant photoemission. These advantages make SX-ARPES ideally suited for buried heterostructure and impurity systems, which are at the heart of current and future electronics. These applications are illustrated here with a few pioneering results, including buried quantum-well states in semiconductor and oxide heterostructures, their bosonic coupling critically affecting electron transport, magnetic impurities in diluted magnetic semiconductors and topological materials, etc. High photon flux and detection efficiency are crucial for pushing the SX-ARPES experiment to these most photon-hungry cases.

cond-mat.mtrl-sci↗

arXiv2015

Polaronic metal state at the LaAlO3/SrTiO3 interface

Interplay of spin, charge, orbital and lattice degrees of freedom in oxide heterostructures results in a plethora of fascinating properties, which can be exploited in new generations of electronic devices with enhanced functionalities. The paradigm example is the interface between the two band insulators LaAlO3 and SrTiO3 (LAO/STO) that hosts two-dimensional electron system (2DES). Apart from the mobile charge carriers, this system exhibits a range of intriguing properties such as field effect, superconductivity and ferromagnetism, whose fundamental origins are still debated. Here, we use soft-X-ray angle-resolved photoelectron spectroscopy to penetrate through the LAO overlayer and access charge carriers at the buried interface. The experimental spectral function directly identifies the interface charge carriers as large polarons, emerging from coupling of charge and lattice degrees of freedom, and involving two phonons of different energy and thermal activity. This phenomenon fundamentally limits the carrier mobility and explains its puzzling drop at high temperatures.

cond-mat.mtrl-sci↗

arXiv2015

Growth-induced electron mobility enhancement at the LaAlO$_3$/SrTiO$_3$ interface

We have studied the electronic properties of the 2D electron liquid present at the LaAlO$_3$/SrTiO$_3$ interface in series of samples prepared at different growth temperatures. We observe that interfaces fabricated at 650°C exhibit the highest low temperature mobility ($\approx 10000 \textrm{ cm}^2/\textrm{Vs}$) and the lowest sheet carrier density ($\approx 5\times 10^{12} \textrm{ cm}^{-2}$). These samples show metallic behavior and Shubnikov-de Haas oscillations in their magnetoresistance. Samples grown at higher temperatures (800-900°C) display carrier densities in the range of $\approx 2-5 \times 10^{13} \textrm{ cm}^{-2}$ and mobilities of $\approx 1000 \textrm{ cm}^2/\textrm{Vs}$ at 4K. Reducing their carrier density by field effect to $8\times 10^{12} \textrm{ cm}^{-2}$ lowers their mobilites to $\approx 50 \textrm{ cm}^2/\textrm{Vs}$ bringing the conductance to the weak-localization regime.

cond-mat.mtrl-sci↗

arXiv2013

Chemistry and structure of homoepitaxial SrTiO$_3$ films and their influence on oxide-heterostructure interfaces

The properties of single-crystal SrTiO$_{3}$ substrates and homoepitaxial SrTiO$_{3}$ films grown by pulsed laser deposition have been compared, in order to understand the loss of interfacial conductivity when more than a critical thickness of nominally homoepitaxial SrTiO$_{3}$ is inserted between a LaAlO$_{3}$ film and a SrTiO$_{3}$ substrate. In particular, the chemical composition and the structure of homoepitaxial SrTiO$_{3}$ investigated by low-energy ion-scattering and surface x-ray diffraction, show that for insulating heterointerfaces, a Sr-excess is present between the LaAlO$_{3}$ and homoepitaxial SrTiO$_{3}$. Furthermore, an increase in the out-of-plane lattice constant is observed in LaAlO$_{3}$, indicating that the conductivity both with and without insertion of SrTiO$_{3}$ thin film originates from a Zener breakdown associated with the polar catastrophe. When more than a critical thickness of homoepitaxial SrTiO$_{3}$ is inserted between LaAlO$_3$ and SrTiO$_3$, the electrons transferred by the electronic reconstruction are trapped by the formation of a Sr-rich secondary phase and Sr-vacancies. The migration of Sr towards the surface of homoepitaxial STO and accompanying loss of interfacial conductivity can be delayed by reducing the Sr-content in the PLD target.

cond-mat.mtrl-sci↗

arXiv2011

Intrinsic origin of the two-dimensional electron gas at polar oxide interfaces

The predictions of the polar catastrophe scenario to explain the occurrence of a metallic interface in heterostructures of the solid solution(LaAlO$_3$)$_{x}$(SrTiO$_3$)$_{1-x}$ (LASTO:x) grown on (001) SrTiO$_3$ were investigated as a function of film thickness and $x$. The films are insulating for the thinnest layers, but above a critical thickness, $t_c$, the interface exhibits a constant finite conductivity which depends in a predictable manner on $x$. It is shown that $t_c$ scales with the strength of the built-in electric field of the polar material, and is immediately understandable in terms of an electronic reconstruction at the nonpolar-polar interface. These results thus conclusively identify the polar-catastrophe model as the intrinsic origin of the doping at this polar oxide interface.

cond-mat.mtrl-sci↗

arXiv2010

Two-dimensional quantum oscillations of the conductance at LaAlO3/SrTiO3 interfaces

We report on a study of magnetotransport in LaAlO3/SrTiO3 interfaces characterized by mobilities of the order of several thousands cm$^{2}$/Vs. We observe Shubnikov-de Haas oscillations that indicate a two-dimensional character of the Fermi surface. The frequency of the oscillations signals a multiple sub-bands occupation in the quantum well or a multiple valley configuration. From the temperature dependence of the oscillation amplitude we extract an effective carrier mass $m^{*}\simeq1.45$\,$m_{e}$. An electric field applied in the back-gate geometry increases the mobility, the carrier density and the oscillation frequency.

cond-mat.mtrl-sci↗

arXiv2009

Tunable Rashba spin-orbit interaction at oxide interfaces

The quasi-two-dimensional electron gas found at the LaAlO3/SrTiO3 interface offers exciting new functionalities, such as tunable superconductivity, and has been proposed as a new nanoelectronics fabrication platform. Here we lay out a new example of an electronic property arising from the interfacial breaking of inversion symmetry, namely a large Rashba spin-orbit interaction, whose magnitude can be modulated by the application of an external electric field. By means of magnetotransport experiments we explore the evolution of the spin-orbit coupling across the phase diagram of the system. We uncover a steep rise in Rashba interaction occurring around the doping level where a quantum critical point separates the insulating and superconducting ground states of the system.

cond-mat.str-el↗