arXiv subjects

Jörg Rottler

Publications and source records attributed to Jörg Rottler.

At least 19 recordsLinked to original sources

arXiv2026

Machine Learning Guided Discovery of Corundum High Entropy Oxides

Early thinking in the field of high entropy oxides (HEOs) emphasized their likely abundance, with combinatorial arguments hinting at a myriad of new materials. The experimental reality has proven more challenging: the stability of HEOs cannot be straightforwardly predicted based on ionic radii, lattice geometry, and charge-balancing considerations alone. In this work, we employ machine learning interatomic potentials (MLIPs) to predict the synthesizability of HEOs of the form $A_2$O$_3$ derived from a selection of trivalent cations. From nearly 500 possible compositions, we identify 16 promising candidates for experimental validation with solid-state and combustion synthesis. We discover three new HEOs in the corundum structure, including (Al,Cr,Fe,Rh,Sc)$_2$O$_3$, and one novel cation-ordered phase, (Al,Fe,Ga,Sc)$_2$O$_3$. By far the most common synthesis outcome was a mixture of competing phases, sometimes involving redox reactions. Our results also reveal profound synthesis method dependence for the final product, where qualitatively equivalent outcomes between the two synthesis methods were only observed for 3 of the 16 tested compositions. We conclude that the occurrence rate of HEOs is far rarer than initially believed and that machine learning approaches can effectively guide us to the "needle in the haystack".

cond-mat.mtrl-sci↗

arXiv2026

Mechanical loss in amorphous solids: spatial correlations, interacting transitions, and annealed thermodynamic pathways

The disordered and defect-rich structure of amorphous solids forms heterogeneous, high-dimensional energy landscapes. Such an energy landscape can be described by a discrete-state network of transitions between stable energy minima. Under low-frequency mechanical oscillations, defect-mediated, thermally activated transitions provide a microscopic mechanism for mechanical dissipation that are the dominant cause of mechanical loss in the mirror coatings of ground based gravitational waves detectors. Using molecular simulations, we find spatially correlated and strongly interacting transitions that require a general network description instead of a superposition of independent two-level systems as traditionally assumed. An annealing study combined with an analysis of dominant relaxation paths in the energy landscape reveals novel mechanisms for reducing room temperature mechanical loss.

cond-mat.mtrl-sci↗

arXiv2026

Connected Network Model for the Mechanical Loss of Amorphous Materials

Dissipation in amorphous solids at low frequencies is commonly attributed to activated transitions of isolated two-level systems (TLS) that come in resonance with elastic or electric fields. Materials with low mechanical or dielectric loss are urgently needed for applications in gravitational wave detection, high precision sensors, and quantum computing. Using atomistic modeling, we explore the energy landscape of amorphous silicon and titanium dioxide, and find that the pairs of energy minima that constitute single TLS form a sparsely connected network with complex topologies. Motivated by this observation, we develop an analytically tractable theory for mechanical loss of the full network from a nonequilibrium thermodynamic perspective. We demonstrate that the connectivity of the network introduces new mechanisms that can both reduce low frequency dissipation through additional low energy relaxation pathways, and increase dissipation through a broad distribution of energy minima. As a result, the connected network model predicts mechanical loss with distinct frequency profiles compared to the isolated TLS model. This not only calls into question the validity of the TLS model, but also gives us many new avenues and properties to analyze for the targeted design of low mechanical loss materials.

cond-mat.mtrl-sci↗

arXiv2025

The influence of solute induced memory on interface migration

Interface migration governs microstructural evolution during phase transformations and grain growth thereby dictating those material properties that depend on microstructure. Recent work continues to highlight the rich range of behaviors exhibited by migrating interfaces and the complex connection between these behaviors and the underlying atomistic processes that determine coarse-grained interfacial mobility. For interfaces moving at low homologous temperatures and small driving forces, we show that significant non-Markovian effects can arise that invalidate commonly used analysis methods. Specifically, we demonstrate that solute can act as a source of such non-Markovian motion. In turn, we introduce a time-local (TCL) propagator approach to account for memory-dominated short and intermediate time interface dynamics. This approach extrapolates to the long time diffusive limit, enabling robust mobility estimates from simulation windows far shorter than those required to observe linear scaling directly. Comparison with solute-free boundaries validates the method and quantifies solute drag in the Cahn-Hillert sense, providing a route to extract drag coefficients and effective mobilities across a range of solute concentrations. Our results demonstrate that analysis including memory is essential for connecting atomistic simulations to continuum models and offer a practical framework for studying interface kinetics in systems with slow internal processes.

cond-mat.mtrl-sci↗

arXiv2025

The origin and scarcity of breathing pyrochlore lattices in spinel oxides

Breathing pyrochlores are a unique class of materials characterized by a three-dimensional lattice of corner-sharing tetrahedra. However, unlike conventional pyrochlores where all tetrahedra are identical in size, the breathing pyrochlore lattice is composed of alternating large and small tetrahedra. Experimental realizations of the breathing pyrochlore lattice are rare but they do occur in $A$-site ordered spinels, as in the prototype materials LiGaCr$_4$O$_8$ and LiInCr$_4$O$_8$. In this work, we demonstrate that Cr cannot be straightforwardly substituted with other magnetic transition metals while retaining the breathing pyrochlore structure. To explain this observation, we perform density functional theory (DFT) calculations to investigate the formation and stability of LiGaCr$_4$O$_8$ and LiInCr$_4$O$_8$, focusing on the energy scales associated with $A$ and $B$-site orderings as well as the magnetic exchange interactions of Cr ions. We identify the strong octahedral site preference of Cr$^{3+}$ as a key factor in protecting the structural integrity of the pyrochlore sublattice, which in turn enables the breathing distortion to proceed. We also demonstrate that the charge order between the $A$ (Li) and $A'$ sites (Ga or In) is maintained at all temperatures up to decomposition. Furthermore, while the magnetic exchange interactions constitute a relatively small energy scale and therefore do not play a fundamental role in the structural stability of LiGaCr$_4$O$_8$ and LiInCr$_4$O$_8$, magnetism may play a critical role in setting the magnitude of the tetrahedral distortion. Ultimately, we conclude that the scarcity of breathing pyrochlores is a consequence of the stringent requirement on site ordering for their formation.

cond-mat.mtrl-sci↗

arXiv2024

Short-range order and local distortions in entropy stabilized oxides

An idealized high entropy oxide is characterized by perfect chemical disorder and perfect positional order. In this work, we investigate the extent to which short-range order (SRO) and local structural distortions impede that idealized scenario. Working in the entropy stabilized $α$-PbO$_2$ structure, we compare a two-component system, (Ti,Zr)O$_2$, with a four-component system, (Ti,Zr,Hf,Sn)O$_2$, using a combination of experimental and computational approaches. Special quasi-random structures are used in conjunction with density functional theory calculations to investigate the local distortions around specific elements revealing significant local distortions that are relatively insensitive to the number of chemical constituents. Using finite temperature Monte Carlo simulations, we are able to reproduce the previously experimentally observed SRO and transition temperature for the two-component system. However, the ideal configurational entropy is never reached, so SRO is expected even at synthesis temperatures. On the other hand, the order-disorder transition temperature is dramatically lower and experimentally inaccessible for the four-component system, while the configurational entropy is closer to ideal and less sensitive to temperature. Total scattering measurements and pair distribution function analysis of slow-cooled and quenched samples support this view. In general, we demonstrate that SRO effects in high entropy materials are less prevalent as more components are added in, provided the pairwise interaction strengths remain comparable, while local distortions are less affected by the number of components.

cond-mat.mtrl-sci↗

arXiv2024

Thermally activated intermittent flow in amorphous solids

Using mean field theory and a mesoscale elastoplastic model, we analyze the steady state shear rheology of thermally activated amorphous solids. At sufficiently high temperature and driving rates, flow is continuous and described by well-established rheological flow laws such as Herschel-Bulkley and logarithmic rate dependence. However, we find that these flow laws change in the regime of intermittent flow, were collective events no longer overlap and serrated flow becomes pronounced. In this regime, we identify a thermal activation stress scale, $x_{a}(T,\dotγ)$, that wholly captures the effect of driving rate $\dotγ$ and temperature $T$ on average flow stress, stress drop (avalanche) size and correlation lengths. Different rheological regimes are summarized in a dynamic phase diagram for the amorphous yielding transition. Theoretical predictions call for a need to re-examine the rheology of very slowly sheared amorphous matter much below the glass transition.

cond-mat.soft↗

arXiv2023

Thawed Matrix method for computing Local Mechanical Properties of Amorphous Solids

We present a method for computing locally varying nonlinear mechanical properties in particle simulations of amorphous solids. Plastic rearrangements outside a probed region are suppressed by introducing an external field that directly penalizes large nonaffine displacements. With increasing strength of the field, plastic deformation can be localized. We characterize the distribution of local plastic yield stresses (residual local stresses to instability) with our approach, and assess the correlation of their spatial maps with plastic activity in a model two-dimensional amorphous solid. Our approach reduces artefacts inherent in a previous method known as the "frozen matrix" approach that enforces fully affine deformation, and improves the prediction of plastic rearrangements from structural information.

cond-mat.soft↗

arXiv2023

Phase stability of entropy stabilized oxides with the $α$-PbO$_2$ structure

The prediction of new high entropy oxides (HEOs) remains a profound challenge due to their inherent chemical complexity. In this work, we combine experimental and computational methods to search for new HEOs in the tetravalent $A$O$_2$ family, using exclusively $d^0$ and $d^{10}$ cations, and to explain the observed phase stability of the $α$-PbO$_2$ structure, as found for the medium entropy oxide (Ti, Zr, Hf, Sn)O$_2$. Using a pairwise approach to approximate the mixing enthalpy, we confirm that $α$-PbO$_2$ is the expected lowest energy structure for this material above other candidates including rutile, baddeleyite, and fluorite structures. We also show that no other five-component compound composed of the tetravalent cations considered here is expected to form under solid state synthesis conditions, which we verify experimentally. Ultimately, we conclude that the flexible geometry of the $α$-PbO$_2$ structure can be used to understand its stability among tetravalent HEOs.

cond-mat.mtrl-sci↗

arXiv2023

Understanding the role of entropy in high entropy oxides

The field of high entropy oxides (HEOs) flips traditional materials science paradigms on their head by seeking to understand what properties arise in the presence of profound configurational disorder. This disorder, which originates from multiple elements sharing a single lattice site, can take on a kaleidoscopic character due to the vast numbers of possible elemental combinations. High configurational disorder appears to imbue some HEOs with functional properties that far surpass their non-disordered analogs. While experimental discoveries abound, efforts to characterize the true magnitude of the configurational entropy and understand its role in stabilizing new phases and generating superior functional properties have lagged behind. Understanding the role of configurational disorder in existing HEOs is the crucial link to unlocking the rational design of new HEOs with targeted properties. In this Perspective, we attempt to establish a framework for articulating and beginning to address these questions in pursuit of a deeper understanding of the true role of entropy in HEOs.

cond-mat.mtrl-sci↗

arXiv2022

Simple generic picture of toughness in solid polymer blends

Toughness $\mathcal{T}$ of a brittle polymeric solid can be enhanced by blending another compatible and ductile polymer. While this common wisdom is generally valid, a generic picture is lacking that connects the atomistic details to the macroscopic non-linear mechanics. Using all-atom and complementary generic simulations we show how a delicate balance between the side group contact density of the brittle polymers $ρ_{\rm c}$ and its dilution upon adding a second component controls $\mathcal{T}$. A broad range of systems follows a universal trend in $\mathcal{T}$ with ${\rm d}ρ_{\rm c}/{\rm d}\varepsilon$, where $\varepsilon$ is the tensile strain. The simulation data is consistent with a simple model based on the parallel spring analogy.

cond-mat.soft↗

arXiv2022

Dynamic phase diagram of plastically deformed amorphous solids at finite temperature

The yielding transition that occurs in amorphous solids under athermal quasistatic deformation has been the subject of many theoretical and computational studies. Here, we extend this analysis to include thermal effects at finite shear rate, focusing on how temperature alters avalanches. We derive a nonequilibrium phase diagram capturing how temperature and strain rate effects compete, when avalanches overlap, and whether finite-size effects dominate over temperature effects. The predictions are tested through simulations of an elastoplastic model in two dimensions and in a mean-field approximation. We find a new scaling for temperature-dependent softening in the low-strain rate regime when avalanches do not overlap, and a temperature-dependent Herschel-Bulkley exponent in the high strain rate regime when avalanches do overlap.

cond-mat.soft↗

arXiv2021

Nanotube heat conductors under tensile strain: Reducing the three-phonon scattering strength of acoustic phonons

Acoustic phonons play a special role in lattice heat transport, and confining these low-energy modes in low-dimensional materials may enable nontrivial transport phenomena. By applying lowest-order anharmonic perturbation theory to an atomistic model of a carbon nanotube, we investigate numerically and analytically the spectrum of three-phonon scattering channels in which at least one phonon is of low energy. Our calculations show that acoustic longitudinal (LA), flexural (FA), and twisting (TW) modes in nanotubes exhibit a distinct dissipative behavior in the long-wavelength limit, $|k| \rightarrow 0$, which manifests itself in scattering rates that scale as $Γ_{\rm{LA}}\sim |k|^{-1/2}$, $Γ_{\rm{FA}}\sim k^0$, and $Γ_{\rm{TW}}\sim |k|^{1/2}$. These scaling relations are a consequence of the harmonic lattice approximation and critically depend on the condition that tubes are free of mechanical strain. In this regard, we show that small amounts of tensile lattice strain $ε$ reduce the strength of anharmonic scattering, resulting in strain-modulated rates that, in the long-wavelength limit, obey $Γ\sim ε^{r} |k|^{s}$ with $r\leq 0$ and $s\geq 1$, irrespectively of acoustic mode polarization. Under the single-mode relaxation time approximation of the linearized Peierls-Boltzmann equation (PBE), the long-tube limit of lattice thermal conductivity in stress-free and stretched tube configurations can be unambiguously characterized. Going beyond relaxation time approximations, analytical results obtained in the present study may help to benchmark numerical routines which aim at deriving the thermal conductivity of nanotubes from an exact solution of the PBE.

cond-mat.mes-hall↗

arXiv2021

Avalanches in the athermal quasistatic limit of sheared amorphous solids: an atomistic perspective

We study the statistical properties of the yielding transition in model amorphous solids in the limit of slow, athermal deformation. Plastic flow occurs via alternating phases of elastic loading punctuated by rapid dissipative events in the form of collective avalanches. We investigate their characterization through energy vs. stress drops and at multiple stages of deformation, thus revealing a change of spatial extent of the avalanches and degree of stress correlations as deformation progresses. We show that the statistics of stress and energy drops only become comparable for large events in the steady flow regime. Results for the critical exponents of the yielding transition are discussed in the context of prior studies of similar type, revealing the influence of model glass and preparation history.

cond-mat.soft↗

arXiv2021

Signatures of the spatial extent of plastic events in the yielding transition in amorphous solids

Amorphous solids are yield stress materials that flow when a sufficient load is applied. Their flow consists of periods of elastic loading interrupted by rapid stress drops, or avalanches, coming from microscopic rearrangements known as shear transformations (STs). Here we show that the spatial extent of avalanches in a steadily sheared amorphous solid has a profound effect on the distribution of local residual stresses $x$. We find that in this distribution, the most unstable sites are located in a system size dependent plateau. While the entrance into the plateau is set by the lower cutoff of the mechanical noise produced by individual STs, the departure from the usually assumed power-law (pseudogap) form $P(x) \sim x^θ$ comes from far field effects related to spatially extended rearrangements. Interestingly, we observe that the average value of weakest sites $\langle x_{min} \rangle$ is located in an intermediate power law regime between the pseudogap and the plateau regimes, whose exponent decreases with system size. Our findings imply a new scaling relation linking the exponents characterizing the avalanche size and residual stress distributions.

cond-mat.dis-nn↗

arXiv2020

Residual stress distributions in athermally deformed amorphous solids from atomistic simulations

The distribution of local residual stresses (threshold to instability) that controls the statistical properties of plastic flow in athermal amorphous solids is examined with an atomistic simulation technique. For quiescent configurations, the distribution has a pseudogap (power-law) form with an exponent that agrees well with global yielding statistics. As soon as deformation sets in, the pseudogap region gives way to a system size dependent plateau at small residual stresses that can be understood from the statistics of local residual stress {\em differences} between plastic events. Results further suggest that the local yield stress in amorphous solids changes even if the given region does not participate in plastic activity.

cond-mat.dis-nn↗

arXiv2020

Heat transport in carbon nanotubes: Length dependence of phononic conductivity from the Boltzmann transport equation and molecular dynamics

In this article, we address lattice heat transport in single-walled carbon nanotubes (CNTs) by a quantum mechanical calculation of three-phonon scattering rates in the framework of the Boltzmann transport equation (BTE) and classical molecular dynamics (MD) simulation. Under a consistent choice of an empirical, realistic atomic interaction potential, we compare the tube length dependence of the lattice thermal conductivity (TC) at room temperature determined from an iterative solution of the BTE and from a nonequilibrium MD (NEMD) approach. Qualitatively similar trends are found in the limit of short tubes, where an extensive regime of ballistic heat transport prevailing in CNTs of lengths $L\lesssim 1\,\rm{μm}$ is independently confirmed. In the limit of long tubes, the BTE approach suggests a saturation of TC with tube length, whereas direct NEMD simulations of tubes extending up to $L=10\,\rm{μm}$ are demonstrated to be insufficient to settle the question of whether a fully diffusive heat transport regime and an intrinsic value of TC exist for CNTs. Noting that acoustic phonon lifetimes lie at the heart of a saturation of TC with tube length as per the BTE framework, we complement the quantum mechanical prediction of acoustic phonon lifetimes with an analysis of phonon modes in the framework of equilibrium MD (EMD). A normal mode analysis (NMA) with an emphasis on long wavelength acoustic modes corroborates the BTE prediction that heat transport in CNTs in the long tube limit is governed by the low attenuation rates of longitudinal and twisting phonons.

cond-mat.mes-hall↗

arXiv2019

Correlations in the shear flow of athermal amorphous solids: A principal component analysis

We apply principal component analysis, a method frequently used in image processing and unsupervised machine learning, to characterize particle displacements observed in the steady shear flow of amorphous solids. PCA produces a low-dimensional representation of the data and clearly reveals the dominant features of elastic (i.e. reversible) and plastic deformation. We show that the principal directions of PCA in the plastic regime correspond to the soft (i.e. zero energy) modes of the elastic propagator that governs the redistribution of shear stress due to localized plastic events. Projections onto these soft modes also correspond to components of the displacement structure factor at the first nonzero wavevectors, in close analogy to PCA results for thermal phase transitions in conserved Ising spin systems. The study showcases the ability of PCA to identify physical observables related to the broken symmetry in a dynamical nonequilibrium transition.

cond-mat.dis-nn↗