Publications

Showing 82 results for Author: Stephan Irle

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May, 2026

Journal

Mechanistic insights into rubidium ion adsorption at the quartz (101) surface from quantum chemical metadynamics

Ion sorption extent and mechanism depend in part on the mineral surface termination, which can be highly complex. Variations in surface functional groups, particularly with defect density and surface roughness, influence mineral reactivity towards solutes. In this work, we investigate the adsorption of a rubidium cation (Rb+) at pristine and defect quartz (101) surface sit…
May, 2026

Journal

Mechanistic insights into rubidium ion adsorption at the quartz (101) surface from quantum chemical metadynamics

Ion sorption extent and mechanism depend in part on the mineral surface termination, which can be highly complex. Variations in surface termination, particularly with defect density and surface roughness, influence mineral reactivity towards solutes. In this work, we investigate the adsorption of a rubidium cation at pristine and defect quartz (101) surface sites using wel…
Apr, 2026

Journal

Density functional theory-based surrogate kinetic models for heterogeneous reactions of hydrocarbon intermediates on silicon carbide

The increasing demand for high-performance materials in advanced technologies highlights the importance of achieving a fundamental understanding and potential control of silicon carbide (SiC) deposition processes. However, existing models often lack sufficient theoretical detail, relying heavily on empirical data and offering limited predictive capability. In particular, t…
Mar, 2026

Conference Paper

Scaling Ensembles of Data-Intensive Quantum Chemical Calculations for Millions of Molecules

Deep learning models are efficient computational tools that can accelerate the inverse design of molecules with desired functional properties by generating predictions at a fraction of the time required by traditional quantum chemical approaches. To ensure that a model maintains accuracy and transferability across broad regions of the chemical space explored during the inv…
Sep, 2025

Journal

Pressure-driven density match nucleates metastable r8 phases from amorphous Si and Ge

The pressure–temperature phase behavior of covalent disordered solids such as amorphous silicon and germanium is complex. Questions remain on possible glass transitions, on polyamorphism via amorphous–amorphous transitions, on connections with liquid–liquid transitions, on structure-behavior relationships, and on their potential as precursor for novel methods for material…
Aug, 2025

Journal

Acidities of MgO surface sites: implications for the formation mechanism of Mg(OH)2

The hydroxylation of periclase (MgO) to brucite (Mg(OH)2) is thought to be an important intermediate step when using MgO to capture CO2 from the atmosphere. However, the mechanism of hydroxylation of MgO to form Mg(OH)2 is poorly understood. In this work, we used atomic-scale density functional tight binding simulations coupled with the metadynamics rare event method to an…
Jul, 2025

Journal

Recent Developments in DFTB+, a Software Package for Efficient Atomistic Quantum Mechanical Simulations

DFTB+ is a flexible, open-source software package developed by its community, designed for fast and efficient atomistic quantum mechanical simulations. It employs various methods that approximate density functional theory (DFT), such as density functional-based tight binding (DFTB) and the extended tight binding (xTB) approach allowing simulations of large systems over ext…
Jun, 2025

Journal

Inverse mapping of properties to composition through generative modeling for designing molten salts

Generative modeling (GM) has been increasingly used for the inverse design and optimization of materials, yet its application to molten salt mixtures remains unexplored despite how a successful approach to the inverse design of molten salts would contribute to efficiently exploiting their customizability and unlocking their advantages in applications, such as energy produc…
Apr, 2025

Journal

Collection: TD-DFT and EOM-CCSD Calculations for the GDB-9-Ex Dataset

We present two datasets that contain quantum chemical electronic structure calculations for organic molecules from the GDB-9-Ex dataset. The “GDB-9-Ex_TD-DFT-PBE0” dataset contains calculations performed using the time-dependent density functional theory (TD-DFT) first principles method, and the “GDB-9-Ex_EOMCCSD” dataset contains calculations performed using the equation-…
Mar, 2025

Journal

Evaluation of Density-Functional Tight-Binding Methods for Simulation of Protic Molecular Ion Pairs

In this work, we benchmark the accuracy of the density-functional tight-binding (DFTB) method, namely the long-range corrected second-order (LC-DFTB2) and third-order (DFTB3) models, for predicting energetics of imidazolium-based ionic liquid (IL) ion pairs. We compare the DFTB models against popular density functionals such as LC-ωPBE and B3LYP, using ab initio domain-bas…
Dec, 2024

Journal

Molecular Origin of Viscoelasticity and Influence of Methylation in Mesophase Pitch

The viscoelastic and thermomechanical properties of pitches are responsible for their melt-spinning behavior, which is a critical step for manufacturing high-performance pitch-based carbon fibers. Here, we systematically explore the impact of methyl group modifications on the viscoelastic and thermal properties of mesophase pitches. We employ a range of atomistic modeling…
Nov, 2024

Journal

Variation in Cation Adsorption Mechanism Controlled by Chemical and Structural Heterogeneities at the Quartz (101)–Water Interface

Mineral–water interfacial reactions are central to chemical processes that control the fate of nutrients and contaminants in natural environments. Mineral surfaces commonly have complex structures and compositions whose impact on interfacial reactivity is poorly understood. Here, we investigated the effects of surface heterogeneities on Rb+ sorption at the quartz (101)–10…

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Publications

Mechanistic insights into rubidium ion adsorption at the quartz (101) surface from quantum chemical metadynamics

Mechanistic insights into rubidium ion adsorption at the quartz (101) surface from quantum chemical metadynamics

Density functional theory-based surrogate kinetic models for heterogeneous reactions of hydrocarbon intermediates on silicon carbide

Scaling Ensembles of Data-Intensive Quantum Chemical Calculations for Millions of Molecules

Pressure-driven density match nucleates metastable r8 phases from amorphous Si and Ge

Acidities of MgO surface sites: implications for the formation mechanism of Mg(OH)2

Recent Developments in DFTB+, a Software Package for Efficient Atomistic Quantum Mechanical Simulations

Inverse mapping of properties to composition through generative modeling for designing molten salts

Collection: TD-DFT and EOM-CCSD Calculations for the GDB-9-Ex Dataset

Evaluation of Density-Functional Tight-Binding Methods for Simulation of Protic Molecular Ion Pairs

Molecular Origin of Viscoelasticity and Influence of Methylation in Mesophase Pitch

Variation in Cation Adsorption Mechanism Controlled by Chemical and Structural Heterogeneities at the Quartz (101)–Water Interface