Publications associées à Development of Accurate and Efficient Electronic Structure Approaches for the Description of Organic Systems

Encoding quantum-chemical knowledge into machine-learning models of complex molecular properties

Statistical (machine-learning, ML) models are more and more often used in computational chemistry as a substitute to more expensive ab initio and parametrizable methods. While the ML algorithms are capable of learning physical laws implicitly from data, ad ...

EPFL2024

Efficient and insightful descriptors for representing molecular and material space

Alexander Jan Goscinski

Data-driven approaches have been applied to reduce the cost of accurate computational studies on materials, by using only a small number of expensive reference electronic structure calculations for a representative subset of the materials space, and using ...

EPFL2024

Novel Alkynylation Methods through the Combination of Hypervalent Iodine Reagents and Alkynyl-trifluoroborate Salts

Julien Aymeric Borrel

The alkyne motif is a versatile functional group often encountered in organic chemistry. It can be involved in various transformations such as the alkyne-azide cycloaddition and has found widespread application in medicinal chemistry, chemical biology and ...

EPFL2024

Molecular hypergraph neural networks

Philippe Schwaller, Junwu Chen

Graph neural networks (GNNs) have demonstrated promising performance across various chemistry-related tasks. However, conventional graphs only model the pairwise connectivity in molecules, failing to adequately represent higher order connections, such as m ...

Aip Publishing2024

Structure and dynamics of liquid water from ab initio simulations: adding Minnesota density functionals to Jacob's ladder

Ursula Röthlisberger, Justin Villard, Martin Peter Bircher

The accurate representation of the structural and dynamical properties of water is essential for simulating the unique behavior of this ubiquitous solvent. Here we assess the current status of describing liquid water using ab initio molecular dynamics, wit ...

Royal Soc Chemistry2024

Excited State-Specific CASSCF Theory for the Torsion of Ethylene

State-specific complete active space self-consistent field (SS-CASSCF) theory has emerged as a promising route to accurately predict electronically excited energy surfaces away from molecular equilibria. However, its accuracy and practicality for chemical ...

Amer Chemical Soc2024

Orbital-Resolved DFT plus U for Molecules and Solids

Nicola Marzari, Iurii Timrov, Eric Macke

We present an orbital-resolved extension of the Hubbard U correction to density-functional theory (DFT). Compared to the conventional shell-averaged approach, the prediction of energetic, electronic and structural properties is strongly improved, particula ...

Amer Chemical Soc2024

Shortwave Infrared-Sensitive, Narrowband Organic Upconversion Devices with a Gain

Wei-Hsu Hu

Sensing and imaging of light in the shortwave infrared (SWIR) range is increasingly used in various fields, including bio-imaging, remote sensing, and semiconductor process control. SWIR-sensitive organic photodetectors (OPDs) are promising because organic ...

EPFL2024

Plasmonic Nanostructures for Photocatalysis: Material, Photonic and Electronic Effects

Fateme Kiani Shahvandi

Plasmonic photochemistry has a large potential to replace energy-intensive chemical processes with low-temperature, low-pressure light-driven chemical reactions. Plasmonic nanostructures have emerged as promising photocatalysts with exceptional and tunable ...

EPFL2024

Exciton migration in two-dimensional materials

Excitons play an essential role in the optical response of two-dimensional materials. These are bound states showing up in the band gaps of many-body systems and are conceived as quasiparticles formed by an electron and a hole. By performing real-time simu ...

Nature Portfolio2024

Charge-Transfer States in Organic Nanowires

Lucile Annie Chassat

Charge separation processes in organic semiconductors play a pivotal role in diverse applications ranging from photovoltaics to photocatalysis. Understanding these mechanisms, particularly the role of hybrid charge-transfer (CT) states, is essential for ad ...

EPFL2024

Computational Studies on the Stability of Organic-Inorganic Hybrid Halide Lead Perovskites

Mathias Dankl

Perovskite-based solar cells are currently the most rapidly advancing photovoltaic technology but concerns about their long-term stability are still impeding full-scale commercialization. This thesis provides computational insights into some of the stabili ...

EPFL2024

Thermal transport of glasses via machine learning driven simulations

Federico Grasselli

Accessing the thermal transport properties of glasses is a major issue for the design of production strategies of glass industry, as well as for the plethora of applications and devices where glasses are employed. From the computational standpoint, the che ...

Frontiers Media Sa2024

Controlling On-Surface Photoactivity: The Impact of π-Conjugation in Anhydride-Functionalized Molecules on a Semiconductor Surface

Karl-Heinz Ernst, Christian Wäckerlin

On-surface synthesis has become a prominent method for growing low-dimensional carbon-based nanomaterials on metal surfaces. However, the necessity of decoupling organic nanostructures from metal substrates to exploit their properties requires either trans ...

Wiley-VCH Verlag GmbH2024

Electronic transport in graphene with out-of-plane disorder

Oleg Yazyev, Yifei Guan

Real-world samples of graphene often exhibit various types of out-of-plane disorder-ripples, wrinkles and folds-introduced at the stage of growth and transfer processes. These complex out-of-plane defects resulting from the interplay between self-adhesion ...

Nature Portfolio2024

Seebeck Coefficient of Ionic Conductors from Bayesian Regression Analysis

We propose a novel approach to evaluating the ionic Seebeck coefficient in electrolytes from relatively short equilibrium molecular dynamics simulations, based on the Green-Kubo theory of linear response and Bayesian regression analysis. By exploiting the ...

Amer Chemical Soc2024

Nonempirical semilocal density functionals for correcting the self-interaction of polaronic states

Alfredo Pasquarello, Stefano Falletta

Through the use of the piecewise-linearity condition of the total energy, we correct the self-interaction for the study of polarons by constructing nonempirical functionals at the semilocal level of theory. We consider two functionals, the gamma DFT and mu ...

Aip Publishing2024

Large-cage occupation and quantum dynamics of hydrogen molecules in sII clathrate hydrates

Richard Gaal, Livia Eleonora Bove Kado, Umbertoluca Ranieri

Hydrogen clathrate hydrates are ice-like crystalline substances in which hydrogen molecules are trapped inside polyhedral cages formed by the water molecules. Small cages can host only a single H-2 molecule, while each large cage can be occupied by up to f ...

Aip Publishing2024

Solvation Free Energies from Machine Learning Molecular Dynamics

Nicola Marzari, Nicéphore Arthur François Bonnet

The present work proposes an extension to the approach of [Xi, C; et al. J. Chem. Theory Comput. 2022, 18, 6878] to calculate ion solvation free energies from first-principles (FP) molecular dynamics (MD) simulations of a hybrid solvation model. The approa ...

Amer Chemical Soc2024

Assessing the Charge Carrier Dynamics at Hybrid Interfaces of Organic Photoanodes for Solar Fuels

Kevin Sivula, Yongpeng Liu, Han-Hee Cho, Alexander Wieczorek

Organic semiconductors (OSCs) have emerged as promising active layers for photoanodes to drive photoelectrochemical (PEC) oxidation reactions. Interfacing an OSC with an inorganic electron transport layer (ETL) is key to enabling both high performance and ...

Amer Chemical Soc2024