Publications related to The Charge Transfer Problem in Density Functional Theory Calculations of Aqueously Solvated Molecules

Advancing Computational Chemistry with Stochastic and Artificial Intelligence Approaches

Computational chemistry aims to simulate reactions and molecular properties at the atomic scale, advancing the design of novel compounds and materials with economic, environmental, and societal implications. However, the field relies on approximate quantum ...

EPFL2023

Towards high-throughput many-body perturbation theory: efficient algorithms and automated workflows

Giovanni Pizzi, Antimo Marrazzo, Miki Bonacci, Junfeng Qiao, Andrea Ferretti

The automation of ab initio simulations is essential in view of performing high-throughput (HT) computational screenings oriented to the discovery of novel materials with desired physical properties. In this work, we propose algorithms and implementations ...

NATURE PORTFOLIO2023

Machine-learning the electronic density of states: electronic properties without quantum mechanics

Chiheb Ben Mahmoud

The electronic density of states (DOS) quantifies the distribution of the energy levels that can be occupied by electrons in a quasiparticle picture and is central to modern electronic structure theory. It also underpins the computation and interpretation ...

EPFL2023

Advancing first principle-based molecular dynamics of biological systems with machine learning

François Louis Mouvet

Molecular dynamics (MD) simulations have emerged as a transformative approach to analyse molecular systems at the atomic level, offering valuable insights into complex biological processes. Many biological phenomena can only accurately be described by inco ...

EPFL2023

Computational Studies for the Design of Metalloenzyme Mimics

Guido Frisari

At present, there is no general standard automated method for engineering metalloenzymes, industrially-relevant systems able to catalyze environmentally friendly reactions. One of the most studied natural metalloenzymes is the second isoform of human carbo ...

EPFL2023

Assessing the persistence of chalcogen bonds in solution with neural network potentials

Anne-Clémence Corminboeuf, Veronika Juraskova, Rubén Laplaza Solanas, Frédéric Célerse

Non-covalent bonding patterns are commonly harvested as a design principle in the field of catalysis, supramolecular chemistry, and functional materials to name a few. Yet, their computational description generally neglects finite temperature and environme ...

2022

Microscopic picture of paraelectric perovskites from structural prototypes

Nicola Marzari, Giovanni Pizzi, Boris Kozinsky, Michele Kotiuga

We highlight with first-principles molecular dynamics the persistence of intrinsic < 111 > Ti off-centerings for BaTiO3 in its cubic paraelectric phase. Intriguingly, these are inconsistent with the Pm (3) over barm space group often used to atomistically ...

AMER PHYSICAL SOC2022

Molecular dynamics simulations of the evaporation of hydrated ions from aqueous solution

Philip Robin Loche

Although important for atmospheric processes and gas-phase catalysis, very little is known about the hydration state of ions in the vapor phase. Here we study the evaporation energetics and kinetics of a chloride ion from liquid water by molecular dynamics ...

NATURE PORTFOLIO2022

Azole-Based Indoleamine 2,3-Dioxygenase 1 (IDO1) Inhibitors

Pierre Vogel, Olivier Michielin, Florence Pojer, Somi Reddy Majjigapu, George Coukos

The heme enzyme indoleamine 2,3-dioxygenase 1 (IDO1) plays an essential role in immunity, neuronal function, and aging through catalysis of the rate-limiting step in the kynurenine pathway of tryptophan metabolism. Many IDO1 inhibitors with different chemo ...

AMER CHEMICAL SOC2021

Ab Initio Electron-Phonon Interactions in Correlated Electron Systems

Nicola Marzari, Matteo Cococcioni, Iurii Timrov, Andrea Floris

Electron-phonon (e-ph) interactions are pervasive in condensed matter, governing phenomena such as transport, superconductivity, charge-density waves, polarons, and metal-insulator transitions. First-principles approaches enable accurate calculations of e- ...

AMER PHYSICAL SOC2021

Coherent energy exchange between carriers and phonons in Peierls-distorted bismuth unveiled by broadband XUV pulses

Iurii Timrov

In Peierls-distorted materials, photoexcitation leads to a strongly coupled transient response between structural and electronic degrees of freedom, always measured independently of each other. Here we use transient reflectivity in the extreme ultraviolet ...

AMER PHYSICAL SOC2021

Catalyzing Bond-Dissociation in Graphene via Alkali-Iodide Molecules

Klaus Kern, Stephan Rauschenbach, Sabine Abb, Sven Alexander Szilagyi, Hannah Julia Ochner

Atomic design of a 2D-material such as graphene can be substantially influenced by etching, deliberately induced in a transmission electron microscope. It is achieved primarily by overcoming the threshold energy for defect formation by controlling the kine ...

WILEY-V C H VERLAG GMBH2021

The ONETEP linear-scaling density functional theory program

Edward Baxter Linscott

We present an overview of the onetep program for linear-scaling density functional theory (DFT) calculations with large basis set (plane-wave) accuracy on parallel computers. The DFT energy is computed from the density matrix, which is constructed from spa ...

AMER INST PHYSICS2020

Deterministic and Statistical Approaches to Quantum Chemistry

Alberto Fabrizio

The field of quantum chemistry has recently undergone a series of paradigm shifts, including a boom in machine learning applications that target the electronic structure problem. Along with these technological innovations, the community continues to identi ...

EPFL2020

Learning the electronic density of states in condensed matter

Michele Ceriotti, Andrea Anelli, Chiheb Ben Mahmoud

The electronic density of states (DOS) quantifies the distribution of the energy levels that can be occupied by electrons in a quasiparticle picture and is central to modern electronic structure theory. It also underpins the computation and interpretation ...

AMER PHYSICAL SOC2020

Prediction of aqueous free energies of solvation using coupled QM and MM explicit solvent simulations

Jeremy Samuel Arey, Daniel David Sadowsky

A method based on molecular dynamics simulations which employ two distinct levels of theory is proposed and tested for the prediction of Gibbs free energies of solvation for non-ionic solutes in water. The method consists of two additive contributions: (i) ...

ROYAL SOC CHEMISTRY2020

Formamidinium-Based Dion-Jacobson Layered Hybrid Perovskites: Structural Complexity and Optoelectronic Properties

Michael Graetzel, Shaik Mohammed Zakeeruddin, Ursula Röthlisberger, Ulf Anders Hagfeldt, Amita Ummadisingu, Mohammad Ibrahim Dar, Marko Mladenovic, Wolfgang Richard Tress, Farzaneh Jahanbakhshi, Paramvir Ahlawat, Brian Irving Carlsen, Yang Li, Jovana Milic, Yang Li, Algirdas Ducinskas

Layered hybrid perovskites have emerged as a promising alternative to stabilizing hybrid organic-inorganic perovskite materials, which are predominantly based on Ruddlesden-Popper structures. Formamidinium (FA)-based Dion-Jacobson perovskite analogs are de ...

2020

Multihole water oxidation catalysis on haematite photoanodes revealed by operando spectroelectrochemistry and DFT

Michael Graetzel, Matthew Thomas Mayer, Yimeng Ma

Water oxidation is the key kinetic bottleneck of photoelectrochemical devices for fuel synthesis. Despite advances in the identification of intermediates, elucidating the catalytic mechanism of this multi-redox reaction on metal-oxide photoanodes remains a ...

NATURE PUBLISHING GROUP2020

ONETEP plus TOSCAM: Uniting Dynamical Mean Field Theory and Linear-Scaling Density Functional Theory

Cédric Weber, Edward Baxter Linscott

We introduce the unification of dynamical mean field theory (DMFT) and linear-scaling density functional theory (DFT), as recently implemented in ONETEP, a linear-scaling DFT package, and TOSCAM, a DMFT toolbox. This code can account for strongly correlate ...

2020

High-throughput computational screening for solid-state Li-ion conductors

Nicola Marzari, Leonid Kahle, Aris Marcolongo

We present a computational screening of experimental structural repositories for fast Li-ion conductors, with the goal of finding new candidate materials for application as solid-state electrolytes in next-generation batteries. We start from similar to 140 ...

ROYAL SOC CHEMISTRY2020