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Density functional theory (DFT) based modeling of electronic excited states is of importance for investigation of the photophysical/photochemical properties and spectroscopic characterization of large systems. The widely used linear…

Chemical Physics · Physics 2021-05-11 Diptarka Hait , Martin Head-Gordon

Ultrafast electronic dynamics in solids lies at the core of modern condensed matter and materials physics. To build up a practical ab initio method for studying solids under photoexcitation, we develop a momentum-resolved real-time time…

Materials Science · Physics 2018-10-17 Chao Lian , Shi-Qi Hu , Meng-Xue Guan , Sheng Meng

In recent times, the use of machine learning in materials design and discovery has aided to accelerate the discovery of innovative materials with extraordinary properties, which otherwise would have been driven by a laborious and…

Materials Science · Physics 2024-08-01 Md Mohaiminul Islam

This paper proposes a machine learning (ML) method to predict stable molecular geometries from their chemical composition. The method is useful for generating molecular conformations which may serve as initial geometries for saving time…

We introduce DeepDFT, a deep learning model for predicting the electronic charge density around atoms, the fundamental variable in electronic structure simulations from which all ground state properties can be calculated. The model is…

Computational Physics · Physics 2020-11-09 Peter Bjørn Jørgensen , Arghya Bhowmik

The primary computational challenge when simulating nonadiabatic ab initio molecular dynamics is the unfavorable compute costs of electronic structure calculations with molecular size. Simple electronic structure theories, like…

Chemical Physics · Physics 2023-06-28 Justin J. Talbot , Martin Head-Gordon , Stephen J. Cotton

To date, density functional theory (DFT) is one of the most accurate and yet practical theory to gain insight about materials properties. Although successful, the computational cost is the main hurdle even today. A way out is combining DFT…

Materials Science · Physics 2019-04-19 Shweta Mehta , Sheena Agarwal , Kavita Joshi

The predictive performance screening of novel compounds can significantly promote the discovery of efficient, cheap, and non-toxic thermoelectric materials. Large efforts to implement machine-learning techniques coupled to materials…

Applied Physics · Physics 2020-12-07 Patrizio Graziosi , Chathurangi Kumarasinghe , Neophytos Neophytou

We present an implementation of time-dependent density-functional theory (TDDFT) in the linear response formalism enabling the calculation of low energy optical absorption spectra for large molecules and nanostructures. The method avoids…

This chapter provides a basic introduction to excited-state extensions of density functional theory (DFT), including time-dependent (TD-)DFT in both its linear-response and its explicitly time-dependent formulations. As applied to the…

Chemical Physics · Physics 2023-05-02 John M. Herbert

Machine learning (ML) can be used to construct surrogate models for the fast prediction of a property of interest. ML can thus be applied to chemical projects, where the usual experimentation or calculation techniques can take hours or days…

Machine Learning (ML) approximations to Density Functional Theory (DFT) potential energy surfaces (PESs) are showing great promise for reducing the computational cost of accurate molecular simulations, but at present they are not applicable…

Chemical Physics · Physics 2020-03-05 Xiaowei Xie , Kristin A. Persson , David W. Small

We review different computational methods for the calculation of photoelectron spectra and angular distributions of atoms and molecules when excited by laser pulses using time-dependent density-functional theory (TDDFT) that are suitable…

Chemical Physics · Physics 2017-03-28 Philipp Wopperer , Umberto De Giovannini , Angel Rubio

Machine learning is rapidly accelerating materials and chemical discovery, but most current models target energies, forces, or selected molecular properties rather than the underlying many-body electronic structure. Learning…

Photoactive iridium complexes are of broad interest due to their applications ranging from lighting to photocatalysis. However, the excited state property prediction of these complexes challenges ab initio methods such as time-dependent…

Chemical Physics · Physics 2022-09-20 Gianmarco Terrones , Chenru Duan , Aditya Nandy , Heather J. Kulik

Computational screening for new and improved catalyst materials relies on accurate and low-cost predictions of key parameters such as adsorption energies. Here, we use recently developed compressed sensing methods to identify descriptors…

Materials Science · Physics 2019-02-21 Mie Andersen , Sergey V. Levchenko , Matthias Scheffler , Karsten Reuter

A mixed quantum-classical approach to simulate the coupled dynamics of electrons and nuclei in nanoscale molecular systems is presented. The method relies on a second order expansion of the Lagrangian in time-dependent density functional…

Chemical Physics · Physics 2009-11-10 T. A. Niehaus , D. Heringer , B. Torralva , Th. Frauenheim

Obtaining the exciton dynamics of large photosynthetic complexes by using mixed quantum mechanics/molecular mechanics (QM/MM) is computationally demanding. We propose a machine learning technique, multi-layer perceptrons, as a tool to…

Chemical Physics · Physics 2016-06-01 Florian Häse , Stéphanie Valleau , Edward Pyzer-Knapp , Alán Aspuru-Guzik

We investigate the time an electronic excitation travels in a supermolecular setup using a measurement process in an open quantum-system framework. The approach is based on the stochastic Schr\"odinger equation and uses a Hamiltonian from…

Materials Science · Physics 2013-12-09 Dirk Hofmann , Heiko Appel , Massimiliano Di Ventra , Stephan Kümmel

Molecular-level understanding of the interactions between the constituents of an atomic structure is essential for designing novel materials in various applications. This need goes beyond the basic knowledge of the number and types of…