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Linear and nonlinear electronic spectra provide an important tool to probe the absorption and transfer of electronic energy. Here we introduce a pure state Ehrenfest approach to obtain accurate linear and nonlinear spectra that is…

Chemical Physics · Physics 2022-12-15 Austin O. Atsango , Andrés Montoya-Castillo , Thomas E. Markland

Molecular absorption and photo-electron spectra can be efficiently predicted with real-time time-dependent density-functional theory (TDDFT). We show here how these techniques can be easily extended to study time-resolved pump-probe…

Atomic and Molecular Clusters · Physics 2013-01-10 Umberto De Giovannini , Gustavo Brunetto , Alberto Castro , Jessica Walkenhorst , Angel Rubio

Two-dimensional electronic spectroscopy has become one of the main experimental tools for analyzing the dynamics of excitonic energy transfer in large molecular complexes. Simplified theoretical models are usually employed to extract model…

Chemical Physics · Physics 2019-01-17 Mirta Rodríguez , Tobias Kramer

The bispectrum is the leading non-Gaussian statistic in large-scale structure, carrying valuable information on cosmology that is complementary to the power spectrum. To access this information, we need to model the bispectrum in the weakly…

Cosmology and Nongalactic Astrophysics · Physics 2022-01-12 Tobias Baldauf , Mathias Garny , Petter Taule , Theo Steele

We present an efficient perturbative method to obtain both static and dynamic polarizabilities and hyperpolarizabilities of complex electronic systems. This approach is based on the solution of a frequency dependent Sternheimer equation,…

Materials Science · Physics 2009-11-13 Xavier Andrade , Silvana Botti , Miguel A. L. Marques , Angel Rubio

Due to its favorable computational efficiency time-dependent (TD) density functional theory (DFT) enables the prediction of electronic spectra in a high-throughput manner across chemical space. Its predictions, however, can be quite…

Spectroscopy is an indispensable tool in understanding the structures and dynamics of molecular systems. However computational modelling of spectroscopy is challenging due to the exponential scaling of computational complexity with system…

Quantum Physics · Physics 2021-06-22 Chee-Kong Lee , Chang-Yu Hsieh , Shengyu Zhang , Liang Shi

We present a computationally efficient method to incorporate density-functional theory into the calculation of reflectivity in low-energy electron microscopy. The reflectivity is determined by matching plane waves representing the electron…

Materials Science · Physics 2013-11-13 John F. McClain , Jiebing Sun , Karsten Pohl , Jian-Ming Tang

In this work we propose an efficient and accurate multi-scale optical simulation algorithm by applying a numerical version of slowly varying envelope approximation in FEM. Specifically, we employ the fast iterative method to quickly compute…

Optics · Physics 2024-12-03 Fan Xiao , Jingwei Wang , Zhongfei Xiong , Yuntian Chen

To leverage the redundancy between the electronic structure computed at each step of first-principles molecular dynamics, we present a data-driven modeling framework for Kohn-Sham Density Functional Theory that bypasses the explicit…

Numerical Analysis · Mathematics 2026-02-27 Siu Wun Cheung , Youngsoo Choi , Jean-Luc Fattebert , Jonas Kaufman , Daniel Osei-Kuffuor

Real-time time-dependent density functional theory, in conjunction with the Ehrenfest molecular dynamics scheme, is becoming a popular methodology to investigate ultrafast phenomena on the nanoscale. Thanks to recent developments, it is…

Materials Science · Physics 2020-08-18 Jannis Krumland , Ana M. Valencia , Stefano Pittalis , Carlo A. Rozzi , Caterina Cocchi

This article is an introduction to a new approach to first principles electronic structure calculation. The starting point is the Hartree-Fock-Roothaan equation, in which molecular integrals are approximated by polynomials by way of Taylor…

Computational Physics · Physics 2019-07-18 Akihito Kikuchi

Recent theoretical studies in quantum spectroscopy have emphasized the potential of non-classical correlations in entangled photon pairs for selectively targeting specific nonlinear optical processes in nonlinear optical responses. However,…

Chemical Physics · Physics 2026-04-21 Yuta Fujihashi , Ozora Iso , Ryosuke Shimizu , Akihito Ishizaki

Accurate and efficient calculations of absorption spectra of molecules and materials are essential for the understanding and rational design of broad classes of systems. Solving the Bethe-Salpeter equation (BSE) for electron-hole pairs…

Materials Science · Physics 2021-02-18 Sijia S. Dong , Marco Govoni , Giulia Galli

We present a review of the basic ideas and techniques of the spectral density functional theory which are currently used in electronic structure calculations of strongly-correlated materials where the one-electron description breaks down.…

Strongly Correlated Electrons · Physics 2009-11-11 G. Kotliar , S. Y. Savrasov , K. Haule , V. S. Oudovenko , O. Parcollet , C. A. Marianetti

Electronic coherences can be leveraged to control molecular dynamics, but such control is limited by ultrafast decoherence driven by coupling between electronic excitations and molecular vibrations. With the goal of understanding and…

Chemical Physics · Physics 2025-05-27 Jiří Suchan , Benjamin G. Levine

Time-resolved spectroscopy is an important tool for unraveling the minute details of structural changes of molecules of biological and technological significance. The nonlinear femtosecond signals detected for such systems must be…

Chemical Physics · Physics 2024-01-17 Sebastian V. Pios , Maxim F. Gelin , Arif Ullah , Pavlo O. Dral , Lipeng Chen

We present a new computation method for simulating reflection high-energy electron diffraction and the total-reflection high-energy positron diffraction experiments. The two experiments are used commonly for the structural analysis of…

Numerical Analysis · Mathematics 2023-06-02 Shuhei Kudo , Yusaku Yamamoto , Takeo Hoshi

Spectral functions are central to link experimental probes to theoretical models in condensed matter physics. However, performing exact numerical calculations for interacting quantum matter has remained a key challenge especially beyond one…

Strongly Correlated Electrons · Physics 2023-08-03 Tiago Mendes-Santos , Markus Schmitt , Markus Heyl

Energy spectroscopy is a powerful tool with diverse applications across various disciplines. The advent of programmable digital quantum simulators opens new possibilities for conducting spectroscopy on various models using a single device.…