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The excited state dynamics of chromophores in complex environments determine a range of vital biological and energy capture processes. Time-resolved, multidimensional optical spectroscopies provide a key tool to investigate these processes.…

Artificial neural networks have been recently introduced as a general ansatz to compactly represent many- body wave functions. In conjunction with Variational Monte Carlo, this ansatz has been applied to find Hamil- tonian ground states and…

Strongly Correlated Electrons · Physics 2018-10-24 Kenny Choo , Giuseppe Carleo , Nicolas Regnault , Titus Neupert

Computing excited-state properties of molecules and solids is considered one of the most important near-term applications of quantum computers. While many of the current excited-state quantum algorithms differ in circuit architecture,…

Quantum Physics · Physics 2024-03-19 Carlos L. Benavides-Riveros , Yuchen Wang , Samuel Warren , David A. Mazziotti

Reactive chemistry of molecular hydrogen at surfaces, notably dissociative sticking and hydrogen evolution, plays a crucial role in energy storage and fuel cells. Theoretical studies can help to decipher underlying mechanisms and reaction…

We present a machine learning (ML) framework for predicting Green's functions of molecular systems, from which photoemission spectra and quasiparticle energies at quantum many-body level can be obtained. Kernel ridge regression is adopted…

Chemical Physics · Physics 2023-12-05 Christian Venturella , Christopher Hillenbrand , Jiachen Li , Tianyu Zhu

We demonstrate a machine learning based approach which can learn the time-dependent electronic excitation dynamics of small molecules subjected to ion irradiation. Ensembles of recurrent neural networks are trained on data generated by…

Chemical Physics · Physics 2024-09-24 Ethan P. Shapera , Cheng-Wei Lee

Conical intersections serve as critical gateways in photochemical reactions, enabling rapid nonradiative transitions between potential energy surfaces that underpin fundamental processes such as photosynthesis or vision. Their calculation…

Chemical Physics · Physics 2025-02-19 Rhyan Barrett , Christoph Ortner , Julia Westermayr

In this study, we explore the potential of machine learning for modeling molecular electronic spectral intensities as a continuous function in a given wavelength range. Since presently available chemical space datasets provide excitation…

Chemical Physics · Physics 2022-08-02 Prakriti Kayastha , Sabyasachi Chakraborty , Raghunathan Ramakrishnan

Two-dimensional electronic spectroscopy (2DES) provides rich information about how the electronic states of molecules, proteins, and solid-state materials interact with each other and their surrounding environment. Atomistic molecular…

Photophysical and photochemical processes are ruled by the interplay between transient vibrational and electronic degrees of freedom, which are ultimately determined by the multidimensional potential energy surfaces (PESs). Differences…

The computation of excited electronic states is an important application for quantum computers. In this work, we simulate the excited state spectra of four aromatic heterocycles on IBM superconducting quantum computers, focusing on active…

Quantum Physics · Physics 2023-09-19 Maria A. Castellanos , Mario Motta , Julia E. Rice

This paper describes a method to do ab initio molecular dynamics in electronically excited systems within the random phase approximation (RPA). Using a dynamical variational treatment of the RPA frequency, which corresponds to the…

Condensed Matter · Physics 2009-10-31 Eric R. Bittner , D. S. Kosov

Equations of State model relations between thermodynamic variables and are ubiquitous in scientific modelling, appearing in modern day applications ranging from Astrophysics to Climate Science. The three desired properties of a general…

Variational calculations of excited electronic states are carried out by finding saddle points on the surface that describes how the energy of the system varies as a function of the electronic degrees of freedom. This approach has several…

Chemical Physics · Physics 2023-02-15 Yorick L. A. Schmerwitz , Gianluca Levi , Hannes Jónsson

We present a variational Monte Carlo algorithm for estimating the lowest excited states of a quantum system which is a natural generalization of the estimation of ground states. The method has no free parameters and requires no explicit…

Computational Physics · Physics 2024-09-04 David Pfau , Simon Axelrod , Halvard Sutterud , Ingrid von Glehn , James S. Spencer

Computing dynamical distributions in quantum many-body systems represents one of the paradigmatic open problems in theoretical condensed matter physics. Despite the existence of different techniques both in real-time and frequency space,…

Disordered Systems and Neural Networks · Physics 2021-08-04 Rouven Koch , Jose L. Lado

The in silico exploration of chemical, physical and biological systems requires accurate and efficient energy functions to follow their nuclear dynamics at a molecular and atomistic level. Recently, machine learning tools gained a lot of…

Chemical Physics · Physics 2020-08-26 Silvan Käser , Oliver T. Unke , Markus Meuwly

Recurrent neural networks are machine learning algorithms which are suited well to predict time series. Echo state networks are one specific implementation of such neural networks that can describe the evolution of dynamical systems by…

Fluid Dynamics · Physics 2021-05-26 Florian Heyder , Jörg Schumacher

Intelligent biological systems are characterized by their embodiment in a complex environment and the intimate interplay between their nervous systems and the nonlinear mechanical properties of their bodies. This coordination, in which the…

Machine Learning · Computer Science 2023-02-02 Deniz Oktay , Mehran Mirramezani , Eder Medina , Ryan P. Adams

Utilizing quantum computer to investigate quantum chemistry is an important research field nowadays. In addition to the ground-state problems that have been widely studied, the determination of excited-states plays a crucial role in the…