Related papers: Simulating Vibronic Spectra without Born-Oppenheim…
Methods for reconstructing the spectral density of a vibrational environment from experimental data can yield key insights into the impact of the environment on molecular function. Although such experimental methods exist, they generally…
We present a theory of electronic excitation energies and optical absorption spectra which incorporates energy-level renormalization and phonon-assisted optical absorption within a unified framework. Using time-independent perturbation…
A pseudo-spectral method with an absorbing outer boundary is used to solve a set of the time-dependent force-free equations. In the method, both electric and magnetic fields are expanded in terms of the vector spherical harmonic (VSH)…
A time-dependent vibrational electronic coupled-cluster (VECC) approach is proposed to simulate photoelectron/ UV-VIS absorption spectra, as well as time-dependent properties for non-adiabatic vibronic models, going beyond the…
We present a general computational scheme based on molecular dynamics (m.d.) simulation for calculating the chemical potential of adsorbed molecules in thermal equilibrium on the surface of a material. The scheme is based on the calculation…
The absorption spectrum of CO$_2$ in the wavelength range 120\,nm --- 160\,nm is analyzed by means of quantum mechanical calculations performed using vibronically coupled PESs of five singlet valence electronic states and the coordinate…
Simulating vibronic spectra is a central task in physical chemistry, offering insight into important properties of molecules. Recently, it has been experimentally demonstrated that photonic platforms based on Gaussian boson sampling (GBS)…
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…
Born-Oppenheimer dynamics is shown to provide an accurate approximation of time-independent Schr\"odinger observables for a molecular system with an electron spectral gap, in the limit of large ratio of nuclei and electron masses, without…
We analytically tackle opto-vibronic interactions in molecular systems driven by either classical or quantum light fields. In particular, we examine a simple model of molecules with two relevant electronic levels, characterized by potential…
Quantum simulation experiments have started to explore regimes that are not accessible with exact numerical methods. In order to probe these systems and enable new physical insights, the need for measurement protocols arises that can bridge…
Quantum computing has the potential to reduce the computational cost required for quantum dynamics simulations. However, existing quantum algorithms for coupled electron-nuclear dynamics simulation either require fault-tolerant devices, or…
We formulate a time-dependent density functional theory for the coupled dynamics of electrons and nuclei that goes beyond the Born-Oppenheimer (BO) approximation. We prove that the time-dependent marginal nuclear probability density…
An accurate treatment of electronic spectra in large systems with a technique such as time dependent density functional theory (TDDFT) is computationally challenging. Due to the Nyquist sampling theorem, direct real time simulations must be…
With the continuous growth of processing power for scientific computing, first principles Born-Oppenheimer molecular dynamics (MD) simulations are becoming increasingly popular for the study of a wide range of problems in materials science,…
We introduce a heterodimer model in which multiple mechanisms of vibronic coupling and their impact on energy transfer can be explicitly studied. We consider vibronic coupling that arises through either Franck-Condon activity in which each…
Quantum simulation in its current state faces experimental overhead in terms of physical space and cooling. We propose boson sampling as an alternative compact synthetic platform performing at room temperature. Identifying the capability of…
Biomolecular light-harvesting antennas operate as nanoscale devices in a regime where the coherent interactions of individual light, matter and vibrational quanta are non-perturbatively strong. The complex behaviour arising from this could,…
We study the impact of experimental imperfections on a recently proposed protocol for performing quantum simulations of vibronic spectroscopy. Specifically, we propose a method for quantifying the impact of these imperfections, optimizing…
Accurate free-energy estimation is essential in molecular simulation, yet the periodic boundary conditions (PBC) commonly used in computer simulations have rarely been explicitly exploited. Equilibrium methods such as umbrella sampling,…