Related papers: Inspecting molecular aggregate quadratic vibronic …
We study the molecular mode coupling theory for a liquid of diatomic molecules. The equations for the critical tensorial nonergodicity parameters ${\bf F}_{ll'}^m(q)$ and the critical amplitudes of the $\beta$ - relaxation ${\bf…
Mixed-quantum classical (MQC) methods for simulating the dynamics of molecules at metal surfaces have the potential to accurately and efficiently provide mechanistic insight into reactive processes. Here, we introduce simple two-dimensional…
Two-dimensional (2D) vibrational spectroscopy is a powerful means of investigating the structure and dynamics of complex molecules in condensed phases. However, even in theory, analysis of 2D spectra resulting from complex inter- and…
We build on the concept of eigenvector continuation to develop an efficient multi-state method for the rigorous and smooth interpolation of a small training set of many-body wavefunctions through chemical space at mean-field cost. The…
Quantum simulation of chemical systems is one of the most promising near-term applications of quantum computers. The variational quantum eigensolver, a leading algorithm for molecular simulations on quantum hardware, has a serious…
In the construction of diabatic vibronic Hamiltonians for quantum dynamics in the excited-state manifold of molecules, the coupling constants are often extracted solely from information on the excited-state energies. Here, a new protocol is…
We employ the Dirac-Frenkel variational principle and multiple Davydov ansatz to study time-dependent fluorescence spectra of a driven qubit in the weak- to strong qubit-reservoir coupling regimes, where both the Rabi frequency and…
We present a time-dependent variational approach with the multiple Davydov $D_2$ trial state to simulate the dynamics of light-matter systems when the field is in a coherent state with an arbitrary finite mean photon number. The variational…
We analyze the creation of spin squeezed atomic ensembles by simultaneous dispersive interactions with several optical frequencies. A judicious choice of optical parameters enables optimization of an interferometric detection scheme that…
Accurately resolving many-body satellite features in molecular core-level spectra requires theoretical approaches that capture electron correlation both efficiently and systematically. The recently developed time-dependent double…
We propose a novel scheme for probing vibronic coherence in charge migration in molecules utilizing strong field sequential double ionization. To demonstrate the feasibility of this approach, we perform full simulations of a pump-probe…
Atoms confined in optical tweezer arrays constitute a platform for the implementation of quantum computers and simulators. State-dependent operations are realized by exploiting electrostatic dipolar interactions that emerge, when two atoms…
Although useful to extract excitation energies of states of double-excitation character in time-dependent density functional theory that are missing in the adiabatic approximation, the frequency-dependent kernel derived earlier [J. Chem.…
We investigate the nonequilibrium population of a vibrational mode in the steady state of a biased molecular junction, using a rate equation approach. We focus on the limit of weak electronic-vibrational coupling and show that, in the…
In this work we develop a semi-analytical variational ansatz to study the properties of few photon excitations interacting with a collection of quantum emitters in regimes that go beyond the rotating wave approximation. This method can be…
Covariant density functional theory, which has so far been applied only within the framework of static and time dependent mean field theory is extended to include Particle-Vibration Coupling (PVC) in a consistent way. Starting from a…
Molecular vibrations underpin important phenomena such as spectral properties, energy transfer, and molecular bonding. However, obtaining a detailed understanding of the vibrational structure of even small molecules is computationally…
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…
Vibrational dynamics of adsorbates near surfaces plays both an important role for applied surface science and as model lab for studying fundamental problems of open quantum systems. We employ a previously developed model for the relaxation…
Inhomogeneous ensembles of quantum dots (QDs) coupled to a charge reservoir are widely studied by using, e.g., electrical methods like capacitance-voltage spectroscopy. We present experimental measurements of the QD capacitance as a…