Related papers: Multistate metadynamics for automatic exploration …
Minimum energy conical intersections can be used to rationalize photochemical processes. In this Letter, we examine an algorithm to locate these structures that does not require the evaluation of nonadiabatic coupling vectors, showing that…
Metadynamics, a member of the `flat histogram' class of advanced sampling algorithms, has been widely used in molecular simulations to drive the exploration of states separated by high free energy barriers and promote comprehensive sampling…
We investigate the structure of a prototypical two-state conical intersection (BeH$_2$) using a phase space electronic Hamiltonian $\hat{H}_{PS}(\bR,\bP)$ that goes beyond the Born-Oppenheimer framework. By parameterizing the electronic…
The choice of the electronic representation in on-the-fly quantum dynamics is crucial. The adiabatic representation is appealing since adiabatic states are readily available from quantum chemistry packages. The nuclear wavepackets are then…
Conical intersections constitute the conceptual bedrock of our working understanding of ultrafast, nonadiabatic processes within photochemistry (and photophysics). Accurate calculation of potential energy surfaces within the vicinity of…
Metadynamics is a commonly used and successful enhanced sampling method. By the introduction of a history dependent bias which depends on a restricted number of collective variables(CVs) it can explore complex free energy surfaces…
Conical intersections are common in molecular physics and photochemistry, and are often invoked to explain observed reaction products. A conical intersection can occur when an excited electronic potential energy surface intersects with the…
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…
Conical intersections between electronic potential energy surfaces are paradigmatic for the study of non-adiabatic processes in the excited states of large molecules. However, since the corresponding dynamics occurs on a femtosecond…
Metastable states appear as long-lived intermediate states in various natural transport phenomena which are governed by energy landscapes. As such, these intermediate metastable states dominate the system's dynamics at coarse grained times.…
Conical intersections (CIs) are seen as the main mediators of nonadiabatic transitions; yet, mixed quantum-classical (MQC) simulations rarely, if ever, sample geometries with exactly degenerate electronic energies. Here we show that this…
Ab initio modeling of conical intersection dynamics is crucial for various photochemical, photophysical, and biological processes. However, adiabatic electronic states obtained from electronic structure computations involve random phases,…
Conical intersections are ubiquitous in polyatomic molecules and responsible for a wide range of phenomena in chemistry and physics. We introduce and implement a local diabatic representation for the correlated electron-nuclear dynamics…
Statistical mechanics is founded on the assumption that a system can reach thermal equilibrium, regardless of the starting state. Interactions between particles facilitate thermalization, but, can interacting systems always equilibrate…
Conical intersections are topologically protected crossings between the potential energy surfaces of a molecular Hamiltonian, known to play an important role in chemical processes such as photoisomerization and non-radiative relaxation.…
Stochastic systems often exhibit multiple viable metastable states that are long-lived. Over very long timescales, fluctuations may push the system to transition between them, drastically changing its macroscopic configuration. In realistic…
We demonstrate coherent control of motional dynamics in trapped Rydberg ions engineered to exhibit a conical intersection between adiabatic potential-energy surfaces. Using quantum optimal control, an optimally shaped electric field drives…
We present a general extension of the metadynamics allowing for an automatic sampling of quantum property manifolds (ASQPM) giving rise to functional landscapes that are analogous to the potential energy surfaces in the frame of the…
Conical intersections play central roles in photoinduced reactions. However, comprehensive conical-intersection datasets that could advance our understanding of excited-state reaction processes remain scarce. To address this gap, we…
The complex physics of glass forming systems is controlled by the structure of the low energy portions of their potential energy landscapes. Here, we report that a modified metadynamics algorithm efficiently explores and samples low energy…