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The recrossing correction to the transition state theory estimate of a thermal rate can be difficult to calculate when the energy barrier is flat. This problem arises, for example, in polymer escape if the polymer is long enough to stretch…
This work identifies geometric effects on dynamics due to nonadiabatic couplings in Born Oppenheimer systems and provides a systematic method for deriving corrections to mixed quantum-classical methods. Specifically, an exact path integral…
Treatment with high energy ionizing radiation is one of the main methods in modern cancer therapy that is in clinical use. During the last decades, two main approaches to dose calculation were used, Monte Carlo simulations and…
The rate of electron transfer between a molecular species and a metal, each at a different local temperature, is examined theoretically through implementation of a bithermal (characterized by two temperatures) Marcus formalism. Expressions…
Quantum rate theory encompasses the electron-transfer rate constant concept of electrochemical reactions as a particular setting, besides demonstrating that the electrodynamics of these reactions obey relativistic quantum mechanical rules.…
The performance of time-independent, orbital optimized calculations of excited states is assessed with respect to charge transfer excitations in organic molecules in comparison to the linear-response time-dependent density functional theory…
Marcus theory famously predicts that electron-transfer rates decrease once the thermodynamic driving force exceeds the reorganization energy. Yet many systems instead exhibit Rehm-Weller kinetics, in which the rate saturates rather than…
We have reexamined the thermally induced Co(NH_3)_6^{2+/3+} [Co(II/III)] redox reaction using the first principles density-functional-theory method, semiclassical Marcus theory, and known charge transfer parameters. We confirm a previously…
Photo-induced excited-state energy transfer (EET) processes play an important role in the solar energy conversions. The phenylene ethynylene (PE) dendrimers display great potential in improving the efficiency of solar cells, because of…
We introduce a novel computational framework for excited-states molecular quantum dynamics simulations driven by quantum computing-based electronic-structure calculations. This framework leverages the fewest-switches surface-hopping method…
Mapping reaction pathways and transition states (TS) is fundamental to chemistry but computationally expensive at scale. The minimum energy pathway (MEP) dictates reaction rates and mechanisms, yet recovering it via electronic-structure…
The effect of solvation on the electron transfer (ET) rate processes is investigated on the basis of the exact theory constructed in J. Phys. Chem. B Vol. 110, (2006); quant-ph/0604071. The nature of solvation is studied in a close relation…
For interacting electrons in solids, Heisenberg's equation is used to calculate the distribution in energy of transitions induced by adding an electron to an atomic-like spin orbital. This is the projected density of transitions which…
We describe a robust and efficient chain-of-states method for computing Minimum Energy Paths~(MEPs) associated to barrier-crossing events in poly-atomic systems. The path is parametrized in terms of a continuous variable $t \in [0,1]$ that…
Semiclassical instanton theory is a form of quantum transition-state theory which can be applied to computing thermal reaction rates for complex molecular systems including quantum tunneling effects. There have been a number of attempts to…
Excitation energy transfer (EET) in an organic/inorganic nanohybrid system, composed of a single \textit{para}-sexiphenyl (6P) molecule physisorbed on a finite-sized MoS$_2$ nanoflake, is investigated theoretically. % The electronic…
We present two multistate ring polymer instanton (RPI) formulations, both obtained from an exact path integral representation of the quantum canonical partition function for multistate systems. The two RPIs differ in their treatment of the…
Realizing efficient and controlled state transfer is necessary for implementing a wide range of classical and quantum information protocols. Recent studies have demonstrated that both asymmetric and symmetric state transfer can be achieved…
We present in this paper the main structural features and enthalpy details for the energy profiles of the title reactions, both for the exothermic (forward) path to NH$_{3}$ formation and for the endothermic (reverse) reaction to…
Two-dimensional electronic spectroscopy (2DES) provides a detailed picture of electronically nonadiabatic dynamics that can be interpreted with the aid of simulations. Here, we develop and contrast trajectory-based nonadiabatic dynamics…