David T. Limmer
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View article: Spin Polarization from Circularly Polarized Light Induced Charge Transfer
Spin Polarization from Circularly Polarized Light Induced Charge Transfer Open
We show how a spin polarization can be generated through the photo-induced electron transfer of an achiral donor-acceptor complex following chiral light excitation. In particular, we illustrate the basic energetic and symmetry requirements…
View article: Reactive path ensembles within nonequilibrium steady states
Reactive path ensembles within nonequilibrium steady states Open
The modern theory of rare events is grounded in near-equilibrium ideas, however, many systems of modern interest are sufficiently far from equilibrium that traditional approaches do not apply. Using the recently developed variational path …
View article: Nonadiabatic Force Matching for Alchemical Free-Energy Estimation
Nonadiabatic Force Matching for Alchemical Free-Energy Estimation Open
We propose a method to compute free-energy differences from nonadiabatic alchemical transformations using flow-based generative models. The method, nonadiabatic force matching, hinges on estimating the dissipation along an alchemical switc…
View article: Solvation of CaCl <sub>2</sub> at the Water–Vapor Interface Revealed by Ambient Pressure X-ray Photoelectron Spectroscopy
Solvation of CaCl <sub>2</sub> at the Water–Vapor Interface Revealed by Ambient Pressure X-ray Photoelectron Spectroscopy Open
View article: Large deviations of ionic currents in dilute electrolytes
Large deviations of ionic currents in dilute electrolytes Open
We evaluate the exponentially rare fluctuations of the ionic current for a dilute electrolyte by means of macroscopic fluctuation theory. We consider the fluctuating hydrodynamics of a fluid electrolyte described by a stochastic Poisson-Ne…
View article: Non-monotonic size-dependent exciton radiative lifetime in CsPbBr3 nanocrystals
Non-monotonic size-dependent exciton radiative lifetime in CsPbBr3 nanocrystals Open
Lead halide perovskite nanocrystals have attracted intense interest due to their desirable optical properties, diverse structural features, and size-tunable excitonic structure. Here we show that, under ambient conditions, a non-monotonic …
View article: A theory for diffusion-controlled reactions within nonequilibrium steady states
A theory for diffusion-controlled reactions within nonequilibrium steady states Open
We study diffusion-controlled processes in nonequilibrium steady states, where standard rate theory assumptions break down. Using transition path theory, we generalize the relations between reactive probability fluxes and measures of the r…
View article: Accelerated Chlorination at the Surface of Organic Aerosol
Accelerated Chlorination at the Surface of Organic Aerosol Open
An interface is a distinct chemical environment where reactivity can proceed differently than the bulk. Although organic interfaces are ubiquitous in nature, they have received comparably less attention than their aqueous counterparts. Her…
View article: Entropy is an important design principle in the photosystem II supercomplex
Entropy is an important design principle in the photosystem II supercomplex Open
Photosystem II (PSII) can achieve near-unity quantum efficiency of light harvesting in ideal conditions and can dissipate excess light energy as heat to prevent the formation of reactive oxygen species (ROS) under light stress. Understandi…
View article: Mechanism of Shape Symmetry Breaking in Surfactant Mediated Crystal Growth
Mechanism of Shape Symmetry Breaking in Surfactant Mediated Crystal Growth Open
We present a dynamical model of crystal growth, in which it is possible to reliably achieve asymmetric products, beginning from symmetric initial conditions and growing within an isotropic environment. The asymmetric growth is the result o…
View article: On the Interplay of Electronic and Lattice Screening on Exciton Binding in Two-Dimensional Lead Halide Perovskites
On the Interplay of Electronic and Lattice Screening on Exciton Binding in Two-Dimensional Lead Halide Perovskites Open
We use path integral Monte Carlo to study the energetics of excitons in layered, hybrid organic-inorganic perovskites in order to elucidate the relative contributions of dielectric confinement and electron-phonon coupling. While the dielec…
View article: Stochastic thermodynamic bounds on logical circuit operation
Stochastic thermodynamic bounds on logical circuit operation Open
Using a thermodynamically consistent, mesoscopic model for modern complementary metal-oxide-semiconductor transistors, we study an array of logical circuits and explore how their function is constrained by recent thermodynamic uncertainty …
View article: Variational Path Sampling of Rare Dynamical Events
Variational Path Sampling of Rare Dynamical Events Open
This article reviews the concepts and methods of variational path sampling. These methods allow computational studies of rare events in systems driven arbitrarily far from equilibrium. Based upon a statistical mechanics of trajectory space…
View article: Variational path sampling of rare dynamical events
Variational path sampling of rare dynamical events Open
This article reviews the concepts and methods of variational path sampling. These methods allow computational studies of rare events in systems driven arbitrarily far from equilibrium. Based upon a statistical mechanics of trajectory space…
View article: Reactive path ensembles within nonequilibrium steady-states
Reactive path ensembles within nonequilibrium steady-states Open
The modern theory of rare events is grounded in near equilibrium ideas, however many systems of modern interest are sufficiently far from equilibrium that traditional approaches do not apply. Using the recently developed variational path s…
View article: Strong adsorption of guanidinium cations to the air–water interface
Strong adsorption of guanidinium cations to the air–water interface Open
Combining Deep-UV second harmonic generation spectroscopy with molecular simulations, we confirm and quantify the specific adsorption of guanidinium cations to the air–water interface. Using a Langmuir analysis of measurements at multiple …
View article: Entropy as a Design Principle in the Photosystem II Supercomplex
Entropy as a Design Principle in the Photosystem II Supercomplex Open
Photosystem II (PSII) can achieve near-unity quantum efficiency of light harvesting in ideal conditions and can dissipate excess light energy as heat to prevent formation of reactive oxygen species under light stress. Understanding how thi…
View article: Microscopic Origin of Twist-Dependent Electron Transfer Rate in Bilayer Graphene
Microscopic Origin of Twist-Dependent Electron Transfer Rate in Bilayer Graphene Open
Using molecular simulation and continuum dielectric theory, we consider how electrochemical kinetics are modulated by the twist angle in bilayer graphene electrodes. By establishing a connection between the twist angle and the screening le…
View article: Surfactant Control of Interfacial Reaction Rates in Aqueous Microdroplets
Surfactant Control of Interfacial Reaction Rates in Aqueous Microdroplets Open
Microdroplets are purported to enhance reaction rates and produce spontaneous chemical transformations that are unfavorable in macroscale systems. The gas-liquid interface is widely implicated for the emergence of these chemical anomalies.…
View article: Evaluation of transition rates from nonequilibrium instantons
Evaluation of transition rates from nonequilibrium instantons Open
Equilibrium rate theories play a crucial role in understanding rare, reactive events. However, they are inapplicable to a range of irreversible processes in systems driven far from thermodynamic equilibrium like active and biological matte…
View article: Transition Path and Interface Sampling of Stochastic Schrödinger Dynamics
Transition Path and Interface Sampling of Stochastic Schrödinger Dynamics Open
We study rare transitions in Markovian open quantum systems driven with Gaussian noise, applying transition path and interface sampling methods to trajectories generated by stochastic Schrödinger dynamics. Interface and path sampling offer…
View article: Modeling the Superlattice Phase Diagram of Transition Metal Intercalation in Bilayer 2H-TaS$_2$
Modeling the Superlattice Phase Diagram of Transition Metal Intercalation in Bilayer 2H-TaS$_2$ Open
Van der Waals hosts intercalated with transition metal (TM) ions exhibit a range of magnetic properties strongly influenced by the structural order of the intercalants. However, predictive computational models for the intercalant ordering …
View article: Elucidating the Mechanism of Helium Evaporation from Liquid Water
Elucidating the Mechanism of Helium Evaporation from Liquid Water Open
We investigate the evaporation of trace amounts of helium solvated in liquid water using molecular dynamics simulations and theory. Consistent with experimental observations, we find a super-Maxwellian distribution of kinetic energies of e…
View article: Distinguishing Surface and Bulk Reactivity: Concentration-Dependent Kinetics of Iodide Oxidation by Ozone in Microdroplets
Distinguishing Surface and Bulk Reactivity: Concentration-Dependent Kinetics of Iodide Oxidation by Ozone in Microdroplets Open
Iodine oxidation reactions play an important role in environmental, biological, and industrial contexts. The multiphase reaction between aqueous iodide and ozone is of particular interest due to its prevalence in the marine atmosphere and …
View article: Theoretical insights into the role of lattice fluctuations on the excited behavior of lead halide perovskites
Theoretical insights into the role of lattice fluctuations on the excited behavior of lead halide perovskites Open
Lead halide perovskites have been extensively studied as a class of materials with unique optoelectronic properties. A fundamental aspect that governs optical and electronic behaviors within these materials is the intricate coupling betwee…
View article: Non-Monotonic Size-Dependent Exciton Radiative Lifetime in CsPbBr3 Nanocrystals
Non-Monotonic Size-Dependent Exciton Radiative Lifetime in CsPbBr3 Nanocrystals Open
Lead-halide perovskite nanocrystals have recently emerged as desirable optical materials for applications such as coherent quantum light emitters and solid-state laser cooling due to their short radiative lifetime and near-unity photolumin…
View article: Adsorption of Guanidinium Cations to the Air-Water Interface
Adsorption of Guanidinium Cations to the Air-Water Interface Open
Combining Deep-UV second harmonic generation spectroscopy with molecular simulations, we confirm and quantify the specific adsorption of guanidinium cations to the air-water interface. Using a Langmuir analysis and measurements at multiple…
View article: Distinguishing Surface and Bulk Reactivity: Concentration Dependent Kinetics of Iodide Oxidation by Ozone in Microdroplets
Distinguishing Surface and Bulk Reactivity: Concentration Dependent Kinetics of Iodide Oxidation by Ozone in Microdroplets Open
Iodine oxidation reactions play an important role in environmental, biological, and industrial contexts. The multiphase reaction between aqueous iodide and ozone is of particular interest due to its prevalence in the marine atmosphere and …
View article: Elucidating the mechanism of helium evaporation from liquid water
Elucidating the mechanism of helium evaporation from liquid water Open
We investigate the evaporation of trace amounts of helium solvated in liquid water using molecular dynamics simulations and theory. Consistent with experimental observations, we find a super-Maxwellian distribution of kinetic energies of e…
View article: Exact Statistics of Helical Wormlike Chains with Twist-Bend Coupling
Exact Statistics of Helical Wormlike Chains with Twist-Bend Coupling Open
We present a solution for the Green's function for the general case of a helical wormlike chain with twist-bend coupling, and demonstrate the applicability of our solution for evaluating general structural and mechanical chain properties. …