87 citations · 510 across the 26 of their papers we have counts for
26 papers
How Symmetry Governs the Dihedral Angle Dependence of Intermolecular Spin-Orbit Coupling
Antonio J. Garzon-Ramirez, Connor K. Terry Weatherly, Kyle T. Kairys +2
Spin-orbit, charge-transfer intersystem crossing (SOCT-ISC) allows for the efficient production of triplet excited states in donor-acceptor (DA) dyads without the involvement of he…
QC Lab: A Python Package for Quantum-Classical Dynamics
Alex Krotz, Ethan Byrd, Ken Miyazaki +1
QC Lab is an open-source Python package for QC dynamics simulations aimed to promote the development of QC algorithms, and their application to a wide variety of relevant model pro…
Optically Addressing Circularly-Polarized Vibrations in Molecules
Chientzu Lin, Connor K. Terry Weatherly, Roel Tempelaar
Circularly-polarized (CP) vibrations are the nuclear-motion analog of CP light, emerging in molecules with non-Abelian point-group symmetry that support orthogonal and degenerate v…
Focused Sampling for Low-Cost and Accurate Ehrenfest Modeling of Cavity Quantum Electrodynamics
Ming-Hsiu Hsieh, Alex Krotz, Roel Tempelaar
An economic modeling approach for cavity quantum electrodynamics is provided by mean-field dynamics, wherein the optical field is described classically while a self-consistent inte…
Surface hopping simulations show valley depolarization driven by exciton-phonon resonance
Alex Krotz, Roel Tempelaar
Resonances between excitonic transitions and nuclear coordinates have been shown to drive a variety of excited-state dynamical phenomena in molecular systems. Here, we report mixed…
Mixed Quantum-Classical Dynamics Yields Anharmonic Rabi Oscillations
Ming-Hsiu Hsieh, Roel Tempelaar
We apply a mixed quantum-classical (MQC) approach to the quantum Rabi model, involving a classical optical field coupled self-consistently to a quantum two-level system. Under the…
Mixed quantum-classical modeling of exciton-phonon scattering in solids: Application to optical linewidths of monolayer MoS2
Alex Krotz, Roel Tempelaar
We present a mixed quantum-classical framework for the microscopic and non-Markovian modeling of exciton-phonon scattering in solid-state materials, and apply it to calculate the o…
Unitary Basis Transformations in Mixed Quantum-Classical Dynamics
Ken Miyazaki, Alex Krotz, Roel Tempelaar
A common approach to minimizing the cost of quantum computations is by transforming a quantum system into a basis that can be optimally truncated. Here, we derive classical equatio…
Ehrenfest Modeling of Cavity Vacuum Fluctuations and How to Achieve Emission from a Three-Level Atom
Ming-Hsiu Hsieh, Alex Krotz, Roel Tempelaar
A much-needed solution for the efficient modeling of strong coupling between matter and optical cavity modes is offered by mean-field mixed quantum--classical dynamics, where a cla…
UV/vis-to-IR Photonic Down Conversion Mediated by Excited State Vibrational Polaritons
Connor K. Terry Weatherly, Justin Provazza, Emily A. Weiss +1
This work proposes a new photophysical phenomenon whereby UV/vis excitation of a molecule involving a Franck-Condon (FC) active vibration yields infrared (IR) emission by strong co…
Overcoming positivity violations for density matrices in surface hopping
Anna S. Bondarenko, Roel Tempelaar
Fewest-switches surface hopping (FSSH) has emerged as one of the leading methods for modeling the quantum dynamics of molecular systems. While its original formulation was limited…
A Mean-Field Treatment of Vacuum Fluctuations in Strong Light-Matter Coupling
Ming-Hsiu Hsieh, Alex Krotz, Roel Tempelaar
Mean-field mixed quantum--classical dynamics could provide a much-needed means to inexpensively model quantum electrodynamical phenomena, by describing the optical field and its va…
Chiral polaritons based on achiral Fabry-Perot cavities using apparent circular dichroism
Andrew H. Salij, Randall H. Goldsmith, Roel Tempelaar
Polariton states with high levels of chiral dissymmetry offer exciting prospects for quantum information, sensing, and lasing applications. Such dissymmetry must emanate from eithe…
Perturbation theory under the truncated Wigner approximation reveals how system-environment entanglement formation drives quantum decoherence
Justin Provazza, Roel Tempelaar
Quantum decoherence is the disappearance of simple phase relations within a discrete quantum system as a result of interactions with an environment. For many applications, the ques…
Treating geometric phase effects in nonadiabatic dynamics
Alex Krotz, Roel Tempelaar
We present an approach for eliminating the gauge freedom for derivative couplings in nonadiabatic dynamics in the presence of geometric phase effects. This approach relies on a bot…
A Reciprocal-Space Formulation of Mixed Quantum-Classical Dynamics
Alex Krotz, Justin Provazza, Roel Tempelaar
We derive a formulation of mixed quantum-classical dynamics for describing electronic carriers interacting with phonons in reciprocal space. For dispersionless phonons, we start by…
Microscopic theory of cavity-confined monolayer semiconductors: polariton-induced valley relaxation and the prospect of enhancing and controlling the valley pseudospin by chiral strong coupling
Andrew Salij, Roel Tempelaar
We apply a microscopic theory of exciton-polaritons in cavity-confined monolayer transition-metal dichalcogenides including both optical polarizations in the monolayer plane, allow…
Acene:spacer blends show exothermic singlet fission to proceed coherently, while endothermic fission proceeds incoherently
Clemens Zeiser, Chad Cruz, David R Reichman +6
The fission of singlet excitons into triplet pairs in organic materials holds great technological promise, but the rational application of this phenomenon is hampered by a lack of…
Removing instabilities in the hierarchical equations of motion: exact and approximate projection approaches
Ian S. Dunn, Roel Tempelaar, David R. Reichman
The hierarchical equations of motion (HEOM) provide a numerically exact approach for computing the reduced dynamics of a quantum system linearly coupled to a bath. We have found th…
Multi-set matrix product state calculations reveal mobile Franck-Condon excitations under strong Holstein-type coupling
Benedikt Kloss, David Reichman, Roel Tempelaar
We show that the dynamics of (vertical) Franck-Condon excitations in the regime where Holstein-coupled vibrational modes mix strongly with electronic degrees of freedom sharply con…
Many-Body Simulation of Two-Dimensional Electronic Spectroscopy of Excitons and Trions in Monolayer Transition-Metal Dichalcogenides
Roel Tempelaar, Timothy C. Berkelbach
We present a many-body formalism for the simulation of time-resolved nonlinear spectroscopy and apply it to study the coherent interaction between excitons and trions in doped tran…
Vibronic exciton theory of singlet fission. III. How vibronic coupling and thermodynamics promote rapid triplet generation in pentacene crystals
Roel Tempelaar, David R. Reichman
We extend the vibronic exciton theory introduced in our previous work to study singlet fission dynamics, in particular addressing recent indications of the importance of vibronic c…
Unravelling coherences in the FMO complex
Erling Thyrhaug, Roel Tempelaar, Marcelo Alcocer +5
The idea that excitonic state (electronic) coherences are of fundamental importance to natural photosynthesis gained popularity when, a decade ago, slowly dephasing quantum beats w…
Exciton-Exciton Annihilation Is Coherently Suppressed in H-Aggregates, but Not in J-Aggregates
Roel Tempelaar, Thomas L. C. Jansen, Jasper Knoester
We theoretically demonstrate a strong dependence of the annihilation rate between (singlet) excitons on the sign of dipole-dipole couplings between molecules. For molecular H-aggre…