Related papers: Reduced density matrix hybrid approach: Applicatio…
We discuss the evolution of purity in mixed quantum/classical approaches to electronic nonadiabatic dynamics in the context of the Ehrenfest model. As it is impossible to exactly determine initial conditions for a realistic system, we…
Near-unity energy transfer efficiency has been widely observed in natural photosynthetic complexes. This phenomenon has attracted broad interest from different fields, such as physics, biology, chemistry and material science, as it may…
We present here a formulation of the electronic ground-state energy in terms of the second order reduced density matrix, using a duality argument. It is shown that the computation of the ground-state energy reduces to the search of the…
An efficient computational algorithm to implement a local operator approach to partitioning electronic energy in general molecular systems is presented. This approach, which rigorously defines the electronic energy on any subsystem within a…
We investigate the energy transfer dynamics in a donor-acceptor model by developing a time-local master equation technique based on a variational transformation of the underlying Hamiltonian. The variational transformation allows a…
In this manuscript we present a theoretical framework and its numerical implementation to simulate the out-of-equilibrium electron dynamics induced by the interaction of ultrashort laser pulses in condensed-matter systems. Our approach is…
Standard variational methods tend to obtain upper bounds on the ground state energy of quantum many-body systems. Here we study a complementary method that determines lower bounds on the ground state energy in a systematic fashion, scales…
We use Magnetospheric Multiscale (MMS) mission data to investigate electron-scale energy transfer due to lower hybrid drift waves during magnetopause reconnection. We analyze waves observed in an electron-scale plasma mixing layer at the…
Primitive photosynthetic cells appear over three billion years prior to any other more complex life-forms, thus it is reasonable to assume that Nature has designed a photosynthetic mechanism using minimal resources but honed to perfection…
Several recent studies of energy transfer in photosynthetic light harvesting complexes have revealed a subtle interplay between coherent and decoherent dynamic contributions to the overall transfer efficiency in these open quantum systems.…
A simple formula is obtained for coupling electrons in a complex system to the electromagnetic field. It includes the effect of intra-atomic excitations and nuclear motion, and can be applied in. e.g., first-principles-based simulations of…
Recently, several works have analysed the efficiency of photosynthetic complexes in a transient scenario and how that efficiency is affected by environmental noise. Here, following a quantum master equation approach, we study the energy and…
Hybrid nanocomposites can offer a wide range of opportunities to control the light-matter interac- tion and electromagnetic energy flow at the nanoscale, leading to exotic optoelectronic devices. We study theoretically the dipole-dipole…
We develop an energy density matrix that parallels the one-body reduced density matrix (1RDM) for many-body quantum systems. Just as the density matrix gives access to the number density and occupation numbers, the energy density matrix…
The thawed Gaussian Ehrenfest dynamics is a single-trajectory method that partially includes both nuclear quantum and electronically nonadiabatic effects by combining the thawed Gaussian wavepacket dynamics with Ehrenfest dynamics. First,…
Excitonic models of light-harvesting complexes, where the vibrational degrees of freedom are treated as a bath, are commonly used to describe the motion of the electronic excitation through a molecule. Recent experiments point toward the…
We provide physically intuitive mechanisms for the effect of noise on excitation energy transfer (EET) in networks. Using these mechanisms of dephasing-assisted transport (DAT) in a hybrid basis of both excitons and sites, we develop a…
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…
We present an analytical model for Forster resonance energy transfer (FRET) between a donor and an acceptor placed in inhomogeneous and absorptive environment characterized by complex dielectric function, e.g., near a metal-dielectric…
Following the calculation of optimal energy transfer in thermal environment in our first paper (Wu et al., New J. Phys., 2010, 12, 105012), full quantum dynamics and leading-order `classical' hopping kinetics are compared in the seven-site…