We investigate transport of a Frenkel exciton in finite one-dimensional chains, where temperature induced interparticle vibrations dynamically modulate the electronic couplings between neighboring particles. In the adiabatic regime, where vibrational motion is slower than excitation transfer between sites, this modulation gives rise to long-lived oscillations in the exciton populations. These oscillations, which we refer to as adiabatic beatings, are most pronounced at the boundaries of the chain. The amplitude of these beatings decreases with increasing chain length and is larger for chains with an odd number of particles than for those with an even number. Furthermore, the beatings are even present for disorder strength smaller than the equilibrium interparticle coupling, although their amplitude decreases gradually and eventually vanishes when the disorder becomes comparable to the coupling strength.

The process tensor framework to open quantum systems provides the most general description of multi-time correlations in non-Markovian quantum dynamics. A compressed representation of a process tensor in terms of matrix product operators (MPO) can be used for numerically exact calculations of multi-time correlation functions in systems strongly coupled to a non-Markovian reservoir. We show here that the numerical effort for computing multi-dimensional spectra can be significantly improved using a time-translation invariant MPO representation of the process tensor obtained from the uniform time-evolving matrix product operator (uniTEMPO) method. In particular, this approach provides a spectral representation of the non-Markovian dynamics that gives direct access to correlation functions in Fourier-space, avoiding explicit real-time evolution. We calculate linear and 2D electronic spectra for an example system and discuss the performance and numerical scaling of our simulations.

We present a size-invariant (i.e., N0) scaling algorithm for simulating fluorescence spectroscopy in large molecular aggregates. We combine the dyadic adaptive hierarchy of pure states (DadHOPS) equation-of-motion with an operator decomposition scheme and an efficient Monte Carlo sampling algorithm to enable a formally exact, local description of the fluorescence spectrum in large molecular aggregates. Furthermore, we demonstrate that the ensemble average inverse participation ratio of DadHOPS wave functions reproduces the delocalization extent extracted from fluorescence spectroscopy of J-aggregates with strong vibronic transitions. This work provides a computationally efficient framework for fluorescence simulations, offering a new tool for understanding the optical properties of mesoscale molecular systems.

We consider assemblies of molecules where the electronic wavefunctions of different molecules do not overlap. Typically, the interaction Hamiltonian between two molecules is then described by their Coulomb interaction, and matrix-elements between products of single-molecule energy eigenstates are calculated using the corresponding (transition) charge densities. In the present work, we compare this approach with one based on (transition) current densities. As an example, we perform calculations for 3,4,9,10-perylenetetracarboxylicacid-dianhydride (PTCDA) molecules in different arrangements. We find that for exact molecular wavefunctions, both methods agree, but there are marked differences for the wavefunctions that we obtained from electronic-structure theory. The main difference can be attributed to the error in the molecular transition energy and results in an arrangement-independent ratio between the interactions calculated with the two approaches. At small separations between the molecules, additional deviations occur, which we trace back to the quality of the molecular electronic wavefunctions. Within both approaches, we calculate interactions for the arrangement of PTCDA on KCl and NaCl surfaces and compare to the ones obtained using the point-dipole approximation. Finally, we provide a simple algorithm that allows fast and accurate calculations of the involved integrals.

We show theoretically that it is possible to coherently transfer vibrational excitation between trapped neutral atoms over a micrometer apart. To this end we consider three atoms, where two are in the electronic ground state and one is excited to a Rydberg state whose electronic orbital overlaps with the positional wave functions of the two ground-state atoms. The resulting scattering of the Rydberg electron with the ground-state atoms provides the interaction required to transfer vibrational excitation from one trapped atom to the other. By numerically investigating the dependence of the transfer dynamics on the distance between traps and their relative frequencies we find that there is a "sweet spot" where the transfer of a vibrational excitation is nearly perfect and fast compared to the Rydberg lifetime. We investigate the robustness of this scenario with respect to changes of the parameters. In addition, we derive a intuitive effective Hamiltonian which explains the observed dynamics.

Quantum transport of charge or energy in networks with discrete sites is central to diverse quantum technologies, from molecular electronics to light harvesting and quantum opto-mechanical metamaterials. A one dimensional network can be viewed as waveguide. We show that if such waveguide is hybridised with a control unit that contains a few sites, then transmission through the waveguide depends sensitively on the motion of the sites in the control unit. Together, the hybrid waveguide and its control-unit form a Fano-Anderson chain whose Born-Oppenheimer surfaces inherit characteristics from both components: A bandstructure from the waveguide and potential energy steps as a function of site coordinates from the control-unit. Using time-dependent quantum wave packets, we reveal conditions under which the hybrid structure becomes transmissive only if the control unit contains mobile sites that induce non-adiabatic transitions between the surfaces. Hence, our approach provides functional synthetic Born-Oppenheimer surfaces for hybrid quantum technologies combining mechanic and excitonic elements, and has possible applications such as switching and temperature sensing.

The question under which conditions oscillators with slightly different frequencies synchronize appears in various settings. We consider the case of a finite number of harmonic oscillators arranged on a ring, with bilinear, dissipative nearest-neighbor coupling. We show that by tuning the gain and loss appropriately, stable synchronized dynamics may be achieved. These findings are interpreted using the complex eigenvalues and eigenvectors of the non-Hermitian matrix describing the dynamics of the system. We provide a complete discussion for the case of two oscillators. Ring sizes with a small number of oscillators are discussed taking the case of N=5 oscillators as an example. For N≳10 we focus on the case where the frequency fluctuations of each oscillator are chosen from a Gaussian distribution with zero mean and standard deviation σ. We derive a scaling law for the largest standard deviation σ_{full} that still permits all oscillators to be fully synchronized: σ_{full}∼N^{-3/2}. Finally, we discuss how such random fluctuations influence the timescale on which the synchronized state is reached and on which timescale the synchronized state then decays.

We consider a system of N bi-linearly coupled damped harmonic quantum oscillators with time-evolution governed by a Lindblad equation. We show that the corresponding stochastic quantum state diffusion equation can be transformed into a set of N independent damped harmonic oscillators. This offers a great reduction in the basis size. We investigate the numerical performance of the method and find, in particular, scaling laws for the number of stochastic trajectories needed to find a certain accuracy.

We examine topological phases and symmetry-protected electronic edge states in the context of a Rydberg composite: a Rydberg atom interfaced with a structured arrangement of ground-state atoms. The electronic Hamiltonian of such a composite possesses a direct mapping to a tight-binding Hamiltonian, which enables the realization and study of a variety of systems with non-trivial topology by tuning the arrangement of ground-state atoms and the excitation of the Rydberg atom. The Rydberg electron moves in a combined potential including the long-ranged Coulomb interaction with the Rydberg core and short-ranged interactions with each neutral atom; the effective interactions between sites are determined by this combination. We first confirm the existence of topologically-protected edge states in a Rydberg composite by mapping it to the paradigmatic Su-Schrieffer-Heeger dimer model. Following that, we study more complicated systems with trimer unit cells which can be easily simulated with a Rydberg composite.

The question under which conditions oscillators with slightly different frequencies synchronize appears in various settings. We show that synchronization can be achieved even for harmonic oscillators that are bilinearly coupled via a purely dissipative interaction. By appropriately tuned gain/loss stable dynamics may be achieved where for the cases studied in this work all oscillators are synchronized. These findings are interpreted using the complex eigenvalues and eigenvectors of the non-Hermitian matrix describing the dynamics of the system.

Nanocomposite materials consist of nanometer-sized quantum objects such as atoms, molecules, voids or nanoparticles embedded in a host material. These quantum objects can be exploited as a super-structure, which can be designed to create material properties targeted for specific applications. For electromagnetism, such targeted properties include field enhancements around the bandgap of a semiconductor used for solar cells, directional decay in topological insulators, high kinetic inductance in superconducting circuits, and many more. Despite very different application areas, all of these properties are united by the common aim of exploiting collective interaction effects between quantum objects. The literature on the topic spreads over very many different disciplines and scientific communities. In this review, we present a cross-disciplinary overview of different approaches for the creation, analysis and theoretical description of nanocomposites with applications related to electromagnetic properties.

Highly excited Rydberg atoms inherit their level structure, symmetries, and scaling behavior from the hydrogen atom. We demonstrate that these fundamental properties enable a thermodynamic limit of a single Rydberg atom subjected to interactions with nearby ground-state atoms. The limit is reached by simultaneously increasing the number of ground-state atoms and the level of excitation of the Rydberg atom, for which the Coulomb potential supplies infinitely many and highly degenerate excited states. Our study reveals a surprising connection to an archetypal concept of condensed matter physics, Anderson localization, facilitated by a direct mapping between the Rydberg atom's electronic spectrum and the spectrum of a tight-binding Hamiltonian. The hopping amplitudes of this tight-binding system are determined by the arrangement of ground-state atoms and can range from oscillatory and long-ranged to nearest-neighbor. In the latter we identify clear signatures of the Anderson localization of the Rydberg electron.

In this paper, we present dyadic adaptive HOPS (DadHOPS), a new method for calculating linear absorption spectra for large molecular aggregates. This method combines the adaptive HOPS (adHOPS) framework, which uses locality to improve computational scaling, with the dyadic HOPS method previously developed to calculate linear and nonlinear spectroscopic signals. To construct a local representation of dyadic HOPS, we introduce an initial state decomposition that reconstructs the linear absorption spectra from a sum over locally excited initial conditions. We demonstrate the sum over initial conditions can be efficiently Monte Carlo sampled and that the corresponding calculations achieve size-invariant [i.e., O(1)] scaling for sufficiently large aggregates while trivially incorporating static disorder in the Hamiltonian. We present calculations on the photosystem I core complex to explore the behavior of the initial state decomposition in complex molecular aggregates as well as proof-of-concept DadHOPS calculations on an artificial molecular aggregate inspired by perylene bis-imide to demonstrate the size-invariance of the method.

Simulation of spectroscopic observables for molecular aggregates with strong and structured coupling of electronic excitation to vibrational degrees of freedom is an important but challenging task. The Hierarchy of Pure States (HOPS) provides a formally exact solution based on local, stochastic trajectories. Exploiting the localization of HOPS for the simulation of absorption spectra in large aggregates requires a formulation in terms of normalized trajectories. Here, we provide a normalized dyadic equation where the ket- and bra-states are propagated in different electronic Hilbert spaces. This work opens the door to applying adaptive HOPS methods for the simulation of absorption spectra.

Simulating quantum systems is believed to be one of the first applications for which quantum computers may demonstrate a useful advantage. For many problems in physics, we are interested in studying the evolution of the electron-phonon Hamiltonian, for which efficient digital quantum computing schemes exist. Yet to date, no accurate simulation of this system has been produced on real quantum hardware. In this work, we consider the absolute resource cost for gate-based quantum simulation of small electron-phonon systems as dictated by the number of Trotter steps and bosonic energy levels necessary for the convergence of dynamics. We then apply these findings to perform experiments on IBM quantum hardware for both weak and strong electron-phonon coupling. Despite significant device noise, through the use of approximate circuit recompilation we obtain electron-phonon dynamics on current quantum computers comparable to exact diagonalisation. Our results represent a significant step in utilising near term quantum computers for simulation of quantum dynamics and highlight the novelty of approximate circuit recompilation as a tool for reducing noise.

A common task is the determination of system parameters from spectroscopy, where one compares the experimental spectrum with calculated spectra, that depend on the desired parameters. Here we discuss an approach based on a machine learning technique, where the parameters for the numerical calculations are chosen from Gaussian Process Regression (GPR). This approach does not only quickly converge to an optimal parameter set, but in addition provides information about the complete parameter space, which allows for example to identify extended parameter regions where numerical spectra are consistent with the experimental one. We consider as example dimers of organic molecules and aim at extracting in particular the interaction between the monomers, and their mutual orientation. We find that indeed the GPR gives reliable results which are in agreement with direct calculations of these parameters using quantum chemical methods.

Laser-induced fluorescence spectra and excitation lifetimes of anthracene, tetracene, and pentacene molecules attached to the surface of solid argon clusters have been measured with respect to cluster size, density of molecules, and excitation density. Results are compared to previous studies on the same sample molecules attached to neon clusters. A contrasting lifetime behavior of anthracene on neon and argon clusters is discussed, and mechanisms are suggested to interpret the results. Although both neon and argon clusters are considered to be weakly interacting environments, we find that the excitation decay dynamics of the studied acenes depends significantly on the cluster material. Moreover, we find even qualitative differences regarding the dependence on the dopant density. Based on these observations, previous assignments of collective radiative and non-radiative decay mechanisms are discussed in the context of the new experimental findings.

The concept of exceptional points-based optical amplifiers (EPOAs) has been recently proposed as a new paradigm for miniaturizing optical amplifiers while simultaneously enhancing their gain-bandwidth product. While the operation of this new family of amplifiers in the classical domain provides a clear advantage, their performance in the quantum domain has not yet been evaluated. Particularly, it is not clear how the quantum noise introduced by vacuum fluctuations will affect their operation. Here, we investigate this problem by considering three archetypal EPOAs structures that rely either on unidirectional coupling, parity-time (PT) symmetry, or particle-hole symmetry for implementing the exceptional point (EP). By using the Heisenberg-Langevin formalism, we calculate the added quantum noise in each of these devices and compare it with that of a quantum-limited amplifier scheme that does not involve any exceptional points. Our analysis reveals several interesting results: most notably that while the quantum noise of certain EPOAs can be comparable to those associated with conventional amplifier systems, in general the noise does not follow a universal scaling as a function of the exceptional point but rather varies from one implementation to another.

We present a methodology for simulating multidimensional electronic spectra of molecular aggregates with coupling of electronic excitation to a structured environment using the stochastic non-Markovian quantum state diffusion (NMQSD) method in combination with perturbation theory for the response functions. A crucial aspect of our approach is that we propagate the NMQSD equation in a doubled system Hilbert space but with the same noise. We demonstrate that our approach shows fast convergence with respect to the number of stochastic trajectories, providing a promising technique for numerical calculation of two-dimensional electronic spectra of large molecular aggregates.

We derive a stochastic hierarchy of matrix product states (HOMPS) for non-Markovian dynamics in open quantum system at finite temperature, which is numerically exact and efficient. HOMPS is obtained from the recently developed stochastic hierarchy of pure states (HOPS) by expressing HOPS in terms of formal creation and annihilation operators. The resulting stochastic first order differential equation is then formulated in terms of matrix product states and matrix product operators. In this way the exponential complexity of HOPS can be reduced to scale polynomial with the number of particles. The validity and efficiency of HOMPS is demonstrated for the spin-boson model and long chains where each site is coupled to a structured, strongly non-Markovian environment.