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arXiv:1804.06600 · Physical Review A

Multiexcitons in flexible Rydberg aggregates

Ghassan Abumwis, Sebastian Wüster

Published Oct 3, 2018• 3 citations
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Abstract

Flexible Rydberg aggregates, assemblies of a few Rydberg atoms coherently sharing electronic excitations while undergoing directed atomic motion, show great promise as a quantum simulation platform for nuclear motion in molecules or quantum energy transport. Here we study additional features that are enabled by the presence of more than a single electronic excitation, thus considering multiexciton states. We describe cases where these can be decomposed into underlying single-exciton states and then present dynamical scenarios with atomic motion that illustrate exciton-exciton collisions, exciton routing, and strong nonadiabatic effects in simple one-dimensional settings.

DOI
10.1103/physreva.98.043606

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Flexible Rydberg aggregates, assemblies of a few Rydberg atoms coherently sharing electronic excitations while undergoing directed atomic motion, show great promise as a quantum simulation platform for nuclear motion in molecules or quantum energy transport. Here we study additional features that are enabled by the presence of more than a single electronic excitation, thus considering multiexciton states. We describe cases where these can be decomposed into underlying single-exciton states and then present dynamical scenarios with atomic motion that illustrate exciton-exciton collisions, exciton routing, and strong nonadiabatic effects in simple one-dimensional settings.
We study the link between atomic motion and exciton transport in flexible Rydberg aggregates, assemblies of highly excited light alkali-metal atoms, for which motion due to dipole-dipole interaction becomes relevant. In two one-dimensional atom chains crossing at a right angle adiabatic exciton transport is affected by a conical intersection of excitonic energy surfaces, which induces controllable nonadiabatic effects. A joint exciton-motion pulse that is initially governed by a single energy surface is coherently split into two modes after crossing the intersection. The modes induce strongly different atomic motion, leading to clear signatures of nonadiabatic effects in atomic density profiles. We have shown how this scenario can be exploited as an exciton switch, controlling direction and coherence properties of the joint pulse on the second of the chains [K. Leonhardt et al., Phys. Rev. Lett. 113, 223001 (2014)]. In this article we discuss the underlying complex dynamics in detail, characterize the switch, and derive our isotropic interaction model from a realistic anisotropic one with the addition of a magnetic bias field.
We review Rydberg aggregates, assemblies of a few Rydberg atoms exhibiting energy transport through collective eigenstates, considering isolated atoms or assemblies embedded within clouds of cold ground-state atoms. We classify Rydberg aggregates, and provide an overview of their possible applications as quantum simulators for phenomena from chemical or biological physics. Our main focus is on flexible Rydberg aggregates, in which atomic motion is an essential feature. In these, simultaneous control over Rydberg-Rydberg interactions, external trapping and electronic energies, allows Born-Oppenheimer surfaces for the motion of the entire aggregate to be tailored as desired. This is illustrated with theory proposals towards the demonstration of joint motion and excitation transport, conical intersections and non-adiabatic effects. Additional flexibility for quantum simulations is enabled by the use of dressed dipole-dipole interactions or the embedding of the aggregate in a cold gas or Bose-Einstein condensate environment. Finally we provide some guidance regarding the parameter regimes that are most suitable for the realization of either static or flexible Rydberg aggregates based on Li or Rb atoms. The current status of experimental progress towards enabling Rydberg aggregates is also reviewed.
Abstract We review Rydberg aggregates, assemblies of a few Rydberg atoms exhibiting energy transport through collective eigenstates, considering isolated atoms or assemblies embedded within clouds of cold ground-state atoms. We classify Rydberg aggregates, and provide an overview of their possible applications as quantum simulators for phenomena from chemical or biological physics. Our main focus is on flexible Rydberg aggregates, in which atomic motion is an essential feature. In these, simultaneous control over Rydberg–Rydberg interactions, external trapping and electronic energies, allows Born–Oppenheimer surfaces for the motion of the entire aggregate to be tailored as desired. This is illustrated with theory proposals towards the demonstration of joint motion and excitation transport, conical intersections and non-adiabatic effects. Additional flexibility for quantum simulations is enabled by the use of dressed dipole–dipole interactions or the embedding of the aggregate in a cold gas or Bose–Einstein condensate environment. Finally we provide some guidance regarding the parameter regimes that are most suitable for the realization of either static or flexible Rydberg aggregates based on Li or Rb atoms. The current status of experimental progress towards enabling Rydberg aggregates is also reviewed.
Strong resonant dipole-dipole interactions in flexible Rydberg aggregates enable the formation of exciton pulses, the interplay of atomic motion and electronic excitation transfer which feature high fidelity entanglement transport. Here, we demonstrate the coherent splitting of such pulses into two modes, which induce strongly different atomic motion, leading to clear signatures of nonadiabatic effects in atomic density profiles. The mechanism exploits local nonadiabatic effects at a conical intersection, turning them from a decoherence source into an asset. The conical intersection is a consequence of the exciton pulses moving along a linear Rydberg chain and approaching an additional linear, perpendicularly aligned Rydberg chain. The intersection provides a sensitive knob controlling the propagation direction and coherence properties of exciton pulses. We demonstrate that this scenario can be exploited as an exciton switch, controlling direction and coherence properties of the joint pulse on the second of the chains. Initially, we demonstrate the pulse splitting on planar aggregates with atomic motion one-dimensionally constrained and employing isotropic interactions. Subsequently, we confirm the splitting mechanism for a fully realistic scenario in which all spatial restrictions are removed and the full anisotropy of the dipole-dipole interactions is taken into account. Our results enable the experimental observation of non-adiabatic electronic dynamics and entanglement transport with Rydberg atoms. The conical intersection crossings are clearly evident, both in atomic mean position information and excited state spectra of the Rydberg system. This suggests flexible Rydberg aggregates as a test-bench for quantum chemical effects in experiments on much-inflated length scales. The fundamental ideas discussed here have general implications for excitons on a dynamic network.
We consider the interplay between excitonic and atomic motion in a regular, flexible chain of Rydberg atoms, extending our recent results on entanglement transport in Rydberg chains (Wuster et al 2010 Phys. Rev. Lett. 105 053004). In such a Rydberg chain, similar to molecular aggregates, an electronic excitation is delocalized due to long-range dipole-dipole interactions among the atoms. The transport of an exciton that is initially trapped by a chain dislocation is strongly coupled to nuclear dynamics, forming a localized pulse of combined excitation and displacement. This pulse transfers entanglement between dislocated atoms adiabatically along the chain. Details about the interaction and the preparation of the initial state are discussed. We also present evidence that the quantum dynamics of this complex many-body problem can be accurately described by selected quantum-classical methods, which greatly simplify investigations of excitation transport in flexible chains.
We consider the interplay between excitonic and atomic motion in a regular, flexible chain of Rydberg atoms, extending our recent results on entanglement transport in Rydberg chains (Wüster et al 2010 Phys. Rev. Lett. 105 053004). In such a Rydberg chain, similar to molecular aggregates, an electronic excitation is delocalized due to long-range dipole–dipole interactions among the atoms. The transport of an exciton that is initially trapped by a chain dislocation is strongly coupled to nuclear dynamics, forming a localized pulse of combined excitation and displacement. This pulse transfers entanglement between dislocated atoms adiabatically along the chain. Details about the interaction and the preparation of the initial state are discussed. We also present evidence that the quantum dynamics of this complex many-body problem can be accurately described by selected quantum–classical methods, which greatly simplify investigations of excitation transport in flexible chains.