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arXiv:1310.6975 · Physical Review Letters

Switching Exciton Pulses Through Conical Intersections

Karsten Leonhardt, Sebastian Wüster, Jan Michael Rost

Published Nov 24, 2014• 18 citations
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Abstract

Exciton pulses transport excitation and entanglement adiabatically through Rydberg aggregates, assemblies of highly excited light atoms, which are set into directed motion by resonant dipole-dipole interaction. Here, we demonstrate the coherent splitting of such pulses as well as the spatial segregation of electronic excitation and atomic motion. Both mechanisms exploit local nonadiabatic effects at a conical intersection, turning them from a decoherence source into an asset. The intersection provides a sensitive knob controlling the propagation direction and coherence properties of exciton pulses. The fundamental ideas discussed here have general implications for excitons on a dynamic network.

DOI
10.1103/physrevlett.113.223001

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Exciton pulses transport excitation and entanglement adiabatically through Rydberg aggregates, assemblies of highly excited light atoms, which are set into directed motion by resonant dipole-dipole interaction. Here, we demonstrate the coherent splitting of such pulses as well as the spatial segregation of electronic excitation and atomic motion. Both mechanisms exploit local nonadiabatic effects at a conical intersection, turning them from a decoherence source into an asset. The intersection provides a sensitive knob controlling the propagation direction and coherence properties of exciton pulses. The fundamental ideas discussed here have general implications for excitons on a dynamic network.
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 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 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.
Abstract We demonstrate that through localised Rydberg excitation in a three-dimensional cold atom cloud atomic motion can be rendered directed and nearly confined to a plane, without spatial constraints for the motion of individual atoms. This enables creation and observation of non-adiabatic electronic Rydberg dynamics in atoms accelerated by dipole–dipole interactions under natural conditions. Using the full l = 0, 1 m = 0 , ± 1 angular momentum state space, our simulations show that conical intersection crossings are clearly evident, both in atomic position information and excited state spectra of the Rydberg system. Hence, flexible Rydberg aggregates suggest themselves for probing quantum chemical effects in experiments on length scales much inflated as compared to a standard molecular situation.
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.