Optical Activity from the Exciton Aharonov-Bohm Effect: A Floquet Engineering Approach

Abstract

Floquet engineering is a convenient strategy to induce nonequilibrium phenomena in molecular and solid-state systems, or to dramatically alter the physicochemical properties of matter, bypassing costly and time-consuming synthetic modifications. In this article, we investigate theoretically some interesting consequences of the fact that an originally achiral molecular system can exhibit nonzero circular dichroism (CD) when it is driven with elliptically polarized light. More specifically, we consider an isotropic ensemble of small cyclic molecular aggregates in solution whose local low-frequency vibrational modes are driven by an elliptically polarized continuous-wave infrared pump. We attribute the origin of a nonzero CD signal to time-reversal symmetry breaking due to an excitonic Aharonov-Bohm (AB) phase arising from a time-varying laser electric field, together with coherent interchromophoric exciton hopping. The obtained Floquet engineered excitonic AB phases are far more tunable than analogous magnetically-induced electronic AB phases in nanoscale rings, highlighting a virtually unexplored potential that Floquet engineered AB phases have in the coherent control of molecular processes and simultaneously introducing new analogues of magneto-optical effects in molecular systems which bypass the use of strong magnetic fields.

References in corpus (20)

• Room-Temperature Quantum Hall Effect in Graphene
• Imaging topological edge states in silicon photonics
• Observation of Floquet-Bloch states on the surface of a topological insulator
• Floquet Engineering of Quantum Materials
• Polarized excitons in nanorings and the `optical' Aharonov-Bohm effect
• Enhancement of Vibronic and Ground-State Vibrational Coherences in 2D Spectra of Photosynthetic Complexes
• Aharonov-Bohm effect of excitons in nano-rings
• Coupled-cluster theory for atoms and molecules in strong magnetic fields
• Optical Aharonov-Bohm effect in stacked type-II quantum dots
• Topologically protected excitons in porphyrin thin films
• Aharonov-Bohm effect in the tunnelling of a quantum rotor in a linear Paul trap
• Periodic array of quantum rings strongly coupled to circularly polarized light as a topological insulator
• Optical absorption properties of laser-dressed matter
• Control of Excitation Energy Transfer in Condensed Phase Molecular Systems by Floquet Engineering
• Optically induced Aharonov-Bohm effect in mesoscopic rings
• Aharonov-Bohm effect for excitons in a semiconductor quantum ring dressed by circularly polarized light
• Aharonov-Bohm effect for an exciton in a finite width nano-ring
• Calculations of Nonlinear Wave-Packet Interferometry Signals in the Pump-Probe Limit as Tests for Vibrational Control over Electronic Excitation Transfer
• Control of Quantum Dynamics of Electron Transfer in Molecular Loop Structures: Spontaneous Breaking of Chiral Symmetry under Strong Decoherence
• Strong magneto-optical response enabled by quantum two level systems

Cited by in corpus (4)

• Chiral topological light for detecting robust enantio-sensitive observables
• On the Proper Derivation of the Floquet-based Quantum Classical Liouville Equation and Surface Hopping Describing a Molecule or Material Subject to an External Field
• Floquet engineering of molecular dynamics via infrared coupling
• Molecular and solid-state topological polaritons induced by population imbalance