Preparation and coherent manipulation of toroidal moments in molecules

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Hauptverfasser: Hymas, Kieran, Soncini, Alessandro
Format: Preprint
Veröffentlicht: 2025
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author Hymas, Kieran
Soncini, Alessandro
author_facet Hymas, Kieran
Soncini, Alessandro
contents Molecules with an odd number of electrons typically display paramagnetic behaviour in a uniform magnetic field. Single-molecule toroics -- a family of open shell lanthanide complexes -- instead display an unprecedented vanishing magnetization. The anomaly is reconciled by degenerate quantum states where electron spins and orbital currents give rise to time-odd and space-odd magnetic vortices known as toroidal moments, that carry a vanishing magnetic dipole. Resilient to stray magnetic fields and susceptible to electric manipulation, toroidal moments have attracted interest for spintronic, magnonic, and photonic applications. While macroscopic toroidal moments feature in some extended systems, molecular toroidal states have yet to be observed, as it remains unclear how existing experimental set-ups could split degenerate states carrying counter-rotating vortices. We propose a realistic pulsed radiation protocol to polarise and observe molecular toroidal moments in a class of MDy$_6$ (M = Al$^{3+}$, Cr$^{3+}$) molecules with coupled Dy$_3$ toroidal moieties. Three resonant MW-pulses -- delivered sequentially or simultaneously -- selectively and coherently transfers population to a long-lived toroidally-polarised state whose ensuing magneto-electric properties provide a read-out mechanism. Our results provide a strategy to measure and coherently manipulate toroidal states in molecular systems, which is expected to trigger applications of molecular toroidal states to quantum technologies.
format Preprint
id arxiv_https___arxiv_org_abs_2504_08701
institution arXiv
publishDate 2025
record_format arxiv
spellingShingle Preparation and coherent manipulation of toroidal moments in molecules
Hymas, Kieran
Soncini, Alessandro
Mesoscale and Nanoscale Physics
Molecules with an odd number of electrons typically display paramagnetic behaviour in a uniform magnetic field. Single-molecule toroics -- a family of open shell lanthanide complexes -- instead display an unprecedented vanishing magnetization. The anomaly is reconciled by degenerate quantum states where electron spins and orbital currents give rise to time-odd and space-odd magnetic vortices known as toroidal moments, that carry a vanishing magnetic dipole. Resilient to stray magnetic fields and susceptible to electric manipulation, toroidal moments have attracted interest for spintronic, magnonic, and photonic applications. While macroscopic toroidal moments feature in some extended systems, molecular toroidal states have yet to be observed, as it remains unclear how existing experimental set-ups could split degenerate states carrying counter-rotating vortices. We propose a realistic pulsed radiation protocol to polarise and observe molecular toroidal moments in a class of MDy$_6$ (M = Al$^{3+}$, Cr$^{3+}$) molecules with coupled Dy$_3$ toroidal moieties. Three resonant MW-pulses -- delivered sequentially or simultaneously -- selectively and coherently transfers population to a long-lived toroidally-polarised state whose ensuing magneto-electric properties provide a read-out mechanism. Our results provide a strategy to measure and coherently manipulate toroidal states in molecular systems, which is expected to trigger applications of molecular toroidal states to quantum technologies.
title Preparation and coherent manipulation of toroidal moments in molecules
topic Mesoscale and Nanoscale Physics
url https://arxiv.org/abs/2504.08701