Spin-correlated exciton–polaritons in a van der Waals magnet

Dirnberger, Florian; Bushati, Rezlind; Datta, Biswajit; Kumar, Ajesh; MacDonald, Allan H.; Baldini, Edoardo; Menon, Vinod M.

doi:10.1038/s41565-022-01204-2

Cited by 46 publications

(41 citation statements)

References 27 publications

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“…32,33 Alternatively, to address magnetic systems, optical cavities have been combined with external drives, 28,29 or been used to modify a system's excited state properties. 30,31 While currently efforts are made to extend the cavity framework to a broader class of materials, and to construct a unified first principles description of cavity quantum fluctuations and quantum matter, 20,23,34 experiments demonstrating polaritonic control of materials are scarce. 35,36 Therefore, to transform this promising approach into a powerful experimental tool, it is of key importance to identify candidate materials where cavity engineering techniques can be explored.…”

Section: Introductionmentioning

confidence: 99%

Controlling the magnetic state of the proximate quantum spin liquid α-RuCl3 with an optical cavity

Boström

Sri

Claassen

et al. 2023

Preprint

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Harnessing the enhanced light-matter coupling and quantum vacuum fluctuations resulting from mode volume compression in optical cavities is a promising route towards functionalizing quantum materials and realizing exotic states of matter. Here, we extend cavity quantum electrodynamical materials engineering to correlated magnetic systems, by demonstrating that a Fabry-Perot cavity can be used to control the magnetic state of the proximate quantum spin liquid α-RuCl3. Depending on specific cavity properties such as the mode frequency, photon occupation, and strength of the light-matter coupling, any of the magnetic phases supported by the extended Kitaev model can be stabilized. In particular, in the THz regime, we show that the cavity vacuum fluctuations alone are sufficient to bring α-RuCl3 from a zigzag antiferromagnetic to a ferromagnetic state. By external pumping of the cavity in the few photon limit, it is further possible to push the system into the antiferromagnetic Kitaev quantum spin liquid state.

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Section: Introductionmentioning

confidence: 99%

Controlling the magnetic state of the proximate quantum spin liquid α-RuCl3 with an optical cavity

Boström

Sri

Claassen

et al. 2023

Preprint

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“…16 While the strongest peak is assigned to a chargetransfer state around 2.2 eV that persists even up to room temperature, 16 photoluminescence (PL) spectroscopy of bulk samples reveals a correlated exciton at lower energies (1.47 eV) that arises intrinsically from the many-body states of the Zhang-Rice singlet upon cooling below the Néel transition temperature TN (150 K). 21 This exciton is assigned to a spin-orbit entangled state (SO-X) displaying an ultra-narrow linewidth, 21 phonon-bound states, 20 spin-correlated behavior, 22 thickness-dependent PL, 21 polariton formation, 23 and can be controlled using light-pumping 24 and external magnetic fields. 22 However, to date, whether or not reduction of the lateral dimension influences these fascinating phenomena has not been explored.…”

Section: Introductionmentioning

confidence: 99%

Correlated Excitonic Signatures in a Nanoscale van der Waals Antiferromagnet

Htoon

Chandrasekaran

DeLaney

et al. 2023

Preprint

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Composite quasi-particles with emergent functionalities in spintronic and quantum information science can be realized in correlated materials due to entangled charge, spin, orbital, and lattice degrees of freedom.1-3 Here we show that by reducing the lateral dimension of correlated antiferromagnet NiPS3 flakes to tens of nanometers, we can switch-off the bulk spin-orbit entangled exciton in the near-infrared (1.47 eV)4-6 and activate visible-range (1.8 – 2.2 eV) transitions with charge-transfer character. These ultra-sharp lines (<120 meV at 4.2 K) share the spin-correlated nature of the bulk exciton by displaying a Néel temperature dependent linear polarization. Furthermore, exciton photoluminescence lineshape analysis reveals a polaronic character via coupling with at-least 3 phonon modes and a comb-like Stark effect through discretization of charges in each layer. These findings augment the knowledge on the many-body nature of excitonic quasi-particles in correlated antiferromagnets and also establish the nanoscale platform as promising for maturing integrated magneto-optic devices.

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“…Magnons have attracted renewed interest for several reasons. They can transport spin currents for applications in nondissipative spintronics, host topological order with chiral edge states, , form exotic collective states such as Bose condensates and spin superfluids; most important for the scope of this work, they can couple to photons. − …”

mentioning

confidence: 99%

Strongly Coupled Magnon–Plasmon Polaritons in Graphene-Two-Dimensional Ferromagnet Heterostructures

et al. 2023

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Magnons and plasmons are different collective modes, involving the spin and charge degrees of freedom, respectively. Formation of hybrid plasmon−magnon polaritons in heterostructures of plasmonic and magnetic systems faces two challenges, the small interaction of the electromagnetic field of the plasmon with the spins, and the energy mismatch, as in most systems plasmons have energies orders of magnitude larger than those of magnons. We show that graphene plasmons form polaritons with the magnons of two-dimensional ferromagnetic insulators, placed up to to half a micrometer apart, with Rabi splittings in the range of 100 GHz (dramatically larger than cavity magnonics). This is facilitated both by the small energy of graphene plasmons and the cooperative super-radiant nature of the plasmon−magnon coupling afforded by phase matching. We show that the coupling can be modulated both electrically and mechanically, and we propose a ferromagnetic resonance experiment implemented with a two-dimensional ferromagnet driven by graphene plasmons.

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Spin-correlated exciton–polaritons in a van der Waals magnet

Cited by 46 publications

References 27 publications

Controlling the magnetic state of the proximate quantum spin liquid α-RuCl3 with an optical cavity

Controlling the magnetic state of the proximate quantum spin liquid α-RuCl3 with an optical cavity

Correlated Excitonic Signatures in a Nanoscale van der Waals Antiferromagnet

Strongly Coupled Magnon–Plasmon Polaritons in Graphene-Two-Dimensional Ferromagnet Heterostructures

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