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npj Quantum Information

Room-temperature cavity quantum electrodynamics with strongly coupled Dicke states

Jonathan Breeze, Enrico Salvadori, Juna Sathian, Neil McN. Alford, Christopher W. M. Kay

Published Sep 20, 2017• 45 citations
Publisher

Abstract

Abstract The strong coupling regime is essential for efficient transfer of excitations between states in different quantum systems on timescales shorter than their lifetimes. The coupling of single spins to microwave photons is very weak but can be enhanced by increasing the local density of states by reducing the magnetic mode volume of the cavity. In practice, it is difficult to achieve both small cavity mode volume and low cavity decay rate, so superconducting metals are often employed at cryogenic temperatures. For an ensembles of N spins, the spin–photon coupling can be enhanced by $$\sqrt N$$ N through collective spin excitations known as Dicke states. For sufficiently large N the collective spin–photon coupling can exceed both the spin decoherence and cavity decay rates, making the strong-coupling regime accessible. Here we demonstrate strong coupling and cavity quantum electrodynamics in a solid-state system at room-temperature. We generate an inverted spin-ensemble with N ~ 1015 by photo-exciting pentacene molecules into spin-triplet states with spin dephasing time $$T_2^*\sim 3$$ T 2 * ~ 3 μs. When coupled to a 1.45 GHz TE01δ mode supported by a high Purcell factor strontium titanate dielectric cavity ( $$V_{\mathrm{m}}\sim 0.25$$ V m ~ 0.25 cm3, Q ~ 8,500), we observe Rabi oscillations in the microwave emission from collective Dicke states and a 1.8 MHz normal-mode splitting of the resultant collective spin–photon polariton. We also observe a cavity protection effect at the onset of the strong-coupling regime which decreases the polariton decay rate as the collective coupling increases.

DOI
10.1038/s41534-017-0041-3

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Abstract The strong coupling regime is essential for efficient transfer of excitations between states in different quantum systems on timescales shorter than their lifetimes. The coupling of single spins to microwave photons is very weak but can be enhanced by increasing the local density of states by reducing the magnetic mode volume of the cavity. In practice, it is difficult to achieve both small cavity mode volume and low cavity decay rate, so superconducting metals are often employed at cryogenic temperatures. For an ensembles of N spins, the spin–photon coupling can be enhanced by N\sqrt NN​ N through collective spin excitations known as Dicke states. For sufficiently large N the collective spin–photon coupling can exceed both the spin decoherence and cavity decay rates, making the strong-coupling regime accessible. Here we demonstrate strong coupling and cavity quantum electrodynamics in a solid-state system at room-temperature. We generate an inverted spin-ensemble with N ~ 1015 by photo-exciting pentacene molecules into spin-triplet states with spin dephasing time T2∗∼3T_2^*\sim 3T2∗​∼3 T 2 * ~ 3 μs. When coupled to a 1.45 GHz TE01δ mode supported by a high Purcell factor strontium titanate dielectric cavity ( Vm∼0.25V_{\mathrm{m}}\sim 0.25Vm​∼0.25 V m ~ 0.25 cm3, Q ~ 8,500), we observe Rabi oscillations in the microwave emission from collective Dicke states and a 1.8 MHz normal-mode splitting of the resultant collective spin–photon polariton. We also observe a cavity protection effect at the onset of the strong-coupling regime which decreases the polariton decay rate as the collective coupling increases.
Strong coupling of light and matter is an essential element of cavity quantum electrodynamics (cavity-QED) and quantum optics, which may lead to novel mixed states of light and matter and to applications such as quantum computation. In the strong-coupling regime, where the coupling strength exceeds the dissipation, the light-matter interaction produces a characteristic vacuum Rabi splitting. Therefore, strong coupling can be utilized as an effective coherent interface between light and matter (in the form of electron charge, spin or superconducting Cooper pairs) to achieve components of quantum information technology including quantum memory, teleportation, and quantum repeaters. Semiconductor quantum dots, nuclear spins and paramagnetic spin systems are only some of the material systems under investigation for strong coupling in solid-state physics. Mixed states of light and matter coupled via electric dipole transitions often suffer from short coherence times (nanoseconds). Even though magnetic transitions appear to be intrinsically more quantum coherent than orbital transitions, their typical coupling strengths have been estimated to be much smaller. Hence, they have been neglected for the purposes of quantum information technology.\nHowever, we predict that strong coupling is feasible between photons and a ferromagnetic nanomagnet, due to exchange interactions that cause very large numbers of spins to coherently lock together with a significant increase in oscillator strength while still maintaining very long coherence times. In order to examine this new exciting possibility, the interaction of a ferromagnetic nanomagnet with a single photonic mode of a cavity is analyzed in a fully quantum-mechanical treatment. Exceptionally large quantum-coherent magnet-photon coupling with coupling terms in excess of several THz are predicted to be achievable in a spherical cavity of ∼ 1 mm radius with a nanomagnet of ∼ 100 nm radius and ferromagnet resonance frequency of ∼ 200 GHz. This should substantially exceed the coupling observed in solids between orbital transitions and light. Eigenstates of the nanomagnet-photon system correspond to entangled states of spin orientation and photon number over 105 values of each quantum number. Initial coherent state of definite spin and photon number evolve dynamically to produce large coherent oscillations in the microwave power with exceptionally long dephasing times of few seconds. In addition to dephasing, several decoherence mechanisms including elementary excitation of magnons and crystalline magnetic anisotropy are investigated and shown to not substantially affect coherence upto room temperature. For small nanomagnets the crystalline magnetic anisotropy of the magnet strongly localize the eigenstates in photon and spin number, quenching the potential for coherent states and for a sufficiently large nanomagnet the macrospin approximation breaks down and different domains of the nanomagnet may couple separately to the photonic mode. Thus the optimal nanomagnet size is predicted to be just below the threshold for failure of the macrospin approximation. Moreover, it is shown that initially unentangled coherent states of light (cavity field) and spin (nanomagnet spin orientation) can be phase-locked to evolve into a coherent entangled states of the system under the influence of strong coupling.
An ensemble of N noninteracting spins being in thermal equilibrium and coupled to the resonant mode of a lossless microwave cavity is studied as the function of the spin temperature τ. Near τ = 0 the system is known to be in a coupled spin-photon state that manifests itself by the splitting of the cavity mode (vacuum Rabi splitting). The cavity emission spectrum is simulated for arbitrary τ. A critical temperature τ C = ω S √N/2, where ω S is the spin excitation energy, is related to the destruction of the strong coupling regime as a consequence of thermal excitations arising within the spin ensemble.
Recent experiments demonstrated the cooling of a microwave mode of a high-quality dielectric resonator coupled to optically cooled nitrogen-vacancy (NV) spins in diamond. Our recent theoretical study [arXiv:2110.10950] pointed out the cooled NV spins can be used to realize cavity quantum electrodynamics effects (C-QED) at room temperature. In this article, we propose to modify the setup used in a recent diamond maser experiment [Nature 55, 493-496 (2018)], which features a higher spin transition frequency, a lower spin-dephasing rate and a stronger NV spins-resonator coupling, to realize better microwave mode cooling and the room-temperature CQED effects. To describe more precisely the optical spin cooling and the collective spin-resonator coupling, we extend the standard Jaynes-Cumming model to account for the rich electronic and spin levels of the NV centers. Our calculations show that for the proposed setup it is possible to cool the microwave mode from 293293293 K (room temperature) to 116116116 K, which is about 727272 K lower than the previous records, and to study the intriguing dynamics of the CQED effects under the weak-to-strong coupling transition by varying the laser power. With simple modifications, our model can be applied to, e.g., other solid-state spins or triplet spins of pentacene molecules, and to investigate other effects, such as the operations of pulsed and continuous-wave masing.
Abstract Hybridizing collective spin excitations and a cavity with high cooperativity provides a new research subject in the field of cavity quantum electrodynamics and can also have potential applications to quantum information. Here we report an experimental study of cavity quantum electrodynamics with ferromagnetic magnons in a small yttrium-iron-garnet (YIG) sphere at both cryogenic and room temperatures. We observe for the first time a strong coupling of the same cavity mode to both a ferromagnetic-resonance (FMR) mode and a magnetostatic (MS) mode near FMR in the quantum limit. This is achieved at a temperature ~22 mK, where the average microwave photon number in the cavity is less than one. At room temperature, we also observe strong coupling of the cavity mode to the FMR mode in the same YIG sphere and find a slight increase of the damping rate of the FMR mode. These observations reveal the extraordinary robustness of the FMR mode against temperature. However, the MS mode becomes unobservable at room temperature in the measured transmission spectrum of the microwave cavity containing the YIG sphere. Our numerical simulations show that this is due to a drastic increase of the damping rate of the MS mode.
Quantum sensors have the potential to operate at fundamental physical performance limits. Among various quantum sensing platforms, solid-state spin emitters stand out due to advantageous characteristics such as room-temperature spin polarization and readout, atomic-scale spatial resolution, and extended coherence times. Despite these strengths, traditional optical detection methods exhibit low readout fidelity in solid-state ensembles, severely limiting their achievable sensitivity. This thesis addresses this limitation by coupling a solid-state emitter ensemble to a microwave cavity, forming a cavity quantum electrodynamics system. Our approach eliminates the need for photon collection required by conventional optical readout methods, and the resulting strongly coupled system allows efficient cavity-based probing of the solid-state spin ensemble. By exploiting the hybrid quantum system with cavity quantum electrodynamics, we achieve record-high sensitivity for solid-state quantum sensors, representing a substantial advancement toward achieving fundamental sensing limits.
We study the nonlinear dynamics of an ensemble of cold trapped atoms with a hyperfine transition magnetically coupled to a resonant microwave cavity mode. Despite the minute single-atom coupling, one obtains strong coupling between collective hyperfine qubits and microwave photons, enabling coherent transfer of an excitation between the long-lived atomic qubit state and the mode. Evidence of strong coupling can be obtained from the cavity transmission spectrum even at finite thermal photon number. The system makes it possible to study further prominent collective phenomena such as superradiant decay of an inverted ensemble or the building of a narrowband stripline micromaser locked to an atomic hyperfine transition.