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arXiv:2602.18103

Polariton-polariton coherent coupling in a molecular spin-superconductor chip

Carolina del Río, Marcos Rubín-Osanz, David Rodriguez, Sebastián Roca-Jerat, María Carmen Pallarés, J. Alejandro de Sousa, Paweł Pakulski, José Luis García Palacios, Daniel Granados, Dawid Pinkowicz, Núria Crivillers, Anabel Lostao, David Zueco, Alicia Gomez, Fernando Luis

quant-phcond-mat.mes-hallSubmitted Feb 20, 2026• Announced Feb 23, 2026• 0 citations
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Abstract

The ability to establish coherent communication channels is key for scaling up quantum devices. Here, we engineer interactions between distant polaritons, hybrid spin-photon excitations formed at different lumped-element superconducting resonators within a chip. The chip consists of several resonator pairs, slightly detuned in frequency to make them addressable, capacitively coupled within each pair and inductively coupled to a common readout line. They interact locally with samples of PTMr and Tripak$^{-}$ organic free radicals, deposited onto their inductors, which provide model $S = 1/2$, $g \simeq 2$ spin ensembles. Frequency-dependent microwave transmission experiments, performed at very low temperatures, measure polariton frequencies as a function of magnetic field in different scenarios. When only one resonator within a pair hosts a molecular sample, the results evidence that spins couple remotely to the empty LER as well as to the local cavity mode. If both resonators interact with a spin ensemble, the magnetic field tunes the polariton frequencies relative to each other, on account of the different spin-photon interactions at each LER. When polaritons are brought into mutual resonance, an avoided level crossing emerges that gives direct spectroscopic evidence for a coherent polariton-polariton interaction mediated by the circuit. Pump-probe experiments reveal that the excitation of a polariton within a connected pair is felt, thus it can be read out, by the other one. These observations, backed by model calculations, illustrate the control and detection of distant photon-photon and spin-spin correlations and entanglement in a scalable modular chip.

Comments
27 pages, 28 figures

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The ability to establish coherent communication channels is key for scaling up quantum devices. Here, we engineer interactions between distant polaritons, hybrid spin-photon excitations formed at different lumped-element superconducting resonators within a chip. The chip consists of several resonator pairs, slightly detuned in frequency to make them addressable, capacitively coupled within each pair and inductively coupled to a common readout line. They interact locally with samples of PTMr and Tripak−^{-}− organic free radicals, deposited onto their inductors, which provide model S=1/2S = 1/2S=1/2, g≃2g \simeq 2g≃2 spin ensembles. Frequency-dependent microwave transmission experiments, performed at very low temperatures, measure polariton frequencies as a function of magnetic field in different scenarios. When only one resonator within a pair hosts a molecular sample, the results evidence that spins couple remotely to the empty LER as well as to the local cavity mode. If both resonators interact with a spin ensemble, the magnetic field tunes the polariton frequencies relative to each other, on account of the different spin-photon interactions at each LER. When polaritons are brought into mutual resonance, an avoided level crossing emerges that gives direct spectroscopic evidence for a coherent polariton-polariton interaction mediated by the circuit. Pump-probe experiments reveal that the excitation of a polariton within a connected pair is felt, thus it can be read out, by the other one. These observations, backed by model calculations, illustrate the control and detection of distant photon-photon and spin-spin correlations and entanglement in a scalable modular chip.
We study the simultaneous interaction of a sample of organic free radicals, which realize the spin-1/2 model with a quasi-isotropic g factor ≈ 2, with three ≈ 5.5 GHz lumped-element superconducting resonators in a chip. Each resonator consists of a finger capacitor in parallel with a single wire inductor, which maximizes the coupling intensity of the spins to the photon magnetic field. Their frequencies have been detuned relative to one another in order to make them individually addressable. Each resonator within the trio is capacitively coupled to its nearest neighbor and inductively coupled to a common readout transmission line, and only the central one hosts a molecular deposit. The device has been characterized by microwave transmission experiments performed as a function of frequency (between 5.3 and 5.7 GHz) and magnetic field (170–220 mT) at very low temperatures (T ≃ 13 mK). The results evidence a strong local interaction of the spins to the central resonator, which reaches the coherent coupling regime. In addition, they show that the same spins also couple to the modes associated with the distant resonators. These data have been analyzed on the basis of a theoretical model that incorporates the direct spin-photon interactions as well as those mediated by the circuit. The results provide a relatively simple, practical method for investigating spin resonance of a material at multiple frequencies. Besides, this method allows designing each resonator differently, to fulfill a specific role, e.g., for optimized control or readout of the spin states, which can be of relevance for the implementation of hybrid quantum computation schemes based on molecular spin qubits.
A promising route toward the realization of a molecular spin quantum processor relies on coupling magnetic molecules to individual photons confined within superconducting resonators. As a simple approximation to such a hybrid scheme, here we explore the conditions that determine the collective coupling of DPPH organic free radicals to lumped-element LC superconducting resonators. In these chips, multiple resonators are coupled to a single readout line. This enables designing the relevant resonator properties, such as resonance frequency, cavity volume, and impedance while keeping a perfect transmission for the device. Here, we exploit these design possibilities to achieve a coherent spin-photon coupling regime. Besides, we study how this coupling depends on the relative orientation of the external dc magnetic field concerning the photon magnetic field and the spins locations concerning the chip surface.
We engineer lumped-element superconducting resonators that maximize magnetic coupling to molecular spin qubits, achieving record single-spin couplings up to 100100100 kHz and collective couplings exceeding 101010 MHz. The resonators interact with PTMr organic free radicals, model spin systems with S=1/2S=1/2S=1/2 and a quasi-isotropic g≃2g \simeq 2g≃2, dispersed in polymer matrices. The highest collective spin-photon coupling strengths are attained with resonators having large inductors, which therefore interact with most spins in the molecular ensemble. By contrast, the coupling of each individual spin G1G_{1}G1​ is maximized in resonators having a minimum size inductor, made of a single wire. The same platform has been used to study spin relaxation and spin coherent dynamics in the dispersive regime, when spins are energetically detuned from the resonator. We find evidences for the Purcell effect, i.e. the photon induced relaxation of those spins that are most strongly coupled to the circuit. The rate of this process gives access to the distribution of single spin photon couplings in a given device. For resonators with a 505050 nm wide constriction at the inductor center, single maximum G1G_{1}G1​ values reach ∼100\sim 100∼100 kHz. Pumping the spins with strong pulses fed through an independent transmission line induces coherent Rabi oscillations. The spin excitation then proceeds via either direct resonant processes induced by the main pulse frequency or, in the case of square-shaped pulses, via the excitation of the cavity by sideband frequency components. The latter process measures the cavity mode hybridization with the spins and can be eliminated by using Gaussian shaped pulses. These results establish a scalable route toward integrated molecular-spin quantum processors.
Within the quest for solid state quantum systems to be used for fundamental as well as applied research, molecular spins have recently emerged as a versatile platform with interesting performances in terms of quantum coherence and correlation. Molecular units provide well defined environment to electronic spins and they represent elementary bricks for complex nano-architectures and nano-devices. Here we review our recent efforts and results on their efficient integration in circuit Quantum ElectroDynamics and, more specifically, in reaching their coherent coupling with microwave photons in planar resonators. To monitor molecular spin performances over a wide temperature and magnetic field range we have first developed microwave planar resonators made of high T c superconductors, obtaining excellent performances up to liquid Nitrogen temperature and in magnetic fields up to 7 Tesla. Ensembles of different molecular spins systems are then systematically tested. The regime of high spin-photon cooperativity is achieved with molecular spins diluted in non-magnetic matrix at 0.5 K, while the strong coupling regime is observed with concentrated samples of organic radicals up to 50 K. The possibility to create coherent states among distinct spin ensembles is further explored in similar spectroscopic experiments. These results show that molecular spins can be efficiently integrated in quantum devices.
We implement superconducting Yttrium barium copper oxide planar resonators with two fundamental modes for circuit quantum electrodynamics experiments. We first demonstrate good tunability in the resonant microwave frequencies and in their interplay, as emerges from the dependence of the transmission spectra on the device geometry. We then investigate the magnetic coupling of the resonant modes with bulk samples of 2,2-diphenyl-1-picrylhydrazyl organic radical spins. The transmission spectroscopy performed at low temperature shows that the coherent spin-photon coupling regime with the spin ensembles can be achieved by each of the resonator modes. The analysis of the results within the framework of the input-output formalism and by means of entropic measures demonstrates coherent mixing of the degrees of freedom corresponding to two remote spin ensembles and, with a suitable choice of the geometry, the approaching of a regime with spin-induced mixing of the two photon modes.
Superconducting qubits are fabricated "loss-free" electrical circuits on a chip with size features of tens of nanometers. If cooled to cryogenic temperatures below -273 °C they behave as quantum elements, similar to atoms and molecules. Such a qubit can be manipulated by fast-oscillating magnetic fields and its resulting quantum state can be measured using a proper magnetic detector. These qubits could be the basic elements for a quantum processor. To that order, multiple qubits have to controllably interact, and to that purpose very high quality resonators are fabricated on the same chip. Effectively the interaction results from the phase-coherent exchange of a single photon between qubit and resonator. In this way it is highly analogous to the so-called cavity QED in atomic physics where single atoms couple to a single trapped photon, all inside a cavity resonator. In this thesis, a superconducting flux qubit has been coupled to an LC resonator and coherent exchange of a single photon between qubit and resonator has been achieved. A striking option in these superconducting circuits, not attainable in "common" atomic cavity-QED, is that the interaction between qubit and photon can be made very large, up to the limit that one no longer can talk about the qubit and resonator as such. This limit requires a fully different description and it leads to novel effects, e.g. in the energy spectrum of the qubit-resonator composite. The Bloch-Siegert spectral shift is experimentally demonstrated in this thesis. As a small but critical technical aside a new type of control line filter has been developed, which allows strong suppression of excess electrical noise that forms a threat for qubit coherence. Having two modes of operation, it shorts all low-frequency noise if control is idle while being transparent if control is active, where short or open is determined by the control line signal level itself.