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Fernando Luis

Publications and source records attributed to Fernando Luis.

At least 19 recordsLinked to original sources

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

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.

quant-ph

Optimizing magnetic coupling in lumped element superconducting resonators for molecular spin qubits

We engineer lumped-element superconducting resonators that maximize magnetic coupling to molecular spin qubits, achieving record single-spin couplings up to $100$ kHz and collective couplings exceeding $10$ MHz. The resonators interact with PTMr organic free radicals, model spin systems with $S=1/2$ and a quasi-isotropic $g \simeq 2$, 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 $G_{1}$ 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 $50$ nm wide constriction at the inductor center, single maximum $G_{1}$ values reach $\sim 100$ 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.

quant-ph

Transformer Wave Function for Quantum Long-Range models

We employ a neural-network architecture based on the Vision Transformer (ViT) architecture to find the ground states of quantum long-range models, specifically the transverse-field Ising model for spin-1/2 chains across different interaction regimes. Harnessing the transformer's capacity to capture long-range correlations, we compute the full phase diagram and critical properties of the model, in both the ferromagnetic and antiferromagnetic cases. Our findings show that the ViT maintains high accuracy across the full phase diagram. We compare these results with previous numerical studies in the literature and, in particular, show that the ViT has a superior performance than a restricted-Boltzmann-machine-like ansatz.

quant-ph

Linear response theory for cavity QED materials at arbitrary light-matter coupling strengths

We develop a linear response theory for materials collectively coupled to a cavity that is valid in all regimes of light-matter coupling, including symmetry-broken phases. We present and compare two different approaches. First, using a coherent path integral formulation for the partition function to obtain thermal Green functions. This approach relies on a saddle point expansion for the action, that can be truncated in the thermodynamic limit. Second, by formulating the equations of motion for the retarded Green functions and solving them. We use a mean-field decoupling of high-order Green functions in order to obtain a closed, solvable system of equations. Both approaches yield identical results in the calculation of response functions for the cavity and material. These are obtained in terms of the bare cavity and material responses. In combination, the two techniques clarify the validity of a mean-field decoupling in correlated light-matter systems and provide complementary means to compute finite-size corrections to the thermodynamic limit. The theory is formulated for a general model that encompasses most of the systems typically considered in the field of cavity QED materials. Finally, we provide a detailed application of the theory to the Quantum Hall effect and to a collection of spin models.

quant-ph

Bound polariton states in the Dicke-Ising model

We present a study of hybrid light-matter excitations in cavity QED materials using the Dicke-Ising model as a theoretical framework. Leveraging linear response theory, we derive the exact excitations of the system in the thermodynamic limit. Our results demonstrate that the cavity can localize spin excitations, leading to the formation of bound polaritons, where the cavity acts as an impurity of the two-excitation band, localizing spin-wave pairs around single-spin domains. We derive the condition for the existence of these bound states and discuss its satisfiability in different regimes. Finally, we show that these effects persist in finite systems using exact-diagonalization calculations.

quant-ph

Waveguide quantum electrodynamics at the onset of spin-spin correlations

We explore the competition between light-mediated and intrinsic matter-matter interactions in waveguide quantum electrodynamics. For this, we couple a superconducting transmission line to a model magnetic material, made of organic free radical molecules with a spin $S=1/2$ and a $g_{S}$ factor very close to that of a free electron. The microwave transmission has been measured in a wide range of temperatures ($0.013$ K $\leq T \leq 2$ K), magnetic fields ($0\leq B \leq 0.5$ T) and frequencies ($0 \leq \omega/2 \pi \leq 14$ GHz). We find that molecules belonging to one of the two crystal sublattices form one-dimensional spin chains. Temperature then controls the intrinsic correlations along these chains in a continuous and monotonic way. In the paramagnetic region ($T > 0.7$ K), the microwave transmission shows evidences for the collective coupling of quasi-identical spins to the propagating photons, with coupling strengths that reach values close to the dissipation rates. As $T$ decreases, the growth of spin correlations, combined with the anisotropy in the spin-spin exchange constants, tend to suppress the collective spin-photon coupling. In this regime, the spin visibility in transmission reflects also a gradual change in the nature of the dominant spin excitations, from single spin flips to bosonic magnons.

quant-ph

Optimal Control of Spin Qudits Subject to Decoherence Using Amplitude-and-Frequency-Constrained Pulses

Quantum optimal control theory (QOCT) can be used to design the shape of electromagnetic pulses that implement operations on quantum devices. By using non-trivially shaped waveforms, gates can be made significantly faster than those built by concatenating monochromatic pulses. Recently, we applied this technique to the control of molecular spin qudits modelled with Schr\"odinger's equation and showed it can speed up operations, helping mitigate the effects of decoherence [Phys. Rev. Appl. 17, 064028 (2022)]. However, short gate times result in large optimal pulse amplitudes, which may not be experimentally accessible. Introducing bounds to the amplitudes then unavoidably leads to longer operation times, for which decoherence can no longer be neglected. Here, we study how to improve this procedure by applying QOCT on top of Lindblad's equation, to design control pulses accounting for decoherence already in the optimization process. In addition, we introduce a formulation that allows us to bound the maximum amplitude and frequency of the signals, which are the typical limitations of waveform generators. The pulses we obtain consistently enhance operation fidelities compared to those achieved with Schr\"odinger's equation across various target gates and durations, demonstrating the flexibility and robustness of our method. The improvement is larger the shorter the spin coherence time $T_{2}$.

quant-ph

Measuring the magnon-photon coupling in shaped ferromagnets: tuning of the resonance frequency

Cavity photons and ferromagnetic spins excitations can exchange information coherently in hybrid architectures, at speeds set by their mutual coupling strength. Speed enhancement is usually achieved by optimizing the geometry of the electromagnetic cavity. Here we show that the geometry of the ferromagnet plays also an important role, by setting the fundamental frequency of the magnonic resonator. Using focused ion beam patterning, we vary the aspect ratio of different Permalloy samples reaching operation frequencies above 10 GHz while working at low external magnetic fields. Additionally, we perform broad band ferromagnetic resonance measurements and cavity experiments that demonstrate that the magnon-photon coupling strength can be estimated using either open transmission lines or resonant cavities, yielding very good agreement. Finally, we describe a simple theoretical framework based on electromagnetic and micromagnetic simulations that successfully accounts for the experimental results. This approach can be used to design hybrid quantum systems exploiting whatsoever magnetostatic mode excited in ferromagnets of arbitrary size and shape and to tune their operation conditions.

cond-mat.mes-hall

Optimal control of molecular spin qudits

We demonstrate, numerically, the possibility of manipulating the spin states of molecular nanomagnets with shaped microwave pulses designed with quantum optimal control theory techniques. The state-to-state or full gate transformations can be performed in this way in shorter times than using simple monochromatic resonant pulses. This enhancement in the operation rates can therefore mitigate the effect of decoherence. The optimization protocols and their potential for practical implementations are illustrated by simulations performed for a simple molecular cluster hosting a single Gd$^{3+}$ ion. Its eight accessible levels (corresponding to a total spin $S=7/2$) allow encoding an $8$-level qudit or a system of three coupled qubits. All necessary gates required for universal operation can be obtained with optimal pulses using the intrinsic couplings present in this system. The application of optimal control techniques can facilitate the implementation of quantum technologies based on molecular spin qudits.

quant-ph

Dispersive readout of molecular spin qudits

We study the physics of a magnetic molecule described by a "giant" spin with multiple ($d > 2$) spin states interacting with the quantized cavity field produced by a superconducting resonator. By means of the input-output formalism, we derive an expression for the output modes in the dispersive regime of operation. It includes the effect of magnetic anisotropy, which makes different spin transitions addressable. We find that the measurement of the cavity transmission allows to uniquely determine the spin state of the qudits. We discuss, from an effective Hamiltonian perspective, the conditions under which the qudit read-out is a non-demolition measurement and consider possible experimental protocols to perform it. Finally, we illustrate our results with simulations performed for realistic models of existing magnetic molecules.

quant-ph

Chemical tuning of spin clock transitions in molecular monomers based on nuclear spin-free Ni(II)

We report the existence of a sizeable quantum tunnelling splitting between the two lowest electronic spin levels of mononuclear Ni complexes. The level anti-crossing, or magnetic clock transition, associated with this gap has been directly monitored by heat capacity experiments. The comparison of these results with those obtained for a Co derivative, for which tunnelling is forbidden by symmetry, shows that the clock transition leads to an effective suppression of intermolecular spin-spin interactions. In addition, we show that the quantum tunnelling splitting admits a chemical tuning via the modification of the ligand shell that determines the crystal field and the magnetic anisotropy. These properties are crucial to realize model spin qubits that combine the necessary resilience against decoherence, a proper interfacing with other qubits and with the control circuitry and the ability to initialize them by cooling.

quant-ph

Photon Condensation and Enhanced Magnetism in Cavity QED

A system of magnetic molecules coupled to microwave cavities ($LC$ resonators) undergoes the equilibrium superradiant phase transition. The transition is experimentally observable. The effect of the coupling is first illustrated by the vacuum-induced ferromagnetic order in a quantum Ising model and then by the modification of the magnetic phase diagram of ${\rm Fe_8}$ dipolar crystals, exemplifying the cooperation between intrinsic and photon-induced spin-spin interactions. Finally, a transmission experiment is shown to resolve the transition, measuring the quantum electrodynamical control of magnetism.

quant-ph

A dissymmetric [Gd$_{2}$] coordination molecular dimer hosting six addressable spin qubits

Artificial magnetic molecules are suitable hosts to one or several spin qubits, which could then implement small-scale algorithms. In order to become of practical use, such molecular spin processors need to increase the dimension $d$ of the available computational space and fulfill the highly demanding conditions that warrant universal operations. Here, we design, synthesize and fully characterize dissymetric molecular dimers hosting either one or two Gd(III) ions. The strong sensitivity of Gd(III) magnetic anisotropy to the symmetry of its local coordination gives rise to different zero-field splittings at each coordination site. As a result, the [LaGd] and [GdLu] complexes provide realizations of distinct $d = 8$ spin qudits, whereas the [Gd$_{2}$] dimer meets all requirements, including a complete set of operations, to act as a $d = 64$ all-electron spin qudit (or, equivalenty, as six addressable qubits). Electron paramagnetic resonance experiments show that the relevant resonant transitions between different spin states can be coherently controlled, with coherence times T$_{M}$ of the order of $1$ $\mu$s limited by intramolecular hyperfine interactions. Coordination complexes with embedded quantum functionalities are promising building blocks for quantum computation and simulation hybrid platforms.

quant-ph

Optimal coupling of HoW$_{10}$ molecular magnets to superconducting circuits near spin clock transitions

A central goal in quantum technologies is to maximize $G$T$_{2}$, where $G$ stands for the coupling of a qubit to control and readout signals and T$_{2}$ is the qubit's coherence time. This is challenging, as increasing $G$ (e.g. by coupling the qubit more strongly to external stimuli) often leads to deleterious effects on T$_{2}$. Here, we study the coupling of pure and magnetically diluted crystals of HoW$_{10}$ magnetic clusters to microwave superconducting coplanar waveguides. Absorption lines give a broadband picture of the magnetic energy level scheme and, in particular, confirm the existence of level anticrossings at equidistant magnetic fields determined by the combination of crystal field and hyperfine interactions. Such 'spin clock transitions' are known to shield the electronic spins against magnetic field fluctuations. The analysis of the microwave transmission shows that the spin-photon coupling becomes also maximum at these transitions. The results show that engineering spin-clock states of molecular systems offers a promising strategy to combine sizeable spin-photon interactions with a sufficient isolation from unwanted magnetic noise sources.

quant-ph

Quantum-enhanced Landauer erasure and storage

The erasure of a bit of information encoded in a physical system is an irreversible operation bound to dissipate an amount of energy $Q = k_\text{B} T\ln 2$. As a result, work $W \geq Q$ has to be applied to the physical system to restore the erased information content. This limit, called Landauer limit, sets a minimal energy dissipation inherent to any classical computation. In the pursuit of the fastest and most efficient means of computation, the ultimate challenge is to produce a memory device executing an operation as close to this limit in the shortest time possible. Here, we use a crystal of molecular nanomagnets as a spin-memory device and measure the work needed to carry out a storage operation. Exploiting a form of quantum annealing, we border the Landauer limit while preserving fast operation. Owing to the tunable and fast dynamics of this process, the performance of our device in terms of energy-time cost is orders of magnitude better than existing memory devices to date. This result suggests a way to enhance classical computations by using quantum processes.

quant-ph

Three addressable spin qubits in a molecular single-ion magnet

We show that several qubits can be integrated in a single magnetic ion, using its internal electronic spin states with energies tuned by a suitably chosen molecular environment. This approach is illustrated with a nearly-isotropic Gd(III) ion entrapped in a polyoxometalate molecule. Experiments with microwave technologies, either three dimensional cavities or quantum superconducting circuits, show that this magnetic molecule possesses the number of spin states and the set of coherently addressable transitions connecting these states that are needed to perform a universal three-qubit processor or, equivalently, a d=8-level 'qudit'. Our findings open prospects for developing more sophisticated magnetic molecules which can result in more powerful and noise resilient quantum computation schemes.

cond-mat.mtrl-sci

Nanometric constrictions in superconducting coplanar waveguide resonators

We report on the design, fabrication and characterization of superconducting coplanar waveguide resonators with nanoscopic constrictions. By reducing the size of the center line down to 50 nm, the radio frequency currents are concentrated and the magnetic field in its vicinity is increased. The device characteristics are only slightly modified by the constrictions, with changes in resonance frequency lower than 1% and internal quality factors of the same order of magnitude as the original ones. These devices could enable the achievement of higher couplings to small magnetic samples or even to single molecular spins and have applications in circuit quantum electrodynamics, quantum computing and electron paramagnetic resonance.

cond-mat.supr-con

Realization of the anisotropic XY model in a Tb(III)-W(V) chain compound

We present evidence of 1D S=1/2 anisotropic XY ferromagnetism in the paramagnetic phase of the cyanido-bridged chain complex [Tb(pzam)3(H2O)M(CN)8]H2O, with M=W(V), based upon the measurement of the specific heat, the uniform susceptibility and the magnetization curve on a powder sample. Both the specific heat and the susceptibility exhibit a transition peak to long-range ferromagnetism, mediated by the residual interchain couplings, at a critical temperature Tc=1.15 K. Yet in the temperature range T > Tc the specific heat exhibits a broad Schottky anomaly which can be very well fitted by the exact result for the 1D S=1/2 XY model with strong anisotropy in the XY plane (Jx = 1.89 K, Jy=2Jx). For the analysis of the susceptibility and magnetization, not directly accessible theoretically via the exact solution of the XY model, we resort to numerically exact quantum Monte Carlo simulations. Very good agreement is found between the powder-sample data and the Monte Carlo data using an effective average g-factor.

cond-mat.str-el