Coherent coupling of molecular spins with microwave photons in planar superconducting resonators

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 Tc 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 nonmagnetic 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

Molecular Spins in the Context of Quantum Technologies

Molecular spins have shown interesting quantum features which make them potential candidates for the implementation of quantum information processing. New challenges related to possible applications in broader class of quantum technologies are currently under discussion. Here, we revisit some key features trying to learn something from experiences in near fields

Ultrastrong Magnon-Photon Coupling Achieved by Magnetic Films in Contact with Superconducting Resonators

Coherent coupling between spin wave excitations (magnons) and microwave photons in a cavity may disclose new paths to unconventional phenomena as well as for novel applications. Here, we present a systematic investigation on YIG (Yttrium Iron Garnet) films on top of coplanar waveguide resonators made of superconducting YBCO. We first show that spin wave excitations with frequency higher than the Kittel mode can be excited by putting in direct contact a 5~$\mu$m thick YIG film with the YBCO coplanar resonator (cavity frequency $\omega_c/2 \pi = 8.65$~GHz). With this configuration, we obtain very large values of the collective coupling strength $\lambda/2 \pi \approx 2$~GHz and cooperativity $C=5 \times 10^4$. Transmission spectra are analyzed by a modified Hopfield model for which we provide an exact solution that allows us to well reproduce spectra by introducing a limited number of free parameters. It turns out that the coupling of the dominant magnon mode with photons exceeds 0.2 times the cavity frequency, thus demonstrating the achievement of the ultrastrong coupling regime with this architecture. Our analysis also shows a vanishing contribution of the diamagnetic term which is a peculiarity of pure spin systems

Coupling Nanostructured CsNiCr Prussian Blue Analogue to Resonant Microwave Fields

Collective spin excitations in magnetically ordered materials are exploited for advanced applications in magnonics and spintronics. In these contexts, conditions for minimizing dissipative effects are sought in order to obtain long living excitations that can be coherently manipulated. Organic and coordination magnetic materials may offer alternative options for their flexibility and low spin-orbit effects. Likewise, ferromagnetic nanostructures provide a versatile platform for hybrid architectures, yet downsizing affects the dynamics of magnetic excitations and needs to be controlled. Here we report a systematic investigation on insulating CsNiCr Prussian blue analogue with different degree of nanostructuring. Combining complementary microwave spectroscopic techniques, we performed magnetic resonance in a wide temperature range across the bulk ferromagnetic transition occurring at TC=90 K. This allows us to monitor key parameters of the spin dynamics through different types of nanostructured samples. We found that, below TC, the Gilbert damping parameter of 10 nm nanoparticles compares well (10-3) with values reported for prototypical inorganic analogues (YIG). Strong coupling with the microwave field of a planar microstrip resonator is then observed for bulk CsNiCr as well as for mutually interacting NPs. These results clarify conditions for the coherent manipulation of collective spin degrees of freedom in nanostructured coordination materials

Microstrip Resonators and Broadband Lines for X-band EPR Spectroscopy of Molecular Nanomagnets

We present a practical setup to perform continuous-wave X-band electron paramagnetic resonance spectroscopy by using planar microstrip lines and general purpose instrumentation. We fabricated Ag/alumina and Nb/sapphire microstrip resonators and transmission lines and compared their performance down to 2 K and under applied magnetic field. We used these devices to study single crystals of molecular Cr3 nanomagnets. By means of X-band planar resonators we measured angle-dependent spectra at fixed frequency, while broadband transmission lines were used to measure continuous wave spectra with varying frequency in the range 2–25 GHz. The spectra acquired at low temperatures allowed to extract the essential parameters of the low-lying energy levels of Cr3 and demonstrate that this method is particularly suitable to study small crystals of molecular nanomagnets

Coherently coupling distinct spin ensembles through a high-Tc superconducting resonator

The problem of coupling multiple spin ensembles through cavity photons is revisited by using (3,5-dichloro-4- pyridyl)bis(2,4,6-trichlorophenyl) methyl (PyBTM) organic radicals and a high-T-c superconducting coplanar resonator. An exceptionally strong coupling is obtained and up to three spin ensembles are simultaneously coupled. The ensembles are made physically distinguishable by chemically varying the g factor and by exploiting the inhomogeneities of the applied magnetic field. The coherent mixing of the spin and field modes is demonstrated by the observed multiple anticrossing, along with the simulations performed within the input-output formalism, and quantified by suitable entropic measures

Oxo-centered carboxylate-bridged trinuclear complexes deposited on Au(111) by a mass-selective electrospray.

We developed an apparatus for nondestructive in vacuum deposition of mass-selected fragile Cr based metal trinuclear complexes, by modifying a commercial Mass Spectrometer containing an electrospray ionization source. Starting from a solution, this system creates a beam of ionized molecules which is then transferred into an evacuated region where the molecules can be mass selected before deposition. To verify the system efficiency, we deposited sub monolayers of oxo-centered carboxylate-bridged trinuclear complexes (Cr3 and Cr2Ni) on Au(111) surface. By XPS and STM we determined the deposited molecule stoichiometry and the surface coverage. The results show that this apparatus is works well for the in vacuum deposition of molecular nanomagnets and, thanks to its reduced dimensions, it is portable

Coupling molecular spin centers to microwave planar resonators: towards integration of molecular qubits in quantum circuits

We present spectroscopic measurements looking for the coherent coupling between molecular magnetic centers and microwave photons. The aim is to find the optimal conditions and the best molecular features to achieve the quantum strong coupling regime, for which coherent dynamics of hybrid photon-spin states take place. To this end, we used a high critical temperature YBCO superconducting planar resonator working at 7.7 GHz and at low temperatures to investigate three molecular mononuclear coordination compounds, namely (PPh4)2[Cu(mnt)2] (where mnt2- = maleonitriledithiolate), [ErPc2]-TBA+ (where pc2- is the phtalocyaninato and TBA+ is the tetra-n-butylammonium cation) and Dy(trensal) (where H3trensal = 2,2′,2′′-tris(salicylideneimino)triethylamine). Although the strong coupling regime was not achieved in these preliminary experiments, the results provided several hints on how to design molecular magnetic centers to be integrated into hybrid quantum circuits