Coherent coupling between Vanadyl Phthalocyanine spin ensemble and microwave photons: towards integration of molecular spin qubits into quantum circuits
Claudio Bonizzoni, Alberto Ghirri, Matteo Atzori, Lorenzo Sorace, Roberta Sessoli, M. Affronte
Abstract Electron spins are ideal two-level systems that may couple with microwave photons so that, under specific conditions, coherent spin-photon states can be realized. This represents a fundamental step for the transfer and the manipulation of quantum information. Along with spin impurities in solids, molecular spins in concentrated phases have recently shown coherent dynamics under microwave stimuli. Here we show that it is possible to obtain high cooperativity regime between a molecular Vanadyl Phthalocyanine (VOPc) spin ensemble and a high quality factor superconducting YBa2Cu3O7 (YBCO) coplanar resonator at 0.5 K. This demonstrates that molecular spin centers can be successfully integrated in hybrid quantum devices.
Abstract Electron spins are ideal two-level systems that may couple with microwave photons so that, under specific conditions, coherent spin-photon states can be realized. This represents a fundamental step for the transfer and the manipulation of quantum information. Along with spin impurities in solids, molecular spins in concentrated phases have recently shown coherent dynamics under microwave stimuli. Here we show that it is possible to obtain high cooperativity regime between a molecular Vanadyl Phthalocyanine (VOPc) spin ensemble and a high quality factor superconducting YBa2Cu3O7 (YBCO) coplanar resonator at 0.5 K. This demonstrates that molecular spin centers can be successfully integrated in hybrid quantum devices.
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 review the progress made in integrating magnetic molecules containing transition metal ions into nanoelectronic solid-state devices and using them as molecular spin qubits. Molecular spin qubits offer numerous advantages over other material platforms, such as being inherently quantum systems with discrete energy levels, having a rich variety of possible chemical designs, and being synthesizable in large quantities with atomic precision. However, the integration of magnetic molecules into practical and scalable molecular spin qubit devices (MSQDs) that offer initialization, coherent control, and readout of quantum spin states remains one of the major bottlenecks on the way toward applications of these systems in quantum computing technologies. We discuss the evolution of the field of MSQDs and review the first successful implementation of essential qubit operations in a single-molecule transistor based on a TbPc 2 molecule. Further development has been achieved through the merging of molecular electronics with the circuit quantum electrodynamics (cQED) approach where molecular spin states can be manipulated by the microwave frequency photons confined in a superconducting waveguide resonator. We discuss examples of such hybrid devices operating via coupling of a superconducting resonator to large spin ensembles, such as bulk samples and thin films. We also review a possible architecture for single-molecule cQED devices and the potential advantages that it offers. Then, we highlight the possibility and benefits of the optical initialization and readout of molecular spin states. This approach has been realized by using an optical pumping technique for the initialization and changes in photoluminescence for the readout of large molecular spin ensembles coupled to a superconducting resonator. The field of MSQDs is highly interdisciplinary, bringing together progress in synthetic chemistry, molecular electronics, cQED, and optical measurements. While it is still in its infancy, there are promising theoretical designs and encouraging proof-of-concept experiments, and we discuss several proposed device architectures that are eagerly awaiting experimental realization. Advances in hybrid MSQDs will open horizons for quantum technologies.
Hybrid quantum systems with high-Tc superconducting resonators
Superconducting microwave resonators are crucial elements of microwave circuits, offering a wide range of potential applications in modern science and technology. While conventional low-T[Formula: see text] superconductors are mainly employed, high-T[Formula: see text] cuprates could offer enhanced temperature and magnetic field operating ranges. Here, we report the realization of [Formula: see text] superconducting coplanar waveguide resonators, and demonstrate a continuous evolution from a lossy undercoupled regime, to a lossless overcoupled regime by adjusting the device geometry, in good agreement with circuit model theory. A high-quality factor resonator was then used to perform electron spin resonance measurements on a molecular spin ensemble across a temperature range spanning two decades. We observe spin-cavity hybridization indicating coherent coupling between the microwave field and the spins in a highly cooperative regime. The temperature dependence of the Rabi splitting and the spin relaxation time point toward an antiferromagnetic coupling of the spins below 2 K. Our findings indicate that high-Tc superconducting resonators hold great promise for the development of functional circuits. Additionally, they suggest novel approaches for achieving hybrid quantum systems based on high-T[Formula: see text] superconductors and for conducting electron spin resonance measurements over a wide range of magnetic fields and temperatures.
A quantum coherent interface between optical and microwave photons can be used as a basic building block within a future quantum information network. The interface is envisioned as an ensemble of rare-earth ions coupled to a superconducting resonator, allowing for coherent transfer between optical and microwave photons. Towards this end, we have realized a hybrid device coupling a Er3+-doped Y2SiO5 crystal in a superconducting coplanar waveguide cavity. We observe a collective spin coupling of 4 MHz and a spin linewidth of down to 75 MHz.
A quantum coherent interface between optical and microwave photons can be used as a basic building block within a future quantum information network. The interface is envisioned as an ensemble of rare-earth ions coupled to a superconducting resonator, allowing for coherent transfer between optical and microwave photons. Towards this end, we have realized a hybrid device coupling a Er3+ doped Y2SiO5 crystal in a superconducting coplanar waveguide cavity. We observe a collective spin coupling of 4 MHz and a spin linewdith of down to 75 MHz.
Quantum entanglement is a kernel of quantum computation and quantum communication. We introduce a theoretical scheme to achieve the entanglement between two separated quantum nodes in a hybrid system. The proposed hybrid system based on diamond nitrogen-vacancy (NV) center spin ensemble is coherently coupled to a superconducting quantum circuit consisting of two quantum nodes and a quantum channel. Each node in our setup is composed of an NV center spin ensemble magnetically coupled to a superconducting coplanar resonator. The NV center spin ensemble composed of N identical and non-interacting NV spins, is placed in the magnetic field antinode of the superconducting coplanar resonator where the coupling is maximized. An array of superconducting quantum interference devices (SQUIDs) is inserted in the central conductor of resonator to make its frequency tunable with the magnetic flux threading through the SQUID loops. This flux is generated by passing current through an on-chip wire, so that the resonator can be brought in resonance with the NV center spins without changing their Zeeman splitting. Quantum qubits encoded into two separate nodes are connected by a vacuum superconducting coplanar resonator that is used as a quantum channel. This setup can potentially take the best elements of each individual system:NV center spin ensemble with longer coherence time capable of preparing, storing and releasing photonic quantum information, and the superconducting quantum circuits are easy to manipulate externally and can perform quantum logic gates to control quantum information rapidly. In order to realize the entanglement between two separated quantum nodes, firstly, we make a canonical transformation and obtain the Hamiltonian of the system that is reduced to two NV center spin ensembles resonantly coupled to a single mode of the superconducting coplanar resonator. Then we put forward the hybrid NV center spin-photon qubit encoding. In this hybrid encoding, the NV center spin and photon degrees of freedom enter on an equal footing into the definition of the qubit, in which case, quantum channel will switch on when three superconducting coplanar resonators are in resonance with each other, and all the manipulations can perform simply by tuning the frequencies of the superconducting coplanar resonators. Under the precise control of the evolution time, high fidelity entanglement between two separated quantum nodes is achieved. We show that this proposal can provide high fidelity quantum entanglement under realistic conditions, both in the resonant and the dispersive interaction cases. This hybrid quantum system will exhibit long coherence time and possess features like easy fabrication, integratability, and potential scalability. Furthermore, the quantum node composed of an NV center spin ensemble magnetically coupled to a superconducting coplanar resonator can be respectively integrated, which has practical applications in the realization of quantum information transmission and quantum entanglement among multiple quantum nodes.