Metalloporphyrin Zr-MOF Nanoparticles Film for Device Integration of Spin Qubits and Qudits
Javier Serrano-Oiza, Inés Tejedor, Eva Natividad, Arnaud Hemmerlé, Philippe Fontaine, Valentin V. Novikov, Guillem Aromı́, Ignacio Gascón, Olivier Roubeau
Integration of molecular spin qubits onto superconducting circuits is one of the current proposals to build a hybrid quantum processor, in which their coupling to resonators would allow complex coherent quantum operations. As an alternative to large magnetically dilute crystals or concentrated nanoscale deposits of paramagnetic molecules studied so far, we consider here preformed nanoparticles of a Zr(IV)-based 3D MOF doped with Cu(II) and V(IV)O metalloporphyrin. Highly crystalline, phase-pure nanoparticles are obtained with an adjustable number of spin carriers and a homogeneous size that is adequate for nanoconstrictions in superconducting resonators. Continuous-wave and time-domain EPR spectroscopy show that the Cu(II) and V(IV) spins in these particles are potential qubits and qudits, respectively, with robust quantum coherence. These nanoparticles form good dispersions in methanol-chloroform mixtures, which allows the formation of monolayers of densely packed particles at the air-water interface. These Langmuir films are successfully transferred to very different substrates, including Nb resonators, homogeneously covering their most sensitive areas, i.e., the edges of the superconducting lines. Finally, the quantum coherence of the qubit nodes is maintained in the transferred nanoparticles, thereby demonstrating the viability of the present approach for the development of hybrid quantum processors.
Integration of molecular spin qubits onto superconducting circuits is one of the current proposals to build a hybrid quantum processor, in which their coupling to resonators would allow complex coherent quantum operations. As an alternative to large magnetically dilute crystals or concentrated nanoscale deposits of paramagnetic molecules studied so far, we consider here preformed nanoparticles of a Zr(IV)-based 3D MOF doped with Cu(II) and V(IV)O metalloporphyrin. Highly crystalline, phase-pure nanoparticles are obtained with an adjustable number of spin carriers and a homogeneous size that is adequate for nanoconstrictions in superconducting resonators. Continuous-wave and time-domain EPR spectroscopy show that the Cu(II) and V(IV) spins in these particles are potential qubits and qudits, respectively, with robust quantum coherence. These nanoparticles form good dispersions in methanol-chloroform mixtures, which allows the formation of monolayers of densely packed particles at the air-water interface. These Langmuir films are successfully transferred to very different substrates, including Nb resonators, homogeneously covering their most sensitive areas, i.e., the edges of the superconducting lines. Finally, the quantum coherence of the qubit nodes is maintained in the transferred nanoparticles, thereby demonstrating the viability of the present approach for the development of hybrid quantum processors.
High Resolution Image Download MS PowerPoint Slide A strategy toward the realization of a quantum spin processor involves the coupling of spin qubits and qudits to photons within superconducting resonators. To enable the realization of such hybrid architecture, here we first explore the design of a chip with multiple lumped-element LC superconducting resonators optimized for their coupling to distinct transitions of a vanadyl porphyrin electronuclear qudit. The controlled integration of the vanadyl qudit onto the superconducting device, both in terms of number and orientation, is then attained using the in situ formation of nanosheets of a 2D framework built on the vanadyl qudit as a node. Low-temperature transmission experiments demonstrate the coupling of photons in resonators with different frequencies to the targeted electronuclear transitions of the vanadyl qudit, also confirming the control over the vanadyl qudit node orientation. The derived collective spin-photon couplings in the 0.3–1.6 MHz range then allow to estimate enhanced, optimal, single spin photon couplings up to 4 Hz.
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.
The performance and coherence of superconducting quantum systems are fundamentally tied to the quality of the materials from which they are built. In superconducting transmon qubits, many loss mechanisms and sources of decoherence originate from material imperfections or unwanted oxide formation. Likewise, semiconductor–superconductor hybrid systems depend on high-quality interfaces to ensure strong coupling between electronic states in the two materials. In such hybrid devices, the accessible operating regime is often dictated by the intrinsic material properties of either the semiconductor or the superconductor. Advancing quantum device performance therefore requires exploring new material systems and optimizing their physical characteristics. In this thesis, we present the development of several superconducting material platforms for quantum technologies, including superconducting qubits, single-photon detectors, and semiconductor superconductor hybrid devices. We focus on the growth and characterization of superconducting films and heterostructures, and we establish clear connections between their material properties and the resulting device performance. First, we will present a novel semiconductor-superconductor hybrid material based on in-situ deposited epitaxial layers of Nb and Al on a shallow InAs quantum well. In this structure, the Al interlayer provides an epitaxial connection between an in-situ magnetron sputtered Nb or NbTi thin film and a shallow InAs two dimensional electron gas. This metal-to-metal epitaxy is achieved by optimization of the material stack and results in an induced superconducting gap of approximately 1 meV, determined from transport measurements of superconductor semiconductor Josephson junctions. This induced gap is approximately five times larger than the values reported for Al-based hybrid materials and indicates the formation of highly-transparent interfaces that are required in high-quality hybrid material platforms. Then, we discuss a different approach in the next chapter where we develop a hybrid material based on a molecular beam epitaxy grown InAsSb surface quantum well with an in-situ deposited Nb layer directly on top of the quantum well. Relative to conventional Al-InAs based systems, the InAsSb surface quantum well offers a lower effective mass and stronger spin-orbit interaction, while the Nb layer has a higher critical temperature and a larger critical magnetic field. The in-situ deposition of the Nb layer directly on top of the quantum well results in a high-quality interface that enables strong coupling to the InAsSb quantum well. Transport measurements on Josephson junctions reveal an induced superconducting gap of 1.3 meV and a critical current density of 3.75 × 10³A/cm². Furthermore, a planar asymmetric SQUID is realized, exhibiting gate-tunable superimposed oscillations originating from both the individual Josephson junction and the full SQUID loop. The large induced superconducting gap combined with strong spin-orbit interaction position this material as an attractive platform for experiments exploring gate-tunable superconductivity and topological superconducting devices. In the next chapter, we will focus on establishing a link between Nb film crystal properties and their performance in superconducting circuits. In this study, we investigate the microwave properties of niobium resonators with different crystalline properties and related surface topographies. We analyze a series of magnetron sputtered films in which the Nb crystal orientation and surface topography are changed by varying the substrate temperatures between room temperature and 975 K. The lowest-loss resonators that we measure have quality factors of over 10⁶ at single-photon powers, among the best ever recorded using the Nb on sapphire platform. We observe the highest quality factors in films grown at an intermediate temperature regime of the growth series (550 K) where the films display both preferential ordering of the crystal domains and low surface roughness. Furthermore, we analyze the temperature-dependent behavior of our resonators to learn about how the quasi-particle density in the Nb film is affected by the niobium crystal structure and the presence of grain boundaries. Then, we explore yet a different material platform by attempting to realize onchip NbTiN single photon detectors on LiNbO₃, an emerging photonic platform with high potential for scalable quantum information processing. We use DC reactive magnetron sputtering to grow high-quality NbTiN thin films and investigate the impact of substrate temperature during NbTiN growth. We achieve four nm thick superconducting films with a critical temperature (𝑇𝑐) of 12.3 K grown at a substrate temperature of 825 K. We demonstrate that the increased substrate temperature reduces the oxygen concentration in our films and improves the overall stoichiometry. In addition, we integrate these films with the LiNbO3 platform and investigate the obtained interface quality. Finally, we fabricate superconducting nanowire single photon detectors from the NbTiN film on LiNbO₃ and characterize the detector performance. Lastly, we report a gate-tunable Josephson diode effect in hybrid nanowire junctions consisting of a spin-orbit-coupled semiconductor core coated with epitaxial ferromagnetic insulator and superconductor shells. The wires display a hysteretic superconducting window as a function of axial magnetic field. In the superconducting regime, the devices exhibit nonreciprocal current transport, with the diode efficiency showing a strong dependence on back-gate voltage. The effect persists in a remanent magnetization state following a controlled demagnetization procedure, establishing zero-field operation. The combination of results presented in this thesis stress the importance of a material-focused approach in advancing the performance of quantum hardware. The novel hybrid material platforms developed in this thesis expand the operating regime of devices, which could enable future experiments involving gate-tunable superconductivity or topological properties. Similarly, we demonstrate that optimizing superconductor crystal structure benefits quantum devices, such as single-photon detectors and superconducting resonators.
Hybrid circuit quantum electrodynamics (cQED) aims at coupling various quantum degrees of freedom, among which are spin and charge degrees of freedom in gate defined quantum dots, phonons or magnons... with quantized electromagnetic fields in superconducting microwave cavities to investigate fundamental physics questions or for quantum computation and simulation. However, low microwave losses, key for many hybrid cQED experiments, are challenging to achieve given the often exotic and/or complex material stacks (e.g. semiconducting material, ferromagnets, or piezoelectric materials) required to host the various quantum degrees of freedom. In this work, we present a 3D-integration process to overcome this challenge for semi-industrial silicon MOS spin qubits. The process is based on dense indium bump interconnects at a pitch of 10 μm and superconducting thin films of Niobium Nitride (NbN). First, we report on DC and RF interconnect properties that demonstrate a high galvanic interconnection yield and internal quality factors above 105 in the single photon regime for NbN resonators interrupted by a single indium bump interconnect. Eventually, we fabricated a 3D-integrated hybrid circuit quantum electrodynamics (cQED) device based on a semi-industrial MOS hole double quantum dot and a high impedance NbN resonator. For this device, we report a cavity internal quality factor above 10000 and demonstrate record sensitivity for gate-based dispersive readout of the charge degree of freedom with an SNR of 100 in 300 ns. Finally, we demonstrate strong spin-photon coupling of gs/2π = 75 MHz, which highlights the viability of 3D-integration for quantum dot based hybrid spin circuit quantum electrodynamics and opens to high-fidelity spin readout and microwave photon-based remote spin qubit entanglement.
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.
The implementation of a universal quantum processor still poses fundamental issues related to error mitigation and correction, which demand to investigate also platforms and computing schemes alternative to the main stream. A possibility is offered by employing multi-level logical units (qudits), naturally provided by molecular spins. Here we present the blueprint of a Molecular Spin Quantum Processor consisting of single Molecular Nanomagnets, acting as qudits, placed within superconducting resonators adapted to the size and interactions of these molecules to achieve a strong single spin to photon coupling. We show how to implement a universal set of gates in such a platform and to readout the final qudit state. Single-qudit unitaries (potentially embedding multiple qubits) are implemented by fast classical drives, while a novel scheme is introduced to obtain two-qubit gates via resonant photon exchange. The latter is compared to the dispersive approach, finding in general a significant improvement. The performance of the platform is assessed by realistic numerical simulations of gate sequences, such as Deutsch-Josza and quantum simulation algorithms. The very good results demonstrate the feasibility of the molecular route towards a universal quantum processor.