Over the past two decades, many quantum systems have been explored as candidate qubits for quantum information processing. Qubits based on nuclear spins enjoy exceptionally long coherence times, especially compared to other solid-state platforms. However, this usually comes at the cost of slow gate operations and weak interqubit interactions, aspects which have so far prevented the development of multi-qubit processors comprised of solid-state nuclear spins. An exception to this is the TbPc$_2$ single-molecule magnet, a nuclear spin qubit which features a remarkable combination of long-lived coherence and fast electrical control. Despite this promise, it has remained an open question how to couple such qubits together to create the entanglement needed for quantum information applications. Given the sensitivity of the TbPc$_2$ molecule to electric fields via the hyperfine Stark effect, it is natural to consider the possibility of using a superconducting transmission line resonator to mediate a long-distance coupling between multiple TbPc$_2$ qubits. We use recent experimental results on single-qubit Rabi oscillations to deduce the strength and nature of the hyperfine Stark effect, information we then use to estimate the qubit-resonator coupling and to design two-qubit entangling gates with fidelities exceeding 99%. Our results suggest that the qubit-resonator interaction is near the edge of the strong coupling regime and could potentially pass into it with further improvements in device designs and components.
Over the past two decades, many quantum systems have been explored as candidate qubits for quantum information processing. Qubits based on nuclear spins enjoy exceptionally long coherence times, especially compared to other solid-state platforms. However, this usually comes at the cost of slow gate operations and weak interqubit interactions, aspects which have so far prevented the development of multi-qubit processors comprised of solid-state nuclear spins. An exception to this is the TbPc2 single-molecule magnet, a nuclear spin qubit which features a remarkable combination of long-lived coherence and fast electrical control. Despite this promise, it has remained an open question how to couple such qubits together to create the entanglement needed for quantum information applications. Given the sensitivity of the TbPc2 molecule to electric fields via the hyperfine Stark effect, it is natural to consider the possibility of using a superconducting transmission line resonator to mediate a long-distance coupling between multiple TbPc2 qubits. We use recent experimental results on single-qubit Rabi oscillations to deduce the strength and nature of the hyperfine Stark effect, information we then use to estimate the qubit-resonator coupling and to design two-qubit entangling gates with fidelities exceeding 99%. Our results suggest that the qubit-resonator interaction is near the edge of the strong coupling regime and could potentially pass into it with further improvements in device designs and components.
Over the past two decades, several molecules have been explored as possible building blocks of a quantum computer, a device that would provide exponential speedups for a number of problems, including the simulation of large, strongly correlated chemical systems. Achieving strong interactions and entanglement between molecular qubits remains an outstanding challenge. Here, we show that the TbPc 2 single-molecule magnet has the potential to overcome this obstacle because of its sensitivity to electric fields stemming from the hyperfine Stark effect. We show how this feature can be leveraged to achieve long-range entanglement between pairs of molecules using a superconducting resonator as a mediator. Our results suggest that the molecule–resonator interaction is near the edge of the strong-coupling regime and could potentially pass into it given a more detailed, quantitative understanding of the TbPc 2 molecule.
One of the key elements in circuit quantum electrodynamics (cQED) is the superconducting microwave resonator, which can enable strong coupling to and between nanoscale quantum systems, and as a result has emerged as an essential tool for both quantum information and quantum sensing. In this thesis, I will discuss new applications of superconducting resonators in both of these fields, which illustrates how quantum information and quantum sensing can be strongly tied together. As the field of quantum information continues to grow, various platforms for realizing a quantum computer have been proposed. One attractive platform is to control and manipulate the spin of an electron to form spin qubits, which have demonstrated a long coherence time, weak coupling to the environment, and high fidelity single- and two-qubit gates. However, scaling beyond two qubits has proven challenging, as has incorporating long-range coupling, although both are crucial for making spin qubits a scalable quantum computing platform. The confinement of electromagnetic fields in superconducting resonators enables strong coupling to small systems, such as the single electrons of a spin qubit. In the first part of this thesis, I will describe how a singlet-triplet spin qubit coupled to a high-impedance superconducting resonator constitutes a promising architecture for mediating long-ranged interactions based on a longitudinal coupling between the resonator and qubit. I will discuss the technical developments needed to successfully implement this novel type of interaction in a hybrid spin qubit-resonator device. This type of interaction has several advantages over the more commonly studied transverse coupling scheme: it does not require careful tuning of the qubit frequency to match that of the resonator, which facilitates scaling to a large number of qubits, and also avoids the loss of coherence, which is inevitable in resonant coupling. This type of interaction therefore opens promising paths for generating high-fidelity long-ranged two-qubit coupling by employing superconducting microwave resonators. By adapting techniques used in quantum information, we have also developed a new technique in quantum sensing, where we employ superconducting resonators as a probe of quantum materials such as mesoscopic systems, two-dimensional materials, and heterostructures, which are otherwise challenging to experimentally access with conventional techniques. In the second part of my thesis, I will discuss how implementing cQED techniques from quantum information allows us to probe the symmetry of the order parameter in unconventional superconductors. Unconventional superconductors are not readily available, and we therefore study an engineered system that comprises of interfacing a ferromagnet and superconductor, in which unconventional pairing can be induced into the ferromagnet. This platform allows us to simultaneously excite spin waves, a collective excitation of spins, in the ferromagnet, which opens new directions for studying interactions between coherently coupled magnons (quanta of spin waves) and unconventional superconducting states. Finally, by applying the same technique to a two-dimensional (2D) superconductor, tungsten ditelluride, we leverage this platform in an attempt to study the order parameter of its intrinsic superconducting phase. The nature of the order parameter in this material remains an open question, as both topological and superconducting phases can exist, possibly simultaneously. This work thus demonstrates a unique use of superconducting resonators beyond quantum information applications.
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.
There is a huge, worldwide effort to build a quantum computer due to its potential to perform chemical and materials simulations and to break current cryptography schemes. While there has been incredible progress in recent years, each potential platform still faces meaningful obstacles. The singlet-triplet qubit in gallium arsenide, which is based on electric spin, boasts several advantages, including fast single-gate times and readout, long lifetimes, and a clear path to large-scale integration using current semiconductor manufacturing techniques. However, it also suffers from electric and magnetic field noise that limits coherence time and weak two-qubit interactions, which have prevented the construction of multi-qubit systems so far. In this thesis, I will discuss my research measuring and working to improve noise and entangling gates in singlet-triplet qubits and will examine the viability of the singlet-triplet qubit as the building block for a quantum computer. \nBy measuring the dynamics of the electric and magnetic field noise that the singlet-triplet experiences, we can develop an understanding of their origins and how to reduce their impact. The singlet-triplet can be operated rapidly enough to use it as a sensor and directly measure the fluctuating magnetic field arising from the nuclear spins in the semiconductor heterostructure surrounding it. We use Hamiltonian parameter estimation, a technique that maximizes the rate at which we learn information, given the strange properties of quantum measurement, to measure magnetic noise to within 15 μT at a rate of 2 kHz, and we use these measurements to provide real-time feedback to system controls, increasing the coherence time by a factor of 30. Charge noise has much larger high-frequency components than magnetic noise, and thus requires use of dynamical decoupling methods borrowed from NMR to measure it. We measure its power spectrum up to 1 MHz and find that it has a 1/f spectrum. We perform these measurements for several different devices and have begun to determine how our growth and fabrication processes affect dephasing. \nPlacing a high-impedance resonator between two singlet-triplet qubits to mediate their interaction shows promise as way to create long-distance entanglement and to increase the speed of the entangling gate. We analyze this gate theoretically, finding that we expect the fidelity to be over 95%, with a straightforward path to increasing it to above 99% with improved resonator parameters. However, because the singlet-triplet qubit is extremely sensitive to changes in its electrostatic environment, which can be affected both by the resonator’s fabrication process and the presence of the proximal resonator gate, implementing this gate experimentally is challenging. We have developed processes for fabricating narrow, thin, NbN resonators directly adjacent to the double quantum dots that compose singlet-triplet qubits. These processes yield quantum dots that can be tuned into low-noise, stable singlet-triplet qubits, and superconducting resonators with impedances over 1 kOhm.
The ability to coherently control and read out qubits with long coherence times in a scalable system is a crucial requirement for any quantum processor. Nuclear spins in the solid state have shown great promise as long-lived qubits. Control and readout of individual nuclear spin qubit registers has made major progress in the recent years using individual electron spin ancilla addressed either electrically or optically. Here, we present a new platform for quantum information processing, consisting of 183W nuclear spin qubits adjacent to an Er3+ impurity in a CaWO4 crystal, interfaced via a superconducting resonator and detected using a microwave photon counter at 10mK. We study two nuclear spin qubits with T2∗ of 0.8(2)s and 1.2(3)s, T2 of 3.4(4)s and 4.4(6) s, respectively. We demonstrate single-shot quantum non-demolition readout of each nuclear spin qubit using the Er3+ spin as an ancilla. We introduce a new scheme for all-microwave single- and two-qubit gates, based on stimulated Raman driving of the coupled electron-nuclear spin system. We realize single- and two-qubit gates on a timescale of a few milliseconds, and prepare a decoherence-protected Bell state with 88% fidelity and T2∗ of 1.7(2)s. Our results are a proof-of-principle demonstrating the potential of solid-state nuclear spin qubits as a promising platform for quantum information processing. With the potential to scale to tens or hundreds of qubits, this platform has prospects for the development of scalable quantum processors with long-lived qubits.
Recent experiments with silicon qubits demonstrated strong coupling of a microwave resonator to the spin of a single electron in a double quantum dot, opening up the possibility of long-range spin-spin interactions. We present our theoretical calculation of effective interactions between distant quantum dot spins coupled by a resonator, and propose a protocol for fast, high-fidelity two-qubit gates consistent with experimentally demonstrated capabilities. Our simulations show that, in the presence of noise, spin-spin entangling gates significantly outperform cavity-mediated gates on charge qubits.