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arXiv:1905.08944 · The Journal of Physical Chemistry Letters

Toward Long-Range Entanglement between Electrically Driven Single-Molecule Magnets

Khadijeh Najafi, Aleksander L. Wysocki, Kyungwha Park, Sophia E. Economou, Edwin Barnes

Published Nov 12, 2019• 22 citations
arXivHTMLPDF

Abstract

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.

DOI
10.1021/acs.jpclett.9b03131

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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.
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_22​ 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_22​ 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_22​ 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.
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 challenge of building a scalable quantum processor requires consolidation of the conflicting requirements of achieving coherent control and preservation of quantum coherence in a large scale quantum system. Moreover, the system should be compatible with miniaturization and integration of quantum circuits. Mesoscopic solid state systems such as superconducting islands and quantum dots feature robust control techniques using local electrical signals and self-evident scaling based on advances in fabrication; however, in general the quantum states of solid state devices tend to decohere rapidly. In contrast, quantum optical systems based on trapped ions and neutral atoms exhibit dramatically better coherence properties, while miniaturization of atomic and molecular systems, and their integration with mesoscopic electrical circuits, remains an important challenge. Below we describe methods for the integration of a single particle system -- an isolated polar molecule -- with mesoscopic solid state devices in a way that produces robust, coherent, quantum-level control. The methods described include the trapping, cooling, detection, coherent manipulation and quantum coupling of isolated polar molecules at sub-micron dimensions near cryogenic stripline microwave resonators. We show that electrostatically trapped polar molecules can exhibit strong confinement and fast, purely electrical gate control. Furthermore, the effect of electrical noise sources, a key issue in quantum information processing, can be suppressed to very low levels via appropriate preparation and manipulation of the polar molecules. Our setup provides a scalable cavity QED-type quantum computer architecture, where entanglement of distant qubits stored in long-lived rotational molecular states is achieved via exchange of microwave photons.
Polar molecules are an emerging platform for quantum technologies based on their long-range electric dipole--dipole interactions, which open new possibilities for quantum information processing and the quantum simulation of strongly correlated systems. Here, we use magnetic and microwave fields to design a fast entangling gate with >0.999>0.999>0.999 fidelity and which is robust with respect to fluctuations in the trapping and control fields and to small thermal excitations. These results establish the feasibility to build a scalable quantum processor with a broad range of molecular species in optical-lattice and optical-tweezers setups.
In this work we study theoretically the coupling of single-molecule magnets (SMMs) to a variety of quantum circuits, including microwave resonators with and without constrictions and flux qubits. The main result of this study is that it is possible to achieve strong and ultrastrong coupling regimes between SMM crystals and the superconducting circuit, with strong hints that such a coupling could also be reached for individual molecules close to constrictions. Building on the resulting coupling strengths and the typical coherence times of these molecules (~ µs), we conclude that SMMs can be used for coherent storage and manipulation of quantum information, either in the context of quantum computing or in quantum simulations. Throughout the work we also discuss in detail the family of molecules that are most suitable for such operations, based not only on the coupling strength, but also on the typical energy gaps and the simplicity with which they can be tuned and oriented. Finally, we also discuss practical advantages of SMMs, such as the possibility to fabricate the SMMs ensembles on the chip through the deposition of small droplets.
In this work we study theoretically the coupling of single-molecule magnets (SMMs) to a variety of quantum circuits, including microwave resonators with and without constrictions and flux qubits. The main result of this study is that it is possible to achieve strong and ultrastrong coupling regimes between SMM crystals and the superconducting circuit, with strong hints that such a coupling could also be reached for individual molecules close to constrictions. Building on the resulting coupling strengths and the typical coherence times of these molecules (∼ μ s), we conclude that SMMs can be used for coherent storage and manipulation of quantum information, either in the context of quantum computing or in quantum simulations. Throughout the work we also discuss in detail the family of molecules that are most suitable for such operations, based not only on the coupling strength, but also on the typical energy gaps and the simplicity with which they can be tuned and oriented. Finally, we also discuss practical advantages of SMMs, such as the possibility to fabricate the SMMs ensembles on the chip through the deposition of small droplets.