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arXiv:2103.08730 · Chemical Science

Controlled coherent dynamics of [VO(TPP)], a prototype molecular nuclear qudit with an electronic ancilla

Simone Chicco, Alessandro Chiesa, G. Allodi, Elena Garlatti, Matteo Atzori, Lorenzo Sorace, R. De Renzi, Roberta Sessoli, Stefano Carretta

Published Jan 1, 2021• 56 citations
arXivHTMLPDF

Abstract

We show that [VO(TPP)] (vanadyl tetraphenylporphyrinate) is a promising system to implement quantum computation algorithms based on encoding information in multi-level (qudit) units. Indeed, it embeds a nuclear spin 7/2 coupled to an electronic spin 1/2 by hyperfine interaction. This qubit-qudit unit can be exploited to implement quantum error correction and quantum simulation algorithms. Through a combined theoretical and broadband nuclear magnetic resonance study, we demonstrate that the elementary operations of such algorithms can be efficiently implemented on the nuclear spin qudit. Manipulation of the nuclear qudit can be achieved by resonant radio-frequency pulses, thanks to the remarkably long coherence times and the effective quadrupolar coupling induced by the strong hyperfine interaction. This approach may open new perspectives for developing new molecular qubit-qudit systems.

DOI
10.1039/d1sc01358k

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•Jan 1, 2008•1 citation
We show that [VO(TPP)] (vanadyl tetraphenylporphyrinate) is a promising system to implement quantum computation algorithms based on encoding information in multi-level (qudit) units. Indeed, it embeds a nuclear spin 7/2 coupled to an electronic spin 1/2 by hyperfine interaction. This qubit-qudit unit can be exploited to implement quantum error correction and quantum simulation algorithms. Through a combined theoretical and broadband nuclear magnetic resonance study, we demonstrate that the elementary operations of such algorithms can be efficiently implemented on the nuclear spin qudit. Manipulation of the nuclear qudit can be achieved by resonant radio-frequency pulses, thanks to the remarkably long coherence times and the effective quadrupolar coupling induced by the strong hyperfine interaction. This approach may open new perspectives for developing new molecular qubit-qudit systems.
The realization of effective quantum error correction protocols remains a central challenge in the development of scalable quantum computers. Employing high-dimensional quantum systems (qudits) can offer more hardware-efficient protocols than qubit-based approaches. Using electron-nuclear double resonance, we implement a logical qubit encoded on the four states of a I=3/2 nuclear spin hyperfine-coupled to an S=1/2 electron spin qubit; the encoding protects against the dominant decoherence mechanism in such systems, i.e., fluctuations of the quantizing magnetic field. We explore the dynamics of the encoded state both under a controlled application of the fluctuation and under natural decoherence processes. Our results confirm the potential of these proposals for practical, implementable, fault-tolerant quantum memories.
The ability to perform quantum error correction (QEC) arbitrarily many cycles is a significant challenge for scalable quantum information processing (QIP). Key requirements for multiple-round QEC are a high degree of quantum control, the ability to efficiently characterize both intrinsic and extrinsic noise, and the ability to dynamically and efficiently extract entropy from ancilla qubits. Nuclear Magnetic Resonance (NMR) based quantum devices have demonstrated high control fidelity with up to 12 qubits, and the noise characterizations can be performed using an efficient protocol known as randomized benchmarking. One of the remaining challenges with NMR systems is that qubit initialization is normally only attainable via thermal equilibration. This results in very low polarizations in reasonable experimental conditions. Moving to electron-nuclear coupled spin systems in a single crystal is a promising solution to the ancilla qubit preparation problem. One obvious advantage of incorporating electron spins comes from higher gyromagnetic ratio of the electron which yields about three orders of magnitude larger thermal spin polarization than that of nuclear spins in the same experimental condition. In addition, fast control of nuclear spins is possible provided appropriate level of anisotropic hyperfine interaction strength. The nuclear spins can be polarized even beyond the thermal electron spin temperature using a technique Heat-Bath Algorithmic Cooling (HBAC). With theoretical ideas in hand, the next step is to develop classical instrumentations to control electron-nuclear coupled systems and accomplish high fidelity coherent control. Noise characterizations are also necessary for benchmarking the quality of control over the electron-nuclear spin system. \nI first present example applications of NMR QIP with small number of qubits: Testing a foundational question in quantum mechanics and measuring spectral density of noise in a quantum system. Then I report on our home-built X-band electron spin resonance (ESR) spectrometer and progress in achieving high fidelity coherent control of electron and nuclear spins for QIP. We focus on implementing nuclear spin manipulation via anisotropic hyperfine interaction and microwave (mw) control, but discussions also include electron nuclear double resonance (ENDOR) control techniques. We perform realistic algorithmic simulations to show that an experimental cooling of nuclear spins below electron thermal temperature is feasible, and to present the electron-nuclear spin systems as promising testbeds for scalable QIP.
Abstract Molecular Nanomagnets may enable the implementation of qudit-based quantum error-correction codes which exploit the many spin levels naturally embedded in a single molecule, a promising step towards scalable quantum processors. To fully realize the potential of this approach, a microscopic understanding of the errors corrupting the quantum information encoded in a molecular qudit is essential, together with the development of tailor-made quantum error correction strategies. We address these central points by first studying dephasing effects on the molecular spin qudit produced by the interaction with surrounding nuclear spins, which are the dominant source of errors at low temperatures. Numerical quantum error correction codes are then constructed, by means of a systematic optimization procedure based on simulations of the coupled system-bath dynamics, that provide a striking enhancement of the coherence time of the molecular computational unit. The sequence of pulses needed for the experimental implementation of the codes is finally proposed.
Coupled electron-nuclear spins are promising physical systems for quantum in-formation processing: By combining the long coherence times of the nuclear spins with the ability to initialize, control, and measure the electron spin state, the favor-able properties of each spin species are utilized. This thesis discusses a procedure to initialize these nuclear spin qubits, and presents a vision of how these systems could be used as the fundamental processing unit of a quantum computer. The fo-cus of this thesis is on control of a system in which a single electron spin is coupled to N nuclear spins via resolvable anisotropic hyperfine (AHF) interactions. High-fidelity universal control of this le-Nn system is possible using only excitations on a single electron spin transition. This electron spin actuator control is implemented by using optimal control theory to find the modulation sequences that generate the desired unitary operations. Decoherence and the challenge of making useful qubits from these systems are also discussed. Experimental evidence of control using an electron spin actuator was acquired with a custom-built pulsed electron spin resonance spectrometer. Complex mod-