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arXiv:2610.19180

Cavity-assisted dynamic nuclear polarisation

Tristan Lorriaux, Yutian Wen, Patrice Bertet, Benjamin Huard, Audrey Bienfait

quant-phcond-mat.mes-hallSubmitted Oct 13, 2026• Announced Oct 15, 2026
arXivHTMLPDF

Abstract

Dynamic nuclear polarisation transfers polarisation from electron to nuclear spins by relying on a dissipative channel. Here we introduce a cavity-based DNP mechanism which uses the radiative relaxation of the electronic spin through the Purcell effect to bring about the nuclear spin polarisation. We implement this protocol on an ensemble of bismuth donor spins (I=9/2, S=1/2) in isotopically purified silicon coupled to a superconducting resonator. A single cycle, combining adiabatic microwave and radio-frequency pulses with Purcell relaxation, increases a target ground state's population by a factor of $1.79\pm0.04$; a cumulative enhancement of $4.6\pm0.2$ is reached with additional cycles, to be compared with the theoretical limit of ninefold set by the degeneracy of the ground manifold. We explain this difference by the competition between Purcell and intrinsic relaxation on the one hand and a collective effect that slows down the electronic spin radiative decay as the nuclear spin population grows on the other hand. Our results place radiative DNP as an available mechanism at millikelvin temperatures where phonon-mediated relaxation is frozen.

Comments
18 pages, 5 figures

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Dynamic nuclear polarisation transfers polarisation from electron to nuclear spins by relying on a dissipative channel. Here we introduce a cavity-based DNP mechanism which uses the radiative relaxation of the electronic spin through the Purcell effect to bring about the nuclear spin polarisation. We implement this protocol on an ensemble of bismuth donor spins (I=9/2, S=1/2) in isotopically purified silicon coupled to a superconducting resonator. A single cycle, combining adiabatic microwave and radio-frequency pulses with Purcell relaxation, increases a target ground state's population by a factor of 1.79±0.041.79\pm0.041.79±0.04; a cumulative enhancement of 4.6±0.24.6\pm0.24.6±0.2 is reached with additional cycles, to be compared with the theoretical limit of ninefold set by the degeneracy of the ground manifold. We explain this difference by the competition between Purcell and intrinsic relaxation on the one hand and a collective effect that slows down the electronic spin radiative decay as the nuclear spin population grows on the other hand. Our results place radiative DNP as an available mechanism at millikelvin temperatures where phonon-mediated relaxation is frozen.
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Dynamic nuclear polarization (DNP) is a promising strategy for generating a significantly increased nonthermal spin polarization in nuclear magnetic resonance (NMR) and its applications that range from medicine diagnostics to material science. Being a genuine nonequilibrium effect, DNP circumvents the need for strong magnetic fields. However, despite intense research, a detailed theoretical understanding of the precise mechanism behind DNP is currently lacking. We address this issue by focusing on a simple instance of DNP-so-called solid effect DNP-which is formulated in terms of a quantum central spin model where a single electron is coupled to an ensemble of interacting nuclei. We show analytically that the nonequilibrium buildup of polarization heavily relies on a mechanism which can be interpreted as kinetically constrained diffusion. Beyond revealing this insight, our approach furthermore permits numerical studies of ensembles containing thousands of spins that are typically intractable when formulated in terms of a quantum master equation. We believe that this represents an important step forward in the quest of harnessing nonequilibrium many-body quantum physics for technological applications.
Realisation of strong coupling between a superconducting microwave resonator and an ensemble of phosphorus donor spins, contained in an isotopically purified silicon host crystal. Investigation of the dynamical properties of the coupled system at mK temperatures and ultra-low microwave powers. The relaxation and coherence times of the coupled system were extracted by pulsed microwave spectroscopy, with the result that the hybrid system's coherence time is enhanced compared to the uncoupled spin system.
Abstract We employ the electronic spin of a single nitrogen-vacancy (NV) defect in diamond to detect and control the quantum state of remote nuclear spins coupled by hyperfine interaction. More precisely, our work focuses on individual 13C^{13}\text {C}13C 13 C nuclei featuring a moderate hyperfine coupling strength ( ∼1\sim 1∼1 ∼ 1 MHz) with the NV’s electron spin. Two different methods providing an efficient room-temperature polarization of these peculiar 13C^{13}\text {C}13C 13 C nuclear spins are described. The first one is based on a polarization transfer from the NV electron spin to the 13C^{13}\text {C}13C 13 C nucleus, which is mediated by the anisotropic component of the hyperfine interaction. The second one relies on coherent population trapping (CPT) within a Λ\Lambda Λ Λ -type energy-level configuration in the microwave domain, which enables to initialize the 13C^{13}\text {C}13C 13 C nuclear spin in any quantum state superposition on the Bloch sphere. This CPT protocol is performed in an unusual regime for which relaxation from the excited level of the Λ\Lambda Λ Λ -scheme is externally triggered by optical pumping and separated in time from coherent microwave excitations. For these two polarization techniques, we investigate the impact of optical illumination on the nuclear spin polarization efficiency. This work adds new methods to the quantum toolbox used for coherent control of individual nuclear spins in diamond, which might find applications in quantum metrology. Graphical Abstract
We report strong coupling between an ensemble of nitrogen-vacancy center electron spins in diamond and a superconducting microwave coplanar waveguide resonator. The characteristic scaling of the collective coupling strength with the square root of the number of emitters is observed directly. Additionally, we measure hyperfine coupling to (13)C nuclear spins, which is a first step towards a nuclear ensemble quantum memory. Using the dispersive shift of the cavity resonance frequency, we measure the relaxation time of the NV center at millikelvin temperatures in a nondestructive way.
Pulsed Dynamic Nuclear Polarization (DNP) is currently receiving substantial interest as a means to enhance the sensitivity of nuclear magnetic resonance (NMR) and magnetic resonance imaging (MRI) by orders of magnitude. It has also received much attention as a central ingredient in many modalities of electron spin-involved quantum sensing. Relative to spin engineering associated with NMR, the design of efficient pulsed DNP experiments with a broad experimental scope are challenged by large electron-nuclear spin systems, large electron spin-involved interactions, and instrumental non-idealities and limitations. All of this may challenge traditional NMR-like theoretical and numerical pulse sequence engineering. Exploiting state-of-the-art instrumentation and taking advantage of the high sensitivity of DNP relative to NMR, we here demonstrate the use of combinations of Bayesian machine learning methods and constrained random walk procedures to design pulse sequences \textit{in situ}, by experiments, directly on the spin systems responding to spectrometer instructions. For trityl and nitroxide samples, it is demonstrated that efficient broadband DNP pulse sequences can be designed in situ with experimental protocols benchmarked against in silico analogs.