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arXiv:2501.10762 · Applied Physics Letters

Superconducting microwave oscillators as detectors for ESR spectroscopy

Roberto Russo, André Chatel, N. Brusadin, R. Yu, Reza Farsi, H. Furci, Juergen Brügger, Giovanni Boero

Published Apr 1, 2025• 2 citations

Abstract

Microwave superconducting resonators are extensively studied in fields such as quantum computing and electron spin resonance (ESR) spectroscopy. However, the integration of superconducting resonators with feedback mechanisms to create ultra-low noise oscillators is a relatively unexplored area, and the application of such oscillators in ESR spectroscopy has not yet been demonstrated. In this work, we report the design, fabrication, and application of microwave oscillators based on superconducting resonators for ESR spectroscopy, illustrating an alternative way for the improvement of the performance of oscillator based ESR sensors. Specifically, ESR spectra are obtained by measuring the oscillator's frequency shift induced by the ESR effect as a function of the applied static magnetic field. The oscillators are composed of a single heterojunction bipolar transistor or high electron mobility transistor coupled with NbTi or YBa2Cu3O7 (YBCO) superconducting resonators. The fabricated oscillators operate at frequencies of 0.6 and 1.7 GHz and temperatures up to 80 K (for YBCO resonators) and 8 K (for NbTi resonators). The lowest measured frequency noise is about 9 mHz/Hz1/2 (−139 dBc/Hz), the best spin sensitivity is about 1×1010 spins/Hz1/2, and the best concentration sensitivity is about 3×1018 spins/Hz1/2m3. The approach proposed in this work should allow for significantly better spin and concentration sensitivities compared to those achievable with normal conductors, up to operating frequencies, magnetic fields, and temperatures, where superconductors exhibit substantially lower effective microwave resistance than normal conductors.

DOI: 10.1063/5.0260098

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Electron spin resonance (ESR) is a powerful spectroscopy method which allows to identify and characterize paramagnetic species. It usually relies on detecting microwave radiation absorbed or emitted by the spins into a microwave resonator tuned to their Larmor precession frequency. Because of the weak spin-microwave coupling, conventional ESR spectroscopy has a low sensitivity. Recent experiments have demonstrated that superconducting quantum circuits have the potential to enhance the spin detection sensitivity to single spin detection; by namely using high quality factor small mode volume resonator. However, these demonstrations have been realized in very restrictive conditions, using well-known spin systems. To probe samples coming from chemistry or biology, quantum-circuit enabled spectrometers have to be adapted to be robust to losses. They have typically two origins: the dielectric losses introduced by the samples, mostly aqueous, and losses coming from the strong magnetic field required to tune the electronic spins to the resonator frequency. This PhD work centered on implementing a resonator that would achieve the same ESR sensitivity while being robust to dielectric losses and strong magnetic fields. Using NbTiN films deposited on sapphire, microwave resonators were shown to have quality factors above Q=105 in magnetic field, even when samples with dielectric losses above tan d > 0.05 were introduced. A study of the resonator intrinsic losses showed marked drops at multiple specific magnetic fields: a signature of coupling to spurious systems. Over the course of the PhD, mitigation nanofabrication techniques for these contaminants were developed, such as hard mask etching and annealing, to remove all but one of this contaminants. Finally, test of the spectrometer on a benchmark species (BDPA, α,γ-Bisdiphenylene-β-phenylallyl, a known ESR marker) were realized.

We use a superconducting flux qubit for the sensing application of electron spin resonance (ESR) spectroscopy.The superconducting flux qubit is a highly sensitive magnetometer with micrometer-scale spatial resolution.The sensitivity of our spectrometer is 400 spins/√Hz, and the sensing volume is 0.05 pL.This high sensitivity and high spatial resolution enable us to investigate a small number of electron spins in a microscale area.The spectrometer also obtains a wider ESR spectrum range with twoparameter (frequency and magnetic field) scanning.This enables us to refine the material parameters.

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Superconducting circuits are promising components for future quantum information technologies such as quantum computing, quantum simulation, and quantum sensing. Superconducting quantum interference devices (SQUIDs) and superconducting flux qubits can be used as a sensitive magnetic field sensor to detect local electron spin resonance (ESR). These types of sensor are characterized by good sensitivity and high spatial resolution for electron spins. In fact, we have achieved a sensitivity of 20 spins/

\sqrt{\text {Hz}}

with a sensing volume of 6 fl combining a flux qubit and qubit readout using a Josephson bifurcation amplifier. As a demonstration, we measured the ESR spectrum of erbium electron spins in a Y

_{2}

SiO

_{5}

crystal and nitrogen vacancy centers in diamond. In both cases, we obtained reasonable electron spin parameters by fitting a simulation to the spectrum. In this way, we proved superconducting circuits to be promising magnetic field sensors for evaluating the properties of solid materials.

Hybrid quantum systems with high-T

_c

superconducting resonators

Superconducting microwave resonators are crucial elements of microwave circuits, offering a wide range of potential applications in modern science and technology. While conventional low-T[Formula: see text] superconductors are mainly employed, high-T[Formula: see text] cuprates could offer enhanced temperature and magnetic field operating ranges. Here, we report the realization of [Formula: see text] superconducting coplanar waveguide resonators, and demonstrate a continuous evolution from a lossy undercoupled regime, to a lossless overcoupled regime by adjusting the device geometry, in good agreement with circuit model theory. A high-quality factor resonator was then used to perform electron spin resonance measurements on a molecular spin ensemble across a temperature range spanning two decades. We observe spin-cavity hybridization indicating coherent coupling between the microwave field and the spins in a highly cooperative regime. The temperature dependence of the Rabi splitting and the spin relaxation time point toward an antiferromagnetic coupling of the spins below 2 K. Our findings indicate that high-Tc superconducting resonators hold great promise for the development of functional circuits. Additionally, they suggest novel approaches for achieving hybrid quantum systems based on high-T[Formula: see text] superconductors and for conducting electron spin resonance measurements over a wide range of magnetic fields and temperatures.