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The Journal of Physical Chemistry Letters

Possible Origin of Low-Frequency Magnetic Flux Noise in Superconducting Devices

Mengli Yao, Xiong Xu, Min Li, Hui Wang

Published Feb 13, 2023• 3 citations
Publisher

Abstract

The magnetic flux noise caused by surface spin fluctuations in superconducting quantum interference devices (SQUIDs) limits their development. In this work, we report that different adsorbents such as H, O 2, NO, and NO 2 that adsorb on the surfaces of Mg-based and Pb-based SQUIDs, respectively, producing large local magnetic moments ranging from 0.7–1.6 μ B, with energy barriers for thermal spin fluctuation as low as 10–30 mK. Moreover, we observe that the presence of H atoms on the surface of MgO can cause the coadsorption of other molecules, which generates additional spin sources. Monte Carlo simulations of the weakly coupled spin on a two-dimensional square lattice produce a low-frequency flux noise spectrum. We suggest eliminating the surface magnetism by coating the surface with monolayer indium phosphide or protecting the surface from other molecules by nonmagnetic preoccupants with a larger adsorption energy. The work provides important physical insights and feasible strategies for reducing magnetic noise sources in superconducting circuits.

DOI
10.1021/acs.jpclett.2c03533

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The magnetic flux noise caused by surface spin fluctuations in superconducting quantum interference devices (SQUIDs) limits their development. In this work, we report that different adsorbents such as H, O 2, NO, and NO 2 that adsorb on the surfaces of Mg-based and Pb-based SQUIDs, respectively, producing large local magnetic moments ranging from 0.7–1.6 μ B, with energy barriers for thermal spin fluctuation as low as 10–30 mK. Moreover, we observe that the presence of H atoms on the surface of MgO can cause the coadsorption of other molecules, which generates additional spin sources. Monte Carlo simulations of the weakly coupled spin on a two-dimensional square lattice produce a low-frequency flux noise spectrum. We suggest eliminating the surface magnetism by coating the surface with monolayer indium phosphide or protecting the surface from other molecules by nonmagnetic preoccupants with a larger adsorption energy. The work provides important physical insights and feasible strategies for reducing magnetic noise sources in superconducting circuits.
A major obstacle to using superconducting quantum interference devices (SQUIDs) as qubits is flux noise. We propose that the heretofore mysterious spins producing flux noise could be O_{2} molecules adsorbed on the surface. Using density functional theory calculations, we find that an O_{2} molecule adsorbed on an α-alumina surface has a magnetic moment of ~1.8 μ_{B}. The spin is oriented perpendicular to the axis of the O-O bond, the barrier to spin rotations is about 10 mK. Monte Carlo simulations of ferromagnetically coupled, anisotropic XY spins on a square lattice find 1/f magnetization noise, consistent with flux noise in Al SQUIDs.
Superconducting qubits are hampered by flux noise produced by surface spins from a variety of microscopic sources. Recent experiments indicated that hydrogen (H) atoms may be one of those sources. Using density functional theory calculations, we report that H atoms either embedded in, or adsorbed on, an $\ensuremath{\alpha}\text{\ensuremath{-}}\mathrm{A}{\mathrm{l}}_{2}{\mathrm{O}}_{3}(0001)$ surface have sizable spin moments ranging from 0.81 to $0.87{\ensuremath{\mu}}_{B}$ with energy barriers for spin reorientation as low as $\ensuremath{\sim}10\phantom{\rule{0.16em}{0ex}}\mathrm{mK}$. Furthermore, H adatoms on the surface attract gas molecules such as O2{\mathrm{O}}_{2}O2​, producing new spin sources. We propose coating the surface with graphene to eliminate H-induced surface spins and to protect the surface from other adsorbates.
Flux noise in superconducting quantum interference devices (SQUIDs) is produced by spins on the surface of metals. We have modeled these with Monte Carlo simulations of 2D and 3D Ising spin glasses that produce magnetization noise SMconsistent with flux noise. The frequency dependence of the magnetization noise goes as 1/fαwhere the exponent a varies slightly with temperature. In 3D the noise power spectrum in the order parameter q goes as 1/ f1.4at Tc. The low frequency noise in both q and the magnetization is a maximum at Tc.
For over three decades, the presence of magnetic flux noise with a power spectral density scaling roughly as SPhi(f)propto1/falphaS_Phi(f) propto 1/f^alphaSP​hi(f)propto1/falpha, where alphalesssim1alpha lesssim 1alphalesssim1, has been known to limit the low-frequency performance of dc superconducting quantum interference devices (SQUIDs). In recent years, experiments indicate that this same noise persists to frequencies up to 1~GHz and is a dominant source of dephasing in flux-sensitive superconducting quantum bits (qubits). Thus, the reduction of flux noise presents a major hurdle towards the successful realization of scalable quantum computers that are based on flux-based qubits. In this thesis, we present experimental measurements, theoretical analyses, and numerical simulations that support a more detailed understanding of both the microscopic and macroscopic properties of flux noise.Our experimental work begins with flux noise measurements of a large number of SQUIDs in the temperature range from 0.1~K to 4~K. We report on measurements of ten SQUIDs with systematically varied geometries and show that alphaalphaalpha increases as the temperature is lowered; in so doing, each spectrum pivots about a nearly constant frequency. The mean square flux noise, inferred by integrating the power spectra, grows rapidly with temperature and at a given temperature is approximately independent of the outer dimension of a given SQUID washer. We show that these results are incompatible with a model based on the random reversal of independent, spins that are located at the surface of the SQUID washer.In the course of our flux noise measurements, we became aware of a spurious contribution to low-frequency critical current noise in Josephson junctions---normally attributed to charge trapping in the barrier---arising from temperature instabilities inherent in cryogenic systems. These temperature fluctuations modify the critical current via its temperature dependence. By computing cross-correlations between measured temperature and critical current noise in Al-AlOx-Al junctions, we show that, despite excellent temperature stability, temperature fluctuations induce observable critical current fluctuations. Particularly, because 1/f1/f1/f critical current noise has decreased with improved fabrication techniques in recent years, it is important to understand and eliminate this additional noise source.Next, we introduce a numerical method of calculating the mean square flux noise PhisqPhisqPhisq from independently fluctuating spins on the surface of thin-film loops of arbitrary geometry. By reciprocity, PhisqPhisqPhisq is proportional to langleBbf(rbf)2ranglelangleBbf(rbf)^2ranglelangleBbf(rbf)2rangle, where Bbf(rbf)Bbf(rbf)Bbf(rbf) is the magnetic field generated by a circulating current around the loop and rbfrbfrbf varies over the loop surface. By discretizing the loop nonuniformly, we efficiently and accurately compute the current distribution and resulting magnetic field, which may vary rapidly across the loop. We use this method to compute PhisqPhisqPhisq in a number of scenarios in which we systematically vary physical parameters of the loop. We compare our simulations to an earlier analytic result predicting that PhisqproptoR/WPhisq propto R/WPhisqproptoR/W in the limit where the loop radius RRR is much greater than the linewidth WWW. We further show that the previously neglected contribution of edge spins to PhisqPhisqPhisq is significant---even dominant---in narrow-linewidth loops.To calculate theoretical dephasing rates in qubits, we consider flux noise with a spectral density SPhi(f)=A2/(f/1 hboxHz)alphaS_Phi(f) = A^2/(f/1~hbox{Hz})^alphaSP​hi(f)=A2/(f/1 hboxHz)alpha, where AAA is of the order of 1~muPhi0,hboxHz−1/2muPhi_0 , hbox{Hz}^{-1/2}muPhi0​,hboxHz−1/2 and 0.6leqalphaleq1.20.6 leq alpha leq 1.20.6leqalphaleq1.2; Phi0Phi_{0}Phi0​ is the flux quantum. For a qubit with an energy level splitting linearly coupled to the applied flux, our calculations of the dependence of the pure dephasing time tauphitau_phitaup​hi of Ramsey and echo pulse sequences on alphaalphaalpha for fixed AAA show that tauphitau_phitaup​hi decreases rapidly as alphaalphaalpha is reduced. We find that tauphitau_phitaup​hi is relatively insensitive to the noise bandwidth, f1leqfleqf2f_1 leq f leq f_2f1​leqfleqf2​, for all alphaalphaalpha provided the ultraviolet cutoff frequency f2>1/tauphif_2 > 1/tau_phif2​>1/taup​hi. We calculate the ratio tauphi,E/tauphi,Rtau_{phi,E} / tau_{phi,R}tauphi,E​/tauphi,R​ of the echo (EEE) and Ramsey (RRR) sequences, and the dependence of the decay function on alphaalphaalpha and f2f_2f2​. We investigate the case in which SPhi(f0)S_Phi(f_0)SP​hi(f0​) is fixed at the ``pivot frequency'' f0neq1f_0 neq 1f0​neq1~Hz while alphaalphaalpha is varied, and find that the choice of f0f_0f0​ can greatly influence the sensitivity of tauphi,Etau_{phi,E}tauphi,E​ and tauphi,Rtau_{phi,R}tauphi,R​ to the value of alphaalphaalpha.Finally, we conclude with a brief review of our principal results and conclusions. We also comment on promising avenues of future research.
Magnetic flux noise is a dominant source of dephasing and energy relaxation in superconducting qubits. The noise power spectral density varies with frequency as 1/fα, with α1, and spans 13 orders of magnitude. Recent work indicates that the noise is from unpaired magnetic defects on the surfaces of the superconducting devices. Here, we demonstrate that adsorbed molecular O2 is the dominant contributor to magnetism in superconducting thin films. We show that this magnetism can be reduced by appropriate surface treatment or improvement in the sample vacuum environment. We observe a suppression of static spin susceptibility by more than an order of magnitude and a suppression of 1/f magnetic flux noise power spectral density of up to a factor of 5. These advances open the door to the realization of superconducting qubits with improved quantum coherence.
Superconducting quantum devices, from qubits and magnetometers to dark matter detectors, are influenced by magnetic flux noise originating from paramagnetic surface defects and impurities. These spin systems can feature complex dynamics, including a Berezinskii-Kosterlitz-Thouless transition, that depend on the lattice, interactions, external fields, and disorder. However, the disorder included in typical models is not materials-specific, diminishing the ability to accurately capture measured flux noise phenomena. We present a first principles-based simulation of a spin lattice consisting of paramagnetic O2_22​ molecules on an Al2_22​O3_33​ surface, a likely flux noise source in superconducting qubits, to elucidate opportunities to mitigate flux noise. We simulate an ensemble of surface adsorbates with disordered orientations and calculate the orientation-dependent exchange couplings using density functional theory. Thus, our spin simulation has no free parameters or assumed functional form of the disorder, and captures correlation in the defect landscape that would appear in real systems. We calculate a range of exchange interactions between electron pairs, with the smallest values, 0.016 meV and -0.023 meV, being in the range required to act as a two-level system and couple to GHz resonators. We calculate the flux noise frequency, temperature, and applied external magnetic field dependence, as well as the susceptibility-flux noise cross-correlation. Calculated trends agree with experiment, demonstrating that a surface harboring paramagnetic adsorbates arranged with materials-specific disorder and interactions captures the various properties of magnetic flux noise observed in superconducting circuits. In addition, we find that an external electric field can tune the spin-spin interaction strength and reduce magnetic flux noise.