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AVS Quantum Science

The role of self-assembled monolayers at substrate–metal interfaces in limiting coherence of superconducting quantum circuits

Saleem G. Rao

Published Dec 1, 2025• 2 citations
Publisher

Abstract

In planar superconducting quantum circuits, two-level system (TLS) defects within amorphous dielectrics at various circuit interfaces, including substrate–metal (SM) and air-interfaces, are a critical source of decoherence. We employed molecular self-assembled monolayer (SAM) at different interfaces to mitigate TLS losses in superconducting coplanar waveguide (CPW) resonators. Previous work has reported an increase in the resonator quality factor when a SAM is applied to air-interfaces, but a contrasting decrease is observed when the SAM is applied to the metal–substrate interfaces. To investigate the reason behind this decrease, we fabricated and characterized niobium (Nb)-based CPW resonator chips on silicon substrates, both with and without a SAM at the SM interface. Quality factor measurements performed at 100 mK across a wide range of driving powers confirmed that the presence of the SAM at the SM interface led to a reduction in the quality factor. This observed decrease is attributed to an increased TLS defect density, as suggested by the topography of niobium deposited on the SAM. Our findings demonstrate that the roughness of the deposited Nb at the SM interface, which is influenced by the SAM, significantly impacts the density of TLS defects at this interface. Furthermore, simulations of TLS losses in CPW resonators supported our experimental observations by evaluating resonator quality factors under various interface modifications, particularly showing a decrease in the quality factor when the SM interface exhibited high loss.

DOI
10.1116/5.0283809

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Abstract Quantum bits (qubits) with long coherence times are an important element for the implementation of medium- and large-scale quantum computers. In the case of superconducting planar qubits, understanding and improving qubits’ quality can be achieved by studying superconducting planar resonators. In this paper, we fabricate and characterize coplanar waveguide resonators made from aluminum thin films deposited on silicon substrates. We perform three different substrate surface treatments prior to aluminum deposition: one chemical treatment based on a hydrofluoric acid clean; one physical treatment consisting of a thermal annealing at 880 °C in high vacuum; and one combined treatment comprising both the chemical and the physical treatments. The aim of these treatments is to remove the two-level state (TLS) defects hosted by the native oxides residing at the various samples’ interfaces. We first characterize the fabricated samples through cross-sectional tunneling electron microscopy, acquiring electron energy loss spectroscopy maps of the samples’ cross sections. These measurements show that both the chemical and the physical treatments almost entirely remove native silicon oxide from the substrate surface and that their combination results in the cleanest interface. Additionally, we analyze the effects of the various substrate treatments on the roughness of the silicon surface by means of atomic force microscopy surface morphology mapping. We then study the quality of the resonators by means of microwave measurements in the ‘quantum regime’, i.e., at a temperature T ∼ 10 mK and at a mean microwave photon number 〈 n ph 〉 ∼ 1 . In this regime, we find that both surface treatments independently improve the resonator’s intrinsic quality factor by ≈172%. The highest quality factor is obtained for the combined treatment, Q i ≈ 0.82 million, corresponding to an improvement by ≈256%. Finally, we find that the TLS quality factor averaged over a time period of 3 h is ∼3 million at 〈 n ph 〉 ∼ 10 , indicating that substrate surface engineering can potentially reduce the TLS loss below other losses such as quasiparticle loss and flux noise.

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In planar superconducting quantum circuits, two-level system (TLS) defects within amorphous dielectrics at various circuit interfaces, including substrate–metal (SM) and air-interfaces, are a critical source of decoherence. We employed molecular self-assembled monolayer (SAM) at different interfaces to mitigate TLS losses in superconducting coplanar waveguide (CPW) resonators. Previous work has reported an increase in the resonator quality factor when a SAM is applied to air-interfaces, but a contrasting decrease is observed when the SAM is applied to the metal–substrate interfaces. To investigate the reason behind this decrease, we fabricated and characterized niobium (Nb)-based CPW resonator chips on silicon substrates, both with and without a SAM at the SM interface. Quality factor measurements performed at 100 mK across a wide range of driving powers confirmed that the presence of the SAM at the SM interface led to a reduction in the quality factor. This observed decrease is attributed to an increased TLS defect density, as suggested by the topography of niobium deposited on the SAM. Our findings demonstrate that the roughness of the deposited Nb at the SM interface, which is influenced by the SAM, significantly impacts the density of TLS defects at this interface. Furthermore, simulations of TLS losses in CPW resonators supported our experimental observations by evaluating resonator quality factors under various interface modifications, particularly showing a decrease in the quality factor when the SM interface exhibited high loss.
In planar superconducting circuits, decoherence due to materials imperfections, especially two-level-system (TLS) defects at different interfaces, is a primary hurdle for advancing quantum computing and sensing applications. Traditional methods for mitigating TLS loss, such as etching oxide layers at metal and substrate interfaces, have proven to be inadequate due to the persistent challenge of oxide regrowth. In this work, we introduce a novel approach that employs molecular self-assembled monolayers (SAMs) to chemically bind at different interfaces of superconducting circuits. This technique is specifically tested here on coplanar waveguide (CPW) resonators, in which this method not only impedes oxide regrowth after surface etching but can also tailors the dielectric properties at different resonators interfaces. The deployment of SAMs results in a consistent improvement in the measured quality factors across multiple resonators, surpassing those with only oxide-etched resonators. The efficiency of our approach i3s supported by microwave measurements of multiple devices conducted at millikelvin temperatures and correlated with detailed X-ray photoelectron spectroscopy (XPS) and transmission electron microscopy (TEM) characterizations of SAM-passivated resonators. The compatibility of SAMs materials with the established fabrication techniques offers a promising route to improve the performance of superconducting quantum devices.
Superconducting coplanar waveguide (CPW) microwave resonators in quantum circuits are the best components for reading and changing the state of artificial atoms because of their excellent coupling to quantum systems. This coupling forms the basis of the developing circuit quantum electrodynamic architecture. In quantum processors, oscillators are used to store and transmit quantum information using microwave-frequency wave packets. However, the presence of amorphous thin-film defects is deleterious and can result in an irrevocable loss of coherent information with uncontrolled degrees of freedom. Although there has been extensive research into techniques to reduce the coherent loss of such devices, the precise structure of amorphous dielectric layers on surfaces and interfaces and their associated loss mechanism are being actively studied. In particular, planar superconducting resonators are very sensitive to defects on their surfaces, such as two-level systems in oxidized metals and nonequilibrium quasiparticles, making these devices suitable probes for the different loss mechanisms. In this work, we present the design, fabrication, and characterization of Nb CPW resonators with different surface treatments with self-assembled monolayers (SAMs), which mitigate the growth of oxides in superconducting circuits. We demonstrate SAM-passivated resonators having internal quality factors of greater than 10 6 at a single-photon excitation power (measured at 100 mK), which were probed using scanning electron microscopy, X-ray photoelectron spectroscopy, and transmission electron microscopy to demonstrate the efficiency of our surface treatment. Finally, we compared the improvements in the experimental quality factors to those obtained by numerical simulation.
Superconducting quantum computing systems, including coplanar waveguide (CPW) resonators and qubits, are highly susceptible to energy dissipation from two-level systems (TLS) within bulk and interfacial dielectrics. CPW resonators serve as an ideal platform for characterizing these material losses at the single-photon excitation level. Building on recent experimental evidence that interface engineering can mitigate TLS losses, this study employs simulations to evaluate resonator quality factors across various interface modifications. Our results demonstrate that reducing losses at the substrate–air (SA) interface can increase the internal quality factor Qi by up to three orders of magnitude. While etching the SA interface also enhances Qi, material loss remains the dominant dissipation mechanism. Furthermore, we find that other lossy interfaces have a significantly smaller impact on the quality factor compared to the SA interface. These simulation results align with established experimental findings, providing a robust framework for refining resonator design. This work offers precise guidelines for TLS mitigation, essential for enhancing coherence times and developing more reliable superconducting quantum processors.
Tantalum is a promising platform for superconducting quantum circuits, yet coherence times remain limited by dielectric losses from interfacial two-level systems (TLS), exacerbated by native oxide regrowth. Here, we implement molecular surface passivation using self-assembled organic monolayers on freshly etched tantalum and silicon in coplanar waveguide resonators. Surface characterization by contact angle, XPS, FTIR and TEM confirm the formation of ordered, nanometer-thick films that suppress oxide formation. Microwave measurements in the ~5-9 GHz range reveal internal quality factors up to 1.8x10^6 in the single-photon regime at 100 mK, representing a ~140% improvement over untreated devices with native oxide. Power and temperature dependent measurements attribute this enhancement to reduced TLS-induced losses. These results demonstrate that molecular passivation effectively engineers low-loss interfaces and provides a scalable route toward high-coherence superconducting quantum devices.
Abstract One main limiting factor towards achieving high coherence times in superconducting circuits is two-level system (TLS) losses. Mitigating such losses requires controlling the formation of native oxides at the metal-air interface. Here, we report the growth of alkyl-phosphonate self-assembled monolayers (SAMs) on Nb thin films following oxide removal. The impact of passivation was evaluated via the performance of coplanar waveguide resonators at 10 mK, in terms of quality factor and resonant frequency, over six days of air exposure. Un-passivated resonators exhibited an ~80% increase in loss at single-photon power levels, whereas SAM-passivated resonators maintained excellent temporal stability, attributed to suppressed oxide regrowth. By employing a two-component TLS model, we discern distinct prominent loss channels for each resonator type and quantified the characteristic TLS loss of the SAMs to be ~5×10 -7 . We anticipate our passivation methodology to offer a promising route toward industrial-scale qubit fabrication, particularly where long-term device stability is critical.
Abstract Quantum bits (qubits) with long coherence times are an important element for the implementation of medium- and large-scale quantum computers. In the case of superconducting planar qubits, understanding and improving qubits’ quality can be achieved by studying superconducting planar resonators. In this paper, we fabricate and characterize coplanar waveguide resonators made from aluminum thin films deposited on silicon substrates. We perform three different substrate surface treatments prior to aluminum deposition: one chemical treatment based on a hydrofluoric acid clean; one physical treatment consisting of a thermal annealing at 880 °C in high vacuum; and one combined treatment comprising both the chemical and the physical treatments. The aim of these treatments is to remove the two-level state (TLS) defects hosted by the native oxides residing at the various samples’ interfaces. We first characterize the fabricated samples through cross-sectional tunneling electron microscopy, acquiring electron energy loss spectroscopy maps of the samples’ cross sections. These measurements show that both the chemical and the physical treatments almost entirely remove native silicon oxide from the substrate surface and that their combination results in the cleanest interface. Additionally, we analyze the effects of the various substrate treatments on the roughness of the silicon surface by means of atomic force microscopy surface morphology mapping. We then study the quality of the resonators by means of microwave measurements in the ‘quantum regime’, i.e., at a temperature T ∼ 10 mK and at a mean microwave photon number 〈 n ph 〉 ∼ 1 . In this regime, we find that both surface treatments independently improve the resonator’s intrinsic quality factor by ≈172%. The highest quality factor is obtained for the combined treatment, Q i ≈ 0.82 million, corresponding to an improvement by ≈256%. Finally, we find that the TLS quality factor averaged over a time period of 3 h is ∼3 million at 〈 n ph 〉 ∼ 10 , indicating that substrate surface engineering can potentially reduce the TLS loss below other losses such as quasiparticle loss and flux noise.