Phonon-induced Cooper pair breaking, inciting nonequilibrium quasiparticle (QP) bursts, is known to deteriorate the performance of superconducting devices. However, a detailed understanding of QP-phonon dynamics is lacking due to the absence of a well-established theoretical framework. This paper presents a fully ab initio scheme of calculating nonequilibrium, polarization-dependent QP-phonon dynamics in superconductors. The authors find that with only an 8% deviation from the equilibrium phonon Bose–Einstein distribution, the resulting nonequilibrium QP population is 83 times larger than the equilibrium Fermi–Dirac distribution, and the longitudinal acoustic (LA) phonon polarization is most responsible for QP generation. The authors demonstrated that the qubit transition rate in Josephson junction-based transmon qubits is increased by orders of magnitude when taking these nonequilibrium distributions into account, compared to equilibrium distributions. This framework allows an in-depth exploration of nonequilibrium QP-phonon dynamics in various Josephson-junction-based superconducting devices. It paves the way for formulating advanced phonon shielding strategies to target the LA polarization, potentially leading to enhanced device performance, such as increased coherence time of transmon qubits or reduced thermal noise in cryogenics.
Phonon-induced Cooper pair breaking, inciting nonequilibrium quasiparticle (QP) bursts, is known to deteriorate the performance of superconducting devices. However, a detailed understanding of QP-phonon dynamics is lacking due to the absence of a well-established theoretical framework. This paper presents a fully ab initio scheme of calculating nonequilibrium, polarization-dependent QP-phonon dynamics in superconductors. The authors find that with only an 8% deviation from the equilibrium phonon Bose–Einstein distribution, the resulting nonequilibrium QP population is 83 times larger than the equilibrium Fermi–Dirac distribution, and the longitudinal acoustic (LA) phonon polarization is most responsible for QP generation. The authors demonstrated that the qubit transition rate in Josephson junction-based transmon qubits is increased by orders of magnitude when taking these nonequilibrium distributions into account, compared to equilibrium distributions. This framework allows an in-depth exploration of nonequilibrium QP-phonon dynamics in various Josephson-junction-based superconducting devices. It paves the way for formulating advanced phonon shielding strategies to target the LA polarization, potentially leading to enhanced device performance, such as increased coherence time of transmon qubits or reduced thermal noise in cryogenics.
Nonequilibrium quasiparticle and phonon dynamics are central to the operation of superconducting devices. Superconducting detectors, such as superconducting nanowire single-photon detectors, transition-edge sensors, or microwave kinetic inductance detectors, perform best when a large quasiparticle population is generated in response to small perturbations. Conversely, for superconducting qubits and topologically protected Majorana fermions, even relatively small quasiparticle densities can lead to significant performance degradation. Hence, ideal materials for these devices would be less susceptible to quasiparticle poisoning. However, existing models of these devices often rely on approximations and phenomenology. Therefore, they lack a rigorous description of the underlying quasiparticle and phonon dynamics that are responsible for device performance. In this article, we combine kinetic equations with density functional theory to model the nonequilibrium quasiparticle and phonon dynamics of a thin superconducting film ab initio. To demonstrate the universality of our model, we illustrate two independent example applications: (1) we develop a theoretical model describing the detection of single photons in superconducting nanowires, and (2) we calculate the energy-relaxation rate of a transmon qubit due to the presence of excess quasiparticles. Our examples demonstrate from first principles that niobium nitride is well suited to be used for single-photon detection and that tantalum transmon qubits possess reduced sensitivity to quasiparticle poisoning relative to other materials, which is likely in part responsible for their longer coherence times. In contrast to previous models of superconducting devices, our ab initio approach makes predictions of device performance without experimental input and thus can be used to accelerate progress in device development. Moreover, by considering the full-bandwidth electron-phonon coupling, our approach can incorporate strong-coupling effects. Our methods effectively integrate ab initio materials modeling with nonequilibrium theory of superconductivity to perform practical modeling of superconducting devices, providing a comprehensive approach that connects fundamental theory with device-level applications.
Even in the quantum limit, non-equilibrium quasiparticle (QP) populations induce QP poisoning that irreversibly relaxes the quantum state and significantly degrades the coherence of transmon qubits. A particularly detrimental yet previously unexplored mechanism arises from QP multiplication facilitated by vortex trapping in superconducting quantum circuits, where a high-energy QP relaxes by breaking additional Cooper pairs and amplifying the QP population due to the locally reduced excitation gap and enhanced quantum confinement within the vortex core. Here we directly resolve this elusive QP multiplication process by revealing vortex-controlled QP self-generation in a highly nonequilibrium regime preceding the phonon bottleneck of QP relaxation. At sufficiently low fluence, femtosecond-resolved magneto-reflection spectroscopy directly reveals a continuously increasing QP population that is strongly dependent on magnetic-field-tuned vortex density and absent at higher excitation fluences. Quantitative analysis of the emergent QP pre-bottleneck dynamics further reveals that, although the phonon population saturates within $\simeq$10~ps, both free and trapped QPs continue to grow in a self-sustained manner--hallmarks of the long-anticipated QP-vortex interactions in nonequilibrium superconductivity. We estimate a substantial increase of $\sim$34\% in QP density at vortex densities of ∼ 100 magnetic flux quanta per μm2. Our findings establish a powerful spectroscopic tool for uncovering QP multiplication and reveal vortex-assisted QP relaxation as a critical materials bottleneck whose mitigation will be essential for resolving QP poisoning and enhancing coherence in superconducting qubits.
The density of quasiparticles typically observed in superconducting qubits exceeds the value expected in equilibrium by many orders of magnitude. Can this out-of-equilibrium quasiparticle density still possess an energy distribution in equilibrium with the phonon bath? Here, we answer this question affirmatively by measuring the thermal activation of charge-parity switching in a transmon qubit with a difference in superconducting gap on the two sides of the Josephson junction. We then demonstrate how the gap asymmetry of the device can be exploited to manipulate its parity.
Micro-fabricated superconducting circuits have emerged as a leading candidate for quantum computers. However, typical error rates of 10-3 for quantum gates remain a challenge for performing error correction and need to be further decreased for achieving practical quantum computation. Improving qubit coherence times for superconducting qubits is a continuous endeavor in order to decrease error rates. As part of this effort, a topic addressed in this dissertation is the study of the generation mechanism and dynamics of non-equilibrium quasiparticles (QPs), which are electron-like excitations of a superconductor. This source of decoherence was studied by measuring the rate of single-electron changes in the parity state of multiple charge-sensitive transmon qubits under different conditions. The presence of non-equilibrium QPs in superconducting resonators and qubits operating at millikelvin temperature has been known for decades. Understanding the sources and dynamics of these QPs is crucial to evaluate and improve the performance of the devices. Specifically, for superconducting qubits, a single QP tunneling across the Josephson junction changes the total charge parity from even to odd or vice versa, and can induce energy relaxation and dephasing, limiting the coherence of the device. To study the dynamics of non-equilibrium QPs, I utilized a Ramsey-like pulse sequence to measure the rate of single-electron parity changes in transmon qubits, which had a weak charge dispersion, with different shunting capacitor geometries and materials. I started out by measuring a charge parity rate of ~ 33 s-1 for a grounded "x-mon" qubit and ~ 17 s-1 for a galvanically isolated "two-pads" qubit with our standard setup. These rates decreased to ~ 5 s-1 and ~ 2 s-1 for the x-mon and two-pads respectively when IR-filters and extra layers of shielding were installed. From my measurements, I found that the charge parity rates are sensitive to the geometry of the shunting capacitor, weakly depend on the amount of shielding surrounding the device, and independent of using Al or Ta for the superconducting shunting capacitor. To distinguish between two possible mechanisms for the parity switching, I measured the parity rates after cooling one of the qubit devices in an external magnetic field to induce vortices in the superconducting electrodes. After increasing the magnetic field above 23 μT, I measured a faster QP trapping rate and a much smaller T1, suggesting that at least one vortex was added to the superconducting electrode near the Josephson junction. On the other hand, the measured charge parity rates exhibited no clear dependence on the background QP trapping rates. These data suggest that a large portion of parity switching events occurs from QPs being produced at the Josephson junction, where pair-breaking radiation is rectified into QPs by the junction, as opposed to tunneling of QPs residing in the electrodes. To understand the difference in the measured parity rates, I simulated the absorption efficiency of pair-breaking radiation for my two designs and observed a similar difference in absorption rates when a single-mode blackbody radiation with an effective temperature T* ~ 300 mK was assumed to be illuminating the devices. This large T*, which is significantly higher than the device's nominal temperature of 20 mK, is consistent with values reported in the literature. However, its physical origin remains not fully understood. For the other part of my dissertation, I developed a new simplified process for making superconducting air bridges. Air bridges are used to suppress unwanted extraneous high frequency chip modes parasitic to superconducting quantum circuits that can couple to qubits and cause decoherence. Traditional ways of making air bridges utilize thermal reflow to create arched photoresist scaffolds that are limited in heights. This results in insufficient mechanical strength of the bridges which tend to collapse when spanning to larger lengths. My simplified fabrication method that utilizes two-photon lithography, a technique that enables creation of three-dimensional micron-scale structures, relaxes this limitation and is capable of making mechanically stable bridges with lengths up to 100 μm. The resulting Al air bridges, having a superconducting transition temperature of Tc = 1.08 mK and a dc residual resistivity ratio of 3.85, were confirmed to form a good electrical contact with the base metal layers and exhibit a small measurable amount of rf loss when placed over coplanar waveguide resonators, on par with other air bridge fabrication methods.
The quasiparticle density observed in low-temperature superconducting circuits is several orders of magnitude larger than the value expected at thermal equilibrium. The tunneling of this excess of quasiparticles across Josephson junctions is recognized as one of the main loss and decoherence mechanisms in superconducting qubits. Here we present a unified impedance theory that accounts for quasiparticle energy loss in circuit regions both far from and near to (across) junctions. Our theory leverages the recent experimental demonstration that the excess quasiparticles are in quasiequilibrium [Connolly et al., Phys. Rev. Lett. 132, 217001 (2024)] and uses a generalized fluctuation-dissipation theorem to predict the amount of charge and flux noise generated by them. We compute the resulting energy relaxation time T1 in transmon qubits with and without junction asymmetric gap engineering, and show that quasiparticles residing away from junctions can play a dominant role in the former case. They also may provide an upper limit for resonator quality factors if the density of amorphous two-level systems is reduced. In addition, we show that charge noise from quasiparticles leads to flux noise that is logarithmic in frequency, giving rise to a ``nearly white'' contribution that is comparable to the flux noise observed in flux qubits. This contrasts with amorphous two-level systems, whose associated flux noise is shown to be super-Ohmic. We discuss how this quasiparticle flux noise can limit ${T}_{2}^{\ensuremath{\ast}}$ coherence times in flux-tunable qubits. The final conclusion is that asymmetric gap engineering can greatly reduce noise and increase coherence times in superconducting qubits.
Nonequilibrium quasiparticles (QPs) generated by stray infrared and ionizing radiation can limit the performance of superconducting quantum processors and present challenges for quantum error correction schemes. Models of QP-induced energy relaxation commonly assume that the characteristic energy of the QPs and the qubit transition energy are both small relative to the superconducting gap. Under these assumptions, certain qubits such as the fluxonium would exhibit protection against QP-induced dissipation at specific bias points. Here, we show that this is not necessarily the case, numerically analyzing the predicted rate of QP-induced dissipation in fluxonium qubits for different QP energy distributions and for QPs created via photon-assisted tunneling processes. We find that accounting for small numerical factors, existing theoretical models predict sensitivity to QP-induced errors at bias points previously thought to be protected. We find that inclusion of asymmetry in the superconducting gap energy across the junction can reintroduce suppression of QP-induced relaxation, as expected. Additionally, for QPs created by photon-assisted tunneling, we predict that T1 protection will only occur for a specific energy of pair-breaking radiation. This understanding of fluxonium sensitivity to QP-induced dissipation informs the development of fluxonium-based processors and future QP-mitigation strategies.