Micron-sized lasers fabricated from upconverting nanoparticles (UCNP) coupled to whispering gallery mode (WGM) microresonators can exhibit continuous-wave anti-Stokes lasing useful for tracking cells, environmental sensing, and coherent stimulation of biological activity. The integration of these microlasers into organisms and microelectronics requires even smaller diameters, however, which raises threshold pump powers beyond practical limits for biological applications. To meet the need for low lasing thresholds and high fidelity fabrication methods, we use correlative optical and electron microscopy to uncover the nanoparticle assembly process and structural factors that determine efficient upconverted lasing. We show that 5 μm microspheres with controlled submonolayer UCNP coatings exhibit, on average, 25-fold lower laser thresholds (1.7 ± 0.7 kW/cm²) compared to the mean values of the lowest threshold UCNP lasers, and variability is reduced 30-fold. WGMs are observed in the upconversion spectra for TiO₂-coated microspheres as small as 3 μm, a size at which optical losses had previously prevented such observations. Finally, we demonstrate that the WGM signatures of these upconverting microlasers can be imaged and distinguished through tissue-mimicking phantoms. These advances will enable the fabrication of more efficient upconverting lasers for imaging, sensing, and actuation in optically complex environments.

As superconducting quantum processors increase in complexity, techniques to overcome constraints on frequency crowding are needed. The recently developed method of laser-annealing provides an effective post-fabrication method to adjust the frequency of superconducting qubits. Here, we present an automated laser-annealing apparatus based on conventional microscopy components and demonstrate preservation of highly coherent transmons. In addition, we perform noise spectroscopy to investigate the change in defect features, in particular, two-level system defects, after laser-annealing. Finally, we present a local heating model as well as demonstrate aging stability for laser-annealing on the wafer scale. Our work constitutes an important step toward both understanding the underlying physical mechanism and scaling up laser-annealing of superconducting qubits.

Multiphoton imaging techniques that convert low-energy excitation to higher energy emission are widely used to improve signal over background, reduce scatter, and limit photodamage. Lanthanide-doped upconverting nanoparticles (UCNPs) are among the most efficient multiphoton probes, but even UCNPs with optimized lanthanide dopant levels require laser intensities that may be problematic. Here, we develop protein-sized, alloyed UCNPs (aUCNPs) that can be imaged individually at laser intensities >300-fold lower than needed for comparably sized doped UCNPs. Using single UCNP characterization and kinetic modeling, we find that addition of inert shells changes optimal lanthanide content from Yb³⁺, Er³⁺-doped NaYF₄ nanocrystals to fully alloyed compositions. At high levels, emitter Er³⁺ ions can adopt a second role to enhance aUCNP absorption cross-section by desaturating sensitizer Yb³⁺ or by absorbing photons directly. Core/shell aUCNPs 12 nm in total diameter can be imaged through deep tissue in live mice using a laser intensity of 0.1 W cm^-2.

Two-dimensional heterostructures composed of layers with slightly different lattice vectors exhibit new periodic structure known as moiré lattices, which, in turn, can support novel correlated and topological phenomena. Moreover, moiré superstructures can emerge from multiple misaligned moiré lattices or inhomogeneous strain distributions, offering additional degrees of freedom in tailoring electronic structure. High-resolution imaging of the moiré lattices and superstructures is critical for understanding the emerging physics. Here, we report the imaging of moiré lattices and superstructures in graphene-based samples under ambient conditions using an ultrahigh-resolution implementation of scanning microwave impedance microscopy. Although the probe tip has a gross radius of ~100 nm, spatial resolution better than 5 nm is achieved, which allows direct visualization of the structural details in moiré lattices and the composite super-moiré. We also demonstrate artificial synthesis of novel superstructures, including the Kagome moiré arising from the interplay between different layers.

Qubits made from superconducting materials are a mature platform for quantum information science application, such as quantum computing. However, material-based losses are now a limiting factor in reaching the coherence times needed for applications. In particular, knowledge of the atomistic structure and properties of the circuit materials is needed to identify, understand, and mitigate material-based decoherence channels. In this work, we characterize the atomic structure of the native oxide film formed on Nb resonators by comparing fluctuation electron microscopy experiments to density functional theory calculations, finding that an amorphous layer is consistent with an Nb2O5 stoichiometry. Comparing x-ray absorption measurements at the Oxygen K edge with first-principles calculations, we find evidence of d-type magnetic impurities in our sample, known to cause impedance in proximal superconductors. This work identifies the structural and chemical composition of the oxide layer grown on Nb superconductors and shows that soft x-ray absorption can fingerprint magnetic impurities in these superconducting systems.

Materials imperfections in planar superconducting quantum circuits - in particular, two-level-system (TLS) defects - contribute significantly to decoherence, ultimately limiting the performance of quantum computation and sensing. The identification of specific parasitic layers and their associated loss contributions has, however, proven elusive. Using a combination of x-ray photoemission spectroscopy (XPS) and analytical scanning transmission electron microscopy (STEM), we determine the thickness, chemical composition, and location of the oxides present in niobium-on-silicon coplanar-waveguide (CPW) resonators and quantify their respective contributions to the measured single-photon quality factor (Q). Using selective chemical etching, we reduce first the substrate-air oxide then the metal-air oxide thickness, dramatically reducing both TLS (δTLS) and non-TLS (δhi) losses, resulting in a median Q value over 5×106, with individual devices approaching 6×106. We find that silicon surface oxides host 70% of TLS losses, with a δTLS:δhi loss-density ratio near 11:1. In contrast, niobium surface oxides host 77% of non-TLS losses, uniformly distributed within the oxide layer, with a δTLS:δhi loss-density ratio of 3:4 for the superconducting circuits investigated in this work. Only 7% of losses come from other sources, including the niobium-silicon interface, which is sufficiently clean in our devices to allow epitaxial Nb nucleation on Si. As we mitigate surface losses through selective modification of the interface dielectrics, we arrive in a regime where TLS losses are no longer dominant, which will allow other types of losses in superconducting circuits to be investigated in more detail, including nonequilibrium quasiparticles.

Quantum sensing and computation can be realized with superconducting microwave circuits. Qubits are engineered quantum systems of capacitors and inductors with non-linear Josephson junctions. They operate in the single-excitation quantum regime, photons of $27 \mu$eV at 6.5 GHz. Quantum coherence is fundamentally limited by materials defects, in particular atomic-scale parasitic two-level systems (TLS) in amorphous dielectrics at circuit interfaces.[1] The electric fields driving oscillating charges in quantum circuits resonantly couple to TLS, producing phase noise and dissipation. We use coplanar niobium-on-silicon superconducting resonators to probe decoherence in quantum circuits. By selectively modifying interface dielectrics, we show that most TLS losses come from the silicon surface oxide, and most non-TLS losses are distributed throughout the niobium surface oxide. Through post-fabrication interface modification we reduced TLS losses by 85% and non-TLS losses by 72%, obtaining record single-photon resonator quality factors above 5 million and approaching a regime where non-TLS losses are dominant. [1]M\"uller, C., Cole, J. H. & Lisenfeld, J. Towards understanding two-level-systems in amorphous solids: insights from quantum circuits. Rep. Prog. Phys. 82, 124501 (2019)