Room temperature optically detected magnetic resonance of single spins in GaN.

High-contrast optically detected magnetic resonance is a valuable property for reading out the spin of isolated defect colour centres at room temperature. Spin-active single defect centres have been studied in wide bandgap materials including diamond, SiC and hexagonal boron nitride, each with associated advantages for applications. We report the discovery of optically detected magnetic resonance in two distinct species of bright, isolated defect centres hosted in GaN. In one group, we find negative optically detected magnetic resonance of a few percent associated with a metastable electronic state, whereas in the other, we find positive optically detected magnetic resonance of up to 30% associated with the ground and optically excited electronic states. We examine the spin symmetry axis of each defect species and establish coherent control over a single defect's ground-state spin. Given the maturity of the semiconductor host, these results are promising for scalable and integrated quantum sensing applications.

Tuning Exciton Emission via Ferroelectric Polarization at a Heterogeneous Interface between a Monolayer Transition Metal Dichalcogenide and a Perovskite Oxide Membrane.

We demonstrate the integration of a thin BaTiO3 (BTO) membrane with monolayer MoSe2 in a dual-gate device that enables in situ manipulation of the BTO ferroelectric polarization with a voltage pulse. While two-dimensional (2D) transition metal dichalcogenides (TMDs) offer remarkable adaptability, their hybrid integration with other families of functional materials beyond the realm of 2D materials has been challenging. Released functional oxide membranes offer a solution for 2D/3D integration via stacking. 2D TMD excitons can serve as a local probe of the ferroelectric polarization in BTO at a heterogeneous interface. Using photoluminescence (PL) of MoSe2 excitons to optically read out the doping level, we find that the relative population of charge carriers in MoSe2 depends sensitively on the ferroelectric polarization. This finding points to a promising avenue for future-generation versatile sensing devices with high sensitivity, fast readout, and diverse applicability for advanced signal processing.

Nanoscale Magnetization and Current Imaging Using Time-Resolved Scanning-Probe Magnetothermal Microscopy.

Magnetic microscopy that combines nanoscale spatial resolution with picosecond scale temporal resolution uniquely enables direct observation of the spatiotemporal magnetic phenomena that are relevant to future high-speed, high-density magnetic storage and logic technologies. Magnetic microscopes that combine these metrics has been limited to facility-level instruments. To address this gap in lab-accessible spatiotemporal imaging, we develop a time-resolved near-field magnetic microscope based on magnetothermal interactions. We demonstrate both magnetization and current density imaging modalities, each with spatial resolution that far surpasses the optical diffraction limit. In addition, we study the near-field and time-resolved characteristics of our signal and find that our instrument possesses a spatial resolution on the scale of 100 nm and a temporal resolution below 100 ps. Our results demonstrate an accessible and comparatively low-cost approach to nanoscale spatiotemporal magnetic microscopy in a table-top form to aid the science and technology of dynamic magnetic devices with complex spin textures.

Engineering Electron-Phonon Coupling of Quantum Defects to a Semiconfocal Acoustic Resonator.

Diamond-based microelectromechanical systems (MEMS) enable direct coupling between the quantum states of nitrogen-vacancy (NV) centers and the phonon modes of a mechanical resonator. One example, a diamond high-overtone bulk acoustic resonator (HBAR), features an integrated piezoelectric transducer and supports high-quality factor resonance modes into the gigahertz frequency range. The acoustic modes allow mechanical manipulation of deeply embedded NV centers with long spin and orbital coherence times. Unfortunately, the spin-phonon coupling rate is limited by the large resonator size, >100 µm, and thus strongly coupled NV electron-phonon interactions remain out of reach in current diamond BAR devices. Here, we report the design and fabrication of a semiconfocal HBAR (SCHBAR) device on diamond (silicon carbide) with f × Q > 1012 (>1013). The semiconfocal geometry confines the phonon mode laterally below 10 µm. This drastic reduction in modal volume enhances defect center coupling to a mechanical mode by 1000 times compared to prior HBAR devices. For the native NV centers inside the diamond device, we demonstrate mechanically driven spin transitions and show a high strain-driving efficiency with a Rabi frequency of (2π)2.19(14) MHz/Vp, which is comparable to a typical microwave antenna at the same microwave power, making SCHBAR a power-efficient device useful for fast spin control, dressed state coherence protection, and quantum circuit integration.

Scalable Synthesis of Switchable Assemblies of Gold Nanorod Lyotropic Liquid Crystal Nanocomposites.

A new class of solvent free, lyotropic liquid crystal nanocomposites based on gold nanorods (AuNRs) with high nanorod content is reported. Application of shear results in switchable, highly ordered alignment of the nanorods over several centimeters with excellent storage stability for months. For the synthesis, AuNRs are surface functionalized with a charged, covalently tethered corona, which induces fluid-like properties. This honey-like material can be deposited on a substrate and a high orientational order parameter of 0.72 is achieved using a simple shearing protocol. Switching shearing direction results in realignment of the AuNRs. For a film containing 75 wt% of AuNRs the alignment persists for several months. In addition to the lyotropic liquid crystal characteristics, the AuNRs films also exhibit anisotropic electrical conductivity with an order of magnitude difference between the conductivities in direction parallel and perpendicular to the alignment of the AuNRs.

Optical Absorption and Emission Mechanisms of Single Defects in Hexagonal Boron Nitride.

We investigate the polarization selection rules of sharp zero-phonon lines (ZPLs) from isolated defects in hexagonal boron nitride (HBN) and compare our findings with the predictions of a Huang-Rhys model involving two electronic states. Our survey, which spans the spectral range ∼550-740 nm, reveals that, in disagreement with a two-level model, the absorption and emission dipoles are often misaligned. We relate the dipole misalignment angle (Δθ) of a ZPL to its energy shift from the excitation energy (ΔE) and find that Δθ≈0° when ΔE corresponds to an allowed HBN phonon frequency and that 0°≤Δθ≤90° when ΔE exceeds the maximum allowed HBN phonon frequency. Consequently, a two-level Huang-Rhys model succeeds at describing excitations mediated by the creation of one optical phonon but fails at describing excitations that require the creation of multiple phonons. We propose that direct excitations requiring the creation of multiple phonons are inefficient due to the low Huang-Rhys factors in HBN and that these ZPLs are instead excited indirectly via an intermediate electronic state. This hypothesis is corroborated by polarization measurements of an individual ZPL excited with two distinct wavelengths that indicate a single ZPL may be excited by multiple mechanisms. These findings provide new insight on the nature of the optical cycle of novel defect-based single-photon sources in HBN.

Temperature Dependence of Wavelength Selectable Zero-Phonon Emission from Single Defects in Hexagonal Boron Nitride.

We investigate the distribution and temperature-dependent optical properties of sharp, zero-phonon emission from defect-based single photon sources in multilayer hexagonal boron nitride (h-BN) flakes. We observe sharp emission lines from optically active defects distributed across an energy range that exceeds 500 meV. Spectrally resolved photon-correlation measurements verify single photon emission, even when multiple emission lines are simultaneously excited within the same h-BN flake. We also present a detailed study of the temperature-dependent line width, spectral energy shift, and intensity for two different zero-phonon lines centered at 575 and 682 nm, which reveals a nearly identical temperature dependence despite a large difference in transition energy. Our temperature-dependent results are well described by a lattice vibration model that considers piezoelectric coupling to in-plane phonons. Finally, polarization spectroscopy measurements suggest that whereas the 575 nm emission line is directly excited by 532 nm excitation, the 682 nm line is excited indirectly.

High Dynamic Range Pixel Array Detector for Scanning Transmission Electron Microscopy.

We describe a hybrid pixel array detector (electron microscope pixel array detector, or EMPAD) adapted for use in electron microscope applications, especially as a universal detector for scanning transmission electron microscopy. The 128×128 pixel detector consists of a 500 µm thick silicon diode array bump-bonded pixel-by-pixel to an application-specific integrated circuit. The in-pixel circuitry provides a 1,000,000:1 dynamic range within a single frame, allowing the direct electron beam to be imaged while still maintaining single electron sensitivity. A 1.1 kHz framing rate enables rapid data collection and minimizes sample drift distortions while scanning. By capturing the entire unsaturated diffraction pattern in scanning mode, one can simultaneously capture bright field, dark field, and phase contrast information, as well as being able to analyze the full scattering distribution, allowing true center of mass imaging. The scattering is recorded on an absolute scale, so that information such as local sample thickness can be directly determined. This paper describes the detector architecture, data acquisition system, and preliminary results from experiments with 80-200 keV electron beams.

Strong Photon-Magnon Coupling Using a Lithographically Defined Organic Ferrimagnet.

A cavity-magnonic system composed of a superconducting microwave resonator coupled to a magnon mode hosted by the organic-based ferrimagnet vanadium tetracyanoethylene (V[TCNE]x) is demonstrated. This work is motivated by the challenge of scalably integrating a low-damping magnetic system with planar superconducting circuits. V[TCNE]x has ultra-low intrinsic damping, can be grown at low processing temperatures on arbitrary substrates, and can be patterned via electron beam lithography. The devices operate in the strong coupling regime, with a cooperativity exceeding 1000 for coupling between the Kittel mode and the resonator mode at T≈0.4 K, suitable for scalable quantum circuit integration. Higher-order magnon modes are also observed with much narrower linewidths than the Kittel mode. This work paves the way for high-cooperativity hybrid quantum devices in which magnonic circuits can be designed and fabricated as easily as electrical wires.

Dephasing by optical phonons in GaN defect single-photon emitters.

Single-photon defect emitters (SPEs), especially those with magnetically and optically addressable spin states, in technologically mature wide bandgap semiconductors are attractive for realizing integrated platforms for quantum applications. Broadening of the zero phonon line (ZPL) caused by dephasing in solid state SPEs limits the indistinguishability of the emitted photons. Dephasing also limits the use of defect states in quantum information processing, sensing, and metrology. In most defect emitters, such as those in SiC and diamond, interaction with low-energy acoustic phonons determines the temperature dependence of the dephasing rate and the resulting broadening of the ZPL with the temperature obeys a power law. GaN hosts bright and stable single-photon emitters in the 600-700 nm wavelength range with strong ZPLs even at room temperature. In this work, we study the temperature dependence of the ZPL spectra of GaN SPEs integrated with solid immersion lenses with the goal of understanding the relevant dephasing mechanisms. At temperatures below ~ 50 K, the ZPL lineshape is found to be Gaussian and the ZPL linewidth is temperature independent and dominated by spectral diffusion. Above ~ 50 K, the linewidth increases monotonically with the temperature and the lineshape evolves into a Lorentzian. Quite remarkably, the temperature dependence of the linewidth does not follow a power law. We propose a model in which dephasing caused by absorption/emission of optical phonons in an elastic Raman process determines the temperature dependence of the lineshape and the linewidth. Our model explains the temperature dependence of the ZPL linewidth and lineshape in the entire 10-270 K temperature range explored in this work. The ~ 19 meV optical phonon energy extracted by fitting the model to the data matches remarkably well the ~ 18 meV zone center energy of the lowest optical phonon band ([Formula: see text]) in GaN. Our work sheds light on the mechanisms responsible for linewidth broadening in GaN SPEs. Since a low energy optical phonon band ([Formula: see text]) is a feature of most group III-V nitrides with a wurtzite crystal structure, including hBN and AlN, we expect our proposed mechanism to play an important role in defect emitters in these materials as well.

Excited-state spin-resonance spectroscopy of V[Formula: see text] defect centers in hexagonal boron nitride.

The recently discovered spin-active boron vacancy (V[Formula: see text]) defect center in hexagonal boron nitride (hBN) has high contrast optically-detected magnetic resonance (ODMR) at room-temperature, with a spin-triplet ground-state that shows promise as a quantum sensor. Here we report temperature-dependent ODMR spectroscopy to probe spin within the orbital excited-state. Our experiments determine the excited-state spin Hamiltonian, including a room-temperature zero-field splitting of 2.1 GHz and a g-factor similar to that of the ground-state. We confirm that the resonance is associated with spin rotation in the excited-state using pulsed ODMR measurements, and we observe Zeeman-mediated level anti-crossings in both the orbital ground- and excited-state. Our observation of a single set of excited-state spin-triplet resonance from 10 to 300 K is suggestive of symmetry-lowering of the defect system from D3h to C2v. Additionally, the excited-state ODMR has strong temperature dependence of both contrast and transverse anisotropy splitting, enabling promising avenues for quantum sensing.

Lorentz electron ptychography for imaging magnetic textures beyond the diffraction limit.

Nanoscale spin textures, especially magnetic skyrmions, have attracted intense interest as candidate high-density and power-efficient information carriers for spintronic devices1,2. Facilitating a deeper understanding of sub-hundred-nanometre to atomic-scale spin textures requires more advanced magnetic imaging techniques3-5. Here we demonstrate a Lorentz electron ptychography method that can enable high-resolution, high-sensitivity magnetic field imaging for widely available electron microscopes. The resolution of Lorentz electron ptychography is not limited by the usual diffraction limit of lens optics, but instead is determined by the maximum scattering angle at which a statistically meaningful dose can still be recorded-this can be an improvement of up to 2-6 times depending on the allowable dose. Using FeGe as the model system, we realize a more accurate magnetic field measurement of skyrmions with an improved spatial resolution and sensitivity by also correcting the probe-damping effect from the imaging optics via Lorentz electron ptychography. This allows us to directly resolve subtle internal structures of magnetic skyrmions near the skyrmion cores, boundaries and dislocations in an FeGe single crystal. Our study establishes a quantitative, high-resolution magnetic microscopy technique that can reveal nanoscale spin textures, especially magnetization discontinuities and topological defects in nanomagnets6. The technique's high-dose efficiency should also make it well suited for the exploration of magnetic textures in electron radiation-sensitive materials such as organic or molecular magnets7.

Nuclear import of serum response factor in airway smooth muscle.

We have previously shown that the transcription-promoting activity of serum response factor (SRF) is partially regulated by its extranuclear redistribution. In this study, we examined the cellular mechanisms that facilitate SRF nuclear entry in canine tracheal smooth muscle cells. We used in vitro pull-down assays to determine which karyopherin proteins bound SRF and found that SRF binds KPNA1 and KPNB1 through its nuclear localization sequence. Immunoprecipitation studies also demonstrated direct SRF-KPNA1 interaction in HEK293 cells. Import assays demonstrated that KPNA1 and KPNB1 together were sufficient to mediate rapid nuclear import of SRF-GFP. Our studies also suggest that SRF is able to gain nuclear entry through an auxiliary, nuclear localization sequence-independent mechanism.

Chip-scale nanofabrication of single spins and spin arrays in diamond.

We demonstrate a technique to nanofabricate nitrogen vacancy (NV) centers in diamond based on broad-beam nitrogen implantation through apertures in electron beam lithography resist. This method enables high-throughput nanofabrication of single NV centers on sub-100-nm length scales. Secondary ion mass spectroscopy measurements facilitate depth profiling of the implanted nitrogen to provide three-dimensional characterization of the NV center spatial distribution. Measurements of NV center coherence with on-chip coplanar waveguides suggest a pathway for incorporating this scalable nanofabrication technique in future quantum applications.

Solution-Processable Thermally Crosslinked Organic Radical Polymer Battery Cathodes.

Organic radical polymers are promising cathode materials for next-generation batteries because of their rapid charge transfer and high cycling stability. However, these organic polymer electrodes gradually dissolve in the electrolyte, resulting in capacity fade. Several crosslinking methods have been developed to improve the performance of these electrodes, but they are either not compatible with carbon additives or compromise the solution processability of the electrodes. A one-step post-synthetic, carbon-compatible crosslinking method was developed to effectively crosslink an organic polymer electrode and allow for easy solution processing. The highest electrode capacity of 104 mAh g-1 (vs. a theoretical capacity of 111 mAh g-1 ) is achieved by introducing 1 mol % of the crosslinker, whereas the highest capacity retention (99.6 %) is obtained with 3 mol % crosslinker. In addition, mass transfer was observed in situ by using electrochemical quartz crystal microbalance with dissipation monitoring. These results may guide future electrode design toward fast-charging and high-capacity organic electrodes.

Local Photothermal Control of Phase Transitions for On-Demand Room-Temperature Rewritable Magnetic Patterning.

The ability to make controlled patterns of magnetic structures within a nonmagnetic background is essential for several types of existing and proposed technologies. Such patterns provide the foundation of magnetic memory and logic devices, allow the creation of artificial spin-ice lattices, and enable the study of magnon propagation. Here, a novel approach for magnetic patterning that allows repeated creation and erasure of arbitrary shapes of thin-film ferromagnetic structures is reported. This strategy is enabled by epitaxial Fe0.52 Rh0.48 thin films designed so that both ferromagnetic and antiferromagnetic phases are bistable at room temperature. Starting with the film in a uniform antiferromagnetic state, the ability to write arbitrary patterns of the ferromagnetic phase is demonstrated by local heating with a focused laser. If desired, the results can then be erased by cooling below room temperature and the material repeatedly re-patterned.

Impact of the Synthesis Method on the Solid-State Charge Transport of Radical Polymers.

There are conflicting reports in the literature about the presence of room temperature conductivity in poly(2,2,6,6-tetramethylpiperidinyloxy methacrylate) (PTMA), a redox active polymer with radical groups pendent to an insulating backbone. To understand the variability in the findings across the literature and synthetic methods, we prepared PTMA using three living methods - anionic, ATRP and RAFT polymerization. We find that all three synthetic methods produce PTMA with radical yields of 70 - 80%, controlled molecular weight, and low dispersity. Additionally, we used on-chip EPR to probe the robustness of radical content in solid films under ambient air and light, and found negligible change in the radical content over time. Electrically, we found that PTMA is highly insulating - conductivity in the range 10-11 S/cm - regardless of the synthetic method of preparation. These findings provide greater clarity for potential applications of PTMA in energy storage.

Theory and practice of electron diffraction from single atoms and extended objects using an EMPAD.

What does the diffraction pattern from a single atom look like? How does it differ from the scattering from long-range potential? With the development of new high-dynamic range pixel array detectors to measure the complete momentum distribution, these questions have immediate relevance for designing and understanding momentum-resolved imaging modes. We explore the asymptotic limits of long-range and short-range potentials. We use a simple quantum mechanical model to explain the general and asymptotic limits for the probability distribution in both real and reciprocal space. Features in the scattering potential much larger than the probe size cause the bright field (BF) disk to deflect uniformly, while features much smaller than the probe size, instead of a deflection, cause a redistribution of intensity within the BF disk. Because long-range and short-range features are encoded differently in the diffraction pattern, it is possible to separate their contributions in differential phase-contrast (DPC) or center-of-mass (CoM) imaging. The shape profiles for atomic resolution CoM imaging are dominated by the shape of the probe gradient and not the highly singular atomic potentials or their local fields. Instead, only the peak height shows an atomic number sensitivity, whose precise dependence is determined by the convergence angle. At lower convergence angles, the contrast oscillates with increasing atomic number, similar to BF imaging. The range of collection angles impacts DPC and CoM imaging differently, with CoM being more sensitive to the upper cutoff limit, while DPC is more sensitive to the lower cutoff.

Chemical Vapor Deposition Growth of Large Single-Crystal Mono-, Bi-, Tri-Layer Hexagonal Boron Nitride and Their Interlayer Stacking.

Two-dimensional hexagonal boron nitride (h-BN) is a wide bandgap material which has promising mechanical and optical properties. Here we report the realization of an initial nucleation density of h-BN <1 per mm2 using low-pressure chemical vapor deposition (CVD) on polycrystalline copper. This enabled wafer-scale CVD growth of single-crystal monolayer h-BN with a lateral size up to ∼300 µm, bilayer h-BN with a lateral size up to ∼60 µm, and trilayer h-BN with a lateral size up to ∼35 µm. Based on the large single-crystal monolayer h-BN domain, the sizes of the as-grown bi- and trilayer h-BN grains are 2 orders of magnitude larger than typical h-BN multilayer domains. In addition, we achieved coalesced h-BN films with an average grain size ∼100 µm. Various flake morphologies and their interlayer stacking configurations of bi- and trilayer h-BN domains were studied. Raman signatures of mono- and multilayer h-BN were investigated side by side in the same film. It was found that the Raman peak intensity can be used as a marker for the number of layers.

Polarization Spectroscopy of Defect-Based Single Photon Sources in ZnO.

Point defects in wide bandgap semiconductors are promising candidates for future applications that necessitate quantum light sources. Recently, defect-based single photon sources have been observed in ZnO that are very bright and remain photoactive from 4.5 K to room temperature. Despite several investigations, the structure and electronic states of these emitters remain unknown. In this work, we establish a procedure to distinguish a Z dipole from an XY dipole when studying quantum emitters that are randomly oriented. Our cryogenic and room temperature polarization measurements collectively establish that these unidentified ZnO quantum emitters have a Z dipole. We show that the associated absorption and emission dipoles are parallel within experimental uncertainty for all 32 individuals studied. Additionally, we apply group theory and find that, assuming the defect symmetry belongs to a point group relevant to the ZnO wurtzite lattice, the ground and excited states are orbital singlets. These results are a significant step in identifying the structure and electronic states of defect-based single photon sources in ZnO.