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At least 91 records · Page 5

Stroboscopic x-ray diffraction microscopy of dynamic strain in diamond thin-film bulk acoustic resonators for quantum control of nitrogen-vacancy centers

Bulk-mode acoustic waves in a crystalline material exert lattice strain through the thickness of the sample, which couples to the spin Hamiltonian of defect-based qubits such as the nitrogen-vacancy (N-V) center defect in diamond. This mechanism has previously been harnessed for unconventional quantum spin control, spin decoherence protection, and quantum sensing. Bulk-mode acoustic wave devices are also important in the microelectronics industry as microwave filters. A key challenge in both applications is a lack of appropriate operando microscopy tools for quantifying and visualizing gigahertz-frequency dynamic strain. Here, in this work, we directly image acoustic strain within N-V center-coupled diamond thin-film bulk acoustic wave resonators using stroboscopic scanning hard x-ray diffraction microscopy at the Advanced Photon Source. The far-field scattering patterns of the nanofocused x-ray diffraction encode strain information entirely through the illuminated thickness of the resonator. These patterns have a real-space spatial variation that is consistent with the bulk strain’s expected modal distribution and a momentum-space angular variation from which the strain amplitude can be quantitatively deduced. We also perform optical measurements of strain-driven Rabi precession of of the N-V center spin ensemble, providing an additional quantitative measurement of the strain amplitude. As a result, we directly measure one of the six N-V spin-stress coupling parameters, 𝑏 =2.73⁢(2) MHz/GPa, by correlating these measurements at the same spatial position and applied microwave power. Our results demonstrate a unique technique for directly imaging ac lattice strain in micromechanical structures and provide a direct measurement of a fundamental constant for the N-V center defect spin Hamiltonian.

acoustic techniques↗

A scanning resonator for probing quantum coherent devices

Superconducting resonators with high quality factors are extremely sensitive detectors of the complex impedance of materials and devices coupled to them. This capability has been used to measure losses in multiple different materials and, in the case of circuit quantum electrodynamics (circuit QED), has been used to measure the coherent evolution of multiple different types of qubits. Here, we report on the implementation of a scanning resonator for probing quantum coherent devices. Our scanning setup enables tunable coherent coupling to systems of interest without the need for fabricating on-chip superconducting resonators. We measure the internal quality factor of our resonator sensor in the single-photon regime to be >104 and demonstrate capacitive imaging using our sensor with zeptoFarad sensitivity and micron spatial resolution at milliKelvin temperatures. We then use our setup to characterize the energy spectrum and coherence times of multiple transmon qubits with no on-chip readout circuitry. Our experiments introduce a new tool for using circuit QED to measure existing and proposed qubit platforms.

47 OTHER INSTRUMENTATION↗

Atomic Force Microscope Active Optical Probe for Single-Molecule Imaging and Time-Resolved Optical Spectroscopy (DOE SBIR Phase II/IIA Final Report)

Actoprobe LLC reports on the results of its DOE SBIR Phase II/IIA project on the development of Atomic Force Microscope Active Optical Probe for Single-Molecule Imaging and Time-Resolved Optical Spectroscopy. While chemistry science and technology greatly benefit from Atomic Force Microscopy in surface characterization, time-resolved chemical imaging on the single-molecule level lags far behind. Current scanning probe microscopy only obtains information about mechanical but not optical/chemical properties. To address this problem, the Actoprobe LLC research team has proposed a novel class of Atomic Force Microscopy probes, Ultra-Fast Pulsed Active Atomic Force Microscopy Optical Probes (UFP AAOPs), that will allow ultrafast time-resolved optical and chemical imaging at the nanoscale. As envisioned, these unique optical probes will perform the functions of conventional Atomic Force Microscopy probes and, in addition, will simultaneously provide chemical information about molecular scale interactions. This innovation is accomplished by integrating an ultrafast pulsed Quantum Dot laser source into an Atomic Force Microscopy probe. This report describes our progress with the fabrication of an ultrafast micrometer-size semiconductor laser, based on “artificial atoms” - Quantum Dots, integrated with an Atomic Force Microscopy probe. In this Phase II/IIA project, we have demonstrated the feasibility of the UFP AAOP concept by fabricating a first prototype of the UFP AAOP. The excellent performance of the probe has been proven in terms of AFM and optical spatial resolution through rigorous tests. The UFP AAOP provides pulses with less than 4 ps duration and higher than 11 GHz repetition rate, and spatial resolution better than 300 nm at 1240 nm wavelength. Technically, it is possible to reduce the pulse width to less than 1 ps and to improve lateral resolution to ~ 0.5 nm, which implies the potential capability for the probe to characterize chemical compounds with single-molecule resolution. The UFP AAOP fabrication procedure has been developed for wafer-scale production of multiple devices, with the yield of the process estimated to be lower than 1% with the limited fabrication capabilities and equipment available for use in the research project. However, using high-volume production tools and special GaAs processing equipment, the yield can be significantly improved, theoretically to ~ 50%. Finally, economic feasibility and scale-up manufacturing potential were analyzed for UFP AAOP and found to be very promising. In summary, the Actoprobe team has successfully demonstrated the feasibility of the UFP AAOP concept.

36 MATERIALS SCIENCE↗

Direct-bonded diamond membranes for heterogeneous quantum and electronic technologies

Diamond has superlative material properties for a broad range of quantum and electronic technologies. However, heteroepitaxial growth of single crystal diamond remains limited, impeding integration and evolution of diamond-based technologies. Here, we directly bond single-crystal diamond membranes to a wide variety of materials including silicon, fused silica, sapphire, thermal oxide, and lithium niobate. Our bonding process combines customized membrane synthesis, transfer, and dry surface functionalization, allowing for minimal contamination while providing pathways for near unity yield and scalability. We generate bonded crystalline membranes with thickness as low as 10 nm, sub-nm interfacial regions, and nanometer-scale thickness variability over 200 by 200 μm 2 areas. We measure spin coherence times T 2 for nitrogen vacancy centers in 150 nm-thick bonded membranes of up to 623 ± 21 μs, suitable for advanced quantum applications. We demonstrate multiple methods for integrating high quality factor nanophotonic cavities with the diamond heterostructures, highlighting the platform versatility in quantum photonic applications. Furthermore, we show that our ultra-thin diamond membranes are compatible with total internal reflection fluorescence (TIRF) microscopy, which enables interfacing coherent diamond quantum sensors with living cells while rejecting unwanted background luminescence. The processes demonstrated herein provide a full toolkit to synthesize heterogeneous diamond-based hybrid systems for quantum and electronic technologies.

color center↗

Defect Complexes in CrSBr Revealed Through Electron Microscopy and Deep Learning

Atomic defects underpin the properties of van der Waals materials, and their understanding is essential for advancing quantum and energy technologies. Scanning transmission electron microscopy is a powerful tool for defect identification in atomically thin materials, and extending it to multilayer and beam-sensitive materials would accelerate their exploration. Here, we establish a comprehensive defect library in a bilayer of the magnetic quasi-1D semiconductor CrSBr by combining atomic-resolution imaging, deep learning, and calculations. We apply a custom-developed machine learning work flow to detect, classify, and average point vacancy defects. This classification enables us to uncover several distinct Cr interstitial defect complexes, combined Cr and Br vacancy defect complexes, and lines of vacancy defects that extend over many unit cells. We show that their occurrence is in agreement with our computed structures and binding energy densities, reflecting the intriguing layer interlocked crystal structure of CrSBr. Our ab initio calculations show that the interstitial defect complexes give rise to highly localized electronic states. These states are of particular interest due to the reduced electronic dimensionality and magnetic properties of CrSBr and are, furthermore, predicted to be optically active. Our results broaden the scope of defect studies in challenging materials and reveal new defect types in bilayer CrSBr that can be extrapolated to the bulk and to over 20 materials belonging to the same FeOCl structural family.

deep learning↗

Data for Magnetic Anisotropy due to Localized Structural Defects in Strained Yttrium Iron Garnet Thin Films

This dataset contains electron microscopy, magnetic, and X-ray diffraction characterization data for YIG/YSGG thin films associated with the manuscript "Magnetic anisotropy due to localized structural defects in strained yttrium iron garnet thin films". Characterizations include: scanning electron nano diffraction (SEND, or 4D-STEM), dark field transmission electron microscopy (DF-TEM), energy dispersive X-ray spectroscopy (EDS), ferrimagnetic resonance (FMR), superconducting quantum interference device (SQUID), scanning transmission electron microscopy (STEM), X-ray diffraction (XRD).

Electron microscopy↗

A Processing and Analytics System for Microscopy Data Workflows: The Pycroscopy Ecosystem of Packages

Major advancements in fields as diverse as biology and quantum computing have relied on a multitude of microscopy techniques. Despite the considerable proliferation of these instruments, significant bottlenecks remain in terms of processing, analysis, storage, and retrieval of the acquired datasets. Aside from lack of file standards, individual domain-specific analysis packages are often disjoint from the underlying datasets, and thus keeping track of analysis and processing steps remains tedious for the end-user, hampering reproducibility. Here, in this study, the pycroscopy ecosystem of packages is introduced, an open-source python-based ecosystem underpinned by a common data model. The data model, termed the N-dimensional spectral imaging data format, is realized in pycroscopy's sidpy package. This package is built on top of dask arrays, thus leveraging dask array attributes, but expanding them to accelerate microscopy relevant analysis and visualization. Several examples of the use of the pycroscopy ecosystem to create workflows for data ingestion and analysis of scanning transmission electron microscopy (STEM) and scanning probe microscopy data are shown. Adoption of such standardized routines will be critical to usher in the next generation of autonomous instruments where processing, computation, and meta-data storage will be critical to overall experimental operations.

97 MATHEMATICS AND COMPUTING↗

Activating dislocation mediated plasticity in boron carbide through Al-doping

Dislocation slip, deformation twinning, phase transformations, and fast fracture are energy dissipation mechanisms that accommodate mechanical loading in materials. The energetically unfavorable formation of dislocation attributes to the ease of cracking and the low damage tolerance observed in superhard ceramics, notably boron carbide. Here, this work demonstrates that room temperature dislocation slip can be enabled in boron carbide by altering its chemistry through Al doping. The activation of dislocation slip is mechanistically explained by quantum mechanics simulations and electron microscopy, which indicate that strain energy is released through basal icosahedral slip facilitated by icosahedral rotation and chain bond breaking and reconfiguring. The new insight gained through this work suggests that atomic doping could be an effective strategy to tune deformation mechanisms in boron carbide, which provides a significant potential for limiting amorphization and catastrophic failure, and opens a new strategy to enhance damage tolerance in brittle ceramics.

36 MATERIALS SCIENCE↗

Variations of light emission and carrier dynamics around V-defects in InGaN quantum wells

Time- and spectrally-resolved scanning near-field optical microscopy was applied to study spatial variations of photoluminescence (PL) spectra and carrier dynamics in polar InGaN/GaN single quantum wells (QWs) emitting from 410 nm to 570 nm. The main attention was devoted to variations of PL properties and carrier dynamics around V-defects. The PL intensity, peak wavelength, and linewidth, as well as the radiative and nonradiative recombination times, were found to be different in V-defect-rich and defect-free regions. The radiative lifetime close to the defects was longer up to several times, which is attributed to an increased electron and hole wave function separation in the QW plane. PL decay times, measured using excitation and collection through the near-field probe, were one to two orders of magnitude shorter than PL decay times measured in the far field. This shows that the near-field PL decay and the integrated PL intensity are primarily determined by the carrier out-diffusion from under the probe. Only in the immediate vicinity of the V-defects, the near-field PL decays due to the nonradiative recombination at dislocations. The area of such enhanced nonradiative recombination is limited to just a few percent of the total QW area. This shows that recombination via dislocations and V-defects does not play a decisive role in the overall nonradiative recombination and internal quantum efficiency of polar InGaN/GaN QWs.

36 MATERIALS SCIENCE↗

Inducing Circularly Polarized Single-Photon Emission via Chiral-Induced Spin Selectivity

One of the central aims of the field of spintronics is the control of individual electron spins to effectively manage the transmission of quantized data. One well-known mechanism for controlling electronic spin transport is the chiral-induced spin-selectivity (CISS) effect in which a helical nanostructure imparts a preferential spin orientation on the electronic transport. One potential application of the CISS effect is as a transduction pathway between electronic spin and circularly polarized light within nonreciprocal photonic devices. Here in this work, we identify and quantify the degree of chiral-induced spin-selective electronic transport in helical polyaniline films using magnetoconductive atomic force microscopy (mcAFM). We then induce circularly polarized quantum light emission from CdSe/CdS core/shell quantum dots placed on these films, demonstrating a degree of circular polarization of up to ~21%. Utilizing time-resolved photoluminescence microscopy, we measure the radiative lifetime difference associated with left- and right-handed circular polarizations of single emitters. These lifetime differences, in combination with Kelvin probe mapping of the variation of surface potential with magnetization of the substrate, help establish an energy level diagram describing the spin-dependent transport pathways that enable the circularly polarized photoluminescence.

36 MATERIALS SCIENCE↗

Quantum Enhanced Probes of Magnetic Circular Dichroism

Magneto-optical microscopies, including optical measurements of magnetic circular dichroism, are increasingly ubiquitous tools for probing spin-orbit coupling, charge-carrier g-factors, and chiral excitations in matter, but the minimum detectable signal in classical magnetic circular dichroism measurements is fundamentally limited by the shot-noise limit of the optical readout field. Here, a two-mode squeezed light source is used to improve the minimum detectable signal in magnetic circular dichroism measurements by 3 decibels compared with state-of-the-art classical measurements, even with relatively lossy samples like terbium gallium garnet. Furthermore, these results provide a framework for new quantum-enhanced magneto-optical microscopies that are particularly critical for environmentally sensitive materials and for low temperature measurements where increased optical power can introduce unacceptable thermal perturbations.

42 ENGINEERING↗

Viewing Optical Processes at the Nanoscale: Combining Scanning Tunneling Microscopy and Optical Spectroscopy

The combination of optical spectroscopy and scanning tunneling microscopy techniques has the potential to yield the unambiguous single-molecule level insight required to fully understand the complex structure–property relationship of emerging material systems. In this Perspective, we highlight the recent progress of single-molecule absorption detected by scanning tunneling microscopy (SMA-STM) to investigate light–matter interactions of supported (nano)particles, quantum dots, and molecular and thin films at the nanoscale. We further show how the SMA-STM technique has been recently extended to expand the classes of materials that can be investigated as well as recent design modifications that enable both time-resolved imaging and tomography. Finally, we hypothesize how these modifications can be further leveraged to advance our current knowledge of light–matter interactions and how the resulting nanoscale insight can be implemented for future material applications.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Imaging moiré excited states with photocurrent tunnelling microscopy

Moiré superlattices provide a highly tuneable and versatile platform to explore novel quantum phases and exotic excited states ranging from correlated insulators to moiré excitons. Scanning tunnelling microscopy has played a key role in probing microscopic behaviours of the moiré correlated ground states at the atomic scale. However, imaging of quantum excited states in moiré heterostructures remains an outstanding challenge. In this report we develop a photocurrent tunnelling microscopy technique that combines laser excitation and scanning tunnelling spectroscopy to directly visualize the electron and hole distribution within the photoexcited moiré exciton in twisted bilayer WS 2 . The tunnelling photocurrent alternates between positive and negative polarities at different locations within a single moiré unit cell. This alternating photocurrent originates from the in-plane charge transfer moiré exciton in twisted bilayer WS 2 , predicted by our GW-Bethe–Salpeter equation calculations, that emerges from the competition between the electron–hole Coulomb interaction and the moiré potential landscape. Our technique enables the exploration of photoexcited non-equilibrium moiré phenomena at the atomic scale.

36 MATERIALS SCIENCE↗

Visualizing the impact of quenched disorder on 2D electron Wigner solids

Electron Wigner solids (WSs) provide an ideal system for understanding the competing effects of electron–electron and electron–disorder interactions, a central unsolved problem in condensed matter physics. Progress in this topic has been limited by a lack of single-defect-resolved experimental measurements as well as accurate theoretical tools to enable realistic experiment/theory comparison. Here, in this study, we overcome these limitations by combining atomically resolved scanning tunnelling microscopy (STM) with neural-quantum-state quantum Monte Carlo (NQS-QMC) simulation of disordered 2D electron WSs to discover new disorder-induced physical regimes of correlated electron behaviour. STM was used to image the electron density (n e )-dependent evolution of electron WSs in gate-tunable bilayer MoSe 2 (BL-MoSe 2 ) devices with varying long-range (n LR ) and short-range (n SR ) disorder densities. These images were compared with NQS-QMC simulations using realistic disorder maps extracted from experiment, thus allowing the roles of different disorder types to be disentangled. We identify two distinct physical regimes for disordered electron WSs that depend on n SR . For n SR ≲ n e , the WS behaviour is dominated by long-range disorder and features extensive mixed solid–liquid phases, a new type of local re-entrant melting/crystallization and prominent Friedel oscillations. By contrast, when n SR ≫ n e , these features are suppressed and a more robust amorphous WS phase emerges that persists to higher n e , highlighting the importance of short-range disorder in this regime. Our work establishes a powerful framework for studying disordered quantum solids through a combined experimental–theoretical approach.

Ge, Zhehao [University of California, Berkeley, CA↗

Colors of entangled two-photon absorption

Multiphoton absorption of entangled photons offers ways for obtaining unique information about chemical and biological processes. Measurements with entangled photons may enable sensing biological signatures with high selectivity and at very low light levels to protect against photodamage. In this paper, we present a theoretical and experimental study of the excitation wavelength dependence of the entangled two-photon absorption (ETPA) process in a molecular system, which provides insights into how entanglement affects molecular spectra. We demonstrate that the ETPA excitation spectrum can be different from that of classical TPA as well as that for one-photon resonant absorption (OPA) with photons of doubled frequency. These results are modeled by assuming the ETPA cross-section is governed by a two-photon excited state radiative linewidth rather than by electron-phonon interactions, and this leads to excitation spectra that match the observed results. Further, we find that the two-photon-allowed states with highest TPA and ETPA intensities have high electronic entanglements, with ETPA especially favoring states with the longest radiative lifetimes. These results provide concepts for the development of quantum light–based spectroscopy and microscopy that will lead to much higher efficiency of ETPA sensors and low-intensity detection schemes.

Science & Technology - Other Topics↗

Waveform analysis of a large-area superconducting nanowire single photon detector

Superconducting nanowire single photon detectors (SNSPDs) are typically used as single-mode-fiber-coupled single-pixel detectors, but large area detectors are increasingly critical for applications ranging from microscopy to free-space quantum communications. However, the long meander-line length of such large-area SNSPDs results in a proportionately large kinetic inductance that affects the waveform generated by the device. Here, we explore changes in the rising edge of the readout pulse for a single-pixel large-area SNSPD as a function of the optical spot size on the detector and compare to the rising edge of the dark-count waveform. We observe a bimodal distribution of bright-count rise times and show that the probability of a slow rise time increases in the limit of large spot sizes, indicative of a position sensitive response. Additionally, in the limit of low bias currents, the dark-count readout pulse is most similar to the large spot-size bright-count readout pulse, which suggests that dark counts arise from locations spanning the device. Overall, these results are consistent with a simple model of traveling microwave modes excited by single photons incident at varying positions along the length of the nanowire.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Scanning SQUID microscopy in a cryogen-free dilution refrigerator

We report a scanning superconducting quantum interference device (SQUID) microscope in a cryogen-free dilution refrigerator with a base temperature at the sample stage of at least 30 mK. The microscope is rigidly mounted to the mixing chamber plate to optimize thermal anchoring of the sample. The microscope housing fits into the bore of a superconducting vector magnet, and our design accommodates a large number of wires connecting the sample and sensor. Through a combination of vibration isolation in the cryostat and a rigid microscope housing, we achieve relative vibrations between the SQUID and the sample that allow us to image with micrometer resolution over a 150 μm range while the sample stage temperature remains at base temperature. To demonstrate the capabilities of our system, we show images acquired simultaneously of the static magnetic field, magnetic susceptibility, and magnetic fields produced by a current above a superconducting micrometer-scale device.

47 OTHER INSTRUMENTATION↗