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Electronic spectroscopy of zero-dimensional (0D) quantum systems, including point defects in solids, atomic states, and small molecules, is a critical tool for developing a fundamental understanding of these systems, with applications ranging from solid-state and molecular materials development to emerging technologies rooted in quantum information science. Toward this end, scanning tunneling spectroscopy (STS) has demonstrated atomic-scale sensitivity, but is not easily scalable for applications, whereas device-based approaches rely on embedding these systems within a solid-state tunnel junction (TJ) and are not generally applicable. Here we demonstrate an all-electrical readout mechanism for these quasi-0D states that is modular and general, dramatically expanding the phase space of accessible quantum systems and providing an approach that is amenable to scaling and integration with other solid-state quantum technologies. Our approach relies on the creation of high-quality tunnel junctions via the mechanical exfoliation and stacking of multi-layer graphene (MLG) and hexagonal boron nitride (hBN) to encapsulate the target quantum system (QS) in an MLG/hBN/QS/hBN/MLG heterostructure. This structure allows for electronic spectroscopy and readout of candidate quantum systems through a combination of Coulomb and spin-blockade, providing access to entire classes of quantum systems that have previously only been accessible via optical spectroscopy or magnetic resonance measurements of large ensembles, if at all.

Spintronic, spin caloritronic, and magnonic phenomena arise from complex interactions between charge, spin, and structural degrees of freedom that are challenging to model and even more difficult to predict. This situation is compounded by the relative scarcity of magnetically-ordered materials with relevant functionality, leaving the field strongly constrained to work with a handful of well-studied systems that do not encompass the full phase space of phenomenology predicted by fundamental theory. Here we present an important advance in this coupled theory-experiment challenge, wherein we extend existing theories of the spin Seebeck effect (SSE) to explicitly include the temperature-dependence of magnon non-conserving processes. This expanded theory quantitatively describes the low-temperature behavior of SSE signals previously measured in the mainstay material yttrium iron garnet (YIG) and predicts a new regime for magnonic and spintronic materials that have low saturation magnetization, $M_S$, and ultra-low damping. Finally, we validate this prediction by directly observing the spin Seebeck resistance (SSR) in the molecule-based ferrimagnetic semiconductor vanadium tetracyanoethylene (V[TCNE]$_x$, $x \sim 2$). These results validate the expanded theory, yielding SSR signals comparable in magnitude to YIG and extracted magnon diffusion length ($\lambda_m>1$ $\mu$ m) and magnon lifetime for V[TCNE]$_x$ ($\tau_{th}\approx 1-10$ $\mu$ s) exceeding YIG ($\tau_{th}\sim 10$ ns). Surprisingly, these properties persist to room temperature despite relatively low spin wave stiffness (exchange). This identification of a new regime for highly efficient SSE-active materials opens the door to a new class of magnetic materials for spintronic and magnonic applications.

We demonstrate indirect electric-field control of ferromagnetic resonance (FMR) in devices that integrate the low-loss, molecule-based, room-temperature ferrimagnet vanadium tetracyanoethylene (V[TCNE]$_{x \sim 2}$) mechanically coupled to PMN-PT piezoelectric transducers. Upon straining the V[TCNE]$_x$ films, the FMR frequency is tuned by more than 6 times the resonant linewidth with no change in Gilbert damping for samples with $\alpha = 6.5 \times 10^{-5}$. We show this tuning effect is due to a strain-dependent magnetic anisotropy in the films and find the magnetoelastic coefficient $|\lambda_S| \sim (1 - 4.4)$ ppm, backed by theoretical predictions from DFT calculations and magnetoelastic theory. Noting the rapidly expanding application space for strain-tuned FMR, we define a new metric for magnetostrictive materials, $\textit{magnetostrictive agility}$, given by the ratio of the magnetoelastic coefficient to the FMR linewidth. This agility allows for a direct comparison between magnetostrictive materials in terms of their comparative efficacy for magnetoelectric applications requiring ultra-low loss magnetic resonance modulated by strain. With this metric, we show V[TCNE]$_x$ is competitive with other magnetostrictive materials including YIG and Terfenol-D. This combination of ultra-narrow linewidth and magnetostriction in a system that can be directly integrated into functional devices without requiring heterogeneous integration in a thin-film geometry promises unprecedented functionality for electric-field tuned microwave devices ranging from low-power, compact filters and circulators to emerging applications in quantum information science and technology.

We demonstrate a hybrid quantum system composed of superconducting resonator photons and magnons hosted by the organic-based ferrimagnet vanadium tetracyanoethylene (V[TCNE]$_x$). Our work is motivated by the challenge of scalably integrating an arbitrarily-shaped, low-damping magnetic system with planar superconducting circuits, thus enabling a host of quantum magnonic circuit designs that were previously inaccessible. For example, by leveraging the inherent properties of magnons, one can enable nonreciprocal magnon-mediated quantum devices that use magnon propagation rather than electrical current. We take advantage of the properties of V[TCNE]$_x$, which has ultra-low intrinsic damping, can be grown at low processing temperatures on arbitrary substrates, and can be patterned via electron beam lithography. We demonstrate the scalable, lithographically integrated fabrication of hybrid quantum magnonic devices consisting of a thin-film superconducting resonator coupled to a low-damping, thin-film V[TCNE]$_x$ microstructure. Our devices operate in the strong coupling regime, with a cooperativity as high as 1181(44) at T$\sim$0.4 K, suitable for scalable quantum circuit integration. This work paves the way for the exploration of high-cooperativity hybrid magnonic quantum devices in which magnonic circuits can be designed and fabricated as easily as electrical wires., Comment: 31 pages preprint format with supplementary materials

Quantum information science and technology (QIST) is a critical and emerging technology with the potential for enormous world impact and is currently invested in by over 40 nations. To bring these large-scale investments to fruition and bridge the lower technology readiness levels (TRLs) of fundamental research at universities to the high TRLs necessary to realize the promise of practical quantum advantage accessible to industry and the public, we present a roadmap for Quantum Technology Demonstration Projects (QTDPs). Such QTDPs, focused on intermediate TRLs, are large-scale public-private partnerships with a high probability of translation from laboratory to practice. They create technology demonstrating a clear 'quantum advantage' for science breakthroughs that are user-motivated and will provide access to a broad and diverse community of scientific users. Successful implementation of a program of QTDPs will have large positive economic impacts., Comment: Updated title and abstract

The rapidly growing quantum information science and engineering (QISE) industry will require both quantum-aware and quantum-proficient engineers at the bachelor's level. We provide a roadmap for building a quantum engineering education program to satisfy this need. For quantum-aware engineers, we describe how to design a first quantum engineering course accessible to all STEM students. For the education and training of quantum-proficient engineers, we detail both a quantum engineering minor accessible to all STEM majors, and a quantum track directly integrated into individual engineering majors. We propose that such programs typically require only three or four newly developed courses that complement existing engineering and science classes available on most larger campuses. We describe a conceptual quantum information science course for implementation at any post-secondary institution, including community colleges and military schools. QISE presents extraordinary opportunities to work towards rectifying issues of inclusivity and equity that continue to be pervasive within engineering. We present a plan to do so and describe how quantum engineering education presents an excellent set of education research opportunities. Finally, we outline a hands-on training plan on quantum hardware, a key component of any quantum engineering program, with a variety of technologies including optics, atoms and ions, cryogenic and solid-state technologies, nanofabrication, and control and readout electronics. Our recommendations provide a flexible framework that can be tailored for academic institutions ranging from teaching and undergraduate-focused two- and four-year colleges to research-intensive universities., Comment: 25 pages, 2 figures

Quantum information science and engineering requires novel low-loss magnetic materials for magnon-based quantum-coherent operations. The search for low-loss magnetic materials, traditionally driven by applications in microwave electronics near room-temperature, has gained additional constraints from the need to operate at cryogenic temperatures for many applications in quantum information science and technology. Whereas yttrium iron garnet (YIG) has been the material of choice for decades, the emergence of molecule-based materials with robust magnetism and ultra-low damping has opened new avenues for exploration. Specifically, thin-films of vanadium tetracyanoethylene (V[TCNE]x) can be patterned into the multiple, connected structures needed for hybrid quantum elements and have shown room-temperature Gilbert damping ({\alpha} = 4 \times 10^-5) that rivals the intrinsic (bulk) damping otherwise seen only in highly-polished YIG spheres (far more challenging to integrate into arrays). Here, we present a comprehensive and systematic study of the low-temperature magnetization dynamics for V[TCNE]x thin films, with implications for their application in quantum systems. These studies reveal a temperature-driven, strain-dependent magnetic anisotropy that compensates the thin-film shape anisotropy, and the recovery of a magnetic resonance linewidth at 5 K that is comparable to room-temperature values (roughly 2 G at 9.4 GHz). We can account for these variations of the V[TCNE]x linewidth within the context of scattering from very dilute paramagnetic impurities, and anticipate additional linewidth narrowing as the temperature is further reduced., Comment: The first two authors contributed equally

We propose an approach to realize a hybrid quantum system composed of a diamond nitrogen-vacancy (NV) center spin coupled to a magnon mode of the low-damping, low-moment organic ferrimagnet vanadium tetracyanoethylene. We derive an analytical expression for the spin-magnon cooperativity as a function of NV position under a micron-scale perpendicularly magnetized disk, and show that, surprisingly, the cooperativity will be higher using this magnetic material than in more conventional materials with larger magnetic moments, due to in part to the reduced demagnetization field. For reasonable experimental parameters, we predict that the spin-magnon-mode coupling strength is $g\sim 10$ kHz. For isotopically pure $^{12}$C diamond we predict strong coupling of an NV spin to the unoccupied magnon mode, with cooperativity $\mathcal C=6$ for a wide range of NV spin locations within the diamond, well within the spatial precision of NV center implantation. Thus our proposal describes a practical pathway for single-spin-state-to-single-magnon-occupancy transduction and for entangling NV centers over micron length scales., Comment: Main text (15 pages + 4 figures) and Supplemental Material

Integrating patterned, low-loss magnetic materials into microwave devices and circuits presents many challenges due to the specific conditions that are required to grow ferrite materials, driving the need for flip-chip and other indirect fabrication techniques. The low-loss ($\alpha = 3.98 \pm 0.22 \times 10^{-5}$), room-temperature ferrimagnetic coordination compound vanadium tetracyanoethylene ($\mathrm{V[TCNE]}_x$) is a promising new material for these applications that is potentially compatible with semiconductor processing. Here we present the deposition, patterning, and characterization of $\mathrm{V[TCNE]}_x$ thin films with lateral dimensions ranging from 1 micron to several millimeters. We employ electron-beam lithography and liftoff using an aluminum encapsulated poly(methyl methacrylate), poly(methyl methacrylate-methacrylic acid) copolymer bilayer (PMMA/P(MMA-MAA)) on sapphire and silicon. This process can be trivially extended to other common semiconductor substrates. Films patterned via this method maintain low-loss characteristics down to 25 microns with only a factor of 2 increase down to 5 microns. A rich structure of thickness and radially confined spin-wave modes reveals the quality of the patterned films. Further fitting, simulation, and analytic analysis provides an exchange stiffness, $A_{ex} = 2.2 \pm 0.5 \times 10^{-10}$ erg/cm, as well as insights into the mode character and surface spin pinning. Below a micron, the deposition is non-conformal, which leads to interesting and potentially useful changes in morphology. This work establishes the versatility of $\mathrm{V[TCNE]}_x$ for applications requiring highly coherent magnetic excitations ranging from microwave communication to quantum information., Comment: 18 pages, 7 figures, submitted to APL Materials

Vanadium tetracyanoethylene (V[TCNE]$_\text{x}$) is an organic-based ferrimagnet that exhibits robust magnetic ordering (T$_\text{C}$ of over 600 K), high quality-factor (high-Q) microwave resonance (Q up to 3,500), and compatibility with a wide variety of substrates and encapsulation technologies. Here, we substantially expand the potential scope and impact of this emerging material by demonstrating the ability to produce engineered nanostructures with tailored magnetic anisotropy that serve as a platform for the exploration of cavity magnonics, revealing strongly coupled quantum confined standing wave modes that can be tuned into and out of resonance with an applied magnetic field. Specifically, time-domain micromagnetic simulations of these nanostructures faithfully reproduce the experimentally measured spectra, including the quasi-uniform mode and higher-order spin-wave (magnon) modes. Finally, when the two dominant magnon modes present in the spectra are brought into resonance by varying the orientation of the in-plane magnetic field, we observe anti-crossing behavior indicating strong coherent coupling between these two magnon modes at room temperature. These results position V[TCNE]$_\text{x}$ as a leading candidate for the development of coherent magnonics, with potential applications ranging from microwave electronics to quantum information., Comment: 25 pages, 3 figures

Ultrathin films of Na3Bi on insulating substrates are desired for opening a bulk band gap and generating the quantum spin Hall effect from a topological Dirac semimetal, though continuous films in the few nanometer regime have been difficult to realize. Here, we utilize alternating layer molecular beam epitaxy (MBE) to achieve uniform and continuous single crystal films of Na3Bi(0001) on insulating Al2O3(0001) substrates and demonstrate electrical transport on films with 3.8 nm thickness (4 unit cells). The high material quality is confirmed through in situ reflection high-energy electron diffraction (RHEED), scanning tunneling microscopy (STM), x-ray diffraction (XRD), and x-ray photoelectron spectroscopy (XPS). In addition, these films are employed as seed layers for subsequent growth by codeposition, leading to atomic layer-by-layer growth as indicated by RHEED intensity oscillations. These material advances facilitate the pursuit of quantum phenomena in thin films of Dirac semimetals., Comment: 11 pages, 5 figures

A key limitation of electron paramagnetic resonance (EPR), an established and powerful tool for studying atomic-scale biomolecular structure and dynamics is its poor sensitivity, samples containing in excess of 10^12 labeled biomolecules are required in typical experiments. In contrast, single molecule measurements provide improved insights into heterogeneous behaviors that can be masked by ensemble measurements and are often essential for illuminating the molecular mechanisms behind the function of a biomolecule. We report EPR measurements of a single labeled biomolecule that merge these two powerful techniques. We selectively label an individual double-stranded DNA molecule with a single nanodiamond containing nitrogen-vacancy (NV) centers, and optically detect the paramagnetic resonance of NV spins in the nanodiamond probe. Analysis of the spectrum reveals that the nanodiamond probe has complete rotational freedom and that the characteristic time scale for reorientation of the nanodiamond probe is slow compared to the transverse spin relaxation time. This demonstration of EPR spectroscopy of a single nanodiamond labeled DNA provides the foundation for the development of single molecule magnetic resonance studies of complex biomolecular systems., Comment: 24 pages, 5 figures

Understanding the complex properties of electronic and spintronic devices at the micro- and nano-scale is a topic of intense current interest as it becomes increasingly important for scientific progress and technological applications. In-operando characterization of such devices by scanned probe techniques is particularly well-suited for the microscopic study of these properties. We have developed a scanned probe microscope (SPM) which is capable of both standard force imaging (atomic, magnetic, electrostatic) and simultaneous electrical transport measurements. We utilize flexible and inexpensive FPGA (field programmable gate array) hardware and a custom software framework developed in National Instrument's LabVIEW environment to perform the various aspects of microscope operation and device measurement. The FPGA-based approach enables sensitive, real-time cantilever frequency-shift detection. Using this system, we demonstrate electrostatic force microscopy of an electrically-biased graphene FET device. The combination of SPM and electrical transport also enables imaging of the transport response to a localized perturbation provided by the scanned cantilever tip. Facilitated by the broad presence of LabVIEW in the experimental sciences and the openness of our software solution, our system permits a wide variety of combined scanning and transport measurements by providing standardized interfaces and flexible access to all aspects of a measurement (input and output signals, and processed data). Our system also enables precise control of timing (synchronization of scanning and transport operations) and implementation of sophisticated feedback protocols, and thus should be broadly interesting and useful to practitioners in the field.

The demonstration of strong photoluminescence polarization anisotropy in semiconducting nanowires embodies both technological promise and scientific challenge. Here we present progress on both fronts through the study of the photoluminescence polarization anisotropy of randomly oriented nanowire ensembles in materials without/with crystalline anisotropy, small/wide bandgap, and both III-V/II-VI chemistry (InP/ZnO nanowires, respectively). Comprehensive control of the polarization anisotropy is realized by dielectric matching with conformally deposited Ta2O5 (dielectric ratios of 9.6:4.41 and 4.0:4.41 for InP and ZnO, respectively). After dielectric matching, the polarization anisotropy of the nanowire ensembles is reduced by 86% for InP:Ta2O5 and 84% for ZnO:Ta2O5.