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Creating materials that do not exist in nature can lead to breakthroughs in science and technology. Magnetic skyrmions are topological excitations that have attracted great attention recently for their potential applications in low power, ultrahigh density memory. A major challenge has been to find materials that meet the dual requirement of small skyrmions stable at room temperature. Here we meet both these goals by developing epitaxial FeGe films with excess Fe using atomic layer molecular beam epitaxy (MBE) far from thermal equilibrium. Our novel atomic layer design permits the incorporation of 20% excess Fe while maintaining a non-centrosymmetric crystal structure supported by theoretical calculations and necessary for stabilizing skyrmions. We show that the Curie temperature is well above room temperature, and that the skyrmions probed by topological Hall effect have sizes down to 15 nm as imaged by Lorentz transmission electron microscopy (LTEM) and magnetic force microscopy (MFM). Our results illustrate new avenues for creating artificial materials tailored at the atomic scale that can impact nanotechnology., Comment: 22 figures, 34 pages

The NV center in diamond has proven to be a powerful tool for locally characterizing the magnetic response of microwave excited ferromagnets. To date, this has been limited by the requirement that the FMR excitation frequency be less than the NV spin resonance frequency. Here we report NV relaxometry based on a two-magnon Raman-like process, enabling detection of FMR at frequencies higher than the NV frequency. For high microwave drive powers, we observe an unexpected field-shift of the NV response relative to a simultaneous microwave absorption signal from a low damping ferrite film. We show that the field-shifted NV response is due to a second order Suhl instability. The instability creates a large population of non-equilibrium magnons which relax the NV spin, even when the uniform mode FMR frequency exceeds that of the NV spin resonance frequency, hence ruling out the possibility that the NV is relaxed by a single NV-resonant magnon. We argue that at high frequencies the NV response is due to a two-magnon relaxation process in which the difference frequency of two magnons matches the NV frequency, and at low frequencies we evaluate the lineshape of the one-magnon NV relaxometry response using spinwave instability theory.

Magnetic sensing technology has found widespread application in a diverse set of industries including transportation, medicine, and resource exploration. These uses often require highly sensitive instruments to measure the extremely small magnetic fields involved, relying on difficult-to-integrate superconducting quantum interference devices and spin-exchange relaxation-free magnetometers. A potential alternative, nitrogen-vacancy (NV) centers in diamond, has shown great potential as a high-sensitivity and high-resolution magnetic sensor capable of operating in an unshielded, room-temperature environment. Transitioning NV center-based sensors into practical devices, however, is impeded by the need for high-power radio frequency (RF) excitation to manipulate them. We report an advance that combines two different physical phenomena to enable a highly efficient excitation of the NV centers: magnetoelastic drive of ferromagnetic resonance and NV-magnon coupling. Our work demonstrates a new pathway that combine acoustics and magnonics that enables highly energy-efficient and local excitation of NV centers without the need for any external RF excitation and, thus, could lead to completely integrated, on-chip, atomic sensors.

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

We demonstrate optical detection of a broad spectrum of ferromagnetic excitations using nitrogen-vacancy (NV) centers in an ensemble of nanodiamonds. Our recently developed approach exploits a straightforward CW detection scheme using readily available diamond detectors, making it easily implementable. The NV center is a local detector, giving the technique spatial resolution, which here is defined by our laser spot, but in principle can be extended far into the nanoscale. Among the excitations we observe are propagating dipolar and dipolar-exchange spinwaves, as well as dynamics associated with the multi-domain state of the ferromagnet at low fields. These results offer an approach, distinct from commonly used ODMR techniques, for spatially resolved spectroscopic study of magnetization dynamics at the nanoscale., Comment: 6 pages and 1 page supplmentary information