Optically pumped room temperature masers are a promising platform for driven dissipative spin photon physics beyond steady state emission. Here we observe a sequence of dynamical thresholds in a room temperature nitrogen vacancy diamond maser as the optical pump is increased above the conventional masing threshold. The first threshold yields narrow-line continuous wave emission, while a second threshold produces a periodic train of microwave pulses whose repetition rate generates a frequency comb spectrum. At higher pump power, a third threshold gives rise to pulses with an oscillatory, frequency chirped decay. Time-resolved measurements link the comb directly to self-pulsing dynamics and Fourier analysis of individual bursts reveals a broad distribution of frequencies consistent with collective spin-resonator dynamics in an inhomogeneously broadened ensemble. These results establish the diamond maser as a room temperature platform for nonlinear nonequilibrium light matter dynamics and microwave comb generation.

We present a quantum theory of diamond masers operating at any temperature using a cavity quantum electrodynamical framework. Special attention is paid to the recently demonstrated room-temperature solid-state masers based on nitrogen-vacancy (NV) defect centers in diamond, but the model can easily be modified for other photoexcited chromophores such as pentacene-doped paraterphenyl, vacancies in silicon-carbide or boron nitride. We show that the eight energy levels involved in the optically pumped NV center polarization process can be mapped to a simple pumped two-level-system. We then derive simple analytical expressions for the optical pump threshold condition for masing as well as the steady-state microwave output power which can be used to design and predict maser performance. Finally, we investigate second-order correlations and find that typical diamond masers operate in an intermediate regime between the good and bad cavity limits where photon emission is driven by both stimulated and superradiant processes.

Tuning magnetic properties in layered van der Waals (vdW) materials has captured significant attention due to the efficient control of ground states by heterostructuring and external stimuli. Electron doping by electrostatic gating, interfacial charge transfer, and intercalation is particularly effective in manipulating the exchange and spin-orbit properties, resulting in a control of Curie temperature (TC) and magnetic anisotropy. Here, an uncharted role of intercalation is discovered to generate magnetic frustration. As a model study, Na atoms are intercalated into the vdW gaps of pristine Cr2Ge2Te6 (CGT) where generated magnetic frustration leads to emerging spin-glass states coexisting with a ferromagnetic order. A series of dynamic magnetic susceptibility measurements/analysis confirms the formation of magnetic clusters representing slow dynamics with a distribution of relaxation times. The intercalation also modifies other macroscopic physical parameters including the significant enhancement of TC from 66 to 240 K and the switching of magnetic easy-hard axis direction. This study identifies intercalation as a unique route to generate emerging frustrated spin states in simple vdW crystals.

Microwave (MW) resonators in Electron Paramagnetic Resonance (EPR) spectroscopy concentrate the MW magnetic field (B1) at the sample and separate the MW electric field from the sample. There are numerous experimental methods in EPR spectroscopy which all impose different requirements on MW resonators (e.g. high or low quality factor, MW conversion, and B1-field homogeneity). Although commercial spectrometers offer standardized MW resonators for a broad application range, newly emerging and highly-specialized research fields push these spectrometers to or beyond their sensitivity limits. Optimizing the MW resonator offers one direct approach to improve the sensitivity. Here we present three low-cost optimization approaches for a commercially available X-band (9-10 GHz) MW resonator for three experimental purposes (continuous-wave (CW), transient and pulse EPR). We obtain enhanced MW conversion factors for all three optimized resonators and higher quality factors for two optimized resonators. The latter is important for CW and transient EPR. Furthermore, we fabricated a resonator which features an extended area of homogeneous B1-field and, hence, improved pulse EPR performance. Our results demonstrate that small changes to a commercial MW resonator can enhance its performance in general or for specific applications.

We experimentally and theoretically demonstrate that nonlinear spin-wave interactions suppress the hybrid magnon-photon quasiparticle or "magnon polariton" in microwave spectra of a yttrium iron garnet film detected by an on-chip split-ring resonator. We observe a strong coupling between the Kittel and microwave cavity modes in terms of an avoided crossing as a function of magnetic fields at low microwave input powers, but a complete closing of the gap at high powers. The experimental results are well explained by a theoretical model including the three-magnon decay of the Kittel magnon into spin waves. The gap closure originates from the saturation of the ferromagnetic resonance above the Suhl instability threshold by a coherent backreaction from the spin waves.

Layered van der Waals (vdW) magnets can maintain a magnetic order even down to the single-layer regime and hold promise for integrated spintronic devices. While the magnetic ground state of vdW magnets was extensively studied, key parameters of spin dynamics, like the Gilbert damping, crucial for designing ultra-fast spintronic devices, remains largely unexplored. Despite recent studies by optical excitation and detection, achieving spin wave control with microwaves is highly desirable, as modern integrated information technologies predominantly are operated with these. The intrinsically small numbers of spins, however, poses a major challenge to this. Here, we present a hybrid approach to detect spin dynamics mediated by photon-magnon coupling between high-Q superconducting resonators and ultra-thin flakes of Cr2Ge2Te6 (CGT) as thin as 11 nm. We test and benchmark our technique with 23 individual CGT flakes and extract an upper limit for the Gilbert damping parameter. These results are crucial in designing on-chip integrated circuits using vdW magnets and offer prospects for probing spin dynamics of monolayer vdW magnets.

The discovery of atomic monolayer magnetic materials has stimulated intense research activities in the two-dimensional (2D) van der Waals (vdW) materials community. The field is growing rapidly and there has been a large class of 2D vdW magnetic compounds with unique properties, which provides an ideal platform to study magnetism in the atomically thin limit. In parallel, based on tunneling magnetoresistance and magneto-optical effect in 2D vdW magnets and their heterostructures, emerging concepts of spintronic and optoelectronic applications such as spin tunnel field-effect transistors and spin-filtering devices are explored. While the magnetic ground state has been extensively investigated, reliable characterization and control of spin dynamics play a crucial role in designing ultrafast spintronic devices. Ferromagnetic resonance (FMR) allows direct measurements of magnetic excitations, which provides insight into the key parameters of magnetic properties such as exchange interaction, magnetic anisotropy, gyromagnetic ratio, spin–orbit coupling, damping rate, and domain structure. In this review article, we present an overview of the essential progress in probing spin dynamics of 2D vdW magnets using FMR techniques. Given the dynamic nature of this field, we focus mainly on broadband FMR, optical FMR, and spin-torque FMR, and their applications in studying prototypical 2D vdW magnets. We conclude with the recent advances in laboratory- and synchrotron-based FMR techniques and their opportunities to broaden the horizon of research pathways into atomically thin magnets.

Microwave (MW) resonators in Electron Paramagnetic Resonance (EPR) spectroscopy concentrate the MW magnetic field (B1) at the sample and separate the MW electric field component from the sample to prevent overheating. There are numerous experimental methods in EPR spectroscopy which all impose different requirements on MW resonators (e.g. high quality factor, high MW conversion factor, B1 field homogeneity). Commercial spectrometers offer already standardized MW resonators for a broad application range. Newly emerging highly specialized research fields push these spectrometers to or beyond their sensitivity limits. Optimizing the MW resonator offers a direct approach to increase the sensitivity. Here we present three low-cost optimization approaches for a commercially available X-band MW resonator for three experimental purposes (CW, transient EPR and pulse EPR). We obtain higher quality factors for two optimized resonators and enhanced the MW conversion factors for all three optimized resonators for CW and transient EPR. Furthermore, we fabricated a resonator which features an extended area of homogeneous B1 magnetic field and hence, improved pulse EPR performance. Our results demonstrate that small changes to a commercial MW resonator can enhance its performance in general or for specific applications.

Whereas the laser is nowadays an ubiquitous technology, applications for its microwave analog, the maser, remain highly specialized, despite the excellent low-noise microwave amplification properties. The widespread application of masers is typically limited by the need of cryogenic temperatures. The recent realization of a continuous-wave room-temperature maser, using NV − centers in diamond, is a first step towards establishing the maser as a potential platform for microwave research and development, yet its design is far from optimal. Here, we design and construct an optimized setup able to characterize the operating space of a maser using NV − centers. We focus on the interplay of two key parameters for emission of microwave photons: the quality factor of the microwave resonator and the degree of spin level-inversion. We characterize the performance of the maser as a function of these two parameters, identifying the parameter space of operation and highlighting the requirements for maximal continuous microwave emission.

Oscar Lee, Kei Yamamoto, ∗ Maki Umeda, 3 Christoph W. Zollitsch, Mehrdad Elyasi, Takashi Kikkawa, Eiji Saitoh, 4, 5, 6 Gerrit E. W. Bauer, and Hidekazu Kurebayashi † London Centre for Nanotechnology, University College London, London WC1H 0AH, United Kingdom Advanced Science Research Center, Japan Atomic Energy Agency, 2-4 Shirakata, Tokai 319-1195, Japan Institute for Materials Research, Tohoku University, Sendai 980-8577, Japan WPI Advanced Institude for Materials Research, Tohoku University, 2-1-1, Katahira, Sendai 980-8577, Japan Department of Applied Physics, The University of Tokyo, Tokyo 113-8656, Japan Institute for AI and Beyond, The University of Tokyo, Tokyo 113-8656, Japan.

As in conventional computing, memories for quantum information benefit from high storage density and, crucially, random access, or the ability to read from or write to an arbitrarily chosen register. However, achieving such random access with quantum memories in a dense, hardware-efficient manner remains a challenge. Here we introduce a protocol using chirped pulses to encode qubits within an ensemble of quantum two-level systems, offering both random access and naturally supporting dynamical decoupling to enhance the memory lifetime. We demonstrate the protocol in the microwave regime using donor spins in silicon coupled to a superconducting cavity, storing up to four weak, coherent microwave pulses in distinct memory modes and retrieving them on demand up to 2 ms later. This approach offers the potential for microwave random access quantum memories with lifetimes exceeding seconds, while the chirped pulse phase encoding could also be applied in the optical regime to enhance quantum repeaters and networks.

Impurity spins in crystal matrices are promising components in quantum technologies, particularly if they can maintain their spin properties when close to surfaces and material interfaces. Here, we investigate an attractive candidate for microwave-domain applications, the spins of group-VI ^{125}Te^{+} donors implanted into natural Si at depths as shallow as 20 nm. We show that surface band bending can be used to ionize such near-surface Te to spin-active Te^{+} state, and that optical illumination can be used further to control the Te donor charge state. We examine spin activation yield, spin linewidth, and relaxation (T_{1}) and coherence times (T_{2}) and show how a zero-field 3.5 GHz "clock transition" extends spin coherence times to over 1 ms, which is about an order of magnitude longer than other near-surface spin systems.

Rare-earth doped crystals have long coherence times and the potential to provide quantum interfaces between microwave and optical photons. Such applications benefit from a high cooperativity between the spin ensemble and a microwave cavity -- this motivates an increase in the rare earth ion concentration which in turn impacts the spin coherence lifetime. We measure spin dynamics of two rare-earth spin species, $^{145}$Nd and Yb doped into Y$_{2}$SiO$_{5}$, coupled to a planar microwave resonator in the high cooperativity regime, in the temperature range 1.2 K to 14 mK. We identify relevant decoherence mechanisms including instantaneous diffusion arising from resonant spins and temperature-dependent spectral diffusion from impurity electron and nuclear spins in the environment. We explore two methods to mitigate the effects of spectral diffusion in the Yb system in the low-temperature limit, first, using magnetic fields of up to 1 T to suppress impurity spin dynamics and, second, using transitions with low effective g-factors to reduce sensitivity to such dynamics. Finally, we demonstrate how the `clock transition' present in the $^{171}$Yb system at zero field can be used to increase coherence times up to $T_{2} = 6(1)$ ms.

Impurity spins in crystal matrices are promising components in quantum technologies, particularly if they can maintain their spin properties when close to surfaces and material interfaces. Here, we investigate an attractive candidate for microwave-domain applications, the spins of group-VI ^{125}Te^{+} donors implanted into natural Si at depths as shallow as 20 nm. We show that surface band bending can be used to ionize such near-surface Te to spin-active Te^{+} state, and that optical illumination can be used further to control the Te donor charge state. We examine spin activation yield, spin linewidth, and relaxation (T_{1}) and coherence times (T_{2}) and show how a zero-field 3.5 GHz "clock transition" extends spin coherence times to over 1 ms, which is about an order of magnitude longer than other near-surface spin systems.

Impurity spins in crystal matrices are promising components in quantum technologies, particularly if they can maintain their spin properties when close to surfaces and material interfaces. Here, we investigate an attractive candidate for microwave-domain applications, the spins of group-VI Impurity spins in crystal matrices are promising components in quantum technologies, particularly if they can maintain their spin properties when close to surfaces and material interfaces. Here, we investigate an attractive candidate for microwave-domain applications, the spins of group-VI $^{125}$Te$^+$ donors implanted into natural Si at depths as shallow as 20~nm. We show that surface band-bending can be used to ionise such near-surface Te to spin-active Te$^+$ state, and that optical illumination can be used further to control the Te donor charge state. We examine spin activation yield, spin linewidth, relaxation ($T_1$) and coherence times (\ttwo) and show how a zero-field 3.5~GHz `clock transition' extends spin coherence times to over 1~ms, which is about an order of magnitude longer than other near-surface spin systems.

James O’Sullivan, ∗ Oscar W. Kennedy, ∗ Kamanasish Debnath, Joseph Alexander, Christoph W. Zollitsch, Mantas Šimėnas, Akel Hashim, 4 Christopher N. Thomas, Stafford Withington, Irfan Siddiqi, 4 Klaus Mølmer, and John J. L. Morton 6 London Centre for Nanotechnology, UCL, 17-19 Gordon Street, London, WC1H 0AH, UK Department of Physics and Astronomy, Aarhus University, DK-8000 Aarhus C, Denmark Quantum Nanoelectronics Laboratory, Department of Physics, UC Berkeley, California 94720, USA Lawrence Berkeley National Laboratory, Berkeley, CA 94720, USA Cavendish Laboratory, University of Cambridge, JJ Thomson Ave, Cambridge CB3 0HE, UK Department of Electrical and Electronic Engineering, UCL, Malet Place, London, WC1E 7JE, UK

Topologically protected nanoscale spin textures, known as magnetic skyrmions, possess particlelike properties and feature emergent magnetism effects. In bulk cubic helimagnets, distinct skyrmion resonant modes are already identified using a technique such as ferromagnetic resonance in spintronics. However, direct light-matter coupling between microwave photons and skyrmion resonance modes still needs to be demonstrated. Utilizing two distinct cavity systems, we observe a direct interaction between the cavity resonant mode and two resonant skyrmion modes, the counterclockwise gyration and breathing modes, in bulk Cu2OSeO3. For both resonant modes, we find the largest coupling strength at 57 K indicated by an enhancement of the cavity linewidth at the degeneracy point. We study the effective coupling strength as a function of temperature within the expected skyrmion phase. We attribute the maximum in effective coupling strength to the presence of a large number of skyrmions, and correspondingly to a completely stable skyrmion lattice. Our experimental findings indicate that the coupling between photons and resonant modes of magnetic skyrmions depends on the relative density of these topological particles instead of the pure spin number in the system.