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Dense spin ensembles in solids present a natural platform for studying quantum many-body dynamics. Multiple-pulse coherent control can be used to manipulate the magnetic dipolar interaction between the spins to engineer their dynamics. Here, we investigate the performance of a series of well-known pulse sequences that aim to suppress interspin dipolar couplings. We use a combination of numerical simulations and solid-state nuclear magnetic resonance experiments on adamantane to evaluate and compare sequence performance. We study the role of sequence parameters like interpulse delays and resonance offsets. Disagreements between experiments and theory are typically explained by the presence of control errors and experimental nonidealities. The simulations allow us to explore the influence of factors such as finite pulse widths, rotation errors, and phase transient errors. We also investigate the role of local disorder and establish that it is, perhaps unsurprisingly, a distinguishing factor in the decoupling efficiency of spectroscopic sequences (that preserve Hamiltonian terms proportional to $S_z$) and time-suspension sequences (which refocus all terms in the internal Hamiltonian). We discuss our findings in the context of previously known analytical results from average Hamiltonian theory. Finally, we explore the ability of time-suspension sequences to protect multispin correlations in the system. Published by the American Physical Society2025 

Abstract The coherence times of solid-state spin qubits are often limited by the presence of a spin bath. Characterizing the spectrum of the local magnetic field fluctuations of the bath is key to understanding spin qubit decoherence. Here we use pulsed electron paramagnetic resonance (pEPR) based noise spectroscopy to measure the magnetic noise power spectra for ensembles of P1 (substitutional nitrogen) centers in diamond that typically form the bath for NV (nitrogen-vacancy) centers. The Carr-Purcell-Meiboom-Gill (CPMG) dynamical decoupling experiments on the P1 centers were performed on a low [N] CVD (chemical vapor deposition) sample and a high [N] HPHT (high-temperature, high-pressure) sample at 89 mT. We characterize the NV centers of the latter sample using the same 2.5 GHz pEPR spectrometer. All power spectra show two distinct features, a broad component that is observed to scale as approximately 1/ω^{0.7-1.0}, and a prominent peak at the 13C Larmor frequency. The behavior of the broad component is consistent with an inhomogeneous distribution of Lorentzian spectra due to clustering of P1 centers, which has recently been shown to be prevalent in HPHT diamond. We develop techniques utilizing harmonics of the CPMG filter function to improve characterization of high-frequency signals, which we demonstrate on the 13C nuclear Larmor frequency. At 190 mT this is 2.04 MHz, 5.7 times higher than the CPMG modulation frequency (<357 kHz, hardware-limited). Understanding the properties of the bath allow us to either exploit it as a quantum resource or optimize decoupling performance, while also informing sample fabrication technologies. The techniques are applicable to ac magnetometry for nanoscale nuclear magnetic resonance and chemical sensing. 

Understanding the spatial distribution of the P1 centers is crucial for diamond-based sensors and quantum devices. P1 centers serve as polarization sources for dynamic nuclear polarization (DNP) quantum sensing and play a significant role in the relaxation of nitrogen vacancy (NV) centers. Additionally, the distribution of NV centers correlates with the distribution of P1 centers, as NV centers are formed through the conversion of P1 centers. We utilized DNP and pulsed electron paramagnetic resonance (EPR) techniques that revealed strong clustering of a significant population of P1 centers that exhibit exchange coupling and produce asymmetric line shapes. The 13C DNP frequency profile at a high magnetic field revealed a pattern that requires an asymmetric EPR line shape of the P1 clusters with electron–electron (e–e) coupling strengths exceeding the 13C nuclear Larmor frequency. EPR and DNP characterization at high magnetic fields was necessary to resolve energy contributions from different e–e couplings. We employed a two-frequency pump–probe pulsed electron double resonance technique to show cross-talk between the isolated and clustered P1 centers. This finding implies that the clustered P1 centers affect all of the P1 populations. Direct observation of clustered P1 centers and their asymmetric line shape offers a novel and crucial insight into understanding magnetic noise sources for quantum information applications of diamonds and for designing diamond-based polarizing agents with optimized DNP efficiency for 13C and other nuclear spins of analytes. We propose that room temperature 13C DNP at a high field, achievable through straightforward modifications to existing solution-state NMR systems, is a potent tool for evaluating and controlling diamond defects. 

Nuclear magnetic resonance (NMR) experiments can reveal local properties in materials, but are often limited by the low signal-to-noise ratio. Spin squeezed states have an improved resolution below the Heisenberg limit in one of the spin components, and have been extensively used to improve the sensitivity of atomic clocks, for example [1]. Interacting and entangled spin ensembles with non-linear coupling are a natural candidate for implementing squeezing. Here, we propose measurement of the spin-squeezing parameter that itself can act as a local probe of emergent orders in quantum materials. In particular, we demonstrate how to investigate an anisotropic electric field gradient via its coupling to the nuclear quadrupole moment. While squeezed spin states are pure, the squeezing parameter can be estimated for both pure and mixed states. We evaluate the range of fields and temperatures for which a thermal-equilibrium state is sufficient to improve the resolution in an NMR experiment and probe relevant parameters of the quadrupole Hamiltonian, including its anisotropy. 

Dynamic nuclear polarization (DNP) is a method of enhancing NMR signals via the transfer of polarization from electron spins to nuclear spins using microwave (MW) irradiation. In most cases, monochromatic continuous-wave (MCW) MW irradiation is used. Recently, several groups have shown that frequency modulation of the MW irradiation can result in an additional increase in DNP enhancement above that obtained with MCW. The effect of frequency modulation on the solid effect (SE) and the cross effect (CE) has previously been studied using the stable organic radical 4-hydroxy TEMPO (TEMPOL) at temperatures under 20 K. Here, in addition to the SE and CE, we discuss the effect of frequency modulation on the Overhauser effect (OE) and the truncated CE (tCE) in the room-temperature 13C-DNP of diamond powders. We recently showed that diamond powders can exhibit multiple DNP mechanisms simultaneously due to the heterogeneity of P1 (substitutional nitrogen) environments within diamond crystallites. We explore how the two parameters that define the frequency modulation: (i) the Modulation frequency, fm (how fast the microwave frequency is varied) and (ii) the Modulation amplitude, Δω (the magnitude of the change in microwave frequency) influence the enhancement obtained via each mechanism. Frequency modulation during DNP not only allows us to improve DNP enhancement, but also gives us a way to control which DNP mechanism is most active. By choosing the appropriate modulation parameters, we can selectively enhance some mechanisms while simultaneously suppressing others.