arXiv subjects

Andrey Jarmola

Publications and source records attributed to Andrey Jarmola.

At least 19 recordsLinked to original sources

arXiv2026

Optically detected nuclear magnetic resonance of carbon-13 in bulk diamond

Precision measurements based on optically detected nuclear magnetic resonance offer exquisite sensitivity to absolute shifts in spin transition frequencies, with potential applications in fundamental physics experiments and inertial sensing. We investigate 13C nuclear spins in diamond as a candidate system for solid-state implementations, which hold the promise for high-fidelity readout of large numbers of coherent nuclear spins in millitesla or lower magnetic fields. We demonstrate a technique that allows for both optical polarization and readout of large ensembles of ~10^{16} polarized nuclear spins. Our method takes advantage of state-selective Landau-Zener transitions under microwave frequency sweeping, which bidirectionally transfer spin polarization between Nitrogen-Vacancy (NV) electron spins and remote 13C nuclear spins. Using natural isotopic abundance diamonds with nitrogen densities of ~0.5-10 ppm, we perform optically-detected 13C Ramsey spectroscopy and realize a nuclear-spin-dependent fluorescence contrast exceeding 0.5% peak-to-peak. We observe nuclear spin dephasing times T2*~2 ms that only modestly improve with homonuclear dipolar decoupling, indicating that they are limited by the longitudinal spin relaxation of nearby NV electron spins. We study the magnetic field dependence of the optical readout and find comparable contrast and dephasing times for magnetic fields in the range 8-20 mT. Our method can be interpreted as a type of repetitive readout, where each NV center optically reads out the spin state of ~100 nuclei before nuclear spins depolarize.

quant-ph↗

arXiv2026

Towards a temperature-insensitive composite diamond clock

Frequency references based on solid state spins promise simplicity, compactness, robustness, multifunctionality, ease of integration, and high densities of emitters. Nitrogen-vacancy (NV) centers in diamond are a natural candidate, but the electronic zero-field splitting exhibits a large fractional temperature dependence, which has precluded its use as a stable clock transition. Here we show that this limitation can be overcome by forming a composite frequency reference that combines measurements of the electronic splitting D with the nuclear quadrupole splitting of the $^{14}$N nuclear spin intrinsic to the NV center. We further benchmark this composite approach against alternative strategies for mitigating temperature sensitivity. By implementing a specially designed pulse sequence with an eight-phase control scheme that suppresses pulse imperfections, we interleave measurements of D and Q in a high-density NV ensemble and demonstrate a temperature-compensated composite frequency reference. The stability of this composite diamond clock is characterized over a 10-day period at room temperature through a comparison to a Rb vapor-cell clock, yielding a fractional instability below $5 \times 10^{-9}$ for an averaging time of $τ= 200$ s and below $1 \times 10^{-8}$ at $τ= 2 \times 10^5$ s, corresponding to measured improvements by a factor of 4 and 200, respectively, over a clock based purely on the single frequency D for the same periods. By characterizing the residual sensitivity to magnetic fields, optical power, and radio-frequency drive amplitudes, we find that temperature is no longer the dominant source of instability. These results establish complementary electron- and nuclear-spin transitions in diamond as a viable route to thermally robust frequency metrology, providing a pathway toward compact, multifunctional solid-state clocks and quantum sensors.

quant-ph↗

arXiv2025

Earth's field diamond vector magnetometry with isotropic magnetic flux concentrators

Vector magnetometers based on the optically detected magnetic resonance (ODMR) of nitrogen-vacancy centers in diamond are being developed for applications such as navigation and geomagnetism. However, at low magnetic fields, such as that on Earth (~50 μT), diamond magnetometers suffer from spectral congestion whereby ODMR peaks are not easily resolved. Here, we experimentally investigate a potential solution of using an isotropic, three-dimensional magnetic flux concentrator to amplify Earth's field without altering its direction. The concentrator consists of six ferrite cones, in a face-centered cubic arrangement, centered about a diamond. We vary the direction of a 50 μT applied field and record and fit the resulting ODMR spectra. By comparing the fitted fields to those of a reference fluxgate magnetometer, we characterize the angular response of the diamond magnetometer and quantify absolute errors in the field magnitude and angle. We find that the enhancement factor is nearly isotropic, with a mean of 19.05 and a standard deviation of 0.16, when weighted by solid angle coverage. Gradient broadening of the ODMR lines is sufficiently small that the spectra are well resolved for nearly all field directions, alleviating spectral congestion. For ~98% of the total 4π solid angle, Cramér-Rao lower bounds for magnetic field estimation uncertainty are within a factor of 2 of those of the fully-resolved case, indicating minimal deadzones. We track the stability of the magnetometer over six hours and observe variations less than or approximately 40 nT/hour, limited by temperature drift. Our study presents a new route for diamond vector magnetometry at Earth's field, with potential applications in geomagnetic surveys, anomaly detection, and navigation.

physics.ins-det↗

arXiv2025

Chemically resolved nuclear magnetic resonance spectroscopy by longitudinal magnetization detection with a diamond magnetometer

Non-inductive magnetometers based on solid-state spins offer a promising solution for small-volume nuclear magnetic resonance (NMR) detection. A remaining challenge is to operate at a sufficiently high magnetic field to resolve chemical shifts at the part-per-billion level. Here, we demonstrate a Ramsey-M_z protocol that uses Ramsey interferometry to convert an analyte's transverse spin precession into a longitudinal magnetization (M_z), which is subsequently modulated and detected with a diamond magnetometer. We record NMR spectra at B0=0.32 T with a fractional spectral resolution of ~350 ppb, limited by the stability of the electromagnet bias field. We perform NMR spectroscopy on a ~1 nL detection volume of ethanol and resolve the chemical shift structure with negligible distortion. Through simulation, we show that the protocol can be extended to fields up to B0=3 T, with minimal spectral distortion, using composite nuclear-spin inversion pulses. For sub-nanoliter analyte volumes, we estimate a resolution of ~1 ppb and concentration sensitivity of ~40 mM s^{1/2} is feasible with improvements to the sensor design. Our results establish diamond magnetometers as high-resolution NMR detectors in the moderate magnetic field regime, with potential applications in metabolomics and pharmaceutical research.

physics.ins-det↗

arXiv2024

The impact of microwave phase noise on diamond quantum sensing

Precision optical measurements of the electron-spin precession of nitrogen-vacancy (NV) centers in diamond form the basis of numerous applications. The most sensitivity-demanding applications, such as femtotesla magnetometry, require the ability to measure changes in GHz spin transition frequencies at the sub-millihertz level, corresponding to a fractional resolution of better than 10^{-12}. Here we study the impact of microwave (MW) phase noise on the response of an NV sensor. Fluctuations of the phase of the MW waveform cause undesired rotations of the NV spin state. These fluctuations are imprinted in the optical readout signal and, left unmitigated, are indistinguishable from magnetic field noise. We show that the phase noise of several common commercial MW generators results in an effective pT s^{1/2}-range noise floor that varies with the MW carrier frequency and the detection frequency of the pulse sequence. The data are described by a frequency domain model incorporating the MW phase noise spectrum and the filter-function response of the sensing protocol. For controlled injection of white and random-walk phase noise, the observed NV magnetic noise floor is described by simple analytic expressions that accurately capture the scaling with pulse sequence length and the number of pi pulses. We outline several strategies to suppress the impact of MW phase noise and implement a version, based on gradiometry, that realizes a >10-fold suppression. Our study highlights an important challenge in the pursuit of sensitive diamond quantum sensors and is applicable to other qubit systems with a large transition frequency.

quant-ph↗

arXiv2024

Ramsey interferometry of nuclear spins in diamond using stimulated Raman adiabatic passage

We report the first experimental demonstration of stimulated Raman adiabatic passage (STIRAP) in nuclear-spin transitions of $^{14}$N within nitrogen-vacancy (NV) color centers in diamond. It is shown that the STIRAP technique suppresses the occupation of the intermediate state, which is a crucial factor for improvements in quantum sensing technology. Building on that advantage, we develop and implement a generalized version of the Ramsey interferometric scheme, employing half-STIRAP pulses to perform the necessary quantum-state manipulation with high fidelity. The enhanced robustness of the STIRAP-based Ramsey scheme to variations in the pulse parameters is experimentally demonstrated, showing good agreement with theoretical predictions. Our results pave the way for improving the long-term stability of diamond-based sensors, such as gyroscopes and frequency standards.

quant-ph↗

arXiv2023

Nuclear quadrupole resonance spectroscopy with a femtotesla diamond magnetometer

Sensitive Radio-Frequency (RF) magnetometers that can detect oscillating magnetic fields at the femtotesla level are needed for demanding applications such as Nuclear Quadrupole Resonance (NQR) spectroscopy. RF magnetometers based on Nitrogen-Vacancy (NV) centers in diamond have been predicted to offer femtotesla sensitivity, but published experiments have largely been limited to the picotesla level. Here, we demonstrate a femtotesla RF magnetometer based on an NV-doped diamond membrane inserted between two ferrite flux concentrators. The device operates in bias magnetic fields of 2-10 microtesla and provides a ~300-fold amplitude enhancement within the diamond for RF magnetic fields in the 0.07-3.6 MHz range. The magnetometer's sensitivity is ~70 fT s^{1/2} at 0.35 MHz, and the noise floor decreases to below 2 fT after 1 hour of acquisition. We used this sensor to detect the 3.6 MHz NQR signal of 14N in sodium nitrite powder at room temperature. NQR signals are amplified by a resonant RF coil wrapped around the sample, allowing for higher signal-to-noise ratio detection. The diamond RF magnetometer's recovery time after a strong RF pulse is ~35 us, limited by the coil ring-down time. The sodium-nitrite NQR frequency shifts linearly with temperature as -1.00 +/- 0.02 kHz/K, the magnetization dephasing time is T2* = 887 +/- 51 us, and a spin-lock spin-echo pulse sequence extends the signal lifetime to 332 +/- 23 ms, all consistent with coil-based NQR studies. Our results expand the sensitivity frontier of diamond magnetometers to the femtotesla range, with potential applications in security, medical imaging, and materials science.

physics.ins-det↗

arXiv2022

Temperature Sensitivity of $^{14}\mathrm{NV}$ and $^{15}\mathrm{NV}$ Ground State Manifolds

We measure electron and nuclear spin transition frequencies in the ground state of nitrogen-vacancy (NV) centers in diamond for two nitrogen isotopes ($^{14}\mathrm{NV}$ and $^{15}\mathrm{NV}$) over temperatures ranging from 77 K to 400 K. Measurements are performed using Ramsey interferometry and direct optical readout of the nuclear and electron spins. We extract coupling parameters $Q$ (for $^{14}\mathrm{NV}$), $D$, $A_{||}$, $A_{\perp}$, $γ_e/γ_n$, and their temperature dependences for both isotopes. The temperature dependences of the nuclear-spin transitions within the $m_s = 0$ spin manifold near room temperature are found to be +0.52(1) ppm/K for $^{14}\mathrm{NV}$ ($|m_I=-1> \leftrightarrow |m_I=+1>$) and -1.1(1) ppm/K for $^{15}\mathrm{NV}$ ($|m_I=-1/2> \leftrightarrow |m_I=+1/2>$). An isotopic shift in the zero-field splitting parameter $D$ between $^{14}\mathrm{NV}$ and $^{15}\mathrm{NV}$ is measured to be $\sim$ 120 kHz. Residual transverse magnetic fields are observed to shift the nuclear spin transition frequencies, especially for $^{15}\mathrm{NV}$. We have precisely determined the set of parameters relevant for the development of nuclear-spin-based diamond quantum sensors with greatly reduced sensitivity to environmental factors.

quant-ph↗

arXiv2021

Demonstration of diamond nuclear spin gyroscope

We demonstrate operation of a rotation sensor based on the $^{14}$N nuclear spins intrinsic to nitrogen-vacancy (NV) color centers in diamond. The sensor employs optical polarization and readout of the nuclei and a radio-frequency double-quantum pulse protocol that monitors $^{14}$N nuclear spin precession. This measurement protocol suppresses the sensitivity to temperature variations in the $^{14}$N quadrupole splitting, and it does not require microwave pulses resonant with the NV electron spin transitions. The device was tested on a rotation platform and demonstrated a sensitivity of 4.7 $^{\circ}/\sqrt{\rm{s}}$ (13 mHz/$\sqrt{\rm{Hz}}$), with bias stability of 0.4 $^{\circ}$/s (1.1 mHz).

quant-ph↗

arXiv2021

Emergent hydrodynamics in a strongly interacting dipolar spin ensemble

Conventional wisdom holds that macroscopic classical phenomena naturally emerge from microscopic quantum laws. However, despite this mantra, building direct connections between these two descriptions has remained an enduring scientific challenge. In particular, it is difficult to quantitatively predict the emergent "classical" properties of a system (e.g. diffusivity, viscosity, compressibility) from a generic microscopic quantum Hamiltonian. Here, we introduce a hybrid solid-state spin platform, where the underlying disordered, dipolar quantum Hamiltonian gives rise to the emergence of unconventional spin diffusion at nanometer length scales. In particular, the combination of positional disorder and on-site random fields leads to diffusive dynamics that are Fickian yet non-Gaussian. Finally, by tuning the underlying parameters within the spin Hamiltonian via a combination of static and driven fields, we demonstrate direct control over the emergent spin diffusion coefficient. Our work opens the door to investigating hydrodynamics in many-body quantum spin systems.

quant-ph↗

arXiv2021

Determination of local defect density in diamond by double electron-electron resonance

Magnetic impurities in diamond influence the relaxation properties and thus limit the sensitivity of magnetic, electric, strain, and temperature sensors based on nitrogen-vacancy color centers. Diamond samples may exhibit significant spatial variations in the impurity concentrations hindering the quantitative analysis of relaxation pathways. Here, we present a local measurement technique which can be used to determine the concentration of various species of defects by utilizing double electron-electron resonance. This method will help to improve the understanding of the physics underlying spin relaxation and guide the development of diamond samples, as well as offering protocols for optimized sensing.

cond-mat.mes-hall↗

arXiv2019

Diamond magnetometer enhanced by ferrite flux concentrators

Magnetometers based on nitrogen-vacancy (NV) centers in diamond are promising room-temperature, solid-state sensors. However, their reported sensitivity to magnetic fields at low frequencies (<1 kHz) is presently >10 pT s^{1/2}, precluding potential applications in medical imaging, geoscience, and navigation. Here we show that high-permeability magnetic flux concentrators, which collect magnetic flux from a larger area and concentrate it into the diamond sensor, can be used to improve the sensitivity of diamond magnetometers. By inserting an NV-doped diamond membrane between two ferrite cones in a bowtie configuration, we realize a ~250-fold increase of the magnetic field amplitude within the diamond. We demonstrate a sensitivity of ~0.9 pT s^{1/2} to magnetic fields in the frequency range between 10 and 1000 Hz, using a dual-resonance modulation technique to suppress the effect of thermal shifts of the NV spin levels. This is accomplished using 200 mW of laser power and 20 mW of microwave power. This work introduces a new dimension for diamond quantum sensors by using micro-structured magnetic materials to manipulate magnetic fields.

physics.ins-det↗

arXiv2019

Two-dimensional nuclear magnetic resonance spectroscopy with a microfluidic diamond quantum sensor

Quantum sensors based on nitrogen-vacancy centers in diamond have emerged as a promising detection modality for nuclear magnetic resonance (NMR) spectroscopy owing to their micron-scale detection volume and non-inductive based detection. A remaining challenge is to realize sufficiently high spectral resolution and concentration sensitivity for multidimensional NMR analysis of picoliter sample volumes. Here, we address this challenge by spatially separating the polarization and detection phases of the experiment in a microfluidic platform. We realize a spectral resolution of 0.65 +/- 0.05 Hz, an order-of-magnitude improvement over previous diamond NMR studies. We use the platform to perform two-dimensional correlation spectroscopy of liquid analytes within an effective ~20 picoliter detection volume. The use of diamond quantum sensors as in-line microfluidic NMR detectors is a significant step towards applications in mass-limited chemical analysis and single cell biology.

physics.ins-det↗

arXiv2018

Diamond magnetic microscopy of malarial hemozoin nanocrystals

Magnetic microscopy of malarial hemozoin nanocrystals was performed using optically detected magnetic resonance imaging of near-surface diamond nitrogen-vacancy centers. Hemozoin crystals were extracted from $Plasmodium$-$falciparum$-infected human blood cells and studied alongside synthetic hemozoin crystals. The stray magnetic fields produced by individual crystals were imaged at room temperature as a function of applied field up to 350 mT. More than 100 nanocrystals were analyzed, revealing the distribution of their magnetic properties. Most crystals ($96\%$) exhibit a linear dependence of stray field magnitude on applied field, confirming hemozoin's paramagnetic nature. A volume magnetic susceptibility $χ=3.4\times10^{-4}$ is inferred using a magnetostatic model informed by correlated scanning electron microscopy measurements of crystal dimensions. A small fraction of nanoparticles (4/82 for $Plasmodium$-produced and 1/41 for synthetic) exhibit a saturation behavior consistent with superparamagnetism. Translation of this platform to the study of living malaria-infected cells may shed new light on hemozoin formation dynamics and their interaction with antimalarial drugs.

cond-mat.mes-hall↗

arXiv2018

Imaging the local charge environment of nitrogen-vacancy centers in diamond

Characterizing the local internal environment surrounding solid-state spin defects is crucial to harnessing them as nanoscale sensors of external fields. This is especially germane to the case of defect ensembles which can exhibit a complex interplay between interactions, internal fields and lattice strain. Working with the nitrogen-vacancy (NV) center in diamond, we demonstrate that local electric fields dominate the magnetic resonance behavior of NV ensembles at low magnetic field. We introduce a simple microscopic model that quantitatively captures the observed spectra for samples with NV concentrations spanning over two orders of magnitude. Motivated by this understanding, we propose and implement a novel method for the nanoscale localization of individual charges within the diamond lattice; our approach relies upon the fact that the charge induces an NV dark state which depends on the electric field orientation.

quant-ph↗

arXiv2016

Microwave-free magnetometry with nitrogen-vacancy centers in diamond

We use magnetic-field-dependent features in the photoluminescence of negatively charged nitrogen-vacancy centers to measure magnetic fields without the use of microwaves. In particular, we present a magnetometer based on the level anti-crossing in the triplet ground state at 102.4 mT with a demonstrated noise floor of 6 nT/$\sqrt{\text{Hz}}$, limited by the intensity noise of the laser and the performance of the background-field power supply. The technique presented here can be useful in applications where the sensor is placed closed to conductive materials, e.g. magnetic induction tomography or magnetic field mapping, and in remote-sensing applications since principally no electrical access is needed.

cond-mat.mes-hall↗

arXiv2015

Optimizing a Dynamical Decoupling Protocol for Solid-State Electronic Spin Ensembles in Diamond

We demonstrate significant improvements of the spin coherence time of a dense ensemble of nitrogen-vacancy (NV) centers in diamond through optimized dynamical decoupling (DD). Cooling the sample down to $77$ K suppresses longitudinal spin relaxation $T_1$ effects and DD microwave pulses are used to increase the transverse coherence time $T_2$ from $\sim 0.7$ ms up to $\sim 30$ ms. We extend previous work of single-axis (CPMG) DD towards the preservation of arbitrary spin states. Following a theoretical and experimental characterization of pulse and detuning errors, we compare the performance of various DD protocols. We identify that the optimal control scheme for preserving an arbitrary spin state is a recursive protocol, the concatenated version of the XY8 pulse sequence. The improved spin coherence might have an immediate impact on improvements of the sensitivities of AC magnetometry. Moreover, the protocol can be used on denser diamond samples to increase coherence times up to NV-NV interaction time scales, a major step towards the creation of quantum collective NV spin states.

quant-ph↗

arXiv2013

The temperature shifts of the resonances of the NV- center in diamond

Significant attention has been recently focused on the realization of high precision nano-thermometry using the spin-resonance temperature shift of the negatively charged nitrogen-vacancy (NV-) center in diamond. However, the precise physical origins of the temperature shift is yet to be understood. Here, the shifts of the center's optical and spin resonances are observed and a model is developed that identifies the origin of each shift to be a combination of thermal expansion and electron-phonon interactions. Our results provide new insight into the center's vibronic properties and reveal implications for NV- thermometry.

cond-mat.mtrl-sci↗