arXiv subjects

Emanuel Druga

Publications and source records attributed to Emanuel Druga.

At least 19 recordsLinked to original sources

arXiv2026

Prethermal rotating-frame solid echo in a dipolar nuclear-spin network

Floquet prethermalization can endow interacting quantum solids with long-lived, approximately conserved quantities, enabling Hamiltonian engineering and new dynamical probes. Using a hyperpolarized network of dipolar-coupled $^{13}$C nuclear spins in diamond driven by pulsed spin-locking, we access a rotating-frame prethermal plateau with quasi-conserved transverse magnetization and cycle-resolved inductive readout. Within this prethermal manifold we observe a robust \emph{rotating-frame solid echo}: after an apparent decay of the rotating-frame free-induction signal over a delay $\tau$, the magnetization revives at time $2\tau$ following a single $(\alpha)_y$ pulse, with maximum amplitude near $\alpha\simeq\pi/2$. The echo envelope decays as a stretched exponential with characteristic time $T_2'\approx 13\,$ms. Analytical arguments and toy-model simulations attribute the revival to Floquet micromotion that transfers coherences between operator subspaces, so that only a subset of the many-body dephasing dynamics is inverted by the $y$ pulse. These results translate classic echo physics into the prethermal rotating frame and point to continuously interrogated prethermal spin ensembles as a versatile platform for high-throughput spectroscopy, Hamiltonian engineering, and long-duration quantum sensing.

quant-ph↗

arXiv2026

DFT-assisted natural abundance 13C zero-field NMR via optical magnetometry

Zero-field (ZF) nuclear magnetic resonance (NMR) spectroscopy probes scalar J-couplings between nuclei while dispensing with large homogeneous magnetic fields, enabling low-cost and geometrically flexible detection, including through conductive enclosures. Despite these advantages, its broader use for chemical analysis has been limited by sensitivity and by the difficulty of predicting the dense spectral multiplets that arise at zero field. Here we demonstrate natural-abundance (1.1%) 13C ZF spectroscopy on off-the-shelf liquids using a compact commercial 87Rb magnetometer for the first time, without hyperpolarization or special sample preparation. Instrumental advances yield improved sensitivity, <250-mHz linewidths and >week-long stability, enabling isotopomer-resolved fingerprint spectra across a 13-molecule library, including the ability to discern rare (0.0121%) doubly 13C-labelled species. In parallel, we demonstrate vibrationally corrected density-functional theory (DFT) based prediction of ZF NMR spectra for chemically diverse molecules with few-hertz accuracy. Comparing experiment with these calculations renders residual deviations as chemically informative, reporting on hydrogen bonding, hydration and ion pairing at high ionic strength. Together, these results contribute towards DFT-assisted ZF NMR as a general platform for field-constraint-free molecular identification and for extracting transient solution-state structure from responsive J-coupling observables.

physics.chem-ph↗

arXiv2026

Robust Quantum Sensing via Prethermal Spin Orbits

Practical performance of quantum sensors is often curtailed by uncontrolled environmental drift (bias-field instability, temperature fluctuations, mechanical vibration), background fields, and imperfect control pulses. This motivates developing physical mechanisms that intrinsically compensate for such perturbations while retaining high sensitivity to target fields. We introduce an interaction-protected magnetometry scheme where periodic driving steers the collective magnetization onto two long-lived, prethermal Floquet "orbit" axes well-separated on the Bloch sphere. Rapid toggling between these axes encodes target fields as a differential signal, whereas background fields appear as common-mode motion that is strongly rejected, achieving >1000-fold suppression while canceling prethermal transients. This enables accurate reconstruction of rapidly varying audio-band magnetic signals without predictive filtering or spectral tuning. We provide an experimental proof-of-principle using a dense ensemble of coupled nuclear spins, operated here as a broadband (0-1 kHz) magnetometer. The protocol is remarkably tolerant to imperfections, operating robustly across millions of pulses under pulse-angle (~10{\deg}) and pulse frequency (>1 kHz) errors, large bias-field drifts (>50 $\mathrm{\mu}$T), temperature variations over 150 K, and harsh mechanical vibrations. These results establish Floquet prethermalization as a resource for robust quantum sensors that combines broadband magnetic-field sensitivity with intrinsic immunity to diverse environmental and control perturbations, opening a path toward stable quantum metrology beyond controlled laboratory conditions.

quant-ph↗

arXiv2025

Optically Detected Magnetic Resonance Imaging and Sensing Within Functionalized Additively Manufactured Microporous Structures

Quantum sensing with nitrogen-vacancy centers in diamond has emerged as a powerful tool for measuring diverse physical parameters, yet the versatility of these measurement approaches is often limited by the achievable layout and dimensionality of bulk-crystal platforms. Here, we demonstrate a versatile approach to creating designer quantum sensors by surface-functionalizing multiphoton lithography microstructures with NV-containing nanodiamonds. We showcase this capability by fabricating a 150 $\mu$m x 150 $\mu$m x 150 $\mu$m triply periodic minimal surface gyroid structure with millions of attached nanodiamonds. We demonstrate a means to volumetrically image these structures using a refractive index matching confocal imaging technique, and extract ODMR spectra from 1.86 $\mu$m x 1.86 $\mu$m areas of highly concentrated nanodiamonds across a cross section of the gyroid. Furthermore, the high density of sensing elements enables ensemble temperature measurements with sensitivity of 0.548 {\deg}K/$\sqrt{Hz}$ at 5 mW excitation power. This approach to creating quantum-enabled microarchitectures opens new possibilities for multimodal sensing in complex three-dimensional environments.

physics.optics↗

arXiv2024

Cryogenic field-cycling instrument for optical NMR hyperpolarization studies

Optical dynamic nuclear polarization (DNP) offers an attractive approach to enhancing the sensitivity of nuclear magnetic resonance (NMR) spectroscopy. Efficient, optically-generated electron polarization can be leveraged to operate across a broad range of temperatures and magnetic fields, making it particularly appealing for applications requiring high DNP efficiency or spatial resolution. While a large class of systems hold promise for optical DNP, many candidates display both variable electron polarizability and electron and nuclear T1 relaxation times as functions of magnetic field and temperature. This necessitates tools capable of studying DNP under diverse experimental conditions. To address this, we introduce a cryogenic field cycling instrument that facilitates optical DNP studies across a wide range of magnetic fields (10mT to 9.4T) and temperatures (10K to 300K). Continuous cryogen replenishment enables sustained, long-term operation. Additionally, the system supports the ability to manipulate and probe hyperpolarized nuclear spins via pulse sequences involving millions of RF pulses. We describe innovations in the device design and demonstrate its operation on a model system of 13C nuclear spins in diamond polarized through optically pumped nitrogen vacancy (NV) centers. We anticipate the use of the instrument for a broad range of optical DNP systems and studies.

quant-ph↗

arXiv2024

High sensitivity pressure and temperature quantum sensing in organic crystals

The inherent sensitivity of quantum sensors to their physical environment can make them good reporters of parameters such as temperature, pressure, strain, and electric fields. Here, we present a molecular platform for pressure (P) and temperature (T) sensing using para-terphenyl crystals doped with pentacene. We leverage the optically detected magnetic resonance (ODMR) of the photoexcited triplet electron in the pentacene molecule, that serves as a sensitive probe for lattice changes in the host para-terphenyl due to pressure or temperature variations. We observe maximal ODMR frequency variations of df/dP=1.8 MHz/bar and df/dT=247 kHz/K, which are over 1,200 times and three times greater, respectively, than those seen in nitrogen-vacancy centers in diamond. This results in a >85-fold improvement in pressure sensitivity over best previously reported. The larger variation reflects the weaker nature of the para-terphenyl lattice, with first-principles DFT calculations indicating that even picometer-level shifts in the molecular orbitals due to P, T changes are measurable. The platform offers additional advantages including high levels of sensor doping, narrow ODMR linewidths and high contrasts, and ease of deployment, leveraging the ability for large single crystals at low cost. Overall, this work paves the way for low-cost, optically-interrogated pressure and temperature sensors and lays the foundation for even more versatile sensors enabled by synthetic tunability in designer molecular systems.

quant-ph↗

arXiv2024

Anomalously extended Floquet prethermal lifetimes and applications to long-time quantum sensing

Floquet prethermalization is observed in periodically driven quantum many-body systems where the system avoids heating and maintains a stable, non-equilibrium state, for extended periods. Here we introduce a novel quantum control method using off-resonance and short-angle excitation to significantly extend Floquet prethermal lifetimes. This is demonstrated on randomly positioned, dipolar-coupled, 13C nuclear spins in diamond, but the methodology is broadly applicable. We achieve a lifetime $T_2'~800 s at 100 K while tracking the transition to the prethermal state quasi-continuously. This corresponds to a >533,000-fold extension over the bare spin lifetime without prethermalization, and constitutes a new record both in terms of absolute lifetime as well as the total number of Floquet pulses applied (here exceeding 7 million). Using Laplace inversion, we develop a new form of noise spectroscopy that provides insights into the origin of the lifetime extension. Finally, we demonstrate applications of these extended lifetimes in long-time, reinitialization-free quantum sensing of time-varying magnetic fields continuously for ~10 minutes at room temperature. Our work facilitates new opportunities for stabilizing driven quantum systems through Floquet control, and opens novel applications for continuously interrogated, long-time responsive quantum sensors.

quant-ph↗

arXiv2024

Sensing with discrete time crystals

Prethermal discrete time crystals (PDTCs) are a nonequilibrium state of matter characterized by long-range spatiotemporal order, and exhibiting a subharmonic response stabilized by many-body interactions under periodic driving. The inherent robustness of time crystalline order to perturbations in the drive protocol makes DTCs promising for applications in quantum technologies. We exploit the susceptibility of PDTC order to deviations in its order parameter to devise highly frequency-selective quantum sensors for time-varying (AC) magnetic fields in a system of strongly-driven, dipolar-coupled 13C nuclear spins in diamond. Integrating a time-varying AC field into the PDTC allows us to exponentially increase its lifetime, with improvements of up to three orders of magnitude (44,204 cycles), and results in a strong resonant response in the time crystalline order parameter. The linewidth of our sensor is limited by the PDTC lifetime alone, as strong interspin interactions help stabilize DTC order. The sensor operates in the 0.5-50kHz range - a challenging frequency regime for sensors based on atomic vapor or electronic spins - and attains a competitive sensitivity. PDTC sensors are resilient to errors in the drive protocol and sample inhomogeneities, and are agnostic to the macroscopic details of the physical platform: the underlying physical principle applies equally to superconducting qubits, neutral atoms, and trapped ions.

quant-ph↗

arXiv2024

High-sensitivity multichannel zero-to-ultralow field NMR with atomic magnetometer arrays

Despite its versatility and high chemical specificity, conventional NMR spectroscopy is limited in measurement throughput due to the need for high-homogeneity magnetic fields, necessitating sequential sample analysis, and bulky devices. Here, we propose a multichannel NMR device that overcomes these limitations that leverages the zero-to-ultralow field (ZULF) regime, where simultaneous detection of multiple samples is carried out via an array of compact optically pumped magnetometers (OPMs). A magnetic field is used only for pre-polarization, permitting the use of large-bore, high-field, inhomogeneous magnets that can accommodate many samples concurrently. Through systematic advances, we demonstrate high-sensitivity, high resolution ZULF NMR spectroscopy with sensitivity comparable to benchtop NMR systems. The spectroscopy remains robust without the need for field shimming for periods on the order of weeks. We show the detection of ZULF NMR signals from organic molecules without isotopic enrichment, and demonstrate the parallelized detection of three distinct samples simultaneously as a proof-of-concept, with the potential to scale further to over 100 channels at a cost comparable to high-resolution liquid state NMR systems. This work sets the stage for using multichannel "NMR camera" devices for inline reaction monitoring, robotic chemistry, quality control, and high-throughput assays.

physics.ins-det↗

arXiv2024

High-precision chemical quantum sensing in flowing monodisperse microdroplets

We report on a novel flow-based method for high-precision chemical detection that integrates quantum sensing with droplet microfluidics. We deploy nanodiamond particles hosting fluorescent nitrogen vacancy defects as quantum sensors in flowing, monodisperse, picoliter-volume microdroplets containing analyte molecules. ND motion within these microcompartments facilitates close sensor-analyte interaction and mitigates particle heterogeneity. Microdroplet flow rates are rapid (upto 4cm/s) and with minimal drift. Pairing this controlled flow with microwave control of NV electronic spins, we introduce a new noise-suppressed mode of Optically Detected Magnetic Resonance that is sensitive to chemical analytes while resilient against experimental variations, achieving detection of analyte-induced signals at an unprecedented level of a few hundredths of a percent of the ND fluorescence. We demonstrate its application to detecting paramagnetic ions in droplets with simultaneously low limit-of-detection and low analyte volumes, in a manner significantly better than existing technologies. This is combined with exceptional measurement stability over >103s and across hundreds of thousands of droplets, while utilizing minimal sensor volumes and incurring low ND costs (<$0.70 for an hour of operation). Additionally, we demonstrate using these droplets as micro-confinement chambers by co-encapsulating ND quantum sensors with analytes, including single cells. This versatility suggests wide-ranging applications, like single-cell metabolomics and real-time intracellular measurements in bioreactors. Our work paves the way for portable, high-sensitivity, amplification-free, chemical assays with high throughput; introduces a new chemical imaging tool for probing chemical reactions in microenvironments; and establishes the foundation for developing movable, arrayed quantum sensors through droplet microfluidics.

quant-ph↗

arXiv2024

Experimental observation of a time rondeau crystal: Temporal Disorder in Spatiotemporal Order

Our understanding of phases of matter relies on symmetry breaking, one example being water ice whose crystalline structure breaks the continuous translation symmetry of space. Recently, breaking of time translation symmetry was observed in systems not in thermal equilibrium. The associated notion of time crystallinity has led to a surge of interest, raising the question about the extent to which highly controllable quantum simulators can generate rich and tunable temporal orders, beyond the conventional classification of order in static systems. Here, we investigate different kinds of partial temporal orders, stabilized by non-periodic yet structured drives, which we call rondeau order. Using a $^{13}$C-nuclear-spin diamond quantum simulator, we report the first experimental observation of a -- tunable degree of -- short-time disorder in a system exhibiting long-time stroboscopic order. This is based on a novel spin control architecture that allows us to implement a family of drives ranging from structureless via structured random to quasiperiodic and periodic drives. Leveraging a high throughput read-out scheme, we continuously observe the spin polarization over 105 pulses to probe rondeau order, with controllable lifetimes exceeding 4 seconds. Using the freedom in the short-time temporal disorder of rondeau order, we show the capacity to encode information in the response of observables. Our work broadens the landscape of observed nonequilibrium temporal order, paving the way for new applications harnessing driven quantum matter.

quant-ph↗

arXiv2024

Room-temperature quantum sensing with photoexcited triplet electrons in organic crystals

Quantum sensors have notably advanced high-sensitivity magnetic field detection. Here, we report quantum sensors constructed from polarized spin-triplet electrons in photoexcited organic chromophores, specifically focusing on pentacene-doped para-terphenyl (${\approx}$0.1%). We demonstrate essential quantum sensing properties at room temperature: electronic optical polarization and state-dependent fluorescence contrast, by leveraging differential pumping and relaxation rates between triplet and ground states. We measure high optically detected magnetic resonance (ODMR) contrast ${\approx}16.8\%$ of the triplet states at room temperature, along with long coherence times under spin echo and CPMG sequences, $T_2{=}2.7\mu$s and $T_2^{DD}{=}18.4\mu$s respectively, limited only by the triplet lifetimes. The material offers several advantages for quantum sensing, including the ability to grow large ($cm$-scale) crystals at low cost, the absence of paramagnetic impurities, and the diamagnetism of electronic states used for sensing when not optically illuminated. Utilizing pentacene as a representative of a broader class of spin triplet-polarizable organic molecules, this study highlights new potential for quantum sensing in chemical systems.

quant-ph↗

arXiv2023

Nanoscale engineering and dynamical stabilization of mesoscopic spin textures

Thermalization phenomena, while ubiquitous in quantum systems, have traditionally been viewed as obstacles to be mitigated. In this study, we demonstrate the ability, instead, to harness thermalization to dynamically engineer and stabilize structured quantum states in a mesoscopically large ensemble of spins. Specifically, we showcase the capacity to generate, control, stabilize, and read out 'shell-like' spin texture with interacting $ {}^{ 13}\mathrm{C}$ nuclear spins in diamond, wherein spins are polarized oppositely on either side of a critical radius. The texture spans several nanometers and encompasses many hundred spins. We capitalize on the thermalization process to impose a quasi-equilibrium upon the generated texture; as a result, it is highly stable, immune to spin diffusion, and endures over multiple-minute long periods -- over a million times longer than the intrinsic interaction scale of the spins. Additionally, the texture is created and interrogated without locally controlling or probing the nuclear spins. These features are accomplished using an electron spin as a nanoscale injector of spin polarization, and employing it as a source of spatially varying dissipation, allowing for serial readout of the emergent spin texture. Long-time stabilization is achieved via prethermalization to a Floquet-induced Hamiltonian under the electronic gradient field. Our work presents a new approach to robust nanoscale spin state engineering and paves the way for new applications in quantum simulation, quantum information science, and nanoscale imaging.

quant-ph↗

arXiv2022

Observation of a critical prethermal discrete time crystal created by two-frequency driving

We report the observation of long-lived Floquet prethermal discrete time crystalline (PDTC) order in a three-dimensional position-disordered lattice of interacting dipolar-coupled 13C nuclei in diamond at room temperature. We demonstrate a novel strategy of "two-frequency" driving, involving an interleaved application of slow and fast drives that simultaneously prethermalize the spins with an emergent quasi-conserved magnetization along the x-axis, while enabling continuous and highly resolved observation of their dynamic evolution when periodically kicked away from x. The PDTC order manifests itself in a robust period doubling response of this drive-induced quasi-conserved spin magnetization interchanging between x and -x; our experiments allow a unique means to study the formation and melting of PDTC order. We obtain movies of the time-crystalline response with a clarity and throughput orders of magnitude greater than previous experiments. Parametric control over the drive frequencies allows us to reach PDTC lifetimes up to 396 Floquet cycles which we measure in a single-shot experiment. Such rapid measurement enables detailed characterization of the entire PDTC phase diagram, rigidity and lifetime, informing on the role of prethermalization towards stabilizing the DTC response. The two-frequency drive approach represents the simplest generalization of DTCs to multi-frequency drives; it expands the toolkit for realizing and investigating long-lived non-equilibrium phases of matter stabilized by emergent quasi-conservation laws.

quant-ph↗

arXiv2022

Rapidly enhanced spin polarization injection in an optically pumped spin ratchet

Rapid injection of spin polarization into an ensemble of nuclear spins is a problem of broad interest, spanning dynamic nuclear polarization (DNP) to quantum information science. We report on a strategy to boost the spin injection rate by exploiting electrons that can be rapidly polarized via high-power optical pumping. We demonstrate this in a model system of Nitrogen Vacancy center electrons injecting polarization into a bath of 13C nuclei in diamond. We deliver >20W of continuous, nearly isotropic, optical power to the sample, constituting a substantially higher power than in previous experiments. Through a spin-ratchet polarization transfer mechanism, we show boosts in spin injection rates by over two orders of magnitude. Our experiments elucidate bottlenecks in the DNP process caused by rates of electron polarization, polarization transfer to proximal nuclei, and spin diffusion. This work demonstrates opportunities for rapid spin injection employing non-thermally generated electron polarization, and has relevance to a broad class of experimental systems including in DNP, quantum sensing, and spin-based MASERs.

quant-ph↗

arXiv2022

Continuously tracked, stable, large excursion trajectories of dipolar coupled nuclear spins

We report an experimental approach to excite, stabilize, and continuously track Bloch sphere orbits of dipolar-coupled nuclear spins in a solid. We demonstrate these results on a model system of hyperpolarized 13C nuclear spins in diamond. Without quantum control, inter-spin coupling leads to rapid spin decay in T2*=1.5ms. We elucidate a method to preserve trajectories for over T2'>27s at excursion solid angles up to 16 degrees, even in the presence of strong inter-spin coupling. This exploits a novel spin driving strategy that thermalizes the spins to a long-lived dipolar many-body state, while driving them in highly stable orbits. We show that motion of the spins can be quasi-continuously tracked for over 35s in three dimensions on the Bloch sphere. In this time the spins complete >68,000 closed precession orbits, demonstrating high stability and robustness against error. We experimentally probe the transient approach to such rigid motion, and thereby show the ability to engineer highly stable "designer" spin trajectories. Our results suggest new ways to stabilize and interrogate strongly-coupled quantum systems through periodic driving and portend powerful applications of rigid spin orbits in quantum sensing.

quant-ph↗

arXiv2021

High-Field Magnetometry with Hyperpolarized Nuclear Spins

Quantum sensors have attracted broad interest in the quest towards sub-micronscale NMR spectroscopy. Such sensors predominantly operate at low magnetic fields. Instead, however, for high resolution spectroscopy, the high-field regime is naturally advantageous because it allows high absolute chemical shift discrimination. Here we propose and demonstrate a high-field spin magnetometer constructed from an ensemble of hyperpolarized ${}^{13}C$ nuclear spins in diamond. The ${}^{13}C$ nuclei are initialized via Nitrogen Vacancy (NV) centers and protected along a transverse Bloch sphere axis for minute-long periods. When exposed to a time-varying (AC) magnetic field, they undergo secondary precessions that carry an imprint of its frequency and amplitude. The method harnesses long rotating frame ${}^{13}C$ sensor lifetimes $T_2^{\prime}{>}$20s, and their ability to be continuously interrogated. For quantum sensing at 7T and a single crystal sample, we demonstrate spectral resolution better than 100 mHz (corresponding to a frequency precision ${<}$1ppm) and single-shot sensitivity better than 70pT. We discuss the advantages of nuclear spin magnetometers over conventional NV center sensors, including deployability in randomly-oriented diamond particles and in optically scattering media. Since our technique employs densely-packed ${}^{13}C$ nuclei as sensors, it demonstrates a new approach for magnetometry in the "coupled-sensor" limit. This work points to interesting opportunities for microscale NMR chemical sensors constructed from hyperpolarized nanodiamonds and suggests applications of dynamic nuclear polarization (DNP) in quantum sensing.

quant-ph↗

arXiv2021

Floquet prethermalization with lifetime exceeding 90s in a bulk hyperpolarized solid

We report the observation of long-lived Floquet prethermal states in a bulk solid composed of dipolar-coupled $^{13}$C nuclei in diamond at room temperature. For precessing nuclear spins prepared in an initial transverse state, we demonstrate pulsed spin-lock Floquet control that prevents their decay over multiple-minute long periods. We observe Floquet prethermal lifetimes $T_2'\approx$90.9s, extended >60,000-fold over the nuclear free induction decay times. The spins themselves are continuously interrogated for $\sim$10min, corresponding to the application of $\approx$5.8M control pulses. The $^{13}$C nuclei are optically hyperpolarized by lattice Nitrogen Vacancy (NV) centers; the combination of hyperpolarization and continuous spin readout yields significant signal-to-noise in the measurements. This allows probing the Floquet thermalization dynamics with unprecedented clarity. We identify four characteristic regimes of the thermalization process, discerning short-time transient processes leading to the prethermal plateau, and long-time system heating towards infinite temperature. This work points to new opportunities possible via Floquet control in networks of dilute, randomly distributed, low-sensitivity nuclei. In particular, the combination of minutes-long prethermal lifetimes and continuous spin interrogation opens avenues for quantum sensors constructed from hyperpolarized Floquet prethermal nuclei.

quant-ph↗