arXiv subjects

Arjun Pillai

Publications and source records attributed to Arjun Pillai.

12 recordsLinked to original sources

arXiv2026

Quantum Sensors for Chemistry and Materials Science

The advancement of chemistry and materials science relies on transformative analytical tools which can overcome the sensitivity, spatial resolution, and throughput limitations of conventional techniques. This review explores the application of quantum sensors - specifically optically pumped magnetometers (OPMs) and nitrogen-vacancy (NV) centers in diamond - as robust platforms for molecular and materials analysis. We contrast the extreme magnetic sensitivity of macroscopic OPM ensembles with the atomic-scale resolution and multimodal capabilities of solid-state NV centers. We highlight their deployment in zero- to ultralow-field and nanoscale NMR spectroscopy, real-time reaction monitoring, and transient radical and pH detection. Furthermore, we discuss their integration into high-throughput chemical assays and non-destructive materials diagnostics, such as operando battery monitoring. With the ongoing commercialization of these technologies and advances in quantum-enhanced sensitivities, quantum sensors are poised to routinely address complex real-world analytical challenges.

quant-ph↗

arXiv2026

First-Token Broadcasters: Mechanistic Origins of Language Identity and Distributed Robustness in Transformers

Why do multilingual language models sometimes generate in the wrong language, and why is this so hard to fix? We introduce Language Identity Head Ablation (LIHA), a causal intervention that zeros each attention head individually and measures the resulting language switch rate across a parallel dataset of 2,700 prompt-language pairs spanning seven languages. Applied to GPT-2, LIHA identifies a small set of first-token broadcaster heads - led by L6H1 (switch rate 0.32, 3.23 $\sigma$ above the population mean) - that attend persistently to the first prompt token, propagating its language signal throughout generation. Compensatory redistribution when heads are ablated is statistically significant (p < $10^{-5}$) and follows a directional, hierarchical pattern: compensation always recruits heads in layers above the ablated head, suggesting a feedforward cascade rather than global diffusion. To probe how training regime shapes these circuits, we apply LIHA to a controlled pair - Qwen2.5-1.5B-Base and Qwen2.5-1.5B-Instruct - identical in architecture and size, differing only in training. The base model is nearly flat (max SR=0.016, 200/336 heads at SR=0.0); the instruct model concentrates causal influence sharply at layer 0, led by L0H5 (SR=0.224, 8.93 $\sigma$ above mean), with all other layers near zero. This controlled comparison provides direct causal evidence that instruction tuning reorganizes language identity circuits toward early-layer localization. Extended experiments with Chinese and Russian confirm that first-token broadcasting is script-specific in GPT-2, with non-Latin languages handled at layer 0 - the same locus as the instruction-tuned model. Code and data will be released upon publication.

cs.CL↗

arXiv2025

Wideband covariance magnetometry below the diffraction limit

We experimentally demonstrate a method for measuring correlations of wideband magnetic signals with spatial resolution below the optical diffraction limit. Our technique employs two nitrogen-vacancy (NV) centers in diamond as nanoscale magnetometers, spectrally resolved by inhomogeneous optical transitions. Using high-fidelity optical readout and long spin coherence time, we probe correlated MHz-range noise with sensitivity of 15 nT Hz$^{-1/4}$. In addition, we use this system for correlated $T_1$ relaxometry, enabling correlation measurements of GHz-range noise. Under such externally applied noise, while individual NV centers exhibit featureless relaxation, their correlation displays rich coherent and incoherent dynamics reminiscent of superradiance physics. This capability to probe high-frequency correlations provides a powerful tool for investigating a variety of condensed-matter phenomena characterized by nonlocal correlations.

quant-ph↗

arXiv2023

Roadmap on Nanoscale Magnetic Resonance Imaging

The field of nanoscale magnetic resonance imaging (NanoMRI) was started 30 years ago. It was motivated by the desire to image single molecules and molecular assemblies, such as proteins and virus particles, with near-atomic spatial resolution and on a length scale of 100 nm. Over the years, the NanoMRI field has also expanded to include the goal of useful high-resolution nuclear magnetic resonance (NMR) spectroscopy of molecules under ambient conditions, including samples up to the micron-scale. The realization of these goals requires the development of spin detection techniques that are many orders of magnitude more sensitive than conventional NMR and MRI, capable of detecting and controlling nanoscale ensembles of spins. Over the years, a number of different technical approaches to NanoMRI have emerged, each possessing a distinct set of capabilities for basic and applied areas of science. The goal of this roadmap article is to report the current state of the art in NanoMRI technologies, outline the areas where they are poised to have impact, identify the challenges that lie ahead, and propose methods to meet these challenges. This roadmap also shows how developments in NanoMRI techniques can lead to breakthroughs in emerging quantum science and technology applications.

cond-mat.mes-hall↗

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

Electron induced nanoscale nuclear spin relaxation probed by hyperpolarization injection

We report on experiments that quantify the role of a central electronic spin as a relaxation source for nuclear spins in its nanoscale environment. Our strategy exploits hyperpolarization injection from the electron as a means to controllably probe an increasing number of nuclear spins in the bath, and subsequently interrogate them with high fidelity. Our experiments are focused on a model system of a nitrogen vacancy (NV) center electronic spin surrounded by several hundred 13C nuclear spins. We observe that the 13C transverse spin relaxation times vary significantly with the extent of hyperpolarization injection, allowing the ability to measure the influence of electron mediated relaxation extending over several nanometers. These results suggest interesting new means to spatially discriminate nuclear spins in a nanoscale environment, and have direct relevance to dynamic nuclear polarization and quantum sensors and memories constructed from hyperpolarized nuclei.

cond-mat.mes-hall↗

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↗

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↗

arXiv2021

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↗

arXiv2021

"Galton board" nuclear hyperpolarization

We consider the problem of determining the spectrum of an electronic spin via polarization transfer to coupled nuclear spins and their subsequent readout. This suggests applications for employing dynamic nuclear polarization (DNP) for "ESR-via-NMR". In this paper, we describe the theoretical basis for this process by developing a model for the evolution dynamics of the coupled electron-nuclear system through a cascade of Landau-Zener anti-crossings (LZ-LACs). We develop a method to map these traversals to the operation of an equivalent "Galton board". Here, LZ-LAC points serve as analogues to Galton board "pegs", upon interacting with which the nuclear populations redistribute. The developed hyperpolarization then tracks the local electronic density of states. We show that this approach yields an intuitive and analytically tractable solution of the polarization transfer dynamics, including when DNP is carried out at the wing of a homogeneously broadened electronic spectral line. We apply this approach to a model system comprised of a Nitrogen Vacancy (NV) center electron in diamond, hyperfine coupled to N neighboring 13C nuclear spins, and discuss applications for nuclear-spin interrogated NV center magnetometry. More broadly, the methodology of "one-to-many" electron-to-nuclear spectral mapping developed here suggests interesting applications in quantum memories and sensing, as well as wider applications in modeling DNP processes in the multiple nuclear spin limit.

quant-ph↗

arXiv2021

Electron-to-nuclear spectral mapping via "Galton board" dynamic nuclear polarization

We report on a strategy to indirectly readout the spectrum of an electronic spin via polarization transfer to nuclear spins in its local environment. The nuclear spins are far more abundant and have longer lifetimes, allowing repeated polarization accumulation in them. Subsequent nuclear interrogation can reveal information about the electronic spectral density of states. We experimentally demonstrate the method for reading out the ESR spectrum of Nitrogen Vacancy center electrons in diamond via readout of lattice 13C nuclei. Spin-lock control on the 13C nuclei yields significantly enhanced signal-to-noise for the nuclear readout. Spectrally mapped readout presents operational advantages in being background-free and immune to crystal orientation and optical scattering. We harness these advantages to demonstrate applications in underwater magnetometry. The physical basis for the "one-to-many" spectral map is itself intriguing. To uncover its origin, we develop a theoretical model that maps the system dynamics, involving traversal of a cascaded structure of Landau-Zener anti-crossings, to the operation of a tilted "Galton board". This work points to new opportunities for "ESR-via-NMR" in dilute electronic systems, and in hybrid electron-nuclear quantum memories and sensors.

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↗