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Raffi Budakian

Publications and source records attributed to Raffi Budakian.

16 recordsLinked to original sources
arXiv2026

Long-Lived Mechanically-Detected Molecular Spins for Quantum Sensing

Quantum sensors based on individual spins provide unprecedented access to local magnetic fields in condensed matter, chemistry, and biology, with solid-state defect spins emerging as the leading platform. However, their molecular-sensing capabilities are limited by confinement to a host lattice, which prevents placement in close proximity to a target molecule. Molecular spins offer an alternative, enabling chemical tunability and flexible positioning relative to the target system. Here we present a nanoscale sensing platform that combines molecular electron spins, ultrasensitive mechanical readout, and Hamiltonian engineering. Using a modified XYXY dipolar decoupling sequence, we suppress electron-electron dipolar interactions across a broad distribution of control fields, extending coherence times to $\sim 400~μ$s in an attoliter-scale droplet containing $\sim$100 trityl-OX063 radicals. Leveraging this sequence, we demonstrate frequency-selective detection of nanotesla-scale AC fields and perform sensing and spectroscopy of small, local nuclear-spin ensembles. Collectively, these results establish SQUINT (Spin-based QUantum Integrated Nanomechanical Transduction) as a framework for quantum sensing that affords molecular-level control over sensor properties and enables direct integration into complex molecular targets.

quant-ph↗
arXiv2025

Magnetically-controlled Vortex Dynamics in a Ferromagnetic Superconductor

Ferromagnetic superconductors are exceptionally rare because the strong ferromagnetic exchange field usually destroys singlet superconductivity. EuFe$_2$(As$_{1-x}$P$_x$)$_2$, an iron-based superconductor with a maximum critical temperature of 25 K, uniquely exhibits full coexistence with ferromagnetic order below $T_\mathrm{FM}$ $\simeq$ $19$ K. The interplay leads to narrowing of ferromagnetic domains at higher temperatures and spontaneous nucleation of vortices/antivortices at lower temperatures. Here we demonstrate how the underlying magnetic structure controls the superconducting vortex dynamics in applied magnetic fields. Just below $T_\mathrm{FM}$ we observe a pronounced peak in the creep activation energy, and magnetic force microscopy measurements reveal the presence of very closely-spaced ($w\ll λ$) vortex clusters. We attribute these observations to the formation of vortex polarons for which we present a theoretical description. In contrast, we link strong magnetic irreversibility at low temperatures to a critical current governed by giant flux creep over an activation barrier for vortex-antivortex annihilation near domain walls. Our work suggests new routes for the magnetic enhancement of vortex pinning with important applications in high-current conductors.

cond-mat.supr-con↗
arXiv2024

Large-Enhancement Nanoscale Dynamic Nuclear Polarization Near a Silicon Nanowire Surface

Dynamic nuclear polarization (DNP) has revolutionized the field of NMR spectroscopy, expanding its reach and capabilities to investigate diverse materials, biomolecules, and complex dynamic processes. Bringing high-efficiency DNP to the nanometer scale would open new avenues for studying nanoscale nuclear spin ensembles, such as single biomolecules, virus particles, and condensed matter systems. Combining pulsed DNP with nanoscale force-detected magnetic resonance measurements, we demonstrated a 100-fold enhancement in the Boltzmann polarization of proton spins in nanoscale sugar droplets at 6 K and 0.33 T. Crucially, this enhancement corresponds to a factor of 200 reduction in the averaging time compared to measurements that rely on the detection of statistical fluctuations in nanoscale nuclear spin ensembles. These results significantly advance the capabilities of force-detected magnetic resonance detection as a practical tool for nanoscale imaging.

cond-mat.mes-hall↗
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↗
arXiv2022

Nanometer-Scale Nuclear Magnetic Resonance Diffraction with Sub-Ångstrom Precision

Achieving atomic resolution is the ultimate limit of magnetic resonance imaging (MRI), and attaining this capability offers enormous technological and scientific opportunities, from drug development to understanding the dynamics in interacting quantum systems. In this work, we present a new approach to nanoMRI utilizing nuclear magnetic resonance diffraction (NMRd) -- a method that extends NMR imaging to probe the structure of periodic spin systems. The realization of NMRd on the atomic scale would create a powerful new methodology for materials characterization utilizing the spectroscopic capabilities of NMR. We describe two experiments that realize NMRd measurement of $^{31}$P spins in an indium-phosphide (InP) nanowire with sub-Ångstrom precision. In the first experiment, we encode a nanometer-scale spatial modulation of the $z$-axis magnetization by periodically inverting the $^{31}$P spins, and detect the period and position of the modulation with a precision of $<0.8$ Å. In the second experiment, we demonstrate an interferometric technique, utilizing NMRd, for detecting an Ångstrom-scale displacement of the InP sample with a precision of 0.07 Å. The diffraction-based techniques developed in this work represent new measurement modalities in NMR for probing the structure and dynamics of spins on sub-Ångstrom length scales, and demonstrate the feasibility of crystallographic MRI measurements.

cond-mat.mes-hall↗
arXiv2021

Imaging and controlling vortex dynamics in mesoscopic superconductor-normal-metal-superconductor arrays

Harnessing the properties of vortices in superconductors is crucial for fundamental science and technological applications; thus, it has been an ongoing goal to locally probe and control vortices. Here, we use a scanning probe technique that enables studies of vortex dynamics in superconducting systems by leveraging the resonant behavior of a raster-scanned, magnetic-tipped cantilever. This experimental setup allows us to image and control vortices, as well as extract key energy scales of the vortex interactions. Applying this technique to lattices of superconductor island arrays on a metal, we obtain a variety of striking spatial patterns that encode information about the energy landscape for vortices in the system. We interpret these patterns in terms of local vortex dynamics and extract the relative strengths of the characteristic energy scales in the system, such as the vortex-magnetic field and vortex-vortex interaction strengths, as well as the vortex chemical potential. We also demonstrate that the relative strengths of the interactions can be tuned and show how these interactions shift with an applied bias. The high degree of tunability and local nature of such vortex imaging and control not only enable new understanding of vortex interactions, but also have potential applications in more complex systems such as those relevant to quantum computing.

cond-mat.supr-con↗
arXiv2021

Numerical Engineering of Robust Adiabatic Operations

Adiabatic operations are powerful tools for robust quantum control in numerous fields of physics, chemistry and quantum information science. The inherent robustness due to adiabaticity can, however, be impaired in applications requiring short evolution times. We present a single versatile gradient-based optimization protocol that combines adiabatic control with effective Hamiltonian engineering in order to design adiabatic operations tailored to the specific imperfections and resources of an experimental setup. The practicality of the protocol is demonstrated by engineering a fast, 2.3 Rabi cycle-long adiabatic inversion pulse for magnetic resonance with built-in robustness to Rabi field inhomogeneities and resonance offsets. The performance and robustness of the pulse is validated in a nanoscale force-detected magnetic resonance experiment on a solid-state sample, indicating an ensemble-averaged inversion accuracy of $\sim 99.997\%$. We further showcase the utility of our protocol by providing examples of adiabatic pulses robust to spin-spin interactions, parameter-selective operations and operations connecting arbitrary states, each motivated by experiments.

quant-ph↗
arXiv2019

Ultra-low dissipation patterned silicon nanowire arrays for scanning probe microscopy

In recent years, self-assembled semiconductor nanowires have been successfully used as ultra-sensitive cantilevers in a number of unique scanning probe microscopy (SPM) settings. We describe the fabrication of ultra-low dissipation patterned silicon nanowire (SiNW) arrays optimized for scanning probe applications. Our fabrication process produces, with high yield, ultra-high aspect ratio vertical SiNWs that exhibit exceptional force sensitivity. The highest sensitivity SiNWs have thermomechanical-noise limited force sensitivity of $9.7\pm0.4~\text{aN}/\sqrt{\text{Hz}}$ at room temperature and $500\pm20~\text{zN}/\sqrt{\text{Hz}}$ at 4 K. To facilitate their use in SPM, the SiNWs are patterned within $7~μ\text{m}$ from the edge of the substrate, allowing convenient optical access for displacement detection.

physics.app-ph↗
arXiv2019

Manipulating multi-vortex states in superconducting structures

We demonstrate a method for manipulating small ensembles of vortices in multiply-connected superconducting structures. A micron-size magnetic particle attached to the tip of a silicon cantilever is used to locally apply magnetic flux through the superconducting structure. By scanning the tip over the surface of the device, and by utilizing the dynamical coupling between the vortices and the cantilever, a high-resolution spatial map of the different vortex configurations is obtained. Moving the tip to a particular location in the map stabilizes a distinct multi-vortex configuration. Thus, the scanning of the tip over a particular trajectory in space permits non-trivial operations to be performed, such as braiding of individual vortices within a larger vortex ensemble -- a key capability required by many proposals for topological quantum computing.

cond-mat.mes-hall↗
arXiv2018

Imaging phase slip dynamics in micron-size superconducting rings

We present a scanning probe technique for measuring the dynamics of individual fluxoid transitions in multiply connected superconducting structures. In these measurements, a small magnetic particle attached to the tip of a silicon cantilever is scanned over a micron-size superconducting ring fabricated from a thin aluminum film. We find that near the superconducting transition temperature of the aluminum, the dissipation and frequency of the cantilever changes significantly at particular locations where the tip-induced magnetic flux penetrating the ring causes the two lowest-energy fluxoid states to become nearly degenerate. In this regime, we show that changes in the cantilever frequency and dissipation are well-described by a stochastic resonance (SR) process, wherein small oscillations of the cantilever in the presence of thermally activated phase slips (TAPS) in the ring give rise to a dynamical force that modifies the mechanical properties of the cantilever. Using the SR model, we calculate the average fluctuation rate of the TAPS as a function of temperature over a 32-dB range in frequency, and we compare it to the Langer-Ambegaokar-McCumber-Halperin theory for TAPS in one-dimensional superconducting structures.

cond-mat.supr-con↗
arXiv2017

Adiabatic-NOVEL for Nano-Scale Magnetic Resonance Imaging

We propose a highly efficient dynamic nuclear polarization technique that is robust against field in-homogeneity. This technique is designed to enhance the detection sensitivity in nano-MRI, where large Rabi field gradients are required. The proposed technique consists of an adiabatic half passage pulse followed by an adiabatic linear sweep of the electron Rabi frequency and can be considered as an adiabatic version of nuclear orientation via electron spin locking (adiabatic-NOVEL). We analyze the spin dynamics of an electron-nuclear system that is under microwave irradiation at high static magnetic field and at cryogenic temperature. The result shows that an amplitude modulation of the microwave field makes adiabatic-NOVEL highly efficient and robust against both the static and microwave field in-homogeneity.

quant-ph↗
arXiv2017

High-Resolution Nanoscale Solid-State Nuclear Magnetic Resonance Spectroscopy

We present a new method for high-resolution nanoscale magnetic resonance imaging (nano-MRI) that combines the high spin sensitivity of nanowire-based magnetic resonance detection with high spectral resolution nuclear magnetic resonance (NMR) spectroscopy. By applying NMR pulses designed using optimal control theory, we demonstrate a factor of $500$ reduction of the proton spin resonance linewidth in a $(50\text{-nm})^{\text{3}}$ volume of polystyrene and image proton spins in one dimension with a spatial resolution below $2~\text{nm}$.

cond-mat.mes-hall↗
arXiv2013

Nanoscale Fourier-transform MRI

We report a method for nanometer-scale pulsed nuclear magnetic resonance imaging and spectroscopy. Periodic radiofrequency pulses are used to create temporal correlations in the statistical polarization of a solid organic sample. The spin density is spatially encoded by applying a series of intense magnetic field gradient pulses generated by focusing electric current through a nanometer-scale metal constriction. We demonstrate this technique using a silicon nanowire mechanical oscillator as a magnetic resonance sensor to image 1H spins in a polystyrene sample. We obtain a two-dimensional projection of the sample proton density with approximately 10-nm resolution.

cond-mat.mes-hall↗
arXiv2011

Nanomechanical detection of nuclear magnetic resonance using a silicon nanowire oscillator

We report the use of a silicon nanowire mechanical oscillator as a low-temperature nuclear magnetic resonance force sensor to detect the statistical polarization of 1H spins in polystyrene. Under operating conditions, the nanowire experienced negligible surface-induced dissipation and exhibited a nearly thermally-limited force noise of 1.9 aN^2/Hz in the measurement quadrature. In order to couple the 1H spins to the nanowire oscillator, we have developed a new magnetic resonance force detection protocol which utilizes a nanoscale current-carrying wire to produce large time-dependent magnetic field gradients as well as the rf magnetic field.

cond-mat.other↗
arXiv2010

Detection of Individual Vortices in Micron-Size Sr2RuO4 Rings by Phase-Locked Cantilever Magnetometry

We describe a feedback-based dynamic cantilever magnetometry technique capable of achieving high magnetic moment sensitivity with low applied fields. Using this technique, we have observed periodic entry of vortices into mesoscopic Sr2RuO4 rings. The quantized jump in the magnetic moment of the particle produced by individual vortices was measured with a resolution of 7x10^-16 e.m.u. at an applied field of 1 Oe.

cond-mat.supr-con↗