arXiv subjects

Christian L. Degen

Publications and source records attributed to Christian L. Degen.

At least 37 records · Page 2Linked to original sources

arXiv2024

Vibrational Squeezing via Spin Inversion Pulses

Magnetic Resonance Force Microscopy (MRFM) describes a range of approaches to detect nuclear spins with mechanical sensors. MRFM has the potential to enable magnetic resonance imaging (MRI) with near-atomic spatial resolution, opening up exciting possibilities in solid state and biological research. In many cases, the spin-mechanics coupling in MRFM is engineered with the help of periodic radio-frequency pulses. In this paper, we report that such pulses can result in unwanted parametric amplification of the mechanical vibrations, causing misinterpretation of the measured signal. We show how the parametric effect can be cancelled by auxiliary radio-frequency pulses or by appropriate post-correction after careful calibration. Future MRFM measurements may even make use of the parametric amplification to reduce the impact of amplifier noise

physics.app-ph↗

arXiv2024

Observation of current whirlpools in graphene at room temperature

Electron-electron interactions in high-mobility conductors can give rise to transport signatures resembling those described by classical hydrodynamics. Using a nanoscale scanning magnetometer, we imaged a distinctive hydrodynamic transport pattern - stationary current vortices - in a monolayer graphene device at room temperature. By measuring devices with increasing characteristic size, we observed the disappearance of the current vortex and thus verify a prediction of the hydrodynamic model. We further observed that vortex flow is present for both hole- and electron-dominated transport regimes, while disappearing in the ambipolar regime. We attribute this effect to a reduction of the vorticity diffusion length near charge neutrality. Our work showcases the power of local imaging techniques for unveiling exotic mesoscopic transport phenomena.

cond-mat.mes-hall↗

arXiv2024

Multiplexed scanning microscopy with dual-qubit spin sensors

Scanning probe microscopy with multi-qubit sensors offers the potential to improve imaging speed and measure previously inaccessible quantities, such as two-point correlations. We develop a multiplexed quantum sensing approach with scanning probes containing two nitrogen-vacancy (NV) centers at the tip apex. A shared optical channel is used for simultaneous qubit initialization and readout, while phase- and frequency-dependent microwave spin manipulations are leveraged for de-multiplexing the optical readout signal. Scanning dual-NV magnetometry is first demonstrated by simultaneously imaging multiple field projections of a ferrimagnetic racetrack device. Then, we record the two-point covariance of spatially correlated field fluctuations across a current-carrying wire. Our multiplex framework establishes a method to investigate a variety of spatio-temporal correlations, including phase transitions and electronic noise, with nanoscale resolution.

quant-ph↗

arXiv2024

Charge and Spin Dynamics and Destabilization of Shallow Nitrogen-Vacancy Centers under UV and Blue Excitation

Shallow nitrogen-vacancy (NV) centers in diamond offer unique opportunities for studying photochemical reactions at the single-molecule level, such as the photogeneration of radical pairs in proximal molecules. A prerequesite for such experimental schemes is the detailed understanding of the charge and spin dynamics of NV centers exposed to the short-wavelength light required for photoexciting chemical species. Here, we measure and analyze the charge and spin dynamics of shallow NV centers under 445 nm (blue) and 375 nm (UV) illumination. With blue excitation, we observe a power-dependent charge-state preparation accompanied by modest preservation of spin initialization fidelity. Under UV excitation, we find a power-independent charge-state preparation and no spin polarization. We further observe an irreversible aging of NV centers under prolonged exposure to UV, and to a lesser extent, blue laser excitation, which we attribute to formation of new electronic trap states. This aging manifests itself in a reduced charge stability and spin contrast, and is detrimental to the NV sensing performance. We evaluate the prospects and limitations of NV centers for probing photogenerated radical pairs based on experimentally measured sensitivities following blue and UV excitation, and outline the design rules for possible sensing schemes.

quant-ph↗

arXiv2024

Enhancing Membrane-Based Scanning Force Microscopy Through an Optical Cavity

The new generation of strained silicon nitride resonators harbors great promise for scanning force microscopy, especially when combined with the extensive toolbox of cavity optomechanics. However, accessing a mechanical resonator inside an optical cavity with a scanning tip is challenging. Here, we experimentally demonstrate a cavity-based scanning force microscope based on a silicon nitride membrane sensor. We overcome geometric constraints by making use of the extended nature of the mechanical resonator normal modes, which allows us to spatially separate the scanning and readout sites of the membrane. Our microscope is geared towards low-temperature applications in the zeptonewton regime, such as nanoscale nuclear spin detection and imaging.

physics.optics↗

arXiv2024

Multidimensional spectroscopy of nuclear spin clusters in diamond

Optically active spin defects in solids offer promising platforms to investigate nuclear spin clusters with high sensitivity and atomic-site resolution. To leverage near-surface defects for molecular structure analysis in chemical and biological contexts using nuclear magnetic resonance (NMR), further advances in spectroscopic characterization of nuclear environments are essential. Here, we report Fourier spectroscopy techniques to improve localization and mapping of the testbed $^{13}\mathrm{C}$ nuclear spin environment of individual, shallow nitrogen-vacancy centers at room temperature. We use multidimensional spectroscopy, well-known from classical NMR, in combination with weak measurements of single-nuclear-spin precession. We demonstrate two examples of multidimensional NMR: (i) improved nuclear spin localization by separate encoding of the two hyperfine components along spectral dimensions and (ii) spectral editing of nuclear-spin pairs, including measurement of internuclear coupling constants. Our work adds important tools for the spectroscopic analysis of molecular structures by single-spin probes.

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 magnets embedded in a microstrip

Nanoscale magnetic resonance imaging (NanoMRI) is an active area of applied research with potential use in structural biology and quantum engineering. The success of this technological vision hinges on improving the instrument's sensitivity and functionality. A particular challenge is the optimization of the magnetic field gradient required for spatial encoding, and of the radio-frequency field used for spin control, in analogy to the components used in clinical MRI. In this work, we present the fabrication and characterization of a magnet-in-microstrip device that yields a compact form factor for both elements. We find that our design leads to a number of advantages, among them a fourfold increase of the magnetic field gradient compared to those achieved with traditional fabrication methods. Our results can be useful for boosting the efficiency of a variety of different experimental arrangements and detection principles in the field of NanoMRI.

physics.app-ph↗

arXiv2023

Near-resonant nuclear spin detection with high-frequency mechanical resonators

Mechanical resonators operating in the high-frequency regime have become a versatile platform for fundamental and applied quantum research. Their exceptional properties, such as low mass and high quality factor, make them also very appealing for force sensing experiments. In this Letter, we propose a method for detecting and ultimately controlling nuclear spins by directly coupling them to high-frequency resonators via a magnetic field gradient. Dynamical backaction between the sensor and an ensemble of nuclear spins produces a shift in the sensor's resonance frequency, which can be measured to probe the spin ensemble. Based on analytical as well as numerical results, we predict that the method will allow nanoscale magnetic resonance imaging with a range of realistic devices. At the same time, this interaction paves the way for new manipulation techniques, similar to those employed in cavity optomechanics, enriching both the sensor's and the spin ensemble's features.

cond-mat.mes-hall↗

arXiv2023

Modeling temperature-dependent population dynamics in the excited state of the nitrogen-vacancy center in diamond

The nitrogen-vacancy (NV) center in diamond is well known in quantum metrology and quantum information for its favorable spin and optical properties, which span a wide temperature range from near zero to over 600 K. Despite its prominence, the NV center's photo-physics is incompletely understood, especially at intermediate temperatures between 10-100 K where phonons become activated. In this work, we present a rate model able to describe the cross-over from the low-temperature to the high-temperature regime. Key to the model is a phonon-driven hopping between the two orbital branches in the excited state (ES), which accelerates spin relaxation via an interplay with the ES spin precession. We extend our model to include magnetic and electric fields as well as crystal strain, allowing us to simulate the population dynamics over a wide range of experimental conditions. Our model recovers existing descriptions for the low- and high-temperature limits, and successfully explains various sets of literature data. Further, the model allows us to predict experimental observables, in particular the photoluminescence (PL) emission rate, spin contrast, and spin initialization fidelity relevant for quantum applications. Lastly, our model allows probing the electron-phonon interaction of the NV center and reveals a gap between the current understanding and recent experimental findings.

cond-mat.mes-hall↗

arXiv2023

Temperature dependence of photoluminescence intensity and spin contrast in nitrogen-vacancy centers

We report on measurements of the photoluminescence (PL) properties of single nitrogen-vacancy (NV) centers in diamond at temperatures between 4-300 K. We observe a strong reduction of the PL intensity and spin contrast between ca. 10-100 K that recovers to high levels below and above. Further, we find a rich dependence on magnetic bias field and crystal strain. We develop a comprehensive model based on spin mixing and orbital hopping in the electronic excited state that quantitatively explains the observations. Beyond a more complete understanding of the excited-state dynamics, our work provides a novel approach for probing electron-phonon interactions and a predictive tool for optimizing experimental conditions for quantum applications.

cond-mat.mes-hall↗

arXiv2023

Multicone Diamond Waveguides for Nanoscale Quantum Sensing

The long-lived electronic spin of the nitrogen-vacancy (NV) center in diamond is a promising quantum sensor for detecting nanoscopic magnetic and electric fields in a variety of experimental conditions. Nevertheless, an outstanding challenge in improving measurement sensitivity is the poor signal-to-noise ratio (SNR) of prevalent optical spin-readout techniques. Here, we address this limitation by coupling individual NV centers to optimized diamond nanopillar structures, thereby improving optical collection efficiency of fluorescence. First, we optimize the structure in simulation, observing an increase in collection efficiency for tall ($\geq$ 5 $μ$m) pillars with tapered sidewalls. We subsequently verify these predictions by fabricating and characterizing a representative set of structures using a reliable and reproducible nanofabrication process. An optimized device yields increased SNR, owing to improvements in collimation and directionality of emission. Promisingly, these devices are compatible with low-numerical-aperture, long-working-distance collection optics, as well as reduced tip radius, facilitating improved spatial resolution for scanning applications.

quant-ph↗

arXiv2023

Towards Quantum Sensing of Chiral-Induced Spin Selectivity: Probing Donor-Bridge-Acceptor Molecules with NV Centers in Diamond

Photoexcitable donor-bridge-acceptor (D-B-A) molecules that support intramolecular charge transfer are ideal platforms to probe the influence of chiral-induced spin selectivity (CISS) in electron transfer and resulting radical pairs. In particular, the extent to which CISS influences spin polarization or spin coherence in the initial state of spin-correlated radical pairs following charge transfer through a chiral bridge remains an open question. Here, we introduce a quantum sensing scheme to measure directly the hypothesized spin polarization in radical pairs using shallow nitrogen-vacancy (NV) centers in diamond at the single- to few-molecule level. Importantly, we highlight the perturbative nature of the electron spin-spin dipolar coupling within the radical pair, and demonstrate how Lee-Goldburg decoupling can preserve spin polarization in D-B-A molecules for enantioselective detection by a single NV center. The proposed measurements will provide fresh insight into spin selectivity in electron transfer reactions.

quant-ph↗

arXiv2023

Current-driven dynamics and ratchet effect of skyrmion bubbles in a ferrimagnetic insulator

Magnetic skyrmions are compact chiral spin textures that exhibit a rich variety of topological phenomena and hold potential for developing high-density memory devices and novel computing schemes driven by spin currents. Here, we demonstrate room temperature interfacial stabilization and current-driven control of skyrmion bubbles in the ferrimagnetic insulator Tm3Fe5O12 (TmIG) coupled to Pt. We track the current-induced motion of individual skyrmion bubbles. The ferrimagnetic order of the crystal together with the interplay of spin-orbit torques and pinning determine the skyrmion dynamics in TmIG and result in a strong skyrmion Hall effect characterized by a negative deflection angle and hopping motion. Further, we show that the velocity and depinning threshold of the skyrmion bubbles can be modified by exchange coupling TmIG to an in-plane magnetized Y3Fe5O12 layer, which distorts the spin texture of the skyrmions and leads to a directional-dependent rectification of their dynamics. This effect, which is equivalent to a magnetic ratchet, is exploited to control the skyrmion flow in a racetrack-like device.

cond-mat.mes-hall↗

arXiv2022

Imaging ferroelectric domains with a single-spin scanning quantum sensor

The ability to sensitively image electric fields is important for understanding many nanoelectronic phenomena, including charge accumulation at surfaces and interfaces and field distributions in active electronic devices. A particularly exciting application is the visualization of domain patterns in ferroelectric and nanoferroic materials owing to their potential in computing and data storage. Here, we use a scanning nitrogen-vacancy (NV) microscope, well known for its use in magnetometry, to image domain patterns in piezoelectric (Pb[Zr$_{x}$Ti$_{1-x}$]O$_{3}$) and improper ferroelectric (YMnO$_{3}$) materials through their electric fields. Electric field detection is enabled by measuring the Stark shift of the NV spin using a gradiometric detection scheme. Analysis of the electric field maps allows us to discriminate between different types of surface charge distributions, as well as to reconstruct maps of the three-dimensional electric field vector and charge density. The ability to measure both stray electric and magnetic fields under ambient conditions opens exciting opportunities for the study of multiferroic and multifunctional materials and devices.

cond-mat.mes-hall↗

arXiv2022

Soft-clamped silicon nitride string resonators at millikelvin temperatures

We demonstrate that soft-clamped silicon nitride strings with large aspect ratio can be operated at \si{\milli\kelvin} temperatures. The quality factors ($Q$) of two measured devices show consistent dependency on the cryostat temperature, with soft-clamped mechanical modes reaching $Q > 10^9$ at $46~\mathrm{mK}$. For low optical readout power, $Q$ is found to saturate, indicating good thermalization between the sample and the stage it is mounted on. Our best device exhibits a force sensitivity of $9.6~\mathrm{zN}/\sqrt{\mathrm{Hz}}$ and a thermal decoherence time of $0.38~\mathrm{s}$ which bode well for future applications such as nanomechanical force sensing and beyond.

cond-mat.mes-hall↗

arXiv2022

Diamond surface engineering for molecular sensing with nitrogen-vacancy centers

Quantum sensing using optically addressable atomic-scale defects, such as the nitrogen--vacancy (NV) center in diamond, provides new opportunities for sensitive and highly localized characterization of chemical functionality. Notably, near-surface defects facilitate detection of the minute magnetic fields generated by nuclear or electron spins outside of the diamond crystal, such as those in chemisorbed and physisorbed molecules. However, the promise of NV centers is hindered by a severe degradation of critical sensor properties, namely charge stability and spin coherence, near surfaces (< ca. 10 nm deep). Moreover, applications in the chemical sciences require methods for covalent bonding of target molecules to diamond with robust control over density, orientation, and binding configuration. This forward-looking Review provides a survey of the rapidly converging fields of diamond surface science and NV-center physics, highlighting their combined potential for quantum sensing of molecules. We outline the diamond surface properties that are advantageous for NV-sensing applications, and discuss strategies to mitigate deleterious effects while simultaneously providing avenues for chemical attachment. Finally, we present an outlook on emerging applications in which the unprecedented sensitivity and spatial resolution of NV-based sensing could provide unique insight into chemically functionalized surfaces at the single-molecule level.

cond-mat.mtrl-sci↗

arXiv2022

Force-detected Magnetic Resonance Imaging of Influenza Viruses in the Overcoupled Sensor Regime

Long and thin scanning force cantilevers are sensitive to small forces, but also vulnerable to detrimental non-contact interactions. Here we present an experiment with a cantilever whose spring constant and static deflection are dominated by the interaction between the tip and the surface, a regime that we refer to as ``overcoupled''. The interactions are an obstacle for ultrasensitive measurements like nanoscale magnetic resonance imaging (nanoMRI). We discuss several strategies to overcome the challenges presented by the overcoupling, and demonstrate proton nanoMRI measurements of individual influenza virus particles.

cond-mat.mes-hall↗