arXiv subjects

Sam C. Scholten

Publications and source records attributed to Sam C. Scholten.

13 recordsLinked to original sources

arXiv2025

Spin-dependent photoluminescence in carbon-based quantum dots

The ability to modulate the photoluminescence (PL) of nanomaterials via spin-related effects is vital for many emerging quantum technologies, with nanoscale quantum sensing and imaging being particular areas of focus. Carbon-based quantum dots (CQDs) are among the most common forms of luminescent nanomaterials, appealing due to their ease of synthesis, tunability through organic chemistry, high brightness, and natural biocompatibility. However, the observation of room temperature, spin-dependent PL has remained elusive. Here we report on the observation of PL modulation of CQDs by magnetic fields ($\sim 10$ mT) under ambient conditions. We synthesize a series of CQDs using 19 different amino acids, which have a range of PL emission spectra and exhibit a clear magneto-PL effect (up to $\sim 1$% change). Furthermore, an electron spin resonance is detected in the PL with a g-factor of g $\approx$ 2, suggesting a process similar to the radical pair mechanism is responsible. Finally, we show that the magneto-PL contrast decreases in the presence of paramagnetic species, which we attribute to an increase in magnetic noise-induced spin relaxation in the CQDs. Our work brings new functionalities to these commonly used and biocompatible luminescent nanoparticles, opening new opportunities for in situ quantum sensing and imaging of biological samples.

cond-mat.mes-hall↗

arXiv2025

Optically detected magnetic resonance of wafer-scale hexagonal boron nitride thin films

Hexagonal boron nitride (hBN) has recently been shown to host native defects exhibiting optically detected magnetic resonance (ODMR) with applications in nanoscale magnetic sensing and imaging. To advance these applications, deposition methods to create wafer-scale hBN films with controlled thicknesses are desirable, but a systematic study of the ODMR properties of the resultant films is lacking. Here we perform ODMR measurements of thin films (3-2000nm thick) grown via three different methods: metal-organic chemical vapour deposition (MOCVD), chemical vapour deposition (CVD), and molecular beam epitaxy (MBE). We find that they all exhibit an ODMR response, including the thinnest 3nm film, albeit with different characteristics. The best volume-normalised magnetic sensitivity obtained is 30uT/sqrt(Hz um^3). We study the effect of growth temperature on a series of MOCVD samples grown under otherwise fixed conditions and find 800-900C to be an optimum range for magnetic sensitivity, with a significant improvement (up to two orders of magnitude) from post-growth annealing. This work provides a useful baseline for the magnetic sensitivity of hBN thin films deposited via standard methods and informs the feasibility of future sensing applications.

cond-mat.mtrl-sci↗

arXiv2025

A charge transfer mechanism for optically addressable solid-state spin pairs

Optically detected magnetic resonance (ODMR) with no resolvable zero-field splitting has been observed from emitters in hexagonal boron nitride across a broad range of wavelengths, but so far an understanding of their microscopic structure and the physical origin of ODMR has been lacking. Here we perform comprehensive measurements and modelling of the spin-resolved photodynamics of ensembles and single emitters, and uncover a universal model that accounts, and provides an intuitive physical explanation, for all key experimental features. The model, inspired by the radical-pair mechanism from spin chemistry, assumes a pair of nearby point defects -- a primary optically active defect and a secondary defect. Charge transfer between the two defects creates a metastable weakly coupled spin pair with ODMR naturally arising from selection rules. Using first-principle calculations, we show that simple defect pairs made of common carbon defects provide a plausible microscopic explanation. Our optical-spin defect pair (OSDP) model resolves several previously open questions including the asymmetric envelope of the Rabi oscillations, the large variability in ODMR contrast amplitude and sign, and the wide spread in emission wavelength. It may also explain similar phenomena observed in other wide bandgap semiconductors such as GaN. The presented framework will be instrumental in guiding future theoretical and experimental efforts to study and engineer solid-state spin pairs.

cond-mat.mes-hall↗

arXiv2024

Radiofrequency receiver based on isotropic solid-state spins

Optically addressable solid-state spins have been proposed as robust radiofrequency (RF)-optical transducers sensitive to a specific RF frequency tuned by an external static magnetic field, but often require precise field alignment with the system's symmetry axis. Here we introduce an isotropic solid-state spin system, namely weakly coupled spin pairs in hexagonal boron nitride (hBN), which acts as an RF-optical transducer independent of the direction of the tuning magnetic field, allowing greatly simplified experimental design. Using this platform, we first demonstrate a single-frequency RF receiver with frequency tunability from 0.1 to 19 GHz. We next demonstrate an instantaneous wideband RF spectrum analyser by applying a magnetic field gradient to encode RF frequency into spatial position. Finally, we utilise the spectrum analyser to detect free-space-transmitted RF signals matching the strength and frequency of typical Wi-Fi signals. This work exemplifies the unique capabilities of isotropic spins in hBN to operate as RF sensors, while circumventing the challenging requirement of precisely aligned magnetic fields facing conventional solid-state spins.

cond-mat.mes-hall↗

arXiv2024

Violet to near-infrared optical addressing of spin pairs in hexagonal boron nitride

Optically addressable solid-state spins are an important platform for practical quantum technologies. Van der Waals material hexagonal boron nitride (hBN) is a promising host as it contains a wide variety of optical emitters, but thus far observations of addressable spins have been sparse, and most of them lacked a demonstration of coherent spin control. Here we demonstrate robust optical readout of spin pairs in hBN with emission wavelengths spanning from violet to the near-infrared. We find these broadband spin pairs exist naturally in a variety of hBN samples from bulk crystals to powders to epitaxial films, and can be coherently controlled across the entire wavelength range. Furthermore, we identify the optimal wavelengths for independent readout of spin pairs and boron vacancy spin defects co-existing in the same sample. Our results establish the ubiquity of the optically addressable spin pair system in hBN across a broad parameter space, making it a versatile playground for spin-based quantum technologies.

cond-mat.mes-hall↗

arXiv2024

Towards high spatial resolution magnetic imaging with a compact practical quantum diamond microscope

Widefield quantum diamond microscopy is a powerful technique for imaging magnetic fields with high sensitivity and spatial resolution. However, current methods to approach the ultimate spatial resolution ($<500\,$nm) are impractical for routine use as they require time-consuming fabrication or transfer techniques to precisely interface the diamond sensor with the sample to be imaged. To address this challenge, we have designed a co-axial sensor holder that enables simple, repeatable sensor-sample interfacing while being compatible with high numerical aperture (NA) optics. With our new design we demonstrate low standoffs $<500\,$nm with a millimetre sized sensor. We also explore the relationship between spatial resolution and NA spanning from 0.13 to 1.3. The spatial resolution shows good agreement with the optical diffraction limit at low NA but deviates at high NA, which is shown to be due to optical aberrations. Future improvements to our design are discussed, which should enable magnetic imaging with $<500\,$nm resolution in an accessible, easy-to-use instrument.

cond-mat.mes-hall↗

arXiv2024

Multi-species optically addressable spin defects in a van der Waals material

Optically addressable spin defects hosted in two-dimensional van der Waals materials represent a new frontier for quantum technologies, promising to lead to a new class of ultrathin quantum sensors and simulators. Recently, hexagonal boron nitride (hBN) has been shown to host several types of optically addressable spin defects, thus offering a unique opportunity to simultaneously address and utilise various spin species in a single material. Here we demonstrate an interplay between two separate spin species within a single hBN crystal, namely $S=1$ boron vacancy defects and visible emitter spins. We unambiguously prove that the visible emitters are $S=\frac{1}{2}$ spins and further demonstrate room temperature coherent control and optical readout of both spin species. Importantly, by tuning the two spin species into resonance with each other, we observe cross-relaxation indicating strong inter-species dipolar coupling. We then demonstrate magnetic imaging using the $S=\frac{1}{2}$ defects, both under ambient and cryogenic conditions, and leverage their lack of intrinsic quantization axis to determine the anisotropic magnetic susceptibility of a test sample. Our results establish hBN as a versatile platform for quantum technologies in a van der Waals host at room temperature.

cond-mat.mes-hall↗

arXiv2023

Stray magnetic field imaging of thin exfoliated iron halides flakes

Magnetic van der Waals materials are often proposed for use in future spintronic devices, aiming to leverage the combination of long-range magnetic order and near-atomic thinness to produce energy-efficient components. One class of material that has been discussed in this context are the iron halides FeCl$_2$ and FeBr$_2$, which are A-type antiferromagnets with strong uniaxial magnetocrystalline anisotropy. However, despite characterization of the bulk materials, the possibility for sustaining the magnetic behaviors that would underpin such applications in thin flakes has not been investigated. In this work, we use nitrogen-vacancy (NV) center microscopy to quantitatively image magnetism in individual exfoliated flakes of these iron halides, revealing the absence of magnetic remanence, a weak induced magnetization under bias field and variable behavior versus temperature. We show that our results are consistent with the antiferromagnetic behavior of the bulk material with a soft ferromagnetic uncompensated layer, indicating that extended ($>1~μ$m) ferromagnetic domains are not sustained even at low temperatures (down to 4 K). Finally, we find that the magnetic order is strongly affected by the sample preparation, with a surprising diamagnetic order observed in a thin, hydrated sample.

cond-mat.mtrl-sci↗

arXiv2023

Detection of paramagnetic spins with an ultrathin van der Waals quantum sensor

Detecting magnetic noise from small quantities of paramagnetic spins is a powerful capability for chemical, biochemical, and medical analysis. Quantum sensors based on optically addressable spin defects in bulk semiconductors are typically employed for such purposes, but the 3D crystal structure of the sensor inhibits the sensitivity by limiting the proximity of the defects to the target spins. Here we demonstrate the detection of paramagnetic spins using spin defects hosted in hexagonal boron nitride (hBN), a van der Waals material which can be exfoliated into the 2D regime. We first create negatively charged boron vacancy (V$_{\rm B}^-$) defects in a powder of ultrathin hBN nanoflakes ($<10$~atomic monolayers thick on average) and measure the longitudinal spin relaxation time ($T_1$) of this system. We then decorate the dry hBN nanopowder with paramagnetic Gd$^{3+}$ ions and observe a clear $T_1$ quenching, under ambient conditions, consistent with the added magnetic noise. Finally, we demonstrate the possibility of performing spin measurements including $T_1$ relaxometry using solution-suspended hBN nanopowder. Our results highlight the potential and versatility of the hBN quantum sensor for a range of sensing applications, and pave the way towards the realisation of a truly 2D, ultrasensitive quantum sensor.

cond-mat.mes-hall↗

arXiv2023

Imaging current control of magnetization in Fe$_3$GeTe$_2$ with a widefield nitrogen-vacancy microscope

Van der Waals (vdW) magnets are appealing candidates for realising spintronic devices that exploit current control of magnetization (e.g. switching or domain wall motion), but so far experimental demonstrations have been sparse, in part because of challenges associated with imaging the magnetization in these systems. Widefield nitrogen-vacancy (NV) microscopy allows rapid, quantitative magnetic imaging across entire vdW flakes, ideal for capturing changes in the micromagnetic structure due to an electric current. Here we use a widefield NV microscope to study the effect of current injection in thin flakes ($\sim10$nm) of the vdW ferromagnet Fe$_3$GeTe$_2$ (FGT). We first observe current-reduced coercivity on an individual domain level, where current injection in FGT causes substantial reduction in the magnetic field required to locally reverse the magnetisation. We then explore the possibility of current-induced domain-wall motion, and provide preliminary evidence for such a motion under relatively low current densities, suggesting the existence of strong current-induced torques in our devices. Our results illustrate the applicability of widefield NV microscopy to imaging spintronic phenomena in vdW magnets, highlight the possibility of efficient magnetization control by direct current injection without assistance from an adjacent conductor, and motivate further investigations of the effect of currents in FGT and other vdW magnets.

cond-mat.mes-hall↗

arXiv2020

Improved current density and magnetisation reconstruction through vector magnetic field measurements

Stray magnetic fields contain significant information about the electronic and magnetic properties of condensed matter systems. For two-dimensional (2D) systems, stray field measurements can even allow full determination of the source quantity. For instance, a 2D map of the stray magnetic field can be uniquely transformed into the 2D current density that gave rise to the field and, under some conditions, into the equivalent 2D magnetisation. However, implementing these transformations typically requires truncation of the initial data and involves singularities that may introduce errors, artefacts, and amplify noise. Here we investigate the possibility of mitigating these issues through vector measurements. For each scenario (current reconstruction and magnetisation reconstruction) the different possible reconstruction pathways are analysed and their performances compared. In particular, we find that the simultaneous measurement of both in-plane components ($B_x$ and $B_y$) enables near-ideal reconstruction of the current density, without singularity or truncation artefacts, which constitutes a significant improvement over reconstruction based on a single component (e.g. $B_z$). On the other hand, for magnetisation reconstruction, a single measurement of the out-of-plane field ($B_z$) is generally the best choice, regardless of the magnetisation direction. We verify these findings experimentally using nitrogen-vacancy magnetometry in the case of a 2D current density and a 2D magnet with perpendicular magnetisation.

physics.app-ph↗

arXiv2020

Imaging domain reversal in an ultrathin van der Waals ferromagnet

The recent isolation of two-dimensional van der Waals magnetic materials has uncovered rich physics that often differs from the magnetic behaviour of their bulk counterparts. However, the microscopic details of fundamental processes such as the initial magnetization or domain reversal, which govern the magnetic hysteresis, remain largely unknown in the ultrathin limit. Here we employ a widefield nitrogen-vacancy (NV) microscope to directly image these processes in few-layer flakes of magnetic semiconductor vanadium triiodide (VI$_3$). We observe complete and abrupt switching of most flakes at fields $H_c\approx0.5-1$ T (at 5 K) independent of thickness down to two atomic layers, with no intermediate partially-reversed state. The coercive field decreases as the temperature approaches the Curie temperature ($T_c\approx50$ K), however, the switching remains abrupt. We then image the initial magnetization process, which reveals thickness-dependent domain wall depinning fields well below $H_c$. These results point to ultrathin VI$_3$ being a nucleation-type hard ferromagnet, where the coercive field is set by the anisotropy-limited domain wall nucleation field. This work illustrates the power of widefield NV microscopy to investigate magnetization processes in van der Waals ferromagnets, which could be used to elucidate the origin of the hard ferromagnetic properties of other materials and explore field- and current-driven domain wall dynamics.

cond-mat.mes-hall↗

arXiv2019

Laser modulation of superconductivity in a cryogenic widefield nitrogen-vacancy microscope

Microscopic imaging based on nitrogen-vacancy (NV) centres in diamond, a tool increasingly used for room-temperature studies of condensed matter systems, has recently been extended to cryogenic conditions. However, it remains unclear whether the technique is viable for imaging temperature-sensitive phenomena below 10 K given the inherent laser illumination requirements, especially in a widefield configuration. Here we realise a widefield NV microscope with a field of view of 100 $μ$m and a base temperature of 4 K, and use it to image Abrikosov vortices and transport currents in a superconducting Nb film. We observe the disappearance of vortices upon increase of laser power and their clustering about hot spots upon decrease, indicating that laser powers as low as 1 mW (4 orders of magnitude below the NV saturation) are sufficient to locally quench the superconductivity of the film ($T_c = 9$ K). This significant local heating is confirmed by resistance measurements, which reveal the presence of large temperature gradients (several K) across the film. We then investigate the effect of such gradients on transport currents, where the current path is seen to correlate with the temperature profile even in the fully superconducting phase. In addition to highlighting the role of temperature inhomogeneities in superconductivity phenomena, this work establishes that, under sufficiently low laser power conditions, widefield NV microscopy enables imaging over mesoscopic scales down to 4 K with a submicrometer spatial resolution, providing a new platform for real-space investigations of a range of systems from topological insulators to van der Waals ferromagnets.

cond-mat.supr-con↗