arXiv subjects

Philipp Reineck

Publications and source records attributed to Philipp Reineck.

At least 19 recordsLinked to original sources

arXiv2026

Characterizing the nitrogen-vacancy center singlet transition and its phonon sideband for absorption-based room-temperature magnetometry

Magnetometry with nitrogen-vacancy (NV) centers in diamond has shown great promise in recent years. In particular, absorption-based magnetometry techniques, employing a cavity to enhance the absorption length, can improve the contrast and sensitivity compared to conventional techniques based on reading out the NV$^-$ triplet fluorescence. The absorption techniques rely on magnetic-field-dependent absorption at the NV$^-$ singlet zero phonon line at 1042$\,$nm and its phonon sideband. In a cavity-enhanced spectroscopy approach, we study pump-laser- and microwave-induced cavity signal changes at room temperature over a spectral range of 680-1050$\,$nm. Through normalization, we eliminate the cavity-enhancement effect and provide quasi-single-pass values for the absorption and optically detected magnetic resonance (ODMR) contrast. The highest contrast is found at 1042$\,$nm, but multiple points of high contrast are found at the peaks of the phonon sideband. Additionally, cavity-enhanced ODMR contrasts in the range of 50-80$\,\%$ are presented. We further measure the broadband singlet absorption cross section at room temperature with a novel method through microwave-induced signal changes. This method is insensitive to pump-laser-induced signal changes by other defects and quantifies the room-temperature absorption strength of the singlet transition and its entire phonon sideband. We determine the absorption cross section at 1042$\,$nm to be $\sigma^{\,\bigstar}_{1042}=(0.89\pm0.14)\cdot 10^{-21}\,\text{m}^2$ or $\sigma^{\,\blacktriangle}_{1042}=(2.9\pm0.5)\cdot 10^{-21}\,\text{m}^2$. depending on the employed 532$\,$nm NV$^-$ absorption cross section.

quant-ph↗

arXiv2026

Ion Concentration and Voltage Imaging with Fluorescent Nanodiamonds

The nitrogen-vacancy (NV) center in diamond exists in different charge states with distinct photoluminescence properties, which are sensitive to the nanoscale electrochemical environment. Hence, the NV charge state is emerging as a powerful all-optical platform for nanoscale sensing and imaging. Although significant progress has been made in engineering near-surface NV centers in bulk diamond, controlling the NV charge state in fluorescent nanodiamonds (FNDs) has proven challenging, limiting the sensitivity and reliability of FND-based charge state sensing. Here, we demonstrate reliable, reversible switching between the fluorescent NV$^0$ and non-fluorescent NV$^+$ charge states in sub-30 nm FNDs via surface oxidation and hydrogenation, respectively, for single particles and particle powder. In aqueous electrochemical cells, we demonstrate voltage and ion concentration imaging based on the NV charge state in self-assembled FND layers on transparent substrates. Applied voltages reliably modulate the FND PL with a sensitivity of up to 16 mV Hz$^{-1/2}$. Importantly, FND PL is also modulated by local changes in salt concentration with a sensitivity of up to 1.8% per millimolar NaCl, enabling all-optical imaging of ion concentration gradients at the microscale. Our results represent a significant step toward realizing fast, stable, and scalable nanoscale charge- and voltage-imaging technologies with sub-micrometer spatial resolution.

cond-mat.mes-hall↗

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

A scalable method for cavity-enhanced solid-state quantum sensors

Photoluminescent color centers in diamond and hexagonal boron nitride (hBN) are powerful nanoscale solid-state quantum sensors that are explored in a plethora of quantum technologies. Methods for integrating them into macroscopic structures that improve their sensitivity and enable their large-scale deployment are highly sought after. Here, we demonstrate cavity-enhanced photoluminescence (PL) of fluorescent nanodiamonds (FNDs) and hBN nanoparticles (NPs) embedded in polymer-based thin-film optical cavities on the centimeter scale. The cavity resonances efficiently modulate the spectral PL peak position of nitrogen-vacancy (NV) centers in FNDs across the NV PL spectrum and lead to an up to 2.9-fold Purcell-enhancement of the NV PL decay rate. The brightness of hBN NPs increases by up to a factor of three and the PL decay rate is enhanced by up to 13-fold inside the cavities. Finally, we find a 4.8 times improved magnetic field sensitivity of 20 nm FNDs in thin-film cavities due to cavity-enhanced optically detected magnetic resonance contrast and PL brightness. Our study demonstrates a low-cost and scalable method for the fabrication of quantum sensor-doped thin-film cavities, which is an important step toward the development of advanced quantum sensing technologies.

physics.optics↗

arXiv2025

The properties of the nitrogen-vacancy center in milled chemical vapor deposition nanodiamonds

Fluorescent nanodiamonds (FNDs) containing negatively charged nitrogen-vacancy (NV-) centers are vital for many emerging quantum sensing applications from magnetometry to intracellular sensing in biology. However, developing a scalable fabrication method for FNDs hosting color centers with consistent bulk-like photoluminescence (PL) and spin coherence properties remains a highly desired but unrealized goal. Here, we investigate optimized ball milling of single-crystal diamonds produced via chemical vapor deposition (CVD) and containing 2 ppm of substitutional nitrogen and 0.3 ppm of NV- to achieve this goal. The NV charge state, PL lifetime, and spin properties of bulk CVD diamond samples are directly compared to milled CVD FNDs and commercial high-pressure high-temperature (HPHT) FNDs. We find that on average, the relative contribution of the NV- charge state to the total NV PL is lower and the NV PL lifetime is longer in CVD FNDs compared to HPHT FNDs, both likely due to the lower Ns0 concentration in CVD FNDs. The CVD bulk and CVD FNDs on average show similar average T1 spin relaxation times of 3.2 $\pm$ 0.7 ms and 4.7 $\pm$ 1.6 ms, respectively, compared to 0.17 $\pm$ 0.01 ms for commercial HPHT FNDs. Our results demonstrate that ball milling of CVD diamonds enables the large-scale fabrication of NV ensembles in FNDs with bulk-like T1 spin relaxation properties.

cond-mat.mes-hall↗

arXiv2025

Self-assembled fluorescent nanodiamond layers for quantum imaging

The nitrogen-vacancy (NV) center in diamond is emerging as a powerful tool for imaging magnetic and electric signals at the microscale and below. However, most imaging demonstrations thus far have relied on costly, millimeter-sized bulk diamond substrates, which cannot be easily scaled or integrated with other materials. Here, we report a scalable method for fabricating NV-containing dense and homogenous fluorescent nanodiamond (FND) layers through electrostatic self-assembly and demonstrate the utility of the FND layers for magnetic imaging. We investigate the effect of FND concentration in suspension, substrate immersion time, and solvent pH on the FND density on the substrate. We identify optimized self-assembly conditions that maximize the FND density while minimizing aggregation. Using FND layers on a quartz substrate, we demonstrate magnetic field and magnetic noise imaging at the microscale, based on NV optically detected magnetic resonance magnetometry and T$_1$ relaxometry, respectively. Our results provide a direction for the development of cost-effective and scalable FND layers and surface coatings. This paves the way for on-demand quantum sensing and imaging on a broad range of surfaces based on NV centers and other diamond quantum emitters.

cond-mat.mes-hall↗

arXiv2025

Nitrogen-vacancy centre formation via local femto-second laser annealing of diamond

Emerging quantum technologies based on the nitrogen-vacancy (NV) centre in diamond require carefully engineered material with controlled defect density, optimised NV formation processes, and minimal crystal strain. The choice of NV generation technique plays a crucial role in determining the quality and performance of these centres. In this work, we investigate NV centre formation in nitrogen-doped diamond using femtosecond (fs) laser processing. We systematically examine the effect of laser pulse energy on NV production and quality using photoluminescence and optically detected magnetic resonance measurements. We also probe the role of pre-existing lattice defects formed by electron irradiation and consider defect evolution over extended dwell times. Finally, we are able to identify a regime where the main action of the fs-laser is to diffuse rather than create vacancies. This local annealing capability expands the toolkit for tailored NV production and presents opportunities for fine tuning defect populations.

cond-mat.mtrl-sci↗

arXiv2025

Robust quantification of the diamond nitrogen-vacancy center charge state via photoluminescence spectroscopy

Nitrogen vacancy (NV) centers in diamond are at the heart of many emerging quantum technologies, all of which require control over the NV charge state. Hence, methods for quantification of the relative photoluminescence (PL) intensities of the NV$^0$ and NV$^-$ charge state, i.e., a charge state ratio, are vital. Several approaches to quantify NV charge state ratios have been reported but are either limited to bulk-like NV diamond samples or yield qualitative results. We propose an NV charge state quantification protocol based on the determination of sample- and experimental setup-specific NV$^0$ and NV$^-$ reference spectra. The approach employs blue (400-470 nm) and green (480-570 nm) excitation to infer pure NV$^0$ and NV$^-$ spectra, which are then used to quantify NV charge state ratios in subsequent experiments via least squares fitting. We test our dual excitation protocol (DEP) for a bulk diamond NV sample, 20 and 100 nm nanodiamond particles and compare results with those obtained via other commonly used techniques such as zero-phonon line fitting and non-negative matrix factorization. We find that DEP can be employed across different samples and experimental setups and yields consistent and quantitative results for NV charge state ratios that are in agreement with our understanding of NV photophysics. By providing robust NV charge state quantification across sample types and measurement platforms, DEP will support the development of NV-based quantum technologies.

cond-mat.mes-hall↗

arXiv2025

All-optical electric field sensing with nanodiamond-doped polymer thin films

The nitrogen-vacancy (NV) center is a photoluminescent defect in diamond that exists in different charge states, NV$^-$ and NV$^0$, that are sensitive to the NV's nanoscale environment. Here, we show that photoluminescence (PL) from NV centers in fluorescent nanodiamonds (FNDs) can be employed for all-optical voltage sensing based on electric field-induced NV charge state modulation. More than 95% of FNDs integrated into a capacitor device show a transient increase in NV$^-$ PL intensity of up to 31% within 0.1 ms after application of an external voltage, accompanied by a simultaneous decrease in NV$^0$ PL. The change in NV$^-$ PL increases with increasing applied voltage from 0 to 100 V, corresponding to an electric field of 0 to 625 kV cm$^ {-1}$ in our devices. The electric field sensitivity of a single FND is 19 V cm$^{-1}$ Hz$^ {-1/2}$. We investigate the NV charge state photodynamics on the millisecond timescale and find that the change in NV PL strongly depends on the rate of photoexcitation. We propose a model that qualitatively explains the observed changes in NV PL based on an electric field-induced redistribution of photoexcited electrons from substitutional nitrogen defects to NV centers, leading to a transient conversion of NV$^0$ to NV$^-$ centers upon application of an external voltage. Our results contribute to the development of FNDs as reliable, all-optical, nanoscale electric field sensors in solid-state systems.

cond-mat.mes-hall↗

arXiv2025

Magnetic field imaging with an optical microscope using a quantum diamond sensor add-on

Widefield magnetic imaging using ensembles of nitrogen-vacancy (NV) centres in diamond has emerged as a useful technique for studying the microscopic magnetic properties of materials. Thus far, this technique has mainly been implemented on custom-made optical microscopes. We have developed an add-on for a standard laboratory optical microscope that integrates the NV-diamond sensor and necessary light source, microwave antenna, and bias magnet, enabling NV-based magnetic imaging while retaining the typical optical measurements modes of the microscope. We demonstrate our retrofitted quantum diamond microscope by imaging a magnetic particle sample using brightfield, darkfield, and magnetic imaging modes. Furthermore, we employ an iso-magnetic field imaging technique to visualise the magnetic field of the sample within seconds, and finally demonstrate three-dimensional stray field imaging. Retrofitting existing microscopes exploits the stability and high quality of traditional optical microscope systems while reducing the cost and space requirements of establishing a standalone magnetic imaging system.

cond-mat.mtrl-sci↗

arXiv2024

The $N_2V$ color center: a ubiquitous visible and near-infrared-II quantum emitter in nitrogen-doped diamond

Photoluminescent defects in diamond, like the nitrogen-vacancy (NV) color center, are at the forefront of emerging optical quantum technologies. Most emit in the visible and near-infrared spectral region below 1000 nm (NIR-I), limiting their applications in photonics, fiber communications, and biology. Here, we show that the nitrogen-vacancy-nitrogen ($N_2V$) center, which emits in the visible and near-infrared-II (NIR-II, 1000-1700 nm), is ubiquitous in as-synthesized and processed nitrogen-doped diamond from bulk samples to nanoparticles. We demonstrate that $N_2V$ is also present in commercially available state-of-the-art NV diamond sensing chips made via chemical vapor deposition (CVD). In high-pressure high-temperature (HPHT) diamonds, the photoluminescence (PL) intensity of both $N_2V$ charge states, $N_2V^0$ in the visible and $N_2V^-$ in the NIR-II, increases with increasing substitutional nitrogen concentration. We determine the PL lifetime of $N_2V^-$ to be 0.3 ns and compare a quantum optical and density functional theory model of the $N_2V^-$ with experimental PL spectra. Finally, we show that detonation nanodiamonds (DND) show stable PL in the NIR-II, which we attribute to the $N_2V$ color center, and use this NIR-II PL to image DNDs inside skin cells. Our results will contribute to the scientific and technological exploration and development of the $N_2V$ color center and inspire more research into its effect on other color centers in diamond.

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

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

A compact, portable device for microscopic magnetic imaging based on diamond quantum sensors

Magnetic imaging based on ensembles of diamond nitrogen-vacancy quantum sensors has emerged as a useful technique for the spatial characterisation of magnetic materials and current distributions. However, demonstrations have so far been restricted to laboratory-based experiments using relatively bulky apparatus and requiring manual handling of the diamond sensing element, hampering broader adoption of the technique. Here we present a simple, compact device that can be deployed outside a laboratory environment and enables robust, simplified operation. It relies on a specially designed sensor head that directly integrates the diamond sensor while incorporating a microwave antenna and all necessary optical components. This integrated sensor head is complemented by a small control unit and a laptop computer that displays the resulting magnetic image. We test the device by imaging a magnetic sample, demonstrating a spatial resolution of 4 $\mu$m over a field of view exceeding 1 mm, and a best sensitivity of 45 $\mu$T/$\sqrt{\rm Hz}$ per ($5\,\mu$m)$^2$ pixel. Our portable magnetic imaging instrument may find use in situations where taking the sample to be measured to a specialist lab is impractical or undesirable.

cond-mat.mtrl-sci↗

arXiv2024

Optimisation of electron irradiation for creating spin ensembles in hexagonal boron nitride

Boron vacancy centre ($V_{\rm B}^-$) ensembles in hexagonal boron nitride (hBN) have attracted recent interest for their potential as two-dimensional solid-state quantum sensors. Irradiation is necessary for $V_{\rm B}^-$ creation, however, to date only limited attention has been given to optimising the defect production process, especially in the case of bulk irradiation with high-energy particles, which offers scalability through the potential for creating ensembles in large volumes of material. Here we systematically investigate the effect of electron irradiation by varying the dose delivered to a range of hBN samples, which differ in their purity, and search for an optimum in measurement sensitivity. We find that moderate electron irradiation doses ($\approx 5\times 10^{18}$~cm$^{-2}$) appear to offer the best sensitivity, and also observe a dependence on the initial crystal purity. These results pave the way for the scalable and cost-effective production of hBN quantum sensors, and provide insight into the mechanisms limiting $V_{\rm B}^-$ spin properties.

cond-mat.mes-hall↗

arXiv2024

Extending the self-discharge time of Dicke quantum batteries using molecular triplets

Quantum batteries, quantum systems for energy storage, have gained interest due to their potential scalable charging power density. A quantum battery proposal based on the Dicke model has been explored using organic microcavities, which enable a cavity-enhanced energy transfer process called superabsorption. However, energy storage lifetime in these devices is limited by fast radiative emission losses, worsened by superradiance. Here, we demonstrate a promising approach to extend the energy storage lifetime of Dicke quantum batteries using molecular triplet states. We examine a type of multi-layer microcavities where an active absorption layer transfers energy to the molecular triplets of a storage layer, identifying two regimes based on exciton-polariton resonances. We tested one of these mechanisms by fabricating and characterising five devices across a triplet-polariton resonance. We conclude by discussing potential optimisation outlooks for this class of devices.

quant-ph↗

arXiv2023

The Acoustophotoelectric Effect: Efficient Phonon-Photon-Electron Coupling in Zero-Voltage-Biased 2D SnS$_2$ for Broadband Photodetection

Two-dimensional (2D) layered metal dichalcogenides constitute a promising class of materials for photodetector applications due to their excellent optoelectronic properties. The most common photodetectors, which work on the principle of photoconductive or photovoltaic effects, however, require either the application of external voltage biases or built-in electric fields, which makes it challenging to simultaneously achieve high responsivities across broadband wavelength excitation - especially beyond the material's nominal band gap - while producing low dark currents. In this work, we report the discovery of an intricate phonon-photon-electron coupling - which we term the acoustophotoelectric effect - in SnS$_2$ that facilitates efficient photodetection through the application of 100-MHz-order propagating surface acoustic waves (SAWs). This effect not only reduces the band gap of SnS$_2$, but also provides the requisite momentum for indirect band gap transition of the photoexcited charge carriers, to enable broadband photodetection beyond the visible light range, whilst maintaining pA-order dark currents - remarkably without the need for any external voltage bias. More specifically, we show in the infrared excitation range that it is possible to achieve up to eight orders of magnitude improvement in the material's photoresponsivity compared to that previously reported for SnS$_2$-based photodetectors, in addition to exhibiting superior performance compared to most other 2D materials reported to date for photodetection.

physics.app-ph↗