Search

Biosensing based on optically trapped fluorescent nanodiamonds is an intriguing research direction potentially allowing to resolve biochemical processes inside living cells. Towards this goal, we investigate infrared near (NIR) laser irradiation at 1064 nm on fluorescent nanodiamonds (FNDs) containing nitrogen-vacancy (NV) centers. By conducting comprehensive experiments, we aim to understand how NIR exposure influences the fluorescence and sensing properties of FNDs and to determine the potential implications for the use of FNDs in various sensing applications. The experimental setup involved exposing FNDs to varying intensities of NIR laser light and analyzing the resultant changes in their optical and physical properties. Key measurements included T1 relaxation times, optical spectroscopy, and optically detected magnetic resonance (ODMR) spectra. The findings reveal how increased NIR laser power correlates with alterations in ODMR central frequency but also that charge state dynamics under NIR irradiation of NV centers plays a role. We suggest protocols with NIR and green light that mitigate the effect of NIR, and demonstrate that FND biosensing works well with such a protocol.

Boron vacancies (VB${^-}$) in hexagonal boron-nitride (hBN) have sparked great interest in recent years, due to their electronic spin properties. Since hBN can be readily integrated into devices where it interfaces a huge variety of other 2D materials, boron vacancies may serve as a precise sensor which can be deployed at very close proximity to many important materials systems. Boron vacancy defects may be produced by a number of existing methods, the use of which may depend on the final application. Any method should reproducibly generate defects with controlled density and desired pattern. To date, however, detailed studies of such methods are missing. In this paper we study various techniques, focused ion beam (FIB), electron irradiation and ion implantation, for the preparation of hBN flakes from bulk crystals, and relevant post-processing treatments to create VB${^-}$s as a function of flake thickness and defect concentrations. We find that flake thickness plays an important role when optimising implantation parameters, while careful sample cleaning proved important to achieve best results.

Magnetic field effects (MFE) in certain chemical reactions have been well established in the last five decades and are attributed to the evolution of transient radical-pairs whose spin dynamics are determined by local and external magnetic fields. The majority of existing experimental techniques used to probe these reactions only provide ensemble averaged reaction parameters and spin chemistry, hindering the observation of the potential presence of quantum coherent phenomena at the single molecule scale. Here, considering a single nitrogen vacancy (NV) centre as quantum sensor, we investigate the prospects and requirements for detection of MFEs on the spin dynamics of radical-pairs at the scale of single and small ensemble of molecules. We employ elaborate and realistic models of radical-pairs, considering its coupling to the local spin environment and the sensor. For two model systems, we derive signals of MFE detectable even in the weak coupling regime between radical-pair and NV quantum sensor, and observe that the dynamics of certain populations, as well as coherence elements, of the density matrix of the radical pair are directly detectable. Our investigations will provide important guidelines for potential detection of spin chemistry of bio-molecules at the single molecule scale, required to witness the hypothesised importance of quantum coherence in biological processes., Comment: 13 pages, 10 figures

Spin-based applications of the negatively charged nitrogen-vacancy (NV) center in diamonds require efficient spin readout. One approach is the spin-to-charge conversion (SCC), relying on mapping the spin states onto the neutral (NV$^0$) and negative (NV$^-$) charge states followed by a subsequent charge readout. With high charge-state stability, SCC enables extended measurement times, increasing precision and minimizing noise in the readout compared to the commonly used fluorescence detection. Nano-scale sensing applications, however, require shallow NV centers within a few $\si{\nano \meter}$ distance from the surface where surface related effects might degrade the NV charge state. In this article, we investigate the charge state initialization and stability of single NV centers implanted $\approx \SI{5}{\nano \meter}$ below the surface of a flat diamond plate. We demonstrate the SCC protocol on four shallow NV centers suitable for nano-scale sensing, obtaining a reduced readout noise of 5--6 times the spin-projection noise limit. We investigate the general applicability of SCC for shallow NV centers and observe a correlation between NV charge-state stability and readout noise. Coating the diamond with glycerol improves both charge initialization and stability. Our results reveal the influence of the surface-related charge environment on the NV charge properties and motivate further investigations to functionalize the diamond surface with glycerol or other materials for charge-state stabilization and efficient spin-state readout of shallow NV centers suitable for nano-scale sensing., Comment: 9 pages, 5 figures

An important tool in the investigation of the early stages of neurodegenerative disease is the study of dissected living tissue from the brain of an animal model. Such investigations allow the physical structure of individual neurons and neural circuits to be probed alongside neuronal electrical activity, disruption of which can shed light on the mechanisms of emergence of disease. Existing techniques for recording activity rely on potentially damaging direct interaction with the sample, either mechanically as point electrical probes or via intense focused laser light combined with highly specific genetic modification and/or potentially toxic fluorescent dyes. In this work, we instead perform passive, microscopic-scale recording of electrical activity using a biocompatible quantum sensor based on colour centres in diamond. We record biomagnetic field induced by ionic currents in mouse corpus callosum axons without direct sample interaction, accurately recovering signals corresponding to action potential propagation while demonstrating in situ pharmacology during biomagnetic recording through tetrodotoxin inhibition of voltage gated sodium channels. Our results open a promising new avenue for the microscopic recording of neuronal signals, offering the prospect of high resolution imaging of electrical circuits in the living mammalian brain.

Optical tweezers are tools made of light that enable contactless pushing, trapping, and manipulation of objects ranging from atoms to space light sails. Since the pioneering work by Arthur Ashkin in the 1970s, optical tweezers have evolved into sophisticated instruments and have been employed in a broad range of applications in life sciences, physics, and engineering. These include accurate force and torque measurement at the femtonewton level, microrheology of complex fluids, single micro- and nanoparticle spectroscopy, single-cell analysis, and statistical-physics experiments. This roadmap provides insights into current investigations involving optical forces and optical tweezers from their theoretical foundations to designs and setups. It also offers perspectives for applications to a wide range of research fields, from biophysics to space exploration., Comment: 181 pages, 61 figures

The detection of physiological activity at the microscopic level is key for understanding the function of biosystems and relating this to physical structure. Current sensing methods often rely on invasive probes to stimulate and detect activity, bearing the risk of inducing damage in the target system. In recent years, a new type of biosensor based on color centers in diamond offers the possibility to passively, noninvasively sense and image living biological systems. Here, we use such a sensor for the \textit{in-vitro} recording of the local magnetic field generated by tightly focused, high intensity pulsed laser optogenetic neuromuscular stimulation of the extensor digitorum longus muscles. Recordings captured a compound action potential response and a slow signal component which we seek to explain using a detailed model of the biological system. We show that our sensor is capable of recording localized neuromuscular activity from the laser stimulation site without photovoltaic or fluorescence artifacts associated with alternative techniques. Our work represents an important step towards selective induction of localized neurobiological activity while performing passive sensing and imaging with diamond sensors, motivating further research into mapping of neural activity and intra-cellular processes.

Ensembles of solid state defects in diamond make promising quantum sensors with high sensitivity and spatiotemporal resolution. The inhomogeneous broadening and drive amplitude variations across such ensembles have differing impacts on the sensitivity depending on the sensing scheme used, adding to the challenge of choosing the optimal sensing scheme for a particular sensing regime. In this work, we numerically investigate and compare the predicted sensitivity of schemes based on continuous-wave (CW) optically detected magnetic resonance (ODMR) spectroscopy, pi-pulse ODMR and Ramsey interferometry for sensing using nitrogen-vacancy centers in the low-frequency (<10 kHz) range typical for signals from biological sources. We show that inhomogeneous broadening has the strongest impact on the sensitivity of Ramsey interferometry, and drive amplitude variations least impact the sensitivity of CW ODMR, with all methods constrained by the Rabi frequency. Based on our results, we can identify three different regions of interest. For inhomogeneous broadening less than 0.3 MHz, typical of diamonds used in state of the art sensing experiments, Ramsey interferometry yields the highest sensitivity. In the regime where inhomogeneous broadening is greater than 0.3 MHz, such as for standard optical grade diamonds or in miniaturized integrated devices, drive amplitude variations determine the optimal protocol to use. For low to medium drive amplitude variations, the highest sensitivity is reached using pi-pulse ODMR. For high drive amplitude variations, relevant for widefield microscopic imaging, CW ODMR can yield the best sensing performance.

The ability to measure the passage of electrical current with high spatial and temporal resolution is vital for applications ranging from inspection of microscopic electronic circuits to biosensing. Being able to image such signals passively and remotely at the same time is of high importance, to measure without invasive disruption of the system under study or the signal itself. A new approach to achieve this utilises point defects in solid state materials, in particular nitrogen vacancy (NV) centres in diamond. Acting as a high density array of independent sensors, addressable opto-electronically and highly sensitive to factors including temperature and magnetic field, these are ideally suited to microscopic widefield imaging. In this work we demonstrate such imaging of signals from a microscopic lithographically patterned circuit at the micrometer scale. Using a new type of lock-in amplifier camera, we demonstrate sub-millisecond (up to 3500 frames-per-second) spatially resolved recovery of AC and pulsed electrical current signals, without aliasing or undersampling. Finally, we demonstrate as a proof of principle the recovery of synthetic signals replicating the exact form of signals in a biological neural network: the hippocampus of a mouse.

Defects in solid state materials provide an ideal, robust platform for quantum sensing. To deliver maximum sensitivity, a large ensemble of non-interacting defects hosting coherent quantum states are required. Control of such an ensemble is challenging due to the spatial variation in both the defect energy levels and in any control field across a macroscopic sample. In this work we experimentally demonstrate that we can overcome these challenges using Floquet theory and optimal control optimization methods to efficiently and coherently control a large defect ensemble, suitable for sensing. We apply our methods experimentally to a spin ensemble of up to 4 $\times$ 10$^9$ nitrogen vacancy (NV) centers in diamond. By considering the physics of the system and explicitly including the hyperfine interaction in the optimization, we design shaped microwave control pulses that can outperform conventional ($\pi$-) pulses when applied to sensing of temperature or magnetic field, with a potential sensitivity improvement between 11 and 78\%. Through dynamical modelling of the behaviour of the ensemble, we shed light on the physical behaviour of the ensemble system and propose new routes for further improvement.

Nitrogen vacancy (NV) centers in diamond have attracted considerable recent interest for use in quantum sensing, promising increased sensitivity for applications ranging from geophysics to biomedicine. Conventional sensing schemes involve monitoring the change in red fluorescence from the NV center under green laser and microwave illumination. Due to the strong fluorescence background from emission in the NV triplet state and low relative contrast of any change in output, sensitivity is severely restricted by a high optical shot noise level. Here, we propose a means to avoid this issue, by using the change in green pump absorption through the diamond as part of a semiconductor external cavity laser run close to lasing threshold. We show theoretical sensitivity to magnetic field on the pT/sqrt(Hz) level is possible using a diamond with an optimal density of NV centers. We discuss the physical requirements and limitations of the method, particularly the role of amplified spontaneous emission near threshold and explore realistic implementations using current technology.

The ability to perform noninvasive, non-contact measurements of electric signals produced by action potentials is essential in biomedicine. A key method to do this is to remotely sense signals by the magnetic field they induce. Existing methods for magnetic field sensing of mammalian tissue, used in techniques such as magnetoencephalography of the brain, require cryogenically cooled superconducting detectors. These have many disadvantages in terms of high cost, flexibility and limited portability as well as poor spatial and temporal resolution. In this work we demonstrate an alternative technique for detecting magnetic fields generated by the current from action potentials in living tissue using nitrogen vacancy centres in diamond. With 50pT/$\sqrt{Hz}$ sensitivity, we show the first measurements of sensing from mammalian tissue with a diamond sensor using mouse muscle optogenetically activated with blue light. We show these measurements can be performed in an ordinary, unshielded lab environment and that the signal can be easily recovered by digital signal processing techniques.

Combining extensive single particle tracking microscopy data of endogenous lipid granules in living fission yeast cells with analytical results we show evidence for anomalous diffusion and weak ergodicity breaking. Namely we demonstrate that at short times the granules perform subdiffusion according to the laws of continuous time random walk theory. The associated violation of ergodicity leads to a characteristic turnover between two scaling regimes of the time averaged mean squared displacement. At longer times the granule motion is consistent with fractional Brownian motion., Comment: 4 pages, 4 figures, REVTeX. Supplementary Material. Physical Review Letters, at press

The first half of this chapter describes the development in mathematical models of Brownian motion after Einstein's seminal papers and current applications to optical tweezers. This instrument of choice among single-molecule biophysicists is also an instrument of precision that requires an understanding of Brownian motion beyond Einstein's. This is illustrated with some applications, current and potential, and it is shown how addition of a controlled forced motion on the nano-scale of the tweezed object's thermal motion can improve the calibration of the instrument in general, and make it possible also in complex surroundings. The second half of the present chapter, starting with Sect. 9, describes the co-evolution of biological motility models with models of Brownian motion, including very recent results for how to derive cell-type-specific motility models from experimental cell trajectories., Comment: 18 pages, 5 figures, to appear in Proceedings of Nobel Symposium 131

In a typical optical tweezers detection system, the position of a trapped object is determined from laser light impinging on a quadrant photodiode. When the laser is infrared and the photodiode is of silicon, they can act together as an unintended low-pass filter. This parasitic effect is due to the high transparency of silicon to near-infrared light. A simple model that accounts for this phenomenon (Berg-Sorensen et al., J. Appl. Phys., 93, 3167-3176 (2003)) is here solved for frequencies up to 100 kHz, and for laser wavelengths between 750 and 1064 nm. The solution is applied to experimental data in the same range, and is demonstrated to give this detection system of optical tweezers a bandwidth, accuracy, and precision that is limited only by the data acquisition board's band-width and bandpass ripples, here 96.7 kHz, resp. 0.005 dB., Comment: 12 pages, 8 figures. Submitted to Review of Scientific Instruments

The TATA-box Binding Protein (TBP) is required by all three eukaryotic RNA polymerases for the initiation of transcription from most promoters. TBP recognizes, binds to, and bends promoter sequences called ``TATA-boxes'' in the DNA. We present results from the study of individual Saccharomyces cerevisia TBPs interacting with single DNA molecules containing a TATA-box. Using video microscopy, we observed the Brownian motion of beads tethered by short surface-bound DNA. When TBP binds to and bends the DNA, the conformation of the DNA changes and the amplitude of Brownian motion of the tethered bead is reduced compared to that of unbent DNA. We detected individual binding and dissociation events and derived kinetic parameters for the process. Dissociation was induced by increasing the salt concentration or by directly pulling on the tethered bead using optical tweezers. In addition to the well-defined free and bound classes of Brownian motion, we observed another two classes of motion. These extra classes were identified with intermediate states on a three-step, linear binding pathway. Biological implications of the intermediate states are discussed., Comment: Accepted for publication in: Biophysical Journal