Nitrogen Vacancy Centers In Diamond Nanocrystals Research Articles

Simultaneous Nanorheometry and Nanothermometry Using Intracellular Diamond Quantum Sensors.

The viscoelasticity of the cytoplasm plays a critical role in cell morphology, cell division, and intracellular transport. Viscoelasticity is also interconnected with other biophysical properties, such as temperature, which is known to influence cellular bioenergetics. Probing the connections between intracellular temperature and cytoplasmic viscoelasticity provides an exciting opportunity for the study of biological phenomena, such as metabolism and disease progression. The small length scales and transient nature of changes in these parameters combined with their complex interdependencies pose a challenge for biosensing tools, which are often limited to a single readout modality. Here, we present a dual-mode quantum sensor capable of performing simultaneous nanoscale thermometry and rheometry in dynamic cellular environments. We use nitrogen-vacancy centers in diamond nanocrystals as biocompatible sensors for in vitro measurements. We combine subdiffraction resolution single-particle tracking in a fluidic environment with optically detected magnetic resonance spectroscopy to perform simultaneous sensing of viscoelasticity and temperature. We use our sensor to demonstrate probing of the temperature-dependent viscoelasticity in complex media at the nanoscale. We then investigate the interplay between intracellular forces and the cytoplasmic rheology in live cells. Finally, we identify different rheological regimes and reveal evidence of active trafficking and details of the nanoscale viscoelasticity of the cytoplasm.

Quantum reference beacon-guided superresolution optical focusing in complex media.

Optical scattering is generally considered to be a nuisance of microscopy that limits imaging depth and spatial resolution. Wavefront shaping techniques enable optical imaging at unprecedented depth, but attaining superresolution within complex media remains a challenge. We used a quantum reference beacon (QRB), consisting of solid-state quantum emitters with spin-dependent fluorescence, to provide subwavelength guidestar feedback for wavefront shaping to achieve a superresolution optical focus. We implemented the QRB-guided imaging with nitrogen-vacancy centers in diamond nanocrystals, which enable optical focusing with a subdiffraction resolution below 186 nanometers (less than half the wavelength). QRB-assisted wavefront-shaping should find use in a range of applications, including deep-tissue quantum enhanced sensing and individual optical excitation of magnetically coupled spin ensembles for applications in quantum information processing.

Photophysics of single nitrogen-vacancy centers in diamond nanocrystals

A study of the photophysical properties of nitrogen-vacancy (NV) color centers in diamond nanocrystals of size of 50~nm or below is carried out by means of second-order time-intensity photon correlation and cross-correlation measurements as a function of the excitation power for both pure charge states, neutral and negatively charged, as well as for the photochromic state, where the center switches between both states at any power. A dedicated three-level model implying a shelving level is developed to extract the relevant photophysical parameters coupling all three levels. Our analysis confirms the very existence of the shelving level for the neutral NV center. It is found that it plays a negligible role on the photophysics of this center, whereas it is responsible for an increasing photon bunching behavior of the negative NV center with increasing power. From the photophysical parameters, we infer a quantum efficiency for both centers, showing that it remains close to unity for the neutral center over the entire power range, whereas it drops with increasing power from near unity to approximately 0.5 for the negative center. The photophysics of the photochromic center reveals a rich phenomenology that is to a large extent dominated by that of the negative state, in agreement with the excess charge release of the negative center being much slower than the photon emission process.

Nanometre-scale thermometry in a living cell

Sensitive probing of temperature variations on nanometre scales is an outstanding challenge in many areas of modern science and technology. In particular, a thermometer capable of subdegree temperature resolution over a large range of temperatures as well as integration within a living system could provide a powerful new tool in many areas of biological, physical and chemical research. Possibilities range from the temperature-induced control of gene expression and tumour metabolism to the cell-selective treatment of disease and the study of heat dissipation in integrated circuits. By combining local light-induced heat sources with sensitive nanoscale thermometry, it may also be possible to engineer biological processes at the subcellular level. Here we demonstrate a new approach to nanoscale thermometry that uses coherent manipulation of the electronic spin associated with nitrogen-vacancy colour centres in diamond. Our technique makes it possible to detect temperature variations as small as 1.8 mK (a sensitivity of 9 mK Hz(-1/2)) in an ultrapure bulk diamond sample. Using nitrogen-vacancy centres in diamond nanocrystals (nanodiamonds), we directly measure the local thermal environment on length scales as short as 200 nanometres. Finally, by introducing both nanodiamonds and gold nanoparticles into a single human embryonic fibroblast, we demonstrate temperature-gradient control and mapping at the subcellular level, enabling unique potential applications in life sciences.

Suitability of nanodiamond nitrogen–vacancy centers for spontaneous emission control experiments

Nitrogen–vacancy (NV) centers in diamond are generally recognized as highly promising as indefinitely stable highly efficient single-photon sources. We report an experimental quantification of the brightness, radiative decay rate, nonradiative decay rate and quantum efficiency of single NV centers in diamond nanocrystals. Our experiments show that the commonly observed large spread in fluorescence decay rates of NV centers in nanodiamond is inconsistent with the common explanation of large nanophotonic mode-density variations in the ultra-small high-index crystals at near-unity quantum efficiency. We report that NV centers in 25 nm nanocrystals are essentially insensitive to local density of optical states (LDOS) variations that we induce at a dielectric interface by using liquids to vary the refractive index, and propose that quantum efficiencies in such nanocrystals are widely distributed between 0 and 20%. For single NV centers in larger 100 nm nanocrystals, we show that decay rate changes can be reversibly induced by nanomechanically approaching a mirror to change the LDOS. Using this scanning mirror method, for the first time we report calibrated quantum efficiencies of NV centers, and show that different but nominally identical nanocrystals have widely distributed quantum efficiencies between 10 and 90%. Our measurements imply that nanocrystals that are to be assembled into hybrid photonic structures for cavity QED should first be individually screened to assess fluorescence properties in detail.

Anomalous saturation effects due to optical spin depolarization in nitrogen-vacancy centers in diamond nanocrystals

Pulsed laser excitation causes the luminescence of Nitrogen Vacancy centers in diamond to unexpectedly decrease with increasing pulse energy. This decrease is observed in both the negatively charged and neutral centers and is caused by shortening of the luminescence lifetimes of the centers of both types. In darkness, the luminescence does not show any recovery on a time scale of 10 microseconds but as little as three low-intensity pulses can return the luminescence to its previous, brighter state. An external magnetic field reduces the magnitude of the effect. A possible mechanism for these phenomena based on optical polarisation and depolarisation of an electronic spin is proposed.

Front Cover: Coupling of single nitrogen‐vacancy defect centers in diamond nanocrystals to optical antennas and photonic crystal cavities (Phys. Status Solidi B 5/2012)

Nitrogen-vacancy (NV) centers in diamond are a promising resource for solid state quantum technology. Wolters et al. (pp. 918–924) demonstrate the ability to integrate single NV centers in diamond nanocrystals into photonic or plasmonic hybrids using state of the art scanning probe lithography. Hereby the emission properties of the single NV centers are strongly modified. The authors review experiments concerning the controlled coupling of single defect centers in nanodiamonds to optical nanoantennas made of gold bowtie structures. By placing one and the same emitter at various locations with high precision, a map of decay rate enhancements is obtained. Furthermore, the authors demonstrate the formation of a hybrid cavity quantum electrodynamics (cQED) system in which a single defect center is coupled to a single mode of a gallium phosphite photonic crystal cavity.