We report the experimental study of the temperature-dependence of the longitudinal spin relaxation time $T_1$ of single Nitrogen-Vacancy (NV) centers hosted in nanodiamonds. To determine the relaxation mechanisms at stake, measurements of the $T_1$ relaxation time are performed for a set of individual NV centers both at room and cryogenic temperatures. The results are consistant with a temperature-dependent relaxation process which is attributed to a thermally-activated magnetic noise produced by paramagnetic impurities lying on the nanodiamond surface. These results confirm the existence of surface-induced spin relaxation processes occurring in nanodiamonds, which are relevant for future developments of sensitive nanoscale NV-based quantum sensors.
Thanks to their versatility, nitrogen-vacancy (NV) centers in nanodiamonds have been widely adopted as nanoscale sensors. However, their sensitivities are limited by their short coherence times relative to NVs in bulk diamond. A more complete understanding of the origins of decoherence in nanodiamonds is critical to improving their performance. Here we present measurements of fast spin relaxation on qutrit transitions between the energy eigenstates composed of the $m_s = \pm1$ states of the NV$^-$ electronic ground state in $\sim40$-nm nanodiamonds under ambient conditions. For frequency split…
The widespread use of nanodiamond as a biomedical platform for drug-delivery, imaging, and sub-cellular tracking applications stems from their non-toxicity and unique quantum mechanical properties. Here, we extend this functionality to the domain of magnetic resonance, by demonstrating that the intrinsic electron spins on the nanodiamond surface can be used to hyperpolarize adsorbed liquid compounds at room temperature. By combining relaxation measurements with hyperpolarization, spins on the surface of the nanodiamond can be distinguished from those in the bulk liquid. These results are likel…
Optically active color centers in nanodiamonds offer unique opportunities for generating and manipulating quantum states of light. These mechanically, chemically, and optically robust emitters can be produced in mass quantities, deterministically manipulated, and integrated with a variety of quantum device geometries and photonic material platforms. Nanodiamonds with deeply sub-wavelength sizes coupled to nanophotonic structures feature a giant enhancement of light-matter interaction, promising high bitrates in quantum photonic systems. We review the recent advances in controlled techniques fo…
We demonstrate cooling of ultrathin fiber tapers coupled with nitrogen vacancy (NV) centers in nanodiamonds to cryogenic temperatures. Nanodiamonds containing multiple NV centers are deposited on the subwavelength 480-nm-diameter nanofiber region of fiber tapers. The fiber tapers are successfully cooled to 9 K using our home-built mounting holder and an optimized cooling speed. The fluorescence from the nanodiamond NV centers is efficiently channeled into a single guided mode and shows characteristic sharp zero-phonon lines of both neutral and negatively charged NV centers. The present nanofib…
Nanodiamonds (NDs) hosting nitrogen-vacancy (NV) centers are promising for applications of quantum sensing. Long spin relaxation times ($T_1$ and $T_2$) are critical for high sensitivity in quantum applications. It has been shown that fluctuations of magnetic fields due to surface spins strongly influences $T_1$ and $T_2$ in NDs. However, their relaxation mechanisms have yet to be fully understood. In this paper, we investigate the relation between surface spins and $T_1$ and $T_2$ of single-substitutional nitrogen impurity (P1) centers in NDs. The P1 centers located typically in the vicinity …
Silicon vacancy (SiV) centers in diamonds have emerged as a very promising candidate for quantum emitter due to their narrow emission line resulting in their indistinguishability. While many different quantum emitters have already been used for excitation of various propagating plasmonic modes, the corresponding exploitation of SiV centers remained so far uncharted territory. Here, we report on excitation of surface plasmon modes supported by silver nanowires using SiV centers in nanodiamonds. The coupling of SiV center fluorescence to surface plasmons is observed, when a nanodiamond situated …
Nanodiamonds containing color centers open up many applications in quantum information processing, metrology, and quantum sensing. In particular, silicon vacancy (SiV) centers are prominent candidates as quantum emitters due to their beneficial optical qualities. Here we characterize nanodiamonds produced by a high-pressure high-temperature method without catalyst metals, focusing on two samples with clear SiV signatures. Different growth temperatures and relative content of silicon in the initial compound between the samples altered their nanodiamond size distributions and abundance of SiV ce…
We have characterized thermal susceptibilities of the spectral band at 740 nm of silicon-vacancy (SiV) centers in Si- and Si,P-doped nanodiamonds over a temperature range from 295 K to 350 K, which is of interest for thermometry in biological systems. Si-doped crystals reveal linear dependence of the SiV zero-phonon line position, width and relative amplitude with susceptibilities of 0.0126(4) nm/K, 0.062(2) nm/K and $-0.037(2)$ K$^{-1}$, respectively. Si,P-doped nanodiamonds show significantly smaller (up to 35 % for the width) susceptibilities and prove control of SiV properties with additio…
Nanodiamonds containing nitrogen vacancy (NV-) centers show promise for a number of emerging applications including targeted in vivo imaging and generating nuclear spin hyperpolarization for enhanced NMR spectroscopy and imaging. Here, we develop a detailed understanding of the magnetic resonance behavior of NV- centers in an ensemble of nanodiamonds with random crystal orientations. Two-dimensional optically detected magnetic resonance spectroscopy reveals the distribution of energy levels, spin populations, and transition probabilities that give rise to a complex spectrum. We identify overto…
Long Spin Relaxation Times in CVD-Grown Nanodiamonds
Hasselt University（哈瑟尔特大学）；Institute for Materials Research (IMO), Hasselt University（哈瑟尔特大学材料研究所）；Institute of Organic Chemistry and Biochemistry of the CAS（捷克科学院有机化学与生物化学研究所）
We discuss the progress in integration of nanodiamonds with photonic devices for quantum optics applications. Experimental results in GaP, SiO2 and SiC-nanodiamond platforms show that various regimes of light and matter interaction can be achieved by engineering color center systems through hybrid approaches. We present our recent results on the growth of color center-rich nanodiamond on prefabricated 3C-SiC microdisk resonators. These hybrid devices achieve up to five-fold enhancement of diamond color center light emission and can be employed for integrated quantum photonics.
Size-calibrated commercial nanodiamonds synthesized by high-pressure high-temperature (HPHT) technique were studied by high-frequency W and conventional X band electron paramagnetic resonance (EPR) spectroscopy. The numbers of spins in the studied samples were estimated. The core-shell model of the HPHT nanodiamonds was proposed to explain the observed dependence of the concentration of the N0 paramagnetic centers. Two other observed paramagnetic centers are attributed to the two types of structures in the nanodiamond shell.
Nanodiamonds containing nitrogen-vacancy (NV) centers offer a versatile platform for sensing applications spanning from nanomagnetism to in-vivo monitoring of cellular processes. In many cases, however, weak optical signals and poor contrast demand long acquisition times that prevent the measurement of environmental dynamics. Here, we demonstrate the ability to perform fast, high-contrast optical measurements of charge distributions in ensembles of NV centers in nanodiamonds and use the technique to improve the spin readout signal-to-noise ratio through spin-to-charge conversion. A study of 38…
Electron spins of diamond nitrogen-vacancy (NV) centers are important quantum resources for nanoscale sensing and quantum information. Combining NV spins with levitated optomechanical resonators will provide a hybrid quantum system for novel applications. Here we optically levitate a nanodiamond and demonstrate electron spin control of its built-in NV centers in low vacuum. We observe that the strength of electron spin resonance (ESR) is enhanced when the air pressure is reduced. To better understand this system, we investigate the effects of trap power and measure the absolute internal temper…
The silicon-vacancy (SiV) color center in diamond is a solid-state single photon emitter and spin quantum bit suited as a component in quantum devices. Here, we show that the SiV center in nanodiamond exhibits a strongly inhomogeneous distribution with regard to the center wavelengths and linewidths of the zero-phonon-line (ZPL) emission at room temperature. We find that the SiV centers separate in two clusters: one group exhibits ZPLs with center wavelengths within a narrow range of approximatly 730 nm to 742 nm and broad linewidths between 5 nm and 17 nm, whereas the second group comprises a…
We report on sensing stability of nanodiamond (ND) quantum sensors in various pH aqueous buffer solutions for the two detection schemes of quantum decoherence spectroscopy and thermometry. The electron spin properties of single nitrogen-vacancy (NV) centers in 25-nm-sized NDs have been characterized by a spin-measurement compatible perfusion (SMCP) chamber where observing the same individual NDs in different buffer solutions is possible. With this system, we have determined the stability of the NV quantum sensors during the pH change from 4 to 11 as the fluctuations of +- 12% and +- 0.2 MHz fo…
The nitrogen vacancy center in diamond in its negative charge state is a promising candidate for quantum optic experiments that require single photon emitters. Important benefits of the NV center are its high brightness and photo-stability, even at room temperature. Engineering the emission properties of NV centers with optical resonators is a widely followed approach to meet the requirements for quantum technological applications, but the effect on non-radiative decay paths is yet to be understood. Here we report on modifying the internal quantum efficiency of a single NV center in a nanodiam…
Coherent quantum systems are a key resource for emerging quantum technology. Solid-state spin systems are of particular importance for compact and scalable devices. However, interaction with the solid-state host degrades the coherence properties. The negatively-charged silicon vacancy center in diamond is such an example. While spectral properties are outstanding, with optical coherence protected by the defects symmetry, the spin coherence is susceptible to rapid orbital relaxation limiting the spin dephasing time. A prolongation of the orbital relaxation time is therefore of utmost urgency an…
Ensembles of negatively charged nitrogen vacancy centers (NV-) in diamond have been proposed for sensing of magnetic fields and paramagnetic agents, and as a source of spin-order for the hyperpolarization of nuclei in magnetic resonance applications. To this end, strongly fluorescent nanodiamonds represent promising materials, with large surface areas and dense ensembles of NV-. However, surface effects tend to favor the less useful neutral form, the NV0 centers. Here, we study the fluorescence properties and optically detected magnetic resonance (ODMR) of NV- centers as a function of laser po…
We present an optimized scheme for nanoscale measurements of temperature in a complex environment using the nitrogen-vacancy center in nanodiamonds. To this end we combine a Ramsey measurement utilized to temperature determination with advanced optimal control theory. We test our new design on single nitrogen-vacancy centers in bulk diamond and fixed nanodiamonds, achieving better readout signal than with common soft or hard microwave control pulses. We demonstrate temperature readout using rotating nanodiamonds in an agarose matrix. Our method opens the way to measure temperature fluctuations…
Nitrogen-vacancy centers in diamond allow for coherent spin state manipulation at room temperature, which could bring dramatic advances to nanoscale sensing and quantum information technology. We introduce a novel method for the optical measurement of the spin contrast in dense nitrogen-vacancy (NV) ensembles. This method brings a new insight into the interplay between the spin contrast and fluorescence lifetime. We show that for improving the spin readout sensitivity in NV ensembles, one should aim at modifying the far field radiation pattern rather than enhancing the emission rate.
The nitrogen-vacancy (NV) center in diamond has been recognized as a high-sensitivity nanometer-scale metrology platform. Thermometry has been a recent focus, with attention largely confined to room temperature applications. Thermometry has been a recent focus, with attention largely confined to room temperature applications. Temperature sensing at low temperatures, however, remains challenging as the sensitivity decreases for many commonly used techniques which rely on a temperature dependent frequency shift of the NV centers spin resonance and its control with microwaves. Here we use an alte…
We report on the isolation of single SiV$^-$ centers in nanodiamonds. We observe the fine-structure of single SiV$^-$ center with improved inhomogeneous ensemble linewidth below the excited state splitting, stable optical transitions, good polarization contrast and excellent spectral stability under resonant excitation. Based on our experimental results we elaborate an analytical strain model where we extract the ratio between strain coefficients of excited and ground states as well the intrinsic zero-strain spin-orbit splittings. The observed strain values are as low as best values in low-str…
Monolithic integration of quantum emitters in nanoscale plasmonic circuitry requires low-loss plasmonic configurations capable of confining light well below the diffraction limit. We demonstrate on-chip remote excitation of nanodiamond-embedded single quantum emitters by plasmonic modes of dielectric ridges atop colloidal silver crystals. The nanodiamonds are produced to incorporate single germanium-vacancy (GeV) centers, providing bright, spectrally narrow and stable single-photon sources suitable for highly integrated circuits. Using electron-beam lithography with hydrogen silsesquioxane (HS…
Fluorescent nanodiamonds (NDs) are crystal defect-based light-emitting nanoparticles that can be applied to quantum information science and quantum sensing. Of particular interest are nitrogen vacancy (NV) centers that allow optical access to their coherently controllable electron spin systems, leading to spin-photon quantum devices and nanoscale sensing of various physical parameters. However, the NV spin coherence time (T2) in NDs has been limited to one or two orders of magnitude shorter than those in bulk diamonds owing to the complicated surface effect that decoheres the NV spin systems. …
Powered by the mutual developments in instrumentation, materials andtheoretical descriptions, sensing and imaging capabilities of quantum emitters insolids have significantly increased in the past two decades. Quantum emitters insolids, whose properties resemble those of atoms and ions, provide alternative waysto probing natural and artificial nanoscopic systems with minimum disturbance andultimate spatial resolution. Among those emerging quantum emitters, the nitrogen-vacancy (NV) color center in diamond is an outstanding example due to its intrinsicproperties at room temperature (highly-lumi…
Self-assembled fluorescent nanodiamond layers for quantum imaging
School of Science, RMIT University（RMIT大学理学院）；National Institutes for Quantum and Radiological Science and Technology（量子辐射科学技术研究院）；Department of Materials Science, Tohoku University（东北大学材料科学系）
Nanodiamond (ND) hosting nitrogen-vacancy (NV) centers is a promising platform for quantum sensing applications. Sensitivity of the applications using NV centers in NDs is often limited due to presence of paramagnetic impurity contents near the ND surface. Here, we investigate near-surface paramagnetic impurities in NDs. Using high-frequency (HF) electron paramagnetic resonance spectroscopy, the near-surface paramagnetic impurity within the shell of NDs is probed and its g-value is determined to be 2.0028(3). Furthermore, HF electron-electron double resonance-detected nuclear magnetic resonanc…
Sensing of a few unpaired electron spins, such as metal ions and radicals, is a useful but difficult task in nanoscale physics, biology, and chemistry. Single nitrogen-vacancy (NV) centers in diamond offer high sensitivity and spatial resolution in the optical detection of weak magnetic fields produced by a spin bath, but often require long acquisition times, of the order of seconds. Here we use a novel approach, based on coupled spin and charge dynamics in dense NV ensembles in strongly fluorescent nanodiamonds (NDs) to sense external magnetic dipoles. We apply this approach to various parama…
Nitrogen-vacancy (NV) centers in diamonds are interesting due to their remarkable characteristics that are well suited to applications in quantum-information processing and magnetic field sensing, as well as representing stable fluorescent sources. Multiple NV centers in nanodiamonds (NDs) are especially useful as biological fluorophores due to their chemical neutrality, brightness and room-temperature photostability. Furthermore, NDs containing multiple NV centers also have potential in high-precision magnetic field and temperature sensing. Coupling NV centers to propagating surface plasmon p…
Amorphous solids, which show characteristic differences from crystals, are common in daily usage. Glasses, gels, and polymers are familiar examples, and polymers are particularly important in terms of their role in construction and crafting. Previous studies have mainly focused on the bulk properties of polymeric products, and the local properties are less discussed. Here, we designed a distinctive protocol using the negatively charged nitrogen vacancy center in nanodiamond to study properties inside polymeric products in situ. Choosing the curing of poly dimethylsiloxane and the polymerizatio…
The sensing capability of a single optically bright electronic spin in diamond can be enhanced by making use of proximal dark nuclei as ancillary spins. Such systems, so far only realized in bulk diamond, provide orders of magnitude higher sensitivity and spectral resolution in the case of magnetic sensing, as well as improved readout fidelity and state storage time in quantum information schemes. In nanodiamonds, which offer additional opportunities as mobile nanoscale sensors, electronic-nuclear spin complexes have remained inaccessible. We demonstrate coherent control of a 13C nuclear spin …
Towards Application of Nanodiamonds for in-situ Monitoring of Radicals in Liquid Phase Chemical Reactions
RPTU University（莱布尼茨技术大学）；State Research Center OPTIMAS, RPTU University（OPTIMAS州立研究中心，莱布尼茨技术大学）；Kiel University（基尔大学）；Kiel Nano, Surface and Interface Science (KiNSIS), Kiel University（基尔纳米、表面与界面科学研究所（KiNSIS），基尔大学）
The nitrogen-vacancy (NV) center in diamond has been extensively studied in recent years for its remarkable quantum coherence properties that make it an ideal candidate for room temperature quantum computing and quantum sensing schemes. However, these schemes rely on spin-spin dipolar interactions, which require the NV centers to be within a few nanometers from each other while still separately addressable, or to be in close proximity of the diamond surface, where their coherence properties significantly degrade. Here we demonstrate a method for overcoming these limitations using a hybrid yttr…
Two novel properties, unique for semiconductors: a negative electron affinity [1-2], and a high p-type surface electrical conductivity [3-4], were discovered in diamond at the end of the last century. Both properties appear when the diamond surface is hydrogenated. A natural question arises: is the influence of the surface hydrogen on diamond limited only to the electrical properties? Here, we report the first observation of a transparency peak at 1328 cm-1 in IR absorption of hydrogen-terminated pure (undoped) nanodiamonds. This new optical property is ascribed to Fano-type destructive interf…
Surface-functionalized nanomaterials can act as theranostic agents that detect disease and track biological processes using hyperpolarized magnetic resonance imaging (MRI). Candidate materials are sparse however, requiring spinful nuclei with long spin-lattice relaxation (T1) and spin-dephasing times (T2), together with a reservoir of electrons to impart hyperpolarization. Here, we demonstrate the versatility of the nanodiamond material system for hyperpolarized 13C MRI, making use of its intrinsic paramagnetic defect centers, hours-long nuclear T1 times, and T2 times suitable for spatially re…
Single photon emitters with narrow linewidths are highly sought after for applications in quantum information processing and quantum communications. In this letter, we report on a bright, highly polarized near infrared single photon emitter embedded in diamond nanocrystals with a narrow, sub GHz optical linewidths at 10K. The observed zero phonon line at ~ 780 nm is optically stable under low power resonant excitation and blue shifts as the excitation power increases. Our results highlight the prospect for using new near infrared color centers in nanodiamonds for quantum applications.
