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Nanophotonics

NV‐plasmonics: modifying optical emission of an NV − center via plasmonic metal nanoparticles

Harini Hapuarachchi, Francesco Campaioli, Jared H. Cole

Published Oct 19, 2022• 16 citations
Publisher

Abstract

The nitrogen-vacancy (NV) center in diamond is very sensitive to magnetic and electric fields, strain, and temperature. In addition, it is possible to optically interrogate individual defects, making it an ideal quantum-limited sensor with nanoscale resolution. A key limitation for the application of NV sensing is the optical brightness and collection efficiency of these defects. Plasmonic resonances of metal nanoparticles have been used in a variety of applications to increase the brightness and efficiency of quantum emitters, and therefore are a promising tool to improve NV sensing. However, the interaction between NV centers and plasmonic structures is largely unexplored. In particular, the back-action between NV and plasmonic nanoparticles is nonlinear and depends on optical wavelength, nanoparticle position, and metal type. Here we present the general theory of NV-plasmonic nanoparticle interactions. We detail how the interplay between NV response, including optical and vibrational signatures, and the plasmonic response of the metal nanoparticle results in modifications to the emission spectra. Our model is able to explain quantitatively the existing experimental measurements of NV centers near metal nanoparticles. In addition, it provides a pathway to developing new plasmonic structures to improve readout efficiencies in a range of applications for the NV center. This will enable higher precision sensors, with greater bandwidth as well as new readout modalities for quantum computing and communication.

DOI
10.1515/nanoph-2022-0429

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The nitrogen-vacancy (NV) center in diamond is very sensitive to magnetic and electric fields, strain, and temperature. In addition, it is possible to optically interrogate individual defects, making it an ideal quantum-limited sensor with nanoscale resolution. A key limitation for the application of NV sensing is the optical brightness and collection efficiency of these defects. Plasmonic resonances of metal nanoparticles have been used in a variety of applications to increase the brightness and efficiency of quantum emitters, and therefore are a promising tool to improve NV sensing. However, the interaction between NV centers and plasmonic structures is largely unexplored. In particular, the back-action between NV and plasmonic nanoparticles is nonlinear and depends on optical wavelength, nanoparticle position, and metal type. Here we present the general theory of NV-plasmonic nanoparticle interactions. We detail how the interplay between NV response, including optical and vibrational signatures, and the plasmonic response of the metal nanoparticle results in modifications to the emission spectra. Our model is able to explain quantitatively the existing experimental measurements of NV centers near metal nanoparticles. In addition, it provides a pathway to developing new plasmonic structures to improve readout efficiencies in a range of applications for the NV center. This will enable higher precision sensors, with greater bandwidth as well as new readout modalities for quantum computing and communication.
A method for enhancement of the sensitivity of a spin sensor based on an ensemble of nitrogen vacancy (NV) color centers was demonstrated. Gold nanoparticles (NPs) were deposited on the bulk diamond, which had NV centers distributed on its surface. The experimental results demonstrate that, when using this simple method, plasmon enhancement of the deposited gold NPs produces an improvement of ∼10 times in the quantum efficiency and has also improved the signal-to-noise ratio by approximately ∼2.5 times. It was also shown that more electrons participated in the spin sensing process, leading to an improvement in the sensitivity of approximately seven times; this has been proved by Rabi oscillation and optical detection of magnetic resonance (ODMR) measurements. The proposed method has proved to be a more efficient way to design an ensemble of NV centers-based sensors; because the result increases in the number of NV centers, the quantum efficiency and the contrast ratio could greatly increase the device's sensitivity.
The NV defect center in diamond forms a pseudo-atomic quantum system with discreet optically excitable transitions between ground and excited states in the gap between valence and conduction bands, making the NV center a deep-level defect center in diamond. For the negatively charged NV center (NV-), both the ground and excited states are spin triplets (S=1) and coupling between optical and spin states provides unique opportunities for optical detection of magnetic resonance (ODMR) and quantum metrology under ambient conditions. As an atomically sized point defect that is stable in single nanodiamonds as small as a few nanometers, the NV center enables spin based imaging of temperature, electric fields, magnetic fields and mechanical strain with nanoscale spatial resolution. Made of carbon, nanodiamonds are also ideal nanoparticles for use in biological systems, exhibiting extremely low cytotoxicity, no photo bleaching and exceptional contrast in transmission electron and light microscopy. With the ability to act as both a passive, non perturbing sensor (e.g. a diamagnetic material used for sensing magnetic fields) and a connection point for two way, direct coupling of far field optics to NV−^-− spins and indirectly to the highly localized neighborhood of atoms, electronic states and phonon modes in the local vicinity, NV diamond provides a route to nanoscale field sensing and spin based optical microscopy. These sensors are also stable in nanodiamonds. For nanoparticles, the reduction in particle diameter dramatically enhances the proportion of the material that is surface exposed, enhancing any surface related properties. Nitrogen Vacancy centers in nanodiamonds provide another example of material properties that vary with particle size. In chapter 5, evidence that modulation of nanodiamonds fluorescent emissions by electrical perturbations in their surrouding environment allows transduction of local electrodynamics into a far field optical signal capable of mapping action potentials in cardiomyocytes in presented. The unifying theme for all of the work presented in this dissertation is to enable the use of magnetic resonance signals and interactions for imaging and sensing in previously inaccessible regimes. The specific focus is on methods and techniques to enable nanoscale physical sensing and functional imaging in live tissues, with the ultimate aim to lay the predicate for the combination of both without compromise.
The nitrogen-vacancy (NV) center is a point defect in diamond and has been championed as a promising solid-state "artificial atom." NV center properties such as its bright luminescence, room-temperature optical readout of spin states, and long spin decoherence lifetime make it an excellent system for applications in quantum information processing, high sensitivity magnetometry, and biotagging. In all applications, near-surface NVs are desirable. However, it has been found that the favorable properties of the NV center are significantly diminished as the NV center nears the surface. \nThis dissertation presents efforts in understanding the effect of the surface on the luminescence of NV centers less than a wavelength of light from the surface. We use plasma assisted etching to, independently, change the surface termination and bring the NV closer to the surface. We find that treating the surface with CF4 plasma results in a deposited polymerous fluorocarbon which helps stabilize nearby NVs. We propose using a downstream etcher to bring NVs closer to the surface, while minimizing damage and maintaining NV luminescence. Finally, we enhance emission of these near-surface NVs by coupling them into a hybrid diamond plasmonic cavity. The fabricated devices result in a measured Q of 170, higher than other previously fabricated diamond plasmonic devices.
In modern-day quantum metrology, quantum sensors are widely employed to detect weak magnetic fields or nanoscale signals. Quantum devices, exploiting quantum coherence, are inevitably connected to physical constants and can achieve accuracy, repeatability, and precision approaching fundamental limits. As a result, these sensors have shown utility in a wide range of research domains spanning both science and technology. A rapidly emerging quantum sensing platform employs atomic-scale defects in crystals. In particular, magnetometry using nitrogen-vacancy (NV) color centers in diamond has garnered increasing interest. NV systems possess a combination of remarkable properties, optical addressability, long coherence times, and biocompatibility. Sensors based on NV centers excel in spatial resolution and magnetic sensitivity. These diamond-based sensors promise comparable combination of high spatial resolution and magnetic sensitivity without cryogenic operation. The above properties of NV magnetometers promise increasingly integrated quantum measurement technology, as a result, they have been extensively developed with various protocols and find use in numerous applications spanning materials characterization, nuclear magnetic resonance (NMR), condensed matter physics, paleomagnetism, neuroscience and living systems biology, and industrial vector magnetometry. In this chapter, NV centers are explored for magnetic sensing in a number of contexts. In general, we introduce novel regimes for magnetic-field probes with NV ensembles. Specifically, NV centers are developed for sensitive magnetometers for applications where microwaves (MWs) are prohibitively invasive and operations need to be carried out under zero ambient magnetic field. The primary goal of our discussion is to improve the utility of these NV center-based magnetometers.
Nitrogen-vacancy centers in diamond have been long used for spin-based optical sensing and also considered viable candidates for implementing quantum information protocols using their spin degree of freedom. Their nanoscale size and the possibility of optical spin readout make them particularly attractive for the use in integrated nanophotonic and quantum optical devices. We will discuss how the optical Purcell effect in plasmonic systems affects the NV spin readout signal and present the demonstration of this readout through optical plasmons in an integrated nanophotonic interface. We will show that spin relaxometry is a powerful tool that allows to probe the magnonic density of states and its electrical tuning with sub-um spatial resolution. Furthermore, we will discuss how spin signal readout sensitivity can be enhanced with the use of plasmonic nanostructures deterministically assembled on the nanoscale.
Abstract The nitrogen-vacancy (NV) color center in diamond has demonstrated great promise in a wide range of quantum sensing. Recently, there have been a series of proposals and experiments using NV centers to detect spin noise of quantum materials near the diamond surface. This is a rich complex area of study with novel nano-magnetism and electronic behavior, that the NV center would be ideal for sensing. However, due to the electronic properties of the NV itself and its host material, getting high quality NV centers within nanometers of such systems is challenging. Band bending caused by space charges formed at the metal-semiconductor interface force the NV center into its insensitive charge states. Here, we investigate optimizing this interface by depositing thin metal films and thin insulating layers on a series of NV ensembles at different depths to characterize the impact of metal films on different ensemble depths. We find an improvement of coherence and dephasing times we attribute to ionization of other paramagnetic defects. The insulating layer of alumina between the metal and diamond provide improved photoluminescence and higher sensitivity in all modes of sensing as compared to direct contact with the metal, providing as much as a factor of 2 increase in sensitivity, decrease of integration time by a factor of 4, for NV T 1 relaxometry measurements.