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New techniques enhance brightness and control of quantum defects in nanodiamonds
(Nanowerk Spotlight) The quest to harness the power of quantum mechanics for practical applications has been a driving force in physics and materials science. At the heart of this endeavor lies the challenge of creating and manipulating quantum systems that can operate reliably at room temperature. While many quantum technologies require extreme cold or vacuum conditions, a promising exception has emerged in the form of diamond defects known as nitrogen-vacancy (NV) centers.
These atomic-scale impurities in diamond's crystal structure have captivated researchers due to their unique quantum properties that persist even in ambient conditions. NV centers can be thought of as artificial atoms trapped within the diamond lattice, possessing electronic and spin states that can be manipulated and read out using light. This makes them powerful tools for sensing magnetic fields, electric fields, and temperature with nanoscale precision.
The potential applications of NV centers span a wide range of fields, from quantum computing and secure communications to medical imaging and geological surveying. However, realizing these applications has been hindered by the challenges of working with bulk diamond, which is expensive, difficult to process, and not easily integrated into existing technologies.
Enter nanodiamonds - tiny particles of diamond typically less than 100 nanometers in size. These nanoparticles retain many of diamond's exceptional properties while offering new possibilities for manipulation and integration. The vision of using NV centers in nanodiamonds as quantum sensors that can be injected into living cells, incorporated into electronic devices, or dispersed in fluids has driven intense research efforts over the past decade.
Yet, significant hurdles have remained. The optical properties of as-produced nanodiamonds are often poor, with surface defects and non-diamond carbon phases quenching the light emission from NV centers. Moreover, precisely controlling the creation and charge state of NV centers in nanoparticles has proven challenging. These limitations have held back the development of nanodiamond-based quantum technologies, leaving their full potential unrealized.
Now, a team of researchers from the University of Torino and the National Institute for Nuclear Physics in Italy has made significant strides in overcoming these obstacles. Their work, published in Advanced Functional Materials ("Creation, Control, and Modeling of NV Centers in Nanodiamonds"), presents new techniques to optimize the optical properties of nanodiamonds and precisely control their NV center content. This research marks a crucial step forward in the long-standing effort to harness the quantum properties of diamond at the nanoscale, potentially opening the door to a new generation of ultra-sensitive quantum sensors and biomedical imaging tools.
The study tackles the challenges of nanodiamond optimization through a systematic exploration of post-production treatments. By carefully investigating the effects of surface oxidation and proton beam irradiation, the researchers have developed methods to dramatically enhance the brightness of NV centers in nanodiamonds while gaining unprecedented control over their creation and charge state.
Their findings not only provide practical techniques for improving nanodiamond properties but also offer deep insights into the fundamental processes governing NV center formation and behavior in nanocrystalline materials. This work builds on years of incremental progress in the field, leveraging advanced characterization techniques and theoretical modeling to push the boundaries of what's possible with these quantum-enhanced nanoparticles.
The study began with a systematic investigation of thermal oxidation treatments on nanodiamonds. The researchers explored a wide range of temperatures (450 °C to 525 °C) and durations (3 to 48 hours) to understand how these parameters affect the surface chemistry and optical properties of the nanoparticles.
Using diffuse reflectance infrared Fourier transform (DRIFT) spectroscopy, the team observed that increasing oxidation levels correlated with a higher number of oxygen-containing chemical groups on the nanodiamond surface. Mild oxidation primarily produced carboxylic acids and anhydrides, while more aggressive treatments led to the formation of aldehydes, lactones, and ketones. At the highest oxidation levels, a significant increase in C-O groups was observed.
These changes in surface chemistry had a profound effect on the optical properties of the nanodiamonds. Photoluminescence (PL) spectroscopy revealed that oxidation treatments could enhance the fluorescence intensity of NV centers by up to two orders of magnitude. This dramatic improvement was attributed to the removal of surface defects and non-diamond carbon phases that typically quench NV center emission.
Interestingly, the researchers found that the ratio of negatively charged (NV-) to neutral (NV0) centers also varied with oxidation conditions. This ratio peaked at intermediate oxidation levels, suggesting a complex interplay between surface chemistry and NV center charge state.
The second major component of the study involved the use of proton beam irradiation to create additional NV centers in the nanodiamonds. The team irradiated samples with 2 MeV protons at various fluences, ranging from 1.5 × 1014 to 1.5 × 1017 cm-2. They found that a fluence of 4.4 × 1016 cm-2 produced the optimal increase in NV center fluorescence, resulting in about an order of magnitude enhancement compared to unirradiated samples.
To understand the mechanisms behind NV center formation and optimize the irradiation process, the researchers developed a novel mathematical model. This model accounts for the creation of vacancies by ion irradiation, their diffusion and combination with nitrogen impurities to form NV centers, and the impact of increasing defect density on fluorescence quenching. By fitting experimental data to this model, the team was able to extract key parameters such as the efficiency of (NV-) and (NV0) formation.
The model revealed that NV- centers form more efficiently than NV0 centers in these nanodiamonds, likely due to the availability of charges at the particle surface. It also predicted that nearly all nitrogen impurities become involved in NV center formation at vacancy densities around 1020 cm-3, which corresponds to an irradiation fluence of about 1017 cm-2.
One of the most significant findings of the study was that combining optimized oxidation treatments with proton irradiation could increase the overall fluorescence intensity of the nanodiamonds by approximately three orders of magnitude compared to untreated samples. This represents a major leap forward in the brightness of nanodiamond-based light sources.
The researchers also conducted detailed investigations of fluorescence lifetime using time-resolved spectroscopy. These measurements provided further insights into the quenching processes affecting NV centers and confirmed the effectiveness of the oxidation treatments in removing surface defects.
The implications of this work are far-reaching. The ability to produce extremely bright, stable fluorescent nanodiamonds opens new possibilities for their use as biomarkers and probes in cellular imaging. The enhanced brightness could allow for single-particle tracking and super-resolution imaging techniques that were previously challenging with nanodiamonds.
Moreover, the precise control over NV center creation and charge state achieved in this study is crucial for quantum sensing applications. The ability to maximize the concentration of NV- centers, which are used for magnetic field and temperature sensing, could lead to significant improvements in the sensitivity of nanodiamond-based quantum sensors.
The mathematical model developed by the team also represents an important contribution to the field. It provides a framework for predicting and optimizing NV center formation in nanodiamonds, which could accelerate the development of tailored nanoparticles for specific applications.
While the current study focused on nanodiamonds produced by high-pressure, high-temperature (HPHT) synthesis, the researchers suggest that their methods and model could be applied to nanodiamonds produced by other means, such as detonation synthesis or chemical vapor deposition (CVD).
Michael Berger By – Michael is author of three books by the Royal Society of Chemistry:
Nano-Society: Pushing the Boundaries of Technology,
Nanotechnology: The Future is Tiny, and
Nanoengineering: The Skills and Tools Making Technology Invisible
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