The extraordinary sensitivity of plasmonic sensors is well known in the optics and photonics community. These sensors exploit simultaneously the enhancement and the localization of electromagnetic fields close to the interface between a metal and a dielectric. This enables, for example, the design of integrated biochemical sensors at scales far below the diffraction limit. Despite their practical realization and successful commercialization, the sensitivity and associated precision of plasmonic sensors are starting to reach their fundamental classical limit given by quantum fluctuations of light -known as the shot-noise limit. To improve the sensing performance of these sensors beyond the classical limit, quantum resources are increasingly being employed. This area of research has become known as 'quantum plasmonic sensing' and it has experienced substantial activity in recent years for applications in chemical and biological sensing. This review aims to cover both plasmonic and quantum techniques for sensing, and shows how they have been merged to enhance the performance of plasmonic sensors beyond traditional methods. We discuss the general framework developed for quantum plasmonic sensing in recent years, covering the basic theory behind the advancements made, and describe the important works that made these advancements. We also describe several key works in detail, highlighting their motivation, the working principles behind them, and their future impact. The intention of the review is to set a foundation for a burgeoning field of research that is currently being explored out of intellectual curiosity and for a wide range of practical applications in biochemistry, medicine, and pharmaceutical research.
Single gold nanoparticles can act as nanoantennas for enhancing the fluorescence of emitters in their near fields. Here we present experimental and theoretical studies of scanning antenna-based fluorescence microscopy as a function of the diameter of the gold nanoparticle. We examine the interplay between fluorescence enhancement and spatial resolution and discuss the requirements for deciphering single molecules in a dense sample. Resolutions better than 20 nm and fluorescence enhancement up to 30 times are demonstrated experimentally. By accounting for the tip shaft and the sample interface in finite-difference time-domain calculations, we explain why the measured fluorescence enhancements are higher in the presence of an interface than the values predicted for a homogeneous environment.
In the past decade, lead halide perovskite nanocrystals or quantum dots (QDs) have attracted keen interest due to their potential applications in many optoelectronic systems. In addition, all-inorganic (CsPbX3) perovskite QDs are suggested to be efficient single photon emitting centers. Herein, we study the photon emission properties of recently synthesized organic–inorganic FAPbBr3 QDs. Our results show that individual FAPbBr3 QDs can act as good single-photon sources with very low multiphoton emission probability achieved by extremely fast nonradiative Auger recombination. However, they exhibit photodegradation and fluorescence intensity intermittency, called blinking. By analyzing the ON(OFF) duration time distribution, particularly the OFF duration times, we suggest that two types of blinking (type-A and type-B) simultaneously contribute to the blinking behavior of FAPbBr3 QDs. In type-A and type-B blinking, the ON/OFF periods are attributed to charged/discharged states and to activation/deactivation of fast nonradiative recombination centers, respectively. By analyzing the ON/OFF duration cutoff time as a function of the excitation intensity, we verify that type-A blinking is caused mainly by diffusion-controlled electron transfer, partially accompanied by Auger ionization processes.
We investigate the use of twin-mode quantum states of light with symmetric statistical features in their photon number for improving intensity-sensitive surface plasmon resonance (SPR) sensors. For this purpose, one of the modes is sent into a prism setup where the Kretschmann configuration is employed as a sensing platform and the analyte to be measured influences the SPR excitation conditions. This influence modifies the output state of light that is subsequently analyzed by an intensity-difference measurement scheme. We show that quantum noise reduction is achieved not only as a result of the sub-Poissonian statistical nature of a single mode, but also as a result of the non-classical correlation of the photon number between the two modes. When combined with the high sensitivity of the SPR sensor, we show that the use of twin-mode quantum states of light notably enhances the estimation precision of the refractive index of an analyte. With this we are able to identify a clear strategy to further boost the performance of SPR sensors, which are already a mature technology in biochemical and medical sensing applications.
Reducing the noise below the shot-noise limit in sensing devices is one of the key promises of quantum technologies. Here, we study quantum plasmonic sensing based on an attenuated total reflection configuration with single photons as input. Our sensor is the Kretschmann configuration with a gold film, and a blood protein in an aqueous solution with different concentrations serves as an analyte. The estimation of the refractive index is performed using heralded single photons. We also determine the estimation error from a statistical analysis over a number of repetitions of identical and independent experiments. We show that the errors of our plasmonic sensor with single photons are below the shot-noise limit even in the presence of various experimental imperfections. Our results demonstrate a practical application of quantum plasmonic sensing is possible given certain improvements are made to the setup investigated, and pave the way for a future generation of quantum plasmonic applications based on similar techniques.
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