Plasmonic nanostructures offer a prominent foundation for plasmon sensing owing to their capacity to confine light within nanoscale regions and enhance the intensity of the local electromagnetic field. Nevertheless, the development of plasmonic sensors that operate in the midinfrared (MIR) region still presents a notable obstacle, primarily due to the limited detection sensitivity of commercial MIR detectors. To break this bottleneck, we demonstrate the characterization of the plasmonic nanostructures' MIR spectral response using a time-stretched quantum spectroscopy with frequency upconversion. Quantum spectroscopy of correlated photon pairs offers a novel approach to overcome the limitations associated with the detection sensitivity of localized surface plasmon resonances (LSPRs), particularly under conditions of excessive noise. This scheme not only extends the application of quantum spectroscopy for the plasmonic nanostructures to the MIR regions, but also circumvents the necessity of employing various types of MIR detectors. In addition, by wavelength-to-time mapping and using a single-pixel detector to obtain the MIR spectral response of a plasmonic sample, nonlocal time stretching significantly increases system stability and efficiently reduces the measurement time under a low-light-level illumination. With an integration time of 600 s, time-stretched quantum spectroscopy demonstrates a detection sensitivity of 0.22 photons per pulse. The outcomes of our research pave the way for the realization of enhanced detection sensitivity in the investigation of plasmonic nanostructures in the MIR range.
Plasmonic nanostructures offer a prominent foundation for plasmon sensing owing to their capacity to confine light within nanoscale regions and enhance the intensity of the local electromagnetic field. Nevertheless, the development of plasmonic sensors that operate in the midinfrared (MIR) region still presents a notable obstacle, primarily due to the limited detection sensitivity of commercial MIR detectors. To break this bottleneck, we demonstrate the characterization of the plasmonic nanostructures' MIR spectral response using a time-stretched quantum spectroscopy with frequency upconversion. Quantum spectroscopy of correlated photon pairs offers a novel approach to overcome the limitations associated with the detection sensitivity of localized surface plasmon resonances (LSPRs), particularly under conditions of excessive noise. This scheme not only extends the application of quantum spectroscopy for the plasmonic nanostructures to the MIR regions, but also circumvents the necessity of employing various types of MIR detectors. In addition, by wavelength-to-time mapping and using a single-pixel detector to obtain the MIR spectral response of a plasmonic sample, nonlocal time stretching significantly increases system stability and efficiently reduces the measurement time under a low-light-level illumination. With an integration time of 600 s, time-stretched quantum spectroscopy demonstrates a detection sensitivity of 0.22 photons per pulse. The outcomes of our research pave the way for the realization of enhanced detection sensitivity in the investigation of plasmonic nanostructures in the MIR range.
Promoting the sensitivity of mid-infrared (MIR) spectroscopy to the single-photon level is a critical need for investigating photosensitive biological samples and chemical reactions. MIR spectroscopy based on frequency upconversion is a compelling pioneer allowing high-efficiency MIR spectral measurement with well-developed single-photon detectors, which overcomes the main limitations of high thermal noise of current MIR detectors. However, noise from other nonlinear processes caused by strong pump fields hinders the development of the upconversion-based MIR spectroscopy to reach the single-photon level. Here, a broadband MIR single-photon frequency upconversion spectroscopy is demonstrated based on the temporal-spectral quantum correlation of non-degenerate photon pairs, which is well preserved in the frequency upconversion process and is fully used in extracting the signals from tremendous noise caused by the strong pump. A correlation spectrum broader than 660 nm is achieved and applied for the demonstration of sample identification under a low incident photon flux of 0.09 average photons per pulse. The system is featured with non-destructive and robust operation, which makes single-photon-level MIR spectroscopy an appealing option in biochemical applications.
In the field of optics and photonics, plasmonic sensors have garnered considerable interest due to their outstanding sensitivity and impressive capacity to control light at the nanoscale. These sensors enable the integration of biochemical sensing platforms by exploiting the combination of enhanced and localized electromagnetic fields at the metal–dielectric interface, and they operate effectively below the diffraction limit. The performance of conventional plasmonic sensors, despite their practical development and commercial success, remains inherently constrained by classical noise constraints, owing to the quantum fluctuations of light, known as the shot-noise limit. Recent advances have introduced quantum optical resources such as entangled and squeezed light states to overcome inherent classical restrictions, thus giving rise to the quantum plasmonic sensing field. This interdisciplinary field combines the ability to enhance electric field capabilities with the precision of quantum metrology, enabling ultrasensitive chemical and biological detection that surpasses classical precision thresholds. In the last decades, theoretical models and experimental demonstrations have greatly advanced the development of quantum plasmonic sensors, improving our comprehension of quantum light–matter interactions and facilitating novel nanoscale sensing designs. This chapter provides a comprehensive overview of the fundamental principles, latest developments, and major concepts that have driven progress in quantum plasmonic sensing and shows that quantum components are being integrated into plasmonic systems, thereby transforming optical sensing to the quantum level.
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 it 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.
Ultrasensitive spectroscopy is an essential component in mid-infrared (MIR) technology. However, the drawbacks of MIR detectors pose challenges to robust MIR spectroscopy at the single-photon level. We propose an MIR single-photon frequency upconversion spectroscopy nonlocally mapping the MIR information to the time domain. Broadband MIR photons from spontaneous parametric downconversion are frequency-upconverted to the near-infrared band with quantum correlation preservation. Via the group delay of fiber, the MIR spectral information within a 1.18-micrometer bandwidth of 2.76 to 3.94 micrometers is then successfully projected to arrival times of correlated photon pairs. Under the conditions of 6.4 × 10 6 photons per second illumination, the transmission spectra of polymers with single-photon sensitivity are demonstrated using single-pixel detectors. The developed approach circumvents scanning and frequency selection instability, which stands out for its inherent compatibility for evolving environments and scalability for various wavelengths. Because of its high sensitivity and robustness, characterization of biochemical samples and weak measurement of quantum systems are possible to foresee.
Photonic sensors have many applications in a range of physical settings, from measuring mechanical pressure in manufacturing to detecting protein concentration in biomedical samples. A variety of sensing approaches exist, and plasmonic systems in particular have received much attention due to their ability to confine light below the diffraction limit, greatly enhancing sensitivity. Recently, quantum techniques have been identified that can outperform classical sensing methods and achieve sensitivity below the so-called shot-noise limit. Despite this significant potential, the use of definite photon number states in lossy plasmonic systems for further improving sensing capabilities is not well studied. Here, we investigate the sensing performance of a plasmonic interferometer that simultaneously exploits the quantum nature of light and its electromagnetic field confinement. We show that, despite the presence of loss, specialized quantum resources can provide improved sensitivity and resolution beyond the shot-noise limit within a compact plasmonic device operating below the diffraction limit.
The possibility of using weak optical signals to perform sensing of delicate samples constitutes one of the main goals of quantum photonic sensing. Furthermore, the nanoscale confinement of electromagnetic near fields in photonic platforms through surface plasmon polaritons has motivated the development of highly sensitive quantum plasmonic sensors. Despite the enormous potential of plasmonic platforms for sensing, this class of sensors is ultimately limited by the quantum statistical fluctuations of surface plasmons. Indeed, the fluctuations of the electromagnetic field severely limit the performance of quantum plasmonic sensing platforms in which delicate samples are characterized using weak near-field signals. Furthermore, the inherent losses associated with plasmonic fields levy additional constraints that challenge the realization of sensitivities beyond the shot-noise limit. Here, we introduce a protocol for quantum plasmonic sensing based on the conditional detection of plasmons. We demonstrate that the conditional detection of plasmonic fields, via plasmon subtraction, provides a new degree of freedom to control quantum fluctuations of plasmonic fields. This mechanism enables improvement of the signal-to-noise ratio of photonic sensors relying on plasmonic signals that are comparable to their associated field fluctuations. Consequently, the possibility of using weak plasmonic signals to sense delicate samples, while preserving the sample properties, has important implications for molecule sensing, and chemical detection.