Spontaneous emission of quantum emitters can be modified by engineering their optical environment. This allows a resonant nanoantenna to significantly modify the radiative properties of a quantum emitter. In this article, we go beyond the common electric dipole approximation for the molecular electronic transition and take light-matter coupling through higher order multipoles into account. We investigate, by means of theory and numerical simulations, a strong enhancement of the magnetic dipole and electric quadrupole emission channels of a molecule adjacent to a plasmonic patch nanoantenna. While this on its own had been considered, the assumption in prior work usually has been that each molecular transition is dominated only by one of those multipolar emission channels. This leads naturally to the notion of discussing the modified emission in terms of a modified local density of states defined for each specific multipolar transition. In reality, this restricts the applicability of the approach, since specific molecular transitions occur via multiple multipolar pathways that have to be considered all at once. Here, we introduce a framework to study interference effects between higher order transitions in molecules by (a) a rigorous quantum-chemical calculation of their multipolar moments and (b) by a consecutive investigation of the transition rate upon coupling to an arbitrarily shaped nanoantenna. Based on that formalism we predict interference effects between these transition channels. This allows for a strong suppression of radiation by exploiting destructive interference. Our work suggests that placing a suitably chosen molecule at a well defined position and at a well defined orientation relative to a nanoantenna can fully suppress the transition probability.
Over the last few years, optical nanoantennas are continuously attracting interest owing to their ability to efficiently confine, localize resonance, and significantly enhanced electromagnetic fields at subwavelength scale. However, such strong confinement can be further enhanced by using an appropriate combination of optical nanoantenna and Slanted Bound states in the continuum cavities. Here, we propose to synergistically bridge the plasmonic nanoantenna and high optical quality-factor cavities to numerically demonstrate three orders of magnitude local intensity enhancement. The proposed hyb…
The nanoscale interaction between single emitters and plasmonic structures is traditionally studied by relying on near-perfect, deterministic, nanoscale-control. This approach is ultra-low throughput thus rendering systematic studies difficult to impossible. Here, we show that super resolution microscopy in combination with data-driven statistical analysis allows studying near-field interactions of single molecules with resonant nanoantennas. We systematically tune the antennas' spectral resonances and show that emitters can be separated according to their coupling strength with said structure…
Bidirectional nanoantennas are of key relevance for advanced functionalities to be implemented at the nanoscale, and in particular for color routing in an ultracompact flat-optics configuration. Here we demonstrate a novel approach avoiding complex collective geometries and/or restrictive morphological parameters, based on cross-polarized detuned plasmonic nanoantennas in a uniaxial (quasi-1D) bimetallic configuration. The nanofabrication of such a flat-optics system is controlled over a large-area (cm^2) by a novel self-organized technique exploiting ion-induced nanoscale wrinkling instabilit…
Plasmonic nanoantennas have the ability to confine and enhance incident electromagnetic fields into very sub-wavelength volumes, while at the same time efficiently radiating energy to the far-field. These properties have allowed plasmonic nanoantennas to be extensively used for exciting quantum emitters-such as molecules and quantum dots-and also for the extraction of photons from them for measurements in the far-field. Due to electromagnetic reciprocity, it is expected that plasmonic nanoantennas radiate energy as efficiently as an external source can couple energy to them. In this paper, we …
Metal nanoantennas enable the manipulation of light emission and detection at the single photon level by confining light into very small volumes. Emitters coupled to these plasmonic structures are thus ideal candidates for usage in quantum information technology. However, controllably and reproducibly placing quantum emitters into nanocavities has been challenging due to the sizes of the systems involved. Here, we investigate the trapping dynamics of single emitters into nanocavities via optical gradient forces by using single-molecule super-resolution imaging and tracking. We show that molecu…
We present a practical new method for fabricating a coupled single quantum emitter-plasmonic nanoantenna system. Emission characteristics of a single defect center embedded in hexagonal Boron Nitride (hBN) multilayers is modified using plasmonic nanoantennas. By dewetting thin silver films on hBN multilayers, plasmonic nanoantennas are obtained in a size controlled way with no adverse effects on the defects. A very same single defect center is investigated with and without nanoantenna in order to demonstrate the modification of its emission characteristics. Based on the initial silver film thi…
Nanotechnology and the consequent emergence of miniaturized devices are driving the need to improve our understanding of the mechanical properties of a myriad of materials. Here we focus on amorphous polymeric materials and introduce a new way to determine the nanoscale mechanical response of polymeric thin films in the GHz range, using ultrafast optical means. Coupling of the films to plasmonic nanoantennas excited at their vibrational eigenfrequencies allows the extraction of the values of the mechanical moduli as well as the estimation of the glass transition temperature via time-domain mea…
We propose and realize a tunable plasmonic nanoantenna design consisting of two stacked Ag cuboids that are integrated into a rolled-up semiconductor microtube. The antenna's resonance is tuned by varying the cuboid's distance to match the photoluminescence emission of an embedded GaAs quantum well. Spatially, spectrally and temporally resolved photoluminescence measurements reveal a redshift and a reduction in lifetime of the quantum-well emission as signatures for the coupling to the antenna system. By means of finite-element electromagnetic simulations, we assign the coupling to an excitati…
We present a novel procedure for manipulating the near-field of plasmonic nanoantennas using neural network-controlled laser pulse-shaping. As model systems we numerically studied the spatial distribution of the second harmonic response of L-shaped nanoantennas illuminated by broadband laser pulses. We first show that a trained neural network can be used to predict the relative intensity of the second-harmonic hotspots of the nanoantenna for a given spectral phase and that it can be employed to deterministically switch individual hotspots on and off on sub-diffraction length scale by shaping t…
Single photon sources with high brightness and subnanosecond lifetimes are key components for quantum technologies. Optical nanoantennas can enhance the emission properties of single quantum emitters, but this approach requires accurate nanoscale positioning of the source at the plasmonic hotspot. Here, we use plasmonic nanoantennas to simultaneously trap single colloidal quantum dots and enhance their photoluminescence. The nano-optical trapping automatically locates the quantum emitter at the nanoantenna hotspot without further processing. Our dedicated nanoantenna design achieves a high tra…
Energy-resolved hot carrier relaxation dynamics in monocrystalline plasmonic nanoantennas
热载流子是驱动大范围化学物理机制的高能光激发载流子。在纳米尺度下，通过照射等离子体天线来促进这些载体的有效生成。然而，超快弛豫速率分别阻碍了它们在未来基于热载流子的器件中的部署。在本文中，我们报告的皮秒弛豫动力学的热载流子在等离子体激元单晶金纳米天线。的时间动力学的热载流子的实验研究通过询问的非线性光致发光响应的天线与光谱分辨的两个脉冲的相关配置。我们测量了随时间变化的非线性阶数从1到8，这挑战了多光子金发光的常见解释。我们证明了光激发载流子的弛豫依赖于它们相对于费米能级的能量。我们发现电子-空穴对能量范围从c. a. 0.2到1.8eV。热载流子能量和弛豫动力学之间的定量关系是优化热载流子辅助过程的重要发现，并揭示了等离子体结构中非线性光致发光的复杂性。
Nanoantennas offer the ultimate spatial control over light by concentrating optical energy well below the diffraction limit, whereas their quality factor (Q) is constrained by large radiative and dissipative losses. Dielectric microcavities, on the other hand, are capable of generating a high Q-factor through an extended photon storage time but have a diffraction-limited optical mode volume. Here we bridge the two worlds, by studying an exemplary hybrid system integrating plasmonic gold nanorods acting as nanoantennas with an on-resonance dielectric photonic crystal (PC) slab acting as a low-l…
Plasmonic nanostructures attract tremendous attention as they confine electromagnetic fields well below the diffraction limit while simultaneously sustaining extreme local field enhancements. To fully exploit these properties, the identification and classification of resonances in such nanostructures is crucial. Recently, a novel figure of merit for resonance classification has been proposed 1 and its applicability was demonstrated mostly to toy model systems. This novel measure, the energy-based plasmonicity index (EPI), characterizes the nature of resonances in molecular nanostructures. The …
The interaction of light with subwavelength metallic nano-structures is at the heart of different current scientific hot topics, namely plasmonics, metamaterials and nanoantennas. Research in these disciplines during the last decade has given rise to new, powerful concepts providing an unprecedented degree of control over light manipulation at the nanoscale. However, only recently have these concepts been used to increase the capabilities of light processing in current photonic integrated circuits (PICs), which traditionally rely only on dielectric materials with element sizes larger than the …
Single-molecule fluorescence techniques are essential for investigating the molecular mechanisms in biological processes. However, achieving sub-millisecond temporal resolution to monitor fast molecular dynamics remains a significant challenge. The fluorescence brightness is the key parameter that generally defines the temporal resolution for these techniques. Conventional microscopes and standard fluorescent emitters fall short in achieving the high brightness required for sub-millisecond monitoring. Plasmonic nanoantennas have been proposed as a solution, but despite huge fluorescence enhanc…
Metal nanostructures are key elements in nanooptics owing to their strong resonant interaction with light through local plasmonic charge oscillations. Their ability to shape light at the nanoscale have made them important across a multitude of areas, including biosensing, energy conversion and ultrathin flat metaoptics. Yet another dimension of avenues is foreseen for dynamic nanoantennas, ranging from tuneable metalenses for miniaturized medical devices to adaptable windows that control radiation flows in and out of buildings. However, enabling nano-optical antennas to be dynamically controll…
Electrically-driven optical antennas can serve as compact sources of electromagnetic radiation operating at optical frequencies. In the most widely explored configurations, the radiation is generated by electrons tunneling between metallic parts of the structure when a bias voltage is applied across the tunneling gap. Rather than relying on an inherently inefficient inelastic light emission in the gap, we suggest to use a ballistic nanoconstriction as the feed element of an optical antenna supporting plasmonic modes. We discuss the underlying mechanisms responsible for the optical emission, an…
Efficient optical excitation of hybridized plasmon modes in nanoantennas is vital to achieve many promising functionalities, but it can be challenging due to a field-profile mismatch between the incident light and the hybrid mode. We present a general approach for efficient hybrid-mode excitation by focusing the incident light field in the basis of cylindrically polarized vector beams of various higher-order spiral phases. Such basis vector beams are described in the higher-order polarization states and Stokes parameters (both defined locally in polar coordinates), and visualized corresponding…
The enhancement of the photoluminescence of quantum dots induced by an optical nanoantenna has been studied considerably, but there is still significant interest in optimizing and miniaturizing such structures, especially when accompanied by an experimental demonstration. Most of the realizations use plasmonic platforms, and some also use all-dielectric nanoantennas, but hybrid dielectric-plasmonic (subwavelength) nanostructures have been very little explored. In this paper, we propose and demonstrate single subwavelength hybrid dielectric-plasmonic optical nanoantennas coupled to localized qu…
Thermonanophotonics, i.e. the study of photothermal effects in optical nanoantennas, has recently attracted growing interest. While thermoplasmonic structures enable a broad range of applications, from imaging and optofluidics devices to medical and photochemical systems, dielectric nanoantennas open new opportunities for thermo-optical modulation and reconfigurable metasurfaces. However, computing both photo-thermal and thermo-optical effects in large arrays of nanoantennas remains a challenge. In this work, we implement a fast numerical method to compute the temperature increase of multi-dim…
