Excitation Enhancement of a Quantum Dot Coupled to a Plasmonic Antenna

Plasmonic antennas are key elements to control the luminescence of quantum emitters. However, the antenna's influence is often hidden by quenching losses. Here, the luminescence of a quantum dot coupled to a gold dimer antenna is investigated. Detailed analysis of the multiply excited states quantifies the antenna's influence on the excitation intensity and the luminescence quantum yield separately

Near-Field Mapping of Plasmonic Antennas by Multiphoton Absorption in Poly(methyl methacrylate)

Mapping the optical near-field response around nanoantennas is a challenging yet indispensable task to engineer light-matter interaction at the nanometer scale. Recently, photosensitive molecular probes, which undergo morphological or chemical changes induced by the local optical response of the nanostructures, have been proposed as a handy alternative to more cumbersome optical and electron-based techniques. Here, we report four-photon absorption in poly(methyl methacrylate) (PMMA) as a very promising tool for nanoimaging the optical near-field around nanostructures over a broad range of near-infrared optical wavelengths. The high performance of our approach is demonstrated on single-rod antennas and coupled gap antennas by comparing experimental maps with 3D numerical simulations of the electric near-field intensity

Light propagation in nanorod arrays

We study propagation of TM- and TE-polarized light in two-dimensional arrays of silver nanorods of various diameters in a gelatin background. We calculate the transmittance, reflectance and absorption of arranged and disordered nanorod arrays and compare the exact numerical results with the predictions of the Maxwell-Garnett effective-medium theory. We show that interactions between nanorods, multipole contributions and formations of photonic gaps affect strongly the transmittance spectra that cannot be accounted for in terms of the conventional effective-medium theory. We also demonstrate and explain the degradation of the transmittance in arrays with randomly located rods as well as weak influence of their fluctuating diameter. For TM modes we outline the importance of skin-effect, which causes the full reflection of the incoming light. We then illustrate the possibility of using periodic arrays of nanorods as high-quality polarizers.Comment: 6 pages, 7 figure

Above threshold ionization by few-cycle spatially inhomogeneous fields

We present theoretical studies of above threshold ionization (ATI) produced by spatially inhomogeneous fields. This kind of field appears as a result of the illumination of plasmonic nanostructures and metal nanoparticles with a short laser pulse. We use the time-dependent Schr\"odinger equation (TDSE) in reduced dimensions to understand and characterize the ATI features in these fields. It is demonstrated that the inhomogeneity of the laser electric field plays an important role in the ATI process and it produces appreciable modifications to the energy-resolved photoelectron spectra. In fact, our numerical simulations reveal that high energy electrons can be generated. Specifically, using a linear approximation for the spatial dependence of the enhanced plasmonic field and with a near infrared laser with intensities in the mid- 10^{14} W/cm^{2} range, we show it is possible to drive electrons with energies in the near-keV regime. Furthermore, we study how the carrier envelope phase influences the emission of ATI photoelectrons for few-cycle pulses. Our quantum mechanical calculations are supported by their classical counterparts

Optimum morphology of gold nanorods for light-induced hyperthermia

Owing to their unique chemical and physical properties, colloidal gold nanoparticles have prompted a wide variety of biocompatible nano-agents for cancer imaging, diagnosis and treatment. In this context, biofunctionalized gold nanorods (AuNRs) are promising candidates for light-induced hyperthermia, to cause local and selective damage in malignant tissue. Yet, the efficacy of AuNR-based hyperthermia is highly dependent on several experimental parameters; in particular, the AuNR morphology strongly affects both physical and biological involved processes. In the present work, we systematically study the influence of different structural parameters like the AuNR aspect ratio, length and molecular weight on in vitro cytotoxicity, cellular uptake and heat generation efficiency. Our results enable us to identify the optimum AuNR morphology to be used for in vivo hyperthermia treatment.Postprint (author's final draft

High-order harmonic generation from inhomogeneous fields

We present theoretical studies of high-order harmonic generation (HHG) produced by non-homogeneous fields as resulting from the illumination of plasmonic nanostructures with a short laser pulse. We show that both the inhomogeneity of the local fields and the confinement of the electron movement play an important role in the HHG process and lead to the generation of even harmonics and a significantly increased cutoff, more pronounced for the longer wavelengths cases studied. In order to understand and characterize the new HHG features we employ two different approaches: the numerical solution of the time dependent Schr\"odinger equation (TDSE) and the semiclassical approach known as Strong Field Approximation (SFA). Both approaches predict comparable results and show the new features, but using the semiclassical arguments behind the SFA and time-frequency analysis tools, we are able to fully understand the reasons of the cutoff extension.Comment: 25 pages, 12 figure

Plasmon-Assisted Delivery of Single Nano-Objects in an Optical Hot Spot

Fully exploiting the capability of nano-optics to enhance light-matter interaction on the nanoscale is conditioned by bringing the nano-object to interrogate within the minuscule volume where the field is concentrated. There currently exists several approaches to control the immobilization of nano-objects but they all involve a cumbersome delivery step and require prior knowledge of the “hot spot” location.1−6 Herein, we present a novel technique in which the enhanced local field in the hot spot is the driving mechanism that triggers the binding of proteins via three-photon absorption. This way, we demonstrate exclusive immobilization of nanoscale amounts of bovine serum albumin molecules into the nanometer-sized gap of plasmonic dimers. The immobilized proteins can then act as a scaffold to subsequently attach an additional nanoscale object such as a molecule or a nanocrystal. This universal technique is envisioned to benefit a wide range of nano-optical functionalities including biosensing,7−12 enhanced spectroscopy like surface-enhanced Raman spectroscopy13,14 or surface-enhanced infrared absorption spectroscopy,15 as well as quantum optics.1,2,