Polarization-resolved extinction and scattering cross-section of individual gold nanoparticles measured by wide-field microscopy on a large ensemble

We report a simple, rapid, and quantitative wide-field technique to measure the optical extinction $\sigma_{\rm ext}$ and scattering $\sigma_{\rm sca}$ cross-section of single nanoparticles using wide-field microscopy enabling simultaneous acquisition of hundreds of nanoparticles for statistical analysis. As a proof of principle, we measured nominally spherical gold nanoparticles of 40\,nm and 100\,nm diameter and found mean values and standard deviations of $\sigma_{\rm ext}$ and $\sigma_{\rm sca}$ consistent with previous literature. Switching from unpolarized to linearly polarized excitation, we measured $\sigma_{\rm ext}$ as a function of the polarization direction, and used it to characterize the asphericity of the nanoparticles. The method can be implemented cost-effectively on any conventional wide-field microscope and is applicable to any nanoparticles

Structure and zero-dimensional polariton spectrum of natural defects in GaAs/AlAs microcavities

We present a correlative study of structural and optical properties of natural defects in planar semiconductor microcavities grown by molecular beam epitaxy, which are showing a localized polariton spectrum as reported in Zajac et al., Phys. Rev. B 85, 165309 (2012). The three-dimensional spatial structure of the defects was studied using combined focussed ion beam (FIB) and scanning electron microscopy (SEM). We find that the defects originate from a local increase of a GaAs layer thickness. Modulation heights of up to 140nm for oval defects and 90nm for round defects are found, while the lateral extension is about 2um for oval and 4um for round defects. The GaAs thickness increase is attributed to Ga droplets deposited during growth due to Ga cell spitting. Following the droplet deposition, the thickness modulation expands laterally while reducing its height, yielding oval to round mounds of the interfaces and the surface. With increasing growth temperature, the ellipticity of the mounds is decreasing and their size is increasing. This suggests that the expansion is related to the surface mobility of Ga, which with increasing temperature is increasing and reducing its anisotropy between the [110] and [1-10] crystallographic directions. Comprehensive data consisting of surface profiles of defects measured using differential interference contrast (DIC) microscopy, volume information obtained using FIB/SEM, and characterization of the resulting confined polariton spectrum are presented

Femtosecond phase-resolved microscopy of plasmon dynamics in individual gold nanospheres

The selective optical detection of individual metallic nanoparticles (NPs) with high spatial and temporal resolution is a challenging endeavour, yet is key to the understanding of their optical response and their exploitation in applications from miniaturised optoelectronics and sensors to medical diagnostics and therapeutics. However, only few reports on ultrafast pump-probe spectroscopy on single small metallic NPs are available to date. Here, we demonstrate a novel phase-sensitive four-wave mixing (FWM) microscopy in heterodyne detection to resolve for the first time the ultrafast changes of real and imaginary part of the dielectric function of single small (<40nm) spherical gold NPs. The results are quantitatively described via the transient electron temperature and density in gold considering both intraband and interband transitions at the surface plasmon resonance. This novel microscopy technique enables background-free detection of the complex susceptibility change even in highly scattering environments and can be readily applied to any metal nanostructure

Comment on "normalization of quasinormal modes in leaky optical cavities and plasmonic resonators"

Recently, Kristensen, Ge and Hughes have compared [Phys. Rev. A 92, 053810 (2015)] three di�erent methods for normalization of quasinormal modes in open optical systems, and concluded that they all provide the same result. We show here that this conclusion is incorrect and illustrate that the normalization of [Opt. Lett. 37, 1649 (2012)] is divergent for any optical mode having a �nite quality factor, and that the Silver-M�uller radiation condition is not ful�lled for quasinormal modes

Ultrafast exciton dephasing in PbS colloidal quantum dots

In this work, we have measured the ground state excitonic dephasing in PbS QDs of sizes from 3.7nm to 5.7nm diameter in the temperature range from 5K to 100K by transient degenerate four-wave mixing (FWM) using 100fs pulses. A combination of heterodyne and k-selection detection was implemented to increase sensitivity and enable 4 orders of magnitude dynamic range in the FWM field detection

Realistic heterointerfaces model for excitonic states in growth-interrupted quantum wells

We present a model for the disorder of the heterointerfaces in GaAs quantum wells including long-range components like monolayer island formation induced by the surface diffusion during the epitaxial growth process. Taking into account both interfaces, a disorder potential for the exciton motion in the quantum well plane is derived. The excitonic optical properties are calculated using either a time-propagation of the excitonic polarization with a phenomenological dephasing, or a full exciton eigenstate model including microscopic radiative decay and phonon scattering rates. While the results of the two methods are generally similar, the eigenstate model does predict a distribution of dephasing rates and a somewhat modified spectral response. Comparing the results with measured absorption and resonant Rayleigh scattering in GaAs/AlAs quantum wells subjected to growth interrupts, their specific disorder parameters like correlation lengths and interface flatness are determined. We find that the long-range disorder in the two heterointerfaces is highly correlated, having rather similar average in-plane correlation lengths of about 60 and 90 nm. The distribution of dephasing rates observed in the experiment is in agreement with the results of the eigenstate model. Finally, we simulate highly spatially resolved optical experiments resolving individual exciton states in the deduced interface structure.Comment: To appear in Physical Review

Optimizing the Drude-Lorentz model for material permittivity: Examples for semiconductors

Approximating the frequency dispersion of the permittivity of materials with simple analytical functions is of fundamental importance for understanding and modeling their optical properties. Quite generally, the permittivity can be treated in the complex frequency plane as an analytic function having a countable number of simple poles which determine the dispersion of the permittivity, with the pole weights corresponding to generalized conductivities of the medium at these resonances. The resulting Drude-Lorentz model separates the poles at frequencies with zero real part (Ohm's law and Drude poles) from poles with finite real part (Lorentz poles). To find the parameters of such an analytic function, we minimize the error weighted deviation between the model and measured values of the permittivity. We show examples of such optimizations for various semiconductors (Si, GaAs and Ge), for different frequency ranges and up to five pairs of Lorentz poles accounted for in the model.Comment: arXiv admin note: substantial text overlap with arXiv:1612.0692

Wide-field imaging of single nanoparticle extinction with sub-nm2 sensitivity

We report a highly sensitive wide-�eld imaging technique for quantitative measurement of the optical extinction cross-section �ext of single nanoparticles. The technique is simple and high-speed, and enables simultaneous acquisition of hundreds of nanoparticles for statistical analysis. Using rapid referencing, fast acquisition, and a deconvolution analysis, a shot-noise limited sensitivity down to 0.4nm2 is achieved. Measurements on a set of individual gold nanoparticles of 5nm diameter using this method yield �ext = (10:0 � 3:1)nm2, consistent with theoretical expectations, and well above the background uctuations of 0.9nm2