Spectroscopic studies of fractal aggregates of silver nanospheres undergoing local restructuring

We present an experimental spectroscopic study of large random colloidal aggregates of silver nanoparticles undergoing local restructuring. We argue that such well-known phenomena as strong fluctuation of local electromagnetic fields, appearance of "hot spots" and enhancement of nonlinear optical responses depend on the local structure on the scales of several nanosphere diameters, rather that the large-scale fractal geometry of the sample.Comment: 3.5 pages, submitted to J. Chem. Phy

Local anisotropy and giant enhancement of local electromagnetic fields in fractal aggregates of metal nanoparticles

We have shown within the quasistatic approximation that the giant fluctuations of local electromagnetic field in random fractal aggregates of silver nanospheres are strongly correlated with a local anisotropy factor S which is defined in this paper. The latter is a purely geometrical parameter which characterizes the deviation of local environment of a given nanosphere in an aggregate from spherical symmetry. Therefore, it is possible to predict the sites with anomalously large local fields in an aggregate without explicitly solving the electromagnetic problem. We have also demonstrated that the average (over nanospheres) value of S does not depend noticeably on the fractal dimension D, except when D approaches the trivial limit D=3. In this case, as one can expect, the average local environment becomes spherically symmetrical and S approaches zero. This corresponds to the well-known fact that in trivial aggregates fluctuations of local electromagnetic fields are much weaker than in fractal aggregates. Thus, we find that, within the quasistatics, the large-scale geometry does not have a significant impact on local electromagnetic responses in nanoaggregates in a wide range of fractal dimensions. However, this prediction is expected to be not correct in aggregates which are sufficiently large for the intermediate- and radiation-zone interaction of individual nanospheres to become important.Comment: 9 pages 9 figures. No revisions from previous version; only figure layout is change

Effects of Size Polydispersity on the Extinction Spectra of Colloidal Nanoparticle Aggregates

We investigate the effect of particle polydispersity on the optical extinction spectra of colloidal aggregates of spherical metallic (silver) nanoparticles, taking into account the realistic interparticle gaps caused by layers of stabilizing polymer adsorbed on the metal surface (adlayers). The spectra of computer-generated aggregates are computed using two different methods. The coupled-multipole method is used in the quasistatic approximation and the coupled-dipole method beyond the quasistatics. The latter approach is applicable if the interparticle gaps are sufficiently wide relative to the particle radii. Simulations are performed for two different particle size distribution functions (bimodal and Gaussian), varying the number of particles per aggregate, and different distribution functions of the interparticle gap width. The strong influence of the latter factor on the spectra is demonstrated and investigated in detail

Convolutional neural networks for mode on-demand high finesse optical resonator design

We demonstrate the use of machine learning through convolutional neural networks to solve inverse design problems of optical resonator engineering. The neural network finds a harmonic modulation of a spherical mirror to generate a resonator mode with a given target topology ("mode on-demand"). The procedure allows us to optimize the shape of mirrors to achieve a significantly enhanced coupling strength and cooperativity between a resonator photon and a quantum emitter located at the center of the resonator. In a second example, a double-peak mode is designed which would enhance the interaction between two quantum emitters, e.g., for quantum information processing.Comment: 9 pages, 7 figure