The optical properties of metal nanoparticles have long been of interest in physical chemistry, starting with Faraday's investigations of colloidal gold in the middle 1800s. More recently, new lithographic techniques as well as improvements to classical wet chemistry methods have made it possible to synthesize noble metal nanoparticles with a wide range of sizes, shapes, and dielectric environments. In this feature article, we describe recent progress in the theory of nanoparticle optical properties, particularly methods for solving Maxwell's equations for light scattering from particles of arbitrary shape in a complex environment. Included is a description of the qualitative features of dipole and quadrupole plasmon resonances for spherical particles; a discussion of analytical and numerical methods for calculating extinction and scattering cross-sections, local fields, and other optical properties for nonspherical particles; and a survey of applications to problems of recent interest involving triangula...

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The Optical Properties of Metal Nanoparticles: The Influence of Size, Shape, and Dielectric Environment

J. Appl. Cryst.の発刊に際して

Fundamentals of Plasmonics.- Electromagnetics of Metals.- Surface Plasmon Polaritons at Metal / Insulator Interfaces.- Excitation of Surface Plasmon Polaritons at Planar Interfaces.- Imaging Surface Plasmon Polariton Propagation.- Localized Surface Plasmons.- Electromagnetic Surface Modes at Low Frequencies.- Applications.- Plasmon Waveguides.- Transmission of Radiation Through Apertures and Films.- Enhancement of Emissive Processes and Nonlinearities.- Spectroscopy and Sensing.- Metamaterials and Imaging with Surface Plasmon Polaritons.- Concluding Remarks.

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Plasmonics: Fundamentals and Applications

Black carbon aerosol plays a unique and important role in Earth's climate system. Black carbon is a type of carbonaceous material with a unique combination of physical properties. This assessment provides an evaluation of black-carbon climate forcing that is comprehensive in its inclusion of all known and relevant processes and that is quantitative in providing best estimates and uncertainties of the main forcing terms: direct solar absorption; influence on liquid, mixed phase, and ice clouds; and deposition on snow and ice. These effects are calculated with climate models, but when possible, they are evaluated with both microphysical measurements and field observations. Predominant sources are combustion related, namely, fossil fuels for transportation, solid fuels for industrial and residential uses, and open burning of biomass. Total global emissions of black carbon using bottom-up inventory methods are 7500 Gg yr−1 in the year 2000 with an uncertainty range of 2000 to 29000. However, global atmospheric absorption attributable to black carbon is too low in many models and should be increased by a factor of almost 3. After this scaling, the best estimate for the industrial-era (1750 to 2005) direct radiative forcing of atmospheric black carbon is +0.71 W m−2 with 90% uncertainty bounds of (+0.08, +1.27) W m−2. Total direct forcing by all black carbon sources, without subtracting the preindustrial background, is estimated as +0.88 (+0.17, +1.48) W m−2. Direct radiative forcing alone does not capture important rapid adjustment mechanisms. A framework is described and used for quantifying climate forcings, including rapid adjustments. The best estimate of industrial-era climate forcing of black carbon through all forcing mechanisms, including clouds and cryosphere forcing, is +1.1 W m−2 with 90% uncertainty bounds of +0.17 to +2.1 W m−2. Thus, there is a very high probability that black carbon emissions, independent of co-emitted species, have a positive forcing and warm the climate. We estimate that black carbon, with a total climate forcing of +1.1 W m−2, is the second most important human emission in terms of its climate forcing in the present-day atmosphere; only carbon dioxide is estimated to have a greater forcing. Sources that emit black carbon also emit other short-lived species that may either cool or warm climate. Climate forcings from co-emitted species are estimated and used in the framework described herein. When the principal effects of short-lived co-emissions, including cooling agents such as sulfur dioxide, are included in net forcing, energy-related sources (fossil fuel and biofuel) have an industrial-era climate forcing of +0.22 (−0.50 to +1.08) W m−2 during the first year after emission. For a few of these sources, such as diesel engines and possibly residential biofuels, warming is strong enough that eliminating all short-lived emissions from these sources would reduce net climate forcing (i.e., produce cooling). When open burning emissions, which emit high levels of organic matter, are included in the total, the best estimate of net industrial-era climate forcing by all short-lived species from black-carbon-rich sources becomes slightly negative (−0.06 W m−2 with 90% uncertainty bounds of −1.45 to +1.29 W m−2). The uncertainties in net climate forcing from black-carbon-rich sources are substantial, largely due to lack of knowledge about cloud interactions with both black carbon and co-emitted organic carbon. In prioritizing potential black-carbon mitigation actions, non-science factors, such as technical feasibility, costs, policy design, and implementation feasibility play important roles. The major sources of black carbon are presently in different stages with regard to the feasibility for near-term mitigation. This assessment, by evaluating the large number and complexity of the associated physical and radiative processes in black-carbon climate forcing, sets a baseline from which to improve future climate forcing estimates.

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Bounding the role of black carbon in the climate system: A scientific assessment

1. Introduction 2. Theoretical foundations 3. Propagation and focusing of optical fields 4. Spatial resolution and position accuracy 5. Nanoscale optical microscopy 6. Near-field optical probes 7. Probe-sample distance control 8. Light emission and optical interaction in nanoscale environments 9. Quantum emitters 10. Dipole emission near planar interfaces 11. Photonic crystals and resonators 12. Surface plasmons 13. Forces in confined fields 14. Fluctuation-induced phenomena 15. Theoretical methods in nano-optics Appendices Index.

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Principles of nano-optics

This tutorial is devoted to the Maxwell Garnett approximation and related theories. Topics covered in this first, introductory part of the tutorial include the Lorentz local field correction, the Clausius–Mossotti relation and its role in the modern numerical technique known as the discrete dipole approximation, the Maxwell Garnett mixing formula for isotropic and anisotropic media, multicomponent mixtures and the Bruggeman equation, the concept of smooth field, and Wiener and Bergman–Milton bounds.

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Introduction to the Maxwell Garnett approximation: tutorial.

Local spectra of self-affine clusters of silver colloid particles recorded with subwavelength resolution by near-field spectroscopy are reported. Spectra were also simulated computationally. The observed and calculated near-field spectra consist of several resonances with highly location-dependent frequencies. The most highly resolved of these resonances correspond to individual surface plasmon (SP) normal modes. All of these features are only observable in the near field. Both theory and experiment also show that when excited by light in the SP region of the spectrum, the field-intensity distribution in the near field is very heterogeneous with most of the excitation concentrated in ``hot spots'' on the cluster surface that are strongly excitation-wavelength dependent. This field-intensity localization provides a rationale for recently reported surface-enhanced Raman enhancements in excess of ${10}^{10}.$

Near-field optical spectroscopy of individual surface-plasmon modes in colloid clusters

Strong fluctuations of local fields may result in very large optical nonlinearities in small-particle composites. Enhancement associated with particle clustering is found for a number of optical processes, including four-wave mixing (FWM), third-harmonic generation (THG), Raman scattering, and nonlinear refraction and absorption in Kerr media. Field fluctuations and optical nonlinear susceptibilities are especially large in fractal clusters. The enhancement of optical processes is expressed in terms of the resonant linear absorption by collective dipolar eigenmodes in a cluster, and quality factors, q, of the modes (q\ensuremath{\gg}1). It is shown that the susceptibility of a composite material consisting of random small-particle clusters is proportional to ${\mathit{q}}^{3}$ for Raman scattering and the Kerr optical nonlinearity, and to ${\mathit{q}}^{4}$ and ${\mathit{q}}^{6}$ for THG and FWM, respectively. For all of these processes, a spectral dependence of the effective susceptibility is found. Broad-scale numerical simulations of the optical response in small-particle composites are performed to complement the theory. The simulations are in reasonable agreement with available experimental data. \textcopyright{} 1996 The American Physical Society.

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Small-particle composites. I. Linear optical properties

The coupled-dipole approximation is used to study theoretically the scattering of light from an infinite linear one-dimensional chain of monomers interacting via dipole fields. It is shown that if the distance between monomers is much less then λ, the shift of optical resonances is governed by only interaction in the near-zone, and the spectral width of resonances, on the contrary, by interaction in all zones (near, intermediate and far-zone). The condition under which the developed theory yields correct depolarization coefficients of a dielectric cylinder in a quasi-static case is found. The extinction cross-section is calculated as a function of driving frequency.

Coupled-dipole Approach to Scattering of Light from a One-dimensional Periodic Dipole Structure

The origin and properties of non-Lorentzian spectral lines in linear chains of nanospheres are discussed. The lines are shown to be super-exponentially narrow with the characteristic width exp[−C(h/a)3] where C is a numerical constant, h the spacing between the nanospheres in the chain and a the sphere radius. The fine structure of these spectral lines is also investigated.

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Vadim A. Markel

Papers

Introduction to the Maxwell Garnett approximation: tutorial.

Near-field optical spectroscopy of individual surface-plasmon modes in colloid clusters

Small-particle composites. I. Linear optical properties

Coupled-dipole Approach to Scattering of Light from a One-dimensional Periodic Dipole Structure

Divergence of dipole sums and the nature of non-Lorentzian exponentially narrow resonances in one-dimensional periodic arrays of nanospheres