Extinction, absorption, and scattering of light by plasmonic spheres embedded in an absorbing host medium

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发布日期 2021-09-15
DOI 10.1039/D1CP03057D
影响因子 3.676
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摘要

Although the general Lorenz–Mie formalism for spheres in an absorbing host has been developed, no correct analytical expressions in the small-particle limit have been published so far. Here, we derive two sets of analytical expressions for the extinction, absorption, and far- and near-field scattering cross sections of small particles embedded in an absorbing host. One set is a modification of the electrostatic approximation (EA) for an absorbing host, whereas the other represents an improved electrostatic approximation (IEA) based on the generalized Lorenz–Mie theory and a new form of Mie coefficients for the internal field expansion. To illustrate the accuracy of the derived approximations, we consider Au and Ag nanospheres embedded in model hosts (real part of the refractive index, 1.33; imaginary part, 0–0.3), in a lossless poly(methyl methacrylate) (PMMA), and a lossy poly(3-hexylthiophene) (P3HT) matrix. In general, the IEA cross sections agree with those calculated using Lorenz–Mie theory if the particle diameter is not greater than 50 nm. Two small-particle limits are found for the near-field scattering cross sections. When host absorption is negligible, the scattering efficiency scales as the fourth power of the size parameter. In contrast, for nonzero absorption, the scattering efficiency scales as the first power of the size parameter. For a spectrally independent host, an increase in host absorption broadens and suppresses plasmonic peaks. We found an exception to this general tendency for near-field scattering by small (10–50 nm) particles; for these, an increase in host absorption increases the scattering peak. This surprising behavior is explained analytically. For 10–30 nm Au particles in the PMMA and P3HT matrixes, the EA and IEA data perfectly agree with the exact Lorenz–Mie simulations, in contrast to the previously reported conclusions. In particular, replacing PMMA with P3HT shifts the plasmonic peaks of the 10 nm particles from 540 nm to 650 nm and strongly enhances near- and far-field scattering. However, far-field scattering does not contribute to the extinction derived from the generalized optical theorem.

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Physical Chemistry Chemical Physics

Physical Chemistry Chemical Physics
CiteScore: 5.5
自引率: 10.3%
年发文量: 3036

Physical Chemistry Chemical Physics (PCCP) is an international journal co-owned by 19 physical chemistry and physics societies from around the world. This journal publishes original, cutting-edge research in physical chemistry, chemical physics and biophysical chemistry. To be suitable for publication in PCCP, articles must include significant innovation and/or insight into physical chemistry; this is the most important criterion that reviewers and Editors will judge against when evaluating submissions. The journal has a broad scope and welcomes contributions spanning experiment, theory, computation and data science. Topical coverage includes spectroscopy, dynamics, kinetics, statistical mechanics, thermodynamics, electrochemistry, catalysis, surface science, quantum mechanics, quantum computing and machine learning. Interdisciplinary research areas such as polymers and soft matter, materials, nanoscience, energy, surfaces/interfaces, and biophysical chemistry are welcomed if they demonstrate significant innovation and/or insight into physical chemistry. Joined experimental/theoretical studies are particularly appreciated when complementary and based on up-to-date approaches.

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