Hybridized/coupled multiple resonances in nacre

Seung Ho Choi and Young L. Kim

Phys. Rev. B 89, 035115 – Published 10 January 2014

Abstract

We report that nacre (also known as mother-of-pearl), a wondrous nanocomposite found in nature, is a rich photonic nanomaterial allowing the experimental realization of collective excitation and light amplification via coupled states. Localized modes in three-dimensional complex media are typically isolated in frequency and space. However, multiple local resonances can be hybridized in multilayered nanostructures of nacre so that the effective cavity size for efficient disordered resonators is scaled up. Localized modes in hybridized states in nacre are overlapped in frequency with similar shapes in space, thus being collectively excited and synergistically amplified. These hybridized states boost light amplification, leading to stable and regular multimode lasing at low excitation energy. The simplicity of ameliorating disordered resonators by mimicking nacre can further serve as platforms for developing cost-effective photonic systems and provide materials for fundamental research on complex media.

Received 9 July 2013
Revised 29 August 2013

DOI:https://doi.org/10.1103/PhysRevB.89.035115

Authors & Affiliations

Seung Ho Choi and Young L. Kim^*

Weldon School of Biomedical Engineering, Purdue University, 206 S. Martin Jischke Drive, West Lafayette, Indiana 47907, USA

^*youngkim@purdue.edu

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Issue

Vol. 89, Iss. 3 — 15 January 2014

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Images

Figure 1
Nanostructures and photonic properties of Haliotis fulgens (green abalone). (a) Confocal fluorescence microscopy image of nacre infiltrated with rhodamine 6G (Rh6G) after deproteinization. Inset: Photograph of the original abalone shell. (b) Scanning electron microscopy (SEM) image of a brick-mortar nanostructure in nacre. (c) The molecular architecture of aragonite viewed from the $C$ axis (top) and off the $C$ axis (bottom). (d) Photograph of deproteinized nacre. (e) Reflectance spectra (spectral resolution = 2 nm) from deproteinized nacre, averaged from ∼100 spectra.
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Figure 2
Numerical experiments of hybridized/coupled states and light amplification in 1D disordered systems. (a) Schematic diagram of the experimental configuration. (b) Dispersion curves of aragonite and gap layers. (c) Real and imaginary parts of susceptibility of gain $χ_{g}$ (λ).
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Figure 3
Formation of hybridized states and isolated modes in nacre and amplification with gain. (a) Transmittance spectra $T$ and log $_{10}$ ( $T$ ) (solid and dashed line in upper panel, respectively). Internal field intensity $I$ (lower panel) of quasimodes (without gain). The white solid line is a phase change in the transmittance spectra. (b) Emission spectra $I_{e}$ (upper panel) and internal field intensity $I$ (lower panel) of lasing modes (with gain). (c) Spatial profiles of integrated quasimodes (green curve) and lasing modes (blue curve) horizontally shifted for visual clarity. (d) $I_{e}$ of lasing modes as a function of the density of excited atoms $N_{ex}$ . (e) Emission intensity at the threshold of $I_{e}^{th}$ (lasing mode) versus $T$ (quasimode) from 32 different disorder configurations. Inset: Occurrence probabilities of two different hybridized states and isolated modes. (f) and (g) Characteristics of $I_{e}^{th}$ (lasing mode) versus $T$ of different states and modes. The colors of the data points in (e) match with the states in the horizontal axes of (f) and (g). * denotes statistically significant differences. The error bars are SDs.
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Figure 4
Photoluminescence experiments using abalone nacre. (a) Schematic diagram of the experimental setup. (b) Integrated emission intensity from Rh6G-infilterated nacre as the excitation energy increases. The intensity is integrated within the same wavelength range. (c) and (d) Pseudocolor microscopic images of spatial fields averaged over wavelength through the 10-nm (FWHM) bandwidth filter: (c) Below the threshold (=0.56 μJ/pulse) and (d) above the threshold (=1.98 μJ/pulse). The solid curves are longitudinal intensity distributions at different horizontal cross sections. (e) Emission spectra as the excitation energy increases. The spectra are also projected onto the grayscale map.
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Figure 5
Nacre lasers using erythrosine. Representative multimode emission spectrum above the threshold (excitation energy = 12.4 μJ/pulse as indicated the red dot in the right inset). Left inset: Structural formula of erythrosine and photography of erythrosine powders. Right inset: Emission intensity integrated within λ = 547–572 nm as a function of the excitation energy.
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Figure 6
Spectral characteristics of lasing emission in nacre originating from hybridized multiple resonances at relatively low excitation energy. (a) Emission spectra at the excitation energy of 15–20 μJ/pulse above the lasing thresholds. (b) Wavelength spacing Δλ and frequency spacing Δω between adjacent peaks, respectively.
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