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Journal of the Optical Society of America B

Spectral emission imaging to map photonic properties below the crystal surface of 3D photonic crystals

Christian Blum, Allard P. Mosk, Cees Otto, Willem L. Vos, Vinod Subramaniam

Published Oct 16, 2009• 5 citations
Publisher

Abstract

We present the application of spectral emission imaging microscopy as a method to quantitatively map photonic properties from below the surface of strongly interacting photonic three-dimensional (3D) crystals. We excite emission from emitters deep inside a photonic crystal and record the local emission spectra with micrometer lateral resolution. The recorded directional emission spectra are modified by Bragg diffraction, which we use to determine the local stop-band attenuation, center frequency, and width. Assembling the values obtained into spatial maps yields detailed access to the distributions of the local photonic properties below the crystal surface. We demonstrate this approach by analyzing the emission from the fluorescent protein DsRed2 infiltrated inside self-organized 3D titanium dioxide inverse opals.

DOI
10.1364/josab.26.002101

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We present the application of spectral emission imaging microscopy as a method to quantitatively map photonic properties from below the surface of strongly interacting photonic three-dimensional (3D) crystals. We excite emission from emitters deep inside a photonic crystal and record the local emission spectra with micrometer lateral resolution. The recorded directional emission spectra are modified by Bragg diffraction, which we use to determine the local stop-band attenuation, center frequency, and width. Assembling the values obtained into spatial maps yields detailed access to the distributions of the local photonic properties below the crystal surface. We demonstrate this approach by analyzing the emission from the fluorescent protein DsRed2 infiltrated inside self-organized 3D titanium dioxide inverse opals.
Performing fluorescence wide-field microscopy we have imaged single semiconductor quantum dots deep inside a 3-dimensional photonic crystal prepared from colloidal polymer beads. Exploring the emission diffraction patterns in defocused images of quantum dots we demonstrate that the direction-dependent photonic stop band imprints an anisotropy to the angular emission of a single quantum dot. Hence a single, quasi-point-like emitter is manipulated to radiate its photons only to certain well-defined directions by means of the anisotropic light propagation in photonic crystals. The experiments thus provide new routes to evaluate local, frequency selective optical properties in 3-dimensional photonic crystals employing single emitters.
Photonic crystals affect the photon emission of embedded emitters due to an altered local density of photon states (LDOS). We review the calculation of the LDOS from eigenmodes in photonic crystals and propose a rate equation model for fluorescent emitters to determine the changes in emission induced by the LDOS. We show how to calculate the modifications of three experimentally accessible characteristics: emission spectrum (spectral redistribution), emitter quantum yield, and fluorescence lifetime. As an example, we present numerical results for the emission of the dye Rhodamine B inside an opal photonic crystal. For such photonic crystals with small permittivity contrast, the LDOS is only weakly modified, resulting in rather small changes. We point out that in experiments, however, usually only part of the emitted light is detected, which can have a very different spectral distribution (e.g., due to a photonic band gap in the direction of detection). We demonstrate the calculation of this detected spectrum for a typical measurement setup. With this reasoning, we explain the previously not fully understood experimental observation that strong spectral modifications occurred, while at the same time only small changes in lifetime were found. With our approach, the mentioned effects can be quantitatively calculated for fluorescent emitters in any photonic crystal.
We have performed angle-resolved measurements of spontaneous-emission spectra from laser dyes and quantum dots in opal and inverse opal photonic crystals. Pronounced directional dependencies of the emission spectra are observed: angular ranges of strongly reduced emission adjoin with angular ranges of enhanced emission. It appears that emission from embedded light sources is affected both by the periodicity and by the structural imperfections of the crystals: the photons are Bragg diffracted by lattice planes and scattered by unavoidable structural disorder. Using a model comprising diffuse light transport and photonic band structure, we quantitatively explain the directional emission spectra. This work provides detailed understanding of the transport of spontaneously emitted light in real photonic crystals, which is essential in the interpretation of quantum optics in photonic-band-gap crystals and for applications wherein directional emission and total emission power are controlled.
The photonic dispersion, the group-velocity dispersion, the effective mass, refractive index, and the spectral distribution of the density of photonic states near the edge of the photonic stop band are numerically calculated in the one-dimensional model for photonic crystals based on synthetic opals. The fluorescence spectra of rhodamine 6G and 2,5-bis(2-benzoxazolyl)hydroquinone molecules infiltrated into a synthetic opal are measured. For both substances, it is observed that the spontaneous emission intensity in the range of the photonic stop band is appreciably suppressed. A blue shift of the fluorescence spectrum of rhodamine 6G molecules is revealed. Secondary emission of synthetic opals infiltrated with colloidal silver is observed in the Stokes range under excitation of opals by radiation at λ = 400 nm. The spectrum of the secondary emission is located in the range 450–590 nm, which contains the stop band and intervals near its edges.
We present the first experiments that demonstrate strong angle-independent modification of spontaneous emission spectra from laser dyes in photonic crystals, made of inverse opals in titania. We show that both the fluorescence quantum efficiency and weak disorder play a key role in interpreting the experimental data. We compare the angle-independent emission spectra of dye in photonic crystals with spectra from such crystals with much smaller lattice spacings, for which emission is in the long wavelength limit. The ratio of emission power spectra shows inhibition of emission up to a factor ∼ 5 over a large bandwidth of 13% of the first order Bragg resonance frequency. The inhibition shifts to increasing wavelength with the lattice parameter, confirming the photonic nature of the phenomenon. The center frequency and bandwidth of the inhibition agree with the calculated total density of states, but the measured inhibition of the vacuum fluctuations is much larger. This result is confirmed by experiments using different dyes. We likely probe the strongly modulated local photonic density of states, due to the spatially nonuniform distribution of dye molecules over the unit cell.