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International Conference on Transparent Optical Networks

Spontaneous Emission Properties of Single Emitters in Planar Photonic Crystals

Martina Gerken, Jurgen Muller, Rainer Bornemann, Georg Bastian, Uli Lemmer, Detlef Schelle, Markus Augustin, Ernst‐Bernhard Kley, Andreas Tünnermann

Published Jun 1, 2006• 0 citations
Publisher

Abstract

We investigate the quantum-optical interplay of two-dimensional (2D) planar photonic crystals with localized emitters. Due to the spatial variation of the photonic density of states in the photonic crystal unit cell the spontaneous emission properties dependent strongly on the location of the emitter. We infiltrate nanospheres doped with small dye molecules as localized probes into 2D hexagonal Nb2O5photonic crystals. Using spatially resolved spectroscopy and time correlated single photon counting direct measurements of the spontaneous emission properties of single, localized emitters are performed

DOI
10.1109/icton.2006.248317

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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.

physica status solidi (a)•Jun 1, 2003•38 citations
We investigate the quantum-optical interplay of two-dimensional (2D) planar photonic crystals with localized emitters. Due to the spatial variation of the photonic density of states in the photonic crystal unit cell the spontaneous emission properties dependent strongly on the location of the emitter. We infiltrate nanospheres doped with small dye molecules as localized probes into 2D hexagonal Nb2O5photonic crystals. Using spatially resolved spectroscopy and time correlated single photon counting direct measurements of the spontaneous emission properties of single, localized emitters are performed
Chapter 1 IntroductionUltimate inhibition of spontaneous emission can be achieved in artificial periodic structures with tailor-made forbidden frequency bands [5].These periodic structures known as photonic crystals consist of different dielectric materials, where the index of refraction varies on length scales comparable to the wavelength of light.Therefore, the periodicity of photonic crystals is about 1000 times as large as that of atomic crystals.Light with specific frequencies is forbidden to propagate along certain directions by wave interference, similarly to Bragg diffraction of x-rays in atomic crystals.Such forbidden frequency ranges are called stopgaps.The larger the contrast of the refractive index between the two materials of a photonic crystal, the more strongly light is influenced, and the broader the stopgaps become.It was predicted in 1987 that an extreme situation may be feasible when light cannot propagate along any direction [6, 7].This situation is called a photonic bandgap.Spontaneous emission is completely inhibited for frequencies inside such a bandgap and, conversely, strongly enhanced for frequencies outside the bandgap.Photonic crystals, therefore, provide an ultimate tool for manipulating with light, which is of extreme interest for scientists and engineers [8, 9].Recent advances in nanotechnology have resulted in ability to synthesize semiconductor structures with dimensions of a few nanometers.Due to the finite sizes, electron-hole pairs (excitons) can be confined in these nanostructures, which leads to discrete excitonic energy levels.The nanocrystals that confine excitons in spherical or circular spaces are known as quantum dots.The discrete structure of the energy levels results in advantageous optical properties of these nanocrystals: narrow and tunable emission spectra.The emission frequencies can be tuned by varying the nanocrystal size: the smaller the size, the higher the emission frequency.These properties make the nanocrystals very promising elementary emitters for new experiments and devices [10, 11]. Outline of the thesisThis thesis describes time-and angle-resolved experiments, in which effects of threedimensional (3D) photonic crystals on spontaneous emission of embedded light sources (quantum dots and dye molecules) were studied.The thesis is organized as follows:In Chapter 2 we review the theoretical basics of the interaction between light and matter.We discuss the factors triggering the process of spontaneous emission and consider in detail the time evolution of the excited state of the emitter that interacts with the quantized 1.
Spontaneous emission is one of the most fundamental out-of-equilibrium processes in which an excited quantum emitter relaxes to the ground state due to quantum fluctuations. In this process, a photon is emitted that can interact with other nearby emitters and establish quantum correlations between them, e.g., via super and subradiance effects. One way to modify these photon-mediated interactions is to alter the dipole radiation patterns of the emitter, e.g., by placing photonic crystals near them. One recent example is the generation of strong directional emission patterns - key to enhancing super and subradiance effects - in two dimensions by employing photonic crystals with band structures characterized by linear isofrequency contours and saddle points. However, these studies have predominantly used oversimplified toy models, overlooking the electromagnetic field's intricacies in actual materials, including aspects like geometrical dependencies, emitter positions, and polarization. Our study delves into the interaction between these directional emission patterns and the variables mentioned above, revealing the untapped potential to fine-tune collective quantum optical phenomena.
Photonic crystals (PCs) with relatively low dielectric contrast (i.e., with pseudogaps) have significant influence on the fluorescence decay of internal emitters. Fluorescence decays of ensembles of dye molecules measured at different positions in the PCs exhibit a nonexponential behavior, which is best fitted by a continuous distribution of decay rates. The most frequent decay rates of these distributions are smaller and their widths are narrower in a PC with a pseudogap acting in the emission range of the emitters than in a PC having the pseudogap out of this range. These experimental results have been well accounted for by calculations of the local density of states and rate constant for spontaneous emission.
Spontaneous emission is one of the most fundamental out-of-equilibrium processes in which an excited quantum emitter relaxes to the ground state due to quantum fluctuations. In this process, a photon is emitted that can interact with other nearby emitters and establish quantum correlations between them, e.g., via super and subradiance effects. One way to modify these photon-mediated interactions is to alter the dipole radiation patterns of the emitter, e.g., by placing photonic crystals near them. One recent example is the generation of strong directional emission patterns-key to enhancing super and subradiance effects-in two dimensions by employing photonic crystals with band structures characterized by linear isofrequency contours and saddle-points. However, these studies have predominantly used oversimplified toy models, overlooking the electromagnetic field's intricacies in actual materials, including aspects like geometrical dependencies, emitter positions, and polarization. Our study delves into the interaction between these directional emission patterns and the aforementioned variables, revealing the untapped potential to fine-tune collective quantum optical phenomena.
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.