In the first part of this introductory review we outline the developments in photonic band gap materials from the physics of photonic band gap formation to the fabrication and potential applications of photonic crystals. We briefly describe the analogies between electron and photon localization, present a simple model of a band structure calculation and describe some of the techniques used for fabricating photonic crystals. Also some applications in the field of photonics and optical circuitry are briefly presented. In the second part, we discuss the consequences for the interaction between an atom and the light field when the former is embedded in photonic crystals of a specific type, exhibiting a specific form of a gap in the density of states. We first briefly review the standard treatment (Weisskopf – Wigner theory) in describing the dynamics of spontaneous emission in free space from first principles, and then proceed by explaining the alterations needed to properly treat the case of a two-level atom embedded in a photonic band gap material.
In the first part of this introductory review we outline the developments in photonic band gap materials from the physics of photonic band gap formation to the fabrication and potential applications of photonic crystals. We briefly describe the analogies between electron and photon localization, present a simple model of a band structure calculation and describe some of the techniques used for fabricating photonic crystals. Also some applications in the field of photonics and optical circuitry are briefly presented. In the second part, we discuss the consequences for the interaction between an atom and the light field when the former is embedded in photonic crystals of a specific type, exhibiting a specific form of a gap in the density of states. We first briefly review the standard treatment (Weisskopf – Wigner theory) in describing the dynamics of spontaneous emission in free space from first principles, and then proceed by explaining the alterations needed to properly treat the case of a two-level atom embedded in a photonic band gap material.
In certain three-dimensional crystals, a frequency range exist for all polarizations for which light is not allowed to propagate in any direction, called the 3D photonic band gap: a frequency range where the density of vacuum fluctuations vanishes in an ideal infinitely large and perfect system. The complete absence of vacuum fluctuations can be interpreted as zero density of states and vice versa. It is well known that the characteristics of spontaneous emission of light depend strongly on the environment of the light source. According to quantum electrodynamics, the emission rate of a two-level quantum emitter as described by Fermi’s “golden rule”, is factorized into one part describing the emitter’s properties and a second part describing the effect of the environment on the light field via the local density of optical state (LDOS). The radiative decay rate of the emitters is proportional to the LDOS. The absence of vacuum fluctuations or the zero LDOS leads to complete inhibition of the spontaneous emission. While many great advances towards a band gap have been made, no complete inhibition has ever been observed to date. In this thesis, for the first time, we have studied the spontaneous emission of PbS quantum dots inside real 3D photonic band gap crystal as a function of frequency throughout the band gap. In our experiments we have observed an inhibited emission of 18x in the band gap. The time-resolved decay curves show evidence for intriguing finite-size effects whereby vacuum fluctuations tunnel into the band gap. Unfortunately, most theories assume crystals of infinite extent, where the inhibition in the band gap is also infinite, as vacuum fluctuations don’t exist inside the crystal. Here we propose an original model to calculate the LDOS in the band gap of a finite photonic crystal based on tunneling of the vacuum fluctuations into the crystal. We validate our model for the one-dimensional situation with a direct comparison to the analytic calculations which exist for one-dimensional photonic crystals. For three dimensional crystals, the theory shows an excellent match to the experiment.
Photonic crystals are optical materials that have an intricate structure with length scales of the order of the wavelength of light. The flow of photons is controlled in a manner analogous to how electrons propagate through semiconductor crystals, i.e., by Bragg diffraction and the formation of band structures. If the interaction between light and matter is made strong, multiple diffraction and multiple scattering effects dominate. A main research goal is the realization of a "photonic band gap", that is, a frequency range for which no light can propagate in a crystal in any direction, which causes radical modifications of the density of radiative states. Important consequences of photonic band gaps are the complete control over spontaneous and stimulated emission of light, as well as over the propagation of light, in particular photon localization. This opens up the possibility to achieve a "cage for light": trap photons and do with them whatever one chooses. In this talk we will also review means for making such structures, and recent experimental advances in optical experiments.
Optical phenomena in materials with a space modulation of dielectric constant at distances close to the light wavelengths (so called photonic band-gap structures or photonic crystals) are of a great interest now because of the existence of band gaps in their photonic band structure (Bykov, 1972; Yablonovitch, 1987; John, 1987). These band gaps represent frequency regions where electromagnetic waves are forbidden, irrespective of the spatial propagation directions. Inside the band gaps, the photon density of states is equal to zero and so the emission of light sources embedded in these crystals should be inhibited in these spectral regions (Vats et al., 2002). Since the time the effect is predicted, many experiments have been devoted to studies of spontaneous emission of molecules embedded in photonic crystals (Gaponenko et al., 1999; Gorelik, 2007). Typical structures of photonic crystals and calculations of corresponding photonic band structures are presented in a book by Prof. Joannopoulos (Joannopoulos et al., 2008). Besides the emission inhibition effect, a number of new optical phenomena in 3D photonic crystals, interesting from the applied point of view, are under intensive study now. The main research directions are the following: Effects of light localisation (John, 1987; Kaliteevskii et al., 2005; Vignolini et al., 2008). Radiation of photonic crystals filled with organic (rhodamine 6G, 1,8-naphthoylene1’,2’-benzimidazole, stilbene) and inorganic (ZnO, ZnS, rare-earth ions Eu3+, Tb3+, Er3+) luminophores near by the edges of photonic band-gap (Gaponenko et al., 1999; Aliev et al., 2002; Emel’chenko et al., 2005; Li et al., 2007). Radiation of CdTe, CdSe/ZnS quantum dots in photonic crystal volume (Gruzintsev et al., 2009; Ambrozevich et al., 2009). Quantum optics phenomena in nano-structured materials based on photonic crystals and nonlinear optical substances (Lin & Vuckovic, 2010). Effects of the radiation field amplification in photonic crystals (Lin & Vuckovic, 2010). Increase of solar cells efficiency with the use of photonic crystals (Florescu et al., 2007).
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.
Quantum electrodynamics of atom spontaneous emission from a three-dimensional photonic crystal is studied in a full vectorial framework. The electromagnetic fields are quantized via solving the eigenproblem of photonic crystals with use of a plane-wave expansion method. It is found that the photon density of states and local density of states (LDOS) with a full band gap vary slowly near the edge of band gap, in significant contrast to the singular character predicted by the previous isotropic model. Therefore, the spontaneous emission can be solved by conventional Weisskopf-Wigner approximate theory, which yields a pure exponentially decaying behavior with a rate proportional to the LDOS.