Introduction The propagation of light in periodically ordered photonic crystals bears a strong analogy to the wave propagation of conduction electrons in atomic crystals. The development of Bloch modes and dispersion are determined by the interference of waves that are diffracted by lattice planes [19, 52]. The periodicity commensurate with the wavelength (a ≈ λ/2) gives rise to Bragg diffraction that is associated with frequency windows for which waves are forbidden to propagate in a particular direction. Such stop gaps have long been known to arise for electromagnetic waves, notably for X-rays in atomic crystals [214]. At optical frequencies, the stop gaps that occur in one-dimensional periodic structures, known as Bragg stacks, are widely used in optical laboratories as broadband highly reflecting dielectric mirrors [556]. The distinguishing feature of three-dimensional (3D) photonic crystals is that a common stop gap can be achieved for all directions and for all polarizations simultaneously: the widely pursued 3D photonic band gap . Historically a 3D band gap has never been considered for the propagation of X-rays in periodic media, since a gap requires a high refractive index contrast of order unity, whereas the refractive index varies by less then 10 −4 in the X-ray range. At frequencies inside the 3D photonic band gap, the density of optical states (DOS) completely vanishes. As the density of states can also be interpreted as the density of vacuum fluctuations [334], a 3D band gap thus serves as an effective shield to these fluctuations. The total absence of optical modes in a photonic band gap has implications beyond classical optics that break the analogy between the behavior of light in photonic crystals and the behavior of electrons in atomic crystals. 3D photonic band gap crystals play an important role in cavity quantum electrodynamics (cQED) [64, 549], where they offer at least five prospects for new physics. Firstly, probably the most eagerly pursued phenomenon is the complete inhibition of spontaneous emission: an excited quantum emitter – such as an atom, molecule, or quantum dot – embedded in a crystal with its transition frequency tuned to within the 3D band gap remains forever excited since it cannot decay to the ground state by emitting a photon.
Introduction The propagation of light in periodically ordered photonic crystals bears a strong analogy to the wave propagation of conduction electrons in atomic crystals. The development of Bloch modes and dispersion are determined by the interference of waves that are diffracted by lattice planes [19, 52]. The periodicity commensurate with the wavelength (a ≈ λ/2) gives rise to Bragg diffraction that is associated with frequency windows for which waves are forbidden to propagate in a particular direction. Such stop gaps have long been known to arise for electromagnetic waves, notably for X-rays in atomic crystals [214]. At optical frequencies, the stop gaps that occur in one-dimensional periodic structures, known as Bragg stacks, are widely used in optical laboratories as broadband highly reflecting dielectric mirrors [556]. The distinguishing feature of three-dimensional (3D) photonic crystals is that a common stop gap can be achieved for all directions and for all polarizations simultaneously: the widely pursued 3D photonic band gap . Historically a 3D band gap has never been considered for the propagation of X-rays in periodic media, since a gap requires a high refractive index contrast of order unity, whereas the refractive index varies by less then 10 −4 in the X-ray range. At frequencies inside the 3D photonic band gap, the density of optical states (DOS) completely vanishes. As the density of states can also be interpreted as the density of vacuum fluctuations [334], a 3D band gap thus serves as an effective shield to these fluctuations. The total absence of optical modes in a photonic band gap has implications beyond classical optics that break the analogy between the behavior of light in photonic crystals and the behavior of electrons in atomic crystals. 3D photonic band gap crystals play an important role in cavity quantum electrodynamics (cQED) [64, 549], where they offer at least five prospects for new physics. Firstly, probably the most eagerly pursued phenomenon is the complete inhibition of spontaneous emission: an excited quantum emitter – such as an atom, molecule, or quantum dot – embedded in a crystal with its transition frequency tuned to within the 3D band gap remains forever excited since it cannot decay to the ground state by emitting a photon.
This paper gives an overview of recent work on three-dimensional (3D) photonic crystals with a "full and complete" 3D photonic band gap. We review five main aspects: 1) spontaneous emission inhibition, 2) spatial localization of light within a tiny nanoscale volume (aka "a nanobox for light"), 3) the introduction of a gain medium leading to thresholdless lasers, 4) breaking of the weak-coupling approximation of cavity QED, both in the frequency and in the time-domain, 5) decoherence, in particular the shielding of vacuum fluctuations by a 3D photonic bandgap. In addition, we list and evaluate all known photonic crystal structures with a demonstrated 3D band gap.
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.
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.
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).
Photonic crystals (PCs) are periodic systems that consist of dielectrics with different refractive indices. Photonic crystals have many potential technological applications. These applications are mainly based on the photonic bang gap effect. However the band gap is not only effect that follows from the periodic changing of the refractive index in the photonic crystal. The periodic change of the photon-matter interaction in photonic crystal medium gives rise to the fact that the mass of an electron in the photonic crystal must differ from its mass in vacuum. Anisotropy of a photonic crystal results in the dependence of the electromagnetic mass correction on the orientation of the electron momentum in a photonic crystal. This orientation dependence in turn gives rise to the significant correction to the transition frequencies in an atom placed in air voids of a photonic crystal. These corrections are shown to be comparable to the atomic optical frequencies. This effect allows one to control the structure of the atomic energy levels and hence to control resonance processes. It can serve as the basis for new line spectrum sources. The effect provides new ways of realization of quantum interference between decay channels that can be important for quantum information science.