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.
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.
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.
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.
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.
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.
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.