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Optica

Effects of resonant-laser excitation on the emission properties in a single quantum dot

Olivier Gazzano, T. Huber, Vivien Loo, S Yu Polyakov, Edward B. Flagg, Glenn S. Solomon

Published Mar 26, 2018• 14 citations
Publisher

Abstract

. This work further clarifies resonance fluorescence in solid-state systems and will aid in the further improvement of solid-state non-classical light sources.
DOI
10.1364/optica.5.000354

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Quantum optics provides a fundamental framework for understanding the interaction between light and matter at the quantum level. Recently, it has been shown that under incoherent pumping, the resonance fluorescence spectrum dramatically changes. Engineering the resonance fluorescence spectrum paves the way towards solid-state-based single-photon sources. In this paper, we start by reviewing and reproducing some of the results concerning the resonance fluorescence spectrum, single-photon sources, dressed-state lasers, and luminescence spectrum of a quantum dot in a microcavity. Photon correlations in quantum optical systems and spectral properties of radiation emitted by atomic and semiconductor systems interacting with external fields are investigated. The well known Mollow triplet structure of the emission spectrum is discussed, together with the role of dressed states in explaining the origin of the three spectral peaks. Furthermore, the luminescence spectra of quantum emitters coupled to microcavities are reviewed. The numerical results presented here contribute to the theoretical understanding of resonance fluorescence, photon correlations, and engineered emission in quantum optical systems. These studies highlight the rich physical properties arising from light matter interaction at the quantum level and demonstrate their relevance for emerging quantum technologies.
This thesis describes the first and second-order correlation measurements that were performed on a III-V self-assembled quantum dot weakly coupled to a H1 nanophotonic crystal cavity. The system has an exceptionally large Purcell factor, which enables new regimes of light-matter coupling to be explored. In particular, the Purcell effect enhances the radiative recombination rate by an unprecedented factor, allowing measurements to take advantage of the fast lifetime and broad, transform-limited linewidth of the excitons excited in the quantum dot. The main results of this thesis are presented in three chapters, which explore, respectively, the application of the system as a single-photon source, the interactions between the quantum dot excitons and their solid-state environment, and the effect of spectral filtering on resonance fluorescence photon statistics. None of these experiments would have been possible without the very large Purcell enhancement of the radiative emission from the quantum dot. In the first set of experiments, the emission properties of the cavity-coupled quantum dot under p-pulsed resonant excitation were investigated. Hanbury Brown and Twiss second-order correlation measurements were used to measure the single-photon purity of the quantum dot emission. Hong-Ou-Mandel measurements were performed to investigate the indistinguishability of the single-photons produced. The emission from the cavity-coupled dot was then investigated under continuous wave excitation. In the second set of experiments, first-order correlation measurements were made in conjunction with spectroscopic measurements to investigate the phonon sideband properties of the quantum dot, both under resonant and slightly detuned excitation. In the final set of measurements, spectral filtering was used to alter the photon statistics observed when measuring the resonance fluorescence from the cavity-coupled quantum dot. Here, the effect of filtering in both the weak and strong driving regimes was investigated by filtering both above and below the linewidth of the quantum dot.
The generation of non-classical states of light [1] is an important scientific challenge with many potential applications. For example, squeezed states of light [2] have generated much interest in the past decade, because measurements can be performed with noise levels that are lower than those available with classical light. A particularly novel non-classical source of light is a triggered single-photon source: a source that has the property to emit with a high degree of certainty one (and only one) photon at a user-specified time. Such a deterministic source of single photons can be important for quantum information processing [3], quantum cryptography [4] and certain quantum computation problems [5]. A single quantum emitter such as a molecule or an atom is a good potential source because it can emit only one photon at a time. The emitted light is antibunched [6, 7] and consists of single photons separated by random time intervals, which depend on the excited state lifetime and on the pumping rate. Thus triggered emission of single photons can be obtained with controlled excitation of a single emitter. The first demonstration of a single photons source [8] using a single molecule in a solid is based on a rapid adiabatic passage method [9] to excite the molecule. In the effective spin picture, the Bloch vector follows the driving magnetic field adiabatically if the laser-molecule frequency detuning is swept slowly through the resonance. Since the passage inverts the field, the system goes from the ground to the excited state. From this fluorescent state the molecule can emit only a single photon. The molecular resonance is swept by Stark effect at fixed laser frequency. This is done easily by applying a radio frequency electric field to the molecule. The results showed photon states with statistics that differ radically from those of coherent states. But this method requires cryogenic temperatures (2K) since narrow zero phonon lines are needed for the adiabatic following. At room temperature a source of triggered single photons based on the concept of pulsed optical excitation of a single highly fluorescent molecule has been demonstrated [10]. A short pulse of green laser light pumps the molecule from the ground state to a vibronically excited level of the first electronic excited state. After fast (ps) relaxation to the lowest electronic excited state, the molecule subsequently emits a single photon. A frequency-doubled mode-locked Nd-YAG laser is used to pump highly stable single terrylene molecules contained in a p-terphenyl molecular crystal where they are protected from exposure to diffusing quenchers (such as oxygen). The result shows that the photons are emitted after the laser pulses at times separated by the laser repetition time within the lifetime of terrylene in p-terphenyl. Since the pump pulse width is very short compared to the fluorescence lifetime, the probability of two (or more) photon emission per pulse is always zero. At the maximum laser power, 90% of the laser pulses lead to a single photon emission. The parameters of this source (repetition rate and single photon generation probability) were limited only by the laser system used; nevertheless, this performance already surpasses that of previous work. The high performance combined with the vanishing two photon emission probability and the simplicity of this source suggests that it can be considered for a variety of quantum optical experiments and for secure quantum cryptography [11]. Semiconductor quantum dots (QD) are other potential systems for single photon generation [12]. QDs are often referred to as “artificial atoms” because many of their optical properties, such as ultranarrow transitions, arise from discrete, atomic-like energy levels [13, 14]. To reinforce this analogy a study of the photon antibunching in this system was needed. QDs differ from atoms and molecules since the creation of multiple excitons is possible in QDs. Consequently, if two electron-hole pairs can radiatively recombine, the simultaneous emission of two photons from a QD is then possible. Thus different regimes of photon statistics were expected because the probability of multiple exciton creation depends on excitation intensity. The fluorescence intensity correlation function of a single CdSe quantum dot has been investigated [15] using a coincidence setup (start-stop experiment). A strong photon antibunching has been observed over a large range of intensities (0.1-100 kW/cm2). The lack of coincidence at zero time delay indicates a highly efficient Auger ionization process [16], which suppresses multi-photon emission in these colloidal quantum dots. This result shows that room temperature single photon sources can be achieved with colloidal nanoparticles.