The advent of quantum computation promises exciting advances, not only in fields like medicine and metrology, but many industries that rely on parameter-heavy calculations or simulation of molecular interaction. At the same time Shor's algorithm for quantum computers presents a threat to current asymmetric encryption protocols used in everyday communication. Flying qubits, i.e. single-photons, can help mitigate this problem via quantum key distribution, which is insusceptible to an increase in computational power. In addition, they can link quantum computers, forming a quantum network, so that quantum states can be transmitted between them. Sources of flying qubits need good performance in key metrics like single--photon purity, repetition rate, indistinguishability and brightness to become useful in these applications. They should ideally emit strongly entangled pairs of photons and be matched to other quantum technologies in bandwidth and emission energy. In this thesis the emission characteristics of single epitaxial quantum dots, the single-photon source of our choice, are investigated. Strongly entangled photon-pair emission is demonstrated for three different quantum-dot systems: InAsP quantum dots embedded in nanowire waveguides, suitable for integration into photonic circuits, show emission of single photons and entangled photon pairs under non-resonant and quasi-resonant excitation. Violation of Bell's inequality is demonstrated using the traditional set of polarization angles. GaAs quantum dots grown in droplet--etched nanoholes are tested with two resonant excitation methods: Using resonance fluorescence, near-unity indistinguishability and re-excitation limited single-photon purity, albeit not simultaneously with laser-inherited bandwidth, are measured. Using two-photon resonant excitation we set a new standard for single-photon purity, can generate pairs of entangled photons but suffer from reduced indistinguishability. In addition, nanofabrication of paraboloid shaped reflectors for enhanced extraction efficiency of photons and strain-tuning of the emission energy into resonance with the 87Rb D1-line are demonstrated. Strain-tunable InAs quantum dots emitting in the telecom C-band are investigated under above-band excitation and two different resonant two-photon excitation techniques, all of which cause pure single-photon emission. Using the robust phonon-assisted two-photon excitation technique, close-to ideal entangled photon-pair emission is demonstrated. For many of these findings photon arrival times were recorded over many hours with temporal precision on the order of 10 ps. We have developed a user-friendly, yet versatile piece of software in order to extract as much information as possible from this vast amount of data. These results will facilitate integration of quantum dot based single- and entangled-photon sources into future quantum networks and quantum key distribution systems.
The advent of quantum computation promises exciting advances, not only in fields like medicine and metrology, but many industries that rely on parameter-heavy calculations or simulation of molecular interaction. At the same time Shor's algorithm for quantum computers presents a threat to current asymmetric encryption protocols used in everyday communication. Flying qubits, i.e. single-photons, can help mitigate this problem via quantum key distribution, which is insusceptible to an increase in computational power. In addition, they can link quantum computers, forming a quantum network, so that quantum states can be transmitted between them. Sources of flying qubits need good performance in key metrics like single--photon purity, repetition rate, indistinguishability and brightness to become useful in these applications. They should ideally emit strongly entangled pairs of photons and be matched to other quantum technologies in bandwidth and emission energy. In this thesis the emission characteristics of single epitaxial quantum dots, the single-photon source of our choice, are investigated. Strongly entangled photon-pair emission is demonstrated for three different quantum-dot systems: InAsP quantum dots embedded in nanowire waveguides, suitable for integration into photonic circuits, show emission of single photons and entangled photon pairs under non-resonant and quasi-resonant excitation. Violation of Bell's inequality is demonstrated using the traditional set of polarization angles. GaAs quantum dots grown in droplet--etched nanoholes are tested with two resonant excitation methods: Using resonance fluorescence, near-unity indistinguishability and re-excitation limited single-photon purity, albeit not simultaneously with laser-inherited bandwidth, are measured. Using two-photon resonant excitation we set a new standard for single-photon purity, can generate pairs of entangled photons but suffer from reduced indistinguishability. In addition, nanofabrication of paraboloid shaped reflectors for enhanced extraction efficiency of photons and strain-tuning of the emission energy into resonance with the 87Rb D1-line are demonstrated. Strain-tunable InAs quantum dots emitting in the telecom C-band are investigated under above-band excitation and two different resonant two-photon excitation techniques, all of which cause pure single-photon emission. Using the robust phonon-assisted two-photon excitation technique, close-to ideal entangled photon-pair emission is demonstrated. For many of these findings photon arrival times were recorded over many hours with temporal precision on the order of 10 ps. We have developed a user-friendly, yet versatile piece of software in order to extract as much information as possible from this vast amount of data. These results will facilitate integration of quantum dot based single- and entangled-photon sources into future quantum networks and quantum key distribution systems.
In the fields of quantum communications and quantum computing, the transmission of information using single photons guarantees the security of the communication and enables calculations that would be impossible with our "classical" computers. One of the key elements in implementing such protocols is the photon source. It must emit, on demand, one and only one photon with specific quantum properties.The aim of this project is to characterise a source of single and indistinguishable photons, designed and manufactured at CEA-Grenoble, and consisting of an indium arsenide (InAs) semiconductor quantum dot integrated into a gallium arsenide (GaAs) nanocavity. With its low quality factor, the nanocavity enables photons to be extracted efficiently over a wide range of wavelengths (30nm). In addition, thanks to its small mode volume, the spontaneous emission of quantum dots within it can be accelerated by Purcell effect (Purcell factor up to 6).In this manuscript, we first detail the implementation and the optimisation of the experimental setups used to characterise the photons emitted by our sample : microphotoluminescence, radiative lifetime measurement, Hanbury-Brown and Twiss (HBT) experiment and Hong-Ou-Mandel (HOM) experiment. Then, we present the experimental results obtained for photons emitted by two distinct quantum dots : One containing neutral exciton states, and the second, containing a charged exciton state. In order to photo-create these exciton states in the quantum dots, two pulsed optical excitation schemes were implemented: the two-photon resonant excitation of the neutral biexciton, and the phonon-assisted quasi-resonant excitation of the neutral and charged excitons. We present the measurement of the three figures of merit of a single photon source for these two quantum dots : the brightness, the single-photon purity and the indistinguishability of the emitted photons. In a second phase, we will focus on the charged exciton state and measure the profile of its emission line and its autocorrelation function under continuous resonant excitation. These results, achieved within the nano-photonics group of the University of Basel, constitute the first demonstration of continuous excitation on these nanostructures, which is a good surprise given their small size.Finally, we will look at the effects of the application of mechanical stress on the energy separation of the two neutral exciton states, known as the "fine structure splitting" (FSS). During the radiative cascade of the neutral biexciton state, the two photons emitted are entangled in polarisation, and the fidelity of the entanglement depends in particular on the FSS. Here, we will consider a second sample, where the InAs quantum dots are embedded in a GaAs photonic nanowire. By bending the nanowire, mechanical stresses are applied to the quantum dots, which will modify the energy of the exciton states. We will present an experimental study aimed at observing a possible effect on the fine structure splitting.In conclusion, we have developed and optimised various experimental setups for characterising photon sources for applications in the fields of quantum communications and quantum computing. For a first version of these photonic nanostructures, the brightness, the single-photon purity and the indistinguishability of the photons emitted by our quantum dots integrated into nanocavities are very encouraging for the future. The next objectives are to improve the nanocavities and to characterise the decoherence phenomena and the mechanical coupling between the quantum dots and these nanostructures.
On demand single-photon and entangled-photon sources are key building-blocks for many proposed photonic quantum technologies. For practical device applications, epitaxially grown quantum dots (QDs) are of increasing importance due to their bright photon emission with sharp line width. Particularly, they are solid-state systems and can be easily embedded within a light-emitting diode (LED) to achieve electrically driven sources. Therefore, one would expect a full-fledged optoelectronic quantum network that is running on macroscopically separated, QD-based single- and entangled-photon devices. An all-electrically operated wavelength-tunable on demand single-photon source (SPS) is demonstrated first. The device consists of a LED in the form of self-assembled InGaAs QDs containing nanomembrane integrated onto a piezoelectric crystal. Triggered single photons are generated via injection of ultra-short electrical pulses into the diode, while their energy can be precisely tuned over a broad range of about 4.8 meV by varying the voltage applied to the piezoelectric crystal. High speed operation of this single-photon emitting diode up to 0.8 GHz is demonstrated. In the second part of this thesis, a fast strain-tunable entangled-light-emitting diode (ELED) is demonstrated. It has been shown that the fine structure splitting of the exciton can be effectively overcome by employing a specific anisotropic strain field. By injecting ultra-fast electrical pulses to the diode, electrically triggered entangled-photon emission with high degree of entanglement is successfully realized. A statistical investigation reveals that more than 30% of the QDs in the strain-tunable quantum LED emit polarization-entangled photon-pairs with entanglement-fidelities up to f+ = 0.83(5). Driven at the highest operation speed ever reported so far (400 MHz), the strain-tunable quantum LED emerges as unique devices for high-data rate entangled-photon applications. In the end of this thesis, on demand and wavelength-tunable LH single-photon emission from strain engineered GaAs QDs is demonstrated. Fourier-transform spectroscopy is performed, from which the coherence time of the LH single-photon emission is studied. It is envisioned that this new type of LH exciton-based SPS can be applied to realize an all-semiconductor based quantum interface in the foreseeable distributed quantum networks.
In the pursuit of developing a quantum information network, photons appear to be the most convenient carriers to interconnect distant ports. The need to get on-demand single photons that is one and only one photon, with a high reliability, is the main driving force for the development of bright solid-state sources. One important parameter is the brightness defined as the probability that one collected pulse contains a single photon. For some applications like quantum information processing or long distance quantum communications, the emitted single photons must be also indistinguishable, so that can make use of their quantum interference to implement effective photon-photon interactions. To reach the ideal source of single and indistinguishable photons, different systems are explored : defects in diamond (NV centers), trapped atoms or ions, single molecules or semiconductor quantum dots.By coupling a semiconductor quantum dot to an optical cavity, the spontaneous emission of the emitter can be modified to obtain bright single-photon sources. An innovative technique was developed by Pr. Pascale Senellart and her team at the Laboratory of Photonics and Nanostructures (LPN) from CNRS that allows making such sources in a very reproducible way.This work explores the performance of single quantum dot coupled to micropillars. Various techniques are used in order to increase the single photon purity and indistinguishability while keeping a high source brightness. First, the cavity was modified using an adiabatic architecture such that a strong acceleration of the spontaneous emission was implemented. Then, a technique to apply an electric bias on the micropillars has been developed. The combination of the electric bias with a resonant optical excitation of the quantum dot allows to generation purely indistinguishable photons with a high brightness.The results developed in this thesis open a vast field of novel applications in quantum technologies, from quantum cryptography, metrology to quantum imaging.
Single-photon sources (SPS) are essential for secure quantum communication and quantum computing. Solid-state systems based on quantum dots (QDs) are particularly attractive for emitting pure, on-demand single photons, making them ideal candidates for flying qubits in quantum key distribution protocols. Integrating a SPS into photonic circuits is a key step toward scalable and "plug-and-play" quantum technologies. However, the SPS with the best performances (III-V QDs) operate only at cryogenic temperatures, a significant drawback for practical implementation. Alternatively, CdSe QDs (II-VI) are operational at 300 K and emit in the blue-green range, thus allowing for free-space long-distance communication in seawater and air.The thesis aims to develop an on-chip single-photon source that can operate at non-cryogenic temperatures. The SPS consists of a CdSe QD embedded within a ZnSe nanowire (NW) shell grown by molecular beam epitaxy on a patterned GaAs (111)B substrate. The NW geometry enhances light extraction by acting as a single-mode waveguide, while the conical ending of the shell improves emission control.We investigated the optical performance of the as-grown QD-NW emitter at room temperature, achieving a promising brightness of 0.17 photons per pulse and antibunching behavior with g(2)(0) < 0.3 within a reduced spectral window. However, the emission spectrum at 300 K features overlapping broad lines, leading to a trade-off between brightness and purity. At 6 K, we used a broadband filter to capture entirely the narrow exciton line and measured directly the photon count rate with an avalanche photodiode. In addition, we observed strong antibunching with a few percent purity through cathodoluminescence.Phonons impact the performance of the SPS at high temperatures, where broad lines overlap, and at cryogenic temperatures, where they reduce the photon indistinguishability. Understanding and controlling the influence of phonons has increased the need for high-accuracy temperature measurements at cryogenic temperatures. We present a calibration-free method to extract the local temperature from the emission spectrum, which we used to investigate the heating effects induced by non-resonant excitation. Additionally, we analysed the line-broadening mechanisms from cryogenic to room temperature. An extension of the Huang-Rhys model is developed to analytically describe the acoustic exciton-phonon interactions, accounting for multi-phonon processes. The model accurately fits emission spectra from 6 K to 300 K using parameters obtained from low-temperature data.The tapered nanowire shape is also an advantage for integration into a photonic device, enabling efficient evanescent coupling when the emitter is positioned next to a waveguide. The direct transfer using micromanipulators in a scanning electron microscope onto pre-fabricated waveguides is very challenging due to the tiny size of the waveguide at an emission wavelength of 550 nm. We developed a new approach, where the emitter is deposited within a large zone and then embedded within a resist, which serves as a mask during waveguide etching. This method significantly reduces the need for micro-manipulation and allows for promising prospects. We used finite-difference time-domain simulations to support the design and fabrication of the waveguides for optimal coupling.
Quantum technology promises to revolutionize various aspects of information processing, communication, and data security, by surpassing the capabilities of classical systems. Central to these advancements are photons, due to their resilience to external influence and ease of transport in air and glass fibers. However, attenuation in glass fiber cores hinders the realization of a worldwide quantum network. To circumvent this limit, the use of quantum repeaters for long-distance communication is required. Pivotal to the realization of quantum repeaters are entangled photons, enabling the distribution of entanglement across intermediate nodes, eventually extending the range of the envisioned quantum network. Despite the availability of numerous photon sources, stringent requirements–such as deterministic photon generation with high purity, high indistinguishability, high efficiency and a high degree of entanglement–hinder the realization of quantum repeaters, as they need to be fulfilled within the same device. Epitaxial quantum dots have emerged as promising candidates for generating pairs of entangled photons with a high purity and a high degree of entanglement. These semiconductor nanostructures, often referred to as “artificial atoms,” confine charge carriers and discretize energy levels like atoms but in a manipulable solid state environment. They exhibit exceptional emission characteristics owing to their high quantum efficiency and tunability via external fields such as electric, magnetic, and strain fields. Nevertheless, the fact that they are embedded in a semiconductor matrix with high refractive index limits their brightness due to challenging light extraction. This PhD thesis investigates the potential of strain-tuned GaAs droplet-etched quantum dots–a system known to generate highly entangled photon pairs–embedded within a photonic cavity, aiming to enhance light extraction efficiency, for an ideal entangled photon source. Device fabrication involves bonding the semiconductor with a micromachined piezoelectric substrate for strain-tuning quantum dots and their deterministic integration with a circular Bragg grating resonator, known as a “bullseye cavity.” Key advancements include cryogenic photoluminescence imaging for precise quantum dot localization, achieving high spatial overlap of the confined excitons with the resonator’s mode volume. Furthermore, postfabrication tuning of the resonator mode via wet chemical etching is employed to optimize spectral overlap. The achievements enable significant Purcell enhancement and high extraction efficiency. Simultaneously, multi-axial strain tuning the quantum dot emission eliminates entanglement degradation caused by the anisotropic exchange interaction of charge carriers. Such an entangled photon source additionally allows to experimentally reveal the limits of entanglement set by the excitation type. Finally, with optimized excitation conditions, a near-ideal entangled photon pair source is realized, which may surpass any other quantum emitter in terms of simultaneous brightness and degree of entanglement. The advancements presented within this PhD thesis represent a significant step towards the integration of quantum dot-based entangled photon sources into real-world quantum technology applications, facilitating the realization of a quantum internet.
Harnessing quantum mechanics to revolutionize various fields of established technology has fueled research activities in recent years. Especially the prospect of inherently secure quantum communication channels has become increasingly desirable to businesses, politicians and society as a whole to protect sensitive information. \nAt heart, quantum communication relies on the distribution of entangled quantum states that make the communication impervious to eavesdroppers. Naturally single photons or photon pairs are an excellent choice for distributing entangled states at the speed-of-light through existing fiber-networks. \nOne of the most promising quantum light sources constitute epitaxial quantum dots. The high oscillator strength renders them exceptionally bright, while still emitting nearly indistinguishable single photons with quantum efficiencies close to unity, an important prerequisite for high-fidelity photonic quantum applications. By carefully manufacturing the semiconductor heterostructure, the optical environment can be individually tailored, utilizing Purcell enhancement, by embedding the emitter in a semiconductor cavity or exploiting wave guiding properties in form of micropillars or nanowires to enhance the extraction efficiency. \nInevitable optical attenuation in fiber networks however necessitates the overall communication channel length to be divided into subsections with nodes that can temporarily store the quantum information. Naturally this requires a quantum memory which can efficiently store the quantum state for a sufficiently long time and subsequently recreate the stored photon on demand. \nIn this framework, atomic memories represent the established benchmark, unrivaled by quantum dots spin states which remain intrinsically limited by the decoherence-inducing interaction with the solid state environment. Combining the excellent single-photon source of a quantum dot with the superior coherence properties of alkali quantum memories in a hybrid system at each quantum node offers the best of both worlds, promising exponential speed-up of truly secure communication. \nThis PhD thesis focuses on the requirements imposed on the quantum dot in such a hybrid quantum network and shows how these challenges can be overcome. \nThe first part of the introduction aims to give a detailed overview on the underlying quantum communication protocol of a hybrid quantum network and how it fares against the more established DLCZ protocol. Next, single-photon sources, and quantum dots in particular, will be outlined and the growth mechanism and optical properties of epitaxial GaAs quantum dots discussed in detail. Lastly, to illustrate the framework in which a quantum dot can efficiently be paired with alkali atoms and to understand the challenges that arise, the mode of operation and attributes of the state-of-art broadband quantum memory will be summarized in chapter 2. \nThe third chapter investigates the optical properties of an epitaxial GaAs quantum dot spectrally matched to rubidium. By means of strain-tuning, the quantum dot can address all hyperfine transitions of the rubidium D2 line and a first interaction with atomic vapors is shown in a transmission measurement. In conjunction with other optical measurements, true Fourier-limited emission of single photons is demonstrated. Furthermore, we establish a possible route to overcome the bandwidth mismatch of the two systems in form of the coherent-scattering regime. \nWhile this coherent-scattering regime offers quantum dot single-photons with sub-natural bandwidths, in form of elastically scattered single photons that predominately retain the small linewidth of the excitation laser, the emission is highly probabilistic and relies on continuous-wave excitation or weak, resonant laser pulses of durations exceeding the exciton lifetime. The fourth chapter demonstrates the generation of true on-demand single photons with tailored temporal waveform envelopes between 14 and 245 ns, overcoming the temporal limitations imposed by the exciton two-level system. The photonic bandwidth is reduced by almost one order of magnitude. \nIn the following, the decay dynamics of a positively charged exciton in an GaAs quantum dot will be investigated by time-resolved photolumincescence and resonance fluorescence measurements (chapter 5). In Chapter 6 the optical properties of GaAs quantum dots in 500 nm thick membranes are characterized. Finally, an outlook into future developments and the solutions to remaining challenges will be presented. \n