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.
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.
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 past decades quantum optics has been at the forefront of quantum innovative technologies. For practical applications, scalable platforms for implementation of quantum optical circuits are vital. This thesis presents two new platforms for scalable implementation of quantum optical circuits, namely, modular approach and monolithic integration. Here, we take the first steps towards the integration of three main elements of every quantum optics circuits: Single-photon emitters, single-photon detectors, and quantum logics. Until now, most quantum optical circuits used separate platforms for single-photon generation and detection. The main challenge in the integration of these technologies, which have different requirements, has slowed down the research in the field. Here, we integrate sources and detectors by first fabricating the devices on their own platform and then transferring and combining them together. Plasma enhanced chemical vapor deposition of silicon nitride followed by etching optical waveguides connect these elements. Removing the Poissonian optical excitation field from the quantum circuit is necessary for integration. Classical optical excitation can be avoided if the sources are electrically pumped. However, fabrication of high-quality electrically pumped sources, suitable for integration, has been limited. The experiments described in chapter 4 are our first step towards addressing the mentioned problem. Defect-free nanowires are grown on <100> direction and their optoelectronic performance are characterized. Nanowire quantum dots, thanks to their waveguiding, purity, coherence and their potentials for deterministic integration with other optical circuits, are promising single-photon sources for on-chip quantum optics. However, precise control of the emission energy of the quantum dots by growth has not become possible yet. Chapter 5 describes a method for on-chip tuning of emission energy of nanowire quantum dots using strain fields. We show the emission energy of independent nanowire quantum dots can be brought into degeneracy without affecting their single-photon emission properties. The quantum optical components have to be routed and connected together to form functional circuits. On a chip, this is usually carried out using optical waveguides. Moreover, manipulation of single photons has to be done in a scalable fashion. Again optical waveguides and ring resonators are very good candidates for this task. Therefore, understanding the behavior of these circuits such as their losses, polarization dependence, and temperature behavior is important. The experiment described in chapter 6 studies the behavior of plasma enhanced silicon nitride waveguides in cryogenic temperatures. We concluded in this chapter that due to weak thermo-optic sensitivity of silicon nitride at cryogenic temperatures, the available thermal budget on the system should be carefully considered. An important step in achieving a scalable platform for quantum optical circuits is deterministic and efficient integration of single-photon sources. In chapter 7, we demonstrate successful integration of III-V nanowire quantum dots with silicon nitride waveguides. The nanowires are deterministically selected and transferred from the original growth chip to the new substrate where they are integrated with low-loss silicon nitride waveguides. Our measurements show that the integrated sources preserve their high quality emission properties. In chapter 8, we describe an alternative approach: amodular method for scalable quantum optics. The proposed technique is based on coupling the single-photon from sources into optical fibers where the photons can be processed and then fed into the single-photon detectors. This approach has high flexibility and is easier to implement but as described in the chapter, at the moment, losses in the interfaces between optical fibers and single-photon sources are a major limiting factor. We conclude the thesis with some possible future directions and exciting new results on integration of single-photon detectors with sources and waveguides. Finally, primary results on on-chip single-photon filtering and removal of the optical excitation field are demonstrated.
Quantum light and in particular single photons have become essential resources for a growing number of quantum applications including quantum computing, quantum key distribution and quantum metrology. Solid-state atomlike systems such as semiconductor quantum dots and color defects in crystals have become the hallmark of highly pure single photon emitters in the past two decades. A particular interest has been developed in nanocrystal quantum dots (NQDs) and color centers in diamond as potential compact room-temperature emitters. There are however several challenges that inhibit the use of such sources in current technologies including low photon extraction efficiency, low emission rates and relatively low single photon purities. In this work we will review our efforts in overcoming these technical difficulties using several complementary methods including designing several nanoantenna devices that enhance the directionality and emission rate of the nanoemitter. In addition, we developed several temporal heralding techniques to overcome the hurdle of low single photon purity in NQDs in an effort to produce a highly pure, bright and efficient single photon source on-chip.
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.
Semiconductor quantum dots (QDs) coupled with optical microcavities provide an excellent platform for generating high-performance single-photon sources. However, the current microcavity structures are difficult to solve the tradeoff between single-photon purity and indistinguishability without additional filtering, due to challenges in suppressing broad phonon sideband spectrum and two-photon emission in the practical experiments. To address these issues, we have developed a novel asymmetric microcavity that supports two nondegenerate polarized modes, both resonant with a single quantum dot. One cavity mode is broadband and is used for excitation to reduce two-photon emission intensity, while the other is narrowband and is used for collection to enhance the indistinguishability of single-photon sources. This asymmetric microcavity also has the ability to overcome at least half of the photon efficiency loss under polarization filtering. Moreover, our model has employed an excitation pulse that resonates with cavity modes eliminating spectral distortion of intracavity fields, and efficiently achieving deterministic population inversion of QDs compared to an elliptical cavity. Our scheme paves the way to develop the excellent performance single-photon sources with higher brightness, near-unity purity, and indistinguishability without any additional filtering in practical experiments.
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.