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
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
A quantum network is believed to be the next generation of quantum technology [1]. In the past decades, individual quantum systems—for example, quantum dot (QD) [2–4], etc.—have been studied in depth and the technologies are mature; therefore, the consideration of combining different systems to construct a quantum network (especially a hybrid one) is timely. Moreover, a quantum network is absolutely necessary in the fulfilment of a general quantum task, which needs the cooperation of many different kinds of quantum units. On a larger scale, the local quantum networks can be further linked to construct a global quantum network, namely the quantum Internet [1]. With this technology at hand, distributed quantum computation can be realized, making scalable quantum information processing possible in multiple sites over long distances. The primary challenge of the construction of a quantum network is the state distribution among different nodes. An elementary quantum network based on two identical nodes each constituted by a single atom in the optical cavity has been realized in an experiment [5]. However, here we focus on the quantum network comprising heterogeneous nodes, which is more general and can combine advantages of different quantum systems to complete more complicated quantum tasks. The construction of a hybrid quantum network is more difficult, since heterogeneous quantum systems have different properties that are not naturally matched, such as the different emission (or absorption) wavelengths and different bandwidths [8], etc. To establish the hybrid interface, QD is a good candidate. QD can act as a deterministic single [2] or entangled [3] photon source and is also a promising physical carrier for solid-state spin qubit [4]. QD has been interfaced with hot atoms [6] and single ions [7] in recent years. Almost at the same time, Li's group experimentally demonstrated the first optical connection between QD and a solid-state quantum memory [8]. Distinguishing from the former works, the all-solid-state character of this work makes the whole architecture more stable and easier to be manipulated and integrated. During this work, the sample was grown by Niu's group [8]. A special sample design moves the emission band of QDs to approximately 879.7 nm—the memory band of the solid-state memory [9]. Since the fine-tuning range is only several 0.1 nm, hundreds of QDs on the sample were detected by Li et al. and finally one of them was selected, whose emission line is located at 879.5 nm. Using a local-heating technique, the researchers precisely tuned the emission wavelength of this QD to the solid-state memory's memory band, whose bandwidth is as narrow as hundreds of MHz [9]. The quantum memory in this experiment was based on the atomic frequency comb (AFC) protocol [10]. The memory efficiency is as high as 20% when the storage time is 40 ns, and the non-collinear configuration for the pump light and the signal photons can substantially reduce the noise from the pump light. To further reduce the detection noise, a superconducting single-photon detector (SSPD), whose dark count rate can be as low as 1.5 per second, is used instead of the silicon single-photon avalanche diode. With these conditions, Li's experiment clearly shows the stored and retrieved single photons that are originally generated from the QD. The signal-to-noise ratio (SNR) is 9:1. The second-order retrieved single photons are even seen in the data, which further validates the experimental result. Another advantage of Li's work is the demonstration of multi-temporal-mode quantum memory with up to 100 narrow deterministic-single-photon pulses [8]. This result is directly associated with the construction of a quantum repeater [11]—one of the essential components for a long-distance quantum network. The primary characteristics of this experiment, namely the deterministic single-photon memory (differing from the previous works) and the multimode memory, are both critically important in the improvement of a quantum repeater's efficiency [12]. Also, Li's further work finished the quantum memory of 51 spatial modes using the orbital angular momentum (OAM) modes of herald single photons [9]. By combining both the temporal and spatial multiplexing, and the deterministic single-photon source, more efficient quantum repeaters can be constructed. We hope that the recent studies [8,9] will pave the way for the construction of quantum repeaters, and furthermore quantum networks—both in the short term and the long term—based on all-solid-state devices. As a special application of a quantum network, quantum key distribution (QKD) can also benefit from Li's work both in security and transmission distance (key rate). QKD utilizes the principles of quantum mechanics to guarantee secure communication between two authorized parties (or quantum nodes, for instance) and the famous protocols including BB84 (proposed by Bennett and Brassard in 1984) [13]), etc. However, the commonly used weak-coherent-pulse photon source (typically attenuated laser) will decrease the security of QKD because of its multiphoton probability, which means that QKD suffers from several certain attacks, such as the photon number splitting (PNS) attack. Although a decoy state has been introduced to achieve potential solutions to this problem, a substantial shrinking of the sifted key will be required and the complexity of the protocol may contain loopholes [14,15]. Therefore, the unconditional security guaranteed by quantum mechanics still requires a single-photon source, such as QD (experimental work regarding QKD on the basis of a QD single-photon source can be referred to in [14,15]), etc. The deterministic-single-photon pulse train generated by QD in Li's experiment [8] can provide a single-photon-source node (in the network) and keep the security of QKD. Moreover, because of both the elimination of multiphoton probability and the multi-temporal-mode single-photon generation, the key rate of QKD will be improved, which is associated with a longer transmission distance. The quantum repeater that benefited from Li's work will also further improve the transmission distance of QKD.
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.
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 realization of a functional quantum repeater is one of the major research goals in long-distance quantum communication. Among the different approaches that are being followed, the one relying on quantum memories interfaced with deterministic quantum emitters is considered as among one of the most promising solutions. In this work, we focus on memory-based quantum-repeater schemes that rely on semiconductor quantum dots for the generation of polarization entangled photons. Going through the most relevant figures of merit related to efficiency of the photon source, we select significant developments in fabrication, processing and tuning techniques aimed at combining high degree of entanglement with on-demand pair generation, with a special focus on the progress achieved in the representative case of the GaAs system. We proceed to offer a perspective on integration with quantum memories, both highlighting preliminary works on natural-artificial atomic interfaces and commenting a wide choice of currently available and potentially viable memory solutions in terms of wavelength, bandwidth and noise-requirements. To complete the overview, we also present recent implementations of entanglement-based quantum communication protocols with quantum dots and highlight the next challenges ahead for the implementation of practical quantum networks.
Summary form only given. Quantum networks consist of many quantum memory nodes that are interconnected via photonic links, transporting single photons carrying quantum information. In the future, such quantum networks may enable: high-speed quantum cryptography for unconditionally secure communication; large-scale quantum computers; and quantum simulators that will allow for exponential speed-up in solving specific complex problems. A promising route towards functional quantum network nodes is the heterogeneous approach [1], where different and separately optimized physical systems are used for single photon generation and storage. For example semiconductor quantum dots may be used as efficient, fast and deterministic single photon sources, while atomic ensembles allow for efficient storage of these photons.We demonstrate a photonic memory in warm Rb vapour with on-demand storage and retrieval, based on electromagnetic induced transparency (EIT). The memory is suitable for storing single photons emitted by a GaAs droplet quantum dots [2] embedded into a state-of-the-art photonic structures [3]. With our experiments we close the gap between low speed quantum memories with acceptance bandwidth well below 100 MHz and ultra-high speed memories with acceptance bandwidth above 1 GHz. We find that in this intermediate regime vapour cell memories offer an excellent compromise between storage efficiency, storage time and experimental complexity.
Single spins confined in semiconductor quantum dots - artificial atoms in the solid-state - are attractive candidates for quantum mechanical bits, the fundamental units and building blocks of a quantum computer. The ability to address quantum dot spins optically allows us to initialise and manipulate the state of the quantum bit. Gaining information on the qubit, for example by reading out its state, not only requires state-selective optical excitation, but also access to the single photons scattered in response by the quantum dot. Further, for a distributed computer architecture where nodes of few quantum bits are interlinked via optical communication channels photonic quantum bits are required to faithfully transmit the quantum information. In this thesis we advocate resonant excitation of quantum dot transitions and collection of the resonance fluorescence to address two outstanding challenges: generating dephasing-free single photons for use as flying quantum bits and single-shot spin readout. To this end we investigate the spectral and first-order coherence properties of quantum dot resonance fluorescence. In particular, we directly observe highly coherent scattering in the low Rabi frequency limit which has remained unexplored for solid-state single photon emitters so far. At the same time, interactions with the semiconductor environment are revealed and quantified through their optical signatures: exciton-phonon coupling, nuclear spin dynamics and local electric field fluctuations signal a departure from the ideal atom-like behaviour. Taking advantage of the laser-like coherence of single phase-locked quantum dot photons in the Heitler regime, we demonstrate near-ideal two-photon quantum interference. This benchmark measurement is a precursor for the photonic entanglement of distant quantum dot spins in a quantum optical network, and the results here predict a high fidelity operation. Finally, moving to tunnel-coupled quantum dot molecules we show that the overlap of carrier wave functions in two closely spaced quantum dots forms new spin-selective optical transitions not available in single quantum dots. Then, the presence or absence of scattered photons reveals the electron spin. Intermittency in the quantum dot resonance fluorescence allowed us, for the first time, to observe spin quantum jumps in real-time. Both achievements - highly coherent photons and spin readout - provide the missing link to attempt creation of a small-scale quantum network now.