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Quantenpunkte als helle Quellen verschränkter Photonenpaare

Tobias M. Krieger

Published Jan 1, 2024• 0 citations
OpenAlex

Abstract

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.

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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.

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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

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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.
A quantum-light source that delivers photons with a high brightness and a high degree of entanglement is fundamental for the development of efficient entanglement-based quantum-key distribution systems. Among all possible candidates, epitaxial quantum dots are currently emerging as one of the brightest sources of highly entangled photons. However, the optimization of both brightness and entanglement currently requires different technologies that are difficult to combine in a scalable manner. In this work, we overcome this challenge by developing a novel device consisting of a quantum dot embedded in a circular Bragg resonator, in turn, integrated onto a micromachined piezoelectric actuator. The resonator engineers the light-matter interaction to empower extraction efficiencies up to 0.69(4). Simultaneously, the actuator manipulates strain fields that tune the quantum dot for the generation of entangled photons with corrected fidelities to a maximally entangled state up to 0.96(1). This hybrid technology has the potential to overcome the limitations of the key rates that plague QD-based entangled sources for entanglement-based quantum key distribution and entanglement-based quantum networks. Supplementary Information: The online version contains supplementary material available at 10.1186/s43593-024-00072-8.
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.
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
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.
The generation and long-haul transmission of highly entangled photon pairs is a cornerstone of emerging photonic quantum technologies with key applications such as quantum key distribution and distributed quantum computing. However, a natural limit for the maximum transmission distance is inevitably set by attenuation in the medium. A network of quantum repeaters containing multiple sources of entangled photons would allow overcoming this limit. For this purpose, the requirements on the source's brightness and the photon pairs' degree of entanglement and indistinguishability are stringent. Despite the impressive progress made so far, a definitive scalable photon source fulfilling such requirements is still being sought after. Semiconductor quantum dots excel in this context as sub-Poissonian sources of polarization entangled photon pairs. In this work, we present the state-of-the-art set by GaAs based quantum dots and use them as a benchmark to discuss the challenges toward the realization of practical quantum networks.
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.