Abstract Spontaneous two-photon emission is a process in which the transition between two quantum states happens via simultaneous emissions of two identical photons. Such second-order quantum radiation is of paramount importance in astrophysics, atomic physics, and quantum technology. In particular, on-demand spontaneous two-photon emission from single quantum emitters has long been envisioned to revolutionize photonic quantum science and technology. To date, experimental realizations of two-photon emission at the single quanta level are still highly challenging yet elusive due to their low probabilities. In this work, we explore spontaneous two-photon emission from a single semiconductor quantum dot deterministically coupled to a high-quality microcavity in which the cavity resonances greatly enhance both excitation and emission processes. When the cavity is resonant to the half energy of the biexciton, the strong vacuum field in the cavity mode drives the biexciton to the ground state and simultaneously emits two photons into the cavity mode, resulting in two-photon emissions with a record brightness comparable to the competing single-photon process and sub-nanowatt power consumption. For the first time, the quantum nature associated with spontaneous two-photon emissions in the cavity quantum electrodynamics regime has been investigated via photon statistics measurements. Furthermore, spontaneous two-photon emission is exploited to build unconventional entangled quantum light sources with the unique advantage of combining the best of two worlds: near-unity entanglement fidelity for spontaneous parametric down-conversion source and on-demand photon emissions for atomic quantum emitters. Our work provides unprecedented insights into the two-photon process in the quantum regime and opens an unexplored avenue for pursuing optically reconfigurable quantum light sources with nonlinear quantum radiations.
Abstract Spontaneous two-photon emission is a process in which the transition between two quantum states happens via simultaneous emissions of two identical photons. Such second-order quantum radiation is of paramount importance in astrophysics, atomic physics, and quantum technology. In particular, on-demand spontaneous two-photon emission from single quantum emitters has long been envisioned to revolutionize photonic quantum science and technology. To date, experimental realizations of two-photon emission at the single quanta level are still highly challenging yet elusive due to their low probabilities. In this work, we explore spontaneous two-photon emission from a single semiconductor quantum dot deterministically coupled to a high-quality microcavity in which the cavity resonances greatly enhance both excitation and emission processes. When the cavity is resonant to the half energy of the biexciton, the strong vacuum field in the cavity mode drives the biexciton to the ground state and simultaneously emits two photons into the cavity mode, resulting in two-photon emissions with a record brightness comparable to the competing single-photon process and sub-nanowatt power consumption. For the first time, the quantum nature associated with spontaneous two-photon emissions in the cavity quantum electrodynamics regime has been investigated via photon statistics measurements. Furthermore, spontaneous two-photon emission is exploited to build unconventional entangled quantum light sources with the unique advantage of combining the best of two worlds: near-unity entanglement fidelity for spontaneous parametric down-conversion source and on-demand photon emissions for atomic quantum emitters. Our work provides unprecedented insights into the two-photon process in the quantum regime and opens an unexplored avenue for pursuing optically reconfigurable quantum light sources with nonlinear quantum radiations.
Narrow line-widths and the possibility of enhanced spontaneous emission via coupling to microcavities make semiconductor quantum dots ideal for harnessing coherent quantum phenomena at the single photon level. So far, however, all approaches have relied on incoherent pumping, which limits the desirable properties of the emission. In contrast, coherent excitation was recognized to be necessary for providing both improved photon indistinguishability and high efficiency, and offers the quantum control capabilities required for basic qubit manipulations. Here we achieve, for the first time, resonant and coherent excitation of a quantum dot with simultaneous collection of the non-classical photon emission. Second-order correlation measurements show the unique signature of a coherently-driven two-level quantum emitter: the photon statistics become oscillatory at high driving fields, reflecting the coherent evolution of the excitonic ground state of the quantum dot.
Semiconductor quantum dots are promising sources for polarization-entangled photons. As an alternative to the usual cascaded biexciton-exciton emission, direct two-photon emission from the biexciton can be used. With a high-quality optical resonator tuned to half the biexciton energy, a large proportion of the photons can be steered into the two-photon emission channel. In this case the degree of polarization entanglement is inherently insensitive to the exciton fine-structure splitting. In the present work we analyze the biexciton emission with particular emphasis on the influence of coupling of the quantum-dot cavity system to its environment. Especially for a high-quality cavity, the coupling to the surrounding semiconductor material can open up additional phonon-assisted decay channels. Our analysis demonstrates that with the cavity tuned to half the biexciton energy, the potentially detrimental influence of the phonons on the polarization entanglement is strongly suppressed---high degrees of entanglement can still be achieved. We further discuss spectral properties and statistics of the emitted twin photons.
A single atom in a cavity is the model system of cavity quantum electrodynamics (CQED). The strong coupling regime between the atom and cavity-confined photon corresponds to the reversible exchange of energy between the two modes, and underpins a wide range of CQED phenomena with applications in quantum information science, including for example as quantum logic gates and as sources of entangled states. An important advance was achieved recently when strong coupling between excitons and cavity photons was reported for the first time for localized quantum dots (QDs) in micron-size solid state cavities. This has significance in terms of scalability and integration with other optical devices, and could lead to the emergence of "quantum optics on a chip" technology. However the results presented so far for quantum dots are in the linear regime, corresponding to coupling to the vacuum field (vacuum Rabi splitting); they are not a true QED effect and can equally well be described by classical physics as the coupling between two oscillators. In this paper, we present evidence for a purely quantum phenomenon for the QD/cavity photon system, namely the increase in splitting of the levels when the mean number of photons in the cavity is increased. This corresponds to non-linearities on the single-photon scale: the presence of a single excitation in the cavity changes the level structure, affecting the emission energies for a second photon. Such results are a first step in demonstrating the promise of quantum dots for CQED applications.
Next-generation information technology is expected to rely on discrete two-state quantum systems that can deterministically emit single photons. Quantum dots are mesoscopic (~10,000 atoms large) semiconductor islands grown in a host crystal of larger band-gap that make well-defined two-level quantum systems and are very attractive due to stability, record coherence times, and the possibility of integrating them into larger structures, such as optical microcavities. This work presents experimental progress towards understanding the coherent optical processes that occur in single quantum dots, particularly such phenomena that might be one day utilized for quantum communication applications. High resolution low temperature optical spectroscopy is used in conjunction with first order (amplitude) and second-order (intensity) correlation measurements of the emitted field. A novel technique is introduced that is capable of harvesting the fluorescence of single dots at the same frequency as the laser, previously impossible due to insurmountable scattering. This technique enables the observation, for the first time, of single quantum dot resonance fluorescence, in both the weak and strong excitation regimes, which forms the basis for deterministic generation of single photons. Guided by the rich theoretical description available from quantum optics with atoms we obtain insight into the complex dynamics of this driven system. Quantum dots confined to novel optical microcavities were further investigated using micro photoluminescence. An optical microcavity properly coupled to a two-level system can profoundly modify its emission characteristics via quantum electrodynamical effects, which are highly attractive for single photon sources. The all-epitaxial structures we probe are distinguished by a bulk morphology that overcomes the fragility problems of existing approaches, and provides high quality factors as well as small mode volumes. Lasing is obtained with larger strucutres. Additionally, isolation of individual dots is further realized in smaller cavities and the Purcell effect observed in time-resolved photon counting experiments.
Over the past decade, much effort has been made in identifying and characterizing systems that can form a building block of quantum networks, among which semiconductor quantum dots (QD) and spontaneous parametric down-conversion (SPDC) source are two of the most promising candidates. The work presented in this thesis will be centered on investigating and engineering the mentioned systems for generating customizable single photons. A type-II SPDC source can generate a highly flexible pair of entangled photons that can be used to interface disparate quantum systems. In this thesis, we have successfully implemented a cavity-SPDC source that emits polarization correlated photons at 942 nm with a lifetime of 950-1050ps that mode matches closely with InAs/GaAs QD photons. The source emits 80 photon pairs per second per mW pump power within the 150MHz bandwidth. Though the detection of idler photons, the source is capable of emitting heralded photons with g2≤0.5 for up to 40 mW pump power. For a low pump power of ~5 mW, the heralded g2 is 0.06, indicating that the system is an excellent heralded single photon source. By directly exciting a single QD with cavity-SPDC photons, we have demonstrated a heralded-absorption of SPDC photons by QD, resulting in the coupling of the two systems. Due to the large pump bandwidth, the emitted source is highly multimode in nature, requiring us to post-filter the downconverted field, resulting in a lower photon pair emission rate. We propose placing an intra-cavity etalon to suppress the multi-mode emissions and increase the photon count rate. Understanding and experimentally implementing two-photon interference (HOM) measurements will be crucial for building a scalable quantum network. A detailed theoretical description of HOM measurements is given and is experimentally demonstrated using photons emitted by QD. Through HOM measurements we demonstrated that the QD sample in the study is capable of emitting indistinguishable photons, with the visibility exceeding 95%. As an alternative approach to modifying the spectral mode of single photons, we performed phase modulation of photons emitted by a QD to generate additional sidebands that are separated by several GHz. By performing HOM measurements, we have shown that the central component and the sidebands are in the superposition states and the spectrally modified photons have a well-preserved indistinguishability. Such spectrally engineered photons can be used for phase-encoded cryptography applications. These experimental results should lay the foundations towards building a scalable hybrid quantum network.
Entangled photon pairs are a crucial resource in quantum information processing. However, common sources of entangled photon pairs, such as generation by spontaneous parametric down-conversion, impose a Poisson distribution on the pairs, limiting their applicability to quantum information processing. Therefore, generating entangled photon pairs exhibiting a sub-Poisson distribution (i.e., entangled photon bundle) would be crucial/an important advancement in the current research context. Recently, it has been proposed that antibunched photon pairs can be generated using pulsed excitation of quantum dots based on photon blockade. In this work we propose a scheme to generate entangled photon pairs with strong antibunching properties via continuous driving. Under two-photon resonant continuous pumping, a quantum dot is first excited to a biexciton state and then emits a pair of entangled photons into a two-mode cavity. Owing to the strong coupling between the quantum dot and optical modes of the cavity, at most one pair of left-/right-polarized photons exists at a time in the cavity. Specifically, the antibunching effect, average photon number, and entanglement of the left- or right-polarized photons can be resonantly enhanced when the coupling strengths between the exciton (biexciton) transition and cavity modes are equal. Moreover, our results show that the binding energy of the biexciton substantially affects the antibunching effect, average photon number, and entanglement of the left-/right-polarized photons. With suitable parameters, we can realize photon pairs with strong antibunching, a large average photon number, and deep entanglement. Hence, the studied quantum dot-cavity system is a promising source of antibunched entangled photon pairs.