Heralded Generation of Correlated Photon Pairs from CdS/CdSe/CdS Quantum Shells
Andrew A. Marder, S. Smith, James Cassidy, Dulanjan Harankahage, Zhongjian Hu, Steve M. Savoy, George Chappell Schatz, Mikhail A. Zamkov, Anton V. Malko
Quantum information processing demands efficient quantum light sources (QLS) capable of producing high-fidelity single photons or entangled photon pairs. Single epitaxial quantum dots (QDs) have long been proven to be efficient sources of deterministic single photons; however, their production via molecular-beam epitaxy presents scalability challenges. Conversely, colloidal semiconductor QDs offer scalable solution processing and tunable photoluminescence, but suffer from broader linewidths and unstable emissions. This leads to spectrally inseparable emission from exciton (X) and biexciton (XX) states, complicating the production of single photons and triggered photon pairs. Here, we demonstrate that colloidal semiconductor quantum shells (QSs) achieve significant spectral separation (∼75-80 meV) and long temporal stability of X and XX emissive states, enabling the observation of exciton-biexciton bunching in colloidal QDs. Our low-temperature single-particle measurements show cascaded XX-X emission of single photon pairs for over 200 s, with minimal overlap between X and XX features. The X-XX distinguishability allows for an in-depth theoretical characterization of cross-correlation strength, placing it in perspective with photon pairs of epitaxial counterparts. These findings highlight a strong potential of semiconductor quantum shells for applications in quantum information processing.
Quantum information processing demands efficient quantum light sources (QLS) capable of producing high-fidelity single photons or entangled photon pairs. Single epitaxial quantum dots (QDs) have long been proven to be efficient sources of deterministic single photons; however, their production via molecular-beam epitaxy presents scalability challenges. Conversely, colloidal semiconductor QDs offer scalable solution processing and tunable photoluminescence, but suffer from broader linewidths and unstable emissions. This leads to spectrally inseparable emission from exciton (X) and biexciton (XX) states, complicating the production of single photons and triggered photon pairs. Here, we demonstrate that colloidal semiconductor quantum shells (QSs) achieve significant spectral separation (∼75-80 meV) and long temporal stability of X and XX emissive states, enabling the observation of exciton-biexciton bunching in colloidal QDs. Our low-temperature single-particle measurements show cascaded XX-X emission of single photon pairs for over 200 s, with minimal overlap between X and XX features. The X-XX distinguishability allows for an in-depth theoretical characterization of cross-correlation strength, placing it in perspective with photon pairs of epitaxial counterparts. These findings highlight a strong potential of semiconductor quantum shells for applications in quantum information processing.
The biexciton-exciton cascade in quantum dots (QDs) yields entangled photon pairs, and recent developments in engineering photonic structures around the dot for efficient light extraction and proper control of the fine-structure splitting, has led to significant breakthroughs in achieving an ideal entangled photon source -- exhibiting properties such as high extraction efficiency, low multi-photon emission and high entanglement fidelity. This thesis presents our development in enhancing the performance of entangled photon generation of QDs towards near-unity efficiency and fidelity. We study InAsP quantum dots in photonic nanowires for efficient light extraction and to reveal the effect of a quantum dot with high nuclear spin on the entanglement fidelity. \n \nRevealing the ultimate limit of entanglement in QDs is still a challenge, and it is generally believed that a sample made of atoms possessing high nuclear spins exhibits limited entanglement due to the dephasing caused by spin-spin interactions. Moreover, it is assumed that the fine-structure splitting of QDs degrades the entanglement fidelity, as it introduces a which-path information in the biexciton-exciton cascade. We have performed two-photon state tomography on InAsP QDs in InP nanowires, comprising of nuclear spin 9/2, and have realized that such a source is capable of generating entangled photon pairs with negligible dephasing during the emission lifetime, with a peak concurrence C = 77% and a count-weighted average concurrence 62%. This result was obtained by comparing the outcome of our measurements with a theoretical model that assumes no dephasing, however, takes into account the details of the detection system, i.e., dark-count rates and timing resolution, as well as, specific features of the QD, e.g., emission lifetime, fine-structure splitting, multi-photon emission probability, etc. Proper engineering of tapered nanowires allows for extraction of the emitted photons with high efficiency, which makes it possible to perform a complete two-photon state tomography and monitoring the evolution of the exciton state, as well as, the entanglement fidelity of the photon-pair, during the emission lifetime. This enabled us to reveal the effect of an imperfect detection system, as well as, multi-photon emission in recording low values for entanglement fidelity. Moreover, our calculations show that proper analysis of the time-energy uncertainty relation provides the necessary means to measure a high entanglement fidelity even in the presence of fine-structure splitting; since, a detection system with high timing resolution can overlook the which-path information, as the uncertainty in measuring the energy of the photons will be larger than the fine-structure splitting. Therefore, realizing near-unity entanglement fidelity using QDs is merely a technical challenge, i.e., resonant excitation of the QD, in order to suppress multi-photon emission, and use of a detection system with low timing jitter and dark-count rates. \n \nAs a next step to achieve this goal, we have performed the resonant two-photon excitation scheme for the first time on a QD in a photonic nanowire, which resulted in an enhancement of the performance of our source. We managed to improve the single-photon purity of the source, g^(2)(0), by two orders of magnitude; moreover, analysis of the emission spectrum reveals that this scheme increases the pair-production efficiency to values above 93% for the biexciton-exciton cascade. Taking the efficiency of our experimental setup into consideration, the results indicate an approximately eight-fold enhancement of the pair-extraction efficiency as compared to the quasi-resonant excitation scheme (12.55% vs. 1.6%). Based on these results, two-photon state tomography on our source, under resonant two-photon excitation and performed by a detection system with high timing resolution and low dark-count rates, yields near-unity entanglement fidelity. By considering the enhancement in pair-extraction efficiency that we obtained, QDs in photonic nanowires can surpass the performance of spontaneous parametric down conversion sources in terms of entanglement fidelity and pair-extraction efficiency. \n \nEven though we have shown a finite fine-structure splitting does not degrade the entanglement fidelity in QDs, for various application in quantum information removing the fine-structure splitting is beneficial. Therefore, we have proposed a universal all-optical approach for removing the fine-structure splitting. In this scheme, the energy of the photons are shifted by using a pair of quarter-wave plates and fast-rotating half-wave plates after they have been emitted; and as a result, the energy difference between the two decay paths in the biexciton-exciton cascade is erased. This method is applicable to any QD source and can be easily implemented using the currently available technology; moreover, no further sample processing will be required in order to achieve zero fine-structure splitting.
Semiconductor quantum dots (QDs) have emerged as a premier solid-state platform for the deterministic generation of nonclassical light, offering a compelling pathway toward scalable quantum photonic systems. While single-photon emission from QDs has reached a high level of maturity, the realization of high-fidelity entangled photon-pair sources remains an active and rapidly evolving frontier. In this review, we survey the recent progress in QD-based entangled photon sources, highlighting the conceptual evolution from the established biexciton-exciton cascade to the emerging paradigm of spontaneous two-photon emission. We further examine how advances in nanophotonic architectures and coherent control strategies are redefining fundamental performance limits, enabling concurrent improvements in source brightness, coherence, and entanglement fidelity. Finally, we discuss the key physical and technological challenges that must be addressed to bridge the gap between laboratory demonstrations and large-scale deployment. We conclude by outlining the future opportunities for integrating QD-based entangled photon sources into practical quantum communication, computation, and sensing platforms.
Semiconductor quantum dots (QDs) have emerged as a premier solid-state platform for the deterministic generation of nonclassical light, offering a compelling pathway toward scalable quantum photonic systems. While single-photon emission from QDs has reached a high level of maturity, the realization of high-fidelity entangled photon-pair sources remains an active and rapidly evolving frontier. In this review, we survey the recent progress in QD-based entangled photon sources, highlighting the conceptual evolution from the established biexciton–exciton cascade to the emerging paradigm of spontaneous two-photon emission. We further examine how advances in nanophotonic architectures and coherent control strategies are redefining fundamental performance limits, enabling concurrent improvements in source brightness, coherence, and entanglement fidelity. Finally, we discuss the key physical and technological challenges that must be addressed to bridge the gap between laboratory demonstrations and large-scale deployment. We conclude by outlining the future opportunities for integrating QD-based entangled photon sources into practical quantum communication, computation, and sensing platforms.
Resonant laser excitation of a two-level system with subsequent single-photon emission can be used to generate single photons with high indistinguishability or Hong-Ou-Mandel (HOM) visibility. However, spectral overlap between excitation laser and emitted photons generally poses significant challenges. Furthermore, emitter re-excitation intrinsically limits achievable single-photon purity. Established solutions mitigate these issues at significant cost to source efficiency and with increased source complexity. This motivates the use of few-level systems with spectral separation of excitation and emission pathways. One option is a three-level cascade. However, without targeted lifetime engineering of emitting states, the cascade naturally limits achievable photon indistinguishability. Here we study a semiconductor quantum dot with resonant and selective cavity-enhancement of biexciton-to-exciton transition. Following resonant two-photon excitation of the biexciton state, we collect the emitted single photon with the cavity. This approach circumvents emitter re-excitation and naturally introduces spectral separation of excitation laser and emitted single photon. Supported by first experimental results, we demonstrate theoretically that with selective Purcell enhancement, the observed quality quantifiers of single-photon emission (purity, equivalently g(2)(0), and HOM visibility V, equivalently indistinguishability) are competitive with respect to high-quality deterministic quantum-dot single-photon sources. This is already achieved without systematic optimization or targeted system engineering, which firmly places the reported approach as a viable route to the next generation of highest-quality quantum-dot based deterministic single-photon sources.
Entangled photon sources are crucial for quantum optics, quantum sensing, and quantum communication. Semiconductor quantum dots generate on-demand entangled photon pairs via the biexciton-exciton cascade. However, the pair of photons are emitted isotropically in all directions, thus limiting the collection efficiency to a fraction of a percent. Moreover, strain and structural asymmetry in quantum dots lift the degeneracy of the intermediate exciton states in the cascade, thus degrading the measured entanglement fidelity. Here, we propose an approach for generating a pair of entangled photons from a semiconductor quantum dot by application of a quadrupole electrostatic potential. We show that the quadrupole electric field corrects for the spatial asymmetry of the excitonic wave function for any quantum dot dipole orientation and fully erases the fine-structure splitting without compromising the spatial overlap between electrons and holes. Our approach is compatible with nanophotonic structures such as microcavities and nanowires, thus paving the way towards a deterministic source of entangled photons with high fidelity and collection efficiency.
Semiconductor quantum light sources are favorable for a wide range of quantum photonic tasks, particularly quantum computing and quantum information processing. Here, we theoretically investigate the properties of quantum emitters as a source of entangled photons with practical quantum properties including heralding of on-demand single photons. Through the theoretical analysis, we characterize the properties of a cascade (biexciton) emitter, including (1) studies of single-photon purity, (2) investigating the first- and second-order correlation functions, and (3) determining the Schmidt number of the entangled photons. The analytical expression derived for the Schmidt number of the cascade emitters reveals a strong dependence on the ratio of decay rates of the first and second photons. Looking into the joint spectral density of the generated biphotons, we show how the purity and degree of entanglement are connected to the production of heralded single photons. Our model is further developed to include polarization effects, fine structure splitting, and the emission delay between the exciton and biexciton emission. The extended model offers more details about the underlying mechanism of entangled photon production, and it provides additional degrees of freedom for manipulating the system and characterizing purity of the output photon. The theoretical investigations and the analysis provide a cornerstone for the experimental design and engineering of on-demand single photons.