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arXiv:2009.14008 · The Journal of Chemical Physics

Mechanistic understanding of entanglement and heralding in cascade emitters

Kobra Nasiri Avanaki, George Chappell Schatz

Published Jan 12, 2021• 9 citations
arXivHTMLPDF

Abstract

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.

DOI
10.1063/5.0032648

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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.
Motivated by recent advances in the development of single photon emitters for quantum information sciences, here we design and formulate a quantum cascade model that describes cascade emission by a quantum dot (QD) in a cavity structure while preserving entanglement that stores information needed for single photon emission. The theoretical approach is based on a photonic structure that consists of two orthogonal cavities in which resonance with either the first or second of the two emitted photons is possible, leading to amplification and rerouting of the entangled light. The cavity-QD scheme uses a four-level cascade emitter that involves three levels for each polarization, leading to two spatially entangled photons for each polarization. By solving the Schrodinger equation, we identify the characteristic properties of the system, which can be used in conjunction with optimization techniques to achieve the "best" design relative to a set of prioritized criteria or constraints in our optical system. The theoretical investigations include an analysis of emission spectra in addition to the joint spectral density profile, and the results demonstrate the ability of the cavities to act as frequency filters for the photons that make up the entanglements and to modify entanglement properties. The results provide new opportunities for the experimental design and engineering of on-demand single photon sources.
The generation of entangled photons from radiative cascades has enabled milestone experiments in quantum information science with several applications in photonic quantum technologies. Significant efforts are being devoted to pushing the performances of near-deterministic entangled-photon sources based on single quantum emitters often embedded in photonic cavities, so to boost the flux of photon pairs. The general postulate is that the emitter generates photons in a nearly maximally entangled state of polarization, ready for application purposes. Here, we demonstrate that this assumption is unjustified. We show that in radiative cascades there exists an interplay between photon polarization and emission wavevector, which can be further amplified by embedding the emitters in micro-cavities. We discuss how the polarization entanglement of photon pairs from a biexciton-exciton cascade in quantum dots strongly depends on their propagation wavevector and we even observe entanglement vanishing for large emission angles. Our experimental results, backed by theoretical modeling, yield a brand-new understanding of cascaded emission for various quantum emitters. In addition, our model provides quantitative guidelines for designing optical microcavities that retain both a high degree of entanglement and collection efficiency, moving the community one step further towards an ideal source of entangled photons for quantum technologies. The assumption that light sources based on radiative cascades provide maximally polarization-entangled photons is not always correct. Here the authors show experimentally in cavity-embedded quantum dots that photon polarization correlates with its emission mode, impacting the degree of entanglement for emitted photon pairs.
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 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.
We analyze the entanglement properties of deterministic path-entangled photonic states generated by coupling the emission of a quantum-dot biexciton cascade to a chiral nanophotonic waveguide, as implemented by \O{}stfeldt et al. [PRX Quantum 3, 020363 (2022)]. We model the degree of entanglement through the concurrence of the two-photon entangled state in the presence of realistic experimental imperfections. The model accounts for imperfect chiral emitter-photon interactions in the waveguide and the asymmetric coupling of the exciton levels introduced by fine-structure splitting along with time jitter in the detection of photons. The analysis shows that the approach offers a promising platform for deterministically generating entanglement in integrated nanophotonic systems in the presence of realistic experimental imperfections.
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.