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arXiv:2509.11704

Heralded Emission Detection in InAs/ZnSe Quantum Dot Solids Using Time-Correlated Photons

Tsao, Chieh, Xiang Li, Alex Hinkle, Chen, Yifan, Elvar Oskarsson, Uri Banin, Hendrik Utzat

Published Sep 15, 2025• 0 citations
arXivHTMLPDF

Abstract

Harnessing quantum correlations between photons is an emerging frontier in optical spectroscopy, yet experimental demonstrations have largely remained limited to molecular systems at room temperature. Here, we investigate heralded emission detection (HED) under continuous-wave entangled-photon excitation of near-infrared (NIR)-emitting colloidal III-V quantum dot (QD) solids at low temperatures. We demonstrate the advantages of superconducting nanowire single-photon detectors (SNSPDs) for high time resolution ($\sim$72 ps) and large-area NIR avalanche photodiodes (APDs) for high emission count rates ($\sim$2000 cps). Second-order photon-correlation analysis reveals exciton lifetimes and fine-structure energy splittings. These results establish NIR colloidal QDs as a bright, tunable model system for quantum-light spectroscopy and highlight their compatibility with optical cavities as a further experimental control parameter.

DOI
10.48550/arxiv.2509.11704

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Scientific Reports•Nov 4, 2019•11 citations
Harnessing quantum correlations between photons is an emerging frontier in optical spectroscopy, yet experimental demonstrations have largely remained limited to molecular systems at room temperature. Here, we investigate heralded emission detection (HED) under continuous-wave entangled-photon excitation of near-infrared (NIR)-emitting colloidal III-V quantum dot (QD) solids at low temperatures. We demonstrate the advantages of superconducting nanowire single-photon detectors (SNSPDs) for high time resolution (∼\sim∼72 ps) and large-area NIR avalanche photodiodes (APDs) for high emission count rates (∼\sim∼2000 cps). Second-order photon-correlation analysis reveals exciton lifetimes and fine-structure energy splittings. These results establish NIR colloidal QDs as a bright, tunable model system for quantum-light spectroscopy and highlight their compatibility with optical cavities as a further experimental control parameter.
Mid-infrared (MIR) spectroscopy serves as a powerful tool for molecular structure identification and chemical composition analysis. However, conventional Fourier-transform infrared spectrometers (FTIR) demonstrate compromised signal-to-noise ratios (SNR) under low-light conditions, which severely limit their performance in high-sensitivity applications. Although MIR superconducting nanowire single-photon detectors (SNSPDs) offer high detection efficiency and low timing jitter, their performance is hindered by background dark counts caused by room-temperature blackbody radiation. In this work, we present a quantum-correlated absorption spectroscopy platform that combines MIR-SNSPDs with entangled photon pairs to overcome these limitations. Leveraging the intrinsic temporal and spectral correlations of the photon pairs, coincidence detection effectively distinguishes signal photons from dominant thermal noise, achieving a remarkable improvement of two orders of magnitude in SNR under ultralow pump power conditions. The system achieves a spectral coverage of 3350-3540 nm with a resolution of 3.7 cm -1 at 3.4 µm, operating at an ultralow illumination photon flux of 4.4 × 10 6 photons/s. Validation experiments using polystyrene and polyethylene samples successfully detected CH 2 vibrational modes, demonstrating the platform’s capability for ultrasensitive biochemical analysis and material characterization. By integrating quantum correlation with MIR-SNSPDs, this work establishes a new paradigm for high-performance MIR spectroscopy in low-light scenarios.
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.
We report the observation of photon antibunching from a single, self-assembled InGaAs quantum dot (QD) at temperatures up to 135 K. The second-order intensity correlation,g(2)g^{(2)}g(2)(0), is less than 0.260$\pm0.024fortemperaturesupto100K.At120K,0.024 for temperatures up to 100 K. At 120 K,0.024fortemperaturesupto100K.At120K,g^{(2)}(0)increasestoabout0.471,whichisslightlylessthanthesecond−orderintensitycorrelationexpectedfromtwoindependentsingleemitters.Inaddition,wecharacterizetheperformanceofasuperconductingsinglephotondetector(SSPD)basedonananopatternedniobiumnitridewirethatexhibits68(0) increases to about 0.471, which is slightly less than the second-order intensity correlation expected from two independent single emitters. In addition, we characterize the performance of a superconducting single photon detector (SSPD) based on a nanopatterned niobium nitride wire that exhibits 68(0)increasestoabout0.471,whichisslightlylessthanthesecond−orderintensitycorrelationexpectedfromtwoindependentsingleemitters.Inaddition,wecharacterizetheperformanceofasuperconductingsinglephotondetector(SSPD)basedonananopatternedniobiumnitridewirethatexhibits68\pm3−pstimingjitterandlessthan100−Hzdarkcountratewithadetectionefficiency(DE)ofupto23-ps timing jitter and less than 100-Hz dark count rate with a detection efficiency (DE) of up to 2% at 902 nm. This detector is used to measure spontaneous emission lifetimes of semiconductor quantum wells (QWs) emitting light at wavelengths of 935 and 1245 nm. The sensitivity to wavelengths longer than 13−pstimingjitterandlessthan100−Hzdarkcountratewithadetectionefficiency(DE)ofupto2\mumandtheGaussiantemporalresponseofthissuperconductingdetectorpresentclearadvantagesovertheconventionaldetectortechnologies.WealsousethisdetectortocharacterizetheemissionfromasingleInGaAsQDembeddedinamicropillarcavity,measuringaspontaneousemissionlifetimeof370psandam and the Gaussian temporal response of this superconducting detector present clear advantages over the conventional detector technologies. We also use this detector to characterize the emission from a single InGaAs QD embedded in a micropillar cavity, measuring a spontaneous emission lifetime of 370 ps and amandtheGaussiantemporalresponseofthissuperconductingdetectorpresentclearadvantagesovertheconventionaldetectortechnologies.WealsousethisdetectortocharacterizetheemissionfromasingleInGaAsQDembeddedinamicropillarcavity,measuringaspontaneousemissionlifetimeof370psandag^{(2)}(0)of0.24(0) of 0.24(0)of0.24\pm$0.03.
We report the routing of quantum light emitted by self-assembled InGaAs quantum dots (QDs) into the optical modes of a GaAs ridge waveguide and its efficient detection on-chip via evanescent coupling to NbN superconducting nanowire single photon detectors (SSPDs). The waveguide coupled SSPDs primarily detect QD luminescence, with scattered photons from the excitation laser onto the proximal detector being negligible by comparison. The SSPD detection efficiency from the evanescently coupled waveguide modes is shown to be two orders of magnitude larger when compared with operation under normal incidence illumination, due to the much longer optical interaction length. Furthermore, in-situ time resolved measurements performed using the integrated detector show an average QD spontaneous emission lifetime of 0.95 ns, measured with a timing jitter of only 72 ps. The performance metrics of the SSPD integrated directly onto GaAs nano-photonic hardware confirms the strong potential for on-chip few-photon quantum optics using such semiconductor-superconductor hybrid systems.
We describe the design and characterization of a fiber-coupled double-channel single-photon detection system based on superconducting single-photon detectors (SSPD), and its application for quantum optics experiments on semiconductor nanostructures. When operated at 2-K temperature, the system shows 10% quantum efficiency at 1.3-¿m wavelength with dark count rate below 10 counts per second and timing resolution <100 ps. The short recovery time and absence of afterpulsing leads to counting frequencies as high as 40 MHz. Moreover, the low dark count rate allows operation in continuous mode (without gating). These characteristics are very attractive-as compared to InGaAs avalanche photodiodes-for quantum optics experiments at telecommunication wavelengths. We demonstrate the use of the system in time-correlated fluorescence spectroscopy of quantum wells and in the measurement of the intensity correlation function of light emitted by semiconductor quantum dots at 1300 nm.
Abstract The realization of high-quality quantum emitters that can operate at room temperature is important for accelerating the application of quantum technologies, such as quantum communication, quantum information processing, and quantum metrology. In this work, we study the photon-antibunching properties on room-temperature emission from individual colloidal quantum dots (CQDs) using superconducting-nanowire single-photon detectors and temporal filtering of the photoluminescence decay curve. We find that high single-photon purities and high photon-generation rates can be simultaneously achieved by removing the signals originating from the sequential two-photon emission of biexcitons created by multiple excitation pulses. We successfully demonstrate that the ultrahigh performance of the room-temperature single-photon sources showing g(2)(0) ≪ 10−2 can be confirmed by the ultralow-dark-count detection of the temporally purified single photons. These findings provide strong evidence for the attractiveness of CQDs as candidates for high-quality room-temperature quantum light sources.