arXiv subjects

Chieh Tsao

Publications and source records attributed to Chieh Tsao.

5 recordsLinked to original sources

arXiv2026

Selective Biexciton Generation Under Energy-Time Entangled Quantum Light in Quantum Dots

Quantum light provides new opportunities for controlling multiphoton absorption beyond classical limits. Here, we investigate biexciton generation in nanocrystal quantum dots driven by energy-time-entangled photon pairs generated via spontaneous parametric down-conversion. We show that frequency-time correlations between paris of photons increase the population of biexcitons over excitons, thereby lending specificity to the excitation of many-body states. By employing a three-level model, we demonstrate that biexciton generation depends nontrivially on the photon entanglement time and the pump bandwidth. We find that maximizing efficiency requires an optimally shaped entangled photon field rather than simply scaling parameters for a monotonic improvement. Extending to a realistic CdSe/CdS core-shell quantum dot containing many excitonic states coupled to the quantum field, we demonstrate that increasing the bi-photon arrival-time entanglement (closer arrival time) enhances constructive pathway interference and expands accessible excitation channels while preserving better energy-conservation excitation than classical light when generating biexcitons. Furthermore, tuning the time correlation properties enables selective excitation of closely spaced biexciton states. These results establish entangled photons as a new tool for selective excitation and control of higher-order excited states in quantum-confined systems.

physics.chem-ph↗

arXiv2025

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

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.

physics.optics↗

arXiv2025

Multi-Dimensional Photon-Correlations Reveal Triexciton Features in Single Perovskite Quantum Dots

Lead-halide perovskite quantum dots (PQDs) are established quantum emitters with potential for entangled photon-pair generation via multiexciton cascades. However, the energetics and dynamics of many-body excitations remain poorly understood. Here, we perform time- and frequency-resolved photon-correlation spectroscopy of single CsPbBr\textsubscript{3} PQDs at low temperatures using a single-photon avalanche diode (SPAD) array detector. We report biexciton binding energies and assign their charged states, which undergo fast ($μ$s) switching dynamics. Most notably, we identify a spectral feature blue-shifted from the exciton by $7.4 \pm 1.9$ meV as the bound triexciton and establish the order of its cascade emission. These results highlight the power of low-temperature, multidimensional photon-correlation spectroscopy for resolving complex many-body dynamics.

cond-mat.mtrl-sci↗

arXiv2025

Enhancing Spectroscopy and Microscopy with Emerging Methods in Photon-Correlation and Quantum Illumination

Quantum optics has driven major advances in our ability to generate and detect correlations between individual photons. Its principles are now increasingly translated into nanoscale characterization techniques, enhancing spectroscopy, microscopy, and metrology. In this Review, we highlight rapid progress in the field driven by advances in single-photon detectors and quantum light sources, including time-resolved single-photon counting cameras, superconducting nanowire detectors, and increasingly bright sources of entangled photons. We emphasize emerging applications in super-resolution microscopy, measurements below classical noise limits, and photon-number-resolved spectroscopy-a powerful paradigm for probing nanoscale electronic materials and molecular dynamics. We conclude by outlining key technological challenges and future opportunities across materials science and bio-nanophotonics.

physics.optics↗

arXiv2024

Stochastic Frequency Fluctuation Super-Resolution Imaging

The inherent non-linearity of intensity correlation functions can be used to spatially distinguish identical emitters beyond the diffraction limit, as achieved, for example, in Super-Resolution Optical Fluctuation Imaging (SOFI). Here, we propose a complementary concept based on spectral correlation functions, termed Spectral Fluctuation Super-Resolution (SFSR) imaging. Through theoretical and computational analysis, we show that spatially resolving time-frequency correlation functions in the image plane can improve the imaging resolution by a factor of $\sqrt2$ in most cases and up to twofold for strictly two emitters. This improvement is achieved by quantifying the degree of correlation in spectral fluctuations across the spatial domain. Experimentally, SFSR can be implemented using a combination of interferometry and photon-correlation measurements. The method works for non-blinking emitters and stochastic spectral fluctuations with arbitrary temporal statistics. This suggests its utility in super-resolution microscopy of quantum emitters at low temperatures, where spectral diffusion is often more pronounced than emitter blinking.

physics.optics↗