Intermittency of CsPbBr$_3$ perovskite quantum dots analyzed by an unbiased statistical analysis
Isabelle M. Palstra, Ilse Maillette de Buy Wenniger, Biplab K. Patra, Erik C. Garnett, A. Femius Koenderink
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Preprint itself 32 pages double spaced with 7 figures. Remainder is supplementary data plots for 40 single quantum dots First update: inserted ZENODO data link, and arxiv identifier for related reference
We analyze intermittency in intensity and fluorescence lifetime of CsPbBr$_3$ perovskite quantum dots by applying unbiased Bayesian inference analysis methods. We apply changepoint analysis (CPA) and a Bayesian state clustering algorithm to determine the timing of switching events and the number of states between which switching occurs in a statistically unbiased manner, which we have benchmarked particularly to apply to highly multistate emitters. We conclude that perovskite quantum dots display a plethora of gray states in which brightness broadly speaking correlates inversely with decay rate, confirming the multiple recombination centers model. We leverage the CPA partitioning analysis to examine aging and memory effects. We find that dots tend to return to the bright state before jumping to a dim state, and that when choosing a dim state they tend to explore the entire set of states available.
Carrier spins in semiconductor nanocrystals are promising candidates for quantum information processing. Using a combination of time-resolved Faraday rotation and photoluminescence spectroscopies, we demonstrate optical spin polarization and coherent spin precession in colloidal CsPbBr3 nanocrystals that persists up to room temperature. By suppressing the influence of inhomogeneous hyperfine fields with a small applied magnetic field, we demonstrate inhomogeneous hole transverse spin-dephasing times (T2*) that approach the nanocrystal photoluminescence lifetime, such that nearly all emitted ph…
Many-body effect and strong Coulomb interaction in monolayer transition metal dichalcogenides lead to shrink the intrinsic bandgap, originating from the renormalization of electrical/optical bandgap, exciton binding energy, and spin-orbit splitting. This renormalization phenomenon has been commonly observed at low temperature and requires high photon excitation density. Here, we present the augmented bandgap renormalization in monolayer MoS_2 anchored on CsPbBr_3 perovskite quantum dots at room temperature via charge transfer. The amount of electrons significantly transferred from perovskite g…
Room Temperature Collective Blinking and Photon Bunching from CsPbBr3 Quantum Dot Superlattice
Institute of Science Tokyo（东京科学大学）；Katholieke Universiteit Leuven（荷语鲁汶大学）；Lingnan Normal University（岭南师范学院）；Max Planck Institute for Polymer Research（马克斯·普朗克聚合物研究所）
Nonlinear optical responses of all-inorganic lead halide perovskite nanostructures by time-resolved beam-deflection technique
我们研究了非线性折射在全无机卤化物钙钛矿，CsPbBr $_3$和CsPbBr $_{1.5}$ I $_{1.5}$纳米片和量子点胶体在甲苯中，通过一种新的光束偏转技术，使用近共振连续波激光。本文所测量的非线性折射及其随时间的演化是由热透镜效应引起的。热输运的强度依赖的热扩散速率的非线性行为已被观察到。在高强度下测量了对流热流的影响。与相应的纳米片样品相比，量子点具有更高的非线性折射，这可能是由于降低的维度。非线性折射率的有效值，估计在这里的近共振激发，超过那些在文献中报道的有机-无机混合钙钛矿在非共振激发制度，由几个数量级。
We report on a Python-toolbox for unbiased statistical analysis of fluorescence intermittency properties of single emitters. Intermittency, i.e., step-wise temporal variations in the instantaneous emission intensity and fluorescence decay rate properties are common to organic fluorophores, II-VI quantum dots and perovskite quantum dots alike. Unbiased statistical analysis of intermittency switching time distributions, involved levels and lifetimes is important to avoid interpretation artefacts. This work provides an implementation of Bayesian changepoint analysis and level clustering applicabl…
Manipulation of solid-state spin coherence is an important paradigm for quantum information processing. Current systems either operate at very low temperatures or are difficult to scale-up. Developing low-cost, scalable materials whose spins can be coherently manipulated at room temperature is thus highly-attractive for a sustainable future of quantum information science. Here we report ambient-condition all-optical initialization, manipulation and readout of single-hole spins in an ensemble of solution-grown CsPbBr3 perovskite QDs. Single-hole spins are obtained by sub-picosecond electron sca…
Quantum photonics technologies like wavelength division multiplexing (WDM) for high-rate quantum key distribution require narrowband, spectrally tunable single photon emitters. Physical methods that rely on the application of large mechanical strain to epitaxial quantum dots or electric and magnetic fields to color centers in 2D metal dichalcogenides provide limited spectral tunability. Here we adopt a chemical approach to synthesize a family of colloidal mixed-cation perovskite quantum dots ($\text{Cs}_{1-x}\text{FA}_{x}\text{PbBr}_3$) that show highly photo-stable, compositionally tunable si…
The easily tunable emission of halide perovskite nanocrystals throughout the visible spectrum makes them an extremely promising material for light-emitting applications. Whereas high quantum yields and long-term colloidal stability have already been achieved for nanocrystals emitting in the red and green spectral range, the blue region currently lags behind, with low quantum yields, broad emission profiles and insufficient colloidal stability. In this work, we present a facile synthetic approach for obtaining two-dimensional CsPbBr3 nanoplatelets with monolayer-precise control over their thick…
