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Added by
Roberto N. Mu\\~noz
Publication date
2021
fields
Physics
and research's language is
English
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The photoluminescence intermittency (blinking) of quantum dots is interesting because it is an easily-measured quantum process whose transition statistics cannot be explained by Fermis Golden Rule. Commonly, the transition statistics are power-law distributed, implying that quantum dots possess at least trivial memories. By investigating the temporal correlations in the blinking data, we demonstrate with high statistical confidence that quantum dot blinking data has non-trivial memory, which we define to be statistical complexity greater than one. We show that this memory cannot be discovered using the transition distribution. We show by simulation that this memory does not arise from standard data manipulations. Finally, we conclude that at least three physical mechanisms can explain the measured non-trivial memory: 1) Storage of state information in the chemical structure of a quantum dot; 2) The existence of more than two intensity levels in a quantum dot; and 3) The overlap in the intensity distributions of the quantum dot states, which arises from fundamental photon statistics.
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Photoluminescence (PL) intermittency is a ubiquitous phenomenon detrimentally reducing the temporal emission intensity stability of single colloidal quantum dots (CQDs) and the emission quantum yield of their ensembles. Despite efforts for blinking reduction via chemical engineering of the QD architecture and its environment, blinking still poses barriers to the application of QDs, particularly in single-particle tracking in biology or in single-photon sources. Here, we demonstrate the first deterministic all-optical suppression of quantum dot blinking using a compound technique of visible and mid-infrared (MIR) excitation. We show that moderate-field ultrafast MIR pulses (5.5 $mu$m, 150 fs) can switch the emission from a charged, low quantum yield grey trion state to the bright exciton state in CdSe/CdS core-shell quantum dots resulting in a significant reduction of the QD intensity flicker. Quantum-tunneling simulations suggest that the MIR fields remove the excess charge from trions with reduced emission quantum yield to restore higher brightness exciton emission. Our approach can be integrated with existing single-particle tracking or super-resolution microscopy techniques without any modification to the sample and translates to other emitters presenting charging-induced PL intermittencies, such as single-photon emissive defects in diamond and two-dimensional materials.
The blinking dynamics of colloidal core-shell CdSe/CdS dot-in-rods is studied in detail at the single particle level. Analyzing the autocorrelation function of the fluorescence intensity, we demonstrate that these nanoemitters are characterized by a short value of the mean duration of bright periods (ten to a few hundreds of microseconds). The comparison of the results obtained for samples with different geometries shows that not only the shell thickness is crucial but also the shape of the dot- in-rods. Increasing the shell aspect ratio results in shorter bright periods suggesting that surface traps impact the stability of the fluorescence intensity.
Abrupt fluorescence intermittency or blinking is long recognized to be characteristic of single nano-emitters. Extended quantum-confined nanostructures also undergo spatially heterogeneous blinking, however, there is no such precedence in dimensionally unconfined (bulk) materials. Here, we report multi-level blinking of entire individual organo-lead bromide perovskite micro-crystals (volume 0.1-3 micron-cuble) under ambient conditions. Extremely high spatiotemporal correlation (>0.9) in intra-crystal emission intensity fluctuations signifies effective communication amongst photogenerated carriers at distal locations (up to ~4 microns) within each crystal. Fused polycrystalline grains also exhibit this intriguing phenomenon, which is rationalized by correlated and efficient migration of carriers to a few transient non-radiative traps, the nature and population of which determine blinking propensity. Observation of spatiotemporally correlated emission intermittency in bulk semiconductor crystals opens up the possibility to design novel devices involving long range (mesoscopic) electronic communication.
We report reproducible fabrication of InP-InAsP nanowire light emitting diodes in which electron-hole recombination is restricted to a quantum-dot-sized InAsP section. The nanowire geometry naturally self-aligns the quantum dot with the n-InP and p-InP ends of the wire, making these devices promising candidates for electrically-driven quantum optics experiments. We have investigated the operation of these nano-LEDs with a consistent series of experiments at room temperature and at 10 K, demonstrating the potential of this system for single photon applications.
Photo-luminescence intermittency (blinking) in semiconductor nanocrystals (NCs), a phenomenon ubiquitous to single-emitters, is generally considered to be temporally random intensity fluctuations between bright (On) and dark (Off) states. However, individual quantum-dots (QDs) rarely exhibit such telegraphic signal, and yet, the vast majority of single-NC blinking data are analyzed using a single fixed threshold, which generates binary trajectories. Further, blinking dynamics can vary dramatically over NCs in the ensemble, and it is unclear whether the exponents (m) of single-particle On-/Off-time distributions (P(t)-On/Off), which are used to validate mechanistic models of blinking, are narrowly distributed or not. Here, we sub-classify an ensemble based on the emissivity of QDs, and subsequently compare the (sub)ensemble behaviors. To achieve this, we analyzed a large number (>1000) of intensity trajectories for a model system, Mn+2 doped ZnCdS QDs, which exhibits diverse blinking dynamics. An intensity histogram dependent thresholding method allowed us to construct distributions of relevant blinking parameters (such as m). Interestingly, we find that single QD P(t)-On/Off s follow either truncated power law or power law, and their relative proportion vary over sub-populations. Our results reveal a remarkable variation in m(On/Off) amongst as well as within sub-ensembles, which implies multiple blinking mechanisms being operational among various QDs. We further show that the m(On/Off) obtained via cumulative single-particle P(t)-On/Off is clearly distinct from the weighted mean value of all single-particle m(On/Off), an evidence for the lack of ergodicity. Thus, investigation and analyses of a large number of QDs, albeit for a limited time-span of few decades, is crucial to characterize possible blinking mechanisms and heterogeneity therein
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