Emission Of Colloidal Quantum Dots Research Articles

Coherent THz wave emission from HgTe quantum dots

Mercury telluride (HgTe) nanocrystals (NCs) are very promising for THz technology as they exhibit broad THz absorption resonances and a carrier lifetime of a few picoseconds as well as being easily fabricated using solution synthesis. In this work, we show their light emission properties in the THz spectral range, up until now unexplored, and show how THz pulse generation can be used for microscopic insights into these NCs. In particular, we report on coherent THz emission from large HgTe NCs excited by linearly polarized optical pulses via second-order nonlinear effects. The peak emission frequency is tunable from 0.4 to 0.8 THz by varying incident angles of optical pulses from 0° to 45°. Our results reveal that the THz emission is induced by transient photocurrents arising from both photogalvanic and photon drag effects. By pushing the light emission of colloidal quantum dots down to the THz spectral range, our study expands the application fields of NCs, especially toward the development of easily integrable and tunable THz emitters and quantum THz devices.

Optical-Gain-based Sensing Using Inorganic-Ligand-Passivated Colloidal Quantum Dots.

Thanks to their extremely large surface-to-volume ratio, colloidal quantum dots are potential high-performance sensing materials. However, previous sensing works using their spontaneous emission suffer from low sensitivities. The absence of an amplification process and the presence of the steric hindrance of long-chain organic ligands are two possible causations. Herein we propose that these two issues can be circumvented by using the amplified spontaneous emission of colloidal quantum dots capped by short-chain inorganic ligands. To exemplify this concept, we performed humidity sensing and observed a ∼31 times enhancement in sensitivity. Meanwhile, we found that the amplified spontaneous emission threshold power was reduced by 34% in a high humidity environment. On the basis of our transient absorption measurements, we attribute these observations to the mitigation of ultrafast subpicosecond trapping processes, which are enabled by the absorption of water molecules.

Direction control of colloidal quantum dot emission using dielectric metasurfaces

Abstract Owing to the recent developments of dielectric metasurfaces, their applications have been expanding from those pertaining to the thickness shrinkage of passive optical elements, such as lenses, polarizers, and quarter-wave plates, to applications pertaining to their integration with active optical devices, such as vertical-cavity surface-emitting lasers. Even though directional lasing and beam shaping of laser emission have been successfully demonstrated, the integration of metasurfaces with random light sources, such as light-emitting diodes, is limited because of function and efficiency issues attributed to the fact that metasurfaces are basically based on the resonance property of the nanostructure. To control the direction of emission from colloidal quantum dots, we present a dielectric metasurface deflector composed of two asymmetric TiO2 nanoposts. TiO2 deflector arrays were fabricated with a dry etching method that is adaptive to mass production and integrated with a colloidal quantum dot resonant cavity formed by sandwiching two distributed Bragg reflectors. To ensure the deflection ability of the fabricated sample, we measured the photoluminescence and far-field patterns of emission from the resonant cavity. From the obtained results, we demonstrated that the colloidal quantum dot emission transmitted through our deflector arrays was deflected by 18°, and the efficiency of deflection was 71% with respect to the emission from the resonant cavity. This integration of dielectric metasurfaces with a resonant cavity shows the possibility of expanding the application of visible metasurfaces in active devices and may help to develop next-generation active devices with novel functions.

Greatly amplified spontaneous emission of colloidal quantum dots mediated by a dielectric-plasmonic hybrid nanoantenna

Abstract Optical nanoantennas can efficiently harvest electromagnetic energy from nanoscale space and boost the local radiation to the far field. The dielectric-metal nanogap is a novel design that can help to overcome the core issue of optical loss in all-metal nanostructures while enabling photon density of states larger than that in all-dielectric counterparts. This article reports that a crystalline spherical silicon nanoparticle on metal film (SiNPoM) nanoantenna can largely enhance the spontaneous emission intensity of quantum dots by an area-normalized factor of 69 and the decay rate by 42-fold compared with quantum dots on glass. A high total quantum efficiency of over 80%, including ~20% for far-field radiation and ~60% for surface plasmon polaritons, is obtained in simulation. Thanks to not only the low optical loss in dielectric nanoparticles but also the appropriate gap thickness which weakens the non-radiative decay due to the quenching from metal. Mie resonant modes additionally provide the flexible control of far-field emission patterns. Such a simple optical nanoantenna can be combined with various nanoscale optical emitters and easily extended to form large area metasurfaces functioning as active regions in light-emitting devices in applications such as advanced display, wireless optical communication, and quantum technology.

Models of semiconductor quantum dots blinking based on spectral diffusion -=SUP=-*-=/SUP=-

AbstractThree models of single colloidal quantum dot emission fluctuations (blinking) based on spectral diffusion were considered analytically and numerically. It was shown that the only one of them, namely the Frantsuzov and Marcus model reproduces the key properties of the phenomenon. The other two models, the Diffusion-Controlled Electron Transfer (DCET) model and the Extended DCET model predict that after an initial blinking period, most of the QDs should become permanently bright or permanently dark which is significantly different from the experimentally observed behavior.

Models of Semiconductor Quantum Dots Blinking based on Spectral Diffusion

Three models of single colloidal quantum dot emission fluctuations (blinking) based on spectral diffusion were considered analytically and numerically. It was shown that the only one of them, namely the Frantsuzov and Marcus model reproduces the key properties of the phenomenon. The other two models, the Diffusion-Controlled Electron Transfer (DCET) model and the Extended DCET model predict that after an initial blinking period, most of the QDs should become permanently bright or permanently dark which is significantly different from the experimentally observed behavior.

Polarized emission in II–VI and perovskite colloidal quantum dots

The polarized emission of colloidal quantum dots from II–VI and perovskite semiconductors were investigated thoroughly, revealing information about the optical transitions in these materials and their potential use in various opto-electronic or spintronic applications. The studies included recording of the micro-photoluminescence of individual nanostructures at cryogenic temperatures, with or without the influence of an external magnetic field. The experimental conditions enabled detection of circular and/or linear polarized emission to elucidate the exciton manifolds, angular momentum of the emitting states, Landé g-factors, single exciton and bi-exciton binding energies, the excitons’ effective Bohr radii, and the unique influence of the Rashba effect. The study advances the understanding of other phenomena such as electron–hole dissociation, long diffusion lengths, and spin coherence, facilitating appropriate design of optical and spin-based devices.

Impact of photoinduced processes on the plasmonic enhancement of colloidal quantum dot emission

ABSTRACTWe study the mutual effects of photoinduced processes (irradiation effects) and plasmonic emission enhancement in close-packed CdSe/ZnS colloidal quantum dots in the vicinity of gold metallic nanoparticles with two significantly different size distributions. For this we examine the impact of the heat generated by the metallic nanoparticles, the strength of plasmonic field enhancement, and the rate of energy transfer from the quantum dots to metallic nanoparticles in the presence of a laser field with low and moderate intensities. Our results show that the interplay between the photophysics of the quantum dots and their plasmonic emission enhancement is significantly pronounced when the metallic nanoparticles are large. In such a case we observed large suppression of photoinduced fluorescence enhancement (PFE). For smaller metallic nanoparticles the results suggest mostly an overall time-independent suppression of the quantum dots’ emission with no significant impact on PFE.

Wavelength, Concentration, and Distance Dependence of Nonradiative Energy Transfer to a Plane of Gold Nanoparticles

Nonradiative energy transfer to metal nanoparticles is a technique used for optical-based distance measurements which is often implemented in sensing. Both Förster resonant energy transfer (FRET) and nanometal surface energy transfer (NSET) mechanisms have been proposed for emission quenching in proximity to metal nanoparticles. Here quenching of emission of colloidal quantum dots in proximity to a monolayer of gold nanoparticles is investigated. Five differently sized CdTe quantum dots are used to probe the wavelength dependence of the quenching mechanism as their emission peak moves from on resonance to off resonance with respect to the localized surface plasmon peak of the gold nanoparticle layer. The gold nanoparticle concentration and distance dependences of energy transfer are discussed. Photoluminescence quenching and lifetime data are analyzed using both FRET and NSET models and the extracted characteristic distances are compared with theory. Good agreement with FRET theory has been found for quantum dots with emission close to the localized surface plasmon resonance, though larger than expected Förster radii are observed for quantum dots with emission red-shifted with respect to the localized surface plasmon peak. Closer agreement between experimental and theoretical characteristic distances can be found across the full wavelength range within a NSET approach.

Correlations between Subsequent Blinking Events in Single Quantum Dots

We explain the long-range correlations found by Stefani and his co-workers between blinking times of single colloidal quantum dot emission. Our explanation is based on the multiple recombination center model we recently suggested. The model produces positive correlations between subsequent on--on and off--off times and negative on--off correlations, as observed in the experiment. We also reproduce qualitatively the dependence of correlations between subsequent on--on, on-off, and off--off times on the number of switching events separating them.

Universal Role of Discrete Acoustic Phonons in the Low-Temperature Optical Emission of Colloidal Quantum Dots

Multiple energy scales contribute to the radiative properties of colloidal quantum dots, including magnetic interactions, crystal field splitting, Pauli exclusion, and phonons. Identification of the exact physical mechanism which couples first to the dark ground state of colloidal quantum dots, inducing a significant reduction in the radiative lifetime at low temperatures, has thus been under significant debate. Here we present measurements of this phenomenon on a variety of materials as well as on colloidal heterostructures. These show unambiguously that the dominant mechanism is coupling of the ground state to a confined acoustic phonon, and that this mechanism is universal.

Statistical analysis of time-resolved emission from ensembles of semiconductor quantum dots: Interpretation of exponential decay models

We present a statistical analysis of time-resolved spontaneous emission decay curves from ensembles of emitters, such as semiconductor quantum dots, with the aim of interpreting ubiquitous non-single-exponential decay. Contrary to what is widely assumed, the density of excited emitters and the intensity in an emission decay curve are not proportional, but the density is a time integral of the intensity. The integral relation is crucial to correctly interpret non-single-exponential decay. We derive the proper normalization for both a discrete and a continuous distribution of rates, where every decay component is multiplied by its radiative decay rate. A central result of our paper is the derivation of the emission decay curve when both radiative and nonradiative decays are independently distributed. In this case, the well-known emission quantum efficiency can no longer be expressed by a single number, but is also distributed. We derive a practical description of non-single-exponential emission decay curves in terms of a single distribution of decay rates; the resulting distribution is identified as the distribution of total decay rates weighted with the radiative rates. We apply our analysis to recent examples of colloidal quantum dot emission in suspensions and in photonic crystals, and we find that this important class of emitters is well described by a log-normal distribution of decay rates with a narrow and a broad distribution, respectively. Finally, we briefly discuss the Kohlrausch stretched-exponential model, and find that its normalization is ill defined for emitters with a realistic quantum efficiency of less than 100%.