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During recent years our enthusiasm for Radiative Decay Engineering (RDE) has continually increased. Many of the early predictions have been confirmed.
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CHE342 L13 Radiative decay

We show that metamaterials with hyperbolic dispersion support a large number of electromagnetic states that can couple to quantum emitters leading to a broadband Purcell effect. The proposed approach of radiative decay engineering, useful for applications such as single photon sources, fluorescence imaging, biosensing, and single molecule detection, also opens up the possibility of using hyperbolic metamaterials to probe the spontaneous emission properties of atoms and artificial atoms such as quantum dots. C American Institute of Physics. Advanced Search.

Privacy Copyright. Skip to main content Purdue e-Pubs. Analytical Biochemistry [14 Oct , ]. Type: Research Support, Non-U.

Radiative decay engineering 5: metal-enhanced fluorescence and plasmon emission.

Abstract There is a continuing need to increase the brightness and photostability of fluorophores for use in biotechnology, medical diagnostics, and cell imaging. One approach developed during the past decade is to use metallic surfaces and nanostructures. It is now known that excited state fluorophores display interactions with surface plasmons, which can increase the radiative decay rates, modify the spatial distribution of emission, and result in directional emission. One important example is surface plasmon-coupled emission SPCE. In this phenomenon, the fluorophores at close distances from a thin metal film, typically silver, display emission over a small range of angles into the substrate.

A disadvantage of SPCE is that the emission occurs at large angles relative to the surface normal and at angles that are larger than the critical angle for the glass substrate. In the current article, we describe a simple multilayer metal-dielectric structure that allows excitation with light that is perpendicular normal to the plane and provides emission within a narrow angular distribution that is normal to the plane. This structure consists of a thin silver film on top of a multilayer dielectric Bragg grating, with no nanoscale features except for the metal or dielectric layer thicknesses.

Our structure is designed to support optical Tamm states, which are trapped electromagnetic modes between the metal film and the underlying Bragg grating. We used simulations with the transfer matrix method to understand the optical properties of Tamm states and localization of the modes or electric fields in the structure. Tamm states can exist with zero in-plane wavevector components and can be created without the use of a coupling prism. Crossover of the Auger rates of two types of basic channels observed here has neither been predicted by theory nor reported experimentally yet.

This would result in overall less efficient Auger recombination of positive trion than that of the corresponding negative trion for those specific QDs Fig. As the shell thickness increases, the other factors well documented in literature overtake the dominating role and cause rate crossover between the Auger recombination of two basic channels. Geometry-dependent dielectric screening not only is responsible for the Auger rate crossover but also represents a new strategy for Auger engineering, which can independently tune the rate of either basic type of Auger recombination.

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We are actively working on these directions, aiming to further enlarge the tuning range of the rates of two basic types of Auger recombination. In terms of non-radiative carrier dynamics, two elementary processes are important. One is the carrier cooling assisted by electron-phonon coupling after excitation, and the other is the electron-electron interaction induced Auger recombination. In the current experiment, the measured photoluminescence decay dynamics is in the nanosecond time range after the initial excitation.

This is far beyond the initial hot carrier cooling, which typically happens within a few picoseconds. We can thus assume the Auger processes start from the ground state of a trion.

Single photon gun: Radiative decay engineering with metamaterials

There is a phonon-assisted Auger process 65 , Within this process, not only the electron or hole can be excited to their higher energy states through the electron-electron interaction, but phonons can be absorbed or emitted. However, these additional channels do not change the overall oscillator strength of the Auger process. Instead, they just spread out the original zero phonon Auger line, thus broadening the Auger peak. In the current study, this effect has been approximated by using a finite broadening of the energy delta function in the Fermi golden rule in Eq.

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Further increasing the peak width does not significantly change the results. In summary, our results suggest that further suppression or enhancement of Auger recombination is feasible with the new strategy. For conventional ensemble optical measurements, QD samples were diluted in toluene until the optical density was around 0. For single-dot spectroscopy experiments, diluted QD solution in toluene with 2.

All optical measurements were performed at room temperature. Steady-state and transient photoluminescence spectra were recorded on an Edinburgh Instruments FLS spectrometer. The system was calibrated with a DHcal standard light source. With different excitation power densities, a series of transient photoluminescence spectra were obtained and thus the biexciton lifetime and QY could be calculated. Photoluminescence intensity trajectories and transient photoluminescence spectra of single QD were measured simultaneously with the same single-photon counting system mentioned above in a time-tagged time-resolved TTTR mode.

After a few minutes of photo-radiation, the QD sample reached a steady-state, indicated by stable absorption and photoluminescence spectra. All above operations were performed at room temperature and under N 2 atmosphere in a glove box. The authors declare that all data supporting the findings of this investigation are available within the article, its Supplementary Information, and from the corresponding authors upon reasonable request. An amendment to this paper has been published and can be accessed via a link at the top of the paper. Brus, L. Electron electron and electron-hole interactions in small semiconductor crystallites—the size dependence of the lowest excited electronic state.

Chepic, D. Auger ionization of semiconductor quantum drops in a glass matrix. Klimov, V. Quantization of multiparticle Auger rates in semiconductor quantum dots. Science , — Pietryga, J.

Radiative decay engineering 5: metal-enhanced fluorescence and plasmon emission.

Spectroscopic and device aspects of nanocrystal quantum dots. Wang, L. Pseudopotential theory of Auger processes in CdSe quantum dots. Optical gain and stimulated emission in nanocrystal quantum dots. Zhu, H. Fan, F.

Continuous-wave lasing in colloidal quantum dot solids enabled by facet-selective epitaxy. Nature , 75—79 Shirasaki, Y. Emergence of colloidal quantum-dot light-emitting technologies.

Lim, J. Droop-free colloidal quantum dot light-emitting diodes. Nano Lett. Bae, W. Controlling the influence of Auger recombination on the performance of quantum-dot light-emitting diodes. Nirmal, M. Fluorescence intermittency in single cadmium selenide nanocrystals.

Nature , — Efros, A. Origin and control of blinking in quantum dots. Qin, H. Photoluminescence intermittency and photo-bleaching of single colloidal quantum dot. Lidke, K. Superresolution by localization of quantum dots using blinking statistics. Express 13 , — Pinaud, F. Probing cellular events, one quantum dot at a time. Methods 7 , — Dertinger, T. Natl Acad. USA , — Lounis, B. Michler, P.