Quantum dots or rings are artificial nanometre-sized clusters that confine electrons in all three directions. They can be fabricated in a semiconductor system by embedding an island of low-bandgap material in a sea of material with a higher bandgap. Quantum dots are often referred to as artificial atoms because, when filled sequentially with electrons, the charging energies are pronounced for particular electron numbers; this is analogous to Hund's rules in atomic physics. But semiconductors also have a valence band with strong optical transitions to the conduction band. These transitions are the basis for the application of quantum dots as laser emitters, storage devices and fluorescence markers. Here we report how the optical emission (photoluminescence) of a single quantum ring changes as electrons are added one-by-one. We find that the emission energy changes abruptly whenever an electron is added to the artificial atom, and that the sizes of the jumps reveal a shell structure.

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Optical emission from a charge-tunable quantum ring

The photoluminescence from a variety of individual molecules and nanometre-sized crystallites is defined by large intensity fluctuations, known as 'blinking', whereby their photoluminescence turns 'on' and 'off' intermittently, even under continuous photoexcitation. For semiconductor nanocrystals, it was originally proposed that these 'off' periods corresponded to a nanocrystal with an extra charge. A charged nanocrystal could have its photoluminescence temporarily quenched owing to the high efficiency of non-radiative (for example, Auger) recombination processes between the extra charge and a subsequently excited electron-hole pair; photoluminescence would resume only after the nanocrystal becomes neutralized again. Despite over a decade of research, completely non-blinking nanocrystals have not been synthesized and an understanding of the blinking phenomenon remains elusive. Here we report ternary core/shell CdZnSe/ZnSe semiconductor nanocrystals that individually exhibit continuous, non-blinking photoluminescence. Unexpectedly, these nanocrystals strongly photoluminesce despite being charged, as indicated by a multi-peaked photoluminescence spectral shape and short lifetime. To model the unusual photoluminescence properties of the CdZnSe/ZnSe nanocrystals, we softened the abrupt confinement potential of a typical core/shell nanocrystal, suggesting that the structure is a radially graded alloy of CdZnSe into ZnSe. As photoluminescence blinking severely limits the usefulness of nanocrystals in applications requiring a continuous output of single photons, these non-blinking nanocrystals may enable substantial advances in fields ranging from single-molecule biological labelling to low-threshold lasers.

Non-blinking semiconductor nanocrystals

Picosecond optical excitation was used to coherently control the excitation in a single quantum dot on a time scale that is short compared with the time scale for loss of quantum coherence. The excitonic wave function was manipulated by controlling the optical phase of the two-pulse sequence through timing and polarization. Wave function engineering techniques, developed in atomic and molecular systems, were used to monitor and control a nonstationary quantum mechanical state composed of a superposition of eigenstates. The results extend the concept of coherent control in semiconductors to the limit of a single quantum system in a zero-dimensional quantum dot.

https://science.sciencemag.org/content/sci/282/5393/1473.full.pdf

Coherent Optical Control of the Quantum State of a Single Quantum Dot

The authors review the physics of ultrafast dynamics in semiconductors and their heterostructures, including both the observed experimental phenomena and the theoretical description of the processes. These are probed by ultrafast optical excitation, generating nonequilibrium states that can be monitored by time-resolved spectroscopy. Light pulses create coherent superpositions of states, and the dynamics of the associated phase relationships can be directly investigated by means of many-pulse experiments. The commonly used experimental techniques are briefly reviewed. A variety of different phenomena can be described within a common theoretical framework based on the density-matrix formalism. The important interactions of the carriers included in the theoretical description are the phonon interactions, the interactions with classical and quantum light fields, and the Coulomb interaction among the carriers themselves. These interactions give rise to a strong interplay between phase coherence and relaxation, which strongly affects the non equilibrium dynamics. Based on the general theory, the authors review the physical phenomena in various semiconductor structures including superlattices, quantum wells, quantum wires, and bulk media. Particular results which have played a central role in understanding the microscopic origins of the relaxation processes are discussed in detail.

Theory of ultrafast phenomena in photoexcited semiconductors

Many potential applications of semiconductor nanocrystals are hindered by nonradiative Auger recombination wherein the electron−hole (exciton) recombination energy is transferred to a third charge carrier. This process severely limits the lifetime and bandwidth of optical gain, leads to large nonradiative losses in light-emitting diodes and photovoltaic cells, and is believed to be responsible for intermittency (“blinking”) of emission from single nanocrystals. The development of nanostructures in which Auger recombination is suppressed has recently been the subject of much research in the colloidal nanocrystal field. Here, we provide direct experimental evidence that so-called “giant” nanocrystals consisting of a small CdSe core and a thick CdS shell exhibit a significant (orders of magnitude) suppression of Auger decay rates. As a consequence, even multiexcitons of a very high order exhibit significant emission efficiencies, which allows us to demonstrate optical amplification with an extraordinarily la...

Suppressed auger recombination in "giant" nanocrystals boosts optical gain performance.

We apply low temperature confocal optical microscopy to spatially resolve, and spectroscopically study, a single self-assembled quantum dot. By comparing the emission spectra obtained at various excitation levels to a theoretical many body model, we show that (a) single exciton radiative recombination is very weak, and (b) sharp spectral lines are due to optical transitions between confined multiexcitonic states among which excitons thermalize within their lifetimes. Once these few states are fully occupied, broadbands appear due to transitions between states which contain electrons in the continuum.

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Multiexciton Spectroscopy of a Single Self-Assembled Quantum Dot

We apply diffraction-limited confocal optical microscopy to spatially resolve, a single self-assembled semiconductor quantum dot. We report for the first time, on the low-temperature photoluminescence spectrum of such a single dot and on its excitation intensity dependence. We demonstrate that sharp spectral lines, in the dots emission spectrum, are due to optical transitions between discrete multiexcitonic states confined within the dot. Under high excitation power, once the limited number of discrete exciton levels are fully occupied, spectrally broad emission bands are formed due to transitions which involve continuum excitonic states. In addition, we show that the single exciton recombination is almost forbidden in this InAs self-assembled quantum dot.

D. Spektor

Papers

Multiexciton Spectroscopy of a Single Self-Assembled Quantum Dot

Optical spectroscopy of a single self-assembled quantum dot