Optical spectroscopy of single quantum dots at tunable positive, neutral, and negative charge states

We report on the observation of photoluminescence from positive, neutral, and negative charge states of single semiconductor quantum dots. For this purpose we designed a structure enabling optical injection of a controlled unequal number of negative electrons and positive holes into an isolated InGaAs quantum dot embedded in a GaAs matrix. Thereby, we optically produced the charge states -3, -2, -1, 0, +1, and +2. The injected carriers form confined collective “artificial atoms and molecules” states in the quantum dot. We resolve spectrally and temporally the photoluminescence from an optically excited quantum dot and use it to identify collective states, which contain charge of one type, coupled to few charges of the other type. These states can be viewed as the artificial analog of charged atoms such as ${\mathrm{H}}^{-},$ ${\mathrm{H}}^{-2},$ ${\mathrm{H}}^{-3},$ and charged molecules such as ${\mathrm{H}}_2^{+}$ and ${\mathrm{H}}_3^{+2\mathrm{}}.$ Unlike higher dimensionality systems, where negative or positive charging always results in reduction of the emission energy due to electron-hole pair recombination, in our dots, negative charging reduces the emission energy, relative to the charge-neutral case, while positive charging increases it. Pseudopotential model calculations reveal that the enhanced spatial localization of the hole wave function, relative to that of the electron in these dots, is the reason for this effect.