Improving single-photon sources with Stark tuning

We investigate the use of the Stark shift in atomlike systems in order to control the interaction with a high-Q/V microcavity. By applying a Stark shift pulse to a single atomlike system, in order to affect and control its detuning from a cavity resonance, the cavity QED interaction can be carefully controlled so as to allow stochastic pumping of the emitting state without causing random timing jitter in the output photon. Using a quantum trajectory approach, we conduct simulations that show this technique is capable of producing indistinguishable single photons that exhibit complete Hong-Ou-Mandel interference. Furthermore, Stark tuning control allows for the generation of arbitrary pulse envelopes. We demonstrate this by showing that a simple asymmetric Stark shifting pulse can lead to the emission of symmetric Gaussian single-photon pulse envelopes, rather than the usual exponential decay. These Gaussian pulses also exhibit complete Hong-Ou-Mandel interference. The use of Stark shifting in solid-state systems could ultimately provide the cheap miniature high quality single-photon sources that are currently required for applications such as all-optical quantum computing

Anomalous power laws of spectral diffusion in quantum dots: A connection to luminescence intermittency

We show that the wandering of transition frequencies in colloidal quantum dots does not follow the statistics expected for ordinary diffusive processes. The trajectory of this anomalous spectral diffusion is characterized by a root t dependence of the squared deviation. The behavior is reproduced when the electronic states of quantum dots are assumed to interact with environments such as, for example, an ensemble of two-level systems, where the correlation times are distributed according to a power law similar to the one generally attributed to the dot's luminescence intermittency

Sensitive detection of sodium in a flame using parametric four-wave mixing and seeded parametric four-wave mixing

Two-photon resonant parametric four-wave mixing and a newly developed variant called seeded parametric four-wave mixing are used to detect trace quantities of sodium in a flame. Both techniques are simple, requiring only a single laser to generate a signal beam at a different wavelength which propagates collinearly with the pump beam, allowing efficient signal recovery. A comparison of the two techniques reveals that seeded parametric four-wave mixing is more than two orders of magnitude more sensitive than parametric four-wave mixing, with an estimated detection sensitivity of 5 x 10(9) atoms/cm(3). Seeded parametric four-wave mixing is achieved by cascading two parametric four-wave mixing media such that one of the parametric fields generated in the first high-density medium is then used to seed the same four-wave mixing process in a second medium in order to increase the four-wave mixing gain. The behavior of this seeded parametric four-wave mixing is described using semiclassical perturbation theory. A simplified small-signal theory is found to model most of the data satisfactorily. However, an anomalous saturationlike behavior is observed in the large signal regime. The full perturbation treatment, which includes the competition between two different four-wave mixing processes coupled via the signal field, accounts for this apparently anomalous behavior

Infrared seeded parametric four-wave mixing for sensitive detection of molecules

We have developed a sensitive resonant four-wave mixing technique based on two-photon parametric four-wave mixing with the addition of a phase matched ''seeder'' field. Generation of the seeder field via the same four-wave mixing process in a high pressure cell enables automatic phase matching to be achieved in a low pressure sample cell. This arrangement facilitates sensitive detection of complex molecular spectra by simply tuning the pump laser. We demonstrate the technique with the detection of nitric oxide down to concentrations more than 4 orders of magnitude below the capability of parametric four-wave mixing alone, with an estimated detection threshold of 10(12) molecules/cm(3)

Spectroscopy of single nanocrystals

As colloidal semiconductor nanocrystals are developed for a wider range of diverse applications, it becomes more important to gain a deeper understanding of their properties in order to direct synthetic efforts. While most synthetic developments are guided by changes in ensemble properties, certain applications such as those in nano-electronics and nano-photonics rely on properties of nanocrystals at the individual level. For such applications and even for a more detailed understanding of the ensemble behavior, single nanocrystal spectroscopy becomes a vital tool. This review looks at how single nanocrystal spectroscopy has been applied to materials based on modern synthetic techniques and how these studies are elucidating properties that remain hidden at the ensemble level. First, recent theoretical models that are important for understanding many observed phenomena are explored. Then the review highlights new insights into many of the photophysical properties that are of interest in semiconductor nanocrystal materials, such as the ubiquitous spectral instability, magneto-optical identification of the band-edge exciton fine structure, emission from multi-excitons, and the spectroscopic properties of charged nanocrystals that challenge long standing theories on photoluminescence blinking behavior. To date most of the research has been conducted on materials based on cadmium selenide primarily due to its many years of development as a prototypical nanocrystal system. The review ends with a discussion of new materials that would also benefit from a detailed photophysical understanding afforded by single nanocrystal spectroscopy

Comment on "Spin-Flip Limited Exciton Dephasing in CdSe/ZnS Colloidal Quantum Dots"

A Comment on the Letter by F. Masia, et al., Phys. Rev. Lett. 108 087401 (2012). The authors of the Letter offer a Reply

Detection of bright trion states using the fine structure emission of single CdSe/ZnS colloidal quantum dots

We report direct observation of the lowest two states of the band-edge exciton fine structure in the photoluminescence from single CdSe/ZnS core/shell nanocrystals at cryogenic temperatures. The temperature dependence of this spectral fingerprint reveals exciton spin relaxation rates as low as 10 mu s(-1). The fine structure is also dependent on the nanocrystal charge state facilitating the identification of a bright negatively charged trion state with a quantum yield comparable to that of neutral emission

Magneto-optical spectroscopy of individual semiconductor nanocrystals

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