[Show abstract][Hide abstract] ABSTRACT: Producing advanced quantum states of light is a priority in quantum
information technologies. While remarkable progress has been made on single
photons and photon pairs, multipartite correlated photon states are usually
produced in purely optical systems by post-selection or cascading, with
extremely low efficiency and exponentially poor scaling. Multipartite states
enable improved tests of the foundations of quantum mechanics as well as
implementations of complex quantum optical networks and protocols. It would be
favorable to directly generate these states using solid state systems, for
better scaling, simpler handling, and the promise of reversible transfer of
quantum information between stationary and flying qubits. Here we use the
ground states of two optically active coupled quantum dots to directly produce
photon triplets. The wavefunctions of photogenerated excitons localized in
these ground states are correlated via molecular hybridization and Coulomb
interactions. The formation of a triexciton leads to a triple cascade
recombination and sequential emission of three photons with strong
correlations. The quantum dot molecule is embedded in an epitaxially grown
nanowire engineered for single-mode waveguiding and improved extraction
efficiency at the emission wavelength. We record 65.62 photon triplets per
minute, surpassing rates of all earlier reported sources, in spite of the
moderate efficiency of our detectors. Our structure and data represent a
breakthrough towards implementing multipartite photon entanglement and
multi-qubit readout schemes in solid state devices, suitable for integrated
quantum information processing.
[Show abstract][Hide abstract] ABSTRACT: We use nominally spheroidal CdSe nanocrystals with a zincblende crystal structure to study how shape perturbations lift the energy degeneracies of the band-edge exciton. Nanocrystals with a low degree of symmetry exhibit splitting of both upper and lower bright-state degeneracies due to valence band mixing combined with the isotropic exchange interaction, allowing active control of the level splitting with a magnetic field. Asymmetry-induced splitting of the bright states is used to reveal the entire 8-state band-edge fine structure, enabling complete comparison with band-edge exciton models.
[Show abstract][Hide abstract] ABSTRACT: The band-edge exciton in elongated CdSe nanocrystals is composed of an upper and lower manifold associated with heavy and light holes in which the energy separation is sensitive to the nanocrystal shape. Using resonant photoluminescence excitation we probe the upper heavy hole exciton manifold and find rapid relaxation to the lower light hole manifold on a 5 ps timescale. State selective excitation allows preparation of single quantum states in this system. We used this to map the hole spin relaxation pathways between the fine structure sublevels which have energy splittings incommensurate with either optical or acoustic phonon energies. This reveals a hitherto unexpected hole spin-relaxation channel in these materials.
[Show abstract][Hide abstract] ABSTRACT: The direct coupling of excited electronic states to optical phonons in single CdSe colloidal quantum dots is explored using both photoluminescence emission and excitation spectroscopies. We find a broad optical phonon spectrum associated with a single fine structure state. Multiple peaks in the optical phonon sideband are ascribed to different optical phonon types emanating from both the core and shell layers. A mixed emission process that involves the simultaneous generation of two different types of optical phonon is also observed. In general, rather than a single mode, each designated phonon type is associated with a dispersed family of modes. Narrow optical phonon sidebands, consistent with the dominant LO mode, are observed in some nanocrystals. A linewidth analysis indicates that optical phonon lifetimes are in the 10 picosecond range. We demonstrate the ability to selectively excite a specific band-edge state by directly exciting its LO phonon sideband.
No preview · Article · Jul 2014 · Physical Chemistry Chemical Physics
[Show abstract][Hide abstract] ABSTRACT: Measurements of the emission linewidth of single nanocrystals are usually limited by spectral diffusion. At cryogenic temperatures, the origin of this instability was revealed to be photo-induced, suggesting that the spectral peak position may be stable in the limit of vanishing optical excitation. Here we test this stability using resonant photoluminescence excitation and find there is persistent spectral broadening, which ultimately limits the emission linewidth in these materials. The spectral broadening is shown to be consistent with spontaneous fluctuations of the local electrostatic field within the disordered environment surrounding the nanocrystal.
[Show abstract][Hide abstract] ABSTRACT: 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.
No preview · Article · Oct 2013 · Chemical Society Reviews
[Show abstract][Hide abstract] ABSTRACT: Charged quantum dots provide an important platform for a range of emerging quantum technologies from spin qubits to single phonon sources. Colloidal quantum dots in particular could offer unique advantages for such applications (eg. facile synthesis, manipulation and compatibility with a wide range of environments), especially if stable charged states can be harnessed in these materials. This possibility has been encouraged by recent reports of trion emission from colloidal quantum dots at cryogenic temperatures [1,2] indicating that trion states can be bright with quantum yields approaching unity . However, these reports relied on random ionization to produce the trion state and did not provide any insight into the charging mechanism.
[Show abstract][Hide abstract] ABSTRACT: Spectroscopically resolved emission from single nanocrystals at cryogenic temperatures provides unique insight into physical processes that occur within these materials. At low temperatures, the emission spectra collapse to narrow lines, revealing a rich spectroscopic landscape and unexpected properties, completely hidden at the ensemble level. Since these techniques were first used, the technology of nanocrystal synthesis has matured significantly, and new materials with outstanding photostability have been reported. In this perspective, we show how cryogenic spectroscopy of single nanocrystals probes the fundamental excitonic structure of the band edge, revealing spectral fingerprints that are highly sensitive to a range of photophysical properties as well as nanocrystal morphology. In particular, spectral and temporal signatures of biexciton and trion emission are revealed, and their relevance to emerging technologies is discussed. Overall we show how cryogenic single nanocrystal spectroscopy can be used as a tool for understanding fundamental photophysics and guiding the synthesis of new nanocrystal materials.
Full-text · Article · Feb 2013 · Journal of Physical Chemistry Letters