Subnanosecond spectral diffusion measurement using photon correlation

Spectral diffusion is a result of random spectral jumps of a narrow line as a result of a fluctuating environment. It is an important issue in spectroscopy, because the observed spectral broadening prevents access to the intrinsic line properties. However, its characteristic parameters provide local information on the environment of a light emitter embedded in a solid matrix, or moving within a fluid, leading to numerous applications in physics and biology. We present a new experimental technique for measuring spectral diffusion based on photon correlations within a spectral line. Autocorrelation on half of the line and cross-correlation between the two halves give a quantitative value of the spectral diffusion time, with a resolution only limited by the correlation set-up. We have measured spectral diffusion of the photoluminescence of a single light emitter with a time resolution of 90 ps, exceeding by four orders of magnitude the best resolution reported to date

Interface optical phonons in spheroidal dots: Raman selection rules

The contribution of interface phonons to the first order Raman scattering in nanocrystals with non spherical geometry is analyzed. Interface optical phonons in the spheroidal geometry are discussed and the corresponding Frohlich-like electron-phonon interaction is reported in the framework of the dielectric continuum approach. It is shown that the interface phonon modes are strongly dependent on the nanocrystal geometry, particularly on the ellipsoid's semi-axis ratio. The new Raman selection rules have revealed that solely interface phonon modes with even angular momentum are allowed to contribute to the first order phonon-assisted scattering of light. On this basis we are able to give an explanation for the observed low frequency shoulders present in the Raman cross-section of several II-VI semiconductor nanostructures.Comment: 8 pages, 2 figure

Absence of correlation between built-in electric dipole moment and quantum Stark effect in InAs/GaAs self-assembled quantum dots

We report significant deviations from the usual quadratic dependence of the ground state interband transition energy on applied electric fields in InAs/GaAs self-assembled quantum dots. In particular, we show that conventional second-order perturbation theory fails to correctly describe the Stark shift for electric field below $F = 10$ kV/cm in high dots. Eight-band ${\bf k}\cdot{\bf p}$ calculations demonstrate this effect is predominantly due to the three-dimensional strain field distribution which for various dot shapes and stoichiometric compositions drastically affects the hole ground state. Our conclusions are supported by two independent experiments.Comment: 4 pages, 4 figure

A pseudopotential study of electron-hole excitations in colloidal, free-standing InAs quantum dots

Excitonic spectra are calculated for free-standing, surface passivated InAs quantum dots using atomic pseudopotentials for the single-particle states and screened Coulomb interactions for the two-body terms. We present an analysis of the single particle states involved in each excitation in terms of their angular momenta and Bloch-wave parentage. We find that (i) in agreement with other pseudopotential studies of CdSe and InP quantum dots, but in contrast to k.p calculations, dot states wavefunction exhibit strong odd-even angular momentum envelope function mixing (e.g. $s$ with $p$) and large valence-conduction coupling. (ii) While the pseudopotential approach produced very good agreement with experiment for free-standing, colloidal CdSe and InP dots, and for self-assembled (GaAs-embedded) InAs dots, here the predicted spectrum does {\em not} agree well with the measured (ensemble average over dot sizes) spectra. (1) Our calculated excitonic gap is larger than the PL measure one, and (2) while the spacing between the lowest excitons is reproduced, the spacings between higher excitons is not fit well. Discrepancy (1) could result from surface states emission. As for (2), agreement is improved when account is taken of the finite size distribution in the experimental data. (iii) We find that the single particle gap scales as $R^{-1.01}$ (not $R^{-2}$), that the screened (unscreened) electron-hole Coulomb interaction scales as $R^{-1.79}$ ($R^{-0.7}$), and that the eccitonic gap sclaes as $R^{-0.9}$. These scaling laws are different from those expected from simple models.Comment: 12 postscript figure

Electric field and exciton structure in CdSe nanocrystals

Quantum Stark effect in semiconductor nanocrystals is theoretically investigated, using the effective mass formalism within a $4\times 4$ Baldereschi-Lipari Hamiltonian model for the hole states. General expressions are reported for the hole eigenfunctions at zero electric field. Electron and hole single particle energies as functions of the electric field ($\mathbf{E}_{QD}$) are reported. Stark shift and binding energy of the excitonic levels are obtained by full diagonalization of the correlated electron-hole Hamiltonian in presence of the external field. Particularly, the structure of the lower excitonic states and their symmetry properties in CdSe nanocrystals are studied. It is found that the dependence of the exciton binding energy upon the applied field is strongly reduced for small quantum dot radius. Optical selection rules for absorption and luminescence are obtained. The electric-field induced quenching of the optical spectra as a function of $\mathbf{E}_{QD}$ is studied in terms of the exciton dipole matrix element. It is predicted that photoluminescence spectra present anomalous field dependence of the emission lines. These results agree in magnitude with experimental observation and with the main features of photoluminescence experiments in nanostructures.Comment: 9 pages, 7 figures, 1 tabl

Time-dependent single molecule spectral lines

A general conceptual problem of time-dependent single molecule spectra is discussed theoretically in the framework of recently developed intensity-time-frequency correlation spectroscopy. It is shown that the new method is closely related to a "gedanken" three-pulse photon echo experiment done on an ensemble of identical molecules interacting with statistically identical microscopic environments. The correlation function is an integral transform (under certain conditions a Fourier transform) of the echo amplitude as a function of the delay between the first and the second pulses. [S0163-1829(99)10907-X]

Ensemble interactions in strained semiconductor quantum dots

Large variations in InxGa1-xAs quantum dot concentrations were obtained with simultaneous growths on vicinal GaAs [001] substrates with different surface step densities. It was found that decreasing dot-dot separation blueshifts all levels, narrows intersublevel transition energies, shortens luminescence decay times for excited states, and increases inhomogeneous photoluminescence broadening. These changes in optical properties are attributed to a progressive strain deformation of the confining potentials and to the increasing effects of positional disorder in denser dot ensembles

Dynamics of Multiple Trafficking Behaviors of Individual Synaptic Vesicles Revealed by Quantum-Dot Based Presynaptic Probe

Although quantum dots (QDs) have provided invaluable information regarding the diffusive behaviors of postsynaptic receptors, their application in presynaptic terminals has been rather limited. In addition, the diffraction-limited nature of the presynaptic bouton has hampered detailed analyses of the behaviors of synaptic vesicles (SVs) at synapses. Here, we created a quantum-dot based presynaptic probe and characterized the dynamic behaviors of individual SVs. As previously reported, the SVs exhibited multiple exchanges between neighboring boutons. Actin disruption induced a dramatic decrease in the diffusive behaviors of SVs at synapses while microtubule disruption only reduced extrasynaptic mobility. Glycine-induced synaptic potentiation produced significant increases in synaptic and inter-boutonal trafficking of SVs, which were NMDA receptor- and actin-dependent while NMDA-induced synaptic depression decreased the mobility of the SVs at synapses. Together, our results show that sPH-AP-QD revealed previously unobserved trafficking properties of SVs around synapses, and the dynamic modulation of SV mobility could regulate presynaptic efficacy during synaptic activity