ABSTRACT
Silicon nanocrystals were synthesized by CO(2) laser pyrolysis of SiH(4). The fresh silicon nanopowder was oxidized in water to obtain SiO(2) nanoparticles (NPs) exhibiting strong red-orange photoluminescence. Samples of SiO(2) NPs embedded in low concentration in a thin polymer layer were prepared by spin-coating a dedicated solution on quartz cover slides. Using an argon ion laser at 488 nm with higher-order laser modes (azimuthally and radially polarized doughnut modes) for excitation, the three-dimensional orientation of the nanoparticles' transition dipole moment was investigated in a confocal microscope. The linear transition dipole moment was found to be rather stable and randomly oriented. However, dynamical effects such as fluorescence intermittency and transition dipole moment flipping could also be observed. The spectral analysis of single SiO(2) NPs revealed double-peak spectra consisting of a narrow zero-phonon line and a broader phonon band being associated with the excitation of longitudinal optical phonons in the SiO(2) NP.
Subject(s)
Luminescence , Nanostructures/chemistry , Silicon Dioxide/chemistry , Argon/chemistry , Electrons , Lasers , Materials Testing , Microscopy, Confocal , Nanotechnology , Particle Size , Surface PropertiesABSTRACT
We studied spatially isolated single-walled carbon nanotubes (SWNTs) immobilized in a quasi-planar optical lambda/2-microresonator using confocal microscopy and spectroscopy. The modified photonic mode density within the resonator is used to selectively enhance or inhibit different Raman transitions of SWNTs. Experimental spectra are presented that exhibit single Raman bands only. Calculations of the relative change in the Raman scattering cross sections underline the potential of our microresonator for the optical control of nonequilibrium phonon populations in SWNT.
Subject(s)
Crystallization/methods , Models, Chemical , Nanotechnology/methods , Nanotubes, Carbon/chemistry , Nanotubes, Carbon/ultrastructure , Spectrum Analysis, Raman/methods , Acoustics , Computer Simulation , Macromolecular Substances/chemistry , Materials Testing , Molecular Conformation , Particle Size , Surface Properties , VibrationABSTRACT
We present for the first time cavity-controlled fluorescence spectra and decay curves of single dipole emitters interacting at room temperature with the first longitudinal mode of a Fabry-Perot microcavity offering a lambda/2-spacing between its silver mirrors. The spontaneous emission rate of individual dye molecules was found to be enhanced by the Purcell effect by up to three times compared to the rate in free space, in agreement with theoretical predictions. Moreover, our new microcavity design was found to provide long-term stability and single-molecule sensitivity under ambient conditions for several months without noticeable reduction of the cavity-Q value. We consider this as a significant advance for single-photon sources operating at room temperature.
