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Register a new userPhotothermal Absorption Spectroscopy of Individual Semiconductor Nanocrystals
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Authors
Stephane Berciaud
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Photothermal heterodyne detection is used to record the first room-temperature absorption spectra of single CdSe/ZnS semiconductor nanocrystals. These spectra are recorded in the high cw excitation regime, and the observed bands are assigned to transitions involving biexciton and trion states. Comparison with the single nanocrystals photoluminescence spectra leads to the measurement of spectral Stokes shifts free from ensemble averaging.
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We introduce a new, highly sensitive, and simple heterodyne optical method for imaging individual nonfluorescent nanoclusters and nanocrystals. A 2 order of magnitude improvement of the signal is achieved compared to previous methods. This allows for the unprecedented detection of individual small absorptive objects such as metallic clusters (of 67 atoms) or nonluminescent semiconductor nanocrystals. The measured signals are in agreement with a calculation based on the scattering field theory from a photothermal-induced modulated index of refraction profile around the nanoparticle.
Current methods for producing single-walled carbon nanotubes (SWNTs) lead to heterogeneous samples containing mixtures of metallic and semiconducting species with a variety of lengths and defects. Optical detection at the single nanotube level should thus offer the possibility to examine these heterogeneities provided that both SWNT species are equally well detected. Here, we used photothermal heterodyne detection to record absorption images and spectra of individual SWNTs. Because this photothermal method relies only on light absorption, it readily detects metallic nanotubes as well as the emissive semiconducting species. The first and second optical transitions in individual semicontucting nanotubes have been probed. Comparison between the emission and absorption spectra of the lowest-lying optical transition reveal mainly small Stokes shifts. Side bands in the near-infrared absorption spectra are observed and assigned to exciton-phonon bound states. No such sidebands are detected around the lowest transition of metallic nanotubes.
Energy transfer from photoexcited zero-dimensional systems to metallic systems plays a prominent role in modern day materials science. A situation of particular interest concerns the interaction between a photoexcited dipole and an atomically thin metal. The recent discovery of graphene layers permits investigation of this phenomenon. Here we report a study of fluorescence from individual CdSe/ZnS nanocrystals in contact with single- and few-layer graphene sheets. The rate of energy transfer is determined from the strong quenching of the nanocrystal fluorescence. For single-layer graphene, we find a rate of ~ 4ns-1, in agreement with a model based on the dipole approximation and a tight-binding description of graphene. This rate increases significantly with the number of graphene layers, before approaching the bulk limit. Our study quantifies energy transfer to and fluorescence quenching by graphene, critical properties for novel applications in photovoltaic devices and as a molecular ruler.
Single-nanotube photometry was used to measure the product of absorption cross-section and fluorescence quantum yield for 12 (n,m) structural species of semiconducting SWNTs in aqueous SDBS suspension. These products ranged from 1.7 to 4.5 x 10(-19) cm2/C atom, generally increasing with optical band gap as described by the energy gap law. The findings suggest fluorescent quantum yields of ~8% for the brightest, (10,2) species and introduce the empirical calibration factors needed to deduce quantitative (n,m) distributions from bulk fluorimetric intensities.
We introduce a new, highly sensitive, and simple heterodyne optical method for imaging individual non-fluorescent nano-objects. A two orders of magnitude improvement of the signal is achieved compared to previous methods. This allows for the unprecedented detection of individual small absorptive objects such as metallic clusters (of 67 atoms) or non-luminescent semiconductor nanocrystals. The measured signals are in agreement with a calculation based on the scattering field theory from a photothermal-induced modulated index of refraction profile around the nanoparticle.
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