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Register a new userDeterminant role of size-dependent electron relaxation processes in the nonlinear luminescence emission of resonantly excited gold nanorods
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The two-photon luminescence (TPL) of gold nanoparticles (NP) was shown to result from the excitation of hot carriers, the plasmonic NP resonances playing an important role both for plasmon enhanced absorption and plasmon enhanced emission. However, the exact parameters enabling to control or optimize the NP nonlinear luminescence still need to be understood in detail. In this paper, we report the two-photon excited photoluminescence of single gold nanorods exhibiting identical aspect ratio (close to 4) and thus identical plasmonic resonances, but increasing volumes V (707 <V< 160 103 nm3 i.e. rod diameters varying between 6 and 40 nm). The two-photon luminescence intensity of a high number of colloidal nanorods was investigated at the single object level, combining polarization resolved TPL and simultaneously acquired topography. Non-monotonic TPL variations are evidenced, nanorods with an intermediate size (diameter around 10 nanometers) exhibiting the highest TPL signal intensity. A model is proposed considering both the local field enhancement effects at the NP and the size-dependent electron thermalization processes. BEM (Boundary Elements Method) simulations are used to compute the fields at both the transverse and longitudinal plasmon resonance. A good fitting of the experimental data is obtained considering integration of the fields over the whole the NP volume.
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The two-photon luminescence (TPL) of small 10 nm x 40 nm colloidal gold nanorods (GNR) is investigated at the single object level, combining polarization resolved TPL and simultaneously acquired topography. A very high dependence of the TPL signal with both the nanorods longitudinal axis and the incident wavelength is observed confirming the plasmonic origin of the signal and pointing the limit of the analogy between GNRs and molecules. The spectral analysis of the TPL evidences two emission bands peaks: in the visible (in direct connection with the gold band structure), and in the infrared. Both bands are observed to vary quadradically with the incident excitation beam but exhibit different polarization properties. The maximum two-photon brightness of a single GNR is measured to be a few millions higher than the two-photon brightness of fluorescein molecules. We show that the important TPL observed in these small gold nanorods results from resonance effects both at the excitation and emission level : local field enhancement at the longitudinal surface plasmon resonances (LSPR) first results in an increase of the electron-hole generation. Further relaxation of electron-hole pairs then mostly leads to the excitation of the GNR transverse plasmon mode and its subsequent radiative relaxation.
We describe how complex fluctuations of the local environment of an optically active quantum dot can leave rich fingerprints in its emission spectrum. A new feature, termed Fluctuation Induced Luminescence (FIL), is observed to arise from extremely rare fluctuation events that have a dramatic impact on the response of the system-so called black swan events. A quantum dissipative master equation formalism is developed to describe this effect phenomenologically. Experiments performed on single quantum dots subject to electrical noise show excellent agreement with our theory, producing the characteristic FIL sidebands.
X-band electron spin resonance (ESR) spectroscopy has been performed for gold nanorods (AuNRs) of four different sizes covered with a diamagnetic stabilizing component, cetyltrimethylammmonium bromide. The ESR spectra show ferromagnetic features such as hysteresis and resonance field shift, depending on the size of the AuNRs. In addition, the ferromagnetic transition is indicated by an abrupt change in the spectra of the two smallest AuNRs studied. A large g-value in the paramagnetic region suggests that the ferromagnetism in the AuNRs originates from strong spin-orbit interaction.
Theory of the electron spin relaxation in graphene on the SiO$_2$ substrate is developed. Charged impurities and polar optical surface phonons in the substrate induce an effective random Bychkov-Rashba-like spin-orbit coupling field which leads to spin relaxation by the Dyakonov-Perel mechanism. Analytical estimates and Monte Carlo simulations show that the corresponding spin relaxation times are between micro- to milliseconds, being only weakly temperature dependent. It is also argued that the presence of adatoms on graphene can lead to spin lifetimes shorter than nanoseconds.
The vibrations of gold nanowires and nanorods are investigated numerically in the framework of continuum elasticity using the Rayleigh-Ritz variational method. Special attention is paid to identify the vibrations relevant in Raman scattering experiments. A comprehensive description of the vibrations of nanorods is proposed by determining their symmetry, comparing with standing waves in the corresponding nanowires and estimating their Raman intensity. The role of experimentally relevant parameters such as the anisotropic cubic lattice structure, the presence of faceted lateral surfaces and the shape of the ends of the nanorods is evaluated. Elastic anisotropy is shown to play a significant role contrarily to the presence of facets. Localized vibrations are found for nanorods with flat ends. Their evolution as the shape of the ends is changed to half-spheres is discussed.
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