PPLN OPCPA based on spectrally addressed amplification

We propose and demonstrate the concept of OPCPA based on spectrally addressed amplification in a periodically poled Lithium niobate

Acoustic vibrations of metal nanoparticles: high order radial mode detection

no abstrac

Temperature dependence of acoustic vibrations of CdSe and CdSe–CdS core–shell nanocrystals measured by low-frequency Raman spectroscopy

We measure the temperature dependence of breathing-mode acoustic vibrations of semiconductor nanocrystals using low-frequency Raman spectroscopy. In CdSe core-only nanocrystals, the lowest-energy l = 0 mode red-shifts with increasing temperature by ∼5% between 77–300 K. Changes to the interatomic bond distances in the inorganic crystal lattice, with corresponding changes to the bulk modulus and density of the material, contribute to the observed energy shift but do not fully explain its magnitude across all nanocrystal sizes. Invariance of the Raman linewidth over the same temperature range suggests that the acoustic breathing mode is inhomogeneously broadened. The acoustic phonons of CdSe/CdS core–shell composite nanocrystals display similar qualitative behavior. However, for large core–shell nanocrystals, we observe a higher-order Raman peak at approximately twice the energy of the l = 0 mode, which we identify as a higher spherical harmonic—the n = 2, l = 0 eigenmode—rather than a two-phonon scattering event.Eni-MIT Solar Frontiers CenterEni S.p.A

Acousto-plasmonic Hot Spots in Metallic Nano-Objects

We investigate the acousto-plasmonic dynamics of metallic nano-objects by means of resonant Raman scattering and time-resolved femtosecond transient absorption. We observe an unexpectedly strong acoustic vibration band in the Raman scattering of silver nanocolumns, usually not found in isolated nano-objects. The frequency and the polarization of this unexpected Raman band allow us to assign it to breathing-like acoustic vibration modes. On the basis of full electromagnetic near-field calculations coupled to the elasticity theory, we introduce a new concept of “acousto-plasmonic hot spots” which arise here because of the indented shape of the nanocolumns. These hot spots combine both highly localized surface plasmons and strong shape deformation by the acoustic vibrations at specific sites of the nano-objects. We show that the coupling between breathing-like acoustic vibrations and surface plasmons at the “acousto-plasmonic hot spots” is strongly enhanced, turning almost silent vibration modes into efficient Raman scatterers

Anomalously Soft and Stiff Modes of Transition-Metal Nanoparticles

We propose an explanation for the enhanced low- and high-energy tails of the vibrational density of states (VDOS) of nanoparticles (NPs) with respect to their bulk counterparts. Density functional theory calculations of the frequency and eigenvector of each mode allow us to identify radial breathing/multipolar and nonradial tidal/shear/torsional vibrations as the modes that populate such tails. These modes have long been obtained from elasticity theory and are thus analogous to the widely studied and observed pulsations in variable stars. The features particular to the VDOS of NPs are rationalized in terms of the charge density distribution around low-coordinated atoms, the quasi-radial geometric distribution of NPs, force constant variations, degree of symmetry of the nanoparticle, discreteness of the spectrum, and the confinement of the eigenmodes. Our results indicate that the high- and low-energy tails of the VDOS may be a powerful tool to reveal information about the chemical composition and geometric structure of small NPs. In particular, the size of the confinement gap at the low-frequency end of the VDOS and the extent by which the high-frequency end surpasses the bulk limit signal whether a NP is bulk-like or non-bulk-like and the extent to which it is disordered. © 2014 American Chemical Society