Non-Fourier heat transport in metal-dielectric core-shell nanoparticles under ultrafast laser pulse excitation

Relaxation dynamics of embedded metal nanoparticles after ultrafast laser pulse excitation is driven by thermal phenomena of different origins the accurate description of which is crucial for interpreting experimental results: hot electron gas generation, electron-phonon coupling, heat transfer to the particle environment and heat propagation in the latter. Regardingthis last mechanism, it is well known that heat transport in nanoscale structures and/or at ultrashort timescales may deviate from the predictions of the Fourier law. In these cases heat transport may rather be described by the Boltzmann transport equation. We present a numerical model allowing us to determine the electron and lattice temperature dynamics in a spherical gold nanoparticle core under subpicosecond pulsed excitation, as well as that of the surrounding shell dielectric medium. For this, we have used the electron-phonon coupling equation in the particle with a source term linked with the laser pulse absorption, and the ballistic-diffusive equations for heat conduction in the host medium. Either thermalizing or adiabatic boundary conditions have been considered at the shell external surface. Our results show that the heat transfer rate from the particle to the matrix can be significantly smaller than the prediction of Fourier's law. Consequently, the particle temperature rise is larger and its cooling dynamics might be slower than that obtained by using Fourier's law. This difference is attributed to the nonlocal and nonequilibrium heat conduction in the vicinity of the core nanoparticle. These results are expected to be of great importance for analyzing pump-probe experiments performed on single nanoparticles or nanocomposite media

'Spillout' effect in gold nanoclusters embedded in c-Al2O3(0001) matrix

Gold nanoclusters are grown by 1.8 MeV Au^\sup{2+} implantation on c-Al\sub{2}O\sub{3}(0001)substrate and subsequent air annealing at temperatures 1273K. Post-annealed samples show plasmon resonance in the optical (561-579 nm) region for average cluster sizes ~1.72-2.4 nm. A redshift of the plasmon peak with decreasing cluster size in the post-annealed samples is assigned to the 'spillout' effect (reduction of electron density) for clusters with ~157-427 number of Au atoms fully embedded in crystalline dielectric matrix with increased polarizability in the embedded system.Comment: 14 Pages (figures included); Accepted in Chem. Phys. Lett (In Press

Resonant Raman Scattering by quadrupolar vibrations of Ni-Ag Core-shell Nanoparticles

Low-frequency Raman scattering experiments have been performed on thin films consisting of nickel-silver composite nanoparticles embedded in alumina matrix. It is observed that the Raman scattering by the quadrupolar modes, strongly enhanced when the light excitation is resonant with the surface dipolar excitation, is mainly governed by the silver electron contribution to the plasmon excitation. The Raman results are in agreement with a core-shell structure of the nanoparticles, the silver shell being loosely bonded to the nickel core.Comment: 3 figures. To be published in Phys. Rev.

Wetting to Non-wetting Transition in Sodium-Coated C_60

Based on ab initi and density-functional theory calculations, an empirical potential is proposed to model the interaction between a fullerene molecule and many sodium atoms. This model predicts homogeneous coverage of C_60 below 8 Na atoms, and a progressive droplet formation above this size. The effects of ionization, temperature, and external electric field indicate that the various, and apparently contradictory, experimental results can indeed be put into agreement.Comment: 4 pages, 4 postscript figure

Origin of Shifts in the Surface Plasmon Resonance Frequencies for Au and Ag Nanoparticles

Origin of shifts in the surface plasmon resonance (SPR) frequency for noble metal (Au, Ag) nanoclusters are discussed in this book chapter. Spill out of electron from the Fermi surface is considered as the origin of red shift. On the other hand, both screening of electrons of the noble metal in porous media and quantum effect of screen surface electron are considered for the observed blue shift in the SPR peak position.Comment: 37 pages, 14 Figures in the submitted book chapter of The Annual Reviews in Plasmonics, edited by Professor Chris D. Geddes. Springer Scinec

Continuum limit of amorphous elastic bodies: A finite-size study of low frequency harmonic vibrations

The approach of the elastic continuum limit in small amorphous bodies formed by weakly polydisperse Lennard-Jones beads is investigated in a systematic finite-size study. We show that classical continuum elasticity breaks down when the wavelength of the sollicitation is smaller than a characteristic length of approximately 30 molecular sizes. Due to this surprisingly large effect ensembles containing up to N=40,000 particles have been required in two dimensions to yield a convincing match with the classical continuum predictions for the eigenfrequency spectrum of disk-shaped aggregates and periodic bulk systems. The existence of an effective length scale \xi is confirmed by the analysis of the (non-gaussian) noisy part of the low frequency vibrational eigenmodes. Moreover, we relate it to the {\em non-affine} part of the displacement fields under imposed elongation and shear. Similar correlations (vortices) are indeed observed on distances up to \xi~30 particle sizes.Comment: 28 pages, 13 figures, 3 table

Nucleation of a sodium droplet on C60

We investigate theoretically the progressive coating of C60 by several sodium atoms. Density functional calculations using a nonlocal functional are performed for NaC60 and Na2C60 in various configurations. These data are used to construct an empirical atomistic model in order to treat larger sizes in a statistical and dynamical context. Fluctuating charges are incorporated to account for charge transfer between sodium and carbon atoms. By performing systematic global optimization in the size range 1<=n<=30, we find that Na_nC60 is homogeneously coated at small sizes, and that a growing droplet is formed above n=>8. The separate effects of single ionization and thermalization are also considered, as well as the changes due to a strong external electric field. The present results are discussed in the light of various experimental data.Comment: 17 pages, 10 figure

Density functional study of Aun_n (n=2-20) clusters: lowest-energy structures and electronic properties

We have investigated the lowest-energy structures and electronic properties of the Au$_n$(n=2-20) clusters based on density functional theory (DFT) with local density approximation. The small Au$_n$ clusters adopt planar structures up to n=6. Tabular cage structures are preferred in the range of n=10-14 and a structural transition from tabular cage-like structure to compact near-spherical structure is found around n=15. The most stable configurations obtained for Au$_{13}$ and Au$_{19}$ clusters are amorphous instead of icosahedral or fcc-like, while the electronic density of states sensitively depend on the cluster geometry. Dramatic odd-even alternative behaviors are obtained in the relative stability, HOMO-LUMO gaps and ionization potentials of gold clusters. The size evolution of electronic properties is discussed and the theoretical ionization potentials of Au$_n$ clusters compare well with experiments.Comment: 6 pages, 7 figure

Stromal Vascular Fraction Transplantation as an Alternative Therapy for Ischemic Heart Failure: Anti-inflammatory Role

<p>Abstract</p> <p>Background</p> <p>The aims of this study were: (1) to show the feasibility of using adipose-derived stromal vascular fraction (SVF) as an alternative to bone marrow mono nuclear cell (BM-MNC) for cell transplantation into chronic ischemic myocardium; and (2) to explore underlying mechanisms with focus on anti-inflammation role of engrafted SVF and BM-MNC post chronic myocardial infarction (MI) against left ventricular (LV) remodelling and cardiac dysfunction.</p> <p>Methods</p> <p>Four weeks after left anterior descending coronary artery ligation, 32 Male Lewis rats with moderate MI were divided into 3 groups. SVF group (n = 12) had SVF cell transplantation (6 × 10⁶cells). BM-MNC group (n = 12) received BM-MNCs (6 × 10⁶) and the control (n = 10) had culture medium. At 4 weeks, after the final echocardiography, histological sections were stained with Styrus red and immunohistochemical staining was performed for α-smooth muscle actin, von Willebrand factor, CD3, CD8 and CD20.</p> <p>Results</p> <p>At 4 weeks, in SVF and BM-MNC groups, LV diastolic dimension and LV systolic dimension were smaller and fractional shortening was increased in echocardiography, compared to control group. Histology revealed highest vascular density, CD3+ and CD20+ cells in SVF transplanted group. SVF transplantation decreased myocardial mRNA expression of inflammatory cytokines TNF-α, IL-6, MMP-1, TIMP-1 and inhibited collagen deposition.</p> <p>Conclusions</p> <p>Transplantation of adipose derived SVF cells might be a useful therapeutic option for angiogenesis in chronic ischemic heart disease. Anti-inflammation role for SVF and BM transplantation might partly benefit for the cardioprotective effect for chronic ischemic myocardium.</p