Time-resolved optical studies, heat dissipation and melting of Ag and Au nanoparticle systems and arrays

Transient absorption spectroscopy has been extensively used in recent years to examine the temporal response of isolated nanoparticles (NPs) to the absorption of light [1]. These studies are largely based on the use of the surface plasmon resonance (SPR) to monitor characteristics of the NP such as electronic and lattice temperature, shape and morphology as a function of time. In the case of extended Au/Ag NP structures the plasmon resonance is strongly distorted due to the inter-particle coupling effects. For example, we have observed this effect in Rhodamine dye functionalized Au nanoparticles which undergo self-assembly to form nanostructures due to the interactions between the dye molecules attached to the surfaces of the nanoparticles. Indeed the SPR splits into two with one resonance remaining in the vicinity of that of the isolated AuNPs and is generally called the transverse SPR while a second resonance due to an extended excitation spanning across multiple particles appears to the lower energies. The precise spectral energy and shape of the extended plasmon resonance depends on the inter-particle distance, the particle disposition and the number of particles involved. When the plasmon band or interband spectral region of the NP is excited by an intense pulse the photon energy absorbed by the electrons is transferred to the lattice of the NP as heat through electron-phonon coupling. Depending on the intensity of the light pulse and thus the initial electron temperature a number of outcomes are possible. The first aim of this work is to use low intensity pump pulses to study the wavelength dependence of the sub 10 ps dynamics which reflects the electron-photon scattering within the nanoparticle structure. On the other hand, the interaction of more intense light with the NPs can modify the morphology of NP systems, for example by reshaping gold nanorods into nanospheres or, in general, mediate the synthesis of metallic nanostructures. At medium intensities the initial temperature is sufficient to induce melting of the NPs which can lead to morphological changes of the NP structure. Higher intensities can cause other effects such as photofragmentation of the NPs, release of stabiliser molecules from the surface of the NPs or even Coulomb explosion due to multiple ionisation events. The second aim of this work is to concentrate on the effects of medium intensity laser excitation of a self-assembled Au/Ag NP systems. The NP system is excited by a femtosecond laser pulse of different wavelengths allowing selective deposition of energy and the subsequent heat dissipation through phonon-phonon coupling and morphological changes are monitored in time by recording transient absorption spectra in the visible range. This wavelength range makes it possible to follow the phonon-phonon coupling effects on the recovery of the bleaching of both the transverse and extended plasmon resonances of the NP system. As the intensity of the pump pulse is increased it can be seen that the NPs are no longer able to dissipate all of the heat before arrival of subsequent laser pulses thus leading to melting of the NP structure and strong changes in the plasmon response of the system. The overall aim of this study is to fully understand the delocalized electron-phonon coupling in the extended plasmon region of the NP structures and to use this knowledge to control the melting in nanostructures. The methods developed can be useful for plasmon mediated nano-engineerin

Interplay of the volume and surface plasmons in the electron energy loss spectra of C60_{60}

The results of a joint experimental and theoretical investigation of the C60 collective excitations in the process of inelastic scattering of electrons are presented. The shape of the electron energy loss spectrum is observed to vary when the scattering angle increases. This variation arising due to the electron diffraction of the fullerene shell is described by a new theoretical model which treats the fullerene as a spherical shell of a finite width and accounts for the two modes of the surface plasmon and for the volume plasmon as well. It is shown that at small angles, the inelastic scattering cross section is determined mostly by the symmetric mode of the surface plasmon, while at larger angles, the contributions of the antisymmetric surface plasmon and the volume plasmon become prominent.Comment: 11 pages, 3 figure

An experimental and theoretical study of the resonant Auger spectrum of the ethene molecule

Resonant Auger spectra of the ethene molecule excited at energies across the C1s → π* energy band are reported. Our measurements address the unexpected variation of the intensity of the A state with respect to the other singly ionized valence states. An approach, based on group theory and calculations using Coulomb 4-center integrals, is proposed to explain the behaviour of the intensity of the ground state and excited states of the ion upon resonant excitation. The new method provides a calculationally inexpensive route to predict relative intensities of different resonant Auger bands in polyatomic molecules, without the need for an exhaustive knowledge of the potential energy surfaces of the electronic states involved

Burden of multimorbidity in relation to age, gender and immigrant status: A cross-sectional study based on administrative data

Objectives Many studies have investigated multimorbidity, whose prevalence varies according to settings and data sources. However, few studies on this topic have been conducted in Italy, a country with universal healthcare and one of the most aged populations in the world. The aim of this study was to estimate the prevalence of multimorbidity in a Northern Italian region, to investigate its distribution by age, gender and citizenship and to analyse the correlations of diseases. Design Cross-sectional study based on administrative data. Setting Emilia-Romagna, an Italian region with-1/44.4 million inhabitants, of which almost one-fourth are aged 6565 years. Participants All adults residing in Emilia-Romagna on 31 December 2012. Hospitalisations, drug prescriptions and contacts with community mental health services from 2003 to 2012 were traced to identify the presence of 17 physical and 9 mental health disorders. Primary and secondary outcome measures Descriptive analysis of differences in the prevalence of multimorbidity in relation to age, gender and citizenship. The correlations of diseases were analysed using exploratory factor analysis. Results The study population included 622 026 men and 751 011women, with a mean age of 66.4 years. Patients with multimorbidity were 33.5% in 75 years and >60% among patients aged 6590 years; among patients aged 6565 years, the proportion of multimorbidity was 39.9%. After standardisation by age and gender, multimorbidity was significantly more frequent among Italian citizens than among immigrants. Factor analysis identified 5 multimorbidity patterns: (1) psychiatric disorders, (2) cardiovascular, renal, pulmonary and cerebrovascular diseases, (3) neurological diseases, (4) liver diseases, AIDS/HIV and substance abuse and (5) tumours. Conclusions Multimorbidity was highly prevalent in Emilia-Romagna and strongly associated with age. This finding highlights the need for healthcare providers to adopt individualised care plans and ensure continuity of care

Signature of two-electron interference in angular resolved double photoionization of Mg

The double photoionization of Mg has been studied experimentally and theoretically in a kinematic where the two photoelectrons equally share the excess energy. The observation of a symmetrized gerade amplitude, which strongly deviates from the Gaussian ansatz, is explained by a two-electron interference predicted theoretically, but never before observed experimentally. Similar to the Cooper minima in the single photoionization cross section, the effect finds its origin in the radial extent and oscillation of the target wave function

The Low Density Matter (LDM) beamline at FERMI: Optical layout and first commissioning

The Low Density Matter (LDM) beamline has been built as part of the FERMI free-electron laser (FEL) facility to serve the atomic, molecular and cluster physics community. After the commissioning phase, it received the first external users at the end of 2012. The design and characterization of the LDM photon transport system is described, detailing the optical components of the beamline

Two electron interference in angular resolved double photoionization of Mg

The signature of the target wavefunction has been observed in the symmetrized amplitude of the resonant double photoionization of Mg. This observation is based on our experimental study of angle-resolved double photoionization of Mg at the photon energy of 55.49 eV (2p → 3d resonance) under equal energy sharing conditions

Photo-double-ionization of water at 20 eV above threshold

The photodouble ionization of the water molecule is studied at 20 eV excess energy in a combined experimental and theoretical investigation. In the experiments, two photoelectrons of equal kinetic energy are detected in coincidence after energy and angular selection. On the theoretical side, a generalized Sturmian function approach is implemented to describe accurately the correlated two-electron continuum, while separable products of Moccia orbitals [J. Chem. Phys. 40, 2164 (1964)JCPSA60021-960610.1063/1.1725489] are used for the initial electronic state of the water molecule. The theoretical triple-differential cross sections (TDCSs) are averaged over all possible molecular orientations in order to be compared with the experiments. The measured TDCSs display rich angular distributions that are in large part well reproduced by the adopted first-order treatment of the interaction with a two-active-electron target.Fil: Randazzo, Juan Martin. Comisión Nacional de Energía Atómica. Gerencia del Área de Energía Nuclear. Instituto Balseiro; Argentina. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Patagonia Norte; ArgentinaFil: Turri, G.. Embry-riddle Aeronautical University, Physical Sciences; Estados UnidosFil: Bolognesi, P.. CNR-Istituto di Struttura della Materia; ItaliaFil: Mathis, J.. Embry-riddle Aeronautical University, Physical Sciences; Estados UnidosFil: Ancarani, L. U.. Université de Lorraine; FranciaFil: Avaldi, L.. CNR-Istituto di Struttura della Materia; Itali

A procedure to extract the complex amplitudes of He photodouble ionization from experimental data

A procedure to extract the two complex amplitudes that govern the He photodouble ionization process from the experimental data is proposed. The results are compared with the predictions of the convergent close coupling and hyperspherical R-matrix with semiclassical outgoing wave theories