Time‐resolved photoelectron nano‐spectroscopy of individual silver particles: Perspectives and limitations

Rohmer, Martin; Bauer, Michael; Leißner, Till; Schneider, Christian; Fischer, Alexander; Niedner‐Schatteburg, Gereon; Issendorff, Bernd von; Aeschlimann, Martin

doi:10.1002/pssb.200945479

Cited by 18 publications

(22 citation statements)

References 28 publications

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“…This is done on purpose as will become clear below in Eq. (20). The self-interaction corrected KS equations are then derived again by variation.…”

Section: The Self-interaction Problem In Dft and Tddftmentioning

confidence: 99%

“…Eqs. (18)(19)(20)(21) formulate the SIC problem in the "2setSIC" scheme. They are solved by interlaced iterations.…”

Section: The Self-interaction Problem In Dft and Tddftmentioning

confidence: 99%

“…Moreover, Time-Resolved (TR) PES and PAD have been recorded in molecules [19] and more recently in clusters, see e.g. [20]. Electrons are thus leading players at all stages of an excitation of a system subject to an external electromagnetic perturbation (i.e.…”

Section: General Introduction and Physical Contextmentioning

confidence: 99%

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Electrons as probes of dynamics in molecules and clusters: A contribution from Time Dependent Density Functional Theory

et al. 2015

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a b s t r a c tThere are various ways to analyze the dynamical response of clusters and molecules to electromagnetic perturbations. Particularly rich information can be obtained from measuring the properties of electrons emitted in the course of the excitation dynamics. Such an analysis of electron signals covers observables such as total ionization, PhotoElectron Spectra (PES), Photoelectron Angular Distributions (PAD), and ideally combined PES/PAD. It has a long history in molecular physics and was increasingly used in cluster physics as well. Recent progress in the design of new light sources (high intensity, high frequency, ultra short pulses) opens new possibilities for measurements and thus has renewed the interest on these observables, especially for the analysis of various dynamical scenarios, well beyond a simple access to electronic density of states. This, in turn, has motivated many theoretical investigations of the dynamics of electronic emission for molecules and clusters up to such a complex and interesting system as C 60 . A theoretical tool of choice is here Time-Dependent Density Functional Theory (TDDFT) propagated in real time and on a spatial grid, and augmented by a Self-Interaction Correction (SIC). This provides a pertinent, robust, and efficient description of electronic emission including the detailed pattern of PES and PAD. A direct comparison between experiments and well founded elaborate microscopic theories is thus readily possible, at variance with more demanding observables such as for example fragmentation or dissociation cross sections.The purpose of this paper is to describe the theoretical tools developed on the basis of real-time and real-space TDDFT and to address in a realistic manner the analysis of electronic emission following irradiation of clusters and molecules by various laser pulses. After a general introduction, we shall present in a second part the available experimental results motivating such studies, starting from the simplest total ionization signals to the more elaborate PES and PAD, possibly combining them and/or resolving them in time. This experimental discussion will be complemented in a third part by a presentation of available theoretical tools focusing on TDDFT and detailing the methods used to address ionization observables. We shall also discuss the shortcomings of standard versions of TDDFT, especially what concerns the SIC problem, and show how to improve formally and practically the theory on that aspect. A long fourth part will be devoted to representative * P. Wopperer et al. / Physics Reports ( ) -results. We shall illustrate the use of total ionization in pump and probe scenarios with fs lasers for tracking ionic dynamics in clusters. More challenging from the experimental point of view is pump and probe setups using attosecond pulses. The effort there is more on the capability to define proper signals to be measured/computed at such a short time scale. TDDFT analysis provides here a valuable tool in the search for the most efficient observab...

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“…This is done on purpose as will become clear below in Eq. (20). The self-interaction corrected KS equations are then derived again by variation.…”

Section: The Self-interaction Problem In Dft and Tddftmentioning

confidence: 99%

“…Eqs. (18)(19)(20)(21) formulate the SIC problem in the "2setSIC" scheme. They are solved by interlaced iterations.…”

Section: The Self-interaction Problem In Dft and Tddftmentioning

confidence: 99%

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Electrons as probes of dynamics in molecules and clusters: A contribution from Time Dependent Density Functional Theory

et al. 2015

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“…Several studies have addressed the surface plasmon propagation directly in and in the vicinity of differently shaped metal nanostructures [4][5][6][7][8]. Quite recently, energy-resolved 2P-PEEM measurements have been demonstrated for the first time [9,10]. Aside from these pure laser pump-probe experiments, combinations with synchrotron X-rays have also been developed to obtain access to the temporal evolution of magnetic structures [11,12].…”

Section: Introductionmentioning

confidence: 99%

Laser-excited PEEM using a fully tunable fs-laser system

et al. 2011

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The ferroelectric domain structure on a (001) surface of a BaTiO 3 single crystal prepared under ultrahigh vacuum conditions is imaged by laser-excited photoemission electron microscopy (PEEM). The PEEM images allow for discrimination of three domain types by their different photoemission yields. To characterize the contrast between the different ferroelectric domains of BaTiO 3 (001) in the region of 4.0-4.6 eV close to the photoemission threshold, the broad wavelength tunability of the femtosecond laser system is used. The femtosecond time resolution within two-photon PEEM experiments, using two fully independently tunable laser beams, is demonstrated for the first image potential state of Ag(001). In a pump-probe setup with a cross-correlation full-width at half-maximum of 70 fs, an angle-integrated apparent lifetime of 40 fs is derived from the PEEM intensities. In contrast with energy-resolved two-photon photoemission measurements, PEEM data reveal a 17-fs shorter lifetime. This difference is discussed by considering the co-excitation of bulk states, which leads to an additional time-dependent photoelectron contribution in PEEM.

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“…This is a non-invasive, element-specific technique providing quantitative information about the chemical composition, electronic structure, and magnetism of individual NP, both static 23,27,28 and time-resolved. 24,29 Using this unique approach, we find that NP that appear homogeneous in crystal quality and macroscopic magnetic response in a monodisperse ensemble can exhibit a striking size-independent coexistence of NP with distinct Fe oxide phases as a result of the uncontrolled reduction of Fe 3+ during the reaction process.…”

Section: Introductionmentioning

confidence: 99%

Probing the variability in oxidation states of magnetite nanoparticles by single-particle spectroscopy

et al. 2018

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We have studied the electronic and chemical properties of a variety of ensembles of size-and shapeselected Fe 3 O 4 nanoparticles with single-particle sensitivity by means of synchrotron-based X-ray photoemission electron microscopy. The local X-ray absorption spectra reveal that the oxidation states and the amount and type of cations within the individual nanoparticles can show a striking local variability even when the average structural and magnetic parameters of the monodisperse ensembles appear to be

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Time‐resolved photoelectron nano‐spectroscopy of individual silver particles: Perspectives and limitations

Cited by 18 publications

References 28 publications

Electrons as probes of dynamics in molecules and clusters: A contribution from Time Dependent Density Functional Theory

Electrons as probes of dynamics in molecules and clusters: A contribution from Time Dependent Density Functional Theory

Laser-excited PEEM using a fully tunable fs-laser system

Probing the variability in oxidation states of magnetite nanoparticles by single-particle spectroscopy

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