Collective Electron Dynamics Research Articles

Contribution of the collective electron dynamics to the polarization response of an atom subjected to intense IR and weak XUV pulses.

We analyze the polarization response of a single Ne atom in an intense infrared (IR) laser field and weak extreme ultraviolet (XUV) isolated attosecond pulse (IAP). The analysis is based on the numerical solution of the time-dependent Kohn-Sham equations and the recently developed perturbation theory in the XUV field for an atom subjected to an intense IR field. In our numerical results, we observe a significant increase in the magnitude of the atomic polarization response at the frequencies near the carrier frequency of the IAP and associate it with XUV-induced collective dynamics contributing to the polarizability of Ne. The specific interference between IR- and XUV-induced channels is discussed, and its utilization for retrieving the phase of the generated harmonics in the IR field is suggested.

Effects of Electronic Structure on Molecular Plasmon Dynamics

Collective, coherent excitations in molecules, termed molecular plasmons, can be observed in neutral and charged polycyclic aromatic hydrocarbons (PAHs). Systems in this few-atom limit show behavior strongly dependent on charge state, where the addition or removal of even a single electron dramatically alters electronic and optical properties. Here, we investigate the dynamics of PAHs by studying their excited-state lifetimes in four different charge states: cation, neutral, anion, and dianion. Those characterized by a closed-shell electronic structurethe neutral molecule and the dianionexhibit long-lived, exponentially decaying lifetimes typical of radiative relaxation. In contrast, the open-shell cationic and anionic states exhibit far more rapid multiexponential decay dynamics. This can be attributed to the nonradiative de-excitation of multiple electron–hole pairs in the molecule through molecular plasmon “dephasing” and vibrational relaxation. This study gives insight into the nature of excited states of open- and closed-shell molecules and illuminates the role played by electronic structure in the collective electron dynamics of few-atom plasmonic systems.

Magnetic moment generation in small gold nanoparticles via the plasmonic inverse Faraday effect

We theoretically investigate the creation of a magnetic moment in gold nanoparticles by circularly polarized laser light. To this end, we describe the collective electron dynamics in gold nanoparticles using a semiclassical approach based on a quantum hydrodynamic model that incorporates the prin- cipal quantum many-body and nonlocal effects, such as the electron spill-out, the Hartree potential, and the exchange and correlation effects. We use a variational approach to investigate the breathing and the dipole dynamics induced by an external electric field. We show that gold nanoparticles can build up a static magnetic moment through the interaction with a circularly polarized laser field. We analyze that the responsible physical mechanism is a plasmonic, orbital inverse Faraday effect, which can be understood from the time-averaged electron current that contains currents rotating on the nanoparticles surface. The computed laser-induced magnetic moments are sizeable, of about 0.35 muB/atom for a laser intensity of 450 GW/cm2 at plasmon resonance.

Modelling the effects of the radiation reaction force on the interaction of thin foils with ultra-intense laser fields

The effects of the radiation reaction (RR) force on thin foils undergoing radiation pressure acceleration (RPA) are investigated. Using QED-particle-in-cell simulations, the influence of the RR force on the collective electron dynamics within the target can be examined. The magnitude of the RR force is found to be strongly dependent on the target thickness, leading to effects which can be observed on a macroscopic scale, such as changes to the distribution of the emitted radiation and the target dynamics. This suggests that such parameters may be controlled in experiments at multi-PW laser facilities. In addition, the effects of the RR force are characterized in terms of an average radiation emission angle. We present an analytical model which, for the first time, describes the effect of the RR force on the collective electron dynamics within the ‘light-sail’ regime of RPA. The predictions of this model can be tested in future experiments with ultra-high intensity lasers interacting with solid targets.

Influence of laser polarization on collective electron dynamics in ultraintense laser–foil interactions

The collective response of electrons in an ultrathin foil target irradiated by an ultraintense ( ${\sim}6\times 10^{20}~\text{W}~\text{cm}^{-2}$ ) laser pulse is investigated experimentally and via 3D particle-in-cell simulations. It is shown that if the target is sufficiently thin that the laser induces significant radiation pressure, but not thin enough to become relativistically transparent to the laser light, the resulting relativistic electron beam is elliptical, with the major axis of the ellipse directed along the laser polarization axis. When the target thickness is decreased such that it becomes relativistically transparent early in the interaction with the laser pulse, diffraction of the transmitted laser light occurs through a so called ‘relativistic plasma aperture’, inducing structure in the spatial-intensity profile of the beam of energetic electrons. It is shown that the electron beam profile can be modified by variation of the target thickness and degree of ellipticity in the laser polarization.

Optical response of C60 fullerene from a time dependent Thomas Fermi approach

We study the collective electron dynamics in C60 clusters within the time dependent Thomas Fermi method in the frame of jellium model. The results regarding the optical spectrum are in good agreement with the experimental data, our simulations being able to reproduce both resonances from and . We compare also, the results with those from other theoretical approaches and investigate the implications of quantum effects including exchange-correlation corrections, or gradient corrections from a Weizsacker term. The nature of the second resonance is studied using transition densities.

Nonperturbative Hydrodynamic Model for Multiple Harmonics Generation in Metallic Nanostructures

The electromagnetic response of a free-electron gas leads to the inherent nonlinear optical behavior of nanostructured plasmonic materials enabled through both strong local field enhancements and complex collective electron dynamics. Here, a time-domain implementation of the hydrodynamic model for conduction electrons in metals has been developed to enable nonperturbative studies of nonlinear coherent interactions between light and plasmonic nanostructures. The effects originating from the convective acceleration, the magnetic contribution of the Lorenz force, the quantum electron pressure, and the presence of the nanostructure's boundaries have been taken into account, leading to the appearance of both second and third harmonics. The proposed time-domain method enables obtaining a universal, self-consistent numerical solution, free from any approximations, allowing investigations of nonlinear optical interactions with arbitrary spatially and temporally shaped optical pulses, opening unique opportunities to approach description of realistic experimental scenarios.

Azimuthal asymmetry in collective electron dynamics in relativistically transparent laser–foil interactions

Asymmetry in the collective dynamics of ponderomotively-driven electrons in the interaction of an ultraintense laser pulse with a relativistically transparent target is demonstrated experimentally. The 2D profile of the beam of accelerated electrons is shown to change from an ellipse aligned along the laser polarization direction in the case of limited transparency, to a double-lobe structure aligned perpendicular to it when a significant fraction of the laser pulse co-propagates with the electrons. The temporally-resolved dynamics of the interaction are investigated via particle-in-cell simulations. The results provide new insight into the collective response of charged particles to intense laser fields over an extended interaction volume, which is important for a wide range of applications, and in particular for the development of promising new ultraintense laser-driven ion acceleration mechanisms involving ultrathin target foils.

Radiative damping and synchronization in a graphene-based terahertz emitter

We investigate the collective electron dynamics in a recently proposed graphene-based terahertz emitter under the influence of the radiative damping effect, which is included self-consistently in a molecular dynamics approach. We show that under appropriate conditions synchronization of the dynamics of single electrons takes place, leading to a rise of the oscillating component of the charge current. The synchronization time depends dramatically on the applied dc electric field and electron scattering rate and is roughly inversely proportional to the radiative damping rate that is determined by the carrier concentration and the geometrical parameters of the device. The emission spectra in the synchronized state, determined by the oscillating current component, are analyzed. The effective generation of higher harmonics for large values of the radiative damping strength is demonstrated.

Lyapunov stability of charge transport in miniband semiconductor superlattices

We discuss a numerical method for the calculation of the spectrum of Lyapunov exponents for spatially extended systems described by coupled Poisson and continuity equations. This approach was applied to the model of collective charge transport in semiconductor superlattices operating in the miniband transport regime. The method is in very good agreement with analytical results obtained for the steady state. As an illustrative example, we consider the collective electron dynamics in the superlattice subjected to an ac voltage and a tilted magnetic field, and conclusively show that, depending on the field parameters, the dynamics can exhibit periodic, quasiperiodic, or chaotic behavior.

High-harmonic and single attosecond pulse generation using plasmonic field enhancement in ordered arrays of gold nanoparticles with chirped laser pulses

Coherent XUV sources, which may operate at MHz repetition rate, could find applications in high-precision spectroscopy and for spatio-time-resolved measurements of collective electron dynamics on nanostructured surfaces. We theoretically investigate utilizing the enhanced plasmonic fields in an ordered array of gold nanoparticles for the generation of high-harmonic, extreme-ultraviolet (XUV) radiation. By optimization of the chirp of ultrashort laser pulses incident on the array, our simulations indicate a potential route towards the temporal shaping of the plasmonic near-field and, in turn, the generation of single attosecond pulses. The inherent effects of inhomogeneity of the local fields on the high-harmonic generation are analyzed and discussed. While taking the inhomogeneity into account does not affect the optimal chirp for the generation of a single attosecond pulse, the cut-off energy of the high-harmonic spectrum is enhanced by about a factor of two.

Enhanced collective focusing of intense neutralized ion beam pulses in the presence of weak solenoidal magnetic fields

The design of ion drivers for warm dense matter and high energy density physics applications and heavy ion fusion involves transverse focusing and longitudinal compression of intense ion beams to a small spot size on the target. To facilitate the process, the compression occurs in a long drift section filled with a dense background plasma, which neutralizes the intense beam self-fields. Typically, the ion bunch charge is better neutralized than its current, and as a result a net self-pinching (magnetic) force is produced. The self-pinching effect is of particular practical importance, and is used in various ion driver designs in order to control the transverse beam envelope. In the present work we demonstrate that this radial self-focusing force can be significantly enhanced if a weak (B ∼ 100 G) solenoidal magnetic field is applied inside the neutralized drift section, thus allowing for substantially improved transport. It is shown that in contrast to magnetic self-pinching, the enhanced collective self-focusing has a radial electric field component and occurs as a result of the overcompensation of the beam charge by plasma electrons, whereas the beam current becomes well-neutralized. As the beam leaves the neutralizing drift section, additional transverse focusing can be applied. For instance, in the neutralized drift compression experiments (NDCX) a strong (several Tesla) final focus solenoid is used for this purpose. In the present analysis we propose that the tight final focus in the NDCX experiments may possibly be achieved by using a much weaker (few hundred Gauss) magnetic lens, provided the ion beam carries an equal amount of co-moving neutralizing electrons from the preceding drift section into the lens. In this case the enhanced focusing is provided by the collective electron dynamics strongly affected by a weak applied magnetic field.

Effect of temperature on resonant electron transport through stochastic conduction channels in superlattices

We show that resonant electron transport in semiconductor superlattices with an applied electric and tilted magnetic field can, surprisingly, become more pronounced as the lattice and conduction electron temperature increases from 4.2 K to room temperature and beyond. It has previously been demonstrated that at certain critical field parameters, the semiclassical trajectories of electrons in the lowest miniband of the superlattice change abruptly from fully localised to completely unbounded. The unbounded electron orbits propagate through intricate web patterns, known as stochastic webs, in phase space, which act as conduction channels for the electrons and produce a series of resonant peaks in the electron drift velocity versus electric field curves. Here, we show that increasing the lattice temperature strengthens these resonant peaks due to a subtle interplay between thermal population of the conduction channels and transport along them. This enhances both the electron drift velocity and the influence of the stochastic webs on the current-voltage characteristics, which we calculate by making self-consistent solutions of the coupled electron transport and Poisson equations throughout the superlattice. These solutions reveal that increasing the temperature also transforms the collective electron dynamics by changing both the threshold voltage required for the onset of self-sustained current oscillations, produced by propagating charge domains, and the oscillation frequency.

Attosecond nanoplasmonic streaking of localized fields near metal nanospheres

Collective electron dynamics in plasmonic nanosystems can unfold on timescales in the attosec- ond regime and the direct measurements of plasmonic near-field oscillations is highly desirable. We report on numerical studies on the application of attosecond nanoplasmonic streaking spectroscopy to the measurement of collective electron dynamics in isolated Au nanospheres. The plasmonic field oscillations are induced by a few-cycle NIR driving field and are mapped by the energy of photoemitted electrons using a synchronized, time-delayed attosecond XUV pulse. By a detailed analysis of the amplitudes and phase shifts, we identify the different regimes of nanoplasmonic streaking and study the dependence on particle size, XUV photoelectron energy and emission position. The simulations indicate that the near-fields around the nanoparticles can be spatio-temporally reconstructed and may give detailed insight into the build-up and decay of collective electron motion.

Attosecond control of electrons emitted from a nanoscale metal tip

Attosecond science is based on steering electrons with the electric field of well controlled femtosecond laser pulses. It has led to the generation of extreme-ultraviolet pulses with a duration of less than 100 attoseconds (ref. 3; 1 as = 10(-18) s), to the measurement of intramolecular dynamics (by diffraction of an electron taken from the molecule under scrutiny) and to ultrafast electron holography. All these effects have been observed with atoms or molecules in the gas phase. Electrons liberated from solids by few-cycle laser pulses are also predicted to show a strong light-phase sensitivity, but only very small effects have been observed. Here we report that the spectra of electrons undergoing photoemission from a nanometre-scale tungsten tip show a dependence on the carrier-envelope phase of the laser, with a current modulation of up to 100 per cent. Depending on the carrier-envelope phase, electrons are emitted either from a single sub-500-attosecond interval of the 6-femtosecond laser pulse, or from two such intervals; the latter case leads to spectral interference. We also show that coherent elastic re-scattering of liberated electrons takes place at the metal surface. Owing to field enhancement at the tip, a simple laser oscillator reaches the peak electric field strengths required for attosecond experiments at 100-megahertz repetition rates, rendering complex amplified laser systems dispensable. Practically, this work represents a simple, extremely sensitive carrier-envelope phase sensor, which could be shrunk in volume to about one cubic centimetre. Our results indicate that the attosecond techniques developed with (and for) atoms and molecules can also be used with solids. In particular, we foresee subfemtosecond, subnanometre probing of collective electron dynamics (such as plasmon polaritons) in solid-state systems ranging in scale from mesoscopic solids to clusters and to single protruding atoms.

Efficient ion acceleration by collective laser-driven electron dynamics with ultra-thin foil targets

AbstractExperiments on ion acceleration by irradiation of ultra-thin diamond-like carbon (DLC) foils, with thicknesses well below the skin depth, irradiated with laser pulses of ultra-high contrast and linear polarization, are presented. A maximum energy of 13 MeV for protons and 71 MeV for carbon ions is observed with a conversion efficiency of ~10%. Two-dimensional particle-in-cell (PIC) simulations reveal that the increase in ion energies can be attributed to a dominantly collective rather than thermal motion of the foil electrons, when the target becomes transparent for the incident laser pulse.

Controlling and enhancing terahertz collective electron dynamics in superlattices by chaos-assisted miniband transport

We show that a tilted magnetic field transforms the structure and THz dynamics of charge domains in a biased semiconductor superlattice. At critical field values, strong coupling between the Bloch and cyclotron motion of a miniband electron triggers chaotic delocalization of the electron orbits, causing strong resonant enhancement of their drift velocity. This dramatically affects the collective electron behavior by inducing multiple propagating charge domains and GHz-THz current oscillations with frequencies ten times higher than with no tilted field.

Ultrafast collective electron dynamics in open-shell ions

We use the time-dependent R-matrix approach to investigate an ultra-short pump-probe scheme to observe collective electron dynamics in C+. The ionization probability of a coherent superposition of the 2s2p2 2D and 2S states shows rapid oscillations due to collective dynamics of the two equivalent 2p electrons, with the frequency of the oscillations linked to the electron-electron interaction. We find that deeper insight into this collective dynamics is gained by transforming the atomic structure from LS symmetry to the uncoupled basis. We discuss how such dynamics may be important in high-harmonic generation using open-shell atoms and ions.

Signatures of collective electron dynamics in the angular distributions of electrons ejected during ultrashort laser pulse interactions with C+

We use the time-dependent R-matrix approach to investigate an ultrashort pump–probe scheme to observe collective electron dynamics in C+ driven by the repulsion of two equivalent p electrons. By studying the two-dimensional momentum distributions of the ejected electron as a function of the time-delay between an ultrashort pump pulse and an ionizing ultrashort probe pulse it is possible to track the collective dynamics inside the C+ ion in the time domain.

Ultrafast Probing of Collective Electron Dynamics Driven by Dielectronic Repulsion

We use the time-dependent R-matrix approach to investigate an ultrashort pump-probe scheme to observe collective electron dynamics in C+. The ionization probability of a coherent superposition of the 2s2p;{2} 2D and 2S states shows rapid modulation due to collective dynamics of the two equivalent 2p electrons, with the modulation frequency linked to the dielectronic repulsion. The best insight into this collective dynamics is achieved by a transformation from LS symmetry to the uncoupled basis. Such dynamics may be important in high-harmonic generation using open-shell atoms and ions.