Theory for the ultrafast dynamics of excited clusters: interplay between elementary excitations and atomic structure

We present a theoretical study of the short-time relaxation of clusters in response to ultrafast excitations using femtosecond laser pulses. We analyze the excitation of different types of clusters (Hg_n, Ag_n, Si_n, C₆₀ and Xe_n) and classify the relaxation dynamics in three different regimes, depending on the intensity of the exciting laser pulse. For low-intensity pulses (I<10¹² W/cm²) we determine the time-dependent structural changes of clusters upon ultrashort ionization and photodetachment. We also study the laser-induced non-equilibrium fragmentation and melting of Si_n and C₆₀ clusters, which occurs for moderate laser intensities, as a function of the pulse duration and energy. As an example for the case of high intensities (I>10¹⁵ W/cm²), the explosion of clusters under the action of very intense ultrashort laser fields is described. Received: 26 November 1999 / Published online: 2 August 2000     

Femtosecond dynamics and coherent control in atoms, molecules and clusters: Theory and experiments

The understanding and control of the dynamics in atoms, molecules and clusters has been a tremendously growing field in the past decade. This has been acknowledged with the 1999 Nobel prize in chemistry awarded to Ahmed Zewail. The present issue collects some of the newest theoretical and experimental results in the field of ultrafast dynamics and coherent control in the gas phase. The papers are grouped into three categories. The first section contains work on the “Coherent Control with Femtosecond Laser Pulses”. Topics like the general theory of quantum control, the control of electron transfer processes, transformation of chiral molecules and coherent population transfer are treated here. The “Femtosecond Dynamics” taking place in molecules and clusters is the topic of the second section. New insight into the nature of atomic motion within molecules and relaxation processes is provided. The last section collects most recent work on the interaction of ultrashort laser pulses with matter. In particular, high harmonic generation, multi-photon ionization and interference effects, as well as the possible orientation of molecules in external fields are discussed. We think that the present compilation demonstrates that the field of ultrashort pulse spectroscopy is of still growing importance and exciting new phenomena have been revealed in the past and will be discovered in the future.     

Optical pump-probe scanning tunneling microscopy for probing ultrafast dynamics on the nanoscale

The development of a method for exploring the ultrafast transient dynamics in small organized structures with high spatial resolution is expected to be a basis for further advances in current science and technology. Recently, we have developed a new microscopy technique by combining scanning tunneling microscopy (STM) with ultrashort-pulse laser technology, which enables the visualization of ultrafast carrier dynamics even on the single-atomic level. A nonequilibrium carrier distribution is generated using ultrashort laser pulses and its relaxation processes are probed by STM using the optical pump-probe method realized in STM by the pulse-picking technique. In this paper, the fundamentals of the new microscopy technique are overviewed.     

Dynamics in a cluster under the influence of intense femtosecond hard X-ray pulses

In this paper we examine the behavior of small cluster of atoms in a short (10-50 fs) very intense hard X-ray (10 keV) pulse. We use numerical modeling based on the non-relativistic classical equation of motion. Quantum processes are taken into account by the respective cross-sections. We show that there is a Coulomb explosion, which has a different dynamics than one finds in classical laser driven cluster explosions. We discuss the consequences of our results to single molecule imaging by the free electron laser pulses.Received: 22 September 2003, Published online: 9 March 2004PACS: 61.80.-x Physical radiation effects, radiation damage - 36.40.-c Atomic and molecular clusters - 61.46. + w Nanoscale materials: clusters, nanoparticles, nanotubes, and nanocrystals     

Controlling energy coupling and particle ejection from aluminum surfaces irradiated with ultrashort laser pulses

Hydrodynamic simulations are used to evaluate the potential of ultrashort laser pulses to localize energy at metallic surfaces, in our case aluminum. The emphasis is put on the dynamic sequence of laser energy deposition steps during the electron-ion nonequilibrium stage and the subsequent matter transformation phases. The simulations indicate correlated optical and thermodynamical states associated to specific electronic collisional mechanisms. The timescales of energy deposition deliver a guideline for using relevant relaxation times to improve the energy coupling into the material. We focus on a class of pump-probe experiments which investigate energy storage and particle emission from solids under ultrafast laser irradiation. Moreover, we have used our model to explain the experimentally observed optimization of energy coupling by tailoring temporal laser intensity envelopes and its subsequent influence on the ablation rate and on the composition of ablation products. Potential control for nanoparticle generation is discussed.     

Energy distribution curves of ultrafast laser-induced field emission and their implications for electron dynamics

Energy distribution curves of laser-induced electron pulses from a tungsten tip have been measured as a function of tip voltage and laser power. Electron emission via tunneling through and/or excitation over the surface barrier from photoexcited nonequilibrium electron distributions are clearly observed. The spectral shapes largely vary with the emission processes and are strongly affected by electron dynamics. Simulations successfully reproduce the spectra, thus allowing direct insight into the involved electron dynamics and revealing the temporal tunability of electron emission via the two experimental parameters. These results should be useful to optimize the pulse characteristics for many applications based on ultrafast laser-induced electron emission.     

Progress in sub-femtosecond control of electron localization in molecules

Recent advances in controlled generation of intense, ultrashort laser pulses in the femtosecond and attosecond time-scales have pushed new avenues of research in the coherent control of ultrafast electron dynamics in atoms and molecules. We present a topical review on the phenomenon of control of electron localization in small dissociating molecules. By creating and controlling coherent superposition of the symmetric and antisymmetric electronic states, it becomes possible to confine the evolving electron cloud onto a preferred nucleus, thereby steering the molecule towards a desired dissociation route. We discuss the origin of the idea and various mechanisms to achieve electron localization in small molecules. To highlight recent experimental progress, we explain how one can employ few-cycle IR pulses and different attosecond extreme ultraviolet (EUV) pulses in various ways to successfully demonstrate the control of electronic dynamics. Future research opportunities and challenges on this topic are envisioned.     

Observation of subpicosecond x-ray emission from laser-cluster interaction

We present the first experimental evidence of the subpicosecond duration of x-ray pulses emitted from laser-irradiated clusters, demonstrating the suitability of such a debris free target for ultrafast x-ray science applications. The K-shell emission (approximately 3 keV) from large Ar clusters (6 x 10(5) to 4 x 10(6) atoms) is time resolved, when irradiated by ultrashort (40 fs to 5 ps) and intense laser pulses (10(15-17) W/cm2). The observations are supported by hydrodynamical and collisional-radiative calculations, that reproduce the extremely short x-ray pulse duration.     

Structural preablation dynamics of graphite observed by ultrafast electron crystallography

By means of time-resolved electron crystallography, we report direct observation of the structural dynamics of graphite, providing new insights into the processes involving coherent lattice motions and ultrafast graphene ablation. When graphite is excited by an ultrashort laser pulse, the excited carriers reach their equilibrium in less then one picosecond by transferring heat to a subset of strongly coupled optical phonons. The time-resolved diffraction data show that on such a time scale the crystal undergoes a contraction whose velocity depends on the excitation fluence. The contraction is followed by a large expansion which, at sufficiently high fluence, leads to the ablation of entire graphene layers, as recently predicted theoretically.     

Generation of Broadband High Harmonics through Linear Mode Conversion in Inhomogeneous Plasmas

The generation of high order harmonics from an inhomogeneous ovderdense plasma target irradiated by an ultrashort intense laser pulse is studied by numerical simulation. During such interaction, ultrafast electron bunches are generated and excite electron plasma oscillations as they pass through the overdense target. These plasma oscillations will emit high-frequency electromagnetic emission by linear mode conversion. Instead of the integer harmonies generation, the emission appears with a broadband and even continuous spectrum corresponding to the electron plasma frequency range of the inhomogeneous plasma density.     

Ultrafast relaxation dynamics of electronic excitations in noble-metal clusters

We investigate non-equilibrium relaxation processes in optically excited large gold and silver clusters. Time-resolved pump-probe experiments and model calculations show that optical excitation of the clusters by femtosecond laser pulses results in a heating of the electron system, which is followed by electron cooling via phonon emission. The electron heating leads to an enhanced damping of the surface-plasmon resonance in the clusters. This enhanced damping is caused by an enhancement of the Landau damping and electron scattering rates at high electron temperatures. Furthermore, we find that the rate of electron cooling in the clusters changes with electron temperature; this is a consequence of the temperature-dependent specific heat of the conduction electrons. Finally, pump-probe experiments on ellipsoidal silver clusters show that the thermal expansion of the heated clusters triggers mechanical vibrations at the acoustic eigenfrequencies of the clusters. Received: 6 December 1999 / Published online: 7 August 2000     

Selective cap opening in carbon nanotubes driven by laser-induced coherent phonons

We demonstrate the possibility of a selective nonequilibrium cap opening of carbon nanotubes as a response to femtosecond laser excitation. By performing molecular dynamics simulations based on a microscopic electronic model we show that the laser-induced ultrafast structural changes differ dramatically from the thermally induced dimer emission. Ultrafast bond weakening and simultaneous excitation of two coherent phonon modes of different frequencies, localized in the spherical caps and cylindrical nanotube body, are responsible for the selective cap opening.     

Dynamics of Na clusters in picosecond laser pulses

We investigate the electronic and ionic dynamics of Na clusters under the influence of a laser pulse in the range 100 femtoseconds to picoseconds. The dynamics is described by means of the time-dependent local-density approximation coupled to ionic molecular dynamics (TDLDA-MD). Variation of pulse length allows us to explore the time scales of ionic motion in a manner similar to pump and probe experiments. Resonant enhancement of electron emission serves as a measure for the time scale of Coulomb explosion. Received: 3 July 2001 / Published online: 10 October 2001     

Insight into the thermionic emission regimes under gold film thermal relaxation excited by a femtosecond pulse

We theoretically investigated different thermal relaxation participating in the ultrafast thermionic emission processes on gold film surface with a femtosecond pulse excitation. The thermionic emission regimes under the two temperature relaxation and the thermal diffusion relaxation were demonstrated. The simulations showed that the thermionic emission properties can be defined in the regime under two temperature relaxation by reducing the laser fluence, or widening the pulse duration or increasing the laser wavelength. It was also found that there exists a transition between the two distinct thermionic emission regimes under peculiar laser parameters of laser fluence, pulse duration and laser wavelength. The results were explained as significant intervene of laser irradiation parameters into gold film thermal relaxation processes.     

Ultrafast laser spectroscopy of semiconductor nanocrystals

A large amount of work has been worldwide directed to understand the properties of semiconductor nanostructures. Ultrafast lasers with pulsewidths of a few femtoseconds allowed the investigation of the dynamics of elementary excitations in semiconductor structures on ultrashort time scales. Recent progress in technology made it possible to fabricate semiconductor nanocrystals (i.e. crystals of nanometer dimensions) of well-defined properties. The purpose of this paper is to review the understanding of carrier relaxation and recombination processes in semiconductor nanocrystals as studied by ultrafast laser spectroscopy. The up-to-date techniques of ultrafast laser spectroscopy as well as the fabrication of semiconductor nanocrystals are discussed in some detail.     

Attosecond pump probe: exploring ultrafast electron motion inside an atom

The attosecond pump probe, in close analogy to the standard femtosecond probing technique, has been proposed and theoretically demonstrated with its application to explore ultrafast electron motions inside atoms. We have performed realistic modeling for the full dynamics of both the femtosecond pumping and the attosecond probing processes. Our simulations have illustrated that an ultrashort oscillation period of 2.0 fs can be mapped out for a wave packet in low-lying excited states of the helium atom. This opens the prospect of a wealth of similar pump probe experiments to examine ultrafast electronic or atomic motions.     

Ultrafast structural dynamics with table top femtosecond hard X-ray and electron diffraction setups

The following tutorial review is directed to graduate students willing to be part of the emerging field of ultrafast structural dynamics. It provides them with an introduction to the field and all the very basic assumptions and experimental tricks involved in femtosecond (fs) diffraction techniques. The concept of stroboscopic photography and its implication in ultrafast science are introduced. Special attention is paid to the generation of ultrashort electron and hard X-ray pulses in table top setups, and a direct comparison in terms of brightness and temporal resolution between current table top and facility-based methodologies is given for proper calibration. This review is focused on ultrafast X-ray and electron diffraction techniques. The progress in the development of fs-structural probes during the last twenty years has been tremendous. Current ultrafast structural probes provide us with the temporal and spatial resolutions required to observe atoms in motion. Different compression approaches have made it possible the generation of ultrashort and ultrabright electron pulses with an effective brightness close to that of fs-hard X-ray pulses produced by free electron lasers. We now have in hand a variety of ultrafast structural cameras ready to be applied for the study of an endless list of dynamical phenomena at the atomic level of inspection.     

Effect of ballistic electrons on ultrafast thermomechanical responses of a thin metal film

The ultrafast thermomechanical coupling problem in a thin gold film irradiated by ultrashort laser pulses with different electron ballistic depths is investigated via the ultrafast thermoelasticity model. The solution of the problem is obtained by solving finite element governing equations. The comparison between the results of ultrafast thermomechanical coupling responses with different electron ballistic depths is made to show the ballistic electron effect. It is found that the ballistic electrons have a significant influence on the ultrafast thermomechanical coupling behaviors of the gold thin film and the best laser micromachining results can be achieved by choosing the specific laser technology(large or small ballistic range).In addition, the influence of simplification of the ultrashort laser pulse source on the results is studied, and it is found that the simplification has a great influence on the thermomechanical responses, which implies that care should be taken when the simplified form of the laser source term is applied as the Gaussian heat source.