Ben Torralva

Single-shot dynamic transmission electron microscopy

A dynamic transmission electron microscope (DTEM) has been designed and implemented to study structural dynamics in condensed matter systems. The DTEM is a conventional in situ transmission electron microscope (TEM) modified to drive material processes with a nanosecond laser, “pump” pulse and measure it shortly afterward with a 30-ns-long probe pulse of ∼107 electrons. An image with a resolution of <20nm may be obtained with a single pulse, largely eliminating the need to average multiple measurements and enabling the study of unique, irreversible events with nanosecond- and nanometer-scale resolution. Space charge effects, while unavoidable at such a high current, may be kept to reasonable levels by appropriate choices of operating parameters. Applications include the study of phase transformations and defect dynamics at length and time scales difficult to access with any other technique. This single-shot approach is complementary to stroboscopic TEM, which is capable of much higher temporal resolution ...

Deforming nanocrystalline nickel at ultrahigh strain rates

The deformation mechanism of nanocrystalline Ni (with grain sizes in the range of 30–100 nm) at ultrahigh strain rates (>107s−1) was investigated. A laser-driven compression process was applied to achieve high pressures (20–70 GPa) on nanosecond timescales and thus induce high-strain-rate deformation in the nanocrystalline Ni. Postmortem transmission electron microscopy examinations revealed that the nanocrystalline structures survive the shock deformation, and that dislocation activity is a prevalent deformation mechanism for the grain sizes studied. No deformation twinning was observed even at stresses more than twice the threshold for twin formation in micron-sized polycrystals. These results agree qualitatively with molecular dynamics simulations and suggest that twinning is a difficult event in nanocrystalline Ni under shock-loading conditions.

Semiclassical electron-radiation-ion dynamics (SERID) and cis-trans photoisomerization of butadiene

Abstract Detailed simulations are reported for the dynamics of electrons and nuclei during the cis—trans isomerization of butadiene following a femtosecond-scale laser pulse. Our technique, semiclassical electron-radiationion dynamics (SERID), is fully described in the text. The one-electron Hamiltonian and ion—ion interactions employed in the present work are density-functional based. Following excitation of electrons by the laser pulse, all three C—C bonds in the butadiene molecule become longer, as electrons are promoted from the HOMO to both the LUMO and LUMO+1 levels. In the excited electronic state, the molecule rotates about all of its three C—C bonds. There are then non-adiabatic events near avoided crossings, with electronic transitions to the ground state via creation of vibrational excitations. The molecule continues to twist around the central bond and one of the terminal C—C bonds, until the trans-conformation is achieved. Various features in the behaviour of the vibrational modes can also be observed, including initial excitations due to the laser pulse, further excitations at avoided crossings and the redistribution of vibrational energy between modes.

Prospects for electron imaging with ultrafast time resolution

Many pivotal aspects of material science, biomechanics, and chemistry would benefit from nanometer imaging with ultrafast time resolution. Here we demonstrate the feasibility of short-pulse electron imaging with t10 nanometer/10 picosecond spatio-temporal resolution, sufficient to characterize phenomena that propagate at the speed of sound in materials (1-10 kilometer/second) without smearing. We outline resolution-degrading effects that occur at high current density followed by strategies to mitigate these effects. Finally, we present a model electron imaging system that achieves 10 nanometer/10 picosecond spatio-temporal resolution.

Importance of electronic self-consistency in the TDDFT based treatment of nonadiabatic molecular dynamics

Abstract.A mixed quantum-classical approach to simulate the coupled dynamics of electrons and nuclei in nanoscale molecular systems is presented. The method relies on a second order expansion of the Lagrangian in time-dependent density functional theory (TDDFT) around a suitable reference density. We show that the inclusion of the second order term renders the method a self-consistent scheme and improves the calculated optical spectra of molecules by a proper treatment of the coupled response. In the application to ion-fullerene collisions, the inclusion of self-consistency is found to be crucial for a correct description of the charge transfer between projectile and target. For a model of the photoreceptor in retinal proteins, nonadiabatic molecular dynamics simulations are performed and reveal problems of TDDFT in the prediction of intra-molecular charge transfer excitations.

Mechanisms for laser control of chemical reactions

During the past several years, a new technique for realistic simulations of the interaction of light with matter has been developed and employed. Recent simulations of laser pulses interacting with molecules clearly demonstrate the potential for control of chemical reactions through various mechanisms, which include the following: (i) excitation of electrons to states that have different bonding properties; (ii) control of electron populations through a coherent pump-pulse, control-pulse sequence; and (iii) control of molecular vibrations through a pump-control sequence. Significant chemical insights are gained when one can watch a realistic animation of species interacting and reacting. One can monitor the time evolution of electronic states and their occupancy, as well as the motion of the atoms. One can also observe the evolution from reactants to products through transition states. Finally, one can determine how this evolution is affected by the various properties of the laser pulses, including intensity, duration, phase, and the interval between pulses.

The role of an interface on Ni film removal and surface roughness after irradiation by femtosecond laser pulses

We have observed thin film removal from glass substrates after the irradiation of Ni films with femtosecond laser pulses in air. It was found that the material removal threshold and laser-induced morphology are dependent on film thickness. With decreasing thickness, material removal transitions from intra-film separation to removal at the Ni-glass interface. The Gaussian energy distribution of the laser pulse allows for intra-film separation in the annular region of the crater and interface separation in the center. We propose a model to explain these data as well as the observed increased surface roughness in the interfacial removal regions.

Laser-induced periodic surface structure formation resulting from single-pulse ultrafast irradiation of Au microstructures on a Si substrate

We have observed laser-induced periodic surface structure (LIPSS) formation with sub-micron periodicities after single-pulse ultrafast irradiation of isolated, 110 nm-tall Au microstructures on Si substrates. Fresnel diffraction patterns are established on both the structure surface and surrounding Si substrate when light is scattered by feature edges, and the resultant intensity distribution is partially responsible for LIPSS formation. LIPSS form for any in-plane, laser polarization orientation with respect to surface feature edges, although the LIPSS amplitude varies with the orientation. This explains the formation of LIPSS patterns having different wavevectors and amplitudes after multi-pulse irradiation of initially smooth surfaces.

Pump-probe imaging of laser-induced periodic surface structures after ultrafast irradiation of Si

Ultrafast pump-probe microscopy has been used to investigate laser-induced periodic surface structure (LIPSS) formation on polished Si surfaces. A crater forms on the surface after irradiation by a 150 fs laser pulse, and a second, subsequent pulse forms LIPSS within the crater. Sequentially delayed images show that LIPSS with a periodicity slightly less than the fundamental laser wavelength of 780 nm appear on Si surfaces ∼50 ps after arrival of the second pump laser pulse, well after the onset of melting. LIPSS are observed on the same timescale as material removal, suggesting that their formation involves material ejection.

Nanoparticle size and morphology control using ultrafast laser induced forward transfer of Ni thin films

We have developed a nanoparticle (NP) printing technique using Ni thin film lift-off from glass substrates after ultrafast irradiation in air. Unique interactions of ultrafast laser pulses with thin films allow for control over NP faceting and size distributions. Control is achieved by changing the laser fluence, film thickness, and film-substrate distance. We demonstrate 20 nm Ni film removal from substrates and rapid NP printing, with size distributions centered at a 6 nm diameter. When the Ni film thickness is lowered to 10 nm, NPs are printed with distributions peaked at a 2 nm diameter.