Intrinsic dichroism in amorphous and crystalline solids with helical light.

Amorphous solids do not exhibit long-range order due to the disordered arrangement of atoms. They lack translational and rotational symmetry on a macroscopic scale and are therefore isotropic. As a result, differential absorption of polarized light, called dichroism, is not known to exist in amorphous solids. Using helical light beams that carry orbital angular momentum as a probe, we demonstrate that dichroism is intrinsic to both amorphous and crystalline solids. We show that in the nonlinear regime, helical dichroism is responsive to the short-range order and its origin is explained in terms of interband multiphoton assisted tunneling. We also demonstrate that the helical dichroism signal is sensitive to chirality and its strength can be controlled and tuned using a superposition of OAM and Gaussian beams. Our research challenges the conventional knowledge that dichroism does not exist in amorphous solids and enables to manipulate the optical properties of solids.

Orbital perspective on high-harmonic generation from solids.

High-harmonic generation in solids allows probing and controlling electron dynamics in crystals on few femtosecond timescales, paving the way to lightwave electronics. In the spatial domain, recent advances in the real-space interpretation of high-harmonic emission in solids allows imaging the field-free, static, potential of the valence electrons with picometer resolution. The combination of such extreme spatial and temporal resolutions to measure and control strong-field dynamics in solids at the atomic scale is poised to unlock a new frontier of lightwave electronics. Here, we report a strong intensity-dependent anisotropy in the high-harmonic generation from ReS2 that we attribute to angle-dependent interference of currents from the different atoms in the unit cell. Furthermore, we demonstrate how the laser parameters control the relative contribution of these atoms to the high-harmonic emission. Our findings provide an unprecedented atomic perspective on strong-field dynamics in crystals, revealing key factors to consider in the route towards developing efficient harmonic emitters.

Saturable Lorentz model for fully explicit three-dimensional modeling of nonlinear optics.

Inclusion of the instantaneous Kerr nonlinearity in the FDTD framework leads to implicit equations that have to be solved iteratively. In principle, explicit integration can be achieved with the use of anharmonic oscillator equations, but it tends to be unstable and inappropriate for studying strong-field phenomena like laser filamentation. In this paper, we show that nonlinear susceptibility can be provided instead by a harmonic oscillator driven by a nonlinear force, chosen in a way to reproduce the polarization obtained from the solution of the quantum mechanical two-level equations. The resulting saturable, nonlinearly-driven, harmonic oscillator model reproduces quantitatively the quantum mechanical solutions of harmonic generation in the under-resonant limit, up to the 9th harmonic. Finally, we demonstrate that fully explicit leapfrog integration of the saturable harmonic oscillator is stable, even for the intense laser fields that characterize laser filamentation and high harmonic generation.

Time-resolved x-ray imaging of anisotropic nanoplasma expansion.

A complete time-resolved x-ray imaging experiment of laser heated solid-density hydrogen clusters is modeled by microscopic particle-in-cell simulations that account self-consistently for the microscopic cluster dynamics and electromagnetic wave evolution. A technique is developed to retrieve the anisotropic nanoplasma expansion from the elastic and inelastic x-ray scattering data. Our method takes advantage of the self-similar evolution of the nanoplasma density and enables us to make movies of ultrafast nanoplasma dynamics from pump-probe x-ray imaging experiments.

Femtosecond 240-keV electron pulses from direct laser acceleration in a low-density gas.

We propose a simple laser-driven electron acceleration scheme based on tightly focused radially polarized laser pulses for the production of femtosecond electron bunches with energies in the few-hundreds-of-keV range. In this method, the electrons are accelerated forward in the focal volume by the longitudinal electric field component of the laser pulse. Three-dimensional test-particle and particle-in-cell simulations reveal the feasibility of generating well-collimated electron bunches with an energy spread of 5% and a temporal duration of the order of 1 fs. These results offer a route towards unprecedented time resolution in ultrafast electron diffraction experiments.

Imaging and modeling collagen architecture from the nano to micro scale.

The collagen meshwork plays a central role in the functioning of a range of tissues including cartilage, tendon, arteries, skin, bone and ligament. Because of its importance in function, it is of considerable interest for studying development, disease and regeneration processes. Here, we have used second harmonic generation (SHG) to image human tissues on the hundreds of micron scale, and developed a numerical model to quantitatively interpret the images in terms of the underlying collagen structure on the tens to hundreds of nanometer scale. Focusing on osteoarthritic changes in cartilage, we have demonstrated that this combination of polarized SHG imaging and numerical modeling can estimate fibril diameter, filling fraction, orientation and bundling. This extends SHG microscopy from a qualitative to quantitative imaging technique, providing a label-free and non-destructive platform for characterizing the extracellular matrix that can expand our understanding of the structural mechanisms in disease.

Spin textures in strongly coupled electron spin and magnetic or nuclear spin systems in quantum dots.

Controlling electron spins strongly coupled to magnetic and nuclear spins in solid state systems is an important challenge in the field of spintronics and quantum computation. We show here that electron droplets with no net spin in semiconductor quantum dots strongly coupled with magnetic ion or nuclear spin systems break down at low temperature and form a nontrivial antiferromagnetic spatially ordered spin texture of magnetopolarons. The spatially ordered combined electron-magnetic ion spin texture, associated with spontaneous symmetry breaking in the parity of electronic charge and spin densities and magnetization of magnetic ions, emerges from an ab initio density functional approach to the electronic system coupled with mean-field approximation for the magnetic or nuclear spin system. The predicted phase diagram determines the critical temperature as a function of coupling strength and identifies possible phases of the strongly coupled spin system. The prediction may arrest fluctuations in the spin system and open the way to control, manipulate, and prepare magnetic and nuclear spin ensembles in semiconductor nanostructures.

Attosecond plasma wave dynamics in laser-driven cluster nanoplasmas.

We introduce a microscopic particle-in-cell approach that allows bridging the microscopic and macroscopic realms of laser-driven plasma physics. As a first application, resonantly driven cluster nanoplasmas are investigated. Our analysis reveals an attosecond plasma-wave dynamics in clusters with radii R is approximately equal to 30 nm. The plasma waves are excited by electrons recolliding with the cluster surface and travel toward the center, where they collide and break. In this process, energetic electron hot spots are generated along with highly localized attosecond electric field fluctuations, whose intensity exceeds the driving laser by more than 2 orders of magnitude. The ionization enhancement resulting from both effects generates a strongly nonuniform ion charge distribution. The observed nonlinear plasma-wave phenomena have a profound effect on the ionization dynamics of nanoparticles and offer a route to extreme nanoplasmonic field enhancements.

Multiscale QM/MM molecular dynamics study on the first steps of guanine damage by free hydroxyl radicals in solution.

Understanding the damage of DNA bases from hydrogen abstraction by free OH radicals is of particular importance to understanding the indirect effect of ionizing radiation. Previous studies address the problem with truncated DNA bases as ab initio quantum simulations required to study such electronic-spin-dependent processes are computationally expensive. Here, for the first time, we employ a multiscale and hybrid quantum mechanical-molecular mechanical simulation to study the interaction of OH radicals with a guanine-deoxyribose-phosphate DNA molecular unit in the presence of water, where all of the water molecules and the deoxyribose-phosphate fragment are treated with the simplistic classical molecular mechanical scheme. Our result illustrates that the presence of water strongly alters the hydrogen-abstraction reaction as the hydrogen bonding of OH radicals with water restricts the relative orientation of the OH radicals with respect to the DNA base (here, guanine). This results in an angular anisotropy in the chemical pathway and a lower efficiency in the hydrogen-abstraction mechanisms than previously anticipated for identical systems in vacuum. The method can easily be extended to single- and double-stranded DNA without any appreciable computational cost as these molecular units can be treated in the classical subsystem, as has been demonstrated here.

Reactive molecular dynamics study on the first steps of DNA damage by free hydroxyl radicals.

We employ a large scale molecular simulation based on bond-order ReaxFF to simulate the chemical reaction and study the damage to a large fragment of DNA molecule in the solution by ionizing radiation. We illustrate that the randomly distributed clusters of diatomic OH radicals that are primary products of megavoltage ionizing radiation in water-based systems are the main source of hydrogen abstraction as well as formation of carbonyl and hydroxyl groups in the sugar moiety that create holes in the sugar rings. These holes grow up slowly between DNA bases and DNA backbone, and the damage collectively propagates to a DNA single and double strand break.

DNA-backbone radio resistivity induced by spin blockade effect.

Coherent control of OH-free radicals interacting with the spin-triplet state of a DNA molecule is investigated. A model Hamiltonian for molecular spin singlet-triplet resonance is developed. We illustrate that the spin-triplet state in DNA molecules can be efficiently populated, as the spin-injection rate can be tuned to be orders of magnitudes greater than the decay rate due to small spin-orbit coupling in organic molecules. Owing to the nano-second life-time of OH free radicals, a non-equilibrium free energy barrier induced by the injected spin triplet state that lasts approximately longer than one-micro second in room temperature can efficiently block the initial Hydrogen abstraction and DNA damage. For a direct demonstration of the spin-blockade effect, a molecular simulation based on an ab-initio Car-Parrinello molecular dynamics is deployed.

Multielectron correlation in high-harmonic generation: a 2D model analysis.

We analyze the role of multielectron dynamics in high-harmonic generation spectroscopy, using an example of a two-electron system. We identify and systematically quantify the importance of correlation and exchange effects. One of the main sources for correlation is identified to be the polarization of the ion by the recombining continuum electron. This effect, which plays an important qualitative and quantitative role, seriously undermines the validity of the standard approaches to high-harmonic generation, which ignore the contribution of excited ionic states to the radiative recombination of the continuum electron.

High harmonic generation and molecular orbital tomography in multielectron systems.

High harmonic radiation is produced when atoms or molecules are ionized by an intense femtosecond laser pulse. The radiated spectrum has been shown experimentally to contain information on the electronic structure of the molecule, which can be interpreted as an image of a single molecular orbital. Previous theory for high harmonic generation has been limited to the single-active-electron approximation. Utilizing semisudden approximation, the authors develop a theory of the recombination step in high harmonic generation and tomographic reconstruction in multielectron systems, taking into account electron spin statistics and electron-electron correlations within the parent molecule and the ion. They show that the resulting corrections significantly modify the theoretical predictions, and bring them in a better agreement with experiment. They further show that exchange contributions to harmonic radiation can be used to extract additional information on the electronic wave function.

Highly charged ions from laser-cluster interactions: local-field-enhanced impact ionization and frustrated electron-ion recombination.

Our molecular dynamics analysis of Xe_{147-5083} clusters identifies two mechanisms that contribute to the yet unexplained observation of extremely highly charged ions in intense laser cluster experiments. First, electron impact ionization is enhanced by the local cluster electric field, increasing the highest charge states by up to 40%; a corresponding theoretical method is developed. Second, electron-ion recombination after the laser pulse is frustrated by acceleration electric fields typically used in ion detectors. This increases the highest charge states by up to 90%, as compared to the usual assumption of total recombination of all cluster-bound electrons. Both effects together augment the highest charge states by up to 120%, in reasonable agreement with experiments.

High harmonic generation and molecular orbital tomography in multielectron systems: beyond the single active electron approximation.

It was recently shown that the highest molecular orbital of N2 could be reconstructed from a series of high harmonic measurements. Existing theories of high harmonic generation and orbital tomographic imaging are based on the single active electron approximation that ignores essential quantum mechanical properties such as the indistinguishability of identical particles and the Pauli exclusion principle. We show that, when fully antisymmetrized multielectron wave functions and electronic relaxation in the cation are considered, molecular orbital tomography records the image of the Dyson orbital plus exchange contributions from inner shells. The mixing of contributions from more than one molecular orbital gives access to additional wave function information. By utilizing the exchange term, harmonic emission from a closed-shell 4-electron system can be interpreted as a complete Hartree-Fock wave function.

Theory of tunnel ionization in complex systems.

A quasianalytical theory of tunnel ionization is developed that is applicable to general complex systems, such as large molecules. Our analysis reveals strong deviations from conventional tunnel ionization theories, dependent upon the system's geometry, angular momentum, and polarizability. A comparison of our theory with recent C(60) ionization experiments yields reasonable agreement.

Microscopic analysis of large-cluster explosion in intense laser fields.

We present a three dimensional microscopic particle in cell code. The code models nanoplasmas in intense laser fields, taking account of all relevant microscopic interactions. Our simulation reveals the physical processes determining the laser induced explosion of large clusters with several 10,000 atoms.

How to use lasers for imaging attosecond dynamics of nuclear processes.

We identify a laser configuration in which attosecond electron wave packets are ionized, accelerated to multi-MeV energies, and refocused onto their parent ion. Magnetic focusing of the electron wave packet results in return currents comparable with large scale accelerator facilities. This technique opens an avenue towards imaging attosecond dynamics of nuclear processes.

Quantum theory of attosecond XUV pulse measurement by laser dressed photoionization.

The first reported measurements of single attosecond pulses use laser dressed single-photon extreme ultraviolet (XUV) ionization of gas atoms. The determination of XUV pulse duration from the electron spectrum is based on a classical theory. Although classical models are known to give a qualitatively correct description of strong laser atom interaction, the validity must be scrutinized by a quantum-mechanical analysis. We establish a theoretical framework for the accurate temporal characterization of attosecond XUV pulses. Our analysis reveals an improved scheme that allows for direct experimental discrimination between single and multiple attosecond pulses.

Numerical characterization of high harmonic attosecond pulses.

A numerical simulation of attosecond harmonic pulse generation in a three-dimensional field-ionizing gas is presented. Calculated harmonic efficiencies quantitatively reproduce experimental findings. This allows a quantitative characterization of attosecond pulse generation revealing information currently not accessible by experiment. The rapid phase variation and spatiotemporal distortions of harmonics are smaller than anticipated, allowing focusing of 30-nm, 750-as pulses to intensities in excess of 10(13) W/cm(2). Feasibility of such pulses brings novel applications such as extreme ultraviolet nonlinear optics and attosecond pump probe spectroscopy within reach.