212 research outputs found
One-Electron Ionization of Multielectron Systems in Strong Nonresonant Laser Fields
We present a novel approach to calculating strong field ionization dynamics
of multielectron molecular targets. Adopting a multielectron wavefunction
ansatz based on field-free ab initio neutral and ionic multielectron states, a
set of coupled time-dependent single-particle Schroedinger equations describing
the neutral amplitude and continuum electron are constructed. These equations,
amenable to direct numerical solution or further analytical treatment, allow
one to study multielectron effects during strong field ionization, recollision,
and high harmonic generation. We apply the method to strong field ionization of
CO_2, and suggest the importance of intermediate core excitation to explain
previous failure of analytical models to reproduce experimental ionization
yields for this molecule.Comment: 25 pages, 6 figure
Alignment dependent enhancement of the photo-electron cutoff for multi-photon ionization of molecules
The multiphoton ionization rate of molecules depends on the alignment of the
molecular axis with respect to the ionizing laser polarization. By studying
molecular frame photo-electron angular distributions from N, O and
benzene, we illustrate how the angle-dependent ionization rate affects the
photo-electron cutoff energy. We find alignment can enhance the high energy
cutoff of the photo-electron spectrum when probing along a nodal plane or when
ionization is otherwise suppressed. This is supported by calculations using a
tunneling model with a single ion state.Comment: 4 pages, 4 figure
Mechanisms of two-color laser-induced field-free molecular orientation
Two mechanisms of two-color (\omega + 2\omega) laser-induced field-free
molecular orientation, based on the hyperpolarizability and ionization
depletion, are explored and compared. The CO molecule is used as a
computational example. While the hyperpolarizability mechanism generates small
amounts of orientation at intensities below the ionization threshold,
ionization depletion quickly becomes the dominant mechanism as soon as ionizing
intensities are reached. Only the ionization mechanism leads to substantial
orientation (e.g. on the order of || > 0.1). For intensities typical
of laser-induced molecular alignment and orientation experiments, the two
mechanism lead to robust, characteristic timings of the field-free orientation
wave-packet revivals relative to the the alignment revivals and the revival
time. The revival timings can be used to detect the active orientation
mechanism experimentally
Potential for ultrafast dynamic chemical imaging with few-cycle infrared lasers
We studied the photoelectron spectra generated by an intense few-cycle
infrared laser pulse. By focusing on the angular distributions of the back
rescattered high energy photoelectrons, we show that accurate differential
elastic scattering cross sections of the target ion by free electrons can be
extracted. Since the incident direction and the energy of the free electrons
can be easily changed by manipulating the laser's polarization, intensity, and
wavelength, these extracted elastic scattering cross sections, in combination
with more advanced inversion algorithms, may be used to reconstruct the
effective single-scattering potential of the molecule, thus opening up the
possibility of using few-cycle infrared lasers as powerful table-top tools for
imaging chemical and biological transformations, with the desired unprecedented
temporal and spatial resolutions.Comment: 16 pages, 6 figure
Oriented rotational wave-packet dynamics studies via high harmonic generation
We produce oriented rotational wave packets in CO and measure their
characteristics via high harmonic generation. The wavepacket is created using
an intense, femtosecond laser pulse and its second harmonic. A delayed 800 nm
pulse probes the wave packet, generating even-order high harmonics that arise
from the broken symmetry induced by the orientation dynamics. The even-order
harmonic radiation that we measure appears on a zero background, enabling us to
accurately follow the temporal evolution of the wave packet. Our measurements
reveal that, for the conditions optimum for harmonic generation, the
orientation is produced by preferential ionization which depletes the sample of
molecules of one orientation
Anomalous transport of a tracer on percolating clusters
We investigate the dynamics of a single tracer exploring a course of fixed
obstacles in the vicinity of the percolation transition for particles confined
to the infinite cluster. The mean-square displacement displays anomalous
transport, which extends to infinite times precisely at the critical obstacle
density. The slowing down of the diffusion coefficient exhibits power-law
behavior for densities close to the critical point and we show that the
mean-square displacement fulfills a scaling hypothesis. Furthermore, we
calculate the dynamic conductivity as response to an alternating electric
field. Last, we discuss the non-gaussian parameter as an indicator for
heterogeneous dynamics
Identification and characterization of Cercospora beticola necrosis-inducing effector CbNip1
Cercospora beticola is a hemibiotrophic fungus that causes cercospora leaf spot disease of sugar beet (Beta vulgaris). After an initial symptomless biotrophic phase of colonization, necrotic lesions appear on host leaves as the fungus switches to a necrotrophic lifestyle. The phytotoxic secondary metabolite cercosporin has been shown to facilitate fungal virulence for several Cercospora spp. However, because cercosporin production and subsequent cercosporin‐initiated formation of reactive oxygen species is light‐dependent, cell death evocation by this toxin is only fully ensured during a period of light. Here, we report the discovery of the effector protein CbNip1 secreted by C. beticola that causes enhanced necrosis in the absence of light and, therefore, may complement light‐dependent necrosis formation by cercosporin. Infiltration of CbNip1 protein into sugar beet leaves revealed that darkness is essential for full CbNip1‐triggered necrosis, as light exposure delayed CbNip1‐triggered host cell death. Gene expression analysis during host infection shows that CbNip1 expression is correlated with symptom development in planta. Targeted gene replacement of CbNip1 leads to a significant reduction in virulence, indicating the importance of CbNip1 during colonization. Analysis of 89 C. beticola genomes revealed that CbNip1 resides in a region that recently underwent a selective sweep, suggesting selection pressure exists to maintain a beneficial variant of the gene. Taken together, CbNip1 is a crucial effector during the C. beticola–sugar beet disease process
Local Anisotropy of Fluids using Minkowski Tensors
Statistics of the free volume available to individual particles have
previously been studied for simple and complex fluids, granular matter,
amorphous solids, and structural glasses. Minkowski tensors provide a set of
shape measures that are based on strong mathematical theorems and easily
computed for polygonal and polyhedral bodies such as free volume cells (Voronoi
cells). They characterize the local structure beyond the two-point correlation
function and are suitable to define indices of
local anisotropy. Here, we analyze the statistics of Minkowski tensors for
configurations of simple liquid models, including the ideal gas (Poisson point
process), the hard disks and hard spheres ensemble, and the Lennard-Jones
fluid. We show that Minkowski tensors provide a robust characterization of
local anisotropy, which ranges from for vapor
phases to for ordered solids. We find that for fluids,
local anisotropy decreases monotonously with increasing free volume and
randomness of particle positions. Furthermore, the local anisotropy indices
are sensitive to structural transitions in these simple
fluids, as has been previously shown in granular systems for the transition
from loose to jammed bead packs
Terahertz control of air lasing
The coherent emission from ionized nitrogen molecules is of interest for remote sensing and astronomical applications. To initiate the lasing process, we used an intense ultrashort near-infrared (NIR) pulse overlapped with a terahertz (THz) single-cycle pulse. We observed that coherent emission could be seeded and modulated by the amplitude of the THz field, which is the result of a combined effective second-order nonlinear polarization and the nonlinear effects induced by the NIR pump. Our results shed light on the role of intense transient fields in the coherent emission from photoexcited gas molecules
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