Search Results
Regulatory impact of the C-terminal tail on charge transfer pathways in drosophila cryptochrome
Interconnected transcriptional and translational feedback loops are at the core of the molecular mechanism of the circadian clock. Such feedback loops are synchronized to external light entrainment by the blue light photoreceptor cryptochrome (CRY) that undergoes conformational changes upon light absorption by an unknown photoexcitation mechanism. Light-induced charge transfer (CT) reactions in Drosophila CRY (dCRY) are investigated by state-of-the-art simulations that reveal a complex, multi-redox site nature of CT dynamics on the microscopic level. The simulations consider redox-active chromophores of the tryptophan triad (Trp triad) and further account for pathways mediated by W314 and W422 residues proximate to the C-terminal tail (CTT), thus avoiding a pre-bias to specific W-mediated CT pathways. The conducted dissipative quantum dynamics simulations employ microscopically derived model Hamiltonians and display complex and ultrafast CT dynamics on the picosecond timescale, subtly balanced by the electrostatic environment of dCRY. In silicio point mutations provide a microscopic basis for rationalizing particular CT directionality and demonstrate the degree of electrostatic control realized by a discrete set of charged amino acid residues. The predicted participation of CT states in proximity to the CTT relates the directionality of CT reactions to the spatial vicinity of a linear interaction motif. The results stress the importance of CTT directional charge transfer in addition to charge transfer via the Trp triad and call for the use of full-length CRY models including the interactions of photolyase homology region (PHR) and CTT domains. © 2020 by the authors. Licensee MDPI, Basel, Switzerland.
Element-specific magnetization dynamics of complex magnetic systems probed by ultrafast magneto-optical spectroscopy
The vision to manipulate and control magnetism with light is driven on the one hand by fundamental questions of direct and indirect photon-spin interactions, and on the other hand by the necessity to cope with ever growing data volumes, requiring radically new approaches on how to write, read and process information. Here, we present two complementary experimental geometries to access the element-specific magnetization dynamics of complex magnetic systems via ultrafast magneto-optical spectroscopy in the extreme ultraviolet spectral range. First, we employ linearly polarized radiation of a free electron laser facility to demonstrate decoupled dynamics of the two sublattices of an FeGd alloy, a prerequisite for all-optical magnetization switching. Second, we use circularly polarized radiation generated in a laboratory-based high harmonic generation setup to show optical inter-site spin transfer in a CoPt alloy, a mechanism which only very recently has been predicted to mediate ultrafast metamagnetic phase transitions. © 2020 by the authors. Licensee MDPI, Basel, Switzerland.
Ellipticity of High-Order Harmonics Generated by Aligned Homonuclear Diatomic Molecules Exposed to an Orthogonal Two-Color Laser Field
We investigate emission rate and ellipticity of high-order harmonics generated exposing a homonuclear diatomic molecule, aligned in the laser-field polarization plane, to a strong orthogonally polarized two-color (OTC) laser field. The linearly polarized OTC-field components have frequencies r? and s?, where r and s are integers. Using the molecular strong-field approximation with dressed initial state and undressed final state, we calculate the harmonic emission rate and harmonic ellipticity for frequency ratios 1:2 and 1:3. The obtained quantities depend strongly on the relative phase between the laser-field components. We show that with the OTC field it is possible to generate elliptically polarized high-energy harmonics with high emission rate. To estimate the relative phase for which the emission rate is maximal we use the simple man’s model. In the harmonic spectra as a function of the molecular orientation there are two types of minima, one connected with the symmetry of the molecular orbital and the other one due to destructive interference between different contributions to the recombination matrix element, where we take into account that the electron can be ionized and recombine at the same or different atomic centers. We derive a condition for the interference minima. These minima are blurred in the OTC field except in the cases where the highest occupied molecular orbital is modeled using only s or only p orbitals in the linear combination of the atomic orbitals. This allows us to use the interference minima to assess which atomic orbitals are dominant in a particular molecular orbital. Finally, we show that the harmonic ellipticity, presented in false colors in the molecular-orientation angle vs. harmonic-order plane, can be large in particular regions of this plane. These regions are bounded by the curves determined by the condition that the harmonic ellipticity is approximately zero, which is determined by the minima of the T-matrix contributions parallel and perpendicular to the fundamental component of the OTC field. © 2020 by the authors. Licensee MDPI, Basel, Switzerland.
Quantum-Optical Spectrometry in Relativistic Laser-Plasma Interactions Using the High-Harmonic Generation Process: A Proposal
Quantum-optical spectrometry is a recently developed shot-to-shot photon correlation-based method, namely using a quantum spectrometer (QS), that has been used to reveal the quantum optical nature of intense laser–matter interactions and connect the research domains of quantum optics (QO) and strong laser-field physics (SLFP). The method provides the probability of absorbing photons from a driving laser field towards the generation of a strong laser–field interaction product, such as high-order harmonics. In this case, the harmonic spectrum is reflected in the photon number distribution of the infrared (IR) driving field after its interaction with the high harmonic generation medium. The method was implemented in non-relativistic interactions using high harmonics produced by the interaction of strong laser pulses with atoms and semiconductors. Very recently, it was used for the generation of non-classical light states in intense laser–atom interaction, building the basis for studies of quantum electrodynamics in strong laser-field physics and the development of a new class of non-classical light sources for applications in quantum technology. Here, after a brief introduction of the QS method, we will discuss how the QS can be applied in relativistic laser–plasma interactions and become the driving factor for initiating investigations on relativistic quantum electrodynamics.
Ultrashort vortex pulses with controlled spectral gouy rotation
Recently, the spatio-spectral propagation dynamic of ultrashort-pulsed vortex beams was demonstrated by 2D mapping of spectral moments. The rotation of characteristic anomalies, so-called "spectral eyes", was explained by wavelength-dependent Gouy phase shift. Controlling of this spectral rotation is essential for specific applications, e.g., communication and processing. Here, we report on advanced concepts for spectral rotational control and related first-proof-of-principle experiments. The speed of rotation of spectral eyes during propagation is shown to be essentially determined by angular and spectral parameters. The performance of fixed diffractive optical elements (DOE) and programmable liquid-crystal-on silicon spatial light modulators (LCoS-SLMs) that act as spiral phase gratings (SPG) or spiral phase plates (SPP) is compared. The approach is extended to radially chirped SPGs inducing axially variable angular velocity. The generation of time-dependent orbital angular momentum (self-torque) by superimposing multiple vortex pulses is proposed. © 2020 by the authors.
Symmetries and Selection Rules of the Spectra of Photoelectrons and High-Order Harmonics Generated by Field-Driven Atoms and Molecules
Using the strong-field approximation we systematically investigate the selection rules for high-order harmonic generation and the symmetry properties of the angle-resolved photoelectron spectra for various atomic and molecular targets exposed to one-component and two-component laser fields. These include bicircular fields and orthogonally polarized two-color fields. The selection rules are derived directly from the dynamical symmetries of the driving field. Alternatively, we demonstrate that they can be obtained using the conservation of the projection of the total angular momentum on the quantization axis. We discuss how the harmonic spectra of atomic targets depend on the type of the ground state or, for molecular targets, on the pertinent molecular orbital. In addition, we briefly discuss some properties of the high-order harmonic spectra generated by a few-cycle laser field. The symmetry properties of the angle-resolved photoelectron momentum distribution are also determined by the dynamical symmetry of the driving field. We consider the first two terms in a Born series expansion of the T matrix, which describe the direct and the rescattered electrons. Dynamical symmetries involving time translation generate rotational symmetries obeyed by both terms. However, those that involve time reversal generate reflection symmetries that are only observed by the direct electrons. Finally, we explain how the symmetry properties, imposed by the dynamical symmetry of the driving field, are altered for molecular targets.
On the Mixed Gas Behavior of Organosilica Membranes Fabricated by Plasma-Enhanced Chemical Vapor Deposition (PECVD)
Selective, nanometer-thin organosilica layers created by plasma-enhanced chemical vapor deposition (PECVD) exhibit selective gas permeation behavior. Despite their promising pure gas performance, published data with regard to mixed gas behavior are still severely lacking. This study endeavors to close this gap by investigating the pure and mixed gas behavior depending on temperatures from 0 °C to 60 °C for four gases (helium, methane, carbon dioxide, and nitrogen) and water vapor. For the two permanent gases, helium and methane, the studied organosilica membrane shows a substantial increase in selectivity from αHe/CH4 = 9 at 0 °C to αHe/CH4 = 40 at 60 °C for pure as well as mixed gases with helium permeance of up to 300 GPU. In contrast, a condensable gas such as CO2 leads to a decrease in selectivity and an increase in permeance compared to its pure gas performance. When water vapor is present in the feed gas, the organosilica membrane shows even stronger deviations from pure gas behavior with a permeance loss of about 60 % accompanied by an increase in ideal selectivity αHe/CO2 from 8 to 13. All in all, the studied organosilica membrane shows very promising results for mixed gases. Especially for elevated temperatures, there is a high potential for separation by size exclusion.
Production of Natural Pigments by Penicillium brevicompactum Using Agro-Industrial Byproducts
The demand for natural pigments for industrial applications has significantly increased. Penicillium brevicompactum was recently reported as a promising pigments producer using submerged fermentation and a synthetic culture medium containing lactose. In this work, pigment production by P. brevicompactum was studied under different fermentation conditions, namely, submerged fermentation with free (SmF) and immobilized mycelium (SmFi), and solid-state fermentation (SSF). The potential of culture media composed of agro-industrial byproducts (cheese-whey (CW) and corn steep liquor (CSL)) was investigated for the first time as low-cost alternatives to pigment production by P. brevicompactum. The fungus showed great adaptability to the different culture media and types of fermentation, being able to synthesize pigments under all the tested conditions. A culture medium composed of 34.6 g/L of CW and 8 g/L of CSL proved to be the most suitable alternative to the synthetic medium, especially under SmF and SmFi. Our data also show that different mixtures of pigments (yellow, orange, and red) can be produced depending on the medium composition and the type of fermentation. Additionally, the immobilization and reuse of biomass to produce pigments by P. brevicompactum were demonstrated for the first time, suggesting the possibility of operating under repeated batch mode at an industrial scale.