Condensed Matter Systems Exposed to Radiation: Multiscale Theory, Simulations, and Experiment

Chemical Reviews, Год журнала: 2024, Номер 124(13), С. 8014 - 8129

Опубликована: Июнь 6, 2024

This roadmap reviews the new, highly interdisciplinary research field studying behavior of condensed matter systems exposed to radiation.The Review highlights several recent advances in and provides a for development over next decade.Condensed radiation can be inorganic, organic, or biological, finite infinite, composed different molecular species materials, exist phases, operate under thermodynamic conditions.Many key phenomena related irradiated are very similar understood based on same fundamental theoretical principles computational approaches.The multiscale nature such requires quantitative description radiation-induced effects occurring at spatial temporal scales, ranging from atomic macroscopic, interlinks between descriptions.The similarity their manifestation origins necessarily bring together disciplines, as physics, chemistry, biology, materials science, nanoscience, biomedical research, demonstrating numerous commonalities them.This is relevant many novel emerging technologies medical applications.

Язык: Английский

---

Full visible range two-dimensional electronic spectroscopy with high time resolution

Optics Express, Год журнала: 2023, Номер 32(1), С. 835 - 835

Опубликована: Дек. 15, 2023

Two-dimensional electronic spectroscopy (2DES) is a powerful method to study coherent and incoherent interactions dynamics in complex quantum systems by correlating excitation detection energies nonlinear experiment. Such can be probed with time resolution limited only the duration of employed laser pulses spectral range defined pulse spectrum. In blue (<500 nm), generation sufficiently broadband ultrashort durations 10 fs or less has been challenging so far. Here, we present 2DES setup based on hollow-core fiber supercontinuum covering full visible (400-700 nm). Pulse compression via custom-made chirped mirrors yields <10 fs. The broad coverage, particular extension spectra into range, unlocks new possibilities for investigations blue-light absorbing multichromophoric compounds, as demonstrated measurement chlorophyll a.

Язык: Английский

---

Magnetic orientation in juvenile Atlantic herring ( Clupea harengus ) could involve cryptochrome 4 as a potential magnetoreceptor

Journal of The Royal Society Interface, Год журнала: 2024, Номер 21(215)

Опубликована: Июнь 1, 2024

The Earth’s magnetic field can provide reliable directional information, allowing migrating animals to orient themselves using a compass or estimate their position relative target map-based orientation. Here we show for the first time that young, inexperienced herring ( Clupea harengus , Ch) have when they migrate hundreds of kilometres feeding grounds. In birds, such as European robin Erithacus rubecula ), radical pair-based magnetoreception involving cryptochrome 4 (ErCRY4) was demonstrated; molecular basis in fish is still elusive. We cry4 expression eye upregulated during migratory season, but not before, indicating possible use migration. amino acid structure ChCRY4 shows four tryptophans and flavin adenine dinucleotide-binding site, prerequisite receptor. Using homology modelling, successfully reconstructed herring, DrCRY4 zebrafish Danio rerio ) StCRY4 brown trout Salmo trutta showed ChCRY4, ErCRY4a, StCRY4, exhibit very comparable dynamic behaviour. electron transfer could take place similar way ErCRY4a. combined behavioural, transcriptomic simulation experiments evidence CRY4 act magnetoreceptor Atlantic herring.

Язык: Английский

---

Importance of Polarizable Embedding for Absorption Spectrum Calculations of Arabidopsis thaliana Cryptochrome 1

The Journal of Physical Chemistry B, Год журнала: 2024, Номер 128(26), С. 6283 - 6290

Опубликована: Июнь 24, 2024

Cryptochromes are essential flavoproteins for circadian rhythms and avian magnetoreception. Flavin adenine dinucleotide (FAD), a chromophore within cryptochromes, absorbs blue light, initiating electron transfer processes that lead to biological signaling cascade. A key step in this cascade is the formation of FAD semiquinone radical (FADH

Язык: Английский

---

European Robin Cryptochrome-4a Associates with Lipid Bilayers in an Ordered Manner, Fulfilling a Molecular-Level Condition for Magnetoreception

ACS Chemical Biology, Год журнала: 2025, Номер unknown

Опубликована: Фев. 21, 2025

Since the middle of 20th century, long-distance avian migration has been known to rely partly on geomagnetic field. However, underlying sensory mechanism is still not fully understood. Cryptochrome-4a (ErCry4a), found in European robin (Erithacus rubecula), a night-migratory songbird, suggested be magnetic molecule. It sensitive external fields via so-called radical-pair mechanism. ErCry4a primarily located outer segments double-cone photoreceptor cells eye, which contain stacked and highly ordered membranes that could facilitate anisotropic attachment needed for compass sensing. Here, we investigate possible interactions with model membrane mimics lipid composition vertebrate using experimental computational approaches. Experimental results show controlled by physical state molecules (average area per lipid) leaflet bilayer. Furthermore, polarization modulation infrared reflection absorption spectroscopy allowed us determine conformation, motional freedom, average orientation α-helices membrane-associated state. Atomistic molecular dynamics studies supported results. A ∼ 1000 kcal mol–1 decrease interaction energy as result binding was determined compared cases where no protein occurred. At level, seems involve negatively charged carboxylate groups phosphoserine lipids C-terminal residues ErCry4a. Our study reveals potential direct discusses how this an essential step propagate signal further thus fulfill role magnetoreceptor.

Язык: Английский

---

Extremely low frequency magnetic field distracts zebrafish from a visual cognitive task

Scientific Reports, Год журнала: 2025, Номер 15(1)

Опубликована: Март 12, 2025

Abstract Electromagnetic fields emitted from overhead power lines and subsea cables are widely regarded to be a disruptive factor for animals using the natural magnetic field as orientation cue guiding their directed movements. However, it is not known if anthropogenic electromagnetic also have potential disturb attending information other sensory modalities. To find out, we trained adult zebrafish ( Danio rerio ) individually perform avoidance behavior in response visual signal (green LED light spot), which exposure group was presented simultaneously with sinusoidally changing (0.3 Hz, A: 0.015 mT, B: 0.06 mT). Despite salience of signal, both sufficient necessary elicit conditioned responses, mT condition had negative impact on learning performance behavior. This suggests that extremely low frequency technical Earth strength amplitude can act cross-modal distractor diverts attention away environmentally relevant cues based nonmagnetic Our research highlights need study role pollutant beyond scope

Язык: Английский

---

Electron transfer engineering of artificially designed cell factory for complete biosynthesis of steroids

Nature Communications, Год журнала: 2025, Номер 16(1)

Опубликована: Апрель 21, 2025

Biosynthesis of steroids by artificially designed cell factories often involves numerous nicotinamide adenine dinucleotide phosphate (NADPH)-dependent enzymes that mediate electron transfer reactions. However, the unclear mechanisms from regeneration to final delivery NADPH-dependent active centers limit systematically engineering improve production. Here, we elucidate for engineer Saccharomyces cerevisiae, including step-by-step residues 7-Dehydrocholesterol reductase (DHCR7) and P450 sterol side chain cleaving enzyme (P450scc), components directing carbon flux, NADPH pathways, high-level production cholesterol (1.78 g/L) pregnenolone (0.83 g/L). The (ETE) process makes chains shorter more stable which significantly accelerates deprotonation proton coupled process. This study underscores significance ETE strategies in biosynthesis expands synthetic biology approaches.

Язык: Английский

---

Linear free energy relationship between reduction potential and photoreduction rate: studies on Drosophila cryptochrome

FEBS Journal, Год журнала: 2025, Номер unknown

Опубликована: Май 15, 2025

Cryptochromes are flavin adenine dinucleotide (FAD)‐containing blue‐light photoreceptors involved in the regulation of circadian clock and may play a role magnetic field sensing. The photochemistry cryptochromes is based on isoalloxazine moiety, which can be photoreduced subsequently reoxidized by an electron acceptor such as oxygen, corresponding to photo‐switch between dark signaling state. We replaced FAD cofactor Drosophila cryptochrome with series cofactors modified at 7α or 8α positions, order modulate chemical properties acceptor. These modifications were shown alter kinetics light‐dependent reactions. Notably, 7‐halogenated FADs form state more than six times faster compared natural cofactor. positive reduction potentials well increased intersystem crossing rates due heavy halogen atoms identified reasons for altered photochemistry. Both parameters show linear dependence reaction kinetics, according Hammett relationship. With this knowledge, defined way without changing its amino acid sequence.

Язык: Английский

---

Capturing structural intermediates in an animal-like cryptochrome photoreceptor by time-resolved crystallography

Science Advances, Год журнала: 2025, Номер 11(20)

Опубликована: Май 16, 2025

Animal-like cryptochromes are photoreceptors that control circadian rhythm and signaling in many eukaryotes. Transient photoreduction of the cryptochrome flavin chromophore initiated via a poorly understood mechanism. By serial femtosecond crystallography (SFX), we show mechanism Chlamydomonas reinhardtii involves three loci [carboxyl-terminal region, transient protonation pathway, adenine dinucleotide (FAD)–binding site] acting unison to accomplish effects: radical pair stabilization, FAD radical, formation state. Using 19 time-resolved SFX snapshots between 10 nanoseconds 233 milliseconds, found light-driven •– /tyrosyl-373 (RP) primes α22 unfolding. Electron transfer–dependent aspartate-321 by tyrosine-373 is epicenter unfolding disrupting salt bridges photolyase homology region. Before helix unfolding, another pathway opens transiently for RP stabilization. This link conformational changes provides structural basis animal-like cryptochromes.

Язык: Английский

---

Decrypting the Nonadiabatic Photoinduced Electron Transfer Mechanism in Light-Sensing Cryptochrome

ACS Central Science, Год журнала: 2025, Номер unknown

Опубликована: Май 30, 2025

Язык: Английский

---