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Analogous electrical networks were previously derived from the Euler–Bernoulli and Kirchhoff–Love theories to represent beams and plates, respectively, for use in multimodal structural vibration damping. However, these networks do not account for shear deformations or rotary inertia, which can result in suboptimal vibration damping performance when used on moderately thick beams and plates. In this paper, we investigate the incorporation of shear deformation and rotary inertia using Timoshenko–Ehrenfest beam theory and Mindlin–Reissner plate theory to develop improved electrical networks that can more accurately represent thick beams and plates. Our findings suggest that the inclusion of shear deformation and rotary inertia can significantly improve the frequency coherence of the electrical networks and multimodal vibration damping for thicker structures. The electrical analogs presented here are of use for various applications, especially to conveniently design complex circuit topologies in fields spanning from vibration attenuation to energy harvesting. [ABSTRACT FROM AUTHOR]

Maintaining lipid asymmetry across membrane leaflets is critical for functions like vesicular traffic and organelle homeostasis. However, a lack of molecular‐level understanding of the mechanisms underlying membrane fission and fusion processes in synthetic systems precludes their development as artificial analogs. Here, we report asymmetry induction of a bilayer membrane formed by an extended π‐conjugated molecule with oxyalkylene side chains bearing terminal tertiary amine moieties (BA1) in water. Autogenous protonation of the tertiary amines in the periphery of the bilayer by water induces anisotropic curvature, resulting in membrane fission to form vesicles and can be monitored using time‐dependent spectroscopy and microscopy. Interestingly, upon loss of the induced asymmetry by extensive protonation using an organic acid restored bilayer membrane. The mechanism leading to the compositional asymmetry in the leaflet and curvature induction in the membrane is validated by density functional theory (DFT) calculations. Studies extended to control molecules having changes in hydrophilic (BA2) and hydrophobic (BA3) segments provide insight into the delicate nature of molecular scale interactions in the dynamic transformation of supramolecular structures. The synergic effect of hydrophobic interaction and the hydrated state of BA1 aggregates provide dynamicity and unusual stability. Our study unveils mechanistic insight into the dynamic transformation of bilayer membranes into vesicles. [ABSTRACT FROM AUTHOR]

Organic piezochromic materials that manifest pressure‐stimuli‐responses are important in various fields such as data storage and anticounterfeiting. The manipulation of piezofluorochromic behaviors for these materials is promising but remains a great challenge. Herein, a non‐luminous components regulated strategy is developed and organic molecular cages (OMCs), a burgeoning class of crystalline organic materials with structural dynamics, are first explored for the design of piezofluorochromic materials with tunable luminescence. A series of OMCs based on aggregation‐induced emission (AIE) chromophores, termed Cage 1–3, are synthesized and their piezofluorochromic behaviors are investigated by diamond anvil cell technique. Due to the sufficient voids between its flexible chromophores offered by the OMC structure, Cage 1 exhibits thermofluorochromic and piezofluorochromic properties. Moreover, the piezofluorochromic performance of this OMC could be further promoted by replacing its non‐luminous components with improved flexibilities, and a remarkable luminescence peak shift by 150 nm together with a response sensitivity of 13.8 nm GPa−1 was achieved upon hydrostatic compression. The cage structure plays a vital role in facilitating efficient and reversible piezofluorochromic behaviors. This study has shed light on the rational design and exploitation of OMCs as an exceptional platform to accomplish customizable piezofluorochromic behaviors and enlarge their potential applications in pressure‐based luminescence. [ABSTRACT FROM AUTHOR]

Maintaining lipid asymmetry across membrane leaflets is critical for functions like vesicular traffic and organelle homeostasis. However, a lack of molecular‐level understanding of the mechanisms underlying membrane fission and fusion processes in synthetic systems precludes their development as artificial analogs. Here, we report asymmetry induction of a bilayer membrane formed by an extended π‐conjugated molecule with oxyalkylene side chains bearing terminal tertiary amine moieties (BA1) in water. Autogenous protonation of the tertiary amines in the periphery of the bilayer by water induces anisotropic curvature, resulting in membrane fission to form vesicles and can be monitored using time‐dependent spectroscopy and microscopy. Interestingly, upon loss of the induced asymmetry by extensive protonation using an organic acid restored bilayer membrane. The mechanism leading to the compositional asymmetry in the leaflet and curvature induction in the membrane is validated by density functional theory (DFT) calculations. Studies extended to control molecules having changes in hydrophilic (BA2) and hydrophobic (BA3) segments provide insight into the delicate nature of molecular scale interactions in the dynamic transformation of supramolecular structures. The synergic effect of hydrophobic interaction and the hydrated state of BA1 aggregates provide dynamicity and unusual stability. Our study unveils mechanistic insight into the dynamic transformation of bilayer membranes into vesicles. [ABSTRACT FROM AUTHOR]

Organic piezochromic materials that manifest pressure‐stimuli‐responses are important in various fields such as data storage and anticounterfeiting. The manipulation of piezofluorochromic behaviors for these materials is promising but remains a great challenge. Herein, a non‐luminous components regulated strategy is developed and organic molecular cages (OMCs), a burgeoning class of crystalline organic materials with structural dynamics, are first explored for the design of piezofluorochromic materials with tunable luminescence. A series of OMCs based on aggregation‐induced emission (AIE) chromophores, termed Cage 1–3, are synthesized and their piezofluorochromic behaviors are investigated by diamond anvil cell technique. Due to the sufficient voids between its flexible chromophores offered by the OMC structure, Cage 1 exhibits thermofluorochromic and piezofluorochromic properties. Moreover, the piezofluorochromic performance of this OMC could be further promoted by replacing its non‐luminous components with improved flexibilities, and a remarkable luminescence peak shift by 150 nm together with a response sensitivity of 13.8 nm GPa−1 was achieved upon hydrostatic compression. The cage structure plays a vital role in facilitating efficient and reversible piezofluorochromic behaviors. This study has shed light on the rational design and exploitation of OMCs as an exceptional platform to accomplish customizable piezofluorochromic behaviors and enlarge their potential applications in pressure‐based luminescence. [ABSTRACT FROM AUTHOR]

Thermally activated delayed fluorescence (TADF) emitters featuring through‐space charge transfer (TSCT) can be excellent candidates for piezochromic luminescent (PCL) materials due to their structural dynamics. Spatial donor‐acceptor (D−A) stacking arrangements enable the modulation of inter‐ and intramolecular D−A interactions, as well as spatial charge transfer states, under varying pressure conditions. Herein, we demonstrate an effective approach toward dynamic reversible full‐color PCL materials with TSCT‐TADF characteristics. Their single crystals exhibit a full‐color‐gamut PCL process spanning a range of 170 nm. Moreover, the TSCT‐TADF‐PCL emitters display a unity photoluminescence quantum yield, and show promising application in X‐ray scintillator imaging. [ABSTRACT FROM AUTHOR]

Thermally activated delayed fluorescence (TADF) emitters featuring through‐space charge transfer (TSCT) can be excellent candidates for piezochromic luminescent (PCL) materials due to their structural dynamics. Spatial donor‐acceptor (D−A) stacking arrangements enable the modulation of inter‐ and intramolecular D−A interactions, as well as spatial charge transfer states, under varying pressure conditions. Herein, we demonstrate an effective approach toward dynamic reversible full‐color PCL materials with TSCT‐TADF characteristics. Their single crystals exhibit a full‐color‐gamut PCL process spanning a range of 170 nm. Moreover, the TSCT‐TADF‐PCL emitters display a unity photoluminescence quantum yield, and show promising application in X‐ray scintillator imaging. [ABSTRACT FROM AUTHOR]

The update of the draft genome assembly of sea urchin, Hemicentrotus pulcherrimus, which is widely studied in East Asia as a model organism of early development, was performed using Oxford nanopore long‐read sequencing. The updated assembly provided ~600‐Mb genome sequences divided into 2,163 contigs with N50 = 516 kb. BUSCO completeness score and transcriptome model mapping ratio (TMMR) of the present assembly were obtained as 96.5% and 77.8%, respectively. These results were more continuous with higher resolution than those by the previous version of H. pulcherrimus draft genome, HpulGenome_v1, where the number of scaffolds = 16,251 with a total of ~100 Mb, N50 = 143 kb, BUSCO completeness score = 86.1%, and TMMR = 55.4%. The obtained genome contained 36,055 gene models that were consistent with those in other echinoderms. Additionally, two tandem repeat sequences of early histone gene locus containing 47 copies and 34 copies of all histone genes, and 185 of the homologous sequences of the interspecifically conserved region of the Ars insulator, ArsInsC, were obtained. These results provide further advance for genome‐wide research of development, gene regulation, and intranuclear structural dynamics of multicellular organisms using H. pulcherrimus. [ABSTRACT FROM AUTHOR]

Layered transition metal oxides are extensively considered as appealing cathode candidates for potassium‐ion batteries (PIBs) due to their abundant raw materials and low cost, but their further implementations are limited by slow dynamics and impoverished structural stability. Herein, a layered composite having a P2 and P3 symbiotic structure is designed and synthesized to realize PIBs with large energy density and long‐term cycling stability. The unique intergrowth of P2 and P3 phases in the obtained layered oxide is plainly characterized by X‐ray diffraction refinement, high‐angle annular dark field and annular bright field‐scanning transmission electron microscopy at atomic resolution, and Fourier transformation images. The synergistic effect of the two phases of this layered P2/P3 composite is well demonstrated in K+ intercalation/extraction process. The as‐prepared layered composite can present a large discharge capacity with the remarkable energy density of 321 Wh kg−1 and also manifest excellent capacity preservation after 600 cycles of K+ uptake/removal. [ABSTRACT FROM AUTHOR]

Layered transition metal oxides are extensively considered as appealing cathode candidates for potassium‐ion batteries (PIBs) due to their abundant raw materials and low cost, but their further implementations are limited by slow dynamics and impoverished structural stability. Herein, a layered composite having a P2 and P3 symbiotic structure is designed and synthesized to realize PIBs with large energy density and long‐term cycling stability. The unique intergrowth of P2 and P3 phases in the obtained layered oxide is plainly characterized by X‐ray diffraction refinement, high‐angle annular dark field and annular bright field‐scanning transmission electron microscopy at atomic resolution, and Fourier transformation images. The synergistic effect of the two phases of this layered P2/P3 composite is well demonstrated in K+ intercalation/extraction process. The as‐prepared layered composite can present a large discharge capacity with the remarkable energy density of 321 Wh kg−1 and also manifest excellent capacity preservation after 600 cycles of K+ uptake/removal. [ABSTRACT FROM AUTHOR]

Eukaryotic DNA replication depends on the primosome – a complex of DNA polymerase alpha (Pol α) and primase – to initiate DNA synthesis by polymerisation of an RNA–DNA primer. Primer synthesis requires the tight coordination of primase and polymerase activities. Recent cryo‐electron microscopy (cryoEM) analyses have elucidated the extensive conformational transitions required for RNA primer handover between primase and Pol α and primer elongation by Pol α. Because of the intrinsic flexibility of the primosome, however, structural information about the initiation of RNA primer synthesis is still lacking. Here, we capture cryoEM snapshots of the priming reaction to reveal the conformational trajectory of the human primosome that brings DNA primase subunits 1 and 2 (PRIM1 and PRIM2, respectively) together, poised for RNA synthesis. Furthermore, we provide experimental evidence for the continuous association of primase subunit PRIM2 with the RNA primer during primer synthesis, and for how both initiation and termination of RNA primer polymerisation are licenced by specific rearrangements of DNA polymerase alpha catalytic subunit (POLA1), the polymerase subunit of Pol α. Our findings fill a critical gap in our understanding of the conformational changes that underpin the synthesis of the RNA primer by the primosome. Together with existing evidence, they provide a complete description of the structural dynamics of the human primosome during DNA replication initiation. [ABSTRACT FROM AUTHOR]

The highly contagious SARS‐CoV‐2 virus, which initiated the COVID‐19 pandemic, has resulted in a significant loss of life worldwide. While vaccines and therapeutics have helped mitigate the impact of SARS‐CoV‐2, worries still persist regarding the emergence of Variants of Concern (VOCs). Additionally, the immunosuppressive effects of SARS‐CoV‐2 and steroid treatments increase susceptibility to complex fungal co–infections (e. g., aspergillosis and candidiasis), complicating treatment and escalating mortality rates. These circumstances highlight the urgent need for novel therapeutics. Thus, this study explores gentisyl alcohol and its derivatives as inhibitors of SARS‐CoV‐2 and fungal pathogens (Aspergillus fumigatus and Candida auris) via in‐silico methodologies. Initial multi–targeted docking simulations revealed that Terrestrol A(10) exhibited highly promising results, displaying the most favourable MolDock‐scores against all targets of interest, particularly against PDB ID 4K90 and 7CR5. The subsequent assessment of Terrestrol A(10) for their druglikeness, ADME, toxicity profiling, bioactivity, and PASS prediction also yielded highly favourable results. Structural dynamics analysis revealed stable yet slightly unfolding complexes, affirming their integrity. DFT studies also demonstrated favourable reactivity of Terrestrol A(10). This investigation identifies Terrestrol A(10) as a highly promising inhibitor against SARS‐CoV‐2 and fungal pathogens, laying the groundwork for in vitro and in vivo validation of its efficacy and clinical utility. [ABSTRACT FROM AUTHOR]

Melatonin (5‐methoxy‐N‐acetyltryptamine) binds with high affinity and specificity to membrane receptors. Several receptor subtypes exist in different species, of which the mammalian MT1 and MT2 receptors are the best‐characterized. They are members of the G protein‐coupled receptor superfamily, preferentially coupling to Gi/o proteins but also to other G proteins in a cell‐context‐depending manner. In this review, experts on melatonin receptors will summarize the current state of the field. We briefly report on the discovery and classification of melatonin receptors, then focus on the molecular structure of human MT1 and MT2 receptors and highlight the importance of molecular simulations to identify new ligands and to understand the structural dynamics of these receptors. We then describe the state‐of‐the‐art of the intracellular signaling pathways activated by melatonin receptors and their complexes. Brief statements on the molecular toolbox available for melatonin receptor studies and future perspectives will round‐up this review. [ABSTRACT FROM AUTHOR]

Rheological analysis of citrus pectin at pH 3 and 7 elucidates its structural dynamics, revealing distinct behaviors influenced by pH. At pH 3, pectin exhibits shear-thinning, with solvent-independent unified rheological profiles identifying three concentration regimes: 0.5%-1.5%, 2%-3%, and 3.5%-4%. These regimes, alongside Cox--Merz superpositions, outline the semi-dilute (c*) and concentrated (c**) transitions at 1.5%-2% and 3%-3.5%, respectively. Moreover, a Morris equation exponent of 0.65 indicates flexible, mobility-restricted macromolecules. Conversely, at pH 7, increased viscosities and Morris plot linearity for p = .1 suggest rigid chain behavior due to electrostatic repulsion among ionized acidic groups. This rigidity leads to concentration-dependent self-assembly structures that diverge from expected unified rheological profiles, a deviation amplified by heating--cooling cycles. This study clarifies the impact of pH on citrus pectin's rheology and emphasizes the intricate relationship between polymeric chain rigidity, self-assembly, and viscosity. By providing a refined understanding of these mechanisms, our findings contribute to the broader field of polysaccharide research, offering insights critical for developing and optimizing pectin-based applications in various industries. [ABSTRACT FROM AUTHOR]

To assess the potential optoelectronic applications of metal‐halide perovskites, it is critical to have a detailed understanding of the nature and dynamics of interactions between carriers and the polar lattices. Here, the electronic and structural dynamics of bismuth‐based perovskite Cs3Bi2I9 are revealed by transient reflectivity and ultrafast electron diffraction. A cross‐examination of these results combined with theoretical analyses allows the identification of the major carrier–phonon coupling mechanism and the associated time scales. It is found that carriers photoinjected into Cs3Bi2I9 form self‐trapped excitons on an ultrafast time scale. However, they retain most of their energy, and their coupling to Fröhlich‐type optical phonons is limited at early times. Instead, the long‐lived excitons exert an electronic stress via deformation potential and develop a prominent, sustaining strain field as coherent acoustic phonons in 10 ps. From sub‐ps to ns and beyond, a similar extent of the atomic displacements is found throughout the different stages of structural distortions, from limited local modulations to a coherent strain field to the Debye–Waller random atomic motions on longer times. The current results suggest the potential use of bismuth‐based perovskites for applications other than photovoltaics to take advantage of the carriers' stronger self‐trapping and long lifetimes. [ABSTRACT FROM AUTHOR]

BACKGROUND: There has been significant interest in pre‐cooked noodles that have a long shelf life and are convenient to cook. However, the thermal processes during preparation, and their high moisture content, can lead to significant quality deterioration during storage. Nevertheless, a comprehensive evaluation of these quality losses has not yet been conducted. RESULTS: The effects of different storage temperatures (25, 4, and −20 °C) on the retrogradation‐related physicochemical changes in pre‐cooked rice noodles were elucidated mainly from the water dynamics and structural viewpoints. Thermal analysis demonstrated that amylopectin recrystallization took place in the noodles stored at refrigerated temperature, followed by room temperature. The refrigerated storage accelerated the starch retrogradation that caused the water molecules to become entrapped within the crystalline structure by lowering the water hydration properties and weighted T2 relaxation times of the pre‐cooked noodles. These water mobility patterns were correlated with the textural changes in the noodles (greater hardness and Rmax/extensibility). Furthermore, the higher structural density and thickness derived from starch retrogradation were observed in the tomographic and microscopic images of the refrigerated noodles. The principal component analysis demonstrated that various physicochemical changes of the pre‐cooked noodles during storage showed high correlations with the degree of starch retrogradation (r > 0.83). CONCLUSION: The physicochemical features of the precooked noodles stored under refrigerated conditions were involved in the molecular dynamics of water, showing a notable water mobility reduction derived from the starch retrogradation, which contributed to their thermal, tomographical, and textural changes. © 2023 Society of Chemical Industry. [ABSTRACT FROM AUTHOR]

Aging is the primary risk factor for the development of numerous human chronic diseases. On a molecular level, it significantly impacts the regulation of protein modifications, leading to the accumulation of degenerative protein modifications (DPMs) such as aberrant serine phosphorylation (p‐Ser) and trioxidized cysteine (t‐Cys) within the proteome. The altered p‐Ser is linked to abnormal cell signaling, while the accumulation of t‐Cys is associated with chronic diseases induced by oxidative stress. Despite this, the potential cross‐effects and functional interplay between these two critical molecular factors of aging remain undisclosed. This study analyzes the aging proteome of wild‐type C57BL/6NTac mice over 2 years using advanced proteomics and bioinformatics. Our objective is to provide a comprehensive analysis of how t‐Cys affects cell signaling and protein structure in the aging process. The results obtained indicate that t‐Cys residues accumulate in the aging proteome, interact with p‐Ser interacting enzymes, as validated in vitro, and alter their structures similarly to p‐Ser. These findings have significant implications for understanding the interplay of oxidative stress and phosphorylation in the aging process. Additionally, they open new venues for further research on the role(s) of these protein modifications in various human chronic diseases and aging, wherein exacerbated oxidation and aberrant phosphorylation are implicated. [ABSTRACT FROM AUTHOR]

At the beginning of the last century, multiple pandemics caused by influenza (flu) viruses severely impacted public health. Despite the development of vaccinations and antiviral medications to prevent and control impending flu outbreaks, unforeseen novel strains and continuously evolving old strains continue to represent a serious threat to human life. Therefore, the recently identified H10N7, for which not much data is available for rational structure‐based drug design, needs to be further explored. Here, we investigated the structural dynamics of neuraminidase N7 upon binding of inhibitors, and the drug resistance mechanisms against the oseltamivir (OTV) and laninamivir (LNV) antivirals due to the crucial R292K mutation on the N7 using the computational microscope, molecular dynamics (MD) simulations. In this study, each system underwent long 2 × 1 μs MD simulations to answer the conformational changes and drug resistance mechanisms. These long time‐scale dynamics simulations and free energy landscapes demonstrated that the mutant systems showed a high degree of conformational variation compared to their wildtype (WT) counterparts, and the LNV‐bound mutant exhibited an extended 150‐loop conformation. Further, the molecular mechanics Poisson–Boltzmann surface area (MM/PBSA) calculation and MM/GBSA free energy decomposition were used to characterize the binding of OTV and LNV with WT, and R292K mutated N7, revealing the R292K mutation as drug‐resistant, facilitated by a decline in binding interaction and a reduction in the dehydration penalty. Due to the broader binding pocket cavity of the smaller K292 mutant residue relative to the wildtype, the drug carboxylate to K292 hydrogen bonding was lost, and the area surrounding the K292 residue was more accessible to water molecules. This implies that drug resistance could be reduced by strengthening the hydrogen bond contacts between N7 inhibitors and altered N7, creating inhibitors that can form a hydrogen bond to the mutant K292, or preserving the closed cavity conformations. [ABSTRACT FROM AUTHOR]

Primary hyperoxaluria type I (PH1) is caused by deficient alanine:glyoxylate aminotransferase (AGT) activity. PH1‐causing mutations in AGT lead to protein mistargeting and aggregation. Here, we use hydrogen‐deuterium exchange (HDX) to characterize the wild‐type (WT), the LM (a polymorphism frequent in PH1 patients) and the LM G170R (the most common mutation in PH1) variants of AGT. We provide the first experimental analysis of AGT structural dynamics, showing that stability is heterogeneous in the native state and providing a blueprint for frustrated regions with potentially functional relevance. The LM and LM G170R variants only show local destabilization. Enzymatic transamination of the pyridoxal 5‐phosphate cofactor bound to AGT hardly affects stability. Our study, thus, supports that AGT misfolding is not caused by dramatic effects on structural dynamics. [ABSTRACT FROM AUTHOR]

Electron donor–acceptor (DA)‐type metal–organic frameworks (MOFs) with valence instability are promising molecular materials for the design of photo‐responsive and electronic/magnetic functional materials. Here, ultrafast photoinduced dynamics in a DA‐type layered MOF that exhibits a charge‐transfer (CT)‐type phase transition are reported: (NPr4)2[Fe2(Cl2An)3], where NPr4+ = tetra‐n‐propylammonium and Cl2An2− = 2,5‐dichloro‐3,6‐dihydroxo‐1,4‐benzoquinonate. At room temperature (300 K: RT), ultrafast photoinduced CT between the Fe and Cl2An ions induces a sensitive change in the state associated with the valence instability from a single‐chain, electron‐correlated state to a new photoinduced, structurally modulated state. In the photoinduced state, two absorption bands are observed, one on the higher‐energy side of the CT band and the other in the mid‐IR range. This strongly implies that the local inversion center on the Cl2An ion that exists in the initial state disappears instantly upon photoexcitation, causing an ultrafast change in the lattice structure due to the softening of rigid bonds. This has never been realized in thermal excitation. These findings demonstrate that a new electronic state with a unique lattice structure—i.e., a photoinduced hidden state—appears in this MOF system at ultra‐high speed (within 110 fs) upon photoexcitation at RT. [ABSTRACT FROM AUTHOR]

Excited state molecular dynamics simulations of the photoexcited phenyl azide have been performed. The semi‐classical surface hopping approximation has enabled an unconstrained analysis of the electronic and nuclear degrees of freedom which contribute to the molecular dissociation of phenyl azide into phenyl nitrene and molecular nitrogen. The significance of the second singlet excited state in leading the photodissociation has been established through electronic structure calculations, based on multi‐configurational schemes, and state population dynamics. The investigations on the structural dynamics have revealed the N−N bond separation to be accompanied by synchronous changes in the azide N−N−N bond angle. The 100 fs simulation results in a nitrene fragment that is electronically excited in the singlet manifold. [ABSTRACT FROM AUTHOR]

An exciting direction in metal‐organic frameworks involves the design and synthesis of flexible structures which can reversibly adapt their structure when triggered by external stimuli. Controlling the extent and nature of response in such solids is critical in order to develop custom dynamic materials for advanced applications. Towards this, it is highly important to expand the diversity of existing flexible MOFs, generating novel materials and gain an in‐depth understanding of the associated dynamic phenomena, eventually unlocking key structure‐property relationships. In the present work, we successfully utilized reticular chemistry for the construction of two novel series of highly crystalline, flexible rare‐earth MOFs, RE‐thc‐MOF‐2 and RE‐teb‐MOF‐1. Extensive single‐crystal to single‐crystal structural analyses coupled with detailed gas and vapor sorption studies, shed light onto the unique responsive behavior. The development of these series is related to the reported RE‐thc‐MOF‐1 solids which were found to display a unique continuous breathing and gas‐trapping property. The synthesis of RE‐thc‐MOF‐2 and RE‐teb‐MOF‐1 materials represents an important milestone as they provide important insights into the key factors that control the responsive properties of this fascinating family of flexible materials and demonstrates that it is possible to control their dynamic behavior and the associated gas and vapor sorption properties. [ABSTRACT FROM AUTHOR]

Singlet exciton fission (SF), the formation of two triplet excitons from one singlet exciton, involves electronic, nuclear, and spin degrees of freedom as well as their couplings. Despite almost 60 years of research on this process, a complete microscopic understanding is still missing. One important open question concerns the role of nuclear motion in SF. In this perspective, recent results on the exciton dynamics are related to the structural dynamics of single‐crystal pentacene and how they provide insights into that open question is shown. To probe the electronic dynamics, orbital‐resolved measurements of the electronic structure are carried out using time‐ and angle‐resolved photoemission spectroscopy. With femtosecond electron diffraction and with ab initio computations, the complementary nuclear dynamics is tracked. The results from both techniques are summarized, and how they relate to each other is discussed. Then, remaining open questions are outlined and potential routes are identified to tackle them, hopefully guiding future studies. [ABSTRACT FROM AUTHOR]

Effects of traffic‐induced vibrations on young concrete: part 1 In the COUNT (Concreting under traffic) research project, the effects of traffic vibrations on young concrete are extensively examined. This research question has recently become more relevant since traffic closures often have to be imposed when bridges are renovated or widened, as there is a concern that the vibrations caused by traffic will damage the young (hardening) concrete. COUNT aims to determine critical vibration values and underlying damage mechanisms based on three test series. Both harmonic and real bridge vibrations due to train, truck and car traffic are adopted, and the effects on the material concrete itself are investigated, as well as on the bond behaviour between concrete and reinforcement, and the contact between existing and new concrete parts. This first part of the article reports on the results of test series 1 and 2, in which small samples were systematically excited by artificial vibrations during hardening. It was found that conventional traffic vibrations do not affect the strength of concrete per se, but that the bond between the concrete and the reinforcement can be weakened if the vibrations are too great. In addition, it was found that (differential) displacements is a more suitable measure for damage assessment than the vibration velocity. [ABSTRACT FROM AUTHOR]

Active deformation behavior reflects cell structural dynamics adapting to varying environmental constraints during malignancy progression. In most cases, cell mechanics is characterized by modeling using static equilibrium systems, which fails to comprehend cell deformation behavior leading to inaccuracies in distinguishing cancer cells from normal cells. Here, a method is introduced to measure the active deformation behavior of cancer cells using atomic force microscopy (AFM) and the newly developed deformation behavior cytometry (DBC). During the measurement, cells are deformed and allows a long timescale relaxation (≈5 s). Two parameters are derived to represent deformation behavior: apparent Poisson's ratio for adherent cells, which is measured with AFM and refers to the ratio of the lateral strain to the longitudinal strain of the cell, and shape recovery for suspended cells, which is measured with DBC. Active deformation behavior defines cancer cell mechanics better than traditional mechanical parameters (e.g., stiffness, diffusion, and viscosity). Additionally, aquaporins are essential for promoting the deformation behavior, while the actin cytoskeleton acts as a downstream effector. Therefore, the potential application of the cancer cell active deformation behavior as a biomechanical marker or therapeutic target in cancer treatment should be evaluated. [ABSTRACT FROM AUTHOR]

In the study of CaO–SiO2–Al2O3–Li2O system slag, molecular dynamics simulations are performed to analyze the behavior of Al3+ at different alkalinities. The results show that the AlO bond length increases with increasing alkalinity and is unstable compared to the SiO bond. The [AlO4]5− tetrahedra are less stable than the [SiO4]4− tetrahedra. The higher the alkalinity, the shorter the AlO bonds and the longer the CaO bonds, thus destroying the aluminum‐oxygen ionophore. Increasing alkalinity converts complex structures into simpler ones, such as AlOAl, bringing the OAlO bond angles closer to the ideal tetrahedron. Reduced slag polymerization increases the distance between neighboring [AlO4]5− tetrahedra, thereby increasing the AlOAl bond angles. The [SiO4]4− tetrahedra prefer to bond with the [AlO4]5− tetrahedra. The change in SiOAl is less than that of SiOSi. The dissociation of CaO provides the O2−, which allows the depolymerization of SiOSi to form nonbridging oxygen SiO, whereas the depolymerization of SiOAl occurs when alkalinity is sufficient to form the SiO and AlO bonds. The [AlO4]5− tetrahedra are more likely to bond with [AlO4]5− tetrahedra than [AlO4]5− tetrahedra. [ABSTRACT FROM AUTHOR]

Carbapenem‐resistant Klebsiella pneumoniae (CRKP) infections continue to impose high morbidity threats to hospitalized patients worldwide, limiting therapeutic options to last‐resort antibiotics like colistin. However, the dynamic genomic landscape of colistin‐resistant K. pneumoniae (COLR‐Kp) invoked ardent exploration of underlying molecular signatures for therapeutic propositions/designs. We unveiled the structural impact of the widespread and emerging PmrB mutations involved in colistin resistance (COLR) in K. pneumoniae. In the present study, clinical isolates of K. pneumoniae expressed variable susceptibilities to colistin (>0.5 μg/mL for resistant and ≤0.25 μg/mL for susceptible) despite mutations such as T157P, G207D and T246A. The protein sequences extracted from in‐house sequenced genomes were used to model mutant PmrB proteins and analyze the underlying structural alterations. The mutations were contrasted based on molecular dynamics simulation trajectories, free‐energy landscapes and structural flexibility profiles. The altered backbone flexibilities can be an essential factor for mutant selection by COLR K. pneumoniae and can provide clues to deal with emerging mutants. Furthermore, PmrB having high druggability confidence (>0.99), was explored as a potential target for 1396 virtually screened FDA‐approved drug candidates. Among the top‐10 compounds (scores >70), amphotericin B was found to be potential candidate with high affinity (Binding energy <−8 kcal/mol) and stable interactions (RMSF <0.7 Å) against PmrB druggable pockets, despite the mutations, which encourages future adjunct therapeutic research against COLR‐Kp. [ABSTRACT FROM AUTHOR]

Climate change is increasing the frequency, intensity, and duration of extreme weather events across the globe. Understanding the capacity for ecological communities to withstand and recover from such events is critical. Typhoons are extreme weather events that are expected to broadly homogenize ecological dynamics through structural damage to vegetation and longer‐term effects of salinization. Given their unpredictable nature, monitoring ecological responses to typhoons is challenging, particularly for mobile animals such as birds. Here, we report spatially variable ecological responses to typhoons across terrestrial landscapes. Using a high temporal resolution passive acoustic monitoring network across 24 sites on the subtropical island of Okinawa, Japan, we found that typhoons elicit divergent ecological responses among Okinawa's diverse terrestrial habitats, as indicated by increased spatial variability of biological sound production (biophony) and individual species detections. This suggests that soniferous communities are capable of a diversity of different responses to typhoons. That is, spatial insurance effects among local ecological communities provide resilience to typhoons at the landscape scale. Even though site‐level typhoon impacts on soundscapes and bird detections were not particularly strong, monitoring at scale with high temporal resolution across a broad spatial extent nevertheless enabled detection of spatial heterogeneity in typhoon responses. Further, species‐level responses mirrored those of acoustic indices, underscoring the utility of such indices for revealing insight into fundamental questions concerning disturbance and stability. Our findings demonstrate the significant potential of landscape‐scale acoustic sensor networks to capture the understudied ecological impacts of unpredictable extreme weather events. [ABSTRACT FROM AUTHOR]

Despite the significant progress in protein‐based materials, creating a tunable protein‐activated hydrogel lens remains an elusive goal. This study leverages the synergistic relationship between protein structural dynamics and polymer hydrogel engineering to introduce a highly transparent protein–polymer actuator. By incorporating bovine serum albumin into polyethyleneglycol diacrylate hydrogels, the authors achieved enhanced light transmittance and conferred actuating capabilities to the hydrogel. Taking advantage of these features, a bilayer protein‐driven hydrogel lens that dynamically modifies its focal length in response to pH changes, mimicking the adaptability of the human lens, is fabricated. The lens demonstrates durability and reproducibility, highlighting its potential for repetitive applications. This integration of protein‐diverse biochemistry, folding nanomechanics, and polymer engineering opens up new avenues for harnessing the wide range of proteins to potentially propel various fields such as diagnostics, lab‐on‐chip, and deep‐tissue bio‐optics, advancing the understanding of incorporating biomaterials in the optical field. [ABSTRACT FROM AUTHOR]

DNA repair protein RAD51 is a key player in the homologous recombination pathway. Upon DNA damage, RAD51 is transported into the nucleus by BRCA2, where it can repair DNA double‐strand breaks. Due to the structural complexity and dynamics, researchers have not yet clarified the mechanistic details of every step of RAD51 recruitment and DNA repair. RAD51 possesses an intrinsic tendency to form oligomeric structures, which make it challenging to conduct biochemical and biophysical investigations. Here, for the first time, we report on the isolation and characterization of a human monomeric RAD51 recombinant form, obtained through a double mutation, which preserves the protein's integrity and functionality. We investigated different buffers to identify the most suitable condition needed to definitively stabilize the monomer. The monomer of human RAD51 provides the community with a unique biological tool for investigating RAD51‐mediated homologous recombination, and paves the way for more reliable structural, mechanistic, and drug discovery studies. [ABSTRACT FROM AUTHOR]

DNA repair protein RAD51 is a key player in the homologous recombination pathway. Upon DNA damage, RAD51 is transported into the nucleus by BRCA2, where it can repair DNA double‐strand breaks. Due to the structural complexity and dynamics, researchers have not yet clarified the mechanistic details of every step of RAD51 recruitment and DNA repair. RAD51 possesses an intrinsic tendency to form oligomeric structures, which make it challenging to conduct biochemical and biophysical investigations. Here, for the first time, we report on the isolation and characterization of a human monomeric RAD51 recombinant form, obtained through a double mutation, which preserves the protein's integrity and functionality. We investigated different buffers to identify the most suitable condition needed to definitively stabilize the monomer. The monomer of human RAD51 provides the community with a unique biological tool for investigating RAD51‐mediated homologous recombination, and paves the way for more reliable structural, mechanistic, and drug discovery studies. [ABSTRACT FROM AUTHOR]

2D‐on‐3D (2D/3D) perovskite heterostructures present a promising strategy to realize efficient and stable photovoltaics. However, their applicability in inverted solar cells is limited due to the quantum confinement of the 2D‐layer and solvent incompatibilities that disrupt the underlying 3D layer, hampering electron transport at the 2D/3D interface. Herein, solvent‐dependent formation dynamics and structural evolution of 2D/3D heterostructures are investigated via in situ X‐ray scattering. It is revealed that solvent interaction with the 3D surface determines the formation sequence and spatial distribution of quasi‐2D phases with n = 2–4. Isopropanol (IPA) reconstructs the perovskite into a PbI2‐rich surface, forming a strata with smaller n first, followed by a thinner substratum of larger n. In contrast, 2,2,2‐Trifluoroethanol (TFE) preserves the 3D surface, promoting the formation of uniformly distributed larger n domains first, and smaller n last. Leveraging these insights, Dion–Jacobson perovskites are used with superior charge transport properties and structural robustness to fabricate 2D/3D heterostructures dominated by n ≥ 3 and engineer a favorable energy landscape for electron tunneling. Inverted solar cells based on 3‐Aminomethylpyridine and TFE achieve a champion efficiency of 23.60%, with Voc and FF of 1.19 V and 84.5%, respectively, and superior stabilities with t94 of 960 h under thermal stress. [ABSTRACT FROM AUTHOR]

In this article, we substantiate the appositeness of the mode‐matching technique to study the scattering response of bridging elastic plates connecting two flexible duct regions of different heights. We present two different solution schemes to analyze the structure‐borne and fluid‐borne radiations in the elastic plate‐bounded waveguide. The first scheme supplements the mode‐matching technique with the so‐called tailored‐Galerkin approach that uses a solution ansatz with homogeneous and integral parts corresponding to the vibrations of the bridging elastic plate and the cavity, respectively. In the second scheme, we supplement the mode‐matching technique with the modal approach wherein the displacement of the bridging elastic plate is projected onto the eigenmodes of the cavity. To handle the non‐orthogonality of the eigenfunctions, we invoke generalized orthogonality relations. An advantage of the proposed mode‐matching schemes is that they provide a convenient way of incorporating a variety of edge conditions on the joints of the plates, including clamped, pin‐joint, or restraint connections. The numerical analysis of the waveguide scattering problems substantiates that edge connections on the joints have a significant impact on the scattering energies and transmission loss. Furthermore, it appears that the transmission loss and structural vibration attenuation in the expansion chamber may be improved by adjusting chamber dimensions and excitation modes. [ABSTRACT FROM AUTHOR]

This paper aims to develop an innovative multiaxial fatigue criterion based on the stress invariant, in order to perform the fatigue damage analysis of engineering structures subjected to random vibrations. First, the change rule of structural vibration fatigue lifetime under different load correlation conditions is systemically studied by experiments. Then, the finite element analysis of such a structure, including the modal analysis and the spectral analysis, is implemented in order to compute the response stress power spectral density (PSD) functions at the critical fatigue‐prone location under coupled random acceleration base excitations. Finally, the influence rule of load correlation on the vibration fatigue damage of such a symmetrical structure is theoretically illustrated through formula derivation. Moreover, combined with the critical distance theory point method, the proposed time/frequency‐domain multiaxial fatigue criterion is applied for vibration fatigue lifetime evaluation of the structure. The lifetime prediction accuracy of the proposed multiaxial fatigue criterion is verified by comparing with the vibration fatigue test results. Highlights: A novel time‐domain multiaxial vibration fatigue analysis method is developed.A novel frequency‐domain multiaxial vibration fatigue analysis method is developed.Influence of load correlation on vibration fatigue damage is investigated.Validity of proposed method is confirmed by fatigue life prediction result. [ABSTRACT FROM AUTHOR]

Biomolecular self‐assembly of hierarchical materials is a precise and adaptable bottom‐up approach to synthesizing across scales with considerable energy, health, environment, sustainability, and information technology applications. To achieve desired functions in biomaterials, it is essential to directly observe assembly dynamics and structural evolutions that reflect the underlying energy landscape and the assembly mechanism. This review will summarize the current understanding of biomolecular assembly mechanisms based on in situ characterization and discuss the broader significance and achievements of newly gained insights. In addition, we will also introduce how emerging deep learning/machine learning‐based approaches, multiparametric characterization, and high‐throughput methods can boost the development of biomolecular self‐assembly. The objective of this review is to accelerate the development of in situ characterization approaches for biomolecular self‐assembly and to inspire the next generation of biomimetic materials. [ABSTRACT FROM AUTHOR]

Biomolecular self‐assembly of hierarchical materials is a precise and adaptable bottom‐up approach to synthesizing across scales with considerable energy, health, environment, sustainability, and information technology applications. To achieve desired functions in biomaterials, it is essential to directly observe assembly dynamics and structural evolutions that reflect the underlying energy landscape and the assembly mechanism. This review will summarize the current understanding of biomolecular assembly mechanisms based on in situ characterization and discuss the broader significance and achievements of newly gained insights. In addition, we will also introduce how emerging deep learning/machine learning‐based approaches, multiparametric characterization, and high‐throughput methods can boost the development of biomolecular self‐assembly. The objective of this review is to accelerate the development of in situ characterization approaches for biomolecular self‐assembly and to inspire the next generation of biomimetic materials. [ABSTRACT FROM AUTHOR]

In this study, we explore a possible platform for the CO2 reduction (CO2R) in one of water's solid phases, namely clathrate hydrates (CHs), by ab initio molecular dynamics and well‐tempered metadynamics simulations with periodic boundary conditions. We found that the stacked H2O nanocages in CHs help to initialize CO2R by increasing the electron‐binding ability of CO2. The substantial CO2R processes are further influenced by the hydrogen bond networks in CHs. The first intermediate CO2− in this process can be stabilized through cage structure reorganization into the H‐bonded [CO2−⋅⋅⋅H−OHcage] complex. Further cooperative structural dynamics enables the complex to convert into a vital transient [CO22−⋅⋅⋅H−OHcage] intermediate in a low‐barrier disproportionation‐like process. Such a highly reactive intermediate spontaneously triggers subsequent double proton transfer along its tethering H‐bonds, finally converting it into HCOOH. These hydrogen‐bonded nanoreactors feature multiple functions in facilitating CO2R such as confining, tethering, H‐bond catalyzing and proton pumping. Our findings have a general interest and extend the knowledge of CO2R into porous aqueous systems. [ABSTRACT FROM AUTHOR]

Candida boidinii NAD+‐dependent formate dehydrogenase (CbFDH) has gained significant attention for its potential application in the production of biofuels and various industrial chemicals from inorganic carbon dioxide. The present study reports the atomic X‐ray crystal structures of wild‐type CbFDH at cryogenic and ambient temperatures, as well as that of the Val120Thr mutant at cryogenic temperature, determined at the Turkish Light Source 'Turkish DeLight'. The structures reveal new hydrogen bonds between Thr120 and water molecules in the active site of the mutant CbFDH, suggesting increased stability of the active site and more efficient electron transfer during the reaction. Further experimental data is needed to test these hypotheses. Collectively, these findings provide invaluable insights into future protein‐engineering efforts that could potentially enhance the efficiency and effectiveness of CbFDH. [ABSTRACT FROM AUTHOR]

The automotive industry must deal with significant challenges in the future. Consequently, predicting the Noise‐Vibration‐Harshness (NVH) in the early design and concept phase becomes essential. Especially dynamic seat behavior immediately affects ride comfort and hence customer acceptance. Therefore, it is necessary to have reliable finite element (FE) models for the simulation‐based prediction of the dynamic seat behavior. This study describes different aspects of the experimental‐ and simulation‐based modeling of a vehicle seat. The experimental modal analysis is used to characterize the seat system as well as the subsystem's seat backrest and frame. The structural dynamics of a seat depend on various sensitive parameters. We identified the dominant mode shapes below 100 Hz, which are lateral, fore‐and‐aft, and twisting modes. We could see that the seat backrest has a substantial mass influence. Besides, we showed that the twisting mode can be modified by varying cross‐direction stiffness. Thus, findings are utilized to improve the predictive power of simulation results. [ABSTRACT FROM AUTHOR]

A large conformational heterogeneity of human NAD(P)H:quinone oxidoreductase 1 (NQO1), a flavoprotein associated with various human diseases, has been observed to occur in the catalytic site of the enzyme. Here, we report the X‐ray structure of NQO1 with phenylmethylsulfonyl fluoride (PMSF) at 1.6 Å resolution. Activity assays confirmed that, despite being covalently bound to the Tyr128 residue at the catalytic site, PMSF did not abolish NQO1 activity. This may indicate that the PMSF molecule does not reduce the high flexibility of Tyr128, thus allowing NADH and DCPIP substrates to bind to the enzyme. Our results show that targeting Tyr128, a key residue in NQO1 function, with small covalently bound molecules could possibly not be a good drug discovery strategy to inhibit this enzyme. [ABSTRACT FROM AUTHOR]

This paper aims to clarify the behaviour and mechanism of electromagnetic vibration in long sheet secondary tubular linear induction motors (LSS‐TLIMs). Firstly, the spatial and temporal characteristics of electromagnetic force acting in the stator are analysed. Secondly, based on the wave propagation method, an analytical model is established to calculate the vibration response of the stator, which is simplified as a finite cylindrical shell. The accuracy of the proposed model, as well as the rationality of the simplification, are verified by 3D FEM simulation. It is indicated that the electromagnetic vibration response of LSS‐TLIMs mainly depends on the "axial breathing mode" (ABM) and corresponding "modal participation factor". Moreover, the influences of the spatial distribution of electromagnetic force and the structural dimensions on the vibration are investigated. Finally, the "static vibration test" is performed to validate the above analysis. It is concluded that, compared with a rotary motor, the low‐frequency vibration of LSS‐TLIMs can be easily controlled since the natural frequency of ABMs tends to be much higher than that of the circumferential mode. [ABSTRACT FROM AUTHOR]

Relaxation occurs spontaneously in all glasses and is a fundamental step of important technological processes, such as annealing, crystal nucleation, and chemical strengthening by ion exchange. Despite extensive studies over the past decades, there are still conflicting results on whether the kinetics of structural relaxation depends on the analyzed property. Thus, in this study, we used a lithium disilicate glass as a model composition to determine the structural relaxation kinetics during physical aging experiments by measuring the time evolution of the refractive index and ionic conductivity down to 35 K below the initial fictive temperature. In all cases, variations in these properties were adequate to capture the structural changes throughout the aging experiments. At each temperature, the experimental relaxation data fit quite well with the classical stretched exponential relation. We also found that the relaxation process starts faster when probed by ionic conductivity than by refractive index; however, they show similar average relaxation times. These very small structural rearrangements are always the same, but ionic conductivity changes faster than refractive index at the beginning of the process. Our comprehensive results strongly indicate that relaxation dynamics is indeed dependent on the analyzed property. [ABSTRACT FROM AUTHOR]

The rapidly emerging perovskites hold immense potential for revolutionizing optoelectronic and photovoltaic applications. However, understanding the complex structural dynamics and their response at extreme conditions in robust environments is crucial for optimizing the practical performance of perovskite‐based devices. Previous X‐ray diffraction studies have shown great potential for studying the average structures of these materials, but for more complex analysis at the local atomic level, Raman spectroscopy is a powerful tool. In this study, temperature‐ and pressure‐dependent Raman spectroscopy was used to elucidate the intricate lattice dynamics, phase transitions, and amorphization of FAPbBr3 single crystals at extreme conditions such as low temperature or high pressure. Temperature‐dependent Raman spectra unveiled significant variations in wavenumbers, full width at half maximum, and the vanishing of specific modes at higher temperatures. These were ascribed to symmetry changes caused by two crystallographic phase transitions at −127°C from orthorhombic to tetragonal and at −33°C from tetragonal to cubic phase. In addition, some of the Raman modes disappeared upon heating at −90°C, which was associated with a crystallographically unresolved transition. Pressure‐dependent Raman scattering revealed two phase transitions at 0.3 GPa and 2.2 GPa, which corresponded to the contraction of the PbBr6 octahedra and their tilting distortion, respectively. Further compression uncovered amorphization at 3.6 GPa, characterized by the vanishing of crystalline Raman modes together with the emergence of broad new modes due to the disorder within the crystal structure. Upon pressure release, the original Raman modes were recovered, indicating the reversibility of the pressure‐induced phase transitions. The changes in the Raman spectra were the most significant, especially in the low‐wavenumber lattice modes, when the FAPbBr3 underwent orthorhombic phase transition. It indicates that the inorganic sublattice is affected by the structural change into the orthorhombic phase caused either by temperature or pressure variation. [ABSTRACT FROM AUTHOR]

In this paper, the numerical properties of a recently developed high‐order Spectral Euler‐Bernoulli Beam Element (SBE) featuring a C1‐continuous approximation of the displacement field are assessed. The C1‐continuous shape functions are based on two main ingredients, which are an Hermitian interpolation scheme and the use of Gauß‐Lobatto‐Legendre (GLL) points. Employing GLL‐points does not only avoid Runge oscillations, but also yields a diagonal mass matrix when exploiting the nodal quadrature technique as a mass lumping scheme. Especially in high‐frequency transient analyses, where often explicit time integration schemes are utilized, having a diagonal mass matrix is an attractive property of the proposed element formulation. This is, however, achieved at the cost of an under‐integration of the mass matrix. Therefore, a special focus of this paper is placed on the evaluation of the numerical properties, such as the conditioning of the element matrices and the attainable rates of convergence (ROCs). To this end, the numerical behavior of the SBEs is comprehensively analyzed by means of selected benchmark examples. In a nutshell, the obtained results demonstrate that the element yields good accuracy in combination with an increased efficiency for structural dynamics exploiting the diagonal structure of the mass matrix. [ABSTRACT FROM AUTHOR]

Supported gold catalysts have been reported to exhibit exceptional selectivity towards the desirable product, an alkene, in chemoselective hydrogenation of highly unsaturated alkynes and alkadienes. However, insights on the interactions between the gold nanoparticles and the 1,3‐butadiene adsorbates are lacking. In this work, using atomic scale in situ ETEM with the support of DFT‐based calculations, the reactivity of TiO2 supported gold nanoparticles below 7 nm towards 1,3‐butadiene is investigated by monitoring their structure and dynamics under 105 Pa of 0.46 % C4H6/He during cooling at 300 °C and 200 °C. For sizes larger than 5 nm, the initial truncated octahedron morphology of gold nanoparticles is found to evolve towards a rounded morphology, with the growth of more open (110) surfaces and higher index facets at the expense of the initially present (100) and (111) facets, reflecting the adsorption of butadiene on low coordination sites at 300 °C. The morphology changes are shown to be accompanied by nucleation and glide of dislocations. At 200 °C, 1,3‐butadiene adsorption is shown to predominateon (111) facets, with the nanoparticles reverting to a faceted morphology while maintaining their fcc structure. For smaller particle size, Au fcc structure is also maintained under 1,3‐butadiene. [ABSTRACT FROM AUTHOR]

The problem of adaptive semi‐active control of transient structural vibration induced by unknown harmonic excitation is studied. The controller adaptation is attained by using a specially designed reinforcement learning algorithm that adjusts the parameters of a switching control policy to guarantee efficient dissipation of the structural energy. This algorithm relies on an efficient gradient‐based sequence that accelerates the learning protocol and results in suboptimal control. The performance of this method is examined through numerical experiments for a span structure that is equipped with a semi‐active device of controlled stiffness and damping parameters. The experiments cover a selection of control learning scenarios and comparisons to optimal open‐loop and heuristic state‐feedback control strategies. This study has confirmed that the developed method has high stabilizing performance, and the relatively low computational burden of the incorporated iterative learning algorithm facilitates its application to multi–degree‐of‐freedom structures. [ABSTRACT FROM AUTHOR]

Two‐dimensional (2D) lead halide perovskites (LHPs) have shown great promises for light‐emitting applications and excitonic devices. Fulfilling these promises demands an in‐depth understanding on the relationships between the structural dynamics and exciton‐phonon interactions that govern the optical properties. Here, we unveil the structural dynamics of 2D lead iodide perovskites with different spacer cations. Loose packing of an undersized spacer cation leads to out‐of‐plane octahedral tilting, whereas compact packing of an oversized spacer cation stretches Pb−I bond length, resulting in Pb2+ off‐center displacement driven by stereochemical expression of the Pb2+ 6s2 lone pair electrons. Density functional theory calculations indicate that the Pb2+ cation is off‐center displaced mainly along the direction where the octahedra are stretched the most by the spacer cation. We find dynamic structural distortions associated with either octahedral tilting or Pb2+ off‐centering lead to a broad Raman central peak background and phonon softening, which increase the non‐radiative recombination loss via exciton‐phonon interactions and quench the photoluminescence intensity. The correlations between the structural, phonon, and optical properties are further confirmed by the pressure tuning of the 2D LHPs. Our results demonstrate that minimizing the dynamic structural distortions via a judicious selection of the spacer cations is essential to realize high luminescence properties in 2D LHPs. [ABSTRACT FROM AUTHOR]

Two‐dimensional (2D) lead halide perovskites (LHPs) have shown great promises for light‐emitting applications and excitonic devices. Fulfilling these promises demands an in‐depth understanding on the relationships between the structural dynamics and exciton‐phonon interactions that govern the optical properties. Here, we unveil the structural dynamics of 2D lead iodide perovskites with different spacer cations. Loose packing of an undersized spacer cation leads to out‐of‐plane octahedral tilting, whereas compact packing of an oversized spacer cation stretches Pb−I bond length, resulting in Pb2+ off‐center displacement driven by stereochemical expression of the Pb2+ 6s2 lone pair electrons. Density functional theory calculations indicate that the Pb2+ cation is off‐center displaced mainly along the direction where the octahedra are stretched the most by the spacer cation. We find dynamic structural distortions associated with either octahedral tilting or Pb2+ off‐centering lead to a broad Raman central peak background and phonon softening, which increase the non‐radiative recombination loss via exciton‐phonon interactions and quench the photoluminescence intensity. The correlations between the structural, phonon, and optical properties are further confirmed by the pressure tuning of the 2D LHPs. Our results demonstrate that minimizing the dynamic structural distortions via a judicious selection of the spacer cations is essential to realize high luminescence properties in 2D LHPs. [ABSTRACT FROM AUTHOR]

It has been recently shown that in some proteins, tertiary‐structure dynamics occur surprisingly fast, that is on the microsecond or sub‐millisecond time scales. In this State of the Art Review, we discuss how such ultrafast domain motions relate to the function of caseinolytic peptidase B (ClpB), a AAA+ disaggregation machine. ClpB is a large hexameric protein that collaborates with cellular chaperone machinery to rescue protein chains from aggregates. We used single‐molecule FRET spectroscopy to capture the dynamics of essential structural elements within this machine. It was found that the middle domain of ClpB, known to act as its activator, toggles between two states much faster than the overall activity cycle of the protein, suggesting a novel mode of continuous, tunable switching. Motions of the N‐terminal domain were observed to restrict the conformational space of the M domain in the absence of a substrate protein, thereby preventing it from tilting and spuriously activating ClpB. Finally, microsecond dynamics of pore loops responsible for substrate pulling through ClpB's central channel, together with their response to specific perturbations, point to a Brownian‐ratchet mechanism for protein translocation. Based on our findings, we propose a two‐time‐scale model for the activity of ClpB, in which fast conformational dynamics affect slower functional steps, determined by ATP hydrolysis time. Future work on this and other proteins is likely to shed further light on the role of ultrafast dynamics on protein function. [ABSTRACT FROM AUTHOR]

Photosynthesis is a very important process for the current biosphere which can maintain such a subtle and stable circulatory ecosystem on earth through the transformation of energy and substance. Even though been widely studied in various aspects, the physiological activities, such as intrinsic structural vibration and self‐regulation process to stress of photosynthetic proteins, are still not in‐depth resolved in real‐time. Herein, utilizing silicon nanowire biosensors with ultrasensitive temporal and spatial resolution, real‐time responses of a single photosystem I‐light harvesting complex I (PSI‐LHCI) supercomplex of Pisum sativum to various conditions, including gradient variations in temperature, illumination, and electric field, are recorded. Under different temperatures, there is a bi‐state switch process associated with the intrinsic thermal vibration behavior. When the variations of illumination and the bias voltage are applied, two additional shoulder states, probably derived from the self‐conformational adjustment, are observed. Based on real‐time monitoring of the dynamic processes of the PSI‐LHCI supercomplex under various conditions, it is successively testified to promising nanotechnology for protein profiling and biological functional integration in photosynthesis studies. [ABSTRACT FROM AUTHOR]