Proc Natl Acad Sci U S A
January 2025
A central paradigm of nonequilibrium physics concerns the dynamics of heterogeneity and disorder, impacting processes ranging from the behavior of glasses to the emergent functionality of active matter. Understanding these complex mesoscopic systems requires probing the microscopic trajectories associated with irreversible processes, the role of fluctuations and entropy growth, and the timescales on which nonequilibrium responses are ultimately maintained. Approaches that illuminate these processes in model systems may enable a more general understanding of other heterogeneous nonequilibrium phenomena, and potentially define ultimate speed and energy cost limits for information processing technologies.
View Article and Find Full Text PDFThe discovery of polar vortices and skyrmions in ferroelectric-dielectric superlattices [such as (PbTiO)/(SrTiO)] has ushered in an era of novel dipolar topologies and corresponding emergent phenomena. The key to creating such emergent features has generally been considered to be related to counterpoising strongly polar and non-polar materials thus creating the appropriate boundary conditions. This limits the utility these materials can have, however, by rendering (effectively) half of the structure unresponsive to applied stimuli.
View Article and Find Full Text PDFThe exotic polarization configurations of topologically protected dipolar textures have opened new avenues for realizing novel phenomena absent in traditional ferroelectric systems. While multiple recent studies have revealed a diverse array of emergent properties in such polar topologies, the details of their atomic and mesoscale structures remain incomplete. Through atomic- and meso-scale imaging techniques, the emergence of a macroscopic ferroelectric polarization along both principal axes of the vortex lattice while performing phase-field modeling to probe the atomic scale origins of these distinct polarization components is demonstrated.
View Article and Find Full Text PDFSpin waves in magnetic materials are promising information carriers for future computing technologies due to their ultra-low energy dissipation and long coherence length. Antiferromagnets are strong candidate materials due, in part, to their stability to external fields and larger group velocities. Multiferroic antiferromagnets, such as BiFeO (BFO), have an additional degree of freedom stemming from magnetoelectric coupling, allowing for control of the magnetic structure, and thus spin waves, with the electric field.
View Article and Find Full Text PDFAntiferromagnets have attracted significant attention in the field of magnonics, as promising candidates for ultralow-energy carriers for information transfer for future computing. The role of crystalline orientation distribution on magnon transport has received very little attention. In multiferroics such as BiFeO the coupling between antiferromagnetic and polar order imposes yet another boundary condition on spin transport.
View Article and Find Full Text PDFStabilization of topological spin textures in layered magnets has the potential to drive the development of advanced low-dimensional spintronics devices. However, achieving reliable and flexible manipulation of the topological spin textures beyond skyrmion in a two-dimensional magnet system remains challenging. Here, we demonstrate the introduction of magnetic iron atoms between the van der Waals gap of a layered magnet, FeGaTe, to modify local anisotropic magnetic interactions.
View Article and Find Full Text PDFA magnon is a collective excitation of the spin structure in a magnetic insulator and can transmit spin angular momentum with negligible dissipation. This quantum of a spin wave has always been manipulated through magnetic dipoles (that is, by breaking time-reversal symmetry). Here we report the experimental observation of chiral spin transport in multiferroic BiFeO and its control by reversing the ferroelectric polarization (that is, by breaking spatial inversion symmetry).
View Article and Find Full Text PDFBismuth ferrite (BiFeO) is a multiferroic material that exhibits both ferroelectricity and canted antiferromagnetism at room temperature, making it a unique candidate in the development of electric-field controllable magnetic devices. The magnetic moments in BiFeO are arranged into a spin cycloid, resulting in unique magnetic properties which are tied to the ferroelectric order. Previous understanding of this coupling has relied on average, mesoscale measurements.
View Article and Find Full Text PDFThe recent discovery of polar topological structures has opened the door for exciting physics and emergent properties. There is, however, little methodology to engineer stability and ordering in these systems, properties of interest for engineering emergent functionalities. Notably, when the surface area is extended to arbitrary thicknesses, the topological polar texture becomes unstable.
View Article and Find Full Text PDFBismuth ferrite has garnered considerable attention as a promising candidate for magnetoelectric spin-orbit coupled logic-in-memory. As model systems, epitaxial BiFeO thin films have typically been deposited at relatively high temperatures (650-800 °C), higher than allowed for direct integration with silicon-CMOS platforms. Here, we circumvent this problem by growing lanthanum-substituted BiFeO at 450 °C (which is reasonably compatible with silicon-CMOS integration) on epitaxial BaPbBiO electrodes.
View Article and Find Full Text PDF2D layered materials with broken inversion symmetry are being extensively pursued as spin source layers to realize high-efficiency magnetic switching. Such low-symmetry layered systems are, however, scarce. In addition, most layered magnets with perpendicular magnetic anisotropy show a low Curie temperature.
View Article and Find Full Text PDFDNA-encoded libraries (DELs) provide unmatched chemical diversity and starting points for novel drug modalities. Here, we describe a workflow that exploits the bifunctional attributes of DEL ligands as a platform to generate BRET probes for live cell target engagement studies. To establish proof of concept, we performed a DEL screen using aurora kinase A and successfully converted aurora DEL ligands as cell-active BRET probes.
View Article and Find Full Text PDFControl and understanding of ensembles of skyrmions is important for realization of future technologies. In particular, the order-disorder transition associated with the 2D lattice of magnetic skyrmions can have significant implications for transport and other dynamic functionalities. To date, skyrmion ensembles have been primarily studied in bulk crystals, or as isolated skyrmions in thin film devices.
View Article and Find Full Text PDFNon-collinear antiferromagnets (AFMs) are an exciting new platform for studying intrinsic spin Hall effects (SHEs), phenomena that arise from the materials' band structure, Berry phase curvature, and linear response to an external electric field. In contrast to conventional SHE materials, symmetry analysis of non-collinear antiferromagnets does not forbid non-zero longitudinal and out-of-plane spin currents with polarization and predicts an anisotropy with current orientation to the magnetic lattice. Here, multi-component out-of-plane spin Hall conductivities are reported in L1 -ordered antiferromagnetic PtMn thin films that are uniquely generated in the non-collinear state.
View Article and Find Full Text PDFTopologically protected polar textures have provided a rich playground for the exploration of novel, emergent phenomena. Recent discoveries indicate that ferroelectric vortices and skyrmions not only host properties markedly different from traditional ferroelectrics, but also that these properties can be harnessed for unique memory devices. Using a combination of capacitor-based capacitance measurements and computational models, it is demonstrated that polar vortices in dielectric-ferroelectric-dielectric trilayers exhibit classical ferroelectric bi-stability together with the existence of low-field metastable polarization states.
View Article and Find Full Text PDFPsilocybin, a serotonergic agonist, was granted a "breakthrough therapy" status by the Food and Drug Administration for clinical trials involving major depressive disorder and treatment-resistant depression. The direct phosphorylation of psilocin to psilocybin that uses a fast crystallization associated with a kinetically controlled process resulted in a smaller particle size distribution. Herein, the measurement of the metastable zone width (MSZW) and nucleation induction enabled a thermodynamically controlled crystallization process, which leads to the formation of a crystal structure with stronger interactions, controlled particle size distribution (PSD), and improved impurity profile.
View Article and Find Full Text PDFActa Crystallogr C Struct Chem
January 2022
Psilocybin {systematic name: 3-[2-(dimethylamino)ethyl]-1H-indol-4-yl dihydrogen phosphate} is a zwitterionic tryptamine natural product found in numerous species of fungi known for their psychoactive properties. Following its structural elucidation and chemical synthesis in 1959, purified synthetic psilocybin has been evaluated in clinical trials and has shown promise in the treatment of various mental health disorders. In a recent process-scale crystallization investigation, three crystalline forms of psilocybin were repeatedly observed: Hydrate A, Polymorph A, and Polymorph B.
View Article and Find Full Text PDFACS Appl Mater Interfaces
October 2021
Narrowband terahertz (THz) radiation is crucial for high-resolution spectral identification, but a narrowband THz source driven by a femtosecond (fs) laser has remained scarce. Here, it is computationally predicted that a metal/dielectric/magnetoelastic heterostructure enables converting a fs laser pulse into a multicycle THz pulse with a narrow linewidth down to ∼1.5 GHz, which is in contrast to the single-cycle, broadband THz pulse from the existing fs-laser-excited emitters.
View Article and Find Full Text PDFMagnetostrictive materials transduce magnetic and mechanical energies and when combined with piezoelectric elements, evoke magnetoelectric transduction for high-sensitivity magnetic field sensors and energy-efficient beyond-CMOS technologies. The dearth of ductile, rare-earth-free materials with high magnetostrictive coefficients motivates the discovery of superior materials. FeGa alloys are amongst the highest performing rare-earth-free magnetostrictive materials; however, magnetostriction becomes sharply suppressed beyond x = 19% due to the formation of a parasitic ordered intermetallic phase.
View Article and Find Full Text PDFThe manipulation of antiferromagnetic order in magnetoelectric CrO using electric field has been of great interest due to its potential in low-power electronics. The substantial leakage and low dielectric breakdown observed in twinned CrO thin films, however, hinders its development in energy efficient spintronics. To compensate, large film thicknesses (250 nm or greater) have been employed at the expense of device scalability.
View Article and Find Full Text PDFA second-generation kilogram-scale synthesis of the psychedelic tryptamine psilocybin has been developed. The synthesis was designed to address several challenges first encountered with the scale-up of previously described literature procedures, which were not optimized for providing consistent yield and purity of products, atom economy, or being run in pilot plant-scale reactors. These challenges were addressed and circumvented with the design of the second-generation route, which featured an optimized cGMP large-scale Speeter-Anthony tryptamine synthesis to the intermediate psilocin with improved in-process control and impurity removal over the three steps.
View Article and Find Full Text PDFConcerted multidisciplinary efforts have led to the development of Cyclin-Dependent Kinase inhibitors (CDKi's) as small molecule drugs and chemical probes of intracellular CDK function. However, conflicting data has been reported on the inhibitory potency of CDKi's and a systematic characterization of affinity and selectivity against intracellular CDKs is lacking. We have developed a panel of cell-permeable energy transfer probes to quantify target occupancy for all 21 human CDKs in live cells, and present a comprehensive evaluation of intracellular isozyme potency and selectivity for a collection of 46 clinically-advanced CDKi's and tool molecules.
View Article and Find Full Text PDFA general synthetic method was developed to access known tryptamine natural products present in psilocybin-producing mushrooms. and experiments were then conducted to inform speculations on the psychoactive properties, or lack thereof, of the natural products. In animal models, psychedelic activity by baeocystin alone was not evident using the mouse head twitch response assay, despite its putative dephosphorylated metabolite, norpsilocin, possessing potent agonist activity at the 5-HT receptor.
View Article and Find Full Text PDFProtein kinases are intensely studied mediators of cellular signaling. While traditional biochemical screens are capable of identifying compounds that modulate kinase activity, these assays are limited in their capability of predicting compound behavior in a cellular environment. Here, we aim to bridge target engagement and compound-cellular phenotypic behavior by utilizing a bioluminescence resonance energy transfer (BRET) assay to characterize target occupancy within living cells for Bruton's tyrosine kinase (BTK).
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