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  1. Abstract

    Kagome vanadatesAV3Sb5display unusual low-temperature electronic properties including charge density waves (CDW), whose microscopic origin remains unsettled. Recently, CDW order has been discovered in a new material ScV6Sn6, providing an opportunity to explore whether the onset of CDW leads to unusual electronic properties. Here, we study this question using angle-resolved photoemission spectroscopy (ARPES) and scanning tunneling microscopy (STM). The ARPES measurements show minimal changes to the electronic structure after the onset of CDW. However, STM quasiparticle interference (QPI) measurements show strong dispersing features related to the CDW ordering vectors. A plausible explanation is the presence of a strong momentum-dependent scattering potential peaked at the CDW wavevector, associated with the existence of competing CDW instabilities. Our STM results further indicate that the bands most affected by the CDW are near vHS, analogous to the case ofAV3Sb5despite very different CDW wavevectors.

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    Free, publicly-accessible full text available December 1, 2025
  2. In recent years, nanocellulose has emerged as a sustainable and environmentally friendly alternative to traditional petroleum-derived structural polymers. Sourced either from plants, algae, or bacteria, nanocellulose can be processed into colloid, gel, film and fiber forms. However, the required fundamental understanding of process parameters that govern the morphology and structure–property relationships of nanocellulose systems, from colloidal suspensions to bulk materials, has not been developed and generalized for all forms of cellulose. This further hinders the more widespread adoption of this biopolymer in applications. Our study investigates the dispersion of cellulose nanofibers (CNFs) produced by a bacterial–yeast co-culture, in solvents, highlighting the role of thermodynamic interactions in influencing their colloidal behavior. By adjusting Hansen solubility parameters, we controlled the thermodynamic relationship between CNFs and solvents across various concentrations, studying the dilute to semi-dilute regimes. Rheological measurements revealed that the threshold at which a concentration-based regime transition occurs is distinctly solvent-dependent. Complementing rheological analysis with small angle X-ray scattering and zeta potential measurements, our findings reveal that enhancing CNF–solvent interactions increases excluded volume in the dilute regime, emphasizing the importance of the balance between fiber–fiber and fiber–solvent interactions. Moreover, we investigated the transition from colloidal to solid state by creating films from dispersions with varying interaction parameters in semi-dilute regimes. Through mechanical testing and scanning electron microscopy imaging of the fracture surfaces, we highlight the significance of electrokinetic effects in such transitions, as dispersions with higher electrokinetic stabilization gave rise to stronger and tougher films despite having less favorable thermodynamic interaction parameters. Our work provides insights into the thermodynamic and electrokinetic interplay that governs bacterial CNF dispersion, offering a foundation for future application and a deeper understanding of nanocellulose's colloidal and structure-property relationships. 
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    Free, publicly-accessible full text available January 1, 2025
  3. Thin metal particles with two-dimensional symmetry are attractive for multiple ap- plications, but are difficult to synthesize in a reproducible manner. Although molecules that selectively adsorb to facets have been used to control nanoparticle shape, there is still limited research into the temporal control of growth processes to control these structural outcomes. Moreover, much of the current research into the growth of thin two-dimensional particles lacks mechanistic details. In this work, we study why the substitution of isoleucine for methionine in a gold binding peptide (Z2, RMRMKMK) results in an increase in gold nanoparticle anisotropy. Nanoplatelet growth in the pres- ence of Z2M246I (RIRIKIK) is characterized using in situ small-angle X-ray scattering (SAXS) and UV-Vis spectroscopy. Fitting time-resolved SAXS profiles reveals that 10 nm thick particles with two-dimensional symmetry are formed within the first few min- utes of the reaction. Next, through a combination of electron diffraction and molecular dynamics simulations, we show that substitution of methionine for isoluecine increases the (111) facet selectivity in Z2M246I, and conclude that this is key to the growth of nanoplatelets. However, the potential application of nanoplatelets formed using Z2M246I is limited due to their uncontrolled lateral growth, aggregation, and rapid sedimentation. Therefore, we use a liquid handling robot to perform temporally con- trolled synthesis and dynamic intervention through the addition of Z2 to nanoplatelets growing in the presence of Z2M246I at different times. UV-Vis spectroscopy dynamic light scattering, and electron microscopy show that dynamic intervention results in control over the mean-size and stability of plate-like particles. Finally, we use in situ UV-Vis spectroscopy to study plate-like particle growth at different times of interven- tion. Our results demonstrate that both the selectivity and magnitude of binding free energy towards lattices is important for controlling nanoparticle growth pathways. 
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    Free, publicly-accessible full text available November 1, 2024