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Search indexed NASA NTRS and DOE OSTI research on propulsion, heat transfer, battery materials and energy systems. Follow report and document links to the original sources.

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At least 991 records · Page 55
All sourcesNASA NTRSDOE OSTI
DOE OSTI2019

Effect of Mixed-Solvent Environments on the Selectivity of Acid-Catalyzed Dehydration Reactions

The composition of the liquid phase can alter the rates of individual reaction steps and thus alter the selectivity of acid-catalyzed reactions, but these solvent effects are difficult to anticipate for design purposes. Herein, we report the kinetics and selectivity of Brønsted acid-catalyzed 1,2-propanediol dehydration in pure water and in aqueous mixtures of the polar aprotic cosolvents γ-valerolactone, 1,4-dioxane, tetrahydrofuran, N-methyl-2-pyrrolidone, tetramethylene sulfoxide, and dimethyl sulfoxide at 433 K. We find that the major product of 1,2-propanediol dehydration is propanal in most mixed-solvent environments with selectivities between 1 and 68 mol %. In contrast, 1,2-propanediol dehydration in aqueous mixtures of dimethyl sulfoxide affords acetone as the major product with up to 48% selectivity with minimal propanal formation. We use classical molecular dynamics simulations to probe these solvent effects by computing the difference between the solvation free energies of 1,2-propanediol and propanal in aqueous mixtures of polar aprotic cosolvents and in pure water. We find that the difference in the solvation free energies is correlated with the rates of propanal formation in all mixed-solvent environments, indicating that the solvent-mediated stabilization of the product state relative to the reactant state translates to increased selectivity toward the same product. Similar agreement between simulated solvation free energies and experimental reaction rates/selectivities is established for the acid-catalyzed dehydration of cis- and trans-1,2-cyclohexanediol and 1,3-cyclohexanediol. Finally, analysis of the solvation environment around 1,2-propanediol shows that dimethyl sulfoxide uniquely competes against water to solvate reactive hydroxyl groups, which causes a change in reaction mechanism in this solvent system that leads to the formation of acetone rather than propanal. Here, these results represent a step toward the computationally efficient screening of solvent systems for acid-catalyzed, liquid-phase processes.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2026

A Chemist’s Guide to Solid-State Qubits: Diamond Color Centers as Embedded Vacancy-Centered Molecules

Diamond point defects or color centers are at the crux of solid-state quantum technology applications, from computing to sensing. Modeling molecular qubits has advanced by leaps and bounds mainly due to the advanced quantum mechanical (QM) tools in the arsenal of quantum chemists for modeling (isolated) molecular systems, which should be easily translatable for analogous systems in the solid state. Here, we simulate a series of diamond defects: a carbon vacancy (V C ) and second row substitutions that are adjacent to a V C or D C V C , with D = B, N, and O, to evaluate their magnetic and optical properties. We applied molecular orbital principles, an embedded cluster method, and a multiconfigurational QM theory to computationally characterize the above-mentioned defects for a multitude of spin, charge, and excited states. Our computational approach delivered high-quality QM insights that compare well with experiments. Furthermore, with this framework, we confirm the spin-triplets B C V C – and O C V C 0 to be analogous to N C V C – , with calculated bright transitions that respectively correspond to UV (3.80 eV) and blue (2.65 eV) light absorption and emission lifetimes (τ) of 2.3 and 5.6 ns, which are higher in energy and more short-lived (and thus brighter) than that for N C V C – : green (2.26 eV), τ = 9.5 ns.

Martirez, John Mark P. [Princeton Plasma Physics L↗
DOE OSTI2021

Interfacial Reactivity and Speciation Emerging from Na-Montmorillonite Interactions with Water and Formic Acid at 200 °C: Insights from Reactive Molecular Dynamics Simulations, Infrared Spectroscopy, and X-ray Scattering Measurements

Reactive organic fluid - mineral interactions at elevated temperatures contribute to the evolution of planetary matter. One of the less studied but important transformations in this regard involves the reactions of formic acid with naturally occurring clays such as sodium montmorillonite. To advance a mechanistic understanding of these interactions, we use ReaxFF reactive molecular dynamics simulations in conjunction with infrared (IR) spectroscopy and X-ray scattering experiments to investigate the speciation behavior of water-formic acid mixtures on sodium montmorillonite interfaces at 473 K and 1 atm. Using a newly developed reactive forcefield, we show that the experimental IR spectra of unreacted and reacted mixture can be accurately reproduced by ReaxFF/MD. We further benchmark the simulation predictions of sodium carbonate and bicarbonate formation in the clay interlayers using Small and Wide-Angle X-ray Scattering measurements. Subsequently, leveraging the benchmarked forcefield, we interrogate the pathway of speciation reactions with emphasis on carbonate, formate, and hydroxide groups elucidating the energetics, transition states, intermediates, and preferred products. Further, we also delineate the differences in reactivities and catalytic effects of clay edges, facets, and interlayers owing to their local chemical environments, which have far reaching consequences in their speciation behavior. The experimental and simulation approaches described in this study and the transferable forcefields can be applied translationally to advance the science of clay-fluid interactions for several applications including subsurface fluid storage and recovery and clay-pollutant dynamics.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2020

Forecasting the Decay of Hybrid Perovskite Performance Using Optical Transmittance or Reflected Dark-Field Imaging

The practicality and economic viability of hybrid perovskite solar cells hinge on their operational lifetime, and methods for forecasting the performance of perovskites under different operational stresses are urgently needed. Here, we explore the evolution of material-level optoelectronic properties as MAPbI 3 degrades and discover universal behaviors where the carrier diffusion length (L D ) decays before quasi-Fermi-level splitting (ΔE F ), regardless of the specific stress protocol (oxygen, humidity, thermal stress, or a combination). We employ a machine learning greedy feature selection model that uses initially measured properties to predict the time it takes L D to decrease to 85% of its initial value with a prediction accuracy of 12.8%. This model reveals a strong correlation between the initial rate of transmittance change and the time until loss of transport. We translate this material-level finding to photovoltaic device-level forecasting by demonstrating that the rate of change of transmittance is equivalent to the rate of change of the spatial standard deviation of dark-field image intensity (i.e., scattered light intensity) collected in reflection mode (and thus applicable to devices with opaque contacts). Furthermore, this work demonstrates that transmittance and scattering methods are highly effective for accelerated material (and device) stability evaluation and forecasting.

14 SOLAR ENERGY↗
DOE OSTI2022

Photoactivated p-Doping of Organic Interlayer Enables Efficient Perovskite/Silicon Tandem Solar Cells

Solution-processed organic semiconductor layers on rough surfaces tend to vary widely in thickness, significantly hindering charge extraction in relevant optoelectronic devices. Herein, we report the photoactivated p-doping of hole-transporting material (HTM) to enhance hole extraction for (textured) perovskite/silicon tandem solar cells, making the device performance less sensitive to the variation of hole transport layer thickness. We used the ionic compound 4-isopropyl-4'-methyldiphenyliodonium tetrakis(penta-fluorophenyl-borate) (DPI-TPFB) as a p-type dopant in poly(triaryl amine) (PTAA), which we used as the HTM. We observed that light soaking DPI-TPFB-doped PTAA shows approximately 22 times higher conductivity compared with an undoped PTAA film, which translated into an improved fill factor (FF) for tandem solar cells. Our tandem solar cells achieved an ~80% FF and 27.8% efficiency and operated at their maximum power point for 200 h without loss of performance, in addition to retaining ~83% of initial performance over a month of operation in an outdoor environment.

CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSICS,S↗
DOE OSTI2026

Microscopic Mechanisms of Superionic Na-ion Conductivity in Crystalline and Amorphous NaMOCl 4 (M = Nb, Ta) Solid Electrolytes

Sodium-ion solid electrolytes offer a sustainable route toward next-generation batteries, but few match the performance of their lithium counterparts. Halide-based NaMOCl 4 (M = Nb, Ta) has recently emerged as a promising analogue to LiMOCl 4 , yet its structure–transport relationships remain unclear due to poor crystallinity in experiments. Here, we combine density functional theory and machine-learned molecular dynamics to reveal that crystalline NaMOCl 4 exhibits negligible room-temperature conductivity with high activation barriers arising from vacancy-mediated diffusion below an order–disorder transition. Above this transition, rotational and translational motion of the [MO 2/2 Cl 4 – ] ∞ chains create new Na sites and enhances transport. In contrast, the amorphous phase inherently supports facile, three-dimensional Na diffusion through dynamic framework flexibility. These results show that ordered crystalline phases hinder ionic transport, while disorder – either thermally induced or structural – facilitates it, revising prior assumptions from the Li system and providing design principles for high-conductivity Na halide electrolytes.

Wei, Grace [University of California, Berkeley, CA↗
DOE OSTI2025

Predicting Liquid–Liquid Phase Separation of Submicrometer Proxies for Atmospheric Secondary Aerosol

Liquid–liquid phase separation (LLPS) of atmospheric aerosols can significantly impact climate, air quality, and human health. However, their complex composition, small size, and history-dependent properties result in great uncertainty in the modeling of aerosol phase state and atmospheric processes. Herein, using cryogenic transmission electron microscopy (cryo-TEM), we examined model submicron aerosols composed of organic compounds and ammonium sulfate, and established a parameterization for the separation relative humidity (SRH) that accounts for chemical composition, particle size, and equilibration time. We evaluated different variables that describe chemical composition: O/C ratio, partition coefficient, solubility, molar mass, and polarizability. The O/C ratio fits the SRH of micrometer droplets best, and by using a scaling factor to translate the micrometer SRH parameterization to submicron aerosols, we incorporate the effects of size and equilibration time. The measured scaling factor for the submicron mean SRH (30nm – 1μm, 20 min equilibration times) is 0.80, the factor becomes 1 with equilibration time over 1 hour, and is equal to 0, meaning that SRH is absent, when the aerosol dry diameter is smaller than 30 nm. Furthermore, our parameterization will aid in universal SRH modeling, potentially leading to more accurate predictions of aerosol mass, optical properties, hygroscopicity, and heterogeneous chemistry.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2021

Quantitative Proteomics and Quantitative PCR as Predictors of cis -1,2-Dichlorethene and Vinyl Chloride Reductive Dechlorination Rates in Bioaugmented Aquifer Microcosms

Quantitative measurement of process-specific biomarker genes of Dehalococcoides mccartyi (Dhc) supports monitoring at chlorinated ethene contaminated sites. In this study, we varied Dhc cell abundances from ~103 to 108 cells/mL in aquifer microcosms and correlated the corresponding reductive dehalogenase (RDase) gene and RDase protein abundances with measured reductive dechlorination (RD) rates of cis-1,2-dichloroethene (cDCE) and vinyl chloride (VC). An additional set of microcosms tested the RD rate-predictive power of the regression analyses. These efforts revealed (1) that targeted proteomics quantifies Dhc biomarker proteins (e.g., TceA and VcrA, OmeA) over a relevant range of Dhc cell densities, and (2) that protein and gene abundances can predict RD rates. Protein detection limits translated to a rate coefficient of 10 –4 day –1 (0.04 year –1 ) for both k cDCE and k vc , which is within the range observed at sites undergoing monitored natural attenuation (MNA) (i.e., without the implementation of enhanced bioremediation treatment). Rates predicted using a combination of quantitative biomarker gene and protein measurements generally resulted in the best match with experimentally determined rate constants. These new findings provide evidence that quantitative biomarker measurements may be useful predictors of in situ RD rates, which would constitute a major advance for the cost-effective management of contaminated sites.

42 ENGINEERING↗
DOE OSTI2020

Confined Crystal Melting in Edgeless Poly( L -lactic acid) Crystalsomes

Polymer single crystals tend to be quasi two-dimensional (2D) lamellae and their small lateral surfaces are the starting points of lamella melting and thickening. However, the recently discovered crystalsomes, which are defined for hollow single crystal-like spherical shells, are edgeless, self-confined, and incommensurate with translational symmetry. Here, this work concerns the structure and melting behavior of these edgeless crystalsomes. Poly(l-lactic acid) crystalsomes were grown using a miniemulsion solution crystallization method. Differential scanning calorimetry and in situ wide-angle X-ray diffraction were used to follow the structural evolution of the crystalsomes upon heating. Our results demonstrated that the structure and melting behavior of crystalsomes are curvature-dependent and significantly different from their flat crystal counterpart.

36 MATERIALS SCIENCE↗
DOE OSTI2020

The Role of Dimer Formation in the Nucleation of Superlattice Transformations and Its Impact on Disorder

The formation of defect-free two-dimensional nanocrystal (NC) superstructures remains a challenge as persistent defects hinder charge delocalization and related device performance. Understanding defect formation is an important step toward developing strategies to mitigate their formation. However, specific mechanisms of defect formation are difficult to determine, as superlattice phase transformations that occur during fabrication are quite complex and there are a variety of factors influencing the disorder in the final structure. Here, we use Molecular Dynamics (MD) and electron microscopy in concert to investigate the nucleation of the epitaxial attachment of lead chalcogenide (PbX, where X = S, Se) NC assemblies. We use an updated implementation of an existing reactive force field in an MD framework to investigate how initial orientational (mis)alignment of the constituent building blocks impacts the final structure of the epitaxially connected superlattice. This Simple Molecular Reactive Force Field (SMRFF) captures both short-range covalent forces and long-range electrostatic forces and allows us to follow orientational and translational changes of NCs during superlattice transformation. Our simulations reveal how robust the oriented attachment is with regard to the initial configuration of the NCs, measuring its sensitivity to both in-plane and out-of-plane misorientation. We show that oriented attachment nucleates through the initial formation of dimers, which corroborate experimentally observed structures. We present high-resolution structural analysis of dimers at early stages of the superlattice transformation and rationalize their contribution to the formation of defects in the final superlattice. Collectively, the simulations and experiments presented in this paper provide insights into the nucleation of NC oriented attachment, the impact of the initial configuration of NCs on the structural fidelity of the final epitaxially connected superlattice, and the propensity to form commonly observed defects, such as missing bridges and atomic misalignment in the superlattice due to the formation of dimers. Here, we present potential strategies to mitigate the formation of superlattice defects.

36 MATERIALS SCIENCE↗
DOE OSTI2020

Hypothetical Efficiency of Electrical to Mechanical Energy Transfer during Individual Stochastic Molecular Switching Events

There are now many examples of single molecule rotors, motors and switches in the literature that, when driven by photons, electrons or chemical reactions, exhibit well defined motions. As a step towards using these single molecule devices to perform useful functions one must understand how they interact with their environment and quantify their ability to perform work on it. Using a single molecule rotary switch we examine the transfer of electrical energy, delivered via electron tunneling, to mechanical motion and measure the forces the switch experiences with a non-contact q-plus atomic force microscope. Action spectra reveal that the molecular switch has two stable states and can be excited resonantly between them at a bias of 100 mV via a one-electron inelastic tunneling process which corresponds to an energy input of 16 zepto Joules. Furthermore, while the electrically induced switching events are stochastic and no net work is to done on the cantilever, by measuring the forces between the molecular switch and the AFM cantilever we can derive the maximum hypothetical work the switch could perform during a single switching event which is ~55 meV, equal to 8.9 zepto Joules which translates to a hypothetical efficiency ~55% per individual inelastic tunneling electron induced switching event. When co considering the total electrical energy input this drops to 1x10 -7 % due to elastic tunneling events that dominate the tunneling current. However, this approach constitutes a general method for quantifying and comparing the energy input and output of molecularmechanical devices.

36 MATERIALS SCIENCE↗
DOE OSTI2020

Colloidal Synthesis Path to 2D Crystalline Quantum Dot Superlattices

By combining colloidal nanocrystal synthesis, self-assembly, and solution phase epitaxial growth techniques, we developed a general method for preparing single dot thick atomically attached quantum dot (QD) superlattices with high-quality translational and crystallographic orientational order along with state-of-the-art uniformity in the attachment thickness. The procedure begins with colloidal synthesis of hexagonal prism shaped core/shell QDs (e.g., CdSe/CdS), followed by liquid subphase self-assembly and immobilization of superlattices on a substrate. Solution phase epitaxial growth of additional semiconductor material fills in the voids between the particles, resulting in a QD-in-matrix structure. The photoluminescence emission spectra of the QD-in-matrix structure retains characteristic 0D electronic confinement. Importantly, annealing of the resulting structures removes inhomogeneities in the QD–QD inorganic bridges, which our atomistic electronic structure calculations demonstrate would otherwise lead to Anderson-type localization. The piecewise nature of this procedure allows one to independently tune the size and material of the QD core, shell, QD–QD distance, and the matrix material. These four choices can be tuned to control many properties (degree of quantum confinement, quantum coupling, band alignments, etc.) depending on the specific applications. Lastly, cation exchange reactions can be performed on the final QD-in-matrix, as demonstrated herein with a CdSe/CdS to HgSe/HgS conversion.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2021

Coherent Electronic Band Structure of TiTe 2 /TiSe 2 Moiré Bilayer

Here, a van der Waals bonded moiré bilayer formed by sequential growth of TiSe 2 and TiTe 2 monolayers exhibits emergent electronic structure as evidenced by angle-resolved photoemission band mapping. The two monolayers adopt the same lattice orientation but incommensurate lattice constants. Despite the lack of translational symmetry, sharp dispersive bands are observed. The dispersion relations appear distinct from those for the component monolayers alone. Theoretical calculations illustrate the formation of composite bands by coherent electronic coupling despite the weak interlayer bonding, which leads to band renormalization and energy shifts.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2022

Observation of an Orientational Glass in a Superlattice of Elliptically-Faceted CdSe Nanocrystals

Extensive prior work has shown that colloidal inorganic nanocrystals coated with organic ligand shells can behave as artificial atoms and, as such, form superlattices with different crystal structures and packing densities. Although ordered superlattices present a high degree of long-range positional order, the relative crystallographic orientation of the inorganic nanocrystals with respect to each other tends to be random. Recent works have shown that superlattices can achieve orientational alignment through combinations of nanocrystal faceting and ligand modification, as well as selective metal particle attachment to particular facets. These studies have focused on the assembly of high-symmetry nanocrystals, such as cubes and cuboctahedra. In this work, we study the assembly of elliptically faceted CdSe/CdS core/shell nanocrystals with one distinctive crystallographic orientation along the major elliptical axis. We show that the nanocrystals form an unexpectedly well-ordered translational superlattice, with a degree of order comparable to that achieved with higher-symmetry nanocrystals. Additionally, we show that, due to the particles' faceted shape, the superlattice is characterized by an orientational glass phase in which only certain orientations are possible due to entropically frustrated crystallization. In this phase, the nanocrystals do not exhibit a local orientational ordering but rather have distinct orientations that emerge at different locations within the same domain. The distinct orientations are a result of a facet-to-facet lock-in mechanism that occurs during the self-assembly process. These facet-to-facet alignments force the nanocrystals to tilt on different lattice planes forming different projections that we termed apparent polydispersity. Our experimental realization of an orientational glass phase for multifaceted semiconducting nanocrystals can be used to investigate how this phase is formed and how it can be utilized for potential optical, electrical, and thermal transport applications.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2022

Bayesian Active Learning for Scanning Probe Microscopy: From Gaussian Processes to Hypothesis Learning

Recent progress in machine learning methods and the emerging availability of programmable interfaces for scanning probe microscopes (SPMs) have propelled automated and autonomous microscopies to the forefront of attention of the scientific community. However, enabling automated microscopy requires the development of task-specific machine learning methods, understanding the interplay between physics discovery and machine learning, and fully defined discovery workflows. This, in turn, requires balancing the physical intuition and prior knowledge of the domain scientist with rewards that define experimental goals and machine learning algorithms that can translate these to specific experimental protocols. Here, we discuss the basic principles of Bayesian active learning and illustrate its applications for SPM. We progress from the Gaussian process as a simple data-driven method and Bayesian inference for physical models as an extension of physics-based functional fits to more complex deep kernel learning methods, structured Gaussian processes, and hypothesis learning. These frameworks allow for the use of prior data, the discovery of specific functionalities as encoded in spectral data, and exploration of physical laws manifesting during the experiment. Here, the discussed framework can be universally applied to all techniques combining imaging and spectroscopy, SPM methods, nanoindentation, electron microscopy and spectroscopy, and chemical imaging methods and can be particularly impactful for destructive or irreversible measurements.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2022

Dual Atomic Coherence in the Self-Assembly of Patchy Heterostructural Nanocrystals

Advances in the synthesis and self-assembly of nanocrystals have enabled researchers to create a plethora of different nanoparticle superlattices. But while many super lattices with complex types of translational order have been realized, rotational order of nanoparticle building blocks within the lattice is more difficult to achieve. Self-assembled superstructures with atomically coherent nanocrystal lattices, which are desirable due to their exceptional electronic and optical properties, have been fabricated only for a few selected systems. Here, we combine experiments with molecular dynamics (MD) simulations to study the self-assembly of heterostructural nanocrystals (HNCs), consisting of a near-spherical quantum dot (QD) host decorated with a small number of epitaxially grown gold nanocrystal (Au NC) "patches ". Self-assembly of these HNCs results in face-centered-cubic (fcc) superlattices with well-defined orientational relationships between the atomic lattices of both QD hosts and Au patches. MD simulations indicate that the observed dual atomic coherence is linked to the number, size, and relative positions of gold patches. Here this study provides a strategy for the design and fabrication of NC superlattices with large structural complexity and delicate orientational order.

77 NANOSCIENCE AND NANOTECHNOLOGY↗
DOE OSTI2023

High-Resolution X-ray Spectromicroscopy Reveals Process-Structure Correlations in sub-5-μm Diameter Carbon Nanotube-Polymer Composite Dry-Spun Yarns

A persistent lack of detailed and quantitative structural analysis of these hierarchical carbon nanotube (CNT) ensembles precludes establishing processing-structure-property relationships that are essential to enhance macroscale performance (e.g., in mechanical, electrical, thermal applications). Here, in this work, we use scanning transmission X-ray microscopy (STXM) to analyze the hierarchical, twisted morphology of dry-spun CNT yarns and their composites, quantifying key structural characteristics such as density, porosity, alignment, and polymer loading. As the yarn twist density increases (15,000 to 150,000 turns per meter), the yarn diameter decreased (4.4–1.4 μm) and density increased (0.55–1.26 g·cm –3 ), as intuitively expected. Yarn density, ρ, ubiquitously scaled with diameter d according to ρ ~ d –2 for all parameters studied here. Spectromicroscopy probes with 30 nm resolution and elemental specificity were employed to analyze the radial and longitudinal distribution of the oxygen-containing polymer content (~30% weight fraction), demonstrating nearly perfect filling of the voids between CNTs with a vapor-phase polymer coating and cross-linking process. These quantitative correlations highlight the intimate connections between processing conditions and yarn structure with important implications for translating the nanoscale properties of CNTs to the macroscale.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2023

Bottlebrush Polymers at Liquid Interfaces: Assembly Dynamics, Mechanical Properties, and All-Liquid Printed Constructs

Bottlebrush polymer surfactants (BPSs), formed by the interfacial interactions between bottlebrush polymers (BPs) with poly(acrylic acid) side chains dissolved in an aqueous phase and amine-functionalized ligands dissolved in the oil phase, assemble and bind strongly to the fluid-fluid interface. The ratio between N BB (backbone degree of polymerization) and N SC (side chain degree of polymerization) defines the initial assembly kinetics, interface packing efficiency, and stress relaxation. The equilibrium interfacial tension (γ) increases when N BB < N SC , but decreases when N BB $\gg$ N SC , correlating to a pronounced change in the effective shape of the BPs from being spherical to worm-like structures. The apparent surface coverage (ASC), i.e., the interfacial packing efficiency, decreases as N BB increases. The dripping-to-jetting transition of an injected polymer solution, as well as fluorescence recovery after photobleaching experiments, revealed faster initial assembly kinetics for BPs with higher N BB . Furhter, Euler buckling of BPS assemblies with different N BB values was used to characterize the stress relaxation behavior and bending modulus. The stress relaxation behavior was directly related to the ASC, reflecting the strong influence of macromolecular shape on packing efficiency. The bending modulus of BPSs decreases for N BB < N SC , but increased when N BB $\gg$ N SC , showing the effect of molecular architecture and multisite anchoring. All-liquid printed constructs with lower N BB BPs yielded more stable structured liquids, underscoring the importance of macromolecular packing efficiency at fluid interfaces. Overall, this work elucidates fundamental relationships between nanoscopic structures and macroscopic properties associated with various bottlebrush polymer architectures, which translate to the stabilization of all-fluidic printed constructs.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗