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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 OSTI2020

Excluded-volume model for quarkyonic matter: Three-flavor baryon-quark mixture

The single-flavor excluded-volume model based on the effective size of baryons reproduces the hard-soft density evolution of the equation of state (EoS) required by the recent studies of GW170817. This phenomenological model basically realizes the concept of quarkyonic matter which is introduced from large-$N_c$ gauge theory for dense matter. Further, enhanced nucleon interactions and dynamically generated quark degrees of freedom can reproduce the hard-soft evolution of the EoS. In this paper, we extend the excluded-volume model to a three-flavor system by considering electromagnetic charge and possible weak equilibrium in order to obtain a proper description for the hard-soft behavior of the EoS inferred from the gravitational waves observations.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2022

Multi-objective optimization of root phenotypes for nutrient capture using evolutionary algorithms

Root phenotypes are avenues to the development of crop cultivars with improved nutrient capture, which is an important goal for global agriculture. The fitness landscape of root phenotypes is highly complex and multidimensional. It is difficult to predict which combinations of traits (phene states) will create the best performing integrated phenotypes in various environments. Brute force methods to map the fitness landscape by simulating millions of phenotypes in multiple environments are computationally challenging. Evolutionary optimization algorithms may provide more efficient avenues to explore high dimensional domains such as the root phenotypic space. We coupled the three-dimensional functional–structural plant model, SimRoot, to the Borg Multi-Objective Evolutionary Algorithm (MOEA) and the evolutionary search over several generations facilitated the identification of optimal root phenotypes balancing trade-offs across nutrient uptake, biomass accumulation, and root carbon costs in environments varying in nutrient availability. Our results show that several combinations of root phenes generate optimal integrated phenotypes where performance in one objective comes at the cost of reduced performance in one or more of the remaining objectives, and such combinations differed for mobile and non-mobile nutrients and for maize (a monocot) and bean (a dicot). Functional–structural plant models can be used with multi-objective optimization to identify optimal root phenotypes under various environments, including future climate scenarios, which will be useful in developing the more resilient, efficient crops urgently needed in global agriculture.

59 BASIC BIOLOGICAL SCIENCES↗
DOE OSTI2021

Symbiont-Mediated Protection of Acromyrmex Leaf-Cutter Ants from the Entomopathogenic Fungus Metarhizium anisopliae

Many fungus-growing ants engage in a defensive symbiosis with antibiotic-producing ectosymbiotic bacteria in the genus Pseudonocardia, which help protect the ants’ fungal mutualist from a specialized mycoparasite, Escovopsis. Here, using germfree ant rearing and experimental pathogen infection treatments, we evaluate if Acromyrmex ants derive higher immunity to the entomopathogenic fungus Metarhizium anisopliae from their Pseudonocardia symbionts. We further examine the ecological dynamics and defensive capacities of Pseudonocardia against M. anisopliae across seven different Acromyrmex species by controlling Pseudonocardia acquisition using ant-nonnative Pseudonocardia switches, in vitro challenges, and in situ mass spectrometry imaging (MSI). We show that Pseudonocardia protects the ants against M. anisopliae across different Acromyrmex species and appears to afford higher protection than metapleural gland (MG) secretions. Although Acromyrmex echinatior ants with nonnative Pseudonocardia symbionts receive protection from M. anisopliae regardless of the strain acquired compared with Pseudonocardia-free conditions, we find significant variation in the degree of protection conferred by different Pseudonocardia strains. Additionally, when ants were reared in Pseudonocardia-free conditions, some species exhibit more susceptibility to M. anisopliae than others, indicating that some ant species depend more on defensive symbionts than others. In vitro challenge experiments indicate that Pseudonocardia reduces Metarhizium conidiospore germination area. Our chemometric analysis using matrix-assisted laser desorption/ionization mass spectrometry imaging (MALDI-MSI) reveals that Pseudonocardia-carrying ants produce more chemical signals than Pseudonocardia-free treatments, indicating that Pseudonocardia produces bioactive metabolites on the Acromyrmex cuticle. Our results indicate that Pseudonocardia can serve as a dual-purpose defensive symbiont, conferring increased immunity for both the obligate fungal mutualist and the ants themselves.

59 BASIC BIOLOGICAL SCIENCES↗
DOE OSTI2017

Molecular Characterization of N-glycan Degradation and Transport in Streptococcus pneumoniae and Its Contribution to Virulence

The carbohydrate-rich coating of human tissues and cells provide a first point of contact for colonizing and invading bacteria. Commensurate with N-glycosylation being an abundant form of protein glycosylation that has critical functional roles in the host, some host-adapted bacteria possess the machinery to process N-linked glycans. The human pathogen Streptococcus pneumoniae depolymerizes complex N-glycans with enzymes that sequentially trim a complex N-glycan down to the Man 3 GlcNAc 2 core prior to the release of the glycan from the protein by endo-β-N-acetylglucosaminidase (EndoD), which cleaves between the two GlcNAc residues. Here we examine the capacity of S. pneumoniae to process high-mannose N-glycans and transport the products. Through biochemical and structural analyses we demonstrate that S. pneumoniae also possesses an α-(1,2)-mannosidase (SpGH92). This enzyme has the ability to trim the terminal α-(1,2)-linked mannose residues of high-mannose N-glycans to generate Man 5 GlcNAc 2 . Through this activity SpGH92 is able to produce a substrate for EndoD, which is not active on high-mannose glycans with α-(1,2)-linked mannose residues. Binding studies and X-ray crystallography show that NgtS, the solute binding protein of an ABC transporter (ABC NG ), is able to bind Man 5 GlcNAc, a product of EndoD activity, with high affinity. Finally, we evaluated the contribution of EndoD and ABC NG to growth of S. pneumoniae on a model N-glycosylated glycoprotein, and the contribution of these enzymes and SpGH92 to virulence in a mouse model. We found that both EndoD and ABC NG contribute to growth of S. pneumoniae, but that only SpGH92 and EndoD contribute to virulence. Therefore, N-glycan processing, but not transport of the released glycan, is required for full virulence in S. pneumoniae. To conclude, we synthesize our findings into a model of N-glycan processing by S. pneumoniae in which both complex and high-mannose N-glycans are targeted, and in which the two arms of this degradation pathway converge at ABC NG .

59 BASIC BIOLOGICAL SCIENCES↗
DOE OSTI2016

Evaluation of Simulated Marine Aerosol Production Using the WaveWatchIII Prognostic Wave Model Coupled to the Community Atmosphere Model within the Community Earth System Model

Primary marine aerosol (PMA) is emitted into the atmosphere via breaking wind waves on the ocean surface. Most parameterizations of PMA emissions use 10-meter wind speed as a proxy for wave action. This investigation coupled the 3 rd generation prognostic WAVEWATCH-III wind-wave model within a coupled Earth system model (ESM) to drive PMA production using wave energy dissipation rate – analogous to whitecapping – in place of 10-meter wind speed. The wind speed parameterization did not capture basin-scale variability in relations between wind and wave fields. Overall, the wave parameterization did not improve comparison between simulated versus measured AOD or Na + , thus highlighting large remaining uncertainties in model physics. Results confirm the efficacy of prognostic wind-wave models for air-sea exchange studies coupled with laboratory- and field-based characterizations of the primary physical drivers of PMA production. No discernible correlations were evident between simulated PMA fields and observed chlorophyll or sea surface temperature.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2016

Seasonal controls on dynamic hyporheic zone redox biogeochemistry

Hyporheic zones (where surface water and groundwater mix in streambeds) play a critical role in the movement of chemicals within watersheds, particularly in upland headwater streams. Seasonal hydrology controls the expansion and contraction of hyporheic zones, with greater downwelling oxic river water influence during periods of peak river discharge (linked to snowmelt), and greater influence of upwelling anoxic groundwater during periods of low- and base-flow. Through this work, we aimed to quantify upwelling and downwelling fluxes across seasons and assess the impact of these dynamics on microbial community assembly and geochemical gradients at East River, Colorado. Further, we performed high spatial resolution sampling to capture heterogeneous mixing patterns around a characteristic meander on the river and developed reactive transport models to explain seasonal patterns of manganese (Mn) cycling in riverbed sediments. We were able to measure a dominant period of downwelling river water associated with high river discharge in Spring 2017 that led to the mixing of microbial communities across a 60-cm depth profile through the riverbed at three locations around the meander, and higher rates of aerobic respiration via delivery of dissolved oxygen (O2) and dissolved organic carbon (DOC). Conversely, we demonstrated that depth-resolved microbial communities became more distinct and stratified across a depth gradient during periods of low- and base-flow when upwelling groundwater exerted more influence in the riverbed. We also observed an increase in Mn concentrations within deeper streambed sediments during the baseflow season. Reactive transport models were developed to understand seasonal changes in Mn cycling in the streambed because Mn oxides influence the mobility of other metals in streams. In field observations and models, dissolved Mn is flushed from the streambed during spring snowmelt. A shift to upwelling conditions over the subsequent baseflow period allows for groundwater rich in dissolved Mn to mix with oxygenated river water in the shallow subsurface, resulting in net accumulation of Mn-oxides until the bed freezes in winter. We also developed models for hydrograph scenarios with snowmelt events of various size and timing. Our scenarios suggest that in years with less snowpack and a longer baseflow season, Mn oxidation will be favored in the upper riverbed sediments over more of the year, which may increase the sorption capacity of the streambed for other metals. Finally, we assessed fine-scale geochemical and hydrologic heterogeneity in the meandering riverbed by sampling pore water at 20 cm depth across more than 100 locations in August 2018. Sample locations span distinct zones of up-welling groundwater that contrast against dominant down-welling conditions. Clear differences in carbon quality and concentrations of redox sensitive solutes were detected between these zones, highlighting the importance of understanding heterogeneity at small scales across streambeds. Geochemical differences were associated with differences in microbial assemblage, but microbial diversity was generally uniform and high across all locations at the same depth, regardless of the extent of groundwater influence.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2019

Development of X-Ray FEL Oscillators with Higher Out-Coupling Efficiency

This program focused on the development of high-outcoupling efficiency resonators for x-ray free-electron laser oscillators (XFELOs). The goal was to produce a viable design for an XFELO that can be implemented on the LCLS-II which is the x-ray FEL facility under construction at the Stanford Linear Accelerator Center (SLAC). The program designed at regenerative amplifier (RAFEL) design that employs a high-gain undulator with a low-Q resonator with the goal of producing a scientific design for the RAFEL as well as a software suite that can be used to design XFELOs. The Phase I program considered a resonator consisting of six diamond Bragg reflectors/mirrors with two focusing lenses. This resonator was used in conjunction with the electron beam produced by the LCLS-II and the HXR undulator to design a RAFEL producing 3.05 keV photons in the fundamental resonance and 9.15 keV photons in the 3rd harmonic. The research program included the extension of the Optics Propagation Code (OPC) to describe Bragg reflection from diamond crystal mirrors and went on to use OPC, in conjunction with the MINERVA simulation code to treat the undulator interaction, to simulate the RAFEL. Simulations were conducted in both the steady-state and time-dependent regimes to determine the basic performance characteristics of the RAFEL.

43 PARTICLE ACCELERATORS↗
DOE OSTI2019

High Momentum Transfer Nucleon Elastic Electromagnetic Form Factor Measurements Using Super BigBite Spectrometer at Jefferson Lab

The nucleons - protons and neutrons - are the basic building blocks of atomic nuclei. We now know that the nucleon consists of fundamental particles called quarks and gluons. The quarks interact with each other by exchanging gluons via the strong interaction. Understanding the quark-gluon structure of the nucleon, especially the confinement of quarks within the nucleon in its ground state, remains one of the main unsolved puzzles of particle physics. The nucleon electromagnetic form factors are directly related to the internal structure of the nucleon. A new generation of high precision experiments, GEp-V, GEn-II, GEn-RP, and GMn, measuring the ground state nucleon space-like electro-magnetic form factor at high momentum transfer is underway at Jefferson Lab experimental Hall-A as part of the Super Bigbite Spectrometer (SBS) program. This series of experiments will provide a new level of understanding of the nucleon structure. These experiments are highly demanding due to the extremely fast drop off of the elastic cross section with the increasing four-momentum transfer squared(Q2). This thesis provides an overview of the SBS physics program and reports on the extensive R&D program carried out to achieve the high rate running conditions essential for carrying out the SBS experiments. SBS will provide an intermediate solid angle of approximately 35 msr, which is significantly larger than the solid angle of other dipole based spectrometers at Jefferson lab. Of course, there are much larger acceptance spectrometers at Jefferson Lab, CLAS12 for example. What is special about SBS is that it provides a sizable acceptance while operating at the highest possible luminosity at Jefferson Lab. With this combination of medium acceptance and the highest available luminosity, SBS provides an unparalleled opportunity to explore the nucleon in its ground state with unprecedented resolution. The relatively large acceptance of SBS is achieved by using a large gap dipole magnet and placing it close to the target. An unavoidable consequence of this is that the SBS GEM trackers and other detectors have a clear line-of-sight view of the target and a portion of the beam-line. As a result, the background hit rate in the SBS front GEM trackers is expected to be up to 500 kHz/cm2, over the entire active area of 6000 cm2. To the best of our knowledge, this extremely high rate over such a large area is unprecedented in any particle tracking system used anywhere in the world before. Correctly reconstructing the particle tracks of interest in this very high background environment is achieved by using especially adapted high rate techniques at every step of the tracking process: optimizing the GEM module and tracker design at the hardware level, using high bandwidth electronics and real time Field Programmable Gate Array (FPGA) based background suppression techniques at the Data Acquisition (DAQ) level, and developing highly specialized tracking algorithms to pick out the signal hits from among the vast amount of background hits. In order to ensure a smooth start and running of the SBS experiments, it is extremely crucial that these techniques are developed, implemented, and tested under realistic conditions well before the actual start of the SBS experimental program. A detailed Geant4 simulation of the experiment was combined with a digitization package to generate the detector level pseudodata similar to what is expected in the actual experiments. The digitization procedures were calibrated against actual GEM data from cosmic-ray runs, X-ray tests, beam test runs in experimental Hall-A, and the PRad experiment in Hall B. Then, optimized tracking algorithms were developed and implemented in an analysis program used to analyze these pseudo-data and to extract expected high-level parameters. These extracted quantities were then compared with the input parameters from the simulation to verify and determine the performance characteristics for the SBS tracker. From this work, a final tracking efficiency of 69% at 25% occupancy was achieved, with the required reconstruction accuracy, for the GMn experiment, the first experiment in the SBS program, with background level at 100 kHz/cm2. These demonstrated parameters are adequate for the successful running of not only the GMn experiment but as well as for GEn-RP and GEn-II experiments, the second and third experiments in the program. This work builds the solid ground to further improve the tracking performance for these experiments and achieve similar conditions for the running of the GEp-V experiment, the most demanding experiment in the SBS program, with an expected background level at 500 kHz/cm2.

Di, Danning↗
DOE OSTI2016

Two poplar-associated bacterial isolates induce additive favorable responses in a constructed plant-microbiome system

Here, the biological function of the plant-microbiome system is the result of contributions from the host plant and microbiome members. In this work we study the function of a simplified community consisting of Pseudomonas and Burkholderia bacterial strains isolated from Populus hosts and inoculated on axenic Populus cutting in controlled laboratory conditions. Inoculation individually with either bacterial isolate increased root growth relative to uninoculated controls. Root area, photosynthetic efficiency, gene expression and metabolite expression data in individual and dual inoculated treatments indicate that the effects of these bacteria are unique and additive, suggesting that the function of a microbiome community may be predicted from the additive functions of the individual members.

59 BASIC BIOLOGICAL SCIENCES↗
DOE OSTI2023

Mass Spectral Imaging to Map Plant–Microbe Interactions

Plant–microbe interactions are of rising interest in plant sustainability, biomass production, plant biology, and systems biology. These interactions have been a challenge to detect until recent advancements in mass spectrometry imaging. Plants and microbes interact in four main regions within the plant, the rhizosphere, endosphere, phyllosphere, and spermosphere. This mini review covers the challenges within investigations of plant and microbe interactions. We highlight the importance of sample preparation and comparisons among time-of-flight secondary ion mass spectroscopy (ToF-SIMS), matrix-assisted laser desorption/ionization (MALDI), laser desorption ionization (LDI/LDPI), and desorption electrospray ionization (DESI) techniques used for the analysis of these interactions. Using mass spectral imaging (MSI) to study plants and microbes offers advantages in understanding microbe and host interactions at the molecular level with single-cell and community communication information. More research utilizing MSI has emerged in the past several years. We first introduce the principles of major MSI techniques that have been employed in the research of microorganisms. An overview of proper sample preparation methods is offered as a prerequisite for successful MSI analysis. Traditionally, dried or cryogenically prepared, frozen samples have been used; however, they do not provide a true representation of the bacterial biofilms compared to living cell analysis and chemical imaging. New developments such as microfluidic devices that can be used under a vacuum are highly desirable for the application of MSI techniques, such as ToF-SIMS, because they have a subcellular spatial resolution to map and image plant and microbe interactions, including the potential to elucidate metabolic pathways and cell-to-cell interactions. Promising results due to recent MSI advancements in the past five years are selected and highlighted. The latest developments utilizing machine learning are captured as an important outlook for maximal output using MSI to study microorganisms.

59 BASIC BIOLOGICAL SCIENCES↗
DOE OSTI2012

Influence of vitamin B auxotrophy on nitrogen metabolism in eukaryotic phytoplankton

While nitrogen availability is known to limit primary production in large parts of the ocean, vitamin starvation amongst eukaryotic phytoplankton is becoming increasingly recognized as an oceanographically relevant phenomenon. Cobalamin (B12) and thiamine (B1) auxotrophy are widespread throughout eukaryotic phytoplankton, with over 50% of cultured isolates requiring B12 and 20% requiring B1. The frequency of vitamin auxotrophy in harmful algal bloom species is even higher. Instances of colimitation between nitrogen and B vitamins have been observed in marine environments, and interactions between these nutrients have been shown to impact phytoplankton species composition. This review surveys available data, including relevant gene expression patterns, to evaluate the potential for interactive effects of nitrogen and vitamin B12 and B1 starvation in eukaryotic phytoplankton. B12 plays essential roles in amino acid and one-carbon metabolism, while B1 is important for primary carbohydrate and amino acid metabolism and likely useful as an anti-oxidant. Here we will focus on three potential metabolic interconnections between vitamin, nitrogen, and sulfur metabolism that may have ramifications for the role of vitamin and nitrogen scarcities in driving ocean productivity and species composition. These include: (1) B12, B1, and N starvation impacts on osmolyte and antioxidant production, (2) B12 and B1 starvation impacts on polyamine biosynthesis, and (3) influence of B12 and B1 starvation on the diatom urea cycle and amino acid recycling through impacts on the citric acid cycle. We evaluate evidence for these interconnections and identify oceanographic contexts in which each may impact rates of primary production and phytoplankton community composition. Major implications include that B12 and B1 deprivation may impair the ability of phytoplankton to recover from nitrogen starvation and that changes in vitamin and nitrogen availability may synergistically impact harmful algal bloom formation.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2016

Matter power spectrum in hidden neutrino interacting dark matter models: a closer look at the collision term

Dark Matter (DM) models providing possible alternative solutions to the small-scale crisis of the standard cosmology are nowadays of growing interest. We consider DM interacting with light hidden fermions via well-motivated fundamental operators showing the resultant matter power spectrum is suppressed on subgalactic scales within a plausible parameter region. Our basic description of the evolution of cosmological perturbations relies on a fully consistent first principles derivation of a perturbed Fokker-Planck type equation, generalizing existing literature. The cosmological perturbation of the Fokker-Planck equation is presented for the first time in two different gauges, where the results transform into each other according to the rules of gauge transformation. Furthermore, our focus lies on a derivation of a broadly applicable and easily computable collision term showing important phenomenological differences to other existing approximations. As one of the main results and concerning the small-scale crisis, we show the equal importance of vector and scalar boson mediated interactions between the DM and the light fermions.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2020

Laser Plasma Interaction in the MG Magnetic Field (Final Report)

Strong magnetic fields change properties of plasma. Employment of the magnetic fields can improve conditions for inertial confinement fusion. Compression and heating of the magnetized plasma is a base of the MagLIF pulsed power approach to the controlled fusion. Study of expansion and heating of plasma in the external magnetic fields, development of plasma instabilities, parametric and other effects are important for basic physics and applications. The main goal of the research for the grant was experimental investigation of laser produced plasma in the well characterized and controlled MG magnetic fields. We developed a platform for investigation of high intensity laser-plasma interaction (LPI) in the MG fields using a university-scale pulsed power machine. A Zebra machine at UNR generated transverse magnetic fields of 3 MG on the surface of the rod load and longitudinal fields of 1.4 MG in the coil loads. The magnetic fields were characterized with two-color Faraday rotation diagnostics. The pulsed power machine provided almost static magnetic fields for LPI compared to the much faster laser driven magnetic fields. We found that eddy currents in the rising magnetic field generate plasma on the metal targets. Eddy currents did not impact Si and CH dielectric targets. A Leopard laser with intensity in the focus up to 10 19 W/cm 2 produced plasma in the MG magnetic fields. The modified reflected Faraday diagnostics was used to study laser driven B-field at the MTW laser at Laboratory for Laser Energetics, UR. We demonstrated a slow dependence of the magnetic field in the coil on the applied laser intensity. The magnetic field increased by a factor of 2 if laser intensity increased by a factor of 30. This scaling is important for comparison of experiments at different laser facilities. Expansion of the plasma in the 2-3 MG external B-field was studied. Laser-produced plasma in the azimuthal magnetic field took the unique form of a thin disc expanding radially with a velocity of 250 km/s and confined in the vertical direction. A HYDRA MHD program at the University of Rochester was applied for simulations of LPI in the magnetic field B >3 MG. Simulations for the plasma disc parameters and the expansion dynamics were in a good agreement with experiments. Generation of narrow dense plasma jets in the longitudinal magnetic field of 0.6-0.8 MG was studied. Narrow plasma jets reached a length of 3-4 mm with the electron plasma density of (0.2-1.2)x10 20 cm -3 . A jet tip propagated with the velocity of 160-200 km/s. MHD simulations showed a good agreement of the dynamics of the formation of plasma jets with experiments. These jets are relevant to astrophysical jets. Simulations of K-shell spectra of Si plasma was performed for LPI in the B-field. The laser prepulse generated plasma near the laser target. A PrismSPECT model with a MeV electron beam produced by the laser was used. The spectral modelling showed the increased plasma density by a factor by 2-3 in the magnetic field. This was in agreement with the observed dynamics of the plasma plume confined by the axial magnetic field. The two-plasmon decay was studied in the 2.5-3 MG transversal magnetic fields. Strong 2-3.5 nm spectral widening and a 2-4 nm shifts of “red” and “blue” 3/2ω 0 spectral components were observed. The large shift and widening exceed the expected temperature and magnetic shift. PIC simulations are performing to clarify physics of this effect. The experimental research program for the grant is completed. New plasma effects in the MG fields were studied at the university-scale pulsed power generator. Two graduate and two undergraduate UNR and UR students carried experiments at the Zebra generator, supported and developed plasma diagnostics, provided data processing, and performed MHD simulations of LPI in the strong magnetic field. Research results are published in 9 referred papers and presented in 12 conferences. Program manager: Kramer U. Akli; Collaborators: R. C. Mancini and H. Sawada, University of Nevada, Reno (UNR); R. Betti and A. V. Maximov, University of Rochester (UR).

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2023

Relaxation dynamics of water in the vicinity of cellulose nanocrystals

Water molecules near cellulose nanocrystals (CNCs; produced via the sulfuric acid-catalyzed hydrolysis of wood pulp) are believed to relax slower than those in the bulk liquid, which may result in unique properties of CNC aqueous dispersions. Herein this study analyzed the polarization behavior of water molecules in CNC aqueous dispersions and other reference samples using a dielectric relaxation spectroscopy (DRS) technique in the microwave frequency range (0.2–20 GHz). As the CNC concentration increases, two slow relaxation components become prominent. The comparison with DRS data of aqueous dispersions of nanoporous silica, polyvinyl alcohol (PVA), and hairy CNC (HCNC) with amorphous chains protruding from both ends suggested that these slow relaxation modes of water near CNC surfaces cannot be attributed to direct hydrogen bonding interactions with the hydroxyl (OH) groups exposed and immobilized at the solid surface. Instead, they are similar to the water molecules interacting with OH groups attached to flexible polymer chains. Molecular dynamics (MD) simulations of the polarization behavior of water near the (110) facet of cellulose Iβ crystals confirmed that the interactions of water molecules with the cellulose crystal surface do not cause slower relaxations in the frequency range studied via the DRS. These results indicated that the CNC surface cannot be depicted with the crystallographic facets of cellulose Iβ; instead, it resembles a polymer-brush surface on which the short glucan residues or fragments of the strong acid-catalyzed hydrolysis process are swollen and extended into the aqueous phase.

59 BASIC BIOLOGICAL SCIENCES↗
DOE OSTI2023

High phase resolution: Probing interactions in complex interfaces with sum frequency generation

An often-quoted statement attributed to Wolfgang Pauli is that God made the bulk, but the surface was invented by the devil. Although humorous, the statement really reflects frustration in developing a detailed picture of a surface. In the last several decades, that frustration has begun to abate with numerous techniques providing clues to interactions and reactions at surfaces. Often these techniques require considerable prior knowledge. Complex mixtures on irregular or soft surfaces—complex interfaces—thus represent the last frontier. Two optical techniques: sum frequency generation (SFG) and second harmonic generation (SHG) are beginning to lift the veil on complex interfaces. Of these techniques, SFG with one excitation in the infrared has the potential to provide exquisite molecular- and moiety-specific vibrational data. This Perspective is intended both to aid newcomers in gaining traction in this field and to demonstrate the impact of high-phase resolution. It starts with a basic description of light-induced surface polarization that is at the heart of SFG. The sum frequency is generated when the input fields are sufficiently intense that the interaction is nonlinear. This nonlinearity represents a challenge for disentangling data to reveal the molecular-level picture. Three, high-phase-resolution methods that reveal interactions at the surface are described.

Biophysics↗