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At least 253 records · Page 14
All sourcesNASA NTRSDOE OSTI
NASA NTRS2018

Tandem LA-ICP-MS & LIBS; A New Micro-Analytical Technique for the Measurement of Every Element in the Periodic Table

Laser Ablation ICP-MS (LA-ICP-MS) has been widely accepted as a microanalytical technique for in-situ trace (ppb) elemental analysis on the micron scale in a variety of geologic materials. LA-ICP-MS (single or multi-collector) provides both elemental and isotopic measurements critical for a wide range of geological research by generating a fine grained aerosol (nm scale) during the laser ablation event and delivering that aerosol to the ICP ion source of the mass spectrometer via an inert carrier gas. LA-ICP-MS, however, suffers from limitations in analyzing high ionization potential elements as well as elements subject to atmospheric and argon based interferences. LA-ICP-MS also has limitations in analyzing major elements due to detector saturation. An alternative laser ablation technique, Laser Induced Breakdown Spectroscopy (LIBS), employs an optical spectrometer integrated into the laser ablation system that analyzes the laser induced plasma at the sample surface across the entire optical spectrum for emission lines of every element in the periodic table. Elements that are difficult or impossible to measure with LA-ICP-MS are now possible to analyze with LIBS down to low ppm levels with CCD and/or ICCD detection. We introduce a new laser based technique, “Tandem LA-LIBS”, that combines LA for ICP-MS and LIBS into one integrated laser ablation system. This system has the effect of expanding the elemental coverage and the dynamic range of the laser ablation experiment as measurements from ppb to % level matrix elements can now be analyzed in a single ablation experiment. We present both femtosecond and nanosecond Tandem LA-LIBS quantitative and qualitative data on wide range of geological materials for those elements that are difficult or impossible by traditional LA-ICP-MS techniques such as F, H, O, N, C, S, halogens, etc. We also demonstrate that the simultaneous measurement of trace, minor and major elements are now possible in a single laser ablation experiment with Tandem LA-LIBS technology.

LA-ICP-MS↗
NASA NTRS2018

The Gas Composition and Deep Cloud Structure of Jupiter's Great Red Spot

We have obtained high-resolution spectra of Jupiter's Great Red Spot (GRS) between 4.6-5.4 microns using telescopes on Mauna Kea to derive gas abundances and to constrain its cloud structure between 0.5-5 bars. We used line profiles of deuterated methane (CH3D) at 4.66 microns to infer the presence of an opaque cloud at 5 plus or minus 1 bars. From thermochemical models, this is almost certainly a water cloud. We also used the strength of Fraunhofer lines in the GRS to obtain the ratio of reflected sunlight to thermal emission. The level of the reflecting layer was constrained to be at 570 plus or minus 30 millibars based on fitting strong NH3 lines at 5.32 microns. We identify this layer as an ammonia cloud based on the temperature where gaseous NH3 condenses. We found evidence for a strongly absorbing but not totally opaque cloud layer at pressures deeper than 1.3 bars by combining Cassini/CIRS (Composite Infrared Spectrometer) spectra of the GRS at 7.18 microns with ground-based spectra at 5 microns. This is consistent with the predicted level of an NH4SH cloud. We also constrained the vertical profile of H2O and NH3. The GRS spectrum is matched by a saturated H2O profile above an opaque water cloud at 5 bars. The pressure of the water cloud constrains Jupiter's O/H ratio to be at least 1.1 times solar. The NH3 mole fraction is 200 plus or minus 50 ppm (parts per million) for pressures between 0.7-5 bars. Its abundance is 40 ppm at the estimated pressure of the reflecting layer. We obtained 0.8 plus or minus 0.2 ppm for PH3, which is a factor of 2 higher than in the warm collar surrounding the GRS. We detected all five naturally occurring isotopes ofgermanium in GeH4 in the GRS. We obtained an average value of 0.35 plus or minus 0.05 ppb (parts per billion) for GeH4. Finally, we measured 0.8 plus or minus 0.2 ppb for CO in the deep atmosphere.

Bjoraker, G. L.↗
NASA NTRS2019

Titan's Ionospheric Chemistry, Fullerenes, Oxygen, Galactic Cosmic Rays and the Formation of Exobiological Molecules on and within its Surfaces and Lakes

We discuss the formation of aerosols within Titan's thermosphere-ionosphere and the different chemical pathways. Negative ion measurements by the Cassini Plasma Spectrometer (CAPS) Electron Spectrometer (ELS) give evidence for formation of unsaturated anion carbon chains, while positive ion measurements of the Cassini Ion Neutral Mass Spectrometer (INMS) indicate formation of more aromatic cation hydrocarbons. There is presently no direct observational evidence for large neutral molecule growth in Titan's thermosphere-ionosphere. The hydrocarbon cations are expected to form Polycyclic Aromatic Hydrocarbons (PAH), those with the addition of nitrogen being called PAHNs. We theorize anion carbon chains can eventually become long enough to fold into fullerene C(60,70) carbon shells, of various charge states. Based on laboratory data the fullerenes can trap incoming O(sup +) magnetospheric ions that have relatively high energy collisions with the fullerenes and, once trapped, protect the oxygen atom from Titan's reducing thermosphere-ionosphere. The fullerenes can form into larger onion fullerenes and condense into larger embryo aerosols (i.e., m/q > 10,000 amu/q anions as observed by CAPS/ELS) eventually falling onto Titan's surface and precipitating to the bottom of its hydrocarbon lakes. Molecule production composed of H, C, N is known to occur in Titan's atmosphere with energy input from the magnetosphere, solar UV, and deeppenetrating irradiation from galactic cosmic rays (GCR). Space radiation effects by GCR irradiation of Titan's surface and lakes can lead to the manufacture of exobiological molecules with oxygen as the new ingredient. We have developed a model of galactic cosmic ray irradiation of Titan's atmosphere, surface, subsurface and bottoms of Titan lakes. GCR would provide further energy for processing of the aerosols into more complex organic forms such as tholins and precursor molecules for amino acids. A second process called hydrolysis then converts the precursor molecules into amino acids. Hydrolysis is provided via meteor impacts with size > 10 km and cryovolcanism both which can produce liquid water on Titan's surface for episodic periods > several 100 to 1000 years. Our model shows that GCR secondary particles can penetrate ~ 100 m below the ice surface (including the bottom of Titan's less dense hydrocarbon lakes ~ 150 m depths) and produce chemically significant dosages over very long timescales ~ 450 Myrs. The GCR model is combined with laboratory data from experiments in which dry methyl ices were irradiated to doses producing prebiotic amino acids such as glycine. The model calculations show glycine can form to ~ 2.5 ppb levels near the surface after ~450 Myrs of GCR proton irradiation and potentially to 5 ppb if heavy-ion GCRs up through Fe are included. If such molecules were detected, this would not only confirm this model but indicate that life forms different from ours may not be required.

Edward C. Sittler Jr↗
NASA NTRS2020

Influence of Dynamic Ozone Dry Deposition on Ozone Pollution

Identifying the contributions of chemistry and transport to observed ozone pollution using regional‐to‐global models relies on accurate representation of ozone dry deposition. We use a recently developed configuration of the NOAA GFDL chemistry‐climate model – in which the atmosphere and land are coupled through dry deposition—to investigate the influence of ozone dry deposition on ozone pollution over northern midlatitudes. In our model, deposition pathways are tied to dynamic terrestrial processes, such as photosynthesis and water cycling through the canopy and soil. Small increases in winter deposition due to more process‐based representation of snow and deposition to surfaces reduce hemispheric‐scale ozone throughout the lower troposphere by 5–12 ppb, improving agreement with observations relative to a simulation with the standard configuration for ozone dry deposition. Declining snow cover by the end of the 21st‐century tempers the previously identified influence of rising methane on winter ozone. Dynamic dry deposition changes summer surface ozone by −4 to +7 ppb. While previous studies emphasize the importance of uptake by plant stomata, new diagnostic tracking of depositional pathways reveals a widespread impact of nonstomatal deposition on ozone pollution. Daily variability in both stomatal and nonstomatal deposition contribute to daily variability in ozone pollution. Twenty‐first century changes in summer deposition result from a balance among changes in individual pathways, reflecting differing responses to both high carbon dioxide (through plant physiology versus biomass accumulation) and water availability. Our findings highlight a need for constraints on the processes driving ozone dry deposition to test representation in regional‐to‐global models.

dry deposition↗
NASA NTRSDate not supplied

Long-range Transport of Siberian Biomass Burning Emissions to North America During FIREX-AQ

Biomass burning from wildfires is a significant global source of aerosol and trace gases which impact air quality, tropospheric and stratospheric composition, and climate. During the summer of 2019, wildfire activity in central and eastern Siberia occurred during the Fire Influence on Regional to Global Environments and Air Quality (FIREX-AQ) campaign conducted between July 24 and September 6, 2019. Ground-based lidar observations from the Autonomous Mobile Ozone Lidar for Tropospheric Experiments (AMOLITE) system in Alberta, Canada retrieved frequent anomalous ozone (O3) and aerosol lamina in the troposphere and lower stratosphere during this campaign. Data from NASA’s GEOS Composition Forecast (GEOS-CF) coupled chemistry meteorology model, TROPOspheric Monitoring Instrument (TROPOMI), Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observation (CALIPSO), and ground-based insitu data were used to define the trans-Pacific and trans-Arctic transport pathway of Siberian biomass burning emissions resulting in the enhanced O3 and aerosol lamina observed by AMOLITE in western Canada. Siberian wildfires impacted North American air quality resulting in enhancements of hourly-averaged surface carbon monoxide (CO) (total CO >150 ppb) and fine particulate matter (PM2.5) (>20 μg m-3) in western Canada, however, minimal increases in surface-level O3 were measured as well as modeled by GEOS-CF. The impact in western Canada due to Siberian wildfires was much larger in the free troposphere, demonstrated by GEOS-CF and AMOLITE O3 lamina 30–40 ppb above background values and model-predicted PM2.5 lamina >30 μg m-3. In addition to tropospheric composition effects, the large wildfire activity in Siberia may have influenced the stratosphere as data from AMOLITE, CALIPSO, and GEOS-CF all suggested aerosol layers from the fires were located 13–18 km above ground level (agl). This study shows that the Siberian biomass burning emissions in the summer of 2019 impacted tropospheric/stratospheric composition in western Canada, and potentially could have influenced areas in the vicinity of FIREX-AQ airborne measurements, and future studies of FIREX-AQ chemical composition should consider how this long-range transport could have influenced the background trace gas and aerosol concentrations being investigated.

Biomass↗
NASA NTRS2021

Spectral attenuation coefficients from measurements of light transmission in bare ice on the Greenland Ice Sheet

Light transmission into bare glacial ice affects surface energy balance, biophotochemistry, and light detection and ranging (lidar) laser elevation measurements but has not previously been reported for the Greenland Ice Sheet. We present measurements of spectral transmittance at 350–900 nm in bare glacial ice collected at a field site in the western Greenland ablation zone (67.15∘ N, 50.02∘ W). Empirical irradiance attenuation coefficients at 350–750 nm are ∼ 0.9–8.0 m−1 for ice at 12–124 cm depth. The absorption minimum is at ∼ 390–397 nm, in agreement with snow transmission measurements in Antarctica and optical mapping of deep ice at the South Pole. From 350–530 nm, our empirical attenuation coefficients are nearly 1 order of magnitude larger than theoretical values for optically pure ice. The estimated absorption coefficient at 400 nm suggests the ice volume contained a light-absorbing particle concentration equivalent to ∼ 1–2 parts per billion (ppb) of black carbon, which is similar to pre-industrial values found in remote polar snow. The equivalent mineral dust concentration is ∼ 300–600 ppb, which is similar to values for Northern Hemisphere warm periods with low aeolian activity inferred from ice cores. For a layer of quasi-granular white ice (weathering crust) extending from the surface to ∼ 10 cm depth, attenuation coefficients are 1.5 to 4 times larger than for deeper bubbly ice. Owing to higher attenuation in this layer of near-surface granular ice, optical penetration depth at 532 nm is 14 cm (20 %) lower than asymptotic attenuation lengths for optically pure bubbly ice. In addition to the traditional concept of light scattering on air bubbles, our results imply that the granular near-surface ice microstructure of weathering crust is an important control on radiative transfer in bare ice on the Greenland Ice Sheet ablation zone, and we provide new values of flux attenuation, absorption, and scattering coefficients to support model development and validation.

IceSat-2↗
NASA NTRSDate not supplied

Double ChemFET for the In-Line Monitoring of Silver Dosing in Potable Water Systems

With NASA Advanced Exploration Systems (AES) Life Support Systems (LSS)baselining ionic silver (Ag+) as the biocide of choice, development in silver monitoring technologies becomes necessary to monitor and control Ag+ release. Ion-selective field effect transistors (ISFETs) and chemically-sensitive field effect transistors (ChemFETs) are capable of selective detection of Ag+ with reversible and low detection limit responses. However, one major hurdle to ChemFET technologies is the requirement of a reference electrode, which can leak its fill solution into the potable water system and is prone to drift requiring frequent calibration. To circumvent this issue, a double chemically-sensitive field effect transistor (dChemFET) is proposed. The dChemFET uses a second ChemFET to selectively monitor the counter ion and serves in place of the reference electrode. This work reports on the development of the dChemFET, starting with the development of the Ag+ andNO3- ion selective membranes (ISMs) to be used in the ChemFETs. The Ag+ ISM was tested in 50-105 ppb Ag+ and showed linear, sub-Nernstian response. The NO3- ISM was tested in50-500 ppb silver ion equivalents of nitrate ion (Ag+ equiv. of NO3-) and shows linear, sub-Nernstian response as well . However, the Ag+ and NO3- ISMs face significant challenges in terms of drift that obstruct its application for long-term monitoring, but it can serve as a starting point for demonstrating the dChemFET proof of concept.

John Abdou↗
NASA NTRSDate not supplied

GeoCarb L2 Validation- Albedo Error Propagation into XCO2 in the Near Infrared

GeoCarb validation activities Pre-launch validation •Thermovac: Nov-Jan, 2022/3: Edwards/Dryden will move to Palo Alto Nov-March 2022/3 •Day-in-the life simulation-2022 •Simulations near Dallas, TX •Validation of TROPOMI in GeoCarb domain-2022 2GeoCarb post-launch GeoCarb will have gas precision of: •0.3% (1.2 ppm) for XCO2 •0.6% (11 ppb) for XCH4 •10% or 12 ppb for XCO GeoCarb SIF with precision of better than 0.75 W/m2/um/sr GeoCarb will utilize TCCON, GML/DOE aircraft, AirCore, and any validation site with systematic errors better than GeoCarb’s

GeoCarb↗
NASA NTRS2022

The Ozone–Climate Penalty Over South America and Africa By 2100

Climate change has the potential to increase surface ozone (O3) concentrations, known as the “ozone–climate penalty”, through changes to atmospheric chemistry, transport and dry deposition. In the tropics, the response of surface O3 to changing climate is relatively understudied but has important consequences for air pollution and human and ecosystem health. In this study, we evaluate the change in surface O3 due to climate change over South America and Africa using three state-of-the-art Earth system models that follow the Shared Socioeconomic Pathway 3-7.0 emission scenario from CMIP6. In order to quantify changes due to climate change alone, we evaluate the difference between simulations including climate change and simulations with a fixed present-day climate. We find that by 2100, models predict an ozone–climate penalty in areas where O3 is already predicted to be high due to the impacts of precursor emissions, namely urban and biomass burning areas, although on average, models predict a decrease in surface O3 due to climate change. We identify a small but robust positive trend in annual mean surface O3 over polluted areas. Additionally, during biomass burning seasons, seasonal mean O3 concentrations increase by 15 ppb (model range 12 to 18 ppb) in areas with substantial biomass burning such as the arc of deforestation in the Amazon. The ozone–climate penalty in polluted areas is shown to be driven by an increased rate of O3 chemical production, which is strongly influenced by NOx concentrations and is therefore specific to the emission pathway chosen. Multiple linear regression finds the change in NOx concentration to be a strong predictor of the change in O3 production, whereas increased isoprene emission rate is positively correlated with increased O3 destruction, suggesting NOx-limited conditions over the majority of tropical Africa and South America. However, models disagree on the role of climate change in remote, low-NOx regions, partly because of significant differences in NOx concentrations produced by each model. We also find that the magnitude and location of the ozone–climate penalty in the Congo Basin has greater inter-model variation than that in the Amazon, so further model development and validation are needed to constrain the response in central Africa. We conclude that if the climate were to change according to the emission scenario used here, models predict that forested areas in biomass burning locations and urban populations will be at increasing risk of high O3 exposure, irrespective of any direct impacts on O3 via the prescribed emission scenario.

Surface ozone↗
NASA NTRSDate not supplied

P52D-1583 - Further Improvements to Constraints on Titan’s Atmospheric n-Butane, via Ground-Based Observations

We have acquired high spectral resolution ground-based observations of Titan in the mid-infrared from NASA Infrared Telescope Facility’s Texas Echelon Cross Echelle Spectrograph instrument , designed to constrain the abundances of new molecules within Titan’s atmosphere. The target molecule for this work, n-butane (n-C H ), though predicted by photochemical models of Titan’s atmosphere , has never been detected. Using the NEMESIS radiative transfer code , we retrieved a disk-averaged temperature profile for Titan by modeling CH emission in the 1248 cm region. Using this temperature profile, we then retrieved disk-averaged profiles of ethene (C H ), propane (C H ), and propene (C H ) in the 956 and 965 cm regions, which are also home to the strong and vibrational features of n-butane. We used an n-butane pseudoline list from JPL in order to systematically introduce a range of n-butane mixing ratios into the model, to constrain the molecule’s abundance based on the model’s changing fit to the data. We derive 3-confidence upper limits at an altitude of 150 km of 48 and 31 ppb for n-butane, via the and bands in the 956 and 965 cm regions, respectively. These are significantly tighter upper limits when compared to the ~300 ppb upper limit found in our recent work which used the same methodology but on much lower resolution limb data collected by the Cassini spacecraft. Upper limits on gas abundances are important for continued improvement of photochemical models of Titan’s atmosphere, which is understood to be an important analog for the prebiotic Earth atmosphere . They are also important for understanding the composition of Titan’s lakes and seas, which are likely to contain these larger hydrocarbons . Finally, as larger molecules like C ’s are thought to be able to serve as formation sites for building haze particles, constraining their abundances is important for understanding the process of haze formation at Titan and at Earth Ref: [1] J. H. Lacy, et al., PASP, 2002. [2] Y.L. Yung, et al., ApJS, 1984. [3] M. Dobrijevic, et al., Icarus, 2021. [4] P. G. J. Irwin et al., JQSRT, 2008. [5] K. Sung, et al., JQSRT, 2020. [6] B. L. Steffens, et al., PSJ, 2022. [7] Clarke & Ferris, Origins Life Evol. Biosphere, 1997. [8] D. Cordier, et al., ApJ, 2008. [9] D. B. Curtis, et al., JPCA, 2005.

Brendan Steffens↗
NASA NTRS2023

Using Regionalized Air Quality Model Performance and Bayesian Maximum Entropy Data Fusion to Map Global Surface Ozone Concentration and Associated Uncertainty

Estimates of ground-level ozone concentrations have been improved through data fusion of observations and atmospheric chemistry models. Our previous global ozone estimates for the Global Burden of Disease study corrected for bias uniformly across continents and then corrected near monitoring stations using the Bayesian Maximum Entropy (BME) framework for data fusion. Here, we use the Regionalized Air Quality Model Performance (RAMP) framework to correct model bias over a much larger spatial range than BME can, accounting for the spatial inhomogeneity of bias and nonlinearity as a function of modeled ozone. RAMP bias correction is applied to a composite of 9 global chemistry-climate models, based on the nearest set of monitors. These estimates are then fused with observations using BME, which matches observations at measurement stations, with the influence of observations declining with distance in space and time. We create global ozone maps for each year from 1990 to 2017 at fine spatial resolution. RAMP is shown to create unrealistic discontinuities due to the spatial clustering of ozone monitors, which we overcome by applying a weighting for RAMP based on the number of monitors nearby. Incorporating RAMP before BME has little effect on model performance near stations, but strongly increases R 2 by 0.15 at locations farther from stations, shown through a checkerboard cross-validation. Corrections to estimates differ based on location in space and time, confirming heterogeneity. We quantify the likelihood of exceeding selected ozone levels, finding that parts of the Middle East, India, and China are most likely to exceed 55 parts per billion (ppb) in 2017. About 96% of the global population was exposed to ozone levels above the World Health Organization guideline of 60 µg m −3 (30 ppb) in 2017. Our annual fine-resolution ozone estimates may be useful for several applications including epidemiology and assessments of impacts on health, agriculture, and ecosystems.

Ozone↗
DOE OSTI2020

Magnetic Field Determination for Run 1 of the Fermilab Muon $g-2$ Experiment

The muon $g-2$ experiment at Fermilab aims to measure the anomalous magnetic moment of the muon, $a_{\mu}$, to a precision of 140 parts per billion (ppb). The measurement will shed light on the current $>$3$\sigma$ deviation between Standard Model calculations and the previous measurement made at Brookhaven National Laboratory, either resolving the discrepancy or confirming it to $>$5$\sigma$. In the muon $g-2$ experiment, muons are stored in a magnetic storage ring and their decays are observed. In order to reach the precision goal, the magnetic field experienced by the muons must be known with an uncertainty of \SI{70}{ppb} or less. To this end, the magnetic field was shimmed to unprecedented homogeneity. Two measurement systems are used to track the evolution of the magnetic field. This dissertation describes the motivations for the $g-2$ experiment, gives a brief overview of the experimental principles, introduces the magnetic field measurement hardware, describes the magnetic field shimming process, and presents an analysis of the magnetic field tracking for data collected in spring 2018 during run 1 of the Fermilab muon $g-2$ experiment.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗
DOE OSTI2021

Reduction of the beam dynamics systematic uncertainties by the phase space matching with RF electric fields in Muon g –2 experiment at Fermilab

Muon g –2 experiment at Fermilab aims to measure the magnetic anomaly of the muon in a precision of 140 parts-per-billion (ppb). It is one of the most strongly motivated precision particle physics experiments to unveil the mystery of the long-standing 3σ-4σ tension between the previous measurement of the muon g –2 experiment at BNL and the Standard Model predictions. One of the main challenges of the experiment is to keep the total systematic uncertainty within 100 ppb budget. In this dissertation, a novel way of matching the phase space in the muon g –2 storage ring to reduce the beam dynamics systematic effects with RF electric fields is presented. Systematic simulation studies and hardware development of the RF matching system are covered, followed by the promising analysis results of the commissioning runs.

Kim, On↗
DOE OSTI2023

Neutron Skin Measurement of 208Pb and 48Ca Using Parity Violating Electron Scattering

Parity-violating electron scattering experiments (PVES) provides a clean probe of neutron densities that is model independent and free from strong interaction uncertainties in interpretation. The PREX-2 and CREX experiments were run in 2019 and 2020 at Jefferson laboratory measured the nucleon skin thickness, the difference between the r.m.s. neutron radius Rn and the r.m.s. proton radius Rp, of 208Pb and 48Ca via parity violating electroweak asymmetry in the elastic scattering of longitudinally polarized electrons. PREX-2 experiment was performed with 950 MeV electrons scattered at a 5¿ angle with Q2 = 0.00616 ± 0.00004 (GeV/c)2, while CREX used 2182 MeV electrons at the same angle with Q2 = 0.0297 ± 0.0002 (GeV/c)2. For PREX-2 the measured asymmetry was AP V = 550 ± 16 (stat.) ± (syst.) ppb, which corresponds to Rskin = 0.278 ± 0.078 (exp.) ± 0.012 (theo.) fm. The CREX asymmetry was AP V = 2668 ± 106 (stat.) ± 40 (syst.) ppb, which corresponds to Rskin = 0.121 ± 0.026 (exp.) ±0.024 (model) fm. One of the crucial systematic uncertainty that PREX-2 and CREX were sensitive to was the non-parity violating asymmetries that resulted from the helicity correlated false asymmetries in the polarized electron beam. There was a lot of work put towards understanding and suppressing the asymmetries arising from these effects. The parity violating asymmetry measurement required a very precise determination of the electron beam polarization. To accurately determine the beam polarization, a Compton polarimeter was used during both PREX-2 and CREX. A careful alignment of the laser to the Fabry-Perot cavity, data analysis and systematic control was employed to get a precise beam polarization result for the experiments. The PREX-2 measurement has broad implications for increasing our knowledge about neutron star structure and the equation of state of nuclear matter. The combined PREX and CREX results will have implications for future energy density functional calculations and the theory of nuclear structure.

Premathilake, Sachinthani↗
DOE OSTI2020

Printing 2D Conjugated Polymer Monolayers and Their Distinct Electronic Properties

Abstract Recently, 2D monolayer films of conjugated polymers have gained increasing attention owing to the preeminence of 2D inorganic films that exhibit unique optoelectronic and mechanical properties compared to their bulk analogs. Despite numerous efforts, crystallization of semiconducting polymers into highly ordered 2D monolayer films still remains challenging. Herein, a dynamic‐template‐assisted meniscus‐guided coating is utilized to fabricate continuous, highly ordered 2D monolayer films of conjugated polymers over a centimeter scale with enhanced backbone π–π stacking. In contrast, monolayer films printed on solid substrates confer upon the 1D fiber networks strong alkyl side‐chain stacking at the expense of backbone packing. From single‐layers to multilayers, the polymer π‐stacks change from edge‐on to bimodal orientation as the film thickness reaches ≈20 nm. Spectroscopic and cyclic voltammetry analysis reveals an abrupt increase in J‐aggregation and absorption coefficient and a decrease in bandgap and highest occupied molecular orbital level until critical thickness, possibly arising from the straightened polymer backbone. This is corroborated by an abrupt increase in hole mobility with film thickness, reaching a maximum of 0.7 cm 2 V −1 s −1 near the critical thickness. Finally, fabrication of chemical sensors incorporating polymer films of various thicknesses is demonstrated, and an ultrahigh sensitivity of the ≈7 nm thick ultrathin film (bilayers) to 1 ppb ammonia is shown.

Kafle, Prapti↗
DOE OSTI2020

Trace-Level, Multi-Gas Detection for Food Quality Assessment Based on Decorated Silicon Transistor Arrays

Multiplexed gas detection at room temperature is critical for practical applications, such as for tracking the complex chemical environments associated with food decomposition and spoilage. Here, an integrated array of multiple silicon-based, chemical-sensitive field effect transistors (CSFETs) is presented to realize selective, sensitive, and simultaneous measurement of gases typically associated with food spoilage. CSFETs decorated with sensing materials based on ruthenium, silver, and silicon oxide are used to obtain stable room-temperature responses to ammonia (NH 3 ), hydrogen sulfide (H 2 S), and humidity, respectively. For example, one multi-CSFET sensor signal changes from its baseline by 13.34 in response to 1 ppm of NH 3 , 724.45 under 1 ppm H 2 S, and 23.46 under 80% relative humidity, with sensitive detection down to 10 ppb of NH 3 and H 2 S. To demonstrate this sensor for practical applications, the CSFET sensor array is combined with a custom-printed circuit board into a compact, fully integrated, and portable system to conduct real-time monitoring of gases generated by decomposing food. By using existing silicon-based manufacturing methodologies, this room-temperature gas sensing array can be fabricated reproducibly and at low cost, making it an attractive platform for ambient gas measurement needed in food safety applications.

36 MATERIALS SCIENCE↗
DOE OSTI2023

Fully Inkjet‐Printed, 2D Materials‐Based Field‐Effect Transistor for Water Sensing

Abstract Despite significant progress in solution‐processing of 2D materials, it remains challenging to reliably print high‐performance semiconducting channels that can be efficiently modulated in a field‐effect transistor (FET). Herein, electrochemically exfoliated MoS 2 nanosheets are inkjet‐printed into ultrathin semiconducting channels, resulting in high on/off current ratios up to 10 3 . The reported printing strategy is reliable and general for thin film channel fabrication even in the presence of the ubiquitous coffee‐ring effect. Statistical modeling analysis on the printed pattern profiles suggests that a spaced parallel printing approach can overcome the coffee‐ring effect during inkjet printing, resulting in uniform 2D flake percolation networks. The uniformity of the printed features allows the MoS 2 channel to be hundreds of micrometers long, which easily accommodates the typical inkjet printing resolution of tens of micrometers, thereby enabling fully printed FETs. As a proof of concept, FET water sensors are demonstrated using printed MoS 2 as the FET channel, and printed graphene as the electrodes and the sensing area. After functionalization of the sensing area, the printed water sensor shows a selective response to Pb 2+ in water down to 2 ppb. This work paves the way for additive nanomanufacturing of FET‐based sensors and related devices using 2D nanomaterials.

36 MATERIALS SCIENCE↗