This is the 30th annual review of the application of atomic spectrometry to the chemical analysis of environmental samples. This Update refers to papers published approximately between August 2013 and July 2014 and continues the series of Atomic Spectrometry Updates (ASUs) in environmental analysis that should be read in conjunction with other related ASUs in the series, namely: clinical and biological materials, foods and beverages, advances in atomic spectrometry and related techniques, elemental speciation,X-ray fluorescence spectrometry, and the analysis of metals, chemicals and functional materials. In the field of air analysis, highlights within this review period included: the use of 3D printing technology for the rapid prototyping of new air sampler components; single particle ICP-MS studies; use of a new triple-quadrupole ICP-MS for the analysis of radioactive species and the use of FEG-SEM and IBA for the analysis of gun-shot residues. In the field of water analysis, methods continue to be developed: for the extraction and preconcentration of elements; speciation of As, Cr, Hg and Sb forms and determination of elemental constituents in colloidal and NP fractions. Instrumental developments reported include the use of MC-ICP-MS for isotopic tracer studies and a review of XRF techniques and associated preconcentration procedures for trace element analysis. Many articles featuring the analysis of plants and soils appeared but, as usual, most focused on environmental applications rather than the advancement of atomic spectrometry. There have, however, been interesting developments, such as the almost bewildering increase in types of micro-extraction for analyte preconcentration and the resurgence of CS-AAS. Clearly LIBS is maturing rapidly, with soil analysis becoming more routine in nature. Also notable was the way the accident at the Fukishima-Daiichi nuclear power plant triggered development of analytical methods for the assessment of contamination in the surrounding area. Recent research indicates that geological applications still drives many of the instrumental and methodological advances in LA-ICP-MS. Fundamental studies continue to shed light on the processes involved and hence ways of improving the analysis of laser-produced aerosols. The preparation of NP powders for the production of matrix-matched RMs for microanalytical techniques such as LA-ICP-MS and SIMS showed great promise for addressing one of the major issues when analysing geological materials by these techniques. Steady advances in MC-ICP-MS methodology is feeding through to applications in isotope geochemistry, while new SIMS instrumentation is being directed towards probing fine growth structures in biogenic carbonates and inferring past climate conditions from their geochemistry. Feedback on this review is most welcome and the review coordinator can be contacted using the email address provided.

/pdf/atomic-spectrometry-update-a-review-of-advances-in-2r8uzbiose.pdf

Atomic spectrometry update – a review of advances in environmental analysis

Laser-induced breakdown spectroscopy (LIBS) is a novel method of elemental analysis based on a laser-generated plasma. Pulses from a laser are focused on a sample to atomize a small amount of material resulting in the formation of a microplasma. Because of the high plasma temperature, the resulting atoms are electronically excited to emit light. The plasma light is spectrally resolved and detected to determine the elemental composition of the sample based on the unique emission spectrum of each element. Because of the simplicity of the method, it is suited for analyses that cannot be carried out using conventional methods of atomic emission spectroscopy (AES). This is particularly true for measurements that must be conducted outside of an analytical laboratory. A particular advantage of LIBS is the ability to analyze most types of samples without any preparation. This allows the interrogation of samples in situ, providing rapid measurement capability, permitting the method to be used in the analysis of gases, liquids, and solids in a variety of different sampling configurations. Although LIBS provides sensitive detection for many elements, it is not an ultrasensitive detection technique. In addition, under field conditions, the method typically does not provide the high accuracy and precision offered by laboratory-based methods of AES. Although basically an element detection method, chemometric methods of analysis are being developed to analyze the LIBS spectrum to provide identification of chemical substances (e.g. explosives, pathogens, and chemical agents).

Laser-induced Breakdown Spectroscopy

Abstract. Northern peatlands have been a large C sink during the Holocene,
but whether they will keep being a C sink under future climate change is
uncertain. This study simulates the responses of northern peatlands to
future climate until 2300 with a Peatland version Terrestrial Ecosystem
Model (PTEM). The simulations are driven with two sets of CMIP5 climate data
(IPSL-CM5A-LR and bcc-csm1-1) under three warming scenarios (RCPs 2.6, 4.5 and
8.5). Peatland area expansion, shrinkage, and C accumulation and
decomposition are modeled. In the 21st century, northern peatlands are
projected to be a C source of 1.2–13.3 Pg C under all climate scenarios
except for RCP 2.6 of bcc-csm1-1 (a sink of 0.8 Pg C). During 2100–2300,
northern peatlands under all scenarios are a C source under IPSL-CM5A-LR
scenarios, being larger sources than bcc-csm1-1 scenarios (5.9–118.3 vs.
0.7–87.6 Pg C). C sources are attributed to (1) the peatland water table depth
(WTD) becoming deeper and permafrost thaw increasing decomposition rate; (2) net primary production (NPP) not increasing much as climate warms because
peat drying suppresses net N mineralization; and (3) as WTD deepens,
peatlands switching from moss–herbaceous dominated to moss–woody dominated,
while woody plants require more N for productivity. Under IPSL-CM5A-LR
scenarios, northern peatlands remain as a C sink until the pan-Arctic annual
temperature reaches −2.6 to −2.89 ∘C, while this threshold is −2.09
to −2.35 ∘C under bcc-csm1-1 scenarios. This study predicts a
northern peatland sink-to-source shift in around 2050, earlier than previous
estimates of after 2100, and emphasizes the vulnerability of northern
peatlands to climate change.


/pdf/peatlands-and-their-carbon-dynamics-in-northern-high-lwwrbqap.pdf

Peatlands and their carbon dynamics in northern high latitudes from 1990 to 2300: a process-based biogeochemistry model analysis

Abstract Peatlands are an important carbon (C) reservoir storing one-third of global soil organic carbon (SOC), but little is known about the fate of these C stocks under climate change. Here, we examine the impact of warming and elevated atmospheric CO 2 concentration (eCO 2 ) on the molecular composition of SOC to infer SOC sources (microbe-, plant- and fire-derived) and stability in a boreal peatland. We show that while warming alone decreased plant- and microbe-derived SOC due to enhanced decomposition, warming combined with eCO 2 increased plant-derived SOC compounds. We further observed increasing root-derived inputs (suberin) and declining leaf/needle-derived inputs (cutin) into SOC under warming and eCO 2 . The decline in SOC compounds with warming and gains from new root-derived C under eCO 2 , suggest that warming and eCO 2 may shift peatland C budget towards pools with faster turnover. Together, our results indicate that climate change may increase inputs and enhance decomposition of SOC potentially destabilising C storage in peatlands. 

Climate warming and elevated CO2 alter peatland soil carbon sources and stability

The development of measurement methodologies to detect and monitor nuclear-relevant materials remains a consistent and significant interest across the nuclear energy, nonproliferation, safeguards, and forensics communities. Optical spectroscopy of laser-produced plasmas is becoming an increasingly popular diagnostic technique to measure radiological and nuclear materials in the field without sample preparation, where current capabilities encompass the standoff, isotopically resolved and phase-identifiable (e.g., UO and UO2) detection of elements across the periodic table. These methods rely on the process of laser ablation (LA), where a high-powered pulsed laser is used to excite a sample (solid, liquid, or gas) into a luminous microplasma that rapidly undergoes de-excitation through the emission of electromagnetic radiation, which serves as a spectroscopic fingerprint for that sample. This review focuses on LA plasmas and spectroscopy for nuclear applications, covering topics from the wide-area environmental sampling and atmospheric sensing of radionuclides to recent implementations of multivariate machine learning methods that work to enable the real-time analysis of spectrochemical measurements with an emphasis on fundamental research and development activities over the past two decades. Background on the physical breakdown mechanisms and interactions of matter with nanosecond and ultrafast laser pulses that lead to the generation of laser-produced microplasmas is provided, followed by a description of the transient spatiotemporal plasma conditions that control the behavior of spectroscopic signatures recorded by analytical methods in atomic and molecular spectroscopy. High-temperature chemical and thermodynamic processes governing reactive LA plasmas are also examined alongside investigations into the condensation pathways of the plasma, which are believed to serve as chemical surrogates for fallout particles formed in nuclear fireballs. Laser-supported absorption waves and laser-induced shockwaves that accompany LA plasmas are also discussed, which could provide insights into atmospheric ionization phenomena from strong shocks following nuclear detonations. Furthermore, the standoff detection of trace radioactive aerosols and fission gases is reviewed in the context of monitoring atmospheric radiation plumes and off-gas streams of molten salt reactors. Finally, concluding remarks will present future outlooks on the role of LA plasma spectroscopy in the nuclear community.

Laser Ablation Plasmas and Spectroscopy for Nuclear Applications.

This work extends a previous percentage level concentration study of the optical emission spectra for six rare earth elements, europium (Eu), gadolinium (Gd), lanthanum (La), praseodymium (Pr), neodymium (Nd), and samarium (Sm), along with the transition metal, yttrium (Y) using laser-induced breakdown spectroscopy (LIBS). The concentration of these six rare earth elements and yttrium has been attempted for the first time systematically down to parts per million (ppm) concentration levels ranging from 30 to 300 ppm. The authors have developed multivariate models for each element capable of predicting concentration with acceptable to excellent levels of accuracy. Additionally, partial least squares regression coefficients were used to identify key spectral features able to be used in this lower concentration regime. This study has demonstrated that it is conceivable to quantify the six rare earth elements along with yttrium at low concentrations in the parts per million levels.

Special Issue: Laser Induced Breakdown Spectroscopy

DOI:10.1017/RDC.2022.1 © Arizona Board of Regents on behalf of the University of Arizona 2022. This is a work of the U.S. Government and is not subject to copyright protection in the United States. Outside of the United States, this is an Open Access article, distributed under the terms of the Creative Commons Attribution-NonCommercial-NoDerivatives licence (http://creativecommons.org/licenses/by-nc-nd/4.0/), which permits non-commercial re-use, distribution, and reproduction in any medium, provided the original work is unaltered and is properly cited. The written permission of Cambridge University Press must be obtained for commercial re-use or in order to create a derivative work.

/pdf/local-spatial-heterogeneity-of-holocene-carbon-accumulation-3n1mhkcz.pdf

Local spatial heterogeneity of holocene carbon accumulation throughout the peat profile of an ombrotrophic northern minnesota bog – corrigendum

This work extends a previous percentage level concentration study of the optical emission spectra for six rare earth elements, europium (Eu), gadolinium (Gd), lanthanum (La), praseodymium (Pr), neodymium (Nd), and samarium (Sm), along with the transition metal, yttrium (Y) using laser-induced breakdown spectroscopy (LIBS). The concentration of these six rare earth elements and yttrium has been attempted for the first time systematically down to parts per million (ppm) concentration levels ranging from 30 to 300 ppm. The authors have developed multivariate models for each element capable of predicting concentration with acceptable to excellent levels of accuracy. Additionally, partial least squares regression coefficients were used to identify key spectral features able to be used in this lower concentration regime. This study has demonstrated that it is conceivable to quantify the six rare earth elements along with yttrium at low concentrations in the parts per million levels. Graphical Abstract

Quantification of Rare Earth Elements in the Parts Per Million Range: A Novel Approach in the Application of Laser-Induced Breakdown Spectroscopy

Warming is expected to increase the net release of carbon from peatland soils, contributing to future warming. This positive feedback may be moderated by the response of peatland vegetation to rising atmospheric [CO2] or to increased soil nutrient availability. We asked whether a gradient of whole-ecosystem warming (from + 0 °C to + 9 °C) would increase plant-available nitrogen and phosphorus in an ombrotrophic bog in northern Minnesota, USA, and whether elevated [CO2] would modify the nutrient response. We tracked changes in plant-available nutrients across space and through time and in comparison with other nutrient pools, and assessed whether nutrient warming responses were captured by a point version of the land-surface model, ELM-SPRUCE. We found that warming exponentially increased plant-available ammonium and phosphate, but that nutrient dynamics were unaffected by elevated [CO2]. The warming response increased by an order of magnitude between the first and fourth year of the experimental manipulation, perhaps because of dramatic mortality of Sphagnum mosses in the surface peat of the warmest treatments. However, neither the magnitude nor the temporal dynamics of the responses were captured by ELM-SPRUCE. Relative increases in plant-available ammonium and phosphate with warming were similar, but the response varied across raised hummocks and depressed hollows and with peat depth. Plant-available nutrient dynamics were only loosely correlated with inorganic and organic porewater nutrients, likely representing different processes. Future predictions of peatland nutrient availability under climate change scenarios must account for dynamic changes in nutrient acquisition by plants and microbes, as well as microtopography and peat depth. 

Whole-Ecosystem Warming Increases Plant-Available Nitrogen and Phosphorus in an Ombrotrophic Bog

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Special Issue: Laser Induced Breakdown Spectroscopy

Local spatial heterogeneity of holocene carbon accumulation throughout the peat profile of an ombrotrophic northern minnesota bog – corrigendum

Quantification of Rare Earth Elements in the Parts Per Million Range: A Novel Approach in the Application of Laser-Induced Breakdown Spectroscopy

Whole-Ecosystem Warming Increases Plant-Available Nitrogen and Phosphorus in an Ombrotrophic Bog