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Development of cavity ring-down spectroscopy (CRDS) has enabled real-time monitoring of carbon stable isotope ratios of carbon dioxide and methane in air. Here we demonstrate that CRDS can be adapted to assess aquatic carbon cycling processes from microbial to ecosystem scales. We first measured in situ isotopologue concentrations of dissolved CO2 ((12)CO2 and (13)CO2) and CH4 ((12)CH4 and (13)CH4) with CRDS via a closed loop gas equilibration device during a survey along an estuary and during a 40 h time series in a mangrove creek (ecosystem scale). A similar system was also connected to an in situ benthic chamber in a seagrass bed (community scale). Finally, a pulse-chase isotope enrichment experiment was conducted by measuring real-time release of (13)CO2 after addition of (13)C enriched phytoplankton to exposed intertidal sediments (microbial scale). Miller-Tans plots revealed complex transformation pathways and distinct isotopic source values of CO2 and CH4. Calculations of δ(13)C-DIC based on CRDS measured δ(13)C-CO2 and published fractionation factors were in excellent agreement with measured δ(13)C-DIC using isotope ratio mass spectroscopy (IRMS). The portable CRDS instrumentation used here can obtain real-time, high precision, continuous greenhouse gas data in lakes, rivers, estuaries and marine waters with less effort than conventional laboratory-based techniques.

Estuarine sediments make an important contribution to the global carbon cycle, but we do not know how this will change under a future climate, which is expected to have lower pH oceans and frequent high‐temperature days. Six combinations of warming and partial pressures of CO2 (pCO2) were chosen to investigate the combined and individual effects of short‐term pressures on the diel metabolic response of shallow unvegetated sediments ex‐situ. Whereas warming significantly increased respiration, making sediments more heterotrophic, high‐pCO2 increased net primary productivity, resulting in less heterotrophic sediments. As a result, warming decreased the carbon burial potential of estuarine sediments and high‐pCO2 had the opposite effect. High‐pCO2 mitigates the negative effects of warming on benthic metabolism under the combined scenario, with carbon burial similar to that expected under high‐pCO2 conditions alone. Climate scenarios also changed the diurnal pCO2 variation, with ranges increasing by 33% with warming, and almost doubling under high‐pCO2 conditions. An additive response in pCO2 variability was observed under the combined scenario, increasing to 2.3× the current diel‐pCO2 range, highlighting the reduced buffering capacity of the water associated with a high CO2 climate. Future carbon burial and export under increased frequencies of unseasonably warm days projected for mid and end of century (30% and 50% of days‐per‐year, respectively) were estimated with and without ocean acidification. By 2100, warming alone could decrease annual estuarine sediment burial potential by 25%. However, ocean acidification could mitigate the negative effects of more frequent high‐temperature days and increase carbon burial potential over current conditions by ~18%. [ABSTRACT FROM AUTHOR]

Relative to their surface area, estuaries make a disproportionately large contribution of dissolved organic carbon (DOC) to the global carbon cycle, but it is unknown how this will change under a future climate. As such, the response of DOC fluxes from microbially dominated unvegetated sediments to individual and combined future climate stressors of temperature change (from Δ- 3 to Δ+ 5 ∘ C compared to ambient mean temperatures) and ocean acidification (OA, ∼ 2 × current CO 2 partial pressure, p CO 2) was investigated ex situ. Warming alone increased sediment heterotrophy, resulting in a proportional increase in sediment DOC uptake; sediments became net sinks of DOC (3.5 to 8.8 mmol C m -2 d -1) at warmer temperatures (Δ+ 3 and Δ+ 5 ∘ C, respectively). This temperature response changed under OA conditions, with sediments becoming more autotrophic and a greater sink of DOC (up to 4 × greater than under current p CO 2 conditions). This response was attributed to the stimulation of heterotrophic bacteria with the autochthonous production of labile organic matter by microphytobenthos. Extrapolating these results to the global area of unvegetated subtidal estuarine sediments, we find that the future climate of warming (Δ+ 3 ∘ C) and OA may decrease estuarine export of DOC by ∼ 80 % (∼ 150 Tg C yr -1) and have a disproportionately large impact on the global DOC budget. [ABSTRACT FROM AUTHOR]

Estuaries make a disproportionately large contribution of dissolved organic carbon (DOC) to the global carbon cycle, but it is unknown how this will change under a future climate. As such, the response of DOC fluxes from microbially dominated unvegetated sediments to individual and combined future climate stressors of warming (from Δ-3 °C to Δ+5 °C on ambient mean temperatures) and ocean acidification (OA, ~2 times the current partial pressure of CO2, pCO2) was investigated ex situ. Warming alone increased sediment heterotrophy, resulting in a proportional increase in sediment DOC uptake, with sediments becoming net sinks of DOC (3.5 to 8.8 mmol-C m-2 d-1) at warmer temperatures (Δ+3 °C and Δ+5 °C, respectively). This temperature response changed under OA conditions, with sediments becoming more autotrophic and a greater sink of DOC (1 to 4 times greater than under current-pCO2). This response was attributed to the stimulation of heterotrophic bacteria with the autochthonous production of labile organic matter by microphytobenthos. Extrapolating these results to the global area of unvegetated subtidal estuarine sediments, the future climate of warming (Δ+3 °C) and OA may decrease the estuarine export of DOC by ~80 % (~150 Tg-C yr-1) and have a disproportionately large impact on the global DOC budget. [ABSTRACT FROM AUTHOR]

Microphytobenthos (MPB) in photic sediments are highly productive but the fate of this production remains uncertain. Over 33 d, tracing of 13C from added bicarbonate in subtropical shallow subtidal sand showed rapid transfer of MPB-derived carbon to deeper sediment; below 2 cm (31% within 60 h) and 5 cm (18%). Despite their high turnover (5.5 d) and only representing ~ 8% of sediment organic carbon, MPB represented up to 35% of the 13C retained in sediments, demonstrating substantial carbon recycling. Carbon was rapidly transferred to heterotrophs, but their contribution to sediment 13C was similar to their biomass contribution (< 0.1% to 3.8%), with the exception of the foraminifera Cellanthus craticulatus, which accounted for up to 33% of the 13C within sediment. There was little loss of MPB-derived carbon via dissolved organic carbon (DOC) effluxes (3%) or resuspension (minimal). Respiration was the major loss pathway (63%), reflecting the high microbial biomass typical of lower latitudes. Given that MPB take up dissolved inorganic carbon (DIC) from overlying water, and the carbon they fix is released as DIC, MPB in subtropical sands are unlikely to substantially alter the form of carbon transported offshore (i.e., there is no conversion to DOC), but processing within the sediment may alter its d13C value. Given that 31% of fixed carbon remained in sediments after 33 d, subtropical sands may act as a carbon sink, thereby affecting the quantity of carbon transported offshore. [ABSTRACT FROM AUTHOR]