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Compound specific hydrogen isotope ratios (delta D) of long chain sedimentary n-alkanes, which mostly originate from the leaf waxes of higher terrestrial plants, are increasingly employed as paleoclimate proxies. While soil water is the ultimate hydrogen source for these lipids and the isotopic fractionation during biosynthesis of lipids is thought to remain constant, environmental parameters and plant physiological processes can alter the apparent hydrogen isotopic fractionation between leaf-wax lipids and a plant's source water. However, the magnitude and timing of these effects and their influence on the isotopic composition of lipids from higher terrestrial plants are still not well understood. Therefore we investigated the seasonal variability of leaf-wax n-alkane delta D values for two different temperate deciduous forest ecosystems that are dominated by two different tree species, Beech (Fagus sylvatica) and Maple (Acer pseudoplatanus). We found significant seasonal variations for both tree species in n-alkane delta D values of up to 40%. on timescales as short as one week. Also, the isotopic difference between different n-alkanes from the same plant species did vary significantly and reached up to 50 parts per thousand at the same time when overall n-alkane concentrations were lowest. Since delta D values of soil water at 5 and 10 cm depth, which we assume represent the delta D value of the major water source for the investigated beech trees, were enriched in autumn compared to the spring by 30 parts per thousand, whereas n-alkane delta D values increased only by 10 parts per thousand, we observed variations in the apparent fractionation between beech leaf derived n-alkanes and soil water of up to 20 parts per thousand on a seasonal scale. This observed change in the apparent fractionation was likely caused by differences in leaf water isotopic enrichment. Based on mechanistic leaf water models we conclude that changes in the isotopic difference between water vapor and soil water were the most likely reason for the observed changes in the apparent fractionation between n- alkanes and soil water. The large variability of n-alkane concentrations and delta D values over time implies a continuous de nova synthesis of these compounds over the growing season with turnover times possibly as short as weeks. The signal to reach the soil therefore represents an integrated record of the last weeks before leaf senescence. This holds true also for the sedimentary record of small catchment lakes in humid, temperate climates, where wind transport of leaf-wax lipids is negligible compared to transfer through soil and the massive input of leaves directly into the lake in autumn.
Atmospheric transport is an understudied mechanism for leaf wax hydrogen isotope applications that contributes to mobilizing and depositing these compounds on the surface of the Earth. While previous efforts have identified the importance of atmospheric leaf wax deposition in remote marine locations, the processes are not well constrained on land in temperate latitudes where lakes are common and sedimentary leaf wax hydrogen isotope values are an attractive tool for understanding past precipitation changes. This work presents results from a field study that was conducted in 2010 and 2011 at Hainich National Park, Germany in order to evaluate the quantity and sources of leaf waxes in the atmosphere. Aerosols were sampled at approximately weekly intervals inside the forest canopy, and n-alkane distributions and hydrogen isotope values were compared with those from major tree species surrounding the sampling site. Despite sampling in what was expected to be a major production center, the distribution and hydrogen isotope values of atmospheric n-alkanes bore little resemblance to those of the local vegetation. Comparison with local meteorological data and to 10-day and 36-h back air mass trajectories indicated shifting effects of winds and temperature, and that mesoscale transport processes were more important than longrange mechanisms. Back trajectories also highlighted source effects, with easterly winds coinciding with relatively lower leaf wax hydrogen isotope values from more continental regions. These results suggest that leaf wax aerosols average over spatial scales that exceed typical surface catchment areas for small lake systems, even in forested areas, yet that the area over which these compounds are derived is still relatively regional. Depositional fluxes were also estimated in order to assess the potential importance of atmospheric transport to sedimentary archives. Although difficult to constrain, these estimates suggest that atmospheric deposition may be non-negligible for lake systems in cases where inputs from rivers or surface runoff are limited. Together, these observations provide new insights on how leaf waxes from different sources are integrated during aeolian transport and the spatial scales over which these processes occur.
We assessed tropical montane cloud forest (TMCF) sensitivity to natural disturbance by drought, fire, and dieback with a 7300-year-long paleorecord. We analyzed pollen assemblages, charcoal accumulation rates, and higher plant biomarker compounds (average chain length [ACL] of n-alkanes) in sediments from Wai 'anapanapa, a small lake near the upper forest limit and the mean trade wind inversion ('IWI) in Hawai`i. The paleorecord of ACL suggests increased drought frequency and a lower awl elevation from 2555-1323 cal yr B.P. and 606-334 cal yr B.P. Charcoal began to accumulate and a novel fire regime was initiated ca. 880 cal yr B.P., followed by a decreased fire return interval at ca. 550 cal yr B.P. Diebacks occurred at 2931, 2161, 1162, and 306 cal yr B.P., and two of these were independent of drought or fire. Pollen assemblages indicate that on average species composition changed only 2.8% per decade. These dynamics, though slight, were significantly associated with disturbance. The direction of species composition change varied with disturbance type. Drought was associated with significantly more vines and lianas; fire was associated with an increase in the tree fern Sadleria and indicators of open, disturbed landscapes at the expense of epiphytic ferns; whereas stand-scale dieback was associated with an increase in the tree fern Cibotium. Though this cloud forest was dynamic in response to past disturbance, it has recovered, suggesting a resilient TMCF with no evidence of state change in vegetation type (e.g., grassland or shrubland).