Assessing the recycling of chlorine and its long-lived ³⁶Cl isotope in terrestrial ecosystems through dynamic...

It is unclear to what extent chlorine (Cl) and its long-lived isotope ³⁶Cl are recycled in different terrestrial environments in response to time-variable inputs. A new version of a dynamic compartment model was developed to examine the transformation and transfer processes influencing the partitioning and persistence of both Cl and ³⁶Cl in forest ecosystems. The model's performance was evaluated by comparing simulations and field observations of scenarios of stable Cl atmospheric deposition and of global ³⁶Cl fallout. The model reproduced Cl storage in soil reasonably well, despite wide heterogeneity in environmental conditions and atmospheric deposits. Sensitivity analysis confirmed that the natural production of organochlorine in soil plays a major role in Cl build-up and affects long-term Cl dynamics. The timeframe required for the soil organochlorine pool to reach equilibrium in a steady-state system was several thousands of years. Interestingly, root uptake flux, a predominant pathway of the inorganic cycle, was found to affect both inorganic and organic pools in soil, highlighting the importance of plant-soil interactions in Cl dynamics. Model outputs agreed well with local ³⁶Cl measurements, and demonstrated that 90% of the ³⁶Cl found in soil may have come from bomb-test fallout. The pattern of estimated ³⁶Cl/Cl ratios showed that soil ³⁶Cl was not in equilibrium with ³⁶Cl levels in rain input in the post-bomb period. Complete recovery of a natural isotopic ratio in drainage water will need a time close to the residence time of organic ³⁶Cl in soil: i.e., 800 years. A simple dynamic model concept was found to be suitable to illustrate the plant-soil interactions combining both the inorganic and organic Cl cycles acting over different time scales.