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For their runtime quality optimization, however, current approaches cannot tackle the variations of quality modeling and harvested energy simultaneously. Therefore, in this article, we are the first to propose a deep reinforcement learning (DRL)-based dynamic voltage frequency scaling (DVFS) method that optimizes the application execution quality of energy harvesting edge devices to mitigate the variations. First, we propose a baseline DRL formulation that novelly migrates the objective of quality maximization into a reward function and constructs a DRL quality agent. Second, we devise a long short-term memory (LSTM)-based selector that performs DRL quality agent selection based on the energy harvesting history. Third, we further propose two optimization methods to alleviate the nonnegligible overhead of DRL computations: 1) an improved thinking-while-moving concurrent DRL scheme to compromise the “state drifting” issue during the DRL decision process and 2) a variable interstate duration decision scheme that compromises the DVFS overhead incurred in each action taken. The experiments take an adaptive stereo matching application as a case study. 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