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Funding Information: This work was supported by US DOE under contract nos. DE-FC02-04ER54698, DE-AC52-07NA27344, and DE-AC05-00OR22725. This work was supported by the Academy of Finland under grant no. 13330050. This report was prepared as an account of work sponsored by an agency of the United States Government. Neither the United States Government nor any agency thereof, nor any of their employees, makes any warranty, express or implied, or assumes any legal liability or responsibility for the accuracy, completeness, or usefulness of any information, apparatus, product, or process disclosed, or represents that its use would not infringe privately owned rights. Reference herein to any specific commercial product, process, or service by trade name, trademark, manufacturer, or otherwise, does not necessarily constitute or imply its endorsement, recommendation, or favoring by the United States Government or any agency thereof. The views and opinions of authors expressed herein do not necessarily state or reflect those of the United States Government or any agency thereof. Funding Information: This work was supported by US DOE under contract nos. DE-FC02-04ER54698 , DE-AC52-07NA27344 , and DE-AC05-00OR22725 . This work was supported by the Academy of Finland under grant no. 13330050 . Publisher Copyright: © 2023 The Authors UEDGE-CRUMPET simulations indicate the impact of the molecular hydrogenic isotopologue effect under high-recycling LFS divertor conditions in DIII-D to be negligible for electron density and temperature profiles at the LFS target plate. A 30% decrease in molecular content, accompanied by a 10% increase in atomic content, is predicted for deuterium compared to hydrogen. The predicted isotopologue effect on the radiative power balance, validated with calibrated spectroscopy, is found to be small despite a 20% increase in LFS divertor molecular band emission for deuterium compared to hydrogen. The predictions and measurements show a negligible contribution of molecularly-induced atomic and direct molecular emission to the total radiative power balance under high-recycling conditions, consistent with previous EDGE2D-EIRENE investigations. The UEDGE-CRUMPET simulations were performed using effective hydrogen and deuterium rates considering molecular breakup and excitation processes for H2 and D2, calculated by theCRUMPET collisional-radiative model.