Srivastava, P.K.Khandelwal, V.Reddy, I.R.Tarafder, K.Ghosh, S.2026-02-032025Journal of Physical Chemistry C, 2025, 129, 41, pp. 18530-1853619327447https://doi.org/10.1021/acs.jpcc.5c04013https://idr.nitk.ac.in/handle/123456789/20024Here, we report on controlling strain in graphene by trapping molecules at the graphene–substrate interface and leveraging molecular dipole moments. Spectroscopic and transport measurements reveal that strain correlates with the dipole moments of trapped molecules extending beyond their molecular sizes, where values ranging from 1.5 to 4.9D lead to a 50-fold increase in strain and a significant rise in residual carrier density. This has been possible by charge transfer between graphene and trapped molecules, altering the C?C bond length and causing biaxial strain. First-principles density functional theory calculations confirm a consistent dependence of the bending height on molecular dipole moments. © 2025 American Chemical SocietyBond lengthCharge transferDensity functional theoryDipole momentInterfaces (materials)MoleculesC-C bondsGraphene substratesGraphenesMolecular dipole momentMolecular sizeResidual carrier densitySpectroscopic measurementsSubstrate interfaceTransport measurementsTrapped moleculesGraphene