Abstract

Dipole–dipole interactions provide a route to couple excitons across materials of different dimensionality. Here, we introduce hybrid films as a cross-dimensional excitonic platform and develop a theory of resonant Raman scattering in the presence of dipolar exciton coupling. Combining a coupled-oscillator model with perturbation theory, we show that coupling renormalizes the exciton–photon matrix elements and modifies nanotube Raman excitation profiles. We test this framework in vacuum-filtered films containing InP/ZnS quantum dots and mixed chirality metallic single-walled carbon nanotubes. The quantum-dot exciton remains near 1.83 eV, while chirality-dependent nanotube excitons span 1.7–1.93 eV, enabling systematic control of excitonic detuning. Relative to pristine nanotube films, the hybrids exhibit detuning-dependent redshifts and blueshifts, Raman-intensity enhancement, reduced effective linewidths, and near-resonant two-branch profiles. The model yields an effective splitting of approximately 110 meV. Resonant Raman scattering thus provides component-selective access to dipolar interactions that are only weakly apparent in ensemble absorption spectra.

Abstract

Dipole–dipole interactions provide a route to couple excitons across materials of different dimensionality. Here, we introduce hybrid films as a cross-dimensional excitonic platform and develop a theory of resonant Raman scattering in the presence of dipolar exciton coupling. Combining a coupled-oscillator model with perturbation theory, we show that coupling renormalizes the exciton–photon matrix elements and modifies nanotube Raman excitation profiles. We test this framework in vacuum-filtered films containing InP/ZnS quantum dots and mixed chirality metallic single-walled carbon nanotubes. The quantum-dot exciton remains near 1.83 eV, while chirality-dependent nanotube excitons span 1.7–1.93 eV, enabling systematic control of excitonic detuning. Relative to pristine nanotube films, the hybrids exhibit detuning-dependent redshifts and blueshifts, Raman-intensity enhancement, reduced effective linewidths, and near-resonant two-branch profiles. The model yields an effective splitting of approximately 110 meV. Resonant Raman scattering thus provides component-selective access to dipolar interactions that are only weakly apparent in ensemble absorption spectra.

Abstract

Dipole–dipole interactions provide a route to couple excitons across materials of different dimensionality. Here, we introduce hybrid films as a cross-dimensional excitonic platform and develop a theory of resonant Raman scattering in the presence of dipolar exciton coupling. Combining a coupled-oscillator model with perturbation theory, we show that coupling renormalizes the exciton–photon matrix elements and modifies nanotube Raman excitation profiles. We test this framework in vacuum-filtered films containing InP/ZnS quantum dots and mixed chirality metallic single-walled carbon nanotubes. The quantum-dot exciton remains near 1.83 eV, while chirality-dependent nanotube excitons span 1.7–1.93 eV, enabling systematic control of excitonic detuning. Relative to pristine nanotube films, the hybrids exhibit detuning-dependent redshifts and blueshifts, Raman-intensity enhancement, reduced effective linewidths, and near-resonant two-branch profiles. The model yields an effective splitting of approximately 110 meV. Resonant Raman scattering thus provides component-selective access to dipolar interactions that are only weakly apparent in ensemble absorption spectra.

Abstract

Dipole–dipole interactions provide a route to couple excitons across materials of different dimensionality. Here, we introduce hybrid films as a cross-dimensional excitonic platform and develop a theory of resonant Raman scattering in the presence of dipolar exciton coupling. Combining a coupled-oscillator model with perturbation theory, we show that coupling renormalizes the exciton–photon matrix elements and modifies nanotube Raman excitation profiles. We test this framework in vacuum-filtered films containing InP/ZnS quantum dots and mixed chirality metallic single-walled carbon nanotubes. The quantum-dot exciton remains near 1.83 eV, while chirality-dependent nanotube excitons span 1.7–1.93 eV, enabling systematic control of excitonic detuning. Relative to pristine nanotube films, the hybrids exhibit detuning-dependent redshifts and blueshifts, Raman-intensity enhancement, reduced effective linewidths, and near-resonant two-branch profiles. The model yields an effective splitting of approximately 110 meV. Resonant Raman scattering thus provides component-selective access to dipolar interactions that are only weakly apparent in ensemble absorption spectra.