Highly efficient stimulated Raman scattering at the air-heavy water interface

In this study, we conducted a detailed exploration of stimulated Raman scattering (SRS) in heavy water (D2O), focusing specifically on its behavior at the air-D2O interface. The analysis revealed discernible SRS characteristic peaks corresponding to different vibrational modes, showing a 3.31-fold reduction in the SRS threshold at the air-D2O interface. Notably, we achieved a remarkable 6.83% energy conversion efficiency, approximately 3.36 times higher than the 2.03% efficiency observed in bulk D2O. Through cascaded Raman scattering and Raman-enhanced four-wave mixing (FWM) processes, up to third-order Stokes and corresponding anti-Stokes SRS were obtained in an unprecedented manner at a low pump energy of 8.26 mJ. Additionally, distinctive conical spatial structures of Stokes and anti-Stokes generated at air-D2O interface were attributed to Raman-enhanced FWM processes. Our investigation into the temporal behavior of SRS pulses revealed a unique mechanism: the initial decline of pump pulse was due to SRS-induced pump energy loss and heat dissipation, while the behavior of latter half resulted from non-uniform refractive index, causing self-defocusing and inhibiting the sustained generation of SRS. Our study sheds light on the development of multi-wavelength and significant frequency shift Raman lasers, offering valuable perspectives for future research endeavors.