Ultimate resolution limits in coherent anti-Stokes Raman scattering imaging

Coherent anti-Stokes Raman scattering is a widely used imaging technique that provides chemical contrast without the need for labels, making it an extremely valuable tool in physics, chemistry, and biology. In this work, we explore its fundamental precision limits by applying tools from quantum information theory. We identify optimal measurement strategies and show that spatial mode demultiplexing–a technique already accessible in current experimental setups–can achieve these quantum limits and, in many situations, improve the sensitivity of conventional intensity measurements. Building on this, we introduce an advanced imaging scheme based on vortex beams, which we predict to enhance the image information in the final quantum state of light and thereby lead to even higher resolution and sensitivity. These findings establish a clear path for enhancing nonlinear imaging techniques using concepts from quantum science, bridging the gap between established microscopy methods and the emerging capabilities of quantum technologies.