One- and two-photon excited optical pH probing for cells using surface-enhanced Raman and hyper-Raman nanosensors

We demonstrate spatially resolved probing and imaging of pH in live cells by mobile and biocompatible nanosensors using surface-enhanced Raman scattering (SERS) of 4-mercaptobenzoic acid (pMBA) on gold nanoaggregates. Moreover, we also show that this concept of pH nanosensors can be extended to two-photon excitation by using surface-enhanced hyper-Raman scattering (SEHRS). In addition to the advantages of two-photon excitation, the SEHRS sensor enables measurements over a wide pH range without the use of multiple probes.