The nanoscale identification of molecules is a driving force for the

knowledge in nanoscience and a key parameter in the further devel-

opment of nanotechnology such as nanoelectronics, biotechnology,

or green technology. Vibration of atoms in molecules provides

valuable information on chemical species and is considered as a

molecular “finger-print.” For example, vibration-based microscopy

has recently shown the ability to track molecules in living tissues

without the need for fluorescent labels [1, 2]. Furthermore,

molecular vibrations or phonons in crystals are also sensitive to

intrinsic perturbations (defects, plasmon-phonon coupling, etc.)

and extrinsic perturbation (charge transfer, pressure, temperature,

optical processes, etc.). Vibrations can be probed by only a limited

number of techniques: infrared spectroscopy, inelastic neutron

scattering, Raman scattering, and, more recently, inelastic scanning

tunneling spectroscopy [3]. The last one “visualizes” the chemical

nature of atoms and molecules on a surface but requires ultra-

high vacuum (UHV) and very low temperature. The inelastic Raman

scattering provides very rich information and does not require

special sample preparation, but faces a low scattering cross section

(10−31-10−26 cm2/molecule [4, 5]), and Abbe’s diffraction limited spatial resolution.