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A framework is proposed for infrared (IR) absorption microscopy in the far-field with a spatial resolution below the diffraction limit. The sub-diffraction resolution is achieved by pumping a transient contrast in the population of a selected vibrational mode with IR pulses that exhibit alternating central minima and maxima, and by probing the corresponding absorbance at the same wavelength with adequately delayed Gaussian pulses. Simulations have been carried out on the basis of empirical parameters emulating patterned thin films of octadecyltrichlorosilane and a resolution of 250 nm was found when probing the CH₂ stretches at 3.5 μm with pump energies less than ten times the vibrational saturation threshold.

A framework for far-field infrared absorption microscopy beyond the diffraction limit