Two-Photon-Excited Photoinduced Force Microscopy.

Tamura, Tetsu; Sagami, Norihide; Sasaki, Takeru; Yamamoto, Wataru; Oketani, Ryosuke; Hiramatsu, Kotaro · Nano Lett · 2026

basic_science · Level V

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Abstract

Sensing photoexcitation-induced forces via atomic force microscopy (AFM) has attracted much attention as a promising nanoscale molecular imaging modality. However, most such nanospectroscopies suffer from linear background and noise under single-photon excitation, including scattering into a quadrant detector or photothermal response from the cantilever or substrate. Here, we present two-photon-excited photoinduced force microscopy (TP-PiFM) to suppress these unwanted linear effects. A theoretical analysis shows that signal demodulation at ω<sub>tip</sub> ± 2ω<sub>opt</sub> can efficiently isolate the photothermal signal under intensity modulation on the pulse train at ω<sub>opt</sub> and tip driving at ω<sub>tip</sub>. As a proof-of-concept demonstration, we obtained TP-PiFM images of 40 nm gold nanoparticles with a higher resolution than that of AFM topography. Backgrounds in TP-PiFM images were suppressed through the demodulation technique as well as a fitting analysis to extract signals quadratically scaling on the illumination power. These results establish TP-PiFM as a robust, background-free nanoimaging method.