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In our former work (Sci. Rep. 4: 6039, 2014), we theoretically and numerically demonstrated that chaotic oscillation can be induced in a nanoscale system consisting of quantum dots between which energy transfer occurs via optical near-field interactions. Furthermore, in addition to the nanoscale implementation of oscillators, it is intriguing that the chaotic behavior is associated with probability derived via a density matrix formalism. Indeed, in our previous work (Sci. Rep. 6: 38634, 2016) we examined such oscillating probabilities via diffusivity analysis by constructing random walkers driven by chaotically driven bias. In this study, we experimentally implemented the concept of probability chaos using a single-photon source that was chaotically modulated by an external electro-optical modulator that directly yielded random walkers via single-photon observations after a polarization beam splitter. An evident signature was observed in the resulting ensemble average of the time-averaged mean square displacement. Although the experiment involved a scaled-up, proof-of-concept model of a genuine nanoscale oscillator, the experimental observations clearly validate the concept of oscillating probability, paving the way toward future ideal nanoscale systems.