a A diagram of an isolated QW for investigating the generalized thermalization, which contains two parts: the discrete infinite lattice and spin (coin) subsystem , coupled by the spin–orbit interaction. b The experimental realization of QW involves the following four modules. (1) Pairs of photons are generated via the spontaneous parametric down-conversion (SPDC) in the BBO2 crystal, where a photon from each pair is directly detected by the APD1 as a trigger and the other signal one as the walker is sent to the subsequent module. (2) First, a localized state is initialized via a PBS-HWP-QWP setting. Second, the signal photons go through at most six steps of walk with each step involving two SU(2) coin tossings achieved by the combination QWP-HWP-QWP and two shift operators achieved by the calcite crystals. An arbitrary Gaussian wavepacket over the lattice space can be obtained after projecting the coin on an unbiased basis using an HWP and PBS. (3) After re-initialization of the coin state (here the time step is also re-initialized as t = 0) and sending the signal photons into a 10-step walk whose coin-tossing rotations along the y-axis and achieved by utilizing the HWP, the relaxation evolution of the coin state can be monitored through a coin analyzer. (4) The time-evolving probability distributions, i.e., the pulse train of signal photons with a time interval of approximately 5 ps, can be analyzed by utilizing the up-converted detector, which comprised a frequency upconversion in the BBO3 crystal, a 4-f system for filtering the spectrum, and a PMT detector. The 4-f system includes a prism for introducing dispersion, a knife-edge for blocking the noise photons whose wavelength is longer than 395 nm, and a mirror reflecting the up-converted signal photons to the PMT. List of the abbreviations: lens (L); β-BaB2O4 (BBO); avalanche photodiode detector (APD); dichroic mirror (DM); polarization-dependent beam splitter (PBS); half-wave plate (HWP); quarter-wave plate (QWP); photomultiplier tube (PMT). Detailed descriptions are provided in the Methods