We perform an accuracy analysis of several possible reflectance–difference (RD) configurations that are compatible with standard molecular‐beam epitaxy (MBE) growth chambers, and describe in detail an optical‐bridge system that can determine relative changes in RD signals as small as 5×105 under standard growth conditions. Using this system, we determine the RD response of GaAs for changes in surface conditions at different wavelengths and correlate these to simultaneously measured reflection high‐energy electron diffraction (RHEED) intensities. Maximum anisotropies are found at 2.0–2.5 and 3.5 eV for Ga on GaAs and Al on AlAs, respectively, providing a way of spectrally distinguishing Ga–Ga and Al–Al dimers for surface‐chemical investigations, and suggesting that these photon energies are also optimal for modifying growth by light. At photon energies well removed from these anisotropy maxima, RD signals follow changes in surface structure, as RHEED. Our RD‐RHEED correlations provide insight concerning crystal growth by MBE and establish a common experimental link between MBE and non‐UHV methods of crystal growth where RHEED cannot be used. Finally, our results illustrate various possibilities of using reflectance difference spectroscopy to investigate surface structure, surface chemistry, and surface dynamics.

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