Materials with large optical anisotropy are sought after for polarization control, nonlinear phase matching, the realization of unconventional surface waves, among other applications in classical and quantum optics. Here, we demonstrate a bulk uniaxial crystal with atomic-scale structural modulations, Sr9/8TiS3, has a record birefringence Δn = 2.1 across a broad transparent window in the mid- to far-infrared. The excess Sr atoms, compared to stoichiometric SrTiS3, introduce additional electrons into TiS6 octahedral blocks to form highly polarizable clouds, which selectively boost the extraordinary refractive index. Structural modulation is a new tool for the engineering of refractive-index and anisotropy of quantum materials.
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