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A transition metal diphosphide, WP 2 , is a candidate for type‐II Weyl semimetals (WSMs) in which spatial inversion symmetry is broken and Lorentz invariance is violated. As one of the prerequisites for the presence of the WSM state in WP 2 , spatial inversion symmetry breaking in this compound has rarely been investigated. Furthermore, the anisotropy of the WP 2  electrical properties and whether its electrical anisotropy can be tuned remain elusive. Angle‐resolved polarized Raman spectroscopy, electrical transport, optical spectroscopy, and first‐principle studies of WP 2  are reported. The energies of the observed Raman‐active phonons and the angle dependences of the detected phonon intensities are consistent with results obtained by first‐principle calculations and analysis of the proposed crystal symmetry without spatial inversion, showing that spatial inversion symmetry is broken in WP 2 . Moreover, the measured ratio ( R c  / R a  ) between the crystalline  c ‐axis and  a ‐axis electrical resistivities exhibits a weak dependence on temperature ( T ) in the temperature range from 100 to 250 K, but increases abruptly at  T  ≤ 100 K, and then reaches the value of ≈8.0 at  T  = 10 K, which is by far the strongest in‐plane electrical resistivity anisotropy among the reported type‐II WSM candidates with comparable carrier concentrations. Optical spectroscopy study, together with the first‐principle calculations on the electronic band structure, reveals that the abrupt enhancement of the electrical resistivity anisotropy at  T  ≤ 100 K mainly arises from a sharp increase in the scattering rate anisotropy at low temperatures. More interestingly, the  R c  / R a   of WP 2  at  T  = 10 K can be tuned from 8.0 to 10.6 as the magnetic field increases from 0 to 9 T. The so‐far‐strongest and magnetic‐field‐tunable electrical resistivity anisotropy found in WP 2  can serve as a degree of freedom for tuning the electrical properties of type‐II WSMs, which paves the way for the development of novel electronic applications based on type‐II WSMs.

Strong and Tunable Electrical Anisotropy in Type‐II Weyl Semimetal Candidate WP 2 with Broken Inversion Symmetry