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Neal, S. N. ; Li, S. ; Birol, T. ; Musfeldt, J. L. ( , npj 2D Materials and Applications)null (Ed.)Abstract We combine infrared absorption and Raman scattering spectroscopies to explore the properties of the heavy transition metal dichalcogenide 1T-HfS 2 . We employ the LO–TO splitting of the E u vibrational mode along with a reevaluation of mode mass, unit cell volume, and dielectric constant to reveal the Born effective charge. We find $${Z}_{{\rm{B}}}^{* }$$ Z B * = 5.3 e , in excellent agreement with complementary first-principles calculations. In addition to resolving the controversy over the nature of chemical bonding in this system, we decompose Born charge into polarizability and local charge. We find α = 5.07 Å 3 and Z * = 5.2 e , respectively. Polar displacement-induced charge transfer from sulfur p to hafnium d is responsible for the enhanced Born charge compared to the nominal 4+ in hafnium. 1T-HfS 2 is thus an ionic crystal with strong and dynamic covalent effects. Taken together, our work places the vibrational properties of 1T-HfS 2 on a firm foundation and opens the door to understanding the properties of tubes and sheets.more » « less
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Hameed, S. ; Joe, J. ; Gautreau, D. M. ; Freeland, J. W. ; Birol, T. ; Greven, M. ( , Physical Review B)
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Kamba, S. ; Goian, V. ; Orlita, M. ; Nuzhnyy, D. ; Lee, J. H. ; Schlom, D. G. ; Rushchanskii, K. Z. ; Ležaić, M. ; Birol, T. ; Fennie, C. J. ; et al ( , Physical Review B)