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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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