Reporting period: 7-1-1997 to s-3f@ya$ n,a,.h ,~~~~~~~ doe yov This project was under the direction of Prof. Xiaoxing Xi since Septemter 1997 when the the former PI, Prof. Jeff Lannin passed away. The main focus of the research has been in the lattice dynamics of ferroelectric thin films. In this report, we summarize the results of this project during this period and the publications resulted from this work.
Central importance of the soft mode in ferroelectricsThe potential of using ferroelectrics in various device applications have initiated a broad interest in the fundamental properties of ferroelectric thin films. For example, the ferroelectric properties are explored for non-volatile ferroelectric random-access memories (FRAM) [ 1, 21, the high static dielectric constant for dynamic random-access memories (DRAM) [3, 41 and gate oxide in MOSFET [5, 61, and the dielectric nonlinearity for tunable microwave devices [7].Lattice dynamics is of central importance for ferroelectrics [8]. The hallmark of ferroelectricity, i. e. the spontaneous polarization, arises from a displacement of the center of positive charge with respect to the center of negative charge in the ferroelectric crystal. This displacement, such as that of the Ti ion with respect to the oxygen cage in the Ti06 octahedra in BaTiOs (BTO), involves the same ionic movement as the vibration of a zone-center transverse optical phonon mode, the %oft mode". The soft mode has a low frequency due to the interplay between the local restoring force and the long range dipole interaction, and it decreases a s the temperature is lowered. When the temperature approaches a Curie temperature T,, the soft-mode frequency tends to zero 19,10) and the soft mode is frozen in the crystal, which transforms t o a ferroelectric phase [ l l ] . The soft-mode theory, due to Cochran [ll] and Anderson [12], has been proven by many lattice dynamics studies.The soft-mode behavior can explain the high dielectric constant in the paraelectric phase of ferroelectrics. According to the Lyddane-Sachs-Teller (LST) relation, which connects the macroscopic dielectric constants to the microscopic parameter -optical phonon frequencies, for a crystal with N optical modes. Here ~ ( 0 ) and E ( W ) are the static and the high frequency dielectric constants, and W L O~ and W T O~ are the frequencies of the longitudinal and transverse optical phonon modes, respectively. It is generally found that the frequencies of the higher optical modes exhibit no sizeable variation with temperature. The decrease in the soft-mode frequency as the temperature approaches T, will thus cause a dramatic increase of ~( 0 ) .In bulk STO crystals