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The charge-density-wave transition in TiSe (2), which results in a commensurate (2x2x2) superlattice at temperatures below approximately 200 K, presumably involves softening of a zone-boundary phonon mode. For the first time, this phonon-softening behavior has been examined over a wide temperature range by synchrotron x-ray thermal diffuse scattering.

We have studied the nanoscale structural evolution of Pb films grown at 110 K on a Si(111) substrate as they are annealed to increasingly higher temperatures. Surface x-ray diffraction from a synchrotron source is used to observe the morphology evolve from an initial smooth film through various metastable states before reaching a state of local equilibrium, at which point the coverage of different height Pb structures is analyzed and related to the thickness-dependent surface energy. Rich patterns are seen in the resulting energy landscape similar to the beating patterns heard from the interference of two musical notes of similar pitch. The explanation is, however, very simple, as demonstrated by a model calculation based on the confinement of free electrons to a quantum well.

The A(n+1)B(n)O(3n+1) Ruddlesden-Popper homologous series offers a wide variety of functionalities including dielectric, ferroelectric, magnetic and catalytic properties. Unfortunately, the synthesis of such layered oxides has been a major challenge owing to the occurrence of growth defects that result in poor materials behaviour in the higher-order members. To understand the fundamental physics of layered oxide growth, we have developed an oxide molecular beam epitaxy system with in situ synchrotron X-ray scattering capability. We present results demonstrating that layered oxide films can dynamically rearrange during growth, leading to structures that are highly unexpected on the basis of the intended layer sequencing. Theoretical calculations indicate that rearrangement can occur in many layered oxide systems and suggest a general approach that may be essential for the construction of metastable Ruddlesden-Popper phases. We demonstrate the utility of the new-found growth strategy by performing the first atomically controlled synthesis of single-crystalline La3Ni2O7.

Lattice distortion due to oxygen octahedral rotations have a significant role in mediating the magnetism in oxides, and recently attracts a lot of interests in the study of complex oxides interface. However, the direct experimental evidence for the interrelation between octahedral rotation and magnetism at interface is scarce. Here we demonstrate that interfacial octahedral rotation are closely linked to the strongly modified ferromagnetism in (LaMnO 3 þ d ) N / (SrTiO 3 ) N superlattices. The maximized ferromagnetic moment in the N ¼ 6 superlattice is accompanied by a metastable structure (space group Imcm) featuring minimal octahedral rotations (a À a À c À , aB4.2°, gB0.5°). Quenched ferromagnetism for No4 superlattices is correlated to a substantially enhanced c axis octahedral rotation (a À a À c À , aB3.8°, gB8°f or N ¼ 2). Monte-Carlo simulation based on double-exchange model qualitatively reproduces the experimental observation, confirming the correlation between octahedral rotation and magnetism. Our study demonstrates that engineering superlattices with controllable interfacial structures can be a feasible new route in realizing functional magnetic materials.

Understanding the underlying physical principles that determine the internal structure of objects at the atomic scale is critical for the advancement of nanoscale science. We have performed synchrotron x-ray diffraction studies to determine the structural properties of smooth Pb films with varying thicknesses of 6 to 18 monolayers deposited on a Si(111) substrate at 110 K. We observe quasibilayer variations in the atomic interlayer spacings of the films consistent with charge density oscillations due to quantum confinement of conduction electrons and surface-interface interference effects. Quantum oscillations in atomic step height are also deduced.