Yat Hang Jeffrey Chan

© The Author 2016.Charge density wave formation, a key physics issue for materials, arises from interactions among electrons and phonons that can also lead to superconductivity and other competing or entangled phases. The prototypical system TiSe 2, with a particularly simple transition and no Kohn anomalies caused by electron-phonon coupling, is a fascinating but unsolved case after decades of research. Our angle-resolved photoemission measurements of the band structure as a function of temperature, aided by first-principles calculations, reveal a hitherto undetected but crucial feature: a electronic order in each layer sets in at ∼232 K before the widely recognized three-dimensional structural order at ∼205 K. The dimensional crossover, likely a generic feature of such layered materials, involves renormalization of different band gaps in two stages.

© 2016 American Chemical Society.Charge density wave formation in solids is a critical phenomenon involving the collective reorganization of the electrons and atoms in the system into a wave structure, and it is expected to be sensitive to the geometric constraint of the system at the nanoscale. Here, we study the CDW transition in TiSe2, a quasi-two-dimensional layered material, to determine the effects of quantum confinement and changing dimensions in films ranging from a single layer to multilayers. Of key interest is the characteristic length scale for the transformation from a two-dimensional case to the three-dimensional limit. Angle-resolved photoemission spectroscopy measurements of films with thicknesses up to six layers reveal substantial variations in the energy structure of discrete quantum well states; however, the temperature-dependent band gap renormalization converges at just three layers. The results indicate a layer-dependent mixture of two transition temperatures and a very-short-range CDW interaction within a three-dimensional framework.

© 2015 Macmillan Publishers Limited. All rights reserved.A single molecular layer of titanium diselenide is a promising material for advanced electronics beyond graphene - a strong focus of current research. Such molecular layers are at the quantum limit of device miniaturization and can show enhanced electronic effects not realizable in thick films. We show that single-layer TiSe2 exhibits a charge density wave transition at critical temperature TC =232±5 K, which is higher than the bulk TC =200±5 K. Angle-resolved photoemission spectroscopy measurements reveal a small absolute bandgap at room temperature, which grows wider with decreasing temperature T below TC in conjunction with the emergence of ordering. The results are rationalized in terms of first-principles calculations, symmetry breaking and phonon entropy effects. The observed Bardeen-Cooper-Schrieffer behaviour of the gap implies a mean-field CDW order in the single layer and an anisotropic CDW order in the bulk.