Electronic structures and photoemission spectroscopy

Abstract:

Patterning of high-quality two-dimensional chalcogenide crystals with unique planar structures and various fascinating electronic properties offers great potential for batch fabrication and integration of electronic and optoelectronic devices. However, it remains a challenge that requires accurate control of the crystallization, thickness, position, orientation and layout. Here we develop a method that combines microintaglio printing with van der Waals epitaxy to efficiently pattern various single-crystal two-dimensional chalcogenides onto transparent insulating mica substrates. Using this approach, we have patterned large-area arrays of two-dimensional single-crystal Bi2Se3 topological insulator with a record high Hall mobility of ∼1,750 cm(2) V(-1) s(-1) at room temperature. Furthermore, our patterned two-dimensional In2Se3 crystal arrays have been integrated and packaged to flexible photodetectors, yielding an ultrahigh external photoresponsivity of ∼1,650 A W(-1) at 633 nm. The facile patterning, integration and packaging of high-quality two-dimensional chalcogenide crystals hold promise for innovations of next-generation photodetector arrays, wearable electronics and integrated optoelectronic circuits.

Abstract:

Cd(3)As(2) is a candidate three-dimensional Dirac semimetal which has exceedingly high mobility and nonsaturating linear magnetoresistance that may be relevant for future practical applications. We report magnetotransport and tunnel diode oscillation measurements on Cd(3)As(2), in magnetic fields up to 65 T and temperatures between 1.5 and 300 K. We find that the nonsaturating linear magnetoresistance persists up to 65 T and it is likely caused by disorder effects, as it scales with the high mobility rather than directly linked to Fermi surface changes even when approaching the quantum limit. From the observed quantum oscillations, we determine the bulk three-dimensional Fermi surface having signatures of Dirac behavior with a nontrivial Berry phase shift, very light effective quasiparticle masses, and clear deviations from the band-structure predictions. In very high fields we also detect signatures of large Zeeman spin splitting (g∼16).

Abstract:

A novel topological insulator with orthorhombic crystal structure is demonstrated. It is characterized by quasi one-dimensional, conducting atomic chains instead of the layered, two-dimensional sheets known from the established Bi2(Se,Te)3 system. The Sb-doped Bi2Se3 nanowires are grown in a TiO2-catalyzed process by chemical vapor deposition. The binary Bi2Se3 is transformed from rhombohedral to orthorhombic by substituting Sb on ~38% of the Bi sites. Pure Sb2Se3 is a topologically trivial band insulator with an orthorhombic crystal structure at ambient conditions, and it is known to transform into a topological insulator at high pressure. Angle-resolved photoemission spectroscopy shows a topological surface state, while Sb doping also tunes the Fermi level to reside in the bandgap.

Abstract:

A novel topological insulator with orthorhombic crystal structure is demonstrated. It is characterized by quasi one-dimensional, conducting atomic chains instead of the layered, two-dimensional sheets known from the established Bi2(Se,Te)3 system. The Sb-doped Bi2Se3 nanowires are grown in a TiO2-catalyzed process by chemical vapor deposition. The binary Bi2Se3 is transformed from rhombohedral to orthorhombic by substituting Sb on ∼38% of the Bi sites. Pure Sb2Se3 is a topologically trivial band insulator with an orthorhombic crystal structure at ambient conditions, and it is known to transform into a topological insulator at high pressure. Angle-resolved photoemission spectroscopy shows a topological surface state, while Sb doping also tunes the Fermi level to reside in the bandgap.

Abstract:

To date, there have been a plethora of reports on different means to fabricate organic-inorganic metal halide perovskite thin films; however, the inorganic starting materials have been limited to halide-based anions. Here we study the role of the anions in the perovskite solution and their influence upon perovskite crystal growth, film formation and device performance. We find that by using a non-halide lead source (lead acetate) instead of lead chloride or iodide, the perovskite crystal growth is much faster, which allows us to obtain ultrasmooth and almost pinhole-free perovskite films by a simple one-step solution coating with only a few minutes annealing. This synthesis leads to improved device performance in planar heterojunction architectures and answers a critical question as to the role of the anion and excess organic component during crystallization. Our work paves the way to tune the crystal growth kinetics by simple chemistry.