Substrate-controlled nucleation and growth kinetics in ultrathin Bi2Te3 films

Abstract Metal chalcogenides are promising layered topological materials, yet their electronic performance is often limited by parasitic bulk conduction arising from defects that introduce excess carriers and shift the Fermi level out of the topological regime. Controlling early-stage growth and defect formation is therefore essential for suppressing bulk transport and enhancing surface-state conduction. Here we investigate ultrathin Bi2Te3 films grown by pulsed laser deposition on substrates spanning van der Waals, lattice-matched, and amorphous regimes to determine how substrate-dependent nucleation pathways influence defect formation and electronic transport. Phase-pure, c-axis-oriented Bi 2 Te 3 forms on all substrates, but the growth morphology varies strongly. Layered growth with well-defined quintuple-layer terraces is associated with smoother substrate surfaces: atomically smooth mica and step-terraced SrTiO3 yield continuous terraces, whereas rougher BaF2 and amorphous Si3N4 produce island-structured films. Between the two smooth substrates, the higher surface energy of SrTiO 3 enhances adatom adsorption and nucleation density, promoting rapid vertical growth and early Te depletion. Transport measurements reveal n-type conduction with carrier densities of 10e19 -10e20 cm-3 . The highest carrier density occurs for films on SrTiO3 , consistent with defect formation during high-density nucleation, whereas mobility correlates with structural coherence and terrace formation. Weak anti-localization signatures confirm phase-coherent transport in films on mica and SrTiO3 . These results show that substrate roughness and nucleation density provide key levers for controlling defect formation and strengthening topological surface transport in Bi2Te3 thin films.