This content will become publicly available on March 1, 2027

Title: Van der Waals epitaxy of millimeter-domain Bi2Se3
The unique electronic structure of Bi2Se3 makes it appealing not only for studying fundamental topological physics but also for pursuing technological applications that include future electronics, spintronics, and quantum computing. This work uses a chemical vapor deposition approach to synthesize submillimeter domain continuous epitaxial thin films as well as continuous films with preferred orientation and domain sizes ranging up to a millimeter. Atomic force microscopy imaging reveals a terraced pyramid structure with step sizes down to one quintuple layer. We observe that large amounts of deposition on the tube walls from previous growths negatively affect the quality of epitaxy but positively affect grain size due to revaporization of previous growth. Transport measurements and Hikami–Larkin–Nagaoka fits of conductivity versus magnetic field indicate a bulk conducting nature to the film. This work pushes forward the domain size Bi2Se3 films by an order of magnitude, while maintaining the regularly reported doping problems of topological insulators.  more » « less
Award ID(s):
2328906 2312944
PAR ID:
10698654
Author(s) / Creator(s):
; ; ; ; ; ; ; ; ; ; ; ; ;
Publisher / Repository:
AVS
Date Published:
Journal Name:
Journal of Vacuum Science & Technology A
Volume:
44
Issue:
2
ISSN:
0734-2101
Format(s):
Medium: X
Sponsoring Org:
National Science Foundation
More Like this
  1. Bi2Se3 thin films have grown in popularity as three-dimensional topological insulators with a host of potential applications. While the films themselves have been widely researched, improvements derived from better substrate preparation have lagged. In this study, investigations into the preparation of c-plane sapphire (c-sapphire) substrates and the influence on film quality were done. Analysis on the effects of substrate pretreat by ultra-high vacuum annealing of the substrates, the use of Nano-strip® as an etchant, and high temperature in air anneal of c-sapphire to form a terraced morphology on Bi2Se3 thin film growth were done for this study. 
    more » « less
  2. Well-defined supported metal nanoparticle catalysts, with high uniformity in particle sizes of the dispersed metal, are crucial for studying their catalyzed reactions that exhibit structure sensitivity. For such catalysts, conventional methods of preparation may prove unsuitable in controlling the nanoparticle size and distribution. In this work, the systematic growth of supported Pd and Pt particles was achieved through the method of electroless deposition (ED), in which additional metal was deposited on preexisting particles of the same metal. The ED process was investigated by varying the pump time, pump speed, and molar ratios of the reagents during the continuous addition of the metal precursor, as well as the reducing agent and stabilizer, which were hydrazine and ethylenediamine, respectively. This allowed for the precise control of deposition rates, thus regulating the supported metal particle size, size distribution, and particle density. A slower deposition rate was achieved by increasing the amount of the ethylenediamine stabilizer and lowering the pumping speed. Slower rates of deposition resulted in smaller particle sizes and tighter size distributions compared to other preparations with the same metal weight loading, as characterized via X-ray diffraction (XRD), chemisorption, and scanning-transmission electron microscopy (STEM) methods. 
    more » « less
  3. Despite the unique advantages of the memristive switching devices based on two-dimensional (2D) transition metal dichalcogenides, scalable growth technologies of such 2D materials and wafer-level fabrication remain challenging. In this work, we present the gold-assisted large-area physical vapor deposition (PVD) growth of Bi2Se3 features for the scalable fabrication of 2D-material-based crossbar arrays of memristor devices. This work indicates that gold layers, prepatterned by photolithography processes, can catalyze PVD growth of few-layer Bi2Se3 with 100-folds larger crystal grain size in comparison with that grown on bare Si/SiO2 substrates. We also present a fluid-guided growth strategy to improve growth selectivity of Bi2Se3 on Au layers. Through the experimental and computational analyses, we identify two key processing parameters, i.e., the distance between Bi2Se3 powder and the target substrate and the distance between the leading edges of the substrate and the substrate holder with a hollow interior, which plays a critical role in realizing large-scale growth. By optimizing these growth parameters, we have successfully demonstrated cm-scale highly-selective Bi2Se3 growth on crossbar-arrayed structures with an in-lab yield of 86%. The whole process is etch- and plasma-free, substantially minimizing the damage to the crystal structure and also preventing the formation of rough 2D-material surfaces. Furthermore, we also preliminarily demonstrated memristive devices, which exhibit reproducible resistance switching characteristics (over 50 cycles) and a retention time of up to 106 s. This work provides a useful guideline for the scalable fabrication of vertically arranged crossbar arrays of 2D-material-based memristive devices, which is critical to the implementation of such devices for practical neuromorphic applications. 
    more » « less
  4. 2D-layered materials (e.g., graphene and transition metal dichalcogenides) have attracted huge attention due to their unique mechanical and electrical properties. Emerging research efforts, which seek to combine device characterization and high-resolution electron micrography analysis for 2D-layered device features, demand nano/microlithographic techniques capable of producing ordered 2D material patterns on ultrathin membranes with nanoscale thicknesses. However, such membranes are so fragile that most conventional lithographic techniques can be hardly performed on them to generate 2D material patterns. Our previous works have demonstrated that the rubbing-induced site-selective (RISS) deposition method can produce arbitrary 2D semiconductor (e.g., MoS2 and Bi2Se3) patterns on regular device substrates. This fabrication route prevents the vulnerable 2D-layered structures from the detrimental damage introduced by plasma etching and resist-based lithography processes. In this work, we explore the applicability of RISS for directly producing 2D material patterns on nanomembranes. Specifically, this work shows that a polymeric interfacing layer on the rubbing template features, which can effectively prevent stress concentration during the rubbing process, is crucial to successful implementation of RISS processes on nanomembranes. Furthermore, we carried out the mechanics simulation of the Von Mises stress and pressure distribution on the RISS-processed membrane to identify the optimal rubbing load, which can generate sufficient triboelectric charge for material deposition but no damage to the membrane. Using this approach, we have successfully demonstrated the deposition of Bi2Se3 patterns on 25 nm SiOx nanomembranes and high-resolution transmission electron micrography characterization of the crystallographic structures. 
    more » « less
  5. Breaking the time-reversal symmetry on the surface of a topological insulator can open a gap for the linear dispersion and make the Dirac fermions massive. This can be achieved by either doping a topological insulator with magnetic elements or proximity-coupling it to magnetic insulators. While the exchange gap can be directly imaged in the former case, measuring it at the buried magnetic insulator/topological insulator interface remains to be challenging. Here, we report the observation of a large nonlinear Hall effect in iron garnet/Bi2Se3 heterostructures. Besides illuminating its magnetic origin, we also show that this nonlinear Hall effect can be utilized to measure the size of the exchange gap and the magnetic-proximity onset temperature. Our results demonstrate the nonlinear Hall effect as a spectroscopic tool to probe the modified band structure at magnetic insulator/topological insulator interfaces. 
    more » « less