skip to main content
US FlagAn official website of the United States government
dot gov icon
Official websites use .gov
A .gov website belongs to an official government organization in the United States.
https lock icon
Secure .gov websites use HTTPS
A lock ( lock ) or https:// means you've safely connected to the .gov website. Share sensitive information only on official, secure websites.

Explore Research Products in the PAR
It may take a few hours for recently added research products to appear in PAR search results.


  • NSF Public Access
  • Search Results
  • Solid State Reaction Epitaxy, A New Approach for Synthesizing Van der Waals heterolayers: The Case of Mn and Cr on Bi 2 Se 3
Title: Solid State Reaction Epitaxy, A New Approach for Synthesizing Van der Waals heterolayers: The Case of Mn and Cr on Bi 2 Se 3
Abstract Van der Waals (vdW) heterostructures that pair materials with diverse properties enable various quantum phenomena. However, the direct growth of vdW heterostructures is challenging. Modification of the surface layer of quantum materials to introduce new properties is an alternative process akin to solid state reaction. Here, vapor deposited transition metals (TMs), Cr and Mn, are reacted with Bi2Se3with the goal to transform the surface layer to XBi2Se4(X = Cr, Mn). Experiments and ab initio MD simulations demonstrate that the TMs have a high selenium affinity driving Se diffusion toward the TM. For monolayer Cr, the surface Bi2Se3is reduced to Bi2‐layer and a stable (pseudo) 2D Cr1+δSe2layer is formed. In contrast, monolayer Mn can transform upon mild annealing into MnBi2Se4. This phase only forms for a precise amount of initial Mn deposition. Sub‐monolayer amounts dissolve into the bulk, and multilayers form stable MnSe adlayers. This study highlights the delicate energy balance between adlayers and desired surface modified layers that governs the interface reactions and that the formation of stable adlayers can prevent the reaction with the substrate. The success of obtaining MnBi2Se4points toward an approach for the engineering of other multicomponent vdW materials by surface reactions.  more » « less
Award ID(s):
2118414
PAR ID:
10641248
Author(s) / Creator(s):
 ;  ;  ;  ;  ;  ;  ;  
Publisher / Repository:
Wiley Blackwell (John Wiley & Sons)
Date Published:
Journal Name:
Advanced Functional Materials
Volume:
34
Issue:
28
ISSN:
1616-301X
Format(s):
Medium: X
Sponsoring Org:
National Science Foundation
More Like this
  1. ; ; ; ; ; ; ; ; ; ; et al (, 2D Materials)
    Abstract MnBi 2 Te 4 /(Bi 2 Te 3 ) n materials system has recently generated strong interest as a natural platform for the realization of the quantum anomalous Hall (QAH) state. The system is magnetically much better ordered than substitutionally doped materials, however, the detrimental effects of certain disorders are becoming increasingly acknowledged. Here, from compiling structural, compositional, and magnetic metrics of disorder in ferromagnetic (FM) MnBi 2 Te 4 /(Bi 2 Te 3 ) n it is found that migration of Mn between MnBi 2 Te 4 septuple layers (SLs) and otherwise non-magnetic Bi 2 Te 3 quintuple layers (QLs) has systemic consequences—it induces FM coupling of Mn-depleted SLs with Mn-doped QLs, seen in ferromagnetic resonance as an acoustic and optical resonance mode of the two coupled spin subsystems. Even for a large SL separation ( n ≳ 4 QLs) the structure cannot be considered as a stack of uncoupled two-dimensional layers. Angle-resolved photoemission spectroscopy and density functional theory studies show that Mn disorder within an SL causes delocalization of electron wave functions and a change of the surface band structure as compared to the ideal MnBi 2 Te 4 /(Bi 2 Te 3 ) n . These findings highlight the critical importance of inter- and intra-SL disorder towards achieving new QAH platforms as well as exploring novel axion physics in intrinsic topological magnets. 
    more » « less
  2. ; ; ; ; ; ; ; ; ; (, Small)
    Abstract The field of photovoltaics is revolutionized in recent years by the development of two–dimensional (2D) type‐II heterostructures. These heterostructures are made up of two different materials with different electronic properties, which allows for the capture of a broader spectrum of solar energy than traditional photovoltaic devices. In this study, the potential of vanadium (V)‐doped WS2is investigated, hereafter labeled V‐WS2, in combination with air‐stable Bi2O2Se for use in high‐performance photovoltaic devices. Various techniques are used to confirm the charge transfer of these heterostructures, including photoluminescence (PL) and Raman spectroscopy, along with Kelvin probe force microscopy (KPFM). The results show that the PL is quenched by 40%, 95%, and 97% for WS2/Bi2O2Se, 0.4 at.% V‐WS2/Bi2O2Se, and 2 at.% V‐WS2/Bi2O2Se, respectively, indicating a superior charge transfer in V‐WS2/Bi2O2Se compared to pristine WS2/Bi2O2Se. The exciton binding energies for WS2/Bi2O2Se, 0.4 at.% V‐WS2/Bi2O2Se and 2 at.% V‐WS2/Bi2O2Se heterostructures are estimated to be ≈130, 100, and 80 meV, respectively, which is much lower than that for monolayer WS2. These findings confirm that by incorporating V‐doped WS2, charge transfer in WS2/Bi2O2Se heterostructures can be tuned, providing a novel light‐harvesting technique for the development of the next generation of photovoltaic devices based on V‐doped transition metal dichalcogenides (TMDCs)/Bi2O2Se. 
    more » « less
  3. ; ; ; ; (, Small)
    Interfacing topological insulators (TI) with magnetic materials enables accessing quantum effects for advanced devices. The synthesis of such heterostructures faces challenges due to interlaying mixing and the often-complex multicomponent materials required to combine the desired properties. An alternative synthesis to direct growth is the modification of 2D materials by topotactic reactions to introduce new functionalities into pre-formed single or few-component 2D sheets. Here, the self-formation of bismuthene (a bilayer of Bi; Bi2) is utilized by thermal decomposition of Bi2Te3 as a platform to create novel 2D overlayers on the TI- substrate. Specifically, the Bi2 layer is modified by reacting it with vapor deposited Mn in an attempt to induce magnetic properties. Scanning tunneling microscopy indicates that the Mn modified surface remains in a planar 2D layer, indicating the formation of an ordered Mn-rich surface layer. Density functional theory (DFT) is used to develop models of both the Bi-rich Bi2Te3 surface as well as their subsequent Mn-modified structure. The DFT models indicate the possibility of magnetic ordering of the high spin Mn2+ ions. The successful synthesis of planar MnBi alloys on a van der Waals material illustrates topotactic reactions as an alternative for creating novel layered heterostructures. 
    more » « less
  4. ; ; ; ; ; ; (, Nanoscale)
    Realization of ferromagnetic (FM) interlayer coupling in magnetic topological insulators (TIs) of the MnBi 2 Te 4 family of materials (MBTs) may pave the way for realizing the high-temperature quantum anomalous Hall effect (high- T QAHE). Here we propose a generic dual d-band (DDB) model to elucidate the energy difference (Δ E = E AFM − E FM ) between the AFM and FM coupling in transition-metal (TM)-doped MBTs, where the valence of TMs splits into d-t 2g and d-e g sub-bands. Remarkably, the DDB shows that Δ E is universally determined by the relative position of the dopant (X) and Mn d-e g / t 2g bands, . If Δ E d > 0, then Δ E > 0 and the desired FM coupling is favored. This surprisingly simple rule is confirmed by first-principles calculations of hole-type 3d and 4d TM dopants. Significantly, by applying the DDB model, we predict the high- T QAHE in the V-doped Mn 2 Bi 2 Te 5 , where the Curie temperature is enhanced by doubling of the MnTe layer, while the topological order mitigated by doping can be restored by strain. 
    more » « less
  5. ; ; ; ; ; ; ; ; ; ; et al (, Advanced Materials)
    Abstract The interface between 2D topological Dirac states and ans‐wave superconductor is expected to support Majorana‐bound states (MBS) that can be used for quantum computing applications. Realizing these novel states of matter and their applications requires control over superconductivity and spin‐orbit coupling to achieve spin‐momentum‐locked topological interface states (TIS) which are simultaneously superconducting. While signatures of MBS have been observed in the magnetic vortex cores of bulk FeTe0.55Se0.45, inhomogeneity and disorder from doping make these signatures unclear and inconsistent between vortices. Here superconductivity is reported in monolayer (ML) FeTe1–ySey(Fe(Te,Se)) grown on Bi2Te3by molecular beam epitaxy (MBE). Spin and angle‐resolved photoemission spectroscopy (SARPES) directly resolve the interfacial spin and electronic structure of Fe(Te,Se)/Bi2Te3heterostructures. Fory = 0.25, the Fe(Te,Se) electronic structure is found to overlap with the Bi2Te3TIS and the desired spin‐momentum locking is not observed. In contrast, fory = 0.1, reduced inhomogeneity measured by scanning tunneling microscopy (STM) and a smaller Fe(Te,Se) Fermi surface with clear spin‐momentum locking in the topological states are found. Hence, it is demonstrated that the Fe(Te,Se)/Bi2Te3system is a highly tunable platform for realizing MBS where reduced doping can improve characteristics important for Majorana interrogation and potential applications. 
    more » « less
  • Citation Formats
  • MLA
  • APA
  • Chicago
  • BibTeX
  • Save / Share this Record
  • Send to Email