Bandgap-tunable lateral and vertical heterostructures based on monolayer Mo1-xWxS2 alloys

The fabrication of heterostructures of two-dimensional semiconductors with specific bandgaps is an important approach to realizing the full potential of these materials in electronic and optoelectronic devices. Several groups have recently reported the direct growth of lateral and vertical heterostructures based on monolayers of typical semiconducting transition metal dichalcogenides (TMDCs) such as WSe2, MoSe2, WS2, and MoS2. Here, we demonstrate the single-step direct growth of lateral and vertical heterostructures based on bandgap-tunable Mo1-xWxS2 alloy monolayers by the sulfurization of patterned thin films of WO3 and MoO3. These patterned films are capable of generating a wide variety of concentration gradients by the diffusion of transition metals during the crystal growth phase. Under high temperatures, this leads to the formation of monolayer crystals of Mo1-xWxS2 alloys with various compositions and bandgaps, depending on the positions of the crystals on the substrates. Heterostructures of these alloys are obtained through stepwise changes in the ratio of W/Mo within a single domain during low-temperature growth. The stabilization of the monolayer Mo1-xWxS2 alloys, which often degrade even under gentle conditions, was accomplished by coating the alloys with other monolayers. The present findings demonstrate an efficient means of both studying and optimizing the optical and electrical properties of TMDC-based heterostructures to allow use of the materials in future device applications.

[1]  Pinshane Y. Huang,et al.  Graphene and boron nitride lateral heterostructures for atomically thin circuitry , 2012, Nature.

[2]  P. McEuen,et al.  Hyperspectral imaging of structure and composition in atomically thin heterostructures. , 2013, Nano letters.

[3]  Aydin Babakhani,et al.  In-plane heterostructures of graphene and hexagonal boron nitride with controlled domain sizes. , 2013, Nature nanotechnology.

[4]  J. Tour,et al.  Thickness-dependent patterning of MoS2 sheets with well-oriented triangular pits by heating in air , 2013, Nano Research.

[5]  K. L. Shepard,et al.  One-Dimensional Electrical Contact to a Two-Dimensional Material , 2013, Science.

[6]  A. Splendiani,et al.  Emerging photoluminescence in monolayer MoS2. , 2010, Nano letters.

[7]  J. Grossman,et al.  Defects activated photoluminescence in two-dimensional semiconductors: interplay between bound, charged, and free excitons , 2013, Scientific Reports.

[8]  Wang Yao,et al.  Lateral heterojunctions within monolayer MoSe2-WSe2 semiconductors. , 2014, Nature materials.

[9]  Arindam Ghosh,et al.  Graphene-MoS2 hybrid structures for multifunctional photoresponsive memory devices. , 2013, Nature nanotechnology.

[10]  K. Shepard,et al.  Boron nitride substrates for high-quality graphene electronics. , 2010, Nature nanotechnology.

[11]  E. Sutter,et al.  Interface formation in monolayer graphene-boron nitride heterostructures. , 2012, Nano letters.

[12]  Yiming Zhu,et al.  Composition-dependent Raman modes of Mo(1-x)W(x)S2 monolayer alloys. , 2014, Nanoscale.

[13]  Xiaohui Qiu,et al.  Toward single-layer uniform hexagonal boron nitride-graphene patchworks with zigzag linking edges. , 2013, Nano letters.

[14]  K. Shepard,et al.  Graphene based heterostructures , 2012 .

[15]  Y. Sasaki,et al.  Fabrication and Characterization of Graphene/Hexagonal Boron Nitride Hybrid Sheets , 2012 .

[16]  A. V. Kretinin,et al.  Detecting topological currents in graphene superlattices , 2014, Science.

[17]  Dong Wang,et al.  Tunable band gap photoluminescence from atomically thin transition-metal dichalcogenide alloys. , 2013, ACS nano.

[18]  S. Haigh,et al.  Vertical field-effect transistor based on graphene-WS2 heterostructures for flexible and transparent electronics. , 2012, Nature nanotechnology.

[19]  T. Taniguchi,et al.  Massive Dirac Fermions and Hofstadter Butterfly in a van der Waals Heterostructure , 2013, Science.

[20]  Qing Hua Wang,et al.  Electronics and optoelectronics of two-dimensional transition metal dichalcogenides. , 2012, Nature nanotechnology.

[21]  Yi Liu,et al.  Equally efficient interlayer exciton relaxation and improved absorption in epitaxial and nonepitaxial MoS2/WS2 heterostructures. , 2014, Nano letters.

[22]  Yu Huang,et al.  Lateral epitaxial growth of two-dimensional layered semiconductor heterojunctions. , 2014, Nature nanotechnology.

[23]  Ruitao Lv,et al.  Extraordinary room-temperature photoluminescence in triangular WS2 monolayers. , 2012, Nano letters.

[24]  S. Okada,et al.  Enhanced chemical reactivity of graphene induced by mechanical strain. , 2013, ACS nano.

[25]  J. Shan,et al.  Atomically thin MoS₂: a new direct-gap semiconductor. , 2010, Physical review letters.

[26]  Kuan-Hua Huang,et al.  Synthesis of lateral heterostructures of semiconducting atomic layers. , 2015, Nano letters.

[27]  Jun Lou,et al.  Vertical and in-plane heterostructures from WS2/MoS2 monolayers. , 2014, Nature materials.

[28]  Xu Cui,et al.  Flexible and transparent MoS2 field-effect transistors on hexagonal boron nitride-graphene heterostructures. , 2013, ACS nano.

[29]  R. Piner,et al.  AN IMPROVED METHOD FOR TRANSFERRING GRAPHENE GROWN BY CHEMICAL VAPOR DEPOSITION , 2012 .

[30]  Hua Zhang,et al.  The chemistry of two-dimensional layered transition metal dichalcogenide nanosheets. , 2013, Nature chemistry.

[31]  L. Chu,et al.  Evolution of electronic structure in atomically thin sheets of WS2 and WSe2. , 2012, ACS nano.

[32]  SUPARNA DUTTASINHA,et al.  Van der Waals heterostructures , 2013, Nature.

[33]  Hiroki Hibino,et al.  Growth and Optical Properties of High-Quality Monolayer WS2 on Graphite. , 2015, ACS nano.

[34]  S. Pei,et al.  Control and characterization of individual grains and grain boundaries in graphene grown by chemical vapour deposition. , 2010, Nature materials.

[35]  Yiming Zhu,et al.  Correction: Composition-dependent Raman modes of Mo1-xWxS2 monolayer alloys. , 2016, Nanoscale.

[36]  J. Idrobo,et al.  Heteroepitaxial Growth of Two-Dimensional Hexagonal Boron Nitride Templated by Graphene Edges , 2014, Science.

[37]  P. Ajayan,et al.  Band gap engineering and layer-by-layer mapping of selenium-doped molybdenum disulfide. , 2014, Nano letters.

[38]  Satoru Suzuki,et al.  Scalable synthesis of layer-controlled WS2 and MoS2 sheets by sulfurization of thin metal films , 2014 .