Supporting Information: Lateral Versus Vertical Growth of Two-Dimensional Layered Transition-Metal Dichalcogenides (MoS2)
Summary¶
This Supporting Information PDF accompanies the Nano Letters thermodynamic analysis of MoS₂ chemical vapor deposition growth windows, focusing on competition between lateral monolayer extension and bilayer nucleation. Rather than introducing new reactive molecular dynamics models, the SI supplies the computational chemistry backbone: Vienna Ab initio Simulation Package–style density functional theory (DFT) settings, additional DFT energy surfaces, CALPHAD thermodynamic database construction for the molybdenum–sulfur subsystem, and multicomponent gas-phase analysis for Mo–S–O–H chemistry using the SGTE-SSUB database. The SI explicitly tests multiple exchange–correlation treatments beyond the PBE+D3 combination highlighted in the main text, including bare GGA-PBE, PBEsol, and PBEsol+D3, with Table S3 benchmarking equations of state for MoS₂, α-alumina, body-centered-cubic molybdenum, and graphite against experiments; the authors state that PBE+D3 offers a favorable balance of efficiency and agreement for the set of training structures used. Supplementary Table S5 bundles a complete thermodynamic database (TDB-style) for the Mo–S system, while supplementary figures extend main-text phase diagrams into broader ranges of temperature, pressure, and composition, clarifying partial pressures of relevant sulfur and oxygen carriers during growth. Operators should pair this file with [[2016shang-venue-nl-2016-02443v]] for scientific conclusions about growth modes.
Methods¶
This SI documents DFT settings and CALPHAD database construction for the MoS\(_2\) growth thermodynamics in [[2016shang-venue-nl-2016-02443v]]. Table S2 lists supercell sizes, plane-wave cutoffs, k-point meshes, and convergence thresholds for periodic MoS\(_2\) and related benchmarks, comparing PBE, PBE+D3, PBEsol, and PBEsol+D3. Table S3 benchmarks equations of state for MoS\(_2\), α-alumina, bcc Mo, and graphite against experiment to justify functional choices. Tables S4–S6 and the bundled Mo–S thermodynamic database support the CALPHAD fit to experimental phase equilibria; supplementary figures extend gas speciation, T–x sections, and P–T diagrams for representative CVD-like gas mixtures.
MD application / force-field training. N/A — the SI is QM + thermodynamics documentation, not a reactive MD or ReaxFF protocol sheet.
DFT documentation in the SI. Tables summarize PBE/PBEsol functionals with and without Grimme D3 dispersion, plane-wave cutoffs, k-point meshes, relaxed geometry benchmarks (equations of state reporting energy versus volume for MoS\(_2\), graphite, bcc Mo, and α-alumina), and derived thermodynamic properties feeding CALPHAD. N/A — full numerical grids on this wiki page—read pdf_path.
Findings¶
Role of the SI. The package makes DFT training data and CALPHAD optimization auditable—how equation-of-state benchmarks and Mo–S parameters constrain the P–T–x windows discussed in the main letter. It does not establish standalone ReaxFF or production MD benchmarks.
Corpus honesty. Headline conclusions on lateral versus vertical growth belong to [[2016shang-venue-nl-2016-02443v]]; use pdf_path for full tables (extraction_quality: partial).
Limitations¶
Corpus extraction quality is flagged partial; rely on the PDF for complete tables. Any mismatch between DFT functionals must be resolved against the main article’s chosen reference treatment before porting numbers into other workflows.
Relevance to group¶
The SI underpins a flagship Penn State–affiliated MoS₂ thermodynamics publication in the corpus, providing DFT and CALPHAD inputs that contextualize later ReaxFF studies of MoS₂ from separate papers.
MAS / retrieval notes¶
Route growth-window questions to [[2016shang-venue-nl-2016-02443v]] for conclusions; use this SI page for DFT k-mesh/cutoff tables and CALPHAD TDB filenames. Extraction quality is partial in corpus metadata—verify critical numbers against the PDF bytes. When users ask for “MoS₂ phase diagrams,” distinguish gas-phase speciation figures in the SI from thin-film growth conclusions in the main letter.
Citations and evidence anchors¶
- Primary PDF:
papers/Others/Shang_Liu_MoS2_growth_NanoLetters2016_SI.pdf - Text-aligned pointers:
normalized/extracts/2016shang-venue-paper_p1-2.txt