Work Methodology and Research Plan
Project Description:
This project aims to comprehensively investigate the potential of 2D monolayers for diverse
clean energy applications, including efficient photocatalytic water splitting, advanced
photovoltaics, and enhanced thermoelectric power generation. By focusing on electronic,
optical, and thermoelectric properties, we seek to uncover novel materials with superior
performance in these critical energy conversion processes.
Project Overview:
The project comprises three interrelated themes, each targeting a specific clean energy
application:
1. Efficient Photocatalytic Water Splitting: In this theme, we will delve into the electronic
structure, band alignment, and charge carrier dynamics of various 2D monolayers. By assessing
their photocatalytic performance, we aim to identify materials with optimal properties for
driving the water splitting reaction efficiently. This will involve theoretical calculations,
experimental validations, and the exploration of heterostructures to enhance photocatalytic
efficiency.
2. Advanced Photovoltaics: Our investigation into 2D monolayers' optical properties and
excitonic behaviors will contribute to the development of cutting-edge photovoltaic
technologies. By designing materials that exhibit excellent light absorption and efficient charge
separation, we seek to enhance the efficiency of photovoltaic devices. This will involve in-
depth optical characterizations, band alignment studies, and the pursuit of novel heterojunction
architectures.
3. Enhanced Thermoelectric Power Generation: The thermoelectric properties of 2D
monolayers will be thoroughly examined to unlock their potential in efficient power generation
from waste heat. By optimizing the electrical conductivity and thermal conductivity, we aim to
engineer materials suitable for thermoelectric applications. This theme will involve
comprehensive material characterizations, including transport properties and theoretical
modeling.
Methodology:
Computational Design of 2D Materials
Task 1.1. Density Functional Theory (DFT) Calculations: Density Functional Theory
calculations will be conducted using the Vienna Ab initio Simulation Package (VASP). The
PBE functional will be employed to treat exchange and correlation interactions. Projected
Augmented Wave (PAW) method will handle electron-ion interactions. An optimal plane wave
cutoff energy will be chosen for accurate calculations. Geometry optimization will utilize tight
energy and force cutoff thresholds. Brillouin zone integration will follow the Monkhorst–Pack
scheme. Convergence of k-points will be determined, and the optimal set will be employed. To
prevent interlayer interactions, Z-direction vacuum layers will be introduced. Van der Waals
(vdW) interactions will be incorporated to account for long-range effects and stability.
Task 1.2. Machine Learning Predictions and Validation: The DFT calculations will serve
as inputs for machine learning algorithms. These algorithms will help predict the photoelectric
conversion coefficients of the materials, thus enabling the identification of the most promising
candidates without the need for exhaustive experimentation. These predictions will be cross-
validated with experimental data to ensure their accuracy and reliability.
Task 1.3. Phonon Calculations: To verify the dynamical stability of predicted structures,
phonon dispersion calculations will be performed. Displaced atom configurations' forces will
be computed using DFT. These force-displacement sets will be utilized in PHONOPY or
ALAMODE packages for phonon dispersion relations. The harmonic approximation will aid
force constant fitting and vibrational frequency calculations. Structures with zero imaginary
vibrational modes will indicate dynamic stability and will proceed to accurate electronic
structure calculations and experimental validation.
Task 1.4. Formation Energy and Convex Hull: The chemical stability of compounds will
be determined through cohesive energy and formation free energy calculations. Gibbs free
energy of the compound and reference structures will enable formation free energy
calculation. Negative formation free energy signifies stable chemical stability. Composition-
dependent convex hull calculations will provide insights into the chemical stability of
proposed structures.
Task 1.5. Interface and Heterostructure Design: Efficient photocatalysts will be targeted
through interface or heterostructure design involving compound combinations. Interfaces and
heterostructures may harness in-built electric fields to reduce exciton binding energy and
charge carrier recombination. Pathways for faster charge carrier mobility will be explored.
Dynamical and chemical stability of designed structures will be verified before experimental
synthesis.
Task 1.6. GW and GW-BSE Optics: Quasiparticle GW calculations will be performed atop
PBE or HSE Self Consistent calculations. BSE calculations will extend to GW calculations to
obtain frequency-dependent dielectric functions. These will facilitate optical absorption and
exciton binding energy assessments. Calculated values will contribute to band alignment
calculations and characterizing excitons using BSE.
Task 1.7. Strain and Defect Engineering: Intrinsic defects, such as vacancies, doping, and
strain-induced lattice distortions, will be investigated for enhancing catalytic activity. Doping
and lattice distortion concepts will enhance charge carrier dynamics and stability through
strain-tuning of phonons.
Task 1.8. Data-Driven Prediction using ML Methods: ML methods will be employed to
predict efficient photo-catalytic 2D materials. Utilizing DFT data sets, known parameters
and calculated values will be incorporated as attributes in regression models. Linear and non-
linear algorithms will be assessed, constructing models to predict responses based on input
variables. Model performance will be gauged using metrics such as root mean square error,
coefficient of determination, and more.
Task 1.9. Cross Validation of ML Predictions: Cross-validation will assess model
effectiveness, especially for overfitting mitigation. Hyperparameters will be tuned to
minimize test error. Cross-validation will ensure robustness of models.
Task 1.10. Prediction of Photocatalytic Properties: This section will present the results of
the DFT calculations, focusing on the prediction of photocatalytic properties. It will discuss
the accuracy of different exchange-correlation functionals in estimating bandgaps, band edge
levels, and optical properties. The discrepancies between theoretical predictions and
experimental data will be highlighted, emphasizing the need for more advanced methods, such
as GW calculations and BSE approaches.
Task 1.11. Engineering 2D Photocatalysis: This section will delve into the strategies
employed to engineer 2D photocatalysts for enhanced water splitting efficiency. It will discuss
the role of doping, defects, alloying, and band edge tuning in optimizing photocatalytic
properties. The impact of these techniques on electronic and optical properties will be
examined, with a focus on how simulations aid in understanding the underlying mechanisms.
Conclusion: The conclusion will summarize the key findings of the project, highlighting the
importance of ab initio simulations in understanding and designing 2D photocatalytic
materials. It will emphasize the potential of 2D materials to revolutionize clean energy
production and underscore the role of theoretical insights in shaping future advancements in
photocatalysis.
Time Schedule of activities
Time period Task to complete
DFT modeling to discover stable 2D materials with improved photo-
0-6 months
conversion and thermoelectric capabilities..
Implementing machine learning algorithms to predict photoelectric
6-12 months conversion coefficients and thermoelectric performance based on
DFT insights for accurate screening.
Implementing doping, defect engineering and strain engineering to
12-18 months
optimize photovoltaic applications of 2D materials.
Scientific paper writing for publication in international journal will
18-24 month
be taken up and final report will be prepared.
