Charge Carrier Dynamics at the Interface of 2D Metal–Organic Frameworks and Hybrid Perovskites for Solar Energy Harvesting

Stanton, Robert; Trivedi, Dhara J.

doi:10.1021/acs.nanolett.3c04054

Cited by 3 publications

(3 citation statements)

References 56 publications

(72 reference statements)

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“…Perovskite-based photovoltaics have served as an indispensable class of materials in solar energy harvesting for decades, with improvements over the past decade leading to power conversion efficiencies as high as 25.8%. − Perovskite solar cells, however, exhibit persistent challenges regarding stability, toxicity of building components, and device longevity which motivate ongoing research efforts to mitigate these pitfalls. − These efforts can largely be categorized by one of three approaches: (1) the investigation into perovskite-based materials of reduced dimensionality, most commonly two-dimensional perovskites (2DPKs), (2) the utilization of a singular replacement divalent B-site cation such as tin or germanium, or (3) the employment of lead-free mixed-metal perovskites that have been termed double perovskites (DPKs) in the literature. − The above approaches have broadly expanded the search space of perovskite-based photovoltaic materials, and mixed success has been achieved in identifying materials which maintain the optoelectronic properties that make lead-iodide perovskites so attractive while mitigating the concerns that come along with them. − …”

Section: Introductionmentioning

confidence: 99%

Two-Dimensional Double Perovskites in the Dion–Jacobson Phase Alleviate Parity Forbidden Transitions for Photovoltaic Applications

Stanton,

Trivedi

2024

ACS Appl. Energy Mater.

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Two-dimensional double perovskites have recently been identified as a potential class of materials for the improvement of halide-perovskite-based solar cell technology. The expanded set of utilizable B-and B′-site cations afforded to double perovskites, combined with tunable structural and electronic properties in twodimensional perovskites, leads to a highly modifiable set of materials, which have yet to be explored. In this study, we investigate the structural, electronic, and thermoelectric properties of these materials and identify a number of key structure−property relationships governing their performance. In the process, we demonstrate a link between the relative electronegativities of the building components and the resultant geometric structures. Furthermore, we provide insights aimed toward alleviating concerns associated with parity forbidden transitions which plague many double perovskite systems. In addition, we identify a number of twodimensional double perovskites including the mixed-oxidation state In 25 Tl 75 Cl-based system which displays optically active transitions as low as 1.41 eV across the Brillouin zone and indicators pointing toward stable experimental synthesis.

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Section: Introductionmentioning

confidence: 99%

Two-Dimensional Double Perovskites in the Dion–Jacobson Phase Alleviate Parity Forbidden Transitions for Photovoltaic Applications

Stanton,

Trivedi

2024

ACS Appl. Energy Mater.

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“…The standard NBRA NA-MD computations typically involve precomputed nuclear trajectories (guiding trajectories) that parametrize the electronic dynamics of a system. While the guiding trajectories may be obtained relatively inexpensively using adiabatic molecular dynamics with force fields, − semiempirical or xTB methods, ,, the propagation of electronic dynamics requires more expensive DFT calculations. Obtaining accurate energies and time overlaps may require the use of expensive hybrid functionals, with the steeply increased computational expenses .…”

Section: Introductionmentioning

confidence: 99%

Machine-Learned Kohn–Sham Hamiltonian Mapping for Nonadiabatic Molecular Dynamics

Shakiba,

Akimov

2024

J. Chem. Theory Comput.

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In this work, we report a simple, efficient, and scalable machinelearning (ML) approach for mapping non-self-consistent Kohn−Sham Hamiltonians constructed with one kind of density functional to the nearly selfconsistent Hamiltonians constructed with another kind of density functional. This approach is designed as a fast surrogate Hamiltonian calculator for use in long nonadiabatic dynamics simulations of large atomistic systems. In this approach, the input and output features are Hamiltonian matrices computed from different levels of theory. We demonstrate that the developed ML-based Hamiltonian mapping method (1) speeds up the calculations by several orders of magnitude, ( 2) is conceptually simpler than alternative ML approaches, (3) is applicable to different systems and sizes and can be used for mapping Hamiltonians constructed with arbitrary density functionals, (4) requires a modest training data, learns fast, and generates molecular orbitals and their energies with the accuracy nearly matching that of conventional calculations, and (5) when applied to nonadiabatic dynamics simulation of excitation energy relaxation in large systems yields the corresponding time scales within the margin of error of the conventional calculations. Using this approach, we explore the excitation energy relaxation in C 60 fullerene and Si 75 H 64 quantum dot structures and derive qualitative and quantitative insights into dynamics in these systems.

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“…Numerous types of sensitizers are being widely researched nowadays including metal free organic dyes like coumarins, polyenes, hemicyanines, catechols; metal organic complexes; porphyrin; − and ruthenium complexes . Among these, porphyrin derivatives have emerged as the focal point of interest due to their tunable absorption properties, excellent light stability, as well as their electrochemical stability, and exceptional photophysical properties .…”

Section: Introductionmentioning

confidence: 99%

Photoinduced Charge Transport Dynamics under the Influence of an Electric Field on Dye-Sensitized Solar Cells with a D−π–A Structure

Kaur,

Goel

2024

ACS Appl. Electron. Mater.

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First-principle studies within the formalism of density functional theory have been performed to investigate the photoinduced charge transfer in Zn-porphyrin based dye-sensitized solar cells (DSSCs). The FSQ101, SM315-based Zn-porphyrin dye has been chosen as a valuable platform to explore the interplay between the direction and strength of the applied electric field and photovoltaic performance. The model system has an electron-rich donor group, a π-linker as a bridge, and a cyanoacrylic acid as an acceptor group. All simulations have been conducted with respect to the TiO2 semiconductor and normalI 3 − /I– electrolyte. The applied electric field (−30 × 10–5 au to 30 × 10–5 au) mimics the inner electric field generated in practice in solar cell devices. Static and time-dependent density functional calculations provide a comprehensive analysis of the dynamics of photovoltaic properties in relation to the applied field strength. The results demonstrate that an electric field can effectively modulate the photoelectric characteristics and enhance the charge transfer process of the dye molecule. When the field is along the positive X-axis, dye exhibits a narrow band gap, well-defined charge separated states, larger λmax, and broader and red-shifted bands toward the near-infrared region. The analysis of frontier orbitals, absorption spectra, chemical reactivity parameters, nonlinear optical properties, and photovoltaic properties (LHE, J SC, V OC, italicE normald normaly normale * , ΔG inj, ΔG reg, EBE, V da, λr, k) provides molecular level understanding of underlying processes such as photoinduced electron injection, generation of electron–hole pair, and intramolecular charge transfer (ICT) that are crucial in deciding the efficiency of the DSSCs. The charge density difference plots were plotted at different field strengths to classify the electronic transitions as ICT or local excited (LE) transitions. The study substantiates the improved performance of the designed DSSC when subjected to a positive field compared to negative and field-free conditions.

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Charge Carrier Dynamics at the Interface of 2D Metal–Organic Frameworks and Hybrid Perovskites for Solar Energy Harvesting

Cited by 3 publications

References 56 publications

Two-Dimensional Double Perovskites in the Dion–Jacobson Phase Alleviate Parity Forbidden Transitions for Photovoltaic Applications

Two-Dimensional Double Perovskites in the Dion–Jacobson Phase Alleviate Parity Forbidden Transitions for Photovoltaic Applications

Machine-Learned Kohn–Sham Hamiltonian Mapping for Nonadiabatic Molecular Dynamics

Photoinduced Charge Transport Dynamics under the Influence of an Electric Field on Dye-Sensitized Solar Cells with a D−π–A Structure

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