Validation of Semi-Empirical xTB Methods for High-Throughput Screening of TADF Emitters: A 747-Molecule Benchmark Study
Fuente:
arXiv
Salvato in:
| Autori principali: | , , , |
|---|---|
| Natura: | Preprint |
| Pubblicazione: |
2025
|
| Soggetti: | |
| Accesso online: | |
| Tags: |
Aggiungi Tag
Nessun Tag, puoi essere il primo ad aggiungerne!!
|
| _version_ | 1866915836381364224 |
|---|---|
| author | Njafa, Jean-Pierre Tchapet Tcheuffa, Elvira Vanelle Kameni Maghame, Aissatou Engo, Serge Guy Nana |
| author_facet | Njafa, Jean-Pierre Tchapet Tcheuffa, Elvira Vanelle Kameni Maghame, Aissatou Engo, Serge Guy Nana |
| contents | Thermally activated delayed fluorescence (TADF) emitters are essential for next-generation, high-efficiency organic light-emitting diodes (OLEDs), yet their rational design is hampered by the high computational cost of accurate excited-state predictions. Here, we present a comprehensive benchmark study validating semi-empirical extended tight-binding (xTB) methods -- specifically sTDA-xTB and sTD-DFT-xTB -- for the high-throughput screening of TADF materials. Using an unprecedentedly large dataset of \num{747} experimentally characterized emitters, our framework demonstrates a computational cost reduction of over \qty{99}{\percent} compared to conventional TD-DFT, while maintaining strong internal consistency between methods (Pearson $r \approx \num{0.82}$ for \deltaest), validating their utility for relative molecular ranking. Validation against \num{312} experimental \deltaest values reveals a mean absolute error of approximately \qty{0.17}{\electronvolt}, a discrepancy attributed to the vertical approximation inherent to the HTS protocol, underscoring the methods' role in screening rather than quantitative prediction. Through large-scale data analysis, we statistically validate key design principles, confirming the superior performance of Donor-Acceptor-Donor (D-A-D) architectures and identifying an optimal D-A torsional angle range of \qtyrange{50}{90}{\degree} for efficient TADF. Principal Component Analysis reveals that the complex property space is fundamentally low-dimensional, with three components capturing nearly \qty{90}{\percent} of the variance. This work establishes these semi-empirical methods as powerful, cost-effective tools for accelerating TADF discovery and provides a robust set of data-driven design rules and methodological guidelines for the computational materials science community. |
| format | Preprint |
| id |
arxiv_https___arxiv_org_abs_2511_00922 |
| institution | arXiv |
| publishDate | 2025 |
| record_format | arxiv |
| spellingShingle | Validation of Semi-Empirical xTB Methods for High-Throughput Screening of TADF Emitters: A 747-Molecule Benchmark Study Njafa, Jean-Pierre Tchapet Tcheuffa, Elvira Vanelle Kameni Maghame, Aissatou Engo, Serge Guy Nana Materials Science Thermally activated delayed fluorescence (TADF) emitters are essential for next-generation, high-efficiency organic light-emitting diodes (OLEDs), yet their rational design is hampered by the high computational cost of accurate excited-state predictions. Here, we present a comprehensive benchmark study validating semi-empirical extended tight-binding (xTB) methods -- specifically sTDA-xTB and sTD-DFT-xTB -- for the high-throughput screening of TADF materials. Using an unprecedentedly large dataset of \num{747} experimentally characterized emitters, our framework demonstrates a computational cost reduction of over \qty{99}{\percent} compared to conventional TD-DFT, while maintaining strong internal consistency between methods (Pearson $r \approx \num{0.82}$ for \deltaest), validating their utility for relative molecular ranking. Validation against \num{312} experimental \deltaest values reveals a mean absolute error of approximately \qty{0.17}{\electronvolt}, a discrepancy attributed to the vertical approximation inherent to the HTS protocol, underscoring the methods' role in screening rather than quantitative prediction. Through large-scale data analysis, we statistically validate key design principles, confirming the superior performance of Donor-Acceptor-Donor (D-A-D) architectures and identifying an optimal D-A torsional angle range of \qtyrange{50}{90}{\degree} for efficient TADF. Principal Component Analysis reveals that the complex property space is fundamentally low-dimensional, with three components capturing nearly \qty{90}{\percent} of the variance. This work establishes these semi-empirical methods as powerful, cost-effective tools for accelerating TADF discovery and provides a robust set of data-driven design rules and methodological guidelines for the computational materials science community. |
| title | Validation of Semi-Empirical xTB Methods for High-Throughput Screening of TADF Emitters: A 747-Molecule Benchmark Study |
| topic | Materials Science |
| url | https://arxiv.org/abs/2511.00922 |