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PreprintCC BYChemRxiv

Unveiling Photoluminescent N-Heterocyclic Silylene-Silver(I) Amides as Dual-Function Photosensitizers and Third-Harmonic Generators

  • Moushakhi Ghosh1,2
  • Abhijit Chatterjee1,2
  • Prakash Panwaria1,2
  • Riteeka Tanwar1,2
  • K. S. Ananthram3
  • Rishukumar Panday1,2
  • Kartick Tarafdar4,5
  • Pankaj Mandal1,2
  • Shabana Khan1,2
  • SHABANA KHAN
5 affiliations
  1. 1Department of Chemistry
  2. 2Indian Institute of Science Education and Research (IISER
  3. 3Department of Physics, NITK Surathkal, Srinivas Nagar, Mangalore, Karnataka-575025
  4. 4Department of Physics
  5. 5Indian Institute of Technology Kharagpur
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Abstract

N-Heterocyclic silylenes (NHSis) have evolved from laboratory curiosities to versatile ligands for small-molecule activation and homogeneous catalysis, yet their potential in photophysics and optical materials remains unexplored. Here, we report for the first time a series of luminescent NHSi-ligated Ag(I) amide complexes (2–4) exhibiting remarkable thermally activated delayed fluorescence (TADF) and dual-emissive behavior. The NHSi→Ag–diphenylamine complex (2) displays pronounced TADF with an exceptionally small singlet–triplet energy gap (ΔES–T ≈ 0.006 eV) and a short delayed-fluorescence lifetime (τTADF ≈ 0.35 μs at 300 K), indicative of efficient reverse intersystem crossing (RISC) driven by NHSi-to-metal amide charge transfer. Complexes 3 and 4 exhibit dual emission and serve as efficient photosensitizers for singlet oxygen (1O2) generation. Remarkably, these complexes (2-4) demonstrate coherent photon up-conversion via third-harmonic generation (THG), representing the first such observation in main-group organometallic chemistry. These findings unveil a new class of main-group metal complexes as promising photosensitizers and third-order nonlinear optical materials.

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Cite

BibTeXRIS
BibTeX
@misc{ghosh2026unveiling,
  title = {{Unveiling Photoluminescent N-Heterocyclic Silylene-Silver(I) Amides as Dual-Function Photosensitizers and Third-Harmonic Generators}},
  author = {Moushakhi Ghosh and Abhijit Chatterjee and Prakash Panwaria and Riteeka Tanwar and K. S. Ananthram and Rishukumar Panday and Kartick Tarafdar and Pankaj Mandal and Shabana Khan and SHABANA KHAN},
  howpublished = {ChemRxiv},
  year = {2026},
  month = oct,
  doi = {10.26434/chemrxiv.15010162/v1},
  url = {https://chemrxiv.org/doi/full/10.26434/chemrxiv.15010162/v1},
  note = {CC BY},
}
RIS
TY  - UNPB
TI  - Unveiling Photoluminescent N-Heterocyclic Silylene-Silver(I) Amides as Dual-Function Photosensitizers and Third-Harmonic Generators
AU  - Moushakhi Ghosh
AU  - Abhijit Chatterjee
AU  - Prakash Panwaria
AU  - Riteeka Tanwar
AU  - K. S. Ananthram
AU  - Rishukumar Panday
AU  - Kartick Tarafdar
AU  - Pankaj Mandal
AU  - Shabana Khan
AU  - SHABANA KHAN
PY  - 2026
DA  - 2026/10/09
PB  - ChemRxiv
DO  - 10.26434/chemrxiv.15010162/v1
UR  - https://chemrxiv.org/doi/full/10.26434/chemrxiv.15010162/v1
AB  - N-Heterocyclic silylenes (NHSis) have evolved from laboratory curiosities to versatile ligands for small-molecule activation and homogeneous catalysis, yet their potential in photophysics and optical materials remains unexplored. Here, we report for the first time a series of luminescent NHSi-ligated Ag(I) amide complexes (2–4) exhibiting remarkable thermally activated delayed fluorescence (TADF) and dual-emissive behavior. The NHSi→Ag–diphenylamine complex (2) displays pronounced TADF with an exceptionally small singlet–triplet energy gap (ΔES–T ≈ 0.006 eV) and a short delayed-fluorescence lifetime (τTADF ≈ 0.35 μs at 300 K), indicative of efficient reverse intersystem crossing (RISC) driven by NHSi-to-metal amide charge transfer. Complexes 3 and 4 exhibit dual emission and serve as efficient photosensitizers for singlet oxygen (1O2) generation. Remarkably, these complexes (2-4) demonstrate coherent photon up-conversion via third-harmonic generation (THG), representing the first such observation in main-group organometallic chemistry. These findings unveil a new class of main-group metal complexes as promising photosensitizers and third-order nonlinear optical materials.
ER  -