Resumen
Optoelectronic properties of anisotropic crystals vary with direction requiring that the orientation of molecular organic semiconductor crystals is controlled in optoelectronic device active layers to achieve optimal performance. Here, a generalizable strategy to introduce periodic variations in the out-of-plane orientations of 5,11-bis(triisopropylsilylethynyl)anthradithiophene (TIPS ADT) crystals is presented. TIPS ADT crystallized from the melt in the presence of 16 wt.% polyethylene (PE) forms banded spherulites of crystalline fibrils that twist in concert about the radial growth direction. These spherulites exhibit band-dependent light absorption, photoluminescence, and Raman scattering depending on the local orientation of crystals. Mueller matrix imaging reveals strong circular extinction (CE), with TIPS ADT banded spherulites exhibiting domains of positive or negative CE signal depending on the crystal twisting sense. Furthermore, orientation-dependent enhancement in charge injection and extraction in films of twisted TIPS ADT crystals compared to films of straight crystals is visualized in local conductive atomic force microscopy maps. This enhancement leads to 3.3- and 6.2-times larger photocurrents and external quantum efficiencies, respectively, in photodetectors comprising twisted crystals than those comprising straight crystals.
| Idioma original | English |
|---|---|
| Número de artículo | 2212531 |
| Publicación | Advanced Functional Materials |
| Volumen | 33 |
| N.º | 19 |
| DOI | |
| Estado | Published - may 8 2023 |
Nota bibliográfica
Publisher Copyright:© 2023 Wiley-VCH GmbH.
Financiación
This work at New York University was primarily supported by the National Science Foundation (NSF) award number DMR-2003997 and secondarily by the New York University Materials Research Science and Engineering Center (MRSEC) program of the NSF under award number DMR-1420073. The authors also acknowledge support from PSEG to advance energy innovation at Stevens Institute of Technology. The work at the University of Kentucky was supported by the NSF award number DMR-1627428 (synthetic efforts of JEA and EKY and computational efforts of LY and CR) and cooperative agreement number 1849213 (computational efforts of VB). Supercomputing resources were provided by the University of Kentucky Information Technology Department and Center for Computational Sciences (CCS). Use of the Advanced Photon Source at Argonne National Laboratory was supported by the U. S. Department of Energy, Office of Science, Office of Basic Energy Sciences, under Contract No. DE-AC02-06CH11357. The X-ray microdiffractometer with GADDS was acquired through the support of the NSF under award number CRIF/CHE-0840277 and NSF MRSEC Program under award number DMR-0820341. NB, JB and TBMA thank the University of Geneva for the financial support. The authors also thank Prof. Ayaskanta Sahu and Håvard Mølnås for access to the EQE measurement setup. This work at New York University was primarily supported by the National Science Foundation (NSF) award number DMR‐2003997 and secondarily by the New York University Materials Research Science and Engineering Center (MRSEC) program of the NSF under award number DMR‐1420073. The authors also acknowledge support from PSEG to advance energy innovation at Stevens Institute of Technology. The work at the University of Kentucky was supported by the NSF award number DMR‐1627428 (synthetic efforts of JEA and EKY and computational efforts of LY and CR) and cooperative agreement number 1849213 (computational efforts of VB). Supercomputing resources were provided by the University of Kentucky Information Technology Department and Center for Computational Sciences (CCS). Use of the Advanced Photon Source at Argonne National Laboratory was supported by the U. S. Department of Energy, Office of Science, Office of Basic Energy Sciences, under Contract No. DE‐AC02‐06CH11357. The X‐ray microdiffractometer with GADDS was acquired through the support of the NSF under award number CRIF/CHE‐0840277 and NSF MRSEC Program under award number DMR‐0820341. NB, JB and TBMA thank the University of Geneva for the financial support. The authors also thank Prof. Ayaskanta Sahu and Håvard Mølnås for access to the EQE measurement setup.
| Financiadores | Número del financiador |
|---|---|
| Université de Genève | |
| New York University Materials Research Science and Engineering Center | |
| U.S. Department of Energy EPSCoR | |
| Office of Science Programs | |
| University of Kentucky Information Technology Department and Center for Computational Sciences | |
| Materials Research Science and Engineering Center, Harvard University | DMR‐0820341, DMR‐1420073 |
| PSEG | DMR‐1627428 |
| DOE Basic Energy Sciences | DE‐AC02‐06CH11357, CRIF/CHE‐0840277 |
| National Science Foundation Arctic Social Science Program | 1849213, DMR‐2003997 |
ASJC Scopus subject areas
- Electronic, Optical and Magnetic Materials
- General Chemistry
- Biomaterials
- General Materials Science
- Condensed Matter Physics
- Electrochemistry