Avoiding the Center-Symmetry Trap: Programmed Assembly of Dipolar Precursors into Porous, Crystalline Molecular Thin Films.

electrostatic design metal-organic frameworks second-harmonic generation

Journal

Advanced materials (Deerfield Beach, Fla.)
ISSN: 1521-4095
Titre abrégé: Adv Mater
Pays: Germany
ID NLM: 9885358

Informations de publication

Date de publication:
Sep 2021
Historique:
revised: 17 06 2021
received: 29 04 2021
pubmed: 23 7 2021
medline: 23 7 2021
entrez: 22 7 2021
Statut: ppublish

Résumé

Liquid-phase, quasi-epitaxial growth is used to stack asymmetric, dipolar organic compounds on inorganic substrates, permitting porous, crystalline molecular materials that lack inversion symmetry. This allows material fabrication with built-in electric fields. A new programmed assembly strategy based on metal-organic frameworks (MOFs) is described that facilitates crystalline, noncentrosymmetric space groups for achiral compounds. Electric fields are integrated into crystalline, porous thin films with an orientation normal to the substrate. Changes in electrostatic potential are detected via core-level shifts of marker atoms on the MOF thin films and agree with theoretical results. The integration of built-in electric fields into organic, crystalline, and porous materials creates possibilities for band structure engineering to control the alignment of electronic levels in organic molecules. Built-in electric fields may also be used to tune the transfer of charges from donors loaded via programmed assembly into MOF pores. Applications include organic electronics, photonics, and nonlinear optics, since the absence of inversion symmetry results in a clear second-harmonic generation signal.

Identifiants

pubmed: 34291511
doi: 10.1002/adma.202103287
doi:

Types de publication

Journal Article

Langues

eng

Sous-ensembles de citation

IM

Pagination

e2103287

Subventions

Organisme : Deutsche Forschungsgemeinschaft (DFG
Organisme : German Research Foundation) under Germany's Excellence Strategy
ID : 2082/1
Organisme : German Research Foundation) under Germany's Excellence Strategy
ID : 390761711
Organisme : Graz University of Technology lead project (LP-03)
Organisme : State of Baden-Württemberg through bwHPC and the German Research Foundation (DFG)
ID : INST 40/575-1 FUGG
Organisme : State of Baden-Württemberg through bwHPC and the German Research Foundation (DFG)
ID : INST 35/1134-1 FUGG
Organisme : Volkswagen Foundation

Informations de copyright

© 2021 The Authors. Advanced Materials published by Wiley-VCH GmbH.

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Auteurs

Alexei Nefedov (A)

Institute of Functional Interfaces (IFG), Karlsruhe Institute of Technology (KIT), Hermann-von-Helmholtz Platz 1, 76344, Eggenstein-Leopoldshafen, Germany.

Ritesh Haldar (R)

Institute of Functional Interfaces (IFG), Karlsruhe Institute of Technology (KIT), Hermann-von-Helmholtz Platz 1, 76344, Eggenstein-Leopoldshafen, Germany.
Tata Institute of Fundamental Research Hyderabad, Gopanpally, Hyderabad, Telangana, 500046, India.

Zhiyun Xu (Z)

Institute of Functional Interfaces (IFG), Karlsruhe Institute of Technology (KIT), Hermann-von-Helmholtz Platz 1, 76344, Eggenstein-Leopoldshafen, Germany.

Hannes Kühner (H)

Institute of Organic Chemistry (IOC), Karlsruhe Institute of Technology (KIT), Fritz-Haber-Weg 6, 76131, Karlsruhe, Germany.

Dennis Hofmann (D)

Physikalisch-Chemisches Institut, Universität Heidelberg, Im Neuenheimer Feld 253, 69120, Heidelberg, Germany.

David Goll (D)

Physikalisch-Chemisches Institut, Universität Heidelberg, Im Neuenheimer Feld 253, 69120, Heidelberg, Germany.

Benedikt Sapotta (B)

Institute of Functional Interfaces (IFG), Karlsruhe Institute of Technology (KIT), Hermann-von-Helmholtz Platz 1, 76344, Eggenstein-Leopoldshafen, Germany.

Stefan Hecht (S)

DWI - Leibniz Institute for Interactive Materials & Institute of Technical and Macromolecular Chemistry, RWTH Aachen University, Forckenbeckstr. 50, 52074, Aachen, Germany.

Marjan Krstić (M)

Institute of Theoretical Solid State Physics (TFP), Karlsruhe Institute of Technology (KIT), Fritz-Wolfgang Gaede Str. 1, 76131, Karlsruhe, Germany.
Institute of Nanotechnology (INT), Karlsruhe Institute of Technology (KIT), Hermann-von-Helmholtz Platz 1, 76344, Eggenstein-Leopoldshafen, Germany.

Carsten Rockstuhl (C)

Institute of Theoretical Solid State Physics (TFP), Karlsruhe Institute of Technology (KIT), Fritz-Wolfgang Gaede Str. 1, 76131, Karlsruhe, Germany.
Institute of Nanotechnology (INT), Karlsruhe Institute of Technology (KIT), Hermann-von-Helmholtz Platz 1, 76344, Eggenstein-Leopoldshafen, Germany.

Wolfgang Wenzel (W)

Institute of Nanotechnology (INT), Karlsruhe Institute of Technology (KIT), Hermann-von-Helmholtz Platz 1, 76344, Eggenstein-Leopoldshafen, Germany.

Stefan Bräse (S)

Institute of Organic Chemistry (IOC), Karlsruhe Institute of Technology (KIT), Fritz-Haber-Weg 6, 76131, Karlsruhe, Germany.
Institute of Biological and Chemical Systems (IBCS-FMS), Karlsruhe Institute of Technology (KIT), Hermann-von-Helmholtz-Platz 1, 76344, Eggenstein-Leopoldshafen, Germany.

Petra Tegeder (P)

Physikalisch-Chemisches Institut, Universität Heidelberg, Im Neuenheimer Feld 253, 69120, Heidelberg, Germany.

Egbert Zojer (E)

Institute of Solid State Physics, Graz University of Technology, NAWI Graz, Petersgasse 16, Graz, 8010, Austria.

Christof Wöll (C)

Institute of Functional Interfaces (IFG), Karlsruhe Institute of Technology (KIT), Hermann-von-Helmholtz Platz 1, 76344, Eggenstein-Leopoldshafen, Germany.

Classifications MeSH