0000000001302430
AUTHOR
Aron Walsh
showing 11 related works from this author
Breathing-Dependent Redox Activity in a Tetrathiafulvalene-Based Metal–Organic Framework
2018
"Breathing" metal-organic frameworks (MOFs) that involve changes in their structural and physical properties upon an external stimulus are an interesting class of crystalline materials due to their range of potential applications including chemical sensors. The addition of redox activity opens up a new pathway for multifunctional "breathing" frameworks. Herein, we report the continuous breathing behavior of a tetrathiafulvalene (TTF)-based MOF, namely MUV-2, showing a reversible swelling (up to ca. 40% of the volume cell) upon solvent adsorption. Importantly, the planarity of the TTF linkers is influenced by the breathing behavior of the MOF, directly impacting on its electrochemical proper…
Investigation of Charge-Transfer Interactions Induced by Encapsulating Fullerene in a Mesoporous Tetrathiafulvalene-Based Metal-Organic Framework
2019
<p>The design of Metal-Organic Frameworks (MOFs) incorporating electroactive guest molecules in the pores has become a subject of great interest in order to install additional electrical functionalities within the framework while maintaining porosity. In this direction, understanding the charge-transfer (CT) process between the framework and the guest molecules is crucial towards the design of new electroactive MOFs. Herein, we present the encapsulation of fullerenes (C<sub>60</sub>) in a mesoporous tetrathiafulvalene(TTF)-based MOF. The CT process between the electron-acceptor C<sub>60 </sub>guest and the electron-donor TTF ligand is studied in detail by means…
Bandgap lowering in mixed alloys of Cs2Ag(SbxBi1−x)Br6 double perovskite thin films
2020
Halide double perovskites have gained significant attention, owing to their composition of low-toxicity elements, stability in air and long charge-carrier lifetimes. However, most double perovskites, including Cs2AgBiBr6, have wide bandgaps, which limit photo conversion efficiencies. The bandgap can be reduced through hallowing with Sb3+, but Sb-rich alloys are difficult to synthesise due to the high formation energy of Cs2AgSbBr6, which itself has a wide bandgap. We develop a solution-based route to synthesis phase-pure Cs2Ag(SbxBi1-x)Br6 thin films, with the mixing parameter x continuous varying over the entire composition range. We reveal that the mixed alloys (x between 0.5 and 0.9) dem…
Ligand engineering in Cu(ii) paddle wheel metal–organic frameworks for enhanced semiconductivity
2020
We report the electronic structure of two metal-organic frameworks (MOFs) with copper paddle wheel nodes connected by a N2(C2H4)3 (DABCO) ligand with accessible nitrogen lone pairs. The coordination is predicted, from first-principles density functional theory, to enable electronic pathways that could facilitate charge carrier mobility. Calculated frontier crystal orbitals indicate extended electronic communication in DMOF-1, but not in MOF-649. This feature is confirmed by bandstructure calculations and effective masses of the valence band egde. We explain the origin of the frontier orbitals of both MOFs based on the energy and symmetry alignment of the underlying building blocks. The effe…
Strong absorption and ultrafast localisation in NaBiS2 nanocrystals with slow charge-carrier recombination.
2022
Funder: AiF Project, no: ZIM-KK5085302DF0
Charge-transfer interactions between fullerenes and a mesoporous tetrathiafulvalene-based metal–organic framework
2019
The design of metal–organic frameworks (MOFs) incorporating electroactive guest molecules in the pores has become a subject of great interest in order to obtain additional electrical functionalities within the framework while maintaining porosity. Understanding the charge-transfer (CT) process between the framework and the guest molecules is a crucial step towards the design of new electroactive MOFs. Herein, we present the encapsulation of fullerenes (C60) in a mesoporous tetrathiafulvalene (TTF)-based MOF. The CT process between the electron-acceptor C60 guest and the electron-donor TTF ligand is studied in detail by means of different spectroscopic techniques and density functional theor…
Bandgap lowering in mixed alloys of Cs2Ag(SbxBi1−x)Br6 double perovskite thin films
2020
Halide double perovskites have gained significant attention, owing to their composition of low-toxicity elements, stability in air and long charge-carrier lifetimes. However, most double perovskites, including Cs2AgBiBr6, have wide bandgaps, which limits photoconversion efficiencies. The bandgap can be reduced through alloying with Sb3+, but Sb-rich alloys are difficult to synthesize due to the high formation energy of Cs2AgSbBr6, which itself has a wide bandgap. We develop a solution-based route to synthesize phase-pure Cs2Ag(SbxBi1−x)Br6 thin films, with the mixing parameter x continuously varying over the entire composition range. We reveal that the mixed alloys (x between 0.5 and 0.9) d…
CCDC 1830490: Experimental Crystal Structure Determination
2018
Related Article: Manuel Souto, Jorge Romero, Joaquín Calbo, Inigo J. Vitorica-Yrezabal, Jose L Zafra, Juan Casado Cordón, Enrique Ortí, Aron Walsh, Guillermo Minguez Espallargas|2018|J.Am.Chem.Soc.|140|10562|doi:10.1021/jacs.8b05890
CCDC 1830488: Experimental Crystal Structure Determination
2018
Related Article: Manuel Souto, Jorge Romero, Joaquín Calbo, Inigo J. Vitorica-Yrezabal, Jose L Zafra, Juan Casado Cordón, Enrique Ortí, Aron Walsh, Guillermo Minguez Espallargas|2018|J.Am.Chem.Soc.|140|10562|doi:10.1021/jacs.8b05890
CCDC 1830489: Experimental Crystal Structure Determination
2018
Related Article: Manuel Souto, Jorge Romero, Joaquín Calbo, Inigo J. Vitorica-Yrezabal, Jose L Zafra, Juan Casado Cordón, Enrique Ortí, Aron Walsh, Guillermo Minguez Espallargas|2018|J.Am.Chem.Soc.|140|10562|doi:10.1021/jacs.8b05890
CCDC 1853491: Experimental Crystal Structure Determination
2018
Related Article: Manuel Souto, Jorge Romero, Joaquín Calbo, Inigo J. Vitorica-Yrezabal, Jose L Zafra, Juan Casado Cordón, Enrique Ortí, Aron Walsh, Guillermo Minguez Espallargas|2018|J.Am.Chem.Soc.|140|10562|doi:10.1021/jacs.8b05890