Center for Molecular Modeling - FWO K. Lejaeghere FWO3E02016002101

Thermal unequilibrium of strained black CsPbI3 thin films

sven — Thu, 25 Jul 2019 18:07:18 +0000

J.A. Steele, H. Jin, I. Dovgaliuk, R.F. Berger, T. Braeckevelt, H. Yuan, C. Martin, E. Solano, K. Lejaeghere, S.M.J. Rogge, C. Notebaert, W. Vandezande, K.P.F. Janssen, B. Goderis, E. Debroye, Y.-K. Wang, Y. Dong, D. Ma, M. Saidaminov, H. Tan, Z. Lu, V. Dyadkin, D. Chernyshov, V. Van Speybroeck, E.H. Sargent, J. Hofkens, M. Roeffaers

Science

365 (6454), 679-684

2019

Abstract

The high-temperature all-inorganic CsPbI₃ perovskite black phase is metastable relative to its yellow non-perovskite phase, at room temperature. Since only the black phase is optically active, this represents an impediment for the use of CsPbI₃ in optoelectronic devices. We report the use of substrate clamping and biaxial strain to render stable, at room temperature, black phase CsPbI₃ thin films. We used synchrotron-based grazing incidence wide angle x-ray scattering to track the introduction of crystal distortions and strain-driven texture formation within black CsPbI₃ thin films when they were cooled following annealing at 330°C. The thermal stability of black CsPbI₃ thin films is vastly improved by the strained interface, a response verified by ab initio thermodynamic modelling.

Open Access version available at UGent repository

Gold Open Access

DOI

http://dx.doi.org/10.1126/science.aax3878

Private attachment

science.aax3878.full_.pdf

Electronic properties of heterogenized Ru(II) polypyridyl photoredox complexes on covalent triazine frameworks

kurt — Wed, 13 Mar 2019 07:02:04 +0000

A. De Vos, K. Lejaeghere, F. Muniz-Miranda, C. Stevens, P. Van der Voort, V. Van Speybroeck

Journal of Materials Chemistry A

7, 8433-8442

2019

Abstract

Ru(II) polypyridyl complexes have been successful for a wide range of photoredox applications thanks to their efficient light-induced metal-to-ligand charge transfer. Using the computational framework of density-functional theory, we report how these complexes can be anchored onto covalent triazine frameworks while maintaining their favorable electronic properties. We moreover show that variation of the nitrogen content of the framework linkers or complex ligands endows the heterogenized catalyst with a unique versatility, spanning a wide range of absorption characteristics and redox potentials. By judiciously choosing the catalyst building blocks, it is even possible to selectively guide the charge transfer toward either the scaffold or the accessible pore sites. Rational design of sustainable and efficient photocatalysts thus comes within reach.

DOI

http://dx.doi.org/10.1039/C9TA00573K

Private attachment

C9TA00573K.pdf

A first-principles reassessment of the Fe-N phase diagram in the low-nitrogen limit

kurt — Fri, 28 Sep 2018 08:44:28 +0000

S. De Waele, K. Lejaeghere, E. Leunis, L. Duprez, S. Cottenier

Journal of Alloys and Compounds

775, 758-768

2019

DOI

http://dx.doi.org/10.1016/j.jallcom.2018.09.356

Exploring lanthanide doping in UiO-66: a combined experimental and computational study of the electronic structure

kurt — Fri, 23 Feb 2018 19:50:21 +0000

K. Hendrickx, J.J. Joos, A. De Vos, D. Poelman, P. F. Smet, V. Van Speybroeck, P. Van der Voort, K. Lejaeghere

Inorganic Chemistry

57, 5463-5474

2018

DOI

http://dx.doi.org/10.1021/acs.inorgchem.8b00425

Private attachment

Hendrickx_2018_InorgChem_lanthanide-UiO-electronic.pdf

Manuscript.pdf

Tuning the balance between dispersion and entropy to design temperature-responsive flexible metal-organic frameworks

kurt — Fri, 23 Feb 2018 19:44:00 +0000

J. Wieme, K. Lejaeghere, G. Kresse, V. Van Speybroeck

Nature Communications

9, 4899

2018

DOI

http://dx.doi.org/10.1038/s41467-018-07298-4

Private attachment

Wieme_2018_NatureCommun_dispersion-vs-entropy-MIL53.pdf

Missing linkers: an alternative pathway to UiO-66 electronic structure engineering

kurt — Sun, 05 Feb 2017 10:38:54 +0000

A. De Vos, K. Hendrickx, P. Van der Voort, V. Van Speybroeck, K. Lejaeghere

Chemistry of Materials

29 (7), 3006–3019

2017

Abstract

UiO-66 is a promising metal-organic framework for photocatalytic applications. However, the ligand-to-metal charge transfer of an excited electron is inefficient in the pristine material. Herein we assess the influence of missing linker defects on the electronic structure of UiO-66 and discuss their ability to improve ligand-to-metal charge transfer. Using a new defect classification system, which is transparent and easily extendable, we identify the most promising photocatalysts by considering both relative stability and electronic structure. We find the properties of UiO-66 defect structures largely to depend on the coordination of the constituent nodes, and the nodes with the strongest local distortions to alter the electronic structure most. Defects hence provide an alternative pathway to tune UiO-66 for photocatalytic purposes, besides linker modification and node metal substitution. In addition, the decomposition of MOF properties into node- and linker-based behavior is more generally valid, so we propose orthogonal electronic structure tuning as a paradigm in MOF electronic structure engineering.

Open Access version available at UGent repository

Gold Open Access

DOI

http://dx.doi.org/10.1021/acs.chemmater.6b05444

Private attachment

acs%2Echemmater%2E6b05444(1).pdf

Dr. Kurt Lejaeghere nominated for EOS Pipet 2016

wim — Thu, 20 Oct 2016 08:01:21 +0000

Dr. Kurt Lejaeghere is nominated for the EOS Pipet 2016 award, an initiative of EOS Science Magazine, highlighting the most promising young scientists of the year. The nomination follows Kurt's paper in Science, entitled 'Reproducibility in density functional theory calculations of solids'.

Vote

Please cast your vote for Kurt on http://eoswetenschap.eu/content/wie-jouw-favoriete-beloftevolle-wetensch...

EUROMAT 2017

sven — Mon, 17 Jul 2017 15:45:23 +0000

Thessaloníki, Greece

Sunday, 17 September, 2017 to Friday, 22 September, 2017

Participant(s)

A. De Vos, J. Wieme, S. De Waele, S.M.J. Rogge, J. Hajek, L. Vanduyfhuys, K. Lejaeghere, A. Ghysels, V. Van Speybroeck

Project ref.

FWO S. Rogge FWO3F02014004601, FWO A. De Vos FWO3F02016005101, FWO J. Wieme FWO3F02015006001, FWO K. Lejaeghere FWO3E02016002101, ERC DYNPOR H20ERC2015000301

Conference reference

EUROMAT 2017

ABIDEV 2017 – 8th ABINIT Developer’s Workshop

wim — Mon, 08 May 2017 06:30:42 +0000

Fréjus, France

Monday, 8 May, 2017 to Friday, 12 May, 2017

Participant(s)

K. Lejaeghere

Project ref.

FWO K. Lejaeghere FWO3E02016002101

Conference reference

ABIDEV 2017 – 8th ABINIT Developer’s Workshop

EMN Conference

wim — Wed, 12 Apr 2017 11:19:22 +0000

Las Vegas, USA

Monday, 10 October, 2016 to Friday, 14 October, 2016

Participant(s)

K. Lejaeghere

Project ref.

FWO K. Lejaeghere FWO3E02016002101

Conference reference

EMN Conference