Periodic Reporting for period 4 - COMPLEXORDER (The Complexity Revolution: Exploiting Unconventional Order in Next-Generation Materials Design)
Berichtszeitraum: 2023-04-01 bis 2024-09-30
Modern materials chemistry has historically focused on structurally simple, crystalline states. However, a growing body of evidence suggests that materials with structural complexity—especially correlated disorder—can exhibit entirely novel physical behaviours that are inaccessible to ordered systems. The “COMPLEXORDER” project set out to pioneer a new materials design paradigm, rooted in this complexity.
The overarching goal was to understand how chemical composition and synthetic control can be used to engineer disordered states with tailored properties, and how such states can be characterised using emerging techniques such as 3D pair distribution function (3D-PDF) analysis. The project aimed to move beyond the conventional unit cell and uncover design rules for exploiting complexity to generate new types of functionality: from battery materials and dielectric response, to topological phases and structural analogues of quantum phenomena.
By investigating eight tightly interlinked objectives—ranging from Prussian blue analogues and hybrid frameworks to mappings between structural and magnetic order—the project has delivered conceptual advances that challenge existing assumptions about the relationship between structure and function in materials.
The overarching goal was to understand how chemical composition and synthetic control can be used to engineer disordered states with tailored properties, and how such states can be characterised using emerging techniques such as 3D pair distribution function (3D-PDF) analysis. The project aimed to move beyond the conventional unit cell and uncover design rules for exploiting complexity to generate new types of functionality: from battery materials and dielectric response, to topological phases and structural analogues of quantum phenomena.
By investigating eight tightly interlinked objectives—ranging from Prussian blue analogues and hybrid frameworks to mappings between structural and magnetic order—the project has delivered conceptual advances that challenge existing assumptions about the relationship between structure and function in materials.
Over the five-year project period, major advances were made in nearly all targeted areas:
* Chemical control of correlated disorder was established through a landmark study of Prussian blue analogues (Nature, 2020), now considered a foundational paper in the field.
* In framework materials, new insights into multipolar order were gained across several families, leading to general rules for controlling symmetry-breaking processes. These insights were consolidated in highly cited review articles.
* A major unexpected discovery was a new class of disordered metal–organic frameworks (MOFs) whose connectivity reflects Truchet tiling motifs. This work, published in Science and Nature Materials, has reshaped understanding of disorder and its functional consequences.
* Techniques developed in the project—especially mean-field analysis, non-negative matrix factorisation (NMF), and hybrid reverse Monte Carlo (HRMC) methods—have broadened the toolkit for analysing diffuse scattering and are now used in both academia and industry (e.g. for pharmaceutical formulations).
* Structural complexity was shown to play an active role in functionality, including disorder-disorder transitions induced by host–guest interactions (Nature Chemistry, 2021), and hidden-order phases with analogies to long-established statistical mechanics models.
* The project also mapped structural degrees of freedom in layered materials to quaternion chain models, revealing analogues to spin-½ systems—offering a surprising classical lens on quantum phenomena.
Throughout, these findings were disseminated through over 60 publications, including 5 high-impact flagship papers, and have inspired a follow-on ERC Advanced Grant (TRUMAT) focused on chemically encoded complexity.
* Chemical control of correlated disorder was established through a landmark study of Prussian blue analogues (Nature, 2020), now considered a foundational paper in the field.
* In framework materials, new insights into multipolar order were gained across several families, leading to general rules for controlling symmetry-breaking processes. These insights were consolidated in highly cited review articles.
* A major unexpected discovery was a new class of disordered metal–organic frameworks (MOFs) whose connectivity reflects Truchet tiling motifs. This work, published in Science and Nature Materials, has reshaped understanding of disorder and its functional consequences.
* Techniques developed in the project—especially mean-field analysis, non-negative matrix factorisation (NMF), and hybrid reverse Monte Carlo (HRMC) methods—have broadened the toolkit for analysing diffuse scattering and are now used in both academia and industry (e.g. for pharmaceutical formulations).
* Structural complexity was shown to play an active role in functionality, including disorder-disorder transitions induced by host–guest interactions (Nature Chemistry, 2021), and hidden-order phases with analogies to long-established statistical mechanics models.
* The project also mapped structural degrees of freedom in layered materials to quaternion chain models, revealing analogues to spin-½ systems—offering a surprising classical lens on quantum phenomena.
Throughout, these findings were disseminated through over 60 publications, including 5 high-impact flagship papers, and have inspired a follow-on ERC Advanced Grant (TRUMAT) focused on chemically encoded complexity.
This project has significantly extended the frontiers of materials chemistry by:
* Establishing correlated disorder as a design principle, rather than a flaw, in functional materials.
* Developing new computational and experimental methodologies for interpreting complex diffraction data, which are now being adopted internationally.
* Demonstrating that emergent properties—such as hidden order, band gaps, and collective excitations—can arise in structurally disordered systems through carefully tuned interactions.
The unexpected discovery of Truchet-inspired MOFs, along with mappings to models from statistical mechanics and quantum theory, represent conceptual breakthroughs that reframe how disorder is understood and harnessed. The project’s impact is visible not only in its high-profile publications and widespread citations, but also in the opening of new research directions and applications—including in neuromorphic computing, energy storage, and responsive materials.
Looking ahead, ongoing work is building on the project's foundation to exploit complexity in real-world applications, with several high-impact manuscripts in preparation and continuing collaboration with industry and international partners.
* Establishing correlated disorder as a design principle, rather than a flaw, in functional materials.
* Developing new computational and experimental methodologies for interpreting complex diffraction data, which are now being adopted internationally.
* Demonstrating that emergent properties—such as hidden order, band gaps, and collective excitations—can arise in structurally disordered systems through carefully tuned interactions.
The unexpected discovery of Truchet-inspired MOFs, along with mappings to models from statistical mechanics and quantum theory, represent conceptual breakthroughs that reframe how disorder is understood and harnessed. The project’s impact is visible not only in its high-profile publications and widespread citations, but also in the opening of new research directions and applications—including in neuromorphic computing, energy storage, and responsive materials.
Looking ahead, ongoing work is building on the project's foundation to exploit complexity in real-world applications, with several high-impact manuscripts in preparation and continuing collaboration with industry and international partners.