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Molecular Motors, powering dynamic functional molecular systems

Periodic Reporting for period 4 - MMDYNASYS (Molecular Motors, powering dynamic functional molecular systems)

Période du rapport: 2021-03-01 au 2021-08-31

The MMDYNASYS project is focused on building molecular unidirectional light, redox and catalytically driven molecular motors into complex molecular systems to generate dynamic control over the behaviour of materials and systems. This includes both fundamental research into the working of artificial molecular machines, as well as application-based research. Once their unidirectional motion can be harnessed as work, molecular motors may be applied to drive the nanomachinery of the future, much like a macro-sized motors drives machines ranging from cars to factory assemblers.
The overall objectives of the project are to gain more fundamental insight into rotary molecular motors, to push the boundaries of nanotechnology, and to demonstrate the potential of these machines to function in new research areas such as biologically relevant media, the solid state and LCs.
Molecular motor research is at a fundamental stage. However, future applications to the benefit of society may include biomedical applications, information storage and smart materials.
The project has been highly successful. The research group has taken considerable steps in rotary molecular motor research. Conclusions reached by the action include a deeper fundamental understanding of directed motion at the molecular scale, the development of several new types of molecular motors, unidirectional motion in the solid state, amplification of motion to the macroscale, and a molecular motor pushing a chemical system out of equilibrium.
The aim of WP1 (catalytic and redox driven rotary motion) was to expand the opportunities for application of synthetic molecular motors in molecular based devices by designing novel systems driven by fuel other than the traditional combination of heat and (potentially harmful) UV light. During the action, we have developed novel rotary systems based on, for example, a palladium redox cycle, and visible/NIR light.
The goal of WP2 (amplification in liquid crystals through cooperative motor function) was the amplification of photo-induced dynamic changes over various length scales. The approach was diversified into the use of Metal Organic Frameworks (MOFs), which allowed to us to demonstrate (for the very first time) unidirectional motor rotation in the solid state.
The goal of WP3 (far-from-equilibrium self-assembly in water) was to design building blocks with intrinsic molecular motor/photoswitch function, study self-assembly and explore responsive behavior. Ultimately, the aim of this approach was to investigate systems far from equilibrium. This work-package was the most successful out of all WPs, leading to several publications in top-tier journals. Highlights include a macro-sized ‘molecular muscle’ and a light-fueled ratchet capable of driving a coupled chemical equilibrium uphill.
The focus of the last WP (dynamic control over biomolecular function) was achieving control over complex functions in aqueous environments using light. We made significant advances towards this goal with the development of several light controlled biohybrid systems. The potential of molecular machines as useful tools in biomolecular research was further demonstrated by a system where stem cell fate could be controlled by surface assembled molecular motors.

All of the results mentioned above have been published in peer reviewed journals. In addition, our research has attracted the attention of the popular science press, and highlights about this work appear regularly in non-scientific media.
Project MMDYNASYS has significantly pushed the boundaries of the potential of molecular machines. Highlights include: molecular motors functioning in water and controlling function of biomolecules, the first catalytic rotary molecular motor, demonstration of motor rotation in the solid state, a whole array of new ultrafast molecular motors operated by visible light, an artificial molecular muscle capable of lifting a macro-sized load, a light-fueled ratchet capable of driving a coupled chemical equilibrium uphill and the determination of stem cell fate by molecular motor rotation.
Several of our developments constitute major breakthroughs. Our development of novel methodology to access P-chirogenic compounds (Nature Catalysis 2021) presents significant advantages over currently used synthetic methods and is sure to find application in, among others, agrochemistry and materials science. Our new light driven molecular ratchet (Nature Nanotechnology 2022) constitutes a landmark for light-driven molecular machines, as by coupling the unidirectional motion to a chemical equilibrium, we manage to convert the work performed by the motor to chemical energy, and thus can fuel a secondary process by unidirectional rotation. This is an essential step towards harnesses the power of molecular machines, and building sophisticated nanomachinery and molecular factories. For macro-sized applications, cooperative and/or collective functioning of machines will be required, as well as an orientation that limits the degrees of freedom. Our publications on switchable porous frameworks (Nature Chemistry 2020) and a molecular muscle (Nature Chemistry 2018) represent the two approaches towards this goal. In the first, it is demonstrated that molecular motors can be oriented in a highly regular fashion within large 3D solid material assemblies while still properly functioning. In the second, a supramolecular approach was highly successful to amplify motion from nanoscale to macroscale dimensions. Finally, suing nanomechanical force of surface bound motors to control stem cell behavior (Science Advances 2020) is unique and opens major opportunities at the biointerface.
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