Local Self‐Assembly of Dissipative Structures Sustained by Substrate Diffusion DOI Creative Commons
Haridas Kar,

Lorenzo Goldin,

Diego Frezzato

и другие.

Angewandte Chemie, Год журнала: 2024, Номер 136(30)

Опубликована: Май 8, 2024

Abstract The coupling between energy‐consuming molecular processes and the macroscopic dimension plays an important role in nature development of active matter. Here, we study temporal evolution a system upon local activation dissipative self‐assembly process. Injection surfactant molecules substrate‐containing hydrogel results substrate‐templated formation assemblies, which are catalysts for conversion substrate into waste. We show that develops (pseudo‐)non‐equilibrium steady state (NESS) characterized by presence energy‐dissipating assemblies persistent waste concentration gradients. For elevated concentrations, this can be maintained more than 4 days. studies reveal interdependence gradients: catalytic activity sustained gradients and, vice versa, continuous diffusion to stabilizes their size. possibility activate with spatial control create long lasting non‐equilibrium states enables structures studied space‐time domain, is relevance understanding biological systems

Язык: Английский

Molecular Ratchets and Kinetic Asymmetry: Giving Chemistry Direction DOI Creative Commons
Stefan Borsley, David A. Leigh, Benjamin M. W. Roberts

и другие.

Angewandte Chemie International Edition, Год журнала: 2024, Номер 63(23)

Опубликована: Апрель 3, 2024

Abstract Over the last two decades ratchet mechanisms have transformed understanding and design of stochastic molecular systems—biological, chemical physical—in a move away from mechanical macroscopic analogies that dominated thinking regarding dynamics in 1990s early 2000s (e.g. pistons, springs, etc), to more scale‐relevant concepts underpin out‐of‐equilibrium research sciences today. Ratcheting has established nanotechnology as frontier for energy transduction metabolism, enabled reverse engineering biomolecular machinery, delivering insights into how molecules ‘walk’ track‐based synthesisers operate, acceleration reactions enables be transduced by catalysts (both motor proteins synthetic catalysts), dynamic systems can driven equilibrium through catalysis. The recognition biology, their invention systems, is proving significant areas diverse supramolecular chemistry, covalent DNA nanotechnology, polymer materials science, heterogeneous catalysis, endergonic synthesis, origin life, many other branches science. Put simply, give chemistry direction. Kinetic asymmetry, key feature ratcheting, counterpart structural asymmetry (i.e. chirality). Given ubiquity processes significance behaviour function it surely just fundamentally important. This Review charts recognition, development ratchets, focussing particularly on role which they were originally envisaged elements machinery. Different kinetically asymmetric are compared, consequences discussed. These archetypal examples demonstrate inexorably equilibrium, rather than relax towards it.

Язык: Английский

Процитировано

35

Local Self‐Assembly of Dissipative Structures Sustained by Substrate Diffusion DOI Creative Commons
Haridas Kar,

Lorenzo Goldin,

Diego Frezzato

и другие.

Angewandte Chemie International Edition, Год журнала: 2024, Номер 63(30)

Опубликована: Май 8, 2024

Abstract The coupling between energy‐consuming molecular processes and the macroscopic dimension plays an important role in nature development of active matter. Here, we study temporal evolution a system upon local activation dissipative self‐assembly process. Injection surfactant molecules substrate‐containing hydrogel results substrate‐templated formation assemblies, which are catalysts for conversion substrate into waste. We show that develops (pseudo‐)non‐equilibrium steady state (NESS) characterized by presence energy‐dissipating assemblies persistent waste concentration gradients. For elevated concentrations, this can be maintained more than 4 days. studies reveal interdependence gradients: catalytic activity sustained gradients and, vice versa, continuous diffusion to stabilizes their size. possibility activate with spatial control create long lasting non‐equilibrium states enables structures studied space‐time domain, is relevance understanding biological systems

Язык: Английский

Процитировано

2

Molecular Ratchets and Kinetic Asymmetry: Giving Chemistry Direction DOI Creative Commons
Stefan Borsley, David A. Leigh, Benjamin M. W. Roberts

и другие.

Angewandte Chemie, Год журнала: 2024, Номер 136(23)

Опубликована: Апрель 3, 2024

Abstract Over the last two decades ratchet mechanisms have transformed understanding and design of stochastic molecular systems—biological, chemical physical—in a move away from mechanical macroscopic analogies that dominated thinking regarding dynamics in 1990s early 2000s (e.g. pistons, springs, etc), to more scale‐relevant concepts underpin out‐of‐equilibrium research sciences today. Ratcheting has established nanotechnology as frontier for energy transduction metabolism, enabled reverse engineering biomolecular machinery, delivering insights into how molecules ‘walk’ track‐based synthesisers operate, acceleration reactions enables be transduced by catalysts (both motor proteins synthetic catalysts), dynamic systems can driven equilibrium through catalysis. The recognition biology, their invention systems, is proving significant areas diverse supramolecular chemistry, covalent DNA nanotechnology, polymer materials science, heterogeneous catalysis, endergonic synthesis, origin life, many other branches science. Put simply, give chemistry direction. Kinetic asymmetry, key feature ratcheting, counterpart structural asymmetry (i.e. chirality). Given ubiquity processes significance behaviour function it surely just fundamentally important. This Review charts recognition, development ratchets, focussing particularly on role which they were originally envisaged elements machinery. Different kinetically asymmetric are compared, consequences discussed. These archetypal examples demonstrate inexorably equilibrium, rather than relax towards it.

Язык: Английский

Процитировано

0

Local Self‐Assembly of Dissipative Structures Sustained by Substrate Diffusion DOI Creative Commons
Haridas Kar,

Lorenzo Goldin,

Diego Frezzato

и другие.

Angewandte Chemie, Год журнала: 2024, Номер 136(30)

Опубликована: Май 8, 2024

Abstract The coupling between energy‐consuming molecular processes and the macroscopic dimension plays an important role in nature development of active matter. Here, we study temporal evolution a system upon local activation dissipative self‐assembly process. Injection surfactant molecules substrate‐containing hydrogel results substrate‐templated formation assemblies, which are catalysts for conversion substrate into waste. We show that develops (pseudo‐)non‐equilibrium steady state (NESS) characterized by presence energy‐dissipating assemblies persistent waste concentration gradients. For elevated concentrations, this can be maintained more than 4 days. studies reveal interdependence gradients: catalytic activity sustained gradients and, vice versa, continuous diffusion to stabilizes their size. possibility activate with spatial control create long lasting non‐equilibrium states enables structures studied space‐time domain, is relevance understanding biological systems

Язык: Английский

Процитировано

0