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Project Title:  Dynamics of Complex Colloidal Molecules Reduce
Images: icon  Fiscal Year: FY 2025 
Division: Physical Sciences 
Research Discipline/Element:
Physical Sciences: COMPLEX FLUIDS/SOFT MATTER--Complex Fluids 
Start Date: 10/01/2019  
End Date: 03/31/2023  
Task Last Updated: 04/16/2025 
Download Task Book report in PDF pdf
Principal Investigator/Affiliation:   Marr, David W.M. Ph.D. / Colorado School of Mines 
Address:  Chemical and Biological Engineering 
1500 Illinois Street 
Golden , CO 80401-1887 
Email: dmarr@mines.edu 
Phone: 303-273-3720  
Congressional District:
Web:  
Organization Type: UNIVERSITY 
Organization Name: Colorado School of Mines 
Joint Agency:  
Comments: https://chemeng.mines.edu/project/marr-david/  
Co-Investigator(s)
Affiliation: 
Wu, Ning  Ph.D. Colorado School of Mines 
Project Information: Grant/Contract No. 80NSSC19K1725 
Responsible Center: NASA GRC 
Grant Monitor: McQuillen, John  
Center Contact: 216-433-2876 
john.b.mcquillen@nasa.gov 
Unique ID: 14867 
Solicitation / Funding Source: 2013 Complex Fluids & Macromolecular Biophysics NNH13ZTT001N 
Grant/Contract No.: 80NSSC19K1725 
Project Type: Ground 
Flight Program:  
No. of Post Docs:
No. of PhD Candidates:
No. of Master's Candidates:  
No. of Bachelor's Candidates:  
No. of PhD Degrees:
No. of Master's Degrees:  
No. of Bachelor's Degrees:  
Program--Element: COMPLEX FLUIDS/SOFT MATTER--Complex Fluids 
Task Description: Biopolymers such as polynucleotides and polypeptides are ubiquitous in nature. Although they have relatively simple backbones, by virtue of site-specific interactions between rather limited sets of subunits along the chains, they can fold into proteins and DNA with well-defined three-dimensional (3D) structures of exquisite complexity and functionality. In addition, biopolymers can also assemble into complex structures such as bundled microtubules, flagella, and cilia that undergo nonreciprocal motion in viscous liquid, which drive processes essential for life ranging from nutrient transport to pathogen clearance to cell migration. Scientists and engineers desire a similar capability to produce self-foldable and active functional materials; however, our knowledge of bottom-up assembly is limited by the difficulty in observing and characterizing the in situ processes at sufficiently small length and fast time scales. Unlike atoms and molecules, colloidal sizes can be conveniently tailored so that they are large enough to be probed individually. Colloidal particles are therefore excellent molecular analogues and their self- and directed-assembly has helped us understand fundamental questions in material science including both equilibrium phase behavior and kinetic processes. However, the types of colloidal molecules studied to date have been limited to small sizes, simple symmetries, and rigid structures. We remain far from accessing the full diversity of fundamentally and technologically relevant structures.

Research Impact/Earth Benefits: In-situ manipulation of interactions and dynamic pathways, based on the use of external fields, could lead to crystalline structures beyond those seen in Nature. Our studies move significantly beyond simple hard spheres and towards experimental models appropriate for studying fundamental questions associated with complex symmetries. Results from this study will lead to improved control of non-covalent assembly of molecules, efficient tailoring of lattice symmetries, and the scalable processing of nano-structured materials. The development of new colloidal molecules and their associated assembled structures may have considerable technological impact as well. Anisotropic interactions,. both at the particle level and via applied fields, have been shown generally to lead to arrays with reduced symmetry and enhanced directionality. Such structures interact with a broad range of electromagnetic radiation in unique ways and can. They can exhibit collective photonic, plasmonic, mechanical, electronic, or magnetic properties that are not manifested at the level of single particles. As a result, they have significant potential as next-generation functional materials. For example, dielectric arrays with diamond-like or quasicrystalline lattices have been proposed as ideal photonic crystals that can manipulate light propagation in three dimensions, forming the basis for next-generation all-optical communication technologies. In addition, colloidal networks are common in a range of pharmaceutical and consumer production applications because of their ability to impart a yield stress that can stabilize active components uniformly throughout the formulation. Developing methods to produce colloidal networks with defined coordination, connectivity, and topology would expand the use and performance of colloidal stabilizing networks in these materials.

Here we use a combination of applied external fields to control the assembly of colloidal particles into new structures and building blocks. Specifically, a combination of an in-plane rotating magnetic field and an out-of-plane electric field has yielded quasicrystals, a morphology that cannot be obtained by either of the fields alone. Only recently discovered, quasicrystals have enjoyed significant recent interest because of their unusual formation mechanisms and high rotational symmetry, which may lead to structures with unique physical and photonic properties. In fact, the quasicrystalline structures that have been made possible by this research have not been previously reversibly and spontaneously fabricated at such large length scales.

Task Progress & Bibliography Information FY2025 
Task Progress: Our progress during this period includes:

1. Identifying the magnetic/electric field combinations necessary for the formation of colloidal quasicrystals.

2. Developing characterization methods for quantifying quasicrystalline morphology.

3. Characterizing quasicrystalline formation kinetics.

Bibliography: Description: (Last Updated: 06/13/2025) 

Show Cumulative Bibliography
 
Articles in Peer-reviewed Journals Gao Y, Sprinkle B, Marr DWM, Wu N. "Direct observation of colloidal quasicrystallization." Nat. Phys. 2025 Mar 31:1-8. https://doi.org/10.1038/s41567-025-02859-z , Mar-2025
Articles in Peer-reviewed Journals Yang T, Sprinkle B, Guo Y, Qian J, Hua D, Donev A, Marr DW, Wu N. "Reconfigurable microbots folded from simple colloidal chains." Proc Natl Acad Sci USA. 2020 Aug 4;117(31):18186-93. https://doi.org/10.1073/pnas.2007255117 ; PMID: 32680965; PMCID: PMC7414297 , Aug-2020
Project Title:  Dynamics of Complex Colloidal Molecules Reduce
Images: icon  Fiscal Year: FY 2023 
Division: Physical Sciences 
Research Discipline/Element:
Physical Sciences: COMPLEX FLUIDS/SOFT MATTER--Complex Fluids 
Start Date: 10/01/2019  
End Date: 03/31/2023  
Task Last Updated: 08/06/2022 
Download Task Book report in PDF pdf
Principal Investigator/Affiliation:   Marr, David W.M. Ph.D. / Colorado School of Mines 
Address:  Chemical and Biological Engineering 
1500 Illinois Street 
Golden , CO 80401-1887 
Email: dmarr@mines.edu 
Phone: 303-273-3720  
Congressional District:
Web:  
Organization Type: UNIVERSITY 
Organization Name: Colorado School of Mines 
Joint Agency:  
Comments: https://chemeng.mines.edu/project/marr-david/  
Co-Investigator(s)
Affiliation: 
Wu, Ning  Ph.D. Colorado School of Mines 
Project Information: Grant/Contract No. 80NSSC19K1725 
Responsible Center: NASA GRC 
Grant Monitor: McQuillen, John  
Center Contact: 216-433-2876 
john.b.mcquillen@nasa.gov 
Unique ID: 14867 
Solicitation / Funding Source: 2013 Complex Fluids & Macromolecular Biophysics NNH13ZTT001N 
Grant/Contract No.: 80NSSC19K1725 
Project Type: Ground 
Flight Program:  
No. of Post Docs:
No. of PhD Candidates:  
No. of Master's Candidates:  
No. of Bachelor's Candidates:  
No. of PhD Degrees:  
No. of Master's Degrees:  
No. of Bachelor's Degrees:  
Program--Element: COMPLEX FLUIDS/SOFT MATTER--Complex Fluids 
Task Description: This is a continuation proposal (previous grant "Fabrication, Crystallization, and Folding of Complex Colloidal Molecules under the Influence of Applied External Fields" NNX13AQ54G) for studies developing fluorescent labelling techniques for fabricating colloidal chains with improved imaging on the International Space Station (ISS). In general, this work is based on the use of colloidal particles as molecular analogues for self- and directed assembly investigations with goals toward understanding fundamental questions in material science including both equilibrium phase behavior and kinetic processes. Building on studies by researchers over recent decades, we move here beyond relatively small sizes, simple symmetries, and rigid structures which have prevented accessing the full diversity of fundamentally and technologically relevant structures. Specifically, we will investigate the behavior of colloidal chains that closely resemble natural and synthetic macromolecules with tunable chain length, flexibility, composition, and architecture. First, we will study the folding dynamics of colloidal chains in three dimensions and under microgravity. The experimental measurements will be compared with theories for polymeric molecules and numerical simulations based on fluctuating hydrodynamics. Second, we will perform experiments on the 3D assembly of two-dimensional microwheel-like colloidal clusters induced by depletion interactions.

Research Impact/Earth Benefits: In-situ manipulation of anisotropic interactions and dynamic pathways, based on rational colloidal particle design and proper use of external fields, could lead to crystalline and aperiodic structures beyond those seen in nature.

The development of new colloidal molecules and their associated assembled structures may have considerable technological impact. Anisotropic interactions developed in this proposal, both at the particle level and via applied fields, have been shown generally to lead to arrays with reduced symmetry and enhanced directionality. Such structures interact with a broad range of electromagnetic radiation in unique ways and can exhibit collective photonic, plasmonic, mechanical, electronic, or magnetic properties that are not manifested at the level of single particles. As a result, they have significant potential as next-generation functional materials. For example, dielectric arrays with diamond-like or quasicrystalline lattices have been proposed as ideal photonic crystals that can manipulate light propagation in three dimensions, forming the basis for next-generation all-optical communication technologies. Chiral tetramers studied here could exhibit distinct plasmonic properties resulting from the collective coupling between particles in the pyramid, as confirmed in numerical modeling, which have great potential for electromagnetic metamaterials and high-resolution sensors. The understanding of mirror-symmetry breaking in racemates is also important for developing improved strategies for separation of pharmaceutical molecules. In addition, anisotropic particles can be used to generate new kinds of colloidal networks with well-defined coordination and connectivity. By combining families of tetramers and chains, double networks – two distinct, but interpenetrating, networks of nodes and linkers – could be formed with combined high mechanical stiffness and high toughness. Colloidal networks are very common in a range of pharmaceutical and consumer production applications because of their ability to impart a yield stress that can stabilize active components uniformly throughout the formulation. Developing methods to produce colloidal networks with defined coordination, connectivity, and topology would expand the use and performance of colloidal stabilizing networks in these materials. Ultimately, successful implementation of our proposed research will provide the fundamental knowledge necessary for the development of technologies to design and control matter with tailored structures and properties.

Task Progress & Bibliography Information FY2023 
Task Progress: Our progress during this period includes:

1. Developed model for chain synthesis.

2. Published manuscript on chain synthesis/model. [Ed. Note: See bibliography for reference information.]

3. Began analysis of data obtained on the International Space Station (ISS).

Bibliography: Description: (Last Updated: 06/13/2025) 

Show Cumulative Bibliography
 
Articles in Peer-reviewed Journals Mhanna R, Gao Y, Van Tol I, Springer E, Wu N, Marr DWM. "Chain assembly kinetics from magnetic colloidal spheres." Langmuir 2022 Apr 29;38(18):5730-37. https://doi.org/10.1021/acs.langmuir.2c00343 , Apr-2022
Project Title:  Dynamics of Complex Colloidal Molecules Reduce
Images: icon  Fiscal Year: FY 2020 
Division: Physical Sciences 
Research Discipline/Element:
Physical Sciences: COMPLEX FLUIDS/SOFT MATTER--Complex Fluids 
Start Date: 10/01/2019  
End Date: 03/31/2023  
Task Last Updated: 02/11/2022 
Download Task Book report in PDF pdf
Principal Investigator/Affiliation:   Marr, David W.M. Ph.D. / Colorado School of Mines 
Address:  Chemical and Biological Engineering 
1500 Illinois Street 
Golden , CO 80401-1887 
Email: dmarr@mines.edu 
Phone: 303-273-3720  
Congressional District:
Web:  
Organization Type: UNIVERSITY 
Organization Name: Colorado School of Mines 
Joint Agency:  
Comments: https://chemeng.mines.edu/project/marr-david/  
Co-Investigator(s)
Affiliation: 
Wu, Ning  Ph.D. Colorado School of Mines 
Project Information: Grant/Contract No. 80NSSC19K1725 
Responsible Center: NASA GRC 
Grant Monitor: McQuillen, John  
Center Contact: 216-433-2876 
john.b.mcquillen@nasa.gov 
Unique ID: 14867 
Solicitation / Funding Source: 2013 Complex Fluids & Macromolecular Biophysics NNH13ZTT001N 
Grant/Contract No.: 80NSSC19K1725 
Project Type: Ground 
Flight Program:  
No. of Post Docs:  
No. of PhD Candidates:  
No. of Master's Candidates:  
No. of Bachelor's Candidates:  
No. of PhD Degrees:  
No. of Master's Degrees:  
No. of Bachelor's Degrees:  
Program--Element: COMPLEX FLUIDS/SOFT MATTER--Complex Fluids 
Task Description: This is a continuation proposal (previous grant "Fabrication, Crystallization, and Folding of Complex Colloidal Molecules under the Influence of Applied External Fields" NNX13AQ54G) for studies developing fluorescent labelling techniques for fabricating colloidal chains with improved imaging on the International Space Station (ISS). In general, this work is based on the use of colloidal particles as molecular analogues for self- and directed assembly investigations with goals toward understanding fundamental questions in material science including both equilibrium phase behavior and kinetic processes. Building on studies by researchers over recent decades, we move here beyond relatively small sizes, simple symmetries, and rigid structures which have prevented accessing the full diversity of fundamentally and technologically relevant structures. Specifically, we will investigate the behavior of colloidal chains that closely resemble natural and synthetic macromolecules with tunable chain length, flexibility, composition, and architecture. First, we will study the folding dynamics of colloidal chains in three dimensions and under microgravity. The experimental measurements will be compared with theories for polymeric molecules and numerical simulations based on fluctuating hydrodynamics. Second, we will perform experiments on the 3D assembly of two-dimensional microwheel-like colloidal clusters induced by depletion interactions.

Research Impact/Earth Benefits: In-situ manipulation of anisotropic interactions and dynamic pathways, based on rational colloidal particle design and proper use of external fields, could lead to crystalline and aperiodic structures beyond those seen in nature.

The development of new colloidal molecules and their associated assembled structures may have considerable technological impact. Anisotropic interactions developed in this proposal, both at the particle level and via applied fields, have been shown generally to lead to arrays with reduced symmetry and enhanced directionality. Such structures interact with a broad range of electromagnetic radiation in unique ways and can exhibit collective photonic, plasmonic, mechanical, electronic, or magnetic properties that are not manifested at the level of single particles. As a result, they have significant potential as next-generation functional materials. For example, dielectric arrays with diamond-like or quasicrystalline lattices have been proposed as ideal photonic crystals that can manipulate light propagation in three dimensions, forming the basis for next-generation all-optical communication technologies. Chiral tetramers studied here could exhibit distinct plasmonic properties resulting from the collective coupling between particles in the pyramid, as confirmed in numerical modeling, which have great potential for electromagnetic metamaterials and high-resolution sensors. The understanding of mirror-symmetry breaking in racemates is also important for developing improved strategies for separation of pharmaceutical molecules. In addition, anisotropic particles can be used to generate new kinds of colloidal networks with well-defined coordination and connectivity. By combining families of tetramers and chains, double networks – two distinct, but interpenetrating, networks of nodes and linkers – could be formed with combined high mechanical stiffness and high toughness. Colloidal networks are very common in a range of pharmaceutical and consumer production applications because of their ability to impart a yield stress that can stabilize active components uniformly throughout the formulation. Developing methods to produce colloidal networks with defined coordination, connectivity, and topology would expand the use and performance of colloidal stabilizing networks in these materials. Ultimately, successful implementation of our proposed research will provide the fundamental knowledge necessary for the development of technologies to design and control matter with tailored structures and properties.

Task Progress & Bibliography Information FY2020 
Task Progress: New project for FY2020.

[Note added to Task Book in February 2022 when received information.]

Bibliography: Description: (Last Updated: 06/13/2025) 

Show Cumulative Bibliography
 
 None in FY 2020