Multiscale Theory for Designing Hierarchical Organic Materials formed by Self-assembly

We explored new hierarchical assemblies of molecules as 2D and 3D crystalline materials. Using an integrated approach that unites synthesis, characterization and simulation together, we showed how molecule-scale dynamics impacts large-scale assembly of molecules at interfaces. We learned how macrocycle assembly depends on rigidity, cooperativity, sidechains, monomer sequence, dynamics, processing, ions and stacking.

We also created a totally new class of fluorescent materials that are the brightest reported. They are called small-molecule ionic-isolation lattices (SMILES). The simplicity, generality, and superior properties of SMILES enables a new platform for programming optical properties seamlessly from molecules to materials.

Publications

Breaking Radial Dipole Symmetry in Planar Macrocycles Modulates Edge‐to‐Edge Packing and Disrupts Cofacial Stacking

Y. Li, H. D. Castillo, J. R. Dobscha, A. R. Morgan, S. L. Tait, and A. H. Flood

12/19/2023

Ultrabright Fluorescent Organic Nanoparticles Based on Small‐Molecule Ionic Isolation Lattices**

J. Chen, S. M. A. Fateminia, L. Kacenauskaite, N. Bærentsen, S. Grønfeldt Stenspil, J. Bredehoeft, K. L. Martinez, A. H. Flood, and B. W. Laursen

3/11/2021

Plug-and-Play Optical Materials from Fluorescent Dyes and Macrocycles

C. R. Benson, L. Kacenauskaite, K. L. VanDenburgh, W. Zhao, B. Qiao, T. Sadhukhan, M. Pink, J. Chen, S. Borgi, C. Chen, B. J. Davis, Y. C. Simon, K. Raghavachari, B. W. Laursen, and A. H. Flood

8/1/2020

Solution-Mediated Annealing Pathways Are Critical for Supramolecular Ordering of Complex Macrocycles at Surfaces

H. D. Castillo, J. Yang, S. Debnath, J. R. Dobscha, C. Q. Trainor, R. D. Mortensen, K. Raghavachari, A. H. Flood, P. J. Ortoleva, and S. L. Tait

3/2/2020

Temporally Coarse-Grained All-Atom Molecular Dynamics Achieved via Stochastic Padé Approximants

Y. V. Sereda, and P. J. Ortoleva

1/20/2020

Sequence-Defined Macrocycles for Understanding and Controlling the Build-up of Hierarchical Order in Self-Assembled 2D Arrays

J. R. Dobscha, H. D. Castillo, Y. Li, R. E. Fadler, R. D. Taylor, A. A. Brown, C. Q. Trainor, S. L. Tait, and A. H. Flood

9/10/2019

Understanding the Origin of 2D Self-Assembly of Tricarbazole Macrocycles: An Integrated Quantum Mechanical/Molecular Dynamics Study

S. Debnath, J. Yang, P. Ortoleva, and K. Raghavachari

7/8/2019

Surface Self-Assembly, Film Morphology, and Charge Transport Properties of Semiconducting Triazoloarenes

D. L. Wisman, S. Kim, T. W. Morris, J. Choi, C. D. Tempas, C. Q. Trainor, D. Lee, and S. L. Tait

4/12/2019

Supramolecular Assemblies on Surfaces: Nanopatterning, Functionality, and Reactivity

D. P. Goronzy, M. Ebrahimi, F. Rosei, Y. Fang, S. De Feyter, S. L. Tait, C. Wang, P. H. Beton, A. T. S. Wee, P. S. Weiss, and D. F. Perepichka

6/22/2018

Host–Host Interactions Control Self‐assembly and Switching of Triple and Double Decker Stacks of Tricarbazole Macrocycles Co‐assembled with anti‐Electrostatic Bisulfate Dimers

J. R. Dobscha, S. Debnath, R. E. Fadler, E. M. Fatila, M. Pink, K. Raghavachari, and A. H. Flood

6/19/2018

Programmed Negative Allostery with Guest-Selected Rotamers Control Anion–Anion Complexes of Stackable Macrocycles

E. G. Sheetz, B. Qiao, M. Pink, and A. H. Flood

6/9/2018

From Foldable Open Chains to Shape-Persistent Macrocycles: Synthesis, Impact on 2D Ordering, and Stimulated Self-Assembly

S. Kim, H. D. Castillo, M. Lee, R. D. Mortensen, S. L. Tait, and D. Lee

3/13/2018

Multiscale Molecular Dynamics Approach to Energy Transfer in Nanomaterials

J. M. Espinosa-Duran, Y. V. Sereda, A. Abi-Mansour, and P. Ortoleva

2/2/2018

Amphiphile self-assembly dynamics at the solution-solid interface reveal asymmetry in head/tail desorption

H. D. Castillo, J. M. Espinosa-Duran, J. R. Dobscha, D. C. Ashley, S. Debnath, B. E. Hirsch, S. R. Schrecke, M. Baik, P. J. Ortoleva, K. Raghavachari, A. H. Flood, and S. L. Tait

1/1/2018

Multiscale time-dependent density functional theory: Demonstration for plasmons

J. Jiang, A. Abi Mansour, and P. J. Ortoleva

8/1/2017

Ion-Pair Oligomerization of Chromogenic Triangulenium Cations with Cyanostar-Modified Anions That Controls Emission in Hierarchical Materials

B. Qiao, B. E. Hirsch, S. Lee, M. Pink, C. Chen, B. W. Laursen, and A. H. Flood

4/24/2017

Complex molecular surfaces and interfaces: concluding remarks

D. B. Amabilino, and S. Tait

1/1/2017

Ionic manipulation of charge-transfer and photodynamics of [60]fullerene confined in pyrrolo-tetrathiafulvalene cage

S. Bähring, K. R. Larsen, M. Supur, K. A. Nielsen, T. Poulsen, K. Ohkubo, C. W. Marlatt, E. Miyazaki, K. Takimiya, A. H. Flood, S. Fukuzumi, and J. O. Jeppesen

1/1/2017

Physical and chemical model of ion stability and movement within the dynamic and voltage-gated STM tip–surface tunneling junction

B. E. Hirsch, K. P. McDonald, S. L. Tait, and A. H. Flood

1/1/2017

Reverse Coarse-Graining for Equation-Free Modeling: Application to Multiscale Molecular Dynamics

A. Abi Mansour, and P. J. Ortoleva

10/24/2016

ProtoMD: A prototyping toolkit for multiscale molecular dynamics

E. Somogyi, A. A. Mansour, and P. J. Ortoleva

5/1/2016

Creating molecular macrocycles for anion recognition

A. H. Flood