/css21
This talk!
Jason Cantarella
U. of Georgia
Tetsuo Deguchi
Ochanomizu U.
Erica Uehara
Ochanomizu U.
Funding: Simons Foundation
A linear polymer is a chain of molecular units with free ends.
Polyethylene
Nicole Gordine [CC BY 3.0] from Wikimedia Commons
In solution, linear polymers become crumpled:
Protonated P2VP
Roiter–Minko, J. Am. Chem. Soc. 127 (2005), 15688-15689
[CC BY-SA 3.0], from Wikimedia Commons
A topological polymer joins monomers in some graph type:
Petersen graph
The Tezuka lab in Tokyo can now synthesize many topological polymers in usable quantities
Y. Tezuka, Acc. Chem. Res. 50 (2017), 2661–2672
What is the probability distribution on the shapes of topological polymers in solution?
Linear polymers
Topological polymers
Random walks with independent steps
Random walks with steps conditioned on ???
Suppose \(\mathcal{G}\) is a directed graph with \(\mathbf{v}\) vertices and \(\mathbf{e}\) edges.
\(L:\mathbb{R}^{\mathbf{v}}\to \mathbb{R}^{\mathbf{v}}\) given by \(L = \partial \partial^T\) is the graph Laplacian.
Think of \(x=(x_1,\dots,x_{\mathbf{v}})\in \mathbb{R}^{\mathbf{v}}\) as a realization of \(\mathcal{G}\) in \(\mathbb{R}\).
Harmonic bonds \(\Rightarrow\) Gaussian vertex distribution:
This is James–Guth–Flory phantom network theory!
Define \(\widetilde{L}:=L+\frac{1}{\mathbf{v}} \mathbf{1}\mathbf{1}^T\).
Proposition.
\(\mu_{\mathcal{G}}\): \(O(d)\)-invariant measure concentrated on \(\operatorname{im}\partial^* \subset \operatorname{ED}\)
\(\nu_{\mathcal{G}}=(\partial^{*+})_\sharp \mu_{\mathcal{G}}\), its pushforward to \(\operatorname{VP}\).
\(\Sigma_{\mathbf{v}}:=\) matrix of expectations of products of a fixed coordinate of the vertices of \(\mathcal{G}\)
\(\Sigma_{\mathbf{e}}\) likewise for edges.
Theorem. The expected radius of gyration is
\(\langle \operatorname{R}_g^2\rangle_{\nu_{\mathcal{G}}} = \frac{d}{\mathbf{v}}\operatorname{tr}(\Sigma_{\mathbf{v}}) = \frac{d}{\mathbf{v}} \operatorname{tr}(\partial^{T+}\Sigma_{\mathbf{e}}\partial^+)\)
When \(\mu_{\mathcal{G}}\) is a standard Gaussian on \(\operatorname{im}\partial^*\),
\(\langle\operatorname{R}_g^2\rangle_{\nu_{\mathcal{G}}}= \frac{d}{\mathbf{v}}\operatorname{tr}\partial^{T+}(\partial^T\partial^{T+})\partial^T = \frac{d}{\mathbf{v}} \operatorname{tr} \partial^{T+}\partial^T = \frac{d}{\mathbf{v}} \operatorname{tr}L^+\).
Theorem. Suppose \(f_0\) and \(f_1\) are injective chain maps between graphs \(\mathcal{G}'\) and \(\mathcal{G}\) of the same cycle rank. Given \(O(d)\)- and translation-invariant \(g:\operatorname{VP} \to \mathbb{R}\) which is expressible in terms of \(\mathcal{G}'\), then
\(\mathcal{E}_{\nu_{\mathcal{G}}}(g) = \mathcal{E}_{\nu'_{\mathcal{G}'}}(g')\).
\(\mathcal{G}\)
\(\mathcal{G}_n\)
Proposition. In phantom network theory, the joint distribution of squared distances between junction vertices in \(\mathcal{G}_n\) is the joint distribution of \(n\) times the squared distances between vertices in \(\mathcal{G}\).
In the freely-jointed chain, each edge is a unit vector.
\(\langle \operatorname{squared\, junction-junction\, distance}\rangle_{\nu_{\mathcal{G}_n}}\) is in principle an \((18n-12)\)-dimensional integral
Using the theorem, can reduce to a \(6\)-dimensional integral.
What about including distributions on bond angles in addition to bond lengths?
Sampling algorithms?
Steric constraints and the complete graph?
J. Cantarella, T. Deguchi, C. Shonkwiler, E. Uehara, Gaussian random embeddings of multigraphs, preprint, 2020, arXiv:2001.11709
J. Cantarella, T. Deguchi, C. Shonkwiler, E. Uehara, Radius of gyration, contraction factors, and subdivisions of topological polymers, preprint, 2020, arXiv:2004.06199
J. Cantarella, T. Deguchi, C. Shonkwiler, E. Uehara, Random graph embeddings with general edge potentials, preprint, 2021, on arXiv soon!