Heterogeneous Solvatochromism of Fluorescent DNA-Stabilized Silver Clusters Precludes Use of Simple Onsager-Based Stokes Shift Models

The Journal of Physical Chemistry Letters
Stacy M CoppElisabeth G Gwinn

Abstract

The diverse optical and chemical properties of DNA-stabilized silver clusters (AgN-DNAs) have challenged the development of a common model for these sequence-tunable fluorophores. Although correlations between cluster geometry and fluorescence color have begun to shed light on how the optical properties of AgN-DNAs are selected, the exact mechanisms responsible for fluorescence remain unknown. To explore these mechanisms, we study four distinct purified AgN-DNAs in ethanol-water and methanol-water mixtures and find that the solvatochromic behavior of AgN-DNAs varies widely among different cluster species and differs markedly from prior results on impure material. Placing AgN-DNAs within the context of standard Lippert-Mataga solvatochromism models based on the Onsager reaction field, we show that such nonspecific solvent models are not universally applicable to AgN-DNAs. Instead, alcohol-induced solvatochromism of AgN-DNAs may be governed by changes in hydration of the DNA template, with spectral shifts resulting from cluster shape changes and/or dielectric changes in the local vicinity of the cluster.

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Citations

May 18, 2016·Nano Letters·Stacy M CoppElisabeth G Gwinn
Nov 9, 2017·Chemical Communications : Chem Comm·Cecilia CerretaniTom Vosch
Jun 22, 2016·Physical Chemistry Chemical Physics : PCCP·Galina V LoukovaVladimir I Minkin
Feb 10, 2018·Methods and Applications in Fluorescence·Sidsel Ammitzbøll BoghTom Vosch
Jul 31, 2018·ACS Nano·Stacy M CoppElisabeth G Gwinn
Nov 3, 2020·ACS Applied Nano Materials·Puskal Kunwar, Pranav Soman
Oct 9, 2020·The Journal of Physical Chemistry Letters·Yuyuan ZhangBern Kohler

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