Understanding Self-Assembled Pseudoisocyanine Dye Aggregates in DNA Nanostructures and Their Exciton Relay Transfer Capabilities.
Understanding Self-Assembled Pseudoisocyanine Dye Aggregates in DNA Nanostructures and Their Exciton Relay Transfer Capabilities.
复制标题
DOI：
10.1021/acs.jpcb.1c09048
复制
发表时间：
2022-01-13
期刊：
影响因子：
--
通讯作者：
Medintz IL
中科院分区：
文献类型：
--
作者：
Chiriboga M;Diaz SA;Mathur D;Hastman DA;Melinger JS;Veneziano R;Medintz IL
使用B型DNA双链体作为模板，在有序的分子聚集体（称为J聚集体）中形成发色团，已经取得了进展。这些聚集体可以表现出强的电子耦合，延长的相干寿命，和长程激子离域在适当的条件下。某些花青染料如假异氰（PIC）染料已经显示出在特定DNA序列中形成聚集体的倾向。特别是，含有非交替聚（dA）-聚（dT）二核苷酸轨道（AT轨道）的DX-瓦片，模板非共价PIC染料聚集体，已被证明表现出有趣的新兴光子特性。这些基于DNA的聚集体由于其与J聚集体的相似性而被称为J比特。在这里，我们组装多荧光团DX瓦片支架模板J位成连续和非连续的线性阵列。我们的目标是了解非连续J位阵列的中继能力，并探讨方向和位置对它们之间的能量传递的影响。我们发现线性连续的J位可以将激子从初始AlexaFluor 405供体中继到终端AlexaFluor 647受体，距离高达16.3 nm。我们观察到在最短支架中能量转移的最大增加为41%，并且在最大距离上能量转移增加了11%。然而，在非线性阵列中，激子转移是不可检测的，即使当离轴J位到J位转移距离<2nm时。这些结果，结合之前对PIC−DNA系统的研究，表明基于PIC− DNA的系统目前可能仅限于简单的1-D设计，这会阻止隔离J位以增强能量传递特性，直到对系统进行进一步的理解和改进。
Progress has been made using B-form DNA duplex strands to template chromophores in ordered molecular aggregates known as J-aggregates. These aggregates can exhibit strong electronic coupling, extended coherent lifetimes, and long-range exciton delocalization under appropriate conditions. Certain cyanine dyes such as pseudoisocyanine (PIC) dye have shown a proclivity to form aggregates in specific DNA sequences. In particular, DX-tiles containing nonalternating poly(dA)−poly(dT) dinucleotide tracks (AT-tracks), which template noncovalent PIC dye aggregates, have been demonstrated to exhibit interesting emergent photonic properties. These DNA-based aggregates are referred to as J-bits for their similarity to J-aggregates. Here, we assemble multifluorophore DX-tile scaffolds which template J-bits into both contiguous and noncontiguous linear arrays. Our goal is to understand the relay capability of noncontiguous J-bit arrays and probe the effects that orientation and position have on the energy transfer between them. We find that linearly contiguous J-bits can relay excitons from an initial AlexaFluor 405 donor to a terminal AlexaFluor 647 acceptor across a distance of up to 16.3 nm. We observed a maximum increase in energy transfer of 41% in the shortest scaffold and an 11% increase in energy transfer across the maximum distance. However, in nonlinear arrays, exciton transfer is not detectable, even when off-axis J-bit-to-J-bit transfer distances were <2 nm. These results, in conjunction with the previous work on PIC−DNA systems, suggest that PIC−DNA-based systems may currently be limited to simple 1-D designs, which prevent isolating J-bits for enhanced energy-transfer characteristics until further understanding and improvements to the system can be made.
登录
查看更多内容
影响因子：
3.4
作者：
Biver, T;De Biasi, A;Yarmoluk, S
通讯作者：
Yarmoluk, S
影响因子：
13.3
作者：
Hannestad, Jonas K.;Gerrard, Simon R.;Albinsson, Bo
通讯作者：
Albinsson, Bo
影响因子：
4.4
作者：
Bricker, William P.;Banal, James L.;Bathe, Mark
通讯作者：
Bathe, Mark
影响因子：
3.3
作者：
Kamalakshan, Adithya;Ansilda, Roselin;Mandal, Sarthak
通讯作者：
Mandal, Sarthak
影响因子：
48
作者：
Algar, W. Russ;Hildebrandt, Niko;Medintz, Igor L.
通讯作者：
Medintz, Igor L.