multiexciton interactions in singlet fission and triplet fusion upconversion dendrimers

Singlet fission (SF) and triplet-triplet annihilation upconversion (TTA-UC) are two multiexciton processes intimately related to the dynamic interaction between one high-lying energy singlet and two low-lying energy triplet excitons. Here, we introduce a series of dendritic macromolecules that serve as a platform to study the effect of interchromophore interactions on the dynamics of multiexciton generation and decay as a function of dendrimer generation. The dendrimers (generations 1-4) consist of trimethylolpropane (TMP) core and 2,2-bis(methylol)propionic acid (bis-MPA) dendrons that provide exponential growth of the branches, leading to a corona decorated with pentacenes for SF or anthracenes for TTA-UC. The findings reveal a trend where a few highly ordered sites emerge as the dendrimer generation grows, dominating the multiexciton dynamics, as deduced from optical spectra, and transient absorption spectroscopy. While the dendritic structures enhance TTA-UC at low annihilator conce..., An dendrimer:Normalized absorbance spectra in chloroform at 0.03 mg/mL.UCPL data were performed with PdTPTBP (50 uM) with corresponding annihilator concentration as shown.
Pc dendrimer:UV-vis and fluorescence spectra were measured using the diluted pentacene dendrimer solution.Transient absorption data were collected by Helios and EOS excited by 600 nm pulse  Here, fs-TA data are after chirp correction and ns-TA are after time zero correction for figures in the manuscript.
Sensitization measurements were performed in toluene solution of anthracene (~10 mM) with low concentrations of dendrimers excited by 360 nm pulse. The data here are after time zero correction., , # Data from: multiexciton interactions in singlet fission and triplet fusion upconversion dendrimers

***

Model systems designed to investigate the multiexciton interactions in dendrimers (G1-G4). Anthracene (An) dendrimer is upconversion-active and pentacene (Pc) dendrimer is singlet fission-active.

UV-vis and fluorescence (including UCPL) of dendrimers were used to generate Fig 2 in this manuscript:

Raw transient absorption data sets using mechanical (fs label) and electronic (ns label) delays. Units are picoseconds for time and nm for wavelength. Sensitization data (sens label) are taken using the nanosecond configuration. These data were used to generate Fig 3 and 4 in this manuscript:

## Description of the Data and file structure

### Table of Contents

***

* An dendrimer:
* Anth-dendrimer UCPL raw data.csv
* TTA-UC dendrimer absorption chloroform.xlsx
* Pc dendrimer
* UV-vis
* G1\_Pc\_tol\_4.txt
* G2\_Pc\_tol\_4.txt
* G3\_Pc\_tol\_4.txt
...

单线态裂变（Singlet Fission, SF）与三线态-三线态湮灭上转换（Triplet-Triplet Annihilation Upconversion, TTA-UC）是两类紧密关联的多激子过程，二者均涉及一个高能量单线态激子与两个低能量三线态激子之间的动态相互作用。本研究构建了一系列树枝状大分子（dendrimer）作为研究平台，用以探究发色团间相互作用对多激子生成与衰减动力学的影响，且该影响随树枝状大分子的代数变化而变化。本研究涉及的树枝状大分子（代数1至4）以三羟甲基丙烷（Trimethylolpropane, TMP）为核，通过2,2-双(羟甲基)丙酸（2,2-bis(methylol)propionic acid, bis-MPA）树枝状臂实现分支的指数级增长，最终在表面修饰可用于单线态裂变的并五苯（pentacenes）或可用于三线态-三线态湮灭上转换的蒽（anthracenes）。
尽管树枝状结构可在低湮灭剂浓度下提升TTA-UC性能，[原文未完整表述] 蒽修饰树枝状大分子：于0.03 mg/mL的氯仿溶液中测得归一化吸收光谱。上转换光致发光（Upconversion Photoluminescence, UCPL）测试以50 μM的PdTPTBP为敏化剂，湮灭剂浓度如文中所示。
并五苯修饰树枝状大分子：采用稀释的并五苯树枝状大分子溶液测试紫外-可见吸收光谱与荧光光谱。瞬态吸收数据由搭载600 nm脉冲激发源的Helios与EOS系统采集：飞秒瞬态吸收（femtosecond Transient Absorption, fs-TA）数据已完成啁啾校正，纳秒瞬态吸收（nanosecond Transient Absorption, ns-TA）数据已完成时间零点校正，用于本文相关图表绘制。
敏化测试在浓度约10 mM的蒽甲苯溶液中开展，采用低浓度的树枝状大分子作为样品，以360 nm脉冲激发，测试数据已完成时间零点校正。

# 数据来源：单线态裂变与三线态融合上转换树枝状大分子中的多激子相互作用

*** 本研究构建模型体系以探究树枝状大分子（代数G1-G4）中的多激子相互作用。其中，蒽（Anthracene, An）修饰树枝状大分子具备上转换活性，而并五苯（Pentacene, Pc）修饰树枝状大分子具备单线态裂变活性。
树枝状大分子的紫外-可见吸收光谱与荧光光谱（含上转换光致发光光谱）用于绘制本文图2：
原始瞬态吸收数据集分为机械延迟（标注fs）与电子延迟（标注ns）两类，时间单位为皮秒，波长单位为纳米。敏化测试数据（标注sens）采用纳秒配置采集，上述数据用于绘制本文图3与图4：

## 数据与文件结构说明
### 目录结构
***
* 蒽修饰树枝状大分子（An dendrimer）：
* Anth-dendrimer UCPL raw data.csv
* TTA-UC dendrimer absorption chloroform.xlsx
* 并五苯修饰树枝状大分子（Pc dendrimer）：
* 紫外-可见吸收数据
* G1_Pc_tol_4.txt
* G2_Pc_tol_4.txt
* G3_Pc_tol_4.txt
...