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首页三重态自旋相互作用对单重态裂变影响的实验研究
三重态自旋相互作用对单重态裂变影响的实验研究
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"该研究论文探讨了三重态之间的自旋-自旋相互作用如何影响中间三重态-三重态对中向单重态裂变的不同自旋态之间的转换,通过光致发光(MFEPL)磁场效应进行实验研究。实验涉及了多晶固体粉末、非晶态固体膜和液体溶液三种形态,并发现多晶固体粉末显示出更强的MFEPL现象,这表明其内部存在增强的三重态间自旋相互作用。这种增强的相互作用促进了单重态裂变的过程。" 本文的研究重点在于理解自旋态之间的相互转化如何影响光诱导的单重态裂变过程。单重态裂变是一种重要的物理现象,在太阳能电池和有机光电子材料中具有潜在应用。在三重态-三重态对中,自旋态的转换是通过三重态间的自旋相互作用来实现的。实验中,作者使用并四苯作为模型系统,通过观察不同形态材料的MFEPL响应来评估自旋相互作用的影响。 多晶固体粉末显示出比非晶态固体膜更强烈的MFEPL效应,这意味着在多晶结构中,三重态间的自旋相互作用更为显著。这种增强的自旋相互作用导致中间三重态对中不同自旋态的转换率增加,进而促进单重态裂变。吸收光谱和X射线衍射数据进一步支持了这一观点,显示多晶固体粉末中的分子间电子相互作用比非晶态更强。 研究还指出,固体粉末中多晶结构的存在可能加剧了这种自旋相互作用,因为分子间的排列更加有序,有利于自旋态的耦合。这些发现对于设计和优化具有高效单重态裂变性能的材料至关重要,特别是在开发新型太阳能技术和其他光子应用中。 这篇研究论文揭示了三重态间自旋-自旋相互作用在单重态裂变过程中的重要作用,强调了材料的微观结构对这一过程的影响。通过增强自旋相互作用,可以有效地调控中间三重态对的自旋态转换,这对于理解和控制有机半导体材料的光物理性质具有深远意义。
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Letter
Inter-triplet spin–spin interaction effects on inter-conversion
between different spin states in intermediate triplet–triplet
pairs towards singlet fission
Xianfeng Qiao
a
, Lin Luan
a
, Yuchun Liu
a
, Zhigang Yu
c
, Bin Hu
a,b,
⇑
a
WuHan National Laboratory for Optoelectronics, Huazhong University of Science and Technology, Wu Han 430074, China
b
Department of Materials Science and Engineering, University of Tennessee, Knoxville, TN 37996, USA
c
Applied Optics Lab. Stanford Research Institute, Ravenswood Ave, Menlo Park, California 94025, USA
article info
Article history:
Received 21 April 2014
Received in revised form 10 May 2014
Accepted 11 June 2014
Available online 22 June 2014
Keywords:
Singlet fission
Spin interaction
Magnetic field effects
Tetracene
Electronic interaction
abstract
This article reports the experimental studies on the effects of inter-triplet spin interaction
on singlet fission by using magnetic field effects of photoluminescence (MFE
PL
) based on
tetracene. The MFE
PL
are compared for three different morphological states based on poly-
crystalline solid powder, amorphous solid film, and liquid solution. It is observed that the
polycrystalline solid powder gives stronger MFE
PL
than that of amorphous solid film, while
the liquid solution exhibits no detectable MFE
PL
. In essence, the MFE
PL
are determined by
the inter-conversion between different spin states initiated by inter-triplet spin interaction
through spin mixing in intermediate triplet–triplet pairs towards the singlet fission. The
different MFE
PL
amplitudes suggest that the polycrystalline solid powder possesses an
enhanced inter-triplet spin interaction in intermediate triplet–triplet pairs as compared
to amorphous solid film. As a result, the enhanced inter-triplet spin interaction can cause
a larger inter-conversion between different spin states in intermediate triplet–triplet pairs
and consequently increases the singlet fission within polycrystalline structures. The
absorption spectral characteristics and X-ray diffraction data confirm that the polycrystal-
line solid powder can indeed exhibits stronger intermolecular electronic interaction rela-
tive to amorphous solid film. Here, the stronger intermolecular electronic interaction
provides an evidence for the enhanced inter-triplet spin interaction occurring within poly-
crystalline structures in the solid powder. Our experimental results indicate that increasing
the inter-triplet spin interaction can boost the inter-conversion between different spin
states in intermediate triplet–triplet pairs and consequently facilitates the singlet fission.
Ó 2014 Elsevier B.V. All rights reserved.
1. Introduction
Singlet fission is a bimolecular process in excited states
occurring in organic photovoltaic and photodetector mate-
rials [1–3]. The singlet fission can be described by Merri-
field theory [4,5] based on spin conservation. Recently, it
has been found that the singlet fission undergoes the inter-
mediate triplet–triplet pair states [6,7]. In particular, the
spin–spin interaction within triplet–triplet pairs is a neces-
sary component to generate the singlet fission. Further-
more, it has been shown that the coupling between
chromophore molecules can largely enhance the singlet
fission [8]. However, it is still not clear on how the spin–
spin interaction is involved in the spin conservation
through intermediate triplet–triplet pair states to generate
http://dx.doi.org/10.1016/j.orgel.2014.06.015
1566-1199/Ó 2014 Elsevier B.V. All rights reserved.
⇑
Corresponding author at: WuHan National Laboratory for Optoelec-
tronics, Huazhong University of Science and Technology, Wu Han
430074,China.
E-mail address: bhu@utk.edu (B. Hu).
Organic Electronics 15 (2014) 2168–2172
Contents lists available at ScienceDirect
Organic Electronics
journal homepage: www.elsevier.com/locate/orgel
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