Three-photon-induced singlet excited-state absorption for tunable ultrafast optical-limiting in distyrylbenzene: a first-principles study

The ground and first singlet excited state absorption in distyrylbenzene (DSB) is simulated based on linear-response time dependent density functional theory (LR-TDDFT). It is found that distyrylbenzene shows a strong reverse saturable absorption effect around the near-infrared range. Combining the...

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Published in:Physical chemistry chemical physics : PCCP 2022-07, Vol.24 (27), p.16852-16861
Main Authors: Zhang, Danyang, Zhu, Hongjuan, Wang, Chunrui, Kang, Shuying, Zhou, Yong, Sheng, Xiaowei
Format: Article
Language:English
Subjects:
Constraining
Density functional theory
Excitation
First principles
Light levels
Luminous intensity
Near infrared radiation
Optical limiters
Photon absorption
Photons
Pi-electrons
Response functions
Response time
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Summary:The ground and first singlet excited state absorption in distyrylbenzene (DSB) is simulated based on linear-response time dependent density functional theory (LR-TDDFT). It is found that distyrylbenzene shows a strong reverse saturable absorption effect around the near-infrared range. Combining the calculations of cubic response functions to simulate the three-photon absorption in distyrylbenzene, we are able to show that distyrylbenzene is a promising ultrafast optical limiter for the light with wavelengths around 775 nm. The primary mechanism for the optical limiting behavior can be well understood by the three-photon induced excited state absorption (3PA-ESA). This result in that DSB has high transmittance for low-intensity ambient light levels and the ultrafast response of optical-limiting. In addition, the limited optical window can be tuned by changing the length of the -electron conjugated structure. It was also discovered that the molecular aggregation has an inhibitory effect on the optical limiting efficiency of distyrylbenzene. The present results may serve as a theoretical guideline for the design of distyrylbenzene-based optical limiting materials. The present paper illustrates that distyrylbenzene is a promising ultrafast optical limiter for wavelengths around 775 nm, which can be well understood by three-photon induced excited state absorption.
ISSN:1463-9076
1463-9084
DOI:10.1039/d2cp01753a