Frequency-Upconverted Stimulated Emission by Up to Six-Photon Excitation from Highly Extended Spiro-Fused Ladder-Type Oligo(p-phenylene)s

Yi Jiang; King Fai Li; Kun Gao; He Lin; Hoi Lam Tam; Yuan-Yuan Liu; Yu Shu; Ka-Leung Wong; Wen-Yong Lai; Kok Wai Cheah; Wei Huang

doi:10.1002/anie.202100542

Frequency-Upconverted Stimulated Emission by Up to Six-Photon Excitation from Highly Extended Spiro-Fused Ladder-Type Oligo(p-phenylene)s

Yi Jiang (Co-first Author), King Fai Li (Co-first Author), Kun Gao, He Lin, Hoi Lam Tam, Yuan-Yuan Liu, Yu Shu, Ka-Leung Wong, Wen-Yong Lai^*, Kok Wai Cheah^*, Wei Huang^*

^*Corresponding author for this work

Research output: Journal Publications and Reviews › RGC 21 - Publication in refereed journal › peer-review

69 Citations (Scopus)

Abstract

Frequency-upconverted fluorescence and stimulated emission induced by multiphoton absorption (MPA) have attracted much interest. As compared with low-order MPA processes, the construction of high-order MPA processes is highly desirable and rather attractive, yet remains a formidable challenge due to its inherent low transition probability. We report the observation of the first experimental frequency-upconverted fluorescence and stimulated emission by simultaneous six-photon excitation in an organic molecular system. The well-designed organic conjugated system based on cross-shaped spiro-fused ladder-type oligo(p-phenylene)s (SpL−z, z=1–3) manifests reasonably high MPA cross-sections and brilliant luminescence emission simultaneously. The six-photon absorption cross-section of SpL-3 with an extended π-conjugation was evaluated as 8.67 × 10⁻¹⁶⁹ cm¹² s⁵ photon⁻⁵. Exceptionally efficient 2- to 6-photon excited stimulated emission was achieved under near-infrared laser excitation. © 2021 Wiley-VCH GmbH.

Original language	English
Pages (from-to)	10007-10015
Number of pages	9
Journal	Angewandte Chemie - International Edition
Volume	60
Issue number	18
Online published	21 Jan 2021
DOIs	https://doi.org/10.1002/anie.202100542
Publication status	Published - 26 Apr 2021
Externally published	Yes

Funding

The authors acknowledge financial support from the National Natural Science Foundation of China (21835003, 91833304, 21422402, 21674050), the National Key Basic Research Program of China (2017YFB0404501, 2014CB648300), the Natural Science Foundation of Jiangsu Province (BE2019120), Program for Jiangsu Specially-Appointed Professor (RK030STP15001), the Six Talent Peaks Project of Jiangsu Province (TD-XCL-009), the 333 Project of Jiangsu Province (BRA2017402), the NUPT “1311 Project” and Scientific Foundation (NY218164, NY217169), the Leading Talent of Technological Innovation of National Ten-Thousands Talents Program of China, the Excellent Scientific and Technological Innovative Teams of Jiangsu Higher Education Institutions (TJ217038), the Synergetic Innovation Center for Organic Electronics and Information Displays, and the Priority Academic Program Development of Jiangsu Higher Education Institutions (PAPD, YX030003).

Research Keywords

frequency-upconverted stimulated emission
MPA cross-section
multiphoton absorption (MPA)
oligo(p-phenylene)s
spiro-fused molecules

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Jiang, Y., Li, K. F., Gao, K., Lin, H., Tam, H. L., Liu, Y.-Y., Shu, Y., Wong, K.-L., Lai, W.-Y., Cheah, K. W., & Huang, W. (2021). Frequency-Upconverted Stimulated Emission by Up to Six-Photon Excitation from Highly Extended Spiro-Fused Ladder-Type Oligo(p-phenylene)s. Angewandte Chemie - International Edition, 60(18), 10007-10015. https://doi.org/10.1002/anie.202100542

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title = "Frequency-Upconverted Stimulated Emission by Up to Six-Photon Excitation from Highly Extended Spiro-Fused Ladder-Type Oligo(p-phenylene)s",

abstract = "Frequency-upconverted fluorescence and stimulated emission induced by multiphoton absorption (MPA) have attracted much interest. As compared with low-order MPA processes, the construction of high-order MPA processes is highly desirable and rather attractive, yet remains a formidable challenge due to its inherent low transition probability. We report the observation of the first experimental frequency-upconverted fluorescence and stimulated emission by simultaneous six-photon excitation in an organic molecular system. The well-designed organic conjugated system based on cross-shaped spiro-fused ladder-type oligo(p-phenylene)s (SpL−z, z=1–3) manifests reasonably high MPA cross-sections and brilliant luminescence emission simultaneously. The six-photon absorption cross-section of SpL-3 with an extended π-conjugation was evaluated as 8.67 × 10−169 cm12 s5 photon−5. Exceptionally efficient 2- to 6-photon excited stimulated emission was achieved under near-infrared laser excitation. {\textcopyright} 2021 Wiley-VCH GmbH.",

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author = "Yi Jiang and Li, {King Fai} and Kun Gao and He Lin and Tam, {Hoi Lam} and Yuan-Yuan Liu and Yu Shu and Ka-Leung Wong and Wen-Yong Lai and Cheah, {Kok Wai} and Wei Huang",

year = "2021",

month = apr,

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doi = "10.1002/anie.202100542",

language = "English",

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Frequency-Upconverted Stimulated Emission by Up to Six-Photon Excitation from Highly Extended Spiro-Fused Ladder-Type Oligo(p-phenylene)s. / Jiang, Yi (Co-first Author); Li, King Fai (Co-first Author); Gao, Kun et al.
In: Angewandte Chemie - International Edition, Vol. 60, No. 18, 26.04.2021, p. 10007-10015.

Research output: Journal Publications and Reviews › RGC 21 - Publication in refereed journal › peer-review

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T1 - Frequency-Upconverted Stimulated Emission by Up to Six-Photon Excitation from Highly Extended Spiro-Fused Ladder-Type Oligo(p-phenylene)s

AU - Jiang, Yi

AU - Li, King Fai

AU - Gao, Kun

AU - Lin, He

AU - Tam, Hoi Lam

AU - Liu, Yuan-Yuan

AU - Shu, Yu

AU - Wong, Ka-Leung

AU - Lai, Wen-Yong

AU - Cheah, Kok Wai

AU - Huang, Wei

PY - 2021/4/26

Y1 - 2021/4/26

N2 - Frequency-upconverted fluorescence and stimulated emission induced by multiphoton absorption (MPA) have attracted much interest. As compared with low-order MPA processes, the construction of high-order MPA processes is highly desirable and rather attractive, yet remains a formidable challenge due to its inherent low transition probability. We report the observation of the first experimental frequency-upconverted fluorescence and stimulated emission by simultaneous six-photon excitation in an organic molecular system. The well-designed organic conjugated system based on cross-shaped spiro-fused ladder-type oligo(p-phenylene)s (SpL−z, z=1–3) manifests reasonably high MPA cross-sections and brilliant luminescence emission simultaneously. The six-photon absorption cross-section of SpL-3 with an extended π-conjugation was evaluated as 8.67 × 10−169 cm12 s5 photon−5. Exceptionally efficient 2- to 6-photon excited stimulated emission was achieved under near-infrared laser excitation. © 2021 Wiley-VCH GmbH.

AB - Frequency-upconverted fluorescence and stimulated emission induced by multiphoton absorption (MPA) have attracted much interest. As compared with low-order MPA processes, the construction of high-order MPA processes is highly desirable and rather attractive, yet remains a formidable challenge due to its inherent low transition probability. We report the observation of the first experimental frequency-upconverted fluorescence and stimulated emission by simultaneous six-photon excitation in an organic molecular system. The well-designed organic conjugated system based on cross-shaped spiro-fused ladder-type oligo(p-phenylene)s (SpL−z, z=1–3) manifests reasonably high MPA cross-sections and brilliant luminescence emission simultaneously. The six-photon absorption cross-section of SpL-3 with an extended π-conjugation was evaluated as 8.67 × 10−169 cm12 s5 photon−5. Exceptionally efficient 2- to 6-photon excited stimulated emission was achieved under near-infrared laser excitation. © 2021 Wiley-VCH GmbH.

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Frequency-Upconverted Stimulated Emission by Up to Six-Photon Excitation from Highly Extended Spiro-Fused Ladder-Type Oligo(p-phenylene)s

Abstract

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Research Keywords

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