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Using the isotope effect to probe an aggregation induced emission mechanism: theoretical prediction and experimental validation.

ABSTRACT: Aggregation-induced emission (AIE) has become a hot topic for a variety of potential applications, but the understanding of its working mechanism is still under scrutiny. Herein, we proposed the use of the isotope effect (IE) to identify the AIE mechanism: under the restriction of an internal motion mechanism, the IE is pronouncedly different in excited-state decay rates when contrasting AIE luminogens (AIEgens) and non-AIEgens in theoretical calculations. For the complete deuteration of AIEgens, the IE of nonradiative decay rate in solution (<-10%) is much weaker than that (-65% to -95%) in aggregate, because the former stems from the overall results of competitive vibronic coupling and the severe mixing of low-frequency modes while the latter mainly comes from the vibronic coupling only. The experimental results confirm the isotopic "jump" behaviors in AIEgens well. However, non-AIEgens exhibit equivalent IEs (-40% to -90%) in both solution and solid phases. Further partial deuteration schemes for the 6-ring AIE analogues show positional dependence.

SUBMITTER: Zhang T

PROVIDER: S-EPMC6022082 | biostudies-other | 2016 Aug

REPOSITORIES: biostudies-other

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Using the isotope effect to probe an aggregation induced emission mechanism: theoretical prediction and experimental validation.

Zhang Tian T Peng Qian Q Quan Changyun C Nie Han H Niu Yingli Y Xie Yujun Y Zhao Zujin Z Tang Ben Zhong BZ Shuai Zhigang Z

Chemical science 20160511 8

Aggregation-induced emission (AIE) has become a hot topic for a variety of potential applications, but the understanding of its working mechanism is still under scrutiny. Herein, we proposed the use of the isotope effect (IE) to identify the AIE mechanism: under the restriction of an internal motion mechanism, the IE is pronouncedly different in excited-state decay rates when contrasting AIE luminogens (AIEgens) and non-AIEgens in theoretical calculations. For the complete deuteration of AIEgens ...[more]

PMID: 30034698

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Project description:We report the effect of the probe location and wavelength on the emission spatial distribution and spectral properties of fluorophores located on structures which display Tamm states. Our structure consists of a one-dimensional photonic crystal (1DPC)-that is, a multilayer structure of alternate high and low refractive index dielectrics-and a thin top silver film. Simulations show the presence of Tamm and surface plasmon modes in the structure. The electric field intensities for the Tamm modes are located mostly in the dielectric layer below the metal film. The corresponding field intensities for the surface plamon modes are located above the metal film in the distal side. Tamm states can be in resonance with the incident light normal or near normal to the surface, within the light line, and can be accessed without the use of a coupling prism or gratings. We investigated the emission spectra and angular distribution of the emission for probes located above and below the metal film to explore the interaction of fluorophores with Tamm plasmons and surface plasmons modes. Three probes were chosen with different overlap of the emission spectra with the Tamm modes. The fluorophores below the metal film coupled predominantly with the Tamm state and displayed more intense and only Tamm state-coupled emission (TSCE). Probes above the metal film display both surface plasmon-coupled emission (SPCE) and Tamm state-coupled emission. In contrast to SPCE, which shows only KR, P-polarized emission, the Tamm states can display both S- and P-polarized emission and can be populated using both RK and KR illuminations. The TSCE angle is highly sensitive to wavelength, which suggests the use of Tamm structures to provide both directional emission and wavelength dispersion. The combination of plasmonic and photonic structures with directional emission close to surface normal offers the opportunities for new design formats for clinical testing, portable devices, and other fluorescence-based applications.

Dataset Information

Using the isotope effect to probe an aggregation induced emission mechanism: theoretical prediction and experimental validation.

Publications

Using the isotope effect to probe an aggregation induced emission mechanism: theoretical prediction and experimental validation.

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