Perspective for aggregation-induced delayed fluorescence mechanism: A QM/MM study

Jie Liu; Jianzhong Fan; Kai Zhang; Yuchen Zhang; Chuan-Kui Wang; Lili Lin

doi:10.1088/1674-1056/aba2d9

Chinese Physics B, Volume. 29, Issue 8, (2020)

Perspective for aggregation-induced delayed fluorescence mechanism: A QM/MM study

Jie Liu, Jianzhong Fan, Kai Zhang, Yuchen Zhang, Chuan-Kui Wang^†, and Lili Lin

Key Laboratory of Medical Physics and Image Processing & Shandong Provincial Engineering and Technical Center of Light Manipulations, School of Physics and Electronics, Shandong Normal University, Jinan 250358, China

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Fig. 1. (a) Chemical structure of DMF-BP-DMAC. (b) The atomic labels and the interesting bond lengths (B₁, B₂), bond angles (θ₁, θ₂), and dihedral angles (α₁, α₂, α₃, and α₄). (c) ONIOM model: surrounding molecules are regarded as low layer and the centered DMF-BP-DMAC is treated as high layer.

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Fig. 2. Geometry changes between two selected states for DMF-BP-DMAC in THF (a) and solid phase (b).

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Fig. 3. Energy levels and distributions of HOMO and LUMO for molecule in THF and solid phase (isovalue = 0.02).

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Fig. 4. Adiabatic excitation energies for DMF-BP-DMAC in THF (a) and solid phase (b).

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Fig. 5. Transition characteristics for S₁, T₁, and T₂ of DMF-BP-DMAC in THF (a) and transition characteristics for S₁, T₁, T₂, and T₃ of DMF-BP-DMAC in solid phase (b) (isovalue = 0.02). The value below every arrow represents the component of localized excitation in the corresponding transition.

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Fig. 6. The calculated HR factors of DMF-BP-DMAC in THF (a) and solid phase (b). The corresponding vibration modes are shown in inset.

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Table 1. Emission wavelength and oscillator strength calculated by different functionals for DMF-BP-DMAC in tetrahydrofuran (THF) and solid phase.
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Table 1. Emission wavelength and oscillator strength calculated by different functionals for DMF-BP-DMAC in tetrahydrofuran (THF) and solid phase.
THF Solid
λ/nm f λ/nm f
B3LYP 590 0.0001 561 0.0068
PBE0 542 0.0001 517 0.0089
BMK 447 0.0006 430 0.0176
M062X 394 0.0223 396 0.0055
Exp.^a 534 – 510 –

Table 2. Geometry parameters of S₀, S₁, T₁, and T₂ states for DMF-BP-DMAC in THF and those of S₀, S₁, T₁, T₂, and T₃ states for DMF-BP-DMAC in solid phase. Bond lengths (B₁, B₂), bond angles (θ₁, θ₂), and dihedral angles (α₁, α₂, α₃, α₄) are marked in Fig. 1(b).

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Table 2. Geometry parameters of S₀, S₁, T₁, and T₂ states for DMF-BP-DMAC in THF and those of S₀, S₁, T₁, T₂, and T₃ states for DMF-BP-DMAC in solid phase. Bond lengths (B₁, B₂), bond angles (θ₁, θ₂), and dihedral angles (α₁, α₂, α₃, α₄) are marked in Fig. 1(b).

	THF				Solid
	S₀	S₁	T₁	T₂	S₀	S₁	T₁	T₂	T₃
B₁	1.23	1.27	1.27	1.27	1.22	1.26	1.26	1.25	1.25
B₂	1.43	1.44	1.43	1.43	1.42	1.45	1.44	1.44	1.44
θ₁	120.39	121.71	121.88	121.71	119.17	119.01	119.50	120.26	120.24
θ₂	119.27	120.20	119.92	120.17	119.96	120.58	120.38	120.05	120.05
α₁	27.62	32.42	32.88	33.71	−40.28	−40.62	−41.10	−34.94	−34.98
α₂	−79.38	−89.98	−67.94	−110.49	75.99	83.60	75.79	78.03	77.98
α₃	81.24	−91.10	−69.22	−111.09	84.53	81.04	73.37	79.48	79.42
α₄	39.06	0.20	−1.88	2.51	−38.53	−33.84	−34.64	−36.44	−36.52

Table 3. Spin–orbit coupling (SOC), reorganization energy (λ), energy difference (ΔE), intersystem crossing rates (K_ISC), and reverse intersystem crossing rates (K_RISC) between single excited states and triplet excited states.

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Table 3. Spin–orbit coupling (SOC), reorganization energy (λ), energy difference (ΔE), intersystem crossing rates (K_ISC), and reverse intersystem crossing rates (K_RISC) between single excited states and triplet excited states.

		SOC^a/cm⁻¹	SOC^b/cm⁻¹	λ_S/meV	λ_T/meV	ΔE/meV	K_ISC/s⁻¹	K_RISC/s⁻¹
THF	S₁–T₁	0.01	0.44	124.2	15.6	24.1	1.98 × 10⁵	1.87 × 10¹⁰
	S₁–T₂	0.67	1.84	106.4	421.1	17.6	4.14 × 10⁶	6.57 × 10⁸
	S₁–T₃	0.33	0.34	271.5	292.3	-419.4	2.51 × 10⁷	2.5
Solid	S₁–T₁	0.19	0.39	52.1	24.5	47.7	4.81 × 10⁷	2.68 × 10⁷
	S₁–T₂	0.38	0.44	148.3	225.4	-146.5	2.00 × 10⁵	1.30 × 10⁸
	S₁–T₃	0.60	0.81	148.5	510.3	-146.5	3.47 × 10⁴	4.40 × 10⁸

Table 4. Calculated radiative rate (K_r), effective intersystem crossing rates ( $K_{ISC}^{Cal}$ ), and effective reverse intersystem crossing rates ( $K_{RISC}^{Cal}$ ).
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Table 4. Calculated radiative rate (K_r), effective intersystem crossing rates ( $K_{ISC}^{Cal}$ ), and effective reverse intersystem crossing rates ( $K_{RISC}^{Cal}$ ).
THF Solid
Kr/s−1 2.27 × 104 2.29 × 106
2.18 × 107 4.79 × 107
1.81 × 1010 4.25 × 108

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Jie Liu, Jianzhong Fan, Kai Zhang, Yuchen Zhang, Chuan-Kui Wang, Lili Lin. Perspective for aggregation-induced delayed fluorescence mechanism: A QM/MM study[J]. Chinese Physics B, 2020, 29(8):

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Paper Information

Received: May. 2, 2020

Accepted: --

Published Online: Apr. 29, 2021

The Author Email: Wang Chuan-Kui (linll@sdnu.edu.cn)

DOI:10.1088/1674-1056/aba2d9

Topics

Nuclear physics

Particles and fields

Particle and nuclear astrophysics and cosmology

Table 1. Emission wavelength and oscillator strength calculated by different functionals for DMF-BP-DMAC in tetrahydrofuran (THF) and solid phase.

Table 1. Emission wavelength and oscillator strength calculated by different functionals for DMF-BP-DMAC in tetrahydrofuran (THF) and solid phase.

Table 2. Geometry parameters of S0, S1, T1, and T2 states for DMF-BP-DMAC in THF and those of S0, S1, T1, T2, and T3 states for DMF-BP-DMAC in solid phase. Bond lengths (B1, B2), bond angles (θ1, θ2), and dihedral angles (α1, α2, α3, α4) are marked in Fig. 1(b).

Table 2. Geometry parameters of S0, S1, T1, and T2 states for DMF-BP-DMAC in THF and those of S0, S1, T1, T2, and T3 states for DMF-BP-DMAC in solid phase. Bond lengths (B1, B2), bond angles (θ1, θ2), and dihedral angles (α1, α2, α3, α4) are marked in Fig. 1(b).

Table 3. Spin–orbit coupling (SOC), reorganization energy (λ), energy difference (ΔE), intersystem crossing rates (KISC), and reverse intersystem crossing rates (KRISC) between single excited states and triplet excited states.

Table 3. Spin–orbit coupling (SOC), reorganization energy (λ), energy difference (ΔE), intersystem crossing rates (KISC), and reverse intersystem crossing rates (KRISC) between single excited states and triplet excited states.

Table 4. Calculated radiative rate (Kr), effective intersystem crossing rates (KISCCal), and effective reverse intersystem crossing rates (KRISCCal).

Table 4. Calculated radiative rate (Kr), effective intersystem crossing rates (KISCCal), and effective reverse intersystem crossing rates (KRISCCal).

Table 3. Spin–orbit coupling (SOC), reorganization energy (λ), energy difference (ΔE), intersystem crossing rates (K_ISC), and reverse intersystem crossing rates (K_RISC) between single excited states and triplet excited states.

Table 3. Spin–orbit coupling (SOC), reorganization energy (λ), energy difference (ΔE), intersystem crossing rates (K_ISC), and reverse intersystem crossing rates (K_RISC) between single excited states and triplet excited states.

Table 4. Calculated radiative rate (K_r), effective intersystem crossing rates ( $K_{ISC}^{Cal}$ ), and effective reverse intersystem crossing rates ( $K_{RISC}^{Cal}$ ).

Table 4. Calculated radiative rate (K_r), effective intersystem crossing rates ( $K_{ISC}^{Cal}$ ), and effective reverse intersystem crossing rates ( $K_{RISC}^{Cal}$ ).