Revealing the marked differences of phosphorescence efficiencies on C˄N˄N‐coordinated Pt(II) complexes: A theoretical study
In this study, green phosphorescent Pt(II) complexes with N,N‐diphenyl‐6‐(1H‐pyrazol‐1‐yl)pyridin‐2‐amine (Ndpp) coordinated ligands, [Pt (Ndpp)Cl] 2a, [Pt (Ndpp)Pb, Pb = (prop‐1‐ynyl)benzene] 2b, and [Pt (Ndpp)CN] 2aCN were theoretically investigated by means of density functional theory and time‐...
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Published in | Applied organometallic chemistry Vol. 35; no. 1 |
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Abstract | In this study, green phosphorescent Pt(II) complexes with N,N‐diphenyl‐6‐(1H‐pyrazol‐1‐yl)pyridin‐2‐amine (Ndpp) coordinated ligands, [Pt (Ndpp)Cl] 2a, [Pt (Ndpp)Pb, Pb = (prop‐1‐ynyl)benzene] 2b, and [Pt (Ndpp)CN] 2aCN were theoretically investigated by means of density functional theory and time‐dependent density functional theory calculations to reveal their marked distinct phosphorescence quantum yields. These complexes exhibit evident absorption bands in the 200–450 nm region but emit strong green light with marked differences of phosphorescence quantum yields. Compared with the complex 2a, the complex 2b possesses large oscillator strengths of absorption spectra, strong spin‐orbit coupling, and transition electric dipole moment, as well as small singlet‐triplet splitting energies, which conduces to enhancing its radiative decay. To illustrate the nonradiative decay process, the transition state (TS) between the triplet metal‐centered (3MC) state and the excited state (T1) was optimized. The 3MC state is found to be the minimum energy crossing point (MECP) between the T1 state and the S0 state. Compared with the complex 2a, the complex 2b possesses a much larger energy barrier to the MECP state from the T1 state, so it is strongly emissive in the green region. Besides, the introduction of CN substitutions on 2a is useful for enhancing the energy barrier to the thermal deactivation pathway of 3MLCT → TS → MECP. These results demonstrate that the modification of metal–ligand conjugation is an effective way to develop high‐performance phosphorescent materials.
The effect of cyclometalated ligand on Фem was theoretically analyzed. Complex 2b and 2aCN possesses a much larger energy barrier to the MECP state from the T1 state relative to 2b, so they strongly emissive in the green region. |
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AbstractList | In this study, green phosphorescent Pt(II) complexes with N,N‐diphenyl‐6‐(1H‐pyrazol‐1‐yl)pyridin‐2‐amine (Ndpp) coordinated ligands, [Pt (Ndpp)Cl]
2a
, [Pt (Ndpp)Pb, Pb = (prop‐1‐ynyl)benzene]
2b
, and [Pt (Ndpp)CN]
2aCN
were theoretically investigated by means of density functional theory and time‐dependent density functional theory calculations to reveal their marked distinct phosphorescence quantum yields. These complexes exhibit evident absorption bands in the 200–450 nm region but emit strong green light with marked differences of phosphorescence quantum yields. Compared with the complex
2a
, the complex
2b
possesses large oscillator strengths of absorption spectra, strong spin‐orbit coupling, and transition electric dipole moment, as well as small singlet‐triplet splitting energies, which conduces to enhancing its radiative decay. To illustrate the nonradiative decay process, the transition state (TS) between the triplet metal‐centered (
3
MC) state and the excited state (
T
1
) was optimized. The
3
MC state is found to be the minimum energy crossing point (MECP) between the
T
1
state and the
S
0
state. Compared with the complex
2a
, the complex
2b
possesses a much larger energy barrier to the MECP state from the
T
1
state, so it is strongly emissive in the green region. Besides, the introduction of
CN
substitutions on
2a
is useful for enhancing the energy barrier to the thermal deactivation pathway of
3
MLCT → TS → MECP. These results demonstrate that the modification of metal–ligand conjugation is an effective way to develop high‐performance phosphorescent materials. In this study, green phosphorescent Pt(II) complexes with N,N‐diphenyl‐6‐(1H‐pyrazol‐1‐yl)pyridin‐2‐amine (Ndpp) coordinated ligands, [Pt (Ndpp)Cl] 2a, [Pt (Ndpp)Pb, Pb = (prop‐1‐ynyl)benzene] 2b, and [Pt (Ndpp)CN] 2aCN were theoretically investigated by means of density functional theory and time‐dependent density functional theory calculations to reveal their marked distinct phosphorescence quantum yields. These complexes exhibit evident absorption bands in the 200–450 nm region but emit strong green light with marked differences of phosphorescence quantum yields. Compared with the complex 2a, the complex 2b possesses large oscillator strengths of absorption spectra, strong spin‐orbit coupling, and transition electric dipole moment, as well as small singlet‐triplet splitting energies, which conduces to enhancing its radiative decay. To illustrate the nonradiative decay process, the transition state (TS) between the triplet metal‐centered (3MC) state and the excited state (T1) was optimized. The 3MC state is found to be the minimum energy crossing point (MECP) between the T1 state and the S0 state. Compared with the complex 2a, the complex 2b possesses a much larger energy barrier to the MECP state from the T1 state, so it is strongly emissive in the green region. Besides, the introduction of CN substitutions on 2a is useful for enhancing the energy barrier to the thermal deactivation pathway of 3MLCT → TS → MECP. These results demonstrate that the modification of metal–ligand conjugation is an effective way to develop high‐performance phosphorescent materials. The effect of cyclometalated ligand on Фem was theoretically analyzed. Complex 2b and 2aCN possesses a much larger energy barrier to the MECP state from the T1 state relative to 2b, so they strongly emissive in the green region. In this study, green phosphorescent Pt(II) complexes with N,N‐diphenyl‐6‐(1H‐pyrazol‐1‐yl)pyridin‐2‐amine (Ndpp) coordinated ligands, [Pt (Ndpp)Cl] 2a, [Pt (Ndpp)Pb, Pb = (prop‐1‐ynyl)benzene] 2b, and [Pt (Ndpp)CN] 2aCN were theoretically investigated by means of density functional theory and time‐dependent density functional theory calculations to reveal their marked distinct phosphorescence quantum yields. These complexes exhibit evident absorption bands in the 200–450 nm region but emit strong green light with marked differences of phosphorescence quantum yields. Compared with the complex 2a, the complex 2b possesses large oscillator strengths of absorption spectra, strong spin‐orbit coupling, and transition electric dipole moment, as well as small singlet‐triplet splitting energies, which conduces to enhancing its radiative decay. To illustrate the nonradiative decay process, the transition state (TS) between the triplet metal‐centered (3MC) state and the excited state (T1) was optimized. The 3MC state is found to be the minimum energy crossing point (MECP) between the T1 state and the S0 state. Compared with the complex 2a, the complex 2b possesses a much larger energy barrier to the MECP state from the T1 state, so it is strongly emissive in the green region. Besides, the introduction of CN substitutions on 2a is useful for enhancing the energy barrier to the thermal deactivation pathway of 3MLCT → TS → MECP. These results demonstrate that the modification of metal–ligand conjugation is an effective way to develop high‐performance phosphorescent materials. |
Author | Ren, Xue‐Feng Liu, Xia Li, Ke Kang, Guo‐Jun |
Author_xml | – sequence: 1 givenname: Xue‐Feng orcidid: 0000-0003-2116-4007 surname: Ren fullname: Ren, Xue‐Feng organization: China University of Mining and Technology – sequence: 2 givenname: Xia surname: Liu fullname: Liu, Xia organization: China University of Mining and Technology – sequence: 3 givenname: Guo‐Jun surname: Kang fullname: Kang, Guo‐Jun email: gjkang@cumt.edu.cn organization: China University of Mining and Technology – sequence: 4 givenname: Ke surname: Li fullname: Li, Ke organization: China University of Mining and Technology |
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Snippet | In this study, green phosphorescent Pt(II) complexes with N,N‐diphenyl‐6‐(1H‐pyrazol‐1‐yl)pyridin‐2‐amine (Ndpp) coordinated ligands, [Pt (Ndpp)Cl] 2a, [Pt... In this study, green phosphorescent Pt(II) complexes with N,N‐diphenyl‐6‐(1H‐pyrazol‐1‐yl)pyridin‐2‐amine (Ndpp) coordinated ligands, [Pt (Ndpp)Cl] 2a , [Pt... |
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SubjectTerms | 3MC Absorption spectra Benzene Chemistry Conjugation Decay Density functional theory Dipole moments Electric dipoles Ligands MECP Oscillator strengths Phosphorescence phosphorescence quantum yields |
Title | Revealing the marked differences of phosphorescence efficiencies on C˄N˄N‐coordinated Pt(II) complexes: A theoretical study |
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