Abstract
A new methodology of single-component photon upconversion (UC) based on S0-to-T1 (S−T) absorption is demonstrated. Although the S−T absorption is spin-forbidden, modification of anthracene chromophores with heavy bromine atoms allows the direct population of the excited triplets in crystals upon near-infrared (NIR) excitation with incident light intensities of ∼W cm−2. The consequent triplet energy migration (TEM) and triplet-triplet annihilation (TTA) events in crystals lead to blue UC emission with a large anti-Stokes shift over 0.9 eV. The generality of the S−T absorption-based UC is further confirmed with crystals of brominated perylene-derivatives that show a green UC emission under a longer-wavelength NIR excitation (λex=856 nm). The single-component UC with large anti-Stokes shifts observed for brominated aromatic crystals compensates for the shortcomings of conventional two-component solid UC system, i. e., energy losses intrinsic to the intersystem crossing of the sensitizers and the triplet energy transfer from sensitizer to emitter. It offers a simple and complementary UC methodology to the conventional two-photon absorption (TPA) and TTA-UC.
| Original language | English |
|---|---|
| Pages (from-to) | 7597-7601 |
| Number of pages | 5 |
| Journal | ChemistrySelect |
| Volume | 2 |
| Issue number | 25 |
| DOIs | |
| Publication status | Published - Jan 1 2017 |
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All Science Journal Classification (ASJC) codes
- Chemistry(all)
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Sensitizer-Free Photon Upconversion in Single-Component Brominated Aromatic Crystals. / Okumura, Keisuke; Matsuki, Masaya; Yamada, Teppei; Yanai, Nobuhiro; Kimizuka, Nobuo.
In: ChemistrySelect, Vol. 2, No. 25, 01.01.2017, p. 7597-7601.Research output: Contribution to journal › Article
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TY - JOUR
T1 - Sensitizer-Free Photon Upconversion in Single-Component Brominated Aromatic Crystals
AU - Okumura, Keisuke
AU - Matsuki, Masaya
AU - Yamada, Teppei
AU - Yanai, Nobuhiro
AU - Kimizuka, Nobuo
PY - 2017/1/1
Y1 - 2017/1/1
N2 - A new methodology of single-component photon upconversion (UC) based on S0-to-T1 (S−T) absorption is demonstrated. Although the S−T absorption is spin-forbidden, modification of anthracene chromophores with heavy bromine atoms allows the direct population of the excited triplets in crystals upon near-infrared (NIR) excitation with incident light intensities of ∼W cm−2. The consequent triplet energy migration (TEM) and triplet-triplet annihilation (TTA) events in crystals lead to blue UC emission with a large anti-Stokes shift over 0.9 eV. The generality of the S−T absorption-based UC is further confirmed with crystals of brominated perylene-derivatives that show a green UC emission under a longer-wavelength NIR excitation (λex=856 nm). The single-component UC with large anti-Stokes shifts observed for brominated aromatic crystals compensates for the shortcomings of conventional two-component solid UC system, i. e., energy losses intrinsic to the intersystem crossing of the sensitizers and the triplet energy transfer from sensitizer to emitter. It offers a simple and complementary UC methodology to the conventional two-photon absorption (TPA) and TTA-UC.
AB - A new methodology of single-component photon upconversion (UC) based on S0-to-T1 (S−T) absorption is demonstrated. Although the S−T absorption is spin-forbidden, modification of anthracene chromophores with heavy bromine atoms allows the direct population of the excited triplets in crystals upon near-infrared (NIR) excitation with incident light intensities of ∼W cm−2. The consequent triplet energy migration (TEM) and triplet-triplet annihilation (TTA) events in crystals lead to blue UC emission with a large anti-Stokes shift over 0.9 eV. The generality of the S−T absorption-based UC is further confirmed with crystals of brominated perylene-derivatives that show a green UC emission under a longer-wavelength NIR excitation (λex=856 nm). The single-component UC with large anti-Stokes shifts observed for brominated aromatic crystals compensates for the shortcomings of conventional two-component solid UC system, i. e., energy losses intrinsic to the intersystem crossing of the sensitizers and the triplet energy transfer from sensitizer to emitter. It offers a simple and complementary UC methodology to the conventional two-photon absorption (TPA) and TTA-UC.
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U2 - 10.1002/slct.201701769
DO - 10.1002/slct.201701769
M3 - Article
AN - SCOPUS:85041943305
VL - 2
SP - 7597
EP - 7601
JO - ChemistrySelect
JF - ChemistrySelect
SN - 2365-6549
IS - 25
ER -