TY - JOUR
T1 - Manipulating nonradiative decay channel by intermolecular charge transfer for exceptionally improved photothermal conversion
AU - Hu, Wenbo
AU - Miao, Xiaofei
AU - Tao, Haojie
AU - Baev, Alexander
AU - Ren, Can
AU - Fan, Quli
AU - He, Tingchao
AU - Huang, Wei
AU - Prasad, Paras N.
N1 - Publisher Copyright:
Copyright © 2019 American Chemical Society.
PY - 2019/10/22
Y1 - 2019/10/22
N2 - In-depth studies of nonradiative (NR) decay, seeking to maximize NR decay rate or manipulate other NR decay channels, are of greatest significance for improving the photothermal conversion efficiency (Ε) of organic materials for phototheranostics; however, to date, relevant work remains scarce. Here, we present an insightful study of NR decay in BODIPY (BDP) dye, in an aggregated state, i.e., in BDP nanoparticles (BDP NPs), which show an efficient additional NR decay channel from the aggregation-stabilized intermolecular charge transfer (CT) state, resulting in exceptionally high Ε (61%) for highly efficient phototheranostics in vivo. BDP NPs exhibit two ultrafast NR decay channels with ultrashort lifetimes of 1.7 and 50 ps, which is in stark contrast to the only S1 → S0 NR channel with a long lifetime of 373 ps in the isolated BDP dye. More importantly, the ultrafast NR channel (1.7 ps) in BDP NPs depletes a substantial portion of the excited-state population (71%), which accounts for its much better photothermal effect as compared with the isolated BDP dye. Finally, BDP NPs display a highly efficient photoacoustic imaging (PAI) guided photothermal therapy (PTT) of tumors in live mice. This study presents a deeper fundamental understanding of NR decay in organic materials, setting a valuable guideline that may be widely applicable to similar molecular structure to develop more advanced organic materials not only for photothermal-related applications.
AB - In-depth studies of nonradiative (NR) decay, seeking to maximize NR decay rate or manipulate other NR decay channels, are of greatest significance for improving the photothermal conversion efficiency (Ε) of organic materials for phototheranostics; however, to date, relevant work remains scarce. Here, we present an insightful study of NR decay in BODIPY (BDP) dye, in an aggregated state, i.e., in BDP nanoparticles (BDP NPs), which show an efficient additional NR decay channel from the aggregation-stabilized intermolecular charge transfer (CT) state, resulting in exceptionally high Ε (61%) for highly efficient phototheranostics in vivo. BDP NPs exhibit two ultrafast NR decay channels with ultrashort lifetimes of 1.7 and 50 ps, which is in stark contrast to the only S1 → S0 NR channel with a long lifetime of 373 ps in the isolated BDP dye. More importantly, the ultrafast NR channel (1.7 ps) in BDP NPs depletes a substantial portion of the excited-state population (71%), which accounts for its much better photothermal effect as compared with the isolated BDP dye. Finally, BDP NPs display a highly efficient photoacoustic imaging (PAI) guided photothermal therapy (PTT) of tumors in live mice. This study presents a deeper fundamental understanding of NR decay in organic materials, setting a valuable guideline that may be widely applicable to similar molecular structure to develop more advanced organic materials not only for photothermal-related applications.
KW - Charge transfer
KW - J-dimers
KW - nonradiative decay
KW - Organic nanoparticles
KW - Photothermal therapy
UR - http://www.scopus.com/inward/record.url?scp=85072992171&partnerID=8YFLogxK
U2 - 10.1021/acsnano.9b06208
DO - 10.1021/acsnano.9b06208
M3 - 文章
C2 - 31518102
AN - SCOPUS:85072992171
SN - 1936-0851
VL - 13
SP - 12006
EP - 12014
JO - ACS Nano
JF - ACS Nano
IS - 10
ER -