Due to the energy gap law, the direct fabrication of efficient organic afterglow materials with long emission wavelengths at ambient conditions remains challenging. Here, luminescent dopants with moderate k RISC values of 10 0 -10 1 s −1 are designed to harvest triplet energies, simultaneously improving afterglow efficiency and maintaining emission lifetimes >0.1 s. Organic matrices with large dipole moments are selected to populate the triplet excited states of the luminescent dopants and suppress their nonradiative decay and quenching. The dopant-matrix systems exhibit TADF-type organic afterglow with quantum efficiency of 20% to 60% and emission wavelengths exceeding 600 nm. Because of their singlet excited state nature, the TADF-type afterglow emitters can efficiently transfer excited energy to rhodamine B or cyanine 5.5 fluorescence dyes for the construction of red and near-infrared afterglow materials which display promising bioimaging applications.
By
synergizing molecular dynamics and dissipative particle dynamics
simulations, we investigate the assembly of amphiphilic grafted copolymers
into vesicles and the loading/release of doxorubicin hydrochloride
(DOX·HCl). The copolymers, PAE-g-PEGLA, comprise
pH-sensitive poly(β-amino ester) grafted with hydrophilic poly(ethylene
glycol) and hydrophobic poly(d,l-lactide). The vesicle
formation is revealed to follow an aggregation–rearrangement
mechanism, in which small clusters first form, then rearrange, and
finally merge into bilayer-structured vesicles. The vesicle interior
size and membrane thickness are substantially affected by the exchange
quantity and frequency between tetrahydrofuran and water. At pH =
7, DOX·HCl is loaded into the vesicle interior, and the loading
efficiency increases with increasing polymer concentration. At pH
< 7, PAE blocks are protonated and hydrophilic, which causes the
structure transition of membrane thus tuning membrane permeability
for DOX·HCl release. When PLA blocks become longer, vesicle stability
is enhanced and DOX·HCl release is suppressed. To mimic controlled
release, a mixture of two copolymers is proposed, which form hybrid
vesicles and lead to a moderate release rate of DOX·HCl. After
multiple sequential pH variations between acidic and neutral circulatory
environment, DOX·HCl is gradually released from the hybrid vesicles.
This multiscale simulation study identifies the key factors governing
vesicle formation and drug loading/release, and provides bottom-up
insights toward the design and optimization of new amphiphilic polymers
for high-efficacy drug delivery.
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