Nitroreductase (NTR) can be overexpressed in hypoxic tumors, thus the selective and efficient detection of NTR is of great importance. To date, although a few optical methods have been reported for the detection of NTR in solution, an effective optical probe for NTR monitoring in vivo is still lacking. Therefore, it is necessary to develop a near-infrared (NIR) fluorescent detection probe for NTR. In this study, five NIR cyanine dyes with fluorescence reporting structure decorated with different nitro aromatic groups, Cy7-1-5, have been designed and explored for possible rapid detection of NTR. Our experimental results presented that only a para-nitro benzoate group modified cyanine probe (Cy7-1) could serve as a rapid NIR fluorescence-enhanced probe for monitoring and bioimaging of NTR. The structure-function relationship has been revealed by theoretical study. The linker connecting the detecting and fluorescence reporting groups and the nitro group position is a key factor for the formation of hydrogen bonds and spatial structure match, inducing the NTR catalytic ability enhancement. The in vitro response and mechanism of the enzyme-catalyzed reduction of Cy7-1 have been investigated through kinetic optical studies and other methods. The results have indicated that an electro-withdrawing group induced electron-transfer process becomes blocked when Cy7-1 is catalytically reduced to Cy7-NH2 by NTR, which is manifested in enhanced fluorescence intensity during the detection process. Confocal fluorescence imaging of hypoxic A549 cells has confirmed the NTR detection ability of Cy7-1 at the cellular level. Importantly, Cy7-1 can detect tumor hypoxia in a murine hypoxic tumor model, showing a rapid and significant enhancement of its NIR fluorescence characteristics suitable for fluorescence bioimaging. This method may potentially be used for tumor hypoxia diagnosis.
Clean energy production and saving play vital impacts on the sustainability of the global community. Herein, high‐performance semitransparent organic solar cells (ST‐OSCs) with excellent features of power generation, being see‐through, and infrared reflection of heat dissipation, with promising perspectives for building‐integrated photovoltaics (BIPVs) are reported. To simultaneously improve average visible transmittance (AVT) and power conversion efficiency (PCE), formally in a trade‐off relationship, of ST‐OSCs, new ternary blends with alloy‐like near‐infrared (NIR) acceptors are employed, which are effective to improve device efficiency while maintaining visible absorption unchanged, resulting in PCEs of 16.8% for opaque devices and 13.1% for semitransparent OSCs (AVT of 22.4% and infrared photon radiation rejection (IRR) of 77%). Further, multifunctional ST‐OSCs are realized via introducing simple, yet effective photonic reflectors, together with optical simulation, leading to not only perfect fitting of the visible transmittance peak (555 nm) to the photopic response of the human eye but also an excellent IRR of 90% (780–2500 nm), along with 23% AVT and over 12% PCE. This is thought to be the best‐performing multifunctional ST‐OSC with promising prospects as BIPVs in terms of power generation, heat dissipation, and being see‐through.
Four new heteroleptic cationic Ir(III) complexes bearing benzothiazolylfluorene motif on the bipyridine (N∧N) (1 and 2) and phenylpyridine (C∧N) (3 and 4) ligands are synthesized and characterized. The influence of the position of the substituent and the extent of π-conjugation on the photophysics of these complexes is systematically investigated by spectroscopic methods and simulated by time-dependent density functional theory (TDDFT). The complexes exhibit ligand-centered (1)π,π* transitions with admixtures of (1)ILCT (π(benzothiazolylfluorene) → π*(bpy)) and (1)MLCT (metal-to-ligand charge transfer) characters below 475 nm, and very weak (1,3)MLCT and (1,3)LLCT (ligand-to-ligand charge transfer) transitions above 475 nm. The emission of these complexes at room temperature in CH2Cl2 solutions is ascribed to be predominantly from the (3)MLCT/(3)LLCT states for 1 and from the (3)π,π* state for 2, while the emitting state of 3 and 4 are assigned to be an admixture of (3)MLCT, (3)LLCT, and (3)π,π* characters. The variations of the photophysical properties of 1-4 are attributed to different degrees of π-conjugation in the bipyridine and phenylpyridine ligands induced by different positions of the benzothiazolylfluorenyl substituents on the bipyridine ligand and different extents of π-conjugation in the phenylpyridine ligands, which alters the energy and lifetime of the lowest singlet and triplet excited states. 1-4 all possess broadband transient absorption (TA) upon nanosecond laser excitation, which extends from the visible to the NIR region. Therefore, 1-4 all exhibit strong reverse saturable absorption (RSA) at 532 nm for ns laser pulses. However, the TA of complexes 1, 2, and 3 are much stronger than that of 4. This feature, combined with the difference in ground-state absorption and triplet excited-state quantum yield, result in the difference in RSA strength, which follows this trend: 1 ≈ 2 ≈ 3 > 4. Therefore, complexes 1-3 are strong reverse saturable absorbers at 532 nm and could potentially be used as broadband nonlinear absorbing materials.
Mixed perovskites have achieved substantial successes in boosting solar cell efficiency, but the complicated perovskite crystal formation pathway remains mysterious. Here, the detailed crystallization process of mixed perovskites (FA0.83MA0.17Pb(I0.83Br0.17)3) during spin‐coating is revealed by in situ grazing‐incidence wide‐angle X‐ray scattering measurements, and three phase‐formation stages are identified: I) precursor solution; II) hexagonal δ‐phase (2H); and III) complex phases including hexagonal polytypes (4H, 6H), MAI–PbI2–DMSO intermediate phases, and perovskite α‐phase. The correlated device performance and ex situ characterizations suggest the existence of an “annealing window” covering the duration of stage II. The spin‐coated film should be annealed within the annealing window to avoid the formation of hexagonal polytypes during the perovskite crystallization process, thus achieving a good device performance. Remarkably, the crystallization pathway can be manipulated by incorporating Cs+ ions in mixed perovskites. Combined with density functional theory calculations, the perovskite system with sufficient Cs+ will bypass the formation of secondary phases in stage III by promoting the formation of α‐phase both kinetically and thermodynamically, thereby significantly extending the annealing window. This study provides underlying reasons of the time sensitivity of fabricating mixed‐perovskite devices and insightful guidelines for manipulating the perovskite crystallization pathways toward higher performance.
Enhancing the luminescence property without sacrificing the charge collection is one key to high-performance organic solar cells (OSCs), while limited by the severe non-radiative charge recombination. Here, we demonstrate efficient OSCs with high luminescence via the design and synthesis of an asymmetric non-fullerene acceptor, BO-5Cl. Blending BO-5Cl with the PM6 donor leads to a record-high electroluminescence external quantum efficiency of 0.1%, which results in a low non-radiative voltage loss of 0.178 eV and a power conversion efficiency (PCE) over 15%. Importantly, incorporating BO-5Cl as the third component into a widely-studied donor:acceptor (D:A) blend, PM6:BO-4Cl, allows device displaying a high certified PCE of 18.2%. Our joint experimental and theoretical studies unveil that more diverse D:A interfacial conformations formed by asymmetric acceptor induce optimized blend interfacial energetics, which contributes to the improved device performance via balancing charge generation and recombination.
Polymerization sites of small molecule acceptors (SMAs) play vital roles in determining device performance of all-polymer solar cells (all-PSCs). Different from our recent work about fluoro-and bromo-co-modified end group of IC-FBr (a mixture of IC-FBr1 and IC-FBr2), in this paper,w e synthesized and purified two regiospecific fluoro-and bromosubstituted end groups (IC-FBr-o &I C-FBr-m), which were then employed to construct two regio-regular polymer acceptors named PYF-T-o and PYF-T-m, respectively.Incomparison with its isomeric counterparts named PYF-T-m with different conjugated coupling sites,P YF-T-o exhibits stronger and bathochromic absorption to achieve better photon harvesting. Meanwhile,PYF-T-o adopts more ordered inter-chain packing and suitable phase separation after blending with the donor polymer PM6, which resulted in suppressed charge recombination and efficient charge transport. Strikingly,w eo bserved ad ramatic performance difference between the two isomeric polymer acceptors PYF-T-o and PYF-T-m. While devices based on PM6:PYF-T-o can yield power conversion efficiency (PCE) of 15.2 %, devices based on PM6:PYF-T-m only show poor efficiencies of 1.4 %. This work demonstrates the success of configuration-unique fluorinated end groups in designing high-performance regular polymer acceptors,w hich provides guidelines towardsdeveloping all-PSCs with better efficiencies.
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