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1.
Fitoterapia ; : 106043, 2024 May 25.
Article in English | MEDLINE | ID: mdl-38801893

ABSTRACT

Three undescribed phenols, mandshusica C-E (1-3) and a new lignan, mandshusica F (5), along with six known compounds (4, 6-10) were isolated from the roots and rhizomes of Clematis terniflora var. manshurica (Rupr.) Ohwi. Their structures were elucidated by extensive spectroscopic analysis as well as NMR and ECD calculations. Moreover, the possible biosynthetic pathways of compounds 1-3 were also discussed. All compounds were evaluated for their anti-inflammatory activities in LPS-induced RAW 264.7 cells. Compounds 1, 3, 4 significantly reduced the levels of NO and TNF-α, while compounds 2 and 8 significantly inhibited NO production in LPS-induced RAW264.7 cells.

2.
J Colloid Interface Sci ; 666: 560-571, 2024 Jul 15.
Article in English | MEDLINE | ID: mdl-38613978

ABSTRACT

The host lattice environments of Sb3+ has a great influence on its photophysical properties. Here, we synthesized three zero-dimensional organic metal halides of (TPA)2SbCl5 (1), Sb3+-doped (TPA)SnCl5(H2O)·2H2O (Sb3+-2), and Sb3+-doped (TPA)2SnCl6 (Sb3+-3). Compared with the intense orange emission of 1, Sb3+-3 has smaller lattice distortion, thus effectively suppressing the exciton transformation from singlet to triplet self-trapped exciton (STE) states, which makes Sb3+-3 has stronger singlet STE emission and further bring a white emission with a photoluminescence quantum efficiency (PLQE) of 93.4%. Conversely, the non-emission can be observed in Sb3+-2 even though it has a similar [SbCl5]2- structure to 1, which should be due to its indirect bandgap characteristics and the effective non-radiative relaxation caused by H2O in the lattice. Interestingly, the non-emission of Sb3+-2 can convert into the bright emission of Sb3+-3 under TPACl DMF solution treatment. Meanwhile, the white emission under 315 nm excitation of Sb3+-3 can change into orange emission upon 365 nm irradiation, and the luminescence can be further quenched by the treatment of HCl. Therefore, a triple-mode reversible luminescence switch of off-onI-onII-off can be achieved. Finally, we demonstrated the applications of Sb3+-doped compounds in single-component white light illumination, latent fingerprint detection, fluorescent anti-counterfeiting, and information encryption.

3.
Colloids Surf B Biointerfaces ; 237: 113833, 2024 May.
Article in English | MEDLINE | ID: mdl-38484444

ABSTRACT

As a rapid, highly sensitive, and user-friendly technique, surface-enhanced Raman scattering (SERS) has an extraordinary appeal to home self-test of COVID-19 during the post pandemic era. However, most of the existing SERS substrates have been still criticized in stability, repeatability, and sample enrichment. To address these obstacles, a novel non-metallic SERS substrate with porous surfaces and array geometry was developed by in-situ growing ZIF-67 particles on two-dimensional violet phosphorus (VP) matrix. Chemical enhancement was prominently promoted by the synergistic photoinduced charge transfer resonance in the hybrid band structure of the ZIF-67@VP substrate, facilitating a noble metal-similar enhancement factor of 6.11 × 107. The biocompatible ZIF-67@VP porous array with attractive enhancement capability and high anchoring efficiency was further utilized to monitoring SARS-CoV-2 spike protein in practical saliva samples based on a sandwich immunostructure, achieving a limit of detection of 1.7 ng/mL assisted by black phosphorus nanosheets. This nonmetallic immunoassay strategy with exceptional sensitivity and specificity is predicted to extend the utilization of SERS obstacle in daily infectious disease screening.


Subject(s)
COVID-19 , Humans , COVID-19/diagnosis , Porosity , SARS-CoV-2 , Spike Glycoprotein, Coronavirus , Immunoassay , Phosphorus , Spectrum Analysis, Raman
4.
Small ; : e2400045, 2024 Mar 07.
Article in English | MEDLINE | ID: mdl-38453678

ABSTRACT

Emerging photoelectrochemical (PEC) photodetectors (PDs) have notable advantages over conventional PDs and have attracted extensive attention. However, harsh liquid environments, such as those with high corrosivity and attenuation, substantially restrict their widespread application. Moreover, most PEC PDs are constructed by assembling numerous nanostructures on current collector substrates, which inevitably contain abundant interfaces and defects, thus greatly weakening the properties of PDs. To address these challenges, a high-performance pH-universal PEC ultraviolet (UV) PD based on a whole single-crystal integrated self-supporting 4H-SiC nanopore array photoelectrode is constructed, which is fabricated using a two-step anodic oxidation approach. The PD exhibits excellent photodetection behavior, with high responsivity (218.77 mA W-1 ), detectivity (6.64 × 1013  Jones), external quantum efficiency (72.47%), and rapid rise/decay times (17/48 ms) under 375 nm light illumination with a low intensity of 0.15 mW cm-2 and a bias voltage of 0.6 V, which is fall in the state-of-the-art of the wide-bandgap semiconductor-based PDs reported thus far. Furthermore, the SiC PEC PD exhibits excellent photoresponse and long-term operational stability in pH-universal liquid environments. The improved photodetection performance of the SiC PEC PD is primarily attributed to the synergistic effect of the nanopore array structure, integrated self-supporting configuration, and single-crystal structure of the whole photoelectrode.

5.
Mater Horiz ; 11(9): 2230-2241, 2024 May 07.
Article in English | MEDLINE | ID: mdl-38421281

ABSTRACT

Recently, organic Sb(III)-based metal halides have achieved significant results in the visible light region due to their efficient emission. However, realizing efficient broadband near-infrared (NIR) emission in such materials is a great challenge. Herein, we developed three different NIR emitters via a coordination structure modulation strategy in Sb3+-doped zero-dimensional organic metal chlorides of (C20H20P)2MnCl4, (C20H20P)2ZnCl4, and (C20H20P)2CdCl4 with tetrahedral structure. More specifically, after the dopant Sb3+ is inserted into the host lattice, the coordination structures of Sb3+ ions can change from [SbCl5]2- square-pyramidal configuration to [SbCl4]- clusters, which will bring a larger lattice distortion degree to the excited state compared to the ground state, resulting in a larger Stokes shift. Thus, efficient NIR emission with near-unity photoluminescence quantum yield (PLQY) can be obtained in Sb3+-doped compounds under 365 nm excitation. Moreover, Sb3+-doped NIR emitters also show remarkable stabilities, which prompts us to fabricate NIR phosphor conversion light-emitting diodes (pc-LEDs) and demonstrate their application in night vision. More interestingly, the Sb3+-doped (C20H20P)2MnCl4 shows tunable emission characteristics, which can be tuned from green to greenish-yellow, orange, red, and NIR emission under different external stimuli, and thus we can demonstrate the applications of this compound in quintuple-mode fluorescence anti-counterfeiting and information encryption.

6.
ACS Appl Mater Interfaces ; 16(9): 11694-11703, 2024 Mar 06.
Article in English | MEDLINE | ID: mdl-38387044

ABSTRACT

Recently, photodetectors based on perovskite nanoplatelets (NPLs) have attracted considerable attention in the visible spectral region owing to their large absorption cross-section, high exciton binding energy, excellent charge transfer properties, and appropriate flexibility. However, their stability and performance are still challenging for perovskite NPL photodetectors. Here, a surface engineering strategy to enhance the optical stability of blue-light CsPbBr3 NPLs by acetylenedicarboxylic acid (ATDA) treatment has been developed. ATDA has strong binding capacity and a short chain length, which can effectively passivate defects and significantly improve the photoluminescence quantum efficiency, stability, and carrier mobility of NPLs. As a result, ATDA-treated CsPbBr3 NPLs exhibit improved optical properties in both solutions and films. The NPL solution maintains high PL performance even after being heated at 80 °C for 2 h, and the NPL film remains nondegradable after 4 h of exposure to ultraviolet irradiation. Especially, photodetectors based on the treated CsPbBr3 NPL films demonstrate exceptional performance, especially when the detectivity approaches up to 9.36 × 1012 Jones, which can be comparable to the best CsPbBr3 NPL photodetectors ever reported. More importantly, the assembled devices demonstrated high stability (stored in an air environment for more than 30 days), significantly exceeding that of untreated NPLs.

7.
J Phys Chem Lett ; 15(1): 201-211, 2024 Jan 11.
Article in English | MEDLINE | ID: mdl-38157217

ABSTRACT

Indium phosphide (InP) and zinc selenium tellurium (ZnSeTe) quantum dots (QDs) as less toxic alternatives have received substantial attention. The structure of QDs generally consists of a QD core, inner shell layer, and outer shell layer. We reckon that the inner shell layer, especially its components and thickness, have a significant influence on the optical and electronic performances of QDs. In this Perspective, we compare optical properties of these QDs with different inner shells and summarize how typical inner shell components and thickness influence their optical properties. The impact of the inner shell on the performance of QD light-emitting diodes (QLEDs) has also been discussed. The appropriate components and thickness of the inner shell both contribute to alleviate valence or lattice mismatch, thereby enhancing the performance of QDs. We expect that this Perspective could heighten awareness of the significance and impact of the inner shell layer in QDs and facilitate further development of QDs and QLEDs.

8.
J Phys Chem Lett ; 14(51): 11543-11549, 2023 Dec 28.
Article in English | MEDLINE | ID: mdl-38095940

ABSTRACT

Mn2+ doped perovskite nanocrystals have garnered significant attention in optoelectronic applications. However, the synthesis of Mn2+ doped perovskite nanowires (NWs) poses challenges, and the dynamics of energy transfer from the exciton to Mn2+ remains unexplored, which is crucial for optimizing Mn2+ luminescence efficiency. Herein, we present a method to synthesize Mn2+ doped CsPbBr3 NWs with a photoluminescence quantum yield of 52% by diffusing Mn2+ into seed CsPbBr3 NWs grown via a hot injection method. We control the solution and lattice chemical potentials of Pb2+ and Mn2+ to enable Mn2+ to diffuse into the CsPbBr3 NWs while minimizing Ostwald ripening. Variable temperature photoluminescence spectroscopy reveals that the energy transfer from the exciton to Mn2+ in Mn2+ doped CsPbBr3 NWs is temperature dependent. A dynamic competition is observed between energy transfer and backward energy transfer, resulting in stronger Mn2+ photoluminescence at 80 K. This work provides a specific synthesis pathway for Mn2+ doped CsPbBr3 NWs and sheds light on their exciton-to-Mn2+ energy transfer dynamics.

9.
Small ; 19(45): e2303247, 2023 Nov.
Article in English | MEDLINE | ID: mdl-37420332

ABSTRACT

High color purity blue quantum dot light-emitting diodes (QLEDs) have great potential applications in the field of ultra-high-definition display. However, the realization of eco-friendly pure-blue QLEDs with a narrow emission linewidth for high color purity remains a significant challenge. Herein, a strategy for fabricating high color purity and efficient pure-blue QLEDs based on ZnSeTe/ZnSe/ZnS quantum dots (QDs) is presented. It is found that by finely controlling the internal ZnSe shell thickness of the QDs, the emission linewidth can be narrowed by reducing the exciton-longitudinal optical phonon coupling and trap states in the QDs. Additionally, the regulation of the QD shell thickness can suppress the Förster energy transfer between QDs in the QLED emission layer, which will help to reduce the emission linewidth of the device. As a result, the fabricated pure-blue (452 nm) ZnSeTe QLED with ultra-narrow electroluminescence linewidth (22 nm) exhibit high color purity with the Commission Internationale de l'Eclairage chromatic coordinates of (0.148, 0.042) and considerable external quantum efficiency (18%). This work provides a demonstration of the preparation of pure-blue eco-friendly QLEDs with both high color purity and efficiency, and it is believed that it will accelerate the application process of eco-friendly QLEDs in ultra-high-definition displays.

10.
ACS Appl Mater Interfaces ; 15(27): 33087-33094, 2023 Jul 12.
Article in English | MEDLINE | ID: mdl-37364060

ABSTRACT

Ion migration and phase separation in perovskite materials have negatively affected the solid-state lighting and display. Studying photo- and thermal-induced degradation is considered as a promising approach to understanding the luminescence mechanism and promoting practical applications. Herein, the Mn-doped two-dimensional PEA2PbX4 (X = Cl, Br, I) microcrystals with changing halogen composition were synthesized by an acid-assisted post-processing strategy. Then, photo- and thermal-induced degradation was studied by using steady-state and time-resolved photoluminescence (PL) spectroscopy. The band edge exciton PL peak of Mn-doped 2D PEA2PbX4 microcrystals was adjusted from 397 to 500 nm. The reduced Mn PL lifetime (1.37 to 0.21 ms) was monitored under ion exchange from Cl to Br to I. The degradation mechanism could be divided into two cases: (i) The halide ion migration in Mn-doped 2D perovskite under continuous illumination was revealed, suggesting that the migration of Cl ions was more accessible than that of Br and I. (ii) The PL redshift and lifetime reduction were observed after annealing at 420 K, which means that thermally induced aggregation of Mn ions resulted in the formation of Mn2+-Mn2+ dimers. In addition, the experimental results indicated that the induced B-site phase separation at high temperature annealing made the mixed perovskite phase of Pb and Mn ultimately transform into pure PEA2PbBr4 and PEA2MnBr4.

11.
Mater Horiz ; 10(3): 960-966, 2023 Mar 06.
Article in English | MEDLINE | ID: mdl-36606592

ABSTRACT

Dual-band electrochromic smart windows (DESWs) can selectively control the transmittance of near-infrared (NIR) and visible (VIS) light, which can significantly reduce building energy consumption. However, almost all the reported DESW colors switch between clear colorless and dark blue. The single color combined with the dazzling visual experience of blue will undoubtedly limit the application scene of DESWs. Herein, for the first time, we report a robust and stable DESW with multicolor conversion capabilities based on the single-component organic polymer polyaniline (PANI). The results show that the progressive electrochemical reaction enabled PANI film to deliver not only efficient and independent control of NIR and VIS light transmittance but also impressive electrochromic performance-rich color conversion (yellow-green-black), good optical modulation (65% at 633 nm and 59% at 1600 nm), high coloration efficiency (367.1 cm2 C-1 at 633 nm and 299.6 cm2 C-1 at 1600 nm), and excellent cycling stability (optical modulation losses of 6% at 633 nm, and 4% at 1600 nm after 10 000 cycles). Thereby, we demonstrated a prototype PANI-based DESW device (10 × 5 cm2), which delivered a multicolor electrochromism together with independent control and modulation of the VIS (sunlight) and NIR (solar heat) transmittance.

12.
ACS Appl Mater Interfaces ; 14(40): 45725-45733, 2022 Oct 12.
Article in English | MEDLINE | ID: mdl-36190450

ABSTRACT

Two-dimensional (2D) hybrid layered perovskites (HLPs) have attracted extensive attention due to their excellent optoelectronic properties. Herein, we successfully prepared high-quality Mn-doped BDACdBr4 (BDA = NH2(CH2)4NH2, butylene diammonium) HLP single crystals (SCs). The incorporation of Mn2+ ions modulates the electronic band structure of BDACdBr4 perovskites and tailors the energy transfer process of excited states. A near-unity photoluminescence (PL) quantum yield of 96% from the Mn2+ emission at 608 nm is achieved. Excitation wavelength-dependent spectroscopic characterizations help to clarify the energy transfer mechanism of Mn-doped BDACdBr4, in which competing PL from the 3Eg → 1A1g transition of Cd2+ and the 4T1(G) → 6A1(S) transition of Mn2+ dopants is observed. Temperature-dependent PL spectroscopic characterizations indicate that the efficient energy transfer from BDACdBr4 perovskite host to Mn2+ dopants requires thermal activation to overcome a potential barrier. This work provides new insight into the photophysics and optical properties of 2D HLPs, especially the influence of Mn2+ doping on competing energy transfer in hybrid luminescent materials.

13.
J Phys Chem Lett ; 13(31): 7177-7184, 2022 Aug 11.
Article in English | MEDLINE | ID: mdl-35904436

ABSTRACT

Low-dimensional metal halides are attractive for applications in photodetectors, solid-state lighting, and solar cells, but poor stability is an obstacle that must be overcome in commercial applications. Herein, we successfully synthesized a Ruddlesden-Popper (RP)-phased perovskite Mn2+:Cs3Cd2Cl7 with high photoluminescence quantum yield (PLQY) and outstanding thermal and environmental stability by a solvothermal method. The pristine sample Cs3Cd2Cl7 exhibits a weak cyan broad emission centered at 510 nm with a low PLQY of ∼4%. Once Mn2+ ions are introduced into the host lattice, a bright orange emission peaking at 580 nm with a high PLQY of ∼74% was achieved, which is attributed to the efficient energy transfer from the host to Mn2+ ions and thus results in the 4T1 → 6A1 radiation transition of Mn2+ ions. The photoluminescence (PL) intensity and environmental stability of Mn2+:Cs3Cd2Cl7 can be further improved through A-site Rb alloying. Finally, an orange LED with outstanding color stability was fabricated on the basis of the Mn2+:Cs3Cd2Cl7. Our work successfully elucidates that dopant plays an integral role in tailoring optical properties.

14.
Light Sci Appl ; 11(1): 162, 2022 May 30.
Article in English | MEDLINE | ID: mdl-35637219

ABSTRACT

InP-based quantum dot light-emitting diodes (QLEDs), as less toxic than Cd-free and Pb-free optoelectronic devices, have become the most promising benign alternatives for the next generation lighting and display. However, the development of green-emitting InP-based QLEDs still remains a great challenge to the environmental preparation of InP quantum dots (QDs) and superior device performance. Herein, we reported the highly efficient green-emitting InP-based QLEDs regulated by the inner alloyed shell components. Based on the environmental phosphorus tris(dimethylamino)phosphine ((DMA)3P), we obtained highly efficient InP-based QDs with the narrowest full width at half maximum (~35 nm) and highest quantum yield (~97%) by inserting the gradient inner shell layer ZnSexS1-x without further post-treatment. More importantly, we concretely discussed the effect and physical mechanism of ZnSexS1-x layer on the performance of QDs and QLEDs through the characterization of structure, luminescence, femtosecond transient absorption, and ultraviolet photoelectron spectroscopy. We demonstrated that the insert inner alloyed shell ZnSexS1-x provided bifunctionality, which diminished the interface defects upon balancing the lattice mismatch and tailored the energy levels of InP-based QDs which could promote the balanced carrier injection. The resulting QLEDs applying the InP/ZnSe0.7S0.3/ZnS QDs as an emitter layer exhibited a maximum external quantum efficiency of 15.2% with the electroluminescence peak of 532 nm, which was almost the highest record of InP-based pure green-emitting QLEDs. These results demonstrated the applicability and processability of inner shell component engineering in the preparation of high-quality InP-based QLEDs.

15.
J Phys Chem Lett ; 13(21): 4701-4709, 2022 Jun 02.
Article in English | MEDLINE | ID: mdl-35608371

ABSTRACT

Despite recent advances in producing perovskite-nanocrystals-in-glass (PNG) for display application, it remains challenging to achieve ultrapure and large-area CsPbBr3 PNG-based flexible films with tunable green emission. Herein, we report a facile strategy to produce flexible film containing CsPbBr3 PNG. Specifically, the achievement of CsPbBr3 PNG with tunable green emissions (517-528 nm) is realized by elaborate regulation of the glass precursor concentration and thermal treatment temperature by an in situ growth method. With the integration of red-light-emitting CsPbBrxI3-x PNG powder, the color gamut of as-prepared white-light-emitting sources can cover up to 126.27% of the NTSC 1953 standard and 93.9% of the Rec. 2020 standard. Notably, flexible and large-area white-light-emitting films can be readily obtained by sandwiching and gluing mixed PNG powders between two layers of hydrophobic and transparent PET films. Intriguingly, as-prepared PNG films exhibit excellent hydrothermal, photostability, and long-term operation stability, making them promising for practical ultrahigh-definition displays.

16.
J Phys Chem Lett ; 13(16): 3682-3690, 2022 Apr 28.
Article in English | MEDLINE | ID: mdl-35438490

ABSTRACT

The rich phase structures of perovskite derivatives have attracted extensive attention and can be applied in the fields of optoelectronics due to their high emission efficiency and tunable emission. Herein, we explored a phase-selective solution synthetic route to obtain different Cd-based perovskite derivatives. First, the pristine tetragonal Cs7Cd3Br13 was obtained by a solvothermal method, and its photoluminescence quantum yield (PLQY) was boosted from 8.28% to 57.62% after appropriate Sb3+ doping. Furthermore, halogen substitution was adopted to modify Sb:Cs7Cd3Br13 and produced a series of Cd-based perovskite derivatives with different crystal structures and tunable emission from cyan to orange (517-625 nm). The mechanisms behind such experimental phenomena were further investigated and discussed on the basis of material characterization and theoretical computation. This study presented an effective strategy to synthesize bright Cd-based perovskite derivatives with different structures and modulated emission, and it also provided insights to understand the structure/emission modulation via halogen substitution.

17.
J Phys Chem Lett ; 13(13): 2878-2884, 2022 Apr 07.
Article in English | MEDLINE | ID: mdl-35333050

ABSTRACT

A modified Langevin model has been proposed to study the electronic and excitonic dynamic processes in quantum dot light-emitting diodes (QLEDs), and the electroluminescence onset processes of the QLEDs under different charge-injection conditions have been explored. The simulation results are in good agreement with experimental curves, confirming the feasibility of this model. It is demonstrated that the formation of an exciton on the quantum dots (QDs) with one electron injected first followed by one hole is much more effective than that with the reverse sequence. That is, charging a QD with one electron first is more favorable for device performance enhancement, which is attributed to the low (high) Auger recombination rate of negative (positive) trions of commonly used type I QDs. Additionally, we demonstrate that enough electron injection is one of the prerequisites for high-performance QLEDs based on these type I QDs.

18.
Inorg Chem ; 61(3): 1486-1494, 2022 Jan 24.
Article in English | MEDLINE | ID: mdl-34982544

ABSTRACT

Controlling the structure of halide perovskites through component engineering, and thus revealing the changes in luminescence properties caused by the conversion of crystal structure, is of great significance. Herein, we report a controllable synthetic strategy of three-dimensional (3D) Cs2KInCl6 and zero-dimensional (0D) (Cs/K)2InCl5(H2O) halide perovskites by changing the Cs/K feed ratio. 3D Cs2KInCl6 double perovskites are obtained at the Cs/K feed ratio of 1:1, while 0D (Cs/K)2InCl5(H2O) perovskites are formed at the Cs/K feed ratio of 2:1. Further, a reversible crystal structure transformation between 3D Cs2KInCl6 double perovskites and 0D (Cs/K)2InCl5(H2O) perovskites can be achieved by subsequent addition of metal-salt precursors. In addition, the emission efficiency of two perovskite structures can be greatly boosted by breaking the forbidden transition through Sb doping, and as a result, a novel green/yellow reversible emission switch is generated. Meanwhile, the relationship between perovskite structure and luminescence mechanism has been systematically revealed. These environmentally stable halide perovskites have great potential to be applied in optoelectronic devices.

19.
Opt Mater (Amst) ; 1232022 Jan.
Article in English | MEDLINE | ID: mdl-35068693

ABSTRACT

Mn-doped I(II)-III-VI NCs (e.g., Mn-doped AgZnInS/ZnS NCs) possessing low-energy excitation, high brightness and long fluorescence lifetimes have been desired for time-gated fluorescence biosensing/imaging. In this type of NCs, their optical properties are significantly affected by the microscopic interactions between Mn and Mn and between Mn and host NC, the compositions of NCs, and the defects in NCs. On the other hand, it is known that Zn etching to core I(II)-III-VI NCs in NC synthesis can significantly enhance the NC brightness because Zn can exchange surface atoms (e.g., Ag and In) in NCs to minimize NC surface-defects. But for Mn-doped I(II)-III-VI NCs, Zn etching could etch out not only surface-atoms of host NCs (e.g., Ag and In) but also Mn in NCs. As a result, it could significantly affect the NC compositions and the microscopic interactions between Mn and Mn as well as between Mn and host NC, and thus the optical properties of NCs (like lifetime and absorption/emission spectra). Therefore, it is needed to investigate how Zn etching would affect the optical properties of such Mn-doped NCs. In this study, a series of Mn-doped AgZnInS NCs with different Mn doping levels were prepared through nucleation doping, and then Zn etching was applied to etch these core NCs. To identify the effects of Zn etching on NC optical properties, ZnS coating (a different ZnS shelling approach by injecting Zn precursor and S precursor alternately in synthesis) was performed on the same Mn:AgZnInS NCs, and the optical properties of NCs with these two different ZnS shelling approaches were compared. Experimental results showed that under appropriate Mn doping levels in synthesis, Zn etching instead of ZnS coating can produce low-energy excitable NCs with higher QYs and longer lifetimes, which would further facilitate the use of such NCs in time-gated fluorescence measurement. To understand the reasons for the different optical properties under different ZnS shelling approaches, the material characteristics of the prepared NCs were further measured/analyzed and the possible fluorescence mechanisms were discussed.

20.
ACS Appl Nano Mater ; 5(12): 17413-17435, 2022 Dec 23.
Article in English | MEDLINE | ID: mdl-36874078

ABSTRACT

Colloidal semiconductor nanocrystals (NCs) have been developed for decades and are widely applied in biosensing/imaging. However, their biosensing/imaging applications are mainly based on luminescence-intensity measurement, which suffers from autofluorescence in complex biological samples and thus limits the biosensing/imaging sensitivities. It is expected for these NCs to be further developed to gain luminescence features that can overcome sample autofluorescence. On the other hand, time-resolved luminescence measurement utilizing long-lived-luminescence probes is an efficient technique to eliminate short-lived autofluorescence of samples while recording time-resolved luminescence of the probes for signal measurement after pulsed excitation from a light source. Despite time-resolved measurement being very sensitive, the optical limitations of many of the current long-lived-luminescence probes cause time-resolved measurement to be generally performed in laboratories with bulky and costly instruments. In order to apply highly sensitive time-resolved measurement for in-field or point-of-care (POC) testing, it is essential to develop probes possessing high brightness, low-energy (visible-light) excitation, and long lifetimes of up to milliseconds. Such desired optical features can significantly simplify the design criteria of time-resolved measurement instruments and facilitate the development of low-cost, compact, sensitive instruments for in-field or POC testing. Mn-doped NCs have recently been in rapid development and provide a strategy to solve the challenges faced by both colloidal semiconductor NCs and time-resolved luminescence measurement. In this review, we outline the major achievements in the development of Mn-doped binary and multinary NCs, with emphasis on their synthesis approaches and luminescence mechanisms. Specifically, we demonstrate how researchers approached these obstacles to achieve the aforementioned desired optical properties on the basis of the progressive understanding of Mn emission mechanisms. Afterward, we review representative applications of Mn-doped NCs in time-resolved luminescence biosensing/imaging and present the potential of Mn-doped NCs in advancing time-resolved luminescence biosensing/imaging for in-field or POC testing.

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