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1.
Recently synthesized small molecule tellurophenes containing ring-appended pinacolboronate (BPin) side groups possess remarkable guest-free air-stable solid-state phosphorescence, structure-based color-tunability and aggregation induced enhanced emission. The charge transport, doping and luminescence behavior of thin transparent films of a tellurophene with BPin groups positioned at the 2,5-positions (B-Te-6-B) was investigated. Film formation played a critical role in determining the hole mobility and the photoluminescence (PL) lifetime. Drop-coated films showed the strongest crystallinity, the highest PL quantum yields and a hole mobility (μp) of 1.1 × 10−4 cm2 V−1 s−1, which places tellurophenes in a select group of high mobility phosphorescent emitters. B-Te-6-B was also found to spontaneously form high aspect-ratio microwires upon drop-casting from supersaturated solutions. Oxidative doping in solution by a N(C6H4Br)3[SbCl6]/LiNTf2 reagent combination (Tf = SO2CF3) increased conductivity by 2-4 orders of magnitude without inducing a color change in the films, while exposure to iodine vapor induced a dramatic change in color together with a 4-6 order of magnitude change in the conductivity. The optical transparency, facile electrical doping and relatively high hole mobilities of B-Te-6-B in solution processed thin films offer promise for the use of tellurophenes as host-free emissive layers and hole transport layers in organic optoelectronic devices.  相似文献   

2.
The discovery of highly efficient broadband near infrared (NIR) emission material is urgent and crucial for constructing NIR lighting sources and emerging applications. Herein, a series of NIR emission hexafluorides A2BMF6:Cr3+ (A = Na, K, Rb, Cs; B = Li, Na, K, Cs; M = Al, Ga, Sc, In) peaking at ≈733–801 nm with a full width at half maximum (FWHM) of ≈98–115 nm are synthesized by a general ammonium salt assisted synthesis strategy. Benefiting from the pre-ammoniation of the trivalent metal sources, the Cr3+ can be more efficiently doped into the A2BMF6 and simultaneously prevent the generation of the competitive phase. Particularly, Na3ScF6:Cr3+em = 774 nm, FWHM ≈ 108 nm) with optimal Cr3+-doping concentration of 35.96% shows a high internal quantum efficiency of 91.5% and an external quantum efficiency of ≈40.82%. A lighting emitting diode (LED) device with a NIR output power of ≈291.05 mW at 100 mA driven current and high photoelectric conversion efficiency of 20.94% is fabricated. The general synthesis strategy opens up new avenues for the exploration of Cr3+-doped high efficiency phosphors, and the as-obtained record NIR output power demonstrates for NIR LED lighting sources applications.  相似文献   

3.
Photoluminescence (PL) spectra of Tl4GaIn3Se2S6 layered crystals grown by the Bridgman method have been studied in the energy region of 2.02–2.35 eV and in the temperature range of 16–45 K. A broad PL band centered at 2.20 eV was observed at T=16 K. Variations of emission band has been studied as a function of excitation laser intensity in the 0.1 to 149.9 mW cm−2 range. Radiative transitions from shallow donor level located at 10 meV below the bottom of conduction band to moderately deep acceptor level located at 180 meV above the top of the valence band were suggested to be responsible for the observed PL band. An energy level diagram showing transitions in the band gap of the crystal was plotted taking into account the results of present work and previously reported paper on thermally stimulated current measurements carried out below room temperature. Analysis of the transmission and reflection measurements performed in the wavelength range of 400–1030 nm at room temperature revealed the presence of indirect transitions with 2.22 eV band gap energy.  相似文献   

4.
This paper reported an enhanced photoluminescence of CaSb2O6:Bi3+ by efficient charge compensation. Charge compensated CaSb2O6:Bi3+,M+ (M=Li, Na and K) phosphors were prepared using a co-precipitation technique followed by heat-treatment. The structure and morphology of the as-prepared CaSb2O6:Bi3+,M+ samples were characterized by X-ray diffraction (XRD) and scanning electron microscope (SEM). The results revealed that the obtained CaSb2O6:Bi3+,M+ samples are hexagonal crystal structure and this structure was retained regardless of co-doping by Li+, Na+ or K+. All samples showed sphere-like shape with particle size of 40–80 nm. The optical properties of products were studied by UV–vis diffuse reflectivity, photoluminescence spectra and luminescence decay measurements. Under the excitation of 336 nm light, all of the samples exhibited a strong blue emission peaking around 437 nm, which is attributed to the 3P11S0 transition of the Bi3+ ion. It was found that the charge compensation has significant effect on the photoluminescence properties of CaSb2O6:Bi3+ and the best luminescence properties have been achieved for CaSb2O6:0.75Bi3+,0.75 Na+. The mechanism for the enhancement of the blue emission has also been studied in detail. Our results suggested that the optical properties of oxide nanostructures can be tailored through co-doping with aliovalent ions and the favorable luminescence properties of CaSb2O6:Bi3+,Na+ make it potential for lighting and display applications.  相似文献   

5.
Monolayer WO3·H2O (ML-WO3·H2O) nanosheets are synthesized via a space-confined strategy, and then a single-atom catalyst (SAC) is constructed by individually immobilizing Pt single atoms (Pt-SA) on monolayer WO3 (ML-WO3). The Pt-SA/ML-WO3 retains the monolayer structure of ML-WO3·H2O, with a quite high monolayer ratio up to ≈ 93%, and possesses rich defects (O and W vacancies). It exhibits excellent electrocatalytic performance, with a small overpotential (η) of − 22 mV to drive − 10 mA cm−2 current, a low Tafel slope of ≈ 27 mV dec−1, an ultrahigh turnover frequency of ≈ 87 H2 s−1 site−1 at η  =   − 50 mV, and long-term stability. Of particular note, it exhibits an ultrahigh mass activity of ≈ 87 A mgPt−1 at η  =   − 50 mV, which is ≈ 160 times greater than that of the state-of-the-art commercial catalyst, 20 wt% Pt/C ( ≈ 0.54 A mgPt−1). Experimental and DFT analyses reveal that its excellent performance arises from the strong synergetic effect between the single Pt atoms and the support. This work provides an effective route for large-scale fabrication of ML-WO3 nanosheets, demonstrates ML-WO3 is an excellent support for SACs, and also reveals the great potential of SACs in reducing the amount of noble metals used in catalysts.  相似文献   

6.
《Microelectronics Journal》1999,30(4-5):357-362
Photoluminescence (PL) measurements were carried out on Si/Ge(n)/Si0.7Ge0.3/Si structures (n is varying from 1 to 7 ML) deposed by gas source molecular beam epitaxy (GS-MBE) on Si(100) surfaces and high index Si(118) vicinal surfaces. Ge nanostructures were confined on the top of the undulation of the Si0.3Ge0.7 wetting layer, according to the Stranski–Krastanov growth mode. PL measurements reveal a correlation between the substrate orientation and the island morphology: square dots for (001) and wires for (118) surface orientation. The results suggest that the SiGe wetting layer is required to ensure a good dot size uniformity. The dependence of the luminescence on the excitation power and the PL decay time indicate that the luminescence transitions likely occur in a type-II band line up. Finally, the dot-related PL persists up to room temperature which is very promising for optoelectronic device applications.  相似文献   

7.
The disappointing stability of perovskites, especially in water, remains a key issue hindering their further commercialization. Here, CsPbBr3/CsPb2Br5@PbBr(OH) (PQDs@PbBr(OH)) nano/microspheres with superior stability and outstanding photoluminescence quantum yield (PLQY, ≈98%) are fabricated through a water-assisted process. The nano/microspheres can maintain excellent photoluminescence (PL) intensity and high PLQY (≈90%) when immersed in water for more than 18 months. By changing the water content in the reaction mixture, the phase, particle size, and PL peaks of the nano/microspheres will change. Compared with CsPbBr3/Cs4PbBr6 nanocrystals synthesized without water, PQDs@PbBr(OH) nano/microspheres exhibit better thermal stability, photostability, and superior stability in water. Based on the first-principles calculations, the enhanced stability results from PbBr(OH) with high decomposition enthalpy in water, which can effectively prevent water from contacting PQDs embedded in it. Moreover, white light-emitting diodes are fabricated by mixing green-emitting PQDs@PbBr(OH) powder and K2SiF6:Mn4+ (KSF) red phosphor on a 460 nm blue chip and the device shows a high luminous efficacy of 101.27 lm W−1 at 10 mA. This work not only provides a reliable method for the facile preparation of ultrastable perovskites, but also has great potentials for future practical applications.  相似文献   

8.
To replace the conventional chemical bath deposition method, which is time‐consuming and has a high impurity level, a chemical single‐step deposition process employing a S/Sb ratio‐controlled SbCl3‐thiourea complex solution is introduced to load Sb2S3 into a mesoporous TiO2 electrode. This technique enables the fabrication of efficient and reproducible Sb2S3‐sensitzed inorganic–organic heterojunction hybrid solar cells with hole‐conducting conjugated polymers. The most efficient cell exhibits a short‐circuit current density of 16.1 mA cm?2, an open circuit voltage of 595.5 mV, and a fill factor of 66.5%, yielding a power conversion efficiency of ≈6.4% at standard AM1.5G condition (100 mW cm?2).  相似文献   

9.
We report a study of a series of heavy rare earth tris‐8‐hydroxyquinolines (REQ3s), using UV‐visible absorption spectroscopy, infrared absorption spectroscopy, and photoluminescence (PL) measurements. We show that the heavy REQ3s are all chemically similar to each other and to aluminium tris‐8‐hydroxyquinoline, at least in terms of the ligand behavior. Characteristic rare earth 4f–4f luminescence is only observed for ErQ3 and YbQ3 due to the relatively low energy of the ligand triplet state. We show that a triplet transfer mechanism cannot be responsible for the observed Yb 4f–4f luminescence observed in YbQ3. Instead, an internal chemiluminescent process is shown to be energetically favorable. The thin film PL spectra of all the heavy REQ3s are dominated by triplet emission, except for that of ErQ3, for which transfer to the Er3+ ion represents an efficient alternative. The PL spectra of powder samples, which would be expected to consist of approximately equal amounts of both isomers, are dominated by singlet emission. This is in contrast to the results from the thin films, and suggests that the isomer which predominates in the thin films has a much higher intersystem crossing rate than the other isomer.  相似文献   

10.
Transient optical spectroscopy is used to quantify the temperature-dependence of charge separation and recombination dynamics in P3TEA:SF-PDI2 and PM6:Y6, two non-fullerene organic photovoltaic (OPV) systems with a negligible driving force and high photocurrent quantum yields. By tracking the intensity of the transient electroabsorption response that arises upon interfacial charge separation in P3TEA:SF-PDI2, a free charge generation rate constant of ≈2.4 × 1010 s−1 is observed at room temperature, with an average energy of ≈230 meV stored between the interfacial charge pairs. Thermally activated charge separation is also observed in PM6:Y6, and a faster charge separation rate of ≈5.5 × 1010 s−1 is estimated at room temperature, which is consistent with the higher device efficiency. When both blends are cooled down to cryogenic temperature, the reduced charge separation rate leads to increasing charge recombination either directly at the donor-acceptor interface or via the emissive singlet exciton state. A kinetic model is used to rationalize the results, showing that although photogenerated charges have to overcome a significant Coulomb potential to generate free carriers, OPV blends can achieve high photocurrent generation yields given that the thermal dissociation rate of charges outcompetes the recombination rate.  相似文献   

11.
Luminescent solar concentrators (LSCs) are able to efficiently harvest solar energy through large‐area photovoltaic windows, where fluorophores are delicately embedded. Among various types of fluorophores, all‐inorganic perovskite nanocrystals (NCs) are emerging candidates as absorbers/emitters in LSCs due to their size/composition/dimensionality tunable optical properties and high photoluminescence quantum yield (PL QY). However, due to the large overlap between absorption and emission spectra, it is still challenging to fabricate high‐efficiency LSCs. Intriguingly, zero‐dimensional (0D) perovskites provide a number of features that meet the requirements for a potential LSC absorber, including i) small absorption/emission spectral overlap (Stokes shift up to 1.5 eV); ii) high PL QY (>95% for bulk crystal); iii) robust stability as a result of its large exciton binding energy; and iv) ease of synthesis. In this work, as a proof‐of‐concept experiment, Cs4PbBr6 perovskite NCs are used to fabricate semi‐transparent large‐area LSCs. Cs4PbBr6 perovskite film exhibits green emission with a high PL QY of ≈58% and a small absorption/emission spectral overlap. The optimized LSCs exhibit an external optical efficiency of as high as 2.4% and a power conversion efficiency of 1.8% (100 cm2). These results indicate that 0D perovskite NCs are excellent candidates for high‐efficiency LSCs compared to 3D perovskite NCs.  相似文献   

12.
Although orthorhombic GeSe is predicted to have an ultrahigh figure of merit, ZT ≈ 2.5, up to now, the highest experimental value is ≈0.2 due to the low carrier concentration (nH ≈ 1018 cm−3). Improving symmetry is an effective approach for enhancing the ZT of GeSe-based materials. With Te-alloying, Ge4Se3Te displays the two-dimensional hexagonal structure and high nH ≈ 1.23 × 1021 cm−3. Interestingly, Ge4Se3Te transformed from the hexagonal into the rhombohedral phase with only ≈2% I–V–VI2-alloying (I = Li, Na, K, Cu, Ag; V = Sb, Bi; VI = Se, Te). According to the calculated results of Ge0.82Ag0.09Bi0.09Se0.614Te0.386 single-crystal grown via AgBiTe2-alloying, it exhibits a higher valley degeneracy than the hexagonal Ge4Se3Te. For instance, AgBiTe2-alloying induces a strong band convergence and band inversion effect, resulting in a significantly enhanced Seebeck coefficient and power factor with a similar nH from 17 µV K−1 and 0.63 µW cm−1 K−2 for pristine Ge4Se3Te to 124 µV K−1 and 5.97 µW cm−1 K−2 for 12%AgBiTe2-alloyed sample, respectively. Moreover, the sharply reduced phonon velocity, nano-domain wall structure, and strong anharmonicity lead to low lattice thermal conductivity. As a result, a record-high average ZT ≈0.95 over 323–773 K with an excellent ZT ≈ 1.30 is achieved at 723 K.  相似文献   

13.
Thermoelectric oxide thin films are promising in chip cooling. The issues on the orientation of thin films are essential as they are related to the structures, morphologies, and thermoelectric properties. In this regard, the orientation modulation is conducted on La-doped SrTiO3 thin films on (LaAlO3)0.3(Sr2TaAlO6)0.7 (LSAT) single crystal substrates. Layer-by-layer growth mode is found in (001)- and (110)- oriented thin films, resulting in few grain boundaries (GBs). In (111)-oriented films, island growth mode leads to columnar grain boundaries that build up potential barriers for electrons to be strongly scattered and filtered, suppressing electron mobility and increasing effective mass. In addition, the GBs serve as oxygen vacancy diffusion paths when annealing, causing increased carrier concentration and lattice contraction. The weighted mobility of 71.9 cm2 V−1 s−1 and electrical conductivity of ≈600 S cm−1 are realized in the (001)-oriented film at room temperature. Ultimately, outstanding power factor values of ≈569 µW m−1 K−2 (room temperature) and ≈791 µW m−1 K−2 (573 K) are successfully achieved, outperforming those in polycrystalline ceramics and (111)-oriented films. This study systematically investigates the influence of grain boundaries and orientations on SrTiO3-based thermoelectric films, which lays a solid foundation for improving thermoelectric performance in other oxide thin films.  相似文献   

14.
Site-selective photoluminescence (PL) and photoluminescence excitation (PLE) spectroscopies carried out at 6K on the ∼1540 nm 4I13/24I15/2 emissions of Er3+ in Er-implanted GaN have revealed the existence of four different Er3+ sites and associated PL spectra in this semiconductor. Three of these four sites are excited by below-gap, impurity- or defect-related absorption bands, with subsequent nonradiative energy transfer to the Er3+ 4f electrons; a fourth site is excited by direct Er3+ 4f shell absorption. PLE spectra obtained by selectively detecting Er3+ PL from each of the three sites pumped by broad below-gap absorption bands are compared with the PLE spectra of broad PL bands attributed to implantation damage-induced defects in the Er-implanted GaN. This comparison enables us to distinguish broad-band, below-gap optical excitation processes for Er3+ emission that are attributable to (1) absorption due to implantation damage-induced defects; (2) absorption due to defects or impurities characteristic of the as-grown GaN film; and (3) an Er-specific absorption band just below the band gap which may involve the formation of an Er-related isoelectronic trap. The two sites excited by impurity-or defect-related absorption bands are also strongly pumped by above-gap excitation, while the sites pumped by the Er-related trap and direct 4f shell absorption are not. This observation indicates that excitation of Er3+ luminescence in crystalline semiconductor hosts by either optical or electrical injection of electron-hole pairs is dominated by trap-mediated carrier capture and energy transfer processes. These trap-mediated processes may also control the thermal quenching of Er3+ emission in semiconductors.  相似文献   

15.
Surface effects in atomically flat colloidal CdSe nanoplatelets (NLPs) are significantly and increasingly important with their thickness being reduced to subnanometer level, generating strong surface related deep trap photoluminescence emission alongside the bandedge emission. Herein, colloidal synthesis of highly luminescent two‐monolayer (2ML) CdSe NPLs and a systematic investigation of carrier dynamics in these NPLs exhibiting broad photoluminescence emission covering the visible region with quantum yields reaching 90% in solution and 85% in a polymer matrix is shown. The astonishingly efficient Stokes‐shifted broadband photoluminescence (PL) emission with a lifetime of ≈100 ns and the extremely short PL lifetime of around 0.16 ns at the bandedge signify the participation of radiative midgap surface centers in the recombination process associated with the underpassivated Se sites. Also, a proof‐of‐concept hybrid LED employing 2ML CdSe NPLs is developed as color converters, which exhibits luminous efficacy reaching 300 lm Wopt?1. The intrinsic absorption of the 2ML CdSe NPLs (≈2.15 × 106 cm?1) reported in this study is significantly larger than that of CdSe quantum dots (≈2.8 × 105 cm?1) at their first exciton signifying the presence of giant oscillator strength and hence making them favorable candidates for next‐generation light‐emitting and light‐harvesting applications.  相似文献   

16.
3D organic-inorganic metal halide perovskites are excellent materials for optoelectronic applications due to their exceptional properties, solution processability, and cost-effectiveness. However, the lack of environmental stability highly restricts them from practical applications. Herein, a stable centimeter-long 2D hybrid perovskite (N-MPDA)[PbBr4] single crystal using divalent N1-methylpropane-1,3-diammonium (N-MPDA) cation as an organic spacer, is reported. The as-grown single crystal exhibits stable optoelectronic performance, low threshold random lasing, and multi-photon luminescence/multi-harmonic generation. A photoconductive device fabricated using (N-MPDA)[PbBr4] single crystal exhibits an excellent photoresponsivity (≈124 AW−1 at 405 nm) that is ≈4 orders of magnitudes higher than that of monovalent organic spacer-assisted 2D perovskites, such as (BA)2PbBr4 and (PEA)2PbBr4, and large specific detectivity (≈1012 Jones). As an optical gain media, the (N-MPDA)[PbBr4] single crystal exhibits a low threshold random lasing (≈6.5 µJ cm−2) with angular dependent narrow linewidth (≈0.1 nm) and high-quality factor (Q ≈ 2673). Based on these results, the outstanding optoelectronic merits of (N-MPDA)[PbBr4] single crystal will offer a high-performance device and act as a dynamic material to construct stable future electronics and optoelectronic-based applications.  相似文献   

17.
Significant advances are realized in perovskite‐converted hybrid light‐emitting diodes (pc‐HLEDs). However, long‐living devices at high efficiencies still represent a major milestone with average stabilities of < 200 h at ≈ 50 lm W?1 under low applied currents ( < 15 mA). Herein, a dual metal oxide‐coated CsPbBr3@SiO2/ZrO2 composite is prepared in a one‐pot synthesis through the kinetic control of the sol–gel reaction, followed by a gentle drying process in air. These hybrid nanoparticles show photoluminescence quantum yields of ≈ 65% that are stable under temperature, ambient, and irradiation stress scenarios. This is translated to pc‐HLEDs with a near‐unity conversion efficiency at any applied current, high efficiencies around 75 lm W?1, and one of the most remarkable stabilities of ≈ 200 and 700 h at 100 and 10 mA, respectively. In addition, the device degradation mechanism is thoughtfully rationalized comparing devices operating under ambient/inert conditions. As such, this work provides three milestones: i) a new room temperature one‐pot protocol to realize the first SiO2/ZrO2 metal oxide coating that effectively protects the emitting perovskite nanoparticle core, ii) one of the most stable and efficient pc‐HLEDs operating under ambient condition at any applied current, and iii) new insights for the degradation of pc‐HLEDs.  相似文献   

18.
Silicon pn diodes were fabricated by ion implantation of B and P ions with different doses and subsequent annealing processes. Room temperature photoluminescence (PL) were investigated and the factors affecting the PL intensity were analyzed. Results show that both kinds of pn diodes have PL peak centered at about 1140 nm. Dislocation loops resulted from ion implantation and annealing process may enhance the light emission of silicon pn diode due to its band quantum confinement effect to carriers. The luminescence intensity depends on the carrier concentrations in the implantation region. It should be controlled at the range of 1–6×1016 cm−3. Moreover, the PL intensities of pn diodes with furnace annealing (FA) are higher than those with rapid thermal annealing, and the annealing temperature range for FA is 900–1100 °C.  相似文献   

19.
Eutectic gallium-indium (EGaIn) liquid metal droplets have been considered as a suitable platform for producing customized 3D composites with functional nanomaterials owing to their soft and highly reductive surface. Herein, the synthesis of a 3D plasmonic oxide framework (POF) is reported by incorporating the ultra-thin angstrom-scale-porous hexagonal molybdenum oxide (h-MoO3) onto the spherical EGaIn nanodroplets through ultrasonication. Simultaneously, a large number of oxygen vacancies form in h-MoO3, boosting its free charge carrier concentration and therefore generating a broad surface plasmon resonance across the whole visible light spectrum. The plasmonic chemical sensing properties of the POF is investigated by the surface-enhanced Raman scattering detection of rhodamine 6G (R6G) at 532 nm, in which the minimum detectable concentration is 10−8 m and the enhancement factor reached up to 6.14 × 106. The extended optical absorption of the POF also allowed the efficient degradation of the R6G dye under the excitation of ultraviolet-filtered simulated solar light. Furthermore, the POF exhibits remarkable photocurrent responses towards the entire visible light region with the maximum response of ≈ 1588 A W−1 at 455 nm. This work demonstrates the great potential of the liquid metal-based POFs for high-performance sensing, catalytic, and optoelectronic devices.  相似文献   

20.
2D InSe is one of the semimetal chalcogenides that has been recently given attention thanks to its excellent electrical properties, such as high mobility near 1000 cm2 V−1 s−1 and moderate band gap of ≈1.26 eV suitable for IR detection. Here, high-performance visible to near-infrared (470–980 nm wavelength (λ)) photodetectors using surface-doped InSe as a channel and few-layer graphenes (FLG) as electrodes are reported, where the InSe top region is relatively p-doped using AuCl3. The surface-doped InSe photodetectors show outstanding performance, achieving a photoresponsivity (R) of ≈19 300 A W−1 and a detectivity (D*) of ≈3 × 1013 Jones at λ = 470 nm, and R of ≈7870 A W−1 and D* of ≈1.5 × 1013 Jones at λ = 980 nm, superior to previously reported 2D material-based IR photodetectors operating without an applied gate bias. Surface doping using AuCl3 renders a band bending at the junction between the InSe surface and the top FLG contact, which facilitates electron-hole pair separation and immediate photodetection. Multiple doped or undoped InSe photodetectors with different device structures are investigated, providing insight into the photodetection mechanism and optimizing performance. Encapsulation with hexagonal boron nitride dielectric also allows for 3-month stability.  相似文献   

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