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1.
Angew Chem Int Ed Engl ; : e202403996, 2024 Apr 28.
Artigo em Inglês | MEDLINE | ID: mdl-38679568

RESUMO

Decreasing perovskite nanocrystal size increases radiative recombination due to the quantum confinement effect, but also increases the Auger recombination rate which leads to carrier imbalance in the emitting layers of electroluminescent devices. Here, we overcome this trade-off by increasing the exciton effective mass without affecting the size, which is realized through the trace Cd2+ doping of formamidinium lead bromide perovskite nanocrystals. We observe an ~2.7 times increase in the exciton binding energy benefiting from a slight distortion of the [BX6]4- octahedra caused by doping in the case of that the Auger recombination rate is almost unchanged. As a result, bright color-saturated green emitting perovskite nanocrystals with a photoluminescence quantum yield of 96 % are obtained. Cd2+ doping also shifts up the energy levels of the nanocrystals, relative to the Fermi level so that heavily n-doped emitters convert into only slightly n-doped ones; this boosts the charge injection efficiency of the corresponding light-emitting diodes. The light-emitting devices based on those nanocrystals reached a high external quantum efficiency of 29.4 % corresponding to a current efficiency of 123 cd A-1, and showed dramatically improved device lifetime, with a narrow bandwidth of 22 nm and Commission Internationale de I'Eclairage coordinates of (0.20, 0.76) for color-saturated green emission for the electroluminescence peak centered at 534 nm, thus being fully compliant with the latest standard for wide color gamut displays.

2.
Nat Commun ; 15(1): 1238, 2024 Feb 09.
Artigo em Inglês | MEDLINE | ID: mdl-38336848

RESUMO

Large-area metamorphic stretchable sensor networks are desirable in haptic sensing and next-generation electronics. Triboelectric nanogenerator-based self-powered tactile sensors in single-electrode mode constitute one of the best solutions with ideal attributes. However, their large-area multiplexing utilizations are restricted by severe misrecognition between sensing nodes and high-density internal circuits. Here, we provide an electrical signal shielding strategy delivering a large-area multiplexing self-powered untethered triboelectric electronic skin (UTE-skin) with an ultralow misrecognition rate (0.20%). An omnidirectionally stretchable carbon black-Ecoflex composite-based shielding layer is developed to effectively attenuate electrostatic interference from wirings, guaranteeing low-level noise in sensing matrices. UTE-skin operates reliably under 100% uniaxial, 100% biaxial, and 400% isotropic strains, achieving high-quality pressure imaging and multi-touch real-time visualization. Smart gloves for tactile recognition, intelligent insoles for gait analysis, and deformable human-machine interfaces are demonstrated. This work signifies a substantial breakthrough in haptic sensing, offering solutions for the previously challenging issue of large-area multiplexing sensing arrays.


Assuntos
Percepção do Tato , Dispositivos Eletrônicos Vestíveis , Humanos , Tato , Eletricidade
3.
Small ; 20(13): e2307201, 2024 Mar.
Artigo em Inglês | MEDLINE | ID: mdl-37950403

RESUMO

Power generation from water-triggered capillary action in porous structures has recently geared extensive attention, offering the potential for generating electricity from ubiquitous water evaporation. However, conclusively establishing the nature of electrical generation and charge transfer is extremely challenging arising from the complicated aqueous solid-liquid interfacial phenomenon. Here, an electric probe-integrated microscope is developed to on-line monitor the correlation between water capillary action and potential values at any desired position of an active layer. With a probe spatial resolution reaching up to fifty micrometers, the internal factors prevailing over the potential distribution across the whole wet and dry regions are comprehensively identified. Further, the self-powered sensing capabilities of this integrated system are also demonstrated, including real-time monitoring of wind speed, environmental humidity, ionic strength, and inclination angle of generators. The combination of electric potential and chemical color indicator suggests that charge generation is likely correlated with ion-selective transport in the nanoporous channel during the water infiltration process. And unipolar ions (for instance protons) should be the dominant charge-transfer species. The work reveals the fundamental principles regulating charge generation/transfer during the water-triggered electric generation process.

4.
Sci Bull (Beijing) ; 68(23): 2954-2961, 2023 Dec 15.
Artigo em Inglês | MEDLINE | ID: mdl-37919156

RESUMO

In terms of tunable luminescence and high quantum efficiency, colloidal quantum dots (CQDs) are promising semiconductors for constructing near-infrared light-emitting diodes (NIR-LEDs). However, currently available NIR-LEDs are susceptible to variations in the emission layer thickness (EMLT), the highest external quantum efficiency (EQE) decreases to below 50% (relative to peak EQE) when the EMLT varies out of a narrow range of (±30 nm). This is due to the thickness-dependent carrier recombination rate and current density variation, resulting in batch-to-batch EQE fluctuations that limit LED reproducibility. Here we report efficient NIR-LEDs that exhibit EQE variations of less than 15% (relative to the champion EQE) over an EMLT range of 40-220 nm; the highest achievable EQE of ∼11.5% was obtained by encapsulating a 212 nm-thick CQD within a type-I inorganic shell to enhance the radiative recombination in the dots, resulting in a high photoluminescence quantum yield of 80%, and by post-treating the films with a bifunctional linking agent to improve and balance the hole and electron mobilities in the entire film (electron mobility: 8.23 × 10-3 cm2 V-1 s-1; hole mobility: 7.0 × 10-3 cm2 V-1 s-1). This work presents the first NIR-LEDs that exhibit EMLT-invariant EQE over an EMLT range of 40-220 nm, which represents the highest EQE among reported CQD NIR-LEDs with a QD thickness exceeding 100 nm.

5.
J Phys Chem Lett ; 14(37): 8376-8384, 2023 Sep 21.
Artigo em Inglês | MEDLINE | ID: mdl-37706473

RESUMO

Perovskite materials are promising candidates for the implementation of electrically pumped lasers considering the enhanced performance of perovskite-based light-emitting diodes. Nonetheless, current methods of fabricating perovskite optical microcavities require complex patterning technologies to build suitable resonant cavities for perovskite laser emission, burdening the device structure design. To address this issue, we applied inkjet printing, a maskless patterning technique, to directly create spontaneous formations of polycrystalline perovskite microcavity arrays to explore their laser-emitting action. The substrate surface tension was tuned to modulate the perovskite crystallization process in combination with optimization of printing ink recipes. As a result, polycrystalline perovskite microcavity arrays were achieved, contributing to the laser emission at 528 nm with a lasing threshold of 1.37 mJ/cm2, while simultaneously achieving high-definition patterning of flexible display. These results clearly illustrate the efficiency of inkjet printing technology in the preparation of polycrystalline perovskite optical microcavities and promote the development of flexible laser arrayed displays, providing a facile process toward the realization of perovskite-cavity laser devices.

6.
Adv Mater ; 35(40): e2305438, 2023 Oct.
Artigo em Inglês | MEDLINE | ID: mdl-37526223

RESUMO

Water-droplet-based electricity generators are emerging hydrovoltaic technologies that harvest energy from water circulation through strong interactions between water and nanomaterials. However, such devices exhibit poor current performance owing to their unclear driving force (evaporation or infiltration) and undesirable reverse diffusion current. Herein, a water-droplet-based hydrovoltaic electricity generator induced by capillary infiltration with an asymmetric structure composed of a diode-like heterojunction formed by negatively and positively charged materials is fabricated. This device can generate current densities of 160 and 450 µA cm-2 at room temperature and 65 °C, respectively. The heterojunction achieves a rectification ratio of 12, which effectively suppresses the reverse current caused by concentration differences. This results in an improved charge accumulation of ≈60 mC cm-2 in 1000 s, which is three times the value observed in the control device. When the area of the device is increased to 6 cm2 , the current increases linearly to 1 mA, thus demonstrating the scale-up potential of the generator. It has been proven that the streaming potential originates from capillary infiltration, and the presence of ion rectification. The proposed method of constructing ion-diode-like structures provides a new strategy for improving generator performance.

7.
Small ; 19(44): e2304829, 2023 Nov.
Artigo em Inglês | MEDLINE | ID: mdl-37403273

RESUMO

Owing to outstanding optoelectronic properties, lead halide perovskite nanocrystals (PNCs) are considered promising emitters for next-generation displays. However, the development of pure blue (460-470 nm) perovskite nanocrystal light-emitting diodes (PNC-LEDs), which correspond to the requirements of Rec. 2020 standard, lag far behind that of their green and red counterparts. Here, pure blue CsPb(Br/Cl)3 nanocrystals with remarkable optical performance are demonstrated by a facile fluorine passivation strategy. Prominently, the fluorine passivation on halide vacancies and strong bonding of Pb-F intensely enhance crystal structure stability and inhibit "particle talking" behaviors under both thermal and electrical conditions. Fluorine-based PNCs with high resistance of luminescence thermal quenching retain 70% of photoluminescent intensity when heated to 343 K, which can be attributed to the elevated activation energy for carrier trapping and unchanged grain size. Fluorine-based PNC-LEDs also exhibit stable pure blue electroluminescence (EL) emission with sevenfold promoted luminance and external quantum efficiencies (EQEs), where the suppression of ion migration is further evidenced by a lateral structure device with applied polarizing potential.

8.
J Phys Chem Lett ; 14(21): 5025-5032, 2023 Jun 01.
Artigo em Inglês | MEDLINE | ID: mdl-37227043

RESUMO

Manipulating the crystallization dynamics of perovskite emitters is an effective strategy for preparing high-performance perovskite light-emitting diodes (PeLEDs). In general, amorphous-like thermodynamically stable intermediates are desirable for a retarded and controllable crystallization process of perovskite emitters. Despite a variety of well-demonstrated strategies for crystallization control, it has been generally realized that perovskite thin-film emitters show problematic reproducibility. Here, we unraveled that the coordinating solvent vapor residues could raise deleterious influences on the formation of amorphous intermediate phases, which thus leads to varying crystal qualities from batch to batch. We demonstrated that undesirable crystalline intermediate phases tend to form with a strong coordination solvent vapor atmosphere, which alters the crystallization process and thus brings about additional ionic defects. By applying an inert gas flush strategy, this detrimental effect could be effectively mitigated, enabling PeLEDs with high reproducibility. This work provides new insight into the fabrication of efficient and reproducible perovskite optoelectronics.

9.
ACS Appl Mater Interfaces ; 15(10): 13753-13760, 2023 Mar 15.
Artigo em Inglês | MEDLINE | ID: mdl-36877864

RESUMO

Molybdenum nitride (MoNx) was perceived as carrier-selective contacts (CSCs) for crystalline silicon (c-Si) solar cells due to having proper work functions and excellent conductivities. However, the poor passivation and non-Ohmic contact at the c-Si/MoNx interface endow an inferior hole selectivity. Here, the surface, interface, and bulk structures of MoNx films are systematically investigated by X-ray scattering, surface spectroscopy, and electron microscope analysis to reveal the carrier-selective features. Surface layers with the composition of MoO2.51N0.21 form upon air exposure, which induces the overestimated work function and explains the origin of inferior hole selectivities. The c-Si/MoNx interface is confirmed to adopt long-term stability, providing guidance for designing stable CSCs. A detailed evolution of the scattering length density, domain sizes, and crystallinity in the bulk phase is presented to elucidate its superior conductivity. These multiscale structural investigations offer a clear structure-function correlation of MoNx films, providing key inspiration for developing excellent CSCs for c-Si solar cells.

10.
Adv Mater ; 35(6): e2208042, 2023 Feb.
Artigo em Inglês | MEDLINE | ID: mdl-36433769

RESUMO

Colored solar panels, realized by depositing various reflection layers or structures, are emerging as power sources for building with visual aesthetics. However, these panels suffer from reduced photocurrent generation due to the less efficient light harvesting from visible light reflection and degraded power conversion efficiency (PCE). Here, color-patterned silicon heterojunction solar cells are achieved by incorporating luminescent quantum dots (QDs) with high quantum yields as light converters to realize an asthenic appearance with high PCE. It is found that large bandgap (blue) QD layers can convert UV light into visible light, which can notably alleviate the parasitic absorption by the front indium tin oxide and doped amorphous silicon. Additionally, a universal optical path model is proposed to understand the light transmission process, which is suitable for luminescent down-shift devices. In this study, solar cells with a PCE exceeding 23.5% are achieved using the combination of a blue QD layer and a top low refractive index anti-reflection layer. Based on our best knoledge,the obtained PCE is the highest for a color-patterned solar cell. The results suggest an enhanced strategy involving incorporation of luminescent QDs with an optical path design for high-performance photovoltaic panels with visual aesthetics.

11.
Small ; 19(4): e2205265, 2023 Jan.
Artigo em Inglês | MEDLINE | ID: mdl-36420652

RESUMO

Electricity generation triggered by the ubiquitous water evaporation process provides an intriguing way to harvest energy from water. Meanwhile, natural water evaporation is also a fundamental way to obtain fresh water for human beings. Here, a wafer-scale nanostructured silicon-based device that takes advantage of its well-aligned configuration that simultaneously realizes solar steam generation (SSG) for freshwater collection and hydrovoltaic effect generation for electricity output is developed. An ingenious porous, black carbon nanotube fabric (CNF) electrode endows the device with sustainable water self-pumping capability, excellent durable conductivity, and intense solar spectrum harvesting. A combined device based on the CNF electrode integrated with nanostructured silicon nanowire arrays (SiNWs) provided an aligned numerous surface-to-volume water evaporation interface that enables a recorded continuous short-circuit current 8.65 mA and a water evaporation rate of 1.31 kg m-2 h-1 under one sun illumination. Such wafer-scale SiNWs-based SSG and hydrovoltaic integration devices would unchain the bottleneck of the weak and discontinuous electrical output of hydrovoltaic devices, which inspires other sorts of semiconductor-based hydrovoltaic device designs to target superior performance.

12.
STAR Protoc ; 3(3): 101631, 2022 09 16.
Artigo em Inglês | MEDLINE | ID: mdl-36035792

RESUMO

Preparation of highly efficient and stable perovskite light-emitting diodes (PeLEDs) with reproducible device performance is challenging. This protocol describes steps for fabrication of high-performance and self-healing PeLEDs. These include instructions for synthesis of charge-transporting zinc oxide (ZnO) nanocrystals, step-by-step device fabrication, and control over self-healing of the degraded devices. For complete details on the use and execution of this protocol, please refer to Teng et al. (2021).


Assuntos
Compostos de Cálcio , Óxidos , Titânio
13.
ACS Appl Mater Interfaces ; 14(21): 24648-24658, 2022 Jun 01.
Artigo em Inglês | MEDLINE | ID: mdl-35581001

RESUMO

There is an increasing need for multifunctional sensors that can detect radiation, biological activity, gas, etc. for efficient health monitoring, neurological medical devices, and human-machine interfaces in recent years. Herein, we demonstrated a multifunctional Sn-doped In2O3 nanocrystal (ITO NC) based device for ulyoutraviolet (UV)/infrared (IR) dual-band photodetection and light-activated efficient nitrogen dioxide (NO2) gas sensing at room temperature (RT). The effects of different surface ligands and annealing process of ITO NCs on their photodetection performance were investigated. The ITO NCs capped with 1,2-ethanedithiol (EDT) show a responsivity of 31.3/177.7 mA W-1 and normalized detectivity of ∼1 × 1010/109 cm Hz1/2 W-1 under UV/IR illumination at 375/2200 nm at RT. The potential of the ITO NCs sensors to monitor low concentrations of NO2 is activated by light illumination. The sensor has a higher response (4.2) to 1 ppm of NO2, shorter response/recovery time (156.8/554.2 s), and a lower detection limit (LOD) (219 ppb) under UV illumination compared within a dark environment. The LOD of the sensor is lower than the allowable exposure limit of NO2 specified in "Air Pollutant Limits" of the Occupational Safety and Health Administration (OSHA). Our work paves an alternative platform for the development of low-cost, integration-friendly multifunctional devices.

14.
Adv Mater ; 34(26): e2200344, 2022 Jul.
Artigo em Inglês | MEDLINE | ID: mdl-35524638

RESUMO

Advanced doped-silicon-layer-based passivating contacts have boosted the power conversion efficiency (PCE) of single-junction crystalline silicon (c-Si) solar cells to over 26%. However, the inevitable parasitic light absorption of the doped silicon layers impedes further PCE improvement. To this end, alternative passivating contacts based on wide-bandgap metal compounds (so-called dopant-free passivating contacts (DFPCs)) have attracted great attention, thanks to their potential merits in terms of parasitic absorption loss, ease-of-deposition, and cost. Intensive research activity has surrounded this topic with significant progress made in recent years. Various electron-selective and hole-selective contacts based on metal compounds have been successfully developed, and a champion PCE of 23.5% has been achieved for a c-Si solar cell with a MoOx -based hole-selective contact. In this work, the fundamentals and development status of DFPCs are reviewed and the challenges and potential solutions for enhancing the carrier selectivity of DFPCs are discussed. Based on comprehensive and in-depth analysis and simulations, the improvement strategies and future prospects for DFPCs design and device implementation are pointed out. By tuning the carrier concentration of the metal compound and the work function of the capping transparent electrode, high PCEs over 26% can be achieved for c-Si solar cells with DFPCs.

15.
ACS Appl Mater Interfaces ; 14(17): 19569-19578, 2022 May 04.
Artigo em Inglês | MEDLINE | ID: mdl-35442031

RESUMO

Moisture-triggered electricity generator (MEG) harvesting energy from the ubiquity of atmospheric moisture is one of the promising potential candidates for renewable power demand. However, MEG device performance is strongly dependent on the moisture concentration, which results in its large fluctuation of the electrical output. Here, a Janus heterojunction MEG device consisting of nanostructured silicon and hygroscopic polyelectrolyte incorporating hydrophilic carbon nanotube mesh is proposed to enable ambient moisture harvesting and continuous stable electrical output delivery. The nanostructured silicon with a large surface/volume ratio provides strong coupling interaction with water molecules for charge generation. A polyelectrolyte of polydiallyl dimethylammonium chloride (PDDA) can facilitate charge selective transporting and enhance the effectiveness of moisture-absorbing in an arid environment simultaneously. The conductive, porous, and hydrophilic carbon nanotube mesh allows water to be ripped through as well as the generated charges being collected timely. As such, any generated charge carriers in the Janus heterojunction can be efficiently swept toward their respective electrodes, because of the device asymmetric contact. A MEG device continuously delivers an open-circuit voltage of 1.0 V, short-circuit current density of 8.2 µA/cm2, and output power density of 2.2 µW/cm2 under an ambient environment (60% relative humidity, 25 °C), which is a record value over the previously reported values. Furthermore, the infrared thermal measurements also reveal that the moisture-triggered electricity generation power is likely ascribed to surrounding thermal energy collected by the MEG device. Our results provide an insightful rationale for the design of device structure and understanding of the working mechanism of MEG, which is of great importance to promote the efficient electricity conversion induced by moisture in the atmosphere.

16.
Opt Lett ; 47(8): 2089-2092, 2022 Apr 15.
Artigo em Inglês | MEDLINE | ID: mdl-35427344

RESUMO

Solution processed colloidal semiconductor quantum dots (QDs) have size-tunable optical transitions and high quantum efficiencies, enabling various applications in opto-electronic devices. To enrich the functionality of QD-based opto-electronic devices, colloidal semiconductor QDs have been frequently coupled with optical cavities to enable emission modulation. However, it remains a challenge to fully understand the interaction between the optical cavity resonance and the QD emission, especially for the planar optical microcavities. Here, we have investigated the light emission of colloidal semiconductor QDs in the planar Fabry-Perot microcavity consisted of two Ag mirrors. With the matched QD and cavity resonance, the microcavity coupled QD samples show a prominently narrower emission linewidth and emission angle range because of the efficient QD-cavity coupling, while with a slightly positive or negative energy detuning, the linewidth and angular distribution of the microcavity coupled QD emission both become broadened. Furthermore, with the standard lithography technique, the microcavity coupled QD sample can be patterned into arbitrary geometries, showing extra features of in-plane mode confinement. Our work highlights the important role of detuning in determining the coupling between colloidal semiconductor QDs and microcavities and paves the way for the future design of microcavity coupled QD devices.

17.
J Phys Chem Lett ; 13(13): 3121-3129, 2022 Apr 07.
Artigo em Inglês | MEDLINE | ID: mdl-35357156

RESUMO

Balanced charge injection is key to achieving perovskite light-emitting diodes (PeLEDs) with a low efficiency roll-off at a high brightness. The use of zinc oxide (ZnO) with a high electron mobility as the charge transport layers is desirable; however, photoluminescence (PL) quenching of a perovskite on ZnO always occurs. Here, a quasi-two-dimensional perovskite on ZnO is explored to uncover the PL quenching mechanism, mainly ascribed to the deprotonation of ammonium cations on the ZnO film in association with the decomposition of low-dimensional perovskite phases. Surprisingly, crystal plane-dependent PL quenching results indicate that the deprotonation rate strongly correlates with the crystal orientation of the ZnO surface. We developed a strategy for suppressing perovskite PL quenching by incorporating an atomic layer deposited Al2O3 onto the ZnO film. Consequently, an efficient inverted PeLED was achieved with a maximum external quantum efficiency of 17.7% and a less discernible efficiency roll-off at a high current density.

18.
Nano Lett ; 22(3): 1331-1337, 2022 Feb 09.
Artigo em Inglês | MEDLINE | ID: mdl-35073101

RESUMO

Quantum emitters are needed for a myriad of applications ranging from quantum sensing to quantum computing. Hexagonal boron nitride (hBN) quantum emitters are one of the most promising solid-state platforms to date due to their high brightness and stability and the possibility of a spin-photon interface. However, the understanding of the physical origins of the single-photon emitters (SPEs) is still limited. Here we report dense SPEs in hBN across the entire visible spectrum and present evidence that most of these SPEs can be well explained by donor-acceptor pairs (DAPs). On the basis of the DAP transition generation mechanism, we calculated their wavelength fingerprint, matching well with the experimentally observed photoluminescence spectrum. Our work serves as a step forward for the physical understanding of SPEs in hBN and their applications in quantum technologies.

19.
Small Methods ; 6(1): e2100916, 2022 Jan.
Artigo em Inglês | MEDLINE | ID: mdl-35041289

RESUMO

It is highly desired to develop advanced characterization techniques to explore the 3D nanoscale morphology of the complicated blend film of ternary organic solar cells (OSCs). Here, ternary OSCs are constructed by incorporating the nonfullerene acceptor perylenediimide (PDI)-diketopyrrolopyrrole (DPP)-PDI and their morphology is characterized in depth to understand the performance variation. In particular, photoinduced force microscopy (PiFM) coupled with infrared laser spectroscopy is conducted to qualitatively study the distribution of donor and acceptors in the blend film by chemical identification and to quantitatively probe the segmentation of domains and the domain size distribution after PDI-DPP-PDI acceptor incorporation by PiFM imaging and data processing. In addition, the energy-filtered transmission electron microscopy with energy loss spectra is utilized to visualize the nanoscale morphology of ultrathin cross-sections in the configuration of the real ternary device for the first time in the field of photovoltaics. These measurements allow to "view" the surface and cross-sectional morphology and provide strong evidence that the PDI-DPP-PDI acceptor can suppress the aggregation of the fullerene molecules and generate the homogenous morphology with a higher-level of the molecularly mixed phase, which can prevent the charge recombination and stabilize the morphology of photoactive layer.

20.
Phys Chem Chem Phys ; 23(40): 23380-23388, 2021 Oct 20.
Artigo em Inglês | MEDLINE | ID: mdl-34636820

RESUMO

The pressure- and temperature-dependent luminescence properties of M'-phase Nd3+:YTaO4 synthesized by a molten salt method are presented. Ten near-infrared emission lines originating from the transitions between the two Stark levels R1,2 of the 3F3/2 state and the five Stark levels Z1,2,3,4,5 of the 4I9/2 state for the doped Nd3+ ions can be clearly identified. All these emission lines are found to shift linearly with pressure in a range up to ∼11 GPa. The R2,1 → Z5 emission lines have larger pressure sensitivities, which are 16.44 and 14.27 cm-1 GPa-1. The intensities of all the emission lines evolve with pressure non-monotonically, and peak at ∼1 GPa. The R1 → Z4,5 and R2 → Z1 emission lines can be obviously narrowed under the hydrostatic pressure, and broadened under the non-hydrostatic pressure, indicating their potential capability for reflecting the characteristic of a pressure environment. The intensity ratio of the R2,1 → Z5 emission lines exhibits a large temperature dependence, with a relative sensitivity between 0.129% and 0.108% K-1 in the physiological temperature range of 290-320 K. Thermal variations of the spectral positions and widths of the R2,1 → Z5 emission lines are also investigated. A high thermal stability for the position of the R2 → Z5 emission line is revealed. Based on the experimental results, the advantages and potential of Nd3+:YTaO4 as a multi-functional sensor for pressure and temperature are discussed.

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