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1.
Nanoscale ; 12(17): 9661-9668, 2020 May 07.
Artigo em Inglês | MEDLINE | ID: mdl-32319509

RESUMO

Colloidal CdSe nanoplatelets, with the electronic structure of quantum wells, self-assemble into lamellar stacks due to large co-facial van der Waals attractions. These lamellar stacks are shown to display coherent acoustic phonons that are detected from oscillatory changes in the absorption spectrum observed in infrared pump, electronic probe measurements. Rather than direct electronic excitation of the nanocrystals using a femtosecond laser, impulsive transfer of heat from the organic ligand shell, excited at C-H stretching vibrational resonances, to the inorganic core of individual nanoplatelets occurs on a time-scale of <100 ps. This heat transfer drives in-phase longitudinal acoustic phonons of the nanoplatelet lamellae, which are accompanied by subtle deformations along the nanoplatelet short axes. The frequencies of the oscillations vary from 0.7 to 2 GHz (3-8 µeV and 0.5-1 ns oscillation period) depending on the thickness of the nanoplatelets-but not their lateral areas-and the temperature of the sample. Temperature-dependence of the acoustic phonon frequency conveys a substantial stiffening of the organic ligand bonds between nanoplatelets with reduced temperature. These results demonstrate a potential for acoustic modulation of the excitonic structure of nanocrystal assemblies in self-assembled anisotropic semiconductor systems at temperatures at or above 300 K.

2.
ACS Nano ; 2020 Mar 30.
Artigo em Inglês | MEDLINE | ID: mdl-32208676

RESUMO

Metal nanocrystals exhibit important optoelectronic and photocatalytic functionalities in response to light. These dynamic energy conversion processes have been commonly studied by transient optical probes to date, but an understanding of the atomistic response following photoexcitation has remained elusive. Here, we use femtosecond resolution electron diffraction to investigate transient lattice responses in optically excited colloidal gold nanocrystals, revealing the effects of nanocrystal size and surface ligands on the electron-phonon coupling and thermal relaxation dynamics. First, we uncover a strong size effect on the electron-phonon coupling, which arises from reduced dielectric screening at the nanocrystal surfaces and prevails independent of the optical excitation mechanism (i.e., inter- and intraband). Second, we find that surface ligands act as a tuning parameter for hot carrier cooling. Particularly, gold nanocrystals with thiol-based ligands show significantly slower carrier cooling as compared to amine-based ligands under intraband optical excitation due to electronic coupling at the nanocrystal/ligand interfaces. Finally, we spatiotemporally resolve thermal transport and heat dissipation in photoexcited nanocrystal films by combining electron diffraction with stroboscopic elastic scattering microscopy. Taken together, we resolve the distinct thermal relaxation time scales ranging from 1 ps to 100 ns associated with the multiple interfaces through which heat flows at the nanoscale. Our findings provide insights into optimization of gold nanocrystals and their thin films for photocatalysis and thermoelectric applications.

3.
ACS Nano ; 2020 Mar 23.
Artigo em Inglês | MEDLINE | ID: mdl-32105062

RESUMO

The morphology of nanocrystals serves as a powerful handle to modulate their functional properties. For semiconducting nanostructures, the shape is no less important than the size and composition, in terms of determining the electronic structure. For example, in the case of nanoplatelets (NPLs), their two-dimensional (2D) electronic structure and atomic precision along the axis of quantum confinement makes them well-suited as pure color emitters and optical gain media. In this study, we describe synthetic efforts to develop ZnSe NPLs emitting in the ultraviolet part of the spectrum. We focus on two populations of NPLs, the first having a sharp absorption onset at 345 nm and a previously unreported species with an absorption onset at 380 nm. Interestingly, we observe that the nanoplatelets are one step in a quantized reaction pathway that starts with (zero-dimensional (0D)) magic-sized clusters, then proceeds through the formation of (one-dimensional (1D)) nanowires toward the (2D) "345 nm" species of NPLs, which finally interconvert into the "380 nm" NPL species. We seek to rationalize this evolution of the morphology, in terms of a general free-energy landscape, which, under reaction control, allows for the isolation of well-defined structures, while thermodynamic control leads to the formation of three-dimensional (3D) nanocrystals.

4.
Nat Mater ; 2020 Jan 27.
Artigo em Inglês | MEDLINE | ID: mdl-31988516

RESUMO

Improving charge mobility in quantum dot (QD) films is important for the performance of photodetectors, solar cells and light-emitting diodes. However, these applications also require preservation of well defined QD electronic states and optical transitions. Here, we present HgTe QD films that show high mobility for charges transported through discrete QD states. A hybrid surface passivation process efficiently eliminates surface states, provides tunable air-stable n and p doping and enables hysteresis-free filling of QD states evidenced by strong conductance modulation. QD films dried at room temperature without any post-treatments exhibit mobility up to µ ~ 8 cm2 V-1 s-1 at a low carrier density of less than one electron per QD, band-like behaviour down to 77 K, and similar drift and Hall mobilities at all temperatures. This unprecedented set of electronic properties raises important questions about the delocalization and hopping mechanisms for transport in QD solids, and introduces opportunities for improving QD technologies.

5.
Nat Commun ; 10(1): 4511, 2019 10 04.
Artigo em Inglês | MEDLINE | ID: mdl-31586067

RESUMO

Colloidal quantum wells are two-dimensional materials grown with atomically-precise thickness that dictates their electronic structure. Although intersubband absorption in epitaxial quantum wells is well-known, analogous observations in non-epitaxial two-dimensional materials are sparse. Here we show that CdSe nanoplatelet quantum wells have narrow (30-200 meV), polarized intersubband absorption features when photoexcited or under applied bias, which can be tuned by thickness across the near-infrared (NIR) spectral window (900-1600 nm) inclusive of important telecommunications wavelengths. By examination of the optical absorption and polarization-resolved measurements, the NIR absorptions are assigned to electron intersubband transitions. Under photoexcitation, the intersubband features display hot carrier and Auger recombination effects similar to excitonic absorptions. Sequenced two-color photoexcitation permits the sub-picosecond modulation of the carrier temperature in such colloidal quantum wells. This work suggests that colloidal quantum wells may be promising building blocks for NIR technologies.

6.
ACS Nano ; 13(12): 13917-13931, 2019 Dec 24.
Artigo em Inglês | MEDLINE | ID: mdl-31609104

RESUMO

Direct optical lithography of functional inorganic nanomaterials (DOLFIN) is a photoresist-free method for high-resolution patterning of inorganic nanocrystals (NCs) that has been demonstrated using deep UV (DUV, 254 nm) photons. Here, we expand the versatility of DOLFIN by designing a series of photochemically active NC surface ligands for direct patterning using various photon energies including DUV, near-UV (i-line, 365 nm), blue (h-line, 405 nm), and visible (450 nm) light. We show that the exposure dose for DOLFIN can be ∼30 mJ/cm2, which is small compared to most commercial photopolymer resists. Patterned nanomaterials can serve as highly robust optical diffraction gratings. We also introduce a general approach for resist-free direct electron-beam lithography of functional inorganic nanomaterials (DELFIN) which enables all-inorganic NC patterns with feature size down to 30 nm, while preserving the optical and electronic properties of patterned NCs. The designed ligand chemistries and patterning techniques offer a versatile platform for nano- and micron-scale additive manufacturing, complementing the existing toolbox for device fabrication.

7.
ACS Nano ; 13(11): 12415-12424, 2019 Nov 26.
Artigo em Inglês | MEDLINE | ID: mdl-31560851

RESUMO

Nanomaterials dispersed in different media, such as liquids or polymers, generate a variety of functional composites with synergistic properties. In this work, we discuss liquid metals as the nanomaterials' dispersion media. For example, 2D transition-metal carbides and nitrides (MXenes) can be efficiently dispersed in liquid Ga and lightweight alloys of Al, Mg, and Li. We show that the Lifshitz theory predicts strong van der Waals attraction between nanoscale objects interacting through liquid metals. However, a uniform distribution of MXenes in liquid metals can be achieved through colloidal gelation, where particles form self-supporting networks stable against macroscopic phase segregation. This network acts as a reinforcement boosting mechanical properties of the resulting metal-matrix composite. By choosing Mg-Li alloy as an example of ultralightweight metal matrix and Ti3C2Tx MXene as a nanoscale reinforcement, we apply a liquid metal gelation technique to fabricate functional nanocomposites with an up to 57% increase in the specific yield strength without compromising the matrix alloy's plasticity. MXenes largely retain their phase and 2D morphology after processing in liquid Mg-Li alloy at 700 °C. The 2D morphology enables formation of a strong semicoherent interface between MXene and metal matrix, manifested by biaxial strain of the MXene lattice inside the metal matrix. This work expands applications for MXenes and shows the potential for developing MXene-reinforced metal matrix composites for structural alloys and other emerging applications with metal-MXene interfaces, such as batteries and supercapacitors.

8.
J Am Chem Soc ; 141(34): 13487-13496, 2019 Aug 28.
Artigo em Inglês | MEDLINE | ID: mdl-31379152

RESUMO

In contrast to molecular systems, which are defined with atomic precision, nanomaterials generally show some heterogeneity in size, shape, and composition. The sample inhomogeneity translates into a distribution of energy levels, band gaps, work functions, and other characteristics, which detrimentally affect practically every property of functional nanomaterials. We discuss a novel synthetic strategy, colloidal atomic layer deposition (c-ALD) with stationary reactant phases, which largely circumvents the limitations of traditional colloidal syntheses of nano-heterostructures with atomic precision. This approach allows for significant reduction of inhomogeneity in nanomaterials in complex nanostructures without compromising their structural perfection and enables the synthesis of epitaxial nano-heterostructures of unprecedented complexity. The improved synthetic control ultimately enables bandgap and strain engineering in colloidal nanomaterials with close to atomic accuracy. To demonstrate the power of the new c-ALD method, we synthesize a library of complex II-VI semiconductor nanoplatelet heterostructures. By combining spectroscopic and computational studies, we elucidate the subtle interplay between quantum confinement and strain effects on the optical properties of semiconductor nanostructures.

9.
ACS Nano ; 13(5): 5760-5770, 2019 May 28.
Artigo em Inglês | MEDLINE | ID: mdl-30964280

RESUMO

The nature of the interface between the solute and the solvent in a colloidal solution has attracted attention for a long time. For example, the surface of colloidal nanocrystals (NCs) is specially designed to impart colloidal stability in a variety of polar and nonpolar solvents. This work focuses on a special type of colloids where the solvent is a molten inorganic salt or organic ionic liquid. The stability of such colloids is hard to rationalize because solvents with high density of mobile charges efficiently screen the electrostatic double-layer repulsion, and purely ionic molten salts represent an extreme case where the Debye length is only ∼1 Å. We present a detailed investigation of NC dispersions in molten salts and ionic liquids using small-angle X-ray scattering (SAXS), atomic pair distribution function (PDF) analysis and molecular dynamics (MD) simulations. Our SAXS analysis confirms that a wide variety of NCs (Pt, CdSe/CdS, InP, InAs, ZrO2) can be uniformly dispersed in molten salts like AlCl3/NaCl/KCl (AlCl3/AlCl4-) and NaSCN/KSCN and in ionic liquids like 1-butyl-3-methylimidazolium halides (BMIM+X-, where X = Cl, Br, I). By using a combination of PDF analysis and molecular modeling, we demonstrate that the NC surface induces a solvent restructuring with electrostatic correlations extending an order of magnitude beyond the Debye screening length. These strong oscillatory ion-ion correlations, which are not accounted by the traditional mechanisms of steric and electrostatic stabilization of colloids, offer additional insight into solvent-solute interactions and enable apparently "impossible" colloidal stabilization in highly ionized media.

10.
ACS Nano ; 13(5): 5375-5384, 2019 May 28.
Artigo em Inglês | MEDLINE | ID: mdl-31017762

RESUMO

Self-assembly of two sizes of nearly spherical colloidal nanocrystals (NCs) capped with hydrocarbon surface ligands has been shown to produce more than 20 distinct phases of binary nanocrystal superlattices (BNSLs). Such structural diversity, in striking contrast to binary systems of micron-sized colloidal beads, cannot be rationalized by models assuming entropy-driven crystallization of simple spheres. In this work, we show that the PbS ligand binding equilibrium controls the relative stability of two closely related BNSL structures featuring alternating layers of PbS and Au NCs. At an intermediate size ratio, as-prepared PbS NCs assemble with Au NCs into CuAu BNSLs featuring orientational coherence of PbS NCs across the lattice. Measurement of interparticle separations within CuAu and modeling of the structure reveal that PbS inorganic cores are nearly in contact through (100) NC surfaces in the square tiling of the CuAu basal plane. On the other hand, AlB2 BNSLs with PbS NCs packed in random orientations were found to be the dominant self-assembly product when the same binary NC solution was evaporated in the presence of added oleic acid (OAH). Solution nuclear magnetic resonance titration experiments confirmed that added OAH binds to PbS NCs, implicating ligand surface coverage as an important factor influencing the relative stability of CuAu and AlB2 BNSLs at the experimental size ratio. From these results, we conclude that as-prepared PbS NCs feature sparsely covered (100) surfaces and thus effectively flat patches along NC x-, y-, and z-directions. Such anisotropic PbS-PbS interactions can be efficiently screened by restoring effectively spherical NC shape via addition of OAH to the binary assembly solution. Our findings underscore the important contribution of NC surfaces to superlattice phase stability and offer a strategy for targeted BNSL assembly.

11.
J Am Chem Soc ; 141(14): 5728-5740, 2019 Apr 10.
Artigo em Inglês | MEDLINE | ID: mdl-30868880

RESUMO

The self-assembly of two sizes of spherical nanocrystals has revealed a surprisingly diverse library of structures. To date, at least 15 distinct binary nanocrystal superlattice (BNSL) structures have been identified. The stability of these binary phases cannot be fully explained using the traditional conceptual framework treating the assembly process as entropy-driven crystallization of rigid spherical particles. Such deviation from hard sphere behavior may be explained by the soft and deformable layer of ligands that envelops the nanocrystals, which contributes significantly to the overall size and shape of assembling particles. In this work, we describe a set of experiments designed to elucidate the role of the ligand corona in shaping the thermodynamics and kinetics of BNSL assembly. Using hydrocarbon-capped Au and PbS nanocrystals as a model binary system, we systematically tuned the core radius ( R) and ligand chain length ( L) of particles and subsequently assembled them into binary superlattices. The resulting database of binary structures enabled a detailed analysis of the role of effective nanocrystal size ratio, as well as softness expressed as L/ R, in directing the assembly of binary structures. This catalog of superlattices allowed us to not only study the frequency of different phases but to also systematically measure the geometric parameters of the BNSLs. This analysis allowed us to evaluate new theoretical models treating the cocrystallization of deformable spheres and to formulate new hypotheses about the factors affecting the nucleation and growth of the binary superlattices. Among other insights, our results suggest that the relative abundance of the binary phases observed may be explained not only by considerations of thermodynamic stability, but also by a postulated preordering of the binary fluid into local structures with icosahedral or polytetrahedral symmetry prior to nucleation.

12.
J Chem Phys ; 149(16): 164505, 2018 Oct 28.
Artigo em Inglês | MEDLINE | ID: mdl-30384750

RESUMO

Charge correlations in dense ionic fluids give rise to novel effects such as long-range screening and colloidal stabilization which are not predicted by the classic Debye-Hückel theory. We show that a Coulomb or charge-frustrated Ising model, which accounts for both long-range Coulomb and short-range molecular interactions, simply describes some of these ionic correlations. In particular, we obtain, at a mean field level and in simulations, a non-monotonic dependence of the screening length on the temperature. Using a combination of simulations and mean field theories, we study how the correlations in the various regimes are affected by the strength of the short ranged interactions.

13.
J Am Chem Soc ; 140(46): 15791-15803, 2018 11 21.
Artigo em Inglês | MEDLINE | ID: mdl-30285448

RESUMO

The ensemble emission spectra of colloidal InP quantum dots are broader than achievable spectra of cadmium- and lead-based quantum dots, despite similar single-particle line widths and significant efforts invested in the improvement of synthetic protocols. We seek to explain the origin of persistently broad ensemble emission spectra of colloidal InP quantum dots by investigating the nature of the electronic states responsible for luminescence. We identify a correlation between red-shifted emission spectra and anomalous broadening of the excitation spectra of luminescent InP colloids, suggesting a trap-associated emission pathway in highly emissive core-shell quantum dots. Time-resolved pump-probe experiments find that electrons are largely untrapped on photoluminescence relevant time scales pointing to emission from recombination of localized holes with free electrons. Two-dimensional electronic spectroscopy on InP quantum dots reveals multiple emissive states and increased electron-phonon coupling associated with hole localization. These localized hole states near the valence band edge are hypothesized to arise from incomplete surface passivation and structural disorder associated with lattice defects. We confirm the presence and effect of lattice disorder by X-ray absorption spectroscopy and Raman scattering measurements. Participation of localized electronic states that are associated with various classes of lattice defects gives rise to phonon-coupled defect related emission. These findings explain the origins of the persistently broad emission spectra of colloidal InP quantum dots and suggest future strategies to narrow ensemble emission lines comparable to what is observed for cadmium-based materials.

14.
Nano Lett ; 18(11): 6948-6953, 2018 11 14.
Artigo em Inglês | MEDLINE | ID: mdl-30244582

RESUMO

Excimers, a portmanteau of "excited dimer", are transient species that are formed from the electronic interaction of a fluorophore in the excited state with a neighbor in the ground state, which have found extensive use as laser gain media. Although common in molecular fluorophores, this work presents evidence for the formation of excimers in a new class of materials: atomically precise two-dimensional semiconductor nanoplatelets. Colloidal nanoplatelets of CdSe display two-color photoluminescence resolved at low temperatures with one band attributed to band-edge fluorescence and a second, red band attributed to excimer fluorescence. Previously reasonable explanations for two-color fluorescence, such as charging, are shown to be inconsistent with additional evidence. As with excimers in other materials systems, excimer emission is increased by increasing nanoplatelet concentration and the degree of cofacial stacking. Consistent with their promise as low-threshold gain media, amplified spontaneous emission emerges from the excimer emission line.

15.
J Am Chem Soc ; 140(38): 12144-12151, 2018 09 26.
Artigo em Inglês | MEDLINE | ID: mdl-30125092

RESUMO

Control of composition, stoichiometry, and defects in colloidal quantum dots (QDs) of III-V semiconductors has proven to be difficult due to their covalent character. Whereas the synthesis of colloidal indium pnictides such as InP, InAs, and InSb has made significant progress, gallium-containing colloidal III-V QDs still remain largely elusive. Gallium pnictides represent an important class of semiconductors due to their excellent optoelectronic properties in the bulk; however, the difficulty with the synthesis of gallium-containing colloidal III-V QDs has largely prohibited their exploration as solution-processed semiconductors. Here we introduce molten inorganic salts as high-temperature solvents for the synthesis and manipulation of III-V QDs. We demonstrate cation exchange reactions on presynthesized InP and InAs QDs to form In1- xGa xP and In1- xGa xAs QDs at temperatures above 380 °C. This approach produces novel ternary alloy QDs with controllable compositions that show size- and composition-dependent absorption and emission features. Emission quantum yields of up to ∼50% can be obtained for In1- xGa xP/ZnS core-shell QDs. A comparison of the optical properties of InP/ZnS core-shells with In1- xGa xP/ZnS core-shells reveals that Ga incorporation leads to significant improvement in the optical properties of III-V/II-VI core-shell emitters which is of great importance for quantum dot-based lighting and display applications. This work also demonstrates the potential of molten inorganic salts as versatile solvents for the synthesis and processing of colloidal nanomaterials at temperatures inaccessible for traditional solvents.

16.
ACS Nano ; 12(9): 9397-9404, 2018 Sep 25.
Artigo em Inglês | MEDLINE | ID: mdl-30125488

RESUMO

HgTe colloidal quantum dots (QDs) are of interest because quantum confinement of semimetallic bulk HgTe allows one to synthetically control the bandgap throughout the infrared. Here, we synthesize highly monodisperse HgTe QDs and tune their doping both chemically and electrochemically. The monodispersity of the QDs was evaluated using small-angle X-ray scattering (SAXS) and suggests a diameter distribution of ∼10% across multiple batches of different sizes. Electron-doped HgTe QDs display an intraband absorbance and bleaching of the first two excitonic features. We see splitting of the intraband peaks corresponding to electronic transitions from the occupied 1Se state to a series of nondegenerate 1Pe states. Spectroelectrochemical studies reveal that the degree of splitting and relative intensity of the intraband features remain constant across doping levels up to two electrons per QD. Theoretical modeling suggests that the splitting of the 1Pe level arises from spin-orbit coupling and reduced QD symmetry. The fine structure of the intraband transitions is observed in the ensemble studies due to the size uniformity of the as-synthesized QDs and strong spin-orbit coupling inherent to HgTe.

17.
Nano Lett ; 18(8): 4647-4652, 2018 08 08.
Artigo em Inglês | MEDLINE | ID: mdl-29985629

RESUMO

Many important light-matter coupling and energy-transfer processes depend critically on the dimensionality and orientation of optical transition dipoles in emitters. We investigate individual quasi-two-dimensional nanoplatelets (NPLs) using higher-order laser scanning microscopy and find that absorption dipoles in NPLs are isotropic in three dimensions at the excitation wavelength. Correlated polarization studies of the NPLs reveal that their emission polarization is strongly dependent on the aspect ratio of the lateral dimensions. Our simulations reveal that this emission anisotropy can be readily explained by the electric field renormalization effect caused by the dielectric contrast between the NPLs and the surrounding medium, and we conclude that emission dipoles in NPLs are isotropic in the plane of the NPLs. Our study presents an approach for disentangling the effects of dipole degeneracy and electric field renormalization on emission anisotropy and can be adapted for studying the intrinsic optical transition dipoles of various nanostructures.


Assuntos
Luminescência , Substâncias Luminescentes/química , Nanopartículas/química , Semicondutores , Anisotropia , Compostos de Cádmio/química , Simulação por Computador , Campos Eletromagnéticos , Luz , Modelos Químicos , Tamanho da Partícula , Fenômenos Físicos , Compostos de Selênio/química , Sulfetos/química , Propriedades de Superfície
18.
J Phys Chem Lett ; 9(2): 286-293, 2018 Jan 18.
Artigo em Inglês | MEDLINE | ID: mdl-29283580

RESUMO

Elevated temperature optoelectronic performance of semiconductor nanomaterials remains an important issue for applications. Here we examine 2D CdSe nanoplatelets (NPs) and CdS/CdSe/CdS shell/core/shell sandwich NPs at temperatures ranging from 300 to 700 K using static and transient spectroscopies as well as in situ transmission electron microscopy. NPs exhibit reversible changes in PL intensity, spectral position, and emission line width with temperature elevation up to ∼500 K, losing a factor of ∼8 to 10 in PL intensity at 400 K relative to ambient. Temperature elevation above ∼500 K yields thickness-dependent, irreversible degradation in optical properties. Electron microscopy relates stability of the core-only NP morphology up to 555 and 600 K for the four and five monolayer NPs, respectively, followed by sintering and evaporation at still higher temperatures. Reversible PL loss, based on differences in decay dynamics between time-resolved photoluminescence and transient absorption, results primarily from hole trapping in both NPs and sandwich NPs.

19.
Nano Lett ; 17(11): 6900-6906, 2017 11 08.
Artigo em Inglês | MEDLINE | ID: mdl-28994296

RESUMO

Nonradiative Auger recombination limits the efficiency with which colloidal semiconductor nanocrystals can emit light when they are subjected to strong excitation, with important implications for the application of the nanocrystals in light-emitting diodes and lasers. This has motivated attempts to engineer the structure of the nanocrystals to minimize Auger rates. Here, we study Auger recombination rates in CdSe/CdS core/shell nanoplatelets, or colloidal quantum wells. Using time-resolved photoluminescence measurements, we show that the rate of biexcitonic Auger recombination has a nonmonotonic dependence on the shell thickness, initially decreasing, reaching a minimum for shells with thickness of 2-4 monolayers, and then increasing with further increases in the shell thickness. This nonmonotonic behavior has not been observed previously for biexcitonic recombination in quantum dots, most likely due to inhomogeneous broadening that is not present for the nanoplatelets.

20.
ACS Nano ; 11(9): 9119-9127, 2017 09 26.
Artigo em Inglês | MEDLINE | ID: mdl-28787569

RESUMO

Quasi-two-dimensional nanoplatelets (NPLs) possess fundamentally different excitonic properties from zero-dimensional quantum dots. We study lateral size-dependent photon emission statistics and carrier dynamics of individual NPLs using second-order photon correlation (g(2)(τ)) spectroscopy and photoluminescence (PL) intensity-dependent lifetime analysis. Room-temperature radiative lifetimes of NPLs can be derived from maximum PL intensity periods in PL time traces. It first decreases with NPL lateral size and then stays constant, deviating from the electric dipole approximation. Analysis of the PL time traces further reveals that the single exciton quantum yield in NPLs decreases with NPL lateral size and increases with protecting shell thickness, indicating the importance of surface passivation on NPL emission quality. Second-order photon correlation (g(2)(τ)) studies of single NPLs show that the biexciton quantum yield is strongly dependent on the lateral size and single exciton quantum yield of the NPLs. In large NPLs with unity single exciton quantum yield, the corresponding biexciton quantum yield can reach unity. These findings reveal that by careful growth control and core-shell material engineering, NPLs can be of great potential for light amplification and integrated quantum photonic applications.

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