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1.
Nano Lett ; 2020 Jul 08.
Artigo em Inglês | MEDLINE | ID: mdl-32574069

RESUMO

Using circularly polarized broadband transient absorption, time-resolved circular photoluminescence, and transient Faraday rotation spectroscopy, we report that spin-dependent interactions have a significant impact on exciton energies and spin depolarization times in layered Ruddlesden-Popper hybrid metal-halide perovskites. In BA2FAPb2I7, we report that room-temperature spin lifetimes are largest (3.2 ps) at a carrier density of ∼1017 cm-3 with increasing depolarization rates at higher exciton densities. This indicates that many-body interactions reduce spin-lifetimes and outcompete the effect of D'yakonov-Perel precessional relaxation that has been previously reported at lower carrier densities. We further observe a dynamic circular dichroism that arises from a photoinduced polarization in the exciton distribution between total angular momentum states. Our findings provide fundamental and application relevant insights into the spin-dependent exciton-exciton interactions in layered hybrid perovskites.

2.
Adv Mater ; 31(42): e1902374, 2019 Oct.
Artigo em Inglês | MEDLINE | ID: mdl-31489713

RESUMO

Mixed-halide lead perovskites have attracted significant attention in the field of photovoltaics and other optoelectronic applications due to their promising bandgap tunability and device performance. Here, the changes in photoluminescence and photoconductance of solution-processed triple-cation mixed-halide (Cs0.06 MA0.15 FA0.79 )Pb(Br0.4 I0.6 )3 perovskite films (MA: methylammonium, FA: formamidinium) are studied under solar-equivalent illumination. It is found that the illumination leads to localized surface sites of iodide-rich perovskite intermixed with passivating PbI2 material. Time- and spectrally resolved photoluminescence measurements reveal that photoexcited charges efficiently transfer to the passivated iodide-rich perovskite surface layer, leading to high local carrier densities on these sites. The carriers on this surface layer therefore recombine with a high radiative efficiency, with the photoluminescence quantum efficiency of the film under solar excitation densities increasing from 3% to over 45%. At higher excitation densities, nonradiative Auger recombination starts to dominate due to the extremely high concentration of charges on the surface layer. This work reveals new insight into phase segregation of mixed-halide mixed-cation perovskites, as well as routes to highly luminescent films by controlling charge density and transfer in novel device structures.

3.
Nano Lett ; 19(9): 6577-6584, 2019 Sep 11.
Artigo em Inglês | MEDLINE | ID: mdl-31448620

RESUMO

We report smart color-sensing devices of two-dimensional lead halide perovskites that exhibit a graded band gap across the film. We observe that the device short-circuit photocurrent is strongly dependent on excitation wavelength λ, and this arises through photoabsorption at different depths in the sample due to the graded bandgaps present. This λ signature in the response of the device is observed in case of steady-state excitation when incident from the high bandgap side of the film, where a complete reversal in the polarity of the photocurrent Iph(t) is obtained as the excitation wavelength is spanned across the visible spectrum. The transient photocurrent reveals λ-specific response arrived from a combination of positive and negative Iph(t) components. The uniqueness of Iph(t) as a function of incident λ can be utilized to examine spectral purity without dispersive optical elements. An equivalent circuit model description provides a possible glimpse into the physical sources involved in contributing to these features.

4.
J Phys Chem Lett ; 9(18): 5604-5611, 2018 Sep 20.
Artigo em Inglês | MEDLINE | ID: mdl-30149711

RESUMO

Ultrafast vibrational spectroscopy is employed to obtain real-time structural information on energy transport in double-walled light-harvesting nanotubes at room temperature, stabilized in a host matrix to mimic the rigid scaffolds of natural light-harvesting systems. We observe evidence of a low-frequency vibrational mode at 315 cm-1, which transfers excitons from the outer wall of the nanotubes to a crossing point through which energy transfer to the inner wall can occur. This mode is furthermore absent in solution phase. Importantly, the coherence of this mode is not transferred to the inner wall upon energy transfer and is only present on the outer wall's excited-state energy surface, highlighting that complete energy transfer between the outer and inner walls does not take place. Isolation of the individual walls of the nanotubes provides evidence that this mode corresponds to a supramolecular motion of the nanotubes. Our results emphasize the importance of the solid-state environment in modulating vibronic coupling and directing energy transfer in molecular light-harvesting systems.

5.
Science ; 360(6396): 1442-1446, 2018 06 29.
Artigo em Inglês | MEDLINE | ID: mdl-29954975

RESUMO

The highest power conversion efficiencies (PCEs) reported for perovskite solar cells (PSCs) with inverted planar structures are still inferior to those of PSCs with regular structures, mainly because of lower open-circuit voltages (Voc). Here we report a strategy to reduce nonradiative recombination for the inverted devices, based on a simple solution-processed secondary growth technique. This approach produces a wider bandgap top layer and a more n-type perovskite film, which mitigates nonradiative recombination, leading to an increase in Voc by up to 100 millivolts. We achieved a high Voc of 1.21 volts without sacrificing photocurrent, corresponding to a voltage deficit of 0.41 volts at a bandgap of 1.62 electron volts. This improvement led to a stabilized power output approaching 21% at the maximum power point.

6.
ACS Nano ; 11(11): 10834-10843, 2017 11 28.
Artigo em Inglês | MEDLINE | ID: mdl-29064668

RESUMO

Self-assembled hybrid perovskite quantum wells have attracted attention due to their tunable emission properties, ease of fabrication, and device integration. However, the dynamics of excitons in these materials, especially how they couple to phonons, remains an open question. Here, we investigate two widely used materials, namely, butylammonium lead iodide (CH3(CH2)3NH3)2PbI4 and hexylammonium lead iodide (CH3(CH2)5NH3)2PbI4, both of which exhibit broad photoluminescence tails at room temperature. We performed femtosecond vibrational spectroscopy to obtain a real-time picture of the exciton-phonon interaction and directly identified the vibrational modes that couple to excitons. We show that the choice of the organic cation controls which vibrational modes the exciton couples to. In butylammonium lead iodide, excitons dominantly couple to a 100 cm-1 phonon mode, whereas in hexylammonium lead iodide, excitons interact with phonons with frequencies of 88 and 137 cm-1. Using the determined optical phonon energies, we analyzed photoluminescence broadening mechanisms. At low temperatures (<100 K), the broadening is due to acoustic phonon scattering, whereas at high temperatures, LO phonon-exciton coupling is the dominant mechanism. Our results help explain the broad photoluminescence line shape observed in hybrid perovskite quantum wells and provide insights into the mechanism of exciton-phonon coupling in these materials.

7.
Nano Lett ; 16(12): 7974-7981, 2016 12 14.
Artigo em Inglês | MEDLINE | ID: mdl-27960450

RESUMO

One-dimensional nanoscale epitaxial arrays serve as a great model in studying fundamental physics and for emerging applications. With an increasing focus laid on the Cs-based inorganic halide perovskite out of its outstanding material stability, we have applied vapor phase epitaxy to grow well aligned horizontal CsPbX3 (X: Cl, Br, or I or their mixed) nanowire arrays in large scale on mica substrate. The as-grown nanowire features a triangular prism morphology with typical length ranging from a few tens of micrometers to a few millimeters. Structural analysis reveals that the wire arrays follow the symmetry of mica substrate through incommensurate epitaxy, paving a way for a universally applicable method to grow a broad family of halide perovskite materials. The unique photon transport in the one-dimensional structure has been studied in the all-inorganic Cs-based perovskite wires via temperature dependent and spatially resolved photoluminescence. Epitaxy of well oriented wire arrays in halide perovskite would be a promising direction for enabling the circuit-level applications of halide perovskite in high-performance electro-optics and optoelectronics.

8.
ACS Appl Mater Interfaces ; 7(44): 24876-86, 2015 Nov 11.
Artigo em Inglês | MEDLINE | ID: mdl-26480854

RESUMO

Perylene diimide (PDI)-based organic photovoltaic devices can potentially deliver high power conversion efficiency values provided the photon energy absorbed is utilized efficiently in charge transfer (CT) reactions instead of being consumed in nonradiative energy transfer (ET) steps. Hitherto, it remains unclear whether ET or CT primarily drives the photoluminescence (PL) quenching of the PDI excimer state in PDI-based blend films. Here, we affirm the key role of the thermally assisted PDI excimer diffusion and subsequent CT reaction in the process of PDI excimer PL deactivation. For our study we perform PL quenching experiments in the model PDI-based composite made of poly[4,8-bis(5-(2-ethylhexyl)thiophen-2-yl)benzo[1,2-b;4,5-b']dithiophene-2,6-diyl-alt-(4-(2-ethylhexanoyl)-thieno[3,4-b]thiophene)-2-6-diyl] (PBDTTT-CT) polymeric donor mixed with the N,N'-bis(1-ethylpropyl)-perylene-3,4,9,10-tetracarboxylic diimide (PDI) acceptor. Despite the strong spectral overlap between the PDI excimer PL emission and UV-vis absorption of PBDTTT-CT, two main observations indicate that no significant ET component operates in the overall PL quenching: the PL intensity of the PDI excimer (i) increases with decreasing temperature and (ii) remains unaffected even in the presence of 10 wt % content of the PBDTTT-CT quencher. Temperature-dependent wide-angle X-ray scattering experiments further indicate that nonradiative resonance ET is highly improbable due to the large size of PDI domains. The dominance of the CT over the ET process is verified by the high performance of devices with an optimum composition of 30:70 PBDTTT-CT:PDI. By adding 0.4 vol % of 1,8-diiodooctane we verify the plasticization of the polymer side chains that balances the charge transport properties of the PBDTTT-CT:PDI composite and results in additional improvement in the device efficiency. The temperature-dependent spectral width of the PDI excimer PL band suggests the presence of energetic disorder in the PDI excimer excited state manifold.

9.
J Phys Chem Lett ; 6(1): 201-5, 2015 Jan 02.
Artigo em Inglês | MEDLINE | ID: mdl-26263114

RESUMO

We report a comparison of charge carrier dynamics and device performance for low band gap polymer PBDTTT-CT in blends with the fullerene acceptor PC71BM and a PDI derivative with similar electron affinities. Charge separation and recombination dynamics are found to be remarkably similar for these two acceptors, with both blends exhibiting efficient, ultrafast charge separation (time constants of 1.6 and 1.4 ps, respectively). The lower device performance for the PDI acceptor (1.75% compared to 3.5% for the equivalent PC71BM device) is shown to result from slower charge transport, increasing nongeminate recombination losses during charge collection.

10.
J Phys Chem Lett ; 3(17): 2405-8, 2012 Sep 06.
Artigo em Inglês | MEDLINE | ID: mdl-26292123

RESUMO

Perylene diimides (PDIs) are attractive alternatives to fullerenes as electron transporters because of their optoelectronic properties, durability, and ease of synthesis. Belying this promise, devices that utilize PDIs as electron acceptors have low efficiencies. The primary deficiency in such cells is the low short circuit current density (JSC), which is traceable to the crystallinity of PDIs. Therefore, disrupting the crystallinity without adversely impacting the charge-transfer properties of PDIs is proposed as an important design principle. This has been achieved using a nonplanar perylene. In combination with a hole transporting polymer, a device efficiency of 2.77% has been achieved. A 10-fold increase in JSC is observed in comparison with a planar PDI, resulting in one of the highest JSC values for a solution processed device featuring a PDI. Indeed, this is one of the highest efficiencies for devices featuring a nonfullerene as the electron transporter.

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