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3.
Nature ; 573(7774): 394-397, 2019 09.
Artigo em Inglês | MEDLINE | ID: mdl-31501570

RESUMO

Organic photovoltaic cells are now approaching commercially viable efficiencies, particularly for applications that make use of their unique potential for flexibility and semitransparency1-3. However, their reliability remains a major concern, as even the most stable devices reported so far degrade within only a few years4-8. This has led to the belief that short operational lifetimes are an intrinsic disadvantage of devices that are fabricated using weakly bonded organic materials-an idea that persists despite the rapid growth and acceptance of organic light-emitting devices, which can achieve lifetimes of several million hours9. Here we study an extremely stable class of thermally evaporated single-junction organic photovoltaic cells. We accelerated the ageing process by exposing the packaged cells to white-light illumination intensities of up to 37 Suns. The cells maintained more than 87 per cent of their starting efficiency after exposure for more than 68 days. The degradation rate increases superlinearly with intensity, leading to an extrapolated intrinsic lifetime, T80, of more than 4.9 × 107 hours, where T80 is the time taken for the power conversion efficiency to decrease to 80 per cent of its initial value. This is equivalent to 27,000 years outdoors. Additionally, we subjected a second group of organic photovoltaic cells to 20 Suns of ultraviolet illumination (centred at 365 nanometres) for 848 hours, a dose that would take 1.7 × 104 hours (9.3 years) to accumulate outdoors. No efficiency loss was observed over the duration of the test. Overall, we find that organic solar cells packaged in an inert atmosphere can be extremely stable, which is promising for their future use as a practical energy-generation technology.

4.
Proc Natl Acad Sci U S A ; 116(10): 3968-3973, 2019 03 05.
Artigo em Inglês | MEDLINE | ID: mdl-30755534

RESUMO

Optoelectronic circuits in 3D shapes with large deformations can offer additional functionalities inaccessible to conventional planar electronics based on 2D geometries constrained by conventional photolithographic patterning processes. A light-sensing focal plane array (FPA) used in imagers is one example of a system that can benefit from fabrication on curved surfaces. By mimicking the hemispherical shape of the retina in the human eye, a hemispherical FPA provides a low-aberration image with a wide field of view. Due to the inherently high value of such applications, intensive efforts have been devoted to solving the problem of transforming a circuit fabricated on a flat wafer surface to an arbitrary shape without loss of performance or distorting the linear layouts that are the natural product of this fabrication paradigm. Here we report a general approach for fabricating electronic circuits and optoelectronic devices on nondevelopable surfaces by introducing shear slip of thin-film circuit components relative to the distorting substrate. In particular, we demonstrate retina-like imagers that allow for a topological transformation from a plane to a hemisphere without changing the relative positions of the pixels from that initially laid out on a planar surface. As a result, the resolution of the imager, particularly in the foveal region, is not compromised by stretching or creasing that inevitably results in transforming a 2D plane into a 3D geometry. The demonstration provides a general strategy for realizing high-density integrated circuits on randomly shaped, nondevelopable surfaces.

5.
J Am Chem Soc ; 141(8): 3576-3588, 2019 Feb 27.
Artigo em Inglês | MEDLINE | ID: mdl-30768250

RESUMO

A series of six luminescent two-coordinate Cu(I) complexes were investigated bearing nonconventional N-heterocyclic carbene ligands, monoamido-aminocarbene (MAC*) and diamidocarbene (DAC*), along with carbazolyl (Cz) as well as mono- and dicyano-substituted Cz derivatives. The emission color can be systematically varied over 270 nm, from violet to red, through proper choice of the acceptor (carbene) and donor (carbazolyl) groups. The compounds exhibit photoluminescent quantum efficiencies up to 100% in fluid solution and polystyrene films with short decay lifetimes (τ ≈ 1 µs). The radiative rate constants for the Cu(I) complexes ( kr = 105-106 s-1) are comparable to state of the art phosphorescent emitters with noble metals such as Ir and Pt. All complexes show strong solvatochromism due to the large dipole moment of the ground states and the transition dipole moment that is in the opposite direction. Temperature-dependent studies of (MAC*)Cu(Cz) reveal a small energy separation between the lowest singlet and triplet states (Δ ES1-T1 = 500 cm-1) and an exceptionally large zero-field splitting (ZFS = 85 cm-1). Organic light-emitting diodes (OLEDs) fabricated with (MAC*)Cu(Cz) as a green emissive dopant have high external quantum efficiencies (EQE = 19.4%) and brightness of 54 000 cd/m2 with modest roll-off at high currents. The complex can also serve as a neat emissive layer to make highly efficient OLEDs (EQE = 16.3%).

6.
Nature ; 554(7690): 77-80, 2018 02 01.
Artigo em Inglês | MEDLINE | ID: mdl-29342132

RESUMO

The unique properties of organic semiconductors, such as flexibility and lightness, are increasingly important for information displays, lighting and energy generation. But organics suffer from both static and dynamic disorder, and this can lead to variable-range carrier hopping, which results in notoriously poor electrical properties, with low electron and hole mobilities and correspondingly short charge-diffusion lengths of less than a micrometre. Here we demonstrate a photoactive (light-responsive) organic heterostructure comprising a thin fullerene channel sandwiched between an electron-blocking layer and a blended donor:C70 fullerene heterojunction that generates charges by dissociating excitons. Centimetre-scale diffusion of electrons is observed in the fullerene channel, and this can be fitted with a simple electron diffusion model. Our experiments enable the direct measurement of charge diffusivity in organic semiconductors, which is as high as 0.83 ± 0.07 square centimetres per second in a C60 channel at room temperature. The high diffusivity of the fullerene combined with the extraordinarily long charge-recombination time yields diffusion lengths of more than 3.5 centimetres, orders of magnitude larger than expected for an organic system.

7.
Nat Commun ; 8: 15566, 2017 05 31.
Artigo em Inglês | MEDLINE | ID: mdl-28561028

RESUMO

Since their introduction over 15 years ago, the operational lifetime of blue phosphorescent organic light-emitting diodes (PHOLEDs) has remained insufficient for their practical use in displays and lighting. Their short lifetime results from annihilation between high-energy excited states, producing energetically hot states (>6.0 eV) that lead to molecular dissociation. Here we introduce a strategy to avoid dissociative reactions by including a molecular hot excited state manager within the device emission layer. Hot excited states transfer to the manager and rapidly thermalize before damage is induced on the dopant or host. As a consequence, the managed blue PHOLED attains T80=334±5 h (time to 80% of the 1,000 cd m-2 initial luminance) with a chromaticity coordinate of (0.16, 0.31), corresponding to 3.6±0.1 times improvement in a lifetime compared to conventional, unmanaged devices. To our knowledge, this significant improvement results in the longest lifetime for such a blue PHOLED.

8.
Opt Lett ; 41(4): 689-92, 2016 Feb 15.
Artigo em Inglês | MEDLINE | ID: mdl-26872164

RESUMO

We present calibrated measurements of single-photon Thomson scattering from free electrons driven by a laser with intensity 1018 W/cm2. The measurements demonstrate that individual electrons radiate with the strength of point emitters, even when their wave packets spread to the scale of the driving-laser wavelength. The result agrees with predictions of quantum electrodynamics.

9.
Nat Mater ; 15(1): 92-8, 2016 Jan.
Artigo em Inglês | MEDLINE | ID: mdl-26480228

RESUMO

The combination of both very high brightness and deep blue emission from phosphorescent organic light-emitting diodes (PHOLED) is required for both display and lighting applications, yet so far has not been reported. A source of this difficulty is the absence of electron/exciton blocking layers (EBL) that are compatible with the high triplet energy of the deep blue dopant and the high frontier orbital energies of hosts needed to transport charge. Here, we show that N-heterocyclic carbene (NHC) Ir(III) complexes can serve as both deep blue emitters and efficient hole-conducting EBLs. The NHC EBLs enable very high brightness (>7,800 cd m(-2)) operation, while achieving deep blue emission with colour coordinates of [0.16, 0.09], suitable for most demanding display applications. We find that both the facial and the meridional isomers of the dopant have high efficiencies that arise from the unusual properties of the NHC ligand-that is, the complexes possess a strong metal-ligand bond that destabilizes the non-radiative metal-centred ligand-field states. Our results represent an advance in blue-emitting PHOLED architectures and materials combinations that meet the requirements of many critical illumination applications.

10.
Nat Commun ; 6: 8947, 2015 Dec 02.
Artigo em Inglês | MEDLINE | ID: mdl-26626796

RESUMO

Metal-free organic phosphorescent materials are attractive alternatives to the predominantly used organometallic phosphors but are generally dimmer and are relatively rare, as, without heavy-metal atoms, spin-orbit coupling is less efficient and phosphorescence usually cannot compete with radiationless relaxation processes. Here we present a general design rule and a method to effectively reduce radiationless transitions and hence greatly enhance phosphorescence efficiency of metal-free organic materials in a variety of amorphous polymer matrices, based on the restriction of molecular motions in the proximity of embedded phosphors. Covalent cross-linking between phosphors and polymer matrices via Diels-Alder click chemistry is devised as a method. A sharp increase in phosphorescence quantum efficiency is observed in a variety of polymer matrices with this method, which is ca. two to five times higher than that of phosphor-doped polymer systems having no such covalent linkage.

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