Controlling and Optimizing Amplified Spontaneous Emission in Perovskites.

Perovskites are currently attracting extensive research interest as a wavelength-tunable lasing material. As a first step toward electrically pumped lasers, numerous investigations have recently reported amplified spontaneous emission (ASE) of optically pumped perovskites with remarkably low thresholds. Here, we investigate the optical aspects of perovskite ASE, to establish the design principle of materials and devices. We show that compared to solution-processed CsPbBr3, vacuum deposition yields superior ASE characteristics with a threshold of 35 µJ/cm2. The optical loss (Rloss) during lateral photon propagation in the waveguide mode is identified as a key parameter to determine the ASE quality. With spatially resolved photoluminescence, we determine Rloss as 40 and >1000 cm-1 for vacuum and solution-processed perovskites, respectively. We present a comprehensive model that relates ASE, gain length, optical loss, temperature, and density of states. Finally, we succeed in demonstrating ASE in perovskite samples with metal electrodes, mimicking a diode architecture for electrical pumping. Optical spacer layers are shown to play a crucial role in preventing metal absorption loss in waveguide modes.

Organic narrowband near-infrared photodetectors based on intermolecular charge-transfer absorption.

Blending organic electron donors and acceptors yields intermolecular charge-transfer states with additional optical transitions below their optical gaps. In organic photovoltaic devices, such states play a crucial role and limit the operating voltage. Due to its extremely weak nature, direct intermolecular charge-transfer absorption often remains undetected and unused for photocurrent generation. Here, we use an optical microcavity to increase the typically negligible external quantum efficiency in the spectral region of charge-transfer absorption by more than 40 times, yielding values over 20%. We demonstrate narrowband detection with spectral widths down to 36 nm and resonance wavelengths between 810 and 1,550 nm, far below the optical gap of both donor and acceptor. The broad spectral tunability via a simple variation of the cavity thickness makes this innovative, flexible and potentially visibly transparent device principle highly suitable for integrated low-cost spectroscopic near-infrared photodetection.

Optical display film as flexible and light trapping substrate for organic photovoltaics.

We demonstrate flexible small molecular solar cells on periodically patterned plastic substrate (LCD display film) using a highly transparent poly(3,4-ethylenedioxythiophene):poly(styrenesulfonate) ( PEDOT: PSS) electrode with flexible thin atomic layer deposited (ALD) AlOx top and bottom encapsulation. The organic photovoltaic device (OPV) on this display film shows a power conversion efficiency of 7.48%, which is a 13.0% improvement as compared to a device fabricated on a planar poly-ethylen-terephtalate (PET) substrate (6.62%) and even higher than the efficiency of a device using planar glass substrate (7.15%). The improvement is mainly due to an enhanced harvesting of photons with wavelengths shorter than 500 nm. Moreover, the fully encapsulated device is sufficiently flexible to withstand a bending with a 10 mm radius for more than 50 cycles at ambient condition. These results indicate that the use of standard optical display films is a cheap, simple and efficient way to increase the photocurrent and overall efficiency of organic photovoltaic devices.

Importance of Interface Diffusion and Climate in Defect Dominated Moisture Ultrabarrier Applications.

OLEDs and organic photovoltaic (OPV) devices require encapsulation from water vapor using a permeation barrier system. As a benchmark for barrier quality, often only a single number is provided as water vapor transmission rate. However, this value is highly dependent on the aging climate. So far, little scientific effort has been undertaken to characterize ultrahigh moisture barriers at different temperatures and relative humidities. We present Ca-test studies on sputtered Zinc-Tin-Oxide and atomic layer deposited AlOx barriers in extensively varied climates. Relative humidities are changed at constant temperatures, and temperatures are changed at constant absolute humidity. We find Henry's law to apply for sorption and discover a fundamental change of the diffusion regime with time related to the interface between the test and the barrier thin-film.

Degradation of Flexible, ITO-Free Oligothiophene Organic Solar Cells.

We investigate the degradation of organic solar cells based on an oligothiophene (DCV5T-Me) small molecule donor and the acceptor C60. Two different flexible, transparent bottom electrode types are employed: a transparent metal electrode (TME) and silver nanowires (AgNWs). They exhibit high optical transparency up to 86% and a sheet resistance as low as 12Ω/□. Power conversion efficiencies of 7.0%, 5.7%, and 7.2% on TME, AgNWs, and indium tin oxide (ITO, reference) are reached, respectively. The solar cells are protected against moisture ingress utilizing a flexible alumina thin-film, exhibiting water vapor transmission rates down to 3 × 10(-5) g m(-2) day(-1) at 38 °C and 90% relative humidity (RH). Implementation of this ultrabarrier as top and bottom encapsulation enables fabrication of fully flexible devices. A decrease in PCE to 80% of initial values is observed after 1000 ± 50 h on flexible, encapsulated TME but only 20 ± 5 h on AgNWs in a climate of 38 °C/50% RH. Degradation in AgNW-based devices is attributed to electrode decomposition.

Breakdown and Protection of ALD Moisture Barrier Thin Films.

The water vapor barrier properties of low-temperature atomic layer deposited (ALD) AlOx thin-films are observed to be unstable if exposed directly to high or even ambient relative humidities. Upon exposure to humid atmospheres, their apparent barrier breaks down and their water vapor transmission rates (WVTR), measured by electrical calcium tests, deteriorate by several orders of magnitude. These changes are accompanied by surface roughening beyond the original thickness, observed by atomic force microscopy. X-ray reflectivity investigations show a strong decrease in density caused by only 5 min storage in a 38 °C, 90% relative humidity climate. We show that barrier stabilities required for device applications can be achieved by protection layers which prevent the direct contact of water condensing on the surface, i.e., the sensitive ALD barrier. Nine different protection layers of either ALD materials or polymers are tested on the barriers. Although ALD materials prove to be ineffective, applied polymers seem to provide good protection independent of thickness, surface free energy, and deposition technique. A glued-on PET foil stands out as a low-cost, easily processed, and especially stable solution. This way, 20 nm single layer ALD barriers for organic electronics are measured. They yield reliable WVTRs down to 2×10(-5) g(H2O) m(-2) day(-1) at 38 °C and 90% relative humidity, highlighting the great potential of ALD encapsulation.