Berkeley Lab researchers uncover hidden structures in domain interfaces that hamper performance
Organic semiconductors are prized for light emitting diodes (LEDs), field effect transistors (FETs) and photovoltaic cells. As they can be printed from solution, they provide a highly scalable, cost-effective alternative to silicon-based devices. Uneven performances, however, have been a persistent problem. Scientists have known that the performance issues originate in the domain interfaces within organic semiconductor thin films, but have not known the cause. This mystery now appears to have been solved.
Naomi Ginsberg, a faculty chemist with the U.S. Department of Energy (DOE)'s Lawrence Berkeley National Laboratory and the University of California (UC) Berkeley, led a team that used a unique form of microscopy to study the domain interfaces within an especially high-performing solution-processed organic semiconductor called TIPS-pentacene. She and her team discovered a cluttered jumble of randomly oriented nanocrystallites that become kinetically trapped in the interfaces during solution casting. Like debris on a highway, these nanocrystallites impede the flow of charge-carriers.
"If the interfaces were neat and clean, they wouldn't have such a large impact on performance, but the presence of the nanocrystallites reduces charge-carrier mobility," Ginsberg says. "Our nanocrystallite model for the interface, which is consistent with observations, provides critical information that can be used to correlate solution-processing methods to optimal device performances."
Ginsberg, who holds appointments with Berkeley Lab's Physical Biosciences Division and its Materials Sciences Division, as well as UC Berkeley's departments of chemistry and physics, is the corresponding author of a paper describing this research in Nature Communications. The paper is titled "Exciton dynamics reveals aggregates with intermolecular order at hidden interfaces in solution-cast organic semiconducting films." Co-authors are Cathy Wong, Benjamin Cotts and Hao Wu.
Organic semiconductors are based on the ability of carbon to form larger molecules, such as benzene and pentacene, featuring electrical conductivity that falls somewhere between insulators and metals. Through solution-processing, organic materials can usually be fashioned into crystalline films without the expensive high-temperature annealing process required for silicon and other inorganic semiconductors. However, even though it has long been clear that the crystalline domain interfaces within semiconductor organic thin films are critical to their performance in devices, detailed information on the morphology of these interfaces has been missing until now.
"Interface domains in organic semiconductor thin films are smaller than the diffraction limit, hidden from surface probe techniques such as atomic force microscopy, and their nanoscale heterogeneity is not typically resolved using X-ray methods," Ginsberg says. "Furthermore, the crystalline TIPS-pentacene we studied has virtually zero emission, which means it can't be studied with photoluminescence microscopy."
Ginsberg and her group overcame the challenges by using transient absorption (TA) microscopy, a technique in which femtosecond laser pulses excite transient energy states and detectors measure the changes in the absorption spectra. The Berkeley researchers carried out TA microscopy on an optical microscope they constructed themselves that enabled them to generate focal volumes that are a thousand times smaller than is typical for conventional TA microscopes. They also deployed multiple different light polarizations that allowed them to isolate interface signals not seen in either of the adjacent domains.
"Instrumentation, including very good detectors, the painstaking collection of data to ensure good signal-to-noise ratios, and the way we crafted the experiment and analysis were all critical to our success," Ginsberg says. "Our spatial resolution and light polarization sensitivity were also essential to be able to unequivocally see a signature of the interface that was not swamped by the bulk, which contributes much more to the raw signal by volume."
The methology developed by Ginsberg and her team to uncover structural motifs at hidden interfaces in organic semiconductor thin films should add a predictive factor to scalable and affordable solution-processing of these materials. This predictive capability should help minimize discontinuities and maximize charge-carrier mobility. Currently, researchers use what is essentially a trial-and-error approach, in which different solution casting conditions are tested to see how well the resulting devices perform.
"Our methodology provides an important intermediary in the feedback loop of device optimization by characterizing the microscopic details of the films that go into the devices, and by inferring how the solution casting could have created the structures at the interfaces," Ginsberg says. "As a result, we can suggest how to alter the delicate balance of solution casting parameters to make more functional films."
This research was primarily funded by the Defense Advanced Research Projects Agency.
Lawrence Berkeley National Laboratory addresses the world's most urgent scientific challenges by advancing sustainable energy, protecting human health, creating new materials, and revealing the origin and fate of the universe. Founded in 1931, Berkeley Lab's scientific expertise has been recognized with 13 Nobel prizes. The University of California manages Berkeley Lab for the U.S. Department of Energy's Office of Science. For more, visit http://www.
Lynn Yarris | EurekAlert!
Transporting spin: A graphene and boron nitride heterostructure creates large spin signals
16.08.2017 | Graphene Flagship
From hot to cold: How to move objects at the nanoscale
10.08.2017 | Scuola Internazionale Superiore di Studi Avanzati
Physicists at the University of Bonn have managed to create optical hollows and more complex patterns into which the light of a Bose-Einstein condensate flows. The creation of such highly low-loss structures for light is a prerequisite for complex light circuits, such as for quantum information processing for a new generation of computers. The researchers are now presenting their results in the journal Nature Photonics.
Light particles (photons) occur as tiny, indivisible portions. Many thousands of these light portions can be merged to form a single super-photon if they are...
For the first time, scientists have shown that circular RNA is linked to brain function. When a RNA molecule called Cdr1as was deleted from the genome of mice, the animals had problems filtering out unnecessary information – like patients suffering from neuropsychiatric disorders.
While hundreds of circular RNAs (circRNAs) are abundant in mammalian brains, one big question has remained unanswered: What are they actually good for? In the...
An experimental small satellite has successfully collected and delivered data on a key measurement for predicting changes in Earth's climate.
The Radiometer Assessment using Vertically Aligned Nanotubes (RAVAN) CubeSat was launched into low-Earth orbit on Nov. 11, 2016, in order to test new...
A study led by scientists of the Max Planck Institute for the Structure and Dynamics of Matter (MPSD) at the Center for Free-Electron Laser Science in Hamburg presents evidence of the coexistence of superconductivity and “charge-density-waves” in compounds of the poorly-studied family of bismuthates. This observation opens up new perspectives for a deeper understanding of the phenomenon of high-temperature superconductivity, a topic which is at the core of condensed matter research since more than 30 years. The paper by Nicoletti et al has been published in the PNAS.
Since the beginning of the 20th century, superconductivity had been observed in some metals at temperatures only a few degrees above the absolute zero (minus...
Researchers from the University of Miami (UM) Rosenstiel School of Marine and Atmospheric Science, the Italian Space Agency (ASI), and the Instituto Geofisico--Escuela Politecnica Nacional (IGEPN) of Ecuador, showed an increasing volcanic danger on Cotopaxi in Ecuador using a powerful technique known as Interferometric Synthetic Aperture Radar (InSAR).
The Andes region in which Cotopaxi volcano is located is known to contain some of the world's most serious volcanic hazard. A mid- to large-size eruption has...
16.08.2017 | Event News
04.08.2017 | Event News
26.07.2017 | Event News
16.08.2017 | Physics and Astronomy
16.08.2017 | Materials Sciences
16.08.2017 | Interdisciplinary Research