Physical Science and Engineering | Physical Science & Engineering

Thursday, October 22, 2020

Perovskite LEDs embrace their flaws.

Chemical treatments enable low-cost light sources to emit specific colors on demand.

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Small flaws found within a new type of light-emitting diode (LED) crystal can play outsized roles in switching their output from white light to pure colors, a KAUST study has found.

Two-dimensional (2D) perovskites are hybrid inorganic/organic materials that can trap electrons inside their slab-like structures. Researchers have shown that by choosing organic layers with different sizes and insulating strengths, the confined electrons can stimulate emission of light in narrow spectral bands. This approach enables the fabrication of LEDs that emit high-purity colors with modest manufacturing costs.

Occasionally, however, the colors emanating from 2D perovskites become swamped behind a broad spectrum of white light. This competition between different light emissions has puzzled scientists: while some studies indicate it arises from photoinduced deformation of the layered structure, others argue that small crystal defects are to blame.

“It’s difficult to verify which of the proposed mechanisms is correct,” explains Jun Yin, a researcher in Omar Mohammed’s group. “Both produce similar photoluminescence features, and sometimes they can co-exist in the same crystal.”

Most LED crystals are produced through slow cooling processes, but the final structures of 2D perovskites depend on complex interactions between solvent molecules and precursor compounds. Yin, along with colleagues at KAUST and the University of Arizona in the United States, realized that this unique crystallization process could help them produce a critical piece of evidence—a perovskite without defects—needed to understand broadband emissions.

By targeting perovskites containing lead salts, the team used their chemical knowledge to create two kinds of 2D layers. Crystallizing the materials from a lead iodide precursor produced large anionic byproducts that reacted with the perovskite, leaving vacant sites in the lattice. However, when lead oxides were used to assemble perovskites with low defect levels, no such damaging anions were observed.

Luminescent measurement experiments confirmed that only the lead-oxide-based synthesis produced LEDs with narrow spectral light; the defect-ridden samples had cross-emission problems. Through computational screening of the possible types of defects, the researchers identified iodine vacancies as the prime origin of broadband light.

To verify their theoretical predictions, the researchers added an excess of iodine and organic ring components to a defect-filled sample and saw an immediate suppression of broadband emissions. “This finding provides physical insights into how to control the optical behaviors of 2D-perovskite structures,” says Mohammed, “and points the way toward next-generation LEDs with highly efficient narrowband emissions.”

-KAUST Discovery

Sunday, October 11, 2020

Nanomaterial acts as a molecular thermometer.

A two-dimensional material mimics the human temperature-sensing system.

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A layered material developed by KAUST researchers can act as a precise temperature sensor by exploiting the same principle used in biological ion channels.

Human cells possess various proteins that act as channels for charged ions. In the skin, certain ion channels rely on heat to drive a flow of ions that generates electrical signals, which we use to sense the temperature of our surroundings.

Inspired by these biological sensors, KAUST researchers prepared a titanium carbide compound (Ti3C2Tx) known as an MXene, which contains multiple layers just a few atoms thick. Each layer is covered with negatively charged atoms, such as oxygen or fluorine. “These groups act as spacers to keep neighboring nanosheets apart, allowing water molecules to enter the interplanar channels,” says KAUST postdoc Seunghyun Hong, part of the team behind the new temperature sensor. The channels between the MXene layers are narrower than a single nanometer.

The researchers used techniques, such as X-ray diffraction and scanning electron microscopy, to investigate their MXene, and they found that adding water to the material slightly widened the channels between layers. When the material touched a solution of potassium chloride, these channels were large enough to allow positive potassium ions to move through the MXene, but blocked the passage of negative chloride ions.

A temperature difference between two ends of an MXene nanochannel causes water and potassium ions to flow from the cool side to the warm side (top). When sunlight heats just one part of an MXene device, a thermo-osmotic flow generates a voltage that can indicate tiny temperature changes (bottom).

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The team created a small device containing the MXene and exposed one end of it to sunlight. MXenes are particularly efficient at absorbing sunlight and converting that energy into heat. The resulting temperature rise prompted water molecules and potassium ions to flow through the nanochannels from the cooler end to the warmer part, an effect known as thermo-osmotic flow. This caused a voltage change comparable to that seen in biological temperature-sensing ion channels. As a result, the device could reliably sense temperature changes of less than one degree Celsius.

Decreasing the salinity of the potassium chloride solution improved the performance of the device, in part by further enhancing the channel’s selectivity for potassium ions.

As the researchers increased the intensity of light shining on the material, its temperature rose at the same rate, as did the ion-transporting response. This suggests that along with acting as a temperature sensor the material could also be used to measure light intensity.

The work was a result of collaboration between the groups of KAUST professors Husam Alshareef and Peng Wang. “We envision that the MXene cation channels have promise for many potential applications, including temperature sensing, photodetection or photothermoelectric energy harvesting,” says Alshareef, who co-led the team.

-KAUST Discovery

Wednesday, October 07, 2020

Seismic data yields deeper quake knowledge.

Analysis of abnormally deep earthquakes may lead to improved seismic forecasting.

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Seismic data yields deeper quake knowledge from KAUST Discovery on Vimeo.

By examining data from large earthquakes, KAUST researchers have linked their magnitude, and the extent to which they cause aftershocks, to new depths in the Earth’s crust: these are depths at which it was previously thought earthquakes could not occur.

“This research is critical to understanding how stress builds up in a fold,” says Paul Martin Mai, who led the research. “If we observe an increase in seismogenic (earthquake generating) depth right after a large earthquake in a given fault system, then we know that the next large earthquake in that area may be stronger than we would have thought possible assuming fixed seismogenic depth.”

Most earthquakes occur in the strongest layer of the Earth’s crust, typically between 13 and 18 kilometers deep. Here, huge confining pressure from above acts to increase the brittle strength of rock to maximum effect such that more stress builds up before it fractures. Below this depth, heat from the Earth’s core raises the temperature to degrees at which rock behaves plastically: deforming like a slow-moving liquid, instead of rupturing.

Until the mid-1980s, earthquakes were thought to not occur in this "aseismic" lower zone. Subsequently, however, seismologists began recording aftershocks in this zone, following large earthquakes in the seismogenic zone above. During this transient increase in seismogenic depth, they surmised that rock in the aseismic zone was behaving like the toy Silly Putty, which will flow under normal conditions but ruptures under abnormal stress.

The team’s hypothesis was that transient seismogenic deepening varies with earthquake magnitude. To test it, the researchers took data from 16 earthquake cycles in four fault zones, with each cycle spanning thousands of tremors leading up to and away from the main quake. The zones, in Alaska, Japan, California and Turkey, were chosen for the quality of their data-collecting seismometer networks. In each of the 16 cycles, the main quake was big enough to rupture the Earth’s crust from the surface all the way down to the aseismic zone.

“I had the idea for this paper 10 years ago, but back then there were few data points,” says research scientist Olaf Zielke. “Holding back until rich enough data sets became available has been a waiting game.”

Now, the team has shown the connection between earthquake magnitude and degree of transient seismogenic deepening. Their finding should lead to a better understanding of earthquake physics, as well as improved seismic hazard assessments.

-KAUST Discovery

Tuesday, October 06, 2020

Energy-harvesting plastics pass the acid test

Air-stable coatings can improve the longevity of wearable devices that tap into body heat.

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A polymer previously used to protect solar cells may find new applications in consumer electronics, reveals a KAUST team studying thin films capable of converting thermal energy into electricity.

When two sides of a semiconductor are at different temperatures, electron migration from hot to cool areas can generate a current. This phenomenon, known as the thermoelectric effect, typically requires semiconductors with rigid ceramic structures to maintain the heat difference between the two sides. But the recent discovery that polymers also exhibit thermoelectric behavior has prompted a rethink of how to exploit this method for improved energy harvesting, including incorporation into wearable devices.

Derya Baran and her team at KAUST are helping to engineer self-powered devices using a conducting polymer containing a blend of poly(3,4-ethylenedioxythiophene) and polystyrenesulfonate (PEDOT:PSS) chains. Relatively inexpensive and easy to process for applications, including inkjet printing, PEDOT:PSS is one of the top-performing thermoelectric polymers thanks to its ability to take in efficiency-boosting additives known as dopants.

A polymer-based thin film developed at KAUST can perform thermoelectric power conversions with less chance of premature failure.

Villalva

Diego Rosas-Villalva, a researcher in Baran’s group, explains that thermoelectric PEDOT:PSS thin films are often exposed to dopants in the form of strong acids. This process washes away loose PSS chains to improve polymer crystallinity and leaves behind particles that oxidize PEDOT chains to boost electrical conductivity.

KAUST

“We use nitric acid because it’s one of the best dopants for PEDOT,” says Rosas-Villalva. “However, it evaporates rather easily, and this decreases the performance of the thermoelectric over time.”

After the doping step is completed, the PEDOT:PSS film has to undergo a reverse procedure to neutralize or "dedope" some conductive particles to improve thermoelectric power generation.

Typical dedopants include short hydrocarbons containing positively charged amine groups. The KAUST researchers were studying a polymerized version of these amine chains, known as ethoxylated polyethylenimine, when they noticed a remarkable effect—PEDOT:PSS films dedoped with polyethylenimine retained twice as much thermoelectric power after one week compared with untreated specimens.

The team’s investigations revealed that polyethylenimine was effective at encapsulating PEDOT:PSS films to prevent nitric acid escape. In addition, this coating modified the electronic properties of the thermoelectric polymer to make it easier to harvest energy from sources, including body heat.

“We were not expecting that this polymer would improve the lifetime of the device, especially because it’s such a thin film—less than 5 nanometers,” says Villalva. “It’s been incorporated into other organic electronics before, but barely explored for thermoelectrics.”

In the development of polymer-based thermoelectrics, PEIE is a useful material for enhancing thermoelectric performance and air-stability. — In the development of polymer-based thermoelectrics, PEIE is a useful material for enhancing thermoelectric performance and air-

-KAUST Discovery

Tuesday, September 15, 2020

A star is born.

Unique star-shaped polymers have highly tunable properties that will open up a range of new applications.

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Plastics are ubiquitous in modern life, used in packaging, computers, medical equipment and many other devices. All of these applications require different material properties, which depend on the nature of the polymer molecules within the plastics.

KAUST researchers are at the forefront of efforts to develop unusual star-shaped polymers that could open up fresh opportunities for these materials. “Because the heart of a material’s properties is at the molecular level, this unique structure gives the materials unique properties and, therefore, applications,” says Distinguished KAUST Professor Nikos Hadjichristidis.

Polymers are built from repeating chemical units called monomers. The identity of the monomer influences a material’s physical properties, but so too does the arrangement of the polymer chains and the interactions among them. By changing a polymer’s architecture, researchers can fine tune important characteristics, such as elasticity and density.

In 1992, Hadjichristidis and his Ph.D. student Hermis Iatrou, now at the University of Athens, Greece, created an entirely new polymer architecture with several different types of polymers all meeting at a point1. Hadjichristidis called them miktoarm star polymers (from the Greek word µικτός, meaning "mixed"). Because they combine different polymers, they are highly tunable, and the discovery spawned a research field that has yielded hundreds of papers.

In their latest research, Hadjichristidis and his colleagues developed a better way to incorporate polyethylene (PE) into miktoarm star polymers2. PE-based materials have a wide range of applications thanks to their excellent properties: they are inexpensive, stable to heat, strong and flexible. Consequently, miktoarm polymers that contain PE might offer a way to combine the tunability of star polymers with the versatility of PE.

The method previously used to make PE-based star polymers led to stars having PE arms with very short branches, which made the material less robust. So Hadjichristidis’ team developed an improved approach that combines two different polymerization techniques.

They built the stars around a molecule called 4-(dichloromethylsilyl)-diphenylethylene, which contains chemical groups that act as anchor points for polymer chains. The researchers hooked two polyisoprene (PI) chains onto this foundation and then grew a third arm from a different anchor point. By choosing different monomers, the star’s third arm could either be PI, polystyrene or polybutadiene.

The team are creating various miktoarm star polymers using a boron reagent to bond additional polymer arms together.

BioRender.com.

The researchers then added a boron reagent that bonded to the tip of this third arm. Another reagent inserted repeating monomer units between the boron atom and the star, creating a section of PE. Once each star was released from the boron atom, this perfectly linear PE chain contained no short branches and was capped by a hydroxyl group.

"By comparing three types of PE-based stars, the researchers could study how the different structures affected their physical properties, such as self-assembly and crystallinity," says Konstantinos Ntetsikas, who led the experimental work at KAUST. “The next step is to synthesize more PE-based star polymers with varied compositions and study their self-assembly behavior,” he says.

The researchers plan to incorporate polymers that make the materials more soluble, for example, to compare how the stars behave in solution. The hydroxyl group at the end of the PE arm could also be used to attach more polymer molecules onto the star, producing even more complex architectures with unprecedented properties.

“With the knowledge achieved from this and other studies, we can design and synthesize the polymers to precisely achieve targeted material properties,” says Edwin L. Thomas at Rice University in Houston, Texas, who collaborated with Hadjichristidis’s team on the research. “Our future work will be aimed at finding processing conditions that will enable the PE arms to have much higher crystallinities, even above 90 percent.”

Hadjichristidis and his KAUST colleague Yves Gnanou hope to incorporate biodegradable sections into miktoarm stars that could make them useful in biomedical applications or add fluorinated polymers so that they might be applied in manufacturing electronic devices. “Their unique microstructures will solve problems otherwise impossible with their linear counterparts,” Hadjichristidis says.

The researchers also aim to develop processes that are more amenable to manufacturing miktoarm star polymers. For now, the methods used to build the new stars are very sensitive to air and moisture, so they must be carried out in high-vacuum conditions. “So far, the easy and cost-effective synthesis of well-defined miktoarm stars remains a challenge,” says Hadjichristidis. “These challenges will undoubtedly inspire more research in the future.”

-KAUST Discovery

Monday, September 14, 2020

Tandem devices feel the heat.

Researchers develop a better understanding of how novel solar cells developed in the lab will operate under real conditions.

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Understanding how solar cell operation changes as it moves from the lab into the real world is essential for optimizing their design prior to mass production. KAUST researchers show how perovskite/silicon tandem solar cells function in a sunny and hot environment.

Silicon dominates commercial solar-cell production. It is abundant and efficient as a converter of light to electricity. But recently, perovskites have emerged as a material with potential for lower cost fabrication using solution-based processes. Their properties can be tuned via changes in chemical composition.

The optical and electronic properties of a material are linked to its bandgap: the minimum energy incoming photons require to be absorbed. The bandgap also determines how much current is generated when the photon is absorbed. In a conventional solar cell, the light absorbing material absorbs only certain wavelengths of light, those with energies above the bandgap, leaving part of the Sun’s energy untapped.

To get the benefits of both the industrial maturity of silicon and the versatility of perovskite, scientists have investigated using both materials in a device known as a tandem solar cell. These have a theoretical efficiency limit of 44 percent, which is beyond the 33 percent limit of conventional solar cells.

“One limitation of this tandem configuration is that it was thought that the perovskite bandgap had to be wider than stable material compositions would allow,” says the first author of the study, Erkan Aydin.

KAUST

New solar cells are tested in the laboratory under standard test conditions. But the ambient temperatures in most areas where solar cells are deployed are much higher than the standard 25 degrees Celsius, and can fluctuate dramatically, which affects performance.

Aydin and his colleagues investigated the performance of perovskite/silicon tandem solar cells outdoors in a hot, sunny climate. The KAUST team show that while the silicon bandgap gets smaller as the device gets hotter, the perovskite bandgap gets larger. This shifts the devices away from their ideal operating point and reduces the efficiency of tandem cells optimized at standard test conditions. Encouragingly, this tendency has the effect of lowering the perovskite bandgap, allowing more stable perovskite compositions to be used in tandem solar cells.

“Our research will next focus on pushing the power conversion efficiency of these devices beyond the highest reported single-junction silicon solar cell efficiency of 26.7 percent with improved stability,” says Aydin. “These improvements will bring the perovskite/silicon tandem solar cells one step closer to the market.”

-KAUST Discovery

Thursday, September 10, 2020

Phasing out a microscope's tricks.

Imaging artifacts discovered in high-resolution electron microscopes may impact development of next-generation electronic devices.

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An instrument error can lead to complete misidentification of certain crystals, reports a KAUST study that suggests researchers need to exercise caution when using electron microscopes to probe two-dimensional (2D) semiconductors.

2D transition metal dichalcogenides (TMDs) are being tapped for new electronic devices because they can exist in several crystal phases with properties ranging from semiconducting to metallic. Researchers use multiple tools to unravel the structure-property relationships in different TMD phases, but one of the most critical is the scanning transmission electron microscope. This instrument is capable of both resolving atoms on surfaces and chemically identifying them using variations in image contrast.

Areej Aljarb, a materials scientist working in Vincent Tung’s group at KAUST, was recently characterizing TMDs made from molybdenum disulfide (MoS2) when she spotted something troubling. Although initial spectroscopic analysis showed that she had produced semiconducting 2D films, the transmission electron microscope images indicated that MoS2 had arranged into a metallic crystal phase.

To resolve this difference, the team enlisted the help of Sergei Lopatin, an expert in microscopy. Together, they noticed that the electron beams emanating from their state-of-the-art instruments had unusual intensity patterns when they contacted the TMD surface. Instead of the expected spherical shapes, the beam’s intensity profiles appeared triangular. "This was clear evidence of an image-focusing problem known as astigmatism," notes Lopatin.

The relative position of the sample supported on TEM holder before (top) and after (bottom) rotation (left).The corresponding HR-STEM ADF images before (top) and after (bottom) an in-plane rotation by 60 degrees (right).

KAUST

The lenses used to focus electron microscope beams always contain small imperfections that can blur images, especially at atomic-scale resolutions. The team realized that the observed astigmatic effects might impact the contrast of atoms appearing on the surface. By correlating computer simulations of the MoS2 surface with experimental microscopy, they saw several instances where crystal phases could be misidentified due to sulfur atoms changing appearance —and even disappearing—during imaging.

“Atomic contrast can be a powerful tool to deduce crystal phases, but these artifacts erode the foundations of such predictions,” says Tung. “It raises the possibility that there may have been many images already taken of 2D TMDs adversely affected by astigmatism.”

Experiments on other 2D surfaces, including graphene, confirmed that false phases can be observed in a range of materials. The researchers demonstrated that these effects could be mitigated by employing beams in which the electrons are nearly all energetically equivalent.

“Scanning transmission electron microscopy is invaluable in imaging the crystal structure of 2D materials; however, we need to be cognizant of imaging artifacts because ignoring them may lead to scientifically false claims,” says Aljarb.

-KAUST Discovery

Thursday, September 10, 2020

Next-gen smartphones to keep their cool.

Multilayered carbon material could be the perfect fit for heat management in electronic devices.

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The powerful electronics packed inside the latest smartphones can be a significant challenge to keep cool. KAUST researchers have developed a fast and efficient way to make a carbon material that could be ideally suited to dissipating heat in electronic devices. This versatile material could also have additional uses ranging from gas sensors to solar cells.

Many electronic devices use graphite films to draw away and dissipate the heat generated by their electronic components. Although graphite is a naturally occurring form of carbon, heat management of electronics is a demanding application and usually relies on use of high-quality micrometer-thick manufactured graphite films. “However, the method used to make these graphite films, using polymer as a source material, is complex and very energy intensive,” says G. Deokar, a postdoc in Pedro Costa's lab, who led the work. The films are made in a multistep process that requires temperatures of up to 3200 degrees Celsius and which cannot produce films any thinner than a few micrometers.

Deokar, Costa and their colleagues have developed a quick, energy-efficient way to make graphite sheets that are approximately 100 nanometers thick. The team grew nanometer-thick graphite films (NGF) on nickel foils using a technique called chemical vapor deposition (CVD) in which the nickel catalytically converts hot methane gas into graphite on its surface. “We achieved NGFs with a CVD growth step of just five minutes at a reaction temperature of 900 degrees Celsius,” Deokar says.

The NGFs, which could be grown in sheets of up to 55 square centimeters, grew on both sides of the foil. It could be extracted and transferred to other surfaces without the need of a polymer supporting layer, which is a common requirement when handling single-layer graphene films.

Working with electron microscopy specialist Alessandro Genovese, the team captured cross-sectional transmission electron microscopy (TEM) images of the NGF on nickel. “Observing the interface of the graphite films to the nickel foil was an unprecedented achievement that will shed additional light on the growth mechanisms of these films,” Costa says.

Polymer-free wet chemical transfer process for NGFs grown on Ni foil.

Pita

In terms of thickness, NGF sits between commercially available micrometer-thick graphite films and single-layer graphene. “NGFs complement graphene and industrial graphite sheets, adding to the toolbox of layered carbon films,” Costa says. Due to its flexibility, for example, NGF could lend itself to heat management in flexible phones now starting to appear on the market. “NGF integration would be cheaper and more robust than what could be obtained with a graphene film,” he adds.

However, NGFs could find many applications in addition to heat dissipation. One intriguing feature, highlighted in the TEM images, was that some sections of the NGF were just a few carbon sheets thick. “Remarkably, the presence of the few-layer graphene domains resulted in a reasonable degree of visible light transparency of the overall film,” Deokar says. The team proposed that conducting, semitransparent NGFs could be used as a component of solar cells, or as a sensor material for detecting NO2 gas. “We plan to integrate NGFs in devices where they would act as a multifunctional active material,” Costa says.

-KAUST Discovery

Monday, September 07, 2020

Peel-apart surfaces drive transistors to the ledge.

Surfaces featuring atomic-scale ledges and steps can act as reusable templates for producing nanoelectronic components.

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Semiconductor manufacturers are paying more attention to two-dimensional materials, such as transition metal dichalcogenides (TMDs), following the discovery, at KAUST, of an epitaxial growth process of single-crystal TMDs nanoribbons.

An emerging trend in transistor design involves space-saving architectures that stack components on top of one other. TMDs have potential for these systems because they readily form into thin sheets, known as nanoribbons, which have electrical, optical and magnetic activity. However, typical semiconductor processes, such as photolithography, require complicated procedures to produce TMDs of sufficient quality for device purposes.

In collaboration with researchers in the U.S., Belgium and Taiwan, Vincent Tung and colleagues at KAUST are developing alternative approaches to TMD fabrication using surface templates to direct single-crystal growth.

While analyzing candidates with high-resolution electron microscopy, researcher Areej Aljarb spotted something unusual about a semiconductor named gallium trioxide (Ga2O3). After peeling off layers of the flaky material using sticky tape, she saw arrays of narrow, terrace-like ledges that stepped up or down the entire Ga2O3 surface.

“The steps are very steep and well-exposed,” says Aljarb. “And because the atoms located near the vicinity of these ledges have asymmetric structures, they can drive growth in specific directions.”

When the team exposed Ga2O3 surfaces to a mix of molybdenum and sulfur gas, they observed that TMD nanoribbons crystallized lengthwise along the ledges with structures that were practically defect free. Microscopy experiments and theoretical models revealed that the ledge atoms had unique energetic features that enabled aligned nucleation to form single-crystal nanoribbons. "For decades, scientists have sought to grow 2D single-crystal semiconductors on insulators, and this work demonstrates that controlling the ledges of the substrate is the key," says Tung.

This cross-section view shows the long and monolayer MoS2 nanoribbon on top of the ledge of Ga2O3 substrate.

Intriguingly, the nanoribbons could be pulled off and transferred to other substrates without damaging them. To explore potential applications of the ledge-directed growth technology, the international group joined together to design a transistor capable of incorporating nanoribbons from the Ga2O3 template. Electronic measurements showed the new transistor could operate at high speeds and had amplification factors similar to TMD materials produced through more labor-intensive techniques.

“The nanoribbons grow along the ledges using weak physical interactions to stay in place, meaning that no chemical bonds form between the TMD and the underlying Ga2O3 substrate,” notes Aljarb. “This unique feature enables us to transfer the nanoribbons onto foreign substrates for many applications, ranging from transistors, sensors, artificial muscles and atomically thin photovoltaics.”

-KAUST Discovery

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