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            Abstract The prediction of crystal properties plays a crucial role in materials science and applications. Current methods for predicting crystal properties focus on modeling crystal structures using graph neural networks (GNNs). However, accurately modeling the complex interactions between atoms and molecules within a crystal remains a challenge. Surprisingly, predicting crystal properties from crystal text descriptions is understudied, despite the rich information and expressiveness that text data offer. In this paper, we develop and make public a benchmark dataset (TextEdge) that contains crystal text descriptions with their properties. We then propose LLM-Prop, a method that leverages the general-purpose learning capabilities of large language models (LLMs) to predict properties of crystals from their text descriptions. LLM-Prop outperforms the current state-of-the-art GNN-based methods by approximately 8% on predicting band gap, 3% on classifying whether the band gap is direct or indirect, and 65% on predicting unit cell volume, and yields comparable performance on predicting formation energy per atom, energy per atom, and energy above hull. LLM-Prop also outperforms the fine-tuned MatBERT, a domain-specific pre-trained BERT model, despite having 3 times fewer parameters. We further fine-tune the LLM-Prop model directly on CIF files and condensed structure information generated by Robocrystallographer and found that LLM-Prop fine-tuned on text descriptions provides a better performance on average. Our empirical results highlight the importance of having a natural language input to LLMs to accurately predict crystal properties and the current inability of GNNs to capture information pertaining to space group symmetry and Wyckoff sites for accurate crystal property prediction.more » « less
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            Abstract The sub‐Terahertz and Terahertz bands play a critical role in next‐generation wireless communication and sensing technologies, thanks to the large amount of available bandwidth in this spectral regime. While long‐wavelength (microwave to mm‐Wave) and short‐wavelength (near‐infrared to ultraviolet) devices are well‐established and studied, the sub‐THz to THz regime remains relatively underexplored and underutilized. Traditional approaches used in the aforementioned spectral regions are more difficult to replicate in the THz band, leading to the need for the development of novel devices and structures that can manipulate THz radiation effectively. Herein a novel organic, solid‐state electrochemical device is presented, capable of achieving modulation depths of over 90% from ≈500 nm of a conducting polymer that switches conductivity over a large dynamic range upon application of an electronically controllable external bias. The stability of such devices under long‐term, repeated voltage switching, as well as continuous biasing at a single voltage, is also explored. Switching stabilities and long‐term bias stabilities are achieved over two days for both use cases. Additionally, both depletion mode (always “ON”) and accumulation mode (always “OFF”) operation are demonstrated. These results suggest applications of organic electrochemical THz modulators in large area and flexible implementations.more » « less
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            Abstract Organic small molecules that exhibit second‐scale phosphorescence at room temperature are of interest for potential applications in sensing, anticounterfeiting, and bioimaging. However, such materials systems are uncommon—requiring millisecond to second‐scale triplet lifetimes, efficient intersystem crossing, and slow rates of nonradiative recombination. Here, a simple and scalable approach is demonstrated to activate long‐lived phosphorescence in a wide variety of molecules by suspending them in rigid polymer hosts and annealing them above the polymer's glass transition temperature. This process produces submicron aggregates of the chromophore, which suppresses intramolecular motion that leads to nonradiative recombination and minimizes triplet–triplet annihilation that quenches phosphorescence in larger aggregates. In some cases, evidence of excimer‐mediated intersystem crossing that enhances triplet generation in aggregated chromophores is found. In short, this approach circumvents the current design rules for long‐lived phosphors, which will streamline their discovery and development.more » « less
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            Abstract Neuromorphic photonics has become one of the research forefronts in photonics, with its benefits in low‐latency signal processing and potential in significant energy consumption reduction when compared with digital electronics. With artificial intelligence (AI) computing accelerators in high demand, one of the high‐impact research goals is to build scalable neuromorphic photonic integrated circuits which can accelerate the computing of AI models at high energy efficiency. A complete neuromorphic photonic computing system comprises seven stacks: materials, devices, circuits, microarchitecture, system architecture, algorithms, and applications. Here, we consider microring resonator (MRR)‐based network designs toward building scalable silicon integrated photonic neural networks (PNN), and variations of MRR resonance wavelength from the fabrication process and their impact on PNN scalability. Further, post‐fabrication processing using organic photochromic layers over the silicon platform is shown to be effective for trimming MRR resonance wavelength variation, which can significantly reduce energy consumption from the MRR‐based PNN configuration. Post‐fabrication processing with photochromic materials to compensate for the variation in MRR fabrication will allow a scalable silicon system on a chip without sacrificing today's performance metrics, which will be critical for the commercial viability and volume production of large‐scale silicon photonic circuits.more » « less
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            Abstract While metal‐halide perovskite light‐emitting diodes (PeLEDs) hold the potential for a new generation of display and lighting technology, their slow operation speed and response time limit their application scope. Here, high‐speed PeLEDs driven by nanosecond electrical pulses with a rise time of 1.2 ns are reported with a maximum radiance of approximately 480 kW sr−1 m−2at 8.3 kA cm−2, and an external quantum efficiency (EQE) of 1% at approximately 10 kA cm−2, through improved device configuration designs and material considerations. Enabled by the fast operation of PeLEDs, the temporal response provides access to transient charge carrier dynamics under electrical excitation, revealing several new electroluminescence quenching pathways. Finally, integrated distributed feedback (DFB) gratings are explored, which facilitate more directional light emission with a maximum radiance of approximately 1200 kW sr−1 m−2at 8.5 kA cm−2, a more than two‐fold enhancement to forward radiation output.more » « less
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            Abstract n‐Doping electron‐transport layers (ETLs) increases their conductivity and improves electron injection into organic light‐emitting diodes (OLEDs). Because of the low electron affinity and large bandgaps of ETLs used in green and blue OLEDs, n‐doping has been notoriously more difficult for these materials. In this work, n‐doping of the polymer poly[(9,9‐dioctylfluorene‐2,7‐diyl)‐alt‐(benzo[2,1,3]thiadiazol‐4,7‐diyl)] (F8BT) is demonstrated via solution processing, using the air‐stable n‐dopant (pentamethylcyclopentadienyl)(1,3,5‐trimethylbenzene)ruthenium dimer [RuCp*Mes]2. Undoped and doped F8BT films are characterized using ultraviolet and inverse photoelectron spectroscopy. The ionization energy and electron affinity of the undoped F8BT are found to be 5.8 and 2.8 eV, respectively. Upon doping F8BT with [RuCp*Mes]2, the Fermi level shifts to within 0.25 eV of the F8BT lowest unoccupied molecular orbital, which is indicative of n‐doping. Conductivity measurements reveal a four orders of magnitude increase in the conductivity upon doping and irradiation with ultraviolet light. The [RuCp*Mes]2‐doped F8BT films are incorporated as an ETL into phosphorescent green OLEDs, and the luminance is improved by three orders of magnitude when compared to identical devices with an undoped F8BT ETL.more » « less
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            Abstract Electrically pumped lasing from hybrid organic–inorganic metal‐halide perovskite semiconductors could lead to nonepitaxial diode lasers that are tunable throughout the visible and near‐infrared spectrum; however, a viable laser diode architecture has not been demonstrated to date. Here, an important step toward this goal is achieved by demonstrating two distinct distributed feedback light‐emitting diode architectures that achieve low threshold, optically pumped lasing. Bottom‐ and top‐emitting perovskite light‐emitting diodes are fabricated on glass and Si substrates, respectively, using a polydimethylsiloxane stamp in the latter case to nanoimprint a second‐order distributed feedback grating directly into the methylammonium lead iodide active layer. The devices exhibit room temperature thresholds as low as ≈6 µJ cm−2, a peak external quantum efficiency of ≈0.1%, and a maximum current density of ≈2 A cm−2that is presently limited by degradation associated with excessive leakage current. In this low current regime, electrical injection does not adversely affect the optical pump threshold, leading to a projected threshold current density of ≈2 kA cm−2. Operation at low temperature can significantly decrease this threshold, but must overcome extrinsic carrier freeze‐out in the doped organic transport layers to maintain a reasonable drive voltage.more » « less
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            Abstract A variety of unconventional materials, including biological nanostructures, organic and hybrid semiconductors, as well as monolayer, and other low‐dimensional systems, are actively explored. They are usually incompatible with standard lithographic techniques that use harsh organic solvents and other detrimental processing. Here, a new class of green and gentle lithographic resists, compatible with delicate materials and capable of both top‐down and bottom‐up fabrication routines is developed. To demonstrate the excellence of this approach, devices with sub‐micron features are fabricated on organic semiconductor crystals and individual animal's brain microtubules. Such structures are created for the first time, thanks to the genuinely water‐based lithography, which opens an avenue for the thorough research of unconventional delicate materials at the nanoscale.more » « less
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            Abstract Highly crystalline thin films in organic semiconductors are important for applications in high‐performance organic optoelectronics. Here, the effect of grain boundaries on the Hall effect and charge transport properties of organic transistors based on two exemplary benchmark systems is elucidated: (1) solution‐processed blends of 2,7‐dioctyl[1]benzothieno[3,2‐b][1]benzothiophene (C8‐BTBT) small molecule and indacenodithiophene‐benzothiadiazole (C16IDT‐BT) conjugated polymer, and (2) large‐area vacuum evaporated polycrystalline thin films of rubrene (C42H28). It is discovered that, despite the high field‐effect mobilities of up to 6 cm2V−1s−1and the evidence of a delocalized band‐like charge transport, the Hall effect in polycrystalline organic transistors is systematically and significantly underdeveloped, with the carrier coherence factor α < 1 (i.e., yields an underestimated Hall mobility and an overestimated carrier density). A model based on capacitively charged grain boundaries explaining this unusual behavior is described. This work significantly advances the understanding of magneto‐transport properties of organic semiconductor thin films.more » « less
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