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31 May 03:38

[ASAP] Optically Readable, Physically Unclonable Subwavelength Pixel via Multicolor Quantum Dot Printing for Anticounterfeiting

by Zaiqin Man, Chenyu Dong, Jie Bian, Zhenda Lu, Yan-qing Lu, and Weihua Zhang

TOC Graphic

Nano Letters
DOI: 10.1021/acs.nanolett.4c01463
30 May 07:03

Low‐Symmetry 2D t‐InTe for Polarization‐Sensitive UV‐Vis‐NIR Photodetection

by Nan Zhou, Ziwei Dang, Haoran Li, Zongdong Sun, Shijie Deng, Junhao Li, Xiaobo Li, Xiaoxia Bai, Yong Xie, Liang Li, Tianyou Zhai
Low-Symmetry 2D t-InTe for Polarization-Sensitive UV-Vis-NIR Photodetection

2D t-InTe crystal is developed to realize broadband-response and high-anisotropy polarized photodetection. Originating from its narrow band gap (≈1.28 eV) and low-symmetry crystal structure, 2D t-InTe-based photodetector demonstrates a UV–vis–NIR broadband photoresponse with excellent near-infrared photodetection performance, and strong anisotropic photoresponsivity with an exceptional anisotropy factor of 1.81@808 nm, confirming its promise for high-performance polarized optoelectronics.


Abstract

Polarization-sensitive photodetection grounded on low-symmetry 2D materials has immense potential in improving detection accuracy, realizing intelligent detection, and enabling multidimensional visual perception, which has promising application prospects in bio-identification, optical communications, near-infrared imaging, radar, military, and security. However, the majority of the reported polarized photodetection are limited by UV–vis response range and low anisotropic photoresponsivity factor, limiting the achievement of high-performance anisotropic photodetection. Herein, 2D t-InTe crystal is introduced into anisotropic systems and developed to realize broadband-response and high-anisotropy-ratio polarized photodetection. Stemming from its narrow band gap and intrinsic low-symmetry lattice characteristic, 2D t-InTe-based photodetector exhibits a UV–vis–NIR broadband photoresponse and significant photoresponsivity anisotropy behavior, with an exceptional in-plane anisotropic factor of 1.81@808 nm laser, surpassing the performance of most reported 2D counterparts. This work expounds the anisotropic structure-activity relationship of 2D t-InTe crystal, and identifies 2D t-InTe as a prospective candidate for high-performance polarization-sensitive optoelectronics, laying the foundation for future multifunctional device applications.

30 May 06:54

A vision chip with complementary pathways for open-world sensing

by Zheyu Yang

Nature, Published online: 29 May 2024; doi:10.1038/s41586-024-07358-4

Inspired by the human visual system, a vision chip with primitive-based complementary pathways is developed to overcome the power and bandwidth wall of vision systems, achieving fast, precise, robust and high-dynamic-range sensing efficiently in the open world.
30 May 06:54

Van der Waals polarity-engineered 3D integration of 2D complementary logic

by Yimeng Guo

Nature, Published online: 29 May 2024; doi:10.1038/s41586-024-07438-5

We develop a method for high-density vertical stacking of active-device multi-layers, implementing memory and logic functions, using unique VIP-FETs where a van der Waals intercalation layer modulates the p- or n-type nature of the FETs.
30 May 06:54

Heterogeneous integration of spin–photon interfaces with a CMOS platform

by Linsen Li

Nature, Published online: 29 May 2024; doi:10.1038/s41586-024-07371-7

A modular quantum system-on-chip architecture integrates thousands of individually addressable spin qubits in two-dimensional quantum microchiplet arrays into an integrated circuit designed for cryogenic control, supporting full connectivity for quantum memory arrays across spin–photon channels.
30 May 06:48

Absorption‐Dominant Electromagnetic Interference (EMI) Shielding across Multiple mmWave Bands Using Conductive Patterned Magnetic Composite and Double‐Walled Carbon Nanotube Film

by Byeongjin Park, Sosan Hwang, Horim Lee, Yeonsu Jung, Taehoon Kim, Suk Jin Kwon, Dawoon Jung, Sang‐bok Lee
Absorption-Dominant Electromagnetic Interference (EMI) Shielding across Multiple mmWave Bands Using Conductive Patterned Magnetic Composite and Double-Walled Carbon Nanotube Film

By integrating a magnetic composite layer, a conductive patterned grid, and a double-walled carbon nanotube film, a novel absorption-dominant EMI shielding film achieves exceptional shielding effectiveness while minimizing reflection and maximizing absorption of EMI in multiple frequency bands. The optimized film shows <0.05 dB SER and over 70 dB SET at three different frequencies with 400 µm thickness.


Abstract

The revolution of millimeter-wave (mmWave) technologies is prompting a need for absorption-dominant EMI shielding materials. While conventional shielding materials struggle in the mmWave spectrum due to their reflective nature, this study introduces a novel EMI shielding film with ultralow reflection (<0.05 dB or 1.5%), ultrahigh absorption (>70 dB or 98.5%), and superior shielding (>70 dB or 99.99999%) across triple mmWave frequency bands with a thickness of 400 µm. By integrating a magnetic composite layer (MCL), a conductive patterned grid (CPG), and a double-walled carbon nanotube film (DWCNTF), specific resonant frequencies of electromagnetic waves are transmitted into the film with minimized reflection, and trapped and dissipated between the CPG and the DWCNTF. The design factors for resonant frequencies, such as the CPG geometry and the MCL refractive index, are systematically investigated based on electromagnetic wave propagation theories. This innovative approach presents a promising solution for effective mmWave EMI shielding materials, with implications for mobile communication, radar systems, and wireless gigabit communication.

30 May 06:42

Carbon‐Based Photonic Microlabels Based on Fluorescent Nanographene‐Polystyrene Composites

by M. Reale, E. Marino, E. Maçôas, F. Ciccarello, M. Cannas, C. M. Cruz, A. G. Campaña, A. Sciortino, F. Messina
Carbon-Based Photonic Microlabels Based on Fluorescent Nanographene-Polystyrene Composites

A straightforward and versatile self-assembly procedure is used to obtain nanographene-doped microparticles. Each designed fluorescent microresonator exhibits distinct emission spectra, modulated by sharp optical resonances that act as a unique fingerprint of each specific microparticle, disclosing numerous functional properties applicable across various applicative fields, including sensing, metrology, encoding, and anticounterfeiting.


Abstract

Nanographenes (NGs) are attracting significant interest as atomically-thin carbon-based optical nanomaterials exhibiting a wide range of optical properties that are fine-tuned with ultimate atomic precision though chemical design. However, the use of NGs in photonic applications remains poorly explored. Here a straightforward procedure is demonstrated to load NGs onto the surface of polystyrene microbeads in order to synthesize a functional light emitting microcomposite. The resulting all-carbon-based microbeads behave as optical microresonators displaying narrowband emission lines spread across the whole visible spectrum. The unique fluorescent pattern of individual microbeads enables applications in metrology and information encoding. This is shown, as a proof-of-concept, by absolute diameter and refractive index estimates of individual polystyrene microbeads with nanometric precision, and the design of an unclonable photonic microtag for anti-counterfeiting applications. These results pave the way to a new family of carbon-based microdevices with a wide range of applications in photonics.

30 May 06:42

A Fully Self‐Healing Patch of Integrated Bio‐Signal Monitoring Sensors with Self‐Healing Microporous Foam and Au Nanosheet Electrodes

by Mihyeon Park, Wonseok Yang, Jung Wook Kim, Yeonji Choi, Somin Kim, Yonghui Lee, Dong Sik Kim, Jiyoon Kim, Dong‐Kwon Lim, Jeong Sook Ha
A Fully Self-Healing Patch of Integrated Bio-Signal Monitoring Sensors with Self-Healing Microporous Foam and Au Nanosheet Electrodes

This work demonstrates a fully self-healing sensor patch of integrated bio-signal monitoring sensors fabricated with self-healing microporous sensor foam, Au nanosheet electrodes, and oxime-carbamate bond-based polyurethane film. With this sensor patch, bio-signals of skin temperature, wrist pulse, and electrocardiogram can be simultaneously detected without interference even after self-healing from complete bisection by heating at 65 °C for 6 h.


Abstract

A fully self-healing sensor patch consisting of an in-plane integrated dual-mode sensor and a pressure sensor with a vertically integrated electrocardiogram (ECG) electrode is reported. For a full-device self-healing, interlayer self-bonding by using self-healing oxime-carbamate bond-based polyurethane and room temperature self-healing TUEG3 capped Au nanosheet (T-Au NS) electrodes are devised. Via the use of a self-healing sensor foam prepared by a coating of a self-healing composite of polyurethane and polyaniline onto a microporous graphene foam, a self-healing dual-mode sensor is fabricated to detect the pressure and temperature simultaneously without interference. Furthermore, the interdigitated self-healing electrode of T-Au NS is applied to the pressure sensor to enhance the sensitivity up to 208.62 kPa−1 (<1 kPa), enabling the detection of small pulse signals even after multiple self-healing events. By using the common self-healing T-Au NS electrode vertically integrated onto the sensor patch, ECG signals are also detected. With this sensor patch, skin temperature, wrist pulse, and ECG signals are successfully detected after a simultaneous full-device self-healing from complete bisection. This study demonstrates the facile fabrication of a high-performance, fully self-healing patch of multi-sensors via the deliberate selection of sensor design and the associated functional materials, confirming its high potential applicability to highly durable health monitoring systems.

29 May 09:19

An Ultra‐Conductive and Patternable 40 nm‐Thick Polymer Film for Reliable Emotion Recognition

by Xiaojia Du, Hai Wang, Yunfei Wang, Zhiqiang Cao, Leyi Yang, Xiaohu Shi, Xiaoxu Zhang, Chengzhi He, Xiaodan Gu, Nan Liu
An Ultra-Conductive and Patternable 40 nm-Thick Polymer Film for Reliable Emotion Recognition

An ultrathin (40 nm) polymer film comprising photolithographic poly(3,4-ethylenedioxythiophene):poly(styrene sulfonate) and graphene (PLPG) is developed as a patternable and compliant bioelectrode. Finite element analysis is adopted to optimize electrode structure for better stress dissipation ability. PLPG demonstrates excellent performance in motion artifact-less electrophysiological sensing. Integrating facial electromyogram with machine learning algorithms, a high emotion recognition accuracy is achieved.


Abstract

Understanding psychology is an important task in modern society which helps predict human behavior and provide feedback accordingly. Monitoring of weak psychological and emotional changes requires bioelectronic devices to be stretchable and compliant for unobtrusive and high-fidelity signal acquisition. Thin conductive polymer film is regarded as an ideal interface; however, it is very challenging to simultaneously balance mechanical robustness and opto-electrical property. Here, a 40 nm-thick film based on photolithographic double-network conductive polymer mediated by graphene layer is reported, which concurrently enables stretchability, conductivity, and conformability. Photolithographic polymer and graphene endow the film photopatternability, enhance stress dissipation capability, as well as improve opto-electrical conductivity (4458 S cm−1@>90% transparency) through molecular rearrangement by π–π interaction, electrostatic interaction, and hydrogen bonding. The film is further applied onto corrugated facial skin, the subtle electromyogram is monitored, and machine learning algorithm is performed to understand complex emotions, indicating the outstanding ability for stretchable and compliant bioelectronics.

29 May 03:13

Realization of Fully High‐Spin State and Strong Ferromagnetism in LaCoO3 Monolayer

by Junhua Liu, Liang Si, Qinghua Zhang, Xiao Wang, Jessica Freese, Grant Harris, Mei Wu, Xinxin Zhang, Ting Lin, Ronny Sutarto, Javier Herrero‐Martín, Charles Guillemard, Manuel Valvidares, Lin Li, Xiaofei Gao, Yaoyao Ji, Zhixiong Deng, Yuhao Hong, Long Wei, Yulin Gan, Lingfei Wang, Guanglei Cheng, Peng Gao, Lin Gu, Jiandi Zhang, Zhiwei Hu, Liu Hao Tjeng, Robert J. Green, Kai Chen, Zhaoliang Liao
Realization of Fully High-Spin State and Strong Ferromagnetism in LaCoO3 Monolayer

An electronic transformation in the LaCoO3 monolayer from the conventional mixed high-spin/low-spin state to an unprecedented fully high-spin state is successfully achieved by constructing SrIrO3/LaCoO3 superlattices. This emergent fully high-spin species exhibits strong 2D ferromagnetism with a Curie temperature exceeding 100 K. Additionally, interfacial Ir/Co hybridization drives orbital reconstruction with polarization beyond standard crystal field expectations.


Abstract

Perovskite LaCoO3 is a subject of extensive and ongoing investigation due to the delicate competition between high-spin (HS) and low-spin (LS) states of Co3+. On the other hand, their indistinct free energy boundary poses a significant challenge to annihilate the magnetically/electrically inert LS Co3+ for yielding fully HS state. Here, electronic transformation from the conventional isovalent mixed HS/LS state (La[CoHS3+,CoLS3+]O3${\mathrm{La}}[ {{\mathrm{Co}}_{HS}^{3 + },{\mathrm{Co}}_{LS}^{3 + }} ]{{{\mathrm{O}}}_3}$) into an unprecedented aliovalent fully HS state (La[CoHS3+,CoHS2+]O3${\mathrm{La}}[{\mathrm{Co}}_{HS}^{3 + },{\mathrm{Co}}_{HS}^{2 + }]{{{\mathrm{O}}}_3}$) is demonstrated in monolayer LaCoO3 confined by 5d SrIrO3 slabs via atomically constructing SrIrO3/LaCoO3 superlattices. Excitingly, this emergent fully HS La[CoHS3+,CoHS2+]O3${\mathrm{La}}[ {{\mathrm{Co}}_{HS}^{3 + },{\mathrm{Co}}_{HS}^{2 + }} ]{{{\mathrm{O}}}_3}$ monolayer exhibits not only remarkable 2D ferromagnetism beyond the Mermin–Wagner restriction, but also larger magnetization (≈1.8µB/Co) and higher Curie temperature (above 100 K) than that of conventional La[CoHS3+,CoLS3+]O3${\mathrm{La}}[ {{\mathrm{Co}}_{HS}^{3 + },{\mathrm{Co}}_{LS}^{3 + }} ]{{{\mathrm{O}}}_3}$ thick film and any previously reported oxide-based monolayer ferromagnets. Furthermore, Ir/Co hybridization driven orbital reconstruction with polarization beyond standard crystal field expectations is observed, which is supported by DFT calculations. The findings not only expand the electronic phase domains of LCO into fully HS state, but also provide a fresh platform for investigating the 2D magnetic physics under strongly spin-orbit coupled regime and developing new 2D spintronic devices.

29 May 03:12

2D/0D Heterojunction Interface with Photovoltaic Enhancement and Stabilization for Label‐Free Exosome Biosensor

by Yindian Wang, Suyun Zhong, Jaebeom Lee, Hongxia Chen
2D/0D Heterojunction Interface with Photovoltaic Enhancement and Stabilization for Label-Free Exosome Biosensor

A novel 2D-semiconductor/0D-plasma heterojunction MXene-TA-Au-PEG (MTAP) has been developed as a high-performance and multifunctional photovoltaic interfacial material. MTAP effectively addresses the conventional “three S” requirements for sensors in terms of sensitivity, specificity, and stability by integrating photoelectric enhancement, interfacial antifouling, and oxidative stabilization characteristics. This study offers novel perspectives on interfacial materials aimed at developing improved exosomes biosensor.


Abstract

The selection and design of interface materials as the key to interface engineering is crucial for the excellent performance of optoelectronic devices, enabling multi-functional integration at interfaces. MXene has been extensively employed in optoelectronic devices as an interface material. The primary drawback in interfacial applications, however, is MXene's vulnerability to oxidation in hot, humid environments, which severely reduces photovoltaic performance. Based on hetero-interface engineering, this work offers a novel 2D-semiconductor/0D-plasma heterojunction MXene-TA-Au-PEG (MTAP) as a high-performance and multifunctional photovoltaic interfacial material. MTAP not only effectively protects MXene against stacking and spontaneous oxidation, but also exhibits excellent optoelectronic properties and interfacial antifouling capability. Moreover, MTAP is employed to enhance SPR spectroscopy, allowing for the direct, real-time detection of tumor cell exosomes with LODs as low as 0.28 particles mL−1. MTAP effectively addresses the conventional “three S” requirements for sensors in terms of sensitivity, specificity, and stability by integrating photoelectric enhancement, interfacial antifouling, and oxidative stabilization characteristics. Finally, the results of serum sample analysis showed the sensor has some potential application value in clinical diagnosis. This study offers novel perspectives on the fabrication of 2D/0D heterojunctions using semiconductor and plasma materials, with the aim of developing improved sensing chips.

29 May 03:12

Enhancing Single‐Layer WSe2 Light Emission in Perylene‐Doped Polymer Films through Efficient Energy Transfer

by Marcos Gadea, Aswin Asaithambi, Raúl Bernabeu‐Cabañero, Alex Farrando‐Pérez, Maria Ramos, Juan C. Sancho‐García, Ilka Kriegel, María A. Díaz‐García, M. Reyes Calvo
Enhancing Single-Layer WSe2 Light Emission in Perylene-Doped Polymer Films through Efficient Energy Transfer

The photoluminescence of single-layer WSe2 experiences over a tenfold enhancement when embedded into a perylene-doped plastic film, facilitated by energy transfer from the dye molecules to the 2D material. The optimization of the photoluminescence of 2D materials within plastic films is a crucial step toward their seamless integration into flexible optoelectronic devices.


Abstract

The optical and mechanical properties of 2D semiconductors make them excellent candidates for the active components of plastic optoelectronic devices. Here, the integration of single-layer WSe2 (1L-WSe2) into a polystyrene (PS) film containing dispersed perylene orange (PDI-O) molecules is investigated. The findings reveal a notable enhancement in the light emission of 1L-WSe2, which occurs exclusively upon PDI-O excitation and scales with the concentration of molecules in the PS film. Moreover, the increase in 1L-WSe2 photoluminescence coincides with a quenching of the PDI-O light emission intensity and a decrease in its lifetime. These results point to efficient long-range interactions, such as Förster energy transfer, between PDI-O (acting as the donor) and 1L-WSe2 (acting as the acceptor), as the mechanism responsible for the enhanced light emission in the latter. These findings are of great interest for the development of flexible optoelectronic devices integrating active 2D materials; the polymeric matrix plays a dual role, serving as both physical support and host for organic dopants that can optimize the light emission properties of the active 2D material.

29 May 03:06

Citric Acid: A Nexus Between Cellular Mechanisms and Biomaterial Innovations

by Hui Xu, Su Yan, Ethan Gerhard, Denghui Xie, Xiaodong Liu, Bing Zhang, Dongquan Shi, Guillermo A. Ameer, Jian Yang
Citric Acid: A Nexus Between Cellular Mechanisms and Biomaterial Innovations

Citrate-based biodegradable polymers represent a distinctive biomaterial platform with tremendous potential for diverse medical applications. With their versatile chemistry, these polymers exhibit a broad range of material and bioactive properties and regulate cell metabolism and stem cell differentiation. This review presents a forward-thinking discussion on the role of citrate in tissue regeneration and the development of functional citrate-based metabotissugenic biomaterials.


Abstract

Citrate-based biodegradable polymers have emerged as a distinctive biomaterial platform with tremendous potential for diverse medical applications. By harnessing their versatile chemistry, these polymers exhibit a wide range of material and bioactive properties, enabling them to regulate cell metabolism and stem cell differentiation through energy metabolism, metabonegenesis, angiogenesis, and immunomodulation. Moreover, the recent US Food and Drug Administration (FDA) clearance of the biodegradable poly(octamethylene citrate) (POC)/hydroxyapatite-based orthopedic fixation devices represents a translational research milestone for biomaterial science. POC joins a short list of biodegradable synthetic polymers that have ever been authorized by the FDA for use in humans. The clinical success of POC has sparked enthusiasm and accelerated the development of next-generation citrate-based biomaterials. This review presents a comprehensive, forward-thinking discussion on the pivotal role of citrate chemistry and metabolism in various tissue regeneration and on the development of functional citrate-based metabotissugenic biomaterials for regenerative engineering applications.

28 May 02:52

Noninvasive imaging-guided ultrasonic neurostimulation with arbitrary 2D patterns and its application for high-quality vision restoration

by Gengxi Lu

Nature Communications, Published online: 27 May 2024; doi:10.1038/s41467-024-48683-6

Researchers have developed a noninvasive retina prosthesis based on ultrasound for treating blindness. This device uses ultrasound waves to stimulate the retina, creating artificial vision confirmed through behavior tests, offering a safer alternative to invasive treatments.
28 May 02:31

Emergence of bidirectional cell laning from collective contact guidance

by Mathilde Lacroix

Nature Physics, Published online: 27 May 2024; doi:10.1038/s41567-024-02510-3

Supracellular cues play a key role in directing collective cell migration in processes such as wound healing and cancer invasion. New findings emphasize the importance of all length scales of the microenvironment in shaping cell migration patterns.
28 May 02:22

Treefrog‐Inspired Flexible Electrode with High Permeability, Stable Adhesion, and Robust Durability

by Tianxiang Lan, Hongmiao Tian, Xiaoliang Chen, Xiangming Li, Chunhui Wang, Duorui Wang, Sheng Li, Gangqiang Liu, Xinkai Zhu, Jinyou Shao
Treefrog-Inspired Flexible Electrode with High Permeability, Stable Adhesion, and Robust Durability

The challenges of instable adhesion, low impedance, and robust durability that hinder the long-term application of in vitro bioelectrodes. Inspired by treefrog web and bird's beak, through the optimization design, a web-like electrode, which can solve these complex integrated challenges, is proposed. Proposed electrode has the most balanced mechanical, electrical, and electrode properties of typical electrodes reported in recent years.


Abstract

Long-term continuous monitoring (LTCM) of physiological electrical signals is an effective means for detecting several cardiovascular diseases. However, the integrated challenges of stable adhesion, low impedance, and robust durability under different skin conditions significantly hinder the application of flexible electrodes in LTCM. This paper proposes a structured electrode inspired by the treefrog web, comprising dispersed pillars at the bottom and asymmetric cone holes at the top. Attachment structures with a dispersed pillar improve the contact stability (adhesion increases 2.79/13.16 times in dry/wet conditions compared to an electrode without structure). Improved permeable duct structure provides high permeability (12 times compared to cotton). Due to high adhesion and permeability, the electrode's durability is 40 times larger than commercial Ag/AgCl electrodes. The treefrog web-like electrode has great advantages in permeability, adhesion, and durability, resulting in prospects for application in physiological electrical signal detection and a new design idea for LTCM wearable dry electrodes.

27 May 09:06

[ASAP] 2D Materials Kill Bacteria from Within

by Delong Hou, Shuai Zhou, Xueling Tan, Dongzhi Yuan, Jun Yan, Qi Zeng, and Yi Chen

TOC Graphic

Nano Letters
DOI: 10.1021/acs.nanolett.4c00803
27 May 04:38

[ASAP] Anomalous Correlation between Thermal Conductivity and Elastic Modulus in Two-Dimensional Hybrid Metal Halide Perovskites

by Ankit Negi, Liang Yan, Cong Yang, Yeonju Yu, Doyun Kim, Subhrangsu Mukherjee, Andrew H. Comstock, Saqlain Raza, Ziqi Wang, Dali Sun, Harald Ade, Qing Tu, Wei You, and Jun Liu

TOC Graphic

ACS Nano
DOI: 10.1021/acsnano.3c12172
27 May 04:36

Correlating Young's Modulus with High Thermal Conductivity in Organic Conjugated Small Molecules

by Jianhui Zeng, Ting Liang, Jingjing Zhang, Daoqing Liu, Shiang Li, Xinhui Lu, Meng Han, Yimin Yao, Jian‐Bin Xu, Rong Sun, Liejun Li
Correlating Young's Modulus with High Thermal Conductivity in Organic Conjugated Small Molecules

Leveraging the inherent rigidity of molecular structural units and robust intermolecular π–π stacking interactions, PTCDI-C8 molecules demonstrate a vertically aligned orientation on substrates, yielding an elevated thermal conductivity of 3.1 ± 0.1 W m−1 K−1. Through a combination of TDTR, nanoindentation, and molecular dynamics simulations, it is ascertained that the significant Young's modulus of PTCDI-C8 is the primary contributor to its high thermal conductivity.


Abstract

Attaining elevated thermal conductivity in organic materials stands as a coveted objective, particularly within electronic packaging, thermal interface materials, and organic matrix heat exchangers. These applications have reignited interest in researching thermally conductive organic materials. The understanding of thermal transport mechanisms in these organic materials is currently constrained. This study concentrates on N, N'-dioctyl-3,4,9,10-perylenedicarboximide (PTCDI-C8), an organic conjugated crystal. A correlation between elevated thermal conductivity and augmented Young's modulus is substantiated through meticulous experimentation. Achievement via employing the physical vapor transport method, capitalizing on the robust C═C covalent linkages running through the organic matrix chain, bolstered by π–π stacking and noncovalent affiliations that intertwine the chains. The coexistence of these dynamic interactions, alongside the perpendicular alignment of PTCDI-C8 molecules, is confirmed through structural analysis. PTCDI-C8 thin film exhibits an out-of-plane thermal conductivity of 3.1 ± 0.1 W m−1 K−1, as determined by time-domain thermoreflectance. This outpaces conventional organic materials by an order of magnitude. Nanoindentation tests and molecular dynamics simulations elucidate how molecular orientation and intermolecular forces within PTCDI-C8 molecules drive the film's high Young's modulus, contributing to its elevated thermal conductivity. This study's progress offers theoretical guidance for designing high thermal conductivity organic materials, expanding their applications and performance potential.

27 May 04:36

Structural Heredity in Catalysis: CO2 Self‐Selective CeO2 Nanocrystals for Efficient Photothermal CO2 Hydrogenation to Methane

by Kai Zhang, Cuiping Xu, Xingjian Zhang, Zhiyi Huang, Qixiang Pian, Kunhong Che, Xiaokun Cui, Yueru Hu, Yimin Xuan
Structural Heredity in Catalysis: CO2 Self-Selective CeO2 Nanocrystals for Efficient Photothermal CO2 Hydrogenation to Methane

A CO2 self-selective hydrothermal growth strategy is designed for the synthesis of CeO2 octahedral nanocrystals that participate in strong interactions with CO2 molecules which persists during successive high-temperature treatments required for Ni deposition. Such an excellent structural heredity leads to an outstanding photothermal CO2 methanation performance. This strategy represents a new pathway for developing effective catalysts for targeted chemical reactions.


Abstract

The chemical inertness of CO2 molecules makes their adsorption and activation on a catalyst surface one of the key challenges in recycling CO2 into chemical fuels. However, the traditional template synthesis and chemical modification strategies used to tackle this problem face severe structural collapse and modifier deactivation issues during the often-needed post-processing procedure. Herein, a CO2 self-selective hydrothermal growth strategy is proposed for the synthesis of CeO2 octahedral nanocrystals that participate in strong physicochemical interactions with CO2 molecules. The intense affinity for CO2 molecules persists during successive high-temperature treatments required for Ni deposition. This demonstrates the excellent structural heredity of the CO2 self-selective CeO2 nanocrystals, which leads to an outstanding photothermal CH4 productivity exceeding 9 mmol h-1 mcat -2 and an impressive selectivity of >99%. The excellent performance is correlated with the abundant oxygen vacancies and hydroxyl species on the CeO2 surface, which create many frustrated Lewis-pair active sites, and the strong interaction between Ni and CeO2 that promotes the dissociation of H2 molecules and the spillover of H atoms, thereby greatly benefitting the photothermal CO2 methanation reaction. This self-selective hydrothermal growth strategy represents a new pathway for the development of effective catalysts for targeted chemical reactions.

27 May 04:34

Mesoscopic Stacking Reconfigurations in Stacked van der Waals Film

by Yoon Seong Heo, Tae Wan Kim, Wooseok Lee, Jungseok Choi, Soyeon Park, Dong‐Il Yeom, Jae‐Ung Lee
Mesoscopic Stacking Reconfigurations in Stacked van der Waals Film

Mesoscopic-scale stacking reconfigurations and their correlations with mechanical distortions are investigated when van der Waals films are stacked. The origins of deformations are revealed from either the transfer process or the extended impact of atomic reconstructions.


Abstract

Mesoscopic-scale stacking reconfigurations are investigated when van der Waals (vdW) films are stacked. A method to visualize complicated stacking structures and mechanical distortions simultaneously in stacked atom-thick films using Raman spectroscopy is developed. In the rigid limit, it is found that the distortions originate from the transfer process, which can be understood through thin film mechanics with a large elastic property mismatch. In contrast, with atomic corrugations, the in-plane strain fields are more closely correlated with the stacking configuration, highlighting the impact of atomic reconstructions on the mesoscopic scale. It is discovered that the grain boundaries do not have a significant effect while the cracks are causing inhomogeneous strain in stacked polycrystalline films. This result contributes to understanding the local variation of emerging properties from moiré structures and advancing the reliability of stacked vdW material fabrication.

27 May 04:34

Miracle in “White”:Hexagonal Boron Nitride

by Jiaqi Wang, Tongzhou Xu, Weipeng Wang, Zhengjun Zhang
Miracle in “White”:Hexagonal Boron Nitride

The concepts of ″Yin″ and ″Yang″ symbolizes the interplay of opposites such as heaven and earth. By employing the metaphor of ″yin″ and ″yang,″ parallels are drawn to the seemingly contradictory properties observed in hexagonal-boron nitride, where these paired properties are perceived as inherently opposite to each other. The understanding and manipulation of these contradictions would lead to a unity of opposites, which will find applications in unique circumstances.


Abstract

The exploration of 2D materials has captured significant attention due to their unique performances, notably focusing on graphene and hexagonal boron nitride (h-BN). Characterized by closely resembling atomic structures arranged in a honeycomb lattice, both graphene and h-BN share comparable traits, including exceptional thermal conductivity, impressive carrier mobility, and robust pi–pi interactions with organic molecules. Notably, h-BN has been extensively examined for its exceptional electrical insulating properties, inert passivation capabilities, and provision of an ideal ultraflat surface devoid of dangling bonds. These distinct attributes, contrasting with those of h-BN, such as its conductive versus insulating behavior, active versus inert nature, and absence of dangling surface bonds versus absorbent tendencies, render it a compelling material with broad application potential. Moreover, the unity of such contradictions endows h-BN with intriguing possibilities for unique applications in specific contexts. This review aims to underscore these key attributes and elucidate the intriguing contradictions inherent in current investigations of h-BN, fostering significant insights into the understanding of material properties.

27 May 04:34

Synthesis of 2D Gallium Sulfide with Ultraviolet Emission by MOCVD

by Oliver Maßmeyer, Robin Günkel, Johannes Glowatzki, Philip Klement, Badrosadat Ojaghi Dogahe, Stefan Renato Kachel, Felix Gruber, Marius Müller, Melanie Fey, Jörg Schörmann, Jürgen Belz, Andreas Beyer, J. Michael Gottfried, Sangam Chatterjee, Kerstin Volz
Synthesis of 2D Gallium Sulfide with Ultraviolet Emission by MOCVD

Two-dimensional gallium sulfide (2D GaS) emitting in the ultraviolet to visible spectral range is synthesized via metal–organic chemical vapor deposition. Pulsed deposition of industry-standard precursors promotes 2D growth. The interface chemistry with the growth of a Ga adlayer as well as strain relation upon the growth of thicker layers resulting in an epitaxial relationship is revealed. Thickness control is enabled by tuning the number of GaS pulses.


Abstract

Two-dimensional (2D) materials exhibit the potential to transform semiconductor technology. Their rich compositional and stacking varieties allow tailoring materials’ properties toward device applications. Monolayer to multilayer gallium sulfide (GaS) with its ultraviolet band gap, which can be tuned by varying the layer number, holds promise for solar-blind photodiodes and light-emitting diodes as applications. However, achieving commercial viability requires wafer-scale integration, contrasting with established, limited methods such as mechanical exfoliation. Here the one-step synthesis of 2D GaS is introduced via metal–organic chemical vapor deposition on sapphire substrates. The pulsed-mode deposition of industry-standard precursors promotes 2D growth by inhibiting the vapor phase and on-surface pre-reactions. The interface chemistry with the growth of a Ga adlayer that results in an epitaxial relationship is revealed. Probing structure and composition validate thin-film quality and 2D nature with the possibility to control the thickness by the number of GaS pulses. The results highlight the adaptability of established growth facilities for producing atomically thin to multilayered 2D semiconductor materials, paving the way for practical applications.

27 May 04:29

Interfaces Between Nanoparticle and Biomacromolecular Network: Dynamic Behaviors, Confinement and Entropy

by Xuanyu Zhang, Xiaobin Dai, Haixiao Wan, Zheng Jiao, Wenlong Chen, Wenjie Wei, Jiaqi Li, Kai Liu, Zhenzhong Yang, Li‐Tang Yan
Interfaces Between Nanoparticle and Biomacromolecular Network: Dynamic Behaviors, Confinement and Entropy

Biomacromolecular networks serve as the structural basis of diverse biological systems. This review seeks to present the state-of-art progress and perspective of the dynamic behaviors, confinement and entropy at the interfaces between nanoparticle and biomacromolecular network.


Abstract

Biomacromolecular networks, crucial components of biological systems, are of great importance in biological and nanomedical science, in which the interfaces between nanoparticle and macromolecular networks are intriguing and drawing great attention. Herein, this review seeks to present the state-of-art progress and perspective of the dynamic behaviors, confinement and entropy at the nanoparticle-biomacromolecular network interfaces. The basic biomacromolecular networks in living systems, recent research on networks with dynamic bonds and various diffusion behaviors of nanoparticles within biomacromolecular networks are summarized. In particular, entropic effects in the confined environments of biological networks are discussed, along with how they impact the mechanical properties and dynamical behaviors. The interesting research and findings included in this review might offer the scientific community a better understanding of how this field has developed thus far, and are anticipated to trigger more systematic and fundamental research to elucidate the underlying physics and broaden the potential applications of macromolecular networks, biological and artificial.

27 May 04:27

Artificial Spores as Multi‐Functional Biocatalysts to Perform Biosynthetic Cascades

by Maialen Iturralde, Magdalena Ripoll, Desiré di Silvio, Marta Gallego, Daniel A. Grajales‐Hernández, Xabier López, Lorena Betancor, Fernando López‐Gallego
Artificial Spores as Multi-Functional Biocatalysts to Perform Biosynthetic Cascades

Artificial sportes formed by gall ink coatings overexpress intracecullar oxidoreductases and display transaminases for cooperative biocatalysis, enabling the biotransformation of polyols into aminoalcohols.


Abstract

Cells exhibit diverse structural formations such as biofilms and spores, enabling them to acquire novel functionalities. Many of these structures display biomacromolecules, including enzymes, tethered to cell walls to support various extracellular processes. Alternatively, encapsulating single cells with polymer coatings offers a strategy that circumvents the need for genetic engineering while imparting artificial functionalities to cells. Here, a universal method is presented for encapsulating single gram-negative microbes with polymeric coatings based on the ancestral gall ink formed by tannic acid-iron complexes. As a result, synthetic spores are achieved that selectively bind His-tagged enzymes through the formation of unprecedented galloyl/imidazole-Fe2+ complexes via ligand substitution demonstrated by density functional theory. These synthetic spores with a thickness of 41.5 ± 4.2 nm and a stiffness of 6.0 ± 3.5 GPa serve as biocatalytic materials for the one-pot oxidative amination of diols into amino alcohols, facilitated by the cooperative catalysis between intracellular endogenous or recombinant oxidoreductases, and an extracellular transaminase from Pseudomonas fluorescens displayed at the spore surface. These spores maintain their performance in three consecutive batch cycles. Integrating isolated enzymes onto the surface of engineered microbes coated with polymers offers novel opportunities for synthetic biology, advancing the efficiency of biosynthetic cascades in solid-state environments.

27 May 04:24

TiO2 Nano‐Biopatterning Reveals Optimal Ligand Presentation for Cell–Matrix Adhesion Formation (Adv. Mater. 21/2024)

by Kashish Jain, Ashish Pandey, Hao Wang, Taerin Chung, Arash Nemati, Pakorn Kanchanawong, Michael P. Sheetz, Haogang Cai, Rishita Changede
TiO2 Nano-Biopatterning Reveals Optimal Ligand Presentation for Cell–Matrix Adhesion Formation (Adv. Mater. 21/2024)

Nano-Biopatterning

In article number 2309284 by Haogang Cai, Rishita Changede, and co-workers, a dielectric nano-biopatterning technology is developed, enabling super-resolution fluorescence microscopy that is challenging for conventional plasmonic nanopatterns with quenching effects. Through both simulations and experiments, nanopattern interactions with adjacent fluorescence and surrounding lipid membranes are studied. This technology will facilitate precise quantitative cell biology studies to investigate molecular-scale signaling events in response to receptor clustering and their nanoscale organization. Image credit: Nanzhong Deng, New York University.


27 May 04:22

Anisotropic 2D van der Waals Magnets Hosting 1D Spin Chains

by Eugene Park, John P. Philbin, Hang Ch, Joshua J. Sanchez, Connor Occhialini, Georgios Varnavides, Jonathan B. Curtis, Zhigang Song, Julian Klein, Joachim D. Thomsen, Myung‐Geun Han, Alexandre C. Foucher, Kseniia Mosina, Deepika Kumawat, N. Gonzalez‐Yepez, Yimei Zhu, Zdenek Sofer, Riccardo Comin, Jagadeesh S. Moodera, Prineha Narang, Frances M. Ross
Anisotropic 2D van der Waals Magnets Hosting 1D Spin Chains

Magnetic chains of atoms (“1D magnets”) have intriguing properties that illuminate fundamental principles in many-body physics while also promising applications in magnonics and spintronics. This article describes AgCrP2S6 and its family, layered crystals that host magnetic chains, focusing on their highly anisotropic properties and the additional degrees of freedom that can arise from patterning or stacking to engineer the structure.


Abstract

The exploration of 1D magnetism, frequently portrayed as spin chains, constitutes an actively pursued research field that illuminates fundamental principles in many-body problems and applications in magnonics and spintronics. The inherent reduction in dimensionality often leads to robust spin fluctuations, impacting magnetic ordering and resulting in novel magnetic phenomena. Here, structural, magnetic, and optical properties of highly anisotropic 2D van der Waals antiferromagnets that uniquely host spin chains are explored. First-principle calculations reveal that the weakest interaction is interchain, leading to essentially 1D magnetic behavior in each layer. With the additional degree of freedom arising from its anisotropic structure, the structure is engineered by alloying, varying the 1D spin chain lengths using electron beam irradiation, or twisting for localized patterning, and spin textures are calculated, predicting robust stability of the antiferromagnetic ordering. Comparing with other spin chain magnets, these materials are anticipated to bring fresh perspectives on harvesting low-dimensional magnetism.

27 May 04:22

In Silico Chemical Experiments in the Age of AI: From Quantum Chemistry to Machine Learning and Back

by Abdulrahman Aldossary, Jorge Arturo Campos‐Gonzalez‐Angulo, Sergio Pablo‐García, Shi Xuan Leong, Ella Miray Rajaonson, Luca Thiede, Gary Tom, Andrew Wang, Davide Avagliano, Alán Aspuru‐Guzik
In Silico Chemical Experiments in the Age of AI: From Quantum Chemistry to Machine Learning and Back

This review examines the use of artificial intelligence (AI) and machine learning (ML) applications for computational chemistry, categorized by the degree of physical information deployed. It discusses the advantages, limitations, and future prospects for each model category toward the ultimate goal of defining the optimal architecture for AI to predict accurate, transferable, and reproducible solutions of the Schrödinger equations.


Abstract

Computational chemistry is an indispensable tool for understanding molecules and predicting chemical properties. However, traditional computational methods face significant challenges due to the difficulty of solving the Schrödinger equations and the increasing computational cost with the size of the molecular system. In response, there has been a surge of interest in leveraging artificial intelligence (AI) and machine learning (ML) techniques to in silico experiments. Integrating AI and ML into computational chemistry increases the scalability and speed of the exploration of chemical space. However, challenges remain, particularly regarding the reproducibility and transferability of ML models. This review highlights the evolution of ML in learning from, complementing, or replacing traditional computational chemistry for energy and property predictions. Starting from models trained entirely on numerical data, a journey set forth toward the ideal model incorporating or learning the physical laws of quantum mechanics. This paper also reviews existing computational methods and ML models and their intertwining, outlines a roadmap for future research, and identifies areas for improvement and innovation. Ultimately, the goal is to develop AI architectures capable of predicting accurate and transferable solutions to the Schrödinger equation, thereby revolutionizing in silico experiments within chemistry and materials science.

24 May 06:39

Single-cell multi-cohort dissection of the schizophrenia transcriptome | Science

The complexity and heterogeneity of schizophrenia have hindered mechanistic elucidation and the development of more effective therapies. Here, we performed single-cell dissection of schizophrenia-associated transcriptomic changes in the human prefrontal ...
24 May 06:39

A data-driven single-cell and spatial transcriptomic map of the human prefrontal cortex | Science

The molecular organization of the human neocortex historically has been studied in the context of its histological layers. However, emerging spatial transcriptomic technologies have enabled unbiased identification of transcriptionally defined spatial ...