{"title":"Ultrasensitive Photonic Synapse with Broadband Response Based on the PdSe2 QDs/GeSe Thin Film.","authors":"Chen Li,Jian Sun,Qi Zhang,Kesheng Cao,Yuchen Liu,Zhixing Gan,Yunsong Di,Xiao-Yang Zhang,Tong Zhang","doi":"10.1021/acs.jpclett.5c02552","DOIUrl":"https://doi.org/10.1021/acs.jpclett.5c02552","url":null,"abstract":"Photonic synapses that integrate optical sensing with synaptic functionalities are becoming increasingly important in the advancement of neuromorphic computing systems. However, achieving broad-band sensing and preprocessing capabilities under weak light illumination remains a significant challenge. Herein, we report a photonic synapse based on the PdSe2 QDs/GeSe thin film which leverages the high photosensitivity and favorable band alignment of the PdSe2 QDs/GeSe heterojunction to emulate essential synaptic functionalities. It also exhibits a broadband photoresponse ranging from ultraviolet (UV, 365 nm) to near-infrared (NIR, 850 nm) and maintains performance under an ultraweak light detection threshold down to 0.15 μW cm-2. Furthermore, its potential applications for optical information processing and facial recognition are demonstrated. This work provides a promising strategy for developing multifunctional photonic synapses based on the PdSe2 QDs/GeSe thin film.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"94 1","pages":"10542-10550"},"PeriodicalIF":6.475,"publicationDate":"2025-10-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145209206","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Muhammed Shabeeb,Satish Bhusan Panda,Bhavika Kalal,Simran Baweja,Kusum Kumari,Saurabh Kumar Singh,Surajit Maity
{"title":"Noncovalent C···N Interaction to Capture CO2 on a Neutral Aromatic Molecule in the Gas Phase: Experimental Determination of the UV-Induced Adsorption Energy.","authors":"Muhammed Shabeeb,Satish Bhusan Panda,Bhavika Kalal,Simran Baweja,Kusum Kumari,Saurabh Kumar Singh,Surajit Maity","doi":"10.1021/acs.jpclett.5c01965","DOIUrl":"https://doi.org/10.1021/acs.jpclett.5c01965","url":null,"abstract":"This work describes a novel experimental method to determine the adsorption energy of a molecular complex in the ground and excited states. An increased CO2 capture efficiency was obtained upon electronic excitation of nitrogen-containing heterocycles, due to the formation of strong C···N noncovalent interaction. We performed a combined experimental and computational investigations, to understand the noncovalent interaction between carbon dioxide (CO2) and 2-(2'-pyridyl)benzimidazole (PBI) in the gas phase. Using R2PI, UV-UV hole burning, and IDIR spectroscopic technique, we characterized the PBI-CO2 complex. The S0 → S1 origin band of the PBI-CO2 complex was red-shifted by 329 cm-1 relative to that of the PBI monomer, indicating that the PBI-CO2 complex become more stable upon UV absorption. Therefore, the adsorption energy of CO2 on PBI increased by nearly 30% upon electronic excitation due to the higher stability of the complex in the excited state, which was bound to the adsorbent mainly via the C···N interaction.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"27 1","pages":"10551-10557"},"PeriodicalIF":6.475,"publicationDate":"2025-10-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145209039","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Tiantian Wu,Ruimin Qin,Mei Xiang,Jianrui Zhang,Yaqiong Su
{"title":"DFT Insights into High-Temperature H2 Production at Dual-Atom Active Sites on CeO2.","authors":"Tiantian Wu,Ruimin Qin,Mei Xiang,Jianrui Zhang,Yaqiong Su","doi":"10.1021/acs.jpclett.5c02549","DOIUrl":"https://doi.org/10.1021/acs.jpclett.5c02549","url":null,"abstract":"CeO2-based catalysts have attracted considerable interest in producing H2 via high-temperature water-splitting reactions, where hydroxyl decomposition into H2 was reported as the reaction limiting step. By conducting density-functional theory calculations, it was found that direct H2 production on CeO2 via hydroxyl decomposition needs to overcome a ∼ 3.0 eV barrier, which competes heavily with an additional water adsorption and dissociation into more hydroxyls. Inducing dual-atom sites in CeO2 by substituting one Ce with two Pd (Ni or Rh) can effectively reduce the reaction barrier to 1.5-2.0 eV at high hydrogen coverage and therefore improve the turnover frequency of producing H2 by 10-12 orders of magnitude compared to CeO2. The decreased activation energy barrier for H2 generation over dual-atom sites is linearly correlated with the hydrogen adsorption energy. This work provides atomic-level understanding on rational design of dual-atom sites in metal oxide-based catalysts.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"44 1","pages":"10521-10527"},"PeriodicalIF":6.475,"publicationDate":"2025-10-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145209234","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Yating Su,Li Zhen,Rumei Song,Dan Wu,Shifeng Zhao,Yulong Bai
{"title":"Self-Powered Bi6Ti3Fe2O18@CuO Core-Shell Ferroelectric Photodetectors Realizing Encryption Communication.","authors":"Yating Su,Li Zhen,Rumei Song,Dan Wu,Shifeng Zhao,Yulong Bai","doi":"10.1021/acs.jpclett.5c02432","DOIUrl":"https://doi.org/10.1021/acs.jpclett.5c02432","url":null,"abstract":"Optoelectronic logics are promising units of data encryption, which struggle with complex manufacture, owing to their fixed photodetection mode. Core-shell heterostructure Bi6Ti3Fe2O18@CuO ferroelectric photodetectors were fabricated by a one-pot method, which hosted UV detection and encrypted optical communication. The CuO quantum dot assembled homotypic transport shell was adopted in photodetectors, and the core-shell interfacial heterojunction as well as the ferroelectric core drove photocarrier separation. The Bi6Ti3Fe2O18@CuO (4 mg/mL) photodetectors show a self-powered performance of R ∼ 0.85 A/W, D* ∼ 4.9 × 1012 Jones, and EQE ∼ 25.3%, which provide a simple strategy for encrypted communication. The dual-band (388 and 420 nm) photocurrent as a type of weight-factor, encrypted optical communication is realized based on \"AND\" optoelectronic logical operation, where the Chinese characters and capital letters \"IMU\" are showcased.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"98 1","pages":"10506-10513"},"PeriodicalIF":6.475,"publicationDate":"2025-10-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145209244","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"The Stability Challenges in Developing QLED Based Display Technology","authors":"Menglin Li, , , Hui Bao, , , Peili Gao, , , Wenlin Liang, , , Xiongfeng Lin, , , Longjia Wu, , , Yiran Yan, , , Shuangpeng Wang, , and , Haizheng Zhong*, ","doi":"10.1021/acs.jpclett.5c02156","DOIUrl":"https://doi.org/10.1021/acs.jpclett.5c02156","url":null,"abstract":"<p >Quantum-dot light-emitting diodes (QLEDs) have emerged as an attractive display technology due to their high brightness, wide color gamut, and ultrahigh resolution. As they transition from prototype devices to commercial display products, the stability of QLED devices becomes a critical challenge for industrialization. In this perspective we highlight the stability challenges in advancing QLED-based display technologies, with a focus on thermodynamic considerations, carrier dynamics, and materials degradation. Based on the analysis of thermodynamics and carrier dynamics, it is more challenging to achieve long-lived blue QLED devices due to their high input power, high photon flux, severe charge accumulation, and strong bulk-surface coupling. Combining the equivalent circuit model and p–n junction theory, stability-related carrier dynamics can be clarified to understand the degradation mechanisms of the operational devices. Finally, in addition to chemical/electrochemical reactions in QLED devices, the intrinsic material stability with/without an electric field needs to be further investigated, which provides additional material selection guides in developing prototype devices. We hope this Viewpoint can motivate more fundamental research on the stability issues of QLEDs toward industrialization.</p>","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"16 39","pages":"10058–10070"},"PeriodicalIF":4.6,"publicationDate":"2025-10-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145195636","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"Electron-Induced Fragmentation of 5-Iodouridine: Implications for Enhanced Radiotherapy.","authors":"Janina Kopyra,Paulina Wierzbicka,Hassan Abdoul-Carime","doi":"10.1021/acs.jpclett.5c01615","DOIUrl":"https://doi.org/10.1021/acs.jpclett.5c01615","url":null,"abstract":"5-Iodouridine is a known and potentially efficient radiosensitizer; however, it has not been considered for clinical use because of its poor metabolic incorporation into DNA. Recent development of a novel pro-drug, ropidoxuridine, has improved the bioavailability of this halogenated nucleoside, although the exact mechanism of its radiosensitizing action remains not fully elucidated. Here, we demonstrate that low-energy electrons─abundantly generated along radiation tracks─efficiently dissociate the halogenated nucleoside via the primary pathway (99%), producing an iodine anion and a uridine-yl• neutral radical, with a high approximate DEA cross section of (2.7 ± 1.9)×10-14 cm2. The latter, known to be highly reactive, subsequently induces hydrogen abstraction, leading to DNA strand breaks. The damage induced in 5IUrd by low-energy electrons is found to be about 700 times greater than that in thymidine and about 4 times that of the clinically used 5-fluorouridine. These findings may contribute to the development of future cancer therapy strategies by synergistically combining 5IUrd with cisplatin or gold nanoparticles, which act as a source of secondary low-energy electrons during radiation therapy.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"100 1","pages":"10536-10541"},"PeriodicalIF":6.475,"publicationDate":"2025-10-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145209040","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"Proton-Tuned Surface Chemistry Promotes Multicarbon Formation in Acidic CO2 Electroreduction.","authors":"Qingqing Song,Feng Li,Aoni Xu,Chenchen Zhang,Yuanming Xie,Junjun Mao,Ying Zhang,Yong Zhao","doi":"10.1021/acs.jpclett.5c02529","DOIUrl":"https://doi.org/10.1021/acs.jpclett.5c02529","url":null,"abstract":"Carbon dioxide electroreduction to multicarbon (C2+) products in strongly acidic media offers a promising approach to mitigate carbon loss observed in alkaline and neutral electrolytes. However, achieving high C2+ selectivity at energy-efficient current densities remains challenging due to competing one-carbon (C1) product generation. Here, we report a proton-availability-promoted C2+ production in acidic CO2 electroreduction within a moderate current density regime. We demonstrated a remarkably enhanced C2+ production─C2+ faradaic efficiency increasing from 23.9 ± 2.7% to 48.1 ± 0.6% and C2+/C1 ratio from 0.4 to 1.6─by increasing the proton concentration from pH 2 to pH 1 in the bulk acidic electrolyte. Our in situ Raman spectroscopy and simulation studies revealed that higher proton concentration enhances *CO coverage and favors a low-frequency *CO binding configuration on copper surface, thereby facilitating C-C coupling and promoting C2+ product formation.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"6 1","pages":"10499-10505"},"PeriodicalIF":6.475,"publicationDate":"2025-10-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145203676","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Umamahesh Thupakula,Shen Chen,Yong Han,Michael C Tringides,Marek Kolmer
{"title":"Subsurface Interface Structure Controlling Local Electronic Properties of Epitaxial Graphene on SiC(0001).","authors":"Umamahesh Thupakula,Shen Chen,Yong Han,Michael C Tringides,Marek Kolmer","doi":"10.1021/acs.jpclett.5c02179","DOIUrl":"https://doi.org/10.1021/acs.jpclett.5c02179","url":null,"abstract":"Recently realized high-mobility semiconducting epitaxial graphene on silicon carbide (SiC) [Zhao, J. Nature 2024, 625 (7993), 60-65, 10.1038/s41586-023-06811-0] provided an important step toward integration of the graphene-based system into active components in postsilicon micro- and nanoelectronics. However, the exact atomic-scale structure and complex bonding configurations of the first epitaxial graphene carbon layer (Cbuffer) remain an open problem. Our recent report [Kolmer, M. Communications Physics 2024, 7 (1), 16, 10.1038/s42005-023-01515-3] has shed new light on understanding this interface, where the external transverse electric field-dependent dynamic switching behavior of the Cbuffer-SiC bonds was observed. Here, using scanning tunneling microscopy and spectroscopy (STM and STS), we present direct evidence of silicon (Si) vacancies at the interface and provide their distribution at the topmost reconstructed SiC(0001) layer. Bias voltage and epitaxial graphene thickness-dependent characterization of the collective Cbuffer-SiC interface showed that \"Si\" vacancy sites beneath Cbuffer are stable under STM electric fields. Moreover, the vacancies introduce localized electronic states below the Fermi level, thereby enhancing the charge-transfer phenomenon across the interface.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"50 1","pages":"10487-10498"},"PeriodicalIF":6.475,"publicationDate":"2025-10-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145203891","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Jing Dong,Hai-Feng Su,Fengwei Zhang,Yu-Xin Wang,Linfeng Liang,Huan Li
{"title":"Real-Time Kinetic Control in the Electrosynthesis of Au10Ag4 Nanoclusters Via Electrical Signal Modulation.","authors":"Jing Dong,Hai-Feng Su,Fengwei Zhang,Yu-Xin Wang,Linfeng Liang,Huan Li","doi":"10.1021/acs.jpclett.5c02653","DOIUrl":"https://doi.org/10.1021/acs.jpclett.5c02653","url":null,"abstract":"Conventional coinage metal nanocluster (NC) synthesis usually requires premixing reagents in bulk solution until thermodynamic equilibrium, inherently precluding on-demand kinetic manipulation. This study reports the first electrosynthesis of a bimetallic NC with atomic precision, demonstrating real-time kinetic control via electrical signal modulations. Key findings reveal that (1) pulsed potential suppresses cathodic deposition more effectively than constant potential; (2) reaction kinetics exhibit a volcano-shaped dependence on pulse duration, with optimal performance at ∼ 10 s; (3) reactions can be instantaneously switched on or off by applying or removing the potential; and (4) reaction rates are precisely tunable via pulse off-time adjustment. This work establishes an electrical signal-modulated strategy for real-time reaction control, presenting a viable strategy for the programmable and controllable synthesis of metal NCs.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"10 1","pages":"10514-10520"},"PeriodicalIF":6.475,"publicationDate":"2025-10-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145209240","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"Light-Powered Transport of Organic Anions by Microbial Rhodopsins.","authors":"Simiao Shen,Shoichiro Akita,Joji Wada,Mako Eguchi,Takashi Tsukamoto,Kwang-Hwan Jung,Yuki Sudo,Takashi Kikukawa","doi":"10.1021/acs.jpclett.5c02551","DOIUrl":"https://doi.org/10.1021/acs.jpclett.5c02551","url":null,"abstract":"Microbial rhodopsins are photoactive membrane proteins known for transporting small inorganic ions such as H+, Cl-, and Na+. Their compact structure─comprising seven transmembrane helices─has long been thought to limit their substrate range to such ions. Here, we report that several anion-pumping rhodopsins can also transport organic anions. In particular, a rhodopsin from cyanobacteria transports bulky organic anions, including those with a benzene ring, with volumes up to ∼120 Å3─five times larger than Cl-. These anions bind in the dark state and are translocated upon photoactivation, via a mechanism similar to Cl-. Notably, only anions with pKa values below 2 are transported, suggesting that negative charge is essential for binding. This study provides the first evidence that naturally occurring proteins can use light to transport organic compounds across membranes. These findings broaden the functional scope of microbial rhodopsins and open new possibilities for light-driven transport of organic ions.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"98 1","pages":"10528-10535"},"PeriodicalIF":6.475,"publicationDate":"2025-10-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145209233","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}