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Nitric oxide-generating metallic wires for enhanced metal implants 用于增强金属植入物的一氧化氮生成金属丝
IF 7.5 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY Pub Date : 2024-07-17 DOI: 10.1038/s43246-024-00564-7
Federico Mazur, Yingzhu Zhou, Gervase Ng, Qingqing Fan, Andy-Hoai Pham, Cyrille Boyer, Rona Chandrawati
Metallic implants are integral in modern medicine, offering excellent biocompatibility and mechanical properties. However, implant-related infections pose a major challenge. Current drug delivery methods, such as surface-coated and drug-eluting implants, are limited by finite drug supplies and complex manufacturing steps. Recent approaches like local drug synthesis, including enzyme-prodrug therapies, present innovative solutions but are hampered by the inherent limitations of enzymes as well as complex procedures. Here, we introduce a simpler alternative: using the intrinsic properties of implant materials to activate prodrugs. Through a simple thermal treatment, metallic implants gain catalytic properties to locally generate nitric oxide, an antibacterial agent. Our findings show this treatment is non-toxic to cells, does not affect cell proliferation rates, and effectively inhibits bacterial biofilm formation. This material-driven approach eliminates the need for external chemical or enzymatic interventions, offering a promising solution to prevent implant-related infections and improve patient outcomes in implant medicine. There are multiple strategies to tackle metallic implant-related infections, but they are complex. Here, a simple thermal treatment process endows metallic implant materials with catalytic properties to locally generate nitric oxide as an effective antibacterial agent.
金属植入物具有良好的生物相容性和机械性能,是现代医学不可或缺的一部分。然而,与植入物相关的感染是一项重大挑战。目前的给药方法,如表面涂层和药物洗脱植入物,受到药物供应有限和制造步骤复杂的限制。最近的方法,如局部药物合成,包括酶促药物疗法,提出了创新的解决方案,但受到酶固有的局限性和复杂程序的阻碍。在此,我们介绍一种更简单的替代方法:利用植入材料的固有特性激活原药。通过简单的热处理,金属植入物可获得催化特性,在局部产生一氧化氮(一种抗菌剂)。我们的研究结果表明,这种处理方法对细胞无毒,不影响细胞增殖率,并能有效抑制细菌生物膜的形成。这种材料驱动的方法无需外部化学或酶干预,为预防植入物相关感染和改善植入物医疗的患者预后提供了一种前景广阔的解决方案。解决金属植入物相关感染有多种策略,但都很复杂。在这里,一种简单的热处理工艺赋予了金属植入材料催化特性,可在局部生成一氧化氮作为有效的抗菌剂。
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引用次数: 0
Anion-cation interactions dictate safe and stable electrolytes for sodium-ion batteries 阴阳离子相互作用决定了钠离子电池电解质的安全性和稳定性
IF 7.5 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY Pub Date : 2024-07-08 DOI: 10.1038/s43246-024-00556-7
Jet-Sing M. Lee
Sodium-ion battery safety can be improved by using non-flammable electrolytes, but they are traditionally incompatible with carbon-based anodes. Now, low-concentration phosphate electrolytes modulated by anion-cation interactions are shown to work well with standard electrodes, displaying stable operation over a wide temperature range.
使用不易燃的电解质可以提高钠离子电池的安全性,但这些电解质传统上与碳基阳极不兼容。现在,通过阴阳离子相互作用调制的低浓度磷酸盐电解质已证明能与标准电极很好地配合使用,并能在很宽的温度范围内稳定工作。
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引用次数: 0
Particle-hole mixed Bogoliubov quasiparticles and Cooper instability in single-unit-cell FeSe/SrTiO3 films 单单元电池 FeSe/SrTiO3 薄膜中的粒子-空穴混合波哥留布夫准粒子和库珀不稳定性
IF 7.5 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY Pub Date : 2024-07-06 DOI: 10.1038/s43246-024-00554-9
Zhiyuan Wei, Shaozhi Li, Bo Liu, Xiupeng Sun, Yinqi Hu, Shuai Sun, Shuting Peng, Yang Luo, Linwei Huai, Jianchang Shen, Bingqian Wang, Yu Miao, Zhipeng Ou, Yao Wang, Kun Jiang, Junfeng He
In conventional superconductors, Bogoliubov quasiparticles and Cooper instability provide a paradigm to describe the superconducting state and the superconducting transition, respectively. However, whether these concepts can be adapted to describe Fe-based superconductors requires rigorous examinations from experiments. Here, we report angle-resolved photoemission studies on single-layer FeSe films grown on SrTiO3 substrate. Due to the improved clarity, our results reveal both particle and hole branches of the energy band with clear quasiparticles. The dispersion and coherence factors are extracted, which unveil the particle-hole mixed Bogoliubov quasiparticles in the superconducting state of the FeSe/STO films. Effective pairing susceptibility is also deduced as a function of temperature, which indicates the persistence of Cooper instability in Fe-based superconductors. It is still under debate whether unconventional superconductors can still be described in terms of Bogoliubov quasiparticles in the superconducting state. Here, angle-resolved photoemission spectroscopy measurements on FeSe/SrTiO3 films reveal particle-hole mixed Bogoliubov quasiparticles, despite the likely unconventional pairing mechanism.
在传统超导体中,Bogoliubov 准粒子和库珀不稳定性分别为描述超导状态和超导转变提供了范例。然而,这些概念能否适用于描述铁基超导体,还需要实验的严格检验。在此,我们报告了在 SrTiO3 衬底上生长的单层 FeSe 薄膜的角度分辨光发射研究。由于清晰度的提高,我们的结果揭示了能带的粒子和空穴分支,并具有清晰的准粒子。通过提取弥散因子和相干因子,我们揭示了 FeSe/STO 薄膜超导态中的粒子-空穴混合 Bogoliubov 准粒子。此外,还推导出了有效配对感度与温度的函数关系,这表明在铁基超导体中存在库珀不稳定性。非常规超导体是否仍能用超导状态下的波哥留布夫准粒子来描述,目前仍存在争议。在这里,对 FeSe/SrTiO3 薄膜进行的角度分辨光发射光谱测量揭示了粒子-空穴混合的 Bogoliubov 准粒子,尽管其配对机制可能是非常规的。
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引用次数: 0
Optoelectronic properties of electron-acceptor molecules adsorbed on graphene/silicon carbide interfaces 吸附在石墨烯/碳化硅界面上的电子受体分子的光电特性
IF 7.5 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY Pub Date : 2024-07-04 DOI: 10.1038/s43246-024-00549-6
Masoud Mansouri, Cristina Díaz, Fernando Martín
Silicon carbide has emerged as an optimal semiconducting support for graphene growth. In previous studies, the formation of an interfacial graphene-like buffer layer covalently bonded to silicon carbide has been observed, revealing electronic properties distinct from ideal graphene. Despite extensive experimental efforts dedicated to this interface, theoretical investigations have been confined to its ground state. Here, we use many-body perturbation theory to study the electronic and optical characteristics of this interface and demonstrate its potential for optoelectronics. By adsorbing graphene, we show that the quasiparticle band structure exhibits a reduced bandgap, associated with an optical onset in the visible energy window. Furthermore, we reveal that the absorption of two prototypical electron-accepting molecules on this substrate results in a significant renormalization of the adsorbate gap, giving rise to distinct low-lying optically excited states in the near-infrared region. These states are well-separated from the substrate’s absorption bands, ensuring wavelength selectivity for molecular optoelectronic applications. The electronic features of graphene/silicon carbide have been well studied experimentally but theoretical investigations are still preliminary. Here, many-body perturbation theory reveals the electronic and optical characteristics of this interface and shows its advantages for optoelectronics.
碳化硅已成为石墨烯生长的最佳半导体支持物。在之前的研究中,已经观察到与碳化硅共价键结合的类似石墨烯的界面缓冲层的形成,揭示了不同于理想石墨烯的电子特性。尽管针对该界面进行了大量实验,但理论研究一直局限于其基态。在这里,我们使用多体扰动理论来研究这一界面的电子和光学特性,并证明其在光电子学方面的潜力。通过吸附石墨烯,我们发现准粒子带结构呈现出带隙减小的现象,这与可见光能窗口中的光学起始点有关。此外,我们还揭示了在这种基底上吸收两种典型的电子接受分子会导致吸附剂间隙的显著重规范化,从而在近红外区域产生独特的低洼光激发态。这些态与基底的吸收带完全分离,确保了分子光电应用的波长选择性。石墨烯/碳化硅的电子特性已得到深入的实验研究,但理论研究仍处于初步阶段。在此,多体扰动理论揭示了这一界面的电子和光学特性,并显示了其在光电子学方面的优势。
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引用次数: 0
Face-centered cubic carbon as a fourth basic carbon allotrope with properties of intrinsic semiconductors and ultra-wide bandgap 面心立方碳作为第四种基本碳同素异形体,具有本征半导体和超宽带隙特性
IF 7.5 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY Pub Date : 2024-07-02 DOI: 10.1038/s43246-024-00547-8
Igor Konyashin, Ruslan Muydinov, Antonio Cammarata, Andrey Bondarev, Marin Rusu, Athanasios Koliogiorgos, Tomáš Polcar, Daniel Twitchen, Pierre-Olivier Colard, Bernd Szyszka, Nicola Palmer
Carbon is considered to exist in three basic forms: diamond, graphite/graphene/fullerenes, and carbyne, which differ in a type of atomic orbitals hybridization. Since several decades the existence of the fourth basic carbon allotropic form with the face-centered cubic (fcc) crystal lattice has been a matter of discussion despite clear evidence for its laboratory synthesis and presence in nature. Here, we obtain this carbon allotrope in form of epitaxial films on diamond in a quantity sufficient to perform their comprehensive studies. The carbon material has an fcc crystal structure, shows a negative electron affinity, and is characterized by a peculiar hybridization of the valence atomic orbitals. Its bandgap (~6 eV) is typical for insulators, whereas the noticeable electrical conductivity (~0.1 S m−1) increases with temperature, which is typical for semiconductors. Ab initio calculations explain this apparent contradiction by noncovalent sharing p-electrons present in the uncommon valence band structure comprising an intraband gap. This carbon allotrope can create a new pathway to ‘carbon electronics’ as the first intrinsic semiconductor with an ultra-wide bandgap. Carbon is known to exist in three basic allotropes depending on the hybridization of s and p orbitals: diamond, graphite/graphene/fullerenes, and carbyne. Here, a fourth carbon allotrope with a face-centered cubic crystal lattice and peculiar hybridization of atoms is obtained in the form of epitaxial films on diamond, showing an ultra-wide bandgap and semiconductor electronic behavior.
碳被认为以三种基本形式存在:金刚石、石墨/石墨烯/富勒烯和碳化烯,它们在原子轨道杂化类型上有所不同。几十年来,第四种基本碳同素异形体(面心立方(fcc)晶格)的存在一直是一个讨论的问题,尽管有明确的证据表明它可以在实验室合成并存在于自然界中。在这里,我们以金刚石外延薄膜的形式获得了这种碳同素异形体,其数量足以对其进行全面研究。这种碳材料具有 fcc 晶体结构,显示出负电子亲和性,并以价电子轨道的奇特杂化为特征。它的带隙(约 6 eV)是典型的绝缘体,而明显的电导率(约 0.1 S m-1)却随温度升高而增加,这是典型的半导体。Ab initio 计算解释了这一明显的矛盾,因为在不常见的价带结构中存在非共价共享 p 电子,从而形成带内间隙。这种碳同素异形体作为第一种具有超宽带隙的本征半导体,可以为 "碳电子学 "开辟一条新的道路。根据 s 和 p 轨道的杂化情况,已知碳有三种基本的同素异形体:金刚石、石墨/石墨烯/富勒烯和碳化烯。在这里,我们以金刚石外延薄膜的形式获得了第四种碳同素异形体,它具有面心立方晶格和奇特的原子杂化,显示出超宽带隙和半导体电子行为。
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引用次数: 0
All-photonic artificial synapses based on photochromic perovskites for noncontact neuromorphic visual perception 基于光致变色过氧化物的全光子人工突触,用于非接触式神经形态视觉感知
IF 7.5 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY Pub Date : 2024-07-02 DOI: 10.1038/s43246-024-00553-w
Xing Zhou, Fangzhen Hu, Qing Hou, Jinming Hu, Yimeng Wang, Xi Chen
Recently optoelectronic synapses generating light-driven electrical memories have played a vital role in the neuromorphic computing of visual perception. However, all the optoelectronic synapses demonstrate photoelectric conversion. Peripheral circuits are used for contact photocurrent measurement, leading to significant energy consumption and impeding the evolution of optical wireless communication. It is crucial to develop noncontact neuromorphic visual perception based on light-driven photonic memories. Herein, we report all-photonic artificial synapses based on photochromic perovskites. Triggered by ultraviolet and visible light pulses, cesium lead iodide bromine induces a structural disorder. Optical transmittance changes induced by the disorder last after the pulses are gone. Next, the photonic memories are propagated in the air and processed by a recurrent neural network. The accuracy of binary image recognition is instantly stabilized at 1.0, and accuracy above 0.8 after 7 epochs is achieved in the recognition of digitals from 0 to 9. The all-photonic synapses realize remote perception with zero in-situ energy consumption and enable artificial sensory systems with low-power computation, remote control, and ultrahigh propagation speed. Optoelectronic synapses are key to artificial visual perception systems based on neuromorphic computing, but they typically rely on photoelectric conversion and peripheral circuits that are energy consuming and prevent optical wireless communication. Here, all-photonic artificial synapses with light-driven optical transmittance memories are fabricated based on photochromic CsPbIBr2 perovskite thin films.
最近,产生光驱动电子记忆的光电突触在视觉感知的神经形态计算中发挥了重要作用。然而,所有光电突触都需要进行光电转换。外围电路用于接触式光电流测量,导致大量能源消耗,阻碍了光无线通信的发展。开发基于光驱动光子记忆的非接触式神经形态视觉感知至关重要。在此,我们报告了基于光致变色过氧化物的全光子人工突触。在紫外线和可见光脉冲的触发下,碘化铯铅溴会诱发结构紊乱。在脉冲消失后,由紊乱引起的光学透射率变化仍会持续。接下来,光子记忆在空气中传播,并由递归神经网络进行处理。二进制图像识别的准确度瞬间稳定在 1.0,而 0 至 9 的数字识别准确度在 7 个历时后达到 0.8 以上。全光子突触实现了零原位能耗的远程感知,并使人工感觉系统具备低功耗计算、远程控制和超高传播速度的能力。光电突触是基于神经形态计算的人工视觉感知系统的关键,但它们通常依赖于光电转换和外围电路,而光电转换和外围电路既耗能又妨碍光无线通信。在此,我们基于光致变色的 CsPbIBr2 包晶体薄膜,制造出了具有光驱动光透射存储器的全光子人工突触。
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引用次数: 0
Perturbation-tuned triple spiral metamagnetism and tricritical point in kagome metal ErMn6Sn6 神户金属 ErMn6Sn6 中的扰动调谐三螺旋元磁性和三临界点
IF 7.5 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY Pub Date : 2024-07-01 DOI: 10.1038/s43246-024-00552-x
Satya Shanmukharao Samatham, Jacob Casey, Adrienn Maria Szucs, Venkateswara Yenugonda, Christopher Burgio, Theo Siegrist, Arjun K. Pathak
Kagome materials are of topical interest for their diverse quantum properties linked with correlated magnetism and topology. Here, we report anomalous hydrostatic pressure (p) effect on ErMn6Sn6 through isobaric and isothermal-isobaric magnetization measurements. Magnetic field (H) suppresses antiferromagnetic TN while simultaneously enhancing the ferrimagnetic TC by exhibiting dual metamagnetic transitions, arising from the triple-spiral-nature of Er and Mn spins. Counter-intuitively, pressure enhances both TC and TN with a growth rate of 74.4 K GPa−1 and 14.4 K GPa−1 respectively. Pressure unifies the dual metamagnetic transitions as illustrated through p-H phase diagrams at 140 and 200 K. Temperature-field-pressure (T-H, T-p) phase diagrams illustrate distinct field- and pressure-induced critical points at (Tcr = 246 K, Hcr = 23.3 kOe) and (Tcr = 435.8 K, pcr = 4.74 GPa) respectively. An unusual increase of magnetic entropy by pressure around Tcr and a putative pressure-induced tricritical point pave a unique way of tuning the magnetic properties of kagome magnets through simultaneous application of H and p. The kagome metal ErMn6Sn6 is known to display interesting physics. Here, the simultaneous effect of a magnetic field and pressure is investigated, revealing the role of the spiral behavior of magnetic layers on magnetic transition temperatures
卡戈米材料因其与相关磁性和拓扑学有关的各种量子特性而备受关注。在这里,我们通过等压和等温-等压磁化测量,报告了 ErMn6Sn6 的反常静水压力(p)效应。磁场(H)在抑制反铁磁性 TN 的同时,还通过 Er 和 Mn 自旋的三重螺旋性质所产生的双元磁转变,增强了铁磁性 TC。与直觉相反的是,压力会同时增强 TC 和 TN,增长率分别为 74.4 K GPa-1 和 14.4 K GPa-1。温度-场-压力(T-H、T-p)相图显示,在(Tcr = 246 K,Hcr = 23.3 kOe)和(Tcr = 435.8 K,pcr = 4.74 GPa)分别存在不同的场临界点和压力临界点。在 Tcr 附近的压力作用下磁性熵的不寻常增加以及假定的压力诱导三临界点为通过同时应用 H 和 p 来调整卡戈梅磁体的磁性铺平了一条独特的道路。这里研究了磁场和压力的同时效应,揭示了磁层的螺旋行为对磁转变温度的作用
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引用次数: 0
Ultra-fast perovskite electro-optic modulator and multi-band transmission up to 300 Gbit s−1 超高速包晶电光调制器和高达 300 Gbit s-1 的多波段传输
IF 7.5 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY Pub Date : 2024-07-01 DOI: 10.1038/s43246-024-00558-5
Jiawei Mao, Futa Uemura, Sahar Alasvand Yazdani, Yuexin Yin, Hiromu Sato, Guo-Wei Lu, Shiyoshi Yokoyama
The gap between the performance of optoelectronic components and the demands of fiber-optic communications has narrowed significantly in recent decades. Yet, the expansion of data communications traffic remains substantial, with fiber-link speeds increases anticipated in the near future. Here, we demonstrate an ultra-high-speed electro-optic waveguide modulator constructed using a thin film of lanthanum-modified lead zirconate titanate with a ferroelectric phase exhibiting a strong Pockels effect. The modulator has a wide optical window; thus, the modulation was demonstrated for 1550 and 1310 nm wavelengths. This device showed electro-optical intensity signaling with line rates of 172 Gbit s−1, in conjunction with on–off keying modulation; this performance could be increased to 304 Gbit s−1 using four-level pulse modulation. The signaling performance of this modulator was found to be robust, with stable performance at temperatures as high as 100 °C. This technology is expected to have applications in a wide range of classical optoelectronic devices and in quantum science and technology. Advanced fiber-optic communications rely on electro-optic materials with suitable properties. Here a perovskite oxide, lanthanum-modified lead zirconate titanate, is used to fabricate a waveguide modulator with line rates as high as 304 Gbit/s using four-level pulse modulation.
近几十年来,光电元件的性能与光纤通信需求之间的差距已大大缩小。然而,数据通信流量仍在大幅增长,预计在不久的将来光纤链路的速度也会提高。在此,我们展示了一种超高速电光波导调制器,该调制器采用了镧改性锆钛酸铅薄膜,其铁电相位具有很强的波克尔斯效应。该调制器具有较宽的光学窗口;因此,在 1550 和 1310 nm 波长下均可进行调制。结合通断键控调制,该设备显示出线路速率为 172 Gbit s-1 的电光强度信号;使用四级脉冲调制,这一性能可提高到 304 Gbit s-1。研究发现,这种调制器的信号传输性能十分稳定,在高达 100 °C 的温度下也能保持稳定。这项技术有望广泛应用于经典光电器件和量子科技领域。先进的光纤通信依赖于具有合适特性的电光材料。在这里,一种包晶氧化物--镧改性锆钛酸铅--被用来制造波导调制器,利用四级脉冲调制,线路速率高达 304 Gbit/s。
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引用次数: 0
Predicting plastron thermodynamic stability for underwater superhydrophobicity 预测水下超疏水的质点热力学稳定性
IF 7.5 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY Pub Date : 2024-06-29 DOI: 10.1038/s43246-024-00555-8
Alexander B. Tesler, Heikki A. Nurmi, Stefan Kolle, Lucia H. Prado, Bhuvaneshwari Karunakaran, Anca Mazare, Ina Erceg, Íris de Brito Soares, George Sarau, Silke Christiansen, Shane Stafslien, Jack Alvarenga, Joanna Aizenberg, Ben Fabry, Robin H. A. Ras, Wolfgang H. Goldmann
Non-wettable surfaces, especially those capable of passively trapping air in rough protrusions, can provide surface resilience to the detrimental effects of wetting-related phenomena. However, the development of such superhydrophobic surfaces with a long-lasting entrapped air layer, called plastron, is hampered by the lack of evaluation criteria and methods that can unambiguously distinguish between stable and metastable Cassie-Baxter wetting regimes. The information to evaluate the stability of the wetting regime is missing from the commonly used contact angle goniometry. Therefore, it is necessary to determine which surface features can be used as a signature to identify thermodynamically stable plastron. Here, we describe a methodology for evaluating the thermodynamic underwater stability of the Cassie-Baxter wetting regime of superhydrophobic surfaces by measuring the surface roughness, solid-liquid area fraction, and Young’s contact angle. The method allowed the prediction of passive plastron stability for over one year of continuous submersion, the impeding of mussel and barnacle adhesion, and inhibition of metal corrosion in seawater. Such submersion-stable superhydrophobicity, in which water is repelled by a stable passive air layer trapped between the solid substrate and the surrounding liquid for extended periods at ambient conditions, opens new avenues for science and technologies that require continuous contact of solids with aqueous media. Upon submersion, a superhydrophobic surface can trap a layer of air, termed “plastron”, that separates it from the surrounding liquid. Here, methodology is reported for predicting the thermodynamic stability of plastron by measuring surface roughness, solid-liquid area fraction, and Young’s contact angle.
非润湿表面,尤其是那些能够在粗糙突起中被动捕获空气的表面,可以提供表面弹性,抵御与润湿相关现象的有害影响。然而,由于缺乏能够明确区分稳定和非稳定卡西-巴克斯特润湿机制的评估标准和方法,这种具有持久夹带空气层(称为plastron)的超疏水性表面的开发受到了阻碍。常用的接触角测角法缺乏评估润湿机制稳定性的信息。因此,有必要确定哪些表面特征可作为识别热力学稳定质点的标志。在此,我们介绍了一种通过测量表面粗糙度、固液面积分数和杨氏接触角来评估超疏水表面卡西-巴克斯特润湿机制的热力学水下稳定性的方法。该方法可预测连续浸没一年以上的被动底盘稳定性、对贻贝和藤壶粘附的阻碍以及对海水中金属腐蚀的抑制。这种浸没稳定的超疏水性,即在环境条件下,固体基底和周围液体之间的稳定被动空气层能长时间排斥水,为需要固体与水介质持续接触的科学和技术开辟了新的途径。超疏水表面在浸入水中后会捕获一层空气,称为 "plastron",将其与周围的液体隔开。本文报告了通过测量表面粗糙度、固液面积分数和杨氏接触角来预测 plastron 热力学稳定性的方法。
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引用次数: 0
Resonance theory of vibrational strong coupling enhanced polariton chemistry and the role of photonic mode lifetime 振动强耦合增强极化子化学共振理论及光子模式寿命的作用
IF 7.5 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY Pub Date : 2024-06-28 DOI: 10.1038/s43246-024-00551-y
Wenxiang Ying, Pengfei Huo
Recent experiments demonstrate polaritons under the vibrational strong coupling (VSC) regime can modify chemical reactivity. Here, we present a complete theory of VSC-modified rate constants when coupling a single molecule to an optical cavity, where the role of photonic mode lifetime is understood. The analytic expression exhibits a sharp resonance behavior, where the maximum rate constant is reached when the cavity frequency matches the vibration frequency. The theory explains why VSC rate constant modification closely resembles the optical spectra of the vibration outside the cavity. Further, we discussed the temperature dependence of the VSC-modified rate constants. The analytic theory agrees well with the numerically exact hierarchical equations of motion (HEOM) simulations for all explored regimes. Finally, we discussed the resonance condition at the normal incidence when considering in-plane momentum inside a Fabry-Pérot cavity. Polariton chemistry, namely the coupling of molecular vibrations to quantized radiation modes inside an optical microcavity, offers a promising strategy to modify chemical reactivities. Here, the authors provide a comprehensive theory of how vibrational strong coupling modifies chemical reaction rates in different cavity regimes.
最近的实验证明,振动强耦合(VSC)机制下的极化子可以改变化学反应活性。在此,我们提出了单分子与光腔耦合时的 VSC 修正速率常数的完整理论,并理解了光子模式寿命的作用。解析表达式显示了一种尖锐的共振行为,当空腔频率与振动频率相匹配时,速率常数达到最大值。该理论解释了为什么 VSC 速率常数的变化与腔外振动的光学光谱非常相似。此外,我们还讨论了 VSC 修正速率常数的温度依赖性。分析理论与针对所有探究机制的精确分层运动方程(HEOM)数值模拟结果十分吻合。最后,我们讨论了在法布里-佩罗腔内考虑面内动量时的法线入射共振条件。极化子化学,即分子振动与光学微腔内量子化辐射模式的耦合,为改变化学反应活性提供了一种前景广阔的策略。在此,作者提供了振动强耦合如何改变不同空腔状态下化学反应速率的综合理论。
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引用次数: 0
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Communications Materials
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