Structural Dynamics-Us最新文献

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Laboratory diffracted x-ray blinking to monitor picometer motions of protein molecules and application to crystalline materials. 实验室衍射x射线眨眼监测蛋白质分子的皮米运动和应用于晶体材料。
IF 2.8 2区 物理与天体物理
Structural Dynamics-Us Pub Date : 2021-07-08 eCollection Date: 2021-07-01 DOI: 10.1063/4.0000112
Tatsuya Arai, Rena Inamasu, Hiroki Yamaguchi, Daisuke Sasaki, Ayana Sato-Tomita, Hiroshi Sekiguchi, Kazuhiro Mio, Sakae Tsuda, Masahiro Kuramochi, Yuji C Sasaki
{"title":"Laboratory diffracted x-ray blinking to monitor picometer motions of protein molecules and application to crystalline materials.","authors":"Tatsuya Arai,&nbsp;Rena Inamasu,&nbsp;Hiroki Yamaguchi,&nbsp;Daisuke Sasaki,&nbsp;Ayana Sato-Tomita,&nbsp;Hiroshi Sekiguchi,&nbsp;Kazuhiro Mio,&nbsp;Sakae Tsuda,&nbsp;Masahiro Kuramochi,&nbsp;Yuji C Sasaki","doi":"10.1063/4.0000112","DOIUrl":"https://doi.org/10.1063/4.0000112","url":null,"abstract":"<p><p>In recent years, real-time observations of molecules have been required to understand their behavior and function. To date, we have reported two different time-resolved observation methods: diffracted x-ray tracking and diffracted x-ray blinking (DXB). The former monitors the motion of diffracted spots derived from nanocrystals labeled onto target molecules, and the latter measures the fluctuation of the diffraction intensity that is highly correlated with the target molecular motion. However, these reports use a synchrotron x-ray source because of its high average flux, resulting in a high time resolution. Here, we used a laboratory x-ray source and DXB to measure the internal molecular dynamics of three different systems. The samples studied were bovine serum albumin (BSA) pinned onto a substrate, antifreeze protein (AFP) crystallized as a single crystal, and poly{2-(perfluorooctyl)ethyl acrylate} (PC<sub>8</sub>FA) polymer between polyimide sheets. It was found that not only BSA but also AFP and PC<sub>8</sub>FA molecules move in the systems. In addition, the molecular motion of AFP molecules was observed to increase with decreasing temperature. The rotational diffusion coefficients (D<sub>R</sub>) of BSA, AFP, and PC<sub>8</sub>FA were estimated to be 0.73 pm<sup>2</sup>/s, 0.65 pm<sup>2</sup>/s, and 3.29 pm<sup>2</sup>/s, respectively. Surprisingly, the D<sub>R</sub> of the PC<sub>8</sub>FA polymer was found to be the highest among the three samples. This is the first report that measures the molecular motion of a single protein crystal and polymer by using DXB with a laboratory x-ray source. This technique can be applied to any kind of crystal and crystalline polymer and provides atomic-order molecular information.</p>","PeriodicalId":48683,"journal":{"name":"Structural Dynamics-Us","volume":null,"pages":null},"PeriodicalIF":2.8,"publicationDate":"2021-07-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://sci-hub-pdf.com/10.1063/4.0000112","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"39181542","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"物理与天体物理","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 6
Real-time interfacial electron dynamics revealed through temporal correlations in x-ray photoelectron spectroscopy. 通过x射线光电子能谱的时间相关性揭示的实时界面电子动力学。
IF 2.8 2区 物理与天体物理
Structural Dynamics-Us Pub Date : 2021-07-08 eCollection Date: 2021-07-01 DOI: 10.1063/4.0000099
Felix Brausse, Mario Borgwardt, Johannes Mahl, Matthew Fraund, Friedrich Roth, Monika Blum, Wolfgang Eberhardt, Oliver Gessner
{"title":"Real-time interfacial electron dynamics revealed through temporal correlations in x-ray photoelectron spectroscopy.","authors":"Felix Brausse,&nbsp;Mario Borgwardt,&nbsp;Johannes Mahl,&nbsp;Matthew Fraund,&nbsp;Friedrich Roth,&nbsp;Monika Blum,&nbsp;Wolfgang Eberhardt,&nbsp;Oliver Gessner","doi":"10.1063/4.0000099","DOIUrl":"https://doi.org/10.1063/4.0000099","url":null,"abstract":"<p><p>We present a novel technique to monitor dynamics in interfacial systems through temporal correlations in x-ray photoelectron spectroscopy (XPS) signals. To date, the vast majority of time-resolved x-ray spectroscopy techniques rely on pump-probe schemes, in which the sample is excited out of equilibrium by a pump pulse, and the subsequent dynamics are monitored by probe pulses arriving at a series of well-defined delays relative to the excitation. By definition, this approach is restricted to processes that can either directly or indirectly be initiated by light. It cannot access spontaneous dynamics or the microscopic fluctuations of ensembles in chemical or thermal equilibrium. Enabling this capability requires measurements to be performed in real (laboratory) time with high temporal resolution and, ultimately, without the need for a well-defined trigger event. The time-correlation XPS technique presented here is a first step toward this goal. The correlation-based technique is implemented by extending an existing optical-laser pump/multiple x-ray probe setup by the capability to record the kinetic energy and absolute time of arrival of every detected photoelectron. The method is benchmarked by monitoring energy-dependent, periodic signal modulations in a prototypical time-resolved XPS experiment on photoinduced surface-photovoltage dynamics in silicon, using both conventional pump-probe data acquisition, and the new technique based on laboratory time. The two measurements lead to the same result. The findings provide a critical milestone toward the overarching goal of studying equilibrium dynamics at surfaces and interfaces through time correlation-based XPS measurements.</p>","PeriodicalId":48683,"journal":{"name":"Structural Dynamics-Us","volume":null,"pages":null},"PeriodicalIF":2.8,"publicationDate":"2021-07-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://sci-hub-pdf.com/10.1063/4.0000099","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"39181541","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"物理与天体物理","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 1
Reproducibility of protein x-ray diffuse scattering and potential utility for modeling atomic displacement parameters. 蛋白质x射线扩散散射的再现性和原子位移参数建模的潜在效用。
IF 2.8 2区 物理与天体物理
Structural Dynamics-Us Pub Date : 2021-07-08 eCollection Date: 2021-07-01 DOI: 10.1063/4.0000087
Zhen Su, Medhanjali Dasgupta, Frédéric Poitevin, Irimpan I Mathews, Henry van den Bedem, Michael E Wall, Chun Hong Yoon, Mark A Wilson
{"title":"Reproducibility of protein x-ray diffuse scattering and potential utility for modeling atomic displacement parameters.","authors":"Zhen Su,&nbsp;Medhanjali Dasgupta,&nbsp;Frédéric Poitevin,&nbsp;Irimpan I Mathews,&nbsp;Henry van den Bedem,&nbsp;Michael E Wall,&nbsp;Chun Hong Yoon,&nbsp;Mark A Wilson","doi":"10.1063/4.0000087","DOIUrl":"https://doi.org/10.1063/4.0000087","url":null,"abstract":"<p><p>Protein structure and dynamics can be probed using x-ray crystallography. Whereas the Bragg peaks are only sensitive to the average unit-cell electron density, the signal between the Bragg peaks-diffuse scattering-is sensitive to spatial correlations in electron-density variations. Although diffuse scattering contains valuable information about protein dynamics, the diffuse signal is more difficult to isolate from the background compared to the Bragg signal, and the reproducibility of diffuse signal is not yet well understood. We present a systematic study of the reproducibility of diffuse scattering from isocyanide hydratase in three different protein forms. Both replicate diffuse datasets and datasets obtained from different mutants were similar in pairwise comparisons (Pearson correlation coefficient ≥0.8). The data were processed in a manner inspired by previously published methods using custom software with modular design, enabling us to perform an analysis of various data processing choices to determine how to obtain the highest quality data as assessed using unbiased measures of symmetry and reproducibility. The diffuse data were then used to characterize atomic mobility using a liquid-like motions (LLM) model. This characterization was able to discriminate between distinct anisotropic atomic displacement parameter (ADP) models arising from different anisotropic scaling choices that agreed comparably with the Bragg data. Our results emphasize the importance of data reproducibility as a model-free measure of diffuse data quality, illustrate the ability of LLM analysis of diffuse scattering to select among alternative ADP models, and offer insights into the design of successful diffuse scattering experiments.</p>","PeriodicalId":48683,"journal":{"name":"Structural Dynamics-Us","volume":null,"pages":null},"PeriodicalIF":2.8,"publicationDate":"2021-07-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://sci-hub-pdf.com/10.1063/4.0000087","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"39181543","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"物理与天体物理","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 4
Highly efficient soft x-ray spectrometer for transient absorption spectroscopy with broadband table-top high harmonic sources. 利用宽带台式高次谐波源进行瞬态吸收光谱分析的高效软 X 射线光谱仪。
IF 2.3 2区 物理与天体物理
Structural Dynamics-Us Pub Date : 2021-06-30 eCollection Date: 2021-05-01 DOI: 10.1063/4.0000096
Carlo Kleine, Maria Ekimova, Marc-Oliver Winghart, Sebastian Eckert, Oliver Reichel, Heike Löchel, Jürgen Probst, Christoph Braig, Christian Seifert, Alexei Erko, Andrey Sokolov, Marc J J Vrakking, Erik T J Nibbering, Arnaud Rouzée
{"title":"Highly efficient soft x-ray spectrometer for transient absorption spectroscopy with broadband table-top high harmonic sources.","authors":"Carlo Kleine, Maria Ekimova, Marc-Oliver Winghart, Sebastian Eckert, Oliver Reichel, Heike Löchel, Jürgen Probst, Christoph Braig, Christian Seifert, Alexei Erko, Andrey Sokolov, Marc J J Vrakking, Erik T J Nibbering, Arnaud Rouzée","doi":"10.1063/4.0000096","DOIUrl":"10.1063/4.0000096","url":null,"abstract":"<p><p>We present a novel soft x-ray spectrometer for ultrafast absorption spectroscopy utilizing table-top femtosecond high-order harmonic sources. Where most commercially available spectrometers rely on spherical variable line space gratings with a typical efficiency on the order of 3% in the first diffractive order, this spectrometer, based on a Hettrick-Underwood design, includes a reflective zone plate as a dispersive element. An improved efficiency of 12% at the N K-edge is achieved, accompanied by a resolving power of 890. The high performance of the soft x-ray spectrometer is further demonstrated by comparing nitrogen K-edge absorption spectra from calcium nitrate in aqueous solution obtained with our high-order harmonic source to previous measurements performed at the electron storage ring facility BESSY II.</p>","PeriodicalId":48683,"journal":{"name":"Structural Dynamics-Us","volume":null,"pages":null},"PeriodicalIF":2.3,"publicationDate":"2021-06-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC8249000/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"39163007","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"物理与天体物理","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Dependence of phase transition uniformity on crystal sizes characterized using birefringence. 相变均匀性对使用双折射表征的晶体尺寸的依赖性。
IF 2.8 2区 物理与天体物理
Structural Dynamics-Us Pub Date : 2021-06-30 eCollection Date: 2021-05-01 DOI: 10.1063/4.0000098
Saminathan Ramakrishnan, Jason R Stagno, Valentin Magidson, William F Heinz, Yun-Xing Wang
{"title":"Dependence of phase transition uniformity on crystal sizes characterized using birefringence.","authors":"Saminathan Ramakrishnan,&nbsp;Jason R Stagno,&nbsp;Valentin Magidson,&nbsp;William F Heinz,&nbsp;Yun-Xing Wang","doi":"10.1063/4.0000098","DOIUrl":"10.1063/4.0000098","url":null,"abstract":"<p><p>Solid-solid phase transitions (SSPTs) have been widely observed in crystals of organic or inorganic small-molecules. Although SSPTs in macromolecular crystals have been reported, the majority involve local atomic changes, such as those induced by changes in hydration. SSPTs driven by large conformational changes, however, can be more difficult to characterize since they often significantly disrupt lattice packing interactions. Such drastic changes make the cooperativity of molecular motion at the atomic level less easily achieved and more dependent on intrinsic properties of the crystal that define lattice order. Here, we investigate the effect of crystal size on the uniformity of SSPT in thin plate-like crystals of the adenine riboswitch aptamer RNA (riboA) by monitoring changes in crystal birefringence upon the diffusion of adenine ligand. The birefringence intensity is directly related to molecular order and the concurrent changes to polarizability of molecules that results from structural changes throughout the phase transition. The riboA crystals were loosely grouped into three categories (small, medium, and large) based on the surface area of the crystal plates. The time width of transition increased as a function of crystal size, ranging from ∼13 s for small crystals to ∼40 s for the largest crystal. Whereas the transitions in small crystals (<10 <i>μ</i>m<sup>2</sup>) were mostly uniform throughout, the medium and large crystals exhibited large variations in the time and width of the transition peak depending on the region of the crystal being analyzed. Our study provides insight into the spatiotemporal behavior of phase transitions in crystals of biological molecules and is of general interest to time-resolved crystallographic studies, where the kinetics of conformational changes may be governed by the kinetics of an associated SSPT.</p>","PeriodicalId":48683,"journal":{"name":"Structural Dynamics-Us","volume":null,"pages":null},"PeriodicalIF":2.8,"publicationDate":"2021-06-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://sci-hub-pdf.com/10.1063/4.0000098","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"39163006","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"物理与天体物理","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 1
Toward ultrafast magnetic depth profiling using time-resolved x-ray resonant magnetic reflectivity. 利用时间分辨 X 射线共振磁反射率实现超快磁深度剖析。
IF 2.8 2区 物理与天体物理
Structural Dynamics-Us Pub Date : 2021-06-23 eCollection Date: 2021-05-01 DOI: 10.1063/4.0000109
Valentin Chardonnet, Marcel Hennes, Romain Jarrier, Renaud Delaunay, Nicolas Jaouen, Marion Kuhlmann, Nagitha Ekanayake, Cyril Léveillé, Clemens von Korff Schmising, Daniel Schick, Kelvin Yao, Xuan Liu, Gheorghe S Chiuzbăian, Jan Lüning, Boris Vodungbo, Emmanuelle Jal
{"title":"Toward ultrafast magnetic depth profiling using time-resolved x-ray resonant magnetic reflectivity.","authors":"Valentin Chardonnet, Marcel Hennes, Romain Jarrier, Renaud Delaunay, Nicolas Jaouen, Marion Kuhlmann, Nagitha Ekanayake, Cyril Léveillé, Clemens von Korff Schmising, Daniel Schick, Kelvin Yao, Xuan Liu, Gheorghe S Chiuzbăian, Jan Lüning, Boris Vodungbo, Emmanuelle Jal","doi":"10.1063/4.0000109","DOIUrl":"10.1063/4.0000109","url":null,"abstract":"<p><p>During the last two decades, a variety of models have been developed to explain the ultrafast quenching of magnetization following femtosecond optical excitation. These models can be classified into two broad categories, relying either on a local or a non-local transfer of angular momentum. The acquisition of the magnetic depth profiles with femtosecond resolution, using time-resolved x-ray resonant magnetic reflectivity, can distinguish local and non-local effects. Here, we demonstrate the feasibility of this technique in a pump-probe geometry using a custom-built reflectometer at the FLASH2 free-electron laser (FEL). Although FLASH2 is limited to the production of photons with a fundamental wavelength of 4 nm ( <math><mrow><mo>≃</mo> <mn>310</mn> <mo> </mo> <mtext>eV</mtext></mrow> </math> ), we were able to probe close to the Fe <i>L</i> <sub>3</sub> edge ( <math><mrow><mn>706.8</mn> <mo> </mo> <mtext>eV</mtext></mrow> </math> ) of a magnetic thin film employing the third harmonic of the FEL. Our approach allows us to extract structural and magnetic asymmetry signals revealing two dynamics on different time scales which underpin a non-homogeneous loss of magnetization and a significant dilation of 2 Å of the layer thickness followed by oscillations. Future analysis of the data will pave the way to a full quantitative description of the transient magnetic depth profile combining femtosecond with nanometer resolution, which will provide further insight into the microscopic mechanisms underlying ultrafast demagnetization.</p>","PeriodicalId":48683,"journal":{"name":"Structural Dynamics-Us","volume":null,"pages":null},"PeriodicalIF":2.8,"publicationDate":"2021-06-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC8225393/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"39163008","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"物理与天体物理","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Ultrafast strain propagation and acoustic resonances in nanoscale bilayer systems. 纳米级双层体系中的超快应变传播和声共振。
IF 2.8 2区 物理与天体物理
Structural Dynamics-Us Pub Date : 2021-06-18 eCollection Date: 2021-05-01 DOI: 10.1063/4.0000079
N Bach, S Schäfer
{"title":"Ultrafast strain propagation and acoustic resonances in nanoscale bilayer systems.","authors":"N Bach, S Schäfer","doi":"10.1063/4.0000079","DOIUrl":"10.1063/4.0000079","url":null,"abstract":"<p><p>Ultrafast structural probing has greatly enhanced our understanding of the coupling of atomic motion to electronic and phononic degrees-of-freedom in quasi-bulk materials. In bi- and multilayer model systems, additionally, spatially inhomogeneous relaxation channels are accessible, often governed by pronounced interfacial couplings and local excitations in confined geometries. Here, we systematically explore the key dependencies of the low-frequency acoustic phonon spectrum in an elastically mismatched metal/semiconductor bilayer system optically excited by femtosecond laser pulses. We track the spatiotemporal strain wave propagation in the heterostructure employing a discrete numerical linear chain simulation and access acoustic wave reflections and interfacial couplings with a phonon mode description based on a continuum mechanics model. Due to the interplay of elastic properties and mass densities of the two materials, acoustic resonance frequencies of the heterostructure significantly differ from breathing modes in monolayer films. For large acoustic mismatch, the spatial localization of phonon eigenmodes is derived from analytical approximations and can be interpreted as harmonic oscillations in decoupled mechanical resonators.</p>","PeriodicalId":48683,"journal":{"name":"Structural Dynamics-Us","volume":null,"pages":null},"PeriodicalIF":2.8,"publicationDate":"2021-06-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC8214470/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"39025628","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"物理与天体物理","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
A novel free-electron laser single-pulse Wollaston polarimeter for magneto-dynamical studies. 用于磁动力学研究的新型自由电子激光单脉冲沃拉斯顿偏振计。
IF 2.8 2区 物理与天体物理
Structural Dynamics-Us Pub Date : 2021-06-18 eCollection Date: 2021-05-01 DOI: 10.1063/4.0000104
Antonio Caretta, Simone Laterza, Valentina Bonanni, Rudi Sergo, Carlo Dri, Giuseppe Cautero, Fabio Galassi, Matteo Zamolo, Alberto Simoncig, Marco Zangrando, Alessandro Gessini, Simone Dal Zilio, Roberto Flammini, Paolo Moras, Alexander Demidovich, Miltcho Danailov, Fulvio Parmigiani, Marco Malvestuto
{"title":"A novel free-electron laser single-pulse Wollaston polarimeter for magneto-dynamical studies.","authors":"Antonio Caretta,&nbsp;Simone Laterza,&nbsp;Valentina Bonanni,&nbsp;Rudi Sergo,&nbsp;Carlo Dri,&nbsp;Giuseppe Cautero,&nbsp;Fabio Galassi,&nbsp;Matteo Zamolo,&nbsp;Alberto Simoncig,&nbsp;Marco Zangrando,&nbsp;Alessandro Gessini,&nbsp;Simone Dal Zilio,&nbsp;Roberto Flammini,&nbsp;Paolo Moras,&nbsp;Alexander Demidovich,&nbsp;Miltcho Danailov,&nbsp;Fulvio Parmigiani,&nbsp;Marco Malvestuto","doi":"10.1063/4.0000104","DOIUrl":"https://doi.org/10.1063/4.0000104","url":null,"abstract":"<p><p>Here, we report on the conceptual design, the hardware realization, and the first experimental results of a novel and compact x-ray polarimeter capable of a single-pulse linear polarization angle detection in the extreme ultraviolet photon energy range. The polarimeter is tested by performing time resolved pump-probe experiments on a Ni<sub>80</sub>Fe<sub>20</sub> Permalloy film at the M<sub>2,3</sub> Ni edge at an externally seeded free-electron laser source. Comparison with similar experiments reported in the literature shows the advantages of our approach also in view of future experiments.</p>","PeriodicalId":48683,"journal":{"name":"Structural Dynamics-Us","volume":null,"pages":null},"PeriodicalIF":2.8,"publicationDate":"2021-06-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://sci-hub-pdf.com/10.1063/4.0000104","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"39025629","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"物理与天体物理","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 2
Ultrafast strong-field dissociation of vinyl bromide: An attosecond transient absorption spectroscopy and non-adiabatic molecular dynamics study. 乙烯基溴的超快强场解离:阿秒瞬态吸收光谱和非绝热分子动力学研究。
IF 2.8 2区 物理与天体物理
Structural Dynamics-Us Pub Date : 2021-06-15 eCollection Date: 2021-05-01 DOI: 10.1063/4.0000102
Florian Rott, Maurizio Reduzzi, Thomas Schnappinger, Yuki Kobayashi, Kristina F Chang, Henry Timmers, Daniel M Neumark, Regina de Vivie-Riedle, Stephen R Leone
{"title":"Ultrafast strong-field dissociation of vinyl bromide: An attosecond transient absorption spectroscopy and non-adiabatic molecular dynamics study.","authors":"Florian Rott,&nbsp;Maurizio Reduzzi,&nbsp;Thomas Schnappinger,&nbsp;Yuki Kobayashi,&nbsp;Kristina F Chang,&nbsp;Henry Timmers,&nbsp;Daniel M Neumark,&nbsp;Regina de Vivie-Riedle,&nbsp;Stephen R Leone","doi":"10.1063/4.0000102","DOIUrl":"https://doi.org/10.1063/4.0000102","url":null,"abstract":"<p><p>Attosecond extreme ultraviolet (XUV) and soft x-ray sources provide powerful new tools for studying ultrafast molecular dynamics with atomic, state, and charge specificity. In this report, we employ attosecond transient absorption spectroscopy (ATAS) to follow strong-field-initiated dynamics in vinyl bromide. Probing the Br M edge allows one to assess the competing processes in neutral and ionized molecular species. Using <i>ab initio</i> non-adiabatic molecular dynamics, we simulate the neutral and cationic dynamics resulting from the interaction of the molecule with the strong field. Based on the dynamics results, the corresponding time-dependent XUV transient absorption spectra are calculated by applying high-level multi-reference methods. The state-resolved analysis obtained through the simulated dynamics and related spectral contributions enables a detailed and quantitative comparison with the experimental data. The main outcome of the interaction with the strong field is unambiguously the population of the first three cationic states, <i>D</i> <sub>1</sub>, <i>D</i> <sub>2</sub>, and <i>D</i> <sub>3</sub>. The first two show exclusively vibrational dynamics while the <i>D</i> <sub>3</sub> state is characterized by an ultrafast dissociation of the molecule via C-Br bond rupture within 100 fs in 50% of the analyzed trajectories. The combination of the three simulated ionic transient absorption spectra is in excellent agreement with the experimental results. This work establishes ATAS in combination with high-level multi-reference simulations as a spectroscopic technique capable of resolving coupled non-adiabatic electronic-nuclear dynamics in photoexcited molecules with sub-femtosecond resolution.</p>","PeriodicalId":48683,"journal":{"name":"Structural Dynamics-Us","volume":null,"pages":null},"PeriodicalIF":2.8,"publicationDate":"2021-06-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://sci-hub-pdf.com/10.1063/4.0000102","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"39025627","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"物理与天体物理","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 4
Design and characterization of a magnetic bottle electron spectrometer for time-resolved extreme UV and X-ray photoemission spectroscopy of liquid microjets. 用于液体微射流时间分辨极紫外和x射线光发射光谱的磁瓶电子能谱仪的设计与表征。
IF 2.8 2区 物理与天体物理
Structural Dynamics-Us Pub Date : 2021-06-09 eCollection Date: 2021-05-01 DOI: 10.1063/4.0000107
Naoya Kurahashi, Stephan Thürmer, Suet Yi Liu, Yo-Ichi Yamamoto, Shutaro Karashima, Atanu Bhattacharya, Yoshihiro Ogi, Takuya Horio, Toshinori Suzuki
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引用次数: 9
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