Structural Dynamics-Us最新文献_第5页

Photodiode-based time zero determination for ultrafast electron microscopy. 用于超快电子显微镜的基于光电二极管的时间零点测定。

IF 2.8 2区物理与天体物理

Structural Dynamics-Us Pub Date : 2023-11-06 eCollection Date: 2023-11-01 DOI: 10.1063/4.0000218

S T Kempers, S Borrelli, E R Kieft, H A van Doorn, P H A Mutsaers, O J Luiten

引用次数: 0

A Δ-learning strategy for interpretation of spectroscopic observables. 用于解释光谱可观察性的Δ-学习策略。

IF 2.8 2区物理与天体物理

Structural Dynamics-Us Pub Date : 2023-11-06 eCollection Date: 2023-11-01 DOI: 10.1063/4.0000215

Luke Watson, Thomas Pope, Raphael M Jay, Ambar Banerjee, Philippe Wernet, Thomas J Penfold

{"title":"A Δ-learning strategy for interpretation of spectroscopic observables.","authors":"Luke Watson, Thomas Pope, Raphael M Jay, Ambar Banerjee, Philippe Wernet, Thomas J Penfold","doi":"10.1063/4.0000215","DOIUrl":"10.1063/4.0000215","url":null,"abstract":"Accurate computations of experimental observables are essential for interpreting the high information content held within x-ray spectra. However, for complicated systems this can be difficult, a challenge compounded when dynamics becomes important owing to the large number of calculations required to capture the time-evolving observable. While machine learning architectures have been shown to represent a promising approach for rapidly predicting spectral lineshapes, achieving simultaneously accurate and sufficiently comprehensive training data is challenging. Herein, we introduce Δ-learning for x-ray spectroscopy. Instead of directly learning the structure-spectrum relationship, the Δ-model learns the structure dependent difference between a higher and lower level of theory. Consequently, once developed these models can be used to translate spectral shapes obtained from lower levels of theory to mimic those corresponding to higher levels of theory. Ultimately, this achieves accurate simulations with a much reduced computational burden as only the lower level of theory is computed, while the model can instantaneously transform this to a spectrum equivalent to a higher level of theory. Our present model, demonstrated herein, learns the difference between TDDFT(BLYP) and TDDFT(B3LYP) spectra. Its effectiveness is illustrated using simulations of Rh L3-edge spectra tracking the C-H activation of octane by a cyclopentadienyl rhodium carbonyl complex.","PeriodicalId":48683,"journal":{"name":"Structural Dynamics-Us","volume":"10 6","pages":"064101"},"PeriodicalIF":2.8,"publicationDate":"2023-11-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC10629969/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"71522979","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

Disentangling the evolution of electrons and holes in photoexcited ZnO nanoparticles. 解开光激发ZnO纳米颗粒中电子和空穴的演化。

IF 2.3 2区物理与天体物理

Structural Dynamics-Us Pub Date : 2023-11-03 eCollection Date: 2023-11-01 DOI: 10.1063/4.0000204

Christopher J Milne, Natalia Nagornova, Thomas Pope, Hui-Yuan Chen, Thomas Rossi, Jakub Szlachetko, Wojciech Gawelda, Alexander Britz, Tim B van Driel, Leonardo Sala, Simon Ebner, Tetsuo Katayama, Stephen H Southworth, Gilles Doumy, Anne Marie March, C Stefan Lehmann, Melanie Mucke, Denys Iablonskyi, Yoshiaki Kumagai, Gregor Knopp, Koji Motomura, Tadashi Togashi, Shigeki Owada, Makina Yabashi, Martin M Nielsen, Marek Pajek, Kiyoshi Ueda, Rafael Abela, Thomas J Penfold, Majed Chergui

{"title":"Disentangling the evolution of electrons and holes in photoexcited ZnO nanoparticles.","authors":"Christopher J Milne, Natalia Nagornova, Thomas Pope, Hui-Yuan Chen, Thomas Rossi, Jakub Szlachetko, Wojciech Gawelda, Alexander Britz, Tim B van Driel, Leonardo Sala, Simon Ebner, Tetsuo Katayama, Stephen H Southworth, Gilles Doumy, Anne Marie March, C Stefan Lehmann, Melanie Mucke, Denys Iablonskyi, Yoshiaki Kumagai, Gregor Knopp, Koji Motomura, Tadashi Togashi, Shigeki Owada, Makina Yabashi, Martin M Nielsen, Marek Pajek, Kiyoshi Ueda, Rafael Abela, Thomas J Penfold, Majed Chergui","doi":"10.1063/4.0000204","DOIUrl":"10.1063/4.0000204","url":null,"abstract":"The evolution of charge carriers in photoexcited room temperature ZnO nanoparticles in solution is investigated using ultrafast ultraviolet photoluminescence spectroscopy, ultrafast Zn K-edge absorption spectroscopy, and ab initio molecular dynamics (MD) simulations. The photoluminescence is excited at 4.66 eV, well above the band edge, and shows that electron cooling in the conduction band and exciton formation occur in <500 fs, in excellent agreement with theoretical predictions. The x-ray absorption measurements, obtained upon excitation close to the band edge at 3.49 eV, are sensitive to the migration and trapping of holes. They reveal that the 2 ps transient largely reproduces the previously reported transient obtained at 100 ps time delay in synchrotron studies. In addition, the x-ray absorption signal is found to rise in ∼1.4 ps, which we attribute to the diffusion of holes through the lattice prior to their trapping at singly charged oxygen vacancies. Indeed, the MD simulations show that impulsive trapping of holes induces an ultrafast expansion of the cage of Zn atoms in <200 fs, followed by an oscillatory response at a frequency of ∼100 cm-1, which corresponds to a phonon mode of the system involving the Zn sub-lattice.","PeriodicalId":48683,"journal":{"name":"Structural Dynamics-Us","volume":"10 6","pages":"064501"},"PeriodicalIF":2.3,"publicationDate":"2023-11-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC10628992/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"71522980","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

Non-thermal structural transformation of diamond driven by x-rays. x射线驱动下金刚石的非热结构转变。

IF 2.8 2区物理与天体物理

Structural Dynamics-Us Pub Date : 2023-10-27 eCollection Date: 2023-09-01 DOI: 10.1063/4.0000193

Philip Heimann, Nicholas J Hartley, Ichiro Inoue, Victor Tkachenko, Andre Antoine, Fabien Dorchies, Roger Falcone, Jérôme Gaudin, Hauke Höppner, Yuichi Inubushi, Konrad J Kapcia, Hae Ja Lee, Vladimir Lipp, Paloma Martinez, Nikita Medvedev, Franz Tavella, Sven Toleikis, Makina Yabashi, Toshinori Yabuuchi, Jumpei Yamada, Beata Ziaja

{"title":"Non-thermal structural transformation of diamond driven by x-rays.","authors":"Philip Heimann, Nicholas J Hartley, Ichiro Inoue, Victor Tkachenko, Andre Antoine, Fabien Dorchies, Roger Falcone, Jérôme Gaudin, Hauke Höppner, Yuichi Inubushi, Konrad J Kapcia, Hae Ja Lee, Vladimir Lipp, Paloma Martinez, Nikita Medvedev, Franz Tavella, Sven Toleikis, Makina Yabashi, Toshinori Yabuuchi, Jumpei Yamada, Beata Ziaja","doi":"10.1063/4.0000193","DOIUrl":"https://doi.org/10.1063/4.0000193","url":null,"abstract":"Intense x-ray pulses can cause the non-thermal structural transformation of diamond. At the SACLA XFEL facility, pump x-ray pulses triggered this phase transition, and probe x-ray pulses produced diffraction patterns. Time delays were observed from 0 to 250 fs, and the x-ray dose varied from 0.9 to 8.0 eV/atom. The intensity of the (111), (220), and (311) diffraction peaks decreased with time, indicating a disordering of the crystal lattice. From a Debye-Waller analysis, the rms atomic displacements perpendicular to the (111) planes were observed to be significantly larger than those perpendicular to the (220) or (311) planes. At a long time delay of 33 ms, graphite (002) diffraction indicates that graphitization did occur above a threshold dose of 1.2 eV/atom. These experimental results are in qualitative agreement with XTANT+ simulations using a hybrid model based on density-functional tight-binding molecular dynamics.","PeriodicalId":48683,"journal":{"name":"Structural Dynamics-Us","volume":"10 5","pages":"054502"},"PeriodicalIF":2.8,"publicationDate":"2023-10-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC10613085/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"71414817","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

Solution phase high repetition rate laser pump x-ray probe picosecond hard x-ray spectroscopy at the Stanford Synchrotron Radiation Lightsource. 斯坦福同步辐射光源的溶液相高重复率激光泵浦x射线探针皮秒硬x射线光谱。

IF 2.8 2区物理与天体物理

Structural Dynamics-Us Pub Date : 2023-10-27 eCollection Date: 2023-09-01 DOI: 10.1063/4.0000207

Marco Reinhard, Dean Skoien, Jacob A Spies, Angel T Garcia-Esparza, Benjamin D Matson, Jeff Corbett, Kai Tian, James Safranek, Eduardo Granados, Matthew Strader, Kelly J Gaffney, Roberto Alonso-Mori, Thomas Kroll, Dimosthenis Sokaras

{"title":"Solution phase high repetition rate laser pump x-ray probe picosecond hard x-ray spectroscopy at the Stanford Synchrotron Radiation Lightsource.","authors":"Marco Reinhard, Dean Skoien, Jacob A Spies, Angel T Garcia-Esparza, Benjamin D Matson, Jeff Corbett, Kai Tian, James Safranek, Eduardo Granados, Matthew Strader, Kelly J Gaffney, Roberto Alonso-Mori, Thomas Kroll, Dimosthenis Sokaras","doi":"10.1063/4.0000207","DOIUrl":"10.1063/4.0000207","url":null,"abstract":"We present a dedicated end-station for solution phase high repetition rate (MHz) picosecond hard x-ray spectroscopy at beamline 15-2 of the Stanford Synchrotron Radiation Lightsource. A high-power ultrafast ytterbium-doped fiber laser is used to photoexcite the samples at a repetition rate of 640 kHz, while the data acquisition operates at the 1.28 MHz repetition rate of the storage ring recording data in an alternating on-off mode. The time-resolved x-ray measurements are enabled via gating the x-ray detectors with the 20 mA/70 ps camshaft bunch of SPEAR3, a mode available during the routine operations of the Stanford Synchrotron Radiation Lightsource. As a benchmark study, aiming to demonstrate the advantageous capabilities of this end-station, we have conducted picosecond Fe K-edge x-ray absorption spectroscopy on aqueous [FeII(phen)3]2+, a prototypical spin crossover complex that undergoes light-induced excited spin state trapping forming an electronic excited state with a 0.6-0.7 ns lifetime. In addition, we report transient Fe Kβ main line and valence-to-core x-ray emission spectra, showing a unique detection sensitivity and an excellent agreement with model spectra and density functional theory calculations, respectively. Notably, the achieved signal-to-noise ratio, the overall performance, and the routine availability of the developed end-station have enabled a systematic time-resolved science program using the monochromatic beam at the Stanford Synchrotron Radiation Lightsource.","PeriodicalId":48683,"journal":{"name":"Structural Dynamics-Us","volume":"10 5","pages":"054304"},"PeriodicalIF":2.8,"publicationDate":"2023-10-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC10613086/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"71414818","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

Tailored nanophononic wavefield in a patterned bilayer system probed by ultrafast convergent beam electron diffraction 用超快会聚束电子衍射探测双层系统中的定制纳米声子波场

IF 2.8 2区物理与天体物理

Structural Dynamics-Us Pub Date : 2022-05-01 DOI: 10.1063/4.0000144

N. Bach, A. Feist, M. Möller, C. Ropers, S. Schäfer

引用次数: 1

Temperature measurements of liquid flat jets in vacuum 真空中液体平面射流的温度测量

IF 2.8 2区物理与天体物理

Structural Dynamics-Us Pub Date : 2021-12-10 DOI: 10.1063/4.0000139

Yi-Ping Chang, Z. Yin, T. Balciunas, H. Wörner, J. Wolf

引用次数: 7

Free Vibration of Single Degree of Freedom System 单自由度系统的自由振动

IF 2.8 2区物理与天体物理

Structural Dynamics-Us Pub Date : 2021-01-01 DOI: 10.1007/978-3-030-69674-0_2

M. Mukhopadhyay

引用次数: 0

Ultrafast coherent exciton dynamics in size-controlled perylene bisimide aggregates 尺寸控制的苝-双酰亚胺聚集体中的超快相干激子动力学

IF 2.8 2区物理与天体物理

Structural Dynamics-Us Pub Date : 2019-11-01 DOI: 10.1063/1.5124148

Seongsoo Kang, Christina Kaufmann, Yongseok Hong, Woojae Kim, Agnieszka Nowak‐Król, F. Würthner, Dongho Kim

{"title":"Ultrafast coherent exciton dynamics in size-controlled perylene bisimide aggregates","authors":"Seongsoo Kang, Christina Kaufmann, Yongseok Hong, Woojae Kim, Agnieszka Nowak‐Król, F. Würthner, Dongho Kim","doi":"10.1063/1.5124148","DOIUrl":"https://doi.org/10.1063/1.5124148","url":null,"abstract":"For H-aggregates of perylene bisimide (PBI), it has been reported that upon photoexcitation, an initially delocalized Frenkel exciton is localized by excimer formation. However, in recent studies, the beforehand exciton dynamics preceding the excimer formation was suggested in larger aggregates consisting of at least more than 10-PBI subunits, which was not observed in small aggregates comprising less than four-PBI subunits. This feature implies that the size of molecular aggregates plays a crucial role in the initial exciton dynamics. In this regard, we have tried to unveil the initial exciton dynamics in PBI H-aggregates by tracking down the transient reorientations of electronic transition dipoles formed by interactions between the PBI subunits in systematically size-controlled PBI H-aggregates. The ultrafast coherent exciton dynamics depending on the molecular aggregate sizes can be distinguished using polarization-dependent femtosecond-transient absorption anisotropy spectroscopic measurements with a time resolution of ∼40 fs. The ultrafast decay profiles of the anisotropy values are unaffected by vibrational relaxation and rotational diffusion processes; hence, the coherent exciton dynamics of the PBI H-aggregates prior to the excimer formation can be directly revealed as the energy migration processes along the PBI H-aggregates.","PeriodicalId":48683,"journal":{"name":"Structural Dynamics-Us","volume":" ","pages":""},"PeriodicalIF":2.8,"publicationDate":"2019-11-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://sci-hub-pdf.com/10.1063/1.5124148","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"48381977","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"物理与天体物理","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 8

Decelerated lattice excitation and absence of bulk phonon modes at surfaces: Ultra-fast electron diffraction from Bi(111) surface upon fs-laser excitation 减速晶格激发和表面不存在体声子模式：fs激光激发下Bi（111）表面的超快电子衍射

IF 2.8 2区物理与天体物理

Structural Dynamics-Us Pub Date : 2019-11-01 DOI: 10.1063/1.5128275

V. Tinnemann, C. Streubühr, B. Hafke, T. Witte, A. Kalus, A. Hanisch-Blicharski, M. Ligges, P. Zhou, D. von der Linde, U. Bovensiepen, M. Horn-von Hoegen

引用次数: 2