利用时间分辨多晶衍射数据的全局拟合方法提取铂中的超快晶格动力学和电子-声子耦合。

IF 2.3 2区 物理与天体物理 Q3 CHEMISTRY, PHYSICAL Structural Dynamics-Us Pub Date : 2021-11-15 eCollection Date: 2021-11-01 DOI:10.1063/4.0000120
Daniela Zahn, Hélène Seiler, Yoav William Windsor, Ralph Ernstorfer
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引用次数: 0

摘要

电子-声子耦合的定量知识对于许多应用以及非平衡弛豫过程的基本理解都非常重要。时间分辨衍射法对激光诱导的晶格动力学非常敏感,因此可以直接获取这方面的知识。在此,我们介绍一种分析时间分辨多晶衍射数据的方法。该方法采用两步程序,最大限度地减少随时间变化的拟合参数数量。提取晶格动态的方法是找到与整个瞬态衍射图样的最佳拟合,而不是分析单个德拜-舍勒环的瞬态变化。铂是新型光催化和自旋电子应用的重要组成部分,其电子-声子耦合参数 G ep 的文献值存在很大差异。根据提取的原子均方位移演化并使用双温模型,我们得到了 G ep = ( 3.9 ± 0.2 ) × 10 17 W m 3 K(统计误差)。我们发现,至少在吸收能量密度达到 124 J/cm3 时,G ep 并不依赖于通量。我们对铂晶格动力学的研究结果提供了对电子-声子耦合和声子热化的见解,并为非平衡条件下铂基异质结构的定量描述奠定了基础。
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Ultrafast lattice dynamics and electron-phonon coupling in platinum extracted with a global fitting approach for time-resolved polycrystalline diffraction data.

Quantitative knowledge of electron-phonon coupling is important for many applications as well as for the fundamental understanding of nonequilibrium relaxation processes. Time-resolved diffraction provides direct access to this knowledge through its sensitivity to laser-induced lattice dynamics. Here, we present an approach for analyzing time-resolved polycrystalline diffraction data. A two-step routine is used to minimize the number of time-dependent fit parameters. The lattice dynamics are extracted by finding the best fit to the full transient diffraction pattern rather than by analyzing transient changes of individual Debye-Scherrer rings. We apply this approach to platinum, an important component of novel photocatalytic and spintronic applications, for which a large variation of literature values exists for the electron-phonon coupling parameter G ep . Based on the extracted evolution of the atomic mean squared displacement and using a two-temperature model, we obtain G ep = ( 3.9 ± 0.2 ) × 10 17 W m 3 K (statistical error). We find that at least up to an absorbed energy density of 124 J/cm3, G ep is not fluence-dependent. Our results for the lattice dynamics of platinum provide insights into electron-phonon coupling and phonon thermalization and constitute a basis for quantitative descriptions of platinum-based heterostructures in nonequilibrium conditions.

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来源期刊
Structural Dynamics-Us
Structural Dynamics-Us CHEMISTRY, PHYSICALPHYSICS, ATOMIC, MOLECU-PHYSICS, ATOMIC, MOLECULAR & CHEMICAL
CiteScore
5.50
自引率
3.60%
发文量
24
审稿时长
16 weeks
期刊介绍: Structural Dynamics focuses on the recent developments in experimental and theoretical methods and techniques that allow a visualization of the electronic and geometric structural changes in real time of chemical, biological, and condensed-matter systems. The community of scientists and engineers working on structural dynamics in such diverse systems often use similar instrumentation and methods. The journal welcomes articles dealing with fundamental problems of electronic and structural dynamics that are tackled by new methods, such as: Time-resolved X-ray and electron diffraction and scattering, Coherent diffractive imaging, Time-resolved X-ray spectroscopies (absorption, emission, resonant inelastic scattering, etc.), Time-resolved electron energy loss spectroscopy (EELS) and electron microscopy, Time-resolved photoelectron spectroscopies (UPS, XPS, ARPES, etc.), Multidimensional spectroscopies in the infrared, the visible and the ultraviolet, Nonlinear spectroscopies in the VUV, the soft and the hard X-ray domains, Theory and computational methods and algorithms for the analysis and description of structuraldynamics and their associated experimental signals. These new methods are enabled by new instrumentation, such as: X-ray free electron lasers, which provide flux, coherence, and time resolution, New sources of ultrashort electron pulses, New sources of ultrashort vacuum ultraviolet (VUV) to hard X-ray pulses, such as high-harmonic generation (HHG) sources or plasma-based sources, New sources of ultrashort infrared and terahertz (THz) radiation, New detectors for X-rays and electrons, New sample handling and delivery schemes, New computational capabilities.
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