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基于散斑技术的同步辐射X射线光子关联谱是研究材料介观尺度动态过程的重要方法,但实验中的光源特性、光束传输及探测器响应等因素对散斑动力学信号的影响机制复杂,难以对其中的影响因素进行单独且直接的观测。为此,本研究旨在通过蒙特卡洛模拟开展全光路数值建模,系统解析各因素的影响,为实验设计与优化提供理论支撑。研究构建了包含布朗粒子动力学、光束相干性及探测器响应的三维仿真框架,模拟从光子发射到信号采集的全流程。基于夫琅禾费衍射理论,开发散斑光场生成算法,通过原子位置动态演化与相位调制,复现实验散斑涨落特性,并通过Siegert关系拟合、散射矢量区域选择及粒子运动步长与温度关系验证了模拟程序的可行性。关键参数灵敏度分析表明,光阑孔径与光束束腰存在最优匹配条件r/σ=1,此时相干性与光子通量达到平衡;机械振动振幅达到运动步长1500倍时,关联函数出现周期性振荡,导致动力学参数提取失真;低光强条件下泊松噪声与光强波动显著降低信噪比。研究建立的全光路模拟框架,揭示了光源特性、光学元件参数及噪声因素对实验结果的影响机制,为XPCS实验参数优化提供了理论依据,明确了噪声抑制与动力学解析的协同机制,为该技术在更多实验场景的应用奠定了模拟基础。X-ray Photon Correlation Spectroscopy (XPCS) is vital for probing mesoscale material dynamics using synchrotron radiation, yet the complex influence of parameters such as light source properties, beam propagation, detector response on speckle dynamics is hard to directly observe. This study develops a Monte Carlo-based full optical path numerical model to systematically analyze these effects, aiding experimental optimization.
A simulation framework integrating Brownian dynamics, beam coherence, and detector response was constructed to replicate the entire photon emission-to-detection process. A Fraunhofer diffraction-based speckle generation algorithm reproduced speckle fluctuations via atomic position evolution and phase modulation. Feasibility was validated via Siegert relation fitting (β, γ), Γ - q2 linearity (R2=0.99904), and consistency with the Einstein-Stokes law.
Key parameter sensitivity analysis revealed:(1) Optimal aperture matching (r/σ=1) balances coherence and photon flux; (2) Mechanical vibrations with Δx/s=1500 induce periodic oscillations in g2(q, τ), masking intrinsic relaxation, as validated by a 24.658 Hz pump experiment; (3) Poisson noise and intensity fluctuations degrade low-light SNR, with Poisson noise causing discrete errors and classical noise inducing baseline shifts.
This framework clarifies how source properties, optical parameters, and noise affect results, providing guidance for XPCS optimization and a foundation for extending its applications to high-precision coherent scattering scenarios.-
Keywords:
- X-ray Photon Correlation Spectroscopy /
- Monte Carlo simulation /
- speckle dynamics /
- full optical path simulation
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[1] Martinelli A, Baldi G, Dallari F, Rufflé B, Zontone F, Monaco G 2020 Philos. Mag. 1002636
[2] Zhong W, Liu F, Wang C 2021 J. Phys. Condens. Matter 33313001
[3] Jo W, Stern S, Westermeier F, Rysov R, Riepp M, Schmehr J, Lange J, Becker J, Sprung M, Laurus T, Graafsma H, Lokteva I, Gruebel G, Roseker W 2023 Opt. Express 313315
[4] Sandy A R, Zhang Q, Lurio L B 2018 Annu. Rev. Mater. Res. 48167
[5] Sutton M, Lhermitte J R, Ehrburger-Dolle F, Livet F 2021 Phys. Rev. Res. 3013119
[6] Mohanty S, Cooper C B, Wang H, Liang M, Cai W 2022 Modell. Simul. Mater. Sci. Eng. 30075004
[7] Rudd R E, Briggs G, Sutton A, Medeiros-Ribeiro G, Williams R S 2003 Phys. Rev. Lett. 90146101
[8] Miao J, Charalambous P, Kirz J, Sayre D 1999 Nature 400342
[9] Tessarini S 2022 Monte Carlo simulation of phase sensitive X-ray imaging. Ph.D. Dissertation, ETH Zurich
[10] Sheyfer D, Zhang Q, Lal J, Loeffler T, Dufresne E M, Sandy A R, Narayanan S, Sankaranarayanan S K R S, Szczygiel R, Maj P, Soderholm L, Antonio M R, Stephenson G B 2020 Phys. Rev. Lett. 125125504
[11] Sheyfer D, Zheng H, Krogstad M, Thompson C, You H, Eastman J A, Liu Y, Wang B X, Ye Z G, Rosenkranz S, Phelan D, Dufresne E M, Stephenson G B, Cao Y 2024 J. Synchrotron Radiat. 3155
[12] Chen Y, Han W, Bin G, Wu S, Morgan S P, Sun S 2024 Sci. Rep. 1427665
[13] Hu Z, Donatelli J J 2024 Phys. Rev. B 110214305
[14] Semeraro E F, Möller J, Narayanan T 2018 J. Appl. Crystallogr. 51706
[15] Narayanan T, Sztucki M, Van Vaerenbergh P, Léonardon J, Gorini J, Claustre L, Sever F, Morse J, Boesecke P 2018 J. Appl. Crystallogr. 511511
[16] Andrews R N, Narayanan S, Zhang F, Kuzmenko I, Ilavsky J 2018 J. Appl. Crystallogr. 5135
[17] Lehmkühler F, Dallari F, Jain A, Sikorski M, Moller J, Frenzel L, Lokteva I, Mills G, Walther M, Sinn H, Schulz F, Dartsch M, Markmann V, Bean R, Kim Y, Vagovic P, Madsen A, Mancuso A P, Grubel G 2020 Proc. Natl. Acad. Sci. U.S.A. 11724110
[18] Berne B J, Pecora R 2000 Dynamic light scattering:with applications to chemistry, biology, and physics (Courier Corporation)
[19] Patterson G D, Lindsey C P 1981 Macromolecules 1483
[20] Khan F, Narayanan S, Sersted R, Schwarz N, Sandy A 2018 J. Synchrotron Radiat. 251135
[21] Arango M T, Zhang Y, Zhao C, Li R, Doerk G, Nykypanchuk D, Chen-Wiegart Y C K, Fluerasu A, Wiegart L 2020 Mater. Today Phys. 14100220
[22] Ruta B, Evenson Z, Hechler S, Stolpe M, Pineda E, Gallino I, Busch R 2015 Phys. Rev. Lett. 115175701
[23] Katzav E, Schwartz M 2004 Phys. Rev. E 69052603
[24] Einstein A 1905 Ann. Phys. 322549
[25] Duhr S, Braun D 2006 Phys. Rev. Lett. 96168301
[26] Zhou Z, Zhang M, Cui C, Wei L, Li S, Guo Z, Xu Y, Tian F, Li X, Jiang H, Tai R 2025 Phys. Scr. 100075115
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