利用 X 射线瞬态吸收光谱同时测量碳 K- 和氯 L2,3- 边缘的相干振动动力学

IF 5.4 1区 物理与天体物理 Q1 PHYSICS, MULTIDISCIPLINARY Communications Physics Pub Date : 2024-09-13 DOI:10.1038/s42005-024-01794-4
Andrew D. Ross, Diptarka Hait, Valeriu Scutelnic, Daniel M. Neumark, Martin Head-Gordon, Stephen R. Leone
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引用次数: 0

摘要

X 射线瞬态吸收光谱(XTAS)是超快分子动力学的强大探针。XTAS 信号的演变受相关核心激发态势能面形状的控制,而这些势能面形状很难直接测量。在这里,我们利用针对 C 1s 和 Cl 2p 电子的 XTAS 研究了拉曼激活的 CCl4 的振动动力学。完全对称的伸展模式会导致键长的协同伸长或收缩,这反过来又会引起与内壳电子激发到价反键水平相关的 X 射线吸收能量发生可测量的红移或蓝移。由此提取的不同核激发势能面(CEPES)斜率之间的比率与限制性开壳 Kohn-Sham 计算结果非常吻合。其他不对称模式对 XTAS 信号的贡献并不明显。这些结果突显了 XTAS 揭示涉及 0.01 Å 原子位移的相干核动力学的能力,同时也提供了对 CEPES 受力的直接测量。在超快分子动力学研究中,X 射线瞬态吸收信号的演变受相关核激发态势能面形状的控制。作者利用实验和理论测量了从 C 1s 和 Cl 2p 壳激发到 CCl4 中价反键轨道的势能面斜率。
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Measurement of coherent vibrational dynamics with X-ray Transient Absorption Spectroscopy simultaneously at the Carbon K- and Chlorine L2,3- edges
X-ray Transient Absorption Spectroscopy (XTAS) is a powerful probe for ultrafast molecular dynamics. The evolution of XTAS signal is controlled by the shapes of potential energy surfaces of the associated core-excited states, which are difficult to directly measure. Here, we study the vibrational dynamics of Raman activated CCl4 with XTAS targeting the C 1s and Cl 2p electrons. The totally symmetric stretching mode leads to concerted elongation or contraction in bond lengths, which in turn induce an experimentally measurable red or blue shift in the X-ray absorption energies associated with inner-shell electron excitations to the valence antibonding levels. The ratios between slopes of different core-excited potential energy surfaces (CEPESs) thereby extracted agree very well with Restricted Open-Shell Kohn-Sham calculations. The other, asymmetric, modes do not measurably contribute to the XTAS signal. The results highlight the ability of XTAS to reveal coherent nuclear dynamics involving  < 0.01 Å atomic displacements and also provide direct measurement of forces on CEPESs. The evolution of X-ray transient absorption signal in studies of ultrafast molecular dynamics is controlled by the shapes of potential energy surfaces of the associated core-excited states. The authors use experiment and theory to measure the slopes of potential energy surfaces for excitations out of the C 1s and Cl 2p shells to valence antibonding orbitals in CCl4
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来源期刊
Communications Physics
Communications Physics Physics and Astronomy-General Physics and Astronomy
CiteScore
8.40
自引率
3.60%
发文量
276
审稿时长
13 weeks
期刊介绍: Communications Physics is an open access journal from Nature Research publishing high-quality research, reviews and commentary in all areas of the physical sciences. Research papers published by the journal represent significant advances bringing new insight to a specialized area of research in physics. We also aim to provide a community forum for issues of importance to all physicists, regardless of sub-discipline. The scope of the journal covers all areas of experimental, applied, fundamental, and interdisciplinary physical sciences. Primary research published in Communications Physics includes novel experimental results, new techniques or computational methods that may influence the work of others in the sub-discipline. We also consider submissions from adjacent research fields where the central advance of the study is of interest to physicists, for example material sciences, physical chemistry and technologies.
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