Nanoscale coherent phonon spectroscopy.

Nanoscale coherent phonon spectroscopy.
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DOI:
10.1126/sciadv.abq5682
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发表时间:
2022-10-21
期刊:
影响因子:
13.6
通讯作者:
--
中科院分区:
综合性期刊1区
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--
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相干声子光谱可以提供对超快晶格动力学及其在非平衡条件下与其他自由度的耦合的微观洞察。超快光谱是研究相干声子的成熟方法,但衍射极限阻碍了直接观察其局部动力学。在这里,我们在等离子体结中使用超快激光诱导扫描隧道显微镜演示了纳米级相干声子光谱。相干声子在超薄氧化锌薄膜中被严格限制的等离子体场局部激发,并通过氧化锌薄膜的电子谐振通过光致隧道电流进行探测。同时进行的尖端增强拉曼光谱使我们能够识别所涉及的声子模式。与拉曼光谱相反,相干声子光谱中观察到的声子动力学表现出强烈的纳米级空间变化,这些变化与扫描隧道光谱解析的电子局域态密度的分布相关。超快扫描隧道显微镜以纳米级空间分辨率观察表面的相干声子。
Coherent phonon spectroscopy can provide microscopic insight into ultrafast lattice dynamics and its coupling to other degrees of freedom under nonequilibrium conditions. Ultrafast optical spectroscopy is a well-established method to study coherent phonons, but the diffraction limit has hampered observing their local dynamics directly. Here, we demonstrate nanoscale coherent phonon spectroscopy using ultrafast laser–induced scanning tunneling microscopy in a plasmonic junction. Coherent phonons are locally excited in ultrathin zinc oxide films by the tightly confined plasmonic field and are probed via the photoinduced tunneling current through an electronic resonance of the zinc oxide film. Concurrently performed tip-enhanced Raman spectroscopy allows us to identify the involved phonon modes. In contrast to the Raman spectra, the phonon dynamics observed in coherent phonon spectroscopy exhibit strong nanoscale spatial variations that are correlated with the distribution of the electronic local density of states resolved by scanning tunneling spectroscopy. Ultrafast scanning tunneling microscopy observes coherent phonons at a surface with nanoscale spatial resolution.
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