Recycling failed photoelectrons via tertiary photoemission

M. Matzelle, Wei-Chi Chiu, Caiyun Hong, Barun Ghosh, Pengxu Ran, R. S. Markiewicz, B. Barbiellini, Changxi Zheng, Sheng Li, Rui-Hua He, Arun Bansil
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Abstract

A key insight of Einstein's theory of the photoelectric effect is that a minimum energy is required for photoexcited electrons to escape from a material. For the past century it has been assumed that photoexcited electrons of lower energies make no contribution to the photoemission spectrum. Here we demonstrate the conceptual possibility that the energy of these 'failed' photoelectrons-primary or secondary-can be partially recycled to generate new 'tertiary' electrons of energy sufficient to escape. Such a 'recycling' step goes beyond the traditional three steps of the photoemission process (excitation, transport, and escape), and, as we illustrate, it can be realized through a novel Auger mechanism that involves three distinct minority electronic states in the material. We develop a phenomenological three-band model to treat this mechanism within a revised four-step framework for photoemission, which contains robust features of linewidth narrowing and population inversion under strong excitation, reminiscent of the lasing phenomena. We show that the conditions for this recycling mechanism are likely satisfied in many quantum materials with multiple flat bands properly located away from the Fermi level, and elaborate on the representative case of SrTiO3 among other promising candidates. We further discuss how this mechanism can explain the recent observation of anomalous intense coherent photoemission from a SrTiO3 surface, and predict its manifestations in related experiments, including the 'forbidden' case of photoemission with photon energies lower than the work function. Our study calls for paradigm shifts across a range of fundamental and applied research fields, especially in the areas of photoemission, photocathodes, and flat-band materials.
通过三次光发射回收失效光电子
爱因斯坦光电效应理论的一个重要观点是,光激发电子从物质中逸出需要最低能量。在过去的一个世纪里,人们一直认为能量较低的光激发电子不会对光发射光谱产生任何影响。在这里,我们展示了一种概念上的可能性,即这些 "失败 "光电子--初级或次级--的能量可以被部分回收利用,以产生能量足以逸出的新的 "三级 "电子。这种 "再循环 "步骤超越了光发射过程的传统三个步骤(激发、传输和逸出),正如我们所说明的,它可以通过一种涉及材料中三种不同少数电子态的新型奥杰机制来实现。我们建立了一个现象学三条带模型,在修订后的光致发光四步框架内处理这一机制,其中包含线宽收窄和强激发下的种群反转等强健特征,让人联想到激光现象。我们的研究表明,在许多具有远离费米级的多个平坦带的量子材料中,都可能满足这种再循环机制的条件。我们进一步讨论了这一机制如何解释最近从 SrTiO3 表面观察到的异常强相干光发射,并预测了其在相关实验中的表现,包括光子能量低于功函数的 "禁止 "光发射情况。我们的研究呼唤着一系列基础和应用研究领域的范式转变,尤其是在光致发光、光电阴极和平带材料领域。
本文章由计算机程序翻译,如有差异,请以英文原文为准。
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