Habibi Mohammad, Beardo Albert, Cui Longji
Department of Mechanical Engineering, University of Colorado Boulder, Boulder, Colorado 80309, United States.
Department of Physics, JILA, and STROBE NSF Science and Technology Center, University of Colorado and NIST, Boulder, Colorado 80309, United States.
ACS Nano. 2025 Feb 18;19(6):6033-6043. doi: 10.1021/acsnano.4c11893. Epub 2025 Feb 9.
Understanding the energy transport properties of hot energy carriers is of great importance for a diverse range of topics from nanoelectronics and photochemistry to the discovery of quantum materials. While much progress has been made in the study of hot carrier dynamics using ultrafast far-field time-resolved spectroscopies, it remains a great challenge to understand hot carrier transport and interaction dynamics at the nanoscale. Existing theoretical models yield only qualitative predictions that are difficult to validate against experiments. Here we present a theoretical framework that extends the study of near-field thermal radiation into the ultrafast time domain, enabling sensitive local probing and quantitative study of nanoscale hot electron and phonon transport effects that have been challenging to quantify. The proposed technique of near-field hot carrier nanoscopy directly links the features of different nonequilibrium effects to near-field thermal absorption and scattering by a scanning nanotip. Our model predicts ultrafast thermal radiation in response to photoexcitation, as well as elucidates the nanoscopic radiation properties of a number of hot carrier dissipation pathways, including nonlinear electron supercollision, second sound, and nonlocal phonon transport. This work is expected to guide experiments to identify the fundamental constraints unlocking thermal wave (second sound) propagation and address the roles of competing hydrodynamic and ballistic phonon effects at the nanoscale.
了解热载流子的能量传输特性对于从纳米电子学、光化学到量子材料发现等众多领域都至关重要。虽然在使用超快远场时间分辨光谱研究热载流子动力学方面已经取得了很大进展,但在纳米尺度上理解热载流子传输和相互作用动力学仍然是一个巨大的挑战。现有的理论模型仅给出定性预测,难以与实验进行验证。在此,我们提出一个理论框架,将近场热辐射的研究扩展到超快时域,从而能够对难以量化的纳米尺度热电子和声子传输效应进行灵敏的局部探测和定量研究。所提出的近场热载流子纳米显微镜技术将不同非平衡效应的特征直接与扫描纳米尖端的近场热吸收和散射联系起来。我们的模型预测了光激发下的超快热辐射,并阐明了包括非线性电子超碰撞、第二声和非局部声子传输在内的多种热载流子耗散途径的纳米级辐射特性。这项工作有望指导实验确定释放热波(第二声)传播的基本限制,并解决纳米尺度上竞争的流体动力学和弹道声子效应的作用。