Aryana Kiumars, Zhang Yifei, Tomko John A, Hoque Md Shafkat Bin, Hoglund Eric R, Olson David H, Nag Joyeeta, Read John C, Ríos Carlos, Hu Juejun, Hopkins Patrick E
Department of Mechanical and Aerospace Engineering, University of Virginia, Charlottesville, VA, 22904, USA.
Department of Materials Science and Engineering, Massachusetts Institute of Technology, Cambridge, MA, USA.
Nat Commun. 2021 Dec 10;12(1):7187. doi: 10.1038/s41467-021-27121-x.
Integrated nanophotonics is an emerging research direction that has attracted great interests for technologies ranging from classical to quantum computing. One of the key-components in the development of nanophotonic circuits is the phase-change unit that undergoes a solid-state phase transformation upon thermal excitation. The quaternary alloy, GeSbSeTe, is one of the most promising material candidates for application in photonic circuits due to its broadband transparency and large optical contrast in the infrared spectrum. Here, we investigate the thermal properties of GeSbSeTe and show that upon substituting tellurium with selenium, the thermal transport transitions from an electron dominated to a phonon dominated regime. By implementing an ultrafast mid-infrared pump-probe spectroscopy technique that allows for direct monitoring of electronic and vibrational energy carrier lifetimes in these materials, we find that this reduction in thermal conductivity is a result of a drastic change in electronic lifetimes of GeSbSeTe, leading to a transition from an electron-dominated to a phonon-dominated thermal transport mechanism upon selenium substitution. In addition to thermal conductivity measurements, we provide an extensive study on the thermophysical properties of GeSbSeTe thin films such as thermal boundary conductance, specific heat, and sound speed from room temperature to 400 °C across varying thicknesses.
集成纳米光子学是一个新兴的研究方向,已引起从经典计算到量子计算等各种技术的广泛关注。纳米光子电路发展中的关键组件之一是相变单元,它在热激发下会发生固态相变。四元合金GeSbSeTe因其宽带透明度和在红外光谱中的大光学对比度,是光子电路应用中最有前景的材料候选者之一。在此,我们研究了GeSbSeTe的热性质,并表明用硒替代碲后,热输运从电子主导 regime 转变为声子主导 regime。通过实施一种超快中红外泵浦 - 探测光谱技术,该技术允许直接监测这些材料中电子和振动能量载流子的寿命,我们发现热导率的降低是GeSbSeTe电子寿命急剧变化的结果,导致在硒替代后从电子主导的热输运机制转变为声子主导的热输运机制。除了热导率测量外,我们还对GeSbSeTe薄膜的热物理性质进行了广泛研究,如热边界电导、比热容和声速,这些性质是在室温至400°C范围内,针对不同厚度进行研究的。