热电材料可实现热能和电能的直接转换，在温差发电和固态制冷领域有巨大的应用潜力和价值。氧化锌（ZnO）材料因其元素储量丰富、无毒无害并且具有良好的化学稳定性和热稳定性以及电学性能易调控等优势而成为一种理想的热电材料。但是本征的ZnO块体材料电导率低、热导率高的劣势，极大地限制了其热电性能。低维化可以增加热输运和电输运性能调控的自由度，因此本文以ZnO热电薄膜材料为研究对象，通过掺杂调控、结构设计、界面优化以及熵工程等方法来综合调控其热电性能。针对本征ZnO载流子浓度低的问题，通过脉冲激光沉积技术制备了高度取向的镓掺杂氧化锌（GZO）薄膜。Ga元素的掺杂有效提升了ZnO的载流子浓度，并且通过调控生长参数，发现673 K的沉积温度有利于生长高质量的GZO薄膜，且在单晶蓝宝石（Al2O3）衬底上生长厚度约为50 nm的薄膜具有最高的载流子浓度和载流子迁移率，功率因子在623 K下达到了333 μW m?1 K−2。针对载流子浓度的提升会恶化塞贝克系数的问题，提出了一种三明治结构（GZO-ZnO-GZO）薄膜结合氧空位调控的策略协同优化了电导率和塞贝克系数，进一步提升了薄膜的热电性能，功率因子在623 K时达到了434 μW m?1 K−2； 基于三明治结构，进一步设计了多ZnO-GZO界面结构薄膜并且采用还原气氛进行热处理，薄膜的功率因子在623 K时达到了439 μW m?1 K−2，相较于未处理的GZO单层薄膜性能提升了约32%。针对GZO薄膜迁移率较低的问题，通过在单晶蓝宝石衬底和薄膜间引入ZnO缓冲层以及直接在单晶ZnO衬底上生长GZO薄膜的方法，有效地提升了载流子迁移率，最高达到了46.5 cm?2 V−1 s?1，同时基于ZnO-GZO的界面效应，协同优化了GZO薄膜的热电性能。最高的功率因子在室温和623 K下分别达到了333 μW m?1 K−2和2214 μW m?1 K−2，是目前本体系的最高值之一。针对GZO薄膜塞贝克系数较低的问题，将高导电的GZO与高塞贝克系数的高熵氧化物（HEO）复合，制备了GZO-HEO-GZO结构薄膜，薄膜的塞贝克系数有所增加，但是由于低电导率HEO层的加入，导致GZO-HEO-GZO的电导率降低，因此功率因子并未因HEO层的加入而提高。

Thermoelectric materials can realize the direct conversion of heat energy and electrical energy, which gives it the potential for broader application in the field of thermoelectric power generation and cooling. Zinc oxide (ZnO) is an ideal thermoelectric material because of its abundant reserves, non-toxicity, harmlessness, good chemical and thermal stability, as well as the controllability of its electrical properties. However, ZnO bulks show poor thermoelectric performance due to their low electrical conductivity and high thermal conductivity. Since dimensionality reduction can increase the degree of freedom to tune the thermal and electrical transport, this paper focused on ZnO thin films and aimed to improve their thermoelectric properties comprehensively by effective doping, structural design, interface optimization and entropy engineering.As to the low carrier concentration of intrinsic ZnO, highly oriented Ga doped ZnO (GZO) thin films were prepared by pulsed laser deposition (PLD) techniques. It showed that Ga doping could effectively improve the carrier concentration of ZnO. Also, by adjusting growth parameters, it was found that the deposition temperature of 673 K was conducive to the growth of high-quality GZO thin films. Furthermore, the thin film with a thickness of around 50 nm grown on the single crystal sapphire substrate had the highest carrier concentration and carrier mobility, whose power factor was 333 μW m?1 K−2 at 623 K.As regards the negative correlation between the Seebeck coefficient and the carrier concentration, a sandwich-structured (GZO-ZnO-GZO) thin film combined with oxygen vacancy control was proposed to simultaneously optimize the electrical conductivity and the Seebeck coefficient. The thermoelectric performance had been improved further, whose power factor reached 434 μW m?1 K−2 at 623 K. Moreover, based on the sandwich structure, the method of multi ZnO-GZO interface structure film combined with heat treatment under a reduction atmosphere was adopted. Consequently, the power factor of the film reached 439 μW m?1 K−2 at 623 K, which is about 32% higher than that of the untreated GZO thin film.In terms of the low mobility of GZO thin films, the study introduced a ZnO buffer layer between the single crystal sapphire substrate and thin films, and also directly grew GZO thin films on single-crystal ZnO substrates. As a result, the carrier mobility was effectively improved, which peaked at 46.5 cm?2 V−1 s?1. At the same time, according to the interface effect of the ZnO-GZO, the thermoelectric properties of GZO thin films were optimized. At room temperature and 623 K, the highest power factors were 333 μW m?1 K−2 and 2214 μW m?1 K−2, respectively, which is also one of the highest values in ZnO based films and bulks at present.To increase the Seebeck coefficient of GZO thin films, this research synthesized a GZO-HEO-ZnO composite film by blending high-conductivity GZO and high-entropy oxide (HEO) with a high Seebeck coefficient. While the Seebeck coefficient of the films augmented, however, the electrical conductivity of GZO-HEO-ZnO dropped due to the low conductivity of HEO, so the power factor did not increase when the HEO layer was added.