【摘要】：在半導(dǎo)體量子點(diǎn)中，因?yàn)橛辛孔酉抻蛐?yīng)的存在，使得其具有獨(dú)特的光學(xué)性質(zhì)。因此，其在生物、光電及光伏等領(lǐng)域具有重要的應(yīng)用前景。本文基于綠色化學(xué)的理念，從材料的合成、光學(xué)機(jī)理及應(yīng)用等方面，對(duì)無(wú)毒的銅銦硫基量子點(diǎn)展開實(shí)驗(yàn)研究，取得了以下創(chuàng)新研究成果： 1．量子點(diǎn)光學(xué)機(jī)理方面的研究。我們合成了CuInS2量子點(diǎn)、CuInS2/ZnS核/殼量子點(diǎn)以及ZnCuInS/ZnSe/ZnS核/殼/殼量子點(diǎn)。在對(duì)其性能的表征過(guò)程中，發(fā)現(xiàn)了此類量子點(diǎn)具有的一些特性，包括吸收光譜和發(fā)光光譜均較寬，存在著較大的Stokes位移等，這是由其能帶結(jié)構(gòu)及發(fā)光機(jī)理決定的。較大的Stokes位移（400-500meV）證明，在此類量子點(diǎn)中主要的復(fù)合過(guò)程是與缺陷能級(jí)有關(guān)的復(fù)合。而較為明顯的尺寸依賴效應(yīng)同時(shí)證明了，施主-受主對(duì)（donor-acceptorpair，縮寫DAP）復(fù)合是該類量子點(diǎn)的多種主要的復(fù)合過(guò)程之一，而并不是占主導(dǎo)的復(fù)合過(guò)程。分別測(cè)試了ZnCuInS/ZnSe/ZnS核/殼/殼量子點(diǎn)、Cu與In比例不同的CuInS2量子點(diǎn)及CuInS2/ZnS核/殼量子點(diǎn)的溫度依賴的光致發(fā)光光譜和時(shí)間分辨光致發(fā)光光譜。通過(guò)對(duì)多種光譜的分析，我們深入地研究了此類量子點(diǎn)的復(fù)合機(jī)理。并提出了，在此類量子點(diǎn)中，同時(shí)存在著多種復(fù)合過(guò)程，包括與表面態(tài)有關(guān)的復(fù)合、導(dǎo)帶與缺陷能級(jí)間的復(fù)合以及DAP復(fù)合。然后，我們改變CuInS2量子點(diǎn)及CuInS2/ZnS核/殼量子點(diǎn)中Cu與In的比例，分析其溫度依賴的光致發(fā)光光譜發(fā)現(xiàn)，當(dāng)In組分含量增大時(shí)，在與表面態(tài)有關(guān)的復(fù)合、導(dǎo)帶與缺陷能級(jí)間的復(fù)合以及DAP復(fù)合中，，DAP復(fù)合所占的比重有所增加。 3．基于ZnCuInS/ZnSe/ZnS核/殼/殼量子點(diǎn)發(fā)光的溫度特性的研究，我們將其應(yīng)用于微區(qū)、面陣的溫度傳感中。測(cè)得該量子點(diǎn)光致發(fā)光強(qiáng)度隨溫度變化的系數(shù)（溫度系數(shù)）達(dá)到0.66%/oC。使用光纖光譜儀與高倍顯微鏡組成了測(cè)試系統(tǒng)，通過(guò)測(cè)試微米區(qū)域的量子點(diǎn)的光致發(fā)光光譜來(lái)完成微區(qū)、面陣的溫度檢測(cè)。該系統(tǒng)測(cè)試的誤差低于2%。 4．量子點(diǎn)發(fā)光二極管（QD-LED）的制備及溫度效應(yīng)的研究。將三個(gè)尺寸的ZnCuInS/ZnSe/ZnS核/殼/殼量子點(diǎn)分別與GaN發(fā)光二極管組裝，制成了紅光、黃光和綠光的QD-LED。在2.6V的工作電壓下，相應(yīng)的三種顏色的QD-LED的功率效率依次為14.0lm/W、47.1lm/W和62.4lm/W。通過(guò)對(duì)不同工作電壓下QD-LED的色坐標(biāo)，光譜峰位，半峰寬及功率效率的分析，我們研究了QD-LED的溫度效應(yīng)。結(jié)果表明，就器件的功率效率隨著電壓升高的下降而言，發(fā)光二極管表面溫度的升高引起的熱猝滅是一個(gè)不可忽視的因素。同時(shí)ZnCuInS/ZnSe/ZnS核/殼/殼量子點(diǎn)的發(fā)射峰位的溫度系數(shù)很低（紅光，黃光及綠光量子點(diǎn)的溫度系數(shù)分別為0.022nm/oC、0.050nm/oC和0.068nm/oC），這使得QD-LED的色坐標(biāo)在不同工作電壓下，變化非常小，證明了該QD-LED的顏色穩(wěn)定性好。與CdSe量子點(diǎn)的相應(yīng)數(shù)據(jù)相比，ZnCuInS/ZnSe/ZnS核/殼/殼量子點(diǎn)在顏色穩(wěn)定性方面，更適合做下轉(zhuǎn)換材料。
[Abstract]:In semiconductor quantum dots, due to the existence of quantum confinement effect, it has unique optical properties. Therefore, it has an important application prospect in biological, photoelectric and photovoltaic fields. In this paper, based on the concept of green chemistry, the nontoxic copper-indium-sulfur-based quantum dots have been experimentally studied from the aspects of material synthesis, optical mechanism and application, and the following innovative achievements have been obtained: 1. The optical mechanism of quantum dots has been studied. We have synthesized CuInS2 quantum dots, CuInS2/ZnS core / shell quantum dots and ZnCuInS/ZnSe/ZnS core / shell quantum dots. During the characterization of the quantum dots, some properties of these quantum dots were found, including the wide absorption and luminescence spectra, and the existence of a large Stokes shift, which is determined by the energy band structure and the luminescence mechanism. The large Stokes shift (400-500meV) proves that the main recombination process in this kind of quantum dots is the recombination related to the defect energy level. The obvious size-dependent effect also proves that the donor-acceptor pair (donor-acceptorpair,-acceptor pair) recombination is one of the main recombination processes of this kind of quantum dots, but not the dominant one. The temperature-dependent photoluminescence spectra and time-resolved photoluminescence spectra of ZnCuInS/ZnSe/ZnS core / shell quantum dots, CuInS2 quantum dots with different ratio of Cu to In and CuInS2/ZnS core / shell quantum dots were measured. Through the analysis of many kinds of spectra, we have studied the recombination mechanism of this kind of quantum dots in depth. It is also proposed that there are many kinds of recombination processes in the quantum dots, including the recombination related to the surface states, the recombination between the conduction band and the defect level, and the DAP recombination. Then, we change the ratio of Cu to In in CuInS2 QDs and CuInS2/ZnS core / shell QDs and analyze their temperature dependent photoluminescence spectra. The recombination between conduction band and defect level and the proportion of DAP recombination in DAP recombination increased. 3. Based on the study of temperature characteristics of ZnCuInS/ZnSe/ZnS core / shell quantum dots, we apply them to temperature sensing of micro-region and area array. The coefficient (temperature coefficient) of photoluminescence intensity of the quantum dot with temperature is 0.66%, and the temperature coefficient of photoluminescence of the quantum dot is 0.66%. An optical fiber spectrometer and a high power microscope are used to measure the temperature of the micro-region and the area array by measuring the photoluminescence spectra of the quantum dots in the micron region. The test error of the system is less than 2%. 4. Preparation of quantum dot light emitting diode (QD-LED) and study of temperature effect. Three sizes of ZnCuInS/ZnSe/ZnS core / shell quantum dots were assembled with GaN light emitting diodes to produce QD-LED. with red, yellow and green light. Under the operating voltage of 2.6 V, the power efficiency of the corresponding three colors of QD-LED is 14.0 lm / W, 47.1lm / W and 62.4lm / w, respectively. By analyzing the color coordinates, spectral peak position, half-peak width and power efficiency of QD-LED at different operating voltages, we have studied the temperature effect of QD-LED. The results show that the thermal quenching caused by the rising surface temperature of light emitting diodes is an important factor for the decrease of the power efficiency of the devices with the increase of the voltage. At the same time, the temperature coefficients of the emission peaks of ZnCuInS/ZnSe/ZnS core / shell QDs are very low (the temperature coefficients of red, yellow and green QDs are 0.022 nm C, 0.050 nm C and 0.068nm/oC, respectively). This makes the color coordinates of QD-LED change little under different working voltages, which proves that the color stability of the QD-LED is good. Compared with the corresponding data of CdSe QDs, ZnCuInS/ZnSe/ZnS core / shell QDs are more suitable for down-conversion materials in terms of color stability.
【學(xué)位授予單位】：吉林大學(xué)
【學(xué)位級(jí)別】：博士
【學(xué)位授予年份】：2015
【分類號(hào)】：O471.1

【共引文獻(xiàn)】

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5 謝翠萍;向衛(wèi)東;駱樂;鐘家松;趙斌宇;梁曉娟;;AgInS_2量子點(diǎn)研究進(jìn)展[J];功能材料;2014年04期

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本文編號(hào)：2436610