掃描隧道顯微鏡誘導(dǎo)發(fā)光技術(shù)在納米表征中的應(yīng)用
發(fā)布時(shí)間：2018-08-27 11:49
【摘要】：如何在單分子尺度上揭示納米結(jié)構(gòu)的光電特性是納米光電子學(xué)研究中的核心科學(xué)問題。掃描隧道顯微鏡(STM)具有單原子級(jí)別的實(shí)空間表征能力,極大地提高了人類認(rèn)識(shí)和操控微觀世界的能力。將STM與光學(xué)檢測(cè)技術(shù)結(jié)合起來的STM誘導(dǎo)發(fā)光技術(shù)(STML),可以把高空間分辨的形貌表征技術(shù)與高靈敏的能量、時(shí)間分辨的光學(xué)檢測(cè)技術(shù)結(jié)合起來,不僅提高了 STM的化學(xué)分析能力,而且還可以幫助我們研究納米結(jié)構(gòu)-固體界面以及納米結(jié)構(gòu)在特定納米環(huán)境中的躍遷及其相關(guān)的動(dòng)力學(xué)過程。本論文的主要工作就是發(fā)展并完善了與超高真空低溫STM聯(lián)用的STML技術(shù),實(shí)現(xiàn)了單分子電致熒光,并利用單分子電致熒光穩(wěn)態(tài)成像技術(shù)表征了分子質(zhì)子轉(zhuǎn)移的瞬態(tài)中間態(tài),為拓展STML技術(shù)在納米光源、光電集成、以及化學(xué)反應(yīng)動(dòng)態(tài)學(xué)等方面的應(yīng)用奠定了基礎(chǔ)。本論文分為四個(gè)部分:第一章,我們首先簡(jiǎn)要介紹了 STM以及表面等離激元(surface plasmons)的物理背景和研究現(xiàn)狀。隨后,我們?cè)敿?xì)介紹了 STM誘導(dǎo)發(fā)光技術(shù)及其研究現(xiàn)狀。最后,我們簡(jiǎn)單地介紹了本工作中所使用的相關(guān)實(shí)驗(yàn)儀器。第二章,我們研究了 STM誘導(dǎo)的單個(gè)空心酞菁分子(H_2Pc)的電致熒光現(xiàn)象。利用NaCl薄膜作為脫耦合層,我們成功地實(shí)現(xiàn)了源自H_2Pc分子HOMO-LUMO能級(jí)間輻射躍遷的單分子電致熒光。通過分析電致發(fā)光光譜隨納腔等離激元模式的變化,我們討論了納腔等離激元在STM誘導(dǎo)分子發(fā)光中的重要作用,并結(jié)合隧穿電導(dǎo)譜討論了單分子電致發(fā)光機(jī)理。我們還利用STM操縱技術(shù)展示了隧道結(jié)中單分子發(fā)光的可調(diào)性。第三章,我們研究了單個(gè)空心酞菁分子內(nèi)的質(zhì)子轉(zhuǎn)移過程。我們利用納腔等離激元共振增強(qiáng),提高了單個(gè)H_2Pc分子的自發(fā)輻射速率,并探測(cè)到單個(gè)H_2Pc分子的熱熒光。結(jié)合光譜成像技術(shù),我們首次在單分子尺度上直接觀察到分子內(nèi)質(zhì)子轉(zhuǎn)移過程中中間態(tài)的存在。我們的結(jié)果不僅可以幫助人們更加深刻地理解卟啉酞菁類分子內(nèi)的質(zhì)子轉(zhuǎn)移過程,而且還提供了一種新的利用非馳豫熒光成像技術(shù)探索表面上分子動(dòng)力學(xué)過程的新思路與新方法。第四章,我們對(duì)現(xiàn)有的STML探測(cè)模式進(jìn)行了拓展。首先,為了表征納米結(jié)構(gòu)的近場(chǎng)光學(xué)特性,我們發(fā)展了近場(chǎng)收集模式。我們使用尖端鍍有半導(dǎo)體透明導(dǎo)電膜(ITO)的光纖探針作為STM針尖,研究了 GaAs(110)表面以及吸附在GaAs(110)表面的H2TBPP分子的STM誘導(dǎo)發(fā)光現(xiàn)象,初步實(shí)現(xiàn)了近場(chǎng)探測(cè)。其次,為了獲取隧道結(jié)中單個(gè)分子輻射的角向分布特性和偏振特性,進(jìn)而分析隧道結(jié)中分子偶極取向等重要信息,我們發(fā)展了低溫超高真空STML的樣品背面的光子收集系統(tǒng),目前已初步實(shí)現(xiàn)了后焦面成像探測(cè),為后續(xù)單分子光源和光電集成的研究奠定了基礎(chǔ)。
[Abstract]:How to reveal the photoelectric properties of nanostructures on a single molecular scale is a key scientific issue in the study of nano-optoelectronics. The scanning tunneling microscope (STM) (STM) has the ability to represent the real space at the single atomic level, which greatly improves the ability of human beings to understand and manipulate the microcosm. STM induced luminescence (STML), which combines STM with optical detection, not only improves the ability of chemical analysis of STM, but also combines high spatial resolution morphology characterization technology with high sensitive energy and time-resolved optical detection technology. It can also help us to study the nanostructure-solid interface and the transition of nanostructures in specific nanoscale environments and the related kinetic processes. The main work of this thesis is to develop and perfect the STML technology combined with ultra-high vacuum low temperature (STM) to realize single molecule electrofluorescence, and to characterize the transient intermediate state of molecular proton transfer by using monolayer electrofluorescence steady-state imaging technique. It lays a foundation for the application of STML technology in nanometer light source, optoelectronic integration, chemical reaction dynamics and so on. This thesis is divided into four parts: in Chapter 1, we briefly introduce the physical background and research status of STM and (surface plasmons). Then, we introduce the STM induced luminescence technology and its research status in detail. Finally, we briefly introduce the related experimental instruments used in this work. In chapter 2, we study the electroluminescence of a single hollow phthalocyanine molecule (H_2Pc) induced by STM. Using the NaCl film as the decoupling layer, we have successfully realized the monolayer electroluminescence from the radiation transition between the HOMO-LUMO energy levels of the H_2Pc molecule. By analyzing the variation of electroluminescence spectra with the mode of nanoscale isophosphors, we discuss the important role of nanoscale isophosphors in STM induced molecular luminescence, and discuss the mechanism of monolayer electroluminescence in combination with tunneling conductance spectroscopy. We also demonstrate the tunability of monolayer luminescence in tunnel junctions by using STM manipulation technique. In chapter 3, we study the proton transfer process in a single hollow phthalocyanine molecule. The spontaneous emission rate of a single H_2Pc molecule is increased and the thermal fluorescence of a single H_2Pc molecule is detected. In combination with spectral imaging techniques, we observed the presence of intermediate states in intramolecular proton transfer processes on a single molecular scale for the first time. Our results not only help people understand the proton transfer process in porphyrin phthalocyanines, It also provides a new idea and a new method to explore the molecular dynamics process on the surface by using the non-relaxation fluorescence imaging technology. In chapter 4, we extend the existing STML detection mode. First, in order to characterize the near-field optical properties of nanostructures, we developed a near-field collection model. The STM induced luminescence of GaAs (110) and H2TBPP molecules adsorbed on the surface of GaAs (110) and on the surface of GaAs (110) have been studied by using the fiber probe coated with semiconductor transparent conductive film (ITO) as the tip of the STM needle. The near field detection has been preliminarily realized. Secondly, in order to obtain the angular distribution and polarization characteristics of single molecule radiation in tunnel junctions, and to analyze the important information of molecular dipole orientation in tunnel junctions, we developed a photon collection system on the back of samples of ultra-high vacuum STML at low temperature. At present, the detection of rear focal plane imaging has been preliminarily realized, which lays a foundation for the further study of monolayer light source and optoelectronic integration.
【學(xué)位授予單位】：中國科學(xué)技術(shù)大學(xué)
【學(xué)位級(jí)別】：博士
【學(xué)位授予年份】：2017
【分類號(hào)】：TH742;TB383.1
本文編號(hào)：2207187
[Abstract]:How to reveal the photoelectric properties of nanostructures on a single molecular scale is a key scientific issue in the study of nano-optoelectronics. The scanning tunneling microscope (STM) (STM) has the ability to represent the real space at the single atomic level, which greatly improves the ability of human beings to understand and manipulate the microcosm. STM induced luminescence (STML), which combines STM with optical detection, not only improves the ability of chemical analysis of STM, but also combines high spatial resolution morphology characterization technology with high sensitive energy and time-resolved optical detection technology. It can also help us to study the nanostructure-solid interface and the transition of nanostructures in specific nanoscale environments and the related kinetic processes. The main work of this thesis is to develop and perfect the STML technology combined with ultra-high vacuum low temperature (STM) to realize single molecule electrofluorescence, and to characterize the transient intermediate state of molecular proton transfer by using monolayer electrofluorescence steady-state imaging technique. It lays a foundation for the application of STML technology in nanometer light source, optoelectronic integration, chemical reaction dynamics and so on. This thesis is divided into four parts: in Chapter 1, we briefly introduce the physical background and research status of STM and (surface plasmons). Then, we introduce the STM induced luminescence technology and its research status in detail. Finally, we briefly introduce the related experimental instruments used in this work. In chapter 2, we study the electroluminescence of a single hollow phthalocyanine molecule (H_2Pc) induced by STM. Using the NaCl film as the decoupling layer, we have successfully realized the monolayer electroluminescence from the radiation transition between the HOMO-LUMO energy levels of the H_2Pc molecule. By analyzing the variation of electroluminescence spectra with the mode of nanoscale isophosphors, we discuss the important role of nanoscale isophosphors in STM induced molecular luminescence, and discuss the mechanism of monolayer electroluminescence in combination with tunneling conductance spectroscopy. We also demonstrate the tunability of monolayer luminescence in tunnel junctions by using STM manipulation technique. In chapter 3, we study the proton transfer process in a single hollow phthalocyanine molecule. The spontaneous emission rate of a single H_2Pc molecule is increased and the thermal fluorescence of a single H_2Pc molecule is detected. In combination with spectral imaging techniques, we observed the presence of intermediate states in intramolecular proton transfer processes on a single molecular scale for the first time. Our results not only help people understand the proton transfer process in porphyrin phthalocyanines, It also provides a new idea and a new method to explore the molecular dynamics process on the surface by using the non-relaxation fluorescence imaging technology. In chapter 4, we extend the existing STML detection mode. First, in order to characterize the near-field optical properties of nanostructures, we developed a near-field collection model. The STM induced luminescence of GaAs (110) and H2TBPP molecules adsorbed on the surface of GaAs (110) and on the surface of GaAs (110) have been studied by using the fiber probe coated with semiconductor transparent conductive film (ITO) as the tip of the STM needle. The near field detection has been preliminarily realized. Secondly, in order to obtain the angular distribution and polarization characteristics of single molecule radiation in tunnel junctions, and to analyze the important information of molecular dipole orientation in tunnel junctions, we developed a photon collection system on the back of samples of ultra-high vacuum STML at low temperature. At present, the detection of rear focal plane imaging has been preliminarily realized, which lays a foundation for the further study of monolayer light source and optoelectronic integration.
【學(xué)位授予單位】：中國科學(xué)技術(shù)大學(xué)
【學(xué)位級(jí)別】：博士
【學(xué)位授予年份】：2017
【分類號(hào)】：TH742;TB383.1
【參考文獻(xiàn)】
相關(guān)期刊論文 前1條
1 董振超;張楊;陶興;楊金龍;侯建國;;掃描隧道顯微鏡誘導(dǎo)發(fā)光的歷史和進(jìn)展[J];科學(xué)通報(bào);2009年08期
，本文編號(hào)：2207187
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