本文選題：二維材料　切入點(diǎn)：石墨烯　出處：《南京大學(xué)》2017年博士論文　論文類型：學(xué)位論文

【摘要】：近些年來(lái),二維材料的廣泛研究是繼石墨烯(graphene)的發(fā)現(xiàn)并證實(shí)它能夠在室溫下穩(wěn)定存在之后。人們相繼發(fā)現(xiàn)其他多種二維材料,例如氮化硼(BN)、過(guò)渡金屬硫族化合物(TMDs)、黑磷(b-P)及黑磷合金等,這些新型二維材料的發(fā)現(xiàn)引起了人們極大的關(guān)注。由于這些新型二維層狀材料具有不同的帶隙大小,因而可以將其分為絕緣體、半導(dǎo)體和半金屬。這些新型二維材料分別具有各自的優(yōu)異性質(zhì)和不足。所幸運(yùn)的是,便捷的二維材料異質(zhì)結(jié)制作和組裝技術(shù)的發(fā)展,使得這些二維材料相互彌補(bǔ)不足和發(fā)揮優(yōu)勢(shì)�？梢酝ㄟ^(guò)任意堆疊次序不同的二維材料形成的異質(zhì)結(jié)。從而我們能夠使用異質(zhì)結(jié)研究一些基礎(chǔ)物理和器件性能。從而使得人們能夠在研究人工結(jié)構(gòu)材料上獲得重大的突破。石墨烯具有線性色散關(guān)系、無(wú)質(zhì)量狄拉克費(fèi)米子、高遷移率和無(wú)帶隙性質(zhì)。更重要的是石墨烯具有相對(duì)較強(qiáng)的光吸收,單原子層吸收2.3%并與層數(shù)無(wú)關(guān)。這些優(yōu)異的物理性質(zhì)使得石墨烯材料在光探測(cè)尤其是紅外波段光探測(cè)和高頻器件具有很好的應(yīng)用前景。最近新發(fā)現(xiàn)的黑磷(b-P)和黑砷磷(b-AsP)合金塊體材料帶隙在0.3-0.1電子伏,同時(shí)黑磷晶體的結(jié)構(gòu)對(duì)稱性較低,具有較強(qiáng)的各向異性和對(duì)偏振光的偏振角度的靈敏依賴。另外黑磷是p-型的二維半導(dǎo)體材料,具有較高的空穴遷移率,使得黑磷是中波紅外光探測(cè)的和偏振光靈敏探測(cè)的理想材料。然而,目前研究最為廣泛的過(guò)渡金屬硫族化合物,由于其具有中等帶隙主要的光電響應(yīng)波段位于可見波段和近紅外波段,而且過(guò)渡金屬硫族化合物具有很強(qiáng)的光與物質(zhì)相互作用、較大的開關(guān)比和比較穩(wěn)定的性質(zhì)等。有望被用于下一代新型邏輯器件和光電子器件。人們?cè)赥MDs中發(fā)現(xiàn)了很多新奇的物理現(xiàn)象和潛在的器件應(yīng)用價(jià)值。氮化硼具有較大帶隙～6.0 eV,對(duì)應(yīng)深紫外波段,屬于二維絕緣體材料,具有較好的介電性能和原子級(jí)平整的襯底,是其他二維半導(dǎo)體材料的很好的保護(hù)層,能夠屏蔽散射獲得較高的電子遷移率。隨著研究的深入,有更多的二維材料等待我們研究發(fā)現(xiàn),有更優(yōu)異的性質(zhì)需要開發(fā)利用為人們更好的服務(wù)。本論文主要研究二維材料及其異質(zhì)結(jié)光電探測(cè),通過(guò)設(shè)計(jì)和制作異質(zhì)結(jié)器件,實(shí)現(xiàn)光探測(cè)中的新的功能和提高探測(cè)器的綜合性能。目前研究最廣泛的半導(dǎo)體二維材料主要是過(guò)渡金屬硫族化合物,由于硫族元素易形成空位,從而容易實(shí)現(xiàn)電子型摻雜,因此過(guò)渡金屬硫族化合物大部分是n-型半導(dǎo)體和雙極性材料。P-n結(jié)具有本征的內(nèi)建電場(chǎng)是邏輯器件和實(shí)現(xiàn)高靈敏光探測(cè)的最基本的需求。目前p-型摻雜的二維材料過(guò)渡金屬硫族化合物還很少,形成能帶結(jié)構(gòu)匹配較好的p-n結(jié),實(shí)現(xiàn)p-型摻雜是目前需要解決的重點(diǎn)之一。對(duì)于高靈敏的光電探測(cè),p-n結(jié)的內(nèi)建電場(chǎng)能夠有效降低暗電流和有效分離光生載流子。制作高質(zhì)量的p-n在光電探測(cè)領(lǐng)域是迫切需要的。我們通過(guò)摻雜Ta實(shí)現(xiàn)WSe2載流子類型的調(diào)控。較強(qiáng)的p-型二維半導(dǎo)體材料是實(shí)現(xiàn)原子層厚度p-n結(jié)的技術(shù)關(guān)鍵。高質(zhì)量的p-n結(jié)是實(shí)現(xiàn)邏輯器件和光伏型探測(cè)的基礎(chǔ)。通過(guò)設(shè)計(jì)p-g-n型異質(zhì)結(jié)器件,實(shí)現(xiàn)寬波段紅外探測(cè),利用石墨烯的無(wú)帶隙性質(zhì),實(shí)現(xiàn)寬波段吸收。通常石墨烯內(nèi)光生載流子的壽命比較短,在內(nèi)建電場(chǎng)作用下可以有效實(shí)現(xiàn)兩種載流子的快速分離�？臻g上的分離能夠有效提高載流子的壽命,同時(shí)內(nèi)建電場(chǎng)有效減低暗電流,從而減小噪聲。因而p-g-n實(shí)現(xiàn)高靈敏寬波段光電探測(cè)。中波紅外在紅外探測(cè)在軍事和導(dǎo)彈制導(dǎo)追蹤等具有重要應(yīng)用價(jià)值。目前,所使用的中波紅外探測(cè)器需要在低溫下工作,需要液氮制冷,使用成本增加和條件苛刻不利于便捷使用。迫切需要發(fā)展和研究室溫便捷的中波紅外探測(cè)器。應(yīng)用窄帶隙b-AsP場(chǎng)效應(yīng)管和b-AsP-MoS2異質(zhì)結(jié)實(shí)現(xiàn)高靈敏室溫中波紅外探測(cè)。在窄帶隙二維層狀材料的合成如PtSe2等和器件應(yīng)用做了一些探索。在第三章中,首先我們?cè)O(shè)計(jì)p-g-n型異質(zhì)結(jié)寬波段光電探測(cè)器。結(jié)合包括拉曼(Raman)、光致發(fā)光(PL)、原子力顯微鏡(AFM)和光學(xué)顯微鏡對(duì)樣品的層數(shù)和薄膜質(zhì)量進(jìn)行了表征。通過(guò)微區(qū)定點(diǎn)轉(zhuǎn)移技術(shù),實(shí)現(xiàn)多層異質(zhì)結(jié)器件的制作。使用具有較大功函數(shù)金屬,例如金屬鈀、鉑、金等實(shí)現(xiàn)WSe2的p-型摻雜調(diào)控。與費(fèi)米面釘扎較強(qiáng)的MoS2形成很好的p-n結(jié)。中間層的無(wú)帶隙的石墨烯可以有效擴(kuò)展響應(yīng)的帶寬。同時(shí)p-g-n異質(zhì)結(jié)還可以使用高遷移率石墨烯作為透明電極,實(shí)現(xiàn)分離后的載流子快速分離。通過(guò)設(shè)計(jì)這種p-g-n異質(zhì)結(jié),我們實(shí)現(xiàn)室溫下探測(cè)波段從400nm-2400nm的寬波段探測(cè)。光電響應(yīng)率高達(dá)4250AW-1,比探測(cè)了高達(dá)1015 Jones。這些高靈敏的光探測(cè)可以實(shí)現(xiàn)光電流成像,較高分辨率的圖像獲得。同時(shí)我們還研究了光電響應(yīng)機(jī)制研究,通過(guò)可見光和近紅外光電流空間成像,得出我們器件的光響應(yīng)是主要來(lái)自p-g-n的內(nèi)建電場(chǎng)的結(jié)區(qū)。另外,背柵和偏置電壓對(duì)光電響應(yīng)具有較好的調(diào)制作用。第四章中我們深入研究了窄帶隙、高遷移率的黑砷磷合金(b-As0.83P0.17)場(chǎng)效應(yīng)器件和黑磷砷合金與硫化鉬(b-Aso.83P0.17-MoS2)異質(zhì)結(jié)器件的中波紅外光探測(cè)性能。重點(diǎn)研究b-As0.83P0.17場(chǎng)效應(yīng)管器件從可見光到中波紅外的光電響應(yīng)的機(jī)制,得出光伏效應(yīng)是紅外波段光電探測(cè)的主要機(jī)制。通過(guò)在黑磷材料中摻雜砷元素并進(jìn)行砷成分調(diào)控,實(shí)現(xiàn)83%的砷摻雜的黑砷磷樣品。通過(guò)樣品吸收光譜的研究發(fā)現(xiàn)b-As0.83Po.17帶隙為～0.15 eV,光學(xué)吸收邊位于1250 cm-1。探測(cè)的探測(cè)波段從可見波段到中波紅外400 nm-8.05 um。我們研究了 b-As0.83P0.17-MoS2異質(zhì)結(jié)的光電響應(yīng),異質(zhì)結(jié)有效降低了暗電流。另外我們研究了異質(zhì)結(jié)器件的噪聲譜,在異質(zhì)結(jié)器件中噪聲功率比b-As0.83P0.17的場(chǎng)效應(yīng)器件噪聲功率密度小兩個(gè)數(shù)量級(jí)。這說(shuō)明異質(zhì)結(jié)器件能夠有效降低暗電流和噪聲功率,有效提高器件的靈敏度。同時(shí)b-As0.83P0.17的樣品具有較強(qiáng)的電學(xué)和光電響應(yīng)的各向異性,因而對(duì)偏振光的偏振角度有靈敏的依賴。我們得到的b-AS0.83P0.17的場(chǎng)效應(yīng)器件比探測(cè)率在所測(cè)波段400 nm-8.05 um都高于108 Jones。對(duì)于異質(zhì)結(jié)器件從400 nm-4.3 um比探測(cè)率高于4.9×1 09 Jones。第五章新型過(guò)渡金屬硫族化合物生長(zhǎng)的探索和窄帶隙材料的合成主要包括以下幾個(gè)部分內(nèi)容,其一,通過(guò)Ta摻雜實(shí)現(xiàn)本征P-型WSe2;其二,CVT合成WSe2納米線;其三,探索窄帶隙低維材料生長(zhǎng)合成,主要包含摻雜的黑磷樣品、CVT方法生長(zhǎng)窄帶隙PtSe2和CVD法硒化金屬鉑獲得PtSe2。采用CVT的方法生長(zhǎng)出了 p-型的Ta摻雜的WSe2單晶,具有良好的p-型導(dǎo)電性質(zhì)。通過(guò)微區(qū)定點(diǎn)轉(zhuǎn)移制備的Ta0.01W0.99Se2-MoS2異質(zhì)結(jié)和Tao.01W0.99Se2-WSe2同質(zhì)結(jié),這些器件表現(xiàn)出理想的二極管性能,理想因子～1,整流比達(dá)到105。光電響應(yīng)實(shí)驗(yàn)進(jìn)一步證明異質(zhì)結(jié)界面質(zhì)量良好。組內(nèi)合作研究了新型二維材料異質(zhì)結(jié)ReS2-BN高靈敏弱光探測(cè)器和WSe2-graphene異質(zhì)結(jié)光電探測(cè)器表現(xiàn)出很好的光電響應(yīng)。最后一章中,我們總結(jié)了一下前面論文中的一些重要結(jié)果,對(duì)目前已取得的進(jìn)展及面臨的一些問題進(jìn)行討論與分析,并且希望來(lái)能夠繼續(xù)推進(jìn)未完成的工作,在二維材料光電探測(cè)的研究方向做出更大的貢獻(xiàn)。
[Abstract]:In recent years, extensive research material is the two-dimensional graphene (graphene) after the discovery and confirmed that it can exist stably at room temperature. People have been found in a variety of other two-dimensional materials such as boron nitride (BN), transition metal chalcogenides (TMDs), black phosphorus (b-P) and black phosphorus alloy and so on, these a novel two-dimensional material discovery has aroused great attention. Because of these new 2D layered materials with different band gap size, which can be divided into insulators, semiconductors and Semimetals. These new materials are two-dimensional with excellent characteristics and disadvantages of each other. Fortunately, the two-dimensional material heterogeneity and convenient node development and assembly technology, the two-dimensional material and each make up for lack of advantage. Can the formation of heterojunction two-dimensional materials through arbitrary stacking sequence different. Thus we can use of a heterojunction Some basic physics and device performance. So that people can obtain the significant breakthrough in the research of artificial material structure. Graphene has a linear dispersion relation, massless Dirac fermions, high mobility and band gap properties. More importantly graphene has relatively strong light absorption, absorption and a single atomic layer 2.3% the number of independent. These excellent physical properties make graphene materials in optical detection especially light detection and high frequency infrared device has good application prospects. The recently discovered black phosphorus (b-P) and black arsenic phosphorus (b-AsP) alloy blocks the band gap in the 0.3-0.1 electron volts, and the crystal structure of black phosphorus low symmetry with strong anisotropy and polarization angle of polarized light sensitive dependence. In addition is a two-dimensional black phosphorus p- type semiconductor material, with high hole mobility, the black phosphorus is mid infrared light detection The ideal material and polarized light sensitive detection. However, the present study of transition metal chalcogenides widely, because of its moderate band gap main photoelectric response band in the visible band and near infrared band, but also has a strong interaction of light and matter transition metal chalcogenides, larger than the switch and the nature relatively stable. It could be used for the next generation of new logic devices and optoelectronic devices. People find a lot of interesting physical phenomena and potential application value in TMDs. Boron nitride has a larger band gap to 6 eV, corresponding to the deep ultraviolet band, belongs to two-dimensional insulator materials, substrate having better dielectric properties and the atomic level, is a good protective layer of other two-dimensional semiconductor material, can obtain higher shielding scattering electron mobility. With the in-depth study, there are two more dimensional materials Wait for our study found that the nature of the need for the development and utilization of more excellent people better service. This thesis mainly studies the two-dimensional heterostructure materials and photoelectric detection, through the design and fabrication of heterojunction devices, to achieve the overall performance of the new light detection function and improve detector. Currently the most widely studied two-dimensional semiconductor material is mainly transition metal chalcogenides, because the sulfur vacancy is easy to form, which is easy to realize the electron doped transition metal chalcogenides, so most of the n- type semiconductor material.P-n and bipolar junction with the built-in electric field is logic devices and high sensitive optical detection of the most basic needs. There are few p- the two-dimensional material doped transition metal chalcogenides, can form good matching with p-n junction structure, the realization of p- type doping is one of the key to be solved at present. High sensitivity photoelectric detection, p-n junction built-in electric field can effectively reduce the dark current and effective separation of photogenerated carriers. The production of high quality p-n is urgently needed in the field of photoelectric detection. We realize the regulation of the WSe2 carrier type by doping Ta. P- type two-dimensional semiconductor material is the key technology to realize the strong atomic layer thickness p-n. High quality p-n node is based on logic devices and photovoltaic detector. Through the design of p-g-n type heterojunction devices, wide band infrared detection, without band gap properties using graphene, wide band absorption. Usually in graphene photocarrier relatively short life span, the effective realization of fast separation two kinds of carriers can be built under the electric field. The spatial separation can effectively improve the carrier lifetime, while the built-in electric field can effectively reduce the dark current, thereby reducing the noise. Therefore p-g-n high Wide band sensitive photoelectric detection. Infrared in infrared detection has important application value in military and missile tracking. At present, MWIR detectors used to work at low temperature, need to increase the cost of using liquid nitrogen refrigeration, and harsh conditions not conducive to convenient use. There is an urgent need to develop and research the medium wave infrared detector at room temperature is convenient application of narrow band gap b-AsP FET and b-AsP-MoS2 heterojunction high sensitive infrared detection at room temperature. In the narrow band gap of two-dimensional layered materials such as PtSe2 and devices used to do some exploration. In the third chapter, we first design a p-g-n type heterojunction wide band photodetector. With Raman (Raman), light the photoluminescence (PL), atomic force microscopy (AFM) and the quality of the film layers of samples and optical microscope were characterized by micro area fixed transfer technology, realize multi different Production quality node devices. With larger work function metals, such as palladium, platinum, gold, p- type doping control WSe2. The Fermi level pinning and strong MoS2 well formed p-n junction. The middle layer graphene without band gap can effectively extend the response bandwidth. At the same time heterogeneous p-g-n nodes can also use the high mobility of graphene as a transparent electrode, separate the carrier separation after. Through the design of the p-g-n heterojunction, we detect from the wide band 400nm-2400nm detection band at room temperature. The photoelectric response rate is as high as 4250AW-1, the ratio of detection up to 1015 Jones. these high sensitive optical detection of light can be realized current imaging, high resolution image is obtained. At the same time we also studied the photoelectric response mechanism, through the visible and near-infrared imaging devices that our current space, the light response is mainly from the p-g-n The junction electric field. In addition, the back gate bias voltage and modulation has better effect on photoelectric response. In the fourth chapter, we deeply study the narrow band gap, black arsenic phosphorus alloy high mobility (b-As0.83P0.17) field effect devices and black phosphorus arsenic alloy and molybdenum sulfide (b-Aso.83P0.17-MoS2) heterojunction device of medium wave infrared detection the mechanism of performance. Focus on b-As0.83P0.17 FET devices from visible to infrared photoelectric response, the photovoltaic effect is the main mechanism of infrared photoelectric detection. By doping in black phosphorus arsenic and arsenic in material composition regulation, black arsenic phosphorus samples with arsenic doped 83%. Through the sample absorption spectrum the study found that the band gap of b-As0.83Po.17 ~ 0.15 eV, detection wavelength optical absorption edge at 1250 cm-1. detection from visible to infrared 400 nm-8.05 um. we studied b-As0.83P0.17-M The photoelectric response of oS2 heterojunction heterojunction, effectively reduce the dark current. Also we study the noise spectrum in heterojunction devices, heterojunction device noise power ratio b-As0.83P0.17 FET noise power density is two orders of magnitude. This shows that the heterojunction device can effectively reduce the dark current and noise power, effectively improve the sensitivity of the device. At the same time, b-As0.83P0.17 samples with strong anisotropic electrical and photoelectric response, and polarization angle on polarized light sensitive dependence. We obtained b-AS0.83P0.17 field effect devices than the detection rate in the band 400 nm-8.05 um higher than 108 Jones. for heterojunction devices from 400 nm-4.3 um than the detection rate is higher than the 4.9 x 109 Jones. fifth new transition metal chalcogenides growth and exploration of narrow gap material synthesis mainly consists of the following parts, the Through the implementation of Ta doped, the intrinsic P- type WSe2; second, CVT synthesis of WSe2 nanowires; third, to explore the growth of synthesis of narrow band gap of low dimensional materials, including black phosphorus doped samples, CVT method and PtSe2 CVD method for growth of narrow band gap metal selenide platinum obtained by PtSe2. CVT WSe2 single crystals were grown by p- Ta doped, p- type with good conductive properties. Through the micro point preparation of transfer Ta0.01W0.99Se2-MoS2 heterostructure and Tao.01W0.99Se2-WSe2 homojunctions, these devices exhibit ideal diode performance, ideal factor rectification ratio reached 105. ~ 1, photoelectric response experiments prove that the heterojunction interface quality. Good cooperation in the group of new the two-dimensional material heterojunction ReS2-BN high sensitive weak light detector and WSe2-graphene heterojunction photodetectors exhibit good photoelectric response. In the last chapter, we sum up in front of the Some important results are discussed and analyzed for the progress and problems currently facing, and we hope that we can continue to push ahead with the unfinished work and make greater contributions to the research direction of two-dimensional material photoelectric detection.

【學(xué)位授予單位】：南京大學(xué)
【學(xué)位級(jí)別】：博士
【學(xué)位授予年份】：2017
【分類號(hào)】：TN15

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