Optimization of surface morphology to reduce the effect of grain boundaries

Optimization of surface morphology to reduce the effect of grain boundaries and contact resistance in small molecule based thin film transistors

Sarita Yadav, Pramod Kumar, and Subhasis Ghosh

Citation: Appl. Phys. Lett. 101, 193307 (2012); doi: 10.1063/1.4766913

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Optimization of surface morphology to reduce the effect of grain boundaries and contact resistance in small molecule based thin film transistors Sarita Y adav,Pramod Kumar,a)and Subhasis Ghosh b)

School of Physical Sciences,Jawaharlal Nehru University,New Delhi,India

(Received9July2012;accepted17October2012;published online9November2012)

Grain boundaries in organic thin?lm have been controlled by engineering the different growth

conditions in such a way that it reduces the contact resistance and enhances the carrier mobility in

p-type copper phthalocyanine and n-type copper hexadeca?uoro phthalocyanine based organic thin

?lm transistors.Reduced effect of grain boundary has been demonstrated by temperature dependence

of charge carrier mobility and other transport parameters.A correlation has been established between

contact resistance and certain thin?lm morphology,achieved by varying different growth

conditions.V C2012American Institute of Physics.[https://www.sodocs.net/doc/c910517271.html,/10.1063/1.4766913]

Organic thin?lm transistors(OTFTs)are of considerable interest because of their potential applications in low cost integrated circuits for a variety of large area electronic appli-cations and display backplanes.1,2Though,the performance of OTFTs becomes comparable to the amorphous silicon thin ?lm transistors,3but there are several issues needed to be addressed in small molecule based OTFTs.One important issue,which remains to be addressed with greater efforts,is the high contact resistance(R C)which directly affects the performance of OTFTs by limiting drain current.Essentially, the two interfaces,i.e.,gate dielectric/organic layer and metal electrodes/organic layer control the performance of OTFT. Compared to the large number of studies directed towards how to increase carrier mobilities by engineering organic/ gate dielectric interface,4–6only few investigations have been directed towards the effect of source/drain(S/D)electrodes/ organic interface7,8which predominantly decides the R C in OTFT.In contrast to inorganic counter parts,R C cannot be optimized with conventional processes such as semiconductor doping or metal alloying in OTFTs.The R C can be reduced intrinsically by reducing the carrier injection barrier arises due to the difference between work function of S/D electro-des and highest occupied molecular orbital(HOMO)or lowest unoccupied molecular orbital(LUMO)of organic semiconductors.By choosing an appropriate S/D electrode material that has a high work function close to the HOMO in case of p-type organic semiconductor or low work function close to LUMO in n-type organic semiconductor,carrier injection barrier,so R C,can be substantially reduced.It has been observed9that in spite of low injection barrier between S/D electrodes and organic layer,R C remains very high. Hence,there is a need to look into contact resistance problem intrinsically.In bottom contact OTFTs,the self assembled monolayer or UV/ozone10,11treatment of bottom contacts help in reduction of R C,and it has been shown that larger grain size is responsible for low R C,but it is not clear whether size of the grain or reduction in barrier energy between elec-trode and organic layer due to surface treatment or both are responsible for reduced R C.Masataka et al.12showed that at low gate voltages,the R C decreases as the active layer thick-ness increases,but at higher gate voltages R C increases as thickness increases.In top contact OTFTs,13–15it has been shown that reduction in trap concentration at organic/dielec-tric interface and enlargement of grains are both responsible for better performance of OTFTs and reduction in R C.But, again it is not very clear whether trap or size of grain or both are responsible for lowering the contact resistance.In view of all these studies,it appears that grain boundary plays impor-tant role on contact resistance,so it is imperative to investi-gate the role of surface morphology of organic thin?lm on the R C.

In the present study,we report that how the R C is con-trolled by engineering the growth conditions of organic layer.We have used OTFTs based on p-type copper phthalo-cyanine(CuPc)and n-type copper hexadeca?uoro phthalo-cyanine(F16CuPc)small molecule organic semiconductors. All organic layers for these devices were grown at extremely low deposition rate($0.1A? /s)to reduce the structural disor-der as far as possible,and growth temperature was varied to achieve different surface morphologies such that contact area between metal electrode and organic layer can be increased.Essentially,it has been attempted to reduce the R C simply by increasing the contact area between S/D metal electrode and organic layer.Generally,organic thin?lms are polycrystalline with isotropic grainy morphology which results in nonuniform interface between metal electrode and organic layer.If surface morphology can be engineered by varying growth conditions to achieve anisotropic large grains with fewer grain boundaries the interface would be uniform and thereby reduce the R C.

We have shown recently how to fabricate small mole-cule based OTFTs with reduced number of traps due to struc-tural disorders by varying different growth conditions for organic thin?lms.16,17High purity CuPc and F16CuPc procured from Sigma Aldrich,USA.The heavily doped Si wafers with300nm SiO2layer were used as transistor sub-strate.65nm thick CuPc or F16CuPc organic semiconductors were deposited on the substrate with a deposition rate of 0.1A? /s and at different substrate temperatures.Finally,Au was deposited on the organic layer to form the source and

a)Present address:Department of Electrical Engineering,Technion–Israel

Institute of Technology,Haifa32000,Israel.

b)Electronic mail:subhasis@mail.jnu.ac.in.

0003-6951/2012/101(19)/193307/4/$30.00V C2012American Institute of Physics

101,193307-1

APPLIED PHYSICS LETTERS101,193307(2012)

drain contacts.The devices have an identical channel width 3mm,but different channel lengths varying from10l m to 100l m.All depositions were done in oil free thermal evapo-ration system at base pressure of10à6mbar.The electrical characterizations of OTFTs were carried out in rough vacuum(10à2mbar)using Keithley sourcemeter,Keithley picoammeter,and Agilent voltage sources.The surface mor-phology of CuPc and F16CuPc?lms was studied with Park Systems XE70atomic force microscopy(AFM).

Fig.1shows the AFM images of CuPc and F16CuPc thin ?lms grown under different growth conditions.Enhanced elongation due to anisotropic growth can be observed in thin ?lm grown at higher substrate temperature(100 C)with slowest deposition rate of0.1A? /s,but at high deposition rate (insets of Fig.1)elongation becomes weaker.The AFM images also show that at relatively low substrate temperature (40 C),morphology shows polycrystalline pattern with grain size varying from40to60nm.The main effect of higher growth temperature and lower deposition rate is to increase the diffusion length of molecules prior to their burial under the arriving?ux of molecules enhancing the migration and rotation of grains or clusters.This leads to coalescence of grains that have the lowest surface energy,resulting in improved crystallinity and less grain boundaries.

The effects of R C on OTFTs are more pronounced in linear region compared to saturation region.The electrical characteristics of OTFTs with various channel length(L)is analyzed by the transmission line method(TLM).In the linear region,the OTFT ON resistance(R ON)can be given by18

R ON?R chtR C?

L

W l C OXeV GSàV TT

tR C;(1)

where C OX is the insulator capacitance per unit area, V GS and V T are the gate voltage and threshold voltage,respectively,and R ch is the channel resistance which scales with channel length,whereas R C does not scale with channel length,and l is the channel mobility.The R C was evaluated at L?0by interpolating linear plot of R ON vs.L.Insets of Fig.2show the width normalized device resistance as a function of channel length of CuPc and F16CuPc based tran-sistors in which organic thin?lm were grown at substrate temperature40 C,and the R CáW of CuPc and F16CuPc based OTFTs are$0.11M X cm and$17.7M X cm at the gate voltage of60V,respectively.It is to be noted that inter-section point does not lie on x-axis but shifted by a distance L0.Similar behavior has been observed in amorphous silicon based TFTs.19,20The L0,which is usually negative and caused by the formation of insulating layer at S/D contact during processing or by imperfections introduced during device fabrication such as processing and reduction of the mask dimension.18,19L0is around0.5l m and6l m in CuPc and F16CuPc based OTFTs,respectively.It has been shown that existence of L0makes carrier mobility and V T depend on the channel length,causing ambiguity in the determina-tion of R C from R ON vs.L plots.Kanicki et al.19proposed that to scale out the dependence of carrier mobility and V T on L,Eq.(1)has to be modi?ed by normalizing with width of the channel W and replacing L with LtL0.

R ON:W?

LtL0

OX GS T

teR C:WT0:(2)

Equations(1)and(2)result in

R C:W?

L0

l C OXeV GSàV TT

teR C:WT0:(3)

Now R C has two components,i.e.,a gate voltage inde-pendent term(R CáW)0and another gate voltage

dependent FIG.1.Molecular structure of CuPc and

F16CuPc and1?1l m2AFM images of (a),(b)CuPc and(c),(d)F16CuPc?lms with the thickness of65nm deposited on

SiO2/Si substrate at two different substrate temperatures with deposition rate0.1 ?A/s. The organic thin?lms of(a)CuPc and(c) F16CuPc grown at substrate temperature 40 C consists of isotropic grains.At sub-strate temperature100 C elongated rod like structure has been observed in both(b) CuPc and(d)F16CuPc thin?lms.Insets of (b)and(d)show the AFM images of the CuPc and F16CuPc thin?lms grown at 100 C,but at higher deposition rate of 10 ?A/s.

term.(R CáW)0associated with the hole or electron injection barrier,and the gate voltage dependent term depends on the contact area between S/D metal electrode and organic layer.

R ONáW vs L plot of CuPc and F16CuPc based OTFT in which organic layer were grown at100 C are shown in Fig.2.The R CáW of CuPc based OTFT in which thin?lm grown at100 C is$16K X cm at the gate voltage of60V is about seven times lower than that of OTFT in which thin ?lm was grown at40 C.R CáW of F16CuPc based OTFTs in which thin?lm grown at100 C is740K X cm which is two order less that in F16CuPc based OTFT in which organic layer was grown at40 C.This implies that the contact resistance depends strongly on surface morphology.More importantly, it has been found that L0does not exist in CuPc based OTFT (Fig.2(a)),and in F16CuPc based OTFTs,L0is substantially reduced to3l m from6l m.The HOMO of CuPc is close to the work function of Au electrode;hence,hole injection from Au in CuPc faces no barrier,whereas in F16CuPc based OTFT,electron injection from Au faces small barrier of 0.3eV,so the contact resistance in F16CuPc based OTFTs is higher than that in CuPc based OTFTs.Experimental data show that R C values are always low in OTFTs which were fabricated at higher substrate temperatures.This infers that at higher substrate temperature anisotropic large grains with fewer grain boundary form a uniform interface between metal electrode and organic layer.The absence of L0indicates bet-ter contact area formed between S/D electrodes and organic layer and reduction of interface imperfection in organic layers grown at higher temperatures.

To corroborate the role of grain boundaries on R C and other relevant transport parameters,we have studied the effect of grain boundaries on the carrier mobility in OTFT. The charge transport in organic transistors occurs via hop-ping through the localized states which results thermally activated mobility.Fig.3shows the temperature dependence of?eld effect mobility in CuPc and F16CuPc based OTFTs. The Arrhenius plots of temperature dependence of carrier mobility in OTFTs fabricated on organic layers grown at 40 C have two slopes with two activation energies(E1*and E2)indicating two different transport processes,whereas Arrhenius plots for OTFTs in which organic thin?lm were grown at100 C show single slope with single activation energy(E1),indicating single transport process over entire range of temperature.It has been shown21the activation energy at higher temperature is due to hopping transport and the activation energy at lower temperature is due to grain boundary between either two grains or https://www.sodocs.net/doc/c910517271.html,anic thin ?lms of CuPc and F16CuPc grown at40 C have polycrystal-line grainy morphology.The interface states between grain boundaries give rise to localized energy levels inside the band gap of the semiconductor.The trapped charges at the grain boundary interface lead the formation of a potential barrier for all transport process.In case of OTFTs fabricated on organic layers grown at40 C,we have observed E1*$0.14eV and0.11eV for300>T>210K and E2$0.07eV and0.08eV for210K>T>120K in CuPc and F16CuPc,https://www.sodocs.net/doc/c910517271.html,anic?lms grown on higher

FIG.2.Width normalized total resistance(R ONáW)as a function of channel

length(L)at gate voltages ofà40V(triangle),à50V(square)andà60V

(circle)for(a)CuPc and at gate voltages of60V(triangle),70V(square),

80V(circle)for(b)F16CuPc based OTFT in which organic thin?lms were

grown at100 C.Insets show the data of OTFT in which organic thin?lms

were grown at40 C.L0is shown by horizontal arrow.

FIG.3.Arrhenius plots of the dependence of mobility l on temperature

obtained from I DS-V DS characteristics in the linear region for(a)CuPc and

(b)F16CuPc based OTFT at V GS?80V.Arrows indicate the increase of

room temperature mobility by one order in CuPc and two orders in F16CuPc

based OTFT as the substrate temperature is changed from40 C to100 C.

Arrhenius plots show two slopes with activation energies E*1and E2and

single slope with activation energy E1in organic?lms grown at40 C and

100 C,respectively.

substrate temperature(100 C)have rod like lamellar struc-ture which reduces substantially the grain boundaries,so at low temperature the grain boundary effect is negligible,and charge transport is only thermally activated with activation energy E1$0.12eV and0.09eV in CuPc and F16CuPc, respectively.We have observed that the activation energies for hopping transport are marginally different in CuPc or F16CuPc thin?lms grown under different conditions. For example,activation energies are E1$0.12eV and E1*$0.14eV in CuPc OTFTs fabricated on thin?lms grown at100 C and40 C,respectively,and those values for F16CuPc are E1$0.09eV and E1*$0.11eV.This change in activation energies in same material is caused by the reduc-tion in carrier concentration due to trapping at grain boundary interfaces in samples with grainy polycrystalline surface mor-phology created by growing thin?lms at lower temperature. As carrier concentration decreases,Fermi level(E F)shifts to lower energy states in HOMO(CuPc)or LUMO(F16CuPc) distancing itself from transport energy(E t),so the activation energy for hopping transport which is the difference22 between E t and E F increases compared to that in samples which were grown in such a way to have surface morphology with reduced number of grain boundaries.Table I summa-rizes the how different device parameters are improved with growth temperature.

In conclusions,we have shown that by engineering the growth conditions of organic thin?lm,the performance of OTFTs can be improved,in particular,the contact resistance can be reduced substantially.At higher substrate temperature and low deposition rate,the surface morphologies of organic thin?lms have been optimized in such a way to have aniso-tropic elongated grains with sizes much larger than the iso-tropic grains commonly observed in polycrystalline organic thin?lms.The typical surface morphology due to anisotropic growth increases the effective contact area between source/ drain electrodes and organic layer resulting reduction in con-tact resistance and the effects of traps at grain boundaries to enhance the transport processes in OTFTs.

S.Y.and P.K.thank Council of Scienti?c&Industrial Research,India for the?nancial support through fellowship. This work was partly supported by DST,Government of India.

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TABLE I.Device parameters of CuPc and F16CuPc based OTFTs in which active layers were grown at different temperatures.

Growth temperature( C)

l

(cm2Và1sà1)V th(V)

R CáW

(M X cm)

(R CáW)0

(M X cm)

CuPc40 1.2?10à3à6.80.1140.054 1001?10à2à5.30.0160.009 F16CuPc40 6.0?10à42417.77 5.308 100 2.0?10à2170.740.256

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英语语言学试题（5） 一、单项选择题(在每小题的四个备选答案中，选出一个正确答案，并将正确答案的序号填在题干的括号内。每小题2分，共20分) 1.The description of a language as it changes through time is a ( ) s tudy. A. comparative B. diachronic C. up-to-date D. descriptive 2. Of the three branches of phonetics, the longest established, and until recently the most highly developed, is ( ) phonetics. A. auditory B. acoustic C. articulatory D. none of the above three 3. What the element …-es? indicates is third person singular, present tens e, the element …-ed? past tense, and …-ing? progressive aspect. Since they are the smallest unit of language and meaningful, they are also ( ). A. phonemes B. morphemes C. allophones D. phones 4. Since early 1980s Noam Chomsky and other generatvie linguists prop osed and developed a theory of universal grammar known as the ( ) theory. A. speech act B. TG C. principles-and-parameters D. minimalist programme 5. One way to analyze lexical meaning is ( ). A. predication analysis B. stylistic analysis C. componential analysis D. proposition analysis 6. Of the three speech acts, linguists are most interested in the ( ) b ecause this kind of speech act is identical with the speaker?s intention. A. locutionary act B. illocutionary act C. perlocutionary act D. constative act 7. The discovery of Indo-European language family began with the work of the British scholar ( ). A. Sir William Jones B. John Firth C. M. A. K. Halliday D. F. D. Saussure 8. A bilingual speaker often uses two languages alternatively during a co nversation with another bilingual speaker, a speech situation known as

语言学纲要习题答案

导言 一,名词解释(分,每小题分) ,研究语言的本质,语言的结构和发展规律. .指我国传统的语文学,包括文字学,音韵学,训诂学三方面的内容. ,个别语言学,以一种(或几种有联系的)语言为研究对象,研究某一种语言的结构. ,静态分析的方法,研究语言相对静止的状态,描写分析语言在某一个时期,某一个阶段的状况,是从横向的方面研究语言. ,动态的角度研究语言发展的历史,观察一种语言的各个结构要素在不同发展阶段的历史演变,是从纵向的方面研究语言的历史. ,探讨人类语言的共同规律,是在具体语言学基础上建立起来的,下面又分普通语音学,普通语法学,普通词汇学等分支学科. 二,填空题(分,每空分) .中国印度古希腊罗马 .文字学音韵学训诂学 .语音词汇和语义语法 .编码发送传递接收 .历时共时历史描写 .历史比较 .《语言论》 .索绪尔 三,问答题(分,每小题分) ①研究对象不同:古代的语言学主要以书面语为主要研究材料,不重视口头语言的研究,而今天的语言学则十分重视口语研究,如制定语言规范,确立共同语的各方面标准等,都要依据口语的研究成果; ②研究目的不同:古代语言学研究语言,主要是给政治,哲学,宗教,历史,文学方面的经典著作作注解,比如我国古代的语文学主要就是围绕阅读先秦经典著作的需要来研究文言的,而现代语言学的研究目的主要是分析语言的结构,以此探讨语言发展的共同规律. 正因为有这些差别,所以古代的语言学还不是独立的学科,处于附庸地位,而现代语言学已经发展成为一门独立的学科,随着现代科学的发展又产生了许多边沿性学科. 人类语言交际的过程,实际上就是信息的传递与接收问题,可分为编码,发送,传递,接收,解码五个阶段.编码就是发话人利用词语组织语句;发送就是把思维成果变成话语,通过发音器官表达出来;传递就是通过空气振动形成声波,把话语传达给受话人;接收是受话人利用听觉器官感知对方所说的话;解码则经过大脑的思维把声波还原成语言,理解对方话语的含义,从而完成信息传递接收.如果受话人收到语言信息有所反馈,那么上述五个阶段则又重复一遍,只是发话人与受话人调换了. (举例说明略,可结合分析任举一个句子作说明.) 语言是伴随着人类一起出现的,是人类社会生活必不可少的,所以人类很早就注意到了语言的重要性,很早就注意研究语言,所以语言学是古老的,但语言学直到世纪下半叶,产生了历史比较语言学,后来又建立了语言学的各个部门,语言研究才发展成为一门独立的学科,同其它学科相比,语言学的确是十分年轻的.语言是社会现象,与社会的政治,经济,文化,历史等密切相关,而语言的发生又与物理,生理,心理等学科密切相关,而现代社会语言与语言的信息处理(如机器翻译,语码转换等)又涉及到数学,计算机科学,所以语言学既与社会科学有密切的联系,又与自然科学有密切的联系.正因为如此,随着语言学与别的学科的交融,又产生了许多新的语言学分支学科,如社会语言学,心理语言学,统计语言学,话语语言学,数理语言学,宇宙语言学等等,这些也体现了语言学是一门年轻的学科. 语言学的作用主要表现在以下几个方面:①学习语言文字是掌握科学技术,提高文化水平的基础,而要学好用好语言,就必须利用语言学的研究成果;②制定语言文字的有关政策,制定语言规范,都要在对语言进行充分研究的基础上进行,而语言学的研究成果正好可以作指导;③新兴技术的出现扩大了语言学的应用范围.至于个人,同样可以利用语言学的成果,比如学习一种语言或方言,最好的办法是找到所学语言同自己母语的各方面的对应规律,这样可以收到事半功倍的效果,这就需要利用语言学的研究成果. (结合实际部分可以根据自己的学习,工作或生活经历举例) 语言学首先可以分为理论语言学和应用语言学,一般所说的语言学,主要是指理论语言学.根据研究对象的不同,理论语言学又分普通语言学和专语语言学(具体语言学).普通语言学以人类所有的语言为研究对象,探讨人类语言的共同规律,是在具体语言学基础上建立起来的,下面又分普通语音学,普通语法学,普通词汇学等分支学科.专语语言学以个别的,具体的语言为研究对象.探讨研究某一种语言的规律.从是静态研究还是研究语言的历史看,又分历时语言学和共时语言学:历时语言学研究具体语言的发展历史,是纵向研究,比如汉语史研究,共时语言学研究具体语言在某一时代的状态(相对静止的状态),规律,对之进行客观的描述,是横向研究.如描写语言学,又分描写语音学,描写语汇学,描写语法学等分支学科,现代汉语就是共时语言学. .在历史语言学产生以前,语言学