Low-energy electronic structure in Y1-xCaxBa2Cu3O7-y comparison of t ime-resolved optical s
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Exploring Chemistry with Electronic Structure MethodSecond EdithionJames B. ForesmanAeleen FrischGaussian, IncPittsburgh, PA2002年9月25日特别声明本文转自南开大学BBS,在此对译者表示衷心感!!!!用Gaussian研究化学问题说明接触Gaussian已经很久了,但真正用Gaussian做东西还是临近博士毕业时的事情。
当时做计算的时候,就特别希望有一本具体怎么使用从头算的书,可惜一直没有找到。
来到这里后,在新买的Gaussian98包中发现了这本书,感觉如获至宝,也希望能够提供应想用Gaussian做东西的朋友。
我不是专门做量化的,很多术语不清楚怎么翻译,手头又没有中文的资料,错误的地方,只能希望行来指点了。
其实这本书里面介绍的东西,不止限于Gaussian 程序的。
对于从事从头算研究的都有帮助。
容中有很多计算实例,都是在Gaussian94,98程序中提供的。
节译自Exploring Chemistry with Electronic Structure Methos,SecondEdition,作者James B。
Foresman,Eleen FrischGaussian,Inc,USA,1996目录特别声明1用Gaussian研究化学问题1说明1前言1运行Gaussian2Unix/Linux平台2Windows平台2输出文件2第一章计算模型31.1 计算化学概述3分子力学理论3电子结构理论4密度泛函(Density Functional Methods)41.2 化学模型(Model Chemistries)4定义化学模型4模型的组合5第二章单点能计算52.1 能量计算设置5路径5计算的名称6分子结构6多步计算62.3 输出文件中的信息6标准几何坐标。
6能量6分子轨道和轨道能级6电荷分布7偶极矩和多极矩7CPU时间和其他72.4 核磁计算7第三章几何优化93.1 势能面93.2 寻找极小值9收敛标准10几何优化的输入10检查优化输出文件103.3 寻找过渡态103.4 难处理的优化11第四章频率分析134.1 预测红外和拉曼光谱13频率计算的输入13频率和强度13矫正因子和零点能。
aufbau principle英语解释The Aufbau Principle, also known as the building-up principle, is a fundamental concept in chemistry that explains the order in which electrons fill atomic orbitals. This principle is essential for understanding the electronic structure of atoms and predicting their chemical properties. It is based on the idea that electrons occupy the lowest energy levels available to them before filling higher energy levels.The Aufbau Principle is a key component of the periodic table, which organizes elements based on their atomic number and electronic configurations. It helps chemists predict the behavior of elements and their compounds, as well as understand trends in their properties across the periodic table.At its core, the Aufbau Principle states that electrons fill atomic orbitals in order of increasing energy. The energy levels of atomic orbitals are determined by their principal quantum number, which corresponds to the size and energy of the orbital. The four quantum numbers (n, l, ml, and ms) define the characteristics of the orbital and the spin of the electron.The order in which electrons fill atomic orbitals is based on the relative energies of the s, p, d, and f orbitals. The s orbitalsare the lowest energy orbitals, followed by the p orbitals, then the d orbitals, and finally the f orbitals. Within each type of orbital, the Aufbau Principle dictates that electrons fill the orbitals in a specific order.For example, in the ground state electron configuration of hydrogen (H), there is one electron in the 1s orbital. The next element, helium (He), has two electrons filling the 1s orbital. As we move down the periodic table to lithium (Li) and beryllium (Be), the electrons begin to fill the 2s orbital before moving on to the 2p orbitals in boron (B) and carbon (C).The Aufbau Principle also explains the exceptions to the order of filling orbitals. For example, transition metals have partially filled d orbitals, which can lead to variations in electron configurations. Additionally, some elements exhibit anomalies in their electron configurations due to the stability associated with having a half-filled or fully filled subshell.In summary, the Aufbau Principle is a foundational concept in chemistry that describes the order in which electrons fill atomic orbitals. It is crucial for understanding the electronic structure of elements and predicting their chemical properties. By following the Aufbau Principle, chemists can predict thearrangement of electrons in atoms and deduce the behavior of elements in chemical reactions.。
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关于科学的英语演讲稿关于科学的英语演讲稿the presence of students, ladies and teachers, everyone! i was prepared intervals of cloud today, in honor here entitled “technology and future” speech, i am very proud of both, but some unease. in recent years, we have seen our great motherland, the cause of the rapid development of technology, which allow me to a chinese i feel very proud. remember that long ago, cell phone use almost the only one, which is called, but a few years ago, cell phones has undergone great changes, not only look more beautiful, but also use more, you can use the phones to take pictures, meetings, internet, text messages, etc. a series of things that i their life more convenient, so i am more aware of the strength of the technology, but i am just a fledgling s students, “technology” as the word also aware of the limited, i am unable to use some very difficult theory to elaborate technology xuanji, no right to work on their elders i can promise of the technology blueprint. but i am willing to use a student’s perspective to the imagine technology and the future.from genetic engineering “is a live princes” dream, nano-technology “- not washing your clothing,” promises; fromartificial intelligence “will give you a cute robot dog” warm, transgenic technology “let people grow mouse ears” wonders. the new technology in the birth of a new technology that will let people wild with joy, because these new technologies is gradually improving our lives, let us learn more about ourselves. in the near term, china completed its first sars virus genome sequencing, sars is now the world’s largest recognized the dangers of the disease, but why not other countries completed first, and we just completed the countries? very si-mp-le, this illustrates that our country backward than others, worse than others, we look at the past, had just started a country’s reform and opening up to the current level of science and technology has lead a large country, our motherland experienced a number of ups and downs, how many difficulties and bumpy however, we still back all of the motherland, the motherland because we firmly believe that - not only technological change destiny, can change the future.for our generation, the general feeling of the community is a strong sense of competition, learning a foot down. science knowledge is the focus of our attention, albert einstein, and stephen hawking, bill gates is the star we have in mind, computer science, physics and chemistry of modern dynamic is constantly affect us. we have to understand theimportance of technology, know that the technology universal.although technology to create a new life prospects soliciting thoughts, inspiring. however, the final analysis is that we rely on our common efforts to realize. , as the future construction of the backbone of our generation of young people shoulders the burden is not light, new opportunities are always accompanied risks and challenges, but we will not give up that easily, we use our youth to predecessors vowed: never live up to their predecessors of our hope.looking back at the history of civilization, anderson is the history of mankind against the darkness of ignorance, is the scientific lit a fire in the raging human soul of hope; technology support civilization, science and technology to create the future, but the future is in our hands. let us become knowledge explorers, let us unknown roaming on the road, let me use our creativity to the world we live a better place.参考翻译:在场的学生们,女士们,老师,大家好!我准备间隔云今天,为了纪念在这里题为“科技与未来”的讲话,我感到非常自豪的两个,但有些不安。
数字电路瞬态故障低能耗自修复方法司慧玲【摘要】当前大多数字电路瞬态故障修复方法需在人工处理下才可完成,修复效率低且能耗高.为此,提出一种新的数字电路瞬态故障低能耗自修复方法.设计了一种修复系统,其主要由自律控制模块与重配置执行模块构成,自律控制模块的核心是嵌入式NiosⅡ处理器.数字电路在出现瞬态故障的情况下,通过小波神经网络算法对数字电路瞬态故障进行诊断,判断电路是否正常运行.重配置执行模块包括逻辑计算节点LC与内部互联网络,主要作用是维持数字电路功能以及与其他模块之间施行信息传递.实验结果表明,所提方法能够有效诊断故障,故障修复成功率和平均适应度高,整体性能强.%At present,most of the digital circuit transient fault repair methods need to be completed by manual processing,the repair efficiency is low and the energy consumption is high.For this,a new kind of digital circuit fault transient low energy self repair method was put forward,design a repair system,which is mainly composed of self reconfiguration control module and execution module, self-discipline of the core control module is embedded Nios processor,digital circuit in the presence of transient fault.The wavelet neural network algorithm the diagnosis of digital circuit transient fault judging circuit,whether the normal operation of.The reconfiguration execution mod-ule consists of a logical computing node LC and an internal interconnection network.The main function is to main-tain the function of the digital circuit and carry out the information transmission between the other modules.The ex-perimental results show that the proposed method can effectively diagnose the fault,the successrate and the average fitness of the fault repair are high,and the overall performance is strong.【期刊名称】《科学技术与工程》【年(卷),期】2017(017)030【总页数】6页(P257-262)【关键词】数字电路;瞬态故障;低能耗;自修复【作者】司慧玲【作者单位】郑州工业应用技术学院机电工程学院,郑州451100【正文语种】中文【中图分类】TP331.2;TM932目前数字电路已经在不同产品上被广泛使用,在使用的过程中数字电路往往会出现一些瞬态故障,导致产品不能正常工作[1,2]。
ARTICLEReceived1Apr2014|Accepted9Jan2015|Published24Feb2015Observation of long-lived interlayer excitonsin monolayer MoSe2–WSe2heterostructuresPasqual Rivera1,John R.Schaibley1,Aaron M.Jones1,Jason S.Ross2,Sanfeng Wu1,Grant Aivazian1,Philip Klement1,Kyle Seyler1,Genevieve Clark2,Nirmal J.Ghimire3,4,Jiaqiang Yan4,5,D.G.Mandrus3,4,5, Wang Yao6&Xiaodong Xu1,2Van der Waals bound heterostructures constructed with two-dimensional materials,such asgraphene,boron nitride and transition metal dichalcogenides,have sparked wide interest indevice physics and technologies at the two-dimensional limit.One highly coveted hetero-structure is that of differing monolayer transition metal dichalcogenides with type-II bandalignment,with bound electrons and holes localized in individual monolayers,that is,interlayer excitons.Here,we report the observation of interlayer excitons in monolayerMoSe2–WSe2heterostructures by photoluminescence and photoluminescence excitationspectroscopy.Wefind that their energy and luminescence intensity are highly tunable by anapplied vertical gate voltage.Moreover,we measure an interlayer exciton lifetime of B1.8ns,an order of magnitude longer than intralayer excitons in monolayers.Our work demonstratesoptical pumping of interlayer electric polarization,which may provoke further explorationof interlayer exciton condensation,as well as new applications in two-dimensional lasers,light-emitting diodes and photovoltaic devices.1Department of Physics,University of Washington,Seattle,Washington98195,USA.2Department of Materials Science and Engineering,University of Washington,Seattle,Washington98195,USA.3Department of Physics and Astronomy,University of T ennessee,Knoxville,T ennessee37996,USA.4Materials Science and T echnology Division,Oak Ridge National Laboratory,Oak Ridge,T ennessee37831,USA.5Department of Materials Science and Engineering,University of T ennessee,Knoxville,T ennessee37996,USA.6Department of Physics and Center of Theoretical and Computational Physics, University of Hong Kong,Hong Kong,China.Correspondence and requests for materials should be addressed to P.R.(email:pasqual@)or to X.X. (email:xuxd@).T he recently developed ability to vertically assemble different two-dimensional(2D)materials heralds a newrealm of device physics based on van der Waals heterostructures(HSs)1.The most successful example to date is the vertical integration of graphene on boron nitride.Such novel HSs not only markedly enhance graphene’s electronic properties2, but also give rise to superlattice structures demonstrating exotic physical phenomena3–5.A fascinating counterpart to gapless graphene is a class of monolayer direct bandgap semiconductors, namely transition metal dichalcogenides(TMDs)6–8.Due to the large binding energy in these2D semiconductors,excitons dominate the optical response,exhibiting strong light–matter interactions that are electrically tunable9,10.The discovery of excitonic valley physics11–15and strongly coupled spin and pseudospin physics16,17in2D TMDs opens up new possibilities for device concepts not possible in other material systems. Monolayer TMDs have the chemical formula MX2where the M is tungsten(W)or molybdenum(Mo),and the X is sulfur(S) or selenium(Se).Although these TMDs share the same crystalline structure,their physical properties,such as bandgap,exciton resonance and spin–orbit coupling strength,can vary signifi-cantly.Therefore,an intriguing possibility is to stack different TMD monolayers on top of one another to form2D HSs.First-principle calculations show that heterojunctions formed between monolayer tungsten and molybdenum dichalcogenides have type-II band alignment18–20.Recently,this has been confirmed by X-ray photoelectron spectroscopy and scanning tunnelling spectroscopy21.Since the Coulomb binding energy in2D TMDs is much stronger than in conventional semiconductors, it is possible to realize interlayer excitonic states in van der Waals bound heterobilayers,that is,bound electrons and holes that are localized in different layers.Such interlayer excitons have been intensely pursued in bilayer graphene for possible exciton condensation22,but direct optical observation demonstrating the existence of such excitons is challenging owing to the lack of a sizable bandgap in graphene.Monolayer TMDs with bandgaps in the visible range provide the opportunity to optically pump interlayer excitons,which can be directly observed through photoluminescence(PL)measurements.In this report,we present direct observation of interlayer excitons in vertically stacked monolayer MoSe2–WSe2HSs.We show that interlayer exciton PL is enhanced under optical excitation resonant with the intralayer excitons in isolated monolayers,consistent with the interlayer charge transfer resulting from the underlying type-II band structure.We demonstrate the tuning of the interlayer exciton energy by applying a vertical gate voltage,which is consistent with the permanent out-of-plane electric dipole nature of interlayer excitons.Moreover,wefind a blue shift in PL energy at increasing excitation power,a hallmark of repulsive dipole–dipole interac-tions between spatially indirect excitons.Finally,time-resolved PL measurements yield a lifetime of1.8ns,which is at least an order of magnitude longer than that of intralayer excitons.Our work shows that monolayer semiconducting HSs are a promising platform for exploring new optoelectronic phenomena.ResultsMoSe2–WSe2HS photoluminescence.HSs are prepared by standard polymethyl methacrylate(PMMA)transfer techniques using mechanically exfoliated monolayers of WSe2and MoSe2(see Methods).Since there is no effort made to match the crystal lattices of the two monolayers,the obtained HSs are considered incom-mensurate.An idealized depiction of the vertical MoSe2–WSe2HS is shown in Fig.1a.We have fabricated six devices that all show similar results as those reported below.The data presented here are from two independent MoSe2–WSe2HSs,labelled device1and device2.Figure1b shows an optical micrograph of device1,which has individual monolayers,as well as a large area of vertically stacked HS.This device architecture allows for the comparison of the excitonic spectrum of individual monolayers with that of the HS region,allowing for a controlled identification of spectral changes resulting from interlayer coupling.We characterize the MoSe2–WSe2monolayers and HS using PL measurements.Inspection of the PL from the HS at room temperature reveals three dominant spectral features(Fig.1c). The emission at1.65and1.57eV corresponds to the excitonic states from monolayer WSe2and MoSe2(refs10,15),respectively. PL from the HS region,outlined by the dashed white line in Fig.1a,reveals a distinct spectral feature at1.35eV(X I).Two-dimensional mapping of the spectrally integrated PL from X I shows that it is isolated entirely to the HS region(inset,Fig.1c), with highly uniform peak intensity and spectral position (Supplementary Materials1).Low-temperature characterization of the HS is performed with 1.88eV laser excitation at20K.PL from individual monolayer WSe2(top),MoSe2(bottom)and the HS area(middle)are shown with the same scale in Fig.1d.At low temperature,the intralayer neutral(X M o)and charged(X MÀ)excitons are resolved10,15,where M labels either W or parison of the three spectra shows that both intralayer X M o and X MÀexist in the HS with emission at the same energy as from isolated monolayers,demonstrating the preservation of intralayer excitons in the HS region.PL from X I becomes more pronounced and is comparable to the intralayer excitons at low temperature.We note that the X I energy position has variation across the pool of HS samples we have studied (Supplementary Fig.1),which we attribute to differences in the interlayer separation,possibly due to imperfect transfer and a different twisting angle between monolayers.We further perform PL excitation(PLE)spectroscopy to investigate the correlation between X I and intralayer excitons.A narrow bandwidth(o50kHz)frequency tunable laser is swept across the energy resonances of intralayer excitons(from1.6to 1.75eV)while monitoring X I PL response.Figure2a shows an intensity plot of X I emission as a function of photoexcitation energy from device2.We clearly observe the enhancement of X I emission when the excitation energy is resonant with intralayer exciton states(Fig.2b).Now we discuss the origin of X I.Since X I has never been observed in our exfoliated monolayer and bilayer samples,if its origin were related to defects,they must be introduced by the fabrication process.This would result in sample-dependent X I properties with non-uniform spatial dependence.However,our data show that key physical properties of X I,such as the resonance energy and intensity,are spatially uniform and isolated to the HS region(inset of Fig.1c and Supplementary Fig.2).In addition,X I has not been observed in WSe2–WSe2homo-structures constructed from exfoliated or physical vapor deposi-tion(PVD)grown monolayers(Supplementary Fig.3).All these facts suggest that X I is not a defect-related exciton.Instead,the experimental results support the observation of an interlayer exciton.Due to the type-II band alignment of the MoSe2–WSe2HS18–20,as shown in Fig.2c,photoexcited electrons and holes will relax(dashed lines)to the conduction band edge of MoSe2and the valence band edge of WSe2,respectively.The Coulomb attraction between electrons in the MoSe2and holes in the WSe2gives rise to an interlayer exciton,X I,analogous to spatially indirect excitons in coupled quantum wells.The interlayer coupling yields the lowest energy bright exciton in the HS,which is consistent with the temperature dependence of X I PL,that is,it increases as temperature decreases (Supplementary Fig.4).From the intralayer and interlayer exciton spectral positions,we can infer the band offsets between the WSe 2and MoSe 2monolayers (Fig.2c).The energy difference between X W and X I at room temperature is 310meV.Considering the smaller binding energy of interlayer than intralayer excitons,this sets a lower bound on the conduction band offset.The energy difference between X M and X I then provides a lower bound on the valence band offset of 230meV.This value is consistent with the valence band offset of 228meV found in MoS 2–WSe 2HSs by micro X-ray photoelectron spectroscopy and scanning tunnelling spectro-scopy measurements 21.This experimental evidence strongly corroborates X I as an interlayer exciton.The observation of bright interlayer excitons in monolayer semiconducting HSs is of central importance,and the remainder of this paper will focus on their physical properties resulting from their spatially indirect nature and the underlying type-II band alignment.WSe 2HSMoSe 2W M SeIn te n s i t y (a .u .)1.31.51.7Energy (eV)MoSe 2HeterostructureWSe 2W0WX X X X −0MoMo−e hehe h1.3 1.41.51.6 1.7I n t e n s i t y (a .u .)Energy (eV)5μm 0123×104Y (μm )246X (μm)0246Figure 1|Intralayer and interlayer excitons of a monolayer MoSe 2–WSe 2vertical heterostructure.(a )Cartoon depiction of a MoSe 2–WSe 2heterostructure (HS).(b )Microscope image of a MoSe 2–WSe 2HS (device 1)with a white dashed line outlining the HS region.(c )Room-temperature photoluminescence of the heterostructure under 20m W laser excitation at 2.33eV.Inset:spatial map of integrated PL intensity from the low-energy peak (1.273–1.400eV),which is only appreciable in the heterostructure area,outlined by the dashed black line.(d )Photoluminescence of individual monolayers and the HS at 20K under 20m W excitation at 1.88eV (plotted on the samescale).Energy (eV)WSe MoSe PL energy (eV)E x c i t a t i o n e n e r g y (e V )1.28 1.3 1.32 1.34 1.36 1.381.61.651.71.754,0006,0008,00010,000IntensityFigure 2|Photoluminescence excitation spectroscopy of the interlayer exciton at 20K.(a )PLE intensity plot of the heterostructure region with an excitation power of 30m W and 5s charge-coupled device CCD integration time.(b )Spectrally integrated PLE response (red dots)overlaid on PL (black line)with 100m W excitation at 1.88eV.(c )Type-II semiconductor band alignment diagram for the 2D MoSe 2–WSe 2heterojunction.interlayer exciton .Applying vertical energy of Figure 3a contact stacked insu-Electrostatic contact shows the 100to about analogue of reversed,varied expected for from reduces device 2,conduction 3b,c.of the in the on top band-offset at X I PL energy of basis of would should have X I PL This effect,intensity.further Power dependence and lifetime of interlayer exciton PL .The interlayer exciton PLE spectrum as a function of laser power with excitation energy in resonance with X W o reveals several properties of the X I .Inspection of the normalized PLE intensity (Fig.4a)shows the evolution of a doublet in the interlayer excitonspectrum,highlighted by the red and Both peaks of the doublet display a consistent increased laser intensity,shown by the dashed which are included as a guide to the eye.intensity of X I also exhibits a strong saturation laser power,as shown in Fig.4b (absolute Supplementary Fig.6).The sublinear power excitation powers above 0.5m W is distinctly the intralayer excitons in isolated monolayers,saturation power threshold of about Fig.7).The low power saturation of X I PL lifetime than that of intralayer excitons.the intralayer exciton is substantially reduced interlayer charge hopping 23,which is quenching of intralayer exciton PL (Fig.Fig.8).Moreover,the lifetime of the interlayer because it is the lowest energy configuration indirect nature leads to a reduced optical long lifetime is confirmed by time-resolved Fig.4c.A fit to a single exponential decay exciton lifetime of 1.8±0.3ns.This timescale the intralayer exciton lifetime,which is ps 24–27.By modelling the saturation behaviour three-level diagram,the calculated saturation interlayer exciton is about 180times (Supplementary Fig.7;Supplementary with our observation of low saturation intensity DiscussionWe attribute the observed doublet feature splitting of the monolayer MoSe 2conduction assignment is mainly based on the fact difference between the doublet is B 25with MoSe 2conduction band splitting predicted calculations 28.This explanation is also supported by the evolution of the relative strength of the two peaks with increasing excitation power,as shown in Fig.4a (similar results in device 1with 1.88eV excitation shown in Supplementary Fig.9).At low power,the lowest energy configuration of interlayer excitons,with the electron in the lower spin-split band of MoSe 2,is populated first.Due to phase space filling effects,the interlayer excitonSiO 2n + Si2MoSe 2e –h +e –h +P Ee –h +V g < 0WSe 2MoSe 2WSe 2MoSe 2h ωV g = 0Photon energy (eV)1.321.361.41.444080e –h +h +PL intensity (a.u.) -hω’-the interlayer exciton and band alignment.(a )Device 2geometry.The interlayer exciton has a out-of-plane electric polarization.(b )Electrostatic control of the band alignment and the interlayer exciton photoluminescence as a function of applied gate voltage under 70m W excitation at 1.744eV,1s integrationconfiguration with the electron in the higher energy spin-split band starts to be filled at higher laser power.Consequently,the higher energy peak of the doublet becomes more prominent at higher excitation powers.The observed blue shift of X I as the excitation power increases,indicated by the dashed arrows in Fig.4a,is a signature of the repulsive interaction between the dipole-aligned interlayer excitons (cf.Fig.3a).This is a hallmark of spatially indirect excitons in gallium arsenide (GaAs)coupled quantum wells,which have been intensely studied for exciton Bose-Einstein condensation (BEC)phenomena 29.The observation of spatially indirect interlayer excitons in a type-II semiconducting 2D HS provides an intriguing platform to explore exciton BEC,where the observed extended lifetimes and repulsive interactions are two key ingredients towards the realization of this exotic state of matter.Moreover,the extraordinarily high binding energy for excitons in this truly 2D system may provide for degenerate exciton gases at elevated temperatures compared with other material systems 30.The long-lived interlayer exciton may also lead to new optoelectronic applications,such as photovoltaics 31–34and 2D HS nanolasers.MethodsDevice fabrication .Monolayers of MoSe 2are mechanically exfoliated onto 300nm SiO 2on heavily doped Si wafers and monolayers of WSe 2onto a layer of PMMA atop polyvinyl alcohol on Si.Both monolayers are identified with an opticalmicroscope and confirmed by their PL spectra.Polyvinyl alcohol is dissolved in H 2O and the PMMA layer is then placed on a transfer loop or thin layer of poly-dimethylsiloxane (PDMS).The top monolayer is then placed in contact with the bottom monolayer with the aid of an optical microscope and micromanipulators.The substrate is then heated to cause the PMMA layer to release from the transfer media.The PMMA is subsequently dissolved in acetone for B 30min and then rinsed with isopropyl alcohol.Low-temperature PL measurements .Low-temperature measurements are con-ducted in a temperature-controlled Janis cold finger cryostat (sample in vacuum)with a diffraction-limited excitation beam diameter of B 1m m.PL is spectrally filtered through a 0.5-m monochromator (Andor–Shamrock)and detected on a charge-coupled device (Andor—Newton).Spatial PL mapping is performed using a Mad City Labs Nano-T555nanopositioning system.For PLE measurements,a continuous wave Ti:sapphire laser (MSquared—SolsTiS)is used for excitation and filtered from the PL signal using an 815-nm-long pass optical filter (Semrock).Electrostatic doping is accomplished with an indium drain contact deposited onto the monolayer WSe 2region of device 2and using the heavily doped Si as a tunable backgate.Time-resolved PL measurements .For interlayer lifetime measurements,we excite the sample with a o 200-fs pulsed Ti:sapphire laser (Coherent—MIRA).Interlayer PL is spectrally filtered through a 0.5-m monochromator (Princeton—Acton 2500),and detected with a fast time-correlated single-photon counting system composed of a fast (o 30ps full width at half maximum)single-photon avalanche detector (Micro Photon Devices—PDM series)and a picosecond event timer (PicoQuant—PicoHarp 300).References1.Geim,A.K.&Grigorieva,I.V.Van der Waals heterostructures.Nature 499,419–425(2013).2.Dean,C.R.et al.Boron nitride substrates for high-quality graphene electronics.Nat.Nanotechnol.5,722–726(2010).3.Hunt,B.et al.Massive Dirac fermions and Hofstadter butterfly in a van derWaals heterostructure.Science 340,1427–1430(2013).4.Dean,C.R.et al.Hofstadter’s butterfly and the fractal quantum Hall effect inmoire superlattices.Nature 497,598–602(2013).5.Ponomarenko,L.A.et al.Cloning of Dirac fermions in graphene superlattices.Nature 497,594–597(2013).6.Novoselov,K.S.et al.Two-dimensional atomic crystals.Proc.Natl Acad.SciUSA 102,10451–10453(2005).7.Mak,K.F.,Lee,C.,Hone,J.,Shan,J.&Heinz,T.F.Atomically thin MoS 2:anew direct-gap semiconductor.Phys.Rev.Lett.105,136805(2010).8.Splendiani,A.et al.Emerging photoluminescence in monolayer MoS 2.NanoLett.10,1271–1275(2010).MoSe2WSe 2dPhoton energy (eV)Laser power (μW)Time (ns)I n t e n s i t y (a .u .)N o r m a l i z e d P L E i n t e n s i t y (c o u n t s (μW s )–1)Power (μW)I n t e g r a t e d P L E i n t e n s i t y (C o u n t s (μW s )–1)2060404Figure 4|Power-dependent photoluminescence of interlayer exciton and its lifetime at 20K.(a )Power dependence of the interlayer exciton for 1.722eV excitation with a bi-Lorentzian fit to the 5and 100m W plots,normalized for power and charge-coupled device (CCD)integration time.(b )Spectrally integrated intensity of the interlayer exciton emission as a function of excitation power shows the saturation effect.(c )Time-resolvedphotoluminescence of the interlayer exciton (1.35eV)shows a lifetime of about 1.8ns.The dashed curve is the instrument response to the excitation laser pulse.(d )Illustration of the heterojunction band diagram,including the spin levels of the MoSe 2conduction band.The X I doublet has energy splitting equal to (o 0I Ào I )E 25meV.9.Mak,K.F.et al.Tightly bound trions in monolayer MoS2.Nat.Mater.12,207–211(2013).10.Ross,J.S.et al.Electrical control of neutral and charged excitons in amonolayer mun.4,1474(2013).11.Xiao,D.,Liu,G.-B.,Feng,W.,Xu,X.&Yao,W.Coupled spin and valleyphysics in monolayers of MoS2and other group-VI dichalcogenides.Phys.Rev.Lett.108,196802(2012).12.Cao,T.et al.Valley-selective circular dichroism of monolayer molybdenummun.3,887(2012).13.Zeng,H.,Dai,J.,Yao,W.,Xiao,D.&Cui,X.Valley polarization inMoS2monolayers by optical pumping.Nat.Nanotechnol.7,490–493(2012).14.Mak,K.F.,He,K.,Shan,J.&Heinz,T.F.Control of valley polarization inmonolayer MoS2by optical helicity.Nat.Nanotechnol.7,494–498(2012). 15.Jones,A.M.et al.Optical generation of excitonic valley coherence inmonolayer WSe2.Nat.Nanotechnol.8,634–638(2013).16.Gong,Z.et al.Magnetoelectric effects and valley-controlled spin quantumgates in transition metal dichalcogenide mun.4,2053(2013).17.Jones,A.M.et al.Spin-layer locking effects in optical orientation of excitonspin in bilayer WSe2.Nat.Phys.10,130–134(2014).18.Kang,J.,Tongay,S.,Zhou,J.,Li,J.&Wu,J.Band offsets and heterostructuresof two-dimensional semiconductors.Appl.Phys.Lett.102,012111–012114 (2013).19.Kos´mider,K.&Ferna´ndez-Rossier,J.Electronic properties of the MoS2-WS2heterojunction.Phys.Rev.B87,075451(2013).20.Terrones,H.,Lopez-Urias,F.&Terrones,M.Novel hetero-layered materialswith tunable direct band gaps by sandwiching different metal disulfides and diselenides.Sci.Rep.3,1549(2013).21.Chiu,M.-H.et al.Determination of band alignment in transition metaldichalcogenide heterojunctions,Preprint at http://arXiv:1406.5137(2014). 22.Su,J.-J.&MacDonald,A.H.How to make a bilayer exciton condensateflow.Nat.Phys.4,799–802(2008).23.Hong,X.P.et al.Ultrafast charge transfer in atomically thin MoS2/WS2heterostructures.Nat.Nanotechnol.9,682–686(2014).24.Wang,G.et al.Valley dynamics probed through charged and neutral excitonemission in monolayer WSe2.Phys.Rev.B90,075413(2014).garde,D.et al.Carrier and polarization dynamics in monolayer MoS2.Phys.Rev.Lett.112,047401(2014).26.Mai,C.et al.Many-body effects in valleytronics:direct measurement of valleylifetimes in single-layer MoS2.Nano Lett.14,202–206(2013).27.Shi,H.et al.Exciton dynamics in suspended monolayer and few-layer MoS22Dcrystals.ACS Nano7,1072–1080(2012).28.Korma´nyos,A.,Zo´lyomi,V.,Drummond,N.D.&Burkard,G.Spin-orbitcoupling,quantum dots,and qubits in monolayer transition metaldichalcogenides.Phys.Rev.X4,011034(2014).29.Butov,L.V.,Lai,C.W.,Ivanov,A.L.,Gossard,A.C.&Chemla,D.S.TowardsBose-Einstein condensation of excitons in potential traps.Nature417,47–52 (2002).30.Fogler,M.M.,Butov,L.V.&Novoselov,K.S.High-temperature superfluiditywith indirect excitons in van der Waals mun.5,4555 (2014).31.Lee,C.H.et al.Atomically thin p-n junctions with van der Waalsheterointerfaces.Nat.Nanotechnol.9,676–681(2014).32.Furchi,M.M.,Pospischil,A.,Libisch,F.,Burgdorfer,J.&Mueller,T.Photovoltaic effect in an electrically tunable van der Waals heterojunction.Nano Lett.14,4785–4791(2014).33.Cheng,R.et al.Electroluminescence and photocurrent generation fromatomically sharp WSe2/MoS2heterojunction p-n diodes.Nano Lett.14,5590–5597(2014).34.Fang,H.et al.Strong interlayer coupling in van der Waals heterostructuresbuilt from single-layer chalcogenides.Proc.Natl A111,6198–6202 (2014).AcknowledgementsThis work is mainly supported by the US DoE,BES,Materials Sciences and Engineering Division(DE-SC0008145).N.J.G.,J.Y.and D.G.M.are supported by US DoE,BES, Materials Sciences and Engineering Division.W.Y.is supported by the Research Grant Council of Hong Kong(HKU17305914P,HKU9/CRF/13G),and the Croucher Foun-dation under the Croucher Innovation Award.X.X.thanks the support of the Cottrell Scholar Award.P.R.thanks the UW GO-MAP program for their support.A.M.J.is partially supported by the NSF(DGE-0718124).J.S.R.is partially supported by the NSF (DGE-1256082).S.W.and G.C.are partially supported by the State of Washington through the UW Clean Energy Institute.Device fabrication was performed at the Washington Nanofabrication Facility and NSF-funded Nanotech User Facility. Author contributionsX.X.and P.R.conceived the experiments.P.R.and P.K.fabricated the devices,assisted by J.S.R.P.R.performed the measurements,assisted by J.R.S.,A.M.J.,J.S.R.,S.W.and G.A. P.R.and X.X.performed data analysis,with input from W.Y.N.J.G.,J.Y.and D.G.M. synthesized and characterized the bulk WSe2crystals.X.X.,P.R.,J.R.S.and W.Y.wrote the paper.All authors discussed the results.Additional informationSupplementary Information accompanies this paper at / naturecommunicationsCompetingfinancial interests:The authors declare no competingfinancial interests. Reprints and permission information is available online at / reprintsandpermissions/How to cite this article:Rivera,P.et al.Observation of long-lived interlayer excitons in monolayer MoSe2–mun.6:6242doi:10.1038/ncomms7242(2015).。
a rX iv:c ond-ma t/99728v1[c ond-m at.s upr-con]2J ul1999Low-energy electronic structure in Y 1−x Ca x Ba 2Cu 3O 7−δ:comparison of time-resolved optical spectroscopy,NMR,neutron and tunneling data.J.Demsar,K.Zagar,V.V.Kabanov and D.Mihailovic ”J.Stefan Institute”,Jamova 39,1001Ljubljana,Slovenia February 1,2008Abstract Time-resolved optical measurements give information on the quasi-particle relaxation dynamics in YBCO,from which the evolution of the gap with doping and temperature can be systematically deduced.In this paper these optical charge-channel ”pseudogap”data are compared with the ”pseudogap”obtained from the NMR Knight shift K s ,spin polar-ized neutron scattering (SPNS)and single particle tunneling measure-ments.A simple energy level diagram is proposed to explain the different ”gap”magnitudes observed by different spectroscopies in YBa 2Cu 3O 7−δ,whereby the spin gap ∆s in NMR and SPNS corresponds to a triplet local pair state,while ∆p in the charge excitation spectrum corresponds to the pair dissociation energy.At optimum doping and in the overdoped state,an additional T -dependent gap becomes evident,which closes at T c ,sug-gesting a cross-over to a more conventional BCS-like superconductivity scenario.1Introduction Spectroscopic studies of cuprates over the years have shown that at low ener-gies these materials exhibit quite a complex spectral structure,which changes with temperature and doping in a complicated way.Often there appears to be reasonable agreement regarding some of the main features between various experimental techniques.For example,optical femtosecond quasiparticle relax-ation measurements and single-particle (Giever)tunneling show a similar size pseudogap in the spectrum over a large portion of the phase diagram,and the latter is remarkably similar to the spectral features measured by angle-resolved photoemission.However,the pseudogap ∆s as observed by spectroscopies like1NMR and spin-polarized neutron scattering appears to be smaller than the opti-cal and tunneling pseudogap∆p by approximately a factor of2,for which there is as yet no accepted theoretical explanation.Thus in spite of the availability of spectral data over a large range of doping in many materials,the interpretata-tion of the low-energy excitation spectrum is still highly controversial.In this paper we summarize some of the results of time-resolved quasiparticle recombi-nation spectroscopy as a function of doping and temperature in YBa2Cu3O7−δ, which appear to give qualitative new insight into the origin of the low-energy spectral features of this material and its phase diagram.We compare the doping-evolution of the pseudogap∆p obtained from time-resolved spectroscopy with a quantitative analysis of the”spin-gap”from the NMR knight shift K s in the underdoped state using the same type of T-independent gap as deduced from the quasiparticle relaxation data.Wefind that the time-resolved QP relax-ation data are quite consistent with Giever tunneling and ARPES data and suggest that all the observations together can be explained by the existence of a pair-breaking pseudogap∆p and a triplet-state local pair excitation∆s at E≈∆p/2.2Time-resolved spectroscopy resultsThe time-resolved optical spectroscopy applied to superconductors and other materials with a gap has been given in detail elsewhere[1,2],so here we shall discuss only the results.The equations describing the temperature dependence of photoexcited QP density and their lifetime as a function of temperature are given by Kabanov et al[1].Using these equations,the properties of the gap can be investigated as a function of doping and temperature.Systematic experi-ments on YBaCuO as a function of O concentration over a wide range ofδhave shown very clear and systematic behavior of the QP dynamics[1].Particularly important is that the results are quite insensitive to surface quality and have been repeated after a period of a year with the same results.Single crystals were also studied and no significant differences were found in comparison with the thinfilm data.These measurements have recently been extended to the over-doped state using calcium-doped(Y,Ca)Ba2Cu3O7−δcrystals by Demsar et al [2],giving data on the whole phase diagram from insulating and underdoped to overdoped YBCO.A typical time-resolved signal in the optimally doped phase is shown in Figure1.Above T c,one exponential short-lived decay is observed whose amplitude is decreasing as T is increased(Figure2),while below T c, two exponentials are clearly seen,one of which has a longer lifetime which is temperature-dependent and diverges as T→T c.Such behaviour is typical also for overdoped samples,but not for underdoped samples,where only a single exponential decay is observed,with a T-indendent time constantτp∼0.4ps showing no anomaly at T c.From these experiments we can deduce that in underdoped state the evolution of the QP dynamics with temperature and dop-2ing is dominated by a temperature-independent pseudogap∆p.Near optimum doping an additional BCS-like temperature-dependent gap∆BCS appears be-low T c,which is present also in all the overdoped samples[2]and gives rise to the additional temperature-dependent relaxation process below T c.The fact theτdiverges near T c unambiguously signifies that∆BCS→0at T c.Thus close to optimum doping and in the overdoped state two gaps appear to be present simultaneously,a feature consistent with the spatially inhomoge-neous ground state[3]in which the pair-breaking excitation is represented by ∆p,while the∆BCS is a gap associated with the collective behaviour of high-carrier density stripes or clusters which start to form near optimum doping.The values of the gaps∆p and∆BCS as a function of doping obtained byfitting the temperature dependence of the photoinduced signal amplitude as shown in Fig. 2with the model calculation of Kabanov et al[1]are plotted in Figure4.3Comparison with other spectroscopiesFrom the time-resolved data on the underdoped YBCO we have deduced that the low-energy spectrum can be described by a single temperature-independent gap∆p.Starting from this observation we decided to analyse the temperature dependence of the NMR Knight shift K s available from the literature using the same T-indepedent∆p.The aim is a)to see if the simple model can describe the T-dependence of K s and b)to see if the values of the pseudogap obtained for the NMR K s agree with the optical values.The NMR knight shift for such a case can be written as[4]K s=K0+AT−βexp[−∆s/k B T],where K0is the value of K s at zero temperature,βis an exponent which depends on the shape of the singularity of the DOS at the gap and A is a constant depending on the NMR nucleus.The results offits to published data in YBCO123and124on89Y[5],63Cu [6]and17O[7]are shown in Figure3usingβ=1/2.In spite of its simplicity,the model appears to describe the data very well.The gap values∆s withβ=1/2 obtained for YBa2Cu3O7−δare shown in Figure4.∆s appears consistently lower than the∆p by approximately a factor of2.Apart from NMR K s,spin-polarized neutron scattering(SPNS)also shows a spin-excitation peak at34meV(∼390K)in underdoped YBa2Cu3O6.6,which is smaller than∆p by approximately a factor of2.However,the anomalies in the phonons signifying the presence of charge excitations occur near70meV (∼810K),also approximately twice the spin excitation energy and very close to the∆p in Fig.4.(see Mook et al,this volume).To explain the two different gaps∆p and∆s,we propose a rather straightfor-ward electronic structure in YBCO.A schematic diagram is shown in the insert to Fig. 4.The ground state is composed of local S=0singlet Cooper pairs. Since∆p is a QP charge excitation it is clearly associated with pair breaking. However,if J<∆p,the triplet local pair state also exists and lies within the3gap.It should be visible by spin-flip spectroscopies like NMR and SPNS,but not by optical spectroscopy or SP tunneling which are charge excitations.We therefore propose that the∆s observed by NMR and SPNS is the S=1local pair triplet excited state.From the experimental data in Fig.4,both∆p and ∆s decrease with increasing doping,more or less as1/x,where x is the hole density.For low doping,atδ∼0.6,J≈800K,consistent with Raman and neutron measurements.We note that possibly the situation might be different in La2−x Sr x CuO4,where the optical gap and the NMR gap appear to have the same energy scale[8],suggesting that either J¿∆p in this material or that the triplet pair state is not a bound state in this material.In underdoped YBCO,at T c there is no anomaly in either the QP relaxation[1] or the NMR K s[5,6].Similarly the SPNS intensity at34meV shows no anomaly at T c itself,but only a gradual drop with increasing T.From this we can de-duce that there is no change in the DOS at T c in the underdoped state,and that all changes of the DOS are gradual with T.This is equivalent to there being no condensation energy associated with the superconducting transition itself which is consistent with the Bose condensation of local pairs scenario,where at T c macrosopic phase coherence is established with no change in pairing am-plitude.A3D superconducting state forms when phase coherence percolates through the entire sample resulting in a transition to a coherent macroscopic state at T c.In contrast,in optimally doped and overdoped YBCO as the carrier density increases,the pairs begin to overlap,collective effects become important and a transition to a more conventional BCS-like scenario takes place[1].QP relaxation,NMR K s,SPNS and tunneling data all show an abrupt anomaly at T c signifying that pairing and phase cohrence occur at the same(or nearly the same)temperature.The most important feature of the QP relaxation data not available from other spectroscopies is the simultaneous unambiguous observation of2gaps in optimally doped and overdoped samples,one T-independent∆p and the other T-dependent∆BCS,with a BCS-like T dependence.References[1]V.V.Kabanov,et al Phys.Rev.B59,1497(1999),J.Demsar et al,Europhys.Lett.45,381(1999)[2]J.Demsar,B.Podobnik,V.V.Kabanov,D.Mihailovic and T.Wolf,subm.toPhys.Rev.Lett(1998)[3]D.Mihailovic and K.A.M¨u ller,p243”High-T c Superconductivity1996:Tenyears after the Discovery”Ed.E.Kaldis,E.Liarokapis,K.A.Muller NATO Series E:Applied Sciences vol.343(Kluwer Academic Publishers1997)4[4]A.S.Alexandrov,V.V.Kabanov and N.F.Mott,Phys.Rev.Lett.77,4796(1996)[5]H.Alloul,T.Ohno,P.Mendels,Physica162-164,193(1989)[6]Curro et al,Phys.Rev.B56,877(1997)[7]Williams et al,Phys.Rev.Lett.78,721(1998)[8]K.A.M¨u ller,Guo-meng Zhao,K.Conder and H.Keller,J.Phys.:Condens.Matter10,L291(1998)5the two-.BCS6ofCa1]7ininet8The areThe。