Mianqi Xue, Tingbing Cao, Duming Wang, Yue Wu, Huaixin Yang, Xiaoli Dong, Junbao He, Fengwang Li, G. F. Chen
We report the observation of superconductivity at 33 K in K-doped 1,2:8,9-dibenzopentacene (C30H18). This is higher than any Tc reported previously for an organic superconductor besides the alkali-metal doped C60. This finding provides an indication that superconductivity at much higher temperature may be possible in such system, if PAHs with longer benzene rings can be synthesized.
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We have prepared potassium intercalated 1,2;8,9-dibenzopentacene films under vacuum conditions. The evolution of the electronic excitation spectra upon potassium addition as measured using electron energy-loss spectroscopy clearly indicate the formation of particular doped phases with compositions K$_x$dibenzopentacene ($x$ = 1,2,3). Moreover, the stability of these phases as a function of temperature has been explored. Finally, the electronic excitation spectra also give insight into the electronic ground state of the potassium doped 1,2;8,9-dibenzopentacene films.
The geometrical and electronic structure of potassium doped phenanthrene, \ce{K3C14H10}, have been studied by first-principles density functional theory. The main effect of potassium doping is to inject charge in the narrow phenanthrene conduction band, rendering the system metallic. The Fermi surface for the experimental X-rays structure is composed of two sheets with marked one and two dimensional character respectively.
By the first principles calculations and X-ray diffraction simulations, we perform a systematic study of multiple superconducting phases of potassium-doped picene [Nature {\bf464} 76, 2010]. The combination of optimized lattice parameters, formation energy, and simulated X-ray diffraction spectra indicates that the superconducting phase with transition temperature (T$_c$) of 7 K corresponds to a charge doped K$_2$picene, which is semiconducting with a 0.1 eV energy gap, while the superconducting phase with T$_c$=18 K corresponds to a metallic K$_3$picene. The distinct crystal and electronic st…
Potassium fluoride doped LaOFeAs multiband superconductors: Evidence for extremely high upper critical field
我们描述了一种新的方法，合成氧铌酸盐超导体与氟化钾作为氟源，而不是氟化镧的来源。这条路线也允许钾在镧网站的替代，这将导致在上临界场的增加，预期为多带超导体。我们还报道了这些超导体的最高Tc起始温度为28.5K和最高的上临界场。
Inspired by the discovery of high temperature superconductivity in potassium-doped $p$-terphenyl, we examine the possibility of superconductivity in $p$-quaterphenyl with one more phenyl ring than $p$-terphenyl. The Meissner effect with critical temperatures ranging from 3.5 K to 120 K is found by the magnetic susceptibility measurements in $p$-quaterphenyl upon doping potassium in the condition of annealing or just pestling. The primary superconducting phase with critical temperature of 7.2 K can be reduplicated in several superconducting samples. In both the annealed and pestled superconduct…
To explore underlying mechanism for the superconducting phase in recent discovered aromatic hydrocarbons, we carry out the first-principles calculations on benzene, the basic and the simplest unit of the series and examine the structural and phase stability when doped by potassium, K$_x$C$_6$H$_6$ ($x=1,2,3$). We find that K$_2$C$_6$H$_6$ with the space group of $Pbca$ is the most stable phase with superconducting transition temperature around 6.2 K. Moreover, we argue that all existing hydrocarbons should have a unified superconducting phase in the same temperature range of 5$-$7 K, when dope…
The chain-like organic compounds with conjugated structure have the potential to become high temperature superconductors. We examine this idea by choosing p-quinquephenyl with five phenyl rings connected in para position. The dc magnetic susceptibility measurements provide solid evidence for the presence of Meissner effect when the compound is doped by potassium. The real part of the ac susceptibility shows exactly same transition temperature as that in dc magnetization, and the imaginary part of nearly zero value after transition implies the realization of zero-resistivity. All these features…
Organic compounds are always promising candidates of superconductors with high transition temperatures. We examine this proposal by choosing 2,2$'$-bipyridine solely composed by C, H, and N atoms. The presence of Meissner effect with a transition temperature of 7.2 K in this material upon potassium doping is demonstrated by the $dc$ magnetic susceptibility measurements. The real part of the $ac$ susceptibility exhibits the same transition temperature as that in $dc$ magnetization, and a sharp peak appeared in the imaginary part indicates the formation of the weakly linked superconducting vorte…
The electronic structure of the unoccupied and occupied states of potassium (K)-doped and undoped picene crystalline films has been investigated by using the element-selective and bulk-sensitive photon-detection methods of X-ray absorption and emission spectroscopies. We observed the formation of the doping-induced unoccupied and occupied electronic states in K-doped picene. By applying the inner-shell resonant-excitation experiments, we observed the evidence for the orbital hybridization between K and picene near the Fermi energy. Furthermore, the resonant X-ray emission experiment suggests t…
Organic materials are believed to be potential superconductor with high transition temperature (TC). Organic superconductors mainly have two families: the quasi-one dimensional (TMTSF)2X and two dimensional (BEDT-TTF)2X (Ref. 1 and 2), in which TMTSF is tetramethyltetraselenafulvalene (C10H12Se4) and BEDT-TTF or "ET" is bis(ethylenedithio)tetrathiafulvalene (C10H8S8). One key feature of the organic superconductors is that they have π-molecular orbitals, and the π-electron can delocalize throughout the crystal giving rise to metallic conductivity due to a π-orbital overlap between adjacent mole…
We performed electron energy-loss spectroscopy studies in order to get a deeper insight into the electronic properties of potassium intercalated picene, a recently discovered superconductor. A comparison of the loss function of the undoped and doped compound shows the appearance of a new peak in the optical gap, which we attribute to the charge carrier plasmon. We find a dramatic increase for the value of the background dielectric constant $ε_{\infty}$ upon doping. Our core level excitation data clearly signal filling of the conduction bands with electrons upon potassium addition.
We performed electron energy-loss spectroscopy studies in transmission in order to obtain insight into the electronic properties of potassium intercalated coronene, a recently discovered superconductor with a rather high transition temperature of about 15\,K. A comparison of the loss function of undoped and potassium intercalated coronene shows the appearance of several new peaks in the optical gap upon potassium addition. Furthermore, our core level excitation data clearly signal filling of the conduction bands with electrons.
Preliminary evidence for the occurrence of high-Tc superconductivity in alkali-doped organic materials, such as potassium-doped p-terphenyl (KPT), were recently obtained by magnetic susceptibility measurements and by the opening of a large superconducting gap as measured by ARPES and STM techniques. In this work, KPT samples have been synthesized by a chemical method and characterized by low-temperature Raman scattering and resistivity measurements. Here, we report the occurrence of a resistivity drop of more than 4 orders of magnitude at low temperatures in KPT samples in the form of compress…
Using a new two-step synthesis method - ultrasound treatment and low temperature annealing, we explore superconductivity in potassium-doped triphenylbismuth, which is composed of one bismuth atom and three phenyl rings. The combination of dc and ac magnetic measurements reveals that one hundred percent of synthesized samples exhibit superconductivity at 3.5 K and/or 7.2 K at ambient pressure. The magnetization hysteresis loops provide a strong evidence of type-II superconductor, with the upper critical magnetic field up to 1.0 Tesla. Both calculated electronic structure and measured Raman spec…
The crystal structure of potassium doped picene with an exact stoichiometry (K3C22H14, K3picene from here onwards) has been theoretically determined within Density Functional Theory allowing complete variational freedom of the crystal structure parameters and the molecular atomic positions. A modified herringbone lattice is obtained in which potassium atoms are intercalated between two paired picene molecules displaying the two possible orientations in the crystal.Along the c-axis, organic molecules alternate with chains formed by three potassium atoms. The electronic structureof the doped mat…
We report on the emergence of two disconnected superconducting domes in alkali-metal potassium (K)-doped FeSe ultra-thin films grown on graphitized SiC(0001). The superconductivity exhibits hypersensitivity to K dosage in the lower-Tc dome, whereas in the heavily electron-doped higher-Tc dome it becomes spatially homogeneous and robust against disorder, supportive of a conventional Cooper-pairing mechanism. Furthermore, the heavily K-doped multilayer FeSe films all reveal a large superconducting gap of ~ 14 meV, irrespective of film thickness, verifying the higher-Tc superconductivity only in …
The potassium-doped p-terphenyl compounds were synthesized in recent experiments and the superconductivity with high transition temperatures were reported, but the atomic structure of potassium-doped p-terphenyl is unclear. In this paper, we studied the structural and electronic properties of potassium-doped p-terphenyl with various doping levels by the first-principles simulation. We first find out the low energy position of K atom in intralayer interstitial space of the molecular layer, then examine whether two rows of K atoms can be accommodated in this one space, at last the effect of the …
We report the growth of potassium-doped BaFe2As2 thin films, where the major charge carriers are holes, on Al2O3 (0001) and LaAlO3 (001) substrates by using an ex-situ pulsed laser deposition technique. The measured Tc's are 40 and 39 K for the films grown on Al2O3 and LaAlO3, respectively and diamagnetism indicates that the films have good bulk superconducting properties below 36 and 30 K, respectively. The X-ray diffraction patterns for both films indicated a preferred c-axis orientation, regardless of the substrate structures of LaAlO3 and Al2O3. The upper critical field at zero temperature…
Synthesis methodology for flakes of p-terphenyl through sublimation under inert atmosphere of argon is presented. Flake morphology of p-terphenyl provides a favourable environment for efficient intercalation of potassium. Ratio of potassium and p-terphenyl is adjusted so as to obtain the desired superconducting phase i.e. potassium doped p-terphenyl (K3C18H14). A clear transition is observed at 107 K under Zero Field Cooled (ZFC) and Field Cooled (FC) mode. But overall the moment is positive possibly due to impurity phase dominating characteristics in the presence of negligible superconducting…
By using high pressure synthesis method, we have fabricated the potassium doped para-terphenyl. The temperature dependence of magnetization measured in both zero-field-cooled and field-cooled processes shows step like transitions at about 125 K. This confirms earlier report about the possible superconductivity like transition in the same system. However, the magnetization hysteresis loop exhibits a weak ferromagnetic background. After removing this ferromagnetic background, a Meissner effect like magnetic shielding can be found. A simple estimate on the diamagnetization of this step tells that…
Recently, superconductivity in potassium (K) doped p-terphenyl (C18H14) has been suggested by the possible observation of the Meissner effect and subsequent photoemission spectroscopy measurements, but the detailed lattice structure and more-direct evidence are still lacking. Here we report a low temperature scanning tunneling microscopy/spectroscopy (STM/STS) study on K-doped single layer p-terphenyl films grown on Au (111). We observe several ordered phases with different morphologies and electronic behaviors, in two of which a sharp and symmetric low-energy gap of about 11 meV opens below 5…
Superconducting layered transition metal dichalcogenides (TMDs) stand out among other superconductors due to the tunable nature of the superconducting transition, coexistence with other collective electronic excitations (charge density waves) and strong intrinsic spin-orbit coupling. Molybdenum disulphide (MoS2) is the most studied representative of this family of materials, especially since the recent demonstration of the possibility to tune its critical temperature, Tc, by electric-field doping. However, just one of its polymorphs, band-insulator 2H-MoS2, has so far been explored for its pot…
Recently, there is a series of reports by Wang et al. on the superconductivity in K-doped p-terphenyl (KxC18H14) with the transition temperatures range from 7 to 123 Kelvin. Identifying the structural and bonding character is the key to understand the superconducting phases and the related properties. Therefore we carried out an extensive study on the crystal structures with different doping levels and investigate the thermodynamic stability, structural, electronic, and magnetic properties by the first-principles calculations. Our calculated structures capture most features of the experimental…
Superconductivity originates from pairing of electrons. Pairing channel on Fermi surface and pairing glue are thus two pivotal issues for understanding a superconductor. Recently, high-temperature superconductivity over 40 K was found in electron-doped FeSe superconductors including K$_x$Fe$_{2-y}$Se$_2$, Li$_{0.8}$Fe$_{0.2}$OHFeSe, and 1 monolayer FeSe thin film. However, their pairing mechanism remains controversial. Here, we studied the systematic evolution of electronic structure in potassium-coated FeSe single crystal. The doping level is controlled precisely by in situ evaporating potass…
We show, by means of ab-initio calculations, that electron-electron correlations play an important role in potassium-doped picene ($K_x$-picene), recently characterized as a superconductor with $T_c = 18K$. The inclusion of exchange interactions by means of hybrid functionals reproduces the correct gap for the undoped compound and predicts an antiferromagnetic state for $x=3$, where superconductivity has been observed. The latter finding is compatible with a sizable value of the correlation strength, in agreement with simple estimates. Our results highlight the similarity between potassium-dop…
The possibility of high temperature superconductivity in organic compounds has been discussed since the pioneering work of Little in 1964, with unsatisfactory progress until the recent report of a weak Meissner shielding effect at 120 Kelvin in potassium-doped para-terphenyl samples. To date however, no other signals of the superconductivity have been shown, including the zero-resistance state or evidence for the formation of the Cooper pairs that are inherent to the superconducting state. Here, using high-resolution photoemission spectroscopy on potassium surface-doped para-terphenyl crystals…
Graphene, a zero-gap semimetal, can be transformed into a metallic, semiconducting or insulating state by either physical or chemical modification. Superconductivity is conspicuously missing among these states despite considerable experimental efforts as well as many theoretical proposals. Here, we report superconductivity in calcium-decorated graphene achieved by intercalation of graphene laminates that consist of well separated and electronically decoupled graphene crystals. In contrast to intercalated graphite, we find that Ca is the only dopant that induces superconductivity in graphene la…
K$_3$-picene is a superconducting molecular crystal with critical temperature T$_c=7$K or 18K, depending on preparation conditions. Using density functional theory we show that electron-phonon interaction accounts for T$_c ~ 3-8$ K. The average electron-phonon coupling, calculated by including the phonon energy scale in the electron-phonon scattering, is $λ=0.73$ and $ω_{\rm log}=18.0\,$ meV. Intercalant and intermolecular phonon-modes contribute substantially (40%) to $λ$ as also shown by the isotope exponents of potassium (0.19) and carbon (0.31). The relevance of these modes makes supercond…
The origin of enhanced superconductivity over 50 K in the recently discovered FeSe monolayer films grown on SrTiO$_{3}$ (STO), as compared to 8 K in bulk FeSe, is intensely debated. As with the ferrochalcogenides A$_{x}$Fe$_{2-y}$Se$_{2}$ and potassium doped FeSe, which also have a relatively high superconducting critical temperature ($T_c$), the Fermi surface (FS) of the FeSe/STO monolayer films is free of hole-like FS, suggesting that a Lifshitz transition by which these hole FSs vanish may help increasing $T_c$. However, the fundamental reasons explaining this increase of $T_c$ remain uncle…
We prepare single layer potassium-doped iron selenide (110) film by molecular beam expitaxy. Such a single layer film can be viewed as a two-dimensional system composed of weakly coupled two-leg iron ladders. Scanning tunneling spectroscopy reveals that superconductivity is developed in this two-leg ladder system. The superconducting gap is similar to that of the multi-layer films. However, the Fermi surface topology given by first-principles calculation is remarkably different from that of the bulk materials. Our results suggest that superconducting pairing is very short-ranged or takes place…
This is a report on the new 122 ternary transition-metal pnictide of BaMn2Bi2, which is crystallized from bismuth flux. BaMn2Bi2 adopts ThCr2Si2-type structure (I4/mmm) with a = 4.4902(3) Å and c = 14.687(1) Å; it is antiferromagnetic with anisotropic magnetic susceptibility and semiconducting with a band gap of Eg = 6 meV. Heat capacity result confirms the insulating ground state in BaMn2Bi2 with the electronic residual Sommerfeld coefficient of γ ~ 0. The high temperature magnetization results show that magnetic ordering temperature is TN ~ 400 K. Hole-doping in BaMn2Bi2 via potassium in Ba1…
We use neutron scattering to study vanadium (hole)-doped LiFe$_{1-x}$V$_x$As. In the undoped state, LiFeAs exhibits superconductivity at $T_c=18$ K and transverse incommensurate spin excitations similar to electron overdoped iron pnictides. Upon vanadium-doping to form LiFe$_{0.955}$V$_{0.045}$, the transverse incommensurate spin excitations in LiFeAs transform into longitudinally elongated in a similar fashion as that of potassium (hole) doped Ba$_{0.7}$K$_{0.3}$Fe$_2$As$_2$, but with dramatically enhanced magnetic scattering and elimination of superconductivity. This is different from the su…
Sr2IrO4 was predicted to be a high temperature superconductor upon electron doping since it highly resembles the cuprates in crystal structure, electronic structure and magnetic coupling constants. Here we report a scanning tunneling microscopy/spectroscopy (STM/STS) study of Sr2IrO4 with surface electron doping by depositing potassium (K) atoms. At the 0.5-0.7 monolayer (ML) K coverage, we observed a sharp, V-shaped gap with about 95% loss of density of state (DOS) at EFand visible coherence peaks. The gap magnitude is 25-30 meV for 0.5-0.6 ML K coverage and it closes around 50 K. These behav…
Potassium-doped picene (K$_x$picene) has recently been reported to be a superconductor at $x=3$ with critical temperatures up to 18 K. Here we study the electronic structure of K-doped picene films by photoelectron spectroscopy and {\it ab initio} density functional theory combined with dynamical mean-field theory (DFT+DMFT). Experimentally we observe that, except for spurious spectral weight due to the lack of a homogeneous chemical potential at low K-concentrations ($x \approx 1$), the spectra always display a finite energy gap. This result is supported by our DFT+DMFT calculations which pro…
In Ba(Fe0.95Co0.05)2As2 all of the 75As NMR intensity at the paramagnetic resonance position vanishes abruptly below Tonset(SDW)=56 K, indicating that magnetic (spin density wave) order is present in all of the sample volume, despite bulk superconductivity below Tc=15 K. The two phases thus coexist homogeneously at the microscopic scale. In Ba0.6K0.4Fe2As2, on the other hand, the signal loss below Tonset(SDW)~75 K is not complete, revealing that magnetic order is bound to finite-size areas of the sample, while the remaining NMR signal shows a clear superconducting response below Tc=37 K. Thus,…
Recent experiments have reported the emergence of high temperature superconductivity with critical temperature $T_c$ between 43K and 123K in a potassium doped aromatic hydrocarbon para-Terphenyl or p-Terphenyl. This achievement provides the record for the highest Tc in an organic superconductor overcoming the previous record of Tc=38 K in Cs3C60 fulleride. Here we propose that the driving mechanism is the quantum resonance between superconducting gaps near a Lifshitz transition which belongs to the class of Fano resonances called shape resonances. For the case of p-Terphenyl our numerical solu…
We used \emph{in-situ} potassium (K) evaporation to dope the surface of the iron-based superconductor FeTe$_{0.55}$Se$_{0.45}$. The systematic study of the bands near the Fermi level confirms that electrons are doped into the system, allowing us to tune the Fermi level of this material and to access otherwise unoccupied electronic states. In particular, we observe an electron band located above the Fermi level before doping that shares similarities with a small three-dimensional pocket observed in the cousin, heavily-electron-doped KFe$_{2-x}$Se$_2$ compound.
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