Observation of high-temperature superconductivity in sulfur hydrides at megabar pressures has generated an irresistible wave on searching for new superconductors in other compressed hydrogen-rich compounds. An immediate effort is towards exploration of the relevant candidate of tellurium hydrides, where tellurium is isoelectronic to sulfur but it has a heavier atomic mass and much weaker electronegativity. The hitherto unknown phase diagram of tellurium hydrides at high pressures was investigated by a first-principles swarm structure search. Four energetically stable and metallic stoichiometries of H4Te, H5Te2, HTe and HTe3 were uncovered above 140 GPa, showing a distinct potential energy map of tellurium hydrides from those in sulfur and selenium hydrides. The two hydrogen-rich H4Te and H5Te2 species adopt ionic structures containing exotic quasi-molecular H2 and linear H3 units, respectively. Strong electron-phonon couplings associated with the intermediate-frequency H-derived wagging and bending modes make them good superconductors with high Tc in the range of 46-104 K.
At present, hydrogen-based compounds constitute one of the most promising classes of materials for applications as a phonon-mediated high-temperature superconductors. Herein, the behavior of the superconducting phase in tellurium hydride (HTe) at high pressure ($p=300$ GPa) is analyzed in details, by using the isotropic Migdal-Eliashberg equations. The chosen pressure conditions are considered here as a case study which corresponds to the highest critical temperature value ($T_{c}$) in the analyzed material, as determined within recent density functional theory simulations. It is found that th…
Physical properties of transition metal hydride superconductors Mg2TmH6 (Tm = Rh, Pd, Ir, Pt) by first-principles calculations
Mawlana Bhashani Science and Technology University（毛拉纳·巴沙尼科技大学）；University of Rajshahi（拉杰沙希大学）；Rajshahi University of Engineering and Technology（拉杰沙希工程与技术大学）
It is argued that most of the RTSC hydrides are intrinsic hard type-II superconductors with strong pinning effects. The pinning centers are long columnar-like defects, with the radius of the order of the superconducting coherence length. The core and electromagnetic pinning are both equally operative, thus giving maximal pinning potential when vortices are oriented along the columnar axis. The theory predicts: (i) large critical currents, (ii) huge decrease of the temperature broadening of the resistance in magnetic field compared with standard superconductors, (iii) large magnetization hyster…
A recent report that sulfur hydride under pressure is an electron-phonon superconductor with a Tc of 190 K has been met with much excitement although it is yet to be confirmed. Based on several electron-phonon spectral density functions already available from density functional theory, we find that the electron-phonon spectrum is near optimum for Tc with a particularly large value of its characteristic phonon energy omega_ln which is due to the small hydrogen mass. We find that the thermodynamic universal BCS ratios are near those for Pb and Nb3Sn. We suggest that optical measurements could be…
In the present paper we report comprehensive analysis of the thermodynamic properties of novel hydrogen dominant potassium hydride superconductor (KH$_{6}$). Our computations are conducted within the Eliashberg theory which yields quantitative estimations of the most important thermodynamic properties of superconducting phase. In particular, we observe, that together with the increasing pressure all the thermodynamic properties decrease, e.g. $T_{C} \in \left< 72.91 , 55.50 \right>$ K for $p \in \left< 166 , 300 \right>$ GPa. It is predicted that such decreasing behavior corresponds to the dec…
Iron-based superconductors have grown to be a new continent of high Tc superconductors comparable to cuprates. The optimal critical temperature (Tc) of 56 K in electron-doped 1111-type iron oxypnictides attracts considerable attention of physicists and chemists. Carrier doping is not only essential to induce superconductivity but also is a critical parameter that governs the electronic, magnetic, and crystallographic properties of ground states in high-Tc superconductors. Hydride ion (H-) which is an anionic state of hydrogen acts as an efficient electron donor in the 1111-type, leading to sev…
Evidence against superconductivity in flux trapping experiments on hydrides under high pressure & On magnetic field screening and expulsion in hydride superconductors
Stability of numerous unexpected actinium hydrides was predicted via evolutionary algorithm USPEX. Electron-phonon interaction was investigated for the hydrogen-richest and most symmetric phases: R$\overline{3}$m-$AcH_{10}$, I4/mmm-$AcH_{12}$ and P$\overline{6}$m2-$AcH_{16}$. Predicted structures of actinium hydrides are consistent with all previously studied Ac-H phases and demonstrate phonon-mediated high-temperature superconductivity with Tc in the range 204-251 K for R$\overline{3}$m-$AcH_{10}$ at 200 GPa and 199-241 K for P$\overline{6}$m2-$AcH_{16}$ at 150 GPa which was estimated by dire…
Recent discovery of high-temperature superconductivity (Tc = 190 K) in sulfur hydrides at megabar pressures breaks the traditional belief on the Tc limit of 40 K for conventional superconductors, and open up the doors in searching new high-temperature superconductors in compounds made up of light elements. Selenium is a sister and isoelectronic element of sulfur, with a larger atomic core and a weaker electronegativity. Whether selenium hydrides share similar high-temperature superconductivity remains elusive, but it is a subject of considerable interest. First-principles swarm structure predi…
We predicted a new ternary hydride Li$_2$SiH$_6$ at high pressures. A systematic structure search in Li$_2$SiH$_6$ compound reveals novel stable phases with intriguing electronic and phonon properties. It is found that Li$_2$SiH$_6$ is dynamically stable from ambient pressure up to 400 GPa with three novel phases: P312, P$\bar{3}$, and P$\bar{6}$2m. The calculation of electron-phonon coupling combined with Bardeen-Cooper-Schrieffer's argument indicates that this compound may be a candidate for high $T_c$ superconductors under high pressures. In particular, the maximum $T_c$ of $P\bar{6}2m$-Li$…
The measurement of superconductivity at above 200K in compressed samples of hydrogen sulfide and lanthanum hydride at 250K is reinvigorating the search for conventional high temperature superconductors. At the same time it exposes a fascinating interplay between theory, computation and experiment. Conventional superconductivity is well understood, and theoretical tools are available for accurate predictions of the superconducting critical temperature. These predictions depend on knowing the microscopic structure of the material under consideration, and can now be provided through computational…
Lanthanum hydride is the superconductor with the highest known critical temperature. It is believed that the superconductivity is of standard BCS-type, with electrons forming Cooper pairs and opening the superconducting band gap. Here we show that the BCS electron pairing is in competition with an alternative pairing: covalent bonding. We show that the covalent pairing is favored at lower pressures, the superconducting cubic phase becomes unstable as pressure is reduced. Previous calculations based on static relaxation neglect three factors, all of which are important in stabilizing the cubic …
Recently, compressed H$_2$S has been shown to become superconducting at 203 K under a pressure of 155 GPa. One might expect fluctuations to dominate at such temperatures. Using the magnetisation critical current, we determine the ground-state London penetration depth, $λ_0$=189 nm, and the superconducting energy gap, $Δ_0$=27.8 meV, and find these parameters are similar to those of cuprate superconductors. We also determine the fluctuation temperature scale, $T_{\textrm{fluc}}=1470$ K, which shows that, unlike the cuprates, $T_c$ of the hydride is not limited by fluctuations. This is due to it…
Due to the value of the isotope shift in sulfur hydrides, a phonon-mediated pairing scenario of superconductivity is generally accepted for these high-temperature superconductors which is consistent with the Bardeen-Cooper-Schrieffer (BCS) framework. Knowing that a large electronic density of states enhances $T_c$, generalized Fermi surface topologies are used to increase it. A multi-band model within the BCS framework is proposed in this work for the description of sulfur hydride superconductors. This model is used to describe some properties of the $H_3S$ superconductor. Strong coupling effe…
Recently, Snider et al (2020 Nature 586 373) reported on the observation of superconductivity in highly-compressed carbonaceous sulfur hydride, $H_x$$(S,C)_y$. The highest critical temperature in $H_x$$(S,C)_y$ by 5 K exceeds previous record of Tc = 280 K reported by Somayazulu et al (2019 Phys. Rev. Lett. 122 027001) for highly-compressed $La$$H_{10}$. In this paper we analyze experimental temperature dependent magnetoresistance data, R(T,B), reported by Snider et al. The analysis shows that $H_x$$(S,C)_y$ compound exhibited Tc = 190 K (P = 210 GPa) has the electron-phonon coupling constant $…
The Meissner effect, magnetic field expulsion, is a hallmark of superconductivity. Associated with it, superconductors exclude applied magnetic fields. Recently Minkov et al. presented experimental results reportedly showing "definitive evidence of the Meissner effect" in sulfur hydride and lanthanum hydride under high pressure [1], and more recently Eremets et al. argued that "the arguments against superconductivity (in hydrides) can be either refuted or explained" [2]. Instead, we show here that the evidence presented in those papers does not support the case for superconductivity in these m…
While great scientific efforts focus on the synthesis and studies of near-room-temperature (NRT) superconductors exhibited record superconducting transition temperatures (for instance, laser annealed H3S, LaH10 and YHn (n = 4,6,7,9) with Tc > 200 K), unannealed low-Tc counterparts of NRT superconductors stay in the background. However, the formers are part of hydrogen-rich superconductors family and the success in understanding of NRT superconductivity depends on the study of these materials too. In this paper we analyse experimental temperature dependent upper critical field data, Bc2(T), rep…
Due to its low atomic mass hydrogen is the most promising element to search for high-temperature phononic superconductors. However, metallic phases of hydrogen are only expected at extreme pressures (400 GPa or higher). The measurement of a record superconducting critical temperature of 190 K in a hydrogen-sulfur compound at 200 GPa of pressure[1], shows that metallization of hydrogen can be reached at significantly lower pressure by inserting it in the matrix of other elements. In this work we re-investigate the phase diagram and the superconducting properties of the H-S system by means of mi…
The recent discovery of room temperature superconductivity (283 K) in carbonaceous sulfur hydride (C-S-H) has attracted lots of interests in ternary hydrogen rich materials. In this report, ternary hydride P-S-H has been synthesized through photochemical reaction from elemental sulfur (S), phosphorus (P) and molecular hydrogen (H2) at high pressures and room temperature. The Raman spectroscopy under pressure shows that H2S and PH3 compounds are synthesized after laser heating at 0.9 GPa and a ternary van der Waals compound P-S-H is synthesized with a further compression to 4.6 GPa. The P-S-H c…
Hydrogen-based superconductors provide a route to the long-sought goal of room-temperature superconductivity, but the high pressures required to metallize these materials limit their immediate application. For example, carbonaceous sulfur hydride, the first room-temperature superconductor, can reach a critical temperature (Tc) of 288 K only at the extreme pressure of 267 GPa. The next recognized challenge is the realization of room-temperature superconductivity at significantly lower pressures. Here, we propose a strategy for the rational design of high-temperature superconductors at low press…
High pressure structures, phase diagram and superconductivity of polonium hydrides have been systematically investigated through the first-principles calculations based on the density functional theory. With the increasing pressure, several stoichiometries (PoH, $\textrm{PoH}_\textrm{2}$, $\textrm{PoH}_4$ and $\textrm{PoH}_6$) are predicted to stabilize in the excess hydrogen environment. All of the reported hydrides, exception of PoH, exhibit intriguing structural character with the appearing $\textrm{H}_2$ units. Moreover, our electronic band structure and the projected density of states (PD…
Noble metals adopt close-packed structures at ambient pressure and rarely undergo structural transformation at high pressures. Platinum (Pt), in particular, is normally considered to be unreactive and is therefore not expected to form hydrides under pressure. We predict that platinum hydride (PtH) has a lower enthalpy than its constituents solid Pt and molecular hydrogen at pressures above 21.5 GPa. We have calculated structural phase transitions from tetragonal to hexagonal close-packed or face-centered cubic (fcc) PtH between 70 and 80 GPa. Linear response calculations indicate that PtH is a…
Fermi velocity, $v_F$, is one of the primary characteristics of any conductor, including superconductors. For conductors at ambient pressure several experimental techniques have been developed to measure $v_F$ and, for instance, Zhou et al (Nature 423 398 (2003)) reported that high-Tc cuprates exhibit universal nodal Fermi velocity of $v_F$ = $2.7*10^5$ m/s. However, there were no experimental techniques applied to measure $v_F$ in highly-compressed near-room-temperature superconductors (NRTS), due to experimental challenges. Here to answer a question about the existence of the universal Fermi…
Inverse Isotope Effect in the Ternary Perovskite Hydride SrPdH/D$_{2.9}$: A Signature of Quantum Zero-Point Fluctuations
Carnegie Institution for Science（卡内基科学研究所）；Graz University of Technology（格拉茨工业大学）；Stockholm University（斯德哥尔摩大学）；Intellectual Ventures（智识风险投资公司）；University of Cambridge（剑桥大学）；Tohoku University（东北大学）；Oak Ridge National Laboratory（橡树岭国家实验室）
Over the past six years, superconductivity at high temperatures has been reported in a variety of hydrogen-rich compounds under high pressure. That high-temperature superconductivity should exist in these materials is expected according to the conventional theory of superconductivity, as shown by detailed calculations. However here we argue that experimental observations rule out conventional superconductivity in these materials. Our results indicate that either these materials are unconventional superconductors of a novel kind, which we term `nonstandard superconductors', or alternatively tha…
We investigated the preferred electron dopants at the oxygen sites of 1111-type SmFeAsO by changing the atmospheres around the precursor with the composition of Sm:Fe:As:O = 1:1:1:1-x in high-pressure synthesis. Under H2O and H2 atmospheres, hydrogens derived from H2O or H2 molecules were introduced into the oxygen sites as a hydride ion, and SmFeAsO1-xHx was obtained. However, when the H2O and H2 sources were removed from the synthetic process, nearly stoichiometric SmFeAsO was obtained and the maximum amount of oxygen vacancies introduced remained x = 0.05(4). Density functional theory calcu…
The discovery of high-$T_c$ conventional superconductivity in high-pressure hydrides has helped establish computational methods as a formidable tool to guide material discoveries in a field traditionally dominated by serendipitous experimental search. This paves the way to an ever-increasing use of data-driven approaches to the study and design of superconductors. In this work, we propose a new method to generate meaningful datasets of superconductors, based on element substitution into a small set of representative structural templates, generated by crystal structure prediction methods (Multi…
Superconducting transitions in the absence of magnetic field should be non-hysteretic. Here we address the fact that the drops in electrical resistance that have been interpreted as evidence of superconductivity in several hydrides under high pressure (so-called "superhydrides") show hysteresis. We argue that the experimental evidence shows that the observed hysteresis cannot be attributed to experimental artifacts but is intrinsic to the samples. Assuming that the drops in resistance signal a thermodynamic phase transition, we argue that the presence of intrinsic thermal hysteresis indicates …
Lanthanum hydride LaH$_{10}$ with a sodalitelike clathrate structure was experimentally realized to exhibit a room-temperature superconductivity under megabar pressures. Based on first-principles calculations, we reveal that the metal framework of La atoms has the excess electrons at interstitial regions. Such anionic electrons are easily captured to form a stable clathrate structure of H cages. We thus propose that the charge transfer from La to H atoms is mostly driven by the electride property of the La framework. Further, the interaction between La atoms and H cages induces a delocalizatio…
At present, metal hydrides are considered highly promising materials for phonon-mediated superconductors, that exhibit high values of the critical temperature. In the present study, the superconducting properties of the compressed selenium hydride in its simplest form (HSe) are analyzed, toward quantitative characterization of this phase. By using the state-of-art Migdal-Eliashberg formalism, it is shown that the critical temperature in this material is relatively high ($T_{c}$=42.65 K) and surpass the level of magnesium diboride superconductor, assuming that the Coulomb pseudopotential takes …
To understand the most-recent experiment on room-temperature superconductivity in carbonaceous sulfur hydride (CSH) systems under high pressure, we have performed extensive stoichiometry and structure searches of ternary CSH compounds using generic evolutionary algorithms. Judged from the formation enthalpy of different CSH compounds, our studies conclude that certain levels of carbon doping (~5%-6%) in sulfur hydride (H$_3$S) in its R3m and phases gives rise to the most-stable structure (second to the H$_3$S itself) among the various CSH systems found. The replacement of a small amount of sul…
Two hydrogen-rich materials, H$_3$S and LaH$_{10}$, synthesized at megabar pressures, have revolutionized the field of condensed matter physics providing the first glimpse to the solution of the hundred-year-old problem of room temperature superconductivity. The mechanism underlying superconductivity in these exceptional compounds is the conventional electron-phonon coupling. Here we describe recent advances in experimental techniques, superconductivity theory and first-principles computational methods which have made possible these discoveries. This work aims to provide an up-to-date compendi…
It was recently pointed out that so-called "superhydrides", hydrogen-rich materials that appear to become superconducting at high temperatures and pressures, exhibit physical properties that are different from both conventional and unconventional standard type I and type II superconductors [1,2]. Here we consider magnetic field expulsion in the first material in this class discovered in 2015, sulfur hydride [3]. A nuclear resonant scattering experiment has been interpreted as demonstration that the Meissner effect takes place in this material [4,5]. Here we point out that the observed effect, …
It has been a hot issue to search for hydrides at high pressure with high superconducting transition temperature (Tc). In this work, ternary hydrogen-rich compounds KYHn (n = 1-16) were studied and calculated using the density function theory (DFT) method and he results showed that the KYH8 demonstrates good stability and superconductivity. And keep thermodynamically stable in the pressure range of 50-300 GPa. The research found that the Tc of KYH8-C2/m was predicted to be 111.3K, 122.0K, and 142.3K at 200, 250 and 300 GPa, respectively. Our current study provides a possibility for searching n…
High-temperature conventional superconductivity in hydrogen-rich materials under high pressure has been reportedly found in twelve different compounds in recent years. However, the experimental evidence on which these claims are based has recently been called into question. Here we discuss the measurement of trapped magnetic flux, that should establish definitively that these materials are indeed high-temperature superconductors. Its absence should confirm claims to the contrary.
