Showing 1–11 of 11 results for author: Bi, T

Toward nanophotonic platforms for solid-state $^{229}$Th nuclear clocks

Authors: Sandro Kraemer, Karen Mamian, Toby Bi, Shun Fujii, Jan de Haan, Harshith Babu, Arno Claessens, Rafael Ferrer Garcia, Fedor Ivandikov, Piet Van Duppen, Andreas Dragoun, Christoph E. Düllmann, Christoph Marquardt, Ulrich Wahl, Bart Kuyken, Thorsten Schumm, Pascal Del'Haye, Lino M. C. Pereira, Georgy A. Kazakov, Kasper Van Gasse, Charles Roques-Carmes

Abstract: While the $^{229}$Th nuclear isomer has recently been observed and laser-excited, converting optical nuclear manipulation into a chip-scale solid-state frequency standard remains an open challenge. Here, we present a nanophotonic platform to realize an all-solid-state nuclear clock based on the low-energy isomeric transition of $^{229}$Th embedded in high-$Q$ fluoride photonic resonators. By coupl… ▽ More While the $^{229}$Th nuclear isomer has recently been observed and laser-excited, converting optical nuclear manipulation into a chip-scale solid-state frequency standard remains an open challenge. Here, we present a nanophotonic platform to realize an all-solid-state nuclear clock based on the low-energy isomeric transition of $^{229}$Th embedded in high-$Q$ fluoride photonic resonators. By coupling ensembles of thorium nuclei to confined optical modes, we show that resonant field build-up in the cavity can substantially enhance the nuclear excitation rate, enabling optical interrogation at practical laser intensities. We model the nuclei-photon interaction dynamics and outline a technological roadmap toward addressing this challenge, including resonator fabrication in fluoride crystals, thorium implantation, nuclear excitation with integrated lasers, and on-chip detection of vacuum-ultraviolet photons. As an initial proof of concept, we implant a crystalline fluoride whispering-gallery-mode resonator with $^{229}$Th and assess the impact of implantation-induced damage on resonator performance. Our platform leverages recent advances in materials integration and nanophotonics to chart a realistic route toward compact and scalable nuclear frequency standards. △ Less

Submitted 22 April, 2026; originally announced April 2026.

Quantum Anharmonic Effects on the Superconductivity of I-43m CH4-H3S at High Pressures: a First-Principles Study

Authors: Pugeng Hou, Francesco Belli, Tiange Bi, Eva Zurek, Ion Errea

Abstract: Making use of first-principles calculations we analyze the effect of quantum ionic fluctuations and lattice anharmonicity on the crystal structure and superconductivity of I-43m CH4-H3S, one of the lowest enthalpy structures in the C-S-H system, in the 150-300 GPa pressure range within the stochastic self-consistent harmonic approximation. We predict a correction to the crystal structure, which is… ▽ More Making use of first-principles calculations we analyze the effect of quantum ionic fluctuations and lattice anharmonicity on the crystal structure and superconductivity of I-43m CH4-H3S, one of the lowest enthalpy structures in the C-S-H system, in the 150-300 GPa pressure range within the stochastic self-consistent harmonic approximation. We predict a correction to the crystal structure, which is formed by an H3S lattice and CH4 molecules, the phonon spectra, and the pressure-dependent superconducting critical temperatures, which have been estimated in previous calculations without considering ionic fluctuations on the crystal structure and assuming the harmonic approximation for the lattice dynamics. Our results show that quantum ionic fluctuations have an impact on the distance between H atoms and S atoms in the H3S host lattice, pushing it towards more symmetric bonds, while the methane molecules are barely affected. According to our anharmonic phonon spectra, this structure is dynamically stable above 150 GPa, which is 30 GPa lower than the pressure at which the harmonic approximation predicts the emergence of an instability. As a consequence of the strong anharmonic enhancement of the phonon frequencies, the electron-phonon coupling constant is suppressed by 46% at 200 GPa, and even more at lower pressures. As a result, the superconducting critical temperature is overestimated by around 50 K at 200 GPa, such that it falls below 150 K in the whole pressure range studied. Our results underline that ternary hydrides are subject to strong anharmonic effects on their structural, vibrational, and superconducting properties. △ Less

Submitted 24 December, 2024; originally announced December 2024.

Comments: arXiv admin note: substantial text overlap with arXiv:2107.08669; text overlap with arXiv:2102.00072

ACM Class: J.2.9

Structural Diversity and Superconductivity in S-P-H Ternary Hydrides Under Pressure

Authors: Nisha Geng, Tiange Bi, Eva Zurek

Abstract: Evolutionary structure searches revealed a plethora of stable and low-enthalpy metastable phases in the S-P-H ternary phase diagram under pressure. A wide variety of crystalline structure types were uncovered ranging from those possessing one-dimensional chains, two-dimensional sheets based on S-H or S-P-H square lattices as well as S-H or P-H honeycombs, and cage-like structures. Some of the cage… ▽ More Evolutionary structure searches revealed a plethora of stable and low-enthalpy metastable phases in the S-P-H ternary phase diagram under pressure. A wide variety of crystalline structure types were uncovered ranging from those possessing one-dimensional chains, two-dimensional sheets based on S-H or S-P-H square lattices as well as S-H or P-H honeycombs, and cage-like structures. Some of the cage-like structures could be derived from doping the high-pressure high-temperature superconducting $Im\bar{3}m$ H$_3$S phase with phosphorous. Most of the discovered compounds were metallic, however those derived from $Im\bar{3}m$ H$_3$S lattices with low levels of P-doping were predicted to possess the highest superconducting critical temperatures ($T_c$s). The propensity for phosphorous to assume octahedral coordination, as well as the similar radii of sulfur and phosphorous are key to maintaining a high density of states at the Fermi level in $Im\bar{3}m$ S$_{0.875}$P$_{0.125}$H$_3$, whose $T_c$ was estimated to be similar to that of H$_3$S at 200~GPa. △ Less

Submitted 1 January, 2022; originally announced January 2022.

Materials under high pressure: A chemical perspective

Authors: Katerina P. Hilleke, Tiange Bi, Eva Zurek

Abstract: At high pressure, the typical behavior of elements dictated by the periodic table - including oxidation numbers, stoichiometries in compounds, and reactivity, to name but a few - is altered dramatically. As pressure is applied, the energetic ordering of atomic orbitals shifts, allowing core orbitals to become chemically active, atypical electron configurations to occur, and in some cases, non-atom… ▽ More At high pressure, the typical behavior of elements dictated by the periodic table - including oxidation numbers, stoichiometries in compounds, and reactivity, to name but a few - is altered dramatically. As pressure is applied, the energetic ordering of atomic orbitals shifts, allowing core orbitals to become chemically active, atypical electron configurations to occur, and in some cases, non-atom-centered orbitals to form in the interstices of solid structures. Strange stoichiometries, structures, and bonding motifs result. Crystal structure prediction tools, not burdened by preconceived notions about structural chemistry learned at atmospheric pressure, have been applied to great success to explore phase diagrams at high pressure, identifying novel structures in diverse chemical systems. Several of these have been subsequently observed by experimental investigations, whose access to high-pressure regimes is bolstered by advances in diamond anvil cell and dynamic compression techniques. The joint efforts of experiment and theory have led to particular success in the realm of high-temperature superconductors, identifying many novel phases whose superconducting transition approaches room temperature. △ Less

Submitted 30 December, 2021; originally announced December 2021.

Comments: 17 pages (35 with references), 6 figures

A Little Bit of Carbon Can do a Lot for Superconductivity in H$_3$S

Authors: Xiaoyu Wang, Tiange Bi, Katerina P. Hilleke, Anmol Lamichhane, Russell J. Hemley, Eva Zurek

Abstract: First-principles calculations were carried out to provide a chemical basis for proposed structures associated with the recently reported room-temperature superconductivity in a carbonaceous sulfur hydride material under pressure. Calculations were performed on supercells of H$_3$S doped with 1.85-25\% carbon, corresponding to SH$_3$~$\rightarrow$~CH$_3$ or SH$_3$~$\rightarrow$~CH$_4$ substitutions… ▽ More First-principles calculations were carried out to provide a chemical basis for proposed structures associated with the recently reported room-temperature superconductivity in a carbonaceous sulfur hydride material under pressure. Calculations were performed on supercells of H$_3$S doped with 1.85-25\% carbon, corresponding to SH$_3$~$\rightarrow$~CH$_3$ or SH$_3$~$\rightarrow$~CH$_4$ substitutions, primarily at pressures of 270 GPa where the maximum critical temperature, $T_c$, has been reported. In the first type of substitution, the carbon atoms can be six-fold coordinated, stabilizing a CH$_6$ configuration within the cubic H$_3$S framework structure that forms under pressure. In the second, the carbon can be four-fold coordinated as methane intercalated into the H-S lattice, with or without an additional hydrogen in the framework. The results indicate that unusual local bonding configurations with respect to carbon can be stabilized under pressure. The doping breaks degenerate bands, lowering the density of states at the Fermi level ($N_F$), and localizing electrons in C-H bonds. Low levels of CH$_4$ doping do not increase $N_F$ to values as high as those calculated for $Im\bar{3}m$ H$_3$S, but they do result in a larger logarithmic average phonon frequency, and an electron-phonon coupling parameter comparable to that of $R3m$ H$_3$S. The $T_c$s estimated for carbon doping levels ranging from 1.85-5.7\% are compatible with experimental measurements for the C-S-H superconductor. △ Less

Submitted 14 November, 2021; v1 submitted 20 September, 2021; originally announced September 2021.

The Li-F-H Ternary System at High Pressures

Authors: Tiange Bi, Andrew Shamp, Tyson Terpstra, Russell J. Hemley, Eva Zurek

Abstract: Evolutionary crystal structure prediction searches have been employed to explore the ternary Li-F-H system at 300 GPa. Metastable phases were uncovered within the static lattice approximation, with LiF$_3$H$_2$, LiF$_2$H, Li$_3$F$_4$H, LiF$_4$H$_4$, Li$_2$F$_3$H and LiF$_3$H lying within 50 meV/atom of the 0 K convex hull. All of these phases contain H$_n$F$_{n+1}^-$ ($n$ = 1; 2) anions, and Li… ▽ More Evolutionary crystal structure prediction searches have been employed to explore the ternary Li-F-H system at 300 GPa. Metastable phases were uncovered within the static lattice approximation, with LiF$_3$H$_2$, LiF$_2$H, Li$_3$F$_4$H, LiF$_4$H$_4$, Li$_2$F$_3$H and LiF$_3$H lying within 50 meV/atom of the 0 K convex hull. All of these phases contain H$_n$F$_{n+1}^-$ ($n$ = 1; 2) anions, and Li$^+$ cations. Other structural motifs such as LiF slabs, H$_3^+$ molecules, and F$^{δ-}$ ions are present in some of the low enthalpy Li-F-H structures. The bonding within the H$_n$F$_{n+1}^-$ molecules, which may be bent or linear, symmetric or asymmetric, is analyzed. The five phases closest to the hull are insulators, while LiF$_3$H is metallic and predicted to have a vanishingly small superconducting critical temperature. This study lays the foundation for future investigations of the role of temperature and anharmonicity on the stability and properties of compounds and alloys in the Li-F-H ternary system. △ Less

Submitted 30 December, 2020; originally announced December 2020.

Comments: 11 pages, 4 figures, 1 table

A Metastable CaSH$_3$ Phase Composed of HS Honeycomb Sheets that is Superconducting Under Pressure

Authors: Yan Yan, Tiange Bi, Nisha Geng, Xiaoyu Wang, Eva Zurek

Abstract: Evolutionary searches predicted a number of ternary phases that could be synthesized at pressures of 100-300~GPa. $P6_3/mmc$ CaSH$_2$, $Pnma$ CaSH$_2$, $Cmc2_1$ CaSH$_6$, and $I\bar{4}$ CaSH$_{20}$ were composed of a Ca-S lattice along with H$_2$ molecules coordinated in a ``side-on'' fashion to Ca. The H-H bond lengths in these semiconducting phases were elongated because of H$_2$ $σ\rightarrow$… ▽ More Evolutionary searches predicted a number of ternary phases that could be synthesized at pressures of 100-300~GPa. $P6_3/mmc$ CaSH$_2$, $Pnma$ CaSH$_2$, $Cmc2_1$ CaSH$_6$, and $I\bar{4}$ CaSH$_{20}$ were composed of a Ca-S lattice along with H$_2$ molecules coordinated in a ``side-on'' fashion to Ca. The H-H bond lengths in these semiconducting phases were elongated because of H$_2$ $σ\rightarrow$ Ca d donation, and Ca d$\rightarrow$ H$_2$ $σ^*$ back-donation, via a Kubas-like mechanism. $P\bar{6}m2$ CaSH$_3$, consisting of two-dimensional HS and CaH$_2$ sheets, was metastable and metallic above \edit{128~GPa}. The presence of van Hove singularities increased its density of states at the Fermi level, and concomitantly the superconducting critical temperature, which was estimated to be as high as \edit{$\sim$100~K at 128~GPa}. This work will inspire the search for superconductivity in materials based upon \edit{honeycomb HX (X=S, Se, Te), and MH$_2$ (M=Mg, Ca, Sr, Ba) layers} under pressure. △ Less

Submitted 29 December, 2020; originally announced December 2020.

High-Temperature Superconductivity in Alkaline and Rare Earth Polyhydrides at High Pressure: A Theoretical Perspective

Authors: Eva Zurek, Tiange Bi

Abstract: The theoretical exploration of the phase diagrams of binary hydrides under pressure using \emph{ab initio} crystal structure prediction techniques coupled with first-principles calculations has led to the \emph{in silico} discovery of numerous novel superconducting materials. This Perspective article focuses on the alkaline earth and rare earth polyhydrides whose superconducting critical temperatu… ▽ More The theoretical exploration of the phase diagrams of binary hydrides under pressure using \emph{ab initio} crystal structure prediction techniques coupled with first-principles calculations has led to the \emph{in silico} discovery of numerous novel superconducting materials. This Perspective article focuses on the alkaline earth and rare earth polyhydrides whose superconducting critical temperature, $T_c$, was predicted to be above the boiling point of liquid nitrogen. After providing a brief overview of the computational protocol used to predict the structures of stable and metastable hydrides under pressure, we outline the equations that can be employed to estimate $T_c$. The systems with a high $T_c$ can be classified according to the motifs found in their hydrogenic lattices. The highest $T_c$s are found for cages that are reminiscent of clathrates, and the lowest for systems that contain atomic and molecular hydrogen. A wide variety of hydrogenic motifs including 1- and 2-dimensional lattices, as well as H$_{10}^{δ-}$ molecular units comprised of fused H$_5^{δ-}$ pentagons are present in phases with intermediate $T_c$s. Some of these phases are predicted to be superconducting at room temperature. Some may have recently been synthesized in diamond anvil cells. △ Less

Submitted 29 October, 2018; originally announced October 2018.

Comments: 12 pages, 5 figures, 3 tables, perspective

Crystal Structures and Properties of Iron Hydrides at High Pressure

Authors: Niloofar Zarifi, Tiange Bi, Hanyu Liu, Eva Zurek

Abstract: Evolutionary algorithms and the particle swarm optimization method have been used to predict stable and metastable high hydrides of iron between 150-300 GPa that have not been discussed in previous studies. Cmca FeH5, Pmma FeH6 and P2/c FeH6 contain hydrogenic lattices that result from slight distortions of the previously predicted I4/mmm FeH5 and Cmmm FeH6 structures. Density functional theory ca… ▽ More Evolutionary algorithms and the particle swarm optimization method have been used to predict stable and metastable high hydrides of iron between 150-300 GPa that have not been discussed in previous studies. Cmca FeH5, Pmma FeH6 and P2/c FeH6 contain hydrogenic lattices that result from slight distortions of the previously predicted I4/mmm FeH5 and Cmmm FeH6 structures. Density functional theory calculations show that neither the I4/mmm nor the Cmca symmetry FeH5 phases are superconducting. A P1 symmetry FeH7 phase, which is found to be dynamically stable at 200 and 300 GPa, adds another member to the set of predicted nonmetallic transition metal hydrides under pressure. Two metastable phases of FeH$_8$ are found, and the preferred structure at 300 GPa contains a unique 1-dimensional hydrogenic lattice. △ Less

Submitted 21 September, 2018; originally announced September 2018.

Comments: 24 pages, 7 figures

The Search for Superconductivity in High Pressure Hydrides

Authors: Tiange Bi, Niloofar Zarifi, Tyson Terpstra, Eva Zurek

Abstract: The computational and experimental exploration of the phase diagrams of binary hydrides under high pressure has uncovered phases with novel stoichiometries and structures, some which are superconducting at quite high temperatures. Herein we review the plethora of studies that have been undertaken in the last decade on the main group and transition metal hydrides, as well as a few of the rare earth… ▽ More The computational and experimental exploration of the phase diagrams of binary hydrides under high pressure has uncovered phases with novel stoichiometries and structures, some which are superconducting at quite high temperatures. Herein we review the plethora of studies that have been undertaken in the last decade on the main group and transition metal hydrides, as well as a few of the rare earth hydrides at pressures attainable in diamond anvil cells. The aggregate of data shows that the propensity for superconductivity is dependent upon the species used to "dope" hydrogen, with some of the highest values obtained for elements that belong to the alkaline and rare earth, or the pnictogen and chalcogen families. △ Less

Submitted 31 May, 2018; originally announced June 2018.

Comments: 73 pages, 18 figures, and 1 table

Decomposition Products of Phosphine Under Pressure: PH2 Stable and Superconducting?

Authors: Andrew Shamp, Tyson Terpstra, Tiange Bi, Zackary Falls, Patrick Avery, Eva Zurek

Abstract: Evolutionary algorithms (EA) coupled with Density Functional Theory (DFT) calculations have been used to predict the most stable hydrides of phosphorous (PHn, n = 1-6) at 100, 150 and 200 GPa. At these pressures phosphine is unstable with respect to decomposition into the elemental phases, as well as PH2 and H2. Three metallic PH2 phases were found to be dynamically stable and superconducting betw… ▽ More Evolutionary algorithms (EA) coupled with Density Functional Theory (DFT) calculations have been used to predict the most stable hydrides of phosphorous (PHn, n = 1-6) at 100, 150 and 200 GPa. At these pressures phosphine is unstable with respect to decomposition into the elemental phases, as well as PH2 and H2. Three metallic PH2 phases were found to be dynamically stable and superconducting between 100-200 GPa. One of these contains five formula units in the primitive cell and has C2/m symmetry (5FU-C2/m). It is comprised of 1D periodic PH3-PH-PH2-PH-PH3 oligomers. Two structurally related phases consisting of phosphorous atoms that are octahedrally coordinated by four phosphorous atoms in the equatorial positions and two hydrogen atoms in the axial positions (I4/mmm and 2FU-C2/m) were the most stable phases between ~160-200 GPa. Their superconducting critical temperatures (Tc) were computed as being 70 and 76 K, respectively, via the Allen-Dynes modified McMillan formula and using a value of 0.1 for the Coulomb pseudopotential, u*. Our results suggest that the superconductivity recently observed by Drozdov, Eremets and Troyan when phosphine was subject to pressures of 207 GPa in a diamond anvil cell may result from these, and other, decomposition products of phosphine. △ Less

Submitted 14 December, 2015; v1 submitted 17 September, 2015; originally announced September 2015.

Comments: 9 pages, 5 figures, 2 tables