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Room-temperature superconductivity in a carbonaceous sulfur hydride

One of the long-standing challenges in experimental physics is the observation of room-temperature superconductivity (RTSC). Recently, high temperature conventional superconductivity in hydrogen-rich materials has been reported in several systems under high pressure. The most significant discovery in reaching RTSC is the pressure-driven disproportionation of hydrogen sulfide (H 2 S) to H 3 S with a confirmed Tc of 203 kelvin at 155 gigapascals. As H 2 S readily mixes with hydrogen to form guest-host structures at lower pressures, the comparable size of methane to H 2 S should allow molecular exchange within a large assemblage of van der Waals solids that are (highly) hydrogen-rich with H 2 inclusions that are then the building blocks for novel superconducting compounds at extreme conditions. Here, we report superconductivity in a photochemically transformed carbonaceous sulfur hydride system with a maximum superconducting transition temperature of 287.7 ± 1.2 kelvin (~15° celsius) achieved at 267 ± 10 gigapascals. The superconducting state is observed over a broad pressure range from 140 to 275 gigapascals, with a dramatic upturn in Tc above 220 gigapascals. Superconductivity is established by the observation of zero resistance, magnetic susceptibility up to 190 gigapascals, and reduction of Tc under an external magnetic field up to 9 tesla, with an upper critical magnetic field of ~62 tesla based on Ginzburg–Landau (GL) model at zero temperature. The light, quantum nature of hydrogen limits structural and stoichiometric determination using x-ray scattering techniques. Raman spectroscopy is used to probe the chemical and structural transformations pre-metallization. In conclusion, the introduction of chemical tuning within our reported ternary system could be the path forward to lowering the pressure while preserving the RTSC properties.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

A superconducting quantum simulator based on a photonic-bandgap metamaterial

Synthesizing many-body quantum systems with various ranges of interactions facilitates the study of quantum chaotic dynamics. Such extended interaction range can be enabled by using nonlocal degrees of freedom such as photonic modes in an otherwise locally connected structure. Here, we present a superconducting quantum simulator in which qubits are connected through an extensible photonic-bandgap metamaterial, thus realizing a one-dimensional Bose-Hubbard model with tunable hopping range and on-site interaction. Using individual site control and readout, we characterize the statistics of measurement outcomes from many-body quench dynamics, which enables in situ Hamiltonian learning. Further, the outcome statistics reveal the effect of increased hopping range, showing the predicted crossover from integrability to ergodicity. Our work enables the study of emergent randomness from chaotic many-body evolution and, more broadly, expands the accessible Hamiltonians for quantum simulation using superconducting circuits.

Science & Technology - Other Topics↗

Quantum Simulation of Molecular Electronic States with a Transcorrelated Hamiltonian: Higher Accuracy with Fewer Qubits

Simulation of electronic structure is one of the most promising applications on noisy intermediate-scale quantum (NISQ) era devices. However, NISQ devices suffer from a number of challenges like limited qubit connectivity, short coherence times, and sizable gate error rates. Thus, desired quantum algorithms should require shallow circuit depths and low qubit counts to take advantage of these devices. Here, we attempt to reduce quantum resource requirements for molecular simulations on a quantum computer while maintaining the desired accuracy with the help of classical quantum chemical theories of canonical transformation and explicit correlation. In this work, compact ab initio Hamiltonians are generated classically, in the second quantized form, through an approximate similarity transformation of the Hamiltonian with (a) an explicitly correlated two-body unitary operator with generalized pair excitations that remove the Coulombic electron–electron singularities from the Hamiltonian and (b) a unitary one-body operator to efficiently capture the orbital relaxation effects required for accurate description of the excited states. The resulting transcorrelated Hamiltonians are able to describe both the ground and the excited states of molecular systems in a balanced manner. Using the variational quantum eigensolver (VQE) method based on the unitary coupled cluster with singles and doubles (UCCSD) ansatz and only a minimal basis set (ANO-RCC-MB), we demonstrate that the transcorrelated Hamiltonians can produce ground state energies comparable to the reference CCSD energies with the much larger cc-pVTZ basis set. This leads to a reduction in the number of required CNOT gates by more than 3 orders of magnitude for the chemical species studied in this work. Furthermore, using the quantum equation of motion (qEOM) formalism in conjunction with the transcorrelated Hamiltonian, we are able to reduce the deviations in the excitation energies from the reference EOM-CCSD/cc-pVTZ values by an order of magnitude. In conclusion, the transcorrelated Hamiltonians developed here are Hermitian and contain only one- and two-body interaction terms and thus can be easily combined with any quantum algorithm for accurate electronic structure simulations.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Quantum simulations of SO(5) many-fermion systems using qudits

The structure and dynamics of many-body systems are the result of a delicate interplay between underlying interactions. Fermionic pairing, for example, plays a central role in various physical systems, ranging from condensed matter to nuclear systems, where it can lead to collective phenomena such as superconductivity and superfluidity. In atomic nuclei, the interplay between pairing and particle-hole interactions leads to a high degree of complexity and intricate entanglement structures. Despite this apparent complexity, symmetries emerge and manifest themselves in observable regular patterns. These symmetries and their breakings have long been used to determine relevant degrees of freedom and simplify classical descriptions of many-body systems. Here, this work explores the potential utility of quantum computers with arrays of qudits in simulating interacting fermionic systems, when the qudits can naturally map the relevant degrees of freedom determined by an underlying symmetry group. The Agassi model of fermions interacting via particle-hole and pairing interactions is based on an underlying so(5) algebra. Such systems can intuitively be partitioned into pairs of modes with five basis states, which thus naturally map to arrays of d = 5 qudits (qu5its). Classical noiseless simulations of the time evolution of systems with up to twelve qu5its are performed, by implementing quantum circuits that are developed herein, using PYTHON codes invoking Google's CIRQ software. The resource requirements of the qu5it circuits are analyzed and compared with two different mappings to qubit systems: a physics-aware Jordan-Wigner mapping requiring four qubits per mode pair and a state-to-state mapping requiring three qubits per mode pair. While the dimensionality of Hilbert spaces in mappings to qu5it systems are less than those for the corresponding qubit systems, the number of entangling operations, depending on the available hardware, can either be greater or smaller than for the physics-aware Jordan-Wigner mapping. The state-to-state mapping, while having a smaller Hilbert space than Jordan-Wigner mappings, appears to be the least efficient in gate counts. Further, a previously unknown sign problem has been identified from Trotterization errors in time evolving high-energy excitations. There appear to be advantages in employing quantum computers with arrays of qudits to perform simulations of many-body dynamics that exploit the role of underlying symmetries, specifically in lowering the required quantum resources and in reducing anticipated errors that take the simulation out of the physical space. If the necessary entangling gates are not directly supported by the hardware, physics-aware mappings to qubits may, however, be advantageous for other aspects.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Structure characterization of MHEMT heterostructure elements with In{sub 0.4}Ga{sub 0.6}As quantum well grown by molecular beam epitaxy on GaAs substrate using reciprocal space mapping

The crystallographic parameters of elements of a metamorphic high-electron-mobility transistor (MHEMT) heterostructure with In{sub 0.4}Ga{sub 0.6}As quantum well are determined using reciprocal space mapping. The heterostructure has been grown by molecular-beam epitaxy (MBE) on the vicinal surface of a GaAs substrate with a deviation angle of 2° from the (001) plane. The structure consists of a metamorphic step-graded buffer (composed of six layers, including an inverse step), a high-temperature buffer of constant composition, and active high-electron-mobility transistor (HEMT) layers. The InAs content in the metamorphic buffer layers varies from 0.1 to 0.48. Reciprocal space mapping has been performed for the 004 and 224 reflections (the latter in glancing exit geometry). Based on map processing, the lateral and vertical lattice parameters of In{sub x}Ga{sub 1–x}As ternary solid solutions of variable composition have been determined. The degree of layer lattice relaxation and the compressive stress are found within the linear elasticity theory. The high-temperature buffer layer of constant composition (on which active MHEMT layers are directly formed) is shown to have the highest (close to 100%) degree of relaxation in comparison with all other heterostructure layers and a minimum compressive stress.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Environment and initial state engineered dynamics of quantum and classical correlations

Based on an open exactly solvable system coupled to an environment with nontrivial spectral density, we connect the features of quantum and classical correlations with some features of the environment, initial states of the system, and the presence of initial system–environment correlations. Some interesting features not revealed before are observed by changing the structure of environment, the initial states of system, and the presence of initial system–environment correlations. The main results are as follows. (1) Quantum correlations exhibit temporary freezing and permanent freezing even at high temperature of the environment, for which the necessary and sufficient conditions are given by three propositions. (2) Quantum correlations display a transition from temporary freezing to permanent freezing by changing the structure of environment. (3) Quantum correlations can be enhanced all the time, for which the condition is put forward. (4) The one-to-one dependency relationship between all kinds of dynamic behaviors of quantum correlations and the initial states of the system as well as environment structure is established. (5) In the presence of initial system–environment correlations, quantum correlations under local environment exhibit temporary multi-freezing phenomenon. While under global environment they oscillate, revive, and damp, an explanation for which is given. - Highlights: • Various interesting behaviors of quantum and classical correlations are observed in an open exactly solvable model. • The important effects of the bath structure on quantum and classical correlations are revealed. • The one-to-one correspondence between the type of dynamical behavior of quantum discord and the initial state is given. • Quantum correlations are given in the presence of initial qubits–bath correlations.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Facile preparation of zinc oxide nanorods surrounded by graphene quantum dots both synthesized via separate pyrolysis procedures for photocatalyst application

Highlights: • ZnO NRs and GQDs were made separately via a simple and one-stage pyrolysis method. • Because of the employed compositing method, GQDs compactly surrounded the ZnO NRs. • Bandgap of ZnO NRs decreased from 3.2 to 2.8 eV after they were surrounded by GQDs. • Despite being inefficient alone, GQDs largely enhanced ZnO photocatalytic activity. • The mechanism was mainly attributed to the decrease in recombination rate of ZnO. - Abstract: A facile pyrolysis method was employed for separate synthesis of zinc oxide nanorods (ZnO NRs) and graphene quantum dots (GQDs) and the structures were composited. The structures were characterized by field emission scanning electron microscopy (FE-SEM), transmission electron microscopy (TEM), X-ray diffractometry (XRD), and Fourier transform infrared (FTIR) spectroscopy. The structures were optically characterized by UV–vis and photoluminescence (PL) spectrometry techniques, showing that the absorption of ZnO NRs increases in the visible region after being surrounded by GQDs. Optical bandgaps of ZnO NRs and ZnO NRs/GQDs composite were estimated as 3.2 and 2.8 eV, respectively. Based on PL analysis, it was deduced that the generated electron-hole recombination rate of ZnO NRs decreases after being surrounded by GQDs. Finally, it was shown that our GQDs, despite being relatively inefficient separately, significantly enhance the photocatalytic activity of ZnO on methylene blue mainly through decreasing the e-h recombination rate of ZnO NRs.

77 NANOSCIENCE AND NANOTECHNOLOGY↗

The first principle study of Ni{sub 2}ScGa and Ni{sub 2}TiGa

We computed the electronic structure, elastic moduli, vibrational properties, and Ni{sub 2}TiGa and Ni{sub 2}ScGa alloys in the cubic L2{sub 1} structure. The obtained equilibrium lattice constants of these alloys are in good agreement with available data. In cubic systems, there are three independent elastic constants, namely C{sub 11}, C{sub 12} and C{sub 44}. We calculated elastic constants in L2{sub 1} structure for Ni{sub 2}TiGa and Ni{sub 2}ScGa using the energy-strain method. The electronic band structure, total and partial density of states for these alloys were investigated within density functional theory using the plane-wave pseudopotential method implemented in Quantum-Espresso program package. From band structure, total and projected density of states, we observed metallic characters of these compounds. The electronic calculation indicate that the predominant contributions of the density of states at Fermi level come from the Ni 3d states and Sc 3d states for Ni{sub 2}TiGa, Ni 3d states and Sc 3d states for Ni{sub 2}ScGa. The computed density of states at Fermi energy are 2.22 states/eV Cell for Ni{sub 2}TiGa, 0.76 states/eV Cell for Ni{sub 2}ScGa. The vibrational properties were obtained using a linear response in the framework at the density functional perturbation theory. For the alloys, the results show that the L2{sub 1} phase is unstable since the phonon calculations have imagine modes.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

How is quantum information localized in gravity?

A notion of localization of information within quantum subsystems plays a key role in describing the physics of quantum systems, and in particular is a prerequisite for discussing important concepts such as entanglement and information transfer. While subsystems can be readily defined for finite quantum systems and in local quantum field theory, a corresponding definition for gravitational systems is significantly complicated by the apparent nonlocality arising due to gauge invariance, enforced by the constraints. A related question is whether "soft hair" encodes otherwise localized information, and the question of such localization also remains an important puzzle for proposals that gravity emerges from another structure such as a boundary field theory as in AdS/CFT. This paper describes different approaches to defining local subsystem structure, and shows that at least classically, perturbative gravity has localized subsystems based on a split structure, generalizing the split property of quantum field theory. This, and related arguments for QED, give simple explanations that in these theories there is localized information that is independent of fields outside a region, in particular so that there is no role for "soft hair" in encoding such information. Additional subtleties appear in quantum gravity. Finally, we argue that localized information exists in perturbative quantum gravity in the presence of global symmetries, but that nonperturbative dynamics is likely tied to a modification of such structure.

79 ASTRONOMY AND ASTROPHYSICS↗

Quasi-one-dimensional Pb 5 Re 3 O 15 : A 5 d realization of the Heisenberg antiferromagnetic spin-1/2 chain

Quasi-one-dimensional (1D) magnetic compounds connect the exact solutions of low-dimensional magnetic geometries, which promise quantum spin liquid behavior and exotic quasiparticles, with real-world materials, in which competing magnetic interactions affect their implementation in quantum information science. Here, the structural determination and quasi-1D magnetic behavior of a previously unreported compound, Pb 5 ⁢Re 3 ⁡O 15 , is presented. Like the anisotropic triangular A 3 ⁢ReO 5 ⁢Cl 2 (A = Ba, Sr, Ca) materials, Pb 5 ⁢Re 3 ⁡O 15 contains [ReO 5 ] square pyramids inserted into anion-centered quasi-two-dimensional layers and hosts spin-1/2 moments on the Re 6+ ions. Pb 5 ⁢Re 3 ⁡O 15 , however, has a more ideal quasi-1D geometry than the A 3 ⁢ReO 5 ⁢Cl 2 materials, with larger interchain distances and interlayer spacing. Quasi-1D magnetic behavior in Pb 5 ⁢Re 3 ⁡O 15 is confirmed by fitting the temperature-dependent magnetic susceptibility with the Bonner-Fisher model for a spin-1/2 antiferromagnetically coupled chain, yielding an intrachain coupling constant of |J|/k B =54.5K. Pb 5 ⁢Re 3 ⁡O 15 is highly insulating at room temperature, and heat capacity data below 10 K reveal a linear-T contribution that suggests the presence of low-temperature spinon excitations. Finally, with a lack of three-dimensional ordering down to at least 0.6 K, Pb 5 ⁢Re 3 ⁡O 15 is proposed as a model system for studying the quantum magnetism of quasi-1D Heisenberg chains in a real-world 5d 1 antiferromagnetic material.

36 MATERIALS SCIENCE↗

High Quality GaAs Growth by MBE on Si Using GeSi Buffers and Prospects for Space Photovoltaics

III-V solar cells on Si substrates are of interest for space photovoltaics since this would combine high performance space cells with a strong, lightweight and inexpensive substrate. However, the primary obstacles blocking III-V/Si cells from achieving high performance to date have been fundamental materials incompatabilities, namely the 4% lattice mismatch between GaAs and Si, and the large mismatch in thermal expansion coefficient. In this paper, we report on the molecular beam epitaxial (MBE) growth and properties of GaAs layers and single junction GaAs cells on Si wafers which utilize compositionally graded GeSi Intermediate buffers grown by ultra-high vacuum chemical vapor deposition (UHVCVD) to mitigate the large lattice mismatch between GaAs and Si. Ga As cell structures were found to incorporate a threading dislocation density of 0.9-1.5 x 10 (exp 6) per square centimeter, identical to the underlying relaxed Ge cap of the graded buffer, via a combination of transmission electron microscopy, electron beam induced current, and etch pit density measurements. AlGaAs/GaAs double heterostructures wre grown on the GeSi/Si substrates for time-resolved photoluminescence measurements, which revealed a bulk GaAs minority carrier lifetime in excess of 10 ns, the highest lifetime ever reported for GaAs on Si. A series of growth were performed to ass3ss the impact of a GaAs buffer to a thickness of only 0.1 micrometer. Secondary ion mass spectroscopy studies revealed that there is negligible cross diffusion of Ga, As and Ge at he III-V/Ge interface, identical to our earlier findings for GaAs grown on Ge wafers using MBE. This indicates that there is no need for a buffer to "bury" regions of high autodopjing,a nd that either pn or np configuration cells are easily accomodated by these substrates. Preliminary diodes and single junction Al Ga As heteroface cells were grown and fabricated on the Ge/GeSi/Si substrates for the first time. Diodes fabricated on GaAs, Ge and Ge/GeSi/Si substrate show nearly identical I-V characteristics in both forward and reverse bias regions. External quantum efficiencies of AlGaAs/GaAs cell structures grown on Ge/GeSi/Si and Ge substrates demonstrated nearly identical photoresponse, which indicates that high lifetimes, diffusion lengths and efficient minority carrier collection is maintained after complete cell processing.

Carlin, J. A.↗

Quantum anomalous Hall insulator phase in asymmetrically functionalized germanene

Here, using first-principles computations, we discuss topological properties of germanene in buckled as well as planar honeycombs with asymmetric passivation via hydrogen and nitrogen (GeHN) atoms. GeHN in the planar structure is found to harbor a quantum anomalous Hall (QAH) insulator phase. Our analysis indicates that the buckled GeHN also possesses a QAH phase under tensile strain. We computed the associated Chern numbers and edge states to confirm the presence of the QAH state. In particular, chiral edge bands connecting conduction and valence bands were found at the edges of a planar zigzag GeHN nanoribbon. By considering a range of buckling distances, we demonstrate how the system undergoes the transition from the trivial to the QAH phase between the buckled and planar structures. Finally, we show CdTe(111) to be a suitable substrate for supporting buckled germanene in the QAH phase. Our results suggest that functionalized germanene could provide a robust QAH-based platform for spintronics applications.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Transmission spectroscopy of CF 4 molecules in intense x-ray fields

The nonlinear interaction of x rays with matter is at the heart of understanding and controlling ultrafast molecular dynamics from an atom-specific viewpoint, providing new scientific and analytical opportunities to explore the structure and dynamics of small quantum systems. At increasingly high x-ray intensity, the sensitivity of ultrashort x-ray pulses to specific electronic states and emerging short-lived transient intermediates is of particular relevance for our understanding of fundamental multiphoton absorption processes. In this work, intense x-ray free-electron laser (XFEL) pulses at the European XFEL are combined with a gas cell and grating spectrometer for a high-intensity transmission spectroscopy study of multiphoton-induced ultrafast molecular fragmentation dynamics in CF 4 . This approach unlocks the direct intrapulse observation of transient fragments, including neutral atoms, by their characteristic absorption lines in the transmitted broadband x-ray spectrum. The dynamics with and without initially producing fluorine 𝐾-shell holes are studied by tuning the central photon energy. The absorption spectra are measured at different FEL intensities to observe nonlinear effects. Transient isolated fluorine atoms and ions are spectroscopically recorded within the ultrashort pulse duration of a few tens of femtoseconds. An isosbestic point that signifies the correlated transition between intact neutral CF 4 molecules and charged atomic fragments is observed near the fluorine 𝐾 edge. The dissociation dynamics and the multiphoton absorption-induced dynamics encoded in the spectra are theoretically interpreted. Overall, this study demonstrates the potential of high-intensity x-ray transmission spectroscopy to study ultrafast molecular dynamics with sensitivity to specific intermediate species and their electronic structure.

74 ATOMIC AND MOLECULAR PHYSICS↗

Unusual structure, bonding and properties in a californium borate

The participation of the valence orbitals of actinides in bonding has been debated for decades. Recent experimental and computational investigations demonstrated the involvement of 6p, 6d and/or 5f orbitals in bonding. However, structural and spectroscopic data, as well as theory, indicate a decrease in covalency across the actinide series, and the evidence points to highly ionic, lanthanide-like bonding for late actinides. Here we show that chemical differentiation between californium and lanthanides can be achieved by using ligands that are both highly polarizable and substantially rearrange on complexation. A ligand that suits both of these desired properties is polyborate. Here, we demonstrate that the 5f, 6d and 7p orbitals are all involved in bonding in a Cf(III) borate, and that large crystal-field effects are present. Synthetic, structural and spectroscopic data are complemented by quantum mechanical calculations to support these observations.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Moving beyond the constraints of chemistry via crystal structure discovery with isotropic multiwell pair potentials

The rigid constraints of chemistry-dictated by quantum mechanics and the discrete nature of the atom-limit the set of observable atomic crystal structures. What structures are possible in the absence of these constraints? Here, we systematically crystallize one-component systems of particles interacting with isotropic multiwell pair potentials. We investigate two tunable families of pairwise interaction potentials. Our simulations self-assemble a multitude of crystal structures ranging from basic lattices to complex networks. Sixteen of the structures have natural analogs spanning all coordination numbers found in inorganic chemistry. Fifteen more are hitherto unknown and occupy the space between covalent and metallic coordination environments. The discovered crystal structures constitute targets for self-assembly and expand our understanding of what a crystal structure can look like.

crystal structures↗

Acidity of arylsulfonamides as function of quantum chemical parameters of sulfonamide nitrogen

The structures of aromatic sulfonamide molecules XPhSO{sub 2}NH{sub 2} (X = H, 4-Me, 4-F, 4-Cl, 4-Br, 4-MeO, 4-OH, 4-NH{sub 2}, 4-CN, 3-NO{sub 2}, 4-NO{sub 2}, 3,5-(NO{sub 2}){sub 2}, 3,4-Cl{sub 2}, 3-Cl-4-Me, 3,4-Me{sub 2}, 3-Me-4-F, 2-Me) were calculated at the M06/6-311++G** (SMD) level of theory. The atomic electrostatic potentials (AEP) and the Hirshfeld charges of the sulfonamide nitrogen atoms were determined. Correlation equations relating the AEP to Bronsted acidities (pK{sub a}) of these compounds were obtained using published data and the previously unknown pK{sub a} values for a number of arylsulfonamides were calculated. These pK{sub a} values are consistent with independently determined free energies of acid dissociation of sulfonamides.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Structure of the Majorana Clifford group

In quantum information science, Clifford operators and stabilizer codes play a central role for systems of qubits (or qudits). In this study, we study their analogs for systems composed of Majorana fermions. In this case, a crucial role is played by fermion parity symmetry, which is an unbreakable symmetry present in any system with fundamentally fermionic degrees of freedom. We prove that the subgroup of parity-preserving Majorana Cliffords can be represented by the orthogonal group over the binary field 𝔽 2 , and we show how it can be generated by braiding operators and used to construct any (even-parity) Majorana stabilizer code. We also analyze the frame potential for this so-called p-Clifford group when acting on a fixed-parity sector of the Hilbert space, proving that it is equivalent to the frame potential of the ordinary Clifford group acting on the same sector.

Computational complexity↗

Spinodal Decomposition in InSb/AlAs Heterostructures

The atomic structure and energy spectrum of heterostructures formed in a system of InAs/AlAs binary compounds are studied. The In{sub x}Al{sub 1–x}Sb{sub y}As{sub 1–y} alloy, from which quantum wells are formed in InSb/AlAs structures, decomposes into two phases with different compositions. The characteristic dimensions of regions containing separate phases of the alloy in the structure plane are 5–7 nm. Spinodal decomposition of the alloy brings about the formation of coexisting indirect-gap regions with type-I and type-II energy spectra in quantum wells of the heterostructures.

36 MATERIALS SCIENCE↗