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Search indexed NASA NTRS and DOE OSTI research on propulsion, heat transfer, battery materials and energy systems. Follow report and document links to the original sources.

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At least 127 records · Page 7
All sourcesNASA NTRSDOE OSTI
DOE OSTI2021

Exploring the Ion Solvation Environments in Solid-State Polymer Electrolytes through Free-Energy Sampling

The success of poly(ethylene oxide) (PEO) in solid-state polymer electrolytes for lithium-ion batteries is well established. Recently, in order to understand this success and to explore possible alternatives, we studied polyacetal electrolytes to deepen the understanding of the effect of the local chemical structure on ion transport. Advanced molecular dynamics techniques using newly developed, tailored interaction potentials have helped elucidate the various coordination environments of ions in these systems. In particular, the competition between cation-Anion pairing and coordination by the polymer has been explored using free-energy sampling (metadynamics). At equivalent reduced temperatures, with respect to the polymer-specific glass-Transition temperature, two-dimensional free-energy plots reveal the existence of multiple coordination environments for the lithium (Li) ions in these systems and their relative stabilities. Furthermore, we observe that the Li-ion movement in PEO follows a serial, stepwise pathway when moving from one coordination state to another, whereas this happens in a more continuous and concerted fashion in a polyacetal such as poly(1,3-dioxalane) [P(EO-MO)]. The implication is that interconversion between coordination states of the Li ions may be easier in P(EO-MO). However, the overarching observation from our free-energy analysis is that Li-ion coordination is dominated by the polymer (in either case) and contact-ion pairs are rare. We rationalize the observed higher increase in glass-Transition temperature (Tg) with salt loading in polyacetals as due to intermolecular Li-ion coordination involving multiple polymer chains, rather than just one chain for PEO-based electrolytes. This interchain coupling in the polyacetals, resulting in the higher Tg, works against any gains due to variations in Li-ion coordination that might enhance transport processes over PEO. Further research is required to overcome the interdependence between local coordination and macroscopic properties to compete with PEO electrolytes at the same absolute working temperature.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2023

Effects of elevated-temperature deposition on the atomic structure of amorphous Ta 2 O 5 films

Brownian thermal noise as a result of mechanical loss in optical coatings will become the dominant source of noise at the most sensitive frequencies of ground-based gravitational-wave detectors. Experiments found, however, that a candidate material, amorphous Ta 2 O 5 , is unable to form an ultrastable glass and, consequently, to yield a film with significantly reduced mechanical loss through elevated-temperature deposition alone. X-ray scattering PDF measurements are carried out on films deposited and subsequently annealed at various temperatures. Inverse atomic modeling is used to analyze the short and medium range features in the atomic structure of these films. Furthermore, in silico deposition simulations of Ta 2 O 5 are carried out at various substrate temperatures and an atomic level analysis of the growth at high temperatures is presented. It is observed that upon elevated-temperature deposition, short range features remain identical, whereas medium range order increases. After annealing, however, both the short and medium range orders of films deposited at different substrate temperatures are nearly identical. A discussion on the surface diffusion and glass transition temperatures indicates that future pursuits of ultrastable low-mechanical-loss films through elevated temperature deposition should focus on materials with a high surface mobility, and/or lower glass transition temperatures in the range of achievable deposition temperatures.

36 MATERIALS SCIENCE↗
DOE OSTI2023

Magnetic frustration driven by conduction carrier blocking in Nd 2 Co 0.85 Si 2.88

The intermetallic compound Nd 2 Co 0.85 Si 2.88 having a triangular lattice could be synthesized in single phase only with defect crystal structure. Investigation through different experimental techniques indicate the presence of two magnetic transitions in the system. As verified experimentally and theoretically, the high-temperature transition $T_H$ ~ 140 K is associated with the development of ferromagnetic interaction between itinerant Co moments, whereas the low-temperature transition at $T_L$ ~ 6.5 K is due to the coupling among Nd–4$\textit{f}$ and Co–3$\textit{d}$ moments, which is antiferromagnetic in nature. Detailed studies of temperature-dependent dc magnetic susceptibility, field dependence of isothermal magnetization, nonequilibrium dynamical behavior, viz., magnetic relaxation, aging effect, magnetic-memory effect, and temperature dependence of heat capacity, along with density functional theory (DFT) calculations, suggest that the ground state is magnetically frustrated spin glass in nature, having competing magnetic interactions of equivalent energies. DFT results further reveal that the 3$\textit{d}$/5$\textit{d}$-conduction carriers are blocked in the system and act as a barrier for the 4$\textit{f}$–4$\textit{f}$ RKKY interactions, resulting in spin frustration. Presence of vacancy defects in the crystal are also conducive to the spin frustration. This is an unique mechanism of magnetic frustration, not emphasized so far in any of the ternary $R_2TX_3$ ($\textit{R}$ = rare earth, $\textit{T}$ = transition elements, and $\textit{X}$ = Si, Ge, In) type compounds. Due to the competing character of the itinerant 3$\textit{d}$ and localized 4$\textit{f}$ moments, the compound exhibits anomalous field dependence of magnetic coercivity. Further, the system also exhibits a considerable magnetic entropy change of –Δ$S_M$ ~ 13.3 J/kg K with a relative cooling power (RCP) of 220 J/kg and adiabatic temperature change $ΔT_{\text{ad}}$ of 6 K for magnetic field change of 70 kOe.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2020

Low Temperature Aggregation Transitions in N3 and Y6 Acceptors Enable Double‐Annealing Method That Yields Hierarchical Morphology and Superior Efficiency in Nonfullerene Organic Solar Cells

Abstract Thermal transition of organic solar cells (OSCs) constituent materials are often insufficiently researched, resulting in trial‐and‐error rather than rational approaches to annealing strategies to improve domain purity to enhance the power conversion efficiency. Despite the potential utility, little is known about the thermal transitions of the modern high‐performance acceptors Y6 and N3. Here, by using an optical method, it is discovered that the acceptor N3 has a clear solid‐state aggregation transition at 82 °C. This unusually low transition not only explains prior optimization protocols, but the transition informs and enables a double‐annealing method that can fine‐tune aggregation and the device morphology. Compared with 16.6% efficiency for PM6:N3:PC 71 BM control devices, higher efficiency of 17.6% is obtained through the improved protocol. Morphology characterization with x‐ray scattering methods reveals the formation of a multilength scale morphology. Moreover, the double‐annealing method is illustrated and easily transferred and validated with Y6‐based devices, using the transition of Y6 at 102 °C. As a result, the PCE improved from 16.0% to 16.8%. Design of high‐performance acceptors with yet lower aggregation transitions might be required for OSCs to successfully transition to low thermal budget industrial processing methods where annealing temperatures on plastic substrates have to be kept low.

Qin, Yunpeng↗
DOE OSTI2022

Ingeniously enhanced ferromagnetism in chemically-reduced 2D Ti 3 C 2 T X MXene

Chemical reduction is a facile and cost-effective technique for the modulation of the physical and chemical properties of nanomaterials. In this work, we demonstrate an enhancement of the magnetic behavior of Ti 3 C 2 T x MXene after its chemical reduction via l-ascorbic acid treatment. Small ferromagnetic loops have been observed below 50 K for Ti 3 C 2 T x prepared by hydrofluoric acid (HF) etching of Al layers from Ti 3 AlC 2 . Such a ferromagnetic ordering of spins was significantly enhanced via a chemical reduction of Ti 3 C 2 T x with l-ascorbic acid. Ferromagnetic hysteresis loops were observed for reduced Ti 3 C 2 T x (r-Ti 3 C 2 T x ) up to 150 K indicating a significant upshift of the paramagnetic to the ferromagnetic transition temperature, pushing towards room temperature. The enhancement of ferromagnetism and upshift of the ferromagnetic transition temperature could be attributed to the localized unpaired electron in Ti-3d orbital of the r-Ti 3 C 2 T x crystal and increase in the number of unsaturated Ti atoms upon l-ascorbic acid treatment. Chemical reduction via l-ascorbic acid treatment shows a promising pathway towards the modulation and enhancement of magnetism in various MXene materials for the development of 2D metallic soft ferromagnets and spintronic devices.

36 MATERIALS SCIENCE↗
DOE OSTI2024

Improving Predictions of Spin-Crossover Complex Properties through DFT Calculations with a Local Hybrid Functional

We conducted a study on the performance of the local hybrid exchange-correlation functional PBE0r for a set of 95 experimentally-characterized iron spin crossover (SCO) complexes. The PBE0r functional is a variant of PBE0 where the exchange correction is restricted to on-site terms formulated within the basis of local orbitals. We determine the free parameters of the PBE0r functional against experimental data and other hybrid functionals. With a Hartree-Fock (HF) exchange factor of 4%, the PBE0r functional accurately reproduces the electronic and free energy trends predicted in prior DFT studies for these 95 complexes using the B3LYP functional. Larger values of HF exchange stabilize high-spin states. The PBE0r-predicted bond lengths tend to exceed the experimental bond lengths, and bond lengths are less sensitive to HF exchange. The predicted SCO transition temperatures T 1/2 from PBE0r correlate moderately with the experimental transition temperatures, showing a slight improvement compared to the previous modB3LYP-predicted T 1/2 . Furthermore, this study suggests the PBE0r functional as computationally cost-effective and offers the possibility of simulating larger complexes with accuracy comparable to other global hybrid functionals, provided the HF exchange parameter is carefully optimized.

25 ENERGY STORAGE↗
DOE OSTI2024

Robust superconductivity and the suppression of charge-density wave in the quasi-skutterudites Ca 3 ( Ir 1 – x Rh x ) 4 Sn 13 single crystals at ambient pressure

Single crystals of the quasi-skutterudite compounds Ca 3 (Ir 1-x Rh x ) 4 Sn 13 (3–4–13) were synthesized by flux growth and characterized by x-ray diffraction, energy dispersive x-ray spectroscopy, magnetization, resistivity, and radio frequency magnetic susceptibility techniques. The coexistence and competition between the charge density wave (CDW) and superconductivity was studied by varying the Rh/Ir ratio. The superconducting transition temperature, T c , varies from 7 K in pure Ir (x = 0) to 8.3 K in pure Rh (x = 1). Temperature-dependent electrical resistivity reveals monotonic suppression of the CDW transition temperature, T CDW (x). The CDW starts in pure Ir, x = 0, at T CDW ≈ 40 K and extrapolates roughly linearly to zero at x c ≈ 0.53–0.58 under the superconducting dome. Magnetization and transport measurements show a significant influence of CDW on superconducting and normal states. Meissner expulsion is substantially reduced in the CDW region, indicating competition between the CDW and superconductivity. The low-temperature resistivity is higher in the CDW part of the phase diagram, consistent with the reduced density of states due to CDW gapping. Its temperature dependence just above T c shows signs of non-Fermi liquid behavior in a cone-like composition pattern. We conclude that the Ca 3 (Ir 1-x Rh x ) 4 Sn 13 alloy is a good candidate for a composition-driven quantum critical point at ambient pressure.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2023

Predicting the superconducting critical temperature in transition metal carbides and nitrides using machine learning

Transition metal carbides and nitrides have unique mechanical and chemical characteristics. At low temperatures many of them also exhibit superconductivity, which can be controlled by substitutions into both the transition metal and carbon/nitrogen sites. To investigate the factors governing the superconducting state, we apply machine learning methods. Here we collected a dataset containing 147 materials, which was used to create a pipeline for predicting their superconducting critical temperature. When this pipeline is applied to a randomly selected test set, it shows a good performance, with of 0.82 and RMSE of 1.9 K. To explore the limits of the machine learning approach, we also use it to predict entire substitution series within the dataset. This represents a realistic test for the predictive models, which can be extremely useful when applied to new substitutions in materials systems. The performance of the pipeline in this case is much more uneven, with good predictions for some series, while for others the model shows minimal predictive power. We discuss possible reasons for these results, as well as methods to estimate the performance of machine learning on new substitution series.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2021

Cooperativity and Metal–Linker Dynamics in Spin Crossover Framework Fe(1,2,3-triazolate) 2

Cooperative interactions are responsible for the useful properties of spin crossover (SCO) materials–large hysteresis windows, critical temperatures near room temperature, and abrupt transitions–with hybrid framework materials exhibiting the greatest cooperativity and hysteresis of all SCO systems. However, little is known about the chemical origin of cooperativity in frameworks. Here, we present a combined experimental–computational approach for identifying the origin of cooperativity in the metal–organic framework (MOF) Fe(1,2,3-triazolate) 2 (Fe(TA) 2 ), which exhibits the largest known hysteresis window of all SCO materials and unusually high transition temperatures, as a roadmap for understanding the manipulation of SCO behavior in general. Variable-temperature vibrational spectroscopy provides evidence that “soft modes” associated with dynamic metal–linker bonding trigger the cooperative SCO transition. Thermodynamic analysis also confirms a cooperativity magnitude much larger than those of other SCO systems, while electron density calculations of Fe(TA) 2 support previous theoretical predictions that large cooperativity arises in materials where SCO produces considerable differences in metal–ligand bond polarities between different spin states. Taken together, this combined experimental–computational study provides a microscopic basis for understanding cooperative magnetism and highlights the important role of dynamic bonding in the functional behavior of framework materials.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Low temperature aging in a molecular glass: the case of cis -methyl formate

Glassy films of cis-methyl formate show spontaneous dipole orientation on deposition from the vacuum, the so-called ‘spontelectric effect’, creating surface potentials and electric fields within the films. We follow the decay of these fields, and their accompanying dipole orientation, on the hours timescale at deposition temperatures between 40 K and 55 K. Our data trace the low temperature ‘secondary decay’ mechanism, at tens of degrees below the glass transition temperature of 90 K. We show that secondary decay is due to molecular rotation, with associated activation energies lying between 0.1 and 0.2 eV. Diffusion is absent, as established from published neutron reflectivity data. Using an analytical model for the spontelectric effect, data are placed on a quantitative footing, showing that angular motion in excess of 50° reproduces the observed values of activation energies. Exploitation of the spontelectric effect is new in the study of glass aging and is shown here to give insight into the elusive processes which take place far from the molecular glass transition temperature.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2021

Role of locally polar regions in the superconductivity of SrTiO 3

Understanding the interaction between polar and superconducting order parameters may hold the key to several classes of superconductors that remain poorly understood, including SrTiO 3 and several tellurides. Here we show that doped, strained SrTiO 3 films can exhibit both global or local polar order, respectively, depending on the amount of epitaxial mismatch strain, thereby providing a platform to understand how inversion symmetry breaking affects superconductivity. We find that the superconducting critical temperature correlates with the length scale of polar order. In particular, the transition temperature is enhanced when polar nanodomains are sufficiently large or, in the extreme limit, films are globally ferroelectric. In these cases, the Cooper pairs reside in a noncentrosymmetric environment. Conversely, low transition temperatures are found when the nanodomains are small. The findings point to the length scale of polar nanodomains and spin-orbit coupling as important parameters controlling the superconductivity of SrTiO 3 . Furthermore, the ability to control the size of the polar domains opens up new opportunities to design and control the nature of superconductivity in a wide range of materials.

36 MATERIALS SCIENCE↗
DOE OSTI2022

Processing of phase change materials by fused deposition modeling: Toward efficient thermal energy storage designs

We report that recently, several efforts have emerged that employ additive manufacturing techniques to integrate phase change material (PCM) thermal energy storage into geometrically complex designs for advanced thermal management. In this work, we contribute to this emerging research by reporting on the production of a composite nylon-based filament for fused deposition modeling incorporating encapsulated PCMs for 3D printing heat sink geometries. Microencapsulated PCM (MEPCM) with a 6 degrees C transition temperature was selected as the material for thermal energy storage. This transition temperature was selected due to its suitability to provide thermal energy storage to target air-conditioning applications in buildings. In an attempt to improve the thermal conductivity of the composite, fine boron nitride fillers were added, although the effect on improvement was found to be negligible in the overall composite mixture. The nylon-MEPCM ratio in the filaments was optimized, and filaments containing up to 40 wt% MEPCM were successfully synthesized, which were found optimal for 3D printing complex heat sink and other geometries. Thermal and mechanical properties of the filaments were characterized, including latent heat of fusion, thermal conductivity, phase change temperature, tensile strength, and more. Thermal infrared imaging of heat sink geometries printed using the MEPCM filaments undergoing thermal discharging was also conducted. This work presents the most promising result to date in the open literature for a 3D-printed PCM composite in the combination of size, energy density, and geometric complexity of printed parts.

25 ENERGY STORAGE↗
DOE OSTI2022

Experimental Determination of the Relationship Between Organic Aerosol Viscosity and Ice Nucleation at Upper Free Tropospheric Conditions

Abstract This work presents measurements of the ice nucleating ability of secondary organic material recorded between −40 and −70°C and relative humidity with respect to ice (RH ice ) between 150% and 220%. For a subset of systems, temperature and humidity dependence of particle viscosity as well as dry glass transition temperature were characterized using the dual tandem differential mobility analyzer method. Eleven unique monoterpene, sesquiterpene and aromatic precursors were used to generate secondary organic material (SOM) using either an oxidation flow reactor (OFR) or an environmental chamber (EC). For the SOM for which viscosity was measured, the particle glass transition temperatures varied between 6 and 23°C ( n = 8). Measurements were performed to verify that increased relative humidity did not plasticize the particles below −10°C at residence times similar to those in the ice nucleation instrument. No heterogeneous ice nucleation was observed at the ∼0.5% onset threshold for any of the materials generated. The ice nucleation occurs by the freezing of SOM solution droplets consistent with homogeneous freezing indicating that they form an aqueous solution, or the SOM particles required water saturation to freeze, indicating that they were hydrophobic. Experiments exploring the influence of functional groups and mass loading did not reveal any obvious influence of particle chemistry or generation conditions on the results. Close structural matches between known organic ice nucleating particles as precursor or formed products did not yield materials that promoted freezing. These experiments suggest that heterogeneous ice formation of glassy secondary organic materials is likely uncommon under upper free tropospheric conditions.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2022

Room-temperature valence transition in a strain-tuned perovskite oxide

Abstract Cobalt oxides have long been understood to display intriguing phenomena known as spin-state crossovers, where the cobalt ion spin changes vs. temperature, pressure, etc. A very different situation was recently uncovered in praseodymium-containing cobalt oxides, where a first-order coupled spin-state/structural/metal-insulator transition occurs, driven by a remarkable praseodymium valence transition. Such valence transitions, particularly when triggering spin-state and metal-insulator transitions, offer highly appealing functionality, but have thus far been confined to cryogenic temperatures in bulk materials (e.g., 90 K in Pr 1- x Ca x CoO 3 ). Here, we show that in thin films of the complex perovskite (Pr 1- y Y y ) 1- x Ca x CoO 3-δ , heteroepitaxial strain tuning enables stabilization of valence-driven spin-state/structural/metal-insulator transitions to at least 291 K, i.e., around room temperature. The technological implications of this result are accompanied by fundamental prospects, as complete strain control of the electronic ground state is demonstrated, from ferromagnetic metal under tension to nonmagnetic insulator under compression, thereby exposing a potential novel quantum critical point.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2020

NMR studies of the ground states of Ni 50-x Co x Mn 35 In 15 (x=1, 2.5) and Ni 45 Co 5 Mn 37 In 13 Heusler alloys

Three temperature-induced phase transitions at T=T 1 , T M /T A , and T C , related to the ferromagnetic order of the martensitic phase (FMMP), martensitic (structural) transitions (MT), and the ferromagnetic order of the austenitic phase (FMAP), respectively, have been observed in the off-stoichiometric Heusler alloys, Ni 50-x Co x Mn 35 In 15 (x=1, 2.5) and Ni 45 Co 5 Mn 37 In 13 . In this work, the phase transitions temperatures are found to be depended on alloy composition. A kinetic arrest of the AP was observed for Ni 47.5 Co 2.5 Mn 35 In 15 in the magnetization measurements during field-cooling cycle (FCC) at 50 kOe. Depending upon the cooling protocols, ZFC and FCC (at H = 50 kOe), two different ground states of the alloys can be found in Ni 47.5 Co 2.5 Mn 35 In 15 and Ni 45 Co 5 Mn 37 In 13 alloys. The ground states (T=4.2 K and external field H=0) of the alloys was found to be characterized by three main line: two, partially overlapping, at higher frequencies (300-450 MHz), most likely corresponding of manganese resonance lines and one at lower frequency at about 200 MHz. A significant shift in the spectrum of Ni 45 Co 5 Mn 37 In 13 by about 100 MHz to higher frequencies was observed. The correlation of magnetizations obtained from magnetic moment and NMR studies is discussed.

36 MATERIALS SCIENCE↗
DOE OSTI2021

A first and second law analysis of a thermoresponsive polymer desiccant dehumidification and cooling cycle

Herein, we present a theoretical description for a new desiccant air conditioning cycle that uses thermoresponsive polymers instead of traditional desiccants. We use a combined first and second law analysis to demonstrate that this new cycle has three major advantages relative to the traditional case: (i) it can regenerate at lower temperatures, (ii) it can harvest liquid water and (iii) it has significantly higher coefficients of performance (COPs). For example, this new cycle can achieve a COP of 5.1 when regenerated at 95 degrees C, whereas the traditional desiccant cycle is limited to a COP of ~ 1. The fundamental origins of these advantages can be traced to the method of regeneration. The traditional desiccant cycle regenerates by flowing hot air over the desiccant, which provides a medium for gaseous water desorption. However, this also generates entropy and places a minimum temperature constraint on the hot air. In contrast, the thermoresponsive polymer cycle regenerates through a polymer phase transition. The polymer absorbs water vapor in humid air, and then it expels liquid water when raised above its transition temperature. This regeneration method generates liquid water that can be harvested and relaxes constraints on entropy generation and minimum temperature. The minimum regeneration temperature of the thermoresponsive cycle is only limited by the transition temperature of the polymer, which can be tuned through materials science. Due to its liquid water harvesting capability, the new cycle potentially eliminates water consumption when used with evaporative cooling, or it can be directly used for atmospheric water harvesting.

32 ENERGY CONSERVATION, CONSUMPTION, AND UTILIZATI↗
DOE OSTI2026

Formulation and Performance Evaluation of Epoxy Sealant Systems for Double-Shell Tank Bottom Refurbishment

The performance of epoxy sealants used in the refurbishment of double-shell tank (DST) systems requires balancing processability, thermomechanical stability, and adhesion to cementitious substrates. This study incorporates Heloxy 8 as a reactive diluent into Westlake 862 epoxy to tailor workability and cured-state properties. Rheological time-sweep analysis demonstrates that increasing the diluent content significantly reduces complex viscosity and extends workability, thereby improving pumpability and flow for large-area applications. However, the targeted 2-hour processing window is not fully achieved. Differential scanning calorimetry (DSC) confirms that all formulations cure at room temperature to glass transition temperatures ( T g ) at least 20 °C above the maximum DST operating temperature (27 °C), thereby ensuring service in the glassy regime. Dynamic mechanical analysis (DMA) reveals formulation-dependent reductions in tan delta and increases in storage modulus, indicating increasingly elastic and mechanically stable networks with diluent incorporation. Pull-off adhesion testing shows that modified formulations (70–90% Westlake epoxy) exhibit significantly higher adhesion strengths than the unmodified system. Grout cohesive failure indicates that interfacial bonding exceeds substrate strength. Collectively, these results demonstrate that controlled reactive diluent incorporation enables optimization of processing behavior, interfacial adhesion, and thermomechanical performance, supporting the suitability of the modified epoxy systems as durable sealant layers for cementitious barrier applications in hazardous waste containment infrastructure.

Differential scanning calorimetry↗
DOE OSTI2026

Parametrically amplified Josephson plasma waves in YBa 2 Cu 3 O 6+ x : Evidence for local superconducting fluctuations up to the pseudogap temperature T ∗

Experiments that subject underdoped YBa 2 Cu 3 O 6+x (YBCO) to intense terahertz pulses at temperatures between the transition temperature T c and the pseudogap scale T ∗ have revealed a reflectivity edge that resembles that of the superconducting state, together with second harmonic generation of a probe pulse modulated at a similar frequency. These have been interpreted in terms of parametric amplification of the lower Josephson plasmon mode. Since this mode is often associated with coherent oscillations between bilayers in the YBCO structure, these experiments have led to the suggestion that the intense pump has created (or revealed) in-plane pair coherence up to T ∗ ≈ 400 K. In this paper we propose an alternative explanation by assuming the existence of local pair amplitude and phase at equilibrium for T c < T < T ∗ . The phase correlation spans only a few lattice constants and we do not assume any pump-induced enhancement of this correlation, either in-plane or between bilayers. Instead, the coherent drive, via a parametric amplification process, induces coherence in the Josephson currents between members of bilayers. When combined with a Floquet framework, the reflectivity data can be explained. The key point is that in the lower Josephson plasmon, the coupling between bilayers is mainly capacitive; the Josephson current between bilayers can be set to zero without strongly affecting the parametric amplification process. Importantly, while superconducting coherence may not be created by the pump, the pseudogap phase must possess a local pairing amplitude at equilibrium. Consequently, these experiments have strong implications for the understanding of the pseudogap phase.

parametric amplification↗