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At least 199 records · Page 11

Entanglement engineering of optomechanical systems by reinforcement learning

Entanglement is fundamental to quantum information science and technology, yet controlling and manipulating entanglement—so-called entanglement engineering—for arbitrary quantum systems remains a formidable challenge. There are two difficulties: the fragility of quantum entanglement and its experimental characterization. We develop a model-free deep reinforcement-learning (RL) approach to entanglement engineering, in which feedback control together with weak continuous measurement and partial state observation is exploited to generate and maintain desired entanglement. We employ quantum optomechanical systems with linear or nonlinear photon–phonon interactions to demonstrate the workings of our machine-learning-based entanglement engineering protocol. In particular, the RL agent sequentially interacts with one or multiple parallel quantum optomechanical environments, collects trajectories, and updates the policy to maximize the accumulated reward to create and stabilize quantum entanglement over an arbitrary amount of time. The machine-learning-based model-free control principle is applicable to the entanglement engineering of experimental quantum systems in general.

97 MATHEMATICS AND COMPUTING↗

Ab initio self-consistent many-body theory of polarons at all couplings

We present a theoretical framework to describe polarons from first principles within a many-body Green’s function formalism. Starting from a general electron-phonon Hamiltonian, we derive a self-consistent Dyson equation in which the phonon-mediated self-energy is composed by two distinct terms. One term is the Fan-Migdal self-energy and describes dynamic electron-phonon processes, the other term is a contribution to the self-energy originating from the static displacements of the atomic nuclei in the polaronic ground state. The lowest-order approximation to the present theory yields the standard many-body perturbation theory approach to electron-phonon interactions in the limit of large polarons, and the ab initio polaron equations introduced in the limit of small polarons. Here, a practical recipe to implement the present unifying formalism in first-principles calculations is outlined. We apply our method to the Fröhlich model, and obtain remarkably accurate polaron energies at all couplings, in line with Feynman’s polaron theory and diagrammatic Monte Carlo calculations. We also recover the well-known results of Fröhlich and Pekar at weak and strong coupling, respectively. The present approach enables predictive many-body calculations of polarons in real materials at all couplings.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Strong Proton‐Phonon Coupling Drives Fast Ion Transport in Perovskites

Conduction of protons in solids is a cooperative process propelled by phonons, with molecular details obscured by the irregular movements in the thermal bath. It is shown that substitution with Y forms an imaginary phonon mode, instrumental for the function as proton conductor and effectively lowering the activation barrier for proton transport. To untangle the interplay in the exemplary proton conductor BaSn 0.9 Y 0.1 O 3 , its crystallographic structure is determined with high resolution neutron diffractometry and its phonon density of states with density functional theory calculations, experimentally validated by element specific nuclear resonant vibration spectroscopy. Based on phonon analysis, a quantitative transport model is present, which predicts the activation energy and performance by the ratio of ionic radii. Rather than individual vibrational modes, it is the oxygen sub-lattice which exerts its momentum on the protons. The extent of this momentum transfer is governed by the ratio of ionic radii. This model extends the transition state theory by the phonon-phonon interaction and complements the previously proposed idea that lattice dynamics is decisive for proton transport and specifies which properties of the material exactly define the vibration properties.

activation barriers↗

Enhanced mobility of cations and anions in the redox state: The polaronium mechanism

Hugely enhanced slow-ion diffusivity has been widely observed under extreme redox conditions and for unclear reasons. Aided by first-principles calculations on model systems of ZrO 2 , CeO 2 , BaTiO 3 and Li 4/3 Mn 2/3 O 2 , here we successfully explained the intriguing phenomenon by a polaronium mechanism. We found a polaronium, defined as a transitory complex of a polaronic electron or hole and a migrating counterion, becomes highly mobile when the counterion comes from a d 0 or f 0 cation (e.g., Zr 4+ , Ti 4+ and Ce 4 ) or a p 6 anion (e.g., O 2- ) in the host compound. Upon a redox reaction, the complex attains a d 1 /f 1 or p 5 configuration, which spontaneously forms because it is favored by an electron-phonon interaction (manifest as the Jahn-Teller effect in high symmetry systems) that enables local relaxation and lowers the system energy. Here our calculations found such interaction reaching its peak at the saddle point where the local environment is softest, so soft that it allows a reorientation of the anisotropic d/f/p orbital to minimize the electron repulsion locally. Since the complex may dissolve after a successful ion-migration event, the redox electron/hole can be recycled to form another free-radical-like polaronium elsewhere, thereby enhancing ion migration repeatedly. The proposed polaronium mechanism, which also operates in ceramics doped with mixed-valence cations, is most relevant under dynamic and extreme thermal/field/irradiation conditions where extra electrons/holes are abundantly generated by non-equilibrium redox reactions. For such operations, some with emerging applications, our diffusion-enhancing mechanism may provide new theoretical insight to help understand their material/microstructure stability and performance.

36 MATERIALS SCIENCE↗

Refining T c Prediction in Hydrides via Symbolic‐Regression‐Enhanced Electron‐Localization‐Function‐Based Descriptors

Hydrogen‐based materials are able to possess extremely high superconducting critical temperatures, T c s , due to hydrogen's low atomic mass and strong electron–phonon interaction. Recently, a descriptor based on the Electron Localization Function (ELF) has enabled the rapid estimation of the T c of hydrogen‐containing compounds from electronic networking properties, but its applicability has been limited by the small size and homogeneity of the training dataset used. Herein, the model is re‐examined, compiling a publicly available combined dataset of 244 binary and ternary hydride superconductors. The analysis shows that though ELF‐based networking remains a valuable descriptor, its predictive power declines with increasing compositional complexity. However, by introducing the molecularity index, defined as the highest value of the ELF at which two hydrogen atoms connect, and applying symbolic regression, the accuracy of the predictions can be substantially enhanced. These results establish a more robust framework for assessing superconductivity in hydride materials, facilitating accelerated screening of novel candidates through integration with crystal structure prediction methods or high‐throughput searches.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Insights into the Mechanism of Chiral‐Induced Spin Selectivity: The Effect of Magnetic Field Direction and Temperature

Chiral oligopeptide monolayers are adsorbed on a ferromagnetic surface and their magnetoresistance is measured as a function of the angle between the magnetization of the ferromagnet and the surface normal. These measurements are conducted as a function of temperature for both enantiomers. The angle dependence is found to follow a changing trend with a period of 360°. Quantum simulations reveal that the angular distribution can be obtained only if the monolayer has significant effective spin orbit coupling (SOC), that includes contribution from the vibrations. The model shows that SOC only in the leads cannot reproduce the observed angular dependence. The simulation can reproduce the experiments if it included electron–phonon interactions and dissipation.

36 MATERIALS SCIENCE↗

Thickness and Spin Dependence of Raman Modes in Magnetic Layered Fe 3 GeTe 2

2D layered Fe 3 GeTe 2 has attracted increasing attention due to its high magnetic ordering temperature and novel physical properties. Lattice dynamics is a fundamental property of Fe 3 GeTe 2 , and its relationships with the number of layers and interlayer spin ordering have not yet been explored in depth. Here, by first-principles density functional theory calculations, the phonon vibrations and Raman intensities of Fe 3 GeTe 2 are systematically studied from the bulk to monolayer structures. Furthermore, the spin-phonon coupling effect is investigated by considering different interlayer magnetic orderings: ferromagnetic and antiferromagnetic. It is found that the frequencies of Raman modes in Fe 3 GeTe 2 exhibit considerable dependence on the layer number and spin ordering. In this work, the results not only reveal the notable spin-phonon interactions in Fe 3 GeTe 2 , but also demonstrate that Raman modes can be utilized for characterizing the sample thickness and interlayer spin ordering in this 2D magnet.

2D magnets↗

Excitonic Dynamics in Janus MoSSe and WSSe Monolayers

We report here details of steady-state and time-resolved spectroscopy of excitonic dynamics for Janus transition metal dichalcogenide monolayers, including MoSSe and WSSe, which were synthesized by low-energy implantation of Se into transition metal disulfides. Absorbance and photoluminescence spectroscopic measurements determined the room-temperature exciton resonances for MoSSe and WSSe monolayers. Transient absorption measurements revealed that the excitons in Janus structures form faster than those in pristine transition metal dichalcogenides by about 30% due to their enhanced electron–phonon interaction by the built-in dipole moment. Here, by combining steady-state photoluminescence quantum yield and time-resolved transient absorption measurements, we find that the exciton radiative recombination lifetime in Janus structures is significantly longer than in their pristine samples, supporting the predicted spatial separation of the electron and hole wave functions due to the built-in dipole moment. These results provide fundamental insight in the optical properties of Janus transition metal dichalcogenides.

36 MATERIALS SCIENCE↗

Structure and Superconductivity of Hydrogenated TiZr Alloys Under High Pressure

The effects of pressure on the structure and electrical transport properties, including electrical resistance and critical magnetic field values for superconductivity in pristine and hydrogenated TiZr alloys, were investigated. As pressure increased from ambient to 55 GPa, the structure of the pristine TiZr alloys transformed from hcp to bcc via an intermediate ω phase. The superconducting transition temperature (T c ) significantly increased from 1.76 K at ambient pressure to 15.5 K at 52.2 GPa, accompanied by an extrapolated upper critical field of 24.5 T at T = 0 K. In contrast, the hydrogenated samples exhibited substantially lower T c values compared to the pristine ones, with a T c of 4.6 K at 50.5 GPa and an extrapolated upper critical field of 1.8 T at T = 0 K. Upon decompression, the superconductivity in the hydrogenated sample persisted down to 25 GPa, disappearing when the pressure was reduced to 19 GPa. Synchrotron X-ray diffractions (XRD) analysis revealed the formation of three hydrides: I4/mmm-(Ti, Zr)H 2 , P6 3 /mmc-(Ti, Zr)H 3 , and I4̅3d-(Ti,Zr) 4 H 15 . Finally, by combining XRD and electrical resistance data, we tentatively propose that the P6 3 /mmc-(Ti, Zr)H 3 predominantly induces superconductivity. In contrast to superhydrides, where electron–phonon interactions increase the superconducting temperature at high pressure, hydrogen atoms in hcp-(Ti, Zr)H 3 reduce T c .

36 MATERIALS SCIENCE↗

Mixed-Chalcogen 2D Silver Phenylchalcogenides (AgE 1– x E x Ph; E = S, Se, Te)

Alloying is a powerful strategy for tuning the electronic band structure and optical properties of semiconductors. Here, we investigate the thermodynamic stability and excitonic properties of mixed-chalcogen alloys of two-dimensional (2D) hybrid organic-inorganic silver phenylchalcogenides (AgEPh; E = S, Se, Te). Using a variety of structural and optical characterization techniques, we demonstrate that the AgSePh-AgTePh system forms homogeneous alloys (AgSe 1-x Te x Ph, 0 ≤ x ≤ 1) across all compositions, whereas the AgSPh-AgSePh and AgSPh-AgTePh systems exhibit distinct miscibility gaps. Density functional theory calculations reveal that chalcogen mixing is energetically unfavorable in all cases, but comparable in magnitude to the ideal entropy of mixing at room temperature. Because AgSePh and AgTePh have the same crystal structure (which is different from AgSPh), alloying is predicted to be thermodynamically preferred over phase separation in the case of AgSePh-AgTePh, whereas phase separation is predicted to be more favorable than alloying for both the AgSPh-AgSePh and AgSPh-AgTePh systems, in agreement with experimental observations. Homogeneous AgSe1-xTexPh alloys exhibit continuously tunable excitonic absorption resonances in the ultraviolet-visible range, while the emission spectrum reveals competition between exciton delocalization and self-trapping behavior. Altogether, these observations provide new insight into the thermodynamics of 2D silver phenylchalcogenides and the effect of lattice composition on electron-phonon interactions in 2D hybrid organic-inorganic semiconductors.

36 MATERIALS SCIENCE↗

Mitigating Band Tailing in Kesterite Solar Absorbers: Ab Initio Quantum Dynamics

Open-circuit voltage deficits are limiting factors in kesterite solar cells. Addressing this issue by suppressing band tailing and nonradiative charge recombination is essential for enhancing the performance. We employ ab initio nonadiabatic molecular dynamics to elucidate the origin of band tailing and charge losses and propose a mitigation strategy. The simulations show that Cu–Zn disorder, associated with antisite defect clusters [Cu Zn +Zn Cu ], is a significant source of band tailing in kesterites, as evidenced by the much larger Urbach energy in disordered than ordered kesterites. Cu–Zn disorder gives rise to new sulfur-centered coordination polyhedra, increases structural inhomogeneity, changes electrostatic potential at sulfur centers, and shifts the S(3p) orbital energy. Differences in the S(3p)/Cu(3d) and S(3p)/Sn(5s) hybridization strengths and the S(3p) orbital energy shift reduce the band gap by 0.37 eV. Furthermore, Cu–Zn disorder enhances vibrational motion of sulfur anions and surrounding cations, increasing band gap fluctuations by 15 meV. The stronger electron–phonon interactions reduce charge carrier lifetimes and limit the kesterite solar cell efficiency. Partial substitution of Zn with Cd facilitates structural ordering and significantly suppresses band tailing, particularly in disordered systems. The improvement can be attributed to the larger atomic radius and mass of Cd, which weakens bonding around the anion, suppresses S-related vibrations within the covalent tetrahedra, and reduces nonadiabatic coupling, thereby increasing charge carrier lifetimes. The reported results establish the key influence of cation disorder on band tailing and reduced charge carrier lifetimes in kesterites and highlight cation disorder engineering as a strategy to achieve high-efficiency kesterite solar cells.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Ultrafast Carrier Self-Trapping Driven by Strong Exciton–Phonon Coupling in 2D MA 3 Bi 2 I 6 Cl 3 Perovskite

Two-dimensional (2D) hybrid bismuth halide perovskites have emerged as promising lead-free materials for optoelectronic applications due to their solution processability and tunable structures. Here, in this study, we investigate 2D layered hybrid perovskite MA 3 Bi 2 I 6 Cl 3 using temperature-dependent photoluminescence (PL) and femtosecond transient absorption spectroscopy. Our results reveal strong coupling between excitons and phonons, evidenced by giant Huang–Rhys factors, coherent phonon oscillations, and ultrafast carrier self-trapping into small-polaron and self-trapped exciton (STE) states. These processes appear as time-dependent ground-state bleach and photoinduced absorption features, highlighting the influence of the lattice in carrier dynamics. Wavelength- and time-resolved measurements reveal that PL emission is dominated by STEs, while free exciton emission is weak and short-lived. By comparing 2D MA 3 Bi 2 I 6 Cl 3 with 0D MA 3 Bi 2 I 9 , which contains molecularly isolated [BiI 6 ] 3− octahedra and 2D MA 3 Bi 2 Br 9 perovskites, we demonstrate how halide composition and structural dimensionality influence the balance between free exciton populations and carrier localization. These insights uncover the intrinsic kinetic landscape of photoexcited states in MA 3 Bi 2 I 6 Cl 3 . Overall, our study contributes to a mechanistic understanding of exciton–phonon interactions in lead-free 2D perovskites.

Pradeep, Kodimana Ramakrishnan [Northwestern Univ.↗

Femtosecond control of phonon dynamics near a magnetic order critical point

The spin-phonon interaction in spin density wave (SDW) systems often determines the free energy landscape that drives the evolution of the system. When a passing energy flux, such as photoexcitation, drives a crystalline system far from equilibrium, the resulting lattice displacement generates transient vibrational states. Manipulating intermediate vibrational states in the vicinity of the critical point, where the SDW order parameter changes dramatically, would then allow dynamical control over functional properties. Here we combine double photoexcitation with an X-ray free-electron laser (XFEL) probe to control and detect the lifetime and magnitude of the intermediate vibrational state near the critical point of the SDW in chromium. We apply Landau theory to identify the mechanism of control as a repeated partial quench and sub picosecond recovery of the SDW. Our results showcase the capabilities to influence and monitor quantum states by combining multiple optical photoexcitations with an XFEL probe. They open new avenues for manipulating and researching the behaviour of photoexcited states in charge and spin order systems near the critical point.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

High-order replica bands in monolayer FeSe/SrTiO3 revealed by polarization-dependent photoemission spectroscopy

Abstract The mechanism of the enhanced superconductivity in monolayer FeSe/SrTiO 3 has been enthusiastically studied and debated over the past decade. One specific observation has been taken to be of central importance: the replica bands in the photoemission spectrum. Although suggestive of electron-phonon interaction in the material, the essence of these spectroscopic features remains highly controversial. In this work, we conduct angle-resolved photoemission spectroscopy measurements on monolayer FeSe/SrTiO 3 using linearly polarized photons. This configuration enables unambiguous characterization of the valence electronic structure with a suppression of the spectral background. We consistently observe high-order replica bands derived from various Fe 3 d bands, similar to those observed on bare SrTiO 3 . The intensity of the replica bands is unexpectedly high and different between d xy and d yz bands. Our results provide new insights on the electronic structure of this high-temperature superconductor and the physical origin of the photoemission replica bands.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Half-Heusler alloys as emerging high power density thermoelectric cooling materials

Abstract To achieve optimal thermoelectric performance, it is crucial to manipulate the scattering processes within materials to decouple the transport of phonons and electrons. In half-Heusler (hH) compounds, selective defect reduction can significantly improve performance due to the weak electron-acoustic phonon interaction. This study utilized Sb-pressure controlled annealing process to modulate the microstructure and point defects of Nb 0.55 Ta 0.40 Ti 0.05 FeSb compound, resulting in a 100% increase in carrier mobility and a maximum power factor of 78 µW cm −1 K −2 , approaching the theoretical prediction for NbFeSb single crystal. This approach yielded the highest average zT of ~0.86 among hH in the temperature range of 300-873 K. The use of this material led to a 210% enhancement in cooling power density compared to Bi 2 Te 3 -based devices and a conversion efficiency of 12%. These results demonstrate a promising strategy for optimizing hH materials for near-room-temperature thermoelectric applications.

36 MATERIALS SCIENCE↗

Manipulating single excess electrons in monolayer transition metal dihalide

Polarons are entities of excess electrons dressed with local response of lattices, whose atomic-scale characterization is essential for understanding the many body physics arising from the electron-lattice entanglement, yet difficult to achieve. Here, using scanning tunneling microscopy and spectroscopy (STM/STS), we show the visualization and manipulation of single polarons in monolayer CoCl 2 , that are grown on HOPG substrate via molecular beam epitaxy. Two types of polarons are identified, both inducing upward local band bending, but exhibiting distinct appearances, lattice occupations and polaronic states. First principles calculations unveil origin of polarons that are stabilized by cooperative electron-electron and electron-phonon interactions. Both types of polarons can be created, moved, erased, and moreover interconverted individually by the STM tip, as driven by tip electric field and inelastic electron tunneling effect. This finding identifies the rich category of polarons in CoCl 2 and their feasibility of precise control unprecedently, which can be generalized to other transition metal halides.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Observation of interlayer plasmon polaron in graphene/WS 2 heterostructures

Harnessing electronic excitations involving coherent coupling to bosonic modes is essential for the design and control of emergent phenomena in quantum materials. In situations where charge carriers induce a lattice distortion due to the electron-phonon interaction, the conducting states get “dressed", which leads to the formation of polaronic quasiparticles. The exploration of polaronic effects on low-energy excitations is in its infancy in two-dimensional materials. Here, we present the discovery of an interlayer plasmon polaron in heterostructures composed of graphene on top of single-layer WS 2 . By using micro-focused angle-resolved photoemission spectroscopy during in situ doping of the top graphene layer, we observe a strong quasiparticle peak accompanied by several carrier density-dependent shake-off replicas around the single-layer WS 2 conduction band minimum. Our results are explained by an effective many-body model in terms of a coupling between single-layer WS 2 conduction electrons and an interlayer plasmon mode. It is important to take into account the presence of such interlayer collective modes, as they have profound consequences for the electronic and optical properties of heterostructures that are routinely explored in many device architectures involving 2D transition metal dichalcogenides.

36 MATERIALS SCIENCE↗

Uncovering the phonon spectra and lattice dynamics of plastically deformable InSe van der Waals crystals

Stacking two-dimensional (2D) van der Waals (vdW) materials in a layered bulk structure provides an appealing platform for the emergence of exotic physical properties. As a vdW crystal with exceptional plasticity, InSe offers the opportunity to explore various effects arising from the coupling of its peculiar mechanical behaviors and other physical properties. Here, we employ neutron scattering techniques to investigate the correlations of plastic interlayer slip, lattice anharmonicity, and thermal transport in InSe crystals. Not only are the interlayer slip direction and magnitude well captured by shifts in the Bragg reflections, but we also observe a deviation from the expected Debye behaviour in the heat capacity and lattice thermal conductivity. Combining the experimental data with first-principles calculations, we tentatively attribute the observed evidence of strong phonon-phonon interactions to a combination of a large acoustic-optical frequency resonance and a nesting effect. These findings correlate the macroscopic plastic slip and the microscopic lattice dynamics, providing insights into the mechano-thermo coupling and modulation in 2D vdW materials.

36 MATERIALS SCIENCE↗