Low-energy Excitations Research Articles

Thermal first-order phase transitions, Ising critical points, and reentrance in the Ising-Heisenberg model on the diamond-decorated square lattice in a magnetic field

The thermal phase transitions of a spin-1/2 Ising-Heisenberg model on the diamond-decorated square lattice in a magnetic field are investigated using a decoration-iteration transformation and classical Monte Carlo simulations. A generalized decoration-iteration transformation maps this model exactly onto an effective classical Ising model on the square lattice with temperature-dependent effective nearest-neighbor interactions and magnetic field strength. The effective field vanishes along a ground-state phase boundary of the original model, separating a ferrimagnetic and a quantum monomer-dimer phase. At finite temperatures this phase boundary gives rise to an exactly solvable surface of discontinuous (first-order) phase transitions, which terminates in a line of Ising critical points. The existence of discontinuous reentrant phase transitions within a narrow parameter regime is reported and explained in terms of the low-energy excitations from both phases. These exact results, obtained from the mapping to the zero-field effective Ising model are corroborated by classical Monte Carlo simulations of the effective model.

Collective excitations in a melt of fast phase change material GeCu2Te3

Inelastic x-ray scattering measurements have been carried out to investigate atomic dynamics in a melt of fast phase change material GeCu2Te3. The dynamic structure factor was analysed using the model function with three damped harmonic oscillator components. By investigating the correlation between the excitation energy and the linewidth, and that between the excitation energy and the intensity on contour maps of a relative approximate probability distribution function proportional to , we could judge the reliability of each inelastic excitation in the dynamic structure factor. The results indicate that there are two inelastic excitation modes besides the longitudinal acoustic one in the liquid. The lower energy excitation could be assigned to the transverse acoustic one whereas the higher energy one disperses like fast sound. The latter result may imply that the liquid ternary alloy exhibits a microscopic phase separation tendency.

Titania nanorods array homojunction with sub-stoichiometric TiO2 for enhanced methylene blue photodegradation

TiO2 thin films are known to promote photodegradation of dyes and pollutants in water solution via heterogeneous photocatalysis. This ability is guided by the photoexcitation through photons having energies above the band gap. To improve photocatalytic activity, nanostructures with high surface area can be applied, which can ease molecular adsorption/desorption mechanisms, enhance electronic transfer properties and lower excitation energy. For this purpose, square cross-section TiO2 vertically aligned nanorod (TNR) array configuration has been chosen as a semiconductor substrate. On top of it, a thin layer of sub-stoichiometric TiO2−x has been deposited, aiming at inducing a vacancy doped homojunction between two different oxygen rich/deficient TiO2 layers, possibly leading to lower band gap and enhanced photochemical activity. In principle, promotion of electron and holes separation and suppression of charge recombination could occur. Vertically aligned TNRs have been deposited through a hydrothermal growth in acidic conditions on a pre-seeded glass conducting substrate, optimizing the seeding process through spin coating. Sub-stoichiometric TiO2−x layer (50 nm nominal thickness) has been deposited on top of TNRs via radiofrequency magnetron sputtering at three different stoichiometries, tuning the oxygen partial pressure in sputtering argon atmosphere at 10 %, 15 % and 20 %, respectively. Photocatalytic activity has been investigated in the photodegradation of an aqueous solution of methylene blue, both under UV and simulated solar light irradiation at room temperature and atmospheric pressure, resulting in the degradation of methylene blue target molecule up to 99 % under UV and 85 % under simulated solar irradiation after 6 h. These promising achievements unlock new environmental applications for enhanced dye degradation industrial processes.

Catalyst‐Free Photochemical Activation of Peroxymonosulfate in Xanthene‐Rich Systems for Fenton‐Like Synergistic Decontamination: Efficacy of Proton Transfer Process

AbstractCatalyst‐free visible light assisted Fenton‐like catalysis offers opportunities to achieve the sustainable water decontamination, but the synergistic decontamination mechanisms are still unclear, especially the effect of proton transfer process (PTP). The conversion of peroxymonosulfate (PMS) in photosensitive dye‐enriched system was detailed. The photo‐electron transfer between excited dye and PMS triggered the efficient activation of PMS and enhanced the production of reactive species. Photochemistry behavior analysis and DFT calculations revealed that PTP was the crucial factor to determine the decontamination performance, leading to the transformation of dye molecules. The excitation process inducing activation of whole system was composed of low energy excitations, and the electrons and holes were almost contributed by LUMO and HOMO. This work provided new ideas for the design of catalyst‐free sustainable system for efficient decontamination.

Catalyst-Free Photochemical Activation of Peroxymonosulfate in Xanthene-Rich Systems for Fenton-Like Synergistic Decontamination: Efficacy of Proton Transfer Process.

Catalyst-free visible light assisted Fenton-like catalysis offers opportunities to achieve the sustainable water decontamination, but the synergistic decontamination mechanisms are still unclear, especially the effect of proton transfer process (PTP). The conversion of peroxymonosulfate (PMS) in photosensitive dye-enriched system was detailed. The photo-electron transfer between excited dye and PMS triggered the efficient activation of PMS and enhanced the production of reactive species. Photochemistry behavior analysis and DFT calculations revealed that PTP was the crucial factor to determine the decontamination performance, leading to the transformation of dye molecules. The excitation process inducing activation of whole system was composed of low energy excitations, and the electrons and holes were almost contributed by LUMO and HOMO. This work provided new ideas for the design of catalyst-free sustainable system for efficient decontamination.

The Excitation Spectrum of Two-Dimensional Bose Gases in the Gross–Pitaevskii Regime

We consider a system of N bosons, in the two-dimensional unit torus. We assume particles to interact through a repulsive two-body potential, with a scattering length that is exponentially small in N (Gross–Pitaevskii regime). In this setting, we establish the validity of the predictions of Bogoliubov theory, determining the ground state energy of the Hamilton operator and its low-energy excitation spectrum, up to errors that vanish in the limit N rightarrow infty .

Confinement-induced enhancement of superconductivity in a spin- 12 fermion chain coupled to a Z2 lattice gauge field

We investigate a spin-$\frac{1}{2}$ fermion chain minimally coupled to a $\mathbb{Z}_2$ gauge field. In the sector of the gauge generator $\hat G_j =-1$, the model reduces to the Hubbard model with repulsive onsite interaction coupled to a $\mathbb{Z}_2$ gauge field. We uncover how electric fields affect low-energy excitations by both analytical and numerical methods. In the half-filling case, despite electric fields, the system is still a Mott insulator, just like the Hubbard model. For hole-doped systems, holes are confined under nonzero electric fields, resulting in a hole-pair bound state. Furthermore, this bound state also significantly affects the superconductivity, which manifests itself in the emergence of attractive interactions between bond singlet Cooper pairs. Specifically, numerical results reveal that the dimension of the dominant superconducting order parameter becomes smaller when increasing the electric field, signaling an enhancement of the superconducting instability induced by lattice fermion confinement. The superconducting order can even be the dominant order of the system for suitable doping and large applied electric field. The confinement also induces a $\pi$ momentum for the dominant superconducting order parameter leading to a quasi-long-range pair density wave order. Our results provide insights for understanding unconventional superconductivity in $\mathbb{Z}_2$ LGTs and might be experimentally addressed in quantum simulators.

Proton-neutron entanglement in the nuclear shell model

We compute the proton-neutron entanglement entropy in the interacting nuclear shell model for a variety of nuclides and interactions. Some results make intuitive sense, for example, that the shell structure, as governed by single-particle and monopole energies, strongly affects the energetically available space and thus the entanglement entropy. We also find a surprising result: that the entanglement entropy at low excitation energy tends to decrease for nuclides when N ≠ Z. While we provide evidence this arises from the physical nuclear force by contrasting with random two-body interactions which shows no such decrease, the exact mechanism is unclear. Nonetheless, the low entanglement suggests that in models of neutron-rich nuclides, the coupling between protons and neutrons may be less computationally demanding than one might otherwise expect.

Exploration of photovoltaic behavior of benzodithiophene based non-fullerene chromophores: first theoretical framework for highly efficient photovoltaic parameters

Keeping in view, the recent energy conditions and contribution of non-fullerene acceptors (NFAs) towards organic solar cells (OSCs), a series of NFAs (D1-D9) was designed. The novel fused ring NFAs (D1-D9) having A-D-A architecture were designed by structural engineering of R molecule with effective benzothiophene based acceptor moieties. For current study, all the calculations were accomplished at M06/6-311G (d,p) level. Different computational approaches like density of states (DOS), binding energy (Eb), transition density matrix (TDM), absorption spectra (UV–Vis), electronic properties (FMOs) and open circuit were performed to investigate the photovoltaic response of newly designed D1-D9 chromophores. The terminal substitution of end-capped acceptors exhibited a reduction in energy gap (ΔE = 2.222–1.986 eV) with high electron mobility rate in all the derivatives (D1-D9) than that of R. All the designed chromophores exhibited wider absorption spectrum (λmax = 845.039–786.552 nm) along with lower excitation energy as compared to R (λmax = 770.040 nm) except D1 and D9. Interestingly, lower binding energy (Eb = 0.419–0.473 eV) accompanying with higher excition dissociation rate was seen in derivatives than that of reference compound. Moreover, a comparable value of Voc was noted in derivatives when calculated via LUMOacceptor–HOMOPBDBT. Among all fore-said chromophores (D1-D9), D4 exhibited lowest binding energy and thus ensured easier and faster excition dissociation rate along with highest Voc (1.586 V). In cessation, this structural modification by utilizing various acceptors played a significant role in obtaining auspicious photovoltaic response in compounds. Hence, our study encourages the experimentalists for synthesizing these proposed organic systems for the attaining high efficacy photovoltaic devices.

Electrically controlled entanglement of cavity photons with electromagnons

Electromagnonics is an emerging field with a focus on entangling magnonic excitations to the microwave cavity photon modes with the prospect for use in quantum information science. Here, we discuss a class of Hamiltonians that embody a substantial steady-state photon-magnon entanglement enabled by a chiral coupling of the magnonic system to the cavity electric field. It is demonstrated how the entanglement can be controlled via external parameters. As a realization, we study a layered system that hosts an interfacial Dzyaloshinskii-Moriya interaction whose strength varies linearly with the cavity electric field rendering the low-energy spin excitations susceptible to an electric field and resulting in nonlinear magnon-photon dynamics. Accounting for interactions with the environment, we derive from the stochastic quantum Langevin equations explicit expressions evidencing the existence of a finite, steady-state entanglement and detailing its dependencies on external probes. The results point to particular types of electromagnonic systems that are potentially useful for quantum information applications.

Exciton-assisted low-energy magnetic excitations in a photoexcited Mott insulator on a square lattice

The photoexcitation of a Mott insulator on a square lattice weakens the intensity of both single- and two-magnon excitations as observed in time-resolved resonant-inelastic X-ray scattering and time-resolved Raman scattering, respectively. However, the spectral changes in the low-energy regions below the magnons have not yet been clearly understood. To uncover the nature of the photoinduced low-energy magnetic excitations of the Mott insulator, we numerically investigate the transient magnetic dynamics in a photoexcited half-filled Hubbard model on a square lattice. After turning off a pump pulse tuned for an absorption edge, new magnetic signals clearly emerge well below the magnon energy in both single- and two-magnon excitations. We find that low-energy excitations are predominantly created via excitonic states at the absorption edge. These exciton-assisted magnetic excitations may provide a possible explanation for the low-energy spectral weight in a recent time-resolved two-magnon Raman scattering experiment on insulating YBa2Cu3O6.1.

Resonant Auger spectroscopy on solid xenon on gold, silver, and copper substrates

An investigation of the radiationless decay of core excited Xe atoms in the region of Xe ${L}_{3}{M}_{4,5}{M}_{4,5}$ Auger electron kinetic energies (using x-ray energies in the vicinity of the ${L}_{3}$ threshold) is presented for Xe adsorbed on Cu, Ag, and Au. The intensity distribution of the decay channels is different compared with Xe in the gas phase. Charge transfer of the core excited electron occurs within tens of attoseconds in all systems for excitation energies approaching the ionization threshold of the condensed system, whereas charge transfer times are substrate-dependent for lower excitation energies. The determination of partial yields into the decay channels allows for the observation of a decay channel present in the Xe/Cu and Xe/Ag systems but not in the case of Xe/Au. Theoretical calculations allow us to interpret this difference as emanating from varying amounts of the ground state hybridization between Xe and the substrates, which impacts the energy of the Auger final states enabling identification of these states giving rise to system specific features in the experimental data.

Electron-phonon correlations inducing excitonic excitations in semimetal and semiconducting materials

The influence of phonons on the low-energy excitonic excitations at zero temperature in the extended Falicov-Kimball model has been investigated. In the framework of the unrestricted Hartree-Fock approximation, a set of self-consistent equations for the excitonic condensate order parameter and a lattice distortion is derived when both electron-phonon coupling and electron-hole Coulomb interaction are treated on an equal footing. The low-energy excitation properties of the excitonic condensate are addressed in signatures of the optical conductivity and the dynamical excitonic susceptibility function. The real part of the optical conductivity is evaluated by the Kubo linear response theory and the imaginary part of the dynamical excitonic susceptibility is found by adapting the random phase approximation. In the semimetal state, one always finds a sharp peak in the optical conductivity spectrum indicating the stability of the excitonic condensation in the BCS type if the correlation between electrons and phonons becomes significant. In contrast, the peak is smeared out on the semiconducting side indicating the stability of the BEC-type excitonic condensate. In this semiconducting side, the sharp peak signature appears and the system turns to the BCS-type excitonic condensation state by increasing the electron-phonon correlations. In either the semimetal or the semiconducting normal state, increasing the electron-phonon correlations always reinforces a low-energy sharp peak in the dynamical excitonic susceptibility spectrum, indicating the existence of the tightly bound excitonic excitations before the condensation state. Specifically, on the semiconducting side, the ``halo'' phase with the preformed excitons exiting outside of the BEC-excitonic condensation state has been specified. The halo phase becomes more recognizable by raising the electron-phonon correlations.

Excitation-Wavelength-Dependent Charge-Carrier Lifetime in Hematite: An Insight from Nonadiabatic Molecular Dynamics.

Experiments have reported that the photoexcited carrier lifetime in α-Fe2O3 has a significant excitation-wavelength dependence but leave the physical mechanism unresolved. In this work, we rationalize the puzzling excitation-wavelength dependence of the photoexcited carrier dynamics in Fe2O3 by performing nonadiabatic molecular dynamics simulation based on the strongly constrained and appropriately normed functional, which accurately describes the electronic structure of Fe2O3. Photogenerated electrons with lower-energy excitation relax fast in the t2g conduction band within about 100 fs, while the photogenerated electrons with higher-energy excitation undergo first a slower interband relaxation from the eg lower state to the t2g upper state on a time scale of 135 ps, followed by the much faster t2g intraband relaxation. This study provides insight into the experimentally reported excitation-wavelength dependence of the carrier lifetime in Fe2O3 and a reference for regulating photogenerated carrier dynamics in transition-metal oxides through the light excitation wavelength.

Drude weights in one-dimensional systems with a single defect

Ballistic transport of a quantum system can be characterized by Drude weight, which quantifies the response of the system to a uniform electric field in the infinitely long timescale. The Drude weight is often discussed in terms of the Kohn formula, which gives the Drude weight by the derivative of the energy eigenvalue of a finite-size system with the periodic boundary condition in terms of the Aharonov-Bohm flux. Recently, the Kohn formula is generalized to nonlinear responses. However, the nonlinear Drude weight determined by the Kohn formula often diverges in the thermodynamic limit. In order to elucidate the issue, in this work we examine a simple example of a one-dimensional tight-binding model in the presence of a single defect at zero temperature. We find that its linear and non-linear Drude weights given by the Kohn formula (i) depend on the Aharonov-Bohm flux and (ii) diverge proportionally to a power of the system size. We argue that the problem can be attributed to different order of limits. The Drude weight according to the Kohn formula (``Kohn--Drude weight'') indicates the response of a finite-size system to an adiabatic insertion of the Aharonov-Bohm flux. While it is a well-defined physical quantity for a finite-size system, its thermodynamic limit does not always describe the ballistic transport of the bulk. The latter should be rather characterized by a ``bulk Drude weight'' defined by taking the thermodynamic limit first before the zero-frequency limit. While the potential issue of the order of limits has been sometimes discussed within the linear response, the discrepancy between the two limits is amplified in nonlinear Drude weights. We demonstrate the importance of the low-energy excitations of $O(1/L)$, which are excluded from the Kohn--Drude weight, in regularizing the bulk Drude weight.

Controlling Magnetism with Light in a Zero Orbital Angular Momentum Antiferromagnet.

Antiferromagnetic materials feature intrinsic ultrafast spin dynamics, making them ideal candidates for future magnonic devices operating at THz frequencies. A major focus of current research is the investigation of optical methods for the efficient generation of coherent magnons in antiferromagnetic insulators. In magnetic lattices endowed with orbital angular momentum, spin-orbit coupling enables spin dynamics through the resonant excitation of low-energy electric dipoles such as phonons and orbital resonances which interact with spins. However, in magnetic systems with zero orbital angular momentum, microscopic pathways for the resonant and low-energy optical excitation of coherent spin dynamics are lacking. Here, we consider experimentally the relative merits of electronic and vibrational excitations for the optical control of zero orbital angular momentum magnets, focusing on a limit case: the antiferromagnet manganese phosphorous trisulfide (MnPS_{3}), constituted by orbital singlet Mn^{2+} ions. We study the correlation of spins with two types of excitations within its band gap: a bound electron orbital excitation from the singlet orbital ground state of Mn^{2+} into an orbital triplet state, which causes coherent spin precession, and a vibrational excitation of the crystal field that causes thermal spin disorder. Our findings cast orbital transitions as key targets for magnetic control in insulators constituted by magnetic centers of zero orbital angular momentum.

Dicarbon defect in hexagonal boron nitride monolayer—a theoretical study

A comprehensive theoretical study of the lowest electronic vertical excitations of the CBCN defect in the monolayer of hexagonal boron nitride has been performed. Both the periodic boundary conditions approach and the finite-cluster simulation of the defect have been utilized at the density-functional theory (DFT) level. Clusters of increasing sizes have been used in order to estimate artefacts resulting from edge effects. The stability of the results with respect to several density functionals and various basis sets has been also examined. High-level ab initio calculations with methods like equation-of-motion coupled cluster method with single and double excitations (EOM-CCSD), algebraic-diagrammatic construction to the second order (ADC(2)), and time-dependent approximate coupled cluster theory to the second order (TD-CC2) were performed for the smallest clusters. It turns out that TD-DFT with the CAM-B3LYP functional gives similar lowest excitation energies as EOM-CCSD, ADC(2), and TD-CC2. The lowest excitation energies resulting from the periodic-boundary calculation utilizing the Bethe–Salpeter equation are in agreement with the results for finite clusters. The analysis of important configurations and transition densities shows that for all studied methods, the lowest excited state is localized on two carbon atoms and their closest neighbours and has a large dipole transition moment. The optimized geometries for the lowest two excited states indicate that in both cases, the carbon–carbon bond becomes a single bond, while for the second excited state, additionally one from boron–nitrogen bonds loses its partially double character. The calculation of the excitation energies at the respective optimal geometry reveals that these two energies become about 0.5 eV lower than vertical excitations from the ground-state geometry.

Strongly Coupled Plasmon and Phonon Polaritons as Seen by Photon and Electron Probes

The ability to control and modify infrared excitations in condensed matter is of both fundamental and applied interest. Here we explore a system supporting low-energy excitations, in particular, mid-infrared localized plasmon modes and phonon polaritons that are tuned to be strongly coupled. We study the coupled modes by using far-field infrared spectroscopy, state-of-the-art monochromated electron energy-loss spectroscopy, numerical simulations, and analytical modeling. We demonstrate that the electron probe facilitates a precise characterization of polaritons constituting the coupled system, and enables an active control over the coupling and the resulting sample response both in frequency and space. Although far-field optical spectra can be substantially different from near-field electron energy-loss spectra, we show that a direct comparison is possible via postprocessing and right positioning of the electron beam. The resulting spectra allow us to evaluate the key parameters of the coupled system, such as the coupling strength, which we demonstrate to be probe independent. Our work establishes a rigorous description of the spectral features observed in light- and localized electron-based spectroscopies, which can be extended to the analysis of analogous optical systems with applications in heat management and electromagnetic field concentration or nanofocusing.

Topological properties of MoP[formula omitted]N[formula omitted] (x = 0, 0.25, 0.5, 0.75, 1) compounds: A density functional approach

Triply Degenerate Point (TDP) fermions in tungsten–carbide-type materials such as MoP which represent new topological states of quantum matter, have generated great interest recently. However, the TDPs in these materials are found to be far below the Fermi level (∼ −1.5eV) leading to the TDP fermions having less contribution to low-energy quasiparticle excitations. Here, we theoretically investigate the existence of TP fermions with TDPs close to the Fermi level in MoN, which has the same structure as MoP, and the ternary MoP1−xNx ordered alloys which their crystal structure is defined by replacing P atoms by N atoms in MoP compound. The topological properties of MoP1−xNx (x = 0, 0.25, 0.5, 0.75, 1) ordered alloys are systematically investigated by combining first-principles calculations and Wannier tight-binding analysis. The obtained Wannier Charge Centers (WCCs) are applied to calculate the topological invariant Z2 number. Our calculations show that hexagonal MoP, MoP0.75N0.25, MoP0.25N0.75, and MoN compounds are topological semimetals hosting triply degenerate nodal points resulting from band crossing between degenerate and nondegenerate bands along the high-symmetry directions of the Brillouin Zone, being protected by crystalline symmetries. Among these compounds, the triple degenerate points in MoP0.75N0.25 are much closer to the Fermi level. MoP0.75N0.25 hosts some points slightly above (42 meV, 73 meV and 87 meV) the Fermi energy. On the other hand, our ab initio calculations suggest that the MoP0.5N0.5 compound with orthorhombic structure does not host any triple degenerate point. It hosts a multitude of topological features including Weyl Points and nodal lines. The calculations indicate that these nodal lines are located in the vicinity of Fermi level.

Commissioning of the novel Continuous Angle Multi-energy Analysis spectrometer at the Paul Scherrer Institut.

We report on the commissioning results of the cold neutron multiplexing secondary spectrometer CAMEA (Continuous Angle Multi-Energy Analysis) at the Swiss Spallation Neutron Source at the Paul Scherrer Institut, Switzerland. CAMEA is optimized for efficient data acquisition of scattered neutrons in the horizontal scattering plane, allowing for detailed and rapid mapping of low-energy excitations under extreme sample environment conditions.