Search Results (49)

Hybrid carbon nanotube–fullerene architectures provide a controllable setting in which to study irreversibility and information flow in strongly structured quantum environments. We analyze entropy generation in a platform where paramagnetic endohedral fullerenes (PEFs), such as N@C₆₀ and P@C₆₀, are encapsulated inside a suspended carbon nanotube (CNT) resonator, such that selected multi-level PEF spin states define an effective qubit coupled to quantized CNT flexural modes. Motivated by prior work on fullerene-filled CNTs, on spin–phonon manipulation in suspended nanotubes, and on exact phase-space propagators for damped driven oscillators, we formulate a hybrid open-system description that combines a driven quantum Brownian description of the CNT resonator with an effective Jaynes–Cummings type spin–vibrational interaction. The resonator dynamics are represented in phase space through the Wigner function, whose time evolution can be written analytically in terms of the initial Wigner distribution and a Gaussian propagator. This representation makes it possible to separate drive-induced phase space displacement, diffusion, and damping, and to connect these features directly to entropy flow. The coupled spin–mechanical dynamics are then embedded in a Lindblad quantum master equation that includes mechanical damping, spin relaxation, pure dephasing, and thermally activated excitation channels. Within this framework we derive the entropy balance equation—identifying entropy flux and non-negative entropy production—and examine how hybridization between the molecular spin and the nanotube vibration redistributes irreversibility between coherent exchange and dissipative channels. We show that spin–phonon coupling enhanced by a magnetic field gradient, resonant driving, and moderate thermal occupation can produce identifiable crossovers between entropy–production regimes dominated by the oscillator and those dominated by the spin. The resulting framework provides a quantitative basis for using CNT–PEF hybrids as nanoscale platforms for studying nonequilibrium quantum thermodynamics, decoherence, and information loss in structured vibrational environments. Full article

A microscopic model has been elaborated for the description of charge transfer-induced spin transitions in crystals containing tetranuclear Fe₂Co₂ clusters as structural units. The model takes into account the energy spectrum of each Fe₂Co₂ cluster, formed by the states arising from its initial configuration, two low-spin Fe^II and two low-spin Co^III, final configuration two low-spin Fe^III, and two high-spin Co^II, as well as the states that originate from four intermediate configurations of the type of low-spin Fe^II, low-spin Co^III, low-spin Fe^III, and high-spin Co^II. Two different types of cooperative interactions are accounted for in the model, namely, the electron–deformational coupling arising as a result of the observed elongation of the cobalt-nitrogen bonds under the low-spin Co^III$\to$ high-spin Co^II transition and the interaction via the field of phonons that originates from the coupling of the Co-ions with the full symmetric displacements of the nearest ligand surrounding, which are modulated by crystalline vibrations. The role of cooperative interactions is discussed in detail. Different types of spin transitions are predicted, including the gradual and abrupt ones as well as those manifesting hysteretic behavior. Within the framework of the developed approach, a qualitative and quantitative explanation of the experimental data on the {[(Tp*)Fe(CN)₃]₂[Co(bpy^Me)₂]₂}(OTf)₂·2DMF·H₂O compound recently reported oniere is given. Full article

Interfacial coupling between CoFe₂O₄ (CFO) nanoparticles and oxidatively functionalized multi-walled carbon nanotubes (MWCNTs) enables controlled modulation of structural, optical, and spin dynamic properties in CFO–MWCNT nanocomposites. The solvothermal synthesis promotes nucleation of CFO on –COOH/–OH functional groups, ensuring uniform anchoring along the nanotube surface. X-ray diffraction confirms a cubic spinel phase with lattice expansion from 8.385 Å to 8.410 Å and crystallite growth from 18 nm to 25 nm, reflecting strain transfer and partial nanoparticle coalescence at the carbon interface. The observed bandgap narrowing from 2.72 eV to 2.50 eV, confirmed via Tauc plot analysis, is attributed to localized defect states induced by charge delocalization and orbital hybridization at the interface of the CFO–MWCNT boundary. DC magnetometry reveals a reduction in saturation magnetization from 46 emu/g to 35 emu/g due to diamagnetic dilution and interfacial spin canting, while coercivity decreases from 852 Oe to 841 Oe, indicating modified pinning and domain-wall dynamics associated with exchange-coupled interfaces. Ferromagnetic resonance measurements show a resonance field shift from 3495 G to 3500 G and an increase in the Landé g-factor from 1.97 to 2.00, signifying altered spin–orbit coupling and enhanced local magnetic perturbations. The spin–lattice relaxation time increases from 1.41 ns to 1.59 ns, demonstrating suppressed phonon-mediated relaxation and improved spin coherence across the hybrid network. Spin density rises from 3.72 × 10²² to 4.58 × 10²² spins/g, confirming an increase in unpaired electrons generated by orbital asymmetry at the interface. The anisotropy field and effective magnetocrystalline anisotropy constant exhibit pronounced modulation, evidencing strengthened exchange stiffness and altered Co²⁺/Fe³⁺ superexchange pathways. These results establish CFO-MWCNT nanocomposites as tuneable platforms for spintronic logic elements, high-frequency microwave attenuation, and magneto-optical device architectures. Full article

Inelastic electron tunneling spectroscopy (IETS) has emerged as a powerful vibrational spectroscopy technique for molecular electronic junctions, providing unique insights into molecular vibrations and electron–phonon coupling at the nanoscale. In this review, we present a comprehensive overview of IETS in molecular junctions, tracing its development from foundational principles to the latest advances. We begin with the theoretical background, detailing the mechanisms by which inelastic tunneling processes generate vibrational fingerprints of molecules, and highlighting how IETS complements optical spectroscopies by accessing electrically driven vibrational excitations. We then discuss recent progress in experimental techniques and device architectures that have broadened the applicability of IETS. Central focus is given to emerging applications of IETS over the last decade: molecular sensing (identification of chemical bonds and conformational changes in junctions), thermoelectric energy conversion (probing vibrational contributions to molecular thermopower), molecular switches and functional devices (monitoring bias-driven molecular state changes via vibrational signatures), spintronic molecular junctions (detecting spin excitations and spin–vibration interplay), and advanced data analysis approaches such as machine learning for interpreting complex tunneling spectra. Finally, we discuss current challenges, including sensitivity at room temperature, spectral interpretation, and integration into practical devices. This review aims to serve as a thorough reference for researchers in physics, chemistry, and materials science, consolidating state-of-the-art understanding of IETS in molecular junctions and its growing role in molecular-scale device characterization. Full article

We present a brief overview of the field of charge density waves (CDW) in condensed systems with focus set to the underlying mechanisms behind the CDW ground state. Our intention in this short review is not to count all related facts from the vast volume of literature about this decades-old and still developing field, but rather to pinpoint the most important, mostly theoretical ones, presenting the development of the field. Starting from the “early days”, mainly based on weakly coupled, chain-like quasi-1D systems and Peierls instability, in which the Fermi surface nesting has been the predominant and practically paradigmatic mechanism of the CDW ground state stabilisation, we track the change in paradigms while entering the field of layered quasi-2D systems, with Fermi surface far away from the nesting regime, in which rather strong, essentially momentum-dependent interactions and particular reconstructions of the Fermi surface become essential. Examples of real quasi-1D materials, such as organic and inorganic conductors like Bechgaard salts or transition metal trichalcogenides and bronzes, in which experiment and theory have been extremely successful in providing detailed understanding, are contrasted to layered quasi-2D materials, such as ${\mathrm{high-T}}_c$ superconducting cuprates, intercalated graphite compounds or transition metal dichalcogenides, for which the theory explaining an onset of the CDWs constitutes a frontier of this fast-evolving field, strongly boosted by development of modern ab initio calculation methods. Full article

Research on two dimensional (2D) antiferromagnetic materials and heterobilayers is gaining prominence in spintronics. This study focuses on MPS₃ monolayers and their van der Waals heterobilayers with GaN monolayers. We systematically investigated the structural stability, electronic properties, and magnetic characteristics of MPS₃ (M = Mn, Fe, and Ni) monolayers via first-principles calculations, and explored their potential applications in optoelectronics and spintronics. Through phonon spectrum analysis, the dynamic stability of MPS₃ monolayers was confirmed, and their bond lengths, charge distributions, and wide-bandgap semiconductor properties were analyzed in detail. In addition, the potential applications of MPS₃ monolayers in UV detection were explored. Upon constructing the MPS₃/GaN heterobilayer structure, a significant reduction in the bandgap was observed, thereby expanding its potential applications in the visible light spectrum. The intrinsic antiferromagnetic nature of MPS₃ monolayers was confirmed through calculations, with the magnetic moments of the magnetic atoms M being 4.560, 3.672, and 1.517, respectively. Moreover, the heterobilayer structures further enhanced the magnetic moments of these elements. The magnetic properties of MPS₃ monolayers were further analyzed using spin-orbit coupling (SOC), confirming their magnetic anisotropy. These results provide a theoretical basis for the design of novel two-dimensional spintronic and optoelectronic devices based on MPS₃. Full article

On the basis of a microscopic model and employing Green’s function technique, the effects of temperature, size, and ion doping on the magnetization and phonon energy of the A_1g mode in double perovskites Ba₂FeReO₆ and Sr₂CrReO₆—both in bulk and nanoscale samples—are investigated for the first time. The Curie temperature T_C and magnetization M decrease as nanoparticle size is reduced. Doping with rare-earth ions such as Sm, Nd, or La at the Ba or Sr sites further reduces M. This behavior originates from the compressive strain induced by the smaller ionic radii of the dopant ions compared to the host ions. As a result, the antiferromagnetic superexchange interaction between Fe or Cr and Re ions is enhanced, along with an increase in the magnetic moment of the Re ion. The dependence of the band gap energy of Sr₂CrReO₆ on temperature, size, and doping is also studied. Near the magnetic-phase-transition temperature T_C, anomalies in phonon energy and damping indicate strong spin–phonon coupling. The theoretical calculations show good qualitative agreement with experimental data. Full article

A new compound [Y₂(sq)₃(H₂O)₄] (Y-sq; sq = squarate (C₄O₄^2–)) was prepared and structurally characterized. Since the RE-sq family (RE = Y, Dy, Yb, Lu) gave isostructural crystals, the objective of this study is to explore the effects of diamagnetic dilution on the SIM behavior through systematic investigation and comparison of diamagnetically diluted and undiluted forms. The 1%-Diluted Dy compounds, Dy@Y-sq and Dy@Lu-sq, showed AC magnetic susceptibility peaks without any DC bias field (H_DC), whereas undiluted Dy-sq showed no AC out-of-phase response under the same conditions. The Orbach and Raman mechanisms are assumed in the Arrhenius plots, giving U_eff/k_B = 139(5) and 135(8) K for Dy@Y-sq and Dy@Lu-sq, respectively, at H_DC = 0 Oe. In contrast, Yb@Y-sq and Yb@Lu-sq behaved different; Yb@Y-sq can be regarded as a field-induced SIM because AC out-of-phase response was recorded only when H_DC was present. On the other hand, Yb@Lu-sq showed a relaxation independent from temperature around 2 K at H_DC = 0 Oe, possibly ascribed to a quantum-tunneling-magnetization mechanism. Applying H_DC = 400 Oe afforded U_eff = 61.2(14) and 62.5(16) K for Yb@Y-sq and Yb@Lu-sq, respectively. The Y/Lu matrix dependence may be related to spin–phonon coupling. The dilution technique is a facile and versatile tool for modification of SIM characteristics. Full article

For more than a decade, the unusual distribution of electrons observed in ARPES (angle-resolved photoemission spectroscopy) data within the energy range of ~30 meV to ~300 meV below the Fermi level, known as the ARPES energy range, has remained a puzzle in the field of iron-based superconductivity. As the electron–phonon coupling of FeSe/SrTiO₃ is very strong, our investigation is centered on exploring the synergistic interplay between spin-density waves (SDW) and charge-density waves (CDW) with differential phonons at the interface between antiferromagnetic maxima and minima under wave interference. Our analysis reveals that the synergistic energy is proportional to the ARPES energy range, as seen in the comparison between FeSe and FeSe/SrTiO₃. This finding may suggest that the instantaneous interplay between these intricate phenomena may play a role in triggering the observed energy range in ARPES. Full article

With the help of a microscopic model and Green’s function technique, we studied the multiferroic and phonon properties of the recently reported new multiferroic Pr₂FeAlO₆ (PFAO) compound, which belongs to the double perovskite A₂BB’O₆ family. The magnetization decreases with the increase in temperature and disappears at the ferromagnetic Curie temperature $T_C^{FM}$. The polarization increases with the application of an external magnetic field, indicating strong magnetoelectric coupling and confirming the multiferroic behavior of PFAO. In the curves of dependence of the phonon energy and their damping with respect to temperature, a kink is observed at $T_C^{FM}$. This is due to the strong anharmonic spin–phonon interactions, which play a crucial role below $T_C^{FM}$ and are frequently observed in other double perovskite compounds. Above $T_C^{FM}$, only anharmonic phonon–phonon coupling remains. The phonon mode is controlled by an external magnetic field. Full article

Phonon blockade is an important quantum effect for revealing the quantum behaviors of mechanical systems. For a nitrogen-vacancy center spin strongly coupled to a mechanical resonator via the second-order magnetic gradient, we show that the qubit driving can lead to the implementation of the two-phonon blockade, while the usual mechanical driving only allows for the appearance of a single-phonon blockade. As a signature, we investigate three-phonon antibunching with a simultaneous two-phonon bunching process by numerically calculating the second-order and third-order correlation functions. We also analyze in detail the influence of the system parameters (including the qubit driving strength, the dephasing rate of the qubit, as well as the thermal phonon number) on the quality of the two-phonon blockade effect. Our work provides an alternative method for extending the concept of a phonon blockade from a single phonon to multiphonon. It is of direct relevance for the engineering of multiphonon quantum coherent devices and thus has potential applications in quantum information processing. Full article

The present study focuses on the spin-dependent vibrational properties of HKUST-1, a metal–organic framework with potential applications in gas storage and separation. Employing density functional theory (DFT), we explore the consequences of spin couplings in the copper paddle wheels (as the secondary building units of HKUST-1) on the material’s vibrational properties. By systematically screening the impact of the spin state on the phonon bands and densities of states in the various frequency regions, we identify asymmetric -COO- stretching vibrations as being most affected by different types of magnetic couplings. Notably, we also show that the DFT-derived insights can be quantitatively reproduced employing suitably parametrized, state-of-the-art machine-learned classical potentials with root-mean-square deviations from the DFT results between 3 cm⁻¹ and 7 cm⁻¹. This demonstrates the potential of machine-learned classical force fields for predicting the spin-dependent properties of complex materials, even when explicitly considering spins only for the generation of the reference data used in the force-field parametrization process. Full article

Transition metal dichalcogenides (TMDs) have unique absorption and emission properties that stem from their large excitonic binding energies, reduced-dielectric screening, and strong spin–orbit coupling. However, the role of substrates, phonons, and material defects in the excitonic scattering processes remains elusive. In tungsten-based TMDs, it is known that the excitons formed from electrons in the lower-energy conduction bands are dark in nature, whereas low-energy emissions in the photoluminescence spectrum have been linked to the brightening of these transitions, either via defect scattering or via phonon scattering with first-order phonon replicas. Through temperature and incident-power-dependent studies of WS₂ grown by CVD or exfoliated from high-purity bulk crystal on different substrates, we demonstrate that the strong exciton–phonon coupling yields brightening of dark transitions up to sixth-order phonon replicas. We discuss the critical role of defects in the brightening pathways of dark excitons and their phonon replicas, and we elucidate that these emissions are intrinsic to the material and independent of substrate, encapsulation, growth method, and transfer approach. Full article

A review is provided here about the thermal effects on optical chirality. To this goal, chiral objects dispersed in an embedding fluid are examined for their magnetoelectric coupling. Thermal effects on several chiral meta-atoms and their ensembles are examined. To this goal, DNA-like helical structures are examined in detail. The mechanical aspect of thermo-elasticity is reviewed along with transverse deformations while drawing analogies from condensed-matter physics. In this respect, the chirality-induced spin selection is reviewed along with the temperature-mediated electron–phonon interactions. A wide range of materials, such as polymers and biological cells, are also examined for temperature effects. A transition temperature delineating a sign flip in the chirality parameter is identified as well. Chirality-associated functionalities such as ratchet motions, switching, and modulations are investigated for their respective thermal effects. Issues of fabricating chiral meta-atoms are also discussed. Full article

We report on the far-infrared, temperature-dependent optical properties of a CrI${}_3$ transition metal halide single crystal, a van der Waals ferromagnet (FM) with a Curie temperature of 61 K. In addition to the expected phonon modes determined by the crystalline symmetry, the optical reflectance and transmittance spectra of CrI${}_3$ single crystals show many other excitations as a function of temperature as a consequence of the combination of a strong lattice anharmonicity and spin–phonon coupling. This complex vibrational spectrum highlights the presence of entangled interactions among the different degrees of freedom in CrI${}_3$. Full article