Hamiltonian Parameters Research Articles

Pseudo-easy-axis anisotropy in antiferromagnetic S=1 diamond-lattice systems

We investigate the magnetic properties of S=1 antiferromagnetic diamond-lattice, NiX2(pyrimidine)2 (X=Cl, Br), hosting a single-ion anisotropy (SIA) orientation which alternates between neighboring sites. Through neutron diffraction measurements of the X=Cl compound, the ordered state spins are found to align collinearly along a pseduo-easy axis, a unique direction created by the intersection of two easy planes. Similarities in the magnetization, exhibiting spin-flop transitions, and the magnetic susceptibility in the two compounds imply that the same magnetic structure and a pseduo-easy axis is also present for X=Br. We estimate the Hamiltonian parameters by combining analytical calculations and Monte Carlo (MC) simulations of the spin-flop and saturation field. The MC simulations also reveal that the spin-flop transition occurs when the applied field is parallel to the pseduo-easy axis. Contrary to conventional easy-axis systems, there exist field directions perpendicular to the pseduo-easy axis for which the magnetic saturation is approached asymptotically and no symmetry-breaking phase transition is observed at finite fields. Published by the American Physical Society 2024

Effect of Oriented External Electric Field in Altering Magnetic Exchange and Magnetic Anisotropy in Lanthanide-Radical Complexes.

Magnetic exchange coupling (J) is one of the important spin Hamiltonian parameters that control the magnetic characteristics of single-molecule magnets (SMMs). While numerous chemical methodologies have been proposed to modify ligands and control the J value, and magneto-structural correlations have been developed accordingly, altering this parameter through non-chemical means remains a challenging task. This study explores the impact of an Oriented-External Electric Field (OEEF) on over twenty lanthanide-radical complexes using Density Functional Theory (DFT) and ab initio Complete Active Space Self-Consistent Field (CASSCF) methods. Five complexes - [{(Me3Si)2N]2Gd(THF)}2(μ-η2:η2-N2)] (1), [Gd(Hbpz3)2(dtbsq)] (2), [Gd(hfac)3(IM-2py)] (3), [Gd(hfac)3(NITBzImH)] (4), and [Gd(hfac)3{2Py-NO}(H2O)] (5) - were selected for detailed analysis, revealing significant OEEF effects on magnetic exchange interactions and structural parameters. Various parameters such as bond distances, bond angles, and torsional angles were examined as a function of OEEF to establish guiding principles for molecule selection. In complexes 1, 2, and 3, OEEF influenced torsional angles and altered exchange interactions. Complex 4 demonstrated enhanced ferromagnetic coupling under OEEF, reaching a maximum J value of +5.3 cm-1. Complex 5 reveals switching the sign of JGd-rad exchange interaction from antiferromagnetic to ferromagnetic under OEEF, highlighting the potential of electric fields in designing materials with tuneable magnetic properties. These findings offer valuable insights for future research and applications in advanced materials and molecular electronics.

High–Field EPR Studies on Three Binuclear μ–Oxo–Bridged Iron(III) Complexes: Na4[Fe(edta)]2O ⋅ 3H2O, [Fe(phen)2(H2O)]2O(NO3)4 ⋅ 5H2O and [Fe(salen)]2O

AbstractA High–Field, High–Frequency Electron Paramagnetic Resonance (HFEPR) study was performed on the binuclear μ–oxo bridged complexes Na4[Fe(edta)]2O ⋅ 3H2O, [Fe(phen)2(H2O)]2O(NO3)4 ⋅ 5H2O and [Fe(salen)]2O, where edtaH4 = ethylenediaminetetraacetic acid, phen=1,10–phenanthroline and salenH2 is NN′–ethylenebis(salicylideneimine). The spin Hamiltonian parameters were determined for the thermally excited spin states with spin S=1, 2 and 3. The contributions to the zero–field splitting due to the local zero field splitting on individual iron ions and to the anisotropic metal–metal interactions were evaluated. Surprisingly large magnitudes of the anisotropic exchange interactions were found.

Superconductivity in the pressurized nickelate La3Ni2O7 in the vicinity of a BEC–BCS crossover

Ever since the discovery of high-temperature superconductivity in cuprates, gaining microscopic insights into the nature of pairing in strongly correlated systems has remained one of the greatest challenges in modern condensed matter physics. Following recent experiments reporting superconductivity in the bilayer nickelate La3Ni2O7 (LNO) with remarkably high critical temperatures of Tc = 80 K, it has been argued that the low-energy physics of LNO can be described by the strongly correlated, mixed-dimensional bilayer t–J model. Here we investigate this bilayer system and utilize density matrix renormalization group techniques to establish a thorough understanding of the model and the magnetically induced pairing through comparison to the perturbative limit of dominating inter-layer spin couplings. In particular, this allows us to explain appearing finite-size effects, firmly establishing the existence of long-range superconducting order in the thermodynamic limit. By analyzing binding energies, we predict a BEC–BCS crossover as a function of the Hamiltonian parameters. We find large binding energies of the order of the inter-layer coupling that suggest strikingly high critical temperatures of the Berezinskii–Kosterlitz–Thouless transition, raising the question of whether (mixD) bilayer superconductors possibly facilitate critical temperatures above room temperature.

Robustly learning the Hamiltonian dynamics of a superconducting quantum processor

Precise means of characterizing analog quantum simulators are key to developing quantum simulators capable of beyond-classical computations. Here, we precisely estimate the free Hamiltonian parameters of a superconducting-qubit analog quantum simulator from measured time-series data on up to 14 qubits. To achieve this, we develop a scalable Hamiltonian learning algorithm that is robust against state-preparation and measurement (SPAM) errors and yields tomographic information about those SPAM errors. The key subroutines are a novel super-resolution technique for frequency extraction from matrix time-series, tensorESPRIT, and constrained manifold optimization. Our learning results verify the Hamiltonian dynamics on a Sycamore processor up to sub-MHz accuracy, and allow us to construct a spatial implementation error map for a grid of 27 qubits. Our results constitute an accurate implementation of a dynamical quantum simulation that is precisely characterized using a new diagnostic toolkit for understanding, calibrating, and improving analog quantum processors.

High‐Frequency Electron Paramagnetic Resonance and Electron‐Nuclear Double Resonance Spectroscopy Study of the Ga Vacancy in β‐Ga2O3

The Ga vacancy (VGa) defect in β‐Ga2O3, generated by proton irradiation, is studied using high‐frequency electron paramagnetic resonance (EPR) and electron‐nuclear double resonance spectroscopy. The previous X‐band EPR studies of this defect, attributed to VGa2−, are extended to higher frequencies (240 GHz) and lower temperatures (T = 6 K). The spin Hamiltonian parameters of the VGa2− center are determined: electron spin S = 1/2, g‐tensor: gb = 2.0313, gc = 2.0079, and ga = 2.0025; the hyperfine interaction parameters with 2 equivalent Ga neighbors: Ab = 14.0 G, Ac = 14.6 G, and Aa* = 12.8 G for 69Ga; the superhyperfine interaction with distant Ga neighbors ASHF(69Ga) = 11 MHz; and the quadrupole interaction Qb(69Ga) = 0.32 MHz and Qb(71Ga) = 0.22 MHz. These results shall allow to refine the assignment of this center to a split vacancy or an unrelaxed VGa2− defect.

Hysteresis behavior and magnetocaloric effect in MnNiGa[formula omitted] full-Heusler alloy

In this manuscript, we studied the magnetic, magnetocaloric, and hysteresis properties of the MnNiGa2 full-Heusler alloy using mean-field theory and first-principles calculations. Initially, we employed the GGA+U method to investigate the structural characteristics of the alloy. Our findings indicated that the ferromagnetic state, with an optimal lattice parameter of 5.88 Å, was the most stable compared to the antiferromagnetic states. Additionally, the exchange interactions, defined as the Hamiltonian parameters of the studied system, were calculated and used in the mean-field approximation. The second-order transition at a Curie temperature of Tc = 373 K, previously revealed experimentally, has been confirmed. Furthermore, the alloy exhibited a relative cooling power (RCP) of 260.43 J/kg and a magnetocaloric effect of 10.34 J/kg.K at an applied magnetic field of 1.4 T. These results suggest that MnNiGa2 is a promising candidate for magnetic refrigeration applications.

Vibronic coupling in the energetically six lowest electronic states of oxirane radical cation.

Multi-dimensional quantum mechanical simulations are carried out to understand the multi-state and multi-mode vibronic interactions in the first six low-lying viz., X̃2B1, Ã2A1, B̃2B2, C̃2A2, D̃2A1, and Ẽ2B1 electronic states of c-C2H4O·+. Vibronic coupling theory is applied to study interactions among electronic states using symmetry selection rules. A model 6 × 6 diabatic electronic Hamiltonian is constructed. The parameters of the diabatic Hamiltonian are estimated by performing extensive abinitio electronic structure calculations, using the EOM-IP-CCSD method. The nuclear dynamics calculations are performed with both time-independent and time-dependent quantum mechanical methods. The calculated vibronic structures of six electronic states are found to be in excellent agreement with the available experimental findings. Progressions found in the theoretical spectrum are assigned in terms of vibrational modes. It is found that extremely strong vibronic interactions among the X̃2B1-Ã2A1, B̃2B2-C̃2A2, and D̃2A1-Ẽ2B1 electronic states results into highly overlapping vibronic bands due to multiple multi-state conical intersections. The impact of associated nonadiabatic effects on the vibronic structure and dynamics of the mentioned electronic states is examined at length. Interesting comparison is made with the results obtained for the isomeric acetaldehyde radical cation.

Braids and higher-order exceptional points from the interplay between lossy defects and topological boundary states

We show that the perturbation of the Su-Schrieffer-Heeger chain by a localized lossy defect leads to higher-order exceptional points (HOEP). Depending on the location of the defect, third- and fourth-order exceptional points (EP3 and EP4) appear in the space of Hamiltonian parameters. On the one hand, they arise due to the non-Abelian braiding properties of exceptional lines (EL) in parameter space. Namely, the HOEPs lie at intersections of mutually noncommuting ELs. On the other hand, we show that such special intersections happen due to the fact that the delocalization of edge states, induced by the non-Hermitian defect, hybridizes them with defect states. These can then coalesce together into an EP3. When the defect lies at the midpoint of the chain, a special symmetry of the full spectrum can lead to an EP4. In this way, our model illustrates the emergence of interesting non-Abelian topological properties in the multiband structure of non-Hermitian perturbations of topological phases. Published by the American Physical Society 2024

Study of the properties of Ru-isotopes using the proton-neutron interacting boson model (IBM-2)

The proton-neutron interacting boson model (IBM-2) has been used to make a schematic study of the Ruthenium ( ) isotopes of mass region around with and . For each isotope of the values of the IBM-2 Hamiltonian parameters, which yield an acceptable results for excitation energies in comparison with those of experimental data, have been determined. Fixed values of the effective charges ( ) and of the proton and neutron g factors ( and ) have been chosen for all isotopes under study. The calculated electric quadrupole moments of state, transitions, the magnetic dipole moments transitions and mixing ratios are in reasonable agreement with the experimental data.

Quantum spin systems: Toroidal classification and geometric duality

We demonstrate a toroidal classification for quantum spin systems, revealing an intrinsic geometric duality within this structure. Through our classification and duality, we reveal that various bipartite quantum features in magnon systems can manifest equivalently in both bipartite ferromagnetic and antiferromagnetic materials, based upon the availability of relevant Hamiltonian parameters. Additionally, the results highlight the antiferromagnetic regime as an ultrafast dual counterpart to the ferromagnetic regime, both exhibiting identical capabilities for quantum spintronics and technological applications. Concrete illustrations are provided, demonstrating how splitting and squeezing types of two-mode magnon quantum correlations can be realized across ferro- and antiferromagnetic regimes. Published by the American Physical Society 2024

High resolution analysis of the CD[formula omitted] deuterated methane: Extended investigation of the pentad region

A highly accurate rotational–vibrational analysis of Fourier transform infrared spectra of the 12CD4 molecule is presented. The high resolution infrared spectra were measured with a IFS125 HR Fourier transform interferometer from Bruker at an optical resolution of 0.003 cm−1 and analyzed in the 1750–2400 cm−1 region. Here the 2ν2, ν2+ν4, 2ν4, ν1 and ν3 bands (altogether, nine sub-bands of different symmetry) of the pentad are located. The number of 1213/1993/1576/77/1582 transitions with the Jmax = 23/23/23/14/32 were assigned to the 2ν2, ν2+ν4, 2ν4, ν1 and ν3 bands of 12CD4. The obtained experimental data were used for the determination of the upper ro-vibrational energy values. To provide more correct values of the upper energies, more than 7800 highly accurate “hot” transitions from the dyad region were additionally processed. In general, 4088 upper ro-vibrational energies of the pentad (for comparison, 2525 upper ro-vibrational energies with the value of Jmax=20 are known in the modern literature up to now) were determined, which were used then in the weighted fit procedure with a goal to determine the spectroscopic parameters (band centers, rotational, centrifugal distortion, tetrahedral splitting and resonance interaction parameters) of the effective Hamiltonian. The obtained drms value is 5.5×10−4 cm−1 which is almost one hundred times better than the reproduction of the same set of experimental data by the parameters known in the earlier literature.

Spectroscopy, crystal-field, and transition intensity analyses of the C[formula omitted](O[formula omitted]) centre in Er[formula omitted] doped CaF2 crystals

Erbium ions in crystals show considerable promise for the technologies that will form the backbone of future networked quantum information technology. Despite advances in leveraging erbium’s fibre-compatible infrared transition for classical and quantum applications, the transitions are, in general, not well understood. We present detailed absorption and laser site-selective spectroscopy of the C3v(O2−) centre in CaF2:Er3+ as an interesting erbium site case study. The 4I15/2Z1→4I13/2Y1 transition has a low-temperature inhomogeneous linewidth of 1 GHz with hyperfine structure observable from the 167Er isotope. A parametrized crystal-field Hamiltonian is fitted to 34 energy levels and the two ground state magnetic splitting factors. The wavefunctions are used to perform a transition intensity analysis and electric-dipole parameters are fitted to absorption oscillator strengths. Simulated spectra for the 4I11/2→4I15/2 and 4I13/2→4I15/2 inter-multiplet transitions are in excellent agreement with the experimentally measured spectra. The 4I13/2 excited state lifetime is 25.0ms and the intensity calculation is in excellent agreement with this value.

Modular Many-Body Quantum Sensors.

Quantum many-body systems undergoing phase transitions have been proposed as probes enabling beyond-classical enhancement of sensing precision. However, this enhancement is usually limited to a very narrow region around the critical point. Here, we systematically develop a modular approach for introducing multiple phase transitions in a many-body system. This naturally allows us to enlarge the region of quantum-enhanced precision by encompassing the newly created phase boundaries. Our approach is general and can be applied to both symmetry-breaking and topological quantum sensors. In symmetry-breaking sensors, we show that the newly created critical points inherit the original universality class and a simple total magnetization measurement already suffices to locate them. In topological sensors, our modular construction creates multiple bands which leads to a rich phase diagram. In both cases, Heisenberg scaling for Hamiltonian parameter estimation is achieved at all the phase boundaries. This can be exploited to create a global sensor which significantly outperforms a uniform probe.

Assignment and modeling of 13CH4 spectrum at 298 K in the lower part of the Tetradecad in the 4970–5300 cm−1 range

The absorption spectrum of the 13CH4 methane isotopologue was recorded on a Bruker IFS-125HR Fourier transform spectrometer at 298 K in the 4970–6200 cm−1 range. In this paper we report the results of assignment and modelling of the line positions and intensities of 13CH4 in the range of weaker absorption between 4970 and 5300 cm−1, corresponding to the lower part of Tetradecad, dominated by the 4ν4 band system near 5180 cm−1. The empirical list in this spectral range contains 1642 lines. Using an effective Hamiltonian initially derived from the analyses of cold Fourier transform (4970–5853 cm−1) and laser direct absorption (5853–6200 cm−1) spectra of the 13CH4, we assigned 1600 lines belonging to four bands of the Tetradecad up to Jmax=16. The 1548 line positions were fitted with an rms deviation of 1.7 × 10−3 cm−1. Measured line intensities were modeled for 674 transitions using the effective dipole transition moments to an rms deviation of about 7 %. The new data were used for the simultaneous global fit of the 13CH4 Hamiltonian parameters for the {Ground state / Dyad / Pentad / Octad / Tetradecad} system and the dipole moment parameters for the {Ground state - Tetradecad} system.

Spin–Orbit Coupling of the Ellipsoidal Secondary in a Binary Asteroid System

In our solar system, spin–orbit coupling is a common phenomenon in binary asteroid systems, where the mutual orbits are no longer invariant due to exchange of angular momentum between translation and rotation. In this work, dynamical structures in phase space are explored for the problem of spin–orbit coupling by taking advantage of analytical and numerical methods. In particular, the technique of Poincaré sections is adopted to reveal numerical structures, which are dependent on the total angular momentum, the Hamiltonian, mass ratio, and asphericity parameter. Analytical study based on perturbative treatments shows that high-order and/or secondary spin–orbit resonances are responsible for numerical structures arising in Poincaré sections. Analytical solutions are applied to (65803) Didymos, (80218) VO123 and (4383) Suruga to reveal their phase-space structures, showing that there is a high possibility for them to locate inside secondary 1:1 spin–orbit resonance.

Observation of Pairwise Level Degeneracies and the Quantum Regime of the Arrhenius Law in a Double-Well Parametric Oscillator

By applying a microwave drive to a specially designed Josephson circuit, we have realized a double-well model system: a Kerr oscillator submitted to a squeezing force. We have observed, for the first time, the spectroscopic fingerprint of a quantum double-well Hamiltonian when its barrier height is increased: a pairwise level kissing (coalescence) corresponding to the exponential reduction of tunnel splitting in the excited states as they sink under the barrier. The discrete levels in the wells also manifest themselves in the activation time across the barrier which, instead of increasing smoothly as a function of the barrier height, presents steps each time a pair of excited states is captured by the wells. This experiment illustrates the quantum regime of Arrhenius’s law, whose observation is made possible here by the unprecedented combination of low dissipation, time-resolved state control, 98.5% quantum nondemolition single shot measurement fidelity, and complete microwave control over all Hamiltonian parameters in the quantum regime. Direct applications to quantum computation and simulation are discussed. Published by the American Physical Society 2024

Individually tunable tunnelling coefficients in optical lattices using local periodic driving

Abstract Ultracold atoms in optical lattices have emerged as powerful quantum simulators of translationally invariant systems with many applications in e.g. strongly-correlated and topological systems. However, the ability to locally tune all Hamiltonian parameters remains an outstanding goal that would enable the simulation of a wider range of quantum phenomena. Motivated by recent advances in quantum gas microscopes and optical tweezers, we here show theoretically how local control over individual tunnelling links in an optical lattice can be achieved by incorporating local time-periodic potentials. We propose to periodically modulate the on-site energy of individual lattice sites and employ Floquet theory to demonstrate how this provides full individual control over the tunnelling amplitudes in one dimension. We provide various example configurations realising interesting topological models such as extended Su–Schrieffer–Heeger models that would be challenging to realise by other means. Extending to two dimensions, we demonstrate that local periodic driving in a Lieb lattice engineers a two-dimensional (2D) network with fully controllable tunnelling magnitudes. In a three-site plaquette, we show full simultaneous control over the relative tunnelling amplitudes and the gauge-invariant flux piercing the plaquette, providing a clear stepping stone to building a fully programmable 2D tight-binding model. We also explicitly demonstrate how utilise our technique to generate a magnetic field gradient in 2D. This local modulation scheme is applicable to many different lattice geometries.

Random matrix theory approach to quantum Fisher information in quantum ergodic systems.

We theoretically investigate quantum parameter estimation in quantum chaotic systems. Our analysis is based on an effective description of quantum ergodic systems in terms of a random matrix Hamiltonian. Based on this approach, we derive an analytical expression for the time evolution of the quantum Fisher information (QFI), which we find to have three distinct timescales. Initially, the QFI increase is quadratic in time, characterizing the timescale over which initial information is extractable from local measurements only. This quickly passes into linear increase with slope determined by the decay rate of the measured spin observable. When the information is fully spread among all degrees of freedom, a second quadratic timescale determines the long-time behavior of the QFI. We test our random matrix theory prediction with the exact diagonalization of a nonintegrable spin system, focusing on the estimation of a local magnetic field by measurements of the many-body state. Our numerical calculations agree with the effective random matrix theory approach and show that the information on the local Hamiltonian parameter is distributed throughout the quantum system during the quantum thermalization process.

Hamiltonian Identification via Quantum Ensemble Classification.

Identifying the Hamiltonian of an unknown quantum system is a critical task in the area of quantum information. In this article, we propose a systematic Hamiltonian identification approach via quantum ensemble multiclass classification (HI-QEMC). This approach is implemented by a three-step iterative refining process, i.e., parameter interval guess, verification, and judgment. In the parameter interval guess step, the parameter interval is divided into several sub-intervals and the true Hamiltonian parameter is guessed in one of them. In the parameter interval verification step, cross verification is applied to verify the accuracy of the guess. In the parameter interval judgment step, an adaptive interval judgment (AIJ) algorithm is designed to determine the sub-interval containing the true Hamiltonian parameter. Numerical results on two typical quantum systems, i.e., two-level quantum systems and three-level quantum systems, demonstrate the effectiveness and superior performance of the proposed approach for quantum Hamiltonian identification.