Electron Systems Research Articles

The inner workings of sp2 clusters in nitrogen-incorporated tetrahedral amorphous carbon thin films according to optical analyses

The conduction mechanism in nitrogen-incorporated tetrahedral amorphous carbon (ta-C: N) thin films is mainly attributed to the conjugation in sp2 clusters. Here, ta-C:N thin films (about 100 nm) were deposited by laser controlled pulsed cathodic vacuum arc (Laser-Arc) at different nitrogen gas flow rates to investigate the electrical properties of such films. Mechanical and structural properties indicate an increase in sp2 fraction with a rise in nitrogen incorporation into the deposited films. However, after an initial decrease in electrical resistivity, it plateaus at higher flow rates while the sp2 content is still rising. Hence, to gain better understanding of the electronic properties, the dielectric constants ε1 and ε2 were obtained from the optical constants [n] and [k], which were numerically determined from reflectance [R] and transmittance [T] measurements in the wavelength range from 190 to 2500 nm (0.5 to 6.5 eV). The dielectric constant ε1 was used to calculate the dielectric volume of the atom, which is interpreted as a measure of the conjugated π electron system. Furthermore, modeling of the dielectric constants yielded the number of conjugated electrons per atom. Through the dielectric volume and number of conjugated electrons, it was discovered that the electrical conductivity does not only depend on the sp2 content and cluster size, but on how many electrons are conjugated and how much space these electrons occupy. The ta-C:N samples with the highest electrical conductivity, were either characterized by the largest occupied volume or the highest number of conjugated electrons.

Quest for Double Möbius Aromaticity.

Neutral four-membered rings with 4n electrons are generally Hückel antiaromatic. On the other hand, 4n electron system can also be Möbius aromatic, although identification has escaped so far. A recent study of double Möbius aromaticity has been put forwarded in the D2h symmetric singlet ground state of four member Pa2B2 ring. Although interesting, but the synthesis possesses a significant challenge as Pa is rare, highly radioactive and toxic. Herein, a synthetically viable four membered Rh2B2 cluster is proposed which contains double Möbius aromaticity. Interestingly, the three membered RhB2 - cluster also possess Möbius aromaticity and is the smallest ring to show such phenomenon.

Bifurcation of Excited-State Population Leads to Anti-Kasha Luminescence in a Disulfide-Decorated Organometallic Rhenium Photosensitizer.

We report a rhenium diimine photosensitizer equipped with a peripheral disulfide unit on one of the bipyridine ligands, [Re(CO)3(bpy)(S-Sbpy4,4)]+ (1+, bpy = 2,2'-bipyridine, S-Sbpy4,4 = [1,2]dithiino[3,4-c:6,5-c']dipyridine), showing anti-Kasha luminescence. Steady-state and ultrafast time-resolved spectroscopies complemented by nonadiabatic dynamics simulations are used to disclose its excited-state dynamics. The calculations show that after intersystem crossing the complex evolves to two different triplet minima: a (S-Sbpy4,4)-ligand-centered excited state (3LC) lying at lower energy and a metal-to-(bpy)-ligand charge transfer (3MLCT) state at higher energy, with relative yields of 90% and 10%, respectively. The 3LC state involves local excitation of the disulfide group into the antibonding σ* orbital, leading to significant elongation of the S-S bond. Intriguingly, it is the higher-lying 3MLCT state, which is assigned to display luminescence with a lifetime of 270 ns: a signature of anti-Kasha behavior. This assignment is consistent with an energy barrier ≥ 0.6 eV or negligible electronic coupling, preventing reaction toward the 3LC state after the population is trapped in the 3MLCT state. This study represents a striking example on how elusive excited-state dynamics of transition-metal photosensitizers can be deciphered by synergistic experiments and state-of-the-art calculations. Disulfide functionalization lays the foundation of a new design strategy toward harnessing excess energy in a system for possible bimolecular electron or energy transfer reactivity.

Strongly correlated electron system NiWO4: A new family of materials for triboelectrics using inherent Coulombic repulsion

The strongly correlated electron system (SCES) insulators promise a wide range of intriguing physical phenomena arising from the exotic charge gap depending on the strength of the Coulombic repulsion between d and f orbital cations. The SCES exhibits polaron hopping conduction, which requires a higher activation energy for carrier conduction between nearest cations, indicating a strong insulating character with relatively high permittivity. Here, we demonstrate that the NiWO4 SCES insulator, which is formed by Coulombic repulsion between the nearest d orbital of Ni, proposes a suitable triboelectric material unlisted system from conventional metal oxides. The higher degree of freedom in NiWO4 by the lower symmetry of monoclinic structure and an additional selection of composition exhibits high relative permittivity (∼13.8) in a wide range of temperatures (up to 180 ℃). The optimized simple mixture of NiWO4 and PDMS (polydimethylsiloxane) for the negatively charged material to triboelectric nanogenerator (TENG) presents 1.78 times higher output compared to the pristine PDMS film-based TENG. NiWO4, considering the physical properties of the SCES determined by Coulombic repulsion strength, paves the way for a new option of TENG materials following the high permittivity.

Unraveling the origin of the Griffiths phase in Ho2NiMnO6: perspectives from linear and nonlinear AC susceptibility

In this study, we investigated the magnetic ordering and underlying mechanism of the Griffiths phase, observed in Ho2NiMnO6 through AC susceptibility measurements. Our results indicate that the transition around 86 K corresponds to a paramagnetic to ferromagnetic transition characterized by classical magnetic ordering. Notably, nonlinear AC susceptibility measurements revealed the existence of ferromagnetic clusters within a paramagnetic background well above the transition temperature, establishing this as the origin of the Griffiths-like phase within the Ni/Mn sublattice of Ho2NiMnO6. Our study on the Ho2NiMnO6 system provides insight into the intricate magnetic phenomena common to various other strongly correlated electron systems.

The Kondo scaling for spin thermocurrent in strongly correlated electron systems

One of the most important feature in the Kondo physics is the universal scaling behavior. In this study, we analyze the transport behavior of the spin thermocurrent driven by a small temperature bias and under a weak magnetic field. We conclude that the spin thermocurrent exhibits a universal scaling behavior, similar to the spin susceptibility. The validity of our conclusion is also checked by using the numerically exact hierarchical equations of motion approach. From our fitting result of the scaling function, it is found that the Kondo temperature can be determined by the maximum of the spin thermocurrent at T/TK=0.383 .

Coherent states in microwave-induced resistance oscillations and zero resistance states

We investigate irradiated high-mobility two-dimensional electron systems (2DES) under low or moderated magnetic fields. These systems present microwave-induced magnetoresistance oscillations (MIRO) which, as we demonstrate, reveal the presence of coherent states of the quantum harmonic oscillator. We also show that the principle of minimum uncertainty of coherent states is at the heart of MIRO and zero-resistance states (ZRS). Accordingly, we are able to explain, based on coherent states, important experimental evidence of these photo-oscillations, such as their physical origin, their periodicity with the inverse of the magnetic field and their peculiar oscillations minima and maxima positions in regards of the magnetic field. Thus, remarkably enough, we come to the conclusion that 2DES, under low magnetic fields, become a system of quasiclassical states or coherent states and MIRO would be the smoking gun of the existence of these peculiar states in these systems. Published by the American Physical Society 2024

Deep learning bulk spacetime from boundary optical conductivity

We employ a deep learning method to deduce the bulk spacetime from boundary optical conductivity. We apply the neural ordinary differential equation technique, tailored for continuous functions such as the metric, to the typical class of holographic condensed matter models featuring broken translations: linear-axion models. We successfully extract the bulk metric from the boundary holographic optical conductivity. Furthermore, as an example for real material, we use experimental optical conductivity of UPd2Al3, a representative of heavy fermion metals in strongly correlated electron systems, and construct the corresponding bulk metric. To our knowledge, our work is the first illustration of deep learning bulk spacetime from boundary holographic or experimental conductivity data.

The Interaction between Surface Acoustic Wave and Quantum Hall Effects

Abstract Surface Acoustic Wave (SAW) is a powerful technique for investigating quantum phases appearing in two-dimensional electron systems. The electrons respond to the piezoelectric field of SAW through screening, attenuating its amplitude and shifting its velocity, which is described by the relaxation model. In this work, we systematically study this interaction using orders of magnitude lower SAW amplitude than that in previous studies. At high magnetic fields when electrons form highly correlated states such as the quantum Hall effect, we observe an anomalously large attenuation of SAW while the acoustic speed remains considerably high, inconsistent with the conventional relaxation model. This anomaly exists only when the SAW power is sufficiently low.

Giant Tunability of Intersubband Transitions and Quantum Hall Quartets in Few-Layer InSe Quantum Wells.

A two-dimensional (2D) quantum electron system is characterized by quantized energy levels, or subbands, in the out-of-plane direction. Populating higher subbands and controlling the intersubband transitions have wide technological applications such as optical modulators and quantum cascade lasers. In conventional materials, however, the tunability of intersubband spacing is limited. Here we demonstrate electrostatic population and characterization of the second subband in few-layer InSe quantum wells, with giant tunability of its energy, population, and spin-orbit coupling strength, via the control of not only layer thickness but also the out-of-plane displacement field. A modulation of as much as 350% or over 250 meV is achievable, underscoring the promise of InSe for tunable infrared and THz sources, detectors, and modulators.

Modelling thermal energy transfer in a femtosecond pulsed laser ablation of metal using a coupled spring-mass oscillator

Femtosecond pulsed laser ablation (fs-PLA) is an interesting yet complicated field of study especially for undergraduate students entering the field. Hence, a bridging concept using classical and mechanical analog will be helpful. In this paper, we modelled the thermal energy transfer between electron and lattice system in a fs-PLA of metal described by two temperature model (TTM) using a coupled spring-mass oscillator. This was achieved by providing correspondence of TTM parameters to the coupled spring-mass oscillator, with temperature as position, electron thermal conductivity as coefficient of friction, electron-phonon coupling factor as spring term, electron/lattice heat capacity as the mass m 1/m 2 respectively, and laser source term as the driving force. The thermophysical properties considered are temperature dependent leading to position dependent parameters of coupled spring-mass oscillator. Results showed that the coupled spring-mass oscillator exhibit many behavior similar to the TTM. Additionally, maximum positions achieved by m 2 behave similarly with maximum lattice temperature after achieving certain threshold value. However, many features of TTM such as spatial dependence and crater formation are not observed in the coupled spring-mass oscillator. Despite its limitation, the coupled spring-mass oscillator model was able to represent many features of the thermal energy transfer of fs-PLA, and could be an easy and useful model in understanding fs-PLA.

Structure, Antioxidant Activity and Antimicrobial Study of Light Lanthanide Complexes with p-Coumaric Acid.

This paper presents the results of a study of the effects of the lanthanide ions Ce3+, Pr3+, Nd3+ and Sm3+ on the electronic structure and antioxidant and biological (antimicrobial and cytotoxic) properties of p-coumaric acid (p-CAH2). Structural studies were conducted via spectroscopic methods (FTIR, ATR, UV). Thermal degradation studies of the complexes were performed. The results are presented in the form of TG, DTG and DSC curves. Antioxidant properties were determined via activity tests against DPPH, ABTS and OH radicals. The reducing ability was tested via CUPRAC assays. Minimum inhibitory concentrations (MICs) of the ligand and lanthanide complexes were determined on E. coli, B. subtilis and C. albicans microorganisms. The antimicrobial activity was also determined using the MTT assay. The results were presented as the relative cell viability of C. albicans, P. aeruginosa, E. coli and S. aureus compared to controls and expressed as percentages. In the obtained complexes in the solid phase, lanthanide ions coordinate three ligands in a bidentate chelating coordination mode through the carboxyl group of the acid. Spectroscopic analysis showed that lanthanide ions increase the aromaticity of the pi electron system of the ligand. Thermal analysis showed that the complexes are hydrated and have a higher thermal stability than the ligand. The products of thermal decomposition of the complexes are lanthanide oxides. In the aqueous phase, the metal combines with the ligand in a 1:1 molar ratio. Antioxidant activity tests showed that the complexes have a similar ability to remove free radicals. ABTS and DPPH tests showed that the complexes have twice the ability to neutralise radicals than the ligand, and a much higher ability to remove the hydroxyl radical. The abilities of the complexes and the free ligand to reduce Cu2+ ions in the CUPRAC test are at a similar level. Lanthanide complexes of p-coumaric acid are characterised by a higher antimicrobial capacity than the free ligand against Escherichia coli bacteria, Bacillus subtilis and Candida albicans fungi.

Direct versus indirect excitation of ultrafast magnetization dynamics in FeNi alloys

Ultrafast demagnetization can be induced either coherently by direct interaction with the optical light field or indirectly via excitation of the electron system, which subsequently couples to the magnetization. An intriguing direct process is optical intersite spin transfer (OISTR), which changes the local magnetic moments during the optical absorption process itself and leads to a potentially coherent net spin transport between two magnetic subsystems. In this paper, we find that both direct and indirect excitation of an FeNi alloy result in identical experimental signatures in transverse magneto-optical measurements in the extreme ultraviolet spectral range, which has been previously interpreted as evidence for the OISTR effect: a delayed onset of the ultrafast response of Ni with respect to Fe as well as an increasing signal for photons probing energies below the Ni resonance. Our findings align with recent theoretical and experimental investigations, which propose alternative explanations of these experimental observations and do not rely on a direct and coherent interaction between light and spin. Instead, the distinctly different magnetization dynamics of Fe and Ni may be governed by intersite spin transfer driven by electron scattering or be the result of element-specific microscopic properties such as inhomogeneous spin-orbit coupling or electron magnon scattering. Published by the American Physical Society 2024

High-Field Electron Transport and High Saturation Velocity in Multilayer Indium Selenide Transistors.

Creating a high-frequency electron system demands a high saturation velocity (υsat). Herein, we report the high-field transport properties of multilayer van der Waals (vdW) indium selenide (InSe). The InSe is on a hexagonal boron nitride substrate and encapsulated by a thin, noncontinuous In layer, resulting in an impressive electron mobility reaching 2600 cm2/(V s) at room temperature. The high-mobility InSe achieves υsat exceeding 2 × 107 cm/s, which is superior to those of other gapped vdW semiconductors, and exhibits a 50-60% improvement in υsat when cooled to 80 K. The temperature dependence of υsat suggests an optical phonon energy (ℏωop) for InSe in the range of 23-27 meV, previously reported values for InSe. It is also notable that the measured υsat values exceed what is expected according to the optical phonon emission model due to weak electron-phonon scattering. The superior υsat of our InSe, despite its relatively small ℏωop, reveals its potential for high-frequency electronics, including applications to control cryogenic quantum computers in close proximity.

Accurate Excitation Energies of Point Defects from Fast Particle-Particle Random Phase Approximation Calculations.

We present an efficient particle-particle random phase approximation (ppRPA) approach that predicts accurate excitation energies of point defects, including the nitrogen-vacancy (NV-) and silicon-vacancy (SiV0) centers in diamond and the divacancy center (VV0) in 4H silicon carbide, with errors of ±0.2 eV compared with experimental values. Starting from the (N + 2)-electron ground state calculated with density functional theory (DFT), the ppRPA excitation energies of the N-electron system are calculated as the differences between the two-electron removal energies of the (N + 2)-electron system. We demonstrate that the ppRPA excitation energies converge rapidly with a few hundred canonical active-space orbitals. We also show that active-space ppRPA has weak DFT starting-point dependence and is significantly cheaper than the corresponding ground-state DFT calculation. This work establishes ppRPA as an accurate and low-cost tool for investigating excited-state properties of point defects and opens up new opportunities for applications of ppRPA to periodic bulk materials.

Chemically Tailored Semiconductor Moiré Superlattices of Janus Heterobilayers

Janus monolayers of transition metal dichalcogenides (TMDCs) are promising building blocks for moiré superlattices because of their built‐in electric field and clean fabrication process. In particular, Janus TMDC monolayers can be chemically converted from conventional TMDC monolayers by atomic substitution, enabling the direct formation of lattice‐mismatched heterobilayers from TMDC bilayers. However, the moiré superlattices of Janus heterobilayers have not been studied experimentally. Herein, this work reports the fabrication and characterization of semiconductor moiré superlattices in chemically tailored Janus heterobilayers. The MoSSe/MoSe2 (or WSSe/WSe2) Janus heterobilayers are prepared by replacing the top layer Se atoms with S atoms in MoSe2 (or WSe2) bilayer using H2 plasma treatment. Scanning transmission electron microscopy reveals that an average moiré period of about 14 nm formed due to lattice mismatch resulting from the chalcogen substitutions. The cryogenic photoluminescence spectra show sharp, near‐infrared emissions, which are attributed to excitons trapped by moiré potentials based on comparison with theoretical calculations. The Janus‐based heterostructures provide a long‐period moiré system with built‐in potential even for nontwisted heterobilayers, allowing the functionalization of confined and correlated electron systems.

Signatures of Correlated Defects in an Ultraclean Wigner Crystal in the Extreme Quantum Limit.

Low-disorder two-dimensional electron systems in the presence of a strong, perpendicular magnetic field terminate at very small Landau level filling factors in a Wigner crystal (WC), where the electrons form an ordered array to minimize the Coulomb repulsion. The nature of this exotic, many-body, quantum phase is yet to be fully understood and experimentally revealed. Here we probe one of WC's most fundamental parameters, namely, the energy gap that determines its low-temperature conductivity, in record mobility, ultrahigh-purity, two-dimensional electrons confined to GaAs quantum wells. The WC domains in these samples contain ≃1000 electrons. The measured gaps are a factor of three larger than previously reported for lower quality samples, and agree remarkably well with values predicted for the lowest-energy, intrinsic, hypercorrelated bubble defects in a WC made of flux-electron composite fermions, rather than bare electrons. The agreement is particularly noteworthy, given that the calculations are done for disorder-free composite fermion WCs, and there are no adjustable parameters. The results reflect the exceptionally high quality of the samples, and suggest that composite fermion WCs are indeed more stable compared to their electron counterparts.

Ordered phases and superconductivity in two-dimensional electron systems subject to pair spin-orbit interaction

Pair spin-orbit interaction can emerge in strongly interacting systems characterized by a large spin-orbit coupling. Here we study the role of this interaction in stabilizing ordered and unconventional superconducting phases. We find that, if the system avoids superconductivity, the order realized is a combination of charge density and spin-vorticity waves. The latter is reminiscent of a loop-current state, albeit in the spin channel, rather than in the charge channel. If the system becomes superconducting, the order parameter assumes the form of a paired density wave, i.e., pairing occurs at finite momentum. Intriguingly, one of the possible pairings acquires a form analogous to Amperean superconductivity. However, the order parameter here is always a blend of paired density wave and Amperean pairing, rather than being purely one or the other. Published by the American Physical Society 2024

Non-perturbative intertwining between spin and charge correlations: A ``smoking gun'' single-boson-exchange result

We study the microscopic mechanism controlling the interplay between local charge and local spin fluctuations in correlated electron systems via a thorough investigation of the generalized on-site charge susceptibility of several fundamental many-electron models, such as the Hubbard atom, the Anderson impurity model, and the Hubbard model. By decomposing the numerically determined generalized susceptibility in terms of physically transparent single-boson exchange processes, we unveil the microscopic mechanisms responsible for the breakdown of the self-consistent many-electron perturbation expansion. In particular, we unambiguously identify the origin of the significant suppression of its diagonal entries in (Matsubara) frequency space and the slight increase of the off-diagonal ones which cause the breakdown. The suppression effect on the diagonal elements originates directly from the electronic scattering on local magnetic moments, reflecting their increasingly longer lifetime as well as their enhanced effective coupling with the electrons. Instead, the slight and diffuse enhancement of the off-diagonal terms can be mostly ascribed to multiboson scattering processes. The strong intertwining between spin and charge sectors is partly weakened at the Kondo temperature due to a progressive reduction of the effective spin-fermion coupling of local magnetic fluctuations in the low frequency regime. Our analysis, thus, clarifies the precise mechanism through which the physical information is transferred between different scattering channels of interacting electron problems and highlights the pivotal role played by such an intertwining in the physics of correlated electrons beyond the perturbative regime.

A simple coordinate transformation method for quickly locating the features of interest in TEM samples.

We developed a simple coordinate transformation method for quickly locating features of interest (FOIs) of samples in transmission electron microscope (TEM). The method is well suited for conducting sample searches in aberration-corrected scanning/transmission electron microscopes (S/TEM), where the survey can be very time-consuming because of the limited field of view imposed by the highly excited objective lens after fine-tuning the aberration correctors. For implementation, a digital image of the sample and the TEM holder was captured using a simple stereo-optical microscope. Naturally presented geometric patterns on the holder were referenced to construct a projective transformation between the electron and optical coordinate systems. The test results demonstrated that the method was accurate and required no electron microscope or specimen holder modifications. Additionally, it eliminated the need to mount the sample onto specific patterned TEM grids or deposit markers, resulting in universal applications for most TEM samples, holders and electron microscopes for fast FOI identification. Furthermore, we implemented the method into a Gatan script for graphical-user-interface-based step-by-step instructions. Through online communication, the script enabled real-time navigation and tracking of the motion of samples in TEM on enlarged optical images with a panoramic view.