arXiv subjects

Peter Elliott

Publications and source records attributed to Peter Elliott.

At least 19 recordsLinked to original sources

arXiv2026

All optical ultrafast pure spin current in the altermagnet Cr$_2$SO

All-optical generation of pure spin current -- the flow of spin in the absence of a corresponding charge flow -- relies on a symmetry based compensation of valley charge. The 2d $d$-wave altermagnets, ideal spintronics materials due to a very low spin-orbit coupling, possess a magnetic point group and highly anisotropic valley manifolds that would appear to preclude such current compensation, excluding them as materials for the ultrafast generation of pure spin current. Here we show that infra-red valley excitation combined with a THz pulse envelope allows the generation of large and nearly 100\% pure spin currents in the altermagnet Cr$_2$SO. Our approach is based on a valley selection rule coupling linearly polarized light to spin opposite valleys, along with the intrinsic momentum shift that a co-occurring THz pulse imbues a valley spin excitation with. These results thus provide a practical and all-optical route to the generation of pure spin current in $d$-wave 2d altermagnets, opening a route to lightwave control of spin in an environment with very low intrinsic spin mixing.

cond-mat.mtrl-sci↗

arXiv2025

Valley polarization of graphene via the saddle point

Graphene, and other members of the monolayer Xene family, represent an ideal materials platform for "valleytronics", the control of valley localized charge excitations. The absence of a gap in these semi-metals, however, precludes valley excitation by circularly polarized light pulses, sharply circumscribing the possibility of a lightwave valleytronics in these materials. Here we show that combining a deep ultraviolet linearly polarized light pulse with a THz envelope can induce highly valley polarized states in graphene. This dual frequency lightform operates by (i) the deep ultraviolet pulse activating a selection rule at the M saddle points and (ii) the THz pulse displacing the M point excitation to one of the low-energy K valleys. Employing both tight-binding and state-of-the-art time dependent density functional theory, we show that such a pulse results in a near perfect valley polarized excitation in graphene, thus providing a route via the saddle point to a lightwave valleytronics in the gapless Xene family.

physics.optics↗

arXiv2025

Ultrafast Saddletronics

Low energy valleys in the band structure of 2d materials represent a potential route to the ultrafast writing of information in quantum matter by laser light, with excited charge at the K or K$^\ast$ valleys representing the fundamental states of 1 and 0. Here we demonstrate that a second electronic feature, the saddle point, is endowed with lightwave control over information states. Linearly polarized light is shown to excite 2 of the 3 inequivalent M point saddles in graphene, generating three possible excited configurations, with which of these are realised determined by the polarization vector direction. We show that saddle excitation is highly robust, with "saddle polarized" states created both in the sub-cycle strong field regime and the long time limit of extended multi-cycle pulses. Our findings, applicable to other members of the graphene family and Xenes such as stanene, point towards a rich and ultrafast light based manipulation of matter based on the saddle point.

cond-mat.mes-hall↗

arXiv2023

How closely does transient magnetic linear dichroism follow the spin moment?

In highly out-of-equilibrium states of matter, such as those induced by a pump laser, the applicability of well established spectroscopic probes of magnetic order are called into question. Here we address the validity of x-ray absorption techniques in pump laser conditions, focusing on magnetic linear dichroism (MLD), a crucial probe of antiferromagnetic (AFM) order. We directly compute the dynamics of the square of the spin moment and compare to those obtained via the MLD response. For AFM FePd the agreement between these distinct routes to the magnetic moment severely degrades at pulse fluences greater than 1 mJ/cm$^2$, indicating a breakdown of the MLD response as an accurate probe of the transient moment. This contrasts with the MLD for ferromagnetic FePt which reliably tracks the moment for fluences (and absorbed energies) up to an order of magnitude greater than the breakdown threshold for AFM FePd. The underlying microscopic reason for this we find to be increased laser induced excitations out of the $d$-band in AFM FePd, where this increase is made possible by the AFM pseudogap.

cond-mat.mtrl-sci↗

arXiv2022

Nanomechanical spectroscopy of 2D materials

We introduce a nanomechanical platform for fast and sensitive measurements of the spectrally-resolved optical dielectric function of 2D materials. At the heart of our approach is a suspended 2D material integrated into a nanomechanical resonator illuminated by a wavelength-tunable laser source. From the heating-related frequency shift of the resonator as well as its optical reflection measured as a function of photon energy, we obtain the real and imaginary parts of the dielectric function. Our measurements are unaffected by substrate-related screening and do not require any assumptions on the underling optical constants. This fast ($\tau_{rise}$ $\sim$ 135 ns), sensitive (noise-equivalent power = 90 $\frac{pW}{\sqrt{Hz}}$ ), and broadband (1.2 $-$ 3.1 eV, extendable to UV-THz) method provides an attractive alternative to spectroscopic or ellipsometric characterisation techniques.

cond-mat.mes-hall↗

arXiv2021

Spin/valley coupled dynamics of electrons and holes at the ${\text{MoS}_{2}-\text{MoSe}_{2}}$ interface

The coupled spin and valley degrees of freedom in transition metal dichalcogenides (TMDs) are considered a promising platform for information processing. Here, we use a TMD heterostructure ${\text{MoS}_{2}-\text{MoSe}_{2}}$ to study optical pumping of spin/valley polarized carriers across the interface and to elucidate the mechanisms governing their subsequent relaxation. By applying time-resolved Kerr and reflectivity spectroscopies, we find that the photoexcited carriers conserve their spin for both tunneling directions across the interface. Following this, we measure dramatically different spin/valley depolarization rates for electrons and holes, $\sim 30\,{\text{ns}}^{-1}$ and $< 1\,{\text{ns}}^{-1}$, respectively and show that this difference relates to the disparity in the spin-orbit splitting in conduction and valence bands of TMDs. Our work provides insights into the spin/valley dynamics of free carriers unaffected by complex excitonic processes and establishes TMD heterostructures as generators of spin currents in spin/valleytronic devices.

cond-mat.mes-hall↗

arXiv2019

Think-aloud interviews: A tool for exploring student statistical reasoning

Think-aloud interviews have been a valuable but underused tool in statistics education research. Think-alouds, in which students narrate their reasoning in real time while solving problems, differ in important ways from other types of cognitive interviews and related education research methods. Beyond the uses already found in the statistics literature -- mostly validating the wording of statistical concept inventory questions and studying student misconceptions -- we suggest other possible use cases for think-alouds and summarize best-practice guidelines for designing think-aloud interview studies. Using examples from our own experiences studying the local student body for our introductory statistics courses, we illustrate how research goals should inform study-design decisions and what kinds of insights think-alouds can provide. We hope that our overview of think-alouds encourages more statistics educators and researchers to begin using this method.

stat.OT↗

arXiv2016

Density-Matrix Propagation Driven by Semiclassical Correlation

Methods based on propagation of the one-body reduced density-matrix hold much promise for the simulation of correlated many-electron dynamics far from equilibrium, but difficulties with finding good approximations for the interaction term in its equation of motion have so far impeded their application. These difficulties include the violation of fundamental physical principles such as energy conservation, positivity conditions on the density, or unchanging natural orbital occupation numbers. We review some of the recent efforts to confront these problems, and explore a semiclassical approximation for electron correlation coupled to time-dependent Hartree-Fock propagation. We find that this approach captures changing occupation numbers, and excitations to doubly-excited states, improving over TDHF and adiabatic approximations in density-matrix propagation. However, it does not guarantee $N$-representability of the density-matrix, consequently resulting sometimes in violation of positivity conditions, even though a purely semiclassical treatment preserves these conditions.

physics.chem-ph↗

arXiv2015

Corrections to Thomas-Fermi densities at turning points and beyond

Uniform semiclassical approximations for the number and kinetic-energy densities are derived for many non-interacting fermions in one-dimensional potentials with two turning points. The resulting simple, closed-form expressions contain the leading corrections to Thomas-Fermi theory, involve neither sums nor derivatives, are spatially uniform approximations, and are exceedingly accurate.

quant-ph↗

arXiv2014

Almost Exact Exchange At Almost No Cost

A recently developed semiclassical approximation to exchange in one dimension is shown to be almost exact, with essentially no computational cost. The variational stability of this approximation is tested, and its far greater accuracy relative to local density functional calculations demonstrated. Even a fully orbital-free potential-functional calculation (no orbitals of any kind) yields little error relative to exact exchange, for more than one orbital.

physics.chem-ph↗

arXiv2014

Kinetic and potential components of the exact time-dependent correlation potential

The exact exchange-correlation (xc) potential of time-dependent density functional theory has been shown to have striking features. For example, step and peak features are generically found when the system is far from its ground-state, and these depend nonlocally on the density in space and time. We analyze the xc potential by decomposing it into kinetic and interaction potential components, and comparing each with their exact-adiabatic counterparts, for a range of dynamical situations in model one-dimensional (1D) two-electron systems. We find that often, but not always, the kinetic contri- bution is mostly responsible for these features, that are missed by the adiabatic approximation. The adiabatic approximation often makes a smaller error for the potential contribution, which we write in two parts, one being the Coulomb potential due to the time-dependent xc hole. These observations also held in non-equilibrium cases we studied where there are large features in the correlation po- tential although no step structure. In ground-state situations, step and peak structures arise in cases of static correlation, when more than one determinant is essential to describe the interacting state. We investigate the time-dependent natural orbital occupation numbers and find the corresponding relation between these and the dynamical step is more complex than for the ground-state case.

physics.chem-ph↗

arXiv2014

Fundamentals of Time-Resolved Charge-Transfer in Time-Dependent Density Functional Theory

We show that as an electron transfers between closed-shell molecular fragments at large separation, the exact correlation potential of time-dependent density functional theory gradually develops a step and peak structure in the bonding region. This structure has a density-dependence that is non-local both in space and time, and even the exact ground-state exchange-correlation functional fails to cap- ture it. In the complementary case of charge-transfer between open-shell fragments, an initial step and peak vanish as the charge-transfer state is reached. Lack of these structures in usual approxima- tions leads to inaccurate charge-transfer dynamics. This is dramatically illustrated by the complete lack of Rabi oscillations in the dipole moment under conditions of resonant charge-transfer.

physics.chem-ph↗

arXiv2012

Universal Dynamical Steps in the Exact Time-Dependent Exchange-Correlation Potential

We show that the exact exchange-correlation potential of time-dependent density-functional theory displays dynamical step structures that have a spatially non-local and time non-local dependence on the density. Using one-dimensional two-electron model systems, we illustrate these steps for a range of non-equilibrium dynamical situations relevant for modeling of photo-chemical/physical processes: field-free evolution of a non-stationary state, resonant local excitation, resonant complete charge-transfer, and evolution under an arbitrary field. Lack of these steps in usual approximations yield inaccurate dynamics, for example predicting faster dynamics and incomplete charge transfer.

physics.chem-ph↗

arXiv2012

Community detection using spectral clustering on sparse geosocial data

In this article we identify social communities among gang members in the Hollenbeck policing district in Los Angeles, based on sparse observations of a combination of social interactions and geographic locations of the individuals. This information, coming from LAPD Field Interview cards, is used to construct a similarity graph for the individuals. We use spectral clustering to identify clusters in the graph, corresponding to communities in Hollenbeck, and compare these with the LAPD's knowledge of the individuals' gang membership. We discuss different ways of encoding the geosocial information using a graph structure and the influence on the resulting clusterings. Finally we analyze the robustness of this technique with respect to noisy and incomplete data, thereby providing suggestions about the relative importance of quantity versus quality of collected data.

stat.AP↗

arXiv2012

Propagation of Initially Excited States in Time-Dependent Density Functional Theory

Many recent applications of time-dependent density functional theory begin in an initially excited state, and propagate it using an adiabatic approximation for the exchange-correlation potential. This however inserts the excited-state density into a ground-state approximation. By studying a series of model calculations, we highlight the relevance of initial-state dependence of the exact functional when starting in an excited state, and explore the errors inherent in the adiabatic approximation that neglect this dependence.

physics.chem-ph↗

arXiv2011

Electron Correlation via Frozen Gaussian Dynamics

We investigate the accuracy and efficiency of the semiclassical Frozen Gaussian method in describing electron dynamics in real time. Model systems of two soft-Coulomb-interacting electrons are used to study correlated dynamics under non-perturbative electric fields, as well as the excitation spectrum. The results show that a recently proposed method that combines exact-exchange with semiclassical correlation to propagate the one-body density-matrix holds promise for electron dynamics in many situations that either wavefunction or density-functional methods have difficulty describing. The results also however point out challenges in such a method that need to be addressed before it can become widely applicable.

physics.chem-ph↗

arXiv2011

Electronic structure via potential functional approximations

The universal functional of Hohenberg-Kohn is given as a coupling-constant integral over the density as a functional of the potential. Conditions are derived under which potential-functional approximations are variational. Construction via this method and imposition of these conditions are shown to greatly improve the accuracy of the non-interacting kinetic energy needed for orbital-free Kohn-Sham calculations.

cond-mat.other↗

arXiv2011

Perspectives on double-excitations in TDDFT

The adiabatic approximation in time-dependent density functional theory (TDDFT) yields reliable excitation spectra with great efficiency in many cases, but fundamentally fails for states of double excitation character. We discuss how double-excitations are at the root of some of the most challenging problems for TDDFT today. We then present new results for (i) the calculation of autoionizing resonances in the helium atom, (ii) understanding the nature of the double excitations appearing in the quadratic response function, and (iii) retrieving double-excitations through a real-time semiclassical approach to correlation in a model quantum dot.

physics.chem-ph↗