arXiv subjects

Aki Pulkkinen

Publications and source records attributed to Aki Pulkkinen.

At least 19 recordsLinked to original sources

arXiv2026

ASE2SPRKKR: a unified Python framework integrating the Spin-Polarized Relativistic Korringa-Kohn-Rostoker method into the Atomic Simulation Environment

The Spin-Polarized Relativistic Korringa-Kohn-Rostoker (SPR-KKR) is an all-electron ab-initio multiple-scattering code that provides unique capabilities for treating chemical disorder, finite-temperature magnetism, relativistic effects, and spectroscopic properties of various types of solids through its fundamental formulation in terms of the single-particle Green's function rather than eigenstates. We present ASE2SPRKKR, a comprehensive Python interface that integrates SPR-KKR into the Atomic Simulation Environment (ASE), making SPR-KKR more accessible, streamlined, and uniform. Our implementation extends the ASE's Atoms object to handle fractional site occupations for coherent-potential-approximation calculations while maintaining full compatibility with ASE's extensive ecosystem of structure builders, optimizers, and analysis tools. Automated input generation with validation, comprehensive output parsing, and direct MPI support enable seamless integration into high-throughput and multi-method workflows. We demonstrate the interface through representative applications: semi-infinite surface calculations reproducing Rashba-split Au(111) surface states; one-step photoemission modeling capturing matrix-element effects; exchange-parameter extraction for atomistic spin dynamics; and X-ray absorption spectroscopy including magnetic circular dichroism. Beyond these demonstrations, ASE2SPRKKR is designed with transferability as a first-class concern. By grounding its architecture in FAIR principles of Findability, Accessibility, Interoperability, and Reusability, it establishes a replicable blueprint for bringing other specialized Green's function and first-principles codes into the collaborative, reproducible workflows that modern materials discovery requires.

cond-mat.mtrl-sci↗

arXiv2026

Magnetic field-induced momentum-dependent symmetry breaking in a kagome superconductor

When multiple degrees of freedom share similar energy scales in quantum materials, intertwined electronic orders, which exhibit broken symmetries, are often strongly coupled. Recent studies on kagome superconductors such as CsV$_3$Sb$_5$ report rotational and time-reversal symmetry breaking linked to a charge density wave. Here, we observe a momentum-selective response of the electronic structure of CsV$_3$Sb$_5$ to an external magnetic field. By performing angle-resolved photoemission spectroscopy in a tuneable magnetic field, we demonstrate that the response of the electronic structure is compatible with piezomagnetism along with strong orbital selectivity. Our results show that the origin of the time-reversal symmetry breaking is associated with the vanadium Van Hove singularities at the onset of the charge density wave order. We also demonstrate the presence of fluctuations beyond the charge ordering temperature. Our results reveal that magnetic fields can be used as tuning knobs for disentangling intertwined orders in the momentum space for quantum materials.

cond-mat.str-el↗

arXiv2025

Detection of Image Potential States above the vacuum level in GeTe

The ferroelectric semiconductor α-GeTe(111) has attracted significant attention in the last decade due to its unique properties, with extensive studies focusing on its occupied electronic bandstructure. In contrast, its unoccupied states - particularly those near the conduction band minimum - remain largely unexplored. In an effort to characterize those states, we surprisingly observe three image potential states (IPS) in α-GeTe(111) extending up to 0.8 eV above the vacuum level. Using time and angle-resolved photoemission spectroscopy, we resolve the full parabolic dispersions of the first three IPS and determine their binding energies. Our analysis, combined with Bloch spectral function calculations, reveals that the unexpected persistence of IPS above the vacuum level originates from strong dipole transitions and the presence of large electron reservoirs in GeTe.

cond-mat.str-el↗

arXiv2025

Probing the semiconductor-to-dirac semimetal transition in Na-Sb-Bi alloys with x-ray Compton scattering

We discuss electron redistribution during the semiconductor-to-Dirac semimetal transition in Na-Sb-Bi alloys using x-ray Compton scattering experiments combined with first-principles electronic structure modeling. A robust signature of the semiconductor-to-Dirac semimetal transition is identified in the spherically averaged Compton profile. We demonstrate how the number of electrons involved in this transition can be estimated to provide a novel descriptor for quantifying the strength of spin-orbit coupling responsible for driving the transition. The associated theoretical deviation of the Born charge of Na in Na$_3$Bi from the expected ionic charge of +1 is found to be consistent with the corresponding experimental value of about 10%. Our study also shows the sensitivity of the Compton scattering technique toward capturing the spillover of Bi 6p relativistic states onto Na sites.

cond-mat.mtrl-sci↗

arXiv2025

Transition from Optically Excited to Intrinsic Spin Polarization in WSe$_2$

Layered 2D van der Waals materials, such as transition metal dichalcogenides, are promising for nanoscale spintronic and optoelectronic applications. Harnessing their full potential requires understanding both intrinsic transport and the dynamics of optically excited spin and charge carriers -- particularly the transition between excited spin polarization and the conduction band's intrinsic spin texture. Here, we investigate the spin polarization of the conduction bands of bulk WSe$_2$ using static and time-resolved spin-resolved photoemission spectroscopy, complemented by photocurrent calculations. Electron doping reveals the intrinsic spin polarization, while time-resolved measurements trace the evolution of excited spin carriers. We find that intervalley scattering is spin-conserving, with spin transport initially governed by photoexcited carriers and aligning with the intrinsic conduction band polarization after $\sim$150 fs.

cond-mat.mes-hall↗

arXiv2025

Kramers nodal lines in intercalated TaS$_2$ superconductors

Kramers degeneracy is one fundamental embodiment of the quantum mechanical nature of particles with half-integer spin under time reversal symmetry. Under the chiral and noncentrosymmetric achiral crystalline symmetries, Kramers degeneracy emerges respectively as topological quasiparticles of Weyl fermions and Kramers nodal lines (KNLs), anchoring the Berry phase-related physics of electrons. However, an experimental demonstration for ideal KNLs well isolated at the Fermi level is lacking. Here, we establish a class of noncentrosymmetric achiral intercalated transition metal dichalcogenide superconductors with large Ising-type spin-orbit coupling, represented by In$_x$TaS$_2$, to host an ideal KNL phase. We provide evidence from angle-resolved photoemission spectroscopy with spin resolution, angle-dependent quantum oscillation measurements, and ab-initio calculations. Our work not only provides a realistic platform for realizing and tuning KNLs in layered materials, but also paves the way for exploring the interplay between KNLs and superconductivity, as well as applications pertaining to spintronics, valleytronics, and nonlinear transport.

cond-mat.supr-con↗

arXiv2025

Reconstructing initial pressure and speed of sound distributions simultaneously in photoacoustic tomography

Image reconstruction in photoacoustic tomography relies on an accurate knowledge of the speed of sound in the target. However, the speed of sound distribution is not generally known, which may result in artefacts in the reconstructed distribution of initial pressure. Therefore, reconstructing the speed of sound simultaneously with the initial pressure would be valuable for accurate imaging in photoacoustic tomography. Furthermore, the speed of sound distribution could provide additional valuable information about the imaged target. In this work, simultaneous reconstruction of initial pressure and speed of sound in photoacoustic tomography is studied. This inverse problem is known to be highly ill-posed. To overcome this, we study an approach where the ill-posedness is alleviated by utilising multiple photoacoustic data sets that are generated by different initial pressure distributions within the same imaged target. Then, these initial pressure distributions are reconstructed simultaneously with the speed of sound distribution. A methodology for solving this minimisation problem is formulated using a gradient-based iterative approach equipped with bound constraints and a multigrid approach. The methodology was evaluated with numerical simulations. Different approaches for generating multiple initial pressure distributions and their effect on the solution of the image reconstruction problem were studied. The results show that initial pressure and speed of sound can be simultaneously reconstructed from photoacoustic data. Furthermore, utilising multiple initial pressure distributions improves the reconstructions such that the locations of initial pressure and speed of sound inhomogeneities can be better distinguished and image artifacts are reduced.

physics.med-ph↗

arXiv2025

Layered Multiple Scattering Approach to Hard X-ray Photoelectron Diffraction: Theory and Application

Photoelectron diffraction (PED) is a powerful and essential experimental technique for resolving the structure of surfaces with sub-angstrom resolution. In the high energy regime, researchers in angle-resolved photoemission spectroscopy (ARPES) observe modulating patterns attributed to X-ray-PED (XPD) effects. This is accompanied by other challenges such as low cross-sections, significant photon momentum transfer, and non-negligible phonon scattering. Overall, XPD is not only an advantageous approach but also exhibits unexpected effects. To disentangle these diffraction influences, we present a PED implementation for the SPRKKR package that utilizes multiple scattering theory and a one-step model in the photoemission process. Unlike real-space implementations of the multiple scattering XPD formalism, we propose a k-space implementation based on the layer KKR method. The main advantage of this method is its ability to address a very broad kinetic energy range (20-8000 eV) without convergence problems related to angular momentum and cluster size. Furthermore, the so-called alloy analogy model can be used to simulate XPD at finite temperatures as well as XPD effects observed in soft and hard X-ray ARPES. For practical applications, we have calculated the circular dichroism in angular distributions (CDAD) associated with core-level photoemission of 2p from Si(100) and 3p from Ge(100). Photoelectrons are excited by hard X-rays (6000 eV) with right and left circularly polarized radiation (RCP and LCP, respectively).

cond-mat.str-el↗

arXiv2025

Unveiling Fine Structure and Energy-driven Transition of Photoelectron Kikuchi Diffraction

The intricate fine structure of Kikuchi diffraction plays a vital role in probing phase transformations and strain distributions in functional materials, particularly in electron microscopy. Beyond these applications, it also proves essential in photoemission spectroscopy (PES) at high photon energies, aiding in the disentanglement of complex angle-resolved PES data and enabling emitter-site-specific studies. However, the detection and analysis of these rich faint structures in photoelectron diffraction (PED), especially in the hard X-ray regime, remain highly challenging, with only a limited number of simulations successfully reproducing these patterns. The strong energy dependence of Kikuchi patterns further complicates their interpretation, necessitating advanced theoretical approaches. To enhance structural analysis, we present a comprehensive theoretical study of fine diffraction patterns and their evolution with energy by simulating core-level emissions from Ge(100) and Si(100). Using multiple-scattering theory and the fully relativistic one-step photoemission model, we simulate faint pattern networks for various core levels across different kinetic energies (106 eV - 4174 eV), avoiding cluster size convergence issues inherent in cluster-based methods. Broadening in patterns is discussed via the inelastic scattering treatment. For the first time, circular dichroism has been observed and successfully reproduced in the angular distribution of Si (100) 1s, revealing detailed features and asymmetries up to 31%. Notably, we successfully replicate experimental bulk and more "surface-sensitivity" diffraction features, further validating the robustness of our simulations. The results show remarkable agreement with the experimental data obtained using circularly polarized radiations, demonstrating the potential of this methodology for advancing high-energy PES investigations.

cond-mat.mtrl-sci↗

arXiv2025

Revealing electronic correlations in YNi$_2$B$_2$C using photoemission spectroscopy

We present a combined density functional theory (DFT), one-step model of photoemission, and soft x-ray angle-resolved photoemission spectroscopy (SX-ARPES) study of the electronic structure of the quaternary borocarbide superconductor YNi$_2$B$_2$C. Our analysis reveals the presence of moderate electronic correlations beyond the semilocal DFT within the generalized gradient approximation. We show that DFT and the full potential Korringa-Kohn-Rostoker method combined with the dynamical mean field theory (DFT+DMFT) with average Coulomb interaction U = 3.0 eV and the exchange energy J = 0.9 eV applied to the Ni d-states are necessary for reproducing the experimentally observed SX-ARPES spectra.

cond-mat.str-el↗

arXiv2025

Reexamining Circular Dichroism in Photoemission From a Topological Insulator

The orbital angular momentum (OAM) of electron states is an essential ingredient for topological and quantum geometric quantities in solids. For example, Dirac surface states with helical spin- and orbital-angular momenta are a hallmark of a 3D topological insulator. Angle-resolved photoemission spectroscopy (ARPES) with variable circular light polarization, known as circular dichroism (CD), has been assumed to be a direct probe of OAM and, by proxy, of the Berry curvature of electronic bands in energy- and momentum-space. Indeed, topological surface states have been shown to exhibit angle-dependent CD (CDAD), and more broadly, CD is often interpreted as evidence of spin-orbit coupling. Meanwhile, it is well-established that CD originates from the photoemission matrix elements, which can have extrinsic contributions related to the experimental geometry and the inherently broken inversion symmetry at the sample surface. Therefore, it is important to broadly examine CD-ARPES to determine the scenarios in which it provides a robust probe of intrinsic material physics. We performed CD-ARPES on the canonical topological insulator $\mathrm{Bi}_2\mathrm{Se}_3$ over a wide range of incident photon energies. Not only do we observe angle-dependent CD in the surface states, as expected, but we also find CD of a similar magnitude in virtually all bulk bands. Since OAM is forbidden by inversion symmetry in the bulk, we conclude this originates from symmetry-breaking in the photoemission process. Comparison with theoretical calculations supports this view and suggests that $\textit{hidden}$ OAM - localized to atomic sites within each unit cell - contributes significantly. Additional effects, including inter-atomic interference and final-state resonances, are responsible for the rapid variation of the CDAD signal with photon energy.

cond-mat.mtrl-sci↗

arXiv2024

Persistent flat band splitting and strong selective band renormalization in a kagome magnet thin film

Magnetic kagome materials provide a fascinating playground for exploring the interplay of magnetism, correlation and topology. Many magnetic kagome systems have been reported including the binary FemXn (X=Sn, Ge; m:n = 3:1, 3:2, 1:1) family and the rare earth RMn6Sn6 (R = rare earth) family, where their kagome flat bands are calculated to be near the Fermi level in the paramagnetic phase. While partially filling a kagome flat band is predicted to give rise to a Stoner-type ferromagnetism, experimental visualization of the magnetic splitting across the ordering temperature has not been reported for any of these systems due to the high ordering temperatures, hence leaving the nature of magnetism in kagome magnets an open question. Here, we probe the electronic structure with angle-resolved photoemission spectroscopy in a kagome magnet thin film FeSn synthesized using molecular beam epitaxy. We identify the exchange-split kagome flat bands, whose splitting persists above the magnetic ordering temperature, indicative of a local moment picture. Such local moments in the presence of the topological flat band are consistent with the compact molecular orbitals predicted in theory. We further observe a large spin-orbital selective band renormalization in the Fe d_xy+d_(x^2-y^2 ) spin majority channel reminiscent of the orbital selective correlation effects in the iron-based superconductors. Our discovery of the coexistence of local moments with topological flat bands in a kagome system echoes similar findings in magic-angle twisted bilayer graphene, and provides a basis for theoretical effort towards modeling correlation effects in magnetic flat band systems.

cond-mat.mes-hall↗

arXiv2024

Two-dimensional to bulk crossover of the WSe$_2$ electronic band structure

Transition Metal Dichalcogenides (TMD) are layered materials obtained by stacking two-dimensional sheets weakly bonded by van der Waals interactions. In bulk TMD, band dispersions are observed in the direction normal to the sheet plane (z-direction) due to the hybridization of out-of-plane orbitals but no kz-dispersion is expected at the single-layer limit. Using angle-resolved photoemission spectroscopy, we precisely address the two-dimensional to three-dimensional crossover of the electronic band structure of epitaxial WSe$_2$ thin films. Increasing number of discrete electronic states appears in given kz-ranges while increasing the number of layers. The continuous bulk dispersion is nearly retrieved for 6-sheet films. These results are reproduced by calculations going from a relatively simple tight-binding model to a sophisticated KKR-Green's function calculation. This two-dimensional system is hence used as a benchmark to compare different theoretical approaches.

cond-mat.mtrl-sci↗

arXiv2023

Persistence of structural distortion and bulk band Rashba splitting in SnTe above its ferroelectric critical temperature

The ferroelectric semiconductor $α$-SnTe has been regarded as a topological crystalline insulator and the dispersion of its surface states has been intensively measured with angle-resolved photoemission spectroscopy (ARPES) over the last decade. However, much less attention has been given to the impact of the ferroelectric transition on its electronic structure, and in particular on its bulk states. Here, we investigate the low-energy electronic structure of $α$-SnTe with ARPES and follow the evolution of the bulk-state Rashba splitting as a function of temperature, across its ferroelectric critical temperature of about $T_c\sim 110$ K. Unexpectedly, we observe a persistent band splitting up to room temperature, which is consistent with an order-disorder contribution to the phase transition that requires the presence of fluctuating local dipoles above $T_c$. We conclude that no topological surface state can occur at the (111) surface of SnTe, at odds with recent literature.

cond-mat.mtrl-sci↗

arXiv2022

Benchmark problems for transcranial ultrasound simulation: Intercomparison of compressional wave models

Computational models of acoustic wave propagation are frequently used in transcranial ultrasound therapy, for example, to calculate the intracranial pressure field or to calculate phase delays to correct for skull distortions. To allow intercomparison between the different modeling tools and techniques used by the community, an international working group was convened to formulate a set of numerical benchmarks. Here, these benchmarks are presented, along with intercomparison results. Nine different benchmarks of increasing geometric complexity are defined. These include a single-layer planar bone immersed in water, a multi-layer bone, and a whole skull. Two transducer configurations are considered (a focused bowl and a plane piston), giving a total of 18 permutations of the benchmarks. Eleven different modeling tools are used to compute the benchmark results. The models span a wide range of numerical techniques, including the finite-difference time-domain method, angular-spectrum method, pseudospectral method, boundary-element method, and spectral-element method. Good agreement is found between the models, particularly for the position, size, and magnitude of the acoustic focus within the skull. When comparing results for each model with every other model in a cross comparison, the median values for each benchmark for the difference in focal pressure and position are less than 10\% and 1 mm, respectively. The benchmark definitions, model results, and intercomparison codes are freely available to facilitate further comparisons.

physics.comp-ph↗

arXiv2021

Break of symmetry at the surface of IrTe$_2$ upon phase transition measured by X-ray photoelectron diffraction

IrTe$_2$ undergoes a series of charge-ordered phase transitions below room temperature that are characterized by the formation of stripes of Ir dimers of different periodicities. Full hemispherical X-ray photoelectron diffraction (XPD) experiments have been performed to investigate the atomic position changes undergone near the surface of $1T-$IrTe$_2$ in the first-order phase transition, from the $(1\times1)$ phase to the $(5\times1)$ phase. Comparison between experiment and simulation allows us to identify the consequence of the dimerization on the Ir atoms local environment. We report that XPD permits to unveil the break of symmetry of IrTe$_2$ trigonal to a monoclonic unit cell and confirm the occurence of the $(5\times1)$ reconstruction within the first few layers below the surface with a staircase-like stacking of dimers.

cond-mat.mtrl-sci↗

arXiv2020

Superconducting and Antiferromagnetic Properties of Dual-Phase V$_3$Ga

The binary compound V$_3$Ga can exhibit two near-equilibrium phases, consisting of the A15 structure that is superconducting, and the Heusler D0$_3$ structure that is semiconducting and antiferromagnetic. Density functional theory calculations show that the two phases are closely degenerate, being separated by only ~10 meV/atom. Magnetization measurements on bulk-grown samples show superconducting behavior below 14 K. These results indicate the possibility of using V$_3$Ga for quantum technology devices utilizing both superconductivity and antiferromagnetism at the same temperature.

cond-mat.mtrl-sci↗

arXiv2020

Exchange-correlation corrections for electronic properties of half-metallic Co$_2$FeSi and nonmagnetic semiconductor CoFeTiAl

We consider two cobalt-based full-Heusler compounds CoFeTiAl and Co$_2$FeSi, for which Coulomb correlation effects play an important role. Since the standard GGA scheme does not provide a precise description of the electronic properties near the Fermi level, we use a meta-GGA functional capable to improve the description of the electronic properties of CoFeTiAl and Co$_2$FeSi. In particular, we find a better agreement with the experiment for the magnetic moment and the energy-band gap. Moreover, our calculations show that pressure enhances the insulating properties of Co$_2$FeSi and CoTiFeAl.

cond-mat.mtrl-sci↗