Simulating Transport Properties of Correlated Materials
Simulating Transport Properties of Correlated Materials
Disciplines
Physics, Astronomy (100%)
Keywords
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Correlated Materials,
Thermoelectricity,
Transport Properties,
Intermetallics,
Electronic Structure,
Response Functions
Conventional materials such as copper and silicon form the bulk of todays electronic devices. Detailed theoretical understandings of these materials, in which electronic conduction is governed by weakly interacting charge carriers, have made designing complex functional structures by computer simulations possible. Correlated materials, systems in which electrons interact strongly, represent another vast untapped resource with tremendous potential for transformative technical innovations. Akin to La Ola, in which each football fans cheer is coordinated into a stadium-wide wave, the motion of one electron in these materials is correlated to the motions of all others. Owing to this synchronized behavior, these materials are highly sensitive to external stimuli, making them prime candidates for technical developments of sensors, switches, transistors, and memory storage. Yet realizing the full potential of these materials requires a thorough understanding of their physical behaviors and the ability to efficiently screen a huge pool of materials for promising functionalities, particularly electronic and thermoelectric transport properties. Here we propose to develop a highly efficient methodology for an accurate description of transport properties of correlated materials. This has so far been elusive: the charge propagation in correlated materials invalidates semi-classical Boltzmann-theory, and a full quantum many-particle treatment is too computationally demanding. We hypothesize that for transport properties the essential many-particle effects can be described to a high accuracy by a simple form of the electron dynamics. This will effectively replace one of the most time-consuming steps by an analytical evaluation, speeding up the simulation by at least 100-fold. We will first develop a full-fledged algorithm for realistic materials calculations. Next we will apply this novel methodology to the strongly correlated semiconductor FeSi to describe the still elusive microscopic mechanism behind its Hall and Nernst effect. We will also calculate the transport properties of transition metal dichalcogenides, scrutinizing if, and how, different dopings affect their thermoelectrical properties. Next we will devise a complete architecture that will, for the first time, make high-throughput simulations of correlated materials affordable, without sacrificing any salient features of the many-particle correlations. From the massive amount of data we will generate, we will be able to extract guiding principles for designing high-performance thermoelectrics for waste-heat recovery or maintenance-free refrigerators. Finally we will implement a user-friendly interface oriented to experimentalists that will allow them to make comparisons between phenomenological models and experimental data easily. This project will catalyze interdisciplinary exchange between theoreticians and experimentalists. Our methodology will enable highly efficient identifications of materials with desired properties and establish design guidelines to maximize functionalities. By screening a huge array of materials much larger than what is feasible by experimental surveys, we hope to guide experimentalist towards materials of the future.
A common way to characterize a material is to study how it conducts electricity and heat. These properties can be quantified in transport coefficients that link an external perturbation (an electric or magnetic field, a difference in temperature) to a current (of charge or energy). Besides fundamental insight, transport also describes useful functionalities: For instance, in thermoelectric devices, temperature differences are converted into electricity or vice versa. Hence, an understanding of transport properties and how they can be predicted and optimized is of practical interest. In the Linear Response Transport Centre (LinReTraCe) project, we devised and implemented a physically accurate and numerically efficient methodology for the simulation of various transport properties. A key advance is the capability to capture quantum effects, in particular incoherence, that are beyond dominantly used semi-classical techniques. Roughly speaking, incoherence means that (unlike a classical particle) an electronic state in a solid does not have a sharply defined energy, but its energy follows a more or less broadened probability distribution. An equivalent viewpoint is to say that an electronic state has a finite lifetime. Our algorithm incorporates these effects with no or little additional numerical cost: LinReTraCe is a conceptual upgrade from semi-classical Boltzmann theories and an efficient alternative to sometimes prohibitively expensive full Kubo approaches, allowing us to access previously challenging settings. So where do these quantum effects come to play? We found them to be particularly important in a class of materials relevant for technological applications: narrow-gap semiconductors. There, we discovered that finite lifetimes of intrinsic carriers cause a rich temperature dependence in all transport quantities. Most notably, we provide a new microscopic scenario for the previously puzzling low-temperature saturation of the resistivity in Kondo insulators and d-electron intermetallic semiconductors. The crucial insight is that (one over) the lifetime of valence and conduction electrons is a relevant energy scale that can have an intricate interplay with other scales of the system (the charge gap or temperature). Previous attempts at modelling resistivity and the coefficients of Hall, Seebeck, and Nernst in these systems had to resort to ad hoc extrinsic in-gap impurity levels. The latters energetic positions then controlled much of the temperature dependence. In our more complete theory, characteristic temperatures naturally emerge from the intrinsic electronic structure, providing a new interpretation of experimental measurements. In all, the LinReTraCe software allows simulating and predicting transport properties as well as extracting microscopic information from experiment. With that, we hope to inform the theoretical-experimental dialogue and facilitate the discovery and optimization of material functionalities.
- Technische Universität Wien - 100%
Research Output
- 191 Citations
- 24 Publications
- 1 Datasets & models
- 1 Fundings
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2022
Title LinReTraCe: The Linear Response Transport Centre DOI 10.48550/arxiv.2206.06097 Type Other Author Maggio E -
2022
Title Phase diagram of nickelate superconductors calculated by dynamical vertex approximation DOI 10.48550/arxiv.2201.01220 Type Other Author Held K -
2022
Title Particle-hole asymmetric lifetimes promoted by nonlocal spin and orbital fluctuations in SrVO3 monolayers DOI 10.1103/physrevresearch.4.033253 Type Journal Article Author Pickem M Journal Physical Review Research Pages 033253 Link Publication -
2022
Title Prototypical many-body signatures in transport properties of semiconductors DOI 10.1103/physrevb.105.085139 Type Journal Article Author Pickem M Journal Physical Review B Pages 085139 Link Publication -
2022
Title Phase Diagram of Nickelate Superconductors Calculated by Dynamical Vertex Approximation DOI 10.3389/fphy.2021.810394 Type Journal Article Author Held K Journal Frontiers in Physics Pages 810394 Link Publication -
2023
Title Coulomb engineering of two-dimensional Mott materials DOI 10.1038/s41699-023-00408-x Type Journal Article Author Van Loon E Journal npj 2D Materials and Applications Pages 47 Link Publication -
2023
Title Codebase release 1.1 for LinReTraCe DOI 10.21468/scipostphyscodeb.16-r1.1 Type Journal Article Author Pickem M Journal SciPost Physics Codebases Link Publication -
2023
Title LinReTraCe: The linear response transport centre DOI 10.21468/scipostphyscodeb.16 Type Journal Article Author Pickem M Journal SciPost Physics Codebases Pages 016 Link Publication -
2023
Title Resistance saturation in semi-conducting polyacetylene molecular wires DOI 10.1007/s10825-023-02043-7 Type Journal Article Author Valli A Journal Journal of Computational Electronics Pages 1363-1376 Link Publication -
2023
Title Resistivity saturation in semi-conducting polyacetylene molecular wires DOI 10.21203/rs.3.rs-2561893/v1 Type Preprint Author Tomczak J -
2021
Title Anisotropy of electronic correlations: On the applicability of local theories to layered materials DOI 10.1103/physrevb.103.045121 Type Journal Article Author Klebel-Knobloch B Journal Physical Review B Pages 045121 Link Publication -
2021
Title Toward Functionalized Ultrathin Oxide Films: The Impact of Surface Apical Oxygen DOI 10.1002/aelm.202101006 Type Journal Article Author Gabel J Journal Advanced Electronic Materials Link Publication -
2021
Title Breaking of Thermopower–Conductivity Trade-Off in LaTiO3 Film around Mott Insulator to Metal Transition DOI 10.1002/advs.202102097 Type Journal Article Author Katase T Journal Advanced Science Pages 2102097 Link Publication -
2021
Title Resistivity saturation in Kondo insulators DOI 10.1038/s42005-021-00723-z Type Journal Article Author Pickem M Journal Communications Physics Pages 226 Link Publication -
2021
Title Large phonon drag thermopower boosted by massive electrons and phonon leaking in LaAlO3/LaNiO3/LaAlO3 heterostructure DOI 10.1021/acs.nanolett.1c03143 Type Journal Article Author Kimura M Journal Nano Letters Pages 9240-9246 Link Publication -
2021
Title Designing a mechanically driven spin-crossover molecular switch via organic embedding DOI 10.48550/arxiv.2105.08699 Type Other Author Bhandary S -
2021
Title Prototypical many-body signatures in transport properties of semiconductors DOI 10.48550/arxiv.2112.07604 Type Other Author Maggio E -
2021
Title Designing a mechanically driven spin-crossover molecular switch via organic embedding DOI 10.1039/d1na00407g Type Journal Article Author Bhandary S Journal Nanoscale Advances Pages 4990-4995 Link Publication -
2021
Title Zoology of spin and orbital fluctuations in ultrathin oxide films DOI 10.1103/physrevb.104.024307 Type Journal Article Author Pickem M Journal Physical Review B Pages 024307 Link Publication -
2020
Title Kondo screening in Co adatoms with full Coulomb interaction DOI 10.1103/physrevresearch.2.033432 Type Journal Article Author Valli A Journal Physical Review Research Pages 033432 Link Publication -
2018
Title Thermoelectricity in correlated narrow-gap semiconductors DOI 10.48550/arxiv.1802.07220 Type Other Author Tomczak J -
2020
Title Isoelectronic tuning of heavy fermion systems: Proposal to synthesize Ce3Sb4Pd3 DOI 10.1103/physrevb.101.035116 Type Journal Article Author Tomczak J Journal Physical Review B Pages 035116 Link Publication -
2018
Title Thermoelectricity in correlated narrow-gap semiconductors DOI 10.1088/1361-648x/aab284 Type Journal Article Author Tomczak J Journal Journal of Physics: Condensed Matter Pages 183001 Link Publication -
2020
Title Coulomb Engineering of two-dimensional Mott materials DOI 10.48550/arxiv.2001.01735 Type Other Author Schüler M
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2020
Link
Title Resistivity Saturation in Kondo Insulators DOI 10.5281/zenodo.4355597 Type Database/Collection of data Public Access Link Link
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2020
Title Project BandITT (PI Emanuele Maggio, co-PI Jan Tomczak) Type Research grant (including intramural programme) Start of Funding 2020 Funder Austrian Science Fund (FWF)