Physical Review B最新文献

{"title":"Topological invariants of vortices, merons, skyrmions, and their combinations in continuous and discrete systems","authors":"Filipp N. Rybakov, Olle Eriksson, Nikolai S. Kiselev","doi":"10.1103/physrevb.111.134417","DOIUrl":"https://doi.org/10.1103/physrevb.111.134417","url":null,"abstract":"Magnetic vortices and skyrmions are typically characterized by distinct topological invariants. This paper presents a unified approach for the topological classification of these textures, encompassing isolated objects and configurations where skyrmions and vortices coexist. Using homotopy group analysis, we derive topological invariants that form the free Abelian group, Z</a:mi>×</a:mo>Z</a:mi></a:mrow></a:math>. We provide an explicit method for calculating the corresponding integer indices in continuous and discrete systems. This unified classification framework extends beyond magnetism and is applicable to physical systems in general. <jats:supplementary-material> <jats:copyright-statement>Published by the American Physical Society</jats:copyright-statement> <jats:copyright-year>2025</jats:copyright-year> </jats:permissions> </jats:supplementary-material>","PeriodicalId":20082,"journal":{"name":"Physical Review B","volume":"35 1","pages":""},"PeriodicalIF":3.7,"publicationDate":"2025-04-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143822816","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"物理与天体物理","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Evidence for reduced periodic lattice distortion within the Sb-terminated surface layer of the kagome metal CsV3Sb5","authors":"Felix Kurtz, Gevin von Witte, Lukas Jehn, Alp Akbiyik, Igor Vinograd, Matthieu Le Tacon, Amir A. Haghighirad, Dong Chen, Chandra Shekhar, Claudia Felser, Claus Ropers","doi":"10.1103/physrevb.111.l140101","DOIUrl":"https://doi.org/10.1103/physrevb.111.l140101","url":null,"abstract":"The discovery of the kagome metal CsV</a:mi></a:mrow>3</a:mn></a:msub>Sb</a:mi></a:mrow>5</a:mn></a:msub></a:math> sparked broad interest, due to the coexistence of a charge density wave (CDW) phase and possible unconventional superconductivity in the material. In this Letter, we use low-energy electron diffraction (LEED) with a <b:math xmlns:b=\"http://www.w3.org/1998/Math/MathML\"><b:mi>µ</b:mi><b:mi mathvariant=\"normal\">m</b:mi></b:math>-sized electron beam to explore the periodic lattice distortion at the antimony-terminated surface in the CDW phase. We recorded high-quality backscattering diffraction patterns in ultrahigh vacuum from multiple cleaved samples. Unexpectedly, we did not find superstructure reflexes at intensity levels predicted from dynamical LEED calculations for the reported <d:math xmlns:d=\"http://www.w3.org/1998/Math/MathML\"><d:mrow><d:mn>2</d:mn><d:mo>×</d:mo><d:mn>2</d:mn><d:mo>×</d:mo><d:mn>2</d:mn></d:mrow></d:math> bulk structure. Our results suggest that in <e:math xmlns:e=\"http://www.w3.org/1998/Math/MathML\"><e:msub><e:mrow><e:mi>CsV</e:mi></e:mrow><e:mn>3</e:mn></e:msub><e:msub><e:mrow><e:mi>Sb</e:mi></e:mrow><e:mn>5</e:mn></e:msub></e:math> the periodic lattice distortion accompanying the CDW is less pronounced at Sb-terminated surfaces than in the bulk. <jats:supplementary-material> <jats:copyright-statement>Published by the American Physical Society</jats:copyright-statement> <jats:copyright-year>2025</jats:copyright-year> </jats:permissions> </jats:supplementary-material>","PeriodicalId":20082,"journal":{"name":"Physical Review B","volume":"39 1","pages":""},"PeriodicalIF":3.7,"publicationDate":"2025-04-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143813463","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"物理与天体物理","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Antichiral surface states and Su-Schrieffer-Heeger physics in rutile altermagnets","authors":"Sopheak Sorn","doi":"10.1103/physrevb.111.l161109","DOIUrl":"https://doi.org/10.1103/physrevb.111.l161109","url":null,"abstract":"We study surface states and domain wall bound states in altermagnets using a rutile-lattice tight-binding model of electrons coupled to a Néel order. We discover that two symmetry-protected Weyl nodal lines in the bulk band structure can give rise to unconventional antichiral surface states—surface states from opposite surfaces propagate in a manner, as opposed to the antiparallel manner for the more conventional chiral surface states. We also find that the antichiral surface states can be turned into chiral surface states upon changing the surface termination. The origin of the surface states, the dependence on the surface termination, and key features of domain wall bound states are explained using a map from the altermagnet to a family of a modified Su-Schrieffer-Heeger chain and the associated bulk-boundary correspondence. Our work reveals rutile altermagnets as a promising candidate among very few quantum materials that can support antichiral surface states. <jats:supplementary-material> <jats:copyright-statement>Published by the American Physical Society</jats:copyright-statement> <jats:copyright-year>2025</jats:copyright-year> </jats:permissions> </jats:supplementary-material>","PeriodicalId":20082,"journal":{"name":"Physical Review B","volume":"39 1","pages":""},"PeriodicalIF":3.7,"publicationDate":"2025-04-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143813464","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"物理与天体物理","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Fragile spin liquid in three dimensions","authors":"Anna Fancelli, R. Flores-Calderón, Owen Benton, Bella Lake, Roderich Moessner, Johannes Reuther","doi":"10.1103/physrevb.111.134413","DOIUrl":"https://doi.org/10.1103/physrevb.111.134413","url":null,"abstract":"Motivated by the recent appearance of the trillium lattice in the search for materials hosting spin liquids, we study the ground state of the classical Heisenberg model on its line graph, the trilline lattice. We find that this network realizes the recently proposed notion of a fragile spin liquid in three dimensions. Additionally, we analyze the Ising case and argue for a possible Z</a:mi>2</a:mn></a:msub></a:math> quantum spin liquid phase in the corresponding quantum dimer model. Like the well-known <c:math xmlns:c=\"http://www.w3.org/1998/Math/MathML\"><c:mrow><c:mi>U</c:mi><c:mo>(</c:mo><c:mn>1</c:mn><c:mo>)</c:mo></c:mrow></c:math> spin liquids, the classical phase hosts moment fractionalization evidenced by the diluted lattice, but unlike those, it exhibits exponential decay in both spin correlations and interactions between fractionalized moments. This provides an instance of a purely short-range correlated classical Heisenberg spin liquid in three dimensions. <jats:supplementary-material> <jats:copyright-statement>Published by the American Physical Society</jats:copyright-statement> <jats:copyright-year>2025</jats:copyright-year> </jats:permissions> </jats:supplementary-material>","PeriodicalId":20082,"journal":{"name":"Physical Review B","volume":"91 1","pages":""},"PeriodicalIF":3.7,"publicationDate":"2025-04-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143813469","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"物理与天体物理","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Translation symmetry restoration under random unitary dynamics","authors":"Katja Klobas, Colin Rylands, Bruno Bertini","doi":"10.1103/physrevb.111.l140304","DOIUrl":"https://doi.org/10.1103/physrevb.111.l140304","url":null,"abstract":"The finite parts of a large, locally interacting many-body system prepared out of equilibrium eventually equilibrate. Characterizing the underlying mechanisms of this process and its timescales, however, is particularly hard as it requires one to decouple universal features from observable-specific ones. Recently, additional insight was gained by studying how certain symmetries of the dynamics that are broken by the initial state are restored at the level of the reduced state of a given subsystem. This provides a high-level, observable-independent probe. Until now, this idea has been applied to the restoration of internal symmetries, e.g., U(1) symmetries related to charge conservation. Here we show that the same logic can be applied to the restoration of space-time symmetries, and hence can be used to characterize the relaxation of fully generic systems. We illustrate this idea by considering the paradigmatic example of “generic” many-body dynamics, i.e., a local random unitary circuit, where our method leads to exact results. We show that the restoration of translation symmetry in these systems only happens on timescales that are proportional to the subsystem's volume. In fact, for large enough subsystems, the time of symmetry restoration becomes initial-state independent (as long as the latter breaks the symmetry at time zero) and coincides with the thermalization time. For intermediate subsystems, however, one can observe the “quantum Mpemba effect,” where the state of the system restores a symmetry faster if it is initially more asymmetric. We provide an exact characterization of this effect in a nonintegrable system. <jats:supplementary-material> <jats:copyright-statement>Published by the American Physical Society</jats:copyright-statement> <jats:copyright-year>2025</jats:copyright-year> </jats:permissions> </jats:supplementary-material>","PeriodicalId":20082,"journal":{"name":"Physical Review B","volume":"49 1","pages":""},"PeriodicalIF":3.7,"publicationDate":"2025-04-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143805565","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"物理与天体物理","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Enhanced quantum sensitivity and coherence of symmetric magnetic clusters","authors":"Lorenzo Amato, Manuel Grimm, Markus Müller","doi":"10.1103/physrevb.111.134406","DOIUrl":"https://doi.org/10.1103/physrevb.111.134406","url":null,"abstract":"Searching for highly coherent degrees of freedom in noisy solid-state environments is a major challenge in condensed matter. In disordered dipolar systems, such as magnetically doped insulators, compact clusters of two-level systems (TLS) have recently been shown to have significantly longer coherence times than typical single TLS. Coupling weakly to their environment, they sense and probe its many-body dynamics through the induced dephasing. However, it has remained an open question whether further mechanisms exist that protect the coherence of such solid-state qubits. Here, we show that symmetric clusters of a few TLS couple even more weakly to their surroundings, making them highly sensitive quantum sensors of slow many-body dynamics. Furthermore, we explore their use as qubits for quantum information storage, detailing the techniques required for their preparation and manipulation. Our findings elucidate the role of symmetry in enhancing quantum coherence in disordered and noisy systems, opening a route toward a sensitive experimental probe of many-body quasilocalization dynamics as well as the development of quantum technologies in solid-state systems. <jats:supplementary-material> <jats:copyright-statement>Published by the American Physical Society</jats:copyright-statement> <jats:copyright-year>2025</jats:copyright-year> </jats:permissions> </jats:supplementary-material>","PeriodicalId":20082,"journal":{"name":"Physical Review B","volume":"90 1","pages":""},"PeriodicalIF":3.7,"publicationDate":"2025-04-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143782859","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"物理与天体物理","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Electronic structure of Bi2Ir2O7 probed by resonant inelastic x-ray scattering at the oxygen K edge: Metallicity, hybridization, and electronic correlations","authors":"P. Olalde-Velasco, Y. Huang, J. Pelliciari, J. Miyawaki, A. Uldry, D. Prabhakaran, B. Delley, Y. Harada, A. T. Boothroyd, H. M. Rønnow, D. F. McMorrow, T. Schmitt","doi":"10.1103/physrevb.111.155106","DOIUrl":"https://doi.org/10.1103/physrevb.111.155106","url":null,"abstract":"The electronic structure of metallic Bi&lt;/a:mi&gt;2&lt;/a:mn&gt;&lt;/a:msub&gt;Ir&lt;/a:mi&gt;2&lt;/a:mn&gt;&lt;/a:msub&gt;O&lt;/a:mi&gt;7&lt;/a:mn&gt;&lt;/a:msub&gt;&lt;/a:mrow&gt;&lt;/a:math&gt; has been investigated by a combination of soft x-ray absorption spectroscopy, x-ray emission spectroscopy (XES), and resonant inelastic x-ray scattering (RIXS) in the vicinity of the oxygen &lt;e:math xmlns:e=\"http://www.w3.org/1998/Math/MathML\"&gt;&lt;e:mrow&gt;&lt;e:mi&gt;K&lt;/e:mi&gt;&lt;/e:mrow&gt;&lt;/e:math&gt; edge. The O &lt;f:math xmlns:f=\"http://www.w3.org/1998/Math/MathML\"&gt;&lt;f:mrow&gt;&lt;f:mi&gt;K&lt;/f:mi&gt;&lt;/f:mrow&gt;&lt;/f:math&gt;-edge RIXS spectra are found to resemble the O &lt;g:math xmlns:g=\"http://www.w3.org/1998/Math/MathML\"&gt;&lt;g:mrow&gt;&lt;g:mi&gt;K&lt;/g:mi&gt;&lt;/g:mrow&gt;&lt;/g:math&gt;-edge XES spectra with resonating features but with an absence of any Raman modes, revealing the highly itinerant nature of this compound. The O &lt;h:math xmlns:h=\"http://www.w3.org/1998/Math/MathML\"&gt;&lt;h:mrow&gt;&lt;h:mi&gt;K&lt;/h:mi&gt;&lt;/h:mrow&gt;&lt;/h:math&gt;-edge response is compared with scalar relativistic band structure calculations within the local density approximation, which captures the main spectral characteristics. The RIXS spectra either display a localized or delocalized Ir &lt;i:math xmlns:i=\"http://www.w3.org/1998/Math/MathML\"&gt;&lt;i:mrow&gt;&lt;i:mn&gt;5&lt;/i:mn&gt;&lt;i:mi&gt;d&lt;/i:mi&gt;&lt;/i:mrow&gt;&lt;/i:math&gt; response, depending on whether the photon energy is tuned to the pre-edge or above. Our results uncover a significant coupling of O &lt;j:math xmlns:j=\"http://www.w3.org/1998/Math/MathML\"&gt;&lt;j:mrow&gt;&lt;j:mi&gt;K&lt;/j:mi&gt;&lt;/j:mrow&gt;&lt;/j:math&gt;-edge RIXS via the O &lt;k:math xmlns:k=\"http://www.w3.org/1998/Math/MathML\"&gt;&lt;k:mrow&gt;&lt;k:mn&gt;2&lt;/k:mn&gt;&lt;k:mi&gt;p&lt;/k:mi&gt;&lt;k:mo&gt;−&lt;/k:mo&gt;&lt;k:mi&gt;Ir&lt;/k:mi&gt;&lt;/k:mrow&gt;&lt;k:mo&gt; &lt;/k:mo&gt;&lt;k:mrow&gt;&lt;k:mn&gt;5&lt;/k:mn&gt;&lt;k:mi&gt;d&lt;/k:mi&gt;&lt;/k:mrow&gt;&lt;/k:math&gt; hybridization to the partial density of states of the Ir &lt;l:math xmlns:l=\"http://www.w3.org/1998/Math/MathML\"&gt;&lt;l:mrow&gt;&lt;l:mn&gt;5&lt;/l:mn&gt;&lt;l:mi&gt;d&lt;/l:mi&gt;&lt;/l:mrow&gt;&lt;/l:math&gt; states. An alternative explanation of the Ir &lt;m:math xmlns:m=\"http://www.w3.org/1998/Math/MathML\"&gt;&lt;m:mrow&gt;&lt;m:mn&gt;5&lt;/m:mn&gt;&lt;m:mi&gt;d&lt;/m:mi&gt;&lt;m:mo&gt;−&lt;/m:mo&gt;&lt;m:mi mathvariant=\"normal\"&gt;O&lt;/m:mi&gt;&lt;/m:mrow&gt;&lt;m:mo&gt; &lt;/m:mo&gt;&lt;m:mrow&gt;&lt;m:mn&gt;2&lt;/m:mn&gt;&lt;m:mi&gt;p&lt;/m:mi&gt;&lt;/m:mrow&gt;&lt;/m:math&gt; hybridization spectral structure in the optical region of the RIXS spectra is given in terms of Ir &lt;o:math xmlns:o=\"http://www.w3.org/1998/Math/MathML\"&gt;&lt;o:mrow&gt;&lt;o:mi&gt;d&lt;/o:mi&gt;&lt;o:mi&gt;d&lt;/o:mi&gt;&lt;/o:mrow&gt;&lt;/o:math&gt; excitations. Our findings allow us to infer that the relative electronic correlations in the metallic &lt;p:math xmlns:p=\"http://www.w3.org/1998/Math/MathML\"&gt;&lt;p:mrow&gt;&lt;p:msub&gt;&lt;p:mi mathvariant=\"normal\"&gt;Bi&lt;/p:mi&gt;&lt;p:mn&gt;2&lt;/p:mn&gt;&lt;/p:msub&gt;&lt;p:msub&gt;&lt;p:mi mathvariant=\"normal\"&gt;Ir&lt;/p:mi&gt;&lt;p:mn&gt;2&lt;/p:mn&gt;&lt;/p:msub&gt;&lt;p:msub&gt;&lt;p:mi mathvariant=\"normal\"&gt;O&lt;/p:mi&gt;&lt;p:mn&gt;7&lt;/p:mn&gt;&lt;/p:msub&gt;&lt;/p:mrow&gt;&lt;/p:math&gt; compound with sizable spin-orbit coupling are &lt;t:math xmlns:t=\"http://www.w3.org/1998/Math/MathML\"&gt;&lt;t:mrow&gt;&lt;t:mn&gt;0.06&lt;/t:mn&gt;&lt;t:mo&gt;≤&lt;/t:mo&gt;&lt;t:mi&gt;U&lt;/t:mi&gt;&lt;/t:mrow&gt;&lt;t:mo&gt;/&lt;/t:mo&gt;&lt;t:mrow&gt;&lt;t:mi&gt;W&lt;/t:mi&gt;&lt;t:mo&gt;≤&lt;/t:mo&gt;&lt;t:mn&gt;0.22&lt;/t:mn&gt;&lt;/t:mrow&gt;&lt;/t:math&gt; and thus are in the moderate-to-weak regime. We found th","PeriodicalId":20082,"journal":{"name":"Physical Review B","volume":"59 1","pages":""},"PeriodicalIF":3.7,"publicationDate":"2025-04-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143775328","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"物理与天体物理","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Variable-temperature and carrier-resolved photo-Hall measurements of high-performance selenium thin-film solar cells","authors":"Rasmus S. Nielsen, Oki Gunawan, Teodor Todorov, Clara B. Møller, Ole Hansen, Peter C. K. Vesborg","doi":"10.1103/physrevb.111.165202","DOIUrl":"https://doi.org/10.1103/physrevb.111.165202","url":null,"abstract":"Selenium is an elemental semiconductor with a wide band gap suitable for a range of optoelectronic and solar energy conversion technologies. However, developing such applications requires an in-depth understanding of the fundamental material properties. Here, we study the properties of the majority and minority charge carriers in selenium using a recently developed carrier-resolved photo-Hall technique, which enables simultaneous mapping of the mobilities and concentrations of both carriers under varying light intensities. Additionally, we perform temperature-dependent Hall measurements to extract information about the acceptor level and ionization efficiency. Our findings are compared to results from other advanced characterization techniques, and the inconsistencies are outlined. Finally, we characterize a high-performance selenium thin-film solar cell, and we perform device simulations to systematically address each discrepancy and accurately reproduce experimental current-voltage and external quantum efficiency measurements. These results contribute to a deeper understanding of the optoelectronic properties and carrier dynamics in selenium, which may guide future improvements and facilitate the development of higher-efficiency selenium solar cells. <jats:supplementary-material> <jats:copyright-statement>Published by the American Physical Society</jats:copyright-statement> <jats:copyright-year>2025</jats:copyright-year> </jats:permissions> </jats:supplementary-material>","PeriodicalId":20082,"journal":{"name":"Physical Review B","volume":"1 1","pages":""},"PeriodicalIF":3.7,"publicationDate":"2025-04-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143775364","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"物理与天体物理","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Numerical calculation of the Hopf index for three-dimensional magnetic textures","authors":"R. Knapman, M. Azhar, A. Pignedoli, L. Gallard, R. Hertel, J. Leliaert, K. Everschor-Sitte","doi":"10.1103/physrevb.111.134408","DOIUrl":"https://doi.org/10.1103/physrevb.111.134408","url":null,"abstract":"To gain deeper insight into the complex, stable, and robust configurations of magnetic textures, topological characterization has proven essential. In particular, while the skyrmion number is a well-established topological invariant for two-dimensional magnetic textures, the Hopf index serves as a key topological descriptor for three-dimensional magnetic structures. In this paper, we present and compare various methods for numerically calculating the Hopf index, provide implementations, and offer a detailed analysis of their accuracy and computational efficiency. Additionally, we identify and address common pitfalls and challenges associated with the numerical computation of the Hopf index, offering insights for improving the robustness of these techniques. <jats:supplementary-material> <jats:copyright-statement>Published by the American Physical Society</jats:copyright-statement> <jats:copyright-year>2025</jats:copyright-year> </jats:permissions> </jats:supplementary-material>","PeriodicalId":20082,"journal":{"name":"Physical Review B","volume":"73 1","pages":""},"PeriodicalIF":3.7,"publicationDate":"2025-04-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143782858","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"物理与天体物理","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Tomographic identification of all molecular orbitals in a wide binding-energy range","authors":"Anja Haags, Dominik Brandstetter, Xiaosheng Yang, Larissa Egger, Hans Kirschner, Alexander Gottwald, Mathias Richter, Georg Koller, François C. Bocquet, Christian Wagner, Michael G. Ramsey, Serguei Soubatch, Peter Puschnig, F. Stefan Tautz","doi":"10.1103/physrevb.111.165402","DOIUrl":"https://doi.org/10.1103/physrevb.111.165402","url":null,"abstract":"In the past decade, photoemission orbital tomography (POT) has evolved into a powerful tool to investigate the electronic structure of organic molecules adsorbed on surfaces. Here we show that POT allows for the comprehensive experimental identification of all molecular orbitals in a substantial binding energy range of more than 10 eV. Making use of the angular distribution of photoelectrons as a function of binding-energy, we exemplify this by extracting an orbital-resolved projected density of states for 15 π</a:mi></a:math> and 23 <b:math xmlns:b=\"http://www.w3.org/1998/Math/MathML\"><b:mi>σ</b:mi></b:math> orbitals from the experimental data of the prototypical organic molecule bisanthene (<c:math xmlns:c=\"http://www.w3.org/1998/Math/MathML\"><c:mrow><c:msub><c:mi mathvariant=\"normal\">C</c:mi><c:mn>28</c:mn></c:msub><c:msub><c:mi mathvariant=\"normal\">H</c:mi><c:mn>14</c:mn></c:msub></c:mrow></c:math>) on a Cu(110) surface. These experimental results for an essentially complete set of orbitals within the given binding-energy range serve as stringent benchmarks for electronic structure methods, which we illustrate by performing density functional calculations employing four frequently used exchange-correlation functionals. By computing the respective molecular-orbital-projected densities of states, a one-to-one comparison with experimental data for an unprecedented number of 38 orbital energies became possible. The quantitative analysis of our data reveals that the range-separated hybrid functional HSE performs best for the investigated organic/metal interface. At a more fundamental level, the remarkable agreement between the experimental and the Kohn-Sham orbital energies over a binding-energy range larger than 10 eV suggests that—perhaps unexpectedly—Kohn-Sham orbitals approximate Dyson orbitals, which would rigorously account for the electron extraction process in photoemission spectroscopy but are notoriously difficult to compute, in a much better way than previously thought. <jats:supplementary-material> <jats:copyright-statement>Published by the American Physical Society</jats:copyright-statement> <jats:copyright-year>2025</jats:copyright-year> </jats:permissions> </jats:supplementary-material>","PeriodicalId":20082,"journal":{"name":"Physical Review B","volume":"18 1","pages":""},"PeriodicalIF":3.7,"publicationDate":"2025-04-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143766334","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"物理与天体物理","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}