Layer-resolved many-electron interactions in delafossite PdCoO2 from standing-wave photoemission spectroscopy

Lu, Qiyang; Martins, Henrique Perin; Kahk, Juhan Matthias; Rimal, Gaurab; Oh, Seongshik; Vishik, Inna; Brahlek, Matthew; Chueh, William C.; Lischner, Johannes; Nemšák, Slavomír

doi:10.1038/s42005-021-00643-y

Cited by 10 publications

(8 citation statements)

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“…Based on this observation, we have chosen to also use the calculated 4f spectral function to construct theoretical 3d and 4d spectra, using the same method as described above. We have recently used a similar approach for predicting core level line shapes in PdCoO 2 [42]. A detailed explanation along with the values used to construct these simulated core level spectra can be found in the Supplemental Material V (see, also, Refs.…”

Section: B G0w0 and Gw + Cmentioning

confidence: 99%

“…To date, no theoretical study of satellites in tungsten has been reported. Such a treatment requires the use of many-body perturbation theory (MBPT), which has already shown promise for the determination of plasmon satellites in sodium [35], aluminium [35,36], germanium [36], and silicon [37][38][39], but also heavier transition metal compounds [40][41][42].…”

Section: Introductionmentioning

confidence: 99%

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Lifetime effects and satellites in the photoelectron spectrum of tungsten metal

et al. 2022

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Tungsten (W) is an important and versatile transition metal and has a firm place at the heart of many technologies. A popular experimental technique for the characterization of tungsten and tungsten-based compounds is x-ray photoelectron spectroscopy (XPS), which enables the assessment of chemical states and electronic structure through the collection of core level and valence band spectra. However, in the case of tungsten metal, open questions remain regarding the origin, nature, and position of satellite features that are prominent in the photoelectron spectrum. These satellites are a fingerprint of the electronic structure of the material and have not been thoroughly investigated, at times leading to their misinterpretation. The present work combines high-resolution soft and hard x-ray photoelectron spectroscopy (SXPS and HAXPES) with reflected electron energy loss spectroscopy (REELS) and a multitiered ab initio theoretical approach, including density functional theory (DFT) and many-body perturbation theory (G0W0 and GW + C), to disentangle the complex set of experimentally observed satellite features attributed to the generation of plasmons and interband transitions. This combined experiment-theory strategy is able to uncover previously undocumented satellite features, improving our understanding of their direct relationship to tungsten's electronic structure. Furthermore, it lays the groundwork for future studies into tungsten-based mixed-metal systems and holds promise for the reassessment of the photoelectron spectra of other transition and post-transition metals, where similar questions regarding satellite features remain.

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Section: B G0w0 and Gw + Cmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

Lifetime effects and satellites in the photoelectron spectrum of tungsten metal

et al. 2022

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“…This compound possesses the largest mean free path for oxides at low temperature, l ∼ 20 µm [4], which is an extremely large value even as compared to the noble metals. Signatures of a hydrodynamic response [6][7][8] and recent work studying phenomena originating from the hexagonal Fermi surface [9] and the quasi-2D nature of the conductivity has stimulated the growing interest in this compound [10][11][12].…”

Section: Introductionmentioning

confidence: 99%

“…The role of disorder in modifying the nature of transport in metallic systems can be used to determine both the origin of scattering in the clean limit as well as play a role in enhancing existing interactions [31]. The tunability of thin films also provides an opportunity to determine if features found in bulk PdCoO 2 samples including inter-layer effects, long in-plane coherent lengths and an incommensurate CDW would be robust for use in thin film devices or heterostructures [12,32,33].…”

Section: Introductionmentioning

confidence: 99%

Disorder-enhanced effective masses and deviations from Matthiessen's rule in PdCoO$_2$ thin films

Barbalas,

Legros,

Rimal

et al. 2022

Preprint

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The observation of hydrodynamic transport in the metallic delafossite PdCoO2 has increased interest in this family of highly conductive oxides, but experimental studies so far have mostly been confined to bulk crystals. In this work, the development of high-quality thin films of PdCoO2 has enabled a thorough study of the conductivity as a function of film thickness using both dc transport and time-domain THz spectroscopy. With increasing film thickness from 12 nm to 102 nm, the residual resistivity decreases and we observe a large deviation from Matthiessen's rule (DMR) in the temperature dependence of the resistivity. We find that the complex THz conductivity is well fit by a single Drude term. We fit the data to extract the spectral weight and scattering rate simultaneously. The temperature dependence of the Drude scattering rate is found to be nearly independent of the residual resistivity and cannot be the primary mechanism for the observed DMR. Rather, we observe large changes in the spectral weight as a function of disorder, changing by a factor of 1.5 from the most disordered to least disordered films. We believe this corresponds to a mass enhancement of ≥ 2 times the value of the bulk effective mass which increases with residual disorder. This suggests that the mechanism behind the DMR observed in dc resistivity is primarily driven by changes in the electron mass. We discuss the possible origins of this behavior including the possibility of disorder-enhanced electron-phonon scattering, which can be systematically tuned by film thickness.

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“…1-4 and others. Myself, I have recently used the GW + cumulant approach that is already quite well established for predicting satellite structures in core and valence level photoelectron spectra of the layered oxide PdCoO 2 and W metal. 5,6 Johannes Lischner commented: The conference organizers have placed talks containing theoretical work into the "Future Directions" session indicating that a closer coupling of theory and experiments is an important step for the interpretation of future photoelectron spectroscopy experiments. In your opinion, what needs to be done to accelerate this process and ensure closer collaborations between theorists and experimentalists?…”

Section: àmentioning

confidence: 99%

Future directions: general discussion

Arrigo¹,

Ban²,

Bartels-Rausch³

et al. 2022

Faraday Discuss.

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Anders Nilsson opened a discussion of the paper by Giulia Galli: When we are comparing the electronic structure of water at ambient conditions with high pressure conditions there can be other changes than only the formation of different species. The basic structure can change quite a bit so that high density becomes more dominating. Can this aspect be part of understanding the electronic structure change?Giulia Galli responded: To really reply to this question we should have simulations (which we do not have yet) as a function of pressure and really have trends as a function of pressure. Hopefully we will have those in the next few months but they are not yet available to us.Anders Nilsson said: There is a shi in the 3a 1 towards the 1b 1 orbital peak when pressure is applied. Could this be the result of forming a disordered bandlike structure in a condensed phase and could there be an increased overlap between orbitals of neighboring molecules with increasing pressure? Giulia Galli replied: Yes indeed, I think this is what we are observing in our simulations. We are now examining other conditions and trying to gure out how this overlap depends on pressure in more detail.Loren Ban commented: Thank you for this nice presentation and the great work, I believe that calculated binding energy spectra of liquids are an important ingredient for further progress in understanding condensed phase electronic structure. These calculations will denitely be very valuable to experimentalists looking at similar systems.You show in Fig. 3 of the paper (https://doi.org/10.1039/d2fd00003b) that the binding energy spectrum of water at HPT is notably different from that at APT both in terms of peak widths and peak positions. For the latter, you nd an overall redshi of the HPT spectra. You also show that ionization energies of 412

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Layer-resolved many-electron interactions in delafossite PdCoO2 from standing-wave photoemission spectroscopy

Cited by 10 publications

References 53 publications

Lifetime effects and satellites in the photoelectron spectrum of tungsten metal

Lifetime effects and satellites in the photoelectron spectrum of tungsten metal

Disorder-enhanced effective masses and deviations from Matthiessen's rule in PdCoO$_2$ thin films

Future directions: general discussion

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