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Title: Quasiperiodic ordering in thick Sn layer on i -Al-Pd-Mn: A possible quasicrystalline clathrate

Abstract

Realization of an elemental solid-state quasicrystal has remained a distant dream so far in spite of extensive work in this direction for almost two decades. In the present work, we report the discovery of quasiperiodic ordering in a thick layer of elemental Sn grown on icosahedral ( i ) -Al-Pd-Mn. The scanning tunneling microscopy (STM) images and the low-energy electron diffraction patterns of the Sn layer show specific structural signatures that portray quasiperiodicity but are distinct from the substrate. Photoemission spectroscopy reveals the existence of the pseudogap around the Fermi energy up to the maximal Sn thickness. The structure of the Sn layer is modeled as a form of quasicrystalline clathrate on the basis of multiple supporting evidences: First, from ab initio total energy evaluation, the energy of bulk Sn clathrate quasicrystal is lower than the high-temperature metallic β -Sn phase, but higher than the low-temperature α -Sn phase. A comparative study of the free slab energetics shows that surface energy favors clathrate over α -Sn up to about 4-nm layer thickness and matches β -Sn for narrow window of slab thickness of 2–3 nm. Second, the bulk clathrate exhibits gap opening near Fermi energy, while the free slab formmore » exhibits a pronounced pseudogap, which explains the pseudogap observed in photoemission. Third, the STM images exhibit good agreement with clathrate model. Finally, we establish the adlayer-substrate compatibility based on very similar (within 1%) the cage-cage separation in the Sn clathrate and the pseudo-Mackay cluster-cluster separation on the i -Al-Pd-Mn surface. Furthermore, the nucleation centers of the Sn adlayer on the substrate are identified and these are shown to be a valid part of the Sn clathrate structure. Thus, based on both experimental and ab initio density functional theory calculations, we propose that 4-nm-thick Sn adlayer deposited on fivefold surface of i -Al-Pd-Mn substrate is in fact a metastable realization of elemental, clathrate family quasicrystal.« less

Authors:
; ; ; ; ; ; ; ; ; ; ;
Publication Date:
Research Org.:
Ames Lab., Ames, IA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1581677
Alternate Identifier(s):
OSTI ID: 1593148
Report Number(s):
IS-J-10136
Journal ID: ISSN 2643-1564; PPRHAI; 013023
Grant/Contract Number:  
AC02-07CH11358; 2/0082/17; 15-0621; 277829
Resource Type:
Published Article
Journal Name:
Physical Review Research
Additional Journal Information:
Journal Name: Physical Review Research Journal Volume: 2 Journal Issue: 1; Journal ID: ISSN 2643-1564
Publisher:
American Physical Society
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE

Citation Formats

Singh, Vipin Kumar, Mihalkovic, Marek, Krajčí, Marian, Sarkar, Shuvam, Sadhukhan, Pampa, Maniraj, M., Rai, Abhishek, Pussi, Katariina, Schlagel, Deborah L., Lograsso, Thomas A., Shukla, Ajay Kumar, and Barman, Sudipta Roy. Quasiperiodic ordering in thick Sn layer on i -Al-Pd-Mn: A possible quasicrystalline clathrate. United States: N. p., 2020. Web. doi:10.1103/PhysRevResearch.2.013023.
Singh, Vipin Kumar, Mihalkovic, Marek, Krajčí, Marian, Sarkar, Shuvam, Sadhukhan, Pampa, Maniraj, M., Rai, Abhishek, Pussi, Katariina, Schlagel, Deborah L., Lograsso, Thomas A., Shukla, Ajay Kumar, & Barman, Sudipta Roy. Quasiperiodic ordering in thick Sn layer on i -Al-Pd-Mn: A possible quasicrystalline clathrate. United States. doi:10.1103/PhysRevResearch.2.013023.
Singh, Vipin Kumar, Mihalkovic, Marek, Krajčí, Marian, Sarkar, Shuvam, Sadhukhan, Pampa, Maniraj, M., Rai, Abhishek, Pussi, Katariina, Schlagel, Deborah L., Lograsso, Thomas A., Shukla, Ajay Kumar, and Barman, Sudipta Roy. Wed . "Quasiperiodic ordering in thick Sn layer on i -Al-Pd-Mn: A possible quasicrystalline clathrate". United States. doi:10.1103/PhysRevResearch.2.013023.
@article{osti_1581677,
title = {Quasiperiodic ordering in thick Sn layer on i -Al-Pd-Mn: A possible quasicrystalline clathrate},
author = {Singh, Vipin Kumar and Mihalkovic, Marek and Krajčí, Marian and Sarkar, Shuvam and Sadhukhan, Pampa and Maniraj, M. and Rai, Abhishek and Pussi, Katariina and Schlagel, Deborah L. and Lograsso, Thomas A. and Shukla, Ajay Kumar and Barman, Sudipta Roy},
abstractNote = {Realization of an elemental solid-state quasicrystal has remained a distant dream so far in spite of extensive work in this direction for almost two decades. In the present work, we report the discovery of quasiperiodic ordering in a thick layer of elemental Sn grown on icosahedral ( i ) -Al-Pd-Mn. The scanning tunneling microscopy (STM) images and the low-energy electron diffraction patterns of the Sn layer show specific structural signatures that portray quasiperiodicity but are distinct from the substrate. Photoemission spectroscopy reveals the existence of the pseudogap around the Fermi energy up to the maximal Sn thickness. The structure of the Sn layer is modeled as a form of quasicrystalline clathrate on the basis of multiple supporting evidences: First, from ab initio total energy evaluation, the energy of bulk Sn clathrate quasicrystal is lower than the high-temperature metallic β -Sn phase, but higher than the low-temperature α -Sn phase. A comparative study of the free slab energetics shows that surface energy favors clathrate over α -Sn up to about 4-nm layer thickness and matches β -Sn for narrow window of slab thickness of 2–3 nm. Second, the bulk clathrate exhibits gap opening near Fermi energy, while the free slab form exhibits a pronounced pseudogap, which explains the pseudogap observed in photoemission. Third, the STM images exhibit good agreement with clathrate model. Finally, we establish the adlayer-substrate compatibility based on very similar (within 1%) the cage-cage separation in the Sn clathrate and the pseudo-Mackay cluster-cluster separation on the i -Al-Pd-Mn surface. Furthermore, the nucleation centers of the Sn adlayer on the substrate are identified and these are shown to be a valid part of the Sn clathrate structure. Thus, based on both experimental and ab initio density functional theory calculations, we propose that 4-nm-thick Sn adlayer deposited on fivefold surface of i -Al-Pd-Mn substrate is in fact a metastable realization of elemental, clathrate family quasicrystal.},
doi = {10.1103/PhysRevResearch.2.013023},
journal = {Physical Review Research},
number = 1,
volume = 2,
place = {United States},
year = {2020},
month = {1}
}

Journal Article:
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DOI: 10.1103/PhysRevResearch.2.013023

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