Nonequivalent Atomic Vibrations at Interfaces in a Polar Superlattice

Hoglund, Eric R.; Walker, Harrison A.; Hussain, Kamal; Bao, De‐Liang; Ni, Haoyang; Mamun, Abdullah; Baxter, Jefferey; Caldwell, Joshua D.; Khan, Asif; Pantelides, Sokrates T.; Hopkins, Patrick E.; Hachtel, Jordan A.

doi:10.1002/adma.202402925

Title: Nonequivalent Atomic Vibrations at Interfaces in a Polar Superlattice

Journal Article · 07 May 2024 · Advanced Materials

DOI: https://doi.org/10.1002/adma.202402925 · OSTI ID:2345724

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Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States); University of Virginia, Charlottesville, VA (United States); Vanderbilt University
Vanderbilt University, Nashville, TN (United States)
University of South Carolina, Columbia, SC (United States)
University of Illinois at Urbana‐Champaign, IL (United States)
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)
University of Virginia, Charlottesville, VA (United States)

In heterostructures made from polar materials, e.g., AlN–GaN–AlN, the nonequivalence of the two interfaces is long recognized as a critical aspect of their electronic properties; in that, they host different 2D carrier gases. Interfaces play an important role in the vibrational properties of materials, where interface states enhance thermal conductivity and can generate unique infrared-optical activity. The nonequivalence of the corresponding interface atomic vibrations, however, is not investigated so far due to a lack of experimental techniques with both high spatial and high spectral resolution. Herein, the nonequivalence of AlN–(Al_0.65Ga_0.35)N and (Al_0.65Ga_0.35)N–AlN interface vibrations is experimentally demonstrated using monochromated electron energy-loss spectroscopy in the scanning transmission electron microscope (STEM-EELS) and density-functional-theory (DFT) calculations are employed to gain insights in the physical origins of observations. It is demonstrated that STEM-EELS possesses sensitivity to the displacement vector of the vibrational modes as well as the frequency, which is as critical to understanding vibrations as polarization in optical spectroscopies. The combination enables direct mapping of the nonequivalent interface phonons between materials with different phonon polarizations. Furthermore, the results demonstrate the capacity to carefully assess the vibrational properties of complex heterostructures where interface states dominate the functional properties.

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Research Organization:: Vanderbilt University, Nashville, TN (United States)

Sponsoring Organization:: USDOE; USDOE Office of Science (SC), Basic Energy Sciences (BES). Materials Sciences & Engineering Division (MSE)

Grant/Contract Number:: AC02-05CH11231; AC05-00OR22725; FG02-09ER46554

OSTI ID:: 2345724

Journal Information:: Advanced Materials, Journal Name: Advanced Materials Journal Issue: 33 Vol. 36; ISSN 0935-9648

Publisher:: WileyCopyright Statement

Country of Publication:: United States

Language:: English

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Title: Nonequivalent Atomic Vibrations at Interfaces in a Polar Superlattice

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