2021 Annual Meeting

(299e) High-Throughput Computational Analysis of the Role of Finite Temperature in the Optical Response of 2D Materials

Authors

Huang, T. A., Boston University
Clark, Q., Boston University
Sharifzadeh, S., Boston University
Stable two-dimensional materials are promising for nanoelectronic applications due to their relatively small form factor, and their great variety of chemical and optoelectronic properties [1]. This allows for the design of light-weight and low-cost materials for optoelectronic devices for applications such as single-electron transistors [2], solar cells [3], and lasers [4]. Here, we utilize first-principles density functional theory (DFT) to investigate the optoelectronic function of these monolayer materials, including the role of electron-phonon interactions.

DFT is the standard modeling methodology for studying the electronic properties of solid-state materials. However, the common T = 0K approximation may result in an erroneous understanding of the material properties [5]. This is especially the case for low-dimensional materials with low-screening that results in increased electron-phonon interactions [6]. We present a high-throughput DFT and beyond-DFT approach to study of the effect of finite temperature on the optical properties of 2D materials, incorporating the role of phonons through a semi-classical approach [7]. We show that the strength of electron-phonon interactions is highly dependent on the bond ionicity within the crystal. We show that this framework allows for a systematic theoretical exploration of new materials for solar energy conversion.

[1] Q. Ma, G. Ren, K. Xu, and J. Z. Ou, “Tunable Optical Properties of 2D Materials and Their Applications,” Advanced Optical Materials, vol. 9, no. 2, p. 2001313, 2021, doi: https://doi.org/10.1002/adom.202001313.

[2] M. Javaid, D. W. Drumm, S. P. Russo, and A. D. Greentree, “Surface-gate-defined single-electron transistor in a MoS 2 bilayer,” Nanotechnology, vol. 28, no. 12, p. 125203, Mar. 2017, doi: 10.1088/1361-6528/aa5ce0.

[3] A. Pospischil, M. M. Furchi, and T. Mueller, “Solar-energy conversion and light emission in an atomic monolayer p–n diode,” Nature Nanotech, vol. 9, no. 4, pp. 257–261, Apr. 2014, doi: 10.1038/nnano.2014.14.

[4] B. Zhang et al., “Recent Progress in 2D Material‐Based Saturable Absorbers for All Solid‐State Pulsed Bulk Lasers,” Laser & Photonics Reviews, vol. 14, no. 2, p. 1900240, Feb. 2020, doi: 10.1002/lpor.201900240.

[5] M. Zacharias, C. E. Patrick, and F. Giustino, “Stochastic Approach to Phonon-Assisted Optical Absorption,” Phys. Rev. Lett., vol. 115, no. 17, p. 177401, Oct. 2015, doi: 10.1103/PhysRevLett.115.177401.

[6] T. Sohier et al., “Enhanced Electron-Phonon Interaction in Multivalley Materials,” Phys. Rev. X, vol. 9, no. 3, p. 031019, Aug. 2019, doi: 10.1103/PhysRevX.9.031019.

[7] M. Zacharias and F. Giustino, “Theory of the special displacement method for electronic structure calculations at finite temperature,” Phys. Rev. Research, vol. 2, no. 1, p. 013357, Mar. 2020, doi: 10.1103/PhysRevResearch.2.013357.