Electronic and vibrational properties of atomically-thin black phosphorus and its nanostructures from first-principles

Cupo, Andrew
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Meunier, Vincent
Terrones, H. (Humberto)
Zhang, Shengbai
Huang, Liping
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This new method is poised to bridge the gap between experiment and theory for many atomically-thin materials supported by substrates of different compositions and orientations. By using ab initio molecular dynamics in combination with the velocity autocorrelation spectral method as well as many-body perturbation theory, we were also able to predict the temperature dependent anharmonicity-induced phonon normal mode frequency shifts and lifetimes for single-layer BP. The lifetimes are a key part in calculating the thermal conductivity, which plays an important role in thermoelectric devices. In realizing that this spectral method is incredibly computationally expensive, we derived lineshapes including the simulation time in addition to the frequency shift and lifetime, and showed that the new formalism can be used to obtained converged temperature dependent phonon properties up to around an order of magnitude faster. This new method could be implemented in computational materials discovery packages to accurately predict what classes of materials would function as optimal thermoelectric materials. Overall, the wide range of new results in this thesis provides motivation to pursue applications in nanoelectronics, optoelectronics, and thermoelectric materials.
May 2019
School of Science
Dept. of Physics, Applied Physics, and Astronomy
Rensselaer Polytechnic Institute, Troy, NY
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