Nanoscale material design for photovoltaic applications

Hua Bao, Purdue University

Abstract

Solar cell technology directly converts the clean, abundant energy of the sun into electricity. To build solar cell modules with low cost and high energy conversion efficiency, nanomaterials such as nanowires, nanotubes and quantum dots are very promising candidates, due to their novel thermal, electrical, and optical properties. This research seeks to use silicon nanowire, carbon nanotube, and semiconductor quantum dot to achieve high optical absorption and low electron-phonon coupling. Multiscale simulation and experiments are combined to investigate the thermal radiative properties of nanowire/nanotube array structures and the electron-phonon interaction in semiconductor quantum dots. Optical properties of nanowire/nanotube structures are numerically investigated by combined ab initio calculation and computational electromagnetic calculations. At the atomic scale, ab initio calculations based on density functional theory are performed to evaluate the spectral dielectric function of the material using the initial atomic structure as the only input parameter. This method considers different absorption mechanisms from far infrared to visible spectrum, and its effectiveness is demonstrated using the material GaAs and small carbon nanotubes. At the nanoscale, the predicted dielectric function of nanowire/nanotube is used as an input parameter in finite-difference time-domain method, so that the optical properties of devices such as nanowire/nanotube arrays can be obtained. Based on this scheme, we have shown that the vertically aligned multiwalled carbon nanotube arrays are nearly perfect absorber in the visible spectrum. Silicon nanowire arrays are less absorptive than carbon nanotube, but we propose and demonstrate that their optical absorption can be greatly enhanced by introducing structural randomness, including random positioning, diameter and length. The enhanced optical absorption implies potential enhancement of the overall efficiency of nanotube/nanowire array solar cells. Phonon-assisted electron decay in semiconductor quantum dots is also investigated in this work. In semiconductor solar cell, a large portion of energy loss is by the fast hot electron cooling, in which a high energy electron decays to the electronic band gap by creating a series of phonons. The excessive electrical energy is then converted to heat and wasted, so that the total photovoltaic energy conversion efficiency is limited. The electron decay rate reduces in semiconductor quantum dots, due to the discrete electron energy levels created by quantum confinement. To design quantum dots with the slowest decay rate, we use the non-adiabatic molecular dynamics to perform real-time simulations of the phonon-assisted electron decay process. This method is based on time-dependent density functional theory, and can directly predict the phonon-assisted electron decay time using the initial quantum dot structure as the only input. The numerical simulation shows that the phonon-induced electron decay can be slowed down in a small PbSe quantum dot. The temperature-dependent relaxation in this quantum dot is also studied, which helps us to propose a multi-channel relaxation mechanism. This mechanism provides new insights to the understanding of electron decay process in quantum dots. The results from this study have potentially important applications in solar energy harvesting and radiative thermal management. It offers a new perspective of nanoscale engineering of materials to achieve more efficient photovoltaic energy conversion.

Degree

Ph.D.

Advisors

Ruan, Purdue University.

Subject Area

Mechanical engineering|Nanotechnology|Optics|Materials science

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