Mesostructured Thin Film Solar Cells: Examining Hole Transfer Mechanisms and Device Stability

Doctoral Dissertation

Abstract

To meet their potential for abundant, cost-effective renewable energy production, photovoltaics must be developed which are simultaneously higher efficiency and lower cost. The rise of nanotechnology has enabled the design of new classes of solar cells, such as extremely thin absorber (ETA) and perovskite solar cells, which could ultimately meet this goal. This dissertation describes progress in the fundamental understanding of charge transfer processes in Sb2S3 ETA solar cells, and improving the stability of CH3NH3PbI3 perovskite solar cells.

ETA solar cells have the distinct advantage of very thin absorber layers which facilitate efficient charge extraction in materials with relatively low minority carrier diffusion lengths. Femtosecond transient absorption spectroscopy was employed to track minority carrier (hole) behavior in Sb2S3 ETA solar cells. Hole transfer out of Sb2S3 is found to be strongly dependent on Sb2S3 thickness, therefore we develop a model which allows for the comprehensive exploration of the mechanism of hole transfer and the elucidation of the rate limiting step. The broader implications of these results on photovoltaic performance are explored through measurements on TiO2/Sb2S3/CuSCN solar cells.

Solar cells employing the hybrid perovskite material CH3NH3PbI3 have recently risen to the forefront due to their unparalleled rise in power conversion efficiency. Nonetheless, the so-called perovskite solar cells have substantial hurdles to overcome on the road to commercialization. Two issues which have risen to the forefront are the cost and stability of the hole transport material (HTM) and the stability of CH3NH3PbI3 when exposed to moisture. We demonstrate that CuI, an inorganic HTM with dramatically lower cost than typical organic HTMs, shows promising stability, displays two orders of magnitude higher p-type conductivity, and reaches 75% of the performance of comparable devices featuring a typical organic HTM. Lastly, we systematically explore the degradation of CH3NH3PbI3 in the presence of atmospheric moisture. It is shown that H2O is able to complex with CH3NH3PbI3, forming a hydrate. We characterize the optical and structural changes associated with this transformation, and subsequently study the deleterious effects of moisture on photovoltaic performance in light on these spectroscopic understandings in order to elucidate the mechanism of degradation.

Attributes

Attribute NameValues
URN
  • etd-03252015-114911

Author Jeffrey Arnold Christians
Advisor Paul W. Bohn
Contributor Ruilan Guo, Committee Member
Contributor Paul W. Bohn, Committee Chair
Contributor Alexander S. Mukasyan , Committee Member
Contributor Prashant V. Kamat, Committee Member
Degree Level Doctoral Dissertation
Degree Discipline Chemical Engineering
Degree Name Doctor of Philosophy
Defense Date
  • 2015-03-20

Submission Date 2015-03-25
Country
  • United States of America

Subject
  • spectroscopy

  • perovskite

  • hole transfer

  • solar cells

  • photovoltaics

  • methylammonium lead iodide

Publisher
  • University of Notre Dame

Language
  • English

Record Visibility and Access Public
Content License
  • All rights reserved

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