Publication Date

5-2023

Date of Final Oral Examination (Defense)

1-10-2023

Type of Culminating Activity

Dissertation

Degree Title

Doctor of Philosophy in Materials Science and Engineering

Department

Materials Science and Engineering

Supervisory Committee Chair

David Estrada, Ph.D.

Supervisory Committee Member

Harish Subbaraman, Ph.D.

Supervisory Committee Member

Brian J. Jaques, Ph.D.

Supervisory Committee Member

Paul Simmonds, Ph.D.

Supervisory Committee Member

Josh D. Wood, Ph.D.

Abstract

As the demand for data-driven technologies such as cloud computing, artificial intelligence, and the Internet of Things increases, the value of data centers rises. However, the cost of optical interconnects that convert optical signals to electrical signals and vice versa limits the bandwidth in these data centers. Historically the optoelectronic materials of group III–V semiconductor materials are grown using epitaxy and transferred to silicon microelectronics using robotic pick-and-place technology. This costly method restricts the large-scale production of on-chip optoelectronic components such as diodes, photodetectors, and lasers. In this dissertation, we investigated the potential of black phosphorus (BP) as a material for optoelectronic devices and aerosol jet printing (AJP) as a viable deposition method. AJP-compatible inks were synthesized by mixing liquid-phase exfoliated HEBM BP flakes with isopropanol and 2-butanol solvents. The resulting printed thin films of HEBM BP exhibited photoluminescence emission suitable for optically pumped devices. Similarly, exfoliated single-crystal BP flakes were mixed with isopropanol, water, and 2-butanol to produce an AJP-compatible ink. Thin films printed on SiO2 with chemical vapor transport grown BP (CVT-BP) inks exhibited photoluminescence emission and electrical properties suitable for optically and electrically pumped optoelectronic devices. We demonstrate that these inks can be printed on various surfaces, such as flexible polyimide, glass, conformal quartz tubes, pre-deposited graphene, and WS2. We examined the relationship between BP's microstructure and its electrical and optical properties using high-resolution transmission electron microscopy. Using a previously established analytical density gradient ultracentrifugation (DGU) model, we purified polydisperse converted-BP dispersions into monolayer dispersions to exploit the layer-dependent bandgap of BP. In addition, we demonstrated that cascade centrifugation and tangential flow filtration (TFF) could be used to generate larger quantities of purified samples. We show that combining cascade centrifugation and TFF BP is an effective solution processing method for BP inks by enabling purification, surfactant removal, solvent exchange, and dispersion concentration. Our results indicate that AJP-printed BP has the potential to function as an active material in optoelectronic devices.

DOI

https://doi.org/10.18122/td.2072.boisestate

Available for download on Thursday, May 01, 2025

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