Structure–Property Relationships in Hybrid Crystalline Materials for Multifunctional Light–Matter Interactions

Light and matter can interact in powerful ways when the light is intense enough. This phenomenon, known as optical nonlinearity, is at the heart of modern technologies that generate new colors of light, process information at ultrafast speeds, and enable quantum communication. However, finding materials that exhibit strong and stable nonlinear responses under everyday conditions remains a major challenge. Many existing materials only work at very low temperatures or degrade quickly when exposed to light, air, or heat. This dissertation explores new strategies for designing hybrid materials that combine the flexibility of organic molecules with the robustness of inorganic frameworks to achieve strong, room-temperature nonlinear optical behavior. We show how solvent molecules, hydrogen bonding, and supramolecular templates, such as crown ethers, can be used to fine-tune crystal structures and enhance light–matter interactions in a controlled, reversible way. One key discovery is that common solar-cell perovskites can be transformed into nonlinear optical materials through molecular templating, giving rise to bright light emission, improved stability, and even recyclability. These materials can be converted back to their original perovskite form without producing any waste, offering a sustainable approach to material design. We further extend this concept to multiferroic systems, where electric, magnetic, and optical properties coexist and interact. By integrating chiral (handed) molecules with magnetic components, we develop materials that can detect and respond differently to left- and right-circularly polarized light, an important step toward next-generation optical sensors and imaging devices. Overall, this dissertation establishes new molecular design principles for stable, tunable, and multifunctional hybrid materials, bridging the fields of nonlinear optics, photonics, and quantum technologies. These advances open up pathways toward more efficient optical communication systems, reconfigurable photonic circuits, and light-controlled magnetic devices operating under ambient conditions.

Name thesis:degree_name

Doctor of Philosophy

Level thesis:degree_level

doctoral

Discipline thesis:degree_discipline

Chemistry

Department dc:contributor.department

Chemistry

Grantor dc:publisher

Virginia Tech

Year dc:date.issued

2026

Author dc:creator

• Wang, Qian

Chair dc:contributor.committeechair

• Quan, Lina

Committee members dc:contributor.committeemember

• Lin, Feng
• Morris, Amanda
• Viehland, Dwight D.

• Supramolecules
• solid state materials
• upcycling
• optical nonlinearity

Statement dc:rights

• In Copyright

Licence dc:rights.uri

• http://rightsstatements.org/vocab/InC/1.0/

Language dc:language.iso

en

Dc Identifier Other

vt_gsexam:45281

OAI identifier oai:identifier

oai:vtechworks.lib.vt.edu:10919/140836