{"id":{"repo_id":"mit","oai_identifier":"oai:dspace.mit.edu:1721.1/144595"},"canonical_url":"https://search.dev.ndltd.org/etd/mit/oai:dspace.mit.edu:1721.1/144595","repository":{"repo_id":"mit","name":"MIT","base_url":"https://dspace.mit.edu/oai/request"},"display":{"title":"Light-Matter Interactions in High-Efficiency Photovoltaics, Light-Emitting Devices, and Strongly Coupled Microcavities","abstract":"The interactions of light and matter drive many of today’s devices, from electricity generation and consumption to manipulation. Within electricity generation, emerging thin film photovoltaics now rival traditional silicon-based solar cells in terms of power conversion efficiency (PCE) due to dramatic improvements to optoelectronic material properties and device architectures. Within electricity consumption, quantum dot light emitting diodes (QD-LEDs) are a high-efficiency, high color purity, versatile material candidate. Recent efforts to develop heavy metal-free QD-LEDs have led to high external quantum efficiencies in InP- and ZnSebased QDs rivaling the performance of the colloidal archetype of Cd-based QD-LEDs. Within energy manipulation, the emergence of photonics from electronics presents opportunities to engineer low-loss, low-threshold information transmission and computation by all-optical means and matter-mediated hybrid electronic/photonic processes. In this work, we investigate light-matter interactions in emerging thin film perovskite photovoltaics, heavy metal-free QD-LEDs and microcavities, and two-dimensional perovskite microcavity exciton-polaritons. First, we quantify the PCE enhancements due to photon recycling in high-efficiency Cs₀.₀₅(MA₀.₁₇FA₀.₈₃)₀.₉₅Pb(I₀.₈₃Br₀.₁₇)₃ (triple-cation) perovskite thin film photovoltaics as a function of material properties such as non-radiative recombination and the probability of photon escape. We determine that a perovskite active layer material with non-radiative rates k₁< 1x10⁴ s⁻¹ can result in practical PCE improvements of up to 1.8% due to photon recycling alone, and present material and device design principles to harness photon recycling effects in next-generation perovskite solar cells. Next, we investigate energy and charge transfer in InP/ZnSe/ZnS QD thin films and QDLEDs as a function of increasing electric field strength. We probe the voltage-controlled photoluminescence (PL) modulation of a QD-LED in reverse bias and achieve 87% PL quenching, which is, to our awareness, the highest reported quenching efficiency in InP-based QDs. We also demonstrate amplified spontaneous emission processes in QD metallic microcavities by spectral coincidence of a three-dimensional confined photon mode and photon recycling-enhanced gain region. Finally, we form exciton-polaritons (polaritons) at room-temperature in 2D perovskite microcavities resulting in, to the best of our knowledge, a record exciton-photon coupling strength for planar (C₆H₅(CH₂)₂NH₃)₂PbI₄ microcavities of ℏΩ subscript Rabi = 260 ± 5 meV. By utilizing wedged microcavities in which the cavity detuning is changed as a function of excitation position, we probe the temperature-dependent polariton photophysics for varying polariton exciton/photon character. In this way, we reveal material-specific polariton relaxation mechanisms and intracavity pumping schemes from the interplay of 2D perovskite excitonic states.","abstract_html":"The interactions of light and matter drive many of today’s devices, from electricity generation and consumption to manipulation. Within electricity generation, emerging thin film photovoltaics now rival traditional silicon-based solar cells in terms of power conversion efficiency (PCE) due to dramatic improvements to optoelectronic material properties and device architectures. Within electricity consumption, quantum dot light emitting diodes (QD-LEDs) are a high-efficiency, high color purity, versatile material candidate. Recent efforts to develop heavy metal-free QD-LEDs have led to high external quantum efficiencies in InP- and ZnSebased QDs rivaling the performance of the colloidal archetype of Cd-based QD-LEDs. Within energy manipulation, the emergence of photonics from electronics presents opportunities to engineer low-loss, low-threshold information transmission and computation by all-optical means and matter-mediated hybrid electronic/photonic processes. In this work, we investigate light-matter interactions in emerging thin film perovskite photovoltaics, heavy metal-free QD-LEDs and microcavities, and two-dimensional perovskite microcavity exciton-polaritons. First, we quantify the PCE enhancements due to photon recycling in high-efficiency Cs₀.₀₅(MA₀.₁₇FA₀.₈₃)₀.₉₅Pb(I₀.₈₃Br₀.₁₇)₃ (triple-cation) perovskite thin film photovoltaics as a function of material properties such as non-radiative recombination and the probability of photon escape. We determine that a perovskite active layer material with non-radiative rates k₁&lt; 1x10⁴ s⁻¹ can result in practical PCE improvements of up to 1.8% due to photon recycling alone, and present material and device design principles to harness photon recycling effects in next-generation perovskite solar cells. Next, we investigate energy and charge transfer in InP/ZnSe/ZnS QD thin films and QDLEDs as a function of increasing electric field strength. We probe the voltage-controlled photoluminescence (PL) modulation of a QD-LED in reverse bias and achieve 87% PL quenching, which is, to our awareness, the highest reported quenching efficiency in InP-based QDs. We also demonstrate amplified spontaneous emission processes in QD metallic microcavities by spectral coincidence of a three-dimensional confined photon mode and photon recycling-enhanced gain region. Finally, we form exciton-polaritons (polaritons) at room-temperature in 2D perovskite microcavities resulting in, to the best of our knowledge, a record exciton-photon coupling strength for planar (C₆H₅(CH₂)₂NH₃)₂PbI₄ microcavities of ℏΩ subscript Rabi = 260 ± 5 meV. By utilizing wedged microcavities in which the cavity detuning is changed as a function of excitation position, we probe the temperature-dependent polariton photophysics for varying polariton exciton/photon character. In this way, we reveal material-specific polariton relaxation mechanisms and intracavity pumping schemes from the interplay of 2D perovskite excitonic states.","abstract_has_math":false,"creators":["Laitz, Madeleine Reynolds"],"institution":"Massachusetts Institute of Technology","degree_name":"Doctoral","degree_level":null,"degree_discipline":null,"degree_department":"Massachusetts Institute of Technology. Department of Electrical Engineering and Computer Science","school":null,"contributors":[],"advisors":["Bulović, Vladimir"],"committee_chairs":[],"committee_members":[],"year":2022,"date_issued":"2022-05","date_published":"2022-05","updated_at":"2026-07-22T22:21:34Z","subjects":[],"languages":[],"rights":["In Copyright - Educational Use Permitted","Copyright MIT"],"rights_urls":["http://rightsstatements.org/page/InC-EDU/1.0/"],"identifier_entries":[]},"links":{"outbound_url":"https://hdl.handle.net/1721.1/144595","outbound_label":"Handle","outbound_source":"dc:identifier.uri"},"metadata_groups":[{"id":"people","label":"People","entries":[{"key":"dc:contributor.advisor","label":"Advisor","values":["Bulović, Vladimir"]},{"key":"dc:contributor.department","label":"Department","values":["Massachusetts Institute of Technology. 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Within electricity generation, emerging thin film photovoltaics now rival traditional silicon-based solar cells in terms of power conversion efficiency (PCE) due to dramatic improvements to optoelectronic material properties and device architectures. Within electricity consumption, quantum dot light emitting diodes (QD-LEDs) are a high-efficiency, high color purity, versatile material candidate. Recent efforts to develop heavy metal-free QD-LEDs have led to high external quantum efficiencies in InP- and ZnSebased QDs rivaling the performance of the colloidal archetype of Cd-based QD-LEDs. Within energy manipulation, the emergence of photonics from electronics presents opportunities to engineer low-loss, low-threshold information transmission and computation by all-optical means and matter-mediated hybrid electronic/photonic processes. In this work, we investigate light-matter interactions in emerging thin film perovskite photovoltaics, heavy metal-free QD-LEDs and microcavities, and two-dimensional perovskite microcavity exciton-polaritons. First, we quantify the PCE enhancements due to photon recycling in high-efficiency Cs₀.₀₅(MA₀.₁₇FA₀.₈₃)₀.₉₅Pb(I₀.₈₃Br₀.₁₇)₃ (triple-cation) perovskite thin film photovoltaics as a function of material properties such as non-radiative recombination and the probability of photon escape. We determine that a perovskite active layer material with non-radiative rates k₁< 1x10⁴ s⁻¹ can result in practical PCE improvements of up to 1.8% due to photon recycling alone, and present material and device design principles to harness photon recycling effects in next-generation perovskite solar cells. Next, we investigate energy and charge transfer in InP/ZnSe/ZnS QD thin films and QDLEDs as a function of increasing electric field strength. We probe the voltage-controlled photoluminescence (PL) modulation of a QD-LED in reverse bias and achieve 87% PL quenching, which is, to our awareness, the highest reported quenching efficiency in InP-based QDs. We also demonstrate amplified spontaneous emission processes in QD metallic microcavities by spectral coincidence of a three-dimensional confined photon mode and photon recycling-enhanced gain region. Finally, we form exciton-polaritons (polaritons) at room-temperature in 2D perovskite microcavities resulting in, to the best of our knowledge, a record exciton-photon coupling strength for planar (C₆H₅(CH₂)₂NH₃)₂PbI₄ microcavities of ℏΩ subscript Rabi = 260 ± 5 meV. By utilizing wedged microcavities in which the cavity detuning is changed as a function of excitation position, we probe the temperature-dependent polariton photophysics for varying polariton exciton/photon character. In this way, we reveal material-specific polariton relaxation mechanisms and intracavity pumping schemes from the interplay of 2D perovskite excitonic states."]},{"key":"dc:description.degree","label":"Dc Description Degree","values":["Ph.D."]},{"key":"dc:title","label":"Title","values":["Light-Matter Interactions in High-Efficiency Photovoltaics, Light-Emitting Devices, and Strongly Coupled Microcavities"]}]}],"canonical_facts":{"dc:contributor.advisor":["Bulović, Vladimir"],"dc:contributor.department":["Massachusetts Institute of Technology. Department of Electrical Engineering and Computer Science"],"dc:creator":["Laitz, Madeleine Reynolds"],"dc:date.accessioned":["2022-08-29T15:58:08Z"],"dc:date.available":["2022-08-29T15:58:08Z"],"dc:date.issued":["2022-05"],"dc:description.abstract":["The interactions of light and matter drive many of today’s devices, from electricity generation and consumption to manipulation. Within electricity generation, emerging thin film photovoltaics now rival traditional silicon-based solar cells in terms of power conversion efficiency (PCE) due to dramatic improvements to optoelectronic material properties and device architectures. Within electricity consumption, quantum dot light emitting diodes (QD-LEDs) are a high-efficiency, high color purity, versatile material candidate. Recent efforts to develop heavy metal-free QD-LEDs have led to high external quantum efficiencies in InP- and ZnSebased QDs rivaling the performance of the colloidal archetype of Cd-based QD-LEDs. Within energy manipulation, the emergence of photonics from electronics presents opportunities to engineer low-loss, low-threshold information transmission and computation by all-optical means and matter-mediated hybrid electronic/photonic processes. In this work, we investigate light-matter interactions in emerging thin film perovskite photovoltaics, heavy metal-free QD-LEDs and microcavities, and two-dimensional perovskite microcavity exciton-polaritons. First, we quantify the PCE enhancements due to photon recycling in high-efficiency Cs₀.₀₅(MA₀.₁₇FA₀.₈₃)₀.₉₅Pb(I₀.₈₃Br₀.₁₇)₃ (triple-cation) perovskite thin film photovoltaics as a function of material properties such as non-radiative recombination and the probability of photon escape. We determine that a perovskite active layer material with non-radiative rates k₁< 1x10⁴ s⁻¹ can result in practical PCE improvements of up to 1.8% due to photon recycling alone, and present material and device design principles to harness photon recycling effects in next-generation perovskite solar cells. Next, we investigate energy and charge transfer in InP/ZnSe/ZnS QD thin films and QDLEDs as a function of increasing electric field strength. We probe the voltage-controlled photoluminescence (PL) modulation of a QD-LED in reverse bias and achieve 87% PL quenching, which is, to our awareness, the highest reported quenching efficiency in InP-based QDs. We also demonstrate amplified spontaneous emission processes in QD metallic microcavities by spectral coincidence of a three-dimensional confined photon mode and photon recycling-enhanced gain region. Finally, we form exciton-polaritons (polaritons) at room-temperature in 2D perovskite microcavities resulting in, to the best of our knowledge, a record exciton-photon coupling strength for planar (C₆H₅(CH₂)₂NH₃)₂PbI₄ microcavities of ℏΩ subscript Rabi = 260 ± 5 meV. By utilizing wedged microcavities in which the cavity detuning is changed as a function of excitation position, we probe the temperature-dependent polariton photophysics for varying polariton exciton/photon character. In this way, we reveal material-specific polariton relaxation mechanisms and intracavity pumping schemes from the interplay of 2D perovskite excitonic states."],"dc:description.degree":["Ph.D."],"dc:identifier.uri":["https://hdl.handle.net/1721.1/144595"],"dc:publisher":["Massachusetts Institute of Technology"],"dc:rights":["In Copyright - Educational Use Permitted","Copyright MIT"],"dc:rights.uri":["http://rightsstatements.org/page/InC-EDU/1.0/"],"dc:title":["Light-Matter Interactions in High-Efficiency Photovoltaics, Light-Emitting Devices, and Strongly Coupled Microcavities"],"dc:type":["Thesis"],"thesis:degree_name":["Doctoral","Doctor of Philosophy"]},"updated_at":"2026-07-22T22:21:34Z"}