Periodic Reporting for period 1 - SUPERLASER (ROOM TEMPERATURE SUPERRADIANT PEROVSKITE LASERS)
Okres sprawozdawczy: 2024-09-01 do 2025-08-31
Coherent light sources are currently limited to state‑of‑the‑art lasers based on free‑electron or solid‑state semiconductor gain media stabilized by high‑quality optical cavities. However, thermal vibrations of the cavity mirrors induce phase noise and linewidth broadening, which fundamentally limits spectral purity. SUPERLASER aims to transform the field of lasing by developing green, low‑cost, solution‑processable, efficient halide perovskite lasers with ultra‑narrow linewidths operating in the superradiant regime. In the first year, SUPERLASER moved from project launch to tangible scientific and technological results along the full chain from materials design to device and sustainability work. Theory and modelling activities established a hierarchical computational framework for perovskite phase prediction. Large single crystals and continuous perovskite structures were grown by solution‑based routes such as inverse temperature crystallization and confined‑growth methods. In parallel, a first generation of functional materials for devices was produced: inorganic electron‑transport layers with tailored band alignment and conductivity, and families of organic semiconductors for electron and hole injection, which are now being shared and integrated across the consortium. For superradiance validation, an advanced optical characterization platform was installed and commissioned, including femtosecond transient absorption spectroscopy combined with a cryostat. First‑generation PeLED stacks using the newly developed transport layers were fabricated, together with optimized electrode layouts and resonator‑compatible substrates.
To achieve its main objectives, SUPERLASER is structured into four key phases:
Phase 1 – Project Launch and Coordination (WP1):
The project officially began with its Kick-off Meeting on September 23–24, 2024, hosted by NCSR “Demokritos” (coordinator). This phase ensured alignment across partners, established management procedures, and secured compliance with EC regulations, budgetary, and contractual obligations.
Phase 2 – Predictive Design and Material Development (WP2, WP3):
This phase focused on predicting and developing over one million potential halide perovskite phases with strong Rashba spin–orbit coupling (SOC) and no critical raw materials. The University of Nottingham (UoN) implemented a hierarchical computational discovery framework combining machine learning (ML), atomistic modeling, and DFT simulations to rapidly assess structural stability and optoelectronic properties. A dataset of 80 representative phases was generated using molecular dynamics accelerated by ML, forming the basis for a predictive tolerance factor model capable of mapping stability and guiding synthesis for 996 novel compounds.
In parallel, Linköping University (LiU) developed inorganic charge-transport layers, such as ZnO, optimized for perfect energy-level matching with perovskite emitters. The National and Kapodistrian University of Athens (NKUA) designed both n-type (e.g. PEI dendrimers, TDPPQ derivatives) and p-type organic semiconductors (e.g. Spiro-OMeTAD and derivatives) as efficient electron and hole injection layers in PeLEDs, enabling improved charge balance and device stability.
Phase 3 – Superlattice Development and Superradiance Validation (WP4, WP5):
This phase focused on fabricating and characterizing superradiant perovskite superlattices using solution-based, low-temperature methods. NCSR “D” successfully grew large MAFAPbI₃ crystals, with and without Rb incorporation, via inverse temperature crystallization. Universitat Jaume I (INAM-UJI) explored complementary synthetic routes such as space confinement and antisolvent-assisted crystallization, achieving Sn-based 3D perovskite single crystals. EPFL produced 2D and quasi-2D superlattices atop 3D perovskite substrates using a solution-phase approach, supporting the development of ordered, defect-minimized structures.
To validate room-temperature superradiance, LiU installed a cryostat-integrated transient absorption spectroscopy setup, enabling measurements from 300 K to 10 K. A new optical coherence protocol based on femtosecond transient absorption spectroscopy was also established, providing a reliable means to detect and quantify superradiant emission and coherence dynamics in perovskite thin films.
Phase 4 – Device Design, Prototyping, and Sustainability Assessment (WP6, WP7):
In the final phase, IMEC fabricated prototype PeLED devices exhibiting ultra-fast response times and current densities exceeding 10⁴ A/cm², establishing the groundwork for electrically pumped superradiant perovskite lasers. These devices will integrate superlattice emitters from earlier phases with optimized organic/inorganic charge transport layers.
Phase 1 – Project Launch and Coordination (WP1):
The project officially began with its Kick-off Meeting on September 23–24, 2024, hosted by NCSR “Demokritos” (coordinator). This phase ensured alignment across partners, established management procedures, and secured compliance with EC regulations, budgetary, and contractual obligations.
Phase 2 – Predictive Design and Material Development (WP2, WP3):
This phase focused on predicting and developing over one million potential halide perovskite phases with strong Rashba spin–orbit coupling (SOC) and no critical raw materials. The University of Nottingham (UoN) implemented a hierarchical computational discovery framework combining machine learning (ML), atomistic modeling, and DFT simulations to rapidly assess structural stability and optoelectronic properties. A dataset of 80 representative phases was generated using molecular dynamics accelerated by ML, forming the basis for a predictive tolerance factor model capable of mapping stability and guiding synthesis for 996 novel compounds.
In parallel, Linköping University (LiU) developed inorganic charge-transport layers, such as ZnO, optimized for perfect energy-level matching with perovskite emitters. The National and Kapodistrian University of Athens (NKUA) designed both n-type (e.g. PEI dendrimers, TDPPQ derivatives) and p-type organic semiconductors (e.g. Spiro-OMeTAD and derivatives) as efficient electron and hole injection layers in PeLEDs, enabling improved charge balance and device stability.
Phase 3 – Superlattice Development and Superradiance Validation (WP4, WP5):
This phase focused on fabricating and characterizing superradiant perovskite superlattices using solution-based, low-temperature methods. NCSR “D” successfully grew large MAFAPbI₃ crystals, with and without Rb incorporation, via inverse temperature crystallization. Universitat Jaume I (INAM-UJI) explored complementary synthetic routes such as space confinement and antisolvent-assisted crystallization, achieving Sn-based 3D perovskite single crystals. EPFL produced 2D and quasi-2D superlattices atop 3D perovskite substrates using a solution-phase approach, supporting the development of ordered, defect-minimized structures.
To validate room-temperature superradiance, LiU installed a cryostat-integrated transient absorption spectroscopy setup, enabling measurements from 300 K to 10 K. A new optical coherence protocol based on femtosecond transient absorption spectroscopy was also established, providing a reliable means to detect and quantify superradiant emission and coherence dynamics in perovskite thin films.
Phase 4 – Device Design, Prototyping, and Sustainability Assessment (WP6, WP7):
In the final phase, IMEC fabricated prototype PeLED devices exhibiting ultra-fast response times and current densities exceeding 10⁴ A/cm², establishing the groundwork for electrically pumped superradiant perovskite lasers. These devices will integrate superlattice emitters from earlier phases with optimized organic/inorganic charge transport layers.
SUPERLASER advances far beyond the state of the art in coherent light generation by introducing a materials-driven paradigm for achieving ultra-coherent laser emission at room temperature without conventional high-Q cavities. While traditional lasers rely on resonator feedback limited by thermal and mechanical noise, SUPERLASER redefines coherence as an intrinsic property of the gain medium, realized through superradiant perovskite superlattices with non-trivial topology.
At the materials level, the project employs a machine-learning-accelerated computational framework that predicts the stability and phase behavior of mixed halide perovskites across vast compositional spaces. This hierarchical design approach establishes the first predictive rules for room-temperature superradiance, surpassing current empirical and low-temperature systems. Molecular dynamics–based phase stability models further enable precise control over structure, electronic coupling, and spin–orbit interactions—capabilities beyond existing simulation tools.
Experimentally, SUPERLASER pioneers the fabrication of continuous perovskite superlattices, eliminating interface-induced coherence loss seen in nanocrystal assemblies. These ordered structures sustain collective light–matter coupling over macroscopic scales, achieving room-temperature superradiance in a solid-state material. Femtosecond transient absorption spectroscopy integrated with cryogenic and ambient setups allows direct measurement of coherence lifetimes and emission dynamics with unprecedented precision.
In device engineering, the project develops advanced charge-transport materials and electrically pumped perovskite lasers capable of sub-nanosecond operation, combining high mobility, low non-radiative loss, and topologically protected emission. This represents a critical breakthrough toward sustainable, high-speed perovskite laser diodes.
Environmentally, SUPERLASER integrates life-cycle assessment (LCA) and circular design principles from the outset, minimizing e-waste and ensuring full recyclability—contrasting sharply with traditional, resource-intensive laser fabrication.
At the materials level, the project employs a machine-learning-accelerated computational framework that predicts the stability and phase behavior of mixed halide perovskites across vast compositional spaces. This hierarchical design approach establishes the first predictive rules for room-temperature superradiance, surpassing current empirical and low-temperature systems. Molecular dynamics–based phase stability models further enable precise control over structure, electronic coupling, and spin–orbit interactions—capabilities beyond existing simulation tools.
Experimentally, SUPERLASER pioneers the fabrication of continuous perovskite superlattices, eliminating interface-induced coherence loss seen in nanocrystal assemblies. These ordered structures sustain collective light–matter coupling over macroscopic scales, achieving room-temperature superradiance in a solid-state material. Femtosecond transient absorption spectroscopy integrated with cryogenic and ambient setups allows direct measurement of coherence lifetimes and emission dynamics with unprecedented precision.
In device engineering, the project develops advanced charge-transport materials and electrically pumped perovskite lasers capable of sub-nanosecond operation, combining high mobility, low non-radiative loss, and topologically protected emission. This represents a critical breakthrough toward sustainable, high-speed perovskite laser diodes.
Environmentally, SUPERLASER integrates life-cycle assessment (LCA) and circular design principles from the outset, minimizing e-waste and ensuring full recyclability—contrasting sharply with traditional, resource-intensive laser fabrication.