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Related Concept Videos

Band Theory02:35

Band Theory

When two or more atoms come together to form a molecule, their atomic orbitals combine and molecular orbitals of distinct energies result. In a solid, there are a large number of atoms, and therefore a large number of atomic orbitals that may be combined into molecular orbitals. These groups of molecular orbitals are so closely placed together to form continuous regions of energies, known as the bands.
The energy difference between these bands is known as the band gap.
Conductor, Semiconductor,...
Fermi Level Dynamics01:12

Fermi Level Dynamics

The vacuum level denotes the energy threshold required for an electron to escape from a material surface. It is usually positioned above the conduction band of a semiconductor and acts as a benchmark for comparing electron energies within various materials.
Electron affinity in semiconductors refers to the energy gap between the minimum of its conduction band and the vacuum level and it is a critical parameter in determining how easily a semiconductor can accept additional electrons.
The work...
Energy Bands in Solids01:01

Energy Bands in Solids

Isolated atoms have discrete energy levels that are well described by the Bohr model. And, it quantifies the energy of an electron in a hydrogen atom as En. Higher quantum numbers 'n' yield less negative, closer electron energy levels.
 Band Formation:
When atoms are brought close together, as in a solid, these discrete energy levels begin to split due to the overlap of electron orbitals from adjacent atoms. This split occurs because of the Pauli exclusion principle, which states that no two...
Semiconductors01:22

Semiconductors

There is variation in the electrical conductivity of materials - metals, semiconductors, and insulators that are showcased with the help of the energy band diagrams.
Metals such as copper (Cu), zinc (Zn), or lead (Pb) have low resistivity and feature conduction bands that are either not fully occupied or overlap with the valence band, making a bandgap non-existent. This allows electrons in the highest energy levels of the valence band to easily transition to the conduction band upon gaining...
Carrier Generation and Recombination01:22

Carrier Generation and Recombination

Carrier generation is the process by which electron-hole pairs (EHPs) are created within the semiconductor. In direct-bandgap semiconductors, such as gallium arsenide (GaAs), this occurs efficiently when energy absorption prompts valence electrons to leap into the conduction band, leaving behind holes.
This process is given by the generation rate G and is efficient due to the conservation of momentum between the valence band maximum and conduction band minimum.
Indirect generation involves an...
Biasing of Metal-Semiconductor Junctions01:27

Biasing of Metal-Semiconductor Junctions

Biasing metal-semiconductor junctions involves applying a voltage across the junction. Specifically, the metal is connected to a voltage source, while the semiconductor is grounded. This technique is essential for controlling the direction and magnitude of current flow in electronic devices, including diodes, transistors, and photovoltaic cells.
In Schottky junctions, where the semiconductor is n-type, applying a positive voltage to the metal relative to the semiconductor reduces its Fermi...

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Tuning Energy Transfer Pathways in Halide Perovskite-Dye Hybrids through Bandgap Engineering.

Akshaya Chemmangat1, Jishnudas Chakkamalayath1, Jeffrey T DuBose1

  • 1Radiation Laboratory, Department of Chemistry and Biochemistry, and Department of Chemical and Biomolecular Engineering, University of Notre Dame, Notre Dame, Indiana 46556, United States.

Journal of the American Chemical Society
|January 24, 2024
PubMed
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We found that modifying rhodamine dyes attached to lead halide perovskite nanocrystals controls energy transfer. Stronger binding of rose Bengal to CsPbI3 perovskites maximized triplet energy transfer efficiency.

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Area of Science:

  • Materials Science
  • Photochemistry
  • Nanotechnology

Background:

  • Lead halide perovskite nanocrystals (LHPs) exhibit broad light absorption, making them promising for photocatalysis and optoelectronics.
  • Energy transfer between LHPs and acceptor dyes can tune hybrid material properties and extend excited-state lifetimes.
  • Understanding factors governing energy transfer is crucial for designing advanced semiconductor-dye hybrid systems.

Purpose of the Study:

  • To investigate the key factors influencing triplet energy transfer between CsPbI3 perovskite nanocrystals and surface-bound rhodamine dyes.
  • To correlate dye structure, surface binding, and energy transfer kinetics and efficiency.
  • To explore bandgap engineering in mixed halide perovskites for controlled singlet/triplet state generation.

Main Methods:

  • Utilized absorption and emission spectroscopies to study energy transfer mechanisms.
  • Investigated three rhodamine dyes (rhodamine B, rhodamine B isothiocyanate, rose Bengal) with varying pendant groups.
  • Employed mixed halide CsPb(Br1-xIx)3 perovskites to tune bandgap energy.

Main Results:

  • Strongest binding of rose Bengal to CsPbI3 resulted in the highest triplet energy transfer efficiency (96%) with a rate constant of 1 × 10^9 s^-1.
  • Triplet energy transfer in CsPbI3-rose Bengal was ~100 times slower than singlet energy transfer in CsPbBr3-rose Bengal (1.1 × 10^11 s^-1).
  • Mixed halide perovskites allowed systematic tuning of singlet vs. triplet excited state generation (0-100%) by adjusting the Br/I ratio.

Conclusions:

  • Pendant groups on acceptor dyes significantly impact surface binding and subsequent energy transfer kinetics and efficiency.
  • Bandgap engineering of halide perovskites offers a route to control the population of singlet and triplet excited states in hybrid systems.
  • These findings enable precise modulation of energy transfer in semiconductor-dye hybrids for advanced optoelectronic applications.