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Transient Spectroscopy of Glass-Embedded Perovskite Quantum Dots: Novel Structures in an Old Wrapping

  • Oleg V. Kozlov , Rohan Singh , Bing Ai , Jihong Zhang , Chao Liu and Victor I. Klimov EMAIL logo
Published/Copyright: April 14, 2018
Zeitschrift für Physikalische Chemie
From the journal Zeitschrift für Physikalische Chemie Volume 232 Issue 9-11

Abstract

Semiconductor doped glasses had been used by the research and engineering communities as color filters or saturable absorbers well before it was realized that their optical properties were defined by tiny specs of semiconductor matter known presently as quantum dots (QDs). Nowadays, the preferred type of QD samples are colloidal particles typically fabricated via organometallic chemical routines that allow for exquisite control of QD morphology, composition and surface properties. However, there is still a number of applications that would benefit from the availability of high-quality glass-based QD samples. These prospective applications include fiber optics, optically pumped lasers and amplifiers and luminescent solar concentrators (LSCs). In addition to being perfect optical materials, glass matrices could help enhance stability of QDs by isolating them from the environment and improving heat exchange with the outside medium. Here we conduct optical studies of a new type of all-inorganic CsPbBr3 perovskite QDs fabricated directly in glasses by high-temperature precipitation. These samples are virtually scattering free and exhibit excellent waveguiding properties which makes them well suited for applications in, for example, fiber optics and LSCs. However, the presently existing problem is their fairly low room-temperature emission quantum yields of only ca. 1%–2%. Here we investigate the reasons underlying the limited emissivity of these samples by conducting transient photoluminescence (PL) and absorption measurements across a range of temperatures from 20 to 300K. We observe that the low-temperature PL quantum yield of these samples can be as high as ~25%. However, it quickly drops (in a nearly linear fashion) with increasing temperature. Interestingly, contrary to traditional thermal quenching models, experimental observations cannot be explained in terms of a thermally activated nonradiative rate but rather suggest the existence of two distinct QD sub-ensembles of “emissive” and completely “nonemissive” particles. The temperature-induced variation in the PL efficiency is likely due to a structural transformation of the QD surfaces or interior leading to formation of extremely fast trapping sites or nonemissive phases resulting in conversion of emissive QDs into nonemissive. Thus, future efforts on improving emissivity of glass-based perovskite QD samples might focus on approaches for extending the range of stability of the low-temperature highly emissive structure/phase of the QDs up to room temperature.

Keywords: Auger recombination; carrier trapping; CsPbBr3; glass matrix; perovskite quantum dot; pholuminescence quantum yield; radiative recombination

Acknowledgments

This work was supported by the Laboratory Directed Research and Development program at Los Alamos National Laboratory. We thank Maksym Kovalenko for insightful comments.

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Supplementary Material:

The online version of this article offers supplementary material (https://doi.org/10.1515/zpch-2018-1168).

Received: 2018-02-28
Accepted: 2018-03-18
Published Online: 2018-04-14
Published in Print: 2018-08-28

©2018 Walter de Gruyter GmbH, Berlin/Boston

Articles in the same Issue

  1. Frontmatter
  2. Preface
  3. Congratulations to Alexander Eychmüller
  4. Halogens in the Synthesis of Colloidal Semiconductor Nanocrystals
  5. Controlled Aqueous Synthesis of CdSe Quantum Dots using Double-Hydrophilic Block Copolymers as Stabilizers
  6. Fabrication of Ag2S/CdS Heterostructured Nanosheets via Self-Limited Cation Exchange
  7. Ion-Selective Ligands: How Colloidal Nano- and Micro-Particles Can Introduce New Functionalities
  8. TEM, FTIR and Electrochemistry Study: Desorption of PVP from Pt Nanocubes
  9. Incorporation of CdTe Nanocrystals into Metal Oxide Matrices Towards Inorganic Nanocomposite Materials
  10. Diatoms – A “Green” Way to Biosynthesize Gold-Silica Nanocomposites?
  11. Evidence for Photo-Switchable Carrier Mobilities in Blends of PbS Nanocrystals and Photochromic Dithienylcyclopentene Derivatives
  12. Gelation-Assisted Layer-by-Layer Deposition of High Performance Nanocomposites
  13. Enhancement of the Fluorescence Quantum Yield of Thiol-Stabilized CdTe Quantum Dots Through Surface Passivation with Sodium Chloride and Bicarbonate
  14. Fluorescence Quenching of CdTe Quantum Dots with Co (III) Complexes via Electrostatic Assembly Formation
  15. Colloidal Photoluminescent Refractive Index Nanosensor Using Plasmonic Effects
  16. Towards Low-Toxic Colloidal Quantum Dots
  17. Color-Enrichment Semiconductor Nanocrystals for Biorhythm-Friendly Backlighting
  18. Transient Absorption Studies on Nanostructured Materials and Composites: Towards the Development of New Photocatalytic Systems
  19. Transient Spectroscopy of Glass-Embedded Perovskite Quantum Dots: Novel Structures in an Old Wrapping
  20. Energy Transfer Between Single Semiconductor Quantum Dots and Organic Dye Molecules
  21. Chemical Routes to Surface Enhanced Infrared Absorption (SEIRA) Substrates
  22. Plasmonic Cu/CuCl/Cu2S/Ag and Cu/CuCl/Cu2S/Au Supports with Peroxidase-Like Activity: Insights from Surface Enhanced Raman Spectroscopy
  23. n-Type Cu2O/α-Fe2O3 Heterojunctions by Electrochemical Deposition: Tuning of Cu2O Thickness for Maximum Photoelectrochemical Performance
  24. The Photoelectrochemistry of Assemblies of Semiconductor Nanoparticles at Interfaces
  25. Surface-Charge Dependent Orientation of Water at the Interface of a Gold Electrode: A Cluster Study
  26. Single Particle Spectroscopy of Radiative Processes in Colloid-to-Film-Coupled Nanoantennas
  27. Coupled Plasmon Resonances and Gap Modes in Laterally Assembled Gold Nanorod Arrays
  28. Anisotropy of Structure and Optical Properties of Self-Assembled and Oriented Colloidal CdSe Nanoplatelets
  29. Simple Electroless Synthesis of Cobalt Nanoparticle Chains, Oriented by Externally Applied Magnetic Fields
  30. Functionalization of Graphene Aerogels and their Applications in Energy Storage and Conversion
  31. Macroscopic Aerogels with Retained Nanoscopic Plasmonic Properties
  32. Application of Aqueous-Based Covalent Crosslinking Strategies to the Formation of Metal Chalcogenide Gels and Aerogels
  33. Cellulose-Based Hydrogels with Controllable Electrical and Mechanical Properties
  34. Naphthalenetetracarboxylic Diimide Derivatives: Molecular Structure, Thin Film Properties and Solar Cell Applications
  35. Metal-Phenolic Encapsulated Mesoporous Silica Nanoparticles for pH-Responsive Drug Delivery and Magnetic Resonance Imaging
  36. Extraction of K2CO3 from Low Concentration [K+] Solutions with the Aid of CO2: A Study on the Metastable Phase Equilibrium of K2CO3-Na2CO3-H2O Ternary System
https://doi.org/10.1515/zpch-2018-1168
Keywords for this article
Auger recombination; carrier trapping; CsPbBr3; glass matrix; perovskite quantum dot; pholuminescence quantum yield; radiative recombination

Articles in the same Issue

  1. Frontmatter
  2. Preface
  3. Congratulations to Alexander Eychmüller
  4. Halogens in the Synthesis of Colloidal Semiconductor Nanocrystals
  5. Controlled Aqueous Synthesis of CdSe Quantum Dots using Double-Hydrophilic Block Copolymers as Stabilizers
  6. Fabrication of Ag2S/CdS Heterostructured Nanosheets via Self-Limited Cation Exchange
  7. Ion-Selective Ligands: How Colloidal Nano- and Micro-Particles Can Introduce New Functionalities
  8. TEM, FTIR and Electrochemistry Study: Desorption of PVP from Pt Nanocubes
  9. Incorporation of CdTe Nanocrystals into Metal Oxide Matrices Towards Inorganic Nanocomposite Materials
  10. Diatoms – A “Green” Way to Biosynthesize Gold-Silica Nanocomposites?
  11. Evidence for Photo-Switchable Carrier Mobilities in Blends of PbS Nanocrystals and Photochromic Dithienylcyclopentene Derivatives
  12. Gelation-Assisted Layer-by-Layer Deposition of High Performance Nanocomposites
  13. Enhancement of the Fluorescence Quantum Yield of Thiol-Stabilized CdTe Quantum Dots Through Surface Passivation with Sodium Chloride and Bicarbonate
  14. Fluorescence Quenching of CdTe Quantum Dots with Co (III) Complexes via Electrostatic Assembly Formation
  15. Colloidal Photoluminescent Refractive Index Nanosensor Using Plasmonic Effects
  16. Towards Low-Toxic Colloidal Quantum Dots
  17. Color-Enrichment Semiconductor Nanocrystals for Biorhythm-Friendly Backlighting
  18. Transient Absorption Studies on Nanostructured Materials and Composites: Towards the Development of New Photocatalytic Systems
  19. Transient Spectroscopy of Glass-Embedded Perovskite Quantum Dots: Novel Structures in an Old Wrapping
  20. Energy Transfer Between Single Semiconductor Quantum Dots and Organic Dye Molecules
  21. Chemical Routes to Surface Enhanced Infrared Absorption (SEIRA) Substrates
  22. Plasmonic Cu/CuCl/Cu2S/Ag and Cu/CuCl/Cu2S/Au Supports with Peroxidase-Like Activity: Insights from Surface Enhanced Raman Spectroscopy
  23. n-Type Cu2O/α-Fe2O3 Heterojunctions by Electrochemical Deposition: Tuning of Cu2O Thickness for Maximum Photoelectrochemical Performance
  24. The Photoelectrochemistry of Assemblies of Semiconductor Nanoparticles at Interfaces
  25. Surface-Charge Dependent Orientation of Water at the Interface of a Gold Electrode: A Cluster Study
  26. Single Particle Spectroscopy of Radiative Processes in Colloid-to-Film-Coupled Nanoantennas
  27. Coupled Plasmon Resonances and Gap Modes in Laterally Assembled Gold Nanorod Arrays
  28. Anisotropy of Structure and Optical Properties of Self-Assembled and Oriented Colloidal CdSe Nanoplatelets
  29. Simple Electroless Synthesis of Cobalt Nanoparticle Chains, Oriented by Externally Applied Magnetic Fields
  30. Functionalization of Graphene Aerogels and their Applications in Energy Storage and Conversion
  31. Macroscopic Aerogels with Retained Nanoscopic Plasmonic Properties
  32. Application of Aqueous-Based Covalent Crosslinking Strategies to the Formation of Metal Chalcogenide Gels and Aerogels
  33. Cellulose-Based Hydrogels with Controllable Electrical and Mechanical Properties
  34. Naphthalenetetracarboxylic Diimide Derivatives: Molecular Structure, Thin Film Properties and Solar Cell Applications
  35. Metal-Phenolic Encapsulated Mesoporous Silica Nanoparticles for pH-Responsive Drug Delivery and Magnetic Resonance Imaging
  36. Extraction of K2CO3 from Low Concentration [K+] Solutions with the Aid of CO2: A Study on the Metastable Phase Equilibrium of K2CO3-Na2CO3-H2O Ternary System
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