High-Efficiency Carrier Multiplication and Ultrafast Charge Separation in Semiconductor Nanocrystals Studied via Time-Resolved Photoluminescence†

2006 ◽  
Vol 110 (50) ◽  
pp. 25332-25338 ◽  
Author(s):  
Richard D. Schaller ◽  
Milan Sykora ◽  
Sohee Jeong ◽  
Victor I. Klimov
Keyword(s):  
Charge Separation ◽  
High Efficiency ◽  
Semiconductor Nanocrystals ◽  
Time Resolved ◽  
Carrier Multiplication ◽  
Time Resolved Photoluminescence

Charge Separation Between Strain Coupled Quantum Dots in a Self-Assembled InAs Quantum Dot Structure

1999 ◽  
Vol 571 ◽  
Author(s):  
W. V. Schoenfeld ◽  
T. Lundstrom ◽  
P. M. Petroff
Keyword(s):  
Quantum Dots ◽  
Quantum Dot ◽  
Preliminary Data ◽  
Charge Separation ◽  
Electron Hole ◽  
Coupled Quantum Dots ◽  
Time Resolved ◽  
Inas Quantum Dot ◽  
Storage Times ◽  
Time Resolved Photoluminescence

ABSTRACTWe present an InAs QDs structure designed to separate and store photo-generated electron-hole pairs. Charge separation in the structure is demonstrated using power dependent photoluminescence and biased photoluminescence. Preliminary data from time resolved photoluminescence suggest storage times in the device in the μsec range.

scholarly journals Spectroscopic investigation of excitonic and charge photogeneration processes in organic photovoltaic cells

2021 ◽  
Author(s):  
◽  
Joseph Gallaher
Keyword(s):  
Excited States ◽  
Charge Separation ◽  
Transient Absorption ◽  
Mirror Image ◽  
Triplet Exciton ◽  
Organic Photovoltaic ◽  
Charge Generation ◽  
Time Resolved ◽  
Blend Morphology ◽  
Time Resolved Photoluminescence

<p>Organic photovoltaic (OPV) cells show significant promise as a renewable energy resource capable of meeting the world’s large and growing energy needs. Increasing device efficiency is central to achieving an economically viable option for widespread applications. To this end, a better understanding of the structure and dynamics of the electronic excited states is needed. In particular, the mechanism by which excitons (electron-hole pairs) escape their Coulombic attraction and generate photocurrent is yet to be established. In this thesis ultrafast laser spectroscopy, in particular transient absorption and time-resolved photoluminescence, are used to study: exciton relaxation, morphological effects on charge separation, and the pathway leading to triplet exciton states.  In Chapter 3, a series of oligothiophenes are synthesised with well-defined conjugation lengths to act as molecular models of polymer backbone sub-units, and thereby probe exciton relaxation processes. Time-resolved photoluminescence (TRPL) and transient absorption (TA) spectroscopy measurements presented in Chapter 4 reveal emission signatures evolve from a mirror image of absorption - which lacks vibronic structure - towards a spectrally narrower and vibronically structured species on the hundreds of femtosecond to early picosecond timescale. Analysis of this spectral evolution shows that a broad distribution of torsional conformers is driven to rapidly planarize in the excited state, including in solid films. This provides evidence that both torsional relaxation and energy migration could contribute to the non-mirror image absorption-emission spectra observed in polymer thin films.  Recently, long lived TA signatures have been attributed to triplet excited states with the suggested formation pathway being similar to organic light emitting diodes, whereby non-geminate (bimolecular) charge recombination leads to the formation of both singlet and triplet states. Isolated oligothiophenes in solution provide an ideal model system to investigate the role of structural relaxation on triplet exciton formation. Through analysis of TA spectral dynamics in Chapter 5, singlet and triplet exciton populations were tracked. Restriction of the torsional relaxation increased triplet yield suggesting vibrational hot states could drive triplet formation. This model could aid in understanding triplet exciton formation in polymer-based solar cells via spin-mixing instead of non-geminate recombination.  In a series of polymer:fullerene blends, the link between the nature of polymerfullerene intermixing and charge generation pathways was investigated. It is shown in Chapter 6 that free charge generation is most efficient in a 3-phase morphology that features intimately mixed polymer:fullerene regions amongst neat polymer and fullerene phases. Distinct spectroscopic signatures made it possible to determine whether holes occupy disordered or crystalline polymer chains. TA spectral dynamics reveal the migration of holes from intermixed to pure olymer regions in 3-phase morphology blends, which contrasted with observations in 2-phase blends. The energy gradient between the intermixed and phase-pure regions may be sufficient to drive efficient separation of charge pairs initially generated in intermixed regions, with free charges subsequently percolating through these phase-pure domains.  The photophysics of a high performance polymer:polymer blend is studied in Chapter 7 in an effort to elucidate how these blends can rival their polymer:fullerene counterparts. Optical spectroscopy reveals incomplete exciton dissociation and rapid geminate recombination in the blends. This is shown to result from a largely phase-separated morphology with domains greater than the exciton diffusion length. Significant loss of charge carriers on early timescales highlights increasing polymer: polymer solar cell efficiency requires optimizing blend morphology to realise facile charge separation.  Taken together, this thesis presents a valuable spectroscopic insight into the pathway of efficient charge separation and the importance of both blend morphology and polymer structure.</p>

scholarly journals Time-resolved photoluminescence measurements for determining voltage-dependent charge-separation efficiencies of subcells in triple-junction solar cells

2015 ◽  
Vol 106 (1) ◽  
pp. 013905 ◽  
Author(s):  
David M. Tex ◽  
Toshiyuki Ihara ◽  
Hidefumi Akiyama ◽  
Mitsuru Imaizumi ◽  
Yoshihiko Kanemitsu
Keyword(s):  
Solar Cells ◽  
Triple Junction ◽  
Charge Separation ◽  
Time Resolved ◽  
Voltage Dependent ◽  
Time Resolved Photoluminescence

PROGRESS IN HIGH EFFICIENCY UV LED RESEARCH FOR REAGENTLESS BIOAGENT DETECTION AND WATER PURIFICATION

2008 ◽  
Vol 18 (01) ◽  
pp. 179-185 ◽  
Author(s):  
MEREDITH L. REED ◽  
GREGORY A. GARRETT ◽  
ANAND V. SAMPATH ◽  
PAUL H. SHEN ◽  
CHARLES J. COLLINS ◽  
...  
Keyword(s):  
Water Purification ◽  
High Efficiency ◽  
Time Resolved ◽  
Current Time ◽  
Light Emitting ◽  
Uv Led ◽  
Photoluminescence Studies ◽  
Ultraviolet Light Emitting Diodes ◽  
Time Resolved Photoluminescence

We present material and device characterization of 280 nm semiconductor ultraviolet light emitting diodes. These devices exhibit low series resistance, wavelength stability with increasing current, and have a half-life in excess of 570hrs, depending upon the injection current. Time-resolved photoluminescence studies of these materials prior to fabrication have been correlated with the device performance. We also discuss the potential for use in water purification.

Role of Tryptophan in Protein–Nanocrystals Interaction: Energy or Charge Transfer

2018 ◽  
Vol 233 (1) ◽  
pp. 41-54 ◽  
Author(s):  
Mona Mittal ◽  
Saurabh Gautam ◽  
Pramit Kumar Chowdhury ◽  
Shashank Deep ◽  
Sameer Sapra
Keyword(s):  
Charge Transfer ◽  
Steady State ◽  
Semiconductor Nanocrystals ◽  
Binding Model ◽  
Time Resolved ◽  
Tryptophan Residues ◽  
Mechanism Of Interaction ◽  
Pl Intensity ◽  
Time Resolved Photoluminescence

Abstract The understanding of the interaction between the semiconductor nanocrystals (NCs) and the proteins are essential for design and fabrication of nanocomposites for application in the field of biotechnology. Herein, we have studied the interaction between CdTe NCs and the proteins by steady-state and time-resolved photoluminescence (PL) spectroscopy. The steady-state PL intensity of CdTe NCs is quenched and enhanced in the presence of lysozyme and bovine serum albumin, respectively. However, the PL intensity of CdTe NCs is not affected with α-synuclein, indicating the role of tryptophan moiety in the protein–NCs interaction. The detailed analysis of PL data allows us to elucidate the dominant mechanism of interaction, i.e. charge or energy transfer, depending on the location of tryptophan residues in the protein. Assuming a Poisson statistic of lysozymes around NCs, the Poisson binding model is used to understand the kinetics of charge transfer from CdTe NCs to the lysozyme. It provides the average number of lysozymes present on the surface of one CdTe NC.

scholarly journals Spectroscopic investigation of excitonic and charge photogeneration processes in organic photovoltaic cells

2021 ◽  
Author(s):  
◽  
Joseph Gallaher
Keyword(s):  
Excited States ◽  
Charge Separation ◽  
Transient Absorption ◽  
Mirror Image ◽  
Triplet Exciton ◽  
Organic Photovoltaic ◽  
Charge Generation ◽  
Time Resolved ◽  
Blend Morphology ◽  
Time Resolved Photoluminescence

<p>Organic photovoltaic (OPV) cells show significant promise as a renewable energy resource capable of meeting the world’s large and growing energy needs. Increasing device efficiency is central to achieving an economically viable option for widespread applications. To this end, a better understanding of the structure and dynamics of the electronic excited states is needed. In particular, the mechanism by which excitons (electron-hole pairs) escape their Coulombic attraction and generate photocurrent is yet to be established. In this thesis ultrafast laser spectroscopy, in particular transient absorption and time-resolved photoluminescence, are used to study: exciton relaxation, morphological effects on charge separation, and the pathway leading to triplet exciton states.  In Chapter 3, a series of oligothiophenes are synthesised with well-defined conjugation lengths to act as molecular models of polymer backbone sub-units, and thereby probe exciton relaxation processes. Time-resolved photoluminescence (TRPL) and transient absorption (TA) spectroscopy measurements presented in Chapter 4 reveal emission signatures evolve from a mirror image of absorption - which lacks vibronic structure - towards a spectrally narrower and vibronically structured species on the hundreds of femtosecond to early picosecond timescale. Analysis of this spectral evolution shows that a broad distribution of torsional conformers is driven to rapidly planarize in the excited state, including in solid films. This provides evidence that both torsional relaxation and energy migration could contribute to the non-mirror image absorption-emission spectra observed in polymer thin films.  Recently, long lived TA signatures have been attributed to triplet excited states with the suggested formation pathway being similar to organic light emitting diodes, whereby non-geminate (bimolecular) charge recombination leads to the formation of both singlet and triplet states. Isolated oligothiophenes in solution provide an ideal model system to investigate the role of structural relaxation on triplet exciton formation. Through analysis of TA spectral dynamics in Chapter 5, singlet and triplet exciton populations were tracked. Restriction of the torsional relaxation increased triplet yield suggesting vibrational hot states could drive triplet formation. This model could aid in understanding triplet exciton formation in polymer-based solar cells via spin-mixing instead of non-geminate recombination.  In a series of polymer:fullerene blends, the link between the nature of polymerfullerene intermixing and charge generation pathways was investigated. It is shown in Chapter 6 that free charge generation is most efficient in a 3-phase morphology that features intimately mixed polymer:fullerene regions amongst neat polymer and fullerene phases. Distinct spectroscopic signatures made it possible to determine whether holes occupy disordered or crystalline polymer chains. TA spectral dynamics reveal the migration of holes from intermixed to pure olymer regions in 3-phase morphology blends, which contrasted with observations in 2-phase blends. The energy gradient between the intermixed and phase-pure regions may be sufficient to drive efficient separation of charge pairs initially generated in intermixed regions, with free charges subsequently percolating through these phase-pure domains.  The photophysics of a high performance polymer:polymer blend is studied in Chapter 7 in an effort to elucidate how these blends can rival their polymer:fullerene counterparts. Optical spectroscopy reveals incomplete exciton dissociation and rapid geminate recombination in the blends. This is shown to result from a largely phase-separated morphology with domains greater than the exciton diffusion length. Significant loss of charge carriers on early timescales highlights increasing polymer: polymer solar cell efficiency requires optimizing blend morphology to realise facile charge separation.  Taken together, this thesis presents a valuable spectroscopic insight into the pathway of efficient charge separation and the importance of both blend morphology and polymer structure.</p>

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