Hot Hole Transfer Increasing Polaron Yields in Hybrid Conjugated Polymer/PbS Blends

Strein, Elisabeth; deQuilettes, Dane W.; Hsieh, Stephen T.; Colbert, Adam E.; Ginger, David S.

doi:10.1021/jz402383x

Cited by 22 publications

(26 citation statements)

References 42 publications

(75 reference statements)

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“…Conversely, upon selective excitation of PbS NCs, PIA spectrum of the hybrid composite shows little, if any, P3HT delocalized polaron signal superimposed to PbS NC photo-induced absorption feature (compare black and red spectra in panel a of Figure 6, respectively) implying that hole transfer from PbS NCs to P3HT is hindered. Despite previous reports accounting for NC-to-CP hole transfer, 38,39 a slight contribution of such photo-induced process to the generation of mobile charge carriers in hybrid composites has been argued. 40 In our nanocomposites however, the decay of PbS NC first excitonic peak bleaching is longer in presence of P3HT (Figure 6b), whereas the ground state of P3HT appears as depopulated upon PbS NC selective excitation (Figure 6a and 6c).…”

Section: Photo-induced Processes At the Hybrid Interfacementioning

confidence: 89%

Molecular‐Level Switching of Polymer/Nanocrystal Non‐Covalent Interactions and Application in Hybrid Solar Cells

Giansante

Mastria

Lerario

et al. 2014

Adv Funct Materials

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Abstract.Hybrid composites obtained upon blending conjugated polymers and colloidal semiconductor nanocrystals are regarded as attractive photoactive materials for optoelectronic applications.Here we demonstrate that tailoring nanocrystal surface chemistry permits to control noncovalent and electronic interactions between organic and inorganic components. We show that the pending moieties of organic ligands at the nanocrystal surface do not merely confer colloidal stability while hindering charge separation and transport, but drastically impact morphology of hybrid composites during formation from blend solutions. The relevance of our approach to photovoltaic applications is demonstrated for composites based on poly(3-hexylthiophene) and lead sulfide nanocrystals, considered as inadequate until this report, which enable the fabrication of hybrid solar cells displaying a power conversion efficiency that reaches 3 %. By investigating (quasi)steady-state and time-resolved photo-induced processes in the nanocomposites and their constituents, we ascertain that electron transfer occurs at the hybrid interface yielding long-lived separated charge carriers, whereas interfacial hole transfer appears hindered. Here we provide a reliable alternative aiming to gain control over macroscopic optoelectronic properties of polymer/nanocrystal composites by mediating their non-covalent interactions via ligands' pending moieties, thus opening new possibilities towards efficient solution-processed hybrid solar cells.3

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Section: Photo-induced Processes At the Hybrid Interfacementioning

confidence: 89%

Molecular‐Level Switching of Polymer/Nanocrystal Non‐Covalent Interactions and Application in Hybrid Solar Cells

Giansante

Mastria

Lerario

et al. 2014

Adv Funct Materials

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“…have also demonstrated hot‐hole relaxation dynamics in pure CdSe/CdZnS core–shell QDs material with a hot‐hole relaxation time of 7 ps, but they did not place any emphasis on hot‐hole extraction. Recently Strein et al 48. reported non‐thermalized hole transfer in blends of poly(3‐hexylthiophene‐2,5‐diyl) (P3HT)/PbS quantum‐dot composite materials in which the hot‐hole transfer time was not mentioned clearly.…”

Section: Introductionmentioning

confidence: 99%

Hot‐Hole Extraction from Quantum Dot to Molecular Adsorbate

Singhal

Ghosh

2015

Chemistry A European J

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Ultrafast thermalized and hot-hole-transfer processes have been investigated in CdSe quantum dot (QD)/catechol composite systems in which hole transfer from photoexcited QDs to the catechols is thermodynamically favorable. A series of catechol derivatives were selected with different electron-donating and -withdrawing groups, and the effect of these groups on hole transfer and charge recombination (CR) dynamics has been investigated. The hole-transfer time was determined using the fluorescence upconversion technique and found to be 2-10 ps depending on the molecular structure of the catechol derivatives. The hot-hole-transfer process was followed after monitoring 2S luminescence of CdSe QDs. Interestingly, hot-hole extraction was observed only in the CdSe/3-methoxycatechol (3-OCH3) composite system owing to the higher electron-donating property of the 3-methoxy group. To confirm the extraction of the hot hole and to monitor the CR reaction in CdSe QD/catechol composite systems, ultrafast transient absorption studies have been carried out. Ultrafast transient-absorption studies show that the bleach recovery kinetics of CdSe QD at the 2S excitonic position is much faster in the presence of 3-OCH3. This faster bleach recovery at the 2S position in CdSe/3-OCH3 suggests hot-hole transfer from CdSe QD to 3-OCH3. CR dynamics in CdSe QD/catechol composite systems was followed by monitoring the excitonic bleach at the 1S position and was found to decrease with free energy of the CR reaction.

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“…3). Note that for a similar hybrid copolymer-NP system, Ginger et al 37,38 have reported that the transient concentration of the copolymer radical cations does not change significantly with excitation of the NP versus the NP and polymer. Thus, it is likely that hole transfer from (+)NP to (À)PDPPPV is the primary process for the formation of (À)PDPPPV(h).…”

mentioning

confidence: 94%

Driving charge separation for hybrid solar cells: photo-induced hole transfer in conjugated copolymer and semiconductor nanoparticle assemblies

Wang

Liu

Mukherjee

et al. 2014

Phys. Chem. Chem. Phys.

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Hot Hole Transfer Increasing Polaron Yields in Hybrid Conjugated Polymer/PbS Blends

Cited by 22 publications

References 42 publications

Molecular‐Level Switching of Polymer/Nanocrystal Non‐Covalent Interactions and Application in Hybrid Solar Cells

Molecular‐Level Switching of Polymer/Nanocrystal Non‐Covalent Interactions and Application in Hybrid Solar Cells

Hot‐Hole Extraction from Quantum Dot to Molecular Adsorbate

Driving charge separation for hybrid solar cells: photo-induced hole transfer in conjugated copolymer and semiconductor nanoparticle assemblies

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