Efficient Energy Transfer from Quantum Dots to Closely‐Bound Dye Molecules without Spectral Overlap DOI Open Access
Quinten A. Akkerman,

Mariam Kurashvili,

Jordi Llusar

et al.

Angewandte Chemie, Journal Year: 2024, Volume and Issue: unknown

Published: Oct. 29, 2024

Abstract Quantum dots (QDs) are semiconductor nanocrystals whose optical properties can be tuned by altering their size. By combining QDs with dyes we make hybrid QD‐dye systems exhibiting energy transfer (ET) between and dyes, which is important in sensing lighting applications. In conventional that need a shell to passivate surface defects, ET usually proceeds through Förster resonance (FRET) requires significant spectral overlap QD emission dye absorbance, as well large oscillator strengths of those transitions. This considerably limits the choice dyes. contrast, perovskite do not require passivating shells for bright emission, makes mechanisms beyond FRET accessible. work explores design CsPbBr 3 system achieve efficient from dimethyl iminium binding groups where close facilitates spatial wavefunction overlap. Using steady‐state time‐resolved photoluminescence experiments, demonstrate minimal via Dexter exchange‐type mechanism, overcomes restriction severely tunability these systems. approach opens new avenues QD‐molecule hybrids wide range applications, such lighting.

Language: Английский

Steering Energy Transfer Pathways through Mn-Doping in Perovskite Nanocrystals DOI

Akshaya Chemmangat,

S. F. Murray, Prashant V. Kamat

et al.

Journal of the American Chemical Society, Journal Year: 2025, Volume and Issue: unknown

Published: Jan. 23, 2025

Modulation of singlet and triplet energy transfer from excited semiconductor nanocrystals to attached dye molecules remains an important criterion for the design light-harvesting assemblies. Whereas one can consider selection donor acceptor with favorable energetics, spectral overlap, kinetics as a means direct pathways, it is not obvious how control characteristics nanocrystal itself. By doping CsPb(Cl0.7Br0.3)3 Mn2+, we have now succeeded in increasing nanocrystals. The between Mn-CsPb(Cl0.7Br0.3)3 cyanine (4,5-benzoindotricarbocyanine) show participation band gap states Mn2+-activated transfer. tracking emission well transient absorption features, were able distinguish two independent pathways. exciton unchanged (2%), concentration Mn2+ perovskite results increase yield up 17.5%. ability enhance through Mn-doping opens new opportunities develop optoelectronic display devices.

Language: Английский

Citations

1
Energy Cascade in Halide Perovskite-Multiple Chromophore Films: Direct versus Mediated Transfer DOI
Jishnudas Chakkamalayath, L. Martin, Prashant V. Kamat

et al.

ACS Photonics, Journal Year: 2024, Volume and Issue: 11(4), P. 1821 - 1831

Published: March 20, 2024

The capability of halide perovskite nanocrystals to sensitize both singlet and triplet excited states a chromophore highlights their potential as photosensitizers in down conversion (singlet energy transfer) or upconversion (triplet transfer followed by triplet–triplet annihilation) applications. In semiconductor-multiple assemblies, however, various possibilities arise modulate the process hence final emission output. By employing CsPbBr3 (Eg = 2.47 eV) primary sensitizer, we have now probed two dyes, viz., rubrene (Es 2.23 DBP, perylene derivative 2.07 eV). first characterizing excited-state interactions between individual dye pairs, establish favorable pathway for donor–acceptor1–acceptor2 assembly. efficiencies CsPbBr3-rubrene, rubrene-DBP, CsPbBr3-DBP systems were quantified 89%, 94%, 28%, respectively. When all three components (CsPbBr3-rubrene-DBP) are present film, observe cascading yield high population excited-states DBP. 1DBP* increased with concentration, thus confirming its mediating role cascade. Thus, proper choice mediator can promote when spectral overlap donor acceptor is poor. Elucidation CsPbBr3-rubrene DBP films offers new insights into sensitization multiple assemblies ways flow.

Language: Английский

Citations

5
Deciphering the Energy Transfer Mechanism Across Metal Halide Perovskite‐Phthalocyanine Interfaces DOI Creative Commons
Alejandro Cortés‐Villena, Alejandro Cadranel, Kobra Azizi

et al.

Advanced Science, Journal Year: 2025, Volume and Issue: unknown

Published: Jan. 10, 2025

Abstract Energy transfer processes in nanohybrids are at the focal point of conceptualizing, designing, and realizing novel energy‐harvesting systems featuring nanocrystals that absorb photons their energy unidirectionally to surface‐immobilized functional dyes. Importantly, functionality these dyes defines ultimate application. Herein, CsPbBr 3 perovskite (NCs) interfaced with zinc phthalocyanine (ZnPc) carboxylic acid. The is photosensitization singlet oxygen. @ZnPc nanohybrid best our knowledge first example, which an unusual Dexter‐type between metal halide enables oxygen generation as a proof‐of‐concept A detailed temporal picture mechanism made possible by combining key time‐resolved spectroscopic techniques, are, femtosecond, nanosecond, microsecond transient absorption spectroscopy well time‐correlated single photon counting, target analyses. In fact, three excitonic components NCs govern concerted transfer. work illustrates potential photosensitizer ZnPc produce ( 1 O 2 ) almost quantitatively while photoexciting .

Language: Английский

Citations

0
Investigating Energy-Transfer Interactions in Perovskite Quantum Dot–Dye Assemblies DOI
Selin E. Donmez, Sisi Wang,

Unaisah Vorajee

et al.

The Journal of Physical Chemistry C, Journal Year: 2025, Volume and Issue: unknown

Published: Feb. 18, 2025

Language: Английский

Citations

0
Photon Management Through Energy Transfer in Halide Perovskite Nanocrystal–Dye Hybrids: Singlet vs Triplet Tuning DOI
Jishnudas Chakkamalayath,

Akshaya Chemmangat,

Jeffrey T. DuBose

et al.

Accounts of Chemical Research, Journal Year: 2025, Volume and Issue: unknown

Published: April 15, 2025

ConspectusPhotoinduced energy and electron transfer processes offer a convenient way to convert light into electrical or chemical energy. These remain the basis of operation thin film solar cells, emitting optoelectronic devices, fuel generation. In many these applications, semiconductor nanocrystals that absorb in visible near-infrared region are building blocks harvest photons initiate surface-bound chromophores. Such multifunctional aspects make it challenging steer pathway selectively. Proper selection nanocrystal donor requires consideration bandgap, along with alignment valence conduction band energies relative acceptor, order achieve desired output transfer.In this Account, we focus on key managing flow from excited The singlet triplet characteristics nanoparticle enable tuning pathways through bandgap engineering. addition levels between singlet/triplet acceptor dye, other parameters such as spectral overlap, surface binding functional groups, rate competing all play integral roles directing transfer. For example, prototypical halide perovskite nanocrystal-rhodamine dye assembly, is observed when high-bandgap (e.g., CsPbBr3, Eg= 2.47 eV). However, low-bandgap CsPbI3, Eg = 1.87 eV), one observes only Tuning mixed perovskites CsPb(BrxI1-x)3) allows for populations both states dye. Additionally, can be further enhanced Mn doping which places low-energy triplet-active within donor.The ability nanocrystal-dye assembly finds its use design semiconductor-multichromophoric films. hybrid films down-shift up-convert incident deliver emission at wavelengths. By selecting high CsPbBr3) cascade, case CsPbBr3-rubrene-tetraphenyldibenzoperiflanthene (DBP) system populate DBP (perylene derivative). On hand, low CsPbI3-rubrene-DBP, via triplet-triplet annihilation. Thus, by steering pathways, possible manage photon obtain output. Fundamental understanding state responsible will assist designing harvesting assemblies delivery effectively display devices devices.

Language: Английский

Citations

0
Differential substitution of Ga3+ by Mn2+ and Cr3+ in LiGa5O8 to prepare multi-mode fluorescent materials as array elements for anti-counterfeiting DOI
Siyu Lu,

Jian Wang,

Qi Zhu

et al.

Journal of Alloys and Compounds, Journal Year: 2024, Volume and Issue: 1003, P. 175567 - 175567

Published: July 15, 2024

Language: Английский

Citations

2
Efficient Energy Transfer from Quantum Dots to Closely‐Bound Dye Molecules without Spectral Overlap DOI Open Access
Quinten A. Akkerman,

Mariam Kurashvili,

Jordi Llusar

et al.

Angewandte Chemie International Edition, Journal Year: 2024, Volume and Issue: unknown

Published: Oct. 29, 2024

Quantum dots (QDs) are semiconductor nanocrystals whose optical properties can be tuned by altering their size. By combining QDs with dyes we make hybrid QD-dye systems exhibiting energy transfer (ET) between and dyes, which is important in sensing lighting applications. In conventional that need a shell to passivate surface defects, ET usually proceeds through Förster resonance (FRET) requires significant spectral overlap QD emission dye absorbance, as well large oscillator strengths of those transitions. This considerably limits the choice dyes. contrast, perovskite do not require passivating shells for bright emission, makes mechanisms beyond FRET accessible. work explores design CsPbBr

Language: Английский

Citations

2
Mapping Binding Sites for Efficient Hole Extraction in Lead Halide Perovskites through Sulfur‐Based Ligand Engineering DOI Open Access

Soumyadeep De,

Siddharth Singh,

Pooja Aggarwal

et al.

Advanced Optical Materials, Journal Year: 2024, Volume and Issue: unknown

Published: Dec. 16, 2024

Abstract Lead halide perovskite nanocrystals (NCs) rapidly emerge as promising materials for photovoltaics. However, to fully harness their potential, efficient charge extraction is crucial. Despite rapid advancements, the specific active sites where acceptor molecules interact remain inadequately understood. Surface chemistry and interfacial properties are pivotal, they directly impact transfer efficiency overall device performance. This study identifies maps binding hole transporters, examining influence on dynamics through ligand engineering with 2,3‐dimercaptopropanol (DMP), a compound strong affinity lead (Pb). DMP effectively passivates Pb in CsPbBr 3 (CPB) NCs, enhancing photoluminescence (PL) by forming stable chelating bonds. DMP‐modified CPB nearly completely suppresses ─COOH‐functionalized ferrocene (FcA) partially ─NMe 2 ‐functionalized (FcAm), suggesting an alternative pathway FcAm. further supported enhanced bromine‐excess (CPB‐Br(XS)) synthesized via SOBr treatment. The distinct interactions validated steady‐state time‐resolved PL, along transient absorption spectroscopy. These findings underscore role of strategic NC‐charge interactions, enabling better extraction, higher solar cell efficiency, reduced toxicity binding.

Language: Английский

Citations

0
Investigation on luminescence photoswitching stability in diarylethene-perovskite quantum dot hybrids DOI
Ashkan Mokhtar, Yuji Akaishi,

Keisuke Tokudome

et al.

Photochemical & Photobiological Sciences, Journal Year: 2024, Volume and Issue: 23(11), P. 2015 - 2027

Published: Oct. 20, 2024

Language: Английский

Citations

0
Efficient Energy Transfer from Quantum Dots to Closely‐Bound Dye Molecules without Spectral Overlap DOI Open Access
Quinten A. Akkerman,

Mariam Kurashvili,

Jordi Llusar

et al.

Angewandte Chemie, Journal Year: 2024, Volume and Issue: unknown

Published: Oct. 29, 2024

Abstract Quantum dots (QDs) are semiconductor nanocrystals whose optical properties can be tuned by altering their size. By combining QDs with dyes we make hybrid QD‐dye systems exhibiting energy transfer (ET) between and dyes, which is important in sensing lighting applications. In conventional that need a shell to passivate surface defects, ET usually proceeds through Förster resonance (FRET) requires significant spectral overlap QD emission dye absorbance, as well large oscillator strengths of those transitions. This considerably limits the choice dyes. contrast, perovskite do not require passivating shells for bright emission, makes mechanisms beyond FRET accessible. work explores design CsPbBr 3 system achieve efficient from dimethyl iminium binding groups where close facilitates spatial wavefunction overlap. Using steady‐state time‐resolved photoluminescence experiments, demonstrate minimal via Dexter exchange‐type mechanism, overcomes restriction severely tunability these systems. approach opens new avenues QD‐molecule hybrids wide range applications, such lighting.

Language: Английский

Citations

0