Article
Chemistry, Multidisciplinary
Austin D. Bailey, Arundhati P. Deshmukh, Nadine C. Bradbury, Monica Pengshung, Timothy L. Atallah, Jillian A. Williams, Ulugbek Barotov, Daniel Neuhauser, Ellen M. Sletten, Justin R. Caram
Summary: Excitonic chromophore aggregates are frequently used in imaging and energy harvesting, but their rational design requires adapting self-assembly principles to excited state coupling. In this study, we synthesized redshifted variants of an amphiphilic cyanine dye and analyzed their self-assembly and photophysics. The new dyes showed tubular self-assembly and similar redshifts, but exhibited a significant decline in superradiance compared to their counterparts. Cryo-TEM revealed the formation of shorter nanotube bundles. Computational screening indicated that the narrower tubes had more disordered excitonic states with similar degrees of redshift.
Article
Chemistry, Physical
Jia-Ning Zhou, Ke-Qin Cheng, Xiaolong Zhang, Shubin Yang, Jie Liu, Wenzuo Li, Qingzhong Li, Juan Han, Xiao-Ying Xie, Ganglong Cui
Summary: Functionalizing single-walled carbon nanotubes (SWNTs) with light-harvesting molecules creates nanoarchitectures with intriguing optoelectronic properties. The effects of the aromaticity of coordinated rings on the optoelectronic properties of the nanocomposites were explored, and it was found that excited energy transfer can occur within certain nanocomposites. Electron and hole transfer from the light-harvesting molecules to SWNTs were found to be asynchronous. The large energy gaps between charge-donor and charge-acceptor states play a crucial role in regulating photoexcited state relaxation dynamics.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2023)
Article
Chemistry, Multidisciplinary
Ziyi Hu, Ben Breeze, Reza J. Kashtiban, Jeremy Sloan, James Lloyd-Hughes
Summary: This study investigated the impact of HgTe NWs synthesized inside SWCNTs on their optical and electronic properties. The results showed that the influence varied with the chirality of the SWCNTs. For semiconducting SWCNTs, HgTe NWs suppressed Auger relaxation processes and enhanced photoluminescence. On the other hand, HgTe NWs increased the Auger relaxation rate and phonon relaxation of metallic SWCNTs, boosting electronic transport.
Article
Materials Science, Multidisciplinary
Sandra Doria, Mariangela Di Donato, Raffaele Borrelli, Maxim F. Gelin, Justin Caram, Marco Pagliai, Paolo Foggi, Andrea Lapini
Summary: In this study, self-assembled light harvesting nanotubes formed by amphiphilic cyanine dyes were characterized and simulated using ultrafast spectroscopy and theoretical approaches. The results demonstrated an unusual ultrafast behavior of the nanotubes, providing new insights into transport mechanisms and excitonic interactions in these complex molecular systems.
JOURNAL OF MATERIALS CHEMISTRY C
(2022)
Article
Chemistry, Physical
Artur M. Andermann, Luis G. C. Rego
Summary: In non-fullerene organic photovoltaics, minimizing energy losses becomes less sensitive to temperature and electric field variations when the energetic driving force approaches the effective reorganization energy at the interface.
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
(2022)
Article
Chemistry, Multidisciplinary
A. Badon, J. -B Marceau, C. Allard, F. Fossard, A. Loiseau, L. Cognet, E. Flahaut, G. Recher, N. Izard, R. Martel, E. Gaufres
Summary: By confining alpha-sexithiophene (6T) molecules in boron nitride nanotubes (6T@BNNTs), fluorescence anisotropy can be induced in a transparent host. The experiments show that individual 6T@BNNTs exhibit high polarization extinction ratio at room temperature, and the fluorescence anisotropy is consistent with the alignment of encapsulated 6T molecules along the nanotube axis. By stretching a flexible transparent polymer film mixed with 6T@BNNTs, macroscopic fluorescence anisotropy can be induced within the film. This work demonstrates the use of dyes@BNNT system as a convenient platform to induce fluorescence anisotropy in photonic materials.
MATERIALS HORIZONS
(2023)
Article
Chemistry, Physical
Leonardo F. Calderon, Chern Chuang, Paul Brumer
Summary: Research shows that vibrations resonant with the energy difference between exciton states in photosynthetic dimers only have a marginal effect on energy transfer and quantum coherence compared to non-resonant vibrations under natural incoherent light excitation conditions.
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
(2023)
Article
Chemistry, Multidisciplinary
Stephanie M. Hart, James L. Banal, Maria A. Castellanos, Larysa Markova, Yuliia Vyborna, Jeffrey Gorman, Robert Haener, Adam P. Willard, Mark Bathe, Gabriela S. Schlau-Cohen
Summary: This study reports a DNA-chromophore platform that enables tailored long-range excitonic couplings and short-range charge-transfer couplings. Through combinatorial screening, the researchers discovered chromophore geometries that can enhance or suppress photochemistry. The results demonstrate the possibility of symmetry-breaking charge transfer in DNA-scaffolded squaraines, which was not previously achieved.
Article
Chemistry, Multidisciplinary
Tao Li, Bin Li, Haoxiang Zhou, Jun Wang, Gang Ni, Wanli Ma, Chuanxiang Sheng, Jianyu Yuan, Haibin Zhao
Summary: This study reports on the ultrafast dynamics of charge transfer and exciton dissociation in single-material organic solar cells for the first time. It is found that the intramolecular interface in the block copolymer has a higher transfer rate, and the dilute PBDB-T-b-PTY6 film has faster exciton dissociation. By optimizing ordering, the power conversion efficiency of organic solar cells can be improved.
ADVANCED FUNCTIONAL MATERIALS
(2023)
Article
Chemistry, Physical
Ajay Jayachandran, Stefan Mueller, Tobias Brixner
Summary: In this study, we demonstrate the acquisition of two-quantum photon echoes using fluorescence detected 2D spectroscopy, allowing for the separation of 2Q-2Q 2D spectra of a squaraine dimer and a squaraine polymer. We verify the effectiveness of cogwheel phase cycling and rationalize the observed difference in homogeneous line width as a result of exciton-exciton annihilation, exciton diffusion, and exciton delocalization.
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
(2022)
Article
Chemistry, Multidisciplinary
Seongsoo Kang, Taeyeon Kim, Yongseok Hong, Frank Wuerthner, Dongho Kim
Summary: This study explores the ultrafast photoinduced dynamics and vibrational coherences of two perylenebisimide (PBI) H-aggregates, revealing the formation of excimer and delocalized radical anion states in the excited state. The intermolecular interactions between PBI units induce the formation of these new excited states, and specific Raman modes can be crucial indicators for coherent exciton dynamics in the aggregates. Additionally, analysis using time-resolved impulsive stimulated Raman scattering provides insights into the vibrational coherences associated with the formation of these states in each aggregate system.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2021)
Article
Energy & Fuels
Ting Wang, Xunchang Wang, Renqiang Yang, Chaoxu Li
Summary: This review discusses the successful application of Forster resonance energy transfer (FRET) in promoting the efficiencies of ternary blend organic solar cells (TOSCs), highlighting the diverse framework structures of FRET pairs and the role of FRET theory in the photoconversion process, including exciton harvesting, exciton diffusion, and charge generation. Existing challenges and future research directions of FRET applications in TOSCs are also proposed.
Article
Chemistry, Multidisciplinary
Wenjing Xu, Miao Zhang, Xiaoling Ma, Xixiang Zhu, Sang Young Jeong, Han Young Woo, Jian Zhang, Wenna Du, Jian Wang, Xinfeng Liu, Fujun Zhang
Summary: Layer-by-layer all-polymer solar cells (LbL all-PSCs) were prepared using PM6 and PY-IT through sequential spin coating. The low exciton dissociation efficiency in the acceptor layer near the electrode is improved by incorporating less PM6 into the PY-IT layer. The addition of 10 wt% PM6 into the PY-IT layer results in a higher power conversion efficiency (PCE) of 17.45% compared to the PM6/PY-IT-based LbL all-PSCs with a PCE of 16.04%.
ADVANCED FUNCTIONAL MATERIALS
(2023)
Article
Energy & Fuels
Junyi Feng, Guanzhao Wen, Rong Hu, Jun Peng, Hong Lu, Ningjiu Zhao, Xianshao Zou, Wei Zhang
Summary: Recent research has shown that low-energy offset polymer solar cells (PSCs) can achieve a power conversion efficiency of over 19%. The study investigates the correlation between energy offsets and the charge photogeneration process in Y-series molecule-based PSCs. The findings reveal the importance of energy offsets for efficient charge photogeneration and recombination in ultrafast timescales for high-performance PSCs.
Article
Biochemistry & Molecular Biology
Jin-Myung Choi, Hiroki Suko, Kyusun Kim, Jiye Han, Sangsu Lee, Yutaka Matsuo, Shigeo Maruyama, Il Jeon, Hirofumi Daiguji
Summary: This study improved the moisture and oxygen barrier ability as well as heat releasing capability in the passivation of perovskite solar cells (PSCs) by adding multi-walled carbon nanotubes to the epoxy resin used for encapsulation. The PSCs encapsulated with carbon nanotube-added resin exhibited more stable operation and only experienced a ca. 30% efficiency decrease over one week compared to the ca. 63% decrease in the reference devices.
Article
Chemistry, Physical
Gajadhar Joshi, Ryan D. D. Dill, Karl J. J. Thorley, John E. E. Anthony, Obadiah G. G. Reid, Justin C. C. Johnson
Summary: We characterize the change in electron spin magnetic resonance in the photoluminescence intensity for a tailored organic molecular crystal. Resonant transitions for both triplet and quintet spin sublevel populations are observed, revealing their optical sensitivity and providing zero-field parameters for each. The data suggests significant spin polarization and orientation selectivity in this system.
JOURNAL OF CHEMICAL PHYSICS
(2022)
Article
Multidisciplinary Sciences
Brandon K. Rugg, Kori E. Smyser, Brian Fluegel, Christopher H. Chang, Karl J. Thorley, Sean Parkin, John E. Anthony, Joel D. Eaves, Justin C. Johnson
Summary: The photo-driven process of singlet fission can generate coupled triplet pairs with intriguing properties. Among the sublevels, the quintet is particularly interesting for quantum information. Previous theoretical work has shown that this sublevel can be selectively populated under certain conditions.
PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
(2022)
Review
Chemistry, Multidisciplinary
Gaurav Vats, Brett Hodges, Andrew J. Ferguson, Lance M. Wheeler, Jeffrey L. Blackburn
Summary: Metal halide perovskite based materials have gained attention as remarkable solution-processable optoelectronic materials with intriguing properties and potential applications. They are being considered for low-energy memory and information processing applications. Recent progress in using photons as a critical degree of freedom for switching, memory, and neuromorphic functionality in metal halide perovskite materials and devices is reviewed.
ADVANCED MATERIALS
(2023)
Article
Chemistry, Physical
Rachel E. Mow, Lucy J. T. Metzroth, Michael J. Dzara, Glory A. Russell-Parks, Justin C. Johnson, Derek R. Vardon, Svitlana Pylypenko, Shubham Vyas, Thomas Gennett, Wade A. Braunecker
Summary: This study reports the synthesis of a Cu(I)-loaded COF material with subnanometer pores and a three-dimensional network morphology, and investigates the sorption mechanisms of hydrogen, ethylene, and carbon monoxide with this material. The results show that all three gases desorb near or above room temperature, and can be desorbed on-demand by irradiation with ultraviolet light. This work represents a step towards developing more practical ambient temperature gas storage and efficient regeneration of sorbents.
JOURNAL OF PHYSICAL CHEMISTRY C
(2022)
Article
Chemistry, Multidisciplinary
Ivan Sudakov, Etienne Goovaerts, Wim Wenseleers, Jeffrey L. Blackburn, Juan G. Duque, Sofie Cambre
Summary: The excitonic structure of single-wall carbon nanotubes (SWCNTs) is chirality dependent and consists of multiple singlet and triplet excitons (TEs) with only one singlet exciton (SE) being optically bright. This study characterizes TEs in chirality-purified samples of (6,5) and (7,5) SWCNTs using optically detected magnetic resonance (ODMR) spectroscopy. The results show that the nanotubes sustain three types of TEs, each with different zero-field splitting (ZFS) parameters and axial symmetry, which depend on the SWCNT diameter and environment.
Article
Chemistry, Physical
Dmitry Levshov, Marina Avramenko, Maksiem Erkens, Huy-Nam Tran, Thi Thanh Cao, Van Chuc Nguyen, Emmanuel Flahaut, Valentin N. Popov, Ahmed-Azmi Zahab, Jean-Louis Sauvajol, Raul Arenal, Wim Wenseleers, Sofie Cambre, Matthieu Paillet
Summary: Measuring electronic Raman scattering (ERS) has become a efficient method for structural characterization of metallic single-wall carbon nanotubes (SWCNT), but its application to other types of SWCNT-based structures, such as double-wall carbon nanotubes (DWCNT), is not well studied. In this work, the authors combine electron diffraction, Rayleigh and Raman spectroscopies to investigate the ERS process in 21 individual DWCNTs with different electronic configurations. They observe partial suppression of ERS intensity in DWCNTs compared to SWCNTs, mainly due to dielectric screening of Coulomb interactions. Based on their experimental findings, the authors propose an adapted method for structural identification of DWCNT samples from ERS data, which can be applied to characterize emerging 1D VDW heterostructures based on metallic SWCNTs.
Article
Chemistry, Physical
Ryan D. Dill, Gajadhar Joshi, Karl J. Thorley, John E. Anthony, Brian Fluegel, Justin C. Johnson, Obadiah G. Reid
Summary: Singlet fission proceeds through a manifold of triplet-pair states that are difficult to distinguish spectroscopically. By introducing photoinduced-absorption-detected magnetic resonance (PADMR), we studied the excited-state absorption spectrum of a TSPS-PDT film. Our results clarify the origin of triplet-associated near-infrared absorption features in singlet-fission materials and demonstrate a useful tool for studying high-spin excited states.
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
(2023)
Article
Chemistry, Multidisciplinary
Marissa S. Martinez, Michelle A. Nolen, Nicholas F. Pompetti, Lee J. Richter, Carrie A. Farberow, Justin C. Johnson, Matthew C. Beard
Summary: Controlling the binding of functional organic molecules on quantum dot surfaces is crucial for understanding the resulting organic-inorganic hybrid behavior. In this study, the binding of tetracenedicarboxylate ligands on PbS quantum dots was varied through solid-state ligand exchange. Different ligand concentrations led to different structures and properties, with low concentrations resulting in mixed ligand structures, intermediate concentrations resulting in ligand-ligand interactions through hydrogen bonding, and high concentrations resulting in complete ligand exchange.
Article
Chemistry, Physical
Rachith Shanivarasanthe Nithyananda Kumar, Robbe Breugelmans, Xueshi Jiang, Shabnam Ahadzadeh, Guy Brammertz, Pieter Verding, Michael Daenen, Melissa Van Landeghem, Sofie Cambre, Koen Vandewal, Wim Deferme
Summary: The use of polyethylenimine ethoxylated (PEIE), Zinc oxide (ZnO) nanoparticles, and a PEIE-ZnO nanocomposite as functional layers for OLEDs fabricated by solution processing improves electron injection and hole blocking properties, resulting in increased external quantum efficiency. This novel deposition technique offers comparable OLED performance to spin coated and vacuum deposited electron injection layers, enabling the large area fabrication of optoelectronic devices with high efficiencies, high output, low cost, and long lifetime.
APPLIED SURFACE SCIENCE
(2023)
Article
Chemistry, Multidisciplinary
Kevin P. P. Ruoff, Melissa K. K. Gish, Ellen Song, Iskander Douair, Pragati Pandey, Mark Steger, Justin C. C. Johnson, Patrick J. J. Carroll, Michael Gau, Christopher H. H. Chang, Ross E. E. Larsen, Andrew J. J. Ferguson, Eric J. J. Schelter
Summary: A new strategy for differentiating between Dy3+ and Y3+ ions by tailoring a photochemical reaction of their isostructural complexes using the f-electron states of Dy3+ as an energy sink was disclosed. This approach provides a new method for differentiating rare earth elements that does not depend on cation size.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Chemistry, Physical
M. Alejandra Hermosilla-Palacios, Marissa Martinez, Evan A. Doud, Tobias Hertel, Alexander M. Spokoyny, Sofie Cambre, Wim Wenseleers, Yong-Hyun Kim, Andrew J. Ferguson, Jeffrey L. Blackburn
Summary: There is a growing demand for high-performance semiconductor materials and devices in order to meet the increasing energy and computing demand. Organic semiconductors (OSCs) are attractive options for opto-electronic devices due to their low cost, easy fabrication, and flexibility. This study demonstrates a direct quantification of charge carrier density and carrier mobility in chemically doped semiconducting single-walled carbon nanotubes (s-SWCNTs) using a nuclear magnetic resonance approach. The results show that hole mobility in doped s-SWCNT networks increases with increasing charge carrier density, contrary to what was expected.
NANOSCALE HORIZONS
(2023)
Article
Chemistry, Multidisciplinary
Liang-Chun Lin, Tanner Smith, Qianxiang Ai, Brandon K. Rugg, Chad Risko, John E. Anthony, Niels H. Damrauer, Justin C. Johnson
Summary: In this study, a pyrene-bridged parallel tetracene dimer (TPT) with optimized interchromophore coupling strength was synthesized. The long-lived and strongly spin-polarized multiexciton quintet state, (TT)-T-5, was observed through transient absorption and electron paramagnetic resonance spectroscopy. The lifetime of (TT)-T-5 was estimated to be >35 μs, with a dephasing time (T-2) of 726 ns at 10 K for the corresponding qubit. The experimental results support recent theoretical models.