Upconversion optical nanomaterials applied for photocatalysis and photovoltaics: Recent advances and perspectives

Atabaev, Timur Sh.; Molkenova, Anara

doi:10.1007/s11706-019-0482-z

Cited by 37 publications

(23 citation statements)

References 49 publications

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“…79 AFQMC/UHF AFQMC/UKS AFQMC/CAS Expt. 80 3.86 (9) 3.62 (8) 3.61(7) >3.35 Table 2. In nearly every case, the DLPNO-CCSD(T) Figure 3: A comparison of T1 values for included TD-DFT functionals, KS-B3LYP, and DLPNO-CCSD(T).…”

Section: Experimental Methodsmentioning

confidence: 99%

In-Silico Prediction of Annihilators for Triplet Fusion Upconversion via Auxiliary-Field Quantum Monte Carlo

Weber

Churchill²,

Arthur³

et al. 2020

Preprint

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<div>The energy of the lowest-lying triplet state (T1) relative to the ground and first-excited singlet states (S0, S1) plays a critical role in optical multiexcitonic processes of organic chromophores. Focusing on triplet fusion upconversion, the S0 to T1 energy gap, known as the triplet energy, is difficult to measure experimentally for most molecules of interest. Ab initio predictions can provide a useful alternative, however</div><div>low-scaling electronic structure methods such as the Kohn-Sham and time-dependent variants of Density Functional Theory (DFT) rely heavily on the fraction of exact exchange chosen for a given functional, and tend to be unreliable when strong electronic correlation is present. Here, we apply auxiliary-field quantum Monte Carlo (AFQMC), a scalable electronic structure method capable of accurately describing even strongly correlated molecules, to predict the triplet energies for a series of candidate annihilators for triplet fusion (TF) upconversion, including 9,10 substituted anthracenes and substituted benzothiadiazole (BTD) and benzoselenodiazole (BSeD) compounds. We compare our results to predictions from a number of commonly used DFT functionals, as well as DLPNO-CCSD(T0), a localized approximation to coupled cluster with singles, doubles, and perturbative triples. Together with S1 estimates from absorption/emission spectra, which are well-reproduced by TD-DFT calculations employing the range-corrected hybrid functional CAM-B3LYP, we provide predictions regarding</div><div>the thermodynamic feasibility of upconversion by requiring a) the measured T1 of the sensitizer exceeds that of the calculated T1 of the candidate annihilator, and b) twice</div><div>the T1 of the annihilator exceeds its S1 energetic value. We demonstrate a successful example of in silico discovery of a novel annihilator, phenyl-substituted BTD, and present experimental validation of upconverted blue light emission when coupled to a platinum octaethylporphyrin (PtOEP) sensitizer. The BTD framework thus represents a new class of annihilators for TF upconversion. Its chemical functionalization, guided by the computational tools utilized herein, provides a promising route towards high energy (violet to near-UV) emission.</div>

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Section: Experimental Methodsmentioning

confidence: 99%

In-Silico Prediction of Annihilators for Triplet Fusion Upconversion via Auxiliary-Field Quantum Monte Carlo

Weber

Churchill²,

Arthur³

et al. 2020

Preprint

View full text Add to dashboard Cite

show abstract

“…Triplet-triplet annihilation (TTA) upconversion is a process which enables a system to emit photons of an energy higher than the energy of absorbed photons. This phenomenon has been used to increase the theoretical efficiency of photovoltaics, 4,8 and to perform optogenetic manipulations and photocatalytic reactions with visible light in media (e.g. biological tissue) accessible only by photons of lower energy.…”

Section: Introductionmentioning

confidence: 99%

In silico prediction of annihilators for triplet–triplet annihilation upconversion via auxiliary-field quantum Monte Carlo

et al. 2021

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“…Lanthanide-doped core–shell upconverting nanoparticles (UCNPs) have been widely studied due to their advantages of enhancing luminescence, improving emission stability, separating multiple dopants, etc., which promises many specific applications, such as bioimaging [ 1 , 2 , 3 , 4 , 5 , 6 ], drug delivery [ 7 , 8 , 9 ], biosensors [ 10 , 11 , 12 ], 3D display [ 13 ], optical multiplexing [ 14 , 15 ], photovoltaics [ 16 ] and photodynamic therapy [ 17 ]. Precisely controlling the shell growth direction is essential in order to guarantee the desired structure and avoid the unwanted crosstalk between different emitters in the multifunctional core–shell nanocrystals [ 18 ].…”

Section: Introductionmentioning

confidence: 99%

Low-Temperature-Induced Controllable Transversal Shell Growth of NaLnF4 Nanocrystals

et al. 2021

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Highly controllable anisotropic shell growth is essential for further engineering the function and properties of lanthanide-doped luminescence nanocrystals, especially in some of the advanced applications such as multi-mode bioimaging, security coding and three-dimensional (3D) display. However, the understanding of the transversal shell growth mechanism is still limited today, because the shell growth direction is impacted by multiple complex factors, such as the anisotropy of surface ligand-binding energy, anisotropic core–shell lattice mismatch, the size of cores and varied shell crystalline stability. Herein, we report a highly controlled transversal shell growth method for hexagonal sodium rare-earth tetrafluoride (β-NaLnF4) nanocrystals. Exploiting the relationship between reaction temperature and shell growth direction, we found that the shell growth direction could be tuned from longitudinal to transversal by decreasing the reaction temperature from 310 °C to 280 °C. In addition to the reaction temperature, we also discussed the roles of other factors in the transversal shell growth of nanocrystals. A suitable core size and a relative lower shell precursor concentration could promote transversal shell growth, although different shell hosts played a minor role in changing the shell growth direction.

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Upconversion optical nanomaterials applied for photocatalysis and photovoltaics: Recent advances and perspectives

Cited by 37 publications

References 49 publications

In-Silico Prediction of Annihilators for Triplet Fusion Upconversion via Auxiliary-Field Quantum Monte Carlo

In-Silico Prediction of Annihilators for Triplet Fusion Upconversion via Auxiliary-Field Quantum Monte Carlo

In silico prediction of annihilators for triplet–triplet annihilation upconversion via auxiliary-field quantum Monte Carlo

Low-Temperature-Induced Controllable Transversal Shell Growth of NaLnF4 Nanocrystals

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