Singlet excited state (S1) of higher fullerenes C76 and C84: correlation between lifetime and HOMO–LUMO energy gap

Cho, Hyun Sun; Ahn, Tae Kyu; Yang, Sung Ik; Jin, Seung Min; Kim, Dongho; Kim, Seong Keun; Kim, Hong Doo

doi:10.1016/s0009-2614(03)00845-5

Cited by 22 publications

(11 citation statements)

References 31 publications

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“…Consistent with reported results, ,,,,, the energy gaps of HOMO and LUMO are oscillatory with respect to the number of carbon, and C 80 and C 110 possess the minimum energy gaps. Meanwhile, HOMO and LUMO distributions are displayed in Figure .…”

Section: Results and Discussionsupporting

confidence: 88%

“…So far, the ISC processes for pristine fullerenes from C 60 to C 84 have been extensively studied experimentally with comprehensive elaborations of the ISC rates and ISC quantum yields over the past several years. ,,,− The measured ISC quantum yields for C 60 , C 70 , C 76 , C 78 , and C 84 are 0.93, 0.90, 0.05, 0.12, and 0.01, respectively, ,,, decreasing with the increase of carbon number of fullerenes. For higher fullerenes C n ( n > 84), experimental studies are lacking for ISC processes because of the difficult isolation from abundant isomers, such as C 92 , C 96 , C 100 , etc.…”

Section: Introductionmentioning

confidence: 99%

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Intersystem Crossing Rates of Isolated Fullerenes: Theoretical Calculations

2017

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Although the triplet states of fullerenes have prosperous applications, it remains unclear how the structural parameters of singlet and triplet states control the intersystem crossing (ISC) rates. Here, electronic structure calculations (reorganization energy, driving force, and spin-orbit coupling) and a rate theory (Marcus formula) are employed to quantitatively predict the ISC rates of isolated fullerenes C (n = 60-110). The results demonstrate that the driving force is not the only factor to predict the ISC rates. For instance, although C, C, and C have the favorable driving force, the ISC rates are close to zero because of small spin obit couplings, whereas small ISC rates of C and C result from quite small reorganization energies. Meanwhile, in addition to well-known C and C, C possesses good ISC property with obviously large ISC rate. C also has a higher triplet-state energy than singlet-state oxygen energy; it may thus have a good photoactive property.

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Section: Results and Discussionsupporting

confidence: 88%

Section: Introductionmentioning

confidence: 99%

Intersystem Crossing Rates of Isolated Fullerenes: Theoretical Calculations

2017

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“…predicted that the addition of C 60 to graphene could enhance both quantum capacitance and EDL capacitance . However, higher fullerenes have not been studied extensively in supercapacitor applications although they may acquire lower bandgaps than that of the C 60 and may provide a better conductivity …”

Section: Introductionmentioning

confidence: 99%

Fullerene C₇₆: An Unexplored Superior Electrode Material with Wide Operating Potential Window for High‐Performance Supercapacitors

2020

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Carbon materials have widely been used to enhance the performance of a plethora of supercapacitor electrode materials. In this regard, it is crucial to identify carbon materials that function over a wide pH range while enjoying a wide potential window. Herein, the DFT calculations were used to elucidate the electronic performance of C 76 and the C 76 /electrolyte interface. The electronic investigation revealed the nature of the conductivity and charge storage mechanism of C 76 based on the bandgap and quantum capacitance calculations. Also, the electrochemical and electronic properties of fullerene C 76 have been extensively investigated over a wide pH range; acidic H 2 SO 4 , basic KOH, and neutral Na 2 SO 4 . The results showed a promising performance in the three electrolytes. Moreover, C 76 electrodes exhibited a potential window of 1.9 V in Na 2 SO 4 electrolyte, resulting in capacitances of 171 F/g and 142 F/g at a scan rate of 1 mV/s in the positive and negative potential windows, respectively. The material showed a pseudocapacitance performance of 65 % in Na 2 SO 4 electrolyte in the positive potential window. We believe higher fullerenes provide a new class of materials for developing versatile supercapacitor devices for efficient energy storage.Laboratory is highly appreciated. We also acknowledge Bibliotheca Alexandrina HPC for allowing us to use the HPC resources.

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“…The initial peak is the excitation of fullerene electrons due to absorption of the pump pulse. Electrons equilibrate among themselves in the first few picoseconds (note, this is not recombination, as recombination rates are on the order of nanoseconds or longer). − The following vibrational relaxation (cooling) is the dominating effect observed as the decay of the TDTT signal for the next few hundred picoseconds. This thermal relaxation rate has been measured experimentally and computationally for higher order fullerenes and ranges from ∼10 to 200 ps with a strong dependence on functionalization. − …”

Section: Resultsmentioning

confidence: 99%

“…used a single-color (λ = 740–800 nm) pump–probe setup, while we use a two-color (λ pump = 400 nm, λ probe = 800 nm) setup, making it easy to filter the pump and detect the probe signal. Lastly, fullerenes absorb an order of magnitude more optical energy at 400 nm compared to 800 nm, , providing larger heating events and thus increased signals due to increased pump absorption.…”

Section: Resultsmentioning

confidence: 99%

Molecular Tuning of the Vibrational Thermal Transport Mechanisms in Fullerene Derivative Solutions

Szwejkowski¹,

Giri²,

Warzoha

et al. 2017

ACS Nano

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Control over the thermal conductance from excited molecules into an external environment is essential for the development of customized photothermal therapies and chemical processes. This control could be achieved through molecule tuning of the chemical moieties in fullerene derivatives. For example, the thermal transport properties in the fullerene derivatives indene-C monoadduct (ICMA), indene-C bisadduct (ICBA), [6,6]-phenyl C butyric acid methyl ester (PCBM), [6,6]-phenyl C butyric acid butyl ester (PCBB), and [6,6]-phenyl C butyric acid octyl ester (PCBO) could be tuned by choosing a functional group such that its intrinsic vibrational density of states bridge that of the parent molecule and a liquid. However, this effect has never been experimentally realized for molecular interfaces in liquid suspensions. Using the pump-probe technique time domain thermotransmittance, we measure the vibrational relaxation times of photoexcited fullerene derivatives in solutions and calculate an effective thermal boundary conductance from the opto-thermally excited molecule into the liquid. We relate the thermal boundary conductance to the vibrational modes of the functional groups using density of states calculations from molecular dynamics. Our findings indicate that the attachment of an ester group to a C molecule, such as in PCBM, PCBB, and PCBO, provides low-frequency modes which facilitate thermal coupling with the liquid. This offers a channel for heat flow in addition to direct coupling between the buckyball and the liquid. In contrast, the attachment of indene rings to C does not supply the same low-frequency modes and, thus, does not generate the same enhancement in thermal boundary conductance. Understanding how chemical functionalization of C affects the vibrational thermal transport in molecule/liquid systems allows the thermal boundary conductance to be manipulated and adapted for medical and chemical applications.

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Singlet excited state (S1) of higher fullerenes C76 and C84: correlation between lifetime and HOMO–LUMO energy gap

Cited by 22 publications

References 31 publications

Intersystem Crossing Rates of Isolated Fullerenes: Theoretical Calculations

Intersystem Crossing Rates of Isolated Fullerenes: Theoretical Calculations

Fullerene C₇₆: An Unexplored Superior Electrode Material with Wide Operating Potential Window for High‐Performance Supercapacitors

Molecular Tuning of the Vibrational Thermal Transport Mechanisms in Fullerene Derivative Solutions

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Singlet excited state (S1) of higher fullerenes C76 and C84: correlation between lifetime and HOMO–LUMO energy gap

Cited by 22 publications

References 31 publications

Intersystem Crossing Rates of Isolated Fullerenes: Theoretical Calculations

Intersystem Crossing Rates of Isolated Fullerenes: Theoretical Calculations

Fullerene C76: An Unexplored Superior Electrode Material with Wide Operating Potential Window for High‐Performance Supercapacitors

Molecular Tuning of the Vibrational Thermal Transport Mechanisms in Fullerene Derivative Solutions

Contact Info

Product

Resources

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Fullerene C₇₆: An Unexplored Superior Electrode Material with Wide Operating Potential Window for High‐Performance Supercapacitors