Carl Johan Ballhausen (1926–2010)

Dahl, Jens Peder

doi:10.1007/430_2011_48

Cited by 1 publication

(1 citation statement)

References 31 publications

(18 reference statements)

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“…These approaches do not explicitly consider the crossover of two electronic levels along the reaction coordinates, and thus fail to describe the nonadiabatic charge transfer. Even though the methods that are based on Fermi's golden rule, such as the Marcus equation [40] and its derivatives [41][42][43][44][45], include the nonadiabatic effect, they must calculate the electronic coupling matrix either by estimating the minimum adiabatic energy splitting or constructing the diabatic states at the crossing region, such as with the Mulliken-Hush method [46,47], the fragment charge difference method [48,49] and bock diagonalization [50,51]. However, one must face the dilemma of using simpler Hartree-Fock methods with these algorithms, which misses the electron correlation effect on the electronic coupling matrix, and therefore they must be carefully applied to some specific system.…”

Section: Introductionmentioning

confidence: 99%

Adiabatic and nonadiabatic charge separation dynamics in graphene oxide quantum dots for overall water splitting

Cui

2018

Nanotechnology

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Chemical functionalization and heteroatom doping are two effective strategies for improving the conductivity of a graphene lattice. Nitrogen-doped graphene oxide quantum dot (GOQD) has been reported to possess both p- and n-conductivity that is induced by an oxygen functional group and nitrogen doping, respectively, and is suitable for catalyzing hydrogen and oxygen evolution reactions for complete water splitting. The experimental study shows that the hydrogen evolution reaction occurs considerably faster than the oxygen evolution reaction. However, the mechanism of this phenomenon remains unknown, which poses a challenge to the chemical modification of such classes of materials. In the present work, we perform nonadiabatic ab initio molecular dynamics to explore the charge separation dynamics in N-doped GOQD with oxygen functional groups. Our results show that there exists multiple charge decay channels governed by different mechanisms, which complicates the overall charge separation dynamics in N-doped GOQD. The intramolecular electron transfer mainly occurs through the nonadiabatic channel, whereas the intramolecular hole transfer mainly occurs through the adiabatic channel. There is an additional adiabatic decay channel in the p-domain, which accelerates electron–hole recombination in the p-domain. We further calculated the decoherence times and found that the decoherence of intramolecular electron transfer occurs considerably faster than that of hole transfer, which slows the quantum transition of intramolecular electron transfer. Finally, we simulated the carrier relaxation times and found that the electron relaxation is approximately one order of magnitude longer than that of the hole relaxation. Our calculation rationalizes the experimentally observed higher catalytic activity towards the hydrogen evolution compared to the oxygen evolution. More importantly, the calculation explains the fundamental roles of nitrogen doping and oxygen functional groups in the adiabatic and nonadiabatic charge decay mechanisms.

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Section: Introductionmentioning

confidence: 99%

Adiabatic and nonadiabatic charge separation dynamics in graphene oxide quantum dots for overall water splitting

Cui

2018

Nanotechnology

View full text Add to dashboard Cite

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Carl Johan Ballhausen (1926–2010)

Cited by 1 publication

References 31 publications

Adiabatic and nonadiabatic charge separation dynamics in graphene oxide quantum dots for overall water splitting

Adiabatic and nonadiabatic charge separation dynamics in graphene oxide quantum dots for overall water splitting

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