Large-scale correlated calculations of linear optical absorption and low-lying excited states of polyacenes: Pariser-Parr-Pople Hamiltonian

Sony, Priya; Shukla, Alok

doi:10.1103/physrevb.75.155208

Cited by 76 publications

(102 citation statements)

References 93 publications

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“…Es gibt theoretische Unterstützung für das Auftreten eines zusätzlichen, relativ intensiven Signals bei größeren Wellenlängen als denen der b-Bande von Heptacen. [27] Weitere experimentelle und theoretische Untersuchungen der höheren Acene sind höchst wünschenswert.…”

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Photochemische Erzeugung von Octacen und Nonacen

Tönshoff

Bettinger

2010

Angewandte Chemie

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Photochemische Erzeugung von Octacen und Nonacen

Tönshoff

Bettinger

2010

Angewandte Chemie

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“…Unfortunately, the large system size of higher acenes hinders the use of many accurate but expensive theoretical tools. Empirical or semiempirical studies (42)(43)(44)(45)(46)(47) are inexpensive but also less accurate, and therefore seem to be less widely accepted. One of the most acknowledged theoretical predictions, up to now, is based on the unrestricted density-functional theory (UDFT) calculation performed more than 10 y ago (48).…”

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confidence: 99%

Nature of ground and electronic excited states of higher acenes

Yang

Davidson

Yang

2016

Proc. Natl. Acad. Sci. U.S.A.

174

208

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Higher acenes have drawn much attention as promising organic semiconductors with versatile electronic properties. However, the nature of their ground state and electronic excited states is still not fully clear. Their unusual chemical reactivity and instability are the main obstacles for experimental studies, and the potentially prominent diradical character, which might require a multireference description in such large systems, hinders theoretical investigations. Here, we provide a detailed answer with the particleparticle random-phase approximation calculation. The 1 A g ground states of acenes up to decacene are on the closed-shell side of the diradical continuum, whereas the ground state of undecacene and dodecacene tilts more to the open-shell side with a growing polyradical character. The ground state of all acenes has covalent nature with respect to both short and long axes. The lowest triplet state 3 B 2u is always above the singlet ground state even though the energy gap could be vanishingly small in the polyacene limit. The bright singlet excited state 1 B 2u is a zwitterionic state to the short axis. The excited 1 A g state gradually switches from a doubleexcitation state to another zwitterionic state to the short axis, but always keeps its covalent nature to the long axis. An energy crossing between the 1 B 2u and excited 1 A g states happens between hexacene and heptacene. Further energetic consideration suggests that higher acenes are likely to undergo singlet fission with a low photovoltaic efficiency; however, the efficiency might be improved if a singlet fission into multiple triplets could be achieved.higher acenes | diradical | double excitation | particle-particle random-phase approximation | charge-transfer excitation

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“…25,26 On the other hand, corresponding destructive interference results in the reduction of the transition dipoles producing dark states as shown in Fig.1(a). Fig.1(b) shows the positively interfering coherent peak (β ), negatively interfering destructive peak (α) and edge state contributing peaks of 7 ring containing acene GQD with 30 carbon atoms.…”

Section: Resultsmentioning

confidence: 99%

“…23,24 Now the coherent control of excitonic states, over the optical transition is dictated by the linear superposition of quantum states with symmetric or anti-symmetric phase matching resulting either addition or reduction of electrical transition dipole. 25,26 The dipole dipole interaction modulates the charge density wave and spin density wave phases, which can modify the optical response in significant way. We have investigated here how the architecture of the boron nitrogen substitution in GQD can govern the Davydov type splitting 27,28 resulting in a coherent control of the excitonic states.…”

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confidence: 99%

Tuning the Optically Bright and Dark States of Doped Graphene Quantum Dots

2016

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Employing a combination of many-body configuration interaction method described by extended Hubbard model along with first principle calculations we predict the emergence of high oscillator strength at near-IR region which originates from the Davydov type of splitting in doped graphene quantum dots (GQD). Incorporation of strain in GQD promotes closely spaced bright states inciting for coherent excitation. Controlling the destructive interference of

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Large-scale correlated calculations of linear optical absorption and low-lying excited states of polyacenes: Pariser-Parr-Pople Hamiltonian

Cited by 76 publications

References 93 publications

Photochemische Erzeugung von Octacen und Nonacen

Photochemische Erzeugung von Octacen und Nonacen

Nature of ground and electronic excited states of higher acenes

Tuning the Optically Bright and Dark States of Doped Graphene Quantum Dots

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