Direct imaging of the electronic dephasing in benzene: Experimental evidence for ultrafast intersystem crossing of<mml:math xmlns:mml="http://www.w3.org/1998/Math/MathML" display="inline"><mml:mrow><mml:msub><mml:mi>T</mml:mi><mml:mn>3</mml:mn></mml:msub><mml:mo>←</mml:mo><mml:msub><mml:mi>S</mml:mi><mml:mn>2</mml:mn></mml:msub></mml:mrow></mml:math>states

Qiu, Xuejun; Qin, Chaochao; Wang, Jian; Tang, Ying; Zhang, Fangfang

doi:10.1103/physreva.86.032505

Cited by 10 publications

(10 citation statements)

References 36 publications

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“…2, is close to the lifetime of the S 2 state for EB's analogues, e.g. benzene with 40-50 fs [7,11,12], toluene with ~65 fs [11,13] and o-xylene with 60 fs [24]. Moreover, it seems that the weak features above 0.53 eV follow the same trend as the strong bands I and II (Fig.…”

Section: Resultssupporting

confidence: 66%

“…Recently, Suzuki et al studied the ultrafast IC of benzene from the S 2 state, at which a time constant of 48 fs was determined from the decay profile of the total photoelectron intensity [11]. More recently, Qiu et al studied the S 2 state of benzene [12]. A longer-lived channel with 1.06 ps was observed and attributed to ISC from S 2 state to T 3 state.…”

Section: Introductionmentioning

confidence: 99%

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Real-time observation of ultrafast internal conversion in ethylbenzene by femtosecond time-resolved photoelectron imaging

Liu¹,

Gerber²,

Sych³

et al. 2013

Opt. Express

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The ultrafast dynamics of the second singlet electronically excited state (S₂) in ethylbenzene has been studied by femtosecond time-resolved photoelectron imaging. The time evolution of the photoelectron signal can be well described by a biexponential decay: a rapid relaxation pathway with a time constant of 60 ( ± 9) fs and a longer-lived channel on a timescale of 2.58 ( ± 0.22) ps. The rapid relaxation is ascribed to the ultrafast internal conversion from the S₂ state to the vibrationally hot S₁ state. This internal conversion process has been observed in real time. The slow photoelectron signal reflects the depopulation of secondarily populated high vibronic S₁ state.

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Section: Resultssupporting

confidence: 66%

Section: Introductionmentioning

confidence: 99%

Real-time observation of ultrafast internal conversion in ethylbenzene by femtosecond time-resolved photoelectron imaging

Liu¹,

Gerber²,

Sych³

et al. 2013

Opt. Express

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show abstract

“…The longer wavelength has been proved to be more sensitive to the "dark" state by Montero and coworkers [17].The comparisons of previous measurements, like in cyclohexene [18][19] and benzene [20][21], indicate that ionization by multi-photon ionization is more effective in probing secondary populated states. In this contribution, we reported single-color multi-photon ionization photoelectron image and two-color time-resolved photoelectron images (using multi-photon ionization for probing) as well as transient signal of the fragments.…”

Section: Introductionmentioning

confidence: 97%

Tracking ultrafast relaxation dynamics of furan by femtosecond photoelectron imaging

et al. 2015

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“…Qiu et al . also report observation of S 2 → T 3 ISC in benzene 67 while other studies assessing the S 2 deactivation of benzene do not report observations on the ISC pathway 65,66 …”

Section: Introductionmentioning

confidence: 98%

Distortion dependent intersystem crossing: A femtosecond time-resolved photoelectron spectroscopy study of benzene, toluene, and p-xylene

Stephansen¹,

Sølling²

2017

Structural Dynamics

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The competition between ultrafast intersystem crossing and internal conversion in benzene, toluene, and p-xylene is investigated with time-resolved photoelectron spectroscopy and quantum chemical calculations. By exciting to S2 out-of-plane symmetry breaking, distortions are activated at early times whereupon spin-forbidden intersystem crossing becomes (partly) allowed. Natural bond orbital analysis suggests that the pinnacle carbon atoms distorting from the aromatic plane change hybridization between the planar Franck-Condon geometry and the deformed (boat-shaped) S2 equilibrium geometry. The effect is observed to increase in the presence of methyl-groups on the pinnacle carbon-atoms, where largest extents of σ and π orbital-mixing are observed. This is fully consistent with the time-resolved spectroscopy data: Toluene and p-xylene show evidence for ultrafast triplet formation competing with internal conversion, while benzene appears to only decay via internal conversion within the singlet manifold. For toluene and p-xylene, internal conversion to S1 and intersystem crossing to T3 occur within the time-resolution of our instrument. The receiver triplet state (T3) is found to undergo internal conversion in the triplet manifold within ≈100–150 fs (toluene) or ≈180–200 fs (p-xylene) as demonstrated by matching rise and decay components of upper and lower triplet states. Overall, the effect of methylation is found to both increase the intersystem crossing probability and direct the molecular axis of the excited state dynamics.

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Direct imaging of the electronic dephasing in benzene: Experimental evidence for ultrafast intersystem crossing ofT3←S2states

Cited by 10 publications

References 36 publications

Real-time observation of ultrafast internal conversion in ethylbenzene by femtosecond time-resolved photoelectron imaging

Real-time observation of ultrafast internal conversion in ethylbenzene by femtosecond time-resolved photoelectron imaging

Tracking ultrafast relaxation dynamics of furan by femtosecond photoelectron imaging

Distortion dependent intersystem crossing: A femtosecond time-resolved photoelectron spectroscopy study of benzene, toluene, and p-xylene

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