Excitation Energy-Dependent Decay Dynamics of the S<sub>1</sub> State of <i>N</i>-Methyl-2-pyridone

Feng, Baihui; Yang, Dongyuan; He, Zhigang; Fang, Benjie; Wu, Guorong; Yang, Xueming

doi:10.1021/acs.jpca.3c05745

Cited by 3 publications

(10 citation statements)

References 39 publications

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“…Herein, the time constant of 1.6 ± 0.2 ps is assigned to the lifetime of the S 1 (1 1 ππ*) state with high vibrational excitation (∼1.04 eV above the S 1 origin). For the pump wavelength of 261.5 nm, the value of 1.6 ± 0.2 ps is consistent with the pump wavelength-dependent lifetimes of the S 1 vibrational states derived from the previous [1 + 1′] TRPES data . The component of IRF may include different originations associated with two-color [1 + 2′] three-photon ionization processes around the time-zero .…”

Section: Resultssupporting

confidence: 88%

“…The femtosecond time-resolved photoelectron imaging (fs-TRPEI) experiment was carried out on a velocity map imaging (VMI) spectrometer . Detailed experimental methods have been given in the previous publications of our recent studies on 2-pyridone and NMP . Therefore, only the key features are mentioned here.…”

Section: Methodsmentioning

confidence: 99%

“…Among these N-containing heterocyclic molecules, 2-pyridone (strictly called 2( 1H )-pyridone) is one of the simplest six-membered nucleobase analogues, the response of which to UV radiation might be associated with the selection of the important building blocks of life on the early earth . In a recent paper ( J. Phys. Chem.…”

Section: Introductionmentioning

confidence: 99%

“…Although there is a keto–enol tautomerization reaction for the parent molecule under our molecular beam conditions, , methylation of the N position of 2-pyridone removes the possibility of other tautomer and“locks” the pyridone into a keto form. Therefore, in the case of NMP, the excitation energy-dependent decay dynamics can be successfully investigated using the [1 + 1′] femtosecond time-resolved photoelectron spectroscopy (TRPES) method . A clear vibrational-state-dependent lifetime of the S 1 state, which is in the range of several picoseconds to a few nanoseconds, has been revealed by our direct pump–probe measurements.…”

Section: Introductionmentioning

confidence: 99%

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Ultrafast Decay Dynamics of the 2¹ππ* Electronic State of N-Methyl-2-pyridone

Feng,

Wu,

et al. 2024

J. Phys. Chem. A

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The ultrafast decay dynamics of N-methyl-2-pyridone upon excitation in the near-ultraviolet range of 261.5−227.9 nm is investigated using the femtosecond timeresolved photoelectron spectroscopy method. Irradiation at 261.5 nm prepares N-methyl-2-pyridone molecules with high vibrational levels in the 1 1 ππ* state. The radiation-less decay to the ground state via internal conversion is suggested to be the dominant channel for the 1 1 ππ* state with large vibrational excess energy, which is revealed by a lifetime of 1.6 ± 0.2 ps. As the pump wavelength decreases, we found that irradiation at 238.5 and 227.9 nm results in the population of the 2 1 ππ* state. This is in agreement with the assignment of the vapor-phase UV absorption bands of N-methyl-2-pyridone. On the basis of the detailed analysis of our measured time-resolved photoelectron spectra at all pump wavelengths, we conclude that the 2 1 ππ* state has an ultrashort lifetime of 50 ± 10 fs. In addition, the S 1 (1 1 ππ*) state is subsequently populated via internal conversion and decays over a lifetime of 680−620 fs. The most probable whole deactivation pathway of the 2 1 ππ* state is discussed. This experimental study provides new insights into the excitation energy-dependent decay dynamics of electronically excited N-methyl-2-pyridone.

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Section: Resultssupporting

confidence: 88%

Section: Methodsmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

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Ultrafast Decay Dynamics of the 2¹ππ* Electronic State of N-Methyl-2-pyridone

Feng,

Wu,

et al. 2024

J. Phys. Chem. A

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“…The fs-TRPEI experiment was carried out on a velocity map imaging (VMI) spectrometer 38 and the experimental methods have been described in our earlier publications. 39–42 Here, only a brief description of the key features will be given. A solid sample of PyNO was purchased commercially with a purity of ≥97% and used directly without further purification.…”

Section: Methodsmentioning

confidence: 99%

Insights into ultrafast decay dynamics of electronically excited pyridine-N-oxide

Feng,

Wu,

Yang

et al. 2024

Phys. Chem. Chem. Phys.

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Insights into Ultrafast Relaxation Dynamics of Electronically Excited Furfural and 5-Methylfurfural

Wu,

Feng,

Tian

et al. 2024

J. Phys. Chem. A

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The ultrafast relaxation dynamics of furfural and 5methylfurfural following excitation in the ultraviolet range is investigated using the femtosecond time-resolved photoelectron spectroscopy method. Specifically, the pump wavelength-dependent decay dynamics of electronically excited furfural and 5-methylfurfural is discussed on the basis of a detailed analysis of our measured time-resolved photoelectron spectroscopy spectra. Irradiation at all pump wavelengths prepares both furfural and 5methylfurfural molecules with different vibrational levels in the first optically bright S 2 ( 1 ππ*) state, the lifetime of which is measured to be at least hundreds of femtoseconds. Besides the prominent deactivation channels of ring-opening and ring-puckering pathways for the S 2 ( 1 ππ*) state, we propose that there is a minor decay channel of internal conversion from the initially prepared S 2 ( 1 ππ*) state to the S 1 ( 1 nπ*) state. The wavepacket decays out of the Franck−Condon region on the S 2 ( 1 ππ*) state potential energy surface and bifurcates into different parts somewhere. A small fraction of the wavepacket funnels down to the S 1 ( 1 nπ*) state via internal conversion. The subsequently populated S 1 ( 1 nπ*) state contains large vibrational excess energy and decays over a lifetime of 2.5−2.8 ps. One of the deactivation channels of the S 1 ( 1 nπ*) state is intersystem crossing to the 3 ππ* triplet state. In addition, methyl substitution effects on the excitedstate dynamics of furfural are also discussed. This experimental study provides new insights into the excitation energy-dependent decay dynamics of photoexcited furfural and 5-methylfurfural.

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Excitation Energy-Dependent Decay Dynamics of the S₁ State of N-Methyl-2-pyridone

Cited by 3 publications

References 39 publications

Ultrafast Decay Dynamics of the 2¹ππ* Electronic State of N-Methyl-2-pyridone

Ultrafast Decay Dynamics of the 2¹ππ* Electronic State of N-Methyl-2-pyridone

Insights into ultrafast decay dynamics of electronically excited pyridine-N-oxide

Insights into Ultrafast Relaxation Dynamics of Electronically Excited Furfural and 5-Methylfurfural

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Excitation Energy-Dependent Decay Dynamics of the S1 State of N-Methyl-2-pyridone

Cited by 3 publications

References 39 publications

Ultrafast Decay Dynamics of the 21ππ* Electronic State of N-Methyl-2-pyridone

Ultrafast Decay Dynamics of the 21ππ* Electronic State of N-Methyl-2-pyridone

Insights into ultrafast decay dynamics of electronically excited pyridine-N-oxide

Insights into Ultrafast Relaxation Dynamics of Electronically Excited Furfural and 5-Methylfurfural

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Product

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Excitation Energy-Dependent Decay Dynamics of the S₁ State of N-Methyl-2-pyridone

Ultrafast Decay Dynamics of the 2¹ππ* Electronic State of N-Methyl-2-pyridone

Ultrafast Decay Dynamics of the 2¹ππ* Electronic State of N-Methyl-2-pyridone