Laser initiated reactions in N2O clusters studied by time-sliced ion velocity imaging technique

Honma, Kenji

doi:10.1063/1.4816008

Cited by 4 publications

(3 citation statements)

References 36 publications

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“…Since N 2 O can be decomposed into O 2 and N 2 through thermocatalysis or under soft irradiation [18,19], atmospheric O 2 could be related to the level of N 2 O if the large-scale generation of N 2 O was possible on the early Earth. Moreover, some studies have also reported the decomposition of N 2 O into O 2 and N 2 from the perspective of photodissociation dynamics [20,21].…”

Section: Introductionmentioning

confidence: 99%

Photocatalysis: A Possible Vital Contributor to the Evolution of the Prebiotic Atmosphere and the Warming of the Early Earth

Cheng,

Xu,

Shi

et al. 2023

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The evolution of the early atmosphere was driven by changes in its chemical composition, which involved the formation of some critical gases. In this study, we demonstrate that nitrous oxide (N2O) can be produced from Miller’s early atmosphere (a mixture of CH4, NH3, H2, and H2O) by way of photocatalysis. Both NH3 and H2O were indispensable for the production of N2O by photocatalysis. Different conditions related to seawater and reaction temperature are also explored. N2O has a strong greenhouse gas effect, which is more able to warm the Earth than other gases and offers a reasonable explanation for the faint young Sun paradox on the early Earth. Moreover, the decomposition of N2O into N2 and O2 can be boosted by soft irradiation, providing a possible and important origin of atmospheric O2 and N2. The occurrence of O2 propelled the evolution of the atmosphere from being fundamentally reducing to oxidizing. This work describes a possible vital contribution of photocatalysis to the evolution of the early atmosphere.

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Section: Introductionmentioning

confidence: 99%

Photocatalysis: A Possible Vital Contributor to the Evolution of the Prebiotic Atmosphere and the Warming of the Early Earth

Cheng,

Xu,

Shi

et al. 2023

Catalysts

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“…In 1926, Leifson et al observed and identified the N 2 O absorption spectrum (150–230 nm) . Since then, tremendous efforts have been made in the photochemistry of N 2 O both experimentally − and theoretically. − While most studies focused on the N 2 O photodissociation in the ultraviolet (UV) region, interesting dynamical phenomena such as the oxygen atom product polarization were observed in the photolysis process, − much fewer work were carried out in the vacuum ultraviolet (VUV) region mainly due to the experimental difficulty in generating a VUV laser light.…”

Section: Introductionmentioning

confidence: 99%

Photodissociation Dynamics of Nitrous Oxide near 145 nm: The O(¹S₀) and O(³P_J=2,1,0) Product Channels

Yuan

Xie

et al. 2018

J. Phys. Chem. A

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We report the study of photodissociation dynamics of nitrous oxide in the vacuum ultraviolet region, using the time-sliced velocity map ion imaging technique. Ion images of the O(S) and O(P ) products were measured at nine photolysis wavelengths from 142.55 to 148.79 nm. The product channels O(S) + N(XΣ) and O(P ) + N(AΣ) have been observed. For these dissociation channels, the total kinetic energy releases of the dissociated products were acquired. With vibrational structures of the N coproducts partially resolved in the experimental images, the branching ratios of different vibrational states of the N coproducts were determined, and the vibrational state specific anisotropy parameters (β values) were derived. Analysis shows that the O(S) + N(XΣ) channel is primarily formed via nonadiabatic couplings between the C (Π) state and the higher-lying D (Σ) state of the NO. A moderate rotational excitation and high vibrational excitation of N(XΣ) products have been observed through this pathway. On the other hand, for the O(P ) + N(AΣ) channels, where a slightly higher rotational excitation of N coproducts have been observed, the possible pathway would be via nonadiabatic couplings from the C (Π) state to the lower-lying A(Σ)state.

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“…For example, the produced NO is one of the key molecules in destroying the stratospheric ozone that make N 2 O a very crucial molecule in the ozone depletion process. , Besides, N 2 O plays an important role in the global nitrogen cycle. Therefore, researchers have devoted much effort to the study of the photochemistry of N 2 O both experimentally − and theoretically. − …”

Section: Introductionmentioning

confidence: 99%

VUV Photodissociation Dynamics of Nitrous Oxide: The N(²D_J=3/2,5/2) and N(²P_J=1/2,3/2) Product Channels

Yuan¹,

Cheng³

et al. 2016

J. Phys. Chem. A

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We report on an experimental study of the vacuum ultraviolet photodissociation dynamics of nitrous oxide as a function of photolysis wavelength. In this study, both the N((2)DJ) + NO(X(2)Π) and N((2)PJ) + NO(X(2)Π) product channels were investigated using the time-sliced velocity ion imaging technique. Images of the N((2)DJ=5/2,3/2) and N((2)PJ=3/2,1/2) products were measured at seven and ten, respectively, photolysis wavelengths between 124.44 and 133.20 nm. The vibrational states of the NO products were partially resolved in the acquired raw ion images. The total kinetic energy release and the branching ratios of different vibrational states of NO products were determined. The vibrational state distributions of NO were found to be inverted for the N((2)DJ=5/2,3/2) and N((2)PJ=3/2,1/2) product channels. This phenomenon indicates that the N-O bond is highly vibrational excited during the breaking of the N-N bond. Vibrational state resolved anisotropic parameters β in both the N((2)DJ) and the N((2)PJ) channels were acquired. The small β values (around 0.5) in the dissociation process suggest that transition states in a bent configuration play an important role in the formation of N + NO products.

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Laser initiated reactions in N2O clusters studied by time-sliced ion velocity imaging technique

Cited by 4 publications

References 36 publications

Photocatalysis: A Possible Vital Contributor to the Evolution of the Prebiotic Atmosphere and the Warming of the Early Earth

Photocatalysis: A Possible Vital Contributor to the Evolution of the Prebiotic Atmosphere and the Warming of the Early Earth

Photodissociation Dynamics of Nitrous Oxide near 145 nm: The O(¹S₀) and O(³P_J=2,1,0) Product Channels

VUV Photodissociation Dynamics of Nitrous Oxide: The N(²D_J=3/2,5/2) and N(²P_J=1/2,3/2) Product Channels

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Laser initiated reactions in N2O clusters studied by time-sliced ion velocity imaging technique

Cited by 4 publications

References 36 publications

Photocatalysis: A Possible Vital Contributor to the Evolution of the Prebiotic Atmosphere and the Warming of the Early Earth

Photocatalysis: A Possible Vital Contributor to the Evolution of the Prebiotic Atmosphere and the Warming of the Early Earth

Photodissociation Dynamics of Nitrous Oxide near 145 nm: The O(1S0) and O(3PJ=2,1,0) Product Channels

VUV Photodissociation Dynamics of Nitrous Oxide: The N(2DJ=3/2,5/2) and N(2PJ=1/2,3/2) Product Channels

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Photodissociation Dynamics of Nitrous Oxide near 145 nm: The O(¹S₀) and O(³P_J=2,1,0) Product Channels

VUV Photodissociation Dynamics of Nitrous Oxide: The N(²D_J=3/2,5/2) and N(²P_J=1/2,3/2) Product Channels