Vacuum ultraviolet excited state dynamics of small amides

Martin A.B. Larsen; Theis I. Sølling; Ruaridh Forbes; Andrey E. Boguslavskiy; Varun Makhija; Kévin Veyrinas; Rune Lausten; Albert Stolow; Magdalena M. Zawadzki; Lisa Saalbach; Nikoleta Kotsina; Martin J. Paterson; Dave Townsend

doi:10.1063/1.5079721

Vacuum ultraviolet excited state dynamics of small amides

Martin A.B. Larsen, Theis I. Sølling, Ruaridh Forbes, Andrey E. Boguslavskiy, Varun Makhija, Kévin Veyrinas, Rune Lausten, Albert Stolow, Magdalena M. Zawadzki, Lisa Saalbach, Nikoleta Kotsina, Martin J. Paterson, Dave Townsend

Kemisk Institut

2 Citationer (Scopus)

Abstract

Time-resolved photoelectron spectroscopy in combination with ab initio quantum chemistry calculations was used to study ultrafast excited state dynamics in formamide (FOR), N,N-dimethylformamide (DMF), and N,N-dimethylacetamide (DMA) following 160 nm excitation. The particular focus was on internal conversion processes within the excited state Rydberg manifold and on how this behavior in amides compared with previous observations in small amines. All three amides exhibited extremely rapid (<100 fs) evolution from the Franck-Condon region. We argue that this is then followed by dissociation. Our calculations indicate subtle differences in how the excited state dynamics are mediated in DMA/DMF as compared to FOR. We suggest that future studies employing longer pump laser wavelengths will be useful for discerning these differences.

Originalsprog	Engelsk
Artikelnummer	054301
Tidsskrift	Journal of Chemical Physics
Vol/bind	150
Udgave nummer	5
Antal sider	12
ISSN	0021-9606
DOI	https://doi.org/10.1063/1.5079721
Status	Udgivet - 2019

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10.1063/1.5079721

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title = "Vacuum ultraviolet excited state dynamics of small amides",

abstract = "Time-resolved photoelectron spectroscopy in combination with ab initio quantum chemistry calculations was used to study ultrafast excited state dynamics in formamide (FOR), N,N-dimethylformamide (DMF), and N,N-dimethylacetamide (DMA) following 160 nm excitation. The particular focus was on internal conversion processes within the excited state Rydberg manifold and on how this behavior in amides compared with previous observations in small amines. All three amides exhibited extremely rapid (<100 fs) evolution from the Franck-Condon region. We argue that this is then followed by dissociation. Our calculations indicate subtle differences in how the excited state dynamics are mediated in DMA/DMF as compared to FOR. We suggest that future studies employing longer pump laser wavelengths will be useful for discerning these differences.",

author = "Larsen, {Martin A.B.} and S{\o}lling, {Theis I.} and Ruaridh Forbes and Boguslavskiy, {Andrey E.} and Varun Makhija and K{\'e}vin Veyrinas and Rune Lausten and Albert Stolow and Zawadzki, {Magdalena M.} and Lisa Saalbach and Nikoleta Kotsina and Paterson, {Martin J.} and Dave Townsend",

year = "2019",

doi = "10.1063/1.5079721",

language = "English",

volume = "150",

journal = "The Journal of Chemical Physics",

issn = "0021-9606",

publisher = "American Institute of Physics",

number = "5",

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TY - JOUR

T1 - Vacuum ultraviolet excited state dynamics of small amides

AU - Larsen, Martin A.B.

AU - Sølling, Theis I.

AU - Forbes, Ruaridh

AU - Boguslavskiy, Andrey E.

AU - Makhija, Varun

AU - Veyrinas, Kévin

AU - Lausten, Rune

AU - Stolow, Albert

AU - Zawadzki, Magdalena M.

AU - Saalbach, Lisa

AU - Kotsina, Nikoleta

AU - Paterson, Martin J.

AU - Townsend, Dave

PY - 2019

Y1 - 2019

N2 - Time-resolved photoelectron spectroscopy in combination with ab initio quantum chemistry calculations was used to study ultrafast excited state dynamics in formamide (FOR), N,N-dimethylformamide (DMF), and N,N-dimethylacetamide (DMA) following 160 nm excitation. The particular focus was on internal conversion processes within the excited state Rydberg manifold and on how this behavior in amides compared with previous observations in small amines. All three amides exhibited extremely rapid (<100 fs) evolution from the Franck-Condon region. We argue that this is then followed by dissociation. Our calculations indicate subtle differences in how the excited state dynamics are mediated in DMA/DMF as compared to FOR. We suggest that future studies employing longer pump laser wavelengths will be useful for discerning these differences.

AB - Time-resolved photoelectron spectroscopy in combination with ab initio quantum chemistry calculations was used to study ultrafast excited state dynamics in formamide (FOR), N,N-dimethylformamide (DMF), and N,N-dimethylacetamide (DMA) following 160 nm excitation. The particular focus was on internal conversion processes within the excited state Rydberg manifold and on how this behavior in amides compared with previous observations in small amines. All three amides exhibited extremely rapid (<100 fs) evolution from the Franck-Condon region. We argue that this is then followed by dissociation. Our calculations indicate subtle differences in how the excited state dynamics are mediated in DMA/DMF as compared to FOR. We suggest that future studies employing longer pump laser wavelengths will be useful for discerning these differences.

U2 - 10.1063/1.5079721

DO - 10.1063/1.5079721

M3 - Journal article

C2 - 30736696

AN - SCOPUS:85061237914

SN - 0021-9606

VL - 150

JO - The Journal of Chemical Physics

JF - The Journal of Chemical Physics

IS - 5

M1 - 054301

ER -

Vacuum ultraviolet excited state dynamics of small amides

Abstract

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