Time-resolved high-harmonic spectroscopy of the photodissociation of CH3I and CF3I
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The photodissociation dynamics of iodomethane (CH3I) and trifluoroiodomethane (CF3I) have been studied using time-resolved high-harmonic spectroscopy. The molecules were photoexcited in a transient grating geometry to their respective A bands by laser pulses centred at 267 nm and were probed through high-harmonic generation driven by a delayed 800 nm laser pulse. Both molecules display a fast buildup of the diffracted high harmonics (H9–H15) followed by a slower decay, while the undiffracted harmonics exhibit an opposite modulation. The time scales on which the signals reach their asymptotic values were found to be slower in CF3I compared to CH3I and to weakly increase with high-harmonic order in both molecules. In the case of CH3I the obtained time scales are in agreement with dissociation times measured by other techniques. Our results on CF3I constitute the first time-resolved measurements of the A-band dissociation. A simple theoretical model for the variation of the harmonic phase induced by the changing vertical ionisation potential is combined with one-dimensional nuclear wave-packet propagation and shown to qualitatively account for the main observations.
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Many experiments use the HHG field itself as the signal; such signals are robust but harder to interpret than a pump-probe because the spectroscopic information is convoluted with the HHG multistep mechanism.
“Many experiments use the HHG field itself as the signal [41].Such signals are robust but harder to interpret than, e.g., a pumpprobe, since the spectroscopic information is convoluted with the HHG multistep mechanism.”
From Roadmap of ultrafast x-ray atomic and molecular physics (2018) · cites this paper as [41]
Tunable, intense attosecond x-ray pulses can probe ultrafast processes such as intersystem crossing and radiationless decay and reveal the nature of elementary photophysical and photochemical events.
“Tunable, intense attosecond x-ray pulses can probe such ultrafast processes and reveal the nature of elementary photophysical and photochemical events [41].”
From Roadmap of ultrafast x-ray atomic and molecular physics (2018) · cites this paper as [41]
Cites
Principles of Nonlinear Optical Spectroscopy
Mukamel, S. (1995) · Cited by 4,566 · see citing works
Theory of high-harmonic generation by low-frequency laser fields
Lewenstein, M., Balcou, P., Ivanov, M., L’Huillier, A., & Corkum, P. B. (1994) · Physical Review A · doi:10.1103/physreva.49.2117 · Cited by 4,158 · see citing works
Tomographic imaging of molecular orbitals
Itatani, J., Levesque, J., Zeidler, D., Niikura, H., Pépin, H., Kieffer, J. C., Corkum, P. B., & Villeneuve, D. M. (2004) · Nature · doi:10.1038/nature03183 · Cited by 2,318 · see citing works
Time-resolved atomic inner-shell spectroscopy
Drescher, M., Hentschel, M., Kienberger, R., Uiberacker, M., Yakovlev, V., Scrinzi, A., Westerwalbesloh, T., Kleineberg, U., Heinzmann, U., & Krausz, F. (2002) · Nature · doi:10.1038/nature01143 · Cited by 1,470 · see citing works
Laser-Induced Dynamic Gratings
Eichler, H. J., Günter, P., & Pohl, D. (1986) · Springer series in optical sciences/SPringer series in optical sciences · doi:10.1007/978-3-540-39662-8 · Cited by 1,388 · see citing works
Introduction to Quantum Mechanics: A Time-Dependent Perspective
Tannor, D. J. (2006) · Cited by 1,027 · see citing works
Quantum interference during high-order harmonic generation from aligned molecules
Kanai, T., Minemoto, S., & Sakai, H. (2005) · Nature · doi:10.1038/nature03577 · Cited by 757 · see citing works
Electron localization following attosecond molecular photoionization
Sansone, G., Kelkensberg, F., Pérez-Torres, J. F., Morales, F., Kling, M. F., Siu, W., Ghafur, O., Johnsson, P., Swoboda, M., Benedetti, E., et al. (2010) · Nature · doi:10.1038/nature09084 · Cited by 736 · see citing works
Generalized molecular orbital tomography
Vozzi, C., Negro, M., Calegari, F., Sansone, G., Nisoli, M., Silvestri, S. D., & Stagira, S. (2011) · Nature Physics · doi:10.1038/nphys2029 · Cited by 465 · see citing works
Following a chemical reaction using high-harmonic interferometry
Wörner, H. J., Bertrand, J. B., Kartashov, D. V., Corkum, P. B., & Villeneuve, D. M. (2010) · Nature · doi:10.1038/nature09185 · Cited by 455 · see citing works
Self-citationTime-Resolved Dynamics in N 2 O 4 Probed Using High Harmonic Generation
Li, W., Zhou, X., Lock, R. M., Patchkovskii, S., Stolow, A., Kapteyn, H. C., & Murnane, M. M. (2008) · Science · doi:10.1126/science.1163077 · Cited by 351 · see citing works
Mulliken, R. S. (1940) · The Journal of Chemical Physics · doi:10.1063/1.1750671 · Cited by 279 · see citing works
Conical Intersection Dynamics in NO 2 Probed by Homodyne High-Harmonic Spectroscopy
Wörner, H. J., Bertrand, J. B., Fabre, B., Higuet, J., Ruf, H., Dubrouil, A., Patchkovskii, S., Spanner, M., Mairesse, Y., Blanchet, V., et al. (2011) · Science · doi:10.1126/science.1208664 · Cited by 260 · see citing works
Self-citationATOMIC IODINE PHOTODISSOCIATION LASER
KASPER, J. V. V., & Pimentel, G. C. (1964) · Applied Physics Letters · doi:10.1063/1.1723603 · Cited by 259 · see citing works
Dynamics of Molecules in Condensed Phases: Picosecond Holographic Grating Experiments
Fayer, M. D. (1982) · Annual Review of Physical Chemistry · doi:10.1146/annurev.pc.33.100182.000431 · Cited by 231 · see citing works
Methyl iodide A-band decomposition study by photofragment velocity imaging
Eppink, A. T. J. B., & Parker, D. H. (1998) · The Journal of Chemical Physics · doi:10.1063/1.477087 · Cited by 212 · see citing works
Eppink, A. T. J. B., & Parker, D. H. (1999) · The Journal of Chemical Physics · doi:10.1063/1.478051 · Cited by 201 · see citing works
Monitoring molecular dynamics using coherent electrons from high harmonic generation
Wagner, N. L., Wüest, A., Christov, I. P., Popmintchev, T., Zhou, X., Murnane, M. M., & Kapteyn, H. C. (2006) · Proceedings of the National Academy of Sciences · doi:10.1073/pnas.0605178103 · Cited by 197 · see citing works
Patchkovskii, S., Zhao, Z., Brabec, T., & Villeneuve, D. M. (2006) · Physical Review Letters · doi:10.1103/physrevlett.97.123003 · Cited by 191 · see citing works
Principles of nonlinear optical spectroscopy
Letokhov, V. S. (1998) · Uspekhi Fizicheskih Nauk · doi:10.3367/ufnr.0168.199805j.0591 · Cited by 187 · see citing works
Theory of tunneling ionization of molecules: Weak-field asymptotics including dipole effects
Tolstikhin, O. I., Morishita, T., & Madsen, L. B. (2011) · Physical Review A · doi:10.1103/physreva.84.053423 · Cited by 182 · see citing works
Ultrafast Time-Resolved Soft X-Ray Photoelectron Spectroscopy of Dissociating Br2
Nugent-Glandorf, L., Scheer, M., Samuels, D. A., Mulhisen, A. M., Grant, E. R., Yang, X., Bierbaum, V. M., & Leone, S. R. (2001) · Physical Review Letters · doi:10.1103/physrevlett.87.193002 · Cited by 175 · see citing works
Molecular Recollision Interferometry in High Harmonic Generation
Zhou, X., Lock, R. M., Li, W., Wagner, N., Murnane, M. M., & Kapteyn, H. C. (2008) · Physical Review Letters · doi:10.1103/physrevlett.100.073902 · Cited by 164 · see citing works
Coherent Electron Scattering Captured by an Attosecond Quantum Stroboscope
Mauritsson, J., Johnsson, P., Mansten, E., Swoboda, M., Ruchon, T., L’Huillier, A., & Schäfer, K. J. (2008) · Physical Review Letters · doi:10.1103/physrevlett.100.073003 · Cited by 147 · see citing works
Ultrahigh-Order Wave Mixing in Noncollinear High Harmonic Generation
Bertrand, J. B., Wörner, H. J., Bandulet, H. C., et al. (2011) · Physical Review Letters · doi:10.1103/physrevlett.106.023001 · Cited by 145 · see citing works
Self-citationZhong, D., & Zewail, A. H. (1998) · The Journal of Physical Chemistry A · doi:10.1021/jp9805196 · Cited by 142 · see citing works
One-electron ionization of multielectron systems in strong nonresonant laser fields
Spanner, M., & Patchkovskii, S. (2009) · Physical Review A · doi:10.1103/physreva.80.063411 · Cited by 135 · see citing works
High-Harmonic Spectroscopy of Oriented OCS Molecules: Emission of Even and Odd Harmonics
Kraus, P. M., Rupenyan, A., & Wörner, H. J. (2012) · Physical Review Letters · doi:10.1103/physrevlett.109.233903 · Cited by 131 · see citing works
Self-citationDestructive Interference during High Harmonic Generation in Mixed Gases
Kanai, T., Takahashi, E. J., Nabekawa, Y., & Midorikawa, K. (2007) · Physical Review Letters · doi:10.1103/physrevlett.98.153904 · Cited by 119 · see citing works
An ab initio study of the CH3I photodissociation. I. Potential energy surfaces
Alekseyev, A. B., Liebermann, H., Buenker, R. J., et al. (2007) · The Journal of Chemical Physics · doi:10.1063/1.2736695 · Cited by 117 · see citing works
A detailed experimental and theoretical study of the femtosecond A-band photodissociation of CH3I
de Nalda, R., Durá, J., García-Vela, A., et al. (2008) · The Journal of Chemical Physics · doi:10.1063/1.2943198 · Cited by 105 · see citing works
Tunnel Ionization of Molecules and Orbital Imaging
Murray, R., Spanner, M., Patchkovskii, S., et al. (2011) · Physical Review Letters · doi:10.1103/physrevlett.106.173001 · Cited by 104 · see citing works
Time-dependent analytical R -matrix approach for strong-field dynamics. II. Many-electron systems
Torlina, L., Ivanov, M., Walters, Z. B., & Smirnova, O. V. (2012) · Physical Review A · doi:10.1103/physreva.86.043409 · Cited by 100 · see citing works
Alignment of symmetric top molecules by short laser pulses
Hamilton, E. L., Seideman, T., Ejdrup, T., Poulsen, M. D., Bisgaard, C. Z., Viftrup, S. S., & Stapelfeldt, H. (2005) · Physical Review A · doi:10.1103/physreva.72.043402 · Cited by 93 · see citing works
Madsen, L. B., Tolstikhin, O. I., & Morishita, T. (2012) · Physical Review A · doi:10.1103/physreva.85.053404 · Cited by 90 · see citing works
Walter, K., Weinkauf, R., Boesl, U., et al. (1988) · The Journal of Chemical Physics · doi:10.1063/1.455088 · Cited by 78 · see citing works
Quantum interference and multielectron effects in high-harmonic spectra of polar molecules
Rupenyan, A., Kraus, P. M., Schneider, J. M., et al. (2013) · Physical Review A · doi:10.1103/physreva.87.031401 · Cited by 70 · see citing works
Real-Time Evolution of the Valence Electronic Structure in a Dissociating Molecule
Wernet, P., Odelius, M., Godehusen, K., et al. (2009) · Physical Review Letters · doi:10.1103/physrevlett.103.013001 · Cited by 67 · see citing works
High-Order Harmonic Transient Grating Spectroscopy in a Molecular Jet
Mairesse, Y., Zeidler, D., Dudovich, N., Spanner, M., Levesque, J., Villeneuve, D. M., & Corkum, P. B. (2008) · Physical Review Letters · doi:10.1103/physrevlett.100.143903 · Cited by 63 · see citing works
Roeterdink, W. G., & Janssen, M. H. M. (2002) · Physical Chemistry Chemical Physics · doi:10.1039/b107897f · Cited by 61 · see citing works
Photodissociation of CF3I at 248 nm: Kinetic energy dependence of the recoil anisotropy
Felder, P. (1991) · Chemical Physics · doi:10.1016/0301-0104(91)80119-3 · Cited by 52 · see citing works
Photoacoustic measurements of photofragmentation in CH3I
Hunter, T. F., & Kristjansson, K. S. (1978) · Chemical Physics Letters · doi:10.1016/0009-2614(78)80296-6 · Cited by 52 · see citing works
All-Optical Measurement of High-Harmonic Amplitudes and Phases in Aligned Molecules
Rupenyan, A., Bertrand, J. B., Villeneuve, D. M., et al. (2012) · Physical Review Letters · doi:10.1103/physrevlett.108.033903 · Cited by 52 · see citing works
Song, Y., Qian, X., Lau, K., et al. (2001) · The Journal of Chemical Physics · doi:10.1063/1.1391268 · Cited by 48 · see citing works
Furlan, A., Gejo, T., & Huber, J. R. (1996) · The Journal of Physical Chemistry · doi:10.1021/jp953130g · Cited by 48 · see citing works
State-selective photofragment imaging of iodine atoms via photodissociation of CF3I at 277 nm
Kim, Y. S., Kang, W. K., & Jung, K. (1996) · The Journal of Chemical Physics · doi:10.1063/1.471908 · Cited by 43 · see citing works
Time-resolved high-harmonic spectroscopy of nonadiabatic dynamics in NO 2
Kraus, P. M., Arasaki, Y., Bertrand, J. B., Patchkovskii, S., Corkum, P. B., Villeneuve, D. M., Takatsuka, K., & Wörner, H. J. (2012) · Physical Review A · doi:10.1103/physreva.85.043409 · Cited by 42 · see citing works
Self-citationImaging transient species in the femtosecond A-band photodissociation of CH3I
Durá, J., de Nalda, R., Amaral, G. A., et al. (2009) · The Journal of Chemical Physics · doi:10.1063/1.3236808 · Cited by 40 · see citing works
High-Harmonic Homodyne Detection of the Ultrafast Dissociation of Br2 Molecules
Wörner, H. J., Bertrand, J. B., Corkum, P. B., & Villeneuve, D. M. (2010) · Physical Review Letters · doi:10.1103/physrevlett.105.103002 · Cited by 40 · see citing works
Self-citationPhotodissociation of CH3I: A Full-Dimensional (9D) Quantum Dynamics Study
Evenhuis, C. R., & Manthe, U. (2011) · The Journal of Physical Chemistry A · doi:10.1021/jp1103998 · Cited by 39 · see citing works
Le, A.-T., Morishita, T., Lucchese, R. R., et al. (2012) · Physical Review Letters · doi:10.1103/physrevlett.109.203004 · Cited by 36 · see citing works
Urban, B., & Bondybey, V. E. (2002) · The Journal of Chemical Physics · doi:10.1063/1.1447219 · Cited by 35 · see citing works
Ab initioconfiguration interaction study of theB- andC-band photodissociation of methyl iodide
Alekseyev, A. B., Liebermann, H., & Buenker, R. J. (2011) · The Journal of Chemical Physics · doi:10.1063/1.3532926 · Cited by 31 · see citing works
Velocity map imaging of femtosecond photodynamics in CF3I
Roeterdink, W. G., & Janssen, M. H. M. (2001) · Chemical Physics Letters · doi:10.1016/s0009-2614(01)00865-x · Cited by 28 · see citing works
He, Y., Qüack, M., Ranz, R., et al. (1993) · Chemical Physics Letters · doi:10.1016/0009-2614(93)89293-q · Cited by 24 · see citing works
Time-resolved high-harmonic spectroscopy of valence electron dynamics
Kraus, P. M., & Wörner, H. J. (2012) · Chemical Physics · doi:10.1016/j.chemphys.2012.01.013 · Cited by 20 · see citing works
Self-citationGrütter, M., Michaud, J. M., & Merkt, F. (2011) · The Journal of Chemical Physics · doi:10.1063/1.3547548 · Cited by 19 · see citing works
Bae, Y. J., & Kim, M. S. (2008) · ChemPhysChem · doi:10.1002/cphc.200800207 · Cited by 17 · see citing works
Krylov, V. N., Nikitchenko, M., Qüack, M., et al. (2004) · Proceedings of SPIE, the International Society for Optical Engineering/Proceedings of SPIE · doi:10.1117/12.530069 · Cited by 7 · see citing works
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Roadmap of ultrafast x-ray atomic and molecular physics
Young, L., Ueda, K., Gühr, M., Bucksbaum, P. H., Simon, M., Mukamel, S., Rohringer, N., Prince, K. C., Masciovecchio, C., Meyer, M., et al. (2018) · Journal of Physics B: Atomic, Molecular and Optical Physics · doi:10.1088/1361-6455/aa9735 · Cited by 337 · see citing works
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- Authors
- Tehlar, A., & Wörner, H. J.
- Affiliations
- ETH Zurich (CH)
- Venue
- Molecular Physics
- Publisher
- Informa UK Limited
- Published
- 2013-04-14
- Volume
- 111
- Issue
- 14-15
- Pages
- 2057-2067
- ISSN
- 0026-8976 (ISSN-L)
- 1362-3028
- OpenAlex
- W2035997712
- Cited by
- 23
- References
- 59
- Citations by year
- 2025: 1 · 2024: 1 · 2021: 2 · 2020: 1 · 2019: 3 · 2018: 6 · 2017: 4 · 2016: 1 · 2015: 1 · 2014: 2 · 2013: 1
- FWCI
- 0.86
- Type
- journal article
- Language
- en
- Open access
- green
- hdl.handle.net
- Licence
- other-oa
- Locations
- Molecular Physics (publishedVersion)
- Repository for Publications and Research Data (ETH Zurich) (submittedVersion, other-oa)
- ETH Zürich Research Collection
- Topics
- Physical Sciences › Physics and Astronomy › Atomic and Molecular Physics, and Optics › Laser-Matter Interactions and Applications
- Physical Sciences › Physics and Astronomy › Atomic and Molecular Physics, and Optics › Spectroscopy and Quantum Chemical Studies
- Physical Sciences › Chemistry › Spectroscopy › Molecular Spectroscopy and Structure
- Keywords
- photodissociation dynamics, methyl iodide, CF3I, transient grating, high harmonic generation, harmonic phase, ionization potential
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