Pulse-shape effects in fifth-order multidimensional optical spectroscopy

T.N. Do; L. Chen; A.K. Belyaev; H.-S. Tan; M.F. Gelin

doi:10.1016/j.chemphys.2018.08.038

Pulse-shape effects in fifth-order multidimensional optical spectroscopy

T.N. Do, L. Chen, A.K. Belyaev, H.-S. Tan, M.F. Gelin

Research output: Contribution to Journal › Article › Academic › peer-review

Abstract

© 2018 Elsevier B.V.We study how the effects of finite pulse durations modify the fifth-order two-quantum two-dimensional (2Q-2D) and three-dimensional (3D) optical spectra. Instead of directly calculating the time domain polarization, the equivalent approach in frequency domain significantly simplifies the calculations and delivers exact expressions for the 2Q-2D and 3D spectra. Our results minimize the number of numerical integrations needed. We also derive simple analytical formulas for practically important situations when the laser pulses are short on the timescale of nuclear motion as well as short (or long) on the timescale of electronic dephasing. These formulas evaluate the measured spectra by multiplying the spectral response function by a factor depending on the spectral pulse envelopes.

Original language	English
Pages (from-to)	119-128
Journal	Chemical Physics
Volume	515
DOIs	https://doi.org/10.1016/j.chemphys.2018.08.038
Publication status	Published - 14 Nov 2018
Externally published	Yes

Funding

The work is supported by grants from the Singapore Ministry of Education Academic Research Fund (Tier 2 MOE2015-T2-1-039) and the Singaporean-German S&T Cooperation Researcher Mobility Scheme (SGP-PROG2-018). L. C. acknowledges support by a postdoctoral fellowship of the Alexander von Humboldt-Foundation. A. K. B. gratefully acknowledges support from the Ministry for Education and Science (Russian Federation), projects No. 3.5042.2017/6.7, 3.1738.2017/4.6. The work is supported by grants from the Singapore Ministry of Education Academic Research Fund (Tier 2 MOE2015-T2-1-039 ) and the Singaporean-German S&T Cooperation Researcher Mobility Scheme (SGP-PROG2-018). L. C. acknowledges support by a postdoctoral fellowship of the Alexander von Humboldt-Foundation. A. K. B. gratefully acknowledges support from the Ministry for Education and Science (Russian Federation), projects No. 3.5042.2017/6.7, 3.1738.2017/4.6.

Funders	Funder number
Singapore Ministry of Education Academic Research Fund	SGP-PROG2-018
Alexander von Humboldt-Stiftung
Ministerul Educatiei Nationale	MOE2015-T2-1-039
Ministry of Education and Science
Council on grants of the President of the Russian Federation	3.1738.2017/4.6, 3.5042.2017/6.7

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title = "Pulse-shape effects in fifth-order multidimensional optical spectroscopy",

abstract = "{\textcopyright} 2018 Elsevier B.V.We study how the effects of finite pulse durations modify the fifth-order two-quantum two-dimensional (2Q-2D) and three-dimensional (3D) optical spectra. Instead of directly calculating the time domain polarization, the equivalent approach in frequency domain significantly simplifies the calculations and delivers exact expressions for the 2Q-2D and 3D spectra. Our results minimize the number of numerical integrations needed. We also derive simple analytical formulas for practically important situations when the laser pulses are short on the timescale of nuclear motion as well as short (or long) on the timescale of electronic dephasing. These formulas evaluate the measured spectra by multiplying the spectral response function by a factor depending on the spectral pulse envelopes.",

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AU - Do, T.N.

AU - Chen, L.

AU - Belyaev, A.K.

AU - Tan, H.-S.

AU - Gelin, M.F.

PY - 2018/11/14

Y1 - 2018/11/14

N2 - © 2018 Elsevier B.V.We study how the effects of finite pulse durations modify the fifth-order two-quantum two-dimensional (2Q-2D) and three-dimensional (3D) optical spectra. Instead of directly calculating the time domain polarization, the equivalent approach in frequency domain significantly simplifies the calculations and delivers exact expressions for the 2Q-2D and 3D spectra. Our results minimize the number of numerical integrations needed. We also derive simple analytical formulas for practically important situations when the laser pulses are short on the timescale of nuclear motion as well as short (or long) on the timescale of electronic dephasing. These formulas evaluate the measured spectra by multiplying the spectral response function by a factor depending on the spectral pulse envelopes.

AB - © 2018 Elsevier B.V.We study how the effects of finite pulse durations modify the fifth-order two-quantum two-dimensional (2Q-2D) and three-dimensional (3D) optical spectra. Instead of directly calculating the time domain polarization, the equivalent approach in frequency domain significantly simplifies the calculations and delivers exact expressions for the 2Q-2D and 3D spectra. Our results minimize the number of numerical integrations needed. We also derive simple analytical formulas for practically important situations when the laser pulses are short on the timescale of nuclear motion as well as short (or long) on the timescale of electronic dephasing. These formulas evaluate the measured spectra by multiplying the spectral response function by a factor depending on the spectral pulse envelopes.

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VL - 515

SP - 119

EP - 128

JO - Chemical Physics

JF - Chemical Physics

ER -

Pulse-shape effects in fifth-order multidimensional optical spectroscopy

Abstract

Funding

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