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Title: Frequency-domain coherent multidimensional spectroscopy when dephasing rivals pulsewidth: Disentangling material and instrument response

Abstract

Ultrafast spectroscopy is often collected in the mixed frequency/time domain, where pulse durations are similar to system dephasing times. In these experiments, expectations derived from the familiar driven and impulsive limits are not valid. This work simulates the mixed-domain four-wave mixing response of a model system to develop expectations for this more complex field-matter interaction. We also explore frequency and delay axes. We show that these line shapes are exquisitely sensitive to excitation pulse widths and delays. Near pulse overlap, the excitation pulses induce correlations that resemble signatures of dynamic inhomogeneity. We describe these line shapes using an intuitive picture that connects to familiar field-matter expressions. We develop strategies for distinguishing pulse-induced correlations from true system inhomogeneity. Our simulations provide a foundation for interpretation of ultrafast experiments in the mixed domain.

Authors:
ORCiD logo [1]; ORCiD logo [1];  [1]
  1. Univ. of Wisconsin, Madison, WI (United States). Dept. of Chemistry
Publication Date:
Research Org.:
Univ. of Wisconsin, Madison, WI (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1393442
Alternate Identifier(s):
OSTI ID: 1377970
Grant/Contract Number:  
SC0002162; FG02-09ER46664
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Chemical Physics
Additional Journal Information:
Journal Volume: 147; Journal Issue: 8; Journal ID: ISSN 0021-9606
Publisher:
American Institute of Physics (AIP)
Country of Publication:
United States
Language:
English
Subject:
14 SOLAR ENERGY; 36 MATERIALS SCIENCE

Citation Formats

Kohler, Daniel D., Thompson, Blaise J., and Wright, John C. Frequency-domain coherent multidimensional spectroscopy when dephasing rivals pulsewidth: Disentangling material and instrument response. United States: N. p., 2017. Web. doi:10.1063/1.4986069.
Kohler, Daniel D., Thompson, Blaise J., & Wright, John C. Frequency-domain coherent multidimensional spectroscopy when dephasing rivals pulsewidth: Disentangling material and instrument response. United States. doi:10.1063/1.4986069.
Kohler, Daniel D., Thompson, Blaise J., and Wright, John C. Thu . "Frequency-domain coherent multidimensional spectroscopy when dephasing rivals pulsewidth: Disentangling material and instrument response". United States. doi:10.1063/1.4986069. https://www.osti.gov/servlets/purl/1393442.
@article{osti_1393442,
title = {Frequency-domain coherent multidimensional spectroscopy when dephasing rivals pulsewidth: Disentangling material and instrument response},
author = {Kohler, Daniel D. and Thompson, Blaise J. and Wright, John C.},
abstractNote = {Ultrafast spectroscopy is often collected in the mixed frequency/time domain, where pulse durations are similar to system dephasing times. In these experiments, expectations derived from the familiar driven and impulsive limits are not valid. This work simulates the mixed-domain four-wave mixing response of a model system to develop expectations for this more complex field-matter interaction. We also explore frequency and delay axes. We show that these line shapes are exquisitely sensitive to excitation pulse widths and delays. Near pulse overlap, the excitation pulses induce correlations that resemble signatures of dynamic inhomogeneity. We describe these line shapes using an intuitive picture that connects to familiar field-matter expressions. We develop strategies for distinguishing pulse-induced correlations from true system inhomogeneity. Our simulations provide a foundation for interpretation of ultrafast experiments in the mixed domain.},
doi = {10.1063/1.4986069},
journal = {Journal of Chemical Physics},
number = 8,
volume = 147,
place = {United States},
year = {2017},
month = {8}
}

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Cited by: 5 works
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Works referenced in this record:

The two-dimensional IR nonlinear spectroscopy of a cyclic penta-peptide in relation to its three-dimensional structure
journal, March 1999

  • Hamm, P.; Lim, M.; DeGrado, W. F.
  • Proceedings of the National Academy of Sciences, Vol. 96, Issue 5
  • DOI: 10.1073/pnas.96.5.2036

The grating decomposition method: A new approach for understanding polarization‐selective transient grating experiments. II. Applications
journal, July 1992

  • Fourkas, John T.; Trebino, Rick; Fayer, M. D.
  • The Journal of Chemical Physics, Vol. 97, Issue 1
  • DOI: 10.1063/1.463525

Infrared Photon Echo Experiments: Exploring Vibrational Dynamics in Liquids and Glasses
journal, November 1995

  • Tokmakoff, A.; Fayer, M. D.
  • Accounts of Chemical Research, Vol. 28, Issue 11
  • DOI: 10.1021/ar00059a001

Dynamics of spectral hole burning
journal, February 1988

  • Brito Cruz, C. H.; Gordon, J. P.; Becker, P. C.
  • IEEE Journal of Quantum Electronics, Vol. 24, Issue 2
  • DOI: 10.1109/3.122

Spectral Simplification in Vibrational Spectroscopy Using Doubly Vibrationally Enhanced Infrared Four Wave Mixing
journal, December 1999

  • Zhao, Wei; Wright, John C.
  • Journal of the American Chemical Society, Vol. 121, Issue 47
  • DOI: 10.1021/ja9926414

The grating decomposition method: A new approach for understanding polarization‐selective transient grating experiments. I. Theory
journal, July 1992

  • Fourkas, John T.; Trebino, Rick; Fayer, M. D.
  • The Journal of Chemical Physics, Vol. 97, Issue 1
  • DOI: 10.1063/1.463565

Picosecond coherence coupling in the pump and probe technique
journal, November 1981


Mixed Frequency-/Time-Domain Coherent Multidimensional Spectroscopy: Research Tool or Potential Analytical Method?
journal, September 2009

  • Pakoulev, Andrei V.; Rickard, Mark A.; Kornau, Kathryn M.
  • Accounts of Chemical Research, Vol. 42, Issue 9
  • DOI: 10.1021/ar900032g

On the nature of “coherent artifact”
journal, February 2005

  • Lebedev, M. V.; Misochko, O. V.; Dekorsy, T.
  • Journal of Experimental and Theoretical Physics, Vol. 100, Issue 2
  • DOI: 10.1134/1.1884668

Ultrafast Dynamics within the 1S Exciton Band of Colloidal PbSe Quantum Dots Using Multiresonant Coherent Multidimensional Spectroscopy
journal, February 2014

  • Kohler, Daniel D.; Block, Stephen B.; Kain, Schuyler
  • The Journal of Physical Chemistry C, Vol. 118, Issue 9
  • DOI: 10.1021/jp412058u

Two-color three pulse photon echo peak shift spectroscopy
journal, April 2002

  • Agarwal, Ritesh; Prall, Bradley S.; Rizvi, Abbas H.
  • The Journal of Chemical Physics, Vol. 116, Issue 14
  • DOI: 10.1063/1.1459414

Femtosecond Stimulated Raman Study of Excited-State Evolution in Bacteriorhodopsin
journal, May 2005

  • McCamant, David W.; Kukura, Philipp; Mathies, Richard A.
  • The Journal of Physical Chemistry B, Vol. 109, Issue 20
  • DOI: 10.1021/jp050095x

Direct identification and decongestion of Fermi resonances by control of pulse time ordering in two-dimensional IR spectroscopy
journal, September 2007

  • Donaldson, Paul M.; Guo, Rui; Fournier, Frederic
  • The Journal of Chemical Physics, Vol. 127, Issue 11
  • DOI: 10.1063/1.2771176

Triply Resonant Sum Frequency Spectroscopy: Combining Advantages of Resonance Raman and 2D-IR
journal, November 2013

  • Boyle, Erin S.; Neff-Mallon, Nathan A.; Wright, John C.
  • The Journal of Physical Chemistry A, Vol. 117, Issue 47
  • DOI: 10.1021/jp409377a

Exciton–bath coupling and inhomogeneous broadening in the optical spectroscopy of semiconductor quantum dots
journal, May 2003

  • Salvador, Mayrose R.; Hines, Margaret A.; Scholes, Gregory D.
  • The Journal of Chemical Physics, Vol. 118, Issue 20
  • DOI: 10.1063/1.1568733

Two-dimensional line-shape analysis of photon-echo signal
journal, December 1999


Analytical solutions to the finite-pulse Bloch model for multidimensional coherent spectroscopy
journal, January 2017

  • Smallwood, Christopher L.; Autry, Travis M.; Cundiff, Steven T.
  • Journal of the Optical Society of America B, Vol. 34, Issue 2
  • DOI: 10.1364/josab.34.000419

Nonresonant Background Suppression in Broadband Vibrational Sum-Frequency Generation Spectroscopy
journal, August 2007

  • Lagutchev, Alexei; Hambir, Selezion A.; Dlott, Dana D.
  • The Journal of Physical Chemistry C, Vol. 111, Issue 37
  • DOI: 10.1021/jp075391j

Fully Coherent Triple Sum Frequency Spectroscopy of a Benzene Fermi Resonance
journal, July 2013

  • Boyle, Erin S.; Pakoulev, Andrei V.; Wright, John C.
  • The Journal of Physical Chemistry A, Vol. 117, Issue 27
  • DOI: 10.1021/jp404713x

Pump/probe self heterodyned 2D spectroscopy of vibrational transitions of a small globular peptide
journal, January 2000

  • Hamm, Peter; Lim, Manho; DeGrado, William F.
  • The Journal of Chemical Physics, Vol. 112, Issue 4
  • DOI: 10.1063/1.480772

Ultrafast Processes
journal, July 1970


Phase-locked heterodyne-detected stimulated photon echo. A unique tool to study solute—solvent interactions
journal, May 1995

  • de Boeij, Wim P.; Pshenichnikov, Maxim S.; Wiersma, Douwe A.
  • Chemical Physics Letters, Vol. 238, Issue 1-3
  • DOI: 10.1016/0009-2614(95)00452-1

Spectroscopic Characteristics of Triply Vibrationally Enhanced Four-Wave Mixing Spectroscopy
journal, July 2004

  • Besemann, Daniel M.; Meyer, Kent A.; Wright, John C.
  • The Journal of Physical Chemistry B, Vol. 108, Issue 29
  • DOI: 10.1021/jp049597l

On the relation between the echo-peak shift and Brownian-oscillator correlation function
journal, April 1996

  • de Boeij, Wim P.; Pshenichnikov, Maxim S.; Wiersma, Douwe A.
  • Chemical Physics Letters, Vol. 253, Issue 1-2
  • DOI: 10.1016/0009-2614(96)00207-2

Photon echoes and related four‐wave‐mixing spectroscopies using phase‐locked pulses
journal, April 1992

  • Cho, Minhaeng; Scherer, Norbert F.; Fleming, Graham R.
  • The Journal of Chemical Physics, Vol. 96, Issue 8
  • DOI: 10.1063/1.462686

Three-Pulse Echo Peak Shift Studies of Polar Solvation Dynamics
journal, January 1997

  • Passino, Sean A.; Nagasawa, Yutaka; Joo, Taiha
  • The Journal of Physical Chemistry A, Vol. 101, Issue 4
  • DOI: 10.1021/jp9621383

Interactions between Light Waves in a Nonlinear Dielectric
journal, September 1962


Generation of Simplified Protein Raman Spectra Using Three-Color Picosecond Coherent Anti-Stokes Raman Spectroscopy
journal, September 2010

  • Donaldson, Paul M.; Willison, Keith R.; Klug, David R.
  • The Journal of Physical Chemistry B, Vol. 114, Issue 37
  • DOI: 10.1021/jp1061607

Molecular, multiresonant coherent four-wave mixing spectroscopy
journal, October 1991

  • Wright, John C.; Carlson, Roger J.; Hurst, Gregory B.
  • International Reviews in Physical Chemistry, Vol. 10, Issue 4
  • DOI: 10.1080/01442359109353262

Phase-stabilized two-dimensional electronic spectroscopy
journal, September 2004

  • Brixner, Tobias; Mančal, Tomáš; Stiopkin, Igor V.
  • The Journal of Chemical Physics, Vol. 121, Issue 9
  • DOI: 10.1063/1.1776112

Two-Color Pump−Probe Spectroscopies of Two- and Three-Level Systems:  2-Dimensional Line Shapes and Solvation Dynamics
journal, August 2003

  • Kwac, Kijeong; Cho, Minhaeng
  • The Journal of Physical Chemistry A, Vol. 107, Issue 31
  • DOI: 10.1021/jp034727w

Transient absorption of vibrationally excited water
journal, February 2002

  • Bakker, H. J.; Nienhuys, H. -K.; Gallot, G.
  • The Journal of Chemical Physics, Vol. 116, Issue 6
  • DOI: 10.1063/1.1432687

Three-pulse scattering for femtosecond dephasing studies: theory and experiment
journal, January 1985

  • Weiner, A. M.; De Silvestri, S.; Ippen, E. P.
  • Journal of the Optical Society of America B, Vol. 2, Issue 4
  • DOI: 10.1364/josab.2.000654

Intersystem crossing from singlet states of molecular dimers and monomers in mixed molecular crystals: picosecond stimulated photon echo experiments
journal, February 1984


Photon-echo relaxation in molecular mixed crystals
journal, September 1976


Ultrabroadband femtosecond two-dimensional ultraviolet transient absorption
journal, January 2012

  • Auböck, Gerald; Consani, Cristina; van Mourik, Frank
  • Optics Letters, Vol. 37, Issue 12
  • DOI: 10.1364/ol.37.002337

The interaction of solutes with their environments
journal, February 1998

  • Fleming, G. R.; Passino, S. A.; Nagasawa, Y.
  • Philosophical Transactions of the Royal Society of London. Series A: Mathematical, Physical and Engineering Sciences, Vol. 356, Issue 1736
  • DOI: 10.1098/rsta.1998.0172

Ultrafast Librational Dynamics of the Hydrated Electron
journal, May 1998


Enhanced selectivity for spectrochemical measurement by mode selection in fully resonant nonlinear mixing
journal, July 1991

  • Carlson, Roger J.; Wright, John C.
  • Analytical Chemistry, Vol. 63, Issue 14
  • DOI: 10.1021/ac00014a019

Frequency and Time-Resolved Triply Vibrationally Enhanced Four-Wave Mixing Spectroscopy
journal, December 2004

  • Meyer, Kent A.; Wright, John C.; Thompson, David E.
  • The Journal of Physical Chemistry A, Vol. 108, Issue 52
  • DOI: 10.1021/jp046137j

Line shape and Doppler broadening in resonant CARS and related nonlinear processes through a diagrammatic approach
journal, January 1979


Resonance IR: A Coherent Multidimensional Analogue of Resonance Raman
journal, April 2014

  • Boyle, Erin S.; Neff-Mallon, Nathan A.; Handali, Jonathan D.
  • The Journal of Physical Chemistry A, Vol. 118, Issue 17
  • DOI: 10.1021/jp5018554

Simulating multidimensional optical wave-mixing signals with finite-pulse envelopes
journal, March 2008


Analysis of Femtosecond Dynamic Absorption Spectra of Nonstationary States
journal, January 1992


Measurement of χ ( 3 ) for Doubly Vibrationally Enhanced Four Wave Mixing Spectroscopy
journal, September 1999


Dependence of line shapes in femtosecond broadband stimulated Raman spectroscopy on pump-probe time delay
journal, January 2005

  • Yoon, Sangwoon; McCamant, David W.; Kukura, Philipp
  • The Journal of Chemical Physics, Vol. 122, Issue 2
  • DOI: 10.1063/1.1828044

Two-dimensional infrared spectroscopy of peptides by phase-controlled femtosecond vibrational photon echoes
journal, July 2000

  • Asplund, M. C.; Zanni, M. T.; Hochstrasser, R. M.
  • Proceedings of the National Academy of Sciences, Vol. 97, Issue 15
  • DOI: 10.1073/pnas.140227997

Optical fingerprinting of peptides using two-dimensional infrared spectroscopy: Proof of principle
journal, March 2008

  • Fournier, Frédéric; Gardner, Elizabeth M.; Guo, Rui
  • Analytical Biochemistry, Vol. 374, Issue 2
  • DOI: 10.1016/j.ab.2007.11.009

Spectral line‐narrowing and saturation effects in fully resonant nondegenerate four wave mixing
journal, March 1988

  • Riebe, Michael T.; Wright, John C.
  • The Journal of Chemical Physics, Vol. 88, Issue 5
  • DOI: 10.1063/1.453939

Measurement of Ultrafast Excitonic Dynamics of Few-Layer MoS 2 Using State-Selective Coherent Multidimensional Spectroscopy
journal, October 2015


Finite pulse effects in single and double quantum spectroscopies
journal, January 2017

  • Perlík, Václav; Hauer, Jürgen; Šanda, František
  • Journal of the Optical Society of America B, Vol. 34, Issue 2
  • DOI: 10.1364/josab.34.000430

Multiresonant Coherent Multidimensional Electronic Spectroscopy of Colloidal PbSe Quantum Dots
journal, October 2011

  • Yurs, Lena A.; Block, Stephen B.; Pakoulev, Andrei V.
  • The Journal of Physical Chemistry C, Vol. 115, Issue 46
  • DOI: 10.1021/jp207273x

Nonlinear Two-Dimensional Vibrational Spectroscopy
journal, July 2000

  • Zhao, Wei; Murdoch, Keith M.; Besemann, Daniel M.
  • Applied Spectroscopy, Vol. 54, Issue 7
  • DOI: 10.1366/0003702001950481

Mixed Frequency/Time Domain Optical Analogues of Heteronuclear Multidimensional NMR
journal, March 2006

  • Pakoulev, Andrei V.; Rickard, Mark A.; Meyer, Kent A.
  • The Journal of Physical Chemistry A, Vol. 110, Issue 10
  • DOI: 10.1021/jp057339y

Two-dimensional heterodyned and stimulated infrared photon echoes of N-methylacetamide-D
journal, January 2001

  • Zanni, Martin T.; Asplund, Matthew C.; Hochstrasser, Robin M.
  • The Journal of Chemical Physics, Vol. 114, Issue 10
  • DOI: 10.1063/1.1346647

Parametric and nonparametric four‐wave mixing in pentacene: p ‐terphenyl
journal, October 1985

  • Steehler, J. K.; Wright, J. C.
  • The Journal of Chemical Physics, Vol. 83, Issue 7
  • DOI: 10.1063/1.449177

Ultrafast Solvation Dynamics Explored by Femtosecond Photon echo Spectroscopies
journal, October 1998


Line narrowing in multiresonant third order molecular spectroscopies
journal, September 1990


Nonlinear spectroscopy by multiresonant four-wave mixing
journal, September 1980


Theoretical Foundations for a New Family of Infrared Four-Wave Mixing Spectroscopies
journal, July 1997

  • Wright, John C.; Chen, Peter C.; Hamilton, James P.
  • Applied Spectroscopy, Vol. 51, Issue 7
  • DOI: 10.1366/0003702971941601

Peak shapes in femtosecond 2D correlation spectroscopy
journal, May 2001


Quantitative Modeling of Nonlinear Processes in Coherent Two-Dimensional Vibrational Spectroscopy
journal, October 2003

  • Wright, John C.; Condon, Nicholas J.; Murdoch, Keith M.
  • The Journal of Physical Chemistry A, Vol. 107, Issue 40
  • DOI: 10.1021/jp034018i

M ULTIDIMENSIONAL F EMTOSECOND C ORRELATION S PECTROSCOPIES OF E LECTRONIC AND V IBRATIONAL E XCITATIONS
journal, October 2000


Diagrammatic analysis of the density operator for nonlinear optical calculations: Pulsed and cw responses
journal, October 1978


Resonant non-linear spectroscopy in strong fields
journal, March 1983


Coherent interactions in pump–probe absorption measurements: the effect of phase gratings
journal, January 1985

  • Palfrey, S. L.; Heinz, T. F.
  • Journal of the Optical Society of America B, Vol. 2, Issue 4
  • DOI: 10.1364/josab.2.000674

Efficient Calculation of Time- and Frequency-Resolved Four-Wave-Mixing Signals
journal, September 2009

  • Gelin, Maxim F.; Egorova, Dassia; Domcke, Wolfgang
  • Accounts of Chemical Research, Vol. 42, Issue 9
  • DOI: 10.1021/ar900045d

Efficient method for the calculation of time- and frequency-resolved four-wave mixing signals and its application to photon-echo spectroscopy
journal, October 2005

  • Gelin, Maxim F.; Egorova, Dassia; Domcke, Wolfgang
  • The Journal of Chemical Physics, Vol. 123, Issue 16
  • DOI: 10.1063/1.2062188

Analysis of vibronic mode coupling in pentacene by fully resonant coherent four‐wave mixing
journal, February 1990

  • Carlson, Roger J.; Nguyen, Dinh C.; Wright, John C.
  • The Journal of Chemical Physics, Vol. 92, Issue 3
  • DOI: 10.1063/1.458084

Compact broadband vibrational sum-frequency generation spectrometer with nonresonant suppression
journal, April 2010

  • Lagutchev, Alexei; Lozano, Aaron; Mukherjee, Prabuddha
  • Spectrochimica Acta Part A: Molecular and Biomolecular Spectroscopy, Vol. 75, Issue 4
  • DOI: 10.1016/j.saa.2009.12.066