Molecular, multiresonant coherent four-wave mixing spectroscopy

Wright, John; Carlson, Roger J.; Hurst, Gregory B.; Steehler, Jack K.; Riebe, Michael T.; Price, Bradford B.; Nguyen, Dinh C.; Lee, Steven H.

doi:10.1080/01442359109353262

Cited by 55 publications

(27 citation statements)

References 64 publications

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“…Triply resonant (or fully resonant) FWM techniques were developed and investigated by Wright et al in the 1980s in order to create a family of highly resonant FWM spectroscopic techniques. 61 In all of these techniques, three separately tunable input photons (o1, o2, o3) are used to generate a fourth output photon (o4 ¼ AE o1 AE o2 AE o3). When any of the photons have frequencies that match natural resonances in a molecule, the intensity of this generated o4 beam grows, resulting in a peak in the nonlinear spectrum.…”

Section: Three General Methods For Generating Coherent Two-dimensionamentioning

confidence: 99%

An Introduction to Coherent Multidimensional Spectroscopy

Chen¹

2016

Appl Spectrosc

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Coherent multidimensional spectroscopy is a field that has drawn much attention as an optical analogue to multidimensional nuclear magnetic resonance imaging. Coherent multidimensional spectroscopic techniques produce spectra that show the magnitude of an optical signal as a function of two or more pulsed laser frequencies. Spectra can be collected in either the frequency or the time domain. In addition to improving resolution and overcoming spectral congestion, coherent multidimensional spectroscopy provides the ability to investigate and conduct studies based upon the relationship between different peaks. The purpose of this paper is to provide a general introduction to the area of coherent multidimensional spectroscopy, to provide a brief overview of current experimental approaches, and to discuss some emerging developments in this relatively young field.

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Section: Three General Methods For Generating Coherent Two-dimensionamentioning

confidence: 99%

An Introduction to Coherent Multidimensional Spectroscopy

Chen¹

2016

Appl Spectrosc

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“…Treatment of the theoretical description of multiresonant CMDS follows that given in earlier publications. ,,, The spatial and temporal dependence of the total electric field from the three excitation pulses is where k⃗ i · z⃗ is the wave vector in the propagation direction, z⃗ i , ω i = 2 πc ν̅ i is the angular frequency, and E i o ( t ) is the slowly varying amplitude of the pulse envelope of the i th excitation beam, typically of the form e –( t –τ) 2 /σ 2 . The electric field creates a nonlinear polarization which, in the frequency domain, is given by P⃗ NL = χ (3) E⃗ 3 where χ (3) is the third order susceptibility tensor.…”

Section: Theorymentioning

confidence: 99%

“…The coherences formed by MENS will constructively interfere if the broadening is correlated, i.e., when the broadening shifts quantum levels in the same direction. These effects are discussed more completely in ref .…”

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Multidimensional Spectral Fingerprints of a New Family of Coherent Analytical Spectroscopies

Neff-Mallon

Wright

2017

Anal. Chem.

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Triply resonant sum frequency (TRSF) and doubly vibrationally enhanced (DOVE) spectroscopies are examples of a recently developed family of coherent multidimensional spectroscopies (CMDS) that are analogous to multidimensional NMR and current analytical spectroscopies. CMDS methods are particularly promising for analytical applications because their inherent selectivity makes them applicable to complex samples. Like NMR, they are based on creating quantum mechanical superposition states that are fully coherent and lack intermediate quantum state populations that cause quenching or other relaxation effects. Instead of the nuclear spin states of NMR, their multidimensional spectral fingerprints result from creating quantum mechanical mixtures of vibrational and electronic states. Vibrational states provide spectral selectivity, and electronic states provide large signal enhancements. This paper presents the first electronically resonant DOVE spectra and demonstrates the capabilities for analytical chemistry applications by comparing electronically resonant TRSF and DOVE spectra with each other and with infrared absorption and resonance Raman spectra using a Styryl 9 M dye as a model system. The methods each use two infrared absorption transitions and a resonant Raman transition to create a coherent output beam, but they differ in how they access the vibrational and electronic states and the frequency of their output signal. Just as FTIR, UV-vis, Raman, and resonance Raman are complementary methods, TRSF and DOVE methods are complementary to coherent Raman methods such as coherent anti-Stokes Raman spectroscopy (CARS).

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“…A multi-resonant series of excitation pulses creates many coherences with unique phase and resonance characteristics [5,47,65]. A multiquantum coherence is a time-dependent state that is a linear combinations of multiple molecular states that are created by resonance with coherent excitations:…”

Section: Introductionmentioning

confidence: 99%

Vibrational correlations via coherent multi-resonant four-wave mixing

Wright

2004

Vibrational Spectroscopy

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Molecular, multiresonant coherent four-wave mixing spectroscopy

Cited by 55 publications

References 64 publications

An Introduction to Coherent Multidimensional Spectroscopy

An Introduction to Coherent Multidimensional Spectroscopy

Multidimensional Spectral Fingerprints of a New Family of Coherent Analytical Spectroscopies

Vibrational correlations via coherent multi-resonant four-wave mixing

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