Spectroscopic applications of three-level microwave double resonance

Andrews, David; Baker, J. G.; Blundell, B.G.; Petty, G.C.

doi:10.1016/0022-2860(83)90203-x

Cited by 13 publications

(7 citation statements)

References 6 publications

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“…Instead we applied a signal pulse to the molecular system to provide for an initial polarisation of the signal transition. The maximum off-resonance of the pump frequency is comparable to the values reported in [2].…”

Section: Introductionsupporting

confidence: 86%

“…The method was not useful for detecting pump transitions when the pump frequency was a few MHz off-resonant, which does not agree with the experience in MW double resonance spectroscopy in the frequency domain. Somewhat later Andrews et al [2] performed a pulse sequence double resonance experiment. They worked with a continuous probe microwave and applied two pump pulses with a variable delay in between.…”

Section: Introductionmentioning

confidence: 99%

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Two-Dimensional Microwave Fourier Transform Spectroscopy

Stahl

Fliege

Dreizler

1984

Zeitschrift Für Naturforschung A

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Section: Introductionsupporting

confidence: 86%

Section: Introductionmentioning

confidence: 99%

Two-Dimensional Microwave Fourier Transform Spectroscopy

Stahl

Fliege

Dreizler

1984

Zeitschrift Für Naturforschung A

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“…17,18 When the coherences involve different states, often localized on different atoms/groups in the molecule and having different frequencies, interaction between these states is required to generate a cross peak in the 2D spectrum. Irrespective of the type of two-dimensional spectroscopy, NMR, 19 IR, 17,20 visible, 21,22 or microwave, 23,24 a 2D spectrum shows a coupling pattern among different states in the molecule. Two-dimensional NMR spectroscopy has been very instrumental in identifying different stereoisomers; the analysis is rooted in the observation that the 3-bond J-couplings between antiperiplanar vs. gauche protons differ by ca.…”

Section: Introductionmentioning

confidence: 99%

Discrimination between coupling networks of glucopyranosides varying at a single stereocenter using two-dimensional vibrational correlation spectroscopy

Lin

Bendiak

Rubtsov

2012

Phys. Chem. Chem. Phys.

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A combination of two-dimensional infrared (2DIR) correlation spectroscopy, linear absorption spectroscopy, and density functional theory quantum calculations was used to identify characteristic spectral features of two anomers of acetylated 2-azido-2-deoxy-D-glucopyranose. While the linear absorption spectra for the α and β anomers were distinctive, a substantial difference between them was observed only in the spectral region below 1200 cm(-1). The infrared correlation spectra of the two anomers differed significantly, even in regions where their linear absorption spectra were similar. Very substantial differences were found for the N≡N/C=O stretch mode region of the 2DIR correlation spectrum, indicating differences in the anharmonic coupling of the N≡N stretching mode of the equatorially oriented N(3) group with the CO modes when the C(1) ester was either in the axial (α anomer) or equatorial (β anomer) orientation. In addition, the energy transport patterns originating from the excited N≡N stretching mode were found to be different for the two anomers; up to a 1.8-fold difference in the energy transport times was observed for the probed modes of the same type in the two anomers. The results demonstrate the capability of 2DIR and relaxation-assisted 2DIR (RA 2DIR) spectroscopies to provide unique spectroscopic data specific to sugar anomers that vary at a single stereochemical center. These methods identify unique coupling networks within individual sugar stereochemical units and demonstrate the potential to identify a number of stereochemical differences among them.

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“…Strong optical fields have been used to drive high-order rotational coherences and to populate high-lying rotational levels (13), to control molecular alignment dynamics (14), and to induce rotational alignment echoes (15,16). Strong microwave fields can drive high-order rotational responses and have been used for double-resonance and 2D rotational spectroscopies (17)(18)(19)(20)(21)(22), mostly at low rotational temperatures. In recent work, we demonstrated second-order interactions between THz frequency fields and molecular rotations, measuring net molecular dipole orientation, manipulating two-quantum coherences (2QCs), and observing rotational populations and their superradiant decays (23)(24)(25).…”

mentioning

confidence: 99%

“…Strong optical fields have been used to drive high-order rotational coherences and to populate high-lying rotational levels 12 , to control molecular alignment dynamics 13 , and to induce rotational alignment echoes 14,15 . Strong microwave fields can drive high-order rotational responses and have been used for double-resonance and 2D rotational spectroscopies [16][17][18][19][20][21] mostly at low rotational temperatures. In recent work, we demonstrated second-order interactions between…”

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confidence: 99%

Nonlinear two-dimensional terahertz photon echo and rotational spectroscopy in the gas phase

Zhang

Hwang

et al. 2016

Proc. Natl. Acad. Sci. U.S.A.

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Ultrafast 2D spectroscopy uses correlated multiple light−matter interactions for retrieving dynamic features that may otherwise be hidden under the linear spectrum; its extension to the terahertz regime of the electromagnetic spectrum, where a rich variety of material degrees of freedom reside, remains an experimental challenge. We report a demonstration of ultrafast 2D terahertz spectroscopy of gas-phase molecular rotors at room temperature. Using time-delayed terahertz pulse pairs, we observe photon echoes and other nonlinear signals resulting from molecular dipole orientation induced by multiple terahertz field−dipole interactions. The nonlinear time domain orientation signals are mapped into the frequency domain in 2D rotational spectra that reveal J-state-resolved nonlinear rotational dynamics. The approach enables direct observation of correlated rotational transitions and may reveal rotational coupling and relaxation pathways in the ground electronic and vibrational state.ultrafast spectroscopy | multidimensional coherent spectroscopy | terahertz | rotational dynamics R ecent years have witnessed increasing interest in 2D infrared (IR) vibrational spectroscopy techniques for studying structural dynamics and correlations between coupled molecular motions in biological systems such as water, proteins, and DNA (1-3). Multidimensional optical spectroscopies were applied to probe the high-order correlations of excitons in quantum wells and organic complexes (4, 5). However, it remains an experimental challenge to extend multidimensional spectroscopies into the terahertz (THz) frequency range where a rich variety of material degrees of freedom, including gas molecular rotations, lattice vibrations in solids, magnetization dynamics in magnetically ordered materials, and many others (6), find fundamental and technological importance. Despite challenges involved, there have been examples of 2D THz and 2D THz−Raman spectroscopies in the studies of electronic nonlinearities in solids (7,8), coupled vibrational modes in liquid molecules (9), and hydrogen bond dynamics in water (10).Rotations of gas molecules have been the subjects of intensive recent efforts in coherent spectroscopy and coherent control, motivated by interests in rotational angular momentum and energy relaxation processes, high-order optical interactions with multilevel quantum systems, and applications of molecular alignment and orientation for various forms of orbital tomography, for example using high-harmonic generation to probe the molecular orbital structures of rotating molecules (11,12). Strong optical fields have been used to drive high-order rotational coherences and to populate high-lying rotational levels (13), to control molecular alignment dynamics (14), and to induce rotational alignment echoes (15, 16). Strong microwave fields can drive high-order rotational responses and have been used for double-resonance and 2D rotational spectroscopies (17-22), mostly at low rotational temperatures. In recent work, we demonstrated second-order int...

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Spectroscopic applications of three-level microwave double resonance

Cited by 13 publications

References 6 publications

Two-Dimensional Microwave Fourier Transform Spectroscopy

Two-Dimensional Microwave Fourier Transform Spectroscopy

Discrimination between coupling networks of glucopyranosides varying at a single stereocenter using two-dimensional vibrational correlation spectroscopy

Nonlinear two-dimensional terahertz photon echo and rotational spectroscopy in the gas phase

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