Multidimensional Femtosecond Correlation Spectroscopies of Electronic and Vibrational Excitations

Mukamel, Shaul

doi:10.1146/annurev.physchem.51.1.691

Cited by 811 publications

(823 citation statements)

References 234 publications

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“…Multidimensional correlation spectroscopies [69] may also be implemented at the nanoscale in this way, without the need for hybrid approaches [70]. Lastly, we wish to point out that these ideas may also be pursued in the infrared spectral range using surface phonon-polaritons [71] or at THz and lower frequencies using spoof SPPs [72,73].…”

Section: Discussionmentioning

confidence: 99%

Light scattering under nanofocusing: Towards coherent nanoscopies

Mohammadi

Agio

2012

Optics Communications

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We investigate light scattering under nanofocusing in the context of coherent spectroscopy. We discuss the different mechanisms that may enhance the signal in extinction and how these depend on nanofocusing as well as on the probed system. We find that nanofocusing may improve the detection sensitivity by orders of magnitude under realistic conditions, enabling scanning implementations of coherent spectroscopy at the nanoscale.

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Section: Discussionmentioning

confidence: 99%

Light scattering under nanofocusing: Towards coherent nanoscopies

Mohammadi

Agio

2012

Optics Communications

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“…55,64,[67][68][69][70] Structural fluctuations give rise to frequency fluctuations. The FFCF is the probability that a molecule with frequency o at time t = 0, still has frequency o at some later time averaged over the complete ensemble of molecules.…”

Section: D Vibrational Echo Experiments a Illustration Of The mentioning

confidence: 99%

Probing dynamics of complex molecular systems with ultrafast 2D IR vibrational echo spectroscopy

Finkelstein

Zheng

Ishikawa

et al. 2007

Phys. Chem. Chem. Phys.

148

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Ultrafast 2D IR vibrational echo spectroscopy is described and a number of experimental examples are given. Details of the experimental method including the pulse sequence, heterodyne detection, and determination of the absorptive component of the 2D spectrum are outlined. As an initial example, the 2D spectrum of the stretching mode of CO bound to the protein myoglobin (MbCO) is presented. The time dependence of the 2D spectrum of MbCO, which is caused by protein structural evolution, is presented and its relationship to the frequency-frequency correlation function is described and used to make protein structural assignments based on comparisons to molecular dynamics simulations. The 2D vibrational echo experiments on the protein horseradish peroxidase are presented. The time dependence of the 2D spectra of the enzyme in the free form and with a substrate bound at the active site are compared and used to examine the influence of substrate binding on the protein's structural dynamics. The application of 2D vibrational echo spectroscopy to the study of chemical exchange under thermal equilibrium conditions is described. 2D vibrational echo chemical exchange spectroscopy is applied to the study of formation and dissociation of organic solute-solvent complexes and to the isomerization around a carbon-carbon single bond of an ethane derivative.

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“…47 Reviews of these inherently multi-dimensional fs spectroscopies of vibronic excitations have recently appeared. 48,49 …”

Section: Introductionmentioning

confidence: 99%

The manipulation of massive ro-vibronic superpositions using time–frequency-resolved coherent anti-Stokes Raman scattering (TFRCARS): from quantum control to quantum computing

et al. 2001

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Molecular ro-vibronic coherences, joint energy-time distributions of quantum amplitudes, are selectively prepared, manipulated, and imaged in TimeFrequency-Resolved Coherent Anti-Stokes Raman Scattering (TFRCARS) measurements using femtosecond laser pulses. The studies are implemented in iodine vapor, with its thermally occupied statistical ro-vibrational density serving as initial state. The evolution of the massive ro-vibronic superpositions, consisting of 10 3 eigenstates, is followed through two-dimensional images. The first-and second-order coherences are captured using time-integrated frequencyresolved CARS, while the third-order coherence is captured using time-gated frequency-resolved CARS. The Fourier filtering provided by time integrated detection projects out single ro-vibronic transitions, while time-gated detection allows the projection of arbitrary ro-vibronic superpositions from the coherent third-order polarization. A detailed analysis of the data is provided to highlight the salient features of this four-wave mixing process. The richly patterned images of the ro-vibrational coherences can be understood in terms of phase evolution in rotation-vibration-electronic Hilbert space, using time circuit diagrams. Beside the control and imaging of chemistry, the controlled manipulation of massive quantum coherences suggests the possibility of quantum computing. We argue that the universal logic gates necessary for arbitrary quantum computing -all single qubit operations and the two-qubit controlled-NOT (CNOT) gate -are available in time resolved four-wave mixing in a molecule. The molecular rotational manifold is naturally "wired" for carrying out all single qubit operations efficiently, and in parallel. We identify vibronic coherences as one example of a naturally available two-qubit CNOT gate, wherein the vibrational qubit controls the switching of the targeted electronic qubit. † Present address:

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Multidimensional Femtosecond Correlation Spectroscopies of Electronic and Vibrational Excitations

Cited by 811 publications

References 234 publications

Light scattering under nanofocusing: Towards coherent nanoscopies

Light scattering under nanofocusing: Towards coherent nanoscopies

Probing dynamics of complex molecular systems with ultrafast 2D IR vibrational echo spectroscopy

The manipulation of massive ro-vibronic superpositions using time–frequency-resolved coherent anti-Stokes Raman scattering (TFRCARS): from quantum control to quantum computing

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