Heterodyne detection of the complete electric field of femtosecond four-wave mixing signals

Gallagher, S.; Albrecht, Allison W.; Hybl, John D.; Landin, B.; Rajaram, B.; Jonas, David M.

doi:10.1364/josab.15.002338

Cited by 149 publications

(122 citation statements)

References 35 publications

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“…Each pulse is sufficiently weak that the signal is proportional to the product of the three field magnitudes. Related third-and higherorder methods (6)(7)(8)(9) have been demonstrated in visible laser spectroscopy (1,2,(10)(11)(12)(13)(14)(15)(16)(17)(18)(19)(20)(21)(22)(23)(24). The method of choice to provide optimal spectral resolution by eliminating the inhomogeneous broadening in the IR spectrum is the photon echo.…”

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confidence: 99%

“…Time gating (16)(17)(18)(19), heterodyne detection (20)(21)(22), and spectrally resolved heterodyne detection (23,24) have been demonstrated for electronic two-level systems. By contrast the vibrational response at the third order involves a multilevel system consisting of the set of coupled v ϭ 0, v ϭ 1, and v ϭ 2 quantum states of the vibrators in the molecule.…”

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confidence: 99%

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Two-dimensional infrared spectroscopy of peptides by phase-controlled femtosecond vibrational photon echoes

Asplund

Zanni

Hochstrasser

2000

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

492

394

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Two-dimensional infrared spectra of peptides are introduced that are the direct analogues of two-and three-pulse multiple quantum NMR. Phase matching and heterodyning are used to isolate the phase and amplitudes of the electric fields of vibrational photon echoes as a function of multiple pulse delays. Structural information is made available on the time scale of a few picoseconds. Line narrowed spectra of acyl-proline-NH2 and cross peaks implying the coupling between its amide-I modes are obtained, as are the phases of the various contributions to the signals. Solvent-sensitive structural differences are seen for the dipeptide. The methods show great promise to measure structure changes in biology on a wide range of time scales.

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confidence: 99%

mentioning

confidence: 99%

Two-dimensional infrared spectroscopy of peptides by phase-controlled femtosecond vibrational photon echoes

Asplund

Zanni

Hochstrasser

2000

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

492

394

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“…Consequent with this desire to measure dissipation, more sophisticated spectroscopies are to be invoked. 2D electronic spectroscopy (2DES) is arguably one of the best spectroscopies to measure decoherence and relaxation between states [22][23][24][25]. It is a four-wave mixing technique that gives the full third-order response, from which one can infer the time evolution of the density matrix.…”

mentioning

confidence: 99%

“…They are possible in the IR region [23] and in the visible range. At visible wavelengths, they can be detected by photon echo [22], by fluorescence [42,43], by photocurrent [43] or by photoelectrons [44]. To each one of these methods corresponds a family of mesoscopic systems that may exhibit Fano profiles and that can be studied.…”

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confidence: 99%

Coherent two-dimensional spectroscopy of a Fano model

Finkelstein-Shapiro¹,

Poulsen²,

Pullerits³

et al. 2016

Phys. Rev. B

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The Fano lineshape arises from the interference of two excitation pathways to reach a continuum. Its generality has resulted in a tremendous success in explaining the lineshapes of many one-dimensional spectroscopies -absorption, emission, scattering, conductance, photofragmentation -applied to very varied systems -atoms, molecules, semiconductors and metals. Unravelling a spectroscopy into a second dimension reveals the relationship between states in addition to decongesting the spectra. Femtosecond-resolved two-dimensional electronic spectroscopy (2DES) is a four-wave mixing technique that measures the time-evolution of the populations, and coherences of excited states. It has been applied extensively to the dynamics of photosynthetic units, and more recently to materials with extended band-structures. In this letter, we solve the full time-dependent third-order response, measured in 2DES, of a Fano model and give the new system parameters that become accessible.Whenever a discrete state and a continuum state interact and radiative transitions are allowed from the ground state to both, an interference occurs that gives rise to the Fano lineshape [1][2][3][4]. In the presence of dissipative processes, it has been shown that the generalized Fano equation consisting of a standard Fano plus a Lorentzian term is [1, 2, 5-9]:where q = µ e /nπV µ c and = (ω L − ω e )/γ e , µ e is the transition dipole moment to the discrete excited state, µ c the transition dipole moment to the continuum, V the coupling of the discrete excited state to the continuum, n the density of states of the continuum, ω e is the energy of the discrete state relative to the ground state, ω L is the radiation field frequency, and γ e = nπV 2 is the linewidth of the excited state, induced by its coupling nV 2 to the continuum set of states. C is the weight of the Lorentzian term and is related to the dissipative processes [6][7][8][9][10]. Since its original inception, the 1961 paper has resulted in more than 8,000 citations testifying to its ubiquity in physics, chemistry and materials science. The first Fano profiles were observed more than 80 years ago in atomic spectra, including photoionization of atoms and photodissociation of small molecules [3,4]. The field of study was established around scattering processes where the phenomena of coupling to a thermal bath resulting in dissipation or decoherence is not important, except in a few cases, notably pressure broadening [11][12][13].The synthesis and control of matter at the nanoscale opened up the observation of Fano profiles to dissipative systems [14][15][16][17][18] which in turn spurred a renewed interest in theoretical descriptions that would solve the problem in open quantum systems [8][9][10][19][20][21], and correctly account for the relaxation. Consequent with this desire to measure dissipation, more sophisticated spectroscopies are to be invoked. 2D electronic spectroscopy (2DES) is arguably one of the best spectroscopies to measure decoherence and relaxation between states [22][23]...

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“…Field measurements of four-wave mixing signals have been accomplished in one-color optical experiments by interferometric techniques. [5] In this paper, we demonstrate the first use of cross-correlation frequency-resolved optical gating (XFROG, [6]) as a means of extracting the amplitude and phase of a spectroscopic signal, that of the free induction decay of HDO molecules in liquid D 2 O. This measurement, performed with 55 fs infrared pulses, resolves the complex linear polarization and provides a foundation for similar studies of nonlinear responses such as pump-perturbed FIDs.…”

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confidence: 99%

Time and frequency-Gated FID: a new approach to study the vibrational dephasing of water

Gruetzmacher

Scherer

2001

Ultrafast Phenomena XII

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Abstract. The ultrafast frequency-resolved upconverted vibrational free induction decay (FID) of HDO in D 2 O was measured, allowing extraction of the amplitude and phase of the coherent transient. The FID Wigner spectrogram shows evidence of λ-dependent dynamics.Considerable experimental and theoretical effort has been expended toward understanding the behavior of liquid water at the molecular level, much of it striving to understand the structural and dynamical character of its hydrogen bonding interactions. Investigations of the hydrogen bonding nature of water via vibrational spectroscopy have focused on the OH-stretching band in the 3 µm region. The broad frequency profile of this band and the correlation between stretching frequency and hydrogen bond strength has prompted debate over the possible existence of distinct hydrogen-bonded species and their timescales of Femtosecond mid-infrared (MIR) pulses were generated by a type-I optical parametric amplifier (OPA) based on the nonlinear crystal KNbO 3 (KN).[7] The OPA is pumped by the fundamental of a home-built Ti:sapphire regenerative amplifier and seeded with the near-infrared portion of a white light continuum

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Heterodyne detection of the complete electric field of femtosecond four-wave mixing signals

Cited by 149 publications

References 35 publications

Two-dimensional infrared spectroscopy of peptides by phase-controlled femtosecond vibrational photon echoes

Two-dimensional infrared spectroscopy of peptides by phase-controlled femtosecond vibrational photon echoes

Coherent two-dimensional spectroscopy of a Fano model

Time and frequency-Gated FID: a new approach to study the vibrational dephasing of water

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