Raman-enhanced polarization beats in Markovian stochastic fields

Zhang, Yanpeng; Chen, Gan; Lu, Keqing; Li, Chuangshe; Hou, Xun

doi:10.1016/s0030-4018(02)01308-1

Cited by 16 publications

(9 citation statements)

References 31 publications

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“…Thus, t A can take on any of the values t 1 , t 2 , and t 3 and likewise for t B and t C . Under the assumption that the noisy fields obey circular complex Gaussian statistics, the field breakdown goes as Modeling noisy-light fields with circular complex Gaussian statisics matches well with experimental results across a range of different nonlinear optical phenomona, , and Zhang and co-workers have explored other statistical models. − …”

Section: Theoreticalsupporting

confidence: 59%

Coherent Two-Quantum Two-Dimensional Electronic Spectroscopy Using Incoherent Light

Ulness

Turner

2017

J. Phys. Chem. A

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Two-quantum two-dimensional electronic spectroscopy (2Q 2D ES) may provide a measure of electron-correlation energies in molecules. Attempts to obtain this profound but elusive signal have relied on experimental implementations using femtosecond laser pulses, which induce an overwhelming background signal of nonresonant response. Here we explore theoretically the signatures of electron correlation in coherent 2Q 2D ES measurements that use spectrally incoherent light, I 2Q 2D ES. One can use such fields to suppress nonresonant response, and therefore this method may better isolate the desired signature of electron correlation. Using an appropriate treatment of the multilevel Bloch electronic system, we find that I 2Q 2D ES presents an opportunity to measure electron-correlation energies in molecules.

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Section: Theoreticalsupporting

confidence: 59%

Coherent Two-Quantum Two-Dimensional Electronic Spectroscopy Using Incoherent Light

Ulness

Turner

2017

J. Phys. Chem. A

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“…In 1984, Morita and Yajima, Asaka et al., and Beach and Hartmann independently demonstrated that noisy light could be used to achieve femtosecond-scale time resolution in degenerate four-wave mixing experiments. During the subsequent decade a variety of noisy-light analogues to more traditional ultrafast experiments were developed. − Although noisy light offers some advantages, it is not as generally useful as its short-pulse counterpart. One exception is coherent anti-Stokes Raman scattering spectroscopy (I (2) CARS), where the noisy-light version has proven to be a very useful tool that is still being used to investigate a variety of systems. ,− Noisy sources have found occasional uses and advantages in other spectral regimes as well. − …”

Section: Introductionmentioning

confidence: 99%

Two-Dimensional Electronic Spectroscopy Using Incoherent Light: Theoretical Analysis

Turner

Howey²,

Sutor³

et al. 2012

J. Phys. Chem. A

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Electronic energy transfer in photosynthesis occurs over a range of time scales and under a variety of intermolecular coupling conditions. Recent work has shown that electronic coupling between chromophores can lead to coherent oscillations in two-dimensional electronic spectroscopy measurements of pigment-protein complexes measured with femtosecond laser pulses. A persistent issue in the field is to reconcile the results of measurements performed using femtosecond laser pulses with physiological illumination conditions. Noisy-light spectroscopy can begin to address this question. In this work we present the theoretical analysis of incoherent two-dimensional electronic spectroscopy, I(4) 2D ES. Simulations reveal diagonal peaks, cross peaks, and coherent oscillations similar to those observed in femtosecond two-dimensional electronic spectroscopy experiments. The results also expose fundamental differences between the femtosecond-pulse and noisy-light techniques; the differences lead to new challenges and new opportunities.

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“…For the macroscopic system where phase matching takes place this signal must be drawn from the P (3) developed on one 'atom' multiplied by the (P (3) ) * that is developed on another 'atom' which must be located elsewhere in space (with summation over all such pairs) [16][17][18][19][20][21][22][23][31][32][33][34][35][36][37][38]. For homodyne detection the FASPB signal is proportional to the average of the absolute square of P (3) over the random variable of the stochastic process |P (3) | 2 , which involves fourth-and second-order coherence functions of u i (t) in phase-conjugation geometry.…”

Section: Second-order Stochastic Correlation Of Faspbmentioning

confidence: 99%

“…Polarization beats, which originate from the interference between the macroscopic polarizations that are excited simultaneously in the sample by twin fields, have attracted a lot of attention recently [24][25][26][27][28][29][30][31][32][33][34][35][36][37][38]. They are closely related to the quantum beat spectroscopy based on superposition-state interference.…”

Section: Introductionmentioning

confidence: 99%

“…Fu et al [28][29][30][31][32][33] then analysed the differencefrequency UMS with phase-conjugate geometry in a Doppler-broadened system by a secondorder coherence-function theory, and found that a Doppler-free precision in the measurement of the energy-level splitting could be achieved. We have also investigated the higher-order stochastic correlation effects of a Markovian field in the femtosecond difference-frequency polarization beats (FDPB) [31][32][33][34][35][36][37][38]. In this paper, we shall systematically study the four-level attosecond sum-frequency polarization beats in twin Markovian stochastic correlation.…”

Section: Introductionmentioning

confidence: 99%

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Twin Markovian field correlation on four-level attosecond polarization beats

Zhang¹,

Chen²,

Li³

et al. 2004

J. Phys. B: At. Mol. Opt. Phys.

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Based on the phase-conjugate polarization interference between two twophoton processes, we obtained an analytic closed form for the second-order or fourth-order Markovian stochastic correlation of the four-level attosecond sumfrequency polarization beat (FASPB) in the extremely Doppler-broadened limit. The homodyne-detected FASPB signal is shown to be particularly sensitive to the statistical properties of the Markovian stochastic light fields with arbitrary bandwidth. The different roles of the amplitude fluctuations and the phase fluctuations can be understood physically in the time-domain picture. The field correlation has a weak influence on the FASPB signal when the laser has narrow bandwidth. In contrast, when the laser has broadband linewidth, the FASPB signal shows resonant-nonresonant cross-correlation, and drastic difference for three Markovian stochastic fields. The maxima of the two twophoton signals are shifted from zero time delay to the opposite direction, and the signal exhibits damping oscillation when the laser frequency is off-resonant from the two-photon transition. A Doppler-free precision in the measurement of the energy-level sum can be achieved with an arbitrary bandwidth. As an attosecond ultrafast modulation process, it can be extended intrinsically to any sum frequency of energy levels.

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Raman-enhanced polarization beats in Markovian stochastic fields

Cited by 16 publications

References 31 publications

Coherent Two-Quantum Two-Dimensional Electronic Spectroscopy Using Incoherent Light

Coherent Two-Quantum Two-Dimensional Electronic Spectroscopy Using Incoherent Light

Two-Dimensional Electronic Spectroscopy Using Incoherent Light: Theoretical Analysis

Twin Markovian field correlation on four-level attosecond polarization beats

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