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Nonlinear optics experiments measuring phase shifts induced in a weak probe pulse by a strong pump pulse must account for coherent effects that only occur when the pump and probe pulses are temporally overlapped. It is well known that a…

We demonstrate an efficient cross-phase modulation (XPM) based on a closed-loop double-{\Lambda} system. The property of the double-{\Lambda} medium can be controlled by changing the phases of the applied optical fields. This…

Ultrafast pump-probe spectroscopy with high temporal and spectral resolutions provides new insight into ultrafast nonequilibrium phenomena. We propose that transient interference between pump and probe pulses is realized in pump-probe…

Strongly Correlated Electrons · Physics 2018-10-04 Kazuya Shinjo , Takami Tohyama

Expressions for the two-dimensional Stimulated x-ray Raman Spectroscopy (2D-SXRS) signal obtained using attosecond x-ray pulses are derived. The 1D- and 2D-SXRS signals are calculated for trans-N-methyl acetamide (NMA) with broad bandwidth…

Chemical Physics · Physics 2012-04-27 Jason D. Biggs , Yu Zhang , Daniel Healion , Shaul Mukamel

The effects of high pulse intensity and chirp on two-dimensional electronic spectroscopy signals are experimentally investigated in the highly non-perturbative regime using atomic rubidium vapor as clean model system. Data analysis is…

A dramatic spectral modulation of third-order harmonic (TH) emission generated in a near in- frared femtosecond (fs) pulse filamentation, assisted by a two-dimensional plasma grating formed by two pump femtosecond pulses, is experimentally…

Two-dimensional electronic spectroscopy (2DES) can be implemented with different geometries, e.g., BOXCARS, collinear and pump-probe geometries. The pump-probe geometry has its advantage of overlapping only two beams and reducing phase…

Quantum Physics · Physics 2024-03-04 Mao-Rui Cai , Xue Zhang , Zi-Qian Cheng , Teng-Fei Yan , Hui Dong

Transmission through photoexcited semiconductors is used to temporally and spectrally shape a Terahertz pulse. By adjusting the optical pump-THz probe delay, we experimentally introduce a polar asymmetry in the pulse profile as high as 92%.…

Two- and multi-dimensional spectroscopy is used in physics and chemistry to obtain structural and dynamical information that would otherwise be invisible by the projection into a one-dimensional data set such as a single emission or…

We calculated third order non-linear polarization to estimate the two-photon absorption of non-interacting two-level molecules in the transmission-type degenerate pump-probe geometry. The spectral intensity and the phase changes of the…

Optics · Physics 2019-05-01 Tsogvoo Khos-Ochir , Kim Myung-Whun , Purevdorj Munkhbaatar

Coherent two-dimensional electronic spectroscopy probes ultrafast dynamics using femtosecond pulses. In case the timescale of the studied dynamics become comparable to the pulse duration, pulse overlap effects may compromise the…

Chemical Physics · Physics 2022-12-27 Ulrich Bangert , Lukas Bruder , Frank Stienkemeier

A theory of pump-probe spectroscopy is developed in which optical fields drive two-quantum, Raman-like transitions between ground state sublevels. Three fields are incident on an ensemble of atoms. Two of the fields act as the pump field…

Atomic Physics · Physics 2009-11-06 P. R. Berman , B. Dubetsky

We show how to emulate a conventional pump-probe scheme using a single frequency-chirped ultrashort UV pulse to obtain a time-resolved image of molecular ultrafast dynamics. The chirp introduces a spectral phase in time that encodes the…

Chemical Physics · Physics 2017-05-03 Denis Jelovina , Johannes Feist , Fernando Martín , Alicia Palacios

We propose a scheme to achieve a uniform cross phase modulation (XPM) for two nonclassical light pulses and study its application for quantum non-demolition measurements of the photon number in a pulse and for controlled phase gates in…

Quantum Physics · Physics 2010-03-12 Karl-Peter Marzlin , Zeng-Bin Wang , Sergey A. Moiseev , Barry C. Sanders

In recent years, ultrafast pump-probe spectroscopy has provided insightful information about nonequilibrium dynamics of excitations in materials. In a typical experiment of time-resolved x-ray absorption spectroscopy, the systems are…

Strongly Correlated Electrons · Physics 2019-05-29 Chen-Yen Lai , Jian-Xin Zhu

We calculate the frequency-dispersed nonlinear transmission signal of a phase-shaped visible pulse to fourth order in the field. Two phase profiles, a phase-step and phase-pulse, are considered. Two dimensional signals obtained by varying…

Chemical Physics · Physics 2015-06-22 Rachel Glenn , Shaul Mukamel

We employ ultrafast pump-probe spectroscopy to directly monitor electron tunneling between discrete orbital states in a pair of spatially separated quantum dots. Immediately after excitation, several peaks are observed in the pump-probe…

We numerically analyze the use of intense entangled twin beams for ultra-sensitive spectroscopic measurements in chemical and biological systems. The examined scheme makes use of intense frequency-modulated (chirped) entangled beams to…

Quantum Physics · Physics 2018-05-16 Jiří Svozilík , Jan Peřina , Roberto de J. León-Montiel

Controlling the phase space of particle beams is essential for the generation of high-quality, ultrashort electron beams in plasma-based accelerators. Accurately diagnosing the transient energy chirp, which evolves rapidly at the onset of…

Plasma Physics · Physics 2024-12-20 Zhijun Zhang , Shiyi Zhou , Jiansheng Liu

Interpretation of time-resolved spectroscopies such as transient absorption (TA) or two-dimensional (2D) spectroscopy often relies on the perturbative description of light-matter interaction. In many cases the third order of nonlinear…

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