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Two-dimensional (2D) spectroscopy combines high temporal and spectral resolution, allowing the observation of ultrafast energy transfer and the separation of homogeneous and inhomogeneous broadening. Typically, 2D spectroscopy is dominated…

Terahertz two-dimensional coherent spectroscopy (THz-2DCS) is transforming our ability to probe, visualize, and control quantum materials far from equilibrium. This emerging technique brings multi-dimensional resolution to the ultrafast…

Superconductivity · Physics 2026-02-09 Chuankun Huang , Martin Mootz , Liang Luo , Ilias E. Perakis , Jigang Wang

Coherent two-dimensional spectroscopy in IR or visible region is very effective for studying correlations, energy relaxation/transfer pathways in complex multi-chromophore or multi-mode systems. However it is usually restricted up to…

Chemical Physics · Physics 2020-09-15 Darius Abramavicius

We characterize the coherent dynamics of a two-level quantum emitter driven by a pair of symmetrically-detuned phase-locked pulses. The promise of dichromatic excitation is to spectrally isolate the excitation laser from the quantum…

Recent work applying multidimentional coherent electronic spectroscopy at dilute samples in the gas phase is reviewed. The development of refined phase-cycling approaches with improved sensitivity has opened-up new opportunities to probe…

Atomic and Molecular Clusters · Physics 2019-09-12 Lukas Bruder , Ulrich Bangert , Marcel Binz , Daniel Uhl , Frank Stienkemeier

Spectroscopic features revealing the coherent interaction of a degenerate two-level atomic system with two optical fields are examined. A model for the numerical calculation of the response of a degenerate two-level system to the action of…

Quantum Physics · Physics 2007-05-23 A. Lezama S. Barreiro A. Lipsich A. M. Akulshin

The role of quantum effects in excitonic energy transport (EET) has been scrutinised intensely and with increasingly sophisticated experimental techniques. This increased complexity requires invoking correspondingly elaborate models to fit…

Quantum Physics · Physics 2019-11-14 Max Marcus , George Knee , Animesh Datta

We present a two-dimensional electronic spectroscopy (2DES) platform driven by a novel Coherent Loop-based Integrated Modulating and Beamsplitting System (CLIMBS). Coupled with an octave-spanning multiple-plate continuum (MPC) source,…

Single-beam spectrally controlled (SBSC) two-dimensional (2D) Raman spectroscopy is a unique 2D vibrational measurement technique utilizing trains of short pulses that are generated from a single broadband pulse by pulse shaping. This…

Chemical Physics · Physics 2021-03-30 Ju-Yeon Jo , Yoshitaka Tanimura

Optical two-dimensional coherent spectroscopy (2DCS) is a powerful ultrafast spectroscopic technique that can greatly benefit from the unique features of a femtosecond laser operating at a kHz repetition rate. However, isolating specific…

Optics · Physics 2024-08-08 Stephen Revesz , Rustam Gatamov , Adolfo Misiara , Hebin Li

A novel technique to sensitively and selectively isolate multiple-quantum coherences in a femtosecond pump-probe setup is presented. Detecting incoherent observables and imparting lock-in amplification, even weak signals of highly dilute…

Atomic Physics · Physics 2017-02-28 Lukas Bruder , Marcel Binz , Frank Stienkemeier

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…

We demonstrate how dynamic correlations of heavy-hole and light-hole excitons in semiconductor quantum wells may be investigated by two dimensional correlation spectroscopy (2DCS). The coherent response to three femtosecond optical pulses…

Mesoscale and Nanoscale Physics · Physics 2007-05-23 Lijun Yang , Igor V. Schweigert , Steven T. Cundiff , Shaul Mukamel

We have realized a hybrid solid-state quantum device in which a single-electron semiconductor double quantum dot is dipole coupled to a superconducting microwave frequency transmission line resonator. The dipolar interaction between the two…

Interactions between particles in quantum many-body systems play a crucial role in determining the electric, magnetic, optical, and thermal properties of the system. The recent progress in the laser-pulse technique has enabled the…

Strongly Correlated Electrons · Physics 2021-09-07 Nguyen Thanh Phuc , Pham Quang Trung

Two-dimensional coherent spectroscopy (2DCS) provides simultaneous measurement of homogeneous and inhomogeneous linewidths through quantitative lineshape analysis. However, conventional lineshape analysis methods assume Gaussian…

We propose a three-pulse coherent ultrafast optical technique that is particularly sensitive to two-exciton correlations. Two Liouville-space pathways for the density matrix contribute to this signal which reveals double quantum coherences…

Mesoscale and Nanoscale Physics · Physics 2009-11-13 Lijun Yang , Shaul Mukamel

We present a quantum sensing technique that utilizes a sequence of $\pi$ pulses to cyclically drive the qubit dynamics along a geodesic path of adiabatic evolution. This approach effectively suppresses the effects of both decoherence noise…

Quantum Physics · Physics 2023-07-21 Ke Zeng , Xiaohui Yu , Martin B. Plenio , Zhen-Yu Wang

Employing electro-optic sampling (EOS) with ultrashort probe pulses, recent experiments showed direct measurements of quantum vacuum fields and their correlations on subcycle timescales. Here, we propose a quantum-enhanced EOS where…

Quantum Physics · Physics 2022-01-12 Stéphane Virally , Patrick Cusson , Denis V. Seletskiy

How atoms and electrons in a molecule move during a chemical reaction and how rapidly energy is transferred to or from the surroundings can be studied with flashes of laser light. However, despite prolonged efforts to develop various…

Chemical Physics · Physics 2022-01-05 JunWoo Kim , Jonggu Jeon , Tai Hyun Yoon , Minhaeng Cho