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Two-dimensional coherent spectroscopy (2DCS) with terahertz radiation offers a promising new avenue for the exploration of many-body phenomena in quantum magnets. This includes the potential diagnosis of fractionalized excitations, for…

Strongly Correlated Electrons · Physics 2024-10-29 Yoshito Watanabe , Simon Trebst , Ciarán Hickey

With recent advances in terahertz (THz) sources and detection, two-dimensional coherent spectroscopy (2DCS), which allows to probe nonlinear responses in a two-frequency plane, now reaches the meV regime relevant for quasiparticle…

Strongly Correlated Electrons · Physics 2025-12-19 Yoshito Watanabe , Simon Trebst , Ciarán Hickey

Two-dimensional coherent spectroscopy (2DCS) is an established method for characterizing molecules and has been proposed in the THz regime as a new tool for probing exotic excitations of quantum magnets; however, the precise nature of the…

Strongly Correlated Electrons · Physics 2025-02-26 Anubhav Srivastava , Stefan Birnkammer , GiBaik Sim , Michael Knap , Johannes Knolle

We present and benchmark a quantum computing approach to calculate the two-dimensional coherent spectrum (2DCS) of high-spin models. Our approach is based on simulating their real-time dynamics in the presence of several magnetic field…

Quantum Physics · Physics 2024-07-02 Martin Mootz , Peter P. Orth , Chuankun Huang , Liang Luo , Jigang Wang , Yong-Xin Yao

We show that the new technique of terahertz 2D coherent spectroscopy is capable of giving qualitatively new information about fractionalized spin systems. For the prototypical example of the transverse field Ising chain, we demonstrate…

Strongly Correlated Electrons · Physics 2021-12-15 Yuan Wan , N. P. Armitage

Two-dimensional correlation spectroscopy (2DCS) based on the nonlinear optical response of excitons to sequences of ultrafast pulses, has the potential to provide some unique insights into carrier dynamics in semiconductors. The most…

Mesoscale and Nanoscale Physics · Physics 2009-11-13 Shaul Mukamel , Rafal Oszwaldowski , Darius Abramavicius

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

We study how sharp signatures of fractionalization emerge in nonlinear spectroscopy experiments on spin liquids with separated energy scales. Our model is that of dipolar-octupolar rare earth pyrochlore materials, prime candidates for…

Strongly Correlated Electrons · Physics 2025-01-22 Mark Potts , Roderich Moessner , Owen Benton

Double-quantum two-dimensional coherent spectroscopy (MDCS) is a powerful optical method that is used to study optical properties of atomic and complex molecular systems and semiconductor materials. Double-quantum 2D spectra and…

Optics · Physics 2020-10-21 Bachana Lomsadze , Steven T. Cundiff

We study electric field induced two-dimensional coherent nonlinear optical spectroscopy (2DCS) in a Kitaev magnet at finite temperature. We show that 2DCS is susceptible to both types of fractional quasiparticles of this quantum…

Strongly Correlated Electrons · Physics 2024-03-15 Wolfram Brenig , Olesia Krupnitska

As optical two-dimensional coherent spectroscopy (2DCS) is extended to a broader range of applications, it is critical to improve the detection sensitivity of optical 2DCS. We developed a fast phase-cycling scheme in a non-collinear optical…

Ultra-fast and multi-dimensional spectroscopy gives a powerful looking glass into the dynamics of molecular systems. In particular two-dimensional electronic spectroscopy (2DES) provides a probe of coherence and the flow of energy within…

Quantum Physics · Physics 2021-03-31 André Anda , Jared H. Cole

Two-dimensional electronic spectroscopy (2DES) is one of the most powerful spectroscopic techniques, capable of attaining a nearly complete picture of a quantum system including its couplings, quantum coherence properties and its real-time…

We show that the nonlinear optical response probed by two-dimensional coherent spectroscopy (2DCS) can discriminate between excitonic and lattice driven order. In the excitonic regime of a realistic model of Ta$_2$NiSe$_5$, the third order…

Strongly Correlated Electrons · Physics 2025-12-23 Jiyu Chen , Jernej Mravlje , Denis Golež , Philipp Werner

Selecting distinct quantum pathways in two-dimensional electronic spectroscopy (2DES) can give particularly deep insights into coherent and incoherent interactions and quantum dynamics in various materials. This includes isolating rephasing…

Calculation of the coherent nonlinear response of a system is essential to correctly interpret results from advanced techniques such as two-dimensional coherent spectroscopy (2DCS). Usually, even for the simplest systems, such calculations…

The dephasing mechanisms of p-shell and s-shell excitons in an InAs self-assembled quantum dot ensemble are examined using two-dimensional coherent spectroscopy (2DCS). 2DCS provides a comprehensive picture of how the energy level structure…

Mesoscale and Nanoscale Physics · Physics 2019-08-16 Takeshi Suzuki , Rohan Singh , Galan Moody , Marc Aßmann , Manfred Bayer , Arne Ludwig , Andreas D. Wieck , and Steven T. Cundiff

Multidimensional coherent spectroscopy (MDCS) has been established in quantum chemistry as a powerful tool for studying the nonlinear response and nonequilibrium dynamics of molecular systems. More recently, the technique has also been…

Strongly Correlated Electrons · Physics 2025-05-12 Jiyu Chen , Philipp Werner

We compute numerically the second and third order nonlinear magnetic susceptibilities of an Ising ladder model in the context of two-dimensional coherent spectroscopy by using the infinite time-evolving block decimation method. The Ising…

Strongly Correlated Electrons · Physics 2023-04-26 Qi Gao , Yang Liu , Haijun Liao , Yuan Wan

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,…

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