Multidimensional Terahertz Probes of Quantum Materials

Abstract

Multidimensional spectroscopy has a long history originating from nuclear magnetic resonance, and has now found widespread application at infrared and optical frequencies as well. However, the energy scales of traditional multidimensional probes have been ill-suited for studying quantum materials. Recent technological advancements have now enabled extension of these multidimensional techniques to the terahertz frequency range, in which collective excitations of quantum materials are typically found. This Perspective introduces the technique of two-dimensional terahertz spectroscopy (2DTS) and the unique physics of quantum materials revealed by 2DTS spectra, accompanied by a selection of the rapidly expanding experimental and theoretical literature. While 2DTS has so far been primarily applied to quantum materials at equilibrium, we provide an outlook for its application towards understanding their dynamical non-equilibrium states and beyond.

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• An optically stimulated superconducting-like phase in K3C60 far above equilibrium Tc
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• Terahertz field-driven magnon upconversion in an antiferromagnet
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• Quantum Coherence Tomography of Lightwave Controlled Superconductivity
• Coherent cyclotron motion beyond Kohn's theorem
• Simultaneous Existence of Confined and Delocalized Vibrational Modes in Colloidal Quantum Dots
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Cited by in corpus (13)

• Unlocking Quantum Control and Multi-Order Correlations via Terahertz Two-Dimensional Coherent Spectroscopy
• Extracting Nonlinear Dynamical Response Functions from Time Evolution
• Multidimensional coherent spectroscopy of correlated lattice systems
• Fundamentals of heterodyne wave mixing spectroscopy: a tutorial
• Sparse Optimization of Two-Dimensional Terahertz Spectroscopy
• Unifying Measurement Schemes in 2-D Terahertz Spectroscopy
• Pulsed Magnetophononics in Gapped Quantum Magnets
• Probing Complex Decoherence Processes in Materials for Quantum Applications
• Phonon spectrum in the spin-Peierls phase of CuGeO${}_3$
• Two-dimensional coherent spectroscopy of disordered superconductors in the narrow-band and broad-band limits
• Momentum-resolved two-dimensional spectroscopy as a probe of nonlinear quantum field dynamics
• Tangent equations of motion for nonlinear response functions
• Two-dimensional THz spectroscopy in electronic systems: a many-body diagrammatic approach