Mapping 
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 Phonon-Polariton Nonlinearities with 2D THz-THz-Raman Spectroscopy

Lin, Haw-Wei; Mead, Griffin; Blake, G. A.

doi:10.1103/physrevlett.129.207401

Cited by 14 publications

(4 citation statements)

References 39 publications

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“…Theoretical simulations by Ito and Tanimura 55 predicted such spectral features and assigned them to both mechanical and electrical anharmonic coupling between the said vibrational modes. Similarly, THz-THz-Raman spectroscopy recently revealed signatures of anharmonic coupling between phonons of ionic solid LiNbO 3 56 . Finally, Raman-THz-THz and THz-Raman-THz spectroscopies have been used to study the inhomogeneity of liquid water and aqueous solutions 57 , 58 , as well as the coupling among intermolecular and intramolecular modes in liquid and solid bromoform 59 , 60 .…”

Section: Introductionmentioning

confidence: 94%

Two-dimensional infrared-Raman spectroscopy as a probe of water’s tetrahedrality

Begušić

Blake

2023

Nat Commun

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Two-dimensional spectroscopic techniques combining terahertz (THz), infrared (IR), and visible pulses offer a wealth of information about coupling among vibrational modes in molecular liquids, thus providing a promising probe of their local structure. However, the capabilities of these spectroscopies are still largely unexplored due to experimental limitations and inherently weak nonlinear signals. Here, through a combination of equilibrium-nonequilibrium molecular dynamics (MD) and a tailored spectrum decomposition scheme, we identify a relationship between the tetrahedral order of liquid water and its two-dimensional IR-IR-Raman (IIR) spectrum. The structure-spectrum relationship can explain the temperature dependence of the spectral features corresponding to the anharmonic coupling between low-frequency intermolecular and high-frequency intramolecular vibrational modes of water. In light of these results, we propose new experiments and discuss the implications for the study of tetrahedrality of liquid water.

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Section: Introductionmentioning

confidence: 94%

Two-dimensional infrared-Raman spectroscopy as a probe of water’s tetrahedrality

Begušić

Blake

2023

Nat Commun

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“…Electric fields are central to many aspects of the physical sciences, including chemical reactivity, cell signaling, and more. − Over 100 years ago, Stark reported that electric fields can affect how atoms and molecules interact with light; in particular, he observed that degenerate spectral lines in hydrogen are split into multiple components in a strong electric field . This phenomenon is now called the Stark effect and provides useful information across much of the electromagnetic spectrum. − For example, electric fields almost fully break degeneracy in gas-phase microwave rotational spectroscopy, facilitating detailed spectral assignments that provide fundamental understanding of molecular structure and geometry. − The electronic Stark effect is the physical basis for sensing cellular potentials with electrochromic dyes, whose fluorescence emission spectra are influenced by the local electric field .…”

mentioning

confidence: 99%

Nitrile Vibrational Lifetimes as Probes of Local Electric Fields

Kocheril,

Wang,

Lee

et al. 2024

J. Phys. Chem. Lett.

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Optical measurements of electric fields have wide-ranging applications in the fields of chemistry and biology. Previously, such measurements focused on shifts in intensity or frequency. Here, we show that nitrile vibrational lifetimes can report local electric fields through ultrasensitive picosecond mid-infrared–near-infrared double-resonance fluorescence spectro-microscopy on Rhodamine 800. Using a robust convolution fitting approach, we observe that the nitrile vibrational lifetimes are strongly linearly correlated (R 2 = 0.841) with solvent reaction fields. Supported by density functional theory, we rationalize this trend through a doorway model of intramolecular vibrational energy redistribution. This work provides new fundamental insights into the nature of vibrational energy flow in large polyatomic molecular systems and establishes a theoretical basis for electric field sensing with vibrational lifetimes, offering a new experimental dimension for probing intracellular electrostatics.

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“…It provides a detailed two-dimensional excitation map of two frequencies that can be used to extract the nature, couplings and lifetimes of elementary excitations. This technique has long been used in the radio and optical frequency range and has only recently been extended to terahertz (THz) frequencies, which are ideal for the study of excitations and collective modes in quantum materials [15][16][17][18][19][20][21][22].…”

mentioning

confidence: 99%

Probing Majorana wavefunctions in Kitaev honeycomb spin liquids with second-order two-dimensional spectroscopy

Qiang¹,

Quito²,

Trevisan³

et al. 2023

Preprint

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Two-dimensional coherent terahertz spectroscopy (2DCS) emerges as a valuable tool to probe the nature, couplings, and lifetimes of excitations in quantum materials. It thus promises to identify unique signatures of spin liquid states in quantum magnets by directly probing properties of their exotic fractionalized excitations. Here, we calculate the second-order 2DCS of the Kitaev honeycomb model and demonstrate that distinct spin liquid fingerprints appear already in this lowest-order nonlinear response χ(2) yzx(ω1, ω2) when using crossed light polarizations. We further relate the offdiagonal 2DCS peaks to the localized nature of the matter Majorana excitations trapped by Z2 flux excitations and show that 2DCS thus directly probes the inverse participation ratio of Majorana wavefunctions. By providing experimentally observable features of spin liquid states in the 2D spectrum, our work can guide future 2DCS experiments on Kitaev magnets.

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Mapping LiNbO3 Phonon-Polariton Nonlinearities with 2D THz-THz-Raman Spectroscopy

Cited by 14 publications

References 39 publications

Two-dimensional infrared-Raman spectroscopy as a probe of water’s tetrahedrality

Two-dimensional infrared-Raman spectroscopy as a probe of water’s tetrahedrality

Nitrile Vibrational Lifetimes as Probes of Local Electric Fields

Probing Majorana wavefunctions in Kitaev honeycomb spin liquids with second-order two-dimensional spectroscopy

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