Terahertz Circular Dichroism Spectroscopy of Molecular Assemblies and Nanostructures

Choi, Won Jin; Lee, Sang Hyun; Park, Bum Chul; Kotov, Nicholas A.

doi:10.1021/jacs.2c04817

Terahertz Circular Dichroism Spectroscopy of Molecular Assemblies and Nanostructures

Journal Article · Thu Dec 08 23:00:00 EST 2022 · Journal of the American Chemical Society

DOI:https://doi.org/10.1021/jacs.2c04817· OSTI ID:1962479

^[1]; Lee, Sang Hyun ^[2]; Park, Bum Chul ^[2]; ^[2]

University of Michigan, Ann Arbor, MI (United States); Lawrence Livermore National Laboratory (LLNL), Livermore, CA (United States)
University of Michigan, Ann Arbor, MI (United States)

Chemical, physical, biological and materials engineering disciplines use a variety of chiroptical spectroscopies to probe geometrical and optical asymmetry in molecules and particles. Electronic (ECD) and vibrational (VCD) circular dichroism are the most common of these techniques and collectively enable the studies of electronic and vibronic transitions with energies between 0.1 and 5.0 eV. The vibrational states with characteristic energies in the range of 0.001–0.01 eV carry valuable information about concerted intermolecular motions in molecules and crystals involving multiple atoms. These vibronic transitions located in the terahertz (THz) part of the spectrum become increasingly more important for the chemistry, physics, and biology of complex molecules and materials However, the methodology and hardware of THz circular dichroism (TCD) are much less developed than the chiroptical spectroscopies for ultraviolet, visible, near- and mid infrared photons. In this report we provide theoretical foundations, practical implementations, comparative assessments, and exemplary applications of TCD spectroscopy. We show that the sign, intensity, and position of TCD peaks are highly sensitive to the three-dimensional structure and long-range organization of molecular crystals, which offer unique capabilities to study (bio) molecules, their crystals, and nanoscale assemblies and apply the novel data processing methodologies. TCD also offers a convenient toolbox to identify new physical phenomena, such as chiral phonons and their propagation in nanostructured matter. We also discuss the major challenges, emerging opportunities and promising research directions, including broad investigation of chiral phonons observed in chiral (nano) crystals and emerging machine learning methodologies for TCD in biological and nanoscale structures. Ubiquity of low-frequency vibrations with rotational components in biomolecular structures, combined with sharpness of peaks in TCD spectra, enables a variety of technological translations.

View Accepted Manuscript (DOE)

Research Organization:: Lawrence Livermore National Laboratory (LLNL), Livermore, CA (United States)

Sponsoring Organization:: USDOE National Nuclear Security Administration (NNSA); USDOE Laboratory Directed Research and Development (LDRD) Program; Vannevar Bush DoD Fellowship; US Department of Navy Office of Naval Research (ONR); US Air Force Office of Scientific Research (AFOSR)

Grant/Contract Number:: AC52-07NA27344

OSTI ID:: 1962479

Report Number(s):: LLNL-JRNL-840148; 1060993

Journal Information:: Journal of the American Chemical Society, Journal Name: Journal of the American Chemical Society Journal Issue: 50 Vol. 144; ISSN 0002-7863

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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THz Characterization of DNA Four-Way Junction and Its Components Lvovska, Maryna I.; Seeman, Nadrian C.; Sha, Ruojie IEEE Transactions on Nanotechnology, Vol. 9, Issue 5 https://doi.org/10.1109/TNANO.2010.2049498	journal	September 2010
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Dimensionality Reduction for Identification of Hepatic Tumor Samples Based on Terahertz Time-Domain Spectroscopy Liu, Haishun; Zhang, Zhenwei; Zhang, Xin IEEE Transactions on Terahertz Science and Technology, Vol. 8, Issue 3 https://doi.org/10.1109/TTHZ.2018.2813085	journal	May 2018
A kinetic study of β-lactoglobulin amyloid fibril formation promoted by urea Hamada, Daizo; Dobson, Christopher M. Protein Science, Vol. 11, Issue 10 https://doi.org/10.1110/ps.0217702	journal	April 2009
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