The Application of Tailored Fields for Studying Chirality and Symmetry
Abstract: Ultrashort laser pulses pose unique tools to trigger and probe the fastest charge dynamics in matter, allowing the investigation of fundamental physical phenomena with unprecedented resolution in space, time, and energy. One of the most fascinating opportunities that ultrashort pulses offer is the possibility of modulating and investigating symmetries by tailoring the properties of the laser beam in the spatial and polarization domains, effectively controlling symmetry breaking on multiple levels. In particular, this allows probing chiral matter and ultrafast chiral dynamics. In recent years, the development of highly sensitive approaches for studying chirality has been a hot topic in physics and chemistry that has developed largely separately from the field of tailored light. This perspective discusses the individual and joint evolution of these fields with an emphasis on how the fields have already cross-fertilized, opening new opportunities in science. We outline a future outlook of how the topics are expected to fully merge and mutually evolve, emphasizing outstanding open issues.
- P. Agostini and L. F. DiMauro, The physics of attosecond light pulses, Reports on Progress in Physics 67, 813 (2004).
- The Nobel Prize in Physics for 2023 was awarded to Pierre Agostini, Ferenc Krausz and Anne L’Huillier for experimental methods of generating attosecond pulses of light for the investigation of electron dynamics in matter: https://www.nobelprize.org/prizes/physics/2023/summary/, .
- P. Peng, C. Marceau, and D. M. Villeneuve, Attosecond imaging of molecules using high harmonic spectroscopy, Nature Reviews Physics 1, 144 (2019).
- P. M. Kraus and H. J. Wörner, Perspectives of attosecond spectroscopy for the understanding of fundamental electron correlations, Angewandte Chemie International Edition 57, 5228 (2018).
- I. S. Wahyutama, T. Sato, and K. L. Ishikawa, Time-dependent multiconfiguration self-consistent-field study on resonantly enhanced high-order harmonic generation from transition-metal elements, Phys. Rev. A 99, 063420 (2019).
- A. S. Kheifets, The attoclock and the tunneling time debate, Journal of Physics B: Atomic, Molecular and Optical Physics 53, 072001 (2020).
- L. Feng and T. Chu, Nuclear signatures on the molecular harmonic emission and the attosecond pulse generation, The Journal of Chemical Physics 136, 054102 (2012).
- W. Demtröder, Laser Spectroscopy: Basic Concepts and Instrumentation (Springer, 2002).
- B. E. A. Saleh and M. C. Teich, Fundamentals of Photonics (John Wiley & Sons, Ltd, 2007).
- A. M. Weiner, Ultrafast Optics (John Wiley & Sons, Ltd, 2011).
- O. Neufeld, D. Podolsky, and O. Cohen, Floquet group theory and its application to selection rules in harmonic generation, Nature Communications 10, 405 (2019a).
- D. B. Milošević, W. Becker, and R. Kopold, Generation of circularly polarized high-order harmonics by two-color coplanar field mixing, Phys. Rev. A 61, 063403 (2000).
- S. Long, W. Becker, and J. K. McIver, Model calculations of polarization-dependent two-color high-harmonic generation, Physical Review A 52, 2262 (1995).
- D. Habibović and D. B. Milošević, Ellipticity of high-order harmonics generated by aligned homonuclear diatomic molecules exposed to an orthogonal two-color laser field, Photonics 7, 10.3390/photonics7040110 (2020).
- D. Habibović, W. Becker, and D. B. Milošević, Symmetries and selection rules of the spectra of photoelectrons and high-order harmonics generated by field-driven atoms and molecules, Symmetry 13, 10.3390/sym13091566 (2021).
- D. K. Kondepudi and D. J. Durand, Chiral asymmetry in spiral galaxies?, Chirality 13, 351 (2001).
- F. Maderspacher, Snail chirality: The unwinding, Current Biology 26, R215 (2016).
- D. Griffiths, Introduction to Elementary Particles (John Wiley & Sons, New York, USA, 2008).
- D. M. Bishop, Group Theory and Chemistry (Dover Publications, New York, USA, 2012).
- I. Erez, E. R. Wallach, and Y. Shagam, Simultaneous enantiomer-resolved ramsey spectroscopy scheme for chiral molecules, Phys. Rev. X 13, 041025 (2023).
- M. Quack, How important is parity violation for molecular and biomolecular chirality?, Angewandte Chemie International Edition 41, 4618 (2002).
- G. J. Simpson, Molecular origins of the remarkable chiral sensitivity of second-order nonlinear optics, ChemPhysChem 5, 1301 (2004).
- P. Fischer and F. Hache, Nonlinear optical spectroscopy of chiral molecules, Chirality 17, 421 (2005).
- D. Patterson and J. M. Doyle, Sensitive chiral analysis via microwave three-wave mixing, Phys. Rev. Lett. 111, 023008 (2013).
- D. Patterson, M. Schnell, and J. M. Doyle, Enantiomer-specific detection of chiral molecules via microwave spectroscopy, Nature 497, 475 (2013).
- M. H. M. Janssen and I. Powis, Detecting chirality in molecules by imaging photoelectron circular dichroism, Phys. Chem. Chem. Phys. 16, 856 (2014).
- K. A. Forbes and D. L. Andrews, Optical orbital angular momentum: twisted light and chirality, Opt. Lett. 43, 435 (2018).
- D. Baykusheva and H. J. Wörner, Chiral discrimination through bielliptical high-harmonic spectroscopy, Phys. Rev. X 8, 031060 (2018).
- D. Ayuso, New opportunities for ultrafast and highly enantio-sensitive imaging of chiral nuclear dynamics enabled by synthetic chiral light, Phys. Chem. Chem. Phys. 24, 10193 (2022).
- K. R. Hamilton, H. W. van der Hart, and A. C. Brown, Pulse-shape control of two-color interference in high-order-harmonic generation, Phys. Rev. A 95, 013408 (2017).
- D. M. Reich and L. B. Madsen, Illuminating molecular symmetries with bicircular high-order-harmonic generation, Phys. Rev. Lett. 117, 133902 (2016).
- Y. Li, L. Feng, and Y. Qiao, Selective enhancement of single-order and two-order harmonics from He atom via two-color and three-color laser fields, Chemical Physics 527, 110497 (2019).
- D. G. Grier, A revolution in optical manipulation, Nature 424, 810 (2003).
- N. B. Simpson, L. Allen, and M. J. Padgett, Optical tweezers and optical spanners with Laguerre–Gaussian modes, Journal of Modern Optics 43, 2485 (1996).
- G. Vicidomini, P. Bianchini, and A. Diaspro, STED super-resolved microscopy, Nature Methods 15, 173 (2018).
- J. Torres, Twisted photons : applications of light with orbital angular momentum (Wiley-VCH Verlag, Weinheim, 2011).
- A. Sakdinawat and Y. Liu, Soft-x-ray microscopy using spiral zone plates, Optics Letters 32, 2635 (2007).
- M. van Veenendaal and I. McNulty, Prediction of strong dichroism induced by X rays carrying orbital momentum, Physical Review Letters 98, 157401 (2007).
- M. R. Dennis and H. H. Wills, Topological singularities in wave fields, in Topological Singularities in Wave Fields (2001).
- W. Whewell, Essay towards a first approximation to a map of cotidal lines, Philosophical Transactions of the Royal Society , 147–236 (1833).
- P. A. M. Dirac, Quantised singularities in the electromagnetic field, Proceedings of The Royal Society A: Mathematical, Physical and Engineering Sciences 133, 60 (1931).
- J. F. Nye and M. V. Berry, Dislocations in wave trains, Proceedings of the Royal Society of London. Series A, Mathematical and Physical Sciences 336, 165 (1974).
- A. Tomita and R. Y. Chiao, Observation of Berry’s topological phase by use of an optical fiber, Phys. Rev. Lett. 57, 937 (1986).
- R. Y. Chiao and Y.-S. Wu, Manifestations of Berry’s topological phase for the photon, Phys. Rev. Lett. 57, 933 (1986).
- P. Coullet, L. Gil, and F. Rocca, Optical vortices, Optics Communications 73, 403 (1989).
- Q. Zhan, Cylindrical vector beams: from mathematical concepts to applications, Adv. Opt. Photon. 1, 1 (2009).
- A. M. Beckley, T. G. Brown, and M. A. Alonso, Full Poincaré beams, Opt. Express 18, 10777 (2010).
- R. W. Hellwarth and P. Nouchi, Focused one-cycle electromagnetic pulses, Phys. Rev. E 54, 889 (1996).
- I. Freund, Optical Möbius strips in three-dimensional ellipse fields: I. lines of circular polarization, Optics Communications 283, 1 (2010).
- The Nobel Prize in Physics for 2016 was shared by David J. Thouless, F. Duncan M. Haldane and J. Michael Kosterlitz for theoretical discoveries of topological phase transitions and topological phases of matter: https://www.nobelprize.org/prizes/physics/2016/summary/, .
- M. S. Rudner and N. H. Lindner, Band structure engineering and non-equilibrium dynamics in Floquet topological insulators, Nature Reviews Physics 2, 229 (2020).
- A. M. Yao and M. J. Padgett, Orbital angular momentum: origins, behavior and applications, Advances in Optics and Photonics 3, 161 (2011).
- D. J. Thouless, Wannier functions for magnetic sub-bands, Journal of Physics C: Solid State Physics 17, L325 (1984).
- T. Thonhauser and D. Vanderbilt, Insulator/chern-insulator transition in the haldane model, Phys. Rev. B 74, 235111 (2006).
- M. G. Silveirinha, Bulk-edge correspondence for topological photonic continua, Phys. Rev. B 94, 205105 (2016).
- I. Dreissigacker and M. Lein, Photoelectron circular dichroism of chiral molecules studied with a continuum-state-corrected strong-field approximation, Phys. Rev. A 89, 053406 (2014).
- D. Habibović, W. Becker, and D. B. Milošević, High-order harmonic generation by aligned heteronuclear diatomic molecules in an orthogonally polarized two-color laser field, The European Physical Journal D 75, 122 (2021).
- D. Habibović, W. Becker, and D. B. Milošević, High-order harmonic generation by two linearly polarized laser fields with an arbitrary angle between their polarization axes, Phys. Rev. A 106, 023119 (2022).
- D. B. Milošević and D. Habibović, High-order harmonic generation by aligned homonuclear diatomic cations, Phys. Chem. Chem. Phys. 25, 28848 (2023).
- Y. Tang and A. E. Cohen, Optical chirality and its interaction with matter, Phys. Rev. Lett. 104, 163901 (2010).
- Y. Tang and A. E. Cohen, Enhanced enantioselectivity in excitation of chiral molecules by superchiral light, Science 332, 333 (2011).
- T. Kanai, S. Minemoto, and H. Sakai, Ellipticity dependence of high-order harmonic generation from aligned molecules, Phys. Rev. Lett. 98, 053002 (2007).
- D. Ayuso, A. F. Ordonez, and O. Smirnova, Ultrafast chirality: the road to efficient chiral measurements, Phys. Chem. Chem. Phys. 24, 26962 (2022).
- P. Laur, Comprehensive Chiroptical Spectroscopy (John Wiley & Sons, Ltd, 2012).
- R. P. Cameron, A. M. Yao, and S. M. Barnett, Diffraction gratings for chiral molecules and their applications, The Journal of Physical Chemistry A 118, 3472 (2014).
- S. Eibenberger, J. Doyle, and D. Patterson, Enantiomer-specific state transfer of chiral molecules, Phys. Rev. Lett. 118, 123002 (2017).
- L. Rego, O. Smirnova, and D. Ayuso, Tilting light’s polarization plane to spatially separate the ultrafast nonlinear response of chiral molecules, Nanophotonics 12, 2873 (2023).
- O. Neufeld and O. Cohen, Optical chirality in nonlinear optics: Application to high harmonic generation, Phys. Rev. Lett. 120, 133206 (2018).
- M. Leibscher, T. F. Giesen, and C. P. Koch, Principles of enantio-selective excitation in three-wave mixing spectroscopy of chiral molecules, The Journal of Chemical Physics 151, 014302 (2019).
- O. Neufeld, M. Even Tzur, and O. Cohen, Degree of chirality of electromagnetic fields and maximally chiral light, Phys. Rev. A 101, 053831 (2020).
- O. Neufeld and O. Cohen, Unambiguous definition of handedness for locally chiral light, Phys. Rev. A 105, 023514 (2022).
- L. Rego and D. Ayuso, Structuring the local handedness of synthetic chiral light: global chirality versus polarization of chirality, New Journal of Physics 25, 093005 (2023).
- D. Green and K. A. Forbes, Optical chirality of vortex beams at the nanoscale, Nanoscale 15, 540 (2023).
- K. A. Forbes, Optical helicity of unpolarized light, Phys. Rev. A 105, 023524 (2022).
- A. Ordóñez, P. Vindel-Zandbergen, and D. Ayuso, Chiral coherent control of electronic population transfer: towards all-optical and highly enantioselective photochemistry (2023), arXiv:2309.02392 [physics.chem-ph] .
- A. F. Ordonez and O. Smirnova, Propensity rules in photoelectron circular dichroism in chiral molecules. i. chiral hydrogen, Phys. Rev. A 99, 043416 (2019).
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