R. Noyori, Asymmetric Catalysis: Science and Opportunities (Nobel Lecture) Copyright?? The Nobel Foundation 2002. We thank the Nobel Foundation, Stockholm, for permission to print this lecture., Angewandte Chemie International Edition, vol.41, issue.12, pp.2008-2022, 2002.
DOI : 10.1002/1521-3773(20020617)41:12<2008::AID-ANIE2008>3.0.CO;2-4

O. Mcconnell, A. Bach, C. Balibar, N. Byrne, Y. Cai et al., Enantiomeric separation and determination of absolute stereochemistry of asymmetric molecules in drug discovery???Building chiral technology toolboxes, Chirality, vol.133, issue.9, pp.658-682, 2007.
DOI : 10.1002/chir.20399

J. Zhang, M. T. Albelda, Y. Liu, and J. W. Canary, Chiral nanotechnology, Chirality, vol.126, issue.7, pp.404-420, 2005.
DOI : 10.1002/chir.20178

L. M. Haupert and G. J. Simpson, Chirality in Nonlinear Optics, Annual Review of Physical Chemistry, vol.60, issue.1, pp.345-365, 2009.
DOI : 10.1146/annurev.physchem.59.032607.093712

E. U. Condon, Theories of Optical Rotatory Power, Reviews of Modern Physics, vol.9, issue.4, pp.432-457, 1937.
DOI : 10.1103/RevModPhys.9.432

L. A. Nafie, Vibrational Optical Activity: Principles and Applications, Molecular Light Scattering and Optical Activity, 2004.
DOI : 10.1002/9781119976516

W. R. Mason, Practical Guide to Magnetic Circular Dichroism Spectroscopy, Chem. Soc. Rev, vol.35, pp.39-51, 2006.
DOI : 10.1002/9780470139233

A. Rizzo and H. Agren, Ab initio study of the circular intensity difference in electric-field-induced second harmonic generation of chiral natural amino acids, Phys. Chem. Chem. Phys., vol.11, issue.4, pp.1198-1207, 2013.
DOI : 10.1039/C2CP42792C

P. Fischer and F. Hache, Nonlinear optical spectroscopy of chiral molecules, Chirality, vol.399, issue.300, pp.421-437, 2005.
DOI : 10.1002/chir.20179
URL : https://hal.archives-ouvertes.fr/hal-00829236

N. Ji, V. Ostroverkhov, M. Belkin, Y. J. Shiu, and Y. R. Shen, Toward Chiral Sum-Frequency Spectroscopy, Journal of the American Chemical Society, vol.128, issue.27, pp.8845-8848, 2006.
DOI : 10.1021/ja060888c

R. Cameron and G. C. Tabisz, Observation of two-photon optical rotation by molecules, Molecular Physics, vol.125, issue.2, pp.159-164, 1997.
DOI : 10.1016/1011-1344(90)85055-2

C. Toro, L. De-boni, N. Lin, F. Santoro, A. Rizzo et al., Two-Photon Absorption Circular Dichroism: A New Twist in Nonlinear Spectroscopy, Chemistry - A European Journal, vol.111, issue.736, pp.3504-3509, 2010.
DOI : 10.1002/chem.200902286

I. Tinoco, Two???photon circular dichroism, The Journal of Chemical Physics, vol.62, issue.3, pp.1006-1009, 1975.
DOI : 10.1063/1.430566

E. A. Power, Two???photon circular dichroism, The Journal of Chemical Physics, vol.63, issue.4, pp.1348-1350, 1975.
DOI : 10.1063/1.431521

F. E. Hernández and A. Rizzo, Two-Photon Polarization Dependent Spectroscopy in Chirality: A Novel Experimental-Theoretical Approach to Study Optically Active Systems, Molecules, vol.16, issue.12, pp.3315-3337, 2011.
DOI : 10.3390/molecules16043315

W. Denk, J. Strickler, and W. Webb, Two-photon laser scanning fluorescence microscopy, Science, vol.248, issue.4951, pp.73-76, 1990.
DOI : 10.1126/science.2321027

Y. Vesga, C. Diaz, M. Higgs, and F. E. Hernandez, Two-photon circular dichroism of molecular structures simulating l-tryptophan residues in proteins with secondary structures, Chemical Physics Letters, vol.601, pp.6-12, 2014.
DOI : 10.1016/j.cplett.2014.03.083

L. De-boni, C. Toro, and F. E. Hernandez, Synchronized double L-scan technique for the simultaneous measurement of polarization-dependent two-photon absorption in chiral molecules, Optics Letters, vol.33, issue.24, pp.2958-2960, 2008.
DOI : 10.1364/OL.33.002958

K. E. Gunde and F. S. Richardson, Fluorescence-detected two-photon circular dichroism of Gd3+ in trigonal Na3[Gd(C4H4O5)3] ?? 2NaClO4 ?? 6H2O, Chemical Physics, vol.194, issue.1, pp.195-206, 1995.
DOI : 10.1016/0301-0104(95)00025-J

M. Savoini, X. Wu, M. Celebrano, J. Ziegler, P. Biagioni et al., Circular Dichroism Probed by Two-Photon Fluorescence Microscopy in Enantiopure Chiral Polyfluorene Thin Films, Journal of the American Chemical Society, vol.134, issue.13, pp.5832-5835, 2012.
DOI : 10.1021/ja209916y

C. Díaz, L. Echevarria, A. Rizzo, and F. E. Hernández, Two-Photon Circular Dichroism of an Axially Dissymmetric Diphosphine Ligand with Strong Intramolecular Charge Transfer, The Journal of Physical Chemistry A, vol.118, issue.5, pp.940-946, 2014.
DOI : 10.1021/jp4119265

C. Díaz, L. Echevarria, and F. E. Hernández, Conformational Study of an Axially Chiral Salen Ligand in Solution using Two-Photon Circular Dichroism and the Fragment-Recombination Approach, The Journal of Physical Chemistry A, vol.117, issue.35, pp.8416-8426, 2013.
DOI : 10.1021/jp4065714

C. Diaz, N. Lin, C. Toro, R. Passier, A. Rizzo et al., The Effect of the ??-Electron Delocalization Curvature on the Two-Photon Circular Dichroism of Molecules with Axial Chirality, The Journal of Physical Chemistry Letters, vol.3, issue.13, pp.1808-1813, 2012.
DOI : 10.1021/jz300577e

T. J. Wigglesworth, D. Sud, T. B. Norsten, V. S. Lekhi, and N. R. Branda, Chiral Discrimination in Photochromic Helicenes, Journal of the American Chemical Society, vol.127, issue.20, pp.7272-7273, 2005.
DOI : 10.1021/ja050190j

M. T. Reetz and S. Sostmann, 2,15-Dihydroxy-hexahelicene (HELIXOL): synthesis and use as an enantioselective fluorescent sensor, Tetrahedron, vol.57, issue.13, pp.2515-2520, 2001.
DOI : 10.1016/S0040-4020(01)00077-1

J. E. Field, G. Muller, J. P. Riehl, and D. Venkataraman, Circularly Polarized Luminescence from Bridged Triarylamine Helicenes, Journal of the American Chemical Society, vol.125, issue.39, pp.11808-11809, 2003.
DOI : 10.1021/ja035626e

T. Verbiest, S. V. Elshocht, M. Kauranen, L. Hellemans, J. Snauwaert et al., Strong Enhancement of Nonlinear Optical Properties Through Supramolecular Chirality, Science, vol.282, issue.5390, pp.913-915, 1998.
DOI : 10.1126/science.282.5390.913

T. Verbiest, S. Sioncke, A. Persoons, L. Vyklicky, and T. J. Katz, Electric-Field-Modulated Circular-Difference Effects in Second-Harmonic Generation from a Chiral Liquid Crystal, Angewandte Chemie International Edition, vol.41, issue.20, pp.3882-3884, 2002.
DOI : 10.1002/1521-3773(20021018)41:20<3882::AID-ANIE3882>3.0.CO;2-C

J. Mí?ek, F. Eplý, I. Stará, and M. Ichý, A Straightforward Route to Helically Chiral N-Heteroaromatic Compounds: Practical Synthesis of Racemic 1,14-Diaza[5]helicene and Optically Pure 1- and 2-Aza[6]helicenes, Angewandte Chemie International Edition, vol.43, issue.17, pp.3188-3191, 2008.
DOI : 10.1002/anie.200705463

M. E. Moussa, M. Srebro, E. Anger, N. Vanthuyne, C. Roussel et al., Chiroptical Properties of Carbo[6]Helicene Derivatives Bearing Extended ??-Conjugated Cyano Substituents, Chirality, vol.18, issue.8, pp.455-465, 2013.
DOI : 10.1002/chir.22201
URL : https://hal.archives-ouvertes.fr/hal-00878615

B. Jansik, A. Rizzo, and H. Agren, Response theory calculations of two-photon circular dichroism, Chemical Physics Letters, vol.414, issue.4-6, pp.461-467, 2005.
DOI : 10.1016/j.cplett.2005.08.114

B. Jansík, A. Rizzo, and H. Agren, Ab Initio Study of the Two-Photon Circular Dichroism in Chiral Natural Amino Acids, The Journal of Physical Chemistry B, vol.111, issue.2, pp.446-460, 2007.
DOI : 10.1021/jp0653555

N. Lin, F. Santoro, X. Zhao, A. Rizzo, and V. Barone, )-(+)-3-Methylcyclopentanone: A Theoretical Study, The Journal of Physical Chemistry A, vol.112, issue.48, pp.12401-12411, 2008.
DOI : 10.1021/jp8064695

M. Guillaume, K. Ruud, A. Rizzo, S. Monti, Z. Lin et al., )-Tryptophan, The Journal of Physical Chemistry B, vol.114, issue.19, pp.6500-6512, 2010.
DOI : 10.1021/jp1004659

E. Runge and E. K. Gross, Density-Functional Theory for Time-Dependent Systems, Physical Review Letters, vol.52, issue.12, pp.997-1000, 1984.
DOI : 10.1103/PhysRevLett.52.997

A. D. Becke, Density-functional exchange-energy approximation with correct asymptotic behavior, Physical Review A, vol.38, issue.6, pp.3098-3100, 1988.
DOI : 10.1103/PhysRevA.38.3098

A. D. Becke, Density???functional thermochemistry. III. The role of exact exchange, The Journal of Chemical Physics, vol.98, issue.7, pp.5648-5652, 1993.
DOI : 10.1063/1.464913

C. Lee, W. Yang, and R. G. Parr, Development of the Colle-Salvetti correlation-energy formula into a functional of the electron density, Physical Review B, vol.37, issue.2, pp.785-789, 1988.
DOI : 10.1103/PhysRevB.37.785

R. Krishnan, J. S. Binkley, R. Seeger, and J. A. Pople, Self???consistent molecular orbital methods. XX. A basis set for correlated wave functions, The Journal of Chemical Physics, vol.72, issue.1, pp.650-654, 1980.
DOI : 10.1063/1.438955

T. Clark, J. Chandrasekhar, G. W. Spitznagel, and P. V. Schleyer, Efficient diffuse function-augmented basis sets for anion calculations. III. The 3-21+G basis set for first-row elements, Li-F, Journal of Computational Chemistry, vol.101, issue.3, pp.294-301, 1983.
DOI : 10.1002/jcc.540040303

J. Tomasi, B. Mennucci, and R. Cammi, Quantum Mechanical Continuum Solvation Models, Chemical Reviews, vol.105, issue.8, pp.2999-3093, 2005.
DOI : 10.1021/cr9904009

T. Yanai, D. P. Tew, and N. C. Handy, A new hybrid exchange???correlation functional using the Coulomb-attenuating method (CAM-B3LYP), Chemical Physics Letters, vol.393, issue.1-3, pp.51-57, 2004.
DOI : 10.1016/j.cplett.2004.06.011

M. A. Marques, N. T. Maitra, F. M. Nogueira, E. K. Gross, A. Rubio et al., Fundamentals of time-dependent density functional theory, Springer, 2012. 56. C. A. Ullrich, Time-dependent density-functional theory: concepts and applications, 2011.

S. Hirata and M. Head-gordon, Time-dependent density functional theory for radicals, Chemical Physics Letters, vol.302, issue.5-6, pp.375-382, 1999.
DOI : 10.1016/S0009-2614(99)00137-2

J. Olsen and P. Jo, Linear and nonlinear response functions for an exact state and for an MCSCF state, The Journal of Chemical Physics, vol.82, issue.7, pp.3235-3264, 1985.
DOI : 10.1063/1.448223

V. A. Rassolov, J. A. Pople, M. A. Ratner, and T. L. Windus, basis set for atoms K through Zn, The Journal of Chemical Physics, vol.109, issue.4, pp.1223-1229, 1998.
DOI : 10.1063/1.476673

R. A. Kendall, T. H. Dunning, and R. J. Harrison, Electron affinities of the first???row atoms revisited. Systematic basis sets and wave functions, Computational Strategies for Spectroscopy, pp.6796-6806, 1992.
DOI : 10.1063/1.462569

T. Thirunamachandran and D. P. Craig, Molecular Quantum Electrodynamics, An Introduction to Radiation Molecule Interaction, J. Chem. Phys, vol.55, pp.2789-2796, 1971.

R. R. Birge and B. M. Pierce, A theoretical analysis of the two-photon properties of linear polyenes and the visual chromophores, The Journal of Chemical Physics, vol.70, issue.1, pp.165-178, 1979.
DOI : 10.1063/1.437217

K. D. Bonin and T. J. Mcilrath, Two-photon electric-dipole selection rules, Journal of the Optical Society of America B, vol.1, issue.1, pp.52-55, 1984.
DOI : 10.1364/JOSAB.1.000052

F. E. Hernandez, K. D. Belfield, I. Cohanoschi, M. Balu, and K. J. Schafer, Three- and four-photon absorption of a multiphoton absorbing fluorescent probe, Applied Optics, vol.43, issue.28, pp.5394-5398, 2004.
DOI : 10.1364/AO.43.005394

M. A. Nascimento, The polarization dependence of two-photon absorption rates for randomly oriented molecules, Chemical Physics, vol.74, issue.1, pp.51-66, 1983.
DOI : 10.1016/0301-0104(83)80007-X

M. M. Alam, M. Chattopadhyaya, S. Chakrabarti, and A. Rizzo, On the origin of the very strong two-photon activity of squaraine dyes ??? a standard/damped response theory study, Physical Chemistry Chemical Physics, vol.128, issue.17, pp.8030-8035, 2014.
DOI : 10.1039/c3cp55485f

M. B. Albota, D. Bredas, J. L. Ehrlich, J. E. Fu, J. Y. Heikal et al., Design of Organic Molecules with Large Two-Photon Absorption Cross Sections, Science, vol.281, issue.5383, pp.1653-1656, 1998.
DOI : 10.1126/science.281.5383.1653