Intensity-dependent degenerate and non-degenerate nonlinear optical absorption of direct-gap semiconductors

The nonlinear optical response of direct-gap semiconductors is investigated with a focus on non-degenerate multiphoton absorption processes. The theoretical approach is based on the semiconductor Bloch equations and yields the absorption rate either perturbatively or non-perturbatively in the incident light intensities. We describe the semiconductor by a two-band model and consider a pump-probe scheme where the weak probe pulse provides one of the simultaneously absorbed photons. The perturbative response can be described analytically within some approximations and we give simple expressions for two, three, and four-photon absorption coefficients. These are compared with numerical results for the absorption of pulses with a finite duration, where the influence of dephasing and relaxation as well as higher-order corrections are also investigated. For strong pump fields that are treated non-perturbatively we demonstrate non-trivial dependencies of the absorption on the time delay between the pulses. In the non-perturbative response of a single light pulse characteristic modulations appear in the absorption dependence on the field strength that may be interpreted as multi-photon Rabi oscillations. Finally, we present measurements of the non-degenerate two-photon absorption coefficient of bulk GaAs via time-delay and polarization-dependent transmissivity changes in a pump probe setup. The observed strong increase of the absorption coefficient with frequency ratios deviating from unity qualitatively agrees with theoretical expectations.

[1]  D. R. Andersen,et al.  Measurement of the anisotropy of two-photon absorption coefficients in zincblende semiconductors , 1993 .

[2]  Huynh Thanh Duc,et al.  Microscopic analysis of the coherent optical generation and the decay of charge and spin currents in semiconductor heterostructures. , 2005, Physical review letters.

[3]  Scott Webster,et al.  Extremely Nondegenerate Two-photon Absorption in Direct-gap Semiconductors [invited] References and Links , 2022 .

[4]  F. Capasso,et al.  Mid-infrared two-photon absorption in an extended-wavelength InGaAs photodetector , 2017, 1712.03580.

[5]  Sipe,et al.  Nonlinear optical response of semiconductors in the independent-particle approximation. , 1993, Physical review. B, Condensed matter.

[6]  M. Betz,et al.  Stimulated two-photon emission in bulk CdSe. , 2018, Optics letters.

[7]  Pavel Ginzburg,et al.  Observation of two-photon emission from semiconductors , 2008 .

[8]  A. Gaeta,et al.  Few-photon all-optical modulation in a photonic band-gap fiber. , 2011, Physical review letters.

[9]  Lami,et al.  Observation of Interband Two-Photon Absorption Saturation in CdS. , 1996, Physical review letters.

[10]  S. Winnerl,et al.  Terahertz two-photon quantum well infrared photodetector. , 2009, Optics express.

[11]  E. W. Stryland,et al.  Sensitive Measurement of Optical Nonlinearities Using a Single Beam Special 30th Anniversary Feature , 1990 .

[12]  D. Yavuz All-optical femtosecond switch using two-photon absorption , 2006 .

[13]  H. Schneider,et al.  Ultrasensitive femtosecond two-photon detector with resonantly enhanced nonlinear absorption. , 2005, Optics letters.

[14]  H. Driel,et al.  Two-photon absorption and Kerr coefficients of silicon for 850–2200nm , 2007 .

[15]  Hughes,et al.  Coherent control of photocurrent generation in bulk semiconductors. , 1996, Physical review letters.

[16]  R. Loudon Theory of Non-linear Optical Processes in Semiconductors and Insulators , 1962 .

[17]  Matthew Reichert,et al.  Observation of Nondegenerate Two-Photon Gain in GaAs. , 2016, Physical review letters.

[18]  Mansoor Sheik-Bahae,et al.  Nondegenerate optical Kerr effect in semiconductors , 1994 .

[19]  Ofer Levi,et al.  Improved dispersion relations for GaAs and applications to nonlinear optics , 2003 .

[20]  Aversa,et al.  Nonlinear optical susceptibilities of semiconductors: Results with a length-gauge analysis. , 1995, Physical review. B, Condensed matter.

[21]  A. Penzkofer,et al.  Two-photon absorption and emission dynamics of bulk GaAs , 1989 .

[22]  Mansoor Sheik-Bahae,et al.  Determination of bound-electronic and free-carrier nonlinearities in ZnSe, GaAs, CdTe, and ZnTe , 1992 .

[23]  J. S. Aitchison,et al.  Role of two‐photon absorption in ultrafast semiconductor optical switching devices , 1990 .

[24]  Aversa,et al.  Third-order optical nonlinearities in semiconductors: The two-band model. , 1994, Physical review. B, Condensed matter.

[25]  David J. Hagan,et al.  Nondegenerate two-photon absorption spectra of ZnSe, ZnS and ZnO , 1993 .

[26]  Mansoor Sheik-Bahae,et al.  Dispersion of bound electron nonlinear refraction in solids , 1991 .

[27]  Thomas,et al.  Dynamic localization in anisotropic Coulomb systems: Field induced crossover of the exciton dimension. , 1995, Physical review letters.

[28]  Joerg Hader,et al.  Coherent electric-field effects in semiconductors , 1998, Photonics West.

[29]  John J. Hopfield,et al.  TWO-QUANTUM ABSORPTION SPECTRUM OF KI AND CsI , 1965 .

[30]  Lindberg,et al.  Transient many-body effects in the semiconductor optical Stark effect: A numerical study. , 1991, Physical review. B, Condensed matter.

[31]  R. Braunstein,et al.  Optical Double-Photon Absorption in CdS , 1964 .

[32]  G. Mahan Theory of Two-Photon Spectroscopy in Solids , 1968 .

[33]  Matthew Reichert,et al.  Three-dimensional IR imaging with uncooled GaN photodiodes using nondegenerate two-photon absorption. , 2016, Optics express.

[34]  Martin M. Fejer,et al.  Multiphoton absorption and nonlinear refraction of GaAs in the mid-infrared , 2007 .

[35]  David J. Hagan,et al.  Sensitive mid-infrared detection in wide-bandgap semiconductors using extreme non-degenerate two-photon absorption , 2011 .

[36]  T. Meier,et al.  Higher-order contributions and nonperturbative effects in the nondegenerate nonlinear optical absorption of semiconductors using a two-band model , 2018, Physical Review B.