Ultrafast two-dimensional terahertz spectroscopy of elementary excitations in solids

Recent experimental progress has allowed for the implementation of nonlinear two-dimensional (2D) terahertz (THz) spectroscopy in the ultrafast time domain. We discuss the principles of this technique based on multiple phase-locked electric field transients interacting in a collinear geometry with a solid and the phase-resolved detection of the THz fields after interaction with the sample. To illustrate the potential of this new method, 2D correlation spectra of coupled intersubband-longitudinal optical phonon excitations in a double quantum well system and a study of ultrafast carrier dynamics in graphene are presented.

[1]  T. Elsaesser,et al.  Two-dimensional terahertz correlation spectra of electronic excitations in semiconductor quantum wells. , 2011, The journal of physical chemistry. B.

[2]  S Winnerl,et al.  Carrier relaxation in epitaxial graphene photoexcited near the Dirac point. , 2011, Physical review letters.

[3]  Junrong Zheng,et al.  Ultrafast Dynamics of Solute-Solvent Complexation Observed at Thermal Equilibrium in Real Time , 2005, Science.

[4]  Martin T. Zanni,et al.  Concepts and Methods of 2D Infrared Spectroscopy , 2011 .

[5]  Andrei Tokmakoff,et al.  Coherent 2D IR Spectroscopy: Molecular Structure and Dynamics in Solution , 2003 .

[6]  Andre K. Geim,et al.  The rise of graphene. , 2007, Nature materials.

[7]  S. Mukamel,et al.  Two-dimensional femtosecond vibrational spectroscopy of liquids , 1993 .

[8]  S. Mukamel.  Principles of Nonlinear Optical Spectroscopy , 1995 .

[9]  A. Pashkin,et al.  Nonperturbative interband response of a bulk InSb semiconductor driven off resonantly by terahertz electromagnetic few-cycle pulses. , 2012, Physical review letters.

[10]  D. Jonas.  Two-dimensional femtosecond spectroscopy. , 2003, Annual review of physical chemistry.

[11]  Thomas Elsaesser,et al.  Ultrafast nonequilibrium carrier dynamics in a single graphene layer , 2011 .

[12]  T. Elsaesser,et al.  Terahertz-induced interband tunneling of electrons in GaAs , 2010 .

[13]  Graham R. Fleming,et al.  Two-dimensional spectroscopy of electronic couplings in photosynthesis , 2005, Nature.

[14]  S. Skupin,et al.  Tailoring terahertz radiation by controlling tunnel photoionization events in gases , 2011, 1107.1767.

[15]  Markus Kress,et al.  Terahertz-pulse generation by photoionization of air with laser pulses composed of both fundamental and second-harmonic waves. , 2004, Optics letters.

[16]  T. Elsaesser,et al.  Strong correlation of electronic and lattice excitations in GaAs/AlGaAs semiconductor quantum wells revealed by two-dimensional terahertz spectroscopy. , 2011, Physical review letters.

[17]  T. Elsaesser,et al.  Ultrafast memory loss and energy redistribution in the hydrogen bond network of liquid H2O , 2005, Nature.

[18]  T. Elsaesser,et al.  High-field transport in an electron-hole plasma: transition from ballistic to drift motion. , 2011, Physical review letters.

[19]  S. Koch,et al.  Terahertz coherent control of optically dark paraexcitons in Cu2O. , 2008, Physical review letters.

[20]  T. Elsaesser,et al.  Generation of single-cycle THz transients with high electric-field amplitudes. , 2005, Optics letters.

[21]  Tianhao Zhang,et al.  Many-body interactions in semiconductors probed by optical two-dimensional fourier transform spectroscopy. , 2006, Physical review letters.

[22]  C. Berger,et al.  Ultrafast dynamics and interlayer thermal coupling of hot carriers in epitaxial graphene , 2009 .

[23]  Alfred Leitenstorfer,et al.  Phase-locked generation and field-resolved detection of widely tunable terahertz pulses with amplitudes exceeding 100 MV/cm. , 2008, Optics letters.

[24]  T. Elsaesser,et al.  Coherent ballistic motion of electrons in a periodic potential. , 2010, Physical review letters.

[25]  T. Elsaesser,et al.  Ultrafast spatiotemporal dynamics of terahertz generation by ionizing two-color femtosecond pulses in gases. , 2010, Physical review letters.

[26]  E. Kane.  Zener tunneling in semiconductors , 1960 .

[27]  E. Schierle,et al.  Resonant elastic soft x-ray scattering , 2012, Reports on progress in physics. Physical Society.

[28]  T. Elsaesser,et al.  Direct field-resolved detection of terahertz transients with amplitudes of megavolts per centimeter. , 2003, Optics letters.

[29]  Jesse Dean,et al.  Ultrafast carrier kinetics in exfoliated graphene and thin graphite films. , 2009, Optics express.

[30]  Alfred Leitenstorfer,et al.  Ultrabroadband detection of multi-terahertz field transients with GaSe electro-optic sensors: Approaching the near infrared , 2004 .

[31]  T. Elsaesser,et al.  Internal motions of a quasiparticle governing its ultrafast nonlinear response , 2007, Nature.

[32]  Gerhard Stock,et al.  Hydrogen-bond lifetime measured by time-resolved 2D-IR spectroscopy: N-methylacetamide in methanol , 2001 .

[33]  T. Elsaesser,et al.  Phase-resolved two-dimensional spectroscopy based on collinear n-wave mixing in the ultrafast time domain. , 2009, The Journal of chemical physics.

[34]  R. Hochstrasser,et al.  Two-dimensional infrared spectroscopy of peptides by phase-controlled femtosecond vibrational photon echoes. , 2000, Proceedings of the National Academy of Sciences of the United States of America.

[35]  George Rodriguez,et al.  Terahertz emission from ultrafast ionizing air in symmetry-broken laser fields. , 2007, Optics express.

[36]  T. Mančal,et al.  Two-dimensional electronic spectroscopy of molecular excitons. , 2009, Accounts of chemical research.

[37]  Xi-Cheng Zhang,et al.  Free-space electro-optics sampling of mid-infrared pulses , 1997 .

[38]  R. Hochstrasser,et al.  STRUCTURE OF THE AMIDE I BAND OF PEPTIDES MEASURED BY FEMTOSECOND NONLINEAR-INFRARED SPECTROSCOPY , 1998 .

[39]  T. Elsaesser,et al.  Nonlinear terahertz response of n-type GaAs , 2006 .

[40]  E. Hendry,et al.  Carrier dynamics in semiconductors studied with time-resolved terahertz spectroscopy , 2011 .

[41]  F. Rana,et al.  Very slow cooling dynamics of photoexcited carriers in graphene observed by optical-pump terahertz-probe spectroscopy. , 2011, Nano letters.

[42]  S. Mukamel,et al.  Multidimensional femtosecond correlation spectroscopies of electronic and vibrational excitations. , 2000, Annual review of physical chemistry.

[43]  R. Hochstrasser,et al.  Intense terahertz pulses by four-wave rectification in air. , 2000, Optics letters.

[44]  T. Elsaesser,et al.  Phase-resolved nonlinear response of a two-dimensional electron gas under femtosecond intersubband excitation. , 2004, Physical review letters.

[45]  K. Nelson,et al.  Generation of 10 μJ ultrashort terahertz pulses by optical rectification , 2007 .

[46]  F. Guinea,et al.  The electronic properties of graphene , 2007, Reviews of Modern Physics.