Optical Spectroscopy of Advanced Materials

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1 Phys 590B Condensed Matter Physics: Experimental Methods Optical Spectroscopy of Advanced Materials Basic optics, nonlinear and ultrafast optics Jigang Wang Department of Physics, Iowa State University and Ames Lab- USDoE

2 Outline (Feb 9 th Feb 9 th, 11 th and 13 th : overview, basic optics and spectroscopy 2. Feb 16 th,18 th and 20 th : Advanced optics, ultrafast and nonlinear spectroscopy - femtosecond lasers: case study; spectroscopy techniques: incoherent & coherent transient, magneto-optical, infrared & time-domain THz General References: Demtroder, Laser Spectroscopy: Basic Concepts and Instrumentation Diels and Rudolph (DR), Ultrashort Laser Pulse Phenomena 20 th ) Shah, Ultrashort Spectroscopy of Semiconductors and Semiconductor Nanostructures Chemla, D.S., Ultrafast Transient Nonlinear Optical Processes in Semiconductors For example, see Copper, S.L, Optical Spectroscopy Studies of Metal-Insulator Transitions in Perovskite-related Oxides Jigang Wang, Feb, 2009

3 Today Overview and Introduction Jigang Wang, Feb, 2009

4 Light is, in short, the most refined form of matter. Louis de Broglie Berkeley, California

5 The first spectroscopy experiment

6 A brief history of optics 17th-century 18 th -century 19th-century 20th-century Kepler, Newton Huygens. Total internal reflection, Telescope, geometrical optics, the wave theory, prism dispersion, the particle theory of light Fresnel, Young Maxwell Michelson Interference, diffraction, expressions for reflected and transmitted waves, unified electricity and magnetism Einstein Light is (1) a phenomenon of empty space (2) both a wave and a particle

7 The equations of optics Maxwell s equations r r r r E = / E = ρ ε r r r r B= 0 B= µε r B t r E t ε is the permittivity, µ is the permeability of the medium

8 Solving Maxwell s s equations r r E µε t 2 2 E = 0 2 r r r r Ert (, ) cos( ωt± k ) Light is an Electromagnetic Wave

9 Wave Properties Velocity E x E t 2 2 µε = Phase velocity ω k = v = 1 µε Group velocity v / g [ dk dω] 1 ω dn vg = v phase / 1+ n dω

10 Wave Properties Spectrum 1 THz = 300 µm = 33 cm -1 = 4.1 mev

11 Refraction At an oblique angle, light can be completely transmitted or completely reflected. "Total internal reflection" is the basis of optical fibers, a billion dollar industry.

12 Conventional Spectroscopy Methods E T R - Absorption, Reflection, Emission, Interference, Scattering - Spectrally resolved before or after sample

13 Absorption Spectroscopy Penetration depth into water vs. wavelength Dispersion elements 1 km Penetration depth into water 1 m 1 mm 1 µm Radio Microwave IR UV X-ray 1 km 1 m 1 mm 1 µm 1 nm Wavelength Visible spectrum

14 Scattering Spectroscopy I Raman 4 λ

15 Fourier Transform Infrared (FTIR) Spectrometer White light Interference

16 Nature can do similar tricks by itself

17 Nature knows interference

18 The amazing light Laser Light amplification of stimulated emission of radiation (Laser) A laser will lase if the beam increases in irradiance during a round trip: that is, if I 3 > I 0.

19 Continuous vs. ultrashort pulses of laser Continuous beam: Ultrashort pulse:

20 How fast is Ultra-fast? milli 10-3 micro 10-6 nano 10-9 pico femto atto 10-18

21 The evolution of pulse Lasers 10 6 Time resolution (seconds) Electronics Optics Year Courtesy of Trebino

22 Long vs. short pulses of laser Long pulse Short pulse

23 Generating short pulses = mode-locking Locking the phases of the laser frequencies yields an ultrashort pulse.

24 A generic ultrashort-pulse laser A generic ultrafast laser has a broadband gain medium,a pulseshortening device, and two or more mirrors: Pulse-shortening devices include: Saturable absorbers Phase modulators Dispersion compensators Optical-Kerr media

25 Ultrashort laser pulse broadening Different fquencies travel at different group velocities in materials, causing pulses to expand to highly "chirped" (frequency-swept) pulses. Input ultrashort pulse Any medium Chirped output not-so-ultrashort pulse

26 Ultrafast Optics is Nonlinear Optics

27 Ultrashort & Ultrabroadband Spectral Density R E T T, α, R PL, FWM Photon Energy (mev) Signal t = -100 fs t = 0 fs λ = 0 fs t = 100 fs λ Time HHG... λ Signals -> M, p, σ, χ (2), χ (3)... Simultaneous high temporal and spectral resolution

28 Strategic advantages Ultrafast Ultrabroadband e - Manipulation

29 Ultrafast Magneto-optical optical Spectroscopy Excitation J Wang, LBNL Carriers M Detection θ k Magnetic Ions η k Tunable pump-probe from MIR, NIR to visible Highly sensitive to time reversal symmetry breaking

30 Ultrafast THz Spectroscopy Electric field in time-domain FFT spectrum Field-resolved Detection EO Signal S/N~10000: THz Time delay (ps) Frequency (THz) Amplitude and Phase information Real & Imaginary Part of σ(ω), ε(ω) Power Spectrum Complex transmission coefficient t ( ω) Ei EOUT ( ω) ω 2 E ( ) 1 + n + d Z σ( ω) 0 IN () t thin film S Et () t

31 Coherent Transient Spectroscopy Ultrafast FWM k1 k3 k2 k1+k2- k3 k k k-q H V (q) int k + q ( a b) Residual coulomb interactions the dynamics between quasiparticles

32 Ultrafast demagnetization (1) (2) (3) (4) θ K /θ K Time Delay (ps)

33 Ultrafast spectroscopy of HTc superconductor Cuprate SC: Generic Phase Diagram R. A Kaindl et al., Science, 287, 470 (2000)

34 Many-body Effects in SWCN α O 1D Band picture e h E g van Hove singularity Energy α - T/T (%) (A) Transmittance Photon Energy (mev) t = -500 fs 200 fs (B) α 1D Exciton picture 1000 fs Energy O 2000 fs O Energy Photon Energy (mev)

35 Ultrafast Laser Lab Tour Short pulse oscillat or t Dispersive delay line Solid state amplifiers t t Pulse compressor Spectral Density HHG... t Photon Energy (mev)

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