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Welcome to Ultrafast Optics Who am I: When, where: Web page: Prerequisites: Grading: Daniel Mittleman (office hours: to be determined) Tues / Thurs @ 9am see canvas Quantum mechanics and E&M at an undergraduate level, or permission of instructor. Come talk to me if you are uncertain. Lecture attendance (mandatory) Problem sets (occasional) Research presentations (everybody)

Textbooks No required text! But if you will be working in this field, you will want to own some of these Recommended reading - lasers and nonlinear optics: Lasers, by A. Siegman (University Science Books, 1986) Fundamentals of Photonics, by Saleh and Teich (Wiley, 1991) The Principles of Nonlinear Optics, by Y. R. Shen (Wiley, 1984) Nonlinear Optics, by R. Boyd (Academic Press, 1992) Optics, by Eugene Hecht (Addison-Wesley, 1987) Recommended reading - ultrafast phenomena: Ultrashort laser pulse phenomena, by J.-C. Diels and W. Rudolph (Second Edition, Academic Press, 2006) Ultrafast Optics, by Andrew Weiner (Wiley, 2009)

Topics to be covered Basic optical physics Pulse propagation 2nd and 3rd-order non-linearities Mode-locking }How do they do this? (and why) Other topics pending www.chem.rug.nl/spectro/projects/laser.html

Prefixes: Small How big and how small? Milli (m) 10-3 Micro (µ) 10-6 Nano (n) 10-9 Pico (p) 10-12 Femto (f) 10-15 Atto (a) 10-18 10 fs light pulse 1 minute Big Kilo (k) 10 +3 Mega (M) 10 +6 Giga (G) 10 +9 Tera (T) 10 +12 Peta (P) 10 +15 Exa (E) 10 +18 Zepto (z) 10-21 Zetta (Z) 10 +21 Yocto (y) 10-24 Yotta (Y) 10 +24 Computer clock cycle Camera flash One month Age of pyramids Human existence Age of universe 10-14 10-9 10-4 10 1 10 6 10 11 10 16 Time (seconds)

Ultrafast Phenomena - The Evolution of Speed 10-6 Speed (seconds) 10-9 10-12 Optics Electronics } currently: factor of 10 6 10-15 1960 1970 1980 1990 2000 Year 2010

A brief history of time resolution Leland Stanford Eadweard Muybridge The "Trotting Horse" Controversy Palo Alto, CA 1872 Time Resolution: 1/60th of a second

'Doc' Edgerton - Strobe Photography Harold Edgerton 1942 MIT Research Laboratory for Electronics How to Make Apple sauce at MIT H. Edgerton, 1964 Splash on a Glass Curtis Hurley Junior High School student 1996 Time Resolution: a few microseconds

It all started with the laser Theodore Maiman (Hughes Research Lab), inventor of the laser, holding his invention (1960)

The Laser - Mode Locking Shortest Pulse Duration (femtoseconds) 1000 100 10 Active mode locking Passive mode locking Extra-cavity pulse compression Colliding pulse mode locking Intra-cavity pulse compression Current record (visible light): 3.4 fsec Yamane, et al. Nov. 2003 '65 '70 '75 '80 '85 '90 '95 Year Mode-locked Ti:sapphire laser

Generating ultrashort pulses: mode locking

Long vs. Short light pulses The uncertainty principle says that the product of the temporal and spectral pulse widths is greater than ~1. Irradiance vs. time Spectrum Long pulse time frequency Short pulse time frequency To make a short pulse, you need a lot of spectral bandwidth.

Consider a pulse: A typical pulse duration = 100 femtoseconds wavelength = 800 nanometers frequency domain: E(ω) time domain: E(t) 2.6 fsec Fourier transform 780 800 820 wavelength (nanometers) -200 0 200 time (femtoseconds) number of cycles ~ (duration of one cycle) / (duration of pulse)

The Shortest Pulses at Different Wavelengths 10-11 3 mm Wavelength 3 µm 3 nm Pulse Duration (seconds) 10-12 10-13 10-14 10-15 One optical cycle New in 2006 New in 2008 New in 2003 10 11 10 12 10 13 10 14 10 15 10 16 10 17 10 18 10 19 Frequency (Hz) New in 2001 current record: 80 attoseconds (x-rays)

The Shortest Pulses at Long Wavelengths Amplitude (arb. units) 4 2 0-2 0 500 1000 1500 2000 Delay (femtoseconds) Amplitude (arb. units) 10 8 6 4 2 0 0 1 2 3 Frequency (THz)

Short Pulses at Short Wavelengths 90 degree relativistic Thompson scattering Lawrence Berkeley National Laboratory

Breaking the attosecond barrier F. Krausz and co-workers, TU Vienna, 2001 A cross-correlation of a 650 attosecond x-ray pulse with a 7.5 femtosecond infrared pulse λ = 13.8 nm measured signal: spectral width of a photoelectron spectrum Required infrared pulse intensity: 5 10 13 W/cm 2

The shortest pulses ever (so far) measured photoelectron spectrum Goulielmakis, et al., Science, June 2008 reconstructed attosecond pulse

Ultrafast set-ups can be very sophisticated.

Why does ultrashort usually mean ultra-intense? A continuous-wave (cw) laser: irradiance time average energy = power/time = joules per second = Watts Example: 1 Watt at λ = 800 nm is 4 10 18 photons per second. So, in a 100 fs window, we have only 4 10 5 photons. A pulsed laser: pulse duration = 100 fs pulse rate = 100 MHz irradiance 10 ns time Example: 1 Watt at λ = 800 nm is 4 10 10 photons per pulse. Energy per pulse = 4 10 10 photons per pulse energy/photon = 10 nj/pulse Peak energy = energy per pulse / pulse duration = 10 5 W Focus this to a 10 µm diameter spot: Peak irradiance = 10 15 W/m 2

Chirped pulse amplification

The Highest Intensities You Can Possibly Imagine 0.2 TW = 200,000,000,000 watts! 1 khz CPA system at the University of California, Santa Barbara

(used to be) The world s biggest laser Nova - Lawrence Livermore National Laboratory

(currently) The world s biggest laser National Ignition Facility (commissioned in 2009) 192 shaped pulses 1.8 MJ total energy

National Ignition Facility In 2012: generated a peak power of 500 terawatts (2 megajoules in 4 nanoseconds) For that brief instant, NIF produced 1000 times as much power as the entire US electrical grid.

Ultrafast Laser Spectroscopy: Why? Most events that occur in atoms and molecules occur on fs and ps time scales. The length scales are very small, so very little time is required for the relevant motion. Excited state decay via fluorescence occurs on a ns time scale, but competing non-radiative processes only speed things up because relaxation rates add: 1 1 1 = + τ ex τ fl τ nr Biologically important processes utilize excitation energy for purposes other than fluorescence and hence must be very fast. Collisions in room-temperature liquids occur on a few-fs time scale, so nearly all processes in liquids are ultrafast. Semiconductor processes of technological interest are necessarily ultrafast or we wouldn t be interested.

The most common type of ultrafast measurement τ Strong pump pulse perturbs the sample at t = 0. A time τ later, a weak probe pulse interrogates the sample. Measure the transmission of the probe pulse at each delay τ. transmitted pulse energy information about the dynamics! τ = 0 delay

PRESS RELEASE 12 OCTOBER 1999 The Royal Swedish Academy of Sciences has awarded the 1999 Nobel Prize in Chemistry to Professor Ahmed H. Zewail, California Institute of Technology, Pasadena, USA for showing that it is possible with rapid laser technique to see how atoms in a molecule move during a chemical reaction. The Academy's citation: For his studies of the transition states of chemical reactions using femtosecond spectroscopy. This year's laureate in Chemistry is being rewarded for his pioneering investigation of fundamental chemical reactions, using ultrashort laser flashes, on the time scale on which the reactions actually occur. Professor Zewail's contributions have brought about a revolution in chemistry and adjacent sciences, since this type of investigation allows us to understand and predict important reactions.

What is "Femtochemistry"? Example: Pump-probe fluorescence of iodine in the gas phase Zewail, et al., J. Chem. Phys., 106, 4353 (1997)

Ultrashort in time is also ultrashort in space cw laser beam laser a few mm pulsed laser beam ultrafast laser 3 meters 30 microns (for a 100 fs pulse) a few mm

Ultrashort in time is also ultrashort in space, part II In multi-photon imaging, we focus an ultrashort pulse tightly into an object and observe the multi-photon signal light. F ~ I 2 F = Two-photon Fluorescence energy

Ultrashort in time is also ultrashort in space, part III One-photon fluorescence from a beam entering from the right Two-photon fluorescence from an identical beam entering from the left Image from Chris Schaffer, UCSD

Ultrashort pulses interact with materials differently groove machined with nanosecond pulse and with femtosecond pulse Clark MXR, Inc., Ann Arbor, MI

Ultrafast lasers make great scalpels! New eye surgery technique developed at CUOS (Center for Ultrafast Optical Sciences), at the University of Michigan www.intralase.com

Lightning protection using amplified short pulses guided and unguided lightning The pulse induces a conducting path, discharging the cloud before lightning can occur.

Ultrafast lasers make great clocks! Temporal spacing of pulses translates to frequency spacing of the comb Temporal spacing can be stabilized to much better than one part in 10 11

PRESS RELEASE 4 OCTOBER 2005 The Royal Swedish Academy of Sciences has awarded the 2005 Nobel Prize in Physics for 2005 with one half to Roy J. Glauber Harvard University, Cambridge, MA, USA "for his contribution to the quantum theory of optical coherence" and one half jointly to John L. Hall National Institute of Standards and Technology, Boulder, CO, USA and Theodor W. Hänsch Max-Planck-Institut für Quantenoptik, Garching, Germany "for their contributions to the development of laser-based precision spectroscopy, including the optical frequency comb technique".

How does it work? In order to understand the formation of femtosecond pulses, we need to know about: how a cw (continuous wave) laser works. how a short pulse propagates through materials at low intensities, and at high intensities. mode locking. Our model system to learn all of this: Titanium-doped sapphire laser (Ti:sapphire)

The Ti:sapphire laser A typical optical layout, if you want to build your own: or you can buy one:

Reminders This class has: mandatory lecture attendance no text book oral presentations by all students in March/April weekly office hours (Tuesday 1:00-2:30 in Brockman 351)