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Cavity-Enhanced Ultrafast Transient Absorption Spectroscopy
Kevin Keleher, Yuning Chen, Melanie Roberts Reber, Thomas K. Allison
Departments of Chemistry and Physics, Stony Brook University
Introduction
Our group is to develop the new technique of cavity-enhanced ultrafast
transient absorption spectroscopy to observe ultrafast dynamics of
molecules. This technique uses high-finesse optical cavities and Ytterbium
fiber laser frequency combs to allow for high sensitivity in the absorption
spectroscopy. In this experiment we will analyze the dynamics of visible
chromophores in the gas phase, and later on observe the vibrational
dynamics of hydrogen-bonded clusters.
Ytterbium Fiber Laser Design
Yb Oscillator Output
The laser can be mode locked in several dispersion regimes by manipulating
the distance between the gratings. Mode locking in the anomalous regime,
where shorter wavelengths have a faster group velocity, allows for a wider
spectrum.
Spectrometer Probe Cavity Supersonic
Expansion
System Setup
Yb Oscillator
Stable YAG
To fo stabilization
electronics
Fiber
Stretcher
AOM
OPO
Pump Cavity
Vacuum Chamber
Tunable PDH
CavityLock
Delay Stage
Doubling
Crystal
Doubling
Crystal
Beam
Splitter
Grating
Compressor
Nonlinear polarization evolution is used to mode lock the laser passively
(no external signal required).
Actual
Laser
Autocorrelator
An intensity autocorrelator is used to determine the pulse duration of the
laser system’s output. A time delay τ is given to one of the split beams.
A second harmonic signal, S(τ), is produced in a BBO crystal.
Mathematically, S(τ) is the autocorrelation of the incident pulse.
𝑆 = 𝐼 𝑡 𝐼 𝑡 − 𝜏 𝑑𝑡
WDM
Pump Laser
Yb-doped
Fiber
λ/4
λ/4
λ/2
Gratings
Polarizing
Beam-Splitter
To Amplifier
HI-1060
Fiber
Piezo
Output Power: 60 mW (average)
Pump Power: 150 mW
Repetition Rate of 60 MHz
Frequency combs in CE spectroscopy
inT
Time difference between pulses can
be adjusted to allow for constructive
interference in the cavity.
Frequency comb teeth line up with
the resonate modes of the cavity.
Dispersion changes the optical cavity modes, shifting them out of
alignment with the comb’s teeth, because of this the dispersion limits the
attainable optical bandwidth in the cavity.
Vacuum Chamber
The chamber has a 4 foot by 2 foot design, and will have a background
pressure of 100 mtorr. Due to the large external forces acting on the
chamber, the aluminum chamber is supported by perpendicular struts on
both top and bottom of the chamber. The throughput of the system will be as
much as 23 TorrL/s and can be calculated by using the following equation.
𝑄 = 𝑆 𝑒𝑓𝑓 × 𝑃𝐶
Where Q = throughput, 𝑃𝐶 = chamber pressure, 𝑆 𝑒𝑓𝑓 = pumping speed
Vacuum pumps currently used are an Edwards EH-1200 roots blower and a
Edwards E2M80 roughing pump. Testing the newly set up pumps resulted in
pressures about 10 mTorr.
Funding
Lab Photos
Increased Sensitivity in Experiment
Having high finesse optical cavities (F ≈ 1000), both pump comb and probe
comb are improved by a factor of ~
𝐹
𝜋
, and improving the signal received by
the spectrometer by (
𝐹
𝜋
)2
. This makes this method approximately 105
times
more sensitive than traditional ultrafast transient absorption spectroscopy.
Actual Chamber
Normal Dispersion Anomalous Dispersion
Comb
Amplifier
Amplifier
The Ytterbium doped fiber of the amplifier increases the signal’s power
through stimulated emission of the doping agent. More than 15 W output can
be obtained for 30 W of pump power. We use chirped pulse amplification,
with ~ 100 ps pulses, to avoid nonlinear effects in the amplifier fiber. A pulse
compressor, consisting of two diffraction gratings and a retroreflector, reduce
the pulse duration follow the amplifier.
Symbolic
Representation

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Revised URECA Poster

  • 1. Cavity-Enhanced Ultrafast Transient Absorption Spectroscopy Kevin Keleher, Yuning Chen, Melanie Roberts Reber, Thomas K. Allison Departments of Chemistry and Physics, Stony Brook University Introduction Our group is to develop the new technique of cavity-enhanced ultrafast transient absorption spectroscopy to observe ultrafast dynamics of molecules. This technique uses high-finesse optical cavities and Ytterbium fiber laser frequency combs to allow for high sensitivity in the absorption spectroscopy. In this experiment we will analyze the dynamics of visible chromophores in the gas phase, and later on observe the vibrational dynamics of hydrogen-bonded clusters. Ytterbium Fiber Laser Design Yb Oscillator Output The laser can be mode locked in several dispersion regimes by manipulating the distance between the gratings. Mode locking in the anomalous regime, where shorter wavelengths have a faster group velocity, allows for a wider spectrum. Spectrometer Probe Cavity Supersonic Expansion System Setup Yb Oscillator Stable YAG To fo stabilization electronics Fiber Stretcher AOM OPO Pump Cavity Vacuum Chamber Tunable PDH CavityLock Delay Stage Doubling Crystal Doubling Crystal Beam Splitter Grating Compressor Nonlinear polarization evolution is used to mode lock the laser passively (no external signal required). Actual Laser Autocorrelator An intensity autocorrelator is used to determine the pulse duration of the laser system’s output. A time delay τ is given to one of the split beams. A second harmonic signal, S(τ), is produced in a BBO crystal. Mathematically, S(τ) is the autocorrelation of the incident pulse. 𝑆 = 𝐼 𝑡 𝐼 𝑡 − 𝜏 𝑑𝑡 WDM Pump Laser Yb-doped Fiber λ/4 λ/4 λ/2 Gratings Polarizing Beam-Splitter To Amplifier HI-1060 Fiber Piezo Output Power: 60 mW (average) Pump Power: 150 mW Repetition Rate of 60 MHz Frequency combs in CE spectroscopy inT Time difference between pulses can be adjusted to allow for constructive interference in the cavity. Frequency comb teeth line up with the resonate modes of the cavity. Dispersion changes the optical cavity modes, shifting them out of alignment with the comb’s teeth, because of this the dispersion limits the attainable optical bandwidth in the cavity. Vacuum Chamber The chamber has a 4 foot by 2 foot design, and will have a background pressure of 100 mtorr. Due to the large external forces acting on the chamber, the aluminum chamber is supported by perpendicular struts on both top and bottom of the chamber. The throughput of the system will be as much as 23 TorrL/s and can be calculated by using the following equation. 𝑄 = 𝑆 𝑒𝑓𝑓 × 𝑃𝐶 Where Q = throughput, 𝑃𝐶 = chamber pressure, 𝑆 𝑒𝑓𝑓 = pumping speed Vacuum pumps currently used are an Edwards EH-1200 roots blower and a Edwards E2M80 roughing pump. Testing the newly set up pumps resulted in pressures about 10 mTorr. Funding Lab Photos Increased Sensitivity in Experiment Having high finesse optical cavities (F ≈ 1000), both pump comb and probe comb are improved by a factor of ~ 𝐹 𝜋 , and improving the signal received by the spectrometer by ( 𝐹 𝜋 )2 . This makes this method approximately 105 times more sensitive than traditional ultrafast transient absorption spectroscopy. Actual Chamber Normal Dispersion Anomalous Dispersion Comb Amplifier Amplifier The Ytterbium doped fiber of the amplifier increases the signal’s power through stimulated emission of the doping agent. More than 15 W output can be obtained for 30 W of pump power. We use chirped pulse amplification, with ~ 100 ps pulses, to avoid nonlinear effects in the amplifier fiber. A pulse compressor, consisting of two diffraction gratings and a retroreflector, reduce the pulse duration follow the amplifier. Symbolic Representation