Fiber-based Ultrafast sources for Nonlinear Spectroscopy€¦ · • Fiber Lasers and Amps have HOD...

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Fiber-based Ultrafast sources for Nonlinear Spectroscopy Preliminary Exam for Scott R Domingue, PhD candidate Department of Electrical and Computer Engineering Colorado State University

Transcript of Fiber-based Ultrafast sources for Nonlinear Spectroscopy€¦ · • Fiber Lasers and Amps have HOD...

Page 1: Fiber-based Ultrafast sources for Nonlinear Spectroscopy€¦ · • Fiber Lasers and Amps have HOD compression constraints Pros • Broadbandwidth:

Fiber-based Ultrafast sources for Nonlinear Spectroscopy

Preliminary Exam for Scott R Domingue, PhD candidate

Department of Electrical and Computer Engineering Colorado State University

Page 2: Fiber-based Ultrafast sources for Nonlinear Spectroscopy€¦ · • Fiber Lasers and Amps have HOD compression constraints Pros • Broadbandwidth:

Nonlinear Interactions for Label-Free Chemical Imaging

The best parts of Multiphoton laser scanning microscopy:

• High Resolution (submicron) • Optical Sectioning • Imaging Through Scattering

media • Non-Invasive

BUT • Require tags/labels • Limited to Endogenous 2-Photon

Fluorescence • Appropriate Structure for SHG

SHG

TPEF

THG

Bartels Group unpublished

Imaging a follicle through 70 um thick murine ovarian tissue

Page 3: Fiber-based Ultrafast sources for Nonlinear Spectroscopy€¦ · • Fiber Lasers and Amps have HOD compression constraints Pros • Broadbandwidth:

Nonlinear Interactions for Label-Free Chemical Imaging

Keep the best parts of Multiphoton laser scanning microscopy:

• High Resolution (submicron) • Optical Sectioning • Imaging Through Scattering media

(maybe extend this) • Non-Invasive

BUT • Interrogate Atomic and Molecular

arrangements (label-free) • IR Spectroscopy (stronger but

sub-optimal sources • Coherent Raman (weaker but

“better” sources • Transient Absorption (leverage

any/all endogenous contrast mechanism)

Bartels Group unpublished

Imaging a follicle through 70 um thick murine ovarian tissue

900 cm-1

1150

1230

SHG

TPEF

THG

Page 4: Fiber-based Ultrafast sources for Nonlinear Spectroscopy€¦ · • Fiber Lasers and Amps have HOD compression constraints Pros • Broadbandwidth:

Nonlinear Imaging Tool Kit Imaging Modality Nonlinear Optical

Element Ultrafast Sources

SC Seeded Narrow-Band Amp

Soliton Self Frequency Shifting

Dual-Band SC

Er Fiber Laser

Normal Dispersion SC

ANDi fiber Laser

ANDi seeded MOPA

Ti:Saphire

SHG, THG, TPEF

SRS, CARS, Time-Resolved Raman

Transient Absorption (TAS)

IR / VO

3-Photon Absorption Rapid Delay

Scanner

Yb:KYW

Page 5: Fiber-based Ultrafast sources for Nonlinear Spectroscopy€¦ · • Fiber Lasers and Amps have HOD compression constraints Pros • Broadbandwidth:

Coherent Raman Excitation

SRS, CARS, Time-Resolved Raman

Ener

gy

CARS 𝜕2𝑅𝜕𝑡2

+ 𝛾𝜕𝑅𝜕𝑡

+ Ω𝜈𝑅 =12𝑀

𝜕𝜕𝜕𝑅

𝐴 𝑡 2

The Frequency Domain representation: 𝐷 Ω ∝ ℱ 𝐴 𝑡 2

Beating between SC pulse pairs (15fsTL) Alternative: SC and Narrow-Band pulses

Classic Harmonic Oscillator

Page 6: Fiber-based Ultrafast sources for Nonlinear Spectroscopy€¦ · • Fiber Lasers and Amps have HOD compression constraints Pros • Broadbandwidth:

IR vs. Vibrational Overtone

IR / VO

Ener

gy

Vibrational Overtone Excitation

Shift to Higher frequencies • Optics are better (High

Resolution Microscope) • Potentially simpler sources • Weaker absorption cross-

sections

Soliton Self Frequency Shifting

Er Fiber Laser

Probe altered Susceptibility: Photothermal Spectroscopy

Page 7: Fiber-based Ultrafast sources for Nonlinear Spectroscopy€¦ · • Fiber Lasers and Amps have HOD compression constraints Pros • Broadbandwidth:

Pump-Probe Spectroscopy

JW, Wilson et al. Selected Topics in Quantum Electronics, IEEE Journal of 18, no. 1 (2012). Robles, Francisco E., et al. Optics Express 20.15 (2012): 17082

Continue Opening-Up Potential of Pump-Probe Spectroscopy as Imaging Modality

Rapid Delay Scanner

Page 8: Fiber-based Ultrafast sources for Nonlinear Spectroscopy€¦ · • Fiber Lasers and Amps have HOD compression constraints Pros • Broadbandwidth:

Spectral Targets for Different the Imaging Modalities

Imaging Modality

Ultrafast Sources

Nonlinear Optical Element

Requires Bandwidth

Spectral Requisites

Page 9: Fiber-based Ultrafast sources for Nonlinear Spectroscopy€¦ · • Fiber Lasers and Amps have HOD compression constraints Pros • Broadbandwidth:

Ultrafast Source Comparison

Yb-Doped

Ti:Saphire

Page 10: Fiber-based Ultrafast sources for Nonlinear Spectroscopy€¦ · • Fiber Lasers and Amps have HOD compression constraints Pros • Broadbandwidth:

Ultrafast Source Comparison

Yb-Doped

Ti:Saphire

Pros • Cheaper: ANDi = $12k • Simple fiber Amplifiers ($10k) • Longer Wavelength: 1/3

scattering, deeper penetration in tissue

• SHG, THG, TPEF microscopy ready

Cons • Narrower bandwidth: 130 fs

pulses • Fiber Lasers and Amps have

HOD compression constraints

Pros • Broadbandwidth: <30 fs pulses • SHG, THG, TPEF microscopy

ready • Also ready limited versions of

CARS and OCT • Pumping OPO’s Cons • Not Cheap: $150k oscillators • No simple amplifiers • Often coupled to OPO’s: another

$150k • More Dispersion in typical

Optical Media

Page 11: Fiber-based Ultrafast sources for Nonlinear Spectroscopy€¦ · • Fiber Lasers and Amps have HOD compression constraints Pros • Broadbandwidth:

Ultrafast Source Comparison

Yb-Doped

Ti:Saphire

Pros • Cheaper: ANDi = $12k • Simple fiber Amplifiers ($10k) • Longer Wavelength: 1/3

scattering, deeper penetration in tissue

• SHG, THG, TPEF microscopy ready

Cons • Narrower bandwidth: 130 fs

pulses • Fiber Lasers and Amps have

HOD compression constraints

Pros • Broadbandwidth: <30 fs pulses • SHG, THG, TPEF microscopy

ready • Also ready limited versions of

CARS and OCT • Pumping OPO’s Cons • Not Cheap: $150k oscillators • No simple amplifiers • Often coupled to OPO’s: another

$150k • More Dispersion in typical

Optical Media

Page 12: Fiber-based Ultrafast sources for Nonlinear Spectroscopy€¦ · • Fiber Lasers and Amps have HOD compression constraints Pros • Broadbandwidth:

Our Goals for Yb-Doped Fiber Sources Capitalizing on and Extending these cheap, agile

sources

4 ANDi’s built and Counting…

Page 13: Fiber-based Ultrafast sources for Nonlinear Spectroscopy€¦ · • Fiber Lasers and Amps have HOD compression constraints Pros • Broadbandwidth:

Nonlinear Imaging Tool Kit Imaging Modality Nonlinear Optical

Element Ultrafast Sources

SC Seeded Narrow-Band Amp

Soliton Self Frequency Shifting

Dual-Band SC

Er Fiber Laser

Normal Dispersion SC

ANDi fiber Laser

ANDi seeded MOPA

Ti:Saphire

SHG, THG, TPEF

SRS, CARS, Time-Resolved Raman

Transient Absorption (TAS)

IR / VO

3-Photon Absorption Rapid Delay

Scanner

Yb:KYW

Page 14: Fiber-based Ultrafast sources for Nonlinear Spectroscopy€¦ · • Fiber Lasers and Amps have HOD compression constraints Pros • Broadbandwidth:

Dispersion Regimes for SC generation

Anomalous, PCF

Normal, PCF

Normal, UHNA

Photonic Crystal Fiber (PCF) • Tunable Dispersion • Tight Mode-field Confinement • Need to seal the ends, tricky to

splice Ultra-high Numerical Aperture (UHNA) • Tight Modefield Confinement • Highly dispersive (~4x that of

normal fiber) • High Germanium content,

reducing the damage threshold

Normal Dispersion SC

SHG, THG, TPEF

SRS, CARS, Time-Resolved Raman

Transient Absorption

Yb:KYW

Page 15: Fiber-based Ultrafast sources for Nonlinear Spectroscopy€¦ · • Fiber Lasers and Amps have HOD compression constraints Pros • Broadbandwidth:

Bachler, B. R., et al Optics Express 20.2 (2012): 835 Dudley, J M., et al., Reviews of modern physics 78.4 (2006)

“Efficient supercontinuum generations in silica

suspended core fibers” N << 16 => P0 < 1.6 kW

Incoherent SC

Not as simple as shooting pulses into small core fibers 350 fs @ 1042 nm => Ldisersion = 4.25 m

Peak Power to keep N small, 50 μW => N = 10.2

𝐿𝐷 = τ2

β2 𝐿𝑁𝑁 =

1𝑃0γ

𝑁2 = 𝐿𝐷𝐿𝑁𝑁

Typical SC Generation with Yb-doped Sources in Anomolous Dispersion Fiber

Page 16: Fiber-based Ultrafast sources for Nonlinear Spectroscopy€¦ · • Fiber Lasers and Amps have HOD compression constraints Pros • Broadbandwidth:

SC Generation in Normal Dispersion Fiber

𝜕𝜕𝜕𝜕

− �in+1

n! βn

𝜕n𝜕𝜕Tn

N

n ≥2

= i γ 𝜕 2𝜕 + iω0

𝜕𝜕𝜕

𝜕 2𝜕 − TR𝜕𝜕 𝜕 2

𝜕𝜕

SPM Self-Steeping Intrapulse Raman Scattering

P║ P

P┴

λ/2 A-λ/2

UHNA `

Time [min]

Normal Dispersion SC

Any Applicable Modality Yb:KYW

Page 17: Fiber-based Ultrafast sources for Nonlinear Spectroscopy€¦ · • Fiber Lasers and Amps have HOD compression constraints Pros • Broadbandwidth:

SC Polarization Instability in Weakly Birefringent Fiber

𝜕𝜕𝜕𝜕

− �in+1

n! βn

𝜕n𝜕𝜕Tn

N

n ≥2

= i γ 𝜕 2𝜕 + iω0

𝜕𝜕𝜕

𝜕 2𝜕 − TR𝜕𝜕 𝜕 2

𝜕𝜕

Domingue, Scott R., and Randy A. Bartels. Optics express 21.11 (2013): 13305.

The orthogonal E-field polarizations are coupled, giving rise to Polarization Modulation Instability

Page 18: Fiber-based Ultrafast sources for Nonlinear Spectroscopy€¦ · • Fiber Lasers and Amps have HOD compression constraints Pros • Broadbandwidth:

SC above Instability Threshold

High Correlation in Spectra Changes Mask Spectrally Integrated Noise

De-Polarization ~ 50 % RMS-N = 8% vs. ΦRSN = 20%

ΦRSN

RMS-N

RSN

Domingue, Scott R., and Randy A. Bartels. Optics express 21.11 (2013): 13305.

ΦRSN = ∫σ λ µ(λ)dλ∫ µ2 λ dλ

∙ 100 %

RSN λ =σ λµ(λ)

⋅ 100 % 375 mW, 330 fs seed pulse

Page 19: Fiber-based Ultrafast sources for Nonlinear Spectroscopy€¦ · • Fiber Lasers and Amps have HOD compression constraints Pros • Broadbandwidth:

SC in Highly Bifrefringent (PM) Nonlinear Fiber

375 mW, 1 m of CorActive PM-HNLF

• Lower Nonlinearity than UHNA-3 • Highly Stable, Efficient generated SC • 21 fs Transform Limit

ΦRSN

RMS-N

RSN

Domingue, Scott R., and Randy A. Bartels. Optics express 21.11 (2013): 13305.

De-Polarization ~ 10 % RMS-N = 0.6% vs. ΦRSN = 0.9%

Page 20: Fiber-based Ultrafast sources for Nonlinear Spectroscopy€¦ · • Fiber Lasers and Amps have HOD compression constraints Pros • Broadbandwidth:

Nonlinear Pulse Compression

Long PM-UHNA fibers = Large GDD and HOD Below: SC with Grating Compressor Only

Normal Dispersion SC

Impulsive Stimulated Raman Scattering Yb:KYW

Page 21: Fiber-based Ultrafast sources for Nonlinear Spectroscopy€¦ · • Fiber Lasers and Amps have HOD compression constraints Pros • Broadbandwidth:

Local Characteristic Lengths Local Characteristic Lengths taken from evolving pulse

properties, local in the fiber

LD(𝜕) =τTL 𝜕 2

β2

LNL 𝜕 =1

P(𝜕)γ0

~1m

~10mm

WB

χi 𝜕 = �d𝜕′

Li 𝜕′z

0

Accumulated Dispersion and Nonlinear Lengths akin to B-Integral

Domingue, Scott R., and Randy A. Bartels. Optics express 21.11 (2013): 13305.

Model

Page 22: Fiber-based Ultrafast sources for Nonlinear Spectroscopy€¦ · • Fiber Lasers and Amps have HOD compression constraints Pros • Broadbandwidth:

Accumulated Dispersion/ Nonlinearity

χD~1, LD ~ 10mm

Nonlinear Pulse Compression: • Pulse Shaper

(Transform Limit) • “Simple

Compressor” (GDD compensation)

Domingue, Scott R., and Randy A. Bartels. Optics express 21.11 (2013): 13305.

Model

Page 23: Fiber-based Ultrafast sources for Nonlinear Spectroscopy€¦ · • Fiber Lasers and Amps have HOD compression constraints Pros • Broadbandwidth:

SC compression with Grating Compressor and Pulse Shaper

Nonlinear Pulse Compression

[fs]

Domingue, Scott R., and Randy A. Bartels. Optics express 21.11 (2013): 13305.

Transform Limit dropped from 21 to 36 fs, due to non-optimal pulse shaper: visible SLM, 4λ SLM Wavefront Error, Spherical Abberation

Wavelength

Page 24: Fiber-based Ultrafast sources for Nonlinear Spectroscopy€¦ · • Fiber Lasers and Amps have HOD compression constraints Pros • Broadbandwidth:

Nonlinear Imaging Tool Kit Imaging Modality Nonlinear Optical

Element Ultrafast Sources

SC Seeded Narrow-Band Amp

Soliton Self Frequency Shifting

Dual-Band SC

Er Fiber Laser

Normal Dispersion SC

ANDi fiber Laser

ANDi seeded MOPA

Ti:Saphire

SHG, THG, TPEF

SRS, CARS, Time-Resolved Raman

Transient Absorption (TAS)

IR / VO

3-Photon Absorption Rapid Delay

Scanner

Yb:KYW

Page 25: Fiber-based Ultrafast sources for Nonlinear Spectroscopy€¦ · • Fiber Lasers and Amps have HOD compression constraints Pros • Broadbandwidth:

Narrow Band Pulse Generation

A-λ/2

PM-UHNA

λ/2

1020-LP

FBG

PM-passive, delay

FBG

WDM

PM Low Yb-doped

915 nm diode

DM

λ/2

Narrow Band Amplifier

25 dB gain

SC Seeded Narrow-Band Amp

SRS, CARS, … Yb-doped

TAS

Page 26: Fiber-based Ultrafast sources for Nonlinear Spectroscopy€¦ · • Fiber Lasers and Amps have HOD compression constraints Pros • Broadbandwidth:

Narrow Band Pulse Generation SC Seeded

Narrow-Band Amp SRS, CARS,

Yb-doped TAS

Successful Proof-of-Concept ~20 dB gain 200 μW Seed => 17.5 mW

Comparison: 300 Δλ square spectrum w/ 500 mW => ~2mW/nm 10x the power spectral density in our 980 pump

Consideration: Maintaining PM

Page 27: Fiber-based Ultrafast sources for Nonlinear Spectroscopy€¦ · • Fiber Lasers and Amps have HOD compression constraints Pros • Broadbandwidth:

Nonlinear Imaging Tool Kit Imaging Modality Nonlinear Optical

Element Ultrafast Sources

SC Seeded Narrow-Band Amp

Soliton Self Frequency Shifting

Dual-Band SC

Er Fiber Laser

Normal Dispersion SC

ANDi fiber Laser

ANDi seeded MOPA

Ti:Saphire

SHG, THG, TPEF

SRS, CARS, Time-Resolved Raman

Transient Absorption (TAS)

IR / VO

3-Photon Absorption Rapid Delay

Scanner

Yb:KYW

?

Page 28: Fiber-based Ultrafast sources for Nonlinear Spectroscopy€¦ · • Fiber Lasers and Amps have HOD compression constraints Pros • Broadbandwidth:

Different Modelocking mechanism (nonlinear polarization evolution) and wildly different dispersion profiles… different SC characteristics?

Normal Dispersion SC

Any Applicable Modality ANDi

λ/2 λ/4 λ/4

CMS Yb DC

FI

PC

BF λ/2

976

nm

diod

e

• ~ 500 mW • ~100 fs FWHM TL

All Normal Dispersion (ANDi) Fiber Lasers

Page 29: Fiber-based Ultrafast sources for Nonlinear Spectroscopy€¦ · • Fiber Lasers and Amps have HOD compression constraints Pros • Broadbandwidth:

λ/2 λ/4 λ/4

CMS Yb DC

FI

PC

BF λ/2

976

nm

diod

e

ANDi Spectral Noise and Pulse Compression

ΦRSN = 0.6% RMS-N = 0.4%

Page 30: Fiber-based Ultrafast sources for Nonlinear Spectroscopy€¦ · • Fiber Lasers and Amps have HOD compression constraints Pros • Broadbandwidth:

Cascaded Nonlinearity Results in Significant Noise Generation

+

Wavelength [nm]

= Domingue, Scott R., and Randy A. Bartels. Optics express 21.11 (2013): 13305.

ΦRSN = 3.6% RMS-N = 0.4%

ΦRSN = 0.6% RMS-N = 0.4%

Page 31: Fiber-based Ultrafast sources for Nonlinear Spectroscopy€¦ · • Fiber Lasers and Amps have HOD compression constraints Pros • Broadbandwidth:

ANDi Pulse Compression

• τFWHM = 177 fs • 130% of TL FWHM • 58% TL Peak Power

Page 32: Fiber-based Ultrafast sources for Nonlinear Spectroscopy€¦ · • Fiber Lasers and Amps have HOD compression constraints Pros • Broadbandwidth:

ANDi Pulse Compression

• τFWHM = 163 fs • 120% of TL FWHM • 73% TL Peak Power

w/ 87% of the Energy

92% of Appodized TL Cubic Aberration maps to TOD

Page 33: Fiber-based Ultrafast sources for Nonlinear Spectroscopy€¦ · • Fiber Lasers and Amps have HOD compression constraints Pros • Broadbandwidth:

ANDi Seeded SC Improvement with Compression

ΦRSN reduced by ~½ BUT, Bandwidth (Power) limited

ΦRSN = 1.5% RMS-N = 0.2%

ΦRSN = 3.6% RMS-N = 0.4%

Page 34: Fiber-based Ultrafast sources for Nonlinear Spectroscopy€¦ · • Fiber Lasers and Amps have HOD compression constraints Pros • Broadbandwidth:

Nonlinear Imaging Tool Kit Imaging Modality Nonlinear Optical

Element Ultrafast Sources

SC Seeded Narrow-Band Amp

Soliton Self Frequency Shifting

Dual-Band SC

Er Fiber Laser

Normal Dispersion SC

ANDi fiber Laser

ANDi seeded MOPA

Ti:Saphire

SHG, THG, TPEF

SRS, CARS, Time-Resolved Raman

Transient Absorption (TAS)

IR VO

3-Photon Absorption Rapid Delay

Scanner

Yb:KYW

?

Page 35: Fiber-based Ultrafast sources for Nonlinear Spectroscopy€¦ · • Fiber Lasers and Amps have HOD compression constraints Pros • Broadbandwidth:

Master Oscillator Power Amplifier (MOPA)

Expectations: • Minimize Noise • Amplify and Broaden

Simultaneously • More Power!

Unexpected Benefits: • Cleaner Chirp • Fine Control over

Power Spectrum

Nonlinear Broadening in Amp

Applicable Modality ANDi

NLO

Page 36: Fiber-based Ultrafast sources for Nonlinear Spectroscopy€¦ · • Fiber Lasers and Amps have HOD compression constraints Pros • Broadbandwidth:

Master Oscillator Power Amplifier (MOPA)

`

1000 l/mm

CMS

PM DC-Yb

λ/2

Page 37: Fiber-based Ultrafast sources for Nonlinear Spectroscopy€¦ · • Fiber Lasers and Amps have HOD compression constraints Pros • Broadbandwidth:

MOPA Pulse Evolution

Min TL 56fs

WB

SPM

WB

Sid

e lo

be

5.2nm => 56 fs TL

How compressible are these pulses??

Page 38: Fiber-based Ultrafast sources for Nonlinear Spectroscopy€¦ · • Fiber Lasers and Amps have HOD compression constraints Pros • Broadbandwidth:

MOPA Compression, SPM

3rd order correction unnecessary for “SPM” pulses

• 27 nJ (1.7 W at 63 MHz)

• 144 fs FWHM, 180 kW peak power.

• 95% of TL peak power (135 fs FWHM)

1.8 nm Seed Bandwidth

10 n

m

Page 39: Fiber-based Ultrafast sources for Nonlinear Spectroscopy€¦ · • Fiber Lasers and Amps have HOD compression constraints Pros • Broadbandwidth:

MOPA Compression, WB W/ out 3rd

order correction (green): • 39% TL PP

3.5 nm Seed Bandwidth On-Axis

Off-Axis

Peak Power Estimates for Equal Average Power (reasonable for microscope

applications)

10 n

m

Page 40: Fiber-based Ultrafast sources for Nonlinear Spectroscopy€¦ · • Fiber Lasers and Amps have HOD compression constraints Pros • Broadbandwidth:

MOPA Compression, WB

W/ 3rd order correction (black) • 80 fs FWHM • 70% TL PP(60 fs

FWHM) • 20.5 nJ, 215 kW

W/ out 3rd

order correction (green): • 39% TL PP • 29 nJ

3rd order correction costs spectral appodization for large Δλ

3.5 nm Seed Bandwidth

Peak Power Estimates for Equal Average Power

10 n

m

Page 41: Fiber-based Ultrafast sources for Nonlinear Spectroscopy€¦ · • Fiber Lasers and Amps have HOD compression constraints Pros • Broadbandwidth:

MOPA Seeded SC Nonlinear

Broadening in Amp ANDi Normal Dispersion SC

Is SC seeded from the MOPA stable?

20 nm

MOPA Stability 2.5x increase in ΦRSN • 155x Gain (22dB) • 10x Δλ (from seed)

SC Stability • Increase in RMS-N

likely due to Collimator Heating

SC nearly maintains seed ΦRSN ΦRSN = 0.6%

RMS-N = 0.4% ΦRSN = 1.6%

RMS-N = 0.2% ΦRSN = 1.9% RMS-N = 1%

Page 42: Fiber-based Ultrafast sources for Nonlinear Spectroscopy€¦ · • Fiber Lasers and Amps have HOD compression constraints Pros • Broadbandwidth:

MOPA Seeded SC

Nonlinear Broadening in Amp

Applicable Modality ANDi Normal

Dispersion SC

Page 43: Fiber-based Ultrafast sources for Nonlinear Spectroscopy€¦ · • Fiber Lasers and Amps have HOD compression constraints Pros • Broadbandwidth:

MOPA Seeded SC

Nonlinear Broadening in Amp

SRS, CARS, Spontaneous.. ANDi

SC Seeded Narrow-Band

Amp

2000 cm-1 = the largest vibrational mode excitable Enough bandwidth to excite target Raman Vibrations

Normal Dispersion SC and Amplified 980 NB pulses

Page 44: Fiber-based Ultrafast sources for Nonlinear Spectroscopy€¦ · • Fiber Lasers and Amps have HOD compression constraints Pros • Broadbandwidth:

Nonlinear Imaging Tool Kit

Imaging Modality Nonlinear Optical Element Ultrafast Sources

SC Seeded Narrow-Band Amp

Soliton Self Frequency Shifting

Dual-Band SC

Er Fiber Laser

Normal Dispersion SC

ANDi fiber Laser

ANDi seeded MOPA

Ti:Saphire

SHG, THG, TPEF

SRS, CARS, Time-Resolved Raman

Transient Absorption (TAS)

IR / VO

3-Photon Absorption Rapid Delay

Scanner

Yb:KYW

Page 45: Fiber-based Ultrafast sources for Nonlinear Spectroscopy€¦ · • Fiber Lasers and Amps have HOD compression constraints Pros • Broadbandwidth:

MOPA Seeded Dual-Band SC

http://www.nktphotonics.com/files/files/NL-1050-ZERO-2.pdf Wang, Hui, and Andrew M. Rollins. Applied optics46.10 (2007): 1787.

Nonlinear Broadening in Amp

Applicable Modality ANDi Dual-Band SC

Page 46: Fiber-based Ultrafast sources for Nonlinear Spectroscopy€¦ · • Fiber Lasers and Amps have HOD compression constraints Pros • Broadbandwidth:

MOPA Seeded Dual-Band SC ` Our Model using a Split-Step

Propagator: MOPA: 130fs pulse 300 mW

Page 47: Fiber-based Ultrafast sources for Nonlinear Spectroscopy€¦ · • Fiber Lasers and Amps have HOD compression constraints Pros • Broadbandwidth:

Yb-doped Fiber Laser Pathway through the Nonlinear Imaging Tool Kit

` Nonlinear

Broadening in Amp Applicable Modality ANDi

NLO

SRS, CARS, …

TAS

SHG, THG, TPEF

SPM-Pulses

WB-Pulses

Page 48: Fiber-based Ultrafast sources for Nonlinear Spectroscopy€¦ · • Fiber Lasers and Amps have HOD compression constraints Pros • Broadbandwidth:

Nonlinear Imaging Tool Kit

Imaging Modality Nonlinear Optical Element Ultrafast Sources

SC Seeded Narrow-Band Amp

Soliton Self Frequency Shifting

Dual-Band SC

Er Fiber Laser

Normal Dispersion SC

ANDi fiber Laser

ANDi seeded MOPA

Ti:Saphire

SHG, THG, TPEF

SRS, CARS, Time-Resolved Raman

Transient Absorption (TAS)

IR / VO

3-Photon Absorption Rapid Delay

Scanner

Yb:KYW

Page 49: Fiber-based Ultrafast sources for Nonlinear Spectroscopy€¦ · • Fiber Lasers and Amps have HOD compression constraints Pros • Broadbandwidth:

Nonlinear Imaging Tool Kit

Imaging Modality Nonlinear Optical Element Ultrafast Sources

SC Seeded Narrow-Band Amp

Soliton Self Frequency Shifting

Dual-Band SC

Er Fiber Laser

Normal Dispersion SC

ANDi fiber Laser

ANDi seeded MOPA

Ti:Saphire

SHG, THG, TPEF

SRS, CARS, Time-Resolved Raman

Transient Absorption (TAS)

IR / VO

3-Photon Absorption Rapid Delay

Scanner

Yb:KYW

Page 50: Fiber-based Ultrafast sources for Nonlinear Spectroscopy€¦ · • Fiber Lasers and Amps have HOD compression constraints Pros • Broadbandwidth:

Rapid Delay Scanner

𝜏 𝜃𝑖 = −2𝑑𝑛𝑔𝑐

𝑛𝑔 + cos 𝜃𝑡 − cos 𝜃𝑖 − 𝜃𝑡𝑛𝑔 cos 𝜃𝑡

SRS, CARS, Time-Resolved Raman Rapid Delay

Scanner Transient

Absorption

BK7

BK7

BS

d

θi

θt

τdelay(θi)

λ/2

General Source

Page 51: Fiber-based Ultrafast sources for Nonlinear Spectroscopy€¦ · • Fiber Lasers and Amps have HOD compression constraints Pros • Broadbandwidth:

Time Resolved Raman Spectroscopy

B-PD

τ

NF

GL

WP

BK7

BS

2 pump-probe delay scans per ½ rev. 4 pump-probe delay scans per rev.

ISRS and Time-Resolved Raman

Rapid Delay Scanner Ti:Saphire

𝐸 𝑡, 𝜏 = 𝐸0𝐴 𝑡 𝑒−𝑖(𝜔𝑡−a sin Ω𝜈𝜏 )

BGO

𝐸 𝑡,Ω𝜈𝜏 = 0 ≈ 𝐸0𝐴 𝑡 𝑒−𝑖(𝜔𝑡−𝑎𝜏) For |A(t)|2 shorter than 1/Ων

ISRS and short probe pulse

Page 52: Fiber-based Ultrafast sources for Nonlinear Spectroscopy€¦ · • Fiber Lasers and Amps have HOD compression constraints Pros • Broadbandwidth:

Time Resolved Raman Spectroscopy B-PD

τ

NF

GL

WP

BK7

BS

• Increased Lighthouse speed from 15 => 175 Hz

• Currently, XPM peaks needed to temporally synch individual scans

Nearly parabolic delay-to-angle (accelerating delay rate) = detector gain bandwidth limitations

BGO

Page 53: Fiber-based Ultrafast sources for Nonlinear Spectroscopy€¦ · • Fiber Lasers and Amps have HOD compression constraints Pros • Broadbandwidth:

Time Resolved Raman Spectroscopy

Reduction in Noise by Scan Averaging

10x reduction in Raman Spectrum Background

500 scans 1 scan

Neat CCl4

Page 54: Fiber-based Ultrafast sources for Nonlinear Spectroscopy€¦ · • Fiber Lasers and Amps have HOD compression constraints Pros • Broadbandwidth:

Time Resolved Raman Spectroscopy

Chemical Imaging

“Crude” discrimination based on peak/valley comparison Principal Component Analysis would improve discrimination among target species 30 and 15 dB discrimination between BGO and CdWO4, respectively.

Page 55: Fiber-based Ultrafast sources for Nonlinear Spectroscopy€¦ · • Fiber Lasers and Amps have HOD compression constraints Pros • Broadbandwidth:

Rapid(er) Delay Scanner

• 12 kHz Resonant Galvo Mirror (RM)

• 24 kHz pump-probe delay scan rate

• Successful Proof-of-Concept Experiment

Issues to Resolve • Switch to window with Isotropic

Optical Response • Align with window at a high angle to

“amplify” the delay range Potential Use: • Generate Modulation signal by

dithering vibrational Excitation

Page 56: Fiber-based Ultrafast sources for Nonlinear Spectroscopy€¦ · • Fiber Lasers and Amps have HOD compression constraints Pros • Broadbandwidth:

Nonlinear Imaging Tool Kit

Imaging Modality Nonlinear Optical Element Ultrafast Sources

SC Seeded Narrow-Band Amp

Soliton Self Frequency Shifting

Dual-Band SC

Er Fiber Laser

Normal Dispersion SC

ANDi fiber Laser

ANDi seeded MOPA

Ti:Saphire

SHG, THG, TPEF

SRS, CARS, Time-Resolved Raman

Transient Absorption (TAS)

IR / VO

3-Photon Absorption Rapid Delay

Scanner

Yb:KYW

Page 57: Fiber-based Ultrafast sources for Nonlinear Spectroscopy€¦ · • Fiber Lasers and Amps have HOD compression constraints Pros • Broadbandwidth:

Photothermal Spectroscopy in 1.6-1.85 μm

Wang, Pu, et al. Journal of Biophotonics 5.1 (2012): 25.

Butter Fat (lipid) => CH2 Type I Collagen (protein) => CH3

Page 58: Fiber-based Ultrafast sources for Nonlinear Spectroscopy€¦ · • Fiber Lasers and Amps have HOD compression constraints Pros • Broadbandwidth:

• 80 fs FWHM seed pulse • ~100 mW (37MHz) available • Reduced to ~60 mW for 1730nm

(and 10 cm fiber) • N ~ 5.2 • Efficiency of Conversion ~ 85%

Generating Light at 1.6-1.85 μm • Modelocked Er-Doped Laser (1550 nm) • Soliton Self-Frequency Shift in

anomalous fiber • Challenge: Balancing Non-linearity and

Soliton Order. dB Linear

Page 59: Fiber-based Ultrafast sources for Nonlinear Spectroscopy€¦ · • Fiber Lasers and Amps have HOD compression constraints Pros • Broadbandwidth:

Vyas, R., et al, Applied Optics 27, (1988): 4701. RICARD-LESPADE, L., et al, Chemical Physics 𝟏𝟏𝟏, (1990): 245.

Signal Estimates for CH2 stretch

𝑠 𝑡 =𝑛𝑛𝑛𝜕𝐸0𝑙𝑧1𝜋𝜋𝐶𝑝

𝜕𝑛𝜕𝜕

1𝑎2 + 8𝐷𝑡 2

• ρ = 998.2 (kg/m3) • D = 0.143 x 10-6 (m2/s) • Cp = 4.18x 103 (J/kg-K) • dn/dt = 8 x 10-5 (K-1)

𝜕𝐸0 → � 𝜇 𝜔 𝑆 𝜔 𝑑𝜔

−∞

𝑙, 𝑧1 = 𝑧𝑅 =𝜋𝑤2

𝜆

𝑎,𝑤0 = 𝜆𝜋𝑁𝜋

, NA = 0.3

Newport Nirvana • Gain = 5.2x105 (V/W) • NEP = 3 (pW/√HZ)

Page 60: Fiber-based Ultrafast sources for Nonlinear Spectroscopy€¦ · • Fiber Lasers and Amps have HOD compression constraints Pros • Broadbandwidth:

Spectral Sensitivity Estimates for CH2 stretch Overtone

Page 61: Fiber-based Ultrafast sources for Nonlinear Spectroscopy€¦ · • Fiber Lasers and Amps have HOD compression constraints Pros • Broadbandwidth:

Modular Pathways through the Nonlinear Tool Kit

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Page 62: Fiber-based Ultrafast sources for Nonlinear Spectroscopy€¦ · • Fiber Lasers and Amps have HOD compression constraints Pros • Broadbandwidth:

Special Thanks The Bartels Ultrafast Lab Randy Bartels Philip Schlup Jeff Field David Winters David Kupka David Smith Keith Wernsing

Committee Members Amber Krummel Diego Krapf Mario Marconi Funding Sources Department of Energy National Institute of Health The Keck Foundation