Transcript Slide 1

Assigned Reading for Next Week
1. Campagnola, P.J., et al., High resolution non-linear optical microscopy
of living cells by second harmonic generation.
Biophys. J., 1999. 77: p. 3341-3349.
2. Campagnola, P.J., et al., 3-Dimesional High-Resolution
Second Harmonic Generation Imaging of Endogenous Structural
Proteins in Biological Tissues. Biophys. J., 2002. 82: p. 493-508.
3. Moreaux, L., O. Sandre, and J. Mertz, Membrane imaging
by second-harmonic generation microscopy.
J. Opt. Soc. Am. B, 2000. 17: p. 1685-1694.
Outline:
1) Fluorescence Lifetime Imaging (FLIM)
2) Fluorescence Resonance Energy Transfer (FRET)
3) FRET/FLIM
Fluorescence Lifetime motivation
1) Sensitive to environment: pH, ions, potential
SNARF, Calcium Green, Cameleons
Perform in vitro calibrations
1) Results Not sensitive to bleaching artifacts
2) Not sensitive to uneven staining (unless self-quenched)
3) Not sensitive to alignment (intensity artifacts)
Fluorescence Quantum Yield φ: important for dyes
Ratio of emitted to absorbed photons
Quantum Yield:

Very fast
1-10 ps

kf
k f  k isc
(k is rate,
Inverse of time)
kf
k f  k isc  k nonrad
 0 1  k f
Natural lifetime
 1  k f  kisc
Measured lifetime is sum of
Rates of natural lifetime
and non radiative decay paths
Oscillator strength, f, and fluorescence lifetime τ
Einstein A coefficient A21=1/τ
f 21
m c3

A21
2 2
8o e
υ=light frequency, m=mass of electron,
c=speed of light, e= electron charge
For band centered at 500 nm,
Fully allowed transition has lifetime of 4 ns
(for one electron)
Dyes has several valence electrons, larger f
Lifetimes between 1-4 ns
Fluorescent lifetime depends on environment:
Used in microscopy as contrast
Unquenched and Quenched Emission
Unquenched emission:
Normal QY, lifetime

kf
k f  k isc
Quenched emission
Decreased QY, lifetime
e.g. metals, aggregation

kf
k f  k isc  k nonrad
Gold somewhat quenches
the fluorescence
2 general approaches: time domain and frequency domain
Short pulse laser modulate CW laser
Frequency Domain Methods for Lifetime Measurements:
Modulate laser and measure phase change of fluorescence
Use cw laser (e.g. argon ion)
Modulate at rate near
Inverse of emission lifetime
10-100 MHz (100 to 10 ns)
Measure phase change
with Lockin amplifier
Modulation Methods in Frequency Domain
Modulate laser
OK for spectroscopy
Modulate laser and ICCD
(intensified CCD camera)
Better S/N for imaging
ICCD Detectors for Lifetime measurements:
Frequency domain and some time-domain
Microchannel plates
Amplify signal ~10 fold
Needs to be gated rapidly
Widefield imaging (no sectioning)
High quantum yield
Very expensive $20-80K
Regular CCDs:10-20K
Historically Most common
Time-domain Widefield Lifetime imaging with ICCD
Variable delayed gate or many gates
is scanned
To sample exponential decay:
Many frames (for each delay)
ICCD has no time intrinsic response: slow readout gated gain.
Use laser pulse width much less than fluorescence lifetime
Two-photon scope has short pulse laser for time-gating
Ti:sapphire
Higher viscosity
Shorter lifetime
Better chance for
Non-radiative decay
French
Optics express
Time domain methods for lifetime measurements
With gated electronics and fast detectors (not gain modulated)
Best for point detection, PMT on laser scanning
Collect data from multiple gates (windows)
At the same time, fit to exponential
Synchronized Gating done by pulsed laser
(e.g. ti:sapphire laser)
PMT Detectors for Lifetime measurements
Dispersion in time of flight
across 14 dynodes
Limits time response
~300 picosecond resolution
Better with deconvolution
Cost ~$500
Microchannel plate photomultiplier: full of holes, kick off electrons
~30 picosecond resolution
No dispersion
Cost ~$15000
fragile
PMTS have low quantum yield
(10-20%), MCP worse ~5%
Avalanche Photodiode (APD)
300-500 picosecond resolution
Very small area (200 sq microns)
Not good for scanning
High quantum yield (up to 70% at 700 nm)
Low count rate (~10 MHz)
$5K
Extremely fragile!!
Time gating measurements of fluorescence decay
Temporal Resolution defined by IRF (laser, detector, electronics)
Ideal IRF
IRF=instrument response function,
Must be (much) shorter than
fluorescence lifetime
(delta function)
to avoid convolution
Real IRF
Gate away from IRF
(laser pulse, PMT response)
Lose photons
Measure IRF with reflection
or known short lifetime
e.g. Rose Bengal (90 ps)
Practical limiting governing of the
Instrument Response Function
1) Laser
modern lasers: ti:sapphires 100 femtosecond
Lifetimes: nanoseconds
Not a factor
Was 20-30 years ago before modelocked lasers
2) Detectors
APD or PMT response ~200 picoseconds: can be
MCP-PMT 30 ps: not typical limitation
3) TCSPC or gating Electronics
20-50 ps (depending on sophistication)
Can be convolved with MCP-PMT response
Time-correlated single photon counting:
•most flexibility, most accurate,
•samples whole decay
•Best time response
Measures time of flight of photons
After excitation pulse
Bins data at each time interval
Rather than gating
Collect enough photons to
approximate exponential:
Slower than gating but
Better measurement,
Can separate biexponentials:
Multiple components
Principles of time-correlated single photon counting
Been around
For decades
TAC or TDC measures time of flight, bins photons
Mark Terasaki Flash animation
http://www.terasaki.us/flash/lab/flim01.swf
Time-Correlated Single Photon Counting electronics
On laser scanning microscope (recent)
TCSPC electronics synchronized with
laser scanning electronics:
Pixel, line, frame synch
Historically very hard: mostly homebuilt (e.g. Gerritsen)
Becker & Hickel addon to Zeiss Laser scanning confocal
Electronics all in one PCI board, ~50K addon
Intensity vs fluorescence lifetime image
Quenched close to
Nucleus due to
Higher concentration
Lower lifetime
Same dye, different lifetime because of environment
Intensity and lifetime measurements
CFP-YFP linked by short peptide chain
Energy is transferred from CFP to YFP
Lifetime reveals info intensity does not
TCSPC FLIM using ECFP
2 distinct lifetimes: meaning?
Duncan, J. Microscopy 2004
GFP lifetime increases
With increasing viscosity
Limits motion, nonrad
Different lifetime for B cells
at immuno Junction
with natural killer (NK) cell
EGFP::MHC
Performance of Frequency and time domain methods
TCSPC best for efficiency, S/N, information content
But more expensive (ti:sapphire laser)
But already have if have 2-photon microscope
Long Acquisition Times for TCSPC FLIM:
Need enough data to approximate decay
Bright stains
106/s
Dim stains
104/s
need
100-100000
Photons/pixel
May bleach before done imaging
Detection with 2-4 gates may be better if
Short on photons
Autofluorescence of Rat Ear
Contains collagen, elastin :
Single exponential not sufficient for multiple components
Time domain
With gated ICCD
Fits to two discrete
components noisy (large residuals)
French, 2001, Biophys J.
Continuous lifetime distribution
Better for multiple components
Mean tau
For pixels
Unless know components
Stretched exp is better
Representative of physiology
and provides more data
Width, h, of
distribution
For pixel
FLIM as Diagnostic of Joint Disorder
H&E staining
Widefield
fluorescence
Widefield
FLIM
Fixed, thin sections
(few microns)
Little info
Detail revealed by FLIM
FLIM as Cancer Diagnostic
H&E staining Widefield FLIM
Benign
More contrast
Than H&E
Carcinoma
Probably
NADH, FAD
FLIM shows morphology like H&E histology
Can optically section and no staining with FLIM
With 2-p can do thick tissues (few hundred microns)
FLIM Diagnostics of arterial plaque
Widefield
auto
fluorescence
Widefield
FLIM
Clear lifetime
Difference in
Normal and plaque:
Not visible by
Fluorescence intensity
FLIM via endoscope as clinical tool
Works like through microscope
White PNAS
2007
Lifetime of NADH, FAD changes from normal
To cancer and high to low-grade
Fluorescence Resonance Energy Transfer (FRET)
Donor
Excitation
Donor
Excitation
Acceptor
Emission
Donor Emission
Donor emission overlaps with Acceptor Absorption:
Highly distance dependent
FRET probes conformational changes
Different conformation gives
Different FRET signature
Inter and Intramolecular
Forms of FRET with
Proteins
CFP-YFP good combo
FRET increases
In both cases
Protein-Protein Interactions
In cytoplasm and
membranes
When FRET Occurs
No FRET for
No overlap of donor emission,
acceptor absorption
No FRET for
Orthogonal dipole
orientation
No FRET for molecules
more than 10 nm apart
R0=distance where FRET=0.5
Typical Values of Ro
green
Donor
Fluorescein
IAEDANS
Acceptor
Ro (Å)
Tetramethylrhodamine 55
Fluorescein
46
EDANS
DABCYL
Fluorescein Fluorescein
BODIPY FL BODIPY FL
33
44
57
Fluorescein
Cy3
CFP
61
53
50
QSY 7 dye
Cy5
YFP
GFPs and other colored “FPs have
transformed FRET microscopy
Before had to label proteins, then introduce
red
Number of FRET Publications since 1989
Fluorescence Resonance Energy Transfer Detection of Probe Proximity
F  FD
FA  F
  D
FRET 
 Max

0
0
FD
FA  FA
 D0
0
D
0
A
0
D
R0 typically 40-50 Angstroms
50% transfer
6
0
R
FRET  6
R  R06
Practical Challenges to FRET Quantitation
•
•
•
•
Emission from A contaminates D channel (filters)
Emission from D contaminates A channel
Unknown labeling levels for D and A
Signal variation due to bleaching
– Complicates kinetic studies
– Bleaching rate of D can actually be slowed by FRET
Solutions:
• Separately labeled D and A controls to define
bleedthrough
0
F
• Acceptor destruction by photobleaching to establish D
• Dual wavelength ratio imaging to normalize away
variations in label levels and bleaching effects
Want sharp filters,
But throw away photons
Fluorescent Proteins as D-A Pairs
Issue of Spectral Overlap
Better overlap,FRET
But more bleedthrough
Poor Spectral overlap,
But less bleedthrough
Survey of FRET-Based
Assays
•
•
•
•
•
•
•
Protease activity
Calcium Ion measurements
cAMP
Protein tyrosine kinase activity
Phospholipase C activity
Protein kinase C activity
Membrane potential
Principle of Operation of Chameleon Calcium Indicators
FRET Increases when CaM binds Calcium ions
Conformation changes, CFP-YFP closer together
Potential Sensor Based on FRET
Donor= Di4-ANEPPS
Fast voltage sensor
Acceptor=Oxonol
Slow voltage sensor
FRET pair more sensitive
Mechanism and Single Cells
Gonzalez and Tsien, Biophys J., 1995
Improved indicators
Gonzalez JE, Tsien RY. 1997.
Chemistry and Biology 4:269-277.
Demonstration on Leech Ganglion
Kleinfeld, et al., Neuron, 1999
Lifetime and FRET
Large change in lifetime for quenched donor upon FRET
F  FD
FA  F
  D
FRET 
 Max

0
0
0
FD
FA  FA
D
0
D
0
A
0
D
FRET should have bi-exponential decay,
quenched and unquenched:
Short and long lifetime components
CFP and YFP FRET by Lifetime Imaging
Channel changes conformation, distance changes,
Donor quenching occurs due to FRET
Short lifetime is FRET from Donor
For given pixel Ratio of fast to slow decay coefficients
is estimate of FRET efficiency
CFP and YFP tethers FRET by Lifetime Imaging
Donor Lifetime goes up post acceptor bleaching
Duncan, J. Microscopy 2004
FRET Outcomes
Donor
decreases
Acceptor
increases
Donor lifetime
decreases
With FRET:
Donor fluorescence
Anisotropy increases
Acceptor decreases
FRET pair anisotropy
Donor Anisotropy
Increases: shorter
Lifetime, less likely to
Rotate before emission
Emission dipole usually
Parallel to excitation dipole:
FRET to other orientation
Depolarizes acceptor emission
Not constrained by laser
Extent of depol
Contains relative
orientation
Piston, BJ
2004
Much better dynamic range
Than lifetime based changes ~10x
Anisotropy measurement more accurate