Chap.7. Raman Systems Francesc Rocadenbosch ETSETB, Dep. TSC, EEF Group Campus Nord, D4-016

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DEP. OF SIGNAL THEORY AND COMMUNICATIONS
Chap.7. Raman Systems
Francesc Rocadenbosch
ETSETB, Dep. TSC, EEF Group
Campus Nord, D4-016
roca@tsc.upc.edu
DEP. OF SIGNAL THEORY AND COMMUNICATIONS
LIDAR (LASER RADAR)
RAMAN LIDAR
MEASUREMENTS:
• Direct: Concentration of chemical
species in the atmosphere such
as
SO2, NO, CO, H2S, C2H4, CH4,
H2CO, H2O, N2, O2...
• Indirect: Temperature, Humidity,
α, β, SM
INELASTIC INTERACTION
VIRTUAL LEVEL
hν *
hν
VIBRATIONALLY
EXCITED LEVEL
GROUND LEVEL
LASER TYPES:
• Ruby (λ = 694.3 nm, 347.2 nm)
• N2 (λ = 337 nm)
• Nd:YAG (λ = 1060 nm, 532 nm, 266 nm)
• Excimer (λ ~ 350 nm)
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2
RAMAN LIDAR
DEP. OF SIGNAL THEORY AND COMMUNICATIONS
LIDAR (LASER RADAR)
OPERATIONAL PRINCIPLE
1) In contrast to elastic systems, the
return wavelength, λR, is shifted
from the incident one, λ0.
2) Wavelength shift, κ, depends on
each molecular species.
λR =
λ0
1 − κλ 0
3) Very faint returns.
• requires photon counting
• very often, night-time operation
Fig. ADAPTED FROM: Inaba, H. Detection of Atoms and Molecules by
Raman Scattering and Resonance Fluorescence. In Laser Monitoring of the
Atmosphere, Hinkley, E. D., Ed.; Springer-Verlag: New York, 1976; Chap. 5,
153-236.
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RAMAN LIDAR
RAMAN SPECTRUM CHARACTERISTICS
DEP. OF SIGNAL THEORY AND COMMUNICATIONS
LIDAR (LASER RADAR)
The Raman shift, κ:
Rayleigh and Mie Scattering
1) does not depend
on the excitation
wavelength λ0 and,
2) it is specific of the
chemical species
A) Laser need not be
tunable
B) The Raman
spectrum is
characteristic of each
molecule
C) Conveys
temperature info.
Anti-Stokes
Stokes lines
Overview of the lidar backscatter signals for 532-nm laser excitation wavelength.
Fig. SOURCE: Behrendt, A., et al., “Combined Raman lidar for the measurement of atmospheric
temperature, water vapor, particle extinction coefficient, and particle backscatter coefficient”,
Appl. Opt. 41 (36), 7657-7666, (2002).
(C) F. Rocadenbosch 2005-2006
4
RAMAN LIDAR
KEY CONCEPTS
DEP. OF SIGNAL THEORY AND COMMUNICATIONS
LIDAR (LASER RADAR)
1) Raman components
• Stokes lines
– molecule gains energy from the
radiation field
– scattered radiation is at λR> λ0
• Anti-Stokes lines (λR<λ0)
2) Motivation for the “wavenumber”
concept (with κ, the Raman shift):
1
1
=
− κ , κ cm −1
λ R λ0
[
Common Raman shifts:
N2
O2
2 3 3 1 c m -1
1 5 5 6 c m -1
H 2O
3 6 5 4 c m -1
Fig. SOURCE: Inaba, H. Detection of Atoms and Molecules
by Raman Scattering and Resonance Fluorescence. In Laser
Monitoring of the Atmosphere, Hinkley, E. D., Ed.; SpringerVerlag: New York, 1976; Chap. 5, p.162.
]
3) Raman cross-sections
• dependency ∝ λ-4
dσ(π )
dσ(π )
≈ 10 −3, −4
dΩ Raman
dΩ Ray
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DEP. OF SIGNAL THEORY AND COMMUNICATIONS
LIDAR (LASER RADAR)
RAMAN LIDAR LINK-BUDGET
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6
TEMPERATURE MEASUREMENT (I)
DEP. OF SIGNAL THEORY AND COMMUNICATIONS
LIDAR (LASER RADAR)
METHODS
1) Rotational Raman (RR)
• Comparison of the envelope
shape of all the lines
• Intensity ratio of selected spectral
regions of the band
Suitable for atmospheric profiling
KEY
Raman signatures are direct
measures of the relative populations
among the internal molecular modes
• (In termal equilibrium) →
fundamental def. of temperature
2) Vibrational Raman (VR)
• +
• Intensity ratio between Stokes
and anti-Stokes components
• Width of a specific Q-branch
Suitable for high-temperature diagnostics
(e.g. flames)
Fig. SOURCE: Inaba, H. Detection of Atoms and Molecules by Raman
Scattering and Resonance Fluorescence. In Laser Monitoring of the
Atmosphere, Hinkley, E. D., Ed.; Springer-Verlag: New York, 1976;
Chap. 5, 153-236.
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7
TEMPERATURE MEASUREMENT (II)
RASC (GKSS) lidar
2) WV (water vapor
mixing ratio)
DEP. OF SIGNAL THEORY AND COMMUNICATIONS
LIDAR (LASER RADAR)
1) T (temperature)
3) α, β, SM
4) RH (humidity)
Fig. SOURCE: Behrendt, A., et al., “Combined Raman lidar for the
measurement of atmospheric temperature, water vapor, particle
extinction coefficient, and particle backscatter coefficient”, Appl.
Opt. 41 (36), 7657-7666, (2002).
(C) F. Rocadenbosch 2005-2006
8
UPC POLYCROMATOR TEST LAYOUT
DEP. OF SIGNAL THEORY AND COMMUNICATIONS
LIDAR (LASER RADAR)
H
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TEMPERATURE MEASUREMENT (III)
DEP. OF SIGNAL THEORY AND COMMUNICATIONS
LIDAR (LASER RADAR)
DISCUSSION PARAMETERS (RASC lidar LAYOUT)
Note:
ND filters are used to cope with saturation effects in the RR channels in the
lower troposfere (correction of photon-counter receiver dead-time effects).
Tab. SOURCE: Behrendt, A., et al., “Combined Raman lidar for the
measurement of atmospheric temperature, water vapor, particle
extinction coefficient, and particle backscatter coefficient”, Appl. Opt.
41 (36), 7657-7666, (2002).
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10
TEMPERATURE MEASUREMENT (IV)
DEP. OF SIGNAL THEORY AND COMMUNICATIONS
LIDAR (LASER RADAR)
Specific RR Temperature
approaches:
Use of two RR channels with opposite
temperature dependency
• + 3rd RR channel (isosbestic point)
as reference or,
• combine them to obtain a
temperature-indep. reference
N RR 2 (T )
Q (T ) =
N RR1 (T )
N ref (z ) = N RR1 ( z ) + cN RR 2 (z )
• calibrate Q(T) with a radiosonde
– find c for minimum temp. variation
Fig. SOURCE: Behrendt, A., et al., “Combined Raman lidar for the
measurement of atmospheric temperature, water vapor, particle
extinction coefficient, and particle backscatter coefficient”, Appl. Opt.
41 (36), 7657-7666, (2002).
(C) F. Rocadenbosch 2005-2006
11
DEP. OF SIGNAL THEORY AND COMMUNICATIONS
LIDAR (LASER RADAR)
TEMPERATURE MEASUREMENT (V)
Problem: Elastic cross-talk with the
RR channel
Action: Calibrate on a cirrus cloud
using
Q (T ) =
N RR 2 (T )
N RR1 (T ) − εN El ( z )
Fig. SOURCE: Behrendt, A., et al., “Combined Raman lidar for
the measurement of atmospheric temperature, water vapor,
particle extinction coefficient, and particle backscatter coefficient”,
Appl. Opt. 41 (36), 7657-7666, (2002).
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12
MOLECULAR SPECIES (GAS) DETECTION (I)
DEP. OF SIGNAL THEORY AND COMMUNICATIONS
LIDAR (LASER RADAR)
CONCEPTS:
1) The absolute concetration of each molecular species can be
performed by comparing the Raman backscattered intensity with that of
the Raman line from N2 which occupy the same volume.
1A) Raman-backscattered signal:
Pλ R (R ) = K λ R
{ [
] }
dσλ R (π )⎤
R
⎡
O (R )
tot
tot
(
)
(
)
(
)
(ξ) dξ
F
T
,
∆
λ
N
R
×
exp
−
α
ξ
+
α
R
R ⎢ R
∫
⎥
2
λ0
λR
0
R
dΩ ⎦
⎣
1B) (Oversimplified) Gas-to-N2 normalised ratio
N2-normalised cross section
Pλ X (R )
O X (R ) FX (T , ∆λ X ) N X (R ) ⎡ dσλ X (π ) dΩ ⎤ ξ(λ X )
∆τ(λ X , λ N , R ),
=
⎥
⎢
Pλ N (R ) ON (R ) FN (T , ∆λ N ) N N (R ) ⎢⎣ dσλ N (π ) dΩ ⎥⎦ ξ(λ N )
solve for Nx(R)
{
known (US-std model, radiosonde)
[
]
}
tot
(
)
where ∆τ(λ X , λ N , R ) = exp − ∫0 αtot
ξ
−
α
λX
λ N (ξ ) dξ
R
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DEP. OF SIGNAL THEORY AND COMMUNICATIONS
LIDAR (LASER RADAR)
MOLECULAR SPECIES (GAS) DETECTION (II)
1C) (Estimation of the) Differential Transmission term:
• Molecular extinction → US-std. atmosphere model + radiosonde
• Aerosol extinction → Cooperative elastic-Raman channel (N2)
– Only in hazy conditions (See Elastic-Raman inversion Sect. in Chap.7)
• Angström coefficient → E.g. Sun photometer calibration
2) The (VR) spectrum is
preferred to the (RR)
• RR lines of major
atmospheric constituents
overlap,
• large Rayleigh-Mie
cross-talk.
• In contrast, VR crosssections are usually
lower than RR ones.
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14
MOLECULAR SPECIES (GAS) DETECTION (III)
Fig.2
DEP. OF SIGNAL THEORY AND COMMUNICATIONS
LIDAR (LASER RADAR)
SOME MEASUREMENT
EXAMPLES
• Fig.1 Raman spectroscopy
from the ordinary atmosphere
• Fig.2 Molecular species in an
oil smoke plume
Fig.1
Fig. SOURCE: Inaba and Kobayasi, Opto-Electron
4, 101 (1972).
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15
WATER-VAPOR MEASUREMENT (I)
DEP. OF SIGNAL THEORY AND COMMUNICATIONS
LIDAR (LASER RADAR)
WATER-VAPOR (WV) KEYS:
• Influences convective stability (likelihood of storm initiation)
• Most active green-house gas
– it absorbs terrestrial radiation more strongly than does CO2
• Water-vapor mixing ratio (w)
w=
MWH 2O N H 2O (R )
MWDryAir N DryAir (R )
≈
MWH 2O
N H 2O (R )
MWDryAir N N 2 (R ) / 0.78
≈ 0.485
N H 2O (R )
N N 2 (R )
– where MWx stands for molecular weight (≈ 18g/mol for H2O and ≈ 28.94
g/mol for dry air) and Nx stands for molecule number concentration.
• Importance of the mixing ratio:
– It is conserved in atmospheric processes that do not involve condensation or
evaporation
– Serves well as a tracer of the movement of air parcels in the atmosphere
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16
WATER-VAPOR MEASUREMENT (II)
DEP. OF SIGNAL THEORY AND COMMUNICATIONS
LIDAR (LASER RADAR)
DERIVATION FROM THE RAMAN CHANNELS
From Eq.(1B) in Slide 12
Pλ H (R ) OH (R ) FH (T , ∆λ R ) N H (R ) ⎡ dσλ H (π ) dΩ ⎤ ξ(λ H )
∆τ(λ H , λ N , R )
=
⎥
⎢
Pλ N (R ) ON (R ) FN (T , ∆λ R ) N N (R ) ⎢⎣ dσλ N (π ) dΩ ⎥⎦ ξ(λ N )
and the definition of the mixing ratio (w)
ON (R ) ⎡ dσλ N (π ) dΩ ⎤ ξ(λ N ) FN (T , ∆λ N ) PH (R )
w = 0,485
∆τ(λ N , λ H , R )
⎢
⎥
OH (R ) ⎢⎣ dσλ H (π ) dΩ ⎥⎦ ξ(λ H ) FH (T , ∆λ H ) PN (R )
System’s calibration factor,
k*(R)
Temperaturedependent ratio
Measurement
factor
– where Px(R) are background-substracted quantities.
In summary,
w = k L* (R )
FN (T , ∆λ N )
Rw (R )∆τ(λ N , λ H , R )
FH (T , ∆λ H )
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Rw =
PH (R )
PN (R )
17
WATER-VAPOR MEASUREMENT (III)
EXAMPLE
DEP. OF SIGNAL THEORY AND COMMUNICATIONS
LIDAR (LASER RADAR)
• In the UV (λL=355 nm), Raman channels: λN=387 nm, λH=408 nm
*
(R )
w = k355
SPECIES
Air
O2
N2
H2O
FN (T , ∆λ N ) PH (R )
∆τ(λ N , λ H , R )
FH (T , ∆λ H ) PN (R )
kappa
(cm-1)
0
1556
2331
3654
lambdaR (1)
(nm)
354,7
375,4
386,7
407,5
lambdaR (2)
(nm)
532,1
580,1
607,4
660,5
*
≈ 0.22
k355
ON (R ) ξ(λ N )
OH (R ) ξ(λ H )
Cross sections are
computed assuming a λ-4
dependency
i.e. higher in the UV than in
the NIR
Excitation wavelength (lambda0)
(1)
354,7 nm (Nd:YAG, THG)
(2)
532,1 nm (Nd:YAG, SHG)
Water-Vapor Mixing Ratio Error
2
2
2
σ2w σk * σ Rw σ2∆τ σ Rw
= *2 + 2 + 2 ≈ 2 ;
2
w
k
Rw ∆τ
Rw
Rw =
PH (R )
PN (R )
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WATER-VAPOR MEASUREMENT (IV)
ERROR SOURCES AND UNCERTAINTIES
DEP. OF SIGNAL THEORY AND COMMUNICATIONS
LIDAR (LASER RADAR)
• Water-Vapor Mixing Ratio Error
σ
σ
PH (R )
= *2 + 2 +
≈ 2 ;
Rw =
w
k
Rw ∆τ
Rw
PN (R )
• k*: Calibration factor → Can be considered to be small
2
w
2
σk2*
σ2Rw
2
∆τ
2
σ2Rw
– Calibrated using a radiosonde (e.g. VAISALA RS80-A) or a MW radiometer
• Rw: Signal-induced statistical error dominates the error budget
• ∆τ(λ N ,λ H , R ) = Differential Transmission (DT).
– λN and λH experience different amounts of attenuation on their return trips,
caused mainly by Rayleigh scattering. The DT can be calibrated by using
1) A radiosonde estimate the molecular number density (i.e, T(z), P(z))
2) For hazy atmospheres (DT < 0.9 for τPBL > 2), the N2-Raman channel is
used to estimate the aerosol extinction (typ., λ-1 dependence)
See Sec. Inversion of Optical Parameters / Extinction inversion, αλaerH , αλaerN
Note: WV absorbs weakly at λH=660 nm ⇒ λL=355 nm preferred to 532 nm
Fig. SOURCE: Inaba, H. Detection of Atoms and Molecules by Raman Scattering and Resonance Fluorescence. In Laser Monitoring of the
Atmosphere, Hinkley, E. D., Ed.; Springer-Verlag: New York, 1976; Chap. 5, p.162.
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19
DEP. OF SIGNAL THEORY AND COMMUNICATIONS
LIDAR (LASER RADAR)
WATER-VAPOR MEASUREMENT (V)
Fig. SOURCE: Goldsmith, J.E.M., et al., “Turn-key Raman lidar for
profiling atmospheric water vapor, clouds, and aerosols”, Appl. Opt.
27 (21), 4979-4990, (1998).
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20
RELATIVE HUMIDITY MEASUREMENT
DEP. OF SIGNAL THEORY AND COMMUNICATIONS
LIDAR (LASER RADAR)
KEY
• Water-vapor mixing ratio (wH2O) + Temperature profile ⇒ RH
• Derivation of the RH profile emerges from specific physical refs.1,2
e( z )
RH (z ) =
ew (z )
where e(z) is the WV pressure, and ew(z) is the saturation pressure,
e( z ) =
P (z )wH 2O (z )
0.622 + wH 2O (z )
,
⎧ M A [T (z ) − 273] ⎫
ew (z ) = 6.107 exp ⎨
⎬
[
(
)
]
M
T
z
+
−
273
⎩ B
⎭
– MA=17.84, 17.08 and MB=245.4, 234.2 for T < and > 273 K, respectively.
REFERENCES:
1) R.R. Rogers and M.K. Yau, A Short Course in Cloud Physics (Pergamon, New York ,1988).
2) R.J. List, ed., Smithsonian Meteorological Tables (Smithsonian Institution, Washington, D.C., 1951).
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21
A COMPLETE RAMAN SYSTEM
DEP. OF SIGNAL THEORY AND COMMUNICATIONS
LIDAR (LASER RADAR)
LAYOUT
•
•
•
•
3 unshifted returns (1064, 532, 355 nm), NO polarization
4 returns (Stokes and anti-Stokes portions) of the N2 RR spectrum
3 vibrational Raman returns (N2 at 387, 607 nm and H2O at 407 nm)
2 returns from the parallel and cross-polarized unshifted 532 nm
Fig. SOURCE: Matthis, I, Ansmann, A et al., “Relative-humidity profiling in the troposphere with a Raman lidar”, Appl. Opt. 41 (30), 64516462, (2002).
(C) F. Rocadenbosch 2005-2006
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A COMPLETE RAMAN SYSTEM
DEP. OF SIGNAL THEORY AND COMMUNICATIONS
LIDAR (LASER RADAR)
COMPOSITE OUTPUTS
Fig. SOURCE: Matthis, I, Ansmann, A et al.,
“Relative-humidity profiling in the troposphere with a
Raman lidar”, Appl. Opt. 41 (30), 6451-6462, (2002).
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23
INVERSION OF OPTICAL PARAMETERS (I)
DEP. OF SIGNAL THEORY AND COMMUNICATIONS
LIDAR (LASER RADAR)
PRINCIPLE
1) Two receiving channels: Besides the ELASTIC receiver, which is only
sensitive to the elastic return, another receiver -i.e., the RAMAN receiveris spectrally tuned to the Raman-shifted wavelength (Q-branch) of any
abundant species of known relative concentration (usually N2).
2) From:
• radiosoundings or
• ground-level measurements of pressure and temperature +
assumption of a standard atmosphere,
the N2 concentration -as a function of the range to the lidar- is inferred.
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24
INVERSION OF OPTICAL PARAMETERS (II)
DEP. OF SIGNAL THEORY AND COMMUNICATIONS
LIDAR (LASER RADAR)
Raman-backscattered signal:
Pλ R (z ) = K λ R
dσ λ R (π ) ⎤
O (z ) ⎡
z mol
aer
mol
aer
(
)
(
)
(
)
(
)
(ξ) dξ
×
exp
−
α
ξ
+
α
ξ
+
α
ξ
+
α
N
z
∫
⎥
⎢
R
2
λ0
λR
λR
0 λ0
dΩ ⎦
z ⎣
{ [
]}
Scattering wavelength dependency: λ-κ
α aer
λ
0
α aer
λ
R
⎛ λ0
= ⎜⎜
⎝ λR
⎞
⎟⎟
⎠
−κ
Raman-channel inverted extinction:
d ⎡
N R (z ) ⎤
mol
mol
(
)
(z )
z
−
α
−
α
⎥
⎢ln
2
λ0
λR
dz ⎢ Pλ (z )z ⎥
INVERTED ATMOSPHERIC
R
aer
⎦
⎣
α λ (z ) =
k
0
OPTICAL PARAMETERS
⎛ λ0 ⎞
⎟⎟
1 + ⎜⎜
⎝ λR ⎠
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25
INVERSION OF OPTICAL PARAMETERS (III)
Backscatter inversion requires:
• combination of lidar returns from both elastic and Raman channels
DEP. OF SIGNAL THEORY AND COMMUNICATIONS
LIDAR (LASER RADAR)
aer
βλ
0
(z ) = −β λ0
mol
Pλ R (z0 )Pλ 0 (z )N R (z )
aer
mol
⎡
⎤
(z ) + ⎢β λ0 (z0 ) + β λ0 (z0 )⎥ ×
×
⎣
⎦ Pλ 0 (z0 )Pλ R (z )N R (z0 )
[
{
×
exp{− ∫ [α
] }
;
(ξ)]dξ}
mol
(
)
(ξ) dξ
exp − ∫z αλaer
ξ
+
α
λ
R
R
z
0
z
z0
aer
λ0
(ξ)
+ αλmol
0
z ≥ z0
• a backscatter calibration at some height R0 so that
aer
mol
⎡
βλ (R0 ) >>βλ (R0 ) → βλ (R0 ) +βλ (R0 )⎤
⎢⎣ 0
⎥⎦
0
0
0
mol
aer
The lidar ratio is found as
Sλaer
( z) =
0
⎤
⎡
⎥
⎢
aer
aer
P, T ⎥
β λ (R ) = f ⎢ Pλ0 , Pλ R , αλ 0 , N R , {
0
424
3
⎥
⎢1
Rayleigh
⎢ channel
comp. ⎥
⎦
⎣ returns
αλaer0 (z )
βλaer0 (z )
(C) F. Rocadenbosch 2005-2006
26
73.8
0.5
73.6
0.3
73.4
0.1
73.2
-0.1
73
-0.3
72.8
0
1
ML estim
2
3
4
Range [km]
5
6
d/dR[ ln(.) ] [a.u.]
2
ln(N/[R ·z(R)]) [a.u.]
DEP. OF SIGNAL THEORY AND COMMUNICATIONS
LIDAR (LASER RADAR)
4. INVERTED OPTICAL PARAMETERS
-0.5
ML estim
∑ σ i2
S
Sˆ =
i
∑σ 2
1
i
(C) F. Rocadenbosch 2005-2006
27
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