Arthur H. Carrieri,
Jerold R. Bottiger,
David J. Owens,
and Erik S. Roese
A. H. Carrieri and J. R. Bottiger are with the U.S. Army Chemical and Biological Defense Command, Edgewood Research, Development and Engineering Center, Research and Technology Directorate, Aberdeen Proving Ground, Maryland 21010-5423.
D. J. Owens and E. S. Roese are with Quetron Systems, Incorporated, 4 Newport Drive, Suite F, Forrest Hill, Maryland 21050.
Arthur H. Carrieri, Jerold R. Bottiger, David J. Owens, and Erik S. Roese, "Differential absorption Mueller matrix spectroscopy and the infrared detection of crystalline organics," Appl. Opt. 37, 6550-6557 (1998)
The complete 16-element Mueller matrices for backscattering from
amino acids, sugars, and other enantiomorphic compounds pressed into
wafer form were measured at infrared wavelengths. For each compound
a pair of CO2 laser lines was selected from the
9.1–11.6-μm region such that one line excited an absorption
band in the compound, whereas the other did not. It was observed
that at least some of the matrix elements differed significantly
depending on which of the two wavelengths was used in the
measurement. We propose that a neural network pattern recognition
system can be trained to detect the presence of specific compounds
based on multiwavelength backscatter Mueller matrix
measurements.
Arthur H. Carrieri, Jack Copper, David J. Owens, Erik S. Roese, Jerold R. Bottiger, Robert D. Everly, II, and Kevin C. Hung Appl. Opt. 49(3) 382-393 (2010)
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Axial Orientations of the Polarimeter’s Linear Polarizer
and Photoelastic Modulator (PEM) Opticsa
Case
Transmitter
Receiver
Linear Polarizer
Photoelastic Modulator
Photoelastic Modulator
Linear Polarizer
A
Vertical
-45°
+45°
Vertical
B
Vertical
-45°
Vertical
-45°
C
+45°
Vertical
Vertical
-45°
D
+45°
Vertical
+45°
Vertical
The vertical direction is perpendicular
to the plane of the instrument’s platform. The sign is relative to
transmitted and backscattered (received) beam wave vectors, i.e.,
along the optical axes when viewing the laser and scattering source,
respectively. A different set of 9 out of 16 Mueller matrix
elements is produced per optical orientation, labeled case A–D.
Table 2
Configurations in which the Mueller Matrix Elements are
Accessible for Measurementa
M
11
M
12
M
13
M
14
Case A
dc
2ω1
0
ω1
Case B
dc
2ω1
0
ω1
Case C
dc
0
2ω1
ω1
Case D
dc
0
2ω1
ω1
M
21
M
22
M
23
M
24
2ω2
2ω2- 2ω1
0
ω1+ 2ω2
0
0
0
0
0
0
0
0
2ω2
0
2ω2- 2ω1
ω1+ 2ω2
M
31
M
32
M
33
M
34
0
0
0
0
2ω2
2ω2- 2ω1
0
ω1+ 2ω2
2ω2
0
2ω2- 2ω1
ω1+ 2ω2
0
0
0
0
M
41
M
42
M
43
M
44
ω2
2ω1+ ω2
0
ω1+ ω2
ω2
2ω1+ ω2
0
ω1+ ω2
ω2
0
2ω1+ ω2
ω1+ ω2
ω2
0
2ω1+ ω2
ω1+ ω2
ω1 and ω2 are
lock-in frequencies from transmitter and receiver photoelastic
modulators, respectively.
Table 3
Measured Polarization Signatures of Some Organic
Wafersa
Compound
Formula or Nomenclature
Mueller Element (Mi,j)
Off-Resonance Reciprocal Wavelength (1/λo, in cm-1)
Normalized Mi,j(α = 90°, λo) (one SD)
On-Resonance Reciprocal Wavelength (1/λr, in cm-1)
Normalized Mi,j(α = 90°, λr) (one SD)
Scaled Difference ΔMi,js(α = 90°, λo, λr)
Correlation of Elements On and Off Resonance
DL-alanine (racemic amino acid)
CH3CH(NH2)--COOH
1,2
1049.3
-0.094 (0.169)
1024.6
0.180 (0.093)
1.340
-0.071
4,3
0.086 (0.041)
-0.022 (0.022)
-0.114
-0.035
3,1
0.246 (0.112)
920.0
0.001 (0.023)
-0.698
-0.135
4,3
0.086 (0.041)
-0.009 (0.010)
-0.091
-0.058
1,2
-0.094 (0.169)
851.8
0.169 (0.082)
0.876
-0.049
4,3
0.086 (0.041)
0.008 (0.019)
-0.079
-0.014
L-alanine (amino acid)
CH3CH (NH2)-COOH
4,2
1050.4
0.004 (0.048)
1024.6
0.111 (0.035)
0.162
-0.024
1,2
-0.001 (0.124)
919.1
0.215 (0.087)
0.274
-0.017
4,3
0.021 (0.034)
851.8
-0.023 (0.012)
-0.029
-0.045
DL-aspartic (amino) acid
HOOCCH2CH-(NH2)COOH
4,3
999.0
0.053 (0.021)
1071.8
0.021 (0.011)
-0.020
-0.070
(1R)-(+)-camphor
1,7,7-Trimethyl-[2.2.1]heptan-2-one
1,2
838.9
0.223 (0.036)
1044.9
-0.056 (0.016)
-0.214
-0.527
2,1
-0.040 (0.070)
0.109 (0.033)
0.489
-0.352
(1S)-(-)-camphor
C10H16O
4,3
935.5
0.019 (0.005)
1042.8
0.004 (0.010)
-0.003
-0.070
D-fructose (fruit sugar)
C6H12O6
1,2
861.3
0.471 (0.096)
977.5
-0.113 (0.096)
-1.683
-0.001
1,2
0.471 (0.096)
1082.3
0.145 (0.055)
-0.554
-0.248
1,3
-0.070 (0.017)
-0.003 (0.028)
0.043
-0.005
1,4
0.033 (0.016)
-0.008 (0.014)
-0.022
-0.045
2,1
0.014 (0.164)
0.647 (0.124)
2.949
-0.038
D-glucose (blood sugar)
C6H12O6
2,4
932.0
0.112 (0.016)
838.9
0.087 (0.033)
-0.023
-0.020
L-histidine (amino acid)
Glyoxaline-5-alanine
1,2
1025.6
0.132 (0.075)
977.5
-0.001 (0.037)
-0.273
-0.069
2,1
0.269 (0.175)
-0.082 (0.077)
-1.757
-0.104
3,4
-0.087 (0.053)
968.1
0.033 (0.025)
0.194
-0.022
3,4
-0.087 (0.053)
923.4
0.021 (0.022)
0.169
-0.054
2,1
0.269 (0.175)
838.9
-0.023 (0.191)
-1.991
-0.054
2,3
0.015 (0.022)
-0.024 (0.015)
-0.033
-0.002
D-mannose (α-form sugar)
C6H12O6
1,2
899.3
0.333 (0.133)
1040.0
-0.016 (0.034)
-0.852
-0.015
2,3
0.009 (0.018)
969.9
-0.035 (0.009)
-0.021
-0.025
L-serine (amino acid)
HOCH2CH--(NH2)COOH
1,2
945.2
0.319 (0.147)
1012.1
0.092 (0.072)
-0.782
-0.064
2,3
0.011 (0.029)
-0.025 (0.005)
-0.031
-0.037
4,3
0.091 (0.037)
0.014 (0.003)
-0.055
-0.077
4,3
0.091 (0.037)
1039.5
-0.017 (0.025)
-0.102
-0.053
L-sorbose (open ring sugar)
C6H12O6
1,3
849.6
0.000 (0.008)
829.9
0.026 (0.004)
0.003
-0.017
3,2
-0.023 (0.004)
-0.006 (0.004)
0.002
-0.001
4,2
0.006 (0.006)
0.018 (0.006)
0.001
-0.057
4,3
0.010 (0.004)
0.021 (0.004)
0.001
-0.057
2,4
0.013 (0.008)
992.1
-0.033 (0.033)
-0.051
-0.034
4,2
0.006 (0.006)
0.052 (0.021)
0.019
-0.080
1,3
0.000 (0.008)
1048.2
0.204 (0.034)
0.168
-0.048
2,1
-0.147 (0.049)
0.114 (0.167)
0.549
-0.237
3,4
0.004 (0.008)
-0.074 (0.033)
-0.077
-0.002
DL-tartaric acid (racemic acid)
2-dihydroxy- butanedioic acid
2,4
-0.081 (0.059)
887.3
0.036 (0.027)
0.211 (0.112)
-0.075
4,2
0.075 (0.042)
0.007 (0.019)
-0.068 (0.053)
-0.019
L-tartaric acid (fruit acid)
[R-(R*, R*)]-2,3- dihydroxy- butanedioic acid
1,3
1029.9
0.058 (0.015)
1082.3
0.188 (0.030)
0.105 (0.029)
-0.001
2,1
0.208 (0.126)
0.704 (0.154)
1.587 (1.081)
-0.089
3,1
0.120 (0.056)
-0.310 (0.092)
-1.101 (0.270)
-0.074
3,4
-0.039 (0.014)
0.131 (0.020)
0.099 (0.015)
-0.031
4,3
-0.038 (0.007)
0.011 (0.013)
0.003 (0.005)
-0.060
D-tartaric acid (levorotatory/ dextro config.)
[S-(R*, R*)]-2,3-dihydroxy-butanedioic acid
1,3
1029.9
0.081 (0.035)
1082.3
0.396 (0.085)
0.552 (0.222)
-0.080
4,3
0.002 (0.014)
0.062 (0.030)
0.011 (0.032)
-0.198
L-tryptophan (amino acid)
2-amino-3- propionic acid
4,3
833.3
0.036 (0.020)
1005.0
-0.006 (0.011)
-0.020 (0.013)
-0.028
L-tyrosine (amino acid)
β-(p-hydroxy- phenyl) alanine
3,4
925.1
0.117 (0.063)
878.7
0.003 (0.020)
-0.190 (0.112)
-0.048
1,2
0.299 (0.148)
1095.3
-0.007 (0.098)
-1.210 (0.838)
-0.074
4,3
-0.041 (0.023)
0.049 (0.024)
0.076 (0.029)
-0.073
The scaled difference
(ΔMi,js) and negative
correlation coefficients of elements are major features for pattern
recognition and detection of the organic. λ0 and
λr are beam wavelengths on resonance and off
resonance of molecular absorption, respectively; α is the scattering
beam orientation; and α = 90° is the normal beam incidence.
Tables (3)
Table 1
Axial Orientations of the Polarimeter’s Linear Polarizer
and Photoelastic Modulator (PEM) Opticsa
Case
Transmitter
Receiver
Linear Polarizer
Photoelastic Modulator
Photoelastic Modulator
Linear Polarizer
A
Vertical
-45°
+45°
Vertical
B
Vertical
-45°
Vertical
-45°
C
+45°
Vertical
Vertical
-45°
D
+45°
Vertical
+45°
Vertical
The vertical direction is perpendicular
to the plane of the instrument’s platform. The sign is relative to
transmitted and backscattered (received) beam wave vectors, i.e.,
along the optical axes when viewing the laser and scattering source,
respectively. A different set of 9 out of 16 Mueller matrix
elements is produced per optical orientation, labeled case A–D.
Table 2
Configurations in which the Mueller Matrix Elements are
Accessible for Measurementa
M
11
M
12
M
13
M
14
Case A
dc
2ω1
0
ω1
Case B
dc
2ω1
0
ω1
Case C
dc
0
2ω1
ω1
Case D
dc
0
2ω1
ω1
M
21
M
22
M
23
M
24
2ω2
2ω2- 2ω1
0
ω1+ 2ω2
0
0
0
0
0
0
0
0
2ω2
0
2ω2- 2ω1
ω1+ 2ω2
M
31
M
32
M
33
M
34
0
0
0
0
2ω2
2ω2- 2ω1
0
ω1+ 2ω2
2ω2
0
2ω2- 2ω1
ω1+ 2ω2
0
0
0
0
M
41
M
42
M
43
M
44
ω2
2ω1+ ω2
0
ω1+ ω2
ω2
2ω1+ ω2
0
ω1+ ω2
ω2
0
2ω1+ ω2
ω1+ ω2
ω2
0
2ω1+ ω2
ω1+ ω2
ω1 and ω2 are
lock-in frequencies from transmitter and receiver photoelastic
modulators, respectively.
Table 3
Measured Polarization Signatures of Some Organic
Wafersa
Compound
Formula or Nomenclature
Mueller Element (Mi,j)
Off-Resonance Reciprocal Wavelength (1/λo, in cm-1)
Normalized Mi,j(α = 90°, λo) (one SD)
On-Resonance Reciprocal Wavelength (1/λr, in cm-1)
Normalized Mi,j(α = 90°, λr) (one SD)
Scaled Difference ΔMi,js(α = 90°, λo, λr)
Correlation of Elements On and Off Resonance
DL-alanine (racemic amino acid)
CH3CH(NH2)--COOH
1,2
1049.3
-0.094 (0.169)
1024.6
0.180 (0.093)
1.340
-0.071
4,3
0.086 (0.041)
-0.022 (0.022)
-0.114
-0.035
3,1
0.246 (0.112)
920.0
0.001 (0.023)
-0.698
-0.135
4,3
0.086 (0.041)
-0.009 (0.010)
-0.091
-0.058
1,2
-0.094 (0.169)
851.8
0.169 (0.082)
0.876
-0.049
4,3
0.086 (0.041)
0.008 (0.019)
-0.079
-0.014
L-alanine (amino acid)
CH3CH (NH2)-COOH
4,2
1050.4
0.004 (0.048)
1024.6
0.111 (0.035)
0.162
-0.024
1,2
-0.001 (0.124)
919.1
0.215 (0.087)
0.274
-0.017
4,3
0.021 (0.034)
851.8
-0.023 (0.012)
-0.029
-0.045
DL-aspartic (amino) acid
HOOCCH2CH-(NH2)COOH
4,3
999.0
0.053 (0.021)
1071.8
0.021 (0.011)
-0.020
-0.070
(1R)-(+)-camphor
1,7,7-Trimethyl-[2.2.1]heptan-2-one
1,2
838.9
0.223 (0.036)
1044.9
-0.056 (0.016)
-0.214
-0.527
2,1
-0.040 (0.070)
0.109 (0.033)
0.489
-0.352
(1S)-(-)-camphor
C10H16O
4,3
935.5
0.019 (0.005)
1042.8
0.004 (0.010)
-0.003
-0.070
D-fructose (fruit sugar)
C6H12O6
1,2
861.3
0.471 (0.096)
977.5
-0.113 (0.096)
-1.683
-0.001
1,2
0.471 (0.096)
1082.3
0.145 (0.055)
-0.554
-0.248
1,3
-0.070 (0.017)
-0.003 (0.028)
0.043
-0.005
1,4
0.033 (0.016)
-0.008 (0.014)
-0.022
-0.045
2,1
0.014 (0.164)
0.647 (0.124)
2.949
-0.038
D-glucose (blood sugar)
C6H12O6
2,4
932.0
0.112 (0.016)
838.9
0.087 (0.033)
-0.023
-0.020
L-histidine (amino acid)
Glyoxaline-5-alanine
1,2
1025.6
0.132 (0.075)
977.5
-0.001 (0.037)
-0.273
-0.069
2,1
0.269 (0.175)
-0.082 (0.077)
-1.757
-0.104
3,4
-0.087 (0.053)
968.1
0.033 (0.025)
0.194
-0.022
3,4
-0.087 (0.053)
923.4
0.021 (0.022)
0.169
-0.054
2,1
0.269 (0.175)
838.9
-0.023 (0.191)
-1.991
-0.054
2,3
0.015 (0.022)
-0.024 (0.015)
-0.033
-0.002
D-mannose (α-form sugar)
C6H12O6
1,2
899.3
0.333 (0.133)
1040.0
-0.016 (0.034)
-0.852
-0.015
2,3
0.009 (0.018)
969.9
-0.035 (0.009)
-0.021
-0.025
L-serine (amino acid)
HOCH2CH--(NH2)COOH
1,2
945.2
0.319 (0.147)
1012.1
0.092 (0.072)
-0.782
-0.064
2,3
0.011 (0.029)
-0.025 (0.005)
-0.031
-0.037
4,3
0.091 (0.037)
0.014 (0.003)
-0.055
-0.077
4,3
0.091 (0.037)
1039.5
-0.017 (0.025)
-0.102
-0.053
L-sorbose (open ring sugar)
C6H12O6
1,3
849.6
0.000 (0.008)
829.9
0.026 (0.004)
0.003
-0.017
3,2
-0.023 (0.004)
-0.006 (0.004)
0.002
-0.001
4,2
0.006 (0.006)
0.018 (0.006)
0.001
-0.057
4,3
0.010 (0.004)
0.021 (0.004)
0.001
-0.057
2,4
0.013 (0.008)
992.1
-0.033 (0.033)
-0.051
-0.034
4,2
0.006 (0.006)
0.052 (0.021)
0.019
-0.080
1,3
0.000 (0.008)
1048.2
0.204 (0.034)
0.168
-0.048
2,1
-0.147 (0.049)
0.114 (0.167)
0.549
-0.237
3,4
0.004 (0.008)
-0.074 (0.033)
-0.077
-0.002
DL-tartaric acid (racemic acid)
2-dihydroxy- butanedioic acid
2,4
-0.081 (0.059)
887.3
0.036 (0.027)
0.211 (0.112)
-0.075
4,2
0.075 (0.042)
0.007 (0.019)
-0.068 (0.053)
-0.019
L-tartaric acid (fruit acid)
[R-(R*, R*)]-2,3- dihydroxy- butanedioic acid
1,3
1029.9
0.058 (0.015)
1082.3
0.188 (0.030)
0.105 (0.029)
-0.001
2,1
0.208 (0.126)
0.704 (0.154)
1.587 (1.081)
-0.089
3,1
0.120 (0.056)
-0.310 (0.092)
-1.101 (0.270)
-0.074
3,4
-0.039 (0.014)
0.131 (0.020)
0.099 (0.015)
-0.031
4,3
-0.038 (0.007)
0.011 (0.013)
0.003 (0.005)
-0.060
D-tartaric acid (levorotatory/ dextro config.)
[S-(R*, R*)]-2,3-dihydroxy-butanedioic acid
1,3
1029.9
0.081 (0.035)
1082.3
0.396 (0.085)
0.552 (0.222)
-0.080
4,3
0.002 (0.014)
0.062 (0.030)
0.011 (0.032)
-0.198
L-tryptophan (amino acid)
2-amino-3- propionic acid
4,3
833.3
0.036 (0.020)
1005.0
-0.006 (0.011)
-0.020 (0.013)
-0.028
L-tyrosine (amino acid)
β-(p-hydroxy- phenyl) alanine
3,4
925.1
0.117 (0.063)
878.7
0.003 (0.020)
-0.190 (0.112)
-0.048
1,2
0.299 (0.148)
1095.3
-0.007 (0.098)
-1.210 (0.838)
-0.074
4,3
-0.041 (0.023)
0.049 (0.024)
0.076 (0.029)
-0.073
The scaled difference
(ΔMi,js) and negative
correlation coefficients of elements are major features for pattern
recognition and detection of the organic. λ0 and
λr are beam wavelengths on resonance and off
resonance of molecular absorption, respectively; α is the scattering
beam orientation; and α = 90° is the normal beam incidence.