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**Correlation techniques for the improvement of signal-to-noise
**

ratio in measurements with stochastic processes

V. Raghavendra Reddy

a,

*, Ajay Gupta

b

, T. Goverdhan Reddy

a

,

P. Yadagiri Reddy

a

, K. Rama Reddy

a

a

Department of Physics, College of Science, Osmania University, Hyderabad 500 007, India

b

Inter University Consortium for DAE Facilities, Khandwa Road, Indore 452 017, India

Received 6 March 2002; received in revised form 7 January 2003; accepted 24 January 2003

Abstract

An AC modulation technique is described to convert stochastic signal variations into an amplitude variation and its

retrieval through Fourier analysis. It is shown that this AC detection of signals of stochastic processes when processed

through auto- and cross-correlation techniques improve the signal-to-noise ratio; the correlation techniques serve a

similar purpose of frequency and phase ﬁltering as that of phase-sensitive detection. A few model calculations applied to

nuclear spectroscopy measurements such as Angular Correlations, Mossbauer spectroscopy and Pulse Height Analysis

reveal considerable improvement in the sensitivity of signal detection. Experimental implementation of the technique is

presented in terms of amplitude variations of harmonics representing the derivatives of normal spectra. Improved

detection sensitivity to spectral variations is shown to be signiﬁcant. These correlation techniques are general and can be

made applicable to all the ﬁelds of particle counting where measurements are amenable to ‘‘dual modulation’’. The

proposed AC modulation technique may be applied in diverse ﬁelds like pulse height analysis in nuclear spectroscopy,

XRD, XRF, RBS, ESCA, positronium resonance, photon counting etc., for enhancing the S=N ratio.

r 2003 Elsevier Science B.V. All rights reserved.

PACS: 76.80

Keywords: Stochastic processes; Correlation functions; Angular correlations; Mossbauer spectroscopy; Dual modulation; Spectral

density and detection sensitivity

1. Introduction

In experiments dealing with particle counting,

measurements are carried out through recording

the count rates as a function of physical para-

meters like angle or energy or external ﬁeld

variations, etc. In the past, specialised techniques

suitable to each ﬁeld of spectroscopy were devel-

oped for improving the detection sensitivity

through the enhancement of S=N ratio. For

example, in angular correlation measurements

involving successive emission of gamma rays, the

accidental coincidence rate which is proportional

to the product of count rates in each of the

detectors coincidence along with the resolving time

is a decisive factor in determining the true

*Corresponding author. Tel.: +91-40-701-8951; fax: +91-

40-701-9020.

E-mail address: varimalla@yahoo.com (V.R. Reddy).

0168-9002/03/$ - see front matter r 2003 Elsevier Science B.V. All rights reserved.

doi:10.1016/S0168-9002(03)00422-4

coincidence rate forming the signal [1,2]. Similarly,

in Mossbauer spectroscopy, the non-resonant

radiation forms an unavoidable background,

which limits the detection sensitivity in observing

the resonance absorption, in a large number of

cases. Techniques like resonance detectors, ava-

lanche counters and conversion electron spectro-

scopy as well as special conﬁgurations of scattering

geometry, etc. have been developed for the

improvement of detection sensitivity in Mossbauer

spectroscopy [3,4]. In all the cases ‘‘background’’

radiation limits the precision to be achieved in

estimating physical parameters as the existing

methods use the DC method of relative variation

of the count rate as a function of the angle or

energy, etc. It is to be noted that the AC

modulation method of detecting analog signals in

the frequency domain before its use in physical

sciences was gainfully employed in radio commu-

nication for its higher sensitivity over the DC

detection method [5]. This technique known as

coherent or phase-sensitive detection is now widely

used in several areas with higher detection

sensitivity [6]. It was shown that improvement in

the estimation of relative power change

DP=PE10

À10

could be achieved in several areas

of measurements which is almost impossible in DC

methods of measurements [7]. However, the DC

detection reproduces line shapes that are almost

free of distortions but the signal detection sensi-

tivity is very poor due to the presence of inherent

unavoidable noise which generally spreads over a

large frequency bandwidth. A very narrow noise

bandwidth can be made possible by converting

signal variations into amplitude variations by

modulation at ﬁxed frequency f

m

: The AC signal

measurement at the modulation frequency ﬁlters

the noise to a great extent and improves the S=N

ratio, resulting in improved sensitivity. Extensive

theoretical studies on the effect of AC modulation

on Lorentzian (or Gaussian) shaped lines in

Electron Spin Resonance (ESR) spectroscopy

[8,9] showed that the coherent detection output

(a) at the ﬁrst harmonic frequency f

m

is an AC

signal with its amplitude proportional to the

differential of the original Lorentzian line and (b)

at the second harmonic frequency 2f

m

is an AC

signal with its amplitude proportional to the

second differential of the original Lorentzian line,

etc. These aspects of highest sensitivity of detec-

tion as well as the modulation line broadening and

line sharpening techniques are being exploited to

the fullest extent in ESR spectroscopy [10].

A few theoretical studies were made for achiev-

ing the improvement of S=N ratio in stochastic

processes also [11–13]. The approach in these cases

involved converting count rate of the stochastic

process into analog signal with the hope of

implementing analog phase lock technique

through dual modulation. But, various experi-

mental limitations of analog phase-sensitive detec-

tion method as applied to stochastic processes

could not be made functional for making it a

viable technique [14].

Having gone through unsuccessful attempts

with frequency domain analog technique of

phase-sensitive detection, we have undertaken an

approach of digital signal processing techniques

involving the concepts of correlations applied to

stochastic processes as the nuclear spectroscopy

originates inherently from stochastic processes. It

is shown that the correlation techniques are

equivalent to phase-sensitive frequency ﬁltering

and it is the best means of retrieving the signal

masked by noise. In Section 2 the equivalence

between correlation analysis and frequency and

phase ﬁltering will be established to gain con-

ﬁdence in applying correlation methods as a means

for ﬁltering the noise. Section 3 contains model

calculations for the purpose of analytic investiga-

tion of various aspects related to S=N improve-

ment. Experimental realisations along with results

are presented in Sections 4 and 5 contain conclu-

sions and implications of the technique in particle/

photon spectroscopy.

2. Correlation and ﬁltering

Consider a measurement function f ðtÞ deﬁned as

a linear sum of the signal sðtÞ and the random

noise nðtÞ expressed as f ðtÞ ¼ sðtÞ þ nðtÞ; where the

extraction of a periodic signal sðtÞ buried in the

function f ðtÞ is to be carried out. Let us assume

that a reference function cðtÞ of the same frequency

as that of the signal to be detected is available. The

V.R. Reddy et al. / Nuclear Instruments and Methods in Physics Research A 501 (2003) 559–575 560

cross-correlation of measurement function f ðtÞ

with the reference signal cðtÞ; by deﬁnition is given

by [15].

j

fc

ðtÞ ¼ Lim

T-N

1

T

_

þT=2

ÀT=2

½sðtÞ þ nðtÞcðt ÀtÞ dt

¼ Lim

T-N

1

T

_

þT=2

ÀT=2

½sðtÞcðt À tÞ dt

þ Lim

T-N

1

T

_

þT=2

ÀT=2

½nðtÞcðt À tÞ dt ð1Þ

¼ u

sc

ðtÞ þu

nc

ðtÞ ð2Þ

where j

12

ðtÞ deﬁnes the correlation between any

two functions. As the reference function cðtÞ is

periodic by choice and uncorrelated with the

random noise nðtÞ; therefore, the correlation of

the noise with a periodic reference function is zero.

Hence,

j

fc

ðtÞEj

sc

ðtÞ as j

nc

ðtÞE0 for large t:

Since the signal sðtÞ is periodic and similar to that

of reference function cðtÞ; therefore, it follows that

the cross-correlation, f

fc

ðtÞ; of the measured

function f ðtÞ with the reference function cðtÞ is

not only a periodic function with periodicity of the

reference function in the time domain but also

deﬁnes the signal amplitude variation rich in signal

content.

Similarly, when the reference signal is not

available even then the noise ﬁltering can be

achieved through the deﬁnition of auto-correlation

function of f ðtÞ as

j

ff

ðtÞ ¼ Lim

T-N

1

T

_

þT=2

ÀT=2

f ðtÞf ðt ÀtÞ dt

¼ Lim

T-N

1

T

_

þT=2

ÀT=2

½sðtÞ þ nðtÞ

Â ½ðsðt ÀtÞ þ nðt À tÞdt ð3Þ

¼ j

ss

ðtÞ þj

sn

ðtÞ þ j

ns

ðtÞ þ j

nn

ðtÞ: ð4Þ

As the signal sðtÞ and the noise nðtÞ are

uncorrelated, we ﬁnd that the cross-correlation

of noise and the signal tends to zero, i.e.,

j

ns

ðtÞ ¼ j

sn

ðtÞ ¼ 0 for t large

and

j

nn

ðtÞ-0 for T-N: ð5Þ

Therefore, it follows that the auto-correlation

function, j

ff

ðtÞ; preserves periodicity of the signal

representing the characteristics of the original

signal function. From the Weiner-Khinchin [16]

theorem it follows that

j

ff

ðtÞ3F

ff

ðoÞ

¸

¸

¸

¸

2

¼ pS

ss

ðoÞ þ pS

nn

ðoÞ

where S

ss

ðoÞ and S

nn

ðoÞ are signal and noise

spectral densities evaluated over a ﬁnite interval of

time.

To establish the relationship between correla-

tion and ﬁltering, consider two functions f

1

ðtÞ and

f

2

ðtÞ: Deﬁning the Fourier transform of f

1

ðtÞ as

f

1

ðtÞ3F

1

ðoÞ and that of f

2

ðtÞ as f

2

ðtÞ3F

2

ðoÞ; it is

easy to show that f

2

ðÀtÞ3F

2

ðÀoÞ:

The convolution function r

12

of f

1

ðtÞ and f

2

ðÀtÞ;

by deﬁnition, is given by [15]

r

12

ðtÞ ¼ f

1

ðtÞ#f

2

ðÀtÞ

¼ Lim

T-N

1

T

_

þT=2

ÀT=2

f

1

ðtÞf

2

ðÀðt À tÞÞ dt

¼ Lim

T-N

1

T

_

þT=2

ÀT=2

f

1

ðtÞf

2

ðt ÀtÞ dt ð6Þ

and its Fourier transform is given by

r

12

ðtÞ3F

1

ðoÞF

2

ðÀoÞ:

The cross-correlation of f

1

ðtÞ and f

2

ðtÞ; following

Eq. (1) is given by

j

12

ðtÞ ¼ Lim

T-N

1

T

_

þT=2

ÀT=2

f

1

ðtÞf

2

ðt À tÞ dt

3F

1

ðoÞF

2

ðÀoÞ: ð7Þ

From the results of Eqs. (6) and (7) it is seen

that the operation of cross-correlation on func-

tions e

1

ðtÞand e

2

ðtÞ is equivalent to the convolu-

tion of e

1

ðtÞ and e

2

ðÀtÞ function and its Fourier

transform is the multiplication of F

1

ðoÞ and

F

2

ðÀoÞ: Thus, the cross-correlation function

j

12

ðtÞ in the t-domain can be visualised as shown

in Fig. 1. Alternately, the signal F

1

ðoÞ applied to a

system with transfer function F

2

ðÀoÞ gives its

V.R. Reddy et al. / Nuclear Instruments and Methods in Physics Research A 501 (2003) 559–575 561

output as F

1

ðoÞF

2

ðÀoÞ: It is seen that the cross-

correlation between f

1

ðtÞ and f

2

ðtÞ may be affected

by applying the signal f

1

ðtÞ to the input terminals

of a linear system with transfer function F

2

ðÀoÞ as

shown in Fig. 2. When the f

2

ðtÞ represents a

monochromatic reference signal cðtÞ given by [17]

cðtÞ ¼ c

0

e

io

0

t

32pC

0

dðo À o

0

Þ ð8Þ

then this operation essentially represents ﬁltering

with a transfer function CðÀoÞ ¼ CðoÞ represent-

ing the system with output as

FðoÞ ¼ 2pF

1

ðo

0

ÞC

0

dðo À o

0

Þ ð9Þ

which attenuates all the frequency amplitudes

except the one at o ¼ o

0

: The output signal in

the time domain, therefore, consists of a signal

amplitude F

1

ðo

0

Þ with frequency o ¼ o

0

: It is

evident that the operation of cross-correlation in

the time domain is equivalent to frequency ﬁltering

in the frequency domain. Therefore, the process of

cross-correlation may be construed as ﬁltering the

noise in the entire region of frequency except at the

signal frequency of o ¼ o

0

:

Finite measuring time effects can be evaluated

by taking time average over a portion (ÀT=2; T=2)

of a random process. When the measuring time

interval T is ﬁnite, the reference function cðÀtÞ ¼

cos o

0

t can be expressed as a gate function

multiplied by cos o

0

t and shifted by ÀT=2

(Fig. 3(i)). From Fourier analysis it follows (mod-

ulation theorem) that the windowed function

becomes a sampling function cðoÞ shifted by

7o

0

(Fig. 3(ii)), i.e.,

j

fc

ðtÞ ¼

1

T

_

T=2

ÀT=2

f ðtÞcðt ÀtÞ dt

32pFðoÞ

sin ðoT=2Þ

oT

: ð10Þ

The cross-correlation of eðtÞ with cðtÞ over a

ﬁnite interval (ÀT; 0) is thus equivalent to ﬁltering

in the vicinity of 7o

0

and attenuating the

remaining frequencies with a bandwidth equal to

1=T as per the ﬁltering by the ‘‘sinc’’ function.

As an example consider Poisson stochastic

process like the process involved in nuclear

radiation emission/absorption measurements. The

auto-correlation function for the Poisson stochas-

tic process of unit impulses deﬁning the noise

function nðtÞ with mean count rate of l is given by

[16]

j

nn

ðtÞ ¼ l

2

þldðtÞ: ð11Þ

Thus, the spectral density S

nn

ðoÞ is given by

j

nn

ðtÞ3SðoÞ ¼

2pA

2

l

2

a

2

dðoÞ þ

Al

a

2

þ o

2

ð12Þ

where A is a constant representing pulse height

and a the pulse decay constant deﬁning the

detector response function [16]. It may be noted

that the ﬁrst term of Eq. (12) represents a large

magnitude at o ¼ 0 proportional to the square of

the count rate and the second term with much

smaller in magnitude varies slowly with frequency

for o > 0: Since a pulse decay rate aE10

6

–10

7

/s,

the frequency dependence of the spectral density

CROSS-CORRELATOR

f

1

(t)

f

2

(t)

ϕ

12

(τ)

Fig. 1. Time domain ﬁlter.

f

2

(-t)

F

2

(-ω)

f

1

(t)

F

1

(ω)

ρ

12

( )

F

1

(ω)F

2

(-ω)

τ

Fig. 2. Frequency domain ﬁlter.

Fig. 3. (a) The reference signal cðÀtÞ multiplied by gate

function and (b) sampling function.

V.R. Reddy et al. / Nuclear Instruments and Methods in Physics Research A 501 (2003) 559–575 562

SðoÞ at low frequencies even up to 10

6

Hz, is

meagre and almost frequency independent.

For the purpose of understanding the ﬁltering

action of the correlation process, Poisson impulses

generated by nuclear detector system was recorded

as a sequence XðnÞ in the Multi Channel Scaling

(MCS) mode. A sequence YðnÞ is deﬁned as a sum

of the noise XðnÞ and an harmonic signal of

amplitude ‘‘a’’ as

YðnÞ¼ Noise þ Signal ¼XðnÞ þ a cosð2pn D

*

8Þ

and the YðnÞ is displayed for the ﬁrst half as the

sequence with amplitude a ¼ 50 (see Fig. 4(i)). The

spectral density of the sequence YðnÞ obtained

through the use of FFT algorithm is shown in

Fig. 4(ii), where the S=NE1: Further, the auto-

correlation j

yy

ðf Þ of the sequence YðnÞ was

obtained as [18]

u

yy

ðjÞ ¼

2

N

N=2

i¼1

YðiÞYði þ j À 1Þ

for j ¼ 1; 2; 3yN=2 with N ¼ 800 ð13Þ

and the FFT of the auto-correlation function

representing the spectral density is shown in

Fig. 4(iii) to illustrate that the auto-correlation

process is capable of ﬁltering the noise except in

the region of signal frequency probably with a

window width of 1=T: This example is an

illustration of the fact that the noise spectral

density is almost zero at all frequencies except

around the signal frequency, which is also small.

From the foregoing results it is seen that one

may also expand the cross-correlation sequence

j

yc

ðtÞ as a discrete Fourier series in terms of the

fundamental and its harmonics of the reference

signal cðtÞ and in which case it is easy to realise

that the evaluation of discrete Fourier series

coefﬁcients is equivalent to perfect ‘‘frequency

and phase’’ ﬁltering. Thus, the correlation techni-

ques along with Fourier analysis as applied to

stochastic processes of signals buried in noise also

improve the S=N ratio.

To determine the amplitude of the sinusoid

buried in Poisson noise, correlation techniques

0 50 100 150 200 250 300 350 400

0 50 100 150 200 250 300 350 400

0 50 100 150 200 250 300 350 400

2300

2400

2500

2600

2700

time (channels)

c

o

u

n

t

s

(i)

0

0.5

1

0

0.5

1

1.5

x 10

-4

frequency (w)

frequency (w)

n

o

r

m

a

l

i

z

e

d

S

(

w

)

n

o

r

m

a

l

i

z

e

d

S

(

w

)

(ii)

(iii)

Fig. 4. (i) Harmonic signal corrupted with noise at S=NE1; (ii) spectral density of the function f ðtÞ=Noise+Signal; (iii) spectral

density obtained through auro-correlation of the function f :

V.R. Reddy et al. / Nuclear Instruments and Methods in Physics Research A 501 (2003) 559–575 563

were used for noise ﬁltering and the FFT for the

determination of the signal amplitude. Results are

summarised in Table 1 for illustrating the ampli-

tude variation with data length and the method

used for the amplitude retrieval.

Having illustrated the basic principle of noise

reduction technique, a few examples of nuclear

spectroscopy such as Mossbauer resonance, per-

turbed angular correlations, angular distribution

of radiation and pulse height analysis are con-

sidered in detail through the ‘‘dual modulation’’ of

the process and by applying correlation and

Fourier techniques for data reduction resulting in

the enhanced S=N ratio.

3. Enhancement of detection sensitivity-simulation

studies

In almost all the experiments involving particle

counting, signal estimations are made through DC

detection by count rate measurement. In such

measurements there is no way of isolating the

background which is also a Poisson stochastic like

the signal statistic. However, modulation of the

signal even if it is a stochastic process, at a

frequency e

m

allows experiments to be carried out

against unmodulated background. In the preced-

ing discussion it was shown that the stochastic

processes are amenable to digital signal processing

involving auto- and cross-correlation techniques.

Therefore, use of digital signal processing methods

can be used to enhance the signal detection

sensitivity, as the correlation techniques in the

digital domain are similar to coherent detection

methods in the analog domain. In the following,

the interesting aspects of foregoing analysis are

applied to a few ﬁelds of nuclear spectroscopy for

illustrating the utility of the proposed technique.

3.1. Mossbauer resonance

In Mossbauer resonance the transmitted gamma

ray intensity through a resonance absorber reach-

ing the detector can be made to depend on dual

Doppler modulation such as ‘‘fast’’ AC velocity

modulation over a slowly varying linear velocity

modulation of the source [14]. Correlation analysis

of the transmitted gamma ray ﬂux at each velocity

setting would give characteristic amplitude modu-

lated transmission whose amplitude depends upon

slope of the normal absorber characteristic func-

tion. But, the non-resonant radiation has no such

dependence and contributes very little to the AC

signal amplitude.

For the purpose of analysis through simulation

studies, let us consider the resonance absorption

for Mossbauer gamma rays as a function of

incident gamma energy expressed as [19]

IðEÞ ¼ 1 À

ðg=2Þ

2

ðg=2Þ

2

þ ðE À E

0

Þ

2

_ _

N

0

þ N

B

ðBackground countsÞ ð14Þ

where N

0

¼ s

0

f

t

N

t

and f

t

¼ f

source

Â f

absorber

is the

total recoil-free fraction for the resonant absorp-

tion with

E ¼ E

0

þ E

D

¼ E

0

þ E

0

þ E

0

v

c

where v ¼ v

0

t

t

0

À

1

2

_ _

with t

0

XtX0:

For the purpose of noise ﬁltering through

correlation analysis, an additional Doppler mod-

ulation at well-deﬁned frequency f

m

such as

v

m

sin 2pe

m

t can be introduced for the velocity

modulation termed as AC modulation. This

additional AC modulation transforms the reso-

nance absorption intensity Iðv; v

m

Þ into a compli-

cated function represented as

Iðv; v

m

Þ ¼

N

0

ðv þ v

m

sin 2pf

m

tÞ

2

=ðg=2Þ

2

1 þ ½ðv þ v

m

sin 2pf

m

tÞ

2

=ðg=2Þ

2

þ N

B

Table 1

Retrieval of harmonic amplitude buried in noise

a

Method used Amplitude with

N ¼ 400 data

points (for 20

trials)

Amplitude with

N ¼ 800 data

points (for 20

trials)

Fourier 50.971.6 50.371.3

Auto correlation 51.471.7 50.371.4

Cross correlation 50.571.6 50.271.2

a

Assumed input amplitude of 50 units at S=NE1

V.R. Reddy et al. / Nuclear Instruments and Methods in Physics Research A 501 (2003) 559–575 564

with v

m

being the velocity amplitude of the

‘‘harmonic modulation’’ under the condition that

the linear scan frequency, 1=t

0

; is much lower than

the modulation frequency [14], i.e., 1=t

0

5f

m

and

the full width at half maximum is expressed in

terms of Doppler velocity.

The absorption intensity Iðv; v

m

Þ can be Fourier

analysed and this process is equivalent to the

process of cross-correlation analysis. Hence, the

Fourier series analysis of the absorption intensity

can be represented as

IðvÞ ¼I

0

½a

0

þ

N

n¼1

fa

n

ðg; v; v

m

Þsin n2pf

m

t

þ b

n

ðg; v; v

m

Þcos n2pf

m

tg ð15Þ

where I

0

is the effective absorption for resonant

gamma rays with a

n

and b

n

as Fourier amplitudes

and the amplitude a

1

would sample the ﬁrst

derivative of the absorption function, a

2

its second

derivative, etc., while I

0

a

0

still represents the

normal absorption.

The simulation of Mossbauer spectra with 256

normal data points are obtained with the help of

analytic Lorentzian curve and the Poisson number

generator algorithm for an assumed mean count

rate N

0

(resonance) and N

B

(background). The

harmonic AC velocity modulation is introduced to

be ‘‘v

m

sin 2pf

m

t’’. The MATLAB function

poissrnd(lambda) is used for generating the

Poisson process [18] for N

0

ðjÞ and N

B

ðjÞ with an

assumed values for mean N

0

and N

B

mean for j ¼

1; 2; y; 256: To be speciﬁc, each velocity (or

channel) in the normal method of absorption

experiments is divided into 1024 data points and a

8 Hz sine wave is used for AC modulation with 8

cycles as a data length which gives a phase

resolution of 360 Â8/1024=2.8

.

For the purpose of correlation studies the

simulated normal Mossbauer spectral data point

generated at count rate of N

0

ðjÞ gets divided by

1024 to form mean count rate n

0

¼ N

t

ðjÞ=1024 for

the generation of 1024 Poisson distributed random

counts nðjÞ: The 1024 random data points obtained

by taking, for example, n

B

¼ N

B

ðjÞ=1024 and

generating 1024 data set of n

B

ðiÞ through random

number generator for deﬁning the function f

i

ðjÞ

with i varying from 1 to 1024 forms data set at a

jth velocity which is given by

f

i

ðjÞ ¼

n

0

ðiÞ v

0

j

256

À

1

2

_ _

þ v

m

sin 2pf

m

iD

_ _

2

=ðg=2Þ

2

1 þ ð2=gÞ

2

v

0

j

256

À

1

2

_ _

þ v

m

sin 2pf

m

iD

_ _

2

þ n

B

ðiÞ: ð16Þ

The Fourier amplitudes a

0

and a

1

at jth velocity

are evaluated as

a

0

ðjÞ ¼

1

1024

1024

i¼1

f

i

ðjÞ

and

a

1

ðjÞ ¼

2

1024

½

1024

i¼1

f

i

ðjÞsin ð2pf

m

iDÞ: ð17Þ

Fig. 5 shows a particular result of the calcula-

tions on the Mossbauer line to illustrate the noise

ﬁltering power of the proposed AC detection

method along with DC signal I

0

a

0

ðjÞ: The differ-

ential amplitude a

i

ðjÞ is not properly normalised as

the step width calibration is not taken into account

and the results presented are relative values only.

The same procedure was adopted in all the

following calculations as the step-width calibration

is different for different physical modulation

parameters depending on the type of application

such as Mossbauer resonance, perturbed angular

correlation, etc. The linear slope seen in Fig. 5(iv)

is an artefact introduced due to computational

error while taking initial value for a

i

: The linear

slope is found to be varying with the nature of

input data and it is being corrected while estimat-

ing Mossbauer parameters through least-squared

analysis (shown in Fig. 10).

The calculations are carried out for different

noise levels, relative absorption, modulation

depths and frequencies. The results of modulation

depth variations conﬁrm the line shape broadening

with the increase of depth of modulation [7]. The

modulation depth of v

m

¼ 2g

nat

units is found to

be an optimal value for highest sensitivity of

detection. The 8 cycles of harmonic modulation at

any velocity ‘‘vðjÞ’’ could be optimised for the

calculation, even though 4 cycles were found to be

sufﬁcient to retrieve the signal shape.

V.R. Reddy et al. / Nuclear Instruments and Methods in Physics Research A 501 (2003) 559–575 565

All the Mossbauer experimental parameters

like line width, line position and f -factor (or the

area under the resonance absorption curve) can be

derived from the differential absorption data.

It is seen that the line position can be derived

from the zero crossing of the differential

absorption data. To evaluate the f -factor and

the line width when the depth of modulation v

m

which perturbs the resonance absorption, one

needs a detailed theoretical analysis and it can be

shown that for lorentzian line shapes, the max-

imum (or minimum) value of the differential

amplitude a

1

for a given modulation depth v

m

is

given by [7]

a

1

¼

72ð1=bÞ

2

ðv

m

=bÞ

f3ðv

m

=bÞ

2

þ 8 þ ½ðv

m

=bÞ

2

þ 4

3=2

g

1=2

ð18Þ

where the b is the natural line width related to

FWHM as g ¼ O3b: Further, the relation between

the natural line width b and the observed line

width b(obs) is given by [7]

bðobsÞ ¼ b

v

m

b

_ _

2

þ5 À 2 4 þ

v

m

b

_ _

2

_ _

1=2

_

_

_

_

_

_

1=2

: ð19Þ

The above two relations may be used for the

evaluation of the depth of modulation and the

natural line width b: If the line width b is known

then any one of the above equations can be used

for estimating the modulation depth. This result

would enable the velocity transducer calibration

from known input AC voltage amplitude used as a

reference signal for the velocity control servo

system.

From Eqs. (18) and (19) it is seen that the

observed peak separation depends upon the depth

of modulation and the line gets broadened by the

AC modulation. It can be shown that the

amplitude a

1

increases linearly with the depth of

modulation v

m

for v

m

ob and, therefore, the area

50 100 150 200 250

7500

8000

8500

9000

9500

channel (velocity) channel (velocity)

c

o

u

n

t

s

p

e

r

u

n

i

t

t

i

m

e

c

o

u

n

t

s

p

e

r

u

n

i

t

t

i

m

e (i)

50 100 150 200 250

50 100 150 200 250

channel (velocity) channel (velocity)

50 100 150 200 250

-400

-200

0

200

400

600

(ii)

-15

-10

-5

0

5

r

e

l

.

a

b

s

o

r

p

t

i

o

n

(

a

r

b

.

u

n

i

t

s

)

(iv)

-0.5

0

0.5

1

r

e

l

.

a

m

p

l

i

t

u

d

e

(iii)

Fig. 5. Simulated Mossbauer spectra for the normal and dual modulation: (i) computer simulated Mossbauer absorption spectrum; (ii)

derivative spectrum of the data given in (i); (iii) the ﬁrst harmonic amplitude spectrum following the cross-correlation technique, (iv)

integral of ﬁrst harmonic amplitude spectrum obtained from the data of (iii).

V.R. Reddy et al. / Nuclear Instruments and Methods in Physics Research A 501 (2003) 559–575 566

evaluated on the basis of differential method

becomes a function of the modulation depth v

m

:

In the preceding section, it was shown that the

Fourier amplitude I

0

a

0

reproduces the Mossbauer

absorption spectrum and its area A

0

for equal

sampling interval [nðjÞ À nðj À 1Þ] of the velocity is

given by

A

0

¼ ½v

j

ðiÞ À vðj À 1Þ

m

j¼1

a

0

ðjÞ: ð20Þ

The area obtained through I

0

a

0

ðjÞ data is weakly

dependent of v

m

; and hence A

0

can be construed to

be independent of v

m

; the depth of modulation.

The double integration of the differential curve

also gives the area A

1

but this result is strongly

dependent on the depth of modulation. For a

given v

m

; the area A

1

is given by

A

1

¼ ½vðjÞ À vðj À 1Þ

2

m

j¼1

ja

1

ðjÞ ð21Þ

and the proportionality factor C where A

0

¼ CA

1

gives the calibration factor for the evaluation of

the f -factor.

Based on the above analysis, it is thus seen that

there is no ambiguity in evaluating all the

Mossbauer parameters including the modulation

depth from the differential measurement through

AC modulation technique. In fact the line posi-

tions correspond to zero crossing which are

independent of the modulation depth.

3.2. Directional correlations

Measurements of nuclear g2g; a2g and b2g

angular correlations involve the true coincidence

counting rates of particles in the presence of

chance coincidence rates. The true and chance

coincidence rates follow the same stochastic

process and there is no way of separating one

from the other in the conventional methods of DC

detection. However, the true coincidence count

rates are functions of physical variables like the

angle between particle detectors, extra nuclear

ﬁelds, etc., where as the chance coincidence count

rates are uniformly distributed at all angles and at

all times. The true coincidence rates get altered

when the correlation variable is modulated ex-

ternally at a ﬁxed frequency e

m

and the data

processing through cross- and auto-correlation

methods ﬁlters also effects of chance coincidence

rates and offer the methods of retrieving the

harmonic amplitude representing the differential

of the original correlation function and its spectral

density, respectively. This AC method of signal

detection has the power of enhancing the S=N

ratio.

3.2.1. Determination of nuclear g-factor of the

excited state

A general expression for the angular correlation

function in the presence of interaction for nuclear

decay by gamma rays and the extra nuclear static

perturbations due to magnetic ﬁelds, etc., acting

on the intermediate state is given by [20]

Wðy; t; BÞ ¼

A

k

ð1ÞA

k

ð2ÞG

kk

ðtÞP

k

ðcos yÞ ð22Þ

where W is the angular correlation function, A

k

ð1Þ

and A

k

ð2Þ are the correlation coefﬁcients and

G

kk

ðtÞ the usual attenuation function. The angular

correlation function becomes particularly simple

when the radiation detectors are in the X2Y plane

and the magnetic ﬁled B is directed along the Z-

axis. The effects of this magnetic perturbation can

be worked out in detail and the ﬁnal expression

can be written as [21]

Wðy; t; BÞ ¼1 þ b

2

cos 2ðy À o

B

tÞ

þ b

4

cos 4ðy À o

B

tÞ: ð23Þ

A convenient geometry adopted for this correla-

tion measurement consists of constant delay

(t ¼ T) between the successive emission of gam-

ma-one and gamma-two, the constant angle y ¼

3p=4 and the variable magnetic ﬁeld. Eq. (23)

under the conditions deﬁned becomes

Wðy; T; BÞ ¼ 1 À b

2

sin 2o

B

T À b

4

cos 4o

B

T ð24Þ

where o

B

T ¼ Àm

N

gB=_ is the precession fre-

quency of the intermediate state nuclear magnetic

moment. The DC magnetic ﬁeld B for the purpose

of AC detection is assumed to vary slowly and

linearly as BðtÞ ¼ B

0

ðt=t

0

Þ where t

0

assumed to be

fairly large (of the order of minutes). A small

modulating AC ﬁeld B

m

sinð2pe

m

tÞ is superim-

posed on the ‘‘DC magnetic ﬁeld’’ as

B ¼ Bðt=t

0

Þ þ B

m

sin2pe

m

t under the constraint

V.R. Reddy et al. / Nuclear Instruments and Methods in Physics Research A 501 (2003) 559–575 567

of t

0

b1=e

m

and B

0

bB

m

: Under this condition of

dual modulation of the magnetic ﬁeld, the

correlation function deﬁned at Eq. (24) becomes

Wðy; t; BÞ ¼1 À b

2

sin ð2o

B

Tt=t

0

Þ þ 2o

B

T

B

m

B

0

sin 2pf

m

t

_ _

Àb

4

cos ð4o

B

Tt=t

0

Þ þ 4o

B

T

B

m

B

0

sin 2pf

m

t

_ _

:

The measured correlation function should con-

tain the effects of true and the chance coincidence

count rates. For the purpose of system identiﬁca-

tion we consider the measured correlation function

‘‘f ’’ to be

f ðBÞ ¼Wð3=4p; T; BÞN

0

ðtrue coincidence rateÞ

þ N

B

ðchance coincidence rateÞ ð25Þ

The data simulation and analysis is carried out

in the format speciﬁed in the preceding example.

The MATLAB function poissrnd(lambda) gener-

ates N

0

ðjÞ and N

B

ðjÞ for j ¼ 1; 2; y with an

assumed mean values as N

t

and N

B

: This process

of generating N

0

ðjÞ and N

B

ðjÞ gives the normal DC

detection in any measurement at each one of the

data points (normal).

For the purpose of AC detection we deﬁne n

s

¼

N

0

ðjÞ=800 and n

B

¼ N

B

ðjÞ=800 as mean values at

any given ﬁeld and random number generator

gives n

0

ðiÞ and n

B

ðiÞ for i varying from 1 to 800.

The AC detected signal amplitude at the jth

magnetic ﬁeld value is given by

f

i

ðjÞ ¼ 1 À b

2

sin yðj=100Þ þ y

B

m

B

0

sin 2pf

m

iD

_ _ _

Àb

4

cos 2yðj=100Þ þ 2y

B

m

B

0

sin 2pf

m

iD

_ __

Â n

0

ðiÞg þ n

B

ðiÞ ð26Þ

where y ¼ 2o

B

T in radians with B

0

¼ 1 T,

o

B

¼ 10:5 MHz, the delay T ¼ 3:75 Â 10

À5

s and

B

m

=B

0

¼ d

m

deﬁnes the modulation depth

The amplitudes f

i

form a data set of 800 data

points at each j of 100 values. The Fourier

amplitudes at the modulation frequency are

evaluated by projecting the f ðjÞf¼ f

1

ðjÞ; f

2

ðjÞyg

on to the modulation frequency using FFT

algorithm. The procedure used here is similar to

the one employed in the preceding example. The

AC signal amplitude a

1

; obtained for each setting

of the DC magnetic ﬁeld, forms the differential of

the original angular correlation function.

For the purpose of numerical evaluation, the

nuclear transition 0-2-0 of the g2g angular

correlation in Pd

106

with b

2

¼ 0:5 and b

4

¼ 0:5

and Eq. (26) has been used. The harmonic

amplitude a

1

at e

m

calculated from the cross-

correlation function f is plotted in Fig. 6. For the

purpose of comparison the results expected from

DC detection method are shown for the angular

correlation function and its derivative are shown

in the same ﬁgure. It is found that the depth of

modulation does not produce much distortion as

the angular correlation function contains harmo-

nic functions. Details on the extraction of g-values

can be worked out for any detailed planned

experiment.

3.2.2. Directional and polarisation correlation

The angular correlations of g2g; a2g and b2g

are measured in coincidence experiments for the

determination of multipolarity of gamma transi-

tions, momentum dependence of b-decay matrix

elements and orientation polarisation of nuclei,

etc. The variation of angle in the DC detection

method is limited to 0pypp; which can be

automated with a period of several minutes.

Repetition of this variation over 0pypp is

equivalent to time averaging for S=N enhance-

ment. The angular correlation function WðyÞ [22–

24] even in these cases still retains the same form as

given in the preceding section, i.e.,

WðyÞ ¼

A

k

ð1ÞA

k

ð2ÞP

k

ðcos yÞ:

To implement the AC detection, the angle y is

modulated as y ¼ y

0

ðt=t

0

Þ þ ðy

m

=2Þsinð2pe

m

tÞ;

0pypp; where y represents the angle between

the detectors and the harmonic variation of one of

the detectors with a few cycles per second can be

implemented in practice. Thus, the measurable

function of correlation can be written as

f ðy; y

m

; sin o

m

tÞ ¼Wðy; y

m

; sin 2

f

m

tÞ

Â N

0

ðtrue coincidence rateÞ

þ N

B

ðchance coincidence rateÞ

where WðyÞ ¼ 1 þ b

2

cos 2y þ b

4

cos 4y with b

2

¼

0:5 and b

4

¼ 0:5 for the 0-2-0 transition as

V.R. Reddy et al. / Nuclear Instruments and Methods in Physics Research A 501 (2003) 559–575 568

considered earlier. Therefore,

f

i

ðjÞ ¼½1 þ 0:5 cos fðxj=100Þ þ y sin 2pf

m

iDg

þ 0:5 cos f2xj=100Þ þ 2y sin 2pf

m

iDg

Â n

0

ðiÞ þ n

B

ðiÞ ð27Þ

where x ¼ 2y

0

and y ¼ xy

m

=ð2y

0

Þ

The data processing for cross- and auto-

correlation of the function f

i

ðjÞ; yields result with

the enhanced S=N: As per the procedure adopted

in the preceding examples, the Fourier analysis of

the cross-correlation function for the in-phase

component at the modulation frequency e

m

gives

the amplitude a

1

and these results are similar to

those given in Fig. 6 and hence the graphical

presentations are not given. In general the depth of

modulation d

m

¼ B

m

=B

0

or d

m

¼ y

m

=y

0

in these

cases does not seem to affect the shape of the

correlation function being measured. It is noted

that the correlation analysis of stochastic processes

through AC modulation technique improves the

sensitivity of detection even in the absence of

background chance coincidence rates.

3.3. Pulse height analysis

The conventional PHA spectrum was generated

by considering it to be the combination of

decreasing count rate, initially by terminating at

zero crossing of the horizontal scale and two

Gaussian lines centred at different channel num-

bers. The simulated spectrum was synthesised

using Poisson random number generator. The

normal pulse height spectrum was modelled to be

AC modulated and the resulting spectrum was

analysed for Fourier amplitudes a

0

and a

1

: The

simulation and the model calculations were very

0 50 100

1

1.05

1.1

1.15

1.2

1.25

x 10

4

magnetic field (arb.units)

0 50 100

magnetic field (arb.units)

c

o

u

n

t

r

a

t

e

(i)

-400

-200

0

200

400

r

e

l

.

c

o

u

n

t

r

a

t

e

r

e

l

.

c

o

u

n

t

r

a

t

e

r

e

l

.

c

o

u

n

t

r

a

t

e

(ii)

20 40 60 80 100

-10

0

10

20

magnetic field (arb.units)

20 40 60 80 100

magnetic field (arb.units)

(iv)

-2

-1

0

1

2

(iii)

Fig. 6. Simulated perturbed angular correlation pattern for the nuclear g-factor determination by constant delay, constant angle and

variable magnetic ﬁeld method: (i) computer simulated perturbed angular correlation function; (ii) derivative of the perturbed function

given in (i); (iii) the ﬁrst harmonic amplitude function following the cross-correlation technique; (iv) integral of the ﬁrst harmonic

amplitude spectrum obtained from data given in (iii).

V.R. Reddy et al. / Nuclear Instruments and Methods in Physics Research A 501 (2003) 559–575 569

similar to one discussed in the preceding Sections

3.1 and 3.2. The results are illustrated in Fig. 7.

4. Experimental realization—Mossbauer

spectroscopy as an example

4.1. Practical implementation of AC signal

detection

Encouraged by the results of model calculations,

an attempt has been made for observing the

Mossbauer resonance using AC dual modulation

by making the desired changes in the electronic

circuits of the conventional Mossbauer spectro-

meter. The dual Doppler velocity modulation of

gamma rays is achieved by imposing an additional

AC harmonic modulation at a well-deﬁned fre-

quency f

m

(80 Hz). The electronic circuit used for

achieving the harmonic modulation, shown in

Fig. 8, consists of a commercially available velo-

city drive system (Weissel drive of GDR make)

operated in the constant velocity mode with an

additional sinusoidal motion superimposed on it.

The square wave of 5 Hz is passed through a 10

turn potentiometer for changing the amplitude

from 0 to 72 V. The square wave is amplitude

modulated with 80 Hz sinusoid of 120 mV in

amplitude (modulation depth equal to g

nat

=4).

This amplitude could be adjustable for varying the

depth of modulation through a function generator.

The modulated signal serves the purpose of

reference signal for the velocity servo control

system. The velocity change is carried out manu-

ally by setting the potentiometer for affecting the

reference square wave amplitude. The potenti-

ometer setting was adjusted manually by a quarter

turn to achieve 41 amplitude settings and at each

setting positive and negative velocities are achieved

to avoid DC drifts, etc. Thus, 82 velocity data

points are recorded for the entire velocity scan.

The Co

57

source in Rh-matrix with stainless

steel absorber and proportional counter set up is

used for recording the spectra. It may be noted

that the constant velocity and the AC modulation

are always kept in-phase by deriving a trigger pulse

0 50 100

1400

1600

1800

2000

2200

2400

channels

0 50 100

channels

c

o

u

n

t

r

a

t

e

(i)

-200

-100

0

100

200

r

e

l

.

c

o

u

n

t

r

a

t

e

(ii)

20 40 60 80 100

-5

0

5

channels

20 40 60 80 100

channels

r

e

l

.

c

o

u

n

t

r

a

t

e

(iv)

-1.5

-1

-0.5

0

0.5

1

1.5

r

e

l

.

c

o

u

n

t

r

a

t

e

(iii)

Fig. 7. Simulated pulse height analysis of gamma ray spectra under normal and AC modulation methods of measurements: (i)

computer simulated PHA of gamma ray spectrum; (ii) derivative of the data given in (i); (iii) the harmonic amplitude function

following the cross-correlation technique; (iv) integral of the ﬁrst harmonic amplitude spectrum obtained from the data given in (iii).

V.R. Reddy et al. / Nuclear Instruments and Methods in Physics Research A 501 (2003) 559–575 570

generated at the start of square wave for the

initiation of MCS mode of operation of the data

recorder and details of deriving the square wave

are given in Fig. 8. The dwell time in each channel

of MCS mode is kept as 124 ms and the data points

collected at each velocity are about 1600 (800 for

the positive and 800 for negative velocity) forming

the time spectrum at each ‘‘velocity’’ setting by

counting of photons in the MCS mode of

operation at each of the pre-assigned velocity

setting. This has resulted in 100 data points in each

cycle of AC modulation, deﬁning a phase resolu-

tion of 3.6

**. Fig. 9 illustrates clearly the effect of
**

normal Mossbauer absorption at a set velocity

being driven with a modulation frequency f

m

: The

initial 100 data points of each positive and

negative velocity cycles of the square wave at any

set amplitude are not considered for the calcula-

tions to overcome the errors of settling down time

of the mechanical velocity servo control system

while the velocity changes from positive to

negative and vice versa. The data of 1600 channels

acquired for a pre-set time at each velocity setting

are transferred to a ﬂoppy the PC and the MCS

system is cleared of data for the next velocity

setting. This process of recording the data and

transfer to ﬂoppy at each scan is repeated at 41

equally spaced velocity amplitude settings. We are

aware that FFT chips are used in radar technology

for on-line data processing but such a facility was

0 100 200 300 400 500 600 700

40

60

80

100

channel number:time

c

o

u

n

t

r

a

t

e

Fig. 9. Relative absorption depicting the effect of AC modula-

tion at a given velocity with each channel representing 3.6

phase interval.

Fig. 8. Functional electronic circuit diagram designed and used for the dual velocity modulation.

V.R. Reddy et al. / Nuclear Instruments and Methods in Physics Research A 501 (2003) 559–575 571

not available to the authors and thus an indirect

method of off-line data processing was implemen-

ted in the following manner.

4.2. Data analysis

4.2.1. Coherent detection

The total of data points consisted of

41 Â1600=65,600 records stored in the matrix

form (41, 1600). Having recorded data in the AC

modulated form, the Fourier coherent amplitude

at the modulation frequency is retrieved for each

of the 41 positive and negative velocity points

using the following expression and by adjusting for

the ﬁnite phase delays caused by the response of

the velocity drive unit

a

1

ðjÞ ¼ 400D

800

n¼1

½f

j

ðnDÞsin ð2pf

m

nD þj

0

Þ ð28Þ

where e

j

ðnDÞ is the data set at the ‘‘velocity j’’

with D ¼ 124 ms. In the present case, the phase

shift f

0

was equivalent to 32 channels in the ﬁrst

half of velocity cycle and 16 channels in the other

half velocity cycle. Driving the transducer with

square wave velocity with zero mean eliminates

any DC drift. Further, by repeating the spectral

scan, time averaging is also achievable [25]. Due to

manual operations of velocity increments such

averaging was not attempted. The MCS operation

with a locally available software operated on the

PC ensured the time spent at each velocity to be

the same as it is controlled by the internal clock

which also deﬁned the channel dwell time.

The numerical integration for the ﬁrst harmonic

amplitude reproduced the normal Mossbauer

spectrum illustrating the signal detection sensitiv-

ity of the analysis. The ﬁrst harmonic detection

contained most of the signal content. The results

observed for v

m

¼ g=4 are least-squared ﬁtted

(Fig. 10) and the estimated parameters are shown

in Table 2 indicating the better precision being

obtained from the technique. For the purpose of

comparison the normal Mossbauer spectrum

obtained by setting the sinusoidal modulation to

zero was computer ﬁtted which resulted in line

positions as 45.7170.21 with FWHM being

11.5270.45 channels. It is to be noted that the

AC modulation broadens the line as recorded at

S.No.1 in Table 2. The parameters derived from

differential spectrum with no AC modulation are

subjected to large variations. The relative line

broadening caused due to AC modulation with

v

m

¼ g=4 as estimated using Eq. (19) is about 1.04

which when corrected for the line broadening due

to AC modulation gives FWHM of line width

similar to those obtained for the normal spectrum

with no AC modulation. The integrated spectrum

seems to be of better precision than the AC

modulated differential spectrum. The line width

and line position parameters estimated from AC

modulation technique have a factor of two better

in precession compared to those estimated from

normal spectrum. Improvement in S=N ratio is

possible with an increase in the amplitude of

modulating signal. It can be shown that the ratio

of retrieved amplitudes a

1

ðjÞ for v

m

¼ 2g and g=4 is

about 3.2 and the corresponding ratio for the

spectral densities is about 10. This would imply

considerable improvement of S=N ratio is in store

when one employs AC modulation technique. It

can be shown that higher modulation depths not

only increases the ﬁrst harmonic amplitudes but

also yields reasonable second harmonic amplitudes

which measure the second derivative of the normal

absorption spectrum.

4.2.2. Auto-correlation analysis

The auto-correlation function has the capability

to enhance the signal-to-noise ratio. As per the

Weiner-Khinchin theorem, the Fourier transform

of the auto-correlation function gives the spectral

density and should be proportional to the square

of the ﬁrst harmonic amplitude obtained from the

cross-correlation technique. Further, the auto-

correlation of the data recorded in the dual

modulated mode as shown in Fig. 11(i) e

j

ðnDÞ is

evaluated as

R

i

ðkÞ ¼

1

350

350

n¼1

½f

i

ðnDÞf

i

ððn þ kÞDÞ

for k ¼ 1; 2; y; 350 ð29Þ

at the ith velocity and the result is shown in

Fig. 11(ii). Only 300 points out of 350 data points

of the auto-correlation function are considered

V.R. Reddy et al. / Nuclear Instruments and Methods in Physics Research A 501 (2003) 559–575 572

Table 2

Estimated Mossbauer parameters through least-squared analysis

S. No Legend Line position in

channels

FWHM (g) in

channels

1. Spectrum perturbed with AC modulation evaluated through a

0

coefﬁcient

45.7870.23 13.4370.51

2. Differential spectrum evaluated through the data of S.No.1 45.1670.78 19.2710.38

3. Differential spectrum with AC modulation evaluated through a

1

coefﬁcient

46.0370.18 12.3870.36

a

(11.9070.34)

4. Integral spectrum obtained through a

1

coefﬁcient 45.3970.07 11.7470.26

a

(11.3070.24)

5. Spectrum with no AC modulation 45.7170.21 11.5270.47

a

Corrected for line broadening

-1500

-1000

-500

0

500

1000

1500

(ii)

r

e

l

a

t

i

v

e

c

o

u

n

t

r

a

t

e

20 40 60 80

47000

48000

49000

50000

51000

52000

53000

54000

(i)

c

o

u

n

t

r

a

t

e

channel number:velocity

20 40 60 80

channel number:velocity

20 40 60 80

channel number:velocity

20 40 60 80

channel number:velocity

-6

-4

-2

0

2

4

6

(iii)

f

i

r

s

t

h

a

r

m

o

n

i

c

a

m

p

l

i

t

u

d

e

(iv)

r

e

l

a

t

i

v

e

a

b

s

o

r

p

t

i

o

n

Fig. 10. Representation of experimental results with the continuous curve representing the best ﬁt: (i) Mossbauer spectrum obtained

through a

0

calculation; (ii) differential of the normal Mossbauer spectrum obtained from the data given in (i); (iii) differential spectrum

obtained through cross-correlation analysis; (iv) integral of the ﬁrst harmonic amplitude method calculated from the data of Fig. 9(iii).

V.R. Reddy et al. / Nuclear Instruments and Methods in Physics Research A 501 (2003) 559–575 573

covering only the three cycles of modulation for

obtaining the spectral density at each velocity by

using the DFT and results for the spectral density

are shown in Fig. 12(i). The square of the Fourier

amplitudes a

1

is also shown in Fig. 12(ii) which is

almost similar to the spectral density results of the

auto-correlation method. It is interesting to note

that the separation between the two spectral

density peaks can be expressed in terms of the

AC modulation depth and the natural line width

and the detailed functional relation can easily be

derived [7], which gives the natural line width.

From this result it is seen that not only one

achieves improvement in the S=N ratio, but also

the resolution enhancement is possible in the AC

detection of signals. Minor differences in peak

heights of spectral densities as observed in the

ﬁgure and shapes may be attributed to experi-

mental problems associated with manual scanning

of velocity settings at 41 positions of the potenti-

ometer as even the minor potentiometer setting

errors get magniﬁed in the differential analysis.

5. Conclusions

The correlation techniques applied to Poisson

stochastic processes are shown to improve the

S=N ratio similar to those of phase-sensitive

detection methods. Simulation studies are shown

to illustrate their applicability in particle counting

measurements by employing easily available mod-

ern methods of data acquisition and analysis.

Results presented in this work demonstrated the

improved sensitivity by employing the AC detec-

tion. It is shown, with the facilities available to the

authors in Mossbauer spectroscopy, that the dual

modulation can be achieved for improving the

S=N ratio. It is shown that Fourier and correlation

analysis can be employed even for stochastic

processes in all ﬁelds of nuclear spectroscopy. As

a result of improved sensitivity of AC signal

detection in stochastic processes, the correlation

0 100 200 300 400 500 600 700

40

60

80

100

(i)

channel number:time

channel number:time

c

o

u

n

t

r

a

t

e

0 50 100 150 200 250 300 350

-1

-0.5

0

0.5

1

x 10

4

(ii)

c

o

r

r

e

l

a

t

i

o

n

a

m

p

l

i

t

u

d

e

Fig. 11. Sample representation of dual modulated absorption

data at a given velocity: (i) time spectrum as recorded in the

MCS mode of operating the spectrometer and (ii) auto-

correlation data resulting in noise reduction.

20 40 60 80

0

1000

2000

3000

4000

5000

(i)

channel number:velocity channel number:velocity

n

o

r

m

a

l

i

s

e

d

s

p

e

c

t

r

a

l

d

e

n

s

i

t

y

20 40 60 80

0

10

20

30

(ii)

n

o

r

m

a

l

i

s

e

d

s

p

e

c

t

r

a

l

d

e

n

s

i

t

y

Fig. 12. Spectral density variation resulting from: (i) auto-correlation method of analysis and (ii) cross-correlation method of analysis.

V.R. Reddy et al. / Nuclear Instruments and Methods in Physics Research A 501 (2003) 559–575 574

methods coupled with Fourier technique should

help in:

1. evaluating the multipolarity of nuclear transi-

tions, nuclear moments, internal hyperﬁne

ﬁelds, nuclear orientation effects, polarization

correlation and b-decay matrix elements, etc.,

with better precision;

2. overcoming the limitation of accidental coin-

cidences in directional correlation measure-

ments [2];

3. observing the positronium triplet state quench-

ing and positronium resonance for detecting

3

S-

1

S transition, which is till now limited by

large chance coincidence rates;

4. evaluating physical parameters with better

precision in all the photon/particle counting

spectroscopy like pulse height analysis, XRD,

XRF, RBS, ESCA, etc., in the differential mode

through the modulation of measurable para-

meters and at times without perturbing the

physical processes in contrast to the perturba-

tion caused by modulating ﬁeld as in NMR and

ESR spectroscopy; and

5. observing rare Mossbauer transitions with low

recoilless factors as well as of sharp line widths

through broadening by modulation [7].

Acknowledgements

The ﬁnancial support of the Department of

Science and Technology, Government of India,

through project no. SP/S2/M 67/96 dated

16.06.1999 and the Inter University Consortium

for DAE facilities for allowing to use the facilities

are acknowledged. The authors thank Mr. S. Das

for his help with the electronic circuit made.

References

[1] H. Frauenfelder, R.M. Steffen, in: K. Seighbahn (Ed.), a-,

b- and g-ray Spectroscopy, North-Holland, Amsterdam,

1965, p. 997.

[2] A.H. Wapstra, in: K. Seighbahn (Ed.), a-, b- and g-ray

Spectroscopy, North-Holland, Amsterdam, 1965, p. 539.

[3] P. DeBrunner, in: I.J. Gruverman (Ed.), Mossbauer Effect

Methodology, Vol. 1, Plenum press, New York, 1965, p.

97.

[4] G.F. Knoll, Radiation Detection and Measurement,

Wiely, New York, 1979.

[5] G. Feher, Bell System Technol. J. 36 (1957) 449.

[6] L.P. Kandanoff, et al., Rev. Mod. Phys. 39 (1967) 395.

[7] C.P. Poole, Electron Spin Resonance, Inter-Science,

London, 1967.

[8] H.J. Wahlquist, Chem. Phys. 35 (1961) 1708.

[9] G.V.H. Wilson, J. Appl. Phys. 34 (1963) 3276.

[10] L.C. Allen, H.M. Gladney, S.H. Glarum, J. Chem. Phys.

40 (1964) 3135.

[11] K. Rama Reddy, Nucl. Instr. and Meth. 190 (1981) 325.

[12] K. Rama Reddy, Nucl. Instr. and Meth. 81 (1970) 183.

[13] P. Rajamani Singh, K. Rama Reddy, Nucl. Instr. and

Meth. 179 (1981) 361.

[14] P. Rajamani Singh, K. Rama Reddy, Girish Chandra,

Indian J. of Pure Appl. Phys. 20 (1982) 297.

[15] A. Voffenheimer, A.S. Willskz, Signals & Systems,

Prentice-Hall of India Pvt. Ltd., India, 1999.

[16] A. Papoulis, Probability, Random Variables and Stochas-

tic Processes, McGraw-Hill, New York, 1965.

[17] Ronald N. Bracewell, Fourier Transforms and Applica-

tions, McGraw-Hill Book Company, New York, 1986.

[18] John G. Proakis, Dinitris G. Manolakis, Digital Signal

Processing, Prentice-Hall of India Pvt. Ltd, New Delhi,

1998.

[19] N.N. Greenwood, T.C. Gibb, Mossbauer Spectroscopy,

Chapman & Hall Ltd, London, 1971.

[20] A. Abragam, R.V. Pound, Phys. Rev. 25 (1953) 943.

[21] M. Morita, Nucl. Phys. 6 (1958) 132.

[22] D.L. Falkoff, G.E. Uhlenbeck, Phys. Rev. 79 (1950) 334.

[23] F. Boehm, V. Soergel, B. Stech, Phys. Rev. Lett. 1 (1958)

77.

[24] P.J. Brussaard, H.A. Tolhock, Physica 24 (1958) 233.

[25] M.P. Klein, G.W. Bar ton Jr., Rev. Sci. Instr. 34 (1963)

754.

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