Indian Institute of Science Education and Research

Kolkata

Department of Physical Sciences

Summer Project Report, June-July 2020

Emission spectra of B-TAN and checking if the

Emitted light has any kind of circular Polarization
Depending on the Helicity of the Molecule (CPL
Spectroscopy)
Submitted by

Koushik Barai

on

15.07.2022

under the supervision of

Prof Bipul Pal

Name of the Department

ISER Kolkata
 Declaration

I declare here that the report included in this project entitled “Emission spectra of B-TAN and
checking if the Emitted light has any kind of circular Polarization Depending on the Helicity of
the Molecule (CPL Spectroscopy)” is the summer internship carried out by me and my other
lab mate Mr. Ayan Sahoo in the Department of Physical Science, Indian Institute of Science
Education and Research Kolkata, India from May 17 to July 15, 2022 under the supervision
of Prof./Dr. Bipul Pal.

In keeping with general practice of reporting scientific observations, due acknowledgements

have been made wherever the work described is based on the findings of other investigators.

Mohanpur 15.07.2022

_____________________ ________________ ________________

Student’s e-Signature Place Date

 CERTIFICATE

It is certified that the summer research work included in the project report entitled “Emission
spectra of B-TAN and checking if the Emitted light has any kind of circular Polarization
Depending on the Helicity of the Molecule (CPL Spectroscopy)” has been carried out by Mr.
Koushik Barai and Mr. Ayan Sahoo jointly under my supervision and guidance. The
content of this project report has not been submitted elsewhere for the award of any acedemic
and professional degree.

Signature of Supervisor
July 15, 2022 (Prof./Dr. Bipul Pal)
IISER Kolkata Project Supervisor
 Table of content

Declaration 2
Certificate 3
Table of content 4
Acknowledgement 5

“Emission spectra of B-TAN and checking if the Emitted light has any
kind of circular Polarization Depending on the Helicity of the Molecule
(CPL Spectroscopy)”

1.1 Introduction 6
1.2 Aim and Objective 6
1.4 Discussion 7- 12
1.3 Experimental section 12-20
1.5 Conclusion 20
1.5 Future Directions 21
1.6 References and Notes 21-22
 Acknowledgements

I sincerely thank IISER Kolkata for giving me the opportunity to carry out my summer
internship.
I would also like to thank Prof. Bipul Pal for his guidance and valuable suggestions.

Mohanpur 15.07.2022

_____________________ ________________ ________________

Student’s e-Signature Place Date

“Emission spectra of B-TAN and checking if the Emitted light has any
kind of circular Polarization Depending on the Helicity of the Molecule
(CPL Spectroscopy)”

Introduction

Polarization of light is a property that applies to turning waves that shows the geometrical blooming of the

oscillations. Depending on the polarization we see different properties.

On the other hand, Luminescence is spontaneous emission of light by a substance not resulting

from heat. This spontaneous emission can also have polarization. Circular polarization of

luminescence is a phenomenon that can be observed for chiral molecules in isotropic solution, for

molecular aggregates and molecular materials. The interest in circularly polarized luminescence

(CPL), which is the differential emission of right- and left-circularly polarized light by chiral

luminescence systems (molecules, polymers, supramolecular aggregates, etc.), has experienced

noticeable growth in recent years. This fact is due to not only the valuable use of CPL as a source of

information on the structure of the involved excited states but also its application in the improvement

and potential development of multiple photonic tools like lasers sensors spintronics based devices,

etc.

Aim and Objective

The basic idea behind this project is to find a way So that we can know about the structure of a molecule with
some simple experimental set up and logics.

The molecule we have chosen for our experiment is BTAN, which presumably has helical structure. So, we
intend to measure the emission spectra and see that if the sample is excited with un-polarized light will the
emitted light has any kind of circular polarization.

If we find any kind of positive results then we can use this experimental setup to get idea about the Molecular
structure of any Sample. This is similar as CPL spectroscopy. The commercial setup for this experiment is
available, but this is very costly. So, our aim is to create a setup that would simply do the desired job.

Theory and Discussion

This is the very basic things that will be helpful for understanding the Project work. This is a short
introduction about the optical components we have used. This is stated without going much deep into
the derivations and mathematical intricacies.

• LASER
A LASER is a device that controls the way that energized atoms release photons. "Laser" is an
acronym for Light Amplification by Stimulated Emission of Radiation, which describes very succinctly
how a laser works.
A laser differs from other sources of light in that it emits light which is coherent. Spatial coherence
allows a laser to be focused to a tight spot.

• Polarizer
A polarizer is a purely optical device that can convert a beam of unpolarized light into one that is
appreciably polarized in some form.
A linear polarizer transmits light uniformly vibrating in a single plane while absorbing the orthogonal
plane. We usually describe a single plane or beam of polarized light in terms of what we call the
pattern of vibration. If the vibrations are in one direction, the light is linearly polarized.

There are two axes: transmitting and absorbing. The transmitting axis is normally referred to as the
“polarizing axis.” Light passing through a single polarizer loses at least 50% transmission, depending
upon the grade of polarizer used (transmission specifications) and the polarization requirements.

Crossing the two linear polarizer axes at 90 degrees to one another can produce near absolute
blockage of light or cancellation. This is called extinction. The ratio of the transmission of two
polarizers with axes parallel to axes crossed is known as the efficiency of the polarizer.

• QWP
A quarter-wave plate consists of a carefully adjusted thickness of a birefringent material such that the
light associated with the larger index of refraction is retarded by 90° in phase (a quarter wavelength)
with respect to that associated with the smaller index. The material is cut so that the optic axis is
parallel to the front and back plates of the plate. Any linearly polarized light which strikes the plate will
be divided into two components with different indices of refraction. One of the useful applications of
this device is to convert linearly polarized light to circularly polarized light and vice versa. This is done
by adjusting the plane of the incident light so that it makes 45° angle with the optic axis. This gives
equal amplitude o- and e-waves. When the o-wave is slower, as in calcite, the o-wave will fall behind
by 90° in phase, producing circularly polarized light.

How a QWP transforms Linearly polarized light into a circularly Polarized light

The quality of the circularly polarized light can be checked by rotating the polarizer - the intensity
of light passing through the polarizer should remain unchanged. If it varies somewhat, it means
that the light is actually elliptically polarized, and the waveplate isn’t exactly a quarter-waveplate at
operating wavelength of your interest. This may be corrected (as with the half-waveplate) by tilting
the waveplate about its fast or slow axes slightly, while rotating the polarizer to check for
constancy.

• Energy states and Vibronic transitions

Solving Schrodinger equation we get a quantization of energy levels, for a one-electron
system like Hydrogen we get a quantization which is represented using the principal quantum
no. n
𝑅ℎ𝑐
𝐸𝑛 = − , where R is called the Rydberg's constant and n = 1,2,3...
𝑛2
So,
1 1
𝛻𝐸𝑛 = −𝑅ℎ𝑐 ( 2 − 2)
𝑛2 𝑛1
Now associated with each electronic level are a number of vibrational energy levels. These
are the sources of the Vibrational Coarse Structure in Electronic Spectroscopy. The
vibrational energy quantization comes from the Harmonic osscilator model applied to various
1
molecules which finally gives us the following expression. 𝐸𝑛 = (𝑛 + 2) ℎ𝑣
where n can be any positive integer or zero representing the n-th state and 𝑣 is the vibrational
frequency.
2
Using Morse Potential Equation, 𝑉𝑟 = 𝐷(1 − 𝑒 −𝛽(𝑟−𝑟𝑛) ) ,The harmonic osscilator model is
made to be closer to the real scenario. Where, D is the dissociation energy and 𝛽 is an
empirical parameter.
Then It is a better representation of real scenario than QHO by adding the Anharmonicity
factor which is;
1 1 2
𝐸𝑛 = (𝑛 + ) ℎ𝑣 + (𝑛 + ) ℎ𝑣 𝜒𝑒
2 2

where 𝜒𝑒 is known as the Anharmonic constant.

Selection Rule associated with such transition is 𝛥𝑛 = ±1

• rotational fine structure in spectral diagram

Each of the Vibrational states are composed of a number of Rotational energy states which
arise from the consideration of Rigid Rotor model. By quantum mechanical approaches again
we quantize these states using some quantum numbers which also represent angular
momentum.
{J(J+1)h2 }
E(J) = {8\pi2 I}

where J is the azimuthal quantum number and I is the moment of inetia of the rotor system.
Like vibrational spectra we can get selection rules for rotational spectra as well given by
𝛥𝐽 = ±1 (in some special cases 𝛥𝐽 might be equal to zero).

Figure 1: Various energy levels and associated transitions

Note, 𝛥E(𝐽) = 2B(J+1) which shoes that the spectral lines are equidistant. But this is not the
real scenario as the space between the lines progressively decreases with increasing J because
of the Centrifugal Distortion.

• Broad Spectrum
Any spectra show sharp peaks and various characteristic structures when there are less
external or inter-molecular effects at play like for example gaseous phase. But in condensed
or solution phase due to various other effects at play the fine structures are lost and a much
broader spectrum is observed.
In our experiment the spectrum is broad because it is made into a solution in DMSO. Also
Note: CPL can depend on the type of the solvent used.

• Polarization of light
Identifying and understanding various polarization states is very important for our
experiment.
We basically use Jones Calculus for easy representation of the states.
We can represent the linear polarized light along x and y axes respectively as;
1 0
|𝑥⟩ = ( ) and |𝑦⟩ = ( )
0 1
We can represent circular polarized light in Jones formalism.

For Right Circular Polarized Wave. 𝐸𝑥 = 𝐸0 𝑒 {𝑖(𝑘𝑧−𝑤𝑡)}

𝜋
{𝑖(𝑘𝑧−𝑤𝑡+ )}
and, 𝐸𝑦 = 𝐸0 𝑒 2 = 𝑖𝐸0 𝑒 {𝑖(𝑘𝑧−𝑤𝑡)}

Hence, we can write;

1 1 1
𝐸 = 𝐸0 |𝑥⟩ + 𝑖 𝐸0 |𝑦⟩ = 𝐸0 ( ) = √2𝐸0 ( )
𝑖 √2 𝑖

So, the normalized Jones vectors for LCP and RCP are given as follows;
1 1
|𝑅𝐶𝑃⟩ = (|𝑥⟩ + 𝑖 |𝑦⟩) |𝐿𝐶𝑃⟩ = (|𝑥⟩ − 𝑖 |𝑦⟩)
√2 √2
Also, these can be used to represent |𝑥⟩ 𝑎𝑛𝑑 |𝑦⟩ as follows;
1 1
|𝑥⟩ = (|𝑅𝐶𝑃⟩ + 𝑖 |𝐿𝐶𝑃⟩) |𝑦⟩ = (|𝑅𝐶𝑃⟩ − 𝑖 |𝐿𝐶𝑃⟩)
√2 √2
 Polar plot for RCP Polar plot for LCP

Jones Formalism is also used to derive matrix representations for various actions like that of
QWP, HWP, LP, etc.
The Jones matrix for a LP with transmission axis tilted at theta degree from x axis is

represented as (𝑇𝐿𝑃 )_𝐹𝜃 = [ cos 2 𝜃 𝑐𝑜𝑠 𝜃 𝑠𝑖𝑛 𝜃 ]

𝑐𝑜𝑠 𝜃 𝑠𝑖𝑛 𝜃 sin2 𝜃
Having fixed our setup at +45 degree for the LP this reduces to
1 1 1
(𝑇𝐿𝑃 (+45) ) = [ ]
2 1 1

• relation of LCP and RCP during energy level transitions

Using the 1-electron model the Schrodinger's equation has been solved to get necessary wave
functions. using these wave functions (assuming unit value for the radial component) one can
derive the vibrational and rotational selection rules we discussed before.
Proceeding with the idea that transition dipole moment is non-zero we derive the selection
rules for vibrational transitions that 𝛥𝑚 = ±1
𝛥𝑚 = +1 corresponds to emission of RCP
𝛥𝑚 = −1 corresponds to emission of LCP
𝛥𝑚 = 0 corresponds to Linearly polarized light

Polar plot for Linear polarized light along x axis light Polar plot for elliptically polarized light with low ellipticity and
phase difference of 90
 Polar plot for elliptically polarized light with high ellipticity and phase difference of 90.

• Photo-Spectrometer
Using this instrument, the distribution of the spectral intensity detected by the spectrometer is
analyzed photoelectrically. In a spectrometer monochromator is used, A monochromator is
incorporated into fluorescence spectrophotometers and emission spectrometers to determine the
wavelength of fluorescence lines or emission lines emitted from the sample.
In this case, the monochromator is located between the sample compartment and detector. It
transmits a mechanically selectable narrow band of wavelengths of light or other radiation chosen
from a wider range of wavelengths available at the input.

Experimental section

Molecular structure of BTAN

Generally, to record an emission-spectra the setup shown below is used.

we made our set up using an incandescent lamp with Tungsten filament as the light source
because of it’s quite good emissivity and also its intensity is very uniform over the visible
spectrum. Moreover, it also gives us the unpolarized light that we need. But while performing
the experiment even though we could see light getting emitted by the sample upon excitation,
it was not getting registered by the CCD's attached to the second monochromator
/spectrograph. The intensity of the emitted light wasn’t enough. So, to get rid of this, we had
to take a laser so that we can have a much more intense beam of light and thus the excitation
is better and so is the intensity of the emitted light. But now we have linearly polarized laser
light so we have to depolarize it and make it unpolarized.
For depolarizing it we first used two sheets of white paper. it gave us some fair depolarization
which we could verify using a polarizer film after the paper (the intensity was varying
between a short range of 7.6 uW to 10.5 uW). But shortly after we got hold of a custom-made
depolarizer which psudo-randomizes the linearly polarized laser light (on keeping a polarizer
after the depolarizer we got a very small variation in intensity, 3.01mW to 3.24mW). But
there was one more requirement of beam expander before we direct the laser in the
depolarizer. Otherwise, the depolarizer wasn’t able to depolarize the light. So, After using
one beam expander this had a good depolarizing effect and also did not have as much loss of
intensity as that of paper.
Now we discuss a bit more about paper depolarization and our experiments on it and
what more we tried:
what we know is that paper causes good scattering of light due to high penetration depth. We
tried to use this scattering phenomena to achieve depolarization of our laser light. but we
faced a problem while doing so because after going through the paper the light intensity was
becoming very less and also much of the light was getting lost due to random direction of
wave vector after the scattering. To improve the transparency of the paper so as to attain
better intensity we put some oil on the paper and make it translucent. Now because of
scattering the light could not be focused nicely using lenses. So, in order to improve that we
used a cardboard blackened on one side with a hole of the size of lens aperture so that we can
block of rogue scattered light and collect only that part which has somewhat directionality
towards the lenses. Obviously, it did cutoff some of the light intensity but we could focus the
light better. Below is the setup shown along with the data (we have also provided the data
with the commercial depolarizer for comparison).
 Set-up for measuring depolarizing capability of oiled paper

One thing to note here is that the focusing of the light was better when the cardboard was
placed just behind the lens almost touching it. In general, scattered light cannot be easily
focused because it goes randomly in any direction without any specific spatial correlation
between different k-vectors. So, our target is to use that part of light which is somewhat
directional with the paper as a pseudo-source. Keeping the cardboard near lens satisfies our
needs because only the light which diverges up-to the lens edge get through the lens and give
more or less parallel light beam (the lens is fixed such that the paper is at its focal length thus
acting as somewhat like a point source for that light going through lens.
Below we try to show the depolarization capability of paper with respect to the commercial
de-polarizer. to check the degree of depolarization we have to use a polarizer which will act
as an analyzer for us. While using a polarizer we should have parallel beam of light pass
through it so that the k-vectors at each and every point of the beam are parallel and the
polarizer acts on them in the exact same way. on the contrary if the beam would have been a
converging one then the k-vectors will also be pointing in different directions at different
points of the beam and thus the polarizer will not be interacting with them in the same way
and the result will be unpredictable.
Below is the polar plots for both of them,
Ideally for unpolarized light the plot should be circles.

So, we can see clearly both of them works well. Still if we want to compare Paper was
depolarizing better than the commercial depolarizer. But at the same time paper was
destroying a lot of intensity, The emitted light has intensity in range of micro watts. So, again
we had to change the paper depolarization idea and go with the commercial depolarizer,
which has intensity in range of mili-watts.

• Experimental Procedure and Emission Spectra of BTAN

So, using a laser which is monochromatic itself (not perfectly still, very short range of
wavelengths to be accurate) we remove the 1st monochromator shown in the schematic
diagram from our setup.
So, we have a laser with output at about 400nm followed by an intensity blocker which is
made of glass with varying thickness of metal coating on it. We can rotate the blocker to get
adequate intensity for our experiment.
After the blocker there is a beam expander. Expanding the cross-section of the laser beam
helps depolarize it better at the depolarizer which is placed after the expander. Finally, a
plano-convex lens is used to focus the beam very tightly on the sample so as to get maximum
excitation.
Now the light emitted by the sample is divergent in all directions. But we intend to use the
light in the perpendicular direction only so that we can avoid the surplus incident light which
passes straight through the sample.
One thing to note here is that we do not intend to focus our incident light on the sample very
tightly because that would cause molecules from a very small space to get excited. rather if
we let the light diverge a little through the sample then more of the molecules will come in
the way of the light and more of them will get excited and thus more luminescence will be
recorded. This was experimentally observed by us while trying to focus the incident light.
We place two more plano-convex lenses for collecting the emission in the perpendicular
direction. The first one collimates the diverging beam whereas the second one focuses it in
the monochromator to get maximum possible intensity (higher the intensity the better we can
distinguish the peaks). This monochromator coupled with a CCD (Charged Coupled Device)
gives the intensities of the emitted light over a range of wavelengths which has been
separated by the diffraction action of the monochromator.

• Further modifications of the setup and approach to detect CPL:

For this part of our experiment, we need some minor changes in our set-up following the
excitation of our sample. Our principle aim in this section is recording the PL spectra of the
light emitted but in two different orientations of the required setup so that LCP and RCP can
be separately identified (if any).

• Finding the plane of polarization of axis and calibrating the angles on LP and QWP

For doing our CPL measurement we needed to calibrate our QWP and LP. To do that we
have used laser light. Now we cannot do the calibration unless we know the plane of
polarization of the laser. For that we make use of Brewster's Law (and also Fresnel
equations). The basic principle is that for TM configuration (where electric field is oscilating
in the plane of incidence, p or parallel polarization) the reflected light intensity will be zero at
Brewster's angle.
So, for that we take check the intensity of reflected light at the Brewster angle of glass (~56
degrees) for two perpendicular planes of incidence in one of which the light will be TM
configuration and that will tell us the plane of polarization of laser. Following this procedure,
we found that the laser is polarized vertically with respect to the optical bench in the lab.
The setup that we used is shown below (Figure 9)

We used a glass slide as our reflecting surface which we could rotate by hand after fixing on
a post/stand.

• Checking if there is at all any specific chirality in the sample

For this we fixed our polarizer at 45 degree with respect to our optical bench. the reason
being that the response of our monochromator is the best at this angle (actually this is to
nullify any polarization dependance of the monochromator). Now we rotate the Quarter
Wave Plate through 360degree in intervals of 10degree. We polar plot the readings and
analyze the shape.
From the shape of the plot, it is evident that the molecule does have some chirality which is
resulting in the emission of circularly polarized (not perfectly) light.
The maxima of each of these lobes occur when the circular polarization after going through
the QWP aligns along the fixed polarizer.

• To record the CPL by recording the PL at two different relative orientations of the
QWP and Linear polarizer. Also, to plot the luminescence dissymmetry factor
against wavelength.

Here we can proceed with the experiment in two different ways;

1. fixing the polarizer at 45 degree itself and rotating the fast axis of quarter wave plate from
90 degree to 180 degree to record two different data which we expect to give us the RCP and
LCP respectively.

2. fixing the wave plate with its fast axis at 90 degree and rotating the polarizer from +45
degree to -45 degree so that we can record RCP and LCP respectively.
After recording the two data files we employ the formula on them at each wavelength;
2[𝐼𝐿 − 𝐼𝑅 ]
𝑔𝑙𝑢𝑚 =
(𝐼𝐿 + 𝐼𝑅 )
and plot it against wavelength.
This is basically the plot for our CPL study known as the luminescence dissymmetry factor
and shows that our sample does have some specific chirality which results in the different
intensities of the LCP and RCP.
• Problems faced
Using the quarter waveplate we had in our lab we got some unexpected results.

As mentioned, before we rotated our QWP by 90 degree. So, upon rotating by 180 degree we
expect to get the same orientation back and thus similar 𝑔𝑙𝑢𝑚 . But we did not get so and for
some of the orientations 𝑔𝑙𝑢𝑚 was coming exactly negative of the plot that was expected.
What we witnessed was that the intensity differences for 180 degree rotation of wave plate
was non-zero and moreover a function of wavelength as shown below and this dependance
was the main reason behind the abnormal plots of 𝑔𝑙𝑢𝑚 we got peviously.

We suspected that the problem might lie in the QWP. To be sure we tried out the action of
QWP on plane polarized light from the laser. We let the laser light through the QWP at two
orientations differing by exactly $180\degree$ and then had it incident on the sample
separately and finally collecting the emitted light using the monochromator. after analyzing
the data for the two orientations we got the plot of their difference in intensities as follows
(apparently a function of wavelength).
This is clearly a problem because, that means the waveplate is not acting in the expected way.
$180\degree$ difference essentially means the exact same orientation and so the difference in
the intensities should have been zero or almost constant near zero. But that not being the case
our CPL plot was also not as per our expectations.

Another possible source of the problem for our CPL experiment is that the emitted light is not
totally circularly polarized and some linearly polarized and elliptically polarized light is also
present. These interacts with the QWP and polarizer differently and do not cancel out in the
calculation of 𝑔𝑙𝑢𝑚 and thus give wrong/unexpected results. So, we should look into it more
in the future.

Conclusion
we can conclude these two points;

1. The quarter wave plate is error prone, so much so that it alters magnitude at
180degree rotation.
From the previous section we can see that the error which is coming in upon rotating the
QWP by 180 degree is of the same order of magnitude as the supposed 𝑔𝑙𝑢𝑚 value. In
such a scenario we cannot get any fixed result. Depending upon the error the 𝑔𝑙𝑢𝑚 will
take positive and negative values at 180degree rotation.

2. We suspect that the sample has low CPL which combined with the QWP was
incapable of giving us a clear result.
The error would not have affected much if the sample had more CPL property. From the
polar plot of B-TAN (Figure 10) we can see that B-TAN has high ellipticity that is RCP and
LCP both are emitted in almost same magnitude or the fraction of light which is circularly
polarized is small in comparison to that of the elliptically ones and thus too hard to detect
 Future Directions

As we stated earlier This is a growing field, trying to see and analyzing properties of light with
quantum mechanical ideas. As due to time constraints we were unable to arrange a quarter wave
plate that would work in our desired wavelength.

But we hope this is a great idea to detect helicity of a molecule from its optical behaviour, So, future
studies to solve this problem and getting a positive result will be great. This will be beneficial from
commercial viewpoint also.

The presence of chirality around us in nature prompts us to explore CPL studies to put it to use (like,
CPL microscopes and other CPL devices like switches and sensors). Active research on a unifying
description of the origin of the circular polarization is still going on. It seems that quantum field theory
of electromagnetic interactions could provide leads for a comprehensive description of the circular
polarization including contributions from helicity at all possible length scales from the molecular to the
macroscopic.

References and Notes

1. https://www.ncbi.nlm.nih.gov/pmc/articles/PMC6321390/

Chen N, Yan B. Recent Theoretical and Experimental Progress in Circularly Polarized Luminescence of Small
Organic Molecules. Molecules. 2018 Dec 19;23(12):3376. doi: 10.3390/molecules23123376. PMID: 30572665;
PMCID: PMC6321390.

2. Meskers, Stefan. (2021). Circular Polarization of Luminescence as a Tool To Study Molecular Dynamical
Processes. ChemPhotoChem. 10.1002/cptc.202100154.

3. Zhang, Xiao-Peng & Wang, Li-Li & Qi, Xiao-Wei & Zhang, Da-Shuai & Yang, Qian-Ying & Shi, Zai-Feng & Lin,
Qiang & Wu, Tao. (2018). Pt···Pt interaction triggered tuning of circularly polarized luminescence activity in
chiral dinuclear platinum(II) complexes. Dalton Transactions. 47. 10.1039/C8DT02277A..

4. Circularly Polarized Luminescence by Visible-Light Absorption in a Chiral O-BODIPY Dye: Unprecedented

Design of CPL Organic Molecules from Achiral Chromophores
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Bryan G. Vo, Gilles Muller, and Santiago de la Moya
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