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1 2. Molecular stucture/basic spectroscopy

2 The electromagnetic spectrum Spectral region for atomic and molecular spectroscopy E. Hecht (2nd Ed.) Optics, Addison-Wesley Publishing Company,1987

3 Spectral regions Molecular l spectroscopy often deals with radiation in the ultraviolet (UV), visible, and infrared (IR) spectral regions. The visible region is from 400 nm 700 nm The ultraviolet region is below 400 nm The infrared region is above 700 nm. 400 nm 500 nm 600 nm 700 nm Spectroscopy: That part of science which uses emission and/or absorption of radiation to deduce atomic/molecular properties

4 Some basics about spectroscopy En nergy 0 = c / c hn = hc /l E = h = hc / E = Energy difference h = Planck's constant, Js = Frequency c = Velocity of light, m/s = Wavelength Often the wave number,, is used to express energy. The unit is cm -1. = E / hc = 1/ Example The energy difference between two states in the OH-molecule is cm -1. Which wavelength is needed to excite the molecule? Answer = 1/ =35714 cm -1 = 1/ = 280 nm. Other ways of expressing this energy: E = hc/ = J E / h = c/ = Hz

5 Species in combustion Combustion involves a large number of species Atoms oxygen (O), hydrogen (H), etc. formed by dissociation at high temperatures Diatomic molecules nitrogen (N 2 ), oxygen (O 2 ) carbon monoxide (CO), hydrogen (H 2 ) nitric i oxide (NO), hydroxyl (OH), CH, etc. Tri-atomic molecules Molecules with more than three atoms water (H 2 O), carbon dioxide (CO 2 ), etc. fuel molecules such as methane, ethene, etc. also molecules formed in rich flames

6 Quantum mechanics According to quantum mechanics all energy levels in atoms and molecules are discrete and are given by the solution to the Schrödinger equation: 2 2 V r = wavefunction 2 h = h/2 (h = Plancks constant) E m m m m 2 reduced mass E = energy levels V = potential energy Since the selections rules only permit certain transitions a spectrum can be very precisely calculated

7 Diatomic molecules: Structure A diatomic molecule consists of two nuclei and an electron cloud. The positive nuclei repel each other. The negative electrons attract the positive nuclei and prevent them from separation. When all electrons have their lowest possible energies, the molecule is in its ground electronic state. Ene ergy Ground electronic state

8 Diatomic molecules: electronic states We observe an outer loosely bound electron. By the addition of energy, it can be moved to another orbit at higher energy, and the molecule end up in an excited electronic state. + + ergy Ene Different electronically excited states Ground 0 electronic state

9 Absorption For many molecules of interest in combustion, absorption of radiation in the ultraviolet and visible spectral region can lead to electronic excitation of a molecule. + + This absorption process can be represented in an energy level diagram: Ene ergy 0 E The energy levels are discrete, and the energy difference can be used to calculate the exact wavelength of the radiation needed for absorption: E = hc/

10 Diatomic molecules: Structure The electronic states of molecules are in analogy with electronic states of atoms. In addition molecules can vibrate and rotate. In the Born-Oppenheimer approximation these - - motions are initially treated separately: E tot = E el + E vib + E rot - - To more easily describe vibrational and rotational energies, a simpler model for the molecule will be used. Consider the diatomic molecule as two atoms joined by a string. Time scales: Electronic interaction ~10-15 s Vibrations ~10-14 s Rotations ~ s - -

11 Diatomic molecules: vibrations Molecules can also vibrate at different frequencies. But only specific discrete vibrational frequencies occur, corresponding to specific energies.

12 Vibrational energy levels The vibrational energy states give a fine structure to the electronic states. v=0 is the lowest vibrational frequency, then higher v numbers correspond to higher vibrational frequencies. Energy } yv=2 Excited v=1 Electronic v=0}state While the separation between electronic energy states is around cm -1, the separation between vibrational energy states is on the order of 2000 cm v=2 v=11 v=0 Ground }Electronic }state

13 Vibrational energy levels Solutions to Schrödinger equation for harmonic oscillator with V(r) = ½ k (r e -r) 2 give E v /hc = G v V(r) = ½ k (r r) 2 ] ω(v 1/2) [cm 1 G 0 = 1/2, G 1 = 3/2, G 2 = 5/2 v = 1 = G(v') - G(v") = (v /2) - (v + 1/2) = V' -corresponds to levels in the excited state V" corresponds to levels in the ground state

14 Vibrational energy levels A better description of the energy is given by the Morse function: V D.[ 1 exp{ a ( req. r )}] [ eq eq 2 where a is a constant for a particular molecule. Energy corrections can now be introduced. Dissociation energy, D e. G v e (v 1/ 2) v = 1, 2, e x e (v 1/ 2) 2 [cm 1 ]

15 The transition from v=0 to v=1 then occurs at; G Vibrational population 2 1 1/ 2 x 1/ 2 1 2x cm 2 v 1 G v 0 1 1/ 2 x 1 1/ 2 e e e e e e e e Whereas the transition from v=1 to v=2 (hot band) occurs at G(v=2) - G(v=l) = e (1-4 e ) cm -1 Population distribution of of NN2 2 Population N v ; N v ~ exp[-g(v)/kt] Fractiona al populatio on 1 0,9 0,8 0,7 0,6 0,5 0,4 0,3 0,2 0, Temperature (K) v=0 v=1 v=2 v=3

16 Diatomic molecules: rotations Molecules can also rotate at different frequencies. But only specific discrete rotational frequencies occur, corresponding to specific energies.

17 Rotational energy levels The rotational energy states give a fine structure to the vibrational states. Energy yv=2 v=1 v=0 J = 6 J=0 is the lowest rotational energy state, then higher J numbers correspond to higher rotational J = 5 states. While the separation between vibrational energy states is around 2000 cm -1, the separation between rotational energy states is on the order of a few to hundreds of cm v=2 v=11 v=0 J = 4 J = 3 J =2 J = 1 J = 0

18 Energy levels for rigid rotator Solutions to Schrödinger equation with V(r) = 0, gives m 1 m 2 C 2 h E J ( 1) r 1 r J J I r 0 2 I r 0 m1 m2 m m 1 m 2 F J Er hc h J(J 1) 2 8 ci BJ(J 1) [cm 1 ]

19 Rotational transitions F = F (J') - F (J") = B J'(J'+l) - B J" (J"+l) J =±l F =2BJ J' - corresponds to levels in the excited state J" corresponds to levels in the ground state

20 Rotational population distribution The rotational population distribution can be calculated as N (2 J 1) e BJ( J 1) hc/ kt If f ( J) (2J 1) e BJ( J 1) hc/ kt f ( J) T then 0,07 gives J max 0 kt 2Bhc 1 2 on Relative e populati 0,09 0,08 0,06 T=300 K 0,05 0,04 0,03 0,02 0,01 Nitrogen T=1700 K Rotational quantum number, J

21 A coupling rotation-vibration Total energy T v,j given by: T v,j G 2 v F J v 1/ 2 x v 1/ 2 BJ J 1 A transition from v to v occurs at: e e e BJ' J' 1 BJ" J" 1 Consider two cases:

22 A coupling rotation-vibration: Example HCl absorption

23 HITRAN HITRAN is an acronym for high- resolution transmission molecular ABSORPTION, which is a database using spectroscopic parameters to predict and simulate the absorption spectra of different molecules

24 Example: The CO vibrational band (0-1) P Branch R Branch

25 Different broadening mechanisms: Collisional broadening and Doppler broadening Lorentz profile: g L 1 bl ( ) ( ) 0 b 2 2 L Doppler profile: ln 2 bd g ( D ) b 0 2 exp( (ln 2)( ) ) D Voigt profile convolution of Doppler and dlorentzian line shape function: ' ' ' V( ) D( ) L( ) g g g d

26 Absorption simulation H2O+CO2 H2O CO2 H2O+CO2 Isotope abundance: 1% Simulated concentration: 500 ppm Detect limit: 5 ppm

27 Transitions between electronic states A Absorption and emission spectra are species specific The energy difference (and thereby v=1 the wavelength) can be calculated v=0 using molecular parameters for the involved electronic states. Absorption Emission X v=1 v=0 } Rotational energy levels in the first excited vibrational state. } Rotational energy levels in the ground vibrational state. Equilibrium distance

28 Molecular structure - OH Q R P

29 Summary 1: Temperature effects At low temperature (room-t) Molecules generally rotate at lower frequencies. vibrate at lower frequencies At high temperature (flame-t) Molecules generally rotate at higher frequencies. vibrate at higher frequencies

30 Summary 2: Temperature effects Prob bability Population distribution over energy states at flame temperature, (also high rotational frequencies, not only lowest vibrational frequency) Pr robability Population distribution over energy states at room temperature, (Low rotational frequencies, lowest vibrational frequency) 0 The population distribution is often what is probed when temperatures are measured Energy

31 Summary: Molecular physics Each molecule is at a certain time in a specific rotational state, J, in a specific vibrational energy level, v, and in a specific electronic energy level. There is a high probability that a molecule changes state as a result of a molecular collision. However, the population distribution over all possible states is the same at a constant temperature (because of the large number of molecules). To excite an atom or a diatomic molecule a laser must be tuned to an exact wavelength for the excitation. A larger molecule, such as a 3-pentanone or acetone, has many more close-lying l states. t To excite such a molecule, l any wavelength within a range can be used for the excitation.

32 Summary Molecules have different energies; rotational energies, vibrational energies, and electronic energies. Information about the energy levels for molecules is used to interpret spectroscopic information from laser-based techniques and other optical techniques. Absorption and laser-induced fluorescence are techniques for which we need to know at which wavelength a certain species can be excited. Temperatures can be measured by probing the population p distribution over different energy levels, for example in Raman and CARS techniques.

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