photoluminescence of chelyabinsk ll5 chondrite with … · 2018. 7. 19. · the fragment of...

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CONCLUSIONS A. S. Vokhmintsev, I. A. Weinstein Ural Federal University, NANOTECH Center Mira street, 19, Ekaterinburg, Russia, 620002, [email protected] SAMPLES AND TECHNIQUE RESULTS AND DISCUSSION INTRODUCTION Recently it was shown that fragments of Chelyabinsk LL5 chondrite, in which lithologies of various types dominate, had dissimilar physical and chemical properties [14]. On the one hand, this makes it possible to use relevant experimental methods to characterize such samples. On the other hand, we can talk about a more rigorous methodological and classification approach in studying the fundamental mechanisms responsible for the formation of observed feartures of the Chelyabinsk meteorite. It was found earlier [3, 4] that optically induced and luminescence processes occur more intensively in samples with light-colored lithology. The high content of inhomogeneous optically active centers, the variety of radiative and non-radiative transitions, the presence of competing systems of discrete and quasicontinuous levels of charge carriers capture in the energy gap lead to a complex kinetics of the observed processes and microscopic mechanisms of radiationally and thermally stimulated responses Chelyabinsk meteorite under different excitations. The purpose of this work was to study the temperature behavior of the photoluminescence (PL) spectra in the 7 300 K range of Chelabinsk LL5 chondrite samples with light-colored lithology. PHOTOLUMINESCENCE OF CHELYABINSK LL5 CHONDRITE WITH LIGHT-COLORED LITHOLOGY IN 7 300 K TEMPERATURE RANGE PL was excited by ultraviolet pulsed radiation from the DTL-389QT solid-state laser (Laser-Export, LLC) with a wavelength of 263 nm and frequency of 1 kHz. PL signal was registered using a Shamrock SR-303i-B spectrograph (Andor, Inc.) with cooled Newton EM DU970P-BV-602 CCD detector (Andor, Inc.). The temperature of the sample was changed by means of a CCS-100/204N helium cryostat (Janis Research Company, LLC) with a closed loop equipped with DT-670B-CU sensor, HC-4E compressor and 335 Model controller (Lake Shore Cryotronics, Inc.). The pressure inside the cryostat was maintained by HiCube 80 Eco vacuum pumping station (Pfeiffer Vacuum, LLC) at a level of P 10 -4 mBar. PL spectra were recorded in the range of λ = 350 900 nm at different temperatures: T = 7 K, in 10 100 K range in steps of 10 K and from 100 to 300 K in steps of 20 K. Spectral parameters The temperature behavior of the photoluminescence spectra in 7 300 K range of the Chelyabinsk LL5 chondrite with light-colored lithology is studied. It is shown that the PL dependences are characterized by two wide bands with maxima at 2.5 eV (490 nm) and 1.8 eV (680 nm) in the spectral range under study. It is found that the ratio of the maximum intensities of the registered bands has a complex dependence on the temperature in the investigated range. Deconvolutions of all experimental PL spectra into several Gaussian components are performed. It is demonstrated that the spectrum observed at 300 K is quite accurately approximated by single Gaussian and the spectrum measured at 7 < T < 150 K is numerically described by three components. Temperature dependences of the maximum PL intensity in the investigated bands are analyzed in the framework of the modified Mott model with “negative” thermal quenching. It is evaluated that the activation energies of the PL negative thermal quenching is E nq = 38 3 meV (7 < T < 240 K) in 2.5 eV band and PL thermal quenching are E q = 300 55 meV (T > 240 K range) and 28 7 meV (7 < T < 240 K) for 2.5 and 1.8 eV bands, correspondingly. The fragment of Chelyabinsk LL5 chondrite characterized by light-colored lithology (LCL) predominantly was selected. The core of the meteorite was separated from fusion crust and crushed into micropowder, which was treated in hydrochloric acid to remove metal particles. Chelyabinsk meteorite samples LCL [1] Popova O.P. et al. 2013. Science 342: 10691073. [2] Kohout T et al. 2014 Icarus 228: 7885. [3] Weinstein et al. 2014. Meteorit. Planet. Sci. 49: A428. [4] Weinstein I.A. et al. 2015. Meteorit. Planet. Sci. 50: 5175. [5] Vokhmintsev A.S. and Weinstein I.A. 2017. Meteorit. Planet. Sci. 52: A371. [6] Shibata H. 1998. Jpn. J. Appl. Phys. Part 1. 37(2): 550-553. 400 500 600 700 800 900 0 5 10 15 PL intensity,10 4 a.u. Wavelength, nm Experimental PL spectra at different temperature: T = 300 K T = 240 K T = 180 K T = 120 K T = 60 K 3.5 3 2.5 2 1.5 Photon energy, eV REFERENCES Thermal quenching of PL in the framework of the modified Mott mechanism [6] : 1 0 1 1 1 nq q nq q E E I(T) I P exp P exp kT kT ex , nm em , nm P nq E nq , meV P q E q , meV T, K Reference 263 490 6 1 38 3 (6 1)10 4 300 55 7 300 This work 680 21 5 28 7 230 480 13.510 4 340 10 300 773 [5] 530 6.210 4 310 10 210 480 31.010 4 360 10 530 10.610 4 320 10 Quenching parameters 50 150 250 350 450 550 0 5 10 15 PL intensity,10 4 a.u. Temperature, K Experimental data: 490 nm (2.5 eV) 680 nm (1.8 eV) Approximation by Eq. (1) Data from work [5]: , 480 nm , 530 nm 1.5 2.0 2.5 3.0 3.5 G3 G2 G1 Experimental data, T=60 K Approximation , , Gaussian peaks Photon energy 900 800 700 600 500 400 Wavelength, nm 1.5 2.0 2.5 3.0 3.5 0 1 Experimental data, T=300 K Gaussian peak Normalized PL intensity, a.u. Photon energy G1 900 800 700 600 500 400 Wavelength, nm Parameter Peak G1 G2 G3 T, K 60 E max , 0.01 eV 2.42 1.86 1.68 , 0.01 eV 0.95 0.21 0.34 T, K 300 E max , 0.01 eV 2.34 , 0.01 eV 0.96 where I 0 is the PL intensity at T = 0 K; P nq and P q are dimensionless pre-exponential factors; k is the Boltzmann constant; E nq and E q are the “negative” quenching and quenching activation energies, respectively.

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Page 1: PHOTOLUMINESCENCE OF CHELYABINSK LL5 CHONDRITE WITH … · 2018. 7. 19. · The fragment of Chelyabinsk LL5 chondrite characterized by light-colored lithology (LCL) predominantly

CONCLUSIONS

A. S. Vokhmintsev, I. A. WeinsteinUral Federal University, NANOTECH Center

Mira street, 19, Ekaterinburg, Russia, 620002, [email protected]

SAMPLES AND TECHNIQUE

RESULTS AND DISCUSSION

INTRODUCTION

Recently it was shown that fragments of Chelyabinsk LL5 chondrite, in which lithologies of various types dominate, had dissimilar physical and chemical

properties [1–4]. On the one hand, this makes it possible to use relevant experimental methods to characterize such samples. On the other hand, we can talk

about a more rigorous methodological and classification approach in studying the fundamental mechanisms responsible for the formation of observed feartures

of the Chelyabinsk meteorite. It was found earlier [3, 4] that optically induced and luminescence processes occur more intensively in samples with light-colored

lithology. The high content of inhomogeneous optically active centers, the variety of radiative and non-radiative transitions, the presence of competing systems

of discrete and quasicontinuous levels of charge carriers capture in the energy gap lead to a complex kinetics of the observed processes and microscopic

mechanisms of radiationally and thermally stimulated responses Chelyabinsk meteorite under different excitations. The purpose of this work was to study the

temperature behavior of the photoluminescence (PL) spectra in the 7 – 300 K range of Chelabinsk LL5 chondrite samples with light-colored lithology.

PHOTOLUMINESCENCE OF CHELYABINSK LL5 CHONDRITE

WITH LIGHT-COLORED LITHOLOGY IN 7 – 300 K

TEMPERATURE RANGE

PL was excited by ultraviolet pulsed radiation from the DTL-389QT solid-state laser (Laser-Export, LLC)

with a wavelength of 263 nm and frequency of 1 kHz. PL signal was registered using a Shamrock SR-303i-B

spectrograph (Andor, Inc.) with cooled Newton EM DU970P-BV-602 CCD detector (Andor, Inc.). The

temperature of the sample was changed by means of a CCS-100/204N helium cryostat (Janis Research

Company, LLC) with a closed loop equipped with DT-670B-CU sensor, HC-4E compressor and 335 Model

controller (Lake Shore Cryotronics, Inc.). The pressure inside the cryostat was maintained by HiCube 80 Eco

vacuum pumping station (Pfeiffer Vacuum, LLC) at a level of P ≤ 10-4 mBar. PL spectra were recorded in the

range of λ = 350 – 900 nm at different temperatures: T = 7 K, in 10 – 100 K range in steps of 10 K and from

100 to 300 K in steps of 20 K.

Spectral parameters

The temperature behavior of the photoluminescence spectra in 7 – 300 K range of the Chelyabinsk LL5 chondrite with light-colored lithology is studied.

It is shown that the PL dependences are characterized by two wide bands with maxima at 2.5 eV (490 nm) and 1.8 eV (680 nm) in the spectral range under

study. It is found that the ratio of the maximum intensities of the registered bands has a complex dependence on the temperature in the investigated range.

Deconvolutions of all experimental PL spectra into several Gaussian components are performed. It is demonstrated that the spectrum observed at 300 K is

quite accurately approximated by single Gaussian and the spectrum measured at 7 < T < 150 K is numerically described by three components.

Temperature dependences of the maximum PL intensity in the investigated bands are analyzed in the framework of the modified Mott model with “negative”

thermal quenching. It is evaluated that the activation energies of the PL negative thermal quenching is Enq = 38 3 meV (7 < T < 240 K) in 2.5 eV band and

PL thermal quenching are Eq = 300 55 meV (T > 240 K range) and 28 7 meV (7 < T < 240 K) for 2.5 and 1.8 eV bands, correspondingly.

The fragment of Chelyabinsk LL5 chondrite characterized by light-colored lithology (LCL) predominantly was selected. The core of the meteorite was

separated from fusion crust and crushed into micropowder, which was treated in hydrochloric acid to remove metal particles.

Chelyabinsk meteorite samples

LCL

[1] Popova O.P. et al. 2013. Science 342: 1069–1073.

[2] Kohout T et al. 2014 Icarus 228: 78–85.

[3] Weinstein et al. 2014. Meteorit. Planet. Sci. 49: A428.

[4] Weinstein I.A. et al. 2015. Meteorit. Planet. Sci. 50: 5175.

[5] Vokhmintsev A.S. and Weinstein I.A. 2017. Meteorit. Planet. Sci. 52: A371.

[6] Shibata H. 1998. Jpn. J. Appl. Phys. Part 1. 37(2): 550-553.

400 500 600 700 800 900

0

5

10

15

PL

inte

nsi

ty,

10

4 a

.u.

Wavelength, nm

Experimental PL spectra

at different temperature:

T = 300 K

T = 240 K

T = 180 K

T = 120 K

T = 60 K

3.5 3 2.5 2 1.5

Photon energy, eV

REFERENCES

Thermal quenching of PL in the framework

of the modified Mott mechanism [6] :

1

01 1 1

nq q

nq q

E EI(T) I P exp P exp

kT kT

ex,

nm

em,

nmPnq

Enq,

meVPq

Eq,

meV

T,

KReference

263490 6 1 38 3 (6 1)104 300 55

7 – 300 This work680 – – 21 5 28 7

230480 – – 13.5104 340 10

300 – 773 [5]530 – – 6.2104 310 10

210480 – – 31.0104 360 10

530 – – 10.6104 320 10

Quenching parameters

50 150 250 350 450 550

0

5

10

15

PL

inte

nsi

ty,

10

4 a

.u.

Temperature, K

Experimental data:

490 nm (2.5 eV)

680 nm (1.8 eV)

Approximation

by Eq. (1)

Data from work [5]:

, 480 nm

, 530 nm

1.5 2.0 2.5 3.0 3.5

G3

G2

G1

Experimental data, T=60 K

Approximation

, , Gaussian peaks

Photon energy

900 800 700 600 500 400

Wavelength, nm

1.5 2.0 2.5 3.0 3.5

0

1

Experimental data, T=300 K

Gaussian peak

No

rmal

ized

PL

in

ten

sity

, a.

u.

Photon energy

G1

900 800 700 600 500 400

Wavelength, nm

ParameterPeak

G1 G2 G3

T, K 60

Emax, 0.01 eV 2.42 1.86 1.68

, 0.01 eV 0.95 0.21 0.34

T, K 300

Emax, 0.01 eV 2.34

, 0.01 eV 0.96

where I0 is the PL intensity at T = 0 K;

Pnq and Pq are dimensionless pre-exponential

factors; k is the Boltzmann constant;

Enq and Eq are the “negative” quenching and

quenching activation energies, respectively.