First-principles investigation of the structural, dynamical, and dielectric properties of kesterite, stannite, and PMCA phases of 
<mml:math xmlns:mml="http://www.w3.org/1998/Math/MathML"><mml:mrow><mml:msub><mml:mi>Cu</mml:mi><mml:mn>2</mml:mn></mml:msub><mml:msub><mml:mi>ZnSnS</mml:mi><mml:mn>4</mml:mn></mml:msub></mml:mrow></mml:math>

Ramkumar, Sriram Poyyapakkam; Gillet, Yannick; Miglio, Anna; Setten, Michiel J. van; Gonze, Xavier; Rignanese, Gian‐Marco

doi:10.1103/physrevb.94.224302

Cited by 25 publications

(16 citation statements)

References 47 publications

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“…Typically, the higher frequency phonon modes, which are predominantly dominated by the motion of S atoms, show a red shift of 15 cm −1 with respect to experiment. Furthermore, in the two earlier works 6,7 in which the Raman intensities were calculated, the first prominent peak was found to be higher in intensity than the second one, in clear contrast with experimental findings.…”

Section: Introductioncontrasting

confidence: 80%

“…As a downside, their efficiency is only close to 8.6% 3 , making them commercially not viable at the moment. One major reason for the low efficiency in CZTS has been attributed to the presence of Cu-Zn disorder, confirmed by several experimental and theoretical studies, including Xray and neutron diffraction 4 , Raman spectra [5][6][7][8] , nuclear magnetic resonance (NMR) 9,10 , and photoluminescence measurements 11 .…”

Section: Introductionmentioning

confidence: 92%

“…We consider a kinetic energy cut-off of 450 eV for truncating the plane-wave basis set and k-point density of 750 points per reciprocal atom centered at Γ. Similar to a previous study by some of us 7 where the effect of XC functional was assumed not to influence the Raman intensities, the HSE Raman spectrum is determined using the intensities from LDA and NC pseudopotentials computed with Abinit.…”

Section: Computational Detailsmentioning

confidence: 99%

“…From the theoretical standpoint, all previous theoretical works [6][7][8]22,24,25 have focused on ordered structures. Most of them relied on semi-local exchange-correlation (XC) functionals such as the local density approximation (LDA) or the generalized gradient approximation (GGA).…”

Section: Introductionmentioning

confidence: 99%

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CZTS Raman spectra beyond kesterite: a first-principles study

Ramkumar,

Miranda,

Gonze

et al. 2021

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Cu2ZnSnS4 is an earth-abundant photovoltaic absorber material predicted to provide a sustainable solution for commercial solar applications. One of the main limitations restricting its commercialization is the issue of cation disorder. Raman spectroscopy has been a sought after technique to characterize disorder in CZTS while a clear consensus between theoretical and experimental results is yet to be achieved. In the present study, via the virtual crystal approximation, we take into account the progressive nature of Cu-Zn disorder in CZTS: we obtain the phonon frequencies at zone-center within the density functional perturbation theory formalism, and further compute the Raman spectra for the disordered phases, achieving a consensus between theory and experiment. These calculations confirm the presence of complete disorder in Cu-Zn 2a, 2c and 2d Wyckoff sites. They also show that the Raman intensities of two prominent A phonon modes characterized by motion of S atoms, also known to be experimentally significant, play a key role in understanding the nature of disorder in CZTS.

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Section: Introductioncontrasting

confidence: 80%

Section: Introductionmentioning

confidence: 92%

Section: Computational Detailsmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

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CZTS Raman spectra beyond kesterite: a first-principles study

Ramkumar,

Miranda,

Gonze

et al. 2021

Preprint

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“…[44][45][46] Multinary semiconductors, including the I 2 -II-IV-VI 4 and I-II 2 -III-VI 4 families of materials have been increasingly of interest in recent years across elds spanning photovoltaics, photocatalysis, nonlinear optics and thermoelectric energy generation. [47][48][49][50][51][52] The promising performance of quaternary thermoelectric materials has been found to be broadly driven by their low thermal conductivity. Kuo ), which were found to possess ultra-low thermal conductivities.…”

Section: Introductionmentioning

confidence: 99%