Nucleation Kinetics of L-Arginine, L-Lysine and L-Alanine Doped Potassium Dihydrogen Phosphate Crystals

Parikh, Ketan; Parekh, B. B.; Dave, D. J.; Joshi, Mayank

doi:10.4236/jcpt.2013.33015

Cited by 18 publications

(4 citation statements)

References 15 publications

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“…We demonstrate an unprecedented degree of supersaturation with KH 2 PO 4 (KDP) aqueous solution, which is more than three times over previously reported values (31)(32)(33)(34)(35)(36)(37)(38)(39) (Table S1) by using the solution ESL apparatus. A crystal-solution interfacial free energy value estimated by CNT was also found to be much greater than previously reported (31)(32)(33)(34)(35)(36)38).…”

Section: Significancementioning

confidence: 43%

“…A crystal-solution interfacial free energy value estimated by CNT was also found to be much greater than previously reported (31)(32)(33)(34)(35)(36)38). In addition, we measure two distinctive probability distributions for the nucleation events as a function of supersaturation, which implies a possible existence of two different solution states.…”

Section: Significancementioning

confidence: 56%

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Multiple pathways of crystal nucleation in an extremely supersaturated aqueous potassium dihydrogen phosphate (KDP) solution droplet

Lee

et al. 2016

Proc. Natl. Acad. Sci. U.S.A.

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Solution studies have proposed that crystal nucleation can take more complex pathways than previously expected in classical nucleation theory, such as formation of prenucleation clusters or densified amorphous/liquid phases. These findings show that it is possible to separate fluctuations in the different order parameters governing crystal nucleation, that is, density and structure. However, a direct observation of the multipathways from aqueous solutions remains a great challenge because heterogeneous nucleation sites, such as container walls, can prevent these paths. Here, we demonstrate the existence of multiple pathways of nucleation in highly supersaturated aqueous KH 2 PO 4 (KDP) solution using the combination of a containerless device (electrostatic levitation), and in situ micro-Raman and synchrotron X-ray scattering. Specifically, we find that, at an unprecedentedly deep level of supersaturation, a highconcentration KDP solution first transforms into a metastable crystal before reaching stability at room temperature. However, a low-concentration solution, with different local structures, directly transforms into the stable crystal phase. These apparent multiple pathways of crystallization depend on the degree of supersaturation.multipath nucleation | liquid-droplet levitation | supersaturation | in situ X-ray diffraction | in situ micro-Raman spectroscopy N ucleation is the first step toward crystallization, in which atoms or particles aggregate to form clusters in a metastable liquid, called crystal nuclei. The crystal nuclei in metastable liquid grow continuously if their size exceeds a critical limit, and are subsequently stabilized. Based on the classical nucleation theory (CNT) (1, 2), nucleation is mainly governed by two factors, that is, interfacial free energy and volume Gibbs free energy (or chemical potential) between liquid and crystal phases. Although the volume Gibbs free energy acts to stabilize the crystal nuclei, the interfacial free energy works as an energy barrier preventing the formation of the nuclei. If the crystal-liquid interfacial free energy creates a sufficiently high energy barrier, the liquid can be supercooled, supersaturated, or even supercompressed. In case of liquid metals (3-6), the crystal-liquid interfacial free energy arises from configurational entropy differences between crystal and liquid. That is, the greater difference in local structural orderings between crystal and liquid phases results in higher interfacial free energy, which consequently leads to a higher nucleation barrier and thus deeper supercooling. This concept has been verified in various metallic systems for elements (7) and many alloys (8-12). However, many experimental and theoretical investigations have raised questions that CNT may not be adequate to describe the initial nucleation processes in biomaterials (13-17) and minerals (18)(19)(20)(21)(22)(23)(24)(25)(26).Recently, an alternate nucleation mechanism, called multipathway nucleation (or crystallization) (13-23, 25, 26), has been proposed fo...

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Section: Significancementioning

confidence: 43%

Section: Significancementioning

confidence: 56%

Multiple pathways of crystal nucleation in an extremely supersaturated aqueous potassium dihydrogen phosphate (KDP) solution droplet

Lee

et al. 2016

Proc. Natl. Acad. Sci. U.S.A.

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“…This value is significantly greater than any other results previously reported [52][53][54][55][56][57][58][59] (i.e. σ = 2~16.87 mJ/m 2 for s = 1.2~1.95).…”

Section: Metastable Monoclinic Kh 2 Po 4 (Kdp) Crystal Formation Fromcontrasting

confidence: 54%

Formation of Metastable Crystals from Supercooled, Supersaturated, and Supercompressed Liquids: Role of Crystal-Liquid Interfacial Free Energy

Lee

2017

Crystals

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Abstract:The formation mechanism of metastable crystals from metastable liquids still remains elusive, although controlling the metastability of crystals and liquids already plays a crucial role in designing new materials in physics, chemistry, biology, and materials science. This review article describes how metastable phases can be obtained by controlling temperature, concentration, and pressure. In particular, I show the role of crystal-liquid interfacial free energy in the formation of metastable crystals from metastable liquids at a given driving force. In a microscopic viewpoint, local structure similarity between the metastable crystals and liquid determines the crystal-liquid interfacial free energy, and thus the nucleation barrier for the metastable crystals. The effect of the interfacial free energy on the formation of metastable crystals from supercooled, supersaturated, and supercompressed liquids will be demonstrated with metallic liquids, aqueous solutions, and water.

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“…Many attempts have been made to modify its properties, either by changing the growth condition or by adding different impurities. [1][2][3][4][5][6][7] P. V. Dhanaraj et al 8 showed that the addition of K 2 CO 3 could make the KDP solution more stable than with other additives and enhanced the metastable zone width of the KDP solution for all temperatures. 8 They also found that the laser-induced damage threshold of a K 2 CO 3 -added KDP crystal was higher than that of the pure KDP crystal.…”

Section: Introductionmentioning

confidence: 99%

Growth of K2CO3-doped KDP crystal from an aqueous solution and an investigation of its physical properties

Rousta¹,

Dizaji²

2016

Mater. Tehnol.

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In this present work, KDP and 2M%-K2CO3-doped KDP crystals were grown by a slow-evaporation solution technique. The grown crystals were characterized by Fourier Transform Infrared (FT-IR) spectroscopy, X-ray diffractometry (XRD), UV-Vis spectroscopy, and laser damage threshold (LDT) analysis. The presence of the functional groups of the grown crystals was identified from the FT-IR spectra. The XRD tests showed that the grown crystals had a tetragonal structure. A comparison of the optical transmission of the grown crystals revealed that the K2CO3-doped KDP crystal had a higher transmission than the pure KDP crystal for the entire UV and visible region. Keywords: growth from solution, slow-evaporation solution technique, KDP crystal, K2CO3 additive V predstavljenem delu so KDP in z 2M % K2CO3 dopirani KDP kristali rasli s tehniko po~asnega izhlapevanja teko~ine. Dobljeni kristali so bili karakterizirani iz infrarde~o spektroskopijo s Fourierjevo transformacijo (FT-IR), z rentgensko difrakcijo (XRD), z UV-Vis spektroskopijo in s pragom po{kodbe z laserjem (LDT). Prisotnost funkcionalnih skupin kristalov v rasti je bila dolo~ena s FT-IR spektrom. XRD je pokazal, da imajo rasto~i kristali tetragonalno zgradbo. Primerjava prepustnosti svetlobe v rasto~ih kristalih je odkrila, da imajo KDP kristali, dopirani s K2CO3, bolj{o prepustnost kot pa~isti KDP v celotnem UV in v vidnem podro~ju. Klju~ne besede: rast iz raztopine, tehnika po~asnega izparevanja raztopine, KDP kristal, dodatek K2CO3

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Nucleation Kinetics of L-Arginine, L-Lysine and L-Alanine Doped Potassium Dihydrogen Phosphate Crystals

Cited by 18 publications

References 15 publications

Multiple pathways of crystal nucleation in an extremely supersaturated aqueous potassium dihydrogen phosphate (KDP) solution droplet

Multiple pathways of crystal nucleation in an extremely supersaturated aqueous potassium dihydrogen phosphate (KDP) solution droplet

Formation of Metastable Crystals from Supercooled, Supersaturated, and Supercompressed Liquids: Role of Crystal-Liquid Interfacial Free Energy

Growth of K2CO3-doped KDP crystal from an aqueous solution and an investigation of its physical properties

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