MMT assay results of the cytotoxic activities of various compounds against cancer cells with their IC50 values.
\\n\\n
Released this past November, the list is based on data collected from the Web of Science and highlights some of the world’s most influential scientific minds by naming the researchers whose publications over the previous decade have included a high number of Highly Cited Papers placing them among the top 1% most-cited.
\\n\\nWe wish to congratulate all of the researchers named and especially our authors on this amazing accomplishment! We are happy and proud to share in their success!
\\n"}]',published:!0,mainMedia:null},components:[{type:"htmlEditorComponent",content:'IntechOpen is proud to announce that 179 of our authors have made the Clarivate™ Highly Cited Researchers List for 2020, ranking them among the top 1% most-cited.
\n\nThroughout the years, the list has named a total of 252 IntechOpen authors as Highly Cited. Of those researchers, 69 have been featured on the list multiple times.
\n\n\n\nReleased this past November, the list is based on data collected from the Web of Science and highlights some of the world’s most influential scientific minds by naming the researchers whose publications over the previous decade have included a high number of Highly Cited Papers placing them among the top 1% most-cited.
\n\nWe wish to congratulate all of the researchers named and especially our authors on this amazing accomplishment! We are happy and proud to share in their success!
\n'}],latestNews:[{slug:"stanford-university-identifies-top-2-scientists-over-1-000-are-intechopen-authors-and-editors-20210122",title:"Stanford University Identifies Top 2% Scientists, Over 1,000 are IntechOpen Authors and Editors"},{slug:"intechopen-authors-included-in-the-highly-cited-researchers-list-for-2020-20210121",title:"IntechOpen Authors Included in the Highly Cited Researchers List for 2020"},{slug:"intechopen-maintains-position-as-the-world-s-largest-oa-book-publisher-20201218",title:"IntechOpen Maintains Position as the World’s Largest OA Book Publisher"},{slug:"all-intechopen-books-available-on-perlego-20201215",title:"All IntechOpen Books Available on Perlego"},{slug:"oiv-awards-recognizes-intechopen-s-editors-20201127",title:"OIV Awards Recognizes IntechOpen's Editors"},{slug:"intechopen-joins-crossref-s-initiative-for-open-abstracts-i4oa-to-boost-the-discovery-of-research-20201005",title:"IntechOpen joins Crossref's Initiative for Open Abstracts (I4OA) to Boost the Discovery of Research"},{slug:"intechopen-hits-milestone-5-000-open-access-books-published-20200908",title:"IntechOpen hits milestone: 5,000 Open Access books published!"},{slug:"intechopen-books-hosted-on-the-mathworks-book-program-20200819",title:"IntechOpen Books Hosted on the MathWorks Book Program"}]},book:{item:{type:"book",id:"5611",leadTitle:null,fullTitle:"Radiotherapy",title:"Radiotherapy",subtitle:null,reviewType:"peer-reviewed",abstract:"Radiotherapy plays a key role in the treatment of many cancer types. 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by",editors:[{id:"39553",title:"Prof.",name:"Everlon",middleName:"Cid",surname:"Rigobelo",slug:"everlon-rigobelo",fullName:"Everlon Rigobelo"}],productType:{id:"1",title:"Edited Volume",chapterContentType:"chapter",authoredCaption:"Edited by"}}},ofsBook:{item:{type:"book",id:"10499",leadTitle:null,title:"Next - generation Greenhouses",subtitle:null,reviewType:"peer-reviewed",abstract:"\r\n\tGreenhouse cultivation has evolved from simple covered rows of open-fields crops to highly sophisticated controlled environment agriculture facilities that projected the image of plant factories for urban agriculture. The advances and improvements in greenhouse technology have promoted scientific solutions for the efficient production of plants in populated cities and multi-story buildings. Successful deployment of high-tech greenhouses for urban agriculture requires many components and subsystems, as well as the understanding of the external influencing factors that should be systematically considered and integrated.
\r\n\r\n\tThis book project aims to highlight some of the most recent advances in modern greenhouse technology for food security and the sustainability of crop production. Each chapter is expected to raise the awareness for technology transfer in advanced controlled environment agriculture, which is necessary for a successful transition to urban agriculture. Contributing chapters will highlight several aspects of a high-tech closed-field plant production system including improvements in the frame and covering materials, environment perception and data sharing, and advanced microclimate control and energy optimization models. In addition, the book will highlight urban agriculture and its derivatives, including vertical farming, rooftop greenhouses, and plant factories which are the extensions of CEA and have emerged as a response to the growing population, environmental degradation, and urbanization that are threatening food security. Finally, several opportunities and challenges will be identified as a summary chapter to show how integrated controlled environment agriculture can be implemented as vertical farming for urban agriculture.
\r\n\t
The term autophagy (from the Greek, auto – oneself, phagy - to eat or autophagy-self eating) was first coined for structures that were observed under an electron microscope and that were consisted of single-or double-membrane lysosomal-derived vesicles containing cytoplasmic particles including organelles during various stages of disintegration [1,2]. Autophagic cell death or autophagy is a type of cell death that occurs in the absence of chromatin condensation but is associated with the massive autophagic vacuolization of the cytoplasm [3]. Autophagy is the process by which cells recycle their own nonessential, redundant, and damaged organelles and macromolecular components. Autophagy also plays its role in the suppression of tumor growth, deletion of toxic misfolded proteins, elimination of intracellular microorganisms, and pathogenesis of several diseases such as cancer and muscular disorders [4-6].
Like apoptosis, autophagy is an evolutionary conserved process that occurs in all eukaryotic cells [7]. Autophagy can be triggered as a result of nutrient deprivation, differentiation, and developmental factors. In contrast to the apoptosis, cells that die with an autophagic morphology have little or no association with phagocytes. Excessive autophagy may be attributed to crumple the cellular functions and induce cell death directly. On the other hand, autophagy can lead to the execution of apoptotic or necrotic cell death programs. It has also been suggested that autophagy may occur as a process alongside apoptosis or it may play a supportive role in apoptosis [8]. Autophagy and apoptosis differ in morphological characteristics. The causative relationship between these two has not been elucidated yet. The increase in autophagosomes indicates an increase in autophagic activity or decreased autophagosome-lysosome fusion. The most important characteristic of autophagic cell death is the appearance of double- or multiple-membrane vesicles (autophagosomes) in cytoplasm, which sequesters cytoplasmic components and organelles such as mitochondria and endoplasmic reticulum [9].
Cancer is an umbrella term covering a plethora of conditions characterized by unscheduled and uncontrolled cellular proliferation [10]. Cancer is the second leading cause of mortality with an incident rate of about 2.6 million cases reported annually across Europe and USA [11]. Autophagy has a multifaceted role in cancer [12,13]. Even though, present studies are only associative, autophagy most probably functions to curtail neoplasia [14]. There are several oncogenes including PI3K and Akt family members, MTOR, and Bcl2 restrain autophagy, while tumor suppressors such as PTEN, HIF1A, and TSC2 endorse autophagy [15]. Paradoxically, autophagy is double-edged sword having a role in promoting both cell survival and cell death [16]. The role of autophagy in the demise of a cell is contentious [17]. Despite the fact that number of autophagosomes increases in some dying cells, it is still ambiguous whether these structures are involved or just facilitate cell death [18]. The genetic deletion of key autophagic genes pick up the pace rather than to inhibit cell death, which accentuate the predominant survival role of autophagy [19].
Although, apoptosis and autophagy are markedly different processes but several lines of evidence have portrayed interplay between these two processes; such as the proteins from the Bcl2 regulate both autophagic and apoptotic machinery [17]. Furthermore, three types of interplay exist between autophagic and apoptotic pathways. Both apoptosis and autophagy function as a collaborator to induce cell death; autophagy act as anagonistic to hamper apoptotic cell death by promoting cell survival, autophagy act as enabler of apoptosis, and contributing in certain morphological and cellular events that occur during apoptotic cell death without leading to death in itself [8].
Cancer is considered as a complex group of genetic disorder with multiple causes. It is thought to be involved in perturbation of several different pathways that control and regulate the cell differentiation, cell proliferation, and cell survival. Another enigma has been the role of autophagy in tumor suppression; cancer may be protected by macroautophagy by sequestering damaged organelles, permitting cellular differentiation, increasing protein catabolism, and promoting autophagic cell death [20]. There are some experimental evidences which support the possibility that autophagy promotes the survival of nutrient-starved tumor cells and in turn contribute to cancer. Recent advances give deep insight into the molecular mechanism of autophagy. These findings more likely favor the concept that autophagy and defects in autophagy contribute to tumor suppression and oncogenesis respectively. Biochemical studies and genetic evidences designed in mammalian cells and in C. elegans respectively suggest that autophagy is positively regulated by the PTEN tumor suppressor gene and negatively regulated by the oncogenic Class I phosphatidylinositol 3-kinase signaling pathway. Furthermore Beclin 1, the mammalian APG gene has tumor suppressor activity and maps a tumor susceptibility locus, which is commonly deleted in human breast and ovarian cancers. The molecular mechanism of oncogenesis in human cancer can be fairly understood through genetic disruption of autophagy control. Such insights may foster the development of novel approaches to restore autophagy in the chemoprevention or treatment of human malignancies [21].
Autophagy is a kind of homeostatic mechanisms which accelerates and induces tumorigenesis when it disrupts. It removes the damaged organelles/proteins, limiting cell growth and causes genomic instability which are involved in the tumor suppression mechanism [22]. The experimental studies show that Beclin 1 is a haploin sufficient tumor suppressor gene. As this protein is used for autophagy induction and Beclin 1+/− mice were shown to be tumor prone [23]. The excessive stimulation of autophagy due to Beclin 1 protein overexpression can inhibit tumor development [24]. The accumulation of p62/SQSTM 1 protein aggregates, damaged mitochondria, and misfolded proteins due to the formation of molecular link between defective autophagy and tumorigenesis generate the reactive oxygen species (ROS) and genomic instability is observed due to the damage of DNA. ROS and the DNA damage can be prevented by knockdown of p62/SQSTM 1 in autophagy-defective cells [22]. The relationship between defective autophagy and p62/SQSTM 1 accumulation with tumorigenesis is further evidenced from a study involving p62/SQSTM 1−/− mice protected from Ras-induced lung carcinoma compared with wild-type animals [25]. It is further concluded that autophagy may also provide protection against tumorigenesis by limiting necrosis and chronic inflammation, which are associated with the release of pro-inflammatory HMGB1 [26]. All above findings give a concentric remark about the role of the autophagy as a mechanism of tumor suppression.
The autophagy plays a predominant role in cancer cells to confer stress tolerance, which serves to maintain tumor cell survival [20]. The induction of cell death mainly relates to the knockdown of essential autophagy genes in tumor cells [27]. Cancer cells have high metabolic demands. The exposure of increased cellular proliferation and in vivo models to metabolic stress was shown to impair the survival of autophagy-deficient cells with compared to autophagy-proficient cells [22]. Moreover, cytotoxic and metabolic stresses, including hypoxia and nutrient deprivation, can activate autophagy for recycling of ATP and in maintaining the cellular biosynthesis and survival. Autophagy is mainly considered to be induced in hypoxic tumor cells from regions that are distal to blood vessels and HIF-1α-dependent and -independent activation have been described [28]. The expression of angiogenic factors, such as vascular endothelial growth factor, platelet-derived growth factor, and nitric oxide synthtase are HIF-1α [28]. Human pancreatic cancer cell lines have increased basal levels of autophagy. These enable tumor cell growth by maintaining cellular energy production. Autophagic inhibition may lead to tumor regression and extended survival in pancreatic cancer xenografts [29]. In the survived cancer cells autophagy generates a state of dormancy in residual cancer cells that may further contribute to tumor recurrence and progression [30]. The increased efficacy of anticancer drugs, in response to inhibition of autophagy, supports cytoprotective role of autophagy in cancer cells. The research data indicate that H-ras or K-ras bearing activating mutations show high basal levels of autophagy in human cell lines irrespective of abundant nutrients [31]. The cell growth in these cell lines was associated with autophagic proteins. In conclusion, it is the autophagy that maintains tumor cell survival. Moreover it suggests that by blocking autophagy in tumors is an effective treatment approach [21].
Under the physiological conditions cells show compliance with respect to how they die responding various stimuli. There are certain factors such as the type of cell, type and intensity of noxious signals, and ATP concentration that determine how cells die [19]. Acute myocardial ischemia (which is involved in the sudden fall in ATP level) induces necrosis, whereas chronic congestive heart failure (with more modest yet chronic decrease in ATP) induces apoptosis [32]. Although, a particular cell death program may preferentially be triggered in different circumstances and multiple pathways may be activated concomitantly or successively in individual dying cells [33]. Furthermore, there seems to exist an interplay among different cell death pathways. Even though apoptosis and autophagy both bear distinct morphological characteristics and physiological processes, still there exist some intricate interrelationships between them. Apoptosis and autophagy, under some conditions, play synergistic effects; while other times autophagy onsets only when apoptotic suppression occurs. Moreover, recent studies have markedly pointed out the existence of strong interconnection between apoptosis and autophagy and also strengthened the concept of simultaneous regulation of both A’s that trigger cell death in cancer. The obstruction of a particular pathway of cell death may not avert the annihilation of the cell but instead may recruit an alternative path such as the broad-spectrum anti-apoptotic caspase inhibitors, zVAD-fmk, modulates the three major types of cell death. Addition of zVAD-fmk blocks apoptotic cell death, sensitizes cells to necrotic cell death, and induces autophagic cell death [34].
The overexpression of anti-apoptotic proteins may lead to the survival of injured cells where critical metabolites are provided by autophagy [35]. Nevertheless, if death stimuli persist, anti-apoptotic pathways and autophagy are unlikely to prolong and necrosis ensues [36]. Most likely, NF-κB, ATG5, ATP, and PARP function as molecular switches that determine whether a cell undergoes apoptosis, necrosis, or autophagy [37-39]. Protein p53 also modulates autophagy and other responses to cell stress. Recent studies reveal that basal p53 activity suppresses autophagy, whereas the activation of p53 by certain stimuli induces autophagy and the activation of p53 by different stimuli results in the PUMA- and NOXA-mediated apoptosis [40-42]. In addition, low and moderate concentrations of some agents have been revealed to induce apoptosis, but increasing the concentration of the same agent triggers necrosis. The challenge is, therefore, not only to understand the mechanisms leading to cell death but also to categorize the connection at the molecular level between different modes of the cell death.
In this chapter, we discussed the natural compounds and their mechanisms by which they induce apoptotic and autophagic cell death in cancer cells and their potential as a novel strategy for the treatment of cancer. We also presented the results of our previously published natural compounds screened against gastric cancer [43]. The screen was used to identify new targets to combat cancer or to identify selective natural compounds those target to apoptosis or autophagy signaling pathways. In this chapter, we reviewed the main effects of natural compounds on the different autophagic cell death signaling pathways. In addition, we focused on highlighting several representative plant-derived natural compounds such as curcumin, resveratrol, evodiamine, oridonin, and magnolol (structures of these compounds are shown in Fig. 1) that may lead to cancer cell death - for regulation of some core autophagic pathways, involved in Ras-Raf signaling, Beclin-1 interactome, BCR-ABL, PI3KCI/Akt/mTOR, FOXO1 signaling, the NF-κB-mediated pathway, the PI3K/Akt signaling pathway, p53 and other main pathways. Two of the identified autophagy inducer natural compounds, magnolol and evodiamine, have been discussed in detail, while the other natural compounds, which had shown an essential role in autophagic cell signaling pathways, been reviewed recently by Zhang et al., 2012 [44].
The structure of natural compounds that act on autophagic cell signaling pathways.
The rationale for overall project design was based on assumptions as presented above, which were motivated by the set of issues. The main goal of the study was to explore naturally occurring compounds that exhibit cytotoxic activity toward cancer cells. To search for compounds with significant cytotoxic activity and unprecedented chemical structures from a variety of traditional Chinese medicines, the crude ethanolic extracts of 300 species of herbal plants, traditionally used in China for the treatment of a variety of diseases, and four hundred TCM compounds were screened. Understanding the interplay of different cancer-related signaling pathways is important for the development of efficacious multi-targeted anticancer drugs. Hence, the underlying molecular mechanisms of the above mentioned natural compounds have been elucidated, which induced cell death.
The screening strategy has been shown in schematic form in Fig. 2. Several cancer cells, including SGC-7901, U87, PANC-1 and A-375 cells were cultured in DMEM supplemented with 10% fetal bovine serum and were exposed to different Chinese medicinal herbs extracts and TCM compounds.
Schematic presentation of strategy of identification, isolation, structure elucidation, and screenings of Traditional Chinese medicines (TCM) against cancer cells.
Acridine orange staining assay was performed according to published procedure [45]. In brief, cells were incubated without (control) and with respective compounds and with rapamycin (positive control group) for indicated time periods and then acridine orange at a final concentration of 1 mg ml-1 was added to cells for a period of 20 minutes in the dark at 37 °C. Then, cells were washed twice with PBS. Images of cells were obtained under fluorescence microscopy
AVOs formation (autophagosomes and autolysosomes) is a characteristic feature of Autophagy [17]. Furthermore, for quantification of AVOs, we used flow cytometry after the cells were stained by Acridine Orange (AO) [46]. AO is a weak base that accumulates in acidic spaces and gives bright red fluorescence (punctate staining (dots) in the cytoplasm which is detected by fluorescence microscopy and the formation of AVOs can be quantified by flow cytometry. The intensity of the red fluorescence is proportional to the degree of acidity.
The large collections of Traditional Chinese medicinal herbs and natural compounds libraries have been used to identify anticancer TCM herbs and natural compounds associated with various cancer specific cellular processes such as apoptosis or autophagy. A list of natural compounds those expressed cytotoxic activity against gastric cancer cells has been presented in Table 1 [43]. Using Traditional Chinese medicinal herbs and natural compounds libraries screen, we discovered several TCM compounds that showed potential anticancer activities [43]. In a natural compounds screen with glioma brain tumor cells, our results revealed that alantolactone and Pseudolaric acid B have shown selective anti-glioma activity with lesser toxic effect over liver and kidney [47,48]. Furthermore, we reported that Dracorhodin perchlorate regulates PI3K/Akt, p53 and NF-κB pathways that are frequently deregulated in cancer and their simultaneous targeting by Dracorhodin perchlorate could result in efficacious and selective killing of cancer cells [49]. Through the screen of natural compounds for apoptosis and autophagic cell signaling pathways, we identified several compounds including costunolide and xanthoxyletin that induce cell death via apoptotic pathways [50,51]. In addition, we also found that several compounds such as curcumin, resveratrol, evodiamine, oridonin, and magnolol induce autophagy and act on autophagic cell signaling pathways (unpublished data). Furthermore, we examined the role of evodiamine- and magnolol-induced autophagy in cancer cell death [52,53]. The role of each of the natural compound in autophagic cell signaling will be discussed later in this chapter.
Plants have a long recorded history to employ in the treatment of cancer [54] and represent the most important direct antecedent to contemporary anticancer drugs [55]. Recently, some of the most encouraging clinical evidences and promising anticancer natural herbal compounds let us to reconstruct the story of these plants and their ultimate role in chemotherapy [56]. To provide a paradigm of the most contemporary progress in this field, there were number of compounds namely artesunate, homoharringtonine, arsenic trioxide and cantharidin isolated from natural products and have the potential for use in cancer therapy. For many years, apoptosis has taken a center stage as the most important mechanism of programmed cell death in mammalian tissues. Apoptosis is a common mode of action for chemotherapeutic agents including natural product-derived drugs [57,58]. Four categories of dynamic cellular activities, which lead to cell death, have been described: apoptosis, autophagy, necrosis, and mitotic catastrophe [59]. With contemporary development in cancer research, it has also been increasingly noted that conventional chemotherapeutic agents not only elicit apoptosis but also activate other modes of cell death such as necrosis, mitotic catastrophe, senescence, and autophagy [60].
MMT assay results of the cytotoxic activities of various compounds against cancer cells with their IC50 values.
Autophagy represents a major route for degradation of aggregated cellular proteins and dysfunctional organelles. Accumulated lines of evidence have recently revealed that targeting autophagic signaling pathways might be a promising avenue for potential therapeutic purposes. Alterations in autophagy are thought to play an important role in the pathogenesis of many diseases—for example, Autophagy is closely associated with tumors and plays an important role in human tumor suppression, so inducing autophagy is a potential therapeutic strategy in adjuvant chemotherapy [61,62]. Many studies have demonstrated that anticancer agents induce autophagy, leading to the implications that autophagic cell death may be a vital mechanism for tumor cell killing by these agents [63] and are beneficial in the context of various models of cancer cells. The autophagy machinery interfaces many cellular stress-response pathways, and recent studies depict that defects in autophagy lead to cancer cell proliferation [64]. The regulation of autophagy in cancer cells can enhance tumor cell survival, yet can also suppress the initiation of tumor growth. Understanding the signaling pathways involved in the regulation of autophagy is crucial to the development of anticancer therapies [21]. In this chapter, we reviewed the natural compounds molecular mechanisms of autophagy and examined ongoing drug discovery strategies for modulating autophagy for therapeutic benefits. The natural anti-tumor agents have led to enhanced enthusiasm for the development of drugs that target the various aspects of the autophagic pathways. Some of these autophagic cellular approaches by representative natural compounds in autophagic induced cell death have been outlined in Fig. 3. In addition, magnolol and evodiamine have been illustrated in detail.
In our own studies, performing the screen for natural compounds that induce autophagy, we identified magnolol [52]. Magnolol, a natural compound, has been reported to inhibit growth in a variety of tumor cells [65]. Several researchers reported that magnolol-induced cell death involve apoptosis while Li et al [66] reported that magnolol-induced death occurs via autophagy but not apoptosis. We observed that there was no significant formation of AVOs at low concentration while AVOs were formed at a higher concentration of magnolol treated cells. The formation of acidic vesicular organelles (AVOs) is one of the characteristic features of cells, which passes through process of autophagy after their exposure to different autophagy inducer agents [67,68]. Autophagic vacuoles (AV) or autophagosomes are formed as result of sequestering of parts of the cytoplasm or entire organelles respectively during the process of autophagy [62]. Currently autophagic cell death has been studied as a potential method for cancer therapy. To determine the role of magnolol-induced autophagy in killing the SGC-7901 cells, we added the autophagy inhibitor, 3-methyladenine (3-MA), which controlled autophagy pathway at various points [8]. In contrast to the previous report [69], it was found that magnolol-induced cell death was not suppressed when treating the cells in combination with 3-MA. These results showed that magnolol-induced autophagy is not involved in the induction of SGC-7901 cell death. In addition, the findings also demonstrated that magnolol-induced autophagy may has an effect on ATP level in the SGC-7901 cells and supported those observations which showed that autophagy may alter the morphological and cellular events (ATP, cells blebbing and DNA fragmentation) that take place in apoptotic cell death, without leading to cell death in itself [8].
Evodiamine is a naturally occurring quinolone alkaloid found in the fruit of Evodia rutaecarpa. The data of several studies concerning the cytotoxic activity on cancer cells demonstrated that evodiamine inhibited the growth of several tumor cells [70]. Results from our screen indicate that evodiamine induced apoptosis and autophagy simultaneously in human gastric cancer cells. Evodiamine has been reported as an inducer of autophagy in human cervical carcinoma HeLa cells [71]. Autophagy is closely associated with tumors and plays an important role in human tumor suppression, so inducing the autophagy is a potential therapeutic strategy in adjuvant chemotherapy [61,62]. When the cells are exposed to various autophagy inducer agents, they form acidic vesicular organelles, which is an important characteristic of autophagy [67,68]. Thus, we observed the effect of evodiamine treatment on the formations of AVOs in SGC-7901 cells using fluorescence microscopy after staining with the lysosomotropic agent, acridine orange (AO). These findings indicate that evodiamine, a natural compound, has the potential to activate autophagy in gastric cancer cells. This result of evodiamine is also consistent with the results of the studies reporting that natural compounds can induce autophagy in various cancer cells. We also demonstrated that evodiamine-induced cell death was partially suppressed when the cells were treated in combination with specific autophagy inhibitor, 3-MA. These results showed that evodiamine-induced autophagy was partially involved in the cell death of cancer cells [52]. While our recent studies demonstrated that autophagy inhibition enhanced evodiamine-induced apoptosis in prostate cancer cells, indicating a survival function of autophagy (unpublished data). These results corroborate the line of evidence demonstrating that evodiamine-induced autophagy, implicated in cell survival, contributes to the cytoprotective role of autophagy [71,72]. These facts demonstrated that there is still a great discrepancy between roles of natural compounds-induced autophagy in cancer cells. The role (or more likely roles because as we discuss, distinct functions for autophagy occur at different times) of natural compounds-induced autophagy in cancer, is a topic of intense debate. These responses might vary with cell type and type of stress, and will undoubtedly reflect the nature of the mutational events occurring in the tumor cells, not only that of BECN1 and the PI3K pathway as described above, but also p53 status [73,74]. Moreover, it is believe that in short term assays, the phenomenal protection caused by autophagy inhibition may be due to delay in cell death instead of true protective effect and this inhibition causes an increase in tumor cell clonogenic growth after drug treatment. In most of the examples cited above, this appears as a starking effect, as the whole debate is about the drug induced autophagy and in response to which the cells die (or cells found dead). This novel approach emerged as an important point because a recent study also supports this myth that rapamycin-induced autophagy can protect various tumor cell lines against apoptosis induced by general apoptotic stimuli [75] and may have a similar effect on the action of anticancer agents. Moreover, similar to etoposide [74], it has been observed that knockdown of Atg genes does confer a clonogenic survival advantage to cells after treating with anticancer agents and the used cells have profound defects in their apoptosis machinery [73,74].
Representative natural compounds (Resveratrol, Oridonin, Curcumin, and Evodiamine) targeting autophagic pathways.
It is generally believed that the complex two-faced nature of autophagy in tumor cell survival versus death may help in determining cancer therapeutic potential. So inhibiting autophagy may enhance anti-cancer drugs efficacy fairly used in chemo- and radiotherapy-induced activation of autophagic signaling pathways and which may augment anti-tumor activity, and thus efficacy of radiation and/or anti-cancer drugs. We are still at the initial stages of understanding the complex interplay of autophagy and cancer, but it is incontrovertible that autophagy is deeply integrated into metabolism, stress response and cell-death pathways [64]. Preliminary evidences, in addition to some natural compounds that induced autophagic cell death, support the idea that natural compounds-induced autophagy enhances tumor cell survival. Anticancer agents that can be involved in the induction of autophagy include tamoxifen, arsenic trioxide, rapamycin, histone deacetylase inhibitors, temozolomide, ionizing radiation [63], vitamin D analogues [76], and etoposide [74]. In addition, several natural compounds, (curcumin, resveratrol, evodiamine, oridonin, and magnolol) in our natural compounds libraries screen for autophagy inducer, were found to be involved in autophagy. However, despite the above examples, is autophagy really an important cell death mechanism? is highly controversial.
Controversy remains as whether autophagy limits or promotes tumor malignancy, till genetic inactivation of autophagy, is found to promote tumorigenesis constituting a new category of tumor suppressors including Beclin 1. Some of the oncogenes including PI3K/AKT/mTOR and Bcl-2 inhibit autophagy causing tumor cells proliferation, while the other oncogenes including Ras and myc stimulate autophagy [63]. The significance of autophagy at different stages of tumor progression can be evaluated considering these kaleidoscopic effects. Further investigations on natural compounds into the impact of autophagy inactivation are warranted. All of the above data draw many questions in autophagy mechanistic pool focusing whether autophagy is really an important mechanism of tumor cell killing by anticancer agents in cells having ability to undergo apoptosis. Rigorous examination also manifest the speculation whether bona-fide cancer drugs are actually capable of killing tumor cells via autophagy, is needed. To answer these questions is the need of the hour, as it may determine the route causes and may best streamline the contradictory approaches in developing effective combination therapies by regulating autophagy along with anticancer agents. In conclusion, we now have sound justifications to visualize that manipulation of autophagy may provide a useful way to prevent cancer development, limit tumor progression, and increase the efficacy of cancer treatments. This comprehension seems reasonable due to the fact that drugs induce autophagy, such as rapamycin (as discussed above), and is rapidly gaining a better understanding of how this process works based on the effects of targeted inactivation of autophagy regulators in mouse models and human tumor cells. More contradictory messages come when we consider how autophagy affects the ways by which the tumor cells die when we treat them with anticancer agents. Over the last several decades the therapeutic use of natural compounds that induce autophagy has been leading us to the implications that autophagic cell death may be a vital mechanism of tumor cell killing by these agents.
Accumulated lines of evidence have recently revealed that targeting autophagic signaling pathways may be a promising avenue for potential therapeutic purposes. Although this chapter has focused on natural compounds and their role in autophagic cell signaling pathways, future studies investigating the mechanisms of natural compounds-induced autophagy and their role in cancer cell death. Progress towards better treatment and understanding by natural compounds may be made by further examining the role of natural compounds and crosstalk between the apoptosis and the autophagy. Despite these obstacles, many compounds bring the hope that with sufficient modification by tools of structural biology and combinatorial chemistry, it might be possible to derive sufficiently potent drugs to target core autophagy pathways, and even autophagic networks in cancer cells, rather than their individual gene or protein components. Indeed, as discussed above, the generally used cancer therapeutics, especially natural compounds abolish tumors by inducing apoptosis and autophagy. On the other hand, a better but growing setting approach is required to make a distinction between the survival-supporting and death-promoting roles of autophagy. Furthermore, for selectivity and specificity, role of autophagy, along with the elucidation of the signaling pathways those confer the autophagic response downstream of different stimuli and activate the specific and therapeutic response, is desired.. In the end we have coherent arguments in favor of principal paradigm that disease-associated autophagy could be selectively targeted for therapeutics.
The recent developments in thin films and nanofabrication techniques of biosensors and related spintronic devices are the forefront of current research efforts, bridging material sciences, physics, chemistry, and engineering, to form a seamless integration of digital world into the soft or living systems. Magnetic functionalities may provide a sense of proximity, orientation, or displacement to this novel formulation of biomedical electronics.
High spin polarization is one of the requested and necessary properties of materials used as electrodes or spin pumping/spin analyzers elements in spintronics, including those used in medicine and this is by definition a characteristic of alloys with half-metallic properties [1, 2]. The property of half-metallic ferromagnetism initially discovered in Cu2MnAl compound [2] consists in a metallic behavior of one spin channel of electronic structure and a semiconducting one in the other, thus creating a material with hybrid properties between metals and semiconductors. As a direct consequence, there will be always a 100% net spin polarization at the Fermi level due to the unique spin polarization of electrons in only one channel.
In materials in which the unit cell consists of two distinct sublattices with antiferromagnetic coupling between them, an internal spin partial compensation occurs and this particular property was referred as half-metallic ferrimagnetism [3, 4], which comparing to half-metallic ferromagnetism exhibits lower magnetic moments per formula unit (f.u) and weaker stray fields. Moreover, if the magnetic moments of the constituent sublattices fully compensate each other (with a net spin = 0 μB/f.u.), an alloy with a completely compensated ferrimagnetism (CCF) [5] resulted and the compound was classified as half-metallic completely compensated ferrimagnet (HM-CCFs) [6]. However, such a complete spin polarization of carriers occurs in the case of zero temperature and only in the absence of the spin-orbit interactions. Apart from this, HM-CCFs are intensively studied to develop new stable spin-polarized electrodes for biomedical in-vivo applications, junctions or integrated spin-transfer torque nano-oscillators for telecommunication.
A particular class of half-metallic materials is Spin Gapless Semiconductors (SGS). These compounds exhibit around Fermi level, in one spin channel a typical semiconducting band gap, while in the other (where in usual half-metallic compounds a metallic character is present), the negligible density of states are equivalent to a very narrow almost zero band gap. The above described characteristic of electronic structure, places SGSs at the boundary between half-metallic compounds and semiconductors.
In this particular case of half-metallicity, the materials act like topological insulators, where in particular high Curie temperature may coexist with high resistance. A combination of spin gapless semiconducting properties with completely compensated ferrimagnetism (0 μB total magnetic moment per f.u.) leads to spin gapless completely compensated ferrimagnetism (SG-CCF) [7].
Particularly, attractive classes of alloys exhibiting half-metallic properties, based on which may be developed biosensors, the new electrode materials with high spin polarization include alloys like Heusler compounds [2]. This class of materials, used in present as electrodes for magnetic tunnel junctions were discovered by Fritz Heusler, in 1903, who reported that Cu2MnAl alloy is ferromagnetic, even though, alone, none of constituent elements has magnetic properties [8]. These intermetallic alloys are described by two variants: the half-Heusler XYZ compounds, with C1b crystal structure and the full-Heusler X2YZ variants which typically crystallize in Cu2MnAl (cubic L21)-type structure; where X is a transition metal, Y may be a rare-metal or a transition metal, and Z is a main group element. Recently, it has been shown that in case of a full-Heusler compounds X2YZ, if the Y element is more electronegative than X, a structure with Hg2CuTi-prototype is observed. This is the so called as inverse Heusler structure, crystallizing in F43m space group [9], with X atoms placed in the 4a(0,0,0) and 4c(1/4,1/4,1/4) Wyckoff positions, Y in 4b(1/2,1/2,1/2) and Z in 4d(3/4,3/4,3/4), respectively. In this crystal structure, no octahedral symmetry Oh is adopted, and all atoms have tetrahedral symmetry Td.
The Slater-Pauling curve gives the interrelation between the total magnetic moment and the valence electron concentration in ferromagnetic/ferrimagnetic alloys [10, 11]. The original Slater-Pauling approach suggests the existence of different laws, due to the average over all atoms of the total magnetic moment and the number of valence electrons. For compounds with different kinds of atoms and ordered crystalline structures, it is more appropriate to consider all atoms of the unit cell, to find the magnetic moment per unit cell.
In terms of two-orbital two-electron stabilizing interactions, within the framework of density functional theory, the states of each spin channel are occupied according to several aspects concerning ionic arguments, crystal structure of primitive cell, lattice parameter, approximations made for the exchange and correlation interaction, energy threshold set between the core and valence states, and also Brillouin zone integration mesh. Based on ionic arguments, the most electropositive element transfers the valence electrons to the most electronegative element. The purpose is to obtain stable closed shell ions. In addition, strongly dependent by the atomic arrangement of atoms and environment, hybridization occurs whenever the sum of metallic radii (12-coordinated) of two first-neighbors exceeds the interatomic distance.
A particularly useful measure to describe the electronic properties of a material is the electron spin polarization P at Fermi level (
where
For ternary 1:1:1 Heusler compounds, the Slater-Pauling rule was firstly reported by Kübler [12]. These compounds, with C1b structure have three atoms per unit cell and follow the Slater-Pauling 18-electron-rule (Mt = Zt - 18), where Mt is the total magnetic moment per the formula unit, Zt is the total number of valence electrons, and 18 represents the number of occupied states in the spin bands. A Slater-Pauling 24-electron-rule (Mt = Zt - 24) was found for the 2:1:1 family of full-Heusler compounds with L21 structure (Cu2MnAl-prototype) [13]. The present work deals only with ternary 2:1:1 full-Heusler compounds with Hg2CuTi type structure. Even though the origin of the band gap in the latter 2:1:1 full-Heusler compounds is different than that of the ternary 1:1:1 Heusler compounds, the corresponding Slater-Pauling rule is similar: 18-electron-rule (Mt = Zt - 18). This Slater-Pauling 18-electron-rule was recently explained for Ti2-based full-Heusler compounds [4, 14].
Many Co2, Mn2, Ti2, and Sc2 – Heusler compounds reported in literature are ferromagnetic [15, 16, 17, 18], ferrimagnetic half-metals [19], or spin gapless semiconductors [20]. Among them, Mn2CoAl full-Heusler compound crystallizing in Hg2CuTi-prototype was extensively studied: theoretically investigated, the structure was experimentally verified by XRD and the electron transport characteristics where obtained by a Physical Properties Measurement System (PPMS) on samples cut from ingots. The total magnetic moment was experimentally measured using a Magnetic Properties Measurement System (MPMS) [20]. Zirconium has a Pauling electronegativity value lower than those of all d-elements and hence Zr-based Heusler materials are supposed to crystallize in Hg2CuTi type structure, similar to Mn2CoAl.
Zirconium-based Heusler compounds were selected because they exhibit low toxicity and are corrosion resistant, being therefore susceptible of convenient preparation and processing in the field of electronic biomedical sensors ranging from healthcare and medical diagnosis, food safety, and environmental monitoring to life science research.
The information about the experimental preparation and electronic structure of Zr-based Heusler compounds with true half-metallic properties are still scarce. Therefore, to understand the properties of potential zirconium-based Heusler compounds, in the beginning, theoretical investigations can be performed via density functional theory (DFT). Self-consistent calculations using a “muffin-tin” model and various approximations to describe the exchange and correlation interactions can lead to valuable information about the energetically favorable crystalline structure, electronic configuration, or magnetic properties by means of the total energy minimization.
This chapter gives a comprehensive overview of the key electronic structures and magnetic properties usually found in half-metallic zirconium-based full-Heusler compounds.
The cubic crystal structure of full-Heusler Zr2YZ variants exhibits two magnetic sublattices, coupled to each other. Thus, the two Zr atoms are located in tetrahedral lattice sites and interact to each other. In addition, Zr and Y atoms form a second and more delocalized magnetic sublattice. Therefore, ferrimagnetic interaction between the Zr and Y atoms is frequently reported phenomena.
The total spin-polarized density of states of a typical half metallic ferrimagnetic material exhibits in the spin-up channel a semiconducting band gap while in the spin-down channel a metallic behavior. A relevant example is illustrated in Figure 1 for Zr2CrAl (unpublished results). The main contribution to the total density of states from spin-down channel comes from transition metal constituent elements, and these results are consistent with other published information [21].
Partial and total density of states (PDOS and TDOS) of half-metallic ferrimagnetic Heusler compound, Zr2CrAl at optimized lattice parameter.
Desirable candidates for magnetoelectronic devices, half-metallic ferrimagnetic compounds provide an unequivocal advantage over their ferromagnetic counterparts by reduction of the magnetic moment due to the ferrimagnetic interaction resulted from compensation of partial magnetic moments of the two different magnetic sublattices. This phenomenon is illustrated in Figure 2 (unpublished results) for the Zr2CrAl compound, where one can notice the magnetic moment of Cr atoms, partially compensated by magnetic moments of Zr located in the two different sublattices and having different neighborhoods. Similar DFT outcome were reported for Zr2YZ (Y = Cr, V, Z = Al, Ga, In, Pb, Sn, Tl) [21, 22, 23, 24].
Partial and total magnetic moments in Zr2CrAl Heusler compound.
Figure 3 (unpublished results) exhibits the position of the Fermi level and the width of the energy gap in spin-up channel as function of the lattice parameter. According to theoretical investigations, the Zr2CrAl compound is a potential ideal candidate for spintronics, due to the presence of a steady energy gap in only one spin channel, for a large lattice parameter range.
The positions of the highest occupied states from the valence band (solid rhombs) and of the lowest unoccupied states from the conduction band (solid stars) of total DOSs (spin-up channel) for Zr2CrAl as function of the lattice parameter.
Table 1 summarizes the published results regarding Zr2CrZ (Z = Al, Ga, In) [21, 22]. As can be seen, the energy band gap (Eg) from spin-up channel increases as the atomic radii of Z elements increase. The ferrimagnetic interaction occurs between the zirconium atoms from both sublattice and the chromium ones, phenomena which are reflected by the opposite sign of the partial magnetic moments of Zr and Cr atoms. The total magnetic moment per f.u. for all compounds strictly follow the Slater Pauling rule described earlier.
Alloy | a (Å) | μZr(4a) (μB/atom) | μZr(4c) (μB/atom) | μY(4b) (μB/atom) | μZ(4d) (μB/atom) | μt (μB/f.u.) | Eg (eV) |
---|---|---|---|---|---|---|---|
Zr2CrAl | 6.59b | −0.955b | −0.768b | 2.835b | −0.110b | 1.000b | 0.452b |
Zr2CrGa | 6.635a | 0.849a | 0.702a | −2.591a | 0.049a | −1.000a | 0.629a |
6.622b | −1.011b | −0.914b | 2.994b | −0.068b | 1.000b | 0.512b | |
Zr2CrIn | 6.875a | 1.016a | 0.859a | −2.930a | 0.034a | −1.000a | 0.673a |
6.812b | −1.213b | −1.080b | 3.343b | −0.049b | 1.000b | 0.615b |
In the ideal case of a fully compensated magnetic moment, a half-metallic ferromagnetic material would be obtained, useful to be applied in a junction device as a stable spin-polarized electrode based on spin-transfer effect.
The theoretical results from in literature for Zr2VZ (Z = Al, Ga, In, Si, Ge, Sn, Pb) [23, 24] report that the most energetically favorable crystalline structure comparing with the Hg2CuTi structure has the prototype Cu2MnAl and in this configuration the materials do not present half-metallic properties. However, the Hg2CuTi type structure can be synthesized experimentally due to the negative entropy of formation. In the inverse Heusler crystalline structure, the Zr2VZ exhibits half metallic ferrimagnetic characteristics, the partial magnetic moment of Vanadium being opposite to the one of zirconium atoms.
Particular cases of half-metallic ferromagnetic materials are the spin gapless semiconductors, where a semiconducting band gap is formed in one spin channel and a pseudo-band gap in the other one. Such a pseudo band gap is often called zero or closed band gap because the maximum energy of the valence band is very close to the minimum energy of the conduction band. The Zr2MnAl compound presents a typical behavior of spin gapless semiconductors and may allow a tunable spin transport (see Figure 4). The Fermi level, located at 0.04 eV below the conduction band minimum, in case of Zr2MnAl, falls into a typical spin gapless semiconducting band gap of 0.41 eV in spin-up channel, according to Ref [25]. In the spin-down channel, a zero band gap is reported around the Fermi level. In both spin channels, the significant contribution to density of states between −4.5 and −1.5 eV comes from the 3d electrons of Mn, while the 4d electrons from Zr atoms have contribution only above the Fermi level.
Partial and total density of states (PDOS and TDOS) of spin gapless semiconductor Zr2MnAl at equilibrium lattice parameter.
Figure 5 presents the contribution of double and triple degenerated states (deg and dt2g, respectively) of Zr and Mn atoms, calculated around the Fermi level, at optimized lattice parameters. In Zr2MnAl compound, the highest bonding states from valence band, below the EF, belong to triple degenerated states of manganese dt2g, while the lowest anti-bonding states from conduction band come from the triple degenerated states dt2g of Zr1, Zr2, and Mn. As a result, the energy gap from spin-up channel results due to Zr-Mn hybridization. The Zr2MnAl alloy presents an indirect band gap of 0.41 eV, in the spin up channel with the higher bonding states from valence band located in the Δ point and the lowest anti-bonding states from the conduction band, distributed in the Δ and W high symmetry points of Brillouin zone.
The densities of states of double and triple degenerated states of Zr and Mn atoms, around the Fermi level, calculated at optimized lattice parameters for Zr2MnAl. The Fermi level, deg and dt2g, are illustrated with black dotted, red dashed, and blue solid line, respectively.
It is obvious that the change in the lattice parameter affects the presence of the zero band gap from spin channel and the width of the semiconducting band gap. In Zr2MnAl alloy, the band gap increases initially by increasing the lattice parameter. The largest band gap is obtained for a lattice parameter of 6.6 Å, which corresponds to a volume increase of 2%. Above the lattice parameter of 6.6 Å, the spin gapless semiconducting properties of Zr2MnAl compound disappear, due to the shifts of the Fermi level in to the conduction band. The width of the energy band gap from spin-up channel decreases as illustrated in Figure 6.
The positions of the highest occupied states from the valence band (solid rhombs) and of the lowest unoccupied states from the conduction band (solid stars) of total DOSs (spin-down channel) for Zr2MnAl as function of the lattice parameter.
The spin gapless semiconductors may present a finite total magnetic moment; however in the particular case, when a perfectly compensated ferrimagnetism appears the total magnetic moment of compound equals zero and the alloy becomes a spin gapless completely compensated ferrimagnet, like Zr2MnAl (see Figure 7).
Total magnetic moments in spin gapless semiconductor Zr2MnAl.
Surprisingly, the zirconium element which does not exhibit natively magnetic properties shows magnetic behavior. A ferrimagnetic interaction occurs between the magnetic moments of Zr and Mn atoms, whereas the zirconium atoms, located in different Wyckoff positions, are coupled ferromagnetically. The magnetic moments of manganese increase with the lattice parameter, in all compounds. The magnetic moments of zirconium atoms coupled ferromagnetically decrease with the lattice parameter increase and compensate the magnetic moment of Mn atoms. The main element Al does not carry significant magnetic moments, but non-negligible contribution to the magnetic moment comes from conduction electrons.
Antiferromagnetic “ab initio” results were reported for Zr2MnZ (Z = A, Ga) [26, 27, 28] and were gathered in Table 2. For Zr2MnAl, the band gap is slightly increased from 0.41 eV for ferromagnetic calculation to 0.48 eV to antiferromagnetic results. However, the semiconducting band gap from spin-down channel decreases when the atomic radius of the main element increases (when Ga replaces Al). Due to the different magnetic ordering structures, having the spin moments of manganese antiparallel (antiferromagnetic configuration) or parallel (ferromagnetic configuration) oriented, the sign of partial magnetic moments from Table 2, differs. However, the opposite spin orientation is clearly explaining the ferrimagnetic interaction between the Mn and Zr atoms and the ferromagnetic coupling between the Zr atoms located in the two distinct sublattice. The total magnetic moment per f.u. calculated in both magnetic configurations is fully compensated by partial magnetic moments of constituents and follow the Slater Pauling curve for typical for half-metals.
Alloy | a (A) | μZr(4a) (μB/atom) | μZr(4c) (μB/atom) | μY(4b) (μB/atom) | μZ(4d) (μB/atom) | μt (μB/f.u.) | Eg (eV) |
---|---|---|---|---|---|---|---|
Zr2MnAl | 6.56a | −0.77a | −0.69a | 2.44a | −0.04a | 0.00a | 0.41a |
6.64b,* | 1.74b,* | 1.50b,* | −3.26b,* | 0.02b,* | 0.00b,* | ||
6.968d,* | 1.47d,* | 1.35d,* | −4.33d,* | 0.088d,* | 0.00d,* | 0.48d | |
Zr2MnGa | 6.59c,* | 1.66c,* | 1.52c,* | −3.08c,* | −0.10c,* | 0.00c,* | |
6.935e | −1.48e | −1.42e | 4.34e | −0.030e | 0.00e | 0.31e |
Ferromagnetic zirconium-based half-metallic Heusler compounds represent another category of materials of specific interest in biomedical spintronic applications where a good response to an external magnetic moment is required and that is mainly related to their large total magnetic moment. From theoretical point of view, the materials which exhibit a metallic character in the majority density of states and a band gap in the minority one, around the Fermi level and the metallic total density of states resulted from summation of partial density of states of all elements are classified as half-metallic ferromagnets.
A typical example of density of states for a half-metallic ferromagnet is exemplified in case of Zr2CoAl [30, 31, 32, 33, 34] (see Figure 8). In the majority channel, the significant contribution to density of states comes from the zirconium, located in the origin of unit cell and the cobalt atom. The band gap from minority channel (Figure 9) is formed between the 3d t2g electrons of Co and the 4d t2g unoccupied electrons of Zr located in origin and 4d t2g occupied Zr electrons locate in the 4c Wyckoff position of Hg2CuTi prototype structure. This type of hybridization between the Y element and the two X atoms of a X2YZ Heusler compounds is often reported for half-metallic ferromagnets.
Partial and total density of states (PDOS, TDOS) of half-metallic ferromagnetic Heusler compound, Zr2CoAl, at optimized lattice parameter.
The band structure of Zr2CoAl for majority and minority spin channel, in the right and left panel, respectively, at equilibrium lattice parameter.
In general, the half metallic ferromagnetic properties characterized by the presence of a semiconducting band gap in the minority spin channel of density of states continue to be maintained for a large enough range of lattice parameter in order to be stable from experimental point of view. This means that even if the unit cell volume increases or decreases the material would present a high spin polarization typical for half metallic materials. In case of Zr2CoAl, the transition from metal behavior to half metallic characteristic occurs at a 6.43 A lattice parameter, and it remains stable at experimentally achievable increases of unit cell volume (Figure 10) [30, 31, 32, 33, 34]. By definition, in the case of a ferromagnetic material, a net magnetization may be measurable because even if the majority and minority density of states is identical and equally occupied; these are shifted against each other. The total magnetic moment is obtained by adding the partial magnetic moments of constituent elements as presented in Figure 11.
The positions of highest bonding states from the valence band (solid purple rhombs) and of lowest anti-bonding states from conduction band (solid magenta stars) of total DOSs for Zr2CoAl as function of lattice constants.
The partial and total magnetic moments as a function of lattice constant for half-metallic ferromagnetic Zr2CoAl Heusler compound.
Table 3 overviews the state of the art ferromagnetic zirconium-based Heusler compounds. Most alloys incorporate cobalt, and the main elements carry an irrelevant partial magnetic moment. However, the influence of main elements over the energy band gap from spin-down channel is significant. The average width of band gap from spin-down channel is large enough to provide stable half-metallic characteristics for a large deformation of the unit cell. All results gathered in Table 3 are obtained based on density functional theory calculations, and these are influenced by the pseudo-potential used for electron-ionic core interaction. This is the reason for various reported band gaps of such compounds, as for example, the band gap reported by Ref [32] which is lower than the other published results. In all compounds, the ferromagnetic interaction between constituent atoms is represented by similar signs of the partial magnetic moments. The total magnetic moments, following Slater-Pauling curve, are higher than for ferromagnetic half-metallic compounds, and as consequence, the compounds may present a better response to an external magnetic field. Theoretical results regarding zirconium-based half-metallic compounds containing nickel provide information about electronic structures and magnetic properties in alloys with Al and Ga. These intermetallic compounds theoretically behave like half-metals from the electronic structure point of view; however their reported total magnetic moments do not follow the Slater Pauling curve. In addition, the band gap from spin-down channel is significant lower than for compounds incorporating cobalt.
Alloy | a (Å) | μZr(4a) (μB/atom) | μZr(4c) (μB/atom) | μY(4b) (μB/atom) | μZ(4d) (μB/atom) | μt (μB/f.u.) | Eg (eV) |
---|---|---|---|---|---|---|---|
Zr2CoAl | 6.54 | 0.757a | 0.54a | 2.00a | 0.48a | ||
6.575i | 1.211i | 0.303i | 0.538i | −0.053i | 2.000i | 0.518i | |
6.59c | 1.34c | 0.36c | 0.4c | −0.1c | 2.00c | 0.6046c | |
6.523d | 1.088d | 0.442d | 0.553d | 0.002d | 2.00d | 0.300d | |
6.575e | 1.21e | 0.3e | 0.54e | −0.05e | 2.00e | 0.518e | |
6.539f | 0.725f | 0.262f | 0.587f | 0.011f | 2.00f | 0.5905f | |
Zr2CoGa | 6.62c | 1.30c | 0.52c | 0.34c | −0.16c | 2.00c | 0.6990c |
6.593i | 1.162i | 0.402i | 0.505i | −0.070i | 2.000i | 0.533i | |
6.509d | 1.074d | 0.526d | 0.522d | 0.013d | 2.00d | 0.353d | |
6.520f | 0.714f | 0.332f | 0.518f | −0.001f | 2.00f | 0.6546f | |
Zr2CoIn | 6.75c | 1.34c | 0.62c | 0.2c | −0.16c | 2.00c | 0.7013c |
6.627i | 1.215i | 0.455i | 0.417i | −0.089i | 2.000i | 0.576i | |
6.714d | 1.085d | 0.581d | 0.427d | 0.011d | 2.00d | 0.268d | |
6.726f | 0.722f | 0.3630f | 0.429f | −0.002f | 1.999f | 0.6580f | |
Zr2CoSi | 6.68c | 1.59c | 0.58c | 1.0c | −0.08c | 3.00c | 0.8419c |
Zr2CoGe | 6.70c | 1.65c | 0.65c | 0.86c | −0.16c | 3.00c | 0.8365c |
Zr2CoSn | 6.76b | 0.946b | 0.446b | 0.8106b | −0.013b | 3.00b | 0543b |
6.790i | 1.625i | 0.605i | 0.829i | −0.060i | 3.000i | 0.614i | |
6.81c | 1.70c | 0.68c | 0.78c | −0.16c | 3.00c | 0.8537c | |
6.745d | 1.429d | 0.746d | 0.858d | 0.044d | 2.998d | 0.406d | |
6.745g | 1.429g | 0.746g | 0.858g | 0.044g | 3.000g | 0.65g | |
Zr2CoPb | 6.86c | 1.72c | 0.76c | −0.16c | −0.24c | 3.00c | 0.58c |
Zr2NiAl | 6.60h | 1.02h | 0.98h | 0.61h | 0.15h | 2.87h | 0.44h |
Zr2NiGa | 6.58h | 1.06h | 0.81h | 0.58h | 0.21h | 2.86h | 0.50h |
The individualized medicine and high precise diagnosis can benefit from the development of smart biosensors based on magnetic functionalities. Foreseeable applications of zirconium-based biosensors with half metallic character include the capability to measure, sense, or respond to magnetic stimuli desirable for in vivo sensitive detection of markers for diseases.
This chapter overviewed the recent advances of zirconium-based full-Heusler compounds from the point of view of electronic structure and magnetic properties. The representative materials described in this chapter obviously were selected to offer significant information to emphasis the certain differences in magnetic features: half-metallic ferrimagnetism, spin-gapless semiconducting, and half-metallic ferromagnetism. Based on this, the Y elements of Zr2YZ were selected from the most commonly used transition metals (Cr, Mn, and Co), while the Z element was identical in all compounds (Al). The purpose was to underline the influence of d electrons of Y elements and hybridization interaction between the electrons of zirconium and Y atoms over the macroscopic magnetic properties.
Furthermore, the theoretical and experimental advances in designing and fabrication technology engage the construction of innovative materials to be integrated in biosensors with significant high throughput able to reform the biomedical field.
We acknowledge the fruitful discussions with Dr. P. Palade. This work was supported by grants of the Romanian Ministry of Research and Innovation, CCCDI – UEFISCDI, project number PN-III-P1-1.2-PCCDI-2017-0062 contract no 58 and project number PN-III-P1-1.2-PCCDI-2017-0871 contract no 47 as well as by the core program at NIMP.
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