Publications
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Anisotropic Thermal Conductivity of Crystalline Layered SnSe2
Xiao P., Chavez-Angel E., Chaitoglou S., Sledzinska M., Dimoulas A., Sotomayor Torres C.M., El Sachat A. Nano Letters; 21 (21): 9172 - 9179. 2021. 10.1021/acs.nanolett.1c03018. IF: 11.189
The degree of thermal anisotropy affects critically key device-relevant properties of layered two-dimensional materials. Here, we systematically study the in-plane and cross-plane thermal conductivity of crystalline SnSe2 films of varying thickness (16-190 nm) and uncover a thickness-independent thermal conductivity anisotropy ratio of about ∼8.4. Experimental data obtained using Raman thermometry and frequency domain thermoreflectance showed that the in-plane and cross-plane thermal conductivities monotonically decrease by a factor of 2.5 with decreasing film thickness compared to the bulk values. Moreover, we find that the temperature-dependence of the in-plane component gradually decreases as the film becomes thinner, and in the range from 300 to 473 K it drops by more than a factor of 2. Using the mean free path reconstruction method, we found that phonons with MFP ranging from ∼1 to 53 and from 1 to 30 nm contribute to 50% of the total in-plane and cross-plane thermal conductivity, respectively. © 2021 The Authors. Published by American Chemical Society.
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Antibacterial activity testing methods for hydrophobic patterned surfaces
Perez-Gavilan A., de Castro J.V., Arana A., Merino S., Retolaza A., Alves S.A., Francone A., Kehagias N., Sotomayor-Torres C.M., Cocina D., Mortera R., Crapanzano S., Pelegrín C.J., Garrigos M.C., Jiménez A., Galindo B., Araque M.C., Dykeman D., Neves N.M., Marimón J.M. Scientific Reports; 11 (1, 6675) 2021. 10.1038/s41598-021-85995-9. IF: 4.380
One strategy to decrease the incidence of hospital-acquired infections is to avoid the survival of pathogens in the environment by the development of surfaces with antimicrobial activity. To study the antibacterial behaviour of active surfaces, different approaches have been developed of which ISO 22916 is the standard. To assess the performance of different testing methodologies to analyse the antibacterial activity of hydrophobic surface patterned plastics as part of a Horizon 2020 European research project. Four different testing methods were used to study the antibacterial activity of a patterned film, including the ISO 22916 standard, the immersion method, the touch-transfer inoculation method, and the swab inoculation method, this latter developed specifically for this project. The non-realistic test conditions of the ISO 22916 standard showed this method to be non-appropriate in the study of hydrophobic patterned surfaces. The immersion method also showed no differences between patterned films and smooth controls due to the lack of attachment of testing bacteria on both surfaces. The antibacterial activity of films could be demonstrated by the touch-transfer and the swab inoculation methods, that more precisely mimicked the way of high-touch surfaces contamination, and showed to be the best methodologies to test the antibacterial activity of patterned hydrophobic surfaces. A new ISO standard would be desirable as the reference method to study the antibacterial behaviour of patterned surfaces. © 2021, The Author(s).
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Construction of 0D/2D composites heterostructured of CdTe QDs/ZnO hybrid layers to improve environmental remediation by a direct Z-scheme
Alegría M., Aliaga J., Jofré P., Ballesteros L., Guzmán D., Sotomayor-Torres C., González G., Benavente E. Catalysis Communications; 159 (106352) 2021. 10.1016/j.catcom.2021.106352. IF: 3.626
Layered hybrid ZnO (2D) intercalated by myristic acid (MA) with (0D) CdTe quantum dots (QDs) was designed to increase the conversion efficiency of photochemical energy. The results showed that the introduction of CdTe QDs in ZnO(MA) layered with more active sites available enhanced the photocatalytic efficiency. The optimal composite sample ZnO(MA)/CdTe (1:0.02) showed excellent dye removal efficiency under simulated solar light irradiation, above 96% after three cyclic experiments. The correlation coefficients possessed the highest reaction rate. This study offers an efficient research approach and vision to support the development of other photocatalytic systems featuring a direct Z scheme. © 2021 The Authors
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Electron beam lithography for direct patterning of MoS2on PDMS substrates
Jumbert G., Placidi M., Alzina F., Sotomayor Torres C.M., Sledzinska M. RSC Advances; 11 (32): 19908 - 19913. 2021. 10.1039/d1ra00885d. IF: 3.361
Precise patterning of 2D materials into micro- and nanostructures presents a considerable challenge and many efforts are dedicated to the development of processes alternative to the standard lithography. In this work we show a fabrication technique based on direct electron beam lithography (EBL) on MoS2on polydimethylsiloxane (PDMS) substrates. This easy and fast method takes advantage of the interaction of the electron beam with the PDMS, which at high enough doses leads to cross-linking and shrinking of the polymer. At the same time, the adhesion of MoS2to PDMS is enhanced in the exposed regions. The EBL acceleration voltages and doses are optimized in order to fabricate well-defined microstructures, which can be subsequently transferred to either a flexible or a rigid substrate, to obtain the negative of the exposed image. The reported procedure greatly simplifies the fabrication process and reduces the number of steps compared to standard lithography and etching. As no additional polymer, such as polymethyl methacrylate (PMMA) or photoresists, are used during the whole process the resulting samples are free of residues. © The Royal Society of Chemistry 2021.
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Fabrication and characterization of large-area suspended MoSe2 crystals down to the monolayer
Varghese S., Reig D.S., Mehew J.D., Block A., El Sachat A., Chávez-Ángel E., Sledzinska M., Ballesteros B., Sotomayor Torres C.M., Tielrooij K.-J. JPhys Materials; 4 (4, 046001) 2021. 10.1088/2515-7639/ac2060. IF: 0.000
Many layered materials, such as graphene and transition metal dichalcogenides, can be exfoliated down to atomic or molecular monolayers. These materials exhibit exciting material properties that can be exploited for several promising device concepts. Thinner materials lead to an increased surface-to-volume ratio, with mono- and bi-layers being basically pure surfaces. Thin crystals containing more than two layers also often behave as an all-surface material, depending on the physical property of interest. As a result, flakes of layered materials are typically highly sensitive to their environment, which is undesirable for a broad range of studies and potential devices. Material systems based on suspended flakes overcome this issue, yet often require complex fabrication procedures. Here, we demonstrate the relatively straightforward fabrication of exfoliated MoSe2 flakes down to the monolayer, suspended over unprecedentedly large holes with a diameter of 15 µm. We describe our fabrication methods in detail, present characterization measurements of the fabricated structures, and, finally, exploit these suspended flakes for accurate optical absorption measurements. © 2021 The Author(s).
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Heat transport control and thermal characterization of low-dimensional materials: A review
El Sachat A., Alzina F., Sotomayor Torres C.M., Chavez-Angel E. Nanomaterials; 11 (1, 175): 1 - 32. 2021. 10.3390/nano11010175. IF: 5.076
Heat dissipation and thermal management are central challenges in various areas of science and technology and are critical issues for the majority of nanoelectronic devices. In this review, we focus on experimental advances in thermal characterization and phonon engineering that have drastically increased the understanding of heat transport and demonstrated efficient ways to control heat propagation in nanomaterials. We summarize the latest device-relevant methodologies of phonon engineering in semiconductor nanostructures and 2D materials, including graphene and transition metal dichalcogenides. Then, we review recent advances in thermal characterization techniques, and discuss their main challenges and limitations. © 2021 by the authors. Licensee MDPI, Basel, Switzerland.
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Impact of surface topography on the bacterial attachment to micro- and nano-patterned polymer films
Francone A., Merino S., Retolaza A., Ramiro J., Alves S.A., de Castro J.V., Neves N.M., Arana A., Marimon J.M., Torres C.M.S., Kehagias N. Surfaces and Interfaces; 27 (101494) 2021. 10.1016/j.surfin.2021.101494. IF: 4.837
The development of antimicrobial surfaces has become a high priority in recent times. There are two ongoing worldwide health crises: the COVID-19 pandemic provoked by the SARS-CoV-2 virus and the antibiotic-resistant diseases provoked by bacteria resistant to antibiotic-based treatments. The need for antimicrobial surfaces against bacteria and virus is a common factor to both crises. Most extended strategies to prevent bacterial associated infections rely on chemical based-approaches based on surface coatings or biocide encapsulated agents that release chemical agents. A critical limitation of these chemistry-based strategies is their limited effectiveness in time while grows the concerns about the long-term toxicity on human beings and environment pollution. An alternative strategy to prevent bacterial attachment consists in the introduction of physical modification to the surface. Pursuing this chemistry-independent strategy, we present a fabrication process of surface topographies [one-level (micro, nano) and hierarchical (micro+nano) structures] in polypropylene (PP) substrates and discuss how wettability, topography and patterns size influence on its antibacterial properties. Using nanoimprint lithography as patterning technique, we report as best results 82 and 86% reduction in the bacterial attachment of E. coli and S. aureus for hierarchically patterned samples compared to unpatterned reference surfaces. Furthermore, we benchmark the mechanical properties of the patterned PP surfaces against commercially available antimicrobial films and provide evidence for the patterned PP films to be suitable candidates for use as antibacterial functional surfaces in a hospital environment. © 2021
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Injection locking in an optomechanical coherent phonon source
Arregui G., Colombano M.F., Maire J., Pitanti A., Capuj N.E., Griol A., Martínez A., Sotomayor-Torres C.M., Navarro-Urrios D. Nanophotonics; 10 (2): 1319 - 1327. 2021. 10.1515/nanoph-2020-0592. IF: 8.449
Spontaneous locking of the phase of a coherent phonon source to an external reference is demonstrated in a deeply sideband-unresolved optomechanical system. The high-amplitude mechanical oscillations are driven by the anharmonic modulation of the radiation pressure force that result from an absorption-mediated free-carrier/temperature limit cycle, i.e., self-pulsing. Synchronization is observed when the pump laser driving the mechanical oscillator to a self-sustained state is modulated by a radiofrequency tone. We employ a pump-probe phonon detection scheme based on an independent optical cavity to observe only the mechanical oscillator dynamics. The lock range of the oscillation frequency, i.e., the Arnold tongue, is experimentally determined over a range of external reference strengths, evidencing the possibility to tune the oscillator frequency for a range up to 350 kHz. The stability of the coherent phonon source is evaluated via its phase noise, with a maximum achieved suppression of 44 dBc/Hz at 1 kHz offset for a 100 MHz mechanical resonator. Introducing a weak modulation in the excitation laser reveals as a further knob to trigger, control and stabilize the dynamical solutions of self-pulsing based optomechanical oscillators, thus enhancing their potential as acoustic wave sources in a single-layer silicon platform. © 2021 Guillermo Arregui et al., published by De Gruyter.
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Layered Nanocomposite 2D-TiO2 with Cu2O Nanoparticles as an Efficient Photocatalyst for 4-Chlorophenol Degradation and Hydrogen Evolution
Alegría M., Aliaga J., Ballesteros L., Sotomayor-Torres C., González G., Benavente E. Topics in Catalysis; 64 (1-2): 167 - 180. 2021. 10.1007/s11244-020-01360-6. IF: 2.910
New composites formed by layered hybrid TiO2(stearic acid) (LHTiO2) and, Cu2O nanoparticles were studied as photocatalysts that extend the response range to light visible for the evolution of hydrogen and the degradation of 4-chlorophenol. The results revealed that LHTiO2/Cu2O exhibited a clearly improved photocatalytic degradation, about 5.6 times faster than pristine TiO2, and hydrogen evolution of about 2.7 times higher than the TiO2 anatase. The enhanced photocatalytic activity can be assigned to the properties of the two-dimensional morphology, in sheets-like arrangement of LHTiO2, benefitting from the high exposure of surface, with more active sites available to improve matching with the surfaces of the Cu2O nanocrystals and significant reduction of migration distances of photogenerated carriers. In the photocatalytic degradation, a mechanism Z-scheme is supported, and in the photocatalytic evolution of hydrogen a mechanism type II band alignment is indicated. Photocatalytic reuse tests showed that stability and catalytic activity of LHTiO2/Cu2O were maintained for three cycles. Photoelectrochemical evaluation were performed through measurements of the photocurrent response and electrochemical impedance. © 2020, Springer Science+Business Media, LLC, part of Springer Nature.
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Near-Field Imaging of Magnetic Complex Mode Volume
Caselli N., Wu T., Arregui G., Granchi N., Intonti F., Lalanne P., Gurioli M. ACS Photonics; 8 (5): 1258 - 1263. 2021. 10.1021/acsphotonics.0c01943. IF: 7.529
The non-Hermitian nature of confined photonic modes is described by the electric complex modal volume, VE, which represents a key parameter that leads to counterintuitive effects, such as negative modal contribution to the local density of states and non-Lorentzian lineshapes. Here, we address the magnetic counterpart of VE by means of near-field perturbation experiments in a photonic crystal slab cavity. We study the relevant role played by the imaginary part of the magnetic modal volume, VH, which can increase the quality factor of the confined modes by means of a local external magnetic perturbation. We show how a mapping of the spatial distribution of both the real and imaginary parts of VH can be inferred by near-field experiments employing Al-covered near-field tips. Our findings deepen the role of the magnetic component of light and could open a new route in employing metamaterials, magnetic quantum emitters, and topological photonics. © 2021 American Chemical Society.
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Optomechanical crystals for spatial sensing of submicron sized particles
Navarro-Urrios D., Kang E., Xiao P., Colombano M.F., Arregui G., Graczykowski B., Capuj N.E., Sledzinska M., Sotomayor-Torres C.M., Fytas G. Scientific Reports; 11 (1, 7829) 2021. 10.1038/s41598-021-87558-4. IF: 4.380
Optomechanical crystal cavities (OMC) have rich perspectives for detecting and indirectly analysing biological particles, such as proteins, bacteria and viruses. In this work we demonstrate the working principle of OMCs operating under ambient conditions as a sensor of submicrometer particles by optically monitoring the frequency shift of thermally activated mechanical modes. The resonator has been specifically designed so that the cavity region supports a particular family of low modal-volume mechanical modes, commonly known as -pinch modes-. These involve the oscillation of only a couple of adjacent cavity cells that are relatively insensitive to perturbations in other parts of the resonator. The eigenfrequency of these modes decreases as the deformation is localized closer to the centre of the resonator. Thus, by identifying specific modes that undergo a frequency shift that amply exceeds the mechanical linewidth, it is possible to infer if there are particles deposited on the resonator, how many are there and their approximate position within the cavity region. OMCs have rich perspectives for detecting and indirectly analysing biological particles, such as proteins, viruses and bacteria. © 2021, The Author(s).
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Quantifying the Robustness of Topological Slow Light
Arregui G., Gomis-Bresco J., Sotomayor-Torres C.M., Garcia P.D. Physical Review Letters; 126 (2, 027403) 2021. 10.1103/PhysRevLett.126.027403. IF: 9.161
The backscattering mean free path ζ, the average ballistic propagation length along a waveguide, quantifies the resistance of slow light against unwanted imperfections in the critical dimensions of the nanostructure. This figure of merit determines the crossover between acceptable slow-light transmission affected by minimal scattering losses and a strong backscattering-induced destructive interference when the waveguide length L exceeds ζ. Here, we calculate the backscattering mean free path for a topological photonic waveguide for a specific and determined amount of disorder and, equally relevant, for a fixed value of the group index ng which is the slowdown factor of the group velocity with respect to the speed of light in vacuum. These two figures of merit, ζand ng, should be taken into account when quantifying the robustness of topological and conventional (nontopological) slow-light transport at the nanoscale. Otherwise, any claim on a better performance of topological guided light over a conventional one is not justified. © 2021 American Physical Society.
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Quantifying thermal transport in buried semiconductor nanostructures: Via cross-sectional scanning thermal microscopy
Spièce J., Evangeli C., Robson A.J., El Sachat A., Haenel L., Alonso M.I., Garriga M., Robinson B.J., Oehme M., Schulze J., Alzina F., Sotomayor Torres C., Kolosov O.V. Nanoscale; 13 (24): 10829 - 10836. 2021. 10.1039/d0nr08768h. IF: 7.790
Managing thermal transport in nanostructures became a major challenge in the development of active microelectronic, optoelectronic and thermoelectric devices, stalling the famous Moore's law of clock speed increase of microprocessors for more than a decade. To find the solution to this and linked problems, one needs to quantify the ability of these nanostructures to conduct heat with adequate precision, nanoscale resolution, and, essentially, for the internal layers buried in the 3D structure of modern semiconductor devices. Existing thermoreflectance measurements and "hot wire"3ω methods cannot be effectively used at lateral dimensions of a layer below a micrometre; moreover, they are sensitive mainly to the surface layers of a relatively high thickness of above 100 nm. Scanning thermal microscopy (SThM), while providing the required lateral resolution, provides mainly qualitative data of the layer conductance due to undefined tip-surface and interlayer contact resistances. In this study, we used cross-sectional SThM (xSThM), a new method combining scanning probe microscopy compatible Ar-ion beam exit nano-cross-sectioning (BEXP) and SThM, to quantify thermal conductance in complex multilayer nanostructures and to measure local thermal conductivity of oxide and semiconductor materials, such as SiO2, SiGex and GeSny. By using the new method that provides 10 nm thickness and few tens of nm lateral resolution, we pinpoint crystalline defects in SiGe/GeSn optoelectronic materials by measuring nanoscale thermal transport and quantifying thermal conductivity and interfacial thermal resistance in thin spin-on materials used in extreme ultraviolet lithography (eUV) fabrication processing. The new capability of xSThM demonstrated here for the first time is poised to provide vital insights into thermal transport in advanced nanoscale materials and devices. © The Royal Society of Chemistry.
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Reversing the Humidity Response of MoS2- And WS2-Based Sensors Using Transition-Metal Salts
Xiao P., Mencarelli D., Chavez-Angel E., Joseph C.H., Cataldo A., Pierantoni L., Sotomayor Torres C.M., Sledzinska M. ACS Applied Materials and Interfaces; 13 (19): 23201 - 23209. 2021. 10.1021/acsami.1c03691. IF: 9.229
Two-dimensional materials, such as transition-metal dichalcogenides (TMDs), are attractive candidates for sensing applications due to their high surface-to-volume ratio, chemically active edges, and good electrical properties. However, their electrical response to humidity is still under debate and experimental reports remain inconclusive. For instance, in different studies, the impedance of MoS2-based sensors has been found to either decrease or increase with increasing humidity, compromising the use of MoS2 for humidity sensing. In this work, we focus on understanding the interaction between water and TMDs. We fabricated and studied humidity sensors based on MoS2 and WS2 coated with copper chloride and silver nitrate. The devices exhibited high chemical stability and excellent humidity sensing performance in relative humidity between 4 and 80%, with response and recovery times of 2 and 40 s, respectively. We have systematically investigated the humidity response of the materials as a function of the type and amount of induced metal salt and observed the reverse action of sensing mechanisms. This phenomenon is explained based on a detailed structural analysis of the samples considering the Grotthuss mechanism in the presence of charge trapping, which was represented by an appropriate lumped-element model. Our findings open up a possibility to tune the electrical response in a facile manner and without compromising the high performance of the sensor. They offer an insight into the time-dependent performance and aging of the TMD-based sensing devices. © 2021 American Chemical Society.
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Review on Sol-Gel Synthesis of Perovskite and Oxide Nanomaterials
Daniel Navas, Sandra Fuentes, Alejandro Castro-Alvarez, Emigdio Chavez-Angel Gels; 7 (4) 2021. 10.3390/gels7040275. IF: 4.702
Sol-Gel is a low cost, well-established and flexible synthetic route to produce a wide range of micro- and nanostructures. Small variations in pH, temperature, precursors, time, pressure, atmosphere, among others, can lead to a wide family of compounds that share the same molecular structures. In this work, we present a general review of the synthesis of LaMnO3, SrTiO3, BaTiO3 perovskites and zinc vanadium oxides nanostructures based on Sol-Gel method. We discuss how small changes in the parameters of the synthesis can modify the morphology, shape, size, homogeneity, aggregation, among others, of the products. We also discuss the different precursors, solvents, working temperature, reaction times used throughout the synthesis. In the last section, we present novel uses of Sol-Gel with organic materials with emphasis on carbon-based compounds. All with a perspective to improve the method for future applications in different technological fields.
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Simulations of micro-sphere/shell 2D silica photonic crystals for radiative cooling
Whitworth G.L., Jaramillo-Fernandez J., Pariente J.A., Garcia P.D., Blanco A., Lopez C., Sotomayor-Torres C.M. Optics Express; 29 (11): 16857 - 16866. 2021. 10.1364/OE.420989. IF: 3.894
Passive daytime radiative cooling has recently become an attractive approach to address the global energy demand associated with modern refrigeration technologies. One technique to increase the radiative cooling performance is to engineer the surface of a polar dielectric material to enhance its emittance atwavelengths in the atmospheric infrared transparency window (8-13 ìm) by outcoupling surface-phonon polaritons (SPhPs) into free-space. Here we present a theoretical investigation of new surface morphologies based upon self-assembled silica photonic crystals (PCs) using an in-house built rigorous coupled-wave analysis (RCWA) code. Simulations predict that silica micro-sphere PCs can reach up to 73 K below ambient temperature, when solar absorption and conductive/convective losses can be neglected. Micro-shell structures are studied to explore the direct outcoupling of the SPhP, resulting in near-unity emittance between 8 and 10 ìm. Additionally, the effect of material composition is explored by simulating soda-lime glass micro-shells, which, in turn, exhibit a temperature reduction of 61 K below ambient temperature. The RCWA code was compared to FTIR measurements of silica micro-spheres, self-assembled on microscope slides. © 2021 Optical Society of America.
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Understanding the molecular basis of 5-ht4 receptor partial agonists through 3d-qsar studies
Castro-Alvarez A., Chávez-ángel E., Nelson R. International Journal of Molecular Sciences; 22 (7, 3602) 2021. 10.3390/ijms22073602. IF: 5.924
Alzheimer’s disease (AD) is a neurodegenerative disorder whose prevalence has an incidence in senior citizens. Unfortunately, current pharmacotherapy only offers symptom relief for patients with side effects such as bradycardia, nausea, and vomiting. Therefore, there is a present need to provide other therapeutic alternatives for treatments for these disorders. The 5-HT4 receptor is an attractive therapeutic target since it has a potential role in central and peripheral nervous system disorders such as AD, irritable bowel syndrome, and gastroparesis. Quantitative structure-activity relationship analysis of a series of 62 active compounds in the 5-HT4 receptor was carried out in the present work. The structure-activity relationship was estimated using three-dimensional quantitative structure-activity relationship (3D-QSAR) techniques based on these structures’ field molecular (force and Gaussian field). The best force-field QSAR models achieve a value for the coefficient of determination of the training set of R2 training = 0.821, and for the test set R2 test = 0.667, while for Gaussian-field QSAR the training and the test were R2 training = 0.898 and R2 test = 0.695, respectively. The obtained results were validated using a coefficient of correlation of the leave-one-out cross-validation of Q2LOO = 0.804 and Q2LOO = 0.886 for force-and Gaussian-field QSAR, respectively. Based on these results, novel 5-HT4 partial agonists with potential biological activity (pEC50 8.209– 9.417 for force-field QSAR and 9.111–9.856 for Gaussian-field QSAR) were designed. In addition, for the new analogues, their absorption, distribution, metabolism, excretion, and toxicity properties were also analyzed. The results show that these new derivatives also have reasonable pharmacokinetics and drug-like properties. Our findings suggest novel routes for the design and development of new 5-HT4 partial agonists. © 2021 by the authors. Licensee MDPI, Basel, Switzerland.
