Thickness-Dependent Charge Transport in Three Dimensional Ru(II)- Tris(phenanthroline)-Based Molecular Assemblies.

We describe here the fabrication of large-area molecular junctions with a configuration of ITO/[Ru(Phen)3]/Al to understand temperature- and thickness-dependent charge transport phenomena. Thanks to the electrochemical technique, thin layers of electroactive ruthenium(II)-tris(phenanthroline) [Ru(Phen)3] with thicknesses of 4-16 nm are covalently grown on sputtering-deposited patterned ITO electrodes. The bias-induced molecular junctions exhibit symmetric current-voltage (j-V) curves, demonstrating highly efficient long-range charge transport and weak attenuation with increased molecular film thickness (ß = 0.70 to 0.79 nm-1). Such a lower ß value is attributed to the accessibility of Ru(Phen)3 molecular conduction channels to Fermi levels of both the electrodes and a strong electronic coupling at ITO-molecules interfaces. The thinner junctions (d = 3.9 nm) follow charge transport via resonant tunneling, while the thicker junctions (d = 10-16 nm) follow thermally activated (activation energy, Ea ∼ 43 meV) Poole-Frenkel charge conduction, showing a clear "molecular signature" in the nanometric junctions.

Metal-organic Frameworks in Semiconductor Devices.

Metal-organic frameworks (MOFs) are a specific class of hybrid, crystalline, nano-porous materials made of metal-ion-based 'nodes' and organic linkers. Most of the studies on MOFs largely focused on porosity, chemical and structural diversity, gas sorption, sensing, drug delivery, catalysis, and separation applications. In contrast, much less reports paid attention to understanding and tuning the electrical properties of MOFs. Poor electrical conductivity of MOFs (~10-7-10-10 S cm-1), reported in earlier studies, impeded their applications in electronics, optoelectronics, and renewable energy storage. To overcome this drawback, the MOF community has adopted several intriguing strategies for electronic applications. The present review focuses on creatively designed bulk MOFs and surface-anchored MOFs (SURMOFs) with different metal nodes (from transition metals to lanthanides), ligand functionalities, and doping entities, allowing tuning and enhancement of electrical conductivity. Diverse platforms for MOFs-based electronic device fabrications, conductivity measurements, and underlying charge transport mechanisms are also addressed. Overall, the review highlights the pros and cons of MOFs-based electronics (MOFtronics), followed by an analysis of the future directions of research, including optimization of the MOF compositions, heterostructures, electrical contacts, device stacking, and further relevant options which can be of interest for MOF researchers and result in improved devices performance.

Electrochemical Potential-Driven High-Throughput Molecular Electronic and Spintronic Devices: From Molecules to Applications.

Molecules are fascinating candidates for constructing tunable and electrically conducting devices by the assembly of either a single molecule or an ensemble of molecules between two electrical contacts followed by current-voltage (I-V) analysis, which is often termed "molecular electronics". Recently, there has been also an upsurge of interest in spin-based electronics or spintronics across the molecules, which offer additional scope to create ultrafast responsive devices with less power consumption and lower heat generation using the intrinsic spin property rather than electronic charge. Researchers have been exploring this idea of utilizing organic molecules, organometallics, coordination complexes, polymers, and biomolecules (proteins, enzymes, oligopeptides, DNA) in integrating molecular electronics and spintronics devices. Although several methods exist to prepare molecular thin-films on suitable electrodes, the electrochemical potential-driven technique has emerged as highly efficient. In this Review we describe recent advances in the electrochemical potential driven growth of nanometric various molecular films on technologically relevant substrates, including non-magnetic and magnetic electrodes to investigate the stimuli-responsive charge and spin transport phenomena.

Reinforced Room-Temperature Spin Filtering in Chiral Paramagnetic Metallopeptides.

Chirality-induced spin selectivity (CISS), whereby helical molecules polarize the spin of electrical current, is an intriguing effect with potential applications in nanospintronics. In this nascent field, the study of the CISS effect using paramagnetic chiral molecules, which could introduce another degree of freedom in controlling the spin transport, remains so far unexplored. To address this challenge, herein we propose the use of self-assembled monolayers (SAMs) of helical lanthanide-binding peptides. To elucidate the effect of the paramagnetic nuclei, monolayers of the peptide coordinating paramagnetic or diamagnetic ions are prepared. By means of spin-dependent electrochemistry, the CISS effect is demonstrated by cyclic voltammetry and electrochemical impedance measurements for both samples. Additionally, an implementation of the standard liquid-metal drop electron transport setup has been carried out, and this process helped to demonstrate the peptides' suitability for solid-state devices. Remarkably, the inclusion of a paramagnetic center in the peptide increases the spin polarization as was independently proved by different techniques. These findings permit the inclusion of magnetic biomolecules in the CISS field and pave the way to their implementation in a new generation of (bio)spintronic nanodevices.

Versatile electrochemical approaches towards the fabrication of molecular electronic devices.

The concept of molecular electronic devices (MEDs) has evolved since the first theoretical report was published in 1974. This theoretical article laid the foundation for understanding charge-transport phenomena by utilizing either a single molecule or numerous molecules sandwiched between two electrical conductors. Since then, many research groups have engaged in molecular junction fabrication using a variety of molecules including organic, inorganic, and organometallic molecules, polymers, and biomolecules that can mimic the electronic functions of traditional silicon-based devices. To date, most of these molecular junctions have been constructed using well-explored molecular assemblies of thiolated derivatives adsorbed mostly on Au substrates. However, the Au-S bond is not considered to be a true covalent bond in view of its surface bond energy, which is ∼1.9 eV, much less than pure covalent bond energy. Additionally, Au-S interfaces suffer from poor reactivity and instability over time; thus, they are not suitable for real world applications. Therefore, an alternative approach for the fabrication of molecular electronic junctions must be envisioned to address all the difficulties mentioned above. Herein, we summarize the most recent experiential outcomes to demonstrate how electrochemical techniques can be employed to form robust molecular layers on various substrates including Au, ZnO, SnO2, H-terminated Si, and conductive carbon electrodes that are suitable for the fabrication of reliable molecular electronics devices for charge-transport studies. This fascinating electrochemical technique is appropriate for producing not only homostructure but also heterostructure molecular layers with desired thicknesses. We also discuss the pros and cons of the electrochemical process for growing molecular layers in the Conclusion and outlook section.

Nanometric Assembly of Functional Terpyridyl Complexes on Transparent and Conductive Oxide Substrates: Structure, Properties, and Applications.

Over the last few decades, molecular assemblies on solid substrates have become increasingly popular, challenging the traditional systems and materials in terms of better control over molecular structure and function at the nanoscale. A variety of such assemblies with high complexity and adjustable properties was generated on the basis of organic, inorganic, organometallic, polymeric, and biomolecular building blocks. Particular versatile elements in this context are terpyridyls due to their wide design flexibility, ease of functionalization, and ability to coordinate to a broad variety of transition-metal ions without forming diastereoisomers, which facilitates tuning of their optical and electronic properties. Specifically, metal-terpyridyl complexes are worthy building blocks for generating optoelectronically active assemblies on technologically relevant transparent and conductive oxide substrates. In this context, the present Account summarizes our recent results on the preparation, characterization, and applications of nanometric (2-10 nm) surface-confined molecular assemblies of Cu2+, Fe2+, Ru2+, and Os2+-terpyridyl complexes on SiOx-based substrates (glass, quartz, silicon, and ITO-coated glass). These assemblies rely on covalent bond formation between the iodo-/chloro-terminated functionalized SiOx substrates and the pendant group (mostly pyridyl) hosted on the terpyridyl complexes. Such an anchoring provides excellent thermal, temporal, radiative, and electrochemical stability to the assemblies as needed for technological applications. The functional, covalently assembled monolayers were extended to fabricate molecular dyads (bilayers), triads (trilayers), and oligomers by an established layer-by-layer procedure using suitable metallolinkers such as Cu2+, Ag+, and Pd2+. The chemical, optical, and electrochemical properties of these assemblies could be precisely adjusted by selection of proper metal-terpyridyl complexes and/or metallolinkers, so that the resulting systems served, relying on the specific design, as sensors, catalysts, molecular logic gates, and photochromic devices. For instance, a Cu-terpyridyl-based assembly on a glass substrate showed "turn on" detection of ascorbic acid. In another example, heterometallic molecular triads were exposed to redox-active NO+ for selective oxidation of the metal ions, and the optical readout was utilized for configuring multiple-input-based molecular logic gates. Furthermore, bias-driven (+0.6 to +1.6 V vs Ag/AgCl) optical properties of the heteroleptic Ru2+/Os2+-terpyridyl monolayers were modulated and "read out" by spectro-electrochemical techniques demonstrating high charge/information density (3-4 × 1014 electrons/cm2). Moreover, the manipulation of the M2+/3+ (M = Fe, Ru, and Os) redox wave in the assembly provided the possibility to create mixed-valence redox-states paving the way toward the fabrication of "multi-bit" memory systems. We truly believe that due to these intriguing characteristics and excellent stability, terpyridyl-based molecular assemblies have the potential to become a versatile platform for the next generation of smart optoelectronic devices.

Electrochemistry of Metalloproteins Attached through Functional Self-Assembled Monolayers on Gold and Ferromagnetic Electrodes.

We report the experimental results of a study of the electron-transfer processes of redox-active metalloproteins bound to mixed self-assembled monolayers (SAMs) on magnetic (nickel or ultrathin gold-coated nickel) or nonmagnetic (gold) electrodes. Metalloproteins, such as hemoglobin (Hb), Cytochrome C (Cyt C), and Cyt C oxidase, are attached through electrostatic interactions to the free carboxylate or imidazole groups present in the mixed SAMs. The formation of both mixed SAMs and SAM/metalloprotein heterostructures were confirmed by using advanced surface analysis techniques, such as polarization modulation infrared reflection absorption spectroscopy and aqueous contact angle measurements. Electrochemical measurements indicated a stronger electronic coupling between Hb and Cyt C oxidase and the mixed-SAM-coated gold or gold-coated-nickel electrodes, whereas a weaker coupling was found between the protein and the pure nickel electrode. Surface coverage and the electron-transfer rate constant were estimated from the cyclic voltammetry data.

Spin-Dependent Transport through Chiral Molecules Studied by Spin-Dependent Electrochemistry.

Molecular spintronics (spin + electronics), which aims to exploit both the spin degree of freedom and the electron charge in molecular devices, has recently received massive attention. Our recent experiments on molecular spintronics employ chiral molecules which have the unexpected property of acting as spin filters, by way of an effect we call "chiral-induced spin selectivity" (CISS). In this Account, we discuss new types of spin-dependent electrochemistry measurements and their use to probe the spin-dependent charge transport properties of nonmagnetic chiral conductive polymers and biomolecules, such as oligopeptides, L/D cysteine, cytochrome c, bacteriorhodopsin (bR), and oligopeptide-CdSe nanoparticles (NPs) hybrid structures. Spin-dependent electrochemical measurements were carried out by employing ferromagnetic electrodes modified with chiral molecules used as the working electrode. Redox probes were used either in solution or when directly attached to the ferromagnetic electrodes. During the electrochemical measurements, the ferromagnetic electrode was magnetized either with its magnetic moment pointing "UP" or "DOWN" using a permanent magnet (H = 0.5 T), placed underneath the chemically modified ferromagnetic electrodes. The spin polarization of the current was found to be in the range of 5-30%, even in the case of small chiral molecules. Chiral films of the l- and d-cysteine tethered with a redox-active dye, toludin blue O, show spin polarizarion that depends on the chirality. Because the nickel electrodes are susceptible to corrosion, we explored the effect of coating them with a thin gold overlayer. The effect of the gold layer on the spin polarization of the electrons ejected from the electrode was investigated. In addition, the role of the structure of the protein on the spin selective transport was also studied as a function of bias voltage and the effect of protein denaturation was revealed. In addition to "dark" measurements, we also describe photoelectrochemical measurements in which light is used to affect the spin selective electron transport through the chiral molecules. We describe how the excitation of a chromophore (such as CdSe nanoparticles), which is attached to a chiral working electrode, can flip the preferred spin orientation of the photocurrent, when measured under the identical conditions. Thus, chirality-induced spin polarization, when combined with light and magnetic field effects, opens new avenues for the study of the spin transport properties of chiral molecules and biomolecules and for creating new types of spintronic devices in which light and molecular chirality provide new functions and properties.

Covalently Assembled Monolayers of Homo- and Heteroleptic FeII -Terpyridyl Complexes on SiOx and ITO-Coated Glass Substrates: An Experimental and Theoretical Study.

Well-defined FeII -terpyridyl monolayers were fabricated on SiOx and conductive ITO-coated glass substrates through covalent-bond formation between the metallo-organic complexes and a preassembled coupling layer. Three different homo- and heteroleptic complexes with terminal pyridyl, amine, and phenyl groups were tested. All the films were found to be densely packed and homogeneous, and consist of molecules standing upright. They exhibited high thermal (up to ≈220 °C) and temporal (up to 5 h at 100 °C) stability. The UV/Vis spectra of the monolayers showed pronounced metal-to-ligand charge-transfer bands with a significant redshift compared with the solution spectra of the metallo-ligands with a pendant pyridyl group quaternized with the coupling layer, whereas the shift was significantly smaller when the coupling layer was bonded to the primary amine (-NH2 ) group of the complex. Cyclic voltammograms of the monolayers showed reversible, one-electron redox behavior and suggested strong electronic coupling between the confined molecules and the underlying substrate. Analysis of the electrochemistry data allowed us to estimate the charge-transfer rate constant between the metal center and the substrate. Additionally, detailed quantum-chemical calculations were performed to support and rationalize the experimentally observed photophysical properties of the FeII -terpyridyl complexes both in the solution state and when bound to a SiOx -based substrate.

Photospintronics: Magnetic Field-Controlled Photoemission and Light-Controlled Spin Transport in Hybrid Chiral Oligopeptide-Nanoparticle Structures.

The combination of photonics and spintronics opens new ways to transfer and process information. It is shown here that in systems in which organic molecules and semiconductor nanoparticles are combined, matching these technologies results in interesting new phenomena. We report on light induced and spin-dependent charge transfer process through helical oligopeptide-CdSe nanoparticles' (NPs) architectures deposited on ferromagnetic substrates with small coercive force (∼100-200 Oe). The spin control is achieved by the application of the chirality-induced spin-dependent electron transfer effect and is probed by two different methods: spin-controlled electrochemichemistry and photoluminescence (PL) at room temperature. The injected spin could be controlled by excitation of the nanoparticles. By switching the direction of the magnetic field of the substrate, the PL intensity could be alternated.

New one-step thiol functionalization procedure for Ni by self-assembled monolayers.

This article reports on a facile and fast strategy for the self-assembled monolayer (SAM) functionalization of nickel surfaces, employing cyclic voltammetry (CV) cycling of a suitable tailored solution containing the species to be adsorbed. Results are presented for ultrathin films formed on Ni by 1-hexadecanethiol (C16), L-cysteine (L-cys), and the poly{methyl (2R)-3-(2,2'-bithiophen-4-ylsulfanyl)-2-[(tert-butoxycarbonyl)amino]propanoate} (PCT-L) thiophene-based chiral polymer. The effective formation of high-quality ultrathin organic films on the nickel was verified both electrochemically and by exploiting typical surface characterization techniques such as contact angle, ellipsometry, atomic force microscopy (AFM), polarization modulation-infrared reflection-absorption spectroscopy (PM-IRRAS), and X-ray photoelectron spectroscopy (XPS).

Metal-free platforms for molecular thin films as high-performance supercapacitors.

Controlling chemical functionalization and achieving stable electrode-molecule interfaces for high-performance electrochemical energy storage applications remain challenging tasks. Herein, we present a simple, controllable, scalable, and versatile electrochemical modification approach of graphite rods (GRs) extracted from low-cost Eveready cells that were covalently modified with anthracene oligomers. The anthracene oligomers with a total layer thickness of ∼24 nm on the GR electrode yield a remarkable specific capacitance of ∼670 F g-1 with good galvanostatic charge-discharge cycling stability (10 000) recorded in 1 M H2SO4 electrolyte. Such a boost in capacitance is attributed mainly to two contributions: (i) an electrical double-layer at the anthracene oligomer/GR/electrolyte interfaces, and (ii) the proton-coupled electron transfer (PCET) reaction, which ensures a substantial faradaic contribution to the total capacitance. Due to the higher conductivity of the anthracene films, it possesses more azo groups (-N[double bond, length as m-dash]N-) during the electrochemical growth of the oligomer films compared to pyrene and naphthalene oligomers, which is key to PCET reactions. AC-based electrical studies unravel the in-depth charge interfacial electrical behavior of anthracene-grafted electrodes. Asymmetrical solid-state supercapacitor devices were made using anthracene-modified biomass-derived porous carbon, which showed improved performance with a specific capacitance of ∼155 F g-1 at 2 A g-1 with an energy density of 5.8 W h kg-1 at a high-power density of 2010 W kg-1 and powered LED lighting for a longer period. The present work provides a promising metal-free approach in developing organic thin-film hybrid capacitors.

Nanoscale molecular rectifiers.

The use of molecules bridged between two electrodes as a stable rectifier is an important goal in molecular electronics. Until recently, however, and despite extensive experimental and theoretical work, many aspects of our fundamental understanding and practical challenges have remained unresolved and prevented the realization of such devices. Recent advances in custom-designed molecular systems with rectification ratios exceeding 105 have now made these systems potentially competitive with existing silicon-based devices. Here, we provide an overview and critical analysis of recent progress in molecular rectification within single molecules, self-assembled monolayers, molecular multilayers, heterostructures, and metal-organic frameworks and coordination polymers. Examples of conceptually important and best-performing systems are discussed, alongside their rectification mechanisms. We present an outlook for the field, as well as prospects for the commercialization of molecular rectifiers.

Coexistence of Electrochromism and Bipolar Nonvolatile Memory in a Single Viologen.

Viologens are fascinating redox-active organic compounds that have been widely explored in electrochromic devices (ECDs). However, the combination of electrochromic and resistive random-access memory in a single viologen remains unexplored. We report the coexistence of bistate electrochromic and single-resistor (1R) memory functions in a novel viologen. A high-performance electrochromic function is achieved by combining viologen (BzV2+2PF6) with polythiophene (P3HT), enabling a "push-pull" electronic effect due to the efficient intermolecular charge transfer in response to an applied bias. The ECDs show high coloration efficiency (ca. 1150 ± 10 cm2 C-1), subsecond switching time, good cycle stability (>103 switching cycles), and low-bias operation (±1.5 V). The ECDs require low power for switching the color states (55 µW cm-2 for magenta and 141 µW cm-2 for blue color). The random-access memory devices (p+2-Si/BzV2+2PF6/Al) exhibit distinct low and high resistive states with an ON/OFF ratio of ∼103, bipolar and nonvolatile characteristics that manifest good performances, and "Write"-"Read"-"Erase" (WRE) functions. The charge conduction mechanism of the RRAM device is elucidated by the Poole-Frenkel model where SET and RESET states arise at a low transition voltage (VT = ±1.7 V). Device statistics and performance parameters for both electrochromic and memory devices are compared with the literature data. Our findings on electrochromism and nonvolatile memory originated in the same viologen could boost the development of multifunctional, smart, wearable, flexible, and low-cost optoelectronic devices.

"Turn on" electron-transfer-based selective detection of ascorbic acid via copper complexes immobilized on glass.

"Turn-on" optical detection of parts-per-million (ppm) levels of ascorbic acid (AA) in water has been determined using a redox-active monolayer on glass.

Systemic deficiency of vitronectin is associated with aortic inflammation and plaque progression in ApoE-Knockout mice.

Optimal cell spreading and interplay of vascular smooth muscle cells (VSMC), inflammatory cells, and cell adhesion molecules (CAM) are critical for progressive atherosclerosis and cardiovascular complications. The role of vitronectin (VTN), a major cell attachment glycoprotein, in the pathogenesis of atherosclerosis remains elusive. In this study, we attempt to examine the pathological role of VTN in arterial plaque progression and inflammation. We found that, relative expression analysis of VTN from the liver of Apolipoprotein E (ApoE) Knockout mice revealed that atherosclerotic progression induced by feeding mice with high cholesterol diet (HCD) causes a significant downregulation of VTN mRNA as well as protein after 60 days. Promoter assay confirmed that cholesterol modulates the expression of VTN by influencing its promoter. Mimicking VTN reduction with siRNA in HCD fed ApoE Knockout mice, accelerated athero-inflammation with an increase in NF-kB, ICAM-1, and VCAM-1 at the site of the plaque along with upregulation of inflammatory proteins like MCP-1 and IL-1ß in the plasma. Also, matrix metalloprotease (MMP)-9 and MMP-12 expression were increased and collagen content was decreased in the plaque, in VTN deficient condition. This might pose a challenge to plaque integrity. Human subjects with acute coronary syndrome or having risk factors of atherosclerosis have lower levels of VTN compared to healthy controls suggesting a clinical significance of plasma VTN in the pathophysiology of coronary artery disease. We establish that, VTN plays a pivotal role in cholesterol-driven atherosclerosis and aortic inflammation and might be a useful indicator for atherosclerotic plaque burden and stability.

Proteomic analysis detects deregulated reverse cholesterol transport in human subjects with ST-segment elevation myocardial infarction.

Reverse cholesterol transport (RCT) plays a critical role in removing cholesterol from the arterial wall. However, very few reports directly relate chronic inflammation and RCT with atherosclerosis. The present study was undertaken to investigate clinical implications of significantly altered circulating proteins in subjects with ST-segment elevation myocardial infarction (STEMI) in the manifestation of atherosclerotic events. Using a case-control design, more than 2500 proteins in both STEMI and healthy control subjects were identified by Orbitrap mass spectrometer. Quantitative proteomics study revealed downregulation of 26 proteins while expression of 38 proteins increased significantly in STEMI subjects compared to healthy controls. Pathway enrichment analyses indicated that most of the identified proteins were related to chronic inflammation, atherosclerosis, and RCT. Altered proteins such as AZGP1, ABCA5, Calicin, PGLYRP2, HAVCR2 and C17ORF57 were further validated by Western blotting analysis of human plasma. Pathophysiological significance was studied using macrophage derived foam cell for their critical role in RCT which indicated the imbalance of RCT via the interaction of AZGP1 with CD36. In summary, this study revealed a unique relationship of some novel proteins apparently responsible for impaired RCT and chronic inflammation leading to atherothrombosis and myocardial infarction. SIGNIFICANCE: In the present study we identified ≥2500 unique circulating proteins in healthy control and clinically diagnosed STEMI subjects among which 423 proteins were found to be common in both the groups. We further show 64 proteins significantly different between healthy control and STEMI subjects. Proteomic analyses reveal a panel of proteins associated with atherosclerosis and STEMI. One of the proteins, AZGP1, an adipokine, is likely to act as the missing link between chronic inflammation and cholesterol transport. Deregulation of reverse cholesterol transport might be orchestrated by AZGP1, CD36, ABCA5, and PPARÉ£ in STEMI subjects. The present study employs shotgun and quantitative proteomics followed by in vitro validations demonstrating a biochemical basis for reverse cholesterol transport in the local milieu of the luminal wall of the artery which are critical for plaque build-up and atherosclerosis.

Redox-Active Ferrocene grafted on H-Terminated Si(111): Electrochemical Characterization of the Charge Transport Mechanism and Dynamics.

Electroactive self-assembled monolayers (SAMs) bearing a ferrocene (Fc) redox couple were chemically assembled on H-terminated semiconducting degenerate-doped n-type Si(111) substrate. This allows to create a Si(111)|organic-spacer|Fc hybrid interface, where the ferrocene moiety is covalently immobilized on the silicon, via two alkyl molecular spacers of different length. Organic monolayer formation was probed by Laser Ablation-Inductively Coupled Plasma-Mass Spectrometry (LA-ICP-MS) and X-ray photoelectron spectroscopy (XPS) measurements, which were also used to estimate thickness and surface assembled monolayer (SAM) surface coverage. Atomic force microscopy (AFM) measurements allowed to ascertain surface morphology and roughness. The single electron transfer process, between the ferrocene redox probe and the Si electrode surface, was probed by cyclic voltammetry (CV) measurements. CVs recorded at different scan rates, in the 10 to 500 mV s-1 range, allowed to determine peak-to-peak separation, half-wave potential, and charge-transfer rate constant (KET). The experimental findings suggest that the electron transfer is a one electron quasi-reversible process. The present demonstration of surface engineering of functional redox-active organometallic molecule can be efficient in the field of molecular electronics, surface-base redox chemistry, opto-electronic applications.

Spin Selectivity in Photoinduced Charge-Transfer Mediated by Chiral Molecules.

Optical control and readout of electron spin and spin currents in thin films and nanostructures have remained attractive yet challenging goals for emerging technologies designed for applications in information processing and storage. Recent advances in room-temperature spin polarization using nanometric chiral molecular assemblies suggest that chemically modified surfaces or interfaces can be used for optical spin conversion by exploiting photoinduced charge separation and injection from well-coupled organic chromophores or quantum dots. Using light to drive photoexcited charge-transfer processes mediated by molecules with central or helical chirality enables indirect measurements of spin polarization attributed to the chiral-induced spin selectivity effect and of the efficiency of spin-dependent electron transfer relative to competitive relaxation pathways. Herein, we highlight recent approaches used to detect and to analyze spin selectivity in photoinduced charge transfer including spin-transfer torque for local magnetization, nanoscale charge separation and polarization, and soft ferromagnetic substrate magnetization- and chirality-dependent photoluminescence. Building on these methods through systematic investigation of molecular and environmental parameters that influence spin filtering should elucidate means to manipulate electron spins and photoexcited states for room-temperature optoelectronic and photospintronic applications.