Methods of photoelectrode characterization with high spatial and temporal resolution

Esposito, Daniel V.; Baxter, Jason B.; John, Jimmy; Lewis, Nathan S.; Moffat, Thomas P.; Ogitsu, Tadashi; O’Neil, Glen D.; Pham, Tuan Anh; Talin, A. Alec; Velázquez, Jesús M.; Wood, Brandon C.

doi:10.1039/c5ee00835b

Cited by 58 publications

(47 citation statements)

References 307 publications

(384 reference statements)

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“…As a probe to study surfaces and interfaces under real conditions, surface-sensitive optical spectroscopy is highly desirable, yet only very few methods with the required spatial resolution are applicable in growth environment or electrochemistry [17,18]. RAS is such an optical technique, probing the anisotropy of a surface at very high surface sensitivity [19], and with additional high in-plane resolution in the case of RA microscopy [20].…”

Section: Introductionmentioning

confidence: 99%

Water adsorption on the P-rich GaP(100) surface: optical spectroscopy from first principles

May

Sprik

2018

New J. Phys.

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The contact of water with semiconductors typically changes its surface electronic structure by oxidation or corrosion processes. A detailed knowledge-or even control of-the surface structure is highly desirable, as it impacts the performance of opto-electronic devices from gas-sensing to energy conversion applications. It is also a prerequisite for density functional theory-based modelling of the electronic structure in contact with an electrolyte. The P-rich GaP(100) surface is extraordinary with respect to its contact with gas-phase water, as it undergoes a surface reordering, but does not oxidise. We investigate the underlying changes of the surface in contact with water by means of theoretically derived reflection anisotropy spectroscopy (RAS). A comparison of our results with experiment reveals that a water-induced hydrogen-rich phase on the surface is compatible with the boundary conditions from experiment, reproducing the optical spectra. We discuss potential reaction paths that comprise a water-enhanced hydrogen mobility on the surface. Our results also show that computational RAS-required for the interpretation of experimental signatures-is feasible for GaP in contact with water double layers. Here, RAS is sensitive to surface electric fields, which are an important ingredient of the Helmholtz-layer. This paves the way for future investigations of RAS at the semiconductor-electrolyte interface.

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Section: Introductionmentioning

confidence: 99%

Water adsorption on the P-rich GaP(100) surface: optical spectroscopy from first principles

May

Sprik

2018

New J. Phys.

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“…Transient absorption spectroscopy (TAS) can directly monitor the dynamics of photogenerated charge carriers. 24 During the past few years, the dynamics of photogenerated charge carriers in hematite with and without surface modification were intensively studied by Durrant's group, [25][26][27][28][29][30][31][32][33] mainly on a time scale of ms-s, which demonstrated that photocurrents were related to photogenerated long-lived holes, 27 and surface modification formed a hetero-conjunction at the surface of hematite films, [28][29][30] thus instead of recombining with photogenerated electrons, surface modification promoted the transfer of holes onto the surface to oxidize water. An ultrafast (fs-ns) TAS study was also undertaken by the same group to explore the effect of applied bias on the ultrafast electron-hole recombination.…”

Section: Introductionmentioning

confidence: 99%

Probing the dynamics of photogenerated holes in doped hematite photoanodes for solar water splitting using transient absorption spectroscopy

Pei

Wijten

Weckhuysen

2018

Phys. Chem. Chem. Phys.

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Hematite (α-Fe2O3) has been extensively studied as a promising candidate for photoelectrochemical water splitting; however its overall efficiency is still relatively low. Doping is believed to be efficient in enhancing the photoactivity, while direct evidence for the promoted charge carrier dynamics is very limited. Herein, transient absorption spectroscopy was used to directly investigate the yield and decay dynamics of the photogenerated holes in Sn and/or Ti doped α-Fe2O3. Sn or Ti doping was observed to have different origins to the enhanced water oxidation photocurrent: Sn doping retarded the electron-hole recombination, while Ti doping mainly increased the photogenerated charge carrier density. Our results also demonstrated that co-doping may combine both advantages to enhance the overall photoactivity of α-Fe2O3.

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“…Spatial resolution—often at the cost of temporal resolution—can also be achieved by various scanning probe techniques such as scanning photocurrent microscopy or electrochemical scanning tunneling microscopy . These techniques do, however, often have the disadvantage of a very limited temporal resolution, which impairs in situ control during surface processing.…”

Section: The Solid–liquid Interfacementioning

confidence: 99%

“…Paired with a detailed understanding of interface formation mechanisms, however, the true power of in situ control is to allow for specific modification and tuning of interface formation for the device of choice. There are several excellent reviews on in situ approaches covering wide ranges of materials from basic science to applications as well as varieties of preparation and analysis techniques . As indicated in Figure , this review will be focused on in situ control over interfaces of materials that are relevant for photoinduced reactions in high‐efficiency solar energy conversion and sensing applications with in situ control of semiconductor/polymer/biological interfaces.…”

Section: Introductionmentioning

confidence: 99%

In Situ Characterization of Interfaces Relevant for Efficient Photoinduced Reactions

Supplie

May

Brückner

et al. 2017

Adv Materials Inter

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which he pioneered and established. In general, interfaces do not only determine electronic properties of the final device; their atomic order also highly affects growth kinetics and defect formation. Moreover, the design of solid-liquid and hybrid interfaces determines their chemical reactivity and stability. In situ monitoring of interface preparation, formation, and interfacial reactions thus promises efficient process control. Paired with a detailed understanding of interface formation mechanisms, however, the true power of in situ control is to allow for specific modification and tuning of interface formation for the device of choice. There are several excellent reviews on in situ approaches covering wide ranges of materials from basic science to applications as well as varieties of preparation and analysis techniques. [2][3][4][5][6][7][8][9][10][11] As indicated in Figure 1, this review will be focused on in situ control over interfaces of materials that are relevant for photoinduced reactions in high-efficiency solar energy conversion and sensing applications with in situ control of semiconductor/polymer/ biological interfaces. We will restrict the techniques to realistic and complex, non-ultrahigh-vacuum (UHV) ambient, where in situ control is most demandingbut also highly desired. The more complex the interfacial reactions are, the more important is the in situ characterization. Ex situ approaches can contribute to an indirect understanding of interface formation, but to understand and, finally, control the dynamic processes taking place, real-time measurements are appropriate. The challenge, we are facing, is twofold: On the one hand, increased interaction with the surrounding ambient causes higher complexity. Yet at the same time, it decreases the number of applicable techniques. On the other hand, those techniques are often elaborate and not necessarily easy to interpret. In a nutshell, we will discuss four main topics:(i) Surface preparation during growth of structures for highefficiency solar energy conversion: World-record conversion efficiencies in both photovoltaics [12,13] and solar water splitting [14] are achieved with multijunction solar cells based on epitaxial III/V compound semiconductor structures. We will discuss in situ controlled preparation Solar energy conversion and photoinduced bioactive sensors are representing topical scientific fields, where interfaces play a decisive role for efficient applications. The key to specifically tune these interfaces is a precise knowledge of interfacial structures and their formation on the microscopic, preferably atomic scale. Gaining thorough insight into interfacial reactions, however, is particularly challenging in relevant complex chemical environment. This review introduces a spectrum of material systems with corresponding interfaces significant for efficient applications in energy conversion and sensor technologies. It highlights appropriate analysis techniques capable of monitoring critical physicochemical reactions in situ during non-vacuu...

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Methods of photoelectrode characterization with high spatial and temporal resolution

Abstract: This article reviews computational and in situ experimental tools capable of characterizing the properties and performance of photoelectrodes used for solar fuels production with high spatial and temporal resolution.

Cited by 58 publications

References 307 publications

Water adsorption on the P-rich GaP(100) surface: optical spectroscopy from first principles

Water adsorption on the P-rich GaP(100) surface: optical spectroscopy from first principles

Probing the dynamics of photogenerated holes in doped hematite photoanodes for solar water splitting using transient absorption spectroscopy

In Situ Characterization of Interfaces Relevant for Efficient Photoinduced Reactions

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