Interface chemistry of H2O on GaAs nanowires probed by near ambient pressure X-ray photoelectron spectroscopy

Zhang, Xueqiang; Lamere, Edward; Liu, Xinyu; Furdyna, J. K.; Ptasińska, Sylwia

doi:10.1016/j.cplett.2014.05.007

Cited by 6 publications

(20 citation statements)

References 28 publications

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“…Andersson et al 33 36 GaAs nanowires, 40 InP(100), 41 and GaN(101̅ 0), 42 as well as several recent theoretical studies on related III−V surfaces. 43−45 We next performed periodic slab calculations using DFT to verify the thermodynamic stabilities of these species under experimental conditions.…”

Section: Resultsmentioning

confidence: 98%

Observation of Surface-Bound Negatively Charged Hydride and Hydroxide on GaP(110) in H₂O Environments

Kronawitter¹,

Lessio²,

Zhao³

et al. 2015

J. Phys. Chem. C

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Surface-bound species on GaP(110) formed upon interaction with water were investigated through experiment and theory. These studies are motivated by and discussed in the context of electrocatalytic and photoelectrocatalytic schemes for solar fuel production, including especially observations of selective CO 2 reduction to methanol in acidified aqueous solutions of CO 2 and nitrogen-containing heteroaromatics. Experimentally, surface-bound species over 10 orders of magnitude of pressure were spectroscopically identified in situ using synchrotron-based ambient pressure photoelectron spectroscopy. Ga 3d and O 1s core-level spectra indicate that the interaction of GaP(110) with H 2 O induces formation of a partially dissociated adlayer, characterized by the presence of both Ga−OH and molecular H 2 O species. Measurements of the P 2p core level indicate formation of a negatively charged hydride that irreversibly bonds to surface P in vacuum. The surface densities of the hydroxide and hydride species increase with increasing pressure (surface coverage) of water. Periodic slab calculations using density functional theory were used to study several relevant water configurations at 298 K on this surface. Consistent with earlier theoretical predictions at 0 K, the calculations confirm that Ga− OH, molecular H 2 O, and P−H species are thermodynamically stable on the GaP(110) surface under experimental conditions. Isobaric measurements at elevated pressures were used to probe the thermal stabilities of adsorbed species as well as the oxidation of surface Ga and P. The observation of stable surface hydride formation induced by interaction with water is especially notable given the critical role of hydride transfer to catalysts and CO 2 during chemical fuel synthesis reactions in aqueous environments. It is hypothesized that the observed high stability of the hydride on GaP may contribute to its associated remarkable near-100% faradaic efficiency for methanol generation by solar-driven CO 2 reduction in acidified aqueous pyridine solutions [J. Am. Chem. Soc. 2008, 130, 6342] because such stability is known to yield high overpotentials for the competing hydrogen evolution reaction.

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Section: Resultsmentioning

confidence: 98%

Observation of Surface-Bound Negatively Charged Hydride and Hydroxide on GaP(110) in H₂O Environments

Kronawitter¹,

Lessio²,

Zhao³

et al. 2015

J. Phys. Chem. C

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“…The signal at each specific condition was collected within one hour; (b) and (c) comparison of high resolution Ga 2p 3/2 and P 2p spectra obtained under UHV conditions and at the H 2 O pressure of 5 mbar and RT. 28,31 The broad peak at 532. Therefore, the Ga 2p 3/2 spectra are normalized to unit intensity of main peaks and shifted to the same background lines; (d) and (e) comparison of high resolution Ga 2p 3/2 and P 2p spectra obtained under UHV and under 0.1 mbar at RT, 673 K and 773 K, and under 0.5 mbar at 773 K. respectively (Fig.…”

Section: Pressure Dependencementioning

confidence: 99%

“…4,15 Using first-principles density functional theory (DFT) calculations, Munoz-Garcia et al reported the presence of hydride-like H atoms on the GaP(110) surface as a result of water dissociation via hydrogenbonded intermediates. 27 There are also other experimental 14,[28][29][30][31] and theoretical 6,16,26,32 studies on the role of hydrogen bonds in water interactions with III-V semiconductor surfaces such as GaP, 6,14 GaAs, 28,31 GaSb, 26,32 and InP. 16,29,30 These studies clearly emphasize the importance of such local hydrogen-bonding in the interfacial dynamics and chemistry of semiconductors.…”

Section: Introductionmentioning

confidence: 97%

“…4,6 Hydrogen-networking and hydrogen transfer are the fundamental processes to be addressed in order to understand and characterize semiconductor surfaces that are exposed to a water environment. 27 There are also other experimental 14,[28][29][30][31] and theoretical 6,16,26,32 studies on the role of hydrogen bonds in water interactions with III-V semiconductor surfaces such as GaP, 6,14 GaAs, 28,31 GaSb, 26,32 and InP. For instance, Wood et al performed ab initio molecular dynamic simulations that revealed an increase in water hydrogenbond strength on a Ga/InP(100) surface that facilitates water dissociation and local proton hopping.…”

Section: Introductionmentioning

confidence: 99%

“…27 These results indicated an enhancement in water dissociation at higher coverage. 28,31 The binding energy (BE) scale for photoelectron spectra was calibrated using the P 2p 3/2 peak, which corresponds to the P-Ga bond with a BE of 128.8 eV. 15 The present study was motivated by the lack of experimental data on chemical characterizations of H 2 O/semiconductor interfaces such as H 2 O/GaP, 14,27 particularly at near-ambient conditions.…”

Section: Introductionmentioning

confidence: 99%

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Distinct and dramatic water dissociation on GaP(111) tracked by near-ambient pressure X-ray photoelectron spectroscopy

Zhang

Ptasińska

2015

Phys. Chem. Chem. Phys.

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Water adsorption and dissociation on a GaP(111) crystal surface are investigated using near-ambient pressure X-ray photoelectron spectroscopy (NAP XPS) in a wide range of pressures (∼10(-10)-5 mbar) and temperatures (∼300-773 K). Dynamic changes in chemical evolution at the H2O/GaP(111) interface are reflected in Ga 2p3/2, O 1s, and P 2p spectra. In the pressure-dependent study performed at room temperature, an enhancement of surface Ga hydroxylation and oxidation with an increase in H2O pressure is observed. In the temperature-dependent study performed at elevated pressures, two distinct regions can be defined in which drastic changes occur in the surface chemistry. Below 673 K, the surface Ga hydroxylation and oxidation progress continuously. However, above 673 K, a large-scale conversion of surface O-Ga-OH species into non-stoichiometric Ga hydroxide along with oxidation of surface P atoms occurs through an intermediate state. The NAP XPS technique enabled us to experimentally track the chemistry at the H2O/GaP interface under near-realistic conditions, thereby providing evidence to compare with recent theoretical efforts to improve the understanding of water-splitting mechanisms and photo-corrosion on semiconductor surfaces.

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Evolution of Atomistic Topology at H₂O/GaSb(100) Interface under Ambient Conditions and GaSb Surface Passivation

Zhang

2019

J. Phys. Chem. C

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Gallium antimonide (GaSb) has emerged as a promising light absorber in solar cells and optoelectronics because of its high hot-carrier mobility. Here, the interfacial physiochemical process of H 2 O/GaSb(100) under a series of isothermal and isobaric conditions was investigated using ambient pressure X-ray photoelectron spectroscopy. At room temperature and elevated H 2 O vapor pressures, we observed the dissociative adsorption of H 2 O onto the GaSb( 100) surface and the preferential formation of (HO)Ga−Sb(H) (atop) and Ga−O(H)−Ga−Sb(H) (bridge) over (H)Ga−O(H)−Sb(H) (bridge), that is, the GaSb(100) surface was covered by hydroxyls instead of oxides. The oxyhydroxylation of the GaSb(100) surface was significantly enhanced at elevated temperatures, coupled with gradual desorption of surface Sb from 373 to 573 K in the form of SbH 3 . Meanwhile, large-scale oxyhydroxylation of GaSb(100) surface at 573 K was captured by on-line mass spectrometry, where the increment in H 2 O consumption and the generation of H 2 were observed. When the temperature reaches 673 K and above, the surface oxyhydroxides formed under lower temperatures desorbs quickly, leaving behind a Sb-terminated GaSb surface and preventing any further H 2 O dissociative adsorption. The combinative isothermal and isobaric study offers a full picture of the H 2 O/GaSb(100) interface in terms of the atomistic topological and structural evolutions under various H 2 O pressures and temperatures. The present study provides a possible venue for low-cost surface passivation of GaSb and III−V semiconductor-based electronic devices.

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Interface chemistry of H2O on GaAs nanowires probed by near ambient pressure X-ray photoelectron spectroscopy

Cited by 6 publications

References 28 publications

Observation of Surface-Bound Negatively Charged Hydride and Hydroxide on GaP(110) in H₂O Environments

Observation of Surface-Bound Negatively Charged Hydride and Hydroxide on GaP(110) in H₂O Environments

Distinct and dramatic water dissociation on GaP(111) tracked by near-ambient pressure X-ray photoelectron spectroscopy

Evolution of Atomistic Topology at H₂O/GaSb(100) Interface under Ambient Conditions and GaSb Surface Passivation

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Interface chemistry of H2O on GaAs nanowires probed by near ambient pressure X-ray photoelectron spectroscopy

Cited by 6 publications

References 28 publications

Observation of Surface-Bound Negatively Charged Hydride and Hydroxide on GaP(110) in H2O Environments

Observation of Surface-Bound Negatively Charged Hydride and Hydroxide on GaP(110) in H2O Environments

Distinct and dramatic water dissociation on GaP(111) tracked by near-ambient pressure X-ray photoelectron spectroscopy

Evolution of Atomistic Topology at H2O/GaSb(100) Interface under Ambient Conditions and GaSb Surface Passivation

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Product

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About

Observation of Surface-Bound Negatively Charged Hydride and Hydroxide on GaP(110) in H₂O Environments

Observation of Surface-Bound Negatively Charged Hydride and Hydroxide on GaP(110) in H₂O Environments

Evolution of Atomistic Topology at H₂O/GaSb(100) Interface under Ambient Conditions and GaSb Surface Passivation